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Sample records for methane oxidation final

  1. Stimulation of methane oxidation potential and effects on vegetation growth by bottom ash addition in a landfill final evapotranspiration cover

    NARCIS (Netherlands)

    Kim, G.W.; Ho, A.; Kim, P.J.; Kim, Sang Yun

    2016-01-01

    The landfilling of municipal solid waste is a significant source of atmospheric methane (CH4), contributing up to 20% of total anthropogenic CH4 emissions. The evapotranspiration (ET) cover system, an alternative final cover system in waste landfills, has been considered to be a promising way to

  2. Limits and dynamics of methane oxidation in landfill cover soils

    Science.gov (United States)

    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...

  3. SUPPLEMENTARY INFORMATION Non-oxidative methane ...

    Indian Academy of Sciences (India)

    dell

    SUPPLEMENTARY INFORMATION. Non-oxidative methane dehydroaromatization reaction over highly active α-MoC1-x ZSM-5 derived from pretreatment. BUDDE PRADEEP KUMAR, ARVIND KUMAR SINGH and SREEDEVI UPADHYAYULA*. Heterogeneous Catalysis & Reaction Engineering Laboratory, Department of ...

  4. Methane oxidation and methane fluxes in the ocean surface layer and deep anoxic waters

    Science.gov (United States)

    Ward, B. B.; Kilpatrick, K. A.; Novelli, P. C.; Scranton, M. I.

    1987-01-01

    Measured biological oxidation rates of methane in near-surface waters of the Cariaco Basin are compared with the diffusional fluxes computed from concentration gradients of methane in the surface layer. Methane fluxes and oxidation rates were investigated in surface waters, at the oxic/anoxic interface, and in deep anoxic waters. It is shown that the surface-waters oxidation of methane is a mechanism which modulates the flux of methane from marine waters to the atmosphere.

  5. High-pressure oxidation of methane

    DEFF Research Database (Denmark)

    Hashemi, Hamid; Christensen, Jakob Munkholt; Gersen, Sander

    2016-01-01

    Methane oxidation at high pressures and intermediate temperatures was investigated in a laminar flow reactor and in a rapid compression machine (RCM). The flow-reactor experiments were conducted at 700–900 K and 100 bar for fuel-air equivalence ratios (Φ) ranging from 0.06 to 19.7, all highly...... diluted in nitrogen. It was found that under the investigated conditions, the onset temperature for methane oxidation ranged from 723 K under reducing conditions to 750 K under stoichiometric and oxidizing conditions. The RCM experiments were carried out at pressures of 15–80 bar and temperatures of 800......–1250 K under stoichiometric and fuel-lean (Φ=0.5) conditions. Ignition delays, in the range of 1–100 ms, decreased monotonically with increasing pressure and temperature. A chemical kinetic model for high-pressure methane oxidation was established, with particular emphasis on the peroxide chemistry...

  6. Methane oxidation in anoxic lake waters

    Science.gov (United States)

    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

  7. Elimination of methane in exhaust gas from biogas upgrading process by immobilized methane-oxidizing bacteria.

    Science.gov (United States)

    Wu, Ya-Min; Yang, Jing; Fan, Xiao-Lei; Fu, Shan-Fei; Sun, Meng-Ting; Guo, Rong-Bo

    2017-05-01

    Biogas upgrading is essential for the comprehensive utilization of biogas as substitute of natural gas. However, the methane in the biogas can be fully recovered during the upgrading process of biogas, and the exhaust gas produced during biogas upgrading may contain a very low concentration of methane. If the exhaust gas with low concentration methane releases to atmosphere, it will be harmful to environment. In addition, the utilization of large amounts of digestate produced from biogas plant is another important issue for the development of biogas industry. In this study, solid digestate was used to produce active carbon, which was subsequently used as immobilized material for methane-oxidizing bacteria (MOB) in biofilter. Biofilter with MOB immobilized on active carbon was used to eliminate the methane in exhaust gas from biogas upgrading process. Results showed porous active carbon was successfully made from solid digestate. The final methane elimination capacity of immobilized MOB reached about 13molh -1 m -3 , which was more 4 times higher than that of MOB without immobilization. Copyright © 2017 Elsevier Ltd. All rights reserved.

  8. High-pressure oxidation of methane

    NARCIS (Netherlands)

    Hashemi, Hamid; Christensen, Jakob M.; Gersen, Sander; Levinsky, Howard; Klippenstein, Stephen J.; Glarborg, Peter

    2016-01-01

    Methane oxidation at high pressures and intermediate temperatures was investigated in a laminar flow reactor and in a rapid compression machine (RCM). The flow-reactor experiments were conducted at 700–900 K and 100 bar for fuel-air equivalence ratios (Φ) ranging from 0.06 to 19.7, all highly

  9. Anaerobic oxidation of methane and ammonium.

    NARCIS (Netherlands)

    Strous, M.; Jetten, M.S.M.

    2004-01-01

    Anaerobic oxidation of methane and ammonium are two different processes catalyzed by completely unrelated microorganisms. Still, the two processes do have many interesting aspects in common. First, both of them were once deemed biochemically impossible and nonexistent in nature, but have now been

  10. Termites facilitate methane oxidation and shape the methanotrophic community

    NARCIS (Netherlands)

    Ho, A.; Erens, H.; Mujinya, B.B.; Boeckx, P.; Baert, G.; Schneider, B.; Frenzel, P.; Boon, N.; Van Ranst, E.

    2013-01-01

    Termite-derived methane contributes 3-4% to the total methane budget globally. Termites are not known to harbor methane-oxidizing microorganisms (methanotrophs). However, a considerable fraction of methane produced can be consumed by methanotrophs that inhabit the mound material. Yet, methanotroph

  11. Trends for Methane Oxidation at Solid Oxide Fuel Cell Conditions

    DEFF Research Database (Denmark)

    Kleis, Jesper; Jones, Glenn; Abild-Pedersen, Frank

    2009-01-01

    First-principles calculations are used to predict a plausible reaction pathway for the methane oxidation reaction. In turn, this pathway is used to obtain trends in methane oxidation activity at solid oxide fuel cell (SOFC) anode materials. Reaction energetics and barriers for the elementary...... the Ni surfaces to other metals of interest. This allows the reactivity over the different metals to be understood in terms of two reactivity descriptors, namely, the carbon and oxygen adsorption energies. By combining a simple free-energy analysis with microkinetic modeling, activity landscapes of anode...

  12. Light-Dependent Aerobic Methane Oxidation Reduces Methane Emissions from Seasonally Stratified Lakes

    Science.gov (United States)

    Oswald, Kirsten; Milucka, Jana; Brand, Andreas; Littmann, Sten; Wehrli, Bernhard; Kuypers, Marcel M. M.; Schubert, Carsten J.

    2015-01-01

    Lakes are a natural source of methane to the atmosphere and contribute significantly to total emissions compared to the oceans. Controls on methane emissions from lake surfaces, particularly biotic processes within anoxic hypolimnia, are only partially understood. Here we investigated biological methane oxidation in the water column of the seasonally stratified Lake Rotsee. A zone of methane oxidation extending from the oxic/anoxic interface into anoxic waters was identified by chemical profiling of oxygen, methane and δ13C of methane. Incubation experiments with 13C-methane yielded highest oxidation rates within the oxycline, and comparable rates were measured in anoxic waters. Despite predominantly anoxic conditions within the zone of methane oxidation, known groups of anaerobic methanotrophic archaea were conspicuously absent. Instead, aerobic gammaproteobacterial methanotrophs were identified as the active methane oxidizers. In addition, continuous oxidation and maximum rates always occurred under light conditions. These findings, along with the detection of chlorophyll a, suggest that aerobic methane oxidation is tightly coupled to light-dependent photosynthetic oxygen production both at the oxycline and in the anoxic bottom layer. It is likely that this interaction between oxygenic phototrophs and aerobic methanotrophs represents a widespread mechanism by which methane is oxidized in lake water, thus diminishing its release into the atmosphere. PMID:26193458

  13. Atmospheric methane removal by methane-oxidizing bacteria immobilized on porous building materials

    NARCIS (Netherlands)

    Ganendra, G; De Muynck, W; Ho, A.; Hoefman, S.; De Vos, P.; Boeckx, P.; Boon, N.

    2014-01-01

    Biological treatment using methane-oxidizing bacteria (MOB) immobilized on six porous carrier materials have been used to mitigate methane emission. Experiments were performed with different MOB inoculated in building materials at high (similar to 20 % (v/v)) and low (similar to 100 ppmv) methane

  14. Improved methane removal in exhaust gas from biogas upgrading process using immobilized methane-oxidizing bacteria.

    Science.gov (United States)

    Sun, Meng-Ting; Yang, Zhi-Man; Fu, Shan-Fei; Fan, Xiao-Lei; Guo, Rong-Bo

    2018-05-01

    Methane in exhaust gas from biogas upgrading process, which is a greenhouse gas, could cause global warming. The biofilter with immobilized methane-oxidizing bacteria (MOB) is a promising approach for methane removal, and the selections of inoculated MOB culture and support material are vital for the biofilter. In this work, five MOB consortia were enriched at different methane concentrations. The MOB-20 consortium enriched at the methane concentration of 20.0% (v/v) was then immobilized on sponge and two particle sizes of volcanic rock in biofilters to remove methane in exhaust gas from biogas upgrading process. Results showed that the immobilized MOB performed more admirable methane removal capacity than suspended cells. The immobilized MOB on sponge reached the highest methane removal efficiency (RE) of 35%. The rough surface, preferable hydroscopicity, appropriate pore size and particle size of support material might favor the MOB immobilization and accordingly methane removal. Copyright © 2018 Elsevier Ltd. All rights reserved.

  15. Methane oxidation coupled to oxygenic photosynthesis in anoxic waters

    Science.gov (United States)

    Milucka, Jana; Kirf, Mathias; Lu, Lu; Krupke, Andreas; Lam, Phyllis; Littmann, Sten; Kuypers, Marcel MM; Schubert, Carsten J

    2015-01-01

    Freshwater lakes represent large methane sources that, in contrast to the Ocean, significantly contribute to non-anthropogenic methane emissions to the atmosphere. Particularly mixed lakes are major methane emitters, while permanently and seasonally stratified lakes with anoxic bottom waters are often characterized by strongly reduced methane emissions. The causes for this reduced methane flux from anoxic lake waters are not fully understood. Here we identified the microorganisms and processes responsible for the near complete consumption of methane in the anoxic waters of a permanently stratified lake, Lago di Cadagno. Interestingly, known anaerobic methanotrophs could not be detected in these waters. Instead, we found abundant gamma-proteobacterial aerobic methane-oxidizing bacteria active in the anoxic waters. In vitro incubations revealed that, among all the tested potential electron acceptors, only the addition of oxygen enhanced the rates of methane oxidation. An equally pronounced stimulation was also observed when the anoxic water samples were incubated in the light. Our combined results from molecular, biogeochemical and single-cell analyses indicate that methane removal at the anoxic chemocline of Lago di Cadagno is due to true aerobic oxidation of methane fuelled by in situ oxygen production by photosynthetic algae. A similar mechanism could be active in seasonally stratified lakes and marine basins such as the Black Sea, where light penetrates to the anoxic chemocline. Given the widespread occurrence of seasonally stratified anoxic lakes, aerobic methane oxidation coupled to oxygenic photosynthesis might have an important but so far neglected role in methane emissions from lakes. PMID:25679533

  16. Could Methane Oxidation in Lakes Be Enhanced by Eutrophication?

    Science.gov (United States)

    Van Grinsven, S.; Villanueva, L.; Harrison, J.; S Sinninghe Damsté, J.

    2017-12-01

    Climate change and eutrophication both affect aquatic ecosystems. Eutrophication is caused by high nutrient inputs, leading to algal blooms, oxygen depletion and disturbances of the natural balances in aquatic systems. Methane, a potent greenhouse gas produced biologically by anaerobic degradation of organic matter, is often released from the sediments of lakes and marine systems to overlying water and the atmosphere. Methane oxidation, a microbial methane consumption process, can limit methane emission from lakes and reservoirs by 50-80%. Here, we studied methane oxidation in a seasonally stratified reservoir: Lacamas Lake in Washington, USA. We found this lake has a large summer storage capacity of methane in its deep water layer, with a very active microbial community capable of oxidizing exceptionally high amounts of methane. The natural presence of terminal electron acceptors is, however, too low to support these high potential rates. Addition of eutrophication-related nutrients such as nitrate and sulfate increased the methane removal rates by 4 to 7-fold. The microbial community was studied using 16S rRNA gene amplicon sequencing and preliminary results indicate the presence of a relatively unknown facultative anaerobic methane oxidizer of the genus Methylomonas, capable of using nitrate as an electron donor. Experiments in which anoxic and oxic conditions were rapidly interchanged showed this facultative anaerobic methane oxidizer has an impressive flexibility towards large, rapid changes in environmental conditions and this feature might be key to the unexpectedly high methane removal rates in eutrophied and anoxic watersheds.

  17. Isotopic studies on oxidative methane coupling over samarium oxide

    International Nuclear Information System (INIS)

    Otsuka, Kiyoshi; Inaida, Masakatsu; Wada, Yuji; Komatsu, Takayuki; Morikawa, Akira

    1989-01-01

    The evident kinetic isotope effect was observed for the formations of ethylene and ethane through the oxidative coupling of methane on Sm 2 O 3 , when CH 4 and CD 4 were used as the reactants. Ethanes formed in the reaction of a mixture of CH 4 , CD 4 , and O 2 were C 2 H 6 , C 2 H 3 D 3 , and C 2 D 6 as major products. These results indicate that the rate-determining step of the reaction is abstraction of hydrogen from methane and that ethane is formed through the coupling of methyl intermediate. (author)

  18. Trace methane oxidation studied in several Euryarchaeota under diverse conditions

    Directory of Open Access Journals (Sweden)

    James J. Moran

    2005-01-01

    Full Text Available We used 13C-labeled methane to document the extent of trace methane oxidation by Archaeoglobus fulgidus, Archaeoglobus lithotrophicus, Archaeoglobus profundus, Methanobacterium thermoautotrophicum, Methanosarcina barkeri and Methanosarcina acetivorans. The results indicate trace methane oxidation during growth varied among different species and among methanogen cultures grown on different substrates. The extent of trace methane oxidation by Mb. thermoautotrophicum (0.05 ± 0.04%, ± 2 standard deviations of the methane produced during growth was less than that by M. barkeri (0.15 ± 0.04%, grown under similar conditions with H2 and CO2. Methanosarcina acetivorans oxidized more methane during growth on trimethylamine (0.36 ± 0.05% than during growth on methanol (0.07 ± 0.03%. This may indicate that, in M. acetivorans, either a methyltransferase related to growth on trimethylamine plays a role in methane oxidation, or that methanol is an intermediate of methane oxidation. Addition of possible electron acceptors (O2, NO3–, SO22–, SO32– or H2 to the headspace did not substantially enhance or diminish methane oxidation in M. acetivorans cultures. Separate growth experiments with FAD and NAD+ showed that inclusion of these electron carriers also did not enhance methane oxidation. Our results suggest trace methane oxidized during methanogenesis cannot be coupled to the reduction of these electron acceptors in pure cultures, and that the mechanism by which methane is oxidized in methanogens is independent of H2 concentration. In contrast to the methanogens, species of the sulfate-reducing genus Archaeoglobus did not significantly oxidize methane during growth (oxidizing 0.003 ± 0.01% of the methane provided to A. fulgidus, 0.002 ± 0.009% to A. lithotrophicus and 0.003 ± 0.02% to A. profundus. Lack of observable methane oxidation in the three Archaeoglobus species examined may indicate that methyl-coenzyme M reductase, which is not present in

  19. Methane and compost from straw. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Rijkens, B A

    1982-01-01

    A concept is developed in which the farmer collects the straw and ferments it anaerobically to compost and methane at the farm. The methane can be used for heating and for production of mechanical energy, while the compost can be returned to the land at any suitable moment. This way of processing conserves part of the energy, present in the straw, that would otherwise be lost by the field-burning or the ploughing-in. In the meantime it solves the field-burning and environmental problems and it provides the possibility to recycle the organic matter in the humus, as well as all the fertilizing compounds K, P, Mg and nitrogen. There are indications that the arable land will need a restocking with humus that has been lost during many years of (modern) farming, leading to loss in structure and production capacity. This study collects the global technical and economical data, enabling us to indicate under which circumstances and local conditions the methane and compost concept would be feasible and would be an alternative to field-burning, ploughing-in or to the purely energetic use of the straw.

  20. Clumped isotope effects during OH and Cl oxidation of methane

    DEFF Research Database (Denmark)

    Whitehill, Andrew R.; Joelsson, Lars Magnus T.; Schmidt, Johan Albrecht

    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 produ......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...... 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...... 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...

  1. Biochemistry of methyl-coenzyme M reductase: the nickel metalloenzyme that catalyzes the final step in synthesis and the first step in anaerobic oxidation of the greenhouse gas methane.

    Science.gov (United States)

    Ragsdale, Stephen W

    2014-01-01

    Methane, the major component of natural gas, has been in use in human civilization since ancient times as a source of fuel and light. Methanogens are responsible for synthesis of most of the methane found on Earth. The enzyme responsible for catalyzing the chemical step of methanogenesis is methyl-coenzyme M reductase (MCR), a nickel enzyme that contains a tetrapyrrole cofactor called coenzyme F430, which can traverse the Ni(I), (II), and (III) oxidation states. MCR and methanogens are also involved in anaerobic methane oxidation. This review describes structural, kinetic, and computational studies aimed at elucidating the mechanism of MCR. Such studies are expected to impact the many ramifications of methane in our society and environment, including energy production and greenhouse gas warming.

  2. Methane oxidation in presence of sulfur dioxide

    International Nuclear Information System (INIS)

    Mantashyan, A.A.; Avetisyan, A.M.; Makaryan, E.M.; Wang, H.

    2006-01-01

    The emission of sulfurous gases including SO 2 from stationary power generation remains to be a serious environmental and ecological problem. Sulfurous gases are almost entirely produced from the combustion of sulfur-containing fuels. While fuel desulfurization and flue gas scrubbing is a viable solution, in the developing countries it remains to be an economical challenge to implement these SO x reduction technologies. The oxidation of methane in presence of sulfurous gas (SO 2 ) addition was studied experimentally. Te experiments were conducted in a static reactor at temperature of 728-786 K, and for mixture of C 4 /O 2 ≡ 1/2 at a pressure of 117 Torr with varying amount of SO 2 addition. It was observed that SO 2 addition accelerated the oxidation process, reduced the induction period and increased the extent of methane consumption. At the relatively short resident time (less than 50 sec) SO 3 was detected, but at longer residence time SO 3 was reduced spontaneously to SO 2

  3. Observations on the methane oxidation capacity of landfill soils

    Science.gov (United States)

    Field data and two independent models indicate that landfill cover methane (CH4) oxidation should not be considered as a constant 10% or any other single value. Percent oxidation is a decreasing exponential function of the total methane flux rate into the cover and is also dependent on climate and c...

  4. Effects of trace volatile organic compounds on methane oxidation

    Directory of Open Access Journals (Sweden)

    Chiemchaisri Wilai

    2001-01-01

    Full Text Available The effects of volatile organic compounds (VOCs on methane oxidation in landfill cover soils were examined. The batch experiments were conducted using single and mixed VOCs, such as, dichloromethane (DCM, trichloroethylene (TCE, tetrachloroethylene (PCE, and benzene. The results from all combinations showed a decrease in methane oxidation rate with increase in VOC concentrations. Moreover, inhibition effects of TCE and DCM were found higher than benzene and PCE. The reduction of methane oxidation by benzene and PCE could be attributed to the toxicity effect, whereas TCE and DCM were found to exhibit the competitive-inhibition effect. When the soil was mixed with DCM, no methane oxidation was found. Damage to the cell's internal membrane was found in a methanotrophic culture exposed to VOC gases which is the attachment site of a key enzyme needed for methane oxidation

  5. A marine microbial consortium apparently mediating anaerobic oxidation of methane

    DEFF Research Database (Denmark)

    Boetius, A.; Ravenschlag, K.; Schubert, CJ

    2000-01-01

    microorganisms mediating this reaction have not yet been isolated, and the pathway of anaerobic oxidation of methane is insufficiently understood. Recent data suggest that certain archaea reverse the process of methanogenesis by interaction with sulphate-reducing bacteria(5-7). Here we provide microscopic...... cells and are surrounded by sulphate-reducing bacteria. These aggregates were abundant in gas-hydrate-rich sediments with extremely high rates of methane-based sulphate reduction, and apparently mediate anaerobic oxidation of methane.......A large fraction of globally produced methane is converted to CO2 by anaerobic oxidation in marine sediments(1). Strong geochemical evidence for net methane consumption in anoxic sediments is based on methane profiles(2), radiotracer experiments(3) and stable carbon isotope data(4). But the elusive...

  6. 'Methane oxidation on supported gold catalysts'

    DEFF Research Database (Denmark)

    Walther, Guido

    2008-01-01

    steady-state activity measurements were performed to obtain the reaction rates for CO and H2 oxidation. These reactions were studied on three different gold particle sizes using either O2 or N2O as oxidation agents. Using particle size distributions obtained from TEM analysis, it was found that the CO......Methane (CH4), a major compound of natural gas, has been suggested as a future energy carrier. However, it is also known to be a strong greenhouse gas. The use of CH4 obtained from crude oil as an associated gas is often uneconomical, and it is thus burned off. Avoiding flaring and making...... the energy stored in the molecule available, is a major research challenge. In this PhD thesis, CH4 oxidation on nanoparticular gold is studied both experimentally and theoretically. In the course of this PhD project, CH4 oxidation was experimentally found more likely to form CO2 and H2O than other low index...

  7. Dissolved methane oxidation and competition for oxygen in down-flow hanging sponge reactor for post-treatment of anaerobic wastewater treatment.

    Science.gov (United States)

    Hatamoto, Masashi; Miyauchi, Tomo; Kindaichi, Tomonori; Ozaki, Noriatsu; Ohashi, Akiyoshi

    2011-11-01

    Post-treatment of anaerobic wastewater was undertaken to biologically oxidize dissolved methane, with the aim of preventing methane emission. The performance of dissolved methane oxidation and competition for oxygen among methane, ammonium, organic matter, and sulfide oxidizing bacteria were investigated using a lab-scale closed-type down-flow hanging sponge (DHS) reactor. Under the oxygen abundant condition of a hydraulic retention time of 2h and volumetric air supply rate of 12.95m(3)-airm(-3)day(-1), greater than 90% oxidation of dissolved methane, ammonium, sulfide, and organic matter was achieved. With reduction in the air supply rate, ammonium oxidation first ceased, after which methane oxidation deteriorated. Sulfide oxidation was disrupted in the final step, indicating that COD and sulfide oxidation occurred prior to methane oxidation. A microbial community analysis revealed that peculiar methanotrophic communities dominating the Methylocaldum species were formed in the DHS reactor operation. Copyright © 2011 Elsevier Ltd. All rights reserved.

  8. Electrocatalytic oxidation of methane: investigations of new catalysts to be used in a solid polymer electrolyte methane fuel-cell; Oxydation electrocatalytique du methane: recherche de catalyseurs en vue d'une application a une pile au methane a electrolyte polymere solide

    Energy Technology Data Exchange (ETDEWEB)

    Berthelot, S

    1998-07-01

    This thesis evaluated the performances of many catalysts facing the methane oxidation which is a critical step in methane fuel cells development. In a first part the study of the methane electro-oxidation has been realized by classical electrochemical technics on many electrodes to determine the most active ones. In a second part the in situ reflection infra-red spectroscopy allowed to identify, during the methane oxidation, the adsorbed species on the electrode and the reaction products. These results also help the understanding of the part of the concerned materials mechanisms in the methane oxidation and then to optimize them for a whole oxidation of the methane in carbon dioxide. The final objective is the use of the methane in a PEMFC fuel cell type. A comparison with the methanol and C2 hydrocarbons behaviour, such as the ethane the ethylene and the acetylene, has been done to evaluate the performances. (A.L.B.)

  9. Advances in the Partial Oxidation of Methane to Synthesis Gas

    Institute of Scientific and Technical Information of China (English)

    Quanli Zhu; Xutao Zhao; Youquan Deng

    2004-01-01

    The conversion and utilization of natural gas is of significant meaning to the national economy,even to the everyday life of people. However, it has not become a popular industrial process as expected due to the technical obstacles. In the past decades, much investigation into the conversion of methane,predominant component of natural gas, has been carried out. Among the possible routes of methane conversion, the partial oxidation of methane to synthesis gas is considered as an effective and economically feasible one. In this article, a brief review of recent studies on the mechanism of the partial oxidation of methane to synthesis gas together with catalyst development is wherein presented.

  10. Methane-oxidizing seawater microbial communities from an Arctic shelf

    Science.gov (United States)

    Uhlig, Christiane; Kirkpatrick, John B.; D'Hondt, Steven; Loose, Brice

    2018-06-01

    Marine microbial communities can consume dissolved methane before it can escape to the atmosphere and contribute to global warming. Seawater over the shallow Arctic shelf is characterized by excess methane compared to atmospheric equilibrium. This methane originates in sediment, permafrost, and hydrate. Particularly high concentrations are found beneath sea ice. We studied the structure and methane oxidation potential of the microbial communities from seawater collected close to Utqiagvik, Alaska, in April 2016. The in situ methane concentrations were 16.3 ± 7.2 nmol L-1, approximately 4.8 times oversaturated relative to atmospheric equilibrium. The group of methane-oxidizing bacteria (MOB) in the natural seawater and incubated seawater was > 97 % dominated by Methylococcales (γ-Proteobacteria). Incubations of seawater under a range of methane concentrations led to loss of diversity in the bacterial community. The abundance of MOB was low with maximal fractions of 2.5 % at 200 times elevated methane concentration, while sequence reads of non-MOB methylotrophs were 4 times more abundant than MOB in most incubations. The abundances of MOB as well as non-MOB methylotroph sequences correlated tightly with the rate constant (kox) for methane oxidation, indicating that non-MOB methylotrophs might be coupled to MOB and involved in community methane oxidation. In sea ice, where methane concentrations of 82 ± 35.8 nmol kg-1 were found, Methylobacterium (α-Proteobacteria) was the dominant MOB with a relative abundance of 80 %. Total MOB abundances were very low in sea ice, with maximal fractions found at the ice-snow interface (0.1 %), while non-MOB methylotrophs were present in abundances similar to natural seawater communities. The dissimilarities in MOB taxa, methane concentrations, and stable isotope ratios between the sea ice and water column point toward different methane dynamics in the two environments.

  11. Methane distribution and methane oxidation in the water column of the Elbe estuary, Germany

    Czech Academy of Sciences Publication Activity Database

    Matoušů, Anna; Osudar, R.; Šimek, Karel; Bussmann, I.

    2017-01-01

    Roč. 79, č. 3 (2017), s. 443-458 ISSN 1015-1621 R&D Projects: GA ČR(CZ) GA13-00243S Institutional support: RVO:60077344 Keywords : estuary * methane * methane budget * ethane oxidation * River Elbe Subject RIV: DA - Hydrology ; Limnology OBOR OECD: Marine biology, freshwater biology, limnology Impact factor: 2.821, year: 2016

  12. Final Technical Report: Metal—Organic Surface Catalyst for Low-temperature Methane Oxidation: Bi-functional Union of Metal—Organic Complex and Chemically Complementary Surface

    Energy Technology Data Exchange (ETDEWEB)

    Tait, Steven L. [Indiana Univ., Bloomington, IN (United States)

    2016-10-01

    serve as easily tuned model systems for exploring the chemistry of single-site transition metals and tandem catalysts that could then be developed into a zeolite or other stable support structures. In this final technical report, three major advances our described that further these goals. The first is a study demonstrating the ability to tune the oxidation state of V single-site centers on a surface by design of the surrounding ligand field. The synthesis of the single-site centers was developed in a previous reporting period of this project and this new advance shows a distinct new ability of the systems to have a designed oxidation state of the metal center. Second, we demonstrate metal complexation at surfaces using vibrational spectroscopy and also show a metal replacement reaction on Ag surfaces. Third, we demonstrate a surface-catalyzed dehydrocyclization reaction important for metal-organic catalyst design at surfaces.

  13. Artificial electron acceptors decouple archaeal methane oxidation from sulfate reduction.

    Science.gov (United States)

    Scheller, Silvan; Yu, Hang; Chadwick, Grayson L; McGlynn, Shawn E; Orphan, Victoria J

    2016-02-12

    The oxidation of methane with sulfate is an important microbial metabolism in the global carbon cycle. In marine methane seeps, this process is mediated by consortia of anaerobic methanotrophic archaea (ANME) that live in syntrophy with sulfate-reducing bacteria (SRB). The underlying interdependencies within this uncultured symbiotic partnership are poorly understood. We used a combination of rate measurements and single-cell stable isotope probing to demonstrate that ANME in deep-sea sediments can be catabolically and anabolically decoupled from their syntrophic SRB partners using soluble artificial oxidants. The ANME still sustain high rates of methane oxidation in the absence of sulfate as the terminal oxidant, lending support to the hypothesis that interspecies extracellular electron transfer is the syntrophic mechanism for the anaerobic oxidation of methane. Copyright © 2016, American Association for the Advancement of Science.

  14. Termites facilitate methane oxidation and shape the methanotrophic community.

    Science.gov (United States)

    Ho, Adrian; Erens, Hans; Mujinya, Basile Bazirake; Boeckx, Pascal; Baert, Geert; Schneider, Bellinda; Frenzel, Peter; Boon, Nico; Van Ranst, Eric

    2013-12-01

    Termite-derived methane contributes 3 to 4% to the total methane budget globally. Termites are not known to harbor methane-oxidizing microorganisms (methanotrophs). However, a considerable fraction of the methane produced can be consumed by methanotrophs that inhabit the mound material, yet the methanotroph ecology in these environments is virtually unknown. The potential for methane oxidation was determined using slurry incubations under conditions with high (12%) and in situ (∼0.004%) methane concentrations through a vertical profile of a termite (Macrotermes falciger) mound and a reference soil. Interestingly, the mound material showed higher methanotrophic activity. The methanotroph community structure was determined by means of a pmoA-based diagnostic microarray. Although the methanotrophs in the mound were derived from populations in the reference soil, it appears that termite activity selected for a distinct community. Applying an indicator species analysis revealed that putative atmospheric methane oxidizers (high-indicator-value probes specific for the JR3 cluster) were indicative of the active nest area, whereas methanotrophs belonging to both type I and type II were indicative of the reference soil. We conclude that termites modify their environment, resulting in higher methane oxidation and selecting and/or enriching for a distinct methanotroph population.

  15. Electrochemical and partial oxidation of methane

    Science.gov (United States)

    Singh, Rahul

    2008-10-01

    negligible coke formation on the novel fabricated anode by electroless plating process. Hydrogen is an environmentally cleaner source of energy. The recent increase in the demand of hydrogen as fuel for all types of fuel cells and petroleum refining process has boosted the need of production of hydrogen. Methane, a major component of natural gas is the major feedstock for production of hydrogen. The route of partial oxidation of methane to produce syngas (CO + H2) offers significant advantages over commercialized steam reforming process for higher efficiency and lower energy requirements. Partial oxidation of methane was studied by pulsing O2 into a CH4 flow over Rh/Al2O3 in a sequence of in situ infrared (IR) cell and fixed bed reactor at 773 K. The results obtained from the sequence of an IR cell followed by a fixed bed reactor show that (i) adsorbed CO produced possesses a long residence time, indicating that adsorbed oxygen leading to the formation of CO is significantly different from those leading to CO2 and (ii) CO2 is not an intermediate species for the formation of CO. In situ IR of pulse reaction coupled with alternating reactor sequence is an effective approach to study the primary and secondary reactions as well as the nature of their adsorbed species. As reported earlier, hydrogen remains to be the most effective fuel for fuel cells, the production of high purity hydrogen from naturally available resources such as coal, petroleum, and natural gas requires a number of energy-intensive steps, making fuel cell processes for stationary electric power generation prohibitively uneconomic. Direct use of coal or coal gas as the feed is a promising approach for low cost electricity generation. Coal gas solid oxide fuel cell was studied by pyrolyzing Ohio #5 coal to coal gas and transporting to a Cu anode solid oxide fuel cell to generate power. The study of coal-gas solid oxide fuel cell is divided into two sections, i.e., (i) understanding the composition of coal gas by

  16. Microbial methane oxidation processes and technologies for mitigation of landfill gas emissions

    DEFF Research Database (Denmark)

    Scheutz, Charlotte; Kjeldsen, Peter; Bogner, J.E.

    2009-01-01

    Landfill gas containing methane is produced by anaerobic degradation of organic waste. Methane is a strong greenhouse gas and landfills are one of the major anthropogenic sources of atmospheric methane. Landfill methane may be oxidized by methanotrophic microorganisms in soils or waste materials...... to predict methane emissions from landfills. Additional research and technology development is needed before methane mitigation technologies utilizing microbial methane oxidation processes can become commercially viable and widely deployed....

  17. Anaerobic methane oxidation coupled to denitrification is the dominant methane sink in a deep lake

    DEFF Research Database (Denmark)

    Deutzmann, Joerg S.; Stief, Peter; Brandes, Josephin

    2014-01-01

    Anaerobic methane oxidation coupled to denitrification, also known as “nitrate/nitrite-dependent anaerobic methane oxidation” (n-damo), was discovered in 2006. Since then, only a few studies have identified this process and the associated microorganisms in natural environments. In aquatic sediments......, the close proximity of oxygen- and nitrate-consumption zones can mask n-damo as aerobic methane oxidation. We therefore investigated the vertical distribution and the abundance of denitrifying methanotrophs related to Candidatus Methylomirabilis oxyfera with cultivation-independent molecular techniques...... in the sediments of Lake Constance. Additionally, the vertical distribution of methane oxidation and nitrate consumption zones was inferred from high-resolution microsensor profiles in undisturbed sediment cores. M. oxyfera-like bacteria were virtually absent at shallow-water sites (littoral sediment) and were...

  18. Catalytic conversion of methane: Carbon dioxide reforming and oxidative coupling

    KAUST Repository

    Takanabe, Kazuhiro

    2012-01-01

    and the oxidative coupling of methane. These two reactions have tremendous technological significance for practical application in industry. An understanding of the fundamental aspects and reaction mechanisms of the catalytic reactions reviewed in this study would

  19. Rain increases methane production and methane oxidation in a boreal thermokarst bog

    Science.gov (United States)

    Neumann, R. B.; Moorberg, C.; Turner, J.; Wong, A.; Waldrop, M. P.; Euskirchen, E. S.; Edgar, C.; Turetsky, M. R.

    2017-12-01

    Bottom-up biogeochemical models of wetland methane emissions simulate the response of methane production, oxidation and transport to wetland conditions and environmental forcings. One reason for mismatches between bottom-up and top-down estimates of emissions is incomplete knowledge of factors and processes that control microbial rates and methane transport. To advance mechanistic understanding of wetland methane emissions, we conducted a multi-year field investigation and plant manipulation experiment in a thermokarst bog located near Fairbanks, Alaska. The edge of the bog is experiencing active permafrost thaw, while the center of the bog thawed 50 to 100 years ago. Our study, which captured both an average year and two of the wettest years on record, revealed how rain interacts with vascular vegetation and recently thawed permafrost to affect methane emissions. In the floating bog, rain water warmed and oxygenated the subsurface, but did not alter soil saturation. The warmer peat temperatures increased both microbial methane production and plant productivity at the edge of the bog near the actively thawing margin, but minimally altered microbial and plant activity in the center of the bog. These responses indicate processes at the edge of the bog were temperature limited while those in the center were not. The compounding effect of increased microbial activity and plant productivity at the edge of the bog doubled methane emissions from treatments with vascular vegetation during rainy years. In contrast, methane emissions from vegetated treatments in the center of the bog did not change with rain. The oxygenating influence of rain facilitated greater methane oxidation in treatments without vascular vegetation, which offset warming-induced increases in methane production at the edge of the bog and decreased methane emissions in the center of the bog. These results elucidate the complex and spatially variable response of methane production and oxidation in

  20. Anaerobic methane oxidation rates at the sulfate-methane transition in marine sediments from Kattegat and Skagerrak (Denmark)

    International Nuclear Information System (INIS)

    Iversen, N.; Jorgensen, B.B.

    1985-01-01

    Concomitant radiotracer measurements were made of in situ rates of sulfate reduction and anaerobic methane oxidation in 2-3-m-long sediment cores. Methane accumulated to high concentrations (> 1 mM CH 4 ) only below the sulfate zone, at 1 m or deeper in the sediment. Sulfate reduction showed a broad maximum below the sediment surface and a smaller, narrow maximum at the sulfate-methane transition. Methane oxidation was low (0.002-0.1 nmol CH 4 cm -3 d -1 ) throughout the sulfate zone and showed a sharp maximum at the sulfate-methane transition, coinciding with the sulfate reduction maximum. Total anaerobic methane oxidation at two stations was 0.83 and 1.16 mmol CH 4 m -2 d -1 , of which 96% was confined to the sulfate-methane transition. All the methane that was calculated to diffuse up into the sulfate-methane transition was oxidized in this zone. The methane oxidation was equivalent to 10% of the electron donor requirement for the total measured sulfate reduction. A third station showed high sulfate concentrations at all depths sampled and the total methane oxidation was only 0.013 mmol m -2 d -1 . From direct measurements of rates, concentration gradients, and diffusion coefficients, simple calculations were made of sulfate and methane fluxes and of methane production rates

  1. Application of the GRI 1.2 Methane Oxidation Model to Methane and Methanol Oxidation in Supercritical Water

    National Research Council Canada - National Science Library

    Rice, Steven

    1997-01-01

    The Gas Research Institute (GRI) has been leading an effort over the past few years to consolidate recent developments in the elementary reaction modeling of the oxidation of methane for combustion applications into a single...

  2. Anaerobic methane oxidation coupled to denitrification is the dominant methane sink in a deep lake.

    Science.gov (United States)

    Deutzmann, Joerg S; Stief, Peter; Brandes, Josephin; Schink, Bernhard

    2014-12-23

    Anaerobic methane oxidation coupled to denitrification, also known as "nitrate/nitrite-dependent anaerobic methane oxidation" (n-damo), was discovered in 2006. Since then, only a few studies have identified this process and the associated microorganisms in natural environments. In aquatic sediments, the close proximity of oxygen- and nitrate-consumption zones can mask n-damo as aerobic methane oxidation. We therefore investigated the vertical distribution and the abundance of denitrifying methanotrophs related to Candidatus Methylomirabilis oxyfera with cultivation-independent molecular techniques in the sediments of Lake Constance. Additionally, the vertical distribution of methane oxidation and nitrate consumption zones was inferred from high-resolution microsensor profiles in undisturbed sediment cores. M. oxyfera-like bacteria were virtually absent at shallow-water sites (littoral sediment) and were very abundant at deep-water sites (profundal sediment). In profundal sediment, the vertical distribution of M. oxyfera-like bacteria showed a distinct peak in anoxic layers that coincided with the zone of methane oxidation and nitrate consumption, a strong indication for n-damo carried out by M. oxyfera-like bacteria. Both potential n-damo rates calculated from cell densities (660-4,890 µmol CH4⋅m(-2)⋅d(-1)) and actual rates calculated from microsensor profiles (31-437 µmol CH4⋅m(-2)⋅d(-1)) were sufficiently high to prevent methane release from profundal sediment solely by this process. Additionally, when nitrate was added to sediment cores exposed to anoxic conditions, the n-damo zone reestablished well below the sediment surface, completely preventing methane release from the sediment. We conclude that the previously overlooked n-damo process can be the major methane sink in stable freshwater environments if nitrate is available in anoxic zones.

  3. Trace methane oxidation and the methane dependency of sulfate reduction in anaerobic granular sludge

    KAUST Repository

    Meulepas, Roel J.W.; Jagersma, Christian G.; Zhang, Yu; Petrillo, Michele; Cai, Hengzhe; Buisman, Cees J.N.; Stams, Alfons J.M.; Lens, Piet N.L.

    2010-01-01

    This study investigates the oxidation of labeled methane (CH4) and the CH4 dependence of sulfate reduction in three types of anaerobic granular sludge. In all samples, 13C-labeled CH4 was anaerobically oxidized to 13C-labeled CO2, while net

  4. Atmospheric methane removal by methane-oxidizing bacteria immobilized on porous building materials.

    Science.gov (United States)

    Ganendra, Giovanni; De Muynck, Willem; Ho, Adrian; Hoefman, Sven; De Vos, Paul; Boeckx, Pascal; Boon, Nico

    2014-04-01

    Biological treatment using methane-oxidizing bacteria (MOB) immobilized on six porous carrier materials have been used to mitigate methane emission. Experiments were performed with different MOB inoculated in building materials at high (~20 % (v/v)) and low (~100 ppmv) methane mixing ratios. Methylocystis parvus in autoclaved aerated concrete (AAC) exhibited the highest methane removal rate at high (28.5 ± 3.8 μg CH₄ g⁻¹ building material h⁻¹) and low (1.7 ± 0.4 μg CH₄ g⁻¹ building material h⁻¹) methane mixing ratio. Due to the higher volume of pores with diameter >5 μm compared to other materials tested, AAC was able to adsorb more bacteria which might explain for the higher methane removal observed. The total methane and carbon dioxide-carbon in the headspace was decreased for 65.2 ± 10.9 % when M. parvus in Ytong was incubated for 100 h. This study showed that immobilized MOB on building materials could be used to remove methane from the air and also act as carbon sink.

  5. Platinum single crystal electrodes for the electrocatalysis of methane oxidation

    Directory of Open Access Journals (Sweden)

    Mayara Munaretto

    2011-03-01

    Full Text Available The main objective of this paper is to characterize the voltammetric profiles of platinum single crystals of low Miller indexes Pt(100 and Pt(110 and study their catalytic activities on the oxidation of methane. In this way, it was developed a metallic surface modified by presence of other metal oxide, which presents catalytic activity for this reaction. It is well known that the electrooxidation of methane (CH4 leads mainly to the formation of CO2 and H2O, however, the oxidation can also lead to the formation of CO, a reaction intermediate that has strong interaction with metal surfaces, such as platinum. This molecule tends to accumulate on the platinum surface and to passive it, due to the self-poisoning, decreasing its catalytic activity. Therefore, the main aim of this work was the development of a platinum electrode modified by deposition of titanium oxide, which presented electrocatalytic properties for the oxidation of methane.

  6. Anaerobic methane oxidation coupled to denitrification is the dominant methane sink in a deep lake

    Science.gov (United States)

    Deutzmann, Joerg S.; Stief, Peter; Brandes, Josephin; Schink, Bernhard

    2014-01-01

    Anaerobic methane oxidation coupled to denitrification, also known as “nitrate/nitrite-dependent anaerobic methane oxidation” (n-damo), was discovered in 2006. Since then, only a few studies have identified this process and the associated microorganisms in natural environments. In aquatic sediments, the close proximity of oxygen- and nitrate-consumption zones can mask n-damo as aerobic methane oxidation. We therefore investigated the vertical distribution and the abundance of denitrifying methanotrophs related to Candidatus Methylomirabilis oxyfera with cultivation-independent molecular techniques in the sediments of Lake Constance. Additionally, the vertical distribution of methane oxidation and nitrate consumption zones was inferred from high-resolution microsensor profiles in undisturbed sediment cores. M. oxyfera-like bacteria were virtually absent at shallow-water sites (littoral sediment) and were very abundant at deep-water sites (profundal sediment). In profundal sediment, the vertical distribution of M. oxyfera-like bacteria showed a distinct peak in anoxic layers that coincided with the zone of methane oxidation and nitrate consumption, a strong indication for n-damo carried out by M. oxyfera-like bacteria. Both potential n-damo rates calculated from cell densities (660–4,890 µmol CH4⋅m−2⋅d−1) and actual rates calculated from microsensor profiles (31–437 µmol CH4⋅m−2⋅d−1) were sufficiently high to prevent methane release from profundal sediment solely by this process. Additionally, when nitrate was added to sediment cores exposed to anoxic conditions, the n-damo zone reestablished well below the sediment surface, completely preventing methane release from the sediment. We conclude that the previously overlooked n-damo process can be the major methane sink in stable freshwater environments if nitrate is available in anoxic zones. PMID:25472842

  7. Nitrogen as a regulatory factor of methane oxidation in soils and sediments

    NARCIS (Netherlands)

    Bodelier, P.L.E.; Laanbroek, H.J.

    2004-01-01

    The oxidation of methane by methane-oxidising microorganisms is an important link in the global methane budget. Oxic soils are a net sink while wetland soils are a net source of atmospheric methane. It has generally been accepted that the consumption of methane in upland as well as lowland systems

  8. Formation of methane and nitrous oxide in plants

    Science.gov (United States)

    Keppler, Frank; Lenhart, Katharina

    2017-04-01

    Methane, the second important anthropogenic greenhouse gas after carbon dioxide, is the most abundant reduced organic compound in the atmosphere and plays a central role in atmospheric chemistry. The global atmospheric methane budget is determined by many natural and anthropogenic terrestrial and aquatic surface sources, balanced primarily by one major sink (hydroxyl radicals) in the atmosphere. Natural sources of atmospheric methane in the biosphere have until recently been attributed to originate solely from strictly anaerobic microbial processes in wetland soils and rice paddies, the intestines of termites and ruminants, human and agricultural waste, and from biomass burning, fossil fuel mining and geological sources including mud volcanoes and seeps. However, recent studies suggested that terrestrial vegetation, fungi and mammals may also produce methane without the help of methanogens and under aerobic conditions (e.g. Keppler et al. 2009, Wang et al. 2013). These novel sources have been termed "aerobic methane production" to distinguish them from the well-known anaerobic methane production pathway. Nitrous oxide is another important greenhouse gas and major source of ozone-depleting nitric oxide. About two thirds of nitrous oxide emissions are considered to originate from anthropogenic and natural terrestrial sources, and are almost exclusively related to microbial processes in soils and sediments. However, the global nitrous oxide budget still has major uncertainties since it is unclear if all major sources have been identified but also the emission estimates of the know sources and stratospheric sink are afflicted with high uncertainties. Plants contribute, although not yet quantified, to nitrous oxide emissions either indirectly as conduits of soil derived nitrous oxide (Pihlatie et al. 2005), or directly via generation of nitrous oxide in leaves (Dean & Harper 1986) or on the leaf surface induced by UV irradiation (Bruhn et al. 2014). Moreover, lichens

  9. A laboratory study of anaerobic oxidation of methane in the presence of methane hydrate

    Science.gov (United States)

    Solem, R.; Bartlett, D.; Kastner, M.; Valentine, D.

    2003-12-01

    In order to mimic and study the process of anaerobic methane oxidation in methane hydrate regions we developed four high-pressure anaerobic bioreactors, designed to incubate environmental sediment samples, and enrich for populations of microbes associated with anaerobic methane oxidation (AMO). We obtained sediment inocula from a bacterial mat at the southern Hydrate Ridge, Cascadia, having cell counts approaching 1010 cells/cc. Ultimately, our goal is to produce an enriched culture of these microbes for characterization of the biochemical processes and chemical fluxes involved, as well as the unique adaptations required for, AMO. Molecular phylogenetic information along with results from fluorescent in situ hybridization indicate that consortia of Archaea and Bacteria are present which are related to those previously described for marine sediment AMO environments. Using a medium of enriched seawater and sediment in a 3:1 ratio, the system was incubated at 4° C under 43 atm of methane pressure; the temperature and pressure were kept constant. We have followed the reactions for seven months, particularly the vigorous consumption rates of dissolved sulfate and alkalinity production, as well as increases in HS-, and decreases in Ca concentrations. We also monitored the dissolved inorganic C (DIC) δ 13C values. The data were reproduced, and indicated that the process is extremely sensitive to changes in methane pressure. The rates of decrease in sulfate and increase in alkalinity concentrations were complimentary and showed considerable linearity with time. When the pressure in the reactor was decreased below the methane hydrate stability field, following the methane hydrate dissociation, sulfate reduction abruptly decreased. When the pressure was restored all the reactions returned to their previous rates. Much of the methane oxidation activity in the reactor is believed to occur in association with the methane hydrate. Upon the completion of one of the experiments

  10. Anaerobic Oxidization of Methane in a Minerotrophic Peatland: Enrichment of Nitrite-Dependent Methane-Oxidizing Bacteria

    Science.gov (United States)

    Zhu, Baoli; van Dijk, Gijs; Fritz, Christian; Smolders, Alfons J. P.; Pol, Arjan; Jetten, Mike S. M.

    2012-01-01

    The importance of anaerobic oxidation of methane (AOM) as a methane sink in freshwater systems is largely unexplored, particularly in peat ecosystems. Nitrite-dependent anaerobic methane oxidation (n-damo) was recently discovered and reported to be catalyzed by the bacterium “Candidatus Methylomirabilis oxyfera,” which is affiliated with the NC10 phylum. So far, several “Ca. Methylomirabilis oxyfera” enrichment cultures have been obtained using a limited number of freshwater sediments or wastewater treatment sludge as the inoculum. In this study, using stable isotope measurements and porewater profiles, we investigated the potential of n-damo in a minerotrophic peatland in the south of the Netherlands that is infiltrated by nitrate-rich ground water. Methane and nitrate profiles suggested that all methane produced was oxidized before reaching the oxic layer, and NC10 bacteria could be active in the transition zone where countergradients of methane and nitrate occur. Quantitative PCR showed high NC10 bacterial cell numbers at this methane-nitrate transition zone. This soil section was used to enrich the prevalent NC10 bacteria in a continuous culture supplied with methane and nitrite at an in situ pH of 6.2. An enrichment of nitrite-reducing methanotrophic NC10 bacteria was successfully obtained. Phylogenetic analysis of retrieved 16S rRNA and pmoA genes showed that the enriched bacteria were very similar to the ones found in situ and constituted a new branch of NC10 bacteria with an identity of less than 96 and 90% to the 16S rRNA and pmoA genes of “Ca. Methylomirabilis oxyfera,” respectively. The results of this study expand our knowledge of the diversity and distribution of NC10 bacteria in the environment and highlight their potential contribution to nitrogen and methane cycles. PMID:23042166

  11. Environmental evidence for net methane production and oxidation in putative ANaerobic MEthanotrophic (ANME) archaea

    DEFF Research Database (Denmark)

    Lloyd, Karen; Teske, Andreas; Alperin, Marc J.

    2011-01-01

    . Anaerobic methane oxidation regulates methane emissions in marine sediments and appears to occur through a reversal of a methane-producing metabolism. We tested the assumption that ANME are obligate methanotrophs by detecting and quantifying gene transcription of ANME-1 across zones of methane oxidation...

  12. Graphene oxide as an optimal candidate material for methane storage.

    Science.gov (United States)

    Chouhan, Rajiv K; Ulman, Kanchan; Narasimhan, Shobhana

    2015-07-28

    Methane, the primary constituent of natural gas, binds too weakly to nanostructured carbons to meet the targets set for on-board vehicular storage to be viable. We show, using density functional theory calculations, that replacing graphene by graphene oxide increases the adsorption energy of methane by 50%. This enhancement is sufficient to achieve the optimal binding strength. In order to gain insight into the sources of this increased binding, that could also be used to formulate design principles for novel storage materials, we consider a sequence of model systems that progressively take us from graphene to graphene oxide. A careful analysis of the various contributions to the weak binding between the methane molecule and the graphene oxide shows that the enhancement has important contributions from London dispersion interactions as well as electrostatic interactions such as Debye interactions, aided by geometric curvature induced primarily by the presence of epoxy groups.

  13. Constraining the relationships between anaerobic oxidation of methane and sulfate reduction under in situ methane concentrations

    Science.gov (United States)

    Zhuang, G.; Wegener, G.; Joye, S. B.

    2017-12-01

    The anaerobic oxidation of methane (AOM) is an important microbial metabolism in the global carbon cycle. In marine methane seeps sediment, this process is mediated by syntrophic consortium that includes anaerobic methanotrophic archaea (ANME) and sulfate-reducing bacteria (SRB). Stoichiometrically in AOM methane oxidation should be coupled to sulfate reduction (SR) in a 1:1 ratio. However, weak coupling of AOM and SR in seep sediments was frequently observed from the ex situ rate measurements, and the metabolic dynamics of AOM and SR under in situ conditions remain poorly understood. Here we investigated the metabolic activity of AOM and SR with radiotracers by restoring in situ methane concentrations under pressure to constrain the in situ relationships between AOM and SR in the cold seep sediments of Gulf of Mexico as well as the sediment-free AOM enrichments cultivated from cold seep of Italian Island Elba or hydrothermal vent of Guaymas Basin5. Surprisingly, we found that AOM rates strongly exceeded those of SR when high pressures and methane concentrations were applied at seep sites of GC600 and GC767 in Gulf of Mexico. With the addition of molybdate, SR was inhibited but AOM was not affected, suggesting the potential coupling of AOM with other terminal processes. Amendments of nitrate, iron, manganese and AQDS to the SR-inhibited slurries did not stimulate or inhibit the AOM activity, indicating either those electron acceptors were not limiting for AOM in the sediments or AOM was coupled to other process (e.g., organic matter). In the ANME enrichments, higher AOM rates were also observed with the addition of high concentrations of methane (10mM and 50 mM). The tracer transfer of CO2 to methane, i.e., the back reaction of AOM, increased with increasing methane concentrations and accounted for 1%-5% of the AOM rates. AOM rates at 10 mM and 50 mM methane concentration were much higher than the SR rates, suggesting those two processes were not tightly coupled

  14. Methane oxidation in contrasting soil types

    DEFF Research Database (Denmark)

    D'Imperio, Ludovica; Nielsen, Cecilie Skov; Westergaard-Nielsen, Andreas

    2017-01-01

    Arctic ecosystems are characterized by a wide range of soil moisture conditions and thermal regimes and contribute differently to the net methane (CH4) budget. Yet, it is unclear how climate change will affect the capacity of those systems to act as a net source or sink of CH4. Here, we present...... subsequently scaled to the entire study area of 0.15 km2, a landscape also consisting of wetlands with a seasonally integrated methane release of 0.10 ± 0.01 g CH4-C m−2 (3.7 ± 1.2 g CO2-eq m−2). The result was a net landscape sink of 12.71 kg CH4-C (0.48 tonne CO2-eq) during the growing season...

  15. Combined gas-phase oxidation of methane and ethylene

    International Nuclear Information System (INIS)

    Pogosyan, N.M.; Pogosyan, M.D.

    2009-01-01

    It is established that depending on the reaction conditions combined oxidation of methane and ethylene may result in ethylene and propylene oxides with high selectivity with respect to the process, where in the initial reaction mixture methane is replaced by the same quantity of nitrogen. The formed additional methyl radicals increase the yield of all reaction products except CO. At low temperatures methyl radicals react with oxygen resulting in methyl peroxide radicals, which in turn, reacting with ethylene provide its epoxidation and formation of other oxygen-containing products. At high temperatures as a result of addition reaction between methyl radicals and ethylene, propyl radicals are formed that, in turn yield propylene. Alongside with positive influence on the yield of reaction products, methane exerts negative influence upon the conversion, that is it decreases the rate of ethylene and oxygen conversion, simultaneously decreasing significantly the yield of CO

  16. Catalytic conversion of methane: Carbon dioxide reforming and oxidative coupling

    KAUST Repository

    Takanabe, Kazuhiro

    2012-01-01

    Natural gas conversion remains one of the essential technologies for current energy needs. This review focuses on the mechanistic aspects of the development of efficient and durable catalysts for two reactions, carbon dioxide reforming and the oxidative coupling of methane. These two reactions have tremendous technological significance for practical application in industry. An understanding of the fundamental aspects and reaction mechanisms of the catalytic reactions reviewed in this study would support the design of industrial catalysts. CO 2 reforming of methane utilizes CO 2, which is often stored in large quantities, to convert as a reactant. Strategies to eliminate carbon deposition, which is the major problem associated with this reaction, are discussed. The oxidative coupling of methane directly produces ethylene in one reactor through a slightly exothermic reaction, potentially minimizing the capital cost of the natural gas conversion process. The focus of discussion in this review will be on the attainable yield of C 2 products by rigorous kinetic analyses.

  17. Methane oxidation at low temperatures in soil exposed to landfill gas

    DEFF Research Database (Denmark)

    Christophersen, Mette; Linderød, L.; Jensen, Pernille Erland

    2000-01-01

    soil moisture regimes, At 2 degreesC the methane oxidation rates were 0.005 to 0.17 mu mol g(-1) h(-1), and calculations showed that it was possible to oxidize all the produced methane at older landfills, even during the winter. Therefore, methane oxidation in top covers of landfills is an alternative...

  18. Methane oxidation and degradation of organic compounds in landfill soil covers

    DEFF Research Database (Denmark)

    Scheutz, Charlotte; Kjeldsen, Peter

    2002-01-01

    High rates of methane oxidation and degradation of the lowed halogenated methanes (TCM and DCM) and HCFCs (HCFC-21 and HCFC-22) were found in an investigation of the oxidation of methane and halogenated organic compunds (HOCs) in landfill gas affected soil. The degradation followed zero-order kin......High rates of methane oxidation and degradation of the lowed halogenated methanes (TCM and DCM) and HCFCs (HCFC-21 and HCFC-22) were found in an investigation of the oxidation of methane and halogenated organic compunds (HOCs) in landfill gas affected soil. The degradation followed zero...

  19. Direct methane and nitrous oxide emissions of monogastric livestock ...

    African Journals Online (AJOL)

    The Intergovernmental Panel on Climate Change (IPCC) methodology adapted to tropical production systems was used to calculate methane (CH4) and nitrous oxide (N2O) emissions. The non-ruminant sector is a minor GHG contributor compared with ruminant CH4 and N2O emissions. The pig industry and ostrich ...

  20. A mechanistic model on methane oxidation in the rice rhizosphere

    NARCIS (Netherlands)

    Bodegom, van P.M.; Leffelaar, P.A.; Goudriaan, J.

    2001-01-01

    A mechanistic model is presented on the processes leading to methane oxidation in rice rhizosphere. The model is driven by oxygen release from a rice root into anaerobic rice soil. Oxygen is consumed by heterotrophic and methanotrophic respiration, described by double Monod kinetics, and by iron

  1. The oxidative coupling of methane with cofeeding of ethane

    NARCIS (Netherlands)

    Chen, Q.; Couwenberg, P.M.; Marin, G.B.

    1994-01-01

    The oxidative coupling of methane with cofeeding of ethane was investigated experimentally both in the absence and in the presence of a Sn/Li/MgO catalyst. Cofeeding ethane in the absence of catalyst results in a higher total radical concentration, explaining the strong increase of the observed feed

  2. Non-oxidative conversion of methane into higher hydrocarbons over ...

    Indian Academy of Sciences (India)

    SOURABH MISHRA

    2017-09-27

    Sep 27, 2017 ... ... in the Design and Development of Catalysts and their Applications ... of methane (natural gas) into transportable chemicals ... molybdenum (Mo) catalyst under non-oxidative condi- ... Micromeritics ASAP 2010 apparatus at liquid nitrogen tem- ... fixed-bed tubular reactor (500 mm length & 15 mm ID) at.

  3. Non-oxidative conversion of methane into higher hydrocarbons over ...

    Indian Academy of Sciences (India)

    SOURABH MISHRA

    2017-09-27

    Sep 27, 2017 ... (Syn-gas, CO+H2) formation via steam reforming, dry reforming or partial oxidation of methane ... Micromeritics ASAP 2010 apparatus at liquid nitrogen tem- perature. Nitrogen (N2) was the adsorbate ... some runs were carried out in triplicate and mass balance for all the runs was measured. Runs with a ...

  4. Spatial variability in nitrous oxide and methane emissions from beef cattle feedyard pen surfaces

    Science.gov (United States)

    Greenhouse gas emissions from beef cattle feedlots include enteric carbon dioxide and methane, and manure-derived methane, nitrous oxide and carbon dioxide. Enteric methane comprises the largest portion of the greenhouse gas footprint of beef cattle feedyards. For the manure component, methane is th...

  5. Market research on biogas valorizations and methanization. Final report

    International Nuclear Information System (INIS)

    2010-09-01

    This market research aims at giving an overview of the existing methanization installations and of their dynamics in France, at assessing biogas production and use, at analyzing the methanization market, and at defining development perspectives for this sector by 2020. Based on a survey of methanization installations, on interviews with many actors of this sector, and on a seminar organized on this topic, this report presents and comments market data for biogas valorization and methanization in different sectors: household, agricultural, and industrial and waste water processing plants. It comments evolution trends by 2020 for these sectors, and the role that the emerging sector of centralized methanization could have in the years to come

  6. Methane and Trichloroethylene Oxidation by an Estuarine Methanotroph, Methylobacter sp. Strain BB5.1

    OpenAIRE

    Smith, Kelly S.; Costello, Andria M.; Lidstrom, Mary E.

    1998-01-01

    An estuarine methanotroph was isolated from sediment enrichments and designated Methylobacter sp. strain BB5.1. In cells grown on medium with added copper, oxidation of methane and trichloroethylene occurred with similar Ks values, but the Vmax for trichloroethylene oxidation was only 0.1% of the methane oxidation Vmax. Cells grown on low-copper medium did not oxidize trichloroethylene and showed a variable rate of methane oxidation.

  7. The Geologic Signature of Anaerobic Oxidation of Methane (Invited)

    Science.gov (United States)

    Ussler, W.; Paull, C. K.

    2010-12-01

    Anaerobic oxidation of methane (AOM) is an enormous sink in anoxic marine sediments for methane produced in situ or ascending through the sediment column towards the seafloor. Existing estimates indicate that between 75 and 382 Tg of sedimentary methane are oxidized each year before reaching the sediment-water interface making AOM a diagenetic process of global significance. This methane is derived from a variety of sources including microbial production, thermocatalytic cracking of complex organic matter, decomposing gas hydrates, and possibly abiogenic processes. Stables isotopes of membrane lipid biomarkers and authigenic carbonates associated with zones of AOM, fluorescence in situ hybridization, and anaerobic methane incubations have substantiated the role Archaea and sulfate-reducing bacteria have in driving AOM. The products of AOM are dissolved inorganic carbon (predominantly HCO3-) and bisulfide (HS-). Stable isotope measurements of authigenic carbonates associated with zones of AOM are consistent with the diagenetic carbon being primarily methane derived. These methane-derived carbonates occur in a variety of forms including sedimentary nodules and thin lenses within and below zones of contemporary AOM; outcrops of slabs, ledges, and jagged authigenic carbonates exhumed on the seafloor; and authigenic carbonate mounds associated with near-subsurface methane gas accumulations. Examples of exhumed authigenic carbonates include rugged outcrops along the Guaymas Transform in the Gulf of California, extensive slabs and ledges in the Eel River Basin, and mounds in various stages of development near Bullseye Vent, off Vancouver Island and in the Santa Monica Basin. It is clear from basic microbial biogeochemistry and the occurrences of massive authigenic carbonate which span a large range in size that DIC produced by AOM is preserved as authigenic carbonate within the seafloor and not on the seafloor. These exhumed authigenic carbonate provide a glimpse of how

  8. The integrated nitrous oxide and methane grassland project

    Energy Technology Data Exchange (ETDEWEB)

    Leffelaar, P.A.; Langeveld, C.A.; Hofman, J.E.; Segers, R.; Van den Pol-van Dasselaar, A.; Goudriaan, J.; Rabbinge, R.; Oenema, O. [Department of Theoretical Production Ecology, Wageningen Agricultural University, Wageningen (Netherlands)

    2000-07-01

    The integrated nitrous oxide (N{sub 2}O) and methane (CH{sub 4}) grassland project aims to estimate and explain emissions of these greenhouse gases from two ecosystems, namely drained agricultural peat soil under grass at the experimental farm Zegveld and undrained peat in the nature preserve Nieuwkoopse Plassen, both Netherlands. Peat soils were chosen because of their expected considerable contribution to the greenhouse gas budget considering the prevailing wet and partial anaerobic conditions. The emission dynamics of these ecosystems are considered representatives of large peat areas because the underlying processes are rather general and driven by variables like organic matter characteristics, water and nutrient conditions and type of vegetation. The research approach comprises measurements and modelling at different integration levels relating to the microbiology of the production and consumption of N{sub 2}O and CH{sub 4} (laboratory studies), their movement through peat soil (rhizolab and field studies), and the resulting fluxes (field studies). Typical emissions from drained soil were 15-40 kg ha{sup -1} y{sup -1} N{sub 2}O and virtually zero for CH{sub 4}. The undrained soil in the nature preserve emitted 100-280 kg ha{sup -1} y{sup -1} CH{sub 4}, and probably little N{sub 2}O. The process knowledge, collected and partly integrated in the models, helps to explain these data. For example, the low methane emission from drained peat can more coherently be understood and extrapolated because: (1) upper soil layers are aerobic, thus limiting methane production and stimulating methane oxidation, (2) absence of aerenchymatous roots of wetland plants that connect deeper anaerobic soil layers where methane is produced to the atmosphere and supply labile carbon, (3) a low methane production potential in deep layers due to the low decomposability of organic matter, and (4) long anaerobic periods needed in the topsoil to develop a methane production potential. This

  9. Different Abilities of Eight Mixed Cultures of Methane-oxidizing Bacteria to Degrade TCE

    DEFF Research Database (Denmark)

    Broholm, Kim; Christensen, Thomas Højlund; Jensen, Bjørn K.

