WorldWideScience

Sample records for global ch4 budget

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

    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

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

    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

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

    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.

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

    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.

  5. Global Carbon Budget 2017

    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

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

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

    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.

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

    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.

  9. Global Carbon Budget 2016

    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

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

    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

  11. The Global Methane Budget 2000-2012

    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

  12. 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

    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.

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

    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

  14. Global carbon budget 2013

    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

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

    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...

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

    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.

  17. Global Carbon Budget 2017

    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 2017

    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

  19. Global Carbon Budget 2016

    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

    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 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 and consistency within and among components, alongside methodology and data limitations. 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 combined evidence from land-cover change data, fire activity associated with deforestation, and models. The global atmospheric CO2 concentration is measured directly and its rate of growth (GATM) is computed from the annual changes in 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. The variability in SOCEAN is evaluated with data products based on surveys of ocean CO2 measurements. The global residual terrestrial CO2 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. We compare the mean land and ocean fluxes and their variability to estimates from three atmospheric inverse methods for three broad latitude bands. All uncertainties are reported as +/- 1(sigma), reflecting the current capacity to characterize the annual estimates of each component of the global carbon budget. For the last decade available (2006-2015), EFF was 9

  20. Global Carbon Budget 2016

    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

    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 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 and consistency within and among components, alongside methodology and data limitations. 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 combined evidence from land-cover change data, fire activity associated with deforestation, and models. The global atmospheric CO2 concentration is measured directly and its rate of growth (GATM) is computed from the annual changes in 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. The variability in SOCEAN is evaluated with data products based on surveys of ocean CO2 measurements. The global residual terrestrial CO2 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. We compare the mean land and ocean fluxes and their variability to estimates from three atmospheric inverse methods for three broad latitude bands. All uncertainties are reported as ±1σ, reflecting the current capacity to characterise the annual estimates of each component of the global carbon budget. For the last decade available (2006-2015), EFF was 9

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

    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.

  2. Global Carbon Budget 2015

    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

    Accurate assessment 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 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 as well as consistency within and among components, alongside methodology and data limitations. CO2 emissions from fossil fuels and industry (EFF) are based on energy statistics and cement production data, 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 CO2 concentration is measured directly and its rate of growth (GATM) is computed from the annual changes in 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. The variability in SOCEAN is evaluated with data products based on surveys of ocean CO2 measurements. The global residual terrestrial CO2 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, CO2, and land-cover change (some including nitrogen-carbon interactions). We compare the mean land and ocean fluxes and their variability to estimates from three atmospheric inverse methods for three broad latitude bands. All uncertainties are reported as ±1σ, reflecting the current capacity to characterise the annual estimates of each component of the global

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

    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.

  4. Global Carbon Budget 2016

    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

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

    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.

  6. 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

    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

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

    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.

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

    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.

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

    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.

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

    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.

  11. [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].

    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.

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

    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.

  13. Intermediate-scale community-level flux of CO2 and CH4 in a Minnesota peatland: putting the SPRUCE project in a global context

    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...

  14. Global research and development budget

    Norman, C

    1980-03-01

    The future political and economic relationships between industrial countries and between the industrial and developing countries will be influenced by the investments now being made for research and development (R and D). There is little public understanding of this $150 billion global investment, 25 percent of which is spent on military programs, 15 percent on basic research, and nearly 10 percent on space exploration, while the most-pressing world problems are receiving relatively little attention. A breakdown of geographic distribution of research and a comparison of government expenditures for different areas of R and D reveals a situation that could be corrected. National and corporate priorities need to be revised and political and institutional barriers must give way to new international and cooperative arrangements. 3 tables, 27 references. (DCK)

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

    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.

  16. Tropospheric radiative forcing of CH4

    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

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

    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.

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

    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)

  19. The global carbon budget 1959–2011

    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

  20. Global analysis of the high temperature infrared emission spectrum of (12)CH4 in the dyad (ν2/ν4) region.

    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.

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

    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, ...

  2. 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

    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.

  3. Effects of globalization on state budgeting system in Ukraine

    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.

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

    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

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

    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.

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

    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...

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

    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.

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

    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.

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

    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.

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

    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

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

    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.

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

    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.

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

    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

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

    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

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

    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...

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

    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.

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

    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.

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

    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.

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

    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

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

    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.

  1. Observational constraints on the global atmospheric budget of ethanol

    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.

  2. Global Methane Biogeochemistry

    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

  3. Climate change and global warming potentials

    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

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

    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.

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

    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.

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

    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

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

    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

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

    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

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

    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.

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

    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.

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

    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

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

    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.

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

    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.

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

    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)

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

    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

  16. Provider Behavior Under Global Budgeting and Policy Responses

    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.

  17. Global atmospheric budget of simple monocyclic aromatic compounds

    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.

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

    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

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

    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.

  20. Microbial CH4 and N2O consumption in acidic wetlands

    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.

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

    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.

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

    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.

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

    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

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

    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.

  5. Dissociative sticking of CH4 on Ru(0001)

    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...

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

    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.

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

    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

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

    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.

  9. Constraining global methane emissions and uptake by ecosystems

    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

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

    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

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

    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.

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

    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.

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

    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

  14. δ13C-CH4 in ice core samples

    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...

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

    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

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

    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.

  17. 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

    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.

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

    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.

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

    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.

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

    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

  1. KlimaCH4. Climate effects of biomethane economy; KlimaCH4. Klimaeffekte von Biomethan

    Westerkamp, Tanja; Reinelt, Torsten; Oehmichen, Katja; Ponitka, Jens; Naumann, Karin

    2014-07-01

    Within the project ''Climate effects of biomethane economy'' (KlimaCH4) of the German Biomass Research Centre two methods for measurement of direct greenhouse gas emissions were analyzed for their applicability and comparability. In the context of concrete measurements direct emissions, mainly of methane, three biogas plants with methane treatment for feeding into the natural gas grid were quantified. These tests were carried out on the one hand directly on-site by using leak detection, enclosures and ''open chamber'' measurements, but also indirectly by optical remote sensing with tunable diode laser absorption spectrometry (TDLAS) and reverse dispersion modelling by inverse dispersion modeling. The on-site method offers the possibility, to investigate the influences of plant operation on emissions of known diffuse sources, inter alia, through the balance of the operating status with the timeline of a specific emission source (e.g. as increased release of methane due to stirring intervals). This is particularly useful for deriving appropriate measures to reduce emissions. The quantification of individual, diffuse emission sources is metrologically possibly only very costly to implement. The effort is depending to a considerable extent by the design and the size of the examined biogas plant. In order to detect the influence seasonal changing of environmental conditions recurring emission measurements were realized. The use of optical telemetry showed as an advantageous alternative to on-site method, because it can significantly reduce time required for emission measurements particularly at large biogas plants or plants with numerous individual sources. With only one measurement sequence all emission sources are covered, without consuming individual measurements. In addition, in comparision to the on-site method, the emission situation of the entire system can be better reproduced, since all individual sources are included in

  2. KlimaCH4. Climate effects of biomethane economy; KlimaCH4. Klimaeffekte von Biomethan

    Westerkamp, Tanja; Reinelt, Torsten; Oehmichen, Katja; Ponitka, Jens; Naumann, Karin

    2014-07-01

    Within the project ''Climate effects of biomethane economy'' (KlimaCH4) of the German Biomass Research Centre two methods for measurement of direct greenhouse gas emissions were analyzed for their applicability and comparability. In the context of concrete measurements direct emissions, mainly of methane, three biogas plants with methane treatment for feeding into the natural gas grid were quantified. These tests were carried out on the one hand directly on-site by using leak detection, enclosures and ''open chamber'' measurements, but also indirectly by optical remote sensing with tunable diode laser absorption spectrometry (TDLAS) and reverse dispersion modelling by inverse dispersion modeling. The on-site method offers the possibility, to investigate the influences of plant operation on emissions of known diffuse sources, inter alia, through the balance of the operating status with the timeline of a specific emission source (e.g. as increased release of methane due to stirring intervals). This is particularly useful for deriving appropriate measures to reduce emissions. The quantification of individual, diffuse emission sources is metrologically possibly only very costly to implement. The effort is depending to a considerable extent by the design and the size of the examined biogas plant. In order to detect the influence seasonal changing of environmental conditions recurring emission measurements were realized. The use of optical telemetry showed as an advantageous alternative to on-site method, because it can significantly reduce time required for emission measurements particularly at large biogas plants or plants with numerous individual sources. With only one measurement sequence all emission sources are covered, without consuming individual measurements. In addition, in comparision to the on-site method, the emission situation of the entire system can be better reproduced, since all individual sources are included in the identical period. In addition, with

  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

    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. Vibrational transition moments of CH4 from first principles

    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. Macromolecule simulation and CH4 adsorption mechanism of coal vitrinite

    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.

  6. Comment on 'Current Budget of the Atmospheric Electric Global Circuit'

    Driscoll, Kevin T.; Blakeslee, Richard J.

    1996-01-01

    In this paper, three major issues relevant to Kasemir's new model will be addressed. The first concerns Kasemir's assertion that there are significant differences between the potentials associated with the new model and the conventional model. A recalculation of these potentials reveals that both models provide equivalent results for the potential difference between the Earth and ionosphere. The second issue to be addressed is Kasemir's assertion that discrepancies in the electric potentials associated with both models can be attributed to modeling the Earth as a sphere, instead of as a planar surface. A simple analytical comparison will demonstrate that differences in the equations for the potentials of the atmosphere derived with a spherical and a planar Earth are negligible for applications to global current flow. Finally, the third issue to be discussed is Kasemir's claim that numerous aspects of the conventional model are incorrect, including the role of the ionosphere in global current flow as well as the significance of cloud-to-ground lightning in supplying charge to the global circuit. In order to refute these misconceptions, it will be shown that these aspects related to the flow of charge in the atmosphere are accurately described by the conventional model of the global circuit.

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

    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.

  8. Renewable energy based catalytic CH4 conversion to fuels

    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

  9. CO2/CH4 Separation via Polymeric Blend Membrane

    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

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

    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...

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

    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...

  12. Global Budgets and Technology-Intensive Medical Services.

    Song, Zirui; Fendrick, A Mark; Safran, Dana Gelb; Landon, Bruce; Chernew, Michael E

    2013-06-01

    In 2009-2010, Blue Cross Blue Shield of Massachusetts entered into global payment contracts (the Alternative Quality contract, AQC) with 11 provider organizations. We evaluated the impact of the AQC on spending and utilization of several categories of medical technologies, including one considered high value (colonoscopies) and three that include services that may be overused in some situations (cardiovascular, imaging, and orthopedic services). Approximately 420,000 unique enrollees in 2009 and 180,000 in 2010 were linked to primary care physicians whose organizations joined the AQC. Using three years of pre-intervention data and a large control group, we analyzed changes in utilization and spending associated with the AQC with a propensity-weighted difference-in-differences approach adjusting for enrollee demographics, health status, secular trends, and cost-sharing. In the 2009 AQC cohort, total volume of colonoscopies increased 5.2 percent (p=0.04) in the first two years of the contract relative to control. The contract was associated with varied changes in volume for cardiovascular and imaging services, but total spending on cardiovascular services in the first two years decreased by 7.4% (p=0.02) while total spending on imaging services decreased by 6.1% (pservices, these decreases were also attributable to shifting care to lower-priced providers. No effect was found in orthopedics. As one example of a large-scale global payment initiative, the AQC was associated with higher use of colonoscopies. Among several categories of services whose value may be controversial, the contract generally shifted volume to lower-priced facilities or services.

  13. Global aerosol transport and consequences for the radiation budget

    Newiger, M.; Grassl, H.; Schussel, P.; Rehkopf, J.

    1984-01-01

    Man's activities may influence global climate by changing the atmospheric composition and surface characteristics and by waste heat. Most prominent within this discussion is the increase or decrease of radiatively active trace gases like CO/sub 2/, N/sub 2/O, O/sub 3/, and others. The general opinion is converging towards a greenhouse effect as a combined action of all trace gases, whose exact magnitude is uncertain mainly because of the unknown reaction of water cycle. The aim of our global 2-D (resolving latitude and height) aerosol transport model is the calculation of aerosol particle number density profiles as a function of latitude for present natural plus anthropogenic emissions. The aerosol transport model uses prescribed meridonal circulation, diffusivity factors and cloud climatology for January as well as July. All these latitude and height dependent input parameters were taken from well known sources. The fixed climatology excludes the feedback of aerosol particle parameter changes on mean circulation. However, the radiative parameters of six clouds types are modified, although they possess by adoption of the Telegadas and London (1954) cloud climatology prescribed amount and height. The inclusion of the feedback on mean circulation seems premature at present. Adding particles either accounting for natural emissions or natural anthropogenic emission and removing particles by all known sinks outside and within clouds gives us - for the stationary state - vertical profiles of aerosol number density in three sizes classes as a function of latitude. These profiles in turn are input for radiation flux calculations in clear and cloudy areas in order to assess net flux changes caused by the present aerosol load in comparison to a scenario without anthropogenic emissions. The net flux changes finally are compared to those calculated for increased CO/sub 2/ levels

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

    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.

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

    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

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

    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

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

    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.

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

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

    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

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

    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

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

    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

  2. Experimental ion mobility measurements in Xe-CH4

    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.

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

    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

  4. Ion irradiation of CH4-containing icy mixtures

    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

  5. Preparation of CH4 for 14C measurements

    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

  6. CH4 emissions from enteric fermentation in Austria

    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)

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

    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...

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

    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.

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

    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.

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

    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.

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

    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

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

    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

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

    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.

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

    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.

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

    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.

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

    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.

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

    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.

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

    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

  19. Methanogenic Conversion of CO2 Into CH4

    Stevens, S.H., Ferry, J.G., Schoell, M.

    2012-05-06

    This SBIR project evaluated the potential to remediate geologic CO2 sequestration sites into useful methane gas fields by application of methanogenic bacteria. Such methanogens are present in a wide variety of natural environments, converting CO2 into CH4 under natural conditions. We conclude that the process is generally feasible to apply within many of the proposed CO2 storage reservoir settings. However, extensive further basic R&D still is needed to define the precise species, environments, nutrient growth accelerants, and economics of the methanogenic process. Consequently, the study team does not recommend Phase III commercial application of the technology at this early phase.

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

    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.

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

    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.

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

    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.

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

    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.

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

    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.

  5. Quantifying Gas Flaring CH4 Consumption Using VIIRS

    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.

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

    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.

  7. CH4 fluxes across the seafloor at three district gas hydrate fields: Impacts on ocean and atmosphere chemistry

    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

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

    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.

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

    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.

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

    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

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

    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.

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

    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.

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

    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.

  14. Evaluation of the Global Mean Sea Level Budget between 1993 and 2014

    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...

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

    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

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

    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.

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

    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.

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

    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

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

    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

  20. The 'Alternative Quality Contract,' based on a global budget, lowered medical spending and improved quality.

    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.

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

    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

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

    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.

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

    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.

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

    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.

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

    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.

  6. 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

    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

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

    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.

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

    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.

  9. 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

    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.

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

    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

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

    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

  12. PENGARUH WAKTU KONTAK TERHADAP DAYA ADSORPSI KARBON AKTIF PADA PROSES PURIFIKASI CH4 DARI BIOGAS

    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

  13. Neutron scattering and proton spin conversion in solid CH4

    Lushington, K.J.; Morrison, J.A.

    1977-01-01

    The total neutron cross section of pure and O 2 -doped condensed CH 4 has been measured in the temperature range 0.75< T<100 K. The neutron wave length was sufficiently long (4.7 A) so that changes in cross section could be directly related to changes in γI(I + 1)μ, the mean squared proton nuclear angular momentum per molecule, to a sensitivity of about 1%. The temperature dependences of γI(I + 1)μ for the pure and doped specimens differ considerably in solid phase II(T<20.4 K). For the former specimen, the change in cross section is consistent with conversion occurring between the nuclear spin symmetry species on the orientationally disordered sublattices only. The addition of oxygen enhances the rate of conversion such that the value of γI(I + 1)μ corresponds to conversion on both the disordered and ordered sublattices. The characteristic lifetimes of the catalyzed and uncatalyzed conversion processes have been estimated. (author)

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

    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,

  15. Constraining the global carbon budget from global to regional scales - The measurement challenge

    Francey, R.J.; Rayner, P.J.; Allison, C.E.

    2002-01-01

    The Global Carbon Cycle can be modelled by a Bayesian synthesis inversion technique, where measured atmospheric CO 2 concentrations and isotopic compositions are analysed by use of an atmospheric transport model and estimates of regional sources and sinks of atmospheric carbon. The uncertainty associated to carbon flux estimates even on a regional scale can be improved considerably using the inversion technique. In this approach, besides the necessary control on the precision of atmospheric transport models and on the constraints for surface fluxes, an important component is the calibration of atmospheric CO 2 concentration and isotope measurements. The recent improved situation in respect to data comparability is discussed using results of conducted interlaboratory comparison exercises and larger scale calibration programs are proposed for the future to further improve the comparability of analytical data. (author)

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

    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

  17. Audit of the global carbon budget: estimate errors and their impact on uptake uncertainty

    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

  18. Ocean heat content and ocean energy budget: make better use of historical global subsurface temperature dataset

    Cheng, L.; Zhu, J.

    2016-02-01

    Ocean heat content (OHC) change contributes substantially to global sea level rise, also is a key metric of the ocean/global energy budget, so it is a vital task for the climate research community to estimate historical OHC. While there are large uncertainties regarding its value, here we review the OHC calculation by using the historical global subsurface temperature dataset, and discuss the sources of its uncertainty. The presentation briefly introduces how to correct to the systematic biases in expendable bathythermograph (XBT) data, a alternative way of filling data gaps (which is main focus of this talk), and how to choose a proper climatology. A new reconstruction of historical upper (0-700 m) OHC change will be presented, which is the Institute of Atmospheric Physics (IAP) version of historical upper OHC assessment. The authors also want to highlight the impact of observation system change on OHC calculation, which could lead to bias in OHC estimates. Furthermore, we will compare the updated observational-based estimates on ocean heat content change since 1970s with CMIP5 results. This comparison shows good agreement, increasing the confidence of the climate models in representing the climate history.

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

    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.

  20. Evaluation of the reactive nitrogen budget of the remote atmosphere in global models using airborne measurements

    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.

