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Sample records for measure ch4 co2

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

    Science.gov (United States)

    Wang, J.-L.; Jacobson, G.; Rella, C. W.; Chang, C.-Y.; Liu, I.; Liu, W.-T.; Chew, C.; Ou-Yang, C.-F.; Liao, W.-C.; Chang, C.-C.

    2013-08-01

    In recent years, cavity ring-down spectrometry (CRDS) has been demonstrated to be a highly sensitive, stable and fast analytical technique for real-time in situ measurements of greenhouse gases. In this study, we propose the technique (which we call flask-CRDS) of analyzing whole air flask samples for CO2, CH4 and CO using a custom gas manifold designed to connect to a CRDS analyzer. Extremely stable measurements of these gases can be achieved over a large pressure range in the flask, from 175 to 760 Torr. The wide pressure range is conducive to flask sample measurement in three ways: (1) flask samples can be collected in low-pressure environments (e.g. high-altitude locations); (2) flask samples can be first analyzed for other trace gases with the remaining low-pressure sample for CRDS analysis of CO2, CH4 and CO; and (3) flask samples can be archived and re-analyzed for validation. The repeatability of this method (1σ of 0.07 ppm for CO2, 0.4 ppb for CH4, and 0.5 ppb for CO) was assessed by analyzing five canisters filled with the same air sample to a pressure of 200 Torr. An inter-comparison of the flask-CRDS data with in-situ CRDS measurements at a high-altitude mountain baseline station revealed excellent agreement, with differences of 0.10 ± 0.09 ppm (1σ) for CO2 and 0.9 ± 1.0 ppb for CH4. This study demonstrated that the flask-CRDS method was not only simple to build and operate but could also perform highly accurate and precise measurements of atmospheric CO2, CH4 and CO in flask samples.

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

    Science.gov (United States)

    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.

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

    Science.gov (United States)

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

    2013-04-01

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

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

    Science.gov (United States)

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

    2008-12-01

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

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

    Science.gov (United States)

    Qin, J.; Rosenbauer, R.J.; Duan, Zhenhao

    2008-01-01

    Reported are the experimental measurements on vapor-liquid equilibria in the H2O + CO2 + CH4 ternary system at temperatures from (324 to 375) K and pressures from (10 to 50) MPa. The results indicate that the CH4 solubility in the ternary mixture is about 10 % to 40 % more than that calculated by interpolation from the Henry's law constants of the binary system, H2O + CH4, and the solubility of CO2 is 6 % to 20 % more than what is calculated by the interpolation from the Henry's law constants of the binary mixture, H 2O + CO2. ?? 2008 American Chemical Society.

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

    Science.gov (United States)

    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.

  7. Remotely operable compact instruments for measuring atmospheric CO2 and CH4 column densities at surface monitoring sites

    Directory of Open Access Journals (Sweden)

    I. Morino

    2010-08-01

    Full Text Available Remotely operable compact instruments for measuring atmospheric CO2 and CH4 column densities were developed in two independent systems: one utilizing a grating-based desktop optical spectrum analyzer (OSA with a resolution enough to resolve rotational lines of CO2 and CH4 in the regions of 1565–1585 and 1674–1682 nm, respectively; the other is an application of an optical fiber Fabry-Perot interferometer (FFPI to obtain the CO2 column density. Direct sunlight was collimated via a small telescope installed on a portable sun tracker and then transmitted through an optical fiber into the OSA or the FFPI for optical analysis. The near infrared spectra of the OSA were retrieved by a least squares spectral fitting algorithm. The CO2 and CH4 column densities deduced were in excellent agreement with those measured by a Fourier transform spectrometer with high resolution. The rovibronic lines in the wavelength region of 1570–1575 nm were analyzed by the FFPI. The I0 and I values in the Beer-Lambert law equation to obtain CO2 column density were deduced by modulating temperature of the FFPI, which offered column CO2 with the statistical error less than 0.2% for six hours measurement.

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

    Science.gov (United States)

    Steenberg Larsen, Klaus; Riis Christiansen, Jesper

    2016-04-01

    switching automatically between transparent and darkened mode enabling for separation of light-sensitive and light-indifferent processes in chambers. In a pilot study we measured hourly fluxes of CO2, H2O and CH4 continuously for two weeks in Danish Calluna vulgaris (common heather) heathland (Larsen et al. 2011). We will present an analysis of the novel, high-frequency data of CH4 fluxes under light and dark conditions, assess the advantages and limitations of the experimental setup and recommend future improvements of the technology involved. References: Carter, M.S., Larsen, K.S., et al. 2012. Synthesizing greenhouse gas fluxes across nine European peatlands and shrublands: responses to climatic and environmental changes. Biogeosciences 3739-3755. Christiansen, J.R., Korhonen, J.F.J., et al. 2011. Assessing the effects of chamber placement, manual sampling and headspace mixing on CH4 fluxes in a laboratory experiment. Plant and Soil 343, 171-185. Christiansen, J.R., Outhwaite, J., et al. 2015. Comparison of CO2, CH4 and N2O soil-atmosphere exchange measured in static chambers with cavity ring-down spectroscopy and gas chromatography. Agricultural and Forest Meteorology 211-212, 48-57. Creelman, C., Nickerson, N., Risk, D., 2013. Quantifying Lateral Diffusion Error in Soil Carbon Dioxide Respiration Estimates using Numerical Modeling. Soil Science Society of America Journal 77, 699-708. Larsen, K.S., Andresen, L.C., et al. 2011. Reduced N cycling in response to elevated CO2, warming, and drought in a Danish heathland: Synthesizing results of the CLIMAITE project after two years of treatments. Global Change Biology 17, 1884-1899. Pihlatie, M.K., Christiansen, J.R., et al. 2013. Comparison of static chambers to measure CH4 emissions from soils. Agricultural and Forest Meteorology 171-172, 124-136.

  9. Performance of a geostationary mission, geoCARB, to measure CO2, CH4 and CO column-averaged concentrations

    Directory of Open Access Journals (Sweden)

    I. N. Polonsky

    2014-04-01

    Full Text Available GeoCARB is a proposed instrument to measure column averaged concentrations of CO2, CH4 and CO from geostationary orbit using reflected sunlight in near-infrared absorption bands of the gases. The scanning options, spectral channels and noise characteristics of geoCARB and two descope options are described. The accuracy of concentrations from geoCARB data is investigated using end-to-end retrievals; spectra at the top of the atmosphere in the geoCARB bands are simulated with realistic trace gas profiles, meteorology, aerosol, cloud and surface properties, and then the concentrations of CO2, CH4 and CO are estimated from the spectra after addition of noise characteristic of geoCARB. The sensitivity of the algorithm to aerosol, the prior distributions assumed for the gases and the meteorology are investigated. The contiguous spatial sampling and fine temporal resolution of geoCARB open the possibility of monitoring localised sources such as power plants. Simulations of emissions from a power plant with a Gaussian plume are conducted to assess the accuracy with which the emission strength may be recovered from geoCARB spectra. Scenarios for "clean" and "dirty" power plants are examined. It is found that a reliable estimate of the emission rate is possible, especially for power plants that have particulate filters, by averaging emission rates estimated from multiple snapshots of the CO2 field surrounding the plant. The result holds even in the presence of partial cloud cover.

  10. 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

    OpenAIRE

    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] ...

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

    NARCIS (Netherlands)

    Pandey, S.

    2015-01-01

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

  12. Evaluation of factors affecting accurate measurements of atmospheric CO2 and CH4 by wavelength-scanned cavity ring-down spectroscopy

    Science.gov (United States)

    Nara, H.; Tanimoto, H.; Tohjima, Y.; Mukai, H.; Nojiri, Y.; Katsumata, K.; Rella, C.

    2012-07-01

    We examined potential interferences from water vapor and atmospheric background gases (N2, O2, and Ar), and biases by isotopologues of target species, on accurate measurement of atmospheric CO2 and CH4 by means of wavelength-scanned cavity ring-down spectroscopy (WS-CRDS). Variations in the composition of the background gas substantially impacted the CO2 and CH4 measurements: the measured amounts of CO2 and CH4 decreased with increasing N2 mole fraction, but increased with increasing O2 and Ar, suggesting that the pressure-broadening effects (PBEs) increased as Ar < O2 < N2. Using these experimental results, we inferred PBEs for the measurement of synthetic standard gases. The PBEs were negligible (up to 0.05 ppm for CO2 and 0.01 ppb for CH4) for gas standards balanced with purified air, although the PBEs were substantial (up to 0.87 ppm for CO2 and 1.4 ppb for CH4) for standards balanced with synthetic air. For isotopic biases on CO2 measurements, we compared experimental results and theoretical calculations, which showed excellent agreement within their uncertainty. We derived empirical correction functions for water vapor for three WS-CRDS instruments (Picarro EnviroSense 3000i, G-1301, and G-2301). Although the transferability of the functions was not clear, no significant difference was found in the water vapor correction values among these instruments within the typical analytical precision at sufficiently low water concentrations (< 0.3%V for CO2 and < 0.4%V for CH4). For accurate measurements of CO2 and CH4 in ambient air, we concluded that WS-CRDS measurements should be performed under complete dehumidification of air samples, or moderate dehumidification followed by application of a water vapor correction function, along with calibration by natural air-based standard gases or purified air-balanced synthetic standard gases with isotopic correction.

  13. Simultaneous Measurements of Soil CO2 and CH4 Fluxes Using Laser Absorption Spectroscopy

    Directory of Open Access Journals (Sweden)

    Rachhpal S. Jassal

    2016-04-01

    Full Text Available We present a method of simultaneously measuring soil CO and CH fluxes using a laser-based cavity ring-down spectrometer (CRDS coupled to an automated non-steady-state chamber system. The differential equation describing the change in the greenhouse gas (GHG mixing ratio in the chamber headspace following lid closure is solved for the condition when a small flow rate of chamber headspace air is pulled through the CRDS by an external pump and exhausted to the atmosphere. The small flow rate allows calculation of fluxes assuming linear relationships between the GHG mixing ratios and chamber lid closure times of a few minutes. We also calibrated the chambers for effective volume ( and show that adsorption of the GHGs on the walls of the chamber caused to be 7% higher than the geometric volume, with the near-surface soil porosity causing another 4% increase in .

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

    Science.gov (United States)

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

    2010-10-01

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

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

    Science.gov (United States)

    Xu, L.; Chanton, J.; McDermitt, D. K.; Li, J.; Green, R. B.

    2015-12-01

    Methane plays a critical role in the radiation balance and chemistry of the atmosphere. Globally, landfill methane emission contributes about 10-19% of the anthropogenic methane burden into the atmosphere. In the United States, 18% of annual anthropogenic methane emissions come from landfills, which represent the third largest source of anthropogenic methane emissions, behind enteric fermentation and natural gas and oil production. One uncertainty in estimating landfill methane emissions is the fraction of methane oxidized when methane produced under anaerobic conditions passes through the cover soil. We developed a simple stoichiometric model to estimate methane oxidation fraction when the anaerobic CO2 / CH4 production ratio is known, or can be estimated. The model predicts a linear relationship between CO2 emission rates and CH4 emission rates, where the slope depends on anaerobic CO2 / CH4 production ratio and the fraction of methane oxidized, and the intercept depends on non-methane-dependent oxidation processes. The model was tested using carbon dioxide emission rates (fluxes) and methane emission rates (fluxes) measured using the eddy covariance method over a one year period at the Turkey Run landfill in Georgia, USA. The CO2 / CH4 production ratio was estimated by measuring CO2 and CH4 concentrations in air sampled under anaerobic conditions deep inside the landfill. We also used a mass balance approach to independently estimate fractional oxidation based on stable isotope measurements (δ13C of methane) of gas samples taken from deep inside the landfill and just above the landfill surface. Results from the two independent methods agree well. The model will be described and methane oxidation will be discussed in relation to wind direction, location at the landfill, and age of the deposited refuse.

  16. A single gas chromatograph for accurate atmospheric mixing ratio measurements of CO2, CH4, N2O, SF6 and CO

    NARCIS (Netherlands)

    van der Laan, S.; Neubert, R. E. M.; Meijer, H. A. J.; Simpson, W.R.

    2009-01-01

    We present an adapted gas chromatograph capable of measuring simultaneously and semi-continuously the atmospheric mixing ratios of the greenhouse gases CO2, CH4, N2O and SF6 and the trace gas CO with high precision and long-term stability. The novelty of our design is that all species are measured

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

    NARCIS (Netherlands)

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

    2015-01-01

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

  18. High-accuracy continuous airborne measurements of greenhouse gases (CO2 and CH4) using the cavity ring-down spectroscopy (CRDS) technique

    NARCIS (Netherlands)

    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.

    2010-01-01

    High-accuracy continuous measurements of greenhouse gases (CO2 and CH4) during the BARCA (Balancao Atmosferico Regional de Carbono na Amazonia) 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

  19. Feasibility study of using a 'travelling' CO2 and CH4 instrument to validate continuous in-situ measurement stations

    Energy Technology Data Exchange (ETDEWEB)

    Hammer, S.; Konrad, G.; Levin, I. [Institut fuer Umweltphysik IUP, Heidelberg University (Germany); Vermeulen, A.T. [Energy research Center of the Netherlands ECN, Petten (Netherlands); Laurent, O.; Delmotte, M.; Hazan, L. [Laboratoire des Sciences du Climat et de l' Environnement LSCE, Gif-sur-Yvette (France); Jordan, A. [Max Planck Institute for Biogeochemistry, Jena (Germany); Conil, S. [Agence Nationale pour la gestion des Dechets Radioactifs ANDRA, Bure (France)

    2012-09-24

    In the course of the ICOS (Integrated Carbon Observation System) Demo Experiment a feasibility study on the usefulness of a Travelling Comparison Instrument (TCI) was conducted in order to evaluate continuous atmospheric CO2 and CH4 measurements at two European stations. The aim of the TCI is to independently measure ambient air in parallel to the standard station instrumentation, thus providing a comprehensive comparison that includes the sample intake system, the instrument itself as well as its calibration and data evaluation. Observed differences between the TCI and the Heidelberg gas chromatographic system, which acted as a reference for the TCI, were -0.02{+-}0.08{mu}mol mol{sup -1} for CO2 and -0.3{+-}2.3{mu}mol mol{sup -1} for CH4. Over a period of two weeks each, the continuous CO2 and CH4 measurements at two ICOS field stations, Cabauw and OPE, were compared to co-located TCI measurements. At Cabauw mean differences of 0.21{+-}0.06{mu}mol mol{sup -1} for CO2 and 0.41{+-}0.50{mu}mol mol{sup -1} for CH4 were found. For OPE the mean differences were 0.13{+-}0.07{mu}mol mol{sup -1} for CO2 and 0.44{+-}0.36{mu}mol mol{sup -1} for CH4. Potential causes of these observed differences are leakages or contaminations in the intake lines and/or there flushing pumps. At Cabauw station an additional error contribution originates from insufficient flushing of standard gases. Offsets arising from differences in the working standard calibrations or leakages/ contaminations in the drying systems are too small to explain the observed differences. Finally a comprehensive quality management strategy for atmospheric monitoring networks is proposed.

  20. SOIL 222Rn CONCENTRATION, CO2 AND CH4 FLUX MEASUREMENTS AROUND THE JWALAMUKHI AREA OF NORTH-WEST HIMALAYAS, INDIA.

    Science.gov (United States)

    Kumar, Arvind; Walia, Vivek; Yang, Tsanyao Frank; Fu, Ching-Chou; Singh, Surinder; Bajwa, Bikramjit Singh; Arora, Vishal

    2016-10-01

    Soil 222 Rn concentration, CO 2 and CH 4 flux measurements were conducted around the Jwalamukhi area of North-West Himalayas, India. During this study, around 37 soil gas points and flux measurements were taken with the aim to assure the suitability of this method in the study of fault zones. For this purpose, RAD 7 (Durridge, USA) was used to monitor radon concentrations, whereas portable diffuse flux meter (West Systems, Italy) was used for the CO 2 and CH 4 flux measurements. The recorded radon concentration varies from 6.1 to 34.5 kBq m -3 with an average value of 16.5 kBq m -3 The anomalous value of radon concentrations was recorded between Jwalamukhi thrust and Barsar thrust. The recorded average of CO 2 and CH 4 flux were 11.8 and 2.7 g m -2 day -1 , respectively. The good correlation between anomalous CO 2 flux and radon concentrations has been observed along the fault zone in the study area, suggesting that radon migration is dependent on CO 2 . © The Author 2016. Published by Oxford University Press. All rights reserved. For Permissions, please email: journals.permissions@oup.com.

  1. A 4 U laser heterodyne radiometer for methane (CH4) and carbon dioxide (CO2) measurements from an occultation-viewing CubeSat

    Science.gov (United States)

    Wilson, Emily L.; DiGregorio, A. J.; Riot, Vincent J.; Ammons, Mark S.; Bruner, William W.; Carter, Darrell; Mao, Jianping; Ramanathan, Anand; Strahan, Susan E.; Oman, Luke D.; Hoffman, Christine; Garner, Richard M.

    2017-03-01

    We present a design for a 4 U (20 cm  ×  20 cm  ×  10 cm) occultation-viewing laser heterodyne radiometer (LHR) that measures methane (CH4), carbon dioxide (CO2) and water vapor (H2O) in the limb that is designed for deployment on a 6 U CubeSat. The LHR design collects sunlight that has undergone absorption by the trace gas and mixes it with a distributive feedback (DFB) laser centered at 1640 nm that scans across CO2, CH4, and H2O absorption features. Upper troposphere/lower stratosphere measurements of these gases provide key inputs to stratospheric circulation models: measuring stratospheric circulation and its variability is essential for projecting how climate change will affect stratospheric ozone.

  2. A 4 U Laser Heterodyne Radiometer for Methane (CH4) and Carbon Dioxide (CO2) Measurements from an Occultation-Viewing CubSat

    Science.gov (United States)

    Wilson, Emily L.; DiGregorio, A. J.; Riot, Vincent J.; Ammons, Mark S.; Bruner, WIlliam W.; Carter, Darrell; Mao, Jianping; Ramanathan, Anand; Strahan, Susan E.; Oman, Luke D.; hide

    2017-01-01

    We present a design for a 4 U (20 cm 20 cm 10 cm) occultation-viewing laser heterodyne radiometer (LHR) that measures methane (CH4), carbon dioxide (CO2) and water vapor(H2O) in the limb that is designed for deployment on a 6 U CubeSat. The LHR design collects sunlight that has undergone absorption by the trace gas and mixes it with a distributive feedback (DFB) laser centered at 1640 nm that scans across CO2, CH4, and H2O absorption features. Upper troposphere lower stratosphere measurements of these gases provide key inputs to stratospheric circulation models: measuring stratospheric circulation and its variability is essential for projecting how climate change will affect stratospheric ozone.

  3. A 4 U laser heterodyne radiometer for methane (CH4) and carbon dioxide (CO2) measurements from an occultation-viewing CubeSat

    International Nuclear Information System (INIS)

    Wilson, Emily L; Oman, Luke D; DiGregorio, A J; Garner, Richard M; Riot, Vincent J; Ammons, Mark S; Bruner, William W; Carter, Darrell; Mao, Jianping; Ramanathan, Anand; Strahan, Susan E; Hoffman, Christine

    2017-01-01

    We present a design for a 4 U (20 cm  ×  20 cm  ×  10 cm) occultation-viewing laser heterodyne radiometer (LHR) that measures methane (CH 4 ), carbon dioxide (CO 2 ) and water vapor (H 2 O) in the limb that is designed for deployment on a 6 U CubeSat. The LHR design collects sunlight that has undergone absorption by the trace gas and mixes it with a distributive feedback (DFB) laser centered at 1640 nm that scans across CO 2 , CH 4 , and H 2 O absorption features. Upper troposphere/lower stratosphere measurements of these gases provide key inputs to stratospheric circulation models: measuring stratospheric circulation and its variability is essential for projecting how climate change will affect stratospheric ozone. (paper)

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

    International Nuclear Information System (INIS)

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

    2014-01-01

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

  5. High-accuracy continuous airborne measurements of greenhouse gases (CO2 and CH4 using the cavity ring-down spectroscopy (CRDS technique

    Directory of Open Access Journals (Sweden)

    V. Y. Chow

    2010-03-01

    Full Text Available 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.

  6. High-accuracy continuous airborne measurements of greenhouse gases (CO2 and CH4) using the cavity ring-down spectroscopy (CRDS) technique

    Science.gov (United States)

    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.

    2010-03-01

    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.

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

    Science.gov (United States)

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

    2015-12-01

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

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

    OpenAIRE

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

    1994-01-01

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

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

    Directory of Open Access Journals (Sweden)

    Hangga Wicaksono

    2017-08-01

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

  10. A Low-Cost Miniaturized Laser Heterodyne Radiometer (Mini-LHR) for Near-ir Measurements of CO2 and CH4 in the Atmospheric Column

    Science.gov (United States)

    Steel, Emily Wilson

    2016-01-01

    The miniaturized laser heterodyne radiometer (mini-LHR) is a ground-based passive variation of a laser heterodyne radiometer that uses sunlight to measure absorption of CO2 andCH4 in the infrared. Sunlight is collected using collimation optics mounted to an AERONET sun tracker, modulated with a fiber switch and mixed with infrared laser light in a fast photoreciever.The amplitude of the resultant RF (radio frequency) beat signal correlates with the concentration of the gas in the atmospheric column.

  11. Automated online measurement of N2, N2O, NO, CO2, and CH4 emissions based on a gas-flow-soil-core technique.

    Science.gov (United States)

    Liao, Tingting; Wang, Rui; Zheng, Xunhua; Sun, Yang; Butterbach-Bahl, Klaus; Chen, Nuo

    2013-11-01

    The gas-flow-soil-core (GFSC) technique allows to directly measure emission rates of denitrification gases of incubated soil cores. However, the technique was still suffering some drawbacks such as inadequate accuracy due to asynchronous detection of dinitrogen (N2) and other gases and low measurement frequency. Furthermore, its application was limited due to intensive manual operation. To overcome these drawbacks, we updated the GFSC system as described by Wang et al. (2011) by (a) using both a chemiluminescent detector and a gas chromatograph detector to measure nitric oxide (NO), (b) synchronizing the measurements of N2, NO, nitrous oxide (N2O), carbon dioxide (CO2) and methane (CH4), and (c) fully automating the sampling/analysis of all the gases. These technical modifications significantly reduced labor demands by at least a factor of two, increased the measurement frequency from 3 to 6 times per day and resulted in remarkable improvements in measurement accuracy (with detection limits of 0.5, 0.01, 0.05, 2.3 and 0.2μgN or Ch(-1)kg(-1)ds, or 17, 0.3, 1.8, 82, and 6μgN or Cm(-2)h(-1), for N2, N2O, NO, CO2, and CH4, respectively). In some circumstances, the modified system measured significantly more N2 and CO2 and less N2O and NO because of the enhanced measurement frequency. The modified system distinguished the differences in emissions of the denitrification gases and CO2 due to a 20% change in initial carbon supplies. It also remarkably recovered approximately 90% of consumed nitrate during incubation. These performances validate the technical improvement, and indicate that the improved GFSC system may provide a powerful research tool for obtaining deeper insights into the processes of soil carbon and nitrogen transformation during denitrification. Copyright © 2013. Published by Elsevier Ltd.

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

    International Nuclear Information System (INIS)

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

    2005-01-01

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

  13. Developments in Miniaturized Laser Heterodyne Radiometer (mini-LHR) construction for groundtruth measurements of CH4 and CO2 in harsh terrain

    Science.gov (United States)

    DiGregorio, A.; Wilson, E. L.; Hoffman, C.; Grunberg, C.; Mao, J.; Ramanathan, A. K.

    2016-12-01

    We present an updated, ruggedized design of NASA Goddard Space Flight Center's Miniaturized Laser Heterodyne Radiometer (mini-LHR), and the results of testing in the Bonanza Creek Research Forest. The mini-LHR is a passive variation of typical heterodyne radiometry instruments, designed to work in tandem with the AERONET sun photometer for collection of column methane (CH4) and carbon dioxide (CO2) in harsh environments. Advancements in the development of the Cube-Sat version of the mini-LHR have allowed a more than 50% reduction in size, weight, and power usage of the mini-LHR. Now small enough to fit in a medium handbag, the mini-LHR can be run off of a small 35 Watt solar panel and backup battery for continuous measurement. Using a touch-screen control interface built off of a Raspberry Pi, the updated mini-LHR is capable of data collection and preliminary data processing, even without internet, cellular, or satellite connectivity. The improvements made to the mini-LHR were tested in a field campaign in May 2016 funded under NASA's IDS program to track CH4 and CO2 emissions above thawing permafrost. In addition to being a comprehensive study of methane release from thawing permafrost, this pilot study tested the ruggedization and functionality of the instrument in three different environments- a black spruce forest, collapsed scar bog, and fen.

  14. CO2/CH4 Separation via Polymeric Blend Membrane

    Directory of Open Access Journals (Sweden)

    H. Sanaeepur

    2013-01-01

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

  15. Effect of air composition (N2, O2, Ar, and H2O) on CO2 and CH4 measurement by wavelength-scanned cavity ring-down spectroscopy: calibration and measurement strategy

    Science.gov (United States)

    Nara, H.; Tanimoto, H.; Tohjima, Y.; Mukai, H.; Nojiri, Y.; Katsumata, K.; Rella, C. W.

    2012-11-01

    We examined potential interferences from water vapor and atmospheric background gases (N2, O2, and Ar), and biases by isotopologues of target species, on accurate measurement of atmospheric CO2 and CH4 by means of wavelength-scanned cavity ring-down spectroscopy (WS-CRDS). Changes of the background gas mole fractions in the sample air substantially impacted the CO2 and CH4 measurements: variation of CO2 and CH4 due to relative increase of each background gas increased as Ar < O2 < N2, suggesting similar relation for the pressure-broadening effects (PBEs) among the background gas. The pressure-broadening coefficients due to variations in O2 and Ar for CO2 and CH4 are empirically determined from these experimental results. Calculated PBEs using the pressure-broadening coefficients are linearly correlated with the differences between the mole fractions of O2 and Ar and their ambient abundances. Although the PBEs calculation showed that impact of natural variation of O2 is negligible on the CO2 and CH4 measurements, significant bias was inferred for the measurement of synthetic standard gases. For gas standards balanced with purified air, the PBEs were estimated to be marginal (up to 0.05 ppm for CO2 and 0.01 ppb for CH4) although the PBEs were substantial (up to 0.87 ppm for CO2 and 1.4 ppb for CH4) for standards balanced with synthetic air. For isotopic biases on CO2 measurements, we compared experimental results and theoretical calculations, which showed excellent agreement within their uncertainty. We derived instrument-specific water correction functions empirically for three WS-CRDS instruments (Picarro EnviroSense 3000i, G-1301, and G-2301), and evaluated the transferability of the water correction function from G-1301 among these instruments. Although the transferability was not proven, no significant difference was found in the water vapor correction function for the investigated WS-CRDS instruments as well as the instruments reported in the past studies

  16. A single gas chromatograph for accurate atmospheric mixing ratio measurements of CO2, CH4, N2O, SF6 and CO

    Directory of Open Access Journals (Sweden)

    H. A. J. Meijer

    2009-09-01

    Full Text Available We present an adapted gas chromatograph capable of measuring simultaneously and semi-continuously the atmospheric mixing ratios of the greenhouse gases CO2, CH4, N2O and SF6 and the trace gas CO with high precision and long-term stability. The novelty of our design is that all species are measured with only one device, making it a very cost-efficient system. No time lags are introduced between the measured mixing ratios. The system is designed to operate fully autonomously which makes it ideal for measurements at remote and unmanned stations. Only a small amount of sample air is needed, which makes this system also highly suitable for flask air measurements. In principle, only two reference cylinders are needed for daily operation and only one calibration per year against international WMO standards is sufficient to obtain high measurement precision and accuracy. The system described in this paper is in use since May 2006 at our atmospheric measurement site Lutjewad near Groningen, The Netherlands at 6°21´ E, 53°24´N, 1 m a.s.l. Results show the long-term stability of the system. Observed measurement precisions at our remote research station Lutjewad were: ±0.04 ppm for CO2, ±0.8 ppb for CH4, ±0.8 ppb for CO, ±0.3 ppb for N2O, and ±0.1 ppt for SF6. The ambient mixing ratios of all measured species as observed at station Lutjewad for the period of May 2007 to August 2008 are presented as well.

  17. Calibration and field testing of cavity ring-down laser spectrometers measuring CH4, CO2, and δ13CH4 deployed on towers in the Marcellus Shale region

    Directory of Open Access Journals (Sweden)

    N. L. Miles

    2018-03-01

    Full Text Available Four in situ cavity ring-down spectrometers (G2132-i, Picarro, Inc. measuring methane dry mole fraction (CH4, carbon dioxide dry mole fraction (CO2, and the isotopic ratio of methane (δ13CH4 were deployed at four towers in the Marcellus Shale natural gas extraction region of Pennsylvania. In this paper, we describe laboratory and field calibration of the analyzers for tower-based applications and characterize their performance in the field for the period January–December 2016. Prior to deployment, each analyzer was tested using bottles with various isotopic ratios, from biogenic to thermogenic source values, which were diluted to varying degrees in zero air, and an initial calibration was performed. Furthermore, at each tower location, three field tanks were employed, from ambient to high mole fractions, with various isotopic ratios. Two of these tanks were used to adjust the calibration of the analyzers on a daily basis. We also corrected for the cross-interference from ethane on the isotopic ratio of methane. Using an independent field tank for evaluation, the standard deviation of 4 h means of the isotopic ratio of methane difference from the known value was found to be 0.26 ‰ δ13CH4. Following improvements in the field tank testing scheme, the standard deviation of 4 h means was 0.11 ‰, well within the target compatibility of 0.2 ‰. Round-robin style testing using tanks with near-ambient isotopic ratios indicated mean errors of −0.14 to 0.03 ‰ for each of the analyzers. Flask to in situ comparisons showed mean differences over the year of 0.02 and 0.08 ‰, for the east and south towers, respectively. Regional sources in this region were difficult to differentiate from strong perturbations in the background. During the afternoon hours, the median differences of the isotopic ratio measured at three of the towers, compared to the background tower, were &minus0.15 to 0.12 ‰ with standard deviations of the 10

  18. Calibration and field testing of cavity ring-down laser spectrometers measuring CH4, CO2, and δ13CH4 deployed on towers in the Marcellus Shale region

    Science.gov (United States)

    Miles, Natasha L.; Martins, Douglas K.; Richardson, Scott J.; Rella, Christopher W.; Arata, Caleb; Lauvaux, Thomas; Davis, Kenneth J.; Barkley, Zachary R.; McKain, Kathryn; Sweeney, Colm

    2018-03-01

    Four in situ cavity ring-down spectrometers (G2132-i, Picarro, Inc.) measuring methane dry mole fraction (CH4), carbon dioxide dry mole fraction (CO2), and the isotopic ratio of methane (δ13CH4) were deployed at four towers in the Marcellus Shale natural gas extraction region of Pennsylvania. In this paper, we describe laboratory and field calibration of the analyzers for tower-based applications and characterize their performance in the field for the period January-December 2016. Prior to deployment, each analyzer was tested using bottles with various isotopic ratios, from biogenic to thermogenic source values, which were diluted to varying degrees in zero air, and an initial calibration was performed. Furthermore, at each tower location, three field tanks were employed, from ambient to high mole fractions, with various isotopic ratios. Two of these tanks were used to adjust the calibration of the analyzers on a daily basis. We also corrected for the cross-interference from ethane on the isotopic ratio of methane. Using an independent field tank for evaluation, the standard deviation of 4 h means of the isotopic ratio of methane difference from the known value was found to be 0.26 ‰ δ13CH4. Following improvements in the field tank testing scheme, the standard deviation of 4 h means was 0.11 ‰, well within the target compatibility of 0.2 ‰. Round-robin style testing using tanks with near-ambient isotopic ratios indicated mean errors of -0.14 to 0.03 ‰ for each of the analyzers. Flask to in situ comparisons showed mean differences over the year of 0.02 and 0.08 ‰, for the east and south towers, respectively. Regional sources in this region were difficult to differentiate from strong perturbations in the background. During the afternoon hours, the median differences of the isotopic ratio measured at three of the towers, compared to the background tower, were &minus0.15 to 0.12 ‰ with standard deviations of the 10 min isotopic ratio differences of 0.8

  19. First Continuous High Frequency in Situ Measurements of CO2 and CH4 in Rwanda Using Cavity Ring-down Spectroscopy

    Science.gov (United States)

    Gasore, J.; DeWitt, L. H.; Prinn, R. G.

    2015-12-01

    Recent IPCC reports emphasize the lack of ground measurements of greenhouse gases on the African continent, despite Africa's significant emissions from agriculture and biomass burning as well as ongoing land use changes. We have established a greenhouse gas monitoring station in northern Rwanda that will be part of the Advanced Global Atmospheric Gases Experiment (AGAGE), a global network of high frequency long-term remote atmospheric measurement stations. Using a Picarro G2401 cavity ring-down analyzer, continuous measurements of CO2, CH4, and CO at a frequency of five seconds are being captured at this equatorial East African site. The measurement site is located near the Virunga mountains, a volcanic range in North-West Rwanda, on the summit of Mt. Mugogo (2507 m above sea level). Mt. Mugogo is located in a rural area 70km away from Kigali, the capital of Rwanda, and about 13km from the nearest town. From HYSPLIT 7-day back-trajectory calculations, we have determined that the station measures air masses originating from East and Central Africa, the Indian Ocean and occasionally from Southern Asia. Depending on the wind direction and local boundary layer height, measurements taken at Mt Mugogo are occasionally influenced by local sources, including emissions from the nearby city and wood fires from small rural settlements around the station. Here we present the first greenhouse gas measurement data from this unique and understudied location in Africa. Using the lagrangian transport and dispersion model FLEXPART, we derive the relationship between the observed mole fractions of CO2 and CH4 and our current knowledge of their sources and sinks, across this large African footprint.

  20. Methanogenic Conversion of CO2 Into CH4

    Energy Technology Data Exchange (ETDEWEB)

    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.

  1. A mobile automatic gas chromatograph system to measure CO2, CH4 and N2O fluxes from soil in the field

    International Nuclear Information System (INIS)

    Silvola, J.; Martikainen, P.; Nykaenen, H.

    1992-01-01

    A caravan has been converted into mobile laboratory for measuring fluxes of CO 2 , CH 4 and N 2 O from the soil in the field. The caravan was equipped with a gas chromatograph fitted with TC-, FI- and EC-detectors, and a PC controlled data logger. The gas collecting chambers can be used up to 50 m from the caravan. The closing and opening of the chambers, as well as the flows of sample gases from chambers to the gas chromatograph. is pneumatically regulated. Simultaneous recordings of temperature, light intensity and the depth of water table are made. The system has been used for two months in 1992, and some preliminary results are presented

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

    Science.gov (United States)

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

    2000-01-01

    The BOREAS TGB-1 team made numerous measurements of trace gas concentrations and fluxes at various NSA sites. This data set contains methane (CH4) and carbon dioxide (CO2) concentrations in soil profiles from the NSA-OJP, NSA-OBS, NSA-YJP, and NSA-BP sites during the period of 23-May to 20-Sep-1994. The soil gas sampling profiles of CH 4 and CO 2 were completed to quantify controls on CO2 and CH4 fluxes in the boreal forest. The data are provided in tabular ASCII files.

  3. Effect of air composition (N2, O2, Ar, and H2O on CO2 and CH4 measurement by wavelength-scanned cavity ring-down spectroscopy: calibration and measurement strategy

    Directory of Open Access Journals (Sweden)

    K. Katsumata

    2012-11-01

    Full Text Available We examined potential interferences from water vapor and atmospheric background gases (N2, O2, and Ar, and biases by isotopologues of target species, on accurate measurement of atmospheric CO2 and CH4 by means of wavelength-scanned cavity ring-down spectroscopy (WS-CRDS. Changes of the background gas mole fractions in the sample air substantially impacted the CO2 and CH4 measurements: variation of CO2 and CH4 due to relative increase of each background gas increased as Ar 2 2, suggesting similar relation for the pressure-broadening effects (PBEs among the background gas. The pressure-broadening coefficients due to variations in O2 and Ar for CO2 and CH4 are empirically determined from these experimental results. Calculated PBEs using the pressure-broadening coefficients are linearly correlated with the differences between the mole fractions of O2 and Ar and their ambient abundances. Although the PBEs calculation showed that impact of natural variation of O2 is negligible on the CO2 and CH4 measurements, significant bias was inferred for the measurement of synthetic standard gases. For gas standards balanced with purified air, the PBEs were estimated to be marginal (up to 0.05 ppm for CO2 and 0.01 ppb for CH4 although the PBEs were substantial (up to 0.87 ppm for CO2 and 1.4 ppb for CH4 for standards balanced with synthetic air. For isotopic biases on CO2 measurements, we compared experimental results and theoretical calculations, which showed excellent agreement within their uncertainty. We derived instrument-specific water correction functions empirically for three WS-CRDS instruments (Picarro EnviroSense 3000i, G-1301, and G-2301, and evaluated the transferability of the water correction function from G-1301 among these instruments. Although the transferability was not proven, no significant difference was found in the water vapor correction function for the investigated WS-CRDS instruments as well as the instruments reported in the past

  4. A measurement system for continuous observations of CO2, CH4, H2O and CO onboard passenger aircraft

    Science.gov (United States)

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

    2013-04-01

    Improved quantification and understanding of surface-atmosphere exchange fluxes of greenhouse gases (GHGs) caused by natural as well as anthropogenic processes is of paramount importance in a world of a changing climate and ever increasing emissions. Top-down estimation of GHG fluxes is traditionally done by inverse transport modeling, using GHG observations from a global network of stations. Uncertainties in modeled vertical transport rates (moist convection, turbulent mixing, stratosphere-troposphere exchange) however greatly affect the quality of flux estimates. More recently, remote sensing of vertical column mole fractions of GHGs have become available for inverse modeling, reducing the impact of vertical transport uncertainties to first order. However, those need validation against in-situ observations. A strategy for regular, global in-situ atmospheric profiling of GHGs, covering at least the troposphere, is thus needed to provide validation of remote sensing and of forward transport modeling of GHGs, to serve as input for inverse modeling, and to reduce the impact of transport uncertainties. IAGOS-ERI (In-service Aircraft for a Global Observing System - European Research Infrastructure) exploits the synergy between globally operating civil aviation and the need for long-term monitoring of atmospheric composition. Within the framework of IAGOS-ERI a cavity ring-down spectroscopy (CRDS) based measurement system for greenhouse gases was designed, tested, and qualified for deployment on commercial airliners. The design meets requirements regarding physical dimensions (size, weight), performance (long-term stability, low maintenance, robustness, full automation) and safety issues (fire prevention regulations, airworthiness). The system uses components of a commercially available CRDS instrument (G2401-m, Picarro Inc.) mounted into a frame suitable for integration in the avionics bay of the Airbus A-340. The first of the IAGOS GHG packages is scheduled for

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

    Directory of Open Access Journals (Sweden)

    Annette Filges

    2015-09-01

    Full Text Available 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 designed, tested and qualified for deployment on commercial airliners. The design meets requirements regarding physical dimensions (size, weight, performance (long-term stability, low maintenance, robustness, full automation and safety issues (fire-prevention regulations. The system uses components of a commercially available CRDS instrument (G2401-m, Picarro Inc. mounted into a frame suitable for integration in the avionics bay of the Airbus A330 and A340 series. To enable robust and automated operation of the IAGOS-core GHG package over 6-month deployment periods, numerous technical issues had to be addressed. An inlet system was designed to eliminate sampling of larger aerosols, ice particles and water droplets, and to provide additional positive ram-pressure to ensure operation throughout an aircraft altitude operating range up to 12.5 km without an upstream sampling pump. Furthermore, no sample drying is required as the simultaneously measured water vapour mole fraction is used to correct for dilution and spectroscopic effects. This also enables measurements of water vapour throughout the atmosphere. To allow for trace gas measurements to be fully traceable to World Meteorological Organization scales, a two-standard calibration system has been designed and tested, which periodically provides calibration gas to the instrument during flight and on ground for each 6-month deployment period. The first of the IAGOS-core GHG packages is scheduled for integration in 2015. The aim is to have five systems operational within 4 yr, providing regular, long-term GHG observations covering major parts of the globe. This paper presents results from recent test

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

    Directory of Open Access Journals (Sweden)

    Reza Abedini

    2014-10-01

    Full Text Available The effect of Materials Institute Lavoisier-53 (MIL-53 particles on gas transport properties of polymethylpentyne (PMP was investigated. MIL-53 was added to the polymer matrix with different loadings of 10, 20 and 30 wt%. The properties of MIL-53 and prepared membranes were analyzed through FTIR, SEM and TGA methods. The adsorption of CO2 and CH4 was conducted and analyzed accurately through Langmuir equation to investigate the gas transport properties of membranes. The results from TGA showed that degradation temperature (Td increases significantly with increasing MIL-53 loading. SEM images demonstrated that MIL-53 particles dispersed well in polymer matrix with no considerable agglomeration and no non-selective void formation at polymer/filler interface. In addition, CO2 and CH4 permeability measurement along with calculation of CO2/CH4 selectivity were performed. The results showed that the permeability of gases (especially for CO2 increased significantly by increasing the MIL-53 loading. Additionally, CO2/CH4 selectivity showed an increasing trend with increasing the MIL-53 weight percent. Unlike CH4, the CO2 solubility coefficient increased with increasing the MIL-53 loading because of high free volume of membrane and selective adsorption of CO2 with MIL-53. Despite CO2 solubility enhancement its diffusivity coefficient remained more or less unchanged. The enhancement in CH4 permeability has been mainly attributed to its slight incremental diffusivity due to the membrane's increasingly higher free volume. Finally, a comparison between membranes performance and CO2/CH4 Robeson upper bound showed that, the performance of membranes improved due to the presence of MIL-53 which was very close to the Robeson bound.

  7. Measurements of CO2, CH4, H2O, and HDO over a 2-km Outdoor Path with Dual-Comb Spectroscopy

    Science.gov (United States)

    Rieker, G. B.; Giorgetta, F. R.; Coddington, I.; Swann, W. C.; Sinclair, L. C.; Cromer, C.; Baumann, E.; Newbury, N. R.; Kofler, J.; Petron, G.; Sweeney, C.; Tans, P. P.

    2013-12-01

    We demonstrate simultaneous sensing of CO2, CH4, H2O, and HDO over a 2-km outdoor open air path using dual-frequency-comb absorption spectroscopy (DCS). Our implementation of the DCS technique simultaneously offers broad spectral coverage (>8 THz, 267 cm-1) and fine spectral point spacing (100 MHz, 0.0033 cm-1) with a coherent eye-safe beam. The spectrometer, which is adapted from [Zolot et al., 2012], consists of two mutually coherent Erbium-doped fiber frequency-comb lasers which create a broad spectrum of perfectly spaced narrow linewidth frequency elements (';comb teeth') near 1.6 μm. The comb light is transmitted by a telescope and active steering mirrors from the roof of the NIST Boulder laboratory to a 50-cm flat mirror located 1 km away. The return light is received by a second telescope and carried via multimode fiber to a detector. The greenhouse gas absorption attenuates the teeth from the two combs that are coincident with the relevant molecular resonant frequencies. We purposefully offset the frequencies between the two frequency combs in a Vernier-like fashion so that each pair of comb teeth from the two combs results in a unique rf heterodyne beat frequency on the photodiode. The spectral spacing between subsequent comb teeth pairs is 100 MHz, far lower than the ~4 GHz linewidths of small molecule absorption features in the atmosphere. Because of the narrow comb linewidth, there is an essentially negligible instrument lineshape. The measured absorption spectrum can thus resolve neighboring absorption features of different species, and can be compared directly with HITRAN and recent greenhouse gas absorption models developed for satellite- and ground-based carbon observatories to determine the path-integrated concentrations of the absorbing species. Measurements covering the complete 30013←00001 absorption band of CO2 and absorption features of CH4, H2O and HDO between 1.6-1.67 μm were performed under a variety of atmospheric conditions. During

  8. Airborne remote-sensing of atmospheric CH4 and CO2 with MAMap: first results of measurements over wetlands in Germany and a N-S transect from Canada to Chile

    Science.gov (United States)

    Tretner, A.; Gerilowski, K.; Bovensmann, H.; Buchwitz, M.; Bertagnolio, P. P.; Erzinger, J.; Burrows, J.

    2008-12-01

    The Methane Airborne Mapper (MAMap) was designed for CO2 and CH4 remote sensing of the atmospheric column between an aircraft and the Earth's surface. The instrument is specified to detect mixing ratio variations below the aircraft of wetlands have been conducted in Germany and correlated to ground-based measurements. A first version of the data retrieval has been developed using a modified version of the WFM-DOAS algorithm. WFM-DOAS is also used for the retrieval of CH4 and CO2 column concentrations from nadir measurements by SCIAMACHY onboard ENVISAT. In November 2008, a transect from Oshawa, Canada to Punta Arenas, Chile will be flown onboard the AWI POLAR 5 aircraft. Along the flight path CH4 and CO2 measurements will be conducted by MAMap. Besides the N-S track (Canada-USA-Bahamas-Panama-Ecuador-Peru-Chile), an additional W-E track from Guayaquil (Ecuador) to Iquitos (Peru) and back is planned, covering large areas of Peruvian rainforest. One focus of this project is the evaluation of tropical rain forest and savannah as sources/sinks of CH4 and CO2. Discrepancies between the models and satellite data regarding atmospheric CH4 concentrations over the tropics have been reported in the past. A first assessment of MAMap measurements performed in 2008 over wetlands in Germany and the AWI-POLAR 5 campaign will be presented.

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

    Science.gov (United States)

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

    2016-12-01

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

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

    Science.gov (United States)

    Zheng, J.

    2016-12-01

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

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

    Science.gov (United States)

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

    2018-04-01

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

  12. A Portable FTIR Analyser for Field Measurements of Trace Gases and their Isotopologues: CO2, CH4, N2O, CO, del13C in CO2 and delD in water vapour

    Science.gov (United States)

    Griffith, D. W.; Bryant, G. R.; Deutscher, N. M.; Wilson, S. R.; Kettlewell, G.; Riggenbach, M.

    2007-12-01

    We describe a portable Fourier Transform InfraRed (FTIR) analyser capable of simultaneous high precision analysis of CO2, CH4, N2O and CO in air, as well as δ13C in CO2 and δD in water vapour. The instrument is based on a commercial 1 cm-1 resolution FTIR spectrometer fitted with a mid-IR globar source, 26 m multipass White cell and thermoelectrically-cooled MCT detector operating between 2000 and 7500 cm-1. Air is passed through the cell and analysed in real time without any pre-treatment except for (optional) drying. An inlet selection manifold allows automated sequential analysis of samples from one or more inlet lines, with typical measurement times of 1-10 minutes per sample. The spectrometer, inlet sampling sequence, real-time quantitative spectrum analysis, data logging and display are all under the control of a single program running on a laptop PC, and can be left unattended for continuous measurements over periods of weeks to months. Selected spectral regions of typically 100-200 cm-1 width are analysed by a least squares fitting technique to retrieve concentrations of trace gases, 13CO2 and HDO. Typical precision is better than 0.1% without the need for calibration gases. Accuracy is similar if measurements are referenced to calibration standard gases. δ13C precision is typically around 0.1‰, and for δD it is 1‰. Applications of the analyser include clean and polluted air monitoring, tower-based flux measurements such as flux gradient or integrated horizontal flux measurements, automated soil chambers, and field-based measurements of isotopic fractionation in soil-plant-atmosphere systems. The simultaneous multi-component advantages can be exploited in tracer-type emission measurements, for example of CH4 from livestock using a co-released tracer gas and downwind measurement. We have also developed an open path variant especially suited to tracer release studies and measurements of NH3 emissions from agricultural sources. An illustrative

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

    Science.gov (United States)

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

    2016-12-01

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

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

    Directory of Open Access Journals (Sweden)

    H. Jamali

    2013-04-01

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

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

    Science.gov (United States)

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

    2013-04-01

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

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

    Science.gov (United States)

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

    2015-01-01

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

  17. The total column of CO2 and CH4 measured with a compact Fourier transform spectrometer at NASA Armstrong Flight Research Center and Railroad Valley, Nevada, USA

    Science.gov (United States)

    Kawakami, S.; Shiomi, K.; Suto, H.; Kuze, A.; Hillyard, P. W.; Tanaka, T.; Podolske, J. R.; Iraci, L. T.; Albertson, R. T.