    1993-01-01

    The ability of eight mixed cultures of methane-oxidizing bacteria to degrade trichloroethylene (TCE) was examined in laboratory batch experiments. This is one of the first reported works studying TCE degradation by mixed cultures of methane-oxidizing bacteria at 10°C, a common temperature for soils...... methanol, but only for a limited time period of about 5 days. Several explanations for the discontinued degradation of TCE are given. An experiment carried out to re-activate the methane-oxidizing bacteria after 8 days of growth on methanol by adding methane did not immediately result in degradation...... of methane and TCE. During the first 10–15 days after the addition of methane a significant degradation of methane and a minor degradation of TCE were observed. This experiment revealed that the ability of mixed cultures of methane-oxidizing bacteria to degrade TCE varied significantly even though...

  10. Community composition and ultrastructure of a nitrate-dependent anaerobic methane-oxidizing enrichment culture

    NARCIS (Netherlands)

    Gambelli, L.; Guerrero-Cruz, Simon; Mesman, R.; Cremers, G.; Jetten, M.S.M.; Camp, H.J.M. op den; Lueke, Claudia; Niftrik, L.A.M.P. van

    2017-01-01

    Methane is a very potent greenhouse gas and can be oxidized aerobically or anaerobically through microbial-mediated processes, thus decreasing methane emissions to the atmosphere. Using a complementary array of methods including phylogenetic analysis, physiological experiments, and light and

  11. OXIDATIVE COUPLING OF METHANE USING INORGANIC MEMBRANE REACTORS

    Energy Technology Data Exchange (ETDEWEB)

    Dr. Y.H. Ma; Dr. W.R. Moser; Dr. A.G. Dixon; Dr. A.M. Ramachandra; Dr. Y. Lu; C. Binkerd

    1998-04-01

    The objective of this research is to study the oxidative coupling of methane in catalytic inorganic membrane reactors. A specific target is to achieve conversion of methane to C{sub 2} hydrocarbons at very high selectivity and higher yields than in conventional non-porous, co-feed, fixed bed reactors by controlling the oxygen supply through the membrane. A membrane reactor has the advantage of precisely controlling the rate of delivery of oxygen to the catalyst. This facility permits balancing the rate of oxidation and reduction of the catalyst. In addition, membrane reactors minimize the concentration of gas phase oxygen thus reducing non selective gas phase reactions, which are believed to be a main route for the formation of CO{sub x} products. Such gas phase reactions are a cause of decreased selectivity in the oxidative coupling of methane in conventional flow reactors. Membrane reactors could also produce higher product yields by providing better distribution of the reactant gases over the catalyst than the conventional plug flow reactors. Membrane reactor technology also offers the potential for modifying the membranes both to improve catalytic properties as well as to regulate the rate of the permeation/diffusion of reactants through the membrane to minimize by-product generation. Other benefits also exist with membrane reactors, such as the mitigation of thermal hot-spots for highly exothermic reactions such as the oxidative coupling of methane. The application of catalytically active inorganic membranes has potential for drastically increasing the yield of reactions which are currently limited by either thermodynamic equilibria, product inhibition, or kinetic selectivity.

  12. Trace methane oxidation and the methane dependency of sulfate reduction in anaerobic granular sludge

    KAUST Repository

    Meulepas, Roel J.W.

    2010-05-01

    This study investigates the oxidation of labeled methane (CH4) and the CH4 dependence of sulfate reduction in three types of anaerobic granular sludge. In all samples, 13C-labeled CH4 was anaerobically oxidized to 13C-labeled CO2, while net endogenous CH4 production was observed. Labeled-CH4 oxidation rates followed CH4 production rates, and the presence of sulfate hampered both labeled-CH4 oxidation and methanogenesis. Labeled-CH4 oxidation was therefore linked to methanogenesis. This process is referred to as trace CH4 oxidation and has been demonstrated in methanogenic pure cultures. This study shows that the ratio between labeled-CH4 oxidation and methanogenesis is positively affected by the CH4 partial pressure and that this ratio is in methanogenic granular sludge more than 40 times higher than that in pure cultures of methanogens. The CH4 partial pressure also positively affected sulfate reduction and negatively affected methanogenesis: a repression of methanogenesis at elevated CH4 partial pressures confers an advantage to sulfate reducers that compete with methanogens for common substrates, formed from endogenous material. The oxidation of labeled CH 4 and the CH4 dependence of sulfate reduction are thus not necessarily evidence of anaerobic oxidation of CH4 coupled to sulfate reduction. © 2010 Federation of European Microbiological Societies.

  13. Oxidative coupling of methane using inorganic membrane reactor

    Energy Technology Data Exchange (ETDEWEB)

    Ma, Y.H.; Moser, W.R.; Dixon, A.G. [Worcester Polytechnic Institute, MA (United States)] [and others

    1995-12-31

    The goal of this research is to improve the oxidative coupling of methane in a catalytic inorganic membrane reactor. A specific target is to achieve conversion of methane to C{sub 2} hydrocarbons at very high selectivity and relatively higher yields than in fixed bed reactors by controlling the oxygen supply through the membrane. A membrane reactor has the advantage of precisely controlling the rate of delivery of oxygen to the catalyst. This facility permits balancing the rate of oxidation and reduction of the catalyst. In addition, membrane reactors minimize the concentration of gas phase oxygen thus reducing non selective gas phase reactions, which are believed to be a main route for formation of CO{sub x} products. Such gas phase reactions are a cause for decreased selectivity in oxidative coupling of methane in conventional flow reactors. Membrane reactors could also produce higher product yields by providing better distribution of the reactant gases over the catalyst than the conventional plug flow reactors. Modeling work which aimed at predicting the observed experimental trends in porous membrane reactors was also undertaken in this research program.

  14. [The processes of methane formation and oxidation in the soils of the Russian arctic tundra].

    Science.gov (United States)

    Berestovskaia, Iu Iu; Rusanov, I I; Vasil'eva, L V; Pimenov, N V

    2005-01-01

    Methane emission from the following types of tundra soils was studied: coarse humic gleyey loamy cryo soil, peaty gley soil, and peaty gleyey midloamy cryo soil of the arctic tundra. All the soils studied were found to be potential sources of atmospheric methane. The highest values of methane emission were recorded in August at a soil temperature of 8-10 degrees C. Flooded parcels were the sources of atmospheric methane throughout the observation period. The rates of methane production and oxidation in tundra soils of various types at 5 and 15 degrees C were studied by the radioisotope method. Methane oxidation was found to occur in bog water, in the green part of peat moss, and in all the soil horizons studied. Methane formation was recorded in the horizons of peat, in clay with plant roots, and in peaty moss dust of the bogey parcels. At both temperatures, the methane oxidation rate exceeded the rate of methane formation in all the horizons of the mossy-lichen tundra and of the bumpy sinkhole complex. Methanogenesis prevailed only in a sedge-peat moss bog at 15 degrees C. Enrichment bacterial cultures oxidizing methane at 5 and 15 degrees C were obtained. Different types of methanotrophic bacteria were shown to be responsible for methane oxidation under these conditions. A representative of type I methylotrophs oxidized methane at 5 degrees C, and Methylocella tundrae, a psychroactive representative of an acidophilic methanotrophic genus Methylocella, at 15 degrees C.

  15. Energy Metabolism during Anaerobic Methane Oxidation in ANME Archaea

    Science.gov (United States)

    McGlynn, Shawn E.

    2017-01-01

    Anaerobic methane oxidation in archaea is often presented to operate via a pathway of “reverse methanogenesis”. However, if the cumulative reactions of a methanogen are run in reverse there is no apparent way to conserve energy. Recent findings suggest that chemiosmotic coupling enzymes known from their use in methylotrophic and acetoclastic methanogens—in addition to unique terminal reductases—biochemically facilitate energy conservation during complete CH4 oxidation to CO2. The apparent enzyme modularity of these organisms highlights how microbes can arrange their energy metabolisms to accommodate diverse chemical potentials in various ecological niches, even in the extreme case of utilizing “reverse” thermodynamic potentials. PMID:28321009

  16. A mechanistic study on the oxidative coupling of methane over lithium doped magnesium oxide catalysts

    NARCIS (Netherlands)

    Geerts, J.W.M.H.; Kasteren, van J.M.N.; Wiele, van der K.; Imarisio, G.; Frias, M.; Berntgen, J.M.

    1988-01-01

    To elucidate the importance of various reaction steps in the oxidative convers ion of methane, experiments were carried out with three reaction products: ethane, ethylene and carbon monoxide. These products were studied seperately, in oxidation experiments with and without a catalyst. Moreover , the

  17. Methane from landfills in Sweden. Final report; Metan fraan avfallsupplag i Sverige. Slutrapport

    Energy Technology Data Exchange (ETDEWEB)

    Samuelsson, Jerker [Chalmers Univ. of Technology, Goeteborg (Sweden); Galle, Bo; Boerjesson, Gunnar [Linkoeping Univ. (Sweden). Dept. of Water and Environmental Studies

    2006-01-15

    Three years of measurements has been conducted at seven Swedish landfills, quantifying methane emission, methane oxidation and methane production. The measurements reveal a large span between the sites in terms of gas recovery efficiency, 29-78% during normal operation. The fraction of the totally produced methane that is eventually leaking out to the atmosphere, was found to vary between 21-68%. Regarding methane oxidation, the study shows that of the methane going from the landfill interior towards the atmosphere, 6-43% is oxidised to CO{sub 2} in the different landfill cover soils. The highest methane oxidation was found in closed landfills during summertime, and the lowest at active landfills during wintertime, due to the strong temperature dependence of the oxidation. The equipment developed for methane emission measurements is based on time resolved concentration measurements with FTIR spectroscopy in combination with tracer gas releases from the surface of the landfill. The method has proven to be able to state the methane emission from the landfills with high accuracy, {+-}18% of the emission estimate (95% confidence interval). This is in line with what has been achieved in the literature for fugitive emission sources. The system has also proven to be useful for on site leak search. The precision for the methane production measurement was demonstrated to be high, down to {+-}4.2%. This enables trend studies and verification of improvement measures taken at the landfill sites. In terms of absolute accuracy for the production estimate, a 95%-confidence interval of down to (-6.0%, +6.2%) has been achieved. At times of strong methane oxidation the uncertainties increase, particularly if the emission is high. The gas production at the landfill site is therefore preferably measured during autumn-winter-spring when the temperature and the methane oxidation are low. The methane oxidation has been measured by carbon isotope technique, utilising the enrichment in

  18. Kinetics and mechanism of methane oxidation in supercritical water

    International Nuclear Information System (INIS)

    Rofer, C.K.; Streit, G.E.

    1988-10-01

    This project, is a Hazardous Waste Remedial Actions Program (HAZWRAP) Research and Development task being carried out by the Los Alamos National Laboratory. Its objective is to achieve an understanding of the technology for use in scaling up and applying oxidation in supercritical water as a viable process for treating a variety of Department of Energy Defense Programs (DOE-DP) waste streams. This report presents experimental results for the kinetics of the oxidation of methane and methanol in supercritical water and computer modeling results for the oxidation of carbonmonoxide and methane in supercritical water. The experimental and modeling results obtained to date on these one-carbon model compounds indicate that the mechanism of oxidation in supercritical water can be represented by free-radical reactions with appropriate modifications for high pressure and the high water concentration. If these current trends are sustained, a large body of existing literature data on the kinetics of elementary reactions can be utilized to predict the behavior of other compounds and their mixtures. 7 refs., 4 figs., 3 tabs

  19. Thermophilic anaerobic oxidation of methane by marine microbial consortia.

    Science.gov (United States)

    Holler, Thomas; Widdel, Friedrich; Knittel, Katrin; Amann, Rudolf; Kellermann, Matthias Y; Hinrichs, Kai-Uwe; Teske, Andreas; Boetius, Antje; Wegener, Gunter

    2011-12-01

    The anaerobic oxidation of methane (AOM) with sulfate controls the emission of the greenhouse gas methane from the ocean floor. AOM is performed by microbial consortia of archaea (ANME) associated with partners related to sulfate-reducing bacteria. In vitro enrichments of AOM were so far only successful at temperatures ≤25 °C; however, energy gain for growth by AOM with sulfate is in principle also possible at higher temperatures. Sequences of 16S rRNA genes and core lipids characteristic for ANME as well as hints of in situ AOM activity were indeed reported for geothermally heated marine environments, yet no direct evidence for thermophilic growth of marine ANME consortia was obtained to date. To study possible thermophilic AOM, we investigated hydrothermally influenced sediment from the Guaymas Basin. In vitro incubations showed activity of sulfate-dependent methane oxidation between 5 and 70 °C with an apparent optimum between 45 and 60 °C. AOM was absent at temperatures ≥75 °C. Long-term enrichment of AOM was fastest at 50 °C, yielding a 13-fold increase of methane-dependent sulfate reduction within 250 days, equivalent to an apparent doubling time of 68 days. The enrichments were dominated by novel ANME-1 consortia, mostly associated with bacterial partners of the deltaproteobacterial HotSeep-1 cluster, a deeply branching phylogenetic group previously found in a butane-amended 60 °C-enrichment culture of Guaymas sediments. The closest relatives (Desulfurella spp.; Hippea maritima) are moderately thermophilic sulfur reducers. Results indicate that AOM and ANME archaea could be of biogeochemical relevance not only in cold to moderate but also in hot marine habitats.

  20. Conventional methanotrophs are responsible for atmospheric methane oxidation in paddy soils

    NARCIS (Netherlands)

    Cai, Yuanfeng; Yan, Zheng; Bodelier, P.L.E.; Conrad, R.; Jia, Zhongjun

    2016-01-01

    Soils serve as the biological sink of the potent greenhouse gas methane with exceptionally low concentrations of ~1.84 p.p.m.v. in the atmosphere. The as-yet-uncultivated methane-consuming bacteria have long been proposed to be responsible for this ‘high-affinity’ methane oxidation (HAMO). Here we

  1. Intensive Ammonia and Methane Oxidation in Organic Liquid Manure Crusts

    DEFF Research Database (Denmark)

    Nielsen, Daniel Aagren; Nielsen, Lars Peter; Schramm, Andreas

    methane oxidizing bacteria (MOB) and are known to accumulate nitrite and nitrate, indicating the presence of ammonia oxidizers (AOB). We have surveyed six manure tanks with organic covers to investigate the prevalence of MOB and AOB and to link the potential activity with physical and chemical aspects...... characterized with respect to O2 availability by in situ profiling with electrochemical microsensors. Results show that oxygen penetration increased from few micrometers up to several centimetres with crust age. AOB and ammonium oxidation are ubiquitously present in well-developed manure crusts whereas MOB were...... also CH4 emission mitigation, an organic surface crust can be effective if populations of MOB and AOB are allowed to build up....

  2. Nitrous oxide and methane in marine systems

    Energy Technology Data Exchange (ETDEWEB)

    De Wilde, H.P.J.

    1999-07-16

    }{sup +} concentration of the river water entering the estuary. An estimate of the N2O production during nitrification in the water column was derived from the ratio between calculated N2O loss to the atmosphere and measured nitrification activity. The differences between the present estuarine N2O distribution and the situation in 1978, as reported in literature, are discussed in the light of the gradually decreasing anthropogenic loadings of organic carbon and nutrients, and the associated increase in oxygen concentrations in the estuary. Finally, the average N2O emission from the Schelde was extrapolated to obtain an estimate of the global estuarine N2O emission. Chapter 4 describes the CH4 distribution in the Rhine estuary, its lower tributaries, and the adjacent Dutch coastal waters during 4 seasons. A CH4 budget was developed on the basis of: (1) the calculated CH4 fluxes between the tributaries, the estuary, and the coastal zone, and (2) estimated gas exchange with the atmosphere. The budget was used to assess the magnitude of in situ CH4 production in the estuary and the coastal zone, respectively. The possible origins of these in situ sources are discussed. Finally, the CH4 emission from the Rhine estuary was extrapolated to assess the global CH4 emission from estuaries to the atmosphere. Chapter 5 addresses the discrepancy between air-sea CH4 fluxes measured by the micrometeorological gradient technique on the one hand, and values calculated from air-sea concentration differences and transfer velocities on the other hand. Both techniques were applied simultaneously at a research platform in the North Sea, located 9 km off the coast of the Netherlands. In addition, the temporal distribution of CH4 saturation in the surface waters around the platform is discussed in relation to fresh water supply and hydrodynamics. Chapter 6 summarises the main results presented in thesis. In addition, the relative importance of various marine systems as sources of atmospheric N2

  3. Acetate repression of methane oxidation by supplemental Methylocella silvestris in a peat soil microcosm.

    Science.gov (United States)

    Rahman, M Tanvir; Crombie, Andrew; Moussard, Hélène; Chen, Yin; Murrell, J Colin

    2011-06-01

    Methylocella spp. are facultative methanotrophs that grow on methane and multicarbon substrates, such as acetate. Acetate represses transcription of methane monooxygenase of Methylocella silvestris in laboratory culture. DNA stable-isotope probing (DNA-SIP) using (13)C-methane and (12)C-acetate, carried out with Methylocella-spiked peat soil, showed that acetate also repressed methane oxidation by Methylocella in environmental samples.

  4. Acetate Repression of Methane Oxidation by Supplemental Methylocella silvestris in a Peat Soil Microcosm ▿ †

    Science.gov (United States)

    Rahman, M. Tanvir; Crombie, Andrew; Moussard, Hélène; Chen, Yin; Murrell, J. Colin

    2011-01-01

    Methylocella spp. are facultative methanotrophs that grow on methane and multicarbon substrates, such as acetate. Acetate represses transcription of methane monooxygenase of Methylocella silvestris in laboratory culture. DNA stable-isotope probing (DNA-SIP) using 13C-methane and 12C-acetate, carried out with Methylocella-spiked peat soil, showed that acetate also repressed methane oxidation by Methylocella in environmental samples. PMID:21515721

  5. Acetate Repression of Methane Oxidation by Supplemental Methylocella silvestris in a Peat Soil Microcosm ▿ †

    OpenAIRE

    Rahman, M. Tanvir; Crombie, Andrew; Moussard, Hélène; Chen, Yin; Murrell, J. Colin

    2011-01-01

    Methylocella spp. are facultative methanotrophs that grow on methane and multicarbon substrates, such as acetate. Acetate represses transcription of methane monooxygenase of Methylocella silvestris in laboratory culture. DNA stable-isotope probing (DNA-SIP) using 13C-methane and 12C-acetate, carried out with Methylocella-spiked peat soil, showed that acetate also repressed methane oxidation by Methylocella in environmental samples.

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

    Science.gov (United States)

    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

  7. Methane production by anaerobic digestion of algae. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Nyns, E.J.; Naveau, H.P.

    Methane is produced experimentally by anaerobic fermentation of algae, principally of species Hydrodictyon and Cladophora, grown in cooling water from nuclear power plants. The accumulation of fatty acids, by-products of fermentation, is found to have an inhibitory effect on methane production. Methods to remove fatty acids and stabilise the reaction are investigated. An economic analysis is presented using a financial model processor based on data from experimental digesters. The experimental work is described and the results are presented in an Appendix (in French). Seven relevant papers, of which two are in French are also annexed.

  8. Iron-mediated anaerobic oxidation of methane in brackish coastal sediments.

    Science.gov (United States)

    Egger, Matthias; Rasigraf, Olivia; Sapart, Célia J; Jilbert, Tom; Jetten, Mike S M; Röckmann, Thomas; van der Veen, Carina; Bândă, Narcisa; Kartal, Boran; Ettwig, Katharina F; Slomp, Caroline P

    2015-01-06

    Methane is a powerful greenhouse gas and its biological conversion in marine sediments, largely controlled by anaerobic oxidation of methane (AOM), is a crucial part of the global carbon cycle. However, little is known about the role of iron oxides as an oxidant for AOM. Here we provide the first field evidence for iron-dependent AOM in brackish coastal surface sediments and show that methane produced in Bothnian Sea sediments is oxidized in distinct zones of iron- and sulfate-dependent AOM. At our study site, anthropogenic eutrophication over recent decades has led to an upward migration of the sulfate/methane transition zone in the sediment. Abundant iron oxides and high dissolved ferrous iron indicate iron reduction in the methanogenic sediments below the newly established sulfate/methane transition. Laboratory incubation studies of these sediments strongly suggest that the in situ microbial community is capable of linking methane oxidation to iron oxide reduction. Eutrophication of coastal environments may therefore create geochemical conditions favorable for iron-mediated AOM and thus increase the relevance of iron-dependent methane oxidation in the future. Besides its role in mitigating methane emissions, iron-dependent AOM strongly impacts sedimentary iron cycling and related biogeochemical processes through the reduction of large quantities of iron oxides.

  9. Final report for the Iowa Livestock Industry Waste Characterization and Methane Recovery Information Dissemination Project; FINAL

    International Nuclear Information System (INIS)

    Garrison, M.V.; Richard, Thomas L

    2001-01-01

    This report summarizes analytical methods, characterizes Iowa livestock wastes, determines fossil fuel displacement by methane use, assesses the market potential, and offers recommendations for the implementation of methane recovery technologies

  10. Temporal variation of aerobic methane oxidation over a tidal cycle in a wetland of northern Taiwan.

    Science.gov (United States)

    Lee, T. Y.; Wang, P. L.; Lin, L. H.

    2017-12-01

    Aerobic methanotrophy plays an important role in controlling methane emitted from wetlands. However, the activity of aerobic methanotrophy regulated by temporal fluctuation of oxygen and methane supply in tidal wetlands is not well known. This study aims to examine the dynamics of methane fluxes and potential aerobic methane consumption rates in a tidal wetland of northern Taiwan, where the variation of environmental characteristics, such as sulfate and methane concentration in pore water has been demonstrated during a tidal cycle. Two field campaigns were carried out in December of 2016 and March of 2017. Fluxes of methane emission, methane concentrations in surface sediments and oxygen profiles were measured at different tidal phases. Besides, batch incubations were conducted on surface sediments in order to quantify potential microbial methane consumption rates and to derive the kinetic parameters for aerobic methanotrophy. Our results demonstrated temporal changes of the surface methane concentration and the methane emission flux during a tidal cycle, while the oxygen flux into the sediment was kept at a similar magnitude. The methane flux was low when the surface was exposed for both shortest and longest periods of time. The potential aerobic methane oxidation rate was high for sample collected from the surface sediments exposed the longest. No correlation could be found between the potential aerobic methane oxidation rate and either the oxygen downward flux or methane emission flux. The decoupled relationships between these observed rates and fluxes suggest that, rather than aerobic methanotrophy, heterotrophic respirations exert a profound control on oxygen flux, and the methane emission is not only been affected by methane consumption but also methane production at depths. The maximum potential rate and the half saturation concentration determined from the batch incubations were high for the surface sediments collected in low tide, suggesting that aerobic

  11. Methane combustion over lanthanum-based perovskite mixed oxides

    Energy Technology Data Exchange (ETDEWEB)

    Arandiyan, Hamidreza [New South Wales Univ., Sydney (Australia). School of Chemical Engineering

    2015-11-01

    This book presents current research into the catalytic combustion of methane using perovskite-type oxides (ABO{sub 3}). Catalytic combustion has been developed as a method of promoting efficient combustion with minimum pollutant formation as compared to conventional catalytic combustion. Recent theoretical and experimental studies have recommended that noble metals supported on (ABO{sub 3}) with well-ordered porous networks show promising redox properties. Three-dimensionally ordered macroporous (3DOM) materials with interpenetrated and regular mesoporous systems have recently triggered enormous research activity due to their high surface areas, large pore volumes, uniform pore sizes, low cost, environmental benignity, and good chemical stability. These are all highly relevant in terms of the utilization of natural gas in light of recent catalytic innovations and technological advances. The book is of interest to all researchers active in utilization of natural gas with novel catalysts. The research covered comes from the most important industries and research centers in the field. The book serves not only as a text for researcher into catalytic combustion of methane, 3DOM perovskite mixed oxide, but also explores the field of green technologies by experts in academia and industry. This book will appeal to those interested in research on the environmental impact of combustion, materials and catalysis.

  12. Formation and retention of methane in coal. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Hucka, V.J.; Bodily, D.M.; Huang, H.

    1992-05-15

    The formation and retention of methane in coalbeds was studied for ten Utah coal samples, one Colorado coal sample and eight coal samples from the Argonne Premium Coal Sample Bank.Methane gas content of the Utah and Colorado coals varied from zero to 9 cm{sup 3}/g. The Utah coals were all high volatile bituminous coals. The Colorado coal was a gassy medium volatile bituminous coal. The Argonne coals cover a range or rank from lignite to low volatile bituminous coal and were used to determine the effect of rank in laboratory studies. The methane content of six selected Utah coal seams and the Colorado coal seam was measured in situ using a special sample collection device and a bubble desorbometer. Coal samples were collected at each measurement site for laboratory analysis. The cleat and joint system was evaluated for the coal and surrounding rocks and geological conditions were noted. Permeability measurements were performed on selected samples and all samples were analyzed for proximate and ultimate analysis, petrographic analysis, {sup 13}C NMR dipolar-dephasing spectroscopy, and density analysis. The observed methane adsorption behavior was correlated with the chemical structure and physical properties of the coals.

  13. Seasonal Oxygen Dynamics in a Thermokarst Bog in Interior Alaska: Implications for Rates of Methane Oxidation

    Science.gov (United States)

    Neumann, R. B.; Moorberg, C.; Wong, A.; Waldrop, M. P.; Turetsky, M. R.

    2015-12-01

    Methane is a potent greenhouse gas, and wetlands represent the largest natural source of methane to the atmosphere. However, much of the methane generated in anoxic wetlands never gets emitted to the atmosphere; up to >90% of generated methane can get oxidized to carbon dioxide. Thus, oxidation is an important methane sink and changes in the rate of methane oxidation can affect wetland methane emissions. Most methane is aerobically oxidized at oxic-anoxic interfaces where rates of oxidation strongly depend on methane and oxygen concentrations. In wetlands, oxygen is often the limiting substrate. To improve understanding of belowground oxygen dynamics and its impact on methane oxidation, we deployed two planar optical oxygen sensors in a thermokarst bog in interior Alaska. Previous work at this site indicated that, similar to other sites, rates of methane oxidation decrease over the growing season. We used the sensors to track spatial and temporal patterns of oxygen concentrations over the growing season. We coupled these in-situ oxygen measurements with periodic oxygen injection experiments performed against the sensor to quantify belowground rates of oxygen consumption. We found that over the season, the thickness of the oxygenated water layer at the peatland surface decreased. Previous research has indicated that in sphagnum-dominated peatlands, like the one studied here, rates of methane oxidation are highest at or slightly below the water table. It is in these saturated but oxygenated locations that both methane and oxygen are available. Thus, a seasonal reduction in the thickness of the oxygenated water layer could restrict methane oxidation. The decrease in thickness of the oxygenated layer coincided with an increase in the rate of oxygen consumption during our oxygen injection experiments. The increase in oxygen consumption was not explained by temperature; we infer it was due to an increase in substrate availability for oxygen consuming reactions and

  14. Lithium chemistry of lithium doped magnesium oxide catalysts used in the oxidative coupling of methane

    NARCIS (Netherlands)

    Korf, S.J.; Roos, J.A.; de Bruijn, N.A.; van Ommen, J.G.; Ross, J.R.H.

    1990-01-01

    Active sites are created on the surface of a Li/MgO catalyst used for the selective oxidation of methane by the gradual loss of carbon dioxide from surface carbonate species in the presence of oxygen. Decomposition of the carbonate species in the absence of oxygen is detrimental to the activity of

  15. Selective oxidation of methane to ethane and ethylene over various oxide catalysts

    NARCIS (Netherlands)

    Roos, J.A.; Bakker, A.G.; Bosch, H.; van Ommen, J.G.; Ross, J.R.H.

    1987-01-01

    Preliminary results are reported for the oxidative coupling of methane to give ethane/ethylene mixtures over a series of different catalyst formulations; the temperature range studied is 650–850°C. A comparison is made of the behaviour of lead/alumina and lithium/magnesia materials. It is found that

  16. Iron oxide reduction in methane-rich deep Baltic Sea sediments

    DEFF Research Database (Denmark)

    Egger, Matthias; Hagens, Mathilde; Sapart, Celia J.

    2017-01-01

    /L transition. Our results reveal a complex interplay between production, oxidation and transport of methane showing that besides organoclastic Fe reduction, oxidation of downward migrating methane with Fe oxides may also explain the elevated concentrations of dissolved ferrous Fe in deep Baltic Sea sediments...... profiles and numerical modeling, we propose that a potential coupling between Fe oxide reduction and methane oxidation likely affects deep Fe cycling and related biogeochemical processes, such as burial of phosphorus, in systems subject to changes in organic matter loading or bottom water salinity....

  17. The oxidative coupling of methane and the oxidative dehydrogenation of ethane over a niobium promoted lithium doped magnesium oxide catalyst

    NARCIS (Netherlands)

    Swaan, H.M.; Swaan, H.M.; Li, X.; Seshan, Kulathuiyer; van Ommen, J.G.; Ross, J.R.H.; Ross, J.R.H.

    1993-01-01

    The promoting effect of niobium in a Li/MgO catalyst for the oxidative coupling of methane (OCM) and for the oxidative dehydrogenation of ethane (ODHE) has been studied in some detail. It has been found that a Li/Nb/MgO catalyst with 16 wt % niobium showed the highest activity for the C2 production

  18. Emissions of nitrous oxide and methane from surface and ground waters in Germany

    International Nuclear Information System (INIS)

    Hiessl, H.

    1993-01-01

    The paper provides a first estimation of the contribution of inland freshwater systems (surface waters and ground waters) to the emission of the greenhouse gases nitrous oxide and methane in Germany. These amounts are compared to other main sources for the emission of nitrous oxide and methane. (orig.) [de

  19. Manual on measurement of methane and nitrous oxide emissions from agriculture

    International Nuclear Information System (INIS)

    1992-11-01

    Nitrous oxide and methane are two of the gases primarily responsible for atmospheric warming, or the ''greenhouse effect''. Agricultural activities are an important source of methane and nitrous oxide emissions, but quantitation of these sources is generally lacking. This manual describes techniques to evaluate current emissions from diverse animal and crop production practices and suggests methods for decreasing these emissions. Refs, figs and tabs

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

    Science.gov (United States)

    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.

  1. Potassium/calcium/nickel oxide catalysts for the oxidative coupling of methane

    NARCIS (Netherlands)

    Dooley, K.; Dooley, Kerry M.; Ross, J.R.H.; Ross, Julian R.H.

    1992-01-01

    A series of potassium/calcium/nickel oxides were tested for the oxidative coupling of methane (OCM) at 843–943 K and water addition to the feed at 0–66 mol-%. The K/Ni ratios varied from 0.0–0.6 and Ca/Ni from 0.0–11; catalysts with no nickel were also tested. At least 10% water in the feed and

  2. Effect of additives on lithium doped magnesium oxide catalysts used in the oxidative coupling of methane

    NARCIS (Netherlands)

    Korf, S.J.; Roos, J.A.; Veltman, L.J.; van Ommen, J.G.; Ross, J.R.H.

    1989-01-01

    It has been found that it is possible to improve the activity and stability for the oxidative coupling of methane of a Li/MgO catalyst by the addition of small amounts of the oxides of various transition and rare earth metals. A number of these additives, e.g. SnO2, TiO2, Dy2O3 and Tb4O7, caused

  3. Assessment of the methane oxidation capacity of compacted soils intended for use as landfill cover materials

    International Nuclear Information System (INIS)

    Rachor, Ingke; Gebert, Julia; Groengroeft, Alexander; Pfeiffer, Eva-Maria

    2011-01-01

    The microbial oxidation of methane in engineered cover soils is considered a potent option for the mitigation of emissions from old landfills or sites containing wastes of low methane generation rates. A laboratory column study was conducted in order to derive design criteria that enable construction of an effective methane oxidising cover from the range of soils that are available to the landfill operator. Therefore, the methane oxidation capacity of different soils was assessed under simulated landfill conditions. Five sandy potential landfill top cover materials with varying contents of silt and clay were investigated with respect to methane oxidation and corresponding soil gas composition over a period of four months. The soils were compacted to 95% of their specific proctor density, resulting in bulk densities of 1.4-1.7 g cm -3 , reflecting considerably unfavourable conditions for methane oxidation due to reduced air-filled porosity. The soil water content was adjusted to field capacity, resulting in water contents ranging from 16.2 to 48.5 vol.%. The investigated inlet fluxes ranged from 25 to about 100 g CH 4 m -2 d -1 , covering the methane load proposed to allow for complete oxidation in landfill covers under Western European climate conditions and hence being suggested as a criterion for release from aftercare. The vertical distribution of gas concentrations, methane flux balances as well as stable carbon isotope studies allowed for clear process identifications. Higher inlet fluxes led to a reduction of the aerated zone, an increase in the absolute methane oxidation rate and a decline of the relative proportion of oxidized methane. For each material, a specific maximum oxidation rate was determined, which varied between 20 and 95 g CH 4 m -2 d -1 and which was positively correlated to the air-filled porosity of the soil. Methane oxidation efficiencies and gas profile data imply a strong link between oxidation capacity and diffusive ingress of

  4. Modeling of termokinetic oscillations at partial oxidation of methane

    Science.gov (United States)

    Arutyunov, A. V.; Belyaev, A. A.; Inovenkov, I. N.; Nefedov, V. V.

    2017-12-01

    Partial oxidation of natural gas at moderate temperatures below 1500 K has significant interest for a number of industrial applications. But such processes can proceed at different unstable regimes including oscillating modes. Nonlinear phenomena at partial oxidation of methane were observed at different conditions. The investigation of the complex nonlinear system of equations that describes this process is a real method to insure its stability at industrial conditions and, at the same time, is an effective tool for its further enhancement. Numerical analysis of methane oxidation kinetics in the continuous stirred-tank reactor, with the use of detailed kinetic model has shown the possibility of the appearance of oscillating modes in the appropriate range of reaction parameters that characterize the composition, pressure, reagents flow, thermophysical features of the system, and geometry of the reactor. The appearance of oscillating modes is connected both with the reaction kinetics, heat release and sink and reagents introduction and removing. At that, oscillations appear only at a limited range of parameters, but can be accompanied by significant change in the yield of products. We have determined the range of initial temperature and pressure at which oscillations can be observed, if all other parameters remained fixed. The boundaries of existence of oscillations on the phase plane were calculated. It was shown that depending on the position inside the oscillation region the oscillations have different frequency and amplitude. It was reviled the role of heat exchange with the environment: at the absence of heat exchange the oscillating modes are impossible. In the vicinity of the boundary of phase range, where oscillations exist, significant change of concentration of some products were observed, for example, that of CO2, which in this case one of the principal products is. At that, insignificant increase in pressure not only change the character of CO2 behaving

  5. Methane and fertilizer production from seaweed biomass. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Betzer, P.R.; Humm, H.J.

    1984-01-01

    It was demonstrated that several varieties of abundant benthic algae indigenous to Tampa Bay (Gracilaria, Hypnea, and Ulva) were readily degradable via anaerobic digestion to methane. The energy yield per unit weight biomass degraded was higher than any previously reported. Given the large masses of readily degradable plants which are annually produced in and around Tampa Bay, the resource is estimated to be at least equivalent to several million gallons of gasoline.

  6. In situ measurement of methane oxidation in groundwater by using natural-gradient tracer tests

    International Nuclear Information System (INIS)

    Smith, R.L.; Howes, B.L.; Garabedian, S.P.

    1991-01-01

    Methane oxidation was measured in an unconfined sand and gravel aquifer (Cape Cod, Mass.) by using in situ natural-gradient tracer tests at both a pristine, oxygenated site and an anoxic, sewage-contaminated site. The tracer sites were equipped with multilevel sampling devices to create target grids of sampling points; the injectate was prepared with groundwater from the tracer site to maintain the same geochemical conditions. Methane oxidation was calculated from breakthrough curves of methane relative to halide and inert gas (hexafluoroethane) tracers and was confirmed by the appearance of 13 C-enriched carbon dioxide in experiments in which 13 C-enriched methane was used as the tracer. A V max for methane oxidation could be calculated when the methane concentration was sufficiently high to result in zero-order kinetics throughout the entire transport interval. Methane breakthrough curves could be simulated by modifying a one-dimensional advection-dispersion transport model to include a Michaelis-Menten-based consumption term for methane oxidation. The K m values for methane oxidation that gave the best match for the breakthrough curve peaks were 6.0 and 9.0 μM for the uncontaminated and contaminated sites, respectively. Natural-gradient tracer tests are a promising approach for assessing microbial processes and for testing in situ bioremediation potential in groundwater systems

  7. Quantification of the methane concentration using anaerobic oxidation of methane coupled to extracellular electron transfer

    Science.gov (United States)

    A biofilm anode acclimated with acetate, acetate+methane, and methane growth media for over three years produced a steady current density of 1.6-2.3 mA/m^2 in a microbial electrochemical cell (MxC) fed with methane as the sole electron donor. Geobacter was the dominant genus for...

  8. Kinetic study on anaerobic oxidation of methane coupled to denitrification.

    Science.gov (United States)

    Yu, Hou; Kashima, Hiroyuki; Regan, John M; Hussain, Abid; Elbeshbishy, Elsayed; Lee, Hyung-Sool

    2017-09-01

    Monod kinetic parameters provide information required for kinetic analysis of anaerobic oxidation of methane coupled to denitrification (AOM-D). This information is critical for engineering AOM-D processes in wastewater treatment facilities. We first experimentally determined Monod kinetic parameters for an AOM-D enriched culture and obtained the following values: maximum specific growth rate (μ max ) 0.121/d, maximum substrate-utilization rate (q max ) 28.8mmol CH 4 /g cells-d, half maximum-rate substrate concentration (K s ) 83μΜ CH 4 , growth yield (Y) 4.76gcells/mol CH 4 , decay coefficient (b) 0.031/d, and threshold substrate concentration (S min ) 28.8μM CH 4 . Clone library analysis of 16S rRNA and mcrA gene fragments suggested that AOM-D reactions might have occurred via the syntrophic interaction between denitrifying bacteria (e.g., Ignavibacterium, Acidovorax, and Pseudomonas spp.) and hydrogenotrophic methanogens (Methanobacterium spp.), supporting reverse methanogenesis-dependent AOM-D in our culture. High μ max and q max , and low K s for the AOM-D enrichment imply that AOM-D could play a significant role in mitigating atmospheric methane efflux. In addition, these high kinetic features suggest that engineered AOM-D systems may provide a sustainable alternative to nitrogen removal in wastewater treatment. Copyright © 2017 Elsevier Inc. All rights reserved.

  9. Fluxes of methane and nitrous oxide from an Indian mangrove

    Energy Technology Data Exchange (ETDEWEB)

    Krithika, K.; Purvaja, R.; Ramesh, R. [Anna Univ., Chennai (India). Institute for Ocean Management

    2008-01-25

    Methane and nitrous oxide are atmospheric trace gases and contribute about 15 and 6% respectively to the greenhouse effect. Both have a long atmospheric residence time of about 114 and 12 years respectively and since they are key compounds in the chemical reaction cycles of the troposphere and the stratosphere, their potential to directly or indirectly influence global climate is high. Fluxes of greenhouse gases, methane (CH{sub 4}) and nitrous oxide (N{sub 2}O), were measured from a mangrove ecosystem of the Cauvery delta (Muthupet) in South India. CH{sub 4} emissions were in the range between 18.99 and 37.53 mg/sq. m/d, with an average of 25.21 mg/sq. m/d, whereas N{sub 2}O emission ranged between 0.41 and 0.80 mg/sq. m/d (average of 0.62 mg/sq. m/d). The emission of CH{sub 4} and N{sub 2}O correlated positively with the number of pneumatophores. In addition to the flux measurements, different parts of the roots of Avicennia marina were quantified for CH{sub 4} concentration. Invariably in all the seasons, measured CH{sub 4} concentrations were high in the cable roots, with gradual decrease through the pneumatophores below water level and the above water level. This clearly indicates the transport of CH{sub 4} through the roots. We were able to establish that CH{sub 4} was released passively through the mangrove pneumatophores and is also a source to the atmosphere. We present some additional information on transport mechanisms of CH{sub 4} through the pneumatophores and bubble release from the mangrove ecosystems.

  10. Urban sources and emissions of nitrous oxide and methane in southern California, USA

    Science.gov (United States)

    Townsend-Small, A.; Pataki, D.; Tyler, S. C.; Czimczik, C. I.; Xu, X.; Christensen, L. E.

    2012-12-01

    Anthropogenic activities have resulted in increasing levels of greenhouse gases, including carbon dioxide, methane, and nitrous oxide. While global and regional emissions sources of carbon dioxide are relatively well understood, methane and nitrous oxide are less constrained, particularly at regional scales. Here we present the results of an investigation of sources and emissions of methane and nitrous oxide in Los Angeles, California, USA, one of Earth's largest urban areas. The original goal of the project was to determine whether isotopes are useful tracers of agricultural versus urban nitrous oxide and methane sources. For methane, we found that stable isotopes (carbon-13 and deuterium) and radiocarbon are good tracers of biogenic versus fossil fuel sources. High altitude observations of methane concentration, measured continuously using tunable laser spectroscopy, and isotope ratios, measured on discrete flask samples using mass spectrometry, indicate that the predominant methane source in Los Angeles is from fossil fuels, likely from "fugitive" emissions from geologic formations, natural gas pipelines, oil refining, or power plants. We also measured nitrous oxide emissions and isotope ratios from urban (landscaping and wastewater treatment) and agricultural sources (corn and vegetable fields). There was no difference in nitrous oxide isotope ratios between the different types of sources, although stable isotopes did differ between nitrous oxide produced in oxic and anoxic wastewater treatment tanks. Our nitrous oxide flux data indicate that landscaped turfgrass emits nitrous oxide at rates equivalent to agricultural systems, indicating that ornamental soils should not be disregarded in regional nitrous oxide budgets. However, we also showed that wastewater treatment is a much greater source of nitrous oxide than soils regionally. This work shows that global nitrous oxide and methane budgets are not easily downscaled to regional, urban settings, which has

  11. High resolution and comprehensive techniques to analyze aerobic methane oxidation in mesocosm experiments

    Science.gov (United States)

    Chan, E. W.; Kessler, J. D.; Redmond, M. C.; Shiller, A. M.; Arrington, E. C.; Valentine, D. L.; Colombo, F.

    2015-12-01

    Many studies of microbially mediated aerobic methane oxidation in oceanic environments have examined the many different factors that control the rates of oxidation. However, there is debate on how quickly methane is oxidized once a microbial population is established and what factor(s) are limiting in these types of environments. These factors include the availability of CH4, O2, trace metals, nutrients, and the density of cell population. Limits to these factors can also control the temporal aspects of a methane oxidation event. In order to look at this process in its entirety and with higher temporal resolution, a mesocosm incubation system was developed with a Dissolved Gas Analyzer System (DGAS) coupled with a set of analytical tools to monitor aerobic methane oxidation in real time. With the addition of newer laser spectroscopy techniques (cavity ringdown spectroscopy), stable isotope fractionation caused by microbial processes can also be examined on a real time and automated basis. Cell counting, trace metal, nutrient, and DNA community analyses have also been carried out in conjunction with these mesocosm samples to provide a clear understanding of the biology in methane oxidation dynamics. This poster will detail the techniques involved to provide insights into the chemical and isotopic kinetics controlling aerobic methane oxidation. Proof of concept applications will be presented from seep sites in the Hudson Canyon and the Sleeping Dragon seep field, Mississippi Canyon 118 (MC 118). This system was used to conduct mesocosm experiments to examine methane consumption, O2 consumption, nutrient consumption, and biomass production.

  12. Remarkable recovery and colonization behaviour of methane oxidizing bacteria in soil after disturbance is controlled by methane source only

    NARCIS (Netherlands)

    Pan, Y.; Abell, G.C.J.; Bodelier, P.L.E.; Meima-Franke, M.; Sessitsch, A.; Bodrossy, L.

    2014-01-01

    Little is understood about the relationship between microbial assemblage history, the composition and function of specific functional guilds and the ecosystem functions they provide. To learn more about this relationship we used methane oxidizing bacteria (MOB) as model organisms and performed soil

  13. Methane and nitrous oxide: Methods in national emissions inventories and options for control

    Energy Technology Data Exchange (ETDEWEB)

    Van Amstel, A.R. (ed.)

    1993-07-01

    The UN Framework Convention on Climate Change signed in Rio de Janeiro, Brazil, calls for the return of anthropogenic emissions of greenhouse gases to their 1990 levels by the year 2000 in industrialized countries. It also calls for a monitoring of the emissions of greenhouse gases. It is important that reliable and scientifically credible national inventories are available for the international negotiations. Therefore a consistent methodology and a transparent reporting format is needed. The title workshop had two main objectives: (1) to support the development a methodology and format for national emissions inventories of greenhouse gases by mid 1993, as coordinated by the Science Working Group of the IPCC and the OECD; and (2) the development of technical options for reduction of greenhouse gases and the assessment of the socio-economic feasibility of these options. The workshop consisted of key note overview presentations, and two rounds of working group sessions, each covering five parallel sessions on selected sources. In the first round of each working group session the literature, existing methods for methane and nitrous oxide inventories, and the OECD/IPCC guidelines have been addressed. Then, in the second round, options for emission reductions have been discussed, as well as their socio-economic implications. The methane sources discussed concern oil and gas, coal mining, ruminants, animal waste, landfills and sewage treatment, combustion and industry, rice production and wetlands, biomass burning. The nitrous oxide sources discussed are agricultural soils and combustion and industry. The proceedings on methane comprise 16 introductory papers and 7 papers on the results of the working groups, while in part two four introductory papers and two papers on the results of working groups on nitrous oxide are presented. In part three future emission reduction policy options are discussed. Finally, 16 poster contributions are included

  14. Methyl Radicals in Oxidative Coupling of Methane Directly Confirmed by Synchrotron VUV Photoionization Mass Spectroscopy

    Science.gov (United States)

    Luo, Liangfeng; Tang, Xiaofeng; Wang, Wendong; Wang, Yu; Sun, Shaobo; Qi, Fei; Huang, Weixin

    2013-01-01

    Gas-phase methyl radicals have been long proposed as the key intermediate in catalytic oxidative coupling of methane, but the direct experimental evidence still lacks. Here, employing synchrotron VUV photoionization mass spectroscopy, we have directly observed the formation of gas-phase methyl radicals during oxidative coupling of methane catalyzed by Li/MgO catalysts. The concentration of gas-phase methyl radicals correlates well with the yield of ethylene and ethane products. These results lead to an enhanced fundamental understanding of oxidative coupling of methane that will facilitate the exploration of new catalysts with improved performance. PMID:23567985

  15. Are termite mounds biofilters for methane? - Challenges and new approaches to quantify methane oxidation in termite mounds

    Science.gov (United States)

    Nauer, Philipp A.; Hutley, Lindsay B.; Bristow, Mila; Arndt, Stefan K.

    2015-04-01

    Methane emissions from termites contribute around 3% to global methane in the atmosphere, although the total source estimate for termites is the most uncertain among all sources. In tropical regions, the relative source contribution of termites can be far higher due to the high biomass and relative importance of termites in plant decomposition. Past research focused on net emission measurements and their variability, but little is known about underlying processes governing these emissions. In particular, microbial oxidation of methane (MOX) within termite mounds has rarely been investigated. In well-studied ecosystems featuring an oxic matrix above an anoxic methane-producing habitat (e.g. landfills or sediments), the fraction of oxidized methane (fox) can reach up to 90% of gross production. However, conventional mass-balance approaches to apportion production and consumption processes can be challenging to apply in the complex-structured and almost inaccessible environment of a termite mound. In effect, all field-based data on termite-mound MOX is based on one study that measured isotopic shifts in produced and emitted methane. In this study a closed-system isotope fractionation model was applied and estimated fox ranged from 10% to almost 100%. However, it is shown here that by applying an open-system isotope-pool model, the measured isotopic shifts can also be explained by physical transport of methane alone. Different field-based methods to quantify MOX in termite mounds are proposed which do not rely on assumptions of physical gas transport. A simple approach is the use of specific inhibitors for MOX, e.g. difluoromethane (CH2F2), combined with chamber-based flux measurements before and after their application. Data is presented on the suitability of different inhibitors and first results of their application in the field. Alternatively, gas-tracer methods allow the quantification of methane oxidation and reaction kinetics without knowledge of physical gas

  16. Methane distribution and oxidation around the Lena Delta in summer 2013

    Science.gov (United States)

    Bussmann, Ingeborg; Hackbusch, Steffen; Schaal, Patrick; Wichels, Antje

    2017-11-01

    The Lena River is one of the largest Russian rivers draining into the Laptev Sea. The predicted increases in global temperatures are expected to cause the permafrost areas surrounding the Lena Delta to melt at increasing rates. This melting will result in high amounts of methane reaching the waters of the Lena and the adjacent Laptev Sea. The only biological sink that can lower methane concentrations within this system is methane oxidation by methanotrophic bacteria. However, the polar estuary of the Lena River, due to its strong fluctuations in salinity and temperature, is a challenging environment for bacteria. We determined the activity and abundance of aerobic methanotrophic bacteria by a tracer method and by the quantitative polymerase chain reaction. We described the methanotrophic population with a molecular fingerprinting method (monooxygenase intergenic spacer analysis), as well as the methane distribution (via a headspace method) and other abiotic parameters, in the Lena Delta in September 2013. The median methane concentrations were 22 nmol L-1 for riverine water (salinity (S) 20). The Lena River was not the source of methane in surface water, and the methane concentrations of the bottom water were mainly influenced by the methane concentration in surface sediments. However, the bacterial populations of the riverine and polar waters showed similar methane oxidation rates (0.419 and 0.400 nmol L-1 d-1), despite a higher relative abundance of methanotrophs and a higher estimated diversity in the riverine water than in the polar water. The methane turnover times ranged from 167 days in mixed water and 91 days in riverine water to only 36 days in polar water. The environmental parameters influencing the methane oxidation rate and the methanotrophic population also differed between the water masses. We postulate the presence of a riverine methanotrophic population that is limited by sub-optimal temperatures and substrate concentrations and a polar

  17. Extreme nitrogen deposition can change methane oxidation rate in moist acidic tundra soil in Arctic regions

    Science.gov (United States)

    Lee, J.; Kim, J.; Kang, H.

    2017-12-01

    Recently, extreme nitrogen(N) deposition events are observed in Arctic regions where over 90% of the annual N deposition occurred in just a few days. Since Arctic ecosystems are typically N-limited, input of extremely high amount of N could substantially affect ecosystem processes. CH4 is a potent greenhouse gas that has 25 times greater global warming potential than CO2 over a 100-year time frame. Ammonium is known as an inhibitor of methane oxidation and nitrate also shows inhibitory effect on it in temperate ecosystems. However, effects of N addition on Arctic ecosystems are still elusive. We conducted a lab-scale incubation experiment with moist acidic tundra (MAT) soil from Council, Alaska to investigate the effect of extreme N deposition events on methane oxidation. Zero point five % methane was added to the head space to determine the potential methane oxidation rate of MAT soil. Three treatments (NH4NO3-AN, (NH4)2SO4-AS, KNO3-PN) were used to compare effects of ammonium, nitrate and salts. All treatments were added in 3 levels: 10μg N gd.w-1(10), 50μg N gd.w-1(50) and 100μg N gd.w-1(100). AN10 and AN50 increased methane oxidation rate 1.7, 6% respectively. However, AN100 shows -8.5% of inhibitory effect. In AS added samples, all 3 concentrations (AN10, AN50, AN100) stimulated methane oxidation rate with 4.7, 8.9, 4%, respectively. On the contrary, PN50 (-9%) and PN100 (-59.5%) exhibited a significant inhibitory effect. We also analyzed the microbial gene abundance and community structures of methane oxidizing bacteria using a DNA-based fingerprinting method (T-RFLP) Our study results suggest that NH4+ can stimulate methane oxidation in Arctic MAT soil, while NO3- can inhibit methane oxidation significantly.

  18. Cordierite-supported metal oxide for non-methane hydrocarbon oxidation in cooking oil fumes.

    Science.gov (United States)

    Huang, Yonghai; Yi, Honghong; Tang, Xiaolong; Zhao, Shunzheng; Gao, Fengyu; Wang, Jiangen; Yang, Zhongyu

    2018-05-21

    Cooking emission is an important reason for the air quality deterioration in the metropolitan area in China. Transition metal oxide and different loading of manganese oxide supported on cordierite were prepared by incipient wetness impregnation method and were used for non-methane hydrocarbon (NMHC) oxidation in cooking oil fumes (COFs). The effects of different calcination temperature and different Mn content were also studied. The SEM photographs and CO 2 temperature-programmed desorption revealed 5 wt% Mn/cordierite had the best pore structure and the largest number of the weak and moderate basic sites so it showed the best performance for NMHC oxidation. XRD analysis exhibited 5 wt% Mn/cordierite had the best dispersion of active phase and the active phase was MnO 2 when the calcination temperature was 400℃ which were good for the catalytic oxidation of NMHC.

  19. In Situ Bioremediation of 1,4-Dioxane by Methane Oxidizing Bacteria in Coupled Anaerobic-Aerobic Zones

    Science.gov (United States)

    2016-02-11

    FINAL REPORT In Situ Bioremediation of 1,4-Dioxane by Methane Oxidizing Bacteria in Coupled Anaerobic-Aerobic Zones SERDP Project ER-2306...volatile organic compound (CVOCs), ethene and ethane in groundwater at Raritan Arsenal Area 18C after in situ bioremediation . 4 List of...aquifers, the bioremediation approach most commonly used for chlorinated solvents. The ability of methanotrophs to biodegrade 1,4-dioxane was

  20. Methane oxidation in pig and cattle slurry storages, and effects of surface crust moisture and methane availability

    DEFF Research Database (Denmark)

    Petersen, S.O.; Ambus, P.

    2006-01-01

    Storages with liquid manure (slurry) may develop a surface crust of particulate organic matter, or an artificial crust can be established. Slurry storages are net sources of atmospheric methane (CH4), but a potential for bacterial oxidation of CH4 in surface crusts was recently suggested in a study......2 during incubation, while intact subsamples were used to characterize CH4 oxidation as a function of CH4 availability and moisture content. Methane oxidation was observed in all materials except for an expanded clay product (Leca) sampled from a pig slurry storage. Despite significant variation...... crusts indicates that there is a potential for stimulating the process by manipulation of gas phase composition above the stored slurry....

  1. Methane-induced Activation Mechanism of Fused Ferric Oxide-Alumina Catalysts during Methane Decomposition

    KAUST Repository

    Reddy Enakonda, Linga; Zhou, Lu; Saih, Youssef; Ould-Chikh, Samy; Lopatin, Sergei; Gary, Daniel; Del-Gallo, Pascal; Basset, Jean-Marie

    2016-01-01

    Activation of Fe2O3-Al2O3 with CH4 (instead of H2) is a meaningful method to achieve catalytic methane decomposition (CMD). This reaction of CMD is more economic and simple against commercial methane steam reforming (MSR) as it produces COx-free H2

  2. Modelling of stable isotope fractionation by methane oxidation and diffusion in landfill cover soils

    International Nuclear Information System (INIS)

    Mahieu, Koenraad; De Visscher, Alex; Vanrolleghem, Peter A.; Van Cleemput, Oswald

    2008-01-01

    A technique to measure biological methane oxidation in landfill cover soils that is gaining increased interest is the measurement of stable isotope fractionation in the methane. Usually to quantify methane oxidation, only fractionation by oxidation is taken into account. Recently it was shown that neglecting the isotope fractionation by diffusion results in underestimation of the methane oxidation. In this study a simulation model was developed that describes gas transport and methane oxidation in landfill cover soils. The model distinguishes between 12 CH 4 , 13 CH 4 , and 12 CH 3 D explicitly, and includes isotope fractionation by diffusion and oxidation. To evaluate the model, the simulations were compared with column experiments from previous studies. The predicted concentration profiles and isotopic profiles match the measured ones very well, with a root mean square deviation (RMSD) of 1.7 vol% in the concentration and a RMSD of 0.8 per mille in the δ 13 C value, with δ 13 C the relative 13 C abundance as compared to an international standard. Overall, the comparison shows that a model-based isotope approach for the determination of methane oxidation efficiencies is feasible and superior to existing isotope methods

  3. Partial oxidation of methane in a temperature-controlled dielectric barrier discharge reactor

    KAUST Repository

    Zhang, Xuming; Cha, Min

    2015-01-01

    We studied the relative importance of the reduced field intensity and the background reaction temperature in the partial oxidation of methane in a temperature-controlled dielectric barrier discharge reactor. We obtained important mechanistic insight

  4. Rare Branched Fatty Acids Characterize the Lipid Composition of the Intra-Aerobic Methane Oxidizer "

    NARCIS (Netherlands)

    Kool, D.M.; Zhu, B.L.; Rijpstra, W.I.C.; Jetten, M.S.M.; Ettwig, K.F.; Sinninghe Damsté, J.S.

    2012-01-01

    The recently described bacterium "Candidatus Methylomirabilis oxyfera" couples the oxidation of the important greenhouse gas methane to the reduction of nitrite. The ecological significance of "Ca. Methylomirabilis oxyfera" is still underexplored, as our ability to identify the presence of this

  5. Ultrastructure and viral metagenome of bacteriophages from an anaerobic methane oxidizing methylomirabilis bioreactor enrichment culture

    NARCIS (Netherlands)

    Gambelli, Lavinia; Cremers, Geert; Mesman, Rob; Guerrero, Simon; Dutilh, Bas E.; Jetten, Mike S M; den Camp, Huub J M Op; van Niftrik, Laura

    2016-01-01

    With its capacity for anaerobic methane oxidation and denitrification, the bacterium Methylomirabilis oxyfera plays an important role in natural ecosystems. Its unique physiology can be exploited for more sustainable wastewater treatment technologies. However, operational stability of full-scale

  6. Ultrastructure and Viral Metagenome of Bacteriophages from an Anaerobic Methane Oxidizing Methylomirabilis Bioreactor Enrichment Culture

    NARCIS (Netherlands)

    Gambelli, L.; Cremers, G.; Mesman, R.; Guerrero, S.; Dutilh, B.E.; Jetten, M.S.; Camp, H.J. Op den; Niftrik, L. van

    2016-01-01

    With its capacity for anaerobic methane oxidation and denitrification, the bacterium Methylomirabilis oxyfera plays an important role in natural ecosystems. Its unique physiology can be exploited for more sustainable wastewater treatment technologies. However, operational stability of full-scale

  7. The indirect global warming potential and global temperature change potential due to methane oxidation

    International Nuclear Information System (INIS)

    Boucher, Olivier; Collins, Bill; Friedlingstein, Pierre; Shine, Keith P

    2009-01-01

    Methane is the second most important anthropogenic greenhouse gas in the atmosphere next to carbon dioxide. Its global warming potential (GWP) for a time horizon of 100 years is 25, which makes it an attractive target for climate mitigation policies. Although the methane GWP traditionally includes the methane indirect effects on the concentrations of ozone and stratospheric water vapour, it does not take into account the production of carbon dioxide from methane oxidation. We argue here that this CO 2 -induced effect should be included for fossil sources of methane, which results in slightly larger GWP values for all time horizons. If the global temperature change potential is used as an alternative climate metric, then the impact of the CO 2 -induced effect is proportionally much larger. We also discuss what the correction term should be for methane from anthropogenic biogenic sources.

  8. Evidence for nitrite-dependent anaerobic methane oxidation as a previously overlooked microbial methane sink in wetlands

    Science.gov (United States)

    Hu, Bao-lan; Shen, Li-dong; Lian, Xu; Zhu, Qun; Liu, Shuai; Huang, Qian; He, Zhan-fei; Geng, Sha; Cheng, Dong-qing; Lou, Li-ping; Xu, Xiang-yang; Zheng, Ping; He, Yun-feng

    2014-01-01

    The process of nitrite-dependent anaerobic methane oxidation (n-damo) was recently discovered and shown to be mediated by “Candidatus Methylomirabilis oxyfera” (M. oxyfera). Here, evidence for n-damo in three different freshwater wetlands located in southeastern China was obtained using stable isotope measurements, quantitative PCR assays, and 16S rRNA and particulate methane monooxygenase gene clone library analyses. Stable isotope experiments confirmed the occurrence of n-damo in the examined wetlands, and the potential n-damo rates ranged from 0.31 to 5.43 nmol CO2 per gram of dry soil per day at different depths of soil cores. A combined analysis of 16S rRNA and particulate methane monooxygenase genes demonstrated that M. oxyfera-like bacteria were mainly present in the deep soil with a maximum abundance of 3.2 × 107 gene copies per gram of dry soil. It is estimated that ∼0.51 g of CH4 m−2 per year could be linked to the n-damo process in the examined wetlands based on the measured potential n-damo rates. This study presents previously unidentified confirmation that the n-damo process is a previously overlooked microbial methane sink in wetlands, and n-damo has the potential to be a globally important methane sink due to increasing nitrogen pollution. PMID:24616523

  9. Modeling of simultaneous anaerobic methane and ammonium oxidation in a membrane biofilm reactor.

    Science.gov (United States)

    Chen, Xueming; Guo, Jianhua; Shi, Ying; Hu, Shihu; Yuan, Zhiguo; Ni, Bing-Jie

    2014-08-19

    Nitrogen removal by using the synergy of denitrifying anaerobic methane oxidation (DAMO) and anaerobic ammonium oxidation (Anammox) microorganisms in a membrane biofilm reactor (MBfR) has previously been demonstrated experimentally. In this work, a mathematical model is developed to describe the simultaneous anaerobic methane and ammonium oxidation by DAMO and Anammox microorganisms in an MBfR for the first time. In this model, DAMO archaea convert nitrate, both externally fed and/or produced by Anammox, to nitrite, with methane as the electron donor. Anammox and DAMO bacteria jointly remove the nitrite fed/produced, with ammonium and methane as the electron donor, respectively. The model is successfully calibrated and validated using the long-term (over 400 days) dynamic experimental data from the MBfR, as well as two independent batch tests at different operational stages of the MBfR. The model satisfactorily describes the methane oxidation and nitrogen conversion data from the system. Modeling results show the concentration gradients of methane and nitrogen would cause stratification of the biofilm, where Anammox bacteria mainly grow in the biofilm layer close to the bulk liquid and DAMO organisms attach close to the membrane surface. The low surface methane loadings result in a low fraction of DAMO microorganisms, but the high surface methane loadings would lead to overgrowth of DAMO bacteria, which would compete with Anammox for nitrite and decrease the fraction of Anammox bacteria. The results suggest an optimal methane supply under the given condition should be applied not only to benefit the nitrogen removal but also to avoid potential methane emissions.