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

    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).

  2. The use and re-use of unsustainably mined groundwater: A global budget

    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.

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

    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.

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

    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...

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

    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...

  6. 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.

    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.

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

    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...

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

    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.

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

    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.

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

    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

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

    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

  12. Global nitrogen budgets in cereals: A 50-year assessment for maize, rice, and wheat production systems.

    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.

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

    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.

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

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

    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.

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

    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.

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

    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...

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

    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...

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

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

    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...

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

    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

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

    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...

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

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

    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.

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

    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

  6. Agency problems in hospitals participating in self-management project under global budget system in Taiwan.

    Yan, Yu-Hua; Hsu, Shuofen; Yang, Chen-Wei; Fang, Shih-Chieh

    2010-02-01

    The main purposes of this study are to clarify the agency problems in the hospitals participating in self-management project within the context of Global Budgeting Payment System regulated by Taiwan government, and also to provide some suggestions for hospital administrator and health policy maker in reducing the waste of healthcare resources resulting from agency problems. For the purposes above, this study examines the relationships between two agency problems (ex ante moral hazard and ex post moral hazard) aroused among the hospitals and Bureau of National Health Insurance in Taiwan's health care sector. This study empirically tested the theoretical model at organization level. The findings suggest that the hospital's ex ante moral hazards before participating the self-management project do have some influence on its ex post moral hazards after participating the self-management project. This study concludes that the goal conflict between the agents and the principal certainly exist. The principal tries hard to control the expenditure escalation and keep the financial balance, but the agents have to subsist within limited healthcare resources. Therefore, the agency cost would definitely occur due to the conflicts between both parties. According to the results of the research, some suggestions and related management concepts were proposed at the end of the paper.

  7. Agency problems of global budget system in Taiwan's National Health Insurance.

    Yan, Yu-Hua; Yang, Chen-Wei; Fang, Shih-Chieh

    2014-05-01

    The main purpose of this study was to investigate the agency problem presented by the global budget system followed by hospitals in Taiwan. In this study, we examine empirically the interaction between the principal: Bureau of National Health Insurance (BNHI) and agency: medical service providers (hospitals); we also describe actual medical service provider and hospital governance conditions from a agency theory perspective. This study identified a positive correlation between aversion to agency hazard (self-interest behavior, asymmetric information, and risk hedging) and agency problem risks (disregard of medical ethics, pursuit of extra-contract profit, disregard of professionalism, and cost orientation). Agency costs refer to BNHI auditing and monitoring expenditures used to prevent hospitals from deviating from NHI policy goals. This study also found agency costs negatively moderate the relationship between agency hazards and agency problems The main contribution of this study is its use of agency theory to clarify agency problems and several potential factors caused by the NHI system. This study also contributes to the field of health policy study by clarifying the nature and importance of agency problems in the health care sector. Copyright © 2014 Elsevier Ireland Ltd. All rights reserved.

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

    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.

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

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

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

    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

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

    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.

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

    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

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

    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

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

    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.

  16. BOREAS TGB-1 Soil CH4 and CO2 Profile Data from NSA Tower Sites

    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.

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

    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

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

    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

  19. CH4/air homogeneous autoignition: A comparison of two chemical kinetics mechanisms

    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

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

    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.

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

    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

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

    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.

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

    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.

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

    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.

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

    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.

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

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

    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.

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

    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.

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

    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.

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

    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.

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

    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

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

    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

  13. The c2d Spitzer spectroscopic survey of ices around low-mass young stellar objects. III. CH4

    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

  14. Impact of climate change on tropospheric ozone and its global budgets

    G. Zeng

    2008-01-01

    Full Text Available We present the chemistry-climate model UMCAM in which a relatively detailed tropospheric chemical module has been incorporated into the UK Met Office's Unified Model version 4.5. We obtain good agreements between the modelled ozone/nitrogen species and a range of observations including surface ozone measurements, ozone sonde data, and some aircraft campaigns.

    Four 2100 calculations assess model responses to projected changes of anthropogenic emissions (SRES A2, climate change (due to doubling CO2, and idealised climate change-associated changes in biogenic emissions (i.e. 50% increase of isoprene emission and doubling emissions of soil-NOx. The global tropospheric ozone burden increases significantly for all the 2100 A2 simulations, with the largest response caused by the increase of anthropogenic emissions. Climate change has diverse impacts on O3 and its budgets through changes in circulation and meteorological variables. Increased water vapour causes a substantial ozone reduction especially in the tropical lower troposphere (>10 ppbv reduction over the tropical ocean. On the other hand, an enhanced stratosphere-troposphere exchange of ozone, which increases by 80% due to doubling CO2, contributes to ozone increases in the extratropical free troposphere which subsequently propagate to the surface. Projected higher temperatures favour ozone chemical production and PAN decomposition which lead to high surface ozone levels in certain regions. Enhanced convection transports ozone precursors more rapidly out of the boundary layer resulting in an increase of ozone production in the free troposphere. Lightning-produced NOx increases by about 22% in the doubled CO2 climate and contributes to ozone production.

    The response to the increase of isoprene emissions shows that the change of ozone is largely determined by background NOx levels: high

  15. Earth Radiation Budget Experiment (ERBE) Data Sets for Global Environment and Climate Change Studies

    Bess, T. Dale; Carlson, Ann B.; Denn, Fredrick M.

    1997-01-01

    For a number of years there has been considerable interest in the earth's radiation budget (ERB) or energy balance, and entails making the best measurements possible of absorbed solar radiation, reflected shortwave radiation (RSW), thermal outgoing longwave radiation (OLR), and net radiation. ERB data are fundamental to the development of realistic climate models and studying natural and anthropogenic perturbations of the climate. Much of the interest and investigations in the earth's energy balance predated the age of earth-orbiting satellites (Hunt et al., 1986). Beginning in the mid 1960's earth-orbiting satellites began to play an important role in making measurements of the earth's radiation flux although much effort had gone into measuring ERB parameters prior to 1960 (House et al., 1986). Beginning in 1974 and extending until the present time, three different satellite experiments (not all operating at the same time) have been making radiation budget measurements almost continually in time. Two of the experiments were totally dedicated to making radiation budget measurements of the earth, and the other experiment flown on NOAA sun-synchronous AVHRR weather satellites produced radiation budget parameters as a by-product. The heat budget data from the AVHRR satellites began collecting data in June 1974 and have operated almost continuously for 23 years producing valuable data for long term climate monitoring.

  16. Long Path Quantum Cascade Laser Based Sensor for Environment Sensing/Ambient Detection of CH4 and N2O

    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.

  17. Carbon emission from global hydroelectric reservoirs revisited.

    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.

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

    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.

  19. CH4 and N2O emissions embodied in international trade of meat

    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)

  20. CO2/CH4 Separation by a Mixed Matrix Membrane of Polymethylpentyne/MIL-53 Particles

    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.

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

    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.

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

    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.

  3. Preparing for budget-based payment methodologies: global payment and episode-based payment.

    Hudson, Mark E

    2015-10-01

    Use of budget-based payment methodologies (capitation and episode-based bundled payment) has been demonstrated to drive value in healthcare delivery. With a focus on high-volume, high-cost surgical procedures, inclusion of anaesthesiology services in these methodologies is likely. This review provides a summary of budget-based payment methodologies and practical information necessary for anaesthesiologists to prepare for participation in these programmes. Although few examples of anaesthesiologists' participation in these models exist, an understanding of the structure of these programmes and opportunities for participation are available. Prospective preparation in developing anaesthesiology-specific bundled payment profiles and early participation in pathway development associated with selected episodes of care are essential for successful participation as a gainsharing partner. With significant opportunity to contribute to care coordination and cost management, anaesthesiology can play an important role in budget-based payment programmes and should expect to participate as full gainsharing partners. Precise costing methodologies and accurate economic modelling, along with identification of quality management and cost control opportunities, will help identify participation opportunities and appropriate payment and gainsharing agreements. Anaesthesiology-specific examples with budget-based payment models are needed to help guide increased participation in these programmes.

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

    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...

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

    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

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

    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.

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

    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.

  8. Identifying sources of methane sampled in the Arctic using δ13C in CH4 and Lagrangian particle dispersion modelling.

    Cain, Michelle; France, James; Pyle, John; Warwick, Nicola; Fisher, Rebecca; Lowry, Dave; Allen, Grant; O'Shea, Sebastian; Illingworth, Samuel; Jones, Ben; Gallagher, Martin; Welpott, Axel; Muller, Jennifer; Bauguitte, Stephane; George, Charles; Hayman, Garry; Manning, Alistair; Myhre, Catherine Lund; Lanoisellé, Mathias; Nisbet, Euan

    2016-04-01

    An airmass of enhanced methane was sampled during a research flight at ~600 m to ~2000 m altitude between the North coast of Norway and Svalbard on 21 July 2012. The largest source of methane in the summertime Arctic is wetland emissions. Did this enhancement in methane come from wetland emissions? The airmass was identified through continuous methane measurements using a Los Gatos fast greenhouse gas analyser on board the UK's BAe-146 Atmospheric Research Aircraft (ARA) as part of the MAMM (Methane in the Arctic: Measurements and Modelling) campaign. A Lagrangian particle dispersion model (the UK Met Office's NAME model) was run backwards to identify potential methane source regions. This was combined with a methane emission inventory to create "pseudo observations" to compare with the aircraft observations. This modelling was used to constrain the δ13C CH4 wetland source signature (where δ13C CH4 is the ratio of 13C to 12C in methane), resulting in a most likely signature of -73‰ (±4‰7‰). The NAME back trajectories suggest a methane source region of north-western Russian wetlands, and -73‰ is consistent with in situ measurements of wetland methane at similar latitudes in Scandinavia. This analysis has allowed us to study emissions from remote regions for which we do not have in situ observations, giving us an extra tool in the determination of the isotopic source variation of global methane emissions.

  9. The Boron Isotopic Composition of Elephant Dung: Inputs to the Global Boron Budget

    Williams, L. B.; Hervig, R. L.

    2011-12-01

    favor of 11B, thus increasing the δ11B of the (solid) digested material relative to the food source. This would not affect the overall BM input to the sediment because the dung contains the undigested plants. If we assume that the average B isotopic composition of dung, ~10ppm B at -20%, represents an average BM in sediment, and that the mass of sediments (1E24 g) is comparable to the mass of seawater with an average 5ppm B at +40%, then it is clear that BM plays a major role in balancing the global B budget. Note: This research was NOT funded by taxpayer dollars. The Phoenix Zoo kindly approved the proposal to sample elephant dung for this study and their support is greatly appreciated.

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

    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.

  11. Comparison of Landfill Methane Oxidation Measured Using Stable Isotope Analysis and CO2/CH4 Fluxes Measured by the Eddy Covariance Method

    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.

  12. Improving accuracy and precision of ice core δD(CH4 analyses using methane pre-pyrolysis and hydrogen post-pyrolysis trapping and subsequent chromatographic separation

    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.

  13. Nutrient Addition Leads to a Weaker CO2 Sink and Higher CH4 Emissions through Vegetation-Microclimate Feedbacks at Mer Bleue Bog, Canada

    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.

  14. Raman spectroscopic characterization of CH4 density over a wide range of temperature and pressure

    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.

  15. Experimental Equipment Validation for Methane (CH4) and Carbon Dioxide (CO2) Hydrates

    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.

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

    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.

  17. Mitigating CH4 and N2O emissions from intensive rice production systems in northern Vietnam

    Tariq, Azeem; Vu, Quynh Duong; Jensen, Lars Stoumann

    2017-01-01

    -growing seasons in northern Vietnam, to evaluate the effectiveness of drainage patterns on methane (CH4) and nitrous oxide (N2O) emissions under farmers’ variable conditions. Two improved drainage practices (pre-planting plus midseason [PM] drainage and early-season plus midseason [EM] drainage) were compared...... with local practices of water management (midseason drainage [M] and conventional continuous flooding (control) [C]) with full residue [F] and reduced residue [R] (local practice of residue management) incorporation. The GHG mitigation potential of water regimes was tested in two water management systems...... (efficient field water management [EWM] system and inefficient field water management [IWM] system). In EWM system, EM resulted an average 14% and 55% reduction in CH4 emissions compared to M with R and F respectively. The EM lowered the CH4 emissions by 67% and 43% compared to C in the EWM and IWM...

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

    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

  19. Accurate Determination of Rotational Energy Levels in the Ground State of ^{12}CH_4

    Abe, M.; Iwakuni, K.; Okubo, S.; Sasada, H.

    2013-06-01

    We have measured absolute frequencies of saturated absorption of 183 allowed and 21 forbidden transitions in the νb{3} band of ^{12}CH_4 using an optical comb-referenced difference-frequency-generation spectrometer from 86.8 to 93.1 THz (from 2890 to 3100 wn). The pump and signal sources are a 1.06-μ m Nd:YAG laser and a 1.5-μ m extended-cavity laser diode. An enhanced-cavity absorption cell increases the optical electric field and enhances the sensitivity. The typical uncertainty is 3 kHz for the allowed transitions and 12 kHz for the forbidden transitions. Twenty combination differences are precisely determined, and the scalar rotational and centrifugal distortion constants of the ground state are thereby yielded as r@ = l@ r@ = l B_{{s}} (157 122 614.2 ± 1.5) kHz, D_{{s}} (3 328.545 ± 0.031) kHz, H_{{s}} (190.90 ± 0.26) Hz, and L_{{s}} (-13.16 ± 0.76) mHz. Here, B_{{s}} is the rotational constant and D_{{s}}, H_{{s}} and L_{{s}} are the scalar quartic, sextic, octic distortion constants. The relative uncertainties are considerably smaller than those obtained from global analysis of Fourier-transform infrared spectroscopy. S. Okubo, H. Nakayama, K. Iwakuni, H. Inaba and H. Sasada, Opt. Express 19, 23878 (2011). M. Abe, K. Iwakuni, S. Okubo, and H. Sasada, J. Opt. Soc. Am. B (to be published). S. Albert, S. Bauerecker, V. Boudon, L. R. Brown, J. -P. Champion, M. Loëte, A. Nikitin, and M. Quack, Chem. Phys. 356, 131 (2009).

  20. Early Mars serpentinization-derived CH4 reservoirs, H2 induced warming and paleopressure evolution

    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.

  1. Sensitizing effects of NOx on CH4 oxidation at high pressure

    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...

  2. 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

    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.

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

    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.

  4. The ‘Alternative Quality Contract’ in Massachusetts, Based on Global Budgets, Lowered Medical Spending and Improved Quality

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

    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

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

    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

  7. Tidal influence on the sea-to-air transfer of CH4 in the coastal ocean

    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

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

    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

  9. What affects CH4/CO2 ratio in cow’s breath

    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...

  10. Presumed PDF modeling of microjet assisted CH4–H2/air turbulent flames

    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.

  11. Diurnal and seasonal variations in CH4 emission from various freshwater wetlands

    Kim, J.; Kim, J.-W.; Verma, B.; Shurpali, N.J.; Harazono, Y.; Miyata, A.; Yun, J.-I.; Tanner, B.

    2000-01-01

    Recent evidence indicates that future increases in atmospheric CO2 concentration may lead to significant increases in methane emissions from wetlands. Based on the concurrent eddy covariance measurements of CH4 and ecosystem production in freshwater wetlands. Also, we briefly discuss the current concerns of the micrometeorological community on the long-term monitoring of these greenhouse gases. 16 refs

  12. Linking soil O2, CO2, and CH4 concentrations in a wetland soil

    Elberling, Bo; Jensen, Louise Askær; Jørgensen, Christian Juncher

    2011-01-01

    and CH4 were measured in the laboratory during flooding of soil columns using a combination of planar O2 optodes and membrane inlet mass spectrometry. Microsensors were used to assess apparent diffusivity under both field and laboratory conditions. Gas concentration profiles were analyzed...... plants tissue on soil gas dynamics and greenhouse gas emissions following marked changes in water level....

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

    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

  14. BOREAS TGB-1/TGB-3 CH4 Chamber Flux Data over the NSA Fen

    Bubier, Jill L.; Moore, Tim R.; Hall, Forrest G. (Editor); Conrad, Sara K. (Editor)

    2000-01-01

    The BOREAS TGB-3 team collected methane (CH4) chamber flux measurements at the NSA fen site during May-September 1994 and June-October 1996. Gas samples were extracted approximately every 7 days from chambers and analyzed at the NSA lab facility. The data are provided in tabular ASCII files.

  15. Assessing fugitive emissions of CH4 from high-pressure gas pipelines in the UK

    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

  16. 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

    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

  17. Non-CO2 greenhouse gas emissions associated with food production: methane (CH4) and nitrous oxide (N2O)

    Carlsson-Kanyama, Annika

    2007-01-01

    It is well known that the agriculture and livestock sectors are large contributors of N 2 O and CH 4 emissions in countries with agricultural activities and that remedial measures are needed in these sectors in order to curb contributions to global warming. This study examines non- CO 2 greenhouse gas emissions associated with the production of food. Methane (CH 4 ) and nitrous oxide (N 2 O) are the most relevant greenhouse gases in this category, and they are emitted mainly in the agricultural sector. These greenhouse gases have a Global Warming Potential much higher than CO 2 itself (25- and 298-fold higher, respectively, in a 100-year perspective). Emission intensities and the corresponding uncertainties were calculated based on the latest procedures and data published by the Intergovernmental Panel on Climate Change and used to facilitate calculations comparing greenhouse gas emissions for food products and diets. When the proposed emission intensities were applied to agricultural production, the results showed products of animal origin and the cultivation of rice under water to have high emissions compared with products of vegetable origin cultivated on upland soils, such as wheat and beans. In animal production the main source of greenhouse gas emissions was methane from enteric fermentation, while emissions of nitrous oxides from fertilisers were the main sources of greenhouse gas emissions for cereal and legume cultivation. For rice cultivation, methane emissions from flooded rice fields contributed most. Other significant sources of greenhouse gas emissions during animal production were manure storage and management. We suggest that the proposed emission factors, together with the associated uncertainties, can be a tool for better understanding the potential to mitigate emissions of greenhouse gases through changes in the diet

  18. Flask sample measurements for CO2, CH4 and CO using cavity ring-down spectrometry

    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.

  19. ISLSCP II GlobalView: Atmospheric Methane Concentrations

    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...