    2014-12-01

    The total columns of carbon dioxide (XCO2) and methane (XCH4) were measured with a compact Fourier transform spectrometer (FTS) at NASA Armstrong Flight Research Center (AFRC) and Railroad Valley, Nevada, USA (RRV) during a vicarious calibration campaign in June 2014. The campaign was performed to estimate changes in the radiometric response of the Thermal and Near Infrared Sensor for carbon Observations Fourier Transform Spectrometer (TANSO-FTS) and the Cloud and Aerosol Imager (TANSO-CAI) aboard Greenhouse gases Observing SATellite (GOSAT). TANSO-FTS measures spectra of radiance scattered by the Earth surface with high- and medium-gain depending on the surface reflectance. At high reflectance areas, such as deserts over north Africa and Australia, TANSO-FTS collects spectra with medium-gain. There was differences on atmospheric pressure and XCO2 retrieved from spectra obtained between high-gain and medium-gain. Because the retrieved products are useful for evaluating the difference of spectral qualities between high- and medium-gain, this work is an attempt to collect validation data for spectra with medium-gain of TANSO-FTS at remote and desert area with a compact and medium-spectral resolution instrument. As a compact FTS, EM27/SUN was used. It was manufactured and newly released on April 1, 2014 by Bruker. It is robust and operable in a high temperature environment. It was housed in a steel box to protect from dust and rain and powered by Solar panels. It can be operated by such a remote and desert area, like a RRV. Over AFRC and RRV, vertical profiles of CO2 and CH4 were measured using the Alpha Jet research aircraft as part of the Alpha Jet Atmospheric eXperiment (AJAX) of ARC, NASA. The values were calibrated to standard gases. To make the results comparable to WMO (World Meteorological Organization) standards, the retrieved XCO2 and XCH4 values are divided by a calibration factor. This values were determined by comparisons with in situ profiles measured by

  18. Continuous multi-plot measurements of CO2, CH4, N2O and H2O in a managed boreal forest - The importance of accounting for all greenhouse gases

    Science.gov (United States)

    Vestin, P.; Mölder, M.; Sundqvist, E.; Båth, A.; Lehner, I.; Weslien, P.; Klemedtsson, L.; Lindroth, A.

    2015-12-01

    In order to assess the effects of different management practices on the exchange of greenhouse gases (GHG), it is desirable to perform repeated and parallel measurements on both experimental and control plots. Here we demonstrate how a system system combining eddy covariance and gradient techniques can be used to perform this assessment in a managed forest ecosystem.The net effects of clear-cutting and stump harvesting on GHG fluxes were studied at the ICOS site Norunda, Sweden. Micrometeorological measurements (i.e., flux-gradient measurements in 3 m tall towers) allowed for quantification of CO2, CH4 and H2O fluxes (from May 2010) as well as N2O and H2O fluxes (from June 2011) at two stump harvested plots and two control plots. There was one wetter and one drier plot of each treatment. Air was continuously sampled at two heights in the towers and gas concentrations were analyzed for CH4, CO2, H2O (LGR DLT-100, Los Gatos Research) and N2O, H2O (QCL Mini Monitor, Aerodyne Research). Friction velocities and sensible heat fluxes were measured by sonic anemometers (Gill Windmaster, Gill Instruments Ltd). Automatic chamber measurements (CO2, CH4, H2O) were carried out in the adjacent forest stand and at the clear-cut during 2010.Average CO2 emissions for the first year ranged between 14.4-20.2 ton CO2 ha-1 yr-1. The clear-cut became waterlogged after harvest and a comparison of flux-gradient data and chamber data (from the adjacent forest stand) indicated a switch from a weak CH4 sink to a significant source at all plots. The CH4 emissions ranged between 0.8-4.5 ton CO2-eq. ha-1 yr-1. N2O emissions ranged between 0.4-2.6 ton CO2-eq. ha-1 yr-1. Enhanced N2O emission on the drier stump harvested plot was the only clear treatment effect on GHG fluxes that was observed. Mean CH4 and N2O emissions for the first year of measurements amounted up to 29% and 20% of the mean annual CO2 emissions, respectively. This highlights the importance of including all GHGs when assessing

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

    Directory of Open Access Journals (Sweden)

    Knut Arne Birkedal

    2015-05-01

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

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

    DEFF Research Database (Denmark)

    Ambus, P.; Robertson, G.P.

    1999-01-01

    Elevated atmospheric CO2 has the potential to change below-ground nutrient cycling and thereby alter the soil-atmosphere exchange of biogenic trace gases. We measured fluxes of CH4 and N2O in trembling aspen (Populus tremuloides Michx.) stands grown in open-top chambers under ambient and twice......-ambient CO2 concentrations crossed with `high' and low soil-N conditions. Flux measurements with small static chambers indicated net CH4 oxidation in the open-top chambers. Across dates, CH4 oxidation activity was significantly (P CO2 (8.7 mu g CH4-C m(-2) h(-1)) than...... with elevated CO2 (6.5 mu g CH4-C m(-2) h(-1)) in the low N soil. Likewise, across dates and soil N treatments CH4 was oxidized more rapidly (P CO2 (9.5 mu g CH4-C m(-2) h(-1)) than in chambers with elevated CO2 (8.8 mu g CH4-C m(-2) h(-1)). Methane oxidation in soils incubated...

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

    Science.gov (United States)

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

    2017-12-01

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

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

    Science.gov (United States)

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

    2012-12-01

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

  3. Thermodynamic stability and guest distribution of CH4/N2/CO2 mixed hydrates for methane hydrate production using N2/CO2 injection

    International Nuclear Information System (INIS)

    Lim, Dongwook; Ro, Hyeyoon; Seo, Yongwon; Seo, Young-ju; Lee, Joo Yong; Kim, Se-Joon; Lee, Jaehyoung; Lee, Huen

    2017-01-01

    Highlights: • We examine the thermodynamic stability and guest distribution of CH 4 /N 2 /CO 2 mixed hydrates. • Phase equilibria of the CH 4 /N 2 /CO 2 mixed hydrates were measured to determine the thermodynamic stability. • The N 2 /CO 2 ratio of the hydrate phase is almost constant despite the enrichment of CO 2 in the hydrate phase. • 13 C NMR results indicate the preferential occupation of N 2 and CO 2 in the small and large cages of sI hydrates, respectively. - Abstract: In this study, thermodynamic stability and cage occupation behavior in the CH 4CO 2 replacement, which occurs in natural gas hydrate reservoirs by injecting flue gas, were investigated with a primary focus on phase equilibria and composition analysis. The phase equilibria of CH 4 /N 2 /CO 2 mixed hydrates with various compositions were measured to determine the thermodynamic stability of gas hydrate deposits replaced by N 2 /CO 2 gas mixtures. The fractional experimental pressure differences (Δp/p) with respect to the CSMGem predictions were found to range from −0.11 to −0.02. The composition analysis for various feed gas mixtures with a fixed N 2 /CO 2 ratio (4.0) shows that CO 2 is enriched in the hydrate phase, and the N 2 /CO 2 ratio in the hydrate phase is independent of the feed CH 4 fractions. Moreover, 13 C NMR measurements indicate that N 2 molecules preferentially occupy the small 5 12 cages of sI hydrates while the CO 2 molecules preferentially occupy the large 5 12 6 2 cages, resulting in an almost constant area ratio of CH 4 molecules in the large to small cages of the CH 4 /N 2 /CO 2 mixed hydrates. The overall experimental results provide a better understanding of stability conditions and guest distributions in natural gas hydrate deposits during CH 4 – flue gas replacement.

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

    International Nuclear Information System (INIS)

    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

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

    Science.gov (United States)

    Pain, A.; Martin, J.; Martin, E. E.

    2017-12-01

    Subglacial carbon processes are of increasing interest as warming induces ice melting and increases fluxes of glacial meltwater into proglacial rivers and the coastal ocean. Meltwater may serve as an atmospheric source or sink of carbon dioxide (CO2) or methane (CH4), depending on the magnitudes of subglacial organic carbon (OC) remineralization, which produces CO2 and CH4, and mineral weathering reactions, which consume CO2 but not CH4. We report wide variability in dissolved CO2 and CH4 concentrations at the beginning of the melt season (May-June 2017) between three sites draining land-terminating glaciers of the Greenland Ice Sheet. Two sites, located along the Watson River in western Greenland, drain the Isunnguata and Russell Glaciers and contained 1060 and 400 ppm CO2, respectively. In-situ CO2 flux measurements indicated that the Isunnguata was a source of atmospheric CO2, while the Russell was a sink. Both sites had elevated CH4 concentrations, at 325 and 25 ppm CH4, respectively, suggesting active anaerobic OC remineralization beneath the ice sheet. Dissolved CO2 and CH4 reached atmospheric equilibrium within 2.6 and 8.6 km downstream of Isunnguata and Russell discharge sites, respectively. These changes reflect rapid gas exchange with the atmosphere and/or CO2 consumption via instream mineral weathering. The third site, draining the Kiagtut Sermiat in southern Greenland, had about half atmospheric CO2 concentrations (250 ppm), but approximately atmospheric CH4 concentrations (2.1 ppm). Downstream CO2 flux measurements indicated ingassing of CO2 over the entire 10-km length of the proglacial river. CO2 undersaturation may be due to more readily weathered lithologies underlying the Kiagtut Sermiat compared to Watson River sites, but low CH4 concentrations also suggest limited contributions of CO2 and CH4 from OC remineralization. These results suggest that carbon processing beneath the Greenland Ice Sheet may be more variable than previously recognized

  6. O3, CH4, CO2, CO, NO2 and NMHC aircraft measurements in the Uinta Basin oil and gas region under low and high ozone conditions in winter 2012 and 2013

    Directory of Open Access Journals (Sweden)

    S. J. Oltmans

    2016-10-01

    Full Text Available Abstract Instrumented aircraft measuring air composition in the Uinta Basin, Utah, during February 2012 and January-February 2013 documented dramatically different atmospheric ozone (O3 mole fractions. In 2012 O3 remained near levels of ∼40 ppb in a well-mixed 500–1000 m deep boundary layer while in 2013, O3 mole fractions >140 ppb were measured in a shallow (∼200 m boundary layer. In contrast to 2012 when mole fractions of emissions from oil and gas production such as methane (CH4, non-methane hydrocarbons (NMHCs and combustion products such as carbon dioxide (CO2 were moderately elevated, in winter 2013 very high mole fractions were observed. Snow cover in 2013 helped produce and maintain strong temperature inversions that capped a shallow cold pool layer. In 2012, O3 and CH4 and associated NMHCs mole fractions were not closely related. In 2013, O3 mole fractions were correlated with CH4 and a suite of NMHCs identifying the gas field as the primary source of the O3 precursor NMHC emissions. In 2013 there was a strong positive correlation between CH4 and CO2 suggesting combustion from oil and natural gas processing activities. The presence of O3 precursor NMHCs through the depth of the boundary layer in 2013 led to O3 production throughout the layer. In 2013, O3 mole fractions increased over the course of the week-long episodes indicating O3 photochemical production was larger than dilution and deposition rates, while CH4 mole fractions began to level off after 3 days indicative of some air being mixed out of the boundary layer. The plume of a coal-fired power plant located east of the main gas field was not an important contributor to O3 or O3 precursors in the boundary layer in 2013.

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

    Science.gov (United States)

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

    2015-04-01

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

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

    Science.gov (United States)

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

    2000-01-01

    The BOREAS TGB-1 team made 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.

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

    Science.gov (United States)

    Sreenivas, Gaddamidi; Mahesh, Pathakoti; Subin, Jose; Lakshmi Kanchana, Asuri; Venkata Narasimha Rao, Pamaraju; Dadhwal, Vinay Kumar

    2016-03-01

    Atmospheric greenhouse gases (GHGs), such as carbon dioxide (CO2) and methane (CH4), are important climate forcing agents due to their significant impacts on the climate system. The present study brings out first continuous measurements of atmospheric GHGs using high-precision LGR-GGA over Shadnagar, a suburban site of Central India during the year 2014. The annual mean CO2 and CH4 over the study region are found to be 394 ± 2.92 and 1.92 ± 0.07 ppm (μ ± 1σ) respectively. CO2 and CH4 show a significant seasonal variation during the study period with maximum (minimum) CO2 observed during pre-monsoon (monsoon), while CH4 recorded the maximum during post-monsoon and minimum during monsoon. Irrespective of the seasons, consistent diurnal variations of these gases are observed. Influences of prevailing meteorology (air temperature, wind speed, wind direction, and relative humidity) on GHGs have also been investigated. CO2 and CH4 show a strong positive correlation during winter, pre-monsoon, monsoon, and post-monsoon with correlation coefficients (Rs) equal to 0.80, 0.80, 0.61, and 0.72 respectively, indicating a common anthropogenic source for these gases. Analysis of this study reveals the major sources for CO2 are soil respiration and anthropogenic emissions while vegetation acts as a main sink, whereas the major source and sink for CH4 are vegetation and presence of hydroxyl (OH) radicals.

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

    Science.gov (United States)

    Minoda, Tomomi; Kimura, Mamoto; Wada, Eitaro

    1996-09-01

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

  11. Analysis of the potential of near-ground measurements of CO2 and CH4 in London, UK, for the monitoring of city-scale emissions using an atmospheric transport model

    Science.gov (United States)

    Boon, Alex; Broquet, Grégoire; Clifford, Deborah J.; Chevallier, Frédéric; Butterfield, David M.; Pison, Isabelle; Ramonet, Michel; Paris, Jean-Daniel; Ciais, Philippe

    2016-06-01

    Carbon dioxide (CO2) and methane (CH4) mole fractions were measured at four near-ground sites located in and around London during the summer of 2012 with a view to investigating the potential of assimilating such measurements in an atmospheric inversion system for the monitoring of the CO2 and CH4 emissions in the London area. These data were analysed and compared with simulations using a modelling framework suited to building an inversion system: a 2 km horizontal resolution south of England configuration of the transport model CHIMERE driven by European Centre for Medium-Range Weather Forecasts (ECMWF) meteorological forcing, coupled to a 1 km horizontal resolution emission inventory (the UK National Atmospheric Emission Inventory). First comparisons reveal that local sources, which cannot be represented in the model at a 2 km resolution, have a large impact on measurements. We evaluate methods to filter out the impact of some of the other critical sources of discrepancies between the measurements and the model simulation except that of the errors in the emission inventory, which we attempt to isolate. Such a separation of the impact of errors in the emission inventory should make it easier to identify the corrections that should be applied to the inventory. Analysis is supported by observations from meteorological sites around the city and a 3-week period of atmospheric mixing layer height estimations from lidar measurements. The difficulties of modelling the mixing layer depth and thus CO2 and CH4 concentrations during the night, morning and late afternoon lead to focusing on the afternoon period for all further analyses. The discrepancies between observations and model simulations are high for both CO2 and CH4 (i.e. their root mean square (RMS) is between 8 and 12 parts per million (ppm) for CO2 and between 30 and 55 parts per billion (ppb) for CH4 at a given site). By analysing the gradients between the urban sites and a suburban or rural reference site, we

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

    Directory of Open Access Journals (Sweden)

    R. B. Rios

    2013-12-01

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

  13. "Atmospheric Measurements by Ultra-Light SpEctrometer" (AMULSE) dedicated to vertical profile measurements of greenhouse gases (CO2, CH4) under stratospheric balloons: instrumental development and field application.

    Science.gov (United States)

    Maamary, Rabih; Joly, Lilian; Decarpenterie, Thomas; Cousin, Julien; Dumelié, Nicolas; Grouiez, Bruno; Albora, Grégory; Chauvin, Nicolas; Miftah-El-Khair, Zineb; Legain, Dominique; Tzanos, Diane; Barrié, Joel; Moulin, Eric; Ramonet, Michel; Bréon, François-Marie; Durry, Georges

    2016-04-01

    Human activities disrupt natural biogeochemical cycles such as the carbon and contribute to an increase in the concentrations of the greenhouse gases (carbone dioxide and methane) in the atmosphere. The current atmospheric transport modeling (the vertical trade) still represents an important source of uncertainty in the determination of regional flows of greenhouse gases, which means that a good knowledge of the vertical distribution of CO2 is necessary to (1) make the link between the ground measurements and spatial measurements that consider an integrated concentration over the entire column of the atmosphere, (2) validate and if possible improve CO2 transport model to make the link between surface emissions and observed concentration. The aim of this work is to develop a lightweight instrument (based on mid-infrared laser spectrometry principles) for in-situ measuring at high temporal/spatial resolution (5 Hz) the vertical profiles of the CO2 and the CH4 using balloons (meteorological and BSO at high precision levels (costs and logistics flights. These laser spectrometers are built on recent instrumental developments. Several flights were successfully done in the region Champagne-Ardenne and in Canada recently. Aknowledgments: The authors acknowledge financial supports from CNES, CNRS défi instrumental and the region Champagne-Ardenne.

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

    DEFF Research Database (Denmark)

    Christensen, TR; Panikov, N; Mastepanov, M

    2003-01-01

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

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

    International Nuclear Information System (INIS)

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

    2014-01-01

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

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

    Science.gov (United States)

    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

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

    Science.gov (United States)

    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.

  18. Transport and transformation of soil-derived CO2, CH4 and DOC sustain CO2 supersaturation in small boreal streams.

    Science.gov (United States)

    Rasilo, Terhi; Hutchins, Ryan H S; Ruiz-González, Clara; Del Giorgio, Paul A

    2017-02-01

    Streams are typically supersaturated in carbon dioxide (CO 2 ) and methane (CH 4 ), and are recognized as important components of regional carbon (C) emissions in northern landscapes. Whereas there is consensus that in most of the systems the CO 2 emitted by streams represents C fixed in the terrestrial ecosystem, the pathways delivering this C to streams are still not well understood. We assessed the contribution of direct soil CO 2 injection versus the oxidation of soil-derived dissolved organic C (DOC) and CH 4 in supporting CO 2 supersaturation in boreal streams in Québec. We measured the concentrations of CO 2 , CH 4 and DOC in 43 streams and adjacent soil waters during summer base-flow period. A mass balance approach revealed that all three pathways are significant, and that the mineralization of soil-derived DOC and CH 4 accounted for most of the estimated stream CO 2 emissions (average 75% and 10%, respectively), and that these estimated contributions did not change significantly between the studied low order (≤3) streams. Whereas some of these transformations take place in the channel proper, our results suggest that they mainly occur in the hyporheic zones of the streams. Our results further show that stream CH 4 emissions can be fully explained by soil CH 4 inputs. This study confirms that these boreal streams, and in particular their hyporheic zones, are extremely active processors of soil derived DOC and CH 4 , not just vents for soil produced CO 2 . Copyright © 2016 Elsevier B.V. All rights reserved.

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

    Science.gov (United States)

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

    2017-12-01

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

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

    Science.gov (United States)

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

    2015-04-01

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

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2017-10-01

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

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

    Science.gov (United States)

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

    2013-12-01

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

  3. Characterization of trace gases measured over Alberta oil sands mining operations: 76 speciated C2-C10 volatile organic compounds (VOCs), CO2, CH4, CO, NO, NO2, NOy, O3 and SO2

    Science.gov (United States)

    Simpson, I. J.; Blake, N. J.; Barletta, B.; Diskin, G. S.; Fuelberg, H. E.; Gorham, K.; Huey, L. G.; Meinardi, S.; Rowland, F. S.; Vay, S. A.; Weinheimer, A. J.; Yang, M.; Blake, D. R.

    2010-12-01

    Oil sands comprise 30% of the world's oil reserves and the crude oil reserves in Canada's oil sands deposits are second only to Saudi Arabia. The extraction and processing of oil sands is much more challenging than for light sweet crude oils because of the high viscosity of the bitumen contained within the oil sands and because the bitumen is mixed with sand and contains chemical impurities such as sulphur. Despite these challenges, the importance of oil sands is increasing in the energy market. To our best knowledge this is the first peer-reviewed study to characterize volatile organic compounds (VOCs) emitted from Alberta's oil sands mining sites. We present high-precision gas chromatography measurements of 76 speciated C2-C10 VOCs (alkanes, alkenes, alkynes, cycloalkanes, aromatics, monoterpenes, oxygenated hydrocarbons, halocarbons and sulphur compounds) in 17 boundary layer air samples collected over surface mining operations in northeast Alberta on 10 July 2008, using the NASA DC-8 airborne laboratory as a research platform. In addition to the VOCs, we present simultaneous measurements of CO2, CH4, CO, NO, NO2, NOy, O3 and SO2, which were measured in situ aboard the DC-8. Carbon dioxide, CH4, CO, NO, NO2, NOy, SO2 and 53 VOCs (e.g., non-methane hydrocarbons, halocarbons, sulphur species) showed clear statistical enhancements (1.1-397×) over the oil sands compared to local background values and, with the exception of CO, were greater over the oil sands than at any other time during the flight. Twenty halocarbons (e.g., CFCs, HFCs, halons, brominated species) either were not enhanced or were minimally enhanced (industry fell into two groups: (1) evaporative emissions from the oil sands and its products and/or from the diluent used to lower the viscosity of the extracted bitumen (i.e., C4-C9 alkanes, C5-C6 cycloalkanes, C6-C8 aromatics), together with CO; and (2) emissions associated with the mining effort, such as upgraders (i.e., CO2, CO, CH4, NO, NO2, NOy

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

    Science.gov (United States)

    Somekawa, Toshihiro; Fujita, Masayuki

    2018-04-01

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

  5. Assessing CH4 and CO2 emissions from wetlands in the Drenthe province, The Netherlands: a modelling approach

    NARCIS (Netherlands)

    Petrescu, A.J.; Huissteden, van J.; Vries, de F.; Bregman, E.P.H.; Scheper, A.

    2009-01-01

    Assessment of land use related greenhouse gas (GHG) emissions on larger spatial scales is usually achieved by modelling. Surface flux measurements are expensive and measurement locations too widely scattered to serve as spatially reliable flux estimates. Here we assess CO2 and CH4 fluxes from

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

    Science.gov (United States)

    Saad Khan, Muhammad; Yaqub, Sana; Manner, Naathiya; Ani Karthwathi, Nur; Qasim, Ali; Mellon, Nurhayati Binti; Lal, Bhajan

    2018-04-01

    Clathrate hydrates are eminent structures regard as a threat to the gas and oil industry in light of their irritating propensity to subsea pipelines. For natural gas transmission and processing, the formation of gas hydrate is one of the main flow assurance delinquent has led researchers toward conducting fresh and meticulous studies on various aspects of gas hydrates. This paper highlighted the thermodynamic analysis on pure CH4 and CO2 gas hydrates on the custom fabricated equipment (Sapphire cell hydrate reactor) for experimental validation. CO2 gas hydrate formed at lower pressure (41 bar) as compared to CH4 gas hydrate (70 bar) while comparison of thermodynamic properties between CH4 and CO2 also presented in this study. This preliminary study could provide pathways for the quest of potent hydrate inhibitors.

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

    International Nuclear Information System (INIS)

    McNamara, N.P.; Plant, T.; Oakley, S.; Ward, S.; Wood, C.; Ostle, N.

    2008-01-01

    Peatlands are long term carbon catchments that sink atmospheric carbon dioxide (CO 2 ) and source methane (CH 4 ). In the uplands of the United Kingdom ombrotrophic blanket peatlands commonly exist within Calluna vulgaris (L.) dominated moorland ecosystems. These landscapes contain a range of topographical features that influence local hydrology, climate and plant community composition. In this study we examined the variation in ecosystem CO 2 respiration and net CH 4 fluxes from typical plant-soil systems in dendritic drainage gullies and adjacent blanket peat during the growing season. Typically, Eriophorum spp., Sphagnum spp. and mixed grasses occupied gullies while C. vulgaris dominated in adjacent blanket peat. Gross CO 2 respiration was highest in the areas of Eriophorum spp. (650 ± 140 mg CO 2 m -2 h -1 ) compared to those with Sphagnum spp. (338 ± 49 mg CO 2 m -2 h -1 ), mixed grasses (342 ± 91 mg CO 2 m -2 h -1 ) and C. vulgaris (174 ± 63 mg CO 2 m -2 h -1 ). Measurements of the net CH 4 flux showed higher fluxes from the Eriophorum spp (2.2 ± 0.6 mg CH 4 m -2 h -1 ) locations compared to the Sphagnum spp. (0.6 ± 0.4 mg CH 4 m -2 h -1 ), mixed grasses (0.1 ±0.1 mg CH 4 m -2 h -1 ) and a negligible flux detected from C. vulgaris (0.0 ± 0.0 mg CH 4 m -2 h -1 ) locations. A GIS approach was applied to calculate the contribution of gullies to landscape scale greenhouse gas fluxes. Findings from the Moor House National Nature Reserve in the UK showed that although gullies occupied only 9.3% of the total land surface, gullies accounted for 95.8% and 21.6% of the peatland net CH 4 and CO 2 respiratory fluxes, respectively. The implication of these findings is that the relative contribution of characteristic gully systems need to be considered in estimates of landscape scale peatland greenhouse gas fluxes

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

    Science.gov (United States)

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

    2016-05-01

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

  9. The IAGOS GHG package: a measurement system for continuous airborne observations of CO2, CH4, H2O and CO

    Science.gov (United States)

    Gerbig, C.; Filges, A.; Franke, H.; Klaus, C.; Chen, H.

    2012-12-01

    A cavity ring-down spectroscopy (CRDS) based measurement system for greenhouse gases was designed, tested, and qualified for deployment on commercial airliners within the IAGOS-ERI (In-service Aircraft for a Global Observing System - European Research Infrastructure) project. The design meets requirements regarding physical dimensions (size, weight), performance (long term stability, low maintenance, robustness, full automation) and safety issues (fire prevention regulations). The system uses components of a commercially available CRDS instrument (G2401-m, Picarro Inc.) integrated in a frame suitable for integration in the avionics bay of the Airbus A-340. The first of the IAGOS GHG packages is scheduled for integration in early 2013. The aim is to have seven systems operational within four years, providing for long-term GHG observations with near-global coverage. To enable robust and automated operation of the IAGOS GHG package over six-month deployment periods, numerous technical issues had to be addressed. An inlet system, designed as virtual impactor to eliminate sampling of larger aerosols, ice particles, and water droplets, and provides additional positive ram-pressure. In combination with a lowered sample flow of 0.1 slpm, this ensures a fully controlled sample pressure in the cavity of 140 torr throughout the aircraft altitude operating range up to 12.5 km without the need of an upstream sampling pump. Furthermore, no sample drying is required, as the simultaneously measured water vapor mole fraction is used to correct for dilution and spectroscopic effects. This also enables the collection of science-quality water vapor measurements throughout the atmosphere. To allow for trace gas measurements to be fully traceable to WMO scales, a two-standard calibration system has been designed and tested that periodically provides calibration gas to the instrument during flight and on ground. A targeted six-month deployment cycle followed by maintenance of the package

  10. Comprehensive laboratory and field testing of cavity ring-down spectroscopy analyzers measuring H2O, CO2, CH4 and CO

    Science.gov (United States)

    Yver Kwok, C.; Laurent, O.; Guemri, A.; Philippon, C.; Wastine, B.; Rella, C. W.; Vuillemin, C.; Truong, F.; Delmotte, M.; Kazan, V.; Darding, M.; Lebègue, B.; Kaiser, C.; Xueref-Rémy, I.; Ramonet, M.

    2015-09-01

    To develop an accurate measurement network of greenhouse gases, instruments in the field need to be stable and precise and thus require infrequent calibrations and a low consumption of consumables. For about 10 years, cavity ring-down spectroscopy (CRDS) analyzers have been available that meet these stringent requirements for precision and stability. Here, we present the results of tests of CRDS instruments in the laboratory (47 instruments) and in the field (15 instruments). The precision and stability of the measurements are studied. We demonstrate that, thanks to rigorous testing, newer models generally perform better than older models, especially in terms of reproducibility between instruments. In the field, we see the importance of individual diagnostics during the installation phase, and we show the value of calibration and target gases that assess the quality of the data. Finally, we formulate recommendations for use of these analyzers in the field.

  11. Comprehensive laboratory and field testing of cavity ring-down spectroscopy analyzers measuring H2O, CO2, CH4 and CO

    Directory of Open Access Journals (Sweden)

    C. Yver Kwok

    2015-09-01

    Full Text Available To develop an accurate measurement network of greenhouse gases, instruments in the field need to be stable and precise and thus require infrequent calibrations and a low consumption of consumables. For about 10 years, cavity ring-down spectroscopy (CRDS analyzers have been available that meet these stringent requirements for precision and stability. Here, we present the results of tests of CRDS instruments in the laboratory (47 instruments and in the field (15 instruments. The precision and stability of the measurements are studied. We demonstrate that, thanks to rigorous testing, newer models generally perform better than older models, especially in terms of reproducibility between instruments. In the field, we see the importance of individual diagnostics during the installation phase, and we show the value of calibration and target gases that assess the quality of the data. Finally, we formulate recommendations for use of these analyzers in the field.

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

    Science.gov (United States)

    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.

  13. Inverse modeling of GOSAT-retrieved ratios of total column CH4 and CO2 for 2009 and 2010

    Directory of Open Access Journals (Sweden)

    S. Pandey

    2016-04-01

    Full Text Available This study investigates the constraint provided by greenhouse gas measurements from space on surface fluxes. Imperfect knowledge of the light path through the atmosphere, arising from scattering by clouds and aerosols, can create biases in column measurements retrieved from space. To minimize the impact of such biases, ratios of total column retrieved CH4 and CO2 (Xratio have been used. We apply the ratio inversion method described in Pandey et al. (2015 to retrievals from the Greenhouse Gases Observing SATellite (GOSAT. The ratio inversion method uses the measured Xratio as a weak constraint on CO2 fluxes. In contrast, the more common approach of inverting proxy CH4 retrievals (Frankenberg et al., 2005 prescribes atmospheric CO2 fields and optimizes only CH4 fluxes. The TM5–4DVAR (Tracer Transport Model version 5–variational data assimilation system inverse modeling system is used to simultaneously optimize the fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy inversions using model-derived CO2 mixing ratios (XCO2model from CarbonTracker and the Monitoring Atmospheric Composition and Climate (MACC Reanalysis CO2 product. The performance of the inverse models is evaluated using measurements from three aircraft measurement projects. Xratio and XCO2model are compared with TCCON retrievals to quantify the relative importance of errors in these components of the proxy XCH4 retrieval (XCH4proxy. We find that the retrieval errors in Xratio (mean  =  0.61 % are generally larger than the errors in XCO2model (mean  =  0.24 and 0.01 % for CarbonTracker and MACC, respectively. On the annual timescale, the CH4 fluxes from the different satellite inversions are generally in agreement with each other, suggesting that errors in XCO2model do not limit the overall accuracy of the CH4 flux estimates. On the seasonal timescale, however, larger differences are found due to uncertainties in XCO2model, particularly

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

    Science.gov (United States)

    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

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

    International Nuclear Information System (INIS)

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

    2014-01-01

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

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

    DEFF Research Database (Denmark)

    Hellwing, Anne Louise Frydendahl; Weisbjerg, Martin Riis; Madsen, Jørgen

    2013-01-01

    under farm management control. CO2 is released largely from microbial decay or burning of plant litter and soil organic matter. CH4 is produced when organic materials decompose under anoxic conditions, notably from fermentative digestion by ruminant livestock, stored manures, wetlands and rice grown...

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

    International Nuclear Information System (INIS)

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

    2006-01-01

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

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

    Science.gov (United States)

    Nordin, Nik Abdul Hadi Md; Ismail, Ahmad Fauzi; Misdan, Nurasyikin; Nazri, Noor Aina Mohd

    2017-10-01

    Tunability of metal-organic frameworks (MOFs) properties enables them to be tailored for specific applications. In this study, zeolitic imidazole framework 8 (ZIF-8), sub-class of MOF, underwent pre-synthesis and post-synthesis modifications. The pre-synthesis modification using GO (ZIF-8/GO) shows slight decrease in textural properties, while the post-synthesis modification using amine solution (ZIF-8/NH2) resulted in superior BET surface area and pore volume. Mixed matrix membranes (MMMs) derived from polysulfone (PSf) and the modified ZIF-8s were then prepared via dry/wet phase inversion. The polymer chain flexibility of the resulted MMMs shows rigidification, where ZIF-8/NH2 as filler resulting higher rigidification compared to ZIF-8/GO. The MMMs were further subjected to pure CO2 and CH4 gas permeation experiments. The PSf/ZIF-8/NH2 shows superior CO2/CH4 selectivity (88% increased) while sacrificing CO2 permeance due to combination of severe polymer chain rigidification and the presence of CO2-philic group, amine. Whereas, the PSf/ZIF-8/GO possess 64% increase in CO2 permeance without notable changes in CO2/CH4 selectivity.

  19. Biogeochemical modeling of CO2 and CH4 production in anoxic Arctic soil microcosms

    Science.gov (United States)

    Tang, Guoping; Zheng, Jianqiu; Xu, Xiaofeng; Yang, Ziming; Graham, David E.; Gu, Baohua; Painter, Scott L.; Thornton, Peter E.

    2016-09-01

    Soil organic carbon turnover to CO2 and CH4 is sensitive to soil redox potential and pH conditions. However, land surface models do not consider redox and pH in the aqueous phase explicitly, thereby limiting their use for making predictions in anoxic environments. Using recent data from incubations of Arctic soils, we extend the Community Land Model with coupled carbon and nitrogen (CLM-CN) decomposition cascade to include simple organic substrate turnover, fermentation, Fe(III) reduction, and methanogenesis reactions, and assess the efficacy of various temperature and pH response functions. Incorporating the Windermere Humic Aqueous Model (WHAM) enables us to approximately describe the observed pH evolution without additional parameterization. Although Fe(III) reduction is normally assumed to compete with methanogenesis, the model predicts that Fe(III) reduction raises the pH from acidic to neutral, thereby reducing environmental stress to methanogens and accelerating methane production when substrates are not limiting. The equilibrium speciation predicts a substantial increase in CO2 solubility as pH increases, and taking into account CO2 adsorption to surface sites of metal oxides further decreases the predicted headspace gas-phase fraction at low pH. Without adequate representation of these speciation reactions, as well as the impacts of pH, temperature, and pressure, the CO2 production from closed microcosms can be substantially underestimated based on headspace CO2 measurements only. Our results demonstrate the efficacy of geochemical models for simulating soil biogeochemistry and provide predictive understanding and mechanistic representations that can be incorporated into land surface models to improve climate predictions.

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

    Science.gov (United States)

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

    2013-12-01

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

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

    Science.gov (United States)

    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

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

    DEFF Research Database (Denmark)

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

    2009-01-01

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

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

    Science.gov (United States)

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

    2014-01-01

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

  4. Integrated Path Detection of Co2 and CH4 Using a Waveform Driven Electro-Optic Single Sideband Laser Source

    Directory of Open Access Journals (Sweden)

    Wagner Gerd

    2016-01-01

    Full Text Available Integrated path concentrations of ambient levels of carbon dioxide and methane have been measured during nighttime periods at NIST, Boulder (CO, USA, using a ground-based, eyesafe laser system. In this contribution, we describe the transmitter and receiver system, demonstrate measurements of CO2 and CH4 in comparison with an in situ point sensor measurement using a commercial cavity ring-down instrument, and demonstrate a speckle noise reduction method.

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

    KAUST Repository

    Al-Sabban, Bedour

    2017-05-02

    Dry reforming of methane (DRM) proceeds via CH4 decomposition to leave surface carbon species, followed by their removal with CO2-derived species. Reactivity tuning for stoichiometric CH4/CO2 reactants was attempted by alloying the non-noble metals Co and Ni, which have high affinity with CO2 and high activity for CH4 decomposition, respectively. This study was focused on providing evidence of the capturing surface coverage of the reactive intermediates and the associated structural changes of the metals during DRM at high temperature using in-operando X-ray absorption spectroscopy (XAS). On the Co catalysts, the first-order effects with respect to CH4 pressure and negative-order effects with respect to CO2 pressure on the DRM rate are consistent with the competitive adsorption of the surface oxygen species on the same sites as the CH4 decomposition reaction. The Ni surface provides comparatively higher rates of CH4 decomposition and the resultant DRM than the Co catalyst but leaves some deposited carbon on the catalyst surface. In contrast, the bimetallic CoNi catalyst exhibits reactivity towards the DRM but with kinetic orders resembling Co catalyst, producing negligible carbon deposition by balancing CH4 and CO2 activation. The in-operando X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) measurements confirmed that the Co catalyst was progressively oxidized from the surface to the bulk with reaction time, whereas CoNi and Ni remained relatively reduced during DRM. Density functional theory (DFT) calculation considering the high reaction temperature for DRM confirmed the unselective site arrangement between Co and Ni atoms in both the surface and bulk of the alloy nanoparticle (NP). The calculated heat of oxygen chemisorption became more exothermic in the order of Ni, CoNi, Co, consistent with the catalytic behavior. The comprehensive experimental and theoretical evidence provided herein clearly suggests

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

    International Nuclear Information System (INIS)

    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.)

  7. Effects of Long-Term CO2 Enrichment on Soil-Atmosphere CH4 Fluxes and the Spatial Micro-Distribution of Methanotrophic Bacteria.

    Science.gov (United States)

    Karbin, Saeed; Guillet, Cécile; Kammann, Claudia I; Niklaus, Pascal A

    2015-01-01

    Effects of elevated atmospheric CO2 concentrations on plant growth and associated C cycling have intensively been studied, but less is known about effects on the fluxes of radiatively active trace gases other than CO2. Net soil-atmosphere CH4 fluxes are determined by the balance of soil microbially-driven methane (CH4) oxidation and methanogenesis, and both might change under elevated CO2. Here, we studied CH4 dynamics in a permanent grassland exposed to elevated CO2 for 14 years. Soil-atmosphere fluxes of CH4 were measured using large static chambers, over a period of four years. The ecosystem was a net sink for atmospheric CH4 for most of the time except summer to fall when net CH4 emissions occurred. We did not detect any elevated CO2 effects on CH4 fluxes, but emissions were difficult to quantify due to their discontinuous nature, most likely because of ebullition from the saturated zone. Potential methanotrophic activity, determined by incubation of fresh sieved soil under standardized conditions, also did not reveal any effect of the CO2 treatment. Finally, we determined the spatial micro-distribution of methanotrophic activity at less than 5× atmospheric (10 ppm) and elevated (10000 ppm) CH4 concentrations, using a novel auto-radiographic technique. These analyses indicated that domains of net CH4 assimilation were distributed throughout the analyzed top 15 cm of soils, with no dependence on CH4 concentration or CO2 treatment. Our investigations suggest that elevated CO2 exerts no or only minor effects on CH4 fluxes in the type of ecosystem we studied, at least as long as soil moisture differences are small or absent as was the case here. The autoradiographic analyses further indicate that the spatial niche of CH4 oxidation does not shift in response to CO2 enrichment or CH4 concentration, and that the same type of methanotrophs may oxidize CH4 from atmospheric and soil-internal sources.

  8. Effects of elevated atmospheric CO2, prolonged summer drought and temperature increase on N2O and CH4 fluxes in a temperate heathland

    DEFF Research Database (Denmark)

    Carter, Mette Sustmann; Ambus, Per; Albert, Kristian Rost

    2011-01-01

    In temperate regions, climate change is predicted to increase annual mean temperature and intensify the duration and frequency of summer droughts, which together with elevated atmospheric carbon dioxide (CO2) concentrations, may affect the exchange of nitrous oxide (N2O) and methane (CH4) between...... terrestrial ecosystems and the atmosphere. We report results from the CLIMAITE experiment, where the effects of these three climate change parameters were investigated solely and in all combinations in a temperate heathland. Field measurements of N2O and CH4 fluxes took place 1–2 years after the climate...... change manipulations were initiated. The soil was generally a net sink for atmospheric CH4. Elevated temperature (T) increased the CH4 uptake by on average 10 μg C m−2 h−1, corresponding to a rise in the uptake rate of about 20%. However, during winter elevated CO2 (CO2) reduced the CH4 uptake, which...

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

    Science.gov (United States)

    Yu, Song; Bo, Jiang; Jiahong, Li

    2017-09-16

    The mechanism for the competitive adsorption of CH 4 and CO 2 on coal vitrinite (DV-8, maximum vitrinite reflectance R o,max  = 0.58%) was revealed through simulation and experimental methods. A saturated state was reached after absorbing 17 CH 4 or 22 CO 2 molecules per DV-8 molecule. The functional groups (FGs) on the surface of the vitrinite can be ranked in order of decreasing CH 4 and CO 2 adsorption ability as follows: [-CH 3 ] > [-C=O] > [-C-O-C-] > [-COOH] and [-C-O-C-] > [-C=O] > [-CH 3 ] > [-COOH]. CH 4 and CO 2 distributed as aggregations and they were both adsorbed at the same sites on vitrinite, indicating that CO 2 can replace CH 4 by occupying the main adsorption sites for CH 4 -vitrinite. High temperatures are not conducive to the adsorption of CH 4 and CO 2 on vitrinite. According to the results of density functional theory (DFT) and grand canonical Monte Carlo (GCMC) calculations, vitrinite has a higher adsorption capacity for CO 2 than for CH 4 , regardless of whether a single-component or binary adsorbate is considered. The equivalent adsorption heat (EAH) of CO 2 -vitrinite (23.02-23.17) is higher than that of CH 4 -vitrinite (9.04-9.40 kJ/mol). The EAH of CO 2 -vitrinite decreases more rapidly with increasing temperature than the EAH of CH 4 -vitrinite does, indicating in turn that the CO 2 -vitrinite bond weakens more quickly with increasing temperature than the CH 4 -vitrinite bond does. Simulation data were found to be in good accord with the corresponding experimental results.

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

    Science.gov (United States)

    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.

  11. Influence of meteorology and interrelationship with greenhouse gases (CO2 and CH4) at a sub-urban site of India

    Science.gov (United States)

    Sreenivas, G.; Mahesh, P.; Subin, J.; Kanchana, A. L.; Rao, P. V. N.; Dadhwal, V. K.

    2015-12-01

    Atmospheric greenhouse gases (GHGs) such as carbon dioxide (CO2) and methane (CH4) are important climate forcing agents due to their significant impact on the climate system. The present study brings out first continuous measurements of atmospheric GHG's using high precision Los Gatos Research's-greenhouse gas analyser (LGR-GGA) over Shadnagar, a suburban site of Central India during the period 2014. The annual mean of CO2 and CH4 over the study region is found to be 394 ± 2.92 and 1.92 ± 0.07 ppm (mean, μ ± 1 SD, σ) respectively. CO2 and CH4 showed a significant seasonal variation during the study period with maximum (minimum) CO2 observed during Pre-monsoon (Monsoon), while CH4 recorded maximum during post-monsoon and minimum in monsoon. A consistent diurnal mixing ratio of these gases is observed with high (low) during night (afternoon) hours throughout the study period. Influences of prevailing meteorology (air temperature, wind speed, wind direction and relative humidity) on GHG's have also been investigated. CO2 and CH4 showed a strong positive correlation during winter, pre-monsoon, monsoon and post-monsoon with R equal to 0.80, 0.80, 0.61 and 0.72 respectively. It implies the seasonal variations in source-sink mechanisms of CO2 and CH4. Present study also confirms implicitly the presence OH radicals as a major sink of CH4 over the study region.

  12. Stable isotope ratios of the atmospheric CH4, CO2 and N2O in Tokai-mura

    International Nuclear Information System (INIS)

    Porntepkasemsan, Boonsom; Andoh, Mariko A.; Amano, Hikaru

    2000-11-01

    This report presents the results and interpretation of stable isotope ratios of the atmospheric CH 4 , CO 2 and N 2 O from a variety of sources in Tokai-mura. The seasonal changes of δ 13 CH 4 , δ 13 CO 2 and δ 15 N 2 O were determined under in-situ conditions in four sampling sites and one control site. Such measurements are expected to provide a useful means of estimating the transport mechanisms of the three trace gases in the environment. These isotopic signatures were analyzed by Isotope Ratio Mass Spectrometer (IRMS, Micromass Isoprime). Our data showed the significant seasonal fluctuation in the Hosoura rice paddy during the entire growing season in 1999. Possible causes for the variation are postulated. Additional measurements on soil properties and on organic δ 13 C in rice plant are suggested. Cited outstanding original papers are summarized in the references. (author)

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

    KAUST Repository

    Al-Sabban, Bedour E.; Falivene, Laura; Kozlov, Sergey M.; Aguilar Tapia, Antonio; Ould-Chikh, Samy; Hazemann, Jean-Louis; Cavallo, Luigi; Basset, Jean-Marie; Takanabe, Kazuhiro

    2017-01-01

    Dry reforming of methane (DRM) proceeds via CH4 decomposition to leave surface carbon species, followed by their removal with CO2-derived species. Reactivity tuning for stoichiometric CH4/CO2 reactants was attempted by alloying the non-noble metals

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

    Science.gov (United States)

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

    2016-07-01

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

  15. Temporal and spatial variations of soil CO2, CH4 and N2O fluxes at three differently managed grasslands

    Directory of Open Access Journals (Sweden)

    D. Imer

    2013-09-01

    Full Text Available A profound understanding of temporal and spatial variabilities of soil carbon dioxide (CO2, methane (CH4 and nitrous oxide (N2O fluxes between terrestrial ecosystems and the atmosphere is needed to reliably quantify these fluxes and to develop future mitigation strategies. For managed grassland ecosystems, temporal and spatial variabilities of these three soil greenhouse gas (GHG fluxes occur due to changes in environmental drivers as well as fertilizer applications, harvests and grazing. To assess how such changes affect soil GHG fluxes at Swiss grassland sites, we studied three sites along an altitudinal gradient that corresponds to a management gradient: from 400 m a.s.l. (intensively managed to 1000 m a.s.l. (moderately intensive managed to 2000 m a.s.l. (extensively managed. The alpine grassland was included to study both effects of extensive management on CH4 and N2O fluxes and the different climate regime occurring at this altitude. Temporal and spatial variabilities of soil GHG fluxes and environmental drivers on various timescales were determined along transects of 16 static soil chambers at each site. All three grasslands were N2O sources, with mean annual soil fluxes ranging from 0.15 to 1.28 nmol m−2 s−1. Contrastingly, all sites were weak CH4 sinks, with soil uptake rates ranging from −0.56 to −0.15 nmol m−2 s−1. Mean annual soil and plant respiration losses of CO2, measured with opaque chambers, ranged from 5.2 to 6.5 μmol m−2 s−1. While the environmental drivers and their respective explanatory power for soil N2O emissions differed considerably among the three grasslands (adjusted r2 ranging from 0.19 to 0.42, CH4 and CO2 soil fluxes were much better constrained (adjusted r2 ranging from 0.46 to 0.80 by soil water content and air temperature, respectively. Throughout the year, spatial heterogeneity was particularly high for soil N2O and CH4 fluxes. We found permanent hot spots for soil N2O emissions as well as

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

    Directory of Open Access Journals (Sweden)

    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.

  17. The Influence of Climate Change on CO2 and CH4 Concentration Near Closed Shaft - Numerical Simulations

    Science.gov (United States)

    Wrona, Paweł

    2017-09-01

    Given the scientific consensus pointing to climate change, the more extreme weather events associated with this will lead to deeper pressure drops. As has already been stated, pressure drops are the main cause of gas flow from underground sites to the surface. This article presents the results of numerical simulations of the change in distribution of CO2 and CH4 near a closed mining shaft under the predicted baric tendency. Simulations have been undertaken by means of the FDS software package with the Pyrosim graphical interface - a CFD tool for fire and ventilation analysis. Assumptions have been based on previous results of in-situ measurements. The results (determined for a height of 1m above the ground) were compared to the following levels (later in the text comparison levels): for CO2 0.1%vol. according to Pettenkoffer's scale and 2.5%vol. for CH4 as the half of Lower Explosive Limit (LEL). The results show that the deeper baric drops anticipated could lead to a wider spread of both greenhouse gases in the vicinity of the shaft, especially along the prevailing wind direction. According to the results obtained, CO2 and CH4 with concentrations above their comparison levels are expected at a distance greater than 50m from the shaft when wind is present for CO2 and at a distance of 4.5m for CH4. Subsequent analysis of the results enabled the determination of functions for describing the concentration of gases along the wind direction line under the projected pressure drop. The results relate to a particular case, although the model could easily be modified to any other example of gas emissions from underground sites.

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

    Science.gov (United States)

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

    2017-12-01

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

  19. Automated CO2, CH4 and N2O Fluxes from Tree Stems and Soils: Magnitudes, Temporal Patterns and Drivers

    Science.gov (United States)

    Barba, J.; Poyatos, R.; Vargas, R.

    2017-12-01

    The emissions of the main greenhouse gases (GHG; CO2, CH4 and N2O) through tree stems are still an uncertain component of the total GHG balance of forests. Despite that stem CO2 emissions have been studied for several decades, it is still unclear the drivers and spatiotemporal patterns of CH4 and N2O stem emissions. Additionally, it is unknown how stem emissions could be related to soil physiological processes or environmental conditions. We measured CO2, CH4 and N2O emissions hourly from April to July 2017 at two different heights (75 [LStem] and 150cm [HStem]) of bitternut hickory (Carya cordiformis) trees and adjacent soil locations in a forested area in the Mid Atlantic of the USA. We designed an automated system to continuously measure the three greenhouse gases (GHG) in stems and soils. Stem and soil CO2 emissions showed similar seasonal patterns with an average of 6.56±0.09 (soil), 3.72±0.05 (LStem) and 2.47±0.04 µmols m-2 s-1 (HStem) (mean±95% CI). Soil temperature controlled CO2 fluxes at both daily and seasonal scales (R2>0.5 for all cases), but there was no clear effect of soil moisture. The stems were a clear CH4 source with emissions decreasing with height (0.35±0.02 and 0.25±0.01 nmols m-2 s-1 for LStem and HStem, respectively) with no apparent seasonal pattern, and no clear relationship with environmental drivers (e.g., temperature, moisture). In contrast, soil was a CH4 sink throughout the experiment (-0.55±0.02 nmols m-2 s-1) and its seasonal pattern responded to moisture changes. Despite soil and stem N2O emissions did not show a seasonal pattern or apparent dependency on temperature or moisture, they showed net N2O emissions with a decrease in emissions with stem height (0.29±0.05 for soil, 0.38±0.06 for LStem and 0.28±0.05 nmols m-2 s-1 for HStem). The three GHG emissions decreased with stem height at similar rates (33%, 28% and 27% for CO2, CH4 and N2O, respectively). These results suggest that the gases were not produced in the stem

  20. CO2CH4 permeation in high zeolite 4A loading mixed matrix membranes

    KAUST Repository

    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.