  10. Internal reforming of methane in solid oxide fuel cell systems

    Science.gov (United States)

    Peters, R.; Dahl, R.; Klüttgen, U.; Palm, C.; Stolten, D.

    Internal reforming is an attractive option offering a significant cost reduction, higher efficiencies and faster load response of a solid oxide fuel cell (SOFC) power plant. However, complete internal reforming may lead to several problems which can be avoided with partial pre-reforming of natural gas. In order to achieve high total plant efficiency associated with low energy consumption and low investment costs, a process concept has been developed based on all the components of the SOFC system. In the case of anode gas recycling an internal steam circuit exists. This has the advantage that there is no need for an external steam generator and the steam concentration in the anode gas is reduced. However, anode gas recycling has to be proven by experiments in a pre-reformer and for internal reforming. The addition of carbon dioxide clearly shows a decrease in catalyst activity, while for temperatures higher than 1000 K hydrogen leads to an increase of the measured methane conversion rates.

  11. Methane-Oxidizing Enzymes: An Upstream Problem in Biological Gas-to-Liquids Conversion.

    Science.gov (United States)

    Lawton, Thomas J; Rosenzweig, Amy C

    2016-08-03

    Biological conversion of natural gas to liquids (Bio-GTL) represents an immense economic opportunity. In nature, aerobic methanotrophic bacteria and anaerobic archaea are able to selectively oxidize methane using methane monooxygenase (MMO) and methyl coenzyme M reductase (MCR) enzymes. Although significant progress has been made toward genetically manipulating these organisms for biotechnological applications, the enzymes themselves are slow, complex, and not recombinantly tractable in traditional industrial hosts. With turnover numbers of 0.16-13 s(-1), these enzymes pose a considerable upstream problem in the biological production of fuels or chemicals from methane. Methane oxidation enzymes will need to be engineered to be faster to enable high volumetric productivities; however, efforts to do so and to engineer simpler enzymes have been minimally successful. Moreover, known methane-oxidizing enzymes have different expression levels, carbon and energy efficiencies, require auxiliary systems for biosynthesis and function, and vary considerably in terms of complexity and reductant requirements. The pros and cons of using each methane-oxidizing enzyme for Bio-GTL are considered in detail. The future for these enzymes is bright, but a renewed focus on studying them will be critical to the successful development of biological processes that utilize methane as a feedstock.

  12. Oxidation of methane in biotrickling filters inoculated with methanotrophic bacteria.

    Science.gov (United States)

    Cáceres, Manuel; Dorado, Antonio D; Gentina, Juan C; Aroca, Germán

    2017-11-01

    The oxidation of methane (CH 4 ) using biofilters has been proposed as an alternative to mitigate anthropogenic greenhouse gas emissions with a low concentration of CH 4 that cannot be used as a source of energy. However, conventional biofilters utilize organic packing materials that have a short lifespan, clogging problems, and are commonly inoculated with non-specific microorganisms leading to unpredictable CH 4 elimination capacities (EC) and removal efficiencies (RE). The main objective of this work was to characterize the oxidation of CH 4 in two biotrickling filters (BTFs) packed with polyethylene rings and inoculated with two methanotrophic bacteria, Methylomicrobium album and Methylocystis sp., in order to determine EC and CO 2 production (pCO 2 ) when using a specific inoculum. The repeatability of the results in both BTFs was determined when they operated at the same inlet load of CH 4 . A dynamic mathematical model that describes the CH 4 abatement in the BTFs was developed and validated using mass transfer and kinetic parameters estimated independently. The results showed that EC and pCO 2 of the BTFs are not identical but very similar for all the conditions tested. The use of specific inoculum has shown a faster startup and higher EC per unit area (0.019 gCH 4  m -2  h -1 ) in comparison to most of the previous studies at the same CH 4 load rate (23.2 gCH 4  m -3  h -1 ). Global mass balance showed that the maximum reduction of CO 2 equivalents was 98.5 gCO 2eq  m -3  h -1 . The developed model satisfactorily described CH 4 abatement in BTFs for a wide range of conditions.

  13. Advances of study on atmospheric methane oxidation (consumption) in forest soil

    Institute of Scientific and Technical Information of China (English)

    WANG Chen-rui; SHI Yi; YANG Xiao-ming; WU Jie; YUE Jin

    2003-01-01

    Next to CO2, methane (CH4) is the second important contributor to global warming in the atmosphere and global atmospheric CH4 budget depends on both CH4 sources and sinks. Unsaturated soil is known as a unique sink for atmospheric CH4 in terrestrial ecosystem. Many comparison studies proved that forest soil had the biggest capacity of oxidizing atmospheric CH4 in various unsaturated soils. However, up to now, there is not an overall review in the aspect of atmospheric CH4 oxidation (consumption) in forest soil. This paper analyzed advances of studies on the mechanism of atmospheric CH4 oxidation, and related natural factors (Soil physical and chemical characters, temperature and moisture, ambient main greenhouse gases concentrations, tree species, and forest fire) and anthropogenic factors (forest clear-cutting and thinning, fertilization, exogenous aluminum salts and atmospheric deposition, adding biocides, and switch of forest land use) in forest soils. It was believed that CH4 consumption rate by forest soil was limited by diffusion and sensitive to changes in water status and temperature of soil. CH4 oxidation was also particularly sensitive to soil C/N, Ambient CO2, CH4 and N2O concentrations, tree species and forest fire. In most cases, anthropogenic disturbances will decrease atmospheric CH4 oxidation, thus resulting in the elevating of atmospheric CH4. Finally, the author pointed out that our knowledge of atmospheric CH4 oxidation (consumption) in forest soil was insufficient. In order to evaluate the contribution of forest soils to atmospheric CH4 oxidation and the role of forest played in the process of global environmental change, and to forecast the trends of global warming exactly, more researchers need to studies further on CH4 oxidation in various forest soils of different areas.

  14. Methane Oxidation and Molecular Characterization of Methanotrophs from a Former Mercury Mine Impoundment

    Directory of Open Access Journals (Sweden)

    Shaun M. Baesman

    2015-06-01

    Full Text Available The Herman Pit, once a mercury mine, is an impoundment located in an active geothermal area. Its acidic waters are permeated by hundreds of gas seeps. One seep was sampled and found to be composed of mostly CO2 with some CH4 present. The δ13CH4 value suggested a complex origin for the methane: i.e., a thermogenic component plus a biological methanogenic portion. The relatively 12C-enriched CO2 suggested a reworking of the ebullitive methane by methanotrophic bacteria. Therefore, we tested bottom sediments for their ability to consume methane by conducting aerobic incubations of slurried materials. Methane was removed from the headspace of live slurries, and subsequent additions of methane resulted in faster removal rates. This activity could be transferred to an artificial, acidic medium, indicating the presence of acidophilic or acid-tolerant methanotrophs, the latter reinforced by the observation of maximum activity at pH = 4.5 with incubated slurries. A successful extraction of sterol and hopanoid lipids characteristic of methanotrophs was achieved, and their abundances greatly increased with increased sediment methane consumption. DNA extracted from methane-oxidizing enrichment cultures was amplified and sequenced for pmoA genes that aligned with methanotrophic members of the Gammaproteobacteria. An enrichment culture was established that grew in an acidic (pH 4.5 medium via methane oxidation.

  15. Methane oxidation and molecular characterization of methanotrophs from a former mercury mine impoundment

    Science.gov (United States)

    Baesman, Shaun; Miller, Laurence G.; Wei, Jeremy H.; Cho, Yirang; Matys, Emily D.; Summons, Roger E.; Welander, Paula V.; Oremland, Ronald S.

    2015-01-01

    The Herman Pit, once a mercury mine, is an impoundment located in an active geothermal area. Its acidic waters are permeated by hundreds of gas seeps. One seep was sampled and found to be composed of mostly CO2 with some CH4 present. The δ13CH4 value suggested a complex origin for the methane: i.e., a thermogenic component plus a biological methanogenic portion. The relatively 12C-enriched CO2 suggested a reworking of the ebullitive methane by methanotrophic bacteria. Therefore, we tested bottom sediments for their ability to consume methane by conducting aerobic incubations of slurried materials. Methane was removed from the headspace of live slurries, and subsequent additions of methane resulted in faster removal rates. This activity could be transferred to an artificial, acidic medium, indicating the presence of acidophilic or acid-tolerant methanotrophs, the latter reinforced by the observation of maximum activity at pH = 4.5 with incubated slurries. A successful extraction of sterol and hopanoid lipids characteristic of methanotrophs was achieved, and their abundances greatly increased with increased sediment methane consumption. DNA extracted from methane-oxidizing enrichment cultures was amplified and sequenced for pmoA genes that aligned with methanotrophic members of the Gammaproteobacteria. An enrichment culture was established that grew in an acidic (pH 4.5) medium via methane oxidation.

  16. Fluxed of nitrous oxide and methane in a lake border ecosystem in northern Germany

    Energy Technology Data Exchange (ETDEWEB)

    Rusch, H.; Rembges, D.; Papke, H.; Rennenberg, H. [Fraunhofer Inst. for Atmospheric Environmental Research, Garmisch-Partenkirchen (Germany)

    1995-12-31

    Methane and nitrous oxide are radiatively active trace gases. This accounts for approximately 20 % of the total anticipated greenhouse effect. The atmospheric mixing ratio of both gases has increased significantly during the last decades at a rate of 0.25 % yr{sup -l} for N{sub 2}O and a rate of 1 % yr{sup -1} for CH{sub 4}. Whether this increase is caused by enhanced biogenic production of both gases or is due to decreased global sinks, has not been definitely elucidated. Soils are an important source of methane and nitrous oxide. Natural wetlands, e.g., have a similar global source strength of methane as rice paddies. On the other hand, well aerated grasslands have been shown to be a sink for atmospheric methane due to methane oxidation. Nitrous oxide is emitted by a wide range of soil types. Its rate of emission is strongly enhanced by nitrogen fertilization. In the present study, fluxes of methane and nitrous oxide were determined in a lake border ecosystem along a toposequence from reed to dry pasture. The aim of this study was to characterize the influence of soil type, land use and season on the flux rates of these greenhouse gases. (author)

  17. Fluxed of nitrous oxide and methane in a lake border ecosystem in northern Germany

    Energy Technology Data Exchange (ETDEWEB)

    Rusch, H; Rembges, D; Papke, H; Rennenberg, H [Fraunhofer Inst. for Atmospheric Environmental Research, Garmisch-Partenkirchen (Germany)

    1996-12-31

    Methane and nitrous oxide are radiatively active trace gases. This accounts for approximately 20 % of the total anticipated greenhouse effect. The atmospheric mixing ratio of both gases has increased significantly during the last decades at a rate of 0.25 % yr{sup -l} for N{sub 2}O and a rate of 1 % yr{sup -1} for CH{sub 4}. Whether this increase is caused by enhanced biogenic production of both gases or is due to decreased global sinks, has not been definitely elucidated. Soils are an important source of methane and nitrous oxide. Natural wetlands, e.g., have a similar global source strength of methane as rice paddies. On the other hand, well aerated grasslands have been shown to be a sink for atmospheric methane due to methane oxidation. Nitrous oxide is emitted by a wide range of soil types. Its rate of emission is strongly enhanced by nitrogen fertilization. In the present study, fluxes of methane and nitrous oxide were determined in a lake border ecosystem along a toposequence from reed to dry pasture. The aim of this study was to characterize the influence of soil type, land use and season on the flux rates of these greenhouse gases. (author)

  18. Remarkable recovery and colonization behaviour of methane oxidizing bacteria in soil after disturbance is controlled by methane source only.

    Science.gov (United States)

    Pan, Yao; Abell, Guy C J; Bodelier, Paul L E; Meima-Franke, Marion; Sessitsch, Angela; Bodrossy, Levente

    2014-08-01

    Little is understood about the relationship between microbial assemblage history, the composition and function of specific functional guilds and the ecosystem functions they provide. To learn more about this relationship we used methane oxidizing bacteria (MOB) as model organisms and performed soil microcosm experiments comprised of identical soil substrates, hosting distinct overall microbial diversities(i.e., full, reduced and zero total microbial and MOB diversities). After inoculation with undisturbed soil, the recovery of MOB activity, MOB diversity and total bacterial diversity were followed over 3 months by methane oxidation potential measurements and analyses targeting pmoA and 16S rRNA genes. Measurement of methane oxidation potential demonstrated different recovery rates across the different treatments. Despite different starting microbial diversities, the recovery and succession of the MOB communities followed a similar pattern across the different treatment microcosms. In this study we found that edaphic parameters were the dominant factor shaping microbial communities over time and that the starting microbial community played only a minor role in shaping MOB microbial community.

  19. Hydrogen and methane synthesis through radiation catalysis. Final report

    International Nuclear Information System (INIS)

    DuBow, J.

    1980-09-01

    The goal of this research was to evaluate the potential for using reactor wastes to synthesize useful products in quasi-photochemical configuration. It was found that semiconductor oxides act as heterogenous catalysts for the formation of H 2 in aqueous media under 60 Co irradiation. The principle of a gamma-ray solar cell was demonstrated experimentally. Experiments with ultraviolet irradiated TiO 2 and ZnO grains demonstrated that both H 2 and H 2 O 2 were formed, in contrast to the results of work by previous authors. These results were rationalized by energy band diagram representations and by applying principles of semiconductor photoelectrochemistry. The concept of gamma-ray assisted desulfurization of coal through radiological degradation and heterogenous catalysis was experimentally demonstrated. The proof-of-concept experiments in the present study provide the basis for further fundamental and applied investigations, particularly in a potentially efficient system with a fresh source and 1.5 m path length

  20. Methane oxidation over noble metal catalysts as related to controlling natural gas vehicle exhaust emissions

    International Nuclear Information System (INIS)

    Oh, S.H.; Mitchell, P.J.; Siewert, R.M.

    1992-01-01

    Natural gas has considerable potential as an alternative automotive fuel. This paper reports on methane, the principal hydrocarbon species in natural-gas engine exhaust, which has extremely low photochemical reactivity but is a powerful greenhouse gas. Therefore, exhaust emissions of unburned methane from natural-gas vehicles are of particular concern. This laboratory reactor study evaluates noble metal catalysts for their potential in the catalytic removal of methane from natural-gas vehicle exhaust. Temperature run-up experiments show that the methane oxidation activity decreases in the order Pd/Al 2 O 3 > Rh/Al 2 O 3 > Pt/Al 2 O 3 . Also, for all the noble metal catalysts studied, methane conversion can be maximized by controlling the O 2 concentration of the feedstream at a point somewhat rich (reducing) of stoichiometry

  1. Hydrogen generator, via catalytic partial oxidation of methane for fuel cells

    Science.gov (United States)

    Recupero, Vincenzo; Pino, Lidia; Di Leonardo, Raffaele; Lagana', Massimo; Maggio, Gaetano

    It is well known that the most acknowledged process for generation of hydrogen for fuel cells is based upon the steam reforming of methane or natural gas. A valid alternative could be a process based on partial oxidation of methane, since the process is mildly exothermic and therefore not energy intensive. Consequently, great interest is expected from conversion of methane into syngas, if an autothermal, low energy intensive, compact and reliable process could be developed. This paper covers the activities, performed by the CNR Institute of Transformation and Storage of Energy (CNR-TAE), on theoretical and experimental studies for a compact hydrogen generator, via catalytic selective partial oxidation of methane, integrated with second generation fuel cells (EC-JOU2 contract). In particular, the project focuses the attention on methane partial oxidation via heterogeneous selective catalysts, in order to: demonstrate the basic catalytic selective partial oxidation of methane (CSPOM) technology in a subscale prototype, equivalent to a nominal output of 5 kWe; develop the CSPOM technology for its application in electric energy production by means of fuel cells; assess, by a balance of plant analysis, and a techno-economic evaluation, the potential benefits of the CSPOM for different categories of fuel cells.

  2. Non-oxidative methane dehydroaromatization reaction over highly ...

    Indian Academy of Sciences (India)

    Pradeep Kumar Budde

    2018-03-02

    Mar 2, 2018 ... damental science to advanced engineering technology for conversion of .... C using an automatic micropore physisorption ana- lyzer (Micrometrics ASAP ..... MoO2 species with methane to form molybdenum car- bide species.

  3. Catalytic combustion of methane over mixed oxides derived from Co-Mg/Al ternary hydrotalcites

    Energy Technology Data Exchange (ETDEWEB)

    Jiang, Zheng [Inorganic Chemistry Laboratory, Department of Chemistry, University of Oxford, OX1 3QR (United Kingdom); Research Centre of Eco-Environmental Sciences, CAS, Beijing 100085 (China); Jesus College, University of Oxford, OX1 3DW (United Kingdom); Yu, Junjie; Cheng, Jie; Hao, Zhengping [Research Centre of Eco-Environmental Sciences, CAS, Beijing 100085 (China); Xiao, Tiancun; Edwards, Peter P. [Inorganic Chemistry Laboratory, Department of Chemistry, University of Oxford, OX1 3QR (United Kingdom); Jones, Martin O. [Inorganic Chemistry Laboratory, Department of Chemistry, University of Oxford, OX1 3QR (United Kingdom); Rutherford Appleton Laboratory, Didcot, OX11 0QX (United Kingdom)

    2010-01-15

    Co{sub x}Mg{sub 3-x} /Al composite oxides (xCoMAO-800) were prepared by calcination of Co{sub x}Mg{sub 3-x}/Al hydrotalcites (x=0.0,0.5,1.0,1.5,2.0,2.5,3.0, respectively) at 800 C. The materials were characterized using XRD, TG-DSC, N{sub 2} adsorption-desorption and TPR. The methane catalytic combustion over the xCoMAO-800 was assessed in a fixed bed micro-reactor. The results revealed that cobalt can be homogenously dispersed into the matrices of the hydrotalcites and determines the structure, specific surface areas and porosity of the derived xCoMAO-800 oxide catalysts. The thermal stability and homogeneity of the hydrotalcites markedly depends on the cobalt concentration in the hydrotalcites. The Co-based hydrotalcite-derived oxides exhibit good activity in the catalytic combustion of methane. The catalytic activity over the xCoMAO-800 oxides enhances with increasing x up to 1.5, but subsequently decreases dramatically as cobalt loadings are further increased. The 1.5CoMAO-800 catalyst shows the best methane combustion activity, igniting methane at 450 C and completing methane combustion around 600 C. The catalytic combustion activity over the xCoMAO-800 oxides are closely related to the strong Co-Mg/Al interaction within the mixed oxides according to the TG-DSC, TPR and activity characteristics. (author)

  4. Methane production by mariculture on land. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Wagener, K.

    1985-01-01

    It was the aim of this program to have the whole cycle running, consisting of algae production, harvesting, fermentation to biogas, and mineral nutrient recycling into the algae ponds in the form of the fermentation residue (sludge). For this purpose two pilot ponds with a total area of 160 m/sup 2/ have been installed and operated which provided a lot of new experience and success in this new field: concerning pond regime, harvesting procedure and species control. As a preparatory step for the fermentation at pilot scale (which is a subject of the next period), the anaerobic digesteability of micro and macro algae was tested at the laboratory scale. The recycling of unoxidized fermentation sludge directly into the algae ponds has successfully been tested over a period of 4 months; it was finished by seasonal circumstances in November 1981. Finally, the productivities of 3 different algal strains, candidates for energy farming, were tested and compared. Tetraselmis showed the highest productivity yielding 65 tons/ha/yr, followed by Oscillatoria with about 88% of this, and Ulva with 68%. It seems, however, that with the last species the optimal yield has not yet been reached.

  5. Anaerobic oxidation of methane coupled to thiosulfate reduction in a biotrickling filter.

    Science.gov (United States)

    Cassarini, Chiara; Rene, Eldon R; Bhattarai, Susma; Esposito, Giovanni; Lens, Piet N L

    2017-09-01

    Microorganisms from an anaerobic methane oxidizing sediment were enriched with methane gas as the substrate in a biotrickling filter (BTF) using thiosulfate as electron acceptor for 213days. Thiosulfate disproportionation to sulfate and sulfide were the dominating sulfur conversion process in the BTF and the sulfide production rate was 0.5mmoll -1 day -1 . A specific group of sulfate reducing bacteria (SRB), belonging to the Desulforsarcina/Desulfococcus group, was enriched in the BTF. The BTF biomass showed maximum sulfate reduction rate (0.38mmoll -1 day -1 ) with methane as sole electron donor, measured in the absence of thiosulfate in the BTF. Therefore, a BTF fed with thiosulfate as electron acceptor can be used to enrich SRB of the DSS group and activate the inoculum for anaerobic oxidation of methane coupled to sulfate reduction. Copyright © 2017 Elsevier Ltd. All rights reserved.

  6. Oxidation of methane and hydrogen on Ce1-xGdxO2-δ flourrites

    DEFF Research Database (Denmark)

    Kammer Hansen, K.; Mogensen, Mogens Bjerg

    2005-01-01

    The oxidation of methane and hydrogen was studied on cone shaped electrodes with the composition Ce1-xGdxO2-delta (x equals 0, 0.1, 0.2, 0.4). It was shown that the area specific resistance values measured at open-circuit voltage (OCV) for the oxidation of both methane and hydrogen is lowest...... for the composition Ce0.9Gd0.1O1.95. The OCV in wet methane was shown to depend on the material composition. It was shown that stable operation in wet methane could be achieved as long as the temperature was kept below 750degreesC. (C) 2004 The Electrochemical Society....

  7. Anaerobic oxidation of methane in grassland soils used for cattle husbandry

    Directory of Open Access Journals (Sweden)

    A. Bannert

    2012-10-01

    Full Text Available While the importance of anaerobic methane oxidation has been reported for marine ecosystems, the role of this process in soils is still questionable. Grasslands used as pastures for cattle overwintering show an increase in anaerobic soil micro-sites caused by animal treading and excrement deposition. Therefore, anaerobic potential methane oxidation activity of severely impacted soil from a cattle winter pasture was investigated in an incubation experiment under anaerobic conditions using 13C-labelled methane. We were able to detect a high microbial activity utilizing CH4 as nutrient source shown by the respiration of 13CO2. Measurements of possible terminal electron acceptors for anaerobic oxidation of methane were carried out. Soil sulfate concentrations were too low to explain the oxidation of the amount of methane added, but enough nitrate and iron(III were detected. However, only nitrate was consumed during the experiment. 13C-PLFA analyses clearly showed the utilization of CH4 as nutrient source mainly by organisms harbouring 16:1ω7 PLFAs. These lipids were also found as most 13C-enriched fatty acids by Raghoebarsing et al. (2006 after addition of 13CH4 to an enrichment culture coupling denitrification of nitrate to anaerobic oxidation of methane. This might be an indication for anaerobic oxidation of methane by relatives of "Candidatus Methylomirabilis oxyfera" in the investigated grassland soil under the conditions of the incubation experiment.

  8. Steam Methane Reformation Testing for Air-Independent Solid Oxide Fuel Cell Systems

    Science.gov (United States)

    Mwara, Kamwana N.

    2015-01-01

    Recently, NASA has been looking into utilizing landers that can be propelled by LOX-CH (sub 4), to be used for long duration missions. Using landers that utilize such propellants, also provides the opportunity to use solid oxide fuel cells as a power option, especially since they are able to process methane into a reactant through fuel reformation. One type of reformation, called steam methane reformation, is a process to reform methane into a hydrogen-rich product by reacting methane and steam (fuel cell exhaust) over a catalyst. A steam methane reformation system could potentially use the fuel cell's own exhaust to create a reactant stream that is hydrogen-rich, and requires less internal reforming of the incoming methane. Also, steam reformation may hold some advantages over other types of reforming, such as partial oxidation (PROX) reformation. Steam reformation does not require oxygen, while up to 25 percent can be lost in PROX reformation due to unusable CO (sub 2) reformation. NASA's Johnson Space Center has conducted various phases of steam methane reformation testing, as a viable solution for in-space reformation. This has included using two different types of catalysts, developing a custom reformer, and optimizing the test system to find the optimal performance parameters and operating conditions.

  9. Anaerobic Oxidation of Methane at a Marine Methane Seep in a Forearc Sediment Basin off Sumatra, Indian Ocean.

    Science.gov (United States)

    Siegert, Michael; Krüger, Martin; Teichert, Barbara; Wiedicke, Michael; Schippers, Axel

    2011-01-01

    A cold methane seep was discovered in a forearc sediment basin off the island Sumatra, exhibiting a methane-seep adapted microbial community. A defined seep center of activity, like in mud volcanoes, was not discovered. The seep area was rather characterized by a patchy distribution of active spots. The relevance of anaerobic oxidation of methane (AOM) was reflected by (13)C-depleted isotopic signatures of dissolved inorganic carbon. The anaerobic conversion of methane to CO(2) was confirmed in a (13)C-labeling experiment. Methane fueled a vital microbial community with cell numbers of up to 4 × 10(9) cells cm(-3) sediment. The microbial community was analyzed by total cell counting, catalyzed reporter deposition-fluorescence in situ hybridization (CARD-FISH), quantitative real-time PCR (qPCR), and denaturing gradient gel electrophoresis (DGGE). CARD-FISH cell counts and qPCR measurements showed the presence of Bacteria and Archaea, but only small numbers of Eukarya. The archaeal community comprised largely members of ANME-1 and ANME-2. Furthermore, members of the Crenarchaeota were frequently detected in the DGGE analysis. Three major bacterial phylogenetic groups (δ-Proteobacteria, candidate division OP9, and Anaerolineaceae) were abundant across the study area. Several of these sequences were closely related to the genus Desulfococcus of the family Desulfobacteraceae, which is in good agreement with previously described AOM sites. In conclusion, the majority of the microbial community at the seep consisted of AOM-related microorganisms, while the relevance of higher hydrocarbons as microbial substrates was negligible.

  10. Regulation of methane oxidation in the facultative methanotroph Methylocella silvestris BL2.

    Science.gov (United States)

    Theisen, Andreas R; Ali, M Hanif; Radajewski, Stefan; Dumont, Marc G; Dunfield, Peter F; McDonald, Ian R; Dedysh, Svetlana N; Miguez, Carlos B; Murrell, J Colin

    2005-11-01

    The molecular regulation of methane oxidation in the first fully authenticated facultative methanotroph Methylocella silvestris BL2 was assessed during growth on methane and acetate. Problems of poor growth of Methylocella spp. in small-scale batch culture were overcome by growth in fermentor culture. The genes encoding soluble methane monooxygenase were cloned and sequenced, which revealed that the structural genes for soluble methane monooxygenase, mmoXYBZDC, were adjacent to two genes, mmoR and mmoG, encoding a sigma54 transcriptional activator and a putative GroEL-like chaperone, located downstream (3') of mmoC. Transcriptional analysis revealed that the genes were all cotranscribed from a sigma54-dependent promoter located upstream (5') of mmo X. The transcriptional start site was mapped. Transcriptional analysis of soluble methane monooxygenase genes and expression studies on fermentor grown cultures showed that acetate repressed transcription of sMMO in M. silvestris BL2. The possibility of the presence of a particulate, membrane-bound methane monooxygenase enzyme in M. silvestris BL2 and the copper-mediated regulation of soluble methane monooxygenase was investigated. Both were shown to be absent. A promoter probe vector was constructed and used to assay transcription of the promoter of the soluble methane monoxygenase genes of M. silvestris BL2 grown under various conditions and with different substrates. These data represent the first insights into the molecular physiology of a facultative methanotroph.

  11. Soil fluxes of methane, nitrous oxide, and nitric oxide from aggrading forests in coastal Oregon

    Science.gov (United States)

    Erickson, Heather E.; Perakis, Steven S.

    2014-01-01

    Soil exchanges of greenhouse and other gases are poorly known for Pacific Northwest forests where gradients in nutrient availability and soil moisture may contribute to large variations in fluxes. Here we report fluxes of methane (CH4), nitrous oxide (N2O), and nitric oxide (NO) over multiple seasons from three naturally N-rich, aggrading forests of coastal Oregon, USA. Mean methane uptake rates (3.2 mg CH4 m−2 d−1) were high compared with forests globally, negatively related to water-filled pore space (WFPS), but unrelated to N availability or temperature. Emissions of NO (6.0 μg NO–N m−2 h−1) exceeded N2O (1.4 μg N2O–N m−2 h−1), except when WFPS surpassed 55%. Spatial variation in NO fluxes correlated positively with soil nitrate concentrations (which generally exceeded ammonium concentrations, indicating the overall high N status for the sites) and negatively with soil pH, and at one site increased with basal area of N2-fixing red alder. Combined NO and N2O emissions were greatest from the site with highest annual net N mineralization and lowest needle litterfall C/N. Our findings of high CH4 uptake and NO/N2O ratios generally >1 most likely reflect the high porosity of the andic soils underlying the widespread regenerating forests in this seasonally wet region.

  12. Methane-Oxidizing Enzymes: An Upstream Problem in Biological Gas-to-Liquids Conversion

    OpenAIRE

    Lawton, Thomas J.; Rosenzweig, Amy C.

    2016-01-01

    Biological conversion of natural gas to liquids (Bio-GTL) represents an immense economic opportunity. In nature, aerobic methanotrophic bacteria and anaerobic archaea are able to selectively oxidize methane using methane monooxygenase (MMO) and methyl coenzyme M reductase (MCR) enzymes. Although significant progress has been made toward genetically manipulating these organisms for biotechnological applications, the enzymes themselves are slow, complex, and not recombinantly tractable in tradi...

  13. Biogeochemical and molecular signatures of anaerobic methane oxidation in a marine sediment.

    Science.gov (United States)

    Thomsen, T R; Finster, K; Ramsing, N B

    2001-04-01

    Anaerobic methane oxidation was investigated in 6-m-long cores of marine sediment from Aarhus Bay, Denmark. Measured concentration profiles for methane and sulfate, as well as in situ rates determined with isotope tracers, indicated that there was a narrow zone of anaerobic methane oxidation about 150 cm below the sediment surface. Methane could account for 52% of the electron donor requirement for the peak sulfate reduction rate detected in the sulfate-methane transition zone. Molecular signatures of organisms present in the transition zone were detected by using selective PCR primers for sulfate-reducing bacteria and for Archaea. One primer pair amplified the dissimilatory sulfite reductase (DSR) gene of sulfate-reducing bacteria, whereas another primer (ANME) was designed to amplify archaeal sequences found in a recent study of sediments from the Eel River Basin, as these bacteria have been suggested to be anaerobic methane oxidizers (K. U. Hinrichs, J. M. Hayes, S. P. Sylva, P. G. Brewer, and E. F. DeLong, Nature 398:802-805, 1999). Amplification with the primer pairs produced more amplificate of both target genes with samples from the sulfate-methane transition zone than with samples from the surrounding sediment. Phylogenetic analysis of the DSR gene sequences retrieved from the transition zone revealed that they all belonged to a novel deeply branching lineage of diverse DSR gene sequences not related to any previously described DSR gene sequence. In contrast, DSR gene sequences found in the top sediment were related to environmental sequences from other estuarine sediments and to sequences of members of the genera Desulfonema, Desulfococcus, and Desulfosarcina. Phylogenetic analysis of 16S rRNA sequences obtained with the primers targeting the archaeal group of possible anaerobic methane oxidizers revealed two clusters of ANME sequences, both of which were affiliated with sequences from the Eel River Basin.

  14. Biological oxidation of dissolved methane in effluents from anaerobic reactors using a down-flow hanging sponge reactor.

    Science.gov (United States)

    Hatamoto, Masashi; Yamamoto, Hiroki; Kindaichi, Tomonori; Ozaki, Noriatsu; Ohashi, Akiyoshi

    2010-03-01

    Anaerobic wastewater treatment plants discharge dissolved methane, which is usually not recovered. To prevent emission of methane, which is a greenhouse gas, we utilized an encapsulated down-flow hanging sponge reactor as a post-treatment to biologically oxidize dissolved methane. Within 3 weeks after reactor start-up, methane removal efficiency of up to 95% was achieved with a methane removal rate of 0.8 kg COD m(-3) day(-1) at an HRT of 2 h. After increasing the methane-loading rate, the maximum methane removal rate reached 2.2 kg COD m(-3) day(-1) at an HRT of 0.5 h. On the other hand, only about 10% of influent ammonium was oxidized to nitrate during the first period, but as airflow was increased to 2.5 L day(-1), nitrification efficiency increased to approximately 70%. However, the ammonia oxidation rate then decreased with an increase in the methane-loading rate. These results indicate that methane oxidation occurred preferentially over ammonium oxidation in the reactor. Cloning of the 16S rRNA and pmoA genes as well as phylogenetic and T-RFLP analyses revealed that type I methanotrophs were the dominant methane oxidizers, whereas type II methanotrophs were detected only in minor portion of the reactor. Copyright 2009 Elsevier Ltd. All rights reserved.

  15. Methanation of carbon oxides. History, status quo and future perspectives

    Energy Technology Data Exchange (ETDEWEB)

    Kaltner, W.; Rakoczy, R.A. [Clariant SE, Muenchen (Germany)

    2012-07-01

    With increasing demand in fossil sources and especially crude oil based energy carrier, proven reserves will be diminishing. Besides alternative and sustainable sources the conversion of coal into fuels which can be distributed within the existing infrastructure becomes extremely important in areas of fast growing energy demand. Driver for these technologies is mostly the lack of crude oil and availability of coal like in China or South Africa. The most common way to convert coal into chemicals and fuels is the gasification to yield a gas mixture known as synthesis gas. Synthesis gas can be converted in highly pure methane used as 'substitute natural gas' (SNG) in gas grids of major cities to produce heat at home and industry. All available SNG technologies are characterized by the difficulty to control the extreme heat release of the methanation reaction. This presentation will give an overview on available gasification and methanation technologies from recent point of view. A lot of processes are already described in literature and there are pilot and real plants for methanation and especially SNG built. Moreover, a new process to produce methane from synthesis gas without the need of recycle streams and high temperatures will be introduced. This novel process developed by Foster Wheeler - using catalysts from Clariant - is called 'VESTA Process' in accordance with the Roman goddess of hearth and fire. (orig.)

  16. Improved stratospheric atmosphere forecasts in the general circulation model through a methane oxidation parametrization

    Science.gov (United States)

    Wang, S.; Jun, Z.

    2017-12-01

    Climatic characteristics of tropical stratospheric methane have been well researched using various satellite data, and numerical simulations have furtherly conducted using chemical climatic models, while the impact of stratospheric methane oxidation on distribution of water vapor is not paid enough attention in general circulation models. Simulated values of water vapour in the tropical upper stratosphere, and throughout much of the extratropical stratosphere, were too low. Something must be done to remedy this deficiency in order to producing realistic stratospheric water vapor using a general circulation model including the whole stratosphere. Introduction of a simple parametrization of the upper-stratospheric moisture source due to methane oxidation and a sink due to photolysis in the mesosphere was conducted. Numerical simulations and analysis of the influence of stratospheric methane on the prediction of tropical stratospheric moisture and temperature fields were carried out. This study presents the advantages of methane oxidation parametrization in producing a realistic distribution of water vapour in the tropical stratosphere and analyzes the impact of methane chemical process on the general circulation model using two storm cases including a heavy rain in South China and a typhoon caused tropical storm.It is obvious that general circulation model with methane oxidation parametrization succeeds in simulating the water vapor and temperature in stratosphere. The simulating rain center value of contrast experiment is increased up to 10% than that of the control experiment. Introduction of methane oxidation parametrization has modified the distribution of water vapour and then producing a broadly realistic distribution of temperature. Objective weather forecast verifications have been performed using simulating results of one month, which demonstrate somewhat positive effects on the model skill. There is a certain extent impact of methane oxidation

  17. Community Composition and Ultrastructure of a Nitrate-Dependent Anaerobic Methane-Oxidizing Enrichment Culture.

    Science.gov (United States)

    Gambelli, Lavinia; Guerrero-Cruz, Simon; Mesman, Rob J; Cremers, Geert; Jetten, Mike S M; Op den Camp, Huub J M; Kartal, Boran; Lueke, Claudia; van Niftrik, Laura

    2018-02-01

    Methane is a very potent greenhouse gas and can be oxidized aerobically or anaerobically through microbe-mediated processes, thus decreasing methane emissions in the atmosphere. Using a complementary array of methods, including phylogenetic analysis, physiological experiments, and light and electron microscopy techniques (including electron tomography), we investigated the community composition and ultrastructure of a continuous bioreactor enrichment culture, in which anaerobic oxidation of methane (AOM) was coupled to nitrate reduction. A membrane bioreactor was seeded with AOM biomass and continuously fed with excess methane. After 150 days, the bioreactor reached a daily consumption of 10 mmol nitrate · liter -1 · day -1 The biomass consisted of aggregates that were dominated by nitrate-dependent anaerobic methane-oxidizing " Candidatus Methanoperedens"-like archaea (40%) and nitrite-dependent anaerobic methane-oxidizing " Candidatus Methylomirabilis"-like bacteria (50%). The " Ca Methanoperedens" spp. were identified by fluorescence in situ hybridization and immunogold localization of the methyl-coenzyme M reductase (Mcr) enzyme, which was located in the cytoplasm. The " Ca Methanoperedens" sp. aggregates consisted of slightly irregular coccoid cells (∼1.5-μm diameter) which produced extruding tubular structures and putative cell-to-cell contacts among each other. " Ca Methylomirabilis" sp. bacteria exhibited the polygonal cell shape typical of this genus. In AOM archaea and bacteria, cytochrome c proteins were localized in the cytoplasm and periplasm, respectively, by cytochrome staining. Our results indicate that AOM bacteria and archaea might work closely together in the process of anaerobic methane oxidation, as the bacteria depend on the archaea for nitrite. Future studies will be aimed at elucidating the function of the cell-to-cell interactions in nitrate-dependent AOM. IMPORTANCE Microorganisms performing nitrate- and nitrite-dependent anaerobic

  18. Quantification of methane and nitrous oxide emissions from various waste treatment facilities by tracer dilution method

    Science.gov (United States)

    Mønster, Jacob; Rella, Chris; Jacobson, Gloria; Kjeldsen, Peter; Scheutz, Charlotte

    2013-04-01

    Urban activities generate solid and liquid waste, and the handling and aftercare of the waste results in the emission of various compounds into the surrounding environment. Some of these compounds are emitted as gasses into the atmosphere, including methane and nitrous oxide. Methane and nitrous oxide are strong greenhouse gases and are considered to have 25 and 298 times the greenhouse gas potential of carbon dioxide on a hundred years term (Solomon et al. 2007). Global observations of both gasses have shown increasing concentrations that significantly contribute to the greenhouse gas effect. Methane and nitrous oxide are emitted from both natural and anthropogenic sources and inventories of source specific fugitive emissions from the anthropogenic sources of methane and nitrous oxide of are often estimated on the basis of modeling and mass balance. Though these methods are well-developed, actual measurements for quantification of the emissions is a very useful tool for verifying the modeling and mass balance as well as for validation initiatives done for lowering the emissions of methane and nitrous oxide. One approach to performing such measurements is the tracer dilution method (Galle et al. 2001, Scheutz et al. 2011), where the exact location of the source is located and a tracer gas is released at this source location at a known flow. The ratio of downwind concentrations of the tracer gas and the methane and nitrous oxide gives the emissions rates of the greenhouse gases. This tracer dilution method can be performed using both stationary and mobile measurements and in both cases, real-time measurements of both tracer and quantified gas are required, placing high demands on the analytical detection method. To perform the methane and nitrous oxide measurements, two robust instruments capable of real-time measurements were used, based on cavity ring-down spectroscopy and operating in the near-infrared spectral region. One instrument measured the methane and

  19. Anaerobic oxidation of methane above gas hydrates at Hydrate Ridge, NE Pacific Ocean

    DEFF Research Database (Denmark)

    Treude, T.; Boetius, A.; Knittel, K.

    2003-01-01

    oxidation was extremely low (2.1 mmol m(-2) d(-1)) and was probably due to aerobic oxidation of methane. SR was fueled largely by methane at flow-impacted sites, but exceeded AOM in some cases, most likely due to sediment heterogeneity. At the Acharax field, SR was decoupled from methane oxidation...... and showed low activity. Aggregates of the AOM consortium were abundant at the fluid-impacted sites (between 5.1 x 10(12) and 7.9 x 10(12) aggregates m(-2)) but showed low numbers at the Acharax field (0.4 x 10(12) aggregates m(-2)). A transportreaction model was applied to estimate AOM at Beggiatoa fields...

  20. Methane distribution and oxidation around the Lena Delta in summer 2013

    Directory of Open Access Journals (Sweden)

    I. Bussmann

    2017-11-01

    Full Text Available The Lena River is one of the largest Russian rivers draining into the Laptev Sea. The predicted increases in global temperatures are expected to cause the permafrost areas surrounding the Lena Delta to melt at increasing rates. This melting will result in high amounts of methane reaching the waters of the Lena and the adjacent Laptev Sea. The only biological sink that can lower methane concentrations within this system is methane oxidation by methanotrophic bacteria. However, the polar estuary of the Lena River, due to its strong fluctuations in salinity and temperature, is a challenging environment for bacteria. We determined the activity and abundance of aerobic methanotrophic bacteria by a tracer method and by the quantitative polymerase chain reaction. We described the methanotrophic population with a molecular fingerprinting method (monooxygenase intergenic spacer analysis, as well as the methane distribution (via a headspace method and other abiotic parameters, in the Lena Delta in September 2013. The median methane concentrations were 22 nmol L−1 for riverine water (salinity (S  < 5, 19 nmol L−1 for mixed water (5 < S < 20 and 28 nmol L−1 for polar water (S > 20. The Lena River was not the source of methane in surface water, and the methane concentrations of the bottom water were mainly influenced by the methane concentration in surface sediments. However, the bacterial populations of the riverine and polar waters showed similar methane oxidation rates (0.419 and 0.400 nmol L−1 d−1, despite a higher relative abundance of methanotrophs and a higher estimated diversity in the riverine water than in the polar water. The methane turnover times ranged from 167 days in mixed water and 91 days in riverine water to only 36 days in polar water. The environmental parameters influencing the methane oxidation rate and the methanotrophic population also differed between the water masses. We

  1. Oscillatory Behavior during the Catalytic Partial Oxidation of Methane: Following Dynamic Structural Changes of Palladium Using the QEXAFS Technique

    DEFF Research Database (Denmark)

    Stoetzel, Jan; Frahm, Ronald; Kimmerle, Bertram

    2012-01-01

    oxidation of methane, the catalyst reduced from the end to the beginning of the catalyst bed and oxidized again toward the end as soon as the entire catalyst bed was reduced. On an entirely oxidized catalyst bed, only total oxidation of methane was observed and consumed the oxygen until the conditions...... of the Pd particles at increasing age of the catalyst was observed, which leads to a lower oscillation frequency. Effects of particle size, oven temperature, and oxygen/methane ratio on the oscillation behavior were studied in detail. The deactivation period (reoxidation of Pd) was much less influenced...... by the oven temperature than the ignition behavior of the catalytic partial oxidation of methane. This indicates that deactivation is caused by an autoreduction of the palladium at the beginning of the catalyst bed due to the high temperature achieved by total oxidation of methane....

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

    International Nuclear Information System (INIS)

    Albanna, Muna; Warith, Mostafa; Fernandes, Leta

    2010-01-01

    In this experimental program, the effects of non-methane organic compounds (NMOCs) on the biological methane (CH 4 ) oxidation process were examined. The investigation was performed on compost experiments incubated with CH 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 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 the V max value was 35.0 μg CH 4 h -1 g wetwt -1 . This value was reduced to 19.1 μg CH 4 h -1 g wetwt -1 when mixed NMOCs were present in the batch reactors under the same environmental conditions. The experimental oxidation rates of CH 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.

  3. High rates of anaerobic oxidation of methane, ethane and propane coupled to thiosulphate reduction.

    Science.gov (United States)

    Suarez-Zuluaga, Diego A; Weijma, Jan; Timmers, Peer H A; Buisman, Cees J N

    2015-03-01

    Anaerobic methane oxidation coupled to sulphate reduction and the use of ethane and propane as electron donors by sulphate-reducing bacteria represent new opportunities for the treatment of streams contaminated with sulphur oxyanions. However, growth of microbial sulphate-reducing populations with methane, propane or butane is extremely slow, which hampers research and development of bioprocesses based on these conversions. Thermodynamic calculations indicate that the growth rate with possible alternative terminal electron acceptors such as thiosulphate and elemental sulphur may be higher, which would facilitate future research. Here, we investigate the use of these electron acceptors for oxidation of methane, ethane and propane, with marine sediment as inoculum. Mixed marine sediments originating from Aarhus Bay (Denmark) and Eckernförde Bay (Germany) were cultivated anaerobically at a pH between 7.2 and 7.8 and a temperature of 15 °C in the presence of methane, ethane and propane and various sulphur electron acceptors. The sulphide production rates in the conditions with methane, ethane and propane with sulphate were respectively 2.3, 2.2 and 1.8 μmol S L(-1) day(-1). For sulphur, no reduction was demonstrated. For thiosulphate, the sulphide production rates were up to 50 times higher compared to those of sulphate, with 86.2, 90.7 and 108.1 μmol S L(-1) day(-1) for methane, ethane and propane respectively. This sulphide production was partly due to disproportionation, 50 % for ethane but only 7 and 14 % for methane and propane respectively. The oxidation of the alkanes in the presence of thiosulphate was confirmed by carbon dioxide production. This is, to our knowledge, the first report of thiosulphate use as electron acceptor with ethane and propane as electron donors. Additionally, these results indicate that thiosulphate is a promising electron acceptor to increase start-up rates for sulphate-reducing bioprocesses coupled to short-chain alkane oxidation.

  4. Tuneable diode laser gas analyser for methane measurements on a large scale solid oxide fuel cell

    Science.gov (United States)

    Lengden, Michael; Cunningham, Robert; Johnstone, Walter

    2011-10-01

    A new in-line, real time gas analyser is described that uses tuneable diode laser spectroscopy (TDLS) for the measurement of methane in solid oxide fuel cells. The sensor has been tested on an operating solid oxide fuel cell (SOFC) in order to prove the fast response and accuracy of the technology as compared to a gas chromatograph. The advantages of using a TDLS system for process control in a large-scale, distributed power SOFC unit are described. In future work, the addition of new laser sources and wavelength modulation will allow the simultaneous measurement of methane, water vapour, carbon-dioxide and carbon-monoxide concentrations.

  5. BOREAS TGB-6 Soil Methane Oxidation and Production from NSA BP and Fen Sites

    Science.gov (United States)

    Deck, Bruce; Wahlen, Martin; Hall, Forrest G. (Editor); Conrad, Sara K. (Editor)

    2000-01-01

    The BOReal Ecosystem-Atmosphere Study Trace Gas Biogeochemistry (BOREAS TGB-6) team collected soil methane measurements at several sites in the Southern Study Area (SSA) and Northern Study Area (NSA). This data set contains soil methane consumption (bacterial CH4 oxidation) and associated C-13 fractionation effects in samples that were collected at various sites in 1994 and 1996 from enclosures (chambers). Methane C-13 data in soil gas samples from the NSA Young Jack Pine (YJP) and Old Jack Pine (OJP) sites for 1994 and 1996 are also given. Additional data on the isotopic composition of methane (carbon and hydrogen isotopes) produced in the NSA beaver ponds and fen bog in 1993 and 1994 are given as well. The data are stored in tabular ASCII files.

  6. Environmental control on anaerobic oxidation of methane in the gassy sediments of Eckernforde Bay (German Baltic)

    DEFF Research Database (Denmark)

    Treude, T.; Kruger, M.; Boetius, A.

    2005-01-01

    We investigated the effect of seasonal environmental changes on the rate and distribution of anaerobic oxidation of methane (AOM) in Eckernforde Bay sediments (German Baltic Sea) and identified organisms that are likely to be involved in the process. Surface sediments were sampled during September...... of methane were measured in vitro. AOM changed seasonally within the upper 20 cm of the sediment, with rates being between 1 and 14 nmol cm(-3) d(-1). Its distribution is suggested to be controlled by oxygen and sulfate penetration, temperature, as well as methane supply, leading to a shallow AOM zone during...... AOM in Eckerntorde Bay. These archaea are known also from other marine methane-rich locations. However, they were not directly associated with sulfate-reducing bacteria. AOM is possibly mediated solely by these archaea that show a mesophilic physiology according to the seasonal temperature changes...

  7. Anaerobic methane oxidation and aerobic methane production in an east African great lake (Lake Kivu)

    DEFF Research Database (Denmark)

    Roland, Fleur A.E.; Morana, Cédric; Darchambeau, François

    2018-01-01

    We investigated CH4 oxidation in the water column of Lake Kivu, a deep meromictic tropical lake with CH4-rich anoxic deep waters. Depth profiles of dissolved gases (CH4 and N2O) and a diversity of potential electron acceptors for anaerobic CH4 oxidation (NO3 −, SO4 2−, Fe and Mn oxides) were dete...

  8. OXIDATIVE-REFORMING OF METHANE AND PARTIAL OXIDATION OF METHANE REACTIONS OVER NiO/PrO2/ZrO2 CATALYSTS: EFFECT OF NICKEL CONTENT

    Directory of Open Access Journals (Sweden)

    Y. J. O. Asencios

    Full Text Available Abstract In this work the behavior of NiO-PrO2-ZrO2 catalysts containing various nickel loadings was evaluated in the partial oxidation of methane and oxidative-reforming reactions of methane. The catalysts were characterized by X-Ray Diffraction Analysis (in situ-XRD, Temperature Programmed Reduction (H2-TPR, Scanning Electron Microscopy (SEM/EDX and Adsorption-Desorption of nitrogen (BET area. The reactions were carried out at 750 °C and 1 atm for 5 hours. The catalysts were studied with different nickel content: 0, 5, 10 and 15% (related to total weight of catalyst, wt%. In both reactions, the catalyst containing the mixture of the three oxides (NiO/PrO2/ZrO2 with 15% nickel (15NiPrZr catalyst showed the best activity for the conversion of the reactants into Syngas and showed high selectivity for H2 and CO. The results suggest that the promoter PrO2 and the Niº centers are in a good proportion in the catalyst with 15% Ni. Our results showed that low nickel concentrations in the catalyst led to high metallic dispersion; however, very low nickel concentrations did not favor the methane transformation into Syngas. The catalyst containing only NiO/ZrO2 in the mixture was not sufficient for the catalysis. The presence of the promoter PrO2 was very important for the catalysis of the POM.

  9. Direct methane and nitrous oxide emissions of South African dairy ...

    African Journals Online (AJOL)

    The enteric methane emission factors for dairy cattle of 76.4 kg CH4/head/year and 71.8 kg CH4/head/year for concentrate fed and pasture-based production systems, respectively, were higher than those reported by other developing countries, as well as the IPCC default value of 46 kg CH4/head/year for developing ...

  10. Methane-induced Activation Mechanism of Fused Ferric Oxide-Alumina Catalysts during Methane Decomposition

    KAUST Repository

    Reddy Enakonda, Linga

    2016-06-27

    Activation of Fe2O3-Al2O3 with CH4 (instead of H2) is a meaningful method to achieve catalytic methane decomposition (CMD). This reaction of CMD is more economic and simple against commercial methane steam reforming (MSR) as it produces COx-free H2. In this study, for the first time, structure changes of the catalyst were screened during CH4 reduction with time on stream. The aim was to optimize the pretreatment conditions through understanding the activation mechanism. Based on results from various characterization techniques, reduction of Fe2O3 by CH4 proceeds in three steps: Fe2O3→Fe3O4→FeO→Fe0. Once Fe0 is formed, it decomposes CH4 with formation of Fe3C, which is the crucial initiation step in the CMD process to initiate formation of multiwall carbon nanotubes. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  11. An afterburner-powered methane/steam reformer for a solid oxide fuel cells application

    Science.gov (United States)

    Mozdzierz, Marcin; Chalusiak, Maciej; Kimijima, Shinji; Szmyd, Janusz S.; Brus, Grzegorz

    2018-04-01

    Solid oxide fuel cell (SOFC) systems can be fueled by natural gas when the reforming reaction is conducted in a stack. Due to its maturity and safety, indirect internal reforming is usually used. A strong endothermic methane/steam reforming process needs a large amount of heat, and it is convenient to provide thermal energy by burning the remainders of fuel from a cell. In this work, the mathematical model of afterburner-powered methane/steam reformer is proposed. To analyze the effect of a fuel composition on SOFC performance, the zero-dimensional model of a fuel cell connected with a reformer is formulated. It is shown that the highest efficiency of a solid oxide fuel cell is achieved when the steam-to-methane ratio at the reforming reactor inlet is high.

  12. Anaerobic oxidation of methane in grassland soils used for cattle husbandry

    Czech Academy of Sciences Publication Activity Database

    Bannert, A.; Bogen, C.; Esperschütz, J.; Koubová, Anna; Buegger, F.; Fischer, D.; Radl, V.; Fuss, R.; Chroňáková, Alica; Elhottová, Dana; Šimek, Miloslav; Schloter, M.

    2012-01-01

    Roč. 9, č. 10 (2012), s. 3891-3899 ISSN 1726-4170 R&D Projects: GA ČR GA526/09/1570 Institutional support: RVO:60077344 Keywords : anaerobic oxidation of methane * grassland soils * cattle husbandry Subject RIV: EH - Ecology, Behaviour Impact factor: 3.754, year: 2012

  13. Reaction scheme of partial oxidation of methane to synthesis gas over yttrium-stabilized zirconia

    NARCIS (Netherlands)

    Zhu, J.J.; van Ommen, J.G.; Lefferts, Leonardus

    2004-01-01

    The partial oxidation of methane to synthesis gas over yttrium-stabilized zirconia (YSZ) was studied with in situ FTIR and both steady-state and transient experiments. The four major products, CO, H2, CO2, and H2O, are primary products of CPOM over YSZ. Besides these major products and traces of

  14. Can pine trees act as sources for nitrous oxide (N2O) and methane (CH4)?

    Czech Academy of Sciences Publication Activity Database

    Macháčová, Kateřina; Pihlatie, M.; Vanhatalo, A.; Halmeenmäki, E.; Aaltonen, H.; Kolari, P.; Aalto, J.; Pumpanen, J.; Pavelka, Marian; Acosta, Manuel; Urban, Otmar; Bäck, J.

    2013-01-01

    Roč. 142, č. 2013 (2013), s. 362-366. ISBN 952-5027-76-7. ISSN 0784-3496 R&D Projects: GA MŠk(CZ) ED1.1.00/02.0073 Institutional support: RVO:67179843 Keywords : methane * nitrous oxide * scots pine * transport Subject RIV: EH - Ecology, Behaviour

  15. Development of a novel reactor concept for the partial oxidation of methane to syngas

    NARCIS (Netherlands)

    Smit, J.; van Sint Annaland, M.; Kuipers, J.A.M.

    2004-01-01

    The gas-to-liquid process, consisting of the partial oxidation of methane (POM) followed by the Fischer-Tropsch reaction, is a promising alternative to conventional oil processing for the production of liquid fuels. The cost of a conventional POM process is mainly determined by cryogenic air

  16. Modelling of a reverse flow catalytic membrane reactor for the partial oxidation of methane

    NARCIS (Netherlands)

    Smit, J.; van Sint Annaland, M.; Kuipers, J.A.M.

    2003-01-01

    Gas-To-Liquid (GTL) processes have great potential as alternative to conventional oil and coal processing for the production of liquid fuels. In GTL-processes the partial oxidation of methane (POM) is combined with the Fischer-Tropsch reaction. An important part of the investment costs of a

  17. Learning the Fundamentals of Kinetics and Reaction Engineering with the Catalytic Oxidation of Methane

    Science.gov (United States)

    Cybulskis, Viktor J.; Smeltz, Andrew D.; Zvinevich, Yury; Gounder, Rajamani; Delgass, W. Nicholas; Ribeiro, Fabio H.

    2016-01-01

    Understanding catalytic chemistry, collecting and interpreting kinetic data, and operating chemical reactors are critical skills for chemical engineers. This laboratory experiment provides students with a hands-on supplement to a course in chemical kinetics and reaction engineering. The oxidation of methane with a palladium catalyst supported on…

  18. Biogeochemical evidence that thermophilic Archaea mediate the anaerobic oxidation of methane

    NARCIS (Netherlands)

    Sinninghe Damsté, J.S.; Schouten, S.; Wakeham, S.G.; Hopmans, E.C.

    2003-01-01

    Distributions and isotopic analyses of lipids from sediment cores at a hydrothermally active site in the Guaymas Basin with a steep sedimentary temperature gradient revealed the presence of archaea that oxidize methane anaerobically. The presence of strongly 13C-depleted lipids at greater depths in

  19. Temperatures In Compost Landfill Covers As Result Of Methane Oxidation And Compost Respiration

    DEFF Research Database (Denmark)

    Scheutz, Charlotte; Merono, A. R.; Pedersen, Rasmus Broen

    2011-01-01

    This study investigated the influence of the temperature on methane (CH4) oxidation and respiration in compost sampled at a full scale biocover implemented at Klintholm landfill exhibiting high temperatures. Compost material was collected at Klintholm landfill and incubated with and without CH4...

  20. Methane Steam Reforming over an Ni-YSZ Solid Oxide Fuel Cell Anode in Stack Configuration

    DEFF Research Database (Denmark)

    Mogensen, David; Grunwaldt, Jan-Dierk; Hendriksen, Peter Vang

    2014-01-01

    The kinetics of catalytic steam reforming of methane over an Ni-YSZ anode of a solid oxide fuel cell (SOFC) have been investigated with the cell placed in a stack configuration. In order to decrease the degree of conversion, a single cell stack with reduced area was used. Measurements were...

  1. The Effect of Nitrogen and Argon Dilution on Methane Oxidation in Laminar Flames

    Czech Academy of Sciences Publication Activity Database

    Kozubková, M.; Kozubek, E.; Nevrlý, V.; Bitala, P.; Štěpánek, O.; Dlabka, J.; Vašinek, M.; Bojko, M.; Zelinger, Zdeněk; Kubát, Pavel; Grigorová, E.

    2012-01-01

    Roč. 42, č. 0 (2012), s. 1826-1839 E-ISSN 1877-7058. [International Congress of Chemical and Process Engineering CHISA 2012 /20./. Prague, 25.08.2012-29.08.2012] R&D Projects: GA MŠk LD12020 Institutional support: RVO:61388955 Keywords : dilution * methane oxidation * global chemistry Subject RIV: CF - Physical ; Theoretical Chemistry

  2. Environmental control on anaerobic oxidation of methane in the gassy sediments of Eckernforde Bay (German Baltic)

    DEFF Research Database (Denmark)

    Treude, T.; Kruger, M.; Boetius, A.

    2005-01-01

    and March. Field rates of AOM and sulfate reduction (SR) were measured with radiotracer methods. Additional parameters were determined that potentially influence AOM, i.e., temperature, salinity, methane, sulfate, and chlorophyll a. Methanogenesis as well as potential rates of AOM and aerobic oxidation...

  3. 2004 Methane and Nitrous Oxide Emissions from Manure Management in South Africa

    Directory of Open Access Journals (Sweden)

    Mokhele Edmond Moeletsi

    2015-03-01

    Full Text Available Manure management in livestock makes a significant contribution towards greenhouse gas emissions in the Agriculture; Forestry and Other Land Use category in South Africa. Methane and nitrous oxide emissions are prevalent in contrasting manure management systems; promoting anaerobic and aerobic conditions respectively. In this paper; both Tier 1 and modified Tier 2 approaches of the IPCC guidelines are utilized to estimate the emissions from South African livestock manure management. Activity data (animal population, animal weights, manure management systems, etc. were sourced from various resources for estimation of both emissions factors and emissions of methane and nitrous oxide. The results show relatively high methane emissions factors from manure management for mature female dairy cattle (40.98 kg/year/animal, sows (25.23 kg/year/animal and boars (25.23 kg/year/animal. Hence, contributions for pig farming and dairy cattle are the highest at 54.50 Gg and 32.01 Gg respectively, with total emissions of 134.97 Gg (3104 Gg CO2 Equivalent. Total nitrous oxide emissions are estimated at 7.10 Gg (2272 Gg CO2 Equivalent and the three main contributors are commercial beef cattle; poultry and small-scale beef farming at 1.80 Gg; 1.72 Gg and 1.69 Gg respectively. Mitigation options from manure management must be taken with care due to divergent conducive requirements of methane and nitrous oxide emissions requirements.

  4. Thermal Modeling and Management of Solid Oxide Fuel Cells Operating with Internally Reformed Methane

    Science.gov (United States)

    Wu, Yiyang; Shi, Yixiang; Cai, Ningsheng; Ni, Meng

    2018-06-01

    A detailed three-dimensional mechanistic model of a large-scale solid oxide fuel cell (SOFC) unit running on partially pre-reformed methane is developed. The model considers the coupling effects of chemical and electrochemical reactions, mass transport, momentum and heat transfer in the SOFC unit. After model validation, parametric simulations are conducted to investigate how the methane pre-reforming ratio affects the transport and electrochemistry of the SOFC unit. It is found that the methane steam reforming reaction has a "smoothing effect", which can achieve more uniform distributions of gas compositions, current density and temperature among the cell plane. In the case of 1500 W/m2 power density output, adding 20% methane absorbs 50% of internal heat production inside the cell, reduces the maximum temperature difference inside the cell from 70 K to 22 K and reduces the cathode air supply by 75%, compared to the condition of completely pre-reforming of methane. Under specific operating conditions, the pre-reforming ratio of methane has an optimal range for obtaining a good temperature distribution and good cell performance.

  5. Mild oxidation of methane to methanol or acetic acid on supported isolated rhodium catalysts

    Science.gov (United States)

    Shan, Junjun; Li, Mengwei; Allard, Lawrence F.; Lee, Sungsik; Flytzani-Stephanopoulos, Maria

    2017-11-01

    An efficient and direct method of catalytic conversion of methane to liquid methanol and other oxygenates would be of considerable practical value. However, it remains an unsolved problem in catalysis, as typically it involves expensive or corrosive oxidants or reaction media that are not amenable to commercialization. Although methane can be directly converted to methanol using molecular oxygen under mild conditions in the gas phase, the process is either stoichiometric (and therefore requires a water extraction step) or is too slow and low-yielding to be practical. Methane could, in principle, also be transformed through direct oxidative carbonylation to acetic acid, which is commercially obtained through methane steam reforming, methanol synthesis, and subsequent methanol carbonylation on homogeneous catalysts. However, an effective catalyst for the direct carbonylation of methane to acetic acid, which might enable the economical small-scale utilization of natural gas that is currently flared or stranded, has not yet been reported. Here we show that mononuclear rhodium species, anchored on a zeolite or titanium dioxide support suspended in aqueous solution, catalyse the direct conversion of methane to methanol and acetic acid, using oxygen and carbon monoxide under mild conditions. We find that the two products form through independent pathways, which allows us to tune the conversion: three-hour-long batch-reactor tests conducted at 150 degrees Celsius, using either the zeolite-supported or the titanium-dioxide-supported catalyst, yield around 22,000 micromoles of acetic acid per gram of catalyst, or around 230 micromoles of methanol per gram of catalyst, respectively, with selectivities of 60-100 per cent. We anticipate that these unusually high activities, despite still being too low for commercial application, may guide the development of optimized catalysts and practical processes for the direct conversion of methane to methanol, acetic acid and other useful

  6. Production of biogenic manganese oxides coupled with methane oxidation in a bioreactor for removing metals from wastewater.