  20. ISLSCP II GlobalView: Atmospheric Methane Concentrations

    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...

  1. Reactions of 11C recoil atoms in the systems H2O-NH3, H2O-CH4 and NH3-CH4

    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

  2. Super Rice Cropping Will Enhance Rice Yield and Reduce CH4 Emission: A Case Study in Nanjing, China

    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.

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

    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.

  4. A synthesis of the impact of Russian forests on the global carbon budget for 1961-1998

    Shvidenko, Anatoly; Nilsson, Sten

    2003-01-01

    An attempt is made to synthesize the current understanding of the impact of Russian forests on the global carbon (C) budget for the period 1961-1998 (37 years), based on a detailed inventory of pools and fluxes in 1988-1992, and a historical reconstruction of a full forest carbon budget for 1961-1998. All major intermediate indicators of the budget (phytomass, net primary production, impact of disturbances, soil respiration, etc.) were independently estimated and compared with earlier reported results. During the entire period, the C pools of Russian forest land (FL, 882.0 106 ha in 1998) increased by 433 Tg C/yr, of which 153 Tg C/yr are accumulated in live biomass, 57 Tg C/yr in above- and below-ground dead wood, and 223 Tg C/yr are sequestered in soil. A significant part of this increase deals with land-cover changes. The annual average C uptake by the FL from the atmosphere, defined by a flux-based method, is estimated to be 322 Tg C/yr for 1961-1998. The lateral transport to the lithosphere and hydrosphere comprised 47 Tg C/yr (including charcoal), which is considered part of the 'missing C sink.' The uncertainties (excluding unrecognized biases) of averages for the entire period are estimated to be in the range of ±5-8% and ±24% for major fluxes out/into the atmosphere and for net ecosystem exchange, respectively (a priori confidential probability of 0.9). If the impact of land-cover change is excluded, the average annual sink in 1961-1998, estimated by both pool- and flux-based methods, was 268 ± 94 and 272 ± 68 Tg C/yr, respectively. The reported results are in line with recent estimates for Northern Eurasia made by inverse modeling at the continental scale, if land classes other than forests contribute to the total sink of terrestrial vegetation

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

    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.

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

    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

  7. US Global Change Research Program Distributed Cost Budget Interagency Funds Transfer from DOE to NSF

    Uhle, Maria [National Science Foundation (NSF), Washington, DC (United States)

    2016-09-22

    These funds were transferred from DOE to NSF as DOE's contribution to the U.S. Global Change Research Program in support of 4 internationalnactivities/programs as approved by the U.S. Global Change Research Program on 14 March 2014. The programs are the International Geosphere-Biosphere Programme, the DIVERSITAS programme, and the World Climate Research Program. All program awards ended as of 09-23-2015.

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

    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. Spatial and Temporal Variations in the Partial Pressure and Emission of CO2 and CH4 in and Amazon Floodplain Lake

    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

  10. Projected Impact of Climate Change on the Water and Salt Budgets of the Arctic Ocean by a Global Climate Model

    Miller, James R.; Russell, Gary L.

    1996-01-01

    The annual flux of freshwater into the Arctic Ocean by the atmosphere and rivers is balanced by the export of sea ice and oceanic freshwater. Two 150-year simulations of a global climate model are used to examine how this balance might change if atmospheric greenhouse gases (GHGs) increase. Relative to the control, the last 50-year period of the GHG experiment indicates that the total inflow of water from the atmosphere and rivers increases by 10% primarily due to an increase in river discharge, the annual sea-ice export decreases by about half, the oceanic liquid water export increases, salinity decreases, sea-ice cover decreases, and the total mass and sea-surface height of the Arctic Ocean increase. The closed, compact, and multi-phased nature of the hydrologic cycle in the Arctic Ocean makes it an ideal test of water budgets that could be included in model intercomparisons.

  11. 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

    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.

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

    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.

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

    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. Simulations and experimental investigations of the competitive adsorption of CH4 and CO2 on low-rank coal vitrinite.

    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.

  15. Emissions of N2O and CH4 from agricultural soils amended with two types of biogas residues

    Odlare, M.; Abubaker, J.; Lindmark, J.; Pell, M.; Thorin, E.; Nehrenheim, E.

    2012-01-01

    Biogas residues contain valuable plant nutrients, important to the crops and also to soil microorganisms. However, application of these materials to the soils may contribute to the emission of greenhouse gases (GHG) causing global warming and climate change. In the present study, incubation experiment was carried out, where the emission rates of N 2 O and CH 4 were measured after amending two soils with two types of biogas residues: (1) a regular residue from a large scale biogas plant (BR) and (2) a residue from an ultra-filtration membrane unit connected to a pilot-scale biogas plant (BRMF). The emissions of N 2 O and CH 4 were measured at two occasions: at 24 h and at 7 days after residue amendment, respectively. Amendment with filtered biogas residues (BRMF) led to an increase in N 2 O emissions with about 6–23 times in organic and clay soil, respectively, in comparison to unfiltered biogas residues (BR). Methane emission was detected in small amounts when filtered biogas residue was added to the soil. Amendment of unfiltered biogas to the organic soil resulted in net consumption. In conclusion, fertilization with BRMF can be combined with risk of an increase N 2 O emission, especially when applied to organic soils. However, in order to transfer these results to real life agriculture, large scale field studies need to be carried out. -- Highlights: ► Membrane filtration of biogas process water is a promising method. ► Fertilization of biogas residue may increase the N 2 O emission from soil. ► Organic soils produced higher emissions than clay soils.

  16. Effects of aerosol from biomass burning on the global radiation budget

    Penner, Joyce E.; Dickinson, Robert E.; O'Neill, Christine A.

    1992-01-01

    An analysis is made of the likely contribution of smoke particles from biomass burning to the global radiation balance. These particles act to reflect solar radiation directly; they also can act as cloud condensation nuclei, increasing the reflectivity of clouds. Together these effects, although uncertain, may add up globally to a cooling effect as large as 2 watts per square meter, comparable to the estimated contribution to sulfate aerosols. Anthropogenic increases of smoke emission thus may have helped weaken the net greenhouse warming from anthropogenic trace gases.

  17. Dissolved organic carbon, CO2, and CH4 concentrations and their stable isotope ratios in thermokarst lakes on the Qinghai-Tibetan Plateau

    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.

  18. Plumbing the global carbon cycle: Integrating inland waters into the terrestrial carbon budget

    Cole, J.; Prairie, Y.T.; Caraco, N.; McDowell, W.H.; Tranvil, L.; Striegl, R.G.; Duarte, C.M.; Kortelainen, P.; Downing, J.A.; Middelburg, J.J.; Melack, J.

    2007-01-01

    Because freshwater covers such a small fraction of the Earth’s surface area, inland freshwater ecosystems (particularly lakes, rivers, and reservoirs) have rarely been considered as potentially important quantitative components of the carbon cycle at either global or regional scales. By taking

  19. Carbon budgets of biological soil crusts at micro-, meso-, and global scales

    Sancho, Leopoldo G; Belnap, Jayne; Colesie, Claudia; Raggio, Jose; Weber, Bettina

    2016-01-01

    The importance of biocrusts in the ecology of arid lands across all continents is widely recognized. In spite of this broad distribution, contributions of biocrusts to the global biogeochemical cycles have only recently been considered. While these studies opened a new view on the global role of biocrusts, they also clearly revealed the lack of data for many habitats and of overall standards for measurements and analysis. In order to understand carbon cycling in biocrusts and the progress which has been made during the last 15 years, we offer a multi-scale approach covering different climatic regions. We also include a discussion on available measurement techniques at each scale: A micro-scale section focuses on the individual organism level, including modeling based on the combination of field and lab data. The meso-scale section addresses the CO2 exchange of a complete ecosystem or at the community level. Finally, we consider the contribution of biocrusts at a global scale, giving a general perspective of the most relevant findings regarding the role of biological soil crusts in the global terrestrial carbon cycle.

  20. Possibilities for the reduction of CO2- and CH4-emissions of natural gas

    Muessig, S.

    1994-01-01

    The use of fossil fuels increases the portion of greenhouse gases, especially CO 2 and CH 4 . In this paper firstly the specific emission rates of these greenhouse gases for the various fuels are compared. Secondly possibilities for the reduction of CO 2 and CH 4 for natural gas which are relatively small anyhow are discussed. Thirdly the use of renewable energy within the gas industry and the ocean and into depleted reservoirs are discussed. It is shown that the efficient use of energy of the fossil fuel natural gas is most successful in all branches of gas consumption to decrease emission. Combined-cycle processes, cogeneration as well as modern domestic heating systems are described. Fuel cells and the application of hydrogen is shortly discussed. (orig.)

  1. Thermodynamic calculations in the system CH4-H2O and methane hydrate phase equilibria

    Circone, S.; Kirby, S.H.; Stern, L.A.

    2006-01-01

    Using the Gibbs function of reaction, equilibrium pressure, temperature conditions for the formation of methane clathrate hydrate have been calculated from the thermodynamic properties of phases in the system CH4-H 2O. The thermodynamic model accurately reproduces the published phase-equilibria data to within ??2 K of the observed equilibrium boundaries in the range 0.08-117 MPa and 190-307 K. The model also provides an estimate of the third-law entropy of methane hydrate at 273.15 K, 0.1 MPa of 56.2 J mol-1 K-1 for 1/n CH4??H 2O, where n is the hydrate number. Agreement between the calculated and published phase-equilibria data is optimized when the hydrate composition is fixed and independent of the pressure and temperature for the conditions modeled. ?? 2006 American Chemical Society.

  2. Feeding the world's increasing population while limiting climate change impacts: linking N2O and CH4 emissions from agriculture to population growth

    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.

  3. Soil CH4 and N2O Emissions from Rice Paddy Fields in Southern Brazil as Affected by Crop Management Levels: a Three-Year Field Study

    Tiago Zschornack

    2018-05-01

    Full Text Available ABSTRACT Rice yield increases in response to improvements in crop management, but the impact on greenhouse gas (GHG emissions in the subtropical region of Southern Brazil remains unknown. A three-year field study was developed aiming to evaluate the impact that an increase in crop management levels (high and very high has on soil methane (CH4 and nitrous oxide (N2O emissions, as compared to the level (medium currently adopted by farmers in Southern Brazil. Differences in crop management included seed and fertilizer rates, irrigation, and pesticide use. The effect of crop management levels on the annual partial global warming potential (pGWP = CH4 × 25 + N2O × 298 ranged from 7,547 to 17,711 kg CO2eq ha−1 and this effect was larger than on the rice grain yield (9,280 to 12,260 kg ha−1, resulting in approximately 60 % higher yield-scaled GHG with the high crop management level compared to the current level. Soil CH4 emissions accounted for 98 % of pGWP in the flooded rice season, whereas N2O prevailed during the drained non-rice season (≈65 %. Although it was impossible to relate emissions to any individual input or practice, soil CH4 emissions in the rice season were linearly related to the biomass produced by the rice crop (p<0.01 and by ryegrass in the previous non-rice season (p<0.1, both of which were possibly related to the supply of labile C for methanogenesis. A future increase in rice yield as a result of the adoption of improved crop management may require additional agricultural practices (e.g., intermittent irrigation to offset the increased GHG emissions.

  4. The cost of pipelining climate change mitigation. An overview of the economics of CH4, CO2 and H2 transportation

    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.

  5. Impact of Equivalence Ratio on the Macrostructure of Premixed Swirling CH 4 /Air and CH 4 /O 2 /CO 2 Flames

    Watanabe, Hirotatsu

    2015-06-15

    Premixed CH4/O2/CO2 flames (oxy-flames) and CH4/air flames (air-flames) were experimentally studied in a swirl-stabilized combustor. For comparing oxy and air flames, the same equivalence ratio and adiabatic flame temperature were used. CO2 dilution was adjusted to attain the same adiabatic temperature for the oxy-flame and the corresponding air-flame while keeping the equivalence ratio and Reynolds number (=20,000) the same. For high equivalence ratios, we observed flames stabilized along the inner and outer shear layers of the swirling flow and sudden expansion, respectively, in both flames. However, one notable difference between the two flames appears as the equivalence ratio reaches 0.60. At this point, the outer shear layer flame disappears in the air-flame while it persists in the oxy-flame, despite the lower burning velocity of the oxy-flame. Prior PIV measurements (Ref. 9) showed that the strains along the outer shear layer are higher than along the inner shear layer. Therefore, the extinction strain rates in both flames were calculated using a counter-flow premixed twin flame configuration. Calculations at the equivalence ratio of 0.60 show that the extinction strain rate is higher in the oxy than in the air flame, which help explain why it persists on the outer shear layer with higher strain rate. It is likely that extinction strain rates contribute to the oxy-flame stabilization when air flame extinguish in the outer shear layer. However, the trend reverses at higher equivalence ratio, and the cross point of the extinction strain rate appears at equivalence ratio of 0.64.

  6. In-operando elucidation of bimetallic CoNi nanoparticles during high-temperature CH 4 /CO 2 reaction

    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

  7. Fluxes of CH4 and N2O in aspen stands grown under ambient and twice-ambient CO2

    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...

  8. Process for the separation of contaminant or mixture of contaminants from a Ch4-comprising gaseous feed streem

    2012-01-01

    The invention provides a process for the separation of a contaminant or mixture of contaminants from a CH4-comprising gaseous feed streem, comprising the subsequent steps of: a) passing a CH4-comprising gaseous feed streem comprising the contaminant or the mixture of contaminants in to and through a

  9. Emissions of CO2 and CH4 from sludge treatment reed beds depend on system management and sludge loading

    Olsson, Linda; Dam Larsen, Julie; Ye, Siyuan

    2014-01-01

    , the SD had no vegetation and a poor dewatering capacity, which resulted in anaerobic conditions favoring CH4 emission. In contrast, the well-managed STRB had more aerobic conditions in the sludge residue resulting in low CH4 emission rates. We conclude that well-designed and well-managed STRBs have a low...

  10. Comprehensive effects of a sedge plant on CH4 and N2O emissions in an estuarine marsh

    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.

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

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

    2016-01-01

    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 lar...

  12. BOREAS TGB-1 NSA CH4 and CO2 Chamber Flux Data

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

    2000-01-01

    The BOREAS TGB-1 team made methane (CH4) and carbon dioxide (CO2) dark chamber flux measurements at the NSA-OJP, NSA-OBS, NSA-BP, and NSA-YJP sites from 16-May-1994 through 13-Sep-1994. Gas samples were extracted approximately every 7 days from dark chambers and analyzed at the NSA lab facility. The data are provided in tabular ASCII files.

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

    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

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

    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

  15. Bioelectrochemical methane (CH4) production in anaerobic digestion at different supplemental voltages.

    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.

  16. Catalytic reduction of NOx with H2/CO/CH4 over PdMOR catalysts

    Pieterse, Johannis A.Z.; Booneveld, Saskia

    2007-01-01

    Conversion of NO x with reducing agents H 2 , CO and CH 4 , with and without O 2 , H 2 O, and CO 2 were studied with catalysts based on MOR zeolite loaded with palladium and cerium. The catalysts reached high NO x to N 2 conversion with H 2 and CO (>90% conversion and N 2 selectivity) range under lean conditions. The formation of N 2 O is absent in the presence of both H 2 and CO together with oxygen in the feed, which will be the case in lean engine exhaust. PdMOR shows synergic co-operation between H 2 and CO at 450-500 K. The positive effect of cerium is significant in the case of H 2 and CH 4 reducing agent but is less obvious with H 2 /CO mixture and under lean conditions. Cerium lowers the reducibility of Pd species in the zeolite micropores. The catalysts showed excellent stability at temperatures up to 673 K in a feed with 2500 ppm CH 4 , 500 ppm NO, 5% O 2 , 10% H 2 O (0-1% H 2 ), N 2 balance but deactivation is noticed at higher temperatures. Combining results of the present study with those of previous studies it shows that the PdMOR-based catalysts are good catalysts for NO x reduction with H 2 , CO, hydrocarbons, alcohols and aldehydes under lean conditions at temperatures up to 673 K. (author)

  17. Modified ZIF-8 mixed matrix membrane for CO2/CH4 separation

    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.

  18. Wastes Management Can Minimize CH4 and N2O Emissions from Wetlands in Indonesia

    Abdul Hadi

    2015-07-01

    Full Text Available Paddy (Oriza sativa L. and Oil palm (Elaeis guineensis Jack are two important crops and are potential to produce wastes which may lead to huge greenhouse gas emissions if they are not managed properly.  Open burning and conventional composting are commonly practiced by farmers and/or planters to managed agricultural wastes in Indonesia.  A series of research has been carried out  to elucidate (1 the reductions of CH4 and N2O due to incertion of a catalitic converter on burning kiln, (2 the best composting technique of oil palm field wastes, and (3 the effects of oil palm field wastes compost application in oil palm fields and of paddy field wastes biochar in integrated oil palm-paddy fields.  The results showed that CH4 and N2O emissions from paddy field wastes (i.e., rice straw or rice husk was lower than that from oil palm empty fruit bunch (EFB.  Furthermore, insertion of a catalytic converter into pyrolysis installation reduced the CO2, CH4 and N2O emissions from paddy field wastes as much as 14.5, 17.8 and 11.1%, respectively.  Incorporation of EFB compost did not increase greenhouse gas emission from oil palm fields. These results suggest that biochar and EFB compost can be practiced to manage agricultural wastes in Indonesia.

  19. Synthesis of Fine Mo2C Powder from Prereduced Mo in Undiluted CH4 Flow

    Cetinkaya, S.; Eroglu, S.

    2017-10-01

    The carburization behavior of prereduced Mo was investigated in undiluted CH4 flow at 900-1000 K. Prior to the experiments, equilibrium thermodynamic analysis was carried out in the Mo-C-H system. The products were characterized by mass measurement, x-ray diffraction and scanning electron microscopy techniques. A single Mo2C phase was obtained within 45 min, 5 min, and 2.5 min at 900 K, 950 K, and 1000 K, respectively, at CH4 contents higher than the predicted ones. The reasons for this behavior were discussed in terms of CH4 stability, open tube flow, and self-created atmosphere in the powder bed. The fractional conversion-time curves indicated that the carburization kinetics followed a linear rate law. The Mo2C crystallite size (26-37 nm) and platelet thickness (50-100 nm) were found to be smaller than those of the parent Mo phase. These findings were attributable to the defects formed as a result of stresses associated with the reduction and the carburization.