  1. CO2CH4 permeation in high zeolite 4A loading mixed matrix membranes

    KAUST Repository

    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.

  2. Remote sensing of CO2 and CH4 using solar absorption spectrometry with a low resolution spectrometer

    Directory of Open Access Journals (Sweden)

    J. Notholt

    2012-07-01

    Full Text Available Throughout the last few years solar absorption Fourier Transform Spectrometry (FTS has been further developed to measure the total columns of CO2 and CH4. The observations are performed at high spectral resolution, typically at 0.02 cm−1. The precision currently achieved is generally better than 0.25%. However, these high resolution instruments are quite large and need a dedicated room or container for installation. We performed these observations using a smaller commercial interferometer at its maximum possible resolution of 0.11 cm−1. The measurements have been performed at Bremen and have been compared to observations using our high resolution instrument also situated at the same location. The high resolution instrument has been successfully operated as part of the Total Carbon Column Observing Network (TCCON. The precision of the low resolution instrument is 0.32% for XCO2 and 0.46% for XCH4. A comparison of the measurements of both instruments yields an average deviation in the retrieved daily means of ≤0.2% for CO2. For CH4 an average bias between the instruments of 0.47% was observed. For test cases, spectra recorded by the high resolution instrument have been truncated to the resolution of 0.11 cm−1. This study gives an offset of 0.03% for CO2 and 0.26% for CH4. These results indicate that for CH4 more than 50% of the difference between the instruments results from the resolution dependent retrieval. We tentatively assign the offset to an incorrect a-priori concentration profile or the effect of interfering gases, which may not be treated correctly.

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

    Czech Academy of Sciences Publication Activity Database

    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. In situ measurements of H2O, CH4 and CO2 in the upper troposphere and the lower stratosphere (UT-LS) with the baloonborne picoSDLA and AMULSE tunable diode laser spectrometers during the 2014 and 2015 "Stratoscience" campaigns

    Science.gov (United States)

    Miftah-El-Khair, Zineb; Joly, Lilian; Decarpenterie, Thomas; Cousin, Julien; Dumelié, Nicolas; Grouiez, Bruno; Albo, Grégory; Chauvin, Nicolas; Maamary, Rabih; Amarouche, Nadir; Durry, Georges

    2016-04-01

    H2O, CH4 and CO2 are major greenhouse gases with a strong impact on climate. The concentrations of CO2 and CH4 have dramatically increased since the beginning of the industrialization era due to anthropogenic activities, contributing thereby to the global warming. Anthropogenic activities as fossil fuels, ruminant, and biomass burning constitute the major sources of carbon dioxide and methane. The increase of H2O concentration in the stratosphere could cause a cooling of this atmospheric region, impacting the recovery of the ozone layer. Therefore, having information and data about the vertical distribution of H2O, CO2 and CH4 is very useful to improve our knowledge of the future of our climate. We have developed, with the help of French space agency (CNES) and CNRS, two laser diode sensors PicoSDLA and AMULSE devoted to the in situ measurements of H2O, CH4 and CO2 from balloon platforms. These instruments were operated from open stratospheric balloons in Timmins, CA, in August 2014 and 2015. We report and discuss the instrumental achievements of both sensors during these flights in the UT-LS. Aknowledgments: The authors acknowledge financial supports from CNES, CNRS and the region Champagne-Ardenne.

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

    KAUST Repository

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

    DEFF Research Database (Denmark)

    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....

  7. A Year in the Life: Annual Patterns of CO2 and CH4 from a Northern Finland Peatland, Including Anaerobic Methane Oxidation and Summer Ebullition Rates

    Science.gov (United States)

    Miller, K.; Lipson, D.; Biasi, C.; Dorodnikov, M.; Männistö, M.; Lai, C. T.

    2014-12-01

    The major ecological controls on methane (CH4) and carbon dioxide (CO2) fluxes in northern wetland systems are well known, yet estimates of source/sink magnitudes are often incongruous with measured rates. This mismatch persists because holistic flux datasets are rare, preventing 'whole picture' determinations of flux controls. To combat this, we measured net CO2 and CH4 fluxes from September 2012-2013 within a peatland in northern Lapland, Finland. In addition, we performed in situ manipulations and in vitro soil incubations to quantify anaerobic methane oxidation and methanogenic rates as they related to alternative electron acceptor availability. Average annual fluxes varied substantially between different depressions within the wetland, a pattern that persisted through all seasons. Season was a strong predictor of both CO2 and CH4 flux rates, yet CH4 rates were not related to melt-season 10cm or 30cm soil temperatures, and only poorly predicted with air temperatures. We found evidence for both autumnal and spring thaw CH4 bursts, collectively accounting for 26% of annual CH4 flux, although the autumnal burst was more than 5 fold larger than the spring burst. CH4 ebullition measured throughout the growing season augmented the CH4 source load by a factor of 1.5, and was linked with fine-scale spatial heterogeneity within the wetland. Surprisingly, CH4 flux rates were insensitive to Fe(III) and humic acid soil amendments, both of which amplified CO2 fluxes. Using in vitro incubations, we determined anaerobic methane oxidation and methanogenesis rates. Measured anaerobic oxidation rates showed potential consumption of between 6-39% of the methane produced, contributing approximately 1% of total carbon dioxide flux. Treatments of nitrate, sulfate and ferric iron showed that nitrate suppressed methanogenesis, but were not associated with anaerobic oxidation rates.

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

    KAUST Repository

    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

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

    Science.gov (United States)

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

    2018-04-01

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

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

    KAUST Repository

    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

  11. Mathematical Modelling of Arctic Polygonal Tundra with Ecosys: 2. Microtopography Determines How CO2 and CH4 Exchange Responds to Changes in Temperature and Precipitation

    Science.gov (United States)

    Grant, R. F.; Mekonnen, Z. A.; Riley, W. J.; Arora, B.; Torn, M. S.

    2017-12-01

    Differences of surface elevation in arctic polygonal landforms cause spatial variation in soil water contents (θ), active layer depths (ALD), and thereby in CO2 and CH4 exchange. Here we test hypotheses in ecosys for topographic controls on CO2 and CH4 exchange in trough, rim, and center features of low- and flat-centered polygons (LCP and FCP) against chamber and eddy covariance (EC) measurements during 2013 at Barrow, Alaska. Larger CO2 influxes and CH4 effluxes were measured with chambers and modeled with ecosys in LCPs than in FCPs and in lower features (troughs) than in higher (rims) within LCPs and FCPs. Spatially aggregated CO2 and CH4 fluxes from ecosys were significantly correlated with EC flux measurements. Lower features were modeled as C sinks (52-56 g C m-2 yr-1) and CH4 sources (4-6 g C m-2 yr-1), and higher features as near C neutral (-2-15 g C m-2 yr-1) and CH4 neutral (0.0-0.1 g C m-2 yr-1). Much of the spatial and temporal variations in CO2 and CH4 fluxes were modeled from topographic effects on water and snow movement and thereby on θ, ALD, and soil O2 concentrations. Model results forced with meteorological data from 1981 to 2015 indicated increasing net primary productivity in higher features and CH4 emissions in some lower and higher features since 2008, attributed mostly to recent rises in precipitation. Small-scale variation in surface elevation causes large spatial variation of greenhouse gas (GHG) exchanges and therefore should be considered in estimates of GHG exchange in polygonal landscapes.

  12. Design and performance of a Nafion dryer for continuous operation at CO2 and CH4 air monitoring sites

    Directory of Open Access Journals (Sweden)

    L. R. Welp

    2013-05-01

    Full Text Available In preparation for routine deployment in a network of greenhouse gas monitoring stations, we have designed and tested a simple method for drying ambient air to near or below 0.2% (2000 ppm mole fraction H2O using a Nafion dryer. The inlet system was designed for use with cavity ring-down spectrometer (CRDS analyzers such as the Picarro model G2301 that measure H2O in addition to their principal analytes, in this case CO2 and CH4. These analyzers report dry-gas mixing ratios without drying the sample by measuring H2O mixing ratio at the same frequency as the main analytes, and then correcting for the dilution and peak broadening effects of H2O on the mixing ratios of the other analytes measured in moist air. However, it is difficult to accurately validate the water vapor correction in the field. By substantially lowering the amount of H2O in the sample, uncertainties in the applied water vapor corrections can be reduced by an order of magnitude or more, thus eliminating the need to determine instrument-specific water vapor correction coefficients and to verify the stability over time. Our Nafion drying inlet system takes advantage of the extra capacity of the analyzer pump to redirect 30% of the dry gas exiting the Nafion to the outer shell side of the dryer and has no consumables. We tested the Nafion dryer against a cryotrap (−97 °C method for removing H2O and found that in wet-air tests, the Nafion reduces the CO2 dry-gas mixing ratios of the sample gas by as much as 0.1 ± 0.01 ppm due to leakage across the membrane. The effect on CH4 was smaller and varied within ± 0.2 ppb, with an approximate uncertainty of 0.1 ppb. The Nafion-induced CO2 bias is partially offset by sending the dry reference gases through the Nafion dryer as well. The residual bias due to the impact of moisture differences between sample and reference gas on the permeation through the Nafion was approximately −0.05 ppm for CO2 and varied within ± 0.2 ppb for CH4. The

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

    Science.gov (United States)

    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

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

    DEFF Research Database (Denmark)

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

    2014-01-01

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

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

    International Nuclear Information System (INIS)

    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%

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

    International Nuclear Information System (INIS)

    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

  17. Glycine formation in CO2:CH4:NH3 ices induced by 0-70 eV electrons

    Science.gov (United States)

    Esmaili, Sasan; Bass, Andrew D.; Cloutier, Pierre; Sanche, Léon; Huels, Michael A.

    2018-04-01

    Glycine (Gly), the simplest amino-acid building-block of proteins, has been identified on icy dust grains in the interstellar medium, icy comets, and ice covered meteorites. These astrophysical ices contain simple molecules (e.g., CO2, H2O, CH4, HCN, and NH3) and are exposed to complex radiation fields, e.g., UV, γ, or X-rays, stellar/solar wind particles, or cosmic rays. While much current effort is focused on understanding the radiochemistry induced in these ices by high energy radiation, the effects of the abundant secondary low energy electrons (LEEs) it produces have been mostly assumed rather than studied. Here we present the results for the exposure of multilayer CO2:CH4:NH3 ice mixtures to 0-70 eV electrons under simulated astrophysical conditions. Mass selected temperature programmed desorption (TPD) of our electron irradiated films reveals multiple products, most notably intact glycine, which is supported by control measurements of both irradiated or un-irradiated binary mixture films, and un-irradiated CO2:CH4:NH3 ices spiked with Gly. The threshold of Gly formation by LEEs is near 9 eV, while the TPD analysis of Gly film growth allows us to determine the "quantum" yield for 70 eV electrons to be about 0.004 Gly per incident electron. Our results show that simple amino acids can be formed directly from simple molecular ingredients, none of which possess preformed C—C or C—N bonds, by the copious secondary LEEs that are generated by ionizing radiation in astrophysical ices.

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

    Science.gov (United States)

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

    2013-12-01

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

  19. Comparison of chamber and eddy covariance-based CO2 and CH4 emission estimates in a heterogeneous grass ecosystem on peat

    International Nuclear Information System (INIS)

    Schrier-Uijl, A.P.; Berendse, F.; Veenendaal, E.M.; Kroon, P.S.; Hensen, A.; Leffelaar, P.A.

    2010-08-01

    Fluxes of methane (CH4) and carbon dioxide (CO2) estimated by empirical models based on small-scale chamber measurements were compared to large-scale eddy covariance (EC) measurements for CH4 and to a combination of EC measurements and EC-based models for CO2. The experimental area was a flat peat meadow in the Netherlands with heterogeneous source strengths for both greenhouse gases. Two scenarios were used to assess the importance of stratifying the landscape into landscape elements before up-scaling the fluxes measured by chambers to landscape scale: one took the main landscape elements into account (field, ditch edge ditch), the other took only the field into account. Non-linear regression models were used to up-scale the chamber measurements to field emission estimates. EC CO2 respiration consisted of measured night time EC fluxes and modeled day time fluxes using the Arrhenius model. EC CH4 flux estimate was based on daily averages and the remaining data gaps were filled by linear interpolation. The EC and chamber-based estimates agreed well when the three landscape elements were taken into account with 16.5% and 13.0% difference for CO2 respiration and CH4, respectively. However, both methods differed 31.0% and 55.1% for CO2 respiration and CH4 when only field emissions were taken into account when up-scaling chamber measurements to landscape scale. This emphasizes the importance of stratifying the landscape into landscape elements. The conclusion is that small-scale chamber measurements can be used to estimate fluxes of CO2 and CH4 at landscape scale if fluxes are scaled by different landscape elements.

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

    Science.gov (United States)

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

    2015-04-01

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

  1. Trapping of CH4, CO, and CO2 in Amorphous Water Ice

    Science.gov (United States)

    Mastrapa, R. M. E.; Brown, R. H.; Anicich, V. G.; Cohen, B. A.; Dai, W.; Lunine, J. I.

    1999-09-01

    In this study, CO, CH4, and CO2 were trapped in H2O at temperatures as low as 20 K and pressures between 10-5 and 10-8 Torr. IR spectra were taken of each sample before sublimation to confirm the presence of volatiles. The samples were then heated at rates from 0.25 K/min to 1 K/min and the escape ranges were measured with a mass spectrometer. The volatiles escaped from the ice mixtures in temperature ranges similar to those found in previous work (1, 2, 3), namely 48-52 K, 145-160 K, 170-185 K. H2O is released from 150 K to 185 K. However, the temperature range of escape is strongly dependent on deposition temperature and heating rate. If the deposition temperature is below the point where the solid volatile rapidly sublimates in the ambient environment of our experiment, then the first range of volatile escape is centered around it's sublimation point, and there is little of the volatile remaining from 170-185 K. The location of the third escape range shifts to lower temperatures with slower sublimation rate. It was determined that 0.5 K/min is the ideal sample heating rate to determine these escape ranges. In our data, the infrared spectrum of CO trapped in water ice shows a splitting of the 2145 cm-1 solid CO line into two bands at 2343 cm-1 and 2135 cm-1. These shifts are similar to those seen by Sandford, et al. (4). (1) Bar-Nun, A., G. Herman, D. Laufer, and M. L. Rappaport, (1985), Icarus, 63, 317-332. (2) Bar-Nun, A., J. Dror, E. Kochavi, and D. Laufer, (1987), Physical Review B, 35, no. 5, 2427-2435. (3) Hudson, R. L., and B. Donn, (1991), Icarus, 94, 326-332. (4) Sandford, S. A., L. J. Allamandola, A. G. G. M. Tielens, and G. J. Valero, (1988), Astrophysical Journal, 329, 498-510.

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

    Science.gov (United States)

    Jacotot, Adrien; Marchand, Cyril; Allenbach, Michel

    2018-08-01

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

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

    Science.gov (United States)

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

    2015-12-01

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

  4. CO2, CH4 and N2O fluxes from soil of a burned grassland in Central Africa

    Directory of Open Access Journals (Sweden)

    R. Valentini

    2010-11-01

    Full Text Available The impact of fire on soil fluxes of CO2, CH4 and N2O was investigated in a tropical grassland in Congo Brazzaville during two field campaigns in 2007–2008. The first campaign was conducted in the middle of the dry season and the second at the end of the growing season, respectively one and eight months after burning. Gas fluxes and several soil parameters were measured in each campaign from burned plots and from a close-by control area preserved from fire. Rain events were simulated at each campaign to evaluate the magnitude and duration of the generated gas flux pulses. In laboratory experiments, soil samples from field plots were analysed for microbial biomass, net N mineralization, net nitrification, N2O, NO and CO2 emissions under different water and temperature soil regimes. One month after burning, field CO2 emissions were significantly lower in burned plots than in the control plots, the average daily CH4 flux shifted from net emission in the unburned area to net consumption in burned plots, no significant effect of fire was observed on soil N2O fluxes. Eight months after burning, the average daily fluxes of CO2, CH4 and N2O measured in control and burned plots were not significantly different. In laboratory, N2O fluxes from soil of burned plots were significantly higher than fluxes from soil of unburned plots only above 70% of maximum soil water holding capacity; this was never attained in the field even after rain simulation. Higher NO emissions were measured in the lab in soil from burned plots at both 10% and 50% of maximum soil water holding capacity. Increasing the incubation temperature from 25 °C to 37 °C negatively affected microbial growth, mineralization and nitrification activities but enhanced N2O and CO2 production. Results indicate that fire did not increase post-burning soil GHG emissions in this tropical grasslands characterized by acidic, well drained and nutrient-poor soil.

  5. The predominance of young carbon in Arctic whole-lake CH4 and CO2 emissions and implications for Boreal yedoma lakes.

    Science.gov (United States)

    Elder, C.; Xu, X.; Walker, J. C.; Walter Anthony, K. M.; Pohlman, J.; Arp, C. D.; Townsend-Small, A.; Hinkel, K. M.; Czimczik, C. I.

    2017-12-01

    Lakes in Arctic and Boreal regions are hotspots for atmospheric exchange of the greenhouse gases CO2 and CH4. Thermokarst lakes are a subset of these Northern lakes that may further accelerate climate warming by mobilizing ancient permafrost C (> 11,500 years old) that has been disconnected from the active C cycle for millennia. Northern lakes are thus potentially powerful agents of the permafrost C-climate feedback. While they are critical for projecting the magnitude and timing these feedbacks from the rapidly warming circumpolar region, we lack datasets capturing the diversity of northern lakes, especially regarding their CH4contributions to whole-lake C emissions and their ability to access and mobilize ancient C. We measured the radiocarbon (14C) ages of CH4 and CO2 emitted from 60 understudied lakes and ponds in Arctic and Boreal Alaska during winter and summer to estimate the ages of the C sources yielding these gases. Integrated mean ages for whole-lake emissions were inferred from the 14C-age of dissolved gases sampled beneath seasonal ice. Additionally, we measured concentrations and 14C values of gases emitted by ebullition and diffusion in summer to apportion C emission pathways. Using a multi-sourced mass balance approach, we found that whole-lake CH4 and CO2 emissions were predominantly sourced from relatively young C in most lakes. In Arctic lakes, CH4 originated from 850 14C-year old C on average, whereas dissolved CO2 was sourced from 400 14C-year old C, and represented 99% of total dissolved C flux. Although ancient C had a minimal influence (11% of total emissions), we discovered that lakes in finer-textured aeolian deposits (Yedoma) emitted twice as much ancient C as lakes in sandy regions. In Boreal, yedoma-type lakes, CH4 and CO2 were fueled by significantly older sources, and mass balance results estimated CH4-ebullition to comprise 50-60% of whole-lake CH4 emissions. The mean 14C-age of Boreal emissions was 6,000 14C-years for CH4-C, and 2

  6. Development of differential absorption lidar (DIAL) for detection of CO2, CH4 and PM in Alberta

    Science.gov (United States)

    Wojcik, Michael; Crowther, Blake; Lemon, Robert; Valupadas, Prasad; Fu, Long; Leung, Bonnie; Yang, Zheng; Huda, Quamrul; Chambers, Allan

    2005-05-01

    Rapid expansion of the oil and gas industry in Alberta, including the oil sands, has challenged the Alberta Government to keep pace in its efforts to monitor and mitigate the environmental impacts of development. The limitations of current monitoring systems has pushed the provincial government to seek out advanced sensing technologies such as satellite imagery and laser based sensors. The Space Dynamics Laboratory (SDL) of Utah State University, in cooperation with Alberta Environmental Monitoring, Evaluation and Reporting Agency (AEMERA), has developed North America's first mobile differential absorption lidar (DIAL) system designed specifically for emissions measurement. This instrument is housed inside a 36' trailer which allows for mobility to travel across Alberta to characterize source emissions and to locate fugitive leaks. DIAL is capable of measuring concentrations for carbon dioxide (CO2) and methane (CH4) at ranges of up to 3 km with a spatial resolution of 10 meters. DIAL can map both CO2 and CH4, as well as particulate matter (PM) in a linear fashion; by scanning the laser beam in both azimuth and elevation DIAL can create images of emissions in two dimensions. DIAL imagery may be used to understand and control production practices, characterize source emissions, determine emission factors, locate fugitive leaks, assess plume dispersion, and confirm air dispersion modeling. A system overview of the DIAL instrument and some representative results will be discussed.

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

    Science.gov (United States)

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

    2014-12-01

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

  8. Soil-atmospheric exchange of CO2, CH4, and N2O in three subtropical forest ecosystems in southern China

    Science.gov (United States)

    Tang, X.; Liu, S.; Zhou, G.; Zhang, Dongxiao; Zhou, C.

    2006-01-01

    The magnitude, temporal, and spatial patterns of soil-atmospheric greenhouse gas (hereafter referred to as GHG) exchanges in forests near the Tropic of Cancer are still highly uncertain. To contribute towards an improvement of actual estimates, soil-atmospheric CO2, CH4, and N2O fluxes were measured in three successional subtropical forests at the Dinghushan Nature Reserve (hereafter referred to as DNR) in southern China. Soils in DNR forests behaved as N2O sources and CH4 sinks. Annual mean CO2, N2O, and CH4 fluxes (mean ?? SD) were 7.7 ?? 4.6MgCO2-Cha-1 yr-1, 3.2 ?? 1.2 kg N2ONha-1 yr-1, and 3.4 ?? 0.9 kgCH4-Cha-1 yr-1, respectively. The climate was warm and wet from April through September 2003 (the hot-humid season) and became cool and dry from October 2003 through March 2004 (the cool-dry season). The seasonality of soil CO2 emission coincided with the seasonal climate pattern, with high CO2 emission rates in the hot-humid season and low rates in the cool-dry season. In contrast, seasonal patterns of CH4 and N2O fluxes were not clear, although higher CH4 uptake rates were often observed in the cool-dry season and higher N2O emission rates were often observed in the hot-humid season. GHG fluxes measured at these three sites showed a clear increasing trend with the progressive succession. If this trend is representative at the regional scale, CO2 and N2O emissions and CH4 uptake in southern China may increase in the future in light of the projected change in forest age structure. Removal of surface litter reduced soil CO2 effluxes by 17-44% in the three forests but had no significant effect on CH4 absorption and N2O emission rates. This suggests that microbial CH4 uptake and N2O production was mainly related to the mineral soil rather than in the surface litter layer. ?? 2006 Blackwell Publishing Ltd.

  9. A Modern Automatic Chamber Technique as a Powerful Tool for CH4 and CO2 Flux Monitoring

    Science.gov (United States)

    Mastepanov, M.; Christensen, T. R.; Lund, M.; Pirk, N.

    2014-12-01

    A number of similar systems were used for monitoring of CH4 and CO2 exchange by the automatic chamber method in a range of different ecosystems. The measurements were carried out in northern Sweden (mountain birch forest near Abisko, 68°N, 2004-2010), southern Sweden (forest bog near Hässleholm, 56°N, 2007-2014), northeastern Greenland (arctic fen in Zackenberg valley, 74°N, 2005-2014), southwestern Greenland (fen near Nuuk, 64°N, 2007-2014), central Svalbard (arctic fen near Longyearbyen, 78°N, 2011-2014). Those in total 37 seasons of measurements delivered not only a large amount of valuable flux data, including a few novel findings (Mastepanov et al., Nature, 2008; Mastepanov et al., Biogeosciences, 2013), but also valuable experience with implementation of the automatic chamber technique using modern analytical instruments and computer technologies. A range of high resolution CH4 analysers (DLT-100, FMA, FGGA - Los Gatos Research), CO2 analyzers (EGM-4, SBA-4 - PP Systems; Li-820 - Li-Cor Biosciences), as well as Methane Carbon Isotope Analyzer (Los Gatos Research) has shown to be suitable for precise measurements of fluxes, from as low as 0.1 mg CH4 m-1 d-1 (wintertime measurements at Zackenberg, unpublished) to as high as 2.4 g CH4 m-1 d-1 (autumn burst 2007 at Zackenberg, Mastepanov et al., Nature, 2008). Some of these instruments had to be customized to accommodate 24/7 operation in harsh arctic conditions. In this presentation we will explain some of these customizations. High frequency of concentration measurements (1 Hz in most cases) provides a unique opportunity for quality control of flux calculations; on the other hand, this enormous amount of data can be analyzed only using highly automated algorithms. A specialized software package was developed and improved through the years of measurements and data processing. This software automates the data flow from raw concentration data of different instruments and sensors and various status records

  10. Vehicle emissions of greenhouse gases and related tracers from a tunnel study: : CO: CO2, N2O: CO2, CH4: CO2, O2: CO2 ratios, and the stable isotopes 13C and 18O in CO2 and CO

    NARCIS (Netherlands)

    Popa, Maria Elena; Vollmer, M. K.; Jordan, A.; Brand, W. A.; Pathirana, S. L.; Rothe, M.; Röckmann, T.

    2014-01-01

    Measurements of CO2, CO, N2O and CH4 mole fractions, O2/N2 ratios and the stable isotopes 13C and 18O in CO2 and CO have been performed in air samples from the Islisberg highway tunnel (Switzerland). The molar CO : CO2 ratios, with an average of (4.15 ± 0.34) ppb:ppm, are lower than reported in

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

    Science.gov (United States)

    P. J. Hanson; A. L. Gill; X. Xu; J. R. Phillips; D. J. Weston; Randy Kolka; J. S. Riggs; L. A. Hook

    2016-01-01

    Peatland measurements of CO2 and CH4 flux were obtained at scales appropriate to the in situ biological community below the tree layer to demonstrate representativeness of the spruce and peatland responses under climatic and environmental change (SPRUCE) experiment. Surface flux measurements were made using dual open-path...

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

    Science.gov (United States)

    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).

  13. Air-sea fluxes of CO2 and CH4 from the Penlee Point Atmospheric Observatory on the south-west coast of the UK

    Science.gov (United States)

    Yang, Mingxi; Bell, Thomas G.; Hopkins, Frances E.; Kitidis, Vassilis; Cazenave, Pierre W.; Nightingale, Philip D.; Yelland, Margaret J.; Pascal, Robin W.; Prytherch, John; Brooks, Ian M.; Smyth, Timothy J.

    2016-05-01

    We present air-sea fluxes of carbon dioxide (CO2), methane (CH4), momentum, and sensible heat measured by the eddy covariance method from the recently established Penlee Point Atmospheric Observatory (PPAO) on the south-west coast of the United Kingdom. Measurements from the south-westerly direction (open water sector) were made at three different sampling heights (approximately 15, 18, and 27 m above mean sea level, a.m.s.l.), each from a different period during 2014-2015. At sampling heights ≥ 18 m a.m.s.l., measured fluxes of momentum and sensible heat demonstrate reasonable ( ≤ ±20 % in the mean) agreement with transfer rates over the open ocean. This confirms the suitability of PPAO for air-sea exchange measurements in shelf regions. Covariance air-sea CO2 fluxes demonstrate high temporal variability. Air-to-sea transport of CO2 declined from spring to summer in both years, coinciding with the breakdown of the spring phytoplankton bloom. We report, to the best of our knowledge, the first successful eddy covariance measurements of CH4 emissions from a marine environment. Higher sea-to-air CH4 fluxes were observed during rising tides (20 ± 3; 38 ± 3; 29 ± 6 µmole m-2 d-1 at 15, 18, 27 m a.m.s.l.) than during falling tides (14 ± 2; 22 ± 2; 21 ± 5 µmole m-2 d-1), consistent with an elevated CH4 source from an estuarine outflow driven by local tidal circulation. These fluxes are a few times higher than the predicted CH4 emissions over the open ocean and are significantly lower than estimates from other aquatic CH4 hotspots (e.g. polar regions, freshwater). Finally, we found the detection limit of the air-sea CH4 flux by eddy covariance to be 20 µmole m-2 d-1 over hourly timescales (4 µmole m-2 d-1 over 24 h).

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

    Science.gov (United States)

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

    2017-04-01

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

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

    Science.gov (United States)

    Forsberg, B. R.; Amaral, J. H.; Barbosa, P.; Kasper, D.; MacIntyre, S.; Cortes, A.; Sarmento, H.; Borges, A. V.; Melack, J. M.; Farjalla, V.

    2015-12-01

    The Amazon floodplain contains a variety of wetland environments which contribute CO2 and CH4 to the regional and global atmospheres. The partial pressure and emission of these greenhouse gases (GHGs) varies: 1) between habitats, 2) seasonally, as the characteristics these habitats changes and 3) diurnally, in response to diurnal stratification. In this study, we investigated the combined influence of these factors on the partial pressure and emission of GHGs in Lago Janauacá, a central Amazon floodplain lake (3o23' S; 60o18' O). All measurements were made between August of 2014 and April of 2015 at two different sites and in three distinct habitats: open water, flooded forest, flooded macrophytes. Concentrations of CO2 and CH4 in air were measured continuously with a cavity enhanced absorption spectrometer, Los Gatos Research´s Ultraportable Greenhouse Gas Analyzer (UGGA). Vertical profiles o pCO2 and pCH4 were measured using the UGGA connected to an electric pump and equilibrator. Diffusive surface emissions were estimated with the UGGA connected to a static floating chamber. To investigate the influence of vertical stratification and mixing on GHG partial pressure and emissions, a meteorological station and submersible sensor chain were deployed at each site. Meteorological sensors included wind speed and direction. The submersible chains included thermistors and oxygen sensors. Depth profiles of partial pressure and diffusive emissions for both CO2 and CH4 varied diurnally, seasonally and between habitats. Both pCO2 and pCH4 were consistently higher in bottom than surface waters with the largest differences occurring at high water when thermal stratification was most stable. Methane emissions and partial pressures were highest at low water while pCO2 and CO2 fluxes were highest during high water periods, with 35% of CO2 fluxes at low water being negative. The highest average surface value of pCO2 (5491 μatm), encountered during rising water, was ~3 times

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

    Directory of Open Access Journals (Sweden)

    Amanda eLawter

    2015-07-01

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

  17. Polygonal tundra geomorphological change in response to warming alters future CO2 and CH4 flux on the Barrow Peninsula.

    Science.gov (United States)

    Lara, Mark J; McGuire, A David; Euskirchen, Eugenie S; Tweedie, Craig E; Hinkel, Kenneth M; Skurikhin, Alexei N; Romanovsky, Vladimir E; Grosse, Guido; Bolton, W Robert; Genet, Helene

    2015-04-01

    The landscape of the Barrow Peninsula in northern Alaska is thought to have formed over centuries to millennia, and is now dominated by ice-wedge polygonal tundra that spans drained thaw-lake basins and interstitial tundra. In nearby tundra regions, studies have identified a rapid increase in thermokarst formation (i.e., pits) over recent decades in response to climate warming, facilitating changes in polygonal tundra geomorphology. We assessed the future impact of 100 years of tundra geomorphic change on peak growing season carbon exchange in response to: (i) landscape succession associated with the thaw-lake cycle; and (ii) low, moderate, and extreme scenarios of thermokarst pit formation (10%, 30%, and 50%) reported for Alaskan arctic tundra sites. We developed a 30 × 30 m resolution tundra geomorphology map (overall accuracy:75%; Kappa:0.69) for our ~1800 km² study area composed of ten classes; drained slope, high center polygon, flat-center polygon, low center polygon, coalescent low center polygon, polygon trough, meadow, ponds, rivers, and lakes, to determine their spatial distribution across the Barrow Peninsula. Land-atmosphere CO2 and CH4 flux data were collected for the summers of 2006-2010 at eighty-two sites near Barrow, across the mapped classes. The developed geomorphic map was used for the regional assessment of carbon flux. Results indicate (i) at present during peak growing season on the Barrow Peninsula, CO2 uptake occurs at -902.3 10(6) gC-CO2 day(-1) (uncertainty using 95% CI is between -438.3 and -1366 10(6) gC-CO2 day(-1)) and CH4 flux at 28.9 10(6) gC-CH4 day(-1) (uncertainty using 95% CI is between 12.9 and 44.9 10(6) gC-CH4 day(-1)), (ii) one century of future landscape change associated with the thaw-lake cycle only slightly alter CO2 and CH4 exchange, while (iii) moderate increases in thermokarst pits would strengthen both CO2 uptake (-166.9 10(6) gC-CO2 day(-1)) and CH4 flux (2.8 10(6) gC-CH4 day(-1)) with geomorphic change from low

  18. Polygonal tundra geomorphological change in response to warming alters future CO2 and CH4 flux on the Barrow Peninsula

    Science.gov (United States)

    Lara, Mark J.; McGuire, A. David; Euskirchen, Eugénie S.; Tweedie, Craig E.; Hinkel, Kenneth M.; Skurikhin, Alexei N.; Romanovsky, Vladimir E.; Grosse, Guido; Bolton, W. Robert; Genet, Helene

    2015-01-01

    The landscape of the Barrow Peninsula in northern Alaska is thought to have formed over centuries to millennia, and is now dominated by ice-wedge polygonal tundra that spans drained thaw-lake basins and interstitial tundra. In nearby tundra regions, studies have identified a rapid increase in thermokarst formation (i.e., pits) over recent decades in response to climate warming, facilitating changes in polygonal tundra geomorphology. We assessed the future impact of 100 years of tundra geomorphic change on peak growing season carbon exchange in response to: (i) landscape succession associated with the thaw-lake cycle; and (ii) low, moderate, and extreme scenarios of thermokarst pit formation (10%, 30%, and 50%) reported for Alaskan arctic tundra sites. We developed a 30 × 30 m resolution tundra geomorphology map (overall accuracy:75%; Kappa:0.69) for our ~1800 km² study area composed of ten classes; drained slope, high center polygon, flat-center polygon, low center polygon, coalescent low center polygon, polygon trough, meadow, ponds, rivers, and lakes, to determine their spatial distribution across the Barrow Peninsula. Land-atmosphere CO2 and CH4 flux data were collected for the summers of 2006–2010 at eighty-two sites near Barrow, across the mapped classes. The developed geomorphic map was used for the regional assessment of carbon flux. Results indicate (i) at present during peak growing season on the Barrow Peninsula, CO2 uptake occurs at -902.3 106gC-CO2 day−1(uncertainty using 95% CI is between −438.3 and −1366 106gC-CO2 day−1) and CH4 flux at 28.9 106gC-CH4 day−1(uncertainty using 95% CI is between 12.9 and 44.9 106gC-CH4 day−1), (ii) one century of future landscape change associated with the thaw-lake cycle only slightly alter CO2 and CH4 exchange, while (iii) moderate increases in thermokarst pits would strengthen both CO2uptake (−166.9 106gC-CO2 day−1) and CH4 flux (2.8 106gC-CH4 day−1) with geomorphic change from

  19. Pure- and Mixed-Gas Permeation Properties of Highly Selective and Plasticization Resistant Hydroxyl-Diamine-Based 6FDA Polyimides for CO2/CH4 Separation

    KAUST Repository

    Alaslai, Nasser Y.; Ghanem, Bader; Alghunaimi, Fahd; Litwiller, Eric; Pinnau, Ingo

    2016-01-01

    The effect of hydroxyl functionalization on the m-phenylene diamine moiety of 6FDA dianhydride-based polyimides was investigated for gas separation applications. Pure-gas permeability coefficients of He, H2, N2, O2, CH4, and CO2 were measured at 35 °C and 2 atm. The introduction of hydroxyl groups in the diamine moiety of 6FDA-diaminophenol (DAP) and 6FDA-diamino resorcinol (DAR) polyimides tightened the overall polymer structure due to increased charge transfer complex formation compared to unfunctionalized 6FDA-m-phenylene diamine (mPDA). The BET surface areas based on nitrogen adsorption of 6FDA-DAP (54 m2g−1) and of 6FDA-DAR (45 m2g−1) were ~18% and 32% lower than that of 6FDA-mPDA (66 m2g−1). 6FDA-mPDA had a pure-gas CO2 permeability of 14 Barrer and CO2/CH4 selectivity of 70. The hydroxyl-functionalized polyimides 6FDA-DAP and 6FDA-DAR exhibited very high pure-gas CO2/CH4 selectivities of 92 and 94 with moderate CO2 permeability of 11 and 8 Barrer, respectively. It was demonstrated that hydroxyl-containing polyimide membranes maintained very high CO2/CH4 selectivity (~ 75 at CO2 partial pressure of 10 atm) due to CO2 plasticization resistance when tested under high-pressure mixed-gas conditions. Functionalization with hydroxyl groups may thus be a promising strategy towards attaining highly selective polyimides for economical membrane-based natural gas sweetening.

  20. Pure- and Mixed-Gas Permeation Properties of Highly Selective and Plasticization Resistant Hydroxyl-Diamine-Based 6FDA Polyimides for CO2/CH4 Separation

    KAUST Repository

    Alaslai, Nasser Y.

    2016-01-05

    The effect of hydroxyl functionalization on the m-phenylene diamine moiety of 6FDA dianhydride-based polyimides was investigated for gas separation applications. Pure-gas permeability coefficients of He, H2, N2, O2, CH4, and CO2 were measured at 35 °C and 2 atm. The introduction of hydroxyl groups in the diamine moiety of 6FDA-diaminophenol (DAP) and 6FDA-diamino resorcinol (DAR) polyimides tightened the overall polymer structure due to increased charge transfer complex formation compared to unfunctionalized 6FDA-m-phenylene diamine (mPDA). The BET surface areas based on nitrogen adsorption of 6FDA-DAP (54 m2g−1) and of 6FDA-DAR (45 m2g−1) were ~18% and 32% lower than that of 6FDA-mPDA (66 m2g−1). 6FDA-mPDA had a pure-gas CO2 permeability of 14 Barrer and CO2/CH4 selectivity of 70. The hydroxyl-functionalized polyimides 6FDA-DAP and 6FDA-DAR exhibited very high pure-gas CO2/CH4 selectivities of 92 and 94 with moderate CO2 permeability of 11 and 8 Barrer, respectively. It was demonstrated that hydroxyl-containing polyimide membranes maintained very high CO2/CH4 selectivity (~ 75 at CO2 partial pressure of 10 atm) due to CO2 plasticization resistance when tested under high-pressure mixed-gas conditions. Functionalization with hydroxyl groups may thus be a promising strategy towards attaining highly selective polyimides for economical membrane-based natural gas sweetening.

  1. Preparation of CH4 for 14C measurements

    International Nuclear Information System (INIS)

    Cechova, A.; Grgula, M.; Povinec, P.; Sivo, A.

    1988-01-01

    An improved method of methane preparation from wood samples is described. It consists of the preparation of α-cellulose to secure a complete removal of contamination from the wood, its combustion to the form of CO 2 and the preparation of CH 4 in a new designed hydrogenation converter. Purified methane is suitable as a gas filling of the proportional counter. (author). 1 fig., 16 ref

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

    International Nuclear Information System (INIS)

    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

  3. In situ Low-temperature Pair Distribution Function (PDF) Analysis of CH4 and CO2 Hydrates

    Science.gov (United States)

    Cladek, B.; Everett, M.; McDonnell, M.; Tucker, M.; Keffer, D.; Rawn, C.

    2017-12-01

    Gas hydrates occur in ocean floor and sub-surface permafrost deposits and are stable at moderate to high pressures and low temperatures. They are a clathrate structure composed of hydrogen bonded water cages that accommodate a wide variety of guest molecules. CO2 and CH4 hydrates both crystallize as the cubic sI hydrate and can form a solid solution. Natural gas hydrates are interesting as a potential methane source and for CO2 sequestration. Long-range diffraction studies on gas hydrates give valuable structural information but do not provide a detailed understanding of the disordered gas molecule interactions with the host lattice. In-situ low temperature total scattering experiments combined with pair distribution function (PDF) analysis are used to investigate the gas molecule motions and guest-cage interactions. CO2 and methane hydrates exhibit different decomposition behavior, and CO2 hydrate has a smaller lattice parameter despite it being a relatively larger molecule. Total scattering studies characterizing both the short- and long-range order simultaneously help to elucidate the structural source of these phenomena. Low temperature neutron total scattering data were collected using the Nanoscale Ordered MAterials Diffractometer (NOMAD) beamline at the Spallation Neutron Source (SNS) on CO2 and CH4 hydrates synthesized with D2O. Guest molecule motion within cages and interactions between gases and cages are investigated through the hydrate stability and decomposition regions. Data were collected from 2-80 K at a pressure of 55 mbar on CO2 and CH4 hydrates, and from 80-270 K at 25 bar on CH4 hydrate. The hydrate systems were modeled with classical molecular dynamic (MD) simulations to provide an analysis of the total energy into guest-guest, guest-host and host-host contributions. Combined Reitveld and Reverse Monte Carlo (RMC) structure refinement were used to fit models of the data. This combined modeling and simulation characterizes the effects of CO2 and

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

    Science.gov (United States)

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

    2015-10-06

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

  5. CO2 injection into submarine, CH4-hydrate bearing sediments: Parameter studies towards the development of a hydrate conversion technology

    Science.gov (United States)

    Deusner, Christian; Bigalke, Nikolaus; Kossel, Elke; Haeckel, Matthias

    2013-04-01

    In the recent past, international research efforts towards exploitation of submarine and permafrost hydrate reservoirs have increased substantially. Until now, findings indicate that a combination of different technical means such as depressurization, thermal stimulation and chemical activation is the most promising approach for producing gas from natural hydrates. Moreover, emission neutral exploitation of CH4-hydrates could potentially be achieved in a combined process with CO2 injection and storage as CO2-hydrate. In the German gas hydrate initiative SUGAR, a combination of experimental and numerical studies is used to elucidate the process mechanisms and technical parameters on different scales. Experiments were carried out in the novel high-pressure flow-through system NESSI (Natural Environment Simulator for sub-Seafloor Interactions). Recent findings suggest that the injection of heated, supercritical CO2 is beneficial for both CH4 production and CO2 retention. Among the parameters tested so far are the CO2 injection regime (alternating vs. continuous injection) and the reservoir pressure / temperature conditions. Currently, the influence of CO2 injection temperature is investigated. It was shown that CH4 production is optimal at intermediate reservoir temperatures (8 ° C) compared to lower (2 ° C) and higher temperatures (10 ° C). The reservoir pressure, however, was of minor importance for the production efficiency. At 8 ° C, where CH4- and CO2-hydrates are thermodynamically stable, CO2-hydrate formation appears to be slow. Eventual clogging of fluid conduits due to CO2-rich hydrate formation force open new conduits, thereby tapping different regions inside the CH4-hydrate sample volume for CH4gas. In contrast, at 2 ° C immediate formation of CO2-hydrate results in rapid and irreversible obstruction of the entire pore space. At 10 ° C pure CO2-hydrates can no longer be formed. Consequently the injected CO2 flows through quickly and interaction with

  6. Fabrication Parameters of Asymmetric Mixed Matrix Matrimid-MIL-53/PMHS Membrane for CO2/CH4 Separation

    Directory of Open Access Journals (Sweden)

    Fatereh Dorosti

    2017-03-01

    Full Text Available Asymmetrically mixed matrix Matrimid-MIL-53 membranes with silicone cover layer were fabricated. For better understanding of membrane fabrication process, three main parameters of fabrication, Matrimid concentration, silicone concentration and weight percentage of metal organic framework (MIL-53 particles, were optimized by an experimental design method. Cross-section SEM images were used to study the membrane structure and polymer-particles interface. Moreover, thermal resistance of the membranes and the existence of various bonds in them were investigated by FTIR and TGA analyses. The results showed that membranes had porous structure with finger-like morphology. At low and moderate percentages of particles, there were no non-selective voids observed at polymer-particles interface. The thermal resistance of membranes increased with the increase of MIL-53 weight percentage and the destruction temperature of polymer increased from 410°C to 450°C. The permeability tests results showed that the Matrimid (20% wt-MIL-53(15% wt/PMHS (10%wt membrane exhibited the highest level of CO2/CH4 selectivity (23.6. However, in the membrane with 30 wt% particles loading, selectivity decreased due to particles agglomeration and void formation. The experimental design results showed that the concentration of silicone in covering solution had significant effect. CO2 and CH4 permeability decreased and ideal selectivity of CO2/CH4 increased with silicone concentration enhancement. Although the Matrimid concentration had a little effect on CO2/CH4 ideal selectivity, its enhancement increased the selectivity of the gases. The optimization results showed the membrane with 17.8% of Matrimd polymer, 13.2% of silicone polymer and 15.5 wt% of MIL-53 particle displayed the highest selectivity and CO2 permeability.

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

    Science.gov (United States)

    Bubier, J. L.; Arnkil, S.; Humphreys, E.; Juutinen, S.; Larmola, T.; Moore, T. R.

    2015-12-01

    Atmospheric nitrogen (N) deposition has led to nutrient enrichment in wetlands globally, affecting plant community composition, carbon (C) cycling, and microbial dynamics. Nutrient-limited boreal bogs are long-term sinks of carbon dioxide (CO2), but sources of methane (CH4), an important greenhouse gas. We fertilized Mer Bleue Bog, a Sphagnum moss and evergreen shrub-dominated ombrotrophic bog near Ottawa, Ontario, for 10-15 years with N as NO3 and NH4 at 5, 10 and 20 times ambient N deposition (0.6-0.8 g N m-2 y-1), with and without phosphorus (P) and potassium (K). Treatments were applied to triplicate plots (3 x 3 m) from May - August 2000-2015 and control plots received distilled water. We measured net ecosystem CO2 exchange (NEE), ecosystem photosynthesis and respiration, and CH4 flux with climate-controlled chambers; leaf-level CO2 exchange and biochemistry; substrate-induced respiration, CH4 production and consumption potentials with laboratory incubations; plant species composition and abundance; and microclimate (peat temperature, moisture, light interception). After 15 years, we have found that NEE has decreased, and CH4 emissions have increased, in the highest nutrient treatments owing to changes in vegetation, microtopography, and peat characteristics. Vegetation changes include a loss of Sphagnum moss and introduction of new deciduous species. Simulated atmospheric N deposition has not benefitted the photosynthetic apparatus of the dominant evergreen shrubs, but resulted in higher foliar respiration, contributing to a weaker ecosystem CO2 sink. Loss of moss has led to wetter near-surface substrate, higher rates of decomposition and CH4 emission, and a shift in microbial communities. Thus, elevated atmospheric deposition of nutrients may endanger C storage in peatlands through a complex suite of feedbacks and interactions among vegetation, microclimate, and microbial communities.

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

    Science.gov (United States)

    Tian, H.

    2017-12-01

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

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

    Science.gov (United States)

    Parker, H. A.; Hedelius, J.; Viatte, C.; Wunch, D.; Wennberg, P. O.; Chen, J.; Wofsy, S.; Jones, T.; Franklin, J.; Dubey, M. K.; Roehl, C. M.; Podolske, J. R.; Hillyard, P. W.; Iraci, L. T.

    2015-12-01

    Measurement, reporting and verification (MRV) of anthropogenic emissions and natural sources and sinks of carbon dioxide (CO2) and methane (CH4) are crucial to predict climate change and develop transparent accounting policies to contain climate forcing. Remote sensing technologies are monitoring column averaged dry air mole fractions of CO2 and CH4 (XCO2 & XCH4) from ground and space (OCO-2 and GOSAT) with solar spectroscopy enabling direct MRV. However, current ground based coverage is sparse due to the need for large and expensive high-resolution spectrometers that are part of the Total Column Carbon Observing Network (TCCON, Bruker 125HR). This limits our MRV and satellite validation abilities, both regionally and globally. There are striking monitoring gaps in Asia, South America and Africa where the CO2 emissions are growing and there is a large uncertainty in fluxes from land use change, biomass burning and rainforest vulnerability. To fill this gap we evaluate the precision, accuracy and stability of compact, affordable and easy to use low-resolution spectrometers (Bruker EM27/SUN) by comparing with XCO2 and XCH4 retrieved from much larger high-resolution TCCON instruments. As these instruments will be used in a variety of locations, we evaluate their performance by comparing with 2 previous and 4 current United States TCCON sites in different regions up to 2700 km apart. These sites range from polluted to unpolluted, latitudes of 32 to 46°N, and altitudes of 230 to 2241 masl. Comparisons with some of these sites cover multiple years allowing assessment of the EM27/SUN performance not only in various regions, but also over an extended period of time and with different seasonal influences. Results show that our 2 EM27/SUN instruments capture the diurnal variability of the aforementioned constituents very well, but with offsets from TCCON and long-term variability which may be due in part to the extensive movement these spectrometers were subjected to. These

  10. Development and characterization of polyethersulfone/TiO2 mixed matrix membranes for CO2/CH4 separation

    Science.gov (United States)

    Galaleldin, S.; Mannan, H. A.; Mukhtar, H.

