Identification, Comparison, and Validation of Robust Rumen Microbial Biomarkers for Methane Emissions Using Diverse Bos Taurus Breeds and Basal Diets

PubMed Central

Auffret, Marc D.; Stewart, Robert; Dewhurst, Richard J.; Duthie, Carol-Anne; Rooke, John A.; Wallace, Robert J.; Freeman, Tom C.; Snelling, Timothy J.; Watson, Mick; Roehe, Rainer

2018-01-01

Previous shotgun metagenomic analyses of ruminal digesta identified some microbial information that might be useful as biomarkers to select cattle that emit less methane (CH4), which is a potent greenhouse gas. It is known that methane production (g/kgDMI) and to an extent the microbial community is heritable and therefore biomarkers can offer a method of selecting cattle for low methane emitting phenotypes. In this study a wider range of Bos Taurus cattle, varying in breed and diet, was investigated to determine microbial communities and genetic markers associated with high/low CH4 emissions. Digesta samples were taken from 50 beef cattle, comprising four cattle breeds, receiving two basal diets containing different proportions of concentrate and also including feed additives (nitrate or lipid), that may influence methane emissions. A combination of partial least square analysis and network analysis enabled the identification of the most significant and robust biomarkers of CH4 emissions (VIP > 0.8) across diets and breeds when comparing all potential biomarkers together. Genes associated with the hydrogenotrophic methanogenesis pathway converting carbon dioxide to methane, provided the dominant biomarkers of CH4 emissions and methanogens were the microbial populations most closely correlated with CH4 emissions and identified by metagenomics. Moreover, these genes grouped together as confirmed by network analysis for each independent experiment and when combined. Finally, the genes involved in the methane synthesis pathway explained a higher proportion of variation in CH4 emissions by PLS analysis compared to phylogenetic parameters or functional genes. These results confirmed the reproducibility of the analysis and the advantage to use these genes as robust biomarkers of CH4 emissions. Volatile fatty acid concentrations and ratios were significantly correlated with CH4, but these factors were not identified as robust enough for predictive purposes. Moreover, the methanotrophic Methylomonas genus was found to be negatively correlated with CH4. Finally, this study confirmed the importance of using robust and applicable biomarkers from the microbiome as a proxy of CH4 emissions across diverse production systems and environments. PMID:29375511

Identification, Comparison, and Validation of Robust Rumen Microbial Biomarkers for Methane Emissions Using Diverse Bos Taurus Breeds and Basal Diets.

PubMed

Auffret, Marc D; Stewart, Robert; Dewhurst, Richard J; Duthie, Carol-Anne; Rooke, John A; Wallace, Robert J; Freeman, Tom C; Snelling, Timothy J; Watson, Mick; Roehe, Rainer

2017-01-01

Previous shotgun metagenomic analyses of ruminal digesta identified some microbial information that might be useful as biomarkers to select cattle that emit less methane (CH 4 ), which is a potent greenhouse gas. It is known that methane production (g/kgDMI) and to an extent the microbial community is heritable and therefore biomarkers can offer a method of selecting cattle for low methane emitting phenotypes. In this study a wider range of Bos Taurus cattle, varying in breed and diet, was investigated to determine microbial communities and genetic markers associated with high/low CH 4 emissions. Digesta samples were taken from 50 beef cattle, comprising four cattle breeds, receiving two basal diets containing different proportions of concentrate and also including feed additives (nitrate or lipid), that may influence methane emissions. A combination of partial least square analysis and network analysis enabled the identification of the most significant and robust biomarkers of CH 4 emissions (VIP > 0.8) across diets and breeds when comparing all potential biomarkers together. Genes associated with the hydrogenotrophic methanogenesis pathway converting carbon dioxide to methane, provided the dominant biomarkers of CH 4 emissions and methanogens were the microbial populations most closely correlated with CH 4 emissions and identified by metagenomics. Moreover, these genes grouped together as confirmed by network analysis for each independent experiment and when combined. Finally, the genes involved in the methane synthesis pathway explained a higher proportion of variation in CH 4 emissions by PLS analysis compared to phylogenetic parameters or functional genes. These results confirmed the reproducibility of the analysis and the advantage to use these genes as robust biomarkers of CH 4 emissions. Volatile fatty acid concentrations and ratios were significantly correlated with CH 4 , but these factors were not identified as robust enough for predictive purposes. Moreover, the methanotrophic Methylomonas genus was found to be negatively correlated with CH 4 . Finally, this study confirmed the importance of using robust and applicable biomarkers from the microbiome as a proxy of CH 4 emissions across diverse production systems and environments.

The global methane budget 2000–2012

DOE PAGES

Saunois, Marielle; Bousquet, Philippe; Poulter, Ben; ...

2016-12-12

The global methane (CH 4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH 4 over the past decade. Emissions and concentrations of CH 4 are continuing to increase, making CH 4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH 4 sources that overlap geographically, and from the destruction of CH 4more » by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (~biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations).« less

The global methane budget 2000–2012

DOE Office of Scientific and Technical Information (OSTI.GOV)

Saunois, Marielle; Bousquet, Philippe; Poulter, Ben

The global methane (CH 4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH 4 over the past decade. Emissions and concentrations of CH 4 are continuing to increase, making CH 4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH 4 sources that overlap geographically, and from the destruction of CH 4more » by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (~biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations).« less

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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. Unlike CO2 whose rate of growth in the atmosphere has remained positive and increased in recent decades, the behavior of atmospheric methane is considerably more complex and is much less understood on account of the spatiotemporal variability of its emissions which include biogenic (e.g. wetlands, ruminants, rice agriculture), thermogenic (fossil fuels), and pyrogenic (i.e. biomass burning) sources. After sustained growth during most of the 20th century, the CH4 growth rate declined falling from 15 ppbv/yr during the 1980s to 6 ppbv/yr in the 1990s to near-zero and even negative values in the early 2000s. With some surprise however, the growth rate rebounded in 2007 and has been on average 6 ppbv/yr during the past 10 years. During this same period the 13CH4/12CH4 ratio of atmospheric CH4 also declined suggesting the recent CH4 growth was caused by an increase in 13CH4-depleted biogenic emissions. Here, we provide additional insight into the recent behavior of atmospheric methane by performing a global three-dimensional Bayesian inversion of surface CH4 and 13CH4/12CH4 ratios over the period 1985-2015 using NOAA Global Monitoring Division (GMD) CH4 measurements and the GEOS-Chem chemical-transport model (CTM) at a horizontal grid resolution of 2ox2.5o. The use of the 3-D model allows us to exploit spatial patterns in the global CH4 and 13CH4/12CH4 fields that provide additional constraints on the retrieval of the time-dependent CH4 fluxes. This work follows up on our previous CH4 inversion where we used a 4ox5o horizontal grid for GEOS-Chem to retrieve fluxes from 1985 to 2009. At higher resolution more information is extracted from the observations due to improved model skill and a smaller number of stations aggregated within model grid cells. This increases the weights of the measurements relative to the a priori fluxes in the inversion producing stronger observational constraints on the optimized fluxes. This work assesses the contribution of spatial heterogeneities in the observed CH4 record to the retrieval of global CH4 fluxes and provides a new look into the causes of the recent growth in atmospheric methane.

Increased importance of methane reduction for a 1.5 degree target

NASA Astrophysics Data System (ADS)

Collins, William J.; Webber, Christopher P.; Cox, Peter M.; Huntingford, Chris; Lowe, Jason; Sitch, Stephen; Chadburn, Sarah E.; Comyn-Platt, Edward; Harper, Anna B.; Hayman, Garry; Powell, Tom

2018-04-01

To understand the importance of methane on the levels of carbon emission reductions required to achieve temperature goals, a processed-based approach is necessary rather than reliance on the transient climate response to emissions. We show that plausible levels of methane (CH4) mitigation can make a substantial difference to the feasibility of achieving the Paris climate targets through increasing the allowable carbon emissions. This benefit is enhanced by the indirect effects of CH4 on ozone (O3). Here the differing effects of CH4 and CO2 on land carbon storage, including the effects of surface O3, lead to an additional increase in the allowable carbon emissions with CH4 mitigation. We find a simple robust relationship between the change in the 2100 CH4 concentration and the extra allowable cumulative carbon emissions between now and 2100 (0.27 ± 0.05 GtC per ppb CH4). This relationship is independent of modelled climate sensitivity and precise temperature target, although later mitigation of CH4 reduces its value and thus methane reduction effectiveness. Up to 12% of this increase in allowable emissions is due to the effect of surface ozone. We conclude early mitigation of CH4 emissions would significantly increase the feasibility of stabilising global warming below 1.5 °C, alongside having co-benefits for human and ecosystem health.

40 CFR 98.343 - Calculating GHG emissions.

Code of Federal Regulations, 2010 CFR

2010-07-01

... potential (metric tons CH4/metric ton waste) = MCF × DOC × DOCF × F × 16/12. MCF = Methane correction factor... = Methane emissions from the landfill in the reporting year (metric tons CH4). GCH 4 = Modeled methane...). Emissions = Methane emissions from the landfill in the reporting year (metric tons CH4). R = Quantity of...

Raman and FTIR spectroscopy of methane in olivine

NASA Astrophysics Data System (ADS)

Smith, A.; Oze, C.; Rossman, G. R.; Celestian, A. J.

2017-12-01

Olivine has been proposed to be a direct source of methane (CH4) in serpentinization systems and experiments. Here, Raman and Fourier Transform Infrared (FTIR) spectroscopy were used to verify the presence and abundance of CH4 in olivine samples from nine localities, including the San Carlos olivine. Raman analyses did not identify any methane in the olivine samples. As olivine is orthorhombic, three polarized FTIR spectra were obtained for the olivine samples. No methane was detected in any of the olivine samples using FTIR. Overall, olivine investigated in this study does not appear to be a primary source of methane.

Methane flux from Minnesota Peatlands

NASA Astrophysics Data System (ADS)

Crill, P. M.; Bartlett, K. B.; Harriss, R. C.; Gorham, E.; Verry, E. S.; Sebacher, D. I.; Madzar, L.; Sanner, W.

1988-12-01

Northern (>40°N) wetlands have been suggested as the largest natural source of methane (CH4) to the troposphere. To refine our estimates of source strengths from this region and to investigate climatic controls on the process, fluxes were measured from a variety of Minnesota peatlands during May, June, and August 1986. Sites included forested and unforested ombrotrophic bogs and minerotrophic fens in and near the U.S. Department of Agriculture Marcell Experimental Forest and the Red Lake peatlands. Late spring and summer fluxes ranged from 11 to 866 mg CH4 m-2 d-1, averaging 207 mg CH4 m-2 d-1 overall. At Marcell Forest, forested bogs and fen sites had lower fluxes (averages of 77 ± 21 mg CH4 m-2 d-1 and 142 ± 19 mg CH4 m-2 d-1) than open bogs (average of 294 ± 30 mg CH4 m-2 d-1). In the Red Lake peatland, circumneutral fens, with standing water above the peat surface, produced more methane than acid bog sites in which the water table was beneath the moss surface (325 ± 31 and 102 ± 13 mg CH4 m-2 d-1, respectively). Peat temperature was an important control. Methane flux increased in response to increasing soil temperature. For example, the open bog in the Marcell Forest with the highest CH4 flux exhibited a 74-fold increase in flux over a three-fold increase in temperature. We estimate that the methane flux from all peatlands north of 40° may be on the order of 70 to 90 Tg/yr though estimates of this sort are plagued by uncertainties in the areal extent of peatlands, length of the CH4 producing season, and the spatial and temporal variability of the flux.

Separation of C2 hydrocarbons from methane in a microporous metal-organic framework

NASA Astrophysics Data System (ADS)

Tang, Fu-Shun; Lin, Rui-Biao; Lin, Rong-Guang; Zhao, John Cong-Gui; Chen, Banglin

2018-02-01

The recovery of C2 hydrocarbons including acetylene, ethylene and ethane is challenging but important for natural gas upgrading. The separation of C2 hydrocarbons over methane was demonstrated here by using a microporous metal-organic framework [Zn3(OH)2(SDB)2] (H2SDB = 4,4'-sulfonyldibenzoic acid) consisting narrow one-dimensional pore channels. Gas sorption experiments revealed that this MOF material showed considerable uptake capacity for C2H2, C2H4 and C2H6 under ambient conditions, while its capacity for CH4 was very low. High selectivity from IAST calculations for C2H2/CH4, C2H4/CH4 and C2H6/CH4 binary mixtures demonstrated that this MOF material were promising for efficiently separating important separation of C2 hydrocarbons from methane in natural gas processing.

Stable carbon isotope ratios in atmospheric methane and some of its sources

NASA Technical Reports Server (NTRS)

Tyler, Stanley C.

1986-01-01

Ratios of C-13/C-12 have been measured in atmospheric methane and in methane collected from sites and biota that represent potentially large sources of atmospheric methane. These include temperate marshes (about -48 percent to about -54 percent), landfills (about -51 percent to about -55 percent), and the first reported values for any species of termite (-72.8 + or - 3.1 percent for Reticulitermes tibialis and -57.3 + or - 1.6 percent for Zootermopsis angusticollis). Numbers in parentheses are delta C-13 values with respect to PDB (Peedee belemnite) carbonate. Most methane sources reported thus far are depleted in C-13 with respect to atmospheric methane (-47.0 + or - 0.3 percent). Individual sources of methane should have C-13/C-12 ratios characteristic of mechanisms of CH4 formation and consumption prior to release to the atmosphere. The mass-weighted average isotopic composition of all sources should equal the mean C-13 of atmospheric methane, corrected for a kinetic isotope effect in the OH attack of CH4. Assuming the kinetic isotope effect to be small (about -3.0 percent correction to -47.0), as in the literature, the new values given here for termite methane do not help to explain the apparent discrepancy between C-13/C-12 ratios of the known CH4 sources and that of atmospheric CH4.

Geochemical indicators of the origins and evolution of methane in groundwater: Gippsland Basin, Australia.

PubMed

Currell, Matthew; Banfield, Dominic; Cartwright, Ian; Cendón, Dioni I

2017-05-01

Recent expansion of shale and coal seam gas production worldwide has increased the need for geochemical studies in aquifers near gas deposits, to determine processes impacting groundwater quality and better understand the origins and behavior of dissolved hydrocarbons. We determined dissolved methane concentrations (n = 36) and δ 13 C and δ 2 H values (n = 31) in methane and groundwater from the 46,000-km 2 Gippsland Basin in southeast Australia. The basin contains important water supply aquifers and is a potential target for future unconventional gas development. Dissolved methane concentrations ranged from 0.0035 to 30 mg/L (median = 8.3 mg/L) and were significantly higher in the deep Lower Tertiary Aquifer (median = 19 mg/L) than the shallower Upper Tertiary Aquifer (median = 3.45 mg/L). Groundwater δ 13 C DIC values ranged from -26.4 to -0.4 ‰ and were generally higher in groundwater with high methane concentrations (mean δ 13 C DIC  = -9.5 ‰ for samples with >3 mg/L CH 4 vs. -16.2 ‰ in all others), which is consistent with bacterial methanogenesis. Methane had δ 13 C CH4 values of -97.5 to -31.8 ‰ and δ 2 H CH4 values of -391 to -204 ‰ that were also consistent with bacterial methane, excluding one site with δ 13 C CH4 values of -31.8 to -37.9 ‰, where methane may have been thermogenic. Methane from different regions and aquifers had distinctive stable isotope values, indicating differences in the substrate and/or methanogenesis mechanism. Methane in the Upper Tertiary Aquifer in Central Gippsland had lower δ 13 C CH4 (-83.7 to -97.5 ‰) and δ 2 H CH4 (-236 to -391 ‰) values than in the deeper Lower Tertiary Aquifer (δ 13 C CH4  = -45.8 to -66.2 ‰ and δ 2 H CH4  = -204 to -311 ‰). The particularly low δ 13 C CH4 values in the former group may indicate methanogenesis at least partly through carbonate reduction. In deeper groundwater, isotopic values were more consistent with acetate fermentation. Not all methane at a given depth and location is interpreted as being necessarily produced in situ. We propose that high dissolved sulphate concentrations in combination with high methane concentrations can indicate gas resulting from contamination and/or rapid migration as opposed to in situ bacterial production or long-term migration. Isotopes of methane and dissolved inorganic carbon (DIC) serve as further lines of evidence to distinguish methane sources. The study demonstrates the value of isotopic characterisation of groundwater including dissolved gases in basins containing hydrocarbons.

Ice core measurements of 14CH4 show no evidence of methane release to atmosphere from methane hydrates during a large warming event 11,600 years ago

NASA Astrophysics Data System (ADS)

Petrenko, V. V.; Severinghaus, J. P.; Smith, A.; Riedel, K.; Brook, E.; Schaefer, H.; Baggenstos, D.; Harth, C. M.; Hua, Q.; Buizert, C.; Schilt, A.; Fain, X.; Mitchell, L.; Bauska, T. K.; Orsi, A. J.; Weiss, R. F.

2016-12-01

Marine methane hydrate destabilization has been proposed as a potentially large source of methane to the atmosphere in response to both past and future warming. We present new measurements of 14C of paleoatmospheric methane (CH4) over the Younger Dryas - Preboreal (YD - PB) abrupt warming event (≈11,600 years ago) from ancient ice outcropping at Taylor Glacier, Antarctica. The YD - PB abrupt warming was centered in the North Atlantic, occurred partway through the global warming of last deglaciation and was associated with a ≈ 50% increase in atmospheric CH4 concentrations. 14C can unambiguously identify CH4 emissions from "old carbon" sources, such as CH4 hydrates. All samples from before, during and after the abrupt warming and associated CH4 increase yielded 14CH4 values that are consistent with 14C of atmospheric CO2 at that time, indicating a purely contemporaneous methane source. Our results show that neither the abrupt regional warming nor the gradual global warming that preceded it resulted in detectable CH4 release to the atmosphere from CH4 hydrates during the YD - PB transition. Our results are thus consistent with the hypothesis that the vast majority of CH4 that is released from dissociating hydrates or other old-carbon seafloor CH4 sources is oxidized prior to reaching the atmosphere.

Improving our process understanding of methane emissions from a mid-latitude reservoir by combining eddy covariance monitoring with spatial surveys

EPA Science Inventory

Reservoirs are a globally important source of methane (CH4) to the atmosphere, but measuring CH4 emission rates from reservoirs is difficult due to the spatial and temporal variability of the various emission pathways, including ebullition and diffusion. We used the eddy covarian...

A vacuum ultraviolet laser pulsed field ionization-photoion study of methane (CH 4): Determination of the appearance energy of methylium from methane with unprecedented precision and the resulting impact on the bond dissociation energies of CH 4 and CH 4 +

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chang, Yih -Chung; Xiong, Bo; Bross, David H.

Here, we report on the successful implementation of a high-resolution vacuum ultraviolet (VUV) laser pulsed field ionization-photoion (PFI-PI) detection method for the study of unimolecular dissociation of quantum-state- or energy-selected molecular ions. As a test case, we have determined the 0 K appearance energy (AE 0) for the formation of methylium, CH 3 +, from methane, CH 4, as AE 0 (CH 3 +/CH 4) = 14.32271 ± 0.00013 eV. This value has a significantly smaller error limit, but is otherwise consistent with previous laboratory and/or synchrotron-based studies of this dissociative photoionization onset. Furthermore, the sum of the VUV lasermore » PFI-PI spectra obtained for the parent CH 4 + ion and the fragment CH 3 + ions of methane is found to agree with the earlier VUV pulsed field ionization-photoelectron (VUV-PFI-PE) spectrum of methane, providing unambiguous validation of the previous interpretation that the sharp VUV-PFI-PE step observed at the AE 0 (CH 3 +/CH 4) threshold ensues because of higher PFI detection efficiency for fragment CH 3 + than for parent CH 4 +. This, in turn, is a consequence of the underlying high- n Rydberg dissociation mechanism for the dissociative photoionization of CH 4, which was proposed in previous synchrotron-based VUV-PFI-PE and VUV-PFI-PEPICO studies of CH 4. The present highly accurate 0 K dissociative ionization threshold for CH 4 can be utilized to derive accurate values for the bond dissociation energies of methane and methane cation. For methane, the straightforward application of sequential thermochemistry via the positive ion cycle leads to some ambiguity because of two competing VUV-PFI-PE literature values for the ionization energy of methyl radical. The ambiguity is successfully resolved by applying the Active Thermochemical Tables (ATcT) approach, resulting in D 0 (H-CH 3) = 432.463 ± 0.027 kJ/mol and D 0(H-CH 3 +) = 164.701 ± 0.038 kJ/mol.« less

A vacuum ultraviolet laser pulsed field ionization-photoion study of methane (CH 4): Determination of the appearance energy of methylium from methane with unprecedented precision and the resulting impact on the bond dissociation energies of CH 4 and CH 4 +

DOE PAGES

Chang, Yih -Chung; Xiong, Bo; Bross, David H.; ...

2017-03-27

Here, we report on the successful implementation of a high-resolution vacuum ultraviolet (VUV) laser pulsed field ionization-photoion (PFI-PI) detection method for the study of unimolecular dissociation of quantum-state- or energy-selected molecular ions. As a test case, we have determined the 0 K appearance energy (AE 0) for the formation of methylium, CH 3 +, from methane, CH 4, as AE 0 (CH 3 +/CH 4) = 14.32271 ± 0.00013 eV. This value has a significantly smaller error limit, but is otherwise consistent with previous laboratory and/or synchrotron-based studies of this dissociative photoionization onset. Furthermore, the sum of the VUV lasermore » PFI-PI spectra obtained for the parent CH 4 + ion and the fragment CH 3 + ions of methane is found to agree with the earlier VUV pulsed field ionization-photoelectron (VUV-PFI-PE) spectrum of methane, providing unambiguous validation of the previous interpretation that the sharp VUV-PFI-PE step observed at the AE 0 (CH 3 +/CH 4) threshold ensues because of higher PFI detection efficiency for fragment CH 3 + than for parent CH 4 +. This, in turn, is a consequence of the underlying high- n Rydberg dissociation mechanism for the dissociative photoionization of CH 4, which was proposed in previous synchrotron-based VUV-PFI-PE and VUV-PFI-PEPICO studies of CH 4. The present highly accurate 0 K dissociative ionization threshold for CH 4 can be utilized to derive accurate values for the bond dissociation energies of methane and methane cation. For methane, the straightforward application of sequential thermochemistry via the positive ion cycle leads to some ambiguity because of two competing VUV-PFI-PE literature values for the ionization energy of methyl radical. The ambiguity is successfully resolved by applying the Active Thermochemical Tables (ATcT) approach, resulting in D 0 (H-CH 3) = 432.463 ± 0.027 kJ/mol and D 0(H-CH 3 +) = 164.701 ± 0.038 kJ/mol.« less

Sources and flux of natural gases from Mono Lake, California

USGS Publications Warehouse

Oremland, R.S.; Miller, L.G.; Whiticar, Michael J.

1987-01-01

The ability to identify a formation mechanism for natural gas in a particular environment requires consideration of several geochemical factors when there are multiple sources present. Four primary sources of methane have been identified in Mono Lake. Two of these sources were associated with numerous natural gas seeps which occur at various locations in the lake and extend beyond its present boundary; the two other gas sources result from current microbiological processes. In the natural gas seeps, we observed flow rates as high as 160 moles CH4 day-1, and estimate total lakewide annual seep flux to be 2.1 ?? 106 moles CH4. Geochemical parameters (??13CH4,??DCH4,CH4/[C2H6+ C3H8]) and ??14CH4measurements revealed that most of the seeps originate from a paleo-biogenic (??13CH4 = about -70%.). natural gas deposit of Pleistocene age which underlies the current and former lakebed. Gas seeps in the vicinity of hot springs had, in combination with the biogenic gas, a prominent thermogenic gas component resulting from hydrothermal alteration of buried organic matter. Current microbiological processes responsible for sources of natural gas in the lake included pelagic meth- anogenesis and decomposition of terrestrial grasses in the littoral zone. Methanogenesis in the pelagic sediments resulted in methane saturation (2-3 mM at 50 cm; ??13CH4 = about -85%.). Interstitial sulfate decreased from 133 mM at the surface to 35 mM by 110 cm depth, indicating that sulfate-reduction and methanogenesis operated concurrently. Methane diffused out of the sediments resulting in concentrations of about 50 ??M in the anoxic bottom waters. Methane oxidation in the oxic/anoxic boundry lowered the concentration by >98%, but values in surface waters (0.1-1.3??M) were supersaturated with respect to the atmosphere. The ??13CH4 (range = -21.8 to -71.8%.) of this unoxidized residual methane was enriched in 13C relative to methane in the bottom water and sediments. Average outward flux of this methane was 2.77 ?? 107 moles yr-1. A fourth, but minor source of methane (??13CH4 = -55.2%.) was associated with the decomposition of terrestrial grasses taking place in the lake's recently expanded littoral zone. ?? 1987.

Milk metabolome relates enteric methane emission to milk synthesis and energy metabolism pathways.

PubMed

Antunes-Fernandes, E C; van Gastelen, S; Dijkstra, J; Hettinga, K A; Vervoort, J

2016-08-01

Methane (CH4) emission of dairy cows contributes significantly to the carbon footprint of the dairy chain; therefore, a better understanding of CH4 formation is urgently needed. The present study explored the milk metabolome by gas chromatography-mass spectrometry (milk volatile metabolites) and nuclear magnetic resonance (milk nonvolatile metabolites) to better understand the biological pathways involved in CH4 emission in dairy cattle. Data were used from a randomized block design experiment with 32 multiparous Holstein-Friesian cows and 4 diets. All diets had a roughage:concentrate ratio of 80:20 (dry matter basis) and the roughage was grass silage (GS), corn silage (CS), or a mixture of both (67% GS, 33% CS; 33% GS, 67% CS). Methane emission was measured in climate respiration chambers and expressed as CH4 yield (per unit of dry matter intake) and CH4 intensity (per unit of fat- and protein-corrected milk; FPCM). No volatile or nonvolatile metabolite was positively related to CH4 yield, and acetone (measured as a volatile and as a nonvolatile metabolite) was negatively related to CH4 yield. The volatile metabolites 1-heptanol-decanol, 3-nonanone, ethanol, and tetrahydrofuran were positively related to CH4 intensity. None of the volatile metabolites was negatively related to CH4 intensity. The nonvolatile metabolites acetoacetate, creatinine, ethanol, formate, methylmalonate, and N-acetylsugar A were positively related to CH4 intensity, and uridine diphosphate (UDP)-hexose B and citrate were negatively related to CH4 intensity. Several volatile and nonvolatile metabolites that were correlated with CH4 intensity also were correlated with FPCM and not significantly related to CH4 intensity anymore when FPCM was included as covariate. This suggests that changes in these milk metabolites may be related to changes in milk yield or metabolic processes involved in milk synthesis. The UDP-hexose B was correlated with FPCM, whereas citrate was not. Both metabolites were still related to CH4 intensity when FPCM was included as covariate. The UDP-hexose B is an intermediate of lactose metabolism, and citrate is an important intermediate of Krebs cycle-related energy processes. Therefore, the negative correlation of UDP-hexose B and citrate with CH4 intensity may reflect a decrease in metabolic activity in the mammary gland. Our results suggest that an integrative approach including milk yield and composition, and dietary and animal traits will help to explain the biological metabolism of dairy cows in relation to methane CH4 emission. Copyright © 2016 American Dairy Science Association. Published by Elsevier Inc. All rights reserved.

Megafauna and frozen soil: the drivers of atmospheric CH4 dynamics

NASA Astrophysics Data System (ADS)

Zimov, N.; Zimov, S. A.

2010-12-01

During the last deglaciation (LD) a strong increase in atmospheric methane (CH4) concentrations occurred simultaneously with a rise in Greenland temperatures indicating that in the north, during this time period, strong CH4 sources “awakened”, as additionally documented by the appearance of a strong gradient between northern (Greenland) and southern (Antarctica) hemisphere atmospheric CH4 concentrations. This rise could not be caused by wetland expansion. A reconstruction of peatland formation dynamics has indicated that wetlands on Earth were few in LD and only actively expanded 10,000 yr BP, after atmospheric CH4 concentrations began to decline. Destabilization of methane clathrates also could not be the source for atmospheric CH4 increase. Geological CH4 (including methane clathrates) has the highest deuterium content (δD) among all of the known sources of CH4 while atmospheric CH4 δD values determined for the LD were record low. To explain recorded atmospheric CH4 and its isotopic dynamics required a strong northern source, which was active only during the LD and that provided very low δD CH4 values. Such a source is permafrost thawing under anaerobic conditions (or better stated soils of mammoth steppe-tundra ecosystems). Permafrost thawing is the strongest, among known, wetland sources (usually over 100g CH4/m2yr) and has a unique isotopic signature (δD = -400 per mil (-338 to -479 per mil), δ13C = -73 per mil (-58 to -99 per mil)). The main sources of atmospheric CH4 have different isotopic signatures (δ13C, δD). The isotopic content of atmospheric CH4 is a simple function of the weight average for all of the sources. Inclusion of permafrost source into a budget model of the atmospheric methane and its isotopes allowed us to reconstruct the dynamics of methane’s main sources. Model indicated geological source to be negligible as in LGM so and in LD and Holocene. During the glaciation, the largest methane source was megafauna, whose 1.4-1.7 billion ton biomass was larger than the modern biomass of human and domestic animals combined. During the LD, the largest methane source was the thawing of steppe-tundra soils. During the Holocene the largest CH4 source was wetlands. All these estimates correspond with the scales of permafrost degradation in the LD, megafaunal extinction and increase in fire intensity derived from charcoal within stratigraphic columns.

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

NASA Astrophysics Data System (ADS)

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 agriculture continue to decline. The use of inverse modeling to exploit the information content of CH4 and 13CH4/12CH4 measurements can provide important constraints on bottom-up estimates of wetland emissions but the method requires choosing numerous model parameters. We explore the sensitivity of our results to a number of these choices.

Oxidative mitigation of aquatic methane emissions in large Amazonian rivers.

PubMed

Sawakuchi, Henrique O; Bastviken, David; Sawakuchi, André O; Ward, Nicholas D; Borges, Clovis D; Tsai, Siu M; Richey, Jeffrey E; Ballester, Maria Victoria R; Krusche, Alex V

2016-03-01

The flux of methane (CH4 ) from inland waters to the atmosphere has a profound impact on global atmospheric greenhouse gas (GHG) levels, and yet, strikingly little is known about the dynamics controlling sources and sinks of CH4 in the aquatic setting. Here, we examine the cycling and flux of CH4 in six large rivers in the Amazon basin, including the Amazon River. Based on stable isotopic mass balances of CH4 , inputs and outputs to the water column were estimated. We determined that ecosystem methane oxidation (MOX) reduced the diffusive flux of CH4 by approximately 28-96% and varied depending on hydrologic regime and general geochemical characteristics of tributaries of the Amazon River. For example, the relative amount of MOX was maximal during high water in black and white water rivers and minimal in clear water rivers during low water. The abundance of genetic markers for methane-oxidizing bacteria (pmoA) was positively correlated with enhanced signals of oxidation, providing independent support for the detected MOX patterns. The results indicate that MOX in large Amazonian rivers can consume from 0.45 to 2.07 Tg CH4 yr(-1) , representing up to 7% of the estimated global soil sink. Nevertheless, climate change and changes in hydrology, for example, due to construction of dams, can alter this balance, influencing CH4 emissions to atmosphere. © 2015 John Wiley & Sons Ltd.

Kinetics of biological methane oxidation in the presence of non-methane organic compounds in landfill bio-covers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Albanna, Muna, E-mail: muna.albanna@gju.edu.j; Warith, Mostafa; Fernandes, Leta

2010-02-15

In this experimental program, the effects of non-methane organic compounds (NMOCs) on the biological methane (CH{sub 4}) oxidation process were examined. The investigation was performed on compost experiments incubated with CH{sub 4} and selected NMOCs under different environmental conditions. The selected NMOCs had different concentrations and their effects were tested as single compounds and mixtures of compounds. The results from all experimental sets showed a decrease in CH{sub 4} oxidation capacity of the landfill bio-cover with the increase in NMOCs concentrations. For example, in the experiment using compost with 100% moisture content at 35 deg. C without any NMOCs themore » V{sub max} value was 35.0 mug CH{sub 4}h{sup -1}g{sub wetwt}{sup -1}. This value was reduced to 19.1 mug CH{sub 4}h{sup -1}g{sub wetwt}{sup -1} when mixed NMOCs were present in the batch reactors under the same environmental conditions. The experimental oxidation rates of CH{sub 4} in the presence of single and mixed NMOCs were modeled using the uncompetitive inhibition model and kinetic parameters, including the dissociation constants, were obtained. Additionally, the degradation rates of the NMOCs and co-metabolic abilities of methanotrophic bacteria were estimated.« less

Modeling natural wetlands: A new global framework built on wetland observations

NASA Astrophysics Data System (ADS)

Matthews, E.; Romanski, J.; Olefeldt, D.

2015-12-01

Natural wetlands are the world's largest methane (CH4) source, and their distribution and CH4 fluxes are sensitive to interannual and longer-term climate variations. Wetland distributions used in wetland-CH4 models diverge widely, and these geographic differences contribute substantially to large variations in magnitude, seasonality and distribution of modeled methane fluxes. Modeling wetland type and distribution—closely tied to simulating CH4 emissions—is a high priority, particularly for studies of wetlands and CH4 dynamics under past and future climates. Methane-wetland models either prescribe or simulate methane-producing areas (aka wetlands) and both approaches result in predictable over- and under-estimates. 1) Monthly satellite-derived inundation data include flooded areas that are not wetlands (e.g., lakes, reservoirs, and rivers), and do not identify non-flooded wetlands. 2) Models simulating methane-producing areas overwhelmingly rely on modeled soil moisture, systematically over-estimating total global area, with regional over- and under-estimates, while schemes to model soil-moisture typically cannot account for positive water tables (i.e., flooding). Interestingly, while these distinct hydrological approaches to identify wetlands are complementary, merging them does not provide critical data needed to model wetlands for methane studies. We present a new integrated framework for modeling wetlands, and ultimately their methane emissions, that exploits the extensive body of data and information on wetlands. The foundation of the approach is an existing global gridded data set comprising all and only wetlands, including vegetation information. This data set is augmented with data inter alia on climate, inundation dynamics, soil type and soil carbon, permafrost, active-layer depth, growth form, and species composition. We investigate this enhanced wetland data set to identify which variables best explain occurrence and characteristics of observed wetland ecosystems. The novelty of the new approach is that it starts from what we know about wetlands, builds ecosystem-specific models from these observations, and avoids known biases in current hydrology-based approaches to wetland definition in methane models.

Effects of paddy rice agriculture on the seasonal dynamics of atmospheric methane concentration

NASA Astrophysics Data System (ADS)

Zhang, G.; Xiao, X.; Dong, J.; Zhang, Y.; Xin, F.; Zhou, Y.; Wang, J.; Wu, X.; Moore, B., III

2017-12-01

Methane (CH4) is an important greenhouse gas (GHG) and may account for 20 % of anticipated global warming. The atmospheric CH4 concentration was nearly constant from 1999 to 2006, following with a strong growth resumed since 2007. Previous study attributed the increase in CH4 to agriculture. Specifically, paddy rice agriculture is a significant source of CH4, but large uncertainty still exists on methane emission estimates from rice paddies, largely due to lack of detailed geospatial datasets of rice paddies. In this study, based on a pixel- and phenology-based image analysis system with multi-temporal MODIS imagery (MODIS-RICE), we generated the paddy rice map in 2005 to document the spatiotemporal pattern of paddy rice dynamics in Monsoon Asia, which accounts for more than 90% of the global rice production. Furthermore, we examined the effects of paddy rice agriculture on atmospheric CH4 concentration over Monsoon Asia, by comparing atmospheric CH4 concentration data from SCIAMACHY sensor and the paddy rice maps in 2005. We found a significant spatial consistency between spatial patterns of paddy rice and atmospheric CH4 concentration. Based on the high resolution paddy rice map, different seasonal dynamics of CH4 concentration, including single, double to triple peaks, were found based on the rice paddy distribution information. That suggests paddy rice agriculture contributes substantially to the spatial and seasonal pattern of atmospheric CH4 concentration in Monsoon Asia. This study provides satellite evidence for seasonal cycle of CH4 dynamics at regional scale, and suggests that shifting regime of paddy rice agriculture and cropping intensity could affect the seasonal dynamics and spatial pattern of atmospheric methane concentration.

Consumption of atmospheric methane by desert soils

USGS Publications Warehouse

Striegl, Robert G.; McConnaughey, T.A.; Thorstenson, D.C.; Weeks, E.P.; Woodward, J.C.

1992-01-01

ATMOSPHERIC concentrations of methane, a greenhouse gas, are increasing at a rate of about 1% yr-1 (refs 1-4). Oxidation by methylotrophic bacteria in soil is the largest terrestrial sink for atmospheric CH4, and is estimated to consume about 30?? 1012 g CH4 yr-1 (refs 4-6). Spatial and temporal variability in the rate of soil CH4 consumption are incompletely understood6-19, as are the apparent inhibitory12,13,18 or enhancing20 effects of changes in land use. Dry deserts, which constitute 20% of total land surface, are not currently included in global soil uptake estimates. Here we describe measurements of the rate of uptake of atmospheric CH4 by undisturbed desert soils. We observed rates as great as 4.38 mg CH4 m-2 day-1; 50% of the measured rates were between 0.24 and 0.92 mg CH4 m2 d-1. Uptake of CH4 by desert soil is enhanced by rainfall after an initial soil-drainage period - opposite to the response of temperate forest soils12. Methane is consumed to a depth of about 2 m, allowing for deep removal of atmospheric CH4 if near-surface conditions are unfavourable for consumption. On the basis of an annual average CH4 consumption rate of 0.66 mg CH4 m-2 d-1, we estimate that the global CH4 sink term needs to be increased by about 7 ?? 1012 g yr-1 to account for the contribution of desert soils.

Production of biogas (methane and hydrogen) from anaerobic digestion of hemicellulosic hydrolysate generated in the oxidative pretreatment of coffee husks.

PubMed

Santos, Lívia Caroline Dos; Adarme, Oscar Fernando Herrera; Baêta, Bruno Eduardo Lobo; Gurgel, Leandro Vinícius Alves; Aquino, Sérgio Francisco de

2018-05-21

Ozone pretreatment of coffee husks (CH) was evaluated to generate hydrolysates for biogas production and to preserve cellulose of the solid phase for 2G ethanol production. Pretreatment variables included liquid-to-solid ratio (LSR), pH and specific applied ozone load (SAOL). Considering single-stage anaerobic digestion (AD), the highest methane production (36 NmL CH 4 /g CH) was achieved with the hydrolysate generated in the experiment using LSR 10 mL/g, pH 11 and SAOL 18.5 mg O 3 /g CH, leading to 0.064 kJ/g CH energy recovery. Due to the presence of toxic compounds in the hydrolysate, the addition of powdered activated carbon (4 g/L) to the reactor enhanced biogas production, leading to 86 NmL CH 4 /g CH yield and 0.58 kJ/g CH energy recovery. When two-stage AD was applied, methane production resulted in 49 NmL CH 4 /g CH, with additional 19 NmL H 2 /g CH production, resulting in a net 0.26 kJ/g CH energy recovery. Copyright © 2018 Elsevier Ltd. All rights reserved.

Role Of Fires On The Global Methane Budget And Atmospheric Methane Increase Since 2006

NASA Astrophysics Data System (ADS)

Worden, J.; Bloom, A. A.; Jiang, Z.; Pandey, S.; Walker, T. W.; Worden, H. M.

2016-12-01

Since 2006, Methane has increased at an average rate of 7 ppb/year. Satellite based measurements of total column CH4 suggest that 70% of this increase is from N. American (likely fossil fuel) sources whereas surface isotope data attribute the increase almost entirely to emissions from tropical wetlands or agriculture. However, large uncertainties in all components of the methane budget suggest any one source could substantially affect the growth rate of atmospheric methane. Here we examine the role of fires on the recent changes in atmospheric methane. We use satellite measurements of CH4 and CO to show that total land-use related CH4 fire emissions have decreased from 14+/-4 Tg during the 2001-2006 time period to 11+/- 4 Tg for the 2007-2015 time period, consistent with bottom-up estimates. Largest reductions are over S. America and Indonesia, likely as a result of increased rainfall during this time period. Fire emissions of methane are isotopically enhanced relative to fossil fuels and wetlands. Including the effects of fires in a global isotopic box model indicates that fossil fuels can account for 1/3 of the recent increase with the remaining due to biogenic sources.

Quantifying sources of methane and light alkanes in the Los Angeles Basin, California

NASA Astrophysics Data System (ADS)

Peischl, Jeff; Ryerson, Thomas; Atlas, Elliot; Blake, Donald; Brioude, Jerome; Daube, Bruce; de Gouw, Joost; Frost, Gregory; Gentner, Drew; Gilman, Jessica; Goldstein, Allen; Harley, Robert; Holloway, John; Kuster, William; Santoni, Gregory; Trainer, Michael; Wofsy, Steven; Parrish, David

2013-04-01

We use ambient measurements to apportion the relative contributions of different source sectors to the methane (CH4) emissions budget of a U.S. megacity. This approach uses ambient measurements of methane and C2-C5 alkanes (ethane through pentanes) and includes source composition information to distinguish between methane emitted from landfills and feedlots, wastewater treatment plants, tailpipe emissions, leaks of dry natural gas in pipelines and/or local seeps, and leaks of locally produced (unprocessed) natural gas. Source composition information can be taken from existing tabulations or developed by direct sampling of emissions using a mobile platform. By including C2-C5 alkane information, a linear combination of these source signatures can be found to match the observed atmospheric enhancement ratios to determine relative emissions strengths. We apply this technique to apportion CH4 emissions in Los Angeles, CA (L.A.) using data from the CalNex field project in 2010. Our analysis of L.A. atmospheric data shows the two largest CH4 sources in the city are emissions of gas from pipelines and/or from geologic seeps (47%), and emissions from landfills (40%). Local oil and gas production is a relatively minor source of CH4, contributing 8% of total CH4 emissions in L.A. Absolute CH4 emissions rates are derived by multiplying the observed CH4/CO enhancement ratio by State of California inventory values for carbon monoxide (CO) emissions in Los Angeles. Apportioning this total suggests that emissions from the combined natural and anthropogenic gas sources account for the differences between top-down and bottom-up CH4 estimates previously published for Los Angeles. Further, total CH4 emission attributed in our analysis to local gas extraction represents 17% of local production. While a derived leak rate of 17% of local production may seem unrealistically high, it is qualitatively consistent with the 12% reported in a recent state inventory survey of the L.A. oil and gas industry.

Methane oxidation in an intensively cropped tropical rice field soil under long-term application of organic and mineral fertilizers.

PubMed

Nayak, D R; Babu, Y Jagadeesh; Datta, A; Adhya, T K

2007-01-01

Methane (CH4) oxidation is the only known biological sink process for mitigating atmospheric and terrestrial emissions of CH4, a major greenhouse gas. Methane oxidation in an alluvial soil planted to rice (Oryza sativa L.) under long-term application of organic (compost with a C/N ratio of 21.71), and mineral fertilizers was measured in a field-cum-laboratory incubation study. Oxidation rates were quantified in terms of decrease in the concentration of CH4 in the headspace of incubation vessels and expressed as half-life (t(1)2) values. Methane oxidation rates significantly differed among the treatments and growth stages of the rice crop. Methane oxidation rates were high at the maximum tillering and maturity stages, whereas they were low at grain-filling stage. Methane oxidation was low (t(1)2) = 15.76 d) when provided with low concentration of CH4. On the contrary, high concentration of CH4 resulted in faster oxidation (t(1)2) = 6.67 d), suggesting the predominance of "low affinity oxidation" in rice fields. Methane oxidation was stimulated following the application of mineral fertilizers or compost implicating nutrient limitation as one of the factors affecting the process. Combined application of compost and mineral fertilizer, however, inhibited CH4 oxidation probably due to N immobilization by the added compost. The positive effect of mineral fertilizer on CH4 oxidation rate was evident only at high CH4 concentration (t(1)2 = 4.80 d), while at low CH4 concentration their was considerable suppression (t(1) = 17.60 d). Further research may reveal that long-term application of fertilizers, organic or inorganic, may not inhibit CH4 oxidation.

Isotopic constraints on methane's global sources and ENSO-dependence

NASA Astrophysics Data System (ADS)

Schaefer, Hinrich; Mikaloff Fletcher, Sara; Veidt, Cora; Lassey, Keith; Brailsford, Gordon; Bromley, Tony; Dlugokencky, Ed; Englund Michel, Sylvia; Miller, John; Levin, Ingeborg; Lowe, Dave; Martin, Ross; Vaughn, Bruce; White, James; Nichol, Sylvia

2017-04-01

Atmospheric levels of the potent greenhouse gas methane (CH4) have been rising since the industrial revolution, except for a plateau during the early 2000s. Stable carbon isotopes in methane (delta-13CH4) provide constraints on the budget changes associated with the plateau's onset and its end. We present a reconstruction of annual global delta-13CH4 averages based on a global network of stations, whose trends are indicative of global methane source and sink activity. A box model analysis shows that from the mid-1990s methane emissions with the characteristic thermogenic delta-13CH4 signature reduced, implying persistently lower emissions from fossil fuel productions as the cause of the plateau. However, variations in hydroxyl, the main CH4 sink, provide an equably plausible explanation for the plateau onset that may also account for strong variability in emission-vs-removal rates during the plateau period. In contrast, the renewed CH4 rise since 2006 can only be explained by increasing emissions with a biogenic isotope signature, i.e. agriculture or wetlands. We present correlation studies that test whether ENSO activity controls atmospheric delta-13CH4, and by extension methane levels, through tropical wetland emissions.

Towards improved bottom-up inventories of methane from the European land surface

NASA Astrophysics Data System (ADS)

Grunwald, Dennis; Fender, Ann-Catrin; Erasmi, Stefan; Jungkunst, Hermann F.

2012-05-01

Forests and wetlands are generally seen as opposites in the methane cycle of terrestrial ecosystems. Wetlands are sources for atmospheric methane and forest soils sinks. However, this greenhouse gas is also emitted by wet forest soils, which is commonly disregarded due to lacking information on their spatial distribution. Here, we estimated the potential bias made for the European methane budget of terrestrial ecosystems when neglecting wet forest ecosystems but including rice paddies and latest estimates for lakes. We appointed distinct annual methane rates for individual land use types based on a literature survey and weighted them according to their European area. This was performed separately for four major ecozones (cold, temperate, continental and Mediterranean). Three approaches were applied: (1) the mean values for forests and wetlands were calculated in three different scenarios, (2) assuming that boreal needle-leaved evergreen forest with a low tree cover (<40%) is predominately forested wetland (3) assuming different shares of wet forest ecosystems in individual forest areas. For the net balance 2.8 Tg CH4-C a-1 were calculated which includes emissions from rice paddies (0.2 Tg CH4-C a-1) and from lakes (2.5 Tg CH4-C a-1). The different approaches for the net balances that included wet forest ecosystems mainly ranged between 4.6 and 6.7 Tg CH4-C a-1. The results suggest that wet forest ecosystems are approximately as important as wetlands for the European methane balance. European bottom-up inventories are improved best by more accurate mapping of wetlands both within and outside forests and more flux data for lakes and continental wetlands.

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

NASA Astrophysics Data System (ADS)

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.

Gammaproteobacterial Methanotrophs Dominate Cold Methane Seeps in Floodplains of West Siberian Rivers

PubMed Central

Oshkin, Igor Y.; Wegner, Carl-Eric; Lüke, Claudia; Glagolev, Mikhail V.; Filippov, Illiya V.; Pimenov, Nikolay V.; Liesack, Werner

2014-01-01

A complex system of muddy fluid-discharging and methane (CH4)-releasing seeps was discovered in a valley of the river Mukhrinskaya, one of the small rivers of the Irtysh Basin, West Siberia. CH4 flux from most (90%) of these gas ebullition sites did not exceed 1.45 g CH4 h−1, while some seeps emitted up to 5.54 g CH4 h−1. The δ13C value of methane released from these seeps varied between −71.1 and −71.3‰, suggesting its biogenic origin. Although the seeps were characterized by low in situ temperatures (3.5 to 5°C), relatively high rates of methane oxidation (15.5 to 15.9 nmol CH4 ml−1 day−1) were measured in mud samples. Fluorescence in situ hybridization detected 107 methanotrophic bacteria (MB) per g of mud (dry weight), which accounted for up to 20.5% of total bacterial cell counts. Most (95.8 to 99.3%) methanotroph cells were type I (gammaproteobacterial) MB. The diversity of methanotrophs in this habitat was further assessed by pyrosequencing of pmoA genes, encoding particulate methane monooxygenase. A total of 53,828 pmoA gene sequences of seep-inhabiting methanotrophs were retrieved and analyzed. Nearly all of these sequences affiliated with type I MB, including the Methylobacter-Methylovulum-Methylosoma group, lake cluster 2, and several as-yet-uncharacterized methanotroph clades. Apparently, microbial communities attenuating methane fluxes from these local but strong CH4 sources in floodplains of high-latitude rivers have a large proportion of potentially novel, psychrotolerant methanotrophs, thereby providing a challenge for future isolation studies. PMID:25063667

An Ecosystem Simulation Model for Methane Production and Emission from Wetlands

NASA Technical Reports Server (NTRS)

Potter, C. S.; Peterson, David L. (Technical Monitor)

1997-01-01

Previous experimental studies suggest that methane emission from wetland is influenced by multiple interactive pathways of gas production and transport through soil and sediment layers to the atmosphere. The objective of this study is to evaluate a new simulation model of methane production and emission in wetland soils that was developed initially to help identify key processes that regulate methanogenesis and net flux of CH4 to the air, but which is designed ultimately for regional simulation using remotely sensed inputs for land cover characteristics. The foundation for these computer simulations is based on a well-documented model (CASA) of ecosystem production and carbon cycling in the terrestrial blaspheme. Modifications to represent flooded wetland soils and anaerobic decomposition include three new sub-models for: (1) layered soil temperature and water table depth (WTD) as a function of daily climate drivers, (2) CH4 production within the anoxic soil layer as a function of WTD and CO2 production under poorly drained conditions, and (3) CH4 gaseous transport pathways (molecular diffusion, ebullition, and plant vascular transport) as a function of WTD and ecosystem type. The model was applied and tested using climate and ecological data to characterize tundra wetland sites near Fairbanks, Alaska studied previously by Whalen and Reeburgh. Comparison of model predictions to measurements of soil temperature and thaw depth, water-table depth, and CH4 emissions over a two year period suggest that inter-site differences in soil physical conditions and methane fluxes could be reproduced accurately for selected periods. Day-to-day comparison of predicted emissions to measured CH4 flux rates reveals good agreement during the early part of the thaw season, but the model tends to underestimate production of CH4 during the months of July and August in both test years. Important seasonal effects, including that of falling WTD during these periods, are apparently overlooked in the model formulation. Nevertheless, reasonably close agreement was achieved between the model's mean daily and seasonal estimates of CH4 flux and observed emission rates for northern wetland ecosystems. Several features of the model are identified as crucial to more accurate prediction of wetland methane emission, including the capacity to incorporate influences of localized topographic and hydrologic features on site-specific soil temperature and WTD dynamics, and mechanistic simulation of methane emission transport pathways from within the soil profile.

The global methane budget 2000-2012

NASA Astrophysics Data System (ADS)

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

2016-12-01

The global methane (CH4) budget is becoming an increasingly important component for managing realistic pathways to mitigate climate change. This relevance, due to a shorter atmospheric lifetime and a stronger warming potential than carbon dioxide, is challenged by the still unexplained changes of atmospheric CH4 over the past decade. Emissions and concentrations of CH4 are continuing to increase, making CH4 the second most important human-induced greenhouse gas after carbon dioxide. Two major difficulties in reducing uncertainties come from the large variety of diffusive CH4 sources that overlap geographically, and from the destruction of CH4 by the very short-lived hydroxyl radical (OH). To address these difficulties, we have established a consortium of multi-disciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate research on the methane cycle, and producing regular (˜ biennial) updates of the global methane budget. This consortium includes atmospheric physicists and chemists, biogeochemists of surface and marine emissions, and socio-economists who study anthropogenic emissions. Following Kirschke et al. (2013), we propose here the first version of a living review paper that integrates results of top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models, inventories and data-driven approaches (including process-based models for estimating land surface emissions and atmospheric chemistry, and inventories for anthropogenic emissions, data-driven extrapolations). For the 2003-2012 decade, global methane emissions are estimated by top-down inversions at 558 Tg CH4 yr-1, range 540-568. About 60 % of global emissions are anthropogenic (range 50-65 %). Since 2010, the bottom-up global emission inventories have been closer to methane emissions in the most carbon-intensive Representative Concentrations Pathway (RCP8.5) and higher than all other RCP scenarios. Bottom-up approaches suggest larger global emissions (736 Tg CH4 yr-1, range 596-884) mostly because of larger natural emissions from individual sources such as inland waters, natural wetlands and geological sources. Considering the atmospheric constraints on the top-down budget, it is likely that some of the individual emissions reported by the bottom-up approaches are overestimated, leading to too large global emissions. Latitudinal data from top-down emissions indicate a predominance of tropical emissions (˜ 64 % of the global budget, < 30° N) as compared to mid (˜ 32 %, 30-60° N) and high northern latitudes (˜ 4 %, 60-90° N). Top-down inversions consistently infer lower emissions in China (˜ 58 Tg CH4 yr-1, range 51-72, -14 %) and higher emissions in Africa (86 Tg CH4 yr-1, range 73-108, +19 %) than bottom-up values used as prior estimates. Overall, uncertainties for anthropogenic emissions appear smaller than those from natural sources, and the uncertainties on source categories appear larger for top-down inversions than for bottom-up inventories and models. The most important source of uncertainty on the methane budget is attributable to emissions from wetland and other inland waters. We show that the wetland extent could contribute 30-40 % on the estimated range for wetland emissions. Other priorities for improving the methane budget include the following: (i) the development of process-based models for inland-water emissions, (ii) the intensification of methane observations at local scale (flux measurements) to constrain bottom-up land surface models, and at regional scale (surface networks and satellites) to constrain top-down inversions, (iii) improvements in the estimation of atmospheric loss by OH, and (iv) improvements of the transport models integrated in top-down inversions. The data presented here can be downloaded from the Carbon Dioxide Information Analysis Center (http://doi.org/10.3334/CDIAC/GLOBAL_METHANE_BUDGET_2016_V1.1) and the Global Carbon Project.

Natural and anthropogenic variations in methane sources during the past two millennia

NASA Astrophysics Data System (ADS)

Sapart, C. J.; Monteil, G.; Prokopiou, M.; Vandewal, R.; Kaplan, J. O.; Sperlich, P.; Krumhardt, K.; van der Veen, C.; Houweling, S.; Krol, M. C.; Blunier, T.; Sowers, T. A.; Martinerie, P.; Witrant, E.; Dahl-Jensen, D.; Roeckmann, T.

2012-12-01

Methane (CH4) is an important greenhouse gas that is emitted from multiple natural and anthropogenic sources. Atmospheric levels of CH4 have varied on various timescales in the past, but in many cases the causes of these variations are not understood. Analysis of the isotopic composition of CH4 provides evidence for the environmental drivers of variations in CH4 atmospheric abundance, because different sources and sinks affect the isotopic composition of CH4 specifically. Our data from air trapped in the NEEM and EUROCORE Greenland ice cores show that the carbon isotopic composition (δ13C) of CH4 underwent pronounced centennial-scale variations between 100 BC and 1600 AD. Two-box model calculations suggest that the centennial-scale variations in isotope ratios are due to changes in both pyrogenic and biogenic sources. These changes are correlated with both natural climate variability including the Medieval Climate Anomaly and the Little Ice Age and with changes in human population, land-use and with the decline of both the Roman Empire and the Han dynasty and the Medieval period. Our findings suggest that between 100 BC and 1600 AD human activities may have been responsible for about 20-30 per cent of the total pyrogenic methane emissions and that they have therefore contributed to variations in methane emissions long before the onset of the industrial revolution.

Modeling methane emissions from Arctic lakes under warming conditions

NASA Astrophysics Data System (ADS)

Zhuang, Qianlai; Tan, Zeli

2014-05-01

To investigate the response of methane emissions from arctic lakes, a process-based climate-sensitive lake methane model is developed. The processes of methane production, oxidation and transport are modeled within a one-dimensional water and sediment column. Dynamics of point-source ebullition seeps are explicitly modeled. The model was calibrated and verified using observational data in the region. The model was further used to estimate the lake methane emissions from the Arctic from 2002 to 2004. We estimate that the total amount of methane emissions is 24.9 Tg CH4 yr-1, which is consistent with a recent estimation of 24±10 Tg CH4 yr-1 and two-fold of methane emissions from natural wetlands in the north of 60 oN. The methane emission rate of lakes spatially varies over high latitudes from 170.5 mg CH4 m-2 day-1 in northern Siberia to only 10.1 mg CH4 m-2 day-1 in northern Europe. A projection assuming 2-7.5oC warming and 15-25% expansion of lake coverage shows that the total amount of methane emitted from Arctic lakes will increase to 29.8-35.6 Tg CH4 yr-1.

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

NASA Technical Reports Server (NTRS)

Greene, Sandra Elam

2015-01-01

In recent years, a variety of injectors for liquid oxygen (LOX) and methane (CH4) propellant systems have been designed, fabricated, and demonstrated with hot-fire testing at Marshall Space Flight Center (MSFC). Successful designs for liquid methane (LCH4) and gaseous methane (GCH4) have been developed. A variety of chambers, including a transpiration cooled design, along with uncooled ablatives and refractory metals, have also been hot-fire tested by MSFC for use with LOX/LCH4 injectors. Hot-fire testing has also demonstrated multiple ignition source options. Heat flux data for selected injectors has been gathered by testing with a calorimeter chamber. High performance and stable combustion have been demonstrated, along with designs for thrust levels ranging from 500 to 7,000 lbf. The newest LOX/CH4 injector and chamber developed by MSFC have been fabricated with additive manufacturing techniques and include unique design features to investigate regenerative cooling with methane. This low cost and versatile hardware offers a design for 4,000 lbf thrust and will be hot-fire tested at MSFC in 2015. Its design and operation can easily be scaled for use in systems with thrust levels up to 25,000 lbf.

Climatic variability, hydrologic anomaly, and methane emission can turn productive freshwater marshes into net carbon sources

Treesearch

Housen Chu; Johan F. Gottgens; Jiquan Chen; Ge Sun; Ankur R. Desai; Zutao Ouyang; Changliang Shao; Kevin Czajkowski

2015-01-01

Freshwater marshes are well-known for their ecological functions in carbon sequestration, but complete carbon budgets that include both methane (CH4) and lateral carbon fluxes for these ecosystems are rarely available. To the best of our knowledge, this is the first full carbon balance for a freshwater marsh where vertical gaseous [carbon dioxide (CO2) and CH4] and...

A stream-based methane monitoring approach for evaluating groundwater impacts associated with unconventional gas development.

PubMed

Heilweil, Victor M; Stolp, Bert J; Kimball, Briant A; Susong, David D; Marston, Thomas M; Gardner, Philip M

2013-01-01

Gaining streams can provide an integrated signal of relatively large groundwater capture areas. In contrast to the point-specific nature of monitoring wells, gaining streams coalesce multiple flow paths. Impacts on groundwater quality from unconventional gas development may be evaluated at the watershed scale by the sampling of dissolved methane (CH4 ) along such streams. This paper describes a method for using stream CH4 concentrations, along with measurements of groundwater inflow and gas transfer velocity interpreted by 1-D stream transport modeling, to determine groundwater methane fluxes. While dissolved ionic tracers remain in the stream for long distances, the persistence of methane is not well documented. To test this method and evaluate CH4 persistence in a stream, a combined bromide (Br) and CH4 tracer injection was conducted on Nine-Mile Creek, a gaining stream in a gas development area in central Utah. A 35% gain in streamflow was determined from dilution of the Br tracer. The injected CH4 resulted in a fivefold increase in stream CH4 immediately below the injection site. CH4 and δ(13) CCH4 sampling showed it was not immediately lost to the atmosphere, but remained in the stream for more than 2000 m. A 1-D stream transport model simulating the decline in CH4 yielded an apparent gas transfer velocity of 4.5 m/d, describing the rate of loss to the atmosphere (possibly including some microbial consumption). The transport model was then calibrated to background stream CH4 in Nine-Mile Creek (prior to CH4 injection) in order to evaluate groundwater CH4 contributions. The total estimated CH4 load discharging to the stream along the study reach was 190 g/d, although using geochemical fingerprinting to determine its source was beyond the scope of the current study. This demonstrates the utility of stream-gas sampling as a reconnaissance tool for evaluating both natural and anthropogenic CH4 leakage from gas reservoirs into groundwater and surface water. Published 2013. This article is a U.S. Government work and is in the public domain in the USA.

The Global Methane Budget 2000-2012

NASA Technical Reports Server (NTRS)

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

Development of the Vista Methane Emissions Inventory for Southern California: A GIS-Based Approach for Mapping Methane Emissions

NASA Astrophysics Data System (ADS)

Carranza, V.; Frausto-Vicencio, I.; Rafiq, T.; Verhulst, K. R.; Hopkins, F. M.; Rao, P.; Duren, R. M.; Miller, C. E.

2016-12-01

Atmospheric methane (CH4) is the second most prevalent anthropogenic greenhouse gas. Improved estimates of CH4 emissions from cities is essential for carbon cycle science and climate mitigation efforts. Development of spatially-resolved carbon emissions data sets may offer significant advances in understanding and managing carbon emissions from cities. Urban CH4 emissions in particular require spatially resolved emission maps to help resolve uncertainties in the CH4 budget. This study presents a Geographic Information System (GIS)-based approach to mapping CH4 emissions using locations of infrastructure known to handle and emit methane. We constrain the spatial distribution of sources to the facility level for the major CH4 emitting sources in the South Coast Air Basin. GIS spatial modeling was combined with publicly available datasets to determine the distribution of potential CH4 sources. The datasets were processed and validated to ensure accuracy in the location of individual sources. This information was then used to develop the Vista emissions prior, which is a one-year long, spatially-resolved CH4 emissions estimate. Methane emissions were calculated and spatially allocated to produce 1 km x 1 km gridded CH4 emission map spanning the Los Angeles Basin. In future work, the Vista CH4 emissions prior will be compared with existing, coarser-resolution emissions estimates and will be evaluated in inverse modeling studies using atmospheric observations. The Vista CH4 emissions inventory presents the first detailed spatial maps of CH4 sources and emissions estimates in the Los Angeles Basin and is a critical step towards sectoral attribution of CH4 emissions at local to regional scales.

An empirical equation with tables of smoothed solubilities of methane in water and aqueous sodium chloride solutions up to 25 weight percent, 360 degrees C, and 138 MPa

USGS Publications Warehouse

Haas, John L.

1978-01-01

The total pressure for the system H2O-CH 4 is given by p(total) = P(H2O,t) + exp10[log x(CH 4) - a - b x(CH4)], where P(H2O,t) is the vapor pressure of H2O liquid at the temperature t (?C) and x(CH 4) is the molal concentration of methane in the solution. The terms a and b are functions of temperature only. Where the total pressure and temperature are known, the concentration of methane, x(CH4), is found by iteration. The concentration of methane in a sodium chloride brine, y(CH4), is estimated using the function log y(CH4) = log x(CH4) - A I, where A is the salting out constant and I is the ionic strength. For sodium chloride solutions, the ionic strength is equal to the molality of the salt. The equations are valid to 360?C, 138 MPa, and 25 weight percent sodium chloride.

Experimental study and detailed modeling of toluene degradation in a low-pressure stoichiometric premixed CH4/O2/N2 flame.

PubMed

Bakali, A El; Dupont, L; Lefort, B; Lamoureux, N; Pauwels, J F; Montero, M

2007-05-17

Temperature and mole fraction profiles have been measured in laminar stoichiometric premixed CH4/O2/N2 and CH4/1.5%C6H5CH3/O2/N2 flames at low pressure (0.0519 bar) by using thermocouple, molecular beam/mass spectrometry (MB/MS), and gas chromatography/mass spectrometry (GC/MS) techniques. The present study completes our previous work performed on the thermal degradation of benzene in CH4/O2/N2 operating at similar conditions. Mole fraction profiles of reactants, final products, and reactive and stable intermediate species have been analyzed. The main intermediate aromatic species analyzed in the methane-toluene flame were benzene, phenol, ethylbenzene, benzylalcohol, styrene, and benzaldehyde. These new experimental results have been modeled with our previous model including submechanisms for aromatics (benzene up to p-xylene) and aliphatic (C1 up to C7) oxidation. Good agreement has been observed for the main species analyzed. The main reaction paths governing the degradation of toluene in the methane flame were identified, and it occurs mainly via the formation of benzene (C6H5CH3 + H = C6H6 + CH3) and benzyl radical (C6H5CH3 + H = C6H5CH2 + H2). Due to the abundance of methyl radicals, it was observed that recombination of benzyl and methyl is responsible for main monosubstitute aromatic species analyzed in the methane-toluene flame. The oxidation of these substitute species led to cyclopentadienyl radical as observed in a methane-benzene flame.

Spectroscopic line parameters of 12CH4 for atmospheric composition retrievals in the 4300-4500 cm-1 region

NASA Astrophysics Data System (ADS)

Hashemi, R.; Predoi-Cross, A.; Nikitin, A. V.; Tyuterev, Vl. G.; Sung, K.; Smith, M. A. H.; Malathy Devi, V.

2017-01-01

Due to the importance of methane as a trace atmospheric gas and a greenhouse gas, we have carried out a precise line-shape study to obtain the CH4-CH4 and CH4-air half-width coefficients, CH4-CH4 and CH4-air shift coefficients and off-diagonal relaxation matrix element coefficients for methane transitions in the spectral range known as the "methane Octad". In addition, the associated temperature dependences of these coefficients have been measured in the 4300-4500 cm-1 region of the Octad. The high signal to noise ratio spectra of pure methane and of dilute mixtures of methane in dry air with high resolution have been recorded at temperatures from 148 K to room temperature using the Bruker IFS 125 HR Fourier transform spectrometer (FTS) at the Jet Propulsion Laboratory, Pasadena, California. The analysis of spectra was done using a multispectrum non-linear least-squares curve fitting technique. Theoretical calculations have been performed and the results are compared with the previously published line positions, intensities and with the line parameters available in the GEISA and HITRAN2012 databases.

Estimating Landfill Methane Oxidation Using the Information of CO2/CH4 Fluxes Measured By the Eddy Covariance Method

NASA Astrophysics Data System (ADS)

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

2016-12-01

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 the landfill methane oxidation fraction when the anaerobic CO2/CH4 production ratio is known. 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 with eddy covariance CO2 and CH4 emission rates at Bluff Road Landfill in Lincoln Nebraska. It predicted zero oxidation rate in the northern portion of this landfill where a membrane and vents were present. The zero oxidation rate was expected because there would be little opportunity for methane to encounter oxidizing conditions before leaving the vents. We also applied the model at the Turkey Run Landfill in Georgia to estimate the CH4 oxidation rate over a one year period. In contrast to Bluff Road Landfill, the Turkey Run Landfill did not have a membrane or vents. Instead, methane produced in the landfill had to diffuse through a 0.5 m soil cap before release to the atmosphere. We observed evidence for methane oxidation ranging from about 18% to above 60% depending upon the age of deposited waste material. The model will be briefly described, and results from the two contrasting landfills will be discussed in this presentation.

Isotopic identification of the source of methane in subsurface sediments of an area surrounded by waste disposal facilities

USGS Publications Warehouse

Hackley, Keith C.; Liu, Chao-Li; Trainor, D.

1999-01-01

The major source of methane (CH4) in subsurface sediments on the property of a former hazardous waste treatment facility was determined using isotopic analyses measured on CH4 and associated groundwater. The site, located on an earthen pier built into a shallow wetland lake, has had a history of waste disposal practices and is surrounded by landfills and other waste management facilities. Concentrations of CH4 up to 70% were found in the headspace gases of several piezometers screened at 3 different depths (ranging from 8 to 17 m) in lacustrine and glacial till deposits. Possible sources of the CH4 included a nearby landfill, organic wastes from previous impoundments and microbial gas derived from natural organic matter in the sediments. Isotopic analyses included ??13C, ??D, 14C, and 3H on select CH4 samples and ??D and ??18O on groundwater samples. Methane from the deepest glacial till and intermediate lacustrine deposits had ??13C values from -79 to -82???, typical of natural 'drift gas' generated by microbial CO2-reduction. The CH4 from the shallow lacustrine deposits had ??13C values from -63 to -76???, interpreted as a mixture between CH4 generated by microbial fermentation and the CO2-reduction processes within the subsurface sediments. The ??D values of all the CH4 samples were quite negative ranging from -272 to -299???. Groundwater sampled from the deeper zones also showed quite negative ??D values that explained the light ??D observed for the CH4. Radiocarbon analyses of the CH4 showed decreasing 14C activity with depth, from a high of 58 pMC in the shallow sediments to 2 pMC in the deeper glacial till. The isotopic data indicated the majority of CH4 detected in the fill deposits of this site was microbial CH4 generated from naturally buried organic matter within the subsurface sediments. However, the isotopic data of CH4 from the shallow piezometers was more variable and the possibility of some mixing with oxidized landfill CH4 could not be completely ruled out.

Top-down methane emissions estimates for the San Francisco Bay Area from 1990 to 2012

DOE PAGES

Fairley, David; Fischer, Marc L.

2015-01-30

Methane is a potent greenhouse gas (GHG) that is now included in both California State and San Francisco Bay Area (SFBA) bottom-up emission inventories as part of California's effort to reduce anthropogenic GHG emissions. Here we provide a top-down estimate of methane (CH 4) emissions from the SFBA by combining atmospheric measurements with the comparatively better estimated emission inventory for carbon monoxide (CO). Local enhancements of CH 4 and CO are estimated using measurements from 14 air quality sites in the SFBA combined together with global background measurements. Mean annual CH 4 emissions are estimated from the product of Baymore » Area Air Quality Management District (BAAQMD) emission inventory CO and the slope of ambient local CH 4 to CO. The resulting top-down estimates of CH 4 emissions are found to decrease slightly from 1990 to 2012, with a mean value of 240 ± 60 GgCH 4 yr⁻¹ (at 95% confidence) in the most recent (2009–2012) period, and correspond to reasonably a constant factor of 1.5–2.0 (at 95% confidence) times larger than the BAAQMD CH 4 emission inventory. However, we note that uncertainty in these emission estimates is dominated by the variation in CH 4:CO enhancement ratios across the observing sites and we expect the estimates could represent a lower-limit on CH 4 emissions because BAAQMD monitoring sites focus on urban air quality and may be biased toward CO rather than CH 4 sources.« less

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

NASA Astrophysics Data System (ADS)

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.

Year-round simulated methane emissions from a permafrost ecosystem in Northeast Siberia

NASA Astrophysics Data System (ADS)

Castro-Morales, Karel; Kleinen, Thomas; Kaiser, Sonja; Zaehle, Sönke; Kittler, Fanny; Kwon, Min Jung; Beer, Christian; Göckede, Mathias

2018-05-01

Wetlands of northern high latitudes are ecosystems highly vulnerable to climate change. Some degradation effects include soil hydrologic changes due to permafrost thaw, formation of deeper active layers, and rising topsoil temperatures that accelerate the degradation of permafrost carbon and increase in CO2 and CH4 emissions. In this work we present 2 years of modeled year-round CH4 emissions into the atmosphere from a Northeast Siberian region in the Russian Far East. We use a revisited version of the process-based JSBACH-methane model that includes four CH4 transport pathways: plant-mediated transport, ebullition and molecular diffusion in the presence or absence of snow. The gas is emitted through wetlands represented by grid cell inundated areas simulated with a TOPMODEL approach. The magnitude of the summertime modeled CH4 emissions is comparable to ground-based CH4 fluxes measured with the eddy covariance technique and flux chambers in the same area of study, whereas wintertime modeled values are underestimated by 1 order of magnitude. In an annual balance, the most important mechanism for transport of methane into the atmosphere is through plants (61 %). This is followed by ebullition ( ˜ 35 %), while summertime molecular diffusion is negligible (0.02 %) compared to the diffusion through the snow during winter ( ˜ 4 %). We investigate the relationship between temporal changes in the CH4 fluxes, soil temperature, and soil moisture content. Our results highlight the heterogeneity in CH4 emissions at landscape scale and suggest that further improvements to the representation of large-scale hydrological conditions in the model will facilitate a more process-oriented land surface scheme and better simulate CH4 emissions under climate change. This is especially necessary at regional scales in Arctic ecosystems influenced by permafrost thaw.

Infrared Spectra and Optical Constants of Elusive Amorphous Methane

NASA Technical Reports Server (NTRS)

Gerakines, Perry A.; Hudson, Reggie L.

2015-01-01

New and accurate laboratory results are reported for amorphous methane (CH4) ice near 10 K for the study of the interstellar medium (ISM) and the outer Solar System. Near- and mid-infrared (IR) data, including spectra, band strengths, absorption coefficients, and optical constants, are presented for the first time for this seldom-studied amorphous solid. The apparent IR band strength near 1300 cm(exp -1) (7.69 micrometer) for amorphous CH4 is found to be about 33% higher than the value long used by IR astronomers to convert spectral observations of interstellar CH4 into CH4 abundances. Although CH4 is most likely to be found in an amorphous phase in the ISM, a comparison of results from various laboratory groups shows that the earlier CH4 band strength at 1300 cm(exp -1) (7.69 micrometer) was derived from IR spectra of ices that were either partially or entirely crystalline CH4 Applications of the new amorphous-CH4 results are discussed, and all optical constants are made available in electronic form.

Mapping the Methane and Aerosol Distributions within Titan's Troposphere: Complementing The Cassini/VIMS T90 Flyby of Titan

NASA Astrophysics Data System (ADS)

Young, Eliot

2012-10-01

Titan's atmosphere is mainly nitrogen gas with several trace constituents, including methane at the few percent level. The presence of methane has been a puzzle for decades, since the CH4 in Titan's atmosphere is expected to be destroyed by UV photolysis in ten million years or so. The source of Titan's atmospheric methane continues to be a major question. We propose a set of three STIS image cubes with the G750M grating at 0.62, 0.72 and 0.89 |*|m methane bands. These bands probe altitudes from the surface to 70 km; unlike CH4 bands at 1.6 or 2.3 |*|m, these cubes will provide a 3-D picture of Titan's troposphere {below 40 km}. The Cassini/VIMS visible channel has not been useful for this purpose for two reasons: its spectral resolution {about R=100} is coarse and its inconsistent background subtraction scheme that can lead to "stripes." HST/STIS resolves Titan's 1" disk into over 80 spatially resolved spectra, each with a spectral resolution greater than R=5000. STIS is a unique tool for mapping the 3-D distributions of CH4 and aerosols in Titan's troposphere.We request observations within a day of the Cassini flyby of Titan on April 5, 2013 around 21:40 UT in order to combine Cassini/VIMS and STIS mage cubes. Together, the visible {STIS} and IR {VIMS} image cubes will probe altitudes from the surface to the stratosphere {several hundred km}. The proposed STIS image cubes will provide the best tropospheric map of CH4 to date, relevant to surface/atmospheric coupling of CH4, latitudinal inhomogeneity of CH4 or aerosols, or the presence of condensates at low altitudes.

Laser-based measurements of δ13 C and δ2 H methane isotope signatures: precisions competitive with mass spectrometry methods

NASA Astrophysics Data System (ADS)

Yacovitch, Tara; Shorter, Joanne; Nelson, David; Herndon, Scott; Agnese, Mike; McManus, Barry; Zahniser, Mark

2017-04-01

In order to understand how and why methane (CH4 ) concentrations change over time, it is necessary to understand their sources and sinks. Stable isotope measurements of 13 CH4 :12 CH4 and CH3 D:12 CH4 ratios constrain the inventory of these sinks and sources. Current measurements often depend on Isotope Ratio Mass Spectrometry (IRMS), which requires extensive sample preparation including cryogenic separation of methane from air and subsequent conversion to either CO2 or H2 . Here, we detail improvements to a direct-absorption laser spectrometer that enable fast and precise measurements of methane isotope ratios (δ13 C and δ2 H ) of ambient air samples, without such sample preparation. The measurement system consists of a laser-based direct absorption spectrometer configured with a sample manifold for measurement of discrete samples (as opposed to flow-through measurements). Samples are trapped in the instrument using a rapid sample switching technique that compares each flask sample against a monitor tank sample. This approach reduces instrument drift and results in excellent precision. Precisions of 0.054 o/oo for δ13 C and 1.4 o/oo for δ2 H have been achieved (Allan-Werle deviations). These results are obtained in 20 minutes using 4 replicate comparisons to a monitor tank.

A density functional theory study on the effect of zero-point energy corrections on the methanation profile on Fe(100).

PubMed

Govender, Ashriti; Ferré, Daniel Curulla; Niemantsverdriet, J W Hans

2012-04-23

The thermodynamics and kinetics of the surface hydrogenation of adsorbed atomic carbon to methane, following the reaction sequence C+4H(-->/<--)CH+3H(-->/<--)CH(2)+2H(-->/<--)CH(3)+H(-->/<--)CH(4), are studied on Fe(100) by means of density functional theory. An assessment is made on whether the adsorption energies and overall energy profile are affected when zero-point energy (ZPE) corrections are included. The C, CH and CH(2) species are most stable at the fourfold hollow site, while CH(3) prefers the twofold bridge site. Atomic hydrogen is adsorbed at both the twofold bridge and fourfold hollow sites. Methane is physisorbed on the surface and shows neither orientation nor site preference. It is easily desorbed to the gas phase once formed. The incorporation of ZPE corrections has a very slight, if any, effect on the adsorption energies and does not alter the trends with regards to the most stable adsorption sites. The successive addition of hydrogen to atomic carbon is endothermic up to the addition of the third hydrogen atom resulting in the methyl species, but exothermic in the final hydrogenation step, which leads to methane. The overall methanation reaction is endothermic when starting from atomic carbon and hydrogen on the surface. Zero-point energy corrections are rarely provided in the literature. Since they are derived from C-H bonds with characteristic vibrations on the order of 2500-3000 cm(-1), the equivalent ZPE of 1/2 hν is on the order of 0.2-0.3 eV and its effect on adsorption energy can in principle be significant. Particularly in reactions between CH(x) and H, the ZPE correction is expected to be significant, as additional C-H bonds are formed. In this instance, the methanation reaction energy of +0.77 eV increased to +1.45 eV with the inclusion of ZPE corrections, that is, less favourable. Therefore, it is crucial to include ZPE corrections when reporting reactions involving hydrogen-containing species. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

First records of a field experiment on fertilizer effects on methane emission from rice fields in Hunan-Province (PR China)

NASA Astrophysics Data System (ADS)

Wassmann, R.; Wang, M. X.; Shangguan, X. J.; Xie, X. L.; Shen, R. X.; Wang, Y. S.; Papen, H.; Rennenberg, H.; Seiler, W.

Fertilizer effects on methane emission from Chinese rice fields were investigated by a praxis-oriented approach applying balanced amendments of N, P and K. The data set obtained covered the emission rates of app. one month in early rice and one month in late rice 1991. An intercomparison between the 4 treatments showed pronounced differences in the magnitudes of methane emission rates. The combined organic/mineral fertilizer application, commonly used as local farming practice, resulted in relatively high seasonal averages of methane emission rates (26.5 mg CH4 m-2 h-1 in early rice and 50.1 mg CH4 m-2 h-1 in late rice). The lowest emission rates were observed in the plot with pure mineral fertilization (6.5 mg CH4 m-2 h-1 in early rice and 14.3 mg CH4 m-2 h-1 in late rice). Pure organic fertilizers by unfermented substances yielded the highest methane emission rates of all field trials (38.6 mg CH4 m-2 h-1 in early rice and 56.2 CH4 m-2 h-1 in late rice). The fertilization with fermented material derived from biogas generators resulted in substantially lower emission rates than the other trials with organic amendments, the seasonal averages corresponded to 15.9 mg CH4 m-2 h-1 (early rice) and 22.5 mg CH4 m-2 h-1 (late rice). Interpretation of the results can be obtained from the different potentials of these fertilizers for methane production. Based on this concept the different methane emission rates observed with organic/mineral, pure mineral and pure unfermented-organic fertilizers could directly be attributed to the different quantities of organic matter incorporated into the soil. The low methane emission from the plot treated with fermented material could be explained by a depletion of potential methane precursors resulting from the preceding fermentation. The results of this investigation provide evidence that the extensive use of specific chemical fertilizers and the application of sludge from the operation of biogas generators could lead to a net reduction of the methane emission from rice fields.

The effects of climate changes on soil methane oxidation in a dry Arctic tundra

NASA Astrophysics Data System (ADS)

D'Imperio, Ludovica

2014-05-01

The effects of climate changes on soil methane oxidation in a dry Arctic tundra. Ludovica D'Imperio1, Anders Michelsen1, Christian J. Jørgensen1, Bo Elberling1 1Center for Permafrost (CENPERM), Department of Geosciences and Natural Resource Management, University of Copenhagen, Denmark At Northern latitudes climatic changes are predicted to be most pronounced resulting in increasing active layer depth and changes in growing season length, vegetation cover and nutrient cycling. As a consequence of increased temperature, large stocks of carbon stored in the permafrost-affected soils could become available for microbial transformations and under anoxic conditions result in increasing methane production affecting net methane (CH4) budget. Arctic tundra soils also serves as an important sink of atmospheric CH4 by microbial oxidation under aerobic conditions. While several process studies have documented the mechanisms behind both production and emissions of CH4 in arctic ecosystems, an important knowledge gap exists with respect to the in situ dynamics of microbial-driven uptake of CH4 in arctic dry lands which may be enhanced as a consequence of global warming and thereby counterbalancing CH4 emissions from Arctic wetlands. In-situ methane measurements were made in a dry Arctic tundra in Disko Island, Western Greenland, during the summer 2013 to assess the role of seasonal and inter-annual variations in temperatures and snow cover. The experimental set-up included snow fences installed in 2012, allowed investigations of the emissions of GHGs from soil under increased winter snow deposition and ambient field conditions. The soil fluxes of CH4 and CO2 were measured using closed chambers in manipulated plots with increased summer temperatures and shrub removal with or without increased winter precipitation. At the control plots, the averaged seasonal CH4 oxidation rates ranged between -0.05 mg CH4 m-2 hr-1 (end of August) and -0.32 mg CH4 m-2 hr-1 (end of June). In the plots with increased summer temperatures the rates ranged between -0.08 mg CH4 m-2 hr-1 (end of August) and -0.40 mg CH4 m-2 hr-1 (beginning of July). Preliminary results show a significant effect of increased winter precipitation (p<0.01) over the season as well as a significant warming effect (p<0.05) during July and August. These results suggest that in a warmer climate increasing CH4 uptake rates in dry Arctic soils could become an important factor for net CH4 budget.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moran, James J.; Whitmore, Laura M.; Jay, Zackary J.

Volcanism and post-magmatism contribute both significant annual CH 4 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 (δ 2H and δ 13C) of CH 4(g) sampled from ten high-temperature geothermal pools in Yellowstone National Parkmore » to show that the predominant flux of CH4(g) is abiotic. The average δ 13C and δ 2H values of CH 4(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 δ 13C CH4 and δ 13C-dissolved inorganic C (DIC) also suggests that CO 2 is a parent C source for the observed CH 4(g). Moreover, CH 4-CO 2 isotopic geothermometry was used to estimate CH 4(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.« less

Adding stable carbon isotopes improves model representation of the role of microbial communities in peatland methane cycling

DOE Office of Scientific and Technical Information (OSTI.GOV)

Deng, Jia; McCalley, Carmody K.; Frolking, Steve

Climate change is expected to have significant and uncertain impacts on methane (CH 4) emissions from northern peatlands. Biogeochemical models can extrapolate site-specific CH 4 measurements to larger scales and predict responses of CH 4 emissions to environmental changes. However, these models include considerable uncertainties and limitations in representing CH4 production, consumption, and transport processes. To improve predictions of CH 4 transformations, we incorporated acetate and stable carbon (C) isotopic dynamics associated with CH 4 cycling into a biogeochemistry model, DNDC. By including these new features, DNDC explicitly simulates acetate dynamics and the relative contribution of acetotrophic and hydrogenotrophic methanogenesismore » (AM and HM) to CH 4 production, and predicts the C isotopic signature (δ 13C) in soil C pools and emitted gases. When tested against biogeochemical and microbial community observations at two sites in a zone of thawing permafrost in a subarctic peatland in Sweden, the new formulation substantially improved agreement with CH 4 production pathways and δ 13C in emitted CH 4 (δ 13C-CH 4), a measure of the integrated effects of microbial production and consumption, and of physical transport. We also investigated the sensitivity of simulated δ 13C-CH 4 to C isotopic composition of substrates and, to fractionation factors for CH4 production (α AM and α HM), CH 4 oxidation (α MO), and plant-mediated CH 4 transport (α TP). The sensitivity analysis indicated that the δ13C-CH 4 is highly sensitive to the factors associated with microbial metabolism (α AM, α HM, and α MO). The model framework simulating stable C isotopic dynamics provides a robust basis for better constraining and testing microbial mechanisms in predicting CH 4 cycling in peatlands.« less

Adding stable carbon isotopes improves model representation of the role of microbial communities in peatland methane cycling

DOE PAGES

Deng, Jia; McCalley, Carmody K.; Frolking, Steve; ...

2017-06-13

Climate change is expected to have significant and uncertain impacts on methane (CH 4) emissions from northern peatlands. Biogeochemical models can extrapolate site-specific CH 4 measurements to larger scales and predict responses of CH 4 emissions to environmental changes. However, these models include considerable uncertainties and limitations in representing CH4 production, consumption, and transport processes. To improve predictions of CH 4 transformations, we incorporated acetate and stable carbon (C) isotopic dynamics associated with CH 4 cycling into a biogeochemistry model, DNDC. By including these new features, DNDC explicitly simulates acetate dynamics and the relative contribution of acetotrophic and hydrogenotrophic methanogenesismore » (AM and HM) to CH 4 production, and predicts the C isotopic signature (δ 13C) in soil C pools and emitted gases. When tested against biogeochemical and microbial community observations at two sites in a zone of thawing permafrost in a subarctic peatland in Sweden, the new formulation substantially improved agreement with CH 4 production pathways and δ 13C in emitted CH 4 (δ 13C-CH 4), a measure of the integrated effects of microbial production and consumption, and of physical transport. We also investigated the sensitivity of simulated δ 13C-CH 4 to C isotopic composition of substrates and, to fractionation factors for CH4 production (α AM and α HM), CH 4 oxidation (α MO), and plant-mediated CH 4 transport (α TP). The sensitivity analysis indicated that the δ13C-CH 4 is highly sensitive to the factors associated with microbial metabolism (α AM, α HM, and α MO). The model framework simulating stable C isotopic dynamics provides a robust basis for better constraining and testing microbial mechanisms in predicting CH 4 cycling in peatlands.« less

Atmospheric methane over Siberia: measurements from the 2014 YAK-AEROSIB aircraft campaign

NASA Astrophysics Data System (ADS)

Paris, Jean-Daniel; Pisso, Ignacio; Ancellet, Gérard; Law, Kathy; Arshinov, Mikhail Yu.; Belan, Boris D.; Nédélec, Philippe; Myhre, Cathrine Lund

2017-04-01

The YAK-AEROSIB program collects high-precision in-situ measurements of the vertical distribution of CO2, CH4, CO, O3, black carbon and ultrafine particles distribution in the Siberian troposphere, as well as other parameters including aerosol lidar profiles, on a pan-Siberian aircraft transect. Recent efforts aim at better understanding the respective role of CH4 emission processes in driving its large scale atmospheric variability over the region. The October 2014 YAK-AEROSIB/MOCA campaign from Novosibirsk to Salekhard and over the Kara sea and the Yamal peninsula sampled air masses affected by local, regional and remote pollution. We analyse the contribution of local anthropogenic sources to measured CH4 enhancements, in relation to atmospheric mixing and transport conditions. Our analysis also attempts to detect CH4 signal from sources of methane in the Siberian shelf and the Arctic ocean during low level flight legs over the Kara sea using the airborne measurements and a Lagrangian model coupled to potential CH4 hydrate and geological sources. The measured CH4 concentrations do not contradict a potential source upstream of our measurements, but the interpretation is challenging due to a very low CH4 signal. The challenging question of the methane budget and its evolution in Siberia leads to a need for new approaches. A new generation of airborne measurements, more flexible, is now needed.