  20. Catalytic performance of activated carbon supported cobalt catalyst for CO2 reforming of CH4.

    Zhang, Guojie; Su, Aiting; Du, Yannian; Qu, Jiangwen; Xu, Ying

    2014-11-01

    Syngas production by CO2 reforming of CH4 in a fixed bed reactor was investigated over a series of activated carbon (AC) supported Co catalysts as a function of Co loading (between 15 and 30wt.%) and calcination temperature (Tc=300, 400 or 500°C). The catalytic performance was assessed through CH4 and CO2 conversions and long-term stability. XRD and SEM were used to characterize the catalysts. It was found that the stability of Co/AC catalysts was strongly dependent on the Co loading and calcination temperature. For the loadings (25wt.% for Tc=300°C), stable activities have been achieved. The loading of excess Co (>wt.% 25) causes negative effects not only on the performance of the catalysts but also on the support surface properties. In addition, the experiment showed that ultrasound can enhance and promote dispersion of the active metal on the carrier, thus improving the catalytic performance of the catalyst. The catalyst activity can be long-term stably maintained, and no obvious deactivation has been observed in the first 2700min. After analyzing the characteristics, a reaction mechanism for CO2 reforming of CH4 over Co/AC catalyst was proposed. Copyright © 2014 Elsevier Inc. All rights reserved.

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

    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.

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

    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.

  3. Contribution of vehicle exhaust to the global N2O budget

    Becker, K.H.; Loerzer, J.C.; Kurtenbach, R.; Wiesen, P.; Jensen, T.E.; Wallington, T.J.

    2000-01-01

    Assessment of the impact of vehicle emissions on the global environment requires accurate data concerning nitrous oxide (N 2 O) emissions. We report herein 'real world' N 2 O emissions from road vehicles in a tunnel in Wuppertal, Germany, together with 'laboratory' emission measurements conducted at the Ford Motor Company using a chassis dynamometer with a standard driving cycle for 26 different cars and trucks. Consistent results were obtained from both approaches suggesting that a good approximation of the average emission factor (g N 2 O/g CO 2 )=(4±2) x 10 -5 . This corresponds to an emission rate of 11-5 mg N 2 O/km for vehicles with fuel economies of 12-6 1/100 km (20-40 miles/US gallon). N 2 O emissions from vehicles have a global warming impact, which is 1-2% of that of the CO 2 emissions from vehicles. We estimate an annual emission of (0.12±0.06) Tg yr -1 of N 2 O (0.08±0.04 Tg N yr -1 ) from the global vehicle fleet which represents 1-4% of the atmospheric growth rate of this species. These results update and supersede our previous study of N 2 O emissions from vehicles. (author)

  4. Numerical Simulation and Industrial Experimental Research on the Coherent Jet with "CH4 + N2" Mixed Fuel Gas

    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.

  5. Development of multi-sensor global cloud and radiance composites for earth radiation budget monitoring from DSCOVR

    Khlopenkov, Konstantin; Duda, David; Thieman, Mandana; Minnis, Patrick; Su, Wenying; Bedka, Kristopher

    2017-10-01

    The Deep Space Climate Observatory (DSCOVR) enables analysis of the daytime Earth radiation budget via the onboard Earth Polychromatic Imaging Camera (EPIC) and National Institute of Standards and Technology Advanced Radiometer (NISTAR). Radiance observations and cloud property retrievals from low earth orbit and geostationary satellite imagers have to be co-located with EPIC pixels to provide scene identification in order to select anisotropic directional models needed to calculate shortwave and longwave fluxes. A new algorithm is proposed for optimal merging of selected radiances and cloud properties derived from multiple satellite imagers to obtain seamless global hourly composites at 5-km resolution. An aggregated rating is employed to incorporate several factors and to select the best observation at the time nearest to the EPIC measurement. Spatial accuracy is improved using inverse mapping with gradient search during reprojection and bicubic interpolation for pixel resampling. The composite data are subsequently remapped into EPIC-view domain by convolving composite pixels with the EPIC point spread function defined with a half-pixel accuracy. PSF-weighted average radiances and cloud properties are computed separately for each cloud phase. The algorithm has demonstrated contiguous global coverage for any requested time of day with a temporal lag of under 2 hours in over 95% of the globe.

  6. CO2 and CH4 fluxes and carbon balance in the atmospheric interaction of boreal peatlands

    Alm, J.

    1997-01-01

    Release of CO 2 from peat was studied using IR analyzer in a range of boreal peatlands under varying nutrient status and moisture conditions. Root associated CO 2 efflux was separated from the total release by experiments both in the field and in a greenhouse. Emissions of CO 2 and CH 4 (the latter by gas chromatography) were measured during the snow-covered period and their contribution to the annual fluxes of these gases was inspected. Ecosystem exchange of CO 2 under varying irradiation, temperature and moisture conditions was measured at different microsites at two peatland sites with different nutrient ecology. One site represented minerotrophic conditions during a wet growing season and the other site ombrotrophic conditions during an exceptionally dry growing season. Annual carbon balances were compiled for the two sites, and the role of the microsites in the annual carbon balance and CH 4 release was studied. The Holocene history of CO 2 sequestration and CH 4 emission dynamics in a raised mire were simulated using lateral and vertical growth rates derived from radiocarbon ages of peat samples from mire bottom and vertical cores. The model was formulated for a geographic information system (GIS). Artificial or natural lowering of water table increased CO 2 release from peat. A drought lasting from late May to July caused a 90 g C m 2 net loss in the annual C balance of a natural ombrotrophic bog. In drained forested sites the increase in peat CO 2 release could be even 100 %, but the development of the tree layer at least partially compensated for these losses. Wet conditions induced a net accumulation of 67 g C m -2 a -1 in the minerotrophic fen site, while the long term average accumulation rate is estimated to be only 15 g C m -2 a -1 for Finnish fens. Carbon balance in boreal peatlands is thus extremely sensitive to year-to-year climatic variations. Root activity of vascular plants contributed to the total peat CO 2 efflux by 10-40 % as root respiration

  7. Global Observations of Aerosols and Clouds from Combined Lidar and Passive Instruments to Improve Radiation Budget and Climate Studies

    Winker, David M.

    1999-01-01

    Current uncertainties in the effects of clouds and aerosols on the Earth radiation budget limit our understanding of the climate system and the potential for global climate change. Pathfinder Instruments for Cloud and Aerosol Spaceborne Observations - Climatologie Etendue des Nuages et des Aerosols (PICASSO-CENA) is a recently approved satellite mission within NASA's Earth System Science Pathfinder (ESSP) program which will address these uncertainties with a unique suite of active and passive instruments. The Lidar In-space Technology Experiment (LITE) demonstrated the potential benefits of space lidar for studies of clouds and aerosols. PICASSO-CENA builds on this experience with a payload consisting of a two-wavelength polarization-sensitive lidar, an oxygen A-band spectrometer (ABS), an imaging infrared radiometer (IIR), and a wide field camera (WFC). Data from these instruments will be used to measure the vertical distributions of aerosols and clouds in the atmosphere, as well as optical and physical properties of aerosols and clouds which influence the Earth radiation budget. PICASSO-CENA will be flown in formation with the PM satellite of the NASA Earth Observing System (EOS) to provide a comprehensive suite of coincident measurements of atmospheric state, aerosol and cloud optical properties, and radiative fluxes. The mission will address critical uncertainties iin the direct radiative forcing of aerosols and clouds as well as aerosol influences on cloud radiative properties and cloud-climate radiation feedbacks. PICASSO-CENA is planned for a three year mission, with a launch in early 2003. PICASSO-CENA is being developed within the framework of a collaboration between NASA and CNES.

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

    Soussana, J.F.; Allard, V.; Pilegaard, K.; Ambus, P.; Amman, C.; Campbell, C.; Ceschia, E.; Clifton-Brown, J.; Czobel, S.; Domingues, R.; Flechard, C.; Fuhrer, J.; Hensen, A.; Horvath, L.; Jones, M.; Kasper, G.J.; Martin, C.; Nagy, Z.; Neftel, A.; Raschi, A.; Baronti, S.

    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

  9. 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

    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.

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

    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

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

    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

  12. Global model simulations of the impact of ocean-going ships on aerosols, clouds, and the radiation budget

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

    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.

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

    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 %.

  15. Spatial and Temporal Variability of CO2 and CH4 Concentrations in the Atmospheric Surface Layer over West Siberia

    Belan, Boris D.; Machida, Toshinobu; Sasakawa, Motoki; Davydov, Denis K.; Fofonov, Alexander V.; Krasnov, Oleg A.; Maksyutov, Shamil; Arshinov, Mikhail Yu.

    2015-04-01

    The investigation of greenhouse gas behavior in the atmosphere plays a key role in predicting the global changes of Earth's climate. In this connection, of particular importance is the study of the distribution of sources/sinks of trace gases in the atmospheric surface layer over the different regions of the globe. In order to fill a gap in the data on greenhouse gas concentrations in Russia, National Institute for Environmental Studies (NIES, Japan) and Institute of Atmospheric Optics (IAO SB RAS, Russia) established a network for GHG monitoring (JR-STATION, Japan-Russia Siberian Tall Tower Inland Observation Network). Gas analyzers and meteorological sensors were mounted at radio relay towers located in different regions of West Siberia. The checking equipment was placed in containers at the tower base. In the containers, the climatic parameters optimal for gas analyzer operation were maintained. The work on the network development started in 2001. Since at each of the sites the measurement duration could be different, in this paper we present the data of the greenhouse gas monitoring for eight sites which give the primary idea on the spatial distribution and temporal dynamics of CO2 and CH4 in the atmospheric surface layer over West Siberia. The analysis of the data showed that the average increase in concentration of carbon dioxide by results of our measurements in this territory increases within 1.95 - 2.53 ppm/year, depending on the area. The analysis of long-term data testifies about existence of growth of concentration of methane within 3.2 - 7.2 ppb / year. The presence of a distributed network of the sites operating in the monitoring regime makes it possible not only to investigate the temporal dynamics of CO2 and CH4 at each site and to determine the spatial differences between the concentrations by comparing the data, but also to plot the distribution charts for different moments of time. This work was supported by the Global Environment Research

  16. Compact Solar Spectrometer Column CO2, and CH4 Observations: Performance Evaluation at Multiple North American TCCON Sites

    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

  17. Role of Megafauna and Frozen Soil in the Atmospheric CH4 Dynamics

    Zimov, Sergey; Zimov, Nikita

    2014-01-01

    Modern wetlands are the world’s strongest methane source. But what was the role of this source in the past? An analysis of global 14C data for basal peat combined with modelling of wetland succession allowed us to reconstruct the dynamics of global wetland methane emission through time. These data show that the rise of atmospheric methane concentrations during the Pleistocene-Holocene transition was not connected with wetland expansion, but rather started substantially later, only 9 thousand years ago. Additionally, wetland expansion took place against the background of a decline in atmospheric methane concentration. The isotopic composition of methane varies according to source. Owing to ice sheet drilling programs past dynamics of atmospheric methane isotopic composition is now known. For example over the course of Pleistocene-Holocene transition atmospheric methane became depleted in the deuterium isotope, which indicated that the rise in methane concentrations was not connected with activation of the deuterium-rich gas clathrates. Modelling of the budget of the atmospheric methane and its isotopic composition allowed us to reconstruct the dynamics of all main methane sources. For the late Pleistocene, the largest methane source was megaherbivores, whose total biomass is estimated to have exceeded that of present-day humans and domestic animals. This corresponds with our independent estimates of herbivore density on the pastures of the late Pleistocene based on herbivore skeleton density in the permafrost. During deglaciation, the largest methane emissions originated from degrading frozen soils of the mammoth steppe biome. Methane from this source is unique, as it is depleted of all isotopes. We estimated that over the entire course of deglaciation (15,000 to 6,000 year before present), soils of the mammoth steppe released 300–550 Pg (1015 g) of methane. From current study we conclude that the Late Quaternary Extinction significantly affected the global

  18. Uranium isotopic compositions of the crust and ocean: Age corrections, U budget and global extent of modern anoxia

    Tissot, François L. H.; Dauphas, Nicolas

    2015-10-01

    the variability of the 238U/235U ratio on Pb-Pb and U-Pb ages and provide analytical formulas to calculate age corrections as a function of the age and isotopic composition of the sample. The crustal ratio may be used in calculation of Pb-Pb and U-Pb ages of continental crust rocks and minerals when the U isotopic composition is unknown. In cosmochemistry, the search for 247Cm (t1/2 = 15.6 Myr), an extinct short-lived radionuclide that decays into 235U, is important for understanding how r-process nuclides were synthesized in stars and learning about the astrophysical context of solar system formation (Chen and Wasserburg, 1981; Wasserburg et al., 1996; Nittler and Dauphas, 2006; Brennecka et al., 2010b; Tissot et al., 2015). In both terrestrial and extraterrestrial samples, variations in the 238U/235U ratio affect Pb-Pb ages (and depending on the analytical protocols, U-Pb ages). Therefore, samples dated by these techniques need to have their U isotopic compositions measured (Stirling et al., 2005, 2006; Weyer et al., 2008; Amelin et al., 2010; Brennecka et al., 2010b; Brennecka and Wadhwa, 2012; Connelly et al., 2012; Goldmann et al., 2015) or uncertainties on the U isotopic composition should be propagated into age calculations. In low temperature aqueous geochemistry, U isotopic fractionation between U4+ and U6+ (driven in part by nuclear field shift effects; Bigeleisen, 1996; Schauble, 2007; Abe et al., 2008), makes U isotopes potential tracers of paleoredox conditions (Montoya-Pino et al., 2010; Brennecka et al., 2011a; Kendall et al., 2013, 2015; Asael et al., 2013; Andersen et al., 2014; Dahl et al., 2014; Goto et al., 2014; Noordmann et al., 2015). The present paper aims at constraining some aspects of the global budget of uranium in the modern oceans using 238U/235U isotope variations, which involves characterizing the U isotopic composition of seawater and several reservoirs involved in the uranium oceanic budget. Uranium can exist in two oxidation states

  19. Experimental measurements of vapor-liquid equilibria of the H2O + CO2 + CH4 ternary system

    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.

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

    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.

  1. High-accuracy continuous airborne measurements of greenhouse gases (CO2 and CH4) during BARCA

    Chen, H.; Winderlich, J.; Gerbig, C.; Hoefer, A.; Rella, C. W.; Crosson, E. R.; van Pelt, A. D.; Steinbach, J.; Kolle, O.; Beck, V.; Daube, B. C.; Gottlieb, E. W.; Chow, V. Y.; Santoni, G. W.; Wofsy, S. C.

    2009-12-01

    High-accuracy continuous measurements of greenhouse gases (CO2 and CH4) during the BARCA (Balanço Atmosférico Regional de Carbono na Amazônia) phase B campaign in Brazil in May 2009 were accomplished using a newly available analyzer based on the cavity ring-down spectroscopy (CRDS) technique. This analyzer was flown without a drying system or any in-flight calibration gases. Water vapor corrections associated with dilution and pressure-broadening effects for CO2 and CH4 were derived from laboratory experiments employing measurements of water vapor by the CRDS analyzer. Before the campaign, the stability of the analyzer was assessed by laboratory tests under simulated flight conditions. During the campaign, a comparison of CO2 measurements between the CRDS analyzer and a nondispersive infrared (NDIR) analyzer on board the same aircraft showed a mean difference of 0.22±0.09 ppm for all flights over the Amazon rain forest. At the end of the campaign, CO2 concentrations of the synthetic calibration gases used by the NDIR analyzer were determined by the CRDS analyzer. After correcting for the isotope and the pressure-broadening effects that resulted from changes of the composition of synthetic vs. ambient air, and applying those concentrations as calibrated values of the calibration gases to reprocess the CO2 measurements made by the NDIR, the mean difference between the CRDS and the NDIR during BARCA was reduced to 0.05±0.09 ppm, with the mean standard deviation of 0.23±0.05 ppm. The results clearly show that the CRDS is sufficiently stable to be used in flight without drying the air or calibrating in flight and the water corrections are fully adequate for high-accuracy continuous airborne measurements of CO2 and CH4.

  2. 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

    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...

  3. PEBAX®/PAN Hollow Fiber Membranes for CO2/CH4 Separation

    Esposito, E.; Clarizia, G.; Bernardo, P.; Jansen, J. C.; Sedláková, Zuzana; Izák, Pavel; Curcio, S.; de Cindio, B.; Tasselli, F.

    2015-01-01

    Roč. 94, SI (2015), s. 53-61 ISSN 0255-2701. [International Congress of Chemical and Process Engineering CHISA 2014 /21./ and Conference PRES 2014 /17./. Prague, 23.08.2014-27.08.2014] R&D Projects: GA ČR GA14-12695S Grant - others:INRP(IT) MicroPERLA:PON01_01840 Institutional support: RVO:67985858 Keywords : composite membrane * hollow fibers * CO2/CH4 separation Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 2.154, year: 2015

  4. Bayesian model comparison using Gauss approximation on multicomponent mass spectra from CH4 plasma

    Kang, H.D.; Dose, V.

    2004-01-01

    We performed Bayesian model comparison on mass spectra from CH4 rf process plasmas to detect radicals produced in the plasma. The key ingredient for its implementation is the high-dimensional evidence integral. We apply Gauss approximation to evaluate the evidence. The results were compared with those calculated by the thermodynamic integration method using Markov Chain Monte Carlo technique. In spite of very large difference in the computation time between two methods a very good agreement was obtained. Alternatively, a Monte Carlo integration method based on the approximated Gaussian posterior density is presented. Its applicability to the problem of mass spectrometry is discussed

  5. Vapor-liquid equilibrium thermodynamics of N2 + CH4 - Model and Titan applications

    Thompson, W. R.; Zollweg, John A.; Gabis, David H.

    1992-01-01

    A thermodynamic model is presented for vapor-liquid equilibrium in the N2 + CH4 system, which is implicated in calculations of the Titan tropospheric clouds' vapor-liquid equilibrium thermodynamics. This model imposes constraints on the consistency of experimental equilibrium data, and embodies temperature effects by encompassing enthalpy data; it readily calculates the saturation criteria, condensate composition, and latent heat for a given pressure-temperature profile of the Titan atmosphere. The N2 content of condensate is about half of that computed from Raoult's law, and about 30 percent greater than that computed from Henry's law.

