WorldWideScience

Sample records for global ch4 budget

  1. The Global Methane Budget 2000-2012

    Science.gov (United States)

    Saunois, Marielle; Bousquet, Philippe; Poulter, Benjamin; Peregon, Anna; Ciais, Philippe; Canadell, Josep G.; Dlugokencky, Edward J.; Etiope, Giuseppe; Bastviken, David; Houweling, Sander; hide

    2016-01-01

    The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (approximately biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modeling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations).For the 2003-2012 decade, global methane emissions are estimated by top-down inversions at 558 TgCH4 yr(exp -1), range 540-568. About 60 of global emissions are anthropogenic (range 50-65%). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP

  2. Contribution of Anthropogenic and Natural Emissions to Global CH4 Balances by Utilizing δ13C-CH4 Observations in CarbonTracker Data Assimilation System (CTDAS)

    Science.gov (United States)

    Kangasaho, V. E.; Tsuruta, A.; Aalto, T.; Backman, L. B.; Houweling, S.; Krol, M. C.; Peters, W.; van der Laan-Luijkx, I. T.; Lienert, S.; Joos, F.; Dlugokencky, E. J.; Michael, S.; White, J. W. C.

    2017-12-01

    The atmospheric burden of CH4 has more than doubled since preindustrial time. Evaluating the contribution from anthropogenic and natural emissions to the global methane budget is of great importance to better understand the significance of different sources at the global scale, and their contribution to changes in growth rate of atmospheric CH4 before and after 2006. In addition, observations of δ13C-CH4 suggest an increase in natural sources after 2006, which matches the observed increase and variation of CH4 abudance. Methane emission sources can be identified using δ13C-CH4, because different sources produce methane with process-specific isotopic signatures. This study focuses on inversion model based estimates of global anthropogenic and natural methane emission rates to evaluate the existing methane emission estimates with a new δ13C-CH4 inversion system. In situ measurements of atmospheric methane and δ13C-CH4 isotopic signature, provided by the NOAA Global Monitoring Division and the Institute of Arctic and Alpine Research, will be assimilated into the CTDAS-13C-CH4. The system uses the TM5 atmospheric transport model as an observation operator, constrained by ECMWF ERA Interim meteorological fields, and off-line TM5 chemistry fields to account for the atmospheric methane sink. LPX-Bern DYPTOP ecosystem model is used for prior natural methane emissions from wetlands, peatlands and mineral soils, GFED v4 for prior fire emissions and EDGAR v4.2 FT2010 inventory for prior anthropogenic emissions. The EDGAR antropogenic emissions are re-divided into enteric fermentation and manure management, landfills and waste water, rice, coal, oil and gas, and residential emissions, and the trend of total emissions is scaled to match optimized anthropogenic emissions from CTE-CH4. In addition to these categories, emissions from termites and oceans are included. Process specific δ13C-CH4 isotopic signatures are assigned to each emission source to estimate 13CH4 fraction

  3. Global Inverse Modeling of CH4 and δ13C-CH4 Measurements to Understand Recent Trends in Methane Emissions

    Science.gov (United States)

    Karmakar, S.; Butenhoff, C. L.; Rice, A. L.; Khalil, A. K.

    2017-12-01

    Methane (CH4) is the second most important greenhouse gas with a radiative forcing of 0.97 W/m2 including both direct and indirect effects and a global warming potential of 28 over a 100-year time horizon. After a decades-long period of decline beginning in the 1980s, the methane growth rate rebounded in 2007 for reasons that are of current debate. During this same growth period atmospheric methane became less enriched in the 13CH4 isotope suggesting the recent CH4 growth was caused by an increase in 13CH4-depleted biogenic emissions. Recent papers have attributed this growth to increasing emissions from wetlands, rice agriculture, and ruminants. In this work we provide additional insight into the recent behavior of atmospheric methane and global wetland emissions by performing a three-dimensional Bayesian inversion of surface CH4 and 13CH4/12CH4 ratios using NOAA Global Monitoring Division (GMD) "event-level" CH4 measurements and the GEOS-Chem chemical-transport model (CTM) at a horizontal grid resolution of 2ox2.5o. The spatial pattern of wetland emissions was prescribed using soil moisture and temperature from GEOS-5 meteorology fields and soil carbon pools from the Lund-Potsdam-Jena global vegetation model. In order to reduce the aggregation error caused by a potentially flawed distribution and to account for isotopic measurements that indicate northern high latitude wetlands are isotopically depleted in 13CH4 relative to tropical wetlands we separated our pattern into three latitudinal bands (90-30°N, 30°N-0, 0-90°S). Our preliminary results support previous claims that the recent increase in atmospheric methane is driven by increases in biogenic CH4 emissions. We find that while wetland emissions from northern high latitudes (90-30°N) remained relatively constant during this time, southern hemisphere wetland emissions rebounded from a decade-long decline and began to rise again in 2007 and have remained elevated to the present. Emissions from rice

  4. Methane bubbling from northern lakes: present and future contributions to the global methane budget.

    Science.gov (United States)

    Walter, Katey M; Smith, Laurence C; Chapin, F Stuart

    2007-07-15

    Large uncertainties in the budget of atmospheric methane (CH4) limit the accuracy of climate change projections. Here we describe and quantify an important source of CH4 -- point-source ebullition (bubbling) from northern lakes -- that has not been incorporated in previous regional or global methane budgets. Employing a method recently introduced to measure ebullition more accurately by taking into account its spatial patchiness in lakes, we estimate point-source ebullition for 16 lakes in Alaska and Siberia that represent several common northern lake types: glacial, alluvial floodplain, peatland and thermokarst (thaw) lakes. Extrapolation of measured fluxes from these 16 sites to all lakes north of 45 degrees N using circumpolar databases of lake and permafrost distributions suggests that northern lakes are a globally significant source of atmospheric CH4, emitting approximately 24.2+/-10.5Tg CH4yr(-1). Thermokarst lakes have particularly high emissions because they release CH4 produced from organic matter previously sequestered in permafrost. A carbon mass balance calculation of CH4 release from thermokarst lakes on the Siberian yedoma ice complex suggests that these lakes alone would emit as much as approximately 49000Tg CH4 if this ice complex was to thaw completely. Using a space-for-time substitution based on the current lake distributions in permafrost-dominated and permafrost-free terrains, we estimate that lake emissions would be reduced by approximately 12% in a more probable transitional permafrost scenario and by approximately 53% in a 'permafrost-free' Northern Hemisphere. Long-term decline in CH4 ebullition from lakes due to lake area loss and permafrost thaw would occur only after the large release of CH4 associated thermokarst lake development in the zone of continuous permafrost.

  5. High Resolution CH4 Emissions and Dissolved CH4 Measurements Elucidate Surface Gas Exchange Processes in Toolik Lake, Arctic Alaska

    Science.gov (United States)

    Del Sontro, T.; Sollberger, S.; Kling, G. W.; Shaver, G. R.; Eugster, W.

    2013-12-01

    Approximately 14% of the Alaskan North Slope is covered in lakes of various sizes and depths. Diffusive carbon emissions (CH4 and CO2) from these lakes offset the tundra sink by ~20 %, but the offset would substantially increase if ebullitive CH4 emissions were also considered. Ultimately, arctic lake CH4 emissions are not insignificant in the global CH4 budget and their contribution is bound to increase due to impacts from climate change. Here we present high resolution CH4 emission data as measured via eddy covariance and a Los Gatos gas analyzer during the ice free period from Toolik Lake, a deep (20 m) Arctic lake located on the Alaskan North Slope, over the last few summers. Emissions are relatively low (Gatos gas analyzer. Thus, having both the flux and the CH4 gradient across the air-water interface measured directly, we can calculate k and investigate the processes influencing CH4 gas exchange in this lake. Preliminary results indicate that there are two regimes in wind speed that impact k - one at low wind speeds up to ~5 m s-1 and another at higher wind speeds (max ~10 m s-1). The differential wind speeds during night and day may compound the effect of convective mixing and cause the diurnal variation in observed fluxes.

  6. Evaluation of CH4 and N2O Budget of Natural Ecosystems and Croplands in Asia with a Process-based Model

    Science.gov (United States)

    Ito, A.

    2017-12-01

    Terrestrial ecosystems are important sink of carbon dioxide (CO2) but significant sources of other greenhouse gases such as methane (CH4) and nitrous oxide (N2O). To resolve the role of terrestrial biosphere in the climate system, we need to quantify total greenhouse gas budget with an adequate accuracy. In addition to top-down evaluation on the basis of atmospheric measurements, model-based approach is required for integration and up-scaling of filed data and for prediction under changing environment and different management practices. Since the early 2000s, we have developed a process-based model of terrestrial biogeochemical cycles focusing on atmosphere-ecosystem exchange of trace gases: Vegetation Integrated SImulator for Trace gases (VISIT). The model includes simple and comprehensive schemes of carbon and nitrogen cycles in terrestrial ecosystems, allowing us to capture dynamic nature of greenhouse gas budget. Beginning from natural ecosystems such as temperate and tropical forests, the models is now applicable to croplands by including agricultural practices such as planting, harvest, and fertilizer input. Global simulation results have been published from several papers, but model validation and benchmarking using up-to-date observations are remained for works. The model is now applied to several practical issues such as evaluation of N2O emission from bio-fuel croplands, which are expected to accomplish the mitigation target of the Paris Agreement. We also show several topics about basic model development such as revised CH4 emission affected by dynamic water-table and refined N2O emission from nitrification.

  7. Net exchanges of CO2, CH4 and N2O between the terrestrial ecosystems and the atmosphere in boreal and arctic region: Towards a full greenhouse gas budget

    Science.gov (United States)

    Zhang, B.; Tian, H.; Lu, C.; Yang, J.; Kamaljit, K.; Pan, S.

    2014-12-01

    Boreal and arctic terrestrial ecosystem is a unique ecological region due to large portion of wetland and permafrost distribution. Increasing disturbances, like permafrost-thaw, fire event, climate extreme, would greatly change the patterns and variations of greenhouse gas emission and further affect the feedback between terrestrial ecosystem and climate change. Carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O) accounted for more than 85% of the radioactive forcing (RF) due to long-lived greenhouse gases. However, few studies have considered the full budget of three gases together in this region. In this study, we used a process-based model (Dynamic Land Ecosystem Model), driven by multiple global change factors, to quantify the magnitude, spatial and temporal variation of CO2, CH4 and N2O across the boreal and arctic regions. Simulated results have been evaluated against field observations, inventory-based and atmospheric inversion estimates. By implementing a set of factorial simulations, we further quantify the relative contribution of climate, atmospheric composition, fire to the CO2, CH4 and N2O fluxes. Continued warming climate potentially could shift the inter-annual and intra-annual variation of greenhouse gases fluxes. The understanding of full budget in this region could provide insights for reasonable future projection, which is also crucial for developing effective mitigation strategies.

  8. Fluxes of CH4 and CO2 from soil and termite mounds in south Sudanian savanna of Burkina Faso (West Africa)

    Science.gov (United States)

    Brümmer, Christian; Papen, Hans; Wassmann, Reiner; Brüggemann, Nicolas

    2009-03-01

    The contribution of West African savanna ecosystems to global greenhouse gas budgets is highly uncertain. In this study we quantified soil-atmosphere CH4 and CO2 fluxes in the southwest of Burkina Faso from June to September 2005 and from April to September 2006 at four different agricultural fields planted with sorghum (n = 2), cotton, and peanut and at a natural savanna site with termite (Cubitermes fungifaber) mounds. During the rainy season both CH4 uptake and CH4 emission were observed in the savanna, which was on average a CH4 source of 2.79 and 2.28 kg CH4-C ha-1 a-1 in 2005 and 2006, respectively. The crop sites were an average CH4 sink of -0.67 and -0.70 kg CH4-C ha-1 a-1 in the 2 years, without significant seasonal variation. Mean annual soil respiration ranged between 3.86 and 5.82 t CO2-C ha-1 a-1 in the savanna and between 2.50 and 4.51 t CO2-C ha-1 a-1 at the crop sites. CH4 emission from termite mounds was 2 orders of magnitude higher than soil CH4 emissions, whereas termite CO2 emissions were of the same order of magnitude as soil CO2 emissions. Termite CH4 and CO2 release in the savanna contributed 8.8% and 0.4% to the total soil CH4 and CO2 emissions, respectively. At the crop sites, where termite mounds had been almost completely removed because of land use change, termite fluxes were insignificant. Mound density-based upscaling of termite CH4 fluxes resulted in a global termite CH4 source of 0.9 Tg a-1, which corresponds to 0.15% of the total global CH4 budget of 582 Tg a-1, hence significantly lower than those obtained previously by biomass-based calculations. This study emphasizes that land use change, which is of high relevance in this region, has particularly affected soil CH4 fluxes in the past and might still do so in the future.

  9. Biogenic CH4 and N2O emissions overwhelm land CO2 sink in Asia: Toward a full GHG budget

    Science.gov (United States)

    Tian, H.

    2017-12-01

    The recent global assessment indicates the terrestrial biosphere as a net source of greenhouse gases to the atmosphere (Tian et al Nature 2016). The fluxes of greenhouse gases (GHG) vary by region. Both TD and BU approaches indicate that human-caused biogenic fluxes of CO2, CH4 and N2O in the biosphere of Southern Asia led to a large net climate warming effect, because the 100-year cumulative effects of CH4 and N2O emissions together exceed that of the terrestrial CO2 sink. Southern Asia has about 90% of the global rice fields and represents more than 60% of the world's nitrogen fertilizer consumption, with 64%-81% of CH4 emissions and 36%-52% of N2O emissions derived from the agriculture and waste sectors. Given the large footprint of agriculture in Southern Asia, improved fertilizer use efficiency, rice management and animal diets could substantially reduce global agricultural N2O and CH4 emissions. This study highlights the importance of including all three major GHGs in regional climate impact assessments, mitigation option and climate policy development.

  10. In situ measurements of HCN and CH3CN over the Pacific Ocean: Sources, sinks, and budgets

    Science.gov (United States)

    Singh, H. B.; Salas, L.; Herlth, D.; Kolyer, R.; Czech, E.; Viezee, W.; Li, Q.; Jacob, D. J.; Blake, D.; Sachse, G.; Harward, C. N.; Fuelberg, H.; Kiley, C. M.; Zhao, Y.; Kondo, Y.

    2003-10-01

    We report the first in situ measurements of hydrogen cyanide (HCN) and methyl cyanide (CH3CN, acetonitrile) from the Pacific troposphere (0-12 km) obtained during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) airborne mission (February-April 2001). Mean HCN and CH3CN mixing ratios of 243 ± 118 (median 218) ppt and 149 ± 56 (median 138) ppt, respectively, were measured. These in situ observations correspond to a mean tropospheric HCN column of 4.2 × 1015 molecules cm-2 and a CH3CN column of 2.5 × 1015 molecules cm-2. This is in good agreement with the 0-12 km HCN column of 4.4 (±0.6) × 1015 molecules cm-2 derived from infrared solar spectroscopic observations over Japan. Mixing ratios of HCN and CH3CN were greatly enhanced in pollution outflow from Asia and were well correlated with each other as well as with known tracers of biomass combustion (e.g., CH3Cl, CO). Volumetric enhancement (or emission) ratios (ERs) relative to CO in free tropospheric plumes, likely originating from fires, were 0.34% for HCN and 0.17% for CH3CN. ERs with respect to CH3Cl and CO in selected biomass burning (BB) plumes in the free troposphere and in boundary layer pollution episodes are used to estimate a global BB source of 0.8 ± 0.4 Tg (N) yr-1 for HCN and 0.4 ± 0.1 Tg (N) yr-1 for CH3CN. In comparison, emissions from industry and fossil fuel combustion are quite small (atmospheric residence time of 5.0 months for HCN and 6.6 months for CH3CN is calculated. A global budget analysis shows that the sources and sinks of HCN and CH3CN are roughly in balance but large uncertainties remain in part due to a lack of observational data from the atmosphere and the oceans. Pathways leading to the oceanic (and soil) degradation of these cyanides are poorly known but are expected to be biological in nature.

  11. Long-Term Drainage Reduces CO2 Uptake and CH4 Emissions in a Siberian Permafrost Ecosystem

    Science.gov (United States)

    Kittler, Fanny; Heimann, Martin; Kolle, Olaf; Zimov, Nikita; Zimov, Sergei; Göckede, Mathias

    2017-12-01

    Permafrost landscapes in northern high latitudes with their massive organic carbon stocks are an important, poorly known, component of the global carbon cycle. However, in light of future Arctic warming, the sustainability of these carbon pools is uncertain. To a large part, this is due to a limited understanding of the carbon cycle processes because of sparse observations in Arctic permafrost ecosystems. Here we present an eddy covariance data set covering more than 3 years of continuous CO2 and CH4 flux observations within a moist tussock tundra ecosystem near Chersky in north-eastern Siberia. Through parallel observations of a disturbed (drained) area and a control area nearby, we aim to evaluate the long-term effects of a persistently lowered water table on the net vertical carbon exchange budgets and the dominating biogeochemical mechanisms. Persistently drier soils trigger systematic shifts in the tundra ecosystem carbon cycle patterns. Both, uptake rates of CO2 and emissions of CH4 decreased. Year-round measurements emphasize the importance of the non-growing season—in particular the "zero-curtain" period in the fall—to the annual budget. Approximately 60% of the CO2 uptake in the growing season is lost during the cold seasons, while CH4 emissions during the non-growing season account for 30% of the annual budget. Year-to-year variability in temperature conditions during the late growing season was identified as the primary control of the interannual variability observed in the CO2 and CH4 fluxes.

  12. Climate change impact of livestock CH4 emission in India: Global temperature change potential (GTP) and surface temperature response.

    Science.gov (United States)

    Kumari, Shilpi; Hiloidhari, Moonmoon; Kumari, Nisha; Naik, S N; Dahiya, R P

    2018-01-01

    Two climate metrics, Global surface Temperature Change Potential (GTP) and the Absolute GTP (AGTP) are used for studying the global surface temperature impact of CH 4 emission from livestock in India. The impact on global surface temperature is estimated for 20 and 100 year time frames due to CH 4 emission. The results show that the CH 4 emission from livestock, worked out to 15.3 Tg in 2012. In terms of climate metrics GTP of livestock-related CH 4 emission in India in 2012 were 1030 Tg CO 2 e (GTP 20 ) and 62 Tg CO 2 e (GTP 100 ) at the 20 and 100 year time horizon, respectively. The study also illustrates that livestock-related CH 4 emissions in India can cause a surface temperature increase of up to 0.7mK and 0.036mK over the 20 and 100 year time periods, respectively. The surface temperature response to a year of Indian livestock emission peaks at 0.9mK in the year 2021 (9 years after the time of emission). The AGTP gives important information in terms of temperature change due to annual CH 4 emissions, which is useful when comparing policies that address multiple gases. Copyright © 2017 Elsevier Inc. All rights reserved.

  13. Airborne measurements of CO2, CH4 and HCN in boreal biomass burning plumes

    Science.gov (United States)

    O'Shea, Sebastian J.; Bauguitte, Stephane; Muller, Jennifer B. A.; Le Breton, Michael; Archibald, Alex; Gallagher, Martin W.; Allen, Grant; Percival, Carl J.

    2013-04-01

    Biomass burning plays an important role in the budgets of a variety of atmospheric trace gases and particles. For example, fires in boreal Russia have been linked with large growths in the global concentrations of trace gases such as CO2, CH4 and CO (Langenfelds et al., 2002; Simpson et al., 2006). High resolution airborne measurements of CO2, CH4 and HCN were made over Eastern Canada onboard the UK Atmospheric Research Aircraft FAAM BAe-146 from 12 July to 4 August 2011. These observations were made as part of the BORTAS project (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites). Flights were aimed at transecting and sampling the outflow from the commonly occurring North American boreal forest fires during the summer months and to investigate and identify the chemical composition and evolution of these plumes. CO2 and CH4 dry air mole fractions were determined using an adapted system based on a Fast Greenhouse Gas Analyser (FGGA, Model RMT-200) from Los Gatos Research Inc, which uses the cavity enhanced absorption spectroscopy technique. In-flight calibrations revealed a mean accuracy of 0.57 ppmv and 2.31 ppbv for 1 Hz observations of CO2 and CH4, respectively, during the BORTAS project. During these flights a number of fresh and photochemically-aged plumes were identified using simultaneous HCN measurements. HCN is a distinctive and useful marker for forest fire emissions and it was detected using chemical ionisation mass spectrometry (CIMS). In the freshest plumes, strong relationships were found between CH4, CO2 and other tracers for biomass burning. From this we were able to estimate that 8.5 ± 0.9 g of CH4 and 1512 ± 185 g of CO2 were released into the atmosphere per kg of dry matter burnt. These emission factors are in good agreement with estimates from previous studies and can be used to calculate budgets for the region. However for aged plumes the correlations between CH4 and other

  14. Impact of short-lived non-CO2 mitigation on carbon budgets for stabilizing global warming

    International Nuclear Information System (INIS)

    Rogelj, Joeri; Riahi, Keywan; Meinshausen, Malte; Schaeffer, Michiel; Knutti, Reto

    2015-01-01

    Limiting global warming to any level requires limiting the total amount of CO 2 emissions, or staying within a CO 2 budget. Here we assess how emissions from short-lived non-CO 2 species like methane, hydrofluorocarbons (HFCs), black-carbon, and sulphates influence these CO 2 budgets. Our default case, which assumes mitigation in all sectors and of all gases, results in a CO 2 budget between 2011–2100 of 340 PgC for a >66% chance of staying below 2°C, consistent with the assessment of the Fifth Assessment Report of the Intergovernmental Panel on Climate Change. Extreme variations of air-pollutant emissions from black-carbon and sulphates influence this budget by about ±5%. In the hypothetical case of no methane or HFCs mitigation—which is unlikely when CO 2 is stringently reduced—the budgets would be much smaller (40% or up to 60%, respectively). However, assuming very stringent CH 4 mitigation as a sensitivity case, CO 2 budgets could be 25% higher. A limit on cumulative CO 2 emissions remains critical for temperature targets. Even a 25% higher CO 2 budget still means peaking global emissions in the next two decades, and achieving net zero CO 2 emissions during the third quarter of the 21st century. The leverage we have to affect the CO 2 budget by targeting non-CO 2 diminishes strongly along with CO 2 mitigation, because these are partly linked through economic and technological factors. (letter)

  15. CH4 emissions from European Major Population Centers: Results from aircraft-borne CH4 in-situ observations during EMeRGe-Europe campaign 2017

    Science.gov (United States)

    Roiger, A.; Klausner, T.; Schlager, H.; Ziereis, H.; Huntrieser, H.; Baumann, R.; Eirenschmalz, L.; Joeckel, P.; Mertens, M.; Fisher, R.; Bauguitte, S.; Young, S.; Andrés Hernández, M. D.

    2017-12-01

    Urban environments represent large and diffuse area sources of CH4 including emissions from pipeline leaks, industrial/sewage treatment plants, and landfills. However, there is little knowledge about the exact magnitude of these emissions and their contribution to total anthropogenic CH4. Especially in the context of an urbanizing world, a better understanding of the methane footprint of urban areas is crucial, both with respect to mitigation and projection of climate impacts. Aircraft-borne in-situ measurements are particularly useful to both quantify emissions from such area sources, as well as to study their impact on the regional distribution. However, airborne CH4 observations downstream of European cities are especially sparse.Here we report from aircraft-borne CH4 in-situ measurements as conducted during the HALO aircraft campaign EMeRGe (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global Scales) in July 2017, which was led by the University of Bremen, Germany. During seven research flights, emissions from a variety of European (Mega)-cities were probed at different altitudes from 3km down to 500m, including measurements in the outflows of London, Rome, Po Valley, Ruhr and Benelux. We will present and compare the CH4 distribution measured downstream of the various studied urban hot-spots. With the help of other trace gas measurements (including e.g. CO2, CO, O3, SO2), observed methane enhancements will be attributed to the different potential source types. Finally, by the combination of in-situ measurements and regional model simulations using the EMAC-MECO(n) model, the contribution of emissions from urban centers to the regional methane budget over Europe will be discussed.

  16. CH_3Cl, CH_2Cl_2, CHCl_3, and CCl_4: Infrared spectra, radiative efficiencies, and global warming potentials

    International Nuclear Information System (INIS)

    Wallington, Timothy J.; Pivesso, Bruno Pasquini; Lira, Alane Moura; Anderson, James E.; Nielsen, Claus Jørgen; Andersen, Niels Højmark; Hodnebrog, Øivind

    2016-01-01

    Infrared spectra for the title compounds were measured experimentally in 700 Torr of air at 295 K and systematically modeled in B3LYP, M06-2X and MP2 calculations employing various basis sets. Calibrated infrared spectra over the wavenumber range 600–3500 cm"−"1 are reported and combined with literature data to provide spectra for use in experimental studies and radiative transfer calculations. Integrated absorption cross sections are (units of cm"−"1 molecule"−"1): CH_3Cl, 660–780 cm"−"1, (3.89±0.19)×10"−"1"8; CH_2Cl_2, 650–800 cm"−"1, (2.16±0.11)×10"−"1"7; CHCl_3, 720–810 cm"−"1, (4.08±0.20)×10"−"1"7; and CCl_4, 730–825 cm"−"1, (6.30±0.31)×10"−"1"7. CH_3Cl, CH_2Cl_2, CHCl_3, and CCl_4 have radiative efficiencies of 0.004, 0.028, 0.070, and 0.174 W m"−"2 ppb"−"1 and global warming potentials (100 year horizon) of 5, 8, 15, and 1775, respectively. Quantum chemistry calculations generally predict larger band intensities than the experimental values. The best agreement with experiments is obtained in MP2(Full) calculations employing basis sets of at least triple-zeta quality augmented by diffuse functions. The B3LYP functional is found ill-suited for calculating vibrational frequencies and infrared intensities of halocarbons. - Highlights: • Infrared spectra reported for CH_3Cl, CH_2Cl_2, CHCl_3, and CCl_4. • REs of CH_3Cl, CH_2Cl_2, CHCl_3, and CCl_4 are 0.004, 0.028, 0.070, and 0.174 W m"−"2 ppb"−"1, respectively. • GWPs of CH_3Cl, CH_2Cl_2, CHCl_3, and CCl_4 are 5, 8, 15, and 1775, respectively.

  17. Global Carbon Budget 2017

    Science.gov (United States)

    Le Quéré, Corinne; Andrew, Robbie M.; Friedlingstein, Pierre; Sitch, Stephen; Pongratz, Julia; Manning, Andrew C.; Korsbakken, Jan Ivar; Peters, Glen P.; Canadell, Josep G.; Jackson, Robert B.; Boden, Thomas A.; Tans, Pieter P.; Andrews, Oliver D.; Arora, Vivek K.; Bakker, Dorothee C. E.; Barbero, Leticia; Becker, Meike; Betts, Richard A.; Bopp, Laurent; Chevallier, Frédéric; Chini, Louise P.; Ciais, Philippe; Cosca, Catherine E.; Cross, Jessica; Currie, Kim; Gasser, Thomas; Harris, Ian; Hauck, Judith; Haverd, Vanessa; Houghton, Richard A.; Hunt, Christopher W.; Hurtt, George; Ilyina, Tatiana; Jain, Atul K.; Kato, Etsushi; Kautz, Markus; Keeling, Ralph F.; Klein Goldewijk, Kees; Körtzinger, Arne; Landschützer, Peter; Lefèvre, Nathalie; Lenton, Andrew; Lienert, Sebastian; Lima, Ivan; Lombardozzi, Danica; Metzl, Nicolas; Millero, Frank; Monteiro, Pedro M. S.; Munro, David R.; Nabel, Julia E. M. S.; Nakaoka, Shin-ichiro; Nojiri, Yukihiro; Padin, X. Antonio; Peregon, Anna; Pfeil, Benjamin; Pierrot, Denis; Poulter, Benjamin; Rehder, Gregor; Reimer, Janet; Rödenbeck, Christian; Schwinger, Jörg; Séférian, Roland; Skjelvan, Ingunn; Stocker, Benjamin D.; Tian, Hanqin; Tilbrook, Bronte; Tubiello, Francesco N.; van der Laan-Luijkx, Ingrid T.; van der Werf, Guido R.; van Heuven, Steven; Viovy, Nicolas; Vuichard, Nicolas; Walker, Anthony P.; Watson, Andrew J.; Wiltshire, Andrew J.; Zaehle, Sönke; Zhu, Dan

    2018-03-01

    Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere - the global carbon budget - is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe data sets and methodology to quantify the five major components of the global carbon budget and their uncertainties. CO2 emissions from fossil fuels and industry (EFF) are based on energy statistics and cement production data, respectively, while emissions from land-use change (ELUC), mainly deforestation, are based on land-cover change data and bookkeeping models. The global atmospheric CO2 concentration is measured directly and its rate of growth (GATM) is computed from the annual changes in concentration. The ocean CO2 sink (SOCEAN) and terrestrial CO2 sink (SLAND) are estimated with global process models constrained by observations. The resulting carbon budget imbalance (BIM), the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the last decade available (2007-2016), EFF was 9.4 ± 0.5 GtC yr-1, ELUC 1.3 ± 0.7 GtC yr-1, GATM 4.7 ± 0.1 GtC yr-1, SOCEAN 2.4 ± 0.5 GtC yr-1, and SLAND 3.0 ± 0.8 GtC yr-1, with a budget imbalance BIM of 0.6 GtC yr-1 indicating overestimated emissions and/or underestimated sinks. For year 2016 alone, the growth in EFF was approximately zero and emissions remained at 9.9 ± 0.5 GtC yr-1. Also for 2016, ELUC was 1.3 ± 0.7 GtC yr-1, GATM was 6.1 ± 0.2 GtC yr-1, SOCEAN was 2.6 ± 0.5 GtC yr-1, and SLAND was 2.7 ± 1.0 GtC yr-1, with a small BIM of -0.3 GtC. GATM continued to be higher in 2016 compared to the past decade (2007-2016), reflecting in part the high fossil emissions and the small SLAND

  18. Global carbon budget 2013

    International Nuclear Information System (INIS)

    Le Quere, C.; Moriarty, R.; Jones, S.D.; Boden, T.A.; Peters, G.P.; Andrew, R.M.; Andres, R.J.; Ciais, P.; Bopp, L.; Maignan, F.; Viovy, N.

    2014-01-01

    Accurate assessment of anthropogenic carbon dioxide (CO 2 ) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe data sets and a methodology to quantify all major components of the global carbon budget, including their uncertainties, based on the combination of a range of data, algorithms, statistics and model estimates and their interpretation by a broad scientific community. We discuss changes compared to previous estimates, consistency within and among components, alongside methodology and data limitations. CO 2 emissions from fossil-fuel combustion and cement production (EFF) are based on energy statistics, while emissions from land-use change (ELUC), mainly deforestation, are based on combined evidence from land-cover change data, fire activity associated with deforestation, and models. The global atmospheric CO 2 concentration is measured directly and its rate of growth (GATM) is computed from the annual changes in concentration. The mean ocean CO 2 sink (SOCEAN) is based on observations from the 1990's, while the annual anomalies and trends are estimated with ocean models. The variability in SOCEAN is evaluated for the first time in this budget with data products based on surveys of ocean CO 2 measurements. The global residual terrestrial CO 2 sink (SLAND) is estimated by the difference of the other terms of the global carbon budget and compared to results of independent dynamic global vegetation models forced by observed climate, CO 2 and land cover change (some including nitrogen-carbon interactions). All uncertainties are reported as ±1, reflecting the current capacity to characterise the annual estimates of each component of the global carbon budget. For the last decade available (2003-2012), EFF was 8.6±0.4 GtC yr -1 , ELUC 0.9±0.5 GtC yr -1 , GATM 4.3±0

  19. Are CH2O measurements in the marine boundary layer suitable for testing the current understanding of CH4 photooxidation?: A model study

    Science.gov (United States)

    Wagner, V.; von Glasow, R.; Fischer, H.; Crutzen, P. J.

    2002-02-01

    On the basis of a data set collected during the Indian Ocean Experiment (INDOEX) campaign 1999, we investigated the formaldehyde (CH2O) budget in the southern Indian Ocean (SIO). With a photochemical box model we simulated the contribution of methane and nonmethane volatile organic compounds to the CH2O budget. To identify the reactions and model constraints that introduce the largest uncertainties in the modeled CH2O concentration, we carried out a local sensitivity analysis. Furthermore, a Monte Carlo method was used to assess the global error of the model predictions. According to this analysis the 2σ uncertainty in the modeled CH2O concentration is 49%. The deviation between observed (200 +/- 70 parts per trillion by volume (pptv) (2σ)) and modeled (224 +/- 110 pptv (2σ)) daily mean CH2O concentration is 12%. However, the combined errors of model and measurement are such that deviations as large as 65% are not significant at the 2σ level. Beyond the ``standard'' photochemistry we analyzed the impact of halogen and aerosol chemistry on the CH2O concentration and investigated the vertical distribution of CH2O in the marine boundary layer (MBL). Calculations with the Model of Chemistry Considering Aerosols indicate that, based on the current understanding, halogen chemistry and aerosol chemistry have no significant impact on the CH2O concentration under conditions encountered in the SIO. However, a detailed investigation including meteorological effects such as precipitation scavenging and convection reveals an uncertainty in state-of-the-art model predictions for CH2O in the MBL that is too large for a meaningful test of the current understanding of CH4 photooxidation.

  20. Global Methane Biogeochemistry

    Science.gov (United States)

    Reeburgh, W. S.

    2003-12-01

    Methane (CH4) has been studied as an atmospheric constituent for over 200 years. A 1776 letter from Alessandro Volta to Father Campi described the first experiments on flammable "air" released by shallow sediments in Lake Maggiore (Wolfe, 1996; King, 1992). The first quantitative measurements of CH4, both involving combustion and gravimetric determination of trapped oxidation products, were reported in French by Boussingault and Boussingault, 1864 and Gautier (1901), who reported CH4 concentrations of 10 ppmv and 0.28 ppmv (seashore) and 95 ppmv (Paris), respectively. The first modern measurements of atmospheric CH4 were the infrared absorption measurements of Migeotte (1948), who estimated an atmospheric concentration of 2.0 ppmv. Development of gas chromatography and the flame ionization detector in the 1950s led to observations of vertical CH4 distributions in the troposphere and stratosphere, and to establishment of time-series sampling programs in the late 1970s. Results from these sampling programs led to suggestions that the concentration of CH4, as that of CO2, was increasing in the atmosphere. The possible role of CH4 as a greenhouse gas stimulated further research on CH4 sources and sinks. Methane has also been of interest to microbiologists, but findings from microbiology have entered the larger context of the global CH4 budget only recently.Methane is the most abundant hydrocarbon in the atmosphere. It plays important roles in atmospheric chemistry and the radiative balance of the Earth. Stratospheric oxidation of CH4 provides a means of introducing water vapor above the tropopause. Methane reacts with atomic chlorine in the stratosphere, forming HCl, a reservoir species for chlorine. Some 90% of the CH4 entering the atmosphere is oxidized through reactions initiated by the OH radical. These reactions are discussed in more detail by Wofsy (1976) and Cicerone and Oremland (1988), and are important in controlling the oxidation state of the atmosphere

  1. Centennial evolution of the atmospheric methane budget: what do the carbon isotopes tell us?

    Directory of Open Access Journals (Sweden)

    K. R. Lassey

    2007-01-01

    Full Text Available Little is known about how the methane source inventory and sinks have evolved over recent centuries. New and detailed records of methane mixing ratio and isotopic composition (12CH4, 13CH4 and 14CH4 from analyses of air trapped in polar ice and firn can enhance this knowledge. We use existing bottom-up constructions of the source history, including "EDGAR"-based constructions, as inputs to a model of the evolving global budget for methane and for its carbon isotope composition through the 20th century. By matching such budgets to atmospheric data, we examine the constraints imposed by isotope information on those budget evolutions. Reconciling both 12CH4 and 13CH4 budgets with EDGAR-based source histories requires a combination of: a greater proportion of emissions from biomass burning and/or of fossil methane than EDGAR constructions suggest; a greater contribution from natural such emissions than is commonly supposed; and/or a significant role for active chlorine or other highly-fractionating tropospheric sink as has been independently proposed. Examining a companion budget evolution for 14CH4 exposes uncertainties in inferring the fossil-methane source from atmospheric 14CH4 data. Specifically, methane evolution during the nuclear era is sensitive to the cycling dynamics of "bomb 14C" (originating from atmospheric weapons tests through the biosphere. In addition, since ca. 1970, direct production and release of 14CH4 from nuclear-power facilities is influential but poorly quantified. Atmospheric 14CH4 determinations in the nuclear era have the potential to better characterize both biospheric carbon cycling, from photosynthesis to methane synthesis, and the nuclear-power source.

  2. Global Carbon Budget 2017

    Directory of Open Access Journals (Sweden)

    C. Le Quéré

    2018-03-01

    Full Text Available Accurate assessment of anthropogenic carbon dioxide (CO2 emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere – the global carbon budget – is important to better understand the global carbon cycle, support the development of climate policies, and project future climate change. Here we describe data sets and methodology to quantify the five major components of the global carbon budget and their uncertainties. CO2 emissions from fossil fuels and industry (EFF are based on energy statistics and cement production data, respectively, while emissions from land-use change (ELUC, mainly deforestation, are based on land-cover change data and bookkeeping models. The global atmospheric CO2 concentration is measured directly and its rate of growth (GATM is computed from the annual changes in concentration. The ocean CO2 sink (SOCEAN and terrestrial CO2 sink (SLAND are estimated with global process models constrained by observations. The resulting carbon budget imbalance (BIM, the difference between the estimated total emissions and the estimated changes in the atmosphere, ocean, and terrestrial biosphere, is a measure of imperfect data and understanding of the contemporary carbon cycle. All uncertainties are reported as ±1σ. For the last decade available (2007–2016, EFF was 9.4 ± 0.5 GtC yr−1, ELUC 1.3 ± 0.7 GtC yr−1, GATM 4.7 ± 0.1 GtC yr−1, SOCEAN 2.4 ± 0.5 GtC yr−1, and SLAND 3.0 ± 0.8 GtC yr−1, with a budget imbalance BIM of 0.6 GtC yr−1 indicating overestimated emissions and/or underestimated sinks. For year 2016 alone, the growth in EFF was approximately zero and emissions remained at 9.9 ± 0.5 GtC yr−1. Also for 2016, ELUC was 1.3 ± 0.7 GtC yr−1, GATM was 6.1 ± 0.2 GtC yr−1, SOCEAN was 2.6 ± 0.5 GtC yr−1, and SLAND was 2.7 ± 1.0 GtC yr−1, with a small BIM of −0.3 GtC. GATM continued to be

  3. Unusually Warm Spring Temperatures Magnify Annual CH4 Losses From Arctic Ecosystems

    Science.gov (United States)

    Goodrich, J. P.; Oechel, W. C.; Gioli, B.; Murphy, P.; Zona, D.

    2015-12-01

    The relatively fast pace of Northern high latitude warming puts the very large permafrost soil C pool at a higher risk of being lost to the atmosphere as CH4. Estimates for the Arctic tundra's contribution to the global wetland CH4 emissions range from 15-27 TgCH4 y-1 (8-14% of total). However, these estimates are largely based on data from the growing season, or from boreal systems underlain by discontinuous permafrost with different physical, hydrological, and biogeochemical dynamics than continuous permafrost zones. Recent data from a transect of eddy covariance flux towers across the North Slope of Alaska revealed the importance of cold season emissions to the annual CH4 budget, which may not correlate with summer flux patterns. However, understanding of the controls and inter-annual variability in fluxes at these different sites is lacking. Here, we present data from ~3 years at 5 tundra ecosystems along this Arctic transect to show the influence of earlier and deeper spring active layer thaw on timing and magnitude of CH4 fluxes. This year's warm spring led to significantly greater thaw depths and lower water tables than the previous year. Substantial CH4 emissions in 2015 were recorded at the wettest sites >20 days earlier than in the more meteorologically normal previous year. Since the soil remained saturated despite a lowered water table, total spring CH4 emissions more than doubled at these wet sites. At the drier sites, soil moisture declined with water table during the warmer spring, resulting in similar emissions to the previous year. However, deeper thaw depths prolonged fall and early winter emissions during the 'zero-curtain' soil temperature freezing phase, particularly at the drier site. In general, warmer spring temperatures in the Arctic may result in large increases in early season CH4 losses at wet sites and prolonged steady losses at the upland sites, enhancing the feedback between changing climate and tundra CH4 emissions at all sites.

  4. Climate change and global warming potentials

    International Nuclear Information System (INIS)

    Vate, J.F. van de

    1996-01-01

    Climate change and the global budgets of the two main energy consumption related greenhouse gases, CO 2 and CH 4 , are discussed. The global warming potential (GWP) of the non-CO 2 greenhouse gases is defined and the large range of GWPs of CH 4 in the literature is discussed. GWPs are expected to play an important role in energy policies and negotiations concerning lowering greenhouse gas emissions. (author). 20 refs, 4 figs, 4 tabs

  5. Tropical/Subtropical Peatland Development and Global CH4 during the Last Glaciation.

    Science.gov (United States)

    Xu, Hai; Lan, Jianghu; Sheng, Enguo; Liu, Yong; Liu, Bin; Yu, Keke; Ye, Yuanda; Cheng, Peng; Qiang, Xiaoke; Lu, Fengyan; Wang, Xulong

    2016-07-28

    Knowledge of peatland development over the tropical/subtropical zone during the last glaciation is critical for understanding the glacial global methane cycle. Here we present a well-dated 'peat deposit-lake sediment' alternate sequence at Tengchong, southwestern China, and discuss the peatland development and its linkage to the global glacial methane cycle. Peat layers were formed during the cold Marine Isotope Stage (MIS)-2 and -4, whereas lake sediments coincided with the relatively warm MIS-3, which is possibly related to the orbital/suborbital variations in both temperature and Asian summer monsoon intensity. The Tengchong peatland formation pattern is broadly synchronous with those over subtropical southern China and other tropical/subtropical areas, but it is clearly in contrast to those over the mid-high Northern Hemisphere. The results of this work suggest that the shifts of peatland development between the tropical/subtropical zone and mid-high Northern Hemisphere may have played important roles in the glacial/interglacial global atmospheric CH4 cycles.

  6. Global Carbon Budget 2016

    Science.gov (United States)

    Quéré, Corinne Le; Andrew, Robbie M.; Canadell, Josep G.; Sitch, Stephen; Korsbakken, Jan Ivar; Peters, Glen P.; Manning, Andrew C.; Boden, Thomas A.; Tans, Pieter P.; Houghton, Richard A.; hide

    2016-01-01

    .3+/-0.5 GtC/yr, ELUC 1.0+/-0.5 GtC/yr,GATM 4.5+/-0.1 GtC/yr, SOCEAN 2.6+/-0.5 GtC/yr, and SLAND 3.1+/-0.9 GtC/yr. For year 2015 alone, the growth in EFF was approximately zero and emissions remained at 9.9+/-0.5 GtC/yr, showing a slowdown in growth of these emissions compared to the average growth of 1.8/yr that took place during 2006-2015.Also, for 2015, ELUC was 1.3+/-0.5 GtC/yr, GATM was 6.3+/-0.2 GtC/yr, SOCEAN was 3.0+/-0.5 GtC/yr, and SLAND was 1.9+/-0.9 GtC/yr. GATM was higher in 2015 compared to the past decade (2006-2015), reflecting a smaller SLAND for that year. The global atmospheric CO2 concentration reached 399.4+/-0.1 ppm averaged over 2015. For 2016, preliminary data indicate the continuation of low growth in EFF with +0.2% (range of -1.0 to +1.8% ) based on national emissions projections for China and USA, and projections of gross domestic product corrected for recent changes in the carbon intensity of the economy for the rest of the world. In spite of the low growth of EFF in 2016, the growth rate in atmospheric CO2 concentration is expected to be relatively high because of the persistence of the smaller residual terrestrial sink (SLAND) in response to El Nino conditions of 2015-2016. From this projection of EFF and assumed constant ELUC for 2016, cumulative emissions of CO2 will reach 565+/-55 GtC (2075+/-205 GtCO2) for 1870-2016, about 75% from EFF and 25% from ELUC. This living data update documents changes in the methods and data sets used in this new carbon budget compared with previous publications of this data set.

  7. Impact of the heatwave in 2003 on the summer CH4 and N2O budget of a spruce forest ecosystem: A four-year comparison

    Science.gov (United States)

    Lamers, M.; Fiedler, S.; Jungkunst, H. F.; Stahr, K.; Streck, T.

    2009-04-01

    Both CH4 and N2O reduction and oxidation are highly sensitive to variation in soil moisture. Significant changes of net CH4 and total N2O fluxes from soils can therefore be expected to accompany redistribution for precipitation in the course of climate change where more extreme events are predicted for the future. The extreme summer drought in 2003 offered the unique opportunity to study the impact of such events on the emission of greenhouse gases, such as methane or nitrous oxide, under field conditions. The main objective of the present study was to evaluate the impact of the summer drought in 2003 on the net methane and nitrous oxide budget of a spruce forest ecosystem (South-West Germany) with large variation in soil drainage. During the summers of 2000-2004 we measured net CH4 and N2O fluxes (bi)-weekly using the closed-chamber technique for six different soil types ranging from well-aerated Cambisols to poorly drained Gleysols and a wet Histosol. With regard to CH4 the extreme summer draught (1) did not elevate net CH4-sink function of soils, but (2) highly reduced net CH4-source strength and (3) reversed the net CH4 source of the investigated catchment into a sink. In all four summers investigated, net ecosystem exchange of CH4 was found only in the hydromorphic soils but not in the dominant well-aerated soils. This highlighted the key role of hydromorphic soils for the investigated pedodiverse system. With regard to N2O the summer draught in 2003 significantly reduced N2O emissions at least for the Humic Gleysol and the Sapric Histosol and hence markedly reduced the net N2O source strength of the investigated ecosystem.

  8. Global Carbon Budget 2015

    Science.gov (United States)

    Le Quéré, C.; Moriarty, R.; Andrew, R. M.; Canadell, J. G.; Sitch, S.; Korsbakken, J. I.; Friedlingstein, P.; Peters, G. P.; Andres, R. J.; Boden, T. A.; Houghton, R. A.; House, J. I.; Keeling, R. F.; Tans, P.; Arneth, A.; Bakker, D. C. E.; Barbero, L.; Bopp, L.; Chang, J.; Chevallier, F.; Chini, L. P.; Ciais, P.; Fader, M.; Feely, R. A.; Gkritzalis, T.; Harris, I.; Hauck, J.; Ilyina, T.; Jain, A. K.; Kato, E.; Kitidis, V.; Klein Goldewijk, K.; Koven, C.; Landschützer, P.; Lauvset, S. K.; Lefèvre, N.; Lenton, A.; Lima, I. D.; Metzl, N.; Millero, F.; Munro, D. R.; Murata, A.; Nabel, J. E. M. S.; Nakaoka, S.; Nojiri, Y.; O'Brien, K.; Olsen, A.; Ono, T.; Pérez, F. F.; Pfeil, B.; Pierrot, D.; Poulter, B.; Rehder, G.; Rödenbeck, C.; Saito, S.; Schuster, U.; Schwinger, J.; Séférian, R.; Steinhoff, T.; Stocker, B. D.; Sutton, A. J.; Takahashi, T.; Tilbrook, B.; van der Laan-Luijkx, I. T.; van der Werf, G. R.; van Heuven, S.; Vandemark, D.; Viovy, N.; Wiltshire, A.; Zaehle, S.; Zeng, N.

    2015-12-01

    carbon budget. For the last decade available (2005-2014), EFF was 9.0 ± 0.5 GtC yr-1, ELUC was 0.9 ± 0.5 GtC yr-1, GATM was 4.4 ± 0.1 GtC yr-1, SOCEAN was 2.6 ± 0.5 GtC yr-1, and SLAND was 3.0 ± 0.8 GtC yr-1. For the year 2014 alone, EFF grew to 9.8 ± 0.5 GtC yr-1, 0.6 % above 2013, continuing the growth trend in these emissions, albeit at a slower rate compared to the average growth of 2.2 % yr-1 that took place during 2005-2014. Also, for 2014, ELUC was 1.1 ± 0.5 GtC yr-1, GATM was 3.9 ± 0.2 GtC yr-1, SOCEAN was 2.9 ± 0.5 GtC yr-1, and SLAND was 4.1 ± 0.9 GtC yr-1. GATM was lower in 2014 compared to the past decade (2005-2014), reflecting a larger SLAND for that year. The global atmospheric CO2 concentration reached 397.15 ± 0.10 ppm averaged over 2014. For 2015, preliminary data indicate that the growth in EFF will be near or slightly below zero, with a projection of -0.6 [range of -1.6 to +0.5] %, based on national emissions projections for China and the USA, and projections of gross domestic product corrected for recent changes in the carbon intensity of the global economy for the rest of the world. From this projection of EFF and assumed constant ELUC for 2015, cumulative emissions of CO2 will reach about 555 ± 55 GtC (2035 ± 205 GtCO2) for 1870-2015, about 75 % from EFF and 25 % from ELUC. This living data update documents changes in the methods and data sets used in this new carbon budget compared with previous publications of this data set (Le Quéré et al., 2015, 2014, 2013). All observations presented here can be downloaded from the Carbon Dioxide Information Analysis Center (doi:10.3334/CDIAC/GCP_2015).

  9. Global Carbon Budget 2017

    NARCIS (Netherlands)

    Le Quere, Corinne; Andrew, Robbie M.; Friedlingstein, Pierre; Sitch, Stephen; Pongratz, Julia; Manning, Andrew C.; Korsbakken, Jan Ivar; Peters, Glen P.; Canadell, Josep G.; Jackson, Robert B.; Boden, Thomas A.; Tans, Pieter P.; Andrews, Oliver D.; Arora, Vivek K.; Bakker, Dorothee C. E.; Barbero, Leticia; Becker, Meike; Betts, Richard A.; Bopp, Laurent; Chevallier, Frederic; Chini, Louise P.; Ciais, Philippe; Cosca, Catherine E.; Cross, Jessica; Currie, Kim; Gasser, Thomas; Harris, Ian; Hauck, Judith; Haverd, Vanessa; Houghton, Richard A.; Hunt, Christopher W.; Hurtt, George; Ilyina, Tatiana; Jain, Atul K.; Kato, Etsushi; Kautz, Markus; Keeling, Ralph F.; Goldewijk, Kees Klein; Koertzinger, Arne; Landschuetzer, Peter; Lefevre, Nathalie; Lenton, Andrew; Lienert, Sebastian; Lima, Ivan; Lombardozzi, Danica; Metzl, Nicolas; Millero, Frank; Monteiro, Pedro M. S.; Munro, David R.; Nabel, Julia E. M. S.; Nakaoka, Shin-ichiro; Nojiri, Yukihiro; Padin, X. Antonio; Peregon, Anna; Pfeil, Benjamin; Pierrot, Denis; Poulter, Benjamin; Rehder, Gregor; Reimer, Janet; Roedenbeck, Christian; Schwinger, Jorg; Seferian, Roland; Skjelvan, Ingunn; Stocker, Benjamin D.; Tian, Hanqin; Tilbrook, Bronte; Tubiello, Francesco N.; van der Laan-Luijkx, Ingrid T.; van der Werf, Guido R.; van Heuven, Steven; Viovy, Nicolas; Vuichard, Nicolas; Walker, Anthony P.; Watson, Andrew J.; Wiltshire, Andrew J.; Zaehle, Soenke; Zhu, Dan

    2018-01-01

    Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere - the "global carbon budget" - is important to better understand the global carbon cycle, support the development of climate policies, and project

  10. Global Carbon Budget 2016

    NARCIS (Netherlands)

    Le Quéré, Corinne; Andrew, Robbie M.; Canadell, Josep G.; Sitch, Stephen; Ivar Korsbakken, Jan; Peters, Glen P.; Manning, Andrew C.; Boden, Thomas A.; Tans, Pieter P.; Houghton, Richard A.; Keeling, Ralph F.; Alin, Simone; Andrews, Oliver D.; Anthoni, Peter; Barbero, Leticia; Bopp, Laurent; Chevallier, Frédéric; Chini, Louise P.; Ciais, Philippe; Currie, Kim; Delire, Christine; Doney, Scott C.; Friedlingstein, Pierre; Gkritzalis, Thanos; Harris, Ian A; Hauck, Judith; Haverd, Vanessa; Hoppema, Mario; Klein Goldewijk, Kees; Jain, Atul K.; Kato, Etsushi; Körtzinger, Arne; Landschützer, Peter; Lefèvre, Nathalie; Lenton, Andrew; Lienert, Sebastian; Lombardozzi, Danica; Melton, Joe R.; Metzl, Nicolas; Millero, Frank; Monteiro, Pedro M S; Munro, David R.; Nabel, Julia E M S; Nakaoka, Shin Ichiro; O'Brien, Kevin; Olsen, Are; Omar, Abdirahman M.; Ono, Tsuneo; Pierrot, Denis; Poulter, Benjamin; Rödenbeck, Christian; Salisbury, Joe; Schuster, Ute; Schwinger, Jörg; Séférian, Roland; Skjelvan, Ingunn; Stocker, Benjamin D.; Sutton, Adrienne J.; Takahashi, Taro; Tian, Hanqin; Tilbrook, Bronte; Van Der Laan-Luijkx, Ingrid T.; Van Der Werf, Guido R.; Viovy, Nicolas; Walker, Anthony P.; Wiltshire, Andrew J.; Zaehle, Sönke

    2016-01-01

    Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere-the "global carbon budget"-is important to better understand the global carbon cycle, support the development of climate policies, and project future

  11. Interannual variability in CO2 and CH4 exchange in a brackish tidal marsh in Northern California

    Science.gov (United States)

    Knox, S. H.; Windham-Myers, L.; Anderson, F. E.; Bergamaschi, B. A.

    2017-12-01

    Carbon (C) cycling in coastal wetlands is difficult to measure and model due to extremely dynamic atmospheric and hydrologic fluxes, as well as sensitivities to dynamic land- and ocean-based drivers. To date, few studies have begun continuous measurements of net ecosystem CO2 exchange (NEE) in these systems, and as such our understanding of the key drivers of NEE in coastal wetlands remain poorly understood. Recent eddy covariance measurements of NEE in these environments show considerable variability both within and across sites, with daily CO2 uptake and annual net CO2 budgets varying by nearly an order of magnitude between years and across locations. Furthermore, measurements of CH4 fluxes in these systems are even more limited, despite the potential for CH4 emissions from brackish and freshwater coastal wetlands. Here we present 3 years of near-continuous eddy covariance measurements of CO2 and CH4 fluxes from a brackish tidal marsh in Northern California and explore the drivers of interannual variability in CO2 and CH4 exchange. CO2 fluxes showed significant interannual variability; net CO2 uptake was near-zero in 2014 (6 ± 26 g C-CO2 m-2 yr-1), while much greater uptake was observed in 2015 and 2016 (209 ± 27 g C- CO2 m-2 yr-1 and 243 ± 26 g C-CO2 m-2 yr-1, respectively). Conversely, annual CH4 emissions were small and consistent across years, with the wetland emitting on average 1 ± 0.1 g C-CH4 m-2 yr-1. With respect to the net atmospheric GHG budget (assuming a sustained global warming potential (SGWP) of 45, expressed in units of CO2 equivalents), the wetland was near neutral in 2014, but a net GHG sink of 706 ± 105 g CO2 eq m-2 yr-1 and 836 ± 83 g CO2 eq m-2 yr-1 in 2015 and 2016, respectively. The large interannual variability in CO2 exchange was driven by notable year-to-year differences in temperature and precipitation as California experienced a severe drought and record high temperatures from 2012 to 2015. The large interannual variability in

  12. Tropospheric radiative forcing of CH4

    International Nuclear Information System (INIS)

    Grossman, A.S.; Grant, K.E.

    1994-04-01

    We have evaluated the tropospheric radiative forcing of CH 4 in the 0-3000 cm -1 wavenumber range and compared this with prior published calculations. The atmospheric test cases involved perturbed methane scenarios in both a McClatchey mid latitude, summer, clear sky approximation, model atmosphere, as well as a globally and seasonally averaged model atmosphere containing a representative cloud distribution. The scenarios involved pure CH 4 radiative forcing and CH 4 plus a mixture of H 2 O, CO 2 , O 3 , and N 2 O. The IR radiative forcing was calculated using a correlated k-distribution transmission model. The major purposes of this paper are to first, use the correlated k-distribution model to calculate the tropospheric radiative forcing for CH 4 , as the only radiatively active gas, and in a mixture with H 2 O, CO 2 , O 3 , and N 2 O, for a McClatchey mid-latitude summer, clear-sky model atmosphere, and to compare the results to those obtained in the studies mentioned above. Second, we will calculate the tropospheric methane forcing in a globally and annually averaged atmosphere with and without a representative cloud distribution in order to validate the conjecture given in IPCC (1990) that the inclusion of clouds in the forcing calculations results in forcing values which are approximately 20 percent less than those obtained using clear sky approximations

  13. Observational constraints on the global atmospheric budget of ethanol

    Directory of Open Access Journals (Sweden)

    V. Naik

    2010-06-01

    Full Text Available Energy security and climate change concerns have led to the promotion of biomass-derived ethanol, an oxygenated volatile organic compound (OVOC, as a substitute for fossil fuels. Although ethanol is ubiquitous in the troposphere, our knowledge of its current atmospheric budget and distribution is limited. Here, for the first time we use a global chemical transport model in conjunction with atmospheric observations to place constraints on the ethanol budget, noting that additional measurements of ethanol (and its precursors are still needed to enhance confidence in our estimated budget. Global sources of ethanol in the model include 5.0 Tg yr−1 from industrial sources and biofuels, 9.2 Tg yr−1 from terrestrial plants, ~0.5 Tg yr−1 from biomass burning, and 0.05 Tg yr−1 from atmospheric reactions of the ethyl peroxy radical (C2H5O2 with itself and with the methyl peroxy radical (CH3O2. The resulting atmospheric lifetime of ethanol in the model is 2.8 days. Gas-phase oxidation by the hydroxyl radical (OH is the primary global sink of ethanol in the model (65%, followed by dry deposition (25%, and wet deposition (10%. Over continental areas, ethanol concentrations predominantly reflect direct anthropogenic and biogenic emission sources. Uncertainty in the biogenic ethanol emissions, estimated at a factor of three, may contribute to the 50% model underestimate of observations in the North American boundary layer. Current levels of ethanol measured in remote regions are an order of magnitude larger than those in the model, suggesting a major gap in understanding. Stronger constraints on the budget and distribution of ethanol and OVOCs are a critical step towards assessing the impacts of increasing the use of ethanol as a fuel.

  14. Global Carbon Budget 2016

    Science.gov (United States)

    Le Quéré, Corinne; Andrew, Robbie M.; Canadell, Josep G.; Sitch, Stephen; Korsbakken, Jan Ivar; Peters, Glen P.; Manning, Andrew C.; Boden, Thomas A.; Tans, Pieter P.; Houghton, Richard A.; Keeling, Ralph F.; Alin, Simone; Andrews, Oliver D.; Anthoni, Peter; Barbero, Leticia; Bopp, Laurent; Chevallier, Frédéric; Chini, Louise P.; Ciais, Philippe; Currie, Kim; Delire, Christine; Doney, Scott C.; Friedlingstein, Pierre; Gkritzalis, Thanos; Harris, Ian; Hauck, Judith; Haverd, Vanessa; Hoppema, Mario; Klein Goldewijk, Kees; Jain, Atul K.; Kato, Etsushi; Körtzinger, Arne; Landschützer, Peter; Lefèvre, Nathalie; Lenton, Andrew; Lienert, Sebastian; Lombardozzi, Danica; Melton, Joe R.; Metzl, Nicolas; Millero, Frank; Monteiro, Pedro M. S.; Munro, David R.; Nabel, Julia E. M. S.; Nakaoka, Shin-ichiro; O'Brien, Kevin; Olsen, Are; Omar, Abdirahman M.; Ono, Tsuneo; Pierrot, Denis; Poulter, Benjamin; Rödenbeck, Christian; Salisbury, Joe; Schuster, Ute; Schwinger, Jörg; Séférian, Roland; Skjelvan, Ingunn; Stocker, Benjamin D.; Sutton, Adrienne J.; Takahashi, Taro; Tian, Hanqin; Tilbrook, Bronte; van der Laan-Luijkx, Ingrid T.; van der Werf, Guido R.; Viovy, Nicolas; Walker, Anthony P.; Wiltshire, Andrew J.; Zaehle, Sönke

    2016-11-01

    .3 ± 0.5 GtC yr-1, ELUC 1.0 ± 0.5 GtC yr-1, GATM 4.5 ± 0.1 GtC yr-1, SOCEAN 2.6 ± 0.5 GtC yr-1, and SLAND 3.1 ± 0.9 GtC yr-1. For year 2015 alone, the growth in EFF was approximately zero and emissions remained at 9.9 ± 0.5 GtC yr-1, showing a slowdown in growth of these emissions compared to the average growth of 1.8 % yr-1 that took place during 2006-2015. Also, for 2015, ELUC was 1.3 ± 0.5 GtC yr-1, GATM was 6.3 ± 0.2 GtC yr-1, SOCEAN was 3.0 ± 0.5 GtC yr-1, and SLAND was 1.9 ± 0.9 GtC yr-1. GATM was higher in 2015 compared to the past decade (2006-2015), reflecting a smaller SLAND for that year. The global atmospheric CO2 concentration reached 399.4 ± 0.1 ppm averaged over 2015. For 2016, preliminary data indicate the continuation of low growth in EFF with +0.2 % (range of -1.0 to +1.8 %) based on national emissions projections for China and USA, and projections of gross domestic product corrected for recent changes in the carbon intensity of the economy for the rest of the world. In spite of the low growth of EFF in 2016, the growth rate in atmospheric CO2 concentration is expected to be relatively high because of the persistence of the smaller residual terrestrial sink (SLAND) in response to El Niño conditions of 2015-2016. From this projection of EFF and assumed constant ELUC for 2016, cumulative emissions of CO2 will reach 565 ± 55 GtC (2075 ± 205 GtCO2) for 1870-2016, about 75 % from EFF and 25 % from ELUC. This living data update documents changes in the methods and data sets used in this new carbon budget compared with previous publications of this data set (Le Quéré et al., 2015b, a, 2014, 2013). All observations presented here can be downloaded from the Carbon Dioxide Information Analysis Center (doi:10.3334/CDIAC/GCP_2016).

  15. [The department budget, in the context of the hospital global budget. Initial results in general medicine].

    Science.gov (United States)

    Besançon, F

    1984-02-23

    In a general hospital (Hôtel-Dieu, in the center of Paris), run with a global budget, budgets determined for each unit were introduced as an experiment in 1980. Physicians were in charge of certain expenses, mainly: linen, drugs, transportation of patients to and from other hospitals within Paris, and blood fractions. The whole does not exceed 4% of the turnover (FF 20 millions in 1980) of a 67 bed internal medicine unit. Other accounts deal with the stays, admissions, prescriptions of technical acts, laboratory analyses, and X-rays. In 1980, expenses were 11% more than budgeted, but the increase in stays and particularly in admissions was significantly greater. The resulting savings were 8.8% and 18.7% for stays and admissions respectively. Psychic reactions were variable. The subsequent budgets followed the fluctuations of recorded expenses, which were fairly important in both directions. The unit budget may be an advance or a regression, in a restrictive and past-perpetuating context. The coherence between the unit budget and the global hospital budget is questionable. Physicians were willing to take part in accounting and saving. They have good reason for not enlarging their financial responsibilities. Conversely, they may give more attention to diseases of public opinion.

  16. Uncertainties in modelling CH4 emissions from northern wetlands in glacial climates: effect of hydrological model and CH4 model structure

    Directory of Open Access Journals (Sweden)

    J. van Huissteden

    2009-07-01

    Full Text Available Methane (CH4 fluxes from northern wetlands may have influenced atmospheric CH4 concentrations at climate warming phases during the last 800 000 years and during the present global warming. Including these CH4 fluxes in earth system models is essential to understand feedbacks between climate and atmospheric composition. Attempts to model CH4 fluxes from wetlands have previously been undertaken using various approaches. Here, we test a process-based wetland CH4 flux model (PEATLAND-VU which includes details of soil-atmosphere CH4 transport. The model has been used to simulate CH4 emissions from continental Europe in previous glacial climates and the current climate. This paper presents results regarding the sensitivity of modeling glacial terrestrial CH4 fluxes to (a basic tuning parameters of the model, (b different approaches in modeling of the water table, and (c model structure. In order to test the model structure, PEATLAND-VU was compared to a simpler modeling approach based on wetland primary production estimated from a vegetation model (BIOME 3.5. The tuning parameters are the CH4 production rate from labile organic carbon and its temperature sensitivity. The modelled fluxes prove comparatively insensitive to hydrology representation, while sensitive to microbial parameters and model structure. Glacial climate emissions are also highly sensitive to assumptions about the extent of ice cover and exposed seafloor. Wetland expansion over low relief exposed seafloor areas have compensated for a decrease of wetland area due to continental ice cover.

  17. Effects of globalization on state budgeting system in Ukraine

    Directory of Open Access Journals (Sweden)

    Bobukh S.О.

    2017-06-01

    Full Text Available When writing the scientific article the scientific approaches of scientists concerning the essence of budgeting have been described. The paper deals with the principles of budgeting on the basis of which three main methodological components are singled out. It also analyzes the budgeting goals. The author investigates the impact of globalization on the system of state budgeting in Ukraine, its positive and negative effects. Despite significant achievements it is necessary to explore the effects of globalization on the system of state budgeting in Ukraine. Budgeting is the management technology that provides the formation of budgets for the selected objects and their use to ensure optimal structure and correlation of profits and expenses, income and expenditure, assets and liabilities of the organization or its components to achieve the set goals taking into account the influence of the environment. It should be emphasized that budgeting in no way replaces the control system, but only creates a new approach to management from the standpoint of the balance of incomes and expenditures, profits and expenses, assets and liabilities of the organization as a whole or its components. The state budgeting of the country as the part of the financial system is the channel through which economic globalization, namely financial globalization, affects economic development of the state. Favorable global effect occurs, in particular, in terms of the impact on financial development. Therefore, it is necessary to + the nature of the relationship between these two processes.

  18. China’s regional CH_4 emissions: Characteristics, interregional transfer and mitigation policies

    International Nuclear Information System (INIS)

    Zhang, Bo; Yang, T.R.; Chen, B.; Sun, X.D.

    2016-01-01

    Highlights: • China’s CH_4 emissions have significant contributions to global climate change. • The total CH_4 emissions in 2010 amount to 44.3 Tg, half from energy activities. • Half of the national total direct emissions are embodied in interregional trade. • 2/3 of the embodied emission transfers via domestic trade are energy-related. • A national comprehensive action plan to reduce CH_4 emissions should be designed. - Abstract: Methane (CH_4), the second largest greenhouse gas emitted in China, hasn’t been given enough attention in the country’s policies and actions for addressing climate change. This paper aims to perform a bottom-up estimation and multi-regional input–output analysis for China’s anthropogenic CH_4 emissions from both production-based and consumption-based insights. As the world’s largest CH_4 emitter, China’s total anthropogenic CH_4 emissions in 2010 are estimated at 44.3 Tg and correspond to 1507.9 Mt CO_2-eq by the lower global warming potential factor of 34. Energy activities as the largest contributor hold about half of the national total emissions, mainly from coal mining. Inherent economic driving factors covering consumption, investment and international exports play an important role in determining regional CH_4 emission inventories. Interregional transfers of embodied emissions via domestic trade are equivalent to half of the national total emissions from domestic production, of which two thirds are energy-related embodied emissions. Most central and western regions as net interregional CH_4 exporters such as Shanxi and Inner Mongolia have higher direct emissions, while the eastern coastal regions as net interregional importers such as Guangdong and Jiangsu always have larger embodied emissions. Since China’s CH_4 emissions have significant contributions to global climate change, a national comprehensive action plan to reduce CH_4 emissions should be designed by considering supply-side and demand

  19. Spatial and temporal patterns of CH4 and N2O fluxes in terrestrial ecosystems of North America during 1979–2008: application of a global biogeochemistry model

    Directory of Open Access Journals (Sweden)

    C. Lu

    2010-09-01

    Full Text Available Continental-scale estimations of terrestrial methane (CH4 and nitrous oxide (N2O fluxes over a long time period are crucial to accurately assess the global balance of greenhouse gases and enhance our understanding and prediction of global climate change and terrestrial ecosystem feedbacks. Using a process-based global biogeochemical model, the Dynamic Land Ecosystem Model (DLEM, we quantified simultaneously CH4 and N2O fluxes in North America's terrestrial ecosystems from 1979 to 2008. During the past 30 years, approximately 14.69 ± 1.64 T g C a−1 (1 T g = 1012 g of CH4, and 1.94 ± 0.1 T g N a−1 of N2O were released from terrestrial ecosystems in North America. At the country level, both the US and Canada acted as CH4 sources to the atmosphere, but Mexico mainly oxidized and consumed CH4 from the atmosphere. Wetlands in North America contributed predominantly to the regional CH4 source, while all other ecosystems acted as sinks for atmospheric CH4, of which forests accounted for 36.8%. Regarding N2O emission in North America, the US, Canada, and Mexico contributed 56.19%, 18.23%, and 25.58%, respectively, to the continental source over the past 30 years. Forests and croplands were the two ecosystems that contributed most to continental N2O emission. The inter-annual variations of CH4 and N2O fluxes in North America were mainly attributed to year-to-year climatic variability. While only annual precipitation was found to have a significant effect on annual CH4 flux, both mean annual temperature and annual precipitation were significantly correlated to annual N2O flux. The regional estimates and spatiotemporal patterns of terrestrial ecosystem CH4 and N2O fluxes in North America generated in this study provide useful information for global change research and policy making.

  20. Comparisons of the error budgets associated with ground-based FTIR measurements of atmospheric CH4 profiles at Île de la Réunion and Jungfraujoch.

    Science.gov (United States)

    Vanhaelewyn, Gauthier; Duchatelet, Pierre; Vigouroux, Corinne; Dils, Bart; Kumps, Nicolas; Hermans, Christian; Demoulin, Philippe; Mahieu, Emmanuel; Sussmann, Ralf; de Mazière, Martine

    2010-05-01

    The Fourier Transform Infra Red (FTIR) remote measurements of atmospheric constituents at the observatories at Saint-Denis (20.90°S, 55.48°E, 50 m a.s.l., Île de la Réunion) and Jungfraujoch (46.55°N, 7.98°E, 3580 m a.s.l., Switzerland) are affiliated to the Network for the Detection of Atmospheric Composition Change (NDACC). The European NDACC FTIR data for CH4 were improved and homogenized among the stations in the EU project HYMN. One important application of these data is their use for the validation of satellite products, like the validation of SCIAMACHY or IASI CH4 columns. Therefore, it is very important that errors and uncertainties associated to the ground-based FTIR CH4 data are well characterized. In this poster we present a comparison of errors on retrieved vertical concentration profiles of CH4 between Saint-Denis and Jungfraujoch. At both stations, we have used the same retrieval algorithm, namely SFIT2 v3.92 developed jointly at the NASA Langley Research Center, the National Center for Atmospheric Research (NCAR) and the National Institute of Water and Atmosphere Research (NIWA) at Lauder, New Zealand, and error evaluation tools developed at the Belgian Institute for Space Aeronomy (BIRA-IASB). The error components investigated in this study are: smoothing, noise, temperature, instrumental line shape (ILS) (in particular the modulation amplitude and phase), spectroscopy (in particular the pressure broadening and intensity), interfering species and solar zenith angle (SZA) error. We will determine if the characteristics of the sites in terms of altitude, geographic locations and atmospheric conditions produce significant differences in the error budgets for the retrieved CH4 vertical profiles

  1. CH-53K Heavy Lift Replacement Helicopter (CH-53K)

    Science.gov (United States)

    2015-12-01

    Selected Acquisition Report (SAR) RCS: DD-A&T(Q&A)823-390 CH-53K Heavy Lift Replacement Helicopter (CH-53K) As of FY 2017 President’s Budget...December 2015 SAR March 4, 2016 10:04:18 UNCLASSIFIED 4 Col Henry Vanderborght PMA-261 Heavy Lift Helicopters Program Executive Office - Air, Anti...757-5780 Fax: 301-757-5109 DSN Phone: 757-5780 DSN Fax: 757-5109 Date Assigned: May 29, 2014 Program Information Program Name CH-53K Heavy Lift

  2. Megafauna and frozen soil: the drivers of atmospheric CH4 dynamics

    Science.gov (United States)

    Zimov, N.; Zimov, S. A.

    2010-12-01

    During the last deglaciation (LD) a strong increase in atmospheric methane (CH4) concentrations occurred simultaneously with a rise in Greenland temperatures indicating that in the north, during this time period, strong CH4 sources “awakened”, as additionally documented by the appearance of a strong gradient between northern (Greenland) and southern (Antarctica) hemisphere atmospheric CH4 concentrations. This rise could not be caused by wetland expansion. A reconstruction of peatland formation dynamics has indicated that wetlands on Earth were few in LD and only actively expanded 10,000 yr BP, after atmospheric CH4 concentrations began to decline. Destabilization of methane clathrates also could not be the source for atmospheric CH4 increase. Geological CH4 (including methane clathrates) has the highest deuterium content (δD) among all of the known sources of CH4 while atmospheric CH4 δD values determined for the LD were record low. To explain recorded atmospheric CH4 and its isotopic dynamics required a strong northern source, which was active only during the LD and that provided very low δD CH4 values. Such a source is permafrost thawing under anaerobic conditions (or better stated soils of mammoth steppe-tundra ecosystems). Permafrost thawing is the strongest, among known, wetland sources (usually over 100g CH4/m2yr) and has a unique isotopic signature (δD = -400 per mil (-338 to -479 per mil), δ13C = -73 per mil (-58 to -99 per mil)). The main sources of atmospheric CH4 have different isotopic signatures (δ13C, δD). The isotopic content of atmospheric CH4 is a simple function of the weight average for all of the sources. Inclusion of permafrost source into a budget model of the atmospheric methane and its isotopes allowed us to reconstruct the dynamics of methane’s main sources. Model indicated geological source to be negligible as in LGM so and in LD and Holocene. During the glaciation, the largest methane source was megafauna, whose 1.4

  3. Global volcanic emissions: budgets, plume chemistry and impacts

    Science.gov (United States)

    Mather, T. A.

    2012-12-01

    Over the past few decades our understanding of global volcanic degassing budgets, plume chemistry and the impacts of volcanic emissions on our atmosphere and environment has been revolutionized. Global volcanic emissions budgets are needed if we are to make effective use of regional and global atmospheric models in order to understand the consequences of volcanic degassing on global environmental evolution. Traditionally volcanic SO2 budgets have been the best constrained but recent efforts have seen improvements in the quantification of the budgets of other environmentally important chemical species such as CO2, the halogens (including Br and I) and trace metals (including measurements relevant to trace metal atmospheric lifetimes and bioavailability). Recent measurements of reactive trace gas species in volcanic plumes have offered intriguing hints at the chemistry occurring in the hot environment at volcanic vents and during electrical discharges in ash-rich volcanic plumes. These reactive trace species have important consequences for gas plume chemistry and impacts, for example, in terms of the global fixed nitrogen budget, volcanically induced ozone destruction and particle fluxes to the atmosphere. Volcanically initiated atmospheric chemistry was likely to have been particularly important before biological (and latterly anthropogenic) processes started to dominate many geochemical cycles, with important consequences in terms of the evolution of the nitrogen cycle and the role of particles in modulating the Earth's climate. There are still many challenges and open questions to be addressed in this fascinating area of science.

  4. Effects of plant species on soil microbial processes and CH4 emission from constructed wetlands

    International Nuclear Information System (INIS)

    Wang, Yanhua; Yang, Hao; Ye, Chun; Chen, Xia; Xie, Biao; Huang, Changchun; Zhang, Jixiang; Xu, Meina

    2013-01-01

    Methane (CH 4 ) emission from constructed wetland has raised environmental concern. This study evaluated the influence of mono and polyculture constructed wetland and seasonal variation on CH 4 fluxes. Methane emission data showed large temporal variation ranging from 0 to 249.29 mg CH 4 m −2 h −1 . Results indicated that the highest CH 4 flux was obtained in the polyculture system, planted with Phragmites australis, Zizania latifolia and Typha latifolia, reflecting polyculture system could stimulate CH 4 emission. FISH analysis showed the higher amount of methanotrophs in the profile of Z. latifolia in both mono and polyculture systems. The highest methanogens amount and relatively lower methanotrophs amount in the profile of polyculture system were obtained. The results support the characteristics of CH 4 fluxes. The polyculture constructed wetland has the higher potential of global warming. -- Highlights: ► The polyculture constructed wetland has the higher contribution to CH 4 emission. ► The CH 4 –C conversion ranged from 0 to 3.7%. ► The Z. latifolia played important roles in methanotrophs growth and CH 4 consumption. ► Major influence of T-N, TOC and plant cover on CH 4 emission was obtained. -- The polyculture constructed wetland has the higher contribution to global warming

  5. Regional emission and loss budgets of atmospheric methane (2002-2012)

    Science.gov (United States)

    Saeki, T.; Patra, P. K.; Dlugokencky, E. J.; Ishijima, K.; Umezawa, T.; Ito, A.; Aoki, S.; Morimoto, S.; Kort, E. A.; Crotwell, A. M.; Ravi Kumar, K.; Nakazawa, T.

    2015-12-01

    Methane (CH4) plays important roles in atmospheric chemistry and short-term forcing of climate. Clear understanding of atmospheric CH4's budget of emissions and losses is required to aid sustainable development of Earth's future environment. We used an atmospheric chemistry-transport model (JAMSTEC's ACTM) for simulating atmospheric CH4. An inverse modeling system has been developed for estimating CH4 emissions (7 ensemble cases) from 53 land regions for 2002-2012 using measurements at 39 sites. Global net CH4 emissions varied between 505-509 and 524-545 Tg/yr during 2002-2004 and 2010-2012, respectively (ranges based on 6 inversion cases), with a step like increase in 2007 in agreement with atmospheric measurement. The inversion system did not account for interannual variations in radicals reacting with CH4 in atmosphere. Our results suggest that the recent update of EDGAR inventory (version 4.2FT2010) overestimated global total emissions by at least 25 Tg/yr in 2010. Increase in CH4 emission since 2004 originated in the tropical and southern hemisphere regions, with timing consistent with an increase of non-dairy cattle stocks by ~10% in 2012 from 1056 million heads in 2002, leading to ~10 Tg/yr increase in emissions from enteric fermentation. All 7 inversions robustly estimated the interannual variations in emissions, but poorly constrained the seasonal cycle amplitude or phase consistently for all regions due to sparse observational network. Forward simulation results using both the a priori and a posteriori emissions are compared with independent aircraft measurements for validation. By doing that we are able to reject the upper limit (545 Tg/yr) of global total emissions as 14 Tg/yr too high during 2008-2012, which allows us to further conclude that CH4 emission increase rate over the East Asia (China mainly) region was 7-8 Tg/yr between the 2002-2006 and 2008-2012 periods, contrary to 1-17 Tg/yr in the a priori emissions.

  6. Carbon emission from global hydroelectric reservoirs revisited.

    Science.gov (United States)

    Li, Siyue; Zhang, Quanfa

    2014-12-01

    Substantial greenhouse gas (GHG) emissions from hydropower reservoirs have been of great concerns recently, yet the significant carbon emitters of drawdown area and reservoir downstream (including spillways and turbines as well as river reaches below dams) have not been included in global carbon budget. Here, we revisit GHG emission from hydropower reservoirs by considering reservoir surface area, drawdown zone and reservoir downstream. Our estimates demonstrate around 301.3 Tg carbon dioxide (CO2)/year and 18.7 Tg methane (CH4)/year from global hydroelectric reservoirs, which are much higher than recent observations. The sum of drawdown and downstream emission, which is generally overlooked, represents 42 % CO2 and 67 % CH4 of the total emissions from hydropower reservoirs. Accordingly, the global average emissions from hydropower are estimated to be 92 g CO2/kWh and 5.7 g CH4/kWh. Nonetheless, global hydroelectricity could currently reduce approximate 2,351 Tg CO2eq/year with respect to fuel fossil plant alternative. The new findings show a substantial revision of carbon emission from the global hydropower reservoirs.

  7. Contrasting regional versus global radiative forcing by megacity pollution emissions

    Science.gov (United States)

    Dang, H.; Unger, N.

    2015-10-01

    We assess the regional and global integrated radiative forcing on 20- and 100-year time horizons caused by a one-year pulse of present day pollution emissions from 10 megacity areas: Los Angeles, Mexico City, New York City, Sao Paulo, Lagos, Cairo, New Delhi, Beijing, Shanghai and Manila. The assessment includes well-mixed greenhouse gases: carbon dioxide (CO2), nitrous oxide (N2O), methane (CH4); and short-lived climate forcers: tropospheric ozone (O3) and fine mode aerosol particles (sulfate, nitrate, black carbon, primary and secondary organic aerosol). All megacities contribute net global warming on both time horizons. Most of the 10 megacity areas exert a net negative effect on their own regional radiation budget that is 10-100 times larger in magnitude than their global radiative effects. Of the cities examined, Beijing, New Delhi, Shanghai and New York contribute most to global warming with values ranging from +0.03 to 0.05 Wm-2yr on short timescales and +0.07-0.10 Wm-2yr on long timescales. Regional net 20-year radiative effects are largest for Mexico City (-0.84 Wm-2yr) and Beijing (-0.78 Wm-2yr). Megacity reduction of non-CH4 O3 precursors to improve air quality offers zero co-benefits to global climate. Megacity reduction of aerosols to improve air quality offers co-benefits to the regional radiative budget but minimal or no co-benefits to global climate with the exception of black carbon reductions in a few cities, especially Beijing and New Delhi. Results suggest that air pollution and global climate change mitigation can be treated as separate environmental issues in policy at the megacity level with the exception of CH4 action. Individual megacity reduction of CO2 and CH4 emissions can mitigate global warming and therefore offers climate safety improvements to the entire planet.

  8. Large emissions from floodplain trees close the Amazon methane budget

    Science.gov (United States)

    Pangala, Sunitha R.; Enrich-Prast, Alex; Basso, Luana S.; Peixoto, Roberta Bittencourt; Bastviken, David; Hornibrook, Edward R. C.; Gatti, Luciana V.; Marotta, Humberto; Calazans, Luana Silva Braucks; Sakuragui, Cassia Mônica; Bastos, Wanderley Rodrigues; Malm, Olaf; Gloor, Emanuel; Miller, John Bharat; Gauci, Vincent

    2017-12-01

    Wetlands are the largest global source of atmospheric methane (CH4), a potent greenhouse gas. However, methane emission inventories from the Amazon floodplain, the largest natural geographic source of CH4 in the tropics, consistently underestimate the atmospheric burden of CH4 determined via remote sensing and inversion modelling, pointing to a major gap in our understanding of the contribution of these ecosystems to CH4 emissions. Here we report CH4 fluxes from the stems of 2,357 individual Amazonian floodplain trees from 13 locations across the central Amazon basin. We find that escape of soil gas through wetland trees is the dominant source of regional CH4 emissions. Methane fluxes from Amazon tree stems were up to 200 times larger than emissions reported for temperate wet forests and tropical peat swamp forests, representing the largest non-ebullitive wetland fluxes observed. Emissions from trees had an average stable carbon isotope value (δ13C) of -66.2 ± 6.4 per mil, consistent with a soil biogenic origin. We estimate that floodplain trees emit 15.1 ± 1.8 to 21.2 ± 2.5 teragrams of CH4 a year, in addition to the 20.5 ± 5.3 teragrams a year emitted regionally from other sources. Furthermore, we provide a ‘top-down’ regional estimate of CH4 emissions of 42.7 ± 5.6 teragrams of CH4 a year for the Amazon basin, based on regular vertical lower-troposphere CH4 profiles covering the period 2010-2013. We find close agreement between our ‘top-down’ and combined ‘bottom-up’ estimates, indicating that large CH4 emissions from trees adapted to permanent or seasonal inundation can account for the emission source that is required to close the Amazon CH4 budget. Our findings demonstrate the importance of tree stem surfaces in mediating approximately half of all wetland CH4 emissions in the Amazon floodplain, a region that represents up to one-third of the global wetland CH4 source when trees are combined with other emission sources.

  9. Large emissions from floodplain trees close the Amazon methane budget.

    Science.gov (United States)

    Pangala, Sunitha R; Enrich-Prast, Alex; Basso, Luana S; Peixoto, Roberta Bittencourt; Bastviken, David; Hornibrook, Edward R C; Gatti, Luciana V; Marotta, Humberto; Calazans, Luana Silva Braucks; Sakuragui, Cassia Mônica; Bastos, Wanderley Rodrigues; Malm, Olaf; Gloor, Emanuel; Miller, John Bharat; Gauci, Vincent

    2017-12-14

    Wetlands are the largest global source of atmospheric methane (CH 4 ), a potent greenhouse gas. However, methane emission inventories from the Amazon floodplain, the largest natural geographic source of CH 4 in the tropics, consistently underestimate the atmospheric burden of CH 4 determined via remote sensing and inversion modelling, pointing to a major gap in our understanding of the contribution of these ecosystems to CH 4 emissions. Here we report CH 4 fluxes from the stems of 2,357 individual Amazonian floodplain trees from 13 locations across the central Amazon basin. We find that escape of soil gas through wetland trees is the dominant source of regional CH 4 emissions. Methane fluxes from Amazon tree stems were up to 200 times larger than emissions reported for temperate wet forests and tropical peat swamp forests, representing the largest non-ebullitive wetland fluxes observed. Emissions from trees had an average stable carbon isotope value (δ 13 C) of -66.2 ± 6.4 per mil, consistent with a soil biogenic origin. We estimate that floodplain trees emit 15.1 ± 1.8 to 21.2 ± 2.5 teragrams of CH 4 a year, in addition to the 20.5 ± 5.3 teragrams a year emitted regionally from other sources. Furthermore, we provide a 'top-down' regional estimate of CH 4 emissions of 42.7 ± 5.6 teragrams of CH 4 a year for the Amazon basin, based on regular vertical lower-troposphere CH 4 profiles covering the period 2010-2013. We find close agreement between our 'top-down' and combined 'bottom-up' estimates, indicating that large CH 4 emissions from trees adapted to permanent or seasonal inundation can account for the emission source that is required to close the Amazon CH 4 budget. Our findings demonstrate the importance of tree stem surfaces in mediating approximately half of all wetland CH 4 emissions in the Amazon floodplain, a region that represents up to one-third of the global wetland CH 4 source when trees are combined with other emission sources.

  10. Constraining global methane emissions and uptake by ecosystems

    International Nuclear Information System (INIS)

    Spahni, R.; Wania, R.; Neef, L.; Van Weele, M.; Van Velthoven, P.; Pison, I.; Bousquet, P.

    2011-01-01

    Natural methane (CH 4 ) emissions from wet ecosystems are an important part of today's global CH 4 budget. Climate affects the exchange of CH 4 between ecosystems and the atmosphere by influencing CH 4 production, oxidation, and transport in the soil. The net CH 4 exchange depends on ecosystem hydrology, soil and vegetation characteristics. Here, the LPJ-WHyMe global dynamical vegetation model is used to simulate global net CH 4 emissions for different ecosystems: northern peat-lands (45 degrees-90 degrees N), naturally inundated wetlands (60 degrees S-45 degrees N), rice agriculture and wet mineral soils. Mineral soils are a potential CH 4 sink, but can also be a source with the direction of the net exchange depending on soil moisture content. The geographical and seasonal distributions are evaluated against multi-dimensional atmospheric inversions for 2003-2005, using two independent four-dimensional variational assimilation systems. The atmospheric inversions are constrained by the atmospheric CH 4 observations of the SCIAMACHY satellite instrument and global surface networks. Compared to LPJ-WHyMe the inversions result in a significant reduction in the emissions from northern peat-lands and suggest that LPJ-WHyMe maximum annual emissions peak about one month late. The inversions do not put strong constraints on the division of sources between inundated wetlands and wet mineral soils in the tropics. Based on the inversion results we diagnose model parameters in LPJ-WHyMe and simulate the surface exchange of CH 4 over the period 1990-2008. Over the whole period we infer an increase of global ecosystem CH 4 emissions of +1.11 TgCH 4 yr -1 , not considering potential additional changes in wetland extent. The increase in simulated CH 4 emissions is attributed to enhanced soil respiration resulting from the observed rise in land temperature and in atmospheric carbon dioxide that were used as input. The long term decline of the atmospheric CH 4 growth rate from 1990

  11. Direct Measurements of Leaf Level CH4 and CO2 Exchange in a Boreal Forest

    Science.gov (United States)

    Crill, P.; Lindroth, A.; Vestin, P.; Båth, A.