Characterization of methane emissions in Los Angeles with airborne hyperspectral imaging

NASA Astrophysics Data System (ADS)

Saad, K.; Tratt, D. M.; Buckland, K. N.; Roehl, C. M.; Wennberg, P. O.; Wunch, D.

2017-12-01

As urban areas develop regulations to limit atmospheric methane (CH4), accurate quantification of anthropogenic emissions will be critical for program development and evaluation. However, relating emissions derived from process-level metadata to those determined from assimilating atmospheric observations of CH4 concentrations into models is particularly difficult. Non-methane hydrocarbons (NMHCs) can help differentiate between thermogenic and biogenic CH4 emissions, as they are primarily co-emitted with the former; however, these trace gases are subject to the same limitations as CH4. Remotely-sensed hyperspectral imaging bridges these approaches by measuring emissions plumes directly with spatial coverage on the order of 10 km2 min-1. We identify the sources of and evaluate emissions plumes measured by airborne infrared hyperspectral imagers flown over the Los Angeles (LA) metropolitan area, which encompasses various CH4 sources, including petroleum and natural gas wells and facilities. We quantify total CH4 and NMHC emissions, as well as their relative column densities, at the point-source level to create fingerprints of source types. We aggregate these analyses to estimate the range of variability in chemical composition across source types. These CH4 and NMHC emissions factors are additionally compared to their tropospheric column abundances measured by the Total Carbon Column Observing Network (TCCON) Pasadena Fourier transform infrared spectrometer, which provides a footprint for the LA basin.

The origin, source, and cycling of methane in deep crystalline rock biosphere.

PubMed

Kietäväinen, Riikka; Purkamo, Lotta

2015-01-01

The emerging interest in using stable bedrock formations for industrial purposes, e.g., nuclear waste disposal, has increased the need for understanding microbiological and geochemical processes in deep crystalline rock environments, including the carbon cycle. Considering the origin and evolution of life on Earth, these environments may also serve as windows to the past. Various geological, chemical, and biological processes can influence the deep carbon cycle. Conditions of CH4 formation, available substrates and time scales can be drastically different from surface environments. This paper reviews the origin, source, and cycling of methane in deep terrestrial crystalline bedrock with an emphasis on microbiology. In addition to potential formation pathways of CH4, microbial consumption of CH4 is also discussed. Recent studies on the origin of CH4 in continental bedrock environments have shown that the traditional separation of biotic and abiotic CH4 by the isotopic composition can be misleading in substrate-limited environments, such as the deep crystalline bedrock. Despite of similarities between Precambrian continental sites in Fennoscandia, South Africa and North America, where deep methane cycling has been studied, common physicochemical properties which could explain the variation in the amount of CH4 and presence or absence of CH4 cycling microbes were not found. However, based on their preferred carbon metabolism, methanogenic microbes appeared to have similar spatial distribution among the different sites.

The origin, source, and cycling of methane in deep crystalline rock biosphere

PubMed Central

Kietäväinen, Riikka; Purkamo, Lotta

2015-01-01

The emerging interest in using stable bedrock formations for industrial purposes, e.g., nuclear waste disposal, has increased the need for understanding microbiological and geochemical processes in deep crystalline rock environments, including the carbon cycle. Considering the origin and evolution of life on Earth, these environments may also serve as windows to the past. Various geological, chemical, and biological processes can influence the deep carbon cycle. Conditions of CH4 formation, available substrates and time scales can be drastically different from surface environments. This paper reviews the origin, source, and cycling of methane in deep terrestrial crystalline bedrock with an emphasis on microbiology. In addition to potential formation pathways of CH4, microbial consumption of CH4 is also discussed. Recent studies on the origin of CH4 in continental bedrock environments have shown that the traditional separation of biotic and abiotic CH4 by the isotopic composition can be misleading in substrate-limited environments, such as the deep crystalline bedrock. Despite of similarities between Precambrian continental sites in Fennoscandia, South Africa and North America, where deep methane cycling has been studied, common physicochemical properties which could explain the variation in the amount of CH4 and presence or absence of CH4 cycling microbes were not found. However, based on their preferred carbon metabolism, methanogenic microbes appeared to have similar spatial distribution among the different sites. PMID:26236303

Estimating wetland methane emissions from the northern high latitudes from 1990 to 2009 using artificial neural networks

NASA Astrophysics Data System (ADS)

Zhu, Xudong; Zhuang, Qianlai; Qin, Zhangcai; Glagolev, Mikhail; Song, Lulu

2013-04-01

Methane (CH4) emissions from wetland ecosystems in nothern high latitudes provide a potentially positive feedback to global climate warming. Large uncertainties still remain in estimating wetland CH4 emisions at regional scales. Here we develop a statistical model of CH4 emissions using an artificial neural network (ANN) approach and field observations of CH4 fluxes. Six explanatory variables (air temperature, precipitation, water table depth, soil organic carbon, soil total porosity, and soil pH) are included in the development of ANN models, which are then extrapolated to the northern high latitudes to estimate monthly CH4 emissions from 1990 to 2009. We estimate that the annual wetland CH4 source from the northern high latitudes (north of 45°N) is 48.7 Tg CH4 yr-1 (1 Tg = 1012 g) with an uncertainty range of 44.0 53.7 Tg CH4 yr-1. The estimated wetland CH4 emissions show a large spatial variability over the northern high latitudes, due to variations in hydrology, climate, and soil conditions. Significant interannual and seasonal variations of wetland CH4 emissions exist in the past 2 decades, and the emissions in this period are most sensitive to variations in water table position. To improve future assessment of wetland CH4 dynamics in this region, research priorities should be directed to better characterizing hydrological processes of wetlands, including temporal dynamics of water table position and spatial dynamics of wetland areas.

The C-13/C-12 kinetic isotope effect for soil oxidation of methane at ambient atmospheric concentrations

NASA Technical Reports Server (NTRS)

King, Stagg L.; Quay, Paul D.; Lansdown, John M.

1989-01-01

During a survey of the Alaskan North Slope to estimate the isotopic composition and fluxes of methane (CH4) from the tundra, two sites were encountered that showed net methane consumption within flux chambers. Methane concentrations decreased from ambient (1.78 ppmv) by up to 50 percent, and the delta C-13 increased by up to 10 percent in the two chamber deployments showing CH4 consumption. CH4 consumption rates were measured to be 1.2 and 0.6 mg CH4/sq m per day; the corresponding carbon kinetic isotope effects (k13/k12) were 0.974 and 0.984, respectively.

Factors affecting methane production and mitigation in ruminants.

PubMed

Shibata, Masaki; Terada, Fuminori

2010-02-01

Methane (CH(4)) is the second most important greenhouse gas (GHG) and that emitted from enteric fermentation in livestock is the single largest source of emissions in Japan. Many factors influence ruminant CH(4) production, including level of intake, type and quality of feeds and environmental temperature. The objectives of this review are to identify the factors affecting CH(4) production in ruminants, to examine technologies for the mitigation of CH(4) emissions from ruminants, and to identify areas requiring further research. The following equation for CH(4) prediction was formulated using only dry matter intake (DMI) and has been adopted in Japan to estimate emissions from ruminant livestock for the National GHG Inventory Report: Y = -17.766 + 42.793X - 0.849X(2), where Y is CH(4) production (L/day) and X is DMI (kg/day). Technologies for the mitigation of CH(4) emissions from ruminants include increasing productivity by improving nutritional management, the manipulation of ruminal fermentation by changing feed composition, the addition of CH(4) inhibitors, and defaunation. Considering the importance of ruminant livestock, it is essential to establish economically feasible ways of reducing ruminant CH(4) production while improving productivity; it is therefore critical to conduct a full system analysis to select the best combination of approaches or new technologies to be applied under long-term field conditions.

Understanding the glacial methane cycle

NASA Astrophysics Data System (ADS)

Hopcroft, Peter O.; Valdes, Paul J.; O'Connor, Fiona M.; Kaplan, Jed O.; Beerling, David J.

2017-02-01

Atmospheric methane (CH4) varied with climate during the Quaternary, rising from a concentration of 375 p.p.b.v. during the last glacial maximum (LGM) 21,000 years ago, to 680 p.p.b.v. at the beginning of the industrial revolution. However, the causes of this increase remain unclear; proposed hypotheses rely on fluctuations in either the magnitude of CH4 sources or CH4 atmospheric lifetime, or both. Here we use an Earth System model to provide a comprehensive assessment of these competing hypotheses, including estimates of uncertainty. We show that in this model, the global LGM CH4 source was reduced by 28-46%, and the lifetime increased by 2-8%, with a best-estimate LGM CH4 concentration of 463-480 p.p.b.v. Simulating the observed LGM concentration requires a 46-49% reduction in sources, indicating that we cannot reconcile the observed amplitude. This highlights the need for better understanding of the effects of low CO2 and cooler climate on wetlands and other natural CH4 sources.

Origin of methane-rich natural gas at the West Pacific convergent plate boundary.

PubMed

Sano, Yuji; Kinoshita, Naoya; Kagoshima, Takanori; Takahata, Naoto; Sakata, Susumu; Toki, Tomohiro; Kawagucci, Shinsuke; Waseda, Amane; Lan, Tefang; Wen, Hsinyi; Chen, Ai-Ti; Lee, Hsiaofen; Yang, Tsanyao F; Zheng, Guodong; Tomonaga, Yama; Roulleau, Emilie; Pinti, Daniele L

2017-11-15

Methane emission from the geosphere is generally characterized by a radiocarbon-free signature and might preserve information on the deep carbon cycle on Earth. Here we report a clear relationship between the origin of methane-rich natural gases and the geodynamic setting of the West Pacific convergent plate boundary. Natural gases in the frontal arc basin (South Kanto gas fields, Northeast Japan) show a typical microbial signature with light carbon isotopes, high CH 4 /C 2 H 6 and CH 4 / 3 He ratios. In the Akita-Niigata region - which corresponds to the slope stretching from the volcanic-arc to the back-arc -a thermogenic signature characterize the gases, with prevalence of heavy carbon isotopes, low CH 4 /C 2 H 6 and CH 4 / 3 He ratios. Natural gases from mud volcanoes in South Taiwan at the collision zone show heavy carbon isotopes, middle CH 4 /C 2 H 6 ratios and low CH 4 / 3 He ratios. On the other hand, those from the Tokara Islands situated on the volcanic front of Southwest Japan show the heaviest carbon isotopes, middle CH 4 /C 2 H 6 ratios and the lowest CH 4 / 3 He ratios. The observed geochemical signatures of natural gases are clearly explained by a mixing of microbial, thermogenic and abiotic methane. An increasing contribution of abiotic methane towards more tectonically active regions of the plate boundary is suggested.

Interannual Variability and Trends of CH4, CO and OH Using the Computationally-Efficient CH4-CO-OH (ECCOH) Module

NASA Technical Reports Server (NTRS)

Elshorbany, Yasin F.; Duncan, Bryan N.; Strode, Sarah A.; Wang, James S.; Kouatchou, Jules

2015-01-01

Methane (CH4) is the second most important anthropogenic greenhouse gas (GHG). Its 100-year global warming potential (GWP) is 34 times larger than that for carbon dioxide. The 100-year integrated GWPof CH4 is sensitive to changes in hydroxyl radical (OH) levels.Oxidation of CH4 and carbon monoxide (CO) by OH is the main loss process, thus affecting the oxidizing capacity of the atmosphere and contributing to the global ozone background. Limitations of using archived, monthly OH fields for studies of methane's and COs evolution are that feedbacks of the CH4-CO-OH system on methane, CO and OH are not captured. In this study, we employ the computationally Efficient CH4-CO-OH (ECCOH) module (Elshorbany et al., 2015) to investigate the nonlinear feedbacks of the CH4-CO-OH system on the interannual variability and trends of the CH4, CO, OH system.

A unified equation for calculating methane vapor pressures in the CH4-H2O system with measured Raman shifts

USGS Publications Warehouse

Lu, W.; Chou, I.-Ming; Burruss, R.C.; Song, Y.

2007-01-01

A unified equation has been derived by using all available data for calculating methane vapor pressures with measured Raman shifts of C-H symmetric stretching band (??1) in the vapor phase of sample fluids near room temperature. This equation eliminates discrepancies among the existing data sets and can be applied at any Raman laboratory. Raman shifts of C-H symmetric stretching band of methane in the vapor phase of CH4-H2O mixtures prepared in a high-pressure optical cell were also measured at temperatures between room temperature and 200 ??C, and pressures up to 37 MPa. The results show that the CH4 ??1 band position shifts to higher wavenumber as temperature increases. We also demonstrated that this Raman band shift is a simple function of methane vapor density, and, therefore, when combined with equation of state of methane, methane vapor pressures in the sample fluids at elevated temperatures can be calculated from measured Raman peak positions. This method can be applied to determine the pressure of CH4-bearing systems, such as methane-rich fluid inclusions from sedimentary basins or experimental fluids in hydrothermal diamond-anvil cell or other types of optical cell. ?? 2007 Elsevier Ltd. All rights reserved.

Isotopic Ratios in Titan's Methane: Measurements and Modeling

NASA Technical Reports Server (NTRS)

Nixon, C. A.; Temelso, B.; Vinatier, S.; Teanby, N. A.; Bezard, B.; Achterberg, R. K.; Mandt, K. E.; Sherrill, C. D.; Irwin, P. G.; Jennings, D. E.;

Diurnal variation of methane emissions from an alpine wetland on the eastern edge of Qinghai-Tibetan Plateau.

PubMed

Chen, Huai; Wu, Ning; Yao, Shouping; Gao, Yongheng; Wang, Yanfen; Tian, Jianqing; Yuan, Xingzhong

2010-05-01

Alpine wetland is a source for CH(4), but little is known about methane emission from such wetland, especially about its diurnal pattern. In this study we tried to probe the diurnal variation in methane emission from alpine wetland vegetation. The average methane emission rate was 9.6 +/- 3.4 mg CH(4) m(-2) h(-1). There was an apparent diurnal variation pattern in methane emission with one minor peak at 06:00 and a major one at 15:00. The sunrise peak was consistent with a two-way transport mechanism for plants (convective at daytime and diffusive at night-time). CH(4) emission was found significantly correlated with redox potentials. The afternoon peak could not be explained by diurnal variation in soil temperature, but could be attributable to changes in CH(4) oxidation and production driven by plant gas transport mechanism. The results have important implications for sampling and scaling strategies for estimating methane emission from alpine wetlands.

Bayesian Analysis of the Glacial-Interglacial Methane Increase Constrained by Stable Isotopes and Earth System Modeling

NASA Astrophysics Data System (ADS)

Hopcroft, Peter O.; Valdes, Paul J.; Kaplan, Jed O.

2018-04-01

The observed rise in atmospheric methane (CH4) from 375 ppbv during the Last Glacial Maximum (LGM: 21,000 years ago) to 680 ppbv during the late preindustrial era is not well understood. Atmospheric chemistry considerations implicate an increase in CH4 sources, but process-based estimates fail to reproduce the required amplitude. CH4 stable isotopes provide complementary information that can help constrain the underlying causes of the increase. We combine Earth System model simulations of the late preindustrial and LGM CH4 cycles, including process-based estimates of the isotopic discrimination of vegetation, in a box model of atmospheric CH4 and its isotopes. Using a Bayesian approach, we show how model-based constraints and ice core observations may be combined in a consistent probabilistic framework. The resultant posterior distributions point to a strong reduction in wetland and other biogenic CH4 emissions during the LGM, with a modest increase in the geological source, or potentially natural or anthropogenic fires, accounting for the observed enrichment of δ13CH4.

Detecting Methane From Leaking Pipelines and as Greenhouse Gas in the Atmosphere

NASA Technical Reports Server (NTRS)

Riris, Haris; Numata, Kenji; Li, Steven; Wu, Stewart; Ramanathan, Anand; Dawsey, Martha

2012-01-01

Laser remote sensing measurements of trace gases from orbit can provide unprecedented information about important planetary science and answer critical questions about planetary atmospheres. Methane (CH4) is the second most important anthropogenically produced greenhouse gas. Though its atmospheric abundance is much less than that of CO2 (1.78 ppm vs. 380 ppm), it has much larger greenhouse heating potential. CH4 also contributes to pollution in the lower atmosphere through chemical reactions, leading to ozone production. Atmospheric CH4 concentrations have been increasing as a result of increased fossil fuel production, rice farming, livestock, and landfills. Natural sources of CH4 include wetlands, wild fires, and termites, and perhaps other unknown sources. Important sinks for CH4 include non-saturated soils and oxidation by hydroxyl radicals in the atmosphere. Remotely measuring CH4 and other biogenic molecules (such as ethane and formaldehyde) on Mars also has important implications on the existence of life on Mars. Measuring CH4 at very low (ppb) concentrations from orbit will dramatically improve the sensitivity and spatial resolution in the search for CH4 vents and sub-surface life on other planets. A capability has been developed using lasers and spectroscopic detection techniques for the remote measurements of trace gases in open paths. Detection of CH4, CO2, H2O, and CO in absorption cells and in open paths, both in the mid- IR and near-IR region, has been demonstrated using an Optical Parametric Amplifier laser transmitter developed at GSFC. With this transmitter, it would be possible to develop a remote sensing methane instrument. CH4 detection also has very important commercial applications. Pipeline leak detection from an aircraft or a helicopter can significantly reduce cost, response time, and pinpoint the location. The main advantage is the ability to rapidly detect CH4 leaks remotely. This is extremely important for the petrochemical industry. This capability can be used in manned or unmanned airborne platforms for the detection of leaks in pipelines and other areas of interest where a CH4 leak is suspected.

Climate-methane cycle feedback in global climate model model simulations forced by RCP scenarios

NASA Astrophysics Data System (ADS)

Eliseev, Alexey V.; Denisov, Sergey N.; Arzhanov, Maxim M.; Mokhov, Igor I.

2013-04-01

Methane cycle module of the global climate model of intermediate complexity developed at the A.M. Obukhov Institute of Atmospheric Physics, Russian Academy of Sciences (IAP RAS CM) is extended by coupling with a detailed module for thermal and hydrological processes in soil (Deep Soil Simulator, (Arzhanov et al., 2008)). This is an important improvement with respect with the earlier IAP RAS CM version (Eliseev et al., 2008) which has employed prescribed soil hydrology to simulate CH4 emissions from soil. Geographical distribution of water inundated soil in the model was also improved by replacing the older Olson's ecosystem data base by the data based on the SCIAMACHY retrievals (Bergamaschi et al., 2007). New version of the IAP RAS CM module for methane emissions from soil is validated by using the simulation protocol adopted in the WETCHIMP (Wetland and Wetland CH4 Inter-comparison of Models Project). In addition, atmospheric part of the IAP RAS CM methane cycle is extended by temperature dependence of the methane life-time in the atmosphere in order to mimic the respective dependence of the atmospheric methane chemistry (Denisov et al., 2012). The IAP RAS CM simulations are performed for the 18th-21st centuries according with the CMIP5 protocol taking into account natural and anthropogenic forcings. The new IAP RAS CM version realistically reproduces pre-industrial and present-day characteristics of the global methane cycle including CH4 concentration qCH4 in the atmosphere and CH4 emissions from soil. The latter amounts 150 - 160 TgCH4-yr for the late 20th century and increases to 170 - 230 TgCH4-yr in the late 21st century. Atmospheric methane concentration equals 3900 ppbv under the most aggressive anthropogenic scenario RCP 8.5 and 1850 - 1980 ppbv under more moderate scenarios RCP 6.0 and RCP 4.5. Under the least aggressive scenario RCP 2.6 qCH4 reaches maximum 1730 ppbv in 2020s and declines afterwards. Climate change impact on the methane emissions from soil enhances build up of the methane stock in the atmosphere by 10 - 25% depending on anthropogenic scenario and time instant. In turn, decrease of methane life-time in the atmosphere suppresses this build up by 5 - 40%. The net effect is uncertain but small in terms of resulting additional greenhouse radiative forcing. This smallness is reflected in small additional (relative to the model version with both methane emissions from soil and methane life-time in the atmosphere fixed at their preindustrial values) near-surface warming which globally is not larger than 1 K, i.e, ˜ 4% of warming exhibited by the model version neglecting climate-methane cycle interaction. References [1] M.M. Arzhanov, P.F. Demchenko, A.V. Eliseev, and I.I. Mokhov. Simulation of characteristics of thermal and hydrologic soil regimes in equilibrium numerical experiments with a climate model of intermediate complexity. Izvestiya, Atmos. Ocean. Phys., 44(5):279-287, 2008. doi: 10.1134/S0001433808050022. [2] P. Bergamaschi, C. Frankenberg, J.F. Meirink, M. Krol, F. Dentener, T. Wagner, U. Platt, J.O. Kaplan, S. Körner, M. Heimann, E.J. Dlugokencky, and A. Goede. Satellite chartography of atmospheric methane from SCIAMACHY on board ENVISAT: 2. Evaluation based on inverse model simulations. J. Geophys. Res., 112(D2):D02304, 2007. doi: 10.1029/2006JD007268. [3] S.N. Denisov, A.V. Eliseev, and I.I. Mokhov. Climate change in the IAP RAS global model with interactive methane cycle under RCP anthropogenic scenarios. Rus. Meteorol. Hydrol., 2012. [submitted]. [4] A.V. Eliseev, I.I. Mokhov, M.M. Arzhanov, P.F. Demchenko, and S.N. Denisov. Interaction of the methane cycle and processes in wetland ecosystems in a climate model of intermediate complexity. Izvestiya, Atmos. Ocean. Phys., 44(2):139-152, 2008. doi: 10.1134/S0001433808020011.

Geographic and seasonal variation of dissolved methane and aerobic methane oxidation in Alaskan lakes

DOE PAGES

Martinez-Cruz, K.; Sepulveda-Jauregui, A.; Walter Anthony, K.; ...

2015-08-04

Methanotrophic bacteria play an important role oxidizing a significant fraction of methane (CH 4) produced in lakes. Aerobic CH 4 oxidation depends mainly on lake CH 4 and oxygen (O 2) concentrations, in such a manner that higher MO rates are usually found at the oxic/anoxic interface, where both molecules are present. MO also depends on temperature, and via methanogenesis, on organic carbon input to lakes, including from thawing permafrost in thermokarst (thaw)-affected lakes. Given the large variability in these environmental factors, CH 4 oxidation is expected to be subject to large seasonal and geographic variations, which have been scarcelymore » reported in the literature. In the present study, we measured CH 4 oxidation rates in 30 Alaskan lakes along a north-south latitudinal transect during winter and summer with a new field laser spectroscopy method. Additionally, we measured dissolved CH 4 and O 2 concentrations. Here, we found that in the winter, aerobic CH 4 oxidation was mainly controlled by the dissolved O 2 concentration, while in the summer it was controlled primarily by the CH 4 concentration, which was scarce compared to dissolved O 2. The permafrost environment of the lakes was identified as another key factor. Thermokarst (thaw) lakes formed in yedoma-type permafrost had significantly higher CH 4 oxidation rates compared to other thermokarst and non-thermokarst lakes formed in non-yedoma permafrost environments. As thermokarst lakes formed in yedoma-type permafrost have been identified to receive large quantities of terrestrial organic carbon from thaw and subsidence of the surrounding landscape into the lake, confirming the strong coupling between terrestrial and aquatic habitats and its influence on CH 4 cycling.« less

Geographic and seasonal variation of dissolved methane and aerobic methane oxidation in Alaskan lakes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Martinez-Cruz, K.; Sepulveda-Jauregui, A.; Walter Anthony, K.

Methanotrophic bacteria play an important role oxidizing a significant fraction of methane (CH 4) produced in lakes. Aerobic CH 4 oxidation depends mainly on lake CH 4 and oxygen (O 2) concentrations, in such a manner that higher MO rates are usually found at the oxic/anoxic interface, where both molecules are present. MO also depends on temperature, and via methanogenesis, on organic carbon input to lakes, including from thawing permafrost in thermokarst (thaw)-affected lakes. Given the large variability in these environmental factors, CH 4 oxidation is expected to be subject to large seasonal and geographic variations, which have been scarcelymore » reported in the literature. In the present study, we measured CH 4 oxidation rates in 30 Alaskan lakes along a north-south latitudinal transect during winter and summer with a new field laser spectroscopy method. Additionally, we measured dissolved CH 4 and O 2 concentrations. Here, we found that in the winter, aerobic CH 4 oxidation was mainly controlled by the dissolved O 2 concentration, while in the summer it was controlled primarily by the CH 4 concentration, which was scarce compared to dissolved O 2. The permafrost environment of the lakes was identified as another key factor. Thermokarst (thaw) lakes formed in yedoma-type permafrost had significantly higher CH 4 oxidation rates compared to other thermokarst and non-thermokarst lakes formed in non-yedoma permafrost environments. As thermokarst lakes formed in yedoma-type permafrost have been identified to receive large quantities of terrestrial organic carbon from thaw and subsidence of the surrounding landscape into the lake, confirming the strong coupling between terrestrial and aquatic habitats and its influence on CH 4 cycling.« less

Quantification of Methane and Ethane Emissions from the San Juan Basin

NASA Astrophysics Data System (ADS)

Smith, M. L.; Kort, E. A.; Karion, A.; Sweeney, C.; Gvakharia, A.

2015-12-01

Methane (CH4), a potent greenhouse gas, and the primary component of natural gas, is emitted from areas of high fossil fuel production and processing. Recently, persistent and large methane emissions (~0.59 Tg yr-1) from the four corners area of the United States have been identified using satellite (SCIAMACHY) observations taken over the years 2003 to 2009. These emissions appear to be the largest CH4 anomaly (positive deviation above background values) in the contiguous U.S., and exceed bottom-up inventory estimates for the area by 1.8 to 3.5 times. The majority of emissions sources expected to contribute to this anomalous CH4 signal are located in the San Juan basin of New Mexico, and include harvesting and processing of natural gas, coal, and coalbed CH4. The magnitude of CH4 emissions from the San Juan basin have not yet been directly quantified using airborne measurements. Additionally, changing fossil fuel-related activities in the basin may have altered the magnitude of CH4 emissions compared to estimates derived from 2003-2009 satellite measurements. Here, we present in-situ airborne observations of CH4 over the San Juan basin, which allow tight quantification of CH4 fluxes using the mass balance method. Observations over the basin were taken for multiple wind directions on multiple days in April, 2015 to obtain a robust estimate of CH4 emissions. The flux of ethane (C2H6), the second most abundant component of natural gas and a tracer species indicative of fossil-derived CH4, was also quantified. Substantial C2H6 emissions may affect regional air quality and chemistry through its influence on tropospheric ozone production.

Adsorption of Simple Benzene Derivatives on Carbon Nanotubes

DTIC Science & Technology

2007-04-17

to the functional groups NH2, CH3, and NO2. These molecules are amonia NH3 for NH2, methane CH4 for CH3, and nitromethane CH3NO2 for NO2, which...DOS is given for nitromethane CH3NO2, methane CH4, and amonia NH3. It can be seen that the adsorption of these molecules also has little effect on

Using carbon isotopes of methane from porewater to understand methane emissions across a permafrost thaw gradient

NASA Astrophysics Data System (ADS)

Varner, R. K.; McCalley, C. K.; Clarizia, P. E.; Verbeke, B. A.; Werner, S. L.; Burke, S. A.; Malhotra, A.; Rocci, K.

2016-12-01

Methane (CH4) emissions from high latitude ecosystems are controlled in part by the presence/absence of permafrost and concomitant modifications in vegetation composition. Rapid transitions in habitat impact CH4 emissions both by changing the moisture regime as well as the production and emission pathways. Measurement of the isotopic composition of CH4 in porewater in these thawed ecosystems can indicate shifts in production pathways of CH4. We measured CH4 and carbon dioxide (CO2) emission, belowground CH4 concentration and 13CH4 of porewater, vegetative type, and vascular greenness area (VGA) along a thaw gradient during summers 2012-2016 in Stordalen Mire, Sweden. Concentrations of CH4 belowground showed positive correlation with aboveground emissions. Carbon isotopic signatures of CH4 varied varied between sites with more hydrogenotrophic signatures in sites dominated by Sphagnum spp. and acetate fermentation signatures in sedge dominated sites (Carex and Eriophorum spp.). These data indicate that these ecosystems transition from thaw, their 13CH4 emissions will change and therefore need to be accounted for in global atmospheric budgets and models.

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

NASA Astrophysics Data System (ADS)

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

2016-10-01

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

Clumped isotope effects during OH and Cl oxidation of methane

NASA Astrophysics Data System (ADS)

Whitehill, Andrew R.; Joelsson, Lars Magnus T.; Schmidt, Johan A.; Wang, David T.; Johnson, Matthew S.; Ono, Shuhei

2017-01-01

A series of experiments were carried out to determine the clumped (13CH3D) methane kinetic isotope effects during oxidation of methane by OH and Cl radicals, the major sink reactions for atmospheric methane. Experiments were performed in a 100 L quartz photochemical reactor, in which OH was produced from the reaction of O(1D) (from O3 photolysis) with H2O, and Cl was from photolysis of Cl2. Samples were taken from the reaction cell and analyzed for methane (12CH4, 12CH3D, 13CH4, 13CH3D) isotopologue ratios using tunable infrared laser direct absorption spectroscopy. Measured kinetic isotope effects for singly substituted species were consistent with previous experimental studies. For doubly substituted methane, 13CH3D, the observed kinetic isotope effects closely follow the product of the kinetic isotope effects for the 13C and deuterium substituted species (i.e., 13,2KIE = 13KIE × 2KIE). The deviation from this relationship is 0.3‰ ± 1.2‰ and 3.5‰ ± 0.7‰ for OH and Cl oxidation, respectively. This is consistent with model calculations performed using quantum chemistry and transition state theory. The OH and Cl reactions enrich the residual methane in the clumped isotopologue in open system reactions. In a closed system, however, this effect is overtaken by the large D/H isotope effect, which causes the residual methane to become anti-clumped relative to the initial methane. Based on these results, we demonstrate that oxidation of methane by OH, the predominant oxidant for tropospheric methane, will only have a minor (∼0.3‰) impact on the clumped isotope signature (Δ13CH3D, measured as a deviation from a stochastic distribution of isotopes) of tropospheric methane. This paper shows that Δ13CH3D will provide constraints on methane source strengths, and predicts that Δ12CH2D2 can provide information on methane sink strengths.

Bimetallo-radical carbon-hydrogen bond activation of methanol and methane.

PubMed

Cui, Weihong; Zhang, X Peter; Wayland, Bradford B

2003-04-30

Carbon-hydrogen bond cleavage reactions of CH3OH and CH4 by a dirhodium(II) diporphyrin complex with a m-xylyl tether (.Rh(m-xylyl)Rh.(1)) are reported. Kinetic-mechanistic studies show that the substrate reactions are bimolecular and occur through the use of two Rh(II) centers in the molecular unit of 1. Second-order rate constants (T = 296 K) for the reactions of 1 with methanol (k(CH3OH) = 1.45 x 10-2 M-1 s-1) and methane (k(CH4) = 0.105 M-1 s-1) show a clear kinetic preference for the methane activation process. The methanol and methane reactions with 1 have large kinetic isotope effects (k(CH3OH)/k(CD3OD) = 9.7 +/- 0.8, k(CH4)/k(CD4) = 10.8 +/- 1.0, T = 296 K), consistent with a rate-limiting step of C-H bond homolysis through a linear transition state. Activation parameters for reaction of 1 with methanol (DeltaH = 15.6 +/- 1.0 kcal mol-1; DeltaS = -14 +/- 5 cal K-1 mol-1) and methane (DeltaH = 9.8 +/- 0.5 kcal mol-1; DeltaS = -30 +/- 3 cal K-1 mol-1) are reported.

Measuring and managing reservoir greenhouse gas emissions

EPA Science Inventory

Methane (CH4) is the second most important anthropogenic greenhouse gas with a heat trapping capacity 34 times greater than that of carbon dioxide on a 100 year time scale. Known anthropogenic CH4 sources include livestock production, rice agriculture, landfills, and natural gas...

Estimation of Methane Emissions in the Los Angeles Basin using CLARS-FTS Observations

NASA Astrophysics Data System (ADS)

Sander, S.; Zeng, Z. C.; Pongetti, T.; Duren, R. M.; Shia, R. L.; Yung, Y. L.; He, L.; Gurney, K. R.

2017-12-01

The Los Angeles Basin (LA Basin), covering almost 10,743 square miles, is home to over 16.8 million people - about half the population of the state of California. It is also the second most populated urban area in the United States and one of the major source of anthropogenic greenhouse gases. Using FTIR observations from the California Laboratory for Atmospheric Remote Sensing (CLARS) located on Mount Wilson at an altitude of 1673m, we measure the reflected near infrared sunlight from 33 surface targets in the Los Angeles megacity including the direct solar beam which gives the free tropospheric background. We then retrieve the excess slant column abundances of important trace gases such as carbon dioxide (CO2) and methane (CH4) in the LA basin. Using atmospheric tracer - tracer correlations for CH4 and CO2 to eliminate the effect of aerosol scattering in the retrieval, we infer methane emissions based on the ratio of XCH4 excess to XCO2 excess. Significant variability is observed in the spatial distributions of excess CH4. Methane emissions in the LA basin show consistent peaks in late summer and winter during the period from Sep 2011 to the present. The strong correlation between natural gas usage data and derived CLARS methane emissions (r2 = 0.5) implies that natural gas leakage during transmission and/or consumption accounts for a significant fraction of the inferred seasonal variability of methane emissions in the LA basin. We will report updated annual trends in CH4 emissions from 2011 to the present. Copyright 2017. All rights reserved.

Resolved 12CH2D2 and 13CH3D in CH4 as Sensitive Indicators of Disequilibrium and Equilibrium during Microbial Methane Cycling

NASA Astrophysics Data System (ADS)

Ash, J. L.; Egger, M.; Slomp, C. P.; Kohl, I. E.; Treude, T.; Rumble, D.; Young, E. D.

2016-12-01

The ability to measure the relative concentrations of at least two doubly-substituted rare isotopologues of gases with biogeochemical relevance provides new constraints on sources and sinks of these gases. In particular, as shown recently for O2, the use of two independent, rare isotopologues allows for detection of thermodynamic intra-species equilibrium and disequilibrium. Here, we report the first measurements of fully resolved 13CH3D and 12CH2D2 from natural samples of microbial methane gas. A suite of sedimentary methane samples from the Bornholm Basin in the Baltic Sea was collected during IODP Exp. 347. Sample depths range from 2-20 meters below seafloor (mbsf). Methane concentrations decrease with depth, and mcrA (a marker for methanogenesis and methanotropy) is present throughout. See Figure. Both Δ13CH3D and Δ12CH2D2 increase with depth as methane concentrations decrease with the shallowest samples exhibiting disequilibrium by up to 2‰ in Δ13CH3D and 13‰ in Δ12CH2D2 while the deepest samples approach isotopic thermodynamic equilibrium (marked by grey bars in Figure). The Fe-mediated anaerobic oxidation of methane (Fe-AOM) has been inferred in these sediments by geochemical modeling . Slow methane cycling by methanogensis and methanotrophy is likely responsible for the approach to isotopic bond order equilibrium in CH4 with depth, consistent with Fe-AOM. While axenic culturing experiments generate methane with large deficits in 12CH2D2 (reported at this meeting), these data from the Baltic Sea demonstrate that isotopic equilibrium can be achieved during microbial recycling of methane. In the absence of Δ12CH2D2, the Δ13CH3D values alone could be misinterpreted as representing gradients in temperature due perhaps to exothermic organic matter degradation. The combination of both mass-18 rare isotopologues of methane provides the means to distinguish equilibrium from disequilibrium and probe microbial methane cycling even where Δ13CH3D suggests reasonable temperatures.

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

PubMed Central

Beck, Jonas; Seth, Barbara; Chappellaz, Jérôme

2017-01-01

Atmospheric methane (CH4) records reconstructed from polar ice cores represent an integrated view on processes predominantly taking place in the terrestrial biogeosphere. Here, we present dual stable isotopic methane records [δ13CH4 and δD(CH4)] from four Antarctic ice cores, which provide improved constraints on past changes in natural methane sources. Our isotope data show that tropical wetlands and seasonally inundated floodplains are most likely the controlling sources of atmospheric methane variations for the current and two older interglacials and their preceding glacial maxima. The changes in these sources are steered by variations in temperature, precipitation, and the water table as modulated by insolation, (local) sea level, and monsoon intensity. Based on our δD(CH4) constraint, it seems that geologic emissions of methane may play a steady but only minor role in atmospheric CH4 changes and that the glacial budget is not dominated by these sources. Superimposed on the glacial/interglacial variations is a marked difference in both isotope records, with systematically higher values during the last 25,000 y compared with older time periods. This shift cannot be explained by climatic changes. Rather, our isotopic methane budget points to a marked increase in fire activity, possibly caused by biome changes and accumulation of fuel related to the late Pleistocene megafauna extinction, which took place in the course of the last glacial. PMID:28673973

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

PubMed

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

2017-07-18

Atmospheric methane (CH 4 ) records reconstructed from polar ice cores represent an integrated view on processes predominantly taking place in the terrestrial biogeosphere. Here, we present dual stable isotopic methane records [δ 13 CH 4 and δD(CH 4 )] from four Antarctic ice cores, which provide improved constraints on past changes in natural methane sources. Our isotope data show that tropical wetlands and seasonally inundated floodplains are most likely the controlling sources of atmospheric methane variations for the current and two older interglacials and their preceding glacial maxima. The changes in these sources are steered by variations in temperature, precipitation, and the water table as modulated by insolation, (local) sea level, and monsoon intensity. Based on our δD(CH 4 ) constraint, it seems that geologic emissions of methane may play a steady but only minor role in atmospheric CH 4 changes and that the glacial budget is not dominated by these sources. Superimposed on the glacial/interglacial variations is a marked difference in both isotope records, with systematically higher values during the last 25,000 y compared with older time periods. This shift cannot be explained by climatic changes. Rather, our isotopic methane budget points to a marked increase in fire activity, possibly caused by biome changes and accumulation of fuel related to the late Pleistocene megafauna extinction, which took place in the course of the last glacial.

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

NASA Astrophysics Data System (ADS)

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

2017-07-01

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

HIGH METHANE EMISSIONS FROM A MID-LATITUDE AGRICULTURAL RESERVOIR

EPA Science Inventory

To assess the magnitude of methane (CH4) emissions from reservoirs in agricultural regions, we measured CH4 emission rates from William H. Harsha Lake, located in southwestern Ohio, USA, over a thirteen month period. The reservoir was a strong source of CH4¬ throughout the year,...

A high level computational study of the CH4/CF4 dimer: how does it compare with the CH4/CH4 and CF4/CF4 dimers?

NASA Astrophysics Data System (ADS)

Biller, Matthew J.; Mecozzi, Sandro

2012-04-01

The interaction within the methane-methane (CH4/CH4), perfluoromethane-perfluoromethane (CF4/CF4) methane-perfluoromethane dimers (CH4/CF4) was calculated using the Hartree-Fock (HF) method, multiple orders of Møller-Plesset perturbation theory [MP2, MP3, MP4(DQ), MP4(SDQ), MP4(SDTQ)], and coupled cluster theory [CCSD, CCSD(T)], as well as the PW91, B97D, and M06-2X density functional theory (DFT) functionals. The basis sets of Dunning and coworkers (aug-cc-pVxZ, x = D, T, Q), Krishnan and coworkers [6-311++G(d,p), 6-311++G(2d,2p)], and Tsuzuki and coworkers [aug(df, pd)-6-311G(d,p)] were used. Basis set superposition error (BSSE) was corrected via the counterpoise method in all cases. Interaction energies obtained with the MP2 method do not fit with the experimental finding that the methane-perfluoromethane system phase separates at 94.5 K. It was not until the CCSD(T) method was considered that the interaction energy of the methane-perfluoromethane dimer (-0.69 kcal mol-1) was found to be intermediate between the methane (-0.51 kcal mol-1) and perfluoromethane (-0.78 kcal mol-1) dimers. This suggests that a perfluoromethane molecule interacts preferentially with another perfluoromethane (by about 0.09 kcal mol-1) than with a methane molecule. At temperatures much lower than the CH4/CF4 critical solution temperature of 94.5 K, this energy difference becomes significant and leads perfluoromethane molecules to associate with themselves, forming a phase separation. The DFT functionals yielded erratic results for the three dimers. Further development of DFT is needed in order to model dispersion interactions in hydrocarbon/perfluorocarbon systems.

Variability and Quasi-Decadal Changes in the Methane Budget over the Period 2000-2012

NASA Technical Reports Server (NTRS)

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

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

NASA Astrophysics Data System (ADS)

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

2017-09-01

Following the recent Global Carbon Project (GCP) synthesis of the decadal methane (CH4) budget over 2000-2012 (Saunois et al., 2016), we analyse here the same dataset with a focus on quasi-decadal and inter-annual variability in CH4 emissions. The GCP dataset integrates results from top-down studies (exploiting atmospheric observations within an atmospheric inverse-modelling framework) and bottom-up models (including process-based models for estimating land surface emissions and atmospheric chemistry), inventories of anthropogenic emissions, and data-driven approaches. The annual global methane emissions from top-down studies, which by construction match the observed methane growth rate within their uncertainties, all show an increase in total methane emissions over the period 2000-2012, but this increase is not linear over the 13 years. Despite differences between individual studies, the mean emission anomaly of the top-down ensemble shows no significant trend in total methane emissions over the period 2000-2006, during the plateau of atmospheric methane mole fractions, and also over the period 2008-2012, during the renewed atmospheric methane increase. However, the top-down ensemble mean produces an emission shift between 2006 and 2008, leading to 22 [16-32] Tg CH4 yr-1 higher methane emissions over the period 2008-2012 compared to 2002-2006. This emission increase mostly originated from the tropics, with a smaller contribution from mid-latitudes and no significant change from boreal regions. The regional contributions remain uncertain in top-down studies. Tropical South America and South and East Asia seem to contribute the most to the emission increase in the tropics. However, these two regions have only limited atmospheric measurements and remain therefore poorly constrained. The sectorial partitioning of this emission increase between the periods 2002-2006 and 2008-2012 differs from one atmospheric inversion study to another. However, all top-down studies suggest smaller changes in fossil fuel emissions (from oil, gas, and coal industries) compared to the mean of the bottom-up inventories included in this study. This difference is partly driven by a smaller emission change in China from the top-down studies compared to the estimate in the Emission Database for Global Atmospheric Research (EDGARv4.2) inventory, which should be revised to smaller values in a near future. We apply isotopic signatures to the emission changes estimated for individual studies based on five emission sectors and find that for six individual top-down studies (out of eight) the average isotopic signature of the emission changes is not consistent with the observed change in atmospheric 13CH4. However, the partitioning in emission change derived from the ensemble mean is consistent with this isotopic constraint. At the global scale, the top-down ensemble mean suggests that the dominant contribution to the resumed atmospheric CH4 growth after 2006 comes from microbial sources (more from agriculture and waste sectors than from natural wetlands), with an uncertain but smaller contribution from fossil CH4 emissions. In addition, a decrease in biomass burning emissions (in agreement with the biomass burning emission databases) makes the balance of sources consistent with atmospheric 13CH4 observations. In most of the top-down studies included here, OH concentrations are considered constant over the years (seasonal variations but without any inter-annual variability). As a result, the methane loss (in particular through OH oxidation) varies mainly through the change in methane concentrations and not its oxidants. For these reasons, changes in the methane loss could not be properly investigated in this study, although it may play a significant role in the recent atmospheric methane changes as briefly discussed at the end of the paper.

Theoretical study on the reaction mechanism of CH 4 with CaO

NASA Astrophysics Data System (ADS)

Yang, Hua-Qing; Hu, Chang-Wei; Qin, Song

2006-11-01

The reaction pathways and energetics for the reaction of methane with CaO are discussed on the singlet spin state potential energy surface at the B3LYP/6-311+G(2df,2p) and QCISD/6-311++G(3df,3pd)//B3LYP/6-311+G(2df,2p) levels of theory. The reaction of methane with CaO is proposed to proceed in the following reaction pathways: CaO + CH 4 → CaOCH 4 → [TS] → CaOH + CH 3, CaO + CH 4 → OCaCH 4 → [TS] → HOCaCH 3 → CaOH + CH 3 or [TS] → CaCH 3OH → Ca + CH 3OH, and OCaCH 4 → [TS] → HCaOCH 3 → CaOCH 3 + H or [TS] → CaCH 3OH → Ca + CH 3OH. The gas-phase methane-methanol conversion by CaO is suggested to proceed via two kinds of important reaction intermediates, HOCaCH 3 and HCaOCH 3, and the reaction pathway via the hydroxy intermediate (HOCaCH 3) is energetically more favorable than the other one via the methoxy intermediate (HCaOCH 3). The hydroxy intermediate HOCaCH 3 is predicted to be the energetically most preferred configuration in the reaction of CaO + CH 4. Meanwhile, these three product channels (CaOH + CH 3, CaOCH 3 + H and Ca + CH 3OH) are expected to compete with each other, and the formation of methyl radical is the most preferable pathway energetically. On the other hand, the intermediates HCaOCH 3 and HOCaCH 3 are predicted to be the energetically preferred configuration in the reaction of Ca + CH 3OH, which is precisely the reverse reaction of methane hydroxylation.

Methane emissions from boreal peatlands in a changing climate: Quantifying the sensitivity of methane fluxes to experimental manipulations of water table and soil temperature regimes in an Alaskan boreal fen

NASA Astrophysics Data System (ADS)

Treat, C. C.; Turetsky, M.; Harden, J.; McGuire, A.

2006-12-01

Peatlands cover only 3-5 % of the world's land surface but store 30 % of the world's soil carbon (C) pool. Peatlands currently are thought to function globally as a net sink for atmospheric CO2, sequestering approximately 76 Tg (1012 g) C yr-1. However, peatlands also function as a net source of atmospheric CH4. Approximately 25% of the 270 Tg CH4 yr-1 emitted from natural sources are emitted from northern wetlands. Methane production (methanogenesis) and consumption (methane oxidation) in peatlands are sensitive to both fluctuations in soil moisture and temperature. Boreal regions already are experiencing rapid changes in climate, including longer and drier growing seasons and the degradation of permafrost. Changes in peat environments in response to these climate changes could have significant implications for CH4 emissions to the atmosphere, and thus the radiative forcing of high latitude regions. In 2005, we initiated a large scale in situ climate experiment in a moderately rich fen near the Bonanza Creek LTER site in central Alaska (APEX: www.apex.msu.edu). The goal of our project is to understand vegetation and C cycling processes under altered water table and soil thermal regimes. We established three water table plots (control, raised, lowered), each about 120 m2 in area, using drainage ditches to lower the water table by 5-10 cm and solar powered pumps to raise the water table by about 5-15 cm. Within each water table plot, we constructed replicate open top chambers (OTCs) to passively increase surface temperatures by about 1 ° C. We used static chambers and gas chromatography to quantify methane fluxes at each water table x soil warming plot through the growing seasons of 2005 and 2006. Additionally, we quantified seasonal CH4 fluxes along an adjacent moisture gradient that included four distinct soil moisture and vegetation zones, including a moderately rich fen (APEX site), an emergent macrophyte marsh, a shrubby permafrost fen, and a black spruce permafrost forest. Our results thus far show that methane fluxes varied by a warming x water table interaction across our experimental treatments (Proc Mixed SAS Repeated Measures ANOVA; F2,8=4.07; p=0.05), with the largest methane fluxes in the warm, wet peatland plots and the lowest methane fluxes in the unwarmed, dry peatland plots. Sites along the moisture gradient transitioned from methane sources in the rich fen site (APEX plots) to small sinks of CH4 in the permafrost forest under drying soil moisture conditions. Our soil climate manipulations allow us to quantify interactions among biogeophysical variables that control CH4 emissions from peatlands. Our coupled experimental and gradient based measurements allow us to explore controls on microbial populations and methane emissions across a wider range of terrestrial boreal environments. This work so far shows that methane cycling in interior Alaskan ecosystems is extremely sensitive to soil climate conditions, and that the fate of methane emissions from high latitudes will be affected primarily by changes in precipitation and soil drainage that control water table position in peatlands and permafrost ecosystems.

Making methane visible

NASA Astrophysics Data System (ADS)

Gålfalk, Magnus; Olofsson, Göran; Crill, Patrick; Bastviken, David

2016-04-01

Methane (CH4) is one of the most important greenhouse gases, and an important energy carrier in biogas and natural gas. Its large scale emission patterns have been unpredictable and the source and sink distributions are poorly constrained. Remote assessment of CH4 with high sensitivity at m2 spatial resolution would allow detailed mapping of near ground distribution and anthropogenic sources and sinks in landscapes but has hitherto not been possible. Here we show that CH4 gradients can be imaged on

DOE Office of Scientific and Technical Information (OSTI.GOV)

Taylor, J.A.; Brasseur, G.P.; Zimmerman, P.R.

Using the hydroxyl radical field calibrated to the methyl chloroform observations, the globally averaged release of methane and its spatial and temporal distribution were investigated. Two source function models of the spatial and temporal distribution of the flux of methane to the atmosphere were developed. The first model was based on the assumption that methane is emitted as a proportion of net primary productivity (NPP). With the average hydroxyl radical concentration fixed, the methane source term was computed as {approximately}623 Tg CH{sub 4}, giving an atmospheric lifetime for methane {approximately}8.3 years. The second model identified source regions for methane frommore » rice paddies, wetlands, enteric fermentation, termites, and biomass burning based on high-resolution land use data. This methane source distribution resulted in an estimate of the global total methane source of {approximately}611 Tg CH{sub 4}, giving an atmospheric lifetime for methane {approximately}8.5 years. The most significant difference between the two models were predictions of methane fluxes over China and South East Asia, the location of most of the world's rice paddies. Using a recent measurement of the reaction rate of hydroxyl radical and methane leads to estimates of the global total methane source for SF1 of {approximately}524 Tg CH{sub 4} giving an atmospheric lifetime of {approximately}10.0 years and for SF2{approximately}514 Tg CH{sub 4} yielding a lifetime of {approximately}10.2 years.« less

Characterisation of methane isotope composition over the Silesian Coal Basin, Poland.

NASA Astrophysics Data System (ADS)

Necki, Jaroslaw; Zimnoch, Miroslaw; Jasek, Alina; Chmura, Lukasz; Galkowski, Michal; Wolkowicz, Wojciech

2017-04-01

Methane emissions from Silesian Coal Basin (SCB), one of European regions associated with coal excavation industry constitute an important component of the continental anthropogenic flux of this gas into the atmosphere. It is estimated by different methodology that SCB is responsible for between 450 - 1350 Gg CH4 of atmospheric methane releases annually, making it one of the most significant sources of this gas in Europe. In this region, active or restructuring coal mining methane emissions may lead to elevated concentrations of this gas in near-ground atmosphere. Observed methane mixing ratio in pbl during nighttime over the specific areas of SCB is elevated by up to 50ppm with carbon isotope source ratio -46‰ to -52‰ with occasionally lighter methane (-58) form particular coal beds. Numbers were derived from direct measurement of samples taken from ventilation shafts (concentration 1.5% to 4% of CH4, subsequently diluted to 2ppm with zero air and measured by Picarro CRDS analyzer). Measurements of CH4 mixing ratios and isotopic composition were performed along latitudinal transects (ca. 50oN), typically extending from ca. 15oE to 20oE, covering the Upper Silesia and bordering regions on the public roads in vicinity of the mine ventilation shafts. Apart from CH4 emissions associated with coal production, other sources of anthropogenic methane are also active over SCB. These include city gas networks leakages that enrich the air by up to 5ppm (in the city centers, carbon isotope ratio on average -52). Most of the numerous landfills, not yet equipped with appropriate CH4 uptake installations, also contribute to substantial anthropogenic flux of this gas to the atmosphere. Values of methane mixing ratio recorded during the in-situ measurements close to the landfill sites reached 15ppm (with carbon isotope ratio -56‰ to -60). The transects of methane concentration over Silesian area, assisted by analysis of its stable isotopic composition has been performed in all of the locations where active and closed mining shafts are positioned, and most of the landfills and cities under the different meteorological and synoptic conditions to provide a base for efficient future verification of methane inventory over SCB. Project will be continued with MEMO2 ITN H2020.

Diagnostic studies of H2 Ar N2 microwave plasmas containing methane or methanol using tunable infrared diode laser absorption spectroscopy

NASA Astrophysics Data System (ADS)

Hempel, F.; Davies, P. B.; Loffhagen, D.; Mechold, L.; Röpcke, J.

2003-11-01

Tunable infrared diode laser absorption spectroscopy has been used to detect the methyl radical and nine stable molecules, CH4, CH3OH, C2H2, C2H4, C2H6, NH3, HCN, CH2O and C2N2, in H2-Ar-N2 microwave plasmas containing up to 7% of methane or methanol, under both flowing and static conditions. The degree of dissociation of the hydrocarbon precursor molecules varied between 20% and 97%. The methyl radical concentration was found to be in the range 1012-1013 molecules cm-3. By analysing the temporal development of the molecular concentrations under static conditions it was found that HCN and NH3 are the final products of plasma chemical conversion. The fragmentation rates of methane and methanol (RF(CH4) = (2-7) × 1015 molecules J-1, RF(CH3OH) = (6-9) × 1015 molecules J-1) and the respective conversion rates to methane, hydrogen cyanide and ammonia (RCmax(CH4) = 1.2 × 1015 molecules J-1, RCmax(HCN) = 1.3 × 1015 molecules J-1, RCmax(NH3) = 1 × 1014 molecules J-1) have been determined for different hydrogen to nitrogen concentration ratios. An extensive model of the chemical reactions involved in the H2-N2-Ar-CH4 plasma has been developed. Model calculations were performed by including 22 species, 145 chemical reactions and appropriate electron impact dissociation rate coefficients. The results of the model calculations showed satisfactory agreement between calculated and measured concentrations. The most likely main chemical pathways involved in these plasmas are discussed and an appropriate reaction scheme is proposed.

Microbial methane from in situ biodegradation of coal and shale: A review and reevaluation of hydrogen and carbon isotope signatures

USGS Publications Warehouse

Vinson, David S.; Blair, Neal E.; Martini, Anna M.; Larter, Steve; Orem, William H.; McIntosh, Jennifer C.

2017-01-01

Stable carbon and hydrogen isotope signatures of methane, water, and inorganic carbon are widely utilized in natural gas systems for distinguishing microbial and thermogenic methane and for delineating methanogenic pathways (acetoclastic, hydrogenotrophic, and/or methylotrophic methanogenesis). Recent studies of coal and shale gas systems have characterized in situ microbial communities and provided stable isotope data (δD-CH4, δD-H2O, δ13C-CH4, and δ13C-CO2) from a wider range of environments than available previously. Here we review the principal biogenic methane-yielding pathways in coal beds and shales and the isotope effects imparted on methane, document the uncertainties and inconsistencies in established isotopic fingerprinting techniques, and identify the knowledge gaps in understanding the subsurface processes that govern H and C isotope signatures of biogenic methane. We also compare established isotopic interpretations with recent microbial community characterization techniques, which reveal additional inconsistencies in the interpretation of microbial metabolic pathways in coal beds and shales. Collectively, the re-assessed data show that widely-utilized isotopic fingerprinting techniques neglect important complications in coal beds and shales.Isotopic fingerprinting techniques that combine δ13C-CH4 with δD-CH4 and/or δ13C-CO2have significant limitations: (1) The consistent ~ 160‰ offset between δD-H2O and δD-CH4 could imply that hydrogenotrophic methanogenesis is the dominant metabolic pathway in microbial gas systems. However, hydrogen isotopes can equilibrate between methane precursors and coexisting water, yielding a similar apparent H isotope signal as hydrogenotrophic methanogenesis, regardless of the actual methane formation pathway. (2) Non-methanogenic processes such as sulfate reduction, Fe oxide reduction, inputs of thermogenic methane, anaerobic methane oxidation, and/or formation water interaction can cause the apparent carbon isotope fractionation between δ13C-CH4 and δ13C-CO2(α13CCO2-CH4) to differ from the true methanogenic fractionation, complicating interpretation of methanogenic pathways. (3) Where little-fractionating non-methanogenic bacterial processes compete with highly-fractionating methanogenesis, the mass balance between CH4 and CO2 is affected. This has implications for δ13C values and provides an alternative interpretation for net C isotope signatures than solely the pathways used by active methanogens. (4) While most of the reviewed values of δD-H2O - δD-CH4 and α13CCO2-CH4 are apparently consistent with hydrogenotrophic methanogenesis as the dominant pathway in coal beds and shales, recent microbial community characterization techniques suggest a possible role for acetoclastic or methylotrophic methanogenesis in some basins.

New Isotopic Constraints on the Sources of Methane at Sites of Active Continental Serpentinization

NASA Astrophysics Data System (ADS)

Wang, D. T.; Gruen, D.; Morrill, P. L.; Rietze, A.; Nealson, K. H.; Kubo, M. D.; Cardace, D.; Schrenk, M. O.; Hoehler, T. M.; McCollom, T. M.; Etiope, G.; Hosgormez, H.; Schoell, M.; Ono, S.

2014-12-01

At continental sites of serpentinization, high concentrations of reduced gases (e.g., H2, CH4) are frequently found in association with highly-alkaline groundwater. Identification of the process(es) responsible for the generation of methane—as well as the source(s) of C & H—in these environments has been challenging. The difficulty is due to both the wide range of processes (microbial, thermal, abiotic) that could be involved, and the limited number of parameters that are accessible to currently-available analytical technologies (e.g., δ13C, δD). The recent development of a new technique based on tunable infrared laser spectroscopy [1] has enabled the fully-resolved quantification of four isotopologues of methane: 12CH4, 13CH4, 12CH3D, and 13CH3D, a doubly-substituted ("clumped") isotopologue. We used this technique to measure 13CH3D in gases sampled from continental sites of serpentinization, in order to provide independent constraints on C-H bond-forming processes involved in the generation of the methane found in these systems. Our study sites are hosted in ultramafic units that are presently undergoing serpentinization. These include The Cedars peridotite body (Calif., USA) [2], the Coast Range Ophiolite Microbial Observatory (Calif., USA) [3], and the Chimaera seep (Tekirova Ophiolite, Turkey) [4]. Preliminary measurements indicate that Δ13CH3D (the deviation of the abundance of 13CH3D from the stochastic distribution) in methane sampled from these sites spans nearly the entire range of thermodynamically-predicted values, from >+5‰ (13CH3D-based apparent equilibrium temperature < 45 °C) to ~0‰ (Tapparent → ∞). The new 13CH3D data is complemented by conventional geochemical analyses (e.g., dissolved ions/organics, δ13C, δD) on samples collected during the same field campaigns. Our study demonstrates that the measurement of 13CH3D provides a new dimension of isotopic constraints for unraveling the complex processes controlling the distribution of methane, and the flow of energy and carbon, in areas of active continental serpentinization. [1] Ono et al. (2014) Anal. Chem. 86, 6487. [2] Morrill et al. (2013) Geochim. Cosmochim. Acta 109, 222. [3] Cardace et al. (2013) Sci. Dril. 16, 45. [4] Etiope et al. (2011) Earth Planet. Sci. Lett. 310, 96.

Temporal variability of methane fluxes in West Siberian taiga bogs and its implications for estimating regional methane emission

NASA Astrophysics Data System (ADS)

Sabrekov, Alexander; Ilyasov, Danil; Terentieva, Irina; Glagolev, Mikhail; Maksyutov, Shamil

2017-04-01

The West Siberia Lowland (WSL) is the biggest peatland area in Eurasia and is situated in the high latitudes experiencing enhanced rate of climate change. During 2015-16 summer periods, seasonal measurements of methane emission were made at the field station «Mukhrino» in the WSL middle taiga zone. The study was made at 3 wetland ecosystem types covering 80% of the taiga wetland area: i) waterlogged hollows or depressed areas with water level above the moss surface, ii) oligotrophic hollows or depressed parts of bogs with water level beneath the moss surface, iii) forested bogs with dwarf shrubs-sphagnum vegetation. Seven series of measurements were made by a static chamber method in 2016 and four series - in 2015. In 2015, we observed non-typical weather conditions including early dry spring and short cold rainy summer. Oppositely, weather conditions in 2016 were closer to average long-term with warmer drier summer. Significant difference between these years allowed analyzing the temporal variability and its sources. Average methane flux rates from forested bogs were 0.57 mgCH4/m2/h in 2016 and 0.33 mgCH4/m2/h in 2015. Seasonal dynamic during both years had similar concave downward shape. The highest fluxes were observed in June and were corresponded to the highest WTL, the main limiting factor of emission from forested bogs. The lowest fluxes in July were related to the low WTL combining with the highest temperature of upper methanotrophy layer. Average methane flux rates from oligotrophic hollows were 7.18 mgCH4/m2/h in 2016 and 4.28 mgCH4/m2/h in 2015. Seasonal dynamic of methane emission was indistinct in 2015. On the contrary, in 2016 it had regular seasonal pattern with peak emissions in July, which were four times higher than in 2015. WTL was not the limiting factor for CH4 emission from oligotrophic hollows, because even in the driest ones it was only 10 cm below the surface. Thus, the difference between peak emissions in 2015 and 2016 was mainly related to the temperature, which was considerably higher in 2016. Average methane flux rates from waterlogged hollows were 2.19 mgCH4/m2/h in 2016 and 4.07 mgCH4/m2/h in 2015. Seasonal dynamic had prominent shape in both years, however, peak emissions were observed in different months. Overall, patterns of emission in these ecosystems had more complicate nature and needs future investigations. Regional methane emission was estimated using new wetland map by Terentieva et al. (2016). Seasonal dynamic data for 2015-16 years gave the regional flux of 161 and 1257 ktCH4/yr for forested bogs and oligotrophic hollows, respectively. Similar values were obtained using not seasonal dynamic but only flux medians for 2015-16 years. However, the usage of old dataset gave only 32 and 841 ktCH4/yr for forested bogs and oligotrophic hollows, respectively. Thus, seasonal dynamics data had lower impact on regional methane emission estimate comparing to interannual variability data. Terentieva, I.E., Glagolev, M.V., Lapshina, E.D., Sabrekov, A.F., Maksyutov, S. Mapping of West Siberian taiga wetland complexes using Landsat imagery: implications for methane emissions // Biogeosciences. 2016. V. 13. № 16. P. 4615-4626.

Spatial variability of methane production and methanogen communities within a eutrophic reservoir: evaluating the importance of organic matter source and quantity

EPA Science Inventory

Freshwater reservoirs are an important source of the greenhouse gas methane (CH4) to the atmosphere, but there is a wide range of estimates of global emissions, due in part to variability of methane emissions rates within reservoirs. While morphological characteristics, including...

Regulators of coastal wetland methane production and responses to simulated global change

Treesearch

Carmella Vizza; William E. West; Stuart E. Jones; Julia A. Hart; Gary A. Lamberti

2017-01-01

Wetlands are the largest natural source of methane (CH4) emissions to the atmosphere, which vary along salinity and productivity gradients. Global change has the potential to reshape these gradients and therefore alter future contributions of wetlands to the global CH4 budget. Our study examined CH4...

Forest ecosystem changes from annual methane source to sink depending on late summer water balance

Treesearch

Julie K. Shoemaker; Trevor F. Keenan; David Y. Hollinger; Andrew D. Richardson

2014-01-01

Forests dominate the global carbon cycle, but their role in methane (CH4) biogeochemistry remains uncertain. We analyzed whole-ecosystem CH4 fluxes from 2 years, obtained over a lowland evergreen forest in Maine, USA. Gross primary productivity provided the strongest correlation with the CH4 flux in...

Impact of transport and modelling errors on the estimation of methane sources and sinks by inverse modelling

NASA Astrophysics Data System (ADS)

Locatelli, Robin; Bousquet, Philippe; Chevallier, Frédéric

2013-04-01

Since the nineties, inverse modelling by assimilating atmospheric measurements into a chemical transport model (CTM) has been used to derive sources and sinks of atmospheric trace gases. More recently, the high global warming potential of methane (CH4) and unexplained variations of its atmospheric mixing ratio caught the attention of several research groups. Indeed, the diversity and the variability of methane sources induce high uncertainty on the present and the future evolution of CH4 budget. With the increase of available measurement data to constrain inversions (satellite data, high frequency surface and tall tower observations, FTIR spectrometry,...), the main limiting factor is about to become the representation of atmospheric transport in CTMs. Indeed, errors in transport modelling directly converts into flux changes when assuming perfect transport in atmospheric inversions. Hence, we propose an inter-model comparison in order to quantify the impact of transport and modelling errors on the CH4 fluxes estimated into a variational inversion framework. Several inversion experiments are conducted using the same set-up (prior emissions, measurement and prior errors, OH field, initial conditions) of the variational system PYVAR, developed at LSCE (Laboratoire des Sciences du Climat et de l'Environnement, France). Nine different models (ACTM, IFS, IMPACT, IMPACT1x1, MOZART, PCTM, TM5, TM51x1 and TOMCAT) used in TRANSCOM-CH4 experiment (Patra el al, 2011) provide synthetic measurements data at up to 280 surface sites to constrain the inversions performed using the PYVAR system. Only the CTM (and the meteorological drivers which drive them) used to create the pseudo-observations vary among inversions. Consequently, the comparisons of the nine inverted methane fluxes obtained for 2005 give a good order of magnitude of the impact of transport and modelling errors on the estimated fluxes with current and future networks. It is shown that transport and modelling errors lead to a discrepancy of 27 TgCH4 per year at global scale, representing 5% of the total methane emissions for 2005. At continental scale, transport and modelling errors have bigger impacts in proportion to the area of the regions, ranging from 36 TgCH4 in North America to 7 TgCH4 in Boreal Eurasian, with a percentage range from 23% to 48%. Thus, contribution of transport and modelling errors to the mismatch between measurements and simulated methane concentrations is large considering the present questions on the methane budget. Moreover, diagnostics of statistics errors included in our inversions have been computed. It shows that errors contained in measurement errors covariance matrix are under-estimated in current inversions, suggesting to include more properly transport and modelling errors in future inversions.

Characterization of methane oxidation in a simulated landfill cover system by comparing molecular and stable isotope mass balances.

PubMed

Schulte, Marcel; Jochmann, Maik A; Gehrke, Tobias; Thom, Andrea; Ricken, Tim; Denecke, Martin; Schmidt, Torsten C

2017-11-01

Biological methane oxidation may be regarded as a method of aftercare treatment for landfills to reduce climate relevant methane emissions. It is of social and economic interest to estimate the behavior of bacterial methane oxidation in aged landfill covers due to an adequate long-term treatment of the gas emissions. Different approaches assessing methane oxidation in laboratory column studies have been investigated by other authors recently. However, this work represents the first study in which three independent approaches, ((i) mass balance, (ii) stable isotope analysis, and (iii) stoichiometric balance of product (CO 2 ) and reactant (CH 4 ) by CO 2 /CH 4 -ratio) have been compared for the estimation of the biodegradation by a robust statistical validation on a rectangular, wide soil column. Additionally, an evaluation by thermal imaging as a potential technique for the localization of the active zone of bacterial methane oxidation has been addressed in connection with stable isotope analysis and CO 2 /CH 4 -ratios. Although landfills can be considered as open systems the results for stable isotope analysis based on a closed system correlated better with the mass balance than calculations based on an open system. CO 2 /CH 4 -ratios were also in good agreement with mass balance. In general, highest values for biodegradation were determined from mass balance, followed by CO 2 /CH 4 -ratio, and stable isotope analysis. The investigated topsoil proved to be very suitable as a potential cover layer by removing up to 99% of methane for CH 4 loads of 35-65gm -2 d -1 that are typical in the aftercare phase of landfills. Finally, data from stable isotope analysis and the CO 2 /CH 4 -ratios were used to trace microbial activity within the reactor system. It was shown that methane consumption and temperature increase, as a cause of high microbial activity, correlated very well. Copyright © 2017 Elsevier Ltd. All rights reserved.

Mobile Measurements of Methane Using High-Speed Open-Path Technology

NASA Astrophysics Data System (ADS)

Burba, G. G.; Anderson, T.; Ediger, K.; von Fischer, J.; Gioli, B.; Ham, J. M.; Hupp, J. R.; Kohnert, K.; Levy, P. E.; Polidori, A.; Pikelnaya, O.; Price, E.; Sachs, T.; Serafimovich, A.; Zondlo, M. A.; Zulueta, R. C.

2016-12-01

Methane plays a critical role in the radiation balance, chemistry of the atmosphere, and air quality. The major anthropogenic sources of CH4 include oil and gas development sites, natural gas distribution networks, landfill emissions, and agricultural production. The majority of oil and gas and urban CH4 emission occurs via variable-rate point sources or diffused spots in topographically challenging terrains (e.g., street tunnels, elevated locations at water treatment plants, vents, etc.). Locating and measuring such CH4 emissions is challenging when using traditional micrometeorological techniques, and requires development of novel approaches. Landfill CH4 emissions traditionally assessed at monthly or longer time intervals are subject to large uncertainties because of the snapshot nature of the measurements and the barometric pumping phenomenon. The majority of agricultural and natural CH4 production occurs in areas with little infrastructure or easily available grid power (e.g., rice fields, arctic and boreal wetlands, tropical mangroves, etc.). A lightweight, high-speed, high-resolution, open-path technology was recently developed for eddy covariance measurements of CH4 flux, with power consumption 30-150 times below other available technologies. It was designed to run on solar panels or a small generator and be placed in the middle of the methane-producing ecosystem without a need for grid power. Lately, this instrumentation has been utilized increasingly more frequently outside of the traditional use on stationary flux towers. These novel approaches include measurements from various moving platforms, such as cars, aircraft, and ships. Projects included mapping of concentrations and vertical profiles, leak detection and quantification, mobile emission detection from natural gas-powered cars, soil CH4 flux surveys, etc. This presentation will describe key projects utilizing the novel lightweight low-power high-resolution open-path technology, and will highlight several novel approaches where such instrumentation was used in mobile deployments in urban, agricultural and natural environments by academic institutions, regulatory agencies and industry.

Understanding the glacial methane cycle

PubMed Central

Hopcroft, Peter O.; Valdes, Paul J.; O'Connor, Fiona M.; Kaplan, Jed O.; Beerling, David J.

2017-01-01

Atmospheric methane (CH4) varied with climate during the Quaternary, rising from a concentration of 375 p.p.b.v. during the last glacial maximum (LGM) 21,000 years ago, to 680 p.p.b.v. at the beginning of the industrial revolution. However, the causes of this increase remain unclear; proposed hypotheses rely on fluctuations in either the magnitude of CH4 sources or CH4 atmospheric lifetime, or both. Here we use an Earth System model to provide a comprehensive assessment of these competing hypotheses, including estimates of uncertainty. We show that in this model, the global LGM CH4 source was reduced by 28–46%, and the lifetime increased by 2–8%, with a best-estimate LGM CH4 concentration of 463–480 p.p.b.v. Simulating the observed LGM concentration requires a 46–49% reduction in sources, indicating that we cannot reconcile the observed amplitude. This highlights the need for better understanding of the effects of low CO2 and cooler climate on wetlands and other natural CH4 sources. PMID:28220787

Theoretical insights into the selective oxidation of methane to methanol in copper-exchanged mordenite

DOE PAGES

Zhao, Zhi -Jian; Kulkarni, Ambarish; Vilella, Laia; ...

2016-05-02

Selective oxidation of methane to methanol is one of the most difficult chemical processes to perform. A potential group of catalysts to achieve CH 4 partial oxidation are Cu-exchanged zeolites mimicking the active structure of the enzyme methane monooxygenase. However, the details of this conversion, including the structure of the active site, are still under debate. In this contribution, periodic density functional theory (DFT) methods were employed to explore the molecular features of the selective oxidation of methane to methanol catalyzed by Cu-exchanged mordenite (Cu-MOR). We focused on two types of previously suggested active species, CuOCu and CuOOCu. Our calculationsmore » indicate that the formation of CuOCu is more feasible than that of CuOOCu. In addition, a much lower C–H dissociation barrier is located on the former active site, indicating that C–H bond activation is easily achieved with CuOCu. We calculated the energy barriers of all elementary steps for the entire process, including catalyst activation, CH 4 activation, and CH 3OH desorption. Finally, our calculations are in agreement with experimental observations and present the first theoretical study examining the entire process of selective oxidation of methane to methanol.« less

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

Recently, we developed a theoretical model to investigate the potential use of 13CH3D and 12CH2D2 as tools for tracking atmospheric methane budget. We used electronic structure methods to estimate kinetic isotope fractionations associated with the major sink reactions of CH4 in air (reactions with •OH and Cl•), and literature data with reconnaissance measurements of the relative abundances of 13CH3D and 12CH2D2 to estimate the compositions of the largest atmospheric sources. Here we present new methane rare isotopologue data from boreal wetlands, comprising one of the most important sources, in order to evaluate the robustness of the model. Boreal wetlands (>55° N) account for more than half of the wetland area in the Northern hemisphere. We analyzed methane samples from high latitude lakes representing different geographical regions, geological and ecological contexts, methane fluxes, and isotopic signatures. Using clumped isotopes of CH4 we are able to determine the likely production mechanism for natural CH4 samples. So far, all of our analyzed samples except one plot in the microbial pure-culture methanogenesis field (Young et al. 2017) with ranges of -0.2‰ to +1.2‰ for Δ13CH3D, and -29.6‰ to -18.2‰ for Δ12CH2D2. These compositions are far from equilibrium. The one exception, from Lake Doughnut, Alaska, exhibits Δ13CH3D and Δ12CH2D2 values of +5.2‰ and +18.7‰, respectively, which fall near ambient thermodynamic equilibrium values. This may be an effect of methanotrophy. Mean Δ13CH3D and Δ12CH2D2 for all lake samples are +1.7‰ and -15.4‰ respectively, compared to our original estimate of +6.1‰ and +21.2‰ for the wetland methane source based on an assumption of equilibrium. If we assume that these samples are representative of the overall wetland source, Δ13CH3D decreases by 0.8‰ and Δ12CH2D2 decreases by 0.6‰ in our model of bulk atmospheric methane. Δ13CH3D and Δ12CH2D2 values of air (including •OH and Cl• sink reactions) are estimated to be +3.6‰ and +112.9‰, respectively. Even if we exclude the Lake Doughnut sample, the total effect on Δ12CH2D2 in air is no more than 2‰. Our model predicts that sink reactions generate a distinctly elevated Δ12CH2D2 (by 104‰) relative to the source composition. In contrast, differences in source compositions have a comparatively small effect, on the order of a few per mil at most.

Ice core δD(CH4) record precludes marine hydrate CH4 emissions at the onset of Dansgaard-Oeschger events

NASA Astrophysics Data System (ADS)

Bock, M.; Schmitt, J.; Möller, L.; Spahni, R.; Blunier, T.; Fischer, H.

2010-12-01

Air enclosures in polar ice cores represent the only direct paleoatmospheric archive (besides firn air) and show that atmospheric CH4 concentrations changed in concert with northern hemisphere temperature during both glacial/interglacial transitions as well as rapid climate changes (Dansgaard-Oeschger events). For stadials and interstadials during Marine Isotope Stage 3 concentration jumps of 100 - 200 ppbv within a few decades are observed. A concentration gradient with higher values in the northern versus the southern hemisphere during warm stages was reconstructed from ice core methane data from Greenland and Antarctica. This gradient indicates additional methane emissions during warm periods located in the northern hemisphere. However, the underlying processes for these changes are still not well understood. With tropical and boreal wetlands, biomass burning, thermokarst lakes, ruminants, termites, UV-induced emissions from organic matter and marine gas hydrates all contributing to the natural atmospheric CH4 level, an unambiguous source attribution remains difficult. Also changes in the methane sinks can modify the tropospheric CH4 budget, as trace gases like volatile organic compounds are competing for the major reactant - the OH radical. Additionally, the changing global atmospheric methane concentration itself feeds back on its lifetime. Together with the CH4 interhemispheric gradient, stable hydrogen and carbon isotopic studies on methane (δD(CH4) and δ13CH4) in ice cores allow to constrain individual CH4 source/sink changes. Here we present clear evidence from the North Greenland Ice Core Project ice core based on the hydrogen isotopic composition of methane δD(CH4) that clathrates did not cause atmospheric methane concentration to rise at the onset of Dansgaard-Oeschger (DO) events 7 and 8 (34 - 41 kilo years before present), however, we can not exclude that they played a minor role during and at the end of an interstadial. Box modeling supports boreal wetland emissions as the most likely explanation for the interstadial increase, strengthening from ~6 to ~30 Tg CH4 yr-1 from stadial to interstadial conditions, respectively. Our steady state model results suggest constant background clathrate emissions for the investigated time slices (~25 Tg CH4 yr-1). Tropical wetland emissions strengthened only moderately for the long interstadial 8 (from ~84 to ~118 Tg CH4 yr-1) and biomass burning emissions show slightly higher values during the interstadial time slices (~55 to ~60 versus ~45 Tg CH4 yr-1 in the stadial). Moreover, our data show that δD(CH4) dropped 500 years before the onset of DO 8, with CH4 concentration rising only slightly. This can be explained by an early climate response of boreal wetlands, which carry the strongly depleted isotopic signature of high-latitude precipitation at that time. Reference: Bock et al., 2010, Science, 328, p1686

Fate of methane in aquatic systems dominated by free-floating plants.

PubMed

Kosten, Sarian; Piñeiro, Marcia; de Goede, Eefje; de Klein, Jeroen; Lamers, Leon P M; Ettwig, Katharina

2016-11-01

Worldwide the area of free-floating plants is increasing, which can be expected to alter methane (CH 4 ) emissions from aquatic systems in several ways. A large proportion of the CH 4 produced may become oxidized below the plants due to the accumulation of CH 4 as a result of a decrease in the diffusive water-atmosphere flux and the entrapment of part of the ebullitive CH 4 , in combination with suitable conditions for methane oxidizing (MOX) bacteria in the aerobic rhizosphere. We used a set of essays to test this hypothesis and to explore the effect of different densities for three widespread free-floating species: Azolla filiculoides, Salvinia natans, and Eichhornia crassipes. The gas exchange velocity, proportion of CH 4 bubbles trapped by the plants, occurrence of radial oxygen loss from roots, and MOX rates on the roots were assessed. We subsequently used the outcome of these experiments to parameterize a simple model. With this model we estimated the proportion of the produced CH 4 that is oxidized, for different plant species and different densities. We found that in a shallow (1 m) system up to 70% of the CH 4 produced may become oxidized as a result of a strong decrease in gas exchange combined with high MOX activity of the rhizosphere microbiome. As floating plants also are likely to increase CH 4 production by organic matter production, especially when their presence induces anaerobic conditions, the overall effect on CH 4 emission will strongly depend on local conditions. This explains the contrasting effects of floating plants on CH 4 emissions in literature as reviewed here. As the effect of floating plants on CH 4 emissions, including the high MOX rates we show here, can be substantial, there is an urgent need to consider this impact when assessing greenhouse gas budgets. Copyright © 2016 Elsevier Ltd. All rights reserved.

Physical and biological controls over patterns of methane flux from wetland soils

NASA Astrophysics Data System (ADS)

Owens, S. M.; von Fischer, J. C.

2006-12-01

While methane (CH4) production and plant-facilitated gas transport both contribute to patterns of CH4 emissions from wetlands, the relative importance of each mechanism is uncertain. In flooded wetland soils, CH4 is produced by anaerobic methanogenic bacteria. In the absence of competing oxidizers (i.e. SO42-, NO3-, O2), CH4 production is limited by the availability of labile carbon, which is supplied from recent plant primary production (e.g. as root exudates) and converted by anaerobic fermenting bacteria into methanogenic substrate (e.g. acetate). Because diffusion of gases through saturated soils is extremely slow, the aerenchymous tissues of wetland plants provide the primary pathway for CH4 emissions in systems dominated by emergent vascular vegetation. Aerenchyma also function to shuttle atmospheric oxygen to belowground plant tissues for respiration. Consequentially, root radial oxygen loss results in an oxidized rhizosphere, which limits CH4 production and provides habitat for aerobic methanotrophic bacteria, potentially reducing CH4 emissions. To test the contribution of recent photosynthates on CH4 emissions, a shading experiment was conducted in a Juncus-dominated wetland in the Colorado Front Range. Shade treatments significantly reduced net ecosystem production (NEE) and gross primary production (GPP) compared to control plots (p=0.0194 and p=0.0551, respectively). While CH4 emissions did not significantly differ between treatments, CH4 flux rates were strongly correlated with NEE (p=0.0063) and GPP (p=0.0020), in support of the hypothesis that labile carbon from recent photosynthesis controls patterns of CH4 emissions. The relative importance of plant gas transport and methane consumption rates on CH4 emissions is not known. Methane flux is more tightly correlated with NEE than GPP, which may be explained by increased CH4 consumption or decreased CH4 production as a result of rhizospheric oxidation. The ability to predict future emissions of this important greenhouse gas will be improved by increased understanding of the controls regulating its emission. Future work will focus on developing a tracer technique using SF6 and 13C-labeled CH4 to determine how plant gas transport properties and CH4 consumption contribute to patterns of methane emissions from wetlands.

Influence of vehicular emissions on atmospheric CH4 and NMHC mixing ratios and its correlation with CO and other VOCs tracers in Mexico City

NASA Astrophysics Data System (ADS)

Solano-Murillo, M.; Torres-Jardón, R.; Ruiz-Suárez, L. G.; Barrera-Huertas, H.; Hernandez-Solis, J. M.

2016-12-01

The Mexico City Metropolitan Area (MCMA) is one of the world's largest and most polluted urban areas. A recent GHC emission inventory for MCMA suggests that vehicular emissions contribute with around 37% of CH4, followed by landfills and dump garbage areas (30%) and construction and manufacturing (27%). Contrary to other urban areas, natural gas is not the main fuel used in MCMA, neither for domestic and industrial heating, nor for transportation. Therefore, there is a great uncertainty about who is the main contributor of CH4 emissions. An intensive monitoring campaign of methane (CH4), Non-methane hydrocarbons (NMHC) and carbon monoxide (CO) was performed between February and March 2015 in southwest MCMA. Methane concentrations showed sometimes a diurnal pattern similar to those of CO and to NMHC but most of the time this similarity was lost (CH4 vs CO, R2 = 0.27; CH4 vs NMHC, R2 = 0.28). However, NMHC correlated well with CO (R2 = 0.75). The intercepts of the CH4-CO correlation resulted in [CH4] 1.8 ppm and that of the CO-NMHC correlation in [CO] 0.080 ppb. The lack of agreement between CH4 and CO indicates these species do not come from the same sources. The results suggest that vehicular emissions are not significant contributors to atmospheric CH4 and that the background methane concentration has not change significantly in 25 years. An attempt to correlate some tracers COVs tracers of vehicular and biomass burning with CH4, NMHC and CH4 is done.

Methane Feedback on Atmospheric Chemistry: Methods, Models, and Mechanisms

NASA Astrophysics Data System (ADS)

Holmes, Christopher D.

2018-04-01

The atmospheric methane (CH4) chemical feedback is a key process for understanding the behavior of atmospheric CH4 and its environmental impact. This work reviews how the feedback is defined and used, then examines the meteorological, chemical, and emission factors that control the feedback strength. Geographical and temporal variations in the feedback are described and explained by HOx (HOx = OH + HO2) production and partitioning. Different CH4 boundary conditions used by models, however, make no meaningful difference to the feedback calculation. The strength of the CH4 feedback depends on atmospheric composition, particularly the atmospheric CH4 burden, and is therefore not constant. Sensitivity tests show that the feedback depends very weakly on temperature, insolation, water vapor, and emissions of NO. While the feedback strength has likely remained within 10% of its present value over the industrial era and likely will over the twenty-first century, neglecting these changes biases our understanding of CH4 impacts. Most environmental consequences per kg of CH4 emissions, including its global warming potential (GWP), scale with the perturbation time, which may have grown as much as 40% over the industrial era and continues to rise.

Estimation of wetland methane emissions in a biogeochemical model integrated in CESM: sensitivity analysis and comparison against surface and atmospheric measurements

NASA Astrophysics Data System (ADS)

Meng, L.; Mahowald, N. M.; Hess, P. G.; Yavitt, J. B.; Riley, W. J.; Subin, Z. M.; Lawrence, D. M.; Swenson, S. C.; Jauhiainen, J.; Fuka, D. R.

2012-12-01

Methane emissions from natural wetlands and rice paddies constitute a large proportion of atmospheric methane, but the magnitude and year-to-year variation of these methane sources is still unpredictable. Here we describe and evaluate the integration of a methane biogeochemical model (CLM4Me; Riley et al. 2011) into the Community Land Model 4.0 (CLM4CN) in order to better explain spatial and temporal variations in methane emissions. We test new functions for soil pH and redox potential that impact microbial methane production in soils. We also constrain aerenchyma in plants in always-inundated areas in order to better represent wetland vegetation. Satellite inundated fraction is explicitly prescribed in the model because there are large differences between simulated fractional inundation and satellite observations and thus we do not use CLM4 simulated inundated area. The model is evaluated at the site level with vegetation cover and water table prescribed from measurements. Explicit site level evaluations of simulated methane emissions are quite different than evaluating the grid cell averaged emissions against available measurements. Using a baseline set of parameter values, our model-estimated average global wetland emissions for the period 1993-2004 were 256 Tg CH4 y-1 (including the soil sink). Tropical wetlands contributed 201 Tg CH4 y-1, or 78% of the global wetland flux. Northern latitude (>50N) systems contributed 12 Tg CH4 y-1. Our sensitivity studies show a large range (150-346 Tg CH4 y-1) in predicted global methane emissions. In order to evaluate our methane emissions on the regional and global scales against atmospheric measurements, we conducted simulations with the Community Atmospheric Model with chemistry (CAM-chem) forced with our baseline simulation of wetland and rice paddy emissions along with other methane sources (e.g. anthropogenic, fire, and termite emissions) and compared model simulations against measured atmospheric concentrations obtained from the World Data Centre for Greenhouse Gases (WDCGG) at http://ds.data.jma.go.jp/gmd/wdcgg/. Overall, using our estimated wetland and rice paddy emissions, CAM-chem model can produce seasonal and interannual variations of observed atmospheric concentration performs well. Thus, within the current level of uncertainty, our emissions appear to be reasonable.

Dissolved Organic Carbon: Nitrate Ratios as a Driver of Methane Fluxes in Stream Ecosystems

NASA Astrophysics Data System (ADS)

Sullivan, B. W.; Wymore, A.; Schade, J. D.; McDowell, W. H.