  6. Carbon nanosheets by microwave plasma enhanced chemical vapor deposition in CH4-Ar system

    Wang Zhipeng; Shoji, Mao; Ogata, Hironori

    2011-01-01

    We employ a new gas mixture of CH 4 -Ar to fabricate carbon nanosheets by microwave plasma enhanced chemical vapor deposition at the growth temperature of less than 500 deg. C. The catalyst-free nanosheets possess flower-like structures with a large amount of sharp edges, which consist of a few layers of graphene sheets according to the observation by transmission electron microscopy. These high-quality carbon nanosheets demonstrated a faster electron transfer between the electrolyte and the nanosheet surface, due to their edge defects and graphene structures.

  7. Field detection of CO and CH4 by NIR 2f modulation laser spectroscopy

    A Khorsandi

    2011-12-01

    Full Text Available   A novel compact fiber-coupled NIR system based on a DFB diode laser source is employed as a portable and sensitive gas sensor for trace detection of combustion pollutant molecules. We demonstrate the performance of such an NIR gas sensor by tracing the absorption lines of CO and CH4 using 2f-WMS technique at moderate temperature of T ~ 600°C in the recuperator channel of an industrial furnace provided by Mobarakeh steel company. This measurement shows the excellent sensitivity of the applied NIR gas sensor to the on-line and in-situ monitoring of such molecular species.

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

    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

  9. Nitric Oxide Mediates Biofilm Formation and Symbiosis in Silicibacter sp. Strain TrichCH4B.

    Rao, Minxi; Smith, Brian C; Marletta, Michael A

    2015-05-05

    Nitric oxide (NO) plays an important signaling role in all domains of life. Many bacteria contain a heme-nitric oxide/oxygen binding (H-NOX) protein that selectively binds NO. These H-NOX proteins often act as sensors that regulate histidine kinase (HK) activity, forming part of a bacterial two-component signaling system that also involves one or more response regulators. In several organisms, NO binding to the H-NOX protein governs bacterial biofilm formation; however, the source of NO exposure for these bacteria is unknown. In mammals, NO is generated by the enzyme nitric oxide synthase (NOS) and signals through binding the H-NOX domain of soluble guanylate cyclase. Recently, several bacterial NOS proteins have also been reported, but the corresponding bacteria do not also encode an H-NOX protein. Here, we report the first characterization of a bacterium that encodes both a NOS and H-NOX, thus resembling the mammalian system capable of both synthesizing and sensing NO. We characterized the NO signaling pathway of the marine alphaproteobacterium Silicibacter sp. strain TrichCH4B, determining that the NOS is activated by an algal symbiont, Trichodesmium erythraeum. NO signaling through a histidine kinase-response regulator two-component signaling pathway results in increased concentrations of cyclic diguanosine monophosphate, a key bacterial second messenger molecule that controls cellular adhesion and biofilm formation. Silicibacter sp. TrichCH4B biofilm formation, activated by T. erythraeum, may be an important mechanism for symbiosis between the two organisms, revealing that NO plays a previously unknown key role in bacterial communication and symbiosis. Bacterial nitric oxide (NO) signaling via heme-nitric oxide/oxygen binding (H-NOX) proteins regulates biofilm formation, playing an important role in protecting bacteria from oxidative stress and other environmental stresses. Biofilms are also an important part of symbiosis, allowing the organism to remain in a

  10. BOREAS TGB-3 CH4 and CO2 Chamber Flux Data over NSA Upland Sites

    Savage, Kathleen; Hall, Forrest G. (Editor); Conrad, Sara K. (Editor); Moore, Tim R.

    2000-01-01

    The BOReal Ecosystem-Atmosphere Study Trace Gas Biogeochemistry (BOREAS TGB-3) team collected methane and carbon dioxide (CH4, CO2) chamber flux measurements at the Northern Study Area (NSA) Fen, Old Black Spruce (OBS), Young Jack Pine (YJP), and auxiliary sites along Gillam Road and the 1989 burn site. Gas samples were extracted from chambers and analyzed at the NSA lab facility approximately every 7 days during May to September 1994 and June to October 1996. The data are provided in tabular ASCII files.

  11. Global atmospheric carbon budget: results from an ensemble of atmospheric CO2 inversions

    P. Peylin

    2013-10-01

    Full Text Available Atmospheric CO2 inversions estimate surface carbon fluxes from an optimal fit to atmospheric CO2 measurements, usually including prior constraints on the flux estimates. Eleven sets of carbon flux estimates are compared, generated by different inversions systems that vary in their inversions methods, choice of atmospheric data, transport model and prior information. The inversions were run for at least 5 yr in the period between 1990 and 2010. Mean fluxes for 2001–2004, seasonal cycles, interannual variability and trends are compared for the tropics and northern and southern extra-tropics, and separately for land and ocean. Some continental/basin-scale subdivisions are also considered where the atmospheric network is denser. Four-year mean fluxes are reasonably consistent across inversions at global/latitudinal scale, with a large total (land plus ocean carbon uptake in the north (−3.4 Pg C yr−1 (±0.5 Pg C yr−1 standard deviation, with slightly more uptake over land than over ocean, a significant although more variable source over the tropics (1.6 ± 0.9 Pg C yr−1 and a compensatory sink of similar magnitude in the south (−1.4 ± 0.5 Pg C yr−1 corresponding mainly to an ocean sink. Largest differences across inversions occur in the balance between tropical land sources and southern land sinks. Interannual variability (IAV in carbon fluxes is larger for land than ocean regions (standard deviation around 1.06 versus 0.33 Pg C yr−1 for the 1996–2007 period, with much higher consistency among the inversions for the land. While the tropical land explains most of the IAV (standard deviation ~ 0.65 Pg C yr−1, the northern and southern land also contribute (standard deviation ~ 0.39 Pg C yr−1. Most inversions tend to indicate an increase of the northern land carbon uptake from late 1990s to 2008 (around 0.1 Pg C yr−1, predominantly in North Asia. The mean seasonal cycle appears to be well constrained by the atmospheric data over

  12. Environmental and vegetation controls on the spatial variability of CH4 emission from wet-sedge and tussock tundra ecosystems in the Arctic.

    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.

  13. The use of CO 2 as an additive for ignition delay and pollutant control in CH 4 /air autoignition

    Tingas, Efstathios Al.; Im, Hong G.; Kyritsis, Dimitrios C.; Goussis, Dimitris A.

    2017-01-01

    The effect of CO2 dilution on the adiabatic and isochoric autoignition of CH4/air mixtures is analyzed with Computational Singular Perturbation (CSP) algorithmic tools, with a particular emphasis on the determination of the features of the chemical

  14. An Ultralow Power Fast-Response Nano-TCD CH4 sensor for UAV Airborne Measurements, Phase I

    National Aeronautics and Space Administration — In this project, KWJ proposes to develop a low power, fast response, lightweight miniature CH4 measurement system based on KWJ nano-TCD sensor for airborne...

  15. Biochars as Potential Adsorbers of CH4, CO2 and H2S

    Sumathi Sethupathi

    2017-01-01

    Full Text Available Methane gas, as one of the major biogases, is a potential source of renewable energy for power production. Biochar can be readily used to purify biogas contaminants such as H2S and CO2. This study assessed the adsorption of CH4, H2S, and CO2 onto four different types of biochars. The adsorption dynamics of biochars were investigated in a fixed-bed column, by determining the breakthrough curves and adsorption capacities of biochars. The physicochemical properties of biochars were considered to justify the adsorption performance. The results showed that CH4 was not adsorbed well by the subjected biochars whereas CO2 and H2S were successfully captured. The H2S and CO2 breakthrough capacity were related to both the surface adsorption and chemical reaction. The adsorption capacity was in the following order: perilla > soybean stover > Korean oak > Japanese oak biochars. The simultaneous adsorption also leads to a competition of sorption sites. Biochars are a promising material for the biogas purification industry.

  16. OEDGE modeling of the DIII-D double null (CH4)-C-13 puffing experiment

    Elder, J.D.; Wampler, W.R.; McLean, A.G.; Stangeby, P.C.; Allen, S.L.; Bray, B.D.; Brooks, N.H.; Leonard, A.W.; Unterberg, Ezekial A.; Watkins, J.G.

    2011-01-01

    Unbalanced double null ELMy H-mode configurations in DIII-D are used to simulate the situation in ITER high triangularity, burning plasma magnetic equilibria, where the second X-point lies close to the top of the vacuum vessel, creating a secondary divertor region at the upper blanket modules. The measured plasma conditions in the outer secondary divertor closely duplicated those projected for ITER. (CH4)-C-13 was injected into the secondary outer divertor to simulate sputtering there. The majority of the C-13 found was in the secondary outer divertor. This material migration pattern is radically different than that observed for main wall (CH4)-C-13 injections into single null configurations where the deposition is primarily at the inner divertor. The implications for tritium codeposition resulting from sputtering at the secondary divertor in ITER are significant since release of tritium from Be co-deposits at the main wall bake temperature for ITER, 240 degrees C, is incomplete. The principal features of the measured C-13 deposition pattern have been replicated by the OEDGE interpretive code.

  17. Burning Behaviour of High-Pressure CH4-H2-Air Mixtures

    Jacopo D'Alessio

    2013-01-01

    Full Text Available Experimental characterization of the burning behavior of gaseous mixtures has been carried out, analyzing spherical expanding flames. Tests were performed in the Device for Hydrogen-Air Reaction Mode Analysis (DHARMA laboratory of Istituto Motori—CNR. Based on a high-pressure, constant-volume bomb, the activity is aimed at populating a systematic database on the burning properties of CH4, H2 and other species of interest, in conditions typical of internal combustion (i.c. engines and gas turbines. High-speed shadowgraph is used to record the flame growth, allowing to infer the laminar burning parameters and the flame stability properties. Mixtures of CH4, H2 and air have been analyzed at initial temperature 293÷305 K, initial pressure 3÷18 bar and equivalence ratio  = 1.0. The amount of H2 in the mixture was 0%, 20% and 30% (vol.. The effect of the initial pressure and of the Hydrogen content on the laminar burning velocity and the Markstein length has been evaluated: the relative weight and mutual interaction has been assessed of the two controlling parameters. Analysis has been carried out of the flame instability, expressed in terms of the critical radius for the onset of cellularity, as a function of the operating conditions.

  18. Serpentinization and the Formation of H2 and CH4 on Celestial Bodies (Planets, Moons, Comets).

    Holm, N G; Oze, C; Mousis, O; Waite, J H; Guilbert-Lepoutre, A

    2015-07-01

    Serpentinization involves the hydrolysis and transformation of primary ferromagnesian minerals such as olivine ((Mg,Fe)2SiO4) and pyroxenes ((Mg,Fe)SiO3) to produce H2-rich fluids and a variety of secondary minerals over a wide range of environmental conditions. The continual and elevated production of H2 is capable of reducing carbon, thus initiating an inorganic pathway to produce organic compounds. The production of H2 and H2-dependent CH4 in serpentinization systems has received significant interdisciplinary interest, especially with regard to the abiotic synthesis of organic compounds and the origins and maintenance of life in Earth's lithosphere and elsewhere in the Universe. Here, serpentinization with an emphasis on the formation of H2 and CH4 are reviewed within the context of the mineralogy, temperature/pressure, and fluid/gas chemistry present in planetary environments. Whether deep in Earth's interior or in Kuiper Belt Objects in space, serpentinization is a feasible process to invoke as a means of producing astrobiologically indispensable H2 capable of reducing carbon to organic compounds.

  19. Summary of LOX/CH4 Thruster Technology Development at NASA/MSFC

    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.

  20. Inverse modelling of European CH4 emissions during 2006-2012 using different inverse models and reassessed atmospheric observations

    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

  1. Implications for carbon processing beneath the Greenland Ice Sheet from dissolved CO2 and CH4 concentrations of subglacial discharge

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

    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.

  3. Metal–organic frameworks for H2 and CH4 storage: insights on the pore geometry–sorption energetics relationship

    Al Kordi, Mohamed; Belmabkhout, Youssef; Cairns, Amy; Eddaoudi, Mohamed

    2017-01-01

    This study aims to assess the possibility of improving H2 and CH4 binding affinity to the aromatic walls of a designed new Metal-Organic Framework (MOF) through simultaneous dispersive interactions. It is suggested here that desirable H2 and CH4 storage media at low pressures require narrow uniform pores associated with large surface area, a trade-off that is challenging to achieve.

  4. Organic chemistry of NH3 and HCN induced by an atmospheric abnormal glow discharge in N2-CH4 mixtures

    2010-01-01

    Abstract The formation of the chemical products produced in an atmospheric glow discharge fed by a N2-CH4 gas mixture has been studied using Fourier Transform InfraRed (FTIR) and Optical Emission Spectrometry (OES). The measurements were carried out in a flowing regime at ambient temperature and pressure with CH4 concentrations ranging from 0.5% to 2%. In the recorded emission spectra the lines of the second positive system CN system and the first negative s...

  5. Quantifying the Variability of CH4 Emissions from Pan-Arctic Lakes with Lake Biogeochemical and Landscape Evolution Models

    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.

  6. Flux and distribution of methane (CH4) in the Gunsan Basin of the southeastern Yellow Sea, off the Western Korea.

    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.

  7. Metal–organic frameworks for H2 and CH4 storage: insights on the pore geometry–sorption energetics relationship

    Al Kordi, Mohamed

    2017-02-09

    This study aims to assess the possibility of improving H2 and CH4 binding affinity to the aromatic walls of a designed new Metal-Organic Framework (MOF) through simultaneous dispersive interactions. It is suggested here that desirable H2 and CH4 storage media at low pressures require narrow uniform pores associated with large surface area, a trade-off that is challenging to achieve.

  8. Contribution of rice straw carbon to CH4 emission from rice paddies using 13C-enriched rice straw

    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.

  9. Effects of shifting growth stage and regulating temperature on seasonal variation of CH4 emission from rice

    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.

  10. Global atmospheric budget of acetaldehyde: 3-D model analysis and constraints from in-situ and satellite observations

    D. B. Millet

    2010-04-01

    Full Text Available We construct a global atmospheric budget for acetaldehyde using a 3-D model of atmospheric chemistry (GEOS-Chem, and use an ensemble of observations to evaluate present understanding of its sources and sinks. Hydrocarbon oxidation provides the largest acetaldehyde source in the model (128 Tg a−1, a factor of 4 greater than the previous estimate, with alkanes, alkenes, and ethanol the main precursors. There is also a minor source from isoprene oxidation. We use an updated chemical mechanism for GEOS-Chem, and photochemical acetaldehyde yields are consistent with the Master Chemical Mechanism. We present a new approach to quantifying the acetaldehyde air-sea flux based on the global distribution of light absorption due to colored dissolved organic matter (CDOM derived from satellite ocean color observations. The resulting net ocean emission is 57 Tg a−1, the second largest global source of acetaldehyde. A key uncertainty is the acetaldehyde turnover time in the ocean mixed layer, with quantitative model evaluation over the ocean complicated by known measurement artifacts in clean air. Simulated concentrations in surface air over the ocean generally agree well with aircraft measurements, though the model tends to overestimate the vertical gradient. PAN:NOx ratios are well-simulated in the marine boundary layer, providing some support for the modeled ocean source. We introduce the Model of Emissions of Gases and Aerosols from Nature (MEGANv2.1 for acetaldehyde and ethanol and use it to quantify their net flux from living terrestrial plants. Including emissions from decaying plants the total direct acetaldehyde source from the land biosphere is 23 Tg a−1. Other terrestrial acetaldehyde sources include biomass burning (3 Tg a−1 and anthropogenic emissions (2 Tg a−1. Simulated concentrations in the continental boundary layer are generally unbiased and capture the spatial

  11. Identification of spikes associated with local sources in continuous time series of atmospheric CO, CO2 and CH4

    El Yazidi, Abdelhadi; Ramonet, Michel; Ciais, Philippe; Broquet, Gregoire; Pison, Isabelle; Abbaris, Amara; Brunner, Dominik; Conil, Sebastien; Delmotte, Marc; Gheusi, Francois; Guerin, Frederic; Hazan, Lynn; Kachroudi, Nesrine; Kouvarakis, Giorgos; Mihalopoulos, Nikolaos; Rivier, Leonard; Serça, Dominique

    2018-03-01

    REBS methods after the best adjustment of parameter values. At PDM, measurements made by two analyzers located 200 m from each other allow us to confirm that the CH4 spikes identified in one of the time series but not in the other correspond to a local source from a sewage treatment facility in one of the observatory buildings. From this experiment, we also found that the REBS method underestimates the number of positive anomalies in the CH4 data caused by local sewage emissions. As a conclusion, we recommend the use of the SD method, which also appears to be the easiest one to implement in automatic data processing, used for the operational filtering of spikes in greenhouse gases time series at global and regional monitoring stations of networks like that of the ICOS atmosphere network.

  12. Identification of spikes associated with local sources in continuous time series of atmospheric CO, CO2 and CH4

    A. El Yazidi

    2018-03-01

    the SD and the REBS methods after the best adjustment of parameter values. At PDM, measurements made by two analyzers located 200 m from each other allow us to confirm that the CH4 spikes identified in one of the time series but not in the other correspond to a local source from a sewage treatment facility in one of the observatory buildings. From this experiment, we also found that the REBS method underestimates the number of positive anomalies in the CH4 data caused by local sewage emissions. As a conclusion, we recommend the use of the SD method, which also appears to be the easiest one to implement in automatic data processing, used for the operational filtering of spikes in greenhouse gases time series at global and regional monitoring stations of networks like that of the ICOS atmosphere network.

  13. Cold season emissions dominate the Arctic tundra methane budget

    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.

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

    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....

  15. Adsorption of CH4 on nitrogen- and boron-containing carbon models of coal predicted by density-functional theory

    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.

  16. Isotopomer analysis of production and consumption mechanisms of N2O and CH4 in an advanced wastewater treatment system.

    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.

  17. Influence of Meteorology and interrelationship with greenhouse gases (CO2 and CH4) at a suburban site of India

    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.

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

    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.

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

    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.