    Science.gov (United States)

    Matsushita, Shuji; Komizo, Daisuke; Cao, Linh Thi Thuy; Aoi, Yoshiteru; Kindaichi, Tomonori; Ozaki, Noriatsu; Imachi, Hiroyuki; Ohashi, Akiyoshi

    2018-03-01

    Biogenic manganese oxide (BioMnO x ) can efficiently adsorb various minor metals. The production of BioMnO x in reactors to remove metals during wastewater treatment processes is a promising biotechnological method. However, it is difficult to preferentially enrich manganese-oxidizing bacteria (MnOB) to produce BioMnO x during wastewater treatment processes. A unique method of cultivating MnOB using methane-oxidizing bacteria (MOB) to produce soluble microbial products is proposed here. MnOB were successfully enriched in a methane-fed reactor containing MOB. BioMnO x production during the wastewater treatment process was confirmed. Long-term continual operation of the reactor allowed simultaneous removal of Mn(II), Co(II), and Ni(II). The Co(II)/Mn(II) and Ni(II)/Mn(II) removal ratios were 53% and 19%, respectively. The degree to which Mn(II) was removed indicated that the enriched MnOB used utilization-associated products and/or biomass-associated products. Microbial community analysis revealed that methanol-oxidizing bacteria belonging to the Hyphomicrobiaceae family played important roles in the oxidation of Mn(II) by using utilization-associated products. Methane-oxidizing bacteria were found to be inhibited by MnO 2 , but the maximum Mn(II) removal rate was 0.49 kg m -3  d -1 . Copyright © 2017 Elsevier Ltd. All rights reserved.

  7. Oxidative coupling of methane over alkali-promoted simple molybdate catalysts

    International Nuclear Information System (INIS)

    Discoll, S.A.; Zhang, L.; Ozkan, U.S.

    1992-01-01

    The study of various metal oxides and alkali promoted metal oxide catalysts has received much interest in recent years after the earlier reports of ethylene synthesis through oxidative coupling of methane, and of achieving high selectivities over a Li/MgO catalyst under methane and oxygen cofeed conditions. The addition of promoter ions to several oxide catalysts has been studied to determine the effect of the promoter ion on catalytic activity and selectivity. The authors' work has focused on the use of alkali promoters for a simple molybdate catalyst. MnMoO 4 . A study of Na, Li, K, Mg, Ba, Mn, Co, Fe, Cu, Zn, and Ni molybdates by Kiwi et al showed that with the exception of NiMoO 4 , the molybdates were stable for long periods of time under reaction conditions for oxidative coupling. At a conversion level of about 60%, selectivities ranged from 9.8% to 16.6%. The MnMoO 4 and K 2 MnMoO 4 molybdates were the least selective catalysts. Another molybdate, PbMoO 4 , was studied by Baerns et al., with 19% selectivity to C 2 hydrocarbons at 1% conversion. An 11.4% conversion to form aldehyde was also reported. In this paper the authors report the characterization and catalytic behavior of MnMoO 4 catalysts promoted with either Li, Na, or K in oxidative coupling of methane

  8. The reaction mechanism of the partial oxidation of methane to synthesis gas: a transient kinetic study over rhodium and a comparison with platinum

    NARCIS (Netherlands)

    Mallens, E.P.J.; Hoebink, J.H.B.J.; Marin, G.B.M.M.

    1997-01-01

    The partial oxidation of methane to synthesis gas over rhodium sponge has been investigated by admitting pulses of pure methane and pure oxygen as well as mixtures of methane and oxygen to rhodium sponge at temperatures from 873 to 1023 K. Moreover, pulses of oxygen followed by methane and vice

  9. Reaction path of the oxidative coupling of methane over a lithium-doped magnesium oxide catalyst : Factors affecting the Rate of Total Oxidation of Ethane and Ethylene

    NARCIS (Netherlands)

    Roos, J.A.; Korf, S.J.; Veehof, R.H.J.; van Ommen, J.G.; Ross, J.R.H.

    1989-01-01

    Experiments using gas mixtures of O2, C2H6 or C2H4 and CH4 or He have been carried out with a Li/MgO catalyst using a well-mixed reaction system which show that the total oxidation products, CO and CO2, are formed predominantly from ethylene, formed in the oxidative coupling of methane. It is

  10. Final Scientific/Technical Report. A closed path methane and water vapor gas analyzer

    Energy Technology Data Exchange (ETDEWEB)

    Xu, Liukang [LI-COR Inc., Lincoln, NE (United States); McDermitt, Dayle [LI-COR Inc., Lincoln, NE (United States); Anderson, Tyler [LI-COR Inc., Lincoln, NE (United States); Riensche, Brad [LI-COR Inc., Lincoln, NE (United States); Komissarov, Anatoly [LI-COR Inc., Lincoln, NE (United States); Howe, Julie [LI-COR Inc., Lincoln, NE (United States)

    2012-02-01

    Robust, economical, low-power and reliable closed-path methane (CH4), carbon dioxide (CO2), and water vapor (H2O) analyzers suitable for long-term measurements are not readily available commercially. Such analyzers are essential for quantifying the amount of CH4 and CO2 released from various ecosystems (wetlands, rice paddies, forests, etc.) and other surface contexts (e.g. landfills, animal husbandry lots, etc.), and for understanding the dynamics of the atmospheric CH4 and CO2 budget and their impact on climate change and global warming. The purpose of this project is to develop a closed-path methane, carbon dioxide gas and water vapor analyzer capable of long-term measurements in remote areas for global climate change and environmental research. The analyzer will be capable of being deployed over a wide range of ecosystems to understand methane and carbon dioxide exchange between the atmosphere and the surface. Measurements of methane and carbon dioxide exchange need to be made all year-round with limited maintenance requirements. During this Phase II effort, we successfully completed the design of the electronics, optical bench, trace gas detection method and mechanical infrastructure. We are using the technologies of two vertical cavity surface emitting lasers, a multiple-pass Herriott optical cell, wavelength modulation spectroscopy and direct absorption to measure methane, carbon dioxide, and water vapor. We also have designed the instrument application software, Field Programmable Gate Array (FPGA), along with partial completion of the embedded software. The optical bench has been tested in a lab setting with very good results. Major sources of optical noise have been identified and through design, the optical noise floor is approaching -60dB. Both laser modules can be temperature controlled to help maximize the stability of the analyzer. Additionally, a piezo electric transducer has been

  11. Green chemistry perspectives of methane conversion via oxidative methylation of aromatics over zeolite catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Adebajo, M.O. [University of Queensland, St Lucia, Qld. (Australia)

    2007-06-15

    This paper provides a general overview of the recent work that we and other researchers have done on the utilisation of methane for catalytic methylation of aromatic compounds and for direct coal liquefaction for the production of liquid hydrocarbons. In particular, the paper presents a detailed description of more recent substantial experimental evidence that we have provided for the requirement of oxygen as a stoichiometry reactant for benzene methylation with methane over moderately acidic zeolite catalysts. The reaction, which has been termed 'oxidative methylation', was thus postulated to involve a two-step mechanism involving intermediate methanol formation by methane partial oxidation, followed by benzene methylation with methanol in the second step. However, strongly acidic zeolites can cause cracking of benzene to yield methylated products in the absence of oxygen. The participation of methane and oxygen, and the effective use of zeolite catalysts in this methylation reaction definitely have some positive green chemistry implications. Thus, the results of these previous studies are also discussed in this review in light of the principles and tools of green chemistry. Various metrics were used to evaluate the greenness, cost-effectiveness, and material and energy efficiency of the oxidative methylation reaction.

  12. Anaerobic Oxidation of Methane Coupled to Nitrite Reduction by Halophilic Marine NC10 Bacteria.

    Science.gov (United States)

    He, Zhanfei; Geng, Sha; Cai, Chaoyang; Liu, Shuai; Liu, Yan; Pan, Yawei; Lou, Liping; Zheng, Ping; Xu, Xinhua; Hu, Baolan

    2015-08-15

    Anaerobic oxidation of methane (AOM) coupled to nitrite reduction is a novel AOM process that is mediated by denitrifying methanotrophs. To date, enrichments of these denitrifying methanotrophs have been confined to freshwater systems; however, the recent findings of 16S rRNA and pmoA gene sequences in marine sediments suggest a possible occurrence of AOM coupled to nitrite reduction in marine systems. In this research, a marine denitrifying methanotrophic culture was obtained after 20 months of enrichment. Activity testing and quantitative PCR (qPCR) analysis were then conducted and showed that the methane oxidation activity and the number of NC10 bacteria increased correlatively during the enrichment period. 16S rRNA gene sequencing indicated that only bacteria in group A of the NC10 phylum were enriched and responsible for the resulting methane oxidation activity, although a diverse community of NC10 bacteria was harbored in the inoculum. Fluorescence in situ hybridization showed that NC10 bacteria were dominant in the enrichment culture after 20 months. The effect of salinity on the marine denitrifying methanotrophic culture was investigated, and the apparent optimal salinity was 20.5‰, which suggested that halophilic bacterial AOM coupled to nitrite reduction was obtained. Moreover, the apparent substrate affinity coefficients of the halophilic denitrifying methanotrophs were determined to be 9.8 ± 2.2 μM for methane and 8.7 ± 1.5 μM for nitrite. Copyright © 2015, American Society for Microbiology. All Rights Reserved.

  13. Effect of methanogenic substrates on anaerobic oxidation of methane and sulfate reduction by an anaerobic methanotrophic enrichment.

    KAUST Repository

    Meulepas, Roel J W

    2010-05-06

    Anaerobic oxidation of methane (AOM) coupled to sulfate reduction (SR) is assumed to be a syntrophic process, in which methanotrophic archaea produce an interspecies electron carrier (IEC), which is subsequently utilized by sulfate-reducing bacteria. In this paper, six methanogenic substrates are tested as candidate-IECs by assessing their effect on AOM and SR by an anaerobic methanotrophic enrichment. The presence of acetate, formate or hydrogen enhanced SR, but did not inhibit AOM, nor did these substrates trigger methanogenesis. Carbon monoxide also enhanced SR but slightly inhibited AOM. Methanol did not enhance SR nor did it inhibit AOM, and methanethiol inhibited both SR and AOM completely. Subsequently, it was calculated at which candidate-IEC concentrations no more Gibbs free energy can be conserved from their production from methane at the applied conditions. These concentrations were at least 1,000 times lower can the final candidate-IEC concentration in the bulk liquid. Therefore, the tested candidate-IECs could not have been produced from methane during the incubations. Hence, acetate, formate, methanol, carbon monoxide, and hydrogen can be excluded as sole IEC in AOM coupled to SR. Methanethiol did inhibit AOM and can therefore not be excluded as IEC by this study.

  14. Dissolved methane oxidation and competition for oxygen in down-flow hanging sponge reactor for post-treatment of anaerobic wastewater treatment

    OpenAIRE

    Hatamoto, Masashi; Miyauchi, Tomo; Kindaichi, Tomonori; Ozaki, Noriatsu; Ohashi, Akiyoshi

    2011-01-01

    Post-treatment of anaerobic wastewater was undertaken to biologically oxidize dissolved methane, with the aim of preventing methane emission. The performance of dissolved methane oxidation and competition for oxygen among methane, ammonium, organic matter, and sulfide oxidizing bacteria were investigated using a lab-scale closed-type down-flow hanging sponge (OHS) reactor. Under the oxygen abundant condition of a hydraulic retention time of 2 h and volumetric air supply rate of 12.95 m(3)-air...

  15. Reaction-transport simulations of non-oxidative methane conversion with continuous hydrogen removal: Homogeneous-heterogeneous methane reaction pathways

    International Nuclear Information System (INIS)

    Li, Lin; Borry, Richard W.; Iglesia, Enrique

    2000-01-01

    Detailed kinetic-transport models were used to explore thermodynamic and kinetic barriers in the non-oxidative conversion of CH4 via homogeneous and homogeneous-heterogeneous pathways and the effects of continuous hydrogen removal and of catalytic sites on attainable yields of useful C2-C10 products. The homogeneous kinetic model combines separately developed models for low-conversion pyrolysis and for chain growth to form large aromatics and carbon. The H2 formed in the reaction decreases CH4 pyrolysis rates and equilibrium conversions and it favors the formation of lighter products. The removal of H2 along tubular reactors with permeable walls increases reaction rates and equilibrium CH4 conversions. C2-C10 yields reach values greater than 90 percent at intermediate values of dimensionless transport rates (delta=1-10), defined as the ratio hydrogen transport and methane conversion rates. Homogeneous reactions require impractical residence times, even with H2 removal, because of slow initiation and chain transfer rates. The introduction of heterogeneous chain initiation pathways using surface sites that form methyl radicals eliminates the induction period without influencing the homogeneous product distribution. Methane conversion, however, occurs predominately in the chain transfer regime, within which individual transfer steps and the formation of C2 intermediates become limited by thermodynamic constraints. Catalytic sites alone cannot overcome these constraints. Catalytic membrane reactors with continuous H2 removal remove these thermodynamic obstacles and decrease the required residence time. Reaction rates become limited by homogeneous reactions of C2 products to form C6+ aromatics. Higher delta values lead to subsequent conversion of the desired C2-C10 products to larger polynuclear aromatics. We conclude that catalytic methane pyrolysis at the low temperatures required for restricted chain growth and the elimination of thermodynamics constraints via

  16. The Apparent Involvement of ANMEs in Mineral Dependent Methane Oxidation, as an Analog for Possible Martian Methanotrophy

    Directory of Open Access Journals (Sweden)

    Victoria J. Orphan

    2011-11-01

    Full Text Available On Earth, marine anaerobic methane oxidation (AOM can be driven by the microbial reduction of sulfate, iron, and manganese. Here, we have further characterized marine sediment incubations to determine if the mineral dependent methane oxidation involves similar microorganisms to those found for sulfate-dependent methane oxidation. Through FISH and FISH-SIMS analyses using 13C and 15N labeled substrates, we find that the most active cells during manganese dependent AOM are primarily mixed and mixed-cluster aggregates of archaea and bacteria. Overall, our control experiment using sulfate showed two active bacterial clusters, two active shell aggregates, one active mixed aggregate, and an active archaeal sarcina, the last of which appeared to take up methane in the absence of a closely-associated bacterial partner. A single example of a shell aggregate appeared to be active in the manganese incubation, along with three mixed aggregates and an archaeal sarcina. These results suggest that the microorganisms (e.g., ANME-2 found active in the manganese-dependent incubations are likely capable of sulfate-dependent AOM. Similar metabolic flexibility for Martian methanotrophs would mean that the same microbial groups could inhabit a diverse set of Martian mineralogical crustal environments. The recently discovered seasonal Martian plumes of methane outgassing could be coupled to the reduction of abundant surface sulfates and extensive metal oxides, providing a feasible metabolism for present and past Mars. In an optimistic scenario Martian methanotrophy consumes much of the periodic methane released supporting on the order of 10,000 microbial cells per cm2 of Martian surface. Alternatively, most of the methane released each year could be oxidized through an abiotic process requiring biological methane oxidation to be more limited. If under this scenario, 1% of this methane flux were oxidized by biology in surface soils or in subsurface aquifers (prior to

  17. Development of Vanadium Phosphaate Catalysts for Methanol Production by Selective Oxidation of Methane.

    Energy Technology Data Exchange (ETDEWEB)

    McCormick, R.L.

    1997-10-01

    This DOE sponsored study of methane partial oxidation was initiated at Amax Research and Development in Golden, CO in October of 1993. Shortly thereafter the management of Amax closed this R&D facility and the PI moved to the Colorado School of Mines. The project was begun again after contract transfer via a novation agreement. Experimental work began with testing of vandyl pyrophosphate (VPO), a well known alkane selective oxidation catalyst. It was found that VPO was not a selective catalyst for methane conversion yielding primarily CO. However, promotion of VPO with Fe, Cr, and other first row transition metals led to measurable yields for formaldehyde, as noted in the summary table. Catalyst characterization studies indicated that the role of promoters was to stabilize some of the vanadium in the V{sup 5+} oxidation state rather than the V{sup 4+} state formally expected for (VO){sub 2}P{sub 2}O{sub 7}.

  18. Partial oxidation of methane in a temperature-controlled dielectric barrier discharge reactor

    KAUST Repository

    Zhang, Xuming

    2015-01-01

    We studied the relative importance of the reduced field intensity and the background reaction temperature in the partial oxidation of methane in a temperature-controlled dielectric barrier discharge reactor. We obtained important mechanistic insight from studying high-temperature and low-pressure conditions with similar reduced field intensities. In the tested range of background temperatures (297 < T < 773 K), we found that the conversion of methane and oxygen depended on both the electron-induced chemistry and the thermo-chemistry, whereas the chemical pathways to the products were overall controlled by the thermo-chemistry at a given temperature. We also found that the thermo-chemistry enhanced the plasma-assisted partial oxidation process. Our findings expand our understanding of the plasma-assisted partial oxidation process and may be helpful in the design of cost-effective plasma reformers. © 2014 The Combustion Institute.

  19. Modeling and parametric simulations of solid oxide fuel cells with methane carbon dioxide reforming

    International Nuclear Information System (INIS)

    Ni, Meng

    2013-01-01

    Highlights: ► A 2D model is developed for solid oxide fuel cells (SOFCs). ► CH 4 reforming by CO 2 (MCDR) is included. ► SOFC with MCDR shows comparable performance with methane steam reforming SOFC. ► Increasing CO electrochemical oxidation greatly enhances the SOFC performance. ► Effects of potential and temperature on SOFC performance are also discussed. - Abstract: A two-dimensional model is developed to simulate the performance of solid oxide fuel cells (SOFCs) fed with CO 2 and CH 4 mixture. The electrochemical oxidations of both CO and H 2 are included. Important chemical reactions are considered in the model, including methane carbon dioxide reforming (MCDR), reversible water gas shift reaction (WGSR), and methane steam reforming (MSR). It’s found that at a CH 4 /CO 2 molar ratio of 50/50, MCDR and reversible WGSR significantly influence the cell performance while MSR is negligibly small. The performance of SOFC fed with CO 2 /CH 4 mixture is comparable to SOFC running on CH 4 /H 2 O mixtures. The electric output of SOFC can be enhanced by operating the cell at a low operating potential or at a high temperature. In addition, the development of anode catalyst with high activity towards CO electrochemical oxidation is important for SOFC performance enhancement. The model can serve as a useful tool for optimization of the SOFC system running on CH 4 /CO 2 mixtures

  20. Development of vanadium-phosphate catalysts for methanol production by selective oxidation of methane

    Energy Technology Data Exchange (ETDEWEB)

    McCormick, R.L. [Colorado School of Mines, Golden, CO (United States)

    1995-12-31

    The United States has vast natural gas reserves which could contribute significantly to our energy security if economical technologies for conversion to liquid fuels and chemicals were developed. Many of these reserves are small scale or in remote locations and of little value unless they can be transported to consumers. Transportation is economically performed via pipeline, but this route is usually unavailable in remote locations. Another option is to convert the methane in the gas to liquid hydrocarbons, such as methanol, which can easily and economically be transported by truck. Therefore, the conversion of methane to liquid hydrocarbons has the potential to decrease our dependence upon oil imports by opening new markets for natural gas and increasing its use in the transportation and chemical sectors of the economy. In this project, we are attempting to develop, and explore new catalysts capable of direct oxidation of methane to methanol. The specific objectives of this work are discussed.

  1. Degradation kinetics of chlorinated aliphatic hydrocarbons by methane oxidizers naturally-associated with wetland plant roots

    Science.gov (United States)

    Powell, C. L.; Goltz, M. N.; Agrawal, A.

    2014-12-01

    Chlorinated aliphatic hydrocarbons (CAHs) are common groundwater contaminants that can be removed from the environment by natural attenuation processes. CAH biodegradation can occur in wetland environments by reductive dechlorination as well as oxidation pathways. In particular, CAH oxidation may occur in vegetated wetlands, by microorganisms that are naturally associated with the roots of wetland plants. The main objective of this study was to evaluate the cometabolic degradation kinetics of the CAHs, cis-1,2-dichloroethene (cisDCE), trichloroethene (TCE), and 1,1,1-trichloroethane (1,1,1TCA), by methane-oxidizing bacteria associated with the roots of a typical wetland plant in soil-free system. Laboratory microcosms with washed live roots investigated aerobic, cometabolic degradation of CAHs by the root-associated methane-oxidizing bacteria at initial aqueous [CH4] ~ 1.9 mg L- 1, and initial aqueous [CAH] ~ 150 μg L- 1; cisDCE and TCE (in the presence of 1,1,1TCA) degraded significantly, with a removal efficiency of approximately 90% and 46%, respectively. 1,1,1TCA degradation was not observed in the presence of active methane oxidizers. The pseudo first-order degradation rate-constants of TCE and cisDCE were 0.12 ± 0.01 and 0.59 ± 0.07 d- 1, respectively, which are comparable to published values. However, their biomass-normalized degradation rate constants obtained in this study were significantly smaller than pure-culture studies, yet they were comparable to values reported for biofilm systems. The study suggests that CAH removal in wetland plant roots may be comparable to processes within biofilms. This has led us to speculate that the active biomass may be on the root surface as a biofilm. The cisDCE and TCE mass losses due to methane oxidizers in this study offer insight into the role of shallow, vegetated wetlands as an environmental sink for such xenobiotic compounds.

  2. The potential of methane-oxidizing bacteria for applications in environmental biotechnology

    Energy Technology Data Exchange (ETDEWEB)

    Wendlandt, Karin-Dagmar; Stottmeister, Ulrich; Jechorek, Mirko [Helmholtz-Center for Environmental Research UFZ, Leipzig (Germany); Helm, Jana [School of Physics and Astronomy, The University of Edinburgh, Edinburgh (United Kingdom); Soltmann, Bettina [Institute for Materials Science, Dresden University of Technology, Dresden (Germany); Beck, Matthias [Oncotec, Pharma Production GmbH, Dessau-Rosslau (Germany)

    2010-04-15

    Methanotrophic bacteria possess a unique set of enzymes enabling them to oxidize, degrade and transform organic molecules and synthesize new compounds. Therefore, they have great potential in environmental biotechnology. The application of these unique properties was demonstrated in three case studies: (i) Methane escaping from leaky gas pipes may lead to massive mortality of trees in urban areas. Lack of oxygen within the soil surrounding tree roots caused by methanotrophic activity was identified as one of the reasons for this phenomenon. The similarity between metabolic reactions performed by the key enzymes of methanotrophs (methane monooxygenase) and ammonium oxidizers (ammonium monooxygenase) might offer a solution to this problem by applying commercially available nitrification and urease inhibitors. (ii) Methanotrophs are able to co-metabolically degrade contaminants such as low-molecular-weight-chlorinated hydrocarbons in soil and water in the presence of methane. Batch and continuous trichloroethylene degradation experiments in laboratory-scale reactors using Methylocystis sp. GB 14 were performed, partly with cells entrapped in a polymer matrix. (iii) Using a short, two-stage pilot-scale process, the intracellular polymer accumulation of poly-{beta}-hydroxybutyrate (PHB) in methanotrophs reached a maximum of 52%. Interestingly, an ultra-high-molecular-weight PHB of 3.1 MDa was accumulated under potassium deficiency. Under strictly controlled conditions (temperature, pH and methane supply) this process can be nonsterile because of the establishment of a stable microbial community (dominant species Methylocystis sp. GB 25 {>=}86% by biomass). The possibility to substitute methane with biogas from renewable sources facilitates the development of a methane-based PHB production process that yields a high-quality biopolymer at competitive costs. (Abstract Copyright [2010], Wiley Periodicals, Inc.)

  3. Ce-Fe-O mixed oxide as oxygen carrier for the direct partial oxidation of methane to syngas

    Institute of Scientific and Technical Information of China (English)

    魏永刚; 王华; 李孔斋

    2010-01-01

    The Ce-Fe-O mixed oxide with a ratio of Ce/Fe=7:3, which was prepared by coprecipitation method and employed as oxygen carrier, for direct partial oxidation of methane to syngas in the absence of gaseous oxygen was explored. The mixed oxide was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM), and the catalytic performances were studied in a fixed-bed quartz reactor and a thermogravimetric reactor, respectively. Approximately 99.4% H2 se...

  4. Electron acceptors for anaerobic oxidation of methane drive microbial community structure and diversity in mud volcanoes.

    Science.gov (United States)

    Ren, Ge; Ma, Anzhou; Zhang, Yanfen; Deng, Ye; Zheng, Guodong; Zhuang, Xuliang; Zhuang, Guoqiang; Fortin, Danielle

    2018-04-06

    Mud volcanoes (MVs) emit globally significant quantities of methane into the atmosphere, however, methane cycling in such environments is not yet fully understood, as the roles of microbes and their associated biogeochemical processes have been largely overlooked. Here, we used data from high-throughput sequencing of microbial 16S rRNA gene amplicons from six MVs in the Junggar Basin in northwest China to quantify patterns of diversity and characterize the community structure of archaea and bacteria. We found anaerobic methanotrophs and diverse sulfate- and iron-reducing microbes in all of the samples, and the diversity of both archaeal and bacterial communities was strongly linked to the concentrations of sulfate, iron and nitrate, which could act as electron acceptors in anaerobic oxidation of methane (AOM). The impacts of sulfate/iron/nitrate on AOM in the MVs were verified by microcosm experiments. Further, two representative MVs were selected to explore the microbial interactions based on phylogenetic molecular ecological networks. The sites showed distinct network structures, key species and microbial interactions, with more complex and numerous linkages between methane-cycling microbes and their partners being observed in the iron/sulfate-rich MV. These findings suggest that electron acceptors are important factors driving the structure of microbial communities in these methane-rich environments. © 2018 The Authors. Environmental Microbiology published by Society for Applied Microbiology and John Wiley & Sons Ltd.

  5. Assessment of the radio 3H-CH4 tracer technique to measure aerobic methane oxidation in the water column

    Czech Academy of Sciences Publication Activity Database

    Bussmann, I.; Matoušů, Anna; Osudar, R.; Mau, S.

    2015-01-01

    Roč. 13, č. 6 (2015), s. 312-327 ISSN 1541-5856 R&D Projects: GA ČR(CZ) GA13-00243S Institutional support: RVO:60077344 Keywords : methane * aerobic methane oxidation * methods * radiotracer Subject RIV: DA - Hydrology ; Limnology Impact factor: 2.008, year: 2015

  6. Experimental Investigation of Flow Resistance in a Coal Mine Ventilation Air Methane Preheated Catalytic Oxidation Reactor

    OpenAIRE

    Zheng, Bin; Liu, Yongqi; Liu, Ruixiang; Meng, Jian; Mao, Mingming

    2015-01-01

    This paper reports the results of experimental investigation of flow resistance in a coal mine ventilation air methane preheated catalytic oxidation reactor. The experimental system was installed at the Energy Research Institute of Shandong University of Technology. The system has been used to investigate the effects of flow rate (200 Nm3/h to 1000 Nm3/h) and catalytic oxidation bed average temperature (20°C to 560°C) within the preheated catalytic oxidation reactor. The pressure drop and res...

  7. Estimation of methane and nitrous oxide emissions from paddy fields in Taiwan

    International Nuclear Information System (INIS)

    Yang, Shang-Shyng; Lai, Chao-Ming; Chang, Hsiu-Lan; Chang, Ed-Huan; Wei, Chia-Bei

    2009-01-01

    To investigate the greenhouse gases emissions from paddy fields, methane and nitrous oxide emissions were estimated with the local measurement and the IPCC method during 1990-2006 in Taiwan. Annual methane emission ranged from 9001 to 14,980 ton in the first crop season for 135,314-242,298 ha of paddy fields, and it was between 16,412 and 35,208 ton for 101,710-211,968 ha in the second crop season with the local measurement for intermittent irrigation. The value ranged from 31,122 to 55,729 ton of methane emission in the first crop season, and it was between 29,493 and 61,471 ton in the second crop season with the IPCC guideline for continuous flooding. Annual nitrous oxide emission from paddy fields was between 371 and 728 ton in the first crop season, and the value ranged from 163 to 365 ton in the second crop season with the local measurement. Methane emission from paddy fields in Taiwan for intermittent irrigation was only 26.72-28.92%, 55.65-57.32% and 41.19-43.10% with the IPCC guidelines for continuous flooding and mean temperature of transplanting stage in the first crop, the second crop and total paddy fields, respectively. The values were 53.44-57.84%, 111.29-114.55% and 82.38-86.20% with the IPCC guidelines for single aeration and mean temperature of transplanting stage, respectively; and the values were 133.60-144.61%, 282.56-286.62% and 205.96-215.49% with the IPCC guidelines for multiple aeration and mean temperature of transplanting stage, respectively. Intermittent irrigation in paddy fields reduces methane emission significantly; appropriate application of nitrogen fertilizer and irrigation in paddy fields also decreases nitrous oxide emission. (author)

  8. Anaerobic oxidation of methane by sulfate in hypersaline groundwater of the Dead Sea aquifer

    Science.gov (United States)

    Avrahamov, N; Antler, G; Yechieli, Y; Gavrieli, I; Joye, S B; Saxton, M; Turchyn, A V; Sivan, O

    2014-01-01

    Geochemical and microbial evidence points to anaerobic oxidation of methane (AOM) likely coupled with bacterial sulfate reduction in the hypersaline groundwater of the Dead Sea (DS) alluvial aquifer. Groundwater was sampled from nine boreholes drilled along the Arugot alluvial fan next to the DS. The groundwater samples were highly saline (up to 6300 mm chlorine), anoxic, and contained methane. A mass balance calculation demonstrates that the very low δ13CDIC in this groundwater is due to anaerobic methane oxidation. Sulfate depletion coincident with isotope enrichment of sulfur and oxygen isotopes in the sulfate suggests that sulfate reduction is associated with this AOM. DNA extraction and 16S amplicon sequencing were used to explore the microbial community present and were found to be microbial composition indicative of bacterial sulfate reducers associated with anaerobic methanotrophic archaea (ANME) driving AOM. The net sulfate reduction seems to be primarily controlled by the salinity and the available methane and is substantially lower as salinity increases (2.5 mm sulfate removal at 3000 mm chlorine but only 0.5 mm sulfate removal at 6300 mm chlorine). Low overall sulfur isotope fractionation observed (34ε = 17 ± 3.5‰) hints at high rates of sulfate reduction, as has been previously suggested for sulfate reduction coupled with methane oxidation. The new results demonstrate the presence of sulfate-driven AOM in terrestrial hypersaline systems and expand our understanding of how microbial life is sustained under the challenging conditions of an extremely hypersaline environment. PMID:25039851

  9. Are high rates of sulphate reduction associated with anaerobic oxidation of methane

    Energy Technology Data Exchange (ETDEWEB)

    Devol, A H; Ahmed, S I

    1981-01-01

    Classical models of sulphur diagenesis in marine sediments are based on the assumption that the rate of sulphate reduction is first order with respect to oxidizable particulate organic carbon (POC). This assumption requires that oxidizable POC, sulphate concentration and the sulphate reduction rate be highest at the top of the sulphate reduction zone and decrease exponentially with increasing sediment depth. However, to explain recent observations of concave upwards methane distributions, the anaerobic consumption of methane has been proposed. Furthermore, it has been proposed that this consumption takes place near the bottom of the sulphate reducing zone where sulphate concentrations are low. Thus, if sulphate reducing bacteria are associated with the anaerobic oxidation of methane, a peak in sulphate reduction rate might be expected in this deep consumption zone. The importance of the process in sedimentary sulphur diagenesis is indicated by calculations estimating that 30 to 75% of the downward sulphate flux at depth may be consumed by methane oxidation within this zone. We present here profiles of sulphate reduction rate in anoxic sediments that show distinct local maxima at the depth where the anaerobic oxidation of methane would be expected. Our measurements were made during July and August 1978 in Saanich Inlet, an anoxic fjord located on the south-east of Vancouver Island, British Columbia. The inlet has a shallow sill (approx 70 m) which restricts circulation of the deeper water (maximum depth 225 m) inside the basin to the extent that for about 8 months of the year the bottom waters contain hydrogen sulphide, the inlet is an ideal location for studying sedimentary sulphate reduction because reactions with oxygen and the effects of burrowing organisms can be neglected.

  10. Inhibition of methane oxidation in slurry surface crust by inorganic nitrogen

    DEFF Research Database (Denmark)

    Duan, Yun-Feng; Elsgaard, Lars; Petersen, Søren O

    2013-01-01

    Livestock slurry is an important source of methane (CH4). Depending on dry matter content, a floating crust may form where methane-oxidizing bacteria (MOB) and CH4 oxidation activity have been found, suggesting that surface crusts may reduce CH4 emissions from slurry. However, it is not known how...... MOB in this environment interact with inorganic nitrogen (N). We studied inhibitory effects of ammonium (NH4+), nitrate (NO3–) and nitrite (NO2–) on potential CH4 oxidation in a cattle slurry surface crust. Methane oxidation was assayed at salt concentrations up to 500 mM at 100 and 10,000 ppmv...... headspace CH4. First-order rate constants were used to evaluate the strength of inhibition. Nitrite was the most potent inhibitor, reducing methanotrophic activity by up to 70% at only 1 mM NO2–. MOB were least sensitive to NO3–, tolerating up to 30 mM NO3– at 100 ppmv CH4 and 50 mM NO3– at 10,000 ppmv CH4...

  11. Improved enrichment culture technique for methane-oxidizing bacteria from marine ecosystems: the effect of adhesion material and gas composition.

    Science.gov (United States)

    Vekeman, Bram; Dumolin, Charles; De Vos, Paul; Heylen, Kim

    2017-02-01

    Cultivation of microbial representatives of specific functional guilds from environmental samples depends largely on the suitability of the applied growth conditions. Especially the cultivation of marine methanotrophs has received little attention, resulting in only a limited number of ex situ cultures available. In this study we investigated the effect of adhesion material and headspace composition on the methane oxidation activity in methanotrophic enrichments obtained from marine sediment. Addition of sterilized natural sediment or alternatively the addition of acid-washed silicon dioxide significantly increased methane oxidation. This positive effect was attributed to bacterial adhesion on the particles via extracellular compounds, with a minimum amount of particles required for effect. As a result, the particles were immobilized, thus creating a stratified environment in which a limited diffusive gas gradients could build up and various microniches were formed. Such diffusive gas gradient might necessitate high headspace concentrations of CH 4 and CO 2 for sufficient concentrations to reach the methane-oxidizing bacteria in the enrichment culture technique. Therefore, high concentrations of methane and carbon dioxide, in addition to the addition of adhesion material, were tested and indeed further stimulated methane oxidation. Use of adhesion material in combination with high concentrations of methane and carbon dioxide might thus facilitate the cultivation and subsequent enrichment of environmentally important members of this functional guild. The exact mechanism of the observed positive effects on methane oxidation and the differential effect on methanotrophic diversity still needs to be explored.

  12. Final report for the Iowa Livestock Industry Waste Characterization and Methane Recovery Information Dissemination Project

    Energy Technology Data Exchange (ETDEWEB)

    Garrison, M.V.; Richard, Thomas L

    2001-11-13

    This report summarizes analytical methods, characterizes Iowa livestock wastes, determines fossil fuel displacement by methane use, assesses the market potential, and offers recommendations for the implementation of methane recovery technologies.

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

    Science.gov (United States)

    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

  14. Methane oxidation by termite mounds estimated by the carbon isotopic composition of methane

    Science.gov (United States)

    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].

  15. Effect of methanogenic substrates on anaerobic oxidation of methane and sulfate reduction by an anaerobic methanotrophic enrichment.

    KAUST Repository

    Meulepas, Roel J W; Jagersma, Christian G; Khadem, Ahmad F; Stams, Alfons J M; Lens, Piet N L

    2010-01-01

    Anaerobic oxidation of methane (AOM) coupled to sulfate reduction (SR) is assumed to be a syntrophic process, in which methanotrophic archaea produce an interspecies electron carrier (IEC), which is subsequently utilized by sulfate-reducing bacteria

  16. Evaluation of the Effects of Iron Oxides on Soil Reducing Conditions and Methane Generation in Cambodian Wetland Rice Fields

    Science.gov (United States)

    Weaver, M.; Benner, S.; Fendorf, S.; Sampson, M.; Leng, M.

    2007-12-01

    Atmospheric concentrations of methane have been steadily increasing over the last 100 years, which has given rise to research of wetland rice fields, recently identified as a major anthropomorphic source of methane. Establishment of experimental soil pots, cultivating an aromatic early variety rice strain in the Kean Svay District of Cambodia, have recently been carried out to evaluate methods to minimize methane release by promoting redox buffering by iron oxides. In the first series of experiments, iron oxides were added to the soils and the rate of change in reducing conditions and methanogenesis onset was monitored. In the second series of experiments, plots are subject to periodic drying cycles to promote rejuvenation of buffering iron oxides. Initial results indicate a delay in the onset of methanogenesis, and overall methane generation, in plots where initial iron oxides concentrations are elevated.

  17. Determination of emissions of methane and nitrous oxide in rice plantations in Guanacaste, Costa Rica

    Directory of Open Access Journals (Sweden)

    Jorge Herrera

    2013-12-01

    Full Text Available Methane and nitrous oxide emissions fluxes were measured in 10 rice plantations located in Liberia, Guanacaste, working at least with 04 varieties of rice and two types of soil in the period August 2012 - April 2013. For the determination of flows static camera technique were used taking four air gas samples located in the headspace of the chamber using a plastic syringe of 12 ml at 0, 10, 20 and 30 min after camera location. The gas samples were analyzed with a gas chromatograph, equipped with FID and ECD. Averages of flow methane and nitrous oxide were recorded between 0,12 to 1,9 kg ha-1d-1 and 0,11 - 1,1 mg ha-1d-1, respectively, and no significant difference was found (p < 0,05 in the values between different rice varieties and soil types subject experimental design.

  18. Low-Energy, Low-Cost Production of Ethylene by Low- Temperature Oxidative Coupling of Methane

    Energy Technology Data Exchange (ETDEWEB)

    Radaelli, Guido [Siluria Technologies, Inc., San Francisco, CA (United States); Chachra, Gaurav [Siluria Technologies, Inc., San Francisco, CA (United States); Jonnavittula, Divya [Siluria Technologies, Inc., San Francisco, CA (United States)

    2017-12-30

    In this project, we develop a catalytic process technology for distributed small-scale production of ethylene by oxidative coupling of methane at low temperatures using an advanced catalyst. The Low Temperature Oxidative Coupling of Methane (LT-OCM) catalyst system is enabled by a novel chemical catalyst and process pioneered by Siluria, at private expense, over the last six years. Herein, we develop the LT-OCM catalyst system for distributed small-scale production of ethylene by identifying and addressing necessary process schemes, unit operations and process parameters that limit the economic viability and mass penetration of this technology to manufacture ethylene at small-scales. The output of this program is process concepts for small-scale LT-OCM catalyst based ethylene production, lab-scale verification of the novel unit operations adopted in the proposed concept, and an analysis to validate the feasibility of the proposed concepts.

  19. Five pesticides decreased oxidation of atmospheric methane in a forest soil

    DEFF Research Database (Denmark)

    Priemé, Anders; Ekelund, Flemming

    2001-01-01

    We found that five tested pesticides (the insecticide Dimethoat 40 EC, the herbicide Tolkan, and the fungicides Tilt 250 EC, Tilt Top, and Corbel) decreased the oxidation of atmospheric methane in slurries from a Danish forest soil. Dimethoat 40 EC was the most toxic with an EC50 value (i.......e. the concentration which caused a 50% inhibition of the methane oxidation) of 10 mg active ingredient (AI) l-1, followed by Tilt 250 EC (EC50=56 mg AI l-1). EC50 of Tilt Top was 350 AI mg l-1, the value of Tolkan was 410 mg AI l-1, while Corbel had a value of 1600 mg AI l-1. Dimethoat 40 EC and Tolkan inhibited...

  20. Thermodynamic Study on the Catalytic Partial Oxidation of Methane to Syngas

    Institute of Scientific and Technical Information of China (English)

    XUJian; WEIWeisheng; 等

    2002-01-01

    The catalytic partial oxidation of methane to syngas (CO+H2) has been simulated thermodynamically with the advanced process simulator PRO/Ⅱ. The influences of temperature,pressure,CH4/O2 ratio and steam addition in feed gas on the conversion of CH4 selectively to syngas and heat duty required were investigated, and their effects on carbon formation were also discussed. The simulation results were in good agreement with the literature data taken from a spouted bed reactor.

  1. Visualizing a Catalyst at Work during the Ignition of the Catalytic Partial Oxidation of Methane

    DEFF Research Database (Denmark)

    Kimmerle, Bertram; Grunwaldt, Jan-Dierk; Baiker, Alfons

    2009-01-01

    We present a spatiotemporal operando X-ray absorption study of a highly dynamic process, the ignition of the noble metal catalyzed partial oxidation of methane. Evolvement and propagation of the platinum component's structural changes are investigated with a high-speed X-ray camera, which...... in combination with temperature profiling by IR-thermography and catalytic activity measurements by online mass spectrometry gives insight into the first stages of the ignition of the reaction toward hydrogen and carbon monoxide....

  2. Comparative study of the addition compounds between lanthanides methane sulfonates (III) and aromatic amino-oxides as ligands

    International Nuclear Information System (INIS)

    Rosario Matos, J. do.

    1989-01-01

    The main goal of this thesis is to further develop the studies on the preparation and characterization of addition compounds obtained from the reaction of lanthanide methane sulfonates and aromatic amino oxides as ligands, pyridine-N-oxides as the picoline-N-oxides (2-pic NO, 3-pic NO and 4-picNO) in order to make a comparative study. (author)

  3. Experimental Investigation of Flow Resistance in a Coal Mine Ventilation Air Methane Preheated Catalytic Oxidation Reactor

    Directory of Open Access Journals (Sweden)

    Bin Zheng

    2015-01-01

    Full Text Available This paper reports the results of experimental investigation of flow resistance in a coal mine ventilation air methane preheated catalytic oxidation reactor. The experimental system was installed at the Energy Research Institute of Shandong University of Technology. The system has been used to investigate the effects of flow rate (200 Nm3/h to 1000 Nm3/h and catalytic oxidation bed average temperature (20°C to 560°C within the preheated catalytic oxidation reactor. The pressure drop and resistance proportion of catalytic oxidation bed, the heat exchanger preheating section, and the heat exchanger flue gas section were measured. In addition, based on a large number of experimental data, the empirical equations of flow resistance are obtained by the least square method. It can also be used in deriving much needed data for preheated catalytic oxidation designs when employed in industry.

  4. Methane oxidation and formation of EPS in compost: effect of oxygen concentration

    International Nuclear Information System (INIS)

    Wilshusen, J.H.; Hettiaratchi, J.P.A.; Visscher, A. de; Saint-Fort, R.

    2004-01-01

    Oxygen concentration plays an important role in the regulation of methane oxidation and the microbial ecology of methanotrophs. However, this effect is still poorly quantified in soil and compost ecosystems. The effect of oxygen on the formation of exopolymeric substances (EPS) is as yet unknown. We studied the effect of oxygen on the evolution of methanotrophic activity. At both high and low oxygen concentrations, peak activity was observed twice within a period of 6 months. Phospholipid fatty acid analysis showed that there was a shift from type I to type II methanotrophs during this period. At high oxygen concentration, EPS production was about 250% of the amount at low oxygen concentration. It is hypothesized that EPS serves as a carbon cycling mechanism for type I methanotrophs when inorganic nitrogen is limiting. Simultaneously, EPS stimulates nitrogenase activity in type II methanotrophs by creating oxygen-depleted zones. The kinetic results were incorporated in a simulation model for gas transport and methane oxidation in a passively aerated biofilter. Comparison between the model and experimental data showed that, besides acting as a micro-scale diffusion barrier, EPS can act as a barrier to macro-scale diffusion, reducing the performance of such biofilters. - 1.5% oxygen resulted in a slightly higher and more stable methane oxidation activity

  5. Numerical modelling of methane oxidation efficiency and coupled water-gas-heat reactive transfer in a sloping landfill cover.

    Science.gov (United States)

    Feng, S; Ng, C W W; Leung, A K; Liu, H W

    2017-10-01

    Microbial aerobic methane oxidation in unsaturated landfill cover involves coupled water, gas and heat reactive transfer. The coupled process is complex and its influence on methane oxidation efficiency is not clear, especially in steep covers where spatial variations of water, gas and heat are significant. In this study, two-dimensional finite element numerical simulations were carried out to evaluate the performance of unsaturated sloping cover. The numerical model was calibrated using a set of flume model test data, and was then subsequently used for parametric study. A new method that considers transient changes of methane concentration during the estimation of the methane oxidation efficiency was proposed and compared against existing methods. It was found that a steeper cover had a lower oxidation efficiency due to enhanced downslope water flow, during which desaturation of soil promoted gas transport and hence landfill gas emission. This effect was magnified as the cover angle and landfill gas generation rate at the bottom of the cover increased. Assuming the steady-state methane concentration in a cover would result in a non-conservative overestimation of oxidation efficiency, especially when a steep cover was subjected to rainfall infiltration. By considering the transient methane concentration, the newly-modified method can give a more accurate oxidation efficiency. Copyright © 2017. Published by Elsevier Ltd.

  6. Iron-Coupled Anaerobic Oxidation of Methane Performed by a Mixed Bacterial-Archaeal Community Based on Poorly Reactive Minerals.

    Science.gov (United States)

    Bar-Or, Itay; Elvert, Marcus; Eckert, Werner; Kushmaro, Ariel; Vigderovich, Hanni; Zhu, Qingzeng; Ben-Dov, Eitan; Sivan, Orit

    2017-11-07

    Anaerobic oxidation of methane (AOM) was shown to reduce methane emissions by over 50% in freshwater systems, its main natural contributor to the atmosphere. In these environments iron oxides can become main agents for AOM, but the underlying mechanism for this process has remained enigmatic. By conducting anoxic slurry incubations with lake sediments amended with 13 C-labeled methane and naturally abundant iron oxides the process was evidenced by significant 13 C-enrichment of the dissolved inorganic carbon pool and most pronounced when poorly reactive iron minerals such as magnetite and hematite were applied. Methane incorporation into biomass was apparent by strong uptake of 13 C into fatty acids indicative of methanotrophic bacteria, associated with increasing copy numbers of the functional methane monooxygenase pmoA gene. Archaea were not directly involved in full methane oxidation, but their crucial participation, likely being mediators in electron transfer, was indicated by specific inhibition of their activity that fully stopped iron-coupled AOM. By contrast, inhibition of sulfur cycling increased 13 C-methane turnover, pointing to sulfur species involvement in a competing process. Our findings suggest that the mechanism of iron-coupled AOM is accomplished by a complex microbe-mineral reaction network, being likely representative of many similar but hidden interactions sustaining life under highly reducing low energy conditions.

  7. Thermal Methane Conversion to Syngas Mediated by Rh1-Doped Aluminum Oxide Cluster Cations RhAl3O4.

    Science.gov (United States)

    Li, Ya-Ke; Yuan, Zhen; Zhao, Yan-Xia; Zhao, Chongyang; Liu, Qing-Yu; Chen, Hui; He, Sheng-Gui

    2016-10-05

    Laser ablation generated RhAl 3 O 4 + heteronuclear metal oxide cluster cations have been mass-selected using a quadrupole mass filter and reacted with CH 4 or CD 4 in a linear ion trap reactor under thermal collision conditions. The reactions have been characterized by state-of-the-art mass spectrometry and quantum chemistry calculations. The RhAl 3 O 4 + cluster can activate four C-H bonds of a methane molecule and convert methane to syngas, an important intermediate product in methane conversion to value-added chemicals. The Rh atom is the active site for activation of the C-H bonds of methane. The high electron-withdrawing capability of Rh atom is the driving force to promote the conversion of methane to syngas. The polarity of Rh oxidation state is changed from positive to negative after the reaction. This study has provided the first example of methane conversion to syngas by heteronuclear metal oxide clusters under thermal collision conditions. Furthermore, the molecular level origin has been revealed for the condensed-phase experimental observation that trace amounts of Rh can promote the participation of lattice oxygen of chemically very inert support (Al 2 O 3 ) to oxidize methane to carbon monoxide.

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

    Science.gov (United States)

    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.

  9. The potential for biologically catalyzed anaerobic methane oxidation on ancient Mars.

    Science.gov (United States)

    Marlow, Jeffrey J; Larowe, Douglas E; Ehlmann, Bethany L; Amend, Jan P; Orphan, Victoria J

    2014-04-01

    This study examines the potential for the biologically mediated anaerobic oxidation of methane (AOM) coupled to sulfate reduction on ancient Mars. Seven distinct fluids representative of putative martian groundwater were used to calculate Gibbs energy values in the presence of dissolved methane under a range of atmospheric CO2 partial pressures. In all scenarios, AOM is exergonic, ranging from -31 to -135 kJ/mol CH4. A reaction transport model was constructed to examine how environmentally relevant parameters such as advection velocity, reactant concentrations, and biomass production rate affect the spatial and temporal dependences of AOM reaction rates. Two geologically supported models for ancient martian AOM are presented: a sulfate-rich groundwater with methane produced from serpentinization by-products, and acid-sulfate fluids with methane from basalt alteration. The simulations presented in this study indicate that AOM could have been a feasible metabolism on ancient Mars, and fossil or isotopic evidence of this metabolic pathway may persist beneath the surface and in surface exposures of eroded ancient terrains.

  10. The effects of fire on biogenic emissions of methane and nitric oxide from wetlands

    Science.gov (United States)

    Levine, Joel S.; Cofer, Wesley R., III; Sebacher, Daniel I.; Rhinehart, Robert P.; Winstead, Edward L.; Sebacher, Shirley; Hinkle, C. Ross; Schmalzer, Paul A.; Koller, Albert M., Jr.

    1990-01-01

    Enhanced emissions of methane (CH4) and nitric oxide (NO) were measured following three controlled burns in a Florida wetlands in 1987 and 1988. Wetlands are the major global source of methane resulting from metabolic activity of methanogenic bacteria. Methanogens require carbon dioxide, acetate, or formate for their growth and the metabolic production of methane. All three water-soluble compounds are produced in large concentrations during biomass burning. Postfire methane emissions exceeded 0.15 g CH 4/sq m per day. Preburn and postburn measurements of soil nutrients indicate significant postburn increases in soil ammonium, from 8.35 to 13.49 parts per million (ppm) in the upper 5 cm of the Juncus marsh and from 8.83 to 23.75 ppm in the upper 5 cm of the Spartina marsh. Soil nitrate concentrations were found to decrease in both marshes after the fire. These measurements indicate that the combustion products of biomass burning exert an important 'fertilizing' effect on the biosphere and on the biogenic production of environmentally significant atmospheric gases.

  11. The production of hydrogen through the uncatalyzed partial oxidation of methane in an internal combustion engine

    Energy Technology Data Exchange (ETDEWEB)

    Karim, Ghazi A.; Wierzba, I. [Department of Mechanical and Manufacturing Engineering, Schulich School of Engineering, University of Calgary, Calgary (Canada)

    2008-04-15

    The thermodynamic and kinetic limitations of the uncatalyzed partial oxidation of methane for the production of synthesis gas, which is made up of mostly hydrogen and carbon monoxide in a variety of proportions, are reviewed. It is suggested that such processes can be made to proceed successfully in a conventional internal combustion engine when operated on excessively rich mixtures of methane and oxygenated air. This is achieved while simultaneously producing power and regenerative exhaust gas heating. Experimental results are described that show a dual fuel engine of the compression ignition type with pilot liquid fuel injection can be operated on excessively rich mixtures of methane and air supplemented with oxygen gas to produce hydrogen rich gas with high methane conversion rates. Similarly, a spark ignition engine was reported to be equally capable of such production and performance. It is shown that there are viable prospects for the simultaneous production of synthesis gas in engines with efficient useful mechanical power and exhaust gas regenerative heating. (author)

  12. Numerical simulation of vertical transport and oxidation of methane in Arctic Ocean

    Science.gov (United States)

    Stepanenko, Victor; Iakovlev, Nikolai

    2013-04-01

    The high abundance of methane in shelf of East Siberian Arctic Seas (ESAS) has been a subject of a number of field studies (e.g. Shakhova et al., 2010). This experimental evidence provoked discussions on probable origins of that methane and possible feedbacks to modern climate change. For instance, the hypothesis of methane hydrates degradation under current ocean warming was tested recently in several modeling studies none of which supported this degradation to be significant feedback for climate change. Regardless the origin of methane the knowledge of its budget in the water column is important to link its bottom flux with emission to the atmosphere (and vice versa). It is frequently assumed that all methane released from a seabed of ESAS shelf reaches the atmosphere. When using ocean circulation models (Biastoch et al., 2011) this simplification is cancelled out but the vertical resolution of 3D models at the shelf (that is several tens meters deep) is not enough to accurately resolve turbulent transport of methane and other gases. Moreover, up the knowledge of authors none of the ocean models includes explicitly bubble transport of gases. These constrains motivate this study. In this study a high-resolution 1D single column ocean model is constructed to explicitly simulate the methane transport, oxidation and emission to the atmosphere. The model accounts for both vertical turbulent transport (using k-ɛ closure) and bubble transport of gases. The ground under the seabed is represented by multilayer heat and moisture transfer model, including methane hydrate evolution. It is forced by time series of atmospheric variables from NCEP reanalysis and horizontal advection terms taken from FEMAO-1 3D ocean model. The baseline simulation is performed for the period 1948-2011. The model is validated using temperature profiles measured at research vessels in ESAS. The annual cycle and multiyear variability of methane profiles in water are studied and compared to

  13. Effects of preconditioning the rhizosphere of different plant species on biotic methane oxidation kinetics.

    Science.gov (United States)

    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.

  14. Induction of enhanced methane oxidation in compost: Temperature and moisture response

    International Nuclear Information System (INIS)

    Mor, Suman; Visscher, Alex de; Ravindra, Khaiwal; Dahiya, R.P.; Chandra, A.; Cleemput, Oswald van

    2006-01-01

    Landfilling is one of the most common ways of municipal solid waste disposal. Degradation of organic waste produces CH 4 and other landfill gases that significantly contribute to global warming. However, before entering the atmosphere, part of the produced CH 4 can be oxidised while passing through the landfill cover. In the present study, the oxidation rate of CH 4 was studied with various types of compost as possible landfill cover. The influence of incubation time, moisture content and temperature on the CH 4 oxidation capacity of different types of compost was examined. It was observed that the influence of moisture content and temperature on methane oxidation is time-dependent. Maximum oxidation rates were observed at moisture contents ranging from 45% to 110% (dry weight basis), while the optimum temperature ranged from 15 to 30 deg. C

  15. Anaerobic Oxidation of Methane in a French meromictic lake (Lake Pavin): Who is responsible?

    Science.gov (United States)

    Grossi, V.; Attard, E.; Birgel, D.; Schaeffer, P.; Jézéquel, D.; Lehours, A.

    2012-12-01

    Methane is an important greenhouse gas and its biogeochemical cycle is of primary significance to the global carbon cycle. The Anaerobic Oxidation of Methane (AOM) has been estimated to be responsible for >90% of methane consumption. This biogeochemical process has been increasingly documented during the last two decades but the underlying microbial processes and their key agents remain incompletely understood. Freshwater lakes account for 2-10% of the total emissions of methane and are therefore an important part of the global methane cycle. Lake Pavin is a French meromictic crater lake with unusual hydrological characteristics: its morphology (depth >92m, mean diameter 750m) induce that waters below 60m are never mixed with overlying waters and remain permanently anoxic. The deep anoxic waters of Lake Pavin contain high concentrations (i.e. 4 mM) of methane but, contrary to other aquatic systems, almost no methane escapes from the lake. Previous biogeochemical and modeling studies suggest that methane is preferentially consumed within the oxic-anoxic transition zone (ca. 55-60 m depth) but that ca. 30% of methane oxidation occurs in the anoxic part of the lake. Phylogenetic (16S rRNA) analyses showed that ANME generally involved in AOM (ANME-1, -2 and -3) are not present in Lake Pavin. Other archaeal groups that do not have any cultured representatives so far appear well represented in the anoxic parts of the lake but their implication in AOM is not demonstrated. The analysis of lipid biomarkers using GC-MS and LC-MS revealed the presence of a low diversity of archaeal-specific biomarkers in the superficial sediments and in the anoxic waters of the lake. Archaeol and caldarcheaol (GDGT-0) are the two main archaeal core lipids detected; other biomarkers generally present in ANME such as pentamethylicosane or hydroxyarchaeol are not present. However, the stable carbon isotopic composition of archaeol (δ13C = -18‰) and of the biphytane chain of GDGT-0 (δ13C

  16. Landfill methane oxidation across climate types in the U.S.

    Science.gov (United States)

    Chanton, Jeffrey; Abichou, Tarek; Langford, Claire; Hater, Gary; Green, Roger; Goldsmith, Doug; Swan, Nathan

    2011-01-01

    Methane oxidation in landfill covers was determined by stable isotope analyses over 37 seasonal sampling events at 20 landfills with intermediate covers over four years. Values were calculated two ways: by assuming no isotopic fractionation during gas transport, which produces a conservative or minimum estimate, and by assuming limited isotopic fractionation with gas transport producing a higher estimate. Thus bracketed, the best assessment of mean oxidation within the soil covers from chamber captured emitted CH(4) was 37.5 ± 3.5%. The fraction of CH(4) oxidized refers to the fraction of CH(4) delivered to the base of the cover that was oxidized to CO(2) and partitioned to microbial biomass instead of being emitted to the atmosphere as CH(4) expressed as a percentage. Air samples were also collected at the surface of the landfill, and represent CH(4) from soil, from leaking infrastructure, and from cover defects. A similar assessment of this data set yields 36.1 ± 7.2% oxidation. Landfills in five climate types were investigated. The fraction oxidized in arid sites was significantly greater than oxidation in mediterranean sites, or cool and warm continental sites. Sub tropical sites had significantly lower CH(4) oxidation than the other types of sites. This relationship may be explained by the observed inverse relationship between cover loading and fractional CH(4) oxidation.

  17. Denitrification coupled with methane anoxic oxidation and microbial community involved identification

    Directory of Open Access Journals (Sweden)

    Renata Medici Frayne Cuba

    2011-02-01

    Full Text Available In this work, the biological denitrification associated with anoxic oxidation of methane and the microbial diversity involved were studied. Kinetic tests for nitrate (NO3- and nitrite (NO2- removal and methane uptake were carried out in 100 mL batch reactors incubated in a shaker (40 rpm at 30 ºC. Denitrificant/methanotrophic biomass was taken from a laboratory scale reactor fed with synthetic nitrified substrates (40 mgN L-1 of NO3- and subsequently NO2- and methane as carbon source. Results obtained from nitrate removal followed a first order reaction, presenting a kinetic apparent constant (kNO3 of 0.0577±0.0057d-1. Two notable points of the denitrification rate (0.12gNO3--N g-1 AVS d-1 and 0.07gNO3--N g-1 AVS d-1 were observed in the beginning and on the seventh day of operation. When nitrite was added as an electron acceptor, denitrification rates were improved, presenting an apparent kinetic constant (kNO2 of 0.0722±0.0044d-1, a maximum denitrification rate of 0.6gNO2--N g-1AVS d-1, and minimum denitrification rate of 0.1gNO2--N g-1AVS d-1 at the beginning and end of the test, respectively. Endogenous material supporting denitrification and methane concentration dissolved in the substrate was discarded from the control experiments in the absence of methane and seed, respectively. Methylomonas sp. was identified in the reactors fed with nitrate and nitrite as well as uncultured bacterium.

  18. Coupled models of free methane gas and anaerobic oxidation of methane : from core to regional scales. Geologica Ultraiectina (339)

    NARCIS (Netherlands)

    Mogollón, J.M.

    2011-01-01

    Methane is a potent greenhouse gas that is produced in marine sediments containing high amounts of degrading organic carbon. It is therefore not surprising that marine sediments contain vast amounts of methane (500-5000 gigatons) present in dissolved (aqueous), free gas (gaseous), and solid

  19. Methane Steam Reforming over an Ni-YSZ Solid Oxide Fuel Cell Anode in Stack Configuration

    Directory of Open Access Journals (Sweden)

    D. Mogensen

    2014-01-01

    Full Text Available The kinetics of catalytic steam reforming of methane over an Ni-YSZ anode of a solid oxide fuel cell (SOFC have been investigated with the cell placed in a stack configuration. In order to decrease the degree of conversion, a single cell stack with reduced area was used. Measurements were performed in the temperature range 600–800°C and the partial pressures of all reactants and products were varied. The obtained rates could be well fitted with a power law expression (r ∝PCH40.7. A simple model is presented which is capable of predicting the methane conversion in a stack configuration from intrinsic kinetics of the anode support material. The predictions are compared with the stack measurements presented here, and good agreement is observed.

  20. Selective catalytic reduction of nitrogen oxides from industrial gases by hydrogen or methane

    International Nuclear Information System (INIS)

    Engelmann Pirez, M.

    2004-12-01

    This work deals with the selective catalytic reduction of nitrogen oxides (NO x ), contained in the effluents of industrial plants, by hydrogen or methane. The aim is to replace ammonia, used as reducing agent, in the conventional process. The use of others reducing agents such as hydrogen or methane is interesting for different reasons: practical, economical and ecological. The catalyst has to convert selectively NO into N 2 , in presence of an excess of oxygen, steam and sulfur dioxide. The developed catalyst is constituted by a support such as perovskites, particularly LaCoO 3 , on which are dispersed noble metals (palladium, platinum). The interaction between the noble metal and the support, generated during the activation of the catalyst, allows to minimize the water and sulfur dioxide inhibitor phenomena on the catalytic performances, particularly in the reduction of NO by hydrogen. (O.M.)

  1. New molecular method to detect denitrifying anaerobic methane oxidation bacteria from different environmental niches.

    Science.gov (United States)

    Xu, Sai; Lu, Wenjing; Muhammad, Farooq Mustafa; Liu, Yanting; Guo, Hanwen; Meng, Ruihong; Wang, Hongtao

    2018-03-01

    The denitrifying anaerobic methane oxidation is an ecologically important process for reducing the potential methane emission into the atmosphere. The responsible bacterium for this process was Candidatus Methylomirabilis oxyfera belonging to the bacterial phylum of NC10. In this study, a new pair of primers targeting all the five groups of NC10 bacteria was designed to amplify NC10 bacteria from different environmental niches. The results showed that the group A was the dominant NC10 phylum bacteria from the sludges and food waste digestate while in paddy soil samples, group A and group B had nearly the same proportion. Our results also indicated that NC10 bacteria could exist in a high pH environment (pH9.24) from the food waste treatment facility. The Pearson relationship analysis showed that the pH had a significant positive relationship with the NC10 bacterial diversity (pbacteria. Copyright © 2017. Published by Elsevier B.V.