    2008-12-01

    Reports of aerobic CH4 sources from leaves and litter of a variety of forests and plant functional types have added a potential mystery to our understanding of CH4 dynamics especially if these sources contribute enough to have a significant impact on the global budget. We have made direct measurements of leaf level CH4 and CO2 exchange using a quartz branch cuvette in a boreal forest in Norunda, Sweden since August of this year. The cuvette was temperature controlled and was designed to close for 5 minutes every 30 minutes. Air was circulated to a Los Gatos CH4/CO2 infrared absorption laser spectrometer. Air and cuvette temperatures, PAR and UV radiation (Kipp and Zonen, CUV4; spectral range 300-380 nm) were measured at the branch chamber. The study was made in the Norunda 100 years old stand consisting of a mixture of Scots pine (Pinus sylvestris L.) , Birch (Betula sp.) and Norway spruce (Picea abies (L.) Karst.). The cuvette was moved between trees at roughly 5 day intervals. A null empty cuvette period was included in the rotation. The initial data show the expected CO2 uptake correlated with incident PAR and low rates of emission at night. However, there was no clear pattern of emissions detectable in the CH4. We estimate that we should be able to resolve a change of 0.5 ppbv CH4 min- 1 with our analytical setup. Both the daytime (1000-1600) and nighttime (2200-0400) averages were less than our detection. Even on very sunny days with high PAR and UV flux values, no consistent pattern was detectable. The lack of a distinct signal may be due to the fact that the past month has been very rainy, it is late in the growth season at these latitudes and sun angles are increasing quickly. The trees were at the northern edge of a clearing and we were also measuring mid height (2-3 m) leaves and branches of young trees. The branch cuvette design can also be optimized to improve its sensitivity.

  12. Integrated rice-duck farming decreases global warming potential and increases net ecosystem economic budget in central China.

    Science.gov (United States)

    Sheng, Feng; Cao, Cou-Gui; Li, Cheng-Fang

    2018-05-31

    Over the past decades, many attempts have been made to assess the effects of integrated rice-duck farming on greenhouse gas emissions, use efficient of energy, soil fertility, and economic significance. However, very few studies have been focused on the effects of the farming on net ecosystem economic budget (NEEB). Here, a 2-year field experiment was conducted to comprehensively investigate the effects of ducks raised in paddy fields on CH 4 and N 2 O emissions, global warming potential (GWP), rice grain yield, and NEEB in central China. The experiment included two treatments: integrated rice-duck farming (RD) and conventional rice farming (R). The introduction of ducks into the paddy fields markedly increased the rice grain yield due to enhanced tiller number and root bleeding rate. RD treatment significantly elevated the N 2 O emissions (p < 0.05) but decreased CH 4 emissions (p < 0.05) during rice growing seasons compared with R treatment. Analysis of GWP based on CH 4 and N 2 O emissions showed that compared with R treatment, RD treatment significantly decreased the GWP by 28.1 and 28.0% and reduced the greenhouse gas intensity by 30.6 and 29.8% in 2009 and 2010, respectively. In addition, RD treatment increased NEEB by 40.8 and 39.7% respectively in 2009 and 2010 relative to R treatment. Taken together, our results suggest that the integrated rice-duck farming system is an effective strategy to optimize the economic and environmental benefits of paddy fields in central China.

  13. Glacial/interglacial wetland, biomass burning, and geologic methane emissions constrained by dual stable isotopic CH4 ice core records

    Science.gov (United States)

    Bock, Michael; Schmitt, Jochen; Beck, Jonas; Seth, Barbara; Chappellaz, Jérôme; Fischer, Hubertus

    2017-07-01

    Atmospheric methane (CH4) records reconstructed from polar ice cores represent an integrated view on processes predominantly taking place in the terrestrial biogeosphere. Here, we present dual stable isotopic methane records [δ13CH4 and δD(CH4)] from four Antarctic ice cores, which provide improved constraints on past changes in natural methane sources. Our isotope data show that tropical wetlands and seasonally inundated floodplains are most likely the controlling sources of atmospheric methane variations for the current and two older interglacials and their preceding glacial maxima. The changes in these sources are steered by variations in temperature, precipitation, and the water table as modulated by insolation, (local) sea level, and monsoon intensity. Based on our δD(CH4) constraint, it seems that geologic emissions of methane may play a steady but only minor role in atmospheric CH4 changes and that the glacial budget is not dominated by these sources. Superimposed on the glacial/interglacial variations is a marked difference in both isotope records, with systematically higher values during the last 25,000 y compared with older time periods. This shift cannot be explained by climatic changes. Rather, our isotopic methane budget points to a marked increase in fire activity, possibly caused by biome changes and accumulation of fuel related to the late Pleistocene megafauna extinction, which took place in the course of the last glacial.

  14. Effect of interannual variation in winter vertical mixing on CH4 dynamics in a subtropical reservoir

    Science.gov (United States)

    Itoh, Masayuki; Kobayashi, Yuki; Chen, Tzong-Yueh; Tokida, Takeshi; Fukui, Manabu; Kojima, Hisaya; Miki, Takeshi; Tayasu, Ichiro; Shiah, Fuh-Kwo; Okuda, Noboru

    2015-07-01

    Although freshwaters are considered to be substantial natural sources of atmospheric methane (CH4), in situ processes of CH4 production and consumption in freshwater ecosystems are poorly understood, especially in subtropical areas, leading to uncertainties in the estimation of global CH4 emissions. To improve our understanding of physical and biogeochemical factors affecting CH4 dynamics in subtropical lakes, we examined vertical and seasonal profiles of dissolved CH4 and its carbon isotope ratio (δ13C) and conducted incubation experiments to assess CH4 production and oxidation in the deep subtropical Fei-Tsui Reservoir (FTR; Taiwan). The mixing pattern of the FTR is essentially monomixis, but the intensity of winter vertical mixing changes with climatic conditions. In years with incomplete vertical mixing (does not reach the bottom) and subsequent strong thermal stratification resulting in profundal hypoxia, we observed increases in sedimentary CH4 production and thus profundal CH4 storage with the development of reducing conditions. In contrast, in years with strong winter vertical mixing to the bottom of the reservoir, CH4 production was suppressed under NO3--rich conditions, during which denitrifiers have the competitive advantage over methanogens. Diffusive emission from profundal CH4 storage appeared to be negligible due to the efficiency of CH4 oxidation during ascent through methane-oxidizing bacteria (MOB) activity. Most of the profundal CH4 was rapidly oxidized by MOB in both oxic and anoxic layers, as characterized by its carbon isotope signature. In contrast, aerobic CH4 production in the subsurface layer, which may be enhanced under high temperatures in summer, may account for a large portion of atmospheric CH4 emissions from this reservoir. Our CH4 profiling results provide valuable information for future studies predicting CH4 emissions from subtropical lakes with the progress of global warming.

  15. The global carbon budget 1959–2011

    Directory of Open Access Journals (Sweden)

    C. Le Quéré

    2013-05-01

    Full Text Available Accurate assessments of anthropogenic carbon dioxide (CO2 emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere is important to better understand the global carbon cycle, support the climate policy process, and project future climate change. Present-day analysis requires the combination of a range of data, algorithms, statistics and model estimates and their interpretation by a broad scientific community. Here we describe datasets and a methodology developed by the global carbon cycle science community to quantify all major components of the global carbon budget, including their uncertainties. We discuss changes compared to previous estimates, consistency within and among components, and methodology and data limitations. CO2 emissions from fossil fuel combustion and cement production (EFF are based on energy statistics, while emissions from Land-Use Change (ELUC, including deforestation, are based on combined evidence from land cover change data, fire activity in regions undergoing deforestation, and models. The global atmospheric CO2 concentration is measured directly and its rate of growth (GATM is computed from the concentration. The mean ocean CO2 sink (SOCEAN is based on observations from the 1990s, while the annual anomalies and trends are estimated with ocean models. Finally, the global residual terrestrial CO2 sink (SLAND is estimated by the difference of the other terms. For the last decade available (2002–2011, EFF was 8.3 ± 0.4 PgC yr−1, ELUC 1.0 ± 0.5 PgC yr−1, GATM 4.3 ± 0.1PgC yr−1, SOCEAN 2.5 ± 0.5 PgC yr−1, and SLAND 2.6 ± 0.8 PgC yr−1. For year 2011 alone, EFF was 9.5 ± 0.5 PgC yr−1, 3.0 percent above 2010, reflecting a continued trend in these emissions; ELUC was 0.9 ± 0.5 PgC yr−1, approximately constant throughout the decade; GATM was 3.6 ± 0.2 PgC yr−1, SOCEAN was 2.7 ± 0.5 PgC yr−1, and SLAND was 4.1 ± 0.9 PgC yr−1. GATM was low in 2011

  16. Toward an Improved Understanding of the Global Fresh Water Budget

    Science.gov (United States)

    Hildebrand, Peter H.

    2005-01-01

    The major components of the global fresh water cycle include the evaporation from the land and ocean surfaces, precipitation onto the Ocean and land surfaces, the net atmospheric transport of water from oceanic areas over land, and the return flow of water from the land back into the ocean. The additional components of oceanic water transport are few, principally, the mixing of fresh water through the oceanic boundary layer, transport by ocean currents, and sea ice processes. On land the situation is considerably more complex, and includes the deposition of rain and snow on land; water flow in runoff; infiltration of water into the soil and groundwater; storage of water in soil, lakes and streams, and groundwater; polar and glacial ice; and use of water in vegetation and human activities. Knowledge of the key terms in the fresh water flux budget is poor. Some components of the budget, e.g. precipitation, runoff, storage, are measured with variable accuracy across the globe. We are just now obtaining precise measurements of the major components of global fresh water storage in global ice and ground water. The easily accessible fresh water sources in rivers, lakes and snow runoff are only adequately measured in the more affluent portions of the world. presents proposals are suggesting methods of making global measurements of these quantities from space. At the same time, knowledge of the global fresh water resources under the effects of climate change is of increasing importance and the human population grows. This paper provides an overview of the state of knowledge of the global fresh water budget, evaluating the accuracy of various global water budget measuring and modeling techniques. We review the measurement capabilities of satellite instruments as compared with field validation studies and modeling approaches. Based on these analyses, and on the goal of improved knowledge of the global fresh water budget under the effects of climate change, we suggest

  17. High rate monitoring CH4 production dynamics and their link with behavioral phases in cattle

    OpenAIRE

    Blaise, Yannick; Lebeau, Frédéric; Andriamandroso, Andriamasinoro; Beckers, Yves; Heinesch, Bernard; Bindelle, Jérôme

    2016-01-01

    Microbial fermentation in the rumen produces methane (CH4) which is a loss of energy for ruminants and also contributes to global warming. While the respiration chamber is the standard reference for CH4 emissions quantification, daily CH4 production dynamics can be measured only by steps of 30 min and measurements on pasture are impossible. The alternative method using SF6 as tracer gas can be applied for grazing animals but provides average CH4 production values over at least several hours, ...

  18. (CH4)-C-14 Measurements in Greenland Ice: Investigating Last Glacial Termination CH4 Sources

    DEFF Research Database (Denmark)

    Petrenko, V. V.; Smith, A. M.; Brook, E. J.

    2009-01-01

    by direct cosmogenic C-14 production in ice. C-14 of CO was measured to better understand this process and correct the sample (CH4)-C-14. Corrected results suggest that wetland sources were likely responsible for the majority of the Younger Dryas-Preboreal CH4 rise.......The cause of a large increase of atmospheric methane concentration during the Younger Dryas-Preboreal abrupt climatic transition (similar to 11,600 years ago) has been the subject of much debate. The carbon-14 (C-14) content of methane ((CH4)-C-14) should distinguish between wetland and clathrate...... contributions to this increase. We present measurements of (CH4)-C-14 in glacial ice, targeting this transition, performed by using ice samples obtained from an ablation site in west Greenland. Measured (CH4)-C-14 values were higher than predicted under any scenario. Sample (CH4)-C-14 appears to be elevated...

  19. Effects of permafrost thaw on CO2 and CH4 exchange in a western Alaska peatland chronosequence

    Science.gov (United States)

    Carmel E. Johnston,; Stephanie A. Ewing,; Harden, Jennifer W.; Ruth K. Varner,; Wickland, Kimberly P.; Koch, Joshua C.; Fuller, Christopher C.; Manies, Kristen L.; M. Torre Jorgenson,

    2014-01-01

    Permafrost soils store over half of global soil carbon (C), and northern frozen peatlands store about 10% of global permafrost C. With thaw, inundation of high latitude lowland peatlands typically increases the surface-atmosphere flux of methane (CH4), a potent greenhouse gas. To examine the effects of lowland permafrost thaw over millennial timescales, we measured carbon dioxide (CO2) and CH4 exchange along sites that constitute a ~1000 yr thaw chronosequence of thermokarst collapse bogs and adjacent fen locations at Innoko Flats Wildlife Refuge in western Alaska. Peak CH4exchange in July (123 ± 71 mg CH4–C m−2 d−1) was observed in features that have been thawed for 30 to 70 (peatlands, particularly those developed on poorly drained mineral substrates, are a key locus of elevated CH4 emission to the atmosphere that must be considered for a complete understanding of high latitude CH4 dynamics.

  20. How to oxidize atmospheric CH4? - A challenge for the future

    International Nuclear Information System (INIS)

    Chazelas, Bruno; Leger, Alain; Ollivier, Marc

    2006-01-01

    Methane is an active Greenhouse effect gas whose concentration will likely increase in the future. The possible destabilisation of CH 4 clathrates (hydrates) due to anthropogenic climate warming, and the resulting outgasing of methane, could lead to a major increase of the global Greenhouse effect, with dramatic consequences for Humanity. For these reasons, the study of possible countermeasures should be actively considered. Here, we suggest taking advantage of the thermodynamic instability of CH 4 in air, and search for ways to oxidize it

  1. Assessment of winter fluxes of CO2 and CH4 in boreal forest soils of central Alaska estimated by the profile method and the chamber method: a diagnosis of methane emission and implications for the regional carbon budget

    International Nuclear Information System (INIS)

    Kim, Yongwon; Ueyama, Masahito; Harazono, Yoshinobu; Tanaka, Noriyuki; Nakagawa, Fumiko; Tsunogai, Urumu

    2007-01-01

    This research was carried out to estimate the winter fluxes of CO 2 and CH 4 using the concentration profile method and the chamber method in black spruce forest soils in central Alaska during the winter of 2004/5. The average winter fluxes of CO 2 and CH 4 by chamber and profile methods were 0.24 ± 0.06 (SE; standard error) and 0.21 ± 0.06 gCO 2 -C/m2/d, and 21.4 ± 5.6 and 21.4 ± 14 μgCH 4 -C/m2/hr. This suggests that the fluxes estimated by the two methods are not significantly different based on a one-way ANOVA with a 95% confidence level. The hypothesis on the processes of CH 4 transport/production/emission in underlying snow-covered boreal forest soils is proven by the pressure differences between air and in soil at 30 cm depth. The winter CO 2 emission corresponds to 23% of the annual CO 2 emitted from Alaska black spruce forest soils, which resulted in the sum of mainly root respiration and microbial respiration during the winter based on the (delta) 13 CO 2 of -2.25%. The average wintertime emissions of CO 2 and CH 4 were 49 ± 13 gCO 2 -C/m 2 /season and 0.11 ± 0.07 gCH 4 -C/m 2 /season, respectively. This implies that winter emissions of CO 2 and CH 4 are an important part of the annual carbon budget in seasonally snow-covered terrain of typical boreal forest soils

  2. Refined global methyl halide budgets with respect to rapeseed (Brassica napus) by life-cycle measurements

    Science.gov (United States)

    Jiao, Y.; Acdan, J.; Xu, R.; Deventer, M. J.; Rhew, R. C.

    2017-12-01

    A precise quantification of global methyl halide budgets is needed to evaluate the ozone depletion potential of these compounds and to predict future changes of stratospheric ozone. However, the global budgets of methyl halides are not balanced between currently identified and quantified sources and sinks. Our study re-evaluated the methyl bromide budget from global cultivated rapeseed (Brassica napus) through life-cycle flux measurements both in the greenhouse and in the field, yielding a methyl bromide emission rate that scales globally to 1.0 - 1.2 Gg yr-1. While this indicates a globally significant source, it is much smaller than the previously widely cited value of 5 - 6 Gg yr-1(Mead et al., 2008), even taking into account the near tripling of annual global yield of rapeseed since the previous evaluation was conducted. Our study also evaluated the methyl chloride and methyl iodide emission levels from rapeseed, yielding emission rates that scale to 5.4 Gg yr-1 for methyl chloride and 1.8 Gg yr-1 of methyl iodide. The concentrations of the methyl donor SAM (S-adenosyl methionine) and the resultant product SAH (S-Adenosyl-L-homocysteine) were also analyzed to explore their role in biogenic methyl halide formation. Halide gradient incubations showed that the magnitude of methyl halide emissions from rapeseed is highly correlated to soil halide levels, thus raising the concern that the heterogeneity of soil halide contents geographically should be considered when extrapolating to global budget.

  3. Study of atmospheric CH4 mole fractions at three WMO/GAW stations in China

    Science.gov (United States)

    Fang, Shuang-Xi; Zhou, Ling-Xi; Masarie, Kenneth A.; Xu, Lin; Rella, Chris W.

    2013-05-01

    CH4 mole fractions were continuously measured from 2009 to 2011 at three WMO/GAW stations in China (Lin'an, LAN; Longfengshan, LFS; and Waliguan, WLG) using three Cavity Ring Down Spectroscopy instruments. LAN and LFS are GAW regional measurement stations. LAN is located in China's most economically developed region, and LFS is in a rice production area (planting area > 40,000 km2). WLG is a global measurement station in remote northwest China. At LAN, high methane mole fractions are observed in all seasons. Surface winds from the northeast enhance CH4 values, with a maximum increase of 32 ± 15 ppb in summer. The peak to peak amplitude of the seasonal cycle is 77 ± 35 ppb. At LFS, the diurnal cycle amplitude is approximately constant throughout the year except summer, when a value of 196 ± 65 ppb is observed. CH4 values at LFS reach their peak in July, which is different from seasonal variations typically observed in the northern hemisphere. CH4 mole fractions at WLG show both the smallest values and the lowest variability. Maximum values occur during summer, which is different from other northern hemisphere WMO/GAW global stations. The seasonal cycle amplitude is 17 ± 11 ppb. The linear growth rates at LAN, LFS, and WLG are 8.0 ± 1.2, 7.9 ± 0.9, and 9.4 ± 0.2 ppb yr-1, respectively, which are all larger than the global mean over the same 3 year period. Results from this study attempt to improve our basic understanding of observed atmospheric CH4 in China.

  4. Using ‘snapshot’ measurements of CH4 fluxes from an ombrotrophic peatland to estimate annual budgets: interpolation versus modelling

    Directory of Open Access Journals (Sweden)

    S.M. Green

    2017-03-01

    Full Text Available Flux-chamber measurements of greenhouse gas exchanges between the soil and the atmosphere represent a snapshot of the conditions on a particular site and need to be combined or used in some way to provide integrated fluxes for the longer time periods that are often of interest. In contrast to carbon dioxide (CO2, most studies that have estimated the time-integrated flux of CH4 on ombrotrophic peatlands have not used models. Typically, linear interpolation is used to estimate CH4 fluxes during the time periods between flux-chamber measurements. CH4 fluxes generally show a rise followed by a fall through the growing season that may be captured reasonably well by interpolation, provided there are sufficiently frequent measurements. However, day-to-day and week-to-week variability is also often evident in CH4 flux data, and will not necessarily be properly represented by interpolation. Using flux chamber data from a UK blanket peatland, we compared annualised CH4 fluxes estimated by interpolation with those estimated using linear models and found that the former tended to be higher than the latter. We consider the implications of these results for the calculation of the radiative forcing effect of ombrotrophic peatlands.

  5. The Extent of CH4 Emission and Oxidation in Thermogenic and Biogenic Gas Hydrate Environments

    Science.gov (United States)

    Kastner, M.; Solem, C.; Bartlett, D.; MacDonald, I.; Valentine, D.

    2003-12-01

    The role of methane hydrate in the global methane budget is poorly understood, because relatively little is known about the transport of gaseous and dissolved methane through the seafloor into the ocean, from the water column into the atmosphere, and the extent of water-column methanotrophy that occurs en route. We characterize the transport and consumption of methane in three distinct gas hydrate environments, spanning the spectrum of thermogenic and biogenic methane occurrences: Bush Hill in the Gulf of Mexico, Eel River off the coast of Northern California, and the Noth and South Hydrate Ridges on the Cascadia Oregon margin. At all the sites studied a significant enrichment in δ 13CH4 with distance along isopycnals away from the methane source is observed, indicative of extensive aerobic bacterial methane oxidation in the water column. The effects of this process are principally pronounced in the mostly biogenic methane setting, with δ 13C-CH4 measured as high as -12 permil (PDB) between North and South Hydrate Ridge. The δ 13C-CH4 values ranged from -12 to -67 permil at Hydrate Ridge, -34 to -52 permil at Eel River, and -41 to -49 permil at Bush Hill. The large variation in methane carbon isotope ranges between the sites suggest that major differences exist in both the rates of aerobic methane oxidation and system openness at the studied locations. A mean kinetic isotope fractionation factor is being determined using a closed-system Rayleigh distillation model. An approximate regional methane flux from the ocean into the atmosphere is being estimated for the Gulf of Mexico, by extrapolation of the flux value from the Bush Hill methane plume over 390 plume locations having persistent oil slicks on the ocean surface, mapped by time series satellite data.

  6. Effect of permafrost thaw on CO2 and CH4 exchange in a western Alaska peatland chronosequence

    International Nuclear Information System (INIS)

    Johnston, Carmel E; Ewing, Stephanie A; Harden, Jennifer W; Fuller, Christopher C; Manies, Kristen; Varner, Ruth K; Wickland, Kimberly P; Koch, Joshua C; Jorgenson, M Torre

    2014-01-01

    Permafrost soils store over half of global soil carbon (C), and northern frozen peatlands store about 10% of global permafrost C. With thaw, inundation of high latitude lowland peatlands typically increases the surface-atmosphere flux of methane (CH 4 ), a potent greenhouse gas. To examine the effects of lowland permafrost thaw over millennial timescales, we measured carbon dioxide (CO 2 ) and CH 4 exchange along sites that constitute a ∼1000 yr thaw chronosequence of thermokarst collapse bogs and adjacent fen locations at Innoko Flats Wildlife Refuge in western Alaska. Peak CH 4 exchange in July (123 ± 71 mg CH 4 –C m −2 d −1 ) was observed in features that have been thawed for 30 to 70 (<100) yr, where soils were warmer than at more recently thawed sites (14 to 21 yr; emitting 1.37 ± 0.67 mg CH 4 –C m −2 d −1 in July) and had shallower water tables than at older sites (200 to 1400 yr; emitting 6.55 ± 2.23 mg CH 4 –C m −2 d −1 in July). Carbon lost via CH 4 efflux during the growing season at these intermediate age sites was 8% of uptake by net ecosystem exchange. Our results provide evidence that CH 4 emissions following lowland permafrost thaw are enhanced over decadal time scales, but limited over millennia. Over larger spatial scales, adjacent fen systems may contribute sustained CH 4 emission, CO 2 uptake, and DOC export. We argue that over timescales of decades to centuries, thaw features in high-latitude lowland peatlands, particularly those developed on poorly drained mineral substrates, are a key locus of elevated CH 4 emission to the atmosphere that must be considered for a complete understanding of high latitude CH 4 dynamics. (paper)

  7. Impact of agronomy practices on the effects of reduced tillage systems on CH4 and N2O emissions from agricultural fields: A global meta-analysis.

    Science.gov (United States)

    Feng, Jinfei; Li, Fengbo; Zhou, Xiyue; Xu, Chunchun; Ji, Long; Chen, Zhongdu; Fang, Fuping

    2018-01-01

    The effect of no- and reduced tillage (NT/RT) on greenhouse gas (GHG) emission was highly variable and may depend on other agronomy practices. However, how the other practices affect the effect of NT/RT on GHG emission remains elusive. Therefore, we conducted a global meta-analysis (including 49 papers with 196 comparisons) to assess the effect of five options (i.e. cropping system, crop residue management, split application of N fertilizer, irrigation, and tillage duration) on the effect of NT/RT on CH4 and N2O emissions from agricultural fields. The results showed that NT/RT significantly mitigated the overall global warming potential (GWP) of CH4 and N2O emissions by 6.6% as compared with conventional tillage (CT). Rotation cropping systems and crop straw remove facilitated no-tillage (NT) to reduce the CH4, N2O, or overall GWP both in upland and paddy field. NT significantly mitigated the overall GWP when the percentage of basal N fertilizer (PBN) >50%, when tillage duration > 10 years or rainfed in upland, while when PBN agronomy practices and land use type.

  8. Validation of farm-scale methane emissions using nocturnal boundary layer budgets

    Directory of Open Access Journals (Sweden)

    J. Stieger

    2015-12-01

    Full Text Available This study provides the first experimental validation of Swiss agricultural methane emission estimates at the farm scale. We measured CH4 concentrations at a Swiss farmstead during two intensive field campaigns in August 2011 and July 2012 to (1 quantify the source strength of livestock methane emissions using a tethered balloon system and (2 to validate inventory emission estimates via nocturnal boundary layer (NBL budgets. Field measurements were performed at a distance of 150 m from the nearest farm buildings with a tethered balloon system in combination with gradient measurements at eight heights on a 10 m tower to better resolve the near-surface concentrations. Vertical profiles of air temperature, relative humidity, CH4 concentration, wind speed, and wind direction showed that the NBL was strongly influenced by local transport processes and by the valley wind system. Methane concentrations showed a pronounced time course, with highest concentrations in the second half of the night. NBL budget flux estimates were obtained via a time–space kriging approach. Main uncertainties of NBL budget flux estimates were associated with nonstationary atmospheric conditions and the estimate of the inversion height zi (top of volume integration. The mean NBL budget fluxes of 1.60 ± 0.31 μg CH4 m-2 s-1 (1.40 ± 0.50 and 1.66 ± 0.20 μg CH4 m-2 s-1 in 2011 and 2012 respectively were in good agreement with local inventory estimates based on current livestock number and default emission factors, with 1.29 ± 0.47 and 1.74 ± 0.63 μg CH4 m-2 s-1 for 2011 and 2012 respectively. This indicates that emission factors used for the national inventory reports are adequate, and we conclude that the NBL budget approach is a useful tool to validate emission inventory estimates.

  9. Validation of farm-scale methane emissions using nocturnal boundary layer budgets

    Science.gov (United States)

    Stieger, J.; Bamberger, I.; Buchmann, N.; Eugster, W.

    2015-12-01

    This study provides the first experimental validation of Swiss agricultural methane emission estimates at the farm scale. We measured CH4 concentrations at a Swiss farmstead during two intensive field campaigns in August 2011 and July 2012 to (1) quantify the source strength of livestock methane emissions using a tethered balloon system and (2) to validate inventory emission estimates via nocturnal boundary layer (NBL) budgets. Field measurements were performed at a distance of 150 m from the nearest farm buildings with a tethered balloon system in combination with gradient measurements at eight heights on a 10 m tower to better resolve the near-surface concentrations. Vertical profiles of air temperature, relative humidity, CH4 concentration, wind speed, and wind direction showed that the NBL was strongly influenced by local transport processes and by the valley wind system. Methane concentrations showed a pronounced time course, with highest concentrations in the second half of the night. NBL budget flux estimates were obtained via a time-space kriging approach. Main uncertainties of NBL budget flux estimates were associated with nonstationary atmospheric conditions and the estimate of the inversion height zi (top of volume integration). The mean NBL budget fluxes of 1.60 ± 0.31 μg CH4 m-2 s-1 (1.40 ± 0.50 and 1.66 ± 0.20 μg CH4 m-2 s-1 in 2011 and 2012 respectively) were in good agreement with local inventory estimates based on current livestock number and default emission factors, with 1.29 ± 0.47 and 1.74 ± 0.63 μg CH4 m-2 s-1 for 2011 and 2012 respectively. This indicates that emission factors used for the national inventory reports are adequate, and we conclude that the NBL budget approach is a useful tool to validate emission inventory estimates.

  10. Eddy covariance flux measurements confirm extreme CH4 emissions from a Swiss hydropower reservoir and resolve their short-term variability

    Directory of Open Access Journals (Sweden)

    S. Sobek

    2011-09-01

    Full Text Available Greenhouse gas budgets quantified via land-surface eddy covariance (EC flux sites differ significantly from those obtained via inverse modeling. A possible reason for the discrepancy between methods may be our gap in quantitative knowledge of methane (CH4 fluxes. In this study we carried out EC flux measurements during two intensive campaigns in summer 2008 to quantify methane flux from a hydropower reservoir and link its temporal variability to environmental driving forces: water temperature and pressure changes (atmospheric and due to changes in lake level. Methane fluxes were extremely high and highly variable, but consistently showed gas efflux from the lake when the wind was approaching the EC sensors across the open water, as confirmed by floating chamber flux measurements. The average flux was 3.8 ± 0.4 μg C m−2 s−1 (mean ± SE with a median of 1.4 μg C m−2 s−1, which is quite high even compared to tropical reservoirs. Floating chamber fluxes from four selected days confirmed such high fluxes with 7.4 ± 1.3 μg C m−2 s−1. Fluxes increased exponentially with increasing temperatures, but were decreasing exponentially with increasing atmospheric and/or lake level pressure. A multiple regression using lake surface temperatures (0.1 m depth, temperature at depth (10 m deep in front of the dam, atmospheric pressure, and lake level was able to explain 35.4% of the overall variance. This best fit included each variable averaged over a 9-h moving window, plus the respective short-term residuals thereof. We estimate that an annual average of 3% of the particulate organic matter (POM input via the river is sufficient to sustain these large CH4 fluxes. To compensate the global warming potential associated with the CH4 effluxes from this hydropower reservoir a 1.3 to 3.7 times larger terrestrial area with net carbon dioxide uptake is needed if a European-scale compilation of grasslands, croplands and forests is taken as reference. This

  11. Linking rhizospheric CH4 oxidation and net CH4 emissions in an arctic wetland based on 13CH4 labeling of mesocosms

    DEFF Research Database (Denmark)

    Nielsen, Cecilie Skov; Michelsen, Anders; Ambus, Per

    2017-01-01

    Aims: Poorly drained arctic ecosystems are potential large emitters of methane (CH4) due to their high soil organic carbon content and low oxygen availability. In wetlands, aerenchymatous plants transport CH4 from the soil to the atmosphere, but concurrently transport O2 to the rhizosphere, which...... may lead to oxidation of CH4. The importance of the latter process is largely unknown for arctic plant species and ecosystems. Here, we aim to quantify the subsurface oxidation of CH4 in a waterlogged arctic ecosystem dominated by Carex aquatilis ssp. stans and Eriophorum angustifolium, and evaluate...... during three weeks after addition of 13C-enriched CH4 below the mesocosm. Results: Most of the recovered 13C label (>98 %) escaped the ecosystem as CH4, while less than 2 % was oxidized to 13CO2. Conclusions: It is concluded that aerenchymatous plants control the overall CH4 emissions but, as a transport...

  12. Quantifying the Global Fresh Water Budget: Capabilities from Current and Future Satellite Sensors

    Science.gov (United States)

    Hildebrand, Peter; Zaitchik, Benjamin

    2007-01-01

    The global water cycle is complex and its components are difficult to measure, particularly at the global scales and with the precision needed for assessing climate impacts. Recent advances in satellite observational capabilities, however, are greatly improving our knowledge of the key terms in the fresh water flux budget. Many components of the of the global water budget, e.g. precipitation, atmospheric moisture profiles, soil moisture, snow cover, sea ice are now routinely measured globally using instruments on satellites such as TRMM, AQUA, TERRA, GRACE, and ICESat, as well as on operational satellites. New techniques, many using data assimilation approaches, are providing pathways toward measuring snow water equivalent, evapotranspiration, ground water, ice mass, as well as improving the measurement quality for other components of the global water budget. This paper evaluates these current and developing satellite capabilities to observe the global fresh water budget, then looks forward to evaluate the potential for improvements that may result from future space missions as detailed by the US Decadal Survey, and operational plans. Based on these analyses, and on the goal of improved knowledge of the global fresh water budget under the effects of climate change, we suggest some priorities for the future, based on new approaches that may provide the improved measurements and the analyses needed to understand and observe the potential speed-up of the global water cycle under the effects of climate change.

  13. Inverse modelling of national and European CH4 emissions using the atmospheric zoom model TM5

    Directory of Open Access Journals (Sweden)

    P. Bergamaschi

    2005-01-01

    Full Text Available A synthesis inversion based on the atmospheric zoom model TM5 is used to derive top-down estimates of CH4 emissions from individual European countries for the year 2001. We employ a model zoom over Europe with 1° × 1° resolution that is two-way nested into the global model domain (with resolution of 6° × 4°. This approach ensures consistent boundary conditions for the zoom domain and thus European top-down estimates consistent with global CH4 observations. The TM5 model, driven by ECMWF analyses, simulates synoptic scale events at most European and global sites fairly well, and the use of high-frequency observations allows exploiting the information content of individual synoptic events. A detailed source attribution is presented for a comprehensive set of 56 monitoring sites, assigning the atmospheric signal to the emissions of individual European countries and larger global regions. The available observational data put significant constraints on emissions from different regions. Within Europe, in particular several Western European countries are well constrained. The inversion results suggest up to 50-90% higher anthropogenic CH4 emissions in 2001 for Germany, France and UK compared to reported UNFCCC values (EEA, 2003. A recent revision of the German inventory, however, resulted in an increase of reported CH4 emissions by 68.5% (EEA, 2004, being now in very good agreement with our top-down estimate. The top-down estimate for Finland is distinctly smaller than the a priori estimate, suggesting much smaller CH4 emissions from Finnish wetlands than derived from the bottom-up inventory. The EU-15 totals are relatively close to UNFCCC values (within 4-30% and appear very robust for different inversion scenarios.

  14. Expanding Spatial and Temporal Coverage of Arctic CH4 and CO2 Fluxes

    Science.gov (United States)

    Murphy, P.; Oechel, W. C.; Moreaux, V.; Losacco, S.; Zona, D.

    2013-12-01

    Carbon storage and exchange in Arctic ecosystems is the subject of intensive study focused on determining rates, controls, and mechanisms of CH4 and CO2 fluxes. The Arctic contains more than 1 Gt of Carbon in the upper meter of soil, both in the active layer and permafrost (Schuur et al., 2008; Tarnocai et al., 2009). However, the annual pattern and controls on the release of CH4 is inadequately understood in Arctic tundra ecosystems. Annual methane budgets are poorly understood, and very few studies measure fluxes through the freeze-up cycle during autumn months (Mastepanov et al., 2008; Mastepanov et al., 2010; Sturtevant et al., 2012). There is no known, relatively continuous, CH4 flux record for the Arctic. Clearly, the datasets that currently exist for budget calculations and model parameterization and verification are inadequate. This is likely due to the difficult nature of flux measurements in the Arctic. In September 2012, we initiated a research project towards continuous methane flux measurements along a latitudinal transect in Northern Alaska. The eddy-covariance (EC) technique is challenging in such extreme weather conditions due to the effects of ice formation and precipitation on instrumentation, including gas analyzers and sonic anemometers. The challenge is greater in remote areas of the Arctic, when low power availability and limited communication can lead to delays in data retrieval or data loss. For these reasons, a combination of open- and closed-path gas analyzers, and several sonic anemometers (including one with heating), have been installed on EC towers to allow for cross-comparison and cross-referencing of calculated fluxes. Newer instruments for fast CH4 flux determination include: the Los Gatos Research Fast Greenhouse Gas Analyzer and the Li-Cor LI-7700. We also included the self-heated Metek Class-A uSonic-3 Anemometer as a new instrument. Previously existing instruments used for comparison include the Li-Cor LI-7500; Li-Cor LI-7200

  15. CO2 and CH4 exchange by Phragmites australis under different climates

    Science.gov (United States)

    Serrano Ortiz, Penélope; Chojnickic, Bogdan H.; Sánchez-Cañete, Enrique P.; Kowalska, Natalia; López-Ballesteros, Ana; Fernández, Néstor; Urbaniak, Marek; Olejnik, Janusz; Kowalski, Andrew S.

    2015-04-01

    The key role of wetlands regarding global warming is the resulting balance between net CO2 assimilation, via photosynthesis, and CO2 and CH4 emissions, given the potential to release stored carbon, because of the high temperature sensitivity of heterotrophic soil respiration and anoxic conditions. However, it is still unknown whether wetlands will convert from long-term carbon sinks to sources as a result of climate change and other anthropogenic effects such as land use changes. Phragmites australis is one of the most common species found in wetlands and is considered the most globally widespread and productive plant species in this type of ecosystem. In this context, the main objective of this study is to analyse the GHG exchange (CO2 and CH4) of two wetlands with Phragmites australis as the dominant species under different climates using the eddy covariance (EC) technique. The first site, Padul, is located in southern Spain, with a sub-humid warm climate, characterised by a mean annual temperature of 16°C and annual precipitation of ca. 470 mm, with a very dry summer. The second site, Rzecin is located in Poland with a mean annual temperature of 8°C, and annual precipitation around 600mm with no dry season. The Padul EC station is equipped with two infrared gas analysers to measure CO2 and CH4 fluxes (LI-7200 and LI-7700 respectively) while the Rzecin EC station has the same CH4 sensor as Padul, but also a sensor measuring both GHG fluxes (DLT-100 Fast Methane Analyser, Los Gatos). In this study, we present: i) the results of a CH4 analyser inter-comparison campaign (LI-7700 vs. Los Gatos), ii) a comparative analysis of the functional behaviour of respiration and photosynthesis in both sites testing relationships between CO2 fluxes measured with the EC technique and meteorological variables such as temperature and direct or diffuse radiation and iii) the CH4 dynamicsat both sites by identifying, when possible, annual, seasonal and diurnal patterns.

  16. Microbial CH4 and N2O consumption in acidic wetlands

    Directory of Open Access Journals (Sweden)

    Steffen eKolb

    2012-03-01

    Full Text Available Acidic wetlands are global sources of the atmospheric greenhouse gases methane (CH4, and nitrous oxide (N2O. Consumption of both atmospheric gases has been observed in various acidic wetlands, but information on the microbial mechanisms underlying these phenomena is scarce. A substantial amount of CH4 is consumed in sub soil by aerobic methanotrophs at anoxic–oxic interfaces (e.g., tissues of Sphagnum mosses, rhizosphere of vascular plant roots. Methylocystis-related species are likely candidates that are involved in the consumption of atmospheric CH4 in acidic wetlands. Oxygen availability regulates the activity of methanotrophs of acidic wetlands. Other parameters impacting on the methanotroph-mediated CH4 consumption have not been systematically evaluated. N2O is produced and consumed by microbial denitrification, thus rendering acidic wetlands as temporary sources or sinks for N2O. Denitrifier communities in such ecosystems are diverse, and largely uncultured and/or new, and environmental factors that control their consumption activity are unresolved. Analyses of the composition of N2O reductase genes in acidic wetlands suggest that acid-tolerant Proteobacteria have the potential to mediate N2O consumption in such soils. Thus, the fragmented current state of knowledge raises open questions concerning methanotrophs and dentrifiers that consume atmospheric CH4 and N2O in acidic wetlands.

  17. Aerial photography based census of Adélie Penguin and its application in CH4 and N2O budget estimation in Victoria Land, Antarctic.

    Science.gov (United States)

    He, Hong; Cheng, Xiao; Li, Xianglan; Zhu, Renbin; Hui, Fengming; Wu, Wenhui; Zhao, Tiancheng; Kang, Jing; Tang, Jianwu

    2017-10-11

    Penguin guano provides favorable conditions for production and emission of greenhouse gases (GHGs). Many studies have been conducted to determine the GHG fluxes from penguin colonies, however, at regional scale, there is still no accurate estimation of total GHG emissions. We used object-based image analysis (OBIA) method to estimate the Adélie penguin (Pygoscelis adeliae) population based on aerial photography data. A model was developed to estimate total GHG emission potential from Adélie penguin colonies during breeding seasons in 1983 and 2012, respectively. Results indicated that OBIA method was effective for extracting penguin information from aerial photographs. There were 17,120 and 21,183 Adélie penguin breeding pairs on Inexpressible Island in 1983 and 2012, respectively, with overall accuracy of the estimation of 76.8%. The main reasons for the increase in Adélie penguin populations were attributed to increase in temperature, sea ice and phytoplankton. The average estimated CH 4 and N 2 O emissions tended to be increasing during the period from 1983 to 2012 and CH 4 was the main GHG emitted from penguin colonies. Total global warming potential (GWP) of CH 4 and N 2 O emissions was 5303 kg CO 2 -eq in 1983 and 6561 kg CO 2 -eq in 2012, respectively.

  18. The global variation of CH4 and CO as seen by SCIAMACHY

    NARCIS (Netherlands)

    Straume, A.G.; Schrijver, H.; Gloudemans, A.M.S.; Houweling, S.; Aben, I.; Maurellis, A.N.; de Laat, A.T.J.; Kleipool, Q.; Lichtenberg, G.; van Hees, R.; Meirink, J.F.; Krol, M.

    2005-01-01

    The methane (CH4) and carbon monoxide (CO) total columns retrieved from SCIAMACHY's near-infrared channel 8 have been compared to satellite measurements by the MOPITT instrument and chemistry transport model calculations (TM3). Results from the SRON retrieval algorithm IMLM (v5.1) are presented here

  19. Comparison of atmospheric CH4 concentration observed by GOSAT and in-situ measurements in Thailand and India

    Science.gov (United States)

    Hayashida, S.; Ono, A.; Ishikawa, S.; Terao, Y.; Takeuchi, W.

    2012-12-01

    The concentration of atmospheric methane (CH4) has more than doubled since pre-industrial levels and the observed long-term changes in the CH4 concentration have been attributed to anthropogenic activity. However, despite the importance of atmospheric CH4 in global warming, the strength of individual sources of CH4 remains highly uncertain [e.g.,Dlugokencky et al., 2011]. To characterize and quantify the emissions of CH4 especially in Monsoon Asia and Siberia, which are the most important regions as CH4 source, we started a new project, "Characterization and Quantification of global methane emissions by utilizing GOSAT and in-situ measurements " by support of the Environment Research and Technology Development Fund (ERTDF) from June 2012 under the umbrella of Ministry of Environment Japan. The projects includes (1) satellite data applications, (2) in-situ measurements in Siberia, over Western Pacific and in Monsoon Asia, (3) development of the inverse model to derive CH4 emissions by top-down approach, and (4) flux measurements in Siberia and Asia to improve the bottom-up inventories. As an initiatory approach in the project, we started air sampling in Thailand and India where there are only a few CH4 data of direct sampling with high precision. We took eight air samples at Kohn Kaen and Pimai in Thailand on June 9 and 10, 2012. The high CH4 concentration near rice paddy field contrasted to the lower CH4 concentration near Cassava field. We are planning to take more samples in India in mid-August. The satellite CH4 data including GOSAT and SCIAMACHY are also compared with the Land Surface Water Coverage (LSWC) and the Normalized Difference Vegetation Index (NDVI). The analysis revealed the seasonal variation in of xCH4 is closely related to the variation of the LSWC, coupled with NDVI. However, the satellite measurements are all column-averaged mixing ratio (xCH4), and therefore do not necessarily reflect high CH4 concentration near the surface over the emission

  20. U.S. Global Change Research Program Budget Crosscut

    Data.gov (United States)

    Office of Science and Technology Policy, Executive Office of the President — U.S. Global Change Research Program budget authority for Agency activities in which the primary focus is on:Observations, research, and analysis of climate change...

  1. Edge effects on N2O, NO and CH4 fluxes in two temperate forests.

    Science.gov (United States)

    Remy, Elyn; Gasche, Rainer; Kiese, Ralf; Wuyts, Karen; Verheyen, Kris; Boeckx, Pascal

    2017-01-01

    Forest ecosystems may act as sinks or sources of nitrogen (N) and carbon (C) compounds, such as the climate relevant trace gases nitrous oxide (N 2 O), nitric oxide (NO) and methane (CH 4 ). Forest edges, which catch more atmospheric deposition, have become important features in European landscapes and elsewhere. Here, we implemented a fully automated measuring system, comprising static and dynamic measuring chambers determining N 2 O, NO and CH 4 fluxes along an edge-to-interior transect in an oak (Q. robur) and a pine (P. nigra) forest in northern Belgium. Each forest was monitored during a 2-week measurement campaign with continuous measurements every 2h. NO emissions were 9-fold higher than N 2 O emissions. The fluxes of NO and CH 4 differed between forest edge and interior, but not for N 2 O. This edge effect was more pronounced in the oak than in the pine forest. In the oak forest, edges emitted less NO (on average 60%) and took up more CH 4 (on average 177%). This suggests that landscape structure can play a role in the atmospheric budgets of these climate relevant trace gases. Soil moisture variation between forest edge and interior was a key variable explaining the magnitude of NO and CH 4 fluxes in our measurement campaign. To better understand the environmental impact of N and C trace gas fluxes from forest edges, additional and long-term measurements in other forest edges are required. Copyright © 2016 Elsevier B.V. All rights reserved.

  2. [Effects of combined applications of pig manure and chemical fertilizers on CH4 and N2O emissions and their global warming potentials in paddy fields with double-rice cropping].

    Science.gov (United States)

    Wang, Cong; Shen, Jian-Lin; Zheng, Liang; Liu, Jie-Yun; Qin, Hong-Ling; Li, Yong; Wu, Jin-Shui

    2014-08-01

    A field experiment was carried out to study the effects of combined applications of pig manure and chemical fertilizers on CH4 and N2O emissions, which were measured using the static chamber/gas chromatography method, and their global warming potentials in typical paddy fields with double-rice cropping in Hunan province. The results showed that the combined applications of pig manure and chemical fertilizers did not change the seasonal patterns of CH4 and N2O emissions from paddy soils, but significantly changed the magnitudes of CH4 and N2O fluxes in rice growing seasons as compared with sole application of chemical fertilizers. During the two rice growing seasons, the cumulative CH4 emissions for the pig manure and chemical nitrogen (N) fertilizer each contributing to 50% of the total applied N (1/2N + PM) treatment were higher than those for the treatments of no N fertilizer (ON), half amount of chemical N fertilizer (1/2N) and 100% chemical N fertilizer (N) by 54.83%, 33.85% and 43.30%, respectively (P global warming potential (GWP) in both rice growing seasons, which contributed more than 99% to the integrated GWP of CH4 and N2O emissions for all the four treatments. Both GWP and yield-scaled GWP for the treatment of 1/2N + PM were significantly higher than the other three treatments. The yield-scaled GWP for the treatment of 1/2N + PM was higher than those for the N, 1/2N and ON treatments by 58.21%, 26.82% and 20. 63%, respectively. Therefore, combined applications of pig manure and chemical fertilizers in paddy fields would increase the GWP of CH4 and N2O emissions during rice growing seasons and this effect should be considered in regional greenhouse gases emissions inventory.

  3. Observing and modeling links between soil moisture, microbes and CH4 fluxes from forest soils

    Science.gov (United States)

    Christiansen, Jesper; Levy-Booth, David; Barker, Jason; Prescott, Cindy; Grayston, Sue

    2017-04-01

    community responds different to environmental change dependent on the soil moisture regime. These results are important to include in future modeling efforts to predict changes in soil-atmosphere exchange of CH4 under global change.

  4. Aviation NOx-induced CH4 effect: Fixed mixing ratio boundary conditions versus flux boundary conditions

    Science.gov (United States)

    Khodayari, Arezoo; Olsen, Seth C.; Wuebbles, Donald J.; Phoenix, Daniel B.

    2015-07-01

    Atmospheric chemistry-climate models are often used to calculate the effect of aviation NOx emissions on atmospheric ozone (O3) and methane (CH4). Due to the long (∼10 yr) atmospheric lifetime of methane, model simulations must be run for long time periods, typically for more than 40 simulation years, to reach steady-state if using CH4 emission fluxes. Because of the computational expense of such long runs, studies have traditionally used specified CH4 mixing ratio lower boundary conditions (BCs) and then applied a simple parameterization based on the change in CH4 lifetime between the control and NOx-perturbed simulations to estimate the change in CH4 concentration induced by NOx emissions. In this parameterization a feedback factor (typically a value of 1.4) is used to account for the feedback of CH4 concentrations on its lifetime. Modeling studies comparing simulations using CH4 surface fluxes and fixed mixing ratio BCs are used to examine the validity of this parameterization. The latest version of the Community Earth System Model (CESM), with the CAM5 atmospheric model, was used for this study. Aviation NOx emissions for 2006 were obtained from the AEDT (Aviation Environmental Design Tool) global commercial aircraft emissions. Results show a 31.4 ppb change in CH4 concentration when estimated using the parameterization and a 1.4 feedback factor, and a 28.9 ppb change when the concentration was directly calculated in the CH4 flux simulations. The model calculated value for CH4 feedback on its own lifetime agrees well with the 1.4 feedback factor. Systematic comparisons between the separate runs indicated that the parameterization technique overestimates the CH4 concentration by 8.6%. Therefore, it is concluded that the estimation technique is good to within ∼10% and decreases the computational requirements in our simulations by nearly a factor of 8.

  5. Annual greenhouse gas budget for a bog ecosystem undergoing restoration by rewetting

    Science.gov (United States)

    Lee, Sung-Ching; Christen, Andreas; Black, Andrew T.; Johnson, Mark S.; Jassal, Rachhpal S.; Ketler, Rick; Nesic, Zoran; Merkens, Markus

    2017-06-01

    Many peatlands have been drained and harvested for peat mining, agriculture, and other purposes, which has turned them from carbon (C) sinks into C emitters. Rewetting of disturbed peatlands facilitates their ecological recovery and may help them revert to carbon dioxide (CO2) sinks. However, rewetting may also cause substantial emissions of the more potent greenhouse gas (GHG) methane (CH4). Our knowledge of the exchange of CO2 and CH4 following rewetting during restoration of disturbed peatlands is currently limited. This study quantifies annual fluxes of CO2 and CH4 in a disturbed and rewetted area located in the Burns Bog Ecological Conservancy Area in Delta, BC, Canada. Burns Bog is recognized as the largest raised bog ecosystem on North America's west coast. Burns Bog was substantially reduced in size and degraded by peat mining and agriculture. Since 2005, the bog has been declared a conservancy area, with restoration efforts focusing on rewetting disturbed ecosystems to recover Sphagnum and suppress fires. Using the eddy covariance (EC) technique, we measured year-round (16 June 2015 to 15 June 2016) turbulent fluxes of CO2 and CH4 from a tower platform in an area rewetted for the last 8 years. The study area, dominated by sedges and Sphagnum, experienced a varying water table position that ranged between 7.7 (inundation) and -26.5 cm from the surface during the study year. The annual CO2 budget of the rewetted area was -179 ± 26.2 g CO2-C m-2 yr-1 (CO2 sink) and the annual CH4 budget was 17 ± 1.0 g CH4-C m-2 yr-1 (CH4 source). Gross ecosystem productivity (GEP) exceeded ecosystem respiration (Re) during summer months (June-August), causing a net CO2 uptake. In summer, high CH4 emissions (121 mg CH4-C m-2 day-1) were measured. In winter (December-February), while roughly equal magnitudes of GEP and Re made the study area CO2 neutral, very low CH4 emissions (9 mg CH4-C m-2 day-1) were observed. The key environmental factors controlling the seasonality of

  6. An audit of the global carbon budget: identifying and reducing sources of uncertainty

    Science.gov (United States)

    Ballantyne, A. P.; Tans, P. P.; Marland, G.; Stocker, B. D.

    2012-12-01

    Uncertainties in our carbon accounting practices may limit our ability to objectively verify emission reductions on regional scales. Furthermore uncertainties in the global C budget must be reduced to benchmark Earth System Models that incorporate carbon-climate interactions. Here we present an audit of the global C budget where we try to identify sources of uncertainty for major terms in the global C budget. The atmospheric growth rate of CO2 has increased significantly over the last 50 years, while the uncertainty in calculating the global atmospheric growth rate has been reduced from 0.4 ppm/yr to 0.2 ppm/yr (95% confidence). Although we have greatly reduced global CO2 growth rate uncertainties, there remain regions, such as the Southern Hemisphere, Tropics and Arctic, where changes in regional sources/sinks will remain difficult to detect without additional observations. Increases in fossil fuel (FF) emissions are the primary factor driving the increase in global CO2 growth rate; however, our confidence in FF emission estimates has actually gone down. Based on a comparison of multiple estimates, FF emissions have increased from 2.45 ± 0.12 PgC/yr in 1959 to 9.40 ± 0.66 PgC/yr in 2010. Major sources of increasing FF emission uncertainty are increased emissions from emerging economies, such as China and India, as well as subtle differences in accounting practices. Lastly, we evaluate emission estimates from Land Use Change (LUC). Although relative errors in emission estimates from LUC are quite high (2 sigma ~ 50%), LUC emissions have remained fairly constant in recent decades. We evaluate the three commonly used approaches to estimating LUC emissions- Bookkeeping, Satellite Imagery, and Model Simulations- to identify their main sources of error and their ability to detect net emissions from LUC.; Uncertainties in Fossil Fuel Emissions over the last 50 years.

  7. Isotopic source signatures: Impact of regional variability on the δ13CH4 trend and spatial distribution

    Science.gov (United States)

    Feinberg, Aryeh I.; Coulon, Ancelin; Stenke, Andrea; Schwietzke, Stefan; Peter, Thomas

    2018-02-01

    The atmospheric methane growth rate has fluctuated over the past three decades, signifying variations in methane sources and sinks. Methane isotopic ratios (δ13CH4) differ between emission categories, and can therefore be used to distinguish which methane sources have changed. However, isotopic modelling studies have mainly focused on uncertainties in methane emissions rather than uncertainties in isotopic source signatures. We simulated atmospheric δ13CH4 for the period 1990-2010 using the global chemistry-climate model SOCOL. Empirically-derived regional variability in the isotopic signatures was introduced in a suite of sensitivity simulations. These simulations were compared to a baseline simulation with commonly used global mean isotopic signatures. We investigated coal, natural gas/oil, wetland, livestock, and biomass burning source signatures to determine whether regional variations impact the observed isotopic trend and spatial distribution. Based on recently published source signature datasets, our calculated global mean isotopic signatures are in general lighter than the commonly used values. Trends in several isotopic signatures were also apparent during the period 1990-2010. Tropical livestock emissions grew during the 2000s, introducing isotopically heavier livestock emissions since tropical livestock consume more C4 vegetation than midlatitude livestock. Chinese coal emissions, which are isotopically heavy compared to other coals, increase during the 2000s leading to higher global values of δ13CH4 for coal emissions. EDGAR v4.2 emissions disagree with the observed atmospheric isotopic trend for almost all simulations, confirming past doubts about this emissions inventory. The agreement between the modelled and observed δ13CH4 interhemispheric differences improves when regional source signatures are used. Even though the simulated results are highly dependent on the choice of methane emission inventories, they emphasize that the commonly used

  8. Combining Microbial Enzyme Kinetics Models with Light Use Efficiency Models to Predict CO2 and CH4 Ecosystem Exchange from Flooded and Drained Peatland Systems

    Science.gov (United States)

    Oikawa, P. Y.; Jenerette, D.; Knox, S. H.; Sturtevant, C. S.; Verfaillie, J. G.; Baldocchi, D. D.

    2014-12-01

    Under California's Cap-and-Trade program, companies are looking to invest in land-use practices that will reduce greenhouse gas (GHG) emissions. The Sacramento-San Joaquin River Delta is a drained cultivated peatland system and a large source of CO2. To slow soil subsidence and reduce CO2 emissions, there is growing interest in converting drained peatlands to wetlands. However, wetlands are large sources of CH4 that could offset CO2-based GHG reductions. The goal of our research is to provide accurate measurements and model predictions of the changes in GHG budgets that occur when drained peatlands are restored to wetland conditions. We have installed a network of eddy covariance towers across multiple land use types in the Delta and have been measuring CO2 and CH4 ecosystem exchange for multiple years. In order to upscale these measurements through space and time we are using these data to parameterize and validate a process-based biogeochemical model. To predict gross primary productivity (GPP), we are using a simple light use efficiency (LUE) model which requires estimates of light, leaf area index and air temperature and can explain 90% of the observed variation in GPP in a mature wetland. To predict ecosystem respiration we have adapted the Dual Arrhenius Michaelis-Menten (DAMM) model. The LUE-DAMM model allows accurate simulation of half-hourly net ecosystem exchange (NEE) in a mature wetland (r2=0.85). We are working to expand the model to pasture, rice and alfalfa systems in the Delta. To predict methanogenesis, we again apply a modified DAMM model, using simple enzyme kinetics. However CH4 exchange is complex and we have thus expanded the model to predict not only microbial CH4 production, but also CH4 oxidation, CH4 storage and the physical processes regulating the release of CH4 to the atmosphere. The CH4-DAMM model allows accurate simulation of daily CH4 ecosystem exchange in a mature wetland (r2=0.55) and robust estimates of annual CH4 budgets. The LUE

  9. CO2 and CH4 fluxes in a Spartina salt marsh and brackish Phragmites marsh in Massachusetts

    Science.gov (United States)

    Tang, J.; Wang, F.; Kroeger, K. D.; Gonneea, M. E.

    2017-12-01

    Coastal salt marshes play an important role in global and regional carbon cycling. Tidally restricted marshes reduce salinity and provide a habitat suitable for Phragmites invasion. We measured greenhouse gas (GHG) emissions (CO2 and CH4) continuously with the eddy covariance method and biweekly with the static chamber method in a Spartina salt marsh and a Phragmites marsh on Cape Cod, Massachusetts, USA. We did not find significant difference in CO2 fluxes between the two sites, but the CH4 fluxes were much higher in the Phragmites site than the Spartina marsh. Temporally, tidal cycles influence the CO2 and CH4 fluxes in both sites. We found that the salt marsh was a significant carbon sink when CO2 and CH4 fluxes were combined. Restoring tidally restricted marshes will significantly reduce CH4 emissions and provide a strong ecosystem carbon service.

  10. Combustion's impact on the global atmosphere

    International Nuclear Information System (INIS)

    Prather, M.J.; Logan, J.A.

    1994-01-01

    The combustion of a hydrocarbon fuel removes molecular oxygen (O 2 ) from the atmosphere and releases equivalent amounts of water (H 2 ) and carbon dioxide (CO 2 ), almost always with trace amounts of numerous other compounds including hydrocarbon (CH 4 , C 2 H 2 , C 2 H 4 , C 2 H 6 , C 3 H 8 , C 6 H 6 , CH 3 CHO, etc.), carbon monoxide (CO), nitrogen oxides (NO, N 2 O) and reduced nitrogen (NH 3 and HCN), sulfur gases (SO 2 , OCS, CS 2 ), halocarbons (CH 3 Al and CH 3 Br), and particles. A review of the atmospheric budgets of these gases shows that burning of fossil fuels and recent biomass has led to global alterations in the composition of the atmosphere. Combustion is clearly responsible for most of the enhanced greenhouse forcing to date (through CO 2 , tropospheric O 3 , soot) and also some counteracting effects (through SO 2 ). It has had minimal impact on stratospheric O 3 (through CH 3 Cl, CH 3 Br, CH 4 ), but has likely changed the tropospheric oxidant levels (through CO, NO x , NMHC), at least over the northern hemisphere. Most of the important greenhouse gases and tropospheric oxidant gases have significant natural sources, which are not well defined today and may be changing; and thus, quantifying the role of combustion is difficult. 113 refs

  11. Growing season CH4 and N2O fluxes from a subarctic landscape in northern Finland; from chamber to landscape scale

    Science.gov (United States)

    Dinsmore, Kerry J.; Drewer, Julia; Levy, Peter E.; George, Charles; Lohila, Annalea; Aurela, Mika; Skiba, Ute M.

    2017-02-01

    Subarctic and boreal emissions of CH4 are important contributors to the atmospheric greenhouse gas (GHG) balance and subsequently the global radiative forcing. Whilst N2O emissions may be lower, the much greater radiative forcing they produce justifies their inclusion in GHG studies. In addition to the quantification of flux magnitude, it is essential that we understand the drivers of emissions to be able to accurately predict climate-driven changes and potential feedback mechanisms. Hence this study aims to increase our understanding of what drives fluxes of CH4 and N2O in a subarctic forest/wetland landscape during peak summer conditions and into the shoulder season, exploring both spatial and temporal variability, and uses satellite-derived spectral data to extrapolate from chamber-scale fluxes to a 2 km × 2 km landscape area.From static chamber measurements made during summer and autumn campaigns in 2012 in the Sodankylä region of northern Finland, we concluded that wetlands represent a significant source of CH4 (3.35 ± 0.44 mg C m-2 h-1 during the summer campaign and 0.62 ± 0.09 mg C m-2 h-1 during the autumn campaign), whilst the surrounding forests represent a small sink (-0.06 ± zero across both ecosystems.We found a weak negative relationship between CH4 emissions and water table depth in the wetland, with emissions decreasing as the water table approached and flooded the soil surface and a positive relationship between CH4 emissions and the presence of Sphagnum mosses. Temperature was also an important driver of CH4 with emissions increasing to a peak at approximately 12 °C. Little could be determined about the drivers of N2O emissions given the small magnitude of the fluxes.A multiple regression modelling approach was used to describe CH4 emissions based on spectral data from PLEIADES PA1 satellite imagery across a 2 km × 2 km landscape. When applied across the whole image domain we calculated a CH4 source of 2.05 ± 0.61 mg C m-2 h-1. This was

  12. Optimisation of expansion liquefaction processes using mixed refrigerant N_2–CH_4

    International Nuclear Information System (INIS)

    Ding, He; Sun, Heng; He, Ming

    2016-01-01

    Highlights: • A refrigerant composition matching method for N_2–CH_4 expansion processes. • Efficiency improvements for propane pre-cooled N_2–CH_4 expansion processes. • The process shows good adaptability to varying natural gas compositions. - Abstract: An expansion process with a pre-cooling system is simulated and optimised by Aspen HYSYS and MATLAB"™. Taking advantage of higher specific refrigeration effect of methane and easily reduced refrigeration temperature of nitrogen, the designed process adopts N_2–CH_4 as a mixed refrigerant. Based on the different thermodynamic properties and sensitivity difference of N_2 and CH_4 over the same heat transfer temperature range, this work proposes a novel method of matching refrigerant composition which aims at single-stage or multi-stage series expansion liquefaction processes with pre-cooling systems. This novel method is applied successfully in propane pre-cooled N_2–CH_4 expansion process, and the unit power consumption is reduced to 7.09 kWh/kmol, which is only 5.35% higher than the global optimised solutions obtained by genetic algorithm. This novel method can fulfil the accomplishments of low energy consumption and high liquefaction rate, and thus decreases the gap between the mixed refrigerant and expansion processes in energy consumption. Furthermore, the high exergy efficiency of the process indicates good adaptability to varying natural gas compositions.

  13. Thermodynamic and hydrochemical controls on CH4 in a coal seam gas and overlying alluvial aquifer: new insights into CH4 origins

    OpenAIRE

    Owen, D. Des. R.; Shouakar-Stash, O.; Morgenstern, U.; Aravena, R.

    2016-01-01

    Using a comprehensive data set (dissolved CH4, ?13C-CH4, ?2H-CH4, ?13C-DIC, ?37Cl, ?2H-H2O, ?18O-H2O, Na, K, Ca, Mg, HCO3, Cl, Br, SO4, NO3 and DO), in combination with a novel application of isometric log ratios, this study describes hydrochemical and thermodynamic controls on dissolved CH4 from a coal seam gas reservoir and an alluvial aquifer in the Condamine catchment, eastern Surat/north-western Clarence-Moreton basins, Australia. ?13C-CH4 data in the gas reservoir (?58? to ?49?) and sha...

  14. Rotational study of the CH4–CO complex: Millimeter-wave measurements and ab initio calculations

    International Nuclear Information System (INIS)

    Surin, L. A.; Tarabukin, I. V.; Panfilov, V. A.; Schlemmer, S.; Kalugina, Y. N.; Faure, A.; Rist, C.; Avoird, A. van der

    2015-01-01

    The rotational spectrum of the van der Waals complex CH 4 –CO has been measured with the intracavity OROTRON jet spectrometer in the frequency range of 110–145 GHz. Newly observed and assigned transitions belong to the K = 2–1 subband correlating with the rotationless j CH4 = 0 ground state and the K = 2–1 and K = 0–1 subbands correlating with the j CH4 = 2 excited state of free methane. The (approximate) quantum number K is the projection of the total angular momentum J on the intermolecular axis. The new data were analyzed together with the known millimeter-wave and microwave transitions in order to determine the molecular parameters of the CH 4 –CO complex. Accompanying ab initio calculations of the intermolecular potential energy surface (PES) of CH 4 –CO have been carried out at the explicitly correlated coupled cluster level of theory with single, double, and perturbative triple excitations [CCSD(T)-F12a] and an augmented correlation-consistent triple zeta (aVTZ) basis set. The global minimum of the five-dimensional PES corresponds to an approximately T-shaped structure with the CH 4 face closest to the CO subunit and binding energy D e = 177.82 cm −1 . The bound rovibrational levels of the CH 4 –CO complex were calculated for total angular momentum J = 0–6 on this intermolecular potential surface and compared with the experimental results. The calculated dissociation energies D 0 are 91.32, 94.46, and 104.21 cm −1 for A (j CH4 = 0), F (j CH4 = 1), and E (j CH4 = 2) nuclear spin modifications of CH 4 –CO, respectively

  15. Precise soil management as a tool to reduce CH4 and N2O emissions from agricultural soils

    NARCIS (Netherlands)

    Mosquera Losada, J.; Hol, J.M.G.; Rappoldt, C.; Dolfing, J.

    2007-01-01

    Soil compaction stimulates the emission of nitrous oxide (N2O) and methane (CH4) from agricultural soils. N2O and CH4 are potent greenhouse gases, with a global warming potential respectively 296 times and 23 times greater than CO2.. Agricultural soils are an important source of N2O. Hence there is

  16. Decadal changes in CH4 and CO2 emissions on the Alaskan North Slope

    Science.gov (United States)

    Sweeney, C.; Commane, R.; Wofsy, S.; Dlugokencky, E. J.; Karion, A.; Stone, R. S.; Chang, R.; Tans, P. P.; Wolter, S.

    2016-12-01

    Large changes in surface air temperature, sea ice cover and permafrost in the Arctic Boreal Ecosystems (ABE) are significantly impacting the critical ecosystem services and human societies that are dependent on the ABE. In order to predict the outcome of continued change in the climate system of the ABE, it is necessary to look at how past changes in climate have affected the ABE. We look at 30 years of CH4 and 42 years of CO2 observations from the NOAA Global Greenhouse Gas Reference Network site in Barrow, Alaska. By eliminating background trends and only looking at data collected when winds are blowing off the North Slope we find very little change in CH4 enhancements, but significant changes in the CO2 enhancements coming off the tundra. The bulk of both CO2 and CH4 emissions appear to be emitted well after the first snow fall on the North Slope. CO2 emissions are a strongly correlation with summer surface temperatures, while CH4 emissions appear insensitive to the large temperature changes that occurred over the measurement period. These results suggest that CO2, and not CH4 emissions, are a likely pathway for the degradation of permafrost carbon.

  17. Cold season emissions dominate the Arctic tundra methane budget

    Science.gov (United States)

    Zona, Donatella; Gioli, Beniamino; Commane, Róisín; Lindaas, Jakob; Wofsy, Steven C.; Miller, Charles E.; Dinardo, Steven J.; Dengel, Sigrid; Sweeney, Colm; Karion, Anna; Chang, Rachel Y.-W.; Henderson, John M.; Murphy, Patrick C.; Goodrich, Jordan P.; Moreaux, Virginie; Liljedahl, Anna; Watts, Jennifer D.; Kimball, John S.; Lipson, David A.; Oechel, Walter C.

    2016-01-01

    Arctic terrestrial ecosystems are major global sources of methane (CH4); hence, it is important to understand the seasonal and climatic controls on CH4 emissions from these systems. Here, we report year-round CH4 emissions from Alaskan Arctic tundra eddy flux sites and regional fluxes derived from aircraft data. We find that emissions during the cold season (September to May) account for ≥50% of the annual CH4 flux, with the highest emissions from noninundated upland tundra. A major fraction of cold season emissions occur during the "zero curtain" period, when subsurface soil temperatures are poised near 0 °C. The zero curtain may persist longer than the growing season, and CH4 emissions are enhanced when the duration is extended by a deep thawed layer as can occur with thick snow cover. Regional scale fluxes of CH4 derived from aircraft data demonstrate the large spatial extent of late season CH4 emissions. Scaled to the circumpolar Arctic, cold season fluxes from tundra total 12 ± 5 (95% confidence interval) Tg CH4 y-1, ∼25% of global emissions from extratropical wetlands, or ∼6% of total global wetland methane emissions. The dominance of late-season emissions, sensitivity to soil environmental conditions, and importance of dry tundra are not currently simulated in most global climate models. Because Arctic warming disproportionally impacts the cold season, our results suggest that higher cold-season CH4 emissions will result from observed and predicted increases in snow thickness, active layer depth, and soil temperature, representing important positive feedbacks on climate warming.

  18. Revisiting the contemporary sea-level budget on global and regional scales.

    Science.gov (United States)

    Rietbroek, Roelof; Brunnabend, Sandra-Esther; Kusche, Jürgen; Schröter, Jens; Dahle, Christoph

    2016-02-09

    Dividing the sea-level budget into contributions from ice sheets and glaciers, the water cycle, steric expansion, and crustal movement is challenging, especially on regional scales. Here, Gravity Recovery And Climate Experiment (GRACE) gravity observations and sea-level anomalies from altimetry are used in a joint inversion, ensuring a consistent decomposition of the global and regional sea-level rise budget. Over the years 2002-2014, we find a global mean steric trend of 1.38 ± 0.16 mm/y, compared with a total trend of 2.74 ± 0.58 mm/y. This is significantly larger than steric trends derived from in situ temperature/salinity profiles and models which range from 0.66 ± 0.2 to 0.94 ± 0.1 mm/y. Mass contributions from ice sheets and glaciers (1.37 ± 0.09 mm/y, accelerating with 0.03 ± 0.02 mm/y(2)) are offset by a negative hydrological component (-0.29 ± 0.26 mm/y). The combined mass rate (1.08 ± 0.3 mm/y) is smaller than previous GRACE estimates (up to 2 mm/y), but it is consistent with the sum of individual contributions (ice sheets, glaciers, and hydrology) found in literature. The altimetric sea-level budget is closed by coestimating a remaining component of 0.22 ± 0.26 mm/y. Well above average sea-level rise is found regionally near the Philippines (14.7 ± 4.39 mm/y) and Indonesia (8.3 ± 4.7 mm/y) which is dominated by steric components (11.2 ± 3.58 mm/y and 6.4 ± 3.18 mm/y, respectively). In contrast, in the central and Eastern part of the Pacific, negative steric trends (down to -2.8 ± 1.53 mm/y) are detected. Significant regional components are found, up to 5.3 ± 2.6 mm/y in the northwest Atlantic, which are likely due to ocean bottom pressure variations.

  19. Consistent regional fluxes of CH4 and CO2 inferred from GOSAT proxy XCH4 : XCO2 retrievals, 2010-2014

    Science.gov (United States)

    Feng, Liang; Palmer, Paul I.; Bösch, Hartmut; Parker, Robert J.; Webb, Alex J.; Correia, Caio S. C.; Deutscher, Nicholas M.; Domingues, Lucas G.; Feist, Dietrich G.; Gatti, Luciana V.; Gloor, Emanuel; Hase, Frank; Kivi, Rigel; Liu, Yi; Miller, John B.; Morino, Isamu; Sussmann, Ralf; Strong, Kimberly; Uchino, Osamu; Wang, Jing; Zahn, Andreas

    2017-04-01

    We use the GEOS-Chem global 3-D model of atmospheric chemistry and transport and an ensemble Kalman filter to simultaneously infer regional fluxes of methane (CH4) and carbon dioxide (CO2) directly from GOSAT retrievals of XCH4 : XCO2, using sparse ground-based CH4 and CO2 mole fraction data to anchor the ratio. This work builds on the previously reported theory that takes into account that (1) these ratios are less prone to systematic error than either the full-physics data products or the proxy CH4 data products; and (2) the resulting CH4 and CO2 fluxes are self-consistent. We show that a posteriori fluxes inferred from the GOSAT data generally outperform the fluxes inferred only from in situ data, as expected. GOSAT CH4 and CO2 fluxes are consistent with global growth rates for CO2 and CH4 reported by NOAA and have a range of independent data including new profile measurements (0-7 km) over the Amazon Basin that were collected specifically to help validate GOSAT over this geographical region. We find that large-scale multi-year annual a posteriori CO2 fluxes inferred from GOSAT data are similar to those inferred from the in situ surface data but with smaller uncertainties, particularly over the tropics. GOSAT data are consistent with smaller peak-to-peak seasonal amplitudes of CO2 than either the a priori or in situ inversion, particularly over the tropics and the southern extratropics. Over the northern extratropics, GOSAT data show larger uptake than the a priori but less than the in situ inversion, resulting in small net emissions over the year. We also find evidence that the carbon balance of tropical South America was perturbed following the droughts of 2010 and 2012 with net annual fluxes not returning to an approximate annual balance until 2013. In contrast, GOSAT data significantly changed the a priori spatial distribution of CH4 emission with a 40 % increase over tropical South America and tropical Asia and a smaller decrease over Eurasia and temperate

  20. Methane feedbacks to the global climate system in a warmer world

    NARCIS (Netherlands)

    Dean, Joshua F.; Middelburg, Jack J.; Röckmann, Thomas; Aerts, Rien; Blauw, Luke G.; Egger, Matthias; Jetten, Mike S.M.; de Jong, Anniek E.E.; Meisel, Ove H.; Rasigraf, Olivia; Slomp, Caroline P.; in't Zandt, Michiel H.; Dolman, A. J.

    Methane (CH4) is produced in many natural systems that are vulnerable to change under a warming climate, yet current CH4 budgets, as well as future shifts in CH4 emissions, have high uncertainties. Climate change has the potential to increase CH4 emissions from critical systems such as wetlands,

  1. CH{sub 4} and N{sub 2}O emissions from China’s beef feedlots with ad libitum and restricted feeding in fall and spring seasons

    Energy Technology Data Exchange (ETDEWEB)

    Lin, Zhi; Liao, Wenhua; Yang, Yuanyuan [College of Resources and Environmental Sciences, Agricultural University of Hebei, 071000 Baoding (China); Gao, Zhiling, E-mail: zhilinggao@hotmail.com [College of Resources and Environmental Sciences, Agricultural University of Hebei, 071000 Baoding (China); Ma, Wenqi; Wang, Dianwu [College of Resources and Environmental Sciences, Agricultural University of Hebei, 071000 Baoding (China); Cao, Yufeng; Li, Jianguo [College of Animal Science and Technology, Agricultural University of Hebei, 071000 Baoding (China); Cai, Zhenjiang [Mechanical and Electric Engineering College, Agricultural University of Hebei, 071000 Baoding (China)

    2015-04-15

    Accurately quantifying methane (CH{sub 4}) and nitrous oxide (N{sub 2}O) emissions from beef operations in China is necessary to evaluate the contribution of beef cattle to greenhouse gas budgets at the national and global level. Methane and N{sub 2}O emissions from two intensive beef feedlots in the North China Plain, one with a restricted feeding strategy and high manure collection frequency and the other with an ad libitum feeding strategy and low manure collection frequency, were quantified in the fall and spring seasons using an inverse dispersion technique. The diel pattern of CH{sub 4} from the beef feedlot with an ad libitum feed strategy (single peak during a day) differed from that under a restricted feeding condition (multiple peaks during a day), but little difference in the diel pattern of N{sub 2}O emissions between two feeding strategies was observed. The two-season average CH{sub 4} emission rates of the two intensive feedlots were 230 and 198 g CH{sub 4} animal{sup −1} d{sup −1} and accounted for 6.7% and 6.8% of the gross energy intake, respectively, indicating little impact of the feeding strategy and manure collection frequency on the CH{sub 4} conversion factor at the feedlot level. However, the average N{sub 2}O emission rates (21.2 g N{sub 2}O animal{sup −1} d{sup −1}) and conversion factor (8.5%) of the feedlot with low manure collection frequency were approximately 131% and 174% greater, respectively, than the feedlot under high frequency conditions, which had a N{sub 2}O emission rate and conversion factor of 9.2 g N{sub 2}O animal{sup −1} d{sup −1} and 3.1%, respectively, indicating that increasing manure collection frequency played an important role in reducing N{sub 2}O emissions from beef feedlots. In addition, comparison indicated that China’s beef and dairy cattle in feedlots appeared to have similar CH{sub 4} conversion factors. - Highlights: • CH{sub 4} and N{sub 2}O emissions from China’s beef feedlots were

  2. Distribution of dissolved green-house gases (CO2, CH4, N2O) in Lakes Edward and George: Results from the first field cruise of the HIPE project

    Science.gov (United States)

    Borges, Alberto V.; Morana, Cédric D. T.; Lambert, Thibault; Okello, William; Bouillon, Steven

    2017-04-01

    Inland waters (streams, rivers, lakes, reservoirs) are quantitatively important components of the global budgets of atmospheric emissions of long-lived greenhouse gases (GHGs) (CO2, CH4, N2O). Available data indicate that a very large fraction of CO2 and CH4 emissions from rivers and reservoirs occurs at tropical latitudes. Data on GHGs at tropical latitudes from lakes however are much more scarse, and the relative importance of emissions, in particular in Africa, remains to be determined. Large tropical lakes are net autotrophic (hence potentially sinks for atmospheric CO2) due generally low dissolved organic carbon concentrations, seasonally near constant light and temperature conditions, and generally deep water columns favourable for export of organic matter to depth. This sharply contrasts with their much better documented temperate and boreal counterparts, usually considered as CO2 sources to the atmosphere sustained by net heterotrophy. Here, we report a data-set of dissolved CO2, CH4, N2O obtained in October 2016 in Lakes Edward and George and adjacent streams and crater lakes in the frame of Belgian Science Policy (BELSPO) HIPE (Human impacts on ecosystem health and resources of Lake Edward, http://www.co2.ulg.ac.be/hipe/) project. Lake George and part of Lake Edward were sinks for atmospheric CO2 and N2O due to high primary production and denitrification in sediments, respectively, and modest sources of CH4 to the atmosphere. Sampled rivers and streams were oversaturated in CO2 and CH4 and close to atmospheric equilibrium with regards to N2O. Spatial variations within rivers and streams were related to elevation and vegetation characteristics on the catchments (savannah versus forest). Levels of CO2, CH4, and N2O were within the range of those we reported in other African rivers. Crater lakes acted as sinks for atmospheric CO2 and N2O but were extremely over-saturated in CH4, due to intense primary production sustained by cyanobacteria. These CH4 levels

  3. The Drivers of the CH4 Seasonal Cycle in the Arctic and What Long-Term Observations of CH4 Imply About Trends in Arctic CH4 Fluxes

    Science.gov (United States)

    Sweeney, C.; Karion, A.; Bruhwiler, L.; Miller, J. B.; Wofsy, S. C.; Miller, C. E.; Chang, R. Y.; Dlugokencky, E. J.; Daube, B.; Pittman, J. V.; Dinardo, S. J.

    2012-12-01

    The large seasonal change in the atmospheric column for CH4 in the Arctic is driven by two dominant processes: transport of CH4 from low latitudes and surface emissions throughout the Arctic region. The NOAA ESRL Carbon Cycle Group Aircraft Program along with the NASA funded Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) have initiated an effort to better understand the factors controlling the seasonal changes in the mole fraction of CH4 in the Arctic with a multi-scale aircraft observing network in Alaska. The backbone of this network is multi-species flask sampling from 500 to 8000 masl that has been conducted every two weeks for the last 10 years over Poker Flat, AK. In addition regular profiles at the interior Alaska site at Poker Flat, NOAA has teamed up with the United States Coast Guard to make profiling flights with continuous observations of CO2, CO, CH4 and Ozone between Kodiak and Barrow every 2 weeks. More recently, CARVE has significantly added to this observational network with targeted flights focused on exploring the variability of CO2, CH4 and CO in the boundary layer both in the interior and the North Slope regions of Alaska. Taken together with the profiling of HIAPER Pole-to-Pole Observations (HIPPO), ground sites at Barrow and a new CARVE interior Alaska surface site just north of Fairbanks, AK, we now have the ability to investigate the full evolution of the seasonal cycle in the Arctic using both the multi-scale sampling offered by the different aircraft platforms as well as the multi-species sampling offered by in-situ and flask sampling. The flasks also provide a valuable tie-point between different platforms so that spatial and temporal gradients can be properly interpreted. In the context of the seasonal cycle observed by the aircraft platforms we will look at long term ground observations over the last 20 years to assess changes in Arctic CH4 emissions which have occurred as a result of 0.6C/decade changes in mean surface

  4. Does a global budget superimposed on fee-for-service payments mitigate hospitals' medical claims in Taiwan?

    Science.gov (United States)

    Hsu, Pi-Fem

    2014-12-01

    Taiwan's global budgeting for hospital health care, in comparison to other countries, assigns a regional budget cap for hospitals' medical benefits claimed on the basis of fee-for-service (FFS) payments. This study uses a stays-hospitals-years database comprising acute myocardial infarction inpatients to examine whether the reimbursement policy mitigates the medical benefits claimed to a third-payer party during 2000-2008. The estimated results of a nested random-effects model showed that hospitals attempted to increase their medical benefit claims under the influence of initial implementation of global budgeting. The magnitudes of hospitals' responses to global budgeting were significantly attributed to hospital ownership, accreditation status, and market competitiveness of a region. The results imply that the regional budget cap superimposed on FFS payments provides only blunt incentive to the hospitals to cooperate to contain medical resource utilization, unless a monitoring mechanism attached with the payment system.

  5. Mapping pan-Arctic CH4 emissions using an adjoint method by integrating process-based wetland and lake biogeochemical models and atmospheric CH4 concentrations

    Science.gov (United States)

    Tan, Z.; Zhuang, Q.; Henze, D. K.; Frankenberg, C.; Dlugokencky, E. J.; Sweeney, C.; Turner, A. J.

    2015-12-01

    Understanding CH4 emissions from wetlands and lakes are critical for the estimation of Arctic carbon balance under fast warming climatic conditions. To date, our knowledge about these two CH4 sources is almost solely built on the upscaling of discontinuous measurements in limited areas to the whole region. Many studies indicated that, the controls of CH4 emissions from wetlands and lakes including soil moisture, lake morphology and substrate content and quality are notoriously heterogeneous, thus the accuracy of those simple estimates could be questionable. Here we apply a high spatial resolution atmospheric inverse model (nested-grid GEOS-Chem Adjoint) over the Arctic by integrating SCIAMACHY and NOAA/ESRL CH4 measurements to constrain the CH4 emissions estimated with process-based wetland and lake biogeochemical models. Our modeling experiments using different wetland CH4 emission schemes and satellite and surface measurements show that the total amount of CH4 emitted from the Arctic wetlands is well constrained, but the spatial distribution of CH4 emissions is sensitive to priors. For CH4 emissions from lakes, our high-resolution inversion shows that the models overestimate CH4 emissions in Alaskan costal lowlands and East Siberian lowlands. Our study also indicates that the precision and coverage of measurements need to be improved to achieve more accurate high-resolution estimates.

  6. Raman spectroscopy measurement of CH4 gas and CH4 dissolved in water for laser remote sensing in water

    Science.gov (United States)

    Somekawa, Toshihiro; Fujita, Masayuki

    2018-04-01

    We examined the applicability of Raman spectroscopy as a laser remote sensing tool for monitoring CH4 in water. The Raman technique has already been used successfully for measurements of CO2 gas in water. In this paper, considering the spectral transmittance of water, third harmonics of Q-switched Nd:YAG laser at 355 nm (UV region) was used for detection of CH4 Raman signals. The Raman signal at 2892 cm-1 from CH4 dissolved in water was detected at a tail of water Raman signal.

  7. Annual methane budgets of sheep grazing systems were regulated by grazing intensities in the temperate continental steppe: A two-year case study

    Science.gov (United States)

    Ma, Lei; Zhong, Mengying; Zhu, Yuhao; Yang, Helong; Johnson, Douglas A.; Rong, Yuping

    2018-02-01

    Methane (CH4) emission from animal husbandry accounts for a large percentage of anthropogenic contributions to CH4 emissions. Fully understanding of grazing management effects on the CH4 budget is essential for mitigating CH4 emissions in the temperate grazing steppe systems. Annual CH4 budgets for the sheep grazed steppes at various grazing intensities, un-grazing (UG, 0 sheep ha-1year-1), defer grazing (DG, 1.0 sheep ha-1 year-1), moderate grazing (MG, 1.43 sheep ha-1year-1), and heavy grazing (HG, 2.43 sheep ha-1year-1) were assessed across 2012-2014 in the agro-pastoral region of northern China. Annual soil CH4 uptake averaged across 2012-2014 were 1.1 ± 0.1, 2.4 ± 0.2, 2.2 ± 0.2, and 1.3 ± 0.1 kg CH4-C ha-1 for UG, DG (only 2013-2014), MG and HG sites. Non-growing season CH4 uptake comprised 50.0 ± 4.3% of annual CH4 uptake in 2012-2013 and 37.7 ± 2.0% in 2013-2014. DG and MG significantly promoted annual soil CH4 uptake (P 0.05). Bell-shaped relationship was presented between stocking rates and soil CH4 uptake (r2 = 0.59, P budgets for the grazed grasslands were -1.1 ± 0.1, 5.7 ± 0.6, 11.5 ± 1.5 and 15.5 ± 1.3 kg CH4-C ha-1 year-1 in UG, DG (only 2013-2014), MG and HG across 2012-2014. Soil CH4 uptake could offset 29.7 ± 5.6, 15.9 ± 4.3 and 6.8 ± 1.0% of total annual CH4 emissions from sheep, sheepfold and faeces in DG, MG, and HG. All grazed steppes are sources for atmospheric CH4 and the magnitude is regulated by grazing intensities. Sheep CH4 emissions for 1-g liveweight gain were 0.21, 0.32 and 0.37 g CH4-C in DG, MG and HG, respectively. DG is the recommended grazing management in this region to achieve greater herbage mass, higher sheep performance and lower CH4 emissions simultaneously.

  8. On the methane paradox: Transport from shallow water zones rather than in situ methanogenesis is the major source of CH4 in the open surface water of lakes

    Science.gov (United States)

    Encinas Fernández, Jorge; Peeters, Frank; Hofmann, Hilmar

    2016-10-01

    Estimates of global methane (CH4) emissions from lakes and the contributions of different pathways are currently under debate. In situ methanogenesis linked to algae growth was recently suggested to be the major source of CH4 fluxes from aquatic systems. However, based on our very large data set on CH4 distributions within lakes, we demonstrate here that methane-enriched water from shallow water zones is the most likely source of the basin-wide mean CH4 concentrations in the surface water of lakes. Consistently, the mean surface CH4 concentrations are significantly correlated with the ratio between the surface area of the shallow water zone and the entire lake, fA,s/t, but not with the total surface area. The categorization of CH4 fluxes according to fA,s/t may therefore improve global estimates of CH4 emissions from lakes. Furthermore, CH4 concentrations increase substantially with water temperature, indicating that seasonally resolved data are required to accurately estimate annual CH4 emissions.

  9. Estimating regional-scale methane flux and budgets using CARVE aircraft measurements over Alaska

    Directory of Open Access Journals (Sweden)

    S. Hartery

    2018-01-01

    Full Text Available Methane (CH4 is the second most important greenhouse gas but its emissions from northern regions are still poorly constrained. In this study, we analyze a subset of in situ CH4 aircraft observations made over Alaska during the growing seasons of 2012–2014 as part of the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE. Net surface CH4 fluxes are estimated using a Lagrangian particle dispersion model which quantitatively links surface emissions from Alaska and the western Yukon with observations of enhanced CH4 in the mixed layer. We estimate that between May and September, net CH4 emissions from the region of interest were 2.2 ± 0.5 Tg, 1.9 ± 0.4 Tg, and 2.3 ± 0.6 Tg of CH4 for 2012, 2013, and 2014, respectively. If emissions are only attributed to two biogenic eco-regions within our domain, then tundra regions were the predominant source, accounting for over half of the overall budget despite only representing 18 % of the total surface area. Boreal regions, which cover a large part of the study region, accounted for the remainder of the emissions. Simple multiple linear regression analysis revealed that, overall, CH4 fluxes were largely driven by soil temperature and elevation. In regions specifically dominated by wetlands, soil temperature and moisture at 10 cm depth were important explanatory variables while in regions that were not wetlands, soil temperature and moisture at 40 cm depth were more important, suggesting deeper methanogenesis in drier soils. Although similar environmental drivers have been found in the past to control CH4 emissions at local scales, this study shows that they can be used to generate a statistical model to estimate the regional-scale net CH4 budget.

  10. Estimating regional-scale methane flux and budgets using CARVE aircraft measurements over Alaska

    Science.gov (United States)

    Hartery, Sean; Commane, Róisín; Lindaas, Jakob; Sweeney, Colm; Henderson, John; Mountain, Marikate; Steiner, Nicholas; McDonald, Kyle; Dinardo, Steven J.; Miller, Charles E.; Wofsy, Steven C.; Chang, Rachel Y.-W.