  20. Modeling Plasma-based CO2 and CH4 Conversion in Mixtures with N2, O2 and H2O: the Bigger Plasma Chemistry Picture

    Wang, Weizong; Snoeckx, Ramses; Zhang, Xuming; Cha, Min; Bogaerts, Annemie

    2018-01-01

    performed regarding the single component gases, i.e. CO2 splitting and CH4 reforming, as well as for two component mixtures, i.e. dry reforming of methane (CO2/CH4), partial oxidation of methane (CH4/O2), artificial photosynthesis (CO2/H2O), CO2

  1. Isocyanic acid in a global chemistry transport model: Tropospheric distribution, budget, and identification of regions with potential health impacts

    Young, Paul. J.; Emmons, Louisa K.; Roberts, James M.; Lamarque, Jean-FrançOis; Wiedinmyer, Christine; Veres, Patrick; Vandenboer, Trevor C.

    2012-05-01

    This study uses a global chemical transport model to estimate the distribution of isocyanic acid (HNCO). HNCO is toxic, and concentrations exceeding 1 ppbv have been suggested to have negative health effects. Based on fire studies, HNCO emissions were scaled to those of hydrogen cyanide (30%), resulting in yearly total emissions of 1.5 Tg for 2008, from both anthropogenic and biomass burning sources. Loss processes included heterogeneous uptake (pH dependent), dry deposition (like formic acid), and reaction with the OH radical (k = 1 × 10-15 molecule-1 cm3 s-1). Annual mean surface HNCO concentrations were highest over parts of China (maximum of 470 pptv), but episodic fire emissions gave much higher levels, exceeding 4 ppbv in tropical Africa and the Amazon, and exceeding 10 ppbv in Southeast Asia and Siberia. This suggests that large biomass burning events could result in deleterious health effects for populations in these regions. For the tropospheric budget, using the model-calculated pH the HNCO lifetime was 37 days, with the split between dry deposition and heterogeneous loss being 95%:5%. Fixing the heterogeneous loss rate at pH = 7 meant that this process dominated, accounting for ˜70% of the total loss, giving a lifetime of 6 days, and resulting in upper tropospheric concentrations that were essentially zero. However, changing the pH does not notably impact the high concentrations found in biomass burning regions. More observational data is needed to evaluate the model, as well as a better representation of the likely underestimated biofuel emissions, which could mean more populations exposed to elevated HNCO concentrations.

  2. MERLIN and MICROCARB : Preparation of 2 space missions for CO2 and CH4

    Deniel, Carole; Millet, Bruno; Buisson, Francois; Pierangelo, Clémence; Jouglet, Denis; Bréon, Francois-Marie; Bousquet, Philippe; Chevallier, Fréderic; Crevoisier, Cyril; Ehret, Gerhard

    2017-04-01

    In collaboration with the research community and with close European partnerships, the French space agency, CNES is developing or co-developing two missions to be launched by 2021, MERLIN and MICROCARB, that are dedicated respectively to the observation of atmospheric concentrations of CH4 and CO2. Both missions are based on innovative instrumentation, microsatellites, specific algorithm inversion processes and calibration /validation approaches. Both will deliver very accurate weighted atmospheric column measurements over the globe for the two species that play a major role in climate change. The MERLIN (MEthane Remote sensing LIdar missioN) space segment consists of the new Myriade-Evolutions platform type (range of 400 kg) developed under CNES control, and of the first IPDA (Integrated Path Differential Absorption) LIDAR (Light Detecting And Ranging) instrument developed under DLR responsibility (Germany). The MERLIN satellite will be operated at an altitude of around 500 km, on a sun-synchronous orbit, either at 06:00 or 18:00 of the local time of the ascending node. The main science objective is to bring a significant improvement on the knowledge of CH4 emissions and sinks, derived from estimates of the CH4 column-averaged dry-mixing ratio at a 50 km horizontal resolution, with a precision of 1% and a challenging targeted accuracy of 0.2%. The MICROCARB mission is based on a compact grating spectrometer (around 60 kg) onboard a Myriade micro-satellite platform (170kg range). The satellite will fly on a sun-synchronous orbit at altitude around 650 km and at around 10h30 local time for the ascending node. The instrument will measure the reflected solar radiance in four spectral ranges in the infrared. Two bands with CO2 absorptions, at 1.6 µm (weak absorptions) and 2.0 µm (strong absorptions), allows retrieving the quantity of molecules of CO2. Two bands centered around 0.76 and 1.27 µm sample oxygen absorption lines and provide a proxy of the atmospheric

  3. Atmospheric modeling of Mars CH4 subsurface clathrates releases mimicking SAM and 2003 Earth-based detections

    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

  4. Forecasting the future reimbursement system of Korean National Health Insurance: a contemplation focusing on global budget and Neo-KDRG-based payment systems.

    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.

  5. A 156 kyr smoothed history of the atmospheric greenhouse gases CO2, CH4, and N2O and their radiative forcing

    Köhler, Peter; Nehrbass-Ahles, Christoph; Schmitt, Jochen; Stocker, Thomas F.; Fischer, Hubertus

    2017-06-01

    Continuous records of the atmospheric greenhouse gases (GHGs) CO2, CH4, and N2O are necessary input data for transient climate simulations, and their associated radiative forcing represents important components in analyses of climate sensitivity and feedbacks. Since the available data from ice cores are discontinuous and partly ambiguous, a well-documented decision process during data compilation followed by some interpolating post-processing is necessary to obtain those desired time series. Here, we document our best possible data compilation of published ice core records and recent measurements on firn air and atmospheric samples spanning the interval from the penultimate glacial maximum ( ˜ 156 kyr BP) to the beginning of the year 2016 CE. We use the most recent age scales for the ice core data and apply a smoothing spline method to translate the discrete and irregularly spaced data points into continuous time series. These splines are then used to compute the radiative forcing for each GHG using well-established, simple formulations. We compile only a Southern Hemisphere record of CH4 and discuss how much larger a Northern Hemisphere or global CH4 record might have been due to its interpolar difference. The uncertainties of the individual data points are considered in the spline procedure. Based on the given data resolution, time-dependent cutoff periods of the spline, defining the degree of smoothing, are prescribed, ranging from 5000 years for the less resolved older parts of the records to 4 years for the densely sampled recent years. The computed splines seamlessly describe the GHG evolution on orbital and millennial timescales for glacial and glacial-interglacial variations and on centennial and decadal timescales for anthropogenic times. Data connected with this paper, including raw data and final splines, are available at PANGAEA.871273" target="_blank">doi:10.1594/PANGAEA.871273.

  6. Impacts of feedlot floor condition, deposition frequency, and inhibitors on N2O and CH4 emissions from feedlot dung and urine patches.

    Liao, Wenhua; Liu, Chunjing; Gao, Zhiling

    2018-04-09

    Patches of dung and urine are major contributors to the feedlot gas emissions. This study investigated the impacts of dung deposition frequency (partly reflecting animal stocking density of a feedlot), dairy feedlot floor conditions (old floor indicated with the presence of consolidated manure pad [CMP] vs. new floor with the absence of consolidated manure pad [CMPn]), and application of dicyandiamide (DCD) and hydroquinone (HQ) on nitrous oxide (N 2 O) and methane (CH 4 ) emissions from patches in the laboratory, and the integrative impacts were expressed in terms of global warming potential (CO 2 -equivalent). Dung deposition frequency, feedlot floor condition, and application of inhibitors showed inverse impacts on N 2 O and CH 4 emissions from patches. Greenhouse gas (GHG) emissions from the dung, urine, and dung+urine patches on the CMP feedlot surface were approximately 7.48, 87.35, and 7.10 times those on the CMPn feedlot surface (P emissions from CMP and CMPn feedlot surfaces under high deposition frequency condition were approximately 10 and 1.7 times those under low-frequency condition. Moreover, application of HQ slightly reduced the GHG emission from urine patches, by 14.9% (P > 0.05), while applying DCD or DCD+HQ significantly reduced the GHG, by 60.3% and 65.0%, respectively (P emission factors for feedlots. In the future, field measurements to quantitatively evaluate the relative contribution of nitrification and denitrification to the N 2 O emissions of feedlot surfaces are highly required for effective N 2 O control. This study shows that feedlot CH 4 and N 2 O emissions inversely respond to the dicyandiamide (DCD) application. Applying DCD significantly reduces GHG emissions of feedlot urine patches. Feedlot floor condition and stocking density strongly impact feedlot GHG emissions. Including feedlot floor condition and stocking density in the feedlot EF determining process is necessary.

  7. A 156 kyr smoothed history of the atmospheric greenhouse gases CO2, CH4, and N2O and their radiative forcing

    P. Köhler

    2017-06-01

    Full Text Available Continuous records of the atmospheric greenhouse gases (GHGs CO2, CH4, and N2O are necessary input data for transient climate simulations, and their associated radiative forcing represents important components in analyses of climate sensitivity and feedbacks. Since the available data from ice cores are discontinuous and partly ambiguous, a well-documented decision process during data compilation followed by some interpolating post-processing is necessary to obtain those desired time series. Here, we document our best possible data compilation of published ice core records and recent measurements on firn air and atmospheric samples spanning the interval from the penultimate glacial maximum ( ∼  156 kyr BP to the beginning of the year 2016 CE. We use the most recent age scales for the ice core data and apply a smoothing spline method to translate the discrete and irregularly spaced data points into continuous time series. These splines are then used to compute the radiative forcing for each GHG using well-established, simple formulations. We compile only a Southern Hemisphere record of CH4 and discuss how much larger a Northern Hemisphere or global CH4 record might have been due to its interpolar difference. The uncertainties of the individual data points are considered in the spline procedure. Based on the given data resolution, time-dependent cutoff periods of the spline, defining the degree of smoothing, are prescribed, ranging from 5000 years for the less resolved older parts of the records to 4 years for the densely sampled recent years. The computed splines seamlessly describe the GHG evolution on orbital and millennial timescales for glacial and glacial–interglacial variations and on centennial and decadal timescales for anthropogenic times. Data connected with this paper, including raw data and final splines, are available at doi:10.1594/PANGAEA.871273.

  8. Budget Options

    2000-01-01

    This volume-part of the Congressional Budget Office's (CBO's) annual report to the House and Senate Committees on the Budget-is intended to help inform policymakers about options for the federal budget...

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

    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

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

    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

  11. Rapid labelling of radiopharmaceuticals using 11CO2 and 11CH4

    Crouzel, C.

    1988-07-01

    In the past two decades, much effort has been devoted to the development of new molecules, labelled with β+ emitters usable for Positron Emission Tomography. Gaseous forms of 11 C ( 11 CO 2 or 11 CH 4 ) must be converted to a reactive form known as a ''radioactive precursor'': 11 C-methanol, 11 C-formaldehyde, 11 C-acetone, 11 C-phosgene, 11 C-diazomethane, 11 C-methylamine. These precursors are used to label radiopharmaceuticals. Few examples are given: 11 C-prazosin, 11 C-CGP 12177, 11 C-pindolol. Such synthesis procedures require strong initial activity (1.5 Ci). The processes are therefore remotely controlled or automated, and confined to shielded cells. Small laboratory robots have lately been introduced for this type of production

  12. Plasma discharge in N2 + CH4 at low pressures - Experimental results and applications to Titan

    Thompson, W. Reid; Henry, Todd J.; Schwartz, Joel M.; Khare, B. N.; Sagan, Carl

    1991-01-01

    Results are reported from laboratory continuous-flow plasma-discharge experiments designed to simulate the formation of hydrocarbons and nitriles from N2 and CH4 in the atmosphere of Titan. Gas-chromatography and mass-spectrometry data were obtained in experiments lasting up to 100 h at temperature 295 K and pressure 17 or 0.24 mbar, modeling (1) cosmic-ray-induced processes in the Titan troposphere and (2) processes related to stratospheric aurorae excited by energetic electrons and ions from the Saturn magnetosphere, respectively. The results are presented in extensive tables and graphs, and the 0.24-mbar yields are incorporated into an eddy-mixing model to give stratospheric column abundances and mole fractions in good agreement with Voyager IRIS observations.

  13. Nitrogen Incorporation in CH4-N2 Photochemical Aerosol Produced by Far UV Irradiation

    Trainer, Melissa G.; Jimenez, Jose L.; Yung, Yuk L.; Toon, Owen B.; Tolbert, Margaret A.

    2012-01-01

    Nitrile incorporation into Titan aerosol accompanying hydrocarbon chemistry is thought to be driven by extreme UV wavelengths (lambda irradiated gas. The aerosol mass greatly decreases when N2 is removed, indicating that N2 plays a major role in aerosol production. Because direct dissociation of N2 is highly improbable given the immeasurably low cross-section at the wavelengths studied, the chemical activation of N2 must occur via another pathway. Any chemical activation of N2 at wavelengths > 120 nm is presently unaccounted for in atmospheric photochemical models. We suggest that reaction with CH radicals produced from CH4 photolysis may provide a mechanism for incorporating N into the molecular structure of the aerosol. Further work is needed to understand the chemistry involved, as these processes may have significant implications for prebiotic chemistry on the early Earth and similar planets.

  14. Effect of CH4–Air Ratios on Gas Explosion Flame Microstructure and Propagation Behaviors

    Ying Zhang

    2012-10-01

    Full Text Available To reveal the inner mechanism of gas explosion dynamic behavior affected by gas equivalent concentration, a high speed Schlieren image system and flow field measurement technology was applied to record the gas explosion flame propagation and flame structure transition. The results show that a flame front structure transition occurs, followed by a flame accelerating propagation process. The laminar to turbulence transition was the essential cause of the flame structure changes. The laminar flame propagation behavior was influenced mainly by gas expansion and fore-compressive wave effect, while the turbulent flame speed mostly depended on turbulence intensity, which also played an important role in peak value of the explosive pressure and flame speed. On the condition that the laminar-turbulent transition was easier to form, the conclusion was drawn that, the lowest CH4 concentration for maximum overpressure can be obtained, which was the essential reason why the ideal explosive concentration differs under different test conditions.

  15. Measurements and models of CO2 and CH4 Flux in the Baltimore/Washington area.

    Dickerson, R. R.; Ren, X.; Salawitch, R. J.; Ahn, D.; Karion, A.; Shepson, P. B.; Whetstone, J. R.; Martin, C.

    2017-12-01

    Direct measurements of concentrations of pollutants such as CO2 and CH4 can be combined with wind fields to determine the flux of these species and to evaluate emissions inventories or models. The mass balance approach, assumng linear flow into and out of a volume set over a city, works best where wind fields are simplest. Over typical American east coast cities, upwind sources and complex circulation (e.g., the sea breeze) complicate such analyses. We will present findings from a coupled measurement and modeling project involving a network of surface-based tower measurements, aircraft observations, and remote sensing that constrain model calculations. Summer and winter scenarios are contrasted, and results help evaluate the emissions of short-lived pollutants. Determinations are compared to several emissions inventories and are being used to help States evaluate evaluate plans for pollution control.

  16. Measurements and Experimental Database Review for Laminar Flame Speed Premixed Ch4/Air Flames

    Zubrilin, I. A.; Matveev, S. S.; Matveev, S. G.; Idrisov, D. V.

    2018-01-01

    Laminar flame speed (SL ) of CH4 was determined at atmospheric pressure and initial gas temperatures in range from 298 to 358 K. The heat flux method was employed to measure the flame speed in non-stretched flames. The kinetic mechanism GRI 3.0 [1] were used to simulate SL . The measurements were compared with available literature results. The data determined with the heat flux method agree with some previous burner measurements and disagree with the data from some vessel closed method and counterflow method. The GRI 3.0 mechanism was able to reproduce the present experiments. Laminar flame speed was determined at pressures range from of 1 to 20 atmospheres through mechanism GRI 3.0. Based on experimental data and calculations was obtained SL dependence on pressure and temperature. The resulting of dependence recommended use during the numerical simulation of methane combustion.

  17. Collision of H+ + CH4 at 30 eV: A simulation study

    Gao, Cong-Zhang; Wang, Jing; Zhang, Feng-Shou

    2013-01-01

    The process of proton impinging upon CH 4 molecule has been theoretically studied at 30 eV. The study is based on time-dependent local density approximation coupled with molecular dynamics model. The electronic density evolution, ionic motion, and the scattering angle are presented. We found that the mechanism of target ionization in present simulation is electron capture. The predicted rainbow angle is in good agreement with experiments and previous calculations. By comparing the scattering angle from present calculation with that from classical collision, we found that the nuclear stopping is dominant in small impact parameters, and the discrepancy in large impact parameters may be due to the neglect of electronic stopping in classical collision

  18. BOREAS TGB-5 CO2, CH4 and CO Chamber Flux Data Over the NSA

    Burke, Roger; Hall, Forrest G. (Editor); Conrad, Sara K. (Editor); Zepp, Richard

    2000-01-01

    The BOReal Ecosystem-Atmosphere Study Trace Gas Biogeochemistry (BOREAS TGB-5) team collected a variety of trace gas concentration and flux measurements at several NSA sites. This data set contains carbon dioxide (CO2), methane (CH4), and carbon monoxide (CO) chamber flux measurements conducted in 1994 at upland forest sites that experienced stand-replacement fires. These measurements were acquired to understand the impact of fires on soil biogeochemistry and related changes in trace gas exchange in boreal forest soils. Relevant ancillary data, including data concerning the soil temperature, solar irradiance, and information from nearby un-burned control sites, are included to provide a basis for modeling the regional impacts of fire and climate changes on trace gas biogeochemistry. The data are provided in tabular ASCII files.