    2017-12-01

    In this study, mixed matrix membranes comprised of polyethersulfone as the bulk polymer phase and titanium dioxide (TiO2) nanoparticles as the inorganic discontinuous phase were prepared for CO2/CH4 separation. Membranes were synthesized at filler loading of 0, 5, 10 and 15 wt % via dry phase inversion method. Morphology, chemical bonding and thermal characteristics of membranes were scrutinized utilizing different techniques, namely: Field Emission Scanning Electron Microscopy (FESEM), Fourier Transform InfraRed (FTIR) spectra and Thermogravimetric analysis (TGA) respectively. Membranes gas separation performance was evaluated for CO2 and CH4 gases at 4 bar feed pressure. The highest separation performance was achieved by mixed matrix membrane (MMM) at 5 % loading of TiO2.

  11. The Design of The Monitoring Tools Of Clean Air Condition And Dangerous Gas CO, CO2 CH4 In Chemical Laboratory By Using Fuzzy Logic Based On Microcontroller

    Science.gov (United States)

    Widodo, Slamet; Miftakul, Amin M.; Sutrisman, Adi

    2018-02-01

    There are many phenomena that human are exposed to toxins from certain types such as of CO2, CO2 and CH4 gases. The device used to detect large amounts of CO, CO2, and CH4 gas in air in enclosed spaces using MQ 135 gas sensors of different types based on the three sensitivity of the Gas. The results of testing the use of sensors MQ 135 on the gas content of CO, CO2 and CH4 received by the sensor is still in the form of ppm based on the maximum ppm detection range of each sensor. Active sensor detects CO 120 ppm gas, CO2 1600 ppm and CH4 1ppm "standby 1" air condition with intermediate rotary fan. Active sensor detects CO 30 ppm gas, CO2 490 ppm and CH4 7 ppm "Standby 2" with low rotating fan output. Fuzzy rulebase logic for motor speed when gas detection sensor CO, CO2, and CH4 output controls the motion speed of the fan blower. Active sensors detect CO 15 ppm, CO2 320 ppm and CH4 45 ppm "Danger" air condition with high fan spin fan. At the gas level of CO 15 ppm, CO2 390 ppm and CH4 3 ppm detect "normal" AC sensor with fan output stop spinning.

  12. Enhanced photocatalytic CO2 reduction to CH4 over separated dual co-catalysts Au and RuO2

    Science.gov (United States)

    Dong, Chunyang; Hu, Songchang; Xing, Mingyang; Zhang, Jinlong

    2018-04-01

    A spatially separated, dual co-catalyst photocatalytic system was constructed by the stepwise introduction of RuO2 and Au nanoparticles (NPs) at the internal and external surfaces of a three dimensional, hierarchically ordered TiO2-SiO2 (HTSO) framework (the final photocatalyst was denoted as Au/HRTSO). Characterization by HR-TEM, EDS-mapping, XRD and XPS confirmed the existence and spatially separated locations of Au and RuO2. In CO2 photocatalytic reduction (CO2PR), Au/HRTSO (0.8%) shows the optimal performance in both the activity and selectivity towards CH4; the CH4 yield is almost twice that of the singular Au/HTSO or HRTSO (0.8%, weight percentage of RuO2) counterparts. Generally, Au NPs at the external surface act as electron trapping agents and RuO2 NPs at the inner surface act as hole collectors. This advanced spatial configuration could promote charge separation and transfer efficiency, leading to enhanced CO2PR performance in both the yield and selectivity toward CH4 under simulated solar light irradiation.

  13. CH4 recovery and CO2 sequestration using flue gas in natural gas hydrates as revealed by a micro-differential scanning calorimeter

    International Nuclear Information System (INIS)

    Lee, Yohan; Kim, Yunju; Lee, Jaehyoung; Lee, Huen; Seo, Yongwon

    2015-01-01

    Highlights: • The extent of the replacement was improved due to the enclathration of N 2 in small cages. • The dissociation enthalpies of the replaced gas hydrates were measured. • There was no noticeable heat flow change during the CH 4 –flue gas replacement. • The replacement could occur without significant destruction of gas hydrates. - Abstract: The CH 4 –flue gas replacement in naturally occurring gas hydrates has attracted significant attention due to its potential as a method of exploitation of clean energy and sequestration of CO 2 . In the replacement process, the thermodynamic and structural properties of the mixed gas hydrates are critical factors to predict the heat flow in the hydrate-bearing sediments and the heat required for hydrate dissociation, and to evaluate the CO 2 storage capacity of hydrate reservoirs. In this study, the 13 C NMR and gas composition analyses confirmed that the preferential enclathration of N 2 molecules in small 5 12 cages of structure I hydrates improved the extent of the CH 4 recovery. A high pressure micro-differential scanning calorimeter (HP μ-DSC) provided reliable hydrate stability conditions and heat of dissociation values in the porous silica gels after the replacement, which confirmed that CH 4 in the hydrates was successfully replaced with flue gas. A heat flow change associated with the dissociation and formation of hydrates was not noticeable during the CH 4 –flue gas replacement. Therefore, this study reveals that CH 4 –flue gas swapping occurs without structural transitions and significant hydrate dissociations

  14. The arctic seasonal cycle of total column CO2 and CH4 from ground-based solar and lunar FTIR absorption spectrometry

    Directory of Open Access Journals (Sweden)

    M. Buschmann

    2017-07-01

    Full Text Available Solar absorption spectroscopy in the near infrared has been performed in Ny-Ålesund (78.9° N, 11.9° E since 2002; however, due to the high latitude of the site, the sun is below the horizon from October to March (polar night and no solar absorption measurements are possible. Here we present a novel method of retrieving the total column dry-air mole fractions (DMFs of CO2 and CH4 using moonlight in winter. Measurements have been taken during the polar nights from 2012 to 2016 and are validated with TCCON (Total Carbon Column Observing Network measurements by solar and lunar absorption measurements on consecutive days and nights during spring and autumn. The complete seasonal cycle of the DMFs of CO2 and CH4 is presented and a precision of up to 0.5 % is achieved. A comparison of solar and lunar measurements on consecutive days during day and night in March 2013 yields non-significant biases of 0. 66 ± 4. 56 ppm for xCO2 and −1. 94 ± 20. 63 ppb for xCH4. Additionally a model comparison has been performed with data from various reanalysis models.

  15. Role of intrachain rigidity in the plasticization of intrinsically microporous triptycene-based polyimide membranes in mixed-Gas CO2/CH4 separations

    KAUST Repository

    Swaidan, Raja; Ghanem, Bader; Al-Saeedi, Majed; Litwiller, Eric; Pinnau, Ingo

    2014-01-01

    is not a singular solution to intrinsic plasticization resistance. Despite the significant intrachain rigidity in TPDA-TMPD, a 300% increase in PMIX(CH4), 50% decrease in α(CO2/CH4) from 24 to 12, and continuous increase in PMIX(CO2) occurred from 4 to 30

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

    Science.gov (United States)

    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

  17. Air–sea fluxes of CO2 and CH4 from the Penlee Point Atmospheric Observatory on the south-west coast of the UK

    Directory of Open Access Journals (Sweden)

    M. Yang

    2016-05-01

    Full Text Available We present air–sea fluxes of carbon dioxide (CO2, methane (CH4, momentum, and sensible heat measured by the eddy covariance method from the recently established Penlee Point Atmospheric Observatory (PPAO on the south-west coast of the United Kingdom. Measurements from the south-westerly direction (open water sector were made at three different sampling heights (approximately 15, 18, and 27 m above mean sea level, a.m.s.l., each from a different period during 2014–2015. At sampling heights  ≥  18 m a.m.s.l., measured fluxes of momentum and sensible heat demonstrate reasonable ( ≤  ±20 % in the mean agreement with transfer rates over the open ocean. This confirms the suitability of PPAO for air–sea exchange measurements in shelf regions. Covariance air–sea CO2 fluxes demonstrate high temporal variability. Air-to-sea transport of CO2 declined from spring to summer in both years, coinciding with the breakdown of the spring phytoplankton bloom. We report, to the best of our knowledge, the first successful eddy covariance measurements of CH4 emissions from a marine environment. Higher sea-to-air CH4 fluxes were observed during rising tides (20 ± 3; 38 ± 3; 29 ± 6 µmole m−2 d−1 at 15, 18, 27 m a.m.s.l. than during falling tides (14 ± 2; 22 ± 2; 21 ± 5 µmole m−2 d−1, consistent with an elevated CH4 source from an estuarine outflow driven by local tidal circulation. These fluxes are a few times higher than the predicted CH4 emissions over the open ocean and are significantly lower than estimates from other aquatic CH4 hotspots (e.g. polar regions, freshwater. Finally, we found the detection limit of the air–sea CH4 flux by eddy covariance to be 20 µmole m−2 d−1 over hourly timescales (4 µmole m−2 d−1 over 24 h.

  18. Selective Reduction of CO2 to CH4 by Tandem Hydrosilylation with Mixed Al/B Catalysts

    KAUST Repository

    Chen, Jiawei

    2016-04-04

    This contribution reports the first example of highly selective reduction of CO2 into CH4 via tandem hydrosilylation with mixed main-group organo-Lewis acid (LA) catalysts [Al(C6F5)3 + B(C6F5)3] {[Al] + [B]}. As shown by this comprehensive experimental and computational study, in this unique tandem catalytic process, [Al] effectively mediates the first step of the overall reduction cycle, namely the fixation of CO2 into HCOOSiEt3 (1) via the LA-mediated C=O activation, while [B] is incapable of promoting the same transformation. On the other hand, [B] is shown to be an excellent catalyst for the subsequent reduction steps 2–4, namely the hydrosilylation of the more basic intermediates [1 to H2C(OSiEt3)2 (2) to H3COSiEt3 (3) and finally to CH4] through the frustrated-Lewis-pair (FLP)-type Si–H activation. Hence, with the required combination of [Al] and [B], a highly selective hydrosilylative reduction of CO2 system has been developed, achieving high CH4 production yield up to 94%. The remarkably different catalytic behaviors between [Al] and [B] are attributed to the higher overall Lewis acidity of [Al] derived from two conflicting factors (electronic and steric effects), which renders the higher tendency of [Al] to form stable [Al]–substrate (intermediate) adducts with CO2 as well as subsequent intermediates 1, 2 and 3. Overall, the roles of [Al] and [B] are not only complementary but also synergistic in the total reduction of CO2, which render both [Al]-mediated first reduction step and [B]-mediated subsequent steps catalytic.

  19. Selective Reduction of CO2 to CH4 by Tandem Hydrosilylation with Mixed Al/B Catalysts

    KAUST Repository

    Chen, Jiawei; Falivene, Laura; Caporaso, Lucia; Cavallo, Luigi; Chen, Eugene Y.-X.

    2016-01-01

    This contribution reports the first example of highly selective reduction of CO2 into CH4 via tandem hydrosilylation with mixed main-group organo-Lewis acid (LA) catalysts [Al(C6F5)3 + B(C6F5)3] {[Al] + [B]}. As shown by this comprehensive experimental and computational study, in this unique tandem catalytic process, [Al] effectively mediates the first step of the overall reduction cycle, namely the fixation of CO2 into HCOOSiEt3 (1) via the LA-mediated C=O activation, while [B] is incapable of promoting the same transformation. On the other hand, [B] is shown to be an excellent catalyst for the subsequent reduction steps 2–4, namely the hydrosilylation of the more basic intermediates [1 to H2C(OSiEt3)2 (2) to H3COSiEt3 (3) and finally to CH4] through the frustrated-Lewis-pair (FLP)-type Si–H activation. Hence, with the required combination of [Al] and [B], a highly selective hydrosilylative reduction of CO2 system has been developed, achieving high CH4 production yield up to 94%. The remarkably different catalytic behaviors between [Al] and [B] are attributed to the higher overall Lewis acidity of [Al] derived from two conflicting factors (electronic and steric effects), which renders the higher tendency of [Al] to form stable [Al]–substrate (intermediate) adducts with CO2 as well as subsequent intermediates 1, 2 and 3. Overall, the roles of [Al] and [B] are not only complementary but also synergistic in the total reduction of CO2, which render both [Al]-mediated first reduction step and [B]-mediated subsequent steps catalytic.

  20. Evaluating the use of electrical resistivity imaging technique for improving CH4 and CO2 emission rate estimations in landfills

    International Nuclear Information System (INIS)

    Georgaki, I.; Soupios, P.; Sakkas, N.; Ververidis, F.; Trantas, E.; Vallianatos, F.; Manios, T.

    2008-01-01

    In order to improve the estimation of surface gas emissions in landfill, we evaluated a combination of geophysical and greenhouse gas measurement methodologies. Based on fifteen 2D electrical resistivity tomographies (ERTs), longitudinal cross section images of the buried waste layers were developed, identifying place and cross section size of organic waste (OW), organic waste saturated in leachates (SOW), low organic and non-organic waste. CH 4 and CO 2 emission measurements were then conducted using the static chamber technique at 5 surface points along two tomographies: (a) across a high-emitting area, ERT no. 2, where different amounts of relatively fresh OW and SOW were detected, and (b) across the oldest (at least eight years) cell in the landfill, ERT no. 6, with significant amounts of OW. Where the highest emission rates were recorded, they were strongly affected by the thickness of the OW and SOW fraction underneath each gas sampling point. The main reason for lower than expected values was the age of the layered buried waste. Lower than predicted emissions were also attributed to soil condition, which was the case at sampling points with surface ponding, i.e. surface accumulation of leachate (or precipitated water)

  1. Application of biochar and nitrogen influences fluxes of CO2, CH4 and N2O in a forest soil.

    Science.gov (United States)

    Hawthorne, Iain; Johnson, Mark S; Jassal, Rachhpal S; Black, T Andrew; Grant, Nicholas J; Smukler, Sean M

    2017-05-01

    Nitrogen (N) fertilization of forests for increasing carbon sequestration and wood volume is expected to influence soil greenhouse gas (GHG) emissions, especially to increase N 2 O emissions. As biochar application is known to affect soil GHG emissions, we investigated the effect of biochar application, with and without N fertilization, to a forest soil on GHG emissions in a controlled laboratory study. We found that biochar application at high (10%) application rates increased CO 2 and N 2 O emissions when applied without urea-N fertilizer. At both low (1%) and high biochar (10%) application rates CH 4 consumption was reduced when applied without urea-N fertilizer. Biochar application with urea-N fertilization did not increase CO 2 emissions compared to biochar amended soil without fertilizer. In terms of CO 2 -eq, the net change in GHG emissions was mainly controlled by CO 2 emissions, regardless of treatment, with CH 4 and N 2 O together accounting for less than 1.5% of the total emissions. Copyright © 2017 Elsevier Ltd. All rights reserved.

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

    Science.gov (United States)

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

    2014-01-01

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

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

    KAUST Repository

    Tingas, Efstathios Al.

    2017-10-05

    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 dynamics that control ignition delay and emission formation. Increasing CO2 dilution causes longer ignition delays, lower final temperatures and decreased formation of NO and CO. These effects of CO2 dilution are shown to be entirely thermal, contrary to what happens with dilution with H2O, which also has chemical activity and can reduce ignition delay. For the same initial mole fraction of the diluent, the decrease in final temperature and in NO concentration is larger in the CO2 case whereas the decrease in CO is larger in the H2O case. The thermal effect of CO2 is entirely analogous with those of dilution with the chemically inert Ar, only stronger for the same percentage of initial dilution, because of the larger specific heat of CO2. The reactions that have the largest contribution to the characteristic explosive time scale of the system during ignition delay (H2O2(+M)→OH+OH(+M), CH3O2+CH2O→CH3O2H+HCO, CH4+CH3O2→CH3+CH3O2H, H+O2→O+OH, etc.) are not substantially affected by CO2 dilution, neither are the species that are pointed by CSP (CH3O2, H2O2, CH2O, etc.) as having the largest impact on the this timescale. The same holds for the modes that control CO and NO formation. The results point to the possibility of cold exhaust gas recirculation being used in order to produce mixtures with longer ignition delays and therefore substantial resistance to uncontrolled ignition.

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

    Directory of Open Access Journals (Sweden)

    Cuicui Mu

    2016-01-01

    Full Text Available Thermokarst lakes are widely distributed on the Qinghai-Tibetan Plateau (QTP, which accounts for 8% of the global permafrost area. These lakes probably promote organic matter biodegradation and thus accelerate the emission of carbon-based greenhouse gases. However, little is known about greenhouse gas concentrations and their stable isotopes characteristics of these lakes. In this study, we measured the concentrations of dissolved organic carbon (DOC, dissolved CO2 and CH4, as well as the distribution of δ13CCO2, δ13CCH4, and δ13COM (organic matter of lake sediments in thermokarst lakes on the QTP. Results showed that the OM of the lake sediments was highly decomposed. The concentrations of DOC, CO2 and CH4 in the lake water on the QTP were 1.2–49.6 mg L–1, 3.6–45.0 μmol L–1 and 0.28–3.0 μmol L–1, respectively. The highest CO2 and CH4 concentrations were recorded in July while the lowest values in September, which suggested that temperature had an effect on greenhouse gas production, although this pattern may also relate to thermal stratification of the water column. The results implied that thermokast lakes should be paid more attention to regarding carbon cycle and greenhouse gas emissions on the QTP.

  5. Changes in concentration and (delta) 13C value of dissolved CH4, CO2 and organic carbon in rice paddies under ambient and elevated concentrations of atmospheric CO2

    International Nuclear Information System (INIS)

    Weiguo Cheng; Yagi, Kazuyuki; Sakai, Hidemitsu; Hua Xu; Kobayashi, Kazuhiko

    2005-01-01

    Changes in concentration and (delta) 13 C value of dissolved CH 4 , CO 2 and organic carbon (DOC) in floodwater and soil solution from a Japanese rice paddy were studied under ambient and elevated concentrations of atmospheric CO 2 in controlled environment chambers. The concentrations of dissolved CH 4 in floodwater increased with rice growth (with some fluctuation), while the concentrations of CO 2 remained between 2.9 to 4.4 and 4.2 to 5.8 μg C mL -1 under conditions of ambient and elevated CO 2 concentration, respectively. The amount of CH 4 dissolved in soil solution under elevated CO 2 levels was significantly lower than under ambient CO 2 in the tillering stage, implying that the elevated CO 2 treatment accelerated CH 4 oxidation during the early stage of growth. However, during later stages of growth, production of CH 4 increased and the amount of CH 4 dissolved in soil solution under elevated CO 2 levels was, on average, greater than that under ambient CO 2 conditions. Significant correlation existed among the (delta) 13 C values of dissolved CH 4 , CO 2 , and DOC in floodwater (except for the samples taken immediately after pulse feeding with 13 C enriched CO 2 ), indicating that the origins and cycling of CH 4 , CO 2 and DOC were related. There were also significant correlations among the (delta) 13 C values of CH 4 , CO 2 and DOC in the soil solution. The turnover rate of CO 2 in soil solution was most rapid in the panicle formation stage of rice growth and that of CH 4 fastest in the grain filling stage. (Author)

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

    Science.gov (United States)

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

    2017-04-01

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

  7. Carbon dioxide induced bubble formation in a CH4-CO2-H2O ternary system: a molecular dynamics simulation study.

    Science.gov (United States)

    Sujith, K S; Ramachandran, C N

    2016-02-07

    The extraction of methane from its hydrates using carbon dioxide involves the decomposition of the hydrate resulting in a CH4-CO2-H2O ternary solution. Using classical molecular dynamics simulations, we investigate the evolution of dissolved gas molecules in the ternary system at different concentrations of CO2. Various compositions considered in the present study resemble the solution formed during the decomposition of methane hydrates at the initial stages of the extraction process. We find that the presence of CO2 aids the formation of CH4 bubbles by causing its early nucleation. Elucidation of the composition of the bubble revealed that in ternary solutions with high concentration of CO2, mixed gas bubbles composed of CO2 and CH4 are formed. To understand the role of CO2 in the nucleation of CH4 bubbles, the structure of the bubble formed was analyzed, which revealed that there is an accumulation of CO2 at the interface of the bubble and the surrounding water. The aggregation of CO2 at the bubble-water interface occurs predominantly when the concentration of CO2 is high. Radial distribution function for the CH4-CO2 pair indicates that there is an increasingly favorable direct contact between dissolved CH4 and CO2 molecules in the bubble-water interface. It is also observed that the presence of CO2 at the interface results in the decrease in surface tension. Thus, CO2 leads to greater stability of the bubble-water interface thereby bringing down the critical size of the bubble nuclei. The results suggest that a rise in concentration of CO2 helps in the removal of dissolved CH4 thereby preventing the accumulation of methane in the liquid phase. Thus, the presence of CO2 is predicted to assist the decomposition of methane hydrates in the initial stages of the replacement process.

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

    Science.gov (United States)

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

    2015-02-01

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

  9. Spatial variability of greenhouse gases emissions (CO2, CH4, N2O) in a tropical hydroelectric reservoir flooding primary forest (Petit Saut Reservoir, French Guiana)

    Science.gov (United States)

    Cailleaud, Emilie; Guérin, Frédéric; Bouillon, Steven; Sarrazin, Max; Serça, Dominique

    2014-05-01

    At the Petit Saut Reservoir (PSR, French Guiana, South America), vertical profiles were performed at 5 stations in the open waters (OW) and 6 stations in two shallow flooded forest (FF) areas between April 2012 and September 2013. Measurements included physico-chemical parameters, ammonium, nitrate and dissolved greenhouse gas (CO2, CH4, N2O) concentrations, dissolved and particulate organic carbon (DOC, POC) and nitrogen (PN), δ13C-POC and δ15N-PN . The diffusive fluxes were calculated from surface concentrations. The aim of this study was to estimate the spatial variations of greenhouse gas emissions at a dentrical hydroelectric reservoir located in the tropics and flooding primary forest. Twenty years after impoundment, the water column of the PSR is permanently and tightly stratified thermally in the FF whereas in the OW, the thermal gradients are not as stable. The different hydrodynamical behaviours between the two different zones have significant consequences on the biogeochemistry: oxygen barely diffuses down to the hypolimnion in the FF whereas destratification occurs sporadically during the rainy season in the OW. Although we found the same range of POC in the FF and the OW (2.5-29 μmol L-1) and 20% more DOC at the bottom of OW than in the FF (229-878 μmol L-1), CO2 and CH4 concentrations were always significantly higher in the FF (CO2: 11-1412 μmol L-1, CH4: 0.001-1015 μmol L-1) than in the OW. On average, the CO2 concentrations were 30-40% higher in the FF than in the OW and the CH4 concentrations were three times higher in the FF than in the OW. The δ13C-POC and C:N values did not suggest substantial differences in the sources of OM between the FF and OW. At all stations, POC at the bottom has an isotopic signature slightly lighter than the terrestrial OM in the surrounding forest whereas the isotopic signature of surface POM would result from phytoplankton and methanotrophs. The vertical profiles of nitrogen compounds reveal that the main

  10. Discussion of the influence of CO and CH4 in CO2 transport, injection, and storage for CCS technology.

    Science.gov (United States)

    Blanco, Sofía T; Rivas, Clara; Bravo, Ramón; Fernández, Javier; Artal, Manuela; Velasco, Inmaculada

    2014-09-16

    This paper discusses the influence of the noncondensable impurities CO and CH4 on Carbon Capture and Storage (CCS) technology. We calculated and drew conclusions about the impact of both impurities in the CO2 on selected transport, injection, and storage parameters (pipeline pressure drop, storage capacity, etc.), whose analysis is necessary for the safe construction and operation of CO2 pipelines and for the secure long-term geological storage of anthropogenic CO2. To calculate these parameters, it is necessary to acquire data on the volumetric properties and the vapor-liquid equilibrium of the fluid being subjected to CCS. In addition to literature data, we used new experimental data, which are presented here and were obtained for five mixtures of CO2+CO with compositions characteristic of the typical emissions of the E.U. and the U.S.A. Temperatures and pressures are based on relevant CO2 pipeline and geological storage site values. From our experimental results, Peng-Robinson, PC-SAFT, and GERG Equations of State for were validated CO2+CO under the conditions of CCS. We conclude that the concentration of both impurities strongly affects the studied parameters, with CO being the most influential and problematic. The overall result of these negative effects is an increase in the difficulties, risks, and overall costs of CCS.

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

    Science.gov (United States)

    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

    This study deals with the problem of identifying atmospheric data influenced by local emissions that can result in spikes in time series of greenhouse gases and long-lived tracer measurements. We considered three spike detection methods known as coefficient of variation (COV), robust extraction of baseline signal (REBS) and standard deviation of the background (SD) to detect and filter positive spikes in continuous greenhouse gas time series from four monitoring stations representative of the European ICOS (Integrated Carbon Observation System) Research Infrastructure network. The results of the different methods are compared to each other and against a manual detection performed by station managers. Four stations were selected as test cases to apply the spike detection methods: a continental rural tower of 100 m height in eastern France (OPE), a high-mountain observatory in the south-west of France (PDM), a regional marine background site in Crete (FKL) and a marine clean-air background site in the Southern Hemisphere on Amsterdam Island (AMS). This selection allows us to address spike detection problems in time series with different variability. Two years of continuous measurements of CO2, CH4 and CO were analysed. All methods were found to be able to detect short-term spikes (lasting from a few seconds to a few minutes) in the time series. Analysis of the results of each method leads us to exclude the COV method due to the requirement to arbitrarily specify an a priori percentage of rejected data in the time series, which may over- or underestimate the actual number of spikes. The two other methods freely determine the number of spikes for a given set of parameters, and the values of these parameters were calibrated to provide the best match with spikes known to reflect local emissions episodes that are well documented by the station managers. More than 96 % of the spikes manually identified by station managers were successfully detected both in the SD and the

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

    Directory of Open Access Journals (Sweden)

    A. El Yazidi

    2018-03-01

    Full Text Available This study deals with the problem of identifying atmospheric data influenced by local emissions that can result in spikes in time series of greenhouse gases and long-lived tracer measurements. We considered three spike detection methods known as coefficient of variation (COV, robust extraction of baseline signal (REBS and standard deviation of the background (SD to detect and filter positive spikes in continuous greenhouse gas time series from four monitoring stations representative of the European ICOS (Integrated Carbon Observation System Research Infrastructure network. The results of the different methods are compared to each other and against a manual detection performed by station managers. Four stations were selected as test cases to apply the spike detection methods: a continental rural tower of 100 m height in eastern France (OPE, a high-mountain observatory in the south-west of France (PDM, a regional marine background site in Crete (FKL and a marine clean-air background site in the Southern Hemisphere on Amsterdam Island (AMS. This selection allows us to address spike detection problems in time series with different variability. Two years of continuous measurements of CO2, CH4 and CO were analysed. All methods were found to be able to detect short-term spikes (lasting from a few seconds to a few minutes in the time series. Analysis of the results of each method leads us to exclude the COV method due to the requirement to arbitrarily specify an a priori percentage of rejected data in the time series, which may over- or underestimate the actual number of spikes. The two other methods freely determine the number of spikes for a given set of parameters, and the values of these parameters were calibrated to provide the best match with spikes known to reflect local emissions episodes that are well documented by the station managers. More than 96 % of the spikes manually identified by station managers were successfully detected both in

  13. Porous carbon derived via KOH activation of a hypercrosslinked porous organic polymer for efficient CO_2, CH_4, H_2 adsorptions and high CO_2/N_2 selectivity

    International Nuclear Information System (INIS)

    Modak, Arindam; Bhaumik, Asim

    2015-01-01

    Microporous carbon having Brunauer-Emmett-Teller (BET) surface area of 2186 m"2 g"−"1 and micropore volume of 0.85 cm"3 g"−"1 has been synthesized via KOH induced high temperature carbonization of a non-conjugated hypercrosslinked organic polymer. Owing to the templating and activation by KOH, we have succeeded in making a microporous carbon from this porous polymer and the resultant carbon material showed high uptake for CO_2 (7.6 mmol g"−"1) and CH_4 (2.4 mmol g"−"1) at 1 atm, 273 K together with very good selectivity for the CO_2/N_2 (30.2) separation. Furthermore, low pressure (1 atm) H_2 (2.6 wt%, 77 K) and water uptake (57.4 wt%, 298 K) ability of this polymer derived porous activated carbon is noteworthy. - Graphical abstract: Microporous carbon with BET surface area of 2186 m"2 g"−"1 has been synthesized via KOH activation of a porous organic polymer and it showed high uptake for CO_2 (7.6 mmol g"−"1), CH_4 (2.4 mmol g"−"1) and H_2 (2.6 wt%) at 1 atm together with very good selectivity for CO_2. - Highlights: • Porous carbon from hypercrosslinked organic polymer. • KOH activated carbon with BET surface area 2186 m"2 g"−"1. • High CO2 uptake (7.6 mmol g"−"1) and CO_2/N_2 selectivity (30.2). • Porous carbon also showed high H_2 (2.6 wt%) and H_2O (57.4 wt%) uptakes.

  14. [Effect of carbon substrate concentration on N2, N2O, NO, CO2, and CH4 emissions from a paddy soil in anaerobic condition].

    Science.gov (United States)

    Chen, Nuo; Liao, Ting-ting; Wang, Rui; Zheng, Xun-hua; Hu, Rong-gui; Butterbach-Bahl, Klaus

    2014-09-01

    Understanding the effects of carbon and nitrogen substrates concentrations on the emissions of denitrification gases including nitrogen (N2) , nitrous oxide (N2O) and nitric oxide (NO), carbon dioxide (CO2) and methane (CH4) from anaerobic paddy soils is believed to be helpful for development of greenhouse gas mitigation strategies. Moreover, understanding the quantitative dependence of denitrification products compositions on carbon substrate concentration could provide some key parameters or parameterization scheme for developing process-oriented model(s) of nitrogen transformation. Using a silt loam soil collected from a paddy field, we investigated the influence of carbon substrate concentration on the emissions of the denitrification gases, CO2 and CH4 from anaerobically incubated soils by setting two treatments: control (CK) with initial soil nitrate and dissolved organic carbon (DOC) concentrations of ~ 50 mg.kg-1 and -28 mg kg-1 , respectively; and DOC added (C + ) with initial soil nitrate and DOC concentrations of ~50 mg.kg-1 and ~300 mg.kg-1 , respectively. The emissions of denitrification gases, CO2 and CH4, as well as concentrations of carbon and nitrogen substrates for each treatment were dynamically measured, using the gas-flow-soil-core technique and a paralleling substrate monitoring system. The results showed that CH4 emission was not observed in CK treatment while observed in C treatment. Aggregate emission of greenhouse gases for C + treatment was significantly higher comparing with the CK treatment (P emissions in total nitrogen gases emissions were approximately 9% , 35% and 56% for CK treatment, respectively; and approximately 31% , 50% and 19% for C+ treatment, respectively, with significant differences between these two treatments (P carbon substrate concentrations can significantly change the composition of nitrogen gas emissions. The results also implicated that organic fertilizer should not be applied to nitrate-rich paddy soils prior to

  15. Hindering effects in diffusion of CO2/CH4 mixtures in ZIF-8 crystals

    NARCIS (Netherlands)

    Chmelik, C.; van Baten, J.; Krishna, R.

    2012-01-01

    Cage-type micro-porous materials such as LTA, CHA, SAPO-34, DDR, ERI, ZIF-7, and ZIF-8 have significant potential for use in membrane technologies for CO2 capture. The permeation selectivities are governed by a combination of adsorption and diffusion selectivities, each of which can be separately

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

    Science.gov (United States)

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

    2009-03-01

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

  17. Experimental ion mobility measurements in Xe-CH4

    Science.gov (United States)

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

    2017-09-01

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

  18. Application of Relaxed Eddy Accumulation (REA) method to estimate CO2 and CH4 surface fluxes in the city of Krakow, southern Poland.

    Science.gov (United States)

    Zimnoch, Miroslaw; Gorczyca, Zbigniew; Pieniazek, Katarzyna; Jasek, Alina; Chmura, Lukasz; Rozanski, Kazimierz

    2013-04-01

    There is a growing interest in the recent years in studies aimed at quantifying carbon cycling in urban centres. Worldwide migration of human population from rural to urban areas and corresponding growth of extensive urban agglomerations and megacities leads to intensification of anthropogenic emissions of carbon and strong disruption of natural carbon cycle on these areas. Therefore, a deeper understanding of the carbon "metabolism" of such regions is required. Apart of better quantification of surface carbon fluxes, also a thorough understanding of the functioning of biosphere under strong anthropogenic influence is needed. Nowadays, covariance methods are widely applied for studying gas exchange between the atmosphere and the Earth's surface. Relaxed Eddy Accumulation method (REA), combined with the CO2 and CH4 CRDS analyser allows simultaneous measurements of surface fluxes of carbon dioxide and methane within the chosen footprint of the detection system, thus making possible thorough characterisation of the overall exchange of those gases between the atmosphere and the urban surface across diverse spatial and temporal scales. Here we present preliminary results of the study aimed at quantifying surface fluxes of CO2 and CH4 in Krakow, southern Poland. The REA system for CO2 and CH4 flux measurements has been installed on top of a 20m high tower mounted on the roof of the faculty building, close to the city centre of Krakow. The sensors were installed ca 42 m above the local ground. Gill Windmaster-Pro sonic anemometer was coupled with self-made system, designed by the Poznan University of Life Sciences, Poland, for collecting air samples in two pairs of 10-liter Tedlar bags, and with Picarro G2101-i CRDS analyser. The air was collected in 30-min intervals. The CO2 and CH4 mixing ratios in these cumulative downdraft and updraft air samples were determined by the CRDS analyser after each sampling interval. Based on the measured mixing ratios difference and the

  19. Plasticization-resistant hollow fiber membranes for CO2/CH4 separation based on a thermally crosslinkable polyimide

    KAUST Repository

    Chen, Chien-Chiang

    2011-10-01

    Decarboxylation-induced thermal crosslinking has been demonstrated to be effective for stabilizing membranes against plasticization in dense films. This study extends this promising crosslinking approach from dense films to industrially relevant asymmetric hollow fiber membranes. Crosslinkable asymmetric hollow fiber membranes were spun from a carboxylic acid containing polyimide, 6FDA-DAM:DABA. Dope and spinning conditions were optimized to obtain fibers with a defect-free selective skin layer. It is found that slightly defective fibers suffered severe selectivity loss after thermal crosslinking, suggesting that defect-free property is essential to the performance of the resulting crosslinked hollow fiber membranes. The crosslinked fibers were tested for CO 2/CH 4 separation. The excellent plasticization resistance under high pressure feeds (with highest CO 2 partial pressure of 400psia) suggests that these robust membranes are promising for aggressive natural gas purification. © 2011 Elsevier B.V.

  20. Plasticization-resistant hollow fiber membranes for CO2/CH4 separation based on a thermally crosslinkable polyimide

    KAUST Repository

    Chen, Chien-Chiang; Qiu, Wulin; Miller, Stephen J.; Koros, William J.

    2011-01-01

    Decarboxylation-induced thermal crosslinking has been demonstrated to be effective for stabilizing membranes against plasticization in dense films. This study extends this promising crosslinking approach from dense films to industrially relevant asymmetric hollow fiber membranes. Crosslinkable asymmetric hollow fiber membranes were spun from a carboxylic acid containing polyimide, 6FDA-DAM:DABA. Dope and spinning conditions were optimized to obtain fibers with a defect-free selective skin layer. It is found that slightly defective fibers suffered severe selectivity loss after thermal crosslinking, suggesting that defect-free property is essential to the performance of the resulting crosslinked hollow fiber membranes. The crosslinked fibers were tested for CO 2/CH 4 separation. The excellent plasticization resistance under high pressure feeds (with highest CO 2 partial pressure of 400psia) suggests that these robust membranes are promising for aggressive natural gas purification. © 2011 Elsevier B.V.

  1. AirCore-HR: a high-resolution column sampling to enhance the vertical description of CH4 and CO2

    Directory of Open Access Journals (Sweden)

    O. Membrive

    2017-06-01

    good agreement is found in terms of vertical structure, the comparison between the various AirCores yields a large and variable bias (up to almost 3 ppm in some parts of the profiles. The reasons of this bias, possibly related to the drying agent used to dry the air, are still being investigated. Finally, the uncertainties associated with the measurements are assessed, yielding an average uncertainty below 3 ppb for CH4 and 0.25 ppm for CO2 with the major source of uncertainty coming from the potential loss of air sample on the ground and the choice of the starting and ending point of the collected air sample inside the tube. In an ideal case where the sample would be fully retained, it would be possible to know precisely the pressure at which air was sampled last and thus to improve the overall uncertainty to about 0.1 ppm for CO2 and 2 ppb for CH4.

  2. Calculated and measured W values in N2, Ar, CH4 and CO2 gases for ions H+, He+, C+, N+, O+ and Ar+ in the energy range 25 KeV to 375 KeV

    International Nuclear Information System (INIS)

    Nguyen Van Dat; Chemtob, Maurice.

    1979-01-01

    The present paper describes the experimental method used for measurement of W values in argon gas and in the three components of T.E. gas: nitrogen, methane and carbon dioxide, for ions with masses in the range 1 to 40 a.m.u. and with energies in the range 25 KeV to 375 KeV. For these ions, the incident velocities are comparable to the electron orbital velocities. At these velocities energy losses due to elastic scattering and electron capture processes are expected to become significant as compared to ionization and excitation which predominate at higher velocities. These measured W values are then compared to calculated values. These calculations are obtained by introducing the inelastic and elastic stopping power cross sections in a transport equation, the resolution of which gives ionization range and the amount of energy released to produce ionization

  3. A microporous MOF with a polar pore surface exhibiting excellent selective adsorption of CO2 from CO2-N2 and CO2-CH4 gas mixtures with high CO2 loading.

    Science.gov (United States)

    Pal, Arun; Chand, Santanu; Elahi, Syed Meheboob; Das, Madhab C

    2017-11-14

    A microporous MOF {[Zn(SDB)(L) 0.5 ]·S} n (IITKGP-5) with a polar pore surface has been constructed by the combination of a V-shaped -SO 2 functionalized organic linker (H 2 SDB = 4,4'-sulfonyldibenzoic acid) with an N-rich spacer (L = 2,5-bis(3-pyridyl)-3,4-diaza-2,4-hexadiene), forming a network with sql(2,6L1) topology. IITKGP-5 is characterized by TGA, PXRD and single crystal X-ray diffraction. The framework exhibits lozenge-shaped channels of an approximate size of 4.2 × 5.6 Å 2 along the crystallographic b axis with a potential solvent accessible volume of 26%. The activated IITKGP-5a revealed a CO 2 uptake capacity of 56.4 and 49 cm 3 g -1 at 273 K/1 atm and 295 K/1 atm, respectively. On the contrary, it takes up a much smaller amount of CH 4 (17 cm 3 g -1 at 273 K and 13.6 cm 3 g -1 at 295 K) and N 2 (5.5 cm 3 g -1 at 273 K; 4 cm 3 g -1 at 295 K) under 1 atm pressure exhibiting its potential for a highly selective adsorption of CO 2 from flue gas as well as a landfill gas mixture. Based on the ideal adsorbed solution theory (IAST), a CO 2 /N 2 selectivity of 435.5 and a CO 2 /CH 4 selectivity of 151.6 have been realized at 273 K/100 kPa. The values at 295 K are 147.8 for CO 2 /N 2 and 23.8 for CO 2 /CH 4 gas mixtures under 100 kPa. In addition, this MOF nearly approaches the target values proposed for PSA and TSA processes for practical utility exhibiting its prospect for flue gas separation with a CO 2 loading capacity of 2.04 mmol g -1 .

  4. Correction: Large-scale electricity storage utilizing reversible solid oxide cells combined with underground storage of CO2 and CH4

    DEFF Research Database (Denmark)

    Jensen, Søren Højgaard; Graves, Christopher R.; Mogensen, Mogens Bjerg

    2017-01-01

    Correction for ‘Large-scale electricity storage utilizing reversible solid oxide cells combined with underground storage of CO2 and CH4’ by S. H. Jensen et al., Energy Environ. Sci., 2015, 8, 2471–2479.......Correction for ‘Large-scale electricity storage utilizing reversible solid oxide cells combined with underground storage of CO2 and CH4’ by S. H. Jensen et al., Energy Environ. Sci., 2015, 8, 2471–2479....

  5. Effect of CH4 on the CO2 breakthrough pressure and permeability of partially saturated low-permeability sandstone in the Ordos Basin, China

    Science.gov (United States)

    Zhao, Yan; Yu, Qingchun

    2018-01-01

    The behavior of CO2 that coexists with CH4 and the effect of CH4 on the CO2 stream need to be deeply analyzed and studied, especially in the presence of water. Our previous studies investigated the breakthrough pressure and permeability of pure CO2 in five partially saturated low-permeability sandstone core samples from the Ordos Basin, and we concluded that rocks with a small pore size and low permeability show considerable sealing capacity even under unsaturated conditions. In this paper, we selected three of these samples for CO2-CH4 gas-mixture breakthrough experiments under various degrees of water saturation. The breakthrough experiments were performed by increasing the gas pressure step by step until breakthrough occurred. Then, the effluent gas mixture was collected for chromatographic partitioning analysis. The results indicate that CH4 significantly affects the breakthrough pressure and permeability of CO2. The presence of CH4 in the gas mixture increases the interfacial tension and, thus, the breakthrough pressure. Therefore, the injected gas mixture that contains the highest (lowest) mole fraction of CH4 results in the largest (smallest) breakthrough pressure. The permeability of the gas mixture is greater than that for pure CO2 because of CH4, and the effective permeability decreases with increased breakthrough pressure. Chromatographic partitioning of the effluent mixture gases indicates that CH4 breaks through ahead of CO2 as a result of its weaker solubility in water. Correlations are established between (1) the breakthrough pressure and water saturation, (2) the effective permeability and water saturation, (3) the breakthrough pressure and effective permeability, and (4) the mole fraction of CO2/CH4 in the effluent mixture gases and water saturation. These results deepen our understanding of the multi-phase flow behavior in the porous media under unsaturated conditions, which have implications for formulating emergency response plans for gas

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

    KAUST Repository

    Wang, Weizong

    2018-01-18

    Due to the unique properties of plasma technology, its use in gas conversion applications is gaining significant interest around the globe. Plasma-based CO2 and CH4 conversion have become major research areas. Many investigations have already been 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 hydrogenation (CO2/H2), and even first steps towards the influence of N2 impurities have been taken, i.e. CO2/N2 and CH4/N2. In this feature article we briefly discuss the advances made in literature for these different steps from a plasma chemistry modeling point of view. Subsequently, we present a comprehensive plasma chemistry set, combining the knowledge gathered in this field so far, and supported with extensive experimental data. This set can be used for chemical kinetics plasma modeling for all possible combinations of CO2, CH4, N2, O2 and H2O, to investigate the bigger picture of the underlying plasmachemical pathways for these mixtures in a dielectric barrier discharge plasma. This is extremely valuable for the optimization of existing plasma-based CO2 conversion and CH4 reforming processes, as well as for investigating the influence of N2, O2 and H2O on these processes, and even to support plasma-based multi-reforming processes.

  7. Release of N 2, CH 4, CO 2, and H 2O from surface ices on Enceladus

    Science.gov (United States)

    Hodyss, Robert; Goguen, Jay D.; Johnson, Paul V.; Campbell, Colin; Kanik, Isik

    2008-09-01

    We vapor deposit at 20 K a mixture of gases with the specific Enceladus plume composition measured in situ by the Cassini INMS [Waite, J.H., Combi, M.R., Ip, W.H., Cravens, T.E., McNutt, R.L., Kasprzak, W., Yelle, R., Luhmann, J., Niemann, H., Gell, D., Magee, B., Fletcher, G., Lunine, J., Tseng, W.L., 2006. Science 311, 1419-1422] to form a mixed molecular ice. As the sample is slowly warmed, we monitor the escaping gas quantity and composition with a mass spectrometer. Pioneering studies [Schmitt, B., Klinger, J., 1987. Different trapping mechanisms of gases by water ice and their relevance for comet nuclei. In: Rolfe, E.J., Battrick, B. (Eds.), Diversity and Similarity of Comets. SP-278. ESA, Noordwijk, The Netherlands, pp. 613-619; Bar-Nun, A., Kleinfeld, I., Kochavi, E., 1988. Phys. Rev. B 38, 7749-7754; Bar-Nun, A., Kleinfeld, I., 1989. Icarus 80, 243-253] have shown that significant quantities of volatile gases can be trapped in a water ice matrix well above the temperature at which the pure volatile ice would sublime. For our Enceladus ice mixture, a composition of escaping gases similar to that detected by Cassini in the Enceladus plume can be generated by the sublimation of the H 2O:CO 2:CH 4:N 2 mixture at temperatures between 135 and 155 K, comparable to the high temperatures inferred from the CIRS measurements [Spencer, J.R., Pearl, J.C., Segura, M., Flasar, F.M., Mamoutkine, A., Romani, P., Buratti, B.J., Hendrix, A.R., Spilker, L.J., Lopes, R.M.C., 2006. Science 311, 1401-1405] of the Enceladus "tiger stripes." This suggests that the gas escape phenomena that we measure in our experiments are an important process contributing to the gases emitted from Enceladus. A similar experiment for ice deposited at 70 K shows that both the processes of volatile trapping and release are temperature dependent over the temperature range relevant to Enceladus.

  8. Adsorption kinetics of CO2, CH4, and their equimolar mixture on coal from the Black Warrior Basin, West-Central Alabama

    Science.gov (United States)

    Gruszkiewicz, M.S.; Naney, M.T.; Blencoe, J.G.; Cole, D.R.; Pashin, J.C.; Carroll, R.E.

    2009-01-01

    Laboratory experiments were conducted to investigate the adsorption kinetic behavior of pure and mixed gases (CO2, CH4, approximately equimolar CO2 + CH4 mixtures, and He) on a coal sample obtained from the Black Warrior Basin at the Littleton Mine (Twin Pine Coal Company), Jefferson County, west-central Alabama. The sample was from the Mary Lee coal zone of the Pottsville Formation (Lower Pennsylvanian). Experiments with three size fractions (45-150????m, 1-2??mm, and 5-10??mm) of crushed coal were performed at 40????C and 35????C over a pressure range of 1.4-6.9??MPa to simulate coalbed methane reservoir conditions in the Black Warrior Basin and provide data relevant for enhanced coalbed methane recovery operations. The following key observations were made: (1) CO2 adsorption on both dry and water-saturated coal is much more rapid than CH4 adsorption; (2) water saturation decreases the rates of CO2 and CH4 adsorption on coal surfaces, but it appears to have minimal effects on the final magnitude of CO2 or CH4 adsorption if the coal is not previously exposed to CO2; (3) retention of adsorbed CO2 on coal surfaces is significant even with extreme pressure cycling; and (4) adsorption is significantly faster for the 45-150????m size fraction compared to the two coarser fractions. ?? 2008 Elsevier B.V.

  9. Pure- and mixed-gas CO2/CH4 separation properties of PIM-1 and an amidoxime-functionalized PIM-1

    KAUST Repository

    Swaidan, Raja

    2014-05-01

    The prototypical solution-processable polymer of intrinsic microporosity, PIM-1, and derivatives thereof offer combinations of permeability and selectivity that make them potential candidate materials for membrane-based gas separations. Paramount to the design and evaluation of PIMs for economical natural gas sweetening is a high and stable CO2/CH4 selectivity under realistic, mixed-gas conditions. Here, amidoxime-functionalized PIM-1 (AO-PIM-1) was prepared and examined for fundamental structure/property relationships. Qualitative NLDFT pore-size distribution analyses of physisorption isotherms (N2 at -196 oC; CO2 at 0 oC) reveal a tightened microstructure indicating size-sieving ultra-microporosity (<7Å). AO-PIM-1 demonstrated a three-fold increase in αD(CO2/CH4) over PIM-1, surpassing the 2008 upper bound with P(CO2)=1153Barrer and ideal α(CO2/CH4)=34. Under a 50:50 CO2:CH4 mixed-gas feed, AO-PIM-1 showed less selectivity loss than PIM-1, maintaining a mixed-gas α(CO2/CH4) ~21 across a 20bar pressure range. Conversely, PIM-1 endured up to 60% increases in mixed-gas CH4 permeability over pure-gas values concurrent with a selectivity of only ~8 at 20bar. A pervasive intermolecular hydrogen bonding network in AO-PIM-1 predominantly yields a rigidified microstructure that mitigates CO2-induced matrix dilations, reducing detrimental mixed-gas CH4 copermeation. © 2014 Elsevier B.V.

  10. A porous Cd(II) metal-organic framework with high adsorption selectivity for CO2 over CH4

    Science.gov (United States)

    Zhu, Chunlan

    2017-05-01

    Metal-organic frameworks (MOFs) have attracted a lot of attention in recent decades. We applied a semi-rigid four-carboxylic acid linker to assemble with Cd(II) ions to generate a novel microporous Cd(II) MOF material. Single crystal X-ray diffraction study reveals the different two dimension (2D) layers can be further packed together with an AB fashion by hydrogen bonds (O4sbnd H4⋯O7 = 1.863 Å) to construct a three dimension (3D) supermolecular architecture. The resulting sample can be synthesized under solvothermal reactions successfully, which exhibits high selectivity adsorption of CO2 over CH4 at room temperature. In addition, the obtained sample was characterized by thermal gravimetric analyses (TGA), Fourier-transform infrared spectra (FT-IR), elemental analysis (CHN) and powder X-ray diffraction (PXRD).