    2018-01-01

    Methane (CH4) is the second most important greenhouse gas but its emissions from northern regions are still poorly constrained. In this study, we analyze a subset of in situ CH4 aircraft observations made over Alaska during the growing seasons of 2012-2014 as part of the Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE). Net surface CH4 fluxes are estimated using a Lagrangian particle dispersion model which quantitatively links surface emissions from Alaska and the western Yukon with observations of enhanced CH4 in the mixed layer. We estimate that between May and September, net CH4 emissions from the region of interest were 2.2 ± 0.5 Tg, 1.9 ± 0.4 Tg, and 2.3 ± 0.6 Tg of CH4 for 2012, 2013, and 2014, respectively. If emissions are only attributed to two biogenic eco-regions within our domain, then tundra regions were the predominant source, accounting for over half of the overall budget despite only representing 18 % of the total surface area. Boreal regions, which cover a large part of the study region, accounted for the remainder of the emissions. Simple multiple linear regression analysis revealed that, overall, CH4 fluxes were largely driven by soil temperature and elevation. In regions specifically dominated by wetlands, soil temperature and moisture at 10 cm depth were important explanatory variables while in regions that were not wetlands, soil temperature and moisture at 40 cm depth were more important, suggesting deeper methanogenesis in drier soils. Although similar environmental drivers have been found in the past to control CH4 emissions at local scales, this study shows that they can be used to generate a statistical model to estimate the regional-scale net CH4 budget.

  11. Global Tree Cover and Biomass Carbon on Agricultural Land: The contribution of agroforestry to global and national carbon budgets.

    Science.gov (United States)

    Zomer, Robert J; Neufeldt, Henry; Xu, Jianchu; Ahrends, Antje; Bossio, Deborah; Trabucco, Antonio; van Noordwijk, Meine; Wang, Mingcheng

    2016-07-20

    Agroforestry systems and tree cover on agricultural land make an important contribution to climate change mitigation, but are not systematically accounted for in either global carbon budgets or national carbon accounting. This paper assesses the role of trees on agricultural land and their significance for carbon sequestration at a global level, along with recent change trends. Remote sensing data show that in 2010, 43% of all agricultural land globally had at least 10% tree cover and that this has increased by 2% over the previous ten years. Combining geographically and bioclimatically stratified Intergovernmental Panel on Climate Change (IPCC) Tier 1 default estimates of carbon storage with this tree cover analysis, we estimated 45.3 PgC on agricultural land globally, with trees contributing >75%. Between 2000 and 2010 tree cover increased by 3.7%, resulting in an increase of >2 PgC (or 4.6%) of biomass carbon. On average, globally, biomass carbon increased from 20.4 to 21.4 tC ha(-1). Regional and country-level variation in stocks and trends were mapped and tabulated globally, and for all countries. Brazil, Indonesia, China and India had the largest increases in biomass carbon stored on agricultural land, while Argentina, Myanmar, and Sierra Leone had the largest decreases.

  12. Annual greenhouse gas budget for a bog ecosystem undergoing restoration by rewetting

    Directory of Open Access Journals (Sweden)

    S.-C. Lee

    2017-06-01

    Full Text Available Many peatlands have been drained and harvested for peat mining, agriculture, and other purposes, which has turned them from carbon (C sinks into C emitters. Rewetting of disturbed peatlands facilitates their ecological recovery and may help them revert to carbon dioxide (CO2 sinks. However, rewetting may also cause substantial emissions of the more potent greenhouse gas (GHG methane (CH4. Our knowledge of the exchange of CO2 and CH4 following rewetting during restoration of disturbed peatlands is currently limited. This study quantifies annual fluxes of CO2 and CH4 in a disturbed and rewetted area located in the Burns Bog Ecological Conservancy Area in Delta, BC, Canada. Burns Bog is recognized as the largest raised bog ecosystem on North America's west coast. Burns Bog was substantially reduced in size and degraded by peat mining and agriculture. Since 2005, the bog has been declared a conservancy area, with restoration efforts focusing on rewetting disturbed ecosystems to recover Sphagnum and suppress fires. Using the eddy covariance (EC technique, we measured year-round (16 June 2015 to 15 June 2016 turbulent fluxes of CO2 and CH4 from a tower platform in an area rewetted for the last 8 years. The study area, dominated by sedges and Sphagnum, experienced a varying water table position that ranged between 7.7 (inundation and −26.5 cm from the surface during the study year. The annual CO2 budget of the rewetted area was −179 ± 26.2 g CO2–C m−2 yr−1 (CO2 sink and the annual CH4 budget was 17 ± 1.0 g CH4–C m−2 yr−1 (CH4 source. Gross ecosystem productivity (GEP exceeded ecosystem respiration (Re during summer months (June–August, causing a net CO2 uptake. In summer, high CH4 emissions (121 mg CH4–C m−2 day−1 were measured. In winter (December–February, while roughly equal magnitudes of GEP and Re made the study area CO2 neutral, very low CH4 emissions (9 mg CH4–C m−2

  13. Tidal variability of CO2 and CH4 emissions from the water column within a Rhizophora mangrove forest (New Caledonia).

    Science.gov (United States)

    Jacotot, Adrien; Marchand, Cyril; Allenbach, Michel

    2018-08-01

    We performed a preliminary study to quantify CO 2 and CH 4 emissions from the water column within a Rhizophora spp. mangrove forest. Mean CO 2 and CH 4 emissions during the studied period were 3.35±3.62mmolCm -2 h -1 and 18.30±27.72μmolCm -2 h -1 , respectively. CO 2 and CH 4 emissions were highly variable and mainly driven by tides (flow/ebb, water column thickness, neap/spring). Indeed, an inverse relationship between the magnitude of the emissions and the thickness of the water column above the mangrove soil was observed. δ 13 CO 2 values ranged from -26.88‰ to -8.6‰, suggesting a mixing between CO 2 -enriched pore waters and lagoon incoming waters. In addition, CO 2 and CH 4 emissions were significantly higher during ebb tides, mainly due to the progressive enrichment of the water column by diffusive fluxes as its residence time over the forest floor increased. Eventually, we observed higher CO 2 and CH 4 emissions during spring tides than during neap tides, combined to depleted δ 13 CO 2 values, suggesting a higher contribution of soil-produced gases to the emissions. These higher emissions may result from higher renewable of the electron acceptor and enhanced exchange surface between the soil and the water column. This study shows that CO 2 and CH 4 emissions from the water column were not negligible and must be considered in future carbon budgets in mangroves. Copyright © 2018 Elsevier B.V. All rights reserved.

  14. On the use of satellite-derived CH4 : CO2 columns in a joint inversion of CH4 and CO2 fluxes

    NARCIS (Netherlands)

    Pandey, S.

    2015-01-01

    We present a method for assimilating total column CH4 : CO2 ratio measurements from satellites for inverse modeling of CH4 and CO2 fluxes using the variational approach. Unlike conventional approaches, in which retrieved CH4 : CO2 are multiplied by model-derived total column CO2 and only the

  15. δ13C-CH4 in ice core samples

    DEFF Research Database (Denmark)

    Sperlich, Peter

    Ice core records of δ13C-CH4 reflect the variability of CH4 biogeochemistry in response to climate change and show this system is far more complex than expected. The first part of this work is concerned with the development of analytical techniques that allow 1) precise referencing and 2) measure......Ice core records of δ13C-CH4 reflect the variability of CH4 biogeochemistry in response to climate change and show this system is far more complex than expected. The first part of this work is concerned with the development of analytical techniques that allow 1) precise referencing and 2......) measurements of δ13C-CH4 in ice core samples as is required when δ13C-CH4 records that are measured in several laboratories are merged for analysis. Both the referencing and measurement techniques have been compared to further laboratories which proofed the accuracy of the analytical systems. The second part...

  16. Effects of the conversion of cropland to forest on the CH4 oxidation capacity in soils.

    Science.gov (United States)

    Bárcena, Teresa G.; D'Imperio, Ludovica; Priemé, Anders; Gundersen, Per; Vesterdal, Lars; Christiansen, Jesper R.

    2013-04-01

    As the second most important greenhouse gas (GHG) in the atmosphere, methane (CH4) plays a central role in global warming. Diverse types of soil have been reported as potential CH4 sinks due to the activity of methane oxidizing bacteria (MOB), underlining the importance of this functional group of microorganisms on a global basis. Agricultural practices are known to negatively affect CH4 oxidation in soil, while afforestation of former agricultural soils has been shown to enhance CH4 oxidation over time. However, knowledge is scarce with regard to the mechanisms driving the process of CH4 oxidation in different land uses. Our aim was to study the changes in CH4 uptake capacity in soils along a land-use change gradient from cropland to forest. We performed an incubation experiment to study the CH4 oxidation capacity of the top mineral soil (0-5 cm and 5-15 cm depth) for sites representing the transition from agriculture to afforestation based on monoculture of three tree species with different stand ages: pedunculate oak (4, 19, 42 and >200 years old), European larch (22 and 41 years old) and Norway spruce (15 and 43 years old). Main soil parameters were also measured to determine differences in soil properties between sites. Methane oxidation rates were related to the abundance of the soil methanotrophic community based on quantitative PCR (qPCR). In addition, we also estimated the abundance of ammonia-oxidizing bacteria (AOB) and archaea (AOA), in order to investigate the link between these two similar functional groups. Although present, the abundance of AOB was under detection limit. The effects and interactions among all measured variables were summarized by Principal Component Analysis (PCA). Along the gradient, CH4 oxidation increased with increasing stand age in both soil layers (ranging from 0-1.3 nmol g-1dw d-1). However, we detected significant differences, in particular between oak and spruce, suggesting a possible tree species effect on the CH4

  17. The nitrogen, carbon and greenhouse gas budget of a grazed, cut and fertilised temperate grassland

    Science.gov (United States)

    Jones, Stephanie K.; Helfter, Carole; Anderson, Margaret; Coyle, Mhairi; Campbell, Claire; Famulari, Daniela; Di Marco, Chiara; van Dijk, Netty; Sim Tang, Y.; Topp, Cairistiona F. E.; Kiese, Ralf; Kindler, Reimo; Siemens, Jan; Schrumpf, Marion; Kaiser, Klaus; Nemitz, Eiko; Levy, Peter E.; Rees, Robert M.; Sutton, Mark A.; Skiba, Ute M.

    2017-04-01

    Intensively managed grazed grasslands in temperate climates are globally important environments for the exchange of the greenhouse gases (GHGs) carbon dioxide (CO2), nitrous oxide (N2O) and methane (CH4). We assessed the N and C budget of a mostly grazed and occasionally cut and fertilised grassland in SE Scotland by measuring or modelling all relevant imports and exports to the field as well as changes in soil C and N stocks over time. The N budget was dominated by import from inorganic and organic fertilisers (21.9 g N m-2 a-1) and losses from leaching (5.3 g N m-2 a-1), N2 emissions (2.9 g N m-2 a-1), and NOx and NH3 volatilisation (3.9 g N m-2 a-1), while N2O emission was only 0.6 g N m-2 a-1. The efficiency of N use by animal products (meat and wool) averaged 9.9 % of total N input over only-grazed years (2004-2010). On average over 9 years (2002-2010), the balance of N fluxes suggested that 6.0 ± 5.9 g N m-2 a-1 (mean ± confidence interval at p > 0.95) were stored in the soil. The largest component of the C budget was the net ecosystem exchange of CO2 (NEE), at an average uptake rate of 218 ± 155 g C m-2 a-1 over the 9 years. This sink strength was offset by carbon export from the field mainly as grass offtake for silage (48.9 g C m-2 a-1) and leaching (16.4 g C m-2 a-1). The other export terms, CH4 emissions from the soil, manure applications and enteric fermentation, were negligible and only contributed to 0.02-4.2 % of the total C losses. Only a small fraction of C was incorporated into the body of the grazing animals. Inclusion of these C losses in the budget resulted in a C sink strength of 163 ± 140 g C m-2 a-1. By contrast, soil stock measurements taken in May 2004 and May 2011 indicated that the grassland sequestered N in the 0-60 cm soil layer at 4.51 ± 2.64 g N m-2 a-1 and lost C at a rate of 29.08 ± 38.19 g C m-2 a-1. Potential reasons for the discrepancy between these estimates are probably an underestimation of C losses, especially from

  18. A Climate Data Record (CDR) for the global terrestrial water budget: 1984-2010

    Science.gov (United States)

    Zhang, Yu; Pan, Ming; Sheffield, Justin; Siemann, Amanda L.; Fisher, Colby K.; Liang, Miaoling; Beck, Hylke E.; Wanders, Niko; MacCracken, Rosalyn F.; Houser, Paul R.; Zhou, Tian; Lettenmaier, Dennis P.; Pinker, Rachel T.; Bytheway, Janice; Kummerow, Christian D.; Wood, Eric F.

    2018-01-01

    Closing the terrestrial water budget is necessary to provide consistent estimates of budget components for understanding water resources and changes over time. Given the lack of in situ observations of budget components at anything but local scale, merging information from multiple data sources (e.g., in situ observation, satellite remote sensing, land surface model, and reanalysis) through data assimilation techniques that optimize the estimation of fluxes is a promising approach. Conditioned on the current limited data availability, a systematic method is developed to optimally combine multiple available data sources for precipitation (P), evapotranspiration (ET), runoff (R), and the total water storage change (TWSC) at 0.5° spatial resolution globally and to obtain water budget closure (i.e., to enforce P - ET - R - TWSC = 0) through a constrained Kalman filter (CKF) data assimilation technique under the assumption that the deviation from the ensemble mean of all data sources for the same budget variable is used as a proxy of the uncertainty in individual water budget variables. The resulting long-term (1984-2010), monthly 0.5° resolution global terrestrial water cycle Climate Data Record (CDR) data set is developed under the auspices of the National Aeronautics and Space Administration (NASA) Earth System Data Records (ESDRs) program. This data set serves to bridge the gap between sparsely gauged regions and the regions with sufficient in situ observations in investigating the temporal and spatial variability in the terrestrial hydrology at multiple scales. The CDR created in this study is validated against in situ measurements like river discharge from the Global Runoff Data Centre (GRDC) and the United States Geological Survey (USGS), and ET from FLUXNET. The data set is shown to be reliable and can serve the scientific community in understanding historical climate variability in water cycle fluxes and stores, benchmarking the current climate, and

  19. Molecular Simulations and Theoretical Predictions for Adsorption and Diffusion of CH{sub 4}/H{sub 2} and CO{sub 2}/CH{sub 4} Mixtures in ZIFs

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Jinchen; Keskin, Seda; Sholl, David S; Johnson, J. Karl

    2011-05-01

    Adsorption and diffusion of CO{sub 2}/CH{sub 4} and CH{sub 4}/H{sub 2} mixtures were computed in zeolite imidazolate frameworks (ZIFs), ZIF-68 and ZIF-70, using atomically detailed simulations. Adsorption selectivity, diffusion selectivity, and membrane selectivity of ZIFs were calculated based on the results of atomistic simulations. Mixture adsorption isotherms predicted by the ideal adsorbed solution theory agree well with the results of molecular simulations for both ZIFs. Mixture diffusivity calculations indicate that diffusion of CH{sub 4} is increased with increasing concentration of H{sub 2} in the CH{sub 4}/H{sub 2} mixture, while the diffusivity of H{sub 2} decreases with increasing CH{sub 4} concentration. In contrast, the diffusivity of CH{sub 4} is essentially independent of the concentration of CO{sub 2} in the CO{sub 2}/CH{sub 4} mixture, while CO{sub 2} diffusivity decreases with increased CH{sub 4} loading, even though the diffusivity of CH{sub 4} is substantially larger than that of CO{sub 2}. This unusual behavior can be explained in terms of differences in adsorption site preferences due to charge–quadrupole interactions.

  20. Effects of aerosol/cloud interactions on the global radiation budget

    International Nuclear Information System (INIS)

    Chuang, C.C.; Penner, J.E.

    1994-01-01

    Aerosols may modify the microphysics of clouds by acting as cloud condensation nuclei (CCN), thereby enhancing the cloud reflectivity. Aerosols may also alter precipitation development by affecting the mean droplet size, thereby influencing cloud lifetimes and modifying the hydrological cycle. Clouds have a major effect on climate, but aerosol/cloud interactions have not been accounted for in past climate model simulations. However, the worldwide steady rise of global pollutants and emissions makes it imperative to investigate how atmospheric aerosols affect clouds and the global radiation budget. In this paper, the authors examine the relationship between aerosol and cloud drop size distributions by using a detailed micro-physical model. They parameterize the cloud nucleation process in terms of local aerosol characteristics and updraft velocity for use in a coupled climate/chemistry model to predict the magnitude of aerosol cloud forcing. Their simulations indicate that aerosol/cloud interactions may result in important increases in reflected solar radiation, which would mask locally the radiative forcing from increased greenhouse gases. This work is aimed at improving the assessment of the effects of anthropogenic aerosols on cloud optical properties and the global radiation budget

  1. Joint Application of Concentrations and Isotopic Signatures to Investigate the Global Atmospheric Carbon Monoxide Budget: Inverse Modeling Approach

    Science.gov (United States)

    Park, K.; Mak, J. E.; Emmons, L. K.

    2008-12-01

    Carbon monoxide is not only an important component for determining the atmospheric oxidizing capacity but also a key trace gas in the atmospheric chemistry of the Earth's background environment. The global CO cycle and its change are closely related to both the change of CO mixing ratio and the change of source strength. Previously, to estimate the global CO budget, most top-down estimation techniques have been applied the concentrations of CO solely. Since CO from certain sources has a unique isotopic signature, its isotopes provide additional information to constrain its sources. Thus, coupling the concentration and isotope fraction information enables to tightly constrain CO flux by its sources and allows better estimations on the global CO budget. MOZART4 (Model for Ozone And Related chemical Tracers), a 3-D global chemical transport model developed at NCAR, MPI for meteorology and NOAA/GFDL and is used to simulate the global CO concentration and its isotopic signature. Also, a tracer version of MOZART4 which tagged for C16O and C18O from each region and each source was developed to see their contributions to the atmosphere efficiently. Based on the nine-year-simulation results we analyze the influences of each source of CO to the isotopic signature and the concentration. Especially, the evaluations are focused on the oxygen isotope of CO (δ18O), which has not been extensively studied yet. To validate the model performance, CO concentrations and isotopic signatures measured from MPI, NIWA and our lab are compared to the modeled results. The MOZART4 reproduced observational data fairly well; especially in mid to high latitude northern hemisphere. Bayesian inversion techniques have been used to estimate the global CO budget with combining observed and modeled CO concentration. However, previous studies show significant differences in their estimations on CO source strengths. Because, in addition to the CO mixing ratio, isotopic signatures are independent tracers

  2. The effects of CO addition on the autoignition of H-2, CH4 and CH4/H-2 fuels at high pressure in an RCM

    NARCIS (Netherlands)

    Gersen, Sander; Darmeveil, Harry; Levinsky, Howard

    2012-01-01

    Autoignition delay times of stoichiometric and fuel-lean (phi = 0.5) H-2, H-2/CO, CH4, CH4/CO, CH4/H-2 and CH4/CO/H-2 mixtures have been measured in an Rapid Compression Machine at pressures ranging from 20 to 80 bar and in the temperature range 900-1100K. The effects of CO addition on the ignition

  3. Atmospheric CH4 in the first decade of the 21st century: Inverse modeling analysis using SCIAMACHY satellite retrievals and NOAA surface measurements

    NARCIS (Netherlands)

    Bergamaschi, P.; Houweling, S.; Segers, A.; Krol, M.; Frankenberg, C.; Scheepmaker, R.A.; Dlugokencky, E.; Wofsy, S.C.; Kort, E.A.; Sweeney, C.; Schuck, T.; Brenninkmeijer, C.; Chen, H.; Beck, V.; Gerbig, C.

    2013-01-01

    The causes of renewed growth in the atmospheric CH4 burden since 2007 are still poorly understood and subject of intensive scientific discussion. We present a reanalysis of global CH4 emissions during the 2000s, based on the TM5-4DVAR inverse modeling system. The model is optimized using

  4. The ecology of methane in streams and rivers: Patterns, controls, and global significance

    Science.gov (United States)

    Stanley, Emily H.; Casson, Nora J.; Christel, Samuel T.; Crawford, John T.; Loken, Luke C.; Oliver, Samantha K.

    2016-01-01

    Streams and rivers can substantially modify organic carbon (OC) inputs from terrestrial landscapes, and much of this processing is the result of microbial respiration. While carbon dioxide (CO2) is the major end-product of ecosystem respiration, methane (CH4) is also present in many fluvial environments even though methanogenesis typically requires anoxic conditions that may be scarce in these systems. Given recent recognition of the pervasiveness of this greenhouse gas in streams and rivers, we synthesized existing research and data to identify patterns and drivers of CH4, knowledge gaps, and research opportunities. This included examining the history of lotic CH4 research, creating a database of concentrations and fluxes (MethDB) to generate a global-scale estimate of fluvial CH4 efflux, and developing a conceptual framework and using this framework to consider how human activities may modify fluvial CH4 dynamics. Current understanding of CH4 in streams and rivers has been strongly influenced by goals of understanding OC processing and quantifying the contribution of CH4 to ecosystem C fluxes. Less effort has been directed towards investigating processes that dictate in situ CH4 production and loss. CH4 makes a meager contribution to watershed or landscape C budgets, but streams and rivers are often significant CH4 sources to the atmosphere across these same spatial extents. Most fluvial systems are supersaturated with CH4 and we estimate an annual global emission of 26.8 Tg CH4, equivalent to ~15-40% of wetland and lake effluxes, respectively. Less clear is the role of CH4 oxidation, methanogenesis, and total anaerobic respiration to whole ecosystem production and respiration. Controls on CH4 generation and persistence can be viewed in terms of proximate controls that influence methanogenesis (organic matter, temperature, alternative electron acceptors, nutrients) and distal geomorphic and hydrologic drivers. Multiple controls combined with its

  5. Photosynthates as dominant source of CH4 and CO2 in soil water and CH4 emitted to the atmosphere from paddy fields

    Science.gov (United States)

    Minoda, Tomomi; Kimura, Mamoto; Wada, Eitaro

    1996-09-01

    Emission rates of CH4 from paddy soil with and without rice straw applications were measured with pot experiments to estimate the contribution of rice straw to the total CH4 emission during the growth period of rice plants. The CH4 derived from rice straw was calculated to be 44% of the total emission. 13CO2 uptake experiments were also carried out four times from June 30 to September 13, 1994, to estimate the contribution of photosynthesized carbon to CH4 emission. The contribution percentages of photosynthesized carbon to the total CH4 emitted to the atmosphere were 3.8% around June 30, 31% around July 25, 30% around August 19, and 14% around September 13 in the treatment with rice straw applications, and 52% around July 25, 28% around August 19, and 15% around September 13 in the treatment without rice straw applications. They were calculated to be 22% and 29% for the entire growth period in the treatments with and without rice straw applications, respectively. The contribution percentages of photosynthesized carbon to the total CH4 and inorganic carbon (Σ CO2) dissolved in soil water were 1.3%, 30%, 29%, and 34% for dissolved CH4 and 3.0%, 36%, 30% and 28% for dissolved inorganic carbon around June 30, July 25, August l9, and September 13, respectively, in the treatment with rice straw applications. They were 70%, 23%, and 32% for dissolved CH4 and 31%, 16%, and 19% for dissolved inorganic carbon around July 25, August 19, and September 13, respectively, in the treatment without rice straw applications.

  6. Effects of coastal marsh conversion to shrimp aquaculture ponds on CH4 and N2O emissions

    Science.gov (United States)

    Yang, P.; Bastviken, D.; Lai, D. Y. F.; Jin, B. S.; Mou, X. J.; Tong, C.; Yao, Y. C.

    2017-12-01

    In this study, we compared the CH4 and N2O fluxes from a tidal brackish Cyperus malaccensis marsh ecosystem and nearby shrimp ponds, converted from C. malaccensis marsh in the last 3-4 years, in the Min River estuary of southeast China over the aquaculture period of the year. Significant differences in CH4 and N2O fluxes were observed in space (between brackish marsh and shrimp ponds) and in time (between sampling occasions that were distributed over the aquaculture period). CH4 fluxes from the shrimp ponds were on an average 10-fold higher than from the brackish marsh. N2O emissions, on the other hand, were lower from the shrimp pond (25% of the emissions from the brackish marsh). Accessory data indicates that these patterns were primarily linked to water level variability and temperature (all fluxes), sediment porewater sulfate concentrations (CH4 flux) and total nitrogen concentrations (N2O flux). Our research demonstrates that the coastal marsh ecosystem converted to aquaculture ponds considerably alter emissions of CH4 and N2O and provides input to the global discussion on how to account for emissions from various types of flooded land in greenhouse gas inventories.

  7. Dissociative sticking of CH4 on Ru(0001)

    DEFF Research Database (Denmark)

    Nielsen, Jane Hvolbæk; Holmblad, Peter Mikal; Chorkendorff, Ib

    1999-01-01

    In this study the CH4 dissociation probability on Ru(0001) is found for various translational and vibrational energies. The absolute sticking values are determined from King and Wells experiments and carbon uptake curves. The carbon amount is determined from the recombination signal of carbon...... with oxygen obtained after the beam exposure when heating in an oxygen atmosphere. The measured sticking coefficient of CH4 is strongly enhanced both by increasing the translational and the vibrational energy of the CH4 molecule. A model is applied to the data and an estimate of the thermal activation energy...

  8. A catchment-scale carbon and greenhouse gas budget of a subarctic landscape

    DEFF Research Database (Denmark)

    Christensen, Torben R; Johansson, Torbjörn; Olsrud, Maria

    2007-01-01

    forest, and mires, lakes and alpine ecosystems. The magnitudes of atmospheric exchange of carbon in the form of the GHGs, CO2 and CH4 in these various ecosystems differ significantly, ranging from little or no flux in barren ecosystems over a small CO2 sink function and low rates of CH4 exchange...... in the heaths to significant CO2 uptake in the forests and also large emissions of CH4 from the mires and small lakes. The overall catchment budget, given the size distribution of the individual ecosystem types and a first approximation of run-off as dissolved organic carbon, reveals a landscape currently...

  9. High net CO2 and CH4 release at a eutrophic shallow lake on a formerly drained fen

    Science.gov (United States)

    Franz, Daniela; Koebsch, Franziska; Larmanou, Eric; Augustin, Jürgen; Sachs, Torsten

    2016-05-01

    Drained peatlands often act as carbon dioxide (CO2) hotspots. Raising the groundwater table is expected to reduce their CO2 contribution to the atmosphere and revitalise their function as carbon (C) sink in the long term. Without strict water management rewetting often results in partial flooding and the formation of spatially heterogeneous, nutrient-rich shallow lakes. Uncertainties remain as to when the intended effect of rewetting is achieved, as this specific ecosystem type has hardly been investigated in terms of greenhouse gas (GHG) exchange. In most cases of rewetting, methane (CH4) emissions increase under anoxic conditions due to a higher water table and in terms of global warming potential (GWP) outperform the shift towards CO2 uptake, at least in the short term.Based on eddy covariance measurements we studied the ecosystem-atmosphere exchange of CH4 and CO2 at a shallow lake situated on a former fen grassland in northeastern Germany. The lake evolved shortly after flooding, 9 years previous to our investigation period. The ecosystem consists of two main surface types: open water (inhabited by submerged and floating vegetation) and emergent vegetation (particularly including the eulittoral zone of the lake, dominated by Typha latifolia). To determine the individual contribution of the two main surface types to the net CO2 and CH4 exchange of the whole lake ecosystem, we combined footprint analysis with CH4 modelling and net ecosystem exchange partitioning.The CH4 and CO2 dynamics were strikingly different between open water and emergent vegetation. Net CH4 emissions from the open water area were around 4-fold higher than from emergent vegetation stands, accounting for 53 and 13 g CH4 m-2 a-1 respectively. In addition, both surface types were net CO2 sources with 158 and 750 g CO2 m-2 a-1 respectively. Unusual meteorological conditions in terms of a warm and dry summer and a mild winter might have facilitated high respiration rates. In sum, even after 9

  10. Cumulative carbon emissions budgets consistent with 1.5 °C global warming

    Science.gov (United States)

    Tokarska, Katarzyna B.; Gillett, Nathan P.

    2018-04-01

    The Paris Agreement1 commits ratifying parties to pursue efforts to limit the global temperature increase to 1.5 °C relative to pre-industrial levels. Carbon budgets2-5 consistent with remaining below 1.5 °C warming, reported in the IPCC Fifth Assessment Report (AR5)2,6,8, are directly based on Earth system model (Coupled Model Intercomparison Project Phase 5)7 responses, which, on average, warm more than observations in response to historical CO2 emissions and other forcings8,9. These models indicate a median remaining budget of 55 PgC (ref. 10, base period: year 1870) left to emit from January 2016, the equivalent to approximately five years of emissions at the 2015 rate11,12. Here we calculate warming and carbon budgets relative to the decade 2006-2015, which eliminates model-observation differences in the climate-carbon response over the historical period9, and increases the median remaining carbon budget to 208 PgC (33-66% range of 130-255 PgC) from January 2016 (with mean warming of 0.89 °C for 2006-2015 relative to 1861-188013-18). There is little sensitivity to the observational data set used to infer warming that has occurred, and no significant dependence on the choice of emissions scenario. Thus, although limiting median projected global warming to below 1.5 °C is undoubtedly challenging19-21, our results indicate it is not impossible, as might be inferred from the IPCC AR5 carbon budgets2,8.

  11. [Effects of biochar application three-years ago on global warming potentials of CH4 and N2O in a rice-wheat rotation system.

    Science.gov (United States)

    Wu, Zhen; Dong, Yu Bing; Xiong, Zheng Qin

    2018-01-01

    To evaluate the long-term effects of biochar amendment on greenhouse gas emissions (GHGs), a field experiment was conducted to examine the effects of 3-year field-aged biochar (B 3 ) and fresh biochar (B 0 ) on global warming potential (GWP) and greenhouse gas intensity (GHGI) of methane (CH 4 ) and nitrous oxide (N 2 O) in a typical rice-wheat rotation system. Four treatments were established as control without nitrogen fertilizer (CK), urea without biochar (N), urea with fresh biochar amended in 2015 (NB 0 ), and urea with 3-year field-aged biochar amended in 2012 (NB 3 ). Results showed that both the NB 0 and NB 3 treatments obviously increased soil pH, soil organic carbon (SOC), total nitrogen (TN) and influenced the potential activity of functional microorganisms related to GHGs compared to the N treatment. Relative to the N treatment, the NB 3 treatment significantly improved crop yield by 14.1% while reduced the CH 4 and N 2 O emissions by 9.0% and 34.0%, respectively. In addition, the NB 0 treatment significantly improved crop yield by 9.3%, while reduced the N 2 O emission by 38.6% though increased the CH 4 emissions by 4.7% relative to the N treatment. Moreover, both the NB 0 and NB 3 treatments could significantly reduce both GWP and GHGI, with NB 3 being more effective in simultaneously mitigating the GHGs emissions and enhancing crop yield. Since field-aged biochar showed obvious effects on GHGs mitigation and carbon sequestration after 3 years, biochar incorporations had long-term effect on GHGs mitigation and crop production in the rice-wheat rotation system.

  12. Using eddy covariance of CO2, 13CO2 and CH4, continuous soil respiration measurements, and PhenoCams to constrain a process-based biogeochemical model for carbon market-funded wetland restoration

    Science.gov (United States)

    Oikawa, P. Y.; Baldocchi, D. D.; Knox, S. H.; Sturtevant, C. S.; Verfaillie, J. G.; Dronova, I.; Jenerette, D.; Poindexter, C.; Huang, Y. W.

    2015-12-01

    We use multiple data streams in a model-data fusion approach to reduce uncertainty in predicting CO2 and CH4 exchange in drained and flooded peatlands. Drained peatlands in the Sacramento-San Joaquin River Delta, California are a strong source of CO2 to the atmosphere and flooded peatlands or wetlands are a strong CO2 sink. However, wetlands are also large sources of CH4 that can offset the greenhouse gas mitigation potential of wetland restoration. Reducing uncertainty in model predictions of annual CO2 and CH4 budgets is critical for including wetland restoration in Cap-and-Trade programs. We have developed and parameterized the Peatland Ecosystem Photosynthesis, Respiration, and Methane Transport model (PEPRMT) in a drained agricultural peatland and a restored wetland. Both ecosystem respiration (Reco) and CH4 production are a function of 2 soil carbon (C) pools (i.e. recently-fixed C and soil organic C), temperature, and water table height. Photosynthesis is predicted using a light use efficiency model. To estimate parameters we use a Markov Chain Monte Carlo approach with an adaptive Metropolis-Hastings algorithm. Multiple data streams are used to constrain model parameters including eddy covariance of CO2, 13CO2 and CH4, continuous soil respiration measurements and digital photography. Digital photography is used to estimate leaf area index, an important input variable for the photosynthesis model. Soil respiration and 13CO2 fluxes allow partitioning of eddy covariance data between Reco and photosynthesis. Partitioned fluxes of CO2 with associated uncertainty are used to parametrize the Reco and photosynthesis models within PEPRMT. Overall, PEPRMT model performance is high. For example, we observe high data-model agreement between modeled and observed partitioned Reco (r2 = 0.68; slope = 1; RMSE = 0.59 g C-CO2 m-2 d-1). Model validation demonstrated the model's ability to accurately predict annual budgets of CO2 and CH4 in a wetland system (within 14% and 1

  13. In-situ studies of microbial CH4 oxidation efficiency in Arctic wetland soils. Applications of stable carbon isotopes

    International Nuclear Information System (INIS)

    Preuss, Inken-Marie

    2013-01-01

    .018 ± 0.009) and needs to be determined on a case by case basis. The impact of both fractionation factors on the quantification of CH 4 oxidation was analyzed by considering both the diffusivity under saturated and unsaturated conditions and potential oxidation rates. The predominant water table determines the magnitude of CH 4 oxidation efficiencies in arctic wetland soils: submerged organic-matter-rich soils indicated CH 4 oxidation efficiencies of 10 to 70 %, while polygon centers and rims with an aerobic surface layer showed capacity of complete oxidation. Temperature increase might affect CH 4 oxidation efficiencies of saturated sites in the long term, however short-time effects were not observed. The improved in-situ quantification of CH 4 oxidation in wetlands enables a better assessment of current and potential CH 4 sources and sinks in permafrost-affected ecosystems and their potential strengths in response to global warming.

  14. Seasonal CH4 and N2O emissions and plant growth characteristics of several cultivars in direct seeded rice systems

    Science.gov (United States)

    Simmonds, M.; Anders, M. M.; Adviento-Borbe, M. A.; Van Kessel, C.; McClung, A.; Linquist, B.

    2014-12-01

    Understanding cultivar effects on field greenhouse gas (GHG) emissions in rice (Oryza sativa L.) systems is needed to improve the accuracy of predictive models used for estimating GHG emissions, and to determine to what extent choice of cultivar may have on GHG mitigation. We compared CH4 and N2O emissions, global warming potential (GWP = N2O + CH4), yield-scaled GWP (GWPY = GWP Mg-1 grain), and plant growth characteristics of 8 cultivars within 4 study sites in California and Arkansas. Seasonal CH4 emissions differed between cultivars by a factor of 2.1 and 1.3 at one California and one Arkansas site, respectively. Nitrous oxide emissions were negligible, comprised food security.

  15. Variations in the methane budget over the last two millennia

    NARCIS (Netherlands)

    Sapart, C.J.

    2012-01-01

    Methane (CH4) is a strong greenhouse gas and even though its atmospheric abundance is lower than carbon dioxide (CO2), CH4 has a global warming potential twenty-five times larger than CO2 and its atmospheric abundance has drastically increased since 1800. Understanding the evolution of the CH4

  16. Electron paramagnetic resonance of gamma irradiated (CH3)3NHClO4 and CH3NH3ClO4 single crystals

    International Nuclear Information System (INIS)

    Yavuz, Metin; Koeksal, Fevzi

    1999-01-01

    Gamma irradiation damage centers in (CH 3 ) 3 NHClO 4 and CH 3 NH 3 ClO 4 single crystals have been investigated at room temperature by the electron paramagnetic resonance (EPR) technique. It has been found that γ-irradiation produces the (CH 3 ) 3 N + radical in the first, and NH + 3 and ClO 3 radicals in the second compound. The EPR parameters of the observed radicals have been determined and discussed

  17. Background CH4 and N2O fluxes in low-input short rotation coppice

    Science.gov (United States)

    Görres, Carolyn-Monika; Zenone, Terenzio; Ceulemans, Reinhart

    2016-04-01

    Extensively managed short rotation coppice systems are characterized by low fluxes of CH4 and N2O. However due to the large global warming potential of these trace gases (GWP100: CH4: 34, N2O: 298), such background fluxes can still significantly contribute to offsetting the CO2 uptake of short rotation coppice systems. Recent technological advances in fast-response CH4 and N2O analysers have improved our capability to capture these background fluxes, but their quantification still remains a challenge. As an example, we present here CH4 and N2O fluxes from a short-rotation bioenergy plantation in Belgium. Poplars have been planted in a double-row system on a loamy sand in 2010 and coppiced in the beginning of 2012 and 2014 (two-year rotation system). In 2013 (June - November) and 2014 (April - August), the plantation's CH4 and N2O fluxes were measured in parallel with an eddy covariance tower (EC) and an automated chamber system (AC). The EC had a detection limit of 13.68 and 0.76 μmol m-2 h-1 for CH4 and N2O, respectively. The median detection limit of the AC was 0.38 and 0.08 μmol m-2 h-1 for CH4 and N2O, respectively. The EC picked up a few high CH4 emission events with daily averages >100 μmol m-2 h-1, but a large proportion of the measured fluxes were within the EC's detection limit. The same was true for the EC-derived N2O fluxes where the daily average flux was often close to the detection limit. Sporadically, some negative (uptake) fluxes of N2O were observed. On the basis of the EC data, no clear link was found between CH4 and N2O fluxes and environmental variables. The problem with fluxes within the EC detection limit is that a significant amount of the values can show the opposite sign, thus "mirroring" the true flux. Subsequently, environmental controls of background trace gas fluxes might be disguised in the analysis. As a next step, it will be tested if potential environmental drivers of background CH4 and N2O fluxes at the plantation can be

  18. Simulasi Numeris Karakteristik Pembakaran CH4/CO2/Udara dan CH4/CO2/O2 pada Counterflow Premixed Burner

    Directory of Open Access Journals (Sweden)

    Hangga Wicaksono

    2017-08-01

    Full Text Available The high amount of CO2 produced in a conventional biogas reactor needs to be considered. A further analysis is needed in order to investigate the effect of CO2 addition especially in thermal and chemical kinetics aspect. This numerical study has been held to analyze the effect of CO2 in CH4/CO2/O­2 and CH4/CO2/Air premixed combustion. In this study one dimensional analisys in a counterflow burner has been performed. The volume fraction of CO2 used in this study was 0%-40% from CH4’s volume fraction, according to the amount of CO2 in general phenomenon. Based on the flammability limits data, the volume fraction of CH4 used was 5-61% in O2 environment and 5-15% in air environment. The results showed a decreasing temperature along with the increasing percentage of CO2 in each mixtures, but the effect was quite smaller especially in stoichiometric and lean mixture. CO2 could affects thermally (by absorbing heat due to its high Cp and also made the production of unburnt fuel species such as CO relatively higher.

  19. Bio-refinery system of DME or CH4 production from black liquor gasification in pulp mills.

    Science.gov (United States)

    Naqvi, M; Yan, J; Fröling, M

    2010-02-01

    There is great interest in developing black liquor gasification technology over recent years for efficient recovery of bio-based residues in chemical pulp mills. Two potential technologies of producing dimethyl ether (DME) and methane (CH(4)) as alternative fuels from black liquor gasification integrated with the pulp mill have been studied and compared in this paper. System performance is evaluated based on: (i) comparison with the reference pulp mill, (ii) fuel to product efficiency (FTPE) and (iii) biofuel production potential (BPP). The comparison with the reference mill shows that black liquor to biofuel route will add a highly significant new revenue stream to the pulp industry. The results indicate a large potential of DME and CH(4) production globally in terms of black liquor availability. BPP and FTPE of CH(4) production is higher than DME due to more optimized integration with the pulping process and elimination of evaporation unit in the pulp mill.

  20. Methane emissions from a human-dominated lowland coastal river network (Shanghai, China)

    Science.gov (United States)

    Wang, D.; Yu, Z.

    2017-12-01

    Evasion of methane (CH4) in streams and rivers play a critical role in global carbon (C) cycle, offsetting the C uptake by terrestrial ecosystems. However, little is known about CH4 emissions from lowland coastal rivers profoundly modified by anthropogenic perturbations. Here, we report results from a long-term, large-scale study of CH4 partial pressures (pCH4) and evasion rates in the Shanghai river network. The spatiotemporal variability of pCH4 was examined along a land-use gradient and the annual CH4 evasion were estimated to assess its role in regional C budget. During the study period, the median pCH4 from 87 surveyed rivers was 241 μatm. CH4 was oversaturated throughout the river network, CH4 hotpots were concentrated in the small urban rivers and highly discharge-dependent. The annual median fCH4 for each site ranged from 3.1 mg C•m-2•d-1 to 296.6 mg C•m-2•d-1. The annual CH4 evasion were 105 Gg CO2-eq•yr-1 and 96 Gg CO2-eq•yr-1 for the entire river network and the mainland rivers, respectively. Given the rapid urbanization in global coastal areas, more research is needed to quantify the role of lowland coastal rivers as a major landscape C source in global C budget.

  1. Northern peatland initiation lagged abrupt increases in deglacial atmospheric CH4.

    Science.gov (United States)

    Reyes, Alberto V; Cooke, Colin A

    2011-03-22

    Peatlands are a key component of the global carbon cycle. Chronologies of peatland initiation are typically based on compiled basal peat radiocarbon (14C) dates and frequency histograms of binned calibrated age ranges. However, such compilations are problematic because poor quality 14C dates are commonly included and because frequency histograms of binned age ranges introduce chronological artefacts that bias the record of peatland initiation. Using a published compilation of 274 basal 14C dates from Alaska as a case study, we show that nearly half the 14C dates are inappropriate for reconstructing peatland initiation, and that the temporal structure of peatland initiation is sensitive to sampling biases and treatment of calibrated 14C dates. We present revised chronologies of peatland initiation for Alaska and the circumpolar Arctic based on summed probability distributions of calibrated 14C dates. These revised chronologies reveal that northern peatland initiation lagged abrupt increases in atmospheric CH4 concentration at the start of the Bølling-Allerød interstadial (Termination 1A) and the end of the Younger Dryas chronozone (Termination 1B), suggesting that northern peatlands were not the primary drivers of the rapid increases in atmospheric CH4. Our results demonstrate that subtle methodological changes in the synthesis of basal 14C ages lead to substantially different interpretations of temporal trends in peatland initiation, with direct implications for the role of peatlands in the global carbon cycle.

  2. Distillation Calculation for the Separation of {sup 13}CH{sub 4} from LNG

    Energy Technology Data Exchange (ETDEWEB)

    Song, K.M.; Son, S.H.; Kim, K.S.; Lee, S.K. [Korea Electric Power Research Institute, Taejon (Korea)

    2002-07-01

    For the purpose of {sup 13}CH{sub 4} production from LNG, the theoretical number of stages and the number of distillation column required for the separation of {sup 13}CH{sub 4} from {sup 12}CH{sub 4}/{sup 13}CH{sub 4} mixture of containing 1%-{sup 13}CH{sub 4} are calculated. Assuming the ideal liquid mixture of containing 1%-{sup 13}CH{sub 4} are calculated. Assuming the ideal liquid mixture of {sup 12}CH{sub 4} and {sup 13}CH{sub 4}, the theoretical number of stages are calculated by smoker equation and FUG method. Using the correlation between the minimum theoretical number of stages and the optimum theoretical number of stages, the number of distillation groups is calculated. From this calculation, we know that 6 groups of distillation tower with 600 stages per one column are needed for the production of 90%-{sup 13}CH{sub 4}. (author). 5 refs., 5 figs., 4 tabs.

  3. Observation of CH4 and other Non-CO2 Green House Gas Emissions from California

    Energy Technology Data Exchange (ETDEWEB)

    Fischer, Marc L.; Zhao, Chuanfeng; Riley, William J.; Andrews, Arlyn C.

    2009-01-09

    In 2006, California passed the landmark assembly bill AB-32 to reduce California's emissions of greenhouse gases (GHGs) that contribute to global climate change. AB-32 commits California to reduce total GHG emissions to 1990 levels by 2020, a reduction of 25 percent from current levels. To verify that GHG emission reductions are actually taking place, it will be necessary to measure emissions. We describe atmospheric inverse model estimates of GHG emissions obtained from the California Greenhouse Gas Emissions Measurement (CALGEM) project. In collaboration with NOAA, we are measuring the dominant long-lived GHGs at two tall-towers in central California. Here, we present estimates of CH{sub 4} emissions obtained by statistical comparison of measured and predicted atmospheric mixing ratios. The predicted mixing ratios are calculated using spatially resolved a priori CH{sub 4} emissions and surface footprints, that provide a proportional relationship between the surface emissions and the mixing ratio signal at tower locations. The footprints are computed using the Weather Research and Forecast (WRF) coupled to the Stochastic Time-Inverted Lagrangian Transport (STILT) model. Integral to the inverse estimates, we perform a quantitative analysis of errors in atmospheric transport and other factors to provide quantitative uncertainties in estimated emissions. Regressions of modeled and measured mixing ratios suggest that total CH{sub 4} emissions are within 25% of the inventory estimates. A Bayesian source sector analysis obtains posterior scaling factors for CH{sub 4} emissions, indicating that emissions from several of the sources (e.g., landfills, natural gas use, petroleum production, crops, and wetlands) are roughly consistent with inventory estimates, but livestock emissions are significantly higher than the inventory. A Bayesian 'region' analysis is used to identify spatial variations in CH{sub 4} emissions from 13 sub-regions within California

  4. Mangrove production and carbon sinks: A revision of global budget estimates

    Science.gov (United States)

    Bouillon, S.; Borges, A.V.; Castaneda-Moya, E.; Diele, K.; Dittmar, T.; Duke, N.C.; Kristensen, E.; Lee, S.-Y.; Marchand, C.; Middelburg, J.J.; Rivera-Monroy, V. H.; Smith, T. J.; Twilley, R.R.

    2008-01-01

    Mangrove forests are highly productive but globally threatened coastal ecosystems, whose role in the carbon budget of the coastal zone has long been debated. Here we provide a comprehensive synthesis of the available data on carbon fluxes in mangrove ecosystems. A reassessment of global mangrove primary production from the literature results in a conservative estimate of ???-218 ?? 72 Tg C a-1. When using the best available estimates of various carbon sinks (organic carbon export, sediment burial, and mineralization), it appears that >50% of the carbon fixed by mangrove vegetation is unaccounted for. This unaccounted carbon sink is conservatively estimated at ??? 112 ?? 85 Tg C a-1, equivalent in magnitude to ??? 30-40% of the global riverine organic carbon input to the coastal zone. Our analysis suggests that mineralization is severely underestimated, and that the majority of carbon export from mangroves to adjacent waters occurs as dissolved inorganic carbon (DIC). CO2 efflux from sediments and creek waters and tidal export of DIC appear to be the major sinks. These processes are quantitatively comparable in magnitude to the unaccounted carbon sink in current budgets, but are not yet adequately constrained with the limited published data available so far. Copyright 2008 by the American Geophysical Union.

  5. [Data processing and QA/QC of atmosphere CO2 and CH4 concentrations by a method of GC-FID in-situ measurement at Waliguan station].

    Science.gov (United States)

    Zhang, Fang; Zhou, Ling-Xi; Liu, Li-Xin; Fang, Shuang-Xi; Yao, Bo; Xu, Lin; Zhang, Xiao-Chun; Masarie, Kenneth A; Conway, Thomas J; Worthy, Douglas E J; Ernst, Michele

    2010-10-01

    To strengthen scientific management and sharing of greenhouse gas data obtained from atmospheric background stations in China, it is important to ensure the standardization of observations and establish the data treatment and quality control procedure so as to maintain consistency in atmospheric carbon dioxide (CO2) and methane (CH4) measurements from different background stations. An automated gas chromatographic system (Hewlett Packard 5890GC employing flame ionization detection) for in situ measurements of atmospheric CO2 and CH4 has been developed since 1994 at the China Global Atmosphere Watch Baseline Observatory at Mt. Waliguan, in Qinhai. In this study, processing and quality control flow of CO2 and CH4 data acquired by HP ChemStation are discussed in detail, including raw data acquisition, data merge, time series inspection, operator flag, principal investigator flag, and the comparison of the GC measurement with the flask method. Atmosphere CO2 and CH4 mixing ratios were separated as background and non-background data using a robust local regression method, approximately 72% and 44% observed values had been filtered as background data for CO2 and CH4, respectively. Comparison of the CO1 and CH, in situ data to the flask sampling data were in good agreement, the relative deviations are within +/- 0.5% for CO2 and for CH4. The data has been assimilated into global database (Globalview-CO2, Globalview-CH4), submitted to the World Data Centre for Greenhouse Gases (WDCGG), and applied to World Meteorological Organization (WMO) Greenhouse Gas Bulletin and assessment reports of the United Nations Intergovernmental Panel on Climate Change (IPCC).

  6. The carbon-budget approach to climate stabilization: Costeffective subglobal versus global action

    OpenAIRE

    Eichner, Thomas; Pethig, Rüdiger

    2010-01-01

    Scientific expertise suggests that mitigating extreme world-wide climate change damages requires avoiding increases in the world mean temperature exceeding 2ê Celsius. To achieve the two degree target, the cumulated global emissions must not exceed some limit, the so-called global carbon budget. In a two-period twocountry general equilibrium model with a finite stock of fossil fuels we compare the cooperative cost-effective policy with the unilateral cost-effective policy of restricting emiss...

  7. CO2/CH4 Separation via Polymeric Blend Membrane

    Directory of Open Access Journals (Sweden)

    H. Sanaeepur

    2013-01-01

    Full Text Available CO2/CH4 gas separation is a very important applicatable process in upgrading the natural gas and landfil gas recovery. In this work, to investigate the membrane separation process performance, the gas permeation results andCO2/CH4 separation characteristics of different prepared membranes (via blending different molecular weights of polyethylene glycol (PEG as a modifier with acrylonitrile-butadiene-styrene (ABS as a backbone structure have been studied. Furthermore, SEM analysis was carried out for morphological investigations. The effect of PEG content on gas transport properties on the selected sample was also studied. The effect of pressure on CO2 permeation was examined and showed that at the pressure beyond 4 bar, permeability is not affected by pressure. The results showed that more or less in all cases, incorporation of PEG molecules without any significant increase in CH4 permeability increases the CO2/CH4 selectivity. From the view point of gas separation applications the resultant data are within commercial attractive range

  8. Gas seepage from Tokamachi mud volcanoes, onshore Niigata Basin (Japan): Origin, post-genetic alterations and CH{sub 4}-CO{sub 2} fluxes

    Energy Technology Data Exchange (ETDEWEB)

    Etiope, G., E-mail: etiope@ingv.it [Istituto Nazionale di Geofisica e Vulcanologia, via V. Murata 605, 00143 Roma (Italy); Nakada, R. [Dept. of Earth and Planetary Systems Science, Graduate School of Science, Hiroshima University (Japan); Tanaka, K. [Graduate School of Science and Engineering, Yamaguchi University (Japan); Yoshida, N. [Dept. of Environmental Chemistry and Engineering, Tokyo Institute of Technology (Japan)

    2011-03-15

    Research highlights: {yields} Tokamachi gas shows signals of subsurface hydrocarbon biodegradation. {yields} Hydrocarbon molecular fractionation depends on gas flux. {yields} Substantial gas emission from mud volcanoes is from invisible diffuse seepage. {yields} Global mud volcano methane emission is likely higher than 10 Mt a{sup -1}. - Abstract: Methane and CO{sub 2} emissions from the two most active mud volcanoes in central Japan, Murono and Kamou (Tokamachi City, Niigata Basin), were measured in from both craters or vents (macro-seepage) and invisible exhalation from the soil (mini- and microseepage). Molecular and isotopic compositions of the released gases were also determined. Gas is thermogenic ({delta}{sup 13}C{sub CH4} from -32.9 per mille to -36.2 per mille), likely associated with oil, and enrichments of {sup 13}C in CO{sub 2} ({delta}{sup 13}C{sub CO2} up to +28.3 per mille) and propane ({delta}{sup 13}C{sub C3H8} up to -8.6 per mille) suggest subsurface petroleum biodegradation. Gas source and post-genetic alteration processes did not change from 2004 to 2010. Methane flux ranged within the orders of magnitude of 10{sup 1}-10{sup 4} g m{sup -2} d{sup -1} in macro-seeps, and up to 446 g m{sup -2} d{sup -1} from diffuse seepage. Positive CH{sub 4} fluxes from dry soil were widespread throughout the investigated areas. Total CH{sub 4} emission from Murono and Kamou were estimated to be at least 20 and 3.7 ton a{sup -1}, respectively, of which more than half was from invisible seepage surrounding the mud volcano vents. At the macro-seeps, CO{sub 2} fluxes were directly proportional to CH{sub 4} fluxes, and the volumetric ratios between CH{sub 4} flux and CO{sub 2} flux were similar to the compositional CH{sub 4}/CO{sub 2} volume ratio. Macro-seep flux data, in addition to those of other 13 mud volcanoes, supported the hypothesis that molecular fractionation (increase of the 'Bernard ratio' C{sub 1}/(C{sub 2} + C{sub 3})) is inversely

  9. Simulated effects of nitrogen saturation the global carbon budget using the IBIS model

    Science.gov (United States)

    Lu, Xuehe; Jiang, Hong; Liu, Jinxun; Zhang, Xiuying; Jin, Jiaxin; Zhu, Qiuan; Zhang, Zhen; Peng, Changhui

    2016-01-01

    Over the past 100 years, human activity has greatly changed the rate of atmospheric N (nitrogen) deposition in terrestrial ecosystems, resulting in N saturation in some regions of the world. The contribution of N saturation to the global carbon budget remains uncertain due to the complicated nature of C-N (carbon-nitrogen) interactions and diverse geography. Although N deposition is included in most terrestrial ecosystem models, the effect of N saturation is frequently overlooked. In this study, the IBIS (Integrated BIosphere Simulator) was used to simulate the global-scale effects of N saturation during the period 1961–2009. The results of this model indicate that N saturation reduced global NPP (Net Primary Productivity) and NEP (Net Ecosystem Productivity) by 0.26 and 0.03 Pg C yr−1, respectively. The negative effects of N saturation on carbon sequestration occurred primarily in temperate forests and grasslands. In response to elevated CO2 levels, global N turnover slowed due to increased biomass growth, resulting in a decline in soil mineral N. These changes in N cycling reduced the impact of N saturation on the global carbon budget. However, elevated N deposition in certain regions may further alter N saturation and C-N coupling.

  10. In-situ studies of microbial CH{sub 4} oxidation efficiency in Arctic wetland soils. Applications of stable carbon isotopes

    Energy Technology Data Exchange (ETDEWEB)

    Preuss, Inken-Marie

    2013-07-05

    , it was found that α{sub ox} differs widely between sites and horizons (mean α{sub ox} = 1.018 ± 0.009) and needs to be determined on a case by case basis. The impact of both fractionation factors on the quantification of CH{sub 4} oxidation was analyzed by considering both the diffusivity under saturated and unsaturated conditions and potential oxidation rates. The predominant water table determines the magnitude of CH{sub 4} oxidation efficiencies in arctic wetland soils: submerged organic-matter-rich soils indicated CH{sub 4} oxidation efficiencies of 10 to 70 %, while polygon centers and rims with an aerobic surface layer showed capacity of complete oxidation. Temperature increase might affect CH{sub 4} oxidation efficiencies of saturated sites in the long term, however short-time effects were not observed. The improved in-situ quantification of CH{sub 4} oxidation in wetlands enables a better assessment of current and potential CH{sub 4} sources and sinks in permafrost-affected ecosystems and their potential strengths in response to global warming.

  11. Exotic Spartina alterniflora invasion alters ecosystem-atmosphere exchange of CH4 and N2O and carbon sequestration in a coastal salt marsh in China.

    Science.gov (United States)

    Yuan, Junji; Ding, Weixin; Liu, Deyan; Kang, Hojeong; Freeman, Chris; Xiang, Jian; Lin, Yongxin

    2015-04-01

    Coastal salt marshes are sensitive to global climate change and may play an important role in mitigating global warming. To evaluate the impacts of Spartina alterniflora invasion on global warming potential (GWP) in Chinese coastal areas, we measured CH4 and N2O fluxes and soil organic carbon sequestration rates along a transect of coastal wetlands in Jiangsu province, China, including open water; bare tidal flat; and invasive S. alterniflora, native Suaeda salsa, and Phragmites australis marshes. Annual CH4 emissions were estimated as 2.81, 4.16, 4.88, 10.79, and 16.98 kg CH4 ha(-1) for open water, bare tidal flat, and P. australis, S. salsa, and S. alterniflora marshes, respectively, indicating that S. alterniflora invasion increased CH4 emissions by 57-505%. In contrast, negative N2O fluxes were found to be significantly and negatively correlated (P carbon sequestration rate of S. alterniflora marsh amounted to 3.16 Mg C ha(-1) yr(-1) in the top 100 cm soil profile, a value that was 2.63- to 8.78-fold higher than in native plant marshes. The estimated GWP was 1.78, -0.60, -4.09, and -1.14 Mg CO2 eq ha(-1) yr(-1) in open water, bare tidal flat, P. australis marsh and S. salsa marsh, respectively, but dropped to -11.30 Mg CO2 eq ha(-1) yr(-1) in S. alterniflora marsh. Our results indicate that although S. alterniflora invasion stimulates CH4 emissions, it can efficiently mitigate increases in atmospheric CO2 and N2O along the coast of China. © 2014 John Wiley & Sons Ltd.

  12. The Ozone Budget in the Upper Troposphere from Global Modeling Initiative (GMI)Simulations

    Science.gov (United States)

    Rodriquez, J.; Duncan, Bryan N.; Logan, Jennifer A.

    2006-01-01

    Ozone concentrations in the upper troposphere are influenced by in-situ production, long-range tropospheric transport, and influx of stratospheric ozone, as well as by photochemical removal. Since ozone is an important greenhouse gas in this region, it is particularly important to understand how it will respond to changes in anthropogenic emissions and changes in stratospheric ozone fluxes.. This response will be determined by the relative balance of the different production, loss and transport processes. Ozone concentrations calculated by models will differ depending on the adopted meteorological fields, their chemical scheme, anthropogenic emissions, and treatment of the stratospheric influx. We performed simulations using the chemical-transport model from the Global Modeling Initiative (GMI) with meteorological fields from (It)h e NASA Goddard Institute for Space Studies (GISS) general circulation model (GCM), (2) the atmospheric GCM from NASA's Global Modeling and Assimilation Office(GMAO), and (3) assimilated winds from GMAO . These simulations adopt the same chemical mechanism and emissions, and adopt the Synthetic Ozone (SYNOZ) approach for treating the influx of stratospheric ozone -. In addition, we also performed simulations for a coupled troposphere-stratosphere model with a subset of the same winds. Simulations were done for both 4degx5deg and 2degx2.5deg resolution. Model results are being tested through comparison with a suite of atmospheric observations. In this presentation, we diagnose the ozone budget in the upper troposphere utilizing the suite of GMI simulations, to address the sensitivity of this budget to: a) the different meteorological fields used; b) the adoption of the SYNOZ boundary condition versus inclusion of a full stratosphere; c) model horizontal resolution. Model results are compared to observations to determine biases in particular simulations; by examining these comparisons in conjunction with the derived budgets, we may pinpoint

  13. 3 CFR 101.2 - Office of Management and Budget.

    Science.gov (United States)

    2010-01-01

    ... 3 The President 1 2010-01-01 2010-01-01 false Office of Management and Budget. 101.2 Section 101.2... PROCEDURES ACT § 101.2 Office of Management and Budget. Freedom of Information regulations for the Office of Management and Budget appear at 5 CFR Ch. III. ...

  14. Bio-refinery system of DME or CH4 production from black liquor gasification in pulp mills

    Energy Technology Data Exchange (ETDEWEB)

    Raza, M.; Jinyue Yan (Dept. of Chemical Engineering and Technology/Energy Processes, Royal Institute of Technology, Stockholm (Sweden)). e-mail: rnaqvi@kth.se; Froeling, Morgan (Dept. of Chemical and Biological Engineering, Chalmers Univ. of Technology, Goeteborg (Sweden))

    2009-07-01

    The consumption of fossil fuels is rapidly increasing and there is an urgent need to develop technologies for renewable fuel production not only as alternatives but also as additional fuels. Efficient polygeneration of transportation fuels with heat and electricity is one of the innovative technologies which have potential to replace fossil fuels and mitigate climate change. Two potential technologies of producing dimethyl ether (DME) and methane (CH4) as alternative fuels integrated with black liquor gasification have been studied and compared in this paper. System performance is evaluated based on: (i) Comparison with the reference pulp mill, (ii) Fuel to product efficiency (FTPE) and (iii) Biofuel Production Potential (BPP). The comparison with the reference mill shows that black liquor to biofuel route will add a highly significant new revenue stream to the pulp industry. The results indicate a large potential of DME and CH4 production globally in terms of black liquor availability. BPP and FTPE of CH4 production is higher than DME due to more optimized integration with the pulping process and elimination of evaporation unit in the pulp mill

  15. Different Apparent Gas Exchange Coefficients for CO2 and CH4: Comparing a Brown-Water and a Clear-Water Lake in the Boreal Zone during the Whole Growing Season.

    Science.gov (United States)

    Rantakari, Miitta; Heiskanen, Jouni; Mammarella, Ivan; Tulonen, Tiina; Linnaluoma, Jessica; Kankaala, Paula; Ojala, Anne

    2015-10-06

    The air-water exchange of carbon dioxide (CO2) and methane (CH4) is a central process during attempts to establish carbon budgets for lakes and landscapes containing lakes. Lake-atmosphere diffusive gas exchange is dependent on the concentration gradient between air and surface water and also on the gas transfer velocity, often described with the gas transfer coefficient k. We used the floating-chamber method in connection with surface water gas concentration measurements to estimate the gas transfer velocity of CO2 (kCO2) and CH4 (kCH4) weekly throughout the entire growing season in two contrasting boreal lakes, a humic oligotrophic lake and a clear-water productive lake, in order to investigate the earlier observed differences between kCO2 and kCH4. We found that the seasonally averaged gas transfer velocity of CH4 was the same for both lakes. When the lakes were sources of CO2, the gas transfer velocity of CO2 was also similar between the two study lakes. The gas transfer velocity of CH4 was constantly higher than that of CO2 in both lakes, a result also found in other studies but for reasons not yet fully understood. We found no differences between the lakes, demonstrating that the difference between kCO2 and kCH4 is not dependent on season or the characteristics of the lake.

  16. Replacement of CH4 in the hydrate by use of liquid CO2

    International Nuclear Information System (INIS)

    Ota, Masaki; Morohashi, Kenji; Abe, Yuki; Watanabe, Masaru; Smith, Richard Lee Jr.; Inomata, Hiroshi

    2005-01-01

    The dynamics of CH 4 replacement in the CH 4 hydrate with saturated liquid CO 2 at 273.2 K was measured with a high pressure optical cell. The results showed that CH 4 in the hydrate gradually moved to the liquid CO 2 phase while CO 2 in the liquid phase penetrated into the hydrate from the quantitative analysis. The decomposing process of the CH 4 hydrate during the replacement was analyzed with in situ Raman spectroscopy, which allowed us to distinguish the cage structure of the CH 4 hydrate and discuss the microscopic view of the replacement in the hydrate. It was found that the decomposition of the medium cage (M-cage) in the CH 4 hydrate proceeded faster than that of the small cage (S-cage). The observed rate difference could be related to the stability of the S-cage in the CH 4 hydrate or the re-formation tendency of CH 4 and water molecules in the S-cage after decomposing the hydrate structure, whereas the guest molecule exchange of CH 4 with CO 2 could occur in the M-cage. Based on the experimental data, we developed a kinetic model for calculation of the CH 4 remaining in the hydrate considering the decomposition rate difference between the M-cage and S-cage in the CH 4 hydrate. The results indicate that the driving force could be the fugacity difference between the fluid phase and the hydrate phase for the replacement process

  17. Methane (CH4) Flux for North America L4 Daily V1 (CMS_CH4_FLX_NAD) at GES DISC

    Data.gov (United States)

    National Aeronautics and Space Administration — The CMS Methane (CH4) Flux for North America data set contains estimates of methane emission in North America based on an inversion of the GEOS-Chem chemical...

  18. On the feasibility of chemi-ion formation in the system CH2CH4A″)+O(3P)

    Science.gov (United States)

    Metropoulos, Aristophanes

    2003-12-01

    We have investigated theoretically the possibility that the CH2CH4A″) radical can generate the CH2CHO+(X1A') ion upon collisions with O(3P). We have concluded that this is very unlikely because the minimum of the ground-state potential-energy surface of the ion is at about the same level as the potential energy of the asymptotic CH2CH4A″)+O(3P) fragments. In addition the Franck-Condon factors should not be favorable because of a drastic change in the geometry of the ion.

  19. Effect of CH4 concentration on the growth behavior, structure, and transparent properties of ultrananocrystalline diamond films synthesized by focused microwave Ar/CH4/H2 plasma jets

    International Nuclear Information System (INIS)

    Liao, Wen-Hsiang; Lin, Chii-Ruey; Wei, Da-Hua

    2013-01-01

    The effects of CH 4 concentration (0.5–5%) on the growth mechanisms, nanostructures, and optically transparent properties of ultrananocrystalline diamond (UNCD) films grown from focused microwave Ar/CH 4 /H 2 (argon-rich) plasma jets were systematically studied. The research results indicated that the grain size and surface roughness of the diamond films increased with increasing CH 4 concentration in the plasma jet, however, the nondiamond contents in films would not be correspondingly decreased resulting from the dispersed diamond nanocrystallites in the films synthesized at higher CH 4 concentration. The reason is due to that the relative emission intensity ratios of the C 2 /H α and the CH/C 2 in the plasma jets were increased and decreased with increasing CH 4 concentration, respectively, to lower the etching of nondiamond phase and the renucleation of diamond during synthesis. The studies of transmission electron microscopy demonstrated that, while the CH 4 introduction of 1% into the plasma jet produced the UNCD films with a spherical geometry (4–8 nm) and the CH 4 introduction of 5% into the plasma jet led to the elongated (∼90 nm in length and ∼35 nm in width) grains in the nanocrystalline diamond (NCD) films with a dendrite-like geometry. The transmittance of diamond films was decreased gradually by films transition from UNCD to NCD, resulting from the enhanced surface roughness and nondiamond contents in films to concurrently increase the light scattering and absorption during photon transmission.

  20. Sediment Budget Analysis; Masonboro Inlet, North Carolina

    Science.gov (United States)

    2017-08-15

    ER D C/ CH L TR -1 7- 13 Regional Sediment Management (RSM) Program Sediment Budget Analysis; Masonboro Inlet, North Carolina Co as ta...ERDC/CHL TR-17-13 August 2017 Sediment Budget Analysis; Masonboro Inlet, North Carolina Kevin B. Conner U.S. Army Engineer District, Wilmington P...Engineers Washington, DC 20314-1000 Under Project 454632, “Sediment Budget Analysis, Masonboro Inlet, NC” ERDC/CHL TR-17-13 ii Abstract A

  1. Long-term global distribution of earth's shortwave radiation budget at the top of atmosphere

    Directory of Open Access Journals (Sweden)

    N. Hatzianastassiou

    2004-01-01

    Full Text Available The mean monthly shortwave (SW radiation budget at the top of atmosphere (TOA was computed on 2.5° longitude-latitude resolution for the 14-year period from 1984 to 1997, using a radiative transfer model with long-term climatological data from the International Satellite Cloud Climatology Project (ISCCP-D2 supplemented by data from the National Centers for Environmental Prediction – National Center for Atmospheric Research (NCEP-NCAR Global Reanalysis project, and other global data bases such as TIROS Operational Vertical Sounder (TOVS and Global Aerosol Data Set (GADS. The model radiative fluxes at TOA were validated against Earth Radiation Budget Experiment (ERBE S4 scanner satellite data (1985–1989. The model is able to predict the seasonal and geographical variation of SW TOA fluxes. On a mean annual and global basis, the model is in very good agreement with ERBE, overestimating the outgoing SW radiation at TOA (OSR by 0.93 Wm-2 (or by 0.92%, within the ERBE uncertainties. At pixel level, the OSR differences between model and ERBE are mostly within ±10 Wm-2, with ±5 Wm-2 over extended regions, while there exist some geographic areas with differences of up to 40 Wm-2, associated with uncertainties in cloud properties and surface albedo. The 14-year average model results give a planetary albedo equal to 29.6% and a TOA OSR flux of 101.2 Wm-2. A significant linearly decreasing trend in OSR and planetary albedo was found, equal to 2.3 Wm-2 and 0.6% (in absolute values, respectively, over the 14-year period (from January 1984 to December 1997, indicating an increasing solar planetary warming. This planetary SW radiative heating occurs in the tropical and sub-tropical areas (20° S–20° N, with clouds being the most likely cause. The computed global mean OSR anomaly ranges within ±4 Wm-2, with signals from El Niño and La Niña events or Pinatubo eruption, whereas significant negative OSR anomalies, starting from year 1992, are also

  2. Activation of sp3-CH Bonds in a Mono(pentamethylcyclopentadienyl)yttrium Complex. X-ray Crystal Structures and Dynamic Behavior of Cp*Y(o-C6H4CH2NMe2)2 and Cp*Y[o-C6H4CH2NMe(CH2-μ)][μ-o-C6H4CH2NMe(CH2-μ)]YCp*[THF

    NARCIS (Netherlands)

    Booij, Martin; Kiers, Niklaas H.; Meetsma, Auke; Teuben, Jan H.; Smeets, Wilberth J.J.; Spek, Anthony L.

    1989-01-01

    Reaction of Y(o-C6H4CH2NMe2)3 (1) with Cp*H gives Cp*Y(o-C6H4CH2NMe2)2 (2), which crystallizes in the monoclinic space group P21/n (No. 14) with a = 18.607 (4) Å, b = 15.633 (3) Å, c = 8.861 (3) Å, β = 102.73 (3)°, and Z = 4. Least-squares refinement with 3006 independent reflections (F > 4.0σ(F))

  3. CH4 and N2O from mechanically turned windrow and vermicomposting systems following in-vessel pre-treatment

    International Nuclear Information System (INIS)

    Hobson, A.M.; Frederickson, J.; Dise, N.B.

    2005-01-01

    Methane (CH 4 ) and nitrous oxide (N 2 O) are included in the six greenhouse gases listed in the Kyoto protocol that require emission reduction. To meet reduced emission targets, governments need to first quantify their contribution to global warming. Composting has been identified as an important source of CH 4 and N 2 O. With increasing divergence of biodegradable waste from landfill into the composting sector, it is important to quantify emissions of CH 4 and N 2 O from all forms of composting and from all stages. This study focuses on the final phase of a two stage composting process and compares the generation and emission of CH 4 and N 2 O associated with two differing composting methods: mechanically turned windrow and vermicomposting. The first stage was in-vessel pre-treatment. Source-segregated household waste was first pre-composted for seven days using an in-vessel system. The second stage of composting involved forming half of the pre-composted material into a windrow and applying half to vermicomposting beds. The duration of this stage was 85 days and CH 4 and N 2 O emissions were monitored throughout for both systems. Waste samples were regularly subjected to respirometry analysis and both processes were found to be equally effective at stabilising the organic matter content. The mechanically turned windrow system was characterised by emissions of CH 4 and to a much lesser extent N 2 O. However, the vermicomposting system emitted significant fluxes of N 2 O and only trace amounts of CH 4 . In-vessel pre-treatment removed considerable amounts of available C and N prior to the second stage of composting. This had the effect of reducing emissions of CH 4 and N 2 O from the second stage compared to emissions from fresh waste found in other studies. The characteristics of each of the two composting processes are discussed in detail. Very different mechanisms for emission of CH 4 and N 2 O are proposed for each system. For the windrow system, development

  4. CO2 and CH4 fluxes from oil palm plantations in Sumatra, Indonesia: effects of palm age and environmental conditions

    Science.gov (United States)

    Meijide, A.; Hassler, E.; Corre, M. D.; June, T.; Sabajo, C.; Veldkamp, E.; Knohl, A.

    2015-12-01

    Global increasing demand of palm oil is leading to the expansion of oil palm plantations, particularly in SE Asia, which in Sumatran lowlands has resulted in a 21% forest area loss. Large photosynthesis rates are expected for oil palms, due to their high growth and yield production. However, there is very limited information on their effect on carbon dioxide (CO2) fluxes and their sink or source strength at ecosystem scale. For methane (CH4) fluxes, research has mainly focused in oil palm plantations located on peatlands, but no information is available at ecosystem level from plantations on mineral soils. With the aim of studying CO2 fluxes during the non-productive and productive phases of oil palm cultivation, an eddy covariance (EC) tower was installed in a 2 year old oil palm plantation, where it was measuring for 8 months, and was subsequently moved to a 12 year old plantation, both in the province of Jambi, Sumatra. The EC system consisted of a Licor 7500A and an ultrasonic Metek anemometer, operating at 10 Hz, installed on a 7m and 22m tower respectively. In the 12 year old plantation, the tower was also equipped with a Los Gatos FGGA-24EP, to assess CH4 fluxes. Chamber measurements were also carried out to obtain information on respiration and CH4 fluxes from the soil. Radiation was the major driver controlling net carbon uptake, while soil moisture did not play a significant role. Average net ecosystem exchange in the hours of the day with higher radiation for the whole measurement period was 10 μmol m-2 s-1 for the 2 year old plantation and -22 μmol m-2 s-1 in the 12 year old. The analysis of the cumulative fluxes show that the non-productive plantation was a carbon source of around 636 g CO2 m-2 during the 8 months of measurements, while in the productive period, it acted as a strong carbon sink (-794 g CO2 m-2 yr-1). Methane uptake was observed in the soil in both plantations and also for the whole ecosystem in the 12 year old one, but its

  5. On the origin and magnitude of pre-industrial anthropogenic CO[sub 2] and CH[sub 4] emissions

    Energy Technology Data Exchange (ETDEWEB)

    Kammen, D.M.; Marino, B.D. (Harvard University, Cambridge, MA (USA). Dept. of Physics)

    Little is known of the origin and magnitude of anthropogenic non-fossil emissions, although this activity currently contributes up to 40% of the global CO[sub 2] emissions. Here we provide estimates of CO[sub 2] and CH[sub 4] emissions resulting from pre-industrial societies by combining historical demographic and archaeological data. Combustion of non-fossil carbon for domestic needs, small-scale industrial/craft activities and resulting from agricultural land management was significant, reaching about 1 Gt of carbon (Gtc) as CO[sub 2] yr[sup -1] and 10 g Tg of carbon CH[sub 4] yr[sup -1] by 1800 A.D. This data implies a significant anthropogenic source of pre-industrial atmospheric greenhouse gases, consistent with estimates derived from carbon cycle model. We illustrate the contribution of archaeological data with two case studies: (1) estimates of CH[sub 4] emissions from agricultural activity from the Maya Lowlands; and (2) evidence of correlations between climatic and socio-economic conditions in North Atlanic Norse settlements. 47 refs., 3 figs., 2 tabs.

  6. Spectrally-resolved UV photodesorption of CH4 in pure and layered ices

    Science.gov (United States)

    Dupuy, R.; Bertin, M.; Féraud, G.; Michaut, X.; Jeseck, P.; Doronin, M.; Philippe, L.; Romanzin, C.; Fillion, J.-H.

    2017-07-01

    Context. Methane is among the main components of the ice mantles of interstellar dust grains, where it is at the start of a rich solid-phase chemical network. Quantification of the photon-induced desorption yield of these frozen molecules and understanding of the underlying processes is necessary to accurately model the observations and the chemical evolution of various regions of the interstellar medium. Aims: This study aims at experimentally determining absolute photodesorption yields for the CH4 molecule as a function of photon energy. The influence of the ice composition is also investigated. By studying the methane desorption from layered CH4:CO ice, indirect desorption processes triggered by the excitation of the CO molecules are monitored and quantified. Methods: Tunable monochromatic vacuum ultraviolet light (VUV) light from the DESIRS beamline of the SOLEIL synchrotron is used in the 7-13.6 eV (177-91 nm) range to irradiate pure CH4 or layers of CH4 deposited on top of CO ice samples. The release of species in the gas phase is monitored by quadrupole mass spectrometry, and absolute photodesorption yields of intact CH4 are deduced. Results: CH4 photodesorbs for photon energies higher than 9.1 eV ( 136 nm). The photodesorption spectrum follows the absorption spectrum of CH4, which confirms a desorption mechanism mediated by electronic transitions in the ice. When it is deposited on top of CO, CH4 desorbs between 8 and 9 eV with a pattern characteristic of CO absorption, indicating desorption induced by energy transfer from CO molecules. Conclusions: The photodesorption of CH4 from pure ice in various interstellar environments is around 2.0 ± 1.0 × 10-3 molecules per incident photon. Results on CO-induced indirect desorption of CH4 provide useful insights for the generalization of this process to other molecules co-existing with CO in ice mantles.

  7. The carbon-budget approach to climate stabilization: Cost-effective subglobal versus global action

    OpenAIRE

    Eichner, Thomas; Pethig, Rüdiger

    2010-01-01

    Scientific expertise suggests that mitigating extreme world-wide climate change damages requires avoiding increases in the world mean temperature exceeding 2 degrees Celsius. To achieve the two degree target, the cumulated global emissions must not exceed some limit, the so-called global carbon budget. In a two-period two country general equilibrium model with a finite stock of fossil fuels we compare the cooperative cost-effective policy with the unilateral cost-effective policy of restricti...

  8. Reconciling uncertainties in integrated science and policy models: Applications to global climate change

    Energy Technology Data Exchange (ETDEWEB)

    Kandlikar, Milind [Carnegie Mellon Univ., Pittsburgh, PA (United States)

    1994-12-01

    In this thesis tools of data reconciliation are used to integrate available information into scientific and policy models of greenhouse gases. The role of uncertainties in scientific and policy models of global climate change is examined, and implications for global change policy are drawn. Methane is the second most important greenhouse gas. Global sources and sinks of methane have significant uncertainties. A chance constrained methodology was developed and used to perform inversions on the global methane cycle. Budgets of methane that are consistent with source fluxes, isotopic and ice core measurements were determined. While it is not possible to come up with a single budget for CH{sub 4}, performing the calculation with a number of sets of assumed priors suggests a convergence in the allowed range for sources. In some cases -- wetlands (70-130 Tg/yr), rice paddies (60-125 Tg/yr) a significant reduction in the uncertainty of the source estimate is achieved. Our results compare favorably with the most recent measurements of flux estimates. For comparison, a similar analysis using bayes monte carlo simulation was performed. The question of the missing sink for carbon remains unresolved. Two analyses that attempt to quantify the missing sink were performed. First, a steady state analysis of the carbon cycle was used to determine the pre-industrial inter-hemispheric carbon concentration gradient. Second, a full blown dynamic inversion of the carbon cycle was performed. An advection diffusion ocean model with surface chemistry, coupled to box models of the atmosphere and the biosphere was inverted to fit available measurements of {sup 12}C and {sup 14}C carbon isotopes using Differential-Algebraic Optimization. The model effectively suggests that the {open_quotes}missing{close_quotes} sink for carbon is hiding in the biosphere. Scenario dependent trace gas indices were calculated for CH{sub 4}, N{sub 2}O, HCFC-22.

  9. A combustion setup to precisely reference δ13C and δ2H isotope ratios of pure CH4 to produce isotope reference gases of δ13C-CH4 in synthetic air

    Directory of Open Access Journals (Sweden)

    H. Schaefer

    2012-09-01

    Full Text Available Isotope records of atmospheric CH4 can be used to infer changes in the biogeochemistry of CH4. One factor currently limiting the quantitative interpretation of such changes are uncertainties in the isotope measurements stemming from the lack of a unique isotope reference gas, certified for δ13C-CH4 or δ2H-CH4. We present a method to produce isotope reference gases for CH4 in synthetic air that are precisely anchored to the VPDB and VSMOW scales and have δ13C-CH4 values typical for the modern and glacial atmosphere. We quantitatively combusted two pure CH4 gases from fossil and biogenic sources and determined the δ13C and δ2H values of the produced CO2 and H2O relative to the VPDB and VSMOW scales within a very small analytical uncertainty of 0.04‰ and 0.7‰, respectively. We found isotope ratios of −39.56‰ and −56.37‰ for δ13C and −170.1‰ and −317.4‰ for δ2H in the fossil and biogenic CH4, respectively. We used both CH4 types as parental gases from which we mixed two filial CH4 gases. Their δ13C was determined to be −42.21‰ and −47.25‰ representing glacial and present atmospheric δ13C-CH4. The δ2H isotope ratios of the filial CH4 gases were found to be −193.1‰ and −237.1‰, respectively. Next, we mixed aliquots of the filial CH4 gases with ultrapure N2/O2 (CH4 ≤ 2 ppb producing two isotope reference gases of synthetic air with CH4 mixing ratios near atmospheric values. We show that our method is reproducible and does not introduce isotopic fractionation for δ13C within the uncertainties of our detection limit (we cannot conclude this for δ2H because our system is currently not prepared for δ2H-CH4 measurements in air samples. The general principle of our method can be applied to produce synthetic isotope reference gases targeting δ2H-CH4 or other gas species.

  10. A new metal-organic framework for separation of C2H2/CH4 and CO2/CH4 at room temperature

    Science.gov (United States)

    Duan, Xing; Zhou, You; Lv, Ran; Yu, Ben; Chen, Haodong; Ji, Zhenguo; Cui, Yuanjing; Yang, Yu; Qian, Guodong

    2018-04-01

    A 3D microporous metal-organic framework with open Cu2+ sites and suitable pore space, [Cu2(L)(H2O)2]·(H2O)4(DMF)8 (ZJU-15, H4L = 5,5‧-(9H-carbazole-2,7-diyl)diisophthalic acid; DMF = N,N-dimethylformamide; ZJU = Zhejiang University), has been constructed and characterized. The activated ZJU-15a has three different types of cages and exhibits BET surface area of 1660 m2 g-1, and can separate gas mixture of C2H2/CH4 and CO2/CH4 at room temperature.

  11. Time-series measurements of methane (CH4) distribution during open water and ice-cover in lakes throughout the Mackenzie River Delta (Canada)

    Science.gov (United States)

    McIntosh, H.; Lapham, L.; Orcutt, B.; Wheat, C. G.; Lesack, L.; Bergstresser, M.; Dallimore, S. R.; MacLeod, R.; Cote, M.

    2016-12-01

    Arctic lakes are known to emit large amounts of methane to the atmosphere and their importance to the global methane (CH4) cycle has been recognized. It is well known CH4 builds up in Arctic lakes during ice-cover, but the amount of and when the CH4 is released to the atmosphere is not well known. Our preliminary results suggest the largest flux of CH4 from lakes to the atmosphere occurs slightly before complete ice-out; while others have shown the largest flux occurs when lakes overturn in the spring. During ice-out, CH4 can also be oxidized by methane oxidizing bacteria before it can efflux to the atmosphere from the surface water. In order to elucidate the processes contributing to Arctic lake CH4 emissions, continuous, long-term and large scale spatial sampling is required; however it is difficult to achieve in these remote locations. We address this problem using two sampling techniques. 1) We deployed osmotically powered pumps (OsmoSamplers), which were able to autonomously and continuously collect lake bottom water over the course of a year from multiple lakes in the Mackenzie River Delta. OsmoSamplers were placed in four lakes in the mid Delta near Inuvik, Northwest Territories, Canada, two lakes in the outer Delta, and two coastal lakes on Richard's Island in 2015. The dissolved CH4 concentration, stable isotope content of CH4 (δ13C-CH4), and dissolved sulfate concentrations in bottom water from these lakes will be presented to better understand methane dynamics under the ice and over time. 2) Along with the time-series data, we will also present data from discrete samples collected from 40 lakes in the mid Delta during key time periods, before and immediately after the spring ice-out. By determining the CH4 dynamics throughout the year we hope to improve predictions of how CH4 emissions may change in a warming Arctic environment.

  12. Additional Value of CH4 Measurement in a Combined 13C/H2 Lactose Malabsorption Breath Test: A Retrospective Analysis

    Science.gov (United States)

    Houben, Els; De Preter, Vicky; Billen, Jaak; Van Ranst, Marc; Verbeke, Kristin

    2015-01-01

    The lactose hydrogen breath test is a commonly used, non-invasive method for the detection of lactose malabsorption and is based on an abnormal increase in breath hydrogen (H2) excretion after an oral dose of lactose. We use a combined 13C/H2 lactose breath test that measures breath 13CO2 as a measure of lactose digestion in addition to H2 and that has a better sensitivity and specificity than the standard test. The present retrospective study evaluated the results of 1051 13C/H2 lactose breath tests to assess the impact on the diagnostic accuracy of measuring breath CH4 in addition to H2 and 13CO2. Based on the 13C/H2 breath test, 314 patients were diagnosed with lactase deficiency, 138 with lactose malabsorption or small bowel bacterial overgrowth (SIBO), and 599 with normal lactose digestion. Additional measurement of CH4 further improved the accuracy of the test as 16% subjects with normal lactose digestion and no H2-excretion were found to excrete CH4. These subjects should have been classified as subjects with lactose malabsorption or SIBO. In conclusion, measuring CH4-concentrations has an added value to the 13C/H2 breath test to identify methanogenic subjects with lactose malabsorption or SIBO. PMID:26371034

  13. Experimental ion mobility measurements in Xe-CH4

    Science.gov (United States)

    Perdigoto, J. M. C.; Cortez, A. F. V.; Veenhof, R.; Neves, P. N. B.; Santos, F. P.; Borges, F. I. G. M.; Conde, C. A. N.

    2017-09-01

    Data on ion mobility is important to improve the performance of large volume gaseous detectors. In the present work, the method, experimental setup and results for the ion mobility measurements in Xe-CH4 mixtures are presented. The results for this mixture show the presence of two distinct groups of ions. The nature of the ions depend on the mixture ratio since they are originated by both Xe and CH4. The results here presented were obtained for low reduced electric fields, E/N, 10-25 Td (2.4-6.1 kV ṡ cm-1 ṡ bar-1), at low pressure (8 Torr) (10.6 mbar), and at room temperature.

  14. Macromolecule simulation and CH4 adsorption mechanism of coal vitrinite

    Science.gov (United States)

    Yu, Song; Yan-ming, Zhu; Wu, Li

    2017-02-01

    The microscopic mechanism of interactions between CH4 and coal macromolecules is of significant practical and theoretical importance in CBM development and methane storage. Under periodic boundary conditions, the optimal energy configuration of coal vitrinite, which has a higher torsion degree and tighter arrangement, can be determined by the calculation of molecular mechanics (MM) and molecular dynamics (MD), and annealing kinetics simulation based on ultimate analysis, 13C NMR, FT IR and HRTEM. Macromolecular stabilization is primarily due to the van der Waals energy and covalent bond energy, mainly consisting of bond torsion energy and bond angle energy. Using the optimal configuration as the adsorbent, GCMC simulation of vitrinite adsorption of CH4 is conducted. A saturated state is reached after absorbing 17 CH4s per coal vitrinite molecule. CH4 is preferentially adsorbed on the edge, and inclined to gathering around the branched chains of the inner vitrinite sites. Finally, the adsorption parameters are calculated through first principle DFT. The adsorbability order is as follows: aromatic structure> heteroatom rings > oxygen functional groups. The adsorption energy order is as follows: Top graphene. However, the energy of the most preferential location is much lower than that of graphite/graphene. CH4 is more easily absorbed on the surface of vitrinite. Adsorbability varies considerably at different adsorption locations and sites on the surface of vitrinite. Crystal parameter of vitrinite is a = b = c = 15.8 Å and majority of its micropores are blow 15.8 Å, indicating that the vitrinite have the optimum adsorption aperture. It can explain its higher observed adsorption capacities for CH4 compared with graphite/graphene.

  15. Evaluation of origins of CH4 carbon emitted from rice paddies

    Science.gov (United States)

    Watanabe, Akira; Takeda, Takuya; Kimura, Makoto

    1999-10-01

    Possible carbon sources for CH4 emitted from rice paddies are organic matter applied to the fields, such as rice straw (RS), soil organic matter (SOM), and carbon supplied from rice plants (RP), such as exudates and sloughed tissues. To estimate the contribution of each carbon source to CH4 emission, a pot experiment was conducted using 13C-enriched soil sample and 13C-enriched RS as tracers. The percentage contribution of RP carbon was estimated by subtraction. When RS was applied at a rate corresponding to 6 t ha-1, the percentage contributions of RS, SOM, and RP carbon to CH4 emission throughout the period of rice growth were 42%, 18-21%, and 37-40%, respectively. The values for SOM and RP carbon for the treatment in which RS was not applied were 15-20% and 80-85%, respectively. Seasonal variations in the percentage contribution of soil organic carbon to CH4 emission were small in the range between 13% and 30% for the pots with RS and between 15% and 24% for the pots without RS. In the RS-applied treatment, RS and SOM accounted for almost 100% of the CH4 carbon early in the period of rice growth, while 65-70% of the CH4 emission in the milky stage was derived from RP carbon.