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

    Science.gov (United States)

    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.

  3. The role of paraffin oil on the interaction between denitrifying anaerobic methane oxidation and Anammox processes.

    Science.gov (United States)

    Fu, Liang; Ding, Zhao-Wei; Ding, Jing; Zhang, Fang; Zeng, Raymond J

    2015-10-01

    Methane is sparingly soluble in water, resulting in a slow reaction rate in the denitrifying anaerobic methane oxidation (DAMO) process. The slow rate limits the feasibility of research to examine the interaction between the DAMO and the anaerobic ammonium oxidation (Anammox) process. In this study, optimized 5 % (v/v) paraffin oil was added as a second liquid phase to improve methane solubility in a reactor containing DAMO and Anammox microbes. After just addition, methane solubility was found to increase by 25 % and DAMO activity was enhanced. After a 100-day cultivation, the paraffin reactor showed almost two times higher consumption rates of NO3 (-) (0.2268 mmol/day) and NH4 (+) (0.1403 mmol/day), compared to the control reactor without paraffin oil. The microbes tended to distribute in the oil-water interface. The quantitative (q) PCR result showed the abundance of gene copies of DAMO archaea, DAMO bacteria, and Anammox bacteria in the paraffin reactor were higher than those in the control reactor after 1 month. Fluorescence in situ hybridization revealed that the percentages of the three microbes were 55.5 and 77.6 % in the control and paraffin reactors after 100 days, respectively. A simple model of mass balance was developed to describe the interactions between DAMO and Anammox microbes and validate the activity results. A mechanism was proposed to describe the possible way that paraffin oil enhanced DAMO activity. It is quite clear that paraffin oil enhances not only DAMO activity but also Anammox activity via the interaction between them; both NO3 (-) and NH4 (+) consumption rates were about two times those of the control.

  4. Changes in methane oxidation activity and methanotrophic community composition in saline alkaline soils.

    Science.gov (United States)

    Serrano-Silva, Nancy; Valenzuela-Encinas, César; Marsch, Rodolfo; Dendooven, Luc; Alcántara-Hernández, Rocio J

    2014-05-01

    The soil of the former Lake Texcoco is a saline alkaline environment where anthropogenic drainage in some areas has reduced salt content and pH. Potential methane (CH4) consumption rates were measured in three soils of the former Lake Texcoco with different electrolytic conductivity (EC) and pH, i.e. Tex-S1 a >18 years drained soil (EC 0.7 dS m(-1), pH 8.5), Tex-S2 drained for ~10 years (EC 9.0 dS m(-1), pH 10.3) and the undrained Tex-S3 (EC 84.8 dS m(-1), pH 10.3). An arable soil from Alcholoya (EC 0.7 dS m(-1), pH 6.7), located nearby Lake Texcoco was used as control. Methane oxidation in the soil Tex-S1 (lowest EC and pH) was similar to that in the arable soil from Alcholoya (32.5 and 34.7 mg CH4 kg(-1) dry soil day(-1), respectively). Meanwhile, in soils Tex-S2 and Tex-S3, the potential CH4 oxidation rates were only 15.0 and 12.8 mg CH4 kg(-1) dry soil day(-1), respectively. Differences in CH4 oxidation were also related to changes in the methane-oxidizing communities in these soils. Sequence analysis of pmoA gene showed that soils differed in the identity and number of methanotrophic phylotypes. The Alcholoya soil and Tex-S1 contained phylotypes grouped within the upland soil cluster gamma and the Jasper Ridge, California JR-2 clade. In soil Tex-S3, a phylotype related to Methylomicrobium alcaliphilum was detected.

  5. Oxidation of methane on nanoparticulate Au/TiO2 at low temperature: A combined microreactor and DFT study

    DEFF Research Database (Denmark)

    Walther, Guido; Jones, Glenn; Jensen, Søren

    2009-01-01

    Herein we present results from experimental and theoretical studies concerning low temperature oxidation of CH4 over TiO2 supported Au nanoparticles. Our findings suggest that partial oxidation cannot be achieved under these conditions (1 bar, 30–250 °C). In order to understand this further, resu......-calculations investigating the thermodynamics of CH4 oxidation on a stepped Au(2 1 1) surface. Keywords: Gold; Titanium dioxide; Catalysis; Microreactor; Methane; Oxidation; Particle size...

  6. Partial oxidation of methane over Ni/Mg/Al/La mixed oxides prepared from layered double hydrotalcites

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Jun [Low Carbon Energy Conversion Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203 (China); State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi (China); Graduate University of Chinese Academy of Sciences, Beijing 100049 (China); Zhao, Ning; Wei, Wei [State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi (China); Sun, Yuhan [Low Carbon Energy Conversion Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201203 (China); State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi (China)

    2010-11-15

    A series of Ni/Mg/Al/La mixed oxides prepared by thermal decomposition of layered double hydrotalcites (HT) were characterized by XRD, ICP, EXAFS, TGA, TPR-H{sub 2}, SEM, and N{sub 2} adsorption/desorption technique. The results revealed the formation of periclase-type catalysts with mesoporous structure, and the addition of La{sup 3+} lowered the phase crystallization with the formation of small oxide particles. Such catalysts had both high activities and stabilities toward partial oxidation of methane (POM). The catalyst containing 6.5 mol.% La{sup 3+} showed the highest performance at 1053 K with CH{sub 4} conversion of 99%, CO selectivity of 93% and H{sub 2} selectivity of 96%, which could be attributed to the presence of highly dispersed nickel and then the resistance to coke formation due to the promotion effect of lanthanum. (author)

  7. chemical kinetic study of nitrogen oxides formation in methane flameless combustion

    International Nuclear Information System (INIS)

    Alvarado T, Pedro N; Cadavid S, Francisco; Mondragon, P Fanor; Ruiz, Wilson

    2009-01-01

    The present paper deals with the nitrogen oxides formation in a flameless combustion process characterized for using air highly diluted and preheated at high temperatures. The combustion model used in this study was the one dimensional counterflow methane air diffusion flame. The NOx production rate analysis showed that the thermal and prompt mechanisms are the most important for the formation and consumption of NO under dilution conditions for the oxidant in N 2 and combustion products. These mechanisms are related since the starting reaction for NO formation (N2 molecular dissociation) belongs to the prompt mechanism while the NO formation is reported mainly for the thermal mechanism reactions. On the other hand, the NO - NO 2 equilibrium showed that the reaction rates are comparable to that obtained by the thermal and prompt mechanisms, but its global contribution to NO formation are almost insignificant due to the oxidation reaction with radicals HO 2 .

  8. Enhancement of methane gas sensing characteristics of graphene oxide sensor by heat treatment and laser irradiation.

    Science.gov (United States)

    Assar, Mohammadreza; Karimzadeh, Rouhollah

    2016-12-01

    The present study uses a rapid, easy and practical method for cost-effective fabrication of a methane gas sensor. The sensor was made by drop-casting a graphene oxide suspension onto an interdigital circuit surface. The electrical conductivity and gas-sensing characteristics of the sensor were determined and then heat treatment and in situ laser irradiation were applied to improve the device conductivity and gas sensitivity. Real-time monitoring of the evolution of the device current as a function of heat treatment time revealed significant changes in the conductance of the graphene oxide sensor. The use of low power laser irradiation enhanced both the electrical conductivity and sensing response of the graphene oxide sensor. Copyright © 2016 Elsevier Inc. All rights reserved.

  9. Anaerobic oxidation of methane (AOM) in marine sediments from the Skagerrak (Denmark): II. Reaction-transport modeling

    DEFF Research Database (Denmark)

    Dale, A.W.; Regnier, P.; Knab, N.J.

    2008-01-01

    A steady-state reaction-transport model is applied to sediments retrieved by gravity core from two stations (S10 and S13) in the Skagerrak to determine the main kinetic and thermodynamic controls on anaerobic oxidation of methane (AOM). The model considers an extended biomass-implicit reaction...... methane diffuses up from the SMTZ to the top of the core without being consumed. The tailing is due to bioenergetic limitation of AOM in the sulfate reduction zone, because the methane concentration is too low to engender favorable thermodynamic drive. AOM is also bioenergetically inhibited below the SMTZ...

  10. Estimation of methane and nitrous oxide emission from paddy fields and uplands during 1990-2000 in Taiwan

    International Nuclear Information System (INIS)

    Shangshyng Yang; Chungming Liu; Yenlan Liu; Chaoming Lai

    2003-01-01

    To investigate the greenhouse gases emissions from paddy fields and uplands, methane and nitrous oxide emissions were estimated from local measurement and the IPCC guidelines during 1990-2000 in Taiwan. Annual methane emission from 182 807 to 242 298 ha of paddy field in the first crop season ranged from 8062 to 12 066 ton, and it was between 16 261 and 25 007 ton for 144 178-211 968 ha in the second crop season with local measurement. The value ranged from 12 132 to 17 465 ton, and from 16 046 to 24 762 ton of methane in the first and second crop season with the IPCC guidelines for multiple aeration treatments, respectively. Annual nitrous oxide emission was between 472 and 670 ton and between 236 and 359 ton in the first and second crop season, respectively. Methane and nitrous oxide emissions from uplands depend on crop, growth season, fertilizer application and environmental conditions. Annual methane emission from upland crops, vegetable, fruit, ornamental plants, forage crops and green manure crops was 138-252, 412-460, 97-100, 3-5, 4-5 and 3-51 ton, respectively. Annual nitrous oxide emission was 1080-1976, 1784-1994, 2540-2622, 31-54, 43-53 and 38-582 ton, respectively. Annual nitrous oxide emission ranged from 91 to 132 ton for 77 593-112 095 ton of nitrogen-fixing crops, from 991 to 1859 ton for 325 9731-6 183 441 ton of non-nitrogen-fixing crops, and from 1.77 to 2.22 Gg for 921 169-1 172 594 ton of chemical fertilizer application. In addition, rice hull burning emitted 19.3-24.2 ton of methane and 17.2-21.5 ton of nitrous oxide, and corn stalk burning emitted 2.1-4.2 ton of methane and 1.9-3.8 ton of nitrous oxide. Methane emission from the agriculture sector was 26 421-37 914 ton, and nitrous oxide emission was 9810-11 649 ton during 1990-2000 in Taiwan. Intermittent irrigation in paddy fields reduces significantly methane emission; appropriate application of nitrogen fertilization and irrigation in uplands and paddy fields also decreases nitrous oxide

  11. Continuous measurements of ammonia, nitrous oxide and methane from air scrubbers at pig housing facilities.

    Science.gov (United States)

    Van der Heyden, C; Brusselman, E; Volcke, E I P; Demeyer, P

    2016-10-01

    Ammonia, largely emitted by agriculture, involves a great risk for eutrophication and acidification leading to biodiversity loss. Air scrubbers are widely applied to reduce ammonia emission from pig and poultry housing facilities, but it is not always clear whether their performance meets the requirements. Besides, there is a growing international concern for the livestock related greenhouse gases methane and nitrous oxide but hardly any data concerning their fate in air scrubbers are available. This contribution presents the results from measurement campaigns conducted at a chemical, a biological and a two-stage biological air scrubber installed at pig housing facilities in Flanders. Ammonia, nitrous oxide and methane at the inlet and outlet of the air scrubbers were monitored on-line during one week using a photoacoustic gas monitor, which allowed to investigate diurnal fluctuations in the removal performance of air scrubbers. Additionally, the homogeneity of the air scrubbers, normally checked by gas detection tubes, was investigated in more detail using the continuous data. The biological air scrubber with extra nitrification tank performed well in terms of ammonia removal (86 ± 6%), while the two-stage air scrubber suffered from nitrifying bacteria inhibition. In the chemical air scrubber the pH was not kept constant, lowering the ammonia removal efficiency. A lower ammonia removal efficiency was found during the day, when the ventilation rate was the highest. Nitrous oxide was produced inside the biological and two-stage scrubber, resulting in an increased outlet concentration of more than 200%. Methane could not be removed in the different air scrubbers because of its low water solubility. Copyright © 2016 Elsevier Ltd. All rights reserved.

  12. Recent patterns of methane and nitrous oxide fluxes in the terrestrial biosphere: The bottom-up approach (Invited)

    Science.gov (United States)

    Tian, H.

    2013-12-01

    Accurately estimating methane and nitrous oxide emissions from terrestrial ecosystems is critical for resolving global budgets of these greenhouse gases (GHGs) and continuing to mitigate climate warming. In this study, we use a bottom-up approach to estimate annual budgets of both methane and nitrous oxide in global terrestrial ecosystem during 1981-2010 and analyze the underlying mechanisms responsible for spatial and temporal variations in these GHGs. Both methane and nitrous oxide emissions significantly increased from 1981 to 2010, primarily owing to increased air temperature, nitrogen fertilizer use, and land use change. Methane and nitrous oxide emissions increased the fastest in Asia due to the more prominent environmental changes compared to other continents. The cooling effects by carbon dioxide sink in the terrestrial biosphere might be completely offset by increasing methane and nitrous oxide emissions, resulting in a positive global warming potential. Asia and South America were the largest contributors to increasing global warming potential. This study suggested that current management practices might not be effective enough to reduce future global warming.

  13. Estimation of methane and nitrous oxide emission from animal production sector in Taiwan during 1990-2000

    International Nuclear Information System (INIS)

    Shangshyng Yang; Chungming Liu; Yenlan Liu

    2003-01-01

    To investigate the greenhouse gases emissions from the feeding and waste management of livestock and poultry, methane and nitrous oxide emissions were estimated from the local measurement and IPCC guidelines during 1990-2000 in Taiwan. Hog is the major livestock and is followed by goat and cattle, while chicken is the major poultry and is followed by duck and geese. Methane emission from enteric fermentation of livestock was 30.9 Gg in 1990, increased to 39.3 Gg in 1996, and then decreased gradually to 34.9 Gg in 2000. Methane emission from the waste management was 48.5 Gg in 1990, reached the peak value of 60.7 Gg in 1996, and then declined to 43.3 Gg in 2000. In the case of poultry, annual methane emission from enteric fermentation and waste management was 30.6-44.1 ton, and 8.7-13.2 Gg, respectively. Nitrous oxide emission from waste management of livestock was 0.78 ton in 1990, increased to 0.86 ton in 1996, and then decreased to 0.65 ton in 2000. Nitrous oxide emission from waste management of poultry was higher than that of livestock with 1.11 ton in 1990, 1.68 ton in 1999, and 1.65 ton in 2000. There is an urgent need to reduce methane emission from enteric fermentation and recover methane from anaerobic waste treatment for energy in livestock and poultry feeding in Taiwan. (Author)

  14. Methane and Nitrous Oxide Emissions from Agriculture on a Regional Scale

    OpenAIRE

    Agnieszka Wysocka-Czubaszek; Robert Czubaszek; Sławomir Roj-Rojewski; Piotr Banaszuk

    2018-01-01

    Nowadays, agriculture has to meet the growing food demand together with high requirements of environmental protection, especially regarding the climate change. The greenhouse gas emissions differ not only on a global, but also on a regional scale, and mitigation strategies are effective when they are adapted properly. Therefore, the aim of this paper is to present the results of methane (CH4) and nitrous oxide (N2O) emissions inventory on a regional level in Poland in years 1999-2015. The CH4...

  15. Methane Transmission and Oxidation throughout the Soil Column from Three Central Florida Sites

    Science.gov (United States)

    Bond-Lamberty, B. P.; Fansler, S.; Becker, K. E.; Hinkle, C. R.; Bailey, V. L.

    2015-12-01

    When methane (CH4) is generated in anoxic soil sites, it may be subsequently re-oxidized to carbon dioxide (CO2). Understanding the controls on, and magnitudes of, these processes is necessary to accurately represent greenhouse gas production and emission from soils. We used a laboratory incubation to examine the influence of variable conditions on methane transmission and oxidation, and identify critical reaction zones throughout the soil column. Sandy soils were sampled from three different sites at Disney Wilderness Preserve (DWP), Florida, USA: a depression marsh characterized by significant surface organic matter accumulation, a dry pine flatwood site with water intrusion and organic horizon at depth (200+ cm); and an intermediate-drainage site. Contiguous, 30-cm long cores were sampled from N=4 random boreholes at each site, from the surface to the water table (varying from 90 to 240 cm). In the lab, each core was monitored for 50 hours to quantify baseline (pretreatment) gas fluxes before injection with 6 ml CH4 (an amount commensurate with previous field collar measurements) at the base of each core. We then monitored CH4 and CO2 evolution for 100 hours after injection, calculating per-gas and total C evolution. Methane emissions spiked ~10 hours after injection for all cores, peaking at 0.001 μmol/g soil/hr, ~30x larger than pre-injection flux rates. On a C basis, CO2 emissions were orders of magnitude larger, and rose significantly after injection, with elevated rates generally sustained throughout the incubation. Cores from the depression marsh and shallower depths had significantly higher fluxes of both gases. We estimate that 99.1% of the original CH4 injection was oxidized to CO2. These findings suggest either that the methane measured in the field at DWP originates from within a few centimeters of the surface, or that it is produced in much larger quantities deeper in the profile before most is subsequently oxidized. This highlights the need for

  16. Methane-free biogas for direct feeding of solid oxide fuel cells

    Science.gov (United States)

    Leone, P.; Lanzini, A.; Santarelli, M.; Calì, M.; Sagnelli, F.; Boulanger, A.; Scaletta, A.; Zitella, P.

    This paper deals with the experimental analysis of the performance and degradation issues of a Ni-based anode-supported solid oxide fuel cell fed by a methane-free biogas from dark-anaerobic digestion of wastes by pastry and fruit shops. The biogas is produced by means of an innovative process where the biomass is fermented with a pre-treated bacteria inoculum (Clostridia) able to completely inhibit the methanization step during the fermentation process and to produce a H 2/CO 2 mixture instead of conventional CH 4/CO 2 anaerobic digested gas (bio-methane). The proposed biogas production route leads to a biogas composition which avoids the need of introducing a reformer agent into or before the SOFC anode in order to reformate it. In order to analyse the complete behaviour of a SOFC with the bio-hydrogen fuel, an experimental session with several H 2/CO 2 synthetic mixtures was performed on an anode-supported solid oxide fuel cell with a Ni-based anode. It was found that side reactions occur with such mixtures in the typical thermodynamic conditions of SOFCs (650-800 °C), which have an effect especially at high currents, due to the shift to a mixture consisting of hydrogen, carbon monoxide, carbon dioxide and water. However, cells operated with acceptable performance and carbon deposits (typical of a traditional hydrocarbon-containing biogas) were avoided after 50 h of cell operation even at 650 °C. Experiments were also performed with traditional bio-methane from anaerobic digestion with 60/40 vol% of composition. It was found that the cell performance dropped after few hours of operation due to the formation of carbon deposits. A short-term test with the real as-produced biogas was also successfully performed. The cell showed an acceptable power output (at 800 °C, 0.35 W cm -2 with biogas, versus 0.55 W cm -2 with H 2) although a huge quantity of sulphur was present in the feeding fuel (hydrogen sulphide at 103 ppm and mercaptans up to 10 ppm). Therefore, it

  17. Methane-free biogas for direct feeding of solid oxide fuel cells

    Energy Technology Data Exchange (ETDEWEB)

    Leone, P.; Lanzini, A.; Santarelli, M.; Cali, M. [Dipartimento di Energetica, Politecnico di Torino, Corso Duca degli Abruzzi 24, 10129 Turin (Italy); Sagnelli, F.; Boulanger, A.; Scaletta, A.; Zitella, P. [BioEnergy Lab, Environment Park S.p.A., Via Livorno 60, 10144 Turin (Italy)

    2010-01-01

    This paper deals with the experimental analysis of the performance and degradation issues of a Ni-based anode-supported solid oxide fuel cell fed by a methane-free biogas from dark-anaerobic digestion of wastes by pastry and fruit shops. The biogas is produced by means of an innovative process where the biomass is fermented with a pre-treated bacteria inoculum (Clostridia) able to completely inhibit the methanization step during the fermentation process and to produce a H{sub 2}/CO{sub 2} mixture instead of conventional CH{sub 4}/CO{sub 2} anaerobic digested gas (bio-methane). The proposed biogas production route leads to a biogas composition which avoids the need of introducing a reformer agent into or before the SOFC anode in order to reformate it. In order to analyse the complete behaviour of a SOFC with the bio-hydrogen fuel, an experimental session with several H{sub 2}/CO{sub 2} synthetic mixtures was performed on an anode-supported solid oxide fuel cell with a Ni-based anode. It was found that side reactions occur with such mixtures in the typical thermodynamic conditions of SOFCs (650-800 C), which have an effect especially at high currents, due to the shift to a mixture consisting of hydrogen, carbon monoxide, carbon dioxide and water. However, cells operated with acceptable performance and carbon deposits (typical of a traditional hydrocarbon-containing biogas) were avoided after 50 h of cell operation even at 650 C. Experiments were also performed with traditional bio-methane from anaerobic digestion with 60/40 vol% of composition. It was found that the cell performance dropped after few hours of operation due to the formation of carbon deposits. A short-term test with the real as-produced biogas was also successfully performed. The cell showed an acceptable power output (at 800 C, 0.35 W cm{sup -2} with biogas, versus 0.55 W cm{sup -2} with H{sub 2}) although a huge quantity of sulphur was present in the feeding fuel (hydrogen sulphide at 103 ppm and

  18. A Metagenomics-Based Metabolic Model of Nitrate-Dependent Anaerobic Oxidation of Methane by Methanoperedens-Like Archaea

    Science.gov (United States)

    Arshad, Arslan; Speth, Daan R.; de Graaf, Rob M.; Op den Camp, Huub J. M.; Jetten, Mike S. M.; Welte, Cornelia U.

    2015-01-01

    Methane oxidation is an important process to mitigate the emission of the greenhouse gas methane and further exacerbating of climate forcing. Both aerobic and anaerobic microorganisms have been reported to catalyze methane oxidation with only a few possible electron acceptors. Recently, new microorganisms were identified that could couple the oxidation of methane to nitrate or nitrite reduction. Here we investigated such an enrichment culture at the (meta) genomic level to establish a metabolic model of nitrate-driven anaerobic oxidation of methane (nitrate-AOM). Nitrate-AOM is catalyzed by an archaeon closely related to (reverse) methanogens that belongs to the ANME-2d clade, tentatively named Methanoperedens nitroreducens. Methane may be activated by methyl-CoM reductase and subsequently undergo full oxidation to carbon dioxide via reverse methanogenesis. All enzymes of this pathway were present and expressed in the investigated culture. The genome of the archaeal enrichment culture encoded a variety of enzymes involved in an electron transport chain similar to those found in Methanosarcina species with additional features not previously found in methane-converting archaea. Nitrate reduction to nitrite seems to be located in the pseudoperiplasm and may be catalyzed by an unusual Nar-like protein complex. A small part of the resulting nitrite is reduced to ammonium which may be catalyzed by a Nrf-type nitrite reductase. One of the key questions is how electrons from cytoplasmically located reverse methanogenesis reach the nitrate reductase in the pseudoperiplasm. Electron transport in M. nitroreducens probably involves cofactor F420 in the cytoplasm, quinones in the cytoplasmic membrane and cytochrome c in the pseudoperiplasm. The membrane-bound electron transport chain includes F420H2 dehydrogenase and an unusual Rieske/cytochrome b complex. Based on genome and transcriptome studies a tentative model of how central energy metabolism of nitrate-AOM could work is

  19. Experimental Study and Mathematical Modeling of Self-Sustained Kinetic Oscillations in Catalytic Oxidation of Methane over Nickel.

    Science.gov (United States)

    Lashina, Elena A; Kaichev, Vasily V; Saraev, Andrey A; Vinokurov, Zakhar S; Chumakova, Nataliya A; Chumakov, Gennadii A; Bukhtiyarov, Valerii I

    2017-09-21

    The self-sustained kinetic oscillations in the oxidation of CH 4 over Ni foil have been studied at atmospheric pressure using an X-ray diffraction technique and mass spectrometry. It has been shown that the regular oscillations appear under oxygen-deficient conditions; CO, CO 2 , H 2 , and H 2 O are detected as the products. According to in situ X-ray diffraction measurements, nickel periodically oxidizes to NiO initiating the reaction-rate oscillations. To describe the oscillations, we have proposed a five-stage mechanism of the partial oxidation of methane over Ni and a corresponding three-variable kinetic model. The mechanism considers catalytic methane decomposition, dissociative adsorption of oxygen, transformation of chemisorbed oxygen to surface nickel oxide, and reaction of adsorbed carbon and oxygen species to form CO. Analysis of the kinetic model indicates that the competition of two processes, i.e., the oxidation and the carbonization of the catalyst surface, is the driving force of the self-sustained oscillations in the oxidation of methane. We have compared this mechanism with the detailed 18-stage mechanism described previously by Lashina et al. (Kinetics and Catalysis 2012, 53, 374-383). It has been shown that both kinetic mechanisms coupled with a continuous stirred-tank reactor model describe well the oscillatory behavior in the oxidation of methane under non-isothermal conditions.

  20. Macroscopic biofilms in fracture-dominated sediment that anaerobically oxidize methane

    Science.gov (United States)

    Briggs, B.R.; Pohlman, J.W.; Torres, M.; Riedel, M.; Brodie, E.L.; Colwell, F.S.

    2011-01-01

    Methane release from seafloor sediments is moderated, in part, by the anaerobic oxidation of methane (AOM) performed by consortia of archaea and bacteria. These consortia occur as isolated cells and aggregates within the sulfate-methane transition (SMT) of diffusion and seep-dominant environments. Here we report on a new SMT setting where the AOM consortium occurs as macroscopic pink to orange biofilms within subseafloor fractures. Biofilm samples recovered from the Indian and northeast Pacific Oceans had a cellular abundance of 10 7 to 10 8 cells cm -3. This cell density is 2 to 3 orders of magnitude greater than that in the surrounding sediments. Sequencing of bacterial 16S rRNA genes indicated that the bacterial component is dominated by Deltaproteobacteria, candidate division WS3, and Chloroflexi, representing 46%, 15%, and 10% of clones, respectively. In addition, major archaeal taxa found in the biofilm were related to the ANME-1 clade, Thermoplasmatales, and Desulfurococcales, representing 73%, 11%, and 10% of archaeal clones, respectively. The sequences of all major taxa were similar to sequences previously reported from cold seep environments. PhyloChip microarray analysis detected all bacterial phyla identified by the clone library plus an additional 44 phyla. However, sequencing detected more archaea than the PhyloChip within the phyla of Methanosarcinales and Desulfurococcales. The stable carbon isotope composition of the biofilm from the SMT (-35 to-43%) suggests that the production of the biofilm is associated with AOM. These biofilms are a novel, but apparently widespread, aggregation of cells represented by the ANME-1 clade that occur in methane-rich marine sediments. ?? 2011, American Society for Microbiology.

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

    Science.gov (United States)

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

    2015-12-01

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

  2. Conversion of Methane into Methanol and Ethanol over Nickel Oxide on Ceria-Zirconia Catalysts in a Single Reactor

    Energy Technology Data Exchange (ETDEWEB)

    Okolie, Chukwuemeka [School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive NW Atlanta GA 30332 USA; Belhseine, Yasmeen F. [School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive NW Atlanta GA 30332 USA; Lyu, Yimeng [School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive NW Atlanta GA 30332 USA; Yung, Matthew M. [National Renewable Energy Laboratory, Golden CO 80401 USA; Engelhard, Mark H. [Environmental Molecular Sciences Laboratory, Pacific Northwest National Lab, Richland WA 99354 USA; Kovarik, Libor [Environmental Molecular Sciences Laboratory, Pacific Northwest National Lab, Richland WA 99354 USA; Stavitski, Eli [National Synchrotron Light Source II, Brookhaven National Laboratory, Upton NY 11973 USA; Sievers, Carsten [School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, 311 Ferst Drive NW Atlanta GA 30332 USA

    2017-09-26

    Direct conversion of methane into alcohols is a promising technology for converting stranded methane reserves into liquids that can be transported in pipelines and upgraded to value-added chemicals. We demonstrate that a catalyst consisting of small nickel oxide clusters supported on ceria-zirconia (NiO/CZ) can selectively oxidize methane to methanol and ethanol in a single, steady-state process at 723 K using O2 as an abundantly available oxidant. The presence of steam is required to obtain alcohols rather than CO2 as the product of catalytic combustion. The unusual activity of this catalyst is attributed to the synergy between the small Lewis acidic NiO clusters and the redox-active CZ support, which also stabilizes the small NiO clusters.

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

    Science.gov (United States)

    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

  4. Methane evasion and oxidation in the Big Cypress National Preserve—a low relief carbonate wetland

    Science.gov (United States)

    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.

  5. Enhanced Emission Performance and Fuel Efficiency for HD Methane Engines. Literature Study. Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Broman, R.; Staalhammar, P.; Erlandsson, L.

    2010-05-15

    A literature survey has been conducted in order to define state-of-the-art for methane fuelled engines to be used in heavy duty vehicles. Use of methane can be favourable to increase security of supply and mitigate CO2 emissions, especially when the methane origins from biomass. Furthermore, methane used as a fuel in heavy duty engines has a potential to reduce toxic exhaust emissions. Historically, use of methane in heavy duty engines has often been hampered by poor efficiency, i.e. high fuel consumption when using the Otto-cycle. However, current generation technology engines might be within 5-10 % of the efficiency of Diesel engine technology. In this context it is worth mentioning that compliance-driven changes for meeting future emission regulations for Diesel engines may have a negative impact on fuel efficiency, thereby narrowing the gap. This may present an opportunity for heavy methane fuelled engines. The reliability and durability of the exhaust aftertreatment devices for methane fuelled engines has also given rise to some concerns. Some concepts are performing acceptable while others do not meet expectations. This is partly due to difficulties in handling methane in the aftertreatment device and partly to issues in the design of the ignition system. Methane is a fuel used worldwide and has a potential to be an important complement to Diesel oil. There are two categories of HD methane engines available to end-users: Retrofitted engines, which often include computer controlled retrofit systems developed as 'bolt-on' technologies that can be removed if necessary, to resell the vehicle with a normal diesel engine, and those developed specifically for and in conjunction with engine manufacturers and delivered to customers as factory-built engines or vehicles (OEM). Additionally, both these categories can include engines that use the Otto- or Diesel combustion cycles. When adapting a HD Diesel engine to run on methane there are two options, either

  6. Emissions of ammonia, nitrous oxide and methane during composting of organic household waste

    International Nuclear Information System (INIS)

    Gunnarsdotter Beck-Friis, Barbro

    2001-01-01

    In Sweden, composting of source-separated organic household waste is increasing, both domestically at the small-scale, and in larger municipal plants. Composting means a microbial decomposition of organic material, which results in the production of environmentally undesirable gases, such as ammonia (NH 3 ), nitrous oxide (N 2 O) and methane (CH 4 ). The aim of this thesis was to study the emissions of NH 3 , N 2 O and CH 4 to the atmosphere during composting of source-separated organic household waste. The studies were conducted in an experimental reactor under constant and controlled conditions and in municipal compost heaps. Emissions of NH 3 , N 2 O and CH 4 occurred at different phases during composting. Ammonia started to volatilise during the shift from mesophilic to thermophilic conditions when short-chained fatty acids were decomposed. Nitrous oxide was only emitted during the first days of composting and later during the cooling phase when nitrate was formed. Methane was only produced during the thermophilic phase. Large municipal compost heaps are a significant source for the production and emission of the greenhouse gases N 2 O and CH 4 . To avoid unwanted gaseous emissions to the atmosphere during composting, gaseous exchange with the atmosphere should be controlled in future composting plants

  7. Linking activity, composition and seasonal dynamics of atmospheric methane oxidizers in a meadow soil

    Science.gov (United States)

    Shrestha, Pravin Malla; Kammann, Claudia; Lenhart, Katharina; Dam, Bomba; Liesack, Werner

    2012-01-01

    Microbial oxidation is the only biological sink for atmospheric methane. We assessed seasonal changes in atmospheric methane oxidation and the underlying methanotrophic communities in grassland near Giessen (Germany), along a soil moisture gradient. Soil samples were taken from the surface layer (0–10 cm) of three sites in August 2007, November 2007, February 2008 and May 2008. The sites showed seasonal differences in hydrological parameters. Net uptake rates varied seasonally between 0 and 70 μg CH4 m−2 h−1. Greatest uptake rates coincided with lowest soil moisture in spring and summer. Over all sites and seasons, the methanotrophic communities were dominated by uncultivated methanotrophs. These formed a monophyletic cluster defined by the RA14, MHP and JR1 clades, referred to as upland soil cluster alphaproteobacteria (USCα)-like group. The copy numbers of pmoA genes ranged between 3.8 × 105–1.9 × 106 copies g−1 of soil. Temperature was positively correlated with CH4 uptake rates (P50 vol% and primarily related to members of the MHP clade. PMID:22189499

  8. Linking activity, composition and seasonal dynamics of atmospheric methane oxidizers in a meadow soil.

    Science.gov (United States)

    Shrestha, Pravin Malla; Kammann, Claudia; Lenhart, Katharina; Dam, Bomba; Liesack, Werner

    2012-06-01

    Microbial oxidation is the only biological sink for atmospheric methane. We assessed seasonal changes in atmospheric methane oxidation and the underlying methanotrophic communities in grassland near Giessen (Germany), along a soil moisture gradient. Soil samples were taken from the surface layer (0-10 cm) of three sites in August 2007, November 2007, February 2008 and May 2008. The sites showed seasonal differences in hydrological parameters. Net uptake rates varied seasonally between 0 and 70 μg CH(4) m(-2) h(-1). Greatest uptake rates coincided with lowest soil moisture in spring and summer. Over all sites and seasons, the methanotrophic communities were dominated by uncultivated methanotrophs. These formed a monophyletic cluster defined by the RA14, MHP and JR1 clades, referred to as upland soil cluster alphaproteobacteria (USCα)-like group. The copy numbers of pmoA genes ranged between 3.8 × 10(5)-1.9 × 10(6) copies g(-1) of soil. Temperature was positively correlated with CH(4) uptake rates (P50 vol% and primarily related to members of the MHP clade.

  9. Effect of inoculum sources on the enrichment of nitrite-dependent anaerobic methane-oxidizing bacteria.

    Science.gov (United States)

    He, Zhanfei; Cai, Chen; Shen, Lidong; Lou, Liping; Zheng, Ping; Xu, Xinhua; Hu, Baolan

    2015-01-01

    Nitrite-dependent anaerobic methane oxidation (n-damo) is a newly discovered biological process that couples anaerobic oxidation of methane (AOM) to nitrite reduction. In this study, three different inocula, methanogenic sludge, paddy soil, and freshwater sediment were used to enrich n-damo bacteria in three sequencing batch reactors (SBRs), and three n-damo enrichment cultures, C1, C2 and C3, were obtained, respectively. After 500 days of incubation, Methylomirabilis oxyfera-like bacteria and n-damo activities were observed in cultures C1, C2, and C3, and the specific activities were 0.8 ± 0.1, 1.4 ± 0.1, and 1.0 ± 0.1 μmol CH4 h(-1) g(-1) VSS, respectively. The copy numbers of 16S rRNA genes from cultures C1, C2, and C3 were 5.0 ± 0.4 × 10(8), 6.1 ± 0.1 × 10(9), and 1.0 ± 0.2 × 10(9) copies g(-1) dry weight, respectively. The results indicated that paddy soil is an excellent inoculum for n-damo bacterial enrichment. This work expanded the alternative source of n-damo inoculum and benefited the further research of n-damo process.

  10. Partial oxidation of methane to methanol over catalyst ZSM-5 from coal fly ash and rice husk ash

    Directory of Open Access Journals (Sweden)

    Mirda Yanti Fusia

    2017-01-01

    Full Text Available Methane is one of the greenhouse gases that can be converted into liquid fuels such as methanol to retain most of the energy of methane and produce a cleaner environment. The conversion of methane to methanol using ZMS-5 represents a breakthrough in the utilization of methane. However, material sources for zeolite synthesis as catalyst usually are pro-analysis grade materials, which are expensive. Therefore, in this research, coal fly ash and rice husk ash were used as raw materials for mesoporous ZSM-5 zeolite synthesis. First, coal fly ash and rice husk were subjected to pre-treatment to extract silicate (SiO44− and aluminate (AlO45− and impurities separation. The ZSM-5 zeolite was synthesized through hydrothermal treatment using two types of templates. After ZSM-5 was synthesized, it was modified with Cobalt through impregnation method. The catalytic activity of both ZSM-5 and Co/ZSM-5 zeolites as heterogeneous catalysts in partial oxidation of methane were preliminary tested and compared with that commercial one. The result showed that the zeolite catalyst ZSM-5 from fly ash coal and rice husk ash has the potential to be used as catalysts in the partial oxidation of methane to methanol.

  11. LANDFILL OPERATION FOR CARBON SEQUESTRATION AND MAXIMUM METHANE EMISSION CONTROL; FINAL

    International Nuclear Information System (INIS)

    Don Augenstein; Ramin Yazdani; Rick Moore; Michelle Byars; Jeff Kieffer; Professor Morton Barlaz; Rinav Mehta

    2000-01-01

    Controlled landfilling is an approach to manage solid waste landfills, so as to rapidly complete methane generation, while maximizing gas capture and minimizing the usual emissions of methane to the atmosphere. With controlled landfilling, methane generation is accelerated to more rapid and earlier completion to full potential by improving conditions (principally moisture, but also temperature) to optimize biological processes occurring within the landfill. Gas is contained through use of surface membrane cover. Gas is captured via porous layers, under the cover, operated at slight vacuum. A field demonstration project has been ongoing under NETL sponsorship for the past several years near Davis, CA. Results have been extremely encouraging. Two major benefits of the technology are reduction of landfill methane emissions to minuscule levels, and the recovery of greater amounts of landfill methane energy in much shorter times, more predictably, than with conventional landfill practice. With the large amount of US landfill methane generated, and greenhouse potency of methane, better landfill methane control can play a substantial role both in reduction of US greenhouse gas emissions and in US renewable energy. The work described in this report, to demonstrate and advance this technology, has used two demonstration-scale cells of size (8000 metric tons[tonnes]), sufficient to replicate many heat and compaction characteristics of larger ''full-scale'' landfills. An enhanced demonstration cell has received moisture supplementation to field capacity. This is the maximum moisture waste can hold while still limiting liquid drainage rate to minimal and safely manageable levels. The enhanced landfill module was compared to a parallel control landfill module receiving no moisture additions. Gas recovery has continued for a period of over 4 years. It is quite encouraging that the enhanced cell methane recovery has been close to 10-fold that experienced with conventional

  12. Biomarker evidence for widespread anaerobic methane oxidation in Mediterranean sediments by a consortium of methanogenic archaea and bacteria : The Medinaut Shipboard Scientific Party

    NARCIS (Netherlands)

    Pancost, Richard D.; Sinninghe Damsté, Jaap S.; de Lint, Saskia; van der Maarel, Marc J.E.C.; Gottschal, JC

    Although abundant geochemical data indicate that anaerobic methane oxidation occurs in marine sediments, the linkage to specific microorganisms remains unclear, In order to examine processes of methane consumption and oxidation, sediment samples from mud volcanoes at two distinct sites on the

  13. Dynamic changes of carbon isotope apparent fractionation factor to describe transition to syntrophic acetate oxidation during cellulose and acetate methanization.

    Science.gov (United States)

    Vavilin, Vasily A; Rytov, Sergey V

    2017-05-01

    To identify predominant metabolic pathway for cellulose methanization new equations that take into account dynamics of 13C are added to the basic model of cellulose methanization. The correct stoichiometry of hydrolysis, acidogenesis, acetogenesis and methanogenesis steps including biomass is considered. Using experimental data by Laukenmann et al. [Identification of methanogenic pathway in anaerobic digesters using stable carbon isotopes. Eng. Life Sci. 2010;10:1-6], who reported about the importance of ace`tate oxidation during mesophilic cellulose methanization, the model confirmed that, at high biomass concentration of acetate oxidizers, the carbon isotope fractionation factor amounts to about 1.085. The same model, suggested firstly for cellulose degradation, was used to describe, secondly, changes in, and in methane and carbon dioxide during mesophylic acetate methanization measured by Grossin-Debattista [Fractionnements isotopiques (13C/12C) engendres par la methanogenese: apports pour la comprehension des processus de biodegradation lors de la digestion anaerobie [doctoral thesis]. 2011. Bordeaux: Universite Bordeaux-1;2011. Available from: http://ori-oai.u-bordeaux1.fr/pdf/2011/GROSSIN-DEBATTISTA_JULIEN_2011.pdf . French].The model showed that under various ammonium concentrations, at dominating acetoclastic methanogenesis, the value decreases over time to a low level (1.016), while at dominating syntrophic acetate oxidation, coupled with hydrogenotrophic methanogenesis, slightly increases, reaching 1.060 at the end of incubation.

  14. Methane oxidation with low O2/CH4 ratios in the present of water: Combustion or reforming

    International Nuclear Information System (INIS)

    Geng, Haojie; Yang, Zhongqing; Zhang, Li; Ran, Jingyu; Yan, Yunfei

    2017-01-01

    Highlights: • Copper catalyst displays an inhibitory effect of water while cobalt catalyst does not. • Both catalysts show their catalytic ability for oxidation and reforming reaction. • Oxidation precedes reforming in methane reaction over both catalysts. • Water participates in reforming reaction and shows increasing effect in high temperature. - Abstract: This paper investigates the reaction of methane over copper and cobalt catalysts under oxygen-deficient conditions with added water. A fixed-bed reactor, TPD analysis, in situ DRIFTS study, and temperature detection were used to test the activity of the methane reaction, water adsorption on the metal surface, OH group behavior, and the endothermic and exothermic processes of the reaction. The results show that the inhibitory effect of water mainly occurs at a low temperature and methane conversion decreases when water is introduced into the feed. Water easily adsorbs on metal clusters and forms OH groups at low temperatures. Copper tends to adsorb more water than cobalt and shows a stronger inhibitory effect. The DRIFTS spectra of the Cu catalyst show strong OH peaks during the reaction, of which the magnitudes increase with the water pressure. When the reaction temperature rises (750 °C), water begins to serve as an oxidant and participates in the reforming reaction. Both catalysts show a transition process between the oxidation and reforming reactions as the temperature increases. Co displays a better catalytic performance in the reforming reaction. Oxidation precedes reforming; water does not participate in the reaction if the oxygen is not fully consumed.

  15. A transient kinetic study of nickel-catalyzed methanation: Final report

    International Nuclear Information System (INIS)

    Hoost, T.E.; Goodwin, J.G. Jr.

    1988-11-01

    The results of this study are in two major parts. In Part I the use of steady-state isotopic transients of multiple elements (C, H, and O) under actual methanation reaction conditions has permitted an assessment of the reactivity of water on a Ni powder catalyst. It was concluded based on the addition of isotopic water that oxygen, once reacted to form water, is able to readsorb even where the surface coverage of CO remains high. At the low relative partial pressures of water used, however, there was no effect of added water on the formation of methane. The surface residence time of water determined from isotopic transients contains the residence time on the surface during the primary formation reaction as well as the time spent during readsorption(s). Part II addressed how a catalyst modifier (in this case Cl) affects methanation in CO hydrogenation using steady-state isotopic transient kinetic analysis (SSITKA) of methanation. The results obtained using silica-supported Ru suggest the structural rearrangements induced by the presence of chlorine, rather than selective site blocking or electronic interactions, may be the primary mechanism of chlorine modification of the catalytic properties of supported metals for CO hydrogenation. SSITKA indicated that the decrease in methanation activity with increasing initial Cl concentration was a function of a decrease in the number of reactive surface intermediates (or sites) and not of a change in site activity. 36 refs., 10 figs., 5 tabs

  16. Immunological detection of enzymes for sulfate reduction in anaerobic methane-oxidizing consortia.

    Science.gov (United States)

    Milucka, Jana; Widdel, Friedrich; Shima, Seigo

    2013-05-01

    Anaerobic oxidation of methane (AOM) coupled to sulfate reduction (SR) at marine gas seeps is performed by archaeal-bacterial consortia that have so far not been cultivated in axenic binary or pure cultures. Knowledge about possible biochemical reactions in AOM consortia is based on metagenomic retrieval of genes related to those in archaeal methanogenesis and bacterial sulfate reduction, and identification of a few catabolic enzymes in protein extracts. Whereas the possible enzyme for methane activation (a variant of methyl-coenzyme M reductase, Mcr) was shown to be harboured by the archaea, enzymes for sulfate activation and reduction have not been localized so far. We adopted a novel approach of fluorescent immunolabelling on semi-thin (0.3-0.5 μm) cryosections to localize two enzymes of the SR pathway, adenylyl : sulfate transferase (Sat; ATP sulfurylase) and dissimilatory sulfite reductase (Dsr) in microbial consortia from Black Sea methane seeps. Both Sat and Dsr were exclusively found in an abundant microbial morphotype (c. 50% of all cells), which was tentatively identified as Desulfosarcina/Desulfococcus-related bacteria. These results show that ANME-2 archaea in the Black Sea AOM consortia did not express bacterial enzymes of the canonical sulfate reduction pathway and thus, in contrast to previous suggestions, most likely cannot perform canonical sulfate reduction. Moreover, our results show that fluorescent immunolabelling on semi-thin cryosections which to our knowledge has been so far only applied on cell tissues, is a powerful tool for intracellular protein detection in natural microbial associations. © 2012 Society for Applied Microbiology and Blackwell Publishing Ltd.

  17. Effect of biomass concentration on methane oxidation activity using mature compost and graphite granules as substrata.

    Science.gov (United States)

    Xie, S; O'Dwyer, T; Freguia, S; Pikaar, I; Clarke, W P

    2016-10-01

    Reported methane oxidation activity (MOA) varies widely for common landfill cover materials. Variation is expected due to differences in surface area, the composition of the substratum and culturing conditions. MOA per methanotrophic cell has been calculated in the study of natural systems such as lake sediments to examine the inherent conditions for methanotrophic activity. In this study, biomass normalised MOA (i.e., MOA per methanotophic cell) was measured on stabilised compost, a commonly used cover in landfills, and on graphite granules, an inert substratum widely used in microbial electrosynthesis studies. After initially enriching methanotrophs on both substrata, biomass normalised MOA was quantified under excess oxygen and limiting methane conditions in 160ml serum vials on both substrata and blends of the substrata. Biomass concentration was measured using the bicinchoninic acid assay for microbial protein. The biomass normalised MOA was consistent across all compost-to-graphite granules blends, but varied with time, reflecting the growth phase of the microorganisms. The biomass normalised MOA ranged from 0.069±0.006μmol CH4/mg dry biomass/h during active growth, to 0.024±0.001μmol CH4/mg dry biomass/h for established biofilms regardless of the substrata employed, indicating the substrata were equally effective in terms of inherent composition. The correlation of MOA with biomass is consistent with studies on methanotrophic activity in natural systems, but biomass normalised MOA varies by over 5 orders of magnitude between studies. This is partially due to different methods being used to quantify biomass, such as pmoA gene quantification and the culture dependent Most Probable Number method, but also indicates that long term exposure of materials to a supply of methane in an aerobic environment, as can occur in natural systems, leads to the enrichment and adaptation of types suitable for those conditions. Copyright © 2016 Elsevier Ltd. All rights

  18. Methane oxidation in a landfill cover soil reactor: Changing of kinetic parameters and microorganism community structure.

    Science.gov (United States)

    Xing, Zhi L; Zhao, Tian T; Gao, Yan H; Yang, Xu; Liu, Shuai; Peng, Xu Y

    2017-02-23

    Changing of CH 4 oxidation potential and biological characteristics with CH 4 concentration was studied in a landfill cover soil reactor (LCSR). The maximum rate of CH 4 oxidation reached 32.40 mol d -1 m -2 by providing sufficient O 2 in the LCSR. The kinetic parameters of methane oxidation in landfill cover soil were obtained by fitting substrate diffusion and consumption model based on the concentration profile of CH 4 and O 2 . The values of [Formula: see text] (0.93-2.29%) and [Formula: see text] (140-524 nmol kg soil-DW -1 ·s -1 ) increased with CH 4 concentration (9.25-20.30%), while the values of [Formula: see text] (312.9-2.6%) and [Formula: see text] (1.3 × 10 -5 to 9.0 × 10 -3 nmol mL -1 h -1 ) were just the opposite. MiSeq pyrosequencing data revealed that Methylobacter (the relative abundance was decreased with height of LCSR) and Methylococcales_unclassified (the relative abundance was increased expect in H 80) became the key players after incubation with increasing CH 4 concentration. These findings provide information for assessing CH 4 oxidation potential and changing of biological characteristics in landfill cover soil.

  19. Methane Emissions from Landfill: Isotopic Evidence for Low Percentage of Oxidation from Gas Wells, Active and Closed Cells

    Science.gov (United States)

    Lowry, David; Fisher, Rebecca; Zazzeri, Giulia; al-Shalaan, Aalia; France, James; Lanoisellé, Mathias; Nisbet, Euan

    2017-04-01

    Large landfill sites remain a significant source of methane emissions in developed and developing countries, with a global estimated flux of 29 Tg / yr in the EDGAR 2008 database. This is significantly lower than 20 years ago due to the introduction of gas extraction systems, but active cells still emit significant amounts of methane before the gas is ready for extraction. Historically the methane was either passively oxidized through topsoil layers or flared. Oxidation is still the primary method of methane removal in many countries, and covered, remediated cells across the world continue to emit small quantities of methane. The isotopic signatures of methane from landfill gas wells, and that emitted from active and closed cells have been characterized for more than 20 UK landfills since 2011, with more recent work in Kuwait and Hong Kong. Since 2013 the emission plumes have been identified by a mobile measurement system (Zazzeri et al., 2015). Emissions in all 3 countries have a characteristic δ13C signature of -58 ± 3 ‰ dominated by emissions from the active cells, despite the hot, dry conditions of Kuwait and the hot, humid conditions of Hong Kong. Gas well samples define a similar range. Surface emissions from closed cells and closed landfills are mostly in the range -56 to -52 ‰Ṫhese are much more depleted values than those observed in the 1990s (up to -35 ) when soil oxidation was the dominant mechanism of methane removal. Calculations using isotopic signatures of the amount of methane oxidised in these closed areas before emission to atmosphere range from 5 to 15%, but average less than 10%, and are too small to calculate from the high-emitting active cells. Compared to other major methane sources, landfills have the most consistent isotopic signature globally, and are distinct from the more 13C-enriched natural gas, combustion and biomass burning sources. Zazzeri, G. et al. (2015) Plume mapping and isotopic characterization of anthropogenic methane

  20. Membranes for corrosive oxidations. Final CRADA report.

    Energy Technology Data Exchange (ETDEWEB)

    Snyder, S. W.; Energy Systems

    2010-02-01

    The objective of this project is to develop porous hydrophilic membranes that are highly resistant to oxidative and corrosive conditions and to deploy them for recovery and purification of high tonnage chemicals such as hydrogen peroxide and other oxychemicals. The research team patented a process for membrane-based separation of hydrogen peroxide (US Patent No. 5,662,878). The process is based on using a hydrophilic membrane to separate hydrogen peroxide from the organic working solution. To enable this process, a new method for producing hydrophilic membrane materials (Patent No.6,464,880) was reported. We investigated methods of producing these hydrophilic materials and evaluated separations performance in comparison to membrane stability. It was determined that at the required membrane flux, membrane stability was not sufficient to design a commercial process. This work was published (Hestekin et al., J. Membrane Science 2006). To meet the performance needs of the process, we developed a membrane contactor method to extract the hydrogen peroxide, then we surveyed several commercial and pre-commercial membrane materials. We identified pre-commercial hydrophilic membranes with the required selectivity, flux, and stability to meet the needs of the process. In addition, we invented a novel reaction/separations format that greatly increases the performance of the process. To test the performance of the membranes and the new formats we procured and integrated reactor/membrane separations unit that enables controlled mixing, flow, temperature control, pressure control, and sampling. The results were used to file a US non-provisional patent application (ANL-INV 03-12). Hydrogen peroxide is widely used in pulp and paper applications, environmental treatment, and other industries. Virtually all hydrogen peroxide production is now based on a process featuring catalytic hydrogenation followed by auto-oxidation of suitable organic carrier molecules. This process has several

  1. Methane and nitrous oxide emissions from a subtropical estuary (the Brisbane River estuary, Australia)

    Energy Technology Data Exchange (ETDEWEB)

    Musenze, Ronald S.; Werner, Ursula [Advanced Water Management Centre (AWMC), the University of Queensland, Brisbane, Qld 4072 (Australia); Grinham, Alistair [Advanced Water Management Centre (AWMC), the University of Queensland, Brisbane, Qld 4072 (Australia); School of Civil Engineering, the University of Queensland, Brisbane, Qld 4072 (Australia); Udy, James [Healthy Waterways Ltd, P.O. Box 13086, George Street, Brisbane, Qld 4003 (Australia); Yuan, Zhiguo, E-mail: z.yuan@awmc.uq.edu.au [Advanced Water Management Centre (AWMC), the University of Queensland, Brisbane, Qld 4072 (Australia)

    2014-02-01

    Methane (CH{sub 4}) and nitrous oxide (N{sub 2}O) are two key greenhouse gases. Their global atmospheric budgeting is, however, flout with challenges partly due to lack of adequate field studies determining the source strengths. Knowledge and data limitations exist for subtropical and tropical regions especially in the southern latitudes. Surface water methane and nitrous oxide concentrations were measured in a subtropical estuarine system in the southern latitudes in an extensive field study from 2010 to 2012 and water–air fluxes estimated using models considering the effects of both wind and flow induced turbulence. The estuary was found to be a strong net source of both CH{sub 4} and N{sub 2}O all-year-round. Dissolved N{sub 2}O concentrations ranged between 9.1 ± 0.4 to 45.3 ± 1.3 nM or 135 to 435% of atmospheric saturation level, while CH{sub 4} concentrations varied between 31.1 ± 3.7 to 578.4 ± 58.8 nM or 1210 to 26,430% of atmospheric saturation level. These results compare well with measurements from tropical estuarine systems. There was strong spatial variability with both CH{sub 4} and N{sub 2}O concentrations increasing upstream the estuary. Strong temporal variability was also observed but there were no clear seasonal patterns. The degree of N{sub 2}O saturation significantly increased with NO{sub x} concentrations (r{sup 2} = 0.55). The estimated water–air fluxes varied between 0.1 and 3.4 mg N{sub 2}O m{sup −2} d{sup −1} and 0.3 to 27.9 mg CH{sub 4} m{sup −2} d{sup −1}. Total emissions (CO{sub 2}-e) were N{sub 2}O (64%) dominated, highlighting the need for reduced nitrogen inputs into the estuary. Choice of the model(s) for estimation of the gas transfer velocity had a big bearing on the estimated total emissions. - Highlights: • The estuary is a strong source of atmospheric methane and nitrous oxide. • Emissions had strong spatial-temporal variability with unclear seasonal patterns. • Dissolved gas saturation comparable to that

  2. Methane and nitrous oxide emissions from a subtropical estuary (the Brisbane River estuary, Australia)

    International Nuclear Information System (INIS)

    Musenze, Ronald S.; Werner, Ursula; Grinham, Alistair; Udy, James; Yuan, Zhiguo

    2014-01-01

    Methane (CH 4 ) and nitrous oxide (N 2 O) are two key greenhouse gases. Their global atmospheric budgeting is, however, flout with challenges partly due to lack of adequate field studies determining the source strengths. Knowledge and data limitations exist for subtropical and tropical regions especially in the southern latitudes. Surface water methane and nitrous oxide concentrations were measured in a subtropical estuarine system in the southern latitudes in an extensive field study from 2010 to 2012 and water–air fluxes estimated using models considering the effects of both wind and flow induced turbulence. The estuary was found to be a strong net source of both CH 4 and N 2 O all-year-round. Dissolved N 2 O concentrations ranged between 9.1 ± 0.4 to 45.3 ± 1.3 nM or 135 to 435% of atmospheric saturation level, while CH 4 concentrations varied between 31.1 ± 3.7 to 578.4 ± 58.8 nM or 1210 to 26,430% of atmospheric saturation level. These results compare well with measurements from tropical estuarine systems. There was strong spatial variability with both CH 4 and N 2 O concentrations increasing upstream the estuary. Strong temporal variability was also observed but there were no clear seasonal patterns. The degree of N 2 O saturation significantly increased with NO x concentrations (r 2 = 0.55). The estimated water–air fluxes varied between 0.1 and 3.4 mg N 2 O m −2 d −1 and 0.3 to 27.9 mg CH 4 m −2 d −1 . Total emissions (CO 2 -e) were N 2 O (64%) dominated, highlighting the need for reduced nitrogen inputs into the estuary. Choice of the model(s) for estimation of the gas transfer velocity had a big bearing on the estimated total emissions. - Highlights: • The estuary is a strong source of atmospheric methane and nitrous oxide. • Emissions had strong spatial-temporal variability with unclear seasonal patterns. • Dissolved gas saturation comparable to that in tropical rivers and polluted estuaries. • Emissions are dominated by N2O, which

  3. Molecular isotopic evidence for anaerobic oxidation of methane in deep-sea hydrothermal vent environment in Okinawa Trough

    Science.gov (United States)

    Uchida, M.; Takai, K.; Inagaki, F.

    2003-04-01

    Large amount of methane in anoxic marine sediments as well as cold seeps and hydrothermal vents is recycled through for an anoxic oxidation of methane processes. Now that combined results of field and laboratory studies revealed that microbiological activity associated with syntrophic consortium of archaea performing reversed methanogenesis and sulfate-reducing bacteria is significant roles in methane recycling, anaerobic oxidation of methane (AOM). In this study, we examined the diversity of archaeal and bacterial assemblages of AOM using compound-specific stable carbon isotopic and phylogenetic analyses. "Iheya North" in Okinawa Trough is sediment-rich, back arc type hydrothermal system (27^o47'N, 126^o53'E). Sediment samples were collected from three sites where are "bubbling sites", yellow-colored microbial mats are formed with continuous bubbling from the seafloor bottom, vent mussel's colonies site together with slowly venting and simmering, and control site off 100 m distance from thermal vent. This subsea floor structure has important effect in the microbial ecosystem and interaction between their activity and geochemical processes in the subseafloor habitats. Culture-independent, molecular biological analysis clearly indicated the presence of thermophilic methanogens in deeper area having higher temperatures and potential activity of AMOs consortium in the shallower area. AMO is composed with sulfate-reducing bacterial components (Desulfosarcina spp.) and anoxic methane oxidizing archaea (ANME-2). These results were consistent with the results of compound-specific carbon analysis of archaeal biomarkers. They showed extremely depleted 13C contents (-80 ppm ˜ -100 ppm), which also appeared to be capable of directly oxidizing methane.

  4. Quantifying the percentage of methane formation via acetoclastic and syntrophic acetate oxidation pathways in anaerobic digesters.

    Science.gov (United States)

    Jiang, Ying; Banks, Charles; Zhang, Yue; Heaven, Sonia; Longhurst, Philip

    2018-01-01

    Ammonia concentration is one of the key factors influencing the methanogenic community composition and dominant methanogenic pathway in anaerobic digesters. This study adopted a radiolabelling technique using [2- 14 C] acetate to investigate the relationship between total ammonia nitrogen (TAN) and the methanogenic pathway. The radiolabelling experiments determined the ratio of 14 CO 2 and 14 CH 4 in the biogas which was used to quantitatively determine the percentage of CH 4 derived from acetoclastic and syntrophic acetate oxidation routes, respectively. This technique was performed on a selection of mesophilic digesters representing samples of low to high TAN concentrations (0.2-11.1gkg -1 wet weight). In high TAN digesters, the ratio between 14 CO 2 and 14 CH 4 was in the range 2.1-3.0; indicating 68-75% of methane was produced via the hydrogenotrophic route; whereas in low ammonia samples the ratio was 0.1-0.3, indicating 9-23% of methane was produced by the hydrogenotrophic route. These findings have been confirmed further by phylogenetic studies. Copyright © 2017. Published by Elsevier Ltd.

  5. A Singular Perturbation Problem for Steady State Conversion of Methane Oxidation in Reverse Flow Reactor

    Directory of Open Access Journals (Sweden)

    Aang Nuryaman

    2012-11-01

    Full Text Available The governing equations describing the methane oxidation process in reverse flow reactor are given by a set of convective-diffusion equations with a nonlinear reaction term, where temperature and methane conversion are dependent variables. In this study, the process is assumed to be one-dimensional pseudo homogeneous model and takes place with a certain reaction rate in which the whole process of reactor is still workable. Thus, the reaction rate can proceed at a fixed temperature. Under this condition, we restrict ourselves to solve the equations for the conversion only. From the available data, it turns out that the ratio of the diffusion term to the reaction term is small. Hence, this ratio is considered as small parameter in our model and this leads to a singular perturbation problem. In the vicinity of small parameter in front of higher order term, the numerical difficulties will be found. Here, we present an analytical solution by means of matched asymptotic expansions. Result shows that, up to and including the first order of approximation, the solution is in agreement with the exact and numerical solutions of the boundary value problem.

  6. Investigation of methane steam reforming in planar porous support of solid oxide fuel cell

    International Nuclear Information System (INIS)

    Yang Yongping; Du Xiaoze; Yang Lijun; Huang Yuan; Xian Haizhen

    2009-01-01

    Adopting the porous support in integrated-planar solid oxide fuel cell (IP-SOFC) can reduce the operating temperature by reducing thickness of electrolyte layer, and also, provide internal reforming environment for hydrogen-rich fuel gas. The distributions of reactant and product components, and temperature of methane steam reforming for IP-SOFC were investigated by the developed physical and mathematical model with thermodynamic analysis, in which eleven possible reaction mechanisms were considered by the source terms and Arrhenius relationship. Numerical simulation of the model revealed that the progress of reforming reaction and the distribution of the product, H 2 , were influenced by the operating conditions, included that of temperature, ratio of H 2 O and CH 4 , as well as by the porosity of the supporting material. The simulating results indicate that the methane conversion rate can reach its maximum value under the operating temperature of 800 deg. C and porosity of ε = 0.4, which rather approximate to the practical operating conditions of IP-SOFC. In addition, characteristics of carbon deposition on surface of catalyst were discussed under various operating conditions and configuration parameters of the porous support. The present works provided some theoretical explanations to the numerous experimental observations and engineered practices

  7. Methane Oxidation to Methanol Catalyzed by Cu-Oxo Clusters Stabilized in NU-1000 Metal-Organic Framework.

    Science.gov (United States)

    Ikuno, Takaaki; Zheng, Jian; Vjunov, Aleksei; Sanchez-Sanchez, Maricruz; Ortuño, Manuel A; Pahls, Dale R; Fulton, John L; Camaioni, Donald M; Li, Zhanyong; Ray, Debmalya; Mehdi, B Layla; Browning, Nigel D; Farha, Omar K; Hupp, Joseph T; Cramer, Christopher J; Gagliardi, Laura; Lercher, Johannes A

    2017-08-02

    Copper oxide clusters synthesized via atomic layer deposition on the nodes of the metal-organic framework (MOF) NU-1000 are active for oxidation of methane to methanol under mild reaction conditions. Analysis of chemical reactivity, in situ X-ray absorption spectroscopy, and density functional theory calculations are used to determine structure/activity relations in the Cu-NU-1000 catalytic system. The Cu-loaded MOF contained Cu-oxo clusters of a few Cu atoms. The Cu was present under ambient conditions as a mixture of ∼15% Cu + and ∼85% Cu 2+ . The oxidation of methane on Cu-NU-1000 was accompanied by the reduction of 9% of the Cu in the catalyst from Cu 2+ to Cu + . The products, methanol, dimethyl ether, and CO 2 , were desorbed with the passage of 10% water/He at 135 °C, giving a carbon selectivity for methane to methanol of 45-60%. Cu oxo clusters stabilized in NU-1000 provide an active, first generation MOF-based, selective methane oxidation catalyst.