  11. Sorption Behavior of CO2 and CH4 of Glassy Polymeric Membranes and Analytical Discussion of Partial Immobilization Model

    Directory of Open Access Journals (Sweden)

    M. Mahdavian

    2007-06-01

    Full Text Available Among various reported membrane-based gas separation processes, the best explanation is generally achieved by the solution-diffusion model. The main factors in this model are the solubility and diffusivity of permeationcomponents through the membrane. The prediction of permeability and diffusivity in multicomponent gas permeation as well as the separation evaluation equilibrium and kinetic interactions requires a proper explanation of sorption and diffusion phenomena in the polymer matrix. Investigation made by various researchers in this area shows that the equilibrium interaction (sorption step plays the key role in determining diffusion and permeation in multicomponent system. Therefore, the proper description of sorption behaviour of gas mixture in the polymer is an essential task. The dual-mode sorption (Langmuir-Henry is usually used for the description of equilibrium isotherm of gases in glassy polymers based on this model; the diffusive behaviour of the system is subsequently analyzed by the partial immobilization model. In this study, the equilibrium sorption of CO2/CH4 mixture in various polymers was modelled using the experimental data available in the literature. The differences in the mechanism of adsorption for CO2 and CH4 were analyzed by considering variations in mode of sorption for each adsorbed component at different pressures. By introducing a new adsorption parameter, P50/50, (the pressure at which the portion of two modes in sorption are equal the contribution of each adsorbed component in occupying Langmuir sites was evaluated. The results indicate that the relative significance of sorption mode for each component is a function of pressure and it is different for various polymers.

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

    Energy Technology Data Exchange (ETDEWEB)

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

    2009-01-09

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

  13. The effect of CO2, H2O and SO2 on the kinetics of NO reduction by CH4 over La2O3

    International Nuclear Information System (INIS)

    Toops, Todd J.; Walters, Arden B.; Vannice, M.A.

    2002-01-01

    The effect of CO 2 , H 2 O and SO 2 on the kinetics of NO reduction by CH 4 over unsupported La 2 O 3 has been examined between 773 and 973K in the presence of O 2 in the feed. La 2 O 3 can maintain a stable, high specific activity (mol/(sm 2 )) for NO reduction with high concentrations of CO 2 and H 2 O in the feed; however, either of these two products reversibly inhibits the activity by about one-half in the presence of excess O 2 . The catalyst is poisoned by SO 2 at these temperatures and an oxysulfate phase is formed, but partial regeneration can be achieved at 1023K. CO 2 in the feed causes the formation of lanthanum oxycarbonate, which reverts to La 2 O 3 when CO 2 is removed, but no bulk La oxyhydroxide is detected after quenching with H 2 O in the feed. The influence of CO 2 and H 2 O on kinetic behavior can be described by assuming they compete with reactants for adsorption on surface sites, including them in the site balance equation, and using the rate expression proposed previously for NO reduction by CH 4 in excess O 2 . With O 2 in the feed, integral conversions of CH 4 and O 2 frequently occurred due to the direct combustion of CH 4 by O 2 , although NO conversions remained differential; thus, an integral reactor model was chosen to analyze the data which utilized a recently determined rate equation for CH 4 combustion on La 2 O 3 in conjunction with a previously proposed model for NO reduction by CH 4 . The following rate expression described the rate of N 2 formation: N 2 T = ' NO P NO P CH 4 P O 2 0.5 / 1 + K NO P NO + K CH 4 P CH 4 + K O 2 0.5 P O 2 0.5 + K CO 2 P CO 2 + K H 2 O P H 2 O 2 . It gave a good fit to the experimental rate data for NO reduction, as well as providing enthalpies and entropies of adsorption obtained from the fitting parameters that demonstrated thermodynamic consistency and were similar to previous values. The heats of adsorption were altered somewhat when either CO 2 or H 2 O was added to the feed, and the following

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

    DEFF Research Database (Denmark)

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

    2007-01-01

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

  15. Quantification of CO2 and CH4 megacity emissions using portable solar absorption spectrometers

    Science.gov (United States)

    Frey, Matthias; Hase, Frank; Blumenstock, Thomas; Morino, Isamu; Shiomi, Kei

    2017-04-01

    Urban areas already contribute to over 50% of the global population, additionally the percentage of the worldwide population living in Metropolitan areas is continuously growing. Thus, a precise knowledge of urban greenhouse gas (GHG) emissions is of utmost importance. Whereas, however, GHG emissions on a nationwide to continental scale can be relatively precisely estimated using satellite observations (and fossil fuel consumption statistics), reliable estimations for local to regional scale emissions pose a bigger problem due to lack of timely and spatially high resolved satellite data and possible biases of passive spectroscopic nadir observations (e.g. enhanced aerosol scattering in a city plume). Furthermore, emission inventories on the city scale might be missing contributions (e.g. methane leakage from gas pipes). Here, newly developed mobile low resolution Fourier Transform spectrometers (Bruker EM27/SUN) are utilized to quantify small scale emissions. This novel technique was successfully tested before by KIT and partners during campaigns in Berlin, Paris and Colorado for detecting emissions from various sources. We present results from a campaign carried out in February - April 2016 in the Tokyo bay area, one of the biggest Metropolitan areas worldwide. We positioned two EM27/SUN spectrometers on the outer perimeter of Tokyo along the prevailing wind axis upwind and downwind of the city source. Before and after the campaign, calibration measurements were performed in Tsukuba with a collocated high resolution FTIR spectrometer from the Total Carbon Column Observing Network (TCCON). During the campaign the observed XCO2 and XCH4 values vary significantly. Additionally, intraday variations are observed at both sites. Furthermore, an enhancement due to the Tokyo area GHG emissions is clearly visible for both XCO2 and XCH4. The observed signals are significantly higher compared to prior campaigns targeting other major cities. We perform a rough estimate of the

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

    Science.gov (United States)

    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.

  17. A procedure to find thermodynamic equilibrium constants for CO2 and CH4 adsorption on activated carbon.

    Science.gov (United States)

    Trinh, T T; van Erp, T S; Bedeaux, D; Kjelstrup, S; Grande, C A

    2015-03-28

    Thermodynamic equilibrium for adsorption means that the chemical potential of gas and adsorbed phase are equal. A precise knowledge of the chemical potential is, however, often lacking, because the activity coefficient of the adsorbate is not known. Adsorption isotherms are therefore commonly fitted to ideal models such as the Langmuir, Sips or Henry models. We propose here a new procedure to find the activity coefficient and the equilibrium constant for adsorption which uses the thermodynamic factor. Instead of fitting the data to a model, we calculate the thermodynamic factor and use this to find first the activity coefficient. We show, using published molecular simulation data, how this procedure gives the thermodynamic equilibrium constant and enthalpies of adsorption for CO2(g) on graphite. We also use published experimental data to find similar thermodynamic properties of CO2(g) and of CH4(g) adsorbed on activated carbon. The procedure gives a higher accuracy in the determination of enthalpies of adsorption than ideal models do.

  18. Fluid geochemistry and soil gas fluxes (CO2-CH4-H2S) at a promissory Hot Dry Rock Geothermal System: The Acoculco caldera, Mexico

    Science.gov (United States)

    Peiffer, L.; Bernard-Romero, R.; Mazot, A.; Taran, Y. A.; Guevara, M.; Santoyo, E.

    2014-09-01

    The Acoculco caldera has been recognized by the Mexican Federal Electricity Company (CFE) as a Hot Dry Rock Geothermal System (HDR) and could be a potential candidate for developing an Enhanced Geothermal System (EGS). Apart from hydrothermally altered rocks, geothermal manifestations within the Acoculco caldera are scarce. Close to ambient temperature bubbling springs and soil degassing are reported inside the caldera while a few springs discharge warm water on the periphery of the caldera. In this study, we infer the origin of fluids and we characterize for the first time the soil degassing dynamic. Chemical and isotopic (δ18O-δD) analyses of spring waters indicate a meteoric origin and the dissolution of CO2 and H2S gases, while gas chemical and isotopic compositions (N2/He, 3He/4He, 13C, 15N) reveal a magmatic contribution with both MORB- and arc-type signatures which could be explained by an extension regime created by local and regional fault systems. Gas geothermometry results are in agreement with temperature measured during well drilling (260 °C-300 °C). Absence of well-developed water reservoir at depth impedes re-equilibration of gases upon surface. A multi-gas flux survey including CO2, CH4 and H2S measurements was performed within the caldera. Using the graphical statistical analysis (GSA) approach, CO2 flux measurements were classified in two populations. Population A, representing 95% of measured fluxes is characterized by low values (mean: 18 g m- 2 day- 1) while the remaining 5% fluxes belonging to Population B are much higher (mean: 5543 g m- 2 day- 1). This low degassing rate probably reflects the low permeability of the system, a consequence of the intense hydrothermal alteration observed in the upper 800 m of volcanic rocks. An attempt to interpret the origin and transport mechanism of these fluxes is proposed by means of flux ratios as well as by numerical modeling. Measurements with CO2/CH4 and CO2/H2S flux ratios similar to mass ratios

  19. Emission factors and their uncertainty for the exchange of CO2, CH4 and N2O in Finnish managed peatlands

    International Nuclear Information System (INIS)

    Alm, J.; Shurpali, N. J.; Minkkinen, K.

    2007-01-01

    This paper summarises the results of several research groups participating in the research programme 'Greenhouse Impacts of the use of Peat and Peatlands in Finland', and presents emission factors for peat-atmosphere fluxes of CO 2 , CH 4 , and N 2 O, filling gaps in knowledge concerning the afforestation of organic croplands and cutaways, and improves the emission assessment of peatlands drained for forestry. Forest drainage may result in net binding of soil carbon or net release, depending on site characteristics and the tree stand. Use of peatlands for agriculture (48-4821 g CO 2 -eq. m -2 a -1 ), even after the cultivation has ceased, or for milled peat harvesting (1948-2478 g CO 2 -eq. m -2 a -1 ) can cause the highest overall emissions. Extremely high CO 2 emissions are possible from peat harvesting areas during wet and warm summers. Afforestation of those peatlands abandoned from cultivation or peat harvesting can reduce the warming impact at least during the first tree generation. Heterotrophic soil respiration may have a systematic south-north difference in temperature response. More data must be collected before the information on peatland forest soil CO 2 emissions can be adapted for different climatic regions in Finland. A test of the model DNDC against measured data showed that DNDC has to be developed further before it can be used in estimating N 2 O emissions from boreal peatlands. (orig.)

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

    Science.gov (United States)

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

    2018-02-01

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

  1. Molecular Dynamics Simulations for Loading-Dependent Diffusion of CO2, SO2, CH4, and Their Binary Mixtures in ZIF-10: The Role of Hydrogen Bond.

    Science.gov (United States)

    Li, Li; Yang, Deshuai; Fisher, Trevor R; Qiao, Qi; Yang, Zhen; Hu, Na; Chen, Xiangshu; Huang, Liangliang

    2017-10-24

    The loading-dependent diffusion behavior of CH 4 , CO 2 , SO 2 , and their binary mixtures in ZIF-10 has been investigated in detail by using classical molecular dynamics simulations. Our simulation results demonstrate that the self-diffusion coefficient D i of CH 4 molecules decreases sharply and monotonically with the loading while those of both CO 2 and SO 2 molecules initially display a slight increase at low uptakes and follow a slow decrease at high uptakes. Accordingly, the interaction energies between CH 4 molecules and ZIF-10 remain nearly constant regardless of the loading due to the absence of hydrogen bonds (HBs), while the interaction energies between CO 2 (or SO 2 ) and ZIF-10 decease rapidly with the loading, especially at small amounts of gas molecules. Such different loading-dependent diffusion and interaction mechanisms can be attributed to the relevant HB behavior between gas molecules and ZIF-10. At low loadings, both the number and strength of HBs between CO 2 (or SO 2 ) molecules and ZIF-10 decrease obviously as the loading increases, which is responsible for the slight increase of their diffusion coefficients. However, at high loadings, their HB strength increases with the loading. Similar loading-dependent phenomena of diffusion, interaction, and HB behavior can be observed for CH 4, CO 2 , and SO 2 binary mixtures in ZIF-10, only associated with some HB competition between CO 2 and SO 2 molecules in the case of the CO 2 /SO 2 mixture.

  2. Small scale soil carbon and moisture gradients in a drained peat bog grassland and their influence on CO2, CH4 and N2O fluxes

    Science.gov (United States)

    Leiber-Sauheitl, K.; Fuß, R.; Freibauer, A.

    2012-04-01

    Due to the UNFCCC report requirements of each country on the emissions of greenhouse gases from key sources the joint research project "Organic Soils" was established in Germany. The project's objective is to improve the data set on greenhousegas emissions from organic soils in Germany. Within 12 German Project Catchments emissions from different types of organic soils, e.g. under different land uses and hydrological conditions, are measured. At the location "Großes Moor" near Gifhorn (Lower Saxony) the effects of small-scale soil organic carbon and groundwater level gradients on the GHG fluxes (CO2, CH4 and N2O) are quantified. The study area is located within a former peat bog altered by drainage and peat cutting, which is currently grassland under extensive agricultural use. The focus of the study is on the acquisition of CO2, CH4 and N2O fluxes on six sites via manual closed chambers. In order to calculate the annual CO2 exchange rate, values are interpolated on a 0.5 hour scale between measurement campaigns. In combination with continually logged meteorological parameters, such as the photosynthetic active radiation as well as air and soil temperatures, we calculate the daily CO2 ecosystem exchange of the different sites. During the 2011 campaign, CO2 was determined as the most important greenhouse gas. The groundwater table was the dominant variable influencing gas emissions. Another important factor was the vegetation composition. In detail, highest CO2 emissions occurred with a water table of 40-50 cm below ground level, temperatures above 10°C and low plant biomass amounts. Due to the more complex formation of N2O by a number of processes, each being promoted by different soil conditions, the measurement of N2O fluxes in the field was complemented by a laboratory experiment. In this, the use of stable isotope tracer techniques enabled us to quantify the contribution of single biochemical pathways to the overall formation of N2O under controlled

  3. Effect of Amine-Functionalized MIL-53 Metal Organic Frameworks on the Performance of Poly(4-methyl-1-pentyne Membrane in CO2/CH4 Separation Gas Mixture

    Directory of Open Access Journals (Sweden)

    Reza Abedini

    2015-06-01

    Full Text Available The effect of NH2-MIL 53 metal organic framework (MOF on gas transport properties of poly(4-methyl-1-pentyne (PMP was investigated. Various characterization methods such as FTIR, DSC, SEM and gas adsorption test as well as a series of CO2/CH4 gas separation tests (i.e., pure and mixed gas test were conducted in order to determine the effect of ligand functionalization (–NH2 on the properties of the prepared mixed matrix membranes and their gas transport characteristics. The results of DSC showed that glass transition temperature (Tg increased by increasing NH2-MIL 53 loading. The SEM images also demonstrated that the NH2-MIL 53 particles were dispersed well in the PMP matrix with no noticeable agglomeration. The gas adsorption test of NH2-MIL 53 particles revealed there was a selective adsorption behavior with respect to CO2. It was also found that, incorporation of NH2-MIL 53 into the PMP resulted in an increase in gas permeability (especially towards CO2 and a higher CO2/CH4 selectivity. Adding 30 wt% NH2-MIL 53 into the polymer matrix increased CO2 permeability and CO2/CH4 selectivity of the mixed gas from 83.35 to 210.21 barrer and 7.61 to 19.88, respectively. Rising the temperature from 30 to 60°C led to the permeability increment of both CO2 and CH4 in the mixed gas test, while the CO2/CH4 selectivity decreased. Moreover, the results showed that amino groups required no regeneration and their performance did not decline during 120 h of permeation test. A comparison between the permeation data and those calculated from permeation models revealed that the Bruggeman model could fit the CO2 permeability data better than the Maxwell and Lewis models.

  4. Edaphic factors controlling summer (rainy season) greenhouse gas emissions (CO2 and CH4) from semiarid mangrove soils (NE-Brazil).

    Science.gov (United States)

    Nóbrega, Gabriel N; Ferreira, Tiago O; Siqueira Neto, M; Queiroz, Hermano M; Artur, Adriana G; Mendonça, Eduardo De S; Silva, Ebenezer De O; Otero, Xosé L

    2016-01-15

    The soil attributes controlling the CO2, and CH4 emissions were assessed in semiarid mangrove soils (NE-Brazil) under different anthropogenic activities. Soil samples were collected from different mangroves under different anthropogenic impacts, e.g., shrimp farming (Jaguaribe River); urban wastes (Cocó River) and a control site (Timonha River). The sites were characterized according to the sand content; physicochemical parameters (Eh and pH); total organic C; soil C stock (SCS) and equivalent SCS (SCSEQV); total P and N; dissolved organic C (DOC); and the degree of pyritization (DOP). The CO2 and CH4 fluxes from the soils were assessed using static closed chambers. Higher DOC and SCS and the lowest DOP promote greater CO2 emission. The CH4 flux was only observed at Jaguaribe which presented higher DOP, compared to that found in mangroves from humid tropical climates. Semiarid mangrove soils cannot be characterized as important greenhouse gas sources, compared to humid tropical mangroves.

  5. Fabrication of 6FDA-durene membrane incorporated with zeolite T and aminosilane grafted zeolite T for CO2/CH4 separation

    Science.gov (United States)

    Jusoh, Norwahyu; Fong Yeong, Yin; Keong Lau, Kok; Shariff, Azmi Mohd

    2017-08-01

    In the present work, zeolite T and aminosilane grafted zeolite T are embedded into 6FDA-durene polyimide phase for the fabrication of mixed matrix membranes (MMMs). FESEM images demonstrated that the improvement of interfacial adhesion between zeolite and polymer phases in MMM loaded with aminosilane grafted zeolite T was not significant as compared to zeolite T/6FDA-durene MMM. From the gas permeation test, CO2/CH4 selectivity up to 26.4 was achieved using MMM containing aminosilane grafted zeolite T, while MMM loaded with ungrafted zeolite T showed CO2/CH4 selectivity of 19.1. In addition, MMM incorporated with aminosilane grafted zeolite T particles successfully lies on Robeson upper bound 2008, which makes it an attractive candidate for CO2/CH4 separation.

  6. Annual emissions of CO2, CH4 and N2O from a temperate peat bog: Comparison of an undrained and four drained sites under permanent grass and arable crop rotations with cereals and potato

    DEFF Research Database (Denmark)

    Kandel, Tanka; Lærke, Poul Erik; Elsgaard, Lars

    2018-01-01

    intervals using static chambers, and auxiliary data were obtained, such as temperature, depth of water table, ratio-vegetation index, pH and soil mineral N. Annual CO2 emissions were derived from empirical modelling, whereas CH4 and N2O emissions were linearly interpolated between measurement dates...

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

    Science.gov (United States)

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

    2017-12-01

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

  8. Analysis of top-down and bottom-up North American CO2 and CH4 emissions estimates in the second State of the Carbon Cycle Report

    Science.gov (United States)

    Miller, J. B.; Jacobson, A. R.; Bruhwiler, L.; Michalak, A.; Hayes, D. J.; Vargas, R.

    2017-12-01

    In just ten years since publication of the original State of the Carbon Cycle Report in 2007, global CO2 concentrations have risen by more than 22 ppm to 405 ppm. This represents 18% of the increase over preindustrial levels of 280 ppm. This increase is being driven unequivocally by fossil fuel combustion with North American emissions comprising roughly 20% of the global total over the past decade. At the global scale, we know by comparing well-known fossil fuel inventories and rates of atmospheric CO2 increase that about half of all emissions are absorbed at Earth's surface. For North America, however, we can not apply a simple mass balance to determine sources and sinks. Instead, contributions from ecosystems must be estimated using top-down and bottom-up methods. SOCCR-2 estimates North American net CO2 uptake from ecosystems using bottom-up (inventory) methods as 577 +/- 433 TgC/yr and 634 +/- 288 TgC/yr from top-down atmospheric inversions. Although the global terrestrial carbon sink is not precisely known, these values represent possibly 30% of the global values. As with net sink estimates reported in SOCCR, these new top-down and bottom-up estimates are statistically consistent with one another. However, the uncertainties on each of these estimates are now substantially smaller, giving us more confidence about where the truth lies. Atmospheric inversions also yield estimates of interannual variations (IAV) in CO2 and CH4 fluxes. Our syntheses suggest that IAV of ecosystem CO2 fluxes is of order 100 TgC/yr, mainly originating in the conterminous US, with lower variability in boreal and arctic regions. Moreover, this variability is much larger than for inventory-based fluxes reported by the US to the UNFCCC. Unlike CO2, bottom-up CH4 emissions are larger than those derived from large-scale atmospheric data, with the continental discrepancy resulting primarily from differences in arctic and boreal regions. In addition to the current state of the science, we

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

    DEFF Research Database (Denmark)

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

    Science.gov (United States)

    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.

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

    Directory of Open Access Journals (Sweden)

    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.

  12. Atmospheric CH4 and CO2 enhancements and biomass burning emission ratios derived from satellite observations of the 2015 Indonesian fire plumes

    Directory of Open Access Journals (Sweden)

    R. J. Parker

    2016-08-01

    subsequent large increases in regional greenhouse gas concentrations. CH4 is particularly enhanced, due to the dominance of smouldering combustion in peatland fires, with CH4 total column values typically exceeding 35 ppb above those of background “clean air” soundings. By examining the CH4 and CO2 excess concentrations in the fire-affected GOSAT observations, we determine the CH4 to CO2 (CH4 ∕ CO2 fire emission ratio for the entire 2-month period of the most extreme burning (September–October 2015, and also for individual shorter periods where the fire activity temporarily peaks. We demonstrate that the overall CH4 to CO2 emission ratio (ER for fires occurring in Indonesia over this time is 6.2 ppb ppm−1. This is higher than that found over both the Amazon (5.1 ppb ppm−1 and southern Africa (4.4 ppb ppm−1, consistent with the Indonesian fires being characterised by an increased amount of smouldering combustion due to the large amount of organic soil (peat burning involved. We find the range of our satellite-derived Indonesian ERs (6.18–13.6 ppb ppm−1 to be relatively closely matched to that of a series of close-to-source, ground-based sampling measurements made on Kalimantan at the height of the fire event (7.53–19.67 ppb ppm−1, although typically the satellite-derived quantities are slightly lower on average. This seems likely because our field sampling mostly intersected smaller-scale peat-burning plumes, whereas the large-scale plumes intersected by the GOSAT Thermal And Near infrared Sensor for carbon Observation – Fourier Transform Spectrometer (TANSO-FTS footprints would very likely come from burning that was occurring in a mixture of fuels that included peat, tropical forest and already-cleared areas of forest characterised by more fire-prone vegetation types than the natural rainforest biome (e.g. post-fire areas of ferns and scrubland, along with agricultural vegetation.The ability to determine large-scale ERs from

  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

    Science.gov (United States)

    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. Hydraulic and Mechanical Effects from Gas Hydrate Conversion and Secondary Gas Hydrate Formation during Injection of CO2 into CH4-Hydrate-Bearing Sediments

    Science.gov (United States)

    Bigalke, N.; Deusner, C.; Kossel, E.; Schicks, J. M.; Spangenberg, E.; Priegnitz, M.; Heeschen, K. U.; Abendroth, S.; Thaler, J.; Haeckel, M.

    2014-12-01

    The injection of CO2 into CH4-hydrate-bearing sediments has the potential to drive natural gas production and simultaneously sequester CO2 by hydrate conversion. The process aims at maintaining the in situ hydrate saturation and structure and causing limited impact on soil hydraulic properties and geomechanical stability. However, to increase hydrate conversion yields and rates it must potentially be assisted by thermal stimulation or depressurization. Further, secondary formation of CO2-rich hydrates from pore water and injected CO2 enhances hydrate conversion and CH4 production yields [1]. Technical stimulation and secondary hydrate formation add significant complexity to the bulk conversion process resulting in spatial and temporal effects on hydraulic and geomechanical properties that cannot be predicted by current reservoir simulation codes. In a combined experimental and numerical approach, it is our objective to elucidate both hydraulic and mechanical effects of CO2 injection and CH4-CO2-hydrate conversion in CH4-hydrate bearing soils. For the experimental approach we used various high-pressure flow-through systems equipped with different online and in situ monitoring tools (e.g. Raman microscopy, MRI and ERT). One particular focus was the design of triaxial cell experimental systems, which enable us to study sample behavior even during large deformations and particle flow. We present results from various flow-through high-pressure experimental studies on different scales, which indicate that hydraulic and geomechanical properties of hydrate-bearing sediments are drastically altered during and after injection of CO2. We discuss the results in light of the competing processes of hydrate dissociation, hydrate conversion and secondary hydrate formation. Our results will also contribute to the understanding of effects of temperature and pressure changes leading to dissociation of gas hydrates in ocean and permafrost systems. [1] Deusner C, Bigalke N, Kossel E

  15. Edaphic factors controlling summer (rainy season) greenhouse gas emissions (CO_2 and CH_4) from semiarid mangrove soils (NE-Brazil)

    International Nuclear Information System (INIS)

    Nóbrega, Gabriel N.; Ferreira, Tiago O.; Siqueira Neto, M.; Queiroz, Hermano M.; Artur, Adriana G.; Mendonça, Eduardo De S.; Silva, Ebenezer De O.

    2016-01-01

    The soil attributes controlling the CO_2, and CH_4 emissions were assessed in semiarid mangrove soils (NE-Brazil) under different anthropogenic activities. Soil samples were collected from different mangroves under different anthropogenic impacts, e.g., shrimp farming (Jaguaribe River); urban wastes (Cocó River) and a control site (Timonha River). The sites were characterized according to the sand content; physicochemical parameters (Eh and pH); total organic C; soil C stock (SCS) and equivalent SCS (SCS_E_Q_V); total P and N; dissolved organic C (DOC); and the degree of pyritization (DOP). The CO_2 and CH_4 fluxes from the soils were assessed using static closed chambers. Higher DOC and SCS and the lowest DOP promote greater CO_2 emission. The CH_4 flux was only observed at Jaguaribe which presented higher DOP, compared to that found in mangroves from humid tropical climates. Semiarid mangrove soils cannot be characterized as important greenhouse gas sources, compared to humid tropical mangroves. - Highlights: • GHG emission was associated with different soil characteristics. • Highest CO_2 emissions were found in mangroves with larger dissolved C and lower DOP. • Less CH_4 flux was due to low DOP in semiarid mangrove soils.

  16. Investigating cluster formation in adsorption of CO2, CH4, and Ar in zeolites and metal organic frameworks at subcritical temperatures

    NARCIS (Netherlands)

    Krishna, R.; van Baten, J.M.

    2010-01-01

    The critical temperatures, T-c, of CO2, CH4, and Ar are 304 K, 191 K, and 151 K, respectively. This paper highlights some unusual characteristics of adsorption and diffusion of these molecules in microporous structures such as zeolites and metal organic frameworks at temperatures T < T-c. Published

  17. Effects of tillage and nitrogen fertilizers on CH4 and CO2 emissions and soil organic carbon in paddy fields of central China.

    Directory of Open Access Journals (Sweden)

    Li Cheng-Fang

    Full Text Available Quantifying carbon (C sequestration in paddy soils is necessary to help better understand the effect of agricultural practices on the C cycle. The objective of the present study was to assess the effects of tillage practices [conventional tillage (CT and no-tillage (NT] and the application of nitrogen (N fertilizer (0 and 210 kg N ha(-1 on fluxes of CH(4 and CO(2, and soil organic C (SOC sequestration during the 2009 and 2010 rice growing seasons in central China. Application of N fertilizer significantly increased CH(4 emissions by 13%-66% and SOC by 21%-94% irrespective of soil sampling depths, but had no effect on CO(2 emissions in either year. Tillage significantly affected CH(4 and CO(2 emissions, where NT significantly decreased CH(4 emissions by 10%-36% but increased CO(2 emissions by 22%-40% in both years. The effects of tillage on the SOC varied with the depth of soil sampling. NT significantly increased the SOC by 7%-48% in the 0-5 cm layer compared with CT. However, there was no significant difference in the SOC between NT and CT across the entire 0-20 cm layer. Hence, our results suggest that the potential of SOC sequestration in NT paddy fields may be overestimated in central China if only surface soil samples are considered.

  18. Pure- and mixed-gas CO2/CH4 separation properties of PIM-1 and an amidoxime-functionalized PIM-1

    KAUST Repository

    Swaidan, Raja; Ghanem, Bader; Litwiller, Eric; Pinnau, Ingo

    2014-01-01

    to the design and evaluation of PIMs for economical natural gas sweetening is a high and stable CO2/CH4 selectivity under realistic, mixed-gas conditions. Here, amidoxime-functionalized PIM-1 (AO-PIM-1) was prepared and examined for fundamental structure

  19. Effects of tillage and nitrogen fertilizers on CH4 and CO2 emissions and soil organic carbon in paddy fields of central China.

    Science.gov (United States)

    Cheng-Fang, Li; Dan-Na, Zhou; Zhi-Kui, Kou; Zhi-Sheng, Zhang; Jin-Ping, Wang; Ming-Li, Cai; Cou-Gui, Cao

    2012-01-01

    Quantifying carbon (C) sequestration in paddy soils is necessary to help better understand the effect of agricultural practices on the C cycle. The objective of the present study was to assess the effects of tillage practices [conventional tillage (CT) and no-tillage (NT)] and the application of nitrogen (N) fertilizer (0 and 210 kg N ha(-1)) on fluxes of CH(4) and CO(2), and soil organic C (SOC) sequestration during the 2009 and 2010 rice growing seasons in central China. Application of N fertilizer significantly increased CH(4) emissions by 13%-66% and SOC by 21%-94% irrespective of soil sampling depths, but had no effect on CO(2) emissions in either year. Tillage significantly affected CH(4) and CO(2) emissions, where NT significantly decreased CH(4) emissions by 10%-36% but increased CO(2) emissions by 22%-40% in both years. The effects of tillage on the SOC varied with the depth of soil sampling. NT significantly increased the SOC by 7%-48% in the 0-5 cm layer compared with CT. However, there was no significant difference in the SOC between NT and CT across the entire 0-20 cm layer. Hence, our results suggest that the potential of SOC sequestration in NT paddy fields may be overestimated in central China if only surface soil samples are considered.

  20. Role of intrachain rigidity in the plasticization of intrinsically microporous triptycene-based polyimide membranes in mixed-Gas CO2/CH4 separations

    KAUST Repository

    Swaidan, Raja

    2014-11-11

    Based on high-pressure pure- and mixed-gas (50:50) CO2/CH4 separation properties of two intrinsically microporous triptycene-based polyimides (TPDA-TMPD and TPDA-6FpDA), the intrachain rigidity central to "conventional PIM" design principles is not a singular solution to intrinsic plasticization resistance. Despite the significant intrachain rigidity in TPDA-TMPD, a 300% increase in PMIX(CH4), 50% decrease in α(CO2/CH4) from 24 to 12, and continuous increase in PMIX(CO2) occurred from 4 to 30 bar. On the other hand, the more flexible and densely packed TPDA-6FpDA exhibited a slight upturn in PMIX(CO2) at 20 bar similar to a dense cellulose acetate (CA) film, also reported here, despite a 4-fold higher CO2 sorption capacity. Microstructural investigations suggest that the interconnected O2- and H2-sieving ultramicroporosity of TPDA-TMPD is more sensitive to slight CO2-induced dilations and is the physical basis for a more extensive and accelerated plasticization. Interchain rigidity, potentially by interchain interactions, is emphasized and may be facilitated by intrachain mobility.

  1. Influence of local emissions on concentration and isotopic composition of trace gases (CO2 and CH4) under strong anthropopression: A case study from Krakow, southern Poland

    International Nuclear Information System (INIS)

    Florkowski, T.; Korus, A.; Kuc, T.; Lasa, J.; Necki, J.M.; Zimnoch, M.

    2002-01-01

    Full text: Measurements of the isotopic composition of carbon dioxide and methane together with their concentrations in the atmosphere, yield useful information on the contribution of anthropogenic sources to regional budgets of these gases and their seasonal changes. Observed correlation between isotopic composition and inverse concentration of these gases is used for estimation of mean isotopic composition of the local source. Monitoring of atmospheric CO 2 has been initiated in Krakow in 1982. The sampling point is located in a polluted urban area with strong contribution of anthropogenic gases originating both from local sources (coal burning, car traffic, leakages from city gas network, landfills) and large distant emitters - industrial district located ca. 80 km to the west from Krakow (Silesia district). Quasi-continuous measurements of CO 2 , and CH 4 concentrations in the low atmosphere are performed using gas chromatographic method. For isotope measurements, the atmospheric CO 2 is continuously sampled by sorption on molecular sieve in be-weekly intervals and radiocarbon concentration is measured by liquid scintillation spectrometer, while δ 13 C is determined by isotope ratio mass spectrometer. Measurement error (1σ for single measurement) is in the order of 0.1 ppm for CO 2 concentration, ±8 per mille for δ 14 C, and ± 0.1 per mille for δ 13 C. In 1994, a new station for regular observations of greenhouse gases in lower atmosphere was set up in the High Tatra mountains, at Kasprowy Wierch (49 deg. N, 20 deg. E, 1980 m a.s.l., 300 m above the tree line). Kasprowy Wierch, with only small influences from local sources of trace gases can be considered as a reference station for this region of Poland. The record of CO 2 and CH 4 concentration and their isotope composition obtained at Kasprowy Wierch is considered as a background level for Krakow observations. The presented study was aimed at better characterisation and quantification of the local

  2. Diffuse soil emission of hydrothermal gases (CO2, CH4, and C6H6) at Solfatara crater (Campi Flegrei, southern Italy)

    International Nuclear Information System (INIS)

    Tassi, F.; Nisi, B.; Cardellini, C.; Capecchiacci, F.; Donnini, M.; Vaselli, O.; Avino, R.; Chiodini, G.

    2013-01-01

    Highlights: • We present the first measurements of soil C 6 H 6 fluxes in a volcanic system. • Methane oxidation rate is controlled by soil gas fluxes. • Benzene oxidation rate is controlled by presence of a SO 4 2- rich aquifer. • Fumarolic emissions cause a strong benzene air contamination at a local scale. • Endogenous monoaromatics are detected in air samples from the whole crater. - Abstract: Measurements of soil fluxes of hydrothermal gases, with special emphasis on C 6 H 6 , as well as chemical composition of mono-aromatic compounds in fumaroles and air, were carried out in April 2012 at the Solfatara crater (Campi Flegrei, Southern Italy) to investigate the distribution and behavior of these species as they migrate through the soil from their deep source to the atmosphere. Soil fluxes of CO 2 , CH 4 and C 6 H 6 exhibit good spatial correlation, suggesting that diffuse degassing is mainly controlled by local fractures. The calculated total output of diffuse C 6 H 6 from Solfatara is 0.10 kg day −1 , whereas fluxes of CO 2 and CH 4 are 79 × 10 3 and 1.04 kg day −1 , respectively. A comparison between soil gas fluxes and fumarole composition reveals that within the crater soil CH 4 is significantly affected by oxidation processes, which are more efficient for low gas fluxes, being dependent on the residence time of the uprising hydrothermal gases at shallow depth. Benzene degradation, mainly proceeding through oxidation via benzoate, seems to be strongly controlled by the presence of a shallow SO 4 2- rich aquifer located in the central and southwestern sectors of the crater, suggesting that the process is particularly efficient when SO 4 2- acts as terminal electron acceptor (SO 4 reduction). Relatively high C 6 H 6 /C 7 H 8 ratios, typical of hydrothermal fluids, were measured in air close to the main fumarolic field of Solfatara crater. Here, C 6 H 6 concentrations, whose detection limit is ∼0.1 μg m −3 , are more than one order of

  3. The Driving Forces of Guest Substitution in Gas Hydrates—A Laser Raman Study on CH4-CO2 Exchange in the Presence of Impurities

    Directory of Open Access Journals (Sweden)

    Bettina Beeskow-Strauch

    2012-02-01

    Full Text Available The recovery of CH4 gas from natural hydrate formations by injection of industrially emitted CO2 is considered to be a promising solution to simultaneously access an unconventional fossil fuel reserve and counteract atmospheric CO2 increase. CO2 obtained from industrial processes may contain traces of impurities such as SO2 or NOx and natural gas hydrates may contain higher hydrocarbons such as C2H6 and C3H8. These additions have an influence on the properties of the resulting hydrate phase and the conversion process of CH4-rich hydrates to CO2-rich hydrates. Here we show results of a microscopic and laser Raman in situ study investigating the effects of SO2-polluted CO2 and mixed CH4-C2H6 hydrate on the exchange process. Our study shows that the key driving force of the exchange processes is the establishment of the chemical equilibrium between hydrate phase and the surrounding phases. The exchange rate is also influenced by the guest-to-cavity ratio as well as the thermodynamic stability in terms of p-T conditions of the original and resulting hydrate phase. The most effective molecule exchange is related to structural changes (sI-sII which indicates that hydrate decomposition and reformation processes are the occurring processes.

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

    Directory of Open Access Journals (Sweden)

    Timothy J. Wallington

    2008-04-01

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

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

    Directory of Open Access Journals (Sweden)

    J. I. L. Morison

    2013-02-01

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

  6. A STUDY ON CARBON ISOTOPE OF CO2 AND CH4 IN WESTERN DIENG PLATEU BY GAS CHROMATOGRAPHY- ISOTOPE RATIO MASS SPECTROMETER (GC-IRMS

    Directory of Open Access Journals (Sweden)

    Hanik Humaida

    2010-06-01

    Full Text Available The carbon isotope can be used to evaluate volcanism phenomenon of volcano. The study of carbon isotope of CO2 and CH4 was carried out in western Dieng Plateau by mass-spectrometer. Before analysis, sampel was separated by gas chromatography using a Porapak-Q column and a FID (Flame Ionization Detector detector. The gas was oxidized by copper oxide at 850oC before being ionized in mass-spectrometer for isotope analysis. The CO2 content in Candradimuka crater (-4.10 O/OO, indicated that the gas may be as volcanic gas. The other CO2 from Sumber and western Gua Jimat, had isotope value  of -10.05 and -12.07 O/OO, respectively, indicating contamination from crustal and subduction material. The carbon isotope of CH4 gas from Pancasan village was -63.42 O/OO, that may be categorized as biogenic gas.   Keywords: isotope, CO2, CH4, Dieng.

  7. Livestock induces strong spatial heterogeneity of soil CO2, N2O and CH4 emissions within a semi-arid sylvo-pastoral landscape in West Africa

    Institute of Scientific and Technical Information of China (English)

    Mohamed H ASSOUMA; Dominique SER(C)A; Frédéric GU(E)RIN; Vincent BLANFORT; Philippe LECOMTE; Ibra TOUR(E); Alexandre ICKOWICZ

    2017-01-01

    Greenhouse gas (GHG) emissions from the surface soils and surface water receiving animal excreta may be important components of the GHG balance of terrestrial ecosystems,but the associated processes are poorly documented in tropical environments,especially in tropical arid and semi-arid areas.A typical sylvo-pastoral landscape in the semi-arid zone of Senegal,West Africa,was investigated in this study.The study area (706 km2 of managed pastoral land) was a circular zone with a radius of 15 km centered on a borehole used to water livestock.The landscape supports a stocking rate ranging from 0.11 to 0.39 tropical livestock units per hectare depending on the seasonal movements of the livestock.Six landscape units were investigated (land in the vicinity of the borehole,natural ponds,natural rangelands,forest plantations,settlements,and enclosed plots).Carbon dioxide (CO2),nitrous oxide (N2O) and methane (CH4) fluxes were measured with static chambers set up at 13 sites covering the six landscape units,and the 13 sites are assumed to be representative of the spatial heterogeneity of the emissions.A total of 216 fluxes were measured during the one-year study period (May 2014 to April 2015).At the landscape level,soits and surface water emitted an average 19.8 t C-CO2 eq/(hm2·a) (CO2:82%,N2O:15%,and CH4:3%),but detailed results revealed notable spatial heterogeneity of GHG emissions.CO2 fluxes ranged from 1148.2 (±91.6) mg/(m2·d) in rangelands to 97,980.2 (±14,861.7) mg/(m2·d) in surface water in the vicinity of the borehole.N2O fluxes ranged from 0.6 (±0.1) mg/(m2·d) in forest plantations to 22.6 (±10.8) mg/(m2·d) in the vicinity of the borehole.CH4 fluxes ranged from-3.2 (±0.3) mg/(m2·d) in forest plantations to 8788.5 (±2295.9) mg/(m2·d) from surface water in the vicinity of the borehole.This study identified GHG emission "hot spots" in the landscape.Emissions from the surface soilts were significantly higher in the landscape units most frequently

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

    Energy Technology Data Exchange (ETDEWEB)

    Van der Zwaan, B.C.C.; Schoots, K.; Rivera-Tinoco, R. [Energy research Center of the Netherlands (ECN), Policy Studies Department, Amsterdam (Netherlands); Verbong, G.P.J. [Eindhoven University of Technology, Department of Industrial Engineering and Innovation Sciences, Eindhoven (Netherlands)

    2011-11-15

    Gases like CH4, CO2 and H2 may play a key role in establishing a sustainable energy system: CH4 is the least carbon-intensive fossil energy resource; CO2 capture and storage can significantly reduce the climate footprint of especially fossil-based electricity generation; and the use of H2 as energy carrier could enable carbon-free automotive transportation. Yet the construction of large pipeline infrastructures usually constitutes a major and time-consuming undertaking, because of safety and environmental issues, legal and (geo)political siting arguments, technically untrivial installation processes, and/or high investment cost requirements. In this article we focus on the latter and present an overview of both the total costs and cost components of the distribution of these three gases via pipelines. Possible intricacies and external factors that strongly influence these costs, like the choice of location and terrain, are also included in our analysis. Our distribution cost breakdown estimates are based on transportation data for CH4, which we adjust for CO2 and H2 in order to account for the specific additional characteristics of these two gases. The overall trend is that pipeline construction is no longer subject to significant cost reductions. For the purpose of designing energy and climate policy we therefore know in principle with reasonable certainty what the minimum distribution cost components of future energy systems are that rely on pipelining these gases. We describe the reasons why we observe limited learning-by-doing and explain why negligible construction cost reductions for future CH4, CO2 and H2 pipeline projects can be expected. Cost data of individual pipeline projects may strongly deviate from the global average because of national or regional effects related to the type of terrain, but also to varying costs of labor and fluctuating market prices of components like steel.

  9. Experimental soil warming effects on CO2 and CH4 flux from a low elevation spruce-fir forest soil in Maine, USA

    Science.gov (United States)

    Lindsey E. Rustad; Ivan J. Fernandez

    1998-01-01

    The effect of soil warming on CO2 and CH4 flux from a spruce-fir forest soil was evaluated at the Howland Integrated Forest Study site in Maine, USA from 1993 to 1995. Elevated soil temperatures (~5 °C) were maintained during the snow-free season (May-November) in replicated 15 × 15-m plots using electric cables buried 1-2...

  10. One-Step Reforming of CO2 and CH4 into High-Value Liquid Chemicals and Fuels at Room Temperature by Plasma-Driven Catalysis.

    Science.gov (United States)

    Wang, Li; Yi, Yanhui; Wu, Chunfei; Guo, Hongchen; Tu, Xin

    2017-10-23

    The conversion of CO 2 with CH 4 into liquid fuels and chemicals in a single-step catalytic process that bypasses the production of syngas remains a challenge. In this study, liquid fuels and chemicals (e.g., acetic acid, methanol, ethanol, and formaldehyde) were synthesized in a one-step process from CO 2 and CH 4 at room temperature (30 °C) and atmospheric pressure for the first time by using a novel plasma reactor with a water electrode. The total selectivity to oxygenates was approximately 50-60 %, with acetic acid being the major component at 40.2 % selectivity, the highest value reported for acetic acid thus far. Interestingly, the direct plasma synthesis of acetic acid from CH 4 and CO 2 is an ideal reaction with 100 % atom economy, but it is almost impossible by thermal catalysis owing to the significant thermodynamic barrier. The combination of plasma and catalyst in this process shows great potential for manipulating the distribution of liquid chemical products in a given process. © 2017 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.

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

    Science.gov (United States)

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

    2017-12-01

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

  12. Annual balances of CH4 and N2O from a managed fen meadow using eddy covariance flux measurements

    International Nuclear Information System (INIS)

    Schrier-Uijl, A.P.; Veenendaal, E.M.; Kroon, P.S.; Hensen, A.; Jonker, H.J.J.

    2010-10-01

    Annual terrestrial balances of methane (CH4) and nitrous oxide (N2O) are presented for a managed fen meadow in the Netherlands for 2006, 2007 and 2008, using eddy covariance (EC) flux measurements. Annual emissions derived from different methods are compared. The most accurate annual CH4 flux is achieved by gap filling EC fluxes with an empirical multivariate regression model, with soil temperature and mean wind velocity as driving variables. This model explains about 60% of the variability in observed daily CH4 fluxes. Annual N2O emissions can be separated into background emissions and event emissions due to fertilization. The background emission is estimated using a multivariate regression model also based on EC flux data, with soil temperature and mean wind velocity as driving variables. The event emissions are estimated using emission factors. The minimum direct emission factor is derived for six fertilization events by subtracting the background emission, and the IPCC default emission factor of 1% is used for the other events. In addition, the maximum direct emission factors are determined for the six events without subtracting the background emission. The average direct emission factor ranges from 1.2 to 2.8%, which is larger than the IPCC default value. Finally, the total terrestrial greenhouse gas balance is estimated at 16 Mg ha -1 year -1 in CO2-equivalents with contributions of 30, 25 and 45% by CO2, CH4 and N2O, respectively.

  13. [Characteristics of N2, N2O, NO, CO2 and CH4 Emissions in Anaerobic Condition from Sandy Loam Paddy Soil].

    Science.gov (United States)

    Cao, Na; Wang, Rui; Liao, Ting-ting; Chen, Nuo; Zheng, Xun-hua; Yao, Zhi-sheng; Zhang, Hai; Butterbach-Bahl, Klaus

    2015-09-01

    Understanding the characteristics of the production of nitrogen gases (N2, N2O and NO), CO2 and CH4 in anaerobic paddy soils is not only a prerequisite for an improved mechanistic understanding of key microbial processes involved in the production of atmospheric greenhouse gases (GHG), but might also provide the basis for designing greenhouse gas mitigation strategies. Moreover, quantifying the composition fractions of denitrification gaseous products is of key importance for improving parameterization schemes of microbial processes in process-oriented models which are increasingly used for assessing soil GHG emissions at site and national scales. In our experiments we investigated two sandy loam soils from two paddy fields. The initial concentrations of soil nitrate and dissolved organic carbon (DOC) were set at approximately 50 mg.kg-1 and mg.kg-1, respectively, by adding a mixture solution of KNO3 and glucose. The emissions of N2, N2O NO, CO2 and CH4, as well as concentrations of carbon and nitrogen substrates for each soil sample were measured simultaneously, using a gas-flow-soil-core technique and a paralleling substrate monitoring system. The results showed that the accumulative emissions of N2, N2O and NO of the two soil samples for the entire incubation period were 6 - 8, 20, and 15 - 18 mg.kg-1, respectively. By measuring the cumulative emissions of denitrification gases (N, = N2 + N2O + NO) we were able to explain 95% to 98% of observed changes in s1ifr nilrate concentrations. The mass fractions of N2, N2O and NO emissions to Nt were approximately 15% -19%, 47% -49%, and 34% -36%, respectively. Thus, in our experiments N2O and NO were the main products of denitrification for the entire incubation period. However, as the temporal courses of hourly or daily production of the denitrification gases showed, NO production dominated and peaked firstly, and then N2O, before finally N2 became the dominant product. Our results show the high temporal dynamic of

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

    Science.gov (United States)

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

    2017-12-01

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

  15. Charge transfer processes in collisions of H+ ions with H2, D2, CO, CO2 CH4, C2H2, C2H6 and C3H8 molecules below 10 keV

    International Nuclear Information System (INIS)

    Kusakabe, T.; Buenker, R.J.; Kimura, M.