  16. Occurrence of greenhouse gases (CO2, N2O and CH4) in groundwater of the Walloon Region (Belgium).

    Science.gov (United States)

    Jurado, Anna; Borges, Alberto V.; Pujades, Estanislao; Hakoun, Vivien; Knöller, Kay; Brouyère, Serge

    2017-04-01

    Greenhouse gases (GHGs) are an environmental problem because their concentrations in the atmosphere have continuously risen since the industrial revolution. They can be indirectly transferred to the atmosphere through groundwater discharge into surface water bodies such as rivers. However, their occurrence is poorly evaluated in groundwater. The aim of this work is to identify the hydrogeological contexts (e.g., chalk and limestone aquifers) and the most conductive conditions for the generation of GHGs in groundwater at a regional scale. To this end, carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O) concentrations, major and minor elements and environmental isotopes were monitored in several groundwater bodies of the Walloon Region (Belgium) from September 2014 to June 2016. The concentrations of GHGs in groundwater ranged from 1769 to 100519 ppm for the partial pressure of CO2 and from 0 to 1064 nmol/L and 1 to 37062 nmol/L for CH4 and N2O respectively. Overall, groundwater was supersaturated in GHGs with respect to atmospheric equilibrium, suggesting that groundwater contribute to the atmospheric GHGs budget. Prior inspection of the data suggested that N2O in groundwater can be produced by denitrification and nitrification. The most suitable conditions for the accumulation of N2O are promoted by intermediate dissolved oxygen concentrations (2.5-3 mg L-1) and the availability of nitrate (NO3-). These observations will be compared with the isotopes of NO3-. CH4 was less detected and at lower concentration than N2O, suggesting that groundwater redox conditions are not reducing enough to promoted the production of CH4. The results will be presented and discussed in detail in the presentation.

  17. A cool-temperate young larch plantation as a net methane source - A 4-year continuous hyperbolic relaxed eddy accumulation and chamber measurements

    Science.gov (United States)

    Ueyama, Masahito; Yoshikawa, Kota; Takagi, Kentaro

    2018-07-01

    Upland forests are thought to be methane (CH4) sinks due to oxidation by methanotrophs in aerobic soils. However, CH4 budget for upland forests are not well quantified at the ecosystem scale, when possible CH4 sources, such as small wet areas, exists in the ecosystem. Here, we quantified CH4 fluxes in a cool-temperate larch plantation based on four-year continuous measurements using the hyperbolic relaxed eddy accumulation (HREA) method and dynamic closed chambers with a laser-based analyzer. After filling data gaps for half-hourly data using machine-learning-based regressions, we found that the forest acted as a net CH4 source at the canopy scale: 30 ± 11 mg CH4 m-2 yr-1 in 2014, 56 ± 8 mg CH4 m-2 yr-1 in 2015, 154 ± 5 mg CH4 m-2 yr-1 in 2016, and 132 ± 6 mg CH4 m-2 yr-1 in 2017. Hotspot emissions from the edge of the pond could strongly contribute to the canopy-scale emissions. The magnitude of the hotspot emissions was 10-100 times greater than the order of the canopy-scale and chamber-based CH4 fluxes at the dry soils. The high temperatures with wet conditions stimulated the hotspot emissions, and thus induced canopy-scale CH4 emissions in the summer. Understanding and modeling the dynamics of hotspot emissions are important for quantifying CH4 budgets of upland forests. Micrometeorological measurements at various forests are required for revisiting CH4 budget of upland forests.

  18. Dielectric Study of the Phase Transitions in [P(CH3)4]2CuY4 (Y = Cl, Br)

    Science.gov (United States)

    Gesi, Kazuo

    2002-05-01

    Phase transitions in [P(CH3)4]2CuY4 (Y = Cl, Br) have been studied by dielectric measurements. In [P(CH3)4]2CuCl4, a slight break and a discontinuous jump on the dielectric constant vs. temperature curve are seen at the normal-incommensurate and the incommensurate-commensurate phase transitions, respectively. A small peak of dielectric constant along the b-direction exists just above the incommensurate-to-commensurate transition temperature. The anisotropic dielectric anomalies of [P(CH3)4]2CuBr4 at phase transitions were measured along the three crystallographic axes. The pressure-temperature phase diagram of [P(CH3)4]2CuCl4 was determined. The initial pressure coefficients of the normal-to-incommensurate and the incommensurate-to-commensurate transition temperatures are 0.19 K/MPa and 0.27 K/MPa, respectively. The incommensurate phase in [P(CH3)4]2CuCl4 disappears at a triple point which exists at 335 MPa and 443 K. The stability and the pressure effects of the incommensurate phases are much different among the four [Z(CH3)4]2CuY4 crystals (Z = N, P; Y = Cl, Br).

  19. Assessing fugitive emissions of CH4 from high-pressure gas pipelines

    Science.gov (United States)

    Worrall, Fred; Boothroyd, Ian; Davies, Richard

    2017-04-01

    The impact of unconventional natural gas production using hydraulic fracturing methods from shale gas basins has been assessed using life-cycle emissions inventories, covering areas such as pre-production, production and transmission processes. The transmission of natural gas from well pad to processing plants and its transport to domestic sites is an important source of fugitive CH4, yet emissions factors and fluxes from transmission processes are often based upon ver out of date measurements. It is important to determine accurate measurements of natural gas losses when compressed and transported between production and processing facilities so as to accurately determine life-cycle CH4 emissions. This study considers CH4 emissions from the UK National Transmission System (NTS) of high pressure natural gas pipelines. Mobile surveys of CH4 emissions using a Picarro Surveyor cavity-ring-down spectrometer were conducted across four areas in the UK, with routes bisecting high pressure pipelines and separate control routes away from the pipelines. A manual survey of soil gas measurements was also conducted along one of the high pressure pipelines using a tunable diode laser. When wind adjusted 92 km of high pressure pipeline and 72 km of control route were drive over a 10 day period. When wind and distance adjusted CH4 fluxes were significantly greater on routes with a pipeline than those without. The smallest leak detectable was 3% above ambient (1.03 relative concentration) with any leaks below 3% above ambient assumed ambient. The number of leaks detected along the pipelines correlate to the estimated length of pipe joints, inferring that there are constant fugitive CH4 emissions from these joints. When scaled up to the UK's National Transmission System pipeline length of 7600 km gives a fugitive CH4 flux of 4700 ± 2864 kt CH4/yr - this fugitive emission from high pressure pipelines is 0.016% of the annual gas supply.

  20. High temporal resolution ecosystem CH4, CO2 and H2O flux data measured with a novel chamber technique

    Science.gov (United States)

    Steenberg Larsen, Klaus; Riis Christiansen, Jesper

    2016-04-01

    Soil-atmosphere exchange of greenhouse gases (GHGs) is commonly measured with closed static chambers (Pihlatie et al., 2013) with off-site gas chromatographic (GC) analysis for CH4 and N2O. Static chambers are widely used to observe in detail the effect of experimental manipulations, like climate change experiments, on GHG exchange (e.g. Carter et al., 2012). However, the low sensitivity of GC systems necessitates long measurement times and manual sampling, which increases the disturbance of the exchange of GHGs and leads to potential underestimation of fluxes (Christiansen et al., 2011; Creelman et al., 2013). The recent emergence of field proof infrared lasers using cavity ring-down spectroscopy (CRDS) have increased frequency and precision of concentration measurements and enabled better estimates of GHG fluxes (Christiansen et al., 2015) due to shorter chamber enclosure times. This minimizes the negative impact of the chamber enclosure on the soil-atmosphere gas exchange rate. Secondly, an integral aspect of understanding GHG exchange in terrestrial ecosystem is to achieve high temporal coverage. This is needed to capture the often dynamic behavior where fluxes can change rapidly over the course of days or even a few hours in response to e.g. rain events. Consequently, low temporal coverage in measurements of GHG exchange have in many past investigations led to highly uncertain annual budgets which severely limits our understanding of the ecosystem processes interacting with the climate system through GHG exchange. Real-time field measurements at high temporal resolution are needed to obtain a much more detailed understanding of the processes governing ecosystem CH4 exchange as well as for better predicting the effects of climate and environmental changes. We combined a state-of-the-art field applicable CH4 sensor (Los Gatos UGGA) with a newly developed ecosystem-level automatic chamber controlled by a LI-COR 8100/8150 system. The chamber is capable of

  1. Hydrogenation of organic matter as a terminal electron sink sustains high CO 2 :CH 4 production ratios during anaerobic decomposition

    Energy Technology Data Exchange (ETDEWEB)

    Wilson, Rachel M.; Tfaily, Malak M.; Rich, Virginia I.; Keller, Jason K.; Bridgham, Scott D.; Zalman, Cassandra Medvedeff; Meredith, Laura; Hanson, Paul J.; Hines, Mark; Pfeifer-Meister, Laurel; Saleska, Scott R.; Crill, Patrick; Cooper, William T.; Chanton, Jeff P.; Kostka, Joel E.

    2017-10-01

    Once inorganic electron acceptors are depleted, organic matter in anoxic environments decomposes by hydrolysis, fermentation, and methanogenesis, requiring syntrophic interactions between microorganisms to achieve energetic favorability. In this classic anaerobic food chain, methanogenesis represents the terminal electron accepting (TEA) process, ultimately producing equimolar CO2 and CH4 for each molecule of organic matter degraded. However, CO2:CH4 production in Sphagnum-derived, mineral-poor, cellulosic peat often substantially exceeds this 1:1 ratio, even in the absence of measureable inorganic TEAs. Since the oxidation state of C in both cellulose-derived organic matter and acetate is 0, and CO2 has an oxidation state of +4, if CH4 (oxidation state -4) is not produced in equal ratio, then some other compound(s) must balance CO2 production by receiving 4 electrons. Here we present evidence for ubiquitous hydrogenation of diverse unsaturated compounds that appear to serve as organic TEAs in peat, thereby providing the necessary electron balance to sustain CO2:CH4 >1. While organic electron acceptors have previously been proposed to drive microbial respiration of organic matter through the reversible reduction of quinone moieties, the hydrogenation mechanism that we propose, by contrast, reduces C-C double bonds in organic matter thereby serving as 1) a terminal electron sink, 2) a mechanism for degrading complex unsaturated organic molecules, 3) a potential mechanism to regenerate electron-accepting quinones, and, in some cases, 4) a means to alleviate the toxicity of unsaturated aromatic acids. This mechanism for CO2 generation without concomitant CH4 production has the potential to regulate the global warming potential of peatlands by elevating CO2:CH4 production ratios.

  2. Effects of elevated ozone concentration on CH4 and N2O emission from paddy soil under fully open-air field conditions.

    Science.gov (United States)

    Tang, Haoye; Liu, Gang; Zhu, Jianguo; Kobayashi, Kazuhiko

    2015-04-01

    We investigated the effects of elevated ozone concentration (E-O3) on CH4 and N2O emission from paddies with two rice cultivars: an inbred Indica cultivar Yangdao 6 (YD6) and a hybrid one II-you 084 (IIY084), under fully open-air field conditions in China. A mean 26.7% enhancement of ozone concentration above the ambient level (A-O3) significantly reduced CH4 emission at tillering and flowering stages leading to a reduction of seasonal integral CH4 emission by 29.6% on average across the two cultivars. The reduced CH4 emission is associated with O3-induced reduction in the whole-plant biomass (-13.2%), root biomass (-34.7%), and maximum tiller number (-10.3%), all of which curbed the carbon supply for belowground CH4 production and its release from submerged soil to atmosphere. Although no significant difference was detected between the cultivars in the CH4 emission response to E-O3, a larger decrease in CH4 emission with IIY084 (-33.2%) than that with YD6 (-7.0%) was observed at tillering stage, which may be due to the larger reduction in tiller number in IIY084 by E-O3. Additionally, E-O3 reduced seasonal mean NOx flux by 5.7% and 11.8% with IIY084 and YD6, respectively, but the effects were not significant statistically. We found that the relative response of CH4 emission to E-O3 was not significantly different from those reported in open-top chamber experiments. This study has thus confirmed that increasing ozone concentration would mitigate the global warming potential of CH4 and suggested consideration of the feedback mechanism between ozone and its precursor emission into the projection of future ozone effects on terrestrial ecosystem. © 2014 John Wiley & Sons Ltd.

  3. Full accounting of the greenhouse gas (CO2, N2O, CH4) budget of nine European grassland sites

    DEFF Research Database (Denmark)

    Soussana, J.E.; Allard, V.; Pilegaard, Kim

    2007-01-01

    The full greenhouse gas balance of nine contrasted grassland sites covering a major climatic gradient over Europe was measured during two complete years. The sites include a wide range of management regimes (rotational grazing, continuous grazing and mowing), the three main types of managed......, automated chambers and tunable diode laser) and CH4 emissions resulting from enteric fermentation of the grazing cattle were measured in situ at four sites using the SF6 tracer method. Averaged over the two measurement years, net ecosystem exchange (NEE) results show that the nine grassland plots displayed...

  4. Vibrational transition moments of CH4 from first principles

    Science.gov (United States)

    Yurchenko, Sergei N.; Tennyson, Jonathan; Barber, Robert J.; Thiel, Walter

    2013-09-01

    New nine-dimensional (9D), ab initio electric dipole moment surfaces (DMSs) of methane in its ground electronic state are presented. The DMSs are computed using an explicitly correlated coupled cluster CCSD(T)-F12 method in conjunction with an F12-optimized correlation consistent basis set of the TZ-family. A symmetrized molecular bond representation is used to parameterise these 9D DMSs in terms of sixth-order polynomials. Vibrational transition moments as well as band intensities for a large number of IR-active vibrational bands of 12CH4 are computed by vibrationally averaging the ab initio dipole moment components. The vibrational wavefunctions required for these averages are computed variationally using the program TROVE and a new ‘spectroscopic’ 12CH4 potential energy surface. The new DMSs will be used to produce a hot line list for 12CH4.

  5. Windrow composting mitigated CH4 emissions: characterization of methanogenic and methanotrophic communities in manure management.

    Science.gov (United States)

    Chen, Ruirui; Wang, Yiming; Wei, Shiping; Wang, Wei; Lin, Xiangui

    2014-12-01

    With increasing livestock breeding, methane (CH4 ) emissions from manure management will increasingly contribute more to atmospheric CH4 concentration. The dynamics of methanogens and methanotrophs have not yet been studied in the manure environment. The current study combines surface CH4 emissions with methanogenic and methanotrophic community analyses from two management practices, windrow composting (WCOM) and solid storage (SSTO). Our results showed that there was an c. 50% reduction of CH4 emissions with WCOM compared with SSTO over a 50-day period. A sharp decrease in the quantities of both methanogens and methanotrophs in WCOM suggested that CH4 mitigation was mainly due to decreased CH4 production rather than increased CH4 oxidation. Pyrosequencing analysis demonstrated that aeration caused a clear shift of dominant methanogens in the manure, with specifically a significant decrease in Methanosarcina and increase in Methanobrevibacter. The composition of methanogenic community was influenced by manure management and regulated CH4 production. A sharp increase in the quantity of methanotrophs in SSTO suggested that microbial CH4 oxidation is an important sink for the CH4 produced. The increased abundance of Methylococcaceae in SSTO suggested that Type I methanotrophs have an advantage in CH4 oxidation in occupying niches under low CH4 and high O2 conditions. © 2014 Federation of European Microbiological Societies. Published by John Wiley & Sons Ltd. All rights reserved.

  6. Effects of Boreal Lake Wetlands on Atmospheric 13CH3D and 12CH2D2

    Science.gov (United States)

    Haghnegahdar, M. A.; Kohl, I. E.; Schauble, E. A.; Walter Anthony, K. M.; Young, E. D.

    2017-12-01

    Recently, we developed a theoretical model to investigate the potential use of 13CH3D and 12CH2D2 as tools for tracking atmospheric methane budget. We used electronic structure methods to estimate kinetic isotope fractionations associated with the major sink reactions of CH4 in air (reactions with •OH and Cl•), and literature data with reconnaissance measurements of the relative abundances of 13CH3D and 12CH2D2 to estimate the compositions of the largest atmospheric sources. Here we present new methane rare isotopologue data from boreal wetlands, comprising one of the most important sources, in order to evaluate the robustness of the model. Boreal wetlands (>55° N) account for more than half of the wetland area in the Northern hemisphere. We analyzed methane samples from high latitude lakes representing different geographical regions, geological and ecological contexts, methane fluxes, and isotopic signatures. Using clumped isotopes of CH4 we are able to determine the likely production mechanism for natural CH4 samples. So far, all of our analyzed samples except one plot in the microbial pure-culture methanogenesis field (Young et al. 2017) with ranges of -0.2‰ to +1.2‰ for Δ13CH3D, and -29.6‰ to -18.2‰ for Δ12CH2D2. These compositions are far from equilibrium. The one exception, from Lake Doughnut, Alaska, exhibits Δ13CH3D and Δ12CH2D2 values of +5.2‰ and +18.7‰, respectively, which fall near ambient thermodynamic equilibrium values. This may be an effect of methanotrophy. Mean Δ13CH3D and Δ12CH2D2 for all lake samples are +1.7‰ and -15.4‰ respectively, compared to our original estimate of +6.1‰ and +21.2‰ for the wetland methane source based on an assumption of equilibrium. If we assume that these samples are representative of the overall wetland source, Δ13CH3D decreases by 0.8‰ and Δ12CH2D2 decreases by 0.6‰ in our model of bulk atmospheric methane. Δ13CH3D and Δ12CH2D2 values of air (including •OH and Cl• sink

  7. OH vibrational activation and decay dynamics of CH4-OH entrance channel complexes

    International Nuclear Information System (INIS)

    Wheeler, Martyn D.; Tsiouris, Maria; Lester, Marsha I.; Lendvay, Gyoergy

    2000-01-01

    Infrared spectroscopy has been utilized to examine the structure and vibrational decay dynamics of CH 4 -OH complexes that have been stabilized in the entrance channel to the CH 4 +OH hydrogen abstraction reaction. Rotationally resolved infrared spectra of the CH 4 -OH complexes have been obtained in the OH fundamental and overtone regions using an IR-UV (infrared-ultraviolet) double-resonance technique. Pure OH stretching bands have been identified at 3563.45(5) and 6961.98(4) cm-1 (origins), along with combination bands involving the simultaneous excitation of OH stretching and intermolecular bending motions. The infrared spectra exhibit extensive homogeneous broadening arising from the rapid decay of vibrationally activated CH 4 -OH complexes due to vibrational relaxation and/or reaction. Lifetimes of 38(5) and 25(3) ps for CH 4 -OH prepared with one and two quanta of OH excitation, respectively, have been extracted from the infrared spectra. The nascent distribution of the OH products from vibrational predissociation has been evaluated by ultraviolet probe laser-induced fluorescence measurements. The dominant inelastic decay channel involves the transfer of one quantum of OH stretch to the pentad of CH 4 vibrational states with energies near 3000 cm-1. The experimental findings are compared with full collision studies of vibrationally excited OH with CH 4 . In addition, ab initio electronic structure calculations have been carried out to elucidate the minimum energy configuration of the CH 4 -OH complex. The calculations predict a C 3v geometry with the hydrogen of OH pointing toward one of four equivalent faces of the CH 4 tetrahedron, consistent with the analysis of the experimental infrared spectra. (c) 2000 American Institute of Physics

  8. Effect of antisymmetric C–H stretching excitation on the dynamics of O({sup 1}D) + CH{sub 4} → OH + CH{sub 3}

    Energy Technology Data Exchange (ETDEWEB)

    Pan, Huilin; Yang, Jiayue; Zhang, Dong; Shuai, Quan; Jiang, Bo [State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023 (China); Dai, Dongxu; Wu, Guorong, E-mail: wugr@dicp.ac.cn, E-mail: xmyang@dicp.ac.cn; Yang, Xueming, E-mail: wugr@dicp.ac.cn, E-mail: xmyang@dicp.ac.cn [State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023 (China); Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026 (China)

    2014-04-21

    The effect of antisymmetric C–H stretching excitation of CH{sub 4} on the dynamics and reactivity of the O({sup 1}D) + CH{sub 4} → OH + CD{sub 3} reaction at the collision energy of 6.10 kcal/mol has been investigated using the crossed-beam and time-sliced velocity map imaging techniques. The antisymmetric C–H stretching mode excited CH{sub 4} molecule was prepared by direct infrared excitation. From the measured images of the CH{sub 3} products with the infrared laser on and off, the product translational energy and angular distributions were derived for both the ground and vibrationally excited reactions. Experimental results show that the vibrational energy of the antisymmetric stretching excited CH{sub 4} reagent is channeled exclusively into the vibrational energy of the OH co-products and, hence, the OH products from the excited-state reaction are about one vibrational quantum hotter than those from the ground-state reaction, and the product angular distributions are barely affected by the vibrational excitation of the CH{sub 4} reagent. The reactivity was found to be suppressed by the antisymmetric stretching excitation of CH{sub 4} for all observed CH{sub 3} vibrational states. The degree of suppression is different for different CH{sub 3} vibrational states: the suppression is about 40%–60% for the ground state and the umbrella mode excited CH{sub 3} products, while for the CH{sub 3} products with one quantum symmetric stretching mode excitation, the suppression is much less pronounced. In consequence, the vibrational state distribution of the CH{sub 3} product from the excited-state reaction is considerably different from that of the ground-state reaction.

  9. The role of boreal forests and forestry in the global carbon budget : a synthesis

    Energy Technology Data Exchange (ETDEWEB)

    Fyles, I.H.; Shaw, C.H.; Apps, M.J.; Karjalainen, T.; Stocks, B.J.; Running, S.W.; Kurz, W.A.; Weyerhaeuser, G.Jr.; Jarvis, P.G.

    2002-10-01

    This paper provides a synthesis of all papers presented at the conference on the role of boreal forests in the global carbon budget. The scientific community is recognizing the critical links between boreal forest ecosystems, carbon dynamics and global climate change. This paper addresses the five main topics discussed at the conference including: (1) carbon stocks and fluxes, (2) the effects of natural disturbances on carbon dynamics, (3) effects of management practices on carbon dynamics, (4) afforestation and carbon sequestration, and (5) effects of climate change and elevated carbon dioxide concentration on carbon dynamics. Large-scale model simulations suggest that increased global temperatures will result in increased net ecosystem productivity (NEP). Several model simulations also indicate that net primary productivity (NPP) will increase. While most forest stands are currently carbon sinks, disturbances such as fire, insects and tree harvesting make forests susceptible to becoming a source of carbon. In contrast, some studies suggest that climate change will cause shifting vegetation patterns, increased soil carbon and higher forest productivity that may result in higher sequestration of carbon in the boreal forest. 84 refs.

  10. A Stable U Isotopic Perspective on the U Budget and Global Extent of Modern Anoxia in the Ocean.

    Science.gov (United States)

    Tissot, F.; Dauphas, N.

    2015-12-01

    Isotopic fractionation between U4+ and U6+makes U stable isotopes potential tracers of global paleoredox conditions. In this work [1], we put the U-proxy up to a test against a highly constrained system: the modern ocean. We measured a large number of seawater samples from geographically diverse locations and found that the open ocean has a homogenous isotopic composition at δ238USW= -0.392 ± 0.005 ‰ (rel. to CRM-112a). From our measurement of rock samples (n=64) and compilations of literature data (n=380), we then estimated the U isotopic compositions of the various reservoirs involved in the modern oceanic U budget, as well as the fractionation factors associated with U incorporation into those reservoirs. Using a steady-state model, we compared the isotopic composition of the seawater predicted by the four most recent U oceanic budgets [2-5] to the modern seawater value we measured. Three of these budgets [2-4] predict a seawater isotopic composition in very good agreement with the observed δ238USW, which strengthens our confidence in the isotopic fractionation factors associated with each deposition environment and the fact that U is at steady-state in the modern ocean. The U oceanic budget of Henderson and Anderson (2003) does not reproduce the observed seawater composition because the U flux to anoxic/euxinic sediments relative to the total U flux out of the ocean is high in their model, which our analysis shows cannot be correct. The U isotopic composition of seawater is used to constrain the extent of anoxia in the modern ocean (% of seafloor covered by anoxic/euxinic sediments), which is 0.21 ± 0.09 %. This work demonstrates that stable isotopes of U can indeed trace the extent of anoxia in the modern global ocean, thereby validating the application of U isotope measurements to paleoredox reconstructions. Based on the above work, we will present the best estimate of the modern oceanic U budget. [1] Tissot F.L.H., Dauphas N. (2015) Geochim Cosmochim

  11. Influence of O_2 exposure on the interaction between CH_4 and amorphous AlYB_1_4

    International Nuclear Information System (INIS)

    Hunold, Oliver; Wiesing, Martin; Arcos, Teresa de los; Music, Denis; Grundmeier, Guido; Schneider, Jochen M.

    2017-01-01

    Highlights: • Influence of O_2 exposure on the surface chemistry of a-AlYB_1_4 on the interaction with CH_4 and PE studied by ab initio and UHV-AFM. • Predicted stronger interaction is consistent with experimentally observed trends. • Upon O_2 exposure surface bonding becomes more semiconducting causing a charge redistribution within the adsorbed CH_4 molecule. • The data serve as proof of concept for exploring polymer − hard coating interactions in varying atmospheres. - Abstract: The influence of surface oxidation on the interaction between CH_4 and amorphous AlYB_1_4 (a-AlYB_1_4) has been studied theoretically by using density functional theory and experimentally by ultra-high vacuum atomic force microscopy (UHV-AFM). CH_4 mimics the –CH_3 termination and aliphatic subunits of a polymer chain. Low-energy ion scattering measurements of magnetron sputtered thin films suggest that the bonding at the surfaces of pristine a-AlYB_1_4 and O_2 exposed a-AlYB_1_4 (O_2//a-AlYB_1_4) is metal-boron and metal-oxygen dominated, respectively. Based on the ab initio calculations the adsorption energies of CH_4 on a-AlYB_1_4 and O_2//a-AlYB_1_4 decreases from −0.07 to −0.30 eV, respectively. This trend is consistent with experimental data obtained by colloidal probe UHV-AFM studies with a polyethylene sphere, where larger adhesion forces for the O_2 exposed surface as compared to the pristine a-AlYB_1_4 surface were measured. No charge transfer takes place between CH_4 and the pristine as well as the O_2 exposed a-AlYB_1_4. Oxygen chemisorption induces changes in surface bonding. States at the Fermi level are depleted upon oxidation, hence the surface bonding becomes more semiconducting causing a charge redistribution within the adsorbed CH_4 molecule. Hence, these data serve as proof of concept for exploring the effect of O_2 exposure on the interaction between aliphatic polymers and a-AlYB_1_4 using a correlative experimental and theoretical research approach.

  12. Effects of experimental warming and nitrogen addition on soil respiration and CH4 fluxes from crop rotations of winter wheat–soybean/fallow

    DEFF Research Database (Denmark)

    Liu, L; Hu, C; Yang, P

    2015-01-01

    Soil respiration and CH4 emissions play a significant role in the global carbon balance. However, in situ studies in agricultural soils on responses of soil respiration and CH4 fluxes to climate warming are still sparse, especially from long-term studies with year-round heating. A warming...... by affecting soil NH4 concentration. Across years, CH4 emissions were negatively correlated with soil temperature in N1 treatment. Soil respiration showed clear seasonal fluctuations, with the largest emissions during summer and smallest in winter. Warming and nitrogen fertilization had no significant effects...... on total cumulative soil CO2 fluxes. Soil respiration was positively correlated with microbial biomass C, and microbial biomass C was not affected significantly by warming or nitrogen addition. The lack of significant effects of warming on soil respiration may have resulted from: (1) warming-induced soil...

  13. RELATIONSHIP BETWEEN ATMOSPHERIC CO_2 AND CH_4 CONCENTRATIONS AT SYOWA STATION, ANTARCTICA

    OpenAIRE

    アオキ, シュウジ; ナカザワ, タカキヨ; ムラヤマ, ショウヘイ; シミズ, アキラ; ハヤシ, マサヒコ; イワイ, クニモト; Shuhji, AOKI; Takakiyo, NAKAZAWA; Shohei, MURAYAMA; Akira, SHIMIZU; Masahiko, HAYASHI; Kunimoto, IWAI

    1994-01-01

    Precise measurements of the atmospheric CO_2 and CH_4 concentrations have been continued at Syowa Station since 1984 and 1987,respectively. Measured concentrations show secular increase, together with seasonal cycle and irregular variations. Negative correlation is clearly seen between the secular trends of the CO_2 and CH_4 concentrations. The increase rates of CO_2 and CH_4 show oscillations with periods of 2.3 to 2.8 years. The phases of the average seasonal cycles of CO_2 and CH_4 coincid...

  14. Reticular synthesis of HKUST-like tbo MOFs with enhanced CH4 storage

    KAUST Repository

    Spanopoulos, Ioannis

    2015-12-22

    Successful implementation of reticular chemistry using a judiciously designed rigid octatopic carboxylate organic linker allowed the construction of expanded HKUST-1-like tbo-MOF series with intrinsic strong CH4 adsorption sites. The Cu-analogue displayed a concomitant enhancement of the gravimetric and volumetric surface area with the highest reported CH4 uptake among the tbo family, comparable to the best performing MOFs for CH4 storage. The corresponding gravimetric (BET) and volumetric surface area of 3971 m2 g-1 and 2363 m2 cm-3 represent an increase of respectively 115 % and 47 % in comparison to the corresponding values for the prototypical HKUST-1 (tbo-MOF-1), and 42 % and 20 % higher than tbo-MOF-2. High pressure methane adsorption isotherms revealed a high total gravimetric and volumetric CH4 uptakes, reaching 372 cm3 (STP) g-1 and 221 cm3 (STP) cm-3 respectively at 85 bar and 298 K. The corresponding working capacities between 5-80 bar were found to be 294 cm3 (STP) g-1 and 175 cm3 (STP) cm-3 and are placed among the best performing MOFs for CH4 storage particularly at relatively low temperature (e.g. 326 cm3 (STP) g-1 and 194 cm3 (STP) cm-3 at 258 K). To better understand the structure-property relationship and gain insight on the mechanism accounting for the resultant enhanced CH4 storage capacity, molecular simulation study was performed and revealed the presence of very strong CH4 adsorption sites at the vicinity of the organic linker with similar adsorption energetics as the open metal sites. The present findings supports the potential of tbo-MOFs based on the supermolecular building layer (SBL) approach as an ideal platform to further enhance the CH4 storage capacity via expansion and functionalization of the quadrangular pillars.

  15. Reticular synthesis of HKUST-like tbo MOFs with enhanced CH4 storage

    KAUST Repository

    Spanopoulos, Ioannis; Tsangarakis, Constantinos; Klontzas, Emmanuel; Tylianakis, Emmanuel; Froudakis, George; Adil, Karim; Belmabkhout, Youssef; Eddaoudi, Mohamed; Trikalitis, Pantelis N.

    2015-01-01

    Successful implementation of reticular chemistry using a judiciously designed rigid octatopic carboxylate organic linker allowed the construction of expanded HKUST-1-like tbo-MOF series with intrinsic strong CH4 adsorption sites. The Cu-analogue displayed a concomitant enhancement of the gravimetric and volumetric surface area with the highest reported CH4 uptake among the tbo family, comparable to the best performing MOFs for CH4 storage. The corresponding gravimetric (BET) and volumetric surface area of 3971 m2 g-1 and 2363 m2 cm-3 represent an increase of respectively 115 % and 47 % in comparison to the corresponding values for the prototypical HKUST-1 (tbo-MOF-1), and 42 % and 20 % higher than tbo-MOF-2. High pressure methane adsorption isotherms revealed a high total gravimetric and volumetric CH4 uptakes, reaching 372 cm3 (STP) g-1 and 221 cm3 (STP) cm-3 respectively at 85 bar and 298 K. The corresponding working capacities between 5-80 bar were found to be 294 cm3 (STP) g-1 and 175 cm3 (STP) cm-3 and are placed among the best performing MOFs for CH4 storage particularly at relatively low temperature (e.g. 326 cm3 (STP) g-1 and 194 cm3 (STP) cm-3 at 258 K). To better understand the structure-property relationship and gain insight on the mechanism accounting for the resultant enhanced CH4 storage capacity, molecular simulation study was performed and revealed the presence of very strong CH4 adsorption sites at the vicinity of the organic linker with similar adsorption energetics as the open metal sites. The present findings supports the potential of tbo-MOFs based on the supermolecular building layer (SBL) approach as an ideal platform to further enhance the CH4 storage capacity via expansion and functionalization of the quadrangular pillars.

  16. Assessing diel variation of CH4 flux from rice paddies through temperature patterns

    Science.gov (United States)

    Centeno, Caesar Arloo R.; Alberto, Ma Carmelita R.; Wassmann, Reiner; Sander, Bjoern Ole

    2017-10-01

    The diel variation in methane (CH4) flux from irrigated rice was characterized during the dry and wet cropping seasons in 2013 and 2014 using the eddy covariance (EC) technique. The EC technique has the advantage of obtaining measurements of fluxes at an extremely high temporal resolution (10Hz), meaning it records 36,000 measurements per hour. The EC measurements can very well capture the temporal variations of the diel (both diurnal and nocturnal) fluxes of CH4 and the environmental factors (temperature, surface energy flux, and gross ecosystem photosynthesis) at 30-min intervals. The information generated by this technique is important to enhance our mechanistic understanding of the different factors affecting the landscape scale diel CH4 flux. Distinct diel patterns of CH4 flux were observed when the data were partitioned into different cropping periods (pre-planting, growth, and fallow). The temporal variations of the diel CH4 flux during the dry seasons were more pronounced than during the wet seasons because the latter had so much climatic disturbance from heavy monsoon rains and occasional typhoons. Pearson correlation analysis and Granger causality test were used to confirm if the environmental factors evaluated were not only correlated with but also Granger-causing the diel CH4 flux. Soil temperature at 2.5 cm depth (Ts 2.5 cm) can be used as simple proxy for predicting diel variations of CH4 fluxes in rice paddies using simple linear regression during both the dry and wet seasons. This simple site-specific temperature response function can be used for gap-filling CH4 flux data for improving the estimates of CH4 source strength from irrigated rice production.

  17. Annual variation of CH4 emissions from the middle taiga in West Siberian Lowland (2005–2009: a case of high CH4 flux and precipitation rate in the summer of 2007

    Directory of Open Access Journals (Sweden)

    M. Sasakawa

    2012-03-01

    Full Text Available We described continuous measurements of CH4 and CO2 concentration obtained at two sites placed in the middle taiga, Karasevoe (KRS and Demyanskoe (DEM, in West Siberian Lowland (WSL from 2005 to 2009. Although both CH4 and CO2 accumulation (ΔCH4 and ▵CO2 during night-time at KRS in June and July 2007 showed an anomalously high concentration, higher ratios of ΔCH4/ΔCO2 compared with those in other years indicated that a considerably higher CH4 flux occurred relative to the CO2 flux. The daily CH4 flux calculated with the ratio of ΔCH4/ΔCO2 and terrestrial biosphere CO2 flux from an ecosystem model showed a maximum in July at the both sites. Although anomalously high flux was observed in June and July 2007 at KRS, only a small flux variation was observed at DEM. The high regional CH4 flux in June and July 2007 at KRS was reproduced using a process-based ecosystem model, Vegetation Integrative Simulator for Trace gases (VISIT, in response to high water table depth caused by the anomalously high precipitation during the summer of 2007.

  18. Organic carbon burial rates in mangrove sediments: strengthening the global budget

    Science.gov (United States)

    Breithaupt, J.; Smoak, Joseph M.; Smith, Thomas J.; Sanders, Christian J.; Hoare, Armando

    2012-01-01

    Mangrove wetlands exist in the transition zone between terrestrial and marine environments and as such were historically overlooked in discussions of terrestrial and marine carbon cycling. In recent decades, mangroves have increasingly been credited with producing and burying large quantities of organic carbon (OC). The amount of available data regarding OC burial in mangrove soils has more than doubled since the last primary literature review (2003). This includes data from some of the largest, most developed mangrove forests in the world, providing an opportunity to strengthen the global estimate. First-time representation is now included for mangroves in Brazil, Colombia, Malaysia, Indonesia, China, Japan, Vietnam, and Thailand, along with additional data from Mexico and the United States. Our objective is to recalculate the centennial-scale burial rate of OC at both the local and global scales. Quantification of this rate enables better understanding of the current carbon sink capacity of mangroves as well as helps to quantify and/or validate the other aspects of the mangrove carbon budget such as import, export, and remineralization. Statistical analysis of the data supports use of the geometric mean as the most reliable central tendency measurement. Our estimate is that mangrove systems bury 163 (+40; -31) g OC m-2 yr-1 (95% C.I.). Globally, the 95% confidence interval for the annual burial rate is 26.1 (+6.3; -5.1) Tg OC. This equates to a burial fraction that is 42% larger than that of the most recent mangrove carbon budget (2008), and represents 10–15% of estimated annual mangrove production. This global rate supports previous conclusions that, on a centennial time scale, 8–15% of all OC burial in marine settings occurs in mangrove systems.

  19. Organic carbon burial rates in mangrove sediments: Strengthening the global budget

    Science.gov (United States)

    Breithaupt, Joshua L.; Smoak, Joseph M.; Smith, Thomas J., III; Sanders, Christian J.; Hoare, Armando

    2012-09-01

    Mangrove wetlands exist in the transition zone between terrestrial and marine environments and as such were historically overlooked in discussions of terrestrial and marine carbon cycling. In recent decades, mangroves have increasingly been credited with producing and burying large quantities of organic carbon (OC). The amount of available data regarding OC burial in mangrove soils has more than doubled since the last primary literature review (2003). This includes data from some of the largest, most developed mangrove forests in the world, providing an opportunity to strengthen the global estimate. First-time representation is now included for mangroves in Brazil, Colombia, Malaysia, Indonesia, China, Japan, Vietnam, and Thailand, along with additional data from Mexico and the United States. Our objective is to recalculate the centennial-scale burial rate of OC at both the local and global scales. Quantification of this rate enables better understanding of the current carbon sink capacity of mangroves as well as helps to quantify and/or validate the other aspects of the mangrove carbon budget such as import, export, and remineralization. Statistical analysis of the data supports use of the geometric mean as the most reliable central tendency measurement. Our estimate is that mangrove systems bury 163 (+40; -31) g OC m-2 yr-1 (95% C.I.). Globally, the 95% confidence interval for the annual burial rate is 26.1 (+6.3; -5.1) Tg OC. This equates to a burial fraction that is 42% larger than that of the most recent mangrove carbon budget (2008), and represents 10-15% of estimated annual mangrove production. This global rate supports previous conclusions that, on a centennial time scale, 8-15% of all OC burial in marine settings occurs in mangrove systems.

  20. CH4 emissions from enteric fermentation in Austria

    International Nuclear Information System (INIS)

    Gebetsroither, E.; Orthofer, R.; Strebl, F.

    2002-07-01

    This report contains the results of an inventory for methane (CH 4 ) emissions from agricultural enteric fermentation in Austria for the period 1980-2001. Emissions were calculated according to IPCC guidelines. The detailed IPCC 'Tier 2' methodology was applied for cattle (which contribute the vast majority of emissions). The 'Tier 2' methodology relies on specific emission factors that are calculated from the energy intake for different cattle farming practices. The less detailed 'Tier 1' methodology was applied for all other animal categories. Emissions from organic and conventional farming practices were calculated separately. Results indicate that CH 4 emissions from manure management have increased from 1980 to a peak in 1984-1985, and since then have steadily declined. CH 4 emissions were about 169.300 t/yr in 'Kyoto' base year 1990 and have since declined by about 11 % to about 150.000 t/yr in 2001. Almost all emissions (95 % in 1990 and 94 % in 2001) are caused by cattle farming. The contribution of 'dairy cattle' to all emissions from cattle was 49 % in 1990, and has declined to 43 % in 2001. The overall reduction was caused mainly by a decrease in the total numbers of animals. However, in the case of dairy cows the reduction of animals is partly counterbalanced by an increase in emissions per animal (because of the increasing gross energy intake and milk production of milk cattle since 1990). Uncertainties of emissions were estimated with a 'Monte Carlo' simulation. Assuming a normal probability distribution, the calculated standard deviation is 4 %. This indicates there is a 95 % probability that CH 4 emissions are between ± 2 standard deviations, i.e. between 153.000 t and 178.000 t in the year 1990 and between 138.000 t and 162.000 t in the year 2001. (author)

  1. CoMet: an airborne mission to simultaneously measure CO2 and CH4 using lidar, passive remote sensing, and in-situ techniques

    Science.gov (United States)

    Fix, Andreas; Amediek, Axel; Bovensmann, Heinrich; Ehret, Gerhard; Gerbig, Christoph; Gerilowski, Konstantin; Pfeilsticker, Klaus; Roiger, Anke; Zöger, Martin

    2018-04-01

    TIn order to improve our current knowledge on the budgets of the two most important anthropogenic greenhouse gases, CO2 and CH4, an airborne mission on board the German research aircraft HALO in coordination with two smaller Cessna aircraft is going to be conducted in April/May 2017. The goal of CoMet is to combine a suite of the best currently available active (lidar) and passive remote sensors as well as in-situ instruments to provide regional-scale data of greenhouse gases which are urgently required.

  2. Greater future global warming inferred from Earth's recent energy budget.

    Science.gov (United States)

    Brown, Patrick T; Caldeira, Ken

    2017-12-06

    Climate models provide the principal means of projecting global warming over the remainder of the twenty-first century but modelled estimates of warming vary by a factor of approximately two even under the same radiative forcing scenarios. Across-model relationships between currently observable attributes of the climate system and the simulated magnitude of future warming have the potential to inform projections. Here we show that robust across-model relationships exist between the global spatial patterns of several fundamental attributes of Earth's top-of-atmosphere energy budget and the magnitude of projected global warming. When we constrain the model projections with observations, we obtain greater means and narrower ranges of future global warming across the major radiative forcing scenarios, in general. In particular, we find that the observationally informed warming projection for the end of the twenty-first century for the steepest radiative forcing scenario is about 15 per cent warmer (+0.5 degrees Celsius) with a reduction of about a third in the two-standard-deviation spread (-1.2 degrees Celsius) relative to the raw model projections reported by the Intergovernmental Panel on Climate Change. Our results suggest that achieving any given global temperature stabilization target will require steeper greenhouse gas emissions reductions than previously calculated.

  3. Effects of prolonged soil drought on CH4 oxidation in a temperate spruce forest

    Science.gov (United States)

    Borken, W.; Brumme, R.; Xu, Y.-J.

    2000-03-01

    Our objective was to determine potential impacts of changes in rainfall amount and distribution on soil CH4 oxidation in a temperate forest ecosystem. We constructed a roof below the canopy of a 65-year-old Norway spruce forest (Picea abies (L.) Karst.) and simulated two climate change scenarios: (1) an extensively prolonged summer drought of 172 days followed by a rewetting period of 19 days in 1993 and (2) a less intensive summer drought of 108 days followed by a rewetting period of 33 days in 1994. CH4 oxidation, soil matric potential, and soil temperature were measured hourly to daily over a 2-year period. The results showed that annual CH4 oxidation in the drought experiment increased by 102% for the climate change scenario 1 and by 41% for the climate change scenario 2, compared to those of the ambient plot (1.33 kg CH4 ha-1 in 1993 and 1.65 kg CH4 ha-1 in 1994). We tested the relationships between CH4 oxidation rates, water-filled pore space (WFPS), soil matric potential, gas diffusivity, and soil temperature. Temporal variability in the CH4 oxidation rates corresponded most closely to soil matric potential. Employing soil matric potential and soil temperature, we developed a nonlinear model for estimating CH4 oxidation rates. Modeled results were in strong agreement with the measured CH4 oxidation for the ambient (r2 = 0.80) and drought plots (r2 = 0.89) over two experimental years, suggesting that soil matric potential is a highly reliable parameter for modeling CH4 oxidation rate.

  4. Landscape Controls of CH4 Fluxes in a Catchment of the Forest Tundra in Northern Siberia

    Science.gov (United States)

    Flessa, H.; Rodionov, A.; Guggenberger, G.; Fuchs, H.; Magdon, P.; Shibistova, O.; Zrazhevskaya, G.; Kasansky, O.; Blodau, C.

    2007-12-01

    Soils have the capacity to both produce and consume atmospheric methane. The direction and the size of net- CH4 exchange between soils and atmosphere is mainly controlled by the soil aeration, temperature and the amount of bioavailable organic matter. All these factors are strongly influenced by distribution and seasonal dynamics of permafrost. Thus, distribution of permafrost and the thickness of the active layer can exert strong influence on CH4 dynamics in artic and northern boreal ecosystems. We analyzed the spatial and temporal variability of net-CH4 exchange within a catchment located in the Siberian forest tundra at the eastern shore of the lower Yenissej River to constrain the current function of this region as a sink or source of atmospheric CH4 and to gain insight into the potential for climatic change to alter the rate and form of carbon cycling and CH4 fluxes in this region. Net-fluxes of CH4 were measured from July to November 2003 and from August 2006 to July 2007 on representative soils of the catchment (mineral soils with different thawing depth, soils of bog plateaux) and on a thermokarst pond. In addition, dissolved CH4 in the stream draining the catchment was determined. Field observations, classification of landscape structures from satellite images and flux measurements were combined to estimate total catchment CH4 exchange. Nearly all soils of the catchment were net-sinks of atmospheric CH4 with annual CH4-C uptake rates ranging between 1.2 and 0.2 kg ha-1 yr-1. The active layer depth was the main factor determining the size of CH4 uptake. Total net-exchange of CH4 from the catchment was dominated by ponds that covered only about 2% of the catchment area. Due to high CH4 emission from these aquatic systems, the catchment was a net source of atmospheric CH4 with a mean annual emission of approximately 170 kg CH4-C ha-1. CH4 concentration in streams draining the catchment can help to identify areas with high CH4 production. The results suggest

  5. A Monte Carlo study of backscattering effects in the photoelectron emission from CsI into CH$_{4}$ and Ar-CH$_{4}$ mixtures

    CERN Document Server

    Escada, J; Rachinhas, P J B M; Lopes, J A M; Santos, F P; Távora, L M N; Conde, C A N; Stauffer, A D

    2007-01-01

    Monte Carlo simulation is used to investigate photoelectron backscattering effects in the emission from a CsI photocathode into CH4 and Ar-CH4 mixtures for incident monochromatic photons with energies Eph in the range 6.8 eV to 9.8 eV (182 nm to 127 nm), and photons from a continuous VUV Hg(Ar) lamp with a spectral distribution peaked at Eph = 6.7 eV (185 nm), considering reduced applied electric fields E/N in the 0.1 Td to 40 Td range. The addition of CH4 to a noble gas efficiently increases electron transmission and drift velocity, due to vibrational excitation of the molecules at low electron energies. Results are presented for the photoelectron transmission efficiencies f, where f is the fraction of the number of photoelectrons emitted from CsI which are transmitted through the gas as compared to vacuum. The dependence of f on Eph, E/N, and mixture composition is analyzed and explained in terms of electron scattering in the different gas media, and results are compared with available measurements. Electro...

  6. Ozone and carbon monoxide budgets over the Eastern Mediterranean

    NARCIS (Netherlands)

    Myriokefalitakis, S.; Daskalakis, N.; Fanourgakis, G.S.; Voulgarakis, A.; Krol, M.C.; Brugh, Aan de J.M.J.; Kanakidou, M.

    2016-01-01

    The importance of the long-range transport (LRT) on O3 and CO budgets over the Eastern Mediterranean has been investigated using the state-of-the-art 3-dimensional global chemistry-transport model TM4-ECPL. A 3-D budget analysis has been performed separating the Eastern from the

  7. Reduced biomass burning emissions reconcile conflicting estimates of the post-2006 atmospheric methane budget.

    Science.gov (United States)

    Worden, John R; Bloom, A Anthony; Pandey, Sudhanshu; Jiang, Zhe; Worden, Helen M; Walker, Thomas W; Houweling, Sander; Röckmann, Thomas

    2017-12-20

    Several viable but conflicting explanations have been proposed to explain the recent ~8 p.p.b. per year increase in atmospheric methane after 2006, equivalent to net emissions increase of ~25 Tg CH 4 per year. A concurrent increase in atmospheric ethane implicates a fossil source; a concurrent decrease in the heavy isotope content of methane points toward a biogenic source, while other studies propose a decrease in the chemical sink (OH). Here we show that biomass burning emissions of methane decreased by 3.7 (±1.4) Tg CH 4 per year from the 2001-2007 to the 2008-2014 time periods using satellite measurements of CO and CH 4 , nearly twice the decrease expected from prior estimates. After updating both the total and isotopic budgets for atmospheric methane with these revised biomass burning emissions (and assuming no change to the chemical sink), we find that fossil fuels contribute between 12-19 Tg CH 4 per year to the recent atmospheric methane increase, thus reconciling the isotopic- and ethane-based results.

  8. The magnitude and persistence of soil NO, N20, CH4, and C02 fluxes from burned tropical savanna in Brazil

    Science.gov (United States)

    Mark Poth; Iris Cofman Anderson; Heloisa Sinatora Miranda; Antonia Carlos Miranda; Philip J. Riggan

    1995-01-01

    Among all global ecosystems, tropical savannas are the most severely and extensively affected by anthropogenic burning. Frequency of fire in cerrado, a type of tropical savanna covering 25% of Brazil, is 2 to 4 years. In 1992 we measured soil fluxes of NO, N20, CH4, and C02 from cerrado sites that had...

  9. Disproportionation and thermochemical sulfate reduction reactions in S-H20-Ch4 and S-D2O-CH4 systems from 200 to 340 °C at elevated pressures

    Science.gov (United States)

    Yuan, Shunda; Chou, I-Ming; Burruss, Robert A.

    2013-01-01

    Elemental sulfur, as a transient intermediate compound, by-product, or catalyst, plays significant roles in thermochemical sulfate reduction (TSR) reactions. However, the mechanisms of the reactions in S-H2O-hydrocarbons systems are not clear. To improve our understanding of reaction mechanisms, we conducted a series of experiments between 200 and 340 °C for S-H2O-CH4, S-D2O-CH4, and S-CH4-1m ZnBr2 systems in fused silica capillary capsules (FSCC). After a heating period ranging from 24 to 2160 hours (hrs), the quenched samples were analyzed by Raman spectroscopy. Combined with the in situ Raman spectra collected at high temperatures and pressures in the S-H2O and S-H2O-CH4 systems, our results showed that (1) the disproportionation of sulfur in the S-H2O-CH4 system occurred at temperatures above 200 °C and produced H2S, SO42-, and possibly trace amount of HSO4-; (2) sulfate (and bisulfate), in the presence of sulfur, can be reduced by methane between 250 and 340 °C to produce CO2 and H2S, and these TSR temperatures are much closer to those of the natural system (2O-CH4 system may take place simultaneously, with TSR being favored at higher temperatures; and (4) in the system S-D2O-CH4, both TSR and the competitive disproportionation reactions occurred simultaneously at temperatures above 300 °C, but these reactions were very slow at lower temperatures. Our observation of methane reaction at 250 °C in a laboratory time scale suggests that, in a geologic time scale, methane may be destroyed by TSR reactions at temperatures > 200 °C that can be reached by deep drilling for hydrocarbon resources.

  10. Methane emissions form terrestrial plants

    Energy Technology Data Exchange (ETDEWEB)

    Bergamaschi, P.; Dentener, F.; Grassi, G.; Leip, A.; Somogyi, Z.; Federici, S.; Seufert, G.; Raes, F. [European Commission, DG Joint Research Centre, Institute for Environment and Sustainability, Ispra (Italy)

    2006-07-01

    In a recent issue of Nature Keppler et al. (2006) report the discovery that terrestrial plants emit CH4 under aerobic conditions. Until now it was thought that bacterial decomposition of plant material under anaerobic conditions, such as in wetlands and water flooded rice paddies, is the main process leading to emissions from terrestrial ecosystems. In a first attempt to upscale these measurements, the authors estimate that global total emissions may be 149 Tg CH4/yr (62-236 Tg CH4/yr), with the main contribution estimated from tropical forests and grasslands (107 Tg CH4/yr with a range of 46-169 Tg CH4/yr). If confirmed, this new source of emission would constitute a significant fraction of the total global methane sources (estimated 500-600 Tg CH4/yr for present day total natural and anthropogenic sources) and have important implications for the global CH4 budget. To accommodate it within the present budget some sources would need to be re-assessed downwards and/or some sinks re-assessed upwards. Furthermore, also considering that methane is a {approx}23 times more powerful greenhouse gas than CO2, the possible feedbacks of these hitherto unknown CH4 emissions on global warming and their impacts on greenhouse gases (GHG) mitigation strategies need to be carefully evaluated. The merit of the paper is without doubt related to the remarkable discovery of a new process of methane emissions active under aerobic conditions. However, we think that the applied approach of scaling up emissions from the leaf level to global totals by using only few measured data (mainly from herbaceous species) and the Net Primary Productivity of the main biomes is scientifically questionable and tends to overestimate considerably the global estimates, especially for forest biomes. Furthermore, some significant constraints on the upper limit of the global natural CH4 emissions arise from the pre-industrial CH4 budget. Pre-industrial atmospheric CH4 mixing ratios have been measured

  11. Macromolecule simulation and CH{sub 4} adsorption mechanism of coal vitrinite

    Energy Technology Data Exchange (ETDEWEB)

    Yu, Song, E-mail: songyu10094488@126.com [School of Resources and Earth Science, China University of Mining & Technology, Xuzhou 221116 (China); Key Laboratory of Coal bed Methane Resource & Reservoir Formation Process, Ministry of Education, Xuzhou 221008 (China); Yan-ming, Zhu; Wu, Li [School of Resources and Earth Science, China University of Mining & Technology, Xuzhou 221116 (China); Key Laboratory of Coal bed Methane Resource & Reservoir Formation Process, Ministry of Education, Xuzhou 221008 (China)

    2017-02-28

    Highlights: • Molecular model of single maceral vitrinite was obtained by {sup 13}C NMR, FT IR and HRTEM. • An optimal configuration was obtained through calculation of MM and MD. • The adsorption parameters for methane and vitrinite were determined with DFT and GCMC. - Abstract: The microscopic mechanism of interactions between CH{sub 4} and coal macromolecules is of significant practical and theoretical importance in CBM development and methane storage. Under periodic boundary conditions, the optimal energy configuration of coal vitrinite, which has a higher torsion degree and tighter arrangement, can be determined by the calculation of molecular mechanics (MM) and molecular dynamics (MD), and annealing kinetics simulation based on ultimate analysis, {sup 13}C NMR, FT IR and HRTEM. Macromolecular stabilization is primarily due to the van der Waals energy and covalent bond energy, mainly consisting of bond torsion energy and bond angle energy. Using the optimal configuration as the adsorbent, GCMC simulation of vitrinite adsorption of CH{sub 4} is conducted. A saturated state is reached after absorbing 17 CH{sub 4}s per coal vitrinite molecule. CH{sub 4} is preferentially adsorbed on the edge, and inclined to gathering around the branched chains of the inner vitrinite sites. Finally, the adsorption parameters are calculated through first principle DFT. The adsorbability order is as follows: aromatic structure> heteroatom rings > oxygen functional groups. The adsorption energy order is as follows: Top < Bond < Center, Up < Down. The order of average RDF better reflects the adsorption ability and that of [-COOH] is lower than those of [−C=O] and [C−O−C]. CH{sub 4} distributed in the distance of 0.99–16 Å to functional groups in the type of monolayer adsorption and the average distance order manifest as [−C=O] (1.64 Å) < [C−O−C] (1.89 Å) < [−COOH] (3.78 Å) < [-CH{sub 3}] (4.11 Å) according to the average RDF curves. CH{sub 4} enriches

  12. Environmental controls of temporal and spatial variability in CO2 and CH4 fluxes in a neotropical peatland.

    Science.gov (United States)

    Wright, Emma L; Black, Colin R; Turner, Benjamin L; Sjögersten, Sofie

    2013-12-01

    Tropical peatlands play an important role in the global storage and cycling of carbon (C) but information on carbon dioxide (CO2) and methane (CH4) fluxes from these systems is sparse, particularly in the Neotropics. We quantified short and long-term temporal and small scale spatial variation in CO2 and CH4 fluxes from three contrasting vegetation communities in a domed ombrotrophic peatland in Panama. There was significant variation in CO2 fluxes among vegetation communities in the order Campnosperma panamensis > Raphia taedigera > Cyperus. There was no consistent variation among sites and no discernible seasonal pattern of CH4 flux despite the considerable range of values recorded (e.g. -1.0 to 12.6 mg m(-2) h(-1) in 2007). CO2 fluxes varied seasonally in 2007, being greatest in drier periods (300-400 mg m(-2) h(-1)) and lowest during the wet period (60-132 mg m(-2) h(-1)) while very high emissions were found during the 2009 wet period, suggesting that peak CO2 fluxes may occur following both low and high rainfall. In contrast, only weak relationships between CH4 flux and rainfall (positive at the C. panamensis site) and solar radiation (negative at the C. panamensis and Cyperus sites) was found. CO2 fluxes showed a diurnal pattern across sites and at the Cyperus sp. site CO2 and CH4 fluxes were positively correlated. The amount of dissolved carbon and nutrients were strong predictors of small scale within-site variability in gas release but the effect was site-specific. We conclude that (i) temporal variability in CO2 was greater than variation among vegetation communities; (ii) rainfall may be a good predictor of CO2 emissions from tropical peatlands but temporal variation in CH4 does not follow seasonal rainfall patterns; and (iii) diurnal variation in CO2 fluxes across different vegetation communities can be described by a Fourier model. © 2013 John Wiley & Sons Ltd.

  13. Local- and regional-scale measurements of CH4, δ13CH4, and C2H6 in the Uintah Basin using a mobile stable isotope analyzer

    Science.gov (United States)

    Rella, C. W.; Hoffnagle, J.; He, Y.; Tajima, S.

    2015-10-01

    In this paper, we present an innovative CH4, δ13CH4, and C2H6 instrument based on cavity ring-down spectroscopy (CRDS). The design and performance of the analyzer is presented in detail. The instrument is capable of precision of less than 1 ‰ on δ13CH4 with 1 in. of averaging and about 0.1 ‰ in an hour. Using this instrument, we present a comprehensive approach to atmospheric methane emissions attribution. Field measurements were performed in the Uintah Basin (Utah, USA) in the winter of 2013, using a mobile lab equipped with the CRDS analyzer, a high-accuracy GPS, a sonic anemometer, and an onboard gas storage and playback system. With a small population and almost no other sources of methane and ethane other than oil and gas extraction activities, the Uintah Basin represents an ideal location to investigate and validate new measurement methods of atmospheric methane and ethane. We present the results of measurements of the individual fugitive emissions from 23 natural gas wells and six oil wells in the region. The δ13CH4 and C2H6 signatures that we observe are consistent with the signatures of the gases found in the wells. Furthermore, regional measurements of the atmospheric CH4, δ13CH4, and C2H6 signatures throughout the basin have been made, using continuous sampling into a 450 m long tube and laboratory reanalysis with the CRDS instrument. These measurements suggest that 85 ± 7 % of the total emissions in the basin are from natural gas production.

  14. Atmospheric chemistry of 4:2 fluorotelomer alcohol (n-C4F9CH2CH2OH)

    DEFF Research Database (Denmark)

    Andersen, Mads Peter Sulbæk; Nielsen, Ole John; Hurley, M. D.

    2005-01-01

    Smog chamber/FTIR techniques were used to study the Cl atom initiated oxidation of 4:2 fluorotelomer alcohol (C4F9CH2CH2OH, 4:2 FTOH) in the presence of NOx in 700 Torr of N-2/O-2 diluent at 296 K. Chemical activation effects play an important role in the atmospheric chemistry of the peroxy...

  15. CH4 Emission Model from Bos Primigenius Waste in Fish-Water: Implications for Integrated Livestock-Fish Farming Systems

    Directory of Open Access Journals (Sweden)

    Joshua O. Okeniyi

    2013-07-01

    Full Text Available This paper studies a methane (CH4 emission model from the waste of cattle (B. primigenius based on trends in integrated livestock-fish farming adoption by farmers in Nigeria. Dung of B. primigenius was employed as substrate in fish-water, obtained from a fish-rearing farm, as a matrix medium for simulating a low-oxygen wastewater environment of an agriculture-aquaculture system. A substrate to fish-water mass ratio of 1:3 was used, developed in a laboratory-size digesting reactor system. Volumetric readings, at ambient temperature conditions and with a retention time of thirty-two days, were then subjected to the logistic probability density function, and tested against correlation coefficient and Nash-Sutcliffe coefficient of efficiency criteria. The readings show that a volume of CH4-containing gas as high as 65.3 x 10−3 dm3 was produced on the 13th day from the B. primigenius substrate. Also, production of 234.59 x 10−3 dm3/kg CH4-containing gas, totaling 703.76 x 10−3 dm3, was observed through the studied retention time. The 60% CH4 constituent model of the measured gas generation showed a potency of 2.0664 kg emission per animal, which is equivalent to 43.3944 CO2eq of global warming potential (GWP annually per animal. This bears environmental and climate change implications, and therefore alternative sustainable practices for integrated livestock-fish farming adoption are suggested.

  16. Enhanced simulations of CH4 and CO2 production in permafrost-affected soils address soil moisture controls on anaerobic decomposition

    Science.gov (United States)

    Graham, D. E.; Zheng, J.; Moon, J. W.; Painter, S. L.; Thornton, P. E.; Gu, B.; Wullschleger, S. D.

    2017-12-01

    Rapid warming of Arctic ecosystems exposes soil organic carbon (SOC) to accelerated microbial decomposition, leading to increased emissions of carbon dioxide (CO2) and methane (CH4) that have a positive feedback on global warming. The magnitude, timing, and form of carbon release will depend not only on changes in temperature, but also on biogeochemical and hydrological properties of soils. In this synthesis study, we assessed the decomposability of thawed organic carbon from active layer soils and permafrost from the Barrow Environmental Observatory across different microtopographic positions under anoxic conditions. The main objectives of this study were to (i) examine environmental conditions and soil properties that control anaerobic carbon decomposition and carbon release (as both CO2 and CH4); (ii) develop a common set of parameters to simulate anaerobic CO2 and CH4 production; and (iii) evaluate uncertainties generated from representations of pH and temperature effects in the current model framework. A newly developed anaerobic carbon decomposition framework simulated incubation experiment results across a range of soil water contents. Anaerobic CO2 and CH4 production have different temperature and pH sensitivities, which are not well represented in current biogeochemical models. Distinct dynamics of CH4 production at -2° C suggest methanogen biomass and growth rate limit activity in these near-frozen soils, compared to warmer temperatures. Anaerobic CO2 production is well constrained by the model using data-informed labile carbon pool and fermentation rate initialization to accurately simulate its temperature sensitivity. On the other hand, CH4 production is controlled by water content, methanogenesis biomass, and the presence of alternative electron acceptors, producing a high temperature sensitivity with large uncertainties for methanogenesis. This set of environmental constraints to methanogenesis is likely to undergo drastic changes due to permafrost

  17. Chemical reaction surface vibrational frequencies evaluated in curvilinear internal coordinates: Application to H + CH(4) H(2) + CH(3).

    Science.gov (United States)

    Banks, Simon T; Clary, David C

    2009-01-14

    We consider the general problem of vibrational analysis at nonglobally optimized points on a reduced dimensional reaction surface. We discuss the importance of the use of curvilinear internal coordinates to describe molecular motion and derive a curvilinear projection operator to remove the contribution of nonzero gradients from the Hessian matrix. Our projection scheme is tested in the context of a two-dimensional quantum scattering calculation for the reaction H + CH(4) --> H(2) + CH(3) and its reverse H(2) + CH(3) --> H + CH(4). Using zero-point energies calculated via rectilinear and curvilinear projections we construct two two-dimensional, adiabatically corrected, ab initio reaction surfaces for this system. It is shown that the use of curvilinear coordinates removes unphysical imaginary frequencies observed with rectilinear projection and leads to significantly improved thermal rate constants for both the forward and reverse reactions.

  18. Agricultural peatland restoration: effects of land-use change on greenhouse gas (CO2 and CH4) fluxes in the Sacramento-San Joaquin Delta.

    Science.gov (United States)

    Knox, Sara Helen; Sturtevant, Cove; Matthes, Jaclyn Hatala; Koteen, Laurie; Verfaillie, Joseph; Baldocchi, Dennis

    2015-02-01

    Agricultural drainage of organic soils has resulted in vast soil subsidence and contributed to increased atmospheric carbon dioxide (CO2) concentrations. The Sacramento-San Joaquin Delta in California was drained over a century ago for agriculture and human settlement and has since experienced subsidence rates that are among the highest in the world. It is recognized that drained agriculture in the Delta is unsustainable in the long-term, and to help reverse subsidence and capture carbon (C) there is an interest in restoring drained agricultural land-use types to flooded conditions. However, flooding may increase methane (CH4) emissions. We conducted a full year of simultaneous eddy covariance measurements at two conventional drained agricultural peatlands (a pasture and a corn field) and three flooded land-use types (a rice paddy and two restored wetlands) to assess the impact of drained to flooded land-use change on CO2 and CH4 fluxes in the Delta. We found that the drained sites were net C and greenhouse gas (GHG) sources, releasing up to 341 g C m(-2) yr(-1) as CO2 and 11.4 g C m(-2) yr(-1) as CH4. Conversely, the restored wetlands were net sinks of atmospheric CO2, sequestering up to 397 g C m(-2) yr(-1). However, they were large sources of CH4, with emissions ranging from 39 to 53 g C m(-2) yr(-1). In terms of the full GHG budget, the restored wetlands could be either GHG sources or sinks. Although the rice paddy was a small atmospheric CO2 sink, when considering harvest and CH4 emissions, it acted as both a C and GHG source. Annual photosynthesis was similar between sites, but flooding at the restored sites inhibited ecosystem respiration, making them net CO2 sinks. This study suggests that converting drained agricultural peat soils to flooded land-use types can help reduce or reverse soil subsidence and reduce GHG emissions. © 2014 John Wiley & Sons Ltd.

  19. Study on the Promotion Effect of Ionic Liquid on CH4 Hydrate Formation

    International Nuclear Information System (INIS)

    Shin, Ju-Young; Mun, Sungyong; Kang, Seong-Pil; Kim, Kisub

    2013-01-01

    In this study, we investigated the kinetics of gas hydrate formation in the presence of ionic liquid (IL). Hydroxyethyl-methyl-morpholinium chloride (HEMM-Cl) was chosen as a material for the promotion effect test. Phase equilibrium curve for CH 4 hydrate with aqueous IL solution was obtained and its induction time and consumed amount of CH 4 gas were also measured. Aqueous solutions containing 20-20,000 ppm of HEMM-Cl was prepared and studied at 70 bar and 274.15 K. To compare the measured results to those of the conventional promoter, sodium dodecyl sulfate was also tested at the same condition. Result showed that the hydrate equilibrium curve was shifted toward higher pressure and lower temperature region. In addition, the induction time on CH 4 hydrate formation in the presence of IL was not shown. The amount of consumed CH 4 was increased with the whole range of tested concentration of IL and the highest consumption of CH 4 happened at 1,000 ppm of HEMM-Cl. HEMM-Cl induced and enhanced the CH 4 hydrate formation with a small amount of addition. Obtained result is expected to be applied for the development of technologies such as gas storage and transport using gas hydrates

  20. From California dreaming to California data: Challenging historic models for landfill CH4 emissions

    Directory of Open Access Journals (Sweden)

    Kurt Spokas

    2015-06-01

    Full Text Available Abstract Improved quantification of diverse CH4 sources at the urban scale is needed to guide local GHG mitigation strategies in the Anthropocene. Herein, we focus on landfill CH4 emissions in California, challenging the current IPCC methodology which focuses on a climate dependency for landfill CH4 generation (methanogenesis, but does not explicitly consider climate or soil dependencies for emissions. Relying on a comprehensive California landfill database, a field-validated process-based model for landfill CH4 emissions (CALMIM, and select field measurements at 10 California sites with a variety of methods, we support the contrary position: Limited climate dependency for methanogenesis, but strong climate dependency for landfill CH4 emissions. Contrary to the historic IPCC empirical model for methanogenesis with kinetic constants related to climate, we demonstrate a simpler and more robust linear empirical relationship (r2 = 0.85; n=128 between waste mass and landfill biogas recovery [126 × 10-6 Nm3 CH4 hr-1 Mgwaste-1]. More interestingly, there are no statistically significant relationships with climate, site age, or status (open/closed for landfill biogas recovery. The current IPCC methodology does not consider soil or climate drivers for gaseous transport or seasonal methanotrophy in different cover soils. On the other hand, we illustrate strong climate and soil dependencies for landfill emissions—e.g., average intermediate cover emissions below 20 g CH4 m-2 d-1 when the site’s mean annual precipitation is >500 mm y-1. Thereby, for the California landfill CH4 inventory, the highest-emitting sites shift from landfills containing the largest mass of waste to sites dominated by intermediate cover types having a reduced rate of soil CH4 oxidation during the annual cycle. These differences have profound implications for developing more realistic, science-based urban and regional scale GHG inventories for landfill CH4 while reducing

  1. Soil CO2, CH4 and N2O effluxes and concentrations in soil profiles down to 15.5m depth in eucalypt plantations under contrasted rainfall regimes

    Science.gov (United States)

    Germon, A.; Nouvellon, Y.; Christophe, J.; Chapuis-Lardy, L.; Robin, A.; Rosolem, C. A.; Gonçalves, J. L. D. M.; Guerrini, I. A.; Laclau, J. P.

    2017-12-01

    Silvicultural practices in planted forests affect the fluxes of greenhouse gases at the soil surface and the major factors driving greenhouse gas production in forest soils (substrate supply, temperature, water content,…) vary with soil depth. Our study aimed to assess the consequences of drought on the temporal variability of CO2, CH4 and N2O fluxes throughout very deep soil profiles in Eucalyptus grandis plantations 3 months before the harvest then in coppice, the first 18 months after clear-cutting. Two treatments were compared: one with 37% of throughfall excluded by plastic sheets (TE), and one without rainfall exclusion (WE). Measurements of soil CO2 efflux were made every two weeks for 30 months using a closed-path Li8100 system in both treatment. Every two weeks for 21 months, CO2, CH4 and N2O surface effluxes were measured using the closed-chamber method and concentrations in the soil were measured at 7 depths down to 15.5 m in both TE and WE. At most measurement dates, soil CO2 efflux were significantly higher in TE than in WE. Across the two treatments and the measurement dates, CO2 concentrations increased from 4446 ± 2188 ppm at 10 cm deep to 15622 ± 3523 ppm at 15.5 m, CH4 concentrations increased from 0.41 ± 0.17 ppm at 10 cm deep to 0.77 ± 0.24 ppm at 15.5 m and N2O concentrations remained roughly constant and were on average 478 ± 55 ppb between soil surface and 15.5 m deep. CO2 and N2O concentrations were on average 20.7 and 7.6% lower in TE than in WE, respectively, across the sampling depths. However, CH4 concentrations in TE were on average 44.4% higher than in WE, throughout the soil profile. Those results suggest that extended drought periods might reduce the production of CO2 and N2O but increase the accumulation of CH4 in eucalypt plantations established in deep tropical soils. Very deep tropical soils cover huge areas worldwide and improving our understanding of the spatiotemporal dynamics of gas concentrations in deep soil layers

  2. The formaldehyde budget as seen by a global-scale multi-constraint and multi-species inversion system

    Directory of Open Access Journals (Sweden)

    A. Fortems-Cheiney

    2012-08-01

    Full Text Available For the first time, carbon monoxide (CO and formaldehyde (HCHO satellite retrievals are used together with methane (CH4 and methyl choloroform (CH3CCl3 or MCF surface measurements in an advanced inversion system. The CO and HCHO are respectively from the MOPITT and OMI instruments. The multi-species and multi-satellite dataset inversion is done for the 2005–2010 period. The robustness of our results is evaluated by comparing our posterior-modeled concentrations with several sets of independent measurements of atmospheric mixing ratios. The inversion leads to significant changes from the prior to the posterior, in terms of magnitude and seasonality of the CO and CH4 surface fluxes and of the HCHO production by non-methane volatile organic compounds (NMVOC. The latter is significantly decreased, indicating an overestimation of the biogenic NMVOC emissions, such as isoprene, in the GEIA inventory. CO and CH4 surface emissions are increased by the inversion, from 1037 to 1394 TgCO and from 489 to 529 TgCH4 on average for the 2005–2010 period. CH4 emissions present significant interannual variability and a joint CO-CH4 fluxes analysis reveals that tropical biomass burning probably played a role in the recent increase of atmospheric methane.

  3. Variability and quasi-decadal changes in the methane budget over the period 2000-2012

    Science.gov (United States)

    Saunois, Marielle; Bousquet, Philippe; Poulter, Ben; Peregon, Anna; Ciais, Philippe; Canadell, Josep G.; Dlugokencky, Edward J.; Etiope, Giuseppe; Bastviken, David; Houweling, Sander; Janssens-Maenhout, Greet; Tubiello, Francesco N.; Castaldi, Simona; Jackson, Robert B.; Alexe, Mihai; Arora, Vivek K.; Beerling, David J.; Bergamaschi, Peter; Blake, Donald R.; Brailsford, Gordon; Bruhwiler, Lori; Crevoisier, Cyril; Crill, Patrick; Covey, Kristofer; Frankenberg, Christian; Gedney, Nicola; Höglund-Isaksson, Lena; Ishizawa, Misa; Ito, Akihiko; Joos, Fortunat; Kim, Heon-Sook; Kleinen, Thomas; Krummel, Paul; Lamarque, Jean-François; Langenfelds, Ray; Locatelli, Robin; Machida, Toshinobu; Maksyutov, Shamil; Melton, Joe R.; Morino, Isamu; Naik, Vaishali; O'Doherty, Simon; Parmentier, Frans-Jan W.; Patra, Prabir K.; Peng, Changhui; Peng, Shushi; Peters, Glen P.; Pison, Isabelle; Prinn, Ronald; Ramonet, Michel; Riley, William J.; Saito, Makoto; Santini, Monia; Schroeder, Ronny; Simpson, Isobel J.; Spahni, Renato; Takizawa, Atsushi; Thornton, Brett F.; Tian, Hanqin; Tohjima, Yasunori; Viovy, Nicolas; Voulgarakis, Apostolos; Weiss, Ray; Wilton, David J.; Wiltshire, Andy; Worthy, Doug; Wunch, Debra; Xu, Xiyan; Yoshida, Yukio; Zhang, Bowen; Zhang, Zhen; Zhu, Qiuan

    2017-09-01

    Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH4) budget over 2000-2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000-2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000-2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008-2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16-32] Tg CH4 yr-1 higher methane emissions over the period 2008-2012 compared to 2002-2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002-2006 and 2008-2012 differs from one atmospheric inversion study to another. However, all top-down studies

  4. Computing energy levels of CH4, CHD3, CH3D, and CH3F with a direct product basis and coordinates based on the methyl subsystem.

    Science.gov (United States)

    Zhao, Zhiqiang; Chen, Jun; Zhang, Zhaojun; Zhang, Dong H; Wang, Xiao-Gang; Carrington, Tucker; Gatti, Fabien

    2018-02-21

    Quantum mechanical calculations of ro-vibrational energies of CH 4 , CHD 3 , CH 3 D, and CH 3 F were made with two different numerical approaches. Both use polyspherical coordinates. The computed energy levels agree, confirming the accuracy of the methods. In the first approach, for all the molecules, the coordinates are defined using three Radau vectors for the CH 3 subsystem and a Jacobi vector between the remaining atom and the centre of mass of CH 3 . Euler angles specifying the orientation of a frame attached to CH 3 with respect to a frame attached to the Jacobi vector are used as vibrational coordinates. A direct product potential-optimized discrete variable vibrational basis is used to build a Hamiltonian matrix. Ro-vibrational energies are computed using a re-started Arnoldi eigensolver. In the second approach, the coordinates are the spherical coordinates associated with four Radau vectors or three Radau vectors and a Jacobi vector, and the frame is an Eckart frame. Vibrational basis functions are products of contracted stretch and bend functions, and eigenvalues are computed with the Lanczos algorithm. For CH 4 , CHD 3 , and CH 3 D, we report the first J > 0 energy levels computed on the Wang-Carrington potential energy surface [X.-G. Wang and T. Carrington, J. Chem. Phys. 141(15), 154106 (2014)]. For CH 3 F, the potential energy surface of Zhao et al. [J. Chem. Phys. 144, 204302 (2016)] was used. All the results are in good agreement with experimental data.

  5. Computing energy levels of CH4, CHD3, CH3D, and CH3F with a direct product basis and coordinates based on the methyl subsystem

    Science.gov (United States)

    Zhao, Zhiqiang; Chen, Jun; Zhang, Zhaojun; Zhang, Dong H.; Wang, Xiao-Gang; Carrington, Tucker; Gatti, Fabien

    2018-02-01

    Quantum mechanical calculations of ro-vibrational energies of CH4, CHD3, CH3D, and CH3F were made with two different numerical approaches. Both use polyspherical coordinates. The computed energy levels agree, confirming the accuracy of the methods. In the first approach, for all the molecules, the coordinates are defined using three Radau vectors for the CH3 subsystem and a Jacobi vector between the remaining atom and the centre of mass of CH3. Euler angles specifying the orientation of a frame attached to CH3 with respect to a frame attached to the Jacobi vector are used as vibrational coordinates. A direct product potential-optimized discrete variable vibrational basis is used to build a Hamiltonian matrix. Ro-vibrational energies are computed using a re-started Arnoldi eigensolver. In the second approach, the coordinates are the spherical coordinates associated with four Radau vectors or three Radau vectors and a Jacobi vector, and the frame is an Eckart frame. Vibrational basis functions are products of contracted stretch and bend functions, and eigenvalues are computed with the Lanczos algorithm. For CH4, CHD3, and CH3D, we report the first J > 0 energy levels computed on the Wang-Carrington potential energy surface [X.-G. Wang and T. Carrington, J. Chem. Phys. 141(15), 154106 (2014)]. For CH3F, the potential energy surface of Zhao et al. [J. Chem. Phys. 144, 204302 (2016)] was used. All the results are in good agreement with experimental data.

  6. Surface study of platinum decorated graphene towards adsorption of NH_3 and CH_4

    International Nuclear Information System (INIS)

    Rad, Ali Shokuhi; Pazoki, Hossein; Mohseni, Soheil; Zareyee, Daryoush; Peyravi, Majid

    2016-01-01

    To distinguish the potential of graphene sensors, there is a need to recognize the interaction between graphene sheet and adsorbing molecules. We used density functional theory (DFT) calculations to study the properties of pristine as well as Pt-decorated graphene sheet upon adsorption of NH_3 and CH_4 on its surface to exploit its potential to be as gas sensors for them. We found much higher adsorption, higher charge transfer, lower intermolecular distance, and higher orbital hybridizing upon adsorption of NH_3 and CH_4 gas molecules on Pt-decorated graphene compared to pristine graphene. Also our calculations reveal that the adsorption energies on Pt-decorated graphene sheet are in order of NH_3 >CH_4 which could be corresponded to the order of their sensitivity on this modified surface. We used orbital analysis including density of states as well as frontier molecular orbital study for all analyte-surface systems to more understanding the kind of interaction (physisorption or chemisorption). Consequently, the Pt-decorated graphene can transform the existence of NH_3 and CH_4 molecules into electrical signal and it may be potentially used as an ideal sensor for detection of NH_3 and CH_4 in ambient situation. - Highlights: • Pt-decorated graphene was investigated as an adsorbent for NH_3 and CH_4. • Much higher adsorption of NH_3 and CH_4 on Pt-decorated graphene than pristine graphene. • Higher adsorption of NH_3 compared to CH_4 on Pt-decorated graphene. • Pt influences the electronic structure of graphene.

  7. The Nitrous Oxide (N2O) Budget: Constraints from Atmospheric Observations and Models

    Science.gov (United States)

    Tian, H.; Thompson, R.; Canadell, J.; Winiwarter, W.; Tian, H.; Thompson, R.; Prather, M. J.

    2017-12-01

    The increasing global abundance of N2O poses a threat to human health and society over this coming century through both climate change and ozone depletion. In the sense of greenhouse gases, N2O ranks third behind CO2 and CH4. In the sense of ozone depletion, N2O stands alone. In order to identify the cause of these increases and hopefully reverse them, we need to have a thorough understanding of the sources and sinks (a.k.a. the budget) of N2O and how they can be altered. A bottom-up approach to the budget evaluates individual biogeochemical sources of N2O from the land and ocean; whereas, a top-down approach uses atmospheric observations of the variability, combined with modeling of the atmospheric chemistry and transport, to infer the magnitude of sources and sinks throughout the Earth system. This paper reviews top-down approaches using atmospheric data; a similar top-down approach can be taken with oceanic measurements of N2O, but is not covered here. Stratospheric chemistry is the predominant loss of N2O, and here we review how a merging of new measurements with stratospheric chemistry models is able to provide a constrained budget for the global N2O sink. N2O surface sources are transported and mixed throughout the atmosphere, providing positive anomalies in the N2O abundance (mole fraction of N2O with respect to dry air); while N2O-depleted air from the stratosphere provides negative anomalies. With accurate atmospheric transport models, including for stratosphere-troposphere exchange, the observed tropospheric variability in N2O is effectively a fingerprint of the location and magnitude of sources. This inverse modeling of sources is part of the top-down constraints and is reviewed here.

  8. CO2 Reforming of CH4 by Atmospheric Pressure Abnormal Glow Plasma

    International Nuclear Information System (INIS)

    Chen Qi; Dai Wei; Tao Xumei; Yu Hui; Dai Xiaoyan; Yin Yongxiang

    2006-01-01

    A novel plasma atmospheric pressure abnormal glow discharge was used to investigate synthesis gas production from reforming methane and carbon dioxide. Special attentions were paid to the discharge characteristics and CH 4 , CO 2 conversion, H 2 , CO selectivity, and ratio of H 2 /CO varied with the changing of discharging power, the total flux, and the ratio of CH 4 /CO 2 . Experiments were performed in wider operation variables, the discharging power of 240 to 600 W, the CH 4 /CO 2 of 0.2 to 1.0 and the total flux of 140 to 500 mL/min. The experiments showed that the conversion of CH 4 and CO 2 was up to 91.9% and 83.2%, the selectivity of CO and H 2 was also up to 80% and 90% and H 2 /CO mole ratio was 0.2 to 1.2, respectively. A brief analysis for discharge characteristics and the experimental results were given

  9. A pan-Arctic synthesis of CH4 and CO2 production from anoxic soil incubations

    Science.gov (United States)

    Treat, C.C.; Natali, Susan M.; Ernakovich, Jessica; Iverson, Colleen M.; Lupasco, Massimo; McGuire, A. David; Norby, Richard J.; Roy Chowdhury, Taniya; Richter, Andreas; Šantrůčková, Hana; Schädel, C.; Schuur, Edward A.G.; Sloan, Victoria L.; Turetsky, Merritt R.; Waldrop, Mark P.

    2015-01-01

    Permafrost thaw can alter the soil environment through changes in soil moisture, frequently resulting in soil saturation, a shift to anaerobic decomposition, and changes in the plant community. These changes, along with thawing of previously frozen organic material, can alter the form and magnitude of greenhouse gas production from permafrost ecosystems. We synthesized existing methane (CH4) and carbon dioxide (CO2) production measurements from anaerobic incubations of boreal and tundra soils from the geographic permafrost region to evaluate large-scale controls of anaerobic CO2 and CH4 production and compare the relative importance of landscape-level factors (e.g., vegetation type and landscape position), soil properties (e.g., pH, depth, and soil type), and soil environmental conditions (e.g., temperature and relative water table position). We found fivefold higher maximum CH4 production per gram soil carbon from organic soils than mineral soils. Maximum CH4 production from soils in the active layer (ground that thaws and refreezes annually) was nearly four times that of permafrost per gram soil carbon, and CH4 production per gram soil carbon was two times greater from sites without permafrost than sites with permafrost. Maximum CH4 and median anaerobic CO2 production decreased with depth, while CO2:CH4 production increased with depth. Maximum CH4 production was highest in soils with herbaceous vegetation and soils that were either consistently or periodically inundated. This synthesis identifies the need to consider biome, landscape position, and vascular/moss vegetation types when modeling CH4 production in permafrost ecosystems and suggests the need for longer-term anaerobic incubations to fully capture CH4 dynamics. Our results demonstrate that as climate warms in arctic and boreal regions, rates of anaerobic CO2 and CH4 production will increase, not only as a result of increased temperature, but also from shifts in vegetation and increased

  10. Rate Coefficient for the (4)Heμ + CH4 Reaction at 500 K: Comparison between Theory and Experiment.

    Science.gov (United States)

    Arseneau, Donald J; Fleming, Donald G; Li, Yongle; Li, Jun; Suleimanov, Yury V; Guo, Hua

    2016-03-03

    The rate constant for the H atom abstraction reaction from methane by the muonic helium atom, Heμ + CH4 → HeμH + CH3, is reported at 500 K and compared with theory, providing an important test of both the potential energy surface (PES) and reaction rate theory for the prototypical polyatomic CH5 reaction system. The theory used to characterize this reaction includes both variational transition-state (CVT/μOMT) theory (VTST) and ring polymer molecular dynamics (RPMD) calculations on a recently developed PES, which are compared as well with earlier calculations on different PESs for the H, D, and Mu + CH4 reactions, the latter, in particular, providing for a variation in atomic mass by a factor of 36. Though rigorous quantum calculations have been carried out for the H + CH4 reaction, these have not yet been extended to the isotopologues of this reaction (in contrast to H3), so it is important to provide tests of less rigorous theories in comparison with kinetic isotope effects measured by experiment. In this regard, the agreement between the VTST and RPMD calculations and experiment for the rate constant of the Heμ + CH4 reaction at 500 K is excellent, within 10% in both cases, which overlaps with experimental error.

  11. Greater future global warming inferred from Earth’s recent energy budget

    Science.gov (United States)

    Brown, Patrick T.; Caldeira, Ken

    2017-12-01

    Climate models provide the principal means of projecting global warming over the remainder of the twenty-first century but modelled estimates of warming vary by a factor of approximately two even under the same radiative forcing scenarios. Across-model relationships between currently observable attributes of the climate system and the simulated magnitude of future warming have the potential to inform projections. Here we show that robust across-model relationships exist between the global spatial patterns of several fundamental attributes of Earth’s top-of-atmosphere energy budget and the magnitude of projected global warming. When we constrain the model projections with observations, we obtain greater means and narrower ranges of future global warming across the major radiative forcing scenarios, in general. In particular, we find that the observationally informed warming projection for the end of the twenty-first century for the steepest radiative forcing scenario is about 15 per cent warmer (+0.5 degrees Celsius) with a reduction of about a third in the two-standard-deviation spread (-1.2 degrees Celsius) relative to the raw model projections reported by the Intergovernmental Panel on Climate Change. Our results suggest that achieving any given global temperature stabilization target will require steeper greenhouse gas emissions reductions than previously calculated.

  12. [Spatiotemporal variations of natural wetland CH4 emissions over China under future climate change].

    Science.gov (United States)

    Liu, Jian-gong; Zhu, Qiu-an; Shen, Yan; Yang, Yan-zheng; Luo, Yun-peng; Peng, Chang-hui

    2015-11-01

    Based on a new process-based model, TRIPLEX-GHG, this paper analyzed the spatio-temporal variations of natural wetland CH4 emissions over China under different future climate change scenarios. When natural wetland distributions were fixed, the amount of CH4 emissions from natural wetland ecosystem over China would increase by 32.0%, 55.3% and 90.8% by the end of 21st century under three representative concentration pathways (RCPs) scenarios, RCP2. 6, RCP4.5 and RCP8.5, respectively, compared with the current level. Southern China would have higher CH4 emissions compared to that from central and northern China. Besides, there would be relatively low emission fluxes in western China while relatively high emission fluxes in eastern China. Spatially, the areas with relatively high CH4 emission fluxes would be concentrated in the middle-lower reaches of the Yangtze River, the Northeast and the coasts of the Pearl River. In the future, most natural wetlands would emit more CH4 for RCP4.5 and RCP8.5 than that of 2005. However, under RCP2.6 scenario, the increasing trend would be curbed and CH4 emissions (especially from the Qinghai-Tibet Plateau) begin to decrease in the late 21st century.

  13. Quantifying 12/13CH4 migration and fate following sub-surface release to an agricultural soil

    International Nuclear Information System (INIS)

    Shaw, G.; Atkinson, B.; Meredith, W.; Snape, C.; Steven, M.; Hoch, A.; Lever, D.

    2014-01-01

    Following gas generation in a Geological Disposal Facility (GDF), 14 C-containing gases could migrate through the geosphere, eventually diffusing into soils at the Earth's surface. This paper reports summary results from laboratory and field experiments to obtain information on the probable rates of a) diffusive transport and b) oxidation of 12/13 CH 4 (as a surrogate for 14 CH 4) in a typical agricultural soil in the UK. Rates of CH 4 oxidation were generally low in the field and undisturbed soil columns, though a re-packed column of homogenised topsoil oxidised ambient atmospheric CH 4 20× faster than an undisturbed soil column. In contrast to low observed rates of CH 4 oxidation, the effective diffusion of CH 4 through the soil was rapid. Isotopically labelled CH 4 injected at a depth of 45 cm in the field diffused to the surface and exited the soil over a time period ranging from 8 to 24 h. The rate of CH 4 diffusion through the soil was increased by the presence of ryegrass roots which increased soil porosity and decreased water content. δ 13 C values for laboratory column soils after labelled CH 4 injection experiments showed no sign of residual 13 C, despite the extremely high δ 13 C values of the injected 12/13 CH 4 . If laboratory observations are confirmed by measurements in field samples it can be concluded that the majority of 14 CH 4 from a GDF which enters a soil with low methanotrophic activity will be lost to the free atmosphere after diffusing rapidly through the soil column

  14. Biogeochemical controls on microbial CH4 and CO2 production in Arctic polygon tundra

    Science.gov (United States)

    Zheng, J.