  8. Methane oxidation in soil profiles of Dutch and Finnish coniferous forests with different soil texture and atmospheric nitrogen deposition

    NARCIS (Netherlands)

    Saari, A.; Martikainen, P.J.; Ferm, A.; Ruuskanen, J.; Boer, W. de; Troelstra, S.R.; Laanbroek, H.J.

    1997-01-01

    We studied methane oxidation capacity in soil profiles of Dutch and Finnish coniferous forests. The Finnish sites (n = 9) had nitrogen depositions from 3 to 36 kg N ha⁻¹ a⁻¹. The deposition of N on the Dutch sites (n = 13) was higher ranging from 50 to 92 kg N ha⁻¹ a⁻¹. The Dutch sites had also

  9. Methane oxidation in soil profiles of Dutch and Finnish coniferous forests with different soil texture and atmospheric nitrogen deposition

    NARCIS (Netherlands)

    Saari, A.; Martikainen, P.J.; Ferm, A.; Ruuskanen, J.; De Boer, W.; Troelstra, S.R.; Laanbroek, H.J.

    1997-01-01

    We studied methane oxidation capacity in soil profiles of Dutch and Finnish coniferous forests. The Finnish sites (n = 9) had nitrogen depositions from 3 to 36 kg N ha(-1) a(-1). The deposition of N on the Dutch sites (n = 13) was higher ranging from 50 to 92 kg N ha(-1) a(-1). The Dutch sites had

  10. More evidence that anaerobic oxidation of methane is prevalent in soils: Is it time to upgrade our biogeochemical models?

    Czech Academy of Sciences Publication Activity Database

    Gauthier, M.; Bradley, R.L.; Šimek, Miloslav

    2015-01-01

    Roč. 80, January (2015), s. 167-174 ISSN 0038-0717 R&D Projects: GA ČR GA526/09/1570 Institutional support: RVO:60077344 Keywords : anaerobic oxidation of methane * isotope dilution * peatland soil * shoreline soil * acid sulfate soil * alternative electron acceptors Subject RIV: EH - Ecology, Behaviour Impact factor: 4.152, year: 2015

  11. Wood ant nests as hot spots of carbon dioxide production and cold spots of methane oxidation in temperate forests

    Czech Academy of Sciences Publication Activity Database

    Jílková, Veronika; Picek, T.; Cajthaml, Tomáš; Frouz, Jan

    2016-01-01

    Roč. 18, April (2016), EGU2016-4634 ISSN 1607-7962. [European Geosciences Union General Assembly 2016. 17.04.2016-22.04.2016, Vienna] Institutional support: RVO:60077344 ; RVO:61388971 Keywords : wood ant nests * hot spots of carbon dioxide production * cold spots of methane oxidation * temperate forests Subject RIV: DF - Soil Science

  12. Effect of surface composition of yttrium-stabilized zirconia on partial oxidation of methane to synthesis gas.

    NARCIS (Netherlands)

    Zhu, J.J.; van Ommen, J.G.; Knoester, A.; Lefferts, Leonardus

    2005-01-01

    Catalytic partial oxidation of methane to synthesis gas (CPOM) over yttrium-stabilized zirconia (YSZ) was studied within a wide temperature window (500¿1100 °C). The catalysts were characterized by X-ray fluorescence (XRF) and low-energy ion scattering (LEIS). The influence of calcination

  13. Mitigation of methane and nitrous oxide emissions from animal operations: II. A review of manure management mitigation options

    NARCIS (Netherlands)

    Montes, F.; Meinen, R.; Dell, C.; Rotz, A.; Hristov, A.N.; Oh, J.; Waghorn, G.; Gerber, P.J.; Henderson, B.L.; Makkar, H.P.S.; Dijkstra, J.

    2013-01-01

    This review analyzes published data on manure management practices used to mitigate methane (CH4) and nitrous oxide (N2O) emissions from animal operations. Reducing excreted nitrogen (N) and degradable organic carbon (C) by diet manipulation to improve the balance of nutrient inputs with production

  14. Measurements and modeling to quantify emissions of methane and VOCs from shale gas operations: Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Presto, Albert A [Carnegie Mellon Univ., Pittsburgh, PA (United States)

    2017-06-30

    The objectives of the project were to determine the leakage rates of methane and ozone-forming Volatile Organic Compounds (VOCs) and the emission rates of air toxics from Marcellus shale gas activities. Methane emissions in the Marcellus Shale region were differentiated between “newer” sources associated with shale gas development and “older” sources associated with coal or conventional natural gas exploration. This project conducted measurements of methane and VOC emissions from both shale and non-shale natural gas resources. The initial scope of the project was the Marcellus Shale basin, and measurements were conducted in both the western wet gas regions (southwest PA and WV) and eastern dry gas region (northeast PA) of the basin. During this project, we obtained additional funding from other agencies to expand the scope of measurements to include additional basins. The data from both the Marcellus and other basins were combined to construct a national analysis of methane emissions from oil & gas production activities.

  15. Composition of methane-oxidizing bacterial communities as a function of nutrient loading in the Florida everglades.

    Science.gov (United States)

    Chauhan, Ashvini; Pathak, Ashish; Ogram, Andrew

    2012-10-01

    Agricultural runoff of phosphorus (P) in the northern Florida Everglades has resulted in several ecosystem level changes, including shifts in the microbial ecology of carbon cycling, with significantly higher methane being produced in the nutrient-enriched soils. Little is, however, known of the structure and activities of methane-oxidizing bacteria (MOB) in these environments. To address this, 0 to 10 cm plant-associated soil cores were collected from nutrient-impacted (F1), transition (F4), and unimpacted (U3) areas, sectioned in 2-cm increments, and methane oxidation rates were measured. F1 soils consumed approximately two-fold higher methane than U3 soils; additionally, most probable numbers of methanotrophs were 4-log higher in F1 than U3 soils. Metabolically active MOB containing pmoA sequences were characterized by stable-isotope probing using 10 % (v/v) (13)CH(4). pmoA sequences, encoding the alpha subunit of methane monooxygenase and related to type I methanotrophs, were identified from both impacted and unimpacted soils. Additionally, impacted soils also harbored type II methanotrophs, which have been shown to exhibit preferences for high methane concentrations. Additionally, across all soils, novel pmoA-type sequences were also detected, indicating presence of MOB specific to the Everglades. Multivariate statistical analyses confirmed that eutrophic soils consisted of metabolically distinct MOB community that is likely driven by nutrient enrichment. This study enhances our understanding on the biological fate of methane being produced in productive wetland soils of the Florida Everglades and how nutrient-enrichment affects the composition of methanotroph bacterial communities.

  16. Soil nitrous oxide and methane fluxes in integrated crop-livestock systems in subtropics

    International Nuclear Information System (INIS)

    Dieckow, Jeferson; Pergher, Maico; Moraes, Anibal de; Piva, Jonatas Thiago; Bayer, Cimélio; Sakadevan, Karuppan

    2015-01-01

    Integrated crop-livestock (ICL) system is an agricultural practice in which crop-pasture rotation is carried out in the same field over time. In Brasil, ICL associated with no-tillage farming is increasingly gaining importance as a soil use strategy that improves food production (grain, milk and beef) and economic returns to farmers. Integrated crop-livestock-forestry (ICLF) is a recent modification of ICL in Brazil, with the inclusion of trees cultivation aiming at additional wood production and offering thermal comfort to livestock (Porfírio-da-Silva & Moraes, 2010). However, despite the increasing importance of ICL, little information is available on how this system may affect soil-atmosphere exchange of nitrous oxide (N 2 O) and methane (CH 4 )

  17. Catalytic oxidation efficiencies for tritium and tritiated methane in a mature, industrial-scale decontamination system

    International Nuclear Information System (INIS)

    Mintz, J.M.; Gildea, P.D.

    1981-01-01

    Almost all tritium decontamination systems proposed for fusion facilities employ catalytic oxidation to water, followed by drying, to remove tritium and tritiated hydrocarbons from gas streams. One such large-scale system, the gas purification system (GPS), has been operating in the Tritium Research Laboratory (TRL) at Sandia National Laboratories, Livermore, CA, since October 1977. A series of experiments have recently been conducted there to assesss the current operating characteristics of the GPS catalyst. The experiments used tritium and tritiated methane and covered a range of temperatures, flow rates, and concentration levels. When contrasted with 1977 data, the results indicate that no measurable degradation of catalyst function had occurred. However, some reduction in active metal surface area, as indicated by B.E.T. surface area measurements (approx. 100 → 90m 2 /g) and AES scans (approx. 1.4 → 0.9 at. % Pt), had occurred. Kinetic rate coefficients were also derived and a rough temperature dependence obtained

  18. Catalytic oxidation efficiencies for tritium and tritiated methane in a mature, industrial-scale decontamination system

    International Nuclear Information System (INIS)

    Mintz, J.M.; Gildea, P.D.

    1980-10-01

    Almost all tritium decontamination systems proposed for fusion facilities employ catalytic oxidation to water, followed by drying, to remove tritium and tritiated hydrocarbons from gas streams. One such large-scale system, the gas purification system (GPS), has been operating in the Tritium Research Laboratory (TRL) at Sandia National Laboratories, Livermore, CA, since October 1977. A series of experiments have recently been conducted there to assess the current operating characteristics of the GPS catalyst. The experiments used tritium and tritiated methane and covered a range of temperatures, flow rates, and concentration levels. When contrasted with 1977 data, the results indicate that no measurable degradation of catalyst function had occurred. However, some reduction in active metal surface area, as indicated by B.E.T. surface area measurements (approx. 100 → 90 m 2 /g) and AES scans (approx. 1.4 → 0.9 at% Pt), had occurred. Kinetic rate coefficients were also derived and a rough temperature dependence obtained

  19. Evaluation of respiration in compost landfill biocovers intended for methane oxidation

    DEFF Research Database (Denmark)

    Scheutz, Charlotte; Pedicone, Alessio; Pedersen, Gitte Bukh

    2011-01-01

    A low-cost alternative approach to reduce landfill gas (LFG) emissions is to integrate compost into the landfill cover design in order to establish a biocover that is optimized for biological oxidation of methane (CH4). A laboratory and field investigation was performed to quantify respiration...... in an experimental compost biocover in terms of oxygen (O2) consumption and carbon dioxide (CO2) production and emission rates. O2 consumption and CO2 production rates were measured in batch and column experiments containing compost sampled from a landfill biowindow at Fakse landfill in Denmark. Column gas...... concentration profiles were compared to field measurements. Column studies simulating compost respiration in the biowindow showed average CO2 production and O2 consumption rates of 107±14gm−2d−1 and 63±12gm−2d−1, respectively. Gas profiles from the columns showed elevated CO2 concentrations throughout...

  20. Thermodynamic and kinetic control on anaerobic oxidation of methane in marine sediments

    DEFF Research Database (Denmark)

    Knab, Nina J.; Dale, Andrew W.; Lettmann, Karsten

    2008-01-01

    The free energy yield of microbial respiration reactions in anaerobic marine sediments must be sufficient to be conserved as biologically usable energy in the form of ATP. Anaerobic oxidation of methane (AOM) coupled to sulfate reduction (SRR) has a very low standard free energy yield of ΔG  = -33...... yield was rarely less than -20 kJ mol-1 and was mostly rather constant throughout this zone. The kinetic drive was highest at the lower part of the SMTZ, matching the occurrence of maximum AOM rates. The results show that the location of maximum AOM rates is determined by a combination of thermodynamic...... and kinetic drive, whereas the rate activity mainly depends on kinetic regulation....

  1. Anaerobic oxidation of methane at a marine methane seep in a forearc sediment basin off Sumatra, Indian Ocean

    Directory of Open Access Journals (Sweden)

    Michael eSiegert

    2011-12-01

    Full Text Available A cold methane-seep was discovered in a forearc sediment basin off the island Sumatra, exhibiting a methane-seep adapted microbial community. A defined seep centre of activity, like in mud volcanoes, was not discovered. The seep area was rather characterized by a patchy distribution of active spots. The relevance of AOM was reflected by 13C depleted isotopic signatures of dissolved inorganic carbon (DIC. The anaerobic conversion of methane to CO2 was confirmed in a 13C-labelling experiment. Methane fuelled a vital microbial and invertebrate community which was reflected in cell numbers of up to 4 x 109 cells cm 3 sediment and 13C depleted guts of crabs populating the seep area. The microbial community was analysed by total cell counting, catalyzed reporter deposition – fluorescence in situ hybridisation (CARD-FISH, quantitative real-time PCR (qPCR and denaturing gradient gel electrophoresis (DGGE. CARD-FISH cell counts and qPCR measurements showed the presence of Bacteria and Archaea, but only small numbers of Eukarya. The archaeal community comprised largely members of ANME-1 and ANME-2. Furthermore, members of the Crenarchaeota were frequently detected in the DGGE analysis. Three major bacterial phylogenetic groups (δ-Proteobacteria, candidate division OP9 and Anaerolineaceae were abundant across the study area. Several of these sequences were closely related to the genus Desulfococcus of the family Desulfobacteraceae, which is in good agreement with previously described AOM sites. In conclusion, the majority of the microbial community at the seep consisted of AOM related microorganisms, while the relevance of higher hydrocarbons as microbial substrates was negligible.

  2. Effects of Mn- and K-addition on catalytic activity of calcium oxide for methane activation

    International Nuclear Information System (INIS)

    Park, Jong Sik; Kong, Jang Il; Lee, Sung Han; Jun, Jong Ho

    1998-01-01

    Pure CaO, Mn-doped CaO, Mn/CaO, and K/CaO catalysts were prepared and tested as catalysts for the oxidative coupling of methane in the temperature range of 600 to 800 .deg. C to investigate the effects of Mn- and K-addition on the catalytic activity of calcium oxide. To characterize the catalysts, X-ray powder diffraction (XRD), XPS, SEM, DSC, and TG analyses were performed. The catalytic reaction was carried out in a single-pass flow reactor using on-line gas chromatography system. Normalized reaction conditions were generally p(CH 4 )/p(O 2 )=250 Torr/50 Torr, total feed flow rate=30 mL/min, and 1 atm of total pressure with He being used as diluent gas. Among the catalysts tested, 6.3 mol% Mn-doped CaO catalyst showed the best C 2 yield of 8.0% with a selectivity of 43.2% at 775 .deg. C. The C 2 selectivity increased on lightly doped CaO catalysts, while decreased on heavily doped CaO((Mn)>6.3 mol%)catalysts. 6 wt.% Mn/CaO and 6 wt.% K/CaO catalysts showed the C 2 selectivities of 13.2% and 30.9%, respectively, for the reaction. Electrical conductivities of CaO and Mn-doped CaO were measured in the temperature range of 500 to 1000 .deg. C at Po2's of 10 -3 to 10 -1 atm. The electrical conductivity was decreased with Mn-doping and increased with increasing Po 2 in the range of 10 -3 to 10 -1 atm, indicating the specimens to be p-type semiconductors. It was suggested that the interstitial oxygen ions formed near the surface can activate methane and the formation of interstitial oxygen ions was discussed on the basis of solid-state chemistry

  3. Interannual Variability of Carbon Dioxide, Methane and Nitrous Oxide Fluxes in Subarctic European Russian Tundra

    Science.gov (United States)

    Marushchak, M. E.; Voigt, C.; Gil, J.; Lamprecht, R. E.; Trubnikova, T.; Virtanen, T.; Kaverin, D.; Martikainen, P. J.; Biasi, C.

    2017-12-01

    Southern tundra landscapes are particularly vulnerable to climate warming, permafrost thaw and associated landscape rearrangement due to near-zero permafrost temperatures. The large soil C and N stocks of subarctic tundra may create a positive feedback for warming if released to the atmosphere at increased rates. Subarctic tundra in European Russia is a mosaic of land cover types, which all play different roles in the regional greenhouse gas budget. Peat plateaus - massive upheaved permafrost peatlands - are large storehouses of soil carbon and nitrogen, but include also bare peat surfaces that act as hot-spots for both carbon dioxide and nitrous oxide emissions. Tundra wetlands are important for the regional greenhouse gas balance since they show high rates of methane emissions and carbon uptake. The most dominant land-form is upland tundra vegetated by shrubs, lichens and mosses, which displays a close-to-neutral balance with respect to all three greenhouse gases. The study site Seida (67°03'N, 62°56'E), located in the discontinuous permafrost zone of Northeast European Russia, incorporates all these land forms and has been an object for greenhouse gas investigations since 2007. Here, we summarize the growing season fluxes of carbon dioxide, methane and nitrous oxide measured by chamber techniques over the study years. We analyzed the flux time-series together with the local environmental data in order to understand the drivers of interannual variability. Detailed soil profile measurements of greenhouse gas concentrations, soil moisture and temperature provide insights into soil processes underlying the net emissions to the atmosphere. The multiannual time-series allows us to assess the importance of the different greenhouse gases and landforms to the overall climate forcing of the study region.

  4. Plasma-assisted partial oxidation of methane at low temperatures: numerical analysis of gas-phase chemical mechanism

    Energy Technology Data Exchange (ETDEWEB)

    Goujard, Valentin; Nozaki, Tomohiro; Yuzawa, Shuhei; Okazaki, Ken [Department of Mechanical and Control Engineering, Tokyo Institute of Technology, 2-12-1 O-okayama, Meguro, 1528552, Tokyo (Japan); Agiral, Anil, E-mail: tnozaki@mech.titech.ac.jp [Mesoscale Chemical Systems, MESA Institute for Nanotechnology, Faculty of Science and Technology, University of Twente, PO Box 217, 7500 AE, Enschede (Netherlands)

    2011-07-13

    Methane partial oxidation was investigated using a plasma microreactor. The experiments were performed at 5 and 300 deg. C. Microreactor configuration allows an efficient evacuation of the heat generated by methane partial oxidation and dielectric barrier discharges, allowing at the same time a better temperature control. At 5 deg. C, liquid condensation of low vapour pressure compounds, such as formaldehyde and methanol, occurs. {sup 1}H-NMR analysis allowed us to demonstrate significant CH{sub 3}OOH formation during plasma-assisted partial oxidation of methane. Conversion and product selectivity were discussed for both temperatures. In the second part of this work, a numerical simulation was performed and a gas-phase chemical mechanism was proposed and discussed. From the comparison between the experimental results and the simulation it was found that CH{sub 3}OO{center_dot} formation has a determinant role in oxygenated compound production, since its fast formation disfavoured radical recombination. At 5 deg. C the oxidation leads mainly towards oxygenated compound formation, and plasma dissociation was the major phenomenon responsible for CH{sub 4} conversion. At 300 deg. C, higher CH{sub 4} conversion resulted from oxidative reactions induced by {center_dot}OH radicals with a chemistry predominantly oxidative, producing CO, H{sub 2}, CO{sub 2} and H{sub 2}O.

  5. Identification of Novel Methane-, Ethane-, and Propane-Oxidizing Bacteria at Marine Hydrocarbon Seeps by Stable Isotope Probing ▿ †

    Science.gov (United States)

    Redmond, Molly C.; Valentine, David L.; Sessions, Alex L.

    2010-01-01

    Marine hydrocarbon seeps supply oil and gas to microorganisms in sediments and overlying water. We used stable isotope probing (SIP) to identify aerobic bacteria oxidizing gaseous hydrocarbons in surface sediment from the Coal Oil Point seep field located offshore of Santa Barbara, California. After incubating sediment with 13C-labeled methane, ethane, or propane, we confirmed the incorporation of 13C into fatty acids and DNA. Terminal restriction fragment length polymorphism (T-RFLP) analysis and sequencing of the 16S rRNA and particulate methane monooxygenase (pmoA) genes in 13C-DNA revealed groups of microbes not previously thought to contribute to methane, ethane, or propane oxidation. First, 13C methane was primarily assimilated by Gammaproteobacteria species from the family Methylococcaceae, Gammaproteobacteria related to Methylophaga, and Betaproteobacteria from the family Methylophilaceae. Species of the latter two genera have not been previously shown to oxidize methane and may have been cross-feeding on methanol, but species of both genera were heavily labeled after just 3 days. pmoA sequences were affiliated with species of Methylococcaceae, but most were not closely related to cultured methanotrophs. Second, 13C ethane was consumed by members of a novel group of Methylococcaceae. Growth with ethane as the major carbon source has not previously been observed in members of the Methylococcaceae; a highly divergent pmoA-like gene detected in the 13C-labeled DNA may encode an ethane monooxygenase. Third, 13C propane was consumed by members of a group of unclassified Gammaproteobacteria species not previously linked to propane oxidation. This study identifies several bacterial lineages as participants in the oxidation of gaseous hydrocarbons in marine seeps and supports the idea of an alternate function for some pmoA-like genes. PMID:20675448

  6. Identification of novel methane-, ethane-, and propane-oxidizing bacteria at marine hydrocarbon seeps by stable isotope probing.

    Science.gov (United States)

    Redmond, Molly C; Valentine, David L; Sessions, Alex L

    2010-10-01

    Marine hydrocarbon seeps supply oil and gas to microorganisms in sediments and overlying water. We used stable isotope probing (SIP) to identify aerobic bacteria oxidizing gaseous hydrocarbons in surface sediment from the Coal Oil Point seep field located offshore of Santa Barbara, California. After incubating sediment with (13)C-labeled methane, ethane, or propane, we confirmed the incorporation of (13)C into fatty acids and DNA. Terminal restriction fragment length polymorphism (T-RFLP) analysis and sequencing of the 16S rRNA and particulate methane monooxygenase (pmoA) genes in (13)C-DNA revealed groups of microbes not previously thought to contribute to methane, ethane, or propane oxidation. First, (13)C methane was primarily assimilated by Gammaproteobacteria species from the family Methylococcaceae, Gammaproteobacteria related to Methylophaga, and Betaproteobacteria from the family Methylophilaceae. Species of the latter two genera have not been previously shown to oxidize methane and may have been cross-feeding on methanol, but species of both genera were heavily labeled after just 3 days. pmoA sequences were affiliated with species of Methylococcaceae, but most were not closely related to cultured methanotrophs. Second, (13)C ethane was consumed by members of a novel group of Methylococcaceae. Growth with ethane as the major carbon source has not previously been observed in members of the Methylococcaceae; a highly divergent pmoA-like gene detected in the (13)C-labeled DNA may encode an ethane monooxygenase. Third, (13)C propane was consumed by members of a group of unclassified Gammaproteobacteria species not previously linked to propane oxidation. This study identifies several bacterial lineages as participants in the oxidation of gaseous hydrocarbons in marine seeps and supports the idea of an alternate function for some pmoA-like genes.

  7. Catalytic partial oxidation of methane over porous silica supported VO{sub x} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Pirovano, C.; Schoenborn, E.; Kalevaru, V.N.; Wohlrab, S.; Luecke, B.; Martin, A. [University Rostock e.V., Rostock (Germany). Leibniz Inst. for Catalysis

    2011-07-01

    High surface area mesoporous siliceous MCM-41 and SBA-15 materials have been used as supports to disperse vanadium oxide species using wet impregnation and incipient wetness impregnation methods. These materials were used as catalysts for the partial oxidation of methane (POM) to formaldehyde. The physico-chemical properties of the solids were studied by means of BET, DR-UV/Vis spectroscopy, Py-FTIR and TEM. The influence of support and the preparation method on the dispersion of VOx is also investigated. The catalytic properties of the catalysts were examined in a fixed bed stainless steel reactor at 923 K. So far a maximum production of formaldehyde can be detected on SBA-15 supported VOx-catalysts prepared by incipient wetness impregnation. On this V/SBA-15 material a covalent attachment of catalytic active molecular vanadium species dominates, which in turn leads to a lower activation temperature and thereby reduced over-oxidation. From the best case, the space time yield of HCHO could be reached close to 775 g{sub HCHO} Kg{sub cat}{sup -1} h{sup -1}. (orig.)

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

    Directory of Open Access Journals (Sweden)

    P. A. Nauer

    2012-06-01

    Full Text Available 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

  9. Evaluation of methane oxidation activity in waste biocover soil during landfill stabilization.

    Science.gov (United States)

    He, Ruo; Wang, Jing; Xia, Fang-Fang; Mao, Li-Juan; Shen, Dong-Sheng

    2012-10-01

    Biocover soil has been demonstrated to have high CH(4) oxidation capacity and is considered as a good alternative cover material to mitigate CH(4) emission from landfills, yet the response of CH(4) oxidation activity of biocover soils to the variation of CH(4) loading during landfill stabilization is poorly understood. Compared with a landfill cover soil (LCS) collected from Hangzhou Tianziling landfill cell, the development of CH(4) oxidation activity of waste biocover soil (WBS) was investigated using simulated landfill systems in this study. Although a fluctuation of influent CH(4) flux occurred during landfill stabilization, the WBS covers showed a high CH(4) removal efficiency of 94-96% during the entire experiment. In the LCS covers, the CH(4) removal efficiencies varied with the fluctuation of CH(4) influent flux, even negative ones occurred due to the storage of CH(4) in the soil porosities after the high CH(4) influent flux of ~137 gm(-2) d(-1). The lower concentrations of O(2) and CH(4) as well as the higher concentration of CO(2) were observed in the WBS covers than those in the LCS covers. The highest CH(4) oxidation rates of the two types of soil covers both occurred in the bottom layer (20-30 cm). Compared to the LCS, the WBS showed higher CH(4) oxidation activity and methane monooxygenase activity over the course of the experiment. Overall, this study indicated the WBS worked well for the fluctuation of CH(4) influent flux during landfill stabilization. Copyright © 2012 Elsevier Ltd. All rights reserved.

  10. Characterization of specific membrane fatty acids as chemotaxonomic markers for sulfate-reducing bacteria involved in anaerobic oxidation of methane

    DEFF Research Database (Denmark)

    Elvert, M.; Boetius, A.; Knittel, K.

    2003-01-01

    Membrane fatty acids were extracted from a sediment core above marine gas hydrates at Hydrate Ridge, NE Pacific. Anaerobic sediments from this environment are characterized by high sulfate reduction rates driven by the anaerobic oxidation of methane (AOM). The assimilation of methane carbon......-reducing bacteria (SRB) of the Desulfosarcina/Desulfococcus group, which are present in the aggregates of AOM consortia in extremely high numbers, these specific fatty acids appear to provide a phenotypic fingerprint indicative for SRB of this group. Correlating depth profiles of specific fatty acid content...

  11. Syntrophic acetate oxidation in two-phase (acid-methane) anaerobic digesters.

    Science.gov (United States)

    Shimada, T; Morgenroth, E; Tandukar, M; Pavlostathis, S G; Smith, A; Raskin, L; Kilian, R E

    2011-01-01

    The microbial processes involved in two-phase anaerobic digestion were investigated by operating a laboratory-scale acid-phase (AP) reactor and analyzing two full-scale, two-phase anaerobic digesters operated under mesophilic (35 °C) conditions. The digesters received a blend of primary sludge and waste activated sludge (WAS). Methane levels of 20% in the laboratory-scale reactor indicated the presence of methanogenic activity in the AP. A phylogenetic analysis of an archaeal 16S rRNA gene clone library of one of the full-scale AP digesters showed that 82% and 5% of the clones were affiliated with the orders Methanobacteriales and Methanosarcinales, respectively. These results indicate that substantial levels of aceticlastic methanogens (order Methanosarcinales) were not maintained at the low solids retention times and acidic conditions (pH 5.2-5.5) of the AP, and that methanogenesis was carried out by hydrogen-utilizing methanogens of the order Methanobacteriales. Approximately 43, 31, and 9% of the archaeal clones from the methanogenic phase (MP) digester were affiliated with the orders Methanosarcinales, Methanomicrobiales, and Methanobacteriales, respectively. A phylogenetic analysis of a bacterial 16S rRNA gene clone library suggested the presence of acetate-oxidizing bacteria (close relatives of Thermacetogenium phaeum, 'Syntrophaceticus schinkii,' and Clostridium ultunense). The high abundance of hydrogen consuming methanogens and the presence of known acetate-oxidizing bacteria suggest that acetate utilization by acetate oxidizing bacteria in syntrophic interaction with hydrogen-utilizing methanogens was an important pathway in the second-stage of the two-phase digestion, which was operated at high ammonium-N concentrations (1.0 and 1.4 g/L). A modified version of the IWA Anaerobic Digestion Model No. 1 (ADM1) with extensions for syntrophic acetate oxidation and weak-acid inhibition adequately described the dynamic profiles of volatile acid production

  12. Estimation of methane and nitrous oxide emission from livestock and poultry in China during 1949-2003

    International Nuclear Information System (INIS)

    Zhou, J.B.; Jiang, M.M.; Chen, G.Q.

    2007-01-01

    To investigate the greenhouse gases emission from enteric fermentation and manure management of livestock and poultry industry in China, the present study presents a systematic estimation of methane and nitrous oxide emission during 1949-2003, based on the local measurement and IPCC guidelines. As far as greenhouse gases emittion is concerned among livestock swine is found to hold major position followed by goat and sheep, while among poultry chicken has the major place and is followed by duck and geese. Methane emission from enteric fermentation is estimated to have increased from 3.04 Tg in 1949 to 10.13 Tg in 2003, an averaged annual growth rate of 2.2%, and methane emission from manure management has increased from 0.16 Tg in 1949 to 1.06 Tg in 2003, an annual growth rate of 3.5%, while nitrous oxide emission from manure management has increased from 47.76 to 241.2 Gg in 2003, with an annual growth rate of 3.0%. The total greenhouse gas emission has increased from 82.01 Tg CO 2 Eq. in 1949 to 309.76 Tg CO 2 Eq. in 2003, an annual growth rate of 2.4%. The estimation of livestock methane and nitrous oxide emissions in China from 1949 to 2003 is shown to be consistent with a linear growth model, and the reduction of greenhouse gas emission is thus considered an urgent and arduous task for the Chinese livestock industry

  13. Direct Synthesis of Methanol by Partial Oxidation of Methane with Oxygen over Cobalt Modified Mesoporous H-ZSM-5 Catalyst

    Directory of Open Access Journals (Sweden)

    Yuni Krisyuningsih Krisnandi

    2015-11-01

    Full Text Available Partial oxidation of methane over mesoporous catalyst cobalt modified H-ZSM-5 has been carried out. Mesoporous Na-ZSM-5 (Si/Al = 35.4 was successfully synthesized using double template method which has high surface area (450 m2/g and average pore diameter distribution of 1.9 nm. The as-synthesized Na-ZSM-5 was converted to H-ZSM-5 through multi-exchange treatment with ammonium ion solution, causing decreased crystallinity and surface area, but increased porous diameter, due to dealumination during treatment process. Moreover, H-ZSM-5 was loaded with cobalt (Co = 2.5% w by the incipient impregnation method and calcined at 550 °C. Partial oxidation of methane was performed in the batch reactor with 0.75 bar methane and 2 bar of nitrogen (with impurities of 0.5% oxygen as the input at various reaction time (30, 60 and 120 min. The reaction results show that cobalt species in catalyst has an important role, because H-ZSM-5 cannot produce methanol in partial oxidation of methane. The presence of molecular oxygen increased the percentage of methanol yield. The reaction is time-dependent with the highest methanol yield (79% was acquired using Co/H-ZSM-5 catalyst for 60 min.

  14. Performance evaluation and comparison of fuel processors integrated with PEM fuel cell based on steam or autothermal reforming and on CO preferential oxidation or selective methanation

    International Nuclear Information System (INIS)

    Ercolino, Giuliana; Ashraf, Muhammad A.; Specchia, Vito; Specchia, Stefania

    2015-01-01

    Highlights: • Modeling of different fuel processors integrated with PEM fuel cell stack. • Steam or autothermal reforming + CO selective methanation or preferential oxidation. • Reforming of different hydrocarbons: gasoline, light diesel oil, natural gas. • 5 kW e net systems comparison via energy efficiency and primary fuel rate consumed. • Highest net efficiency: steam reformer + CO selective methanation based system. - Abstract: The performances of four different auxiliary power unit (APU) schemes, based on a 5 kW e net proton exchange membrane fuel cell (PEM-FC) stack, are evaluated and compared. The fuel processor section of each APU is characterized by a reformer (autothermal ATR or steam SR), a non-isothermal water gas shift (NI-WGS) reactor and a final syngas catalytic clean-up step: the CO preferential oxidation (PROX) reactor or the CO selective methanation (SMET) one. Furthermore, three hydrocarbon fuels, the most commonly found in service stations (gasoline, light diesel oil and natural gas) are considered as primary fuels. The comparison is carried out examining the results obtained by a series of steady-state system simulations in Aspen Plus® of the four different APU schemes by varying the fed fuel. From the calculated data, the performance of CO-PROX is not very different compared to that of the CO-SMET, but the performance of the SR based APUs is higher than the scheme of the ATR based APUs. The most promising APU scheme with respect to an overall performance target is the scheme fed with natural gas and characterized by a fuel processor chain consisting of SR, NI-WGS and CO-SMET reactors. This processing reactors scheme together with the fuel cell section, notwithstanding having practically the same energy efficiency of the scheme with SR, NI-WGS and CO-PROX reactors, ensures a less complex scheme, higher hydrogen concentration in the syngas, lower air mass rate consumption, the absence of nitrogen in the syngas and higher potential

  15. Final Report: Room Temperature Electrochemical Upgrading of Methane to Oxygenate Fuels

    Energy Technology Data Exchange (ETDEWEB)

    Mustain, William

    2018-01-02

    The overall objective of this project is to discover the nature of the electrochemically active sites and to uncover the mechanisms for the electrocatalytic transformation of small organic molecules to oxygenate products such as methanol, formaldehyde, carbon monoxide and acetylene. Among the feedstocks of interest in this study are: methane, carbon dioxide, and acetic acid. Methane is an incredibly attractive potential feedstock because of the recent discovery of large shale deposits; carbon dioxide is potentially a very available feedstock from carbon capture technologies; acetic acid (as well as CH4 and CO2 and ethanol) has potential as a bio-derived feedstock. This report summarizes the major results to date regarding the electrochemical transformation of CH4, CO2 and acetic acid to chemicals and fuels – with a primary focus on methane. Finer details are available in each of the projects annual reports. In addition to the primary objective, the work in this project has led to synergistic discoveries that are advantageous to other fields including: catalyst layer deposition, anion exchange membrane fuel cells, CO2 capture and li-ion batteries. Those are very briefly discussed as well.

  16. Recovery and biological oxidation of dissolved methane in effluent from UASB treatment of municipal sewage using a two-stage closed downflow hanging sponge system.

    Science.gov (United States)

    Matsuura, Norihisa; Hatamoto, Masashi; Sumino, Haruhiko; Syutsubo, Kazuaki; Yamaguchi, Takashi; Ohashi, Akiyoshi

    2015-03-15

    A two-stage closed downflow hanging sponge (DHS) reactor was used as a post-treatment to prevent methane being emitted from upflow anaerobic sludge blanket (UASB) effluents containing unrecovered dissolved methane. The performance of the closed DHS reactor was evaluated using real municipal sewage at ambient temperatures (10-28 °C) for one year. The first stage of the closed DHS reactor was intended to recover dissolved methane from the UASB effluent and produce a burnable gas with a methane concentration greater than 30%, and its recovery efficiency was 57-88%, although the amount of dissolved methane in the UASB effluent fluctuated in the range of 46-68 % of methane production greatly depending on the temperature. The residual methane was oxidized and the remaining organic carbon was removed in the second closed DHS reactor, and this reactor performed very well, removing more than 99% of the dissolved methane during the experimental period. The rate at which air was supplied to the DHS reactor was found to be one of the most important operating parameters. Microbial community analysis revealed that seasonal changes in the methane-oxidizing bacteria were key to preventing methane emissions. Copyright © 2014 Elsevier Ltd. All rights reserved.

  17. Catalytic properties of new anode materials for solid oxide fuel cells operated under methane at intermediary temperature

    Science.gov (United States)

    Sauvet, A.-L.; Fouletier, J.

    The recent trend in solid oxide fuel cell concerns the use of natural gas as fuel. Steam reforming of methane is a well-established process for producing hydrogen directly at the anode side. In order to develop new anode materials, the catalytic activities of several oxides for the steam reforming of methane were characterized by gas chromatography. We studied the catalytic activity as a function of steam/carbon ratios r. The methane and the steam content were varied between 5 and 30% and between 1.5 and 3.5%, respectively, corresponding to r-values between 0.07 and 0.7. Catalyst (ruthenium and vanadium)-doped lanthanum chromites substituted with strontium, gadolinium-doped ceria (Ce 0.9Gd 0.1O 2) referred as to CeGdO 2, praseodymium oxide, molybdenum oxide and copper oxide were tested. The working temperature was fixed at 850°C, except for 5% ruthenium-doped La 1- xSr xCrO 3 where the temperature was varied between 700 and 850°C. Two types of behavior were observed as a function of the activity of the catalyst. The higher steam reforming efficiency was observed with 5% of ruthenium above 750°C.

  18. Biotic manganese oxidation coupled with methane oxidation using a continuous-flow bioreactor system under marine conditions.

    Science.gov (United States)

    Kato, Shingo; Miyazaki, Masayuki; Kikuchi, Sakiko; Kashiwabara, Teruhiko; Saito, Yumi; Tasumi, Eiji; Suzuki, Katsuhiko; Takai, Ken; Cao, Linh Thi Thuy; Ohashi, Akiyoshi; Imachi, Hiroyuki

    2017-10-01

    Biogenic manganese oxides (BioMnOx) can be applied for the effective removal and recovery of trace metals from wastewater because of their high adsorption capacity. Although a freshwater continuous-flow system for a nitrifier-based Mn-oxidizing microbial community for producing BioMnOx has been developed so far, a seawater continuous-flow bioreactor system for BioMnOx production has not been established. Here, we report BioMnOx production by a methanotroph-based microbial community by using a continuous-flow bioreactor system. The bioreactor system was operated using a deep-sea sediment sample as the inoculum with methane as the energy source for over 2 years. The BioMnOx production became evident after 370 days of reactor operation. The maximum Mn oxidation rate was 11.4 mg L -1 day -1 . An X-ray diffraction analysis showed that the accumulated BioMnOx was birnessite. 16S rRNA gene-based clone analyses indicated that methanotrophic bacterial members were relatively abundant in the system; however, none of the known Mn-oxidizing bacteria were detected. A continuous-flow bioreactor system coupled with nitrification was also run in parallel for 636 days, but no BioMnOx production was observed in this bioreactor system. The comparative experiments indicated that the methanotroph-based microbial community, rather than the nitrifier-based community, was effective for BioMnOx production under the marine environmental conditions.

  19. Development of METHANE de-NOX Reburn Process for Wood Waste and Biomass Fired Stoker Boilers - Final Report - METHANE de-NOX Reburn Technology Manual

    Energy Technology Data Exchange (ETDEWEB)

    J. Rabovitser; B. Bryan; S. Wohadlo; S. Nester; J. Vaught; M. Tartan (Gas Technology Institute); R. Glickert (ESA Environmental Solutions)

    2007-12-31

    The overall objective of this project was to demonstrate the effectiveness of the METHANE de-NOX® (MdN) Reburn process in the Forest Products Industry (FPI) to provide more efficient use of wood and sludge waste (biosolids) combustion for both energy generation and emissions reduction (specifically from nitrogen oxides (NOx)) and to promote the transfer of the technology to the wide range of wood waste-fired stoker boilers populating the FPI. This document, MdN Reburn Commercial Technology Manual, was prepared to be a resource to promote technology transfer and commercialization activities of MdN in the industry and to assist potential users understand its application and installation requirements. The Manual includes a compilation of MdN commercial design data from four different stoker boiler designs that were baseline tested as part of the development effort. Design information in the Manual include boiler CFD model studies, process design protocols, engineering data sheets and commercial installation drawings. Each design package is unique and implemented in a manner to meet specific mill requirements.

  20. Formaldehyde formation in coupled oxidation of methane and methanol over V2O5 and MoO3 silica supported catalysts

    International Nuclear Information System (INIS)

    Lojewska, J.; Makowski, W.; Fajardo Farre, A.; Dziembaj, R.

    2003-01-01

    The effect of methanol on partial oxidation of methane has been studied on standard molybdena and vanadia catalysts supported on silica. Prior to catalytic tests the catalysts were characterized by BET, SEM/EDAX and TPR/O methods. Three types of catalytic tests were performed giving temperature and contact time dependence on the catalyst activity and selectivity: partial oxidations of methane, methanol and methane/methanol mixtures. The methanol showed an activating impact on the partial oxidation of methane over all used catalysts samples, but the strongest one over Mo 3 /SiO 2 . In the absence of CH 3 OH the only catalyst, which exhibited HCHO selectivity, was low loaded vanadia catalyst. It has been put forward that methanol may enhance formation of oxygen active species, prerequisites for activating methane molecules, through reducing vanadia cations and causing breakage of vanadium oxygen bonds. (author)

  1. Environmental and microbial factors influencing methane and nitrous oxide fluxes in Mediterranean cork oak woodlands: trees make a difference.

    Science.gov (United States)

    Shvaleva, Alla; Siljanen, Henri M P; Correia, Alexandra; Costa E Silva, Filipe; Lamprecht, Richard E; Lobo-do-Vale, Raquel; Bicho, Catarina; Fangueiro, David; Anderson, Margaret; Pereira, João S; Chaves, Maria M; Cruz, Cristina; Martikainen, Pertti J

    2015-01-01

    Cork oak woodlands (montado) are agroforestry systems distributed all over the Mediterranean basin with a very important social, economic and ecological value. A generalized cork oak decline has been occurring in the last decades jeopardizing its future sustainability. It is unknown how loss of tree cover affects microbial processes that are consuming greenhouse gases in the montado ecosystem. The study was conducted under two different conditions in the natural understory of a cork oak woodland in center Portugal: under tree canopy (UC) and open areas without trees (OA). Fluxes of methane and nitrous oxide were measured with a static chamber technique. In order to quantify methanotrophs and bacteria capable of nitrous oxide consumption, we used quantitative real-time PCR targeting the pmoA and nosZ genes encoding the subunit of particulate methane mono-oxygenase and catalytic subunit of the nitrous oxide reductase, respectively. A significant seasonal effect was found on CH4 and N2O fluxes and pmoA and nosZ gene abundance. Tree cover had no effect on methane fluxes; conversely, whereas the UC plots were net emitters of nitrous oxide, the loss of tree cover resulted in a shift in the emission pattern such that the OA plots were a net sink for nitrous oxide. In a seasonal time scale, the UC had higher gene abundance of Type I methanotrophs. Methane flux correlated negatively with abundance of Type I methanotrophs in the UC plots. Nitrous oxide flux correlated negatively with nosZ gene abundance at the OA plots in contrast to that at the UC plots. In the UC soil, soil organic matter had a positive effect on soil extracellular enzyme activities, which correlated positively with the N2O flux. Our results demonstrated that tree cover affects soil properties, key enzyme activities and abundance of microorganisms and, consequently net CH4 and N2O exchange.

  2. Catalysis by Nanostructures: Methane, Ethylene Oxide, and Propylene Oxide Synthesis on Ag, Cu or Au Nanoclusters

    Science.gov (United States)

    2008-02-07

    22 nm) were prepared by reducing a Au salt, and encapsulating the Au nanoparticles formed in a polymer33 . A variety of high area oxides (TiO 2, ZnO ...Morphologies Utilizing a Combinatorial Electrochemistry Methodology. Ph. D. dissertation, Chemical Engineering, University of California, Santa Barbara (2004

  3. Selective bio-oxidation of propane to acetone using methane-oxidizing Methylomonas sp. DH-1.

    Science.gov (United States)

    Hur, Dong Hoon; Nguyen, Thu Thi; Kim, Donghyuk; Lee, Eun Yeol

    2017-07-01

    Propane is the major component of liquefied petroleum gas (LPG). Nowadays, the use of LPG is decreasing, and thus utilization of propane as a chemical feedstock is in need of development. An efficient biological conversion of propane to acetone using a methanotrophic whole cell as the biocatalyst was proposed and investigated. A bio-oxidation pathway of propane to acetone in Methylomonas sp. DH-1 was analyzed by gene expression profiling via RNA sequencing. Propane was oxidized to 2-propanol by particulate methane monooxygenase and subsequently to acetone by methanol dehydrogenases. Methylomonas sp. DH-1 was deficient in acetone-converting enzymes and thus accumulated acetone in the absence of any enzyme inhibition. The maximum accumulation, average productivity and specific productivity of acetone were 16.62 mM, 0.678 mM/h and 0.141 mmol/g cell/h, respectively, under the optimized conditions. Our study demonstrates a novel method for the bioconversion of propane to acetone using methanotrophs under mild reaction condition.

  4. Nitrogen source effects on the denitrifying anaerobic methane oxidation culture and anaerobic ammonium oxidation bacteria enrichment process.

    Science.gov (United States)

    Fu, Liang; Ding, Jing; Lu, Yong-Ze; Ding, Zhao-Wei; Zeng, Raymond J

    2017-05-01

    The co-culture system of denitrifying anaerobic methane oxidation (DAMO) and anaerobic ammonium oxidation (Anammox) has a potential application in wastewater treatment plant. This study explored the effects of permutation and combination of nitrate, nitrite, and ammonium on the culture enrichment from freshwater sediments. The co-existence of NO 3 - , NO 2 - , and NH 4 + shortened the enrichment time from 75 to 30 days and achieved a total nitrogen removal rate of 106.5 mg/L/day on day 132. Even though ammonium addition led to Anammox bacteria increase and a higher nitrogen removal rate, DAMO bacteria still dominated in different reactors with the highest proportion of 64.7% and the maximum abundance was 3.07 ± 0.25 × 10 8 copies/L (increased by five orders of magnitude) in the nitrite reactor. DAMO bacteria showed greater diversity in the nitrate reactor, and one was similar to M. oxyfera; DAMO bacteria in the nitrite reactor were relatively unified and similar to M. sinica. Interestingly, no DAMO archaea were found in the nitrate reactor. This study will improve the understanding of the impact of nitrogen source on DAMO and Anammox co-culture enrichment.

  5. Potential roles of anaerobic ammonium and methane oxidation in the nitrogen cycle of wetland ecosystems.

    Science.gov (United States)

    Zhu, Guibing; Jetten, Mike S M; Kuschk, Peter; Ettwig, Katharina F; Yin, Chengqing

    2010-04-01

    Anaerobic ammonium oxidation (anammox) and anaerobic methane oxidation (ANME coupled to denitrification) with nitrite as electron acceptor are two of the most recent discoveries in the microbial nitrogen cycle. Currently the anammox process has been relatively well investigated in a number of natural and man-made ecosystems, while ANME coupled to denitrification has only been observed in a limited number of freshwater ecosystems. The ubiquitous presence of anammox bacteria in marine ecosystems has changed our knowledge of the global nitrogen cycle. Up to 50% of N(2) production in marine sediments and oxygen-depleted zones may be attributed to anammox bacteria. However, there are only few indications of anammox in natural and constructed freshwater wetlands. In this paper, the potential role of anammox and denitrifying methanotrophic bacteria in natural and artificial wetlands is discussed in relation to global warming. The focus of the review is to explore and analyze if suitable environmental conditions exist for anammox and denitrifying methanotrophic bacteria in nitrogen-rich freshwater wetlands.

  6. Electrochemical promotion of oxidative coupling of methane on platinum/polybenzimidazole catalyst

    DEFF Research Database (Denmark)

    Petrushina, Irina; Bandur, Viktor; Bjerrum, Niels

    2002-01-01

    The electrochemical promotion of catalytic methane oxidation was studied using a (CH4,O-2,Ar), Pt\\polybenzimidazole (PBI)-H3PO4\\Pt,(H-2,Ar) fuel cell at 135degreesC. It has been found that C2H2, CO2, and water are the main oxidation products. Without polarization the yield of C2H2 was 0......, meaning that there was a maximum promotion effect at a polarization of -0.15 V, or 0.45 V catalyst potential vs. a hydrogen electrode (3.8% C2H2 yield). The catalytic rate enhancement ratio, r(C-2)/r(o)(C-2), at this maximum was 4.2. There was no C2H2 production at polarization greater than or equal to0.......9% and the yield of CO2 was 7.3%. This means that C-2 open-circuit selectivity was approximately 11%. Open-circuit voltage was around 0.6 V. It has been shown that the CH4 --> C2H2 catalytic reaction can be electrochemically promoted at negative polarization and exhibits a clear "volcano-type'' promotion behavior...

  7. Response of methane production via propionate oxidation to carboxylated multiwalled carbon nanotubes in paddy soil enrichments

    Directory of Open Access Journals (Sweden)

    Jianchao Zhang

    2018-01-01

    Full Text Available Carboxylated multiwalled carbon nanotubes (MWCNTs-COOH have become a growing concern in terms of their fate and toxicity in aqueous environments. Methane (CH4 is a major product of organic matter degradation in waterlogged environments. In this study, we determined the effect of MWCNTs-COOH on the production of CH4 from propionate oxidation in paddy soil enrichments. The results showed that the methanogenesis from propionate degradation was accelerated in the presence of MWCNTs-COOH. In addition, the rates of CH4 production and propionate degradation increased with increasing concentrations of MWCNTs-COOH. Scanning electron microscopy (SEM observations showed that the cells were intact and maintained their structure in the presence of MWCNTs-COOH. In addition, SEM and fluorescence in situ hybridization (FISH images revealed that the cells were in direct contact with the MWCNTs and formed cell-MWCNTs aggregates that contained both bacteria and archaea. On the other hand, nontoxic magnetite nanoparticles (Fe3O4 had similar effects on the CH4 production and cell integrity as the MWCNTs-COOH. Compared with no nanomaterial addition, the relative abundances of Geobacter and Methanosarcina species increased in the presence of MWCNTs-COOH. This study suggests that MWCNTs-COOH exerted positive rather than cytotoxic effects on the syntrophic oxidation of propionate in paddy soil enrichments and affected the bacterial and archaeal community structure at the test concentrations. These findings provide novel insight into the consequences of nanomaterial release into anoxic natural environments.

  8. Anaerobic Methane-Oxidizing Microbial Community in a Coastal Marine Sediment: Anaerobic Methanotrophy Dominated by ANME-3.

    Science.gov (United States)

    Bhattarai, Susma; Cassarini, Chiara; Gonzalez-Gil, Graciela; Egger, Matthias; Slomp, Caroline P; Zhang, Yu; Esposito, Giovanni; Lens, Piet N L

    2017-10-01

    The microbial community inhabiting the shallow sulfate-methane transition zone in coastal sediments from marine Lake Grevelingen (The Netherlands) was characterized, and the ability of the microorganisms to carry out anaerobic oxidation of methane coupled to sulfate reduction was assessed in activity tests. In vitro activity tests of the sediment with methane and sulfate demonstrated sulfide production coupled to the simultaneous consumption of sulfate and methane at approximately equimolar ratios over a period of 150 days. The maximum sulfate reduction rate was 5 μmol sulfate per gram dry weight per day during the incubation period. Diverse archaeal and bacterial clades were retrieved from the sediment with the majority of them clustered with Euryarchaeota, Thaumarcheota, Bacteroidetes, and Proteobacteria. The 16S rRNA gene sequence analysis showed that the sediment from marine Lake Grevelingen contained anaerobic methanotrophic Archaea (ANME) and methanogens as archaeal clades with a role in the methane cycling. ANME at the studied site mainly belong to the ANME-3 clade. This study provides one of the few reports for the presence of ANME-3 in a shallow coastal sediment. Sulfate-reducing bacteria from Desulfobulbus clades were found among the sulfate reducers, however, with very low relative abundance. Desulfobulbus has previously been commonly found associated with ANME, whereas in our study, ANME-3 and Desulfobulbus were not observed simultaneously in clusters, suggesting the possibility of independent AOM by ANME-3.

  9. Optimization geometries of a vortex gliding-arc reactor for partial oxidation of methane

    International Nuclear Information System (INIS)

    Guofeng, Xu; Xinwei, Ding

    2012-01-01

    The effects of the geometry of gliding-arc reactor – such as distance between the electrodes, outlet diameter, and inlet position – on the reactor characteristics (methane conversion, hydrogen yield, and energy efficiency) have not been fully investigated. In this paper, AC gliding-arc reactors including the vortex flow configuration are designed to produce hydrogen from the methane by partial oxidation. The influence of vortex flow configuration on the reactor characteristics is also studied by varying the inlet position. When the inlet of the gliding-arc reactor is positioned close to the outlet, reverse vortex flow reactor (RVFR), the maximum energy efficiency reaches 50% and the yields of hydrogen and carbon monoxide are 40% and 65%, respectively. As the distance between electrodes increases from 5 mm to 15 mm, both hydrogen yield and energy efficiency increase approximately 10% for the RVFR. The energy efficiency and hydrogen yield are highest when the ratio of the outlet diameter to the inner diameter is 0.5 for the RVFR. Experimental results indicate that the flow field in the plasma reactor has an important influence on the reactor performance. Furthermore, hydrogen production increases as the number of feed gas flows in contact with the plasma zone increases. -- Highlights: ► Gliding-arc reactors were designed to produce hydrogen for studying the characteristics of the vortex flow reactor. ► Hydrogen yield of reverse vortex flow reactor was 10% higher than that of forward vortex flow reactor. ► Maximum energy efficiency was 50% for reverse vortex flow reactor. ► If discharge power was supplied to the reactors, the reactor performance increased with increasing distance between electrodes. ► Optimum ratio of the outlet and inner diameter was 1/2.

  10. Nitrous oxide and methane emissions and nitrous oxide isotopic composition from waste incineration in Switzerland.

    Science.gov (United States)

    Harris, Eliza; Zeyer, Kerstin; Kegel, Rainer; Müller, Beat; Emmenegger, Lukas; Mohn, Joachim

    2015-01-01

    Solid waste incineration accounts for a growing proportion of waste disposal in both developed and developing countries, therefore it is important to constrain emissions of greenhouse gases from these facilities. At five Swiss waste incineration facilities with grate firing, emission factors for N2O and CH4 were determined based on measurements of representative flue gas samples, which were collected in Tedlar bags over a one year period (September 2010-August 2011) and analysed with FTIR spectroscopy. All five plants burn a mixture of household and industrial waste, and two of the plants employ NOx removal through selective non-catalytic reduction (SNCR) while three plants use selective catalytic reduction (SCR) for NOx removal. N2O emissions from incineration plants with NOx removal through selective catalytic reduction were 4.3 ± 4.0g N2O tonne(-1) waste (wet) (hereafter abbreviated as t(-1)) (0.4 ± 0.4 g N2O GJ(-1)), ten times lower than from plants with selective non-catalytic reduction (51.5 ± 10.6g N2O t(-1); 4.5 ± 0.9g N2O GJ(-1)). These emission factors, which are much lower than the value of 120g N2O t(-1) (10.4g N2O GJ(-1)) used in the 2013 Swiss national greenhouse gas emission inventory, have been implemented in the most recent Swiss emission inventory. In addition, the isotopic composition of N2O emitted from the two plants with SNCR, which had considerable N2O emissions, was measured using quantum cascade laser spectroscopy. The isotopic site preference of N2O - the enrichment of (14)N(15)NO relative to (15)N(14)NO - was found to be 17.6 ± 0.8‰, with no significant difference between the two plants. Comparison to previous studies suggests SP of 17-19‰ may be characteristic for N2O produced from SNCR. Methane emissions were found to be insignificant, with a maximum emission factor of 2.5 ± 5.6g CH4 t(-1) (0.2 ± 0.5g CH4 GJ(-1)), which is expected due to high incinerator temperatures and efficient combustion. Copyright © 2014 Elsevier Ltd

  11. Factors that control the stable carbon isotopic composition of methane produced in an anoxic marine sediment

    Science.gov (United States)

    Alperin, M. J.; Blair, Neal E.; Albert, D. B.; Hoehler, T. M.; Martens, C. S.

    1993-01-01

    The carbon isotopic composition of methane produced in anoxic marine sediment is controlled by four factors: (1) the pathway of methane formation, (2) the isotopic composition of the methanogenic precursors, (3) the isotope fractionation factors for methane production, and (4) the isotope fractionation associated with methane oxidation. The importance of each factor was evaluated by monitoring stable carbon isotope ratios in methane produced by a sediment microcosm. Methane did not accumulate during the initial 42-day period when sediment contained sulfate, indicating little methane production from 'noncompetitive' substrates. Following sulfate depletion, methane accumulation proceeded in three distinct phases. First, CO2 reduction was the dominant methanogenic pathway and the isotopic composition of the methane produced ranged from -80 to -94 per thousand. The acetate concentration increased during this phase, suggesting that acetoclastic methanogenic bacteria were unable to keep pace with acetate production. Second, acetate fermentation became the dominant methanogenic pathway as bacteria responded to elevated acetate concentrations. The methane produced during this phase was progressively enriched in C-13, reaching a maximum delta(C-13) value of -42 per thousand. Third, the acetate pool experienced a precipitous decline from greater than 5 mM to less than 20 micro-M and methane production was again dominated by CO2 reduction. The delta(C-13) of methane produced during this final phase ranged from -46 to -58 per thousand. Methane oxidation concurrent with methane production was detected throughout the period of methane accumulation, at rates equivalent to 1 to 8 percent of the gross methane production rate. Thus methane oxidation was too slow to have significantly modified the isotopic signature of methane. A comparison of microcosm and field data suggests that similar microbial interactions may control seasonal variability in the isotopic composition of methane

  12. Methane and nitrous oxide emissions from livestock agriculture in 16 local administrative districts of Korea.

    Science.gov (United States)

    Ji, Eun Sook; Park, Kyu-Hyun

    2012-12-01

    This study was conducted to evaluate methane (CH4) and nitrous oxide (N2O) emissions from livestock agriculture in 16 local administrative districts of Korea from 1990 to 2030. National Inventory Report used 3 yr averaged livestock population but this study used 1 yr livestock population to find yearly emission fluctuations. Extrapolation of the livestock population from 1990 to 2009 was used to forecast future livestock population from 2010 to 2030. Past (yr 1990 to 2009) and forecasted (yr 2010 to 2030) averaged enteric CH4 emissions and CH4 and N2O emissions from manure treatment were estimated. In the section of enteric fermentation, forecasted average CH4 emissions from 16 local administrative districts were estimated to increase by 4%-114% compared to that of the past except for Daejeon (-63%), Seoul (-36%) and Gyeonggi (-7%). As for manure treatment, forecasted average CH4 emissions from the 16 local administrative districts were estimated to increase by 3%-124% compared to past average except for Daejeon (-77%), Busan (-60%), Gwangju (-48%) and Seoul (-8%). For manure treatment, forecasted average N2O emissions from the 16 local administrative districts were estimated to increase by 10%-153% compared to past average CH4 emissions except for Daejeon (-60%), Seoul (-4.0%), and Gwangju (-0.2%). With the carbon dioxide equivalent emissions (CO2-Eq), forecasted average CO2-Eq from the 16 local administrative districts were estimated to increase by 31%-120% compared to past average CH4 emissions except Daejeon (-65%), Seoul (-24%), Busan (-18%), Gwangju (-8%) and Gyeonggi (-1%). The decreased CO2-Eq from 5 local administrative districts was only 34 kt, which was insignificantly small compared to increase of 2,809 kt from other 11 local administrative districts. Annual growth rates of enteric CH4 emissions, CH4 and N2O emissions from manure management in Korea from 1990 to 2009 were 1.7%, 2.6%, and 3.2%, respectively. The annual growth rate of total CO2-Eq was 2

  13. Oxidative coupling of methane. Still a challenge for catalyst development and reaction engineering

    Energy Technology Data Exchange (ETDEWEB)

    Schomaecker, R.; Arnd, S.; Beck, B. [Technical Univ. of Berlin (Germany). Dept. of Chemistry] [and others

    2013-11-01

    The oxidative coupling of methane to ethylene offers great industrial potential, because it would broaden the feedstock basis for chemical industry. Because methane is the most stable hydrocarbon, its activation requires high temperatures and it is a great scientific challenge to overcome the apparent yield limit of about 25%. This barrier has never been exceeded since the beginning of OCM research more than 20 years ago. Results and Discussion: This challenge is one of the key projects of the Cluster of Excellence UNICAT and requires joined efforts and contributions from many disciplines, because this reaction shows a combined surface/gas phase reaction mechanism which results in very unusual and complex dependencies on the reaction conditions. Although dozens of materials are known to catalyze the reaction, the selection of a catalyst suitable for an industrial process is difficult, due to severe stability problems of many materials. Li/MgO was chosen by the UNICAT-team as model catalyst, because of the extended literature about it. But it shows uncontrollable deactivation, no matter what precursor and method were used for its preparation. Nevertheless, it is a suitable catalyst for fundamental studies, due to its formal chemical simplicity. A key result of the joined research activities was the disproval of the Lunsford mechanism and the elucidation of the real function of lithium as a surface modifier creating a rough and defect-rich surface. For the development of an OCM process another catalyst, Na{sub 2}WO{sub 4}/Mn/SiO{sub 2}, was chosen from the rich literature on OCM. Although less is known about its structure and the reaction mechanism at this catalyst, its stability was the most important reason to select it for further engineering studies. Kinetic isotope measurements and studies in a TAP reactor demonstrate the similarity of the reaction mechanisms at both catalysts, despite the completely different materials. The selectivity is largely controlled by

  14. Assessing the High Temperature, High Pressure Subsurface for Anaerobic Methane Oxidation

    Science.gov (United States)

    Harris, R. L.; Bartlett, D.; Byrnes, A. W.; Walsh, K. M.; Lau, C. Y. M.; Onstott, T. C.

    2017-12-01

    The anaerobic oxidation of methane (AOM) is an important sink in the global methane (CH4) budget. ANMEs are known to oxidize CH4 either independently or in consortia with bacteria, coupling the reduction of electron acceptors such as, SO42-, NO2-, NO3-, Mn4+, or Fe3+. To further constrain the contribution of AOM to the global CH4 budget, it is important to assess unexplored environments where AOM is thermodynamically possible such as the high pressure, high temperature deep biosphere. Provided plausible electron acceptor availability, increased temperature and pCH4 yield favorable Gibbs free energies for AOM reactions and the production of ATP (Fig. 1). To date, only sulfate-dependent AOM metabolism has been documented under high temperature conditions (50-72˚C), and AOM has not been assessed above 10.1 MPa. Given that ANMEs share close phylogenetic and metabolic heritage with methanogens and that the most heat-tolerant microorganism known is a barophilic methanogen, there possibly exist thermophilic ANMEs. Here we describe preliminary results from high pressure, high temperature stable isotope tracer incubation experiments on deep biosphere samples. Deep sub-seafloor sediments collected by IODP 370 from the Nankai Trough (257 - 865 m below seafloor) and deep fracture fluid from South Africa (1339 m below land surface) were incubated anaerobically in hydrostatic pressure vessels at 40 MPa in simulated in situ temperatures (40˚ - 80˚C). Sediments and fracture fluid were incubated in sulfate-free artificial seawater, a 2:98 13CH4:N2 headspace, and treated with one of the potential electron acceptors listed above in addition to kill and endogenous activity (i.e. no added electron acceptor) controls. Stable isotope analysis of dissolved inorganic carbon (DIC) suggests that AOM occurred within 60 days of incubation for all investigated electron acceptors and temperatures except 50˚C. Sulfate-dependent AOM rates are consistent with those previously reported in the

  15. Nitrous oxide and methane emissions and nitrous oxide isotopic composition from waste incineration in Switzerland

    Energy Technology Data Exchange (ETDEWEB)

    Harris, Eliza, E-mail: eliza.harris@empa.ch [Empa, Laboratory for Air Pollution and Environmental Technology, Überlandstrasse 129, CH-8600 Dübendorf (Switzerland); Zeyer, Kerstin [Empa, Laboratory for Air Pollution and Environmental Technology, Überlandstrasse 129, CH-8600 Dübendorf (Switzerland); Kegel, Rainer; Müller, Beat [FOEN, Federal Office for the Environment, Air Pollution Control and Chemicals, CH-3003 Berne (Switzerland); Emmenegger, Lukas; Mohn, Joachim [Empa, Laboratory for Air Pollution and Environmental Technology, Überlandstrasse 129, CH-8600 Dübendorf (Switzerland)

    2015-01-15

    plants with SNCR, which had considerable N{sub 2}O emissions, was measured using quantum cascade laser spectroscopy. The isotopic site preference of N{sub 2}O – the enrichment of {sup 14}N{sup 15}NO relative to {sup 15}N{sup 14}NO – was found to be 17.6 ± 0.8‰, with no significant difference between the two plants. Comparison to previous studies suggests SP of 17–19‰ may be characteristic for N{sub 2}O produced from SNCR. Methane emissions were found to be insignificant, with a maximum emission factor of 2.5 ± 5.6 g CH{sub 4} t{sup −1} (0.2 ± 0.5 g CH{sub 4} GJ{sup −1}), which is expected due to high incinerator temperatures and efficient combustion.