2016-12-01

Fluvial ecosystems are poorly understood components of the global methane (CH4) budget because the ecology of CH4 fluxes in streams has yet to be sufficiently elucidated. Both CH4 production and uptake via oxidation are microbially mediated processes, but it is unclear where in the fluvial environment are the sources and sinks of CH4 and what role terrestrial inputs of carbon (C) and nutrients have on the magnitude and direction of CH4 flux. To address these uncertainties, we measured CH4 fluxes in a laboratory incubation from two temperate headwater streams that differed in ambient dissolved organic carbon (DOC) and nitrate (NO3-) concentrations. We amended stream water and sediment microcosms from each site with labile DOC from senesced leaf litter to assess how DOC concentration and the DOC:NO3- ratio affect proximate controls on CH4 flux. Lastly, we manipulated sediment and water column ratios (0-100%) to estimate sources and fates of CH4 flux within the ecosystem. We measured CH4 fluxes for the first 120 minutes of the incubation to simulate short-term, in stream processes. Initially, streams were a source of methane, but switched to a sink within 120 minutes. Methane fluxes were statistically similar in both stream sediment and water, suggesting that microbial processing of CH4 has similar directionality and magnitude in each environment. Both CH4 oxidation and production were significantly correlated with the DOC: NO3- ratio over the course of the incubation. Early in the incubation, increasing DOC: NO3- increased CH4 flux, but late in the incubation, increasing DOC: NO3- increased CH4 oxidation. Together, our results challenge existing paradigms of CH4 flux in the fluvial environment and identify the DOC:NO3- ratio as a possible mechanism that can explain spatial and temporal CH4 flux patterns in streams.

Evidence for methane production by marine algae (Emiliana huxleyi) and its implication for the methane paradox in oxic waters

NASA Astrophysics Data System (ADS)

Lenhart, K.; Klintzsch, T.; Langer, G.; Nehrke, G.; Bunge, M.; Schnell, S.; Keppler, F.

2015-12-01

Methane (CH4), an important greenhouse gas that affects radiation balance and consequently the earth's climate, still has uncertainties in its sinks and sources. The world's oceans are considered to be a source of CH4 to the atmosphere, although the biogeochemical processes involved in its formation are not fully understood. Several recent studies provided strong evidence of CH4 production in oxic marine and freshwaters but its source is still a topic of debate. Studies of CH4 dynamics in surface waters of oceans and large lakes have concluded that pelagic CH4 supersaturation cannot be sustained either by lateral inputs from littoral or benthic inputs alone. However, frequently regional and temporal oversaturation of surface waters occurs. This comprises the observation of a CH4 oversaturating state within the surface mixed layer, sometimes also termed the "oceanic methane paradox". In this study we considered marine algae as a possible direct source of CH4. Therefore, the coccolithophore Emiliania huxleyi was grown under controlled laboratory conditions and supplemented with two 13C-labelled carbon substrates, namely bicarbonate and a position-specific 13C-labelled methionine (R-S-13CH3). The CH4 production was 0.7 μg POC g-1 d-1, or 30 ng g-1 POC h-1. After supplementation of the cultures with the 13C labelled substrate, the isotope label was observed in headspace-CH4. Moreover, the absence of methanogenic archaea within the algal culture and the oxic conditions during CH4 formation suggest that marine algae such as Emiliania huxleyi contribute to the observed spatial and temporal restricted CH4 oversaturation in ocean surface waters.

Modeling greenhouse gas emissions from dairy farms

USDA-ARS?s Scientific Manuscript database

Dairy farms have been identified as an important source of greenhouse gas emissions. Within the farm, important emissions include enteric methane (CH4) from the animals, CH4 and nitrous oxide (N2O) from manure in housing facilities, during long-term storage and during field application, and N2O from...

Methane Emissions in the London Region: Deciphering Regional Sources with Mobile Measurements

NASA Astrophysics Data System (ADS)

Zazzeri, G.; Lowry, D.; Fisher, R. E.; France, J. L.; Lanoisellé, M.; Bjorkegren, A.; Nisbet, E. G.

2014-12-01

Methane stable isotope analysis, coupled with mole fraction measurement, has been used to link isotopic signature to methane emissions from the leading methane sources in the London region, such as landfills and gas leaks. A mobile Picarro G2301 CRDS analyser was installed in a vehicle, together with an anemometer and a Hemisphere GPS receiver, to measure atmospheric methane mole fractions and their relative location. When methane plumes were located and intercepted, air samples were collected in Tedlar bags, for δ13C-CH4 isotopic analysis by CF-GC-IRMS (Continous Flow-Gas Chromatography-Isotopic Ratio Mass Spectroscopy). This method provides high precision isotopic values, determining δ13C-CH4 to ±0.05 per mil. The bulk signature of the methane plume into the atmosphere from the whole source area was obtained by Keeling plot analysis, and a δ13C-CH4 signature, with the relative uncertainty, allocated to each methane source investigated. The averaged δ13C-CH4 signature for landfill sites around the London region is - 58 ± 3 ‰, whereas the δ13C-CH4 signature for gas leaks is fairly constant at -36 ± 2 ‰, a value characteristic of North Sea supply. The Picarro G2301 analyser was installed also on the roof of King's College London, located in the centre of the city, and connected to an air inlet located 7 meters above roof height. An auto-sampler was connected to the same air inlet and launched remotely when a high nocturnal build up was expected, allowing up to twenty air bags to be collected for methane isotopic analysis over a 24 hour period. The main source contributing to overnight methane build up in central London is fugitive gas, in agreement with inventories. From the isotopic characterisation of urban methane sources and the source mix in London, the contribution to the urban methane budget and the local distribution of the methane sources given in inventories can be validated.

High Temporal and Spatial Variability of Atmospheric-Methane Oxidation in Alpine Glacier Forefield Soils

PubMed Central

Chiri, Eleonora; Nauer, Philipp A.; Rainer, Edda-Marie; Zeyer, Josef

2017-01-01

ABSTRACT Glacier forefield soils can provide a substantial sink for atmospheric CH4, facilitated by aerobic methane-oxidizing bacteria (MOB). However, MOB activity, abundance, and community structure may be affected by soil age, MOB location in different forefield landforms, and temporal fluctuations in soil physical parameters. We assessed the spatial and temporal variability of atmospheric-CH4 oxidation in an Alpine glacier forefield during the snow-free season of 2013. We quantified CH4 flux in soils of increasing age and in different landforms (sandhill, terrace, and floodplain forms) by using soil gas profile and static flux chamber methods. To determine MOB abundance and community structure, we employed pmoA gene-based quantitative PCR and targeted amplicon sequencing. Uptake of CH4 increased in magnitude and decreased in variability with increasing soil age. Sandhill soils exhibited CH4 uptake rates ranging from −3.7 to −0.03 mg CH4 m−2 day−1. Floodplain and terrace soils exhibited lower uptake rates and even intermittent CH4 emissions. Linear mixed-effects models indicated that soil age and landform were the dominating factors shaping CH4 flux, followed by cumulative rainfall (weighted sum ≤4 days prior to sampling). Of 31 MOB operational taxonomic units retrieved, ∼30% were potentially novel, and ∼50% were affiliated with upland soil clusters gamma and alpha. The MOB community structures in floodplain and terrace soils were nearly identical but differed significantly from the highly variable sandhill soil communities. We concluded that soil age and landform modulate the soil CH4 sink strength in glacier forefields and that recent rainfall affects its short-term variability. This should be taken into account when including this environment in future CH4 inventories. IMPORTANCE Oxidation of methane (CH4) in well-drained, “upland” soils is an important mechanism for the removal of this potent greenhouse gas from the atmosphere. It is largely mediated by aerobic, methane-oxidizing bacteria (MOB). Whereas there is abundant information on atmospheric-CH4 oxidation in mature upland soils, little is known about this important function in young, developing soils, such as those found in glacier forefields, where new sediments are continuously exposed to the atmosphere as a result of glacial retreat. In this field-based study, we investigated the spatial and temporal variability of atmospheric-CH4 oxidation and associated MOB communities in Alpine glacier forefield soils, aiming at better understanding the factors that shape the sink for atmospheric CH4 in this young soil ecosystem. This study contributes to the knowledge on the dynamics of atmospheric-CH4 oxidation in developing upland soils and represents a further step toward the inclusion of Alpine glacier forefield soils in global CH4 inventories. PMID:28687652

High temporal and spatial variability of atmospheric-methane oxidation in Alpine glacier-forefield soils.

PubMed

Chiri, Eleonora; Nauer, Philipp A; Rainer, Edda-Marie; Zeyer, Josef; Schroth, Martin H

2017-07-07

Glacier-forefield soils can provide a substantial sink for atmospheric CH 4 , facilitated by aerobic methane-oxidizing bacteria (MOB). However, MOB activity, abundance, and community structure may be affected by soil age, location in different forefield landforms, and temporal fluctuations in soil-physical parameters. We assessed spatial and temporal variability of atmospheric CH 4 oxidation in an Alpine glacier forefield during the snow-free season 2013. We quantified CH 4 flux in soils of increasing age and in different landforms (sandhill, terrace, floodplain) using soil-gas-profile and static flux-chamber methods. To determine MOB abundance and community structure, we employed pmoA -gene-based quantitative PCR and targeted-amplicon sequencing. Uptake of CH 4 increased in magnitude and decreased in variability with increasing soil age. Sandhill soils exhibited CH 4 uptake ranging from -0.03- -3.7 mg CH 4 m -2 d -1 Floodplain and terrace soils exhibited smaller uptake and even intermittent CH 4 emissions. Linear mixed-effect models indicated that soil age and landform were dominating factors shaping CH 4 flux, followed by cumulative rainfall (weighted sum ≤ 4 d prior to sampling). Of 31 MOB operational taxonomic units retrieved, ∼30% were potentially novel, and ∼50% were affiliated with Upland Soil Clusters gamma and alpha. The MOB community structures in floodplain and terrace soils were nearly identical, but differed significantly from highly variable sandhill-soil communities. We conclude that soil age and landform modulate the soil CH 4 sink strength in glacier forefields, and recent rainfall affects its short-term variability. This should be taken into account when including this environment in future CH 4 inventories. Importance Oxidation of methane (CH 4 ) in well-drained, "upland" soils is an important mechanism for the removal of this potent greenhouse gas from the atmosphere. It is largely mediated by aerobic, methane-oxidizing bacteria (MOB). Whereas there is abundant information on atmospheric CH 4 oxidation in mature upland soils, little is known about this important function in young, developing soils such as those found in glacier forefields, where new sediments are continuously exposed to the atmosphere as a result of glacial retreat.In this field-based study we investigated spatial and temporal variability of atmospheric CH 4 oxidation and associated MOB communities in Alpine glacier-forefield soils, aiming at better understanding factors that shape the sink for atmospheric CH 4 in this young soil ecosystem. The study contributes to the knowledge on the dynamics of atmospheric CH 4 oxidation in developing upland soils, and represents a further step towards the inclusion of Alpine glacier-forefield soils in global CH 4 inventories. Copyright © 2017 American Society for Microbiology.

Data-Constrained Projections of Methane Fluxes in a Northern Minnesota Peatland in Response to Elevated CO 2 and Warming

DOE PAGES

Ma, Shuang; Jiang, Jiang; Huang, Yuanyuan; ...

2017-10-20

Large uncertainties exist in predicting responses of wetland methane (CH 4) fluxes to future climate change. However, sources of the uncertainty have not been clearly identified despite the fact that methane production and emission processes have been extensively explored. In this study, we took advantage of manual CH 4 flux measurements under ambient environment from 2011 to 2014 at the Spruce and Peatland Responses Under Changing Environments (SPRUCE) experimental site and developed a data-informed process-based methane module. The module was incorporated into the Terrestrial ECOsystem (TECO) model before its parameters were constrained with multiple years of methane flux data formore » forecasting CH 4 emission under five warming and two elevated CO 2 treatments at SPRUCE. We found that 9°C warming treatments significantly increased methane emission by approximately 400%, and elevated CO 2 treatments stimulated methane emission by 10.4%–23.6% in comparison with ambient conditions. The relative contribution of plant-mediated transport to methane emission decreased from 96% at the control to 92% at the 9°C warming, largely to compensate for an increase in ebullition. The uncertainty in plant-mediated transportation and ebullition increased with warming and contributed to the overall changes of emissions uncertainties. At the same time, our modeling results indicated a significant increase in the emitted CH 4:CO 2 ratio. This result, together with the larger warming potential of CH 4, will lead to a strong positive feedback from terrestrial ecosystems to climate warming. In conclusion, the model-data fusion approach used in this study enabled parameter estimation and uncertainty quantification for forecasting methane fluxes.« less

Data-Constrained Projections of Methane Fluxes in a Northern Minnesota Peatland in Response to Elevated CO2 and Warming

NASA Astrophysics Data System (ADS)

Ma, Shuang; Jiang, Jiang; Huang, Yuanyuan; Shi, Zheng; Wilson, Rachel M.; Ricciuto, Daniel; Sebestyen, Stephen D.; Hanson, Paul J.; Luo, Yiqi

2017-11-01

Large uncertainties exist in predicting responses of wetland methane (CH4) fluxes to future climate change. However, sources of the uncertainty have not been clearly identified despite the fact that methane production and emission processes have been extensively explored. In this study, we took advantage of manual CH4 flux measurements under ambient environment from 2011 to 2014 at the Spruce and Peatland Responses Under Changing Environments (SPRUCE) experimental site and developed a data-informed process-based methane module. The module was incorporated into the Terrestrial ECOsystem (TECO) model before its parameters were constrained with multiple years of methane flux data for forecasting CH4 emission under five warming and two elevated CO2 treatments at SPRUCE. We found that 9°C warming treatments significantly increased methane emission by approximately 400%, and elevated CO2 treatments stimulated methane emission by 10.4%-23.6% in comparison with ambient conditions. The relative contribution of plant-mediated transport to methane emission decreased from 96% at the control to 92% at the 9°C warming, largely to compensate for an increase in ebullition. The uncertainty in plant-mediated transportation and ebullition increased with warming and contributed to the overall changes of emissions uncertainties. At the same time, our modeling results indicated a significant increase in the emitted CH4:CO2 ratio. This result, together with the larger warming potential of CH4, will lead to a strong positive feedback from terrestrial ecosystems to climate warming. The model-data fusion approach used in this study enabled parameter estimation and uncertainty quantification for forecasting methane fluxes.

Data-Constrained Projections of Methane Fluxes in a Northern Minnesota Peatland in Response to Elevated CO 2 and Warming

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ma, Shuang; Jiang, Jiang; Huang, Yuanyuan

Large uncertainties exist in predicting responses of wetland methane (CH 4) fluxes to future climate change. However, sources of the uncertainty have not been clearly identified despite the fact that methane production and emission processes have been extensively explored. In this study, we took advantage of manual CH 4 flux measurements under ambient environment from 2011 to 2014 at the Spruce and Peatland Responses Under Changing Environments (SPRUCE) experimental site and developed a data-informed process-based methane module. The module was incorporated into the Terrestrial ECOsystem (TECO) model before its parameters were constrained with multiple years of methane flux data formore » forecasting CH 4 emission under five warming and two elevated CO 2 treatments at SPRUCE. We found that 9°C warming treatments significantly increased methane emission by approximately 400%, and elevated CO 2 treatments stimulated methane emission by 10.4%–23.6% in comparison with ambient conditions. The relative contribution of plant-mediated transport to methane emission decreased from 96% at the control to 92% at the 9°C warming, largely to compensate for an increase in ebullition. The uncertainty in plant-mediated transportation and ebullition increased with warming and contributed to the overall changes of emissions uncertainties. At the same time, our modeling results indicated a significant increase in the emitted CH 4:CO 2 ratio. This result, together with the larger warming potential of CH 4, will lead to a strong positive feedback from terrestrial ecosystems to climate warming. In conclusion, the model-data fusion approach used in this study enabled parameter estimation and uncertainty quantification for forecasting methane fluxes.« less

The lipid response of aerobic marine methanotroph communities under changing environmental conditions.

NASA Astrophysics Data System (ADS)

Rush, D.; Villanueva, L.; van der Meer, M.; S Sinninghe Damsté, J.

2017-12-01

Methane (CH4) originating from marine environments accounts for a significant amount of atmospheric greenhouse gas. Aerobic methanotrophs, which convert CH4 to CO­2, are responsible for quenching a part of this methane before its release. Modern-day climate projections show a rapid shift towards a warmer, more acidic ocean. How do these important methanotrophic communities respond to such changes to their environment? Here, we present the results of microcosm experiments from three marine regions influenced by CH4. Particulate organic matter and sediment were collected from the Black Sea, the Baltic Sea, and the North Sea, at depths ideal for aerobic methanotroph communities at the time of sampling (e.g. oxic, in area of active CH4 release). These were incubated under different temperatures, pHs, and labelled 13CH4 concentrations. We monitored methane concentration in these microcosms as an indication of 13CH4 consumption by methanotrophs. Once the methane concentration was <0.1%, incubations were terminated. We will trace isotopically heavy 13C in the DNA and lipids of the organisms oxidising methane in order to elucidate which organisms are performing methane oxidation and whether they synthesize specific biomarker lipids. Particular attention will be paid to the abundances and diversity of bacteriohopanepolyol lipids, known methanotroph biomarkers. The ultimate goal of our investigation is to determine the effect changes in these environmental parameters have on aerobic methanotroph community structures and their lipid fingerprints. By establishing reliable biomarker lipids for aerobic methanotrophy at certain conditions, we will then be able to investigate the contribution of aerobic methanotrophy throughout Earth's history, especially at times when CH4 concentrations were higher than they are at present.

Aquatic methane dynamics in a human-impacted river-floodplain of the Danube.

PubMed

Sieczko, Anna Katarzyna; Demeter, Katalin; Singer, Gabriel Andreas; Tritthart, Michael; Preiner, Stefan; Mayr, Magdalena; Meisterl, Karin; Peduzzi, Peter

2016-11-01

River-floodplain systems are characterized by changing hydrological connectivity and variability of resources delivered to floodplain water bodies. Although the importance of hydrological events has been recognized, the effect of flooding on CH 4 concentrations and emissions from European, human-impacted river-floodplains is largely unknown. This study evaluates aquatic concentrations and emissions of CH 4 from a highly modified, yet partly restored river-floodplain system of the Danube near Vienna (Austria). We covered a broad range of hydrological conditions, including a 1-yr flood event in 2012 and a 100-yr flood in 2013. Our findings demonstrate that river-floodplain waters were supersaturated with CH 4 , hence always serving as a source of CH 4 to the atmosphere. Hydrologically isolated habitats in general have higher concentrations and produce higher fluxes despite lower physically defined velocities. During surface connection, however, CH 4 is exported from the floodplain to the river, suggesting that the main channel serves as an "exhaust pipe" for the floodplain. This mechanism was especially important during the 100-yr flood, when a clear pulse of CH 4 was flushed from the floodplain with surface floodwaters. Our results emphasize the importance of floods differing in magnitude for methane evasion from river-floodplains; 34% more CH 4 was emitted from the entire system during the year with the 100-yr flood compared to a hydrologically "normal" year. Compared to the main river channel, semiisolated floodplain waters were particularly strong sources of CH 4 . Our findings also imply that the predicted increased frequency of extreme flooding events will have significant consequences for methane emission from river-floodplain systems.

Modelling the Effect of Diet Composition on Enteric Methane Emissions across Sheep, Beef Cattle and Dairy Cows

PubMed Central

Bell, Matt; Eckard, Richard; Moate, Peter J.; Yan, Tianhai

2016-01-01

Simple Summary Enteric methane emissions produced by ruminant livestock has gained global interest due to methane being a potent greenhouse gas and ruminants being a significant source of emissions. In the absence of measurements, prediction models can facilitate the estimation of enteric methane emissions from ruminant livestock and aid investigation of mitigation options. This study developed a practical method using feed analysis information for predicting enteric methane emissions from sheep, beef cattle and dairy cows fed diets encompassing a wide range of nutrient concentrations. Abstract Enteric methane (CH4) is a by-product from fermentation of feed consumed by ruminants, which represents a nutritional loss and is also considered a contributor to climate change. The aim of this research was to use individual animal data from 17 published experiments that included sheep (n = 288), beef cattle (n = 71) and dairy cows (n = 284) to develop an empirical model to describe enteric CH4 emissions from both cattle and sheep, and then evaluate the model alongside equations from the literature. Data were obtained from studies in the United Kingdom (UK) and Australia, which measured enteric CH4 emissions from individual animals in calorimeters. Animals were either fed solely forage or a mixed ration of forage with a compound feed. The feed intake of sheep was restricted to a maintenance amount of 875 g of DM per day (maintenance level), whereas beef cattle and dairy cows were fed to meet their metabolizable energy (ME) requirement (i.e., production level). A linear mixed model approach was used to develop a multiple linear regression model to predict an individual animal’s CH4 yield (g CH4/kg dry matter intake) from the composition of its diet. The diet components that had significant effects on CH4 yield were digestible organic matter (DOMD), ether extract (EE) (both g/kg DM) and feeding level above maintenance intake: CH4 (g/kg DM intake) = 0.046 (±0.001) × DOMD − 0.113 (±0.023) × EE − 2.47 (±0.29) × (feeding level − 1), with concordance correlation coefficient (CCC) = 0.655 and RMSPE = 14.0%. The predictive ability of the model developed was as reliable as other models assessed from the literature. These components can be used to predict effects of diet composition on enteric CH4 yield from sheep, beef and dairy cattle from feed analysis information. PMID:27618107

Estimating global natural wetland methane emissions using process modelling: spatio-temporal patterns and contributions to atmospheric methane fluctuations

USGS Publications Warehouse

Zhu, Qiuan; Peng, Changhui; Chen, Huai; Fang, Xiuqin; Liu, Jinxun; Jiang, Hong; Yang, Yanzheng; Yang, Gang

2015-01-01

Aim The fluctuations of atmospheric methane (CH4) that have occurred in recent decades are not fully understood, particularly with regard to the contribution from wetlands. The application of spatially explicit parameters has been suggested as an effective method for reducing uncertainties in bottom-up approaches to wetland CH4 emissions, but has not been included in recent studies. Our goal was to estimate spatio-temporal patterns of global wetland CH4 emissions using a process model and then to identify the contribution of wetland emissions to atmospheric CH4fluctuations. Location Global. Methods A process-based model integrated with full descriptions of methanogenesis (TRIPLEX-GHG) was used to simulate global wetland CH4emissions. Results Global annual wetland CH4 emissions ranged from 209 to 245 Tg CH4 year−1 between 1901 and 2012, with peaks occurring in 1991 and 2012. There is a decreasing trend between 1990 and 2010 with a rate of approximately 0.48 Tg CH4 year−1, which was largely caused by emissions from tropical wetlands showing a decreasing trend of 0.44 Tg CH4 year−1 since the 1970s. Emissions from tropical, temperate and high-latitude wetlands comprised 59, 26 and 15% of global emissions, respectively. Main conclusion Global wetland CH4 emissions, the interannual variability of which was primary controlled by tropical wetlands, partially drive the atmosphericCH4 burden. The stable to decreasing trend in wetland CH4 emissions, a result of a balance of emissions from tropical and extratropical wetlands, was a particular factor in slowing the atmospheric CH4 growth rate during the 1990s. The rapid decrease in tropical wetland CH4emissions that began in 2000 was supposed to offset the increase in anthropogenic emissions and resulted in a relatively stable level of atmospheric CH4 from 2000 to 2006. Increasing wetland CH4 emissions, particularly after 2010, should be an important contributor to the growth in atmospheric CH4 seen since 2007.

Investigation of Wyoming Bentonite Hydration in Dry to Water-Saturated Supercritical CH4 and CH4/CO2 Mixtures: Implications for CO2-Enhanced Gas Production

NASA Astrophysics Data System (ADS)

Loring, J.; Thompson, C.; Ilton, E. S.; McGrail, B. P.; Schaef, T.

2014-12-01

Injection of CO2 into low permeability shale formations leads to additional gas recovery and reduces the flux of CO2 into the atmosphere, thus combining a strong economic incentive with a permanent storage option for CO2. Reduced formation transmissivity due to clay swelling is a concern in CO2 -enhanced gas production. Clay minerals partly determine the physical (i.e. permeability, brittleness) and certain chemical properties (i.e. wetting ability, gas adsorption) of shales, and montmorillonites are of particular interest because they swell by the uptake of species in their interlayer. In this study, the hydration and expansion of a Na-saturated montmorillonite (Na-SWy-2) in high-pressure (90 bar) and moderate temperature (50 °C) methane and mixtures of methane and carbon dioxide were investigated usingCH4 IR spectroscopic titrations andCH4 XRD. The goals were to (1) determine if the hydration/expansion behavior of the clay in supercritical methane is different than in supercritical CO2, (2) determine if methane intercalates the clay, and (3) probe the effects of increasing CO2 concentrations. IR spectra were collected as Na-SWy-2 was titrated with water under several fluid exposures: pure methane, 25, 50, and 75 mole% CO2 in methane, and pure CO2. ComplementaryCH4 XRD experiments were conducted in the same fluids at discrete dissolved water concentrations to measure the d001 values of the clay and thus its volume change on hydration and CH4 and/or CO2 intercalation. In pure methane, no direct evidence of CH4 intercalation was detected in CH bending or stretching regions of the IR spectra. Similarly, in situ XRD indicated the montmorillonite structure was stable in the presence of CH4 and no measurable changes to the basal spacing were observed. However, under low water conditions where the montmorillonite structure was partially expanded (~sub 1W), the IR data indicated a rapid intercalation of CO2 into the interlayer, even with fluid mixtures containing the lowest concentrations of CO2. Likewise,CH4 XRD showed indirect evidence of CO2 intercalation from an increase in the basal spacing from 11.8 to 12.3 under identical conditions. These findings demonstrate that water and CO2 intercalation processes could lead to permeability changes that directly impact methane transmissivity in shales.

Evaluation of shallow sediment methane cycling in a pockmark field on the Chatham Rise, New Zealand

NASA Astrophysics Data System (ADS)

Coffin, R. B.; Rose, P. S.; Klaucke, I.; Bialas, J.; Pecher, I. A.; Gorman, A. R.

2014-12-01

Seismic studies have identified an extensive field (>20,000 km2) of seafloor depressions, or pockmarks, on the southwestern flank of the Chatham Rise, New Zealand. It has been suggested that these pockmarks result from gas hydrate dissociation linked to sea-level changes during glacial-interglacial cycles. Gas hydrates are predominately composed of methane (CH4), a potent greenhouse gas. Surface sediment cores (~ 8 m) were collected from the pockmark field on the Chatham Rise during a research cruise in February 2013 to evaluate the association of the features with CH4 releases. A suite of geochemical parameters are interpreted to determine the methane contribution to solid phase sediment and pore water. The upward flux of CH4 in sediments is often quantified using pore water sulfate (SO42-) profiles, assuming steady-state consumption of SO42- and CH4 by anaerobic oxidation of methane (AOM): CH4 + SO42- → HCO3- + HS- + H2O. This reaction is one of the primary controls on CH4 distributions in sediments. This work will present pore water SO42-, sulfide (HS-) and chloride (Cl-) depth profiles in sediment collected from the pockmark field. Theoretical SO42- distributions in the absence of AOM are compared to observed SO42- profiles as a preliminary assessment of the influence of CH4 on sediment geochemistry in and around the seafloor depressions. In addition isotopically-light CH4 is incorporated into sediment carbon pools via AOM and subsequent CO2 fixation. Stable carbon isotope distributions in the organic and inorganic carbon pools are presented to determine the influence of CH4 in sediments in the vicinty of the pockmarks. Collectively, the geochemical data are used to assess the role of gas hydate dissociation in pockmark formation on the Chatham Rise. Despite sesimic data interpretation in this region there is no modern day contribution of CH4 to shallow sediment carbon cycling and data are presented to assess paleogeochemical methane cycling.

Assessing Methane Fluxes in a Small Run-of-River Reservoir: The Importance of Adjacent Marshland

NASA Astrophysics Data System (ADS)

McGinnis, D. F.; Flury, S.; Fietzek, P.; Bilsley, N. A.; Bodmer, P.; Premke, K.; Maeck, A.; Lorke, A.; Schmidt, M.

2013-12-01

We investigate methane (CH4) emissions from a small run-of-river impoundment, the Schwentine River in Kiel, Germany. Small dammed rivers, while important regions for carbon transformation, are presently not considered in the terrestrial carbon budget and are under-represented in CH4 emission studies. Using state-of-the-art monitoring techniques, we determine that 1) the CH4 emissions well-exceed those reported for temperate reservoirs and 2) the hydrodynamic linkage to bordering marshland (consisting of reed belts, sidebays and creeks) is an important CH4 source for Schwentine River CH4. During our study, the Schwentine River discharged into the Kieler Fjord at 3 - 12 m3/s. CH4 measurements included 1) a moored sensor near the dam discharge, 2) discrete water sampling, and 3) real time surface flux measurements with floating chambers. We observed that the CH4 concentration increased nearly linearly from 2.5 km upstream towards the dam. The CH4 concentration near the dam discharge was logged and reported every 30 minutes nearly continuously from 11 July - 28 Sept 2011, and varied from 500 μmol/L to 2,200 μmol/L. Surprisingly, the CH4 mass discharge from the dam - ranging from 4 to 20 kg/day - increased with both temperature and flowrate, suggesting a flow-dependent CH4 source. We found that the bordering and numerous inundated reed belts, sidebays and small creeks, had significantly elevated CH4 concentrations. These marshland regions are relatively productive and quiescent compared to the main river, and trap organic and particulate matter, leading to enhanced CH4 production. As the river flowrate increases, the lateral exchange with these adjacent areas also increases. Using the CH4 concentration time series, measured surface diffusive and ebullition fluxes, and sediment CH4 porewater profiles, we estimate the relative contributions of CH4 in the main branch due to 1) sediment diffusion, 2) dissolution from sediment CH4 bubble release, and 3) lateral fluxes from the marshland. Damming of the rivers potentially creates or increases adjacent marshland, leading to methane production/emission hotspots. Considering only the main branch, the Schwentine River CH4 emission rate is similar to tropical reservoirs. However, including bubble and diffusive emissions from the reed belts and many small side bays and streams could significantly increase this estimate. As millions of such small river impoundments exist worldwide, we discuss the hydrodynamic alterations promoting CH4 production/emission hotspots, illustrate the importance of collecting high-resolution time series data for assessing emissions, and finally estimate the potential contribution of these small aquatic systems to the global terrestrial carbon balance.

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

NASA Astrophysics Data System (ADS)

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.

Hourly methane production in finishing steers fed at different levels of dry matter intake

USDA-ARS?s Scientific Manuscript database

Methane (CH4) loss from finishing cattle is important as it represents an energy loss that could be used for maintenance and growth, and CH4 is a greenhouse gas with a global warming potential 21 to 25 times that of CO2. Our objectives were to determine hourly CH4 production from growing cattle fed...

Plume mapping and isotopic characterisation of anthropogenic methane sources

NASA Astrophysics Data System (ADS)

Zazzeri, G.; Lowry, D.; Fisher, R. E.; France, J. L.; Lanoisellé, M.; Nisbet, E. G.

2015-06-01

Methane stable isotope analysis, coupled with mole fraction measurement, has been used to link isotopic signature to methane emissions from landfill sites, coal mines and gas leaks in the United Kingdom. A mobile Picarro G2301 CRDS (Cavity Ring-Down Spectroscopy) analyser was installed on a vehicle, together with an anemometer and GPS receiver, to measure atmospheric methane mole fractions and their relative location while driving at speeds up to 80 kph. In targeted areas, when the methane plume was intercepted, air samples were collected in Tedlar bags, for δ13C-CH4 isotopic analysis by CF-GC-IRMS (Continuous Flow Gas Chromatography-Isotope Ratio Mass Spectrometry). This method provides high precision isotopic values, determining δ13C-CH4 to ±0.05 per mil. The bulk signature of the methane plume into the atmosphere from the whole source area was obtained by Keeling plot analysis, and a δ13C-CH4 signature, with the relative uncertainty, allocated to each methane source investigated. Both landfill and natural gas emissions in SE England have tightly constrained isotopic signatures. The averaged δ13C-CH4 for landfill sites is -58 ± 3‰. The δ13C-CH4 signature for gas leaks is also fairly constant around -36 ± 2‰, a value characteristic of homogenised North Sea supply. In contrast, signatures for coal mines in N. England and Wales fall in a range of -51.2 ± 0.3‰ to -30.9 ± 1.4‰, but can be tightly constrained by region. The study demonstrates that CRDS-based mobile methane measurement coupled with off-line high precision isotopic analysis of plume samples is an efficient way of characterising methane sources. It shows that isotopic measurements allow type identification, and possible location of previously unknown methane sources. In modelling studies this measurement provides an independent constraint to determine the contributions of different sources to the regional methane budget and in the verification of inventory source distribution.

Coupling a Neural Network with Atmospheric Flow Simulations to Locate and Quantify CH4 Emissions at Well Pads

NASA Astrophysics Data System (ADS)

Travis, B. J.; Sauer, J.; Dubey, M. K.

2017-12-01

Methane (CH4) leaks from oil and gas production fields are a potentially significant source of atmospheric methane. US DOE's ARPA-E office is supporting research to locate methane emissions at 10 m size well pads to within 1 m. A team led by Aeris Technologies, and that includes LANL, Planetary Science Institute and Rice University has developed an autonomous leak detection system (LDS) employing a compact laser absorption methane sensor, a sonic anemometer and multiport sampling. The LDS system analyzes monitoring data using a convolutional neural network (cNN) to locate and quantify CH4 emissions. The cNN was trained using three sources: (1) ultra-high-resolution simulations of methane transport provided by LANL's coupled atmospheric transport model HIGRAD, for numerous controlled methane release scenarios and methane sampling configurations under variable atmospheric conditions, (2) Field tests at the METEC site in Ft. Collins, CO., and (3) Field data from other sites where point-source surface methane releases were monitored downwind. A cNN learning algorithm is well suited to problems in which the training and observed data are noisy, or correspond to complex sensor data as is typical of meteorological and sensor data over a well pad. Recent studies with our cNN emphasize the importance of tracking wind speeds and directions at fine resolution ( 1 second), and accounting for variations in background CH4 levels. A few cases illustrate the importance of sufficiently long monitoring; short monitoring may not provide enough information to determine accurately a leak location or strength, mainly because of short-term unfavorable wind directions and choice of sampling configuration. Length of multiport duty cycle sampling and sample line flush time as well as number and placement of monitoring sensors can significantly impact ability to locate and quantify leaks. Source location error at less than 10% requires about 30 or more training cases.

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

NASA Astrophysics Data System (ADS)

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

2016-09-01

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

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

PubMed

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

2016-09-26

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

Year-round methane emissions from permafrost in a North-east Siberian region

NASA Astrophysics Data System (ADS)

Castro-Morales, Karel; Kaiser, Sonja; Kleinen, Thomas; Kwon, Min Jung; Kittler, Fanny; Zaehle, Sönke; Beer, Christian; Göckede, Mathias

2017-04-01

In recent decades, permafrost regions in northern latitudes are thawing as a response of climate warming. Soils in permafrost areas contain vast amounts of organic material that is released into the environment after thaw, providing new labile material for bacterial decomposition. As a result, higher production of methane in the anoxic soil layers and within anaerobic wetlands is anticipated, and this will be further released to the atmosphere. In order to assess the current large-scale methane emissions from a wetland permafrost-thaw affected area, we present results of year-round simulated methane emissions at regional scale for a section at the Russian far Northeast in Siberia, located in the low Arctic tundra and characterized by continuous permafrost. For this we use a newly developed process-based methane model built in the framework of the land surface model JSBACH. The model contains explicit permafrost processes and an improved representation of the horizontal extent of wetlands with a hydrological model (TOPMODEL). Model simulated distribution and horizontal extent of wetlands is evaluated against high-resolution remote sensing data. Total and individual regional methane emissions by ebullition, molecular diffusion, plant-mediated and emissions through snow are presented for 2014 and 2015. The model shows a reasonable seasonal transition between the individual methane emission paths. Most of the methane emissions to the atmosphere occur in summer (July, August, September), with the peak of the emissions during August. In this month, plant-mediated transport is the dominant emission path with about 15 mg CH4 m-2 d-1 in 2014, followed by ebullition (7 mg CH4 m-2 d-1) accounting for about half of the emissions thorough plants. Molecular diffusion is a minor contributor with only 0.006 mg CH4 m-2 d-1 at the peak of the summer emissions. Methane emissions through snow occur only during spring, fall and winter months, with higher emissions in spring and autumn (max. 2 mg CH4 m-2 d-1) when the thickness of the snow layer starts to melt or accumulate, respectively. The performance of the model was evaluated by comparing the modeled total methane emissions from a section of the Kolyma river floodplain near Chersky, against methane fluxes obtained from eddy covariance (for 2014 and 2015) and chambers (for June - August 2014) measured in the same area. Model results agree well with observations, with the highest emissions during August each year with 92.3 mg CH4 m-2 d-1 from eddy fluxes, 72.5 mg CH4 m-2 d-1 from chambers and 79.0 mg CH4 m-2 d-1 from the model in 2014, while 64.4 mg CH4 m-2 d-1 from eddy and 66.3 mg CH4 m-2 d-1 from the model in August 2015. The model underestimates winter emissions by up to 15 mg CH4 m-2 d-1, however a better agreement is observed in April 2014. To understand the shortcomings of the model against observations, the heterogeneity between model grid cells will be discussed.

Effects of algal-derived carbon on sediment methane ...

EPA Pesticide Factsheets

Nutrient loading is known to have adverse consequences for aquatic ecosystems, particularly in the form of algal blooms that may result. These blooms pose problems for humans and wildlife, including harmful toxin release, aquatic hypoxia and increased costs for water treatment. Another potential disservice resulting from algal blooms is the enhanced production of methane (CH4), a potent greenhouse gas, in aquatic sediments. Laboratory experiments have shown that algal biomass additions to sediment cores increase rates of CH4 production, but it is unclear whether or not this effect occurs at the ecosystem scale. The goal of this research was to explore the link between algal-derived carbon and methane production in the sediment of a eutrophic reservoir located in southwest Ohio, using a sampling design that capitalized on spatial and temporal gradients in autochthonous carbon input to sediments. Specifically, we aimed to determine if the within-reservoir gradient of sediment algal-derived organic matter and sediment CH4 production rates correlate. This was done by retrieving sediment cores from 15 sites within the reservoir along a known gradient of methane emission rates, at two separate time points in 2016: late spring before the sediments had received large amounts of algal input and mid-summer after algal blooms had been prevalent in the reservoir. Potential CH4 production rates, sediment organic matter source, and microbial community composition were charac

Eddy covariance measurements of the net turbulent methane flux in the city centre - results of 2-year campaign in Łódź, Poland

NASA Astrophysics Data System (ADS)

Pawlak, Włodzimierz; Fortuniak, Krzysztof

2016-07-01

To investigate temporal variability of methane (CH4) fluxes in an urban environment, air-surface exchange fluxes of CH4 were continuously measured using eddy covariance techniques at a city-centre site in Łódź, Poland, from July 2013 to August 2015. In the immediate vicinity of the measurement site, potential methane sources include vehicle traffic, dense sewerage infrastructure and natural gas networks. Sensible and latent heat fluxes have also been measured since 2000 and carbon dioxide fluxes since 2007 at this site. Upward CH4 fluxes dominated during the measurement period, indicating that the city centre is a net source of CH4 to the troposphere. The highest monthly fluxes were observed in winter (2.0 to 2.7 g m-2 month-1) and the lowest in summer (0.8 to 1.0 g m-2 month-1). Fluxes on working days were around 6 % higher than on weekends. The cumulative flux indicates that the city centre emitted a net quantity of nearly 18 g m-2 of CH4 in 2014. Stable values of the FCO2/ FCH4 ratio in months (minimum 2.41 × 10-3, maximum 5.3 × 10-3) and the lack of a clear annual course suggest comparable magnitude of both fluxes.

The Relative Abundances of Resolved 12CH2D2 and 13CH3D and Mechanisms Controlling Isotopic Bond Ordering in Abiotic and Biotic Methane Gases

NASA Astrophysics Data System (ADS)

Young, E. D.; Kohl, I. E.; Sherwood Lollar, B.; Etiope, G.; Rumble, D.; Li, S.; Haghnegahdar, M. A.; Schauble, E. A.; McCain, K.; Foustoukos, D.; Sutcliffe, C. N.; Warr, O.; Ballentine, C. J.; Onstott, T. C.; Hosgormez, H.; Neubeck, A.; Marques, J. M.; Perez-Rodriguez, I. M.; Rowe, A. R.; LaRowe, D.; Magnabosco, C.; Bryndzia, T.

2016-12-01

We report measurements of resolved 12CH2D2 and 13CH3D at natural abundances in a variety of methane gases produced naturally and in the laboratory. The ability to resolve 12CH2D2 from 13CH3D provides unprecedented insights into the origin and evolution of CH4. The results identify conditions under which either isotopic bond order disequilibrium or equilibrium are expected. Where equilibrium obtains, concordant Δ12CH2D2 and Δ13CH3D temperatures can be used reliably for thermometry. We find that concordant temperatures do not always match previous hypotheses based on indirect estimates of temperature of formation nor temperatures derived from CH4/H2 D/H exchange, underscoring the importance of reliable thermometry based on the CH4 molecules themselves. Where Δ12CH2D2 and Δ13CH3D values are inconsistent with thermodynamic equilibrium, temperatures of formation derived from these species are spurious. In such situations, while formation temperatures are unavailable, disequilibrium isotopologue ratios nonetheless provide important information about the formation mechanism of the gas and the presence or absence of multiple sources or sinks. In particular, disequilibrium isotopologue ratios may provide the means for differentiating between methane produced by abiotic synthesis versus biological processes. Deficits in 12CH2D2 compared with equilibrium values in CH4 gas made by surface-catalyzed abiotic reactions are so large as to point towards a quantum tunneling origin. Tunneling also accounts for the more moderate depletions in 13CH3D that accompany the low 12CH2D2 abundances produced by abiotic reactions. The tunneling signature of abiotic CH4 formation may prove to be an important tracer of abiotic methane formation, especially where it is preserved by dissolution of gas in cool hydrothermal systems (e.g., Mars). Isotopologue signatures of abiotic methane production can be erased by infiltration of microbial communities, and Δ12CH2D2 values are a key tracer of microbial recycling.

Mobile mapping of methane emissions and isoscapes

NASA Astrophysics Data System (ADS)

Takriti, Mounir; Ward, Sue; Wynn, Peter; Elias, Dafydd; McNamara, Niall

2017-04-01

Methane (CH4) is a potent greenhouse gas emitted from a variety of natural and anthropogenic sources. It is crucial to accurately and efficiently detect CH4 emissions and identify their sources to improve our understanding of changing emission patterns as well as to identify ways to curtail their release into the atmosphere. However, using established methods this can be challenging as well as time and resource intensive due to the temporal and spatial heterogeneity of many sources. To address this problem, we have developed a vehicle mounted mobile system that combines high precision CH4 measurements with isotopic mapping and dual isotope source characterisation. We here present details of the development and testing of a unique system for the detection and isotopic analysis of CH4 plumes built around a Picarro isotopic (13C/12C) gas analyser and a high precision Los Gatos greenhouse gas analyser. Combined with micrometeorological measurements and a mechanism for collecting discrete samples for high precision dual isotope (13C/12C, 2H/1H) analysis the system enables mapping of concentrations as well as directional and isotope based source verification. We then present findings from our mobile methane surveys around the North West of England. This area includes a variety of natural and anthropogenic methane sources within a relatively small geographical area, including livestock farming, urban and industrial gas infrastructure, landfills and waste water treatment facilities, and wetlands. We show that the system was successfully able to locate leaks from natural gas infrastructure and emissions from agricultural activities and to distinguish isotope signatures from these sources.

Multispectrum analysis of air-broadened spectra in the ν3 Q branch of 12CH4

NASA Astrophysics Data System (ADS)

Devi, V. Malathy; Benner, D. Chris; Gamache, Robert R.; Tran, H.; Smith, Mary Ann H.; Sams, Robert L.

2018-02-01

We report experimental measurements of spectral line shape parameters (air-broadened width, shift, and line mixing coefficients) for several transitions in the ν3 Q branch of methane in the 3000-3023 cm-1 region. 13 high-resolution, room temperature laboratory spectra of pure methane and air-broadened methane recorded with two different Fourier transform spectrometers are fitted. 12 of these spectra were acquired at 0.01 cm-1 resolution with the McMath-Pierce FTS at the National Solar Observatory on Kitt Peak, and one higher-resolution (∼0.0011 cm-1) low pressure methane spectrum was obtained with the Bruker IFS-120HR FTS at the Pacific Northwest National Laboratory, in Richland, Washington. All the spectra were obtained using high purity natural samples of CH4 and lean mixtures of the same natural CH4 in dry air. For the 12 spectra recorded at Kitt Peak, three different absorption cells (L = 5, 25 and 150 cm) were used while the methane spectrum at PNNL was obtained using a 19.95 cm long absorption cell. For the analysis, an interactive multispectrum nonlinear least squares fitting software was employed where all the 13 spectra were fitted simultaneously. An accurate and self-consistent set of line parameters were determined by constraining a few of those for severely blended transitions. Line mixing was measured for 14 transition pairs for the CH4-air collision system. A constant speed dependence parameter, consistent with measured speed dependence values obtained in other methane bands, was applied to all the transitions included in the fitted region. The present measurements are compared to values reported in the literature.

Multispectrum analysis of air-broadened spectra in the ν 3 Q branch of 12CH4

DOE PAGES

Devi, V. Malathy; Benner, D. Chris; Gamache, Robert R.; ...

2017-12-06

In this paper, we report experimental measurements of spectral line shape parameters (air-broadened width, shift, and line mixing coefficients) for several transitions in the ν 3 Q branch of methane in the 3000–3023 cm -1 region. 13 high-resolution, room temperature laboratory spectra of pure methane and air-broadened methane recorded with two different Fourier transform spectrometers are fitted. 12 of these spectra were acquired at 0.01 cm -1 resolution with the McMath-Pierce FTS at the National Solar Observatory on Kitt Peak, and one higher-resolution (~0.0011 cm-1) low pressure methane spectrum was obtained with the Bruker IFS-120HR FTS at the Pacific Northwestmore » National Laboratory, in Richland, Washington. All the spectra were obtained using high purity natural samples of CH 4 and lean mixtures of the same natural CH 4 in dry air. For the 12 spectra recorded at Kitt Peak, three different absorption cells (L= 5, 25 and 150 cm) were used while the methane spectrum at PNNL was obtained using a 19.95 cm long absorption cell. For the analysis, an interactive multispectrum nonlinear least squares fitting software was employed where all the 13 spectra were fitted simultaneously. An accurate and self-consistent set of line parameters were determined by constraining a few of those for severely blended transitions. Line mixing was measured for fourteen transition pairs for the CH 4-air collision system. Lastly, a constant speed dependence parameter, consistent with measured speed dependence values obtained in other methane bands, was applied to all the transitions included in the fitted region. The present measurements are compared to values reported in the literature.« less

Reductive elimination/oxidative addition of carbon-hydrogen bonds at Pt(IV)/Pt(II) centers: mechanistic studies of the solution thermolyses of Tp(Me2)Pt(CH3)2H.

PubMed

Jensen, Michael P; Wick, Douglas D; Reinartz, Stefan; White, Peter S; Templeton, Joseph L; Goldberg, Karen I

2003-07-16

Reductive elimination of methane occurs upon solution thermolysis of kappa(3)-Tp(Me)2Pt(IV)(CH(3))(2)H (1, Tp(Me)2 = hydridotris(3,5-dimethylpyrazolyl)borate). The platinum product of this reaction is determined by the solvent. C-D bond activation occurs after methane elimination in benzene-d(6), to yield kappa(3)-Tp(Me)2Pt(IV)(CH(3))(C(6)D(5))D (2-d(6)), which undergoes a second reductive elimination/oxidative addition reaction to yield isotopically labeled methane and kappa(3)-Tp(Me)2Pt(IV)(C(6)D(5))(2)D (3-d(11)). In contrast, kappa(2)-Tp(Me)2Pt(II)(CH(3))(NCCD(3)) (4) was obtained in the presence of acetonitrile-d(3), after elimination of methane from 1. Reductive elimination of methane from these Pt(IV) complexes follows first-order kinetics, and the observed reaction rates are nearly independent of solvent. Virtually identical activation parameters (DeltaH(++)(obs) = 35.0 +/- 1.1 kcal/mol, DeltaS(++)(obs) = 13 +/- 3 eu) were measured for the reductive elimination of methane from 1 in both benzene-d(6) and toluene-d(8). A lower energy process (DeltaH(++)(scr) = 26 +/- 1 kcal/mol, DeltaS(++)(scr) = 1 +/- 4 eu) scrambles hydrogen atoms of 1 between the methyl and hydride positions, as confirmed by monitoring the equilibration of kappa(3)-Tp(Me)()2Pt(IV)(CH(3))(2)D (1-d(1)()) with its scrambled isotopomer, kappa(3)-Tp(Me)2Pt(IV)(CH(3))(CH(2)D)H (1-d(1'). The sigma-methane complex kappa(2)-Tp(Me)2Pt(II)(CH(3))(CH(4)) is proposed as a common intermediate in both the scrambling and reductive elimination processes. Kinetic results are consistent with rate-determining dissociative loss of methane from this intermediate to produce the coordinatively unsaturated intermediate [Tp(Me)2Pt(II)(CH(3))], which reacts rapidly with solvent. The difference in activation enthalpies for the H/D scrambling and C-H reductive elimination provides a lower limit for the binding enthalpy of methane to [Tp(Me)2Pt(II)(CH(3))] of 9 +/- 2 kcal/mol.

Effect of summer throughfall exclusion, summer drought, and winter snow cover on methane fluxes in a temperate forest soil

USGS Publications Warehouse

Borken, W.; Davidson, E.A.; Savage, K.; Sundquist, E.T.; Steudler, P.

2006-01-01

Soil moisture strongly controls the uptake of atmospheric methane by limiting the diffusion of methane into the soil, resulting in a negative correlation between soil moisture and methane uptake rates under most non-drought conditions. However, little is known about the effect of water stress on methane uptake in temperate forests during severe droughts. We simulated extreme summer droughts by exclusion of 168 mm (2001) and 344 mm (2002) throughfall using three translucent roofs in a mixed deciduous forest at the Harvard Forest, Massachusetts, USA. The treatment significantly increased CH4 uptake during the first weeks of throughfall exclusion in 2001 and during most of the 2002 treatment period. Low summertime CH4 uptake rates were found only briefly in both control and exclusion plots during a natural late summer drought, when water contents below 0.15 g cm-3 may have caused water stress of methanotrophs in the A horizon. Because these soils are well drained, the exclusion treatment had little effect on A horizon water content between wetting events, and the effect of water stress was smaller and more brief than was the overall treatment effect on methane diffusion. Methane consumption rates were highest in the A horizon and showed a parabolic relationship between gravimetric water content and CH4 consumption, with maximum rate at 0.23 g H2O g-1 soil. On average, about 74% of atmospheric CH4 was consumed in the top 4-5 cm of the mineral soil. By contrast, little or no CH4 consumption occurred in the O horizon. Snow cover significantly reduced the uptake rate from December to March. Removal of snow enhanced CH4 uptake by about 700-1000%, resulting in uptake rates similar to those measured during the growing season. Soil temperatures had little effect on CH4 uptake as long as the mineral soil was not frozen, indicating strong substrate limitation of methanotrophs throughout the year. Our results suggest that the extension of snow periods may affect the annual rate of CH4 oxidation and that summer droughts may increase the soil CH4 sink of temperate forest soils. ?? 2005 Elsevier Ltd. All rights reserved.

A comparison of PCA and PMF models for source identification of fugitive methane emissions

NASA Astrophysics Data System (ADS)

Assan, Sabina; Baudic, Alexia; Bsaibes, Sandy; Gros, Valerie; Ciais, Philippe; Staufer, Johannes; Robinson, Rod; Vogel, Felix

2017-04-01

Methane (CH_4) is a greenhouse gas with a global warming potential 28-32 times that of carbon dioxide (CO_2) on a 100 year period, and even greater on shorter timescales [Etminan, et al., 2016, Allen, 2014]. Thus, despite its relatively short life time and smaller emission quantities compared to CO_2, CH4 emissions contribute to approximately 20{%} of today's anthropogenic greenhouse gas warming [Kirschke et al., 2013]. Major anthropogenic sources include livestock (enteric fermentation), oil and gas production and distribution, landfills, and wastewater emissions [EPA, 2011]. Especially in densely populated areas multiple CH4 sources can be found in close vicinity. Thus, when measuring CH4 emissions at local scales it is necessary to distinguish between different CH4 source categories to effectively quantify the contribution of each sector and aid the implementation of greenhouse gas reduction strategies. To this end, source apportionment models can be used to aid the interpretation of spatial and temporal patterns in order to identify and characterise emission sources. The focus of this study is to evaluate two common linear receptor models, namely Principle Component Analysis (PCA) and Positive Matrix Factorisation (PMF) for CH4 source apportionment. The statistical models I will present combine continuous in-situ CH4 , C_2H_6, δ^1^3CH4 measured using a Cavity Ring Down Spectroscopy (CRDS) instrument [Assan et al. 2016] with volatile organic compound (VOC) observations performed using Gas Chromatography (GC) in order to explain the underlying variance of the data. The strengths and weaknesses of both models are identified for data collected in multi-source environments in the vicinity of four different types of sites; an agricultural farm with cattle, a natural gas compressor station, a wastewater treatment plant, and a pari-urban location in the Ile de France region impacted by various sources. To conclude, receptor model results to separate statistically the different sources from the variability of atmospheric observations are compared with an independent source identification method using stable methane isotopic analysis and simple CH_4/VOC ratios. Allen, D. T. (2014). Methane emissions from natural gas production and use: reconciling bottom-up and top-down measurements. Current Opinion in Chemical Engineering, 5, 78-83. Assan, S., Baudic, A., Guemri, A., Ciais, P., Gros, V., and Vogel, F. R.: Characterisation of interferences to in-situ observations of δ13CH4 and C2H6 when using a Cavity Ring Down Spectrometer at industrial sites, Atmos. Meas. Tech. Discuss., doi:10.5194/amt-2016-261, in review, 2016. Etminan, M., G. Myhre, E. J. Highwood and K. P. Shine (2016), Radiative forcing of carbon dioxide, methane, and nitrous oxide: A significant revision of the methane radiative forcing, Geophys. Res.Lett,43. Kirschke, S., Bousquet, P., Ciais, P., Saunois, M., Canadell, J. G., Dlugokencky, E. et al. (2013). Three decades of global methane sources and sinks. Nature Geoscience, 6(10), 813-823. U.S. Environmental Protection Agency's (U.S. EPA's). (2011) Global Anthropogenic Emissions of Non-CO2 Greenhouse Gases: 1990-2030. EPA 430-D-11-003

Effects of nitrogen and phosphorus additions on soil methane uptake in disturbed forests

NASA Astrophysics Data System (ADS)

Zheng, Mianhai; Zhang, Tao; Liu, Lei; Zhang, Wei; Lu, Xiankai; Mo, Jiangming

2016-12-01

Atmospheric nitrogen (N) deposition is generally thought to suppress soil methane (CH4) uptake in natural forests, and phosphorus (P) input may alleviate this negative effect. However, it remains unclear how N and P inputs control soil CH4 uptake in disturbed forests. In this study, soil CH4 uptake rates were measured in two disturbed forests, including a secondary forest (with previous, but not recent, disturbance) and a plantation forest (with recent continuous disturbance), in southern China for 34 months of N and/or P additions: control, N addition (150 kg N ha-1 yr-1), P addition (150 kg P ha-1 yr-1), and NP addition (150 kg N ha-1 yr-1 plus 150 kg P ha-1 yr-1). Mean CH4 uptake rate in control plots was significantly higher in the secondary forest (24.40 ± 0.81 µg CH4-C m-2 h-1) than in the plantation forest (17.07 ± 0.70 µg CH4-C m-2 h-1). CH4 uptake rate had negative relationships with soil water-filled pore space in both forests. In the secondary forest, N, P, and NP additions significantly decreased CH4 uptake by 39.7%, 27.8%, and 37.6%, respectively, but had no significant effects in the plantation forest, indicating that P input does not alleviate the suppression of CH4 uptake by N deposition. Taken together, our findings suggest that reducing anthropogenic disturbance, including harvesting of forest floor, and anthropogenic N and P inputs will increase soil CH4 uptake in disturbed forests, which is important in view of the increased trends in global warming during recent decades.

Deep peat warming increases surface methane and carbon dioxide emissions in a black spruce-dominated ombrotrophic bog.

PubMed

Gill, Allison L; Giasson, Marc-André; Yu, Rieka; Finzi, Adrien C

2017-12-01

Boreal peatlands contain approximately 500 Pg carbon (C) in the soil, emit globally significant quantities of methane (CH 4 ), and are highly sensitive to climate change. Warming associated with global climate change is likely to increase the rate of the temperature-sensitive processes that decompose stored organic carbon and release carbon dioxide (CO 2 ) and CH 4 . Variation in the temperature sensitivity of CO 2 and CH 4 production and increased peat aerobicity due to enhanced growing-season evapotranspiration may alter the nature of peatland trace gas emission. As CH 4 is a powerful greenhouse gas with 34 times the warming potential of CO 2 , it is critical to understand how factors associated with global change will influence surface CO 2 and CH 4 fluxes. Here, we leverage the Spruce and Peatland Responses Under Changing Environments (SPRUCE) climate change manipulation experiment to understand the impact of a 0-9°C gradient in deep belowground warming ("Deep Peat Heat", DPH) on peat surface CO 2 and CH 4 fluxes. We find that DPH treatments increased both CO 2 and CH 4 emission. Methane production was more sensitive to warming than CO 2 production, decreasing the C-CO 2 :C-CH 4 of the respired carbon. Methane production is dominated by hydrogenotrophic methanogenesis but deep peat warming increased the δ 13 C of CH 4 suggesting an increasing contribution of acetoclastic methanogenesis to total CH 4 production with warming. Although the total quantity of C emitted from the SPRUCE Bog as CH 4 is <2%, CH 4 represents >50% of seasonal C emissions in the highest-warming treatments when adjusted for CO 2 equivalents on a 100-year timescale. These results suggest that warming in boreal regions may increase CH 4 emissions from peatlands and result in a positive feedback to ongoing warming. © 2017 John Wiley & Sons Ltd.

The Application Of Biofilter System For Reduction Of Methane Emissions From Modern Sanitary Landfills

NASA Astrophysics Data System (ADS)

Sung, K.; Park, S.

2007-12-01

Increased atmospheric concentrations of greenhouse gases (GHG) caused by anthropogenic activities has been related to global climate change. Methane, the second most important GHG after CO2, is 21 times more effective at trapping heat than CO2. Therefore, methane emission control is of utmost importance for global warming reduction. To minimize leachate production and protect groundwater resources, modern sanitary landfills are equipped with composite covers and gas collection systems. Methane from modern sanitary landfills is vented directly to the atmosphere, except for some of the largest landfills where it is recovered as energy and burned at the site. However, the efficiency of energy recovery systems in larger landfills is reduced as the amount of CH4 generated from landfill begins to decrease. In this study, the performance of a lab-scale model biofilter system was investigated to treat CH4 gas emitted from modern sanitary landfills by conducting batch and column experiments using landfill cover soil amended with earthworm cast as the filter bed medium. From the batch experiments to measure the influence of moisture content and temperature of the filter medium on CH4 removal capacity of a biofilter system, the optimum moisture content and temperature were found to be 10-15% by weight and 25-35°C, respectively. The column experiment was conducted to measure the influence of inlet CH4 concentration and CH4 loading rate on CH4 removal capacity of a biofilter system. As the inlet CH4 concentration decreased, the percentage of CH4 oxidized increased. Up to a CH4 loading rate of 2785 g CH4 m3 h- 1 (EBRT = 7.7 min), the CH4 removal efficiency of the biofilter was able to reach 100%. Based on the results of the study, the installation of a properly managed biofilter system should be capable of achieving a reduction in atmospheric CH4 emissions from modern sanitary landfills at low CH4 generation stage.

Global Methane Budget 2000-2012 (V.1.0, issued June 2016 and V.1.1, issued December 2016)

DOE Data Explorer

Saunois, Marielle [University of Paris - Saclay, Gif-surYvette, France; Bousquet, Phillippe [University of Paris - Saclay, Gif-surYvette, France; Poulter, Ben [NASA Goddard Space Flight Center, Biospheric Science Laboratory, Greenbelt, MD (USA); Peregon, Anna [University of Paris - Saclay, Gif-surYvette, France; Ciais, Philippe [University of Paris - Saclay, Gif-surYvette, France

2016-01-01

After carbon dioxide (CO2), methane (CH4) is the second most important well-mixed greenhouse gas contributing to human-induced climate change. In a time-horizon of 100 years, CH4 has a Global Warming Potential (GWP-100) 28 times larger than CO2. The level of CH4 in the atmosphere is over 150% higher than pre-industrial times (cf. 1750), and it is responsible for 20% of the global warming produced by all well-mixed greenhouse gases. Methane is transformed into water vapor in the stratosphere. Methane also produces ozone in the troposphere, which is a pollutant with negative impacts on human health and ecosystems. The atmospheric life time of methane is 10 ± 2 years. [Copied from the Global Carbon Project, Global Methane Budget Highlights at http://www.globalcarbonproject.org/methanebudget/16/hl-compact.htm

The chemistry and transport of methane and carbon monoxide in the troposphere

NASA Technical Reports Server (NTRS)

Peters, L. K.; Chameides, W. L.

1980-01-01

The present understanding of the physical and chemical behavior of methane, carbon monoxide and the chemical species involved in the conversion of CH4 to CO in the troposphere is reviewed. Following a brief summary of CO and CH4 emission and reactions in urban areas, attention is given to measurements of the spatial and temporal distributions of CO and CH4 in the rural atmosphere, the contribution of the oceans to atmospheric CO and CH4 concentrations, and interactions of CH4 and CO with soils and vegetation. Estimates of the transport of CH4 and CO from the troposphere to the stratosphere are discussed, and photochemical reactions of the constituents are examined. Two- and three-dimensional models for CH4 and CO transport are presented, and possible future variations in atmospheric abundances of the molecules are considered. Finally, present estimates of the global methane and carbon dioxide budgets are summarized, and it is pointed out that, despite the large contribution of anthropogenic sources, the budgets appear to be in balance.

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

NASA Astrophysics Data System (ADS)

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.

Diurnal variation in greenhouse fluxes from a feedyard pen surface

USDA-ARS?s Scientific Manuscript database

Accurate estimation of greenhouse gas (GHG) emissions, including nitrous oxide (N2O) and methane (CH4) from open-lot beef cattle feedlots is an increasing concern given the current and potential future reporting requirements for GHG emissions. Research concerning N2O and CH4 emission fluxes from the...

METHANE EMISSIONS FROM INDUSTRIAL SOURCES

EPA Science Inventory

The chapter identifies and describes major industrial sources of methane (CH4) emissions. or each source type examined, it identifies CH4 release points and discusses in detail the factors affecting emissions. t also summarizes and discusses available global and country-specific ...

Methane-Cycling Microbial Communities and Methane Emission in Natural and Restored Peatlands

PubMed Central

Hynninen, Anu; Nieminen, Mika; Tuomivirta, Tero T.; Tuittila, Eeva-Stiina; Nousiainen, Hannu; Kell, Dana K.; Yrjälä, Kim; Tervahauta, Arja; Fritze, Hannu

2012-01-01

We addressed how restoration of forestry-drained peatlands affects CH4-cycling microbes. Despite similar community compositions, the abundance of methanogens and methanotrophs was lower in restored than in natural sites and correlated with CH4 emission. Poor establishment of methanogens may thus explain low CH4 emissions on restored peatlands even 10 to 12 years after restoration. PMID:22752167

A Variational Inverse Model Study of Amazonian Methane Emissions including Observations from the AMAZONICA campaign

NASA Astrophysics Data System (ADS)

Wilson, C. J.; Gloor, M.; Chipperfield, M.; Miller, J. B.; Gatti, L.

2013-12-01

Methane (CH4) is a greenhouse gas which is emitted from a range of anthropogenic and natural sources, and since the industrial revolution its mean atmospheric concentration has climbed dramatically, reaching values unprecedented in at least the past 650,000 years. CH4 produces a relatively high radiative forcing effect upon the Earth's climate, and its atmospheric lifetime of approximately 10 years makes it a more appealing target for the mitigation of climate change over short timescales than long-lived greenhouse gases such as carbon dioxide. However, the spatial and temporal variation of CH4 emissions are still not well understood, though in recent years a number of top-down and bottom-up studies have attempted to construct improved emission budgets. Some top-down studies may suffer from poor observational coverage in tropical regions, however, especially in the planetary boundary layer, where the atmosphere is highly sensitive to emissions. For example, although satellite observations often take a large volume of measurements in tropical regions, these retrievals are not usually sensitive to concentrations at the planet's surface. Methane emissions from Amazon region, in particular, are often poorly constrained. Since emissions form this region, coming mainly from wetland and biomass burning sources, are thought to be relatively high, additional observations in this region would greatly help to constrain the geographical distribution of the global CH4 emission budget. In order to provide such measurements, the AMAZONICA project began to take regular flask measurements of CH4 and other trace gases from aircraft over four Amazonian sites from the year 2010 onwards. We first present a forward modelling study of these observations of Amazonian methane for the year 2010 using the TOMCAT Chemical Transport Model. The model is used to attribute variations at each site to a source type and region, and also to assess the ability of our current CH4 flux estimates to reproduce these observations. Although there is mostly good agreement between the modelled and observed CH4, we find discrepancies between the two at one site in the east of the region, indicating possible errors surrounding the surface fluxes of methane affecting this site. We also present the results of an inverse modelling study of methane emissions for the year 2010, using INVICAT, which is a new variational inverse model based upon TOMCAT. This study represents the first use of the INVICAT scheme to constrain emissions of an atmospheric trace gas. Similarly to many previous inverse model studies, this top-down study assimilates ground-based flask observations of CH4 from the NOAA ground network. However, in order to provide additional constraints of CH4 emissions in the Amazon region, flask observations taken as part of the AMAZONICA campaign are also assimilated. The results of this inversion provide improved Amazonian and global CH4 emission budgets for the year 2010.

Monodeuterated Methane, an Isotopic Tool To Assess Biological Methane Metabolism Rates

PubMed Central

Steele, Joshua A.; Ziebis, Wiebke; Scheller, Silvan; Case, David; Reynard, Linda M.; Orphan, Victoria J.

2017-01-01

ABSTRACT Biological methane oxidation is a globally relevant process that mediates the flux of an important greenhouse gas through both aerobic and anaerobic metabolic pathways. However, measuring these metabolic rates presents many obstacles, from logistical barriers to regulatory hurdles and poor precision. Here we present a new approach for investigating microbial methane metabolism based on hydrogen atom dynamics, which is complementary to carbon-focused assessments of methanotrophy. The method uses monodeuterated methane (CH3D) as a metabolic substrate, quantifying the aqueous D/H ratio over time using off-axis integrated cavity output spectroscopy. This approach represents a nontoxic, comparatively rapid, and straightforward approach that supplements existing radiotopic and stable carbon isotopic methods; by probing hydrogen atoms, it offers an additional dimension for examining rates and pathways of methane metabolism. We provide direct comparisons between the CH3D procedure and the well-established 14CH4 radiotracer method for several methanotrophic systems, including type I and II aerobic methanotroph cultures and methane-seep sediment slurries and carbonate rocks under anoxic and oxic incubation conditions. In all applications tested, methane consumption values calculated via the CH3D method were directly and consistently proportional to 14C radiolabel-derived methane oxidation rates. We also employed this method in a nontraditional experimental setup, using flexible, gas-impermeable bags to investigate the role of pressure on seep sediment methane oxidation rates. Results revealed an 80% increase over atmospheric pressure in methanotrophic rates the equivalent of ~900-m water depth, highlighting the importance of this parameter on methane metabolism and exhibiting the flexibility of the newly described method. IMPORTANCE Microbial methane consumption is a critical component of the global carbon cycle, with wide-ranging implications for climate regulation and hydrocarbon exploitation. Nonetheless, quantifying methane metabolism typically involves logistically challenging methods and/or specialized equipment; these impediments have limited our understanding of methane fluxes and reservoirs in natural systems, making effective management difficult. Here, we offer an easily implementable, precise method using monodeuterated methane (CH3D) that advances three specific aims. First, it allows users to directly compare methane consumption rates between different experimental treatments of the same inoculum. Second, by empirically linking the CH3D procedure with the well-established 14C radiocarbon approach, we determine absolute scaling factors that facilitate rate measurements for several aerobic and anaerobic systems of interest. Third, CH3D represents a helpful tool in evaluating the relationship between methane activation and full oxidation in methanotrophic metabolisms. The procedural advantages, consistency, and novel research questions enabled by the CH3D method should prove useful in a wide range of culture-based and environmental microbial systems to further elucidate methane metabolism dynamics. PMID:28861523

Monodeuterated Methane, an Isotopic Tool To Assess Biological Methane Metabolism Rates.

PubMed

Marlow, Jeffrey J; Steele, Joshua A; Ziebis, Wiebke; Scheller, Silvan; Case, David; Reynard, Linda M; Orphan, Victoria J

2017-01-01

Biological methane oxidation is a globally relevant process that mediates the flux of an important greenhouse gas through both aerobic and anaerobic metabolic pathways. However, measuring these metabolic rates presents many obstacles, from logistical barriers to regulatory hurdles and poor precision. Here we present a new approach for investigating microbial methane metabolism based on hydrogen atom dynamics, which is complementary to carbon-focused assessments of methanotrophy. The method uses monodeuterated methane (CH 3 D) as a metabolic substrate, quantifying the aqueous D/H ratio over time using off-axis integrated cavity output spectroscopy. This approach represents a nontoxic, comparatively rapid, and straightforward approach that supplements existing radiotopic and stable carbon isotopic methods; by probing hydrogen atoms, it offers an additional dimension for examining rates and pathways of methane metabolism. We provide direct comparisons between the CH 3 D procedure and the well-established 14 CH 4 radiotracer method for several methanotrophic systems, including type I and II aerobic methanotroph cultures and methane-seep sediment slurries and carbonate rocks under anoxic and oxic incubation conditions. In all applications tested, methane consumption values calculated via the CH 3 D method were directly and consistently proportional to 14 C radiolabel-derived methane oxidation rates. We also employed this method in a nontraditional experimental setup, using flexible, gas-impermeable bags to investigate the role of pressure on seep sediment methane oxidation rates. Results revealed an 80% increase over atmospheric pressure in methanotrophic rates the equivalent of ~900-m water depth, highlighting the importance of this parameter on methane metabolism and exhibiting the flexibility of the newly described method. IMPORTANCE Microbial methane consumption is a critical component of the global carbon cycle, with wide-ranging implications for climate regulation and hydrocarbon exploitation. Nonetheless, quantifying methane metabolism typically involves logistically challenging methods and/or specialized equipment; these impediments have limited our understanding of methane fluxes and reservoirs in natural systems, making effective management difficult. Here, we offer an easily implementable, precise method using monodeuterated methane (CH 3 D) that advances three specific aims. First, it allows users to directly compare methane consumption rates between different experimental treatments of the same inoculum. Second, by empirically linking the CH 3 D procedure with the well-established 14 C radiocarbon approach, we determine absolute scaling factors that facilitate rate measurements for several aerobic and anaerobic systems of interest. Third, CH 3 D represents a helpful tool in evaluating the relationship between methane activation and full oxidation in methanotrophic metabolisms. The procedural advantages, consistency, and novel research questions enabled by the CH 3 D method should prove useful in a wide range of culture-based and environmental microbial systems to further elucidate methane metabolism dynamics.

Evaluation of modelled methane emissions over northern peatland sites

NASA Astrophysics Data System (ADS)

Gao, Yao; Burke, Eleanor; Chadburn, Sarah; Raivonen, Maarit; Susiluoto, Jouni; Vesala, Timo; Aurela, Mika; Lohila, Annalea; Aalto, Tuula

2017-04-01

Methane (CH4) is a powerful greenhouse gas, with approximately 34 times the global warming potential of carbon dioxide (CO2) over a century time horizon (IPCC, 2013). The strong sensitivity of methane emissions to environmental factors has led to concerns about potential positive feedbacks to climate change. Evaluation of the ability of the process-based land surface models of earth system models (ESMs) in simulating CH4 emission over peatland is needed for more precise future predictions. In this study, two peatland sites of poor and rich soil nutrient conditions, in southern and northern Finland respectively, are adopted. The measured CH4 fluxes at the two sites are used to evaluate the CH4 emissions simulated by the land surface model (JULES) of the UK Earth System model and by the Helsinki peatland methane emission model (HIMMELI), which is developed at Finnish Meteorological Institute and Helsinki University. In JULES, CH4 flux is simply related to soil temperature, wetland fraction and effective substrate availability. However, HIMMELI has detailed descriptions of microbial and transport processes for simulating CH4 flux. The seasonal dynamics of CH4 fluxes at the two sites are relatively well captured by both models, but model biases exist. Simulated CH4 flux is sensitive to water table depth (WTD) at both models. However, the simulated WTD is limited to be below ground in JULES. It is also important to have the annual cycle of LAI correct when coupling JULES with HIMMELI.

Permafrost Thaw Induces Methane Oxidation in Transitional Thaw Stages in a Subarctic Peatland

NASA Astrophysics Data System (ADS)

Perryman, C. R.; Kashi, N. N.; Malhotra, A.; McCalley, C. K.; Varner, R. K.

2015-12-01

Rising temperatures in the subarctic are accelerating permafrost thaw and increasing methane (CH4) emissions from subarctic peatlands. Methanotrophs in these peatlands can consume/oxidize CH4, potentially mitigating CH4 emissions in these peatlands. Oxidation rates can exceed 90% of CH4 production in some settings, depending on O2 and CH4 availability and environmental conditions. Malhotra and Roulet identified 10 thaw stages in Stordalen Mire near Abisko, Sweden (68°21'N,18°49'E ) with variable vegetation, environmental conditions, and associated CH4 emissions. We investigated potential methane oxidation rates across these thaw stages. Peat cores were extracted from two depths at each stage and incubated in 350ml glass jars at in situ temperatures and CH4 concentrations. Headspace samples were collected from each incubation jar over a 48-hour period and analyzed for CH4 concentration using flame ionization detection gas chromatography (GC-FID). Oxidation rates ranged from <0.1 to 17 μg of CH4 per gram of dry biomass per day. Water table depth and pore water pH were the strongest environmental correlates of oxidation (sample size = 56, p < 0.001). The highest potential oxidation rates were observed in collapsing palsa sites and recently collapsed sedge-dominated open water sites near palsa mounds. Our results suggest that permafrost thaw induces high CH4 oxidation rates by creating conditions ideal for both methanogenic and methanotrophic microbial communities. Our results also reinforce the importance of incorporating transitional thaw stages in landscape level carbon budgets of thawing peatlands emphasized by Malhotra and Roulet. Forthcoming microbial analysis and stable isotope analysis will further elucidate the factors controlling methane oxidation rates at Stordalen Mire.

Data-Constrained Projections of Methane Fluxes in a Northern Minnesota Peatland in Response to Elevated CO2 and Warming

Treesearch

Shuang Ma; Jiang Jiang; Yuanyuan Huang; Zheng Shi; Rachel M. Wilson; Daniel Ricciuto; Stephen D. Sebestyen; Paul J. Hanson; Yiqi Luo

2017-01-01

Large uncertainties exist in predicting responses of wetland methane (CH4) fluxes to future climate change. However, sources of the uncertainty have not been clearly identified despite the fact that methane production and emission processes have been extensively explored. In this study, we took advantage of manual CH4 flux...

Activity and diversity of methane-oxidizing bacteria in glacier forefields on siliceous and calcareous bedrock

NASA Astrophysics Data System (ADS)

Nauer, P. A.; Dam, B.; Liesack, W.; Zeyer, J.; Schroth, M. H.

2012-01-01

The global methane (CH4) cycle is largely driven by methanogenic archaea and methane-oxidizing bacteria (MOB), but little is known about their activity and diversity in pioneer ecosystems. We conducted a field survey in forefields of 13 receding Swiss glaciers on both siliceous and calcareous bedrock to investigate and quantify CH4 turnover based on soil-gas CH4 concentration profiles, and to characterize MOB communities using pmoA sequencing and T-RFLP. Methane turnover was fundamentally different in the two bedrock categories. Of the 36 CH4 concentration profiles from siliceous locations, 11 showed atmospheric CH4 consumption at concentrations of ∼1-2 μl l-1 with soil-atmosphere CH4 fluxes of -0.14 to -1.1 mg m-2 d-1. Another 11 profiles showed no apparent activity, while the remaining 14 exhibited slightly increased CH4 concentrations of ∼2-10 μl l-1, most likely due to microsite methanogenesis. In contrast, all profiles from calcareous sites suggested a substantial, yet unknown CH4 source below our sampling zone, with soil-gas CH4 concentrations reaching up to 1400 μl l-1. Remarkably, most soils oxidized ∼90% of the deep-soil CH4, resulting in soil-atmosphere fluxes of 0.12 to 31 mg m-2 d-1. MOB showed limited diversity in both siliceous and calcareous forefields: all identified pmoA sequences formed only 5 OTUs and, with one exception, could be assigned to either Methylocystis or the as-yet-uncultivated Upland Soil Cluster γ (USCγ). The latter dominated T-RFLP patterns of all siliceous and most calcareous samples, while Methylocystis dominated in 4 calcareous samples. As Type I MOB are widespread in cold climate habitats with elevated CH4 concentrations, USCγ might be the corresponding Type I MOBs in habitats exposed to near-atmospheric CH4 concentrations.

Chamber-Based Estimates of Methane Production in Coastal Estuarine Systems in Southern California

NASA Astrophysics Data System (ADS)

Brigham, B.; Lipson, D.; Lai, C.

2008-12-01

Wetland systems are believed to produce between 100 - 231 Tg CH4 yr-1 which is roughly 20% of global methane emissions. The uncertainty in methane emissions models stem from the lack of detailed information about methane gas production within regional wetland systems. The aim of this study is to report the range of methane fluxes observed along salinity gradients at two San Diego coastal wetland systems, the Tijuana Estuary (Tijuana River National Estuarine Research Reserve) and the Peñasquitos Lagoon (Torrey Pines State Park Reserve). Soil water samples are used to elucidate factors responsible for the observed variation in methane fluxes. Air samples were subsequently collected from the headspace of a static soil chamber and stored in pre- evacuated vials. Methane concentrations were analyzed within hours after collection by gas chromatography in the laboratory. The chemical and physical properties of the soil, including salinity, pH, redox potential and temperature are measured with a hand-held probe nearby soil collars. The biological properties of the soil, including dissolved organic carbon, nitrate, and ammonia levels are measured from soil water samples in the laboratory. We find that saline sites under direct tidal influence produced methane fluxes ranging from -3.10 to 9.10 (mean 2.18) mg CH4 m-2 day-1. We also find that brackish sites (0.6 to 3.2 ppt in salinity) with fresh water input from residential runoff at the Peñasquitos Lagoon produced methane fluxes ranging from 0.53 to 192.10 (mean 33.34) mg CH4 m-2 day-1. Sampling was done over the course of 5 weeks during August-September of 2008. We hypothesize that the contrasting methane fluxes found between the saline and the brackish sites is due primarily to the different salinity, and in turn sulfate levels found at the two sites. The reduction of sulfate to produce energy is more energetically favorable than the reduction of carbon dioxide to produce methane. Thus the presence of sulfate may act as a methanogensis inhibitor resulting in higher methane flux in low salinity conditions such as those found at the brackish sites.

Pinus sylvestris as a missing source of nitrous oxide and methane in boreal forest.

PubMed

Machacova, Katerina; Bäck, Jaana; Vanhatalo, Anni; Halmeenmäki, Elisa; Kolari, Pasi; Mammarella, Ivan; Pumpanen, Jukka; Acosta, Manuel; Urban, Otmar; Pihlatie, Mari

2016-03-21

Boreal forests comprise 73% of the world's coniferous forests. Based on forest floor measurements, they have been considered a significant natural sink of methane (CH4) and a natural source of nitrous oxide (N2O), both of which are important greenhouse gases. However, the role of trees, especially conifers, in ecosystem N2O and CH4 exchange is only poorly understood. We show for the first time that mature Scots pine (Pinus sylvestris L.) trees consistently emit N2O and CH4 from both stems and shoots. The shoot fluxes of N2O and CH4 exceeded the stem flux rates by 16 and 41 times, respectively. Moreover, higher stem N2O and CH4 fluxes were observed from wet than from dry areas of the forest. The N2O release from boreal pine forests may thus be underestimated and the uptake of CH4 may be overestimated when ecosystem flux calculations are based solely on forest floor measurements. The contribution of pine trees to the N2O and CH4 exchange of the boreal pine forest seems to increase considerably under high soil water content, thus highlighting the urgent need to include tree-emissions in greenhouse gas emission inventories.

Methane uptake in urban forests and lawns.

PubMed

Groffman, Peter M; Pouyat, Richard V

2009-07-15

The largest natural biological sink for the radiatively active trace gas methane (CH4) is bacteria in soils that consume CH4 as an energy and carbon source. This sink has been shown to be sensitive to nitrogen (N) inputs and alterations of soil physical conditions. Given this sensitivity, conversion of native ecosystems to urban, suburban, and exurban managed lawns thus has potential to affect regional CH4 budgets. We measured CH4 fluxes monthly from four urban forest, four rural forest and four urban lawn plots in the Baltimore, MD, metropolitan area from 2001 to 2005. Our objectives were to evaluate the effects of urban atmospheric and land use change on CH4 uptake and the importance of these changes relative to other greenhouse forcings in the urban landscape. Rural forests had a high capacity for CH4 uptake (1.68 mg m(-2) day(-1)). This capacity was reduced in urban forests (0.23 mg m(-2) day(-1)) and almost completely eliminated in lawns. Possible mechanisms for these reductions include increases in atmospheric N deposition and CO2 levels, fertilization of lawns, and alteration of soil physical conditions that influence diffusion. Although conversion of native forests to lawns had dramatic effects on CH4 uptake, these effects do not appear to be significant to statewide greenhouse gas forcing.

Enhancing surface methane fluxes from an oligotrophic lake: exploring the microbubble hypothesis.

PubMed

McGinnis, Daniel F; Kirillin, Georgiy; Tang, Kam W; Flury, Sabine; Bodmer, Pascal; Engelhardt, Christof; Casper, Peter; Grossart, Hans-Peter

2015-01-20

Exchange of the greenhouse gases carbon dioxide (CO2) and methane (CH4) across inland water surfaces is an important component of the terrestrial carbon (C) balance. We investigated the fluxes of these two gases across the surface of oligotrophic Lake Stechlin using a floating chamber approach. The normalized gas transfer rate for CH4 (k600,CH4) was on average 2.5 times higher than that for CO2 (k600,CO2) and consequently higher than Fickian transport. Because of its low solubility relative to CO2, the enhanced CH4 flux is possibly explained by the presence of microbubbles in the lake’s surface layer. These microbubbles may originate from atmospheric bubble entrainment or gas supersaturation (i.e., O2) or both. Irrespective of the source, we determined that an average of 145 L m(–2) d(–1) of gas is required to exit the surface layer via microbubbles to produce the observed elevated k600,CH4. As k600 values are used to estimate CH4 pathways in aquatic systems, the presence of microbubbles could alter the resulting CH4 and perhaps C balances. These microbubbles will also affect the surface fluxes of other sparingly soluble gases in inland waters, including O2 and N2.

Methane production and consumption in an active volcanic environment of Southern Italy.

PubMed

Castaldi, Simona; Tedesco, Dario

2005-01-01

Methane fluxes were measured, using closed chambers, in the Crater of Solfatara volcano, Campi Flegrei (Southern Italy), along eight transects covering areas of the crater presenting different landscape physiognomies. These included open bare areas, presenting high geothermal fluxes, and areas covered by vegetation, which developed along a gradient from the central open area outwards, in the form of maquis, grassland and woodland. Methane fluxes decreased logarithmically (from 150 to -4.5 mg CH4 m(-2)day(-1)) going from the central part of the crater (fangaia) to the forested edges, similarly to the CO2 fluxes (from 1500 g CO2 m(-2)day(-1) in the centre of the crater to almost zero flux in the woodlands). In areas characterized by high emissions, soil presented elevated temperature (up to 70 degrees C at 0-10 cm depth) and extremely low pH (down to 1.8). Conversely, in woodland areas pH was higher (between 3.7 and 5.1) and soil temperature close to air values. Soil (0-10 cm) was sampled, in two different occasions, along the eight transects, and was tested for methane oxidation capacity in laboratory. Areas covered by vegetation mostly consumed CH4 in the following order woodland>macchia>grassland. Methanotrophic activity was also measured in soil from the open bare area. Oxidation rates were comparable to those measured in the plant covered areas and were significantly correlated with field CH4 emissions. The biological mechanism of uptake was demonstrated by the absence of activity in autoclaved replicates. Thus results suggest the existence of a population of micro-organisms adapted to this extreme environment, which are able to oxidize CH4 and whose activity could be stimulated and supported by elevated concentrations of CH4.

Sequential parametric optimization of methane production from different sources of forest raw material

PubMed Central

Matsakas, Leonidas; Rova, Ulrika; Christakopoulos, Paul

2015-01-01

The increase in environmental problems and the shortage of fossil fuels have led to the need for action in the development of sustainable and renewable fuels. Methane is produced through anaerobic digestion of organic materials and is a biofuel with very promising characteristics. The success in using methane as a biofuel has resulted in the operation of several commercial-scale plants and the need to exploit novel materials to be used. Forest biomass can serve as an excellent candidate for use as raw material for anaerobic digestion. During this work, both hardwood and softwood species—which are representative of the forests of Sweden—were used for the production of methane. Initially, when untreated forest materials were used for the anaerobic digestion, the yields obtained were very low, even with the addition of enzymes, reaching a maximum of only 40 mL CH4/g VS when birch was used. When hydrothermal pretreatment was applied, the enzymatic digestibility improved up to 6.7 times relative to that without pretreatment, and the yield of methane reached up to 254 mL CH4/g VS. Then the effect of chemical/enzymatic detoxification was examined, where laccase treatment improved the methane yield from the more harshly pretreated materials while it had no effect on the more mildly pretreated material. Finally, addition of cellulolytic enzymes during the digestion improved the methane yields from spruce and pine, whereas for birch separate saccharification was more beneficial. To achieve high yields in spruce 30 filter paper units (FPU)/g was necessary, whereas 15 FPU/g was enough when pine and birch were used. During this work, the highest methane yields obtained from pine and birch were 179.9 mL CH4/g VS and 304.8 mL CH4/g VS, respectively. For mildly and severely pretreated spruce, the methane yields reached 259.4 mL CH4/g VS and 276.3 mL CH4/g VS, respectively. We have shown that forest material can serve as raw material for efficient production of methane. The initially low yields from the untreated materials were significantly improved by the introduction of a hydrothermal pretreatment. Moreover, enzymatic detoxification was beneficial, but mainly for severely pretreated materials. Finally, enzymatic saccharification increased the methane yields even further. PMID:26539186

Potential for methane production from anaerobic co-digestion of swine manure with winery wastewater.

PubMed

Riaño, B; Molinuevo, B; García-González, M C

2011-03-01

This work examines the methane production potential for the anaerobic co-digestion of swine manure (SM) with winery wastewater (WW). Batch and semi-continuous experiments were carried out under mesophilic conditions. Batch experiments revealed that the highest specific methane yield was 348 mL CH(4)g(-1) COD added, obtained at 85.4% of WW and 0.7 g COD g(-1)VS. Specific methane yield from SM alone was 27 mL CH(4)g(-1) COD added d(-1). Furthermore, specific methane yields were 49, 87 and 107 mL CH(4)g(-1) COD added d(-1) for the reactors co-digesting mixtures with 10% WW, 25% WW and 40% WW, respectively. Co-digestion with 40% WW improved the removal efficiencies up to 52% (TCOD), 132% (SCOD) and 61% (VSS) compared to SM alone. These results suggest that methane can be produced very efficiently by the co-digestion of swine manure with winery wastewater. Copyright © 2011 Elsevier Ltd. All rights reserved.

Breath Methane Excretion Is not An Accurate Marker of Colonic Methane Production in Irritable Bowel Syndrome.