  19. Reduced gas seepages in ophiolitic complexes: Evidences for multiple origins of the H2-CH4-N2 gas mixtures

    Vacquand, Christèle; Deville, Eric; Beaumont, Valérie; Guyot, François; Sissmann, Olivier; Pillot, Daniel; Arcilla, Carlo; Prinzhofer, Alain

    2018-02-01

    This paper proposes a comparative study of reduced gas seepages occurring in ultrabasic to basic rocks outcropping in ophiolitic complexes based on the study of seepages from Oman, the Philippines, Turkey and New Caledonia. This study is based on analyses of the gas chemical composition, noble gases contents, stable isotopes of carbon, hydrogen and nitrogen. These seepages are mostly made of mixtures of three main components which are H2, CH4 and N2 in various proportions. The relative contents of the three main gas components show 4 distinct types of gas mixtures (H2-rich, N2-rich, N2-H2-CH4 and H2-CH4). These types are interpreted as reflecting different zones of gas generation within or below the ophiolitic complexes. In the H2-rich type, associated noble gases display signatures close to the value of air. In addition to the atmospheric component, mantle and crustal contributions are present in the N2-rich, N2-H2-CH4 and H2-CH4 types. H2-bearing gases are either associated with ultra-basic (pH 10-12) spring waters or they seep directly in fracture systems from the ophiolitic rocks. In ophiolitic contexts, ultrabasic rocks provide an adequate environment with available Fe2+ and alkaline conditions that favor H2 production. CH4 is produced either directly by reaction of dissolved CO2 with basic-ultrabasic rocks during the serpentinization process or in a second step by H2-CO2 interaction. H2 is present in the gas when no more carbon is available in the system to generate CH4. The N2-rich type is notably associated with relatively high contents of crustal 4He and in this gas type N2 is interpreted as issued mainly from sediments located below the ophiolitic units.

  20. Sensitivity analysis of a new SWIR-channel measuring tropospheric CH 4 and CO from space

    Jongma, Rienk T.; Gloudemans, Annemieke M. S.; Hoogeveen, Ruud W. M.; Aben, Ilse; de Vries, Johan; Escudero-Sanz, Isabel; van den Oord, Gijsbertus; Levelt, Pieternel F.

    2006-08-01

    In preparation for future atmospheric space missions a consortium of Dutch organizations is performing design studies on a nadir viewing grating-based imaging spectrometer using OMI and SCIAMACHY heritage. The spectrometer measures selected species (O 3, NO II, HCHO, H IIO, SO II, aerosols (optical depth, type and absorption index), CO and CH4) with sensitivity down to the Earth's surface, thus addressing science issues on air quality and climate. It includes 3 UV-VIS channels continuously covering the 270-490 nm range, a NIR-channel covering the 710-775 nm range, and a SWIR-channel covering the 2305-2385 nm range. This instrument concept is, named TROPOMI, part of the TRAQ-mission proposal to ESA in response to the Call for Earth Explorer Ideas 2005, and, named TROPI, part of the CAMEO-proposal prepared for the US NRC decadal study-call on Earth science and applications from space. The SWIR-channel is optional in the TROPOMI/TRAQ instrument and included as baseline in the TROPI/CAMEO instrument. This paper focuses on derivation of the instrument requirements of the SWIR-channel by presenting the results of retrieval studies. Synthetic detector spectra are generated by the combination of a forward model and an instrument simulator that includes the properties of state-of-the-art detector technology. The synthetic spectra are input to the CO and CH 4 IMLM retrieval algorithm originally developed for SCIAMACHY. The required accuracy of the Level-2 SWIR data products defines the main instrument parameters like spectral resolution and sampling, telescope aperture, detector temperature, and optical bench temperature. The impact of selected calibration and retrieval errors on the Level-2 products has been characterized. The current status of the SWIR-channel optical design with its demanding requirements on ground-pixel size, spectral resolution, and signal-to-noise ratio will be presented.

  1. Carbon dynamics and CO2 and CH4 outgassing in the Mekong delta

    Borges, Alberto V.; Abril, Gwenaël; Bouillon, Steven

    2018-02-01

    We report a data set of biogeochemical variables related to carbon cycling obtained in the three branches (Mỹ Tho, Hàm Luông, Cố Chiên) of the Mekong delta (Bến Tre province, Vietnam) in December 2003, April 2004, and October 2004. Both the inner estuary (upstream of the mouth) and the outer estuary (river plume) were sampled, as well as side channels. The values of the partial pressure of CO2 (pCO2) ranged between 232 and 4085 ppm, O2 saturation level (%O2) between 63 and 114 %, and CH4 between 2 and 2217 nmol L-1, within the ranges of values previously reported in temperate and tropical meso- and macro-tidal estuaries. Strong seasonal variations were observed. In the upper oligohaline estuary, low pCO2 (479-753 ppm) and high %O2 (98-106 %) values were observed in April 2004 most probably related to freshwater phytoplankton growth owing to low freshwater discharge (1400 m3 s-1) and increase in water residence time; during the two other sampling periods with a higher freshwater discharge (9300-17 900 m3 s-1), higher pCO2 (1895-2664 ppm) and lower %O2 (69-84 %) values were observed in the oligohaline part of the estuary. In October 2004, important phytoplankton growth occurred in the offshore part of the river plume as attested by changes in the contribution of particulate organic carbon (POC) to total suspended matter (TSM) (%POC) and the stable isotope composition of POC (δ13C-POC), possibly related to low TSM values (improvement of light conditions for phytoplankton development), leading to low pCO2 (232 ppm) and high %O2 (114 %) values. Water in the side channels in the Mekong delta was strongly impacted by inputs from the extensive shrimp farming ponds. The values of pCO2, CH4, %O2, and the stable isotope composition of dissolved inorganic carbon (δ13C-DIC) indicated intense organic matter degradation that was partly mediated by sulfate reduction in sediments, as revealed by the slope of total alkalinity (TA) and DIC covariations. The δ13C

  2. One year of continuous measurements of soil CH4 and CO2 fluxes in a Japanese cypress forest: Temporal and spatial variations associated with Asian monsoon rainfall

    Sakabe, Ayaka; Kosugi, Yoshiko; Takahashi, Kenshi; Itoh, Masayuki; Kanazawa, Akito; Makita, Naoki; Ataka, Mioko

    2015-01-01

    We examined the effects of Asian monsoon rainfall on CH[4] absorption of water-unsaturated forest soil. We conducted a 1 year continuous measurement of soil CH[4] and CO[2] fluxes with automated chamber systems in three plots with different soil characteristics and water content to investigate how temporal variations in CH[4] fluxes vary with the soil environment. CH[4] absorption was reduced by the “Baiu” summer rainfall event and peaked during the subsequent hot, dry period. Although CH[4] ...

  3. The cost of pipelining climate change mitigation: An overview of the economics of CH4, CO2 and H2 transportation

    Zwaan, B.C.C. van der; Schoots, K.; Rivera-Tinoco, R.; Verbong, G.P.J.

    2011-01-01

    limited learning-by-doing and explain why negligible construction cost reductions for future CH 4 , CO 2 and H 2 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.

  4. Greenhouse gas (CO2 and CH4) emissions from a high altitude hydroelectric reservoir in the tropics (Riogrande II, Colombia)

    Guérin, Frédéric; Leon, Juan

    2015-04-01

    Tropical hydroelectric reservoirs are considered as very significant source of methane (CH4) and carbon dioxide (CO2), especially when flooding dense forest. We report emissions from the Rio Grande II Reservoir located at 2000 m.a.s.l. in the Colombian Andes. The dam was built at the confluence of the Rio Grande and Rio Chico in 1990. The reservoir has a surface of 12 km2, a maximum depth of 40m and a residence time of 2.5 month. Water quality (temperature, oxygen, pH, conductivity), nitrate, ammonium, dissolved and particulate organic carbon (DOC and POC), CO2 and CH4 were monitored bi-monthly during 1.5 year at 9 stations in the reservoir. Diffusive fluxes of CO2 and CH4 and CH4 ebullition were measured at 5 stations. The Rio grande II Reservoir is weakly stratified thermally with surface temperature ranging from 20 to 24°C and a constant bottom temperature of 18°C. The reservoir water column is well oxygenated at the surface and usually anoxic below 10m depth. At the stations close to the tributaries water inputs, the water column is well mixed and oxygenated from the surface to the bottom. As reported for other reservoirs located in "clear water" watersheds, the concentrations of nutrients are low (NO3-10 mmol m-2 d-1) were observed during the dry season. Close to the tributaries water inputs where the water column is well mixed, the average diffusive flux is 8 mmol m-2 d-1. CH4 ebullition was 3.5 mmol m-2 d-1 and no ebullition was observed for a water depth higher than 5m. The zone under the influence of the water inputs from tributaries represents 25% of the surface of the reservoir but contributed half of total CH4 emissions from the reservoir (29MgC month-1). Ebullition contributed only to 12% of total CH4 emissions over a year but it contributed up to 60% during the dry season. CH4 emissions from the Rio Grande Reservoir contributed 30% of the total GHG emissions (38GgCO2eq y-1). Overall, this study show that the majority of CH4 emissions from this

  5. Adsorption of Dissolved Gases (CH4, CO2, H2, Noble Gases) by Water-Saturated Smectite Clay Minerals

    Bourg, I. C.; Gadikota, G.; Dazas, B.

    2016-12-01

    Adsorption of dissolved gases by water-saturated clay minerals plays important roles in a range of fields. For example, gas adsorption in on clay minerals may significantly impact the formation of CH4 hydrates in fine-grained sediments, the behavior of CH4 in shale, CO2 leakage across caprocks of geologic CO2 sequestration sites, H2 leakage across engineered clay barriers of high-level radioactive waste repositories, and noble gas geochemistry reconstructions of hydrocarbon migration in the subsurface. Despite its importance, the adsorption of gases on clay minerals remains poorly understood. For example, some studies have suggested that clay surfaces promote the formation of CH4 hydrates, whereas others indicate that clay surfaces inhibit the formation of CH4 hydrates. Here, we present molecular dynamics (MD) simulations of the adsorption of a range of gases (CH4, CO2, H2, noble gases) on clay mineral surfaces. Our results indicate that the affinity of dissolved gases for clay mineral surfaces has a non-monotone dependence on the hydrated radius of the gas molecules. This non-monotone dependence arises from a combination of two effects: the polar nature of certain gas molecules (in particular, CO2) and the templating of interfacial water structure by the clay basal surface, which results in the presence of interfacial water "cages" of optimal size for intermediate-size gas molecules (such as Ne or Ar).

  6. A simple calculation algorithm to separate high-resolution CH4 flux measurements into ebullition and diffusion-derived components

    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.

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

    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

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

    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. Low-Cost Miniaturized Laser Heterodyne Radiometer for Highly Sensitive Detection of CO2 and CH4 in the Atmospheric Column

    Wilson, Emily L.; McLinden, Matthew L.; Miller, J. Houston

    2011-01-01

    We present a new passive ground-network instrument capable of measuring carbon dioxide (CO2) at 1.57 microns and methane (CH4) at 1.62 microns -- key for validation of OCO-2, ASCENDS, OCO-3, and GOSAT. Designed to piggy-back on an AERONET sun tracker (AERONET is a global network of more than 450 aerosol sensing instruments), this instrument could be rapidly deployed into the established AERONET network of ground sensors. Because aerosols induce a radiative effect that influences terrestrial carbon exchange, this simultaneous measure of aerosols and carbon cycle gases offers a uniquely comprehensive approach. This instrument is a variation of a laser heterodyne radiometer (LHR) that leverages recent advances in telecommunications lasers to miniaturize the instrument (the current version fits in a carry-on suitcase). In this technique, sunlight that has undergone absorption by the trace gas is mixed with laser light at a frequency matched to a trace gas absorption feature in the infrared (IR). Mixing results in a beat signal in the RF (radio frequency) region that can be related to the atmospheric concentration. By dividing this RF signal into a filter bank, concentrations at different altitudes can be resolved. For a one second integration, we estimate column sensitivities of 0.1 ppmv for CO2, and <1 ppbv for CH4.

  10. Active standoff detection of CH4 and N2O leaks using hard-target backscattered light using an open-path quantum cascade laser sensor

    Diaz, Adrian; Thomas, Benjamin; Castillo, Paulo; Gross, Barry; Moshary, Fred

    2016-05-01

    Fugitive gas emissions from agricultural or industrial plants and gas pipelines are an important environmental concern as they contribute to the global increase of greenhouse gas concentrations. Moreover, they are also a security and safety concern because of possible risk of fire/explosion or toxicity. This study presents standoff detection of CH4 and N2O leaks using a quantum cascade laser open-path system that retrieves path-averaged concentrations by collecting the backscattered light from a remote hard target. It is a true standoff system and differs from other open-path systems that are deployed as point samplers or long-path transmission systems that use retroreflectors. The measured absorption spectra are obtained using a thermal intra-pulse frequency chirped DFB quantum cascade laser at ~7.7 µm wavelength range with ~200 ns pulse width. Making fast time resolved observations, the system simultaneously realizes high spectral resolution and range to the target, resulting in path-averaged concentration retrieval. The system performs measurements at high speed ~15 Hz and sufficient range (up to 45 m, ~148 feet) achieving an uncertainty of 3.1 % and normalized sensitivity of 3.3 ppm m Hz-1/2 for N2O and 9.3 % and normalized sensitivity of 30 ppm m Hz-1/2 for CH4 with a 0.31 mW average power QCL. Given these characteristics, this system is promising for mobile or multidirectional search and remote detection of gas leaks.

  11. Study of the daily and seasonal atmospheric CH4 mixing ratio variability in a rural Spanish region using 222Rn tracer

    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.

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

    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

  13. Potential for negative emissions of greenhouse gases (CO2, CH4 and N2O) through coastal peatland re-establishment: Novel insights from high frequency flux data at meter and kilometer scales

    Windham-Myers, Lisamarie; Bergamaschi, Brian; Anderson, Frank; Knox, Sara; Miller, Robin; Fujii, Roger

    2018-04-01

    High productivity temperate wetlands that accrete peat via belowground biomass (peatlands) may be managed for climate mitigation benefits due to their global distribution and notably negative emissions of atmospheric carbon dioxide (CO2) through rapid storage of carbon (C) in anoxic soils. Net emissions of additional greenhouse gases (GHG)—methane (CH4) and nitrous oxide (N2O)—are more difficult to predict and monitor due to fine-scale temporal and spatial variability, but can potentially reverse the climate mitigation benefits resulting from CO2 uptake. To support management decisions and modeling, we collected continuous 96 hour high frequency GHG flux data for CO2, CH4 and N2O at multiple scales—static chambers (1 Hz) and eddy covariance (10 Hz)—during peak productivity in a well-studied, impounded coastal peatland in California’s Sacramento Delta with high annual rates of C fluxes, sequestering 2065 ± 150 g CO2 m‑2 y‑1 and emitting 64.5 ± 2.4 g CH4 m‑2 y‑1. Chambers (n = 6) showed strong spatial variability along a hydrologic gradient from inlet to interior plots. Daily (24 hour) net CO2 uptake (NEE) was highest near inlet locations and fell dramatically along the flowpath (‑25 to ‑3.8 to +2.64 g CO2 m‑2 d‑1). In contrast, daily net CH4 flux increased along the flowpath (0.39 to 0.62 to 0.88 g CH4 m‑2 d‑1), such that sites of high daily CO2 uptake were sites of low CH4 emission. Distributed, continuous chamber data exposed five novel insights, and at least two important datagaps for wetland GHG management, including: (1) increasing dominance of CH4 ebullition fluxes (15%–32% of total) along the flowpath and (2) net negative N2O flux across all sites as measured during a 4 day period of peak biomass (‑1.7 mg N2O m‑2 d‑1 0.51 g CO2 eq m‑2 d‑1). The net negative emissions of re-established peat-accreting wetlands are notably high, but may be poorly estimated by

  14. Carbonate control of H2 and CH4 production in serpentinization systems at elevated P-Ts

    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.

  15. Thermal effects of an ICL-based mid-infrared CH4 sensor within a wide atmospheric temperature range

    Ye, Weilin; Zheng, Chuantao; Sanchez, Nancy P.; Girija, Aswathy V.; He, Qixin; Zheng, Huadan; Griffin, Robert J.; Tittel, Frank K.

    2018-03-01

    The thermal effects of an interband cascade laser (ICL) based mid-infrared methane (CH4) sensor that uses long-path absorption spectroscopy were studied. The sensor performance in the laboratory at a constant temperature of ∼25 °C was measured for 5 h and its Allan deviation was ∼2 ppbv with a 1 s averaging time. A LabVIEW-based simulation program was developed to study thermal effects on infrared absorption and a temperature compensation technique was developed to minimize these effects. An environmental test chamber was employed to investigate the thermal effects that occur in the sensor system with variation of the test chamber temperature between 10 and 30 °C. The thermal response of the sensor in a laboratory setting was observed using a 2.1 ppm CH4 standard gas sample. Indoor/outdoor CH4 measurements were conducted to evaluate the sensor performance within a wide atmospheric temperature range.

  16. Site specific comparison of H2, CH4 and compressed air energy storage in porous formations

    Tilmann Pfeiffer, Wolf; Wang, Bo; Bauer, Sebastian

    2016-04-01

    The supply of energy from renewable sources like wind or solar power is subject to fluctuations determined by the climatic and weather conditions, and shortage periods can be expected on the order of days to weeks. Energy storage is thus required if renewable energy dominates the total energy production and has to compensate the shortages. Porous formations in the subsurface could provide large storage capacities for various energy carriers, such as hydrogen (H2), synthetic methane (CH4) or compressed air (CAES). All three energy storage options have similar requirements regarding the storage site characteristics and consequently compete for suitable subsurface structures. The aim of this work is to compare the individual storage methods for an individual storage site regarding the storage capacity as well as the achievable delivery rates. This objective is pursued using numerical simulation of the individual storage operations. In a first step, a synthetic anticline with a radius of 4 km, a drop of 900 m and a formation thickness of 20 m is used to compare the individual storage methods. The storage operations are carried out using -depending on the energy carrier- 5 to 13 wells placed in the top of the structure. A homogeneous parameter distribution is assumed with permeability, porosity and residual water saturation being 500 mD, 0.35 and 0.2, respectively. N2 is used as a cushion gas in the H2 storage simulations. In case of compressed air energy storage, a high discharge rate of 400 kg/s equating to 28.8 mio. m³/d at surface conditions is required to produce 320 MW of power. Using 13 wells the storage is capable of supplying the specified gas flow rate for a period of 31 hours. Two cases using 5 and 9 wells were simulated for both the H2 and the CH4 storage operation. The target withdrawal rates of 1 mio. sm³/d are maintained for the whole extraction period of one week in all simulations. However, the power output differs with the 5 well scenario producing

  17. Phosphorus addition mitigates N2O and CH4 emissions in N-saturated subtropical forest, SW China

    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.