    2016-12-01

    Accurately simulating methane (CH4) and carbon dioxide (CO2) emissions from high latitude soils is critically important for reducing uncertainties in soil carbon-climate feedback predictions. The signature polygonal ground of Arctic tundra generates high level of heterogeneity in soil thermal regime, hydrology and oxygen availability, which limits the application of current land surface models with simple moisture response functions. We synthesized CH4 and CO2 production measurements from soil microcosm experiments across a wet-to dry permafrost degradation gradient from low-centered (LCP) to flat-centered (FCP), and high-centered polygons (HCP) to evaluate the relative importance of biogeochemical processes and their response to warming. More degraded polygon (HCP) showed much less carbon loss as CO2 or CH4, while the total CO2 production from FCP is comparable to that from LCP. Maximum CH4 production from the active layer of LCP was nearly 10 times that of permafrost and FCP. Multivariate analyses identifies gravimetric water content and organic carbon content as key predictors for CH4 production, and iron reduction as a key regulator of pH. The synthesized data are used to validate the geochemical model PHREEQC with extended anaerobic organic substrate turnover, fermentation, iron reduction, and methanogenesis reactions. Sensitivity analyses demonstrate that better representations of anaerobic processes and their pH dependency could significantly improve estimates of CH4 and CO2 production. The synthesized data suggest local decreases in CH4 production along the polygon degradation gradient, which is consistent with previous surface flux measurements. Methane oxidation occurring through the soil column of degraded polygons contributes to their low CH4 emissions as well.

  15. The oceanic cycle and global atmospheric budget of carbonyl sulfide

    Energy Technology Data Exchange (ETDEWEB)

    Weiss, P.S.

    1994-12-31

    A significant portion of stratospheric air chemistry is influenced by the existence of carbonyl sulfide (COS). This ubiquitous sulfur gas represents a major source of sulfur to the stratosphere where it is converted to sulfuric acid aerosol particles. Stratospheric aerosols are climatically important because they scatter incoming solar radiation back to space and are able to increase the catalytic destruction of ozone through gas phase reactions on particle surfaces. COS is primarily formed at the surface of the earth, in both marine and terrestrial environments, and is strongly linked to natural biological processes. However, many gaps in the understanding of the global COS cycle still exist, which has led to a global atmospheric budget that is out of balance by a factor of two or more, and a lack of understanding of how human activity has affected the cycling of this gas. The goal of this study was to focus on COS in the marine environment by investigating production/destruction mechanisms and recalculating the ocean-atmosphere flux.

  16. ON THE ORIGIN OF C_4H AND CH_3OH IN PROTOSTELLAR ENVELOPES

    International Nuclear Information System (INIS)

    Lindberg, Johan E.; Charnley, Steven B.; Cordiner, Martin A.

    2016-01-01

    The formation pathways of different types of organic molecules in protostellar envelopes and other regions of star formation are subjects of intense current interest. We present here observations of C_4H and CH_3OH, tracing two distinct groups of interstellar organic molecules, toward 16 protostars in the Ophiuchus and Corona Australis molecular clouds. Together with observations in the literature, we present C_4H and CH_3OH data from single-dish observations of 40 embedded protostars. We find no correlation between the C_4H and CH_3OH column densities in this large sample. Based on this lack of correlation, a difference in line profiles between C_4H and CH_3OH, and previous interferometric observations of similar sources, we propose that the emission from these two molecules is spatially separated, with the CH_3OH tracing gas that has been transiently heated to high (∼70–100 K) temperatures and the C_4H tracing the cooler large-scale envelope where CH_4 molecules have been liberated from ices. These results provide insight in the differentiation between hot corino and warm carbon-chain chemistry in embedded protostars.

  17. UAV Remote Sensing Can Reveal the Effects of Low-Impact Seismic Lines on Surface Morphology, Hydrology, and Methane (CH4) Release in a Boreal Treed Bog

    Science.gov (United States)

    Lovitt, J.; Rahman, M. M.; Saraswati, S.; McDermid, G. J.; Strack, M.; Xu, B.

    2018-03-01

    Peatlands are globally significant stores of soil carbon, where local methane (CH4) emissions are strongly linked to water table position and microtopography. Historically, these factors have been difficult to measure in the field, constraining our capacity to observe local patterns of variability. In this paper, we show how remote sensing surveys conducted from unmanned aerial vehicle (UAV) platforms can be used to map microtopography and depth to water over large areas with good accuracy, paving the way for spatially explicit estimates of CH4 emissions. This approach enabled us to observe—for the first time—the effects of low-impact seismic lines (LIS; petroleum exploration corridors) on surface morphology and CH4 emissions in a treed-bog ecosystem in northern Alberta, Canada. Through compaction, LIS lines were found to flatten the observed range in microtopographic elevation by 46 cm and decrease mean depth to water by 15.4 cm, compared to surrounding undisturbed conditions. These alterations are projected to increase CH4 emissions by 20-120% relative to undisturbed areas in our study area, which translates to a total rise of 0.011-0.027 kg CH4 day-1 per linear kilometer of LIS ( 2 m wide). The 16 km of LIS present at our 61 ha study site were predicted to boost CH4 emissions by 20-70 kg between May and September 2016.

  18. ISLSCP II GlobalView: Atmospheric Methane Concentrations

    Data.gov (United States)

    National Aeronautics and Space Administration — ABSTRACT: The GlobalView Methane (CH4) data product contains synchronized and smoothed time series of atmospheric CH4 concentrations at selected sites that were...

  19. Straw enhanced CO2 and CH4 but decreased N2O emissions from flooded paddy soils: Changes in microbial community compositions

    Science.gov (United States)

    Wang, Ning; Yu, Jian-Guang; Zhao, Ya-Hui; Chang, Zhi-Zhou; Shi, Xiao-Xia; Ma, Lena Q.; Li, Hong-Bo

    2018-02-01

    To explore microbial mechanisms of straw-induced changes in CO2, CH4, and N2O emissions from paddy field, wheat straw was amended to two paddy soils from Taizhou (TZ) and Yixing (YX), China for 60 d under flooded condition. Illumia sequencing was used to characterize shift in bacterial community compositions. Compared to control, 1-5% straw amendment significantly elevated CO2 and CH4 emissions with higher increase at higher application rates, mainly due to increased soil DOC concentrations. In contrast, straw amendment decreased N2O emission. Considering CO2, CH4, and N2O emissions as a whole, an overall increase in global warming potential was observed with straw amendment. Total CO2 and CH4 emissions from straw-amended soils were significantly higher for YX than TZ soil, suggesting that straw-induced greenhouse gas emissions depended on soil characteristics. The abundance of C-turnover bacteria Firmicutes increased from 28-41% to 54-77% with straw amendment, thereby increasing CO2 and CH4 emissions. However, straw amendment reduced the abundance of denitrifying bacteria Proteobacteria from 18% to 7.2-13% or increased the abundance of N2O reducing bacteria Clostridium from 7.6-11% to 13-30%, thereby decreasing N2O emission. The results suggested straw amendment strongly influenced greenhouse gas emissions via alerting soil properties and bacterial community compositions. Future field application is needed to ascertain the effects of straw return on greenhouse gas emissions.

  20. Evaluating Impacts of CO2 and CH4 Gas Intrusion into an Unconsolidated Aquifer: Fate of As and Cd

    Directory of Open Access Journals (Sweden)

    Amanda eLawter

    2015-07-01

    Full Text Available The sequestration of carbon dioxide (CO2 in deep underground reservoirs has been identified as an important strategy to decrease atmospheric CO2 levels and mitigate global warming, but potential risks on overlying aquifers currently lack a complete evaluation. In addition to CO2, other gases such as methane (CH4 may be present in storage reservoirs. This paper explores for the first time the combined effect of leaking CO2 and CH4 gasses on the fate of major, minor and trace elements in an aquifer overlying a potential sequestration site. Emphasis is placed on the fate of arsenic (As and cadmium (Cd released from the sediments or present as soluble constituents in the leaking brine. Results from macroscopic batch and column experiments show that the presence of CH4 (at a concentration of 1 % in the mixture CO2/CH4 does not have a significant effect on solution pH or the concentrations of most major elements (such as Ca, Ba, and Mg. However, the concentrations of Mn, Mo, Si and Na are inconsistently affected by the presence of CH4 (i.e., in at least one sediment tested in this study. Cd is not released from the sediments and spiked Cd is mostly removed from the aqueous phase most likely via adsorption. The fate of sediment associated As [mainly sorbed arsenite or As(III in minerals] and spiked As [i.e., As5+] is complex. Possible mechanisms that control the As behavior in this system are discussed in this paper. Results are significant for CO2 sequestration risk evaluation and site selection and demonstrate the importance of evaluating reservoir brine and gas stream composition during site selection to ensure the safest site is being chosen.

  1. Variability and quasi-decadal changes in the methane budget over the period 2000–2012

    Directory of Open Access Journals (Sweden)

    M. Saunois

    2017-09-01

    Full Text Available Following the recent Global Carbon Project (GCP synthesis of the decadal methane (CH4 budget over 2000–2012 (Saunois et al., 2016, we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry, inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000–2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000–2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008–2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16–32] Tg CH4 yr−1 higher methane emissions over the period 2008–2012 compared to 2002–2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002–2006 and 2008–2012 differs from one atmospheric inversion study to

  2. Radiative forcing calculations for CH3Cl

    International Nuclear Information System (INIS)

    Grossman, A.S.; Grant, K.E.; Wuebbles, D.J.

    1994-06-01

    Methyl chloride, CH 3 Cl, is the major natural source of chlorine to the stratosphere. The production of CH 3 Cl is dominated by biological sources from the oceans and biomass burning. Production has a seasonal cycle which couples with the short lifetime of tropospheric CH 3 Cl to produce nonuniform global mixing. As an absorber of infrared radiation, CH 3 Cl is of interest for its potential affect on the tropospheric energy balance as well as for its chemical interactions. In this study, we estimate the radiative forcing and global warming potential (GWP) of CH 3 Cl. Our calculations use an infrared radiative transfer model based on the correlated k-distribution algorithm for band absorption. Global and annual average vertical profiles of temperature and trace gas concentration were assumed. The effects of clouds are modeled using three layers of global and annual average cloud optical properties. A radiative forcing value of 0.0053 W/m 2 ppbv was obtained for CH 3 Cl and is approximately linear in the background abundance. This value is about 2 percent of the forcing of CFC-11 and about 300 times the forcing of CO 2 , on a per molecule basis. The radiative forcing calculation for CH 3 Cl is used to estimate the global warming potential (GWP) of CH 3 Cl. The results give GWPs for CH 3 Cl of the order of 25 at a time of 20 years(CO 2 = 1). This result indicates that CH 3 Cl has the potential to be a major greenhouse gas if significant human related emissions were introduced into the atmosphere

  3. Response of CH4 and N2O emissions and wheat yields to tillage method changes in the North China plain.

    Directory of Open Access Journals (Sweden)

    Shenzhong Tian

    Full Text Available The objective of this study was to quantify soil methane (CH(4 and nitrous oxide (N(2O emissions when converting from minimum and no-tillage systems to subsoiling (tilled soil to a depth of 40 cm to 45 cm in the North China Plain. The relationships between CH(4 and N(2O flux and soil temperature, moisture, NH(4 (+-N, organic carbon (SOC and pH were investigated over 18 months using a split-plot design. The soil absorption of CH(4 appeared to increase after conversion from no-tillage (NT to subsoiling (NTS, from harrow tillage (HT to subsoiling (HTS and from rotary tillage (RT to subsoiling (RTS. N(2O emissions also increased after conversion. Furthermore, after conversion to subsoiling, the combined global warming potential (GWP of CH(4 and N(2O increased by approximately 0.05 kg CO(2 ha(-1 for HTS, 0.02 kg CO(2 ha(-1 for RTS and 0.23 kg CO(2 ha(-1 for NTS. Soil temperature, moisture, SOC, NH(4 (+-N and pH also changed after conversion to subsoiling. These changes were correlated with CH(4 uptake and N(2O emissions. However, there was no significant correlation between N(2O emissions and soil temperature in this study. The grain yields of wheat improved after conversion to subsoiling. Under HTS, RTS and NTS, the average grain yield was elevated by approximately 42.5%, 27.8% and 60.3% respectively. Our findings indicate that RTS and HTS would be ideal rotation tillage systems to balance GWP decreases and grain yield improvements in the North China Plain region.

  4. Kinetics of the CH3 + HCl/DCl → CH4/CH3D + Cl and CD3 + HCl/DCl → CD3H/CD4 + Cl reactions: An experimental H atom tunneling investigation

    International Nuclear Information System (INIS)

    Eskola, Arkke J.; Seetula, Jorma A.; Timonen, Raimo S.

    2006-01-01

    The kinetics of the radical reactions of CH 3 with HCl or DCl and CD 3 with HCl or DCl have been investigated in a temperature controlled tubular reactor coupled to a photoionization mass spectrometer. The CH 3 (or CD 3 ) radical, R, was produced homogeneously in the reactor by a pulsed 193 nm exciplex laser photolysis of CH 3 COCH 3 (or CD 3 COCD 3 ). The decay of CH 3 /CD 3 was monitored as a function of HCl/DCl concentration under pseudo-first-order conditions to determine the rate constants as a function of temperature, typically from 188 to 500 K. The rate constants of the CH 3 and CD 3 reactions with HCl had strong non-Arrhenius behavior at low temperatures. The rate constants were fitted to a modified Arrhenius expression k = QA exp (-E a /RT) (error limits stated are 1σ + Students t values, units in cm 3 molecule -1 s -1 ): k(CH 3 + HCl) = [1.004 + 85.64 exp (-0.02438 x T/K)] x (3.3 ± 1.3) x 10 -13 exp [-(4.8 ± 0.6) kJ mol -1 /RT] and k(CD 3 + HCl) = [1.002 + 73.31 exp (-0.02505 x T/K)] x (2.7 ± 1.2) x 10 -13 exp [-(3.5 ± 0.5) kJ mol -1 /RT]. The radical reactions with DCl were studied separately over a wide ranges of temperatures and in these temperature ranges the rate constants determined were fitted to a conventional Arrhenius expression k = A exp (-E a /RT) (error limits stated are 1σ + Students t values, units in cm 3 molecule -1 s -1 ): k(CH 3 + DCl) = (2.4 ± 1.6) x 10 -13 exp [-(7.8 ± 1.4) kJ mol -1 /RT] and k(CD 3 + DCl) = (1.2 ± 0.4) x 10 -13 exp [-(5.2 ± 0.2) kJ mol -1 /RT] cm 3 molecule -1 s -1 . Curvature in the Arrhenius plots of the H-atom abstraction reactions at low temperatures was analyzed by considering H-atom tunneling through the reaction barrier and primary kinetic isotope effect. Contribution of tunneling in it was concluded to be negligible. In addition, secondary isotope effect was measured

  5. ISLSCP II GlobalView: Atmospheric Methane Concentrations

    Data.gov (United States)

    National Aeronautics and Space Administration — The GlobalView Methane (CH4) data product contains synchronized and smoothed time series of atmospheric CH4 concentrations at selected sites that were created using...

  6. Method for indirect quantification of CH4 production via H2O production using hydrogenotrophic methanogens

    Directory of Open Access Journals (Sweden)

    Ruth-Sophie eTaubner

    2016-04-01

    Full Text Available ydrogenotrophic methanogens are an intriguing group of microorganisms from the domain Archaea. They exhibit extraordinary ecological, biochemical, physiological characteristics colorbox{yellow}{and have a huge biotechnological potential}. Yet, the only possibility to assess the methane (CH$_4$ production potential of hydrogenotrophic methanogens is to apply gas chromatographic quantification of CH$_4$.In order to be able to effectively screen pure cultures of hydrogenotrophic methanogens regarding their CH$_4$ production potential we developed a novel method for indirect quantification of colorbox{yellow}{the} volumetric CH$_4$ production rate by measuring colorbox{yellow}{the} volumetric water production rate. This colorbox{yellow}{ } method was established in serum bottles for cultivation of methanogens in closed batch cultivation mode. Water production was colorbox{yellow}{estimated} by determining the difference in mass increase in an isobaric setting.This novel CH$_4$ quantification method is an accurate and precise analytical technique, colorbox{yellow}{which can be used} to rapidly screen pure cultures of methanogens regarding colorbox{yellow}{their} volumetric CH$_{4}$ evolution rate. colorbox{yellow}{It} is a cost effective alternative colorbox{yellow}{determining} CH$_4$ production of methanogens over CH$_4$ quantification by using gas chromatography, especially if colorbox{yellow}{ } applied as a high throughput quantification method. colorbox{yellow}{Eventually, the} method can be universally applied for quantification of CH$_4$ production from psychrophilic, thermophilic and hyperthermophilic hydrogenotrophic methanogens.

  7. Revisiting global mean sea level budget closure : Preliminary results from an integrative study within ESA's Climate Change Initiative -Sea level Budget Closure-Climate Change Initiative

    Science.gov (United States)

    Palanisamy, H.; Cazenave, A. A.

    2017-12-01

    The global mean sea level budget is revisited over two time periods: the entire altimetry era, 1993-2015 and the Argo/GRACE era, 2003-2015 using the version '0' of sea level components estimated by the SLBC-CCI teams. The SLBC-CCI is an European Space Agency's project on sea level budget closure using CCI products. Over the entire altimetry era, the sea level budget was performed as the sum of steric and mass components that include contributions from total land water storage, glaciers, ice sheets (Greenland and Antarctica) and total water vapor content. Over the Argo/GRACE era, it was performed as the sum of steric and GRACE based ocean mass. Preliminary budget analysis performed over the altimetry era (1993-2015) results in a trend value of 2.83 mm/yr. On comparison with the observed altimetry-based global mean sea level trend over the same period (3.03 ± 0.5 mm/yr), we obtain a residual of 0.2 mm/yr. In spite of a residual of 0.2 mm/yr, the sea level budget result obtained over the altimetry era is very promising as this has been performed using the version '0' of the sea level components. Furthermore, uncertainties are not yet included in this study as uncertainty estimation for each sea level component is currently underway. Over the Argo/GRACE era (2003-2015), the trend estimated from the sum of steric and GRACE ocean mass amounts to 2.63 mm/yr while that observed by satellite altimetry is 3.37 mm/yr, thereby leaving a residual of 0.7 mm/yr. Here an ensemble GRACE ocean mass data (mean of various available GRACE ocean mass data) was used for the estimation. Using individual GRACE data results in a residual range of 0.5 mm/yr -1.1 mm/yr. Investigations are under way to determine the cause of the vast difference between the observed sea level and the sea level obtained from steric and GRACE ocean mass. One main suspect is the impact of GRACE data gaps on sea level budget analysis due to lack of GRACE data over several months since 2011. The current action plan

  8. Facile And Reversible Co Insertion Into The Ir-ch3 Bond Of [ir4(ch3)(co)8(μ4- η3-ph2pccph)(μ-pph2)

    OpenAIRE

    Vargas M.D.; Pereira R.M.S.; Braga D.; Grepioni F.

    1993-01-01

    Reaction of [Ir4H(CO)10(mu-PPh2)) with BuLi, Ph2PC=CPh and then Mel gives [Ir4(CH3)(CO)8(mu4-eta3-Ph2PCCPh)(mu-PPh2)], which undergoes a reversible two-step CO insertion under extremely mild conditions to yield Ir4{(CH3C(O)}(CO)8-(mu4:eta3-Ph2PCCPh)(mu-PPh2)] as the final product; the structures of both species have been established by X-ray diffraction studies.

  9. Automatic installation of separating 13CH4 from natural CH4, representing a profiled cascade, achieved on the basis of the thermodiffusion column study

    International Nuclear Information System (INIS)

    Ghete, P.

    1976-01-01

    In order to enrich 13 CH 4 from natural CH 4 , an installation, partly automated, has been achieved, using thermodifussion as a separation process for stable isotopes. The thermodifussion columns is original both as construction and solution used for heating the concentric tube. It has been studied the heat transfer properties of the column, the mass transfer and it has been realized an original calculation program concerning the T.D. cascade performances, pointing out an energetical optimum. The experimental results are presented in diagrams each point representing the result of the statistical processing of at least 10 experimental measurements. (author)

  10. Experimental confirmation of the Jahn-Teller distortion of CH4+

    International Nuclear Information System (INIS)

    Gemmell, D.S.; Kanter, E.P.; Pietsch, W.J.

    1979-01-01

    Measured energy and angular distributions are reported for H + and C/sup n+/ (n = 2,3,4) fragments resulting from the collisional dissociation of 200-keV/amu CH/sub m/ + (m = 0 to 4) in thin carbon targets. From the systematic trends of these Coulomb explosion spectra, qualitative information can be obtained on the structures of these species. In particular, the series displays a narrowing of the carbon angular and energy widths as protons are symmetrically added around a central carbon atom and provide a focusing effect. Because of the Jahn-Teller distortion, the carbon width in CH 4 + is dramatically increased. 8 references

  11. FY97 nuclear-related budgets total 493 billion yen (4.4 billion dollars)

    International Nuclear Information System (INIS)

    Anon.

    1996-01-01

    On September 13, the Atomic Energy Commission of Japan announced the estimated nuclear-related budget requests for FY1997 (April, 1997 - Mach, 1998), giving the breakdowns for eight ministries and agencies. The total amount requested by the government bodies was 493.3 billion yen, 0.8% increase as compared with FY96. this figure includes the budget requests of the Science and Technology Agency (STA), the Ministry of International Trade and Industry (MITI), the Ministry of Foreign Affairs, the Ministry of Transport, the Ministry of Agriculture, Forestry and Fisheries, the Okinawa Development Agency, and the Ministry of Home Affairs, but excludes the budget request made by the Ministry of Education. The budget requests of STA and MITI are 360 billion yen and 126 billion yen, respectively. On August 29, STA released its estimated FY97 budget request. The nuclear-related 360.4 billion yen is 0.9% more than that in year before. Of this sum, 199.9 billion yen is in the general account, and 160.6 billion yen is in the special account for power source development. The details of the nuclear-related amounts are explained. On August 26, MITI released its estimated budget request for FY97, and of the nuclear-related 125.7 billion yen (0.1% increase from FY96), 200 million yen is in the general account, and 98.9 billion yen and 26.6 billion yen are in the special accounts for power resource development and power source diversification, respectively. (K.I.)

  12. Comparisons of continuous atmospheric CH4, CO2 and N2O measurements - results from a travelling instrument campaign at Mace Head

    International Nuclear Information System (INIS)

    Vardag, S.N.; Hammer, S.; Levin, I.; O'Doherty, S.; Spain, T.G.; Wastine, B.; Jordan, A.

    2014-01-01

    A 2-month measurement campaign with a Fourier transform infrared analyser as a travelling comparison instrument (TCI) was performed at the Advanced Global Atmospheric Gases Experiment (AGAGE) and World Meteorological Organization (WMO) Global Atmosphere Watch (GAW) station at Mace Head, Ireland. The aim was to evaluate the compatibility of atmospheric methane (CH 4 ), carbon dioxide (CO 2 ) and nitrous oxide (N 2 O) measurements of the routine station instrumentation, consisting of a gas chromatograph (GC) for CH 4 and N 2 O as well as a cavity ring-down spectroscopy (CRDS) system for CH 4 and CO 2 . The advantage of a TCI approach for quality control is that the comparison covers the entire ambient air measurement system, including the sample intake system and the data evaluation process. For initial quality and performance control, the TCI was run in parallel with the Heidelberg GC before and after the measurement campaign at Mace Head. Median differences between the Heidelberg GC and the TCI were well within the WMO inter-laboratory compatibility target for all three greenhouse gases. At Mace Head, the median difference between the station GC and the TCI were -0.04 nmol mol -1 for CH 4 and -0.37 nmol mol -1 for N 2 O (GC-TCI). For N 2 O, a similar difference (-0.40 nmol mol -1 ) was found when measuring surveillance or working gas cylinders with both instruments. This suggests that the difference observed in ambient air originates from a calibration offset that could partly be due to a difference between the WMON2O X2006a reference scale used for the TCI and the Scripps Institution of Oceanography (SIO-1998) scale used at Mace Head and in the whole AGAGE network. Median differences between the CRDS G1301 and the TCI at Mace Head were 0.12 nmol mol -1 for CH 4 and 0.14 μmol mol -1 for CO 2 (CRDS G1301 - TCI). The difference between both instruments for CO 2 could not be explained, as direct measurements of calibration gases show no such difference. The CH 4

  13. Global atmospheric budget of simple monocyclic aromatic compounds

    Directory of Open Access Journals (Sweden)

    D. Cabrera-Perez

    2016-06-01

    Full Text Available The global atmospheric budget and distribution of monocyclic aromatic compounds is estimated, using an atmospheric chemistry general circulation model. Simulation results are evaluated with an ensemble of surface and aircraft observations with the goal of understanding emission, production and removal of these compounds.Anthropogenic emissions provided by the RCP database represent the largest source of aromatics in the model (≃ 23 TgC year−1 and biomass burning from the GFAS inventory the second largest (≃ 5 TgC year−1. The simulated chemical production of aromatics accounts for  ≃ 5 TgC year−1. The atmospheric burden of aromatics sums up to 0.3 TgC. The main removal process of aromatics is photochemical decomposition (≃ 27 TgC  year−1, while wet and dry deposition are responsible for a removal of  ≃ 4 TgC year−1.Simulated mixing ratios at the surface and elsewhere in the troposphere show good spatial and temporal agreement with the observations for benzene, although the model generally underestimates mixing ratios. Toluene is generally well reproduced by the model at the surface, but mixing ratios in the free troposphere are underestimated. Finally, larger discrepancies are found for xylenes: surface mixing ratios are not only overestimated but also a low temporal correlation is found with respect to in situ observations.

  14. Synthesis and thermolysis of Cp*(C5Me4CH2)TiR complexes

    NARCIS (Netherlands)

    Luinstra, GA; Brinkmann, PHP; Teuben, JH; Luinstra, Gerrit A.

    1997-01-01

    Substitution of the chloride in Cp*FvTiCl with MR (Fv = C5Me4CH2; R = Me, CH2SiMe3, CH2CMe3, CH = CH2, M = Li; R = CH2Ph, M = K; R = C3H5, M = MgCl; R = Ph, M = Na . NaCl) gives Cp*FvTiR. NMR spectroscopic evidence points towards a series of structurally related compounds with a bent-sandwich

  15. Large CO2 and CH4 release from a flooded formerly drained fen

    Science.gov (United States)

    Sachs, T.; Franz, D.; Koebsch, F.; Larmanou, E.; Augustin, J.

    2016-12-01

    Drained peatlands are usually strong carbon dioxide (CO2) sources. In Germany, up to 4.5 % of the national CO2 emissions are estimated to be released from agriculturally used peatlands and for some peatland-rich northern states, such as Mecklenburg-Western Pomerania, this share increases to about 20%. Reducing this CO2 source and restoring the peatlands' natural carbon sink is one objective of large-scale nature protection and restoration measures, in which 37.000 ha of drained and degraded peatlands in Mecklenburg-Western Pomerania are slated for rewetting. It is well known, however, that in the initial phase of rewetting, a reduction of the CO2 source strength is usually accompanied by an increase in CH4 emissions. Thus, whether and when the intended effects of rewetting with regard to greenhouse gases are achieved, depends on the balance of CO2 and CH4 fluxes and on the duration of the initial CH4 emission phase. In 2013, a new Fluxnet site went online at a flooded formerly drained river valley fen site near Zarnekow, NE Germany (DE-Zrk), to investigate the combined CO2 and CH4 dynamics at such a heavily degraded and rewetted peatland. The site is dominated by open water with submerged and floating vegetation and surrounding Typha latifolia.Nine year after rewetting, we found large CH4 emissions of 53 g CH4 m-2 a-1 from the open water area, which are 4-fold higher than from the surrounding vegetation zone (13 g CH4 m-2 a-1). Surprisingly, both the open water and the vegetated area were net CO2 sources of 158 and 750 g CO2 m-2 a-1, respectively. Unusual meteorological conditions with a warm and dry summer and a mild winter might have facilitated high respiration rates, particularly from temporally non-inundated organic mud in the vegetation zone.

  16. Constraining the carbon tetrachloride (CCl4) budget using its global trend and inter-hemispheric gradient

    Science.gov (United States)

    Liang, Qing; Newman, Paul A.; Daniel, John S.; Reimann, Stefan; Hall, Bradley D.; Dutton, Geoff; Kuijpers, Lambert J. M.

    2014-07-01

    Carbon tetrachloride (CCl4) is a major anthropogenic ozone-depleting substance and greenhouse gas and has been regulated under the Montreal Protocol. However, the near-zero 2007-2012 emissions estimate based on the UNEP reported production and feedstock usage cannot be reconciled with the observed slow decline of atmospheric concentrations and the inter-hemispheric gradient (IHG) for CCl4. Our 3-D model simulations suggest that the observed IHG (1.5 ± 0.2 ppt for 2000-2012) is primarily caused by ongoing current emissions, while ocean and soil losses and stratosphere-troposphere exchange together contribute a small negative gradient (~0 - -0.3 ppt). Using the observed CCl4 global trend and IHG, we deduce that the mean global emissions for the 2000-2012 period are 393445 Gg/yr (~30% of the peak 1980s emissions) and a corresponding total lifetime of 353732 years.

  17. From California dreaming to California data: Challenging historic models for landfill CH4 emissions

    OpenAIRE

    Spokas, Kurt; Bogner, Jean; Corcoran, Meg; Walker, Scott

    2015-01-01

    Abstract Improved quantification of diverse CH4 sources at the urban scale is needed to guide local GHG mitigation strategies in the Anthropocene. Herein, we focus on landfill CH4 emissions in California, challenging the current IPCC methodology which focuses on a climate dependency for landfill CH4 generation (methanogenesis), but does not explicitly consider climate or soil dependencies for emissions. Relying on a comprehensive California landfill database, a field-validated process-based m...

  18. Focus on cumulative emissions, global carbon budgets and the implications for climate mitigation targets

    Science.gov (United States)

    Damon Matthews, H.; Zickfeld, Kirsten; Knutti, Reto; Allen, Myles R.

    2018-01-01

    The Environmental Research Letters focus issue on ‘Cumulative Emissions, Global Carbon Budgets and the Implications for Climate Mitigation Targets’ was launched in 2015 to highlight the emerging science of the climate response to cumulative emissions, and how this can inform efforts to decrease emissions fast enough to avoid dangerous climate impacts. The 22 research articles published represent a fantastic snapshot of the state-or-the-art in this field, covering both the science and policy aspects of cumulative emissions and carbon budget research. In this Review and Synthesis, we summarize the findings published in this focus issue, outline some suggestions for ongoing research needs, and present our assessment of the implications of this research for ongoing efforts to meet the goals of the Paris climate agreement.

  19. Hospital non-price competition under the Global Budget Payment and Prospective Payment Systems.

    Science.gov (United States)

    Chen, Wen-Yi; Lin, Yu-Hui

    2008-06-01

    This paper provides theoretical analyses of two alternative hospital payment systems for controlling medical cost: the Global Budget Payment System (GBPS) and the Prospective Payment System (PPS). The former method assigns a fixed total budget for all healthcare services over a given period with hospitals being paid on a fee-for-service basis. The latter method is usually connected with a fixed payment to hospitals within a Diagnosis-Related Group. Our results demonstrate that, given the same expenditure, the GBPS would approach optimal levels of quality and efficiency as well as the level of social welfare provided by the PPS, as long as market competition is sufficiently high; our results also demonstrate that the treadmill effect, modeling an inverse relationship between price and quantity under the GBPS, would be a quality-enhancing and efficiency-improving outcome due to market competition.

  20. Improved CRDS δ13C Stability Through New Calibration Application For CO2 And CH4

    Science.gov (United States)

    Rella, Chris; Arata, Caleb; Saad, Nabil; Leggett, Graham; Miles, Natasha; Richardson, Scott; Davis, Ken

    2015-04-01

    Stable carbon isotope ratio measurements of CO2 and CH4 provide valuable insight into global and regional sources and sinks of the two most important greenhouse gases. Methodologies based on Cavity Ring-Down Spectroscopy (CRDS) have been developed and are capable of delivering δ13C measurements with a precision better than 0.12 permil for CO2 and 0.4 permil for CH4 (1 hour window, 5 minute average). Here we present a method to further improve this measurement stability. We have developed a two-point calibration method which corrects for δ13C drift due to a dependence on carbon species concentration. This method calibrates for both carbon species concentration as well as δ13C. In addition, we further demonstrate that this added stability is especially valuable when using carbon isotope data in linear regression models such as Keeling plots, where even small amounts of error can be magnified to give inconclusive results. Furthermore, we show how this method is used to validate multiple instruments simultaneously and can be used to create the standard samples needed for field calibrations.

  1. Methane Feedbacks to the Global Climate System in a Warmer World

    Science.gov (United States)

    Dean, Joshua F.; Middelburg, Jack J.; Röckmann, Thomas; Aerts, Rien; Blauw, Luke G.; Egger, Matthias; Jetten, Mike S. M.; de Jong, Anniek E. E.; Meisel, Ove H.; Rasigraf, Olivia; Slomp, Caroline P.; in't Zandt, Michiel H.; Dolman, A. J.

    2018-03-01

    Methane (CH4) is produced in many natural systems that are vulnerable to change under a warming climate, yet current CH4 budgets, as well as future shifts in CH4 emissions, have high uncertainties. Climate change has the potential to increase CH4 emissions from critical systems such as wetlands, marine and freshwater systems, permafrost, and methane hydrates, through shifts in temperature, hydrology, vegetation, landscape disturbance, and sea level rise. Increased CH4 emissions from these systems would in turn induce further climate change, resulting in a positive climate feedback. Here we synthesize biological, geochemical, and physically focused CH4 climate feedback literature, bringing together the key findings of these disciplines. We discuss environment-specific feedback processes, including the microbial, physical, and geochemical interlinkages and the timescales on which they operate, and present the current state of knowledge of CH4 climate feedbacks in the immediate and distant future. The important linkages between microbial activity and climate warming are discussed with the aim to better constrain the sensitivity of the CH4 cycle to future climate predictions. We determine that wetlands will form the majority of the CH4 climate feedback up to 2100. Beyond this timescale, CH4 emissions from marine and freshwater systems and permafrost environments could become more important. Significant CH4 emissions to the atmosphere from the dissociation of methane hydrates are not expected in the near future. Our key findings highlight the importance of quantifying whether CH4 consumption can counterbalance CH4 production under future climate scenarios.

  2. 4-(2-Tetrathiafulvalenyl-ethenyl)pyridine (TTF-CH=CH-Py) radical cation salts containing poly(beta-diketonate) rare earth complexes: synthesis, crystal structure, photoluminescent and magnetic properties.

    Science.gov (United States)

    Pointillart, Fabrice; Maury, Olivier; Le Gal, Yann; Golhen, Stéphane; Cador, Olivier; Ouahab, Lahcène

    2009-08-03

    The reactions between the redox-active 4-(2-tetrathiafulvalenyl-ethenyl)pyridine ligand (TTF-CH=CH-Py) and the tris(1,1,1,5,5,5-hexafluoroacetylacetonate)Ln(III) (Ln = La and Nd) lead to the formation of compounds with the formulas {[La(hfac)(5)][(TTF-CH=CH-Py(*+))](2)} (1), {[Nd(hfac)(4)(H(2)O)][(TTF-CH=CH-Py(*+))]}(2) (2), and {[Nd(hfac)(4)(H(2)O)][(TTF-CH=CH-Py(*+))]}(2)(H(2)O)(C(6)H(14))(0.5) (3) (hfac(-) = 1,1,1,5,5,5-hexafluoroacetylacetonate anion). These compounds have been characterized by single-crystal X-ray diffraction, optical, and magnetic measurements. Compounds 1, 2, and 3 crystallize in the monoclinic C2/c, triclinic P1, and monoclinic P2(1)/c space groups, respectively. La(III) adopts a tetradecahedral geometry, while Nd(III) stands in a distorted capped square antiprism one. In 1, the inorganic network is formed by the [La(hfac)(5)](2-) dianionic complexes, while it is formed by a pseudo-dimeric dianionic unit of formula {[Nd(hfac)(4)(H(2)O)](2)}(2-) in 2 and 3. In all crystal structures, the organic network is constituted by the TTF-CH=CH-Py(*+) radical cations. The inorganic and organic networks interact through intermolecular contacts between the pyridine moieties of the TTF-CH=CH-Py(*+) radical cations and the Ln(III) ions. The luminescence properties of the Nd(III) ions (9400 cm(-1)) and fluorescence band of the TTF-CH=CH-Py(*+) radical cations (10200 cm(-1)) have been observed and studied for compound 2. Complexes 2 and 3 are paramagnetic because of Nd(III) ions. Compound 2 is a paramagnetic luminescent TTF-radical-cation-based material. Resistivity measurements have also been performed on these materials.

  3. Application of machine learning methods to histone methylation ChIP-Seq data reveals H4R3me2 globally represses gene expression

    Science.gov (United States)

    2010-01-01

    Background In the last decade, biochemical studies have revealed that epigenetic modifications including histone modifications, histone variants and DNA methylation form a complex network that regulate the state of chromatin and processes that depend on it including transcription and DNA replication. Currently, a large number of these epigenetic modifications are being mapped in a variety of cell lines at different stages of development using high throughput sequencing by members of the ENCODE consortium, the NIH Roadmap Epigenomics Program and the Human Epigenome Project. An extremely promising and underexplored area of research is the application of machine learning methods, which are designed to construct predictive network models, to these large-scale epigenomic data sets. Results Using a ChIP-Seq data set of 20 histone lysine and arginine methylations and histone variant H2A.Z in human CD4+ T-cells, we built predictive models of gene expression as a function of histone modification/variant levels using Multilinear (ML) Regression and Multivariate Adaptive Regression Splines (MARS). Along with extensive crosstalk among the 20 histone methylations, we found H4R3me2 was the most and second most globally repressive histone methylation among the 20 studied in the ML and MARS models, respectively. In support of our finding, a number of experimental studies show that PRMT5-catalyzed symmetric dimethylation of H4R3 is associated with repression of gene expression. This includes a recent study, which demonstrated that H4R3me2 is required for DNMT3A-mediated DNA methylation--a known global repressor of gene expression. Conclusion In stark contrast to univariate analysis of the relationship between H4R3me2 and gene expression levels, our study showed that the regulatory role of some modifications like H4R3me2 is masked by confounding variables, but can be elucidated by multivariate/systems-level approaches. PMID:20653935

  4. BOREAS TGB-1 CH4 Concentration and Flux Data from NSA Tower Sites

    Science.gov (United States)

    Hall, Forrest G. (Editor); Conrad, Sara K. (Editor); Crill, Patrick; Varner, Ruth K.

    2000-01-01

    The BOREAS TGB-1 team made numerous measurements of trace gas concentrations and fluxes at various NSA sites. This data set contains half-hourly averages of ambient methane (CH4) measurements and calculated fluxes for the NSA-Fen in 1996 and the NSA-BP and NSA-OJP tower sites in 1994. The purpose of this study was to determine the CH4 flux from the study area by measuring ambient CH 4 concentrations. This flux can then be compared to the chamber flux measurements taken at the same sites. The data are provided in tabular ASCII files.

  5. Impacts of climate and land use on N2 O and CH4 fluxes from tropical ecosystems in the Mt. Kilimanjaro region, Tanzania.

    Science.gov (United States)

    Gütlein, Adrian; Gerschlauer, Friederike; Kikoti, Imani; Kiese, Ralf

    2018-03-01

    In this study, we quantify the impacts of climate and land use on soil N 2 O and CH 4 fluxes from tropical forest, agroforest, arable and savanna ecosystems in Africa. To do so, we measured greenhouse gases (GHG) fluxes from 12 different ecosystems along climate and land-use gradients at Mt. Kilimanjaro, combining long-term in situ chamber and laboratory soil core incubation techniques. Both methods showed similar patterns of GHG exchange. Although there were distinct differences from ecosystem to ecosystem, soils generally functioned as net sources and sinks for N 2 O and CH 4 respectively. N 2 O emissions correlated positively with soil moisture and total soil nitrogen content. CH 4 uptake rates correlated negatively with soil moisture and clay content and positively with SOC. Due to moderate soil moisture contents and the dominance of nitrification in soil N turnover, N 2 O emissions of tropical montane forests were generally low (<1.2 kg N ha -1  year -1 ), and it is likely that ecosystem N losses are driven instead by nitrate leaching (~10 kg N ha -1  year -1 ). Forest soils with well-aerated litter layers were a significant sink for atmospheric CH 4 (up to 4 kg C ha -1  year -1 ) regardless of low mean annual temperatures at higher elevations. Land-use intensification significantly increased the soil N 2 O source strength and significantly decreased the soil CH 4 sink. Compared to decreases in aboveground and belowground carbon stocks enhanced soil non-CO 2 GHG emissions following land-use conversion from tropical forests to homegardens and coffee plantations were only a small factor in the total GHG budget. However, due to lower ecosystem carbon stock changes, enhanced N 2 O emissions significantly contributed to total GHG emissions following conversion of savanna into grassland and particularly maize. Overall, we found that the protection and sustainable management of aboveground and belowground carbon and nitrogen stocks of agroforestry and

  6. Emissions of CO2, CO, NOx, HC, PM, HFC-134a, N2O and CH4 from the global light duty vehicle fleet

    Directory of Open Access Journals (Sweden)

    Timothy J. Wallington

    2008-04-01

    Full Text Available Vehicles emit carbon dioxide (CO2, carbon monoxide (CO, nitrogen oxides (NOx, hydrocarbons (HC, particulate matter (PM, hydrofluorocarbon 134a (HFC-134a, methane (CH4, and nitrous oxide (N2O. An understanding of these emissions is needed in discussions of climate change and local air pollution issues. To facilitate such discussions an overview of past, present, and likely future emissions from light duty vehicles is presented. Emission control technologies have reduced the emissions of CO, VOCs, PM, HFC-134a, CH4, and N2O from modern vehicles to very low levels.

  7. CO2 adsorption-assisted CH4 desorption on carbon models of coal surface: A DFT study

    Science.gov (United States)

    Xu, He; Chu, Wei; Huang, Xia; Sun, Wenjing; Jiang, Chengfa; Liu, Zhongqing

    2016-07-01

    Injection of CO2 into coal is known to improve the yields of coal-bed methane gas. However, the technology of CO2 injection-enhanced coal-bed methane (CO2-ECBM) recovery is still in its infancy with an unclear mechanism. Density functional theory (DFT) calculations were performed to elucidate the mechanism of CO2 adsorption-assisted CH4 desorption (AAD). To simulate coal surfaces, different six-ring aromatic clusters (2 × 2, 3 × 3, 4 × 4, 5 × 5, 6 × 6, and 7 × 7) were used as simplified graphene (Gr) carbon models. The adsorption and desorption of CH4 and/or CO2 on these carbon models were assessed. The results showed that a six-ring aromatic cluster model (4 × 4) can simulate the coal surface with limited approximation. The adsorption of CO2 onto these carbon models was more stable than that in the case of CH4. Further, the adsorption energies of single CH4 and CO2 in the more stable site were -15.58 and -18.16 kJ/mol, respectively. When two molecules (CO2 and CH4) interact with the surface, CO2 compels CH4 to adsorb onto the less stable site, with a resulting significant decrease in the adsorption energy of CH4 onto the surface of the carbon model with pre-adsorbed CO2. The Mulliken charges and electrostatic potentials of CH4 and CO2 adsorbed onto the surface of the carbon model were compared to determine their respective adsorption activities and changes. At the molecular level, our results showed that the adsorption of the injected CO2 promoted the desorption of CH4, the underlying mechanism of CO2-ECBM.

  8. Temperature-dependent kinetics of charge transfer, hydrogen-atom transfer, and hydrogen-atom expulsion in the reaction of CO+ with CH4 and CD4.

    Science.gov (United States)

    Melko, Joshua J; Ard, Shaun G; Johnson, Ryan S; Shuman, Nicholas S; Guo, Hua; Viggiano, Albert A

    2014-09-18

    We have determined the rate constants and branching ratios for the reactions of CO(+) with CH4 and CD4 in a variable-temperature selected ion flow tube. We find that the rate constants are collisional for all temperatures measured (193-700 K for CH4 and 193-500 K for CD4). For the CH4 reaction, three product channels are identified, which include charge transfer (CH4(+) + CO), H-atom transfer (HCO(+) + CH3), and H-atom expulsion (CH3CO(+) + H). H-atom transfer is slightly preferred to charge transfer at low temperature, with the charge-transfer product increasing in contribution as the temperature is increased (H-atom expulsion is a minor product for all temperatures). Analogous products are identified for the CD4 reaction. Density functional calculations on the CO(+) + CH4 reaction were also conducted, revealing that the relative temperature dependences of the charge-transfer and H-atom transfer pathways are consistent with an initial charge transfer followed by proton transfer.

  9. Russian boreal peatlands dominate the natural European methane budget

    International Nuclear Information System (INIS)

    Schneider, Julia; Jungkunst, Hermann F; Wolf, Ulrike; Schreiber, Peter; Kutzbach, Lars; Gazovic, Michal; Miglovets, Mikhail; Mikhaylov, Oleg; Grunwald, Dennis; Erasmi, Stefan; Wilmking, Martin

    2016-01-01

    About 60% of the European wetlands are located in the European part of Russia. Nevertheless, data on methane emissions from wetlands of that area are absent. Here we present results of methane emission measurements for two climatically different years from a boreal peatland complex in European Russia. Winter fluxes were well within the range of what has been reported for the peatlands of other boreal regions before, but summer fluxes greatly exceeded the average range of 5–80 mg CH 4 m −2 d −1 for the circumpolar boreal zone. Half of the measured fluxes ranged between 150 and 450 mg CH 4 m −2 d −1 . Extrapolation of our data to the whole boreal zone of European Russia shows that theses emissions could amount to up to 2.7 ± 1.1 Tg CH 4 a −1 , corresponding to 69% of the annual emissions from European wetlands or 33% of the total annual natural European methane emission. In 2008, climatic conditions corresponded to the long term mean, whereas the summer of 2011 was warmer and noticeably drier. Counterintuitively, these conditions led to even higher CH 4 emissions, with peaks up to two times higher than the values measured in 2008. As Russian peatlands dominate the areal extend of wetlands in Europe and are characterized by very high methane fluxes to the atmosphere, it is evident, that sound European methane budgeting will only be achieved with more insight into Russian peatlands. (letter)

  10. CO2 and CH4 fluxes of contrasting pristine bogs in southern Patagonia (Tierra del Fuego, Argentina)

    Science.gov (United States)

    Münchberger, Wiebke; Blodau, Christian; Kleinebecker, Till; Pancotto, Veronica

    2015-04-01

    South Patagonian peatlands cover a wide range of the southern terrestrial area and thus are an important component of the terrestrial global carbon cycle. These extremely southern ecosystems have been accumulating organic material since the last glaciation up to now and are - in contrast to northern hemisphere bogs - virtually unaffected by human activities. So far, little attention has been given to these pristine ecosystems and great carbon reservoirs which will potentially be affected by climate change. We aim to fill the knowledge gap in the quantity of carbon released from these bogs and in what controls their fluxes. We study the temporal and spatial variability of carbon fluxes in two contrasting bog ecosystems in southern Patagonia, Tierra del Fuego. Sphagnum-dominated bog ecosystems in Tierra del Fuego are similar to the ones on the northern hemisphere, while cushion plant-dominated bogs can almost exclusively be found in southern Patagonia. These unique cushion plant-dominated bogs are found close to the coast and their occurrence changes gradually to Sphagnum-dominated bogs with increasing distance from the coast. We conduct closed chamber measurements and record relevant environmental variables for CO2 and CH4 fluxes during two austral vegetation periods from December to April. Chamber measurements are performed on microforms representing the main vegetation units of the studied bogs. Gas concentrations are measured with a fast analyzer (Los Gatos Ultraportable Greenhouse Gas Analyzer) allowing to accurately record CH4 fluxes in the ppm range. We present preliminary results of the carbon flux variability from south Patagonian peat bogs and give insights into their environmental controls. Carbon fluxes of these two bog types appear to be highly different. In contrast to Sphagnum-dominated bogs, cushion plant-dominated bogs release almost no CH4 while their CO2 flux in both, photosynthesis and respiration, can be twice as high as for Sphagnum

  11. Biotic controls on CO2 and CH4 exchange in wetlands - a closed environment study

    DEFF Research Database (Denmark)

    Christensen, TR; Panikov, N; Mastepanov, M

    2003-01-01

    Wetlands are significant sources of the important greenhouse gas CH4. Here we explore the use of an experimental system developed for the determination of continuous fluxes of CO2 and CH4 in closed ecosystem monoliths including the capture of (CO2)-C-14 and (CH4)-C-14 following pulse labelling...... with (CO2)-C-14. We show that, in the ecosystem studied, ebullition (bubble emission) may account for 18 to 50% of the total CH4 emission, representing fluxes that have been difficult to estimate accurately in the past. Furthermore, using plant removal and C-14 labelling techniques, we use the system....../atmosphere interactions, including possible feedback effects on climate change. In recent years much attention has been devoted to ascertaining and subsequently using the relationship between net ecosystem productivity and CH4 emission as a basis for extrapolation of fluxes across large areas. The experimental system...

  12. Evaluating CO2 and CH4 dynamics of Alaskan ecosystems during the Holocene Thermal Maximum

    Science.gov (United States)

    He, Yujie; Jones, Miriam C.; Zhuang, Qianlai; Bochicchio, Christopher; Felzer, B. S.; Mason, Erik; Yu, Zicheng

    2014-01-01

    The Arctic has experienced much greater warming than the global average in recent decades due to polar amplification. Warming has induced ecological changes that have impacted climate carbon-cycle feedbacks, making it important to understand the climate and vegetation controls on carbon (C) dynamics. Here we used the Holocene Thermal Maximum (HTM, 11–9 ka BP, 1 ka BP = 1000 cal yr before present) in Alaska as a case study to examine how ecosystem Cdynamics responded to the past warming climate using an integrated approach of combining paleoecological reconstructions and ecosystem modeling. Our paleoecological synthesis showed expansion of deciduous broadleaf forest (dominated by Populus) into tundra and the establishment of boreal evergreen needleleaf and mixed forest during the second half of the HTM under a warmer- and wetter-than-before climate, coincident with the occurrence of the highest net primary productivity, cumulative net ecosystem productivity, soil C accumulation and CH4 emissions. These series of ecological and biogeochemical shifts mirrored the solar insolation and subsequent temperature and precipitation patterns during HTM, indicating the importance of climate controls on C dynamics. Our simulated regional estimate of CH4 emission rates from Alaska during the HTM ranged from 3.5 to 6.4 Tg CH4 yr−1 and highest annual NPP of 470 Tg C yr−1, significantly higher than previously reported modern estimates. Our results show that the differences in static vegetation distribution maps used in simulations of different time slices have greater influence on modeled C dynamics than climatic fields within each time slice, highlighting the importance of incorporating vegetation community dynamics and their responses to climatic conditions in long-term biogeochemical modeling.

  13. The IAGOS-core greenhouse gas package : a measurement system for continuous airborne observations of CO2, CH4, H2O and CO

    NARCIS (Netherlands)

    Filges, Annette; Gerbig, Christoph; Chen, Huilin; Franke, Harald; Klaus, Christoph; Jordan, Armin

    2015-01-01

    Within the framework of IAGOS-ERI (In-service Aircraft for a Global Observing System - European Research Infrastructure), a cavity ring-down spectroscopy (CRDS)-based measurement system for the autonomous measurement of the greenhouse gases (GHGs) CO2 and CH4, as well as CO and water vapour was

  14. Annual variation of CH{sub 4} emissions from the middle taiga in West Siberian Lowland (2005-2009): a case of high CH{sub 4} flux and precipitation rate in the summer of 2007

    Energy Technology Data Exchange (ETDEWEB)

    Sasakawa, M.; Ito, A.; Machida, T. (Center for Global Environmental Research, National Inst. for Environmental Studies, Tsukuba (Japan)), Email: sasakawa.motoki@nies.go.jp; Tsuda, N. (Global Environmental Forum, Bunkyo-ku Tokyo (Japan)); Niwa, Y. (Meteorological Research Inst., Tsukuba (Japan)); Davydov, D.; Fofonov, A.; Arshinov, M. (V.E. Zuev Inst. of Atmospheric Optics, Russian Academy of Sciences, Siberian Branch, Tomsk (Russian Federation))

    2012-03-15

    We described continuous measurements of CH{sub 4} and CO{sub 2} concentration obtained at two sites placed in the middle taiga, Karasevoe (KRS) and Demyanskoe (DEM), in West Siberian Lowland (WSL) from 2005 to 2009. Although both CH{sub 4} and CO{sub 2} accumulation (DELTACH{sub 4} and DELTACO{sub 2}) during night-time at KRS in June and July 2007 showed an anomalously high concentration, higher ratios of DELTACH{sub 4}/DELTACO{sub 2} compared with those in other years indicated that a considerably higher CH{sub 4} flux occurred relative to the CO{sub 2} flux. The daily CH{sub 4} flux calculated with the ratio of DELTACH{sub 4}/DELTACO{sub 2} and terrestrial biosphere CO{sub 2} flux from an ecosystem model showed a maximum in July at the both sites. Although anomalously high flux was observed in June and July 2007 at KRS, only a small flux variation was observed at DEM. The high regional CH{sub 4} flux in June and July 2007 at KRS was reproduced using a process-based ecosystem model, Vegetation Integrative Simulator for Trace gases (VISIT), in response to high water table depth caused by the anomalously high precipitation during the summer of 2007

  15. Assessing Hydrological and Energy Budgets in Amazonia through Regional Downscaling, and Comparisons with Global Reanalysis Products

    Science.gov (United States)

    Nunes, A.; Ivanov, V. Y.

    2014-12-01

    Although current global reanalyses provide reasonably accurate large-scale features of the atmosphere, systematic errors are still found in the hydrological and energy budgets of such products. In the tropics, precipitation is particularly challenging to model, which is also adversely affected by the scarcity of hydrometeorological datasets in the region. With the goal of producing downscaled analyses that are appropriate for a climate assessment at regional scales, a regional spectral model has used a combination of precipitation assimilation with scale-selective bias correction. The latter is similar to the spectral nudging technique, which prevents the departure of the regional model's internal states from the large-scale forcing. The target area in this study is the Amazon region, where large errors are detected in reanalysis precipitation. To generate the downscaled analysis, the regional climate model used NCEP/DOE R2 global reanalysis as the initial and lateral boundary conditions, and assimilated NOAA's Climate Prediction Center (CPC) MORPHed precipitation (CMORPH), available at 0.25-degree resolution, every 3 hours. The regional model's precipitation was successfully brought closer to the observations, in comparison to the NCEP global reanalysis products, as a result of the impact of a precipitation assimilation scheme on cumulus-convection parameterization, and improved boundary forcing achieved through a new version of scale-selective bias correction. Water and energy budget terms were also evaluated against global reanalyses and other datasets.

  16. The relationships between termite mound CH4/CO2 emissions and internal concentration ratios are species specific

    Directory of Open Access Journals (Sweden)

    H. Jamali

    2013-04-01

    Full Text Available We investigated the relative importance of CH4 and CO2 fluxes from soil and termite mounds at four different sites in the tropical savannas of northern Australia near Darwin and assessed different methods to indirectly predict CH4 fluxes based on CO2 fluxes and internal gas concentrations. The annual flux from termite mounds and surrounding soil was dominated by CO2 with large variations among sites. On a carbon dioxide equivalent (CO2-e basis, annual CH4 flux estimates from termite mounds were 5- to 46-fold smaller than the concurrent annual CO2 flux estimates. Differences between annual soil CO2 and soil CH4 (CO2-e fluxes were even greater, soil CO2 fluxes being almost three orders of magnitude greater than soil CH4 (CO2-e fluxes at site. The contribution of CH4 and CO2 emissions from termite mounds to the total CH4 and CO2 emissions from termite mounds and soil in CO2-e was less than 1%. There were significant relationships between mound CH4 flux and mound CO2 flux, enabling the prediction of CH4 flux from measured CO2 flux; however, these relationships were clearly termite species specific. We also observed significant relationships between mound flux and gas concentration inside mound, for both CH4 and CO2, and for all termite species, thereby enabling the prediction of flux from measured mound internal gas concentration. However, these relationships were also termite species specific. Using the relationship between mound internal gas concentration and flux from one species to predict mound fluxes from other termite species (as has been done in the past would result in errors of more than 5-fold for mound CH4 flux and 3-fold for mound CO2 flux. This study highlights that CO2 fluxes from termite mounds are generally more than one order of magnitude greater than CH4 fluxes. There are species-specific relationships between CH4 and CO2 fluxes from a mound, and between the inside mound concentration of a gas and the mound flux emission of the

  17. The relationships between termite mound CH4/CO2 emissions and internal concentration ratios are species specific

    Science.gov (United States)

    Jamali, H.; Livesley, S. J.; Hutley, L. B.; Fest, B.; Arndt, S. K.

    2013-04-01

    We investigated the relative importance of CH4 and CO2 fluxes from soil and termite mounds at four different sites in the tropical savannas of northern Australia near Darwin and assessed different methods to indirectly predict CH4 fluxes based on CO2 fluxes and internal gas concentrations. The annual flux from termite mounds and surrounding soil was dominated by CO2 with large variations among sites. On a carbon dioxide equivalent (CO2-e) basis, annual CH4 flux estimates from termite mounds were 5- to 46-fold smaller than the concurrent annual CO2 flux estimates. Differences between annual soil CO2 and soil CH4 (CO2-e) fluxes were even greater, soil CO2 fluxes being almost three orders of magnitude greater than soil CH4 (CO2-e) fluxes at site. The contribution of CH4 and CO2 emissions from termite mounds to the total CH4 and CO2 emissions from termite mounds and soil in CO2-e was less than 1%. There were significant relationships between mound CH4 flux and mound CO2 flux, enabling the prediction of CH4 flux from measured CO2 flux; however, these relationships were clearly termite species specific. We also observed significant relationships between mound flux and gas concentration inside mound, for both CH4 and CO2, and for all termite species, thereby enabling the prediction of flux from measured mound internal gas concentration. However, these relationships were also termite species specific. Using the relationship between mound internal gas concentration and flux from one species to predict mound fluxes from other termite species (as has been done in the past) would result in errors of more than 5-fold for mound CH4 flux and 3-fold for mound CO2 flux. This study highlights that CO2 fluxes from termite mounds are generally more than one order of magnitude greater than CH4 fluxes. There are species-specific relationships between CH4 and CO2 fluxes from a mound, and between the inside mound concentration of a gas and the mound flux emission of the same gas, but

  18. Activation of CH4 by Th(+) as studied by guided ion beam mass spectrometry and quantum chemistry.

    Science.gov (United States)

    Cox, Richard M; Armentrout, P B; de Jong, Wibe A

    2015-04-06

    The reaction of atomic thorium cations with CH4 (CD4) and the collision-induced dissociation (CID) of ThCH4(+) with Xe are studied using guided ion beam tandem mass spectrometry. In the methane reactions at low energies, ThCH2(+) (ThCD2(+)) is the only product; however, the energy dependence of the cross-section is inconsistent with a barrierless exothermic reaction as previously assumed on the basis of ion cyclotron resonance mass spectrometry results. The dominant product at higher energies is ThH(+) (ThD(+)), with ThCH3(+) (ThCD3(+)) having a similar threshold energy. The latter product subsequently decomposes at still higher energies to ThCH(+) (ThCD(+)). CID of ThCH4(+) yields atomic Th(+) as the exclusive product. The cross-sections of all product ions are modeled to provide 0 K bond dissociation energies (in eV) of D0(Th(+)-H) ≥ 2.25 ± 0.18, D0(Th(+)-CH) = 6.19 ± 0.16, D0(Th(+)-CH2) ≥ 4.54 ± 0.09, D0(Th(+)-CH3) = 2.60 ± 0.30, and D0(Th(+)-CH4) = 0.47 ± 0.05. Quantum chemical calculations at several levels of theory are used to explore the potential energy surfaces for activation of methane by Th(+), and the effects of spin-orbit coupling are carefully considered. When spin-orbit coupling is explicitly considered, a barrier for C-H bond activation that is consistent with the threshold measured for ThCH2(+) formation (0.17 ± 0.02 eV) is found at all levels of theory, whereas this barrier is observed only at the BHLYP and CCSD(T) levels otherwise. The observation that the CID of the ThCH4(+) complex produces Th(+) as the only product with a threshold of 0.47 eV indicates that this species has a Th(+)(CH4) structure, which is also consistent with a barrier for C-H bond activation. This barrier is thought to exist as a result of the mixed ((4)F,(2)D) electronic character of the Th(+) J = (3)/2 ground level combined with extensive spin-orbit effects.

  19. Radiative forcing calculations for CH3Br

    International Nuclear Information System (INIS)

    Grossman, A.S.; Blass, W.E.; Wuebbles, D.J.

    1995-06-01

    Methyl Bromide, CH 3 Br, is the major organobromine species in the lower atmosphere and is a primary source of bromine in the stratosphere. It has a lifetime of 1.3 years. The IR methyl bromide spectra in the atmospheric window region, 7--13μ, was determined using a well tested Coriolis resonance and ell-doubling (and ell-resonance) computational system. A radiative forcing value of 0.00493 W/m 2 /ppbv was obtained for CH 3 Br and is approximately linear in the background abundance. This value is about 2 percent of the forcing of CFC-11 and about 278 times the forcing of C0 2 , on a per molecule basis. The radiative forcing calculation is used to estimate the global warming potential (GWP) of CH 3 Br. The results give GWPs for CH 3 Br of the order of 13 for an integration period of 20 years and 4 for an integration period of 100 years (assuming C0 2 = 1, following IPCC [1994]). While CH 3 Br has a GWP which is approximately 25 percent of the GWP of CH 4 , the current emission rates are too low to cause serious atmospheric greenhouse heating effects at this time

  20. Fluxes of greenhouse gases CH{sub 4}, CO{sub 2} and N{sub 2}O on some peat mining areas in Finland

    Energy Technology Data Exchange (ETDEWEB)

    Nykaenen, H; Martikainen, P J [National Public Health Inst., Kuopio (Finland). Dept. of Biology; Silvola, J; Alm, J [Joensuu Univ. (Finland). Dept. of Biology

    1997-12-31

    The increase in concentration of greenhouse gases (CO{sub 2}, CH{sub 4} and N{sub 2}O) in atmosphere is associated with burning of fossil fuels and also changes in biogeochemistry due to land use activities. Virgin peatlands are globally important stores of carbon and sources of CH4. Peatland drainage changes the processes in carbon and nitrogen cycles responsible for the fluxes of CO{sub 2}, CH{sub 4} and N{sub 2}O. Preparing of peatlands for peat mining greatly change their biogeochemical processes. Effective drainage decreases water table and allows air to penetrate deep into peat profile. Aerobic conditions inhibit activities of anaerobic microbes, including the methanogens, whereas aerobic processes like methane oxidation are stimulated. Destruction of vegetation cover stops the carbon input to peat. In Finland the actual peat mining area is 0.05 x 106 hectares and further 0.03 x 106 hectares have been prepared or are under preparation for peat mining. The current total peatland area in the world used for mining is 0.94 x 106 ha and the area already mined is 1.15 x 106 ha. In this presentation fluxes of greenhouse gases (CH{sub 4}, CO{sub 2} and N{sub 2}O) on some mires under peat mining are reported and compared with those on natural mires and with the emissions from peat combustion. (15 refs.)

  1. Fluxes of greenhouse gases CH{sub 4}, CO{sub 2} and N{sub 2}O on some peat mining areas in Finland

    Energy Technology Data Exchange (ETDEWEB)

    Nykaenen, H.; Martikainen, P.J. [National Public Health Inst., Kuopio (Finland). Dept. of Biology; Silvola, J.; Alm, J. [Joensuu Univ. (Finland). Dept. of Biology

    1996-12-31

    The increase in concentration of greenhouse gases (CO{sub 2}, CH{sub 4} and N{sub 2}O) in atmosphere is associated with burning of fossil fuels and also changes in biogeochemistry due to land use activities. Virgin peatlands are globally important stores of carbon and sources of CH4. Peatland drainage changes the processes in carbon and nitrogen cycles responsible for the fluxes of CO{sub 2}, CH{sub 4} and N{sub 2}O. Preparing of peatlands for peat mining greatly change their biogeochemical processes. Effective drainage decreases water table and allows air to penetrate deep into peat profile. Aerobic conditions inhibit activities of anaerobic microbes, including the methanogens, whereas aerobic processes like methane oxidation are stimulated. Destruction of vegetation cover stops the carbon input to peat. In Finland the actual peat mining area is 0.05 x 106 hectares and further 0.03 x 106 hectares have been prepared or are under preparation for peat mining. The current total peatland area in the world used for mining is 0.94 x 106 ha and the area already mined is 1.15 x 106 ha. In this presentation fluxes of greenhouse gases (CH{sub 4}, CO{sub 2} and N{sub 2}O) on some mires under peat mining are reported and compared with those on natural mires and with the emissions from peat combustion. (15 refs.)

  2. The H2/CH4 ratio during serpentinization cannot reliably identify biological signatures.

    Science.gov (United States)

    Huang, Ruifang; Sun, Weidong; Liu, Jinzhong; Ding, Xing; Peng, Shaobang; Zhan, Wenhuan

    2016-09-26

    Serpentinization potentially contributes to the origin and evolution of life during early history of the Earth. Serpentinization produces molecular hydrogen (H 2 ) that can be utilized by microorganisms to gain metabolic energy. Methane can be formed through reactions between molecular hydrogen and oxidized carbon (e.g., carbon dioxide) or through biotic processes. A simple criterion, the H 2 /CH 4 ratio, has been proposed to differentiate abiotic from biotic methane, with values approximately larger than 40 for abiotic methane and values of serpentinization experiments at 200 °C and 0.3 kbar. However, it is not clear whether the criterion is applicable at a wider range of temperatures. In this study, we performed sixteen experiments at 311-500 °C and 3.0 kbar using natural ground peridotite. Our results demonstrate that the H 2 /CH 4 ratios strongly depend on temperature. At 311 °C and 3.0 kbar, the H 2 /CH 4 ratios ranged from 58 to 2,120, much greater than the critical value of 40. By contrast, at 400-500 °C, the H 2 /CH 4 ratios were much lower, ranging from 0.1 to 8.2. The results of this study suggest that the H 2 /CH 4 ratios cannot reliably discriminate abiotic from biotic methane.

  3. The H2/CH4 ratio during serpentinization cannot reliably identify biological signatures

    Science.gov (United States)

    Huang, Ruifang; Sun, Weidong; Liu, Jinzhong; Ding, Xing; Peng, Shaobang; Zhan, Wenhuan

    2016-09-01

    Serpentinization potentially contributes to the origin and evolution of life during early history of the Earth. Serpentinization produces molecular hydrogen (H2) that can be utilized by microorganisms to gain metabolic energy. Methane can be formed through reactions between molecular hydrogen and oxidized carbon (e.g., carbon dioxide) or through biotic processes. A simple criterion, the H2/CH4 ratio, has been proposed to differentiate abiotic from biotic methane, with values approximately larger than 40 for abiotic methane and values of serpentinization experiments at 200 °C and 0.3 kbar. However, it is not clear whether the criterion is applicable at a wider range of temperatures. In this study, we performed sixteen experiments at 311-500 °C and 3.0 kbar using natural ground peridotite. Our results demonstrate that the H2/CH4 ratios strongly depend on temperature. At 311 °C and 3.0 kbar, the H2/CH4 ratios ranged from 58 to 2,120, much greater than the critical value of 40. By contrast, at 400-500 °C, the H2/CH4 ratios were much lower, ranging from 0.1 to 8.2. The results of this study suggest that the H2/CH4 ratios cannot reliably discriminate abiotic from biotic methane.

  4. Global and regional phosphorus budgets in agricultural systems and their implications for phosphorus-use efficiency

    Science.gov (United States)

    Lun, Fei; Liu, Junguo; Ciais, Philippe; Nesme, Thomas; Chang, Jinfeng; Wang, Rong; Goll, Daniel; Sardans, Jordi; Peñuelas, Josep; Obersteiner, Michael

    2018-01-01

    The application of phosphorus (P) fertilizer to agricultural soils increased by 3.2 % annually from 2002 to 2010. We quantified in detail the P inputs and outputs of cropland and pasture and the P fluxes through human and livestock consumers of agricultural products on global, regional, and national scales from 2002 to 2010. Globally, half of the total P inputs into agricultural systems accumulated in agricultural soils during this period, with the rest lost to bodies of water through complex flows. Global P accumulation in agricultural soil increased from 2002 to 2010 despite decreases in 2008 and 2009, and the P accumulation occurred primarily in cropland. Despite the global increase in soil P, 32 % of the world's cropland and 43 % of the pasture had soil P deficits. Increasing soil P deficits were found for African cropland vs. increasing P accumulation in eastern Asia. European and North American pasture had a soil P deficit because the continuous removal of biomass P by grazing exceeded P inputs. International trade played a significant role in P redistribution among countries through the flows of P in fertilizer and food among countries. Based on country-scale budgets and trends we propose policy options to potentially mitigate regional P imbalances in agricultural soils, particularly by optimizing the use of phosphate fertilizer and the recycling of waste P. The trend of the increasing consumption of livestock products will require more P inputs to the agricultural system, implying a low P-use efficiency and aggravating P-stock scarcity in the future. The global and regional phosphorus budgets and their PUEs in agricultural systems are publicly available at https://doi.pangaea.de/10.1594/PANGAEA.875296.

  5. Phase transitions in solid Kr-CH4 solutions and rotational excitations in phase II

    International Nuclear Information System (INIS)

    Bagatskii, M.I.; Mashchenko, D.A.; Dudkin, V.V.

    2007-01-01

    The heat capacity C p of solid Kr-n CH 4 solutions with the CH 4 concentrations n=0.82, 0.86, 0.90 as well as solutions with n=0.90, 0.95 doped with 0.002 O 2 impurity has been investigated under equilibrium vapor pressure over the internal 1-24 K. The (T,n)-phase diagram was refined and the region of two-phase states was determined for Kr-n CH 4 solid solutions. The contribution of the rotational subsystem, C r ot, to the heat capacity of the solutions has been separated. Analysis of C r ot(T) at T 1 and E 2 between the tunnel levels of the A-, T- and A-, E--nuclear-spin species of CH 4 molecules in the orientationally ordered subsystem, and to determine the effective energy gaps E 1 between lowest levels of the A- and T- species. The relations τ(n) and E 1 (n) stem from changes of the effective potential field caused as the replacement of CH 4 molecules by Kr atoms at sites of the ordered sublattices. The effective gaps E L between a group of tunnel levels of the ground-state liberation state and the nearest group of excited levels of the liberation state of the ordered CH 4 molecules in the solutions with n=0.90 (E L =52 K) and 0.95 (E L =55 K) has been estimated

  6. VAR—ANALYSIS OF GLOBAL FINANCIAL ECONOMIC CRISIS IMPACT ON PUBLIC BUDGET AND UNEMPLOYMENT: EVIDENCE FROM THE ECONOMY OF THE KYRGYZ REPUBLIC

    Directory of Open Access Journals (Sweden)

    Nargiza Bakytovna Alymkulova

    2016-12-01

    Full Text Available The Global financial crisis hit the economy of the Kyrgyz Republic by the third wave of its transmission in the early of 2009. The article examines the impact of the Global financial economic crisis on the public budget and unemployment of the Kyrgyz Republic. We analyzed the transmission of the crisis on the public budget firstly and its effect on unemployment level by using the vector autoregression approach (VAR and quarterly data for 2005–2013 within the framework of IS-LM model for small open economies with floating exchange rate. There is an inverse relationship between the public budget and remittances inflow, liquidity level, volume of deposits, and exchange rate. As a result of the study, the fall in remittances inflows, liquidity level of the banking system, depreciation of the national currency lead to an increase in public revenue. Therefore, the increase in public spending during the crisis period, with the aim of unemployment reduction, may be considered as a crucial policy. The study result allows to policy-makers to exactly know what channels of transmission mechanism transfer the Global crisis on the public budget and its effect on unemployment level of the republic in order to undertake anticrisis macroeconomic policy. The final result of the study indicates that the increase of unemployment level by 1 % requires the increase of public spending by 0.63 %.

  7. Global budget of tropospheric ozone: Evaluating recent model advances with satellite (OMI), aircraft (IAGOS), and ozonesonde observations

    Science.gov (United States)

    Hu, Lu; Jacob, Daniel J.; Liu, Xiong; Zhang, Yi; Zhang, Lin; Kim, Patrick S.; Sulprizio, Melissa P.; Yantosca, Robert M.

    2017-10-01

    The global budget of tropospheric ozone is governed by a complicated ensemble of coupled chemical and dynamical processes. Simulation of tropospheric ozone has been a major focus of the GEOS-Chem chemical transport model (CTM) over the past 20 years, and many developments over the years have affected the model representation of the ozone budget. Here we conduct a comprehensive evaluation of the standard version of GEOS-Chem (v10-01) with ozone observations from ozonesondes, the OMI satellite instrument, and MOZAIC-IAGOS commercial aircraft for 2012-2013. Global validation of the OMI 700-400 hPa data with ozonesondes shows that OMI maintained persistent high quality and no significant drift over the 2006-2013 period. GEOS-Chem shows no significant seasonal or latitudinal bias relative to OMI and strong correlations in all seasons on the 2° × 2.5° horizontal scale (r = 0.88-0.95), improving on previous model versions. The most pronounced model bias revealed by ozonesondes and MOZAIC-IAGOS is at high northern latitudes in winter-spring where the model is 10-20 ppbv too low. This appears to be due to insufficient stratosphere-troposphere exchange (STE). Model updates to lightning NOx, Asian anthropogenic emissions, bromine chemistry, isoprene chemistry, and meteorological fields over the past decade have overall led to gradual increase in the simulated global tropospheric ozone burden and more active ozone production and loss. From simulations with different versions of GEOS meteorological fields we find that tropospheric ozone in GEOS-Chem v10-01 has a global production rate of 4960-5530 Tg a-1, lifetime of 20.9-24.2 days, burden of 345-357 Tg, and STE of 325-492 Tg a-1. Change in the intensity of tropical deep convection between these different meteorological fields is a major factor driving differences in the ozone budget.

  8. Biosphere-Atmosphere Exchange of NOx, CH4, and O3 in Central Amazon

    Science.gov (United States)

    Wiedemann, K. T.; Munger, J. W.; Wofsy, S. C.; Budney, J.; Rizzo, L. V.; Campos, K.; Rocha, H.; Freitas, H.

    2016-12-01

    Oxidation by OH is the dominant pathway for removing important trace gases such as CH4, CO, CH3Br, and HCFCs. The primary source of atmospheric OH is the photolysis of O3 in the presence of water vapor, and NOx are the main precursors of O3 and OH. Thus, in NOx-rich environments that have both high humidity and high solar radiation, OH concentrations are enhanced, and therefore, tropical forests dominate global oxidation of long-lived gases. The Amazon rain forest has a unique combination of vegetation with diverse characteristics, climate, and a dynamic land use, factors that altogether govern the emission and fate of trace-gases and control particle formation and atmospheric chemistry. Understanding the interactions among the mechanisms that govern local precursor emissions will lead to a better description of the local atmospheric chemistry, which have global impacts. As part of the GoAmazon project, an array of complementary measurements was conducted in a research site in central Amazon, southeast of Santarem (PA, Brazil), situated inside the Tapajos National Forest. The site where the measurements were taken is surrounded by intact rain forest in a 6 km radius, and a 45 m closed canopy. In the east side out of this radius (upwind), some settlements are distributed in a stripe along a road, which were cleared for agriculture and are sparsely populated. The 67 m tower was assembled in the site in 2001 for flux measurements (CO2 and H2O), and included CO in order to assess local and regional biomass burning. In mid 2014 additional instrumentation were added, measuring NOx, O3, CH4, and SO2 fluxes and profiles. The SO2 measurements (until early 2015) showed concentrations up to 0.1 ppb during the peak of the dry season, and a small vertical gradient, suggesting the predominance of biogenic sources. Preliminary results show no significant seasonality in the daytime and nighttime O3 vertical profiles. Occasionally, nighttime profiles showed high concentrations for

  9. Correlations among atmospheric CO[sub 2], CH[sub 4] and CO in the Arctic, March 1989

    Energy Technology Data Exchange (ETDEWEB)

    Conway, T.J.; Steele, L.P.; Novelli, P.C. (NOAA Climate Monitoring and Diagnostics Lab., Boulder, CO (United States))

    1993-12-01

    During six aircraft flights conducted as part of the third Arctic Gas and Aerosol Sampling Program (AGASP III, March 1989), 189 air samples were collected throughout the Arctic troposphere and lower stratosphere for analysis of CO[sub 2], CH[sub 4] and CO. The mixing ratios of the three gases varied significantly both horizontally and vertically. Elevated concentrations were found in layers with high anthropogenic aerosol concentrations (Arctic Haze). The mixing ratios of CO[sub 2], CH[sub 4] and CO were highly correlated on all flights. A linear regression of CH[sub 4] vs CO[sub 2] for pooled data from all flights yielded a correlation coefficient (r[sup 2]) of 0.88 and a slope of 13.5 ppb CH[sub 4]/ppm CO[sub 2] (n 186). For CO vs CO[sub 2] a pooled linear regression gave r[sup 2] 0.91 and a slope of 15.8 ppb CO/ppm CO[sub 2] (n 182). Carbon dioxide CH[sub 4] and CO also exhibited mean vertical gradients with slopes of 0.37, -4.4 and -4.2 ppb km[sup -1], respectively. Since the carbon dioxide variations observed in the Arctic atmosphere during winter are due primarily to variations in the emissions and transport of anthropogenic CO[sub 2] from Europe and Asia, the strong correlations that we have found suggest that a similar interpretation applies to CH[sub 4] and CO. Using reliable estimates of CO[sub 2] emissions for the source regions and the measured CH[sub 4]/CO[sub 2] and CO/CO[sub 2] ratios, we estimate a regional European CH[sub 4] source of 47[+-] 6 Tg CH[sub 4] yr[sup -1] that may be associated with fossil fuel combustion. A similar calculation for CO results in an estimated regional CO source of 82[+-]2 Tg CO yr[sup -1]. 31 refs., 7 figs., 4 tabs.

  10. The relationship between termite mound CH4/CO2 emissions and internal concentration ratios are species specific

    Science.gov (United States)

    Jamali, H.; Livesley, S. J.; Hutley, L. B.; Fest, B.; Arndt, S. K.

    2012-12-01

    1. We investigated the relative importance of CH4 and CO2 fluxes from soil and termite mounds at four different sites in the tropical savannas of Northern Australia near Darwin and assessed different methods to indirectly predict CH4 fluxes based on CO2 fluxes and internal gas concentrations. 2. The annual flux from termite mounds and surrounding soil was dominated by CO2 with large variations among sites. On a CO2-e basis, annual CH4 flux estimates from termite mounds were 5- to 46-fold smaller than the concurrent annual CO2 flux estimates. Differences between annual soil CO2 and soil CH4 (CO2-e) fluxes were even greater, soil CO2 fluxes being almost three orders of magnitude greater than soil CH4 (CO2-e) fluxes at site. 3. There were significant relationships between mound CH4 flux and mound CO2 flux, enabling the prediction of CH4 flux from measured CO2 flux, however, these relationships were clearly termite species specific. 4. We also observed significant relationships between mound flux and gas concentration inside mound, for both CH4 and CO2, and for all termite species, thereby enabling the prediction of flux from measured mound internal gas concentration. However, these relationships were also termite species specific. Using the relationship between mound internal gas concentration and flux from one species to predict mound fluxes from other termite species (as has been done in past) would result in errors of more than 5-fold for CH4 and 3-fold for CO2. 5. This study highlights that CO2 fluxes from termite mounds are generally more than one order of magnitude greater than CH4 fluxes. There are species-specific relationships between CH4 and CO2 fluxes from a~mound, and between the inside mound concentration of a gas and the mound flux emission of the same gas, but these relationships vary greatly among termite species. Consequently, there is no generic relationship that will allow for the prediction of CH4 fluxes from termite mounds of all species.

  11. Investigating CH4 production in an oxic plant-soil system -a new approach combining isotopic labelling (13C) and inhibitors

    Science.gov (United States)

    Lenhart, Katharina; Keppler, Frank

    2017-04-01

    Typically, aerated soil are net sinks of atmospheric methane (CH4), being highest in native ecosystems (pristine forests > managed forests > grasslands > crop fields). However, this does not exclude a simultaneous endogenic CH4 production in the plant-soil system, which cannot be detected simply via CH4 flux measurements. Methanogenic archaea producing CH4 under anoxic conditions were thought to be the only biotic source of CH4 in the soil. However, until recently a non-archaeal pathway of CH4 formation is known where CH4 is produced under oxic conditions in plants (Keppler et al. 2006) and fungi (Lenhart et al. 2012). Additionally, abiotic formation of CH4 from soil organic matter was reported (Jugold et al. 2012) and may be ubiquitous in terrestrial ecosystems. The major goal of this project was to determine soil endogenic CH4 sources and to estimate their contribution to the endogenic CH4 production. Especially the effect of plants and fungi on soil CH4 production was investigated. Therefore, a series of experiments was carried out on field fresh soil collected in a grassland and a forest ecosystem under controlled laboratory conditions. By combining selective inhibitors and 13C labelling, CH4 production rates of several CH4 sources were quantified. The major difficulty was to detect the comparatively small flux of CH4 production against the background of the high CH4 consumption rates due to methanotrophic bacteria. Therefore, we supplemented bare soil and soil with vegetation with selective inhibitors and 13C labelled substrates in a closed chamber system. In a first step, CH4 production was determined by the inhibition of CH4 oxidizing bacteria with Difluoromethane (DFM, 2ml l-1). In the following, a 13C labelled substrate (either CO2, Acetate, or Methionine -S-CH3 labelled) was added in combination with a specific inhibitor -either for archaeal methanogenesis (Bromoethanesulfonate), bacteria (Streptomycin), or fungi (Captan, Cycloheximide). Gas samples were

  12. Kinetic isotope effects in the gas phase reactions of OH and Cl with CH3Cl, CD3Cl, and 13CH3Cl

    Directory of Open Access Journals (Sweden)

    A. A. Gola

    2005-01-01

    Full Text Available The kinetic isotope effects in the reactions of CH3Cl, 13CH3Cl and CD3Cl with OH radicals and Cl atoms were studied in relative rate experiments at 298±2 K and 1013±10 mbar. The reactions were carried out in a smog chamber using long path FTIR detection and the spectroscopic data analyzed employing a non-linear least squares spectral fitting method using measured high-resolution infrared spectra as well as absorption cross sections from the HITRAN database. The reaction rates of 13CH3Cl and CD3Cl with OH and Cl were determined relative to CH3Cl as: kOH+CH3ClkOH+CH3Cl/kOH+13CH3Cl}kOH+13CH3Cl=1.059±0.008, kOH+CH3ClkOH+CH3Cl/kOH+CD3ClkOH+CD3Cl=3.9±0.4, kCl+CH3ClkCl+CH3Cl/kCl+13CH3ClkCl+13CH3Cl =1.070±0.010 and kCl+CH3ClkCl+CH3Cl/kCl+CD3ClkCl+CD3Cl=4.91±0.07. The uncertainties given are 2σ from the statistical analyses and do not include possible systematic errors. The unexpectedly large 13C kinetic isotope effect in the OH reaction of CH3Cl has important implications for the global emission inventory of CH3Cl.

  13. Uncertainties in modelling CH4 emissions from northern wetlands in glacial climates: the role of vegetation parameters

    Directory of Open Access Journals (Sweden)

    J. van Huissteden

    2011-10-01

    Full Text Available Marine Isotope Stage 3 (MIS 3 interstadials are marked by a sharp increase in the atmospheric methane (CH4 concentration, as recorded in ice cores. Wetlands are assumed to be the major source of this CH4, although several other hypotheses have been advanced. Modelling of CH4 emissions is crucial to quantify CH4 sources for past climates. Vegetation effects are generally highly generalized in modelling past and present-day CH4 fluxes, but should not be neglected. Plants strongly affect the soil-atmosphere exchange of CH4 and the net primary production of the vegetation supplies organic matter as substrate for methanogens. For modelling past CH4 fluxes from northern wetlands, assumptions on vegetation are highly relevant since paleobotanical data indicate large differences in Last Glacial (LG wetland vegetation composition as compared to modern wetland vegetation. Besides more cold-adapted vegetation, Sphagnum mosses appear to be much less dominant during large parts of the LG than at present, which particularly affects CH4 oxidation and transport. To evaluate the effect of vegetation parameters, we used the PEATLAND-VU wetland CO2/CH4 model to simulate emissions from wetlands in continental Europe during LG and modern climates. We tested the effect of parameters influencing oxidation during plant transport (fox, vegetation net primary production (NPP, parameter symbol Pmax, plant transport rate (Vtransp, maximum rooting depth (Zroot and root exudation rate (fex. Our model results show that modelled CH4 fluxes are sensitive to fox and Zroot in particular. The effects of Pmax, Vtransp and fex are of lesser relevance. Interactions with water table modelling are significant for Vtransp. We conducted experiments with different wetland vegetation types for Marine Isotope Stage 3 (MIS 3 stadial and interstadial climates and the present-day climate, by coupling PEATLAND-VU to high resolution climate model simulations for Europe. Experiments assuming

  14. Uncertainties in modelling CH4 emissions from northern wetlands in glacial climates: the role of vegetation parameters

    Science.gov (United States)

    Berrittella, C.; van Huissteden, J.

    2011-10-01

    Marine Isotope Stage 3 (MIS 3) interstadials are marked by a sharp increase in the atmospheric methane (CH4) concentration, as recorded in ice cores. Wetlands are assumed to be the major source of this CH4, although several other hypotheses have been advanced. Modelling of CH4 emissions is crucial to quantify CH4 sources for past climates. Vegetation effects are generally highly generalized in modelling past and present-day CH4 fluxes, but should not be neglected. Plants strongly affect the soil-atmosphere exchange of CH4 and the net primary production of the vegetation supplies organic matter as substrate for methanogens. For modelling past CH4 fluxes from northern wetlands, assumptions on vegetation are highly relevant since paleobotanical data indicate large differences in Last Glacial (LG) wetland vegetation composition as compared to modern wetland vegetation. Besides more cold-adapted vegetation, Sphagnum mosses appear to be much less dominant during large parts of the LG than at present, which particularly affects CH4 oxidation and transport. To evaluate the effect of vegetation parameters, we used the PEATLAND-VU wetland CO2/CH4 model to simulate emissions from wetlands in continental Europe during LG and modern climates. We tested the effect of parameters influencing oxidation during plant transport (fox), vegetation net primary production (NPP, parameter symbol Pmax), plant transport rate (Vtransp), maximum rooting depth (Zroot) and root exudation rate (fex). Our model results show that modelled CH4 fluxes are sensitive to fox and Zroot in particular. The effects of Pmax, Vtransp and fex are of lesser relevance. Interactions with water table modelling are significant for Vtransp. We conducted experiments with different wetland vegetation types for Marine Isotope Stage 3 (MIS 3) stadial and interstadial climates and the present-day climate, by coupling PEATLAND-VU to high resolution climate model simulations for Europe. Experiments assuming dominance of

  15. Formation of H2 and CH4 by weathering of olivine at temperatures between 30 and 70°C

    Directory of Open Access Journals (Sweden)

    Crill Patrick

    2011-06-01

    Full Text Available Abstract Hydrocarbons such as CH4 are known to be formed through the Fischer-Tropsch or Sabatier type reactions in hydrothermal systems usually at temperatures above 100°C. Weathering of olivine is sometimes suggested to account for abiotic formation of CH4 through its redox lowering and water splitting properties. Knowledge about the CH4 and H2 formation processes at low temperatures is important for the research about the origin and cause of early Earth and Martian CH4 and for CO2 sequestration. We have conducted a series of low temperature, long-term weathering experiments in which we have tested the CH4 and H2 formation potential of forsteritic olivine. The results show low temperature CH4 production that is probably influenced by chromite and magnetite as catalysts. Extensive analyses of a potential CH4 source trapped in the crystal structure of the olivine showed no signs of incorporated CH4. Also, the available sources of organic carbon were not enough to support the total amount of CH4 detected in our experiments. There was also a linear relationship between silica release into solution and the net CH4 accumulation into the incubation bottle headspaces suggesting that CH4 formation under these conditions could be a qualitative indicator of olivine dissolution. It is likely that minerals such as magnetite, chromite and other metal-rich minerals found on the olivine surface catalyze the formation of CH4, because of the low temperature of the system. This may expand the range of environments plausible for abiotic CH4 formation both on Earth and on other terrestrial bodies.