PubMed

Di Stefano, Michele; Mengoli, Caterina; Bergonzi, Manuela; Klersy, Catherine; Pagani, Elisabetta; Miceli, Emanuela; Corazza, Gino Roberto

2015-06-01

The role of colonic methane production in functional bowel disorders is still uncertain. In small samples of irritable bowel syndrome (IBS) patients, it was shown that methane breath excretion correlates with clinical presentation and delayed gastrointestinal transit time. The aim of this study was to evaluate the relationship between intestinal production and breath excretion of CH4 and to correlate CH4 production with the presence and the severity of symptoms, in a large cohort of IBS patients and in a group of healthy volunteers. A group of 103 IBS patients and a group of 28 healthy volunteers were enrolled. The presence and severity of symptoms and gastrointestinal transit were evaluated in all subjects, who underwent breath H2/CH4 measurement for 7 h after lactulose to identify breath excretors of these gases; H2 and CH4 were also measured in rectal samples to identify colonic producers. Cumulative H2 and CH4 excretion and production were evaluated by the area under the time-concentration curve calculation (AUC). In IBS patients, CH4 was detected in rectal samples in 48 patients (47%), but only 27 of them (26% of the 103 enrolled patients) excreted this gas with breath. In CH4 producers, the prevalence and severity of symptoms and gastrointestinal transit time were not significantly different with respect to non-producers. IBS subtypes were homogeneously represented in CH4 producers and in non-producers. Healthy volunteers, compared with IBS patients, showed a significantly lower prevalence of CH4 excretion, whereas no difference was found in the prevalence of colonic CH4 production; moreover, in healthy volunteers compared with IBS, CH4 breath excretion and CH4 production were not different in quantitative terms. Our data show that colonic CH4 production is not associated with clinical presentation in IBS patients and does not correlate with symptom severity or with gastrointestinal transit time. Clinical inferences based on breath CH4 excretion should undergo an in-depth revision, as this method is not a good marker of CH4 colonic production.

Depth distribution of microbial production and oxidation of methane in northern boreal peatlands.

PubMed

Sundh, I; Nilsson, M; Granberg, G; Svensson, B H

1994-05-01

The depth distributions of anaerobic microbial methane production and potential aerobic microbial methane oxidation were assessed at several sites in both Sphagnum- and sedge-dominated boreal peatlands in Sweden, and compared with net methane emissions from the same sites. Production and oxidation of methane were measured in peat slurries, and emissions were measured with the closed-chamber technique. Over all eleven sites sampled, production was, on average, highest 12 cm below the depth of the average water table. On the other hand, highest potential oxidation of methane coincided with the depth of the average water table. The integrated production rate in the 0-60 cm interval ranged between 0.05 and 1.7 g CH4 m (-2) day(-) and was negatively correlated with the depth of the average water table (linear regression: r (2) = 0.50, P = 0.015). The depth-integrated potential CH4-oxidation rate ranged between 3.0 and 22.1 g CH4 m(-2) day(-1) and was unrelated to the depth of the average water table. A larger fraction of the methane was oxidized at sites with low average water tables; hence, our results show that low net emission rates in these environments are caused not only by lower methane production rates, but also by conditions more favorable for the development of CH4-oxidizing bacteria in these environments.

Effects of Marine and Freshwater Macroalgae on In Vitro Total Gas and Methane Production

PubMed Central

Machado, Lorenna; Magnusson, Marie; Paul, Nicholas A.; de Nys, Rocky; Tomkins, Nigel

2014-01-01

This study aimed to evaluate the effects of twenty species of tropical macroalgae on in vitro fermentation parameters, total gas production (TGP) and methane (CH4) production when incubated in rumen fluid from cattle fed a low quality roughage diet. Primary biochemical parameters of macroalgae were characterized and included proximate, elemental, and fatty acid (FAME) analysis. Macroalgae and the control, decorticated cottonseed meal (DCS), were incubated in vitro for 72 h, where gas production was continuously monitored. Post-fermentation parameters, including CH4 production, pH, ammonia, apparent organic matter degradability (OMd), and volatile fatty acid (VFA) concentrations were measured. All species of macroalgae had lower TGP and CH4 production than DCS. Dictyota and Asparagopsis had the strongest effects, inhibiting TGP by 53.2% and 61.8%, and CH4 production by 92.2% and 98.9% after 72 h, respectively. Both species also resulted in the lowest total VFA concentration, and the highest molar concentration of propionate among all species analysed, indicating that anaerobic fermentation was affected. Overall, there were no strong relationships between TGP or CH4 production and the >70 biochemical parameters analysed. However, zinc concentrations >0.10 g.kg−1 may potentially interact with other biochemical components to influence TGP and CH4 production. The lack of relationship between the primary biochemistry of species and gas parameters suggests that significant decreases in TGP and CH4 production are associated with secondary metabolites produced by effective macroalgae. The most effective species, Asparagopsis, offers the most promising alternative for mitigation of enteric CH4 emissions. PMID:24465524

Impact of an historic underground gas well blowout on the current methane chemistry in a shallow groundwater system

PubMed Central

Schout, Gilian; Hartog, Niels; Hassanizadeh, S. Majid; Griffioen, Jasper

2018-01-01

Blowouts present a small but genuine risk when drilling into the deep subsurface and can have an immediate and significant impact on the surrounding environment. Nevertheless, studies that document their long-term impact are scarce. In 1965, a catastrophic underground blowout occurred during the drilling of a gas well in The Netherlands, which led to the uncontrolled release of large amounts of natural gas from the reservoir to the surface. In this study, the remaining impact on methane chemistry in the overlying aquifers was investigated. Methane concentrations higher than 10 mg/L (n = 12) were all found to have δ13C-CH4 values larger than −30‰, typical of a thermogenic origin. Both δ13C-CH4 and δD-CH4 correspond to the isotopic composition of the gas reservoir. Based on analysis of local groundwater flow conditions, this methane is not a remnant but most likely the result of ongoing leakage from the reservoir as a result of the blowout. Progressive enrichment of both δ13C-CH4 and δD-CH4 is observed with increasing distance and decreasing methane concentrations. The calculated isotopic fractionation factors of εC = 3 and εD = 54 suggest anaerobic methane oxidation is partly responsible for the observed decrease in concentrations. Elevated dissolved iron and manganese concentrations at the fringe of the methane plume show that oxidation is primarily mediated by the reduction of iron and manganese oxides. Combined, the data reveal the long-term impact that underground gas well blowouts may have on groundwater chemistry, as well as the important role of anaerobic oxidation in controlling the fate of dissolved methane. PMID:29279383

Airborne Ethane Observations in the Barnett Shale: Quantification of Ethane Flux and Attribution of Methane Emissions.

PubMed

Smith, Mackenzie L; Kort, Eric A; Karion, Anna; Sweeney, Colm; Herndon, Scott C; Yacovitch, Tara I

2015-07-07

We present high time resolution airborne ethane (C2H6) and methane (CH4) measurements made in March and October 2013 as part of the Barnett Coordinated Campaign over the Barnett Shale formation in Texas. Ethane fluxes are quantified using a downwind flight strategy, a first demonstration of this approach for C2H6. Additionally, ethane-to-methane emissions ratios (C2H6:CH4) of point sources were observationally determined from simultaneous airborne C2H6 and CH4 measurements during a survey flight over the source region. Distinct C2H6:CH4 × 100% molar ratios of 0.0%, 1.8%, and 9.6%, indicative of microbial, low-C2H6 fossil, and high-C2H6 fossil sources, respectively, emerged in observations over the emissions source region of the Barnett Shale. Ethane-to-methane correlations were used in conjunction with C2H6 and CH4 fluxes to quantify the fraction of CH4 emissions derived from fossil and microbial sources. On the basis of two analyses, we find 71-85% of the observed methane emissions quantified in the Barnett Shale are derived from fossil sources. The average ethane flux observed from the studied region of the Barnett Shale was 6.6 ± 0.2 × 10(3) kg hr(-1) and consistent across six days in spring and fall of 2013.

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

PubMed Central

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

2016-01-01

Serpentinization potentially contributes to the origin and evolution of life during early history of the Earth. Serpentinization produces molecular hydrogen (H2) that can be utilized by microorganisms to gain metabolic energy. Methane can be formed through reactions between molecular hydrogen and oxidized carbon (e.g., carbon dioxide) or through biotic processes. A simple criterion, the H2/CH4 ratio, has been proposed to differentiate abiotic from biotic methane, with values approximately larger than 40 for abiotic methane and values of <40 for biotic methane. The definition of the criterion was based on two serpentinization experiments at 200 °C and 0.3 kbar. However, it is not clear whether the criterion is applicable at a wider range of temperatures. In this study, we performed sixteen experiments at 311–500 °C and 3.0 kbar using natural ground peridotite. Our results demonstrate that the H2/CH4 ratios strongly depend on temperature. At 311 °C and 3.0 kbar, the H2/CH4 ratios ranged from 58 to 2,120, much greater than the critical value of 40. By contrast, at 400–500 °C, the H2/CH4 ratios were much lower, ranging from 0.1 to 8.2. The results of this study suggest that the H2/CH4 ratios cannot reliably discriminate abiotic from biotic methane. PMID:27666288

New assignments in the 2 μm transparency window of the 12CH4 Octad band system

NASA Astrophysics Data System (ADS)

Daumont, L.; Nikitin, A. V.; Thomas, X.; Régalia, L.; Von der Heyden, P.; Tyuterev, Vl. G.; Rey, M.; Boudon, V.; Wenger, Ch.; Loëte, M.; Brown, L. R.

2013-02-01

This paper reports new assignments of rovibrational transitions of 12CH4 bands in the range 4600-4887 cm-1 which is usually referred to as a part of the 2 μm methane transparency window. Several experimental data sources for methane line positions and intensities were combined for this analysis. Three long path Fourier transform spectra newly recorded in Reims with 1603 m absorption path length and pressures of 1, 7 and 34 hPa for samples of natural abundance CH4 provided new measurements of 12CH4 lines. Older spectra for 13CH4 (90% purity) from JPL with 73 m absorption path length were used to identify the corresponding lines. Most of the lines in this region belong to the Octad system of 12CH4. The new spectra allowed us to assign 1014 new line positions and to measure 1095 line intensities in the cold bands of the Octad. These new line positions and intensities were added to the global fit of Hamiltonian and dipole moment parameters of the Ground State, Dyad, Pentad and Octad systems. This leads to a noticeable improvement of the theoretical description in this methane transparency window and a better global prediction of the methane spectrum.

Effect of temperature and oxidation rate on carbon-isotope fractionation during methane oxidation by landfill cover materials.

PubMed

Chanton, Jeffrey P; Powelson, David K; Abichou, Tarek; Fields, Dana; Green, Roger

2008-11-01

The quantification of methane oxidation is one of the major uncertainties in estimating CH4 emissions from landfills. Stable isotope methods provide a useful field approach for the quantification of methane oxidation in landfill cover soils. The approach relies upon the difference between the isotopic composition of oxidized gas at the location of interest and anaerobic zone CH4 and knowledge of alpha(ox), a term that describes the isotopic fractionation of the methanotrophic bacteria in their discrimination against (13)CH4. Natural variability in alpha(0x) in different landfill soils and the effect of temperature and other environmental factors on this parameter are not well defined. Therefore, standard determinations of alpha(ox), batch incubations of landfill cover soils with CH4, were conducted to determine alpha(ox) under a variety of conditions. When these results were combined with those of previous landfill incubation studies, the average alpha(ox) at 25 degrees C was 1.022 +/- 0.0015. alpha(ox) decreased with increasing temperature (-0.00039 alpha(ox) degrees C(-1)) overthe temperature range of 3-35 degrees C. alpha(ox) was found to be higher when determined after CH4-free storage and declined following CH4 pretreatment. alpha(ox) declined nonlinearly with increasing methane oxidation rate, Vmax.

A record of aerobic methane oxidation in tropical Africa over the last 2.5 Ma

NASA Astrophysics Data System (ADS)

Spencer-Jones, Charlotte L.; Wagner, Thomas; Talbot, Helen M.

2017-12-01

Methane and CO2 are climatically active greenhouse gases (GHG) and are powerful drivers of rapid global warming. Comparable to the Arctic, the tropics store large volumes of labile sedimentary carbon that is vulnerable to climate change. However, little is known about this labile carbon reservoir, in particular the behaviour of high methane-producing environments (e.g. wetlands), and their role in driving or responding to past periods of global climate change. In this study, we use a microbial biomarker approach that traces continental aerobic methane oxidation (AMO) from sedimentary organic matter in deep-sea fan sediments off the Congo River to reconstruct the link between central African methane cycling and continental export during key periods of global Pleistocene warmth. We use 35-amino bacteriohopanepolyols (BHPs), specifically aminobacteriohopane-31,32,33,34-tetrol (aminotetrol) and 35-aminobacteriohopane-30,31,32,33,34-pentol (aminopentol) as diagnostic molecular markers for AMO (CH4 oxidation markers) and the prevalence of continental wetland environments. BHPs were analysed in sediments from the Congo fan (ODP 1075) dated to 2.5 Ma. High resolution studies of key warm marine isotope stages (MIS) 5, 11 and 13 are included to test the relationship between CH4 oxidation markers in sediments at different levels of elevated global atmospheric GHG. This study presents the oldest reported occurrence, to date, of 35-amino BHPs up to 200 m below sea floor (∼2.5 Ma) with no strong degradation signature observed. Low concentrations of CH4 oxidation markers identified between 1.7 Ma and 1 Ma suggest a reduction in wetland extent in tropical Africa in response to more arid environmental conditions. Correlation of high resolution CH4 oxidation marker signatures with global atmospheric GHG concentrations during MIS 5, 11 and 13 further emphasize periods of enhanced tropical C cycling. However, subsequent analysis would be required to further extrapolate the relative importance of tropical methane sources as a driver of global methane concentrations during the Pleistocene.

The relative abundances of resolved l2CH2D2 and 13CH3D and mechanisms controlling isotopic bond ordering in abiotic and biotic methane gases

NASA Astrophysics Data System (ADS)

Young, E. D.; Kohl, I. E.; Lollar, B. Sherwood; Etiope, G.; Rumble, D.; Li, S.; Haghnegahdar, M. A.; Schauble, E. A.; McCain, K. A.; Foustoukos, D. I.; Sutclife, C.; Warr, O.; Ballentine, C. J.; Onstott, T. C.; Hosgormez, H.; Neubeck, A.; Marques, J. M.; Pérez-Rodríguez, I.; Rowe, A. R.; LaRowe, D. E.; Magnabosco, C.; Yeung, L. Y.; Ash, J. L.; Bryndzia, L. T.

2017-04-01

We report measurements of resolved 12CH2D2 and 13CH3D at natural abundances in a variety of methane gases produced naturally and in the laboratory. The ability to resolve 12CH2D2 from 13CH3D provides unprecedented insights into the origin and evolution of CH4. The results identify conditions under which either isotopic bond order disequilibrium or equilibrium are expected. Where equilibrium obtains, concordant Δ12CH2D2 and Δ13CH3D temperatures can be used reliably for thermometry. We find that concordant temperatures do not always match previous hypotheses based on indirect estimates of temperature of formation nor temperatures derived from CH4/H2 D/H exchange, underscoring the importance of reliable thermometry based on the CH4 molecules themselves. Where Δ12CH2D2 and Δ13CH3D values are inconsistent with thermodynamic equilibrium, temperatures of formation derived from these species are spurious. In such situations, while formation temperatures are unavailable, disequilibrium isotopologue ratios nonetheless provide novel information about the formation mechanism of the gas and the presence or absence of multiple sources or sinks. In particular, disequilibrium isotopologue ratios may provide the means for differentiating between methane produced by abiotic synthesis vs. biological processes. Deficits in 12CH2D2 compared with equilibrium values in CH4 gas made by surface-catalyzed abiotic reactions are so large as to point towards a quantum tunneling origin. Tunneling also accounts for the more moderate depletions in 13CH3D that accompany the low 12CH2D2 abundances produced by abiotic reactions. The tunneling signature may prove to be an important tracer of abiotic methane formation, especially where it is preserved by dissolution of gas in cool hydrothermal systems (e.g., Mars). Isotopologue signatures of abiotic methane production can be erased by infiltration of microbial communities, and Δ12CH2D2 values are a key tracer of microbial recycling.

Evaluating methane inventories by isotopic analysis in the London region.

PubMed

Zazzeri, G; Lowry, D; Fisher, R E; France, J L; Lanoisellé, M; Grimmond, C S B; Nisbet, E G

2017-07-07

A thorough understanding of methane sources is necessary to accomplish methane reduction targets. Urban environments, where a large variety of methane sources coexist, are one of the most complex areas to investigate. Methane sources are characterised by specific δ 13 C-CH 4 signatures, so high precision stable isotope analysis of atmospheric methane can be used to give a better understanding of urban sources and their partition in a source mix. Diurnal measurements of methane and carbon dioxide mole fraction, and isotopic values at King's College London, enabled assessment of the isotopic signal of the source mix in central London. Surveys with a mobile measurement system in the London region were also carried out for detection of methane plumes at near ground level, in order to evaluate the spatial allocation of sources suggested by the inventories. The measured isotopic signal in central London (-45.7 ±0.5‰) was more than 2‰ higher than the isotopic value calculated using emission inventories and updated δ 13 C-CH 4 signatures. Besides, during the mobile surveys, many gas leaks were identified that are not included in the inventories. This suggests that a revision of the source distribution given by the emission inventories is needed.

Methane alleviates copper-induced seed germination inhibition and oxidative stress in Medicago sativa.

PubMed

Samma, Muhammad Kaleem; Zhou, Heng; Cui, Weiti; Zhu, Kaikai; Zhang, Jing; Shen, Wenbiao

2017-02-01

Recent results discovered the protective roles of methane (CH 4 ) against oxidative stress in animals. However, the possible physiological roles of CH 4 in plants are still unknown. By using physiological, histochemical and molecular approaches, the beneficial role of CH 4 in germinating alfalfa seeds upon copper (Cu) stress was evaluated. Endogenous production of CH 4 was significantly increased in Cu-stressed alfalfa seeds, which was mimicked by 0.39 mM CH 4 . The pretreatment with CH 4 significantly alleviated the inhibition of seed germination and seedling growth induced by Cu stress. Cu accumulation was obviously blocked as well. Meanwhile, α/β amylase activities and sugar contents were increased, all of which were consistent with the alleviation of seed germination inhibition triggered by CH 4 . The Cu-triggered oxidative stress was also mitigated, which was confirmed by the decrease of lipid peroxidation and reduction of Cu-induced loss of plasma membrane integrity in CH 4 -pretreated alfalfa seedlings. The results of antioxidant enzymes, including ascorbate peroxidase (APX), superoxide dismutase (SOD), catalase (CAT), and guaiacol peroxidase (POD) total or isozymatic activities, and corresponding transcripts (APX1/2, Cu/Zn SOD and Mn-SOD), indicated that CH 4 reestablished cellular redox homeostasis. Further, Cu-induced proline accumulation was partly impaired by CH 4 , which was supported by the alternation of proline metabolism. Together, these results indicated that CH 4 performs an advantageous effect on the alleviation of seed germination inhibition caused by Cu stress, and reestablishment of redox homeostasis mainly via increasing antioxidant defence.

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 4: STATISTICAL METHODOLOGY

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

Tropical rainforest methane consumption during the El Niño of 2015-16

NASA Astrophysics Data System (ADS)

Aronson, E. L.; Dierick, D.; Botthoff, J.; Swanson, A. C.; Allen, M. F.

2016-12-01

Tropical forests sequester up to 40% of the anthropogenic and natural carbon exchanged with the atmosphere. Even though soils are the largest pool of terrestrial carbon, relatively little is known about the methane consumption capacity of tropical forest soils. Under high water, low oxygen (anaerobic) conditions, carbon decomposed is respired as methane (CH4) by methanogen microorganisms. During dry seasons, deeper rainforest soils remain wet, but dry at the surface. Since molecule for molecule the global warming potential of CH4 is two orders of magnitude greater than CO2, the relative production and sequestration of CO2 versus CH4 in tropical rainforests has a large impact on global climate trends. In 2015-16, the globe experienced an unusually strong ENSO event, which impacted the tropics. Atypical ENSO climatic events such as this include drought in tropical forests of Central America. We hypothesized that ENSO controls much of the year-to-year variability in the global CH4 cycle, primarily by turning the tropical forest from a strong annual source for CH4 during the La Niña or normal rainy season, to a year-round sink for CH4 during El Niño events. Further, we hypothesized that during a strong El Niño event, the unusually dry conditions of the tropical rainy season lead to the methanotrophs in these soils consuming large amounts of CH4. In order to investigate these predictions, CH4 flux was measured in three campaigns in March, during peak ENSO impact, as well as May and July 2016, at the La Selva Biological Station, Costa Rica. Fluxes were measured in eight paired plots, each with four collars. The collars measure 20 cm diameter by 12 cm in length, inserted into the soil, with a collar height of around 8 cm, in February 2016, a month before the first field campaign. Air samples were injected into pre-evacuated exetainers, and analyzed by gas chromatograph within 72 h. We found an average CH4 sink of -0.018 mg m-2 h-1. This flux is roughly four times lower than the average forest consumption rate, however most forest CH4 flux data is from temperate and boreal forests. While differences in flux magnitude between months were not significant, CH4 consumption was greatest in May, at -0.025 mg m-2 h-1, and lowest in March, at -0.011 mg m-2 h-1. These data help to fill the gap in knowledge of tropical forest methane flux.

Little evidence for significant increases of methane emissions from oil and gas operations in the U.S.

NASA Astrophysics Data System (ADS)

Lan, X.; Tans, P. P.; Sweeney, C.; Andrews, A. E.; Dlugokencky, E. J.; Lang, P. M.; Crotwell, M.; Miller, B.; Kofler, J.; Newberger, T.; McKain, K.; Wolter, S.; Montzka, S. A.

2016-12-01

Recent studies on whether methane (CH4) emissions from oil and natural gas (ONG) operations in the U.S. have increased are still inconclusive. To provide observational evidence we carefully analyzed the in-situ CH4 measurements from the NOAA/ESRL Global Greenhouse Gas Reference Network (GGGRN) for the best estimates of CH4 trends for 2006-2016. Methane data from more than 20 surface and aircraft sites across the U.S. were included in this study. Variations of sampling frequencies in different seasons were taken into account for accurate trend detection. Correlations among measurements within short sampling intervals were also considered for uncertainty estimates. We found that most of our sites had similar CH4 trends of 6 ppb/yr, which was comparable with the recent global background CH4 trend. Substantially higher growth rates were found at the Southern Great Plain site in Oklahoma (SGP, downwind of the Eagle Ford, Barnett Shale and Woodford ONG fields) and the Dahlen sites in North Dakota (DND, downwind of the Bakken ONG field), which indicated influences from regional ONG activities. Ethane (C2H6) measurements from SGP (C2H6 measurements were not available from DND) and propane (C3H8) measurements from both SPG and DND exhibited significant increasing trends, while trends at other sites were either non-significant (trend < 2*S.D.) or only marginally significant. Linear correlations were well identified for surface C3H8 and CH4 enhancements at these two sites, relative to observations at higher altitudes. However, by applying the observed enhancement ratios of surface C3H8 /CH4 and the C3H8 trends (as indicator for ONG emissions) on CH4 trend estimates, we would infer much larger surface CH4 trends than what we actually observed at these two sites. This discrepancy suggests that using enhancement ratios of C3H8 /CH4 is not likely a reliable approach to compute CH4 emission trends.

Exploratory study of atmospheric methane enhancements derived from natural gas use in the Houston urban area

NASA Astrophysics Data System (ADS)

Sanchez, Nancy P.; Zheng, Chuantao; Ye, Weilin; Czader, Beata; Cohan, Daniel S.; Tittel, Frank K.; Griffin, Robert J.

2018-03-01

The extensive use of natural gas (NG) in urban areas for heating and cooking and as a vehicular fuel is associated with potentially significant emissions of methane (CH4) to the atmosphere. Methane, a potent greenhouse gas that influences the chemistry of the atmosphere, can be emitted from different sources including leakage from NG infrastructure, transportation activities, end-use uncombusted NG, landfills and livestock. Although significant CH4 leakage associated with aging local NG distribution systems in the U.S. has been reported, further investigation is required to study the role of this infrastructure component and other NG-related sources in atmospheric CH4 enhancements in urban centers. In this study, neighborhood-scale mobile-based monitoring of potential CH4 emissions associated with NG in the Greater Houston area (GHA) is reported. A novel dual-gas 3.337 μm interband cascade laser-based sensor system was developed and mobile-mode deployed for simultaneous CH4 and ethane (C2H6) monitoring during a period of over 14 days, corresponding to ∼ 90 h of effective data collection during summer 2016. The sampling campaign covered ∼250 exclusive road miles and was primarily concentrated on eight residential zones with distinct infrastructure age and NG usage levels. A moderate number of elevated CH4 concentration events (37 episodes) with mixing ratios not exceeding 3.60 ppmv and associated with atmospheric background enhancements below 1.21 ppmv were observed during the field campaign. Source discrimination analyses based on the covariance between CH4 and C2H6 levels indicated the predominance of thermogenic sources (e.g., NG) in the elevated CH4 concentration episodes. The volumetric fraction of C2H6 in the sources associated with the thermogenic CH4 spikes varied between 2.7 and 5.9%, concurring with the C2H6 content in NG distributed in the GHA. Isolated CH4 peak events with significantly higher C2H6 enhancements (∼11%) were observed at industrial areas and locations with high density of petroleum and gas pipelines in the GHA, indicating potential variability in Houston's thermogenic CH4 sources.

Large emissions from floodplain trees close the Amazon methane budget.

PubMed

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

2017-12-14

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

Large emissions from floodplain trees close the Amazon methane budget

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Determination of biogas generation potential as a renewable energy source from supermarket wastes.

PubMed

Alkanok, Gizem; Demirel, Burak; Onay, Turgut T

2014-01-01

Fruit, vegetable, flower waste (FVFW), dairy products waste (DPW), meat waste (MW) and sugar waste (SW) obtained from a supermarket chain were anaerobically digested, in order to recover methane as a source of renewable energy. Batch mesophilic anaerobic reactors were run at total solids (TS) ratios of 5%, 8% and 10%. The highest methane yield of 0.44 L CH4/g VS(added) was obtained from anaerobic digestion of wastes (FVFW+DPW+MW+SW) at 10% TS, with 66.4% of methane (CH4) composition in biogas. Anaerobic digestion of mixed wastes at 5% and 8% TS provided slightly lower methane yields of 0.41 and 0.40 L CH4/g VS(added), respectively. When the wastes were digested alone without co-substrate addition, the highest methane yield of 0.40 L CH4/g VS(added) was obtained from FVFW at 5% TS. Generally, although the volatile solids (VS) conversion percentages seemed low during the experiments, higher methane yields could be obtained from anaerobic digestion of supermarket wastes. A suitable carbon/nitrogen (C/N) ratio, proper adjustment of the buffering capacity and the addition of essential trace nutrients (such as Ni) could improve VS conversion and biogas production yields significantly. Copyright © 2013 Elsevier Ltd. All rights reserved.

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

NASA Astrophysics Data System (ADS)

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

2003-12-01

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

Methane-producing bacteria - Natural fractionations of the stable carbon isotopes

NASA Technical Reports Server (NTRS)

Games, L. M.; Hayes, J. M.; Gunsalus, R. P.

1978-01-01

Procedures for determining the C-13/C-12 fractionation factors for methane-producing bacteria are described, and the fractionation factors (CO2/CH4) for the reduction of CO2 to CH4 by pure cultures are 1.045 for Methanosarcina barkeri at 40 C, 1.061 for Methanobacterium strain M.o.H. at 40 C, and 1.025 for Methanobacterium thermoautotrophicum at 65 C. The data are consistent with the field determinations if fractionation by acetate dissimilation approximates fractionations observed in natural environments. In other words, the acetic acid used by acetate dissimilating bacteria, if they play an important role in natural methane production, must have an intramolecular isotopic fractionation (CO2H/CH3) approximating the observed CO2/CH4 fractionation.

Response of the global climate to changes in atmospheric chemical composition due to fossil fuel burning

NASA Technical Reports Server (NTRS)

Cess, R. D.; Hameed, S.; Hogan, J. S.

1980-01-01

Tropospheric ozone and methane might increase in the future as the result of increasing anthropogenic emissions of CO, NOx and CH4 due to fossil fuel burning. Since O3 and CH4 are both greenhouse gases, increases in their concentrations could augment global warming due to larger future amounts of atmospheric CO2. To test this possible climatic impact, a zonal energy-balance climate model has been combined with a vertically-averaged tropospheric chemical model. The latter model includes all relevant chemical reactions which affect species derived from H2O, O2, CH4 and NOx. The climate model correspondingly incorporates changes in the infrared heating of the surface-troposphere system resulting from chemically induced changes in tropospheric ozone and methane. This coupled climate-chemical model indicates that global climate is sensitive to changes in emissions of CO, NOx and CH4, and that future increases in these emissions could enhance global warming due to increasing atmospheric CO2.

Enhanced contribution of wetland methane variability during recent El Nino

NASA Astrophysics Data System (ADS)

Zhang, Z.; Poulter, B.

2017-12-01

Wetlands are thought to be the dominant contributor to interannual variability in atmospheric methane (CH4) with a strong influence from the El Niño-Southern Oscillation (ENSO). However, whether the increase in emissions during El Nino droughts versus La Nina pluvial is from wetlands versus fire is unclear. Here we use a terrestrial ecosystem model LPJ-wsl that included permafrost and wetland dynamics, and compare how three climate datasets with different temporal resolution (daily: MERRA2, ERA-Interim; monthly: CRU), to simulate the spatio-temporal dynamics of wetland CH4 emissions from 1980-2016 to compare it against the MEI ENSO index and in-site surface observations. We find that strong El Niño event in 2015-2016 caused a record-high growth rate of wetland CH4 emissions compared to previous decades, which was mainly due to the combined effects of droughts and widespread warming over tropics on soil respiration. Our study will bring new insights into the role of wetlands in driving the variability of atmospheric CH4.

Identifying Anthropogenic Emissions of Atmospheric Mercury and Methane in Urban Houston Using Measurements from A Mobile Laboratory

NASA Astrophysics Data System (ADS)

Lan, X.; Laine, P. L.; Talbot, R. W.; Lefer, B. L.; Flynn, J. H.; Sive, B. C.

2013-12-01

The Houston area is heavily polluted with more than 400 refineries and other industrial facilities in the surrounding regions. From our 2-year continuous measurements at this area, we observed frequent occurrences of large peaks in both atmospheric mercury and methane. The highest elemental mercury level we observed was 27,327 ppqv, and the highest CH4 level reached 25 ppmv. We found that some mercury spikes occurred simultaneously with peaks in CH4, CO, CO2, and NO. Many high mercury episodes showed different features of CO, CO2, CH4, NOx and SO2, indicating contributions from different sources. To identify and quantify the sources of mercury and methane in this area, a mobile van equipped with mercury instruments together with CH4, CO2, δ13CH4, δ13CO2 (Picarro G2201-i), and CO, O3, and NOx will be used to sample the emissions from surrounding oil refineries facilities, natural gas processing plants, coal-fired power plants, sewage treatment plants, landfills, petrochemical manufacturing facilities, etc. A Proton Transfer Reaction Mass Spectrometer is also equipped in the mobile van to measure some VOCs species, such as benzene, toluene, isoprene, acetaldehyde, formaldehyde, methanol, acetone, MVK, MEK+MACR, C8 aromatics. The CH4 isotopic and VOCs signatures, and the ratios of mercury versus important species (i.e., CO and CO2) will help us to identify the mercury and methane sources, to investigate the methane leakage problem from natural gas operations, and improve the mercury and methane emission inventories in Houston area. We believe this study will also provide important information on industrial emissions that are missing from the EPA National Emission Inventory.

Understanding complete oxidation of methane on spinel oxides at a molecular level

DOE PAGES

Tao, Franklin Feng; Shan, Jun-jun; Nguyen, Luan; ...

2015-08-04

It is crucial to develop a catalyst made of earth-abundant elements highly active for a complete oxidation of methane at a relatively low temperature. NiCo 2O 4 consisting of earth-abundant elements which can completely oxidize methane in the temperature range of 350-550 °C. Being a cost-effective catalyst, NiCo 2O 4 exhibits activity higher than precious-metal-based catalysts. Here we report that the higher catalytic activity at the relatively low temperature results from the integration of nickel cations, cobalt cations and surface lattice oxygen atoms/oxygen vacancies at the atomic scale. Finally, in situ studies of complete oxidation of methane on NiCo 2Omore » 4 and theoretical simulations show that methane dissociates to methyl on nickel cations and then couple with surface lattice oxygen atoms to form -CH 3O with a following dehydrogenation to -CH 2O; a following oxidative dehydrogenation forms CHO; CHO is transformed to product molecules through two different sub-pathways including dehydrogenation of OCHO and CO oxidation.« less

Adsorptive separation studies of ethane-methane and methane-nitrogen systems using mesoporous carbon.

PubMed

Yuan, Bin; Wu, Xiaofei; Chen, Yingxi; Huang, Jianhan; Luo, Hongmei; Deng, Shuguang

2013-03-15

Adsorptive separations of C(2)H(6)/CH(4) and CH(4)/N(2) binary mixtures are of paramount importance from the energy and environmental points of view. A mesoporous carbon adsorbent was synthesized using a soft template method and characterized with TEM, TGA, and nitrogen adsorption/desorption. Adsorption equilibrium and kinetics of C(2)H(6), CH(4), and N(2) on the mesoporous carbon adsorbent were determined at 278, 298, and 318 K and pressures up to 100 kPa. The adsorption capacities of C(2)H(6) and CH(4) on the mesoporous carbon adsorbent at 298 K and 100 kPa are 2.20 mmol/g and 1.05 mmol/g, respectively. Both are significantly higher than those of many adsorbents including pillared clays and ETS-10 at a similar condition. The equilibrium selectivities of C(2)H(6)/CH(4) and CH(4)/N(2) at 298 K are 19.6 and 5.8, respectively. It was observed that the adsorption of C(2)H(6), CH(4), and N(2) gases on the carbon adsorbent was reversible with modest isosteric heats of adsorption, which implies that this carbon adsorbent can be easily regenerated in a cyclic adsorption process. These results suggest that the mesoporous carbon studied in this work is a promising alternative adsorbent for the separations of C(2)H(6)/CH(4) and CH(4)/N(2) gas mixtures. Copyright © 2012 Elsevier Inc. All rights reserved.

Global Wetland Contribution to 2000-2012 Atmospheric Methane Growth Rate Dynamics

NASA Technical Reports Server (NTRS)

Poulter, Benjamin; Bousquet, Philippe; Canadell, Josep G.; Ciais, Philippe; Peregon, Anna; Saunois, Marielle; Arora, Vivek K.; Beerling, David J.; Brovkin, Victor; Jones, Chris D.;

Methane production and emissions from four reclaimed and pristine wetlands of Southeastern United States

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schipper, L.A.; Reddy, K.R.

Wetlands are significant contributors to global CH[sub 4] emission. We measured CH[sub 4] emissions at two pristine wetlands [Okefenokee swamp and the Everglades (Water Conservation Area 2A)] and two reclaimed wetlands (Sunny Hill Farm and Apopka Marsh) in Southeastern USA, and we attempted to relate emissions to CH[sub 4] production rates of the soil and the soil's biological and chemical properties. Methane emissions through cattail [Typha sp.] and waterilly [Nymphaea ordorata (L.)] ranged from 0.09 to 1.7 g CH[sub 4] m[sup [minus]2] d[sup [minus]1] and exhibited high spatial and temporal variability. Diffusive flux of CH[sub 4] was calculated using dissolvedmore » CH[sub 4] profiles in the soil pore water and accounted for <5% of the plant-mediated emissions. Potential CH[sub 4] production rates were measured as a function of depth using soil samples obtained at 2-cm increments. Methane production rates were the same order of magnitude at all sites (<1-70 ng CH[sub 4]-C g[sup [minus]1] soil C d[sup [minus]1]) and were highest in the surface soils (0-6 cm) at three of the wetland sites, indicating that the predominant source of C available to methanogens was in the surface soils. Methane production rates in the top 24 cm ranged from 0.3 to 1.1 g CH[sub 4] m[sup [minus]2] d[sup [minus]1] and annual C losses due to anaerobic decomposition accounted for between 0.68 and 3.7% of the total C in the surface 24-cm soil depth. 36 refs., 3 figs., 3 tabs.« less

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

PubMed

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

2007-07-15

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

Emissions of coalbed and natural gas methane from abandoned oil and gas wells in the United States

NASA Astrophysics Data System (ADS)

Townsend-Small, Amy; Ferrara, Thomas W.; Lyon, David R.; Fries, Anastasia E.; Lamb, Brian K.

2016-03-01

Recent work indicates that oil and gas methane (CH4) inventories for the United States are underestimated. Here we present results from direct measurements of CH4 emissions from 138 abandoned oil and gas wells, a source currently missing from inventories. Most abandoned wells do not emit CH4, but 6.5% of wells had measurable CH4 emissions. Twenty-five percent of wells we visited that had not been plugged emitted > 5 g CH4 h-1. Stable isotopes indicate that wells emit natural gas and/or coalbed CH4. We estimate that abandoned wells make a small contribution (<1%) to regional CH4 emissions in our study areas. Additional data are needed to accurately determine the contribution of abandoned wells to national CH4 budgets, particularly measurements in other basins and better characterization of the abundance and regional distribution of high emitters.

Influence of transient flooding on methane fluxes from subtropical pastures

USDA-ARS?s Scientific Manuscript database

Seasonally flooded subtropical pastures are major methane (CH4) sources, where transient flooding drives episodic and high-magnitude emissions from the underlying landscape. Understanding the mechanisms that drive these patterns is needed to better understand pasture CH4 emissions and their response...

Functionalized multi-walled carbon nanotube based sensors for distributed methane leak detection

EPA Science Inventory

This paper presents a highly sensitive, energy efficient and low-cost distributed methane (CH4) sensor system (DMSS) for continuous monitoring, detection and localization of CH4 leaks in natural gas infrastructure such as transmission and distribution pipelines, wells, and produc...

Control of Methane Production and Exchange in Northern Peatlands

NASA Technical Reports Server (NTRS)

Crill, Patrick

1997-01-01

This proposal has successfully supported studies that have developed unique long ten-n datasets of methane (CH4) emissions and carbon dioxide (CO2) exchange in order to quantify the controls on CH4 production and exchange especially the linkages to the carbon cycle in northern peatlands. The primary research site has been a small fen in southeastern New Hampshire where a unique multi-year data baseline of CH4 flux measurements was begun (with NASA funding) in 1989. The fen has also been instrumented for continuous hydrological and meteorological observations and year-round porewater sampling. Multiyear datasets of methane flux are very valuable and very rare. Datasets using the same sampling techniques at the same sites are the only way to assess the effect of the integrated ecosystem response to climatological variability. The research has had two basic objectives: 1. To quantify the effect of seasonal and interannual variability on CH4flux. 2. To examine process level controls on methane dynamics.

Ancient dissolved methane in inland waters at low concentrations revealed by a new collection method for radiocarbon (^{14}C) analysis

NASA Astrophysics Data System (ADS)

Dean, Joshua F.; Billett, Michael F.; Murray, Callum; Garnett, Mark H.

2017-04-01

Methane (CH4) is a powerful greenhouse gas and is released to the atmosphere from freshwater systems in numerous biomes globally. Radiocarbon (14C) analysis of methane can provide unique information about its age, source and rate of cycling in natural environments. Methane is often released from aquatic sediments in bubbles (ebullition), but dissolved methane is also present in lakes and streams at lower concentrations, and may not be of the same age or source. Obtaining sufficient non-ebullitive aquatic methane for 14C analysis remains a major technical challenge. Previous studies have shown that freshwater methane, in both dissolved and ebullitive form, can be significantly older than other forms of aquatic carbon (C), and it is therefore important to characterise this part of the terrestrial C balance. We present a novel method to capture sufficient amounts of dissolved methane from freshwater environments for 14C analysis by circulating water across a hydrophobic, gas-permeable membrane and collecting the methane in a large collapsible vessel. The results of laboratory and field tests show that reliable dissolved δ13CH4 and 14CH4 samples can be readily collected over short time periods (˜4 to 24 hours), at relatively low cost and from a variety of surface water types. The initial results further support previous findings that dissolved methane can be significantly older than other forms of aquatic C, especially in organic-rich catchments, and is currently unaccounted for in many terrestrial C balances and models. This method is suitable for use in remote locations, and could potentially be used to detect the leakage of unique 14CH4 signatures from point sources into waterways, e.g. coal seam gas and landfill gas.

Model Analysis of the Factors Regulating Trends and Variability of Methane, Carbon Monoxide and OH: 1. Model Validation

NASA Technical Reports Server (NTRS)

Elshorbany, Y. F.; Strode, S.; Wang, J.; Duncan, B.

2014-01-01

Methane (CH4) is the second most important anthropogenic greenhouse gas (GHG). Its 100-year global warming potential (GWP) is 25 times larger than that for carbon dioxide. The 100-yr integrated GWP of CH4 is sensitive to changes in OH levels. Methane's atmospheric growth rate was estimated to be more than 10 ppb yr(exp -1) in 1998 but less than zero in 2001, 2004 and 2005 (Kirschke et al., 2013). Since 2006, the CH4 is increasing again. This phenomena is yet not well understood. Oxidation of CH4 by OH is the main loss process, thus affecting the oxidizing capacity of the atmosphere and contributing to the global ozone background. Current models typically use an annual cycle of offline OH fields to simulate CH4. The implemented OH fields in these models are typically tuned so that simulated CH4 growth rates match that measured. For future and climate simulations, the OH tuning technique may not be suitable. In addition, running full chemistry, multi-decadal CH4 simulations is a serious challenge and currently, due to computational intensity, almost impossible.

Investigating the emission, dissolution, and oxidation of CH4 within and around a seep bubble plume in the Gulf of Mexico.

NASA Astrophysics Data System (ADS)

Leonte, M.; Kessler, J. D.; Socolofsky, S. A.

2016-02-01

One of the largest carbon reservoirs on the planet is stored as methane (CH4) in and below the seafloor. However, a large discrepancy exists between estimated fluxes of CH4 into the water column and CH4 fluxes from the sea surface to the atmosphere, suggesting that a significant fraction of CH4 released from seafloor seeps is dissolved and potentially removed through microbial oxidation. Here we present data investigating the fate of CH4 released from the Sleeping Dragon seep site in the Gulf of Mexico. The bubble plume was followed from the seafloor until it fully dissolved using a remotely operated vehicle (ROV). Water samples were collected by the ROV at different depths as well as lateral transects through the bubble plume. These samples were analyzed for dissolved concentrations of methane, ethane, propane, and butane as well as the 13C isotopic ratio of methane. Furthermore, seep bubbles from the seafloor were also collected and analyzed for the same properties. Based on these chemical data, the rate of CH4 emission from the seafloor, oxidation in the water column, and dissolution are investigated.

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

NASA Astrophysics Data System (ADS)

Liu, Xiao-Qiang; Xue, Ying; Tian, Zhi-Yue; Mo, Jing-Jing; Qiu, Nian-Xiang; Chu, Wei; Xie, He-Ping

2013-11-01

Graphene doped by nitrogen (N) and/or boron (B) is used to represent the surface models of coal with the structural heterogeneity. Through the density functional theory (DFT) calculations, the interactions between coalbed methane (CBM) and coal surfaces have been investigated. Several adsorption sites and orientations of methane (CH4) on graphenes were systematically considered. Our calculations predicted adsorption energies of CH4 on graphenes of up to -0.179 eV, with the strongest binding mode in which three hydrogen atoms of CH4 direct to graphene surface, observed for N-doped graphene, compared to the perfect (-0.154 eV), B-doped (-0.150 eV), and NB-doped graphenes (-0.170 eV). Doping N in graphene increases the adsorption energies of CH4, but slightly reduced binding is found when graphene is doped by B. Our results indicate that all of graphenes act as the role of a weak electron acceptor with respect to CH4. The interactions between CH4 and graphenes are the physical adsorption and slightly depend upon the adsorption sites on graphenes and the orientations of methane as well as the electronegativity of dopant atoms in graphene.

Evaluating Bay Area Methane Emission Inventory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fischer, Marc; Jeong, Seongeun

As a regulatory agency, evaluating and improving estimates of methane (CH4) emissions from the San Francisco Bay Area is an area of interest to the Bay Area Air Quality Management District (BAAQMD). Currently, regional, state, and federal agencies generally estimate methane emissions using bottom-up inventory methods that rely on a combination of activity data, emission factors, biogeochemical models and other information. Recent atmospheric top-down measurement estimates of methane emissions for the US as a whole (e.g., Miller et al., 2013) and in California (e.g., Jeong et al., 2013; Peischl et al., 2013) have shown inventories underestimate total methane emissions bymore » ~ 50% in many areas of California, including the SF Bay Area (Fairley and Fischer, 2015). The goal of this research is to provide information to help improve methane emission estimates for the San Francisco Bay Area. The research effort builds upon our previous work that produced methane emission maps for each of the major source sectors as part of the California Greenhouse Gas Emissions Measurement (CALGEM) project (http://calgem.lbl.gov/prior_emission.html; Jeong et al., 2012; Jeong et al., 2013; Jeong et al., 2014). Working with BAAQMD, we evaluate the existing inventory in light of recently published literature and revise the CALGEM CH4 emission maps to provide better specificity for BAAQMD. We also suggest further research that will improve emission estimates. To accomplish the goals, we reviewed the current BAAQMD inventory, and compared its method with those from the state inventory from the California Air Resources Board (CARB), the CALGEM inventory, and recent published literature. We also updated activity data (e.g., livestock statistics) to reflect recent changes and to better represent spatial information. Then, we produced spatially explicit CH4 emission estimates on the 1-km modeling grid used by BAAQMD. We present the detailed activity data, methods and derived emission maps by sector. In total, we estimate the anthropogenic emissions for BAAQMD to be 116.4 Gg (1 Gg = 109 g) CH4/yr, with a likely uncertainty of ~ 50% or more (e.g., NRC, 2010; US-EPA, 2015). Including the emissions from wetland (Jeong et al., 2013), the total CH4 emission estimate for BAAQMD is 120.1 Gg CH4/yr. Table 1 summarizes the estimated CH4 emissions for 2011 by sector. The sectors were categorized following those that are used in recent regional emission quantification studies (e.g., Jeong et al., 2013; Peischl et al., 2013; Wecht et al., 2014). However, we note that this result is marginally lower than the top-down estimate of 240 ± 60 Gg CH4/yr (at 95% confidence) reported by Fairley and Fischer (2015), suggesting some combination of systematic error in the top-down estimate, underestimation of emissions from known sources, or as yet unidentified sources may be present. With respect to the relative contributions from different source sectors, the CH4 emissions from the region are dominated by urban activities. Landfill emissions represent 53% of the District’s total emission followed by livestock (16%) and natural gas (15%). These three dominant sectors account for 84% of the total anthropogenic emission in BAAQMD. This suggests that mitigation efforts need to focus on these three sources. Figure 1 shows the gridded anthropogenic CH4 emissions on the BAAQMD’s 1-km grid. In general, the spatial pattern of emissions follows the density of population while strong point sources are also distributed in the rural areas of the District. Detailed methods and emissions for each sector and county are described in the following sections.« less

Underlying Ecosystem Methane Emissions Exceed Cattle-Derived Methane from Subtropical Lowland Pastures.

NASA Astrophysics Data System (ADS)

Chamberlain, S. D.; Sparks, J. P.

2014-12-01

Grazing cattle are a major methane (CH4) source from pasture ecosystems, however the underlying landscape is a potentially significant CH4 source that has received far less attention. Ecosystem surface emissions of CH4 are poorly quantified, vary widely across time and space, and are easily underestimated if emission hotspots or episodic fluxes are overlooked. We used static chambers, eddy covariance, and mobile cavity-ringdown spectrometry surveys to quantify spatially and temporally variable CH4 emissions from subtropical lowland pastures. We conclude emissions from soil and standing water are the dominant CH4 source, and cattle were responsible for only 13% of annual CH4emissions. The ecosystem emit 33.8 ± 2.2 g CH4 m-2 yr-1, however surface CH4 emissions were highly variable in both time and space. Seasonal flooding of pastures and low-lying landforms (canals, ditches, wetlands) drove high magnitude CH4 emissions. We observed large CH4 emissions from wetlands and, to a lesser extent, the entire landscape during the wet season. In contrast, during the dry season there was no appreciable CH4 accumulation in pastures when cattle were not present, and canals, which comprise 1.7% of the total land area, were responsible 97.7 % of dry season emissions. Ecosystem CH4 fluxes, measured by eddy covariance, varied seasonally and positively correlated to soil and air temperature, topsoil water content, and water table depth. Our work is the first to use mobile spectrometers to map biogenic CH4 emissions at the landscape scale, and demonstrates that soils and water are a strong pasture CH4 source that must be considered in addition to cattle emissions.

Specific model for the estimation of methane emission from municipal solid waste landfills in India.

PubMed

Kumar, Sunil; Nimchuk, Nick; Kumar, Rakesh; Zietsman, Josias; Ramani, Tara; Spiegelman, Clifford; Kenney, Megan

2016-09-01

The landfill gas (LFG) model is a tool for measuring methane (CH4) generation rates and total CH4 emissions from a particular landfill. These models also have various applications including the sizing of the LFG collection system, evaluating the benefits of gas recovery projects, and measuring and controlling gaseous emissions. This research paper describes the development of a landfill model designed specifically for Indian climatic conditions and the landfill's waste characteristics. CH4, carbon dioxide (CO2), oxygen (O2) and temperature were considered as the prime factor for the development of this model. The developed model was validated for three landfill sites in India: Shillong, Kolkata, and Jaipur. The autocorrelation coefficient for the model was 0.915, while the R(2) value was 0.429. Copyright © 2016 Elsevier Ltd. All rights reserved.

Culture scale-up and immobilisation of a mixed methanotrophic consortium for methane remediation in pilot-scale bio-filters.

PubMed

Karthikeyan, Obulisamy Parthiba; Saravanan, Nadarajan; Cirés, Samuel; Alvarez-Roa, Carlos; Razaghi, Ali; Chidambarampadmavathy, Karthigeyan; Velu, Chinnathambi; Subashchandrabose, Gobalakrishnan; Heimann, Kirsten

2017-02-01

Robust methanotrophic consortia for methane (CH 4 ) remediation and by-product development are presently not readily available for industrial use. In this study, a mixed methanotrophic consortium (MMC), sequentially enriched from a marine sediment, was assessed for CH 4 removal efficiency and potential biomass-generated by-product development. Suitable packing material for bio-filters to support MMC biofilm establishment and growth was also evaluated. The enriched MMC removed ∼7-13% CH 4 under a very high gas flow rate (2.5 L min -1 ; 20-25% CH 4 ) in continuous-stirred tank reactors (∼10 L working volume) and the biomass contained long-chain fatty acids (i.e. C 16 and C 18 ). Cultivation of the MMC on plastic bio-balls abated ∼95-97% CH 4 in pilot-scale non-sterile outdoor-operated bio-filters (0.1 L min -1 ; 1% CH 4 ). Contamination by cyanobacteria had beneficial effects on treating low-level CH 4 , by providing additional oxygen for methane oxidation by MMC, suggesting that the co-cultivation of MMC with cyanobacterial mats does not interfere with and may actually be beneficial for remediation of CH 4 and CO 2 at industrial scale.

Hydrogen and carbon isotope systematics in hydrogenotrophic methanogenesis under H2-limited and H2-enriched conditions: implications for the origin of methane and its isotopic diagnosis

NASA Astrophysics Data System (ADS)

Okumura, Tomoyo; Kawagucci, Shinsuke; Saito, Yayoi; Matsui, Yohei; Takai, Ken; Imachi, Hiroyuki

2016-12-01

Hydrogen and carbon isotope systematics of H2O-H2-CO2-CH4 in hydrogenotrophic methanogenesis and their relation to H2 availability were investigated. Two H2-syntrophic cocultures of fermentatively hydrogenogenic bacteria and hydrogenotrophic methanogens under conditions of <102 Pa-H2 and two pure cultures of hydrogenotrophic methanogens under conditions of 105 Pa-H2 were tested. Carbon isotope fractionation between CH4 and CO2 during hydrogenotrophic methanogenesis was correlated with pH2, as indicated in previous studies. The hydrogen isotope ratio of CH4 produced during rapid growth of the thermophilic methanogen Methanothermococcus okinawensis under high pH2 conditions ( 105 Pa) was affected by the isotopic composition of H2, as concluded in a previous study of Methanothermobacter thermautotrophicus. This " {δ D}_{{H}_2} effect" is a possible cause of the diversity of previously reported values for hydrogen isotope fractionation between CH4 and H2O examined in H2-enriched culture experiments. Hydrogen isotope fractionation between CH4 and H2O, defined by (1000 + {δ D}_{{CH}_4} )/(1000 + {δ D}_{{H}_2O} ), during hydrogenotrophic methanogenesis of the H2-syntrophic cocultures was in the range 0.67-0.69. The hydrogen isotope fractionation of our H2-syntrophic dataset overlaps with those obtained not only from low- pH2 experiments reported so far but also from natural samples of "young" methane reservoirs (0.66-0.74). Conversely, such hydrogen isotope fractionation is not consistent with that of "aged" methane in geological samples (≥0.79), which has been regarded as methane produced via hydrogenotrophic methanogenesis from the carbon isotope fractionation. As a possible process inducing the inconsistency in hydrogen isotope signatures between experiments and geological samples, we hypothesize that the hydrogen isotope signature of CH4 imprinted at the time of methanogenesis, as in the experiments and natural young methane, may be altered by diagenetic hydrogen isotope exchange between extracellular CH4 and H2O through reversible reactions of the microbial methanogenic pathway in methanogenic region and/or geological methane reservoirs.

The Description and Validation of a Computationally-Efficient CH4-CO-OH (ECCOH) Module for 3D Model Applications

NASA Technical Reports Server (NTRS)

Elshorbany, Yasin F.; Duncan, Bryan N.; Strode, Sarah A.; Wang, James S.; Kouatchou, Jules

2015-01-01

We present the Efficient CH4-CO-OH Module (ECCOH) that allows for the simulation of the methane, carbon monoxide and hydroxyl radical (CH4-CO-OH cycle, within a chemistry climate model, carbon cycle model, or earth system model. The computational efficiency of the module allows many multi-decadal, sensitivity simulations of the CH4-CO-OH cycle, which primarily determines the global tropospheric oxidizing capacity. This capability is important for capturing the nonlinear feedbacks of the CH4-CO-OH system and understanding the perturbations to relatively long-lived methane and the concomitant impacts on climate. We implemented the ECCOH module into the NASA GEOS-5 Atmospheric Global Circulation Model (AGCM), performed multiple sensitivity simulations of the CH4-CO-OH system over two decades, and evaluated the model output with surface and satellite datasets of methane and CO. The favorable comparison of output from the ECCOH module (as configured in the GEOS-5 AGCM) with observations demonstrates the fidelity of the module for use in scientific research.

The Description and Validation of a Computationally-Efficient CH4-CO-OH (ECCOHv1.01) Chemistry Module for 3D Model Applications

NASA Technical Reports Server (NTRS)

Elshorbany, Yasin F.; Duncan, Bryan N.; Strode, Sarah A.; Wang, James S.; Kouatchou, Jules

2016-01-01

We present the Efficient CH4-CO-OH (ECCOH) chemistry module that allows for the simulation of the methane, carbon monoxide, and hydroxyl radical (CH4-CO- OH) system, within a chemistry climate model, carbon cycle model, or Earth system model. The computational efficiency of the module allows many multi-decadal sensitivity simulations of the CH4-CO-OH system, which primarily determines the global atmospheric oxidizing capacity. This capability is important for capturing the nonlinear feedbacks of the CH4-CO-OH system and understanding the perturbations to methane, CO, and OH, and the concomitant impacts on climate. We implemented the ECCOH chemistry module in the NASA GEOS-5 atmospheric global circulation model (AGCM), performed multiple sensitivity simulations of the CH4-CO-OH system over 2 decades, and evaluated the model output with surface and satellite data sets of methane and CO. The favorable comparison of output from the ECCOH chemistry module (as configured in the GEOS- 5 AGCM) with observations demonstrates the fidelity of the module for use in scientific research.

Methane production in ruminants: Its effect on the doubly labeled water method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Midwood, A.J.; Haggarty, P.; McGaw, B.A.

1989-12-01

The doubly labeled water (DLW) technique for measuring CO2 production (rCO2) in free-living animals requires an assessment of the elimination of both 2H and 18O from the body over a long period of time. To calculate rCO2, it is necessary to calculate water turnover (rH2O) from the 2H flux rate. In ruminant animals, the accuracy of this calculation is affected by the loss of 2H in methane. We have quantified the effect of methane production (rCH4) on the 2H flux rate, determined in four sheep given 2H2O. The methane produced was depleted in 2H relative to the urine. A relationshipmore » between the enrichment of the methane and urine was established. The ratio of urine to methane enrichment was found on average to be 0.6536, and this value was unaffected by the level of rCH4 but showed some dependence on the absolute concentration of 2H in urine. For this reason, the ratio value obtained from four sheep not given 2H2O was different, a mean of 0.6886 was measured, this ratio was unaffected by changes in the diet supplied to the animals. Computer modeling was used to illustrate the dependence of the isotopically derived value for rCO2 on not only rCH4 but also the magnitude of rCO2 itself. The effect of rCH4 on the DLW method can be predicted from the observed ratio of rCO2 to rCH4 and the value of 0.6536 obtained for the ratio of methane to urine enrichment. With the use of data from several studies at this Institute, a limited range of 10 to 20 was found for rCO2/rCH4 in animals fed at or above maintenance.« less

Airborne Measurements of Atmospheric Methane Using Pulsed Laser Transmitters

NASA Technical Reports Server (NTRS)

Numata, Kenji; Riris, Haris; Wu, Stewart; Gonzalez, Brayler; Rodriguez, Michael; Hasselbrack, William; Fahey, Molly; Yu, Anthony; Stephen, Mark; Mao, Jianping;

Exploratory study of atmospheric methane enhancements derived from natural gas use in the Houston urban area

DOE PAGES

Sanchez, Nancy P.; Zheng, Chuantao; Ye, Weilin; ...

2018-01-04

Here, the extensive use of natural gas (NG) in urban areas for heating, cooking and as a vehicular fuel is associated with potentially significant emissions of methane (CH 4) to the atmosphere. Methane, a potent greenhouse gas that influences the chemistry of the atmosphere, can be emitted from different sources including leakage from NG infrastructure, transportation activities, end-use uncombusted NG, landfills and livestock. Although significant CH 4 leakage associated with aging local NG distribution systems in the U.S. has been reported, further investigation is required to study the role of this infrastructure component and other NG-related sources in atmospheric CHmore » 4 enhancements in urban centers. In this study, neighborhood-scale mobile-based monitoring of potential CH 4 emissions associated with NG in the Greater Houston area (GHA) is reported. A novel dual-gas 3.337 μm interband cascade laser-based sensor system was developed and mobile-mode deployed for simultaneous CH 4 and ethane (C 2H 6) monitoring during a period of over 14 days, corresponding to ~ 90 hours of effective data collection during summer 2016. The sampling campaign covered ~ 250 road miles and was primarily concentrated on eight residential zones with distinct infrastructure age and NG usage levels. A moderate number of elevated CH 4 concentration events (37 episodes) with mixing ratios not exceeding 3.60 ppmv and associated with atmospheric background enhancements below 1.21 ppmv were observed during the field campaign. Source discrimination analyses based on the covariance between CH 4 and C 2H 6 levels indicated the predominance of thermogenic sources (e.g., NG) in the elevated CH 4 concentration episodes. The volumetric fraction of C 2H 6 in the sources associated with the thermogenic CH 4 spikes varied between 2.7 and 5.9%, concurring with the C 2H 6 content in NG distributed in the GHA. Isolated CH 4 peak events with significantly higher C 2H 6 enhancements (~11 %) were observed at industrial areas and locations with high density of petroleum and gas pipelines in the GHA, indicating potential variability in Houston’s thermogenic CH 4 sources.« less

Exploratory study of atmospheric methane enhancements derived from natural gas use in the Houston urban area

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sanchez, Nancy P.; Zheng, Chuantao; Ye, Weilin

Here, the extensive use of natural gas (NG) in urban areas for heating, cooking and as a vehicular fuel is associated with potentially significant emissions of methane (CH 4) to the atmosphere. Methane, a potent greenhouse gas that influences the chemistry of the atmosphere, can be emitted from different sources including leakage from NG infrastructure, transportation activities, end-use uncombusted NG, landfills and livestock. Although significant CH 4 leakage associated with aging local NG distribution systems in the U.S. has been reported, further investigation is required to study the role of this infrastructure component and other NG-related sources in atmospheric CHmore » 4 enhancements in urban centers. In this study, neighborhood-scale mobile-based monitoring of potential CH 4 emissions associated with NG in the Greater Houston area (GHA) is reported. A novel dual-gas 3.337 μm interband cascade laser-based sensor system was developed and mobile-mode deployed for simultaneous CH 4 and ethane (C 2H 6) monitoring during a period of over 14 days, corresponding to ~ 90 hours of effective data collection during summer 2016. The sampling campaign covered ~ 250 road miles and was primarily concentrated on eight residential zones with distinct infrastructure age and NG usage levels. A moderate number of elevated CH 4 concentration events (37 episodes) with mixing ratios not exceeding 3.60 ppmv and associated with atmospheric background enhancements below 1.21 ppmv were observed during the field campaign. Source discrimination analyses based on the covariance between CH 4 and C 2H 6 levels indicated the predominance of thermogenic sources (e.g., NG) in the elevated CH 4 concentration episodes. The volumetric fraction of C 2H 6 in the sources associated with the thermogenic CH 4 spikes varied between 2.7 and 5.9%, concurring with the C 2H 6 content in NG distributed in the GHA. Isolated CH 4 peak events with significantly higher C 2H 6 enhancements (~11 %) were observed at industrial areas and locations with high density of petroleum and gas pipelines in the GHA, indicating potential variability in Houston’s thermogenic CH 4 sources.« less

Effect of oilseed source on ruminal fermentation and methane production of a grass-legume diet in continuous culture

USDA-ARS?s Scientific Manuscript database

Addition of oilseeds to pasture-based ruminant diets has been shown to decrease enteric CH4 emissions. However, little research has directly compared the effect of oilseed source on ruminal fermentation and Methane (CH4) production. A 4-unit continuous culture fermentor system was used to test 4 oil...

Advances in Methane Isotope Measurements via Direct Absorption Spectroscopy with Applications to Oil and Gas Source Characterization

NASA Astrophysics Data System (ADS)

Yacovitch, T. I.; Herndon, S. C.; Roscioli, J. R.; Petron, G.; Shorter, J. H.; Jervis, D.; McManus, J. B.; Nelson, D. D.; Zahniser, M. S.; Kolb, C. E., Jr.

2015-12-01

Instrumental developments in the measurement of multiple isotopes of methane (12CH4, 13CH4 and 12CH3D) are presented. A first generation 8-micron instrument quantifies 12CH4 and 13CH4 at a 1-second rate via tunable infrared direct absorption spectroscopy (TILDAS). A second generation instrument uses two 3-micron intraband cascade lasers in an Aerodyne dual laser chassis for simultaneous measurement of 12CH4, 13CH4 and 12CH3D. Sensitivity and noise performance improvements are examined. The isotopic signature of methane provides valuable information for emission source identification of this greenhouse gas. A first generation spectrometer has been deployed in the field on a mobile laboratory along with a sophisticated 4-tank calibration system. Calibrations are done on an agressive schedule, allowing for the correction of measured isotope ratios to an absolute isotope scale. Distinct isotopic signatures are found for a number of emission sources in the Denver-Julesburg Basin: oil and gas gathering stations, compressor stations and processing plants; a municipal landfill, and dairy/cattle operations. The isotopic signatures are compared with measured ethane/methane ratios. These direct absorption measurements have larger uncertainties than samples measured via gas chromatography-mass spectrometry, but have several advantages over canister sampling methods: individual sources of short duration are easier to isolate; calibrated isotope ratio results are available immediately; replicate measurements on a single source are easily performed; and the number of sources sampled is not limited by canister availability and processing time.

ESTIMATE OF METHANE EMISSIONS FROM U.S. LANDFILLS

EPA Science Inventory

The report describes the development of a statistical regression model used for estimating methane (CH4) emissions, which relates landfill gas (LFG) flow rates to waste-in-place data from 105 landfills with LFG recovery projects. (NOTE: CH4 flow rates from landfills with LFG reco...

Accuracy of noninvasive breath methane measurements using Fourier transform infrared methods on individual cows.

PubMed

Lassen, J; Løvendahl, P; Madsen, J

2012-02-01

Individual methane (CH(4)) production was recorded repeatedly on 93 dairy cows during milking in an automatic milking system (AMS), with the aim of estimating individual cow differences in CH(4) production. Methane and CO(2) were measured with a portable air sampler and analyzer unit based on Fourier transform infrared (FTIR) detection. The cows were 50 Holsteins and 43 Jerseys from mixed parities and at all stages of lactation (mean=156 d in milk). Breath was captured by the FTIR unit inlet nozzle, which was placed in front of the cow's head in each of the 2 AMS as an admixture to normal barn air. The FTIR unit was running continuously for 3 d in each of 2 AMS units, 1 with Holstein and another with Jersey cows. Air was analyzed every 20 s. From each visit of a cow to the AMS, CH(4) and CO(2) records were summarized into the mean, median, 75, and 90% quantiles. Furthermore, the ratio between CH(4) and CO(2) was used as a derived measure with the idea of using CO(2) in breath as a tracer gas to quantify the production of methane. Methane production records were analyzed with a mixed model, containing cow as random effect. Fixed effects of milk yield and daily intake of the total mixed ration and concentrates were also estimated. The repeatability of the CH(4)-to-CO(2) ratio was 0.39 for Holsteins and 0.34 for Jerseys. Both concentrate intake and total mixed ration intake were positively related to CH(4) production, whereas milk production level was not correlated with CH(4) production. In conclusion, the results from this study suggest that the CH(4)-to-CO(2) ratio measured using the noninvasive method is an asset of the individual cow and may be useful in both management and genetic evaluations. Copyright © 2012 American Dairy Science Association. Published by Elsevier Inc. All rights reserved.

Management practices and controls on methane emissions from sub-tropical wetlands

NASA Astrophysics Data System (ADS)

DeLucia, Nicholas; Casa-Nova Gomez, Nuri; Bernacchi, Carl

2015-04-01

It is well documented that green house gas concentrations have risen at unequivocal rates since the industrial revolution but the disparity between anthropogenic sources and natural sources is uncertain. Wetlands are one example of a natural ecosystem that can be a substantial source or sink for methane (CH4) depending on any combination of climate conditions, natural and anthropogenic disturbances, or ecosystem perturbations. Due to strict anaerobic conditions required for CH4-generating microorganisms, natural wetlands are the main source for biogenic CH4. Although wetlands occupy less than 5% of total land surface area, they contribute approximately 20% of total CH4 emissions to the atmosphere. CH4 is one of the most damaging green house gases with current emission estimates ranging from 55 to 231 Tg CH4 yr-1. The processes regulating CH4 emissions are sensitive to land use and management practices of areas surrounding wetlands. Variation in adjacent vegetation or grazing intensity by livestock can, for example, alter CH4 fluxes from wetland soils by altering nutrient balance, carbon inputs and hydrology. Therefore, understanding how these changes will affect wetland source strength is essential to understand the impact of wetland management practices on the global climate system. In this study we quantify wetland methane fluxes from subtropical wetlands on a working cattle ranch in central Florida near Okeechobee Lake (27o10'52.04"N, 81o21'8.56"W). To determine differences in CH4 fluxes associated with land use and management, a replicated (n = 4) full factorial experiment was designed for wetlands where the surrounding vegetation was (1) grazed or un-grazed and (2) composed of native vegetation or improved pasture. Net exchange of CH4 and CO2 between the land surface and the atmosphere were sampled with a LICOR Li-7700 open path CH4 analyzer and Li-7500A open path CO2/H20 analyzer mounted in a 1-m3 static gas-exchange chamber. Our results showed and verified that CH4 emissions from subtropical wetlands were larger when high soil moisture was coupled with high temperatures. Grazing alone, does not appear to alter net ecosystem CH4 emissions from subtropical semi-native and improved wetlands. Pasture type is a stronger indicator of wetland methane potential. Wetlands embedded in improved pastures exhibited periods of increased methane emission that was particularly noticeable during the wet season (July- Nov). These results help quantify GHG emissions from subtropical wetlands under different management practices while demonstrating the differences in these fluxes based on the surrounding ecosystem.

A novel pathway of direct methane production and emission by eukaryotes including plants, animals and fungi: An overview

NASA Astrophysics Data System (ADS)

Liu, Jiangong; Chen, Huai; Zhu, Qiuan; Shen, Yan; Wang, Xue; Wang, Meng; Peng, Changhui

2015-08-01

Methane (CH4) is a powerful greenhouse gas with a global warming potential 28 times that of carbon dioxide (CO2). CH4 is responsible for approximately 20% of the Earth's warming since pre-industrial times. Knowledge of the sources of CH4 is crucial due to the recent substantial interannual variability of growth rates and uncertainties regarding individual sources. The prevailing paradigm is that methanogenesis carried out by methanogenic archaea occurs primarily under strictly anaerobic conditions. However, in the past decade, studies have confirmed direct CH4 release from three important kingdoms of eukaryotes-Plantae, Animalia and Fungi-even in the presence of oxygen. This novel CH4 production pathway has been aptly termed ;aerobic CH4 production; to distinguish it from the well-known anaerobic CH4 production pathway, which involves catalytic activity by methanogenic archaeal enzymes. In this review, we collated recent experimental evidence from the published literature and documented this novel pathway of direct CH4 production and emission by eukaryotes. The mechanisms involved in this pathway may be related to protective strategies of eukaryotes in response to changing environmental stresses, with CH4 a by-product or end-product during or at the end of the process(es) that originates from organic methyl-type compounds. Based on the existing, albeit uncertain estimates, plants seem to contribute less to the global CH4 budget (3-24%) compared to previous estimates (10-37%). We still lack estimates of CH4 emissions by animals and fungi. Overall, there is an urgent need to identify the precursors for this novel CH4 source and improve our understanding of the mechanisms of direct CH4 production and the impacts of environmental stresses. An estimate of this new CH4 source, which was not considered as a CH4 source by the Intergovernmental Panel on Climate Change (IPCC) (2013), could be useful for better quantitation of the global CH4 budget.

The stable carbon isotope composition of methane produced and emitted from northern peatlands

NASA Astrophysics Data System (ADS)

Hornibrook, Edward R. C.

Stable carbon isotope values, pore water concentration, and flux data for methane (CH4) were compiled for 26 peatlands situated in the northern hemisphere to explore relationships between trophic status and CH4 cycling. Methane produced in ombrotrophic bogs has δ13C values that are significantly more negative than CH4 formed in fens apparently because of poor dissociation of acetic acid or an absence of methanogenic archaea capable of metabolizing acetic acid under low pH conditions. The δ 13C values of CH4 in pore water of ombrotrophic and minerotrophic peatlands exhibit the opposite trend: δ13C(CH4) values become more positive with depth in rain-fed bogs and more negative with depth in fens. The key zone for methanogenesis occurs at shallow depths in both types of peatland and consequently, δ13C values of CH4 emitted from ombrotrophic bogs (-74.9 ± 9.8‰ n = 42) are more negative than from fens (-64.8 ± 4.0‰ n = 38). An abundance of graminoids in fens contributes to more positive δ13C(CH4) values in pore water through (1) release of root exudates which promotes aceticlastic methanogenesis, (2) rhizosphere oxidization of CH4 causing localized enrichment of 13CH4, and (3) preferential export of 12CH4 through aerenchyma, which also enriches pore water in 13CH4. Emissions from blanket bogs and raised bogs should be attributed more negative δ13C(CH4) values relative to fens in isotope-weighted mass balance budgets. Further study is needed of bogs that have an apparently low nutrient status but exhibit a pore water distribution of δ13C(CH4) values similar to fens.

Sensitivity Analysis Reveals Critical Factors that Affect Wetland Methane Emissions using Soil Biogeochemistry Model

NASA Astrophysics Data System (ADS)

Alonso-Contes, C.; Gerber, S.; Bliznyuk, N.; Duerr, I.

2017-12-01

Wetlands contribute approximately 20 to 40 % to global sources of methane emissions. We build a Methane model for tropical and subtropical forests, that allows inundated conditions, following the approaches used in more complex global biogeochemical emission models (LPJWhyMe and CLM4Me). The model was designed to replace model formulations with field and remotely sensed collected data for 2 essential drivers: plant productivity and hydrology. This allows us to directly focus on the central processes of methane production, consumption and transport. One of our long term goals is to make the model available to a scientists interested in including methane modeling in their location of study. Sensitivity analysis results help in focusing field data collection efforts. Here, we present results from a pilot global sensitivity analysis of the model order to determine which parameters and processes contribute most to the model's uncertainty of methane emissions. Results show that parameters related to water table behavior, carbon input (in form of plant productivity) and rooting depth affect simulated methane emissions the most. Current efforts include to perform the sensitivity analysis again on methane emissions outputs from an updated model that incorporates a soil heat flux routine and to determine the extent by which the soil temperature parameters affect CH4 emissions. Currently we are conducting field collection of data during Summer 2017 for comparison among 3 different landscapes located in the Ordway-Swisher Biological Station in Melrose, FL. We are collecting soil moisture and CH4 emission data from 4 different wetland types. Having data from 4 wetland types allows for calibration of the model to diverse soil, water and vegetation characteristics.

Rice emissions during field flooding and air pollution feedbacks across South Korea

NASA Astrophysics Data System (ADS)

So, C.; Diskin, G. S.; DiGangi, J. P.; Choi, Y.; Rana, M.; Hughes, S.; Blake, D. R.; Nault, B.; Schroeder, J.; Campuzano Jost, P.; Jimenez, J. L.; Kim, M. J.; Teng, A.; Crounse, J. D.; Wenneberg, P.; Kaser, L.; Mikoviny, T.; Müller, M.; Wisthaler, A.; Pusede, S. E.

2017-12-01

Nitrous oxide (N2O) and methane (CH4) are important long-lived greenhouse gases. Known anthropogenic sources of these gases include rice cultivation, which represents anywhere between 5% and 20% of methane emissions globally. Other volatile molecules are also produced by soil biogeochemistry when rice fields are flooded, including small organic oxygenates. Here, we use recent aircraft measurements from the KORUS-AQ experiment to describe controls over rice emissions of N2O and CH4 at regional-scales across the South Korean Peninsula. We also investigate potential emissions of molecular hydrogen and volatile alcohols and organic acids and consider the effect of aerosol nitrate and sulfate deposition on rice soil biogeochemistry on paddies downwind of polluted urban areas.

Methane Emissions from Semi-natural, Drained and Re-wetted Peatlands in Germany

NASA Astrophysics Data System (ADS)

Tiemeyer, B.; Bechtold, M.; Albiac Borraz, E.; Augustin, J.; Drösler, M.; Beetz, S.; Beyer, C.; Eickenscheidt, T.; Fiedler, S.; Förster, C.; Giebels, M.; Glatzel, S.; Heinichen, J.; Höper, H.; Leiber-Sauheitl, K.; Peichl-Brak, M.; Rosskopf, N.; Sommer, M.; Zeitz, J.; Freibauer, A.

2014-12-01

Drained peatlands contribute around 5% to the total German greenhouse gas emissions. While these areas are hotspots for carbon dioxide (CO2) and nitrous oxide (N2O) emissions, some re-wetted peatlands may emit large amounts of methane (CH4). To quantify the GHG emission reductions achieved by the re-wetting of peatlands, the reduced CO2 emissions and the potential CH4fluxes need to be balanced. We synthesized methane flux data from 14 peatlands with 122 sites. At each site, methane fluxes were measured for one to three years with static chambers. The sites comprise arable land, intensive and extensive grassland, forest and peat mining areas as well as semi-natural and re-wetted peatlands on both bog peat, fen peat and other soils rich in organic carbon. Besides the groundwater table we consider further potential drivers for the CH4fluxes such as soil properties (carbon, nitrogen, pH, and physical properties), climatic parameters, land use, and vegetation composition. Annual methane fluxes ranged from low uptake rates (around -1 g CH4-C m² a-1) to very high emissions (> 200 g CH4-C m² a-1). Intensively drained sites showed very low emissions, while for annual mean water levels higher than 5-10 cm below ground, elevated emissions of more than 20 g CH4-C may occur. At some re-wetted sites CH4 emissions of more than 100 g CH4-C m² a-1 were measured, which roughly equal the Global Warming Potential of the CO2-emissions from intensively drained agricultural sites. These high fluxes were probably caused by a combination of nutrient-rich conditions, the dieback of poorly adapted plants and a fast accumulation of organic sediments. However, this was the exception and not the rule even for very wet re-wetted sites. Achieving a model efficiency of 0.72 during cross-validation, a boosted regression tree (BRT) model was well able to describe logarithmic CH4-fluxes. Groundwater level, biotope type, soil nitrogen content, and ponding duration during summer were the most important controls. Combining the BRT model with soil, land use, and groundwater table maps as well as weather data, methane fluxes were upscaled for Germany.

A two component model for thermal emission from organic grains in Comet Halley

NASA Technical Reports Server (NTRS)

Chyba, Christopher; Sagan, Carl

1988-01-01

Observations of Comet Halley in the near infrared reveal a triple-peaked emission feature near 3.4 micrometer, characteristic of C-H stretching in hydrocarbons. A variety of plausible cometary materials exhibit these features, including the organic residue of irradiated candidate cometary ices (such as the residue of irradiated methane ice clathrate, and polycyclic aromatic hydrocarbons. Indeed, any molecule containing -CH3 and -CH2 alkanes will emit at 3.4 micrometer under suitable conditions. Therefore tentative identifications must rest on additional evidence, including a plausible account of the origins of the organic material, a plausible model for the infrared emission of this material, and a demonstration that this conjunction of material and model not only matches the 3 to 4 micrometer spectrum, but also does not yield additional emission features where none is observed. In the case of the residue of irradiated low occupancy methane ice clathrate, it is argued that the lab synthesis of the organic residue well simulates the radiation processing experienced by Comet Halley.

Role of atmospheric oxidation in recent methane growth

PubMed Central

Rigby, Matthew; Montzka, Stephen A.; Prinn, Ronald G.; White, James W. C.; Young, Dickon; Lunt, Mark F.; Ganesan, Anita L.; Manning, Alistair J.; Simmonds, Peter G.; Salameh, Peter K.; Harth, Christina M.; Mühle, Jens; Weiss, Ray F.; Fraser, Paul J.; Steele, L. Paul; McCulloch, Archie; Park, Sunyoung

2017-01-01

The growth in global methane (CH4) concentration, which had been ongoing since the industrial revolution, stalled around the year 2000 before resuming globally in 2007. We evaluate the role of the hydroxyl radical (OH), the major CH4 sink, in the recent CH4 growth. We also examine the influence of systematic uncertainties in OH concentrations on CH4 emissions inferred from atmospheric observations. We use observations of 1,1,1-trichloroethane (CH3CCl3), which is lost primarily through reaction with OH, to estimate OH levels as well as CH3CC3 emissions, which have uncertainty that previously limited the accuracy of OH estimates. We find a 64–70% probability that a decline in OH has contributed to the post-2007 methane rise. Our median solution suggests that CH4 emissions increased relatively steadily during the late 1990s and early 2000s, after which growth was more modest. This solution obviates the need for a sudden statistically significant change in total CH4 emissions around the year 2007 to explain the atmospheric observations and can explain some of the decline in the atmospheric 13CH4/12CH4 ratio and the recent growth in C2H6. Our approach indicates that significant OH-related uncertainties in the CH4 budget remain, and we find that it is not possible to implicate, with a high degree of confidence, rapid global CH4 emissions changes as the primary driver of recent trends when our inferred OH trends and these uncertainties are considered. PMID:28416657

Inventory of anthropogenic methane emissions in mainland China from 1980 to 2010

NASA Astrophysics Data System (ADS)

Peng, Shushi; Piao, Shilong; Bousquet, Philippe; Ciais, Philippe; Li, Bengang; Lin, Xin; Tao, Shu; Wang, Zhiping; Zhang, Yuan; Zhou, Feng

2016-11-01

Methane (CH4) has a 28-fold greater global warming potential than CO2 over 100 years. Atmospheric CH4 concentration has tripled since 1750. Anthropogenic CH4 emissions from China have been growing rapidly in the past decades and contribute more than 10 % of global anthropogenic CH4 emissions with large uncertainties in existing global inventories, generally limited to country-scale statistics. To date, a long-term CH4 emission inventory including the major sources sectors and based on province-level emission factors is still lacking. In this study, we produced a detailed annual bottom-up inventory of anthropogenic CH4 emissions from the eight major source sectors in China for the period 1980-2010. In the past 3 decades, the total CH4 emissions increased from 24.4 [18.6-30.5] Tg CH4 yr-1 in 1980 (mean [minimum-maximum of 95 % confidence interval]) to 44.9 [36.6-56.4] Tg CH4 yr-1 in 2010. Most of this increase took place in the 2000s decade with averaged yearly emissions of 38.5 [30.6-48.3] Tg CH4 yr-1. This fast increase of the total CH4 emissions after 2000 is mainly driven by CH4 emissions from coal exploitation. The largest contribution to total CH4 emissions also shifted from rice cultivation in 1980 to coal exploitation in 2010. The total emissions inferred in this work compare well with the EPA inventory but appear to be 36 and 18 % lower than the EDGAR4.2 inventory and the estimates using the same method but IPCC default emission factors, respectively. The uncertainty of our inventory is investigated using emission factors collected from state-of-the-art published literatures. We also distributed province-scale emissions into 0.1° × 0.1° maps using socioeconomic activity data. This new inventory could help understanding CH4 budgets at regional scale and guiding CH4 mitigation policies in China.

Methane potential from municipal biowaste: Insights from six communities in Maharashtra, India.

PubMed

Breitenmoser, Lena; Dhar, Hiya; Gross, Thomas; Bakre, Milan; Huesch, Ragini; Hugi, Christoph; Wintgens, Thomas; Kumar, Rakesh; Kumar, Sunil

2018-04-01

Anaerobic digestion (AD) of biowaste can generate biogas with methane (CH 4 ) as energy source and contribute to sustainable municipal solid waste management in India. Characteristic municipal biowastes sampled seasonally from household, fruit and vegetable market and agricultural waste collection points in villages, towns and cities in Maharashtra were analysed to assess the potential as substrate for AD. The mean biochemical methane potential (BMP, at 37 °C) across seasons and community sizes was between 200-260, 175-240 and 101-286 NL CH4  kg vs -1 for household, market and agricultural biowaste, respectively. CH 4 yields were comparable in villages, towns and cities. Seasonal variations in CH 4 yields were observed for market and agricultural biowaste with highest values during pre-monsoon season. Results underpin that municipal biowaste is a suitable substrate for AD in India. However, low purity of available biowaste resulted in lower CH 4 yields compared to recent studies using source-segregated biowaste. Copyright © 2018 Elsevier Ltd. All rights reserved.

Determination of as-discarded methane potential in residential and commercial municipal solid waste.

PubMed

Chickering, Giles W; Krause, Max J; Townsend, Timothy G

2018-06-01

Methane generation potential, L 0 , is a primary parameter of the first-order decay (FOD) model used for prediction and regulation of landfill gas (LFG) generation in municipal solid waste (MSW) landfills. The current US EPA AP-42 default value for L 0 , which has been in place for almost 20 years, is 100 m 3 CH 4 /Mg MSW as-discarded. Recent research suggests the yield of landfilled waste could be less than 60 m 3 CH 4 /Mg MSW. This study aimed to measure the L 0 of present-day residential and commercial as-discarded MSW. In doing so, 39 waste collection vehicles were sorted for composition before samples of each biodegradable fraction were analyzed for methane generation potential. Methane yields were determined for over 450 samples of 14 different biodegradable MSW fractions, later to be combined with moisture content and volatile solids data to calculate L 0 values for each waste load. An average value of 80 m 3 CH 4 /Mg MSW was determined for all samples with 95% of values in the interval 74-86 m 3 CH 4 /Mg MSW as-discarded. While no statistically significant difference was observed, commercial MSW yields (mean 85, median 88 m 3 CH 4 /Mg MSW) showed a higher average L 0 than residential MSW (mean 75, median 71 m 3 CH 4 /Mg MSW). Many methane potential values for individual fractions described in previous work were found within the range of values determined by BMP in this study. Copyright © 2018 Elsevier Ltd. All rights reserved.

Rapid Sediment Accumulation Results in High Methane Effluxes from Coastal Sediments

PubMed Central

Lenstra, Wytze; Jong, Dirk; Meysman, Filip J. R.; Sapart, Célia J.; van der Veen, Carina; Röckmann, Thomas; Gonzalez, Santiago; Slomp, Caroline P.

2016-01-01

Globally, the methane (CH4) efflux from the ocean to the atmosphere is small, despite high rates of CH4 production in continental shelf and slope environments. This low efflux results from the biological removal of CH4 through anaerobic oxidation with sulfate in marine sediments. In some settings, however, pore water CH4 is found throughout the sulfate-bearing zone, indicating an apparently inefficient oxidation barrier for CH4. Here we demonstrate that rapid sediment accumulation can explain this limited capacity for CH4 removal in coastal sediments. In a saline coastal reservoir (Lake Grevelingen, The Netherlands), we observed high diffusive CH4 effluxes from the sediment into the overlying water column (0.2–0.8 mol m-2 yr-1) during multiple years. Linear pore water CH4 profiles and the absence of an isotopic enrichment commonly associated with CH4 oxidation in a zone with high rates of sulfate reduction (50–170 nmol cm-3 d-1) both suggest that CH4 is bypassing the zone of sulfate reduction. We propose that the rapid sediment accumulation at this site (~ 13 cm yr-1) reduces the residence time of the CH4 oxidizing microorganisms in the sulfate/methane transition zone (< 5 years), thus making it difficult for these slow growing methanotrophic communities to build-up sufficient biomass to efficiently remove pore water CH4. In addition, our results indicate that the high input of organic matter (~ 91 mol C m-2 yr-1) allows for the co-occurrence of different dissimilatory respiration processes, such as (acetotrophic) methanogenesis and sulfate reduction in the surface sediments by providing abundant substrate. We conclude that anthropogenic eutrophication and rapid sediment accumulation likely increase the release of CH4 from coastal sediments. PMID:27560511

Infrared Spectroscopy of the Entrance Channel Complex Formed Between the Hydroxyl Radical and Methane in Helium Nanodroplets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Raston, Paul L.; Obi, Emmanuel I.; Douberly, Gary E.

Here, the entrance channel complex in the exothermic OH + CH 4 → H 2O + CH 3 reaction has been isolated in helium nanodroplets following the sequential pick-up of the hydroxyl radical and methane. The a-type OH stretching band was probed with infrared depletion spectroscopy, revealing a spectrum qualitatively similar to that previously reported in the gas phase, but with additional substructure that is due to the different internal rotation states of methane (j CH4 = 0, 1, or 2) in the complex. We fit the spectra by assuming the rotational constants of the complex are the same formore » all internal rotation states; however, subband origins are found to decrease with increasing j CH4. Measurements of deuterated complexes have also been made (OD–CH 4, OH–CD 4, and OD–CD 4), the relative linewidths of which provide information about the flow of vibrational energy in the complexes; vibrational lifetime broadening is prominent for OH–CH 4 and OD–CD 4, for which the excited OX stretching state has a nearby CY 4 stretching fundamental (X, Y = H or D).« less

Infrared Spectroscopy of the Entrance Channel Complex Formed Between the Hydroxyl Radical and Methane in Helium Nanodroplets

DOE PAGES

Raston, Paul L.; Obi, Emmanuel I.; Douberly, Gary E.