    2002-01-01

    Charge transfer processes resulting from collisions of H + ions with H 2 , D 2 , CO, CO 2 CH 4 , C 2 H 2 , C 2 H 6 and C 3 H 8 molecules have been investigated in the energy range of 0.2 to 4.0 keV experimentally and theoretically. The initial growth rate method was employed in the experiment for studying the dynamics and cross sections. Theoretical analysis based on a molecular-orbital expansion method for H 2 , D 2 , CO, CH 4 and C 2 H 2 targets was also carried out. The present results for the H 2 , CO and CO 2 molecules by H + impact are found to be in excellent accord with most of previous measurements above 1 keV, but they show some differences below this energy where our result displays a stronger energy-dependence. For CH 4 , C 2 H 2 , C 2 H 6 and C 3 H 8 targets, both experimental and theoretical results indicate that if one assumes vibrationally excited molecular ions (CH 4 + , C 2 H 2 + , C 2 H 6 + and C 3 H 8 + ) formed in the exit channel, then charge transfer processes sometimes become more favorable since these vibrationally excited fragments meet an accidental resonant condition. This is a clear indication of the role of vibrational excited states for charge transfer, and is an important realization for general understanding. (author)

  16. Effects of elevated CO2 on forest soil CH4 consumption in Changbai Mountains%CO2浓度增加对长白山森林土壤甲烷氧化影响

    Institute of Scientific and Technical Information of China (English)

    关键; 张颖; 史荣久; 李慧; 韩斯琴; 徐慧

    2012-01-01

    Elevated atmospheric CO2 concentration may affect the oxidation rate of methane ( CH4) in forest soil. In this study, the effects of a 6-year exposure to elevated CO2 concentration (500 μnol · mol-1 ) on the soil microbial process of CH4 oxidation under Quercus mongolica seedlings were investigated with open top chamber (OTC) , and specific 16S rRNA and pmoA gene fragment primers were adopted to analyze the diversity and abundance of soil methanotrophs. Comparing with that under ambient CO2 and open-air, the soil methane consumption under elevated atmospheric CO2 during growth season was reduced by 4% and 22% , respectively. The specific 16S rRNA PCR-DGGE analysis showed that under elevated CO2, the community structure of methane-oxidizing bacteria ( MOB) changed, and the diversity index decreased. Elevated CO2 concentration had no distinct effects on the abundance of Type Ⅰ MOB, but decreased the amount of Type Ⅱ MOB significantly. The pmoA gene copy number under elevated CO2 concentration decreased by 15% and 46% , respectively, as compared with that under ambient CO2 and open-air. Our results suggested that elevated atmospheric CO2 decreased the abundance and activity of soil methanotrophs, and the main cause could be the increase of soil moisture content.%大气CO2浓度升高可能对森林土壤的甲烷(CH4)氧化速率产生影响.本文采用开顶箱技术,对连续6年高浓度CO2(500 μmol·mol-1)处理的长白山森林典型树种蒙古栎树下土壤CH4氧化速率进行研究,并利用CH4氧化菌的16S rRNA特异性引物以及CH4单加氧酶功能基因引物分析了土壤中CH4氧化菌的群落结构与数量.结果表明:CO2浓度增高后,生长季土壤甲烷氧化量与对照和裸地相比分别降低了4%和22%;基于16S rRNA特异性引物的DGGE分析表明,CO2浓度增高导致两类甲烷氧化菌的多样性指数降低;CO2浓度增高对土壤中Ⅰ类甲烷氧化菌数量无显著影响,而使土壤中Ⅱ类甲烷氧

  17. Choice of precipitant and calcination temperature of precursor for synthesis of NiCo2O4 for control of CO-CH4 emissions from CNG vehicles.

    Science.gov (United States)

    Trivedi, Suverna; Prasad, Ram

    2018-03-01

    Compressed natural gas (CNG) is most appropriate an alternative of conventional fuel for automobiles. However, emissions of carbon-monoxide and methane from such vehicles adversely affect human health and environment. Consequently, to abate emissions from CNG vehicles, development of highly efficient and inexpensive catalysts is necessary. Thus, the present work attempts to scan the effects of precipitants (Na 2 CO 3 , KOH and urea) for nickel cobaltite (NiCo 2 O 4 ) catalysts prepared by co-precipitation from nitrate solutions and calcined in a lean CO-air mixture at 400°C. The catalysts were used for oxidation of a mixture of CO and CH 4 (1:1). The catalysts were characterized by X-ray diffractometer, Brunauer-Emmett-Teller surface-area, X-ray photoelectron spectroscopy; temperature programmed reduction and Scanning electron microscopy coupled with Energy-Dispersive X-Ray Spectroscopy. The Na 2 CO 3 was adjudged as the best precipitant for production of catalyst, which completely oxidized CO-CH 4 mixture at the lowest temperature (T 100 =350°C). Whereas, for catalyst prepared using urea, T 100 =362°C. On the other hand the conversion of CO-CH 4 mixture over the catalyst synthesized by KOH limited to 97% even beyond 400°C. Further, the effect of higher calcination temperatures of 500 and 600°C was examined for the best catalyst. The total oxidation of the mixture was attained at higher temperatures of 375 and 410°C over catalysts calcined at 500 and 600°C respectively. Thus, the best precipitant established was Na 2 CO 3 and the optimum calcination temperature of 400°C was found to synthesize the NiCo 2 O 4 catalyst for the best performance in CO-CH 4 oxidation. Copyright © 2017. Published by Elsevier B.V.

  18. The Iġnik Sikumi Field Experiment, Alaska North Slope: Design, operations, and implications for CO2CH4 exchange in gas hydrate reservoirs

    Science.gov (United States)

    Boswell, Ray; Schoderbek, David; Collett, Timothy S.; Ohtsuki, Satoshi; White, Mark; Anderson, Brian J.

    2017-01-01

    The Iġnik Sikumi Gas Hydrate Exchange Field Experiment was conducted by ConocoPhillips in partnership with the U.S. Department of Energy, the Japan Oil, Gas and Metals National Corporation, and the U.S. Geological Survey within the Prudhoe Bay Unit on the Alaska North Slope during 2011 and 2012. The primary goals of the program were to (1) determine the feasibility of gas injection into hydrate-bearing sand reservoirs and (2) observe reservoir response upon subsequent flowback in order to assess the potential for CO2 exchange for CH4 in naturally occurring gas hydrate reservoirs. Initial modeling determined that no feasible means of injection of pure CO2 was likely, given the presence of free water in the reservoir. Laboratory and numerical modeling studies indicated that the injection of a mixture of CO2 and N2 offered the best potential for gas injection and exchange. The test featured the following primary operational phases: (1) injection of a gaseous phase mixture of CO2, N2, and chemical tracers; (2) flowback conducted at downhole pressures above the stability threshold for native CH4 hydrate; and (3) an extended (30-days) flowback at pressures near, and then below, the stability threshold of native CH4 hydrate. The test findings indicate that the formation of a range of mixed-gas hydrates resulted in a net exchange of CO2 for CH4 in the reservoir, although the complexity of the subsurface environment renders the nature, extent, and efficiency of the exchange reaction uncertain. The next steps in the evaluation of exchange technology should feature multiple well applications; however, such field test programs will require extensive preparatory experimental and numerical modeling studies and will likely be a secondary priority to further field testing of production through depressurization. Additional insights gained from the field program include the following: (1) gas hydrate destabilization is self-limiting, dispelling any notion of the potential for

  19. Future concentrations of atmospheric greenhouse gases CO2, CFC and CH4 - an assessment on the educational level

    International Nuclear Information System (INIS)

    Hoppenau, S.

    1992-01-01

    A model on the educational level is described to estimate effective future atmospheric CO 2 concentrations. The effects of chlorofluorocarbon and methane emission and deforestation are taken into account. The influence of different emission scenarios on the time evolution of greenhouse-gas concentration are illustrated. Future global energy policies are discussed both under the aspects of rising world population and the reduction in global CO 2 emissions. The model can be handled on a PC or even on a pocket calculator

  20. Structural study of CH4, CO2 and H2O clusters containing from several tens to several thousands of molecules

    Science.gov (United States)

    Torchet, G.; Farges, J.; de Feraudy, M. F.; Raoult, B.

    Clusters are produced during the free jet expansion of gaseous CH4, CO2 or H2O. For a given stagnation temperature To, the mean cluster size is easily increased by increasing the stagnation pressure p0. On the other hand, the cluster temperature does not depend on stagnation conditions but mainly on properties of the condensed gas. An electron diffraction analysis provides information about the cluster structure. Depending on whether the diffraction patterns exhibit crystalline lines or not, the structure is worked out either by using crystallographic methods or by constructing cluster models. When they contain more than a few thousand molecules, clusters show a crystalline structure identical to that of one phase, namely, the cubic phase, known in bulk solid: plastic phase (CH4), unique solid phase (CO2) or metastable cubic phase (H2O). When decreasing the cluster size, the studied compounds behave quite differently: CO2 clusters keep the same crystalline structure, CH4 clusters show the multilayer icosahedral structure wich has been found in rare gas clusters, and H2O clusters adopt a disordered structure different from the amorphous structures of bulk ice. Des agrégats sont produits au cours de la détente en jet libre des gaz CH4, CO2 ou H2O. Pour une température initiale donnée To, on accroît facilement la taille moyenne des agrégats en augmentant la pression initiale po . Par contre, la température des agrégats dépend principalement des propriétés du gaz condensé. Une analyse par diffraction électronique permet l'étude de la structure des agrégats. Selon que les diagrammes de diffraction contiennent ou non des raies cristallines, on a recours soit à des méthodes cristallographiques soit à la construction de modèles d'agrégats. Lorsqu'ils renferment plus de quelques milliers de molécules, les agrégats adoptent la structure cristalline de l'une des phases connues du solide massif et plus précisément la phase cubique : phase plastique pour

  1. A Single-Culture Bioprocess of Methanothermobacter thermautotrophicus to Upgrade Digester Biogas by CO2-to-CH4 Conversion with H2

    Science.gov (United States)

    Martin, Matthew R.; Fornero, Jeffrey J.; Angenent, Largus T.

    2013-01-01

    We optimized and tested a postbioprocessing step with a single-culture archaeon to upgrade biogas (i.e., increase methane content) from anaerobic digesters via conversion of CO2 into CH4 by feeding H2 gas. We optimized a culture of the thermophilic methanogen Methanothermobacter thermautotrophicus using: (1) a synthetic H2/CO2 mixture; (2) the same mixture with pressurization; (3) a synthetic biogas with different CH4 contents and H2; and (4) an industrial, untreated biogas and H2. A laboratory culture with a robust growth (dry weight of 6.4–7.4 g/L; OD600 of 13.6–15.4), a volumetric methane production rate of 21 L/L culture-day, and a H2 conversion efficiency of 89% was moved to an industrial anaerobic digester facility, where it was restarted and fed untreated biogas with a methane content of ~70% at a rate such that CO2 was in excess of the stoichiometric requirements in relation to H2. Over an 8-day operating period, the dry weight of the culture initially decreased slightly before stabilizing at an elevated level of ~8 g/L to achieve a volumetric methane production rate of 21 L/L culture-day and a H2 conversion efficiency of 62%. While some microbial contamination of the culture was observed via microscopy, it did not affect the methane production rate of the culture. PMID:24194675

  2. A Single-Culture Bioprocess of Methanothermobacter thermautotrophicus to Upgrade Digester Biogas by CO2-to-CH4 Conversion with H2

    Directory of Open Access Journals (Sweden)

    Matthew R. Martin

    2013-01-01

    Full Text Available We optimized and tested a postbioprocessing step with a single-culture archaeon to upgrade biogas (i.e., increase methane content from anaerobic digesters via conversion of CO2 into CH4 by feeding H2 gas. We optimized a culture of the thermophilic methanogen Methanothermobacter thermautotrophicus using: (1 a synthetic H2/CO2 mixture; (2 the same mixture with pressurization; (3 a synthetic biogas with different CH4 contents and H2; and (4 an industrial, untreated biogas and H2. A laboratory culture with a robust growth (dry weight of 6.4–7.4 g/L; OD600 of 13.6–15.4, a volumetric methane production rate of 21 L/L culture-day, and a H2 conversion efficiency of 89% was moved to an industrial anaerobic digester facility, where it was restarted and fed untreated biogas with a methane content of ~70% at a rate such that CO2 was in excess of the stoichiometric requirements in relation to H2. Over an 8-day operating period, the dry weight of the culture initially decreased slightly before stabilizing at an elevated level of ~8 g/L to achieve a volumetric methane production rate of 21 L/L culture-day and a H2 conversion efficiency of 62%. While some microbial contamination of the culture was observed via microscopy, it did not affect the methane production rate of the culture.

  3. Natural bog pine ecosystem in southern Germany is a steady and robust sink of CO2 but a minor source of CH4

    Science.gov (United States)

    Hommeltenberg, Janina; Schmid, Hans Peter; Droesler, Matthias; Werle, Peter

    2013-04-01

    Natural peatland ecosystems sequester carbon dioxide. They do this slowly but steadily, but also emit methane in small rates. Thus peatlands have both positive and negative greenhouse gas balance impacts on the climate system due to their influence on atmospheric CO2 and CH4 concentration. We present data of net ecosystem CO2 exchange (NEE) of almost three years (July 2010 to March 2013) and of methane fluxes over a period of nine months (July 2012 to March 2013), measured by eddy covariance technique in the bog forest "Schechenfilz". The site (47°48' N; 11°19' E, 590 m a.s.l.) is an ICOS-ecosystems associate site, located in the pre-alpine region of southern Germany, where a natural Pinus mugo rotundata forest grows on an undisturbed, almost 6 m thick peat layer. The slow growing bog pines and their low rates of carbon sequestration, in combination with high water table and thus low availability of oxygen, lead to low carbon dioxide fluxes. Photosynthesis as well as soil respiration are considerably attenuated compared to upland sites. Additionally, the high soil water content is damping the impact of dry and hot periods on CO2 exchange. Thus the CO2 balance is very robust to changing environmental parameters. While the CO2 exchange is clearly related to soil temperature and photosynthetic active radiation, we have not yet identified a parameter that governs variations in methane exchange. Various environmental parameters appear to be related to methane emissions (including soil moisture, soil and air temperature and wind direction), but the scatter with respect to half hourly methane fluxes is too large to be useful for gap modeling. Analysis of daily averages reduces the scatter, but since methane exchange exhibits considerable daily variation, daily averages are not useful to fill data gaps of half hourly fluxes. In consequence, as the daily course is the summary result of all environmental parameters having influence on the methane exchange at the half

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

    International Nuclear Information System (INIS)

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

    2011-01-01

    Highlights: → Learning for pipeline construction, if available, is outshadowed by cost variability. → Pipelining is a mature technology, for which much experience has been gained. → Pipeline projects are heterogeneous with widely varying technical and cost specifics. → Pipeline cost components tend to reflect (commodity) market price developments. → Pipeline costs are strongly determined by the properties of the transported gas. -- Abstract: Gases like CH 4 , CO 2 and H 2 may play a key role in establishing a sustainable energy system: CH 4 is the least carbon-intensive fossil energy resource; CO 2 capture and storage can significantly reduce the climate footprint of especially fossil-based electricity generation; and the use of H 2 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 un-trivial 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 CH 4 , which we adjust for CO 2 and H 2 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

  5. The European land and inland water CO2, CO, CH4 and N2O balance between 2001 and 2005

    NARCIS (Netherlands)

    Luyssaert, S.; Abril, G.; Andres, R.; Bastviken, D.; Bellassen, V.; Bergamaschi, P.; Bousquet, P.; Chevallier, F.; Ciais, P.; Corazza, M.; Dechow, R.; Erb, K.H.; Etiope, G.; Fortems-Cheiney, A.; Grassi, G.; Hartmann, J.; Jung, M.; Lathiere, J.; Lohila, A.; Mayorga, E.; Moosdorf, N.; Njakou, D.S.; Otto, J.; Papale, D.; Peters, W.; Peylin, P.; Raymond, P.; Rodenbeck, C.; Saarnio, S.; Schulze, E.D.; Szopa, S.; Thompson, R.; Verkerk, P.J.; Vuichard, N.; Wang, R.; Wattenbach, M.; Zaehle, S.

    2012-01-01

    Globally, terrestrial ecosystems have absorbed about 30% of anthropogenic greenhouse gas emissions over the period 2000-2007 and inter-hemispheric gradients indicate that a significant fraction of terrestrial carbon sequestration must be north of the Equator. We present a compilation of the CO2, CO,

  6. Dual stable isotopes of CH 4 from Yellowstone hot-springs suggest hydrothermal processes involving magmatic CO 2

    Energy Technology Data Exchange (ETDEWEB)

    Moran, James J.; Whitmore, Laura M.; Jay, Zackary J.; Jennings, Ryan deM.; Beam, Jacob P.; Kreuzer, Helen W.; Inskeep, William P.

    2017-07-01

    Volcanism and post-magmatism contribute both significant annual CH4 fluxes to the atmosphere (on par with other natural sources such as forest fire and wild animal emissions) and have been implicated in past climate-change events. The Yellowstone hot spot is one of the largest volcanic systems on Earth and is known to emit methane in addition to other greenhouse gases (e.g. carbon dioxide) but the ultimate source of this methane flux has not been elucidated. Here we use dual stable isotope analysis (δ2H and δ13C) of CH4(g) sampled from ten high-temperature geothermal pools in Yellowstone National Park to show that the predominant flux of CH4(g) is abiotic. The average δ13C and δ2H values of CH4(g) emitted from hot springs (-26.7 (±2.4) and -236.9 (±12.0) ‰, respectively) are not consistent with biotic (microbial or thermogenic) methane sources, but are within previously reported ranges for abiotic methane production. Correlation between δ13CCH4 and δ13C-dissolved inorganic C (DIC) also suggests that CO2 is a parent C source for the observed CH4(g). Moreover, CH4-CO2 isotopic geothermometry was used to estimate CH4(g) formation temperatures ranging from ~ 250 - 350°C, which is just below the temperature estimated for the hydrothermal reservoir and consistent with the hypothesis that subsurface, rock-water interactions are responsible for large methane fluxes from this volcanic system. An understanding of conditions leading to the abiotic production of methane and associated isotopic signatures are central to understanding the evolutionary history of deep carbon sources on Earth.

  7. Effects of hydroxyl-functionalization and sub-Tg thermal annealing on high pressure pure- and mixed-gas CO2/CH4 separation by polyimide membranes based on 6FDA and triptycene-containing dianhydrides

    KAUST Repository

    Swaidan, Raja

    2015-02-01

    A sub-Tg thermally-annealed (250°C, 24h) ultra-microporous PIM-polyimide bearing a 9,10-diisopropyl-triptycene contortion center and hydroxyl-functionalized diamine (2,2-bis(3-amino-4-hydroxyphenyl)-hexafluoropropane, APAF) exhibited plasticization resistance up to 50bar for a 1:1 CO2/CH4 feed mixture, with a 9-fold higher CO2 permeability (30Barrer) and 2-fold increase in CO2/CH4 permselectivity (~50) over conventional dense cellulose acetate membranes at 10bar CO2 partial pressure. Interestingly, mixed-gas CO2/CH4 permselectivities were 10-20% higher than those evaluated under pure-gas conditions due to reduction of mixed-gas CH4 permeability by co-permeation of CO2. Gas transport, physisorption and fluorescence studies indicated a sieving pore-structure engaged in inter-chain charge transfer complexes (CTCs), similar to that of low-free-volume 6FDA-APAF polyimide. The isosteric heat of adsorption of CO2 as well as CO2/CH4 solubility selectivities varied negligibly upon replacement of OH with CH3 but CTC formation was hindered, CO2 sorption increased, CO2 permeability increased ~3-fold, CO2/CH4 permselectivity dropped to ~30 and CH4 mixed-gas co-permeation increased. These results suggest that hydroxyl-functionalization did not cause preferential polymer-gas interactions but primarily elicited diffusion-dominated changes owing to a tightened microstructure more resistant to CO2-induced dilations. Solution-processable hydroxyl-functionalized PIM-type polyimides provide a new platform of advanced materials that unites the high selectivities of low-free-volume polymers with the high permeabilities of PIM-type materials particularly for natural gas sweetening applications.

  8. Seasonal variations in CO2 and CH4 fluxes of four different plant compositions of a Sphagnum-dominated Alpine peat bog

    Science.gov (United States)

    Drollinger, Simon; Maier, Andreas; Karer, Jasmin; Glatzel, Stephan

    2017-04-01

    Peatlands are the only type of ecosystems which have the ability to accumulate significant amounts of carbon (C) under undisturbed conditions. The amount of C sequestered in peatlands depends on the balance between gross primary production, ecosystem respiration and decomposition of plant material. Sphagnum-dominated bogs possess the greatest peat accumulation potential of all peatlands, thus in turn, feature highest C release potentials. Many studies report about the C balances of undisturbed northern peat bogs, however, little is known about the effects of peatland degradation on the C balance between different plant compositions within peat bog ecosystems. Particularly in the Alpine region, where temperature increase during the last century has been almost twice as high as the global mean. The investigated peat bog is located in the inner Alpine Enns valley in the Eastern Alps, Austria (N 47˚ 34.873' E 14˚ 20.810'). It is a pine peat bog covered by Sphagnum mosses and a present extent of about 62 ha. Due to increasing differences in surface height of the peatland compared to the surrounding areas and related lowered water retention capacity attributed to the subsidence of the adjacent intensively managed meadows on deeply drained peat soils, the function of the peatland as a carbon sink is strongly endangered. Hence, the current mean water table depth of the central peat bog area is about -12 cm. To reveal differences in peatland-atmosphere C exchanges within the peatland ecosystem, we investigated CO2 and CH4 fluxes of four different vegetation compositions (PM1-PM4) at the treeless central peat bog area. PM1 is dominated by the graminoids Rhynchospora alba and Eriophorum vaginatum. PM2 is inhabited by small individuals (< 35 cm) of the conifer Pinus mugo, whereas PM3 is dominated by the ericaceous plant Calluna vulgaris. PM4 again is populated by Pinus mugo, but higher growing (35 - 60 cm) and with corresponding higher amount of biomass. Fluxes were measured

  9. Influence of pyrolysis conditions on the CO2/CH4 and O2/N2 perm selectivity of supported carbon molecular sieve membranes

    International Nuclear Information System (INIS)

    Mohd Fikri Abdul Rahman; Wan Mohd Hafiz Faizal Wan Harun; Mohd Azmier Ahmad

    2010-01-01

    This work focused on the effect of pyrolysis conditions onto supported carbon molecular sieve membranes performance in pure gas permeation and perm selectivity. The membrane support was synthesis by carbonization of titania mixed with cellulose acetate at temperature of 125 degree Celsius. The molecular sieving membrane layer was obtained by coating the polyvinyl alcohol-glutaraldehyde solution onto the membrane support before heated at various pyrolysis temperatures and holding times. The optimum preparation conditions were found at pyrolysis temperature and holding time of 400 degree Celsius and 30 minutes, respectively. At this point, the CO 2 and O 2 permeation flux were 2.63 ml/ min and 2.67 ml/ min, respectively. Meanwhile, the perm selectivities of CO 2 / CH 4 and O 2 / N 2 were 1.87 and 1.92, respectively. (author)

  10. Effect of frame size and season on enteric methane (CH4) and carbon dioxide (CO2)emissions in Angus brood cows grazing native tall-grass prairie in central Oklahoma USA

    Science.gov (United States)

    Effect of frame size and season on enteric methane (CH4) and carbon dioxide (CO2) emissions in Angus brood cows grazing native tall-grass prairie in central Oklahoma, USA J.P.S. Neel USDA ARS, El Reno, OK A reduction in enteric CH4 production in ruminants is associated with improved production effic...

  11. Enhanced selective photocatalytic reduction of CO2 to CH4 over plasmonic Au modified g-C3N4 photocatalyst under UV-vis light irradiation

    Science.gov (United States)

    Li, Hailong; Gao, Yan; Xiong, Zhuo; Liao, Chen; Shih, Kaimin

    2018-05-01

    A series of Au-g-C3N4 (Au-CN) catalysts were prepared through a NaBH4-reduction method using g-C3N4 (CN) from pyrolysis of urea as precursor. The catalysts' surface area, crystal structure, surface morphology, chemical state, functional group composition and optical properties were characterized by X-ray diffraction, transmission electron microscope, X-ray photoelectron spectroscopy, ultraviolet visible (UV-vis) diffuse reflectance spectra, fourier transform infrared, photoluminescence and transient photocurrent analysis. The carbon dioxide (CO2) photoreduction activities under ultraviolet visible (UV-vis) light irradiation were significantly enhanced when gold (Au) was loaded on the surface of CN. 2Au-CN catalyst with Au to CN mole ratio of 2% showed the best catalytic activity. After 2 h UV-vis light irradiation, the methane (CH4) yield over the 2Au-CN catalyst was 9.1 times higher than that over the pure CN. The CH4 selectivity also greatly improved for the 2Au-CN compared to the CN. The deposited Au nanoparticles facilitated the separation of electron-hole pairs on the CN surface. Moreover, the surface plasmon resonance effect of Au further promoted the generation of hot electrons and visible light absorption. Therefore, Au loading significantly improved CO2 photoreduction performance of CN under UV-vis light irradiation.

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

    Science.gov (United States)

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

    2015-10-01

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

  13. High catalytic activity and stability of Ni/CexZr1-xO2/MSU-H for CH4/CO2 reforming reaction

    Science.gov (United States)

    Chang, Xiaoqian; Liu, Bingsi; Xia, Hong; Amin, Roohul

    2018-06-01

    How to reduce emission of CO2 as greenhouse gases, which resulted in global warming, is of very important significance. A series of Ni/CexZr1-xO2/MSU-H catalysts was prepared by means of hexagonally ordered mesoporous MSU-H with thermal and hydrothermal stabilities, which is cheap and can be synthesized in the large scale. The 10%Ni/Ce0.75Zr0.25O2/MSU-H catalyst presents high catalytic activity, stability and the ability of coke-resistance for CH4/CO2 reforming reaction due to high SBET (428 m2/g) and smaller Nio nanoparticle size (3.14 nm). The high dispersed Nio nanoparticles over MSU-H promoted the decomposition of CH4 and the carbon species accumulated on active Nio sites reacting with crystal lattice oxygen in Ce0.75Zr0.25O2 to form CO molecules. In the meantime, the remained oxygen vacancies on the interface between Nio and Ce0.75Zr0.25O2 could be supplemented via CO2. HRTEM images and XRD results of Ni/Ce0.75Zr0.25O2/MSU-H verified that high dispersion of Ni nanoparticles over Ni/Ce0.75Zr0.25O2/MSU-H correlated closely with the synergistic action between Ce0.75Zr0.25O2 and MSU-H as well as hexagonally ordered structure of MSU-H, which can provide effectively the oxygen storage capacity and inhibit the formation of coke.

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

    International Nuclear Information System (INIS)

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

    2007-01-01

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

  15. Amino-Functionalized ZIF-7 Nanocrystals: Improved Intrinsic Separation Ability and Interfacial Compatibility in Mixed-Matrix Membranes for CO2 /CH4 Separation.

    Science.gov (United States)

    Xiang, Long; Sheng, Luqian; Wang, Chongqing; Zhang, Lixiong; Pan, Yichang; Li, Yanshuo

    2017-08-01

    Highly permeable and selective, as well as plasticization-resistant membranes are desired as promising alternatives for cost- and energy-effective CO 2 separation. Here, robust mixed-matrix membranes based on an amino-functionalized zeolitic imidazolate framework ZIF-7 (ZIF-7-NH 2 ) and crosslinked poly(ethylene oxide) rubbery polymer are successfully fabricated with filler loadings up to 36 wt%. The ZIF-7-NH 2 materials synthesized from in situ substitution of 2-aminobenzimidazole into the ZIF-7 structure exhibit enlarged aperture size compared with monoligand ZIF-7. The intrinsic separation ability for CO 2 /CH 4 on ZIF-7-NH 2 is remarkably enhanced as a result of improved CO 2 uptake capacity and diffusion selectivity. The incorporation of ZIF-7-NH 2 fillers simultaneously makes the neat polymer more permeable and more selective, surpassing the state-of-the-art 2008 Robeson upper bound. The chelating effect between metal (zinc) nodes of fillers and ester groups of a polymer provides good bonding, enhancing the mechanical strength and plasticization resistance of the neat polymer membrane. The developed novel ZIF-7 structure with amino-function and the resulting nanocomposite membranes are very attractive for applications like natural-gas sweetening or biogas purification. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  16. Flow characterization and dilution effects of N2 and CO2 on premixed CH4/air flames in a swirl-stabilized combustor

    International Nuclear Information System (INIS)

    Han Yue; Cai Guo-Biao; Wang Hai-Xing; Bruno Renou; Abdelkrim Boukhalfa

    2014-01-01

    Numerically-aided experimental studies are conducted on a swirl-stabilized combustor to investigate the dilution effects on flame stability, flame structure, and pollutant emissions of premixed CH 4 /air flames. Our goal is to provide a systematic assessment on combustion characteristics in diluted regimes for its application to environmentally-friendly approaches such as biogas combustion and exhaust-gas recirculation technology. Two main diluting species, N 2 and CO 2 , are tested at various dilution rates. The results obtained by means of optical diagnostics show that five main flame regimes can be observed for N 2 -diluted flames by changing excess air and dilution rate. CO 2 -diluted flames follow the same pattern evolution except that all the domains are shifted to lower excess air. Both N 2 and CO 2 dilution affect the lean blowout (LBO) limits negatively. This behavior can be counter-balanced by reactant preheating which is able to broaden the flammability domain of the diluted flames. Flame reactivity is degraded by increasing dilution rate. Meanwhile, flames are thickened in the presence of both diluting species. NO x emissions are significantly reduced with dilution and proved to be relevant to flame stability diagrams: slight augmentation in NO x emission profiles is related to transitional flame states where instability occurs. Although dilution results in increase in CO emissions at certain levels, optimal dilution rates can still be proposed to achieve an ideal compromise

  17. New type ternary NiAlCe layered double hydroxide photocatalyst for efficient visible-light photoreduction of CO2 into CH4

    Science.gov (United States)

    Li, Ji; (Bill Yang, Y. J.

    2018-02-01

    New type of ternary NiAlCe layered double hydroxide photocatalyst was synthesized by a simple hydrothermal reaction. The obtained photocatalyst shows efficient visible-light activity for CO2 reduction to CH4. We have investigated the optimal Ce content in the catalyst and analyzed the mechanism by materials characterization. Additionally, a novel alkali etching method was used to construct the porous structure. The effect of the porosity and morphologies on the activity is investigated. It is found that the ternary NiAlCe layered double hydroxide photocatalyst with porosity showing the best photocatalytic activity among all the samples. Based on the characterization and first principle calculation, the detailed photocatalytic mechanism of the ternary NiAlCe layered double hydroxide photocatalyst is deduced.

  18. Effect of drainage on CO2, CH4, and N2O fluxes from aquaculture ponds during winter in a subtropical estuary of China.

    Science.gov (United States)

    Yang, Ping; Lai, Derrick Y F; Huang, Jia F; Tong, Chuan

    2018-03-01

    Aquaculture ponds are dominant features of the landscape in the coastal zone of China. Generally, aquaculture ponds are drained during the non-culture period in winter. However, the effects of such drainage on the production and flux of greenhouse gases (GHGs) from aquaculture ponds are largely unknown. In the present study, field-based research was performed to compare the GHG fluxes between one drained pond (DP, with a water depth of 0.05m) and one undrained pond (UDP, with a water depth of 1.16m) during one winter in the Min River estuary of southeast China. Over the entire study period, the mean CO 2 flux in the DP was (0.75±0.12) mmol/(m 2 ·hr), which was significantly higher than that in the UDP of (-0.49±0.09) mmol/(m 2 ·hr) (paquaculture ponds from a net sink to a net source of CO 2 in winter. Mean CH 4 and N 2 O emissions were significantly higher in the DP compared to those in the UDP (CH 4 =(0.66±0.31) vs. (0.07±0.06) mmol/(m 2 ·hr) and N 2 O=(19.54±2.08) vs. (0.01±0.04) µmol/(m 2 ·hr)) (paquaculture ponds can increase the emissions of potent GHGs from the coastal zone of China to the atmosphere during winter, further aggravating the problem of global warming. Copyright © 2017. Published by Elsevier B.V.

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

    NARCIS (Netherlands)

    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

  20. High pressure pure- and mixed-gas separation of CO2/CH4 by thermally-rearranged and carbon molecular sieve membranes derived from a polyimide of intrinsic microporosity

    KAUST Repository

    Swaidan, Raja

    2013-11-01

    Natural gas sweetening, one of the most promising venues for the growth of the membrane gas separation industry, is dominated by polymeric materials with relatively low permeabilities and moderate selectivities. One strategy towards improving the gas transport properties of a polymer is enhancement of microporosity either by design of polymers of intrinsic microporosity (PIMs) or by thermal treatment of polymeric precursors. For the first time, the mixed-gas CO2/CH4 transport properties are investigated for a complete series of thermally-rearranged (TR) (440°C) and carbon molecular sieve (CMS) membranes (600, 630 and 800°C) derived from a polyimide of intrinsic microporosity (PIM-6FDA-OH). The pressure dependence of permeability and selectivity is reported up to 30bar for 1:1, CO2:CH4 mixed-gas feeds at 35°C. The TR membrane exhibited ~15% higher CO2/CH4 selectivity relative to pure-gas feeds due to reductions in mixed-gas CH4 permeability reaching 27% at 30bar. This is attributed to increased hindrance of CH4 transport by co-permeation of CO2. Interestingly, unusual increases in mixed-gas CH4 permeabilities relative to pure-gas values were observed for the CMS membranes, resulting in up to 50% losses in mixed-gas selectivity over the applied pressure range. © 2013 Elsevier B.V.

  1. Effects of hydroxyl-functionalization and sub-Tg thermal annealing on high pressure pure- and mixed-gas CO2/CH4 separation by polyimide membranes based on 6FDA and triptycene-containing dianhydrides

    KAUST Repository

    Swaidan, Raja; Ghanem, Bader; Litwiller, Eric; Pinnau, Ingo

    2015-01-01

    -structure engaged in inter-chain charge transfer complexes (CTCs), similar to that of low-free-volume 6FDA-APAF polyimide. The isosteric heat of adsorption of CO2 as well as CO2/CH4 solubility selectivities varied negligibly upon replacement of OH with CH3 but CTC

  2. Sorption Behavior of Compressed CO2 and CH4 on Ultrathin Hybrid Poly(POSS-imide) Layers.

    Science.gov (United States)

    Raaijmakers, Michiel J T; Ogieglo, Wojciech; Wiese, Martin; Wessling, Matthias; Nijmeijer, Arian; Benes, Nieck E

    2015-12-09

    Sorption of compressed gases into thin polymeric films is essential for applications including gas sensors and membrane based gas separation. For glassy polymers, the sorption behavior is dependent on the nonequilibrium status of the polymer. The uptake of molecules by a polymer is generally accompanied by dilation, or swelling, of the polymer material. In turn, this dilation can result in penetrant induced plasticization and physical aging that affect the nonequilibrium status of the polymer. Here, we investigate the dilation and sorption behavior of ultrathin membrane layers of a hybrid inorganic-organic network material that consists of alternating polyhedral oligomeric silsesquioxane and imide groups, upon exposure to compressed carbon dioxide and methane. The imide precursor contains fluoroalkene groups that provide affinity toward carbon dioxide, while the octa-functionalized silsesquioxane provides a high degree of cross-linking. This combination allows for extremely high sorption capacities, while structural rearrangements of the network are hindered. We study the simultaneous uptake of gases and dilation of the thin films at high pressures using spectroscopic ellipsometry measurements. Ellipsometry provides the changes in both the refractive index and the film thickness, and allows for accurate quantification of sorption and swelling. In contrast, gravimetric and volumetric measurements only provide a single parameter; this does not allow an accurate correction for, for instance, the changes in buoyancy because of the extensive geometrical changes of highly swelling films. The sorption behavior of the ultrathin hybrid layers depends on the fluoroalkene group content. At low pressure, the apparent molar volume of the gases is low compared to the liquid molar volume of carbon dioxide and methane, respectively. At high gas concentrations in the polymer film, the apparent molar volume of carbon dioxide and methane exceeds that of the liquid molar volume, and

  3. Integrated underground gas storage of CO2 and CH4 to decarbonize the "power-to-gas-to-gas-to-power" technology

    Science.gov (United States)

    Kühn, Michael; Streibel, Martin; Nakaten, Natalie; Kempka, Thomas

    2014-05-01

    Massive roll-out of renewable energy production units (wind turbines and solar panels) leads to date to excess energy which cannot be consumed at the time of production. So far, long-term storage is proposed via the so called 'power-to-gas' technology. Energy is transferred to methane gas and subsequently combusted for power production - 'power-to-gas-to-power' (PGP) - when needed. PGP profits from the existing infrastructure of the gas market and could be deployed immediately. However, major shortcoming is the production of carbon dioxide (CO2) from renewables and its emission into the atmosphere. We present an innovative idea which is a decarbonised extension of the PGP technology. The concept is based on a closed carbon cycle: (1) Hydrogen (H2) is generated from renewable energy by electrolysis and (2) transformed into methane (CH4) with CO2 taken from an underground geological storage. (3) CH4 produced is stored in a second storage underground until needed and (4) combusted in a combined-cycled power plant on site. (5) CO2 is separated during energy production and re-injected into the storage formation. We studied a show case for the cities Potsdam and Brandenburg/Havel in the Federal State of Brandenburg in Germany to determine the energy demand of the entire process chain and the costs of electricity (COE) using an integrated techno-economic modelling approach (Nakaten et al. 2014). Taking all of the individual process steps into account, the calculation shows an overall efficiency of 27.7 % (Streibel et al. 2013) with total COE of 20.43 euro-cents/kWh (Kühn et al. 2013). Although the level of efficiency is lower than for pump and compressed air storage, the resulting costs are similar in magnitude, and thus competitive on the energy storage market. The great advantage of the concept proposed here is that, in contrast to previous PGP approaches, this process is climate-neutral due to CO2 utilisation. For that purpose, process CO2 is temporally stored in an

  4. Land-use change effects on fluxes and isotopic composition of CO2 and CH4 in Panama, and possible insights into the atmospheric H2 cycle

    Science.gov (United States)

    Pendall, E.; Schwendenmann, L.; Potvin, C.

    2003-12-01

    Land-use changes in tropical regions are believed to release a quantity of C to the atmosphere which is similar in magnitude to the entire "missing" sink for anthropogenic CO2. Our research attempts to evaluate carbon cycling in three land-cover systems in central Panama: cow pasture, native tree plantation, and undisturbed moist forest. In this ongoing project, we are collecting samples of air from profiles in the stable, nocturnal boundary layer, which is dominated by ecosystem respiration. Samples are analyzed for CO2 and its isotopes, CH4 and its C isotopic composition, N2O, H2, CO, and SF6. We use a flux-gradient method to estimate ecosystem-scale fluxes of trace gases from soil to the atmosphere. Keeling plot intercepts reflect the respiratory contribution of C3 and C4 biomass under contrasting land cover systems, and how this varies with pronounced wet-dry seasonal cycles. C isotopes of methane and gradients of molecular hydrogen provide insight into the source of methane production from pasture and plantation soils. Rainforest soils, in contrast, are sinks for both atmospheric methane and hydrogen. The process oriented nature of this field experiment will contribute to parameterization of carbon cycle models at a variety of spatial scales.

  5. Syngas Production from Catalytic CO2 Reforming of CH4 over CaFe2O4 Supported Ni and Co Catalysts: Full Factorial Design Screening

    Directory of Open Access Journals (Sweden)

    M. Anwar Hossain

    2018-01-01

    Full Text Available In this study, the potential of dry reforming reaction over CaFe2O4 supported Ni and Co catalysts were investigated. The Co/CaFe2O4 and Ni/CaFe2O4 catalysts were synthesized using wet impregnation method by varying the metal loading from 5-15 %. The synthesized catalysts were tested in methane dry reforming reaction at atmospheric pressure and reaction temperature ranged 700-800 oC. The catalytic performance of the catalysts based on the initial screening is ranked as 5%Co/CaFe2O4 < 10%Co/CaFe2O4 < 5%Ni/CaFe2O4 < 10%Ni/CaFe2O4 according to their performance. The Ni/CaFe2O4 catalyst was selected for further investigation using full factorial design of experiment. The interaction effects of three factors namely metal loading (5-15 %, feed ratio (0.4-1.0, and reaction temperature (700-800 oC were evaluated on the catalytic activity in terms of CH4 and CO2 conversion as well as H2 and CO yield. The interaction between the factors showed significant effects on the catalyst performance at metal loading, feed ratio and reaction temperature of 15 %, 1.0, and 800 oC. respectively. The 15 wt% Ni/CaFe2O4 was subsequently characterized by Thermogravimetric (TGA, X-ray Diffraction (XRD, Field Emission Scanning Electron Microscopy (FESEM, Energy Dispersive X-ray Spectroscopy (EDX, X-ray Photoelectron Spectroscopy (XPS, N2-physisorption, Temperature Programmed Desorption (TPD-NH3, TPD-CO2, and Fourier Transform Infra Red (FTIR to ascertain its physiochemical properties.  This study demonstrated that the CaFe2O4 supported Ni catalyst has a good potential to be used for syngas production via methane dry reforming. Copyright © 2018 BCREC Group. All rights reserved Received: 5th May 2017; Revised: 8th August 2017; Accepted: 9th August 2017; Available online: 22nd January 2018; Published regularly: 2nd April 2018 How to Cite: Hossain, M.A., Ayodele, B.V., Cheng, C.K., Khan, M.R. (2018. Syngas Production from Catalytic CO2 Reforming of CH4 over CaFe2O4 Supported

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

    Science.gov (United States)

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

    2017-04-01

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

  7. Application of trajectory clustering and source attribution methods for investigating regional CO2 and CH4 concentrations at Germany's highest mountain site

    Science.gov (United States)

    Giemsa, Esther; Jacobeit, Jucundus; Ries, Ludwig; Frank, Gabriele; Hachinger, Stephan; Meyer-Arnek, Julian

    2017-04-01

    Carbon dioxide (CO2) and methane (CH4) represent the most important contributors to increased radiative forcing enhancing it together by contemporary 2.65 W/m2 on the global average (IPCC 2013). The unbroken increase of atmospheric greenhouse gases (GHG) has been unequivocally attributed to human emissions mainly coming from fossil fuel burning and land-use changes, while the oceans and terrestrial ecosystems slightly attenuate this rise with seasonally varying strength. Short-term fluctuations in the GHG concentrations that superimpose the seasonal cycle and the climate change driven trend reflect the presence of regional sources and sinks. A perfect place for investigating the comprehensive influence of these regional emissions is provided by the Environmental Research Station Schneefernerhaus (47.42°N, 10.98°E, 2.650m a.s.l.) situated in the eastern Alps at the southern side of Zugspitze mountain. Located just 300m below the highest peak of the German Alps, the exposed site is one of the currently 30 global core sites of the World Meteorological Organisation (WMO) Global Atmosphere Watch (GAW) programme and thus provides ideal conditions to study source-receptor relationships for greenhouse gases. We propose a stepwise statistical methodology for examining the relationship between synoptic-scale atmospheric transport patterns and climate gas mole fractions to finally receive a characterization of the sampling site with regard to the key processes driving CO2 and CH4 concentration levels. The first step entails a reliable radon-based filtering approach to subdivide the detected air masses according to their regional or 'background' origin. Simultaneously, a large number of ten-day back-trajectories from Schneefernerhaus every two hours over the entire study period 2011 - 2015 is calculated with the Lagrangian transport and dispersion model FLEXPART (Stohl et al. 2005) and subjected to cluster analysis. The weather- and emission strength-related (short

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

    Science.gov (United States)

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

    2015-01-01

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

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

    Directory of Open Access Journals (Sweden)

    S.M. Green

    2017-03-01

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

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

    Science.gov (United States)

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

    2012-12-01

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

  11. Measurements of 14C in ancient ice from Taylor Glacier, Antarctica constrain in situ cosmogenic 14CH4 and 14CO production rates

    Science.gov (United States)

    Petrenko, Vasilii V.; Severinghaus, Jeffrey P.; Schaefer, Hinrich; Smith, Andrew M.; Kuhl, Tanner; Baggenstos, Daniel; Hua, Quan; Brook, Edward J.; Rose, Paul; Kulin, Robb; Bauska, Thomas; Harth, Christina; Buizert, Christo; Orsi, Anais; Emanuele, Guy; Lee, James E.; Brailsford, Gordon; Keeling, Ralph; Weiss, Ray F.

    2016-03-01

    Carbon-14 (14C) is incorporated into glacial ice by trapping of atmospheric gases as well as direct near-surface in situ cosmogenic production. 14C of trapped methane (14CH4) is a powerful tracer for past CH4 emissions from ;old; carbon sources such as permafrost and marine CH4 clathrates. 14C in trapped carbon dioxide (14CO2) can be used for absolute dating of ice cores. In situ produced cosmogenic 14C in carbon monoxide (14CO) can potentially be used to reconstruct the past cosmic ray flux and past solar activity. Unfortunately, the trapped atmospheric and in situ cosmogenic components of 14C in glacial ice are difficult to disentangle and a thorough understanding of the in situ cosmogenic component is needed in order to extract useful information from ice core 14C. We analyzed very large (≈1000 kg) ice samples in the 2.26-19.53 m depth range from the ablation zone of Taylor Glacier, Antarctica, to study in situ cosmogenic production of 14CH4 and 14CO. All sampled ice is >50 ka in age, allowing for the assumption that most of the measured 14C originates from recent in situ cosmogenic production as ancient ice is brought to the surface via ablation. Our results place the first constraints on cosmogenic 14CH4 production rates and improve on prior estimates of 14CO production rates in ice. We find a constant 14CH4/14CO production ratio (0.0076 ± 0.0003) for samples deeper than 3 m, which allows the use of 14CO for correcting the 14CH4 signals for the in situ cosmogenic component. Our results also provide the first unambiguous confirmation of 14C production by fast muons in a natural setting (ice or rock) and suggest that the 14C production rates in ice commonly used in the literature may be too high.

  12. Seasonal changes of CO2, CH4 and N2O fluxes in relation to land-use change in tropical peatlands located in coastal area of South Kalimantan

    International Nuclear Information System (INIS)

    Inubushi, K.; Furukawa, Y.; Hadi, A.; Purnomo, E.; Tsuruta, H.

    2003-01-01

    Tropical peatland could be a source of greenhouse gases emission because it contains large amounts of soil carbon and nitrogen. However these emissions are strongly influenced by soil moisture conditions. Tropical climate is characterized typically by wet and dry seasons. Seasonal changes in the emission of carbon dioxide (CO 2 ), methane (CH 4 ) and nitrous oxide (N 2 O) were investigated over a year at three sites (secondary forest, paddy field and upland field) in the tropical peatland in South Kalimantan, Indonesia. The amount of these gases emitted from the fields varied widely according to the seasonal pattern of precipitation, especially methane emission rates were positively correlated with precipitation. Converting from secondary forest peatland to paddy field tended to increase annual emissions of CO 2 and CH 4 to the atmosphere (from 1.2 to 1.5 kg CO 2 -C m -2 y -1 and from 1.2 to 1.9 g CH 4 -C m -2 y -1 ), while changing land-use from secondary forest to upland tended to decrease these gases emissions (from 1.2 to 1.0 kg CO 2 -C m -2 y -1 and from 1.2 to 0.6 g CH 4 -C m -2 y -1 ), but no clear trend was observed for N 2 O which kept negative value as annual rates at three sites. (Author)

  13. Formation and High-order Carboxylic Acids (RCOOH) in Interstellar Analogous Ices of Carbon Dioxide (CO2) and Methane(CH4)

    Science.gov (United States)

    Zhu, Cheng; Turner, Andrew M.; Abplanalp, Matthew J.; Kaiser, Ralf I.

    2018-01-01

    This laboratory study simulated the abiotic formation of carboxylic acids (RCOOH) in interstellar analogous ices of carbon dioxide (CO2) and methane (CH4) at 10 K upon exposure to energetic electrons. The chemical processing of the ices and the subsequent warm-up phase were monitored online and in situ, exploiting Fourier Transform Infrared Spectrometry and quadrupole mass spectrometry. Characteristic absorptions of functional groups of carboxylic acids (RCOOH) were observed in the infrared spectra of the irradiated ice. Two proposed reaction mechanisms replicated the kinetic profiles of the carboxylic acids along with the decay profile of the precursors during the irradiation via hydrocarbon formation, followed by carboxylation and/or through acetic acid along with mass growth processes of the alkyl chain. Mass spectra recorded during the warm-up phase demonstrated that these acids are distributed from acetic acid (CH3COOH) up to decanoic acid (C9H19COOH). High-dose irradiation studies (91 ± 14 eV) converted low-molecular-weight acids such as acetic acid (CH3COOH) and propionic acid (C2H5COOH) to higher-molecular-weight carboxylic acids, compared to low-dose irradiation studies (18 ± 3 eV). The traces of the {{{H}}}2{{C}}= {{C}}({OH}{)}2+ (m/z = 60) fragment—a link to linear carboxylic acids—implied that higher-order acids (C n H2n+1COOH, n ≥ 5) are likely branched, which correlates with the recent analysis of the structures of the monocarboxylic acids in the Murchison meteorite.