  16. Betaine Phosphate (CH3)3N+CH2COO-.H3PO4 Modification Using D2O

    International Nuclear Information System (INIS)

    Saryati; Ridwan; Deswita; Sugiantoro, Sugik

    2002-01-01

    Betaine fosfate (CH 3 ) 3 N + CH 2 COO - .H 3 PO 4 modification by using D 2 O has been studied. This modification was carried out by slowly evaporation the saturated Betaine phosphat in the D 2 O solution in the dry box at 40 o C, until the dry crystal were formed. Based on the NMR data, can be concluded that the exchange process with D has been runed well and Betaine phosphate-D (CH 3 ) 3 N + CH 2 COO - .H 3 PO 4 has been resulted. From the X-ray diffraction pattern data can be concluded that there are a deference in the crystal structure between Betaine phosphate and Betaine phosphate modification result. From the Differential Scanning Colorimeter (DSC) diagram at the range temperature from 30 o C to 250 o C, can be shown that the Betaine phosphate-H has two endothermic transition phase, at 99 o C with a very little adsorbed calor and at 221.50 o C with -26.75 cal/g. Modified Betaine phosphate has also two endothermic transition phase, at 99.86 o C with -1.94 cal/g and at 171.01 o C with -3.48 cal/g. It can be conclosed that the D atom substitution on the H atoms in Betaine phosphate, to change the crystal and the endothermic fase temperature and energy

  17. Transport Mechanisms for CO2-CH4 Exchange and Safe CO2 Storage in Hydrate-Bearing Sandstone

    Directory of Open Access Journals (Sweden)

    Knut Arne Birkedal

    2015-05-01

    Full Text Available CO2 injection in hydrate-bearing sediments induces methane (CH4 production while benefitting from CO2 storage, as demonstrated in both core and field scale studies. CH4 hydrates have been formed repeatedly in partially water saturated Bentheim sandstones. Magnetic Resonance Imaging (MRI and CH4 consumption from pump logs have been used to verify final CH4 hydrate saturation. Gas Chromatography (GC in combination with a Mass Flow Meter was used to quantify CH4 recovery during CO2 injection. The overall aim has been to study the impact of CO2 in fractured and non-fractured samples to determine the performance of CO2-induced CH4 hydrate production. Previous efforts focused on diffusion-driven exchange from a fracture volume. This approach was limited by gas dilution, where free and produced CH4 reduced the CO2 concentration and subsequent driving force for both diffusion and exchange. This limitation was targeted by performing experiments where CO2 was injected continuously into the spacer volume to maintain a high driving force. To evaluate the effect of diffusion length multi-fractured core samples were used, which demonstrated that length was not the dominating effect on core scale. An additional set of experiments is presented on non-fractured samples, where diffusion-limited transportation was assisted by continuous CO2 injection and CH4 displacement. Loss of permeability was addressed through binary gas (N2/CO2 injection, which regained injectivity and sustained CO2-CH4 exchange.

  18. Regional scale variations of atmospheric CO2 and CH4 from satellite observation

    International Nuclear Information System (INIS)

    Ru, F; Lei, L; Guan, X; Bu, R; Qi, J

    2014-01-01

    To identify the sources, sinks and changes of atmospheric CO 2 and CH 4 , this study investigates the spatio-temporal changes of atmospheric CO 2 and CH 4 concentration on the regional scale by the satellite observations. In this paper, choosing the land region of China as the study area, we investigate the spatio-temporal changes of atmospheric CO 2 and CH 4 concentrations using the data of the CO 2 dry air mixing ratio (XCO 2 ), and the CH 4 dry air mixing ratio (XCH 4 ), retrieved by the Greenhouse Gases Observing Satellite (GOSAT) from Jan. 2010 to Dec. 2012. The results show that (1) both XCO 2 and XCH 4 show higher concentrations in southeastern regions than that in the northwestern, and tend to yearly increasing from 2010 to 2013; (2) XCO 2 shows obvious seasonal change with higher values in the spring than that in summer. The seasonal peak-to-peak amplitude is 8 ppm and the annual growth is about 2 ppm. XCH 4 , however, does not show a seasonal change; (3) With regard to different land-use backgrounds, XCO 2 shows larger concentrations over the areas of urban agglomeration than that over the grasslands and deserts, and XCH 4 shows lower concentrations over deserts than that over the Yangtze River Delta region and Sichuan Basin

  19. Ion imaging study of reaction dynamics in the N{sup +}+ CH{sub 4} system

    Energy Technology Data Exchange (ETDEWEB)

    Pei, Linsen; Farrar, James M. [Department of Chemistry, University of Rochester, Rochester, New York 14627 (United States)

    2012-10-21

    The velocity map ion imaging method is applied to the ion-molecule reactions of N{sup +} with CH{sub 4}. The velocity space images are collected at collision energies of 0.5 and 1.8 eV, providing both product kinetic energy and angular distributions for the reaction products CH{sub 4}{sup +}, CH{sub 3}{sup +}, and HCNH{sup +}. The charge transfer process is energy resonant and occurs by long-range electron transfer that results in minimal deflection of the products. The formation of the most abundant product, CH{sub 3}{sup +}, proceeds by dissociative charge transfer rather than hydride transfer, as reported in earlier publications. The formation of HCNH{sup +} by C-N bond formation appears to proceed by two different routes. The triplet state intermediates CH{sub 3}NH{sup +} and CH{sub 2}NH{sub 2}{sup +} that are formed as N{sup +}({sup 3}P) approaches CH{sub 4} may undergo sequential loss of two hydrogen atoms to form ground state HCNH{sup +} products on a spin-allowed pathway. However, the kinetic energy distributions for formation of HCNH{sup +} extend past the thermochemical limit to form HCNH{sup +}+ 2H, implying that HCNH{sup +} may also be formed in concert with molecular hydrogen, and requiring that intersystem crossing to the singlet manifold must occur in a significant ({approx}25%) fraction of reactive collisions. We also report GAUSSIAN G2 calculations of the energies and structures of important singlet and triplet [CNH{sub 4}{sup +}] complexes that serve as precursors to product formation.

  20. Quantifying the causes of differences in tropospheric OH within global models

    Science.gov (United States)

    Nicely, Julie M.; Salawitch, Ross J.; Canty, Timothy; Anderson, Daniel C.; Arnold, Steve R.; Chipperfield, Martyn P.; Emmons, Louisa K.; Flemming, Johannes; Huijnen, Vincent; Kinnison, Douglas E.; Lamarque, Jean-François; Mao, Jingqiu; Monks, Sarah A.; Steenrod, Stephen D.; Tilmes, Simone; Turquety, Solene

    2017-02-01

    The hydroxyl radical (OH) is the primary daytime oxidant in the troposphere and provides the main loss mechanism for many pollutants and greenhouse gases, including methane (CH4). Global mean tropospheric OH differs by as much as 80% among various global models, for reasons that are not well understood. We use neural networks (NNs), trained using archived output from eight chemical transport models (CTMs) that participated in the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport Model Intercomparison Project (POLMIP), to quantify the factors responsible for differences in tropospheric OH and resulting CH4 lifetime (τCH4) between these models. Annual average τCH4, for loss by OH only, ranges from 8.0 to 11.6 years for the eight POLMIP CTMs. The factors driving these differences were quantified by inputting 3-D chemical fields from one CTM into the trained NN of another CTM. Across all CTMs, the largest mean differences in τCH4 (ΔτCH4) result from variations in chemical mechanisms (ΔτCH4 = 0.46 years), the photolysis frequency (J) of O3 → O(1D) (0.31 years), local O3 (0.30 years), and CO (0.23 years). The ΔτCH4 due to CTM differences in NOx (NO + NO2) is relatively low (0.17 years), although large regional variation in OH between the CTMs is attributed to NOx. Differences in isoprene and J(NO2) have negligible overall effect on globally averaged tropospheric OH, although the extent of OH variations due to each factor depends on the model being examined. This study demonstrates that NNs can serve as a useful tool for quantifying why tropospheric OH varies between global models, provided that essential chemical fields are archived.

  1. Molecular Level Investigation of CH 4 and CO 2 Adsorption in Hydrated Calcium–Montmorillonite

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Mal-Soon [Physical; McGrail, B. Peter [Physical; Rousseau, Roger [Physical; Glezakou, Vassiliki-Alexandra [Physical

    2017-11-17

    We have studied the mechanism of intercalation and methane adsorption from a H2O/CH4/CO2 mixture on a prototypical shale component, Ca-montmorillonite. We employed ab initio molecular dynamics simulations at 323 K and 90 bar to obtain molecular level information of adsorption energetics, speciation, and structural and thermodynamic properties. Interaction of CH4 with surface Lewis acidic sites (Ca2+, surface OH) results in large induced dipoles (~1 D) that lead to relatively strong adsorption energies that level off once a full CH4 layer is formed. Intercalated CH4, also exhibits induced dipoles at low hydration levels, when the interaction with Ca2+ cations are less hindered. CO2 displaces CH4 in the coordination sphere of the cations (in the interlayer) or in the surface, thereby driving CH4 extraction. Our simulations indicate that there is a Goldilocks pressure range (~60-100 bar) where scCO2 –facilitated CH4 extraction will be maximized.

  2. Accurate quantum calculations of the reaction rates for H/D+ CH4

    NARCIS (Netherlands)

    Harrevelt, R. van; Nyman, G.; Manthe, U.

    2007-01-01

    In previous work [T. Wu, H. J. Werner, and U. Manthe, Science 306, 2227 (2004)], accurate quantum reaction rate calculations of the rate constant for the H+CH4 -> CH3+H-2 reaction have been presented. Both the electronic structure calculations and the nuclear dynamics calculations are converged with

  3. Atmospheric chemistry of 4 : 2 fluorotelomer alcohol (CF3(CF2)(3)CH2CH2OH): Products and mechanism of Cl atom initiated oxidation

    DEFF Research Database (Denmark)

    Hurley, MD; Ball, JC; Wallington, TJ

    2004-01-01

    Smog chamber/FTIR techniques were used to study the products and mechanism of the Cl atom initiated oxidation of 4:2 fluorotelomer alcohol (CF3(CF2)(3)CH2CH2OH) in 700 Torr of N-2/O-2 diluent at 296 K. CF3(CF2)(3)CH2CHO is the sole primary oxidation product. CF3(CF2)(3)CHO, CF3(CF2)(3)CH2COOH...... respectively. Using relative rate techniques, a value of k(Cl + CF3(CF2)(3)CH2CHO) = (1.84 +/- 0.30) x 10(-11) cm(3) molecule(-1) s(-1) was determined. The yield of the perfluorinated acid, CF3(CF2)(3)COOH, from the 4:2 fluorotelomer alcohol increased with the diluent gas oxygen concentration......, and CF3(CF2)(3)CH2C(O)OOH are secondary oxidation products. Further irradiation results in the formation of CF3(CF2)(3)COOH, COF2, and CF3OH. CF3(CF2)(3)CHO, CF3(CF2)(3)CH2COOH, and CF3(CF2)(3)CH2C(O)OOH are formed from CF3(CF2)(3)CH2CHO oxidation in yields of 46 27 and less than or equal to 27...

  4. CO2 and CH4 in sea ice from a subarctic fjord under influence of riverine input

    DEFF Research Database (Denmark)

    Crabeck, O.; Delille, B.; Thomas, D. N.

    2014-01-01

    We present CH4 concentration [CH4] and the partial pressure of CO2 (pCO2) in bulk sea ice from subarctic, land-fast sea ice in the Kapisillit fjord, Greenland. The bulk ice [CH4] ranged from 1.8 to 12.1 nmol L−1, which corresponds to a partial pressure range of 3 to 28 ppmv. This is markedly higher......-saturated compared to the atmosphere (390 ppmv). Our study adds to the few existing studies of CH4 and CO2 in sea ice and concludes that sub-arctic sea can be a sink for atmospheric CO2, while being a net source of CH4. Processes related to the freezing and melting of sea ice represents large unknowns...... to the exchange of CO2 but also CH4. It is therefore imperative to assess the consequences of these unknowns through further field campaigns and targeted research under other sea ice conditions at both hemispheres....

  5. Surface study of platinum decorated graphene towards adsorption of NH{sub 3} and CH{sub 4}

    Energy Technology Data Exchange (ETDEWEB)

    Rad, Ali Shokuhi, E-mail: a.shokuhi@gmail.com [Department of Chemical Engineering, Qaemshahr Branch, Islamic Azad University, Qaemshahr (Iran, Islamic Republic of); Pazoki, Hossein; Mohseni, Soheil [Department of Chemical Engineering, Qaemshahr Branch, Islamic Azad University, Qaemshahr (Iran, Islamic Republic of); Zareyee, Daryoush [Department of Chemistry, Qaemshahr Branch, Islamic Azad University, Qaemshahr (Iran, Islamic Republic of); Peyravi, Majid [Faculty of Chemical Engineering, Babol University of Technology, Babol (Iran, Islamic Republic of)

    2016-10-01

    To distinguish the potential of graphene sensors, there is a need to recognize the interaction between graphene sheet and adsorbing molecules. We used density functional theory (DFT) calculations to study the properties of pristine as well as Pt-decorated graphene sheet upon adsorption of NH{sub 3} and CH{sub 4} on its surface to exploit its potential to be as gas sensors for them. We found much higher adsorption, higher charge transfer, lower intermolecular distance, and higher orbital hybridizing upon adsorption of NH{sub 3} and CH{sub 4} gas molecules on Pt-decorated graphene compared to pristine graphene. Also our calculations reveal that the adsorption energies on Pt-decorated graphene sheet are in order of NH{sub 3} >CH{sub 4} which could be corresponded to the order of their sensitivity on this modified surface. We used orbital analysis including density of states as well as frontier molecular orbital study for all analyte-surface systems to more understanding the kind of interaction (physisorption or chemisorption). Consequently, the Pt-decorated graphene can transform the existence of NH{sub 3} and CH{sub 4} molecules into electrical signal and it may be potentially used as an ideal sensor for detection of NH{sub 3} and CH{sub 4} in ambient situation. - Highlights: • Pt-decorated graphene was investigated as an adsorbent for NH{sub 3} and CH{sub 4}. • Much higher adsorption of NH{sub 3} and CH{sub 4} on Pt-decorated graphene than pristine graphene. • Higher adsorption of NH{sub 3} compared to CH{sub 4} on Pt-decorated graphene. • Pt influences the electronic structure of graphene.

  6. Global and regional phosphorus budgets in agricultural systems and their implications for phosphorus-use efficiency

    Directory of Open Access Journals (Sweden)

    F. Lun

    2018-01-01

    Full Text Available The application of phosphorus (P fertilizer to agricultural soils increased by 3.2 % annually from 2002 to 2010. We quantified in detail the P inputs and outputs of cropland and pasture and the P fluxes through human and livestock consumers of agricultural products on global, regional, and national scales from 2002 to 2010. Globally, half of the total P inputs into agricultural systems accumulated in agricultural soils during this period, with the rest lost to bodies of water through complex flows. Global P accumulation in agricultural soil increased from 2002 to 2010 despite decreases in 2008 and 2009, and the P accumulation occurred primarily in cropland. Despite the global increase in soil P, 32 % of the world's cropland and 43 % of the pasture had soil P deficits. Increasing soil P deficits were found for African cropland vs. increasing P accumulation in eastern Asia. European and North American pasture had a soil P deficit because the continuous removal of biomass P by grazing exceeded P inputs. International trade played a significant role in P redistribution among countries through the flows of P in fertilizer and food among countries. Based on country-scale budgets and trends we propose policy options to potentially mitigate regional P imbalances in agricultural soils, particularly by optimizing the use of phosphate fertilizer and the recycling of waste P. The trend of the increasing consumption of livestock products will require more P inputs to the agricultural system, implying a low P-use efficiency and aggravating P-stock scarcity in the future. The global and regional phosphorus budgets and their PUEs in agricultural systems are publicly available at https://doi.pangaea.de/10.1594/PANGAEA.875296.

  7. From California dreaming to California data: Challenging historic models for landfill CH4 emissions

    Science.gov (United States)

    Improved quantification of diverse CH4 sources at the urban scale is needed to guide local greenhouse gas (GHG) mitigation strategies in the Anthropocene. Herein, we focus on landfill CH4 emissions in California, challenging the current IPCC methodology which focuses on a climate dependency for land...

  8. Soil CO2 CH4 and N2O fluxes from an afforested lowland raised peatbog in Scotland: implications for drainage and restoration

    Directory of Open Access Journals (Sweden)

    J. I. L. Morison

    2013-02-01

    Full Text Available The effect of tree (lodgepole pine planting with and without intensive drainage on soil greenhouse gas (GHG fluxes was assessed after 45 yr at a raised peatbog in West Flanders Moss, central Scotland. Fluxes of CO2 CH4 and N2O from the soil were monitored over a 2-yr period every 2 to 4 weeks using the static opaque chamber method in a randomised experimental block trial with the following treatments: drained and planted (DP, undrained and planted (uDP, undrained and unplanted (uDuP and for reference also from an adjoining near-pristine area of bog at East Flanders Moss (n-pris. There was a strong seasonal pattern in both CO2 and CH4 effluxes which were significantly higher in late spring and summer months because of warmer temperatures. Effluxes of N2O were low and no significant differences were observed between the treatments. Annual CH4 emissions increased with the proximity of the water table to the soil surface across treatments in the order: DP 4 m−2 yr−1, respectively. For CO2, effluxes increased in the order uDP 2 m−2 yr−1, respectively. CO2 effluxes dominated the total net GHG emission, calculated using the global warming potential (GWP of the three GHGs for each treatment (76–98%, and only in the n-pris site was CH4 a substantial contribution (23%. Based on soil effluxes only, the near pristine (n-pris peatbog had 43% higher total net GHG emission compared with the DP treatment because of high CH4 effluxes and the DP treatment had 33% higher total net emission compared with the uDP because drainage increased CO2 effluxes. Restoration is likely to increase CH4 emissions, but reduce CO2 effluxes. Our study suggests that if estimates of CO2 uptake by vegetation from similar peatbog sites were included, the total net GHG emission of restored peatbog would still be higher than that of the peatbog with trees.

  9. Factors affecting variation in CH4 emission from paddy soils grown with different rice cultivars: A pot experiment

    Science.gov (United States)

    Watanabe, Akira; Kimura, Makoto

    1998-08-01

    The growth of rice plants greatly influences CH4 emission from paddy fields through the supply of organic materials such as root exudates and sloughed tissues, the release of oxygen to the root environment, and the transfer of CH4 from the rhizosphere into the atmosphere through the aerenchyma. In the present pot experiments, the effects of the release of water-soluble organic substances from roots, the air space in roots, and the CH4-oxidizing capacity of roots on intervarietal differences in CH4 emission were examined using three Japonica type cultivars (Norin 25, Nipponbare, and Aoinokaze), which differ in morphological properties. The CH4 emission rates varied among the cultivars from mid-July (tillering stage) to the beginning of September (heading stage).Total CH4 emission throughout the rice growth period was largest for Norin 25, followed by Nipponbare, and Aoinokaze. In August, the rate of release of water-soluble organic substances from roots was largest for Norin 25. The air space in roots was also largest in Norin 25 and least in Aoinokaze. The stable carbon isotopic ratios (δ13C) of CH4 in roots were 3-10‰ higher than those in soil in August. The difference in δ13C values of CH4 between roots and soil was largest for Aoinokaze and smallest for Norin 25. In September, the difference in δ13C values of CH4 between roots and soil became small (2-3‰). These findings suggest that the proportion of CH4 oxidation in the rhizosphere was largest in the cultivar which emitted the smallest amount of CH4 and that the proportion became smaller with continued plant growth.

  10. Studies on the adsorption behavior of CO2-CH4 mixtures using activated carbon

    Directory of Open Access Journals (Sweden)

    R. B. Rios

    2013-12-01

    Full Text Available Separation of CO2 from CO2-CH4 mixtures is an important issue in natural gas and biogas purification. The design of such separation processes depends on the knowledge of the behavior of multicomponent adsorption, particularly that of CO2-CH4 mixtures. In this study, we present a series of experimental binary equilibrium isotherms for CO2-CH4 mixtures on an activated carbon at 293 K and compare them with predicted values using the Ideal Adsorption Solution Theory (IAST and the Extended Langmuir (EL model. Even at concentrations of ca. 20% for all binary isotherms, CO2 already presents higher adsorbed amounts with respect to CH4. A maximum selectivity of around 8.7 was observed for a nearly equimolar mixture at 0.1 MPa. The IAST in conjunction with the Toth equation showed slightly better results than IAST using the Langmuir equation and both showed better results than the EL model.

  11. Intermolecular Force Field Parameters Optimization for Computer Simulations of CH4 in ZIF-8

    Directory of Open Access Journals (Sweden)

    Phannika Kanthima

    2016-01-01

    Full Text Available The differential evolution (DE algorithm is applied for obtaining the optimized intermolecular interaction parameters between CH4 and 2-methylimidazolate ([C4N2H5]− using quantum binding energies of CH4-[C4N2H5]− complexes. The initial parameters and their upper/lower bounds are obtained from the general AMBER force field. The DE optimized and the AMBER parameters are then used in the molecular dynamics (MD simulations of CH4 molecules in the frameworks of ZIF-8. The results show that the DE parameters are better for representing the quantum interaction energies than the AMBER parameters. The dynamical and structural behaviors obtained from MD simulations with both sets of parameters are also of notable differences.

  12. Quantifying Gas Flaring CH4 Consumption Using VIIRS

    Directory of Open Access Journals (Sweden)

    Xiaodong Zhang

    2015-07-01

    Full Text Available A method was developed to estimate the consumption of CH4 and the release of CO2 by gas flaring using VIIRS nighttime data. The results agreed with the field data collected at six stations in Bakken field, North Dakota, USA, within ±50%, as measured by mean relative errors and with a correlation coefficient of 0.75. This improved over the NOAA NightFire estimates, likely due to: (1 more stringent data selection using only the middle portion of cloud-free VIIRS nighttime imagery; (2 the use of a lower heating rate, which is more suitable for the field condition; and (3 more accurate efficiency factors in calculating completeness in combustion and conversion of total reaction energy into radiant energy that can be sensed by a satellite sensor. While using atmospherically-corrected data can further improve the estimate of CH4 consumption by ~10%, the major uncertainty remains as being the form factor of the flares, particularly the ratio of total surface area of a flare to the cross-section area that was seen by a satellite sensor.

  13. EMISSION ASSESSMENT AT THE ŠTĚPÁNOVICE MUNICIPAL SOLID WASTE LANDFILL FOCUSING ON CH4 EMISSIONS

    Directory of Open Access Journals (Sweden)

    Dana Adamcová

    2016-07-01

    Full Text Available The study was conducted to measure the emission from landfill in the years 2005–2011. The results are used to diagnose the emissions of CH4. The mean value of CH4 in vol. % in the collection wells ranged from 0 to 2.14 vol. % the mean concentration of CH4 in mg/m3 ranged from 0 to 25 251 mg/m3 the average concentration of CH4 in mg/Nm3 at the measuring and control points ranged from 2.2 to 24.1 mg/Nm3. CH4 emissions from the landfill do not exceed the reporting thresholds the landfill does not meet conditions for being included in the Integrated Register of Pollutants.

  14. Subterranean karst environments as a global sink for atmospheric methane

    Science.gov (United States)

    Webster, Kevin D.; Drobniak, Agnieszka; Etiope, Giuseppe; Mastalerz, Maria; Sauer, Peter E.; Schimmelmann, Arndt

    2018-03-01

    The air in subterranean karst cavities is often depleted in methane (CH4) relative to the atmosphere. Karst is considered a potential sink for the atmospheric greenhouse gas CH4 because its subsurface drainage networks and solution-enlarged fractures facilitate atmospheric exchange. Karst landscapes cover about 14% of earth's continental surface, but observations of CH4 concentrations in cave air are limited to localized studies in Gibraltar, Spain, Indiana (USA), Vietnam, Australia, and by incomplete isotopic data. To test if karst is acting as a global CH4 sink, we measured the CH4 concentrations, δ13CCH4, and δ2HCH4 values of cave air from 33 caves in the USA and three caves in New Zealand. We also measured CO2 concentrations, δ13CCO2, and radon (Rn) concentrations to support CH4 data interpretation by assessing cave air residence times and mixing processes. Among these caves, 35 exhibited subatmospheric CH4 concentrations in at least one location compared to their local atmospheric backgrounds. CH4 concentrations, δ13CCH4, and δ2HCH4 values suggest that microbial methanotrophy within caves is the primary CH4 consumption mechanism. Only 5 locations from 3 caves showed elevated CH4 concentrations compared to the atmospheric background and could be ascribed to local CH4 sources from sewage and outgassing swamp water. Several associated δ13CCH4 and δ2HCH4 values point to carbonate reduction and acetate fermentation as biochemical pathways of limited methanogenesis in karst environments and suggest that these pathways occur in the environment over large spatial scales. Our data show that karst environments function as a global CH4 sink.

  15. Sensitizing effects of NOx on CH4 oxidation at high pressure

    DEFF Research Database (Denmark)

    Rasmussen, Christian Lund; Rasmussen, Anja Egede; Glarborg, Peter

    2008-01-01

    The CH4/O2/NOx system is investigated in a laboratory-scale high pressure laminar flow reactor with the purpose of elucidating the sensitizing effects of NOx on CH4 oxidation at high pressures and medium temperatures. Experiments are conducted at 100, 50, and 20 bar, 600-900 K, and stoichiometric...... ratios ranging from highly reducing to oxidizing conditions. The experimental results are interpreted in terms of a detailed kinetic model drawn from previous work of the authors, including an updated reaction subset for the direct interactions of NOx and C1-2 hydrocarbon species relevant...

  16. Super Rice Cropping Will Enhance Rice Yield and Reduce CH4 Emission: A Case Study in Nanjing, China

    Directory of Open Access Journals (Sweden)

    Yu JIANG

    2013-11-01

    Full Text Available A pot experiment was performed to learn the differences in plant productivity and CH4 emission between two rice cultivars, super rice variety Ningjing 1 and traditional variety Zhendao 11, which were currently commercially applied in Nanjing, China. Similar seasonal changes of CH4 emission fluxes and soil solution CH4 contents were found between the tested cultivars. Although there was no significant difference in plant biomass production between the cultivars, the grain yield of Ningjing 1 was significantly higher by 35.0% (P < 0.05 than that of Zhendao 11, whereas the total CH4 emission from Ningjing 1 was 35.2% lower (P < 0.05. The main difference in the amounts of CH4 emission between the cultivars occurred in the period from the tillering stage to the heading stage. The biomass-scaled and yield-scaled CH4 emissions were respectively 3.8 and 5.2 mg/g for Ningjing 1, significantly lower than those for Zhendao 11 (7.4 and 12.8 mg/g, respectively. According to the relationships between the plant growth characteristics and the CH4 emission, a stronger root system contributed mainly to the lower CH4 emission of Ningjing 1, as compared with Zhendao 11. Our results demonstrated that super rice has advantages not only in grain productivity but also in CH4 emission mitigation. Further expansion of super rice cropping will enhance rice yield and reduce greenhouse gas emission in China.

  17. Simulations and experimental investigations of the competitive adsorption of CH4 and CO2 on low-rank coal vitrinite.

    Science.gov (United States)

    Yu, Song; Bo, Jiang; Jiahong, Li

    2017-09-16

    The mechanism for the competitive adsorption of CH 4 and CO 2 on coal vitrinite (DV-8, maximum vitrinite reflectance R o,max  = 0.58%) was revealed through simulation and experimental methods. A saturated state was reached after absorbing 17 CH 4 or 22 CO 2 molecules per DV-8 molecule. The functional groups (FGs) on the surface of the vitrinite can be ranked in order of decreasing CH 4 and CO 2 adsorption ability as follows: [-CH 3 ] > [-C=O] > [-C-O-C-] > [-COOH] and [-C-O-C-] > [-C=O] > [-CH 3 ] > [-COOH]. CH 4 and CO 2 distributed as aggregations and they were both adsorbed at the same sites on vitrinite, indicating that CO 2 can replace CH 4 by occupying the main adsorption sites for CH 4 -vitrinite. High temperatures are not conducive to the adsorption of CH 4 and CO 2 on vitrinite. According to the results of density functional theory (DFT) and grand canonical Monte Carlo (GCMC) calculations, vitrinite has a higher adsorption capacity for CO 2 than for CH 4 , regardless of whether a single-component or binary adsorbate is considered. The equivalent adsorption heat (EAH) of CO 2 -vitrinite (23.02-23.17) is higher than that of CH 4 -vitrinite (9.04-9.40 kJ/mol). The EAH of CO 2 -vitrinite decreases more rapidly with increasing temperature than the EAH of CH 4 -vitrinite does, indicating in turn that the CO 2 -vitrinite bond weakens more quickly with increasing temperature than the CH 4 -vitrinite bond does. Simulation data were found to be in good accord with the corresponding experimental results.

  18. Early Mars serpentinization-derived CH4 reservoirs, H2 induced warming and paleopressure evolution

    Science.gov (United States)

    Lasue, J.; Chassefiere, E.; Langlais, B.; Quesnel, Y.

    2016-12-01

    CH4 has been observed on Mars both by remote sensing and in situ during the past 15 years. Early Mars serpentinization is one possible abiotic mechanism that could not only produce methane, but also explain the observed Martian remanent magnetic field. Assuming a cold early Mars, a cryosphere could trap such CH4 as clathrates in stable form at depth. We recently estimated the maximum storage capacity of such clathrate layer to be about 2x1019 to 2x1020 moles of methane. Such reservoirs may be stable or unstable, depending on many factors that are poorly constrained: major and sudden geological events such as the Tharsis bulge formation, the Hellas impact or the martian polar wander, could have destabilized the clathrates early in the history of the planet and released large quantities of gas in the atmosphere. Here we estimate the associated amounts of serpentinization-derived CH4 stored in the cryosphere that have been released to the atmosphere at the end of the Noachian and the beginning of the Hesperian. Due to rapid clathrate dissociation and photochemical conversion of CH4 to H2, these episodes of massive CH4 release may have resulted in transient H2-rich atmospheres, at typical levels of 10-20% in a background 1-2 bar CO2 atmosphere. We propose that the early Mars cryosphere had a sufficient CH4 storage capacity to have maintained H2-rich transient atmospheres during a total time period up to several Myr or tens of Myr, having potentially contributed - by collision-induced heating effect of atmospheric H2 - to the formation of valley networks during the late Noachian and early Hesperian.

  19. Evaluation of the reactive nitrogen budget of the remote atmosphere in global models using airborne measurements

    Science.gov (United States)

    Murray, L. T.; Strode, S. A.; Fiore, A. M.; Lamarque, J. F.; Prather, M. J.; Thompson, C. R.; Peischl, J.; Ryerson, T. B.; Allen, H.; Blake, D. R.; Crounse, J. D.; Brune, W. H.; Elkins, J. W.; Hall, S. R.; Hintsa, E. J.; Huey, L. G.; Kim, M. J.; Moore, F. L.; Ullmann, K.; Wennberg, P. O.; Wofsy, S. C.

    2017-12-01

    Nitrogen oxides (NOx ≡ NO + NO2) in the background atmosphere are critical precursors for the formation of tropospheric ozone and OH, thereby exerting strong influence on surface air quality, reactive greenhouse gases, and ecosystem health. The impact of NOx on atmospheric composition and climate is sensitive to the relative partitioning of reactive nitrogen between NOx and longer-lived reservoir species of the total reactive nitrogen family (NOy) such as HNO3, HNO4, PAN and organic nitrates (RONO2). Unfortunately, global chemistry-climate models (CCMs) and chemistry-transport models (CTMs) have historically disagreed in their reactive nitrogen budgets outside of polluted continental regions, and we have lacked in situ observations with which to evaluate them. Here, we compare and evaluate the NOy budget of six global models (GEOS-Chem CTM, GFDL AM3 CCM, GISS E2.1 CCM, GMI CTM, NCAR CAM CCM, and UCI CTM) using new observations of total reactive nitrogen and its member species from the NASA Atmospheric Tomography (ATom) mission. ATom has now completed two of its four planned deployments sampling the remote Pacific and Atlantic basins of both hemispheres with a comprehensive suite of measurements for constraining reactive photochemistry. All six models have simulated conditions climatologically similar to the deployments. The GMI and GEOS-Chem CTMs have in addition performed hindcast simulations using the MERRA-2 reanalysis, and have been sampled along the flight tracks. We evaluate the performance of the models relative to the observations, and identify factors contributing to their disparate behavior using known differences in model oxidation mechanisms, heterogeneous loss pathways, lightning and surface emissions, and physical loss processes.

  20. Influence of atmospheric stability and transport on CH{sub 4} concentrations in northern Spain

    Energy Technology Data Exchange (ETDEWEB)

    García, M. Ángeles, E-mail: magperez@fa1.uva.es; Sánchez, M. Luisa; Pérez, Isidro A.; Ozores, Marta I.; Pardo, Nuria

    2016-04-15

    Continuous methane (CH{sub 4}) concentrations were measured in Northern Spain over two years (2011–2012) by multi-point sampling at 1.8, 3.7 and 8.3 m using a Picarro analyser. The technique is based on cavity ring-down spectroscopy. The contrast in mean concentrations was about 1.2 ppb, with 95th percentiles differing by 2.2 ppb and mean minimum concentrations proving similar. Temporal variations of CH{sub 4} were also analysed, with a similar seasonal variability being found for the three heights. The highest CH{sub 4} concentrations were obtained in late autumn and winter and the lowest in summer, yielding a range of 52 ppb. This variation may depend on the active photochemical reaction with OH radical during a period of intense solar radiation and changes in soil conditions together with variations in emissions. Peak concentration levels were recorded at night-time, between 5:00–7:00 GMT, with mean values ranging between 1920 and 1923 ppb. The lowest value, around 1884 ppb, was obtained at 16:00 GMT. This diurnal variation was mainly related to vertical mixing and photochemistry. Therefore, CH{sub 4} concentrations were also examined using the bulk Richardson number (R{sub B}) as a stability indicator. Four groups were distinguished: unstable cases, situations with pure shear flow, transitional stages and drainage flows. The highest contrast in mean CH{sub 4} concentrations between lower and upper heights was obtained for the transition and drainage cases, mainly associated to high concentrations from nearby sources. The impact of long range transport was analysed by means of 3-day isobaric backward air mass trajectories, which were calculated taking into account origins from Europe, Africa, the Atlantic Ocean and Local conditions. Assessment of the results showed the influence of S and SE wind sectors, especially with Local conditions associated with low winds. Finally, an estimation of the background CH{sub 4} concentration in the study period provided an

  1. Comparison of Landfill Methane Oxidation Measured Using Stable Isotope Analysis and CO2/CH4 Fluxes Measured by the Eddy Covariance Method

    Science.gov (United States)

    Xu, L.; Chanton, J.; McDermitt, D. K.; Li, J.; Green, R. B.

    2015-12-01

    Methane plays a critical role in the radiation balance and chemistry of the atmosphere. Globally, landfill methane emission contributes about 10-19% of the anthropogenic methane burden into the atmosphere. In the United States, 18% of annual anthropogenic methane emissions come from landfills, which represent the third largest source of anthropogenic methane emissions, behind enteric fermentation and natural gas and oil production. One uncertainty in estimating landfill methane emissions is the fraction of methane oxidized when methane produced under anaerobic conditions passes through the cover soil. We developed a simple stoichiometric model to estimate methane oxidation fraction when the anaerobic CO2 / CH4 production ratio is known, or can be estimated. The model predicts a linear relationship between CO2 emission rates and CH4 emission rates, where the slope depends on anaerobic CO2 / CH4 production ratio and the fraction of methane oxidized, and the intercept depends on non-methane-dependent oxidation processes. The model was tested using carbon dioxide emission rates (fluxes) and methane emission rates (fluxes) measured using the eddy covariance method over a one year period at the Turkey Run landfill in Georgia, USA. The CO2 / CH4 production ratio was estimated by measuring CO2 and CH4 concentrations in air sampled under anaerobic conditions deep inside the landfill. We also used a mass balance approach to independently estimate fractional oxidation based on stable isotope measurements (δ13C of methane) of gas samples taken from deep inside the landfill and just above the landfill surface. Results from the two independent methods agree well. The model will be described and methane oxidation will be discussed in relation to wind direction, location at the landfill, and age of the deposited refuse.

  2. Intermolecular interactions involving C-H bonds, 3, Structure and energetics of the interaction between CH{sub 4} and CN{sup {minus}}

    Energy Technology Data Exchange (ETDEWEB)

    Novoa, J.J.; Whangbo, Myung-Hwan [North Carolina State Univ., Raleigh, NC (United States). Dept. of Chemistry; Williams, J.M. [Argonne National Lab., IL (United States)

    1991-12-31

    On the basis of SCF and single reference MP2 calculations, the full potential energy surface of the interaction between CH{sub 4} and CN{sup {minus}} was studied using extended basis sets of up to near Hartree-Fock limit quality. Colinear arrangements C-N{sup {minus}}{hor_ellipsis}H-CH{sub 3} and N-C{sup {minus}}{hor_ellipsis}H-CH{sub 3} are found to be the only two energy minima. The binding energies of these two structures are calculated to be 2.5 and 2.1 kcal/mol, respectively, at the MP2 level. The full vibrational analyses of two structures show a red shift of about 30 cm{sup {minus}1} for the v{sub s} C-H stretching.

  3. Management effects on net ecosystem carbon and GHG budgets at European crop sites

    DEFF Research Database (Denmark)

    Ceschia, Eric; Bêziat, P; Dejoux, J.F.

    2010-01-01

    The greenhouse gas budgets of 15 European crop sites covering a large climatic gradient and corresponding to 41 site-years were estimated. The sites included a wide range of management practices (organic and/or mineral fertilisation, tillage or ploughing, with or without straw removal....... The variability of the different terms and their relative contributions to the net ecosystem carbon budget (NECB) were analysed for all site-years, and the effect of management on NECB was assessed. To account for greenhouse gas (GHG) fluxes that were not directly measured on site, we estimated the emissions...... caused by field operations (EFO) for each site using emission factors from the literature. The EFO were added to the NECB to calculate the total GHG budget (GHGB) for a range of cropping systems and management regimes. N2O emissions were calculated following the IPCC (2007) guidelines, and CH4 emissions...

  4. Optical properties of bias-induced CH sub 4 -H sub 2 plasma for diamond film deposition

    CERN Document Server

    Zhu, X D; Zhou, H Y; Wen, X H; Li, D

    2002-01-01

    Methane (CH sub 4) and hydrogen (H sub 2) reactive gas mixture has been in situ investigated in a hot filament diamond chemical vapor deposition reactor with a negatively variable biasing voltage applied to the hot filament with respect to the substrate using infrared absorption spectroscopy and optical emission spectroscopy. It is found that CH sub 4 converts increasingly to C sub 2 H sub 2 upon raising the filament temperature in a pure thermal activation state, no optical emission of species is observed. Upon bias application, both CH sub 4 and C sub 2 H sub 2 in infrared (IR) absorption intensity decrease with increasing bias current, even the IR absorption intensity of C sub 2 H sub 2 decreases more rapidly than that of CH sub 4. Meanwhile, the clear emission lines indexed to H, CH, and CH sup + appear in the optical emission spectrum obtained, showing that a large amount of excited radicals are produced in the gas phase after applying bias. It is believed that the further generation of activated radical...

  5. Effects of shifting growth stage and regulating temperature on seasonal variation of CH4 emission from rice

    Science.gov (United States)

    Watanabe, Akira; Yamada, Hiromi; Kimura, Makoto

    2001-09-01

    Seasonal variations in CH4 emission rates from rice paddies have been reported to have one or more maxima during the middle and late periods of rice growth. The factor affecting an appearance of CH4 emission maxima was examined in three types of pot experiments. In the experiment 1, four rice cultivars with difference in length of the period from transplanting to heading were transplanted on the same days. For the experiment 2, a cultivar was transplanted 4 times with interval of two weeks. In these experiments, the heading differed about a month between the earliest and latest treatments, respectively. However, shifting growth stage of rice plants did not shift the CH4 emission maxima, and the CH4 emission maxima often matched the maxima of daily mean air temperature. The effect of variation in temperature on CH4 emission rate was further investigated in the experiment 3 by placing the rice-planted pots under regulated temperature. Besides the first emission peak of CH4 attributable to rice straw (RS) carbon, three emission peaks corresponding to the peaks of air temperature were detected for the RS-applied pots placed outdoors. These three peaks were not observed or much less conspicuous for the RS-applied pots in a phytotron at 30°C. Temporal decreases in CH4 emission were detected both for the pots placed in the phytotron and outdoors just after the topdressing of (NH4)2SO4, which was considered to be a major cause of irregular disagreement between the variations in CH4 emission rates and in air temperature during the middle period of rice growth.

  6. CO2/CH4 Separation by a Mixed Matrix Membrane of Polymethylpentyne/MIL-53 Particles

    Directory of Open Access Journals (Sweden)

    Reza Abedini

    2014-10-01

    Full Text Available The effect of Materials Institute Lavoisier-53 (MIL-53 particles on gas transport properties of polymethylpentyne (PMP was investigated. MIL-53 was added to the polymer matrix with different loadings of 10, 20 and 30 wt%. The properties of MIL-53 and prepared membranes were analyzed through FTIR, SEM and TGA methods. The adsorption of CO2 and CH4 was conducted and analyzed accurately through Langmuir equation to investigate the gas transport properties of membranes. The results from TGA showed that degradation temperature (Td increases significantly with increasing MIL-53 loading. SEM images demonstrated that MIL-53 particles dispersed well in polymer matrix with no considerable agglomeration and no non-selective void formation at polymer/filler interface. In addition, CO2 and CH4 permeability measurement along with calculation of CO2/CH4 selectivity were performed. The results showed that the permeability of gases (especially for CO2 increased significantly by increasing the MIL-53 loading. Additionally, CO2/CH4 selectivity showed an increasing trend with increasing the MIL-53 weight percent. Unlike CH4, the CO2 solubility coefficient increased with increasing the MIL-53 loading because of high free volume of membrane and selective adsorption of CO2 with MIL-53. Despite CO2 solubility enhancement its diffusivity coefficient remained more or less unchanged. The enhancement in CH4 permeability has been mainly attributed to its slight incremental diffusivity due to the membrane's increasingly higher free volume. Finally, a comparison between membranes performance and CO2/CH4 Robeson upper bound showed that, the performance of membranes improved due to the presence of MIL-53 which was very close to the Robeson bound.

  7. Bioelectrochemical methane (CH4) production in anaerobic digestion at different supplemental voltages.

    Science.gov (United States)

    Choi, Kwang-Soon; Kondaveeti, Sanath; Min, Booki

    2017-12-01

    Microbial electrolysis cells (MECs) at various cell voltages (0.5, 0.7 1.0 and 1.5V) were operated in anaerobic fermentation. During the start-up period, the cathode potential decreased from -0.63 to -1.01V, and CH 4 generation increased from 168 to 199ml. At an applied voltage of 1.0V, the highest methane yields of 408.3ml CH 4 /g COD glucose was obtained, which was 30.3% higher than in the control tests (313.4ml CH 4 /g COD glucose). The average current of 5.1mA was generated at 1.0V at which the maximum methane yield was obtained. The other average currents were 1.42, 3.02, 0.53mA at 0.5, 0.7, and 1.5V, respectively. Cyclic voltammetry and EIS analysis revealed that enhanced reduction currents were present at all cell voltages with biocatalyzed cathode electrodes (no reduction without biofilm), and the highest value was obtained with 1V external voltage. Copyright © 2017 Elsevier Ltd. All rights reserved.

  8. Fluxes of CH4 and N2O in aspen stands grown under ambient and twice-ambient CO2

    DEFF Research Database (Denmark)

    Ambus, P.; Robertson, G.P.

    1999-01-01

    Elevated atmospheric CO2 has the potential to change below-ground nutrient cycling and thereby alter the soil-atmosphere exchange of biogenic trace gases. We measured fluxes of CH4 and N2O in trembling aspen (Populus tremuloides Michx.) stands grown in open-top chambers under ambient and twice......-ambient CO2 concentrations crossed with `high' and low soil-N conditions. Flux measurements with small static chambers indicated net CH4 oxidation in the open-top chambers. Across dates, CH4 oxidation activity was significantly (P CO2 (8.7 mu g CH4-C m(-2) h(-1)) than...... with elevated CO2 (6.5 mu g CH4-C m(-2) h(-1)) in the low N soil. Likewise, across dates and soil N treatments CH4 was oxidized more rapidly (P CO2 (9.5 mu g CH4-C m(-2) h(-1)) than in chambers with elevated CO2 (8.8 mu g CH4-C m(-2) h(-1)). Methane oxidation in soils incubated...

  9. Ionic fragmentation following core-level photoionization of Sn(CH3)4 by soft X-rays

    International Nuclear Information System (INIS)

    Ueda, Kiyoshi; Shigemasa, Eiji; Sato, Yukinori; Yagishita, Akira; Hayaishi, Tatsuji

    1990-01-01

    Ionic fragmentation following the photoionization of Sn(CH 3 ) 4 (TMT) has been studied in the photon energy range of 60-600 eV using synchrotron radiation and time-of-flight mass spectrometry. Each of the Sn:4d, 4p, 3d and C:1s photoionization leads to a type of ionic fragmentation that is characteristic of each ionized core. The Sn:4d photoionization above 60 eV predominantly produces the doubly-charged TMT which dissociates into two singly-charged ions and some neutral fragments. The ions produced in this pathway are CH 3 + , C 2 H 3 + , C 2 H 5 + , SnCH m + and/or Sn + . The Sn:4p photoionization produces the triply-charged TMT and enhances the production of H + , CHsub(m' + ) (m' = 0-3) and Sn + significantly. The Sn:3d photoionization produces multiply-charged TMT whose charges are 3-5 and enhances the production of H + , CHsub(m' + ) (m' = 0-2) and Sn + significantly. The C:1s photoionization produces doubly-charged TMT via the KVV Auger transition and enhances the production of CH 3 + , C 2 H 3 + , SnCH m + and/or Sn + . (orig.)

  10. Experimental Equipment Validation for Methane (CH4) and Carbon Dioxide (CO2) Hydrates

    Science.gov (United States)

    Saad Khan, Muhammad; Yaqub, Sana; Manner, Naathiya; Ani Karthwathi, Nur; Qasim, Ali; Mellon, Nurhayati Binti; Lal, Bhajan

    2018-04-01

    Clathrate hydrates are eminent structures regard as a threat to the gas and oil industry in light of their irritating propensity to subsea pipelines. For natural gas transmission and processing, the formation of gas hydrate is one of the main flow assurance delinquent has led researchers toward conducting fresh and meticulous studies on various aspects of gas hydrates. This paper highlighted the thermodynamic analysis on pure CH4 and CO2 gas hydrates on the custom fabricated equipment (Sapphire cell hydrate reactor) for experimental validation. CO2 gas hydrate formed at lower pressure (41 bar) as compared to CH4 gas hydrate (70 bar) while comparison of thermodynamic properties between CH4 and CO2 also presented in this study. This preliminary study could provide pathways for the quest of potent hydrate inhibitors.

  11. PENGARUH WAKTU KONTAK TERHADAP DAYA ADSORPSI KARBON AKTIF PADA PROSES PURIFIKASI CH4 DARI BIOGAS

    Directory of Open Access Journals (Sweden)

    Nani Harihastuti

    2016-11-01

    udara , maka dapat memicu efek gas rumah kaca dan pemanasan global karena biogas mengandung gas  CH4 dan CO2 yang sangat signifikan jumlahnya. Kata Kunci : waktu kontak, adsorpsi, karbon aktif, purifikasi,biogas ABSTRACT The use of biogas as a fuel directly use often problem occur that is awful odor, equipment fast burner and rusted metal, kitchen walls eroded and fire often turns off its self. This is due in a biogas other than methane (CH4 contained other gases, H2S, NH3, CO2, H2, CO and water vapor (H2O. Some gases which are impurities (H2S, NH3, CO2 and water vapor/H2O will lower the value of calories from biogas and detrimental to the environment and health. The purpose of this research is to eliminate impurities from gases biogas through a process of purification until obtained biogas which has higher heat value and enviromental friendly. The Methods undertaken by adsorption process using adsorbent activated carbon with variable time contacts, to obtain the optimum adsorption power of activated carbon toward gas impurities that are present in wastewater. The results of this research were obtained data removal/reduction of H2S gas impuritis achieve 99.99%, from 4200 ppm to be 0.22 ppm NH3 gas removal, reach the 12.7%, from 94,96 ppm be 0.65 ppm, removal of CO2 gas reached 77.48%, from levels 30, 77% to 6.93%, removal of water vapour (H2O reached 97,95%, from 0.584 mg/l be 0.012 mg/l.The increase in the concentration of methane (CH4 from 38.2% to 84.12%. Results of methane (CH4 as a result of this biogas is renewable energy sources that are safe and environmentally friendly and can be developed  in other Tofu IKM. The Time saturated activated carbon adsorbents obtained after 48 hours, the process of purification occur. Optimum active Carbon adsorption power towards each component gas impuritis is as follows against the H2S is 10.98 mg H2S/gram of activated carbon/minute, against the NH3 is 0.016 mg NH3/gram of activated carbon/minute, against CO2 is 0.090mg

  12. Study of the daily and seasonal atmospheric CH4 mixing ratio variability in a rural Spanish region using 222Rn tracer

    Science.gov (United States)

    Grossi, Claudia; Vogel, Felix R.; Curcoll, Roger; Àgueda, Alba; Vargas, Arturo; Rodó, Xavier; Morguí, Josep-Anton

    2018-04-01

    The ClimaDat station at Gredos (GIC3) has been continuously measuring atmospheric (dry air) mixing ratios of carbon dioxide (CO2) and methane (CH4), as well as meteorological parameters, since November 2012. In this study we investigate the atmospheric variability of CH4 mixing ratios between 2013 and 2015 at GIC3 with the help of co-located observations of 222Rn concentrations, modelled 222Rn fluxes and modelled planetary boundary layer heights (PBLHs). Both daily and seasonal changes in atmospheric CH4 can be better understood with the help of atmospheric concentrations of 222Rn (and the corresponding fluxes). On a daily timescale, the variation in the PBLH is the main driver for 222Rn and CH4 variability while, on monthly timescales, their atmospheric variability seems to depend on emission changes. To understand (changing) CH4 emissions, nocturnal fluxes of CH4 were estimated using two methods: the radon tracer method (RTM) and a method based on the EDGARv4.2 bottom-up emission inventory, both using FLEXPARTv9.0.2 footprints. The mean value of RTM-based methane fluxes (FR_CH4) is 0.11 mg CH4 m-2 h-1 with a standard deviation of 0.09 or 0.29 mg CH4 m-2 h-1 with a standard deviation of 0.23 mg CH4 m-2 h-1 when using a rescaled 222Rn map (FR_CH4_rescale). For our observational period, the mean value of methane fluxes based on the bottom-up inventory (FE_CH4) is 0.33 mg CH4 m-2 h-1 with a standard deviation of 0.08 mg CH4 m-2 h-1. Monthly CH4 fluxes based on RTM (both FR_CH4 and FR_CH4_rescale) show a seasonality which is not observed for monthly FE_CH4 fluxes. During January-May, RTM-based CH4 fluxes present mean values 25 % lower than during June-December. This seasonal increase in methane fluxes calculated by RTM for the GIC3 area appears to coincide with the arrival of transhumant livestock at GIC3 in the second half of the year.

  13. BOREAS TGB-1 Soil CH4 and CO2 Profile Data from NSA Tower Sites

    Science.gov (United States)

    Crill, Patrick; Varner, Ruth K.; Hall, Forrest G. (Editor); Conrad, Sara K. (Editor)

    2000-01-01

    The BOREAS TGB-1 team made numerous measurements of trace gas concentrations and fluxes at various NSA sites. This data set contains methane (CH4) and carbon dioxide (CO2) concentrations in soil profiles from the NSA-OJP, NSA-OBS, NSA-YJP, and NSA-BP sites during the period of 23-May to 20-Sep-1994. The soil gas sampling profiles of CH 4 and CO 2 were completed to quantify controls on CO2 and CH4 fluxes in the boreal forest. The data are provided in tabular ASCII files.

  14. Determination of chloromethane and dichloromethane in a tropical terrestrial mangrove forest in Brazil by measurements and modelling

    Science.gov (United States)

    Kolusu, S. R.; Schlünzen, K. H.; Grawe, D.; Seifert, R.

    2018-01-01

    Chloromethane (CH3Cl) and dichloromethane (CH2Cl2) are known to have both natural and anthropogenic sources to the atmosphere. From recent studies it is known that tropical and sub tropical plants are primary sources of CH3Cl in the atmosphere. In order to quantify the biogenic emissions of CH3Cl and CH2Cl2 from mangroves, field measurement were conducted in a tropical mangrove forest on the coast of Brazil. To the best of our knowledge these field measurements were the first of its kind conducted in the tropical mangrove ecosystem of Braganca. A mesoscale atmospheric model, MEsoscale TRAnsport and fluid (Stream) model (METRAS), was used to simulate passive tracers concentrations and to study the dependency of concentrations on type of emission function and meteorology. Model simulated concentrations were normalized using the observed field data. With the help of the mesoscale model results and the observed data the mangrove emissions were estimated at the local scale. By using this bottom-up approach the global emissions of CH3Cl and CH2Cl2 from mangroves were quantified. The emission range obtained with different emission functions and different meteorology are 4-7 Gg yr-1 for CH3Cl and 1-2 Gg yr2 for CH2Cl2. Based on the present study the mangroves contribute 0.3 percent of CH2Cl2 and 0.2 percent of CH3Cl in the global emission budget. This study corroborates the study by Manley et al. (2007) which estimated that mangroves produce 0.3 percent of CH3Cl in the global emission budget. Although they contribute a small percentage in the global budget, their long lifetime enables them to contribute to the destruction of ozone in the stratosphere. From the detailed analyses of the model results it can be concluded that meteorology has a larger influence on the variability of concentrations than the temporal variability of the emission function.

  15. A Switchable Molecular Dielectric with Two Sequential Reversible Phase Transitions: [(CH3)4P]4[Mn(SCN)6].

    Science.gov (United States)

    Li, Qiang; Shi, Ping-Ping; Ye, Qiong; Wang, Hui-Ting; Wu, De-Hong; Ye, Heng-Yun; Fu, Da-Wei; Zhang, Yi

    2015-11-16

    A new organic-inorganic hybrid switchable and tunable dielectric compound, [(CH3)4P]4[Mn(SCN)6] (1), exhibits three distinct dielectric states above room temperature and undergoes two reversible solid-state phase transitions, including a structural phase transition at 330 K and a ferroelastic phase transition with the Aizu notation of mmmF2/m at 352 K. The variable-temperature structural analyses disclose that the origin of the phase transitions and dielectric anomalies can be ascribed to the reorientation or motion of both the [(CH3)4P](+) cations and [Mn(SCN)6](4-) anions in solid-state crystals.

  16. Nutrient Addition Leads to a Weaker CO2 Sink and Higher CH4 Emissions through Vegetation-Microclimate Feedbacks at Mer Bleue Bog, Canada

    Science.gov (United States)

    Bubier, J. L.; Arnkil, S.; Humphreys, E.; Juutinen, S.; Larmola, T.; Moore, T. R.

    2015-12-01

    Atmospheric nitrogen (N) deposition has led to nutrient enrichment in wetlands globally, affecting plant community composition, carbon (C) cycling, and microbial dynamics. Nutrient-limited boreal bogs are long-term sinks of carbon dioxide (CO2), but sources of methane (CH4), an important greenhouse gas. We fertilized Mer Bleue Bog, a Sphagnum moss and evergreen shrub-dominated ombrotrophic bog near Ottawa, Ontario, for 10-15 years with N as NO3 and NH4 at 5, 10 and 20 times ambient N deposition (0.6-0.8 g N m-2 y-1), with and without phosphorus (P) and potassium (K). Treatments were applied to triplicate plots (3 x 3 m) from May - August 2000-2015 and control plots received distilled water. We measured net ecosystem CO2 exchange (NEE), ecosystem photosynthesis and respiration, and CH4 flux with climate-controlled chambers; leaf-level CO2 exchange and biochemistry; substrate-induced respiration, CH4 production and consumption potentials with laboratory incubations; plant species composition and abundance; and microclimate (peat temperature, moisture, light interception). After 15 years, we have found that NEE has decreased, and CH4 emissions have increased, in the highest nutrient treatments owing to changes in vegetation, microtopography, and peat characteristics. Vegetation changes include a loss of Sphagnum moss and introduction of new deciduous species. Simulated atmospheric N deposition has not benefitted the photosynthetic apparatus of the dominant evergreen shrubs, but resulted in higher foliar respiration, contributing to a weaker ecosystem CO2 sink. Loss of moss has led to wetter near-surface substrate, higher rates of decomposition and CH4 emission, and a shift in microbial communities. Thus, elevated atmospheric deposition of nutrients may endanger C storage in peatlands through a complex suite of feedbacks and interactions among vegetation, microclimate, and microbial communities.

  17. Numerical Simulation and Industrial Experimental Research on the Coherent Jet with "CH4 + N2" Mixed Fuel Gas

    Science.gov (United States)

    Hu, Shaoyan; Zhu, Rong; Dong, Kai; Liu, Runzao

    2018-06-01

    Coherent jet technology is widely used in the electric arc furnace (EAF) steelmaking process to deliver more energy and momentum into the molten steel bath. Meanwhile, the characteristics of a coherent jet using pure CH4 as the fuel gas have been well investigated in previous studies. To reduce the consumption of CH4, coherent jet technology using "CH4 + N2" mixed fuel gas instead of pure CH4 was proposed and studied in detail by numerical simulation in the present work. The Eddy Dissipation Concept model, which has detailed chemical kinetic mechanisms, was adopted to model the fuel gas combustion reactions. Experimental measurements were carried out to validate the accuracy of the computational model. The present study shows that the jet characteristics of the main oxygen improve along with the increase of the CH4 ratio in fuel gas and with the increase of the flow rate of fuel gas. When the CH4 ratio in the fuel gas is 25 pct, the fuel gas flow rate only has a limited influence on the jet characteristics, unlike the rest of the fuel gas compositions, because a high N2 proportion deteriorates the combustion performance and leads to severe incomplete combustion. Moreover, a false potential core phenomenon was observed and explained in the present study. Based on the average values, the jet length of a coherent jet with 75 pct CH4 can achieve 89.8 pct of that with 100 pct CH4. Finally, an industrial experiment was carried out on a commercial 100t EAF using coherent jet with 75 pct CH4, showing that the average CH4 consumption was reduced from 3.84 to 3.05 Nm3 t-1 under the premise of no obvious changes in the other production indexes.

  18. Synthesis of fluorinated ReCl(4,4'-R2-2,2'-bipyridine)(CO)3 complexes and their photophysical characterization in CH3CN and supercritical CO2.

    Science.gov (United States)

    Doherty, Mark D; Grills, David C; Fujita, Etsuko

    2009-03-02

    Two new CO(2)-soluble rhenium(I) bipyridine complexes bearing the fluorinated alkyl ligands 4,4'-(C(6)F(13)CH(2)CH(2)CH(2))(2)-2,2'-bipyridine (1a), and 4,4'-(C(8)F(17)CH(2)CH(2)CH(2))(2)-2,2'-bipyridine (1b) have been prepared and their photophysical properties investigated in CH(3)CN and supercritical CO(2). Electrochemical and spectroscopic characterization of these complexes in CH(3)CN suggests that the three methylene units effectively insulate the bipyridyl rings and the rhenium center from the electron-withdrawing effect of the fluorinated alkyl chains. Reductive quenching of the metal-to-ligand charge-transfer excited states with triethylamine reveals quenching rate constants in supercritical CO(2) that are only 6 times slower than those in CH(3)CN.

  19. Synthesis and crystal structure of 4-fluorobenzylammonium dihydrogen phosphate, [FC6H4CH2NH3]H2PO4

    Directory of Open Access Journals (Sweden)

    Ali Rayes

    2016-12-01

    Full Text Available The asymmetric unit of the title salt, [p-FC6H4CH2NH3]+·H2PO4−, contains one 4-fluorobenzylammonium cation and one dihydrogen phosphate anion. In the crystal, the H2PO4− anions are linked by O—H...O hydrogen bonds to build corrugated layers extending parallel to the ab plane. The FC6H4CH2NH3+ cations lie between these anionic layers to maximize the electrostatic interactions and are linked to the H2PO4− anions through N—H...O hydrogen bonds, forming a three-dimensional supramolecular network. Two hydrogen atoms belonging to the dihydrogen phosphate anion are statistically occupied due to disorder along the OH...HO direction.

  20. Dentritic Carbosilanes Containing Silicon-Bonded 1-[C6H2(CH2NMe2)2-3,5-Li-4] or 1-[C6H3(CH2NMe2)-4-Li-3] Mono-and Bis(amino)aryllithium End Groups: Structure of {[CH2SiMe2C6H3(CH2NMe2)-4-Li-3]2}2

    NARCIS (Netherlands)

    Koten, G. van; Kleij, A.W.; Kleijn, H.; Jastrzebski, J.T.B.H.; Smeets, W.J.J.; Spek, A.L.

    1999-01-01

    A useful synthetic procedure for the incorporation of the potentially multidentate monoanionic 1-[C6H2(CH2NMe2)2-3,5]- (=NCN) and 1-[C6H3(CH2NMe2)-4]- (=CN) ligands via the para-position on the periphery of carbosilane (CS) dendrimers has been developed. Lithiation of suitable brominated precursors

  1. Eight-dimensional quantum reaction rate calculations for the H+CH4 and H2+CH3 reactions on recent potential energy surfaces.

    Science.gov (United States)

    Zhou, Yong; Zhang, Dong H

    2014-11-21

    Eight-dimensional (8D) transition-state wave packet simulations have been performed on two latest potential energy surfaces (PES), the Zhou-Fu-Wang-Collins-Zhang (ZFWCZ) PES [Y. Zhou, B. Fu, C. Wang, M. A. Collins, and D. H. Zhang, J. Chem. Phys. 134, 064323 (2011)] and the Xu-Chen-Zhang (XCZ)-neural networks (NN) PES [X. Xu, J. Chen, and D. H. Zhang, Chin. J. Chem. Phys. 27, 373 (2014)]. Reaction rate constants for both the H+CH4 reaction and the H2+CH3 reaction are calculated. Simulations of the H+CH4 reaction based on the XCZ-NN PES show that the ZFWCZ PES predicts rate constants with reasonable high accuracy for low temperatures while leads to slightly lower results for high temperatures, in line with the distribution of interpolation error associated with the ZFWCZ PES. The 8D H+CH4 rate constants derived on the ZFWCZ PES compare well with full-dimensional 12D results based on the equivalent m-ZFWCZ PES, with a maximum relative difference of no more than 20%. Additionally, very good agreement is shown by comparing the 8D XCZ-NN rate constants with the 12D results obtained on the ZFWCZ-WM PES, after considering the difference in static barrier height between these two PESs. The reaction rate constants calculated for the H2+CH3 reaction are found to be in good consistency with experimental observations.

  2. Advances of study on atmospheric methane oxidation (consumption) in forest soil

    Institute of Scientific and Technical Information of China (English)

    WANG Chen-rui; SHI Yi; YANG Xiao-ming; WU Jie; YUE Jin

    2003-01-01

    Next to CO2, methane (CH4) is the second important contributor to global warming in the atmosphere and global atmospheric CH4 budget depends on both CH4 sources and sinks. Unsaturated soil is known as a unique sink for atmospheric CH4 in terrestrial ecosystem. Many comparison studies proved that forest soil had the biggest capacity of oxidizing atmospheric CH4 in various unsaturated soils. However, up to now, there is not an overall review in the aspect of atmospheric CH4 oxidation (consumption) in forest soil. This paper analyzed advances of studies on the mechanism of atmospheric CH4 oxidation, and related natural factors (Soil physical and chemical characters, temperature and moisture, ambient main greenhouse gases concentrations, tree species, and forest fire) and anthropogenic factors (forest clear-cutting and thinning, fertilization, exogenous aluminum salts and atmospheric deposition, adding biocides, and switch of forest land use) in forest soils. It was believed that CH4 consumption rate by forest soil was limited by diffusion and sensitive to changes in water status and temperature of soil. CH4 oxidation was also particularly sensitive to soil C/N, Ambient CO2, CH4 and N2O concentrations, tree species and forest fire. In most cases, anthropogenic disturbances will decrease atmospheric CH4 oxidation, thus resulting in the elevating of atmospheric CH4. Finally, the author pointed out that our knowledge of atmospheric CH4 oxidation (consumption) in forest soil was insufficient. In order to evaluate the contribution of forest soils to atmospheric CH4 oxidation and the role of forest played in the process of global environmental change, and to forecast the trends of global warming exactly, more researchers need to studies further on CH4 oxidation in various forest soils of different areas.

  3. Kinetics of the Formation and Dissociation of Gas Hydrates from CO2-CH4 Mixtures

    Directory of Open Access Journals (Sweden)

    Devinder Mahajan

    2012-07-01

    Full Text Available Sequestration of carbon dioxide (CO2 in the form of its hydrates in natural methane (CH4 hydrate reservoirs, via CO2/CH4 exchange, is an attractive pathway that also yields valuable CH4 gas as product. In this paper, we describe a macroscale experiment to form CO2 and CH4-CO2 hydrates, under seafloor-mimic conditions, in a vessel fitted with glass windows that provides visualization of hydrates throughout formation and dissociation processes. Time resolved pressure and temperature data as well as images of hydrates are presented. Quantitative gas conversions with pure CO2, calculated from gas chromatographic measurements yielded values that range from 23 – 59% that correspond to the extent of formed hydrates. In CH4-rich CH4-CO2 mixed gas systems, CH4 hydrates were found to form preferentially.

  4. Assessing fugitive emissions of CH4 from high-pressure gas pipelines in the UK

    Science.gov (United States)

    Clancy, S.; Worrall, F.; Davies, R. J.; Almond, S.; Boothroyd, I.

    2016-12-01

    Concern over the greenhouse gas impact of the exploitation of unconventional natural gas from shale deposits has caused a spotlight to be shone on to the entire hydrocarbon industry. Numerous studies have developed life-cycle emissions inventories to assess the impact that hydraulic fracturing has upon greenhouse gas emissions. Incorporated within life-cycle assessments are transmission and distribution losses, including infrastructure such as pipelines and compressor stations that pressurise natural gas for transport along pipelines. Estimates of fugitive emissions from transmission, storage and distribution have been criticized for reliance on old data from inappropriate sources (1970s Russian gas pipelines). In this study, we investigate fugitive emissions of CH4 from the UK high pressure national transmission system. The study took two approaches. Firstly, CH4 concentration is detected by driving along roads bisecting high pressure gas pipelines and also along an equivalent distance along a route where no high pressure gas pipeline was nearby. Five pipelines and five equivalent control routes were driven and the test was that CH4 measurements, when adjusted for distance and wind speed, should be greater on any route with a pipe than any route without a pipe. Secondly, 5 km of a high pressure gas pipeline and 5 km of equivalent farmland, were walked and soil gas (above the pipeline where present) was analysed every 7 m using a tunable diode laser. When wind adjusted 92 km of high pressure pipeline and 72 km of control route were drive over a 10 day period. When wind and distance adjusted CH4 fluxes were significantly greater on routes with a pipeline than those without. The smallest leak detectable was 3% above ambient (1.03 relative concentration) with any leaks below 3% above ambient assumed ambient. The number of leaks detected along the pipelines correlate to the estimated length of pipe joints, inferring that there are constant fugitive CH4 emissions from

  5. Evaluation of the Global Mean Sea Level Budget between 1993 and 2014

    DEFF Research Database (Denmark)

    Chambers, Don P.; Cazenave, Anny; Champollion, Nicolas

    2017-01-01

    Evaluating global mean sea level (GMSL) in terms of its components—mass and steric—is useful for both quantifying the accuracy of the measurements and understanding the processes that contribute to GMSL rise. In this paper, we review the GMSL budget over two periods—1993 to 2014 and 2005 to 2014......—using multiple data sets of both total GMSL and the components (mass and steric). In addition to comparing linear trends, we also compare the level of agreement of the time series. For the longer period (1993–2014), we find closure in terms of the long-term trend but not for year-to-year variations...

  6. Methane emissions from global wetlands: An assessment of the uncertainty associated with various wetland extent data sets

    Science.gov (United States)

    Zhang, Bowen; Tian, Hanqin; Lu, Chaoqun; Chen, Guangsheng; Pan, Shufen; Anderson, Christopher; Poulter, Benjamin

    2017-09-01

    A wide range of estimates on global wetland methane (CH4) fluxes has been reported during the recent two decades. This gives rise to urgent needs to clarify and identify the uncertainty sources, and conclude a reconciled estimate for global CH4 fluxes from wetlands. Most estimates by using bottom-up approach rely on wetland data sets, but these data sets show largely inconsistent in terms of both wetland extent and spatiotemporal distribution. A quantitative assessment of uncertainties associated with these discrepancies among wetland data sets has not been well investigated yet. By comparing the five widely used global wetland data sets (GISS, GLWD, Kaplan, GIEMS and SWAMPS-GLWD), it this study, we found large differences in the wetland extent, ranging from 5.3 to 10.2 million km2, as well as their spatial and temporal distributions among the five data sets. These discrepancies in wetland data sets resulted in large bias in model-estimated global wetland CH4 emissions as simulated by using the Dynamic Land Ecosystem Model (DLEM). The model simulations indicated that the mean global wetland CH4 emissions during 2000-2007 were 177.2 ± 49.7 Tg CH4 yr-1, based on the five different data sets. The tropical regions contributed the largest portion of estimated CH4 emissions from global wetlands, but also had the largest discrepancy. Among six continents, the largest uncertainty was found in South America. Thus, the improved estimates of wetland extent and CH4 emissions in the tropical regions and South America would be a critical step toward an accurate estimate of global CH4 emissions. This uncertainty analysis also reveals an important need for our scientific community to generate a global scale wetland data set with higher spatial resolution and shorter time interval, by integrating multiple sources of field and satellite data with modeling approaches, for cross-scale extrapolation.

  7. Renewable energy based catalytic CH4 conversion to fuels

    NARCIS (Netherlands)

    Baltrusaitis, Jonas; Jansen, I.; Schuttlefield, J.D.S.

    2014-01-01

    Natural gas is envisioned as a primary source of hydrocarbons in the foreseeable future. With the abundance of shale gas, the main concerns have shifted from the limited hydrocarbon availability to the sustainable methods of CH4 conversion to fuels. This is necessitated by high costs of natural gas

  8. The 'Alternative Quality Contract,' based on a global budget, lowered medical spending and improved quality.

    Science.gov (United States)

    Song, Zirui; Safran, Dana Gelb; Landon, Bruce E; Landrum, Mary Beth; He, Yulei; Mechanic, Robert E; Day, Matthew P; Chernew, Michael E

    2012-08-01

    Seven provider organizations in Massachusetts entered the Blue Cross Blue Shield Alternative Quality Contract in 2009, followed by four more organizations in 2010. This contract, based on a global budget and pay-for-performance for achieving certain quality benchmarks, places providers at risk for excessive spending and rewards them for quality, similar to the new Pioneer Accountable Care Organizations in Medicare. We analyzed changes in spending and quality associated with the Alternative Quality Contract and found that the rate of increase in spending slowed compared to control groups, more so in the second year than in the first. Overall, participation in the contract over two years led to savings of 2.8 percent (1.9 percent in year 1 and 3.3 percent in year 2) compared to spending in nonparticipating groups. Savings were accounted for by lower prices achieved through shifting procedures, imaging, and tests to facilities with lower fees, as well as reduced utilization among some groups. Quality of care also improved compared to control organizations, with chronic care management, adult preventive care, and pediatric care within the contracting groups improving more in year 2 than in year 1. These results suggest that global budgets with pay-for-performance can begin to slow underlying growth in medical spending while improving quality of care.

  9. Release of CO{sub 2} and CH{sub 4} from small wetland lakes in western Siberia

    Energy Technology Data Exchange (ETDEWEB)

    Repo, M.E.; Huttunen, J.T.; Martikainen, P.J. [Univ. of Kuopio, Dept. of Env ironmental Science, FI-70211 Kuopio (Finland); Naumov, A.V.; Chichulin, A.V. [I nst. of Soil Science and Agrochemistry, Russian Academy of Science, 630099 Novos ibirsk (Russian Federation); Lapshina, E.D. [Yugra State Univ., 628012, Khanty-Mansiysk (Russian Federation); Bleuten , W. [Utrecht Univ., Dept. of Physical Geography,3508 TC Utrecht (Netherlands)

    2007-11-15

    CO{sub 2} and CH{sub 4} fluxes were measured from three small wetland lakes located in the middle taiga and forest tundra zones on West Siberian Lowlands (WSL), the world's largest wetland area. Fluxes were measured during summer 2005 using floating chambers and were validated against the thin boundary layer model based on the relationship between gas exchange and wind speed. All studied lakes were supersaturated with CO{sub 2} and CH{sub 4}, and acted on a seasonal basis as sources of these greenhouse gases to the atmosphere. Daily mean CO{sub 2} fluxes measured with chambers ranged from near the zero to 3.1 g CO{sub 2}/m{sup 2}/d and corresponding CH{sub 4} fluxes from 1.1 to 120 mg CH{sub 4}/m{sup 2}/d. CH{sub 4} ebullition (0.65-11 mg CH{sub 4}/m{sup 2}/d) was detected in two of the lakes. Total carbon evasion from the studied lakes during the active season was 23-66 g C/m{sup 2}, of which more than 90% was released as CO{sub 2}-C. The carbon loss per unit area from the studied lakes was of similar magnitude as previously reported values of net carbon uptake of Siberian peatlands. This emphasizes the importance of small water-bodies in the carbon balance of West Siberian landscape.

  10. GCIP water and energy budget synthesis (WEBS)

    Science.gov (United States)

    Roads, J.; Lawford, R.; Bainto, E.; Berbery, E.; Chen, S.; Fekete, B.; Gallo, K.; Grundstein, A.; Higgins, W.; Kanamitsu, M.; Krajewski, W.; Lakshmi, V.; Leathers, D.; Lettenmaier, D.; Luo, L.; Maurer, E.; Meyers, T.; Miller, D.; Mitchell, Ken; Mote, T.; Pinker, R.; Reichler, T.; Robinson, D.; Robock, A.; Smith, J.; Srinivasan, G.; Verdin, K.; Vinnikov, K.; Vonder, Haar T.; Vorosmarty, C.; Williams, S.; Yarosh, E.

    2003-01-01

    As part of the World Climate Research Program's (WCRPs) Global Energy and Water-Cycle Experiment (GEWEX) Continental-scale International Project (GCIP), a preliminary water and energy budget synthesis (WEBS) was developed for the period 1996-1999 fromthe "best available" observations and models. Besides this summary paper, a companion CD-ROM with more extensive discussion, figures, tables, and raw data is available to the interested researcher from the GEWEX project office, the GAPP project office, or the first author. An updated online version of the CD-ROM is also available at http://ecpc.ucsd.edu/gcip/webs.htm/. Observations cannot adequately characterize or "close" budgets since too many fundamental processes are missing. Models that properly represent the many complicated atmospheric and near-surface interactions are also required. This preliminary synthesis therefore included a representative global general circulation model, regional climate model, and a macroscale hydrologic model as well as a global reanalysis and a regional analysis. By the qualitative agreement among the models and available observations, it did appear that we now qualitatively understand water and energy budgets of the Mississippi River Basin. However, there is still much quantitative uncertainty. In that regard, there did appear to be a clear advantage to using a regional analysis over a global analysis or a regional simulation over a global simulation to describe the Mississippi River Basin water and energy budgets. There also appeared to be some advantage to using a macroscale hydrologic model for at least the surface water budgets. Copyright 2003 by the American Geophysical Union.

  11. Atmospheric chemistry of CH3O(CF2CF2O)(n)CH3 (n=1-3): Kinetics and mechanism of oxidation initiated by Cl atoms and OH radicals, IR spectra, and global warmin potentials

    DEFF Research Database (Denmark)

    Andersen, Mads Peter Sulbæk; Hurley, MD; Wallington, TJ

    2004-01-01

    Smog chambers equipped with FTIR spectrometers were used to study the Cl atom and OH radical initiated oxidation of CH3O(CF2CF2O)(n)CH3 (n = 1-3) in 720 +/- 20 Torr of air at 296 +/- 3 K. Relative rate techniques were used to measure k(Cl + CH3O(CF2CF2O)(n)CH3) (3.7 +/- 10.7) x 10(-13) and k......(OH + CH3O(CF2CF2O)(n)CH3) = (2.9 +/- 0.5) x 10(-11) cm(3) molecule(-1) s(-1) leading to an estimated atmospheric lifetime of 2 years for CH3O(CF2CF2O),CH3. The Cl initiated oxidation of CH3O(CF2CF2O),CH3 in air diluent gives CH3O(CF2CF2O)(n)C(O)H in a yield which is indistinguishable from 100 Further...... oxidation leads to the diformate, H(O)CO(CF2CF2O)(n)C(O)H. A rate constant of k(Cl + CH3O(CF2CF2O)(n)CHO) = (1.81 +/- 0.36) x 10(-13) cm(3) molecule(-1) s-1 was determined. Quantitative infrared spectra for CH3O(CF2CF2O)(n)CH3 (n = 1-3) were recorded and used to estimate halocarbon global warming potentials...

  12. Terrestrial plant methane production and emission

    DEFF Research Database (Denmark)

    Bruhn, Dan; Møller, Ian M.; Mikkelsen, Teis Nørgaard

    2012-01-01

    In this minireview, we evaluate all experimental work published on the phenomenon of aerobic methane (CH4) generation in terrestrial plants and plant. Clearly, despite much uncertainty and skepticism, we conclude that the phenomenon is true. Four stimulating factors have been observed to induce...... aerobic CH4 into a global budget is inadequate. Thus it is too early to draw the line under the aerobic methane emission in plants. Future work is needed for establishing the relative contribution of several proven potential CH4 precursors in plant material....

  13. Methane production as key to the greenhouse gas budget of thawing permafrost

    Science.gov (United States)

    Knoblauch, Christian; Beer, Christian; Liebner, Susanne; Grigoriev, Mikhail N.; Pfeiffer, Eva-Maria

    2018-04-01

    Permafrost thaw liberates frozen organic carbon, which is decomposed into carbon dioxide (CO2) and methane (CH4). The release of these greenhouse gases (GHGs) forms a positive feedback to atmospheric CO2 and CH4 concentrations and accelerates climate change1,2. Current studies report a minor importance of CH4 production in water-saturated (anoxic) permafrost soils3-6 and a stronger permafrost carbon-climate feedback from drained (oxic) soils1,7. Here we show through seven-year laboratory incubations that equal amounts of CO2 and CH4 are formed in thawing permafrost under anoxic conditions after stable CH4-producing microbial communities have established. Less permafrost carbon was mineralized under anoxic conditions but more CO2-carbon equivalents (CO2-Ce) were formed than under oxic conditions when the higher global warming potential (GWP) of CH4 is taken into account8. A model of organic carbon decomposition, calibrated with the observed decomposition data, predicts a higher loss of permafrost carbon under oxic conditions (113 ± 58 g CO2-C kgC-1 (kgC, kilograms of carbon)) by 2100, but a twice as high production of CO2-Ce (241 ± 138 g CO2-Ce kgC-1) under anoxic conditions. These findings challenge the view of a stronger permafrost carbon-climate feedback from drained soils1,7 and emphasize the importance of CH4 production in thawing permafrost on climate-relevant timescales.

  14. Formation of doubly and triply bonded unsaturated compounds HCN, HNC, and CH2NH via N + CH4 low-temperature solid state reaction: from molecular clouds to solar system objects

    Science.gov (United States)

    Mencos, Alejandro; Krim, Lahouari

    2018-06-01

    We show in the current study carried out in solid phase at cryogenic temperatures that methane (CH4) ice exposed to nitrogen atoms is a source of two acids HCN, HNC, and their corresponding hydrogenated unsaturated species CH2NH, in addition to CH3, C2H6, CN-, and three nitrogen hydrides NH, NH2, and NH3. The solid state N + CH4 reaction taken in the ground state seems to be strongly temperature dependent. While at temperatures lower than 10 K only CH3, NH, NH2, and NH3 species formation is promoted due to CH bond dissociation and NH bond formation, stable compounds with CN bonds are formed at temperatures ranged between 10 and 40 K. Many of these reaction products, resulting from CH4 + N reaction, have already been observed in N2-rich regions such as the atmospheres of Titan, Kuiper belt objects, and molecular clouds of the interstellar medium. Our results show the power of the solid state N-atom chemistry in the transformation of simple astrochemical relevant species, such as CH4 molecules and N atoms into complex organic molecules which are also potentially prebiotic species.

  15. Preparation of CH4 for 14C measurements

    International Nuclear Information System (INIS)

    Cechova, A.; Grgula, M.; Povinec, P.; Sivo, A.

    1988-01-01

    An improved method of methane preparation from wood samples is described. It consists of the preparation of α-cellulose to secure a complete removal of contamination from the wood, its combustion to the form of CO 2 and the preparation of CH 4 in a new designed hydrogenation converter. Purified methane is suitable as a gas filling of the proportional counter. (author). 1 fig., 16 ref

  16. Direct measurements of methoxy removal rate constants for collisions with CH4, Ar, N2, Xe, and CF4 in the temperature range 673--973K

    International Nuclear Information System (INIS)

    Wantuck, P.J.; Oldenborg, R.C.; Baugchum, S.L.; Winn, K.R.

    1988-01-01

    Removal rate constants for CH 3 O by CH 4 , Ar, N 2 , Xe, and CF 4 were measured over a 400K temperature range using a laser photolysis/laser-induced fluorescence technique. Rapid methoxy removal rates are observed for the non-reactive collision partners (Ar, N 2 , Xe, and CF 4 ) at elevated temperatures showing that the dissociation and isomerization channels for CH 3 O are indeed important. The total removal rate constant (reaction /plus/ dissociation and/or isomerization) for CH 4 exhibits a linear dependence on temperature and has a removal rate constant, k/sub r/ /equals/ (1.2 +- 0.6) /times/ 10/sup /minus/8/exp[(/minus/101070 +- 350)/T]cm 3 molecule/sup /minus/1/s/sup /minus/1/. Assuming that the removal rate constant due to dissociation and/or isomerization are similar for CH 4 and CF 4 , the reaction rate constant for CH 3 O /plus/ CH 4 is equal to (1.7 +- 1.0) /times/ 10/sup /minus/10/exp[(/minus/7480 +- 1100)/T]cm 3 molecule/sup /minus/1/s/sup /minus/1/. 7 refs., 4 figs

  17. Atmospheric modeling of Mars CH4 subsurface clathrates releases mimicking SAM and 2003 Earth-based detections

    Science.gov (United States)

    Pla-García, J.; Rafkin, S. C.

    2017-12-01

    The aim of this work is to establish the amount of mixing during all martian seasons to test whether CH4 releases inside or outside of Gale crater are consistent with MSL-SAM observations. Several modeling scenarios were configured, including instantaneous and steady releases, both inside and outside the crater. A simulation to mimic the 2003 Earth-based detections (Mumma et al. 2009 or M09) was also performed. In the instantaneous release inside Gale experiments, Ls270 was shown to be the faster mixing season when air within and outside the crater was well mixed: all tracer mass inside the crater is diluted after just 8 hours. The mixing of near surface crater air with the external environment in the rest of the year is potentially rapid but slower than Ls270.In the instantaneous release outside Gale (NW) experiment, in just 12 hours the CH4 that makes it to the MSL landing location is diluted by six orders of magnitude. The timescale of mixing in MRAMS experiments is on the order of 1 sol regardless of season. The duration of the CH4 peak observed by SAM is 100 sols. Therefore there is a steady release inside the crater, or there is a very large magnitude steady release outside the crater. In the steady release Gale experiments, CH4 flux rate from ground is 1.8 kg m-2 s-1 (derived from Gloesener et al. 2017 clathrates fluxes) and it is not predictive. In these experiments, 200 times lower CH4 values detected by SAM are modeled around MSL location. There are CH4 concentration variations of orders of magnitude depending on the hour, so timing of SAM measurements is important. With a larger (but further away) outside crater release area compared to inside, similar CH4 values around MSL are modeled, so distance to source is important. In the steady experiments mimicking M09 detection release area, only 12 times lower CH4 values detected by SAM are modeled around MSL. The highest value in the M09 modeled scenario (0.6 ppbv) is reached in Ls270. This value is the

  18. The c2d Spitzer spectroscopic survey of ices around low-mass young stellar objects. III. CH4

    NARCIS (Netherlands)

    Oberg, Karin I.; Boogert, A. C. Adwin; Pontoppidan, Klaus M.; Blake, Geoffrey A.; Evans, Neal J.; Lahuis, Fred; van Dishoeck, Ewine F.

    2008-01-01

    CH4 is proposed to be the starting point of a rich organic chemistry. Solid CH4 abundances have previously been determined mostly toward high-mass star-forming regions. Spitzer IRS now provides a unique opportunity to probe solid CH4 toward low-mass star-forming regions as well. Infrared spectra

  19. Year-Round Carbon Fluxes in a Subarctic Landscape Show the Importance of Lake Emissions According to Season

    Science.gov (United States)

    Jammet, M.; Crill, P. M.; Friborg, T.

    2014-12-01

    Lakes are increasingly recognized as important components of the global terrestrial carbon budget. Northern lakes are especially of interest due to a high density of open-water ecosystems in Northern latitudes and a potential increase in lake areal extent where permafrost is thawing. A better understanding of lake-atmosphere interactions requires long-term and direct measurement of surface fluxes. This is rarely achieved in Northern landscapes where seasonally ice-covered lakes are mostly studied during the open water season, and measurement methods do not always allow an integration of all gas transport pathways to the atmosphere. We present here ecosystem-scale data from Stordalen (68°20'N, 19°03'E), a thawing permafrost peatland in subarctic Sweden, where an eddy covariance system is used in an innovative way to quantify the importance of methane (CH4) emissions from a shallow lake. After more than a year of surface flux monitoring, it is found that spring is a crucial season for lake-atmosphere CH4 exchange. Despite its shallow depth, more than half of annual CH4 emissions from the lake were recorded at ice-out, suggesting significant winter CH4 production in lake sediments. Lake water dynamics seemed to drive the observed spring release rates. In contrast, summer methane emissions in Stordalen were dominated by the minerotrophic fens. This underlines the importance of considering the full annual budget when assessing the carbon source strength of seasonally ice-covered lakes. Carbon dioxide fluxes were also monitored and will be briefly discussed, as well as the significance of northern lakes spring burst for global atmospheric CH4 budget.

  20. Reactivity of chemisorbed oxygen atoms and their catalytic consequences during CH4-O2 catalysis on supported Pt clusters.

    Science.gov (United States)

    Chin, Ya-Huei Cathy; Buda, Corneliu; Neurock, Matthew; Iglesia, Enrique

    2011-10-12

    Kinetic and isotopic data and density functional theory treatments provide evidence for the elementary steps and the active site requirements involved in the four distinct kinetic regimes observed during CH(4) oxidation reactions using O(2), H(2)O, or CO(2) as oxidants on Pt clusters. These four regimes exhibit distinct rate equations because of the involvement of different kinetically relevant steps, predominant adsorbed species, and rate and equilibrium constants for different elementary steps. Transitions among regimes occur as chemisorbed oxygen (O*) coverages change on Pt clusters. O* coverages are given, in turn, by a virtual O(2) pressure, which represents the pressure that would give the prevalent steady-state O* coverages if their adsorption-desorption equilibrium was maintained. The virtual O(2) pressure acts as a surrogate for oxygen chemical potentials at catalytic surfaces and reflects the kinetic coupling between C-H and O═O activation steps. O* coverages and virtual pressures depend on O(2) pressure when O(2) activation is equilibrated and on O(2)/CH(4) ratios when this step becomes irreversible as a result of fast scavenging of O* by CH(4)-derived intermediates. In three of these kinetic regimes, C-H bond activation is the sole kinetically relevant step, but occurs on different active sites, which evolve from oxygen-oxygen (O*-O*), to oxygen-oxygen vacancy (O*-*), and to vacancy-vacancy (*-*) site pairs as O* coverages decrease. On O*-saturated cluster surfaces, O*-O* site pairs activate C-H bonds in CH(4) via homolytic hydrogen abstraction steps that form CH(3) groups with significant radical character and weak interactions with the surface at the transition state. In this regime, rates depend linearly on CH(4) pressure but are independent of O(2) pressure. The observed normal CH(4)/CD(4) kinetic isotope effects are consistent with the kinetic-relevance of C-H bond activation; identical (16)O(2)-(18)O(2) isotopic exchange rates in the presence or

  1. SECTION 4 : BUDGET Remarque : Pour en savoir plus sur les ...

    International Development Research Centre (IDRC) Digital Library (Canada)

    (anonymous)

    SECTION 4 : BUDGET. Remarque : Pour en savoir plus sur les restrictions budgétaires, consulter l'appel à propositions et la foire aux questions. Inscrire toutes les sommes en dollars canadiens. 4.1 Indiquez toutes les dépenses prévues (en CAD). Inscrire une valeur numérique sans caractères, ni espaces, ni virgules (p. ex ...

  2. Study of the properties of plasma of CH4/H2 and its interactions with liquid hydrocarbons

    International Nuclear Information System (INIS)

    Gambus, G.; Patino, P.