2017-09-22

Here, the entrance channel complex in the exothermic OH + CH 4 → H 2O + CH 3 reaction has been isolated in helium nanodroplets following the sequential pick-up of the hydroxyl radical and methane. The a-type OH stretching band was probed with infrared depletion spectroscopy, revealing a spectrum qualitatively similar to that previously reported in the gas phase, but with additional substructure that is due to the different internal rotation states of methane (j CH4 = 0, 1, or 2) in the complex. We fit the spectra by assuming the rotational constants of the complex are the same formore » all internal rotation states; however, subband origins are found to decrease with increasing j CH4. Measurements of deuterated complexes have also been made (OD–CH 4, OH–CD 4, and OD–CD 4), the relative linewidths of which provide information about the flow of vibrational energy in the complexes; vibrational lifetime broadening is prominent for OH–CH 4 and OD–CD 4, for which the excited OX stretching state has a nearby CY 4 stretching fundamental (X, Y = H or D).« less

Activity and diversity of methane-oxidizing bacteria in glacier forefields on siliceous and calcareous bedrock

NASA Astrophysics Data System (ADS)

Nauer, P. A.; Dam, B.; Liesack, W.; Zeyer, J.; Schroth, M. H.

2012-06-01

The global methane (CH4) cycle is largely driven by methanogenic archaea and methane-oxidizing bacteria (MOB), but little is known about their activity and diversity in pioneer ecosystems. We conducted a field survey in forefields of 13 receding Swiss glaciers on both siliceous and calcareous bedrock to investigate and quantify CH4 turnover based on soil-gas CH4 concentration profiles, and to characterize the MOB community by sequencing and terminal restriction fragment length polymorphism (T-RFLP) analysis of pmoA. Methane turnover was fundamentally different in the two bedrock categories. Of the 36 CH4 concentration profiles from siliceous locations, 11 showed atmospheric CH4 consumption at concentrations of ~1-2 μL L-1 with soil-atmosphere CH4 fluxes of -0.14 to -1.1 mg m-2 d-1. Another 11 profiles showed no apparent activity, while the remaining 14 exhibited slightly increased CH4 concentrations of ~2-10 μL L-1 , most likely due to microsite methanogenesis. In contrast, all profiles from calcareous sites suggested a substantial, yet unknown CH4 source below our sampling zone, with soil-gas CH4 concentrations reaching up to 1400 μL L-1. Remarkably, most soils oxidized ~90 % of the deep-soil CH4, resulting in soil-atmosphere fluxes of 0.12 to 31 mg m-2 d-1. MOB showed limited diversity in both siliceous and calcareous forefields: all identified pmoA sequences formed only 5 operational taxonomic units (OTUs) at the species level and, with one exception, could be assigned to either Methylocystis or the as-yet-uncultivated Upland Soil Cluster γ (USCγ). The latter dominated T-RFLP patterns of all siliceous and most calcareous samples, while Methylocystis dominated in 4 calcareous samples. Members of Upland Soil Cluster α (USCα) were not detected. Apparently, USCγ adapted best to the oligotrophic cold climate conditions at the investigated pioneer sites.

Seasonal and interannual variability in wetland methane emissions simulated by CLM4Me' and CAM-chem and comparisons to observations of concentrations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meng, L.; Paudel, R.; Hess, P. G. M.

Understanding the temporal and spatial variation of wetland methane emissions is essential to the estimation of the global methane budget. Our goal for this study is three-fold: (i) to evaluate the wetland methane fluxes simulated in two versions of the Community Land Model, the Carbon-Nitrogen (CN; i.e., CLM4.0) and the Biogeochemistry (BGC; i.e., CLM4.5) versions using the methane emission model CLM4Me' so as to determine the sensitivity of the emissions to the underlying carbon model; (ii) to compare the simulated atmospheric methane concentrations to observations, including latitudinal gradients and interannual variability so as to determine the extent to which themore » atmospheric observations constrain the emissions; (iii) to understand the drivers of seasonal and interannual variability in atmospheric methane concentrations. Simulations of the transport and removal of methane use the Community Atmosphere Model with chemistry (CAM-chem) model in conjunction with CLM4Me' methane emissions from both CN and BGC simulations and other methane emission sources from literature. In each case we compare model-simulated atmospheric methane concentration with observations. In addition, we simulate the atmospheric concentrations based on the TransCom wetland and rice paddy emissions derived from a different terrestrial ecosystem model, Vegetation Integrative Simulator for Trace gases (VISIT). Our analysis indicates CN wetland methane emissions are higher in the tropics and lower at high latitudes than emissions from BGC. In CN, methane emissions decrease from 1993 to 2004 while this trend does not appear in the BGC version. In the CN version, methane emission variations follow satellite-derived inundation wetlands closely. However, they are dissimilar in BGC due to its different carbon cycle. CAM-chem simulations with CLM4Me' methane emissions suggest that both prescribed anthropogenic and predicted wetlands methane emissions contribute substantially to seasonal and interannual variability in atmospheric methane concentration. Simulated atmospheric CH 4 concentrations in CAM-chem are highly correlated with observations at most of the 14 measurement stations evaluated with an average correlation between 0.71 and 0.80 depending on the simulation (for the period of 1993–2004 for most stations based on data availability). Our results suggest that different spatial patterns of wetland emissions can have significant impacts on Northern and Southern hemisphere (N–S) atmospheric CH 4 concentration gradients and growth rates. In conclusion, this study suggests that both anthropogenic and wetland emissions have significant contributions to seasonal and interannual variations in atmospheric CH 4 concentrations. However, our analysis also indicates the existence of large uncertainties in terms of spatial patterns and magnitude of global wetland methane budgets, and that substantial uncertainty comes from the carbon model underlying the methane flux modules.« less

Seasonal and interannual variability in wetland methane emissions simulated by CLM4Me' and CAM-chem and comparisons to observations of concentrations

DOE PAGES

Meng, L.; Paudel, R.; Hess, P. G. M.; ...

2015-07-03

Understanding the temporal and spatial variation of wetland methane emissions is essential to the estimation of the global methane budget. Our goal for this study is three-fold: (i) to evaluate the wetland methane fluxes simulated in two versions of the Community Land Model, the Carbon-Nitrogen (CN; i.e., CLM4.0) and the Biogeochemistry (BGC; i.e., CLM4.5) versions using the methane emission model CLM4Me' so as to determine the sensitivity of the emissions to the underlying carbon model; (ii) to compare the simulated atmospheric methane concentrations to observations, including latitudinal gradients and interannual variability so as to determine the extent to which themore » atmospheric observations constrain the emissions; (iii) to understand the drivers of seasonal and interannual variability in atmospheric methane concentrations. Simulations of the transport and removal of methane use the Community Atmosphere Model with chemistry (CAM-chem) model in conjunction with CLM4Me' methane emissions from both CN and BGC simulations and other methane emission sources from literature. In each case we compare model-simulated atmospheric methane concentration with observations. In addition, we simulate the atmospheric concentrations based on the TransCom wetland and rice paddy emissions derived from a different terrestrial ecosystem model, Vegetation Integrative Simulator for Trace gases (VISIT). Our analysis indicates CN wetland methane emissions are higher in the tropics and lower at high latitudes than emissions from BGC. In CN, methane emissions decrease from 1993 to 2004 while this trend does not appear in the BGC version. In the CN version, methane emission variations follow satellite-derived inundation wetlands closely. However, they are dissimilar in BGC due to its different carbon cycle. CAM-chem simulations with CLM4Me' methane emissions suggest that both prescribed anthropogenic and predicted wetlands methane emissions contribute substantially to seasonal and interannual variability in atmospheric methane concentration. Simulated atmospheric CH 4 concentrations in CAM-chem are highly correlated with observations at most of the 14 measurement stations evaluated with an average correlation between 0.71 and 0.80 depending on the simulation (for the period of 1993–2004 for most stations based on data availability). Our results suggest that different spatial patterns of wetland emissions can have significant impacts on Northern and Southern hemisphere (N–S) atmospheric CH 4 concentration gradients and growth rates. In conclusion, this study suggests that both anthropogenic and wetland emissions have significant contributions to seasonal and interannual variations in atmospheric CH 4 concentrations. However, our analysis also indicates the existence of large uncertainties in terms of spatial patterns and magnitude of global wetland methane budgets, and that substantial uncertainty comes from the carbon model underlying the methane flux modules.« less

Low-temperature conversion of methane to methanol on CeO x/Cu 2O catalysts: Water controlled activation of the C–H Bond

DOE PAGES

Zuo, Zhijun; Ramírez, Pedro J.; Senanayake, Sanjaya D.; ...

2016-10-10

Here, an inverse CeO 2/Cu 2O/Cu(111) catalyst is able to activate methane at room temperature producing C, CH x fragments and CO x species on the oxide surface. The addition of water to the system leads to a drastic change in the selectivity of methane activation yielding only adsorbed CH x fragments. At a temperature of 450 K, in the presence of water, a CH 4 → CH 3OH catalytic transformation occurs with a high selectivity. OH groups formed by the dissociation of water saturate the catalyst surface, removing sites that could decompose CH x fragments, and generating centers onmore » which methane can directly interact to yield methanol.« less

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

PubMed

Lee, Jun-Ho; Woo, Han Jun; Son, Seung-Kyu; Kim, Moonkoo; Lee, Dong-Hun; Tsunogai, Urumu; Jeong, Kap-Sik

2018-04-16

The flux and distribution of methane (CH 4 ) was investigated in the seawater column at 14 stations in the Gunsan Basin, the southeastern part of Yellow Sea from 2013 to 2015. Here CH 4 is concentrated 2.4-4.7 (3.4 ± 0.7) nM in the surface and 2.5-7.4 (5.2 ± 1.7) nM in the bottom layer. The CH 4 saturation ratios ranged from 65.5% to 295.5% (162.6 ± 68.7), comprising the mean sea-to-air CH 4 flux of 3.8 to 25.3 (15.6 ± 5.5) µM m -2 d -1 . Methane concentration was largely different in the upper and the lower seawater layers that is separated by the thermocline of which depth is variable (20-60 m) depending on the time of sampling. The concentration of seawater dissolved CH 4 is high between the bottom surface of the thermocline layer and the sea floor. Generally it tends to decrease from the south-westernmost part of the basin toward the west coast of Korea. This distribution pattern of CH 4 seems to result from the CH 4 supply by decomposition of organic matters produced in the upper seawater layer that is superimposed by the larger supply from the underlying sediment layer especially beneath the thermocline. The latter is manifested by ubiquitous CH 4 seeps from the seafloor sediments.

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

USDA-ARS?s Scientific Manuscript database

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...

Soil Methane Sink Capacity Response to a Long-Term Wildfire Chronosequence in Northern Sweden.

PubMed

McNamara, Niall P; Gregg, Ruth; Oakley, Simon; Stott, Andy; Rahman, Md Tanvir; Murrell, J Colin; Wardle, David A; Bardgett, Richard D; Ostle, Nick J

2015-01-01

Boreal forests occupy nearly one fifth of the terrestrial land surface and are recognised as globally important regulators of carbon (C) cycling and greenhouse gas emissions. Carbon sequestration processes in these forests include assimilation of CO2 into biomass and subsequently into soil organic matter, and soil microbial oxidation of methane (CH4). In this study we explored how ecosystem retrogression, which drives vegetation change, regulates the important process of soil CH4 oxidation in boreal forests. We measured soil CH4 oxidation processes on a group of 30 forested islands in northern Sweden differing greatly in fire history, and collectively representing a retrogressive chronosequence, spanning 5000 years. Across these islands the build-up of soil organic matter was observed to increase with time since fire disturbance, with a significant correlation between greater humus depth and increased net soil CH4 oxidation rates. We suggest that this increase in net CH4 oxidation rates, in the absence of disturbance, results as deeper humus stores accumulate and provide niches for methanotrophs to thrive. By using this gradient we have discovered important regulatory controls on the stability of soil CH4 oxidation processes that could not have not been explored through shorter-term experiments. Our findings indicate that in the absence of human interventions such as fire suppression, and with increased wildfire frequency, the globally important boreal CH4 sink could be diminished.

Soil Methane Sink Capacity Response to a Long-Term Wildfire Chronosequence in Northern Sweden

PubMed Central

McNamara, Niall P.; Gregg, Ruth; Oakley, Simon; Stott, Andy; Rahman, Md. Tanvir; Murrell, J. Colin; Wardle, David A.; Bardgett, Richard D.; Ostle, Nick J.

2015-01-01

Boreal forests occupy nearly one fifth of the terrestrial land surface and are recognised as globally important regulators of carbon (C) cycling and greenhouse gas emissions. Carbon sequestration processes in these forests include assimilation of CO2 into biomass and subsequently into soil organic matter, and soil microbial oxidation of methane (CH4). In this study we explored how ecosystem retrogression, which drives vegetation change, regulates the important process of soil CH4 oxidation in boreal forests. We measured soil CH4 oxidation processes on a group of 30 forested islands in northern Sweden differing greatly in fire history, and collectively representing a retrogressive chronosequence, spanning 5000 years. Across these islands the build-up of soil organic matter was observed to increase with time since fire disturbance, with a significant correlation between greater humus depth and increased net soil CH4 oxidation rates. We suggest that this increase in net CH4 oxidation rates, in the absence of disturbance, results as deeper humus stores accumulate and provide niches for methanotrophs to thrive. By using this gradient we have discovered important regulatory controls on the stability of soil CH4 oxidation processes that could not have not been explored through shorter-term experiments. Our findings indicate that in the absence of human interventions such as fire suppression, and with increased wildfire frequency, the globally important boreal CH4 sink could be diminished. PMID:26372346

METHANE EMISSIONS FROM THE U.S. PETROLEUM INDUSTRY

EPA Science Inventory

The report quantifies methane (CH4) emissions from the U.S. petroleum industry by identifying sources of CH4 from the production, transportation, and refining of oil. Emissions are reported for the base year 1993 and for the years 1986 through 1992, based on adjustments to the ba...

Limits and dynamics of methane oxidation in landfill cover soils

USDA-ARS?s Scientific Manuscript database

In order to understand the limits and dynamics of methane (CH4) oxidation in landfill cover soils, we investigated CH4 oxidation in daily, intermediate, and final cover soils from two California landfills as a function of temperature, soil moisture and CO2 concentration. The results indicate a signi...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 9: UNDERGROUND PIPELINES

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 14: GLYCOL DEHYDRATORS

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 8: EQUIPMENT LEAKS

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 5: ACTIVITY FACTORS

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 2: TECHNICAL REPORT

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 3: GENERAL METHODOLOGY

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 12: PNEUMATIC DEVICES

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 1: EXECUTIVE SUMMARY

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

High methane emissions from a midlatitude reservoir draining an agricultural watershed

EPA Science Inventory

To assess the magnitude of methane (CH4) emissions from reservoirs in mid-latitude agricultural regions, we measured CH4 and carbon dioxide (CO2) emission rates from William H. Harsha Lake, an agricultural impacted reservoir located in southwestern Ohio, USA, over a thirteen mont...

Effects of an experimental water-level drawdown on methane emissions from a eutrophic reservoir

EPA Science Inventory

Reservoirs are a globally significant source of methane (CH4) to the atmosphere. However, emission rate estimates may be biased low due to inadequate monitoring during brief periods of elevated emission rates (i.e. hot-moments). Here we investigate CH4 bubbling (i.e. ebullition...

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

NASA Astrophysics Data System (ADS)

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

2016-04-01

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

Assessing Methane in Shallow Groundwater in Unconventional Oil and Gas Play Areas, Eastern Kentucky.

PubMed

Zhu, Junfeng; Parris, Thomas M; Taylor, Charles J; Webb, Steven E; Davidson, Bart; Smath, Richard; Richardson, Stephen D; Molofsky, Lisa J; Kromann, Jenna S; Smith, Ann P

2018-05-01

The expanding use of horizontal drilling and hydraulic fracturing technology to produce oil and gas from tight rock formations has increased public concern about potential impacts on the environment, especially on shallow drinking water aquifers. In eastern Kentucky, horizontal drilling and hydraulic fracturing have been used to develop the Berea Sandstone and the Rogersville Shale. To assess baseline groundwater chemistry and evaluate methane detected in groundwater overlying the Berea and Rogersville plays, we sampled 51 water wells and analyzed the samples for concentrations of major cations and anions, metals, dissolved methane, and other light hydrocarbon gases. In addition, the stable carbon and hydrogen isotopic composition of methane (δ 13 C-CH 4 and δ 2 H-CH 4 ) was analyzed for samples with methane concentration exceeding 1 mg/L. Our study indicates that methane is a relatively common constituent in shallow groundwater in eastern Kentucky, where methane was detected in 78% of the sampled wells (40 of 51 wells) with 51% of wells (26 of 51 wells) exhibiting methane concentrations above 1 mg/L. The δ 13 C-CH 4 and δ 2 H-CH 4 ranged from -84.0‰ to -58.3‰ and from -246.5‰ to -146.0‰, respectively. Isotopic analysis indicated that dissolved methane was primarily microbial in origin formed through CO 2 reduction pathway. Results from this study provide a first assessment of methane in the shallow aquifers in the Berea and Rogersville play areas and can be used as a reference to evaluate potential impacts of future horizontal drilling and hydraulic fracturing activities on groundwater quality in the region. © 2017, National Ground Water Association.

Effect of temperature on continuous dry fermentation of swine manure.

PubMed

Deng, Liangwei; Chen, Chuang; Zheng, Dan; Yang, Hongnan; Liu, Yi; Chen, Ziai

2016-07-15

Laboratory-scale experiments were performed on the dry digestion of solid swine manure in a semi-continuous mode using 4.5 L down plug-flow anaerobic reactors with an organic loading rate of 3.46 kg volatile solids (VS) m(-3) d(-1) to evaluate the effects of temperature (15, 25 and 35 °C). At 15 °C, biogas production was the poorest due to organic overload and acidification, with a methane yield of 0.036 L CH4 g(-1) VS added and a volumetric methane production rate of 0.125 L CH4 L(-1) d(-1). The methane yield and volumetric methane production rate at 25 °C (0.226 L CH4 g(-1) VS added and 0.783 L CH4 L(-1) d(-1), respectively) were 6.24 times higher than those at 15 °C. However, the methane yield (0.237 L CH4 g(-1) VS added) and the volumetric methane production rate (0.821 L CH4 L(-1) d(-1)) at 35 °C were only 4.86% higher than those at 25 °C, which indicated similar results were obtained at 25 °C and 35 °C. The lower biogas production at 35 °C in dry digestion compared with that in wet digestion could be attributed to ammonia inhibition. For a single pig farm, digestion of solid manure is accomplished in small-scale domestic or small-farm bioreactors, for which operating temperatures of 35 °C are sometimes difficult to achieve. Considering biogas production, ammonia inhibition and net energy recovery, an optimum temperature for dry digestion of solid swine manure is 25 °C. Copyright © 2016 Elsevier Ltd. All rights reserved.

An investigation of regional tropospheric methane in central interior Alaska using direct-sun FTIR

NASA Astrophysics Data System (ADS)

Jacobs, N.; Simpson, W. R.; Strong, K.; Conway, S. A.; Kasai, Y.; Dubey, M. K.; Parker, H. A.; Hase, F.; Blumenstock, T.; Tu, Q.

2016-12-01

Observations suggest that a warming climate is causing permafrost degradation in the sub-Arctic to increase and the boundaries of the Boreal Forest to advance Northward. Many low-lying (often wetland) areas that were once frozen are thawing, changing soil processes, which have the potential to alter carbon gas exchange. Possible changes in carbon emissions in subarctic ecosystems, such as those found in central interior Alaska, warrant an investigation of atmospheric methane (CH4) on a regional scale. In a joint US-Japanese project, ground-based direct-sun Fourier Transform Infrared (FTIR) spectra were collected at Poker Flat Research Range, Alaska (65.12ºN, 147.43ºW) from 2000 to 2010 using a Bruker IFS120HR spectrometer. From these spectra, vertical profiles of CH4 volume mixing ratio (VMR), as a function of altitude, were estimated with SFIT4 fitting software. A method for calculating VMRs of tropospheric CH4 proposed by Washenfelder et al. (2003, DOI: 10.1029/2003gl017969) was explored and compared to profile estimates for layers with the lowest altitude. This method uses HF total column measurements as a proxy for CH4 oxidation in the stratosphere to correct for stratospheric methane loss. Comparative timeseries were constructed relating CH4 VMR estimated for the surface layer of SFIT4 profiles, tropospheric CH4 VMR calculated using HF total columns, and in situ data from the NOAA site in Barrow, Alaska. In this presentation, we compare the various methods for tropospheric methane measurements and present a timeseries of methane over the ten-year period. The observations can be used in the future to constrain regional methane budgets in the sub-Arctic/Boreal Forest region. Similar direct-sun FTIR observations with a pair of Bruker EM27/Sun mobile spectromoters are being carried out in August and September 2016, and preliminary results from this campaign will also be presented.

Infrared band intensities of saturated hydrocarbons

NASA Technical Reports Server (NTRS)

Pinkley, L. W.; Sethna, P. P.; Williams, D.

1978-01-01

Kramers-Kronig analysis is applied to measured values of spectral reflectance at near-normal incidence to determine the real and the imaginary parts of the complex index of refraction for methane, ethane, propane, n-butane, n-hexane, n-heptane, and n-decane in the liquid state. The results indicate that the strengths of the characteristic bands as measured by the integral of the imaginary part are roughly constant for all the liquid alkanes except for methane. The intensity of the CH valence vibration bands in the spectra of the alkanes except methane is directly proportional to the number of CH groups per unit volume. The relations for the intensity of the bands due to CH2 and CH3 deformations are examined. Characteristic band intensities of the type established for NH4(+) and SO4(2-) groups in solutions and crystals cannot be extended to the more closely coupled CH2 and CH3 groups in alkane molecules.

Testing and Validation Studies of the NSMII-Benthic Sediment Diagenesis Module

DTIC Science & Technology

2016-07-01

NSMII analytical vs. numerical solutions of sediment methane ............................ 27 3.2.4 Comparisons of the diagenesis rates of three sediment...26 Figure 12. Comparisons of NSMII analytical vs. numerical solutions of sediment methane : (a) layer 2’s CH4, (b...oxygen demand mg-O2 L-1 0-10 CH4 Methane mg-O2 L-1 On/Off HxS Total dissolved sulfides mg-O2 L-1 On/Off DO Dissolved oxygen mg-O2 L-1 On BSi

Evaluating greenhouse gas emissions from hydropower complexes on large rivers in Eastern Washington

DOE Office of Scientific and Technical Information (OSTI.GOV)

Arntzen, Evan V.; Miller, Benjamin L.; O'Toole, Amanda C.

2013-03-15

Water bodies, such as freshwater lakes, are known to be net emitters of carbon dioxide (CO2), and methane (CH4). In recent years, significant greenhouse gas (GHG) emissions from tropical, boreal, and mid-latitude reservoirs have been reported. At a time when hydropower is increasing worldwide, better understanding of seasonal and regional variation in GHG emissions is needed in order to develop a predictive understanding of such fluxes within man-made impoundments. We examined power-producing dam complexes within xeric temperate locations in the northwestern United States. Sampling environments on the Snake (Lower Monumental Dam Complex) and Columbia Rivers (Priest Rapids Dam Complex) includedmore » tributary, mainstem, embayment, forebay, and tailrace areas during winter and summer 2012. At each sampling location, GHG measurement pathways included surface gas flux, degassing as water passed through dams during power generation, ebullition within littoral embayments, and direct sampling of hyporheic pore-water. Measurements were also carried out in a free-flowing reach of the Columbia River to estimate unaltered conditions. Surface flux resulted in very low emissions, with reservoirs acting as a sink for CO2 (up to –262 mg m-2 d-1, which is within the range previously reported for similarly located reservoirs). Surface flux of methane remained below 1 mg CH4 m-2d-1, a value well below fluxes reported previously for temperate reservoirs. Water passing through hydroelectric projects acted as a sink for CO2 during winter and a small source during summer, with mean degassing fluxes of –117 and 4.5 t CO2 d-1, respectively. Degassing of CH4 was minimal, with mean fluxes of 3.1 × 10-6 and –5.6 × 10-4 t CH4 d-1 during winter and summer, respectively. Gas flux due to ebullition was greater in coves located within reservoirs than in coves within the free flowing Hanford Reach–and CH4 flux exceeded that of CO2. Methane emissions varied widely across sampling locations, ranging from 10.5 to 1039 mg CH4 m-2 d-1, with mean fluxes of 324 mg CH4 m-2 d-1in Lower Monumental Dam reservoir and 482 mg CH4 m-2d-1 in the Priest Rapids Dam reservoir. The magnitude of methane flux due to ebullition was unexpectedly high, and falls within the range recently reported for other temperate reservoirs around the world, further suggesting that this methane source should be considered in estimates of global greenhouse gas emissions. Methane flux from sediment pore-water within littoral embayments averaged 4.2 mg m-2 d-1 during winter and 8.1 mg m-2 d-1 during summer, with a peak flux of 19.8 mg m-2d-1 (at the same location where CH4 ebullition was also the greatest). Carbon dioxide flux from sediment pore-water averaged approximately 80 mg m-2d-1 with little difference between winter and summer. Similar to emissions from ebullition, flux from sediment pore-water was higher in reservoirs than in the free flowing reach.« less

Differentiating biotic from abiotic methane genesis in hydrothermally active planetary surfaces

PubMed Central

Oze, Christopher; Jones, L. Camille; Goldsmith, Jonas I.; Rosenbauer, Robert J.

2012-01-01

Molecular hydrogen (H2) is derived from the hydrothermal alteration of olivine-rich planetary crust. Abiotic and biotic processes consume H2 to produce methane (CH4); however, the extent of either process is unknown. Here, we assess the temporal dependence and limit of abiotic CH4 related to the presence and formation of mineral catalysts during olivine hydrolysis (i.e., serpentinization) at 200 °C and 0.03 gigapascal. Results indicate that the rate of CH4 production increases to a maximum value related to magnetite catalyzation. By identifying the dynamics of CH4 production, we kinetically model how the H2 to CH4 ratio may be used to assess the origin of CH4 in deep subsurface serpentinization systems on Earth and Mars. Based on our model and available field data, low H2/CH4 ratios (less than approximately 40) indicate that life is likely present and active. PMID:22679287

Differentiating biotic from abiotic methane genesis in hydrothermally active planetary surfaces.

PubMed

Oze, Christopher; Jones, L Camille; Goldsmith, Jonas I; Rosenbauer, Robert J

2012-06-19

Molecular hydrogen (H(2)) is derived from the hydrothermal alteration of olivine-rich planetary crust. Abiotic and biotic processes consume H(2) to produce methane (CH(4)); however, the extent of either process is unknown. Here, we assess the temporal dependence and limit of abiotic CH(4) related to the presence and formation of mineral catalysts during olivine hydrolysis (i.e., serpentinization) at 200 °C and 0.03 gigapascal. Results indicate that the rate of CH(4) production increases to a maximum value related to magnetite catalyzation. By identifying the dynamics of CH(4) production, we kinetically model how the H(2) to CH(4) ratio may be used to assess the origin of CH(4) in deep subsurface serpentinization systems on Earth and Mars. Based on our model and available field data, low H(2)/CH(4) ratios (less than approximately 40) indicate that life is likely present and active.

Nondestructive natural gas hydrate recovery driven by air and carbon dioxide

PubMed Central

Kang, Hyery; Koh, Dong-Yeun; Lee, Huen

2014-01-01

Current technologies for production of natural gas hydrates (NGH), which include thermal stimulation, depressurization and inhibitor injection, have raised concerns over unintended consequences. The possibility of catastrophic slope failure and marine ecosystem damage remain serious challenges to safe NGH production. As a potential approach, this paper presents air-driven NGH recovery from permeable marine sediments induced by simultaneous mechanisms for methane liberation (NGH decomposition) and CH4-air or CH4-CO2/air replacement. Air is diffused into and penetrates NGH and, on its surface, forms a boundary between the gas and solid phases. Then spontaneous melting proceeds until the chemical potentials become equal in both phases as NGH depletion continues and self-regulated CH4-air replacement occurs over an arbitrary point. We observed the existence of critical methane concentration forming the boundary between decomposition and replacement mechanisms in the NGH reservoirs. Furthermore, when CO2 was added, we observed a very strong, stable, self-regulating process of exchange (CH4 replaced by CO2/air; hereafter CH4-CO2/air) occurring in the NGH. The proposed process will work well for most global gas hydrate reservoirs, regardless of the injection conditions or geothermal gradient. PMID:25311102

Future methane emissions from animals

NASA Astrophysics Data System (ADS)

Anastasi, C.; Simpson, V. J.

1993-04-01

The future global emission of CH4 from enteric fermentation in animals has been estimated for cattle, sheep, and buffalo, which together contribute approximately 91% of the total CH4 emitted from domesticated animals at present. A simple model has been used to relate livestock levels to the national human populations for each country involved in breeding the three species included in this analysis. United Nations population predictions to 2025 were then included in the model to estimate future CH4 emissions. A variational analysis was carried out to investigate the effect of future changes in both the land available for grazing and the nutritional content of feedstocks. Results suggest that the total emission of CH4 from enteric fermentation in domestic animals will increase from 84 Tg CH4 per year (Tg = 1012 g) in 1990 to 119 (±12) Tg CH4 yr-1 by 2025. These values correspond to an average rate of increase over the next 35 years of 1.0 Tg CH4 yr-1.

Measurement of the Carbon Isotopic Composition of Methane Using Helicoidal Laser Eigenstates

NASA Astrophysics Data System (ADS)

Jacob, D.; Le Floch, A.; Bretenaker, F.; Guenot, P.

1996-06-01

The spatially generalized Jones matrix formalism is used to design a laser cavity to make intracavity measurements of the carbon isotopic composition of methane. the method is based on a double optical lever effect for helicoidally polarized eigenstates, permitting to measure successively the ^{12}CH_4 and ^{13}CH_4 concentrations. To choose the probed isotope, one simply tunes the frequency of the laser by Zeeman effect. The experiment exhibits a good agreement with the predictions and permits to measure the ^{13}CH4/^{12}CH_4 composition ratio of methane with an uncertainty of the order of ± 0.07% for a sample containing only 6× 10^{-9} mole of methane. On utilise le formalisme des matrices de Jones généralisées spatialement pour concevoir une cavité laser permettant la mesure intra-cavité de la composition isotopique du carbone présent dans le méthane. La méthode est fondée sur une double application de l'effet de levier optique pour les états propres hélicoïdaux, permettant de mesurer successivement les concentrations de ^{12}CH_4 et de ^{13}CH_4. Pour passer d'un isotope à l'autre, on ajuste simplement la fréquence du laser par effet Zeeman. L'expérience est en bon accord avec les prédictions et permet d'effectuer la mesure du rapport isotopique ^{13}CH4/^{12}CH_4 avec une fourchette d'incertitude de ± 0,07% pour des échantillons de gaz ne contenant que 6× 10^{-9} mole de méthane.

Variations in the methane budget over the last two millennia

NASA Astrophysics Data System (ADS)

Sapart, C. J.

2012-06-01

Methane (CH4) is a strong greenhouse gas and even though its atmospheric abundance is lower than carbon dioxide (CO2), CH4 has a global warming potential twenty-five times larger than CO2 and its atmospheric abundance has drastically increased since 1800. Understanding the evolution of the CH4 atmospheric abundance is complex, because it is controlled by multiple sources (e.g. wetlands, biomass burning, ruminants, rice paddies and fossil fuel) and sinks, and large uncertainties exist on how sensitive those sources and sinks are to climate variability. The aim of this research is to understand the influence of climate variability and anthropogenic activity on the CH4 budget, i.e. the balance between the different sources and sinks, during the last two millennia. For this purpose a technique was developed to analyze the CH4 isotopic composition of air in ice cores. Analysis of the isotopic composition of CH4 preserved in ice cores provides evidence for the environmental drivers of variations in CH4 mixing ratios, because different sources and sinks affect the isotopic composition of CH4 uniquely. Our main results from air trapped in Greenland ice cores shows that the carbon isotopic composition (d13C) of CH4 underwent pronounced centennial-scale variations between 200 BC and 1600 AD without clear corresponding changes in CH4 mixing ratios. Two-box model calculations suggest that those centennial-scale variations in isotope ratios are due to changes in biomass burning and biogenic sources (e.g. wetlands, agriculture), which are correlated with both natural climate variability, including the Medieval Climate Anomaly and with changes in human population, land-use and important events in history as the expansion of the Roman Empire, the fall of the Han dynasty and the Medieval period. This shows that human activity had an impact on the methane budget already two thousand years ago and is likely responsible for the atmospheric methane increase in the atmosphere during this period. Also the more recent CH4 budget has been investigated by measuring the isotope composition of CH4 in air trapped in the surface layer of the ice sheet (called firn). Several processes involving isotopic fractionation occur in the firn, hence corrections need to be apply to the isotope data in order to reconstruct the atmospheric history. Those corrections were carried out with a firn air transport model and the best-estimate scenario shows an enrichment in d13C of CH4 over the last 50 years very likely caused by enhanced fossil fuel production and consumption during this period. The role of wetlands, the main natural CH4 source, has also been investigated using measurements of d13C from air trapped in ice covering Arctic lakes in the winter. Those data showed that during the winter and in presence of ice cover, CH4, which is produced in the lake sediment, is partly removed by oxidation in the water column. Therefore, shorter is the period of ice cover on Arctic lakes, more CH4 will reach the atmosphere. This process may be of major importance in a future changing climate.

Methane concentration and isotopic composition measurements with a mid-infrared quantum-cascade laser

NASA Technical Reports Server (NTRS)

Kosterev, A. A.; Curl, R. F.; Tittel, F. K.; Gmachl, C.; Capasso, F.; Sivco, D. L.; Baillargeon, J. N.; Hutchinson, A. L.; Cho, A. Y.

1999-01-01

A quantum-cascade laser operating at a wavelength of 8.1 micrometers was used for high-sensitivity absorption spectroscopy of methane (CH4). The laser frequency was continuously scanned with current over more than 3 cm-1, and absorption spectra of the CH4 nu 4 P branch were recorded. The measured laser linewidth was 50 MHz. A CH4 concentration of 15.6 parts in 10(6) ( ppm) in 50 Torr of air was measured in a 43-cm path length with +/- 0.5-ppm accuracy when the signal was averaged over 400 scans. The minimum detectable absorption in such direct absorption measurements is estimated to be 1.1 x 10(-4). The content of 13CH4 and CH3D species in a CH4 sample was determined.

Titan's Carbon Isotopic Ratio: A Clue To Atmospheric Evolution?

NASA Astrophysics Data System (ADS)

Nixon, C. A.; Jennings, D. E.; Romani, P. N.; Jolly, A.; Teanby, N. A.; Irwin, P. G.; Bézard, B.; Vinatier, S.; Coustenis, A.; Flasar, F. M.

2009-12-01

In this presentation we describe the latest results to come from Cassini CIRS and ground-based telescopic measurements of Titan's 12C/13C ratio in atmospheric molecules, focusing on hydrocarbons. Previously, the Huygens GCMS instrument measured 12CH4/13CH4 to be 82±1 (Niemann et al., Nature, 438, 779-784, 2005), substantially and significantly lower than the VPDB inorganic Earth standard of 89.4. It is also at odds with measurements for the giant planets. Cassini CIRS infrared spectra have confirmed this enhancement in 13CH4, but also revealed that the ratio in ethane, the major photochemical product of methane photolysis, does not appear enhanced (90±7) (Nixon et al.. Icarus, 195, 778-791, 2008) and is compatible with the terrestrial and combined giant planet value (88±7, Sada et al., Ap. J., 472, p. 903-907, 1996). Recently-published results from spectroscopy using the McMath-Pierce telescope at Kitt Pitt (Jennings et al., JCP, 2009, in press) have confirmed this deviation between methane and ethane, and an explanation has been proposed. This invokes a kinetic isotope effect (KIE) in the abstraction of methane by ethynyl, a major ethane formation pathway, to preferentially partition 12C into ethane and leave an enhancement in atmospheric 13CH4 relative to the incoming flux from the reservoir. Modeling shows that a steady-state solution exists where the 12C/13C methane is decreased from the reservoir value by exactly the KIE factor (the ratio of 12CH4 to 13CH4 abstraction reaction rates): which is plausibly around 1.08, very close to the observed amount. However, a second solution exists in which we are observing Titan about ~1 methane lifetime after a major injection of methane into the atmosphere which is rapidly being eliminated. Updated measurements by Cassini CIRS of both the methane and ethane 12C/13C ratios will be presented, along with progress in interpreting this ratio. In addition, we summarize the 12C/13C measurements by CIRS in multiple other Titan hydrocarbons, and announce the first measurement of 13C-diacetylene (13C12C3H4) in Titan's atmosphere.

Laboratory Study of Methane Flux from Acid Sulphate Soil in South Kalimantan

NASA Astrophysics Data System (ADS)

Annisa, W.; Cahyana, D.; Syahbuddin, H.; Rachman, A.

2017-06-01

Addition of organic matter in waterlogged conditions will enhance methanogenesis process that produces greenhouse gases. Fresh organic material is considered reactive because it contains carbons that is subject to decompose, therefore, when it exposed to acid sulphate soil, both in natural condition (aeration required) and intensive (aeration not required) will lower the value of redox potential. This experiment aimed to determine the flux of methane (CH4) from various locally available organic materials applied to acid sulphate soil. The experiment was arranged in factorial design with two factors. The first factor was the source of organic matter, i.e. fresh rice straw, fresh purun, fresh cattle manure, composted rice straw, composted purun and composted cattle manure, and control. The second factor was the management of organic matter i.e. placed on the soil surface with no tillage and mixed with soil during tillage. The results showed that application of fresh organic matter into inundated acid sulphate soil increased CH4 fluxes up to 23.78 µg CH4 g1 d1 which was higher than from composted organic matter (4.327 µg CH4.g1.d1). Methane flux due to organic matter management was significantly negatively (p=0.001) correlated with soil redox potential (Eh) with R2 of - 0.76. Organic matter placed on the soil surface with no tillage produced methane flux ranged from 0.33 to 20.78 g CH4 g1 d1, which was lower than methane flux produced from organic matter mixed with soil during tillage (0.38 to 27.27 g CH4 g1 d1). Composting organic matter before application and mixing them with the soil through tillage are highly recommended to reduce greenhouse gas emissions from cultivated acid sulphate soils.

Global wetland contribution to 2000–2012 atmospheric methane growth rate dynamics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Poulter, Benjamin; Bousquet, Philippe; Canadell, Josep G.

Increasing atmospheric methane (CH 4) concentrations have contributed to approximately 20% of anthropogenic climate change. Despite the importance of CH 4 as a greenhouse gas, its atmospheric growth rate and dynamics over the past two decades, which include a stabilization period (1999–2006), followed by renewed growth starting in 2007, remain poorly understood. We provide an updated estimate of CH 4 emissions from wetlands, the largest natural global CH 4 source, for 2000–2012 using an ensemble of biogeochemical models constrained with remote sensing surface inundation and inventory-based wetland area data. Between 2000–2012, boreal wetland CH 4 emissions increased by 1.2 Tgmore » yr –1 (–0.2–3.5 Tg yr –1), tropical emissions decreased by 0.9 Tg yr –1 (–3.2–1.1 Tg yr –1), yet globally, emissions remained unchanged at 184 ± 22 Tg yr –1. Changing air temperature was responsible for increasing high-latitude emissions whereas declines in low-latitude wetland area decreased tropical emissions; both dynamics are consistent with features of predicted centennial-scale climate change impacts on wetland CH 4 emissions. Despite uncertainties in wetland area mapping, our study shows that global wetland CH 4 emissions have not contributed significantly to the period of renewed atmospheric CH 4 growth, and is consistent with findings from studies that indicate some combination of increasing fossil fuel and agriculture-related CH 4 emissions, and a decrease in the atmospheric oxidative sink.« less

Global wetland contribution to 2000–2012 atmospheric methane growth rate dynamics

DOE PAGES

Poulter, Benjamin; Bousquet, Philippe; Canadell, Josep G.; ...

2017-09-13

Increasing atmospheric methane (CH 4) concentrations have contributed to approximately 20% of anthropogenic climate change. Despite the importance of CH 4 as a greenhouse gas, its atmospheric growth rate and dynamics over the past two decades, which include a stabilization period (1999–2006), followed by renewed growth starting in 2007, remain poorly understood. We provide an updated estimate of CH 4 emissions from wetlands, the largest natural global CH 4 source, for 2000–2012 using an ensemble of biogeochemical models constrained with remote sensing surface inundation and inventory-based wetland area data. Between 2000–2012, boreal wetland CH 4 emissions increased by 1.2 Tgmore » yr –1 (–0.2–3.5 Tg yr –1), tropical emissions decreased by 0.9 Tg yr –1 (–3.2–1.1 Tg yr –1), yet globally, emissions remained unchanged at 184 ± 22 Tg yr –1. Changing air temperature was responsible for increasing high-latitude emissions whereas declines in low-latitude wetland area decreased tropical emissions; both dynamics are consistent with features of predicted centennial-scale climate change impacts on wetland CH 4 emissions. Despite uncertainties in wetland area mapping, our study shows that global wetland CH 4 emissions have not contributed significantly to the period of renewed atmospheric CH 4 growth, and is consistent with findings from studies that indicate some combination of increasing fossil fuel and agriculture-related CH 4 emissions, and a decrease in the atmospheric oxidative sink.« less

Centennial to millennial variations of atmospheric methane during the early Holocene

NASA Astrophysics Data System (ADS)

Yang, Ji-Woong; Ahn, Jinho; Brook, Edward

2015-04-01

Atmospheric CH4 is one of the most important greenhouse gases. Ice core studies revealed strong correlations between millennial CH4 variations and Greenland climate during the last glacial period. However, millennial to sub-millennial CH4 variations during interglacial periods are not well studied. Recently, several high-resolution data sets have been produced for the late Holocene, but it is difficult to distinguish natural- from anthropogenic changes. In contrast, the methane budget of the early Holocene is not affected by anthropogenic disturbances, thus may help us better understand natural CH4 control mechanisms under interglacial climate boundary conditions. Here we present our new high-precision and high-resolution atmospheric CH4 record from Siple Dome ice core, Antarctica that covers the early Holocene. We used our new wet extraction system at Seoul National University that shows a good precision of ~1 ppb. Our data show several tens of ppb of centennial- to millennial CH4 variations and an anti-correlative evolution with Greenland climate on the millennial time scale. The CH4 record could have been affected by many different types of forcing, including temperature, precipitation (monsoon intensity), biomass burning, sea surface temperature, and solar activity. According to our data, early Holocene CH4 is well correlated with records of hematite stained grains (HSG) in North Atlantic sediment records, within age uncertainties. A red-noise spectral analysis yields peaks at frequencies of ~1270 and ~80 years, which are similar to solar frequencies, but further investigations are needed to determine major controlling factor of atmospheric CH4during the early Holocene.

High diversity of methanotrophic bacteria in geothermal soils affected by high methane fluxes

NASA Astrophysics Data System (ADS)

D'Alessandro, Walter; Gagliano, Antonina Lisa; Quatrini, Paola; Parello, Francesco

2014-05-01

Volcanic and geothermal systems emit endogenous gases by widespread degassing from soils, including CH4, a greenhouse gas 25 times as potent as CO2. Recently, it has been demonstrated that volcanic/geothermal soils act as source, but also as biological filter for methane release to the atmosphere. For long time, volcanic/geothermal soils has been considered inhospitable for methanotrophic microorganisms, but new extremophile methanotrophs belonging to Verrucomicrobia were identified in three different areas (Pozzuoli, Italy; Hell's Gate, New Zealand; Kamchatka, Russia), explaining anomalous behaviours in methane leakages of several geothermal/volcanic sites. Our aim was to increase the knowledge of the relationship between methane emissions from volcanic/geothermal areas and biological methane oxidation, by investigating a geothermal site of Pantelleria island (Italy). Pantelleria Island hosts a high enthalpy geothermal system characterized by high temperature, high CH4 and very low H2S fluxes. Such characteristics are reflected in potentially great supply of methane for methanotrophs and scarce presence of inhibitors of their activity (H2S and NH3) in the Pantelleria soils. Potential methanotrophic activity within these soils was already evidenced by the CH4/CO2 ratio of the flux measurements which was lower than that of the respective fumarolic manifestations indicating a loss of CH4 during the gas travel towards the earth's surface. In this study laboratory incubation experiments using soils sampled at Favara Grande, the main hydrothermal area of Pantelleria, showed very high methane consumption rates (up to 9500 ng CH4 h-1 g-1). Furthermore, microbiological and culture-independent molecular analyses allowed to detect the presence of methanotrophs affiliated to Gamma- and Alpha-Proteobacteria and to the newly discovered acidothermophilic methanotrophs Verrucomicrobia. Culturable methanotrophic Alpha-proteobacteria of the genus Methylocystis were isolated by enrichment cultures. The isolates showed a wide range of tolerance to pH (3.5 - 8) and temperatures (18 - 45°C), and an average methane oxidation rate of 450 ppm/h. A larger diversity of proteobacterial and verrucomicrobial methanotrophs was detected by the amplification of the methane mono-oxygenase gene pmoA. This study demonstrates the coexistence of both the methanotrophic phyla Verrucomicrobia and Proteobacteria in the same geothermal site. The presence of proteobacterial methanotrophs was quite unexpected because they are generally considered not adapted to live in such harsh environments. Their presence at Favara Grande could be explained by not so low soil pH values (> 5) of this specific geothermal site and by the high methane availability. Such species could have found their niches in the shallowest part of the soils, were the temperatures are not so high, thriving on the abundant upraising methane. Understanding the ecology of methanotrophy in geothermal sites will increase our knowledge of their role in methane emissions to the atmosphere.

Estimating Amazonian methane emissions through 4D-Var inverse modelling with satellite observations from GOSAT and IASI

NASA Astrophysics Data System (ADS)

Wilson, C. J.; Chipperfield, M.; Gloor, M.; McNorton, J.; Miller, J. B.; Gatti, L. V.; Siddans, R.; Bloom, A. A.; Basso, L. S.; Boesch, H.; Parker, R.; Monks, S. A.

2015-12-01

Methane (CH4) is emitted from a range of anthropogenic and natural sources, and since the industrial revolution its mean atmospheric concentration has climbed dramatically. CH4 produces a relatively high radiative forcing effect upon the Earth's climate, and its atmospheric lifetime of approximately 10 years makes it an appealing target for the mitigation of climate change. However, the spatial and temporal variation of CH4 emissions are not well understood, though in recent years a number of top-down and bottom-up studies have attempted to construct improved emission budgets. However, some top-down studies suffer from poor observational coverage near the Amazon basin, particularly in the planetary boundary layer. Since emissions from this region, coming mainly from wetland and burning sources, are thought to be relatively high, additional observations in this region would greatly help to constrain the geographical distribution of the global CH4 emission budget. To this end, regular flask measurements of CH4 and other trace gases have been taken during flights over four Amazonian sites since 2010, as part of the AMAZONICA project. The GOSAT has been used to retrieve global column-average CH4 concentrations since mid-2009, whilst IASI, on-board Metop-A, has also been measuring atmospheric CH4 concentrations since its launch in 2006. We present an assessment of Amazonian methane emissions for 2010 and 2011 using the TOMCAT Chemical Transport Model and the new variational inverse model, INVICAT. These models are used to attribute methane variations at each Amazon site to a source type and region, to assess the ability of our current CH4 flux estimates to reproduce these observations and to produce improved posterior emission estimates through assimilation of atmospheric observations. This study represents the first use of the INVICAT scheme to constrain emissions of any atmospheric trace gas. Whilst there is generally good agreement between the model and the observations prior to data assimilation, some high-methane events indicated by the observations are not captured by the model. We assimilate observations from the NOAA surface measurement network, from the AMAZONICA aircraft and from the GOSAT and IASI satellites, and find that tropical South American CH4 emissions approach 50 Tg(CH4)/yr.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heath, Garvin; Warner, Ethan; Steinberg, Daniel

A growing number of studies have raised questions regarding uncertainties in our understanding of methane (CH 4) emissions from fugitives and venting along the natural gas (NG) supply chain. In particular, a number of measurement studies have suggested that actual levels of CH 4 emissions may be higher than estimated by EPA" tm s U.S. GHG Emission Inventory. We reviewed the literature to identify the growing number of studies that have raised questions regarding uncertainties in our understanding of methane (CH 4) emissions from fugitives and venting along the natural gas (NG) supply chain.

Evidence for methane production by the marine algae Emiliania huxleyi

NASA Astrophysics Data System (ADS)

Lenhart, Katharina; Klintzsch, Thomas; Langer, Gerald; Nehrke, Gernot; Bunge, Michael; Schnell, Sylvia; Keppler, Frank

2016-06-01

Methane (CH4), an important greenhouse gas that affects radiation balance and consequently the earth's climate, still has uncertainties in its sinks and sources. The world's oceans are considered to be a source of CH4 to the atmosphere, although the biogeochemical processes involved in its formation are not fully understood. Several recent studies provided strong evidence of CH4 production in oxic marine and freshwaters, but its source is still a topic of debate. Studies of CH4 dynamics in surface waters of oceans and large lakes have concluded that pelagic CH4 supersaturation cannot be sustained either by lateral inputs from littoral or benthic inputs alone. However, regional and temporal oversaturation of surface waters occurs frequently. This comprises the observation of a CH4 oversaturating state within the surface mixed layer, sometimes also termed the "oceanic methane paradox". In this study we considered marine algae as a possible direct source of CH4. Therefore, the coccolithophore Emiliania huxleyi was grown under controlled laboratory conditions and supplemented with two 13C-labeled carbon substrates, namely bicarbonate and a position-specific 13C-labeled methionine (R-S-13CH3). The CH4 production was 0.7 µg particular organic carbon (POC) g-1 d-1, or 30 ng g-1 POC h-1. After supplementation of the cultures with the 13C-labeled substrate, the isotope label was observed in headspace CH4. Moreover, the absence of methanogenic archaea within the algal culture and the oxic conditions during CH4 formation suggest that the widespread marine algae Emiliania huxleyi might contribute to the observed spatially and temporally restricted CH4 oversaturation in ocean surface waters.

Constraints on oceanic methane emissions west of Svalbard from atmospheric in situ measurements and Lagrangian transport modeling

NASA Astrophysics Data System (ADS)

Pisso, Ignacio; Myhre, Cathrine Lund; Platt, Stephen Matthew; Eckhardt, Sabine; Hermansen, Ove; Schmidbauer, Norbert; Mienert, Jurgen; Vadakkepuliyambatta, Sunil; Bauguitte, Stephane; Pitt, Joseph; Allen, Grant; Bower, Keith; O'Shea, Sebastian; Gallagher, Martin; Percival, Carl; Pyle, John; Cain, Michelle; Stohl, Andreas

2017-04-01

Methane stored in seabed reservoirs such as methane hydrates can reach the atmosphere in the form of bubbles or dissolved in water. Hydrates could destabilize with rising temperature further increasing greenhouse gas emissions in a warming climate. To assess the impact of oceanic emissions from the area west of Svalbard, where methane hydrates are abundant, we used measurements collected with a research aircraft (FAAM) and a ship (Helmer Hansen) during the Summer 2014, and for Zeppelin Observatory for the full year. We present a model-supported analysis of the atmospheric CH4 mixing ratios measured by the different platforms. To address uncertainty about where CH4 emissions actually occur, we explored three scenarios: areas with known seeps, a hydrate stability model and an ocean depth criterion. We then used a budget analysis and a Lagrangian particle dispersion model to compare measurements taken upwind and downwind of the potential CH4 emission areas. We found small differences between the CH4 mixing ratios measured upwind and downwind of the potential emission areas during the campaign. By taking into account measurement and sampling uncertainties and by determining the sensitivity of the measured mixing ratios to potential oceanic emissions, we provide upper limits for the CH4 fluxes. The CH4 flux during the campaign was small, with an upper limit of 2.5 nmol / m s in the stability model scenario. The Zeppelin Observatory data for 2014 suggests CH4 fluxes from the Svalbard continental platform below 0.2 Tg/yr . All estimates are in the lower range of values previously reported.

Modeling the Interaction of H2 on Root Exudate Degradation and Methanogenesis in Wetland Sediments

NASA Astrophysics Data System (ADS)

Pal, D. S.; Jaffe, P. R.

2014-12-01

CH4 is produced in wetland sediments from the microbial degradation of organic carbon through multiple fermentation steps and methanogenesis pathways. There are many potential sources of carbon for methananogenesis; in vegetated wetland sediments, microbial communities consume root exudates as a major source of organic carbon. In many methane models propionate is used as a model carbon molecule. This simple sugar is fermented into acetate and H2, acetate is transformed to methane and CO2 while the H2 and CO2 is synthesized to form an additional CH4 molecule. The hydrogenotrophic pathway involves the equilibrium of two dissolved gases, CH4 and H2. In an effort to limit CH4 emissions from wetlands, there has been growing interest in finding ways to limit plant transport of soil gases through root systems. While this may decrease the direct emissions of methane, there is little understanding about how H2 dynamics may feedback into overall methane production. Since H2 is used in methane production and produced in propionate fermentation, increased subsurface H2 concentrations can simultaneously inhibit propionate fermentation and acetate production and enhance hydrogenotrophic methanogenesis. For this study, we incubated soil samples from vegetated wetland sediments with propionate or acetate and four different hydrogen concentrations. The headspaces from these incubations were simultaneously analyzed for H2 and CH4 at multiple time points over two months. The comparison of methane production between different hydrogen concentrations and different carbon sources can indicate which process is most affected by increased hydrogen concentrations. The results from this study were combined with a newly formulated steady-state model of propionate degradation and formation of methane, that also accounts for the venting off both gases via plants. The resulting model indicates how methane production and emissions would be affected by plant volatilization.

Compositional and functional stability of aerobic methane consuming communities in drained and rewetted peat meadows.

PubMed

Krause, Sascha; Niklaus, Pascal A; Badwan Morcillo, Sara; Meima Franke, Marion; Lüke, Claudia; Reim, Andreas; Bodelier, Paul L E

2015-11-01

The restoration of peatlands is an important strategy to counteract subsidence and loss of biodiversity. However, responses of important microbial soil processes are poorly understood. We assessed functioning, diversity and spatial organization of methanotrophic communities in drained and rewetted peat meadows with different water table management and agricultural practice. Results show that the methanotrophic diversity was similar between drained and rewetted sites with a remarkable dominance of the genus Methylocystis. Enzyme kinetics depicted no major differences, indicating flexibility in the methane (CH4) concentrations that can be used by the methanotrophic community. Short-term flooding led to temporary elevated CH4 emission but to neither major changes in abundances of methane-oxidizing bacteria (MOB) nor major changes in CH4 consumption kinetics in drained agriculturally used peat meadows. Radiolabeling and autoradiographic imaging of intact soil cores revealed a markedly different spatial arrangement of the CH4 consuming zone in cores exposed to near-atmospheric and elevated CH4. The observed spatial patterns of CH4 consumption in drained peat meadows with and without short-term flooding highlighted the spatial complexity and responsiveness of the CH4 consuming zone upon environmental change. The methanotrophic microbial community is not generally altered and harbors MOB that can cover a large range of CH4 concentrations offered due to water-table fluctuations, effectively mitigating CH4 emissions. © FEMS 2015. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.

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

NASA Astrophysics Data System (ADS)

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 regions. To optimize "inverse approach", we need to investigate the relation between xCH4 and the surface concentration, and need to combine it to the bottom-up approach. We will also discuss representativeness of GOSAT measurement from the viewpoint of spatial and time scale when it observes such heterogeneous emission regions.

Air emissions of ammonia and methane from livestock operations: valuation and policy options.

PubMed

Shih, Jhih-Shyang; Burtraw, Dallas; Palmer, Karen; Siikamäki, Juha

2008-09-01

The animal husbandry industry is a major emitter of ammonia (NH3), which is a precursor of fine particulate matter (PM2.5)--arguably, the number-one environment-related public health threat facing the nation. The industry is also a major emitter of methane (CH4), which is an important greenhouse gas (GHG). We present an integrated process model of the engineering economics of technologies to reduce NH3 and CH4 emissions at dairy operations in California. Three policy options are explored: PM offset credits for NH3 control, GHG offset credits for CH4 control, and expanded net metering policies to provide revenue for the sale of electricity generated from captured methane (CH4) gas. Individually these policies vary substantially in the economic incentives they provide for farm operators to reduce emissions. We report on initial steps to fully develop the integrated process model that will provide guidance for policy-makers.

Hydrogen Migration and Vinylidene Pathway for Formation of Methane in the 193 nm Photodissociation of Propene: CH3CH=CH2 and CD3CD=CD2

NASA Technical Reports Server (NTRS)

Zhao, Yi-Lei; Laufer, Allan H.; Halpern, Joshua B.; Fahr, Askar

2007-01-01

Photodissociation channels and the final product yields from the 193 nm photolysis of propene-h6 (CH2=CHCH3) and propene-d6 (CD2=CDCD3) have been investigated, employing gas chromatography, mass spectroscopy, and flame ionization (GC/MS/FID) detection methods. The yields of methane as well as butadiene relative to ethane show considerable variations when propene-h6 or propene-d6 are photolyzed. This suggests significant variances in the relative importance of primary photolytic processes and/or secondary radical reactions, occurring subsequent to the photolysis. Theoretical calculations suggest the potential occurrence of an intramolecular dissociation through a mechanism involving vinylidene formation, accompanied by an ethylenic H-migration through the pi-orbitals. This process affects the final yields of methane-h4 versus methane-d4 with respect to other products. The product yields from previous studies of the 193 nm photolysis of methyl vinyl ketone-h6 and -d6 (CH2=CHCOCH3, CD2=CDCOCD3), alternative precursors for generating methyl and vinyl radicals, are compared with the current results for propene.

The Effect of the Interannual Variability of the OH Sink on the Interannual Variability of the Atmospheric Methane Mixing Ratio and Carbon Stable Isotope Composition

NASA Astrophysics Data System (ADS)

Guillermo Nuñez Ramirez, Tonatiuh; Houweling, Sander; Marshall, Julia; Williams, Jason; Brailsford, Gordon; Schneising, Oliver; Heimann, Martin

2013-04-01

The atmospheric hydroxyl radical concentration (OH) varies due to changes in the incoming UV radiation, in the abundance of atmospheric species involved in the production, recycling and destruction of OH molecules and due to climate variability. Variability in carbon monoxide emissions from biomass burning induced by El Niño Southern Oscillation are particularly important. Although the OH sink accounts for the oxidation of approximately 90% of atmospheric CH4, the effect of the variability in the distribution and strength of the OH sink on the interannual variability of atmospheric methane (CH4) mixing ratio and stable carbon isotope composition (δ13C-CH4) has often been ignored. To show this effect we simulated the atmospheric signals of CH4 in a three-dimensional atmospheric transport model (TM3). ERA Interim reanalysis data provided the atmospheric transport and temperature variability from 1990 to 2010. We performed simulations using time dependent OH concentration estimations from an atmospheric chemistry transport model and an atmospheric chemistry climate model. The models assumed a different set of reactions and algorithms which caused a very different strength and distribution of the OH concentration. Methane emissions were based on published bottom-up estimates including inventories, upscaled estimations and modeled fluxes. The simulations also included modeled concentrations of atomic chlorine (Cl) and excited oxygen atoms (O(1D)). The isotopic signal of the sources and the fractionation factors of the sinks were based on literature values, however the isotopic signal from wetlands and enteric fermentation processes followed a linear relationship with a map of C4 plant fraction. The same set of CH4emissions and stratospheric reactants was used in all simulations. Two simulations were done per OH field: one in which the CH4 sources were allowed to vary interannually, and a second where the sources were climatological. The simulated mixing ratios and isotopic compositions at global reference stations were used to construct more robust indicators such as global and zonal means and interhemispheric differences. We also compared the model CH4 mixing ratio to satellite observations, for the period 2003 to 2004 with SCIAMACHY and from 2009 to 2010 with GOSAT. The interannual variability of the different OH fields imprinted an interannual variation of the atmospheric CH4 mixing ratio with a magnitude of ±10 ppb, which is comparable to the effect of all sources combined. Meanwhile its effect on the interannual variability of δ13C-CH4 was minor (< 10%). The interannual variability of the mixing ratio interhemispheric difference is dominated by the sources because the OH sink is concentrated in the tropics, thus its interannual variability affects both hemispheres. Meanwhile, although the OH plays an important role in the establishment of an interhemispheric gradient of δ13C-CH4, the interannual variation of this gradient is negligibly affected by the choice of OH field. Overall the study showed that the variability of the OH sink plays a significant role in the interannual variability of the atmospheric methane mixing ratio, and must be considered to improve our understanding of the recent trends in the global methane budget.

Methane oxidation and attenuation of sulphur compounds in landfill top cover systems: Lab-scale tests.

PubMed

Raga, Roberto; Pivato, Alberto; Lavagnolo, Maria Cristina; Megido, Laura; Cossu, Raffaello

2018-03-01

In this study, a top cover system is investigated as a control for emissions during the aftercare of new landfills and for old landfills where biogas energy production might not be profitable. Different materials were studied as landfill cover system in lab-scale columns: mechanical-biological pretreated municipal solid waste (MBP); mechanical-biological pretreated biowaste (PB); fine (PBS f ) and coarse (PBS c ) mechanical-biological pretreated mixtures of biowaste and sewage sludge, and natural soil (NS). The effectiveness of these materials in removing methane and sulphur compounds from a gas stream was tested, even coupled with activated carbon membranes. Concentrations of CO 2 , CH 4 , O 2 , N 2 , H 2 S and mercaptans were analysed at different depths along the columns. Methane degradation was assessed using mass balance and the results were expressed in terms of methane oxidation rate (MOR). The highest maximum and mean MOR were observed for MBP (17.2gCH 4 /m 2 /hr and 10.3gCH 4 /m 2 /hr, respectively). Similar values were obtained with PB and PBS c . The lowest values of MOR were obtained for NS (6.7gCH 4 /m 2 /hr) and PBS f (3.6gCH 4 /m 2 /hr), which may be due to their low organic content and void index, respectively. Activated membranes with high load capacity did not seem to have an influence on the methane oxidation process: MBP coupled with 220g/m 2 and 360g/m 2 membranes gave maximum MOR of 16.5gCH 4 /m 2 /hr and 17.4gCH 4 /m 2 /hr, respectively. Activated carbon membranes proved to be very effective on H 2 S adsorption. Furthermore, carbonyl sulphide, ethyl mercaptan and isopropyl mercaptan seemed to be easily absorbed by the filling materials. Copyright © 2017. Published by Elsevier B.V.

Effect of feeding legumes containing condensed tannins with orchardgrass on ruminal fermentation and methane production in continuous culture

USDA-ARS?s Scientific Manuscript database

Developing feeding strategies that allow farmers to reduce methane (CH4) emissions from livestock is gaining interest worldwide. Legumes containing condensed tannins (CT) have been shown to decrease enteric CH4 in ruminants; however, research is lacking on how increased CT levels affect ruminal ferm...

ANALYSIS OF FACTORS AFFECTING METHANE GAS RECOVERY FROM SIX LANDFILLS

EPA Science Inventory

The report gives results of a pilot study of six U.S. landfills that have methane (CH4) gas recovery systems. NOTE: The study was a first step in developing a field testing program to gather data to identify key variables that affect CH4 generation and to develop an empirical mod...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 13: CHEMICAL INJECTION PUMPS

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 15: GAS-ASSISTED GLYCOL PUMPS

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 6: VENTED & COMBUSTION SOURCE SUMMARY

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 11: COMPRESSOR DRIVER EXHAUST

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 7: BLOW AND PURGE ACTIVITIES

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

Studies of methane fluxes reveal that desert soils can mitigate global climate change

Treesearch

Jean E. T. McLain; Dean A. Martens

2005-01-01

Moisture limitations have led researchers to believe that semiarid soils are not significant consumers or producers of trace gases, and these regions are often overlooked in greenhouse gas inventories. We are studying environmental influences on soil fluxes of methane (CH4) in southeastern Arizona. We found negligible CH4...

Methane uptake in urban forests and lawns

Treesearch

Peter M. Groffman; Richard V. Pouyat

2009-01-01

The largest natural biological sink for the radiatively active trace gas methane (CH4) is bacteria in soils that consume CH4 as an energy and carbon source. This sink has been shown to be sensitive to nitrogen (N) inputs and alterations of soil physical conditions. Given this sensitivity, conversion of native ecosystems to...

Eddy covariance measurements of methane fluxes over grazed native and improved prairies in Oklahoma

USDA-ARS?s Scientific Manuscript database

Although several studies have reported eddy covariance (EC) measurements at several tallgrass prairie sites to investigate the dynamics of carbon and water vapor fluxes, the EC measurements of methane (CH4) fluxes over grazed tallgrass prairie sites are lacking. CH4 fluxes were measured during the 2...

ESTIMATE OF GLOBAL METHANE EMISSIONS FROM LANDFILLS AND OPEN DUMPS

EPA Science Inventory

The report presents an empirical model to estimate global methane (CH4) emissions from landfills and open dumps based on EPA data from landfill gas (LFG) recovery projects. The EPA CH4 estimates for 1990 range between 19 and 40 teragrams (10 to the 12th power) per year (Tg/yr), w...

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

NASA Astrophysics Data System (ADS)

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

2018-02-01

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

Statistical assessment of dumpsite soil suitability to enhance methane bio-oxidation under interactive influence of substrates and temperature.

PubMed

Bajar, Somvir; Singh, Anita; Kaushik, C P; Kaushik, Anubha

2017-05-01

Biocovers are considered as the most effective and efficient way to treat methane (CH 4 ) emission from dumpsites and landfills. Active methanotrophs in the biocovers play a crucial role in reduction of emissions through microbiological methane oxidation. Several factors affecting methane bio-oxidation (MOX) have been well documented, however, their interactive effect on the oxidation process needs to be explored. Therefore, the present study was undertaken to investigate the suitability of a dumpsite soil to be employed as biocover, under the influence of substrate concentrations (CH 4 and O 2 ) and temperature at variable incubation periods. Statistical design matrix of Response Surface Methodology (RSM) revealed that MOX rate up to 69.58μgCH 4 g -1 dw h -1 could be achieved under optimum conditions. MOX was found to be more dependent on CH 4 concentration at higher level (30-40%, v/v), in comparison to O 2 concentration. However, unlike other studies MOX was found in direct proportionality relationship with temperature within a range of 25-35°C. The results obtained with the dumpsite soil biocover open up a new possibility to provide improved, sustained and environmental friendly systems to control even high CH 4 emissions from the waste sector. Copyright © 2017 Elsevier Ltd. All rights reserved.

Microwave Spectrum and Structure of the Methane-Propane Complex

NASA Astrophysics Data System (ADS)

Peterson, Karen I.; Lin, Wei; Arsenault, Eric A.; Choi, Yoon Jeong; Novick, Stewart E.

2017-06-01

Methane is exceptional in its solid-phase orientational disorder that persists down to 24 K. Only below that temperature does the structure become partially ordered, and full crystallinity requires even lower temperatures and high pressures. Not surprisingly, methane appears to freely rotate in most van der Waals complexes, although two notable exceptions are CH_4-HF and CH_4-C_5H_5N. Of interest to us is how alkane interactions affect the methane rotation. Except for CH_4-CH_4, rotationally-resolved spectra of alkane-alkane complexes have not been studied. To fill this void, we present the microwave spectrum of CH_4-C_3H_8 which is the smallest alkane complex with a practical dipole moment. The microwave spectrum of CH_4-C_3H_8 was measured using the Fourier Transform microwave spectrometer at Wesleyan University. In the region between 7100 and 25300 MHz, we observed approximately 70 transitions that could plausibly be attributed to the CH_4-C_3H_8 complex (requiring high power and the proper mixture of gases). Of these, 16 were assigned to the A-state (lowest internal rotor state of methane) and four to the F-state. The A-state transitions were fitted with a Watson Hamiltonian using nine spectroscopic constants of which A = 7553.8144(97) MHz, B = 2483.9183(35) MHz, and C = 2041.8630(21) MHz. The A rotational constant is only 1.5 MHz higher than that of Ar-C_3H_8 and, since the a-axis of the complex passes approximately through the centers of mass of the subunits, this indicates a similar relative orientation. Thus, we find that the CH_4 is located above the plane of the propane. The center-of-mass separation of the subunits in CH_4-C_3H_8 is calculated to be 3.993 Å, 0.16 Å longer than the Ar-C_3H_8 distance of 3.825 Å, a reasonable difference considering the larger van der Waals radius of CH_4. The four F-state lines, which were about twice as strong as the A-state lines, could be fitted to A, B, and C rotational constants, and further analysis is in progress.

Patterns of in-soil methane production and atmospheric emission among different land covers of a Lake Erie estuarine wetland

NASA Astrophysics Data System (ADS)

Rey Sanchez, C.; Morin, T. H.; Stefanik, K. C.; Angle, J.; Wrighton, K. C.; Bohrer, G.

2017-12-01

Wetland soils store a great amount of carbon, but also accumulate and emit methane (CH4), a powerful greenhouse gas. To better understand the vertical and horizontal spatial variability of CH4 emissions, we monitored production and fluxes of CH4 in Old Woman Creek, an estuarine wetland of Lake Erie, Ohio, during the growing seasons of 2015 and 2016. Our combined observation methods targeted three different scales: 1) the eddy covariance technique provided continuous high frequency observations integrated over a large spatial footprint; 2) monthly chamber measurements provided sparse point measurements of fluxes in four distinct land-cover types in the wetland: open water, emergent vegetation (Typha spp.), floating vegetation (Nelumbo spp.) and mud flats; and 3) in-situ porewater dialysis samplers, "peepers", provided vertical CH4 concentration data in the soil at the same locations and temporal time steps as the chambers. In addition, we studied gene transcripts to quantify methanogenesis activity along the vertical soil profile. Using integrated chamber and EC measurements, we found an average surface emission rate from Typha, the most abundant vegetated land cover, of 219.4 g CH4-C m-2 y-1, which was much higher than rates reported in similar emergent vegetation types in other wetlands. There was large spatial variation of flux rates, with mud flats having the highest rates of CH4 emission, followed by Nelumbo and Typha patches, and with open water having the lowest emissions. Within the soil column, we applied a numerical model to convert soil methane concentrations to emissions rates. We found that, contrary to current ideas of methane production, most methane was being produced in the well-oxygenated surface soils, probably in anoxic microsites within the oxic layer. Our metatranscriptomic data supported these findings, clearly showing nine times greater methanogenic activity in oxic surface soils relative to deeper anoxic soils. Combined, our results provide important insights for the representation of processes of methane production and consumption in models, which can largely affect the estimates of methane emission from wetlands.

Methane oxidation associated to submerged brown-mosses buffers methane emissions from Siberian polygonal peatlands

NASA Astrophysics Data System (ADS)

Liebner, Susanne; Zeyer, Josef; Knoblauch, Christian

2010-05-01

Circumpolar peatlands store roughly 18 % of the globally stored carbon in soils [based on 1, 2]. Also, northern wetlands and tundra are a net source of methane (CH4), an effective greenhouse gas (GHG), with an estimated annual CH4 release of 7.2% [3] or 8.1% [4] of the global total CH4 emission. Although it is definite that Arctic tundra significantly contributes to the global methane emissions in general, regional variations in GHG fluxes are enormous. CH4 fluxes of polygonal tundra within the Siberian Lena Delta, for example, were reported to be low [5, 6], particularly at open water polygonal ponds and small lakes [7] which make up around 10 % of the delta's surface. Low methane emissions from polygonal ponds oppose that Arctic permafrost thaw ponds are generally known to emit large amounts of CH4 [8]. Combining tools of biogeochemistry and molecular microbiology, we identified sinks of CH4 in polygonal ponds from the Lena Delta that were not considered so far in GHG studies from Arctic wetlands. Pore water CH4 profiling in polygonal ponds on Samoylov, a small island in the central part of the Lena Delta, revealed a pronounced zone of CH4 oxidation near the vegetation surface in submerged layers of brown-mosses. Here, potential CH4 oxidation was an order of magnitude higher than in non-submerged mosses and in adjacent bulk soil. We could additionally show that this moss associated methane oxidation (MAMO) is hampered when exposure of light is prevented. Shading of plots with submerged Scorpidium scorpioides inhibited MAMO leading to higher CH4 concentrations and an increase in CH4 fluxes by a factor of ~13. Compared to non-submerged mosses, the submerged mosses also showed significantly lower δ13C values indicating that they use carbon dioxide derived from methane oxidation for photosynthesis. Applying stable isotope probing of DNA, type II methanotrophs were identified to be responsible for the oxidation of CH4 in the submerged Scorpidium scorpioides. Our study gives first evidence for MAMO in submerged brown-mosses and in the oligotrophic polygonal peatlands of the Lena Delta. It shows that MAMO might effectively reduce methane fluxes to the atmosphere also in Arctic GHG emission hot spots. References: [1] Zhang, T., Barry, R.G., Knowles, K., Heginbottom, J.A., and Brown, J. (1999) Statistics and characteristics of permafrost and ground-ice distribution in the Northern Hemisphere. Polar Geography 23(2): 132-154 [2] Schuur, E.A.G., Bockheim, J., Candell, J.G., Euskirchen, E., Field, C.B., Goryachkin, S.V., Hagemann, S., Kuhry, P., Lafleur, P.M., Lee, H., Mazhitova, G., Nelson, F.E., Rinke, A., Romanovsky, V., Shiklomanov, N., Tarnocai, C., Venevsky, S., Vogel, J., and Zimov, S. (2008) Vulnerability of Permafrost Carbon to Climate Change: Implications for the Global Carbon Cycle. BioScience 58 (8): 701-714 [3] Denman, K.L., Brasseur G., Chidthaisong A., Ciais, P., Cox, P.M., Dickinson, R.E., Hauglustaine, D., Heinze, C., Holland, E., Jacob, D., Lohmann, U., Ramachandran, S., da Silva Dias, P.L., Wofsy, S.C., and Zhang, X. (2007) Couplings Between Changes in the Climate System and Biogeochemistry. In: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change [Solomon, S., D. Qin, M. Manning, Z. Chen, M. Marquis, K.B. Averyt, M.Tignor and H.L. Miller (eds.)]. Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA [4] Wuebbles, J., and Hayhoe, K. (2002) Atmospheric methane and global change. Earth-Science Reviews 57: 177-210 [5] Sachs, T., Wille, C., Boike, J., and Kutzbach, L. (2008) Environmental controls on ecosystem-scale CH4 emission from polygonal tundra in the Lena River Delta, Siberia. Journal of Geophysical Research 113: G00A03 [6] Wille, C., Kutzbach, L., Sachs, T., Wagner, D., and Pfeiffer, E.M. (2008) Methane emissions from Siberian arctic polygonal tundra: Eddy covariance measurements and modeling. Global Change Biology 14: 1395-1408 [7] Schneider, J., Grosse, G., and Wagner, D. (2009) Land cover classification of tundra environments in the Arctic Lena Delta based on Landsat 7 ETM+ data and its application for upscaling of methane emissions. Remote Sensing of Environment 113: 380-391 [8] Walter, K.M., Edwards, M.E., Grosse, G., Zimov, S.A., and Chapin III, F.S. (2007) Thermokarst Lakes as a Source of Atmospheric CH4 During the Last Deglaciation. Science 318: 633-636

Vibrational energy levels for CH4 from an ab initio potential

NASA Technical Reports Server (NTRS)

Schwenke, D. W.; Partridge, H.

2001-01-01

Many areas of astronomy and astrophysics require an accurate high temperature spectrum of methane (CH4). The goal of the present research is to determine an accurate ab initio potential energy surface (PES) for CH4. As a first step towards this goal, we have determined a PES including up to octic terms. We compare our results with experiment and to a PES based on a quartic expansion. Our octic PES gives good agreement with experiment for all levels, while the quartic PES only for the lower levels.

Information content analysis: the potential for methane isotopologue retrieval from GOSAT-2

NASA Astrophysics Data System (ADS)

Malina, Edward; Yoshida, Yukio; Matsunaga, Tsuneo; Muller, Jan-Peter

2018-02-01

Atmospheric methane is comprised of multiple isotopic molecules, with the most abundant being 12CH4 and 13CH4, making up 98 and 1.1 % of atmospheric methane respectively. It has been shown that is it possible to distinguish between sources of methane (biogenic methane, e.g. marshland, or abiogenic methane, e.g. fracking) via a ratio of these main methane isotopologues, otherwise known as the δ13C value. δ13C values typically range between -10 and -80 ‰, with abiogenic sources closer to zero and biogenic sources showing more negative values. Initially, we suggest that a δ13C difference of 10 ‰ is sufficient, in order to differentiate between methane source types, based on this we derive that a precision of 0.2 ppbv on 13CH4 retrievals may achieve the target δ13C variance. Using an application of the well-established information content analysis (ICA) technique for assumed clear-sky conditions, this paper shows that using a combination of the shortwave infrared (SWIR) bands on the planned Greenhouse gases Observing SATellite (GOSAT-2) mission, 13CH4 can be measured with sufficient information content to a precision of between 0.7 and 1.2 ppbv from a single sounding (assuming a total column average value of 19.14 ppbv), which can then be reduced to the target precision through spatial and temporal averaging techniques. We therefore suggest that GOSAT-2 can be used to differentiate between methane source types. We find that large unconstrained covariance matrices are required in order to achieve sufficient information content, while the solar zenith angle has limited impact on the information content.

The Missing Link: Early Methane ("T") Dwarfs in the Sloan Digital Sky Survey.

PubMed

Leggett; Geballe; Fan; Schneider; Gunn; Lupton; Knapp; Strauss; McDaniel; Golimowski; Henry; Peng; Tsvetanov; Uomoto; Zheng; Hill; Ramsey; Anderson; Annis; Bahcall; Brinkmann; Chen; Csabai; Fukugita; Hennessy; Hindsley; Ivezic; Lamb; Munn; Pier; Schlegel; Smith; Stoughton; Thakar; York

2000-06-10

We report the discovery of three cool brown dwarfs that fall in the effective temperature gap between the latest L dwarfs currently known, with no methane absorption bands in the 1-2.5 µm range, and the previously known methane (T) dwarfs, whose spectra are dominated by methane and water. The newly discovered objects were detected as very red objects in the Sloan Digital Sky Survey imaging data and have JHK colors between the red L dwarfs and the blue Gl 229B-like T dwarfs. They show both CO and CH(4) absorption in their near-infrared spectra in addition to H(2)O, with weaker CH(4) absorption features in the H and K bands than those in all other methane dwarfs reported to date. Due to the presence of CH(4) in these bands, we propose that these objects are early T dwarfs. The three form part of the brown dwarf spectral sequence and fill in the large gap in the overall spectral sequence from the hottest main-sequence stars to the coolest methane dwarfs currently known.

Effect of dilution and ash supplement on the bio-methane potential of palm oil mill effluent (POME)

NASA Astrophysics Data System (ADS)

Jijai, Sunwanee; Muleng, Saina; Siripatana, Chairat

2017-08-01

This study aimed to evaluate the bio-methane potential of POME at different dilutions (100, 80, 60, 40, and 20 percent of initial POME) and different pH dues to different levels of ash supplement. Five different amounts of ash were added to digesters (0, 2, 4, 6, and 8 grams of ash were added to 170 ml of POME respectively). The digesters were operated in batch anaerobic digestion systems at room temperature (28-30 °C) and the experiments were performed in duplicate manner. The results showed that POME without dilution gave highest cumulative biogas (950 ml). However, 80% dilution from original POME gave the highest methane yield (45.83 mL CH4/ gCODadded or 103.13 mL CH4/ gCODremoved). Finally, the results of experiment 2, this adding ash into POME increased pH as well as enhanced the biogas production. It was found that adding ash at the ash:POME ratio of 2 g: 170 ml gave the highest both the cumulative biogas and methane yield (1,520 mL and 218.79 mL CH4/ gCODremoved respectively). The addition of ash in the raw waste of POME gave the pH in the range of criteria and highest bio-methane potential. The modified Gompertz equation, Schnute as well as Monod kinetic models were used to compare the data from the experiments. It was found that the factors that affected included, the bio-methane production and the kinetic parameters (the maximum specific methane production rates (Rm ml/day) and the methane production potential (P, mL)), initial COD, nutrients, levels of dilution, and initial pH (by adding different level of ash). However, λ (lag phase period) was not affected by initial COD and other factors. While Monod kinetics provides valuable insight in explaining what could happen behind the systematic trends.

Investigating the Hydro-geochemical Impact of Fugitive Methane on Groundwater: The Borden Aquifer Controlled Release Study

NASA Astrophysics Data System (ADS)

Cahill, A. G.; Parker, B. L.; Cherry, J. A.; Mayer, K. U.; Mayer, B.; Ryan, C.

2014-12-01

Shale gas development by hydraulic fracturing is believed by many to have the potential to transform the world's energy economy. The propensity of this technique to cause significant environmental impact is strongly contested and lacks evidence. Fugitive methane (CH4), potentially mobilized during well drilling, the complex extraction process and/or leaking well seals over time is arguably the greatest concern. Advanced understanding of CH4 mobility and fate in the subsurface is needed in order to assess risks, design suitable monitoring systems and gain public trust. Currently knowledge on subsurface CH4 mobilization and migration at scales relevant to shale gas development is lacking. Consequently a shallow aquifer controlled CH4 release experiment is being conducted at the Borden aquifer research facility (an unconfined, unconsolidated silicate sand aquifer) in Ontario, Canada. During the experiment, 100 m3 of gas phase CH4 was injected into the saturated zone over approximately 60 days through 2 inclined sparging wells (4.5 and 9 m depth) at rates relevant to natural gas well casing vent flows. The gas mobility and fate is being comprehensively monitored temporally and spatially in both the saturated and unsaturated zones considering; aqueous chemistry (including stable isotopes), soil gas characterization, surface efflux, geophysics (GPR and ERT), real time sensors (total dissolved gas pressure, soil moisture content, CH4 and CO2), mineralogical and microbiological characterization before, during and after injection. An overview of this unique study will be given including experimental design, monitoring system configuration and preliminary results. This multidisciplinary study will provide important insights regarding the mechanisms and rates for shallow CH4 migration, attenuation and water quality impacts that will inform baseline groundwater monitoring programs and retrospective forensic studies.

Investigating the Hydro-geochemical Impact of Fugitive Methane on Groundwater: The Borden Aquifer Controlled Release Study

NASA Astrophysics Data System (ADS)

Cahill, A. G.; Parker, B. L.; Cherry, J. A.; Mayer, K. U.; Mayer, B.; Ryan, C.

2015-12-01

Shale gas development by hydraulic fracturing is believed by many to have the potential to transform the world's energy economy. The propensity of this technique to cause significant environmental impact is strongly contested and lacks evidence. Fugitive methane (CH4), potentially mobilized during well drilling, the complex extraction process and/or leaking well seals over time is arguably the greatest concern. Advanced understanding of CH4 mobility and fate in the subsurface is needed in order to assess risks, design suitable monitoring systems and gain public trust. Currently knowledge on subsurface CH4 mobilization and migration at scales relevant to shale gas development is lacking. Consequently a shallow aquifer controlled CH4 release experiment is being conducted at the Borden aquifer research facility (an unconfined, unconsolidated silicate sand aquifer) in Ontario, Canada. During the experiment, 100 m3 of gas phase CH4 was injected into the saturated zone over approximately 60 days through 2 inclined sparging wells (4.5 and 9 m depth) at rates relevant to natural gas well casing vent flows. The gas mobility and fate is being comprehensively monitored temporally and spatially in both the saturated and unsaturated zones considering; aqueous chemistry (including stable isotopes), soil gas characterization, surface efflux, geophysics (GPR and ERT), real time sensors (total dissolved gas pressure, soil moisture content, CH4 and CO2), mineralogical and microbiological characterization before, during and after injection. An overview of this unique study will be given including experimental design, monitoring system configuration and preliminary results. This multidisciplinary study will provide important insights regarding the mechanisms and rates for shallow CH4 migration, attenuation and water quality impacts that will inform baseline groundwater monitoring programs and retrospective forensic studies.

Methane emission from animals: A Global High-Resolution Data Base

NASA Astrophysics Data System (ADS)

Lerner, Jean; Matthews, Elaine; Fung, Inez

1988-06-01

We present a high-resolution global data base of animal population densities and associated methane emission. Statistics on animal populations from the Food and Agriculture Organization and other sources have been compiled. Animals were distributed using a 1° resolution data base of countries of the world and a 1° resolution data base of land use. The animals included are cattle and dairy cows, water buffalo, sheep, goats, camels, pigs, horses and caribou. Published estimates of methane production from each type of animal have been applied to the animal populations to yield a global distribution of annual methane emission by animals. There is large spatial variability in the distribution of animal populations and their methane emissions. Emission rates greater than 5000 kg CH4 km-2 yr-1 are found in small regions such as Bangladesh, the Benelux countries, parts of northern India, and New Zealand. Of the global annual emission of 75.8 Tg CH4 for 1984, about 55% is concentrated between 25°N and 55°N, a significant contribution to the observed north-south gradient of atmospheric methane concentration. A magnetic tape of the global data bases is available from the authors.

Effects of experimental warming and elevated CO2 on surface methane and CO­2 fluxes from a boreal black spruce peatland

NASA Astrophysics Data System (ADS)

Gill, A. L.; Finzi, A.; Hsieh, I. F.; Giasson, M. A.

2016-12-01

High latitude peatlands represent a major terrestrial carbon store sensitive to climate change, as well as a globally significant methane source. While elevated atmospheric carbon dioxide concentrations and warming temperatures may increase peat respiration and C losses to the atmosphere, reductions in peatland water tables associated with increased growing season evapotranspiration may alter the nature of trace gas emission and increase peat C losses as CO2 relative to methane (CH4). As CH4 is a greenhouse gas with twenty times the warming potential of CO2, it is critical to understand how surface fluxes of CO2 and CH4 will be influenced by factors associated with global climate change. We used automated soil respiration chambers to assess the influence of elevated atmospheric CO2 and whole ecosystem warming on peatland CH4 and CO2 fluxes at the SPRUCE (Spruce and Peatland Responses Under Climatic and Environmental Change) Experiment in northern Minnesota. Here we report soil iCO2 and iCH4 flux responses to the first year of belowground warming and the first season of whole ecosystem warming and elevated CO2 treatments. We find that peat methane fluxes are more sensitive to warming treatments than peat CO2 fluxes, particularly in hollow peat microforms. Surface CO2:CH4 flux ratios decreased across warming treatments, suggesting that the temperature sensitivity of methane production overshadows the effect of peat drying and surface aeration in the short term. δ13C of the emitted methane was more depleted in the early and late growing season, indicating a transition from hydrogenotrophic to acetoclastic methanogenesis during periods of high photosynthetic input. The measurement record demonstrates that belowground warming has measureable impacts on the nature of peat greenhouse gas emission within one year of treatment.