  14. Redução da emissão de CO2, CH4 e H2S através da compostagem de dejetos suínos Reduction emissions of CO2, CH4 and H2S through composting of swine manure

    Directory of Open Access Journals (Sweden)

    Luana G. Sardá

    2010-09-01

    Full Text Available Em conjunto com o crescente desenvolvimento da tecnologia para a produção de suínos ocorreu uma forte exploração e degradação do ambiente, razão pela qual a atividade se transformou em fonte poluidora das regiões produtoras. Buscam-se, então, alternativas que minimizem o potencial poluidor do atual sistema de produção. O trabalho proposto foi comparar o perfil de emissão de dióxido de carbono (CO2, metano (CH4 e gás sulfídrico (H2S do manejo de dejetos suínos nas formas sólida (compostagem e líquida (esterqueira, e avaliar a eficiência do processo de compostagem através dos parâmetros físico-químicos. O ensaio foi implantado no campo experimental da EMBRAPA Suínos e Aves, localizada no município de Concórdia, SC. Contatou-se, na compostagem, uma redução de 7 vezes na emissão de CH4, com relação à esterqueira; a emissão de CO2 representou 78,5% do carbono total mineralizado. Considerando-se que a emissão de H2S foi expressiva apenas no manejo dos dejetos na forma líquida, pode-se afirmar que o manejo dos resíduos na forma sólida é uma alternativa para a redução dos impactos ambientais pela mitigação do efeito estufa e pela redução de odores.In conjunction with the development of technologies for the production of swine meat, a strong exploration and degradation of the environment occurred and the activity became a source of pollution in the producing regions. Therefore, there is a need for alternative technologies that minimize the pollutant potential of the current system of production. The proposed work was to analyze and to compare the emission of carbon dioxide (CO2, methane (CH4 and hydrogen sulfide (H2S between the management of swine manure in solid form (composting and liquid manure (deep pit, and assess the efficiency of the process of composting through the physical and chemical parameters. The test was implemented in the experimental field of Embrapa Suínos e Aves, located in Concordia (SC

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

    International Nuclear Information System (INIS)

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

    2015-01-01

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

  16. Greenhouse effect gases sources and sinks (CO2, CH4, N2O) in grasslands and reduction strategies. Greenhouse effect gases prairies. Final report of the second part of the project. April 2004

    International Nuclear Information System (INIS)

    Soussana, J.F.

    2004-04-01

    The project 'GES-Prairies' (Greenhouse Gases - Grasslands) had two main objectives: 1. To measure more accurately the fluxes of CO 2 , CH 4 and N 2 O of French grasslands and determine the greenhouse gas (GHG) balance of these areas. 2. To calculate the net GHG emissions of cattle production farms and finally to propose and evaluate some management scenarios leading to a reduction of GHG emissions. This project deals with three different spatial scales: the field scale, the farm scale and finally, the regional scale. At the field scale, during two years, fluxes of CO 2 , CH 4 and N 2 O were measured in a mid-mountain permanent grassland, previously managed intensively by cutting and grazing (Laqueuille, Auvergne, France). Results from the first complete year of measurements show that the extensification process (reduction of the stocking rate and stopping N fertilization) allows to stock more carbon in the ecosystem. At the farm scale, We developed a model (FARMSIM, coupled to PASIM) able to simulate the GHG balance of a livestock farm. FARMSIM has been tested with data obtained from a mixed livestock farm in Lorraine (dairy and meat production, annual average stocking rate = 1.3 LU ha -1 ) of 100 ha (including 76 ha of grasslands and 21 of annual crops). The results indicate a net emission of 175 t equivalent C-CO 2 for this farm. If expressed per unit of product, it represents 1.34 t equivalent C-CO 2 per LU and per year or 0.54 kg CO 2 per kg of milk and per year. At the regional scale/. The PASIM model has been used to simulate the European grasslands with a spatial resolution of 1' (about 200 * 200 km). For each grid cell, a sensibility analysis allowed to determine the N application which correspond to 30% of the N application that would maximize the annual yield of the pasture. Simulation runs on mixed systems (combining grazing and cutting) show that almost one half of the grassland area is, on average, used for cutting. These simulations predict N 2 O

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

    Data.gov (United States)

    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...

  18. One-Pot Synthesis of Cu-Nanocluster-Decorated Brookite TiO2 Quasi-Nanocubes for Enhanced Activity and Selectivity of CO2 Photoreduction to CH4.

    Science.gov (United States)

    Jin, Jingpeng; Luo, Jiang; Zan, Ling; Peng, Tianyou

    2017-11-17

    A new kind of metallic Cu-loaded brookite TiO 2 composite, in which Cu nanoclusters with a small size of 1-3 nm are decorated on brookite TiO 2 quasi nanocube (BTN) surfaces (hereafter referred to as Cu-BTN), is synthesized via a one-pot hydrothermal process and then used as photocatalyst for CO 2 reduction. It was found that the decoration of Cu nanoclusters on BTN surfaces can improve the activity and selectivity of CO 2 photoreduction to CH 4 , and 1.5 % Cu-BTN gives a maximum overall photocatalytic activity (150.9 μmol g -1  h -1 ) for CO/CH 4 production, which is ≈11.4 and ≈3.3 times higher than those of pristine BTN (13.2 μmol g -1  h -1 ) and Ag-BTN (45.2 μmol g -1  h -1 ). Moreover, the resultant Cu-BTN products can promote the selective generation of CH 4 as compared to CO due to the number of surface oxygen vacancies and the CO 2 /H 2 O adsorption behavior, which differs from that of the pristine BTN. The present results demonstrate that brookite TiO 2 would be a potential effective photocatalyst for CO 2 photoreduction, and that Cu nanoclusters can act as an inexpensive and efficient co-catalyst alternative to the commonly used noble metals to improve the photoactivity and selectivity for CO 2 reduction to CH 4 . © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

    Science.gov (United States)

    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.

  20. How well can we assess impacts of agricultural land management changes on the total greenhouse gas balance (CO2, CH4 and N2O) of tropical rice-cropping systems with biogeochemical models?

    Science.gov (United States)

    Kraus, David; Weller, Sebastian; Janz, Baldur; Klatt, Steffen; Santabárbara, Ignacio; Haas, Edwin; Werner, Christian; Wassmann, Reiner; Kiese, Ralf; Butterbach-Bahl, Klaus

    2016-04-01

    Paddy rice cultivation is increasingly challenged by physical and economic irrigation water scarcity. This already results in the trend of converting paddy rice to upland crop cultivation (e.g., maize, aerobic rice) in large parts of South East Asia. Such land management change from flooded lowland systems to well-aerated upland systems drastically affects soil C and N cycling and related emissions of greenhouse gases. Emissions of methane (CH4) are expected to decrease, while emissions of nitrous oxide (N2O) will most likely increase. In addition to such fast evolving 'pollution swapping' it is expected that on longer time scales significant amounts of soil organic carbon (SOC) stocks will be lost in form of carbon dioxide (CO2). Within the DFG-funded research unit ICON (Introducing non-flooded crops in rice-dominated landscapes: Impact on carbon, nitrogen and water cycles), we investigated environmental impacts of land management change from historical paddy rice cultivation to the upland crops maize and aerobic rice at experimental sites at the International Rice Research Institute (IRRI), the Philippines. To present, more than three years of continuous measurement data of CH4 and N2O emissions under different fertilization regimes have been collected. In addition, measurements of SOC contents and bulk densities in different soil horizons allow for an overall very good characterization of the environmental impacts of mentioned land management change. In this contribution we will show how well mentioned land management change effects in tropical agricultural systems can be represented and thus better understood by the help of process-based biogeochemical models. Seasonal emissions of CH4 and N2O are simulated with r2 values of 0.85 and 0.78 and average underestimations of 15 and 14 %, respectively. These underestimations predominantly originate from treatments in which no fertilizer is applied (CH4) as well as uncertainties of soil hydrology (N2O). Long

  1. Effect of the Amide Bond Diamine Structure on the CO 2 , H 2 S, and CH 4 Transport Properties of a Series of Novel 6FDA-Based Polyamide–Imides for Natural Gas Purification

    KAUST Repository

    Vaughn, J.

    2012-09-11

    A series of higher permeability polyamide-imides based on 2,2′-bis(3,4-dicarboxyphenyl) hexafluoropropane dianhydride with comparable plasticization resistance to Torlon were synthesized and formed into dense film membranes. Polymers possessing 2,4-diamino mesitylene (DAM) were stable up to 56 atm of pure CO 2, which is due to enhanced charge transfer complex formation compared to polymers containing 4,4′- (hexafluoroisopropylidene) dianiline (6FpDA) and 2,3,5,6-tetramethyl-1,4- phenylenediamine (TmPDA). The new polymers containing DAM and TmPDA showed ideal CO 2/CH 4 selectivities of near 50 with CO 2 and H 2S permeabilities over an order of magnitude higher than Torlon. CO 2 and CH 4 sorption in the DAM- and TmPDA-based materials was reduced, whereas H 2S sorption was enhanced relative to membranes containing fluorinated 6FpDA. Consequently, DAM- and TmPDA-based membranes showed increased stability toward high pressure CO 2 but lower plasticization resistance toward pure H 2S. These results highlight the differences between CO 2 and H 2S that challenge the rational design of materials targeting simultaneous separation of both contaminants. © 2012 American Chemical Society.

  2. Impact of elevated CO2 and temperature on soil C and N dynamics in relation to CH4 and N2O emissions from tropical flooded rice (Oryza sativa L.).

    Science.gov (United States)

    Bhattacharyya, P; Roy, K S; Neogi, S; Dash, P K; Nayak, A K; Mohanty, S; Baig, M J; Sarkar, R K; Rao, K S

    2013-09-01

    A field experiment was carried out to investigate the impact of elevated carbon dioxide (CO2) (CEC, 550 μmol mol(-1)) and elevated CO2+elevated air temperature (CECT, 550 μmol mol(-1) and 2°C more than control chamber (CC)) on soil labile carbon (C) and nitrogen (N) pools, microbial populations and enzymatic activities in relation to emissions of methane (CH4) and nitrous oxide (N2O) in a flooded alluvial soil planted with rice cv. Naveen in open top chambers (OTCs). The labile soil C pools, namely microbial biomass C, readily mineralizable C, water soluble carbohydrate C and potassium permanganate oxidizable C were increased by 27, 23, 38 and 37% respectively under CEC than CC (ambient CO2, 394 μmol mol(-1)). The total organic carbon (TOC) in root exudates was 28.9% higher under CEC than CC. The labile N fractions were also increased significantly (29%) in CEC than CC. Methanogens and denitrifier populations in rhizosphere were higher under CEC and CECT. As a result, CH4 and N2O-N emissions were enhanced by 26 and 24.6% respectively, under CEC in comparison to open field (UC, ambient CO2, 394 μmol mol(-1)) on seasonal basis. The global warming potential (GWP) was increased by 25% under CEC than CC. However, emissions per unit of grain yield under elevated CO2 and temperature were similar to those observed at ambient CO2. The stimulatory effect on CH4 and N2O emissions under CEC was linked with the increased amount of soil labile C, C rich root exudates, lowered Eh, higher Fe(+2) concentration and increased activities of methanogens and extracellular enzymes. Copyright © 2013 Elsevier B.V. All rights reserved.

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

    Science.gov (United States)

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

    2014-12-01

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

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

    Science.gov (United States)

    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.

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

    Science.gov (United States)

    Hoffmann, Mathias; Schulz-Hanke, Maximilian; Garcia Alba, Joana; Jurisch, Nicole; Hagemann, Ulrike; Sachs, Torsten; Sommer, Michael; Augustin, Jürgen

    2016-04-01

    Processes driving methane (CH4) emissions in wetland ecosystems are highly complex. Especially, the separation of CH4 emissions into ebullition and diffusion derived flux components, a perquisite for the mechanistic process understanding and identification of potential environmental driver is rather challenging. We present a simple calculation algorithm, based on an adaptive R-script, which separates open-water, closed chamber CH4 flux measurements into diffusion- and ebullition-derived components. Hence, flux component specific dynamics are revealed and potential environmental driver identified. Flux separation is based on a statistical approach, using ebullition related sudden concentration changes obtained during high resolution CH4 concentration measurements. By applying the lower and upper quartile ± the interquartile range (IQR) as a variable threshold, diffusion dominated periods of the flux measurement are filtered. Subsequently, flux calculation and separation is performed. The algorithm was verified in a laboratory experiment and tested under field conditions, using flux measurement data (July to September 2013) from a flooded, former fen grassland site. Erratic ebullition events contributed 46% to total CH4 emissions, which is comparable to values reported by literature. Additionally, a shift in the diurnal trend of diffusive fluxes throughout the measurement period, driven by the water temperature gradient, was revealed.

  6. Assessing methane oxidation under landfill covers and its contribution to the above atmospheric CO2 levels: The added value of the isotope (δ13C and δ18O CO2; δ13C and δD CH4) approach

    International Nuclear Information System (INIS)

    Widory, D.; Proust, E.; Bellenfant, G.; Bour, O.

    2012-01-01

    Highlights: ► Comparison of the isotope and mass balance approaches to evaluate the level of methane oxidation within a landfill. ► The level of methane oxidation is not homogenous under the landfill cover and is strongly correlated to the methane flux. ► Isotope tracking of the contribution of the methane oxidation to the CO 2 concentrations in the ambient air. - Abstract: We are presenting here a multi-isotope approach (δ 13 C and δ 18 O of CO 2 ; δ 13 C and δD of CH 4 ) to assess (i) the level(s) of methane oxidation during waste biodegradation and its migration through a landfill cover in Sonzay (France), and (ii) its contribution to the atmospheric CO 2 levels above the surface. The isotope approach is compared to the more conventional mass balance approach. Results from the two techniques are comparable and show that the CH 4 oxidation under the landfill cover is heterogenous, with low oxidation percentages in samples showing high biogas fluxes, which was expected in clay covers presenting fissures, through which CH 4 is rapidly transported. At shallow depth, more immobile biogas pockets show a higher level of CH 4 oxidation by the methanotrophic bacteria. δ 13 C of CO 2 samples taken at different heights (from below the cover up to 8 m above the ground level) were also used to identify and assess the relative contributions of its main sources both under the landfill cover and in the surrounding atmosphere.

  7. Effects of Climate Change and Organic Matter Amendments on the Fate of Soil Carbon and the Global Warming Potential of CO2, CH4, and N2O Emissions in an Upland Soil

    Science.gov (United States)

    Simmonds, M.; Muehe, E. M.; Fendorf, S. E.

    2017-12-01

    Our current understanding of the mechanisms driving carbon stabilization in soil organic matter (SOM) and its release to the atmosphere is insufficient for predicting the response of soil carbon dynamics to future climatic conditions. The persistence of SOM has been studied primarily within the context of biochemical, physical, and geochemical protection from decomposition. More recently, bioenergetic constraints on SOM decomposition due to oxygen limitations have been demonstrated in submerged soils. However, the relevance of anaerobic domains in upland soils is uncertain. To better understand how upland soils will respond to climate change, we conducted a 52-day incubation of an upland soil at constant soil moisture (field capacity) under varying air temperatures (32°C and 37°C), CO2 concentrations (398 and 850 ppmv), and soil organic carbon contents (1.3%, 2.4%). Overall, we observed a stimulatory effect of future climate (elevated temperature and CO2) and higher carbon inputs on net SOM mineralization rates (higher CO2, CH4 and N2O emissions). Importantly, CH4 emissions were observed in the soils with added plant residue, indicating anaerobic microsites are relevant in upland soils, and significantly impact microbial respiration pathways, rates of SOM mineralization, and the global warming potential of trace gas emissions. These findings have important implications for positive soil carbon-climate feedbacks, and warrant further investigation into representing anaerobic soil domains of upland soils in biogeochemical models.

  8. Evaluation of the greenhouse effect gases (CO2, CH4, N2O) in grass land and in the grass breeding. Greenhouse effect gases prairies. report of the first part of the project December 2002

    International Nuclear Information System (INIS)

    Soussana, J.F.

    2002-12-01

    In the framework of the Kyoto protocol on the greenhouse effect gases reduction, many ecosystems as the prairies can play a main role for the carbon sequestration in soils. The conservation of french prairies and their management adaptation could allow the possibility of carbon sequestration in the soils but also could generate emissions of CO 2 and CH 4 (by the breeding animals on grass) and N 2 O (by the soils). This project aims to establish a detailed evaluation of the contribution of the french prairies to the the greenhouse effect gases flux and evaluate the possibilities of reduction of the emissions by adaptation of breeding systems. (A.L.B.)

  9. Gases (CH4, CO2 and N2 and pore water chemistry in the surface sediments of Lake Orta, Italy: acidification effects on C and N gas cycling

    Directory of Open Access Journals (Sweden)

    Donald D. ADAMS

    2001-02-01

    Full Text Available Lake Orta, a subalpine, warm monomictic lake in northwestern Italy was heavily polluted from rayon factory discharges of ammonium and copper since 1926. In the 1950s accumulations of contaminants resulted in whole lake pHs of 3.8-4.0 from ammonium oxidation. Partial remediation started in the 1950s, but by 1985-89 the water remained acidified at pHs of 4.0. Artificial liming (14,500 t in 1989-90 resulted in improved water quality and substantial recovery of the biological community. Sediment gases, sampled in 1989 before liming, from the lake's four basins showed severe inhibition of methanogenesis (CH4 = 0.0-0.15 mM in the surface sediments (0.5-5 cm of the southern basin, location of the plant effluent, as compared to the deep central and northern basins (0.9-1.4 mM. Four years after liming, cores collected in 1994 near the 1989 southern basin sites showed a slight change in surface sediment methane (0.07-0.82 mM, yet suggested continual sediment toxicity, at least to carbon cycling through methanogenesis. Calculations of diffuse flux of CH4 at the sediment-water interface (SWI in 1989 were 6.6-7.4 mM m-2 day-1 for the central and northern basins and 0.13 for the southern basin. CH4 fluxes increased 16x to 2 mM m-2 day-1 in 1994 in the southern basin, possibly from remediation of near surface sediments. The impact of pollution on denitrification (formation of sediment N2 gas was not so obvious since two processes could counteract each other (high NO3 - stimulating denitrification versus possible negative effects from acidity and metals. The calculated flux of N2 from the southern basin sediments increased 5x four years after liming compared to the period of acidification, suggesting possible toxicity towards denitrifiers during the earlier period. Core overlying water (0.68 mM exhibited N2 concentrations close to saturation, while most surface sediments were twice as much (1.5 mM. Surface (0-6 cm sediment N2 was similar at most sites, with the

  10. Net Fluxes of CO2, but not N20 or CH4, are Affected Following Agronomic-Scale Additions of Urea to Prairie and Arable Soils

    Science.gov (United States)

    Microbial production of carbon dioxide (CO2) increased with nitrogen (N) application rate for both arable and prairie soils incubated at 21 °C. Rate of N applied as urea (0, 11, 56, 112 kg N ha-1) did not affect soil methane consumption and nitrous oxide production for soil collected from either ec...

  11. Laboratory-scale measurements of N2O and CH4 emissions from hybrid poplars (Populus deltoides x Populus nigra).

    Science.gov (United States)

    McBain, M C; Warland, J S; McBride, R A; Wagner-Riddle, C

    2004-12-01

    The purpose of this study was to determine whether or not young hybrid poplar (Populus deltoides x Populus nigra) could transport landfill biogas internally from the root zone to the atmosphere, thereby acting as conduits for landfill gas release. Fluxes of methane (CH4) and nitrous oxide (N2O) from the seedlings to the atmosphere were measured under controlled conditions using dynamic flux chambers and a tunable diode laser trace gas analyser (TDLTGA). Nitrous oxide was emitted from the seedlings, but only when extremely high soil N2O concentrations were applied to the root zone. In contrast, no detectable emissions of CH4 were measured in a similar experimental trial. Visible plant morphological responses, characteristic of flood-tolerant trees attempting to cope with the negative effects of soil hypoxia, were observed during the CH4 experiments. Leaf chlorosis, leaf abscission and adventitious roots were all visible plant responses. In addition, seedling survival was observed to be highest in the biogas 'hot spot' areas of a local municipal solid waste landfill involved in this study. Based on the available literature, these observations suggest that CH4 can be transported internally by Populus deltoides x Populus nigra seedlings in trace amounts, although future research is required to fully test this hypothesis.

  12. SYNGAS PRODUCTION FROM CO2-REFORMING OF CH4 OVER SOL-GEL SYNTHESIZED Ni-Co/Al2O3-MgO-ZrO2 NANOCATALYST: EFFECT OF ZrO2 PRECURSOR ON CATALYST PROPERTIES AND PERFORMANCE

    Directory of Open Access Journals (Sweden)

    Seyed Mehdi Sajjadi

    2015-05-01

    Full Text Available Ni-Co/Al2O3-MgO-ZrO2 nanocatalyst with utilization of two different zirconia precursors, namely, zirconyl nitrate hydrate (ZNH and zirconyl nitrate solution (ZNS, was synthesized via the sol-gel method. The physiochemical properties of nanocatalysts were characterized by XRD, FESEM, EDX, BET and FTIR analyses and employed for syngas production from CO2-reforming of CH4. XRD patterns, exhibiting proper crystalline structure and homogeneous dispersion of active phase for the nanocatalyst ZNS precursor employed (NCAMZ-ZNS. FESEM and BET results of NCAMZ-ZNS presented more uniform morphology and smaller particle size and consequently higher surface areas. In addition, average particle size of NCAMZ-ZNS was 15.7 nm, which is close to the critical size for Ni-Co catalysts to avoid carbon formation. Moreover, FESEM analysis indicated both prepared samples were nanoscale. EDX analysis confirmed the existence of various elements used and also supported the statements made in the XRD and FESEM analyses regarding dispersion. Based on the excellent physiochemical properties, NCAMZ-ZNS exhibited the best reactant conversion across all of the evaluated temperatures, e.g. CH4 and CO2 conversions were 97.2 and 99% at 850 ºC, respectively. Furthermore, NCAMZ-ZNS demonstrated a stable yield with H2/CO close to unit value during the 1440 min stability test.

  13. Fundamental Understanding of Methane-Carbon Dioxide-Water (CH4-CO2-H2O) Interactions in Shale Nanopores under Reservoir Conditions.

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Yifeng [Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

    2018-02-01

    Shale is characterized by the predominant presence of nanometer-scale (1-100 nm) pores. The behavior of fluids in those pores directly controls shale gas storage and release in shale matrix and ultimately the wellbore production in unconventional reservoirs. Recently, it has been recognized that a fluid confined in nanopores can behave dramatically differently from the corresponding bulk phase due to nanopore confinement (Wang, 2014). CO2 and H2O, either preexisting or introduced, are two major components that coexist with shale gas (predominately CH4) during hydrofracturing and gas extraction. Note that liquid or supercritical CO2 has been suggested as an alternative fluid for subsurface fracturing such that CO2 enhanced gas recovery can also serve as a CO2 sequestration process. Limited data indicate that CO2 may preferentially adsorb in nanopores (particularly those in kerogen) and therefore displace CH4 in shale. Similarly, the presence of water moisture seems able to displace or trap CH4 in shale matrix. Therefore, fundamental understanding of CH4-CO2-H2O behavior and their interactions in shale nanopores is of great importance for gas production and the related CO2 sequestration. This project focuses on the systematic study of CH4-CO2-H2O interactions in shale nanopores under high-pressure and high temperature reservoir conditions. The proposed work will help to develop new stimulation strategies to enable efficient resource recovery from fewer and less environmentally impactful wells.

  14. Stable isotope measurements of atmospheric CO2

    International Nuclear Information System (INIS)

    White, J.W.C.; Ferretti, D.F.; Vaughn, B.H.; Francey, R.J.; Allison, C.E.

    2002-01-01

    The measurement of stable carbon isotope ratios of atmospheric carbon dioxide, δ 13 CO 2 are useful for partitioning surface-atmospheric fluxes into terrestrial and oceanic components. δC 18 OO also has potential for segregating photosynthetic and respiratory fluxes in terrestrial ecosystems. Here we describe in detail the techniques for making these measurements. The primary challenge for all of the techniques used to measure isotopes of atmospheric CO 2 is to achieve acceptable accuracy and precision and to maintain them over the decades needed to observe carbon cycle variability. The keys to success such an approach are diligent intercalibrations of laboratories from around the world, as well as the use of multiple techniques such as dual inlet and GC-IRMS and the intercomparison of such measurements. We focus here on two laboratories, the Stable Isotope Lab at the Institute for Arctic and Alpine Research (INSTAAR) at the University of Colorado is described and the Commonwealth Scientific and Industrial Research Organisation - Atmospheric Research (CSIRO). Different approaches exist at other laboratories (e.g. programs operated by Scripps Institution of Oceanography (SIO) and The Center for Atmospheric and Oceanic Studies, Toboku University (TU)) however these are not discussed here. Finally, we also discuss the recently developed Gas Chromatography - Isotope Ratio Mass Spectrometry (GC-IRMS) technique which holds significant promise for measuring ultra-small samples of gas with good precision. (author)

  15. Iterative maximum a posteriori (IMAP-DOAS for retrieval of strongly absorbing trace gases: Model studies for CH4 and CO2 retrieval from near infrared spectra of SCIAMACHY onboard ENVISAT

    Directory of Open Access Journals (Sweden)

    C. Frankenberg

    2005-01-01

    Full Text Available In the past, differential optical absorption spectroscopy (DOAS has mostly been employed for atmospheric trace gas retrieval in the UV/Vis spectral region. New spectrometers such as SCIAMACHY onboard ENVISAT also provide near infrared channels and thus allow for the detection of greenhouse gases like CH4, CO2, or N2O. However, modifications of the classical DOAS algorithm are necessary to account for the idiosyncrasies of this spectral region, i.e. the temperature and pressure dependence of the high resolution absorption lines. Furthermore, understanding the sensitivity of the measurement of these high resolution, strong absorption lines by means of a non-ideal device, i.e. having finite spectral resolution, is of special importance. This applies not only in the NIR, but can also prove to be an issue for the UV/Vis spectral region. This paper presents a modified iterative maximum a posteriori-DOAS (IMAP-DOAS algorithm based on optimal estimation theory introduced to the remote sensing community by rodgers76. This method directly iterates the vertical column densities of the absorbers of interest until the modeled total optical density fits the measurement. Although the discussion in this paper lays emphasis on satellite retrieval, the basic principles of the algorithm also hold for arbitrary measurement geometries. This new approach is applied to modeled spectra based on a comprehensive set of atmospheric temperature and pressure profiles. This analysis reveals that the sensitivity of measurement strongly depends on the prevailing pressure-height. The IMAP-DOAS algorithm properly accounts for the sensitivity of measurement on pressure due to pressure broadening of the absorption lines. Thus, biases in the retrieved vertical columns that would arise in classical algorithms, are obviated. Here, we analyse and quantify these systematic biases as well as errors due to variations in the temperature and pressure profiles, which is indispensable for

  16. Tunable diode laser in-situ CH4 measurements aboard the CARIBIC passenger aircraft: instrument performance assessment

    Science.gov (United States)

    Dyroff, C.; Zahn, A.; Sanati, S.; Christner, E.; Rauthe-Schöch, A.; Schuck, T. J.

    2014-03-01

    A laser spectrometer for automated monthly measurements of methane (CH4) mixing ratios aboard the CARIBIC passenger aircraft is presented. The instrument is based on a commercial Fast Greenhouse Gas Analyser (FGGA, Los Gatos Res.), which was adapted to meet the requirements imposed by unattended airborne operation. It was characterised in the laboratory with respect to instrument stability, precision, cross sensitivity to H2O, and accuracy. For airborne operation, a calibration strategy is described that utilises CH4 measurements obtained from flask samples taken during the same flights. The precision of airborne measurements is 2 ppb for 10 s averages. The accuracy at aircraft cruising altitude is 3.85 ppb. During aircraft ascent and descent, where no flask samples were obtained, instrumental drifts can be less accurately determined and the uncertainty is estimated to be 12.4 ppb. A linear humidity bias correction was applied to the CH4 measurements, which was most important in the lower troposphere. On average, the correction bias was around 6.5 ppb at an altitude of 2 km, and negligible at cruising flight level. Observations from 103 long-distance flights are presented that span a large part of the northern hemispheric upper troposphere and lowermost stratosphere (UT/LMS), with occasional crossing of the tropics on flights to southern Africa. These accurate data mark the largest UT/LMS in-situ CH4 dataset worldwide. An example of a tracer-tracer correlation study with ozone is given, highlighting the possibility for accurate cross-tropopause transport analyses.

  17. Strategic use of the underground for an energy mix plan, synergies among CO2 and CH4 Geological Storage and Geothermal Energy: Italian Energy review and Latium case study

    Science.gov (United States)

    Procesi, M.; Cantucci, B.; Buttinelli, M.; Armezzani, G.; Quattrocchi, F.

    2012-04-01

    Since the world-wide energy demand has been growing so much in the last years, it is necessary to develop a strategic mix-energy plan to supply low GHG (GreenHouseGas) emissions energy and solve the problem of CO2 emission increasing. A recent study published by European Commission shows that, if existing trends continue, by 2050 CO2 emissions will be unsustainably high: 900-1000 parts per million by volume. The European Commission in 2007 underline the necessity to elaborate, at European level, a Strategic Energy Technology Plan focused on non-carbon or reduced-carbon sources of energy, as renewable energies, CO2 capture and storage technologies, smart energy networks and energy efficiency and savings. Future scenarios for 2030 elaborated by the International Energy Agency (IEA) shows as a mix energy plan could reduce the global CO2 emissions from 27Gt to 23 Gt (about 15%). A strategic use of the underground in terms of: - development of CCS (Carbon dioxide Capture and Storage) associated to fossil fuel combustion; - increase of CH4 geological storage sites; - use of renewable energies as geothermic for power generation; could open a new energy scenario, according to the climate models published by IPCC. Nowadays CCS market is mainly developed in USA and Canada, but still not much accounted in Europe. In Italy there aren't active CCS projects, even if potential areas have been already identified. Many CH4 storage sites are located in Northern America, while other are present in Europe and Italy, but the number of sites is limited despite the huge underground potentiality. In Italy the power generation from geothermal energy comes exclusively from Tuscany (Larderello-Travale and Mt. Amiata geothermal fields) despite the huge potentiality of other regions as Latium, Campania and Sicily (Central and South Italy). The energy deficit and the relevant CO2 emissions represent a common status for many Italian regions, especially for the Latium Region. This suggests that a

  18. Suitability of quantum cascade laser spectroscopy for CH4 and N2O eddy covariance flux measurements

    Directory of Open Access Journals (Sweden)

    A. T. Vermeulen

    2007-08-01

    Full Text Available A quantum cascade laser spectrometer was evaluated for eddy covariance flux measurements of CH4 and N2O using three months of continuous measurements at a field site. The required criteria for eddy covariance flux measurements including continuity, sampling frequency, precision and stationarity were examined. The system operated continuously at a dairy farm on peat grassland in the Netherlands from 17 August to 6 November 2006. An automatic liquid nitrogen filling system for the infrared detector was employed to provide unattended operation of the system. The electronic sampling frequency was 10 Hz, however, the flow response time was 0.08 s, which corresponds to a bandwidth of 2 Hz. A precision of 2.9 and 0.5 ppb Hz−1/2 was obtained for CH4 and N2O, respectively. Accuracy was assured by frequent calibrations using low and high standard additions. Drifts in the system were compensated by using a 120 s running mean filter. The average CH4 and N2O exchange was 512 ngC m−2 s−1 (2.46 mg m−2 hr−1 and 52 ngN m−2 s−1 (0.29 mg m−2 hr−1. Given that 40% of the total N2O emission was due to a fertilizing event.

  19. An automated GC-C-GC-IRMS setup to measure palaeoatmospheric δ13C-CH4, δ15N-N2O and δ18O-N2O in one ice core sample

    Directory of Open Access Journals (Sweden)

    P. Sperlich

    2013-08-01

    Full Text Available Air bubbles in ice core samples represent the only opportunity to study the mixing ratio and isotopic variability of palaeoatmospheric CH4 and N2O. The highest possible precision in isotope measurements is required to maximize the resolving power for CH4 and N2O sink and source reconstructions. We present a new setup to measure δ13C-CH4, δ15N-N2O and δ18O-N2O isotope ratios in one ice core sample and with one single IRMS instrument, with a precision of 0.09, 0.6 and 0.7‰, respectively, as determined on 0.6–1.6 nmol CH4 and 0.25–0.6 nmol N2O. The isotope ratios are referenced to the VPDB scale (δ13C-CH4, the N2-air scale (δ15N-N2O and the VSMOW scale (δ18O-N2O. Ice core samples of 200–500 g are melted while the air is constantly extracted to minimize gas dissolution. A helium carrier gas flow transports the sample through the analytical system. We introduce a new gold catalyst to oxidize CO to CO2 in the air sample. CH4 and N2O are then separated from N2, O2, Ar and CO2 before they get pre-concentrated and separated by gas chromatography. A combustion unit is required for δ13C-CH4 analysis, which is equipped with a constant oxygen supply as well as a post-combustion trap and a post-combustion GC column (GC-C-GC-IRMS. The post-combustion trap and the second GC column in the GC-C-GC-IRMS combination prevent Kr and N2O interferences during the isotopic analysis of CH4-derived CO2. These steps increase the time for δ13C-CH4 measurements, which is used to measure δ15N-N2O and δ18O-N2O first and then δ13C-CH4. The analytical time is adjusted to ensure stable conditions in the ion source before each sample gas enters the IRMS, thereby improving the precision achieved for measurements of CH4 and N2O on the same IRMS. The precision of our measurements is comparable to or better than that of recently published systems. Our setup is calibrated by analysing multiple reference gases that were injected over bubble-free ice samples. We show

  20. Combining soil and tree-stem flux measurements and soil gas profiles to understand CH4 pathways in Fagus sylvatica forests

    Czech Academy of Sciences Publication Activity Database

    Maier, M.; Macháčová, Kateřina; Lang, F.; Svobodová, Kateřina; Urban, Otmar

    2018-01-01

    Roč. 181, č. 1 (2018), s. 31-35 ISSN 1436-8730 R&D Projects: GA MŠk(CZ) LO1415 Institutional support: RVO:86652079 Keywords : ch4 * soil gas profile * gas flux * co2 * methanogenesis Subject RIV: ED - Physiology OBOR OECD: Plant sciences, botany Impact factor: 2.102, year: 2016

  1. Measurements and Interpretation of Surface Mixing Ratios of CH4 and CO and δ 13C and δ D of CH4 in Air from Pacific Ocean Transects Between Auckland, New Zealand and Los Angeles, California

    Science.gov (United States)

    Ajie, H. O.; Tyler, S. C.; Gotoh, A. A.; McMillan, A. M.; Rice, A. L.; Lowe, D. C.

    2003-12-01

    We report on measurements of atmospheric CH4 and CO mixing ratios and δ 13C of CH4 from air samples collected every 2.5 to 5° latitude along a transect over the Pacific Ocean using container ships of P&O Nedlloyd (formerly Blue Star) shipping line. Data presented here begins in June 1996 and extends to January 2002. Scientists from the National Institute of Water and Atmospheric Research in New Zealand and from University of California, Irvine alternate sampling trips so that a transect between Auckland, New Zealand (35° S) and Los Angeles, California (35° N) can be sampled over a period of ˜15 days approximately every four months. Data sets from the two laboratories are intercalibrated through a sample exchange program. The data provide detail on the spatial and seasonal variation of CH4 and CO mixing ratios and stable isotope ratios of CH4 over the Pacific equatorial region, including the Intertropical Convergence Zone (ITCZ) and both northern and southern temperate zones to about 30° latitude, including the South Pacific Convergence Zone (SPCZ). Data from 18 transect samplings so far clearly show that δ 13C in the mid latitudes of both hemispheres are ˜6 months out of phase. In June, a minimum in δ 13C CH4 in the southern hemisphere (SH) coincides approximately with the maximum in the northern hemisphere (NH) seasonal cycle. Because the NH is less enriched in 13C than the SH this situation results in a remarkably flat gradient between 30° N and 30° S. In November the opposite situation occurs with the SH mid latitude maximum coinciding with the minimum in the NH cycle, leading to a relatively large gradient of ˜0.5‰ between the hemispheres. We discuss how CH4 and CO mixing ratios are related to the changing positions and strengths of the ITCZ and SPCZ and how this data can be used in multi-dimensional models of atmospheric chemistry and transport to better define CH4 sources and sinks both temporally and spatially.

  2. Methane and CO2 fluxes of moving point sources - Beyond or within the limits of eddy covariance measurements

    Science.gov (United States)

    Felber, Raphael; Neftel, Albrecht; Münger, Andreas; Ammann, Christof

    2014-05-01

    The eddy covariance (EC) technique has been extensively used for CO2 and energy exchange measurements over different ecosystems. For some years, it has been also becoming widely used to investigate CH4 and N2O exchange over ecosystems including grazing systems. EC measurements represent a spatially integrated flux over an upwind area (footprint). Whereas for extended homogenous areas EC measurements work well, the animals in a grazing system are a challenge as they represent moving point sources that create inhomogeneous conditions in space and time. The main issues which have to be taken into account when applying EC flux measurements over a grazed system are: i) In the presence of animals the high time resolution concentration measurements show large spikes in the signal. These spikes may be filtered/reduced by standard quality control software in order to avoid wrong measurements. ii) Data on the position of the animals relative to the flux footprint is needed to quantify the contribution of the grazing animals to the measured flux. For one grazing season we investigated the ability of EC flux measurements to reliably quantify the contribution of the grazing animals to the CH4 and CO2 exchange over pasture systems. For this purpose, a field experiment with a herd of twenty dairy cows in a full-day rotational grazing system was carried out on the Swiss central plateau. Net CH4 and CO2 exchange of the pasture system was measured continuously by the eddy covariance technique (Sonic Anemometer HS-50, Gill Instruments Ltd; FGGA, Los Gatos Research Inc.). To quantify the contribution of the animals to the net flux, the position of the individual cows was recorded using GPS (5 s time resolution) on each animal. An existing footprint calculation tool (ART footprint tool) was adapted and CH4 emissions of the cows were calculated. CH4 emissions from cows could be used as a tracer to investigate the quality of the evaluation of the EC data, since the background exchange of

  3. Uncertainty in CH4 and N2O emission estimates from a managed fen meadow using EC measurements

    International Nuclear Information System (INIS)

    Kroon, P.S.; Hensen, A.; Van 't Veen, W.H.; Vermeulen, A.T.; Jonker, H.

    2009-02-01

    The overall uncertainty in annual flux estimates derived from chamber measurements may be as high as 50% due to the temporal and spatial variability in the fluxes. As even a large number of chamber plots still cover typically less than 1% of the total field area, the field-scale integrated emission necessarily remains a matter of speculation. High frequency micrometeorological methods are a good option for obtaining integrated estimates on a hectare scale with a continuous coverage in time. Instrumentation is now becoming available that meets the requirements for CH4 and N2O eddy covariance (EC) measurements. A system consisting of a quantum cascade laser (QCL) spectrometer and a sonic anemometer has recently been proven to be suitable for performing EC measurements. This study analyses the EC flux measurements of CH4 and N2O and its corrections, like calibration, Webb-correction, and corrections for high and low frequency losses, and assesses the magnitude of the uncertainties associated with the precision of the measurement instruments, measurement set-up and the methodology. The uncertainty of one single EC flux measurement, a daily, monthly and 3-monthly average EC flux is estimated. In addition, the cumulative emission of C-CH4 and N-N2O and their uncertainties are determined over several fertilizing events at a dairy farm site in the Netherlands. These fertilizing events are selected from the continuously EC flux measurements from August 2006 to September 2008. The EC flux uncertainties are compared by the overall uncertainty in annual flux estimates derived from chamber measurements. It will be shown that EC flux measurements can decrease the overall uncertainty in annual flux estimates

  4. Uncertainty in CH4 and N2O emission estimates from a managed fen meadow using EC measurements

    Energy Technology Data Exchange (ETDEWEB)

    Kroon, P.S.; Hensen, A.; Van ' t Veen, W.H.; Vermeulen, A.T. [ECN Biomass, Coal and Environment, Petten (Netherlands); Jonker, H. [Delft University of Technology, Delft (Netherlands)

    2009-02-15

    The overall uncertainty in annual flux estimates derived from chamber measurements may be as high as 50% due to the temporal and spatial variability in the fluxes. As even a large number of chamber plots still cover typically less than 1% of the total field area, the field-scale integrated emission necessarily remains a matter of speculation. High frequency micrometeorological methods are a good option for obtaining integrated estimates on a hectare scale with a continuous coverage in time. Instrumentation is now becoming available that meets the requirements for CH4 and N2O eddy covariance (EC) measurements. A system consisting of a quantum cascade laser (QCL) spectrometer and a sonic anemometer has recently been proven to be suitable for performing EC measurements. This study analyses the EC flux measurements of CH4 and N2O and its corrections, like calibration, Webb-correction, and corrections for high and low frequency losses, and assesses the magnitude of the uncertainties associated with the precision of the measurement instruments, measurement set-up and the methodology. The uncertainty of one single EC flux measurement, a daily, monthly and 3-monthly average EC flux is estimated. In addition, the cumulative emission of C-CH4 and N-N2O and their uncertainties are determined over several fertilizing events at a dairy farm site in the Netherlands. These fertilizing events are selected from the continuously EC flux measurements from August 2006 to September 2008. The EC flux uncertainties are compared by the overall uncertainty in annual flux estimates derived from chamber measurements. It will be shown that EC flux measurements can decrease the overall uncertainty in annual flux estimates.

  5. Phase Equilibrium Measurements and Modeling of 1-Propanethiol+1-Butanethiol + CH4 in Methane Ternary System at 303, 336, and 368 K and Pressure Up to 9 MPa

    DEFF Research Database (Denmark)

    Awan, Javeed A.; Coquelet, Christophe; Tsivintzelis, Ioannis

    2016-01-01

    New vapor-liquid equilibrium (VLE) data for 1-propanethiol + 1-butanethiol + CH4 ternary system is reported. Measurements were performed at three different temperatures (303, 336, and 368 K), and the pressure ranged from 1 to 9 MPa. The total system pressure was maintained by CH4. The inlet mole...

  6. Ground-based DIAL and IPDA Systems for Remote Sensing of CO2, CH4, and H2O near 1.6 µm

    Science.gov (United States)

    Wagner, G. A.; Plusquellic, D. F.

    2017-12-01

    Integrated path differential absorption (IPDA) and differential absorption LIDAR (DIAL) are well established methods to monitor atmospheric constituents. At NIST, IPDA and DIAL systems have been developed as standoff systems and their overall performance has been evaluated through intercomparisons including the traceability to point sensor measurements. The all-fiber IPDA system is based on a low-power (Armstrong, and A. V. Smith, "150-mJ 1550-nm KTA OPO with Good Beam Quality and High Efficiency," SPIE, 5337, 71-80 (2004). 3. K. O. Douglass, S. E. Maxwell, D. F. Plusquellic, J. T. Hodges, R. D. van Zee, D. V. Samarov, J. R. Whetstone, "Construction of a High Power OPO Laser System for Differential Absorption LIDAR," SPIE, 8159, 81590D (2011).

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

    International Nuclear Information System (INIS)

    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

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

    Directory of Open Access Journals (Sweden)

    M. Sasakawa

    2012-03-01

    Full Text Available We described continuous measurements of CH4 and CO2 concentration obtained at two sites placed in the middle taiga, Karasevoe (KRS and Demyanskoe (DEM, in West Siberian Lowland (WSL from 2005 to 2009. Although both CH4 and CO2 accumulation (ΔCH4 and ▵CO2 during night-time at KRS in June and July 2007 showed an anomalously high concentration, higher ratios of ΔCH4CO2 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 ΔCH4CO2 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.

  9. Spectroscopic technique for measuring atmospheric CO2

    International Nuclear Information System (INIS)

    Stokes, G.M.; Stokes, R.A.

    1979-01-01

    As part of a continuing effort to identify areas in which astronomical techniques and data may be profitably applied to atmospheric problems, both new and archival solar spectra have been collected to prepare for an analysis of their use for studying the changes of the atmospheric CO 2 burden. This analysis has resulted in the initiation of an observing program using the Fourier Transform Spectrometer (FTS) of the McMath Solar Telescope at Kitt Peak National Observatory (KPNO). This program is generating spectra, the quality of which should not only aid the archival CO 2 study but also lead to analyses of other trace gases

  10. Recent Experiments Leading to the Characterization of the Performance of Portable (He-Ne)/CH4 Lasers: Part II: Results of the 1986 LPTF Absolute Frequency Measurements

    Science.gov (United States)

    Clairon, A.; Dahmani, B.; Acef, O.; Granveaud, M.; Domnin, Yu S.; Pouchkine, S. B.; Tatarenkov, V. M.; Felder, R.

    1988-01-01

    Comparison of the VNIIFTRI and LPTF frequency multiplication chains has been carried out through the measurement of the frequency of a portable VNIIFTRI (He-Ne)/CH4 laser. Agreement is within 100 Hz (1.1 parts in 1012) and is secured by the very good medium-term frequency repeatability of the (He-Ne)/CH4 VNIIFTRI portable laser (a few parts in 1013). On the same occasion a measurement of the frequency of the BIPM (He-Ne)/CH4 reference laser (B.3) has been performed at LPTF. Other experiments carried out on the BIPM laser show that the reproducibility of the (He-Ne)/CH4 system could be improved by a systematic study and then by a better control of the various perturbing factors which influence the shape of the methane-saturated absorption peak.

  11. CO2 measurements during transcranial Doppler examinations in headache patients

    DEFF Research Database (Denmark)

    Thomsen, L L; Iversen, Helle Klingenberg

    1994-01-01

    Transcranial Doppler (TCD) examinations are increasingly being used in studies of headache pathophysiology. Because blood velocity is highly dependent on PCO2, these parameters should be measured simultaneously. The most common way of performing measurements during TCD examinations is as end......-tidal pCO2 with a capnograph. When patients are nauseated and vomit, as in migraine, the mask or mouthpiece connected to the capnograph represents a problem. We therefore evaluated whether a transcutaneous pCO2 electrode was as useful as the capnograph for pCO2 measurements in TCD examinations. We...... conclude that this is not the case, and recommend capnographic end-tidal pCO2 measurements during TCD examinations. However, transcutaneous pCO2 measurements may represent a supplement to spot measurements of end-tidal pCO2 in stable conditions when long-term monitoring is needed, and the mask...

  12. Sono-synthesis and characterization of bimetallic Ni-Co/Al2O3-MgO nanocatalyst: Effects of metal content on catalytic properties and activity for hydrogen production via CO2 reforming of CH4.

    Science.gov (United States)

    Abdollahifar, Mozaffar; Haghighi, Mohammad; Babaluo, Ali Akbar; Talkhoncheh, Saeed Khajeh

    2016-07-01

    Sono-dispersion of Ni, Co and Ni-Co over Al2O3-MgO with Al/Mg ratio of 1.5 was prepared and tested for dry reforming of methane. The samples were characterized by XRD, FESEM, PSD, EDX, TEM, BET and FTIR analyses. In order to assess the effect of ultrasound irradiation, Ni-Co/Al2O3-MgO with Co content of 8% prepared via sonochemistry and impregnation methods. The sono-synthesized sample showed better textural properties and higher activity than that of impregnated one. Comparison of XRD patterns indicated that the NiO peaks became broader by increasing Co content over the support. The FESEM images displayed the particles are small and well-dispersed as a result of sonochemistry method. Also, EDX analysis demonstrated better dispersion of Ni and Co as a result of sonochemistry method in confirmation of XRD analysis. The sono-synthesized Ni-Co/Al2O3-MgO as a superior nanocatalyst with Co content of 3% illustrates much higher conversions (97.5% and 99% for CH4 and CO2 at 850 °C), yields (94% and 96% for H2 and CO at 850 °C) and 0.97 of H2/CO molar ratio in all samples using an equimolar feed ratio at 850 °C. During the 1200 min stability test, H2/CO molar ratio remained constant for the superior nanocatalyst. Copyright © 2016 Elsevier B.V. All rights reserved.

  13. Miniaturized Laser Heterodyne Radiometer for Measurements of CO2 in the Atmospheric Column

    Science.gov (United States)

    Wilson, E. L.; Mclinden, M. L.; Miller, J. H.; Allan, G. R.; Lott, L. E.; Melroy, H. R.; Clarke, G. B.

    2013-01-01

    We have developed a low-cost, miniaturized laser heterodyne radiometer for highly sensitive measurements of carbon dioxide (CO2) in the atmospheric column. In this passive design, sunlight that has undergone absorption by CO2 in the atmosphere is collected and mixed with continuous wave laser light that is step-scanned across the absorption feature centered at 1,573.6 nm. The resulting radio frequency beat signal is collected as a function of laser wavelength, from which the total column mole fraction can be de-convolved. We are expanding this technique to include methane (CH4) and carbon monoxide (CO), and with minor modifications, this technique can be expanded to include species such as water vapor (H2O) and nitrous oxide (N2O).

  14. Hydrogel-based sensor for CO2 measurements

    NARCIS (Netherlands)

    Herber, S.; Olthuis, Wouter; Bergveld, Piet; van den Berg, Albert

    2004-01-01

    A hydrogel-based sensor is presented for CO2 measurements. The sensor consists of a pressure sensor and porous silicon cover. A pH-sensitive hydrogel is confined between the two parts. Furthermore the porous cover contains a bicarbonate solution and a gaspermeable membrane. CO2 reacts with the

  15. Gain measurements in CO2 CW low pressure lasers

    International Nuclear Information System (INIS)

    Rodrigues, N.A.S.; Chanes Junior, J.B.; Jayaram, K.