  18. Prediction CH4 Emissions from the Wetlands in the Sanjiang Plain of Northeastern China in the 21st Century.

    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. Determination of Model Kinetics for Forced Unsteady State Operation of Catalytic CH4 Oxidation

    Effendy Mohammad

    2016-01-01

    Full Text Available The catalytic oxidation of methane for abating the emission vented from coal mine or natural gas transportation has been known as most reliable method. A reverse flow reactor operation has been widely used to oxidize this methane emission due to its capability for autothermal operation and heat production. The design of the reverse flow reactor requires a proper kinetic rate expression, which should be developed based on the operating condition. The kinetic rate obtained in the steady state condition cannot be applied for designing the reactor operated under unsteady state condition. Therefore, new approach to develop the dynamic kinetic rate expression becomes indispensable, particularly for periodic operation such as reverse flow reactor. This paper presents a novel method to develop the kinetic rate expression applied for unsteady state operation. The model reaction of the catalytic methane oxidation over Pt/-Al2O3 catalyst was used with kinetic parameter determined from laboratory experiments. The reactor used was a fixed bed, once-through operation, with a composition modulation in the feed gas. The switching time was set at 3 min by varying the feed concentration, feed flow rate, and reaction temperature. The concentrations of methane in the feed and product were measured and analysed using gas chromatography. The steady state condition for obtaining the kinetic rate expression was taken as a base case and as a way to judge its appropriateness to be applied for dynamic system. A Langmuir-Hinshelwood reaction rate model was developed. The time period during one cycle was divided into some segments, depending on the ratio of CH4/O2. The experimental result shows that there were kinetic regimes occur during one cycle: kinetic regime controlled by intrinsic surface reaction and kinetic regime controlled by external diffusion. The kinetic rate obtained in the steady state operation was not appropriate when applied for unsteady state operation

  20. Inter-annual variability and trend detection of urban CO2, CH4 and CO emissions

    Lauvaux, T.; Deng, A.; Gurney, K. R.; Nathan, B.; Ye, X.; Oda, T.; Karion, A.; Hardesty, M.; Harvey, R. M.; Richardson, S.; Whetstone, J. R.; Hutyra, L.; Davis, K. J.; Brewer, A.; Gaudet, B. J.; Turnbull, J. C.; Sweeney, C.; Shepson, P. B.; Miles, N.; Bonin, T.; Wu, K.; Balashov, N. V.

    2017-12-01

    The Indianapolis Flux (INFLUX) Experiment has conducted an unprecedented volume of atmospheric greenhouse gas measurements across the Indianapolis metropolitan area from aircraft, remote-sensing, and tower-based observational platforms. Assimilated in a high-resolution urban inversion system, atmospheric data provide an independent constraint to existing emission products, directly supporting the integration of economic data into urban emission systems. We present here the first multi-year assessment of carbon dioxide (CO2), methane (CH4), and carbon monoxide (CO) emissions from anthropogenic activities in comparison to multiple bottom-up emission products. Biogenic CO2 fluxes are quantified using an optimized biogeochemical model at high resolution, further refined within the atmospheric inversion system. We also present the first sector-based inversion by jointly assimilating CO2 and CO mixing ratios to quantify the dominant sectors of emissions over the entire period (2012-2015). The detected trend in CO2 emissions over 2012-2015 from both bottom-up emission products and tower-based inversions agree within a few percent, with a decline in city emissions over the 3-year time period. Major changes occur at the primary power plant, suggesting a decrease in energy production within the city limits. The joint assimilation of CO2 and CO mixing ratios confirms the absence of trends in other sectors. However, top-down and bottom-up approaches tend to disagree annually, with a decline in urban emissions suggested by atmospheric data in 2014 that is several months earlier than is observed in the bottom-up products. Concerning CH4 emissions, the inversion shows a decrease since mid-2014 which may be due to lower landfill emissions or lower energy consumption (from coal and natural gas). This first demonstration of a high-accuracy long-term greenhouse gas measurement network merged with a high-resolution bottom-up information system highlights the potential for informing

  1. Corona discharge experiments in admixtures of N2 and CH4: a laboratory simulation of Titan's atmosphere

    Horvath, G.; Skalny, J. D.; Mason, N. J.; Klas, M.; Zahoran, M.; Vladoiu, R.; Manole, M.

    2009-01-01

    A positive corona discharge fed by a N2:CH4 mixture (98:2) at atmospheric pressure and ambient temperature has been studied as a laboratory mimic of the chemical processes occurring in the atmosphere of Titan, Saturn's largest moon. In-situ measurements of UV and IR transmission spectra within the discharge have shown that the main chemical product is C2H2, produced by dissociation of CH4, with small but significant traces of ethane and HCN, all species that have been detected in Titan's atmo...

  2. Gully hotspot contribution to landscape methane (CH4) and carbon dioxide (CO2) fluxes in a northern peatland

    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

  3. Vacuum ultraviolet photochemistry of CH4 and isotopomers. II. Product channel fields and absorption spectra

    Wang, Jen-Han; Liu, Kopin; Min, Zhiyuan; Su, Hongmei; Bersohn, Richard; Preses, Jack; Larese, John Z.

    2000-01-01

    In part I of this work the relative velocities and anisotropies of the atomic H and D fragments from methane photolysis at 10.2 eV were measured. In this paper the relative abundance of the methyl and methylene fragments are reported. A complete set of quantum yields for the different photodissociation channels of each isotopomer is obtained by combining the two sets of data. Previously it was found that H atoms are almost four times more likely than D atoms to be ejected; now it is found that hydrogen molecule photofragments are much richer in H atoms than in D. Overall, the heavier D atoms are more likely than the H atoms to remain attached to the carbon atom. An implication for astrophysics is discussed. The VUV absorption spectra of CH 4 and CH 3 D are almost identical both at room temperature and 75 K. There is, as expected, no variation in the absorption spectrum with temperature. Evidence is given that all or almost all of the methylene is produced in the a 1 A 1 and not in the ground 3 B 1 state. (c) 2000 American Institute of Physics

  4. Homogeneity of Continuum Model of an Unsteady State Fixed Bed Reactor for Lean CH4 Oxidation

    Subagjo

    2014-07-01

    Full Text Available In this study, the homogeneity of the continuum model of a fixed bed reactor operated in steady state and unsteady state systems for lean CH4 oxidation is investigated. The steady-state fixed bed reactor system was operated under once-through direction, while the unsteady-state fixed bed reactor system was operated under flow reversal. The governing equations consisting of mass and energy balances were solved using the FlexPDE software package, version 6. The model selection is indispensable for an effective calculation since the simulation of a reverse flow reactor is time-consuming. The homogeneous and heterogeneous models for steady state operation gave similar conversions and temperature profiles, with a deviation of 0.12 to 0.14%. For reverse flow operation, the deviations of the continuum models of thepseudo-homogeneous and heterogeneous models were in the range of 25-65%. It is suggested that pseudo-homogeneous models can be applied to steady state systems, whereas heterogeneous models have to be applied to unsteady state systems.

  5. A theoretical study of CH4 dissociation on pure and gold-alloyed Ni(111) surfaces

    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...

  6. CH4/air homogeneous autoignition: A comparison of two chemical kinetics mechanisms

    Tingas, Efstathios Al.

    2018-03-11

    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 (53/325 species/reactions with N-chemistry) and the AramcoMech mechanism from NUI Galway (113/710 species/reactions without N-chemistry; Combustion and Flame 162:315-330, 2015). Although the two mechanisms provide qualitatively similar results (regarding ignition delay and profiles of temperature, of mass fractions and of explosive time scale), the 113/710 mechanism was shown to reproduce the experimental data with higher accuracy than the 53/325 mechanism. The present analysis explores the origin of the improved accuracy provided by the more complex kinetics mechanism. It is shown that the reactions responsible for the generation of the explosive time scale differ significantly. This is reflected to differences in the length of the chemical and thermal runaways and in the set of the most influential species.

  7. Production of hydrogen through the carbonation-calcination reaction applied to CH4/CO2 mixtures

    Barelli, L.; Bidini, G.; Corradetti, A.; Desideri, U.

    2007-01-01

    The production of hydrogen combined with carbon capture represents a possible option for reducing CO 2 emissions in atmosphere and anthropogenic greenhouse effect. Nowadays the worldwide hydrogen production is based mainly on natural gas reforming, but the attention of the scientific community is focused also on other gas mixtures with significant methane content. In particular mixtures constituted mainly by methane and carbon dioxide are extensively used in energy conversion applications, as they include land-fill gas, digester gas and natural gas. The present paper addresses the development of an innovative system for hydrogen production and CO 2 capture starting from these mixtures. The plant is based on steam methane reforming, coupled with the carbonation and calcination reactions for CO 2 absorption and desorption, respectively. A thermodynamic approach is proposed to investigate the plant performance in relation to the CH 4 content in the feeding gas. The results suggest that, in order to optimize the hydrogen purity and the efficiency, two different methodologies can be adopted involving both the system layout and operating parameters. In particular such methodologies are suitable for a methane content, respectively, higher and lower than 65%

  8. CO2–CH4 permeation in high zeolite 4A loading mixed matrix membranes

    Adams, Ryan T.

    2011-02-01

    Mixed matrix membranes (MMMs) with low particle loadings have been shown to improve the properties of pure polymers for many gas separations. Comparatively few reports have been made for high particle loading (≥50vol.%) MMMs. In this work, CO2-CH4 feeds were used to study the potential of 50vol.% zeolite 4A-poly(vinyl acetate) (PVAc) MMMs for natural gas separations. A low CO2 partial pressure mixed feed probed MMM performance below the plasticization pressure of PVAc and a high CO2 partial pressure mixed feed probed MMM performance at industrially relevant conditions above the plasticization pressure.Under both mixed feed conditions at 35°C, substantial improvements in overall separation performance were observed. At low CO2 partial pressures, CO2 permeability roughly doubled with a nearly 50% increase in selectivity versus pure PVAc under the same conditions. For the high CO2 partial pressure feed, CO2 permeability remained effectively unchanged with a 63% increase in selectivity versus pure PVAc. Surprisingly, the performance of these PVAc based MMMs approached the properties of current " upper bound" polymers. Overall, this work shows that significantly improved performance MMMs can be made with traditional techniques from a low cost, low performance polymer without costly adhesion promoters. © 2010.

  9. CO2–CH4 permeation in high zeolite 4A loading mixed matrix membranes

    Adams, Ryan T.; Lee, Jong Suk; Bae, Tae-Hyun; Ward, Jason K.; Johnson, J.R.; Jones, Christopher W.; Nair, Sankar; Koros, William J.

    2011-01-01

    Mixed matrix membranes (MMMs) with low particle loadings have been shown to improve the properties of pure polymers for many gas separations. Comparatively few reports have been made for high particle loading (≥50vol.%) MMMs. In this work, CO2-CH4 feeds were used to study the potential of 50vol.% zeolite 4A-poly(vinyl acetate) (PVAc) MMMs for natural gas separations. A low CO2 partial pressure mixed feed probed MMM performance below the plasticization pressure of PVAc and a high CO2 partial pressure mixed feed probed MMM performance at industrially relevant conditions above the plasticization pressure.Under both mixed feed conditions at 35°C, substantial improvements in overall separation performance were observed. At low CO2 partial pressures, CO2 permeability roughly doubled with a nearly 50% increase in selectivity versus pure PVAc under the same conditions. For the high CO2 partial pressure feed, CO2 permeability remained effectively unchanged with a 63% increase in selectivity versus pure PVAc. Surprisingly, the performance of these PVAc based MMMs approached the properties of current " upper bound" polymers. Overall, this work shows that significantly improved performance MMMs can be made with traditional techniques from a low cost, low performance polymer without costly adhesion promoters. © 2010.

  10. Measurements of N2O and CH4 from the aerated composting of food waste

    He, Y.; Sun, T.; Inamori, Y.; Mizuochi, M.; Kong, H.; Iwami, N.

    2000-01-01

    Emissions of N 2 O and CH 4 from an aerated composting system were investigated using small-scale simulated reactors. The results show relatively high emissions of N 2 O at the beginning of composting, in proportion to the application amount of food waste. After 2 days, the N 2 O emission decreased to 0.53 ppmv on average, near to the background level in the atmosphere (0.45 ppmv). The addition of composted cattle manure increased N 2 O emissions not only at the beginning of composting, but also during the later period and resulted in two peak emission curves. Good correlation was observed between the N 2 O concentration at the air outlet and NO 2 - concentration in waste, suggesting a generation pathway for N 2 O from NO 2 - to N 2 O. Methane was only detected in treatments containing composted cattle manure. The high emission of methane illustrates the involvement of anoxic/anaerobic microorganisms with the addition of composted manure. The result suggests the existence of anoxic or anaerobic microsite inside the waste particles even though ventilation was employed during the composting process

  11. Intermolecular potential energy surface and thermophysical properties of the CH4-N2 system.

    Hellmann, Robert; Bich, Eckard; Vogel, Eckhard; Vesovic, Velisa

    2014-12-14

    A five-dimensional potential energy surface (PES) for the interaction of a rigid methane molecule with a rigid nitrogen molecule was determined from quantum-chemical ab initio calculations. The counterpoise-corrected supermolecular approach at the CCSD(T) level of theory was utilized to compute a total of 743 points on the PES. The interaction energies were calculated using basis sets of up to quadruple-zeta quality with bond functions and were extrapolated to the complete basis set limit. An analytical site-site potential function with nine sites for methane and five sites for nitrogen was fitted to the interaction energies. The PES was validated by calculating the cross second virial coefficient as well as the shear viscosity and binary diffusion coefficient in the dilute-gas limit for CH4-N2 mixtures. An improved PES was obtained by adjusting a single parameter of the analytical potential function in such a way that quantitative agreement with the most accurate experimental values of the cross second virial coefficient was achieved. The transport property values obtained with the adjusted PES are in good agreement with the best experimental data.

  12. Reactivity of chemisorbed oxygen atoms and their catalytic consequences during CH4-O2 catalysis on supported Pt clusters.

    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

  13. Use of selected ambulatory dental services in Taiwan before and after global budgeting: a longitudinal study to identify trends in hospital and clinic-based services

    Lin Chienhung

    2012-09-01

    Full Text Available Abstract Background The Taiwan government adopted National Health Insurance (NHI in 1995, providing universal health care to all citizens. It was financed by mandatory premium contributions made by employers, employees, and the government. Since then, the government has faced increasing challenges to control NHI expenditures. The aim of this study was to determine trends in the provision of dental services in Taiwan after the implementation of global budgeting in 1998 and to identify areas of possible concern. Methods This longitudinal before/after study was based on data from the National Health Insurance Research Database from 1996 to 2001. These data were subjected to logistic regression analysis. Linear regression analysis was used to examine changes in delivery of specific services after global budgeting implementation. Utilization of hospital and clinic services was compared. Results Reimbursement for dental services increased significantly while the number of visits per patient remained steady in both hospitals and clinics. In hospitals, visits for root canal procedures, ionomer restoration, tooth extraction and tooth scaling increased significantly. In dental clinics, visits for amalgam restoration decreased significantly while those for ionomer restoration, tooth extraction, and tooth scaling increased significantly. After the adoption of global budgeting, expenditures for dental services increased dramatically while the number of visits per patient did not, indicating a possible shift in patients to hospital facilities that received additional National Health Insurance funding. Conclusions The identified trends indicate increased utilization of dental services and uneven distribution of care and dentists. These trends may be compromising the quality of dental care delivered in Taiwan.

  14. 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

    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.

  15. Projected Impact of Climate Change on the Energy Budget of the Arctic Ocean by a Global Climate Model

    Miller, James R.; Russell, Gary L.; Hansen, James E. (Technical Monitor)

    2001-01-01

    The annual energy budget of the Arctic Ocean is characterized by a net heat loss at the air-sea interface that is balanced by oceanic heat transport into the Arctic. The energy loss at the air-sea interface is due to the combined effects of radiative, sensible, and latent heat fluxes. The inflow of heat by the ocean can be divided into two components: the transport of water masses of different temperatures between the Arctic and the Atlantic and Pacific Oceans and the export of sea ice, primarily through Fram Strait. Two 150-year simulations (1950-2099) of a global climate model are used to examine how this balance might change if atmospheric greenhouse gases (GHGs) increase. One is a control simulation for the present climate with constant 1950 atmospheric composition, and the other is a transient experiment with observed GHGs from 1950 to 1990 and 0.5% annual compounded increases of CO2 after 1990. For the present climate the model agrees well with observations of radiative fluxes at the top of the atmosphere, atmospheric advective energy transport into the Arctic, and surface air temperature. It also simulates the seasonal cycle and summer increase of cloud cover and the seasonal cycle of sea-ice cover. In addition, the changes in high-latitude surface air temperature and sea-ice cover in the GHG experiment are consistent with observed changes during the last 40 and 20 years, respectively. Relative to the control, the last 50-year period of the GHG experiment indicates that even though the net annual incident solar radiation at the surface decreases by 4.6 W(per square meters) (because of greater cloud cover and increased cloud optical depth), the absorbed solar radiation increases by 2.8 W(per square meters) (because of less sea ice). Increased cloud cover and warmer air also cause increased downward thermal radiation at the surface so that the net radiation into the ocean increases by 5.0 Wm-2. The annual increase in radiation into the ocean, however, is

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

    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.

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

    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.

  18. A permutationally invariant full-dimensional ab initio potential energy surface for the abstraction and exchange channels of the H + CH4 system

    Li, Jun; Chen, Jun; Zhao, Zhiqiang; Zhang, Dong H.; Xie, Daiqian; Guo, Hua

    2015-01-01

    We report a permutationally invariant global potential energy surface (PES) for the H + CH 4 system based on ∼63 000 data points calculated at a high ab initio level (UCCSD(T)-F12a/AVTZ) using the recently proposed permutation invariant polynomial-neural network method. The small fitting error (5.1 meV) indicates a faithful representation of the ab initio points over a large configuration space. The rate coefficients calculated on the PES using tunneling corrected transition-state theory and quasi-classical trajectory are found to agree well with the available experimental and previous quantum dynamical results. The calculated total reaction probabilities (J tot = 0) including the abstraction and exchange channels using the new potential by a reduced dimensional quantum dynamic method are essentially the same as those on the Xu-Chen-Zhang PES [Chin. J. Chem. Phys. 27, 373 (2014)

  19. Regional Variation of CH4 and N2 Production P