Methane emissions from a Californian landfill, determined from airborne remote sensing and in situ measurements

NASA Astrophysics Data System (ADS)

Krautwurst, Sven; Gerilowski, Konstantin; Jonsson, Haflidi H.; Thompson, David R.; Kolyer, Richard W.; Iraci, Laura T.; Thorpe, Andrew K.; Horstjann, Markus; Eastwood, Michael; Leifer, Ira; Vigil, Samuel A.; Krings, Thomas; Borchardt, Jakob; Buchwitz, Michael; Fladeland, Matthew M.; Burrows, John P.; Bovensmann, Heinrich

2017-09-01

Fugitive emissions from waste disposal sites are important anthropogenic sources of the greenhouse gas methane (CH4). As a result of the growing world population and the recognition of the need to control greenhouse gas emissions, this anthropogenic source of CH4 has received much recent attention. However, the accurate assessment of the CH4 emissions from landfills by modeling and existing measurement techniques is challenging. This is because of inaccurate knowledge of the model parameters and the extent of and limited accessibility to landfill sites. This results in a large uncertainty in our knowledge of the emissions of CH4 from landfills and waste management. In this study, we present results derived from data collected during the research campaign COMEX (CO2 and MEthane eXperiment) in late summer 2014 in the Los Angeles (LA) Basin. One objective of COMEX, which comprised aircraft observations of methane by the remote sensing Methane Airborne MAPper (MAMAP) instrument and a Picarro greenhouse gas in situ analyzer, was the quantitative investigation of CH4 emissions. Enhanced CH4 concentrations or CH4 plumes were detected downwind of landfills by remote sensing aircraft surveys. Subsequent to each remote sensing survey, the detected plume was sampled within the atmospheric boundary layer by in situ measurements of atmospheric parameters such as wind information and dry gas mixing ratios of CH4 and carbon dioxide (CO2) from the same aircraft. This was undertaken to facilitate the independent estimation of the surface fluxes for the validation of the remote sensing estimates. During the COMEX campaign, four landfills in the LA Basin were surveyed. One landfill repeatedly showed a clear emission plume. This landfill, the Olinda Alpha Landfill, was investigated on 4 days during the last week of August and first days of September 2014. Emissions were estimated for all days using a mass balance approach. The derived emissions vary between 11.6 and 17.8 kt CH4 yr-1 with related uncertainties in the range of 14 to 45 %. The comparison of the remote sensing and in situ based CH4 emission rate estimates reveals good agreement within the error bars with an average of the absolute differences of around 2.4 kt CH4 yr-1 (±2. 8 kt CH4 yr-1). The US Environmental Protection Agency (EPA) reported inventory value is 11.5 kt CH4 yr-1 for 2014, on average 2.8 kt CH4 yr-1 (±1. 6 kt CH4 yr-1) lower than our estimates acquired in the afternoon in late summer 2014. This difference may in part be explained by a possible leak located on the southwestern slope of the landfill, which we identified in the observations of the Airborne Visible/Infrared Imaging Spectrometer - Next Generation (AVIRIS-NG) instrument, flown contemporaneously aboard a second aircraft on 1 day.

Sources and sinks of methane in the African Savanna. CH4 emissions from biomass burning

NASA Astrophysics Data System (ADS)

Delmas, R. A.; Marenco, A.; Tathy, J. P.; Cros, B.; Baudet, J. G. R.

1991-04-01

Sources and sinks of atmospheric methane are studied in savanna regions of west and central Africa. Flux measured over dry savanna soils, using static chambers, is always negative the average uptake rate being 2×1010 molecules/cm2/s. In these regions, sources are linked to biomass burning. Methane and CO2 emission from combustion of savanna plants and wood is studied by both field experiments and laboratory experiments using a combustion chamber. For savanna plants most of the carbon (85%) contained in the biomaterial is volatilized as CO2 and 0.1 to 0.25% as methane. For graminaceous plants like loudetia simplex the ratio C-CH4/C-CO2 is 0.11%; it is 0.28% for hyparrhenia the other main type of savanna plants and it attains 1.4% for the combustion of wood. In natural fire plumes this ratio is around 0.26% for savanna fires and 0.56 to 2.22% for forest fires. These results show that methane release is highly dependent on the type of combustion. Methane to CO2 ratios are also studied in vertical profiles in the troposphere taken during the TROPOZ I campaign, an aerial research expedition carried out over west Africa during the bushfire period. Within polluted layers, the average ratio of CH4 to CO2 excess over ambient air concentration is 0.34%. These results show that biomass burning in tropical Africa constitutes an important source of atmospheric methane estimated to about 9.2×106 T(CH4)/yr.

Flux Chamber Measurements of Methane Emissions and Stable Isotope Composition from an Arctic Wetland Using Field-Deployed Real-Time CRDS Vs Lab Measurements

NASA Astrophysics Data System (ADS)

Thompson, H. A.; Stern, J. C.; Graham, H. V.; Pratt, L. M.; White, J. R.

2014-12-01

The emission of CH4 from Arctic landscapes under warming climate is an important feedback in Earth's climate system. Studies of CH4 flux from Arctic wetlands have been growing in recent years, but few provide details on biogeochemical controls. Stable isotopic measurements help elucidate methane production and consumption pathways and offer important understanding about dynamics of CH4 cycling in Arctic systems. In order to demonstrate the possible instrumental approaches to measuring methane dynamics of wetlands in the Arctic, a fringing wetland of a small lake near the Russell Glacier in Southwestern Greenland was outfitted with static flux chambers and instrumented with a field-deployable Cavity Ring Down Spectrometer (CRDS) to measure real-time concentrations of CH4 and CO2 and their stable carbon isotopes. Several different wetland plant communities were included in the flux chamber experiments and field tests were conducted during several weeks in July 2014. Analytical measurements by CRDS were compared to batch samples analyzed in the laboratory using both Off-Axis Integrated Cavity Output Spectroscopy (ICOS) and Gas Chromatography-Combustion-Isotope Ratio Mass Spectrometry (GC-C-IRMS) with cryogenic pre-concentration. Results from flux chamber deployments will be presented and comparisons between the real-time field measurements and laboratory instrumental techniques will be evaluated.

Methane Emissions from Bangladesh: Bridging the Gap Between Ground-based and Space-borne Estimates

NASA Astrophysics Data System (ADS)

Peters, C.; Bennartz, R.; Hornberger, G. M.

2015-12-01

Gaining an understanding of methane (CH4) emission sources and atmospheric dispersion is an essential part of climate change research. Large-scale and global studies often rely on satellite observations of column CH4 mixing ratio whereas high-spatial resolution estimates rely on ground-based measurements. Extrapolation of ground-based measurements on, for example, rice paddies to broad region scales is highly uncertain because of spatio-temporal variability. We explore the use of ground-based river stage measurements and independent satellite observations of flooded area along with satellite measurements of CH4 mixing ratio to estimate the extent of methane emissions. Bangladesh, which comprises most of the Ganges Brahmaputra Meghna (GBM) delta, is a region of particular interest for studying spatio-temporal variation of methane emissions due to (1) broadscale rice cultivation and (2) seasonal flooding and atmospheric convection during the monsoon. Bangladesh and its deltaic landscape exhibit a broad range of environmental, economic, and social circumstances that are relevant to many nations in South and Southeast Asia. We explore the seasonal enhancement of CH4 in Bangladesh using passive remote sensing spectrometer CH4 products from the SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY) and the Atmospheric Infrared Sounder (AIRS). The seasonal variation of CH4 is compared to independent estimates of seasonal flooding from water gauge stations and space-based passive microwave water-to-land fractions from the Tropical Rainfall Measuring Mission Microwave Imager (TRMM-TMI). Annual cycles in inundation (natural and anthropogenic) and atmospheric CH4 concentrations show highly correlated seasonal signals. NOAA's HYSPLIT model is used to determine atmospheric residence time of ground CH4 fluxes. Using the satellite observations, we can narrow the large uncertainty in extrapolation of ground-based CH4 emission estimates from rice paddies, allowing for country-wide upscaling of high spatial resolution data. This approach allows for better informed carbon cycling modeling for the GBM delta and is applicable to other regions.

Adsorption and transport of methane in biochars derived from waste wood.

PubMed

Sadasivam, Bala Yamini; Reddy, Krishna R

2015-09-01

Mitigation of landfill gas (LFG) is among the critical aspects considered in the design of a landfill cover in order to prevent atmospheric pollution and control global warming. In general, landfill cover soils can partially remove methane (CH4) through microbial oxidation carried out by methanotrophic bacteria present within them. The oxidizing capacity of these landfill cover soils may be improved by adding organic materials, such as biochar, which increase adsorption and promote subsequent or simultaneous oxidation of CH4. In this study, seven wood-derived biochars and granular activated carbon (GAC) were characterized for their CH4 adsorption capacity by conducting batch and small-scale column studies. The effects of influential factors, such as exposed CH4 concentration, moisture content and temperature on CH4 adsorption onto biochars, were determined. The CH4 transport was modeled using a 1-D advection-dispersion equation that accounted for sorption. The effects of LFG inflow rates and moisture content on the combined adsorption and transport properties of biochars were determined. The maximum CH4 adsorption capacity of GAC (3.21mol/kg) was significantly higher than that of the biochars (0.05-0.9mol/kg). The CH4 gas dispersion coefficients for all of the biochars ranged from 1×10(-3) to 3×10(-3)m(2)s(-1). The presence of moisture significantly suppressed the extent of methane adsorption onto the biochars and caused the methane to break through within shorter periods of time. Overall, certain biochar types have a high potential to enhance CH4 adsorption and transport properties when used as a cover material in landfills. However, field-scale studies need to be conducted in order to evaluate the performance of biochar-based cover system under a more dynamic field condition that captures the effect of seasonal and temporal changes. Copyright © 2015 Elsevier Ltd. All rights reserved.

Arctic lakes are continuous methane sources to the atmosphere under warming conditions

NASA Astrophysics Data System (ADS)

Tan, Zeli; Zhuang, Qianlai

2015-05-01

Methane is the second most powerful carbon-based greenhouse gas in the atmosphere and its production in the natural environment through methanogenesis is positively correlated with temperature. Recent field studies showed that methane emissions from Arctic thermokarst lakes are significant and could increase by two- to four-fold due to global warming. But the estimates of this source are still poorly constrained. By using a process-based climate-sensitive lake biogeochemical model, we estimated that the total amount of methane emissions from Arctic lakes is 11.86 Tg yr-1, which is in the range of recent estimates of 7.1-17.3 Tg yr-1 and is on the same order of methane emissions from northern high-latitude wetlands. The methane emission rate varies spatially over high latitudes from 110.8 mg CH4 m-2 day-1 in Alaska to 12.7 mg CH4 m-2 day-1 in northern Europe. Under Representative Concentration Pathways (RCP) 2.6 and 8.5 future climate scenarios, methane emissions from Arctic lakes will increase by 10.3 and 16.2 Tg CH4 yr-1, respectively, by the end of the 21st century.

Estimating methane emissions in California's urban and rural regions using multitower observations

DOE PAGES

Jeong, Seongeun; Newman, Sally; Zhang, Jingsong; ...

2016-11-05

Here, we present an analysis of methane (CH 4) emissions using atmospheric observations from 36 thirteen sites in California during June 2013 – May 2014. A hierarchical Bayesian inversion 37 method is used to estimate CH 4 emissions for spatial regions (0.3° pixels for major regions) by 38 comparing measured CH 4 mixing ratios with transport model (WRF-STILT) predictions based 39 on seasonally varying California-specific CH 4 prior emission models. The transport model is 40 assessed using a combination of meteorological and carbon monoxide (CO) measurements 41 coupled with the gridded California Air Resources Board (CARB) carbon monoxide (CO) 42more » emission inventory. Hierarchical Bayesian inversion suggests that state annual anthropogenic 43 CH 4 emissions are 2.42 ± 0.49 Tg CH 4/yr (at 95% confidence, including transport bias 44 uncertainty), higher (1.2 - 1.8 times) than the CARB current inventory (1.64 Tg CH 4/yr in 2013). 45 We note that the estimated CH 4 emissions drop to 1.0 - 1.6 times the CARB inventory if we 46 correct for the 10% median CH 4 emissions assuming the bias in CO analysis is applicable to 47 CH 4. The CH 4 emissions from the Central Valley and urban regions (San Francisco Bay and 48 South Coast Air Basins) account for ~58% and 26% of the total posterior emissions, 49 respectively. This study suggests that the livestock sector is likely the major contributor to the 50 state total CH 4 emissions, in agreement with CARB’s inventory. Attribution to source sectors for 51 sub-regions of California using additional trace gas species would further improve the 52 quantification of California’s CH 4 emissions and mitigation efforts towards the California Global 53 Warming Solutions Act of 2006 (AB-32).« less

Estimating methane emissions in California's urban and rural regions using multitower observations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jeong, Seongeun; Newman, Sally; Zhang, Jingsong

Here, we present an analysis of methane (CH 4) emissions using atmospheric observations from 36 thirteen sites in California during June 2013 – May 2014. A hierarchical Bayesian inversion 37 method is used to estimate CH 4 emissions for spatial regions (0.3° pixels for major regions) by 38 comparing measured CH 4 mixing ratios with transport model (WRF-STILT) predictions based 39 on seasonally varying California-specific CH 4 prior emission models. The transport model is 40 assessed using a combination of meteorological and carbon monoxide (CO) measurements 41 coupled with the gridded California Air Resources Board (CARB) carbon monoxide (CO) 42more » emission inventory. Hierarchical Bayesian inversion suggests that state annual anthropogenic 43 CH 4 emissions are 2.42 ± 0.49 Tg CH 4/yr (at 95% confidence, including transport bias 44 uncertainty), higher (1.2 - 1.8 times) than the CARB current inventory (1.64 Tg CH 4/yr in 2013). 45 We note that the estimated CH 4 emissions drop to 1.0 - 1.6 times the CARB inventory if we 46 correct for the 10% median CH 4 emissions assuming the bias in CO analysis is applicable to 47 CH 4. The CH 4 emissions from the Central Valley and urban regions (San Francisco Bay and 48 South Coast Air Basins) account for ~58% and 26% of the total posterior emissions, 49 respectively. This study suggests that the livestock sector is likely the major contributor to the 50 state total CH 4 emissions, in agreement with CARB’s inventory. Attribution to source sectors for 51 sub-regions of California using additional trace gas species would further improve the 52 quantification of California’s CH 4 emissions and mitigation efforts towards the California Global 53 Warming Solutions Act of 2006 (AB-32).« less

Above- and below-ground methane fluxes and methanotrophic activity in a landfill-cover soil

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schroth, M.H., E-mail: martin.schroth@env.ethz.ch; Eugster, W.; Gomez, K.E.

2012-05-15

Highlights: Black-Right-Pointing-Pointer We quantify above- and below-ground CH{sub 4} fluxes in a landfill-cover soil. Black-Right-Pointing-Pointer We link methanotrophic activity to estimates of CH{sub 4} loading from the waste body. Black-Right-Pointing-Pointer Methane loading and emissions are highly variable in space and time. Black-Right-Pointing-Pointer Eddy covariance measurements yield largest estimates of CH{sub 4} emissions. Black-Right-Pointing-Pointer Potential methanotrophic activity is high at a location with substantial CH{sub 4} loading. - Abstract: Landfills are a major anthropogenic source of the greenhouse gas methane (CH{sub 4}). However, much of the CH{sub 4} produced during the anaerobic degradation of organic waste is consumed by methanotrophic microorganismsmore » during passage through the landfill-cover soil. On a section of a closed landfill near Liestal, Switzerland, we performed experiments to compare CH{sub 4} fluxes obtained by different methods at or above the cover-soil surface with below-ground fluxes, and to link methanotrophic activity to estimates of CH{sub 4} ingress (loading) from the waste body at selected locations. Fluxes of CH{sub 4} into or out of the cover soil were quantified by eddy-covariance and static flux-chamber measurements. In addition, CH{sub 4} concentrations at the soil surface were monitored using a field-portable FID detector. Near-surface CH{sub 4} fluxes and CH{sub 4} loading were estimated from soil-gas concentration profiles in conjunction with radon measurements, and gas push-pull tests (GPPTs) were performed to quantify rates of microbial CH{sub 4} oxidation. Eddy-covariance measurements yielded by far the largest and probably most representative estimates of overall CH{sub 4} emissions from the test section (daily mean up to {approx}91,500 {mu}mol m{sup -2} d{sup -1}), whereas flux-chamber measurements and CH{sub 4} concentration profiles indicated that at the majority of locations the cover soil was a net sink for atmospheric CH{sub 4} (uptake up to -380 {mu}mol m{sup -2} d{sup -1}) during the experimental period. Methane concentration profiles also indicated strong variability in CH{sub 4} loading over short distances in the cover soil, while potential methanotrophic activity derived from GPPTs was high (v{sub max} {approx} 13 mmol L{sup -1}(soil air) h{sup -1}) at a location with substantial CH{sub 4} loading. Our results provide a basis to assess spatial and temporal variability of CH{sub 4} dynamics in the complex terrain of a landfill-cover soil.« less

Landscape analysis of soil methane flux across complex terrain

NASA Astrophysics Data System (ADS)

Kaiser, Kendra E.; McGlynn, Brian L.; Dore, John E.

2018-05-01

Relationships between methane (CH4) fluxes and environmental conditions have been extensively explored in saturated soils, while research has been less prevalent in aerated soils because of the relatively small magnitudes of CH4 fluxes that occur in dry soils. Our study builds on previous carbon cycle research at Tenderfoot Creek Experimental Forest, Montana, to identify how environmental conditions reflected by topographic metrics can be leveraged to estimate watershed scale CH4 fluxes from point scale measurements. Here, we measured soil CH4 concentrations and fluxes across a range of landscape positions (7 riparian, 25 upland), utilizing topographic and seasonal (29 May-12 September) gradients to examine the relationships between environmental variables, hydrologic dynamics, and CH4 emission and uptake. Riparian areas emitted small fluxes of CH4 throughout the study (median: 0.186 µg CH4-C m-2 h-1) and uplands increased in sink strength with dry-down of the watershed (median: -22.9 µg CH4-C m-2 h-1). Locations with volumetric water content (VWC) below 38 % were methane sinks, and uptake increased with decreasing VWC. Above 43 % VWC, net CH4 efflux occurred, and at intermediate VWC net fluxes were near zero. Riparian sites had near-neutral cumulative seasonal flux, and cumulative uptake of CH4 in the uplands was significantly related to topographic indices. These relationships were used to model the net seasonal CH4 flux of the upper Stringer Creek watershed (-1.75 kg CH4-C ha-1). This spatially distributed estimate was 111 % larger than that obtained by simply extrapolating the mean CH4 flux to the entire watershed area. Our results highlight the importance of quantifying the space-time variability of net CH4 fluxes as predicted by the frequency distribution of landscape positions when assessing watershed scale greenhouse gas balances.

Influence of water table fluctuations on subsurface methane dynamics and surface fluxes in seasonally flooded subtropical pastures.

NASA Astrophysics Data System (ADS)

Chamberlain, S.; Gomez-Casanovas, N.; Boughton, E.; Keel, E.; Walter, M. T.; Groffman, P. M.; Sparks, J. P.

2015-12-01

Seasonally flooded subtropical pastures are major sources of methane (CH4), and periodic flooding drives complex emission dynamics from these ecosystems. Understanding the mechanisms of belowground CH4 dynamics driving soil surface fluxes is needed to better understand emissions from these systems and their response to environmental change. We investigated subsurface CH4 dynamics in relation to net surface fluxes using laboratory water table manipulations and compared these results to eddy covariance-measured fluxes to link within-soil CH4 dynamics to observed ecosystem fluxes. Pronounced hysteresis was observed in ecosystem CH4 fluxes during precipitation driven flooding events. This dynamic was replicated in mesocosm experiments, with maximum CH4 fluxes observed during periods of water table recession. Hysteresis dynamics were best explained by oxygen dynamics during precipitation recharge events and the oxidation of CH4 produced in organic soil horizons during water table recession. We observed distinct CH4 dynamics between surface organic and deeper mineral soil horizons. In surface organic soil horizons, high levels of CH4 production were temporally linked to observed surface emissions. In contrast, high concentrations of CH4 observed in deeper mineral soils did not contribute to surface fluxes. Methane production potentials in surface organic soils were orders of magnitude higher than in mineral soils, suggesting that over longer flooding regimes CH4 produced in mineral horizons is unlikely to be a significant component of net surface emissions. Our results demonstrate that distinct CH4 dynamics may be stratified by depth, and flooding of the near-surface organic soils drives the high magnitude CH4 fluxes observed from subtropical pastures. These results suggest that relatively small changes in pasture water table dynamics can drive large changes in net CH4 emissions if surface organic soils remain saturated over longer time scales.

Carbon and hydrogen isotopic systematics of dissolved methane in small seasonally ice-covered lakes near the margin of the Greenland ice sheet

NASA Astrophysics Data System (ADS)

Cadieux, S. B.; White, J. R.; Pratt, L. M.; Peng, Y.; Young, S. A.

2013-12-01

Northern lakes contribute from 6-16% of annual methane inputs to Earth's atmosphere, yet little is known about the seasonal biogeochemistry of CH4 cycling, particularly for lakes in the Arctic. Studies during ice-free conditions have been conducted in Alaskan, Swedish and Siberian lakes. However, there is little information on CH4 cycling under ice-covered conditions, and few stable isotopic measurements, which can help elucidate production and consumption pathways. In order to better understand methane dynamics of ice-covered Arctic lakes, 4 small lakes (surface area <1 km2) within a narrow valley extending from the Russells Glacier to Søndre Strømfjord in Southwestern Greenland were examined during summer stratification and winter ice-cover. Lakes in the study area are ice-covered from mid-September to mid-June. In both seasons, variations in the concentrations and isotopic composition of methane with depth were related to redox fluctuations. During late winter under~2 m of ice, the entire water column was anoxic with wide variation in methane concentrationsand isotopic composition from lake to lake. In three of the lakes, CH4 concentrations and δ13C were relatively stable over the depth of the water column, averaging from 120 to 480μM, with δ13CH4 values from -56‰ to -66‰, respectively. Methane concentrations in the other lake increased with depth from <1 μM below the ice to 800 μM at the sediment/water interface, while δ13C decreased by 30‰ from -30‰ to -70‰ over this depth. In all the lakes, δ13C of sediment porewater was lighter than the overlying water by at least 10‰. The δD-CH4 in the water column ranged from -370‰ to -50‰, exhibiting covariance with δ13C consistent with significant methanotrophic activity. In the sediment, δD-CH4 values ranged from -330‰ to -275‰, and were inversely correlated with δ13C. We will present detailed information on redox dynamics as a controlling factor in methane cycling, and explore the effects of differing microbial communities and carbon supply. Our study suggests that shallow lakes in continuous permafrost landscapes of the Arctic develop distinct methane cycling dynamics despite their close proximity.

Methane production potential and emission at different water levels in the restored reed wetland of Hangzhou Bay

PubMed Central

Sheng, Xuancai; Wu, Ming; Wu, Hao; Ning, Xiao

2017-01-01

Changes in the hydrological conditions of coastal wetlands may potentially affect the role of wetlands in the methane (CH4) cycle. In this study, the CH4 production potential and emissions from restored coastal reed wetlands at different water levels were examined in eastern China at a field scale in two phenological seasons. Results showed that the total CH4 flux from reeds at various water levels were positive, indicating that they were “sources” of CH4. During the peak growing season, CH4 flux from reeds was greater than that during the spring thaw. CH4 flux from reeds in inundated conditions was greater than that in non-inundated conditions. The CH4 production potential during the peak growing season was far greater than that during the spring thaw. However, the effect of water level on wetland CH4 production potential differed among seasons. The correlations among CH4 production potential, soil properties and CH4 flux change at different water level. These results demonstrate that water level was related to CH4 production and CH4 flux. The growing season also plays a role in CH4 fluxes. Controlling the hydrological environment in restored wetlands has important implications for the maintenance of their function as carbon sinks. PMID:28968419

Global methane and nitrous oxide emissions from terrestrial ecosystems due to multiple environmental changes

DOE PAGES

Tian, Hanqin; Chen, Guangsheng; Lu, Chaoqun; ...

2015-03-16

Greenhouse gas (GHG)-induced climate change is among the most pressing sustainability challenges facing humanity today, posing serious risks for ecosystem health. Methane (CH 4) and nitrous oxide (N 2O) are the two most important GHGs after carbon dioxide (CO 2), but their regional and global budgets are not well known. In this paper, we applied a process-based coupled biogeochemical model to concurrently estimate the magnitude and spatial and temporal patterns of CH 4 and N 2O fluxes as driven by multiple environmental changes, including climate variability, rising atmospheric CO 2, increasing nitrogen deposition, tropospheric ozone pollution, land use change, andmore » nitrogen fertilizer use.« less

A laser flash photolysis-resonance fluorescence kinetics study of the reaction Cl/2P/ + CH4 yields CH3 + HCl

NASA Technical Reports Server (NTRS)

Ravishankara, A. R.; Wine, P. H.

1980-01-01

The technique of laser flash photolysis-resonance fluorescence is employed to study the kinetics of the reaction Cl(2P) + CH4 yields CH3 + HCl over the temperature range 221-375 K. At temperatures less than or equal to 241 K the apparent bimolecular rate constant is found to be dependent upon the identity of the chemically inert gases in the reaction mixture. For Cl2/CH4/He reaction mixtures (total pressure = 50 torr) different bimolecular rate constants are measured at low and high methane concentrations. For Cl2/CH4/CCl/He and Cl2/CH4/Ar reaction mixtures, the bimolecular rate constant is independent of methane concentration, being approximately equal to the rate constant measured at low methane concentrations for Cl2/CH4/He mixtures. These rate constants are in good agreement with previous results obtained using the discharge flow-resonance fluorescence and competitive chlorination techniques. At 298 K the measured bimolecular rate constant is independent of the identity of the chemically inert gases in the reaction mixture and in good agreement with all previous investigations. The low-temperature results obtained in this investigation and all previous investigations can be rationalized in terms of a model which assumes that the Cl(2P 1/2) state reacts with CH4 much faster than the Cl(2P 3/2) state. Extrapolation of this model to higher temperatures, however, is not straightforward.

Marine bacterial degradation of brominated methanes

USGS Publications Warehouse

Goodwin, K.D.; Lidstrom, M.E.; Oremland, R.S.

1997-01-01

Brominated methanes are ozone-depleting compounds whose natural sources include marine algae such as kelp. Brominated methane degradation by bacteria was investigated to address whether bacterial processes might effect net emission of these compounds to the atmosphere. Bacteria in seawater collected from California kelp beds degraded CH2Br2 but not CHBr3. Specific inhibitors showed that methanotrophs and nitrifiers did not significantly contribute to CH2Br2 removal. A seawater enrichment culture oxidized 14CH2Br2 to 14CO2 as well as 14CH3Br to 14CO2. The rates of CH2Br2 degradation in laboratory experiments suggest that bacterial degradation of CH2Br2 in a kelp bed accounts for <1% of the CH2Br2 produced by the kelp. However, the half-life of CH2Br2 due to bacterial removal appears faster than hydrolysis and within an order of magnitude of volatilization to the atmosphere.Brominated methanes are ozone-depleting compounds whose natural sources include marine algae such as kelp. Brominated methane degradation by bacteria was investigated to address whether bacterial processes might effect net emission of these compounds to the atmosphere. Bacteria in seawater collected from California kelp beds degraded CH2Br2 but not CHBr3. Specific inhibitors showed that methanotrophs and nitrifiers did not significantly contribute to CH2Br2 removal. A seawater enrichment culture oxidized 14CH2Br2 to 14CO2 as well as 14CH3Br to 14CO2. The rates of CH2Br2 degradation in laboratory experiments suggest that bacterial degradation of CH2Br2 in a kelp bed accounts for <1% of the CH2Br2 produced by the kelp. However, the half-life of CH2Br2 due to bacterial removal appears faster than hydrolysis and within an order of magnitude of volatilization to the atmosphere.

Tidal variability in methane and nitrous oxide emissions along a subtropical estuarine gradient

NASA Astrophysics Data System (ADS)

Sturm, Katrin; Werner, Ursula; Grinham, Alistair; Yuan, Zhiguo

2017-06-01

This study investigates the tidal variability in methane (CH4) and nitrous oxide (N2O) emissions along a gradient of the subtropical Brisbane River estuary. Sampling was conducted at the upper, middle and lower reaches over two tidal cycles in 2013 and 2014. Methane and N2O emissions varied significantly over tidal cycles at all sites. Methane and N2O emissions measured at all locations and in both campaigns varied substantially in time, with the maximum to minimum flux ratio in a cycle varying between 2.5 - 9 and 1.7-4.7 times, respectively. Methane emissions peaked just before or at slack tides. In comparison, no clear patterns were observed between the N2O emissions and the tidal cycle despite there being large variations in N2O emissions in some cases. Methane concentrations were elevated during low tides whereas N2O concentrations showed no clear pattern over the tidal cycle. Surface water concentrations and tidal currents played important roles in CH4 and N2O emissions, but wind did not. Our findings show that measurements at a single point in time and site would result in significant errors in CH4 and N2O emission estimates. An adequate and careful sampling scheme is required to capture spatial and temporal variations of CH4 and N2O emissions and surface water concentrations which should cover at least one tidal cycle in different estuarine sections.

Detections and Sensitive Upper Limits for Methane and Related Trace Gases on Mars during 2003-2014, and planned extensions in 2016

NASA Astrophysics Data System (ADS)

Mumma, Michael J.; Villanueva, Geronimo L.; Novak, Robert E.

2015-11-01

Five groups report methane detections on Mars; all results suggest local release and high temporal variability [1-7]. Our team searched for CH4 on many dates and seasons and detected it on several dates [1, 9, 10]. TLS (Curiosity rover) reported methane upper limits [6], and then detections [7] that were consistent in size with earlier reports and that also showed rapid modulation of CH4 abundance.[8] argued that absorption features assigned to Mars 12CH4 by [1] might instead be weak lines of terrestrial 13CH4. If not properly removed, terrestrial 13CH4 signatures would appear on the blue wing of terrestrial 12CH4 even when Mars is red-shifted - but they do not (Fig. S6 of [1]), demonstrating that terrestrial signatures were correctly removed. [9] demonstrated that including the dependence of δ13CH4 with altitude did not affect the residual features, nor did taking δ13CH4 as zero. Were δ13CH4 important, its omission would have overemphasized the depth of 13CH4 terrestrial absorption, introducing emission features in the residual spectra [1]. However, the residual features are seen in absorption, establishing their origin as non-terrestrial - [8] now agrees with this view.We later reported results for multiple organic gases (CH4, CH3OH, H2CO, C2H6, C2H2, C2H4), hydroperoxyl (HO2), three nitriles (N2O, NH3, HCN) and two chlorinated species (HCl, CH3Cl) [9]. Most of these species cannot be detected with current space assets, owing to instrumental limitations (e.g., spectral resolving power). However, the high resolution infrared spectrometers (NOMAD, ACS) on ExoMars 2016 (Trace Gas Orbiter) will begin measurements in late 2016. In solar occultation, TGO sensitivities will far exceed prior capabilities.We published detailed hemispheric maps of H2O and HDO on Mars, inferring the size of a lost early ocean [10]. In 2016, we plan to acquire 3-D spatial maps of HDO and H2O with ALMA, and improved maps of organics with iSHELL/NASA-IRTF.References: [1] Mumma et al. Sci09; [2] Formisano et al. Sci04; [3] Krasnopolsky et al. Icar04; [4] Fonti and Marzo A&A10 [5] Krasnopolsky, Icar12; [6] Webster et al. Sci13; [7] Webster et al. Sci15; [8] Zahnle et al. Icar11; [9] Villanueva et al. Icar13; [10] Villanueva et al. Sci15.

New Y and T Dwarfs from WISE Identified by Methane Imaging

NASA Astrophysics Data System (ADS)

Tinney, C. G.; Kirkpatrick, J. Davy; Faherty, Jacqueline K.; Mace, Gregory N.; Cushing, Mike; Gelino, Christopher R.; Burgasser, Adam J.; Sheppard, Scott S.; Wright, Edward L.

2018-06-01

We identify new Y- and T-type brown dwarfs from the WISE All Sky data release using images obtained in filters that divide the traditional near-infrared H and J bands into two halves—specifically {CH}}4{{s}} and CH4l in the H and J2, and J3 in the J. This proves to be very effective at identifying cool brown dwarfs via the detection of their methane absorption, as well as providing preliminary classification using methane colors and WISE -to-near-infrared colors. New and updated calibrations between T/Y spectral types and {CH}}4{{s}}–CH4l J3–W2, and {CH}}4{{s}}–W2 colors are derived, producing classification estimates good to a few spectral sub-types. We present photometry for a large sample of T and Y dwarfs in these filters, together with spectroscopy for 23 new ultra-cool dwarfs—2 Y dwarfs and 21 T dwarfs. We identify a further 8 new cool brown dwarfs, which we have high confidence are T dwarfs based on their methane photometry. We find that, for objects observed on a 4 m class telescope at J-band magnitudes of ∼20 or brighter, {CH}}4{{s}}–CH4l is the more powerful color for detecting objects and then estimating spectral types. Due to the lower sky background in the J-band, the J3 and J2 bands are more useful for identifying fainter cool dwarfs at J ≳ 22. The J3–J2 color is poor at estimating spectral types. But fortunately, once J3–J2 confirms that an object is a cool dwarf, the J3–W2 color is very effective at estimating approximate spectral types.

Methane and carbon dioxide emissions from 40 lakes along a north–south latitudinal transect in Alaska

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sepulveda-Jauregui, A.; Walter Anthony, K. M.; Martinez-Cruz, K.

Uncertainties in the magnitude and seasonality of various gas emission modes, particularly among different lake types, limit our ability to estimate methane (CH 4) and carbon dioxide (CO 2) emissions from northern lakes. Here we assessed the relationship between CH 4 and CO 2 emission modes in 40 lakes along a latitudinal transect in Alaska to physicochemical limnology and geographic characteristics, including permafrost soil type surrounding lakes. Emission modes included Direct Ebullition, Diffusion, Storage flux, and a newly identified Ice-Bubble Storage (IBS) flux. We found that all lakes were net sources of atmospheric CH 4 and CO 2, but themore » climate warming impact of lake CH 4 emissions was two times higher than that of CO 2. Ebullition and Diffusion were the dominant modes of CH 4 and CO 2 emissions respectively. IBS, ~ 10% of total annual CH 4 emissions, is the release to the atmosphere of seasonally ice-trapped bubbles when lake ice confining bubbles begins to melt in spring. IBS, which has not been explicitly accounted for in regional studies, increased the estimate of springtime emissions from our study lakes by 320%. Geographically, CH 4 emissions from stratified, dystrophic interior Alaska thermokarst (thaw) lakes formed in icy, organic-rich yedoma permafrost soils were 6-fold higher than from non-yedoma lakes throughout the rest of Alaska. Total CH 4 emission was correlated with concentrations of phosphate and total nitrogen in lake water, Secchi depth and lake area, with yedoma lakes having higher nutrient concentrations, shallower Secchi depth, and smaller lake areas. Our findings suggest that permafrost type plays important roles in determining CH 4 emissions from lakes by both supplying organic matter to methanogenesis directly from thawing permafrost and by enhancing nutrient availability to primary production, which can also fuel decomposition and methanogenesis.« less

Methane and carbon dioxide emissions from 40 lakes along a north–south latitudinal transect in Alaska

DOE PAGES

Sepulveda-Jauregui, A.; Walter Anthony, K. M.; Martinez-Cruz, K.; ...

2014-09-12

Uncertainties in the magnitude and seasonality of various gas emission modes, particularly among different lake types, limit our ability to estimate methane (CH 4) and carbon dioxide (CO 2) emissions from northern lakes. Here we assessed the relationship between CH 4 and CO 2 emission modes in 40 lakes along a latitudinal transect in Alaska to physicochemical limnology and geographic characteristics, including permafrost soil type surrounding lakes. Emission modes included Direct Ebullition, Diffusion, Storage flux, and a newly identified Ice-Bubble Storage (IBS) flux. We found that all lakes were net sources of atmospheric CH 4 and CO 2, but themore » climate warming impact of lake CH 4 emissions was two times higher than that of CO 2. Ebullition and Diffusion were the dominant modes of CH 4 and CO 2 emissions respectively. IBS, ~ 10% of total annual CH 4 emissions, is the release to the atmosphere of seasonally ice-trapped bubbles when lake ice confining bubbles begins to melt in spring. IBS, which has not been explicitly accounted for in regional studies, increased the estimate of springtime emissions from our study lakes by 320%. Geographically, CH 4 emissions from stratified, dystrophic interior Alaska thermokarst (thaw) lakes formed in icy, organic-rich yedoma permafrost soils were 6-fold higher than from non-yedoma lakes throughout the rest of Alaska. Total CH 4 emission was correlated with concentrations of phosphate and total nitrogen in lake water, Secchi depth and lake area, with yedoma lakes having higher nutrient concentrations, shallower Secchi depth, and smaller lake areas. Our findings suggest that permafrost type plays important roles in determining CH 4 emissions from lakes by both supplying organic matter to methanogenesis directly from thawing permafrost and by enhancing nutrient availability to primary production, which can also fuel decomposition and methanogenesis.« less

Eddy Covariance Measurements of Methane Flux at Remote Sites with New Low-Power Lightweight Fast Gas Analyzer

NASA Astrophysics Data System (ADS)

Xu, Liukang; Burba, George; Schedlbauer, Jessica; Zona, Donatella; McDermitt, Dayle K.; Anderson, Tyler; Oberbauer, Steven; Oechel, Walter; Komissarov, Anatoly; Riensche, Brad

2010-05-01

Majority of natural methane production happens at remote unpopulated areas in ecosystems with little or no infrastructure or easily available grid power, such as arctic and boreal wetlands, tropical mangroves, etc. Present approaches for direct measurements of CH4 fluxes rely on fast closed-path analyzers, which have to work under significantly reduced pressures, and require powerful pumps and grid power. Power and labor demands may be reasons why CH4 flux is often measured at locations with good infrastructure and grid power, and not with high CH4 production. An instrument was developed to allow Eddy Covariance measurements of CH4 flux with power consumption 30-150 times below presently available technologies. This instrument, LI-7700, uses <10W of power, and can easily be run on solar panel, or with small portable generator, while present technologies require 300-1500 Watts of the grid power. The proposed extremely low-power technology would allows placing methane Eddy Covariance stations in the middle of the source (wetland, rice paddy, forest, etc.) in the absence of the grid power. This could significantly expand the Eddy Covariance CH4 flux measurements coverage, and possibly, significantly improve the budget estimates of world CH4 emissions and budget. Various prototypes of the LI-7700 were field-tested for three seasons at the remote site in middle of Everglades National Park (Florida, USA) using solar panels, at three stationary and several mobile sites during three seasons at remote Arctic wetlands near Barrow (Alaska, USA), in the tropical mangroves near La Paz (Mexico) using portable generator, and in bare agricultural field near Mead (Nebraska, USA) during 2005 through 2010. Latest data on CH4 concentration, co-spectra and fluxes, and latest details of instrumental design are examined in this presentation. Overall, hourly methane fluxes ranged from near-zero at night to about 4 mg m-2 h-1 in midday in arctic tundra. Observed fluxes were within the ranges reported in the literature for a number of wetlands in North America, including the Everglades wetlands. Diurnal patterns were similar to those measured by closed-path sensors. The LI-7700 open-path analyzer is a valuable tool for measuring long-term eddy fluxes of methane due to the good frequency response and undisturbed in-situ sampling. It enables long-term deployment of permanent, portable or mobile CH4 flux stations at remote locations with high CH4 production, because it can be powered by a solar panels or a small generator. Authors appreciate help and support provided by the LI-COR Engineering Team, Barrow Arctic Science Consortium (BASC), and numerous colleagues involved in measurements, logistics, and maintenance of the experimental field sites. This project was supported by the Small Business Innovation Research (SBIR) and Small Business Technology Transfer Program (STTR) program of the Department of Energy (DOE), Grant Number DE-FG02-05ER84283.

Reaction pathways of producing and losing particles in atmospheric pressure methane nanosecond pulsed needle-plane discharge plasma

NASA Astrophysics Data System (ADS)

Zhao, Yuefeng; Wang, Chao; Li, Li; Wang, Lijuan; Pan, Jie

2018-03-01

In this work, a two-dimensional fluid model is built up to numerically investigate the reaction pathways of producing and losing particles in atmospheric pressure methane nanosecond pulsed needle-plane discharge plasma. The calculation results indicate that the electron collisions with CH4 are the key pathways to produce the neutral particles CH2 and CH as well as the charged particles e and CH3+. CH3, H2, H, C2H2, and C2H4 primarily result from the reactions between the neutral particles and CH4. The charge transfer reactions are the significant pathways to produce CH4+, C2H2+, and C2H4+. As to the neutral species CH and H and the charged species CH3+, the reactions between themselves and CH4 contribute to substantial losses of these particles. The ways responsible for losing CH3, H2, C2H2, and C2H4 are CH3 + H → CH4, H2 + CH → CH2 + H, CH4+ + C2H2 → C2H2+ + CH4, and CH4+ + C2H4 → C2H4+ + CH4, respectively. Both electrons and C2H4+ are consumed by the dissociative electron-ion recombination reactions. The essential reaction pathways of losing CH4+ and C2H2+ are the charge transfer reactions.

Additively Manufactured Combustion Devices Components for LOX/Methane Applications

NASA Technical Reports Server (NTRS)

Greene, Sandra Elam; Protz, Christopher; Garcia, Chance; Goodman, Dwight; Baker, Kevin

2016-01-01

Marshall Space Flight Center (MSFC) has designed, fabricated, and hot-fire tested a variety of successful injectors, chambers, and igniters for potential liquid oxygen (LOX) and methane (CH4) systems since 2005. The most recent efforts have focused on components with additive manufacturing (AM) to include unique design features, minimize joints, and reduce final machining efforts. Inconel and copper alloys have been used with AM processes to produce a swirl coaxial injector and multiple methane cooled thrust chambers. The initial chambers included unique thermocouple ports for measuring local coolant channel temperatures along the length of the chamber. Results from hot-fire testing were used to anchor thermal models and generate a regeneratively cooled thruster for a 4,000 lbf LOX/CH4 engine. The completed thruster will be hot-fire tested in the summer of 2016 at MSFC. The thruster design can also be easily scaled and used on a 25,000 lbf engine. To further support the larger engine design, an AM gas generator injector has been designed. Hot-fire testing on this injector is planned for the summer of 2016 at MSFC.

Measurement of the Isotopic Signatures of Water on Mars: Implications for Studying Methane

NASA Technical Reports Server (NTRS)

Novak, R. E.; Mumma, M. J.; Villanueva, G. L.

2010-01-01

The recent discovery of methane on Mars has led to much discussion concerning its origin. On Earth, the isotopic signatures of methane vary with the nature of its production. Specifically, the ratios among 12CH4, 13CH4, and 12CH3D differ for biotic and abiotic origins. On Mars, measuring these ratios would provide insights into the origins of methane and measurements of water isotopologues co-released with methane would assist in testing their chemical relationship. Since 1997, we have been measuring HDO and H2O in Mars atmosphere and comparing their ratio to that in Earth s oceans. We recently incorporated a line-by-line radiative transfer model (LBLRTM) into our analysis. Here, we present a map for [HDO]/[H2O] along the central meridian (1541W) for Ls 501. From these results, we constructed models to determine the observational conditions needed to quantify the isotopic ratios of methane in Mars atmosphere. Current ground-based instruments lack the spectral resolution and sensitivity needed to make these measurements. Measurements of the isotopologues of methane will likely require in situ sampling.

Competitive interactions between methane- and ammonia-oxidizing bacteria modulate carbon and nitrogen cycling in paddy soil

NASA Astrophysics Data System (ADS)

Zheng, Y.; Huang, R.; Wang, B. Z.; Bodelier, P. L. E.; Jia, Z. J.

2014-06-01

Pure culture studies have demonstrated that methanotrophs and ammonia oxidizers can both carry out the oxidation of methane and ammonia. However, the expected interactions resulting from these similarities are poorly understood, especially in complex, natural environments. Using DNA-based stable isotope probing and pyrosequencing of 16S rRNA and functional genes, we report on biogeochemical and molecular evidence for growth stimulation of methanotrophic communities by ammonium fertilization, and that methane modulates nitrogen cycling by competitive inhibition of nitrifying communities in a rice paddy soil. Pairwise comparison between microcosms amended with CH4, CH4+Urea, and Urea indicated that urea fertilization stimulated methane oxidation activity 6-fold during a 19-day incubation period, while ammonia oxidation activity was significantly suppressed in the presence of CH4. Pyrosequencing of the total 16S rRNA genes revealed that urea amendment resulted in rapid growth of Methylosarcina-like MOB, and nitrifying communities appeared to be partially inhibited by methane. High-throughput sequencing of the 13C-labeled DNA further revealed that methane amendment resulted in clear growth of Methylosarcina-related MOB while methane plus urea led to an equal increase in Methylosarcina and Methylobacter-related type Ia MOB, indicating the differential growth requirements of representatives of these genera. An increase in 13C assimilation by microorganisms related to methanol oxidizers clearly indicated carbon transfer from methane oxidation to other soil microbes, which was enhanced by urea addition. The active growth of type Ia methanotrops was significantly stimulated by urea amendment, and the pronounced growth of methanol-oxidizing bacteria occurred in CH4-treated microcosms only upon urea amendment. Methane addition partially inhibited the growth of Nitrosospira and Nitrosomonas in urea-amended microcosms, as well as growth of nitrite-oxidizing bacteria. These results suggest that type I methanotrophs can outcompete type II methane oxidizers in nitrogen-rich environments, rendering the interactions among methane and ammonia oxidizers more complicated than previously appreciated.

Role of regional wetland emissions in atmospheric methane variability

NASA Astrophysics Data System (ADS)

McNorton, J.; Gloor, E.; Wilson, C.; Hayman, G. D.; Gedney, N.; Comyn-Platt, E.; Marthews, T.; Parker, R. J.; Boesch, H.; Chipperfield, M. P.

2016-11-01

Atmospheric methane (CH4) accounts for 20% of the total direct anthropogenic radiative forcing by long-lived greenhouse gases. Surface observations show a pause (1999-2006) followed by a resumption in CH4 growth, which remain largely unexplained. Using a land surface model, we estimate wetland CH4 emissions from 1993 to 2014 and study the regional contributions to changes in atmospheric CH4. Atmospheric model simulations using these emissions, together with other sources, compare well with surface and satellite CH4 data. Modeled global wetland emissions vary by ±3%/yr (σ = 4.8 Tg), mainly due to precipitation-induced changes in wetland area, but the integrated effect makes only a small contribution to the pause in CH4 growth from 1999 to 2006. Increasing temperature, which increases wetland area, drives a long-term trend in wetland CH4 emissions of +0.2%/yr (1999 to 2014). The increased growth post-2006 was partly caused by increased wetland emissions (+3%), mainly from Tropical Asia, Southern Africa, and Australia.

Temperature and hydrology affect methane emissions from Prairie Pothole Wetlands

USGS Publications Warehouse

Bansal, Sheel; Tangen, Brian; Finocchiaro, Raymond

2016-01-01

The Prairie Pothole Region (PPR) in central North America consists of millions of depressional wetlands that each have considerable potential to emit methane (CH4). Changes in temperature and hydrology in the PPR from climate change may affect methane fluxes from these wetlands. To assess the potential effects of changes in climate on methane emissions, we examined the relationships between flux rates and temperature or water depth using six years of bi-weekly flux measurements during the snow-free period from six temporarily ponded and six permanently ponded wetlands in North Dakota, USA. Methane flux rates were among the highest reported for freshwater wetlands, and had considerable spatial and temporal variation. Methane flux rates increased with increasing temperature and water depth, and were especially high when conditions were warmer and wetter than average (163 ± 28 mg CH4 m−2 h−1) compared to warmer and drier (37 ± 7 mg CH4 m−2 h−1). Methane emission rates from permanent wetlands were less sensitive to changes in temperature and water depth compared to temporary wetlands, likely due to higher sulfate concentrations in permanent wetlands. While the predicted increase in temperature with climate change will likely increase methane emission rates from PPR wetlands, drier conditions could moderate these increases.

Evaluating the Classical Versus an Emerging Conceptual Model of Peatland Methane Dynamics

Treesearch

Wendy H. Yang; Gavin McNicol; Yit Arn Teh; Katerina Estera-Molina; Tana E. Wood; Whendee L. Silver

2017-01-01

Methane (CH4) is a potent greenhouse gas that is both produced and consumed in soils by microbially mediated processes sensitive to soil redox. We evaluated the classical conceptual model of peatland CH4 dynamics—in which the water table position determines the vertical distribution of methanogenesis and methanotrophy—...

Measurement of methane fluxes from terrestrial landscapes using static, non-steady state enclosures. Chapter 12

Treesearch

Peter Weishampel; Randall Kolka

2008-01-01

Wetlands are a dominant natural source of atmospheric methane (CH4), a potent greenhouse gas whose concentration in the atmosphere has doubled over the past 150 years. Evaluating the impacts of CH4 emissions on global climate and developing policies to mitigate those impacts requires a quantifiable and predictive...

Effects of experimental warming and elevated CO2 on surface methane and CO­2 fluxes from a boreal black spruce peatland

NASA Astrophysics Data System (ADS)

Gill, A. L.; Finzi, A.; Giasson, M. A.

2015-12-01

High latitude peatlands represent a major terrestrial carbon store sensitive to climate change, as well as a globally significant methane source. While elevated atmospheric carbon dioxide concentrations and warming temperatures may increase peat respiration and C losses to the atmosphere, reductions in peatland water tables associated with increased growing season evapotranspiration may alter the nature of trace gas emission and increase peat C losses as CO2 relative to methane (CH4). As CH4 is a greenhouse gas with twenty times the warming potential of CO2, it is critical to understand how surface fluxes of CO2 and CH4 will be influenced by factors associated with global climate change. We used automated soil respiration chambers to assess the influence of elevated atmospheric CO2 and whole ecosystem warming on peatland CH4 and CO2 fluxes at the SPRUCE (Spruce and Peatland Responses Under Climatic and Environmental Change) Experiment in northern Minnesota. Belowground warming treatments were initiated in July 2014 and whole ecosystem warming and elevated CO2 treatments began in August 2015. Here we report soil iCO2 and iCH4 flux responses to the first year of belowground warming and the first two months of whole ecosystem manipulation. We also leverage the spatial and temporal density of measurements across the twenty autochambers to assess how physical (i.e., plant species composition, microtopography) and environmental (i.e., peat temperature, water table position, oxygen availability) factors influence observed rates of CH4 and CO2 loss. We find that methane fluxes increased significantly across warming treatments following the first year of belowground warming, while belowground warming alone had little influence on soil CO2 fluxes. Peat microtopography strongly influenced trace gas emission rates, with higher CH4 fluxes in hollow locations and higher CO2 fluxes in hummock locations. While there was no difference in the isotopic composition of the methane fluxes between hollow and hummock locations, δ13CH4 was more depleted in the early and late growing season, indicating a transition from hydrogenotrophic to acetoclastic methanogenesis during periods of high photosynthetic input.

Methane adsorption capacity on graphene derived from glucose and ferric chloride

NASA Astrophysics Data System (ADS)

Ismail, M. S.; Yusof, N.; Yusop, M. Zamri; Ismail, A. F.; Nasri, N. S.; Othman, F. E. Che

2018-05-01

This study examines the methane adsorption capacity using graphene derived from glucose and ferric chloride (FeCl3). The graphene was prepared via simple method by dissolution of glucose and FeCl3 in water, vaporization of water in oven, and calcination process in quartz furnace. Graphene was successfully produced with impregnation ratio of glucose and FeCl3 at 1:1 and calcination temperature of 650 °C. The prepared graphene subsequently underwent a volumetric adsorption setup, to measure the adsorption capacity of methane (CH4). The highest CH4 adsorption capacity obtained was 6.37 mmol/g at 3.5 bar and 298 K for 40 minutes. These result shows that the prepared graphene displayed good adsorption characteristic for CH4.

Distribution, abundance and carbon isotopic composition of gaseous hydrocarbons in Big Soda Lake, Nevada: An alkaline, meromictic lake

USGS Publications Warehouse

Oremland, R.S.; Des Marais, D.J.

1983-01-01

Distribution and isotopic composition (??13C) of low molecular weight hydrocarbon gases were studied in Big Soda Lake (depth = 64 m), an alkaline, meromictic lake with permanently anoxic bottom waters. Methane increased with depth in the anoxic mixolimnion (depth = 20-35 m), reached uniform concentrations (55 ??M/l) in the monimolimnion (35-64 m) and again increased with depth in monimolimnion bottom sediments (>400 ??M/kg below 1 m sub-bottom depth). The ??13C[CH4] values in bottom sediment below 1 m sub-bottom depth (<-70 per mil) increased with vertical distance up the core (??13C[CH4] = -55 per mil at sediment surface). Monimolimnion ??13C[CH4] values (-55 to -61 per mil) were greater than most ??13C[CH4] values found in the anoxic mixolimnion (92% of samples had ??13C[CH4] values between -20 and -48 per mil). No significant concentrations of ethylene or propylene were found in the lake. However ethane, propane, isobutane and n-butane concentrations all increased with water column depth, with respective maximum concentrations of 260, 80, 23 and 22 nM/l encountered between 50-60 m depth. Concentrations of ethane, propane and butanes decreased with depth in the bottom sediments. Ratios of CH4 [C2H6 + C3H8] were high (250-620) in the anoxic mixolimnion, decreased to ~161 in the monimolimnion and increased with depth in the sediment to values as high as 1736. We concluded that methane has a biogenic origin in both the sediments and the anoxic water column and that C2-C4 alkanes have biogenic origins in the monimolimnion water and shallow sediments. The changes observed in ??13C[CH4] and CH4 (C2H6 + C3H8) with depth in the water column and sediments are probably caused by bacteria] processes. These might include anaerobic methane oxidation and different rates of methanogenesis and C2 to C4 alkane production by microorganisms. ?? 1983.

Sound management may sequester methane in grazed rangeland ecosystems

PubMed Central

Wang, Chengjie; Han, Guodong; Wang, Shiping; Zhai, Xiajie; Brown, Joel; Havstad, Kris M.; Ma, Xiuzhi; Wilkes, Andreas; Zhao, Mengli; Tang, Shiming; Zhou, Pei; Jiang, Yuanyuan; Lu, Tingting; Wang, Zhongwu; Li, Zhiguo

2014-01-01

Considering their contribution to global warming, the sources and sinks of methane (CH4) should be accounted when undertaking a greenhouse gas inventory for grazed rangeland ecosystems. The aim of this study was to evaluate the mitigation potential of current ecological management programs implemented in the main rangeland regions of China. The influences of rangeland improvement, utilization and livestock production on CH4 flux/emission were assessed to estimate CH4 reduction potential. Results indicate that the grazed rangeland ecosystem is currently a net source of atmospheric CH4. However, there is potential to convert the ecosystem to a net sink by improving management practices. Previous assessments of capacity for CH4 uptake in grazed rangeland ecosystems have not considered improved livestock management practices and thus underestimated potential for CH4 uptake. Optimal fertilization, rest and light grazing, and intensification of livestock management contribute mitigation potential significantly. PMID:24658176

Sound management may sequester methane in grazed rangeland ecosystems.

PubMed

Wang, Chengjie; Han, Guodong; Wang, Shiping; Zhai, Xiajie; Brown, Joel; Havstad, Kris M; Ma, Xiuzhi; Wilkes, Andreas; Zhao, Mengli; Tang, Shiming; Zhou, Pei; Jiang, Yuanyuan; Lu, Tingting; Wang, Zhongwu; Li, Zhiguo

2014-03-24

Considering their contribution to global warming, the sources and sinks of methane (CH4) should be accounted when undertaking a greenhouse gas inventory for grazed rangeland ecosystems. The aim of this study was to evaluate the mitigation potential of current ecological management programs implemented in the main rangeland regions of China. The influences of rangeland improvement, utilization and livestock production on CH4 flux/emission were assessed to estimate CH4 reduction potential. Results indicate that the grazed rangeland ecosystem is currently a net source of atmospheric CH4. However, there is potential to convert the ecosystem to a net sink by improving management practices. Previous assessments of capacity for CH4 uptake in grazed rangeland ecosystems have not considered improved livestock management practices and thus underestimated potential for CH4 uptake. Optimal fertilization, rest and light grazing, and intensification of livestock management contribute mitigation potential significantly.

A 21st-century shift from fossil-fuel to biogenic methane emissions indicated by ¹³CH₄.

PubMed

Schaefer, Hinrich; Mikaloff Fletcher, Sara E; Veidt, Cordelia; Lassey, Keith R; Brailsford, Gordon W; Bromley, Tony M; Dlugokencky, Edward J; Michel, Sylvia E; Miller, John B; Levin, Ingeborg; Lowe, Dave C; Martin, Ross J; Vaughn, Bruce H; White, James W C

2016-04-01

Between 1999 and 2006, a plateau interrupted the otherwise continuous increase of atmospheric methane concentration [CH4] since preindustrial times. Causes could be sink variability or a temporary reduction in industrial or climate-sensitive sources. We reconstructed the global history of [CH4] and its stable carbon isotopes from ice cores, archived air, and a global network of monitoring stations. A box-model analysis suggests that diminishing thermogenic emissions, probably from the fossil-fuel industry, and/or variations in the hydroxyl CH4 sink caused the [CH4] plateau. Thermogenic emissions did not resume to cause the renewed [CH4] rise after 2006, which contradicts emission inventories. Post-2006 source increases are predominantly biogenic, outside the Arctic, and arguably more consistent with agriculture than wetlands. If so, mitigating CH4 emissions must be balanced with the need for food production. Copyright © 2016, American Association for the Advancement of Science.

Illuminating Geochemical Controls of Methane Oxidation Along a Gradient of Permafrost Thaw

NASA Astrophysics Data System (ADS)

Perryman, C. R.; Kashi, N.; McCalley, C. K.; Malhotra, A.; Giesler, R.; Varner, R.

2017-12-01

Increases in annual mean temperature in the subarctic have accelerated the thaw of organic-rich permafrost peatlands, exacerbating methane (CH4) production from microbial decomposition of peat deposits and subsequent CH4 emissions. Methanotrophic bacteria may oxidize/consume upwards of 90% of produced CH4 in some settings, pending substrate availability and environmental conditions. Redox chemistry may also control the rate of CH4 oxidation in thawing permafrost areas, particularly redox potential (Eh) and the availability of oxygen (O2) and other terminal electron receptors. We investigated potential CH4 oxidation rates across a permafrost thaw gradient in Stordalen Mire (68°21'N,18°49'E) near Abisko, Sweden. Methane oxidation rates for sites from thawing and collapsed palsa, semi-wet Sphagnum, and open-water sedge sites were determined through laboratory incubations. Peat cores were extracted from two depths at each site and incubated at in situ temperatures and CH4 concentrations. Headspace samples were collected over a 48-hour period and analyzed for CH4 concentration using flame ionization detection gas chromatography (GC-FID). Dissolved O2, Eh, and dissolved CH4 were measured in sites with porewater. Oxidation rates ranged from <0.1 to 19 μg of CH4 per gram of dry biomass per day. Eh remained positive (41.6 to 316.8 mV) with available dissolved O2 (0.3 - 5.2 mg/L) in all measurement locations down to 20cm, indicating in situ aerobic CH4 oxidation is viable across these environments. Potential CH4 oxidation rates increased with increasing dissolved CH4 concentration. Highest potential CH4 oxidation rates were found in open-water sedge sites. Eh and dissolved O2 were lowest at these sites, suggesting that methanotrophs with low-O2 demand may populate sedge areas. Furthermore, potential CH4 oxidation rates were higher at depth than at the surface in thawing palsa, suggesting CH4 oxidation may mitigate CH4 production triggered by warming in these actively thawing environments. Forthcoming elemental analyses of peat and pore water will further elucidate trends and geochemical controls of CH4 oxidation rates in thawing permafrost areas.

Continuous Measurement of Methane Ebullition Flux from a Northern Peatland using a Fast Methane Analyzer

NASA Astrophysics Data System (ADS)

Zhongjie, Y.; Schafer, K. V.; Slater, L. D.; Varner, R. K.; Amante, J.; Comas, X.; Reeve, A. S.; Alcivar, W.; Gonzalez, D.

2012-12-01

Northern peatlands are an important source of methane (CH4) release to the atmosphere, estimated at between 20 and 50 Tg/yr. Recent work on CH4 emissions from peatlands has demonstrated that ebullition can be a more important emission pathway than previously assumed. However, accurate quantification of the atmospheric CH4 burden due to ebullition is still very limited because ebullition exhibits high spatiotemporal variability such that sudden episodic events are difficult to capture and quantify with existing experimental methods. We have initiated a novel measurement program to better quantify the spatiotemporal variability in CH4 flux in peatlands, and to examine potential effects of vegetation and environmental factors, e.g. atmospheric pressure, water table, etc on these releases. A flow-through system was designed, consisting of a closed static chamber and a fast methane analyzer (FMA) (LI-COR model 7700) that has been employed at both the field and laboratory scale. The CH4 concentration in the air flowing through the chamber is continuously measured by the analyzer and used to reconstruct continuous CH4 emission fluxes. The high sampling rate of the FMA makes it sensitive to both ebullition and diffusion of gaseous CH4, capturing short duration, episodic ebullition fluxes. Non-steady static chamber measurements were also conducted to cross-validate the continuous measurements. Results acquired during summer 2011 show that episodic ebullition occurred more frequently at the pool site where previous studies indicate extensive wood layers at depth and the vegetation was a mix of Sphagnum and wooded heath. During a 3 day period of continuous measurements captured the passage of a tropical storm Irene, where short term episodic releases of CH4, ranging from 113 mg CH4/m2/d to 202 mg CH4/m2/d, were observed at the time of lowest atmospheric pressure, providing new evidence that atmospheric pressure is an important factor to controlling CH4 ebullition from peatlands. While traditional techniques, e.g. static chamber measurement can only occasionally detect the occurrence of ebullition, the continuous measurement by using a flow-through system is able to resolve spatiotemporal complexity of episodic CH4 ebullition events. These continuous CH4 measurements provide new insights into the timing of CH4 ebullition from peatlands to the atmosphere as climate changes and the role of environmental variables in regulating these CH4 releases.

Methane and hydrogen sulfide emissions in UASB reactors treating domestic wastewater.

PubMed

Souza, C L; Chernicharo, C A L; Melo, G C B

2012-01-01

The release of CH(4) and H(2)S in UASB reactors was evaluated with the aim to quantify the emissions from the liquid surfaces (three-phase separator and settler compartment) and also from the reactor's discharge hydraulic structures. The studies were carried out in two pilot- (360 L) and one demo-scale (14 m(3)) UASB reactors treating domestic wastewater. As expected, the release rates were much higher across the gas/liquid interfaces of the three-phase separators (5.4-9.7 kg CH(4) m(-2) d(-1) and 23.0-35.8 g S m(-2) d(-1)) as compared with the quiescent settler surfaces (11.0-17.8 g CH(4) m(-2) d(-1) and 0.21 to 0.37 g S m(-2) d(-1)). The decrease of dissolved methane and dissolved hydrogen sulfide was very large in the discharging hydraulic structures very close to the reactor (>60 and >80%, respectively), largely due to the loss to the atmosphere, indicating that the concentration of these compounds will probably fall to values close to zero in the near downstream structures. The emission factors due to the release of dissolved methane in the discharge structure amounted to around 0.040 g CH(4) g COD(infl)(-1) and 0.060 g CH(4) g COD(rem)(-1), representing around 60% of the methane collected in the three-phase separator.

Infrared spectroscopy of water clusters isolated in methane matrices: Effects of isotope substitution and annealing

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yamakawa, Koichiro, E-mail: koichiro.yamakawa@gakushuin.ac.jp; Ehara, Namika; Ozawa, Nozomi

2016-07-15

Using infrared-active solvents of CH{sub 4} and CD{sub 4} for matrix isolation, we measured infrared spectra of H{sub 2}O and D{sub 2}O clusters at 7 K. The solute-concentration dependence of the spectrum of H{sub 2}O clusters in a CH{sub 4} matrix was investigated and was used for the peak assignment. Annealing procedures were found to promote the size growth of water clusters in methane matrices for all the combinations of (H{sub 2}O, CH{sub 4}), (H{sub 2}O, CD{sub 4}), (D{sub 2}O, CH{sub 4}), and (D{sub 2}O, CD{sub 4}). We also monitored the ν{sub 3} absorption due to methane to find themore » annealing-induced structural change only of solid CH{sub 4}. The matrix effects on the vibrations of the clusters are discussed on the basis of “T{sub c} plots”, where their frequencies are plotted as a function of the square root of the matrix critical temperature, T{sub c}. The obtained plots assure the validity of the assignment of the cluster peaks.« less

Methane evasion and oxidation in the Big Cypress National Preserve—a low relief carbonate wetland

NASA Astrophysics Data System (ADS)

Ward, N. D.; Bianchi, T. S.; Cohen, M. J.; Martin, J. B.; Quintero, C.; Brown, A.; Osborne, T.; Sawakuchi, H. O.

2016-12-01

The Big Cypress National Preserve is a low relief carbonate wetland characterized by unique basin patterning known as "cypress domes." Here we examine the concentration and stable isotopic composition of methane in pore waters, surface waters, and bubbles from the sediment across horizontal gradients in four domes during three sampling campaigns. The proportion of methane oxidized in surface waters was estimated based on isotopic differences between surface water and pore waters/bubbles. Rates of methane evasion from surface waters, soils, and cypress knees to the atmosphere were also measured. Surface water CH4 concentrations ranged from 170 to 4,533 ppm with the highest levels generally being observed during wet periods. Pore water CH4 concentrations ranged from 748 to 75,213 ppm. The concentration of methane in bubbles ranged from 6.5 to 71%. The stable isotopic composition of CH4 ranged from -69.2 to -43.8‰ for all samples and was generally more enriched in surface waters compared to bubbles and porewaters, particularly in the two domes that were persistently inundated throughout the year. Based on these isotopic values, the average percentage of surface water CH4 that was oxidized was 37 ± 16% (maximum of 67%) and 19 ± 4% (maximum of 47%) in the two domes that are persistently inundated versus the two domes that are not inundated during the dry season, respectively. The average rate of CH4 evasion was 3.6 ± 1.6 mmol m-2 d-1 via diffusion, 7.6 ± 4.7 mmol m-2 d-1 via ebullition, 10.9 ± 11.4 mmol m-2 d-1­ from soil surfaces, and 34.3 ± 27.4 mmol m-2 d-1 from cypress knees. These results indicate that CH4 is produced in great quantities in inundated sediments, particularly in the center of the cypress domes. Diffusive fluxes from surface waters are suppressed by microbial oxidation in the water column, whereas ebullition from sediments and evasion through cypress knees, and likely other vascular vegetation, are the primary pathways for CH4 outgassing.

Observations of atmospheric methane and its stable isotope ratio (δ13C) over the Arctic seas from ship cruises in the summer and autumn of 2015

NASA Astrophysics Data System (ADS)

Skorokhod, Andrey; Belikov, Igor; Pankratova, Natalia; Novigatsky, Alexander; Thompson, Rona

2016-04-01

Atmospheric methane (CH4) is the second most important long-lived greenhouse gas. The Arctic has significant sources of CH4, such as from wetlands and possibly also from methane hydrates, which may act as a positive feedback on the climate system. Despite significant efforts in establishing a network of ground-based CH4 observations in the Arctic zone, there is still a lack of measurements over the Arctic Ocean and sub-polar seas. From 21 July to 9 October 2015, concentrations of CH4 and CO2, as well as of the 13C:12C isotopic ratio in CH4, i.e., δ13C, were measured in the marine boundary layer from aboard the Research Vessel "Akademik Mstislav Keldysh" by the Shirshov Institute of Oceanology. Measurements were made using a Cavity Ring Down Spectroscopy instrument from Picarro™ (model G2132-i). The cruises covered a vast area including the North Atlantic up to 70°N, the Baltic, North, Norwegian, Greenland, Barents, White, Kara and Laptev Seas. To the best of our knowledge, these are the first measurements of their type made in these regions. Concentrations of CH4 typically had low variations (in the range of a few ppb) in the open sea but relatively large variations (of the order of 100 ppb) were recorded near and during stops in ports. High variability of atmospheric CH4 was also registered near the delta of the Lena River in the Laptev Sea, which has been suggested to be a large CH4 reservoir and where bubbles rising through the water column have been observed. The obtained set of δ13CCH4 is characterized by significant range of the measured values varying from open Atlantic to polluted regions near large sea ports. The Keeling plot analyses were implemented to study possible CH4 sources according to its isotopic signature. Footprint analyses are presented for the shipboard observations, as well as comparisons to simulated CH4 concentrations and δ13C using the Lagrangian transport model, FLEXPART. This work has been carried-out with the financial support of RFBR (Project #14-05-93089) and RSF (Project #14-47-00049).

40 CFR 86.1801-12 - Applicability.

Code of Federal Regulations, 2012 CFR

2012-07-01

... standards in this subpart, including carbon dioxide (CO2), nitrous oxide (N2O), and methane (CH4). (j... the manufacturer's expansion in vehicle production, the manufacturer shall comply with the emission...

Constraints on oceanic methane emissions west of Svalbard from atmospheric in situ measurements and Lagrangian transport modeling.

PubMed

Pisso, I; Myhre, C Lund; Platt, S M; Eckhardt, S; Hermansen, O; Schmidbauer, N; Mienert, J; Vadakkepuliyambatta, S; Bauguitte, S; Pitt, J; Allen, G; Bower, K N; O'Shea, S; Gallagher, M W; Percival, C J; Pyle, J; Cain, M; Stohl, A

2016-12-16

Methane stored in seabed reservoirs such as methane hydrates can reach the atmosphere in the form of bubbles or dissolved in water. Hydrates could destabilize with rising temperature further increasing greenhouse gas emissions in a warming climate. To assess the impact of oceanic emissions from the area west of Svalbard, where methane hydrates are abundant, we used measurements collected with a research aircraft (Facility for Airborne Atmospheric Measurements) and a ship (Helmer Hansen) during the Summer 2014 and for Zeppelin Observatory for the full year. We present a model-supported analysis of the atmospheric CH 4 mixing ratios measured by the different platforms. To address uncertainty about where CH 4 emissions actually occur, we explored three scenarios: areas with known seeps, a hydrate stability model, and an ocean depth criterion. We then used a budget analysis and a Lagrangian particle dispersion model to compare measurements taken upwind and downwind of the potential CH 4 emission areas. We found small differences between the CH 4 mixing ratios measured upwind and downwind of the potential emission areas during the campaign. By taking into account measurement and sampling uncertainties and by determining the sensitivity of the measured mixing ratios to potential oceanic emissions, we provide upper limits for the CH 4 fluxes. The CH 4 flux during the campaign was small, with an upper limit of 2.5 nmol m -2  s -1 in the stability model scenario. The Zeppelin Observatory data for 2014 suggest CH 4 fluxes from the Svalbard continental platform below 0.2 Tg yr -1 . All estimates are in the lower range of values previously reported.

Constraints on oceanic methane emissions west of Svalbard from atmospheric in situ measurements and Lagrangian transport modeling

PubMed Central

Myhre, C. Lund; Platt, S. M.; Eckhardt, S.; Hermansen, O.; Schmidbauer, N.; Mienert, J.; Vadakkepuliyambatta, S.; Bauguitte, S.; Pitt, J.; Allen, G.; Bower, K. N.; O'Shea, S.; Gallagher, M. W.; Percival, C. J.; Pyle, J.; Cain, M.; Stohl, A.

2016-01-01

Abstract Methane stored in seabed reservoirs such as methane hydrates can reach the atmosphere in the form of bubbles or dissolved in water. Hydrates could destabilize with rising temperature further increasing greenhouse gas emissions in a warming climate. To assess the impact of oceanic emissions from the area west of Svalbard, where methane hydrates are abundant, we used measurements collected with a research aircraft (Facility for Airborne Atmospheric Measurements) and a ship (Helmer Hansen) during the Summer 2014 and for Zeppelin Observatory for the full year. We present a model‐supported analysis of the atmospheric CH4 mixing ratios measured by the different platforms. To address uncertainty about where CH4 emissions actually occur, we explored three scenarios: areas with known seeps, a hydrate stability model, and an ocean depth criterion. We then used a budget analysis and a Lagrangian particle dispersion model to compare measurements taken upwind and downwind of the potential CH4 emission areas. We found small differences between the CH4 mixing ratios measured upwind and downwind of the potential emission areas during the campaign. By taking into account measurement and sampling uncertainties and by determining the sensitivity of the measured mixing ratios to potential oceanic emissions, we provide upper limits for the CH4 fluxes. The CH4 flux during the campaign was small, with an upper limit of 2.5 nmol m−2 s−1 in the stability model scenario. The Zeppelin Observatory data for 2014 suggest CH4 fluxes from the Svalbard continental platform below 0.2 Tg yr−1. All estimates are in the lower range of values previously reported. PMID:28261536

Constraints on oceanic methane emissions west of Svalbard from atmospheric in situ measurements and Lagrangian transport modeling

NASA Astrophysics Data System (ADS)

Pisso, I.; Myhre, C. Lund; Platt, S. M.; Eckhardt, S.; Hermansen, O.; Schmidbauer, N.; Mienert, J.; Vadakkepuliyambatta, S.; Bauguitte, S.; Pitt, J.; Allen, G.; Bower, K. N.; O'Shea, S.; Gallagher, M. W.; Percival, C. J.; Pyle, J.; Cain, M.; Stohl, A.

2016-12-01

Methane stored in seabed reservoirs such as methane hydrates can reach the atmosphere in the form of bubbles or dissolved in water. Hydrates could destabilize with rising temperature further increasing greenhouse gas emissions in a warming climate. To assess the impact of oceanic emissions from the area west of Svalbard, where methane hydrates are abundant, we used measurements collected with a research aircraft (Facility for Airborne Atmospheric Measurements) and a ship (Helmer Hansen) during the Summer 2014 and for Zeppelin Observatory for the full year. We present a model-supported analysis of the atmospheric CH4 mixing ratios measured by the different platforms. To address uncertainty about where CH4 emissions actually occur, we explored three scenarios: areas with known seeps, a hydrate stability model, and an ocean depth criterion. We then used a budget analysis and a Lagrangian particle dispersion model to compare measurements taken upwind and downwind of the potential CH4 emission areas. We found small differences between the CH4 mixing ratios measured upwind and downwind of the potential emission areas during the campaign. By taking into account measurement and sampling uncertainties and by determining the sensitivity of the measured mixing ratios to potential oceanic emissions, we provide upper limits for the CH4 fluxes. The CH4 flux during the campaign was small, with an upper limit of 2.5 nmol m-2 s-1 in the stability model scenario. The Zeppelin Observatory data for 2014 suggest CH4 fluxes from the Svalbard continental platform below 0.2 Tg yr-1. All estimates are in the lower range of values previously reported.

Inversion Estimate of California Methane Emissions Using a Bayesian Inverse Model with Multi-Tower Greenhouse Gas Monitoring Network and Aircraft Measurements

NASA Astrophysics Data System (ADS)

Cui, Y.; Falk, M.; Chen, Y.; Herner, J.; Croes, B. E.; Vijayan, A.

2017-12-01

Methane (CH4) is an important short-lived climate pollutant (SLCP), and the second most important greenhouse gas (GHG) in California which accounts for 9% of the statewide GHG emissions inventory. Over the years, California has enacted several ambitious climate change mitigation goals, including the California Global Warming Solutions Act of 2006 which requires ARB to reduce statewide GHG emissions to 1990 emission level by 2020, as well as Assembly Bill 1383 which requires implementation of a climate mitigation program to reduce statewide methane emissions by 40% below the 2013 levels. In order to meet these requirements, ARB has proposed a comprehensive SLCP Strategy with goals to reduce oil and gas related emissions and capture methane emissions from dairy operations and organic waste. Achieving these goals will require accurate understanding of the sources of CH4 emissions. Since direct monitoring of CH4 emission sources in large spatial and temporal scales is challenging and resource intensive, we developed a complex inverse technique combined with atmospheric three-dimensional (3D) transport model and atmospheric observations of CH4 concentrations from a regional tower network and aircraft measurements, to gain insights into emission sources in California. In this study, develop a comprehensive inversion estimate using available aircraft measurements from CalNex airborne campaigns (May-June 2010) and three years of hourly continuous measurements from the ARB Statewide GHG Monitoring Network (2014-2016). The inversion analysis is conducted using two independent 3D Lagrangian models (WRF-STILT and WRF-FLEXPART), with a variety of bottom-up prior inputs from national and regional inventories, as well as two different probability density functions (Gaussian and Lognormal). Altogether, our analysis provides a detailed picture of the spatially resolved CH4 emission sources and their temporal variation over a multi-year period.

Temperature and Mechanisms of Methane Transport in Trees

NASA Astrophysics Data System (ADS)

Kutschera, E.; Khalil, A. K.; Rice, A. L.; Rosenstiel, T. N.; Butenhoff, C. L.

2012-12-01

The mechanisms of methane (CH4) transport through trees are still not well understood. Previous work has established that transport mechanisms likely differ from rice and emergent aquatic plants. Establishing the role of trees in overall plant CH4 emissions requires a thorough understanding of tree transport. Using stable isotope measurements of CH4 assists in elucidating these transport mechanisms. Although it has been shown that CH4 is transported through the stems of trees, emission from leaves by transpiration has not been ruled out. The effect of temperature on these mechanisms is important to the prediction of changes in CH4 emissions from the biosphere in altered global climates. The effect of temperature on methane (CH4) emitted from black cottonwood (Populus trichocarpa) trees has been measured. Trees were grown hydroponically under greenhouse conditions. After several months of growth, CH4 canopy flux was measured over three weeks. Temperatures were altered from 22oC the first week to 25oC the second week and to 18oC the final week. CH4 flux increased with temperature, where the difference in flux between the coolest and warmest week was statistically significant. A Q10 for CH4 flux from trees was calculated to be 2.7. Stable carbon isotope measurements of emitted CH4 were enriched at the warmest temperature compared to the coolest temperature, although all measurements were depleted with respect to the isotopic composition of root water CH4. This data not only gives insight into the temperature effects on CH4 flux from trees, but the mechanisms of CH4 flux themselves. This research was supported in part by the Office of Science (BER), U. S. Department of Energy, Grant No. DE-FG02-08ER64515, and through NASA / Oregon Space Grant Consortium, grants NNG05GJ85H and NNX10AK68H.

Recent Advances in Measurement and Dietary Mitigation of Enteric Methane Emissions in Ruminants

PubMed Central

Patra, Amlan K.

2016-01-01

Methane (CH4) emission, which is mainly produced during normal fermentation of feeds by the rumen microorganisms, represents a major contributor to the greenhouse gas (GHG) emissions. Several enteric CH4 mitigation technologies have been explored recently. A number of new techniques have also been developed and existing techniques have been improved in order to evaluate CH4 mitigation technologies and prepare an inventory of GHG emissions precisely. The aim of this review is to discuss different CH4 measuring and mitigation technologies, which have been recently developed. Respiration chamber technique is still considered as a gold standard technique due to its greater precision and reproducibility in CH4 measurements. With the adoption of recent recommendations for improving the technique, the SF6 method can be used with a high level of precision similar to the chamber technique. Short-term measurement techniques of CH4 measurements generally invite considerable within- and between-animal variations. Among the short-term measuring techniques, Greenfeed and methane hood systems are likely more suitable for evaluation of CH4 mitigation studies, if measurements could be obtained at different times of the day relative to the diurnal cycle of the CH4 production. Carbon dioxide and CH4 ratio, sniffer, and other short-term breath analysis techniques are more suitable for on farm screening of large number of animals to generate the data of low CH4-producing animals for genetic selection purposes. Different indirect measuring techniques are also investigated in recent years. Several new dietary CH4 mitigation technologies have been explored, but only a few of them are practical and cost-effective. Future research should be directed toward both the medium- and long-term mitigation strategies, which could be utilized on farms to accomplish substantial reductions of CH4 emissions and to profitably reduce carbon footprint of livestock production systems. This review presents recent developments and critical analysis on different measurements and dietary mitigation of enteric CH4 emissions technologies. PMID:27243027

Recent Advances in Measurement and Dietary Mitigation of Enteric Methane Emissions in Ruminants.

PubMed

Patra, Amlan K

2016-01-01

Methane (CH4) emission, which is mainly produced during normal fermentation of feeds by the rumen microorganisms, represents a major contributor to the greenhouse gas (GHG) emissions. Several enteric CH4 mitigation technologies have been explored recently. A number of new techniques have also been developed and existing techniques have been improved in order to evaluate CH4 mitigation technologies and prepare an inventory of GHG emissions precisely. The aim of this review is to discuss different CH4 measuring and mitigation technologies, which have been recently developed. Respiration chamber technique is still considered as a gold standard technique due to its greater precision and reproducibility in CH4 measurements. With the adoption of recent recommendations for improving the technique, the SF6 method can be used with a high level of precision similar to the chamber technique. Short-term measurement techniques of CH4 measurements generally invite considerable within- and between-animal variations. Among the short-term measuring techniques, Greenfeed and methane hood systems are likely more suitable for evaluation of CH4 mitigation studies, if measurements could be obtained at different times of the day relative to the diurnal cycle of the CH4 production. Carbon dioxide and CH4 ratio, sniffer, and other short-term breath analysis techniques are more suitable for on farm screening of large number of animals to generate the data of low CH4-producing animals for genetic selection purposes. Different indirect measuring techniques are also investigated in recent years. Several new dietary CH4 mitigation technologies have been explored, but only a few of them are practical and cost-effective. Future research should be directed toward both the medium- and long-term mitigation strategies, which could be utilized on farms to accomplish substantial reductions of CH4 emissions and to profitably reduce carbon footprint of livestock production systems. This review presents recent developments and critical analysis on different measurements and dietary mitigation of enteric CH4 emissions technologies.

Challenges in global modeling of wetland extent and wetland methane dynamics

NASA Astrophysics Data System (ADS)

Spahni, R.; Melton, J. R.; Wania, R.; Stocker, B. D.; Zürcher, S.; Joos, F.

2012-12-01

Global wetlands are known to be climate sensitive, and are the largest natural emitters of methane (CH4). Increased wetland CH4 emissions could act as a positive feedback to future warming. Modelling of global wetland extent and wetland CH4 dynamics remains a challenge. Here we present results from the Wetland and Wetland CH4 Inter-comparison of Models Project (WETCHIMP) that investigated our present ability to simulate large scale wetland characteristics (e.g. wetland type, water table, carbon cycling, gas transport, etc.) and corresponding CH4 emissions. Ten models participated, covering the spectrum from simple to relatively complex, including models tailored either for regional or global simulations. The WETCHIMP experiments showed that while models disagree in spatial and temporal patterns of simulated CH4 emissions and wetland areal extent, they all do agree on a strong positive response to increased carbon dioxide concentrations. WETCHIMP made clear that we currently lack observation data sets that are adequate to evaluate model CH4 soil-atmosphere fluxes at a spatial scale comparable to model grid cells. Thus there are substantial parameter and structural uncertainties in large-scale CH4 emission models. As an illustration of the implications of CH4 emissions on climate we show results of the LPX-Bern model, as one of the models participating in WETCHIMP. LPX-Bern is forced with observed 20th century climate and climate output from an ensemble of five comprehensive climate models for a low and a high emission scenario till 2100 AD. In the high emission scenario increased substrate availability for methanogenesis due to a strong stimulation of net primary productivity, and faster soil turnover leads to an amplification of CH4 emissions with the sharpest increase in peatlands (+180% compared to present). Combined with prescribed anthropogenic CH4 emissions, simulated atmospheric CH4 concentration reaches ~4500 ppbv by 2100 AD, about 800 ppbv more than in standard IPCC scenarios. This represents a significant contribution to radiative forcing of global climate.

Cold season emissions dominate the Arctic tundra methane budget

NASA Astrophysics Data System (ADS)

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

2016-01-01

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

Cold season emissions dominate the Arctic tundra methane budget.

PubMed

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

2016-01-05

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

Cold season emissions dominate the Arctic tundra methane budget

PubMed Central

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

2016-01-01

Arctic terrestrial ecosystems are major global sources of methane (CH4); hence, it is important to understand the seasonal and climatic controls on CH4 emissions from these systems. Here, we report year-round CH4 emissions from Alaskan Arctic tundra eddy flux sites and regional fluxes derived from aircraft data. We find that emissions during the cold season (September to May) account for ≥50% of the annual CH4 flux, with the highest emissions from noninundated upland tundra. A major fraction of cold season emissions occur during the “zero curtain” period, when subsurface soil temperatures are poised near 0 °C. The zero curtain may persist longer than the growing season, and CH4 emissions are enhanced when the duration is extended by a deep thawed layer as can occur with thick snow cover. Regional scale fluxes of CH4 derived from aircraft data demonstrate the large spatial extent of late season CH4 emissions. Scaled to the circumpolar Arctic, cold season fluxes from tundra total 12 ± 5 (95% confidence interval) Tg CH4 y−1, ∼25% of global emissions from extratropical wetlands, or ∼6% of total global wetland methane emissions. The dominance of late-season emissions, sensitivity to soil environmental conditions, and importance of dry tundra are not currently simulated in most global climate models. Because Arctic warming disproportionally impacts the cold season, our results suggest that higher cold-season CH4 emissions will result from observed and predicted increases in snow thickness, active layer depth, and soil temperature, representing important positive feedbacks on climate warming. PMID:26699476

Cold season emissions dominate the Arctic tundra methane budget

DOE PAGES

Zona, Donatella; Gioli, Beniamino; Commane, Róisín; ...

2015-12-22

Arctic terrestrial ecosystems are major global sources of methane (CH 4); hence, it is important to understand the seasonal and climatic controls on CH 4 emissions from these systems. Here, we report year-round CH 4 emissions from Alaskan Arctic tundra eddy flux sites and regional fluxes derived from aircraft data. We find that emissions during the cold season (September to May) account for ≥ 50% of the annual CH 4 flux, with the highest emissions from noninundated upland tundra. A major fraction of cold season emissions occur during the “zero curtain” period, when subsurface soil temperatures are poised near 0more » °C. The zero curtain may persist longer than the growing season, and CH 4 emissions are enhanced when the duration is extended by a deep thawed layer as can occur with thick snow cover. Regional scale fluxes of CH 4 derived from aircraft data demonstrate the large spatial extent of late season CH 4 emissions. Scaled to the circumpolar Arctic, cold season fluxes from tundra total 12 ± 5 (95% confidence interval) Tg CH 4 y –1, ~25% of global emissions from extratropical wetlands, or ~6% of total global wetland methane emissions. Here, the dominance of late-season emissions, sensitivity to soil environmental conditions, and importance of dry tundra are not currently simulated in most global climate models. Because Arctic warming disproportionally impacts the cold season, our results suggest that higher cold-season CH 4 emissions will result from observed and predicted increases in snow thickness, active layer depth, and soil temperature, representing important positive feedbacks on climate warming.« less

Methane oxidation in anoxic lake waters

NASA Astrophysics Data System (ADS)

Su, Guangyi; Zopfi, Jakob; Niemann, Helge; Lehmann, Moritz

2017-04-01

Freshwater habitats such as lakes are important sources of methante (CH4), however, most studies in lacustrine environments so far provided evidence for aerobic methane oxidation only, and little is known about the importance of anaerobic oxidation of CH4 (AOM) in anoxic lake waters. In marine environments, sulfate reduction coupled to AOM by archaea has been recognized as important sinks of CH4. More recently, the discorvery of anaerobic methane oxidizing denitrifying bacteria represents a novel and possible alternative AOM pathway, involving reactive nitrogen species (e.g., nitrate and nitrite) as electron acceptors in the absence of oxygen. We investigate anaerobic methane oxidation in the water column of two hydrochemically contrasting sites in Lake Lugano, Switzerland. The South Basin displays seasonal stratification, the development of a benthic nepheloid layer and anoxia during summer and fall. The North Basin is permanently stratified with anoxic conditions below 115m water depth. Both Basins accumulate seasonally (South Basin) or permanently (North Basin) large amounts of CH4 in the water column below the chemocline, providing ideal conditions for methanotrophic microorganisms. Previous work revealed a high potential for aerobic methane oxidation within the anoxic water column, but no evidence for true AOM. Here, we show depth distribution data of dissolved CH4, methane oxidation rates and nutrients at both sites. In addition, we performed high resolution phylogenetic analyses of microbial community structures and conducted radio-label incubation experiments with concentrated biomass from anoxic waters and potential alternative electron acceptor additions (nitrate, nitrite and sulfate). First results from the unamended experiments revealed maximum activity of methane oxidation below the redoxcline in both basins. While the incubation experiments neither provided clear evidence for NOx- nor sulfate-dependent AOM, the phylogenetic analysis revealed the presence of members of the Methylomirabiliaceae family (NC10 phylum), known to perform AOM with nitrite as terminal electron acceptor. Interestingly, albeit the similarly favorable conditions in both basins, the South Basin showed nearly two-fold higher CH4 oxidation rates, but the Methylomirabiliaceae abundance appeared to be much higher in the meromictic North Basin. Ongoing work will attempt to verify whether the apparent difference in the abundance of Methylomirabiliaceae is a permanent feature. We will further seek to determine the relative contribution of bacterial nitrite-dependent AOM to total methane oxidation, as well as the environmental controls that may explain the differential importance of Methylomirabiliaceae in the two connected lake basins.