    1983-01-01

    A series of gain measurements in low pressure CO 2 CW laser were performed in order to study the behaviour of a CO 2 laser ampliflier as a function of pressure and discharge current. A theoretical model, based on rate equations is also presented to describe the laser behaviour and the experimental procedure adopted. (C.L.B.) [pt

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

    Science.gov (United States)

    McEwing, Katherine Rose; Fisher, James Paul; Zona, Donatella

    Despite multiple studies investigating the environmental controls on CH 4 fluxes from arctic tundra ecosystems, the high spatial variability of CH 4 emissions is not fully understood. This makes the upscaling of CH 4 fluxes from plot to regional scale, particularly challenging. The goal of this study is to refine our knowledge of the spatial variability and controls on CH 4 emission from tundra ecosystems. CH 4 fluxes were measured in four sites across a variety of wet-sedge and tussock tundra ecosystems in Alaska using chambers and a Los Gatos CO 2 and CH 4 gas analyser. All sites were found to be sources of CH 4 , with northern sites (in Barrow) showing similar CH 4 emission rates to the southernmost site (ca. 300 km south, Ivotuk). Gross primary productivity (GPP), water level and soil temperature were the most important environmental controls on CH 4 emission. Greater vascular plant cover was linked with higher CH 4 emission, but this increased emission with increased vascular plant cover was much higher (86 %) in the drier sites, than the wettest sites (30 %), suggesting that transport and/or substrate availability were crucial limiting factors for CH 4 emission in these tundra ecosystems. Overall, this study provides an increased understanding of the fine scale spatial controls on CH 4 flux, in particular the key role that plant cover and GPP play in enhancing CH 4 emissions from tundra soils.

  17. Experimental Ion Mobility measurements in Ne-CO$_2$ and CO$_2$-N$_2$ mixtures

    CERN Document Server

    Encarnação, P.M.C.C.; Veenhof, R.; Neves, P.N.B.; Santos, F.P.; Trindade, A.M.F.; Borges, F.I.G.M.; Conde, C.A.N.

    2016-01-01

    In this paper we present the experimental results for the mobility, K0, of ions in neon-carbon dioxide (Ne-CO2) and carbon dioxide-nitrogen (CO2-N2) gaseous mixtures for total pressures ranging from 8–12 Torr, reduced electric fields in the 10–25 Td range, at room temperature. Regarding the Ne-CO2 mixture only one peak was observed for CO2 concentrations above 25%, which has been identified as an ion originated in CO2, while below 25% of CO2 a second-small peak appears at the left side of the main peak, which has been attributed to impurities. The mobility values for the main peak range between 3.51 ± 0.05 and 1.07 ± 0.01 cm2V−1s−1 in the 10%-99% interval of CO2, and from 4.61 ± 0.19 to 3.00 ± 0.09 cm2V−1s−1 for the second peak observed (10%–25% of CO2). For the CO2-N2, the time-of-arrival spectra displayed only one peak for CO2 concentrations above 10%, which was attributed to ions originated in CO2, namely CO2+(CO2), with a second peak appearing for CO2 concentrations below 10%. This secon...

  18. Detection of CO2 leaks from carbon capture and storage sites with combined atmospheric CO2 and O-2 measurements

    NARCIS (Netherlands)

    van Leeuwen, Charlotte; Meijer, Harro A. J.

    2015-01-01

    This paper presents a transportable instrument that simultaneously measures the CO2 and (relative) O-2 concentration of the atmosphere with the purpose to aid in the detection of CO2 leaks from CCS sites. CO2 and O-2 are coupled in most processes on earth (e.g., photosynthesis, respiration and

  19. Direct measurements of methoxy removal rate constants for collisions with CH4, Ar, N2, Xe, and CF4 in the temperature range 673--973K

    International Nuclear Information System (INIS)

    Wantuck, P.J.; Oldenborg, R.C.; Baugchum, S.L.; Winn, K.R.

    1988-01-01

    Removal rate constants for CH 3 O by CH 4 , Ar, N 2 , Xe, and CF 4 were measured over a 400K temperature range using a laser photolysis/laser-induced fluorescence technique. Rapid methoxy removal rates are observed for the non-reactive collision partners (Ar, N 2 , Xe, and CF 4 ) at elevated temperatures showing that the dissociation and isomerization channels for CH 3 O are indeed important. The total removal rate constant (reaction /plus/ dissociation and/or isomerization) for CH 4 exhibits a linear dependence on temperature and has a removal rate constant, k/sub r/ /equals/ (1.2 +- 0.6) /times/ 10/sup /minus/8/exp[(/minus/101070 +- 350)/T]cm 3 molecule/sup /minus/1/s/sup /minus/1/. Assuming that the removal rate constant due to dissociation and/or isomerization are similar for CH 4 and CF 4 , the reaction rate constant for CH 3 O /plus/ CH 4 is equal to (1.7 +- 1.0) /times/ 10/sup /minus/10/exp[(/minus/7480 +- 1100)/T]cm 3 molecule/sup /minus/1/s/sup /minus/1/. 7 refs., 4 figs

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

    Science.gov (United States)

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

    2010-05-01

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

  1. Ventilation in Sewers Quantified by Measurements of CO2

    DEFF Research Database (Denmark)

    Fuglsang, Emil Dietz; Vollertsen, Jes; Nielsen, Asbjørn Haaning

    2012-01-01

    Understanding and quantifying ventilation in sewer systems is a prerequisite to predict transport of odorous and corrosive gasses within the system as well as their interaction with the urban atmosphere. This paper studies ventilation in sewer systems quantified by measurements of the natural...... occurring compound CO2. Most often Danish wastewater is supersaturated with CO2 and hence a potential for stripping is present. A novel model was built based on the kinetics behind the stripping process. It was applied to simulate ventilation rates from field measurements of wastewater temperature, p...

  2. Experimental ion mobility measurements in Xe-CO2

    Science.gov (United States)

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

    2017-06-01

    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-CO2 mixtures are presented. The results for this mixture show the presence of only one peak for all gas ratios of Xe-CO2, low reduced electric fields, E/N, 10-25 Td (2.4-6.1 kV·cm-1·bar-1), low pressures 6-8 Torr (8-10.6 mbar), at room temperature.

  3. CO2 DIAL system: construction, measurements, and future development

    Science.gov (United States)

    Vicenik, Jiri

    1999-07-01

    A miniature CO2 DIAL system has been constructed. Dimension of the system are 500 X 450 X 240 mm, its mass is only 28 kg. The system consists of two tunable TEA CO2 lasers, receiving optics, IR detector, signal processing electronics and single chip microcomputer with display. The lasers are tuned manually by means of micrometric screw and are capable to generate pulses on more than 50 CO2 laser lines. The output energy is 50 mJ. The system was tested using various toxic gases and simulants, mostly at range 300 m, most of the measurements were done using pyrodetector in the receiver. The system shows good sensitivity, but it exhibits substantial instability of zero concentration. In the next stage the work will be concentrated on use of high-sensitivity MCT detector in the receiver and implementation of automatic tuning of lasers to the system.

  4. Field measurements and modeling to resolve m2 to km2 CH4 emissions for a complex urban source: An Indiana landfill study

    Directory of Open Access Journals (Sweden)

    Maria Obiminda L. Cambaliza

    2017-07-01

    Full Text Available Large spatial and temporal uncertainties for landfill CH4 emissions remain unresolved by short-term field campaigns and historic greenhouse gas (GHG inventory models. Using four field methods (aircraft-based mass balance, tracer correlation, vertical radial plume mapping, static chambers and a new field-validated process-based model (California Landfill Methane Inventory Model, CALMIM 5.4, we investigated the total CH4 emissions from a central Indiana landfill as well as the partitioned emissions inclusive of methanotrophic oxidation for the various cover soils at the site. We observed close agreement between whole site emissions derived from the tracer correlation (8 to 13 mol s–1 and the aircraft mass balance approaches (7 and 17 mol s–1 that were statistically indistinguishable from the modeling result (12 ± 2 mol s–1 inclusive of oxidation. Our model calculations indicated that approximately 90% of the annual average CH4 emissions (11 ± 1 mol s–1; 2200 ± 250 g m–2 d–1 derived from the small daily operational area. Characterized by a thin overnight soil cover directly overlying a thick sequence of older methanogenic waste without biogas recovery, this area constitutes only 2% of the 0.7 km2 total waste footprint area. Because this Indiana landfill is an upwind source for Indianapolis, USA, the resolution of m2 to km2 scale emissions at various temporal scales contributes to improved regional inventories relevant for addressing GHG mitigation strategies. Finally, our comparison of measured to reported CH4 emissions under the US EPA National GHG Reporting program suggests the need to revisit the current IPCC (2006 GHG inventory methodology based on CH4 generation modeling. The reasonable prediction of emissions at individual U.S. landfills requires incorporation of both cover-specific landfill climate modeling (e.g., soil temperature/moisture variability over a typical annual cycle driving CH4 transport and oxidation rates as

  5. 2-Micron Laser Transmitter for Coherent CO2 DIAL Measurement

    Science.gov (United States)

    Singh, Upendra N.; Bai, Yingxin; Yu, Jirong

    2009-01-01

    Carbon dioxide (CO2) has been recognized as one of the most important greenhouse gases. It is essential for the study of global warming to accurately measure the CO2 concentration in the atmosphere and continuously record its variation. A high repetition rate, highly efficient, Q-switched 2-micron laser system as the transmitter of a coherent differential absorption lidar for CO2 measurement has been developed in NASA Langley Research Center. This laser system is capable of making a vertical profiling of CO2 from ground and column measurement of CO2 from air and space-borne platform. The transmitter is a master-slave laser system. The master laser operates in a single frequency, either on-line or off-line of a selected CO2 absorption line. The slave laser is a Q-switched ring-cavity Ho:YLF laser which is pumped by a Tm:fiber laser. The repetition rate can be adjusted from a few hundred Hz to 10 kHz. The injection seeding success rate is from 99.4% to 99.95%. For 1 kHz operation, the output pulse energy is 5.5mJ with the pulse length of 50 ns. The optical-to-optical efficiency is 39% when the pump power is 14.5W. A Ho:YLF laser operating in the range of 2.05 micrometers can be tuned over several characteristic lines of CO2 absorption. Experimentally, a diode pumped Ho:Tm:YLF laser has been successfully used as the transmitter of coherent differential absorption lidar for the measurement of CO2 with a repetition rate of 5 Hz and pulse energy of 75 mJ. For coherent detection, high repetition rate is required for speckle averaging to obtain highly precise measurements. However, a diode pumped Ho:Tm:YLF laser can not operate in high repetition rate due to the large heat loading and up-conversion. A Tm:fiber laser pumped Ho:YLF laser with low heat loading can operate in high repetition rate. A theoretical model has been established to simulate the performance of Tm:fiber laser pumped Ho:YLF lasers. For continuous wave (CW) operation, high pump intensity with small beam

  6. Effect of the Amide Bond Diamine Structure on the CO 2 , H 2 S, and CH 4 Transport Properties of a Series of Novel 6FDA-Based Polyamide–Imides for Natural Gas Purification

    KAUST Repository

    Vaughn, J.; Koros, W. J.

    2012-01-01

    S sorption was enhanced relative to membranes containing fluorinated 6FpDA. Consequently, DAM- and TmPDA-based membranes showed increased stability toward high pressure CO 2 but lower plasticization resistance toward pure H 2S. These results

  7. Estimates of CO2 traffic emissions from mobile concentration measurements

    Science.gov (United States)

    Maness, H. L.; Thurlow, M. E.; McDonald, B. C.; Harley, R. A.

    2015-03-01

    We present data from a new mobile system intended to aid in the design of upcoming urban CO2-monitoring networks. Our collected data include GPS probe data, video-derived traffic density, and accurate CO2 concentration measurements. The method described here is economical, scalable, and self-contained, allowing for potential future deployment in locations without existing traffic infrastructure or vehicle fleet information. Using a test data set collected on California Highway 24 over a 2 week period, we observe that on-road CO2 concentrations are elevated by a factor of 2 in congestion compared to free-flow conditions. This result is found to be consistent with a model including vehicle-induced turbulence and standard engine physics. In contrast to surface concentrations, surface emissions are found to be relatively insensitive to congestion. We next use our model for CO2 concentration together with our data to independently derive vehicle emission rate parameters. Parameters scaling the leading four emission rate terms are found to be within 25% of those expected for a typical passenger car fleet, enabling us to derive instantaneous emission rates directly from our data that compare generally favorably to predictive models presented in the literature. The present results highlight the importance of high spatial and temporal resolution traffic data for interpreting on- and near-road concentration measurements. Future work will focus on transport and the integration of mobile platforms into existing stationary network designs.

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

    Science.gov (United States)

    Lenhart, Katharina; Keppler, Frank

    2017-04-01

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

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

    International Nuclear Information System (INIS)

    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

  10. Measurement of N2O and CH4 soil fluxes from garden, agricultural and natural soils using both closed and open chamber systems coupled with high-precision CRDS analyzer

    Science.gov (United States)

    He, Yonggang; Jacobson, Gloria; Alexander, Chris; Fleck, Derek; Hoffnagel, John; Del Campo, Bernardo; Rella, Chris

    2013-04-01

    Studying the emission and uptake of greenhouse gases from soil is essential for understanding, adapting to and ultimately mitigating the effects of climate change. To-date, majority of such studies have been focused on carbon dioxide (CO2 ) , however, in 2006 the EPA estimated that "Agricultural activities currently generate the largest share, 63 percent, of the world's anthropogenic non-carbon dioxide (non-CO2) emissions (84 percent of nitrous oxide [N2O] and 52 percent of methane[CH4]), and make up roughly 15 percent of all anthropogenic greenhouse gas emissions" (Prentice et al., 2001). Therefore, enabling accurate N2O and CH4 flux measurements in the field are clearly critical to our ability to better constrain carbon and nitrogen budgets, characterize soil sensitivities, agricultural practices, and microbial processes like denitrification and nitrification. To aide in these studies, Picarro has developed a new analyzer based on its proven, NIR technology platform, which is capable of measuring both N2O and CH4 down to ppb levels in a single, field-deployable analyzer. This analyzer measures N2O with a 1-sigma, precision of 3.5 ppb and CH4 with a 1-sigma precision of 3ppb on a 5 minute average. The instrument also has extremely low drift to enable accurate measurements with infrequent calibrations. The data rate of the analyzer is on the order of 5 seconds in order to capture fast, episodic emission events. One of the keys to making accurate CRDS measurements is to thoroughly characterize and correct for spectral interfering species. This is especially important for closed system soil chambers used on agricultural soils where a variety of soil amendments may be applied and gases not usually present in ambient air could concentrate to high levels. In this work, we present the results of analyzer interference testing and corrections completed for the interference of carbon dioxide, methane, ammonia, ethane, ethylene, acetylene, and water on N2O. In addition, we

  11. Progress Toward Measuring CO2 Isotopologue Fluxes in situ with the LLNL Miniature, Laser-based CO2 Sensor

    Science.gov (United States)

    Osuna, J. L.; Bora, M.; Bond, T.

    2015-12-01

    One method to constrain photosynthesis and respiration independently at the ecosystem scale is to measure the fluxes of CO2­ isotopologues. Instrumentation is currently available to makes these measurements but they are generally costly, large, bench-top instruments. Here, we present progress toward developing a laser-based sensor that can be deployed directly to a canopy to passively measure CO2 isotopologue fluxes. In this study, we perform initial proof-of-concept and sensor characterization tests in the laboratory and in the field to demonstrate performance of the Lawrence Livermore National Laboratory (LLNL) tunable diode laser flux sensor. The results shown herein demonstrate measurement of bulk CO2 as a first step toward achieving flux measurements of CO2 isotopologues. The sensor uses a Vertical Cavity Surface Emitting Laser (VCSEL) in the 2012 nm range. The laser is mounted in a multi-pass White Cell. In order to amplify the absorption signal of CO2 in this range we employ wave modulation spectroscopy, introducing an alternating current (AC) bias component where f is the frequency of modulation on the laser drive current in addition to the direct current (DC) emission scanning component. We observed a strong linear relationship (r2 = 0.998 and r2 = 0.978 at all and low CO2 concentrations, respectively) between the 2f signal and the CO2 concentration in the cell across the range of CO2 concentrations relevant for flux measurements. We use this calibration to interpret CO2 concentration of a gas flowing through the White cell in the laboratory and deployed over a grassy field. We will discuss sensor performance in the lab and in situ as well as address steps toward achieving canopy-deployed, passive measurements of CO2 isotopologue fluxes. This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344. LLNL-ABS-675788

  12. An automated setup to measure paleoatmospheric δ13C-CH4, δ15N-N2O and δ18O-N2O in one ice core sample

    NARCIS (Netherlands)

    Sperlich, P.; Buizert, C.; Jenk, T.M.; Sapart, C.J.; Prokopiou, M.; Röckmann, T.; Blunier, T.

    2013-01-01

    Air bubbles in ice core samples represent the only opportunity to study the isotopic variability of paleoatmospheric CH4 and N2O. The highest possible precision in isotope measurements is required to maximize the resolving power for CH4 and N2O sink and source reconstructions. We present a new setup

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

    Directory of Open Access Journals (Sweden)

    H. Schaefer

    2012-09-01

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

  14. Tropospheric radiative forcing of CH4

    International Nuclear Information System (INIS)

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

    1994-04-01

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

  15. Assembly of [Cu2(COO)4] and [M3(μ3-O)(COO)6] (M = Sc, Fe, Ga, and In) building blocks into porous frameworks towards ultra-high C2H2/CO2 and C2H2/CH4 separation performance.

    Science.gov (United States)

    Zhang, Jian-Wei; Hu, Man-Cheng; Li, Shu-Ni; Jiang, Yu-Cheng; Qu, Peng; Zhai, Quan-Guo

    2018-02-20

    A porous MOF platform (SNNU-65s) formed by creatively combining paddle-wheel-like [Cu 2 (COO) 4 ] and trigonal prismatic [M 3 (μ 3 -O)(COO) 6 ] building blocks was designed herein. The mixed and high-density open metal sites and the OH-functionalized pore surface promote SNNU-65s to exhibit ultra-high C 2 H 2 uptake and separation performance. Impressively, SNNU-65-Cu-Ga stands out for the highest C 2 H 2 /CO 2 (18.7) and C 2 H 2 /CH 4 (120.6) selectivity among all the reported MOFs at room temperature.

  16. Evidence for long-lived polar vortex air in the mid-latitude summer stratosphere from in situ laser diode CH4 and H2O measurements

    Directory of Open Access Journals (Sweden)

    G. Durry

    2005-01-01

    Full Text Available A balloon borne diode laser spectrometer was launched in southern France in June 2000 to yield in situ stratospheric CH4 and H2O measurements. In the altitude region ranging from 20km to 25km, striking large spatial structures were observed in the vertical concentration profiles of both species. We suggest these patterns are due to the presence of long-lived remnants of the wintertime polar vortex in the mid-latitude summer stratosphere. To support this interpretation, a high resolution advection model for potential vorticity is used to investigate the evolution of the Arctic vortex after its breakdown phase in spring 2000.

  17. Preparation and Characterization of Facilitated Transport Membranes Composed of Chitosan-Styrene and Chitosan-Acrylonitrile Copolymers Modified by Methylimidazolium Based Ionic Liquids for CO2 Separation from CH4 and N2

    Directory of Open Access Journals (Sweden)

    Ksenia V. Otvagina

    2016-06-01

    Full Text Available CO2 separation was found to be facilitated by transport membranes based on novel chitosan (CS–poly(styrene (PS and chitosan (CS–poly(acrylonitrile (PAN copolymer matrices doped with methylimidazolium based ionic liquids: [bmim][BF4], [bmim][PF6], and [bmim][Tf2N] (IL. CS plays the role of biodegradable film former and selectivity promoter. Copolymers were prepared implementing the latest achievements in radical copolymerization with chosen monomers, which enabled the achievement of outstanding mechanical strength values for the CS-based membranes (75–104 MPa for CS-PAN and 69–75 MPa for CS-PS. Ionic liquid (IL doping affected the surface and mechanical properties of the membranes as well as the gas separation properties. The highest CO2 permeability 400 Barrers belongs to CS-b-PS/[bmim][BF4]. The highest selectivity α (CO2/N2 = 15.5 was achieved for CS-b-PAN/[bmim][BF4]. The operational temperature of the membranes is under 220 °C.

  18. Effect of Ni/Al2O3-SiO2 and Ni/Al2O3-SiO2 with K2O Promoter Catalysts on H2, CO and CH4 Concentration by CO2 Gasification of Rosa Multiflora Biomass

    Directory of Open Access Journals (Sweden)

    Tursunov Obid

    2017-11-01

    Full Text Available The thermal behaviour of the Rosa mutiflora biomass by thermogravimetric analysis was studied at heating rate 3 K min−1 from ambient temperature to 950 °C. TGA tests were performed in high purity carbon dioxide (99 998% with a flow rate 200 ml/min and 100 mg of sample, milled and sieved to a particle size below 250 µm. Moreover, yields of gasification products such as hydrogen (H2, carbon monoxide (CO and methane (CH4 were determined based on the thermovolumetric measurements of catalytic (Ni/Al2O3-SiO2 and Ni/Al2O3-SiO2 with K2O promoter catalysts and non-catalytic gasification of the Rosa multiflora biomass. Additionally, carbon conversion degrees are presented. Calculations were made of the kinetic parameters of carbon monoxide and hydrogen formation reaction in the catalytic and non-catalytic CO2 gasification processes. A high temperature of 950 °C along with Ni/Al2O3-SiO2and Ni/Al2O3-SiO2 with K2O promoter catalysts resulted in a higher conversion of Rosa multiflora biomass into gaseous yield production with greatly increasing of H2 and CO contents. Consequently, H2 and CO are the key factors to produce renewable energy and bio-gases (synthesis gas. The parameters obtained during the experimental examinations enable a tentative assessment of plant biomasses for the process of large-scale gasification in industrial sectors.

  19. Geoelectric Monitoring of geological CO2 storage at Ketzin, Germany (CO2SINK project): Downhole and Surface-Downhole measurements

    Science.gov (United States)

    Kiessling, D.; Schuett, H.; Schoebel, B.; Krueger, K.; Schmidt-Hattenberger, C.; Schilling, F.

    2009-04-01

    Numerical models of the CO2 storage experiment CO2SINK (CO2 Storage by Injection into a Natural Saline Aquifer at Ketzin), where CO2 is injected into a deep saline aquifer at roughly 650 m depth, yield a CO2 saturation of approximately 50% for large parts of the plume. Archie's equation predicts an increase of the resistivity by a factor of approximately 3 to 4 for the reservoir sandstone, and laboratory tests on Ketzin reservoir samples support this prediction. Modeling results show that tracking the CO2 plume may be doable with crosshole resistivity surveys under these conditions. One injection well and two observation wells were drilled in 2007 to a depth of about 800 m and were completed with "smart" casings, arranged L-shaped with distances of 50 m and 100 m. 45 permanent ring-shaped steel electrodes were attached to the electrically insulated casings of the three Ketzin wells at 590 m to 735 m depth with a spacing of about 10 m. It is to our knowledge the deepest permanent vertical electrical resistivity array (VERA) worldwide. The electrodes are connected to the current power supply and data registration units at the surface through custom-made cables. This deep electrode array allows for the registration of electrical resistivity tomography (ERT) data sets at basically any desired repetition rate and at very low cost, without interrupting the injection operations. The installation of all 45 electrodes succeeded. The electrodes are connected to the electrical cable, and the insulated casing stood undamaged. Even after 2-odd years under underground conditions only 6 electrodes are in a critical state now, caused by corrosion effects. In the framework of the COSMOS project (CO2-Storage, Monitoring and Safety Technology), supported by the German "Geotechnologien" program, the geoelectric monitoring has been performed. The 3D crosshole time-laps measurements are taken using dipole-dipole configurations. The data was inverted using AGI EarthImager 3D to obtain 3D

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

    Science.gov (United States)

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

    2016-12-01

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

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

    Science.gov (United States)

    Grossi, Claudia; Vogel, Felix R.; Curcoll, Roger; Àgueda, Alba; Vargas, Arturo; Rodó, Xavier; Morguí, Josep-Anton

    2018-04-01

    The ClimaDat station at Gredos (GIC3) has been continuously measuring atmospheric (dry air) mixing ratios of carbon dioxide (CO2) and methane (CH4), as well as meteorological parameters, since November 2012. In this study we investigate the atmospheric variability of CH4 mixing ratios between 2013 and 2015 at GIC3 with the help of co-located observations of 222Rn concentrations, modelled 222Rn fluxes and modelled planetary boundary layer heights (PBLHs). Both daily and seasonal changes in atmospheric CH4 can be better understood with the help of atmospheric concentrations of 222Rn (and the corresponding fluxes). On a daily timescale, the variation in the PBLH is the main driver for 222Rn and CH4 variability while, on monthly timescales, their atmospheric variability seems to depend on emission changes. To understand (changing) CH4 emissions, nocturnal fluxes of CH4 were estimated using two methods: the radon tracer method (RTM) and a method based on the EDGARv4.2 bottom-up emission inventory, both using FLEXPARTv9.0.2 footprints. The mean value of RTM-based methane fluxes (FR_CH4) is 0.11 mg CH4 m-2 h-1 with a standard deviation of 0.09 or 0.29 mg CH4 m-2 h-1 with a standard deviation of 0.23 mg CH4 m-2 h-1 when using a rescaled 222Rn map (FR_CH4_rescale). For our observational period, the mean value of methane fluxes based on the bottom-up inventory (FE_CH4) is 0.33 mg CH4 m-2 h-1 with a standard deviation of 0.08 mg CH4 m-2 h-1. Monthly CH4 fluxes based on RTM (both FR_CH4 and FR_CH4_rescale) show a seasonality which is not observed for monthly FE_CH4 fluxes. During January-May, RTM-based CH4 fluxes present mean values 25 % lower than during June-December. This seasonal increase in methane fluxes calculated by RTM for the GIC3 area appears to coincide with the arrival of transhumant livestock at GIC3 in the second half of the year.

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

    NARCIS (Netherlands)

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

    2013-01-01

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

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

    Directory of Open Access Journals (Sweden)

    S. Sobek

    2011-09-01

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

  4. Retrieval of average CO2 fluxes by combining in situ CO2 measurements and backscatter lidar information

    Science.gov (United States)

    Gibert, Fabien; Schmidt, Martina; Cuesta, Juan; Ciais, Philippe; Ramonet, Michel; Xueref, IrèNe; Larmanou, Eric; Flamant, Pierre Henri

    2007-05-01

    The present paper deals with a boundary layer budgeting method which makes use of observations from various in situ and remote sensing instruments to infer regional average net ecosystem exchange (NEE) of CO2. Measurements of CO2 within and above the atmospheric boundary layer (ABL) by in situ sensors, in conjunction with a precise knowledge of the change in ABL height by lidar and radiosoundings, enable to infer diurnal and seasonal NEE variations. Near-ground in situ CO measurements are used to discriminate natural and anthropogenic contributions of CO2 diurnal variations in the ABL. The method yields mean NEE that amounts to 5 μmol m-2 s-1 during the night and -20 μmol m-2 s-1 in the middle of the day between May and July. A good agreement is found with the expected NEE accounting for a mixed wheat field and forest area during winter season, representative of the mesoscale ecosystems in the Paris area according to the trajectory of an air column crossing the landscape. Daytime NEE is seen to follow the vegetation growth and the change in the ratio diffuse/direct radiation. The CO2 vertical mixing flux during the rise of the atmospheric boundary layer is also estimated and seems to be the main cause of the large decrease of CO2 mixing ratio in the morning. The outcomes on CO2 flux estimate are compared to eddy-covariance measurements on a barley field. The importance of various sources of error and uncertainty on the retrieval is discussed. These errors are estimated to be less than 15%; the main error resulted from anthropogenic emissions.

  5. Calibration of column-averaged CH4 over European TCCON FTS sites with airborne in-situ measurements

    NARCIS (Netherlands)

    Geibel, M. C.; Messerschmidt, J.; Gerbig, C.; Blumenstock, T.; Chen, H.; Hase, F.; Kolle, O.; Lavric, J. V.; Notholt, J.; Palm, M.; Rettinger, M.; Schmidt, Martina; Sussmann, R.; Warneke, T.; Feist, D. G.

    2012-01-01

    In September/October 2009, six European ground-based Fourier Transform Spectrometers (FTS) of the Total Carbon Column Observation Network (TCCON) were calibrated for the first time using aircraft measurements. The campaign was part of the Infrastructure for Measurement of the European Carbon Cycle

  6. Evaluating Humidity and Sea Salt Disturbances on CO2 Flux Measurements

    DEFF Research Database (Denmark)

    Nilsson, Erik; Bergström, Hans; Rutgersson, Anna

    2018-01-01

    Global oceans are an important sink of atmospheric carbon dioxide (CO2). Therefore, understanding the air–sea flux of CO2 is a vital part in describing the global carbon balance. Eddy covariance (EC) measurements are often used to study CO2 fluxes from both land and ocean. Values of CO2 are usual...

  7. Multi-Scale Approach for Measuring N2O and CH4 Emissions in Drainage Water Managed Corn-Soybean System

    Science.gov (United States)

    Hagedorn, J.; Zhu, Q.; Davidson, E. A.; Castro, M.

    2017-12-01

    Managing resources wisely while reducing environmental impact is the backbone of agricultural sustainability. Agricultural practices must develop strategies to effectively reduce nutrient runoff from farmed lands. Preliminary research suggests that one such strategy is drainage water management by which water levels are intentionally elevated following fertilization to favor subsoil denitrification and thereby reduce nitrogen leaching into groundwater and streams. Despite documented success in nitrate reduction, this best management practice (BMP) has not been widely adopted in part because users are not aware of the potential. But before extension agencies begin promoting this practice, evaluation of unintentional consequences must be studied. There is a risk that by elevating water levels for the purpose of creating suitable conditions for denitrification, more potent greenhouse gases such as nitrous oxide (N2O) and methane (CH4) could be produced, in which case the practice would be swapping one form of pollution for another. A multi-scale experimental design, using soil chambers and a tower-based gradient method, was implemented in a drainage water managed corn-soybean system on the Eastern Shore of Maryland. Emissions, soil moisture content, and soil nitrate measurements have been collected and analyzed to evaluate for differences between treatment and control plots as standard farm management practices, such as fertilization, occur. Preliminary results based on monthly sampling of transects of stationary soil chambers characterize the spatial heterogeneity of the fields and reveal that there are detectable differences in N2O and CH4 emissions between fields. There are also significant relationships between soil moisture, soil nitrate content and N2O emissions. The tower-based gradient method with micrometerological measurements provides high temporal resolution at the full field scale that complements the soil chamber work. This multi-scale resolution balance

  8. On the optimisation of trace gas measurements : A new method for in situ measurements of CO2, CH4, CO, SF6 and N2O

    NARCIS (Netherlands)

    Laan van der, Sander

    2005-01-01

    The release of anthropogenic greenhouse gases into the earth’s atmosphere is by far the largest uncontrolled experiment in the history of the earth. Mankind is drastically modifying the composition of the atmosphere, both in greenhouse gases and aerosols

  9. Combining tracer flux ratio methodology with low-flying aircraft measurements to estimate dairy farm CH4 emissions

    Science.gov (United States)

    Daube, C.; Conley, S.; Faloona, I. C.; Yacovitch, T. I.; Roscioli, J. R.; Morris, M.; Curry, J.; Arndt, C.; Herndon, S. C.

    2017-12-01

    Livestock activity, enteric fermentation of feed and anaerobic digestion of waste, contributes significantly to the methane budget of the United States (EPA, 2016). Studies question the reported magnitude of these methane sources (Miller et. al., 2013), calling for more detailed research of agricultural animals (Hristov, 2014). Tracer flux ratio is an attractive experimental method to bring to this problem because it does not rely on estimates of atmospheric dispersion. Collection of data occurred during one week at two dairy farms in central California (June, 2016). Each farm varied in size, layout, head count, and general operation. The tracer flux ratio method involves releasing ethane on-site with a known flow rate to serve as a tracer gas. Downwind mixed enhancements in ethane (from the tracer) and methane (from the dairy) were measured, and their ratio used to infer the unknown methane emission rate from the farm. An instrumented van drove transects downwind of each farm on public roads while tracer gases were released on-site, employing the tracer flux ratio methodology to assess simultaneous methane and tracer gas plumes. Flying circles around each farm, a small instrumented aircraft made measurements to perform a mass balance evaluation of methane gas. In the course of these two different methane quantification techniques, we were able to validate yet a third method: tracer flux ratio measured via aircraft. Ground-based tracer release rates were applied to the aircraft-observed methane-to-ethane ratios, yielding whole-site methane emission rates. Never before has the tracer flux ratio method been executed with aircraft measurements. Estimates from this new application closely resemble results from the standard ground-based technique to within their respective uncertainties. Incorporating this new dimension to the tracer flux ratio methodology provides additional context for local plume dynamics and validation of both ground and flight-based data.

  10. Implications of overestimated anthropogenic CO2 emissions on East Asian and global land CO2 flux inversion

    Science.gov (United States)

    Saeki, Tazu; Patra, Prabir K.

    2017-12-01

    Measurement and modelling of regional or country-level carbon dioxide (CO2) fluxes are becoming critical for verification of the greenhouse gases emission control. One of the commonly adopted approaches is inverse modelling, where CO2 fluxes (emission: positive flux, sink: negative flux) from the terrestrial ecosystems are estimated by combining atmospheric CO2 measurements with atmospheric transport models. The inverse models assume anthropogenic emissions are known, and thus the uncertainties in the emissions introduce systematic bias in estimation of the terrestrial (residual) fluxes by inverse modelling. Here we show that the CO2 sink increase, estimated by the inverse model, over East Asia (China, Japan, Korea and Mongolia), by about 0.26 PgC year-1 (1 Pg = 1012 g) during 2001-2010, is likely to be an artifact of the anthropogenic CO2 emissions increasing too quickly in China by 1.41 PgC year-1. Independent results from methane (CH4) inversion suggested about 41% lower rate of East Asian CH4 emission increase during 2002-2012. We apply a scaling factor of 0.59, based on CH4 inversion, to the rate of anthropogenic CO2 emission increase since the anthropogenic emissions of both CO2 and CH4 increase linearly in the emission inventory. We find no systematic increase in land CO2 uptake over East Asia during 1993-2010 or 2000-2009 when scaled anthropogenic CO2 emissions are used, and that there is a need of higher emission increase rate for 2010-2012 compared to those calculated by the inventory methods. High bias in anthropogenic CO2 emissions leads to stronger land sinks in global land-ocean flux partitioning in our inverse model. The corrected anthropogenic CO2 emissions also produce measurable reductions in the rate of global land CO2 sink increase post-2002, leading to a better agreement with the terrestrial biospheric model simulations that include CO2-fertilization and climate effects.

  11. Quantitative comparison of in situ soil CO2 flux measurement methods

    Science.gov (United States)

    Jennifer D. Knoepp; James M. Vose

    2002-01-01

    Development of reliable regional or global carbon budgets requires accurate measurement of soil CO2 flux. We conducted laboratory and field studies to determine the accuracy and comparability of methods commonly used to measure in situ soil CO2 fluxes. Methods compared included CO2...

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

    Science.gov (United States)

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

    2017-12-01

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

  13. CO2 Capacity Sorbent Analysis Using Volumetric Measurement Approach

    Science.gov (United States)

    Huang, Roger; Richardson, Tra-My Justine; Belancik, Grace; Jan, Darrell; Knox, Jim

    2017-01-01

    In support of air revitalization system sorbent selection for future space missions, Ames Research Center (ARC) has performed CO2 capacity tests on various solid sorbents to complement structural strength tests conducted at Marshall Space Flight Center (MSFC). The materials of interest are: Grace Davison Grade 544 13X, Honeywell UOP APG III, LiLSX VSA-10, BASF 13X, and Grace Davison Grade 522 5A. CO2 capacity was for all sorbent materials using a Micromeritics ASAP 2020 Physisorption Volumetric Analysis machine to produce 0C, 10C, 25C, 50C, and 75C isotherms. These data are to be used for modeling data and to provide a basis for continued sorbent research. The volumetric analysis method proved to be effective in generating consistent and repeatable data for the 13X sorbents, but the method needs to be refined to tailor to different sorbents.

  14. Biases of chamber methods for measuring soil CO2 efflux demonstrated with a laboratory apparatus.

    Science.gov (United States)

    S. Mark Nay; Kim G. Mattson; Bernard T. Bormann

    1994-01-01

    Investigators have historically measured soil CO2 efflux as an indicator of soil microbial and root activity and more recently in calculations of carbon budgets. The most common methods estimate CO2 efflux by placing a chamber over the soil surface and quantifying the amount of CO2 entering the...

  15. Determination of microbial versus root-produced CO2 in an agricultural ecosystem by means of δ13CO2 measurements in soil air

    NARCIS (Netherlands)

    Schüßler, Wolfram; Neubert, Rolf; Levin, Ingeborg; Fischer, Natalie; Sonntag, Christian

    2000-01-01

    The amounts of microbial and root-respired CO2 in a maize/winter wheat agricultural system in south western Germany were investigated by measurements of the CO2 mixing ratio and the 13C/12C ratio in soil air. CO2 fluxes at the soil surface for the period of investigation (1993–1995) were also

  16. Quantifying Gas Flaring CH4 Consumption Using VIIRS

    Directory of Open Access Journals (Sweden)

    Xiaodong Zhang

    2015-07-01

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

  17. Comparative methane estimation from cattle based on total CO2 production using different techniques

    Directory of Open Access Journals (Sweden)

    Md N. Haque

    2017-06-01

    Full Text Available The objective of this study was to compare the precision of CH4 estimates using calculated CO2 (HP by the CO2 method (CO2T and measured CO2 in the respiration chamber (CO2R. The CO2R and CO2T study was conducted as a 3 × 3 Latin square design where 3 Dexter heifers were allocated to metabolic cages for 3 periods. Each period consisted of 2 weeks of adaptation followed by 1 week of measurement with the CO2R and CO2T. The average body weight of the heifer was 226 ± 11 kg (means ± SD. They were fed a total mixed ration, twice daily, with 1 of 3 supplements: wheat (W, molasses (M, or molasses mixed with sodium bicarbonate (Mbic. The dry mater intake (DMI; kg/day was significantly greater (P < 0.001 in the metabolic cage compared with that in the respiration chamber. The daily CH4 (L/day emission was strongly correlated (r = 0.78 between CO2T and CO2R. The daily CH4 (L/kg DMI emission by the CO2T was in the same magnitude as by the CO2R. The measured CO2 (L/day production in the respiration chamber was not different (P = 0.39 from the calculated CO2 production using the CO2T. This result concludes a reasonable accuracy and precision of CH4 estimation by the CO2T compared with the CO2R.

  18. Field measurements and modeling to resolve m2 to km2 CH4 emissions for a complex urban source: An Indiana landfill study

    Science.gov (United States)

    Large uncertainties for landfill CH4 emissions due to spatial and temporal variabilities remain unresolved by short-term field campaigns and historic GHG inventory models. Using four field methods (aircraft-based mass balance, tracer correlation, vertical radial plume mapping, and static chambers) ...

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

    Science.gov (United States)

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

    2002-02-01

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

  20. Raman spectroscopic measurements of CO2 density: Experimental calibration with high-pressure optical cell (HPOC) and fused silica capillary capsule (FSCC) with application to fluid inclusion observations

    Science.gov (United States)

    Wang, X.; Chou, I-Ming; Hu, W.; Burruss, Robert; Sun, Q.; Song, Y.

    2011-01-01

    Raman spectroscopy is a powerful method for the determination of CO2 densities in fluid inclusions, especially for those with small size and/or low fluid density. The relationship between CO2 Fermi diad split (Δ, cm−1) and CO2 density (ρ, g/cm3) has been documented by several previous studies. However, significant discrepancies exist among these studies mainly because of inconsistent calibration procedures and lack of measurements for CO2fluids having densities between 0.21 and 0.75 g/cm3, where liquid and vapor phases coexist near room temperature.In this study, a high-pressure optical cell and fused silica capillary capsules were used to prepare pure CO2 samples with densities between 0.0472 and 1.0060 g/cm3. The measured CO2 Fermi diad splits were calibrated with two well established Raman bands of benzonitrile at 1192.6 and 1598.9 cm−1. The relationship between the CO2 Fermi diad split and density can be represented by: ρ = 47513.64243 − 1374.824414 × Δ + 13.25586152 × Δ2 − 0.04258891551 × Δ3(r2 = 0.99835, σ = 0.0253 g/cm3), and this relationship was tested by synthetic fluid inclusions and natural CO2-rich fluid inclusions. The effects of temperature and the presence of H2O and CH4 on this relationship were also examined.

  1. Measurements and modeling of absorption by CO2 + H2O mixtures in the spectral region beyond the CO2 ν3-band head

    Science.gov (United States)

    Tran, H.; Turbet, M.; Chelin, P.; Landsheere, X.

    2018-05-01

    In this work, we measured the absorption by CO2 + H2O mixtures from 2400 to 2600 cm-1 which corresponds to the spectral region beyond the ν3 band head of CO2. Transmission spectra of CO2 mixed with water vapor were recorded with a high-resolution Fourier-transform spectrometer for various pressure, temperature and concentration conditions. The continuum absorption by CO2 due to the presence of water vapor was determined by subtracting from measured spectra the contribution of local lines of both species, that of the continuum of pure CO2 as well as of the self- and CO2-continua of water vapor induced by the H2O-H2O and H2O-CO2 interactions. The obtained results are in very good agreement with the unique previous measurement (in a narrower spectral range). They confirm that the H2O-continuum of CO2 is significantly larger than that observed for pure CO2. This continuum thus must be taken into account in radiative transfer calculations for media involving CO2+ H2O mixture. An empirical model, using sub-Lorentzian line shapes based on some temperature-dependent correction factors χ is proposed which enables an accurate description of the experimental results.

  2. Faults as Windows to Monitor Gas Seepage: Application to CO2 Sequestration and CO2-EOR

    Directory of Open Access Journals (Sweden)

    Ronald W. Klusman

    2018-03-01

    Full Text Available Monitoring of potential gas seepage for CO2 sequestration and CO2-EOR (Enhanced Oil Recovery in geologic storage will involve geophysical and geochemical measurements of parameters at depth and at, or near the surface. The appropriate methods for MVA (Monitoring, Verification, Accounting are needed for both cost and technical effectiveness. This work provides an overview of some of the geochemical methods that have been demonstrated to be effective for an existing CO2-EOR (Rangely, CA, USA and a proposed project at Teapot Dome, WY, USA. Carbon dioxide and CH4 fluxes and shallow soil gas concentrations were measured, followed by nested completions of 10-m deep holes to obtain concentration gradients. The focus at Teapot Dome was the evaluation of faults as pathways for gas seepage in an under-pressured reservoir system. The measurements were supplemented by stable carbon and oxygen isotopic measurements, carbon-14, and limited use of inert gases. The work clearly demonstrates the superiority of CH4 over measurements of CO2 in early detection and quantification of gas seepage. Stable carbon isotopes, carbon-14, and inert gas measurements add to the verification of the deep source. A preliminary accounting at Rangely confirms the importance of CH4 measurements in the MVA application.

  3. Carbon balance of China constrained by CONTRAIL aircraft CO2 measurements

    Science.gov (United States)

    Jiang, F.; Wang, H. M.; Chen, J. M.; Machida, T.; Zhou, L. X.; Ju, W. M.; Matsueda, H.; Sawa, Y.

    2014-09-01

    Terrestrial carbon dioxide (CO2) flux estimates in China using atmospheric inversion method are beset with considerable uncertainties because very few atmospheric CO2 concentration measurements are available. In order to improve these estimates, nested atmospheric CO2 inversion during 2002-2008 is performed in this study using passenger aircraft-based CO2 measurements over Eurasia from the Comprehensive Observation Network for Trace gases by Airliner (CONTRAIL) project. The inversion system includes 43 regions with a focus on China, and is based on the Bayesian synthesis approach and the TM5 transport model. The terrestrial ecosystem carbon flux modeled by the Boreal Ecosystems Productivity Simulator (BEPS) model and the ocean exchange simulated by the OPA-PISCES-T model are considered as the prior fluxes. The impacts of CONTRAIL CO2 data on inverted China terrestrial carbon fluxes are quantified, the improvement of the inverted fluxes after adding CONTRAIL CO2 data are rationed against climate factors and evaluated by comparing the simulated atmospheric CO2 concentrations with three independent surface CO2 measurements in China. Results show that with the addition of CONTRAIL CO2 data, the inverted carbon sink in China increases while those in South and Southeast Asia decrease. Meanwhile, the posterior uncertainties over these regions are all reduced (2-12%). CONTRAIL CO2 data also have a large effect on the inter-annual variation of carbon sinks in China, leading to a better correlation between the carbon sink and the annual mean climate factors. Evaluations against the CO2 measurements at three sites in China also show that the CONTRAIL CO2 measurements may have improved the inversion results.

  4. TG-FTIR measurement of CO2-H2O co-adsorption for CO2 air capture sorbent screening

    NARCIS (Netherlands)

    Smal, I.M.; Yu, Qian; Veneman, Rens; Fränzel-Luiten, B.; Brilman, Derk Willem Frederik

    2014-01-01

    Capturing atmospheric CO2 using solid sorbents is gaining interest. As ambient air normally contains much more (up to 100 times) water than CO2, a selective sorbent is desirable as co-adsorption will most likely occur. In this study, a convenient method based on an TG-FTIR analysis system is

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

    NARCIS (Netherlands)

    Gersen, Sander; Darmeveil, Harry; Levinsky, Howard

    2012-01-01

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

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

    Science.gov (United States)

    Clancy, S.; Worrall, F.; Davies, R. J.; Almond, S.; Boothroyd, I.

    2016-12-01

    these joints. When scaled up to the UK's National Transmission System pipeline length of 7600 km gives a fugitive CH4 flux of 62.6 kt CH4/yr with a CO2 equivalent of 1570 kt CO2eq/yr - this fugitive emission from high pressure pipelines is 0.14% of the annual gas supply.

  7. Interpretation and evaluation of combined measurement techniques for soil CO2 efflux: Discrete surface chambers and continuous soil CO2 concentration probes

    Science.gov (United States)

    Diego A. Riveros-Iregui; Brian L. McGlynn; Howard E. Epstein; Daniel L. Welsch

    2008-01-01

    Soil CO2 efflux is a large respiratory flux from terrestrial ecosystems and a critical component of the global carbon (C) cycle. Lack of process understanding of the spatiotemporal controls on soil CO2 efflux limits our ability to extrapolate from fluxes measured at point scales to scales useful for corroboration with other ecosystem level measures of C exchange....

  8. Wine ethanol C-14 as a tracer for fossil fuel CO2 emissions in Europe : Measurements and model comparison

    NARCIS (Netherlands)

    Palstra, Sanne W. L.; Karstens, Ute; Streurman, Harm-Jan; Meijer, Harro A. J.

    2008-01-01

    C-14 (radiocarbon) in atmospheric CO2 is the most direct tracer for the presence of fossil-fuel-derived CO2 (CO2-ff). We demonstrate the C-14 measurement of wine ethanol as a way to determine the relative regional atmospheric CO2-ff concentration compared to a background site ("regional CO2-ff

  9. Development of Double and Triple-Pulsed 2-micron IPDA Lidars for Column CO2 Measurements

    Science.gov (United States)

    Singh, Upendra N.; Yu, Jirong; Petros, Mulugeta; Refaat, Tamer F.; Remus, Ruben G.; Reithmaier, Karl

    2015-01-01

    Carbon dioxide (CO2) is an important greenhouse gas that significantly contributes to the carbon cycle and globalradiation budget on Earth. CO2 role on Earth’s climate is complicated due to different interactions with various climatecomponents that include the atmosphere, the biosphere and the hydrosphere. Although extensive worldwide efforts formonitoring atmospheric CO2 through various techniques, including in-situ and passive sensors, are taking place highuncertainties exist in quantifying CO2 sources and sinks. These uncertainties are mainly due to insufficient spatial andtemporal mapping of the gas. Therefore it is required to have more rapid and accurate CO2 monitoring with higheruniform coverage and higher resolution. CO2 DIAL operating in the 2-µm band offer better near-surface CO2measurement sensitivity due to the intrinsically stronger absorption lines. For more than 15 years, NASA LangleyResearch Center (LaRC) contributed in developing several 2-?m CO2 DIAL systems and technologies. This paperfocuses on the current development of the airborne double-pulsed and triple-pulsed 2-?m CO2 integrated pathdifferential absorption (IPDA) lidar system at NASA LaRC. This includes the IPDA system development andintegration. Results from ground and airborne CO2 IPDA testing will be presented. The potential of scaling suchtechnology to a space mission will be addressed.

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

    Science.gov (United States)

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

    2016-04-01

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

  11. Measurements of sulfur compounds in CO2 by diode laser atomic absorption spectrometry

    International Nuclear Information System (INIS)

    Franzke, J.; Stancu, D.G.; Niemax, K.

    2003-01-01

    Two simple methods for the analysis of the total concentration of sulfur in CO 2 by diode laser atomic absorption spectrometry of excited, metastable sulfur atoms in a direct current discharge are presented. In the first method, the CO 2 sample gas is mixed with the plasma gas (Ar or He) while the second is based on reproducible measurements of the sulfur released from the walls in a helium discharge after being deposited as a result of operating the discharge in pure CO 2 sample gas. The detection limits obtained satisfy the requirements for the control of sulfur compounds in CO 2 used in the food and beverage industry

  12. Inter annual variability of the global carbo