  16. Formation of polycyclic aromatic hydrocarbons and soot in fuel-rich oxidation of methane in a laminar flow reactor

    DEFF Research Database (Denmark)

    Skjøth-Rasmussen, Martin Skov; Glarborg, Peter; Østberg, M.

    2004-01-01

    Conversion of methane to higher hydrocarbons, polycyclic aromatic hydrocarbons (PAHs), and soot was investigated under fuel-rich conditions in a laminar flow reactor. The effects of stoichiometry, dilution, and water vapor addition were studied at temperatures between 1073 and 1823 K. A chemical...... kinetic mechanism was established for methane oxidation, with emphasis on formation of higher hydrocarbons and PAH. A submodel for soot formation was adopted from the work of Frenklach and co-workers without changes. Modeling predictions showed good agreement with experimental results. Reactants, stable...... decrease with increasing addition of water vapor. The effect is described qualitatively by the reaction mechanism. The enhanced oxidation of acetylene is attributed to higher levels of hydroxyl radicals, formed from the reaction between the water vapor and hydrogen atoms....

  17. Anaerobic oxidation of methane and sulfate reduction along the Chilean continental margin

    DEFF Research Database (Denmark)

    Treude, T.; Niggemann, J.; Kallmeyer, J.

    2005-01-01

    of AOM and SR activity, methane, sulfate, sulfide, pH, total chlorins, and a variety of other geochemical parameters. Depth-integrated rates of AOM within the SMT were between 7 and 1124 mmol m(-2) a(-1), effectively removing methane below the sediment-water interface. Single measurements revealed AOM...... with high organic input, to analyze the impact of AOM on the methane budget, and to determine the contribution of AOM to SR within the sulfate-methane transition zone (SMT). Furthermore, we investigated the formation of authigenic carbonates correlated with AOM. We determined the vertical distribution...

  18. Oscillatory behaviour of catalytic properties, structure and temperature during the catalytic partial oxidation of methane on Pd/Al2O3

    DEFF Research Database (Denmark)

    Kimmerle, B.; Baiker, A.; Grunwaldt, Jan-Dierk

    2010-01-01

    Pd/Al2O3 catalysts showed an oscillatory behaviour during the catalytic partial oxidation (CPO) of methane, which was investigated simultaneously by IR-thermography, X-ray absorption spectroscopy, and online mass-spectrometry to correlate the temperature, state of the catalyst and catalytic...... to self-reduction leading to extinction of the process. The latter was the key driver for the oscillations and thus gave additional insight into the mechanism of partial methane oxidation....

  19. Sulfate reduction and methane oxidation activity below the sulfate-methane transition zone in Alaskan Beaufort Sea continental margin sediments: Implications for deep sulfur cycling

    Science.gov (United States)

    Treude, Tina; Krause, Stefan; Maltby, Johanna; Dale, Andrew W.; Coffin, Richard; Hamdan, Leila J.

    2014-11-01

    Two ∼6 m long sediment cores were collected along the ∼300 m isobath on the Alaskan Beaufort Sea continental margin. Both cores showed distinct sulfate-methane transition zones (SMTZ) at 105 and 120 cm below seafloor (cmbsf). Sulfate was not completely depleted below the SMTZ but remained between 30 and 500 μM. Sulfate reduction and anaerobic oxidation of methane (AOM) determined by radiotracer incubations were active throughout the methanogenic zone. Although a mass balance could not explain the source of sulfate below the SMTZ, geochemical profiles and correlation network analyses of biotic and abiotic data suggest a cryptic sulfur cycle involving iron, manganese and barite. Inhibition experiments with molybdate and 2-bromoethanesulfonate (BES) indicated decoupling of sulfate reduction and AOM and competition between sulfate reducers and methanogens for substrates. While correlation network analyses predicted coupling of AOM to iron reduction, the addition of manganese or iron did not stimulate AOM. Since none of the classical archaeal anaerobic methanotrophs (ANME) were abundant, the involvement of unknown or unconventional phylotypes in AOM is conceivable. The resistance of AOM activity to inhibitors implies deviation from conventional enzymatic pathways. This work suggests that the classical redox cascade of electron acceptor utilization based on Gibbs energy yields does not always hold in diffusion-dominated systems, and instead biotic processes may be more strongly coupled to mineralogy.

  20. Assessment of substrate potential resources which can be used in methanization - Final report

    International Nuclear Information System (INIS)

    Bastide, Guillaume

    2013-04-01

    This report proposes a method to elaborate a detailed and precise assessment of potential resources of substrates which can be used for methanization. It aims at obtaining global results at the national level while proposing figures at the district level which can be integrated into regional documents. Four types of resources have been addressed: the production raw resource, the available raw resource, the available net resource, and the mobilisable resource by 2030. These resources have different origins: agriculture (breeding effluents, crop residues, energetic intermediate crops), various agri-food industries, sanitation systems, green wastes, and bio-wastes from different origins (restaurants, small shops, retail trade, markets). Some other sources (green algae, micro-algae, roadside grass, meadows, farming fruits and vegetables) have only been identified but are considered as experiments or difficult to be assessed

  1. Eddy covariance observations of methane and nitrous oxide emissions. Towards more accurate estimates from ecosystems

    International Nuclear Information System (INIS)

    Kroon, P.S.

    2010-09-01

    About 30% of the increased greenhouse gas (GHG) emissions of carbon dioxide (CO2), methane (CH4) and nitrous oxide (N2O) are related to land use changes and agricultural activities. In order to select effective measures, knowledge is required about GHG emissions from these ecosystems and how these emissions are influenced by management and meteorological conditions. Accurate emission values are therefore needed for all three GHGs to compile the full GHG balance. However, the current annual estimates of CH4 and N2O emissions from ecosystems have significant uncertainties, even larger than 50%. The present study showed that an advanced technique, micrometeorological eddy covariance flux technique, could obtain more accurate estimates with uncertainties even smaller than 10%. The current regional and global trace gas flux estimates of CH4 and N2O are possibly seriously underestimated due to incorrect measurement procedures. Accurate measurements of both gases are really important since they could even contribute for more than two-third to the total GHG emission. For example: the total GHG emission of a dairy farm site was estimated at 16.10 3 kg ha -1 yr -1 in CO2-equivalents from which 25% and 45% was contributed by CH4 and N2O, respectively. About 60% of the CH4 emission was emitted by ditches and their bordering edges. These emissions are not yet included in the national inventory reports. We recommend including these emissions in coming reports.

  2. [Comparative characterization of cultured methane-oxidizing bacteria by serological and molecular methods].

    Science.gov (United States)

    Slobodova, N V; Kolganova, T V; Bulygina, E S; Kuznetsov, B B; Turova, T P; Kravchenko, I K

    2006-01-01

    Three stable methane-oxidizing enrichment cultures, SB26, SB31, and SB31A were analyzed by transmission electron microscopy and by serological and molecular techniques. Electron microscopy revealed the presence of both type I and type II methanotrophs in SB31 and SB31A enrichments; only type II methanotrophs were found in SB26 enrichment. Methylosinus trichosporium was detected in all three enrichments by the application of species-specific antibodies. Additionally, Methylocystis echinoides was found in SB26 culture; Methylococcus capsulatus, in SB31 and SB31A; and Methylomonas methanica, in SB31. The analysis with pmoA and nifH gene sequences as phylogenetic markers revealed the presence of Methylosinus/Methylocystis group in all communities. Moreover, the analysis of pmoA sequences revealed the presence of Methylomonas in SB31. Methylocella was detected in SB31 and SB31A enrichments only by nifH analysis. It was concluded that the simultaneous application of different approaches reveals more reliable information on the diversity of methanotrophs.

  3. Ecosystem respiration, methane and nitrous oxide fluxes from ecotopes in a rewetted extracted peatland in Sweden

    Directory of Open Access Journals (Sweden)

    S. Jordan

    2016-09-01

    Full Text Available Ecosystem respiration (carbon dioxide; CO2, methane (CH4 and nitrous oxide (N2O fluxes to the atmosphere were determined using an opaque closed chamber method within various ecotopes (vegetation covered, bare peat and open water in a rewetted extracted peatland and within an adjacent open poor fen in Sweden. Ecotopes had a significant impact on CO2 and CH4 fluxes to the atmosphere. Ecosystem respiration and CH4 emissions from the bare peat site, the constructed shallow lake and the open poor fen were low but were much higher from ecotopes with Eriophorum vaginatum tussocks and Eriophorum angustifolium. A combination of vascular plant cover and high soil temperatures enhanced ecosystem respiration, while a combination of vascular plant cover, high water table levels and high soil temperatures enhanced CH4 emissions. N2O emissions contributed little to total greenhouse gas (GHG fluxes from the soil-plant-water systems to the atmosphere. However, the overall climate impact of CH4 emissions from the study area did not exceed the impact of soil and plant respiration. With regard to management of extracted peatlands, the construction of a nutrient-poor shallow lake showed great potential for lowering GHG fluxes to the atmosphere.

  4. Activity and diversity of methane-oxidizing bacteria along a Norwegian sub-Arctic glacier forefield.

    Science.gov (United States)

    Mateos-Rivera, Alejandro; Øvreås, Lise; Wilson, Bryan; Yde, Jacob C; Finster, Kai W

    2018-05-01

    Methane (CH4) is one of the most abundant greenhouse gases in the atmosphere and identification of its sources and sinks is crucial for the reliability of climate model outputs. Although CH4 production and consumption rates have been reported from a broad spectrum of environments, data obtained from glacier forefields are restricted to a few locations. We report the activities of methanotrophic communities and their diversity along a chronosequence in front of a sub-Arctic glacier using high-throughput sequencing and gas flux measurements. CH4 oxidation rates were measured in the field throughout the growing season during three sampling times at eight different sampling points in combination with laboratory incubation experiments. The overall results showed that the methanotrophic community had similar trends of increased CH4 consumption and increased abundance as a function of soil development and time of year. Sequencing results revealed that the methanotrophic community was dominated by a few OTUs and that a short-term increase in CH4 concentration, as performed in the field measurements, altered slightly the relative abundance of the OTUs.

  5. Stimulation by ammonium-based fertilizers of methane oxidation in soil around rice roots

    NARCIS (Netherlands)

    Bodelier, P.L.E.; Roslev, P.; Henckel, T.; Frenzel, P.

    2000-01-01

    Methane is involved in a number of chemical and physical processes in the Earths atmosphere, including global warming(1), Atmospheric methane originates mainly from biogenic sources, such as rice paddies and natural wetlands; the former account for at least 30% of the global annual emission of

  6. Kinetic Studies of Oxidative Coupling of Methane Reaction on Model Catalysts

    KAUST Repository

    Khan, Abdulaziz M.

    2016-04-26

    With the increasing production of natural gas as a result of the advancement in the technology, methane conversion to more valuable products has become a must. One of the most attractive processes which allow the utilization of the world’s most abundant hydrocarbon is the oxidative coupling. The main advantage of this process is the ability of converting methane into higher paraffins and olefins (primarily C2) in a direct way using a single reactor. Nevertheless, low C2+ yields have prevented the process to be commercialized despite the fact that great number of attempts to prepare catalysts were conducted so that it can be economically viable. Due to these limitations, understanding the mechanism and kinetics of the reaction can be utilized in improving the catalysts’ performance. The reaction involves the formation of methyl radicals that undergo gas-phase radical reactions. CH4 activation is believed to be done the surface oxygen species. However, recent studies showed that, in addition to the surface oxygen mediated pathway, an OH radical mediated pathway have a large contribution on the CH4 activation. The experiments of Li/MgO, Sr/La2O3 and NaWO4/SiO2 catalysts revealed variation of behavior in activity and selectivity. In addition, water effect analysis showed that Li/MgO deactivate at the presence of water due to sintering phenomena and the loss of active sites. On the other hand, negative effect on the C2 yield and CH4 conversion rate was observed with Sr/La2O3 with increasing the water partial pressure. Na2WO4/SiO2 showed a positive behavior with water in terms of CH4 conversion and C2 yield. In addition, the increment in CH4 conversion rate was found to be proportional with PO2 ¼ PH2O ½ which is consistent with the formation of OH radicals and the OH-mediated pathway. Experiments of using ring-dye laser, which is used to detect OH in combustion experiments, were tried in order to detect OH radicals in the gas-phase of the catalyst. Nevertheless

  7. Mechanistic insights into heterogeneous methane activation

    International Nuclear Information System (INIS)

    Latimer, Allegra A.; Aljama, Hassan; Kakekhani, Arvin; Yoo, Jong Suk; Kulkarni, Ambarish

    2017-01-01

    While natural gas is an abundant chemical fuel, its low volumetric energy density has prompted a search for catalysts able to transform methane into more useful chemicals. This search has often been aided through the use of transition state (TS) scaling relationships, which estimate methane activation TS energies as a linear function of a more easily calculated descriptor, such as final state energy, thus avoiding tedious TS energy calculations. It has been shown that methane can be activated via a radical or surface-stabilized pathway, both of which possess a unique TS scaling relationship. Herein, we present a simple model to aid in the prediction of methane activation barriers on heterogeneous catalysts. Analogous to the universal radical TS scaling relationship introduced in a previous publication, we show that a universal TS scaling relationship that transcends catalysts classes also seems to exist for surface-stabilized methane activation if the relevant final state energy is used. We demonstrate that this scaling relationship holds for several reducible and irreducible oxides, promoted metals, and sulfides. By combining the universal scaling relationships for both radical and surface-stabilized methane activation pathways, we show that catalyst reactivity must be considered in addition to catalyst geometry to obtain an accurate estimation for the TS energy. Here, this model can yield fast and accurate predictions of methane activation barriers on a wide range of catalysts, thus accelerating the discovery of more active catalysts for methane conversion.

  8. Modelling TCE degradation by a mixed culture of methane-oxidizing bacteria

    DEFF Research Database (Denmark)

    Broholm, Kim; Christensen, Thomas Højlund; Jensen, Bjørn K.

    1992-01-01

    A model describing the growth of bacteria and the degradation of methane and trichloroethylene (TCE) based on the concept of competitive inhibition is proposed. The model has been applied to laboratory batch experiments representing different initial TCE concentrations (50–4300 μg/l) and initial...... methane concentrations (0.53–3.2 mg/l). The proposed model simulated successfully the data obtained for initial methane concentration (less than 1.8 mg/l), causing constant experimental growth conditions during the experiments. This indicates that the interactions between methane and TCE degradation can...... be explained as competitive inhibition. The model simulations of the results from the experiments with the highest initial methane concentration of 3.2 mg/l failed, supposedly because the growth conditions changed during the experiments. The proposed model is a useful engineering tool for design of treatment...

  9. Estimation of methane and nitrous oxide emission from livestock and poultry in China during 1949-2003

    Energy Technology Data Exchange (ETDEWEB)

    Zhou, J.B.; Jiang, M.M.; Chen, G.Q. [National Laboratory for Complex Systems and Turbulence, Department of Mechanics, Peking University, Beijing 100871 (China)

    2007-07-15

    To investigate the greenhouse gases emission from enteric fermentation and manure management of livestock and poultry industry in China, the present study presents a systematic estimation of methane and nitrous oxide emission during 1949-2003, based on the local measurement and IPCC guidelines. As far as greenhouse gases emission is concerned among livestock swine is found to hold major position followed by goat and sheep, while among poultry chicken has the major place and is followed by duck and geese. Methane emission from enteric fermentation is estimated to have increased from 3.04 Tg in 1949 to 10.13 Tg in 2003, an averaged annual growth rate of 2.2%, and methane emission from manure management has increased from 0.16 Tg in 1949 to 1.06 Tg in 2003, an annual growth rate of 3.5%, while nitrous oxide emission from manure management has increased from 47.76 to 241.2 Gg in 2003, with an annual growth rate of 3.0%. The total greenhouse gas emission has increased from 82.01 Tg CO{sub 2} Eq. in 1949 to 309.76 Tg CO{sub 2} Eq. in 2003, an annual growth rate of 2.4%. The estimation of livestock methane and nitrous oxide emissions in China from 1949 to 2003 is shown to be consistent with a linear growth model, and the reduction of greenhouse gas emission is thus considered an urgent and arduous task for the Chinese livestock industry. (author)

  10. Carbon and hydrogen isotope composition and C-14 concentration in methane from sources and from the atmosphere: Implications for a global methane budget. Final report, 1 January-30 June 1991

    International Nuclear Information System (INIS)

    Wahlen, M.

    1994-03-01

    The topics covered include the following: biogenic methane studies; forest soil methane uptake; rice field methane sources; atmospheric measurements; stratospheric samples; Antarctica; California; and Germany

  11. Market research on biogas valorizations and methanization. Final report; Etude de marche de la methanisation et des valorisations du biogaz. Rapport final

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2010-09-15

    This market research aims at giving an overview of the existing methanization installations and of their dynamics in France, at assessing biogas production and use, at analyzing the methanization market, and at defining development perspectives for this sector by 2020. Based on a survey of methanization installations, on interviews with many actors of this sector, and on a seminar organized on this topic, this report presents and comments market data for biogas valorization and methanization in different sectors: household, agricultural, and industrial and waste water processing plants. It comments evolution trends by 2020 for these sectors, and the role that the emerging sector of centralized methanization could have in the years to come

  12. Fluxes of methane and nitrogen oxides in various boreal mire ecosystems. Effects of land-use activities and environmental changes

    International Nuclear Information System (INIS)

    Martikainen, P.J.; Nykaenen, H.; Regina, K.; Alm, J.; Silvola, J.

    1996-01-01

    Atmospheric impact of peatlands is a sum of their gas fluxes. In contrast to carbon dioxide, peatlands are net sources for methane (CH 4 ). Methane is an end product in the anaerobic decomposition processes and it has greater capacity to absorb infrared radiation than carbon dioxide. Most of the data on the CH 4 release from northern peatlands is from North America. The total amount of methane released from wetlands is calculated to be 110 Tg yr -1 of which 34 percent (38 Tg yr -1 ) is estimated to be emitted from the northern peatlands. Peat with high content of nitrogen is a potential source for gaseous nitrogen oxides, i.e. nitrous oxide (N 2 O) and nitric oxide (NO). However, the importance of peatlands in producing these trace gases is poorly known. Nitrous oxide and nitric oxide are important components in the atmospheric chemistry and N 2 O also is an effective greenhouse gas. Land-use activities and environmental changes can affect the atmospheric impacts of peatlands by modifying their biogeochemistry. This article presents a short summary of the studies whose objectives were: (1) to measure fluxes of CH 4 and N 2 O on wide range of natural mires in Finland, (2) to study the short- and long-term changes in fluxes of CH 4 , N 2 O and NO on boreal peatlands after lowering their water table. Peatlands used for agriculture, forestry and peat mining were included in the studies. The results from mires drained for forestry may reflect the possible changes in the trace gas fluxes if water table will drop in the northern peatlands as a result of drier climate, (3) to study the effects of nitrogen load on the fluxes of CH 4 , N 2 O and NO, (4) to identify the microbiological processes important for the fluxes of N 2 O, NO and CH 4 , and to study the environmental factors regulating these microbial processes

  13. Methane and Nitrous Oxide Emissions from Agriculture on a Regional Scale

    Directory of Open Access Journals (Sweden)

    Agnieszka Wysocka-Czubaszek

    2018-05-01

    Full Text Available Nowadays, agriculture has to meet the growing food demand together with high requirements of environmental protection, especially regarding the climate change. The greenhouse gas emissions differ not only on a global, but also on a regional scale, and mitigation strategies are effective when they are adapted properly. Therefore, the aim of this paper is to present the results of methane (CH4 and nitrous oxide (N2O emissions inventory on a regional level in Poland in years 1999-2015. The CH4 and N2O emissions were calculated according to the methodology used by the National Centre for Emissions Management (NCEM for national inventory for United Nations Framework Convention on Climate Change and Kyoto Protocol. The data were taken from Central Statistical Office of Poland. The CH4 emissions in all studied years varied strongly between voivodeships and ranged from 5.6-7.5 Gg y-1 in the Lubuskie Voivodeship to 84.8-104.3 Gg y-1 in the Mazowieckie Voivodeship. While in most voivodeships the CH4 emissions dropped down, in Podlaskie, Mazursko-Warmińskie, and Wielkopolskie voivodeships, the emissions of this gas increased significantly as a consequence of the development of dairy and meat production. In 1999, the highest N2O fluxes were calculated for the Wielkopolskie (5.7 Gg y-1, Mazowieckie (4.8 Gg y-1 Kujawsko-Pomorskie (3.5 Gg y-1 and Lubelskie (3.3 Gg y-1 voivodeships, while in 2015, the highest nitrous oxide emissions were calculated for the Wielkopolskie (7.3 Gg y-1, Mazowieckie (5.5 Gg y-1, Kujawsko-Pomorskie (4.1 Gg y-1 and Podlaskie (4.1 Gg y-1 voivodeships. In the studied period, the contribution of N2O emissions from crop production increased in almost all voivodeships except the Podlaskie, Lubuskie and Warmińsko-Mazurskie regions. The growth in emissions from mineral fertilization and crop residue incorporation, together with the increase of emission from the animal sector in some regions of Poland, resulted in the higher national

  14. Spatial and temporal distribution of nitrite-dependent anaerobic methane-oxidizing bacteria in an intertidal zone of the East China Sea.

    Science.gov (United States)

    Wang, Jiaqi; Shen, Lidong; He, Zhanfei; Hu, Jiajie; Cai, Zhaoyang; Zheng, Ping; Hu, Baolan

    2017-11-01

    Nitrite-dependent anaerobic methane oxidation (N-DAMO), which couples anaerobic methane oxidation and nitrite reduction, is a recently discovered bioprocess coupling microbial nitrogen and carbon cycles. The discovery of this microbial process challenges the traditional knowledge of global methane sinks and nitrogen losses. In this study, the abundance and activity of N-DAMO bacteria were investigated and their contributions to methane sink and nitrogen loss were estimated in different seasons and different partitions of an intertidal zone of the East China Sea. The results showed that N-DAMO bacteria were extensively and continuously present in the intertidal zone, with the number of cells ranging from 5.5 × 10 4 to 2.8 × 10 5 copy g -1 soil and the potential activity ranging from 0.52 to 5.7 nmol CO 2  g -1 soil day -1 , contributing 5.0-36.6% of nitrite- and sulfate-dependent anaerobic methane oxidation in the intertidal zone. The N-DAMO activity and its contribution to the methane consumption were highest in the spring and in the low intertidal zone. These findings showed that the N-DAMO process is an important methane and nitrogen sink in the intertidal zone and varies with the seasons and the partitions of the intertidal zone.

  15. Analysis of uncertainties in the estimates of nitrous oxide and methane emissions in the UK's greenhouse gas inventory for agriculture

    Science.gov (United States)

    Milne, Alice E.; Glendining, Margaret J.; Bellamy, Pat; Misselbrook, Tom; Gilhespy, Sarah; Rivas Casado, Monica; Hulin, Adele; van Oijen, Marcel; Whitmore, Andrew P.

    2014-01-01

    The UK's greenhouse gas inventory for agriculture uses a model based on the IPCC Tier 1 and Tier 2 methods to estimate the emissions of methane and nitrous oxide from agriculture. The inventory calculations are disaggregated at country level (England, Wales, Scotland and Northern Ireland). Before now, no detailed assessment of the uncertainties in the estimates of emissions had been done. We used Monte Carlo simulation to do such an analysis. We collated information on the uncertainties of each of the model inputs. The uncertainties propagate through the model and result in uncertainties in the estimated emissions. Using a sensitivity analysis, we found that in England and Scotland the uncertainty in the emission factor for emissions from N inputs (EF1) affected uncertainty the most, but that in Wales and Northern Ireland, the emission factor for N leaching and runoff (EF5) had greater influence. We showed that if the uncertainty in any one of these emission factors is reduced by 50%, the uncertainty in emissions of nitrous oxide reduces by 10%. The uncertainty in the estimate for the emissions of methane emission factors for enteric fermentation in cows and sheep most affected the uncertainty in methane emissions. When inventories are disaggregated (as that for the UK is) correlation between separate instances of each emission factor will affect the uncertainty in emissions. As more countries move towards inventory models with disaggregation, it is important that the IPCC give firm guidance on this topic.

  16. Simultaneous enrichment of denitrifying anaerobic methane-oxidizing microorganisms and anammox bacteria in a hollow-fiber membrane biofilm reactor.

    Science.gov (United States)

    Ding, Zhao-Wei; Lu, Yong-Ze; Fu, Liang; Ding, Jing; Zeng, Raymond J

    2017-01-01

    In this study, the coculture system of denitrifying anaerobic methane oxidation (DAMO) microbes and anaerobic ammonium oxidation (anammox) bacteria was successfully enriched in a hollow-fiber membrane biofilm reactor (HfMBR) using freshwater sediment as the inoculum. The maximal removal rates of nitrate and ammonium were 78 mg N/L/day (131 mg N/m 2 /day) and 26 mg N/L/day (43 mg N/m 2 /day), respectively. Due to the high rate of methane mass transfer in HfMBR, the activity of DAMO archaea continued to increase during the enrichment period, indicating that HfMBR could be a powerful tool to enrich DAMO microorganisms. Effects of partial methane pressure, temperature, and pH on the cocultures were obvious. However, the microbial activity in HfMBR could be recovered quickly after the shock change of environmental factors. Furthermore, the result also found that DAMO bacteria likely had a stronger competitive advantage than anammox bacteria under the operating conditions in this study. High-throughput sequencing 16S rRNA genes illustrated that the dominant microbes were NC10, Euryarchaeota, Proteobacteria, Planctomycetes, and Chlorobi with relative abundance of 38.8, 26.2, 13.78, 6.2, and 3.6 %, respectively.

  17. Subgroup characteristics of marine methane-oxidizing ANME-2 archaea and their syntrophic partners revealed by integrated multimodal analytical microscopy.

    Science.gov (United States)

    McGlynn, Shawn E; Chadwick, Grayson L; O'Neill, Ariel; Mackey, Mason; Thor, Andrea; Deerinck, Thomas J; Ellisman, Mark H; Orphan, Victoria J

    2018-04-06

    Phylogenetically diverse environmental ANME archaea and sulfate-reducing bacteria cooperatively catalyze the anaerobic oxidation of methane oxidation (AOM) in multi-celled consortia within methane seep environments. To better understand these cells and their symbiotic associations, we applied a suite of electron microscopy approaches including correlative f luorescence i n s itu h ybridization - e lectron m icroscopy (FISH-EM), t ransmission e lectron m icroscopy (TEM), and s erial b lock face scanning e lectron m icroscopy 3D reconstructions (SBEM). FISH-EM of methane seep derived consortia revealed phylogenetic variability in terms of cell morphology, ultrastructure, and storage granules. Representatives of the ANME-2b clade, but not other ANME-2 groups, contained polyphosphate-like granules, while some bacteria associated with ANME-2a/2c contained two distinct phases of iron mineral chains resembling magnetosomes. 3D segmentation of two ANME-2 consortia types revealed cellular volumes of ANME and their symbiotic partners which were larger than previous estimates based on light microscopy. Phosphorous granule containing ANME (tentatively ANME-2b) were larger than both ANME with no granules and partner bacteria. This cell type was observed with up to 4 granules per cell and the volume of the cell was larger in proportion to the number of granules inside it, but the percent of the cell occupied by these granules did not vary with granule number. These results illuminate distinctions between ANME-2 archaeal lineages and partnering bacterial populations that are apparently unified in their capability of performing anaerobic methane oxidation. Importance Methane oxidation in anaerobic environments can be accomplished by a number of archaeal groups, some of which live in syntrophic relationships with bacteria in structured consortia. Little is known as to the distinguishing characteristics of these groups. Here we applied imaging approaches to better understand the

  18. Co-existence of Anaerobic Ammonium Oxidation Bacteria and Denitrifying Anaerobic Methane Oxidation Bacteria in Sewage Sludge: Community Diversity and Seasonal Dynamics

    DEFF Research Database (Denmark)

    Xu, Sai; Lu, Wenjing; Mustafa, Muhammad Farooq

    2017-01-01

    Anaerobic ammonium oxidation (ANAMMOX) and denitrifying anaerobic methane oxidation (DAMO) have been recently discovered as relevant processes in the carbon and nitrogen cycles of wastewater treatment plants. In this study, the seasonal dynamics of ANAMMOX and DAMO bacterial community structures......, and an unknown cluster was primarily detected in autumn and winter. Similar patterns of seasonal variation in the community structure of DAMO bacteria were also observed. Group B was the dominant in spring and summer, whereas in autumn and winter, group A and group B presented almost the same proportion...

  19. Quantification of Methane and Nitrous Oxide Emissions from Wastewater Collection Systems (Cincinnati, Ohio, USA)

    Science.gov (United States)

    Fries, A. E.; Townsend-Small, A.; Shuster, W.; Schifman, L. A.

    2016-12-01

    Greenhouse gas emissions from urban areas is an emerging topic in environmental science, but source apportionment of these emissions, particularly for methane (CH4) and nitrous oxide (N2O), is still underway. Here we present an analysis of CH4 and N2O sources from urban pipelines in Cincinnati, Ohio, USA. Leaks from manholes and sewer grates in Cincinnati are found by using a Bascom Turner Gas Rover to indicate CH4 enhancements, along with spatial data for CH4 enhancements at street level from previously published work. When possible, the atmospheric flux of CH4 and N2O of these leaks are quantified by using a flux chamber method. Source apportionment is determined by using carbon and hydrogen stable isotope ratios (13C and D) and CH4 to N2O ratios. Biogenic CH4 has a δ13C of approximately -55‰ and δD of approximately -270‰, whereas thermogenic CH4 has a δ13C of approximately -45‰ and δD of approximately -150‰. Biogenic CH4 may also co-occur with N2O, whereas thermogenic natural gas does not contain N2O. Contrary to our expectations, we found a portion of CH4 enhancements that are biogenic CH4, presumably from sewer gas, whereas most studies have assumed them to be natural gas leaks. In the future we will be working on determining the exact proportion of biogenic and thermogenic CH4 in street leaks and further quantifying CH4 and N2O emissions throughout Cincinnati. Our work indicates that CH4 leaks in cities may be a mixture of sewer gas and natural gas, especially in cities like Cincinnati where natural gas pipelines have been replaced with less leak-prone pipe materials.

  20. Stable isotopic indicators of nitrous oxide and methane sources in Los Angeles, California

    Science.gov (United States)

    Townsend-Small, A.; Pataki, D.; Tyler, S.; Trumbore, S.

    2008-12-01

    As urbanization increasingly encroaches upon agricultural landscapes, there are greater potential sources of greenhouse gases and other atmospheric contaminants. Measurements of the isotopic composition of trace gases have the potential to distinguish between pollutant sources and quantify the proportional contribution of agricultural activities to the total atmospheric pool. In this study, we are measuring the isotopic composition of greenhouse gases N2O and CH4 emitted from cropland, animal feeding operations, and urban activities in the South Coast Air Basin in southern California. The ultimate goal of our project is to utilize atmospheric measurements of the isotopic composition of N2O and CH4 combined with studies of source signatures to determine the proportional contributions of cropland, animal operations, and urban sources of greenhouse gases to the atmosphere. Measurements of the δ13C of methane show excellent separation between urban sources, such as vehicle emissions, power plants, oil refineries, landfills, and sewage treatment plants and agricultural sources like cows, biogas, and cattle feedlots. For nitrous oxide, soil N2O sources showed good separation from wastewater treatment facilities using δ15N and δ18O. Within soil N2O sources, the isotopic composition of N2O from cropland soils was similar to N2O emissions from urban turfgrass. These data indicate that nitrification may be as important a source of N2O as denitrification in urban soils. We are also measuring N2O fluxes from soils and from sewage treatment processes, and preliminary data indicate that urban N2O fluxes are higher than initially assumed by managers and regulatory agencies.

  1. Nitrous oxide and methane fluxes in six different land use systems in the Peruvian Amazon

    Science.gov (United States)

    Palm, C. A.; Alegre, J. C.; Arevalo, L.; Mutuo, P. K.; Mosier, A. R.; Coe, R.

    2002-12-01

    The contribution of different land-use systems in the humid tropics to increasing atmospheric trace gases has focused on forests, pastures, and crops with few measurements from managed, tree-based systems that dominate much of the landscape. This study from the Peruvian Amazon includes monthly nitrous oxide and methane fluxes from two cropping systems, three tree-based systems, and a 23-year secondary forest control. Average N2O fluxes from the cropping systems were two to three times higher than the secondary forest control (9.1 μg N m-2 h-1), while those of the tree-based systems were similar to the secondary forest. Increased fluxes in the cropping systems were attributed to N fertilization, while fluxes from the tree-based systems were related to litterfall N. Average CH4 consumption was reduced by up to half that of the secondary forest (-30.0 μg C m-2 h-1) in the tree-based and low-input cropping systems. There was net CH4 production in the high-input cropping system. This switch to net production was a result of increased bulk density and increased soil respiration resulting in anaerobic conditions. Reduced rates of N2O emissions, similar CH4 consumption, and high C sequestration rates in these tree-based systems compared with mature forests, coupled with the large area of these systems in the humid tropics, may partially offset the past effects of deforestation on increased atmospheric trace gas concentrations. In contrast, cropping systems with higher N2O emissions, substantially reduced CH4 consumption or even net CH4 emissions, and little C sequestration exacerbate those effects.

  2. Density functional theory analysis of the reaction pathway for methane oxidation to acetic acid catalyzed by Pd2+ in sulfuric acid.

    Science.gov (United States)

    Chempath, Shaji; Bell, Alexis T

    2006-04-12

    Density functional theory has been used to investigate the thermodynamics and activation barriers associated with the direct oxidation of methane to acetic acid catalyzed by Pd2+ cation in concentrated sulfuric acid. Pd2+ cations in such solutions are ligated by two bisulfate anions and by one or two molecules of sulfuric acid. Methane oxidation is initiated by the addition of CH4 across one of the Pd-O bonds of a bisulfate ligand to form Pd(HSO4)(CH3)(H2SO4)2. The latter species will react with CO to produce Pd(HSO4)(CH3CO)(H2SO4)2. The most likely path to the final products is found to be via oxidation of Pd(HSO4)(CH3)(H2SO4)2 and Pd(HSO4)(CH3CO)(H2SO4)2 to form Pd(eta2-HSO4)(HSO4)2(CH3)(H2SO4) and Pd(eta2-HSO4)(HSO4)2(CH3CO)(H2SO4), respectively. CH3HSO4 or CH3COHSO4 is then produced by reductive elimination from the latter two species, and CH(3)COOH is then formed by hydrolysis of CH3COHSO4. The loss of Pd2+ from solution to form Pd(0) or Pd-black is predicted to occur via reduction with CO. This process is offset, though, by reoxidation of palladium by either H2SO4 or O2.

  3. Reaction phenomena of catalytic partial oxidation of methane under the impact of carbon dioxide addition and heat recirculation

    International Nuclear Information System (INIS)

    Chen, Wei-Hsin; Lin, Shih-Cheng

    2015-01-01

    The reaction phenomena of CPOM (catalytic partial oxidation of methane) in a Swiss-roll reactor are studied numerically where a rhodium-based catalyst bed is embedded at the center of the reactor. CO 2 is added into the feed gas and excess enthalpy recovery is performed to evaluate their influences on CPOM performance. In the study, the mole ratio of O 2 to CH 4 (O 2 /CH 4 ratio) is fixed at 0.5 and the mole ratio of CO 2 to O 2 (CO 2 /O 2 ratio) is in the range of 0–2. The results reveal that CO 2 addition into the influent has a slight effect on methane combustion, but significantly enhances dry reforming and suppresses steam reforming. The reaction extents of steam reforming and dry reforming in CPOM without heat recovery and CO 2 addition are in a comparable state. Once CO 2 is added into the feed gas, the dry reforming is enhanced, thereby dominating CH 4 consumption. Compared to the reactor without excess enthalpy recovery, heat recirculation drastically increases the maximum reaction temperature and CH 4 conversion in the catalyst bed; it also intensifies the H 2 selectivity, H 2 yield, CO 2 conversion, and syngas production rate. The predictions indicate that the heat recirculation is able to improve the syngas formation up to 45%. - Highlights: • Catalytic partial oxidation of methane with CO 2 addition and heat recovery is studied. • CO 2 addition has a slight effect on methane combustion. • CO 2 addition significantly enhances dry reforming and suppresses steam reforming. • Dry reforming dominates CH 4 consumption when CO 2 addition is large. • Heat recirculation can improve the syngas formation up to 45%

  4. Evidence of sulfate-dependent anaerobic methane oxidation... Wolfe & Wilkin data table vers 1

    Data.gov (United States)

    U.S. Environmental Protection Agency — Data file (.csv) including data plotted in manuscript figures: methane and sulfate concentrations, and stable isotope data for carbon, hydrogen, sulfur, and oxygen....

  5. Magnesium carbide synthesis from methane and magnesium oxide - a potential methodology for natural gas conversion to premium fuels and chemicals

    Energy Technology Data Exchange (ETDEWEB)

    Diaz, A.F.; Modestino, A.J.; Howard, J.B. [Massachusetts Institute of Technology, Cambridge, MA (United States)] [and others

    1995-12-31

    Diversification of the raw materials base for manufacturing premium fuels and chemicals offers U.S. and international consumers economic and strategic benefits. Extensive reserves of natural gas in the world provide a valuable source of clean gaseous fuel and chemical feedstock. Assuming the availability of suitable conversion processes, natural gas offers the prospect of improving flexibility in liquid fuels and chemicals manufacture, and thus, the opportunity to complement, supplement, or displace petroleum-based production as economic and strategic considerations require. The composition of natural gas varies from reservoir to reservoir but the principal hydrocarbon constituent is always methane (CH{sub 4}). With its high hydrogen-to-carbon ratio, methane has the potential to produce hydrogen or hydrogen-rich products. However, methane is a very chemically stable molecule and, thus, is not readily transformed to other molecules or easily reformed to its elements (H{sub 2} and carbon). In many cases, further research is needed to augment selectivity to desired product(s), increase single-pass conversions, or improve economics (e.g. there have been estimates of $50/bbl or more for liquid products) before the full potential of these methodologies can be realized on a commercial scale. With the trade-off between gas conversion and product selectivity, a major challenge common to many of these technologies is to simultaneously achieve high methane single-pass conversions and high selectivity to desired products. Based on the results of the scoping runs, there appears to be strong indications that a breakthrough has finally been achieved in that synthesis of magnesium carbides from MgO and methane in the arc discharge reactor has been demonstrated.

  6. Analytical investigation of high temperature 1 kW solid oxide fuel cell system feasibility in methane hydrate recovery and deep ocean power generation

    International Nuclear Information System (INIS)

    Azizi, Mohammad Ali; Brouwer, Jacob; Dunn-Rankin, Derek

    2016-01-01

    Highlights: • A dynamic Solid Oxide Fuel Cell (SOFC) model was developed. • Hydrate bed methane dissociation model was integrated with the SOFC model. • SOFC operated steadily for 120 days at high pressure deep ocean environment. • Burning some of the dissociated gas for SMR heat leads to more net methane produced. • Higher SOFC fuel utilization produces higher integrated system efficiency. - Abstract: Methane hydrates are potential valuable energy resources. However, finding an efficient method for methane gas recovery from hydrate sediments is still a challenge. New challenges arise from increasing environmental protection. This is due in part to the technical difficulties involved in the efficient dissociation of methane hydrates at high pressures. In this study, a new approach is proposed to produce valuable products of: 1. Net methane gas recovery from the methane hydrate sediment, and 2. Deep ocean power generation. We have taken the first steps toward utilization of a fuel cell system in methane gas recovery from deep ocean hydrate sediments. An integrated high pressure and high temperature solid oxide fuel cell (SOFC) and steam methane reformer (SMR) system is analyzed for this application and the recoverable amount of methane from deep ocean sediments is measured. System analysis is accomplished for two major cases regarding system performance: 1. Energy for SMR is provided by the burning part of the methane gas dissociated from the hydrate sediment. 2. Energy for SMR is provided through heat exchange with fuel cell effluent gases. We found that the total production of methane gas is higher in the first case compared to the second case. The net power generated by the fuel cell system is estimated for all cases. The primary goal of this study is to evaluate the feasibility of integrated electrochemical devices to accomplish energy efficient dissociation of methane hydrate gases in deep ocean sediments. Concepts for use of electrochemical devices

  7. Occasional large emissions of nitrous oxide and methane observed in stormwater biofiltration systems

    International Nuclear Information System (INIS)

    Grover, Samantha P.P.; Cohan, Amanda; Chan, Hon Sen; Livesley, Stephen J.; Beringer, Jason; Daly, Edoardo

    2013-01-01

    in the cell without the saturated zone CO 2 fluxes decreased as soil moisture increased. Other studies of CO 2 fluxes from urban soils have found both similar and larger CO 2 emissions than those measured in the biofilter. The results of this study suggest that the greenhouse gas footprint of stormwater treatment warrant consideration in the planning and implementation of engineered green infrastructures. - Highlights: ► First study of greenhouse gas fluxes from a stormwater biofilter. ► Observed occasional large emissions of nitrous oxide and methane. ► Biofilter designs with and without a saturated zone were net sinks for methane. ► Carbon dioxide emissions were four times less than those from lawns

  8. Occasional large emissions of nitrous oxide and methane observed in stormwater biofiltration systems

    Energy Technology Data Exchange (ETDEWEB)

    Grover, Samantha P.P., E-mail: samantha.grover@monash.edu [Department of Civil Engineering, Monash University, Clayton, Victoria, 3800 (Australia); Cohan, Amanda, E-mail: acoh5@student.monash.edu [Department of Civil Engineering, Monash University, Clayton, Victoria, 3800 (Australia); Chan, Hon Sen, E-mail: hon.sen.chan@gmail.com [Department of Civil Engineering, Monash University, Clayton, Victoria, 3800 (Australia); Livesley, Stephen J., E-mail: sjlive@unimelb.edu.au [Department of Resource Management and Geography, The University of Melbourne, Richmond, Victoria, 3121 (Australia); Beringer, Jason, E-mail: jason.beringer@monash.edu [School of Geography and Environmental Science, Monash University, Clayton, Victoria, 3800 (Australia); Monash Water for Liveability, Monash University, Clayton, Victoria, 3800 (Australia); Daly, Edoardo, E-mail: edoardo.daly@monash.edu [Department of Civil Engineering, Monash University, Clayton, Victoria, 3800 (Australia); Monash Water for Liveability, Monash University, Clayton, Victoria, 3800 (Australia)

    2013-11-01

    inflow events, which were not seen in other urban systems. CO{sub 2} fluxes increased with soil temperature in both cells, and in the cell without the saturated zone CO{sub 2} fluxes decreased as soil moisture increased. Other studies of CO{sub 2} fluxes from urban soils have found both similar and larger CO{sub 2} emissions than those measured in the biofilter. The results of this study suggest that the greenhouse gas footprint of stormwater treatment warrant consideration in the planning and implementation of engineered green infrastructures. - Highlights: ► First study of greenhouse gas fluxes from a stormwater biofilter. ► Observed occasional large emissions of nitrous oxide and methane. ► Biofilter designs with and without a saturated zone were net sinks for methane. ► Carbon dioxide emissions were four times less than those from lawns.

  9. Nitrous oxide and methane emission in an artificial wetland treating polluted runoff from an agricultural catchment

    Science.gov (United States)

    Mander, Ülo; Tournebize, Julien; Soosaar, Kaido; Chaumont, Cedric; Hansen, Raili; Muhel, Mart; Teemusk, Alar; Vincent, Bernard

    2015-04-01

    . Nitrous oxide flux was low (average 1.1, variation from -25 to 63 μg N2O-N m-2 h-1) and showed consumption during the daytime. Similarly to CH4, most of the N2O emission originated from ebullition. The potential N2 flux from sediments was high (990-1920 μg N m-2 h-1). In November, with HRT at about 3 days, the average NO3- concentration decreased from 45 to 20 mg/L. Methane flux was 2-3 times lower and N2O emission about 2 times higher than in May. This is related to the lower water temperature (20°C in May and 10°C in November) and shorter HRT in November. However, in situ pipe reactors showed a 90% NO3- removal potential in both periods. Offshore artificial wetlands can efficiently remove NO3- without significant N2O emission, although CH4 flux can be high during the first 5 years after establishment.

  10. Characteristic analysis of methane-gas generation by oxidizing heat of stored coal and hold ventilation control; Sekitan unpansen ni okeru sanka hatsunetsu ni yoru methane gas hassei to sonai kankyo seigyo ni tsuite

    Energy Technology Data Exchange (ETDEWEB)

    Fukuchi, N; Nakashima, T [Kyushu Univ., Fukuoka (Japan); Kudo, S

    1999-12-31

    A demand of coal shows the tendency in the increase worldwide, with this, the marine transportation of the coal gradually increases, and the collier has also enlarged. The traffic pattern of coal is mainly the bulk transportation. In this transportation system, by the oxidation exothermic reaction of the coal, methane gas is produced, simultaneously the coal quality such as coking property or heat quantity is decreased and sometimes spontaneous ignition is caused. Therefore, it is necessary to equip with a ventilator to control the concentration of methane gas and to avoid the self heating of the coal. In this study, the quantity of methane-gas produced by heating coal using an electric furnace was measured and the experiment to investigate the temperature dependency of the methane-gas generated from the coal was conducted. By using the result of the measurement, the quantity of methane-gas produced from the coal stored in the hold of a coal cargo was estimated. And, the mathematical analyses on the changing degree depend on the times of a temperature in the hold under navigation, a concentration of oxygen and a concentration of methane-gas, were conducted. 11 refs., 19 figs., 2 tabs.

  11. On direct internal methane steam reforming kinetics in operating solid oxide fuel cells with nickel-ceria anodes

    Science.gov (United States)

    Thallam Thattai, A.; van Biert, L.; Aravind, P. V.

    2017-12-01

    Major operating challenges remain to safely operate methane fuelled solid oxide fuel cells due to undesirable temperature gradients across the porous anode and carbon deposition. This article presents an experimental study on methane steam reforming (MSR) global kinetics for single operating SOFCs with Ni-GDC (gadolinium doped ceria) anodes for low steam to carbon (S/C) ratios and moderate current densities. The study points out the hitherto insufficient research on MSR global and intrinsic kinetics for operating SOFCs with complete Ni-ceria anodes. Further, it emphasizes the need to develop readily applicable global kinetic models as a subsequent step from previously reported state-of-art and complex intrinsic models. Two rate expressions of the Power law (PL) and Langmuir-Hinshelwood (LH) type have been compared and based on the analysis, limitations of using previously proposed rate expressions for Ni catalytic beds to study MSR kinetics for complete cermet anodes have been identified. Firstly, it has been shown that methane reforming on metallic (Ni) current collectors may not be always negligible, contrary to literature reports. Both PL and LH kinetic models predict significantly different local MSR reaction rate and species partial pressure distributions along the normalized reactor length, indicating a strong need for further experimental verifications.

  12. Modeling of electrochemistry and steam-methane reforming performance for simulating pressurized solid oxide fuel cell stacks

    Energy Technology Data Exchange (ETDEWEB)

    Recknagle, Kurtis P.; Ryan, Emily M.; Koeppel, Brian J.; Mahoney, Lenna A.; Khaleel, Moe A. [Pacific Northwest National Laboratory, Richland, WA 99352 (United States)

    2010-10-01

    This paper examines the electrochemical and direct internal steam-methane reforming performance of the solid oxide fuel cell when subjected to pressurization. Pressurized operation boosts the Nernst potential and decreases the activation polarization, both of which serve to increase cell voltage and power while lowering the heat load and operating temperature. A model considering the activation polarization in both the fuel and the air electrodes was adopted to address this effect on the electrochemical performance. The pressurized methane conversion kinetics and the increase in equilibrium methane concentration are considered in a new rate expression. The models were then applied in simulations to predict how the distributions of direct internal reforming rate, temperature, and current density are effected within stacks operating at elevated pressure. A generic 10 cm counter-flow stack model was created and used for the simulations of pressurized operation. The predictions showed improved thermal and electrical performance with increased operating pressure. The average and maximum cell temperatures decreased by 3% (20 C) while the cell voltage increased by 9% as the operating pressure was increased from 1 to 10 atm. (author)

  13. Methylocapsa acidiphila gen. nov., sp. nov., a novel methane-oxidizing and dinitrogen-fixing acidophilic bacterium from Sphagnum bog.

    Science.gov (United States)

    Dedysh, Svetlana N; Khmelenina, Valentina N; Suzina, Natalia E; Trotsenko, Yuri A; Semrau, Jeremy D; Liesack, Werner; Tiedje, James M

    2002-01-01

    A novel genus and species, Methylocapsa acidiphila gen. nov., sp. nov., are proposed for a methane-oxidizing bacterium isolated from an acidic Sphagnum peat bog. This bacterium, designated strain B2T, represents aerobic, gram-negative, colourless, non-motile, curved coccoids that form conglomerates covered by an extracellular polysaccharide matrix. The cells use methane and methanol as sole sources of carbon and energy and utilize the serine pathway for carbon assimilation. Strain B2T is a moderately acidophilic organism with growth between pH 4.2 and 7.2 and at temperatures from 10 to 30 degrees C. The cells possess a well-developed system of intracytoplasmic membranes (ICM) packed in parallel on only one side of the cell membrane. This type of ICM structure represents a novel arrangement, which was termed type III. The resting cells are Azotobacter-type cysts. Strain B2T is capable of atmospheric nitrogen fixation; it possesses particulate methane monooxygenase and does not express soluble methane monooxygenase. The major phospholipid fatty acid is 18:1omega7c and the major phospholipids are phosphatidylglycerols. The G+C content of the DNA is 63.1 mol%. This bacterium belongs to the alpha-subclass of the Proteobacteria and is most closely related to the acidophilic methanotroph Methylocella palustris KT (97.3% 16S rDNA sequence similarity). However, the DNA-DNA hybridization value between strain B2T and Methylocella palustris K(T) is only 7%. Thus, strain B2T is proposed to comprise a novel genus and species, Methylocapsa acidiphila gen. nov., sp. nov. Strain B2T (= DSM 13967T = NCIMB 13765T) is the type strain.

  14. Trace Metal Requirements for Microbial Enzymes Involved in the Production and Consumption of Methane and Nitrous Oxide

    Science.gov (United States)

    Glass, Jennifer B.; Orphan, Victoria J.

    2011-01-01

    Fluxes of greenhouse gases to the atmosphere are heavily influenced by microbiological activity. Microbial enzymes involved in the production and consumption of greenhouse gases often contain metal cofactors. While extensive research has examined the influence of Fe bioavailability on microbial CO2 cycling, fewer studies have explored metal requirements for microbial production and consumption of the second- and third-most abundant greenhouse gases, methane (CH4), and nitrous oxide (N2O). Here we review the current state of biochemical, physiological, and environmental research on transition metal requirements for microbial CH4 and N2O cycling. Methanogenic archaea require large amounts of Fe, Ni, and Co (and some Mo/W and Zn). Low bioavailability of Fe, Ni, and Co limits methanogenesis in pure and mixed cultures and environmental studies. Anaerobic methane oxidation by anaerobic methanotrophic archaea (ANME) likely occurs via reverse methanogenesis since ANME possess most of the enzymes in the methanogenic pathway. Aerobic CH4 oxidation uses Cu or Fe for the first step depending on Cu availability, and additional Fe, Cu, and Mo for later steps. N2O production via classical anaerobic denitrification is primarily Fe-based, whereas aerobic pathways (nitrifier denitrification and archaeal ammonia oxidation) require Cu in addition to, or possibly in place of, Fe. Genes encoding the Cu-containing N2O reductase, the only known enzyme capable of microbial N2O conversion to N2, have only been found in classical denitrifiers. Accumulation of N2O due to low Cu has been observed in pure cultures and a lake ecosystem, but not in marine systems. Future research is needed on metalloenzymes involved in the production of N2O by enrichment cultures of ammonia oxidizing archaea, biological mechanisms for scavenging scarce metals, and possible links between metal bioavailability and greenhouse gas fluxes in anaerobic environments where metals may be limiting due to sulfide

  15. Final Report for Wetlands as a Source of Atmospheric Methane: A Multiscale and Multidisciplinary Approach

    Energy Technology Data Exchange (ETDEWEB)

    McFarlane, Karis J. [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

    2016-10-28

    Boreal peatlands contain large amounts of old carbon, protected by anaerobic and cold conditions. Climate change could result in favorable conditions for the microbial decomposition and release of this old peat carbon as CO2 or CH4 back into the atmosphere. Our goal was to test the potential for this positive biological feedback to climate change at SPRUCE (Spruce and Peatland Response Under Climatic and Environmental Change), a manipulation experiment funded by DOE and occurring in a forested bog in Minnesota. Taking advantage of LLNL’s capabilities and expertise in chemical and isotopic signatures we found that carbon emissions from peat were dominated by recently fixed photosynthates, even after short-term experimental warming. We also found that subsurface hydrologic transport was surprisingly rapid at SPRUCE, supplying microbes with young dissolved organic carbon (DOC). We also identified which microbes oxidize CH4 to CO2 at SPRUCE and found that the most active of these also fix N2 (which means they can utilize atmospheric N, making it accessible for other microbes and plants). These results reflect important interactions between hydrology, carbon cycling, and nitrogen cycling present at the bog and relevant to interpreting experimental results and modeling the wetland response to experimental treatments. LLNL involvement at SPRUCE continues through collaborations and a small contract with ORNL, the lead lab for the SPRUCE experiment.

  16. Thermodynamic and Kinetic Requirements in Anaerobic Methane Oxidizing Consortia Exclude Hydrogen, Acetate, and Methanol as Possible Electron Shuttles.

    Science.gov (United States)

    Sørensen, K.B.; Finster, K.; Ramsing, N.B.

    2001-07-01

    Anaerobic methane oxidation (AMO) has long remained an enigma in microbial ecology. In the process the net reaction appears to be an oxidation of methane with sulfate as electron acceptor. In order to explain experimental data such as effects of inhibitors and isotopic signals in biomarkers it has been suggested that the process is carried out by a consortium of bacteria using an unknown compound to shuttle electrons between the participants. The overall change in free energy during AMO with sulfate is very small (?22 kJ mol-1) at in situ concentrations of methane and sulfate. In order to share the available free energy between the members of the consortium, the concentration of the intermediate electron shuttle compound becomes crucial. Diffusive flux of a substrate (i.e, the electron shuttle) between bacteria requires a stable concentration gradient where the concentration is higher in the producing organism than in the consuming organism. Since changes in concentrations cause changes in reaction free energies, the diffusive flux of a catabolic product/substrate between bacteria is associated with a net loss of available energy. This restricts maximal inter-bacterial distances in consortia composed of stationary bacteria. A simple theoretical model was used to describe the relationship between inter-bacterial distances and the energy lost due to concentration differences in consortia. Key parameters turned out to be the permissible concentration range of the electron shuttle in the consortium (i.e., the concentration range that allows both participants to gain sufficient energy) and the stoichiometry of the partial reactions. The model was applied to two known consortia degrading ethanol and butyrate and to four hypothetical methane-oxidizing consortia (MOC) based on interspecies transfer of hydrogen, methanol, acetate, or formate, respectively. In the first three MOCs the permissible distances between producers and consumers of the transferred compounds were

  17. The response of methane and nitrous oxide fluxes to forest change in Europe

    Directory of Open Access Journals (Sweden)

    P. Gundersen

    2012-10-01

    Full Text Available Forests in Europe are changing due to interactions between climate change, nitrogen (N deposition and new forest management practices. The concurrent impact on the forest greenhouse gas (GHG balance is at present difficult to predict due to a lack of knowledge on controlling factors of GHG fluxes and response to changes in these factors. To improve the mechanistic understanding of the ongoing changes, we studied the response of soil–atmosphere exchange of nitrous oxide (N2O and methane (CH4 at twelve experimental or natural gradient forest sites, representing anticipated future forest change. The experimental manipulations, one or more per site, included N addition (4 sites, changes of climate (temperature, 1 site; precipitation, 2 sites, soil hydrology (3 sites, harvest intensity (1 site, wood ash fertilisation (1 site, pH gradient in organic soil (1 site and afforestation of cropland (1 site.

    On average, N2O emissions increased by 0.06 ± 0.03 (range 0–0.3 g N2O-N m−2 yr−1 across all treatments on mineral soils, but the increase was up to 10 times higher in an acidic organic soil. Soil moisture together with mineral soil C / N ratio and pH were found to significantly influence N2O emissions across all treatments. Emissions were increased by elevated N deposition, especially in interaction with increased soil moisture. High pH reduced the formation of N2O, even under otherwise favourable soil conditions.

    Oxidation (uptake of CH4 was on average reduced from 0.16 ± 0.02 to 0.04 ± 0.05 g CH4-C m−2 yr−1 by the investigated treatments. The CH4 exchange was significantly influenced by soil moisture and soil C / N ratio across all treatments, and CH4 emissions occurred only in wet or water-saturated conditions.

    For most of the investigated forest manipulations

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

    International Nuclear Information System (INIS)

    Carlsson-Kanyama, Annika

    2007-01-01

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

  19. Hydrogen or synthesis gas production via the partial oxidation of methane over supported nickel-cobalt catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Koh, Alaric C.W. [Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore); Institute of Chemical and Engineering Sciences, 1 Pesek Road, Jurong Island, Singapore 627833 (Singapore); Chen, Luwei; Lin, Jianyi [Institute of Chemical and Engineering Sciences, 1 Pesek Road, Jurong Island, Singapore 627833 (Singapore); Kee Leong, Weng [Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore); Johnson, Brian F.G.; Khimyak, Tetyana [University Chemical Laboratory, University of Cambridge, Lensfield Road, Cambridge, UK CB2 1EW (United Kingdom)

    2007-05-15

    Activity, selectivity, and coking-resistance of a series of Ni{sub x}Co{sub y} (where x,y are the respective metal loadings of 0, 1, 2 or 3 wt.%; x+y=3) bimetallic catalysts supported on CaAl{sub 2}O{sub 4}/Al{sub 2}O{sub 3} have been studied for hydrogen/synthesis gas production via the catalytic partial oxidation (CPO) of methane. Catalysts were characterized by temperature programmed reduction (TPR), transmission electron microscopy (TEM) and X-ray fluorescence multi-element analysis (XRF). Their activity for the partial oxidation of methane to hydrogen and carbon monoxide (at 1 bar, gas hourly space velocity (GHSV) of 144,000cm{sup 3}g{sup -1}h{sup -1} and CH{sub 4}/O{sub 2} molar ratio of 2) was investigated, and coke deposited on the spent catalysts was studied by scanning electron microscopy (SEM), energy dispersive X-ray analysis (EDX) and thermogravimetric analysis (TGA). The activity was found to decrease in the order of Ni{sub 2}Co>Ni{sub 3}>NiCo{sub 2}>>Co{sub 3}, while CO and H{sub 2} selectivities were found to be in the order ofNi{sub 2}Co>Ni{sub 3}{approx}NiCo{sub 2}>Co{sub 3}. Ni{sub 2}Co is also shown to be more resistant to coking as compared to Ni{sub 3}, which is a current catalyst of choice. Results show that not only does Ni{sub 2}Co have the highest activity and selectivity among all the catalysts tested, it is also relatively resistant to coking. This finding would be helpful for catalyst design to achieve high coking resistivity catalysts for hydrogen production from CPO of methane. (author)

  20. Fluxes of methane and nitrogen oxides in various boreal mire ecosystems. Effects of land-use activities and environmental changes

    Energy Technology Data Exchange (ETDEWEB)

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

    1996-12-31

    Atmospheric impact of peatlands is a sum of their gas fluxes. In contrast to carbon dioxide, peatlands are net sources for methane (CH{sub 4}). Methane is an end product in the anaerobic decomposition processes and it has greater capacity to absorb infrared radiation than carbon dioxide. Most of the data on the CH{sub 4} release from northern peatlands is from North America. The total amount of methane released from wetlands is calculated to be 110 Tg yr{sup -1} of which 34 percent (38 Tg yr{sup -1}) is estimated to be emitted from the northern peatlands. Peat with high content of nitrogen is a potential source for gaseous nitrogen oxides, i.e. nitrous oxide (N{sub 2}O) and nitric oxide (NO). However, the importance of peatlands in producing these trace gases is poorly known. Nitrous oxide and nitric oxide are important components in the atmospheric chemistry and N{sub 2}O also is an effective greenhouse gas. Land-use activities and environmental changes can affect the atmospheric impacts of peatlands by modifying their biogeochemistry. This article presents a short summary of the studies whose objectives were: (1) to measure fluxes of CH{sub 4} and N{sub 2}O on wide range of natural mires in Finland, (2) to study the short- and long-term changes in fluxes of CH{sub 4}, N{sub 2}O and NO on boreal peatlands after lowering their water table. Peatlands used for agriculture, forestry and peat mining were included in the studies. The results from mires drained for forestry may reflect the possible changes in the trace gas fluxes if water table will drop in the northern peatlands as a result of drier climate, (3) to study the effects of nitrogen load on the fluxes of CH{sub 4}, N{sub 2}O and NO, (4) to identify the microbiological processes important for the fluxes of N{sub 2}O, NO and CH{sub 4}, and to study the environmental factors regulating these microbial processes

  1. Fluxes of methane and nitrogen oxides in various boreal mire ecosystems. Effects of land-use activities and environmental changes

    Energy Technology Data Exchange (ETDEWEB)

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

    1997-12-31

    Atmospheric impact of peatlands is a sum of their gas fluxes. In contrast to carbon dioxide, peatlands are net sources for methane (CH{sub 4}). Methane is an end product in the anaerobic decomposition processes and it has greater capacity to absorb infrared radiation than carbon dioxide. Most of the data on the CH{sub 4} release from northern peatlands is from North America. The total amount of methane released from wetlands is calculated to be 110 Tg yr{sup -1} of which 34 percent (38 Tg yr{sup -1}) is estimated to be emitted from the northern peatlands. Peat with high content of nitrogen is a potential source for gaseous nitrogen oxides, i.e. nitrous oxide (N{sub 2}O) and nitric oxide (NO). However, the importance of peatlands in producing these trace gases is poorly known. Nitrous oxide and nitric oxide are important components in the atmospheric chemistry and N{sub 2}O also is an effective greenhouse gas. Land-use activities and environmental changes can affect the atmospheric impacts of peatlands by modifying their biogeochemistry. This article presents a short summary of the studies whose objectives were: (1) to measure fluxes of CH{sub 4} and N{sub 2}O on wide range of natural mires in Finland, (2) to study the short- and long-term changes in fluxes of CH{sub 4}, N{sub 2}O and NO on boreal peatlands after lowering their water table. Peatlands used for agriculture, forestry and peat mining were included in the studies. The results from mires drained for forestry may reflect the possible changes in the trace gas fluxes if water table will drop in the northern peatlands as a result of drier climate, (3) to study the effects of nitrogen load on the fluxes of CH{sub 4}, N{sub 2}O and NO, (4) to identify the microbiological processes important for the fluxes of N{sub 2}O, NO and CH{sub 4}, and to study the environmental factors regulating these microbial processes

  2. Effect of Elevated CO2 Concentration, Elevated Temperature and No Nitrogen Fertilization on Methanogenic Archaeal and Methane-Oxidizing Bacterial Community Structures in Paddy Soil.