    2003-01-01

    Properties of a CH 4 /H 2 plasma, as a reducing agent in heterogeneous reactions with one olefin hydrocarbon, were studied in this work. The characterization of the plasma was carried out by means of optical emission spectroscopy, by varying the gas composition (CH 4 /H 2 ) and the working pressure, in a radio frequency discharge. The variation of the relative populations of H and CH radicals was followed, at pressures between 0.001 and 0.4 mbar and CH 4 /H 2 proportions 1:1 to 1:5. The conditions selected for treating squalene were 0.1 mbar and CH 4 /H 2 of 1:5. Although these conditions did not yield the maximum intensities for the two signals, these were strong enough and black carbon and polymers ceased from being produced under this regime. At 5 C, more than two double bonds per molecule, out of six, were hydrogenated with the plasma in 12 hours. (Author)

  3. Beaver-mediated methane emission: The effects of population growth in Eurasia and the Americas.

    Science.gov (United States)

    Whitfield, Colin J; Baulch, Helen M; Chun, Kwok P; Westbrook, Cherie J

    2015-02-01

    Globally, greenhouse gas budgets are dominated by natural sources, and aquatic ecosystems are a prominent source of methane (CH(4)) to the atmosphere. Beaver (Castor canadensis and Castor fiber) populations have experienced human-driven change, and CH(4) emissions associated with their habitat remain uncertain. This study reports the effect of near extinction and recovery of beavers globally on aquatic CH4 emissions and habitat. Resurgence of native beaver populations and their introduction in other regions accounts for emission of 0.18-0.80 Tg CH(4) year(-1) (year 2000). This flux is approximately 200 times larger than emissions from the same systems (ponds and flowing waters that became ponds) circa 1900. Beaver population recovery was estimated to have led to the creation of 9500-42 000 km(2) of ponded water, and increased riparian interface length of >200 000 km. Continued range expansion and population growth in South America and Europe could further increase CH(4) emissions.

  4. Audit of the global carbon budget: estimate errors and their impact on uptake uncertainty

    Science.gov (United States)

    Ballantyne, A. P.; Andres, R.; Houghton, R.; Stocker, B. D.; Wanninkhof, R.; Anderegg, W.; Cooper, L. A.; DeGrandpre, M.; Tans, P. P.; Miller, J. B.; Alden, C.; White, J. W. C.

    2015-04-01

    Over the last 5 decades monitoring systems have been developed to detect changes in the accumulation of carbon (C) in the atmosphere and ocean; however, our ability to detect changes in the behavior of the global C cycle is still hindered by measurement and estimate errors. Here we present a rigorous and flexible framework for assessing the temporal and spatial components of estimate errors and their impact on uncertainty in net C uptake by the biosphere. We present a novel approach for incorporating temporally correlated random error into the error structure of emission estimates. Based on this approach, we conclude that the 2σ uncertainties of the atmospheric growth rate have decreased from 1.2 Pg C yr-1 in the 1960s to 0.3 Pg C yr-1 in the 2000s due to an expansion of the atmospheric observation network. The 2σ uncertainties in fossil fuel emissions have increased from 0.3 Pg C yr-1 in the 1960s to almost 1.0 Pg C yr-1 during the 2000s due to differences in national reporting errors and differences in energy inventories. Lastly, while land use emissions have remained fairly constant, their errors still remain high and thus their global C uptake uncertainty is not trivial. Currently, the absolute errors in fossil fuel emissions rival the total emissions from land use, highlighting the extent to which fossil fuels dominate the global C budget. Because errors in the atmospheric growth rate have decreased faster than errors in total emissions have increased, a ~20% reduction in the overall uncertainty of net C global uptake has occurred. Given all the major sources of error in the global C budget that we could identify, we are 93% confident that terrestrial C uptake has increased and 97% confident that ocean C uptake has increased over the last 5 decades. Thus, it is clear that arguably one of the most vital ecosystem services currently provided by the biosphere is the continued removal of approximately half of atmospheric CO2 emissions from the atmosphere

  5. Contribution of rice straw carbon to CH4 emission from rice paddies using 13C-enriched rice straw

    Science.gov (United States)

    Watanabe, Akira; Yoshida, Mariko; Kimura, Makoto

    1998-04-01

    It is generally recognized that the application of rice straw (RS) increases CH4 emission from rice paddies. To estimate the contribution of RS carbon to CH4 emission, a pot experiment was conducted using 13C-enriched RS. The percentage contributions of RS carbon to CH4 emission throughout the rice growth period were 10±1, 32±3, and 43±3% for the treatments with RS applied at the rates of 2, 4, and 6 g kg-1 soil, respectively. The increase in the rate of application of RS increased CH4 emission derived from both RS carbon and other carbon sources. The percentage contribution of RS carbon to CH4 emission was larger in the earlier period (maximum 96%) when the decomposition rate of RS was larger. After RS decomposition had slowed, CH4 emission derived from RS carbon decreased. However, the δ13C values of CH4 emitted from the pots with 13C-enriched RS applied at rates of 4 and 6 g kg-1 soil were significantly higher than those from the pots with natural RS until the harvesting stage. An increased atom-13C% of roots of rice plants growing in the pots with 6 g kg-1 of 13C-enriched RS at around the maximum tiller number stage and a decrease during the following 2 months suggested that rice plants assimilated RS carbon once and then released a portion of it. This supply of RS carbon from roots may be one of the sources of CH4 in the late period of rice growth.

  6. SYNTHESIS OF NEW BIS(CYCLOPENTADIENYL)YTTRIUM COMPLEXES WITH ETHER FUNCTIONALIZED CYCLOPENTADIENYL LIGANDS - CRYSTAL-STRUCTURE OF [(C(5)H(4)CH(2)CH(2)OME)(2)Y(MU-H)(2)BH2

    NARCIS (Netherlands)

    LASKE, DA; DUCHATEAU, R; TEUBEN, JH; SPEK, AL

    1993-01-01

    Treatment of C(5)H(4)CH(2)CH(2)OMe.Li(TMEDA) (TMEDA = N, N, N', N' tetramethylethylenediamine) with half an equivalent of YCl3(THF)(3.5) in toluene afforded the salt- and solvent-free dimeric biscyclopentadienyl yttrium chloride [(C(5)H(4)CH(2)CH(2)OMe)(2)Y-(mu-Cl)](2) (1). Reaction of 1 with one

  7. Comprehensive effects of a sedge plant on CH4 and N2O emissions in an estuarine marsh

    Science.gov (United States)

    Li, Yangjie; Wang, Dongqi; Chen, Zhenlou; Hu, Hong

    2018-05-01

    Although there have been numerous studies focusing on plants' roles in methane (CH4) emissions, the influencing mechanism of wetland plants on nitrous oxide (N2O) emissions has rarely been studied. Here, we test whether wetland plants also play an important role in N2O emissions. Gas fluxes were determined using the in situ static flux chamber technique. We also carried out pore-water extractions, sedge removal experiments and tests of N2O transportation. The brackish marsh acted as a net source of both CH4 and N2O. However, sedge plants played the opposite role in CH4 and N2O emissions. The removal of the sedges led to reduced CH4 emissions and increased accumulation of CH4 inside the sediment. Apart from being a conduit for CH4 transport, the sedges made a greater contribution to CH4 oxidation than CH4 production. The sedges exerted inhibitory effects on the release of N2O. The N2O was barely detectable inside the sediment in both vegetated and vegetation-removed plots. The denitrification measurements and nitrogen addition (the addition rates were equal to 0.028, 0.056 and 0.112 g m-2) experiments suggest that denitrification associated with N2O production occurred mainly in the surface sediment layer. The vascular sedge could transport atmospheric N2O downward into the rhizosphere. The rhizospheric sediment, together with the vascular sedge, became an effective sink of atmospheric N2O.

  8. Dissolved organic carbon, CO2, and CH4 concentrations and their stable isotope ratios in thermokarst lakes on the Qinghai-Tibetan Plateau

    Directory of Open Access Journals (Sweden)

    Cuicui Mu

    2016-01-01

    Full Text Available Thermokarst lakes are widely distributed on the Qinghai-Tibetan Plateau (QTP, which accounts for 8% of the global permafrost area. These lakes probably promote organic matter biodegradation and thus accelerate the emission of carbon-based greenhouse gases. However, little is known about greenhouse gas concentrations and their stable isotopes characteristics of these lakes. In this study, we measured the concentrations of dissolved organic carbon (DOC, dissolved CO2 and CH4, as well as the distribution of δ13CCO2, δ13CCH4, and δ13COM (organic matter of lake sediments in thermokarst lakes on the QTP. Results showed that the OM of the lake sediments was highly decomposed. The concentrations of DOC, CO2 and CH4 in the lake water on the QTP were 1.2–49.6 mg L–1, 3.6–45.0 μmol L–1 and 0.28–3.0 μmol L–1, respectively. The highest CO2 and CH4 concentrations were recorded in July while the lowest values in September, which suggested that temperature had an effect on greenhouse gas production, although this pattern may also relate to thermal stratification of the water column. The results implied that thermokast lakes should be paid more attention to regarding carbon cycle and greenhouse gas emissions on the QTP.

  9. Environmental and vegetation controls on the spatial variability of CH4 emission from wet-sedge and tussock tundra ecosystems in the Arctic.

    Science.gov (United States)

    McEwing, Katherine Rose; Fisher, James Paul; Zona, Donatella

    Despite multiple studies investigating the environmental controls on CH 4 fluxes from arctic tundra ecosystems, the high spatial variability of CH 4 emissions is not fully understood. This makes the upscaling of CH 4 fluxes from plot to regional scale, particularly challenging. The goal of this study is to refine our knowledge of the spatial variability and controls on CH 4 emission from tundra ecosystems. CH 4 fluxes were measured in four sites across a variety of wet-sedge and tussock tundra ecosystems in Alaska using chambers and a Los Gatos CO 2 and CH 4 gas analyser. All sites were found to be sources of CH 4 , with northern sites (in Barrow) showing similar CH 4 emission rates to the southernmost site (ca. 300 km south, Ivotuk). Gross primary productivity (GPP), water level and soil temperature were the most important environmental controls on CH 4 emission. Greater vascular plant cover was linked with higher CH 4 emission, but this increased emission with increased vascular plant cover was much higher (86 %) in the drier sites, than the wettest sites (30 %), suggesting that transport and/or substrate availability were crucial limiting factors for CH 4 emission in these tundra ecosystems. Overall, this study provides an increased understanding of the fine scale spatial controls on CH 4 flux, in particular the key role that plant cover and GPP play in enhancing CH 4 emissions from tundra soils.

  10. Intermediate-scale community-level flux of CO2 and CH4 in a Minnesota peatland: putting the SPRUCE project in a global context

    Science.gov (United States)

    P. J. Hanson; A. L. Gill; X. Xu; J. R. Phillips; D. J. Weston; Randy Kolka; J. S. Riggs; L. A. Hook

    2016-01-01

    Peatland measurements of CO2 and CH4 flux were obtained at scales appropriate to the in situ biological community below the tree layer to demonstrate representativeness of the spruce and peatland responses under climatic and environmental change (SPRUCE) experiment. Surface flux measurements were made using dual open-path...

  11. Inverse modelling of European CH4 emissions during 2006-2012 using different inverse models and reassessed atmospheric observations

    Science.gov (United States)

    Bergamaschi, Peter; Karstens, Ute; Manning, Alistair J.; Saunois, Marielle; Tsuruta, Aki; Berchet, Antoine; Vermeulen, Alexander T.; Arnold, Tim; Janssens-Maenhout, Greet; Hammer, Samuel; Levin, Ingeborg; Schmidt, Martina; Ramonet, Michel; Lopez, Morgan; Lavric, Jost; Aalto, Tuula; Chen, Huilin; Feist, Dietrich G.; Gerbig, Christoph; Haszpra, László; Hermansen, Ove; Manca, Giovanni; Moncrieff, John; Meinhardt, Frank; Necki, Jaroslaw; Galkowski, Michal; O'Doherty, Simon; Paramonova, Nina; Scheeren, Hubertus A.; Steinbacher, Martin; Dlugokencky, Ed

    2018-01-01

    We present inverse modelling (top down) estimates of European methane (CH4) emissions for 2006-2012 based on a new quality-controlled and harmonised in situ data set from 18 European atmospheric monitoring stations. We applied an ensemble of seven inverse models and performed four inversion experiments, investigating the impact of different sets of stations and the use of a priori information on emissions. The inverse models infer total CH4 emissions of 26.8 (20.2-29.7) Tg CH4 yr-1 (mean, 10th and 90th percentiles from all inversions) for the EU-28 for 2006-2012 from the four inversion experiments. For comparison, total anthropogenic CH4 emissions reported to UNFCCC (bottom up, based on statistical data and emissions factors) amount to only 21.3 Tg CH4 yr-1 (2006) to 18.8 Tg CH4 yr-1 (2012). A potential explanation for the higher range of top-down estimates compared to bottom-up inventories could be the contribution from natural sources, such as peatlands, wetlands, and wet soils. Based on seven different wetland inventories from the Wetland and Wetland CH4 Inter-comparison of Models Project (WETCHIMP), total wetland emissions of 4.3 (2.3-8.2) Tg CH4 yr-1 from the EU-28 are estimated. The hypothesis of significant natural emissions is supported by the finding that several inverse models yield significant seasonal cycles of derived CH4 emissions with maxima in summer, while anthropogenic CH4 emissions are assumed to have much lower seasonal variability. Taking into account the wetland emissions from the WETCHIMP ensemble, the top-down estimates are broadly consistent with the sum of anthropogenic and natural bottom-up inventories. However, the contribution of natural sources and their regional distribution remain rather uncertain. Furthermore, we investigate potential biases in the inverse models by comparison with regular aircraft profiles at four European sites and with vertical profiles obtained during the Infrastructure for Measurement of the European Carbon

  12. Kinetics of the CH{sub 3} + HCl/DCl {sup {yields}} CH{sub 4}/CH{sub 3}D + Cl and CD{sub 3} + HCl/DCl {sup {yields}} CD{sub 3}H/CD{sub 4} + Cl reactions: An experimental H atom tunneling investigation

    Energy Technology Data Exchange (ETDEWEB)

    Eskola, Arkke J. [Laboratory of Physical Chemistry, P.O. Box 55 (A.I. Virtasen aukio 1), FIN-00014, University of Helsinki, Helsinki (Finland); Seetula, Jorma A. [Laboratory of Physical Chemistry, P.O. Box 55 (A.I. Virtasen aukio 1), FIN-00014, University of Helsinki, Helsinki (Finland)], E-mail: seetula@csc.fi; Timonen, Raimo S. [Laboratory of Physical Chemistry, P.O. Box 55 (A.I. Virtasen aukio 1), FIN-00014, University of Helsinki, Helsinki (Finland)

    2006-12-11

    The kinetics of the radical reactions of CH{sub 3} with HCl or DCl and CD{sub 3} with HCl or DCl have been investigated in a temperature controlled tubular reactor coupled to a photoionization mass spectrometer. The CH{sub 3} (or CD{sub 3}) radical, R, was produced homogeneously in the reactor by a pulsed 193 nm exciplex laser photolysis of CH{sub 3}COCH{sub 3} (or CD{sub 3}COCD{sub 3}). The decay of CH{sub 3}/CD{sub 3} was monitored as a function of HCl/DCl concentration under pseudo-first-order conditions to determine the rate constants as a function of temperature, typically from 188 to 500 K. The rate constants of the CH{sub 3} and CD{sub 3} reactions with HCl had strong non-Arrhenius behavior at low temperatures. The rate constants were fitted to a modified Arrhenius expression k = QA exp (-E {sub a}/RT) (error limits stated are 1{sigma} + Students t values, units in cm{sup 3} molecule{sup -1} s{sup -1}): k(CH{sub 3} + HCl) = [1.004 + 85.64 exp (-0.02438 x T/K)] x (3.3 {+-} 1.3) x 10{sup -13} exp [-(4.8 {+-} 0.6) kJ mol{sup -1}/RT] and k(CD{sub 3} + HCl) = [1.002 + 73.31 exp (-0.02505 x T/K)] x (2.7 {+-} 1.2) x 10{sup -13} exp [-(3.5 {+-} 0.5) kJ mol{sup -1}/RT]. The radical reactions with DCl were studied separately over a wide ranges of temperatures and in these temperature ranges the rate constants determined were fitted to a conventional Arrhenius expression k = A exp (-E {sub a}/RT) (error limits stated are 1{sigma} + Students t values, units in cm{sup 3} molecule{sup -1} s{sup -1}): k(CH{sub 3} + DCl) = (2.4 {+-} 1.6) x 10{sup -13} exp [-(7.8 {+-} 1.4) kJ mol{sup -1}/RT] and k(CD{sub 3} + DCl) = (1.2 {+-} 0.4) x 10{sup -13} exp [-(5.2 {+-} 0.2) kJ mol{sup -1}/RT] cm{sup 3} molecule{sup -1} s{sup -1}. Curvature in the Arrhenius plots of the H-atom abstraction reactions at low temperatures was analyzed by considering H-atom tunneling through the reaction barrier and primary kinetic isotope effect. Contribution of tunneling in it was concluded to be

  13. In-operando elucidation of bimetallic CoNi nanoparticles during high-temperature CH 4 /CO 2 reaction

    KAUST Repository

    Al-Sabban, Bedour E.; Falivene, Laura; Kozlov, Sergey M.; Aguilar Tapia, Antonio; Ould-Chikh, Samy; Hazemann, Jean-Louis; Cavallo, Luigi; Basset, Jean-Marie; Takanabe, Kazuhiro

    2017-01-01

    Dry reforming of methane (DRM) proceeds via CH4 decomposition to leave surface carbon species, followed by their removal with CO2-derived species. Reactivity tuning for stoichiometric CH4/CO2 reactants was attempted by alloying the non-noble metals

  14. Improving accuracy and precision of ice core δD(CH4 analyses using methane pre-pyrolysis and hydrogen post-pyrolysis trapping and subsequent chromatographic separation

    Directory of Open Access Journals (Sweden)

    M. Bock

    2014-07-01

    Full Text Available Firn and polar ice cores offer the only direct palaeoatmospheric archive. Analyses of past greenhouse gas concentrations and their isotopic compositions in air bubbles in the ice can help to constrain changes in global biogeochemical cycles in the past. For the analysis of the hydrogen isotopic composition of methane (δD(CH4 or δ2H(CH4 0.5 to 1.5 kg of ice was hitherto used. Here we present a method to improve precision and reduce the sample amount for δD(CH4 measurements in (ice core air. Pre-concentrated methane is focused in front of a high temperature oven (pre-pyrolysis trapping, and molecular hydrogen formed by pyrolysis is trapped afterwards (post-pyrolysis trapping, both on a carbon-PLOT capillary at −196 °C. Argon, oxygen, nitrogen, carbon monoxide, unpyrolysed methane and krypton are trapped together with H2 and must be separated using a second short, cooled chromatographic column to ensure accurate results. Pre- and post-pyrolysis trapping largely removes the isotopic fractionation induced during chromatographic separation and results in a narrow peak in the mass spectrometer. Air standards can be measured with a precision better than 1‰. For polar ice samples from glacial periods, we estimate a precision of 2.3‰ for 350 g of ice (or roughly 30 mL – at standard temperature and pressure (STP – of air with 350 ppb of methane. This corresponds to recent tropospheric air samples (about 1900 ppb CH4 of about 6 mL (STP or about 500 pmol of pure CH4.

  15. Effects of Long-Term CO2 Enrichment on Soil-Atmosphere CH4 Fluxes and the Spatial Micro-Distribution of Methanotrophic Bacteria.

    Science.gov (United States)

    Karbin, Saeed; Guillet, Cécile; Kammann, Claudia I; Niklaus, Pascal A

    2015-01-01

    Effects of elevated atmospheric CO2 concentrations on plant growth and associated C cycling have intensively been studied, but less is known about effects on the fluxes of radiatively active trace gases other than CO2. Net soil-atmosphere CH4 fluxes are determined by the balance of soil microbially-driven methane (CH4) oxidation and methanogenesis, and both might change under elevated CO2. Here, we studied CH4 dynamics in a permanent grassland exposed to elevated CO2 for 14 years. Soil-atmosphere fluxes of CH4 were measured using large static chambers, over a period of four years. The ecosystem was a net sink for atmospheric CH4 for most of the time except summer to fall when net CH4 emissions occurred. We did not detect any elevated CO2 effects on CH4 fluxes, but emissions were difficult to quantify due to their discontinuous nature, most likely because of ebullition from the saturated zone. Potential methanotrophic activity, determined by incubation of fresh sieved soil under standardized conditions, also did not reveal any effect of the CO2 treatment. Finally, we determined the spatial micro-distribution of methanotrophic activity at less than 5× atmospheric (10 ppm) and elevated (10000 ppm) CH4 concentrations, using a novel auto-radiographic technique. These analyses indicated that domains of net CH4 assimilation were distributed throughout the analyzed top 15 cm of soils, with no dependence on CH4 concentration or CO2 treatment. Our investigations suggest that elevated CO2 exerts no or only minor effects on CH4 fluxes in the type of ecosystem we studied, at least as long as soil moisture differences are small or absent as was the case here. The autoradiographic analyses further indicate that the spatial niche of CH4 oxidation does not shift in response to CO2 enrichment or CH4 concentration, and that the same type of methanotrophs may oxidize CH4 from atmospheric and soil-internal sources.

  16. Forecasting the future reimbursement system of Korean National Health Insurance: a contemplation focusing on global budget and Neo-KDRG-based payment systems.

    Science.gov (United States)

    Kim, Yang-Kyun

    2012-05-01

    With the adoption of national health insurance in 1977, Korea has been utilizing fee-for-service payment with contract-based healthcare reimbursement system in 2000. Under the system, fee-for-service reimbursement has been accused of augmenting national healthcare expenditure by excessively increasing service volume. The researcher examined in this paper two major alternatives including diagnosis related group-based payment and global budget to contemplate the future of reimbursement system of Korean national health insurance. Various literature and preceding studies on pilot project and actual implementation of Neo-KDRG were reviewed. As a result, DRG-based payment was effective for healthcare cost control but low in administrative efficiency. Global budget may be adequate for cost control and improving the quality of healthcare and administrative efficiency. However, many healthcare providers disagree that excess care arising from fee-for-service payment alone has led to financial deterioration of national health insurance and healthcare institutions should take responsibility with global budget payment as an appropriate solution. Dissimilar payment systems may be applied to different types of institutions to reflect their unique attributes, and this process can be achieved step-by-step. Developing public sphere among the stakeholders and striving for consensus shall be kept as collateral to attain the desirable reimbursement system in the future.

  17. Spatial and Temporal Variations in the Partial Pressure and Emission of CO2 and CH4 in and Amazon Floodplain Lake

    Science.gov (United States)

    Forsberg, B. R.; Amaral, J. H.; Barbosa, P.; Kasper, D.; MacIntyre, S.; Cortes, A.; Sarmento, H.; Borges, A. V.; Melack, J. M.; Farjalla, V.

    2015-12-01

    The Amazon floodplain contains a variety of wetland environments which contribute CO2 and CH4 to the regional and global atmospheres. The partial pressure and emission of these greenhouse gases (GHGs) varies: 1) between habitats, 2) seasonally, as the characteristics these habitats changes and 3) diurnally, in response to diurnal stratification. In this study, we investigated the combined influence of these factors on the partial pressure and emission of GHGs in Lago Janauacá, a central Amazon floodplain lake (3o23' S; 60o18' O). All measurements were made between August of 2014 and April of 2015 at two different sites and in three distinct habitats: open water, flooded forest, flooded macrophytes. Concentrations of CO2 and CH4 in air were measured continuously with a cavity enhanced absorption spectrometer, Los Gatos Research´s Ultraportable Greenhouse Gas Analyzer (UGGA). Vertical profiles o pCO2 and pCH4 were measured using the UGGA connected to an electric pump and equilibrator. Diffusive surface emissions were estimated with the UGGA connected to a static floating chamber. To investigate the influence of vertical stratification and mixing on GHG partial pressure and emissions, a meteorological station and submersible sensor chain were deployed at each site. Meteorological sensors included wind speed and direction. The submersible chains included thermistors and oxygen sensors. Depth profiles of partial pressure and diffusive emissions for both CO2 and CH4 varied diurnally, seasonally and between habitats. Both pCO2 and pCH4 were consistently higher in bottom than surface waters with the largest differences occurring at high water when thermal stratification was most stable. Methane emissions and partial pressures were highest at low water while pCO2 and CO2 fluxes were highest during high water periods, with 35% of CO2 fluxes at low water being negative. The highest average surface value of pCO2 (5491 μatm), encountered during rising water, was ~3 times

  18. Global Carbon Budget 2016

    NARCIS (Netherlands)

    Quéré, Le Corinne; Andrew, Robbie M.; Canadell, Josep G.; Sitch, Stephen; Korsbakken, Jan Ivar; Peters, Glen P.; Manning, Andrew C.; Boden, Thomas A.; Tans, Pieter P.; Houghton, Richard A.; Keeling, Ralph F.; Alin, Simone; Andrews, Oliver D.; Anthoni, Peter; Barbero, Leticia; Bopp, Laurent; Chevallier, Frédéric; Chini, Louise P.; Ciais, Philippe; Currie, Kim; Delire, Christine; Doney, Scott C.; Friedlingstein, Pierre; Gkritzalis, Thanos; Harris, Ian; Hauck, Judith; Haverd, Vanessa; Hoppema, Mario; Klein Goldewijk, Kees; Jain, Atul K.; Kato, Etsushi; Körtzinger, Arne; Landschützer, Peter; Lefèvre, Nathalie; Lenton, Andrew; Lienert, Sebastian; Lombardozzi, Danica; Melton, Joe R.; Metzl, Nicolas; Millero, Frank; Monteiro, Pedro M.S.; Munro, David R.; Nabel, Julia E.M.S.; Nakaoka, S.; O'Brien, Kevin; Olsen, Are; Omar, Abdirahman M.; Ono, Tsuneo; Pierrot, Denis; Poulter, Benjamin; Rödenbeck, Christian; Salisbury, Joe; Schuster, Ute; Schwinger, Jörg; Séférian, Roland; Skjelvan, Ingunn; Stocker, Benjamin D.; Sutton, Adrienne J.; Takahashi, Taro; Tian, Hanqin; Tilbrook, Bronte; Laan-Luijkx, van der Ingrid T.; Werf, van der Guido R.; Viovy, Nicolas; Walker, Anthony P.; Wiltshire, Andrew J.; Zaehle, Sönke

    2016-01-01

    Accurate assessment of anthropogenic carbon dioxide (CO2) emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere – the “global carbon budget” – is important to better understand the global carbon cycle, support the development of climate policies, and project

  19. Tidal influence on the sea-to-air transfer of CH4 in the coastal ocean

    International Nuclear Information System (INIS)

    Hahm, Doshik; Kim, Guebuem; Lee, Yong-Woo; Nam, Sungh-Yun; Kim, Kyung-Ryul; Kim, Kuh

    2006-01-01

    We obtained real-time monitoring data of water temperature, salinity, wind, current, CH 4 and other oceanographic parameters in a coastal bay in the southern sea of Korea from July 8 to August 15, 2003, using an environmental monitoring buoy. In general, the transfer velocity of environmental gases across the air-sea interface is obtained exclusively from empirical relationships with wind speeds. However, our monitoring data demonstrate that the agitation of the aqueous boundary layer is controlled significantly by tidal turbulence, similar to the control exercised by wind stress in the coastal ocean. The sea-to-air transfer of CH 4 is enhanced significantly during spring tide due to an increase in the gas transfer velocity and vertical CH 4 transport from bottom water to the surface layer. Thus, our unique time-series results imply that the sea-to-air transfer of gases, such as CH 4 , DMS, DMHg, N 2 O, CO 2 and 222 Rn, from highly enriched coastal bottom waters, is controlled not only by episodic wind events but also by regular tidal turbulence in the coastal ocean

  20. Dual stable isotopes of CH 4 from Yellowstone hot-springs suggest hydrothermal processes involving magmatic CO 2

    Energy Technology Data Exchange (ETDEWEB)

    Moran, James J.; Whitmore, Laura M.; Jay, Zackary J.; Jennings, Ryan deM.; Beam, Jacob P.; Kreuzer, Helen W.; Inskeep, William P.

    2017-07-01

    Volcanism and post-magmatism contribute both significant annual CH4 fluxes to the atmosphere (on par with other natural sources such as forest fire and wild animal emissions) and have been implicated in past climate-change events. The Yellowstone hot spot is one of the largest volcanic systems on Earth and is known to emit methane in addition to other greenhouse gases (e.g. carbon dioxide) but the ultimate source of this methane flux has not been elucidated. Here we use dual stable isotope analysis (δ2H and δ13C) of CH4(g) sampled from ten high-temperature geothermal pools in Yellowstone National Park to show that the predominant flux of CH4(g) is abiotic. The average δ13C and δ2H values of CH4(g) emitted from hot springs (-26.7 (±2.4) and -236.9 (±12.0) ‰, respectively) are not consistent with biotic (microbial or thermogenic) methane sources, but are within previously reported ranges for abiotic methane production. Correlation between δ13CCH4 and δ13C-dissolved inorganic C (DIC) also suggests that CO2 is a parent C source for the observed CH4(g). Moreover, CH4-CO2 isotopic geothermometry was used to estimate CH4(g) formation temperatures ranging from ~ 250 - 350°C, which is just below the temperature estimated for the hydrothermal reservoir and consistent with the hypothesis that subsurface, rock-water interactions are responsible for large methane fluxes from this volcanic system. An understanding of conditions leading to the abiotic production of methane and associated isotopic signatures are central to understanding the evolutionary history of deep carbon sources on Earth.

  1. Raman spectroscopic characterization of CH4 density over a wide range of temperature and pressure

    Science.gov (United States)

    Shang, Linbo; Chou, I-Ming; Burruss, Robert; Hu, Ruizhong; Bi, Xianwu

    2014-01-01

    The positions of the CH4 Raman ν1 symmetric stretching bands were measured in a wide range of temperature (from −180 °C to 350 °C) and density (up to 0.45 g/cm3) using high-pressure optical cell and fused silica capillary capsule. The results show that the Raman band shift is a function of both methane density and temperature; the band shifts to lower wavenumbers as the density increases and the temperature decreases. An equation representing the observed relationship among the CH4 ν1 band position, temperature, and density can be used to calculate the density in natural or synthetic CH4-bearing inclusions.

  2. Ion irradiation of CH4-containing icy mixtures

    International Nuclear Information System (INIS)

    Baratta, G.A.; Domingo, M.; Ferini, G.; Leto, G.; Palumbo, M.E.; Satorre, M.A.; Strazzulla, G.

    2003-01-01

    We have studied by infrared absorption spectroscopy the effects of ion irradiation with 60 keV Ar 2+ ions on pure methane (CH 4 ) ice at 12 K and mixtures with water (H 2 O) and nitrogen (N 2 ). Ion irradiation, among other effects, causes the rupture of original molecular bonds and the formation of molecular species not present in the initial ice. Here we present the experimental results and discuss their astrophysical relevance

  3. Quantifying the Variability of CH4 Emissions from Pan-Arctic Lakes with Lake Biogeochemical and Landscape Evolution Models

    Science.gov (United States)

    Tan, Z.; Zhuang, Q.

    2014-12-01

    Recent studies in the arctic and subarctic show that CH4 emissions from pan-arctic lakes are playing much more significant roles in the regional carbon cycling than previously estimated. Permafrost thawing due to pronounced warming at northern high latitudes affects lake morphology, changing its CH4 emissions. Thermokarst can enlarge the extent of artic lakes, exposing stable ancient carbon buried in the permafrost zone for degradation and changing a previously known carbon sink to a large carbon source. In some areas, the thawing of subarctic discontinuous and isolated permafrost can diminish thermokarst lakes. To date, few models have considered these important hydrological and biogeochemical processes to provide adequate estimation of CH4 emissions from these lakes. To fill this gap, we have developed a process-based climate-sensitive lake biogeochemical model and a landscape evolution model, which have been applied to quantify the state and variability of CH4 emissions from this freshwater system. Site-level experiments show the models are capable to capture the spatial and temporal variability of CH4 emissions from lakes across Siberia and Alaska. With the lake biogeochemical model solely, we estimate that the magnitude of CH4 emissions from lakes is 13.2 Tg yr-1 in the north of 60 ºN at present, which is on the same order of CH4 emissions from northern high-latitude wetlands. The maximum increment is 11.8 Tg CH4 yr-1 by the end of the 21st century when the worst warming scenario is assumed. We expect the landscape evolution model will improve the existing estimates.

  4. Global atmospheric chemistry – which air matters

    Directory of Open Access Journals (Sweden)

    M. J. Prather

    2017-07-01

    Full Text Available An approach for analysis and modeling of global atmospheric chemistry is developed for application to measurements that provide a tropospheric climatology of those heterogeneously distributed, reactive species that control the loss of methane and the production and loss of ozone. We identify key species (e.g., O3, NOx, HNO3, HNO4, C2H3NO5, H2O, HOOH, CH3OOH, HCHO, CO, CH4, C2H6, acetaldehyde, acetone and presume that they can be measured simultaneously in air parcels on the scale of a few km horizontally and a few tenths of a km vertically. As a first step, six global models have prepared such climatologies sampled at the modeled resolution for August with emphasis on the vast central Pacific Ocean basin. Objectives of this paper are to identify and characterize differences in model-generated reactivities as well as species covariances that could readily be discriminated with an unbiased climatology. A primary tool is comparison of multidimensional probability densities of key species weighted by the mass of such parcels or frequency of occurrence as well as by the reactivity of the parcels with respect to methane and ozone. The reactivity-weighted probabilities tell us which parcels matter in this case, and this method shows skill in differentiating among the models' chemistry. Testing 100 km scale models with 2 km measurements using these tools also addresses a core question about model resolution and whether fine-scale atmospheric structures matter to the overall ozone and methane budget. A new method enabling these six global chemistry–climate models to ingest an externally sourced climatology and then compute air parcel reactivity is demonstrated. Such an objective climatology containing these key species is anticipated from the NASA Atmospheric Tomography (ATom aircraft mission (2015–2020, executing profiles over the Pacific and Atlantic Ocean basins. This modeling study addresses a core part of the design of ATom.

  5. CH4 fluxes across the seafloor at three district gas hydrate fields: Impacts on ocean and atmosphere chemistry

    Energy Technology Data Exchange (ETDEWEB)

    Kastner, M.; Bartlett, D.; MacDonald, I.; Solomon, E.

    2005-07-01

    The role of methane hydrate in the global methane budget is poorly documented because relatively little is known about the transport of methane through the seafloor into the ocean and atmosphere, and the extent of en route water-column methanotrophy. Pore fluids and water column samples within and adjacent to methane plumes were analyzed for methane, dissolved inorganic C (DIC), sulfide/sulfate, alkalinity, and major element concentrations, and for delta{sup 13}C-CH4 and DIC, at three distinct gas hydrate environments. The three environments are: Bush Hill (BH) in the northern Gulf of Mexico (GOM), Eel River (ER) offshore Northern California, and North and South Hydrate Ridges (HR), Cascadia, Oregon margin. The methane source at these sites ranges from mostly thermogenic at GOM to primarily biogenic at HR. At these three distinct gas hydrate environments, at all the sites a significant enrichment in {sup 13}C-CH4 along isopycnals away from the methane plumes is observed, indicating extensive aerobic bacterial methane oxidation in the water column, and correspondingly of oxygen consumption. This is principally pronounced in the mostly biogenic methane setting. The delta{sup 13}C-CH4 values range from approx. 12 to -67 , PDB, at the Hydrate Ridges, from approx. 34 to -52 at Eel River, and from approx. 41 to -67 at Bush Hill. The large variation in methane C isotope ranges between the sites suggests that major differences exist in both the rates of aerobic methane oxidation and system openness at the studied locations. Methane fluxes across the sediment/seawater interface were measured, with a flux meter, MOSQUITO (Multiple Orifice Sampler and Quantitative Injection Tracer Observers) only at BH (Solomon et al., 2005). Water column methane concentrations are on average lower at HR than at ER and GOM. Preliminary estimates suggests that aerobic oxidation is nearly complete, consumes most to all of the water column methane at HR, but at the GOM only approx. 80% to a

  6. Adsorption of CH4 on nitrogen- and boron-containing carbon models of coal predicted by density-functional theory

    Science.gov (United States)

    Liu, Xiao-Qiang; Xue, Ying; Tian, Zhi-Yue; Mo, Jing-Jing; Qiu, Nian-Xiang; Chu, Wei; Xie, He-Ping

    2013-11-01

    Graphene doped by nitrogen (N) and/or boron (B) is used to represent the surface models of coal with the structural heterogeneity. Through the density functional theory (DFT) calculations, the interactions between coalbed methane (CBM) and coal surfaces have been investigated. Several adsorption sites and orientations of methane (CH4) on graphenes were systematically considered. Our calculations predicted adsorption energies of CH4 on graphenes of up to -0.179 eV, with the strongest binding mode in which three hydrogen atoms of CH4 direct to graphene surface, observed for N-doped graphene, compared to the perfect (-0.154 eV), B-doped (-0.150 eV), and NB-doped graphenes (-0.170 eV). Doping N in graphene increases the adsorption energies of CH4, but slightly reduced binding is found when graphene is doped by B. Our results indicate that all of graphenes act as the role of a weak electron acceptor with respect to CH4. The interactions between CH4 and graphenes are the physical adsorption and slightly depend upon the adsorption sites on graphenes and the orientations of methane as well as the electronegativity of dopant atoms in graphene.

  7. Modified ZIF-8 mixed matrix membrane for CO2/CH4 separation

    Science.gov (United States)

    Nordin, Nik Abdul Hadi Md; Ismail, Ahmad Fauzi; Misdan, Nurasyikin; Nazri, Noor Aina Mohd

    2017-10-01

    Tunability of metal-organic frameworks (MOFs) properties enables them to be tailored for specific applications. In this study, zeolitic imidazole framework 8 (ZIF-8), sub-class of MOF, underwent pre-synthesis and post-synthesis modifications. The pre-synthesis modification using GO (ZIF-8/GO) shows slight decrease in textural properties, while the post-synthesis modification using amine solution (ZIF-8/NH2) resulted in superior BET surface area and pore volume. Mixed matrix membranes (MMMs) derived from polysulfone (PSf) and the modified ZIF-8s were then prepared via dry/wet phase inversion. The polymer chain flexibility of the resulted MMMs shows rigidification, where ZIF-8/NH2 as filler resulting higher rigidification compared to ZIF-8/GO. The MMMs were further subjected to pure CO2 and CH4 gas permeation experiments. The PSf/ZIF-8/NH2 shows superior CO2/CH4 selectivity (88% increased) while sacrificing CO2 permeance due to combination of severe polymer chain rigidification and the presence of CO2-philic group, amine. Whereas, the PSf/ZIF-8/GO possess 64% increase in CO2 permeance without notable changes in CO2/CH4 selectivity.

  8. Plant-mediated CH4 transport and C gas dynamics quantified in-situ in a Phalaris arundinacea-dominant wetland

    DEFF Research Database (Denmark)

    Jensen, Louise Askær; Elberling, Bo; Friborg, Thomas

    2011-01-01

    passive. Thus, diurnal variations are less important in contrast to wetland vascular plants facilitating convective gas flow. Despite of plant-dominant CH4 transport, net CH4 fluxes were low (–0.005–0.016 µmol m-2 s-1) and annually less than 1% of the annual C-CO2 assimilation. This is considered a result......±35% of ecosystem CH4 emissions were plant-mediated, but data show no evidence of significant diurnal variations related to convective gas flow regardless of season or plant growth stages. Therefore, despite a high percentage of arenchyma, P. arundinacea-mediated CH4 transport is interpreted to be predominantly...

  9. The cost of pipelining climate change mitigation. An overview of the economics of CH4, CO2 and H2 transportation

    Energy Technology Data Exchange (ETDEWEB)

    Van der Zwaan, B.C.C.; Schoots, K.; Rivera-Tinoco, R. [Energy research Center of the Netherlands (ECN), Policy Studies Department, Amsterdam (Netherlands); Verbong, G.P.J. [Eindhoven University of Technology, Department of Industrial Engineering and Innovation Sciences, Eindhoven (Netherlands)

    2011-11-15

    Gases like CH4, CO2 and H2 may play a key role in establishing a sustainable energy system: CH4 is the least carbon-intensive fossil energy resource; CO2 capture and storage can significantly reduce the climate footprint of especially fossil-based electricity generation; and the use of H2 as energy carrier could enable carbon-free automotive transportation. Yet the construction of large pipeline infrastructures usually constitutes a major and time-consuming undertaking, because of safety and environmental issues, legal and (geo)political siting arguments, technically untrivial installation processes, and/or high investment cost requirements. In this article we focus on the latter and present an overview of both the total costs and cost components of the distribution of these three gases via pipelines. Possible intricacies and external factors that strongly influence these costs, like the choice of location and terrain, are also included in our analysis. Our distribution cost breakdown estimates are based on transportation data for CH4, which we adjust for CO2 and H2 in order to account for the specific additional characteristics of these two gases. The overall trend is that pipeline construction is no longer subject to significant cost reductions. For the purpose of designing energy and climate policy we therefore know in principle with reasonable certainty what the minimum distribution cost components of future energy systems are that rely on pipelining these gases. We describe the reasons why we observe limited learning-by-doing and explain why negligible construction cost reductions for future CH4, CO2 and H2 pipeline projects can be expected. Cost data of individual pipeline projects may strongly deviate from the global average because of national or regional effects related to the type of terrain, but also to varying costs of labor and fluctuating market prices of components like steel.

  10. Thermodynamic activity of saturated solutions of CsClO4 in ethylene glycol and its analogs of the HOCH2(CH2CH2O)nCH2OH series

    International Nuclear Information System (INIS)

    Krasnoperova, A.P.; Ivanova, E.F.; Kijko, S.M.; Yukhno, G.D.

    1997-01-01

    Solubility of CsClO 4 in ethylene glycol, diethylene glycol, triethylene glycol, tetraethylene glycol, polyethylene glycols with molar mass 300 and 400 in the temperature range of 273.15-318.15 K has been ascertained by the method of radioactive indicators. Dependence of saturated solutions activity on temperature, dielectric permittivity and the number of (CH 2 CH 2 O) ether groups in glycols is discussed

  11. Entropy budget of the earth,atmosphere and ocean system

    Institute of Scientific and Technical Information of China (English)

    GAN Zijun; YAN Youfangand; QI Yiquan

    2004-01-01

    The energy budget in the system of the earth, atmosphere and ocean conforms to the first law of thermodynamics, namely the law of conservation of energy, and it is balanced when the system is in a steady-state condition. However, the entropy budget following the second law of thermodynamics is unbalanced. In this paper, we deduce the expressions of entropy flux and re-estimate the earth, atmosphere and ocean annual mean entropy budget with the updated climatologically global mean energy budget and the climatologically air-sea flux data. The calculated results show that the earth system obtains a net influx of negative entropy (-1179.3 mWm-2K-1) from its surroundings, and the atmosphere and the ocean systems obtain a net input of negative entropy at about -537.4 mWm-2K-1 and -555.6 mWm-2K-1, respectively. Calculations of the entropy budget can provide some guidance for further understanding the spatial-temporal change of the local entropy flux, and the entropy production resulting from all kinds of irreversible processes inside these systems.

  12. Global model simulations of the impact of ocean-going ships on aerosols, clouds, and the radiation budget

    Directory of Open Access Journals (Sweden)

    A. Lauer

    2007-10-01

    Full Text Available International shipping contributes significantly to the fuel consumption of all transport related activities. Specific emissions of pollutants such as sulfur dioxide (SO2 per kg of fuel emitted are higher than for road transport or aviation. Besides gaseous pollutants, ships also emit various types of particulate matter. The aerosol impacts the Earth's radiation budget directly by scattering and absorbing the solar and thermal radiation and indirectly by changing cloud properties. Here we use ECHAM5/MESSy1-MADE, a global climate model with detailed aerosol and cloud microphysics to study the climate impacts of international shipping. The simulations show that emissions from ships significantly increase the cloud droplet number concentration of low marine water clouds by up to 5% to 30% depending on the ship emission inventory and the geographic region. Whereas the cloud liquid water content remains nearly unchanged in these simulations, effective radii of cloud droplets decrease, leading to cloud optical thickness increase of up to 5–10%. The sensitivity of the results is estimated by using three different emission inventories for present-day conditions. The sensitivity analysis reveals that shipping contributes to 2.3% to 3.6% of the total sulfate burden and 0.4% to 1.4% to the total black carbon burden in the year 2000 on the global mean. In addition to changes in aerosol chemical composition, shipping increases the aerosol number concentration, e.g. up to 25% in the size range of the accumulation mode (typically >0.1 μm over the Atlantic. The total aerosol optical thickness over the Indian Ocean, the Gulf of Mexico and the Northeastern Pacific increases by up to 8–10% depending on the emission inventory. Changes in aerosol optical thickness caused by shipping induced modification of aerosol particle number concentration and chemical composition lead to a change in the shortwave radiation budget at the top of the

  13. WRF-Chem simulations in the Amazon region during wet and dry season transitions: evaluation of methane models and wetland inundation maps

    Science.gov (United States)

    Beck, V.; Gerbig, C.; Koch, T.; Bela, M. M.; Longo, K. M.; Freitas, S. R.; Kaplan, J. O.; Prigent, C.; Bergamaschi, P.; Heimann, M.

    2013-08-01

    The Amazon region, being a large source of methane (CH4), contributes significantly to the global annual CH4 budget. For the first time, a forward and inverse modelling framework on regional scale for the purpose of assessing the CH4 budget of the Amazon region is implemented. Here, we present forward simulations of CH4 as part of the forward and inverse modelling framework based on a modified version of the Weather Research and Forecasting model with chemistry that allows for passive tracer transport of CH4, carbon monoxide, and carbon dioxide (WRF-GHG), in combination with two different process-based bottom-up models of CH4 emissions from anaerobic microbial production in wetlands and additional datasets prescribing CH4 emissions from other sources such as biomass burning, termites, or other anthropogenic emissions. We compare WRF-GHG simulations on 10 km horizontal resolution to flask and continuous CH4 observations obtained during two airborne measurement campaigns within the Balanço Atmosférico Regional de Carbono na Amazônia (BARCA) project in November 2008 and May 2009. In addition, three different wetland inundation maps, prescribing the fraction of inundated area per grid cell, are evaluated. Our results indicate that the wetland inundation maps based on remote-sensing data represent the observations best except for the northern part of the Amazon basin and the Manaus area. WRF-GHG was able to represent the observed CH4 mixing ratios best at days with less convective activity. After adjusting wetland emissions to match the averaged observed mixing ratios of flights with little convective activity, the monthly CH4 budget for the Amazon basin obtained from four different simulations ranges from 1.5 to 4.8 Tg for November 2008 and from 1.3 to 5.5 Tg for May 2009. This corresponds to an average CH4 flux of 9-31 mg m-2 d-1 for November 2008 and 8-36 mg m-2 d-1 for May 2009.

  14. Effects of Climate Change and Organic Matter Amendments on the Fate of Soil Carbon and the Global Warming Potential of CO2, CH4, and N2O Emissions in an Upland Soil

    Science.gov (United States)

    Simmonds, M.; Muehe, E. M.; Fendorf, S. E.

    2017-12-01

    Our current understanding of the mechanisms driving carbon stabilization in soil organic matter (SOM) and its release to the atmosphere is insufficient for predicting the response of soil carbon dynamics to future climatic conditions. The persistence of SOM has been studied primarily within the context of biochemical, physical, and geochemical protection from decomposition. More recently, bioenergetic constraints on SOM decomposition due to oxygen limitations have been demonstrated in submerged soils. However, the relevance of anaerobic domains in upland soils is uncertain. To better understand how upland soils will respond to climate change, we conducted a 52-day incubation of an upland soil at constant soil moisture (field capacity) under varying air temperatures (32°C and 37°C), CO2 concentrations (398 and 850 ppmv), and soil organic carbon contents (1.3%, 2.4%). Overall, we observed a stimulatory effect of future climate (elevated temperature and CO2) and higher carbon inputs on net SOM mineralization rates (higher CO2, CH4 and N2O emissions). Importantly, CH4 emissions were observed in the soils with added plant residue, indicating anaerobic microsites are relevant in upland soils, and significantly impact microbial respiration pathways, rates of SOM mineralization, and the global warming potential of trace gas emissions. These findings have important implications for positive soil carbon-climate feedbacks, and warrant further investigation into representing anaerobic soil domains of upland soils in biogeochemical models.

  15. Flux and distribution of methane (CH4) in the Gunsan Basin of the southeastern Yellow Sea, off the Western Korea.

    Science.gov (United States)

    Lee, Jun-Ho; Woo, Han Jun; Son, Seung-Kyu; Kim, Moonkoo; Lee, Dong-Hun; Tsunogai, Urumu; Jeong, Kap-Sik

    2018-04-16

    The flux and distribution of methane (CH 4 ) was investigated in the seawater column at 14 stations in the Gunsan Basin, the southeastern part of Yellow Sea from 2013 to 2015. Here CH 4 is concentrated 2.4-4.7 (3.4 ± 0.7) nM in the surface and 2.5-7.4 (5.2 ± 1.7) nM in the bottom layer. The CH 4 saturation ratios ranged from 65.5% to 295.5% (162.6 ± 68.7), comprising the mean sea-to-air CH 4 flux of 3.8 to 25.3 (15.6 ± 5.5) µM m -2 d -1 . Methane concentration was largely different in the upper and the lower seawater layers that is separated by the thermocline of which depth is variable (20-60 m) depending on the time of sampling. The concentration of seawater dissolved CH 4 is high between the bottom surface of the thermocline layer and the sea floor. Generally it tends to decrease from the south-westernmost part of the basin toward the west coast of Korea. This distribution pattern of CH 4 seems to result from the CH 4 supply by decomposition of organic matters produced in the upper seawater layer that is superimposed by the larger supply from the underlying sediment layer especially beneath the thermocline. The latter is manifested by ubiquitous CH 4 seeps from the seafloor sediments.

  16. In-operando elucidation of bimetallic CoNi nanoparticles during high-temperature CH 4 /CO 2 reaction

    KAUST Repository

    Al-Sabban, Bedour

    2017-05-02

    Dry reforming of methane (DRM) proceeds via CH4 decomposition to leave surface carbon species, followed by their removal with CO2-derived species. Reactivity tuning for stoichiometric CH4/CO2 reactants was attempted by alloying the non-noble metals Co and Ni, which have high affinity with CO2 and high activity for CH4 decomposition, respectively. This study was focused on providing evidence of the capturing surface coverage of the reactive intermediates and the associated structural changes of the metals during DRM at high temperature using in-operando X-ray absorption spectroscopy (XAS). On the Co catalysts, the first-order effects with respect to CH4 pressure and negative-order effects with respect to CO2 pressure on the DRM rate are consistent with the competitive adsorption of the surface oxygen species on the same sites as the CH4 decomposition reaction. The Ni surface provides comparatively higher rates of CH4 decomposition and the resultant DRM than the Co catalyst but leaves some deposited carbon on the catalyst surface. In contrast, the bimetallic CoNi catalyst exhibits reactivity towards the DRM but with kinetic orders resembling Co catalyst, producing negligible carbon deposition by balancing CH4 and CO2 activation. The in-operando X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) measurements confirmed that the Co catalyst was progressively oxidized from the surface to the bulk with reaction time, whereas CoNi and Ni remained relatively reduced during DRM. Density functional theory (DFT) calculation considering the high reaction temperature for DRM confirmed the unselective site arrangement between Co and Ni atoms in both the surface and bulk of the alloy nanoparticle (NP). The calculated heat of oxygen chemisorption became more exothermic in the order of Ni, CoNi, Co, consistent with the catalytic behavior. The comprehensive experimental and theoretical evidence provided herein clearly suggests

  17. Selective Generation of the Radical Cation Isomers [CH3CN](•+) and [CH2CNH](•+) via VUV Photoionization of Different Neutral Precursors and Their Reactivity with C2H4.

    Science.gov (United States)

    Polášek, Miroslav; Zins, Emilie-Laure; Alcaraz, Christian; Žabka, Ján; Křížová, Věra; Giacomozzi, Linda; Tosi, Paolo; Ascenzi, Daniela

    2016-07-14

    Experimental and theoretical studies have been carried out to demonstrate the selective generation of two different C2H3N(+) isomers, namely, the acetonitrile [CH3CN](•+) and the ketenimine [CH2CNH](•+) radical cations. Photoionization and dissociative photoionization experiments from different neutral precursors (acetonitrile and butanenitrile) have been performed using vacuum ultraviolet (VUV) synchrotron radiation in the 10-15 eV energy range, delivered by the DESIRS beamline at the SOLEIL storage ring. For butanenitrile (CH3CH2CH2CN) an experimental ionization threshold of 11.29 ± 0.05 eV is obtained, whereas the appearance energy for the formation of [CH2CNH](•+) fragments is 11.52 ± 0.05 eV. Experimental findings are fully supported by theoretical calculations at the G4 level of theory (ZPVE corrected energies at 0 K), giving a value of 11.33 eV for the adiabatic ionization energy of butanenitrile and an exothermicity of 0.49 for fragmentation into [CH2CNH](•+) plus C2H4, hampered by an energy barrier of 0.29 eV. The energy difference between [CH3CN](•+) and [CH2CNH](•+) is 2.28 eV (with the latter being the lowest energy isomer), and the isomerization barrier is 0.84 eV. Reactive monitoring experiments of the [CH3CN](•+) and [CH2CNH](•+) isomers with C2H4 have been performed using the CERISES guided ion beam tandem mass spectrometer and exploiting the selectivity of ethylene that gives exothermic charge exchange and proton transfer reactions with [CH3CN](•+) but not with [CH2CNH](•+) isomers. In addition, minor reactive channels are observed leading to the formation of new C-C bonds upon reaction of [CH3CN](•+) with C2H4, and their astrochemical implications are briefly discussed.

  18. The use and re-use of unsustainably mined groundwater: A global budget

    Science.gov (United States)

    Grogan, D. S.; Prousevitch, A.; Wisser, D.; Lammers, R. B.; Frolking, S. E.

    2015-12-01

    Many of the world's major groundwater aquifers are rapidly depleting due to unsustainable groundwater pumping, while demand for food production - and therefore demand for irrigation water ­- is increasing. While it is likely that groundwater users will be impacted by the future's inevitable reduction in groundwater availability, there is a major gap in our understanding of potential impacts downstream of pumping sites. Due to inefficiencies in irrigation systems, significant amounts of abstracted groundwater become runoff, entering surface waters and flowing downstream to be re-abstracted and used again. In this study, we use a gridded water balance model to calculate the amount of unsustainably pumped groundwater that enters surface water systems by way of irrigation runoff, and quantify the additional irrigation water supplied by the re-use of this water. We assess the global budget of unsustainable groundwater sources and sinks, including downstream re-use, groundwater recharge, and flow to the oceans. Globally, we find that 80% of unsustainable groundwater is re-abstracted for irrigation either downstream or locally from groundwater recharge. This re-abstracted water contributes the water equivalent needed to irrigate 200,000 km2 of cropland globally. Including irrigation runoff reuse in an assessment of irrigation efficiency, we see that the traditional concept of irrigation efficiency (net irrigation/gross irrigation) significantly overestimates water "waste". We define a basin efficiency for unsustainable groundwater use that includes re-use, and see that while global irrigation efficiency is often estimated at 50%, global average unsustainable water use efficiency is > 60%. Losing this re-use resource by increasing irrigation efficiency does little to alleviate unsustainable groundwater demands.

  19. ISLSCP II Surface Radiation Budget (SRB) Radiation Data

    Data.gov (United States)

    National Aeronautics and Space Administration — ABSTRACT: This data set contains global Surface Radiation Budget (SRB) and a few top-of-atmosphere (TOA) radiation budget parameters on a 1-degree x 1-degree spatial...

  20. Optimal estimation of the surface fluxes of methyl chloride using a 3-D global chemical transport model

    Directory of Open Access Journals (Sweden)

    X. Xiao

    2010-06-01

    Full Text Available Methyl chloride (CH3Cl is a chlorine-containing trace gas in the atmosphere contributing significantly to stratospheric ozone depletion. Large uncertainties in estimates of its source and sink magnitudes and temporal and spatial variations currently exist. GEIA inventories and other bottom-up emission estimates are used to construct a priori maps of the surface fluxes of CH3Cl. The Model of Atmospheric Transport and Chemistry (MATCH, driven by NCEP interannually varying meteorological data, is then used to simulate CH3Cl mole fractions and quantify the time series of sensitivities of the mole fractions at each measurement site to the surface fluxes of various regional and global sources and sinks. We then implement the Kalman filter (with the unit pulse response method to estimate the surface fluxes on regional/global scales with monthly resolution from January 2000 to December 2004. High frequency observations from the AGAGE, SOGE, NIES, and NOAA/ESRL HATS in situ networks and low frequency observations from the NOAA/ESRL HATS flask network are used to constrain the source and sink magnitudes. The inversion results indicate global total emissions around 4100 ± 470 Gg yr−1 with very large emissions of 2200 ± 390 Gg yr−1 from tropical plants, which turn out to be the largest single source in the CH3Cl budget. Relative to their a priori annual estimates, the inversion increases global annual fungal and tropical emissions, and reduces the global oceanic source. The inversion implies greater seasonal and interannual oscillations of the natural sources and sink of CH3Cl compared to the a priori. The inversion also reflects the strong effects of the 2002/2003 globally widespread heat waves and droughts on global emissions from tropical plants, biomass burning and salt marshes, and on the soil sink.

  1. Capture and dissociation in the complex-forming CH + H2 → CH2 + H, CH + H2 reactions.

    Science.gov (United States)

    González, Miguel; Saracibar, Amaia; Garcia, Ernesto

    2011-02-28

    The rate coefficients for the capture process CH + H(2)→ CH(3) and the reactions CH + H(2)→ CH(2) + H (abstraction), CH + H(2) (exchange) have been calculated in the 200-800 K temperature range, using the quasiclassical trajectory (QCT) method and the most recent global potential energy surface. The reactions, which are of interest in combustion and in astrochemistry, proceed via the formation of long-lived CH(3) collision complexes, and the three H atoms become equivalent. QCT rate coefficients for capture are in quite good agreement with experiments. However, an important zero point energy (ZPE) leakage problem occurs in the QCT calculations for the abstraction, exchange and inelastic exit channels. To account for this issue, a pragmatic but accurate approach has been applied, leading to a good agreement with experimental abstraction rate coefficients. Exchange rate coefficients have also been calculated using this approach. Finally, calculations employing QCT capture/phase space theory (PST) models have been carried out, leading to similar values for the abstraction rate coefficients as the QCT and previous quantum mechanical capture/PST methods. This suggests that QCT capture/PST models are a good alternative to the QCT method for this and similar systems.

  2. Correlations between substrate availability, dissolved CH4, and CH4 emissions in an arctic wetland subject to warming and plant removal

    DEFF Research Database (Denmark)

    Nielsen, Cecilie Skov; Michelsen, Anders; Strobel, Bjarne W.

    2017-01-01

    The Arctic is warming which may potentially affect substrate availability, organic matter decomposition, plant growth, and plant species composition. This may lead to changes in the exchange of methane (CH4) and carbon dioxide (CO2) between the soil system and the atmosphere. Yet the correlations...

  3. Methanesulfonates of high-valent metals. Syntheses and structural features of MoO_2(CH_3SO_3)_2, UO_2(CH_3SO_3)_2, ReO_3(CH_3SO_3), VO(CH_3SO_3)_2, and V_2O_3(CH_3SO_3)_4 and their thermal decomposition under N_2 and O_2 atmosphere

    International Nuclear Information System (INIS)

    Betke, Ulf; Neuschulz, Kai; Wickleder, Mathias S.

    2011-01-01

    Oxide methanesulfonates of Mo, U, Re, and V have been prepared by reaction of MoO_3, UO_2(CH_3COO)_2.2 H_2O, Re_2O_7(H_2O)_2, and V_2O_5 with CH_3SO_3H or mixtures thereof with its anhydride. These compounds are the first examples of solvent-free oxide methanesulfonates of these elements. MoO_2(CH_3SO_3)_2 (Pbca, a=1487.05(4), b=752.55(2), c=1549.61(5) pm, V=1.73414(9) nm"3, Z=8) contains [MoO_2] moieties connected by [CH_3SO_3] ions to form layers parallel to (100). UO_2(CH_3SO_3)_2 (P2_1/c, a=1320.4(1), b=1014.41(6), c=1533.7(1) pm, β=112.80(1) "c"i"r"c"l"e, V=1.8937(3) nm"3, Z=8) consists of linear UO_2"2"+ ions coordinated by five [CH_3SO_3] ions, forming a layer structure. VO(CH_3SO_3)_2 (P2_1/c, a=1136.5(1), b=869.87(7), c=915.5(1) pm, β=113.66(1) "c"i"r"c"l"e, V=0.8290(2) nm"3, Z=4) contains [VO] units connected by methanesulfonate anions to form corrugated layers parallel to (100). In ReO_3(CH_3SO_3) (P anti 1, a=574.0(1), b=1279.6(3), c=1641.9(3) pm, α=102.08(2), β=96.11(2), γ=99.04(2) "c"i"r"c"l"e, V=1.1523(4) nm"3, Z=8) a chain structure exhibiting infinite O-[ReO_2]-O-[ReO_2]-O chains is formed. Each [ReO_2]-O-[ReO_2] unit is coordinated by two bidentate [CH_3SO_3] ions. V_2O_3(CH_3SO_3)_4 (I2/a, a=1645.2(3), b=583.1(1), c=1670.2(3) pm, β=102.58(3), V=1.5637(5) pm"3, Z=4) adopts a chain structure, too, but contains discrete [VO]-O-[VO] moieties, each coordinated by two bidentate [CH_3SO_3] ligands. Additional methanesulfonate ions connect the [V_2O_3] groups along [001]. Thermal decomposition of the compounds was monitored under N_2 and O_2 atmosphere by thermogravimetric/differential thermal analysis and XRD measurements. Under N_2 the decomposition proceeds with reduction of the metal leading to the oxides MoO_2, U_3O_7, V_4O_7, and VO_2; for MoO_2(CH_3SO_3)_2, a small amount of MoS_2 is formed. If the thermal decomposition is carried out in a atmosphere of O_2 the oxides MoO_3 and V_2O_5 are formed. (Copyright copyright 2011 WILEY-VCH Verlag

  4. Summary of LOX/CH4 Thruster Technology Development at NASA/MSFC

    Science.gov (United States)

    Greene, Sandra Elam

    2015-01-01

    In recent years, a variety of injectors for liquid oxygen (LOX) and methane (CH4) propellant systems have been designed, fabricated, and demonstrated with hot-fire testing at Marshall Space Flight Center (MSFC). Successful designs for liquid methane (LCH4) and gaseous methane (GCH4) have been developed. A variety of chambers, including a transpiration cooled design, along with uncooled ablatives and refractory metals, have also been hot-fire tested by MSFC for use with LOX/LCH4 injectors. Hot-fire testing has also demonstrated multiple ignition source options. Heat flux data for selected injectors has been gathered by testing with a calorimeter chamber. High performance and stable combustion have been demonstrated, along with designs for thrust levels ranging from 500 to 7,000 lbf. The newest LOX/CH4 injector and chamber developed by MSFC have been fabricated with additive manufacturing techniques and include unique design features to investigate regenerative cooling with methane. This low cost and versatile hardware offers a design for 4,000 lbf thrust and will be hot-fire tested at MSFC in 2015. Its design and operation can easily be scaled for use in systems with thrust levels up to 25,000 lbf.

  5. Variable temperature ion trap studies of CH4+ + H2, HD and D2: negative temperature dependence and significant isotope effect

    International Nuclear Information System (INIS)

    Asvany, O.; Savic, I.; Schlemmer, S.; Gerlich, D.

    2004-01-01

    Reactions of methane cations, CH 4 + , with H 2 , HD and D 2 have been studied in a variable temperature 22-pole ion trap from room temperature down to 15 K. The formation of CH 5 + in collisions with H 2 is slow at 300 K, but it becomes faster by at least one order of magnitude when the temperature is lowered to 15 K. This behavior is tentatively explained with a longer complex lifetime at low temperatures. However, since tunneling is most probably not responsible for product formation, other dynamical or statistical restrictions must be responsible for the negative temperature dependence. In collisions of CH 4 + with HD, the CH 5 + product ion (68% at 15 K) prevails over CH 4 D + (32%). Reaction of CH 4 + with D 2 is found to be much slower than with H 2 or HD. The rate coefficient for converting CH 4 + into CH 3 D + by H-D exchange has been determined to be smaller than 10 -12 cm 3 /s, indicating that scrambling in the CH 6 + complex is very unlikely

  6. Efficient Synthesis of Ethanol from CH4 and Syngas on a Cu-Co/TiO2 Catalyst Using a Stepwise Reactor

    Science.gov (United States)

    Zuo, Zhi-Jun; Peng, Fen; Huang, Wei

    2016-10-01

    Ethanol synthesis from CH4 and syngas on a Cu-Co/TiO2 catalyst is studied using experiments, density functional theory (DFT) and microkinetic modelling. The experimental results indicate that the active sites of ethanol synthesis from CH4 and syngas are Cu and CoO, over which the ethanol selectivity is approximately 98.30% in a continuous stepwise reactor. DFT and microkinetic modelling results show that *CH3 is the most abundant species and can be formed from *CH4 dehydrogenation or through the process of *CO hydrogenation. Next, the insertion of *CO into *CH3 forms *CH3CO. Finally, ethanol is formed through *CH3CO and *CH3COH hydrogenation. According to our results, small particles of metallic Cu and CoO as well as a strongly synergistic effect between metallic Cu and CoO are beneficial for ethanol synthesis from CH4 and syngas on a Cu-Co/TiO2 catalyst.

  7. Measurements and Interpretation of Surface Mixing Ratios of CH4 and CO and δ 13C and δ D of CH4 in Air from Pacific Ocean Transects Between Auckland, New Zealand and Los Angeles, California

    Science.gov (United States)

    Ajie, H. O.; Tyler, S. C.; Gotoh, A. A.; McMillan, A. M.; Rice, A. L.; Lowe, D. C.

    2003-12-01

    We report on measurements of atmospheric CH4 and CO mixing ratios and δ 13C of CH4 from air samples collected every 2.5 to 5° latitude along a transect over the Pacific Ocean using container ships of P&O Nedlloyd (formerly Blue Star) shipping line. Data presented here begins in June 1996 and extends to January 2002. Scientists from the National Institute of Water and Atmospheric Research in New Zealand and from University of California, Irvine alternate sampling trips so that a transect between Auckland, New Zealand (35° S) and Los Angeles, California (35° N) can be sampled over a period of ˜15 days approximately every four months. Data sets from the two laboratories are intercalibrated through a sample exchange program. The data provide detail on the spatial and seasonal variation of CH4 and CO mixing ratios and stable isotope ratios of CH4 over the Pacific equatorial region, including the Intertropical Convergence Zone (ITCZ) and both northern and southern temperate zones to about 30° latitude, including the South Pacific Convergence Zone (SPCZ). Data from 18 transect samplings so far clearly show that δ 13C in the mid latitudes of both hemispheres are ˜6 months out of phase. In June, a minimum in δ 13C CH4 in the southern hemisphere (SH) coincides approximately with the maximum in the northern hemisphere (NH) seasonal cycle. Because the NH is less enriched in 13C than the SH this situation results in a remarkably flat gradient between 30° N and 30° S. In November the opposite situation occurs with the SH mid latitude maximum coinciding with the minimum in the NH cycle, leading to a relatively large gradient of ˜0.5‰ between the hemispheres. We discuss how CH4 and CO mixing ratios are related to the changing positions and strengths of the ITCZ and SPCZ and how this data can be used in multi-dimensional models of atmospheric chemistry and transport to better define CH4 sources and sinks both temporally and spatially.

  8. Reducing CH{sub 4} and CO{sub 2} emissions from waterlogged paddy soil with biochar

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Yuxue; Yang, Min; Chen, Yingxu; Wu, Weixiang [Zhejiang Univ., Hangzhou (China). Inst. of Environmental Science and Technology; Wu, Yimin [Hangzhou No. 2 High School, Hangzhou (China); Wang, Hailong [Scion, Rotorua (New Zealand)

    2011-09-15

    Purpose: A potential means to diminish increasing levels of CO{sub 2} in the atmosphere is the use of pyrolysis to convert biomass into biochar, which stabilizes the carbon (C) that is then applied to soil. Before biochar can be used on a large scale, especially in agricultural soils, its effects on the soil system need to be assessed. This is especially important in rice paddy soils that release large amounts of greenhouse gases to the atmosphere. Materials and methods: In this study, the effects of biochar on CH{sub 4} and CO{sub 2} emissions from paddy soil with and without rice straw added as an additional C source were investigated. The biochars tested were prepared from bamboo chips or rice straw which yielded bamboo char (BC) and straw char (SC), respectively. BC and SC were applied to paddy soil to achieve low, medium, and high rates, based on C contents of the biochars. The biochar-amended soils were incubated under waterlogged conditions in the laboratory. Results and discussion: Adding rice straw significantly increased CH{sub 4} and CO{sub 2} emissions from the paddy soil. However, when soils were amended with biochar, CH{sub 4} emissions were reduced. CH{sub 4} emissions from the paddy soil amended with BC and SC at high rate were reduced by 51.1% and 91.2%, respectively, compared with those without biochar. Methanogenic activity in the paddy soil decreased with increasing rates of biochar, whereas no differences in denaturing gradient gel electrophoresis patterns were observed. CO{sub 2} emission from the waterlogged paddy soil was also reduced in the biochar treatments. Conclusions: Our results showed that SC was more effective than BC in reducing CH{sub 4} and CO{sub 2} emissions from paddy soils. The reduction of CH{sub 4} emissions from paddy soil with biochar amendment may result from the inhibition of methanogenic activity or a stimulation of methylotrophic activity during the incubation period. (orig.)

  9. Real-time analysis of δ13C- and δD-CH4 by high precision laser spectroscopy

    Science.gov (United States)

    Eyer, Simon; Emmenegger, Lukas; Tuzson, Béla; Fischer, Hubertus; Mohn, Joachim

    2014-05-01

    Methane (CH4) is the most important non-CO2 greenhouse gas (GHG) contributing 18% to total radiative forcing. Anthropogenic sources (e.g. ruminants, landfills) contribute 60% to total emissions and led to an increase in its atmospheric mixing ratio from 700 ppb in pre-industrial times to 1819 ± 1 ppb in 2012 [1]. Analysis of the most abundant methane isotopologues 12CH4, 13CH4 and 12CH3D can be used to disentangle the various source/sink processes [2] and to develop target oriented reduction strategies. High precision isotopic analysis of CH4 can be accomplished by isotope-ratio mass-spectrometry (IRMS) [2] and more recently by mid-infrared laser-based spectroscopic techniques. For high precision measurements in ambient air, however, both techniques rely on preconcentration of the target gas [3]. In an on-going project, we developed a fully-automated, field-deployable CH4 preconcentration unit coupled to a dual quantum cascade laser absorption spectrometer (QCLAS) for real-time analysis of CH4 isotopologues. The core part of the rack-mounted (19 inch) device is a highly-efficient adsorbent trap attached to a motorized linear drive system and enclosed in a vacuum chamber. Thereby, the adsorbent trap can be decoupled from the Stirling cooler during desorption for fast desorption and optimal heat management. A wide variety of adsorbents, including: HayeSep D, molecular sieves as well as the novel metal-organic frameworks and carbon nanotubes were characterized regarding their surface area, isosteric enthalpy of adsorption and selectivity for methane over nitrogen. The most promising candidates were tested on the preconcentration device and a preconcentration by a factor > 500 was obtained. Furthermore analytical interferants (e.g. N2O, CO2) are separated by step-wise desorption of trace gases. A QCL absorption spectrometer previously described by Tuzson et al. (2010) for CH4 flux measurements was modified to obtain a platform for high precision and simultaneous

  10. Application of stable isotope analysis for improved understanding of the methane budget: comparison of TROICA measurements with TM3 model simulations

    NARCIS (Netherlands)

    Tarasova, O.A.; Houweling, S.; Elansky, N.F.; Brenninkmeijer, C.A.M.

    2010-01-01

    Presented is a detailed comparison of CH4 and δ13C–CH4 measurements with simulations of the global transport model TM3. Experimental data were obtained during campaigns along the Trans-Siberian railroad in the framework of the TROICA project. Two summer (1999 and 2001) and one spring (2003)

  11. Gully hotspot contribution to landscape methane (CH4) and carbon dioxide (CO2) fluxes in a northern peatland

    International Nuclear Information System (INIS)

    McNamara, N.P.; Plant, T.; Oakley, S.; Ward, S.; Wood, C.; Ostle, N.

    2008-01-01

    Peatlands are long term carbon catchments that sink atmospheric carbon dioxide (CO 2 ) and source methane (CH 4 ). In the uplands of the United Kingdom ombrotrophic blanket peatlands commonly exist within Calluna vulgaris (L.) dominated moorland ecosystems. These landscapes contain a range of topographical features that influence local hydrology, climate and plant community composition. In this study we examined the variation in ecosystem CO 2 respiration and net CH 4 fluxes from typical plant-soil systems in dendritic drainage gullies and adjacent blanket peat during the growing season. Typically, Eriophorum spp., Sphagnum spp. and mixed grasses occupied gullies while C. vulgaris dominated in adjacent blanket peat. Gross CO 2 respiration was highest in the areas of Eriophorum spp. (650 ± 140 mg CO 2 m -2 h -1 ) compared to those with Sphagnum spp. (338 ± 49 mg CO 2 m -2 h -1 ), mixed grasses (342 ± 91 mg CO 2 m -2 h -1 ) and C. vulgaris (174 ± 63 mg CO 2 m -2 h -1 ). Measurements of the net CH 4 flux showed higher fluxes from the Eriophorum spp (2.2 ± 0.6 mg CH 4 m -2 h -1 ) locations compared to the Sphagnum spp. (0.6 ± 0.4 mg CH 4 m -2 h -1 ), mixed grasses (0.1 ±0.1 mg CH 4 m -2 h -1 ) and a negligible flux detected from C. vulgaris (0.0 ± 0.0 mg CH 4 m -2 h -1 ) locations. A GIS approach was applied to calculate the contribution of gullies to landscape scale greenhouse gas fluxes. Findings from the Moor House National Nature Reserve in the UK showed that although gullies occupied only 9.3% of the total land surface, gullies accounted for 95.8% and 21.6% of the peatland net CH 4 and CO 2 respiratory fluxes, respectively. The implication of these findings is that the relative contribution of characteristic gully systems need to be considered in estimates of landscape scale peatland greenhouse gas fluxes

  12. CH-TRU Content Codes (CH-TRUCON)

    International Nuclear Information System (INIS)

    2005-01-01

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes 'shipping categories' that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the 'General Case,' which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for 'Close-Proximity Shipments' (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for 'Controlled Shipments

  13. CH-TRU Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2005-10-15

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  14. The reaction of fluorine atoms with methanol: yield of CH3O/CH2OH and rate constant of the reactions CH3O + CH3O and CH3O + HO2.

    Science.gov (United States)

    Assaf, Emmanuel; Schoemaecker, Coralie; Vereecken, Luc; Fittschen, Christa

    2018-04-25

    Xenondifluoride, XeF2, has been photolysed in the presence of methanol, CH3OH. Two reaction pathways are possible: F + CH3OH → CH2OH + HF and F + CH3OH → CH3O + HF. Both products, CH2OH and CH3O, will be converted to HO2 in the presence of O2. The rate constants for the reaction of both radicals with O2 differ by more than 3 orders of magnitude, which allows an unequivocal distinction between the two reactions when measuring HO2 concentrations in the presence of different O2 concentrations. The following yields have then been determined from time-resolved HO2 profiles: φCH2OH = (0.497 ± 0.013) and φCH3O = (0.503 ± 0.013). Experiments under low O2 concentrations lead to reaction mixtures containing nearly equal amounts of HO2 (converted from the first reaction) and CH3O (from the second reaction). The subsequent HO2 decays are very sensitive to the rate constants of the reaction between these two radicals and the following rate constants have been obtained: k(CH3O + CH3O) = (7.0 ± 1.4) × 10-11 cm3 s-1 and k(CH3O + HO2) = (1.1 ± 0.2) × 10-10 cm3 s-1. The latter reaction has also been theoretically investigated on the CCSD(T)//M06-2X/aug-cc-pVTZ level of theory and CH3OH + O2 have been identified as the main products. Using μVTST, a virtually pressure independent rate constant of k(CH3O + HO2) = 4.7 × 10-11 cm3 s-1 has been obtained, in good agreement with the experiment.

  15. 生物炭对土壤N2O和CH4排放影响的研究进展%Advances in Effects of Biochar on the Soil N2O and CH4 Emissions

    Institute of Scientific and Technical Information of China (English)

    颜永毫; 王丹丹; 郑纪勇

    2013-01-01

    In order to study the pathway and mechanism of biochar affecting soil N2O and CH4 emissions, based on comprehensive evaluation of published researches, the factors, pathway and mechanism that biochar affected soil N2O and CH4 emissions were analyzed, the principles of biochar addition in different types of soil were then proposed. The key problems that should be paid attention to in future studies were pointed out: (1) the characters of these two GHG emissions in soil should be explicited, the biochar type should be chosen according to the local soil conditions. (2) The time and amount of biochar addition should be reasonable. (3) Nowadays because of the differences of biochars and soil types that different scholars used, the research conclusions about the effects of biochar on the soil N2O and CH4 emissions were still controversial. In future, the more clear conclusions about the effects of biochar on the soil N2O and CH4 would be attained till the experiments of returning biochar into field according to the local soil type should be continued after the complement of biochar applying standard.%为了探讨生物炭对土壤N2O和CH4排放影响的途径和机理,在综合评述前人研究的基础上,就生物炭对土壤N2O和CH4排放的影响因素、途径和影响机理进行了分析,提出了不同土壤的生物炭施用原则,并指出了今后生物炭研究应注意的问题:(1)明确土壤中2种温室气体排放特点,园地制宜地选择合适的生物炭类型;(2)注意生物炭的添加时机和用量;(3)目前学者所用的生物炭类型以及土壤种类不同,关于生物炭影响土壤N2O和CH4排放的研究结论不同.在这方面的研究工作还应在完善生物炭施用标准的基础上,继续进行生物炭还田的本地化试验验证,才能为生物炭对土壤N2O和CH4排放的影响得出更明确的结论.

  16. Calibration and field testing of cavity ring-down laser spectrometers measuring CH4, CO2, and δ13CH4 deployed on towers in the Marcellus Shale region

    Directory of Open Access Journals (Sweden)

    N. L. Miles

    2018-03-01

    Full Text Available Four in situ cavity ring-down spectrometers (G2132-i, Picarro, Inc. measuring methane dry mole fraction (CH4, carbon dioxide dry mole fraction (CO2, and the isotopic ratio of methane (δ13CH4 were deployed at four towers in the Marcellus Shale natural gas extraction region of Pennsylvania. In this paper, we describe laboratory and field calibration of the analyzers for tower-based applications and characterize their performance in the field for the period January–December 2016. Prior to deployment, each analyzer was tested using bottles with various isotopic ratios, from biogenic to thermogenic source values, which were diluted to varying degrees in zero air, and an initial calibration was performed. Furthermore, at each tower location, three field tanks were employed, from ambient to high mole fractions, with various isotopic ratios. Two of these tanks were used to adjust the calibration of the analyzers on a daily basis. We also corrected for the cross-interference from ethane on the isotopic ratio of methane. Using an independent field tank for evaluation, the standard deviation of 4 h means of the isotopic ratio of methane difference from the known value was found to be 0.26 ‰ δ13CH4. Following improvements in the field tank testing scheme, the standard deviation of 4 h means was 0.11 ‰, well within the target compatibility of 0.2 ‰. Round-robin style testing using tanks with near-ambient isotopic ratios indicated mean errors of −0.14 to 0.03 ‰ for each of the analyzers. Flask to in situ comparisons showed mean differences over the year of 0.02 and 0.08 ‰, for the east and south towers, respectively. Regional sources in this region were difficult to differentiate from strong perturbations in the background. During the afternoon hours, the median differences of the isotopic ratio measured at three of the towers, compared to the background tower, were &minus0.15 to 0.12 ‰ with standard deviations of the 10

  17. Calibration and field testing of cavity ring-down laser spectrometers measuring CH4, CO2, and δ13CH4 deployed on towers in the Marcellus Shale region

    Science.gov (United States)

    Miles, Natasha L.; Martins, Douglas K.; Richardson, Scott J.; Rella, Christopher W.; Arata, Caleb; Lauvaux, Thomas; Davis, Kenneth J.; Barkley, Zachary R.; McKain, Kathryn; Sweeney, Colm

    2018-03-01

    Four in situ cavity ring-down spectrometers (G2132-i, Picarro, Inc.) measuring methane dry mole fraction (CH4), carbon dioxide dry mole fraction (CO2), and the isotopic ratio of methane (δ13CH4) were deployed at four towers in the Marcellus Shale natural gas extraction region of Pennsylvania. In this paper, we describe laboratory and field calibration of the analyzers for tower-based applications and characterize their performance in the field for the period January-December 2016. Prior to deployment, each analyzer was tested using bottles with various isotopic ratios, from biogenic to thermogenic source values, which were diluted to varying degrees in zero air, and an initial calibration was performed. Furthermore, at each tower location, three field tanks were employed, from ambient to high mole fractions, with various isotopic ratios. Two of these tanks were used to adjust the calibration of the analyzers on a daily basis. We also corrected for the cross-interference from ethane on the isotopic ratio of methane. Using an independent field tank for evaluation, the standard deviation of 4 h means of the isotopic ratio of methane difference from the known value was found to be 0.26 ‰ δ13CH4. Following improvements in the field tank testing scheme, the standard deviation of 4 h means was 0.11 ‰, well within the target compatibility of 0.2 ‰. Round-robin style testing using tanks with near-ambient isotopic ratios indicated mean errors of -0.14 to 0.03 ‰ for each of the analyzers. Flask to in situ comparisons showed mean differences over the year of 0.02 and 0.08 ‰, for the east and south towers, respectively. Regional sources in this region were difficult to differentiate from strong perturbations in the background. During the afternoon hours, the median differences of the isotopic ratio measured at three of the towers, compared to the background tower, were &minus0.15 to 0.12 ‰ with standard deviations of the 10 min isotopic ratio differences of 0.8

  18. Glacial-interglacial water cycle, global monsoon and atmospheric methane changes

    Energy Technology Data Exchange (ETDEWEB)

    Guo, Zhengtang; Wu, Haibin [Chinese Academy of Sciences, Key Laboratory of Cenozoic Geology and Environment, Institute of Geology and Geophysics, Beijing (China); Zhou, Xin [Chinese Academy of Sciences, Key Laboratory of Cenozoic Geology and Environment, Institute of Geology and Geophysics, Beijing (China); University of Science and Technology of China, School of Earth and Space Sciences and Institute of Polar Environment, Hefei (China)

    2012-09-15

    The causes of atmospheric methane (CH{sub 4}) changes are still a major contention, in particular with regards to the relative contributions of glacial-interglacial cycles, monsoons in both hemispheres and the late Holocene human intervention. Here, we explore the CH{sub 4} signals in the Antarctic EPICA Dome C and Vostok ice records using the methods of timeseries analyses and correlate them with insolation and geological records to address these issues. The results parse out three distinct groups of CH{sub 4} signals attributable to different drivers. The first group ({proportional_to}80% variance), well tracking the marine {delta}{sup 18}O record, is attributable to glacial-interglacial modulation on the global water cycle with the effects shared by wetlands at all latitudes, from monsoonal and non-monsoonal regions in both hemispheres. The second group ({proportional_to}15% variance), centered at the {proportional_to}10-kyr semi-precession frequency, is linkable with insolation-driven tropical monsoon changes in both hemispheres. The third group ({proportional_to}5% variance), marked by millennial frequencies, is seemingly related with the combined effect of ice-volume and bi-hemispheric insolation changes at the precession bands. These results indicate that bi-hemispheric monsoon changes have been a constant driver of atmospheric CH{sub 4}. This mechanism also partially explains the Holocene CH{sub 4} reversal since {proportional_to}5 kyr BP besides the human intervention. In the light of these results, we propose that global monsoon can be regarded as a system consisting of two main integrated components, one primarily driven by the oscillations of Inter-Tropical Convergence Zone (ITCZ) in response to the low-latitude summer insolation changes, anti-phase between the two hemispheres (i.e. the ITCZ monsoon component); and another modulated by the glacial-interglacial cycles, mostly synchronous at the global scale (i.e. the glacial-interglacial monsoon

  19. Biodiversity effects of benthic ecosystem engineers on the spatial patterns of sediment CH4 concentration in an urban Neotropical coastal lagoon

    Directory of Open Access Journals (Sweden)

    Adriano Caliman

    Full Text Available AIM: Biodiversity of sediment bioturbators has been shown to be important for to the magnitude and stability of benthic-pelagic processes. However, no study to date has evaluated the importance of the biodiversity of benthic invertebrate bioturbators to the spatial patterns of sediment CH4 concentration ([CH4]. Here we conducted a laboratorial experiment to test the following predictions: (1 Bioturbator species richness will reduce the sediment [CH4]; (2 individual bioturbator species (i.e. species composition will have different effects on sediment [CH4]; (3 and both the effects of bioturbator species richness and composition on sediment [CH4] will be dependent on sediment depth. METHODS: We manipulated the number and composition of three functional divergent benthic invertebrate bioturbators species that are widespread in South Atlantic coastal lagoons, in laboratorial sediment chambers containing the sediment and water of an urban impacted coastal lagoon RESULTS: Bioturbator species richness had no overall significant effect on sediment [CH4] when comparisons of sediment [CH4] were made among species richness levels. However, bioturbator species richness significantly reduced sediment [CH4] when species richness levels were compared to the control (defaunated treatments, but this effect was significant only at the deepest sediment layer. Furthermore, bioturbator species composition had significant, but distinct effects on the patterns of reduction in sediment [CH4], depending on the sediment depth and the bioturbator species. CONCLUSIONS: We conclude that both the number and composition of bioturbator species are important to determine the effects of benthic bioturbators on spatial patterns of sediment [CH4], but the strength of these effects depend on species traits that determine interspecific interactions strength across the sediment vertical niche space.

  20. CH4 and N2O emissions embodied in international trade of meat

    International Nuclear Information System (INIS)

    Caro, Dario; Caldeira, Ken; LoPresti, Anna; Davis, Steven J; Bastianoni, Simone

    2014-01-01

    Although previous studies have quantified carbon dioxide emissions embodied in products traded internationally, there has been limited attention to other greenhouse gases such as methane (CH 4 ) and nitrous oxide (N 2 O). Following IPCC guidelines, we estimate non-CO 2 emissions from beef, pork and chicken produced in 237 countries over the period 1990–2010, and assign these emissions to the country where the meat is ultimately consumed. We find that, between 1990 and 2010, an average of 32.8 Mt CO 2 -eq emissions (using 100 year global warming potentials) are embodied in beef, pork and chicken traded internationally. Further, over the 20 year period, the quantity of CO 2 -eq emissions embodied in traded meat increased by 19%. The largest trade flows of emissions embodied in meat were from Brazil and Argentina to Russia (2.8 and 1.4 Mt of CO 2 -eq, respectively). Trade flows within the European region are also substantial: beef and pork exported from France embodied 3.3 Mt and 0.4 Mt of CO 2 -eq, respectively. Emissions factor of meat production (i.e. CO 2 -eq emissions per kg of meat) produced depend on ambient temperature, development level, livestock category (e.g. cattle, pork, and chicken) and livestock management practices. Thus, trade may result in an overall increase of GHG emissions when meat-consuming countries import meat from countries with a greater emissions intensity of meat production rather than producing the meat domestically. Comparing the emissions intensity of meat production of trading partners, we assess trade flows according to whether they tend to reduce or increase global emissions from meat production. (letter)

  1. Implications for carbon processing beneath the Greenland Ice Sheet from dissolved CO2 and CH4 concentrations of subglacial discharge

    Science.gov (United States)

    Pain, A.; Martin, J.; Martin, E. E.

    2017-12-01

    Subglacial carbon processes are of increasing interest as warming induces ice melting and increases fluxes of glacial meltwater into proglacial rivers and the coastal ocean. Meltwater may serve as an atmospheric source or sink of carbon dioxide (CO2) or methane (CH4), depending on the magnitudes of subglacial organic carbon (OC) remineralization, which produces CO2 and CH4, and mineral weathering reactions, which consume CO2 but not CH4. We report wide variability in dissolved CO2 and CH4 concentrations at the beginning of the melt season (May-June 2017) between three sites draining land-terminating glaciers of the Greenland Ice Sheet. Two sites, located along the Watson River in western Greenland, drain the Isunnguata and Russell Glaciers and contained 1060 and 400 ppm CO2, respectively. In-situ CO2 flux measurements indicated that the Isunnguata was a source of atmospheric CO2, while the Russell was a sink. Both sites had elevated CH4 concentrations, at 325 and 25 ppm CH4, respectively, suggesting active anaerobic OC remineralization beneath the ice sheet. Dissolved CO2 and CH4 reached atmospheric equilibrium within 2.6 and 8.6 km downstream of Isunnguata and Russell discharge sites, respectively. These changes reflect rapid gas exchange with the atmosphere and/or CO2 consumption via instream mineral weathering. The third site, draining the Kiagtut Sermiat in southern Greenland, had about half atmospheric CO2 concentrations (250 ppm), but approximately atmospheric CH4 concentrations (2.1 ppm). Downstream CO2 flux measurements indicated ingassing of CO2 over the entire 10-km length of the proglacial river. CO2 undersaturation may be due to more readily weathered lithologies underlying the Kiagtut Sermiat compared to Watson River sites, but low CH4 concentrations also suggest limited contributions of CO2 and CH4 from OC remineralization. These results suggest that carbon processing beneath the Greenland Ice Sheet may be more variable than previously recognized

  2. How to determine the GHG budget of a pasture field with grazing animals

    Science.gov (United States)

    Ammann, Christof; Neftel, Albrecht; Felber, Raphael

    2016-04-01

    Up to now the scientific investigation and description of the agriculture related greenhouse gas (GHG) exchange has been largely separated into (i) direct animal related and (ii) ecosystem area related processes and measurement methods. An overlap of the two usually separated topics occurs for grazed pastures, where direct animal and pasture area emissions are relevant. In the present study eddy covariance (EC) flux measurements on the field scale were combined with a source location attribution (footprint) model and with GPS position measurements of the individual animals. The experiment was performed on a pasture field in Switzerland under a rotational full grazing regime with dairy cows. The exchange fluxes of CH4, CO2, and N2O were measured simultaneously over the entire year. The observed CH4 emission fluxes correlated well with the presence of cows in the flux footprint. When converted to average emission per cow, the results agreed with published values from respiration chamber experiments with similar cows. For CO2 a sophisticated partitioning algorithm was applied to separate the pasture and animal contributions, because both were in the same order of magnitude. The N2O exchange fully attributable to the pasture soil showed considerable and continuous emissions through the entire seasonal course mainly modulated by soil moisture and temperature. The resulting GHG budget shows that the largest GHG effect of the pasture system was due to enteric CH4 emissions followed by soil N2O emissions, but that the carbon storage change was affected by a much larger uncertainty. The results demonstrate that the EC technique in combination with animal position information allows to consistently quantify the exchange of all three GHG on the pasture and to adequately distinguish between direct animal and diffuse area sources (and sinks). Yet questions concerning a standardized attribution of animal related emissions to the pasture GHG budget still need to be resolved.