Seasonal variations in methane fluxes in response to summer warming and leaf litter addition in a subarctic heath ecosystem

NASA Astrophysics Data System (ADS)

Pedersen, Emily Pickering; Elberling, Bo; Michelsen, Anders

2017-08-01

Methane (CH4) is a powerful greenhouse gas controlled by both biotic and abiotic processes. Few studies have investigated CH4 fluxes in subarctic heath ecosystems, and climate change-induced shifts in CH4 flux and the overall carbon budget are therefore largely unknown. Hence, there is an urgent need for long-term in situ experiments allowing for the study of ecosystem processes over time scales relevant to environmental change. Here we present in situ CH4 and CO2 flux measurements from a wet heath ecosystem in northern Sweden subjected to 16 years of manipulations, including summer warming with open-top chambers, birch leaf litter addition, and the combination thereof. Throughout the snow-free season, the ecosystem was a net sink of CH4 and CO2 (CH4 -0.27 mg C m-2 d-1; net ecosystem exchange -1827 mg C m-2 d-1), with highest CH4 uptake rates (-0.70 mg C m-2 d-1) during fall. Warming enhanced net CO2 flux, while net CH4 flux was governed by soil moisture. Litter addition and the combination with warming significantly increased CH4 uptake rates, explained by a pronounced soil drying effect of up to 32% relative to ambient conditions. Both warming and litter addition also increased the seasonal average concentration of dissolved organic carbon in the soil. The site was a carbon sink with a net uptake of 60 g C m-2 over the snow-free season. However, warming reduced net carbon uptake by 77%, suggesting that this ecosystem type might shift from snow-free season sink to source with increasing summer temperatures.

Methane contamination of drinking water accompanying gas-well drilling and hydraulic fracturing

PubMed Central

Osborn, Stephen G.; Vengosh, Avner; Warner, Nathaniel R.; Jackson, Robert B.

2011-01-01

Directional drilling and hydraulic-fracturing technologies are dramatically increasing natural-gas extraction. In aquifers overlying the Marcellus and Utica shale formations of northeastern Pennsylvania and upstate New York, we document systematic evidence for methane contamination of drinking water associated with shale-gas extraction. In active gas-extraction areas (one or more gas wells within 1 km), average and maximum methane concentrations in drinking-water wells increased with proximity to the nearest gas well and were 19.2 and 64 mg CH4 L-1 (n = 26), a potential explosion hazard; in contrast, dissolved methane samples in neighboring nonextraction sites (no gas wells within 1 km) within similar geologic formations and hydrogeologic regimes averaged only 1.1 mg L-1 (P < 0.05; n = 34). Average δ13C-CH4 values of dissolved methane in shallow groundwater were significantly less negative for active than for nonactive sites (-37 ± 7‰ and -54 ± 11‰, respectively; P < 0.0001). These δ13C-CH4 data, coupled with the ratios of methane-to-higher-chain hydrocarbons, and δ2H-CH4 values, are consistent with deeper thermogenic methane sources such as the Marcellus and Utica shales at the active sites and matched gas geochemistry from gas wells nearby. In contrast, lower-concentration samples from shallow groundwater at nonactive sites had isotopic signatures reflecting a more biogenic or mixed biogenic/thermogenic methane source. We found no evidence for contamination of drinking-water samples with deep saline brines or fracturing fluids. We conclude that greater stewardship, data, and—possibly—regulation are needed to ensure the sustainable future of shale-gas extraction and to improve public confidence in its use. PMID:21555547

Effects of preconditioning the rhizosphere of different plant species on biotic methane oxidation kinetics.

PubMed

Ndanga, Éliane M; Lopera, Carolina B; Bradley, Robert L; Cabral, Alexandre R

2016-09-01

The rhizosphere is known as the most active biogeochemical layer of the soil. Therefore, it could be a beneficial environment for biotic methane oxidation. The aim of this study was to document - by means of batch incubation tests - the kinetics of CH4 oxidation in rhizosphere soils that were previously exposed to methane. Soils from three pre-exposure to CH4 zones were sampled: the never-before pre-exposed (NEX), the moderately pre-exposed (MEX) and the very pre-exposed (VEX). For each pre-exposure zone, the rhizosphere of several plant species was collected, pre-incubated, placed in glass vials and submitted to CH4 concentrations varying from 0.5% to 10%. The time to the beginning of CH4 consumption and the CH4 oxidation rate were recorded. The results showed that the fastest CH4 consumption occurred for the very pre-exposed rhizosphere. Specifically, a statistically significant difference in CH4 oxidation half-life was found between the rhizosphere of the VEX vegetated with a mixture of different plants and the NEX vegetated with ryegrass. This difference was attributed to the combined effect of the preconditioning level and plant species as well as to the organic matter content. Regardless of the preconditioning level, the oxidation rate values obtained in this study were comparable to those reported in the reviewed literature for mature compost. Copyright © 2016 Elsevier Ltd. All rights reserved.

Integrating Source Apportionment Tracers into a Bottom-up Inventory of Methane Emissions in the Barnett Shale Hydraulic Fracturing Region.

PubMed

Townsend-Small, Amy; Marrero, Josette E; Lyon, David R; Simpson, Isobel J; Meinardi, Simone; Blake, Donald R

2015-07-07

A growing dependence on natural gas for energy may exacerbate emissions of the greenhouse gas methane (CH4). Identifying fingerprints of these emissions is critical to our understanding of potential impacts. Here, we compare stable isotopic and alkane ratio tracers of natural gas, agricultural, and urban CH4 sources in the Barnett Shale hydraulic fracturing region near Fort Worth, Texas. Thermogenic and biogenic sources were compositionally distinct, and emissions from oil wells were enriched in alkanes and isotopically depleted relative to natural gas wells. Emissions from natural gas production varied in δ(13)C and alkane ratio composition, with δD-CH4 representing the most consistent tracer of natural gas sources. We integrated our data into a bottom-up inventory of CH4 for the region, resulting in an inventory of ethane (C2H6) sources for comparison to top-down estimates of CH4 and C2H6 emissions. Methane emissions in the Barnett are a complex mixture of urban, agricultural, and fossil fuel sources, which makes source apportionment challenging. For example, spatial heterogeneity in gas composition and high C2H6/CH4 ratios in emissions from conventional oil production add uncertainty to top-down models of source apportionment. Future top-down studies may benefit from the addition of δD-CH4 to distinguish thermogenic and biogenic sources.

In situ permafrost thaw due to climate change drives holistic microbial community shifts with implications for methane cycling

NASA Astrophysics Data System (ADS)

Mondav, Rhiannon; McCalley, Carmody; Hodgkins, Suzanne; Rich, Virginia; Frolking, Steve; Saleska, Scott; Barnes, Andrew; Chanton, Jeff; Crill, Patrick

2014-05-01

Thawing permafrost is a potentially significant source of radiative forcing feedback due to increased emissions of methane, a biogenic greenhouse gas (GHG). This study investigated changes in the microbial community along a permafrost thaw gradient at Stordalen Mire, Sweden using 16S rRNA gene amplicon and metagenomic methods. In situ measurements of geochemical parameters, including CH4 and C isotopes, enabled linkage of community dynamics to significant shifts in C balance. The thaw gradient ranged from intact at a palsa (low productivity and GHG emissions), through partially thawed in a bog (high productivity, low GHG emissions) to a completely thawed fen (high productivity and GHG emissions). Microbial assemblages in both the palsa and fen were highly diverse (in both richness and evenness), consistent with climax communities. The microbial community in the bog had distinctly lower diversity, characteristic of ecosystem disturbance. The palsa community was dominated by Acidobacteria and Proteobacteria, as is typical of a range of soils including permafrost. Methanogens dominated both the bog and fen and were most abundant within the zone of water table fluctuation. Inferring methanogens' production pathway from phylogeny showed a shift from mostly hydrogenotrophic methanogens in the bog towards acetotrophic methanogens in the fen. This corroborated porewater and flux emitted CH4 and CO2 carbon isotopic 13C signatures of CH4 and CO2. The fen, where the highest CH4 flux was recorded, was significantly richer in methanogenic archaea. A novel archaea, Candidatus Methanoflorens stordalenmirensis, was present at up to 70% relative abundance in the bog, enabling recovery of a population genome. The genome (and associated metaproteome) of 'M. stordalenmirensis' indicates that hydrogenotrophic methane production is its main energy conservation pathway. 'Methanoflorens' may be an indicator species of permafrost thaw, it is globally ubiquitous, and appears a major contributor to global methane production. Our results revealed a distinct difference in the microbial community structure and membership at each site, which can be directly associated with increasing methane emission and thaw state.

Using Mass Spectroscopy to Examine Wetland Carbon Flow from Plants to Methane

NASA Astrophysics Data System (ADS)

Waldo, N.; Tfaily, M. M.; Moran, J.; Hu, D.; Cliff, J. B.; Gough, H. L.; Chistoserdova, L.; Beck, D.; Neumann, R. B.

2017-12-01

In the anoxic soil of wetlands, microbes produce methane (CH4), a greenhouse gas. Prior studies have documented an increase in CH4 emissions as plant productivity increases, likely due to plants releasing more labile organic carbon from roots. But in the field, it is difficult to separate changes in plant productivity and root carbon exudation from other seasonal changes that can affect methane emissions, e.g. temperature. Clarifying the role that root exudation plays in fueling methane production is important because increasing atmospheric temperatures and CO2 levels are projected to increase plant productivity and exudation. To advance understanding of climate-methane feedbacks, this study tracked the flow of carbon from plants into the wetland rhizosphere as plant productivity increased in controlled laboratory conditions. We grew Carex aquatilis, a wetland sedge, in peat-filled rootboxes. Both early and late during the plant growth cycle, we exposed plants to headspace 13CO2, which the plants fixed. Some of this labeled carbon was exuded by the roots and used by rhizosphere microbes. We tracked the isotope ratio of emitted CH4 to establish the time required for plant-released carbon to fuel methanogenesis, and to determine the relative contribution of plant-derived carbon to total CH4 emission. We destructively harvested root and rhizosphere samples from various locations that we characterized by isotope ratio mass spectrometry (MS) to determine isotopic enrichment and therefore relative abundance of root exudates. We analyzed additional aliquots of rhizosphere soil by Fourier transform ion cyclotron resonance MS to track chemical changes in soil carbon as root exudates were converted into methane. To advance mechanistic understanding of the synergistic and competitive microbial interactions that affect methane dynamics in the wetland rhizosphere, we used fluorescence in-situ hybridization to visualize microbial community composition and spatial associations, and nanoscale secondary ion MS to measure isotopic enrichment of visualized microbes. Collectively, these data will elucidate how root-induced chemical changes in the soil impact microbial generation of CH4.

Enrichment in 13C of atmospheric CH4 during the Younger Dryas termination

NASA Astrophysics Data System (ADS)

Melton, J. R.; Schaefer, H.; Whiticar, M. J.

2012-07-01

The abrupt warming across the Younger Dryas termination (~11 600 yr before present) was marked by a large increase in the global atmospheric methane mixing ratio. The debate over sources responsible for the rise in methane centers on the roles of global wetlands, marine gas hydrates, and thermokarst lakes. We present a new, higher-precision methane stable carbon isotope ratio (δ13CH4) dataset from ice sampled at Påkitsoq, Greenland that shows distinct 13C-enrichment associated with this rise. We investigate the validity of this finding in face of known anomalous methane concentrations that occur at Påkitsoq. Comparison with previously published datasets to determine the robustness of our results indicates a similar trend in ice from both an Antarctic ice core and previously published Påkitsoq data measured using four different extraction and analytical techniques. The δ13CH4 trend suggests that 13C-enriched CH4 sources played an important role in the concentration increase. In a first attempt at quantifying the various contributions from our data, we apply a methane triple mass balance of stable carbon and hydrogen isotope ratios and radiocarbon. The mass balance results suggest biomass burning (42-66% of total methane flux increase) and thermokarst lakes (27-59%) as the dominant contributing sources. Given the high uncertainty and low temporal resolution of the 14CH4 dataset used in the triple mass balance, we also performed a mass balance test using just δ13C and δD. These results further support biomass burning as a dominant source, but do not allow distinguishing of thermokarst lake contributions from boreal wetlands, aerobic plant methane, or termites. Our results in both mass balance tests do not suggest as large a role for tropical wetlands or marine gas hydrates as commonly proposed.

The role of Sphagnum mosses in the methane cycling of a boreal mire.

PubMed

Larmola, Tuula; Tuittila, Eeva-Stiina; Tiirola, Marja; Nykänen, Hannu; Martikainen, Pertti J; Yrjälä, Kim; Tuomivirta, Tero; Fritze, Hannu

2010-08-01

Peatlands are a major natural source of atmospheric methane (CH4). Emissions from Sphagnum-dominated mires are lower than those measured from other mire types. This observation may partly be due to methanotrophic (i.e., methane-consuming) bacteria associated with Sphagnum. Twenty-three of the 41 Sphagnum species in Finland can be found in the peatland at Lakkasuo. To better understand the Sphagnum-methanotroph system, we tested the following hypotheses: (1) all these Sphagnum species support methanotrophic bacteria; (2) water level is the key environmental determinant for differences in methanotrophy across habitats; (3) under dry conditions, Sphagnum species will not host methanotrophic bacteria; and (4) methanotrophs can move from one Sphagnum shoot to another in an aquatic environment. To address hypotheses 1 and 2, we measured the water table and CH4 oxidation for all Sphagnum species at Lakkasuo in 1-5 replicates for each species. Using this systematic approach, we included Sphagnum spp. with narrow and broad ecological tolerances. To estimate the potential contribution of CH4 to moss carbon, we measured the uptake of delta13C supplied as CH4 or as carbon dioxide dissolved in water. To test hypotheses 2-4, we transplanted inactive moss patches to active sites and measured their methanotroph communities before and after transplantation. All 23 Sphagnum species showed methanotrophic activity, confirming hypothesis 1. We found that water level was the key environmental factor regulating methanotrophy in Sphagnum (hypothesis 2). Mosses that previously exhibited no CH4 oxidation became active when transplanted to an environment in which the microbes in the control mosses were actively oxidizing CH4 (hypothesis 4). Newly active transplants possessed a Methylocystis signature also found in the control Sphagnum spp. Inactive transplants also supported a Methylocystis signature in common with active transplants and control mosses, which rejects hypothesis 3. Our results imply a loose symbiosis between Sphagnum spp. and methanotrophic bacteria that accounts for potentially 10-30% of Sphagnum carbon.

Global trends in peatland methane production

NASA Astrophysics Data System (ADS)

Hoyt, A.; Corbett, J. E.; Gandois, L.; Cobb, A.; Pangala, S. R.; Gauci, V.; Harvey, C. F.

2017-12-01

Peatland methane production rates and fluxes to the atmosphere vary globally. Here we present a systematic comparison of peatland CH4 production across latitudes. We developed and applied an isotope-based mass transport model to characterize rates of methanogenesis and recharge rates across ten ombrotrophic peatlands from around the world. We validated our model against peat incubations and surface fluxes where data was available. We found striking similarities in the DIC and CH4 concentrations and δ13C isotope profiles across northern bogs, despite highly variable precipitation, recharge rates, and peat characteristics. Profiles from northern sites were similar because increased recharge rates were always compensated by increased CH4 production rates. This could represent a feedback mechanism between recharge rates and methanogenesis in northern bogs or could represent a shared dependence of these two properties on the degree of peat decomposition. We also found strong differences between northern and tropical sites, both in the rate of CH4 production, the recharge rate, and in the transport pathways and fluxes to the atmosphere. Our findings have important implications for methane transport and release to the atmosphere. In northern bogs, low flow rates allow CH4 concentrations to build up, and CH4 escapes by surface diffusion, ebullition, and plant-mediated transport. Thus, the majority of CH4 produced escapes through the peat surface. In tropical peatlands, high flow rates suppress CH4 concentrations, which do not build up above the threshold for ebullition. Instead, CH4 leaves the peat by lateral transport and surface fluxes are small. This work provides evidence that peat properties and hydrology are fundamental controls on decomposition, CH4 production, and peat formation across latitudes.

Pig feeding strategy coupled with effluent management - fresh or stored slurry, solid phase separation - on methane potential and methane conversion factors during storage

NASA Astrophysics Data System (ADS)

Jarret, Guillaume; Martinez, José; Dourmad, Jean-Yves

2011-11-01

In the guideline for the determination of methane (CH 4) emission from animal manure (IPCC) the amount of CH 4 emitted is generally calculated according to an equation combining the amount of organic matter (OM) or volatile solids excreted, the ultimate CH 4 potential ( B0) of excreta and a system-specific methane conversion factor (MCF, %) that reflects the portion of B0 that is really converted into CH 4. The objective of the present study was to investigate the effect of the modification of dietary crude protein and fibre levels on B0 of pig slurry and on subsequent MCF according to different strategies of slurry management. Five experimental diets differing mainly in their crude protein and fibre content were compared. Two types of measurement of CH 4 emission were performed. The first was the measurement of B0 of slurry using biomethanogene potential (BMP) test. The second consisted in a storage simulation, which was performed on different kinds of effluents: fresh slurry (FSl), stored slurry (SSl), and faeces mixed with water (FaW). The type of diet and the type of effluent affected ( P < 0.001) CH 4 production after 30, 50 and 100 days. Moreover, the interaction between type of effluent and type of diet was significant for CH 4 emission and for MCF. CH 4 production was the highest for BMP, the average production of CH 4 during storage from FaW, FSl and SSl samples representing 77%, 58% and 64% of the B0 value. The dynamic of CH 4 production during BMP tests was rather similar for all dietary treatments whereas it differed for storage simulation studies with significant effects of dietary CP and fibre contents. The results from this study indicate that the type of diet has a significant but rather limited effect on B0 value of effluent. The effect of diet is much more marked on MCF, with lower values for high protein diets, and higher values for high fibre diets. MCF is also affected by manure management, the values measured on separated faeces from urine being much higher than for slurry.

Quantifying the relative contribution of natural gas fugitive emissions to total methane emissions in Colorado, Utah, and Texas using mobile δ13CH4 analysis

NASA Astrophysics Data System (ADS)

Rella, C.; Crosson, E.; Petron, G.; Sweeney, C.; Karion, A.

2013-12-01

Fugitive emissions of methane into the atmosphere are a major concern facing the natural gas production industry. Because methane is more energy-rich than coal per kg of CO2 emitted into the atmosphere, it represents an attractive alternative to coal for electricity generation, provided that the fugitive emissions of methane are kept under control. A key step in assessing these emissions in a given region is partitioning the observed methane emissions between natural gas fugitive emissions and other sources of methane, such as from landfills or agricultural activities. One effective method for assessing the contribution of these different sources is stable isotope analysis, using the δ13CH4 signature to distinguish between natural gas and landfills or ruminants. We present measurements of mobile field δ13CH4 using a spectroscopic stable isotope analyzer based on cavity ringdown spectroscopy, in three intense natural gas producing regions of the United States: the Denver-Julesburg basin in Colorado, the Uintah basin in Utah, and the Barnett Shale in Texas. Mobile isotope measurements of individual sources and in the nocturnal boundary layer have been combined to establish the fraction of the observed methane emissions that can be attributed to natural gas activities. The fraction of total methane emissions in the Denver-Julesburg basin attributed to natural gas emissions is 78 +/- 13%. In the Uinta basin, which has no other significant sources of methane, the fraction is 96% +/- 15%. In addition, results from the Barnett shale are presented, which includes a major urban center (Dallas / Ft. Worth). Methane emissions in this region are spatially highly heterogeneous. Spatially-resolved isotope and concentration measurements are interpreted using a simple emissions model to arrive at an overall isotope ratio for the region. (left panel) Distribution of oil and gas well pads (yellow) and landfills (blue) in the Dallas / Ft. Worth area. Mobile nocturnal measurements of methane are shown in red, indicating a strong degree of source heterogeneity. (right panel) Histogram of individual isotopic source signatures, showing distinct signatures for landfills (red) and oil and gas sources (green).

How does whole ecosystem warming of a peatland affect methane production and consumption?

NASA Astrophysics Data System (ADS)

Hopple, A.; Brunik, K.; Keller, J.; Pfeifer-Meister, L.; Woerndle, G.; Zalman, C.; Hanson, P.; Bridgham, S. D.

2017-12-01

Peatlands are among Earth's most important terrestrial ecosystems due to their massive soil carbon (C) stores and significant release of methane (CH4) into the atmosphere. Methane has a sustained-flux global warming potential 45-times greater than carbon dioxide (CO2), and the accuracy of Earth system model projections relies on our mechanistic understanding of peatland CH4 cycling in the context of environmental change. The objective of this study was to determine, under in situ conditions, how heating of the peat profile affects ecosystem-level anaerobic C cycling. We assessed the response of CO2 and CH4 production, as well as the anaerobic oxidation of CH4 (AOM), in a boreal peatland following 13 months of deep peat heating (DPH) and 16 months of subsequent whole-ecosystem warming (surface and deep heating; WEW) as part of the Spruce and Peatland Responses Under Changing Environments (SPRUCE) project in northern Minnesota, USA. The study uses a regression-based experimental design including 5 temperature treatments that warmed the entire 2 m peat profile from 0 to +9 °C above ambient temperature. Soil cores were collected at multiple depths (25-200 cm) from each experimental chamber at the SPRUCE site and anaerobically incubated at in situ temperatures for 1-2 weeks. Methane and CO2 production in surface peat were positively correlated with elevated temperature, but no consistent temperature response was found at depth (75-200 cm) following DPH. However, during WEW, we observed significant increases in both surface and deep peat methanogenesis with increasing temperature. Surface peat had greater CH4 production rates than deeper peat, implying that the increased CH4 emissions observed in the field were largely driven by surface peat warming. The CO2:CH4 ratio was inversely correlated with temperature across all depths following 16 months of WEW, indicating that the entire peat profile is becoming more methanogenic with warming. We also observed AOM throughout the whole peat profile, with the highest rates observed at the surface and initial data suggesting a positive correlation with increasing temperature. While SPRUCE will continue for many years, our initial results suggest that the vast C stores at depth in peatlands are minimally responsive to warming and any response will be driven largely by surface peat.

Field Exploration of Methane Seep Near Atqasuk

DOE Office of Scientific and Technical Information (OSTI.GOV)

Katey Walter, Dennis Witmer, Gwen Holdmann

2008-12-31

Methane (CH{sub 4}) in natural gas is a major energy source in the U.S., and is used extensively on Alaska's North Slope, including the oilfields in Prudhoe Bay, the community of Barrow, and the National Petroleum Reserve, Alaska (NPRA). Smaller villages, however, are dependent on imported diesel fuel for both power and heating, resulting in some of the highest energy costs in the U.S. and crippling local economies. Numerous CH{sub 4} gas seeps have been observed on wetlands near Atqasuk, Alaska (in the NPRA), and initial measurements have indicated flow rates of 3,000-5,000 ft{sup 3} day{sup -1} (60-100 kg CH{submore » 4} day{sup -1}). Gas samples collected in 1996 indicated biogenic origin, although more recent sampling indicated a mixture of biogenic and thermogenic gas. In this study, we (1) quantified the amount of CH{sub 4} generated by several seeps and evaluated their potential use as an unconventional gas source for the village of Atqasuk; (2) collected gas and analyzed its composition from multiple seeps several miles apart to see if the source is the same, or if gas is being generated locally from isolated biogenic sources; and (3) assessed the potential magnitude of natural CH{sub 4} gas seeps for future use in climate change modeling.« less

Soil methane and CO2 fluxes in rainforest and rubber plantations

NASA Astrophysics Data System (ADS)

Lang, Rong; Blagodatsky, Sergey; Goldberg, Stefanie; Xu, Jianchu

2017-04-01

Expansion of rubber plantations in South-East Asia has been a land use transformation trend leading to losses of natural forest cover in the region. Besides impact on ecosystem carbon stocks, this conversion influences the dynamics of greenhouse gas fluxes from soil driven by microbial activity, which has been insufficiently studied. Aimed to understand how land use change affects the soil CO2 and CH4 fluxes, we measured surface gas fluxes, gas concentration gradient, and 13C signature in CH4 and soil organic matter in profiles in a transect in Xishuangbanna, including a rainforest site and three rubber plantation sites with age gradient. Gas fluxes were measured by static chamber method and open chamber respiration system. Soil gases were sampled from installed gas samplers at 5, 10, 30, and 75cm depth at representative time in dry and rainy season. The soil CO2 flux was comparable in rainforest and old rubber plantations, while young rubber plantation had the lowest rate. Total carbon content in the surface soil well explained the difference of soil CO2 flux between sites. All sites were CH4 sinks in dry season and uptake decreased in the order of rainforest, old rubber plantations and young rubber plantation. From dry season to rainy season, CH4 consumption decreased with increasing CH4 concentration in the soil profile at all depths. The enrichment of methane by 13CH4 shifted towards to lowerδ13C, being the evidence of enhanced CH4 production process while net surface methane flux reflected the consumption in wet condition. Increment of CH4 concentration in the profile from dry to rainy season was higher in old rubber plantation compared to rainforest, while the shifting of δ13CH4 was larger in rainforest than rubber sites. Turnover rates of soil CO2 and CH4 suggested that the 0-5 cm surface soil was the most active layer for gaseous carbon exchange. δ13C in soil organic matter and soil moisture increased from rainforest, young rubber plantation to old rubber plantations. Conversion the forest into rubber plantation decreased soil respiration in young plantation and it recovered during rubber development. However, the CH4consumption by tropical upland forest soil decreased in converted rubber plantations of all ages, with more decrement in old plantation. Change forest into rubber plantations weakened the soil function as CH4 sink.

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

NASA Astrophysics Data System (ADS)

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 taken during the incubation for CH4 and CO2 concentration measurements and isotope ratio mass spectrometry (CH4, CO2). Grassland and forest soils showed differences in CO2 and CH4 production rates. Based on the 13C-CH4 signature we found that all substrates were metabolized to CH4, but to a different degree. Inhibitors reduced CH4 production and conversion of certain substrates to a different degree. Using the example of acetate and cycloheximide, in both soils acetate increased respiration, whereas cycloheximide reduced respiration by 56 and 62 %, respectively. For CH4 production, however, no effect was visible for the grassland soil, but in the forest soil CH4 production increased by 69 %. Cycloheximide inhibited the substrate-induced CH4 production by 63 %, indicating that fungi were responsible for this pathway. Moreover, the finding that fungi use the methyl group of acetate to produce CH4 was also verified with a sterile culture. References Lenhart, K. et al. Evidence for methane production by saprotrophic fungi. Nat Commun 3, 1046, (2012). Keppler, F., et al. Methane emissions from terrestrial plants under aerobic conditions. Nature 439, 187-191 (2006). Jugold, A. et al. Non-microbial methane formation in oxic soils. Biogeosciences 9, 5291-5301, (2012).

Effects of mass air flow rate through an open-circuit gas quantification system when measuring carbon emissions

USDA-ARS?s Scientific Manuscript database

Methane (CH4) and carbon dioxide (CO2) represent 11 and 81%, respectively, of all anthropogenic greenhouse gas emissions. Agricultural CH4 emissions account for approximately 43% of all anthropogenic CH4 emissions. Most agricultural CH4 emissions are attributed to enteric fermentation within rumin...

Methane Fingerprinting: Isotopic Methane and Ethane-to-Methane Ratio Analysis Using a Cavity Ring-Down Spectrometer

NASA Astrophysics Data System (ADS)

Saad, Nabil; Fleck, Derek; Hoffnagle, John

2016-04-01

Emissions of Natural gas, and methane (CH4) specifically, have come under increased scrutiny by virtue of methane's 28-36x greenhouse warming potential compared to carbon dioxide (CO2) while accounting for 10% of the total greenhouse gas emissions in the US. Large uncontrolled leaks, such as the recent Aliso Canyon leak, originating from uncapped wells, coal mines and storage facilities have increased the total global contribution of methane missions even further. Determining the specific fingerprint of methane sources, by quantifying δ13C values and C2:C1 ratios, provides the means to understand methane producing processes and allows for sources of methane to be mapped and classified through these processes; i.e. biogenic vs. thermogenic, wet vs dry. In this study we present a fully developed Cavity Ring-Down Spectrometer (CRDS) that precisely measures 12CH4 concentration and its 13CH4 isotope concentration, yielding δ13C measurements, C2H6 concentration, along with CO2 and H2O. This provides real-time continuous measurements without an upfront separation requirement or multiple analyses to derive the origin of the gas samples. The highly sensitive analyzer allows for measurements of scarce molecules down to sub-ppb 1-σ precision in 5 minutes of measurement: with CH4 <0.1ppb, δ13C <1‰ C2H6 <1ppb and CO2 <1ppm. To complement this work, we provide the analysis of different methane sources providing a 2-dimensional mapping of methane sources as functions of δ13C and C2:C1 ratios, which can be thought of as a modified Bernard Plot. This dual ratio mapping can be used to discriminate between naturally occurring biogenic methane sources, naturally occurring enriched thermogenic sources, and natural gas distribution sources. This also shows future promise in aiding gas and oil exploration, in distinguishing oil vs coal gases, as well as a valuable tool in the development of methane sequestration.

Evaluating the biochemical methane potential (BMP) of low-organic waste at Danish landfills.

PubMed

Mou, Zishen; Scheutz, Charlotte; Kjeldsen, Peter

2014-11-01

The biochemical methane potential (BMP) is an essential parameter when using first order decay (FOD) landfill gas (LFG) generation models to estimate methane (CH4) generation from landfills. Different categories of waste (mixed, shredder and sludge waste) with a low-organic content and temporarily stored combustible waste were sampled from four Danish landfills. The waste was characterized in terms of physical characteristics (TS, VS, TC and TOC) and the BMP was analyzed in batch tests. The experiment was set up in triplicate, including blank and control tests. Waste samples were incubated at 55°C for more than 60 days, with continuous monitoring of the cumulative CH4 generation. Results showed that samples of mixed waste and shredder waste had similar BMP results, which was in the range of 5.4-9.1 kg CH4/ton waste (wet weight) on average. As a calculated consequence, their degradable organic carbon content (DOCC) was in the range of 0.44-0.70% of total weight (wet waste). Numeric values of both parameters were much lower than values of traditional municipal solid waste (MSW), as well as default numeric values in current FOD models. The sludge waste and temporarily stored combustible waste showed BMP values of 51.8-69.6 and 106.6-117.3 kg CH4/ton waste on average, respectively, and DOCC values of 3.84-5.12% and 7.96-8.74% of total weight. The same category of waste from different Danish landfills did not show significant variation. This research studied the BMP of Danish low-organic waste for the first time, which is important and valuable for using current FOD LFG generation models to estimate realistic CH4 emissions from modern landfills receiving low-organic waste. Copyright © 2014 Elsevier Ltd. All rights reserved.

Temperate forest methane sink diminished by tree emissions.

PubMed

Pitz, Scott; Megonigal, J Patrick

2017-06-01

Global budgets ascribe 4-10% of atmospheric methane (CH 4 ) sinks to upland soils and have assumed until recently that soils are the sole surface for CH 4 exchange in upland forests. Here we report that CH 4 is emitted from the stems of dominant tree species in a temperate upland forest, measured using both the traditional static-chamber method and a new high-frequency, automated system. Tree emissions averaged across 68 observations on 17 trees from May to September were 1.59 ± 0.88 μmol CH 4  m -2  stem h -1 (mean ± 95% confidence interval), while soils adjacent to the trees consumed atmospheric CH 4 at a rate of -4.52 ± 0.64 μmol CH 4  m -2  soil h -1 (P < 0.0001). High-frequency measurements revealed diurnal patterns in the rate of tree-stem CH 4 emissions. A simple scaling exercise suggested that tree emissions offset 1-6% of the growing season soil CH 4 sink and may have briefly changed the forest to a net CH 4 source. © 2017 The Authors. New Phytologist © 2017 New Phytologist Trust.

Methane flux from mangrove sediments along the southwestern coast of Puerto Rico

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sotomayor, D.; Corredor, J.E.; Morell, J.M.

1994-03-01

Although the sediments of coastal marine mangrove forests have been considered a minor source of atmospheric methane, these estimate have been based on sparse data from similar areas. We have gathered evidence that shows that external nutrient and freshwater loading in mangrove sediments may have a significant effect on methane flux. Experiments were performed to examine methane fluxes from anaerobic sediments in a mangrove forest subjected to secondary sewage effluents on the southwestern coast of Puerto Rico. Emission rates were measured in situ using a static chamber technique, and subsequent laboratory analysis of samples was by gas chromatography using amore » flame ionization detector. Results indicate that methane flux rates were lowest at the landward fringe nearest to the effluent discharge, higher in the seaward fringe occupied by red mangroves, and highest in the transition zone between black and red mangrove communities, with average values of 4 mg CH[sub 4] m[sup [minus]2] d[sup [minus]1], 42 mg CH[sub 4] m[sup [minus]2] d[sup [minus]1], and 82 mg CH[sub 4] m[sup [minus]2] d[sup [minus]1], respectively. Overall mean values show these sediments may emit as much as 40 times more methane than unimpacted pristine areas. Pneumatophores of Aviciennia germinans have been found to serve as conduits to the atmosphere for this gas. Fluctuating water level overlying the mangrove sediment is an important environmental factor controlling seasonal and interannual CH[sub 4] flux variations. Environmental controls such as freshwater inputs and increased nutrient loading influence in situ methane emissions from these environments. 34 refs., 3 figs., 3 tabs.« less

Determination of biogas generation potential as a renewable energy source from supermarket wastes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alkanok, Gizem; Demirel, Burak, E-mail: burak.demirel@boun.edu.tr; Onay, Turgut T.

2014-01-15

Highlights: • Disposal of supermarket wastes in landfills may contribute to environmental pollution. • High methane yields can be obtained from supermarket wastes by anaerobic co-digestion. • Fruit and vegetable wastes or dairy products wastes could individually be handled by a two-stage anaerobic process. • Buffering capacity, trace metal and C/N ratio are essential for digestion of supermarket wastes. - Abstract: Fruit, vegetable, flower waste (FVFW), dairy products waste (DPW), meat waste (MW) and sugar waste (SW) obtained from a supermarket chain were anaerobically digested, in order to recover methane as a source of renewable energy. Batch mesophilic anaerobic reactorsmore » were run at total solids (TS) ratios of 5%, 8% and 10%. The highest methane yield of 0.44 L CH{sub 4}/g VS{sub added} was obtained from anaerobic digestion of wastes (FVFW + DPW + MW + SW) at 10% TS, with 66.4% of methane (CH{sub 4}) composition in biogas. Anaerobic digestion of mixed wastes at 5% and 8% TS provided slightly lower methane yields of 0.41 and 0.40 L CH{sub 4}/g VS{sub added}, respectively. When the wastes were digested alone without co-substrate addition, the highest methane yield of 0.40 L CH{sub 4}/g VS{sub added} was obtained from FVFW at 5% TS. Generally, although the volatile solids (VS) conversion percentages seemed low during the experiments, higher methane yields could be obtained from anaerobic digestion of supermarket wastes. A suitable carbon/nitrogen (C/N) ratio, proper adjustment of the buffering capacity and the addition of essential trace nutrients (such as Ni) could improve VS conversion and biogas production yields significantly.« less

Influence of preadsorbed oxygen on activated chemisorption of methane on Pd(110)

NASA Astrophysics Data System (ADS)

Valden, M.; Pere, J.; Xiang, N.; Pessa, M.

1996-07-01

Dissociative chemisorption of methane on clean and oxygen modified Pd(110) has been studied by using molecular beam surface scattering. The absolute dissociation probability of CH 4 ( Stot) is found to increase exponentially with the incident normal energy ( En) of CH 4 and with surface temperature ( TS) on clean Pd(110). The kinetic isotope effect is also found; namely, Stot of CD 4 is 4 to 5 times smaller than Stot of CH 4 throughout the entire range of En studied. These results are consistent with a direct dissociation mechanism. Measurements on preadsorbed oxygen on Pd(110) show that Stot of CH 4 decreases linearly, as oxygen coverage is increased from 0 to 0.4 ML in good agreement with the first-order Langmuir kinetics when approximately two active sites are blocked by one oxygen atom. No influence of the oxygen induced surface reconstructions on the dissociative adsorption kinetics of CH 4 is observed.

Water drives the deuterium content of the methane emitted from plants

NASA Astrophysics Data System (ADS)

Vigano, I.; Holzinger, R.; Keppler, F.; Greule, M.; Brand, W. A.; Geilmann, H.; van Weelden, H.; Röckmann, T.

2010-07-01

The spatial distribution of the deuterium content of precipitation has a well-established latitudinal variation that is reflected in organic molecules in plants growing at different locations. Some laboratory and field studies have already shown that the deuterium content of methane emitted from methanogens can be partially related to δD variations of the water in the surrounding environment. Here we present a similar relation for the methane emitted from plant biomass under UV radiation. To show this relation, we determined the hydrogen isotopic composition of methane released from leaves of a range of plants grown with water of different deuterium content (δD = -130‰ to +115‰). The plant leaves were irradiated with UV light and the CH 4 isotopic composition was measured by continuous flow isotope ratio mass spectrometry (CF-IRMS). Furthermore, the deuterium content of bulk biomass and of the methoxyl (OCH 3) groups of the biomass was measured. The D/H ratio successively decreases from bulk biomass (δD = -106‰ to -50‰) via methoxyl groups (δD = -310‰ to -115‰) to the CH 4 emitted (δD = -581‰ to -196‰). The range of isotope ratios in bulk biomass and OCH 3 groups is smaller than in the water used to grow the plants. Methoxyl groups, which contain only non-exchangeable hydrogen, can be used to assess the fraction of external water that was incorporated before OCH 3 groups were formed. Surprisingly, the CH 4 formed under UV irradiation has a wider isotopic range than the OCH 3 groups. Although the precise production pathway cannot be fully determined, the presented experiments indicate that methoxyl groups are not the only source substrate for CH 4, but that other sources, including very depleted ones, must contribute. The main limitation to the interpretation of the data is the possible influence of exchangeable water, which could not be quantified. Future studies should include measurements of leaf water and avoid interaction between different plants via the gas phase. Despite these deficiencies, the results suggest that the deuterium content of the methane generated from plants under UV irradiation is closely linked to δD in precipitation. This dependency, which should also exist for other biogenic methane sources could be evaluated with global isotope models.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Devi, V. Malathy; Benner, D. Chris; Gamache, Robert R.

In this paper, we report experimental measurements of spectral line shape parameters (air-broadened width, shift, and line mixing coefficients) for several transitions in the ν 3 Q branch of methane in the 3000–3023 cm -1 region. 13 high-resolution, room temperature laboratory spectra of pure methane and air-broadened methane recorded with two different Fourier transform spectrometers are fitted. 12 of these spectra were acquired at 0.01 cm -1 resolution with the McMath-Pierce FTS at the National Solar Observatory on Kitt Peak, and one higher-resolution (~0.0011 cm-1) low pressure methane spectrum was obtained with the Bruker IFS-120HR FTS at the Pacific Northwestmore » National Laboratory, in Richland, Washington. All the spectra were obtained using high purity natural samples of CH 4 and lean mixtures of the same natural CH 4 in dry air. For the 12 spectra recorded at Kitt Peak, three different absorption cells (L= 5, 25 and 150 cm) were used while the methane spectrum at PNNL was obtained using a 19.95 cm long absorption cell. For the analysis, an interactive multispectrum nonlinear least squares fitting software was employed where all the 13 spectra were fitted simultaneously. An accurate and self-consistent set of line parameters were determined by constraining a few of those for severely blended transitions. Line mixing was measured for fourteen transition pairs for the CH 4-air collision system. Lastly, a constant speed dependence parameter, consistent with measured speed dependence values obtained in other methane bands, was applied to all the transitions included in the fitted region. The present measurements are compared to values reported in the literature.« less

METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 10: METERING AND PRESSURE REGULATING STATIONS IN NATURAL GAS TRANSMISSIONS AND DISTRIBUTION

EPA Science Inventory

The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...

Interannual, seasonal, and retrospective analysis of the methane and carbon dioxide budgets of a temperate peatland

Treesearch

D.M. Olson; T.J. Griffis; A. Noormets; R. Kolka; J. Chen

2013-01-01

Three years (2009-2011) of near-continuous methane (CH4) and carbon dioxide (CO2) fluxes were measured with the eddy covariance (EC) technique at a temperate peatland located within the Marcell Experimental Forest, in northern Minnesota, USA. The peatland was a net source of CH4 and a net sink of CO...

Synthesis of Bilayer Graphene on 90/10 Copper (Cu)/Nickel (Ni) Alloy and Transfer by Electrochemical Delamination

DTIC Science & Technology

2017-09-01

C) and slow decomposition rate in methane (CH4).11 Cu alone has sometimes been shown to form incomplete bilayers with a significant fraction of...argon BLG bilayer graphene C carbon CH4 methane Cu2O cuprous oxide Cu copper CVD chemical vapor deposition DI deionized FeCl3 iron

Biogas reforming over multi walled carbon nanotubes with Co-Mo/MgO nanoparticles

NASA Astrophysics Data System (ADS)

Khavarian, Mehrnoush; Mohamed, Abdul Rahman

2017-12-01

The utilization of biogas for the production of valuable chemicals is among the very important processes in the energy research field. The most suitable process for biogas reforming is dry reforming of methane. An obvious drawback is the variable composition of biogas rather than the stoichiometrically equimolar quantities of methane and carbon dioxide. Moreover, activating the methane and carbon dioxide molecules in the reforming reaction provides many challenges in exploring new concepts and opportunities for development of unique catalysts. In the present work, the catalytic activity behavior of Co-Mo-MgO/multi-walled carbon nanotubes (MWCNTs) nanocomposite in dry reforming was investigated with different CO2/CH4 feed ratio to evaluate the performance of this catalyst for biogas reforming reaction. It was found that conversions of methane and carbon dioxide were greatly influenced by the feed gas ratio. The CH4 and CO2 conversions are 83 % and 87 % at the reaction temperature of 825 °C, GHSV of 175 L/h.gcat and CO2/CH4 feed ratio of unity. The minimum carbon deposition rate is observed at the CO2/CH4 feed ratio of 0.6 which is 0.080 gc/gcat-h.

Anaerobic digestion of pre-fermented potato peel wastes for methane production.

PubMed

Liang, Shaobo; McDonald, Armando G

2015-12-01

This study investigated the feasibility of anaerobic digestion (AD) of potato peel waste (PPW) and its lactic acid fermentation residue (PPW-FR) for methane (CH4) production. The experimental results showed that about 60-70% CH4 content was obtained. The digester using PPW-FR as feedstock exhibited better performance and produced a highest cumulative CH4 production of 273 L/kg VS fed, followed by 239 L/kg VS fed using PPW under the same conditions. However, with increasing solid loadings of PPW-FR feedstock from 6.4% to 9.1%, the CH4 production was inhibited. The generation, accumulation, and degradation of volatile fatty acids (VFAs) in digesters were also investigated in this research. Copyright © 2015 Elsevier Ltd. All rights reserved.

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

PubMed

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.

Controls of Methane Dynamics and Emissions in an Arctic Warming Experiment

NASA Astrophysics Data System (ADS)

Nielsen, C. S.; Elberling, B.; Michelsen, A.; Strobel, B. W.; Wulff, K.; Banyasz, I.

2015-12-01

Climatic changes have resulted in increasing air temperatures across the Arctic. This may increase anaerobic decomposition of soil organic matter to methane (CH4) in wetlands and increase plant growth and thereby production of substrate. Little is known about how seasonal variations in dissolved CH4 in soil water, substrate availability, and the effect of warming affect arctic wetland dynamics of CH4 production and emission. In 2013 we established two experiments in a fen at Disko Island, W Greenland; one with year round warming by open-top chambers and removal of shrubs, and one with removal of the aerenchymatous sedge Carex aquatilis ssp. stans. Throughout the growing season 2014 we measured how the treatments affected CH4 emissions, dissolved CH4 in the soil water, and substrate availability. Ecosystem CH4 emissions peaked at August 5th 2014 (7.5 μmol m-2 h-1) without coinciding with time of highest concentrations of dissolved CH4 or acetate indicating a decoupling between production and emission of CH4. The peak in dissolved CH4 concentration, at ten cm depth (1368 ppm, September 18th 2014), followed the peak in concentration of acetate in the same depth (0.30 ppm, August 30th 2014) highlighting the importance of this substance as a substrate for methanogenesis. C. aquatilis ssp. stans accounted for 60% and 77% of the ecosystem CH4 emissions in areas of the fen with water table above and below soil surface showing the importance of the presence of this species to serve as a pipe for CH4 emission which is bypassing the upper soil zone and potential methane oxidation. Throughout the season, warming increased the air temperature at soil surface by on average 0.89°C and occasionally warming and shrub removal increased soil temperature in 2 and 5 cm depth, but there was no effect of the treatments on the CH4 emissions indicating that this wetland is quite resilient towards future climate change.

Shallow Aquifer Methane Gas Source Assessment

NASA Astrophysics Data System (ADS)

Coffin, R. B.; Murgulet, D.; Rose, P. S.; Hay, R.

2014-12-01

Shale gas can contribute significantly to the world's energy demand. Hydraulic fracturing (fracking) on horizontal drill lines developed over the last 15 years makes formerly inaccessible hydrocarbons economically available. From 2000 to 2035 shale gas is predicted to rise from 1% to 46% of the total natural gas for the US. A vast energy resource is available in the United States. While there is a strong financial advantage to the application of fracking there is emerging concern about environmental impacts to groundwater and air quality from improper shale fracking operations. Elevated methane (CH4) concentrations have been observed in drinking water throughout the United States where there is active horizontal drilling. Horizontal drilling and hydraulic-fracturing can increase CH4 transport to aquifers, soil and the vadose zone. Seepage can also result from casing failure in older wells. However, there is strong evidence that elevated CH4 concentrations can be associated with topographic and hydrogeologic features, rather than shale-gas extraction processes. Carbon isotope geochemistry can be applied to study CH4source(s) in shallow vadose zone and groundwater systems. A preliminary TAMU-CC isotope data set from samples taken at different locations in southern Texas shows a wide range of CH4 signatures suggesting multiple sources of methane and carbon dioxide. These data are interpreted to distinguish regions with methane contributions from deep-sourced horizontal drilling versus shallow system microbial production. Development of a thorough environmental assessment using light isotope analysis can provide understanding of shallow anthropogenic versus natural CH4sources and assist in identifying regions that require remedial actions.

Influence of the ultrasound pretreatment on anaerobic digestion of cattle manure, food waste and crude glycerine.

PubMed

Ormaechea, Pedro; Castrillón, Leonor; Marañón, Elena; Fernández-Nava, Yolanda; Negral, Luis; Megido, Laura

2017-03-01

To increase the production of methane, when cattle manure (CM) is digested, pretreatments can be applied and/or the manure can be co-digested with other wastes. In this research work, a mixture of CM, food waste (FW) and raw glycerine (Gly) in a proportion in weight of 87% CM, 10% FW and 3% Gly was digested, (a) without pretreatment and (b) with pretreatment by ultrasound, applying a sonication energy of 1040 kJ/kg total solids. Specific methane production was 290 L CH 4 /kg volatile solids (VS) without pretreatment and 520 L CH 4 /kg VS with pretreatment. With respect to the volumetric methane production, 1.07 L CH 4 /L reactor .day was produced in the first case, and in the second case, 1.98 L CH 4 /L reactor .day. We can conclude that the application of ultrasound pretreatment significantly improved the production of biogas.

Analysis of operational methane emissions from pressure relief valves from biogas storages of biogas plants.

PubMed

Reinelt, Torsten; Liebetrau, Jan; Nelles, Michael

2016-10-01

The study presents the development of a method for the long term monitoring of methane emissions from pressure relief valves (PRV(1)) of biogas storages, which has been verified during test series at two PRVs of two agricultural biogas plants located in Germany. The determined methane emission factors are 0.12gCH4kWhel(-1) (0.06% CH4-loss, within 106days, 161 triggering events, winter season) from biogas plant A and 6.80/7.44gCH4kWhel(-1) (3.60/3.88% CH4-loss, within 66days, 452 triggering events, summer season) from biogas plant B. Besides the operational state of the biogas plant (e.g. malfunction of the combined heat and power unit), the mode of operation of the biogas flare, which can be manually or automatically operated as well as the atmospheric conditions (e.g. drop of the atmospheric pressure) can also affect the biogas emission from PRVs. Copyright © 2016 Elsevier Ltd. All rights reserved.

Reservoir water level drawdown as a novel, substantial, and manageable control on methane release to the atmosphere

NASA Astrophysics Data System (ADS)

Harrison, J.; Deemer, B. R.; Birchfield, M. K.

2014-12-01

Reservoirs constitute a globally important source of atmospheric methane (CH4). Although it is reasonably well-established that hydrostatic and barometric pressure can influence rates of CH4 release from lake and tidal sediments, the relationship between water-level manipulation and CH4 release from man-made impoundments has not been quantified or characterized. Furthermore, cross-system controls on CH4 production and release to the atmosphere have not been established. We collected CH4 emission (diffusion and ebullition) data for 8 reservoirs in the U.S. Pacific Northwest that are subject to a range of trophic conditions and water level management regimes. Our aim was to: (1) characterize CH4 emissions from these systems, and (2) quantify effects of water level management and eutrophication on CH4 fluxes. Results indicate very high fluxes, in some cases the highest reported reservoir emission rates, and a strong correspondence between lake level reduction and CH4 emissions, including quantitatively important bursts of CH4 bubbling. In one reservoir, drawdown-associated CH4 fluxes accounted for over 25% of annual CH4 emissions in a period of just 16 days (4% of the year). Average CH4 ebullition rates in a reservoir managed for hydropower peaking were nearly three-fold higher than in a paired upstream reservoir managed to maintain a constant water level (528 mg CH4 m-2 d-1 and 187 mg CH4 m-2 d-1 respectively). Highest gas fluxes were observed during the water level drawdown component of the hydropower peaking cycle (14.3 g CH4 m-2 d-1). In addition we observe a strong, positive relationship between eutrophication (as indicated by surface Chl a concentrations) and CH4 production (r2 = 0.88; P<0.001) and between eutrophication and the sensitivity of CH4 emissions to drawdown (r2 = 0.84; P<0.001). This work suggests that manipulation of water levels can significantly affect CH4 emissions from reservoirs to the atmosphere, and that sampling programs that miss drawdown periods may substantially underestimate CH4 fluxes. It also suggests that controlling nutrient loading may reduce greenhouse gas fluxes from surface waters to the atmosphere.

Nitrogen oxides and methane treatment by non-thermal plasma

NASA Astrophysics Data System (ADS)

Alva, E.; Pacheco, M.; Colín, A.; Sánchez, V.; Pacheco, J.; Valdivia, R.; Soria, G.

2015-03-01

Non thermal plasma was used to treat nitrogen oxides (NOx) and methane (CH4), since they are important constituents of hydrocarbon combustion emissions processes and, both gases, play a key role in the formation of tropospheric ozone. These gases are involved in environmental problems like acid rain and some diseases such as bronchitis and pneumonia. In the case of methane is widely known its importance in the global climate change, and currently accounts for 30% of global warming. There is a growing concern for methane leaks, associated with a rapid expansion of unconventional oil and gas extraction techniques as well as a large-scale methane release from Arctic because of ice melting and the subsequent methane production of decaying organic matter. Therefore, methane mitigation is a key to avoid dangerous levels of global warming. The research, here reported, deals about the generation of non-thermal plasma with a double dielectric barrier (2DBD) at atmospheric pressure with alternating current (AC) for NOx and CH4 treatment. The degradation efficiencies and their respective power consumption for different reactor configurations (cylindrical and planar) are also reported. Qualitative and quantitative analysis of gases degradation are reported before and after treatment with cold plasma. Experimental and theoretical results are compared obtaining good removal efficiencies, superior to 90% and to 20% respectively for NOx and CH4.

Methane production enhancement by an independent cathode in integrated anaerobic reactor with microbial electrolysis.

PubMed

Cai, Weiwei; Han, Tingting; Guo, Zechong; Varrone, Cristiano; Wang, Aijie; Liu, Wenzong

2016-05-01

Anaerobic digestion (AD) represents a potential way to achieve energy recovery from waste organics. In this study, a novel bioelectrochemically-assisted anaerobic reactor is assembled by two AD systems separated by anion exchange membrane, with the cathode placing in the inside cylinder (cathodic AD) and the anode on the outside cylinder (anodic AD). In cathodic AD, average methane production rate goes up to 0.070 mL CH4/mL reactor/day, which is 2.59 times higher than AD control reactor (0.027 m(3) CH4/m(3)/d). And COD removal is increased ∼15% over AD control. When changing to sludge fermentation liquid, methane production rate has been further increased to 0.247 mL CH4/mL reactor/day (increased by 51.53% comparing with AD control). Energy recovery efficiency presents profitable gains, and economic revenue from increased methane totally self-cover the cost of input electricity. The study indicates that cathodic AD could cost-effectively enhance methane production rate and degradation of glucose and fermentative liquid. Copyright © 2016 Elsevier Ltd. All rights reserved.

Measurement of methane emissions from ruminant livestock using a SF[sub 6] tracer technique

DOE Office of Scientific and Technical Information (OSTI.GOV)

Johnson, K.; Huyler, M.; Westberg, H.

1994-02-01

The purpose of this paper is to describe a method for determining methane emission factors for cattle. The technique involves the direct measurement of methane emissions from livestock in their natural environment. A small permeation tube containing SF[sub 6] is placed in the cow's rumen, and SF[sub 6] and CH[sub 4] concentrations are measured near the mouth and nostrils of the cow. The SF[sub 6] release provides a way to account for the dilution of gases near the animal's mouth. The CH[sub 4] emission rate can be calculated from the known SF[sub 6] emission rate and the measured SF[sub 6]more » and CH[sub 4] concentrations. The tracer method described provides an easy means for acquiring a large methane emissions data base from domestic livestock. The low cost and simplicity should make it possible to monitor a large number of animals in countries throughout the world. An expanded data base of this type helps to reduce uncertainty in the ruminant contribution to the global methane budget. 18 refs., 3 figs., 3 tabs.« less

Living Trees are a Major Source of Methane in the Temperate Forest

NASA Astrophysics Data System (ADS)

Covey, Kristofer

2017-04-01

Globally, forests sequester about 1.1 ± 0.8 Pg C yr-1, an ecosystem service worth hundreds of billions of dollars annually. Following the COP21 meeting in Paris, an international consensus emerged: The protection and expansion of forests worldwide is a necessary component of climate mitigation strategies to limit warming to less than 2°C. The physiological processes governing sequestration of CO2 in living trees are well studied and the resulting pattern in global forest carbon sequestration is clear. The role living trees play in the production and emission of methane (CH4) remains unclear, despite the fact it has the potential to offset climate benefits of forest CO2 sequestration. A known but largely unexplored pathway of forest CH4 production involves microbial-based methanogenesis in the wood of living trees. In the first regional-scale study of tree trunk gas composition, we examine the ubiquity and potential source strength of this pathway. Trunk methane concentrations were as high as 67.4% by volume (375,000-times atmospheric), with the highest concentrations found in older angiosperms (18,293 μLṡL-1 ± 3,096). Bark flux chambers from 23 living trees show emissions under field conditions, and large static chambers demonstrate high rates of production in felled Acer rubrum trunk sections. Diffusion flux modeling of trunk concentrations suggests wood-based microflora could produce a global CH4 efflux of 26 Tg CH4 yr-1. Applying these fluxes to provide a spatially explicit map of trunk-based CH4 flux, we estimate the potential relationship between carbon sequestration rates and CH4 emission by forest trees in Eastern North America. Methane emissions from the trunk-based methanogenic pathway could reduce the average climate mitigation value of these temperate forests by 10-30%. We highlight the need to improve earth systems models to account for the full complexity of forest climate interactions and provide a data layer useful in reducing large uncertainty in global methane budgets.

Methane emissions from western Canadian peatland lakes: assessing interactive effects of groundwater connectivity and permafrost thaw

NASA Astrophysics Data System (ADS)

Kuhn, M. A.; Riechert, C.; Estop Aragones, C.; Broder, T.; Bastviken, D.; Knorr, K. H.; Olefeldt, D.

2017-12-01

Rising temperatures and the submergence of recently thawed permafrost into lakes has been identified as a major driver of methane (CH4) emissions in northern regions. Lakes on the vast Taiga Plains in western Canada represent a vital unknown with respect to CH4 fluxes and their sensitivity to permafrost thaw. The Taiga Plains has several characteristics that could influence magnitude and controls on lake CH4 emissions in comparison to other regions, including high soil organic carbon stores, distinct permafrost history, and complex groundwater interactions that influence availability of terminal electron acceptor concentrations among lakes. The goal of this research is to describe the similarities and differences in processes governing lake CH4 emissions between western Canada and other northern regions. We carried out biweekly diffusive and ebullition flux measurements and monitored sediment redox profiles from two lakes near the border between Alberta and the Northwest Territories. The two lakes differ in contributions of surface water and groundwater inputs, respectively. Floating chamber-based fluxes were measured leading from the edges to the centers of the lakes from ice-out in early May until ice-cover in the fall. Preliminary redox profile analyses suggest the groundwater-fed lake has extremely high concentrations of sulfides (>200 µmol L-1) down to a depth of 30 cm, while the surface water lake has little to no sulfide, but high concentrations of reduced iron (>200 µmol L-1 ). Despite high sulfide concentrations in the sediments, the groundwater-fed lake had generally higher diffusive fluxes compared to the surface water lake, but there were no differences between the center and along the actively collapsing thermokarst edges. However, ebullition fluxes were highest from a recently thawed lake edge compared to the center of the lake and stable, non-thaw influenced edges. The results of this project will help improve current regional CH4 models by including ground-based methane flux measurements from the vast and previously unstudied region of western Canada.

Mapping urban pipeline leaks: methane leaks across Boston.

PubMed

Phillips, Nathan G; Ackley, Robert; Crosson, Eric R; Down, Adrian; Hutyra, Lucy R; Brondfield, Max; Karr, Jonathan D; Zhao, Kaiguang; Jackson, Robert B

2013-02-01

Natural gas is the largest source of anthropogenic emissions of methane (CH(4)) in the United States. To assess pipeline emissions across a major city, we mapped CH(4) leaks across all 785 road miles in the city of Boston using a cavity-ring-down mobile CH(4) analyzer. We identified 3356 CH(4) leaks with concentrations exceeding up to 15 times the global background level. Separately, we measured δ(13)CH(4) isotopic signatures from a subset of these leaks. The δ(13)CH(4) signatures (mean = -42.8‰ ± 1.3‰ s.e.; n = 32) strongly indicate a fossil fuel source rather than a biogenic source for most of the leaks; natural gas sampled across the city had average δ(13)CH(4) values of -36.8‰ (± 0.7‰ s.e., n = 10), whereas CH(4) collected from landfill sites, wetlands, and sewer systems had δ(13)CH(4) signatures ~20‰ lighter (μ = -57.8‰, ± 1.6‰ s.e., n = 8). Repairing leaky natural gas distribution systems will reduce greenhouse gas emissions, increase consumer health and safety, and save money. Copyright © 2012 Elsevier Ltd. All rights reserved.

Methane oxidation by termite mounds estimated by the carbon isotopic composition of methane

NASA Astrophysics Data System (ADS)

Sugimoto, Atsuko; Inoue, Tetsushi; Kirtibutr, Nit; Abe, Takuya

1998-12-01

Emission rates and carbon isotope ratios of CH4, emitted by workers of termites, and of CH4, emitted from their mounds, were observed in a dry evergreen forest in Thailand to estimate the proportion of CH4 oxidized during emission through the mound. The δ13C of CH4 emitted from a termite mound (-70.9 to -82.4‰) was higher than that of CH4 emitted by workers in the mound (-85.4 to -97. l‰). Using a fractionation factor (a = 0.987) for oxidation of CH4 which was obtained in the incubation experiment, an emission factor defined as (CH4 emitted from a termite mound/CH4 produced by termites) was calculated. The emission factor obtained in each termite mound was nearly zero for Macrotermes (fungus-growing termites), of which the nest has a thick soil wall and subterrannean termites, and 0.17 to 0.47 for Termitinae (small-mound-making termites). Global CH4 emission by termites was estimated on the basis of the CH4 emission rates by workers and termite biomass with the emission factors. The calculated result was 1.5 to 7.4 Tg/y (0.3 to 1.3% of total source), which is considerably smaller than the estimate by the IPCC [1994].

Effects of matrix shrinkage and swelling on the economics of enhanced-coalbed-methane production and CO{sub 2} sequestration in coal

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gorucu, F.B.; Jikich, S.A.; Bromhal, G.S.

2007-08-15

In this work, the Palmer-Mansoori model for coal shrinkage and permeability increases during primary methane production was rewritten to also account for coal swelling caused by CO{sub 2} sorption. The generalized model was added to a compositional, dual porosity coalbed-methane reservoir simulator for primary (CBM) and ECBM production. A standard five-spot of vertical wells and representative coal properties for Appalachian coals was used. Simulations and sensitivity analyses were performed with the modified simulator for nine different parameters, including coal seam and operational parameters and economic criteria. The coal properties and operating parameters that were varied included Young's modulus, Poisson's ratio,more » cleat porosity, and injection pressure. The economic variables included CH{sub 4}, price, Col Cost, CO{sub 2} credit, water disposal cost, and interest rate. Net-present value (NPV) analyses of the simulation results included profits resulting from CH{sub 4}, production and potential incentives for sequestered CO{sub 2}, This work shows that for some coal seams, the combination of compressibility, cleat porosity, and shrinkage/swelling of the coal may have a significant impact on project economics.« less

Methane Concentrations and Biogeochemistry in Lake Sediments from Stordalen Mire, Sub-Arctic Sweden

NASA Astrophysics Data System (ADS)

Halloran, M.; DeStasio, J.; Erickson, L.; Johnson, J. E.; Varner, R. K.; Setera, J.; Prado, M. F.; Wik, M.; Crill, P. M.

2013-12-01

Lake sediments are an important global carbon sink of both allochthonous and autochthonous inputs. However, lakes are also known to emit carbon in gaseous form, most often as methane (CH4) or carbon dioxide (CO2), which are potent greenhouse gases. As northern latitudes warm, it is increasingly important to understand these gases and the sediments that store them. In July of 2013 we took 48 cores at 16 sites throughout three lakes surrounding a mire underlain by degrading permafrost in sub-arctic Sweden. The goal was to characterize the sedimentology and geochemistry of the lake sediments to better understand the production, distribution, and flux of CO2 and CH4 from these lakes. Villasjön is a shallow lake less than 1.5 meters deep, Mellan Harrsjön has a maximum depth of 7 meters and is stream-fed, and Inre Harrsjön has a maximum depth of 5 meters and is connected to Mellan Harrsjön. Published radiocarbon dates suggest that all three lakes formed approximately 3400 years ago. At each sample site, we retrieved 2 to 4 cores from the lake bottom, approximately 40-80 cm in length. The cores were sub-sampled for measurements of bulk TOC, TC, TN, TS, and CaCO3 (by difference) using a CHNS Elemental Analyzer, and grain size using a laser particle size analyzer. Headspace CO2 and CH4 by gas chromatography and infrared gas analysis (IRGA) yielded production rates and CH4 sediment concentrations. Dissolved inorganic carbon (DIC) from porewater extractions were analyzed using IRGA and stable carbon isotopes of DIC were analyzed via a Quantum Cascade Laser. The recovered sediments in the cores from all three lakes were composed of three layers: an upper layer of organic rich sediment (30-40 cm thick), a middle transition layer of mixed organic and lithogenic materials (5-10 cm thick), and a deep layer of grey lithogenic clay with less organic carbon (of variable thickness). Preliminary results from the 12 Villasjön sites indicate that CH4 is present and produced from the organic-rich layer in the upper 20-40 cm of the sediment. TOC values in this lake range from <1 to 44 wt. %. The TOC maximum (approximately 20-40 wt. %) consistently occurred at the same depth as the methane maximum, centered at ~20 cm. A TOC minimum zone (approximately 0-5 wt. %) occurs from 35-80 cm. Particle size distributions in this lake are dominated by silt and sand size fractions (>4 um). Calcium carbonate (CaCO3) concentrations varied, but the maximum always occurred in the upper 20 cm of the core. Core sites with known high lake surface methane fluxes from bubble trap measurements also show high methane concentrations in the sediment, high DIC concentrations in the pore fluids, and δ 13C signatures of CO2 ranging from 0 to 10, consistent with methanogenesis. Similar results are expected from the integration of pending sediment methane profiles with these data from the other two lakes: Mellan Harrsjön and Inre Harrsjön. Future work, including 14C dating, microbial community profiling, and δ13C signatures of CH4 will yield more insight into the biogeochemical mechanisms that regulate sediment methane distributions. 13C isotopes of methane and DIC should indicate if methane consumption through AOM or diffusion is controlling its distribution.

Prospects in straw disintegration for biogas production.

PubMed

Maroušek, Josef

2013-10-01

The pretreatment methods for enhancing biogas production from oat straw under study include hot maceration, steam explosion, and pressure shockwaves. The micropore area (9, 55, and 64 m(2) g(-1)) inhibitor formations (0, 15, and 0 mL L(-1)) as well as the overall methane yields (67, 179, and 255 CH4 VS t(-1)) were robustly analyzed. It was confirmed that the operating conditions of the steam explosion must be precisely tailored to the substrate. Furthermore, it was beneficial to prepend the hot maceration before the steam explosion and the pressure shockwaves. The second alternative may give increased methane yields (246 in comparison to 273 CH4 VS t(-1)); however, the application of pressure shockwaves still faces limitations for deployment on a commercial scale.

Clumped isotopologue constraints on the origin of methane at seafloor hot springs

NASA Astrophysics Data System (ADS)

Wang, David T.; Reeves, Eoghan P.; McDermott, Jill M.; Seewald, Jeffrey S.; Ono, Shuhei

2018-02-01

Hot-spring fluids emanating from deep-sea vents hosted in unsedimented ultramafic and mafic rock commonly contain high concentrations of methane. Multiple hypotheses have been proposed for the origin(s) of this methane, ranging from synthesis via reduction of aqueous inorganic carbon (∑CO2) during active fluid circulation to leaching of methane-rich fluid inclusions from plutonic rocks of the oceanic crust. To further resolve the process(es) responsible for methane generation in these systems, we determined the relative abundances of several methane isotopologues (including 13CH3D, a "clumped" isotopologue containing two rare isotope substitutions) in hot-spring source fluids sampled from four geochemically-distinct hydrothermal vent fields (Rainbow, Von Damm, Lost City, and Lucky Strike). Apparent equilibrium temperatures retrieved from methane clumped isotopologue analyses average 310-42+53 °C, with no apparent relation to the wide range of fluid temperatures (96-370 °C) and chemical compositions (pH, [H2], [∑CO2], [CH4]) represented. Combined with very similar bulk stable isotope ratios (13C/12C and D/H) of methane across the suite of hydrothermal fluids, all available geochemical and isotopic data suggest a common mechanism of methane generation at depth that is disconnected from active fluid circulation. Attainment of equilibrium amongst methane isotopologues at temperatures of ca. 270-360 °C is compatible with the thermodynamically-favorable reduction of CO2 to CH4 at temperatures at or below ca. 400 °C under redox conditions characterizing intrusive rocks derived from sub-ridge melts. Collectively, the observations support a model where methane-rich aqueous fluids, known to be trapped in rocks of the oceanic lithosphere, are liberated from host rocks during hydrothermal circulation and perhaps represent the major source of methane venting with thermal waters at unsedimented hydrothermal fields. The results also provide further evidence that water-rock reactions occurring at temperatures lower than 200 °C do not contribute significantly to the quantities of methane venting at mid-ocean ridge hot springs.

Microbial Abundances Predict Methane and Nitrous Oxide Fluxes from a Windrow Composting System

PubMed Central

Li, Shuqing; Song, Lina; Gao, Xiang; Jin, Yaguo; Liu, Shuwei; Shen, Qirong; Zou, Jianwen

2017-01-01

Manure composting is a significant source of atmospheric methane (CH4) and nitrous oxide (N2O) that are two potent greenhouse gases. The CH4 and N2O fluxes are mediated by methanogens and methanotrophs, nitrifying and denitrifying bacteria in composting manure, respectively, while these specific bacterial functional groups may interplay in CH4 and N2O emissions during manure composting. To test the hypothesis that bacterial functional gene abundances regulate greenhouse gas fluxes in windrow composting systems, CH4 and N2O fluxes were simultaneously measured using the chamber method, and molecular techniques were used to quantify the abundances of CH4-related functional genes (mcrA and pmoA genes) and N2O-related functional genes (amoA, narG, nirK, nirS, norB, and nosZ genes). The results indicate that changes in interacting physicochemical parameters in the pile shaped the dynamics of bacterial functional gene abundances. The CH4 and N2O fluxes were correlated with abundances of specific compositional genes in bacterial community. The stepwise regression statistics selected pile temperature, mcrA and NH4+ together as the best predictors for CH4 fluxes, and the model integrating nirK, nosZ with pmoA gene abundances can almost fully explain the dynamics of N2O fluxes over windrow composting. The simulated models were tested against measurements in paddy rice cropping systems, indicating that the models can also be applicable to predicting the response of CH4 and N2O fluxes to elevated atmospheric CO2 concentration and rising temperature. Microbial abundances could be included as indicators in the current carbon and nitrogen biogeochemical models. PMID:28373862

Methane absorption in the visible spectra of the outer planets and Titan

NASA Technical Reports Server (NTRS)

Owen, T.; Cess, R. D.

1975-01-01

New spectra of Jupiter, Saturn, and Titan show weak methane bands in the region below 6000 A which have been known for many years in the spectra of Uranus and Neptune. Adopting the known abundance of methane on Jupiter, we have used a band model to determine CH4 abundances and broadening pressures for the other objects. The results indicate high values of the CH4 to H2 concentration ratio for Uranus and Neptune; for Titan, a surface pressure in excess of 1 atm is implied.

Modeling methane emissions by cattle production systems in Mexico

NASA Astrophysics Data System (ADS)

Castelan-Ortega, O. A.; Ku Vera, J.; Molina, L. T.

2013-12-01

Methane emissions from livestock is one of the largest sources of methane in Mexico. The purpose of the present paper is to provide a realistic estimate of the national inventory of methane produced by the enteric fermentation of cattle, based on an integrated simulation model, and to provide estimates of CH4 produced by cattle fed typical diets from the tropical and temperate climates of Mexico. The Mexican cattle population of 23.3 million heads was divided in two groups. The first group (7.8 million heads), represents cattle of the tropical climate regions. The second group (15.5 million heads), are the cattle in the temperate climate regions. This approach allows incorporating the effect of diet on CH4 production into the analysis because the quality of forages is lower in the tropics than in temperate regions. Cattle population in every group was subdivided into two categories: cows (COW) and other type of cattle (OTHE), which included calves, heifers, steers and bulls. The daily CH4 production by each category of animal along an average production cycle of 365 days was simulated, instead of using a default emission factor as in Tier 1 approach. Daily milk yield, live weight changes associated with the lactation, and dry matter intake, were simulated for the entire production cycle. The Moe and Tyrrell (1979) model was used to simulate CH4 production for the COW category, the linear model of Mills et al. (2003) for the OTHE category in temperate regions and the Kurihara et al. (1999) model for the OTHE category in the tropical regions as it has been developed for cattle fed tropical diets. All models were integrated with a cow submodel to form an Integrated Simulation Model (ISM). The AFRC (1993) equations and the lactation curve model of Morant and Gnanasakthy (1989) were used to construct the cow submodel. The ISM simulates on a daily basis the CH4 production, milk yield, live weight changes associated with lactation and dry matter intake. The total daily CH4 emission per region was calculated by multiplying the number of heads of cattle in each region by their corresponding simulated emission factor, either COW or OTHE, as predicted by the ISM. The total CH4 emissions from the Mexican cattle population was then calculated by adding up the daily emissions from each region. The predicted total emission of methane produced by the 23.3 million heads of cattle in Mexico is approximately 2.02 Tg/year, from which 1.28 Tg is produced by cattle in temperate regions and the rest by cattle in the tropics. It was concluded that the modeling approach was suitable in producing a better estimate of the national methane inventory for cattle. It is flexible enough to incorporate more cattle groups or classification schemes and productivity levels.

Ammonium conversion and its feedback effect on methane oxidation of Methylosinus sporium.

PubMed

He, Ruo; Chen, Min; Ma, Ruo-Chan; Su, Yao; Zhang, Xuan

2017-04-01

Ammonium (NH 4 + ) is not only nitrogen source that can support methanotrophic growth, but also it can inhibit methane (CH 4 ) oxidation by competing with CH 4 for the active site of methane monooxygenase. NH 4 + conversion and its feedback effect on the growth and activity of methanotrophs were evaluated with Methylosinus sporium used as a model methanotroph. Nitrogen sources could affect the CH 4 -derived carbon distribution, which varied with incubation time and nitrogen concentrations. More CH 4 -derived carbon was incorporated into biomass in the media with NH 4 + -N, compared to nitrate-nitrogen (NO 3 - -N), as sole nitrogen source at the nitrogen concentrations of 10-18 mmol L -1 . Although ammonia (NH 3 ) oxidation activity of methanotrophs was considerably lower, only accounting for 0.01-0.06% of CH 4 oxidation activity in the experimental cultures, NH 4 + conversion could lead to the pH decrease and toxic intermediates accumulation in the their habits. Compared with NH 4 + , nitrite (NO 2 - ) accumulation in the NH 4 + conversion of methanotroph had stronger inhibition on its activity, especially the joint inhibition of NO 2 - accumulation and the pH decrease during the NH 4 + -N conversion. These results suggested that more attention should be paid to the feedback effects of NH 4 + conversion by methanotrophs to understand effects of NH 4 + on CH 4 oxidation in the environments. Copyright © 2017 The Society for Biotechnology, Japan. Published by Elsevier B.V. All rights reserved.

Real-time analysis of δ13C- and δD-CH4 in ambient air with laser spectroscopy: Method development and intercomparison

NASA Astrophysics Data System (ADS)

Harris, E. J.; Eyer, S.; Mohn, J.; Röckmann, T.; Popa, E.; Lowry, D.; Nisbet, E. G.; Fisher, R. E.; Brennwald, M. S.; Fischer, H.; Emmenegger, L.; Tuzson, B.; Zellweger, C.

2015-12-01

Methane (CH4) is the second most important anthropogenically emitted greenhouse gas after carbon dioxide (CO2). Its mole fraction has increased from around 722 ppb in pre-industrial times to 1824 ppb in 2013 and the anthropogenic fraction is estimated to be 60 % of the total emissions. A promising approach to improve the understanding of the CH4 budget is the use of isotopologues to distinguish between various CH4 source processes. In the presented study in situ and simultaneous measurement of the three most abundant isotopologues of methane using mid-infrared laser absorption spectroscopy is demonstrated. A field-deployable, autonomous platform is realized by coupling a compact quantum cascade laser absorption spectrometer (QCLAS) to a preconcentration unit, called TRace gas EXtractor (TREX). This unit enhances CH4 mole fractions by a factor of up to 500 above ambient levels and quantitatively separates interfering trace gases such as N2O and CO2. The analytical precision of the QCLAS isotope measurement on the preconcentrated (750 ppm, parts-per-million, mmole/mole) methane is 0.1‰ and 0.5 ‰ for δ13C- and δD-CH4 at 10 min averaging time. [1] Based on replicate measurements of compressed air during a two-week intercomparison campaign, the repeatability of the TREX-QCLAS was determined to be 0.19 ‰ and 1.9 ‰ for δ13C and δD-CH4, respectively. In this intercomparison campaign the new in situ technique is compared to IRMS based on glass flask and bag sampling and real time CH4 isotope analysis by two commercially available laser spectrometers (Figure). Both laser-based analyzers were limited to methane mole fraction and δ13C-CH4 analysis, and only one of them, a cavity ring down spectrometer, was capable to deliver meaningful data for the isotopic composition. After correcting for scale offsets, the average difference between TREX-QCLAS data and bag/flask sampling-IRMS values are within the extended WMO compatibility goals of 0.2 and 5 ‰ for δ13C- and δD-CH4, respectively. Thus, the intercomparison also reveals the need for reference air samples with accurately determined isotopic composition of CH4 to further improve the interlaboratory compatibility. [1] References: [1] S. Eyer et al. (2015) submitted to AMTD

Identification of functionally active aerobic methanotrophs in sediments from an arctic lake using stable isotope probing

USGS Publications Warehouse

He, Ruo; Wooller, Matthew J.; Pohlman, John W.; Catranis, Catharine; Quensen, John; Tiedje, James M.; Leigh, Mary Beth

2012-01-01

Arctic lakes are a significant source of the greenhouse gas methane (CH4), but the role that methane oxidizing bacteria (methanotrophs) play in limiting the overall CH4 flux is poorly understood. Here, we used stable isotope probing (SIP) techniques to identify the metabolically active aerobic methanotrophs in upper sediments (0–1 cm) from an arctic lake in northern Alaska sampled during ice-free summer conditions. The highest CH4 oxidation potential was observed in the upper sediment (0–1 cm depth) with 1.59 μmol g wet weight-1 day-1 compared with the deeper sediment samples (1–3 cm, 3–5 cm and 5–10 cm), which exhibited CH4 oxidation potentials below 0.4 μmol g wet weight-1 day-1. Both type I and type II methanotrophs were directly detected in the upper sediment total communities using targeted primer sets based on 16S rRNA genes. Sequencing of 16S rRNA genes and functional genes (pmoA and mxaF) in the 13C-DNA from the upper sediment indicated that type I methanotrophs, mainly Methylobacter, Methylosoma, Methylomonas and Methylovulum miyakonense, dominated the assimilation of CH4. Methylotrophs, including the genera Methylophilus and/or Methylotenera, were also abundant in the 13CDNA. Our results show that a diverse microbial consortium acquired carbon from CH4 in the sediments of this arctic lake.

Assimilation of atmospheric methane products into the MACC-II system: from SCIAMACHY to TANSO and IASI

NASA Astrophysics Data System (ADS)

Massart, S.; Agusti-Panareda, A.; Aben, I.; Butz, A.; Chevallier, F.; Crevosier, C.; Engelen, R.; Frankenberg, C.; Hasekamp, O.

2014-06-01

The Monitoring Atmospheric Composition and Climate Interim Implementation (MACC-II) delayed-mode (DM) system has been producing an atmospheric methane (CH4) analysis 6 months behind real time since June 2009. This analysis used to rely on the assimilation of the CH4 product from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) instrument onboard Envisat. Recently the Laboratoire de Météorologie Dynamique (LMD) CH4 products from the Infrared Atmospheric Sounding Interferometer (IASI) and the SRON Netherlands Institute for Space Research CH4 products from the Thermal And Near-infrared Sensor for carbon Observation (TANSO) were added to the DM system. With the loss of Envisat in April 2012, the DM system now has to rely on the assimilation of methane data from TANSO and IASI. This paper documents the impact of this change in the observing system on the methane tropospheric analysis. It is based on four experiments: one free run and three analyses from respectively the assimilation of SCIAMACHY, TANSO and a combination of TANSO and IASI CH4 products in the MACC-II system. The period between December 2010 and April 2012 is studied. The SCIAMACHY experiment globally underestimates the tropospheric methane by 35 part per billion (ppb) compared to the HIAPER Pole-to-Pole Observations (HIPPO) data and by 28 ppb compared the Total Carbon Column Observing Network (TCCON) data, while the free run presents an underestimation of 5 ppb and 1 ppb against the same HIPPO and TCCON data, respectively. The assimilated TANSO product changed in October 2011 from version v.1 to version v.2.0. The analysis of version v.1 globally underestimates the tropospheric methane by 18 ppb compared to the HIPPO data and by 15 ppb compared to the TCCON data. In contrast, the analysis of version v.2.0 globally overestimates the column by 3 ppb. When the high density IASI data are added in the tropical region between 30° N and 30° S, their impact is mainly positive but more pronounced and effective when combined with version v.2.0 of the TANSO products. The resulting analysis globally underestimates the column-averaged dry-air mole fractions of methane (xCH4) just under 1 ppb on average compared to the TCCON data, whereas in the tropics it overestimates xCH4 by about 3 ppb. The random error is estimated to be less than 7 ppb when compared to TCCON data.

Cross continental increase in methane ebullition under climate change.

PubMed

Aben, Ralf C H; Barros, Nathan; van Donk, Ellen; Frenken, Thijs; Hilt, Sabine; Kazanjian, Garabet; Lamers, Leon P M; Peeters, Edwin T H M; Roelofs, Jan G M; de Senerpont Domis, Lisette N; Stephan, Susanne; Velthuis, Mandy; Van de Waal, Dedmer B; Wik, Martin; Thornton, Brett F; Wilkinson, Jeremy; DelSontro, Tonya; Kosten, Sarian

2017-11-22

Methane (CH 4 ) strongly contributes to observed global warming. As natural CH 4 emissions mainly originate from wet ecosystems, it is important to unravel how climate change may affect these emissions. This is especially true for ebullition (bubble flux from sediments), a pathway that has long been underestimated but generally dominates emissions. Here we show a remarkably strong relationship between CH 4 ebullition and temperature across a wide range of freshwater ecosystems on different continents using multi-seasonal CH 4 ebullition data from the literature. As these temperature-ebullition relationships may have been affected by seasonal variation in organic matter availability, we also conducted a controlled year-round mesocosm experiment. Here 4 °C warming led to 51% higher total annual CH 4 ebullition, while diffusion was not affected. Our combined findings suggest that global warming will strongly enhance freshwater CH 4 emissions through a disproportional increase in ebullition (6-20% per 1 °C increase), contributing to global warming.

Assessing the Gap Between Top-down and Bottom-up Measured Methane Emissions in Indianapolis, IN.

NASA Astrophysics Data System (ADS)

Prasad, K.; Lamb, B. K.; Cambaliza, M. O. L.; Shepson, P. B.; Stirm, B. H.; Salmon, O. E.; Lavoie, T. N.; Lauvaux, T.; Ferrara, T.; Howard, T.; Edburg, S. L.; Whetstone, J. R.

2014-12-01

Releases of methane (CH4) from the natural gas supply chain in the United States account for approximately 30% of the total US CH4 emissions. However, there continues to be large questions regarding the accuracy of current emission inventories for methane emissions from natural gas usage. In this paper, we describe results from top-down and bottom-up measurements of methane emissions from the large isolated city of Indianapolis. The top-down results are based on aircraft mass balance and tower based inverse modeling methods, while the bottom-up results are based on direct component sampling at metering and regulating stations, surface enclosure measurements of surveyed pipeline leaks, and tracer/modeling methods for other urban sources. Mobile mapping of methane urban concentrations was also used to identify significant sources and to show an urban-wide low level enhancement of methane levels. The residual difference between top-down and bottom-up measured emissions is large and cannot be fully explained in terms of the uncertainties in top-down and bottom-up emission measurements and estimates. Thus, the residual appears to be, at least partly, attributed to a significant wide-spread diffusive source. Analyses are included to estimate the size and nature of this diffusive source.

Global Methane Biogeochemistry

NASA Astrophysics Data System (ADS)

Reeburgh, W. S.

2003-12-01

Methane (CH4) has been studied as an atmospheric constituent for over 200 years. A 1776 letter from Alessandro Volta to Father Campi described the first experiments on flammable "air" released by shallow sediments in Lake Maggiore (Wolfe, 1996; King, 1992). The first quantitative measurements of CH4, both involving combustion and gravimetric determination of trapped oxidation products, were reported in French by Boussingault and Boussingault, 1864 and Gautier (1901), who reported CH4 concentrations of 10 ppmv and 0.28 ppmv (seashore) and 95 ppmv (Paris), respectively. The first modern measurements of atmospheric CH4 were the infrared absorption measurements of Migeotte (1948), who estimated an atmospheric concentration of 2.0 ppmv. Development of gas chromatography and the flame ionization detector in the 1950s led to observations of vertical CH4 distributions in the troposphere and stratosphere, and to establishment of time-series sampling programs in the late 1970s. Results from these sampling programs led to suggestions that the concentration of CH4, as that of CO2, was increasing in the atmosphere. The possible role of CH4 as a greenhouse gas stimulated further research on CH4 sources and sinks. Methane has also been of interest to microbiologists, but findings from microbiology have entered the larger context of the global CH4 budget only recently.Methane is the most abundant hydrocarbon in the atmosphere. It plays important roles in atmospheric chemistry and the radiative balance of the Earth. Stratospheric oxidation of CH4 provides a means of introducing water vapor above the tropopause. Methane reacts with atomic chlorine in the stratosphere, forming HCl, a reservoir species for chlorine. Some 90% of the CH4 entering the atmosphere is oxidized through reactions initiated by the OH radical. These reactions are discussed in more detail by Wofsy (1976) and Cicerone and Oremland (1988), and are important in controlling the oxidation state of the atmosphere. Methane absorbs infrared radiation in the troposphere, as do CO2 and H2O, and is an important greenhouse gas (Lacis et al., 1981; Ramanathan et al., 1985).A number of review articles on atmospheric CH4 have appeared during the last 15 years. Cicerone and Oremland (1988) reviewed evidence for the temporal atmospheric increase, updated source estimates in the global CH4 budget, and placed constraints on the global budget, emphasizing that the total is well constrained, but that the constituent sources may be uncertain by a factor of 2 or more. This paper was part of a special section in Global Biogeochemical Cycles that resulted from a 1987 American Chemical Society Symposium, "Atmospheric Methane: Formation and Fluxes form the Biosphere and Geosphere." Tyler (1991) and Wahlen (1993) emphasized new information on stable isotopes of CH4 and 14CH4, respectively. Several reviews deal with the microbially mediated CH4 oxidation. King (1992) reviewed the ecology of microbial CH4 oxidation, emphasizing the important role of this process in global CH4 dynamics. R. S. Hanson and T. E. Hanson (1996) reviewed the physiology and taxonomy of methylotrophic bacteria, their role in the global carbon cycle, and the ecology of methanotrophic bacteria. Conrad (1996) reviewed the role of soils and soil microbial communities as controllers of CH4 fluxes, as well as those of H2, CO, OCS, N2O, and NO. Two meetings focusing on CH4 biogeochemistry were held in 1991: an NATO Advanced Science Workshop held at Mt. Hood, OR, and the Tenth International Symposium on Environmental Biogeochemistry (ISEB). A dedicated issue of Chemosphere (26(1-4), 1993) contains contributions from the NATO workshop; two additional volumes (Khalil, 1993 and Khalil, 2000) contain a report of the workshop and updates of important topics. Contributions to the ISEB meeting are presented in Oremland (1993). Wuebbles and Hayhoe (2002) reviewed the effects of CH4 on atmospheric chemistry and examined the direct and indirect impact of CH4 on climate. The Intergovernmental Panel on Climate Change (IPCC) has published periodic updates (see, e.g., IPCC, 2001).Substantial advances have resulted from research aimed at understanding the global CH4 mixing ratio increase. Time-series measurements of atmospheric CH4 have continued, new CH4 flux measurements in a range of environments have been reported, and data allowing use of the stable isotope (13C/12C, 2H/1H) composition of CH4 as an independent budget constraint have increased. The importance of microbial oxidation of CH4 has been recognized and modeled; the possible role of CH4 clathrate hydrates in the global budget has been clarified with the introduction of new technology. Studies of CH4 trapped in ice cores from the Greenland and Antarctic ice caps have continued, resulting in higher-resolution records and new interpretations of past conditions. There have been few recent changes in our understanding of the atmospheric chemistry of CH4, and since this is covered in Cicerone and Oremland (1988) it will not be covered here. The aim here is not to repeat information contained in the reviews mentioned above, but to present results that have appeared in the literature since their publication, to outline major questions, and to point to promising new approaches.

Estimate of methane emissions from oil and gas operations in the Uintah Basin using airborne measurements and Lidar wind data

NASA Astrophysics Data System (ADS)

Karion, A.; Sweeney, C.; Petron, G.; Frost, G. J.; Trainer, M.; Brewer, A.; Hardesty, R.; Conley, S. A.; Wolter, S.; Newberger, T.; Kofler, J.; Tans, P. P.

2012-12-01

During a February 2012 campaign in the Uintah oil and gas basin in northeastern Utah, thirteen research flights were conducted in conjunction with a variety of ground-based measurements. Using aircraft-based high-resolution (0.5 Hz) observations of methane (CH4) and carbon dioxide (CO2), along with High-Resolution Doppler Lidar wind observations from a ground site in the basin, we have calculated the basin-wide CH4 flux on several days. Uncertainty estimates are calculated for each day and are generally large for all but one flight day. On one day, February 3, uncertainty on the estimate from a mass balance approach is better than 30% due to ideal meteorological conditions, including a well-mixed boundary layer and low wind variability both in time and altitude, as determined from the Lidar wind observations. This aircraft-based mass balance approach to flux estimates is a critical and valuable tool for estimating CH4 emissions from oil and gas basins.

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moran, James J.; Whitmore, Laura M.; Jay, Zackary J.

Volcanism and post-magmatism contribute significant annual methane (CH 4) 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 CH 4 (as well as carbon dioxide (CO 2) and other gases), but the ultimate sources of this CH 4 flux have not been elucidated. In this paper, we use dual stable isotope analysis (δ 2H and δ 13C) of CH 4 sampled from ten high-temperature geothermalmore » pools in Yellowstone National Park along with other isotopic and gas analyses to evaluate potential sources of methane. The average δ 13C and δ 2H values of CH 4 emitted from hot springs ( 26.7 (± 2.4) and - 236.9 (± 12.0) ‰, respectively) are inconsistent with microbial methanogenesis but do not allow distinction between thermogenic and abiotic sources. Correlation between δ 13C CH4 and δ 13C of dissolved inorganic C (DIC) is consistent with DIC as the parent C source for the observed CH 4, or with equilibration of CH 4 and DIC. Methane formation temperatures estimated by isotopic geothermometry based on δ 13C CH4 and δ 13C CO2 ranged from ~ 250–350 °C, which is just below previous temperature estimates for the hydrothermal reservoir. Further, the δ 2H H2O of the thermal springs and the measured δ 2H CH4 values are consistent with equilibration between the source water and the CH 4 at the formation temperatures. Though the ultimate origin of the CH 4 could be attributed to either abiotic of themorgenic processes with subsequent isotopic equilibration, the C 1/C 2+ composition of the gases is more consistent with abiotic origins for most of the samples. Finally, our data support the hypothesis that subsurface rock-water interactions are responsible for at least a significant fraction of the CH 4 flux from the Yellowstone National Park volcanic system.« less

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

DOE PAGES

Moran, James J.; Whitmore, Laura M.; Jay, Zackary J.; ...

2017-05-16

Volcanism and post-magmatism contribute significant annual methane (CH 4) 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 CH 4 (as well as carbon dioxide (CO 2) and other gases), but the ultimate sources of this CH 4 flux have not been elucidated. In this paper, we use dual stable isotope analysis (δ 2H and δ 13C) of CH 4 sampled from ten high-temperature geothermalmore » pools in Yellowstone National Park along with other isotopic and gas analyses to evaluate potential sources of methane. The average δ 13C and δ 2H values of CH 4 emitted from hot springs ( 26.7 (± 2.4) and - 236.9 (± 12.0) ‰, respectively) are inconsistent with microbial methanogenesis but do not allow distinction between thermogenic and abiotic sources. Correlation between δ 13C CH4 and δ 13C of dissolved inorganic C (DIC) is consistent with DIC as the parent C source for the observed CH 4, or with equilibration of CH 4 and DIC. Methane formation temperatures estimated by isotopic geothermometry based on δ 13C CH4 and δ 13C CO2 ranged from ~ 250–350 °C, which is just below previous temperature estimates for the hydrothermal reservoir. Further, the δ 2H H2O of the thermal springs and the measured δ 2H CH4 values are consistent with equilibration between the source water and the CH 4 at the formation temperatures. Though the ultimate origin of the CH 4 could be attributed to either abiotic of themorgenic processes with subsequent isotopic equilibration, the C 1/C 2+ composition of the gases is more consistent with abiotic origins for most of the samples. Finally, our data support the hypothesis that subsurface rock-water interactions are responsible for at least a significant fraction of the CH 4 flux from the Yellowstone National Park volcanic system.« less

Climate-driven increase of natural wetland methane emissions offset by human-induced wetland reduction in China over the past three decades

USGS Publications Warehouse

Zhu, Qiuan; Peng, Changhui; Liu, Jinxun; Jiang, Hong; Fang, Xiuqin; Chen, Huai; Niu, Zhichun; Gong, Peng; Lin, Guanghui; Wang, Meng; Yang, Yanzheng; Chang, Jie; Ge, Ying; Xiang, Wenhua; Deng, Xiangwen; He, Jin-Sheng

2016-01-01

Both anthropogenic activities and climate change can affect the biogeochemical processes of natural wetland methanogenesis. Quantifying possible impacts of changing climate and wetland area on wetland methane (CH4) emissions in China is important for improving our knowledge on CH4 budgets locally and globally. However, their respective and combined effects are uncertain. We incorporated changes in wetland area derived from remote sensing into a dynamic CH4 model to quantify the human and climate change induced contributions to natural wetland CH4 emissions in China over the past three decades. Here we found that human-induced wetland loss contributed 34.3% to the CH4 emissions reduction (0.92 TgCH4), and climate change contributed 20.4% to the CH4 emissions increase (0.31 TgCH4), suggesting that decreasing CH4 emissions due to human-induced wetland reductions has offset the increasing climate-driven CH4 emissions. With climate change only, temperature was a dominant controlling factor for wetland CH4 emissions in the northeast (high latitude) and Qinghai-Tibet Plateau (high altitude) regions, whereas precipitation had a considerable influence in relative arid north China. The inevitable uncertainties caused by the asynchronous for different regions or periods due to inter-annual or seasonal variations among remote sensing images should be considered in the wetland CH4 emissions estimation.

Climate-driven increase of natural wetland methane emissions offset by human-induced wetland reduction in China over the past three decades

PubMed Central

Zhu, Qiuan; Peng, Changhui; Liu, Jinxun; Jiang, Hong; Fang, Xiuqin; Chen, Huai; Niu, Zhenguo; Gong, Peng; Lin, Guanghui; Wang, Meng; Wang, Han; Yang, Yanzheng; Chang, Jie; Ge, Ying; Xiang, Wenhua; Deng, Xiangwen; He, Jin-Sheng

2016-01-01

Both anthropogenic activities and climate change can affect the biogeochemical processes of natural wetland methanogenesis. Quantifying possible impacts of changing climate and wetland area on wetland methane (CH4) emissions in China is important for improving our knowledge on CH4 budgets locally and globally. However, their respective and combined effects are uncertain. We incorporated changes in wetland area derived from remote sensing into a dynamic CH4 model to quantify the human and climate change induced contributions to natural wetland CH4 emissions in China over the past three decades. Here we found that human-induced wetland loss contributed 34.3% to the CH4 emissions reduction (0.92 TgCH4), and climate change contributed 20.4% to the CH4 emissions increase (0.31 TgCH4), suggesting that decreasing CH4 emissions due to human-induced wetland reductions has offset the increasing climate-driven CH4 emissions. With climate change only, temperature was a dominant controlling factor for wetland CH4 emissions in the northeast (high latitude) and Qinghai-Tibet Plateau (high altitude) regions, whereas precipitation had a considerable influence in relative arid north China. The inevitable uncertainties caused by the asynchronous for different regions or periods due to inter-annual or seasonal variations among remote sensing images should be considered in the wetland CH4 emissions estimation. PMID:27892535

Biogenic methane, hydrogen escape, and the irreversible oxidation of early Earth.

PubMed

Catling, D C; Zahnle, K J; McKay, C

2001-08-03

The low O2 content of the Archean atmosphere implies that methane should have been present at levels approximately 10(2) to 10(3) parts per million volume (ppmv) (compared with 1.7 ppmv today) given a plausible biogenic source. CH4 is favored as the greenhouse gas that countered the lower luminosity of the early Sun. But abundant CH4 implies that hydrogen escapes to space (upward arrow space) orders of magnitude faster than today. Such reductant loss oxidizes the Earth. Photosynthesis splits water into O2 and H, and methanogenesis transfers the H into CH4. Hydrogen escape after CH4 photolysis, therefore, causes a net gain of oxygen [CO2 + 2H2O --> CH4 + 2O2 --> CO2 + O2 + 4H(upward arrow space)]. Expected irreversible oxidation (approximately 10(12) to 10(13) moles oxygen per year) may help explain how Earth's surface environment became irreversibly oxidized.

Ecosystem and physiological controls over methane production in northern wetlands

NASA Technical Reports Server (NTRS)

Valentine, David W.; Holland, Elisabeth A.; Schimel, David S.

1994-01-01

Peat chemistry appears to exert primary control over methane production rates in the Canadian Northern Wetlands Study (NOWES) area. We determined laboratory methane production rate potentials in anaerobic slurries of samples collected from a transect of sites through the NOWES study area. We related methane production rates to indicators of resistance to microbial decay (peat C: N and lignin: N ratios) and experimentally manipulated substrate availability for methanogenesis using ethanol (EtOH) and plant litter. We also determined responses of methane production to pH and temperature. Methane production potentials declined along the gradient of sites from high rates in the coastal fens to low rates in the interior bogs and were generally highest in surface layers. Strong relationships between CH4 production potentials and peat chemistry suggested that methanogenesis was limited by fermentation rates. Methane production at ambient pH responded strongly to substrate additions in the circumneutral fens with narrow lignin: N and C: N ratios (delta CH4/delta EtOH = 0.9-2.3 mg/g) and weakly in the acidic bogs with wide C: N and lignin: N ratios (delta CH4/delta EtOH = -0.04-0.02 mg/g). Observed Q(sub 10) values ranged from 1.7 to 4.7 and generally increased with increasing substrate availability, suggesting that fermentation rates were limiting. Titration experiments generally demonstrated inhibition of methanogenesis by low pH. Our results suggest that the low rates of methane emission observed in interior bogs during NOWES likely resulted from pH and substrate quality limitation of the fermentation step in methane production and thus reflect intrinsically low methane production potentials. Low methane emission rates observed during NOWES will likely be observed in other northern wetland regions with similar vegetation chemistry.

Variability in methane emissions from West Siberia's shallow boreal lakes on a regional scale and its environmental controls

NASA Astrophysics Data System (ADS)

Sabrekov, Aleksandr F.; Runkle, Benjamin R. K.; Glagolev, Mikhail V.; Terentieva, Irina E.; Stepanenko, Victor M.; Kotsyurbenko, Oleg R.; Maksyutov, Shamil S.; Pokrovsky, Oleg S.

2017-08-01

Small lakes represent an important source of atmospheric CH4 from northern wetlands. However, spatiotemporal variations in flux magnitudes and the lack of knowledge about their main environmental controls contribute large uncertainty into the global CH4 budget. In this study, we measured methane fluxes from small lakes using chambers and bubble traps. Field investigations were carried out in July-August 2014 within the West Siberian middle and southern taiga zones. The average and median of measured methane chamber fluxes were 0.32 and 0.30 mgCH4 m-2 h-1 for middle taiga lakes and 8.6 and 4.1 mgCH4 m-2 h-1 for southern taiga lakes, respectively. Pronounced flux variability was found during measurements on individual lakes, between individual lakes and between zones. To analyze these differences and the influences of environmental controls, we developed a new dynamic process-based model. It shows good performance with emission rates from the southern taiga lakes and poor performance for individual lakes in the middle taiga region. The model shows that, in addition to well-known controls such as temperature, pH and lake depth, there are significant variations in the maximal methane production potential between these climatic zones. In addition, the model shows that variations in gas-filled pore space in lake sediments are capable of controlling the total methane emissions from individual lakes. The CH4 emissions exhibited distinct zonal differences not only in absolute values but also in their probability density functions: the middle taiga lake fluxes were best described by a lognormal distribution while the southern taiga lakes followed a power-law distribution. The latter suggests applicability of self-organized criticality theory for methane emissions from the southern taiga zone, which could help to explain the strong variability within individual lakes.

The variations of Oxidation-Reduction Potential in paddy soil and effects on the methane emission from a periodically irrigated paddy field.

NASA Astrophysics Data System (ADS)

Yagi, K.; Iwata, T.; Wakikuromaru, N.

2014-12-01

Paddy fields are one of the most important eco-system in monsoon Asia and one of the largest source of CH4 emission. CH4 has significant contribution to the global warming next to CO2 and its greenhouse effect is about 21 times as large as same amount of CO2. CH4 is generated by decomposition of organic matter in soil under anaerobic condition. Oxidation-Reduction Potential (ORP) is the most suitable index representing soil aerobic condition. Or, CH4 is more generated under lower ORP conditions. In this study, ORP in paddy soil was measured during rice cultivated season at a periodically irrigated paddy field, and some effects on the methane flux from the paddy soil was investigated. 3-days flood and 4-days drained condition were regularly repeated at the site from late-June to early October. ORP under flooded condition was measured during irrigated term in 2013 at two mode; regular interval measurement every 2 weeks and intensive measurements during two flooded periods. Methane flux was also measured by the aerodynamic gradient technique. ORP showed rapid decrease when irrigation water was introduced in the paddy field, and lower ORP was shown under the longer flooded condition. From the seasonal-term point of view, lower ORP was shown in later rice season. ORP was suitably modeled as a function of irrigation time. During an irrigation period for four days, higher methane emissions were shown under lower OPR conditions as shown in Fig.1. From the seasonal-term point of view, however, no significant relationship between ORP and methane fluxes. Rapid rise of CH4 flux in early August and gradual decrease between late August and September were shown. It is suggested that seasonal change of methane flux is affected by seasonal changes of soil temperature or the growth level of rice plants.

Separating methane emissions from agricultural sources and natural gas: direct measurements of excess columns of CH4, C2H6 and NH3 in the Colorado Front Range

NASA Astrophysics Data System (ADS)

Kille, N.; Chiu, R.; Frey, M.; Hase, F.; Kumar Sha, M.; Blumenstock, T.; Hannigan, J. W.; Volkamer, R. M.

2017-12-01

Methane (CH4) is a major greenhouse gas emitted from biogenic, thermogenic, and pyrogenic sources. Here we demonstrate a novel approach to separate sources of CH4 emissions based on a network of small portable sensors performing column measurements in the Northern Colorado Front Range (NCFR). In the study area CH4 is emitted from biogenic sources such as concentrated animal feeding operations (CAFOs) and natural gas production and storage. In March 2015 we deployed a network of five Fourier Transform Spectrometers (FTS) to characterize the regional scale methane dome in Colorado's Denver-Julesburg Basin based on excess vertical column measurements (the column enhancement inside the dome over background). Three EM27sun FTS measured CH4, oxygen (O2) and water vapor (H2O) columns at Eaton, CO (inside the dome) and at two boundary sites; the CU mobile SOF (Solar Occultation Flux) measured ethane (C2H6), ammonia (NH3), and H2O at Eaton, CO. The column averaged dry air mole fractions XCH4, XC2H6, and XNH3 were determined using O2 columns for air mass factor normalization, and background column was subtracted to derive excess vertical columns of DXCH4, DXC2H6, DXNH3 at Eaton, CO. Eaton is located both near CAFOs and at the northern edge of oil and natural gas production wells. Our approach for source apportioning methane employs a linear regression analysis that explains DXCH4 in terms of DXC2H6 as tracer for natural gas sources, and DXNH3 as tracer for CAFO emissions. The results of the source apportionment are compared with literature values of the NH3/CH4 and C2H6/CH4 ratio to evaluate the method of excess columns, which is independent of boundary layer height.

Effects of Methane-Rich Saline on the Capability of One-Time Exhaustive Exercise in Male SD Rats

PubMed Central

Xin, Lei; Sun, Xuejun; Lou, Shujie

2016-01-01

Purpose To explore the effects of methane-rich saline (CH4 saline) on the capability of one-time exhaustive exercise in male SD rats. Methods Thirty rats were equally divided into to three groups at random: control group (C), placebo group (P) and methane saline group (M). Rats in M group underwent intraperitoneal injection of CH4 saline, and the other two groups simultaneously underwent intraperitoneal injection of normal saline. Then, the exercise capability of rats was tested through one-time exhaustive treadmill exercise except C group. Exercise time and body weight were recorded before and after one-time exhaustive exercise. After exhaustive exercise, the blood and gastrocnemius samples were collected from all rats to detect biochemical parameters in different methods. Results It was found that the treadmill running time was significantly longer in rats treated with CH4 saline. At the same time, CH4 saline reduced the elevation of LD and UN in blood caused by one-time exhaustive exercise. The low level of blood glucose induced by exhaustive exercise was also normalized by CH4 saline. Also CH4 saline lowered the level of CK in plasma. Furthermore, this research indicated that CH4 saline markedly increased the volume of T-AOC in plasma and alleviated the peak of TNF-α in both plasma and gastrocnemius. From H&E staining, CH4 saline effectively improved exercise-induced structural damage in gastrocnemius. Conclusions CH4 saline could enhance exercise capacity in male SD rats through increase of glucose aerobic oxidation, improvement of metabolic clearance and decrease of exhaustive exercise-induced gastrocnemius injury. PMID:26942576

Estimates of methane emissions from India using CH4-CO-C2H6 relationships from CARIBIC observations in monsoon convective outflow

NASA Astrophysics Data System (ADS)

Baker, A. K.; Rauthe-Schöch, A.; Schuck, T. J.; van Velthoven, P. F.; Slemr, F.; Brenninkmeijer, C. A.

2010-12-01

A large fraction of methane sources are anthropogenic, and include fossil fuel use, biomass/biofuel burning, agriculture and waste treatment. Recently, much attention regarding emissions of greenhouse gases has focused on large, developing nations, as their emissions are expected to rise rapidly over the coming decades. As the second most populous country in the world, and one of the fastest growing economies, India has been of particular interest. Arguably the most important feature of meteorology in India is the Asian summer monsoon. During the monsoon period there exists persistent deep convection over Southern Asia, and the composition of convected air masses is strongly influenced by emissions from India. This ultimately results in a well-mixed air parcel containing air from India being transported to the upper troposphere. Over the course of the 2008 monsoon period the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) passenger aircraft conducted monthly measurement flights which probed this outflow. Data collected during these flights provides a unique opportunity to examine sources of atmospheric species in India. Here we use measurements of methane (CH4), carbon monoxide (CO) and ethane (C2H6) from whole air samples collected during CARIBIC flights to estimate emissions of methane and to quantify those emissions related to flooding during the monsoon. Methane data from the monsoon period show enhancements inside the monsoon plume, which increase as the monsoon progresses. Using emission data for CO and ΔCH4/ΔCO derived from CARIBIC measurements, we estimate total methane emissions to be ~40 Tg yr-1. Relationships of methane to ethane, which shares the bulk of its sources with methane but lacks a biological component, are further used to estimate the fraction of “extra” emissions from biological activity related to increased monsoon rains. This additional methane is a considerable fraction of total methane emissions. As emissions from rice paddies, which are not restricted to the monsoon season, are estimated to be 4±2 Tg yr-1, we expect that the additional methane emitted during the monsoon season is a product of anaerobic microbial activity related to persistent and widespread flooding during the monsoon, although the exact sources cannot be identified from our data.

Stable isotope and microbial analyses of methane-producing process in a geothermal aquifer associated with the subsurface of the accretionary prism, Japan

NASA Astrophysics Data System (ADS)

Hattori, S.; Kimura, H.; Nashimoto, H.; Koba, K.; Yamada, K.; Shimizu, M.; Watanabe, H.; Yoh, M.; Yoshida, N.

2009-04-01

The sedimentary layer in the southern part of Japan is accretionary prism which includes enriched organic materials derived from sediment on oceanic plate. There is geothermal aquifer in which a large amount of methane (CH4) dissolved. Since CH4 is important as a greenhouse gas and an important natural gas fuel, revealing CH4-producing process in subsurface environment is required. To understand the process of the CH4 production, we collected the groundwater from the aquifer of 1,189-1,489 m depth, and analyzed by using stable isotope and microbial analyses. 16S rRNA gene analysis showed a dominancy of hydrogenotrophic methanogens in domain Archaea and a dominancy of anaerobic heterotrophes to be known to produce H2 and CO2 by fermentation process in domain Bacteria. The anaerobic enrichment cultures with the groundwater amended with organic substrates showed that CH4 was produced by co-culture between the fermenters and hydrogenotrophic methanogens. On the other hand, conventional isotopic estimations for the origin of CH4 using δ13C-CH4 and δD-CH4 as well as δ13C-CH4and molecular ratio of C1/(C2+C3) indicated that CH4 was derived from thermogenic pathway. The values of δ13C-CO2, however, had higher values and carbon isotope fractionation factors between CH4 and CO2(α(CO2-CH4)) were approximately 1.05 to 1.06 indicating the possibility of biogenic CH4 production. Therefore, the origin of CH4 production was estimated as mixing both thermogenic and CO2 reduction from isotopic data. Furthermore, we incubated these enriched co-cultures and measure stable carbon isotope ratios of CH4 and CO2 and stable hydrogen isotope ratios of H2O and CH4. We revealed that concentration of H2 were kept lower by these co-cultures between fermenters and hydrogenotrophic methanogens and α(CO2-CH4) values were higher than that of cultures with the ground water amended with high concentration of H2+ CO2. Hydrogen isotope fractionation factor between H2O and CH4 by these co-culture increased (αH values decreased) with increasing H2 concentration.

High methane emissions from a midlatitude reservoir draining an agricultural watershed.

PubMed

Beaulieu, Jake J; Smolenski, Rebecca L; Nietch, Christopher T; Townsend-Small, Amy; Elovitz, Michael S

2014-10-07

Reservoirs are a globally significant source of methane (CH4), although most measurements have been made in tropical and boreal systems draining undeveloped watersheds. To assess the magnitude of CH4 emissions from reservoirs in midlatitude agricultural regions, we measured CH4 and carbon dioxide (CO2) emission rates from William H. Harsha Lake (Ohio, U.S.A.), an agricultural impacted reservoir, over a 13 month period. The reservoir was a strong source of CH4 throughout the year, emitting on average 176 ± 36 mg C m(-2) d(-1), the highest reservoir CH4 emissions profile documented in the United States to date. Contrary to our initial hypothesis, the largest CH4 emissions were during summer stratified conditions, not during fall turnover. The river-reservoir transition zone emitted CH4 at rates an order of magnitude higher than the rest of the reservoir, and total carbon emissions (i.e., CH4 + CO2) were also greater at the transition zone, indicating that the river delta supported greater carbon mineralization rates than elsewhere. Midlatitude agricultural impacted reservoirs may be a larger source of CH4 to the atmosphere than currently recognized, particularly if river deltas are consistent CH4 hot spots. We estimate that CH4 emissions from agricultural reservoirs could be a significant component of anthropogenic CH4 emissions in the U.S.A.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mugedo, J.Z.A.

Termites are reported to emit large quantities of methane, carbon dioxide, carbon monoxide, hydrogen and dimethyl sulfide. The emission of other trace gases, namely C{sub 2} to C{sub 10} hydrocarbons, is also documented. We have carried out, both in the field and in the laboratory, measurements of methane emissions by Macrotermes subhyalinus (Macrotermitinae), Trinervitermes bettonianus (Termitinae), and unidentified Cubitermes and Microcerotermes species. Measured CH{sub 4} field flux rates ranged from 3.66 to 98.25g per m{sup 2} of termite mound per year. Laboratory measurements gave emission rates that ranged from 14.61 to 165.05 mg CH{sub 4} per termite per year. Gaseousmore » production in all species sampled varied both within species and from species to species. Recalculated global emission of methane from termites was found to be 14.0 x 10{sup 12} g CH{sub 4}, per year. From our study, termites contribution to atmospheric methane content is between 1.11% and 4.25% per year. This study discusses the greenhouse effects as well as photochemical disposal of methane in the lower atmosphere in the tropics and the impacts on the chemistry of HO{sub x} systems and CL{sub x} cycles.« less

Seasonal and diel variations of ammonia and methane emissions from a naturally ventilated dairy building and the associated factors influencing emissions.

PubMed

Saha, C K; Ammon, C; Berg, W; Fiedler, M; Loebsin, C; Sanftleben, P; Brunsch, R; Amon, T

2014-01-15

Understanding seasonal and diel variations of ammonia (NH3) and methane (CH4) emissions from a naturally ventilated dairy (NVD) building may lead to develop successful control strategies for reducing emissions throughout the year. The main objective of this study was to quantify seasonal and diel variations of NH3 and CH4 emissions together with associated factors influencing emissions. Measurements were carried out with identical experimental set-up to cover three winter, spring and summer seasons, and two autumn seasons in the years 2010, 2011, and 2012. The data from 2010 and 2011 were used for developing emission prediction models and the data from 2012 were used for model validation. The results showed that NH3 emission varied seasonally following outside temperature whereas CH4 emission did not show clear seasonal trend. Diel variation of CH4 emission was less pronounced than NH3. The average NH3 and CH4 emissions between 6a.m. and 6p.m. were 66% and 33% higher than the average NH3 and CH4 emissions between 6p.m. and 6a.m., respectively for all seasons. The significant relationships (P<0.0001) between NH3 and influencing factors were found including outside temperature, humidity, wind speed and direction, hour of the day and day of the year. The significant effect (P<0.0001) of climate factors, hours of the day and days of the year on CH4 emission might be directly related to activities of the cows. © 2013.

Genetic correlations between methane production and fertility, health, and body type traits in Danish Holstein cows.

PubMed

Zetouni, L; Kargo, M; Norberg, E; Lassen, J

2018-03-01

Our aim was to investigate the genetic correlations between CH 4 production and body conformation, fertility, and health traits in dairy cows. Data were collected from 10 commercial Holstein herds in Denmark, including 5,758 cows with records for body conformation traits, 7,390 for fertility traits, 7,439 for health traits, and 1,397 with individual CH 4 measurements. Methane production was measured during milking in automatic milking systems, using a sniffer approach. Correlations between CH 4 and several different traits were estimated. These traits were interval between calving and first insemination, interval between first and last insemination, number of inseminations, udder diseases, other diseases, height, body depth, chest width, dairy character, top line, and body condition score. Bivariate linear models were used to estimate the genetic parameters within and between CH 4 and the other traits. In general, the genetic correlations between CH 4 and the traits investigated were low. The heritability of CH 4 was 0.25, and ranged from 0.02 to 0.07 for fertility and health traits, and from 0.17 to 0.74 for body conformation traits. Further research with a larger data set should be performed to more accurately establish how CH 4 relates to fertility, health, and body conformation traits in dairy cattle. This will be useful in the design of future breeding goals that consider the production of CH 4 . The Authors. Published by the Federation of Animal Science Societies and Elsevier Inc. on behalf of the American Dairy Science Association®. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/3.0/).

Evaluation and characterization of the methane-carbon dioxide decomposition reaction

NASA Technical Reports Server (NTRS)

Davenport, R. J.; Schubert, F. H.; Shumar, J. W.; Steenson, T. S.

1975-01-01

A program was conducted to evaluate and characterize the carbon dioxide-methane (CO2-CH4) decomposition reaction, i.e., CO2 + CH4 = 2C + 2H2O. The primary objective was to determine the feasibility of applying this reaction at low temperatures as a technique for recovering the oxygen (O2) remaining in the CO2 which exits mixed with CH4 from a Sabatier CO2 reduction subsystem (as part of an air revitalization system of a manned spacecraft). A test unit was designed, fabricated, and assembled for characterizing the performance of various catalysts for the reaction and ultraviolet activation of the CH4 and CO2. The reactor included in the test unit was designed to have sufficient capacity to evaluate catalyst charges of up to 76 g (0.17 lb). The test stand contained the necessary instrumentation and controls to obtain the data required to characterize the performance of the catalysts and sensitizers tested: flow control and measurement, temperature control and measurement, product and inlet gas analysis, and pressure measurement. A product assurance program was performed implementing the concepts of quality control and safety into the program effort.

Response of the global climate to changes in atmospheric chemical composition due to fossil fuel burning

NASA Technical Reports Server (NTRS)

Hameed, S.; Cess, R. D.; Hogan, J. S.

1980-01-01

Recent modeling of atmospheric chemical processes (Logan et al, 1978; Hameed et al, 1979) suggests that tropospheric ozone and methane might significantly increase in the future as the result of increasing anthropogenic emissions of CO, NO(x), and CH4 due to fossil fuel burning. Since O3 and CH4 are both greenhouse gases, increases in their concentrations could augment global warming due to larger future amounts of atmospheric CO2. To test the possible climatic impact of changes in tropospheric chemical composition, a zonal energy-balance climate model has been combined with a vertically averaged tropospheric chemical model. The latter model includes all relevant chemical reactions which affect species derived from H2O, O2, CH4, and NO(x). The climate model correspondingly incorporates changes in the infrared heating of the surface-troposphere system resulting from chemically induced changes in tropospheric ozone and methane. This coupled climate-chemical model indicates that global climate is sensitive to changes in emissions of CO, NO(x) and CH4, and that future increases in these emissions could augment global warming due to increasing atmospheric CO2.

H2O-CH4 and H2S-CH4 complexes: a direct comparison through molecular beam experiments and ab initio calculations.

PubMed

Cappelletti, David; Bartocci, Alessio; Frati, Federica; Roncaratti, Luiz F; Belpassi, Leonardo; Tarantelli, Francesco; Lakshmi, Prabha Aiswarya; Arunan, Elangannan; Pirani, Fernando

2015-11-11

New molecular beam scattering experiments have been performed to measure the total (elastic plus inelastic) cross sections as a function of the velocity in collisions between water and hydrogen sulfide projectile molecules and the methane target. Measured data have been exploited to characterize the range and strength of the intermolecular interaction in such systems, which are of relevance as they drive the gas phase molecular dynamics and the clathrate formation. Complementary information has been obtained by rotational spectra, recorded for the hydrogen sulfide-methane complex, with a pulsed nozzle Fourier transform microwave spectrometer. Extensive ab initio calculations have been performed to rationalize all the experimental findings. The combination of experimental and theoretical information has established the ground for the understanding of the nature of the interaction and allows for its basic components to be modelled, including charge transfer, in these weakly bound systems. The intermolecular potential for H2S-CH4 is significantly less anisotropic than for H2O-CH4, although both of them have potential minima that can be characterized as 'hydrogen bonded'.

Modeling the impediment of methane ebullition bubbles by seasonal lake ice

DOE Office of Scientific and Technical Information (OSTI.GOV)

Greene, S.; Walter Anthony, K. M.; Archer, D.

Microbial methane (CH 4) ebullition (bubbling) from anoxic lake sediments comprises a globally significant flux to the atmosphere, but ebullition bubbles in temperate and polar lakes can be trapped by winter ice cover and later released during spring thaw. This "ice-bubble storage" (IBS) constitutes a novel mode of CH 4 emission. Before bubbles are encapsulated by downward-growing ice, some of their CH 4 dissolves into the lake water, where it may be subject to oxidation. We present field characterization and a model of the annual CH 4 cycle in Goldstream Lake, a thermokarst (thaw) lake in interior Alaska. We findmore » that summertime ebullition dominates annual CH 4 emissions to the atmosphere. Eighty percent of CH 4 in bubbles trapped by ice dissolves into the lake water column in winter, and about half of that is oxidized. The ice growth rate and the magnitude of the CH 4 ebullition flux are important controlling factors of bubble dissolution. Seven percent of annual ebullition CH 4 is trapped as IBS and later emitted as ice melts. In a future warmer climate, there will likely be less seasonal ice cover, less IBS, less CH 4 dissolution from trapped bubbles, and greater CH 4 emissions from northern lakes.« less

Modeling the impediment of methane ebullition bubbles by seasonal lake ice

DOE PAGES

Greene, S.; Walter Anthony, K. M.; Archer, D.; ...

2014-12-08

Microbial methane (CH 4) ebullition (bubbling) from anoxic lake sediments comprises a globally significant flux to the atmosphere, but ebullition bubbles in temperate and polar lakes can be trapped by winter ice cover and later released during spring thaw. This "ice-bubble storage" (IBS) constitutes a novel mode of CH 4 emission. Before bubbles are encapsulated by downward-growing ice, some of their CH 4 dissolves into the lake water, where it may be subject to oxidation. We present field characterization and a model of the annual CH 4 cycle in Goldstream Lake, a thermokarst (thaw) lake in interior Alaska. We findmore » that summertime ebullition dominates annual CH 4 emissions to the atmosphere. Eighty percent of CH 4 in bubbles trapped by ice dissolves into the lake water column in winter, and about half of that is oxidized. The ice growth rate and the magnitude of the CH 4 ebullition flux are important controlling factors of bubble dissolution. Seven percent of annual ebullition CH 4 is trapped as IBS and later emitted as ice melts. In a future warmer climate, there will likely be less seasonal ice cover, less IBS, less CH 4 dissolution from trapped bubbles, and greater CH 4 emissions from northern lakes.« less

Seasonal trends and environmental controls of methane emissions in a rice paddy field in Northern Italy

NASA Astrophysics Data System (ADS)

Meijide, A.; Manca, G.; Goded, I.; Magliulo, V.; di Tommasi, P.; Seufert, G.; Cescatti, A.

2011-09-01

Rice paddy fields are one of the greatest anthropogenic sources of methane (CH4), the third most important greenhouse gas after water vapour and carbon dioxide. In agricultural fields, CH4 is usually measured with the closed chamber technique, resulting in discontinuous series of measurements performed over a limited area, that generally do not provide sufficient information on the short-term variation of the fluxes. On the contrary, aerodynamic techniques have been rarely applied for the measurement of CH4 fluxes in rice paddy fields. The eddy covariance (EC) technique provides integrated continuous measurements over a large area and may increase our understanding of the underlying processes and diurnal and seasonal pattern of CH4 emissions in this ecosystem. For this purpose a Fast Methane Analyzer (Los Gatos Research Ltd.) was installed in an eddy-covariance field set-up in a rice paddy field in the Po Valley (Northern Italy). Methane fluxes were measured during the rice growing season, both with EC and with manually operated closed chambers. Methane fluxes were strongly influenced by the presence of the water table, with emissions peaking when it was above 10-12 cm. Further studies are required to evaluate if water table management could decrease CH4 emissions. The development of rice plants and soil temperature were also responsible of the seasonal variation on the fluxes. The EC measured showed a diurnal cycle in the emissions, which was more relevant during the vegetative period, and with CH4 emissions being higher in the late evening, possibly associated with higher water temperature. The comparison between both measurement techniques shows that greater fluxes are measured with the chambers, especially when higher fluxes are being produced, resulting in 30 % higher seasonal estimations with the chambers than with the EC (41.1 and 31.8 g CH4 m-2 measured with chambers and EC respectively). The differences may be a result of the combined effect of overestimation with the chambers, the possible underestimation by the EC technique and of not having considered the daily course of the fluxes for the calculation of seasonal emissions from chambers.

Soil Methane uptake Model (MeMo): a process based model for global methane consumption by soils

NASA Astrophysics Data System (ADS)

Murguia-Flores, F.; Arndt, S.; Ganesan, A.; Hornibrook, E. R. C.; Murray-Tortarolo, G.

2016-12-01

Atmospheric methane (CH4) is a powerful greenhouse gas, responsible for 20% of global warming. The only terrestrial and biological sink is the uptake in the soils by methanotrophic bacteria, however there is large spatial and temporal heterogeneity in the magnitude of this sink. One way to provide a global understanding of this process is by using a mathematical model to simulate the mechanisms of the underlying physical and biological drivers. Here we present the soil Methane uptake Model (MeMo) a process-based model for the global methane consumption by soils. We have built on previous models by Ridgwell et al., (1999) and Curry et al., (2007), by making several advances. First, a general analytical solution of the one-dimensional diffusion-reaction equation was implemented that accounts for a maximum uptake depth and for a CH4 flux coming from below the surface (i.e. CH4 production in the soil). Secondly, we revisited and improved the effect of nitrogen inhibition, soil moisture and soil temperature on CH4 uptake in the light of newly available data and advances in our understanding of these drivers. Using observed forcing data, we estimated a global mean CH4 uptake of 31.2±1.2 Tg y-1 for the period 1990-2009 with an increasing trend of 0.1 Tg y-2. Our model represented the latitudinal pattern of uptake shown by field observations, with the highest uptake per unit area occurring over dry tropical forest and the lowest uptake in the polar desert. The highest seasonality occurred in the Northern Hemisphere, showing that the main driver of variability in a given year is from a combination of temperature and soil moisture. Our model showed that CH4 uptake is reduced from previous studies by approximately 10% at the regions with the highest nitrogen deposition: East Asia and Europe. Finally, our results suggest that more field measurements are needed to improve the modelling of the process, such as the basal oxidation rate for different ecosystems, the Q10 temperature response across different conditions and long term field CH4 uptake records.

Atmospheric methane isotopic record favors fossil sources flat in 1980s and 1990s with recent increase.

PubMed

Rice, Andrew L; Butenhoff, Christopher L; Teama, Doaa G; Röger, Florian H; Khalil, M Aslam K; Rasmussen, Reinhold A

2016-09-27

Observations of atmospheric methane (CH4) since the late 1970s and measurements of CH4 trapped in ice and snow reveal a meteoric rise in concentration during much of the twentieth century. Since 1750, levels of atmospheric CH4 have more than doubled to current globally averaged concentration near 1,800 ppb. During the late 1980s and 1990s, the CH4 growth rate slowed substantially and was near or at zero between 1999 and 2006. There is no scientific consensus on the drivers of this slowdown. Here, we report measurements of the stable isotopic composition of atmospheric CH4 ((13)C/(12)C and D/H) from a rare air archive dating from 1977 to 1998. Together with more modern records of isotopic atmospheric CH4, we performed a time-dependent retrieval of methane fluxes spanning 25 y (1984-2009) using a 3D chemical transport model. This inversion results in a 24 [18, 27] Tg y(-1) CH4 increase in fugitive fossil fuel emissions since 1984 with most of this growth occurring after year 2000. This result is consistent with some bottom-up emissions inventories but not with recent estimates based on atmospheric ethane. In fact, when forced with decreasing emissions from fossil fuel sources our inversion estimates unreasonably high emissions in other sources. Further, the inversion estimates a decrease in biomass-burning emissions that could explain falling ethane abundance. A range of sensitivity tests suggests that these results are robust.

Atmospheric methane isotopic record favors fossil sources flat in 1980s and 1990s with recent increase

NASA Astrophysics Data System (ADS)

Rice, Andrew L.; Butenhoff, Christopher L.; Teama, Doaa G.; Röger, Florian H.; Khalil, M. Aslam K.; Rasmussen, Reinhold A.

2016-09-01

Observations of atmospheric methane (CH4) since the late 1970s and measurements of CH4 trapped in ice and snow reveal a meteoric rise in concentration during much of the twentieth century. Since 1750, levels of atmospheric CH4 have more than doubled to current globally averaged concentration near 1,800 ppb. During the late 1980s and 1990s, the CH4 growth rate slowed substantially and was near or at zero between 1999 and 2006. There is no scientific consensus on the drivers of this slowdown. Here, we report measurements of the stable isotopic composition of atmospheric CH4 (13C/12C and D/H) from a rare air archive dating from 1977 to 1998. Together with more modern records of isotopic atmospheric CH4, we performed a time-dependent retrieval of methane fluxes spanning 25 y (1984-2009) using a 3D chemical transport model. This inversion results in a 24 [18, 27] Tg y-1 CH4 increase in fugitive fossil fuel emissions since 1984 with most of this growth occurring after year 2000. This result is consistent with some bottom-up emissions inventories but not with recent estimates based on atmospheric ethane. In fact, when forced with decreasing emissions from fossil fuel sources our inversion estimates unreasonably high emissions in other sources. Further, the inversion estimates a decrease in biomass-burning emissions that could explain falling ethane abundance. A range of sensitivity tests suggests that these results are robust.

Physical and Biological Carbon Isotope Fractionation in Methane During Gas-Push-Pull-Tests

NASA Astrophysics Data System (ADS)

Gonzalez-Gil, G.; Schroth, M. H.; Gomez, K.; Zeyer, J.

2005-12-01

Stable isotope analyses have become a common tool to assess microbially-mediated processes in subsurface environments. We investigated if stable carbon isotope analysis can be used as a tool to complement gas push-pull tests (GPPTs), a novel technique that was recently developed and tested for the in-situ quantification of CH4 oxidation in soils. During a GPPT a gas mixture containing CH4, O2 and nonreactive tracer gases is injected into the soil, where CH4 is oxidized by indigenous microorganisms. Thereafter, a blend of injected gas mixture and soil air is extracted from the same location, and CH4 oxidation is quantified from an analysis of extracted CH4 and tracer gases. To assess the magnitude of physical isotope fractionation due to molecular diffusion during GPPTs, we conducted laboratory experiments in the absence of microbial activity in a 1m-high, 1m-diameter tank filled with dry sand. During the GPPTs' extraction phase, the isotopic composition of methane was analyzed. Results indicated strong carbon isotope fractionation (>20 per mil) during GPPTs. To assess the combined effect of physical and biological isotope fractionation, numerical simulations of GPPTs were conducted in which microbial CH4 isotope fractionation was simulated using first-order rate constants and microbial kinetic isotope fractionation factors previously reported for methane oxidation in landfill environments. Results of these simulations indicated that for small CH4 oxidation rates, overall isotope fractionation in CH4 is dominated by physical fractionation. Conversely, for high CH4 oxidation rates, overall fractionation is dominated by biological fractionation. Thus, CH4 isotope fractionation data alone from a single GPPT cannot be used to assess microbial CH4 oxidation. However, biological fractionation may be quantified if physical fractionation due to diffusion is known. This can be achieved by conducting two sequential GPPTs, with microbial activity being inhibited in the second test.

Response of global soil consumption of atmospheric methane to changes in atmospheric climate and nitrogen deposition

USGS Publications Warehouse

Zhuang, Qianlai; Chen, Min; Xu, Kai; Tang, Jinyun; Saikawa, Eri; Lu, Yanyu; Melillo, Jerry M.; Prinn, Ronald G.; McGuire, A. David

2013-01-01

Soil consumption of atmospheric methane plays an important secondary role in regulating the atmospheric CH4 budget, next to the dominant loss mechanism involving reaction with the hydroxyl radical (OH). Here we used a process-based biogeochemistry model to quantify soil consumption during the 20th and 21st centuries. We estimated that global soils consumed 32–36 Tg CH4 yr−1 during the 1990s. Natural ecosystems accounted for 84% of the total consumption, and agricultural ecosystems only consumed 5 Tg CH4 yr−1 in our estimations. During the twentieth century, the consumption rates increased at 0.03–0.20 Tg CH4 yr−2 with seasonal amplitudes increasing from 1.44 to 3.13 Tg CH4 month−1. Deserts, shrublands, and xeric woodlands were the largest sinks. Atmospheric CH4 concentrations and soil moisture exerted significant effects on the soil consumption while nitrogen deposition had a moderate effect. During the 21st century, the consumption is predicted to increase at 0.05-1.0 Tg CH4 yr−2, and total consumption will reach 45–140 Tg CH4 yr−1 at the end of the 2090s, varying under different future climate scenarios. Dry areas will persist as sinks, boreal ecosystems will become stronger sinks, mainly due to increasing soil temperatures. Nitrogen deposition will modestly reduce the future sink strength at the global scale. When we incorporated the estimated global soil consumption into our chemical transport model simulations, we found that nitrogen deposition suppressed the total methane sink by 26 Tg during the period 1998–2004, resulting in 6.6 ppb higher atmospheric CH4 mixing ratios compared to without considering nitrogen deposition effects. On average, a cumulative increase of every 1 Tg soil CH4 consumption decreased atmospheric CH4 mixing ratios by 0.26 ppb during the period 1998–2004.

Determination of Methane Hydrate Solubility in the Absence of Vapor Phase by in-situ Raman Spectroscopy

NASA Astrophysics Data System (ADS)

Lu, W.; Chou, I.; Burruss, R.

2006-12-01

Prediction of the occurrence, distribution, and evolution of methane hydrate in porous marine sediments requires information on solubilities of methane hydrate in water. Solubilities of methane hydrate in the presence of a vapor phase are well established, but those in the absence of a vapor phase are not well defined with differences up to 30%. We have measured methane concentrations in pure water in equilibrium with sI methane hydrate, in the absence of vapor phase, by in-situ Raman spectroscopy at temperatures (T) from 2 to 20 (± 0.3) °C and pressures (P) at 10, 20, 30, and 40 (± 0.4%) MPa. Methane hydrate was synthesized in a high-pressure capillary optical cell (Chou et al., 2005; Advances in High-Pressure Technology for Geophysical Applications. Ed. J. Chen et al., Chapter 24, p. 475, Elsevier). A small quantity of methane was first loaded in an evacuated cell and then pressurized by water. Hydrate crystals were formed near the liquid-vapor interface near the enclosed end of the optical tube at room T, and were then placed at the center of a USGS-type heating-cooling stage. By adjusting sample P and T, the crystals went through dissolution-formation cycles three to four times in three days until the vapor phase was completely consumed and several crystals (typically 40 x 40 x 10 μm) were formed. These crystals were located at about 200 μm from the enclosed end and were about 20 to 40 μm from each other. Raman spectra were collected for the liquid phase adjacent to hydrate crystals near the enclosed end of the tube. A volumetric decrease in crystal size was observed away from the sampling spot; however, no such volumetric decrease was observed in or near the sampling spot. Therefore, equilibrium was likely established locally within the sampling area. The results are represented by the following linear isobaric equations: 10 MPa: ln [X(CH4)] = 0.06175 T - 6.79507; r2 = 0.9991 (n = 6) 20 MPa: ln [X(CH4)] = 0.06170 T - 6.82816; r2 = 0.9985 (n = 6) 30 MPa: ln [X(CH4)] = 0.06186 T - 6.87463; r2 = 0.9971 (n = 10) 40 MPa: ln [X(CH4)] = 0.06147 T - 6.95384; r2 = 0.9983 (n = 22), where X(CH4) is the mole fraction of CH4 in solution and n is the number of observations. These results are in good agreement with measurements by Servio and Englezos (2002, J. Chem. Eng. Data., 47, p. 87) and Kim et al. (2003, Ind. Eng. Chem. Res., 42, p. 2409) and predictions by Glew et al. (2003, Can. J. of Chem., 81, p.1443). However, our solubilities are about 10 to 30% higher than those measured by Yang et al. (2001, Fluid Phase Equilibria, 185, p. 53) and those predicted by Davie et al. (2004, Marine Geol., 203, p. 177) and Zhang and Xu (2003, Earth and Planet. Sci. Lett., 213, p. 133). It should be noted that our solubilities are minimum values if an equilibrium state was not reached during our measurements. When compared with previous direct sampling method, the advantages of our method include: (1) the use of in-situ Raman signals for methane concentration measurements eliminates possible uncertainty caused by pressure drops during sampling; (2) simple and efficient; and (3) high-pressure data can be obtained without safety concern.

Soil methane oxidation in both dry and wet temperate eucalypt forests shows a near-identical relationship with soil air-filled porosity

NASA Astrophysics Data System (ADS)

Fest, Benedikt J.; Hinko-Najera, Nina; Wardlaw, Tim; Griffith, David W. T.; Livesley, Stephen J.; Arndt, Stefan K.

2017-01-01

Well-drained, aerated soils are important sinks for atmospheric methane (CH4) via the process of CH4 oxidation by methane-oxidising bacteria (MOB). This terrestrial CH4 sink may contribute towards climate change mitigation, but the impact of changing soil moisture and temperature regimes on CH4 uptake is not well understood in all ecosystems. Soils in temperate forest ecosystems are the greatest terrestrial CH4 sink globally. Under predicted climate change scenarios, temperate eucalypt forests in south-eastern Australia are predicted to experience rapid and extreme changes in rainfall patterns, temperatures and wild fires. To investigate the influence of environmental drivers on seasonal and inter-annual variation of soil-atmosphere CH4 exchange, we measured soil-atmosphere CH4 exchange at high-temporal resolution (< 2 h) in a dry temperate eucalypt forest in Victoria (Wombat State Forest, precipitation 870 mm yr-1) and in a wet temperature eucalypt forest in Tasmania (Warra Long-Term Ecological Research site, 1700 mm yr-1). Both forest soil systems were continuous CH4 sinks of -1.79 kg CH4 ha-1 yr-1 in Victoria and -3.83 kg CH4 ha-1 yr-1 in Tasmania. Soil CH4 uptake showed substantial temporal variation and was strongly controlled by soil moisture at both forest sites. Soil CH4 uptake increased when soil moisture decreased and this relationship explained up to 90 % of the temporal variability. Furthermore, the relationship between soil moisture and soil CH4 flux was near-identical at both forest sites when soil moisture was expressed as soil air-filled porosity (AFP). Soil temperature only had a minor influence on soil CH4 uptake. Soil nitrogen concentrations were generally low and fluctuations in nitrogen availability did not influence soil CH4 uptake at either forest site. Our data suggest that soil MOB activity in the two forests was similar and that differences in soil CH4 exchange between the two forests were related to differences in soil moisture and thereby soil gas diffusivity. The differences between forest sites and the variation in soil CH4 exchange over time could be explained by soil AFP as an indicator of soil moisture status.

Feces composition and manure derived methane yield from dairy cows: Influence of diet with focus on fat supplement and roughage type

NASA Astrophysics Data System (ADS)

Møller, Henrik Bjarne; Moset, Verónica; Brask, Maike; Weisbjerg, Martin Riis; Lund, Peter

2014-09-01

The objective of the present study was to evaluate the effect of dairy cow diets on feces composition and methane (CH4) potential from manure with emphasis on fat level and roughage type and compare these results with the corresponding enteric CH4 emission. In experiment 1 six different diets, divided into two fat levels (low and high) and three different roughage types (early cut grass silage, late cut grass silage and maize silage), were used. The high fat level was achieved by adding crushed rapeseed. In experiment 2, the influence of increasing the fat level by using three different types of rapeseed: rapeseed cake, whole seed and rapeseed oil against a low fat ration with no rapeseed fat supplementation was studied. The diet and fat level had a significant influence on feces composition and CH4 yield. In general, ultimate CH4 yields (B0) were 8-9% higher than the present international default values for diets without extra fat and in feces from diets with extra fat supply the yield was 25-31% higher. It was possible to predict the B0 value from feed and feces characteristics; in fact, the best correlation was obtained by including both feed and feces characteristics. Addition of crude fat to diets to dairy cows reduced enteric CH4 emission but at the same time increased CH4 potential from feces both in terms of organic matter in feces and dry matter intake which might lead to increasing emissions unless proper manure handling such as anaerobic digestion is included. Without subsequent anaerobic digestion to produce energy the positive effect achieved at cow level could be counteracted by increasing manure emissions.

Methane Emissions from the Inland Waters of Alaska

NASA Astrophysics Data System (ADS)

Striegl, R. G.; Butman, D. E.; Stackpoole, S. M.; Dornblaser, M.

2017-12-01

Inland waters at high latitudes generally emit methane (CH4) continuously to the atmosphere during the open water season and build-up CH4 under ice during winter that is released over a short period following ice melt. Landscape position, stream and river size, water source, and turbulence created by water flow largely control CH4 emissions from streams and rivers. Organic carbon sources for CH4 production in lakes vary widely among lakes and landscapes and include hydrologic inputs from terrestrial sources, releases from permafrost thaw (thermokarst), and autochthonous inputs from aquatic macrophytes and algae. Lake emissions are therefore controlled by the balance between within-lake CH4 production and consumption, surface turbulence at the water-air interface, and CH4 ebullition. This creates a complex range of conditions that are difficult to characterize, where dissolved CH4 concentrations may vary by up to 4 orders of magnitude among lakes and/or within a single lake over an annual seasonal cycle. Moreover, large inputs of organic matter from permafrost thaw or other sources commonly result in high rates of bubble production and ebullition from some lakes, while other lakes have negligible ebullition. We quantified water surface areas and estimated CH4 emission rates for lakes, streams and rivers for the six major hydrologic regions of Alaska and determined that they collectively emit about 0.124 Tg C per year as CH4 to the atmosphere. Lake emissions comprise about 75% of the total. When adjusted for total land surface area in Alaska, our lake emission estimate is substantially smaller than previous global estimates for inland waters north of 50 degrees North latitude. We attribute this to incorporation of results that cover a broad range of lake conditions in interior Alaska and to new data from lakes in southwest Alaska that have very low CH4 concentration but very large surface area.

A computational study of CH 4 storage in porous framework materials with metalated linkers: connecting the atomistic character of CH 4 binding sites to usable capacity

DOE PAGES

Tsivion, Ehud; Mason, Jarad A.; Gonzalez, Miguel. I.; ...

2016-03-29

In order to store natural gas (NG) inexpensively at adequate densities for use as a fuel in the transportation sector, new porous materials are being developed. Our work uses computational methods to explore strategies for improving the usable methane storage capacity of adsorbents, including metal-organic frameworks (MOFs), that feature open-metal sites incorporated into their structure by postsynthetic modification. The adsorption of CH 4 on several open-metal sites is studied by calculating geometries and adsorption energies and analyzing the relevant interaction factors. Approximate site-specific adsorption isotherms are obtained, and the open-metal site contribution to the overall CH 4 usable capacity ismore » evaluated. It is found that sufficient ionic character is required, as exemplified by the strong CH 4 affinities of 2,2'-bipyridine-CaCl 2 and Mg, Ca-catecholate. In addition, it is found that the capacity of a single metal site depends not only on its affinity but also on its geometry, where trigonal or "bent" low-coordinate exposed sites can accommodate three or four methane molecules, as exemplified by Ca-decorated nitrilotriacetic acid. The effect of residual solvent molecules at the open-metal site is also explored, with some positive conclusions. Not only can residual solvent stabilize the open-metal site, surprisingly, solvent molecules do not necessarily reduce CH 4 affinity, but can contribute to increased usable capacity by modifying adsorption interactions.« less

On the state of methane and nitrogen ice on Pluto and Triton: Implications of the binary phase diagram

NASA Astrophysics Data System (ADS)

Trafton, Laurence M.

2015-01-01

Compositional analyses of Pluto's surface ice in the literature typically include large areas on the body where CH4 and other volatiles are segregated in the pure form from the solid solution N2:CH4 in which CH4 is diluted. However, the existence of continent-size areas of pure CH4 are in conflict with both of the alternative models that successfully explain the enhancement of CH4 in Pluto's atmosphere, the Detailed Balancing thermal equilibrium model and the Hot Methane Patch model. Pluto's spectrum includes an apparently unshifted CH4 component while Triton's does not, and 93% of the concentration range of the binary phase diagram at 38 K shows that these species exist as a mixture of two saturated solid solution phases. Recognizing this, we propose that both of these saturated phases are present on Pluto and the CH4-rich phase of the mixture, CH4:N2, is the source of the relatively unshifted CH4 spectrum attributed to pure CH4. We also propose that CH4 is less abundant in Triton's ice to the point where either the ice is not saturated or the saturated CH4:N2 phase has not been detected. In this scenario, the partial vapor pressures do not change when the relative proportions of these saturated phases are varied in the mixture. Thus, the partial vapor pressures are independent of N2-CH4 concentrations if both saturated phases are present. Accordingly, the longitudinal and seasonal variations of CH4 and N2 features in Pluto's spectrum would be attributed to spatial variations in the relative proportions of these species. This may occur during volatile transport in the sublimation wind through extensive influences. The lower, unsaturated, values of the mole fraction of CH4 in the ice reported by Owen et al. (Owen et al. [1993]. Science 261, 745-748) and Cruikshank et al. (Cruikshank, D.P., Rush, T.L., Owen, T.C., Quirico, E., de Bergh, C. [1998]. The surface compositions of Triton, Pluto, and Charon. In: Solar System Ices. Astrophysics and Space Science Library Series, vol. 227. Kluwer Academic Publishers, Dordrecht), and by Doute et al. (Doute, S., Schmitt, B., Quirico, E., Owen, T.C., Cruikshank, D.P., de Bergh, C., Geballe, T.R., Roush, T.L. [1999]. Icarus 142, 421-444) based on a compositional analysis of Pluto's surface, were not obtained using optical constants for components consistent with the constraints of the phase diagram.

Stable isotopes as tracers of methane dynamics in Everglades marshes with and without active populations of methane oxidizing bacteria

NASA Technical Reports Server (NTRS)

Happell, James D.; Chanton, Jeffrey P.; Whiting, Gary J.; Showers, William J.

1993-01-01

The stable carbon isotopic composition of CH4 is used to study the processes that affect it during transport through plants from sediment to the atmosphere. The enhancement of CH4 flux from Cladium and Eleocharis over the flux from open water or clipped sites indicated that these plants served as gas conduits between the sediments and the atmosphere. Lowering of the water table below the sediment surface caused an Everglades sawgrass marsh to shift from emission of CH4 to consumption of atmospheric CH4. Cladium transported gases passively mainly via molecular diffusion and/or effusion instead of actively via bulk flow. Stable isotropic data gave no evidence that CH4 oxidation was occurring in the rhizosphere of Cladium. Both CH4 stable carbon isotope and flux data indicated a lack of CH4 oxidation at the sediment-water interface in Everglades marl soils and its presence in peat soils where 40 to 92 percent of the flux across the sediment-water interface was oxidized.

Effect of grazing on methane uptake from Eurasian steppe of China.

PubMed

Tang, Shiming; Zhang, Yujuan; Zhai, Xiajie; Wilkes, Andreas; Wang, Chengjie; Wang, Kun

2018-03-20

The effects of grazing on soil methane (CH 4 ) uptake in steppe ecosystems are important for understanding carbon sequestration and cycling because the role of grassland soil for CH 4 uptake can have major impacts at the global level. Here, a meta-analysis of 27 individual studies was carried out to assess the response patterns of soil CH 4 uptake to grazing in steppe ecosystems of China. The weighted log response ratio was used to assess the effect size. We found that heavy grazing significantly depressed soil CH 4 uptake by 36.47%, but light and moderate grazing had no significant effects in grassland ecosystem. The response of grassland soil CH 4 uptake to grazing also was found to depend upon grazing intensity, grazing duration and climatic types. The increase in soil temperature and reduced aboveground biomass and soil moisture induced by heavy grazing may be the major regulators of the soil CH 4 uptake. These findings imply that grazing effects on soil CH 4 uptake are highly context-specific and that grazing in different grasslands might be managed differently to help mitigate greenhouse gas emissions.

Using stable isotopes of hydrogen to quantify biogenic and thermogenic atmospheric methane sources: A case study from the Colorado Front Range

NASA Astrophysics Data System (ADS)

Townsend-Small, Amy; Botner, E. Claire; Jimenez, Kristine L.; Schroeder, Jason R.; Blake, Nicola J.; Meinardi, Simone; Blake, Donald R.; Sive, Barkley C.; Bon, Daniel; Crawford, James H.; Pfister, Gabriele; Flocke, Frank M.

2016-11-01

Global atmospheric concentrations of methane (CH4), a powerful greenhouse gas, are increasing, but because there are many natural and anthropogenic sources of CH4, it is difficult to assess which sources may be increasing in magnitude. Here we present a data set of δ2H-CH4 measurements of individual sources and air in the Colorado Front Range, USA. We show that δ2H-CH4, but not δ13C, signatures are consistent in air sampled downwind of landfills, cattle feedlots, and oil and gas wells in the region. Applying these source signatures to air in ground and aircraft samples indicates that at least 50% of CH4 emitted in the region is biogenic, perhaps because regulatory restrictions on leaking oil and natural gas wells are helping to reduce this source of CH4. Source apportionment tracers such as δ2H may help close the gap between CH4 observations and inventories, which may underestimate biogenic as well as thermogenic sources.

Atmospheric methane sources - Alaskan tundra bogs, an alpine fen, and a subarctic boreal marsh

NASA Technical Reports Server (NTRS)

Sebacher, D. I.; Harriss, R. C.; Grice, S. S.; Bartlett, K. B.; Sebacher, S. M.

1986-01-01

Methane (CH4) flux measurements from Alaska tundra bogs, an alpine fen, and a subarctic boreal marsh were obtained at field sites ranging from Prudhoe Bay on the coast of the Arctic Ocean to the Alaskan Range south of Fairbanks during August 1984. In the tundra, average CH4 emission rates varied from 4.9 mg CH4 per sq m per day (moist tundra) to 119 mg CH4 per sq m per day (waterlogged tundra). Fluxes averaged 40 mg CH4 per sq m per day from wet tussock meadows in the Brooks Range and 289 mg Ch4 per sq m per day from an alpine fen in the Alaskan Range. The boreal marsh had an average CH4 emission rate of 106 mg CH4 per sq m per day. Significant emissions were detected in tundra areas where peat temperatures were as low as 4 C, and permafrost was only 25 cm below the ground surface. Emission rates from the 17 sites sampled were found to be logarithmically related to water levels at the sites. Extrapolation of the data to an estimate of the total annual CH4 emission from all arctic and boreal wetlands suggests that these ecosystems are a major source of atmospheric CH4 and could account for up to 23 percent of global CH4 emissions from wetlands.

Large-scale controls of methanogenesis inferred from methane and gravity spaceborne data.

PubMed

Bloom, A Anthony; Palmer, Paul I; Fraser, Annemarie; Reay, David S; Frankenberg, Christian

2010-01-15

Wetlands are the largest individual source of methane (CH4), but the magnitude and distribution of this source are poorly understood on continental scales. We isolated the wetland and rice paddy contributions to spaceborne CH4 measurements over 2003-2005 using satellite observations of gravity anomalies, a proxy for water-table depth Gamma, and surface temperature analyses TS. We find that tropical and higher-latitude CH4 variations are largely described by Gamma and TS variations, respectively. Our work suggests that tropical wetlands contribute 52 to 58% of global emissions, with the remainder coming from the extra-tropics, 2% of which is from Arctic latitudes. We estimate a 7% rise in wetland CH4 emissions over 2003-2007, due to warming of mid-latitude and Arctic wetland regions, which we find is consistent with recent changes in atmospheric CH4.

Effects of temperature, ultraviolet radiation and pectin methyl esterase on aerobic methane release from plant material.

PubMed

Bruhn, D; Mikkelsen, T N; Obro, J; Willats, W G T; Ambus, P

2009-11-01

This study examines the effects of different irradiance types on aerobic methane (CH(4)) efflux rates from terrestrial plant material. Furthermore, the role of the enzyme pectin methyl esterase (PME) on CH(4) efflux potential was also examined. Different types of plant tissue and purified pectin were incubated in glass vials with different combinations of irradiation and/or temperature. Purified dry pectin was incubated in solution, and with or without PME. Before and after incubation, the concentration of CH(4) was measured with a gas chromatograph. Rates of CH(4) emission were found to depend exponentially on temperature and linearly on UV-B irradiance. UV-B had a greater stimulating effect than UV-A, while visible light had no effect on emission rates. PME was found to substantially reduce the potential for aerobic CH(4) emissions upon demethylation of pectin.

Growth of copper-benzene-1,3,5-tricarboxylate on boron nitride nanotubes and application of the composite in methane sensing

NASA Astrophysics Data System (ADS)

Xiang, Cuili; Chen, Ting; Zhang, Haitao; Zou, Yongjin; Chu, Hailiang; Zhang, Huanzhi; Xu, Fen; Sun, Lixian; Tang, Chengying

2017-12-01

A new composite material based on copper-benzene-1,3,5-tricarboxylate (Cu-BTC) deposited on boron nitride nanotubes (BNNTs) in a hydrothermal process were investigated for methane (CH4) sensing. The composite was characterized by X-ray diffraction, scanning electron microscopy, and transmission electron microscopy. The Cu-BTC deposited on the BNNTs had an average grain size of 80 nm. The sensing performance of the as-grown product was studied for different concentrations of CH4 (20-200 ppm) at 150 °C. The results revealed that the Cu-BTC/BNNT composite exhibited high sensitivity and selectivity toward CH4. The good sensing performance of the composite was attributed to the high surface area and high affinity of Cu-BTC for CH4, which would allow the composite to act like a preconcentrator for CH4 gas sensing.

Large-Scale Controls of Methanogenesis Inferred from Methane and Gravity Spaceborne Data

NASA Astrophysics Data System (ADS)

Bloom, A. Anthony; Palmer, Paul I.; Fraser, Annemarie; Reay, David S.; Frankenberg, Christian

2010-01-01

Wetlands are the largest individual source of methane (CH4), but the magnitude and distribution of this source are poorly understood on continental scales. We isolated the wetland and rice paddy contributions to spaceborne CH4 measurements over 2003-2005 using satellite observations of gravity anomalies, a proxy for water-table depth Γ, and surface temperature analyses TS. We find that tropical and higher-latitude CH4 variations are largely described by Γ and TS variations, respectively. Our work suggests that tropical wetlands contribute 52 to 58% of global emissions, with the remainder coming from the extra-tropics, 2% of which is from Arctic latitudes. We estimate a 7% rise in wetland CH4 emissions over 2003-2007, due to warming of mid-latitude and Arctic wetland regions, which we find is consistent with recent changes in atmospheric CH4.

Modelling methane emissions from natural wetlands by development and application of the TRIPLEX-GHG model

USGS Publications Warehouse

Zhu, Qing; Liu, Jinxun; Peng, C.; Chen, H.; Fang, X.; Jiang, H.; Yang, G.; Zhu, D.; Wang, W.; Zhou, X.

2014-01-01

A new process-based model TRIPLEX-GHG was developed based on the Integrated Biosphere Simulator (IBIS), coupled with a new methane (CH4) biogeochemistry module (incorporating CH4 production, oxidation, and transportation processes) and a water table module to investigate CH4 emission processes and dynamics that occur in natural wetlands. Sensitivity analysis indicates that the most sensitive parameters to evaluate CH4 emission processes from wetlands are r (defined as the CH4 to CO2 release ratio) and Q10 in the CH4 production process. These two parameters were subsequently calibrated to data obtained from 19 sites collected from approximately 35 studies across different wetlands globally. Being heterogeneously spatially distributed, r ranged from 0.1 to 0.7 with a mean value of 0.23, and the Q10 for CH4 production ranged from 1.6 to 4.5 with a mean value of 2.48. The model performed well when simulating magnitude and capturing temporal patterns in CH4 emissions from natural wetlands. Results suggest that the model is able to be applied to different wetlands under varying conditions and is also applicable for global-scale simulations.

Methane and nitrous oxide analyzer comparison and emissions from dairy freestall barns with manure flushing and scraping

NASA Astrophysics Data System (ADS)

Cortus, Erin L.; Jacobson, Larry D.; Hetchler, Brian P.; Heber, Albert J.; Bogan, Bill W.

2015-01-01

Continuous methane (CH4) and nitrous oxide (N2O) emission measurements were conducted at two crossflow-ventilated dairy freestall barns located in the state of Wisconsin, USA during a 19-month period from 2008 to 2010. The two cross-flow mechanically ventilated buildings (275 and 375 cow capacities) were evaluated in the National Air Emissions Monitoring Study. In September of 2008, the barns' manure collection systems were changed from flushing open gutter using manure basin effluent to a tractor scrape. A photoacoustic multi-gas analyzer (PAMGA) and a direct methane/non-methane hydrocarbon analyzer (GC-FID) provided side-by-side measurements of methane (CH4) for 13 months. The PAMGA also measured nitrous oxide (N2O), and a side-by-side comparison was performed with a gas-filter correlation analyzer (GFC) for six months. Barn ventilation rates were measured by recording run times of the 127-cm diameter exhaust fans. All 125 belt-driven exhaust fans were identical, and in situ airflow measurements using the Fan Assessment Numeration System (FANS) were conducted once at the beginning and twice during the test. Daily CH4 and N2O emission rates were calculated over approximately 19 and 6 month periods respectively, on per barn, head, animal unit, floor area space and barn capacity bases. The differences between the analyzers' concentration measurements were compared in conjunction with water vapor and other gases. The analyzer type had a significant impact on the average CH4 emission rate (p < 0.001) and the average N2O emission rate (p < 0.05). Based on the CH4 measurements with the GC-FID, average daily mean CH4 emissions were approximately 290 g AU-1 d-1 (390 g cow-1 d-1) with very limited seasonal effects. Little variation was observed in CH4 emission rates before and after the change in manure collection method, suggesting that most of the CH4 emissions were enteric losses directly from the cows. The average daily mean N2O emission rates based on the GFC were very low, with an approximate rate of only 690 mg AU-1 d-1 (970 mg cow-1 d-1). The change in manure collection had no apparent effect on N2O emission.

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

PubMed

Choi, Kwang-Soon; Kondaveeti, Sanath; Min, Booki

2017-12-01

Microbial electrolysis cells (MECs) at various cell voltages (0.5, 0.7 1.0 and 1.5V) were operated in anaerobic fermentation. During the start-up period, the cathode potential decreased from -0.63 to -1.01V, and CH 4 generation increased from 168 to 199ml. At an applied voltage of 1.0V, the highest methane yields of 408.3ml CH 4 /g COD glucose was obtained, which was 30.3% higher than in the control tests (313.4ml CH 4 /g COD glucose). The average current of 5.1mA was generated at 1.0V at which the maximum methane yield was obtained. The other average currents were 1.42, 3.02, 0.53mA at 0.5, 0.7, and 1.5V, respectively. Cyclic voltammetry and EIS analysis revealed that enhanced reduction currents were present at all cell voltages with biocatalyzed cathode electrodes (no reduction without biofilm), and the highest value was obtained with 1V external voltage. Copyright © 2017 Elsevier Ltd. All rights reserved.

Structures of microbial communities found in anaerobic batch runs that produce methane from propionic acid--Seeded from full-scale anaerobic digesters above a certain threshold.

PubMed

Kim, Woong; Shin, Seung Gu; Han, Gyuseong; Cho, Kyungjin; Hwang, Seokhwan

2015-11-20

The volatile fatty acid propionate inhibits anaerobic digestion during organic waste treatments. To examine potential microbial interactions that accelerate propionate oxidation, anaerobic digestion systems seeded with various types of anaerobic sludge were analyzed. Seed samples were collected from 10 different full-scale anaerobic reactors in South Korea. Propionate oxidation was estimated as the methane production rate per gram of propionate used per day. Two domestic sewage sludge showed the highest methane production rate values, 109.1 ± 4.2 and 74.5 ± 8.6 mL CH4/(g propionate ∙ d). A food waste recycling wastewater source exhibited the lowest methane production rate, 33.2 ± 2.6 mL CH4/(g propionate ∙ d). To investigate how the microbial community structure affected propionate oxidation, qualitative molecular analyses were carried out using denaturing gradient gel electrophoresis. Methanosaeta concilii, an aceticlastic methanogen, was detected in most batch runs. Smithella propionica, a unique propionate oxidizer and simultaneous producer of acetate, was found in domestic sewage sludge sources showing the highest methane production rate; in contrast, Desulfobulbus rhabdoformis, a sulfate reducer coupled with the consumption of acetate to be used as a precursor of methane, was observed in food waste recycling wastewater sludge source showing the lowest methane production rate. Thus, we propose that S. propionica, a syntrophic acetate producer using propionate, might cooperate with aceticlastic methanogens for high methane production during anaerobic digestion that included propionate. Copyright © 2015 Elsevier B.V. All rights reserved.

Inverse Estimation of California Methane Emissions and Their Uncertainties using FLEXPART-WRF

NASA Astrophysics Data System (ADS)

Cui, Y.; Brioude, J. F.; Angevine, W. M.; McKeen, S. A.; Peischl, J.; Nowak, J. B.; Henze, D. K.; Bousserez, N.; Fischer, M. L.; Jeong, S.; Liu, Z.; Michelsen, H. A.; Santoni, G.; Daube, B. C.; Kort, E. A.; Frost, G. J.; Ryerson, T. B.; Wofsy, S. C.; Trainer, M.

2015-12-01

Methane (CH4) has a large global warming potential and mediates global tropospheric chemistry. In California, CH4 emissions estimates derived from "top-down" methods based on atmospheric observations have been found to be greater than expected from "bottom-up" population-apportioned national and state inventories. Differences between bottom-up and top-down estimates suggest that the understanding of California's CH4 sources is incomplete, leading to uncertainty in the application of regulations to mitigate regional CH4 emissions. In this study, we use airborne measurements from the California research at the Nexus of Air Quality and Climate Change (CalNex) campaign in 2010 to estimate CH4 emissions in the South Coast Air Basin (SoCAB), which includes California's largest metropolitan area (Los Angeles), and in the Central Valley, California's main agricultural and livestock management area. Measurements from 12 daytime flights, prior information from national and regional official inventories (e.g. US EPA's National Emission Inventory, the California Air Resources Board inventories, the Liu et al. Hybrid Inventory, and the California Greenhouse Gas Emissions Measurement dataset), and the FLEXPART-WRF transport model are used in our mesoscale Bayesian inverse system. We compare our optimized posterior CH4 inventory to the prior bottom-up inventories in terms of total emissions (Mg CH4/hr) and the spatial distribution of the emissions (0.1 degree), and quantify uncertainties in our posterior estimates. Our inversions show that the oil and natural gas industry (extraction, processing and distribution) is the main source accounting for the gap between top-down and bottom-up inventories over the SoCAB, while dairy farms are the largest CH4 source in the Central Valley. CH4 emissions of dairy farms in the San Joaquin Valley and variations of CH4 emissions in the rice-growing regions of Sacramento Valley are quantified and discussed. We also estimate CO and NH3 surface fluxes and use their observed correlation with CH4 mixing ratio to further evaluate our CH4 total emission estimates, and understand the spatial distribution of CH4 emissions.

Development of a low-maintenance measurement approach to continuously estimate methane emissions: A case study.

PubMed

Riddick, S N; Hancock, B R; Robinson, A D; Connors, S; Davies, S; Allen, G; Pitt, J; Harris, N R P

2018-03-01

The chemical breakdown of organic matter in landfills represents a significant source of methane gas (CH 4 ). Current estimates suggest that landfills are responsible for between 3% and 19% of global anthropogenic emissions. The net CH 4 emissions resulting from biogeochemical processes and their modulation by microbes in landfills are poorly constrained by imprecise knowledge of environmental constraints. The uncertainty in absolute CH 4 emissions from landfills is therefore considerable. This study investigates a new method to estimate the temporal variability of CH 4 emissions using meteorological and CH 4 concentration measurements downwind of a landfill site in Suffolk, UK from July to September 2014, taking advantage of the statistics that such a measurement approach offers versus shorter-term, but more complex and instantaneously accurate, flux snapshots. Methane emissions were calculated from CH 4 concentrations measured 700m from the perimeter of the landfill with observed concentrations ranging from background to 46.4ppm. Using an atmospheric dispersion model, we estimate a mean emission flux of 709μgm -2 s -1 over this period, with a maximum value of 6.21mgm -2 s -1 , reflecting the wide natural variability in biogeochemical and other environmental controls on net site emission. The emissions calculated suggest that meteorological conditions have an influence on the magnitude of CH 4 emissions. We also investigate the factors responsible for the large variability observed in the estimated CH 4 emissions, and suggest that the largest component arises from uncertainty in the spatial distribution of CH 4 emissions within the landfill area. The results determined using the low-maintenance approach discussed in this paper suggest that a network of cheaper, less precise CH 4 sensors could be used to measure a continuous CH 4 emission time series from a landfill site, something that is not practical using far-field approaches such as tracer release methods. Even though there are limitations to the approach described here, this easy, low-maintenance, low-cost method could be used by landfill operators to estimate time-averaged CH 4 emissions and their impact downwind by simultaneously monitoring plume advection and CH 4 concentrations. Copyright © 2016. Published by Elsevier Ltd.

Natural gas pipeline leaks across Washington, DC.

PubMed

Jackson, Robert B; Down, Adrian; Phillips, Nathan G; Ackley, Robert C; Cook, Charles W; Plata, Desiree L; Zhao, Kaiguang

2014-01-01

Pipeline safety in the United States has increased in recent decades, but incidents involving natural gas pipelines still cause an average of 17 fatalities and $133 M in property damage annually. Natural gas leaks are also the largest anthropogenic source of the greenhouse gas methane (CH4) in the U.S. To reduce pipeline leakage and increase consumer safety, we deployed a Picarro G2301 Cavity Ring-Down Spectrometer in a car, mapping 5893 natural gas leaks (2.5 to 88.6 ppm CH4) across 1500 road miles of Washington, DC. The δ(13)C-isotopic signatures of the methane (-38.2‰ ± 3.9‰ s.d.) and ethane (-36.5 ± 1.1 s.d.) and the CH4:C2H6 ratios (25.5 ± 8.9 s.d.) closely matched the pipeline gas (-39.0‰ and -36.2‰ for methane and ethane; 19.0 for CH4/C2H6). Emissions from four street leaks ranged from 9200 to 38,200 L CH4 day(-1) each, comparable to natural gas used by 1.7 to 7.0 homes, respectively. At 19 tested locations, 12 potentially explosive (Grade 1) methane concentrations of 50,000 to 500,000 ppm were detected in manholes. Financial incentives and targeted programs among companies, public utility commissions, and scientists to reduce leaks and replace old cast-iron pipes will improve consumer safety and air quality, save money, and lower greenhouse gas emissions.

[Mid-infrared distributed-feedback quantum cascade laser-based photoacoustic detection of trace methane gas].

PubMed

Tan, Song; Liu, Wan-feng; Wang, Li-jun; Zhang, Jin-chuan; Li, Lu; Liu, Jun-qi; Liu, Feng-qi; Wang, Zhan-guo

2012-05-01

There have been considerable interests in methane detection based on infrared absorption spectroscopy for industrial and environment monitoring. The authors report on the realization of photoacoustic detection of methane (CH4) using mid-infrared distributed-feedback quantum cascade laser (DFB-QCL). The absorption line at 1316.83 cm(-1) was selected for CH4 detection, which can be reached by the self-manufactured DFB-QCL source operating in pulsed mode near 7.6 microm at room-temperature. The CH4 gas is filled to a Helmholtz resonant photoacoustic cell, which was equipped with a commercial electret microphone. The DFB-QCL was operated at 234 Hz with an 80 mW optical peak power. A detection limit of 189 parts per billion in volume was derived when the signal-to-noise ratio equaled 1.

Continuous, Pulsed Export of Methane-Supersaturated Meltwaters from the Bed of the Greenland Ice Sheet

NASA Astrophysics Data System (ADS)

Lamarche-Gagnon, G.; Wadham, J.; Beaton, A.; Fietzek, P.; Stanley, K. M.; Tedstone, A.; Sherwood Lollar, B.; Lacrampe Couloume, G.; Telling, J.; Liz, B.; Hawkings, J.; Kohler, T. J.; Zarsky, J. D.; Stibal, M.; Mowlem, M. C.

2016-12-01

Both past and present ice sheets have been proposed to cap large quantities of methane (CH4), on orders of magnitude significant enough to impact global greenhouse gas concentrations during periods of rapid ice retreat. However, to date most evidence for sub-ice sheet methane has been indirect, derived from calculations of the methanogenic potential of basal-ice microbial communities and biogeochemical models; field-based empirical measurements are lacking from large ice sheet catchments. Here, we present the first continuous, in situ record of dissolved methane export from a large catchment of the Greenland Ice Sheet (GrIS) in South West Greenland from May-July 2015. Our results indicate that glacial runoff was continuously supersaturated with methane over the observation period (dissolved CH4 concentrations of 30-700 nM), with total methane flux rising as subglacial discharge increased. Periodic subglacial drainage events, characterised by rapid changes (i.e. pulses) in meltwater hydrochemistry, also coincided with a rise in methane concentrations. We argue that these are likely indicative of the flushing of subglacial reservoirs of CH4 beneath the ice sheet. Total methane export was relatively modest when compared to global methane budgets, but too high to be explained by previously determined methanogenic rates from Greenland basal ice. Discrepancies between estimated Greenland methane reserves and observed fluxes stress the need to further investigate GrIS methane fluxes and sources, and suggest a more biogeochemically active subglacial environment than previously considered. Results indicate that future warming, and a coincident increase in ice melt rates, would likely make the GrIS, and by extension the Antarctic Ice Sheet, more significant sources of atmospheric methane, consequently acting as a positive feedback to a warming climate.

Relative linkages of peatland methane and carbon dioxide fluxes with climatic, environmental and ecological parameters and their inter-comparison

NASA Astrophysics Data System (ADS)

Banerjee, Tirtha; Hommeltenberg, Janina; Roy, Avipsa; De Roo, Frederik; Mauder, Matthias

2016-04-01

Although methane (CH4) is the second most important greenhouse gas (GHG) after CO2, about 80% of its global production is biogenic (wetlands, enteric fermentation and water disposal from animals) contrary to major anthropogenic sources of most other GHGs. Although on a shorter time scale, global emissions of methane are greater (10 year time frame) or about 80% (20 year time frame) of those of carbon dioxide in terms of their influence on global warming, methane emissions have been studied much less than CO2 emissions. Lakes, reservoirs and wetlands are estimated to contribute about 15-40% to the global methane source budget, which is higher than total oceanic CH4 emission. Half of the world's wetlands are represented by peatlands which cover 3% of the global total land area. Peatlands have a thick water-logged organic soil layer (peat) made up of dead and decaying plant material. Moreover, they are carbon rich, containing twice as much stock as the entire forest biomass of the world (550 Gt carbon). When disturbed, they can become significant sources of greenhouse gas emissions. The organic carbon exposed to air due to various mechanisms can release CH4 or CO2 in the atmosphere. Thus the nature of vegetation cover, radiation environment, wind turbulence, soil characteristics, water table depth etc. are expected to be important forcings that influence the emission of CH4 or CO2 in the shorter time scale. However, long term climate change can also influence these governing factors themselves over a larger time scale, which in turn can influence the wetland GHG emissions. Thus developing a predictive framework and long term source appropriation for wetland CH4 or CO2 warrants an identification of the major environmental forcings on the CH4 or CO2 flux. In the present work, we use a simple and systematic data-analytics approach to determine the relative linkages of different climate and environmental variables with the canopy level half-hourly CH4 or CO2 fluxes over a peatland in Germany. We utilize multivariate pattern recognition techniques of principle component and factor analysis to group and classify climatic, environmental and ecological variables based on their similarity as drivers. Three biophysical process components emerge from the clustering analysis which describe the system-data variances. We find that soil conditions (soil temperature and soil heat flux) are most important in explaining the CH4 flux. The radiation and energy components (sensible heat flux, photosynthetically active radiation (PAR), latent heat flux, net radiation) and turbulence components (wind speed, friction velocity) are moderately linked with the CH4 flux. On the other hand, the CO2 flux has poor linkage with the soil environment variables, while it is strongly linked with the radiation environment components and the turbulence parameters. Quantifying these linkages using factor analysis can be up-scaled to include decadal scale variability to study the effect of climate change on wetland GHG emissions as well.

Assessing methane oxidation under landfill covers and its contribution to the above atmospheric CO{sub 2} levels: The added value of the isotope ({delta}{sup 13}C and {delta}{sup 18}O CO{sub 2}; {delta}{sup 13}C and {delta}D CH{sub 4}) approach

DOE Office of Scientific and Technical Information (OSTI.GOV)

Widory, D., E-mail: d.widory@brgm.fr; Proust, E.; Bellenfant, G.

2012-09-15

Highlights: Black-Right-Pointing-Pointer Comparison of the isotope and mass balance approaches to evaluate the level of methane oxidation within a landfill. Black-Right-Pointing-Pointer The level of methane oxidation is not homogenous under the landfill cover and is strongly correlated to the methane flux. Black-Right-Pointing-Pointer Isotope tracking of the contribution of the methane oxidation to the CO{sub 2} concentrations in the ambient air. - Abstract: We are presenting here a multi-isotope approach ({delta}{sup 13}C and {delta}{sup 18}O of CO{sub 2}; {delta}{sup 13}C and {delta}D of CH{sub 4}) to assess (i) the level(s) of methane oxidation during waste biodegradation and its migration through amore » landfill cover in Sonzay (France), and (ii) its contribution to the atmospheric CO{sub 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{sub 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{sub 4} is rapidly transported. At shallow depth, more immobile biogas pockets show a higher level of CH{sub 4} oxidation by the methanotrophic bacteria. {delta}{sup 13}C of CO{sub 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.« less

Effect of water on methane adsorption on the kaolinite (0 0 1) surface based on molecular simulations

NASA Astrophysics Data System (ADS)

Zhang, Bin; Kang, Jianting; Kang, Tianhe

2018-05-01

CH4 adsorption isotherms of kaolinite with moisture contents ranging from 0 to 5 wt% water, the effects of water on maximum adsorption capacity, kaolinite swelling, and radial distribution function were modelled by the implementing combined Monte Carlo (MC) and molecular dynamics (MD) simulations at 293.15 K (20 °C) and a pressure range of 1-20 MPa. The simulation results showed that the absolute adsorption of CH4 on both dry and moist kaolinite followed a Langmuir isotherm within the simulated pressure range, and both the adsorption capacity and the rate of CH4 adsorption decreased with the water content increases. The adsorption isosteric heats of CH4 on kaolinite decreased linearly with increasing water content, indicating that at higher water contents, the interaction energy between the CH4 and kaolinite was weaker. The interaction between kaolinite and water dominates and was the main contributing factor to kaolinite clay swelling. Water molecules were preferentially adsorbed onto oxygen and hydrogen atoms in kaolinite, while methane showed a tendency to be adsorbed only onto oxygen. The simulation results of our study provide the quantitative analysis of effect of water on CH4 adsorption capacity, adsorption rate, and interaction energy from a microscopic perspective. We hope that our study will contribute to the development of strategies for the further exploration of coal bed methane and shale gas.

Characterizing Methane Emissions at Local Scales with a 20 Year Total Hydrocarbon Time Series, Imaging Spectrometry, and Web Facilitated Analysis

NASA Astrophysics Data System (ADS)

Bradley, Eliza Swan

Methane is an important greenhouse gas for which uncertainty in local emission strengths necessitates improved source characterizations. Although CH4 plume mapping did not motivate the NASA Airborne Visible InfraRed Imaging Spectrometer (AVIRIS) design and municipal air quality monitoring stations were not intended for studying marine geological seepage, these assets have capabilities that can make them viable for studying concentrated (high flux, highly heterogeneous) CH4 sources, such as the Coal Oil Point (COP) seep field (˜0.015 Tg CH4 yr-1) offshore Santa Barbara, California. Hourly total hydrocarbon (THC) data, spanning 1990 to 2008 from an air pollution station located near COP, were analyzed and showed geologic CH4 emissions as the dominant local source. A band ratio approach was developed and applied to high glint AVIRIS data over COP, resulting in local-scale mapping of natural atmospheric CH4 plumes. A Cluster-Tuned Matched Filter (CTMF) technique was applied to Gulf of Mexico AVIRIS data to detect CH4 venting from offshore platforms. Review of 744 platform-centered CTMF subsets was facilitated through a flexible PHP-based web portal. This dissertation demonstrates the value of investigating municipal air quality data and imaging spectrometry for gathering insight into concentrated methane source emissions and highlights how flexible web-based solutions can help facilitate remote sensing research.