    Science.gov (United States)

    Liu, Dongyan; Tago, Kanako; Hayatsu, Masahito; Tokida, Takeshi; Sakai, Hidemitsu; Nakamura, Hirofumi; Usui, Yasuhiro; Hasegawa, Toshihiro; Asakawa, Susumu

    2016-09-29

    Elevated concentrations of atmospheric CO2 ([CO2]) enhance the production and emission of methane in paddy fields. In the present study, the effects of elevated [CO2], elevated temperature (ET), and no nitrogen fertilization (LN) on methanogenic archaeal and methane-oxidizing bacterial community structures in a free-air CO2 enrichment (FACE) experimental paddy field were investigated by PCR-DGGE and real-time quantitative PCR. Soil samples were collected from the upper and lower soil layers at the rice panicle initiation (PI) and mid-ripening (MR) stages. The composition of the methanogenic archaeal community in the upper and lower soil layers was not markedly affected by the elevated [CO2], ET, or LN condition. The abundance of the methanogenic archaeal community in the upper and lower soil layers was also not affected by elevated [CO2] or ET, but was significantly increased at the rice PI stage and significantly decreased by LN in the lower soil layer. In contrast, the composition of the methane-oxidizing bacterial community was affected by rice-growing stages in the upper soil layer. The abundance of methane-oxidizing bacteria was significantly decreased by elevated [CO2] and LN in both soil layers at the rice MR stage and by ET in the upper soil layer. The ratio of mcrA/pmoA genes correlated with methane emission from ambient and FACE paddy plots at the PI stage. These results indicate that the decrease observed in the abundance of methane-oxidizing bacteria was related to increased methane emission from the paddy field under the elevated [CO2], ET, and LN conditions.

  3. Rare branched fatty acids characterize the lipid composition of the intra-aerobic methane oxidizer "Candidatus Methylomirabilis oxyfera".

    Science.gov (United States)

    Kool, Dorien M; Zhu, Baoli; Rijpstra, W Irene C; Jetten, Mike S M; Ettwig, Katharina F; Sinninghe Damsté, Jaap S

    2012-12-01

    The recently described bacterium "Candidatus Methylomirabilis oxyfera" couples the oxidation of the important greenhouse gas methane to the reduction of nitrite. The ecological significance of "Ca. Methylomirabilis oxyfera" is still underexplored, as our ability to identify the presence of this bacterium is thus far limited to DNA-based techniques. Here, we investigated the lipid composition of "Ca. Methylomirabilis oxyfera" to identify new, gene-independent biomarkers for the environmental detection of this bacterium. Multiple "Ca. Methylomirabilis oxyfera" enrichment cultures were investigated. In all cultures, the lipid profile was dominated up to 46% by the fatty acid (FA) 10-methylhexadecanoic acid (10MeC(16:0)). Furthermore, a unique FA was identified that has not been reported elsewhere: the monounsaturated 10-methylhexadecenoic acid with a double bond at the Δ7 position (10MeC(16:1Δ7)), which comprised up to 10% of the total FA profile. We propose that the typical branched fatty acids 10MeC(16:0) and 10MeC(16:1Δ7) are key and characteristic components of the lipid profile of "Ca. Methylomirabilis oxyfera." The successful detection of these fatty acids in a peatland from which one of the enrichment cultures originated supports the potential of these unique lipids as biomarkers for the process of nitrite-dependent methane oxidation in the environment.

  4. Li-doped MgO as catalysts for oxidative coupling of methane: A positron annihilation study

    Science.gov (United States)

    Dai, G. H.; Yan, Q. J.; Wang, Y.; Liu, Q. S.

    1991-08-01

    Magnesium oxides intentionally doped with lithium (with a maximum Li content of 40 tool%) for use as catalysts for oxidative coupling of methane were characterized by means of positron annihilation. The positron lifetime spectra, which could be reasonably well interpreted within the framework of the well-known trapping model, depend on the amount of Li doping of the MgO suggesting that positrons are trapped at dispersed small Li 2CO 3 precipitates. Very similar dependencies on lithium doping of the C 2 selectivity and the positron trapping rate ϰ imply an intimate relationship between the concentration of [Li] 0-centers (also referred to as [Li +O -] centers) and the selective activity of Li/MgO during catalytic reactions.

  5. Partial oxidation of methane to syngas on Rh/Al{sub 2}O{sub 3} and Rh/Ce-ZrO{sub 2} catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Oliveira, Raquel L.; Bitencourt, Isabela G.; Passos, Fabio B., E-mail: fbpassos@vm.uff.br [Universidade Federal Fluminense (UFF), Niteroi, RJ (Brazil). Dept. de Engenharia Quimica e Petroleo

    2013-01-15

    The partial oxidation of methane with {gamma}-Al{sub 2}O{sub 3}-, CeO{sub 2}-, ZrO{sub 2}- and Ce-ZrO{sub 2}-supported rhodium catalysts was investigated. DRIFTS (diffuse reflectance infrared spectroscopy) measurements of adsorbed CO showed the formation of different rhodium species on different supports, which influenced the dispersion of the metal. The effects of the metal dispersion, oxygen storage capacity on the activity of these catalysts for the partial oxidation of methane are discussed. (author)

  6. Production of sustainable methane from renewable energy and captured carbon dioxide with the use of Solid Oxide Electrolyzer: A thermodynamic assessment

    International Nuclear Information System (INIS)

    Stempien, Jan Pawel; Ni, Meng; Sun, Qiang; Chan, Siew Hwa

    2015-01-01

    A possible pathway for renewable and sustainable methane production from captured carbon dioxide, water (or seawater) and renewable electricity is proposed and analysed. The proposed system includes Solid Oxide Electrolyzer Cell combined with ex-situ methane synthesis reactor comprising Sabatier, Methanation and Water-Gas Shift reactions. A well validated electrochemical model is used to describe the behaviour of the electrolyzer for steam/carbon dioxide co-electrolysis. The methane synthesis reactor is modelled by a set of equations based on thermodynamic equilibrium reaction constants. Effects of current density, temperature, pressure and initial steam to carbon dioxide ratio on system performance are analysed and their effects are discussed. It is found that a simple, single-pass system without heat recuperation could achieve a maximum overall energy efficiency of 60.87% (based on lower heating value), a maximum electrical energy efficiency of 81.08% (based on lower heating value), and a maximum amount of methane production of ∼1.52 Nm 3  h −1  m −2 of electrolyzer. It is also found that conversion of ∼100% captured carbon dioxide is possible in the proposed system. - Highlights: • Analysis of Solid Oxide Electrolyzer combined with methane synthesis process. • Efficiency of converting water and carbon dioxide into synthetic, renewable methane above 81%. • Effects of process temperature, pressure, gas flux and compositions were analysed. • Methane production of ∼1.52 [Nm 3 h −1 m −2 of electrolyzer]. • Conversion of ∼100% of captured CO 2 is possible

  7. Constraints on mechanisms and rates of anaerobic oxidation of methane by microbial consortia: process-based modeling of ANME-2 archaea and sulfate reducing bacteria interactions

    Directory of Open Access Journals (Sweden)

    B. Orcutt

    2008-11-01

    Full Text Available Anaerobic oxidation of methane (AOM is the main process responsible for the removal of methane generated in Earth's marine subsurface environments. However, the biochemical mechanism of AOM remains elusive. By explicitly resolving the observed spatial arrangement of methanotrophic archaea and sulfate reducing bacteria found in consortia mediating AOM, potential intermediates involved in the electron transfer between the methane oxidizing and sulfate reducing partners were investigated via a consortium-scale reaction transport model that integrates the effect of diffusional transport with thermodynamic and kinetic controls on microbial activity. Model simulations were used to assess the impact of poorly constrained microbial characteristics such as minimum energy requirements to sustain metabolism and cell specific rates. The role of environmental conditions such as the influence of methane levels on the feasibility of H2, formate and acetate as intermediate species, and the impact of the abundance of intermediate species on pathway reversal were examined. The results show that higher production rates of intermediates via AOM lead to increased diffusive fluxes from the methane oxidizing archaea to sulfate reducing bacteria, but the build-up of the exchangeable species can cause the energy yield of AOM to drop below that required for ATP production. Comparison to data from laboratory experiments shows that under the experimental conditions of Nauhaus et al. (2007, none of the potential intermediates considered here is able to support metabolic activity matching the measured rates.

  8. Production of nitrous oxide and consumption of methane by forest soils

    Science.gov (United States)

    Keller, M.; Wofsy, S. C.; Kaplan, W. A.; Mcelroy, M. B.; Goreau, T. J.

    1983-01-01

    Soils in an Amazonian rainforest are observed to release N2O at a rate larger than the global mean by about a factor of 20. Emissions from a New England hardwood forest are approximately 30 times smaller then Brazilian values. Atmospheric methane is consumed by soils in both systems. Tropical forests would provide a major source of atmospheric N2O if the Brazilian results are representative.

  9. High abundance and diversity of nitrite-dependent anaerobic methane-oxidizing bacteria in a paddy field profile.

    Science.gov (United States)

    Zhou, Leiliu; Wang, Yu; Long, Xi-En; Guo, Jianhua; Zhu, Guibing

    2014-11-01

    The discovery of nitrite-dependent anaerobic methane oxidation (n-damo) mediated by 'Candidatus Methylomirabilis oxyfera' with nitrite and methane as substrates has connected biogeochemical carbon and nitrogen cycles in a new way. The paddy fields often carry substantial methane and nitrate, thus may be a favorable habitat for n-damo bacteria. In this paper, the vertical-temporal molecular fingerprints of M. oxyfera-like bacteria, including abundance and community composition, were investigated in a paddy soil core in Jiangyin, near the Yangtze River. Through qPCR investigation, high abundance of M. oxyfera-like bacteria up to 1.0 × 10(8) copies (g d.w.s.)(-1) in summer and 8.5 × 10(7) copies (g d.w.s.)(-1) in winter was observed in the ecotone of soil and groundwater in the paddy soil core, which was the highest in natural environments to our knowledge. In the ecotone, the ratio of M. oxyfera-like bacteria to total bacteria reached peak values of 2.80% in summer and 4.41% in winter. Phylogenetic analysis showed n-damo bacteria in the paddy soil were closely related to M. oxyfera and had high diversity in the soil/groundwater ecotone. All of the results indicated the soil/groundwater ecotone of the Jiangyin paddy field was a favorable environment for the growth of n-damo bacteria. © 2014 Federation of European Microbiological Societies. Published by John Wiley & Sons Ltd. All rights reserved.

  10. Assessment of methane emission and oxidation at Air Hitam Landfill site cover soil in wet tropical climate.

    Science.gov (United States)

    Abushammala, Mohammed F M; Basri, Noor Ezlin Ahmad; Elfithri, Rahmah

    2013-12-01

    Methane (CH₄) emissions and oxidation were measured at the Air Hitam sanitary landfill in Malaysia and were modeled using the Intergovernmental Panel on Climate Change waste model to estimate the CH₄ generation rate constant, k. The emissions were measured at several locations using a fabricated static flux chamber. A combination of gas concentrations in soil profiles and surface CH₄ and carbon dioxide (CO₂) emissions at four monitoring locations were used to estimate the CH₄ oxidation capacity. The temporal variations in CH₄ and CO₂ emissions were also investigated in this study. Geospatial means using point kriging and inverse distance weight (IDW), as well as arithmetic and geometric means, were used to estimate total CH₄ emissions. The point kriging, IDW, and arithmetic means were almost identical and were two times higher than the geometric mean. The CH₄ emission geospatial means estimated using the kriging and IDW methods were 30.81 and 30.49 gm(−2) day(−1), respectively. The total CH₄ emissions from the studied area were 53.8 kg day(−1). The mean of the CH₄ oxidation capacity was 27.5 %. The estimated value of k is 0.138 year(−1). Special consideration must be given to the CH₄ oxidation in the wet tropical climate for enhancing CH₄ emission reduction.

  11. Methane dry reforming over Ni catalysts supported on Ce–Zr oxides prepared by a route involving supercritical fluids

    Directory of Open Access Journals (Sweden)

    Smirnova Marina Yu.

    2017-12-01

    Full Text Available Ce0.5Zr0.5O2 mixed oxides were prepared in a flow reactor in supercritical isopropanol with acetylacetone as a complexing agent. Variation of the nature of the Zr salt and the temperature of synthesis affected the phase composition, morphology and specific surface area of oxides. X-ray diffraction and Raman spectroscopy studies revealed formation of metastable t” and t’ phases. Oxides are comprised of agglomerates with sizes depending on the synthesis parameters. Loading NiO decreases the specific surface area without affecting X-ray particle sizes of supports. Such sintering was the most pronounced for a support with the highest specific surface area, which resulted in the lowest surface content of Ni as estimated by X-ray photoelectron spectroscopy and in the formation of flattened NiO particles partially embedded into the support. The catalytic activity and stability of these samples in the dry reforming of methane were determined by the surface concentration of Ni and the morphology of its particle controlled by the metal-support interaction, which also depends on the type of catalyst pretreatment. Samples based on ceria-zirconia oxides prepared under these conditions provide a higher specific catalytic activity as compared with the traditional Pechini route, which makes them promising for the practical application.

  12. Influence of capillary barrier effect on biogas distribution at the base of passive methane oxidation biosystems: Parametric study.

    Science.gov (United States)

    Ahoughalandari, Bahar; Cabral, Alexandre R

    2017-05-01

    The efficiency of methane oxidation in passive methane oxidation biosystems (PMOBs) is influenced by, among other things, the intensity and distribution of the CH 4 loading at the base of the methane oxidation layer (MOL). Both the intensity and distribution are affected by the capillary barrier that results from the superposition of the two materials constituting the PMOB, namely the MOL and the gas distribution layer (GDL). The effect of capillary barriers on the unsaturated flow of water has been well documented in the literature. However, its effect on gas flow through PMOBs is still poorly documented. In this study, sets of numerical simulations were performed to evaluate the effect of unsaturated hydraulic characteristics of the MOL material on the value and distribution of moisture and hence, the ease and uniformity in the distribution of the upward flow of biogas along the GDL-MOL interface. The unsaturated hydraulic parameters of the materials used to construct the experimental field plot at the St-Nicephore landfill (Quebec, Canada) were adopted to build the reference simulation of the parametric study. The behavior of the upward flow of biogas for this particular material was analyzed based on its gas intrinsic permeability function, which was obtained in the laboratory. The parameters that most influenced the distribution and the ease of biogas flow at the base of the MOL were the saturated hydraulic conductivity and pore size distribution of the MOL material, whose effects were intensified as the slope of the interface increased. The effect of initial dry density was also assessed herein. Selection of the MOL material must be made bearing in mind that these three parameters are key in the effort to prevent unwanted restriction in the upward flow of biogas, which may result in the redirection of biogas towards the top of the slope, leading to high CH 4 fluxes (hotspots). In a well-designed PMOB, upward flow of biogas across the GDL-MOL interface is

  13. Understanding the performance and mechanism of Mg-containing oxides as support catalysts in the thermal dry reforming of methane.

    Science.gov (United States)

    Khairudin, Nor Fazila; Sukri, Mohd Farid Fahmi; Khavarian, Mehrnoush; Mohamed, Abdul Rahman

    2018-01-01

    Dry reforming of methane (DRM) is one of the more promising methods for syngas (synthetic gas) production and co-utilization of methane and carbon dioxide, which are the main greenhouse gases. Magnesium is commonly applied in a Ni-based catalyst in DRM to improve catalyst performance and inhibit carbon deposition. The aim of this review is to gain better insight into recent developments on the use of Mg as a support or promoter for DRM catalysts. Its high basicity and high thermal stability make Mg suitable for introduction into the highly endothermic reaction of DRM. The introduction of Mg as a support or promoter for Ni-based catalysts allows for good metal dispersion on the catalyst surface, which consequently facilitates high catalytic activity and low catalyst deactivation. The mechanism of DRM and carbon formation and reduction are reviewed. This work further explores how different constraints, such as the synthesis method, metal loading, pretreatment, and operating conditions, influence the dry reforming reactions and product yields. In this review, different strategies for enhancing catalytic activity and the effect of metal dispersion on Mg-containing oxide catalysts are highlighted.

  14. A novel surface-enhanced Raman scattering (SERS) detection for natural gas exploration using methane-oxidizing bacteria.

    Science.gov (United States)

    Liang, Weiwei; Chen, Qiao; Peng, Fang; Shen, Aiguo; Hu, Jiming

    2018-07-01

    Methane-oxidizing bacteria (MOB), a unique group of Gram-negative bacteria utilizing methane as a sole source of carbon and energy, have been proved to be a biological indicator for gas prospecting. Field and cultivation-free detection of MOB is important but still challenging in current microbial prospecting of oil and gas (MPOG) system. Herein, SERS was used for the first time to our knowledge to investigate two species of methanotrophs and four closely relevant bacteria that universally coexisted in the upper soil of natural gas. A special but very simple approach was utilized to make silver nanoparticles (Ag NPs) sufficiently contact with every single bacterial cell, and highly strong and distinct Raman signals free from any native fluorescence have been obtained, and successfully utilized for distinguishing MOB from other species. A more convincing multi-Raman criterion based on single Raman bands, and further the entire Raman spectrum in combination with statistical analysis (e.g., principal component analysis (PCA)), which were found capable of classifying MOB related bacterial cells in soil with an accuracy of 100%. This study therefore demonstrated sensitive and rapid SERS measurement technique accompanied by complete Raman database of various gas reservoirs related bacteria could aid field exploration of natural gas reservoir. Copyright © 2018 Elsevier B.V. All rights reserved.

  15. Methane and nitrous oxide emissions from animal manure management, 1990 - 2003 - Background document on the calculation method for the Dutch National Inventory Report

    NARCIS (Netherlands)

    Hoek KW van der; Schijndel MW van; MNP; LVM

    2006-01-01

    Since 2005 the Netherlands has used a new country-specific method to calculate the methane and nitrous oxide emissions from animal manure management. Compared to the default methods provided by the Intergovernmental Panel on Climate Change, this method has led to a more realistic estimate of the

  16. Experimental and Modeling Investigation of the Effect of H2S Addition to Methane on the Ignition and Oxidation at High Pressures

    NARCIS (Netherlands)

    Gersen, Sander; van Essen, Martijn; Darmeveil, Harry; Hashemi, Hamid; Rasmussen, Christian Tihic; Christensen, Jakob Munkholdt; Glarborg, Peter; Levinsky, Howard

    The autoignition and oxidation behavior of CH4/H2S mixtures has been studied experimentally in a rapid compression machine (RCM) and a high-pressure flow reactor. The RCM measurements show that the addition of 1% H2S to methane reduces the autoignition delay time by a factor of 2 at pressures

  17. Insight into the structure of Pd/ZrO2 during the total oxidation of methane using combined in situ XRD, X.-ray absorption and Raman spectroscopy

    DEFF Research Database (Denmark)

    Grunwaldt, Jan-Dierk; van Vegten, Niels; Baiker, Alfons

    2009-01-01

    The structure of palladium during the total combustion of methane has been studied by a combination of the complementary in situ techniques X-ray absorption spectroscopy, Raman spectroscopy and X-ray diffraction. The study demonstrates that finely dispersed and oxidized palladium is most active f...

  18. Effects of the 2014 major Baltic inflow on methane and nitrous oxide dynamics in the water column of the central Baltic Sea

    DEFF Research Database (Denmark)

    Myllykangas, Jukka-Pekka; Jilbert, Tom; Jakobs, Gunnar

    2017-01-01

    In late 2014, a large, oxygen-rich salt water inflow entered the Baltic Sea and caused considerable changes in deep water oxygen concentrations. We studied the effects of the inflow on the concentration patterns of two greenhouse gases, methane and nitrous oxide, during the following year (2015...

  19. Methane, Carbon Dioxide and Nitrous Oxide Fluxes in Soil Profile under a Winter Wheat-Summer Maize Rotation in the North China Plain

    NARCIS (Netherlands)

    Wang, Y.Y.; Hu, C.S.; Ming, H.; Oenema, O.; Schaefer, D.A.; Dong, W.X.; Zhang, Y.M.; Li, X.X.

    2014-01-01

    The production and consumption of the greenhouse gases (GHGs) methane (CH4), carbon dioxide (CO2) and nitrous oxide (N2O) in soil profile are poorly understood. This work sought to quantify the GHG production and consumption at seven depths (0-30, 30-60, 60-90, 90-150, 150-200, 200-250 and 250-300

  20. Statistical Analysis of Past Catalytic Data on Oxidative Methane Coupling for New Insights into the Composition of High-Performance Catalysts

    Czech Academy of Sciences Publication Activity Database

    Zavyalova, U.; Holeňa, Martin; Schlögl, R.; Baerns, M.

    2011-01-01

    Roč. 3, č. 12 (2011), s. 1935-1947 ISSN 1867-3880 Institutional research plan: CEZ:AV0Z10300504 Keywords : catalyst development * heterogeneous catalysis * methane * oxidative coupling * catalyst composition * statistical analysis Subject RIV: IN - Informatics, Computer Science Impact factor: 5.207, year: 2011

  1. Soil-atmosphere exchange of nitrous oxide, methane and carbon dioxide in a gradient of elevation in the coastal Brazilian Atlantic forest

    Science.gov (United States)

    E. Sousa Neto; J.B. Carmo; Michael Keller; S.C. Martins; L.F. Alves; S.A. Vieira; M.C. Piccolo; P. Camargo; H.T.Z. Couto; C.A. Joly; L.A. Martinelli

    2011-01-01

    Soils of tropical forests are important to the global budgets of greenhouse gases. The Brazilian Atlantic Forest is the second largest tropical moist forest area of South America, after the vast Amazonian domain. This study aimed to investigate the emissions of nitrous oxide (N2O), carbon dioxide (CO2) and methane (CH4) fluxes along an altitudinal transect and the...

  2. Effect of bio-column composed of aged refuse on methane abatement--a novel configuration of biological oxidation in refuse landfill.

    Science.gov (United States)

    Han, Dan; Zhao, Youcai; Xue, Binjie; Chai, Xiaoli

    2010-01-01

    An experimental bio-column composed of aged refuse was installed around the exhaust pipe as a new way to mitigate methane in refuse landfill. One of the objectives of this work was to assess the effect of aged refuse thickness in bio-column on reducing CH4 emissions. Over the study period, methane oxidation was observed at various thicknesses, 5 cm (small size), 10 cm (middle size) and 15 cm (large size), representing one to three times of pipeline diameters. The middle and large size both showed over 90% methane conversion, and the highest methane conversion rate of above 95% occurred in the middle-size column cell. Michaelis-Menten equation addressed the methanotrophs diffusion in different layers of the bio-columns. Maximum methanotrophic activity (Vmax) measured at the three thicknesses ranged from 6.4 x 10(-3) to 15.6 x 10(-3) units, and the half-saturation value (K(M)) ranged from 0.85% to 1.67%. Both the highest Vmax and K(M) were observed at the middle-size of the bio-column, as well as the largest methanotrophs population, suggesting a significant efficiency of methane mitigation happened in the optimum zone with greatest affinity and methanotrophic bacteria activities. Therefore, bio-column is a potential style for methane abatement in landfill, and the aged refuse both naturally formed and artificially placed in the column plays a critical role in CH4 emission.

  3. Methane production and oxidation in lakes impacted by the May 18, 1980 eruption of Mount St. Helens

    International Nuclear Information System (INIS)

    Lilley, M.D.; Baross, J.A.; Dahm, C.N.

    1988-01-01

    The concentrations of CH 4 and CH 4 oxidation rates were measured in lakes impacted by the May 18, 1980 eruption of Mount St. Helens. The highest CH 4 concentrations were recorded during the first summer after the eruption and ranged in surface waters from 5 microM in the moderately impacted Ryan Lake to 28 microM in the heavily impacted North Coldwater Lake. At depths below the oxic/anoxic interface, CH 4 levels reached 250 microM in North Coldwater Lake, 184 microM in Spirit Lake, 70 microM in Castle Creek lake, and 60 microM in Ryan Lake. The CH 4 flux measurements from these lakes during the summer following the May 18, 1980 eruption were the highest ever recorded in lakes with ranges of 1.1-2.9 mmol CH 4 /sq m/day in the light to moderately impacted McBride and Ryan Lakes to ranges of 17.4-25.3 mmol CH 4 /sq m/day in the heavily impacted Castle Creek, North Coldwater, and Spirit Lakes. Evidence of CH 4 oxidation was seen in all of the lakes during the summer of 1981, and rates of CH 4 oxidation using C 14 -CH 4 were measured in spirit Lake from 1982 to 1986. The highest rates of CH 4 oxidation measured were during the summer stratification and ranged from 50 to 150 nmol CH 4 oxidized/L/day. methane oxidation rates were measured in waters having oxygen concentrations less than 100 microM with highest activity occurring at concentrations of 30-60 microM. 36 refs., 12 figs. 3 tabs

  4. Biotechnological aspects of anaerobic oxidation of methane coupled to sulfate reduction

    NARCIS (Netherlands)

    Meulepas, R.J.W.

    2009-01-01

    Sulfate reduction (SR) can be used for the removal and recovery of metals and oxidized sulfur compounds from waste streams. Sulfate-reducing bacteria reduce oxidized sulfur compounds to sulfide. Subsequently, sulfide can precipitate dissolved metals or can be oxidized to elemental sulfur. Both metal

  5. Early drainage mitigates methane and nitrous oxide emissions from organically amended paddy soils

    DEFF Research Database (Denmark)

    Tariq, Azeem; Jensen, Lars Stoumann; de Tourdonnet, Stephane

    2017-01-01

    Elevated greenhouse gas (GHG) emissions, particularly of methane (CH4) from flooded rice production systems contribute to global warming. Different crop management strategies, such as drainage of paddy soils and climate-smart residue management, are essential in order to mitigate GHG emissions from...... flooded rice systems, but they often conflict with practical management preferences.The aim of this study was to assess the potential of early-season drainage for mitigating CH4 and N2O emissions from soils with and without added organic amendments in relation to native soil organic carbon (SOC). Rice...

  6. The Influence of oxide additives on Ni/Al2O3 catalysts in low temperature methane steam reforming

    International Nuclear Information System (INIS)

    Lazar, Mihaela; Dan, Monica; Mihet, Maria; Almasan, Valer

    2009-01-01

    Hydrogen is industrially produced by methane steam reforming. The process is catalytic and the usual catalyst is based on Ni as the active element. The main problem of this process is its inefficiency. It requires high temperatures at which Ni also favors the formation of graphite, which deactivates the catalysts. Ni has the advantage of being much cheaper than noble metal catalysts, so many researches are done in order to improve the properties of supported Ni catalysts and to decrease the temperature at which the process is energetically efficient. In order to obtain catalysts with high activity and stability, it is essential to maintain the dispersion of the active phase (Ni particles) and the stability of the support. Both properties can be improved by addition of a second oxide to the support. In this paper we present the results obtained in preparation and characterization of Ni/Al 2 O 3 catalysts modified by addition of CeO 2 and La 2 O 3 to alumina support. The following catalysts were prepared by impregnation method: Ni/Al 2 O 3 , Ni/CeO 2 -Al 2 O 3 and Ni/La 2 O 3 -Al 2 O 3 (10 wt.% Ni and 6 wt.% additional oxide). The catalytic surface was characterized by N 2 adsorption - desorption isotherms. The hydrogen - surface bond was characterized by Thermo-Programmed-Desorption (TPD) method. All catalysts were tested in steam reforming reaction of methane in the range of 600 - 700 deg. C, at atmospheric pressure working with CH 4 :H 2 O ratio of 1:3. The modified catalysts showed a better catalytic activity and selectivity for H 2 and CO 2 formation, at lower temperatures than the simple Ni/Al 2 O 3 catalyst. (authors)

  7. Partial catalytic oxidation of CH{sub 4} to synthesis gas for power generation - Final report

    Energy Technology Data Exchange (ETDEWEB)

    Mantzaras, I.; Schneider, A.

    2006-03-15

    The partial oxidation of methane to synthesis gas over rhodium catalysts has been investigated experimentally and numerically in the pressure range of 4 to 10 bar. The methane/oxidizer feed has been diluted with large amounts of H{sub 2}O and CO{sub 2} (up to 70% vol.) in order to simulate new power generation cycles with large exhaust gas recycle. Experiments were carried out in an optically accessible channel-flow reactor that facilitated laser-based in situ measurements, and also in a subscale gas-turbine catalytic reactor. Full-elliptic steady and transient two-dimensional numerical codes were used, which included elementary hetero-/homogeneous chemical reaction schemes. The following are the key conclusions: a) Heterogeneous (catalytic) and homogeneous (gas-phase) schemes have been validated for the partial catalytic oxidation of methane with large exhaust gas recycle. b) The impact of added H{sub 2}O and CO{sub 2} has been elucidated. The added H{sub 2}O increased the methane conversion and hydrogen selectivity, while it decreased the CO selectivity. The chemical impact of CO{sub 2} (dry reforming) was minimal. c) The numerical model reproduced the measured catalytic ignition times. It was further shown that the chemical impact of H{sub 2}O and CO{sub 2} on the catalytic ignition delay times was minimal. d) The noble metal dispersion increased with different support materials, in the order Rh/{alpha}-Al{sub 2}O{sub 3}, Rh/ZrO{sub 2}, and Rh/Ce-ZrO{sub 2}. An evident relationship was established between the noble metal dispersion and the catalytic behavior. (authors)

  8. Rational design of Mg-Al mixed oxide-supported bimetallic catalysts for dry reforming of methane

    Energy Technology Data Exchange (ETDEWEB)

    Tsyganok, Andrey I. [Centre for Catalysis Research and Innovation, Department of Chemistry, University of Ottawa, D' Iorio Hall, 10 Marie Curie Street, Ottawa, Ont. (Canada); Inaba, Mieko [Natural Gas Technology Development Team, Teikoku Oil Co., 9-23-30 Kitakarasuyama, Setagaya-ku, Tokyo 157-0061 (Japan); Tsunoda, Tatsuo; Uchida, Kunio; Suzuki, Kunio; Hayakawa, Takashi [Institute for Materials and Chemical Process, National Institute of Advanced Industrial Science and Technology (AIST), Tsukuba Central 5, 1-1-1 Higashi, Tsukuba 305-8565 (Japan); Takehira, Katsuomi [Department of Applied Chemistry, Faculty of Engineering, Hiroshima University, 1-4-1 Kagamiyama, Higashi-Hiroshima 739-8527 (Japan)

    2005-09-18

    A novel synthetic strategy for preparing bimetallic Ru-M (M=Cr, Fe, Co, Ni and Cu) catalysts, supported on Mg-Al mixed oxide, has been introduced. It was based on a 'memory effect', i.e. on the ability of Mg-Al mixed oxide to reconstruct a layered structure upon rehydration with an aqueous solution. By repeated calcinations-rehydration cycles, layered double hydroxide (LDH) precursors of catalysts containing two different metals were synthesized. Bimetallic catalysts were then generated (1) in situ from LDH under methane reforming reaction conditions and (2) from mixed metal oxides obtained by preliminary LDH calcination. Among all the LDH-derived catalysts, a Ru{sup 0.1%}-Ni{sup 5.0%}/MgAlO{sub x} sample revealed the highest activity and selectivity to syngas, a suitable durability and a low coking capacity. A promoting effect of ruthenium on catalytic function of supported nickel was demonstrated. Preliminary LDH calcination was shown to markedly affect the catalytic activity of the derived catalysts and especially their coking properties.

  9. Seasonal variability in methane and nitrous oxide fluxes from tropical peatlands in the western Amazon basin

    Directory of Open Access Journals (Sweden)

    Y. A. Teh

    2017-08-01

    Full Text Available The Amazon plays a critical role in global atmospheric budgets of methane (CH4 and nitrous oxide (N2O. However, while we have a relatively good understanding of the continental-scale flux of these greenhouse gases (GHGs, one of the key gaps in knowledge is the specific contribution of peatland ecosystems to the regional budgets of these GHGs. Here we report CH4 and N2O fluxes from lowland tropical peatlands in the Pastaza–Marañón foreland basin (PMFB in Peru, one of the largest peatland complexes in the Amazon basin. The goal of this research was to quantify the range and magnitude of CH4 and N2O fluxes from this region, assess seasonal trends in trace gas exchange, and determine the role of different environmental variables in driving GHG flux. Trace gas fluxes were determined from the most numerically dominant peatland vegetation types in the region: forested vegetation, forested (short pole vegetation, Mauritia flexuosa-dominated palm swamp, and mixed palm swamp. Data were collected in both wet and dry seasons over the course of four field campaigns from 2012 to 2014. Diffusive CH4 emissions averaged 36.05 ± 3.09 mg CH4–C m−2 day−1 across the entire dataset, with diffusive CH4 flux varying significantly among vegetation types and between seasons. Net ebullition of CH4 averaged 973.3 ± 161.4 mg CH4–C m−2 day−1 and did not vary significantly among vegetation types or between seasons. Diffusive CH4 flux was greatest for mixed palm swamp (52.0 ± 16.0 mg CH4–C m−2 day−1, followed by M. flexuosa palm swamp (36.7 ± 3.9 mg CH4–C m−2 day−1, forested (short pole vegetation (31.6 ± 6.6 mg CH4–C m−2 day−1, and forested vegetation (29.8 ± 10.0 mg CH4–C m−2 day−1. Diffusive CH4 flux also showed marked seasonality, with divergent seasonal patterns among ecosystems. Forested vegetation and mixed palm swamp showed significantly higher

  10. Seasonal variability in methane and nitrous oxide fluxes from tropical peatlands in the western Amazon basin

    Science.gov (United States)

    Arn Teh, Yit; Murphy, Wayne A.; Berrio, Juan-Carlos; Boom, Arnoud; Page, Susan E.

    2017-08-01

    The Amazon plays a critical role in global atmospheric budgets of methane (CH4) and nitrous oxide (N2O). However, while we have a relatively good understanding of the continental-scale flux of these greenhouse gases (GHGs), one of the key gaps in knowledge is the specific contribution of peatland ecosystems to the regional budgets of these GHGs. Here we report CH4 and N2O fluxes from lowland tropical peatlands in the Pastaza-Marañón foreland basin (PMFB) in Peru, one of the largest peatland complexes in the Amazon basin. The goal of this research was to quantify the range and magnitude of CH4 and N2O fluxes from this region, assess seasonal trends in trace gas exchange, and determine the role of different environmental variables in driving GHG flux. Trace gas fluxes were determined from the most numerically dominant peatland vegetation types in the region: forested vegetation, forested (short pole) vegetation, Mauritia flexuosa-dominated palm swamp, and mixed palm swamp. Data were collected in both wet and dry seasons over the course of four field campaigns from 2012 to 2014. Diffusive CH4 emissions averaged 36.05 ± 3.09 mg CH4-C m-2 day-1 across the entire dataset, with diffusive CH4 flux varying significantly among vegetation types and between seasons. Net ebullition of CH4 averaged 973.3 ± 161.4 mg CH4-C m-2 day-1 and did not vary significantly among vegetation types or between seasons. Diffusive CH4 flux was greatest for mixed palm swamp (52.0 ± 16.0 mg CH4-C m-2 day-1), followed by M. flexuosa palm swamp (36.7 ± 3.9 mg CH4-C m-2 day-1), forested (short pole) vegetation (31.6 ± 6.6 mg CH4-C m-2 day-1), and forested vegetation (29.8 ± 10.0 mg CH4-C m-2 day-1). Diffusive CH4 flux also showed marked seasonality, with divergent seasonal patterns among ecosystems. Forested vegetation and mixed palm swamp showed significantly higher dry season (47.2 ± 5.4 mg CH4-C m-2 day-1 and 85.5 ± 26.4 mg CH4-C m-2 day-1, respectively) compared to wet season emissions

  11. Solid oxide fuel cells towards real life applications. Final report

    Energy Technology Data Exchange (ETDEWEB)

    2010-07-01

    Solid Oxide Fuel Cells offer a clean and efficient way of producing electricity and heat from a wide selection of fuels. The project addressed three major challenges to be overcome by the technology to make commercialisation possible. (1) At the cell level, increased efficiency combined with production cost reduction has been achieved through an optimization of the manufacturing processes, b) by using alternative raw materials with a lower purchase price and c) by introducing a new generation of fuel cells with reduced loss and higher efficiency. (2) At the stack level, production cost reduction is reduced and manufacturing capacity is increased through an optimization of the stack production. (3) At the system level, development of integrated hotbox concepts for the market segments distributed generation (DG), micro combined heat and power (mCHP), and auxiliary power units (APU) have been developed. In the mCHP segment, two concepts have been developed and validated with regards to market requirements and scalability. In the APU-segment, different types of reformers have been tested and it has been proven that diesel can be reformed through appropriate reformers. Finally, operation experience and feedback has been gained by deployment of stacks in the test facility at the H.C. OErsted Power Plant (HCV). This demonstration has been carried out in collaboration between TOFC and DONG Energy Power A/S (DONG), who has participated as a subcontractor to TOFC. The demonstration has given valuable knowledge and experience with design, start-up and operation of small power units connected to the grid and future development within especially the mCHP segment will benefit from this. In this report, the project results are described for each of the work packages in the project. (Author)

  12. Identification of a Methane Oxidation Intermediate on Solid Oxide Fuel Cell Anode Surfaces with Fourier Transform Infrared Emission.

    Science.gov (United States)

    Pomfret, Michael B; Steinhurst, Daniel A; Owrutsky, Jeffrey C

    2013-04-18

    Fuel interactions on solid oxide fuel cell (SOFC) anodes are studied with in situ Fourier transform infrared emission spectroscopy (FTIRES). SOFCs are operated at 800 °C with CH4 as a representative hydrocarbon fuel. IR signatures of gas-phase oxidation products, CO2(g) and CO(g), are observed while cells are under load. A broad feature at 2295 cm(-1) is assigned to CO2 adsorbed on Ni as a CH4 oxidation intermediate during cell operation and while carbon deposits are electrochemically oxidized after CH4 operation. Electrochemical control provides confirmation of the assignment of adsorbed CO2. FTIRES has been demonstrated as a viable technique for the identification of fuel oxidation intermediates and products in working SOFCs, allowing for the elucidation of the mechanisms of fuel chemistry.

  13. Effects of the 2014 major Baltic inflow on methane and nitrous oxide dynamics in the water column of the central Baltic Sea

    Science.gov (United States)

    Myllykangas, Jukka-Pekka; Jilbert, Tom; Jakobs, Gunnar; Rehder, Gregor; Werner, Jan; Hietanen, Susanna

    2017-09-01

    In late 2014, a large, oxygen-rich salt water inflow entered the Baltic Sea and caused considerable changes in deep water oxygen concentrations. We studied the effects of the inflow on the concentration patterns of two greenhouse gases, methane and nitrous oxide, during the following year (2015) in the water column of the Gotland Basin. In the eastern basin, methane which had previously accumulated in the deep waters was largely removed during the year. Here, volume-weighted mean concentration below 70 m decreased from 108 nM in March to 16.3 nM over a period of 141 days (0.65 nM d-1), predominantly due to oxidation (up to 79 %) following turbulent mixing with the oxygen-rich inflow. In contrast nitrous oxide, which was previously absent from deep waters, accumulated in deep waters due to enhanced nitrification following the inflow. Volume-weighted mean concentration of nitrous oxide below 70 m increased from 11.8 nM in March to 24.4 nM in 141 days (0.09 nM d-1). A transient extreme accumulation of nitrous oxide (877 nM) was observed in the deep waters of the Eastern Gotland Basin towards the end of 2015, when deep waters turned anoxic again, sedimentary denitrification was induced and methane was reintroduced to the bottom waters. The Western Gotland Basin gas biogeochemistry was not affected by the inflow.

  14. Integration of CO2 air capture and solid oxide electrolysis for methane production

    DEFF Research Database (Denmark)

    Ebbehøj, Søren Lyng

    from all sectors of the energy system except for transportation. In the recently published Energikoncept 2035 [1], the Danish grid operator, Energinet.dk lays out a scenario based on 72 % wind power and 21 %biomass and waste in the electricity grid mix. In this scenario, biogas and electrolysis gasses....... were estimated according to standard methods.The plant had a yearly production capacity of 575,000 Nm3 of SNG with a methane content above 98.5 % which resulted in a Wobbe index of 49 MJ/Nm3 which is sufficient for injection into the natural gas grid. The SOEC stack power was around 700 k...... are projected to be used for production of process heat, peak-load power generation and on the longer term to replace hydrocarbons in the most energy intensive parts of the transportation sector; especially aviation. As a prerequisite for the scenario, no biomass can be imported to enhance the supply...

  15. Supercritical water oxidation data acquisition testing. Final report, Volume I

    International Nuclear Information System (INIS)

    1996-11-01

    This report discusses the phase one testing of a data acquisition system for a supercritical water waste oxidation system. The system is designed to destroy a wide range of organic materials in mixed wastes. The design and testing of the MODAR Oxidizer is discussed. An analysis of the optimized runs is included

  16. Systematic Identification of Promoters for Methane Oxidation Catalysts Using Size- and Composition-Controlled Pd-Based Bimetallic Nanocrystals.

    Science.gov (United States)

    Willis, Joshua J; Goodman, Emmett D; Wu, Liheng; Riscoe, Andrew R; Martins, Pedro; Tassone, Christopher J; Cargnello, Matteo

    2017-08-30

    Promoters enhance the performance of catalytic active phases by increasing rates, stability, and/or selectivity. The process of identifying promoters is in most cases empirical and relies on testing a broad range of catalysts prepared with the random deposition of active and promoter phases, typically with no fine control over their localization. This issue is particularly relevant in supported bimetallic systems, where two metals are codeposited onto high-surface area materials. We here report the use of colloidal bimetallic nanocrystals to produce catalysts where the active and promoter phases are colocalized to a fine extent. This strategy enables a systematic approach to study the promotional effects of several transition metals on palladium catalysts for methane oxidation. In order to achieve these goals, we demonstrate a single synthetic protocol to obtain uniform palladium-based bimetallic nanocrystals (PdM, M = V, Mn, Fe, Co, Ni, Zn, Sn, and potentially extendable to other metal combinations) with a wide variety of compositions and sizes based on high-temperature thermal decomposition of readily available precursors. Once the nanocrystals are supported onto oxide materials, thermal treatments in air cause segregation of the base metal oxide phase in close proximity to the Pd phase. We demonstrate that some metals (Fe, Co, and Sn) inhibit the sintering of the active Pd metal phase, while others (Ni and Zn) increase its intrinsic activity compared to a monometallic Pd catalyst. This procedure can be generalized to systematically investigate the promotional effects of metal and metal oxide phases for a variety of active metal-promoter combinations and catalytic reactions.

  17. Selective catalytic reduction of nitrogen oxides from industrial gases by hydrogen or methane; Reduction catalytique selective des oxydes d'azote (NO{sub x}) provenant d'effluents gazeux industriels par l'hydrogene ou le methane

    Energy Technology Data Exchange (ETDEWEB)

    Engelmann Pirez, M

    2004-12-15

    This work deals with the selective catalytic reduction of nitrogen oxides (NO{sub x}), contained in the effluents of industrial plants, by hydrogen or methane. The aim is to replace ammonia, used as reducing agent, in the conventional process. The use of others reducing agents such as hydrogen or methane is interesting for different reasons: practical, economical and ecological. The catalyst has to convert selectively NO into N{sub 2}, in presence of an excess of oxygen, steam and sulfur dioxide. The developed catalyst is constituted by a support such as perovskites, particularly LaCoO{sub 3}, on which are dispersed noble metals (palladium, platinum). The interaction between the noble metal and the support, generated during the activation of the catalyst, allows to minimize the water and sulfur dioxide inhibitor phenomena on the catalytic performances, particularly in the reduction of NO by hydrogen. (O.M.)

  18. Using 13C isotopes to explore denitrification-dependent anaerobic methane oxidation in a paddy-peatland.

    Science.gov (United States)

    Shi, Yao; Wang, Zhongqiang; He, Chunguang; Zhang, Xinyu; Sheng, Lianxi; Ren, Xiaodong

    2017-01-18

    Peatlands are organic-matter-rich but nitrogen-limited natural systems, the carbon/nitrogen (C/N) status of which are subject to increasing exposure from long-term nitrate (NO 3 - ) fertilizer inputs and atmospheric nitrogen (N) deposits. To manage and protect these unique environments, an improved understanding of denitrification-dependent anaerobic oxidation of methane (DAMO) in peatlands is needed. In this study, we used stable isotope measurements and incubation with NO 3 - additions to facilitate an investigation and comparison of the potential DAMO rates in a paddy-peatland that has been influenced by N fertilizer over 40 years and an undisturbed peatland in northeast China. Monitoring of 13 CO 2 production confimed DAMO did occur in both the paddy-peatland and the undisturbed peatland, the rates of which increased with NO 3 - additions, but decreased logarithmically with time. When NO 3 - was added, there were no significant differences between the CH 4 oxidation in the paddy-peatland and peatland samples after 36 hours of incubation (97.08 vs. 143.69 nmol g -1 dry peat) and the potential DAMO rate after incubation for 1 hour (92.53 vs. 69.99 nmol g -1  h -1 ). These results indicate that the occurrence of DAMO in peatlands might be controlled by the amount of NO 3 - applied and the depth to which it penetrates into the anoxic layer.

  19. Internal reforming characteristics of cermet supported solid oxide fuel cell using yttria stabilized zirconia fed with partially reformed methane

    Energy Technology Data Exchange (ETDEWEB)

    Momma, Akihiko; Takano, Kiyonami; Tanaka, Yohei; Negishi, Akira; Kato, Ken; Nozaki, Ken; Kato, Tohru [Energy Technology Research Institute, National Institute of Advanced Industrial Science and Technology, 1-1-1 Umezono Tsukuba Ibaraki, 305-8568 (Japan); Ichigi, Takenori; Matsuda, Kazuyuki; Ryu, Takashi [Application Development Project, Corporate R and D, NGK Insulators, Ltd., 2-56 Suda-cho Mizuho-ku Nagoya-shi Aichi, 467-8530 (Japan)

    2009-08-01

    In order to investigate the internal reforming characteristics in a cermet supported solid oxide fuel cell (SOFC) using YSZ as the electrolyte, the concentration profiles of the gaseous species along the gas flow direction in the anode were measured. Partially reformed methane using a pre-reformer kept at a constant temperature is supplied to the center of the cell which is operated with a seal-less structure at the gas outlet. The anode gas is sucked in via silica capillaries to the initially evacuated gas tanks. The process is simultaneously carried out using five sampling ports. The sampled gas is analyzed by a gas chromatograph. Most of the measurements are made at the cell temperature (T{sub cell}) of 750 C and at various temperatures of the pre-reformer (T{sub ref}) with various fuel utilizations (U{sub f}) of the cell. The composition of the fuel at the inlet of the anode was confirmed to be almost the same as that theoretically calculated assuming equilibrium at the temperature of the pre-reformer. The effect of internal reforming in the anode is clearly observed as a steady decrease in the methane concentration along the flow axis. The effect of the water-gas shift reaction is also observed as a decrease in the CO{sub 2} concentration and an increase of CO concentration around the gas inlet region, as the water-gas shift reaction inversely proceeds when T{sub cell} is higher than T{sub ref}. The diffusion of nitrogen from the seal-less outermost edge is observed, and the diffusion is confirmed to be more significant as U{sub f} decreases. The observations are compared with the results obtained by the SOFC supported by lanthanum gallate electrolyte. With respect to the internal reforming performance, the cell investigated here is found to be more effective when compared to the previously reported electrolyte supported cell. (author)

  20. Internal reforming characteristics of cermet supported solid oxide fuel cell using yttria stabilized zirconia fed with partially reformed methane

    Science.gov (United States)

    Momma, Akihiko; Takano, Kiyonami; Tanaka, Yohei; Negishi, Akira; Kato, Ken; Nozaki, Ken; Kato, Tohru; Ichigi, Takenori; Matsuda, Kazuyuki; Ryu, Takashi

    In order to investigate the internal reforming characteristics in a cermet supported solid oxide fuel cell (SOFC) using YSZ as the electrolyte, the concentration profiles of the gaseous species along the gas flow direction in the anode were measured. Partially reformed methane using a pre-reformer kept at a constant temperature is supplied to the center of the cell which is operated with a seal-less structure at the gas outlet. The anode gas is sucked in via silica capillaries to the initially evacuated gas tanks. The process is simultaneously carried out using five sampling ports. The sampled gas is analyzed by a gas chromatograph. Most of the measurements are made at the cell temperature (T cell) of 750 °C and at various temperatures of the pre-reformer (T ref) with various fuel utilizations (U f) of the cell. The composition of the fuel at the inlet of the anode was confirmed to be almost the same as that theoretically calculated assuming equilibrium at the temperature of the pre-reformer. The effect of internal reforming in the anode is clearly observed as a steady decrease in the methane concentration along the flow axis. The effect of the water-gas shift reaction is also observed as a decrease in the CO 2 concentration and an increase of CO concentration around the gas inlet region, as the water-gas shift reaction inversely proceeds when T cell is higher than T ref. The diffusion of nitrogen from the seal-less outermost edge is observed, and the diffusion is confirmed to be more significant as U f decreases. The observations are compared with the results obtained by the SOFC supported by lanthanum gallate electrolyte. With respect to the internal reforming performance, the cell investigated here is found to be more effective when compared to the previously reported electrolyte supported cell.

  1. The effect of noble metals on catalytic methanation reaction over supported Mn/Ni oxide based catalysts

    Directory of Open Access Journals (Sweden)

    Wan Azelee Wan Abu Bakar

    2015-09-01

    Full Text Available Carbon dioxide (CO2 in sour natural gas can be removed using green technology via catalytic methanation reaction by converting CO2 to methane (CH4 gas. Using waste to wealth concept, production of CH4 would increase as well as creating environmental friendly approach for the purification of natural gas. In this research, a series of alumina supported manganese–nickel oxide based catalysts doped with noble metals such as ruthenium and palladium were prepared by wetness impregnation method. The prepared catalysts were run catalytic screening process using in-house built micro reactor coupled with Fourier Transform Infra Red (FTIR spectroscopy to study the percentage CO2 conversion and CH4 formation analyzed by GC. Ru/Mn/Ni(5:35:60/Al2O3 calcined at 1000 °C was found to be the potential catalyst which gave 99.74% of CO2 conversion and 72.36% of CH4 formation at 400 °C reaction temperature. XRD diffractogram illustrated that the supported catalyst was in polycrystalline with some amorphous state at 1000 °C calcination temperature with the presence of NiO as active site. According to FESEM micrographs, both fresh and used catalysts displayed spherical shape with small particle sizes in agglomerated and aggregated mixture. Nitrogen Adsorption analysis revealed that both catalysts were in mesoporous structures with BET surface area in the range of 46–60 m2/g. All the impurities have been removed at 1000 °C calcination temperature as presented by FTIR, TGA–DTA and EDX data.

  2. Advanced manufacturing of intermediate temperature, direct methane oxidation membrane electrode assemblies for durable solid oxide fuel cell, Phase I

    Data.gov (United States)

    National Aeronautics and Space Administration — ITN proposes to create an innovative anode supported membrane electrode assembly (MEA) for solid oxide fuel cells (SOFCs) that is capable of long-term operation at...

  3. Improving methane gas sensing properties of multi-walled carbonnanotubes by vanadium oxide filling

    CSIR Research Space (South Africa)

    Chimowa, George

    2017-08-01

    Full Text Available Manipulation of electrical properties and hence gas sensing properties of multi-walled carbon nanotubes (MWNTs) by filling the inner wall with vanadium oxide is presented. Using a simple capillary technique, MWNTs are filled with vanadium metal...

  4. Methane production by anaerobic digestion of biomass. Final report of innovative research program subtask, December 1977--September 1978

    Energy Technology Data Exchange (ETDEWEB)

    Murphy, V G

    1978-10-01

    It has long been known that methane is produced during the anaerobic digestion of agricultural wastes, but this potential source of fuel has not been greatly exploited in the United States. The chief reason is that anaerobic decomposition of lignocellulosic materials occurs very slowly, resulting in a need for long detention times and large digestion vessels, both of which markedly increase process costs. However, recent work at CSU has shown that pretreatment of manure fibers (an abundant agricultural waste) with saturated steam at 130 to 210/sup 0/C renders this material more susceptible to attack by microbial enzymes. The main objectives of this project were to identify the chemical events occurring during the steam treatment and to correlate these with the rate of methane generating during subsequent anaerobic digestion. The study was expected to lead to an optimal pretreatment strategy.

  5. Methanation. Utilization of CO{sub 2} instead of final storage; Methanisierung. CO{sub 2} nutzen statt endlagern

    Energy Technology Data Exchange (ETDEWEB)

    Schmid, Juergen [Fraunhofer Institut fuer Windenergie und Energiesystemtechnik (IWES), Kassel (Germany); Wissenschaftlicher Beirat der Bundesregierung Globale Umweltveraenderungen (WBGU), Potsdam (Germany); Guenther, Matthias [Fraunhofer Institut fuer Windenergie und Energiesystemtechnik (IWES), Kassel (Germany)

    2013-03-15

    The capture and permanent storage of carbon dioxide (CCS) is a possibility to limit the anthropogenic climate change. However, the financial and technical challenges for CCS on a large scale are significant. In addition to CCS, also other possibilities have to be considered in order to limit the content of carbon dioxide in the atmosphere. The methanation of carbon dioxide is at least an interesting possibility in order to feed the greenhouse gas to an additional cycle of usage.

  6. Zircaloy cladding ID/OD oxidation studies. Final report

    International Nuclear Information System (INIS)

    Westerman, R.E.; Hesson, G.M.

    1977-11-01

    The ID/OD oxide ratio that forms on Zircaloy tubing at temperatures relevant to postulated LOCA conditions was measured as a function of time, temperature, and distance from the rupture. The average ratio at the rupture position was less than unity, and decreased with decreasing test time and increasing distance from the point of rupture. The maximum observed ID/OD oxide ratio was 1.4. Ratios in excess of unity were typically found to be a consequence of the OD oxide being thinner than would have been anticipated from the nominal test conditions. Confirmatory data were also obtained on the isothermal oxidation kinetics of Zircaloy. These data are in good agreement with those obtained by other investigators and confirm the conservative nature of the Baker-Just equation that is required for use in licensing calculations

  7. Illumina sequencing-based analysis of a microbial community enriched under anaerobic methane oxidation condition coupled to denitrification revealed coexistence of aerobic and anaerobic methanotrophs.

    Science.gov (United States)

    Siniscalchi, Luciene Alves Batista; Leite, Laura Rabelo; Oliveira, Guilherme; Chernicharo, Carlos Augusto Lemos; de Araújo, Juliana Calabria

    2017-07-01

    Methane is produced in anaerobic environments, such as reactors used to treat wastewaters, and can be consumed by methanotrophs. The composition and structure of a microbial community enriched from anaerobic sewage sludge under methane-oxidation condition coupled to denitrification were investigated. Denaturing gradient gel electrophoresis (DGGE) analysis retrieved sequences of Methylocaldum and Chloroflexi. Deep sequencing analysis revealed a complex community that changed over time and was affected by methane concentration. Methylocaldum (8.2%), Methylosinus (2.3%), Methylomonas (0.02%), Methylacidiphilales (0.45%), Nitrospirales (0.18%), and Methanosarcinales (0.3%) were detected. Despite denitrifying conditions provided, Nitrospirales and Methanosarcinales, known to perform anaerobic methane oxidation coupled to denitrification (DAMO) process, were in very low abundance. Results demonstrated that aerobic and anaerobic methanotrophs coexisted in the reactor together with heterotrophic microorganisms, suggesting that a diverse microbial community was important to sustain methanotrophic activity. The methanogenic sludge was a good inoculum to enrich methanotrophs, and cultivation conditions play a selective role in determining community composition.

  8. Methane isotopic signature of gas bubbles in permafrost winter lake ice: a tool for quantifying variable oxidation levels

    Science.gov (United States)

    Sapart, C. J.; Boereboom, T.; Roeckmann, T.; Tison, J.-L.

    2012-04-01

    Methane (CH4) is a strong greenhouse gas and its atmospheric mixing ratio has strongly increased since pre-industrial times. This increase was primarily due to emissions from anthropogenic sources, but there is growing concern about possible feedbacks of natural sources in a changing climate. Thawing of permafrost areas in the Arctic is considered as an important feedback, since the Arctic region undergoes the fastest climate change and hosts large carbon stocks. Subarctic lakes are considered as "hotspots" for CH4 emissions, but the role of the ice cover during the winter period is not well understood to date. Here, we present measurements of CH4 mixing ratio and δ13C-CH4 in 4 types of bubbles identified in subarctic lake ice covers located in a sporadic or discontinuous permafrost area. Our analysis reveals that different bubble types contain CH4 with different, specific isotopic signatures. The evolution of mixing ratio and δ13C-CH4 suggest that oxidation of dissolved CH4 is the most important process determining the isotopic composition of CH4 in bubbles. This results from gas exsolution occurring during the ice growth process. A first estimate of the CH4 oxidation budget (mean = 0.12 mg CH4 m-2 d-1) enables to quantify the impact of the ice cover on CH4 emissions from subartic lakes. The increased exchange time between gases coming from the sediments and the water column, due to the capping effect of the lake ice cover, reduces the amount of CH4 released "as is" and favours its oxidation into carbon dioxide; the latter being further added to the HCO3- pool through the carbonate equilibration reactions.

  9. Micro solid oxide fuel cell on the chip. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Stutz, M.; Hotz, N.; Bieri, N.; Poulikakos, D.

    2006-07-01

    The aim of this project is the numerical and experimental investigation of hydrocarbon-to-syngas reforming in micro reformers for incorporation into an entire micro fuel cell system. Numerical simulations are used to achieve deeper understanding of several determining aspects in such a micro reformer. These insights are used to optimize the reforming performance by proper choice of operational and geometrical parameters of a reformer. These numerical results are continued by comprehensive experimental studies. In the first chapter, the effect of wall conduction of a tubular methane micro reformer is investigated numerically. Methane is used as the representative hydrocarbon because its detailed surface reaction mechanism is known. It is found that the axial wall conduction can strongly influence the performance of the microreactor and should not be neglected without a careful a priori investigation of its impact. In the second chapter, the effect of the catalyst amount and reactor geometry on the reforming process was investigated. It was found that the hydrogen selectivity changes significantly with varying catalyst loading. Thus, the reaction path leading to higher hydrogen production becomes more important by increasing the catalyst surface site density on the active surface. Another unexpected result is the presence of optimum channel geometry and optimum catalyst amount. In the third chapter of this project, the capability of flame-made Rh/Ce{sub 0.5}Zr{sub 0.5}O{sub 2} nanoparticles catalyzing the reforming of butane to H{sub 2}- and CO-rich syngas was investigated experimentally in a packed bed reactor. The main goal of this study was the efficient reforming of butane at temperatures between 500 and 600 {sup o}C for a micro intermediate-temperature SOFC system. Our results showed that Rh/Ce{sub 0.5}Zr{sub 0.5}O{sub 2} nanoparticles proved to be a very promising material for butane-to-syngas reforming with complete butane conversion and a hydrogen yield of 77

  10. Electrode design for direct-methane micro-tubular solid oxide fuel cell (MT-SOFC)

    Science.gov (United States)

    Rabuni, Mohamad Fairus; Li, Tao; Punmeechao, Puvich; Li, Kang

    2018-04-01

    Herein, a micro-structured electrode design has been developed via a modified phase-inversion method. A thin electrolyte integrated with a highly porous anode scaffold has been fabricated in a single-step process and developed into a complete fuel cell for direct methane (CH4) utilisation. A continuous and well-dispersed layer of copper-ceria (Cu-CeO2) was incorporated inside the micro-channels of the anode scaffold. A complete cell was investigated for direct CH4 utilisation. The well-organised micro-channels and nano-structured Cu-CeO2 anode contributed to an increase in electrochemical reaction sites that promoted charge-transfer as well as facilitating gaseous fuel distribution, resulting in outstanding performances. Excellent electrochemical performances have been achieved in both hydrogen (H2) and CH4 operation. The power density of 0.16 Wcm-2 at 750 °C with dry CH4 as fuel is one of the highest ever reported values for similar anode materials.

  11. Bioelectrochemical enhancement of methane production from highly concentrated food waste in a combined anaerobic digester and microbial electrolysis cell.

    Science.gov (United States)

    Park, Jungyu; Lee, Beom; Tian, Donjie; Jun, Hangbae

    2018-01-01

    A microbial electrolysis cell (MEC) is a promising technology for enhancing biogas production from an anaerobic digestion (AD) reactor. In this study, the effects of the MEC on the rate of methane production from food waste were examined by comparing an AD reactor with an AD reactor combined with a MEC (AD+MEC). The use of the MEC accelerated methane production and stabilization via rapid organic oxidation and rapid methanogenesis. Over the total experimental period, the methane production rate and stabilization time of the AD+MEC reactor were approximately 1.7 and 4.0 times faster than those of the AD reactor. Interestingly however, at the final steady state, the methane yields of both the reactors were similar to the theoretical maximum methane yield. Based on these results, the MEC did not increase the methane yield over the theoretical value, but accelerated methane production and stabilization by bioelectrochemical reactions. Copyright © 2017 Elsevier Ltd. All rights reserved.

  12. Structure of praseodymium tris-dipivalyl-methanate adduct with triphenylphosphine oxide

    International Nuclear Information System (INIS)

    Aslanov, L.A.; Ionov, V.M.; Rybakov, V.B.; Korytnyj, E.F.; Martynenko, L.I.

    1978-01-01

    Crystal structure of Pr(DPM) 3 xTPPO, where DPM-dipivalylmethanate, TPPO,triphenylphosphine oxide is investigated X-ray method. Unit cell parameters are: a=11,551(2), b=22,201(5), c=21,786(6) A, j=104,92(2) deg, P2 1 /n, Z=4. The complexes are mononuclear, dipivalylmethanate ligands are chelates, triphenylphosphine oxide is bound with Pr atom by means of oxygen atom. Pr atom coordination polyhedron is a one-cap trigonal prism. Coordination number is 7

  13. Effect of nutrient and selective inhibitor amendments on methane oxidation, nitrous oxide production, and key gene presence and expression in landfill cover soils: characterization of the role of methanotrophs, nitrifiers, and denitrifiers.

    Science.gov (United States)

    Lee, Sung-Woo; Im, Jeongdae; Dispirito, Alan A; Bodrossy, Levente; Barcelona, Michael J