  3. Pure- and mixed-gas CO2/CH4 separation properties of PIM-1 and an amidoxime-functionalized PIM-1

    KAUST Repository

    Swaidan, Raja

    2014-05-01

    The prototypical solution-processable polymer of intrinsic microporosity, PIM-1, and derivatives thereof offer combinations of permeability and selectivity that make them potential candidate materials for membrane-based gas separations. Paramount to the design and evaluation of PIMs for economical natural gas sweetening is a high and stable CO2/CH4 selectivity under realistic, mixed-gas conditions. Here, amidoxime-functionalized PIM-1 (AO-PIM-1) was prepared and examined for fundamental structure/property relationships. Qualitative NLDFT pore-size distribution analyses of physisorption isotherms (N2 at -196 oC; CO2 at 0 oC) reveal a tightened microstructure indicating size-sieving ultra-microporosity (<7Å). AO-PIM-1 demonstrated a three-fold increase in αD(CO2/CH4) over PIM-1, surpassing the 2008 upper bound with P(CO2)=1153Barrer and ideal α(CO2/CH4)=34. Under a 50:50 CO2:CH4 mixed-gas feed, AO-PIM-1 showed less selectivity loss than PIM-1, maintaining a mixed-gas α(CO2/CH4) ~21 across a 20bar pressure range. Conversely, PIM-1 endured up to 60% increases in mixed-gas CH4 permeability over pure-gas values concurrent with a selectivity of only ~8 at 20bar. A pervasive intermolecular hydrogen bonding network in AO-PIM-1 predominantly yields a rigidified microstructure that mitigates CO2-induced matrix dilations, reducing detrimental mixed-gas CH4 copermeation. © 2014 Elsevier B.V.

  4. CMS (Carbon Monitoring System) Methane (CH4) Flux for North America 0.5 degree x 0.667 degree V1 (CMS_CH4_FLX_NA) at GES DISC

    Data.gov (United States)

    National Aeronautics and Space Administration — The CMS Methane (CH4) Flux for North America data set contains estimates of methane emission in North America based on an inversion of the GEOS-Chem chemical...

  5. Soil Methanotrophy Model (MeMo v1.0): a process-based model to quantify global uptake of atmospheric methane by soil

    Science.gov (United States)

    Murguia-Flores, Fabiola; Arndt, Sandra; Ganesan, Anita L.; Murray-Tortarolo, Guillermo; Hornibrook, Edward R. C.

    2018-06-01

    Soil bacteria known as methanotrophs are the sole biological sink for atmospheric methane (CH4), a potent greenhouse gas that is responsible for ˜ 20 % of the human-driven increase in radiative forcing since pre-industrial times. Soil methanotrophy is controlled by a plethora of factors, including temperature, soil texture, moisture and nitrogen content, resulting in spatially and temporally heterogeneous rates of soil methanotrophy. As a consequence, the exact magnitude of the global soil sink, as well as its temporal and spatial variability, remains poorly constrained. We developed a process-based model (Methanotrophy Model; MeMo v1.0) to simulate and quantify the uptake of atmospheric CH4 by soils at the global scale. MeMo builds on previous models by Ridgwell et al. (1999) and Curry (2007) by introducing several advances, including (1) a general analytical solution of the one-dimensional diffusion-reaction equation in porous media, (2) a refined representation of nitrogen inhibition on soil methanotrophy, (3) updated factors governing the influence of soil moisture and temperature on CH4 oxidation rates and (4) the ability to evaluate the impact of autochthonous soil CH4 sources on uptake of atmospheric CH4. We show that the improved structural and parametric representation of key drivers of soil methanotrophy in MeMo results in a better fit to observational data. A global simulation of soil methanotrophy for the period 1990-2009 using MeMo yielded an average annual sink of 33.5 ± 0.6 Tg CH4 yr-1. Warm and semi-arid regions (tropical deciduous forest and open shrubland) had the highest CH4 uptake rates of 602 and 518 mg CH4 m-2 yr-1, respectively. In these regions, favourable annual soil moisture content ( ˜ 20 % saturation) and low seasonal temperature variations (variations < ˜ 6 °C) provided optimal conditions for soil methanotrophy and soil-atmosphere gas exchange. In contrast to previous model analyses, but in agreement with recent observational data

  6. Flask sample measurements for CO2, CH4 and CO using cavity ring-down spectrometry

    Science.gov (United States)

    Wang, J.-L.; Jacobson, G.; Rella, C. W.; Chang, C.-Y.; Liu, I.; Liu, W.-T.; Chew, C.; Ou-Yang, C.-F.; Liao, W.-C.; Chang, C.-C.

    2013-08-01

    In recent years, cavity ring-down spectrometry (CRDS) has been demonstrated to be a highly sensitive, stable and fast analytical technique for real-time in situ measurements of greenhouse gases. In this study, we propose the technique (which we call flask-CRDS) of analyzing whole air flask samples for CO2, CH4 and CO using a custom gas manifold designed to connect to a CRDS analyzer. Extremely stable measurements of these gases can be achieved over a large pressure range in the flask, from 175 to 760 Torr. The wide pressure range is conducive to flask sample measurement in three ways: (1) flask samples can be collected in low-pressure environments (e.g. high-altitude locations); (2) flask samples can be first analyzed for other trace gases with the remaining low-pressure sample for CRDS analysis of CO2, CH4 and CO; and (3) flask samples can be archived and re-analyzed for validation. The repeatability of this method (1σ of 0.07 ppm for CO2, 0.4 ppb for CH4, and 0.5 ppb for CO) was assessed by analyzing five canisters filled with the same air sample to a pressure of 200 Torr. An inter-comparison of the flask-CRDS data with in-situ CRDS measurements at a high-altitude mountain baseline station revealed excellent agreement, with differences of 0.10 ± 0.09 ppm (1σ) for CO2 and 0.9 ± 1.0 ppb for CH4. This study demonstrated that the flask-CRDS method was not only simple to build and operate but could also perform highly accurate and precise measurements of atmospheric CO2, CH4 and CO in flask samples.

  7. Quantitative ChIP-Seq Normalization Reveals Global Modulation of the Epigenome

    Directory of Open Access Journals (Sweden)

    David A. Orlando

    2014-11-01

    Full Text Available Epigenomic profiling by chromatin immunoprecipitation coupled with massively parallel DNA sequencing (ChIP-seq is a prevailing methodology used to investigate chromatin-based regulation in biological systems such as human disease, but the lack of an empirical methodology to enable normalization among experiments has limited the precision and usefulness of this technique. Here, we describe a method called ChIP with reference exogenous genome (ChIP-Rx that allows one to perform genome-wide quantitative comparisons of histone modification status across cell populations using defined quantities of a reference epigenome. ChIP-Rx enables the discovery and quantification of dynamic epigenomic profiles across mammalian cells that would otherwise remain hidden using traditional normalization methods. We demonstrate the utility of this method for measuring epigenomic changes following chemical perturbations and show how reference normalization of ChIP-seq experiments enables the discovery of disease-relevant changes in histone modification occupancy.

  8. A theoretical study of CH4 dissociation on pure and gold-alloyed Ni(111) surfaces

    DEFF Research Database (Denmark)

    Kratzer, P.; Hammer, Bjørk; Nørskov, Jens Kehlet

    1996-01-01

    We present a density functional theory study of the first step of CH4 adsorption on the Ni(111) surface, dissociation into adsorbed CH3 and H. The rupture of the C-H bond occurs preferentially on top of a Ni atom, with a dissociation barrier of about 100 kJ/mol (including zero point corrections......). The transition state involves considerable internal excitation of the molecule. The active C-H bond is both stretched to 1.6 Angstrom and tilted relative to the methyl group. A normal mode analysis shows that the reaction coordinate is mainly a C-H stretch, while the orientation of the C-H bond relative...... to the surface is responsible for the highest real mode. Alloying the surface with gold also affects the reactivity of the Ni atoms on adjacent surface sites. The dissociation barrier is increased by 16 and 38 kJ/mol for a Ni atom with one or two gold neighbors, respectively. We attribute these changes...

  9. Methane Production by Seagrass Ecosystems in the Red Sea

    KAUST Repository

    Garcias Bonet, Neus; Duarte, Carlos M.

    2017-01-01

    Atmospheric methane (CH) is the second strongest greenhouse gas and it is emitted to the atmosphere naturally by different sources. It is crucial to define the dimension of these natural emissions in order to forecast changes in atmospheric CH mixing ratio in future scenarios. However, CH emissions by seagrass ecosystems in shallow marine coastal systems have been neglected although their global extension. Here we quantify the CH production rates of seagrass ecosystems in the Red Sea. We measured changes in CH concentration and its isotopic signature by cavity ring-down spectroscopy on chambers containing sediment and plants. We detected CH production in all the seagrass stations with an average rate of 85.09 ± 27.80 μmol CH m d. Our results show that there is no seasonal or daily pattern in the CH production rates by seagrass ecosystems in the Red Sea. Taking in account the range of global estimates for seagrass coverage and the average seagrass CH production, the global CH production and emission by seagrass ecosystems could range from 0.09 to 2.7 Tg yr. Because CH emission by seagrass ecosystems had not been included in previous global CH budgets, our estimate would increase the contribution of marine global emissions, hitherto estimated at 9.1 Tg yr, by about 30%. Thus, the potential contribution of seagrass ecosystems to marine CH emissions provides sufficient evidence of the relevance of these fluxes as to include seagrass ecosystems in future assessments of the global CH budgets.

  10. Methane Production by Seagrass Ecosystems in the Red Sea

    KAUST Repository

    Garcias Bonet, Neus

    2017-11-07

    Atmospheric methane (CH) is the second strongest greenhouse gas and it is emitted to the atmosphere naturally by different sources. It is crucial to define the dimension of these natural emissions in order to forecast changes in atmospheric CH mixing ratio in future scenarios. However, CH emissions by seagrass ecosystems in shallow marine coastal systems have been neglected although their global extension. Here we quantify the CH production rates of seagrass ecosystems in the Red Sea. We measured changes in CH concentration and its isotopic signature by cavity ring-down spectroscopy on chambers containing sediment and plants. We detected CH production in all the seagrass stations with an average rate of 85.09 ± 27.80 μmol CH m d. Our results show that there is no seasonal or daily pattern in the CH production rates by seagrass ecosystems in the Red Sea. Taking in account the range of global estimates for seagrass coverage and the average seagrass CH production, the global CH production and emission by seagrass ecosystems could range from 0.09 to 2.7 Tg yr. Because CH emission by seagrass ecosystems had not been included in previous global CH budgets, our estimate would increase the contribution of marine global emissions, hitherto estimated at 9.1 Tg yr, by about 30%. Thus, the potential contribution of seagrass ecosystems to marine CH emissions provides sufficient evidence of the relevance of these fluxes as to include seagrass ecosystems in future assessments of the global CH budgets.

  11. Adsorption of CH{sub 4} on nitrogen- and boron-containing carbon models of coal predicted by density-functional theory

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Xiao-Qiang [College of Chemistry, Key Lab of Green Chemistry and Technology in Ministry of Education, Sichuan University, Chengdu 610064 (China); Xue, Ying, E-mail: yxue@scu.edu.cn [College of Chemistry, Key Lab of Green Chemistry and Technology in Ministry of Education, Sichuan University, Chengdu 610064 (China); Tian, Zhi-Yue; Mo, Jing-Jing; Qiu, Nian-Xiang [College of Chemistry, Key Lab of Green Chemistry and Technology in Ministry of Education, Sichuan University, Chengdu 610064 (China); Chu, Wei [Department of Chemical Engineering, Sichuan University, Chengdu 610065 (China); Xie, He-Ping [Key Laboratory of Energy Engineering Safety and Mechanics on Disasters, The Ministry of Education, Sichuan University, Chengdu 610065 (China)

    2013-11-15

    Graphene doped by nitrogen (N) and/or boron (B) is used to represent the surface models of coal with the structural heterogeneity. Through the density functional theory (DFT) calculations, the interactions between coalbed methane (CBM) and coal surfaces have been investigated. Several adsorption sites and orientations of methane (CH{sub 4}) on graphenes were systematically considered. Our calculations predicted adsorption energies of CH{sub 4} on graphenes of up to −0.179 eV, with the strongest binding mode in which three hydrogen atoms of CH{sub 4} direct to graphene surface, observed for N-doped graphene, compared to the perfect (−0.154 eV), B-doped (−0.150 eV), and NB-doped graphenes (−0.170 eV). Doping N in graphene increases the adsorption energies of CH{sub 4}, but slightly reduced binding is found when graphene is doped by B. Our results indicate that all of graphenes act as the role of a weak electron acceptor with respect to CH{sub 4}. The interactions between CH{sub 4} and graphenes are the physical adsorption and slightly depend upon the adsorption sites on graphenes and the orientations of methane as well as the electronegativity of dopant atoms in graphene.

  12. Changes of global terrestrial carbon budget and major drivers in recent 30 years simulated using the remote sensing driven BEPS model

    Science.gov (United States)

    Ju, W.; Chen, J.; Liu, R.; Liu, Y.

    2013-12-01

    The process-based Boreal Ecosystem Productivity Simulator (BEPS) model was employed in conjunction with spatially distributed leaf area index (LAI), land cover, soil, and climate data to simulate the carbon budget of global terrestrial ecosystems during the period from 1981 to 2008. The BEPS model was first calibrated and validated using gross primary productivity (GPP), net primary productivity (NPP), and net ecosystem productivity (NEP) measured in different ecosystems across the word. Then, four global simulations were conducted at daily time steps and a spatial resolution of 8 km to quantify the global terrestrial carbon budget and to identify the relative contributions of changes in climate, atmospheric CO2 concentration, and LAI to the global terrestrial carbon sink. The long term LAI data used to drive the model was generated through fusing Moderate Resolution Imaging Spectroradiometer (MODIS) and historical Advanced Very High Resolution Radiometer (AVHRR) data pixel by pixel. The meteorological fields were interpolated from the 0.5° global daily meteorological dataset produced by the land surface hydrological research group at Princeton University. The results show that the BEPS model was able to simulate carbon fluxes in different ecosystems. Simulated GPP, NPP, and NEP values and their temporal trends exhibited distinguishable spatial patterns. During the period from 1981 to 2008, global terrestrial ecosystems acted as a carbon sink. The averaged global totals of GPP NPP, and NEP were 122.70 Pg C yr-1, 56.89 Pg C yr-1, and 2.76 Pg C yr-1, respectively. The global totals of GPP and NPP increased greatly, at rates of 0.43 Pg C yr-2 (R2=0.728) and 0.26 Pg C yr-2 (R2=0.709), respectively. Global total NEP did not show an apparent increasing trend (R2= 0.036), averaged 2.26 Pg C yr-1, 3.21 Pg C yr-1, and 2.72 Pg C yr-1 for the periods from 1981 to 1989, from 1990 to 1999, and from 2000 to 2008, respectively. The magnitude and temporal trend of global

  13. Probing the global potential energy minimum of (CH2O)2: THz absorption spectrum of (CH2O)2 in solid neon and para-hydrogen.

    Science.gov (United States)

    Andersen, J; Voute, A; Mihrin, D; Heimdal, J; Berg, R W; Torsson, M; Wugt Larsen, R

    2017-06-28

    The true global potential energy minimum configuration of the formaldehyde dimer (CH 2 O) 2 , including the presence of a single or a double weak intermolecular CH⋯O hydrogen bond motif, has been a long-standing subject among both experimentalists and theoreticians as two different energy minima conformations of C s and C 2h symmetry have almost identical energies. The present work demonstrates how the class of large-amplitude hydrogen bond vibrational motion probed in the THz region provides excellent direct spectroscopic observables for these weak intermolecular CH⋯O hydrogen bond motifs. The combination of concentration dependency measurements, observed isotopic spectral shifts associated with H/D substitutions and dedicated annealing procedures, enables the unambiguous assignment of three large-amplitude infrared active hydrogen bond vibrational modes for the non-planar C s configuration of (CH 2 O) 2 embedded in cryogenic neon and enriched para-hydrogen matrices. A (semi)-empirical value for the change of vibrational zero-point energy of 5.5 ± 0.3 kJ mol -1 is proposed for the dimerization process. These THz spectroscopic observations are complemented by CCSD(T)-F12/aug-cc-pV5Z (electronic energies) and MP2/aug-cc-pVQZ (force fields) electronic structure calculations yielding a (semi)-empirical value of 13.7 ± 0.3 kJ mol -1 for the dissociation energy D 0 of this global potential energy minimum.

  14. What affects CH4/CO2 ratio in cow’s breath

    DEFF Research Database (Denmark)

    Hellwing, Anne Louise Frydendahl; Weisbjerg, Martin Riis; Madsen, Jørgen

    2013-01-01

    under farm management control. CO2 is released largely from microbial decay or burning of plant litter and soil organic matter. CH4 is produced when organic materials decompose under anoxic conditions, notably from fermentative digestion by ruminant livestock, stored manures, wetlands and rice grown...

  15. Experimental measurements of vapor-liquid equilibria of the H2O + CO2 + CH4 ternary system

    Science.gov (United States)

    Qin, J.; Rosenbauer, R.J.; Duan, Zhenhao

    2008-01-01

    Reported are the experimental measurements on vapor-liquid equilibria in the H2O + CO2 + CH4 ternary system at temperatures from (324 to 375) K and pressures from (10 to 50) MPa. The results indicate that the CH4 solubility in the ternary mixture is about 10 % to 40 % more than that calculated by interpolation from the Henry's law constants of the binary system, H2O + CH4, and the solubility of CO2 is 6 % to 20 % more than what is calculated by the interpolation from the Henry's law constants of the binary mixture, H 2O + CO2. ?? 2008 American Chemical Society.

  16. Methane airborne measurements and comparison to global models during BARCA

    Science.gov (United States)

    Beck, Veronika; Chen, Huilin; Gerbig, Christoph; Bergamaschi, Peter; Bruhwiler, Lori; Houweling, Sander; Röckmann, Thomas; Kolle, Olaf; Steinbach, Julia; Koch, Thomas; Sapart, Célia J.; van der Veen, Carina; Frankenberg, Christian; Andreae, Meinrat O.; Artaxo, Paulo; Longo, Karla M.; Wofsy, Steven C.

    2012-08-01

    Tropical regions, especially the Amazon region, account for large emissions of methane (CH4). Here, we present CH4 observations from two airborne campaigns conducted within the BARCA (Balanço Atmosférico Regional de Carbono na Amazônia) project in the Amazon basin in November 2008 (end of the dry season) and May 2009 (end of the wet season). We performed continuous measurements of CH4 onboard an aircraft for the first time in the Amazon region, covering the whole Amazon basin with over 150 vertical profiles between altitudes of 500 m and 4000 m. The observations support the finding of previous ground-based, airborne, and satellite measurements that the Amazon basin is a large source of atmospheric CH4. Isotope analysis verified that the majority of emissions can be attributed to CH4 emissions from wetlands, while urban CH4 emissions could be also traced back to biogenic origin. A comparison of five TM5 based global CH4 inversions with the observations clearly indicates that the inversions using SCIAMACHY observations represent the BARCA observations best. The calculated CH4 flux estimate obtained from the mismatch between observations and TM5-modeled CH4 fields ranges from 36 to 43 mg m-2 d-1 for the Amazon lowland region.

  17. Feeding the world's increasing population while limiting climate change impacts: linking N2O and CH4 emissions from agriculture to population growth

    International Nuclear Information System (INIS)

    Beek, Christy L. van; Meerburg, Bastiaan G.; Schils, Rene L.M.; Verhagen, Jan; Kuikman, Peter J.

    2010-01-01

    The global demand for agricultural products, including food, is rapidly increasing due to population growth and shifts in consumption patterns. The required increase in agricultural production is predominantly to be achieved in countries with relatively low agricultural production levels at present. These are mainly developing countries and countries in transition, the so-called non-Annex I countries of the UNFCCC. However, intensification of agricultural production systems is currently closely linked to high emissions of greenhouse gases notably nitrous oxide (N 2 O) and methane (CH 4 ). In this paper the relations between population growth, agricultural development and emissions of N 2 O and CH 4 were assessed for 10 non-Annex I countries, viz. China, India, Vietnam, Brazil, Argentina, Mexico, Mongolia, Nigeria, Tanzania and South Africa. We combined FAO data on agricultural production levels, CENSUS data on population statistics and EDGAR data on N 2 O and CH 4 emissions. The projected trends in agricultural production indicate that emissions of N 2 O and CH 4 are expected to increase rapidly in the coming years and will level off from 2040 onwards. The results confirm the positive relation between population increase and increased emissions from agricultural activities for most countries. However, for some countries (South Africa, China and Mexico) this relation was weak or absent. Although numerous factors (e.g. changes in international trade) may have scattered the relation and we were unable to explain this decoupling, it suggests that population growth can be possible without additional emissions. The variation between the different countries and farming systems is however large and mitigation measures at farm-level should be tailored to the wide diversity in environmental conditions, regional customs and farming systems.

  18. Fluid properties control degassing or storage of abiogenic CH4 during slab exhumation: the fluid inclusion record from the Western Alps.

    Science.gov (United States)

    Ferrando, S.; Castelli, D.; Frezzotti, M. L.

    2017-12-01

    Abiogenic CH4 can be produced by interaction between carbonates and reducing fluids derived from the hydration of ultramafics (e.g., mantle peridotite or HP Ol-serpentinite). This process occurs during slab exhumation because cooling promotes serpentinization of olivine in presence of water (Fo + H2O = Atg + Brc and the linked reactions: Fa + H2O = Fe-Atg + Mag + H2 and Atg + CaCO3 + H2 = Di + Brc + CH4 + H2O) at ca. 500-375°C (P=2.0-0.2 GPa). Experiments in the CH4-H2O-NaCl system indicate that, at these conditions, fluids are immiscible even for very low salinity (ca. 3 wt%) and that the NaCl content in the aqueous part of the fluid increases with temperature whereas the CH4 content in the gaseous part shows an opposite trend (Lamb et al., 2002; Li, 2017).In HP rodingite from the Piemonte ophiolite Zone (W Alps), primary fluid inclusions consisting of a brine (6 wt% CaCl2 + 6 wt% NaCl) with H2 + CH4 ≤ 1 mol % [CH4/(H2+CH4) = 0.37-10] occur in vesuvianite veins that formed at P=0.2 GPa and T=375°C. We interpret them as the aqueous part of an immiscible reducing fluid produced during late Alpine serpentinization of the surrounding ultramafics. Interestingly, CH4-H2 gaseous fluids are never reported in rodingite, whereas early CH4-H2O-H2±graphite and CH4-H2±graphite fluid inclusions, with variable gas-water proportions, trapped in calcite at P≤1.0 GPa and T≤450°C, are recently reported from HP "graphitized" ophicarbonate from the Lanzo peridotite Massif (W Alps; Vitale Brovarone et al., 2017).Both HP ophiolites and partially-serpentinized peridotite massifs are, thus, efficient lithologies to produce CH4 during exhumation. The amount of released CH4 depends on the amount of water available during exhumation. However, when fluids immiscibility occurs, the gaseous-rich part (CH4-H2) of the immiscible fluid produced in ultramafics likely remains confined in the slab because it is less mobile with respect to the aqueous-rich part due to its high dihedral

  19. The Soil Sink for Nitrous Oxide: Trivial Amount but Challenging Question

    Science.gov (United States)

    Davidson, E. A.; Savage, K. E.; Sihi, D.

    2015-12-01

    Net uptake of atmospheric nitrous oxide (N2O) has been observed sporadically for many years. Such observations have often been discounted as measurement error or noise, but they were reported frequently enough to gain some acceptance as valid. The advent of fast response field instruments with good sensitivity and precision has permitted confirmation that some soils can be small sinks of N2O. With regards to "closing the global N2O budget" the soil sink is trivial, because it is smaller than the error terms of most other budget components. Although not important from a global budget perspective, the existence of a soil sink for atmospheric N2O presents a fascinating challenge for understanding the physical, chemical, and biological processes that explain the sink. Reduction of N2O by classical biological denitrification requires reducing conditions generally found in wet soil, and yet we have measured the N2O sink in well drained soils, where we also simultaneously measure a sink for atmospheric methane (CH4). Co-occurrence of N2O reduction and CH4 oxidation would require a broad range of microsite conditions within the soil, spanning high and low oxygen concentrations. Abiotic sinks for N2O or other biological processes that consume N2O could exist, but have not yet been identified. We are attempting to simulate processes of diffusion of N2O, CH4, and O2 from the atmosphere and within a soil profile to determine if classical biological N2O reduction and CH4 oxidation at rates consistent with measured fluxes are plausible.

  20. Hot filament-dissociation of (CH3)3SiH and (CH3)4Si, probed by vacuum ultra violet laser time of flight mass spectroscopy.

    Science.gov (United States)

    Sharma, Ramesh C; Koshi, Mitsuo

    2006-11-01

    The decomposition of trimethylsilane and tetramethylsilane has been investigated for the first time, using hot wire (catalytic) at various temperatures. Trimethylsilane is catalytic-dissociated in these species SiH(2), CH(3)SiH, CH(3), CH(2)Si. Time of flight mass spectroscopy signal of these species are linearly increasing with increasing catalytic-temperature. Time of flight mass spectroscopy (TOFMS) signals of (CH(3))(3)SiH and photodissociated into (CH(3))(2)SiH are decreasing with increasing hot filament temperature. TOFMS signal of (CH(3))(4)Si is decreasing with increasing hot wire temperature, but (CH(3))(3)Si signal is almost constant with increasing the temperature. We calculated activation energies of dissociated species of the parental molecules for fundamental information of reaction kinetics for the first time. Catalytic-dissociation of trimethylsilane, and tetramethylsilane single source time of flight coupled single photon VUV (118 nm) photoionization collisionless radicals at temperature range of tungsten filament 800-2360 K. The study is focused to understand the fundamental information on reaction kinetics of these molecules at hot wire temperature, and processes of catalytic-chemical vapour deposition (Cat-CVD) technique which could be implemented in amorphous and crystalline SiC semiconductors thin films.

  1. Compact Solar Spectrometer Column CO2, and CH4 Observations: Performance Evaluation at Multiple North American TCCON Sites

    Science.gov (United States)

    Parker, H. A.; Hedelius, J.; Viatte, C.; Wunch, D.; Wennberg, P. O.; Chen, J.; Wofsy, S.; Jones, T.; Franklin, J.; Dubey, M. K.; Roehl, C. M.; Podolske, J. R.; Hillyard, P. W.; Iraci, L. T.

    2015-12-01

    Measurement, reporting and verification (MRV) of anthropogenic emissions and natural sources and sinks of carbon dioxide (CO2) and methane (CH4) are crucial to predict climate change and develop transparent accounting policies to contain climate forcing. Remote sensing technologies are monitoring column averaged dry air mole fractions of CO2 and CH4 (XCO2 & XCH4) from ground and space (OCO-2 and GOSAT) with solar spectroscopy enabling direct MRV. However, current ground based coverage is sparse due to the need for large and expensive high-resolution spectrometers that are part of the Total Column Carbon Observing Network (TCCON, Bruker 125HR). This limits our MRV and satellite validation abilities, both regionally and globally. There are striking monitoring gaps in Asia, South America and Africa where the CO2 emissions are growing and there is a large uncertainty in fluxes from land use change, biomass burning and rainforest vulnerability. To fill this gap we evaluate the precision, accuracy and stability of compact, affordable and easy to use low-resolution spectrometers (Bruker EM27/SUN) by comparing with XCO2 and XCH4 retrieved from much larger high-resolution TCCON instruments. As these instruments will be used in a variety of locations, we evaluate their performance by comparing with 2 previous and 4 current United States TCCON sites in different regions up to 2700 km apart. These sites range from polluted to unpolluted, latitudes of 32 to 46°N, and altitudes of 230 to 2241 masl. Comparisons with some of these sites cover multiple years allowing assessment of the EM27/SUN performance not only in various regions, but also over an extended period of time and with different seasonal influences. Results show that our 2 EM27/SUN instruments capture the diurnal variability of the aforementioned constituents very well, but with offsets from TCCON and long-term variability which may be due in part to the extensive movement these spectrometers were subjected to. These

  2. Emerging role of wetland methane emissions in driving 21st century climate change.

    Science.gov (United States)

    Zhang, Zhen; Zimmermann, Niklaus E; Stenke, Andrea; Li, Xin; Hodson, Elke L; Zhu, Gaofeng; Huang, Chunlin; Poulter, Benjamin

    2017-09-05

    Wetland methane (CH 4 ) emissions are the largest natural source in the global CH 4 budget, contributing to roughly one third of total natural and anthropogenic emissions. As the second most important anthropogenic greenhouse gas in the atmosphere after CO 2 , CH 4 is strongly associated with climate feedbacks. However, due to the paucity of data, wetland CH 4 feedbacks were not fully assessed in the Intergovernmental Panel on Climate Change Fifth Assessment Report. The degree to which future expansion of wetlands and CH 4 emissions will evolve and consequently drive climate feedbacks is thus a question of major concern. Here we present an ensemble estimate of wetland CH 4 emissions driven by 38 general circulation models for the 21st century. We find that climate change-induced increases in boreal wetland extent and temperature-driven increases in tropical CH 4 emissions will dominate anthropogenic CH 4 emissions by 38 to 56% toward the end of the 21st century under the Representative Concentration Pathway (RCP2.6). Depending on scenarios, wetland CH 4 feedbacks translate to an increase in additional global mean radiative forcing of 0.04 W·m -2 to 0.19 W·m -2 by the end of the 21st century. Under the "worst-case" RCP8.5 scenario, with no climate mitigation, boreal CH 4 emissions are enhanced by 18.05 Tg to 41.69 Tg, due to thawing of inundated areas during the cold season (December to May) and rising temperature, while tropical CH 4 emissions accelerate with a total increment of 48.36 Tg to 87.37 Tg by 2099. Our results suggest that climate mitigation policies must consider mitigation of wetland CH 4 feedbacks to maintain average global warming below 2 °C.

  3. [CH4 emission features of leading super-rice varieties and their relationships with the varieties growth characteristics in Yangtze Delta of China].

    Science.gov (United States)

    Yan, Xiao-Jun; Wang, Li-Li; Jiang, Yu; Deng, Ai-Xing; Tian, Yun-Lu; Zhang, Wei-Jian

    2013-09-01

    A pot experiment was conducted to study the CH4 emission features of fourteen leading super-rice varieties (six Japonica rice varieties and eight Indica hybrid rice varieties) and their relationships with the varieties growth characteristics in Yangtze Delta. Two distinct peaks of CH4 emission were detected during the entire growth period of the varieties, one peak occurred at full-tillering stage, and the other appeared at booting stage. The average total CH4 emission of Japonica rice varieties was 37.6% higher than that of the Indica hybrid rice varieties (Price types occurred at the post-anthesis phase. For all the varieties, there was a significant positive correlation between the total CH4 emission and the maximum leaf area, but the correlations between the CH4 emission and the other growth characteristics varied with variety type. The total CH4 emission of Japonica rice varieties had a significant positive correlation with plant height, while the correlations between the total CH4 emission of Indica hybrid rice varieties and their plant height were not significant. The total CH4 emission of Indica hybrid rice varieties had significant negative correlations with the total aboveground biomass, grain yield, and harvest index, but the correlations were not significant for Japonica rice varieties. The lower CH4 emission of Indica hybrid rice varieties was likely due to their significantly higher root biomass, as compared with Japonica rice varieties.

  4. CH-TRU Waste Content Codes (CH-TRUCON)

    International Nuclear Information System (INIS)

    2007-01-01

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes 'shipping categories' that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the 'General Case,' which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for 'Close-Proximity Shipments' (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for 'Controlled Shipments

  5. CH-TRU Waste Content Codes (CH-TRUCON)

    International Nuclear Information System (INIS)

    2006-01-01

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes 'shipping categories' that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the 'General Case,' which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for 'Close-Proximity Shipments' (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for 'Controlled Shipments

  6. CH-TRU Waste Content Codes (CH-TRUCON)

    International Nuclear Information System (INIS)

    2005-01-01

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes 'shipping categories' that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the 'General Case,' which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for 'Close-Proximity Shipments' (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for 'Controlled Shipments

  7. CH-TRU Waste Content Codes (CH-TRUCON)

    International Nuclear Information System (INIS)

    2004-01-01

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes 'shipping categories' that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the 'General Case,' which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for 'Close-Proximity Shipments' (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for 'Controlled Shipments

  8. CH-TRU Waste Content Codes (CH-TRUCON)

    International Nuclear Information System (INIS)

    2008-01-01

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes 'shipping categories' that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the 'General Case,' which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for 'Close-Proximity Shipments' (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for 'Controlled Shipments

  9. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2006-09-15

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  10. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2005-05-01

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  11. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2007-02-15

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  12. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2005-06-20

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  13. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2006-06-20

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  14. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2005-01-15

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codesand corresponding shipping categories for "Controlled Shipments

  15. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2006-12-20

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  16. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2006-08-15

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  17. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2006-01-18

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  18. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2004-10-01

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  19. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2005-03-15

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  20. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2007-09-20

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  1. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2007-08-15

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  2. CH-TRU Waste Content Codes (CH TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2004-12-01

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  3. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2005-11-20

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  4. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2005-12-15

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  5. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2005-01-30

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  6. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2005-08-15

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  7. CH-TRU Waste Content Codes (CH-TRUCON)

    Energy Technology Data Exchange (ETDEWEB)

    Washington TRU Solutions LLC

    2007-06-15

    The CH-TRU Waste Content Codes (CH-TRUCON) document describes the inventory of the U.S. Department of Energy (DOE) CH-TRU waste within the transportation parameters specified by the Contact-Handled Transuranic Waste Authorized Methods for Payload Control (CH-TRAMPAC). The CH-TRAMPAC defines the allowable payload for the Transuranic Package Transporter-II (TRUPACT-II) and HalfPACT packagings. This document is a catalog of TRUPACT-II and HalfPACT authorized contents and a description of the methods utilized to demonstrate compliance with the CH-TRAMPAC. A summary of currently approved content codes by site is presented in Table 1. The CH-TRAMPAC describes "shipping categories" that are assigned to each payload container. Multiple shipping categories may be assigned to a single content code. A summary of approved content codes and corresponding shipping categories is provided in Table 2, which consists of Tables 2A, 2B, and 2C. Table 2A provides a summary of approved content codes and corresponding shipping categories for the "General Case," which reflects the assumption of a 60-day shipping period as described in the CH-TRAMPAC and Appendix 3.4 of the CH-TRU Payload Appendices. For shipments to be completed within an approximately 1,000-mile radius, a shorter shipping period of 20 days is applicable as described in the CH-TRAMPAC and Appendix 3.5 of the CH-TRU Payload Appendices. For shipments to WIPP from Los Alamos National Laboratory (LANL), Nevada Test Site, and Rocky Flats Environmental Technology Site, a 20-day shipping period is applicable. Table 2B provides a summary of approved content codes and corresponding shipping categories for "Close-Proximity Shipments" (20-day shipping period). For shipments implementing the controls specified in the CH-TRAMPAC and Appendix 3.6 of the CH-TRU Payload Appendices, a 10-day shipping period is applicable. Table 2C provides a summary of approved content codes and corresponding shipping categories for "Controlled Shipments

  8. Presumed PDF modeling of microjet assisted CH4–H2/air turbulent flames

    International Nuclear Information System (INIS)

    Chouaieb, Sirine; Kriaa, Wassim; Mhiri, Hatem; Bournot, Philippe

    2016-01-01

    Highlights: • Microjet assisted CH 4 –H 2 /air turbulent flames are numerically investigated. • Temperature, species and soot are well predicted by the Presumed PDF model. • An inner flame is identified due to the microjet presence. • The addition of hydrogen to the microjet assisted flames enhances mixing. • Soot emission is reduced by 36% for a 10% enriched microjet assisted flame. - Abstract: The characteristics of microjet assisted CH 4 –H 2 /air flames in a turbulent mode are numerically investigated. Simulations are performed using the Computational Fluid Dynamics code Fluent. The Presumed PDF and the Discrete Ordinates models are considered respectively for combustion and radiation modeling. The k–ε Realizable model is adopted as a turbulence closure model. The Tesner model is used to calculate soot particle quantities. In the first part of this paper, the Presumed PDF model is compared to the Eddy Dissipation model and to slow chemistry combustion models from literature. Results show that the Presumed PDF model predicts correctly thermal and species fields, as well as soot formation. The effect of hydrogen enrichment on CH 4 /air confined flames under the addition of an air microjet is investigated in the second part of this work. The found results show that an inner flame was identified due to the air microjet for the CH 4 –H 2 /air flames. Moreover, the increase of hydrogen percentage in the fuel mixture leads to mixing enhancement and consequently to considerable soot emission reduction.

  9. N{sub 2}O and CH{sub 4} Emission from Wastewater Collection and Treatment Systems (GWRC). Technical Report

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2011-11-15

    The Global Water Research Coalition (GWRC) is an international organisation that is dedicated to the exchange and generation of knowledge to support sustainable development and management of the urban water cycle. The research agenda is developed by the member organisations of the GWRC and reflects their priorities and recognises global trends and drivers that affect the urban water cycle. The present research agenda includes Climate Change as one of the priorities areas. This research area comprises topics related to the possible impact of climate change on the urban water sector as well as the possible contribution to climate change by the urban water sector via the direct and indirect emission of greenhouse gasses (GHG). The objective of this joint effort was to collect and develop knowledge needed to understand and manage the emission of N{sub 2}O (nitrous oxide) and CH{sub 4} (methane) by wastewater collection and treatment systems. Starting with a kick-off meeting in Vienna in September 2008, the GWRC members involved in this activity have bundled their individual research programs on this topic, aligned methodologies used and exchanged and discussed the resulting information of the programs and developed additional actions where needed. The outcomes were reviewed and discussed at a final workshop in Montreal in September 2010. These activities have resulted in two reports: the State of the Science report which presents an overview of the current knowledge and know-how regarding the emissions of N{sub 2}O and CH{sub 4} by wastewater collection and treatment systems and this Technical Report which includes all the details, facts and figures of the underlying studies used to develop the State of the Science report. For the State of Science Report a separate record has been prepared.

  10. Long Path Quantum Cascade Laser Based Sensor for Environment Sensing/Ambient Detection of CH4 and N2O

    Science.gov (United States)

    Castillo, P. C.; Sydoryk, I.; Gross, B.; Moshary, F.

    2013-12-01

    Methane (CH4) and Nitrous Oxide (N2O) are long-lived greenhouse gases in the atmosphere with significant global warming effects. These gases also are known to be produced in a number of anthropogenic settings such as manure management systems, which releases substantial GHGs and is mandated by the EPA to provide continuous monitoring. In addition, natural gas leaks in urban areas is another source of strong spatially inhomogeneous methane emissions Most open path methods for quantitative detection of trace gases utilize either Fourier Transform Spectrometer (FTIR) or near-IR differential optical absorption spectroscopy (DOAS). Although, FTIR is suitable for ambient air monitoring measurement of more abundant gases such as CO2 and H20 etc., the lack of spectral resolution makes the retrieval of weaker absorbing features such as N20 more difficult. On the other hand, conventional DOAS systems can be large and impractical. As an alternative, we illustrate a robust portable quantum cascade laser (QCL) approach for simultaneous detection of CH4 and N2O. In particular, gas spectra were recorded by ultrafast pulse intensity (thermal) chirp tuning over the 1299 - 1300cm-1 spectral window. Etalon measurements insure stable tuning was obtained. To deal with multiple species, a LSQ spectral fitting approach was used which accounted for both the overlapping trace gases , background water vapor as well as detector drift and calibration. In summary, ambient concentrations of CH4 with and N2O with accuracy < 1% was obtained on the order of 5ms using optical paths of 500 m path length. In addition, unattended long term operation was demonstrated and validations using other sensors when possible were shown to be consistent. The system accuracy is limited by systemic errors, which are still being explored.

  11. Soil Methanotrophy Model (MeMo v1.0: a process-based model to quantify global uptake of atmospheric methane by soil

    Directory of Open Access Journals (Sweden)

    F. Murguia-Flores

    2018-06-01

    Full Text Available Soil bacteria known as methanotrophs are the sole biological sink for atmospheric methane (CH4, a potent greenhouse gas that is responsible for  ∼  20 % of the human-driven increase in radiative forcing since pre-industrial times. Soil methanotrophy is controlled by a plethora of factors, including temperature, soil texture, moisture and nitrogen content, resulting in spatially and temporally heterogeneous rates of soil methanotrophy. As a consequence, the exact magnitude of the global soil sink, as well as its temporal and spatial variability, remains poorly constrained. We developed a process-based model (Methanotrophy Model; MeMo v1.0 to simulate and quantify the uptake of atmospheric CH4 by soils at the global scale. MeMo builds on previous models by Ridgwell et al. (1999 and Curry (2007 by introducing several advances, including (1 a general analytical solution of the one-dimensional diffusion–reaction equation in porous media, (2 a refined representation of nitrogen inhibition on soil methanotrophy, (3 updated factors governing the influence of soil moisture and temperature on CH4 oxidation rates and (4 the ability to evaluate the impact of autochthonous soil CH4 sources on uptake of atmospheric CH4. We show that the improved structural and parametric representation of key drivers of soil methanotrophy in MeMo results in a better fit to observational data. A global simulation of soil methanotrophy for the period 1990–2009 using MeMo yielded an average annual sink of 33.5 ± 0.6 Tg CH4 yr−1. Warm and semi-arid regions (tropical deciduous forest and open shrubland had the highest CH4 uptake rates of 602 and 518 mg CH4 m−2 yr−1, respectively. In these regions, favourable annual soil moisture content ( ∼  20 % saturation and low seasonal temperature variations (variations  <   ∼  6 °C provided optimal conditions for soil methanotrophy and soil–atmosphere gas exchange

  12. CH4/air homogeneous autoignition: A comparison of two chemical kinetics mechanisms

    KAUST Repository

    Tingas, Efstathios Al.; Manias, Dimitris M.; Sarathy, Mani; Goussis, Dimitris A.

    2018-01-01

    Reactions contributing to the generation of the explosive time scale that characterise autoignition of homogeneous stoichiometric CH4/air mixture are identified using two different chemical kinetics models; the well known GRI-3.0 mechanism (53

  13. Development of a method for estimating total CH{sub 4} emission from rice paddies in Japan using the DNDC-Rice model

    Energy Technology Data Exchange (ETDEWEB)

    Katayanagi, Nobuko [National Institute for Agro-Environmental Sciences, 3-1-3 Kannondai, Tsukuba, Ibaraki 305-8604 (Japan); Fumoto, Tamon, E-mail: tamon@affrc.go.jp [National Institute for Agro-Environmental Sciences, 3-1-3 Kannondai, Tsukuba, Ibaraki 305-8604 (Japan); Hayano, Michiko [National Institute for Agro-Environmental Sciences, 3-1-3 Kannondai, Tsukuba, Ibaraki 305-8604 (Japan); Kyushu Okinawa Agricultural Research Center, National Agriculture and Food Research Organization, Anno 1742-1, Nishinoomote, Kagoshima 891-3102 (Japan); Takata, Yusuke; Kuwagata, Tsuneo; Shirato, Yasuhito [National Institute for Agro-Environmental Sciences, 3-1-3 Kannondai, Tsukuba, Ibaraki 305-8604 (Japan); Sawano, Shinji [Forestry and Forest Products Research Institute (FFPRI), 1 Matsunosato, Tsukuba, Ibaraki 305-8687 (Japan); Kajiura, Masako; Sudo, Shigeto; Ishigooka, Yasushi; Yagi, Kazuyuki [National Institute for Agro-Environmental Sciences, 3-1-3 Kannondai, Tsukuba, Ibaraki 305-8604 (Japan)

    2016-03-15

    Methane (CH{sub 4}) is a greenhouse gas, and paddy fields are one of its main anthropogenic emission sources. To mitigate this emission based on effective management measures, CH{sub 4} emission from paddy fields must be quantified at a national scale. In Japan, country-specific emission factors have been applied since 2003 to estimate national CH{sub 4} emission from paddy fields. However, this method cannot account for the effects of weather conditions and temporal variability of nitrogen fertilizer and organic matter application rates; thus, the estimated emission is highly uncertain. To improve the accuracy of national-scale estimates, we calculated country-specific emission factors using the DeNitrification–DeComposition-Rice (DNDC-Rice) model. First, we calculated CH{sub 4} emission from 1981 to 2010 using 986 datasets that included soil properties, meteorological data, and field management data. Using the simulated site-specific emission, we calculated annual mean emission for each of Japan's seven administrative regions, two water management regimes (continuous flooding and conventional mid-season drainage), and three soil drainage rates (slow, moderate, and fast). The mean emission was positively correlated with organic carbon input to the field, and we developed linear regressions for the relationships among the regions, water management regimes, and drainage rates. The regression results were within the range of published observation values for site-specific relationships between CH{sub 4} emission and organic carbon input rates. This suggests that the regressions provide a simplified method for estimating CH{sub 4} emission from Japanese paddy fields, though some modifications can further improve the estimation accuracy. - Highlights: • DNDC-Rice is a process-based model to simulate rice CH{sub 4} emission from rice paddies. • We simulated annual CH{sub 4} emissions from 986 paddy fields in Japan by DNDC-Rice. • Regional means of CH{sub 4

  14. Influence of meteorology and interrelationship with greenhouse gases (CO2 and CH4) at a sub-urban site of India

    Science.gov (United States)

    Sreenivas, G.; Mahesh, P.; Subin, J.; Kanchana, A. L.; Rao, P. V. N.; Dadhwal, V. K.

    2015-12-01

    Atmospheric greenhouse gases (GHGs) such as carbon dioxide (CO2) and methane (CH4) are important climate forcing agents due to their significant impact on the climate system. The present study brings out first continuous measurements of atmospheric GHG's using high precision Los Gatos Research's-greenhouse gas analyser (LGR-GGA) over Shadnagar, a suburban site of Central India during the period 2014. The annual mean of CO2 and CH4 over the study region is found to be 394 ± 2.92 and 1.92 ± 0.07 ppm (mean, μ ± 1 SD, σ) respectively. CO2 and CH4 showed a significant seasonal variation during the study period with maximum (minimum) CO2 observed during Pre-monsoon (Monsoon), while CH4 recorded maximum during post-monsoon and minimum in monsoon. A consistent diurnal mixing ratio of these gases is observed with high (low) during night (afternoon) hours throughout the study period. Influences of prevailing meteorology (air temperature, wind speed, wind direction and relative humidity) on GHG's have also been investigated. CO2 and CH4 showed a strong positive correlation during winter, pre-monsoon, monsoon and post-monsoon with R equal to 0.80, 0.80, 0.61 and 0.72 respectively. It implies the seasonal variations in source-sink mechanisms of CO2 and CH4. Present study also confirms implicitly the presence OH radicals as a major sink of CH4 over the study region.

  15. F-state quenching with CH4 for buffer-gas cooled 171Y b+ frequency standard

    Directory of Open Access Journals (Sweden)

    Y.-Y. Jau

    2015-11-01

    Full Text Available We report that methane, CH4, can be used as an efficient F-state quenching gas for trapped ytterbium ions. The quenching rate coefficient is measured to be (2.8 ± 0.3 × 106 s−1 Torr−1. For applications that use microwave hyperfine transitions of the ground-state 171Y b ions, the CH4 induced frequency shift coefficient and the decoherence rate coefficient are measured as δν/ν = (−3.6 ± 0.1 × 10−6 Torr−1 and 1/T2 = (1.5 ± 0.2 × 105 s−1 Torr−1. In our buffer-gas cooled 171Y b+ microwave clock system, we find that only ≤10−8 Torr of CH4 is required under normal operating conditions to efficiently clear the F-state and maintain ≥85% of trapped ions in the ground state with insignificant pressure shift and collisional decoherence of the clock resonance.

  16. A simple calculation algorithm to separate high-resolution CH4 flux measurements into ebullition and diffusion-derived components

    Science.gov (United States)

    Hoffmann, Mathias; Schulz-Hanke, Maximilian; Garcia Alba, Joana; Jurisch, Nicole; Hagemann, Ulrike; Sachs, Torsten; Sommer, Michael; Augustin, Jürgen

    2016-04-01

    Processes driving methane (CH4) emissions in wetland ecosystems are highly complex. Especially, the separation of CH4 emissions into ebullition and diffusion derived flux components, a perquisite for the mechanistic process understanding and identification of potential environmental driver is rather challenging. We present a simple calculation algorithm, based on an adaptive R-script, which separates open-water, closed chamber CH4 flux measurements into diffusion- and ebullition-derived components. Hence, flux component specific dynamics are revealed and potential environmental driver identified. Flux separation is based on a statistical approach, using ebullition related sudden concentration changes obtained during high resolution CH4 concentration measurements. By applying the lower and upper quartile ± the interquartile range (IQR) as a variable threshold, diffusion dominated periods of the flux measurement are filtered. Subsequently, flux calculation and separation is performed. The algorithm was verified in a laboratory experiment and tested under field conditions, using flux measurement data (July to September 2013) from a flooded, former fen grassland site. Erratic ebullition events contributed 46% to total CH4 emissions, which is comparable to values reported by literature. Additionally, a shift in the diurnal trend of diffusive fluxes throughout the measurement period, driven by the water temperature gradient, was revealed.

  17. Global nitrogen budgets in cereals: A 50-year assessment for maize, rice, and wheat production systems.

    Science.gov (United States)

    Ladha, J K; Tirol-Padre, A; Reddy, C K; Cassman, K G; Verma, Sudhir; Powlson, D S; van Kessel, C; de B Richter, Daniel; Chakraborty, Debashis; Pathak, Himanshu

    2016-01-18

    Industrially produced N-fertilizer is essential to the production of cereals that supports current and projected human populations. We constructed a top-down global N budget for maize, rice, and wheat for a 50-year period (1961 to 2010). Cereals harvested a total of 1551 Tg of N, of which 48% was supplied through fertilizer-N and 4% came from net soil depletion. An estimated 48% (737 Tg) of crop N, equal to 29, 38, and 25 kg ha(-1) yr(-1) for maize, rice, and wheat, respectively, is contributed by sources other than fertilizer- or soil-N. Non-symbiotic N2 fixation appears to be the major source of this N, which is 370 Tg or 24% of total N in the crop, corresponding to 13, 22, and 13 kg ha(-1) yr(-1) for maize, rice, and wheat, respectively. Manure (217 Tg or 14%) and atmospheric deposition (96 Tg or 6%) are the other sources of N. Crop residues and seed contribute marginally. Our scaling-down approach to estimate the contribution of non-symbiotic N2 fixation is robust because it focuses on global quantities of N in sources and sinks that are easier to estimate, in contrast to estimating N losses per se, because losses are highly soil-, climate-, and crop-specific.

  18. Inventory of anthropogenic methane emissions in mainland China from 1980 to 2010

    Science.gov (United States)

    Peng, Shushi; Piao, Shilong; Bousquet, Philippe; Ciais, Philippe; Li, Bengang; Lin, Xin; Tao, Shu; Wang, Zhiping; Zhang, Yuan; Zhou, Feng

    2016-11-01

    Methane (CH4) has a 28-fold greater global warming potential than CO2 over 100 years. Atmospheric CH4 concentration has tripled since 1750. Anthropogenic CH4 emissions from China have been growing rapidly in the past decades and contribute more than 10 % of global anthropogenic CH4 emissions with large uncertainties in existing global inventories, generally limited to country-scale statistics. To date, a long-term CH4 emission inventory including the major sources sectors and based on province-level emission factors is still lacking. In this study, we produced a detailed annual bottom-up inventory of anthropogenic CH4 emissions from the eight major source sectors in China for the period 1980-2010. In the past 3 decades, the total CH4 emissions increased from 24.4 [18.6-30.5] Tg CH4 yr-1 in 1980 (mean [minimum-maximum of 95 % confidence interval]) to 44.9 [36.6-56.4] Tg CH4 yr-1 in 2010. Most of this increase took place in the 2000s decade with averaged yearly emissions of 38.5 [30.6-48.3] Tg CH4 yr-1. This fast increase of the total CH4 emissions after 2000 is mainly driven by CH4 emissions from coal exploitation. The largest contribution to total CH4 emissions also shifted from rice cultivation in 1980 to coal exploitation in 2010. The total emissions inferred in this work compare well with the EPA inventory but appear to be 36 and 18 % lower than the EDGAR4.2 inventory and the estimates using the same method but IPCC default emission factors, respectively. The uncertainty of our inventory is investigated using emission factors collected from state-of-the-art published literatures. We also distributed province-scale emissions into 0.1° × 0.1° maps using socioeconomic activity data. This new inventory could help understanding CH4 budgets at regional scale and guiding CH4 mitigation policies in China.

  19. Provider Behavior Under Global Budgeting and Policy Responses

    Directory of Open Access Journals (Sweden)

    Chao-Kai Chang MD, PhD

    2015-08-01

    Full Text Available Third-party payer systems are consistently associated with health care cost escalation. Taiwan’s single-payer, universal coverage National Health Insurance (NHI adopted global budgeting (GB to achieve cost control. This study captures ophthalmologists’ response to GB, specifically service volume changes and service substitution between low-revenue and high-revenue services following GB implementation, the subsequent Bureau of NHI policy response, and the policy impact. De-identified eye clinic claims data for the years 2000, 2005, and 2007 were analyzed to study the changes in Simple Claim Form (SCF claims versus Special Case Claims (SCCs. The 3 study years represent the pre-GB period, post-GB but prior to region-wise service cap implementation period, and the post-service cap period, respectively. Repeated measures multilevel regression analysis was used to study the changes adjusting for clinic characteristics and competition within each health care market. SCF service volume (low-revenue, fixed-price patient visits remained constant throughout the study period, but SCCs (covering services involving variable provider effort and resource use with flexibility for discretionary billing increased in 2005 with no further change in 2007. The latter is attributable to a 30% cap negotiated by the NHI Bureau with the ophthalmology association and enforced by the association. This study demonstrates that GB deployed with ongoing monitoring and timely policy responses that are designed in collaboration with professional stakeholders can contain costs in a health insurance–financed health care system.

  20. Soil-atmospheric exchange of CO2, CH4, and N2O in three subtropical forest ecosystems in southern China

    Science.gov (United States)

    Tang, X.; Liu, S.; Zhou, G.; Zhang, Dongxiao; Zhou, C.

    2006-01-01

    The magnitude, temporal, and spatial patterns of soil-atmospheric greenhouse gas (hereafter referred to as GHG) exchanges in forests near the Tropic of Cancer are still highly uncertain. To contribute towards an improvement of actual estimates, soil-atmospheric CO2, CH4, and N2O fluxes were measured in three successional subtropical forests at the Dinghushan Nature Reserve (hereafter referred to as DNR) in southern China. Soils in DNR forests behaved as N2O sources and CH4 sinks. Annual mean CO2, N2O, and CH4 fluxes (mean ?? SD) were 7.7 ?? 4.6MgCO2-Cha-1 yr-1, 3.2 ?? 1.2 kg N2ONha-1 yr-1, and 3.4 ?? 0.9 kgCH4-Cha-1 yr-1, respectively. The climate was warm and wet from April through September 2003 (the hot-humid season) and became cool and dry from October 2003 through March 2004 (the cool-dry season). The seasonality of soil CO2 emission coincided with the seasonal climate pattern, with high CO2 emission rates in the hot-humid season and low rates in the cool-dry season. In contrast, seasonal patterns of CH4 and N2O fluxes were not clear, although higher CH4 uptake rates were often observed in the cool-dry season and higher N2O emission rates were often observed in the hot-humid season. GHG fluxes measured at these three sites showed a clear increasing trend with the progressive succession. If this trend is representative at the regional scale, CO2 and N2O emissions and CH4 uptake in southern China may increase in the future in light of the projected change in forest age structure. Removal of surface litter reduced soil CO2 effluxes by 17-44% in the three forests but had no significant effect on CH4 absorption and N2O emission rates. This suggests that microbial CH4 uptake and N2O production was mainly related to the mineral soil rather than in the surface litter layer. ?? 2006 Blackwell Publishing Ltd.

  1. Tunneling in the CH{sub 3} + H{sub 2} {yields} CH{sub 4} + H reaction and its isotopic analog: an anomalous isotope effect

    Energy Technology Data Exchange (ETDEWEB)

    Kurosaki, Yuzuru; Takayanagi, Toshiyuki [Japan Atomic Energy Research Inst., Tokai, Ibaraki (Japan). Tokai Research Establishment

    1998-10-01

    Vibrationally adiabatic ground-state potential curves for the CH{sub 3} + H{sub 2} {yields} CH{sub 4} + H (I) and CD{sub 3} + H{sub 2} {yields} CD{sub 4}H + H (II) reactions were obtained by adding zero-point energies of harmonic vibrations orthogonal to intrinsic reaction coordinate (IRC) to bare potential curves along IRC. It was clarified that both the barrier height and barrier width of reaction II are smaller than those of reaction I. This computational result qualitatively explains the experimental observation of Momose et al. (J. Chem. Phys. 108 (1998) 7334) that reaction II occurs but reaction I does not occur in solid parahydrogen at 5 K. (author)

  2. Global analysis of the high temperature infrared emission spectrum of (12)CH4 in the dyad (ν2/ν4) region.

    Science.gov (United States)

    Amyay, Badr; Louviot, Maud; Pirali, Olivier; Georges, Robert; Vander Auwera, Jean; Boudon, Vincent

    2016-01-14

    We report new assignments of vibration-rotation line positions of methane ((12)CH4) in the so-called dyad (ν2/ν4) region (1100-1500 cm(-1)), and the resulting update of the vibration-rotation effective model of methane, previously reported by Nikitin et al. [Phys. Chem. Chem. Phys. 15, 10071 (2013)], up to and including the tetradecad. High resolution (0.01 cm(-1)) emission spectra of methane have been recorded up to about 1400 K using the high-enthalpy source developed at Institut de Physique de Rennes associated with the Fourier transform spectrometer of the SOLEIL synchrotron facility (AILES beamline). Analysis of these spectra allowed extending rotational assignments in the well-known cold band (dyad-ground state (GS)) and related hot bands in the pentad-dyad system (3000 cm(-1)) up to Jmax = 30 and 29, respectively. In addition, 8512 new transitions belonging to the octad-pentad (up to J = 28) and tetradecad-octad (up to J = 21) hot band systems were successfully identified. As a result, the MeCaSDa database of methane was significantly improved. The line positions assigned in this work, together with the information available in the literature, were fitted using 1096 effective parameters with a dimensionless standard deviation σ = 2.09. The root mean square deviations dRMS are 3.60 × 10(-3) cm(-1) for dyad-GS cold band, 4.47 ×10(-3) cm(-1) for the pentad-dyad, 5.43 × 10(-3) cm(-1) for the octad-pentad, and 4.70 × 10(-3) cm(-1) for the tetradecad-octad hot bands. The resulting new line list will contribute to improve opacity and radiative transfer models for hot atmospheres, such as those of hot-Jupiter type exoplanets.

  3. Inverse modeling of GOSAT-retrieved ratios of total column CH4 and CO2 for 2009 and 2010

    Directory of Open Access Journals (Sweden)

    S. Pandey

    2016-04-01

    Full Text Available This study investigates the constraint provided by greenhouse gas measurements from space on surface fluxes. Imperfect knowledge of the light path through the atmosphere, arising from scattering by clouds and aerosols, can create biases in column measurements retrieved from space. To minimize the impact of such biases, ratios of total column retrieved CH4 and CO2 (Xratio have been used. We apply the ratio inversion method described in Pandey et al. (2015 to retrievals from the Greenhouse Gases Observing SATellite (GOSAT. The ratio inversion method uses the measured Xratio as a weak constraint on CO2 fluxes. In contrast, the more common approach of inverting proxy CH4 retrievals (Frankenberg et al., 2005 prescribes atmospheric CO2 fields and optimizes only CH4 fluxes. The TM5–4DVAR (Tracer Transport Model version 5–variational data assimilation system inverse modeling system is used to simultaneously optimize the fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy inversions using model-derived CO2 mixing ratios (XCO2model from CarbonTracker and the Monitoring Atmospheric Composition and Climate (MACC Reanalysis CO2 product. The performance of the inverse models is evaluated using measurements from three aircraft measurement projects. Xratio and XCO2model are compared with TCCON retrievals to quantify the relative importance of errors in these components of the proxy XCH4 retrieval (XCH4proxy. We find that the retrieval errors in Xratio (mean  =  0.61 % are generally larger than the errors in XCO2model (mean  =  0.24 and 0.01 % for CarbonTracker and MACC, respectively. On the annual timescale, the CH4 fluxes from the different satellite inversions are generally in agreement with each other, suggesting that errors in XCO2model do not limit the overall accuracy of the CH4 flux estimates. On the seasonal timescale, however, larger differences are found due to uncertainties in XCO2model, particularly

  4. The ‘Alternative Quality Contract’ in Massachusetts, Based on Global Budgets, Lowered Medical Spending and Improved Quality

    Science.gov (United States)

    Song, Zirui; Safran, Dana Gelb; Landon, Bruce E.; Landrum, Mary Beth; He, Yulei; Mechanic, Robert E.; Day, Matthew P.; Chernew, Michael E.

    2012-01-01

    Seven provider organizations in Massachusetts entered the Blue Cross Blue Shield Alternative Quality Contract in 2009, followed by four more organizations in 2010. This contract, based on a global budget and pay-for-performance for achieving certain quality benchmarks, places providers at risk for excessive spending and rewards them for quality, similar to the new Pioneer Accountable Care Organizations in Medicare. We analyzed changes in spending and quality associated with the Alternative Quality Contract and found that the rate of increase in spending slowed compared to control groups. Overall, participation in the contract over two years led to a savings of 3.3% (1.9% in year-1, 3.3% in year-2) compared to spending in groups not participating in the contract. The savings were even higher for groups whose previous experience had been only in fee-for-service contracting. Such groups’ quarterly savings over two years averaged 8.2% (6.3% in year-1, 9.9% in year-2). Quality of care also improved within organizations participating in the Alternative Quality Contract compared to control organizations in both years. Chronic care management, adult preventive care, and pediatric care improved from year 1 to year 2 within the contracting groups. These results suggest that global budgets coupled with pay-for-performance can begin to slow the underlying growth in medical spending while improving quality. PMID:22786651

  5. Isotopomer analysis of production and consumption mechanisms of N2O and CH4 in an advanced wastewater treatment system.

    Science.gov (United States)

    Toyoda, Sakae; Suzuki, Yuuri; Hattori, Shohei; Yamada, Keita; Fujii, Ayako; Yoshida, Naohiro; Kouno, Rina; Murayama, Kouki; Shiomi, Hiroshi

    2011-02-01

    Wastewater treatment processes are believed to be anthropogenic sources of nitrous oxide (N(2)O) and methane (CH(4)). However, few studies have examined the mechanisms and controlling factors in production of these greenhouse gases in complex bacterial systems. To elucidate production and consumption mechanisms of N(2)O and CH(4) in microbial consortia during wastewater treatment and to characterize human waste sources, we measured their concentrations and isotopomer ratios (elemental isotope ratios and site-specific N isotope ratios in asymmetric molecules of NNO) in water and gas samples collected by an advanced treatment system in Tokyo. Although the estimated emissions of N(2)O and CH(4) from the system were found to be lower than those from the typical treatment systems reported before, water in biological reaction tanks was supersaturated with both gases. The concentration of N(2)O, produced mainly by nitrifier-denitrification as indicated by isotopomer ratios, was highest in the oxic tank (ca. 4000% saturation). The dissolved CH(4) concentration was highest in in-flow water (ca. 3000% saturation). It decreased gradually during treatment. Its carbon isotope ratio indicated that the decrease resulted from bacterial CH(4) oxidation and that microbial CH(4) production can occur in anaerobic and settling tanks.

  6. New superhindered polydentate polyphosphine ligands P(CH2CH2P(t)Bu2)3, PhP(CH2CH2P(t)Bu2)2, P(CH2CH2CH2P(t)Bu2)3, and their ruthenium(II) chloride complexes.

    Science.gov (United States)

    Gilbert-Wilson, Ryan; Field, Leslie D; Bhadbhade, Mohan M

    2012-03-05

    The synthesis and characterization of the extremely hindered phosphine ligands, P(CH(2)CH(2)P(t)Bu(2))(3) (P(2)P(3)(tBu), 1), PhP(CH(2)CH(2)P(t)Bu(2))(2) (PhP(2)P(2)(tBu), 2), and P(CH(2)CH(2)CH(2)P(t)Bu(2))(3) (P(3)P(3)(tBu), 3) are reported, along with the synthesis and characterization of ruthenium chloro complexes RuCl(2)(P(2)P(3)(tBu)) (4), RuCl(2)(PhP(2)P(2)(tBu)) (5), and RuCl(2)(P(3)P(3)(tBu)) (6). The bulky P(2)P(3)(tBu) (1) and P(3)P(3)(tBu) (3) ligands are the most sterically encumbered PP(3)-type ligands so far synthesized, and in all cases, only three phosphorus donors are able to bind to the metal center. Complexes RuCl(2)(PhP(2)P(2)(tBu)) (5) and RuCl(2)(P(3)P(3)(tBu)) (6) were characterized by crystallography. Low temperature solution and solid state (31)P{(1)H} NMR were used to demonstrate that the structure of RuCl(2)(P(2)P(3)(tBu)) (4) is probably analogous to that of RuCl(2)(PhP(2)P(2)(tBu)) (5) which had been structurally characterized.

  7. Carbonate control of H2 and CH4 production in serpentinization systems at elevated P-Ts

    Science.gov (United States)

    Jones, L. Camille; Rosenbauer, Robert; Goldsmith, Jonas I.; Oze, Christopher

    2010-01-01

    Serpentinization of forsteritic olivine results in the inorganic synthesis of molecular hydrogen (H2) in ultramafic hydrothermal systems (e.g., mid-ocean ridge and forearc environments). Inorganic carbon in those hydrothermal systems may react with H2 to produce methane (CH4) and other hydrocarbons or react with dissolved metal ions to form carbonate minerals. Here, we report serpentinization experiments at 200°C and 300 bar demonstrating Fe2+ being incorporated into carbonates more rapidly than Fe2+ oxidation (and concomitant H2 formation) leading to diminished yields of H2 and H2-dependent CH4. In addition, carbonate formation is temporally fast in carbonate oversaturated fluids. Our results demonstrate that carbonate chemistry ultimately modulates the abiotic synthesis of both H2 and CH4 in hydrothermal ultramafic systems and that ultramafic systems present great potential for CO2-mineral sequestration.

  8. Influence of vehicular emissions on atmospheric CH4 and NMHC mixing ratios and its correlation with CO and other VOCs tracers in Mexico City

    Science.gov (United States)

    Solano-Murillo, M.; Torres-Jardón, R.; Ruiz-Suárez, L. G.; Barrera-Huertas, H.; Hernandez-Solis, J. M.

    2016-12-01

    The Mexico City Metropolitan Area (MCMA) is one of the world's largest and most polluted urban areas. A recent GHC emission inventory for MCMA suggests that vehicular emissions contribute with around 37% of CH4, followed by landfills and dump garbage areas (30%) and construction and manufacturing (27%). Contrary to other urban areas, natural gas is not the main fuel used in MCMA, neither for domestic and industrial heating, nor for transportation. Therefore, there is a great uncertainty about who is the main contributor of CH4 emissions. An intensive monitoring campaign of methane (CH4), Non-methane hydrocarbons (NMHC) and carbon monoxide (CO) was performed between February and March 2015 in southwest MCMA. Methane concentrations showed sometimes a diurnal pattern similar to those of CO and to NMHC but most of the time this similarity was lost (CH4 vs CO, R2 = 0.27; CH4 vs NMHC, R2 = 0.28). However, NMHC correlated well with CO (R2 = 0.75). The intercepts of the CH4-CO correlation resulted in [CH4] 1.8 ppm and that of the CO-NMHC correlation in [CO] 0.080 ppb. The lack of agreement between CH4 and CO indicates these species do not come from the same sources. The results suggest that vehicular emissions are not significant contributors to atmospheric CH4 and that the background methane concentration has not change significantly in 25 years. An attempt to correlate some tracers COVs tracers of vehicular and biomass burning with CH4, NMHC and CH4 is done.

  9. Atmospheric chemistry of cyc-CF2CF2CF2CH=CH-: Kinetics, products, and mechanism of gas-phase reaction with OH radicals, and atmospheric implications

    Science.gov (United States)

    Guo, Qin; Zhang, Ni; Uchimaru, Tadafumi; Chen, Liang; Quan, Hengdao; Mizukado, Junji

    2018-04-01

    The rate constants for the gas-phase reactions of cyc-CF2CF2CF2CH=CH- with OH radicals were determined by a relative rate method between 253 and 328 K. The rate constant k1 at 298 K was measured to be (1.08 ± 0.04) × 10-13 cm3 molecule-1 s-1, and the Arrhenius expression was k1 = (3.72 ± 0.14) × 10-13 exp [(-370 ± 12)/T]. The atmospheric lifetime of cyc-CF2CF2CF2CH=CH- was calculated to be 107 d. The products and mechanism for the reaction of cyc-CF2CF2CF2CH=CH- with OH radicals were also investigated. CO, CO2, and COF2 were identified as the main carbon-containing products following the OH-initiated reaction. Moreover, the radiative efficiency (RE) was determined to be 0.143 W m-2 ppb-1, and the global warming potentials (GWPs) for 20, 100, and 500 yr were 54, 15, and 4, respectively. The photochemical ozone creation potential of the title compound was estimated to be 1.3.

  10. Challenges and Conundrums in Modeling Global Methane Emissions from Wetlands: An Empiricist's Viewpoint

    Science.gov (United States)

    Bridgham, S. D.

    2015-12-01

    Wetlands emit a third to half of the global CH4 flux and have the largest uncertainty of any emission source. Moreover, wetlands have provided an important radiative feedback to climate in the geologic and recent past. A number of largescale wetland CH4 models have been developed recently, but intermodel comparisons show wide discrepancies in their predictions. I present an empiricist's overview of the current limitations and challenges of more accurately modeling wetland CH4 emissions. One of the largest limitations is simply the poor knowledge of wetland area, with estimated global values varying by a more than a factor of three. The areas of seasonal and tropical wetlands are particularly poorly constrained. There are also few wetlands with complete, multi-year datasets for all of the input variables for many models, and this lack of data is particularly alarming in tropical wetlands given that they are arguably the single largest natural or anthropogenic global CH4 source. Almost all largescale CH4 models have little biogeochemical mechanistic detail and treat anaerobic carbon cycling in a highly simplified manner. The CH4:CO2 ratio in anaerobic carbon mineralization is a central parameter in many models, but is at most set at a few values with no mechanistic underpinning. However, empirical data show that this ratio varies by five orders of magnitude in different wetlands, and tropical wetlands appear to be particularly methanogenic, all for reasons that are very poorly understood. The predominance of the acetoclastic pathway of methanogenesis appears to be related to total CH4 production, but different methanogenesis pathways are generally not incorporated into models. Other important anaerobic processes such as humic substances acting as terminal electron acceptors, fermentation, homoacetogenesis, and anaerobic CH4 oxidation are also not included in most models despite evidence of their importance in empirical studies. Moreover, there has been an explosion

  11. Finding the Missing Stratospheric Br(sub y): A Global Modeling Study of CHBr3 and CH2Br2

    Science.gov (United States)

    Liang, Q.; Stolarski, R. S.; Kawa, S. R.; Nielsen, J. E.; Douglass, A. R.; Rodriguez, J. M.; Blake, D. R.; Atlas, E. L.; Ott, L. E.

    2010-01-01

    Recent in situ and satellite measurements suggest a contribution of 5 pptv to stratospheric inorganic bromine from short-lived bromocarbons. We conduct a modeling study of the two most important short-lived bromocarbons, bromoform (CHBr3) and dibromomethane (CH2Br2), with the Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) to account for this missing stratospheric bromine. We derive a "top-down" emission estimate of CHBr3 and CH2Br2 using airborne measurements in the Pacific and North American troposphere and lower stratosphere obtained during previous NASA aircraft campaigns. Our emission estimate suggests that to reproduce the observed concentrations in the free troposphere, a global oceanic emission of 425 Gg Br yr(exp -1) for CHBr3 and 57 Gg Br yr(exp -l) for CH2Br2 is needed, with 60% of emissions from open ocean and 40% from coastal regions. Although our simple emission scheme assumes no seasonal variations, the model reproduces the observed seasonal variations of the short-lived bromocarbons with high concentrations in winter and low concentrations in summer. This indicates that the seasonality of short-lived bromocarbons is largely due to seasonality in their chemical loss and transport. The inclusion of CHBr3 and CH2Br2 contributes 5 pptv bromine throughout the stratosphere. Both the source gases and inorganic bromine produced from source gas degradation (BrSLS) in the troposphere are transported into the stratosphere, and are equally important. Inorganic bromine accounts for half (2.5 pptv) of the bromine from the inclusion of CHBr3 and CHzBr2 near the tropical tropopause and its contribution rapidly increases to 100% as altitude increases. More than 85% of the wet scavenging of Br(sub y)(sup VSLS) occurs in large-scale precipitation below 500 hPa. Our sensitivity study with wet scavenging in convective updrafts switched off suggests that Br(sub y)(sup SLS) in the stratosphere is not sensitive to convection. Convective scavenging only

  12. New accurate theoretical line lists of 12CH4 and 13CH4 in the 0-13400 cm-1 range: Application to the modeling of methane absorption in Titan's atmosphere

    Science.gov (United States)

    Rey, Michaël; Nikitin, Andrei V.; Bézard, Bruno; Rannou, Pascal; Coustenis, Athena; Tyuterev, Vladimir G.

    2018-03-01

    The spectrum of methane is very important for the analysis and modeling of Titan's atmosphere but its insufficient knowledge in the near infrared, with the absence of reliable absorption coefficients, is an important limitation. In order to help the astronomer community for analyzing high-quality spectra, we report in the present work the first accurate theoretical methane line lists (T = 50-350 K) of 12CH4 and 13CH4 up to 13400 cm-1 ( > 0.75 μm). These lists are built from extensive variational calculations using our recent ab initio potential and dipole moment surfaces and will be freely accessible via the TheoReTS information system (http://theorets.univ-reims.fr, http://theorets.tsu.ru). Validation of these lists is presented throughout the present paper. For the sample of lines where upper energies were available from published analyses of experimental laboratory 12CH4 spectra, small empirical corrections in positions were introduced that could be useful for future high-resolution applications. We finally apply the TheoRetS line list to model Titan spectra as observed by VIMS and by DISR, respectively onboard Cassini and Huygens. These data are used to check that the TheoReTS line lists are able to model observations. We also make comparisons with other experimental or theoretical line lists. It appears that TheoRetS gives very reliable results better than ExoMol and even than HITRAN2012, except around 1.6 μm where it gives very similar results. We conclude that TheoReTS is suitable to be used for the modeling of planetary radiative transfer and photometry. A re-analysis of spectra recorded by the DISR instrument during the descent of the Huygens probe suggests that the CH4 mixing ratio decreases with altitude in Titan's stratosphere, reaching a value of ∼10-2 above the 110 km altitude.

  13. Influence of Meteorology and interrelationship with greenhouse gases (CO2 and CH4) at a suburban site of India

    Science.gov (United States)

    Sreenivas, Gaddamidi; Mahesh, Pathakoti; Subin, Jose; Lakshmi Kanchana, Asuri; Venkata Narasimha Rao, Pamaraju; Dadhwal, Vinay Kumar

    2016-03-01

    Atmospheric greenhouse gases (GHGs), such as carbon dioxide (CO2) and methane (CH4), are important climate forcing agents due to their significant impacts on the climate system. The present study brings out first continuous measurements of atmospheric GHGs using high-precision LGR-GGA over Shadnagar, a suburban site of Central India during the year 2014. The annual mean CO2 and CH4 over the study region are found to be 394 ± 2.92 and 1.92 ± 0.07 ppm (μ ± 1σ) respectively. CO2 and CH4 show a significant seasonal variation during the study period with maximum (minimum) CO2 observed during pre-monsoon (monsoon), while CH4 recorded the maximum during post-monsoon and minimum during monsoon. Irrespective of the seasons, consistent diurnal variations of these gases are observed. Influences of prevailing meteorology (air temperature, wind speed, wind direction, and relative humidity) on GHGs have also been investigated. CO2 and CH4 show a strong positive correlation during winter, pre-monsoon, monsoon, and post-monsoon with correlation coefficients (Rs) equal to 0.80, 0.80, 0.61, and 0.72 respectively, indicating a common anthropogenic source for these gases. Analysis of this study reveals the major sources for CO2 are soil respiration and anthropogenic emissions while vegetation acts as a main sink, whereas the major source and sink for CH4 are vegetation and presence of hydroxyl (OH) radicals.

  14. Phosphorus addition mitigates N2O and CH4 emissions in N-saturated subtropical forest, SW China

    Directory of Open Access Journals (Sweden)

    L. Yu

    2017-06-01

    Full Text Available Chronically elevated nitrogen (N deposition has led to severe nutrient imbalance in forest soils. Particularly in tropical and subtropical forest ecosystems, increasing N loading has aggravated phosphorus (P limitation of biomass production, and has resulted in elevated emissions of nitrous oxide (N2O and reduced uptake of methane (CH4, both of which are important greenhouse gases. Yet, the interactions of N and P and their effects on greenhouse gas emissions remain elusive. Here, we report N2O and CH4 emissions together with soil N and P data for a period of 18 months following a single P addition (79 kg P ha−1, as NaH2PO4 powder to an N-saturated, Masson pine-dominated forest soil at TieShanPing (TSP, Chongqing, south-western (SW China. We observed a significant decline in both nitrate (NO3− concentrations in soil water (5 and 20 cm depths and in soil N2O emissions, following P application. We hypothesise that enhanced N uptake by plants in response to P addition, resulted in less available NO3− for denitrification. By contrast to most other forest ecosystems, TSP is a net source of CH4. P addition significantly decreased CH4 emissions and turned the soil from a net source into a net sink. Based on our observation and previous studies in South America and China, we believe that P addition relieves N inhibition of CH4 oxidation. Within the 1.5 years after P addition, no significant increase of forest growth was observed and P stimulation of forest N uptake by understorey vegetation remains to be confirmed. Our study indicates that P fertilisation of N-saturated, subtropical forest soils may mitigate N2O and CH4 emissions, in addition to alleviating nutrient imbalances and reducing losses of N through NO3− leaching.

  15. Transport and transformation of soil-derived CO2, CH4 and DOC sustain CO2 supersaturation in small boreal streams.

    Science.gov (United States)

    Rasilo, Terhi; Hutchins, Ryan H S; Ruiz-González, Clara; Del Giorgio, Paul A

    2017-02-01

    Streams are typically supersaturated in carbon dioxide (CO 2 ) and methane (CH 4 ), and are recognized as important components of regional carbon (C) emissions in northern landscapes. Whereas there is consensus that in most of the systems the CO 2 emitted by streams represents C fixed in the terrestrial ecosystem, the pathways delivering this C to streams are still not well understood. We assessed the contribution of direct soil CO 2 injection versus the oxidation of soil-derived dissolved organic C (DOC) and CH 4 in supporting CO 2 supersaturation in boreal streams in Québec. We measured the concentrations of CO 2 , CH 4 and DOC in 43 streams and adjacent soil waters during summer base-flow period. A mass balance approach revealed that all three pathways are significant, and that the mineralization of soil-derived DOC and CH 4 accounted for most of the estimated stream CO 2 emissions (average 75% and 10%, respectively), and that these estimated contributions did not change significantly between the studied low order (≤3) streams. Whereas some of these transformations take place in the channel proper, our results suggest that they mainly occur in the hyporheic zones of the streams. Our results further show that stream CH 4 emissions can be fully explained by soil CH 4 inputs. This study confirms that these boreal streams, and in particular their hyporheic zones, are extremely active processors of soil derived DOC and CH 4 , not just vents for soil produced CO 2 . Copyright © 2016 Elsevier B.V. All rights reserved.

  16. Soil greenhouse gas emissions and carbon budgeting in a short-hydroperiod floodplain wetland

    Science.gov (United States)

    Batson, Jackie; Noe, Gregory B.; Hupp, Cliff R.; Krauss, Ken W.; Rybicki, Nancy B.; Schenk, Edward R.

    2015-01-01

    Understanding the controls on floodplain carbon (C) cycling is important for assessing greenhouse gas emissions and the potential for C sequestration in river-floodplain ecosystems. We hypothesized that greater hydrologic connectivity would increase C inputs to floodplains that would not only stimulate soil C gas emissions but also sequester more C in soils. In an urban Piedmont river (151 km2 watershed) with a floodplain that is dry most of the year, we quantified soil CO2, CH4, and N2O net emissions along gradients of floodplain hydrologic connectivity, identified controls on soil aerobic and anaerobic respiration, and developed a floodplain soil C budget. Sites were chosen along a longitudinal river gradient and across lateral floodplain geomorphic units (levee, backswamp, and toe slope). CO2 emissions decreased downstream in backswamps and toe slopes and were high on the levees. CH4 and N2O fluxes were near zero; however, CH4emissions were highest in the backswamp. Annual CO2 emissions correlated negatively with soil water-filled pore space and positively with variables related to drier, coarser soil. Conversely, annual CH4 emissions had the opposite pattern of CO2. Spatial variation in aerobic and anaerobic respiration was thus controlled by oxygen availability but was not related to C inputs from sedimentation or vegetation. The annual mean soil CO2 emission rate was 1091 g C m−2 yr−1, the net sedimentation rate was 111 g C m−2 yr−1, and the vegetation production rate was 240 g C m−2 yr−1, with a soil C balance (loss) of −338 g C m−2 yr−1. This floodplain is losing C likely due to long-term drying from watershed urbanization.

  17. Reactions of 11C recoil atoms in the systems H2O-NH3, H2O-CH4 and NH3-CH4

    International Nuclear Information System (INIS)

    Nebeling, B.

    1988-11-01

    In this study the chemical reactions of recoil carbon 11 in the binary gas mixtures H 2 O-NH 3 , H 2 O-CH 4 and NH 3 -CH 4 in different mixing ratios as well as in solid H 2 O and in a solid H 2 O-NH 3 mixture were analyzed in dependence of the dose. The analyses were to serve e.g. the simulation of chemical processes caused by solar wind, solar radiation and cosmic radiation in the coma and core of comets. They were to give further information about the role of the most important biogeneous element carbon, i.e. carbon, in the chemical evolution of the solar system. Besides the actual high energy processes resulting in the so-called primary products, also the radiation-chemical changes of the primary products were also observed in a wide range of dosing. The generation of the energetic 11 C atoms took place according to the target composition by the nuclear reactions 14 N(p,α) 11 C, 12 C( 3 He,α) 11 C or the 16 O(p,αpn) 11 C reaction. The identification of the products marked with 11 C was carried out by means of radio gas chromatography or radio liquid chromatography (HPLC). (orig./RB) [de

  18. Prediction CH4 Emissions from the Wetlands in the Sanjiang Plain of Northeastern China in the 21st Century.

    Directory of Open Access Journals (Sweden)

    Tingting Li

    Full Text Available The Sanjiang Plain has been experienced significant wetland loss due to expanded agricultural activities, and will be potentially restored by the China National Wetland Conservation Action Plan (NWCP in future. The objective of this study is to evaluate the impact of future climate warming and wetland restoration on wetland CH4 emissions in northeast China. We used an atmosphere-vegetation interaction model (AVIM2 to drive a modified biogeophysical model (CH4MODwetland, and projected CH4 flux variations from the Sanjiang Plain wetlands under different Representative Concentration Pathway scenarios throughout the 21st century. Model validation showed that the regressions between the observed and simulated CH4 fluxes by the modified model produced an R2 of 0.49 with a slope of 0.87 (p<0.001, n = 237. According to the AVIM2 simulation, the net primary productivity of the Sanjiang Plain wetlands will increase by 38.2 g m-2 yr-1, 116.6 g m-2 yr-1 and 250.4 g m-2 yr-1 under RCP 2.6, RCP 4.5 and RCP 8.5, respectively, by the end of this century. For RCP 2.6, 4.5 and 8.5 scenarios, the CH4 fluxes will increase by 5.7 g m-2 yr-1, 57.5 g m-2 yr-1 and 112.2 g m-2 yr-1. Combined with the wetland restoration, the regional emissions will increase by 0.18‒1.52 Tg. The CH4 emissions will be stimulated by climate change and wetland restoration. Regional wetland restoration planning should be directed against different climate scenarios in order to suppress methane emissions.

  19. Tropical wetlands: A missing link in the global carbon cycle?

    Science.gov (United States)

    Sjögersten, Sofie; Black, Colin R; Evers, Stephanie; Hoyos-Santillan, Jorge; Wright, Emma L; Turner, Benjamin L

    2014-01-01

    Tropical wetlands are not included in Earth system models, despite being an important source of methane (CH4) and contributing a large fraction of carbon dioxide (CO2) emissions from land use, land use change, and forestry in the tropics. This review identifies a remarkable lack of data on the carbon balance and gas fluxes from undisturbed tropical wetlands, which limits the ability of global change models to make accurate predictions about future climate. We show that the available data on in situ carbon gas fluxes in undisturbed forested tropical wetlands indicate marked spatial and temporal variability in CO2 and CH4 emissions, with exceptionally large fluxes in Southeast Asia and the Neotropics. By upscaling short-term measurements, we calculate that approximately 90 ± 77 Tg CH4 year−1 and 4540 ± 1480 Tg CO2 year−1 are released from tropical wetlands globally. CH4 fluxes are greater from mineral than organic soils, whereas CO2 fluxes do not differ between soil types. The high CO2 and CH4 emissions are mirrored by high rates of net primary productivity and litter decay. Net ecosystem productivity was estimated to be greater in peat-forming wetlands than on mineral soils, but the available data are insufficient to construct reliable carbon balances or estimate gas fluxes at regional scales. We conclude that there is an urgent need for systematic data on carbon dynamics in tropical wetlands to provide a robust understanding of how they differ from well-studied northern wetlands and allow incorporation of tropical wetlands into global climate change models. PMID:26074666

  20. Methane emissions associated with the conversion of marshland to cropland and climate change on the Sanjiang Plain of northeast China from 1950 to 2100

    Directory of Open Access Journals (Sweden)

    T. Li

    2012-12-01

    Full Text Available Wetland loss and climate change are known to alter regional and global methane (CH4 budgets. Over the last six decades, an extensive area of marshland has been converted to cropland on the Sanjiang Plain in northeast China, and a significant increase in air temperature has also been observed there, while the impacts on regional CH4 budgets remain uncertain. Through model simulation, we estimated the changes in CH4 emissions associated with the conversion of marshland to cropland and climate change in this area. Model simulations indicated a significant reduction of 1.1 Tg yr−1 (0.7–1.8 Tg yr−1 from the 1950s to the 2000s in regional CH4 emissions. The cumulative reduction of CH4 from 1960 to 2009 was estimated to be ~36 Tg (24–57 Tg relative to the 1950s, and marshland conversion and the climate contributed 86% and 14% of this change, respectively. Interannual variation in precipitation (linear trend with P > 0.2 contributed to yearly fluctuations in CH4 emissions, but the relatively lower amount of precipitation over the period 1960–2009 (47 mm yr−1 lower on average than in the 1950s contributed ~91% of the reduction in the area-weighted CH4 flux. Global warming at a rate of 0.3 ° per decade (P < 0.001 has increased CH4 emissions significantly since the 1990s. Relative to the mean of the 1950s, the warming-induced increase in the CH4 flux has averaged 19 kg ha−1 yr−1 over the last two decades. In the RCP (Representative Concentration Pathway 2.6, RCP 4.5, RCP 6.0 and RCP 8.5 scenarios of the fifth IPCC assessment report (AR5, the CH4 fluxes are predicted to increase by 36%, 52%, 78% and 95%, respectively, by the 2080s compared to 1961–1990 in response to climate warming and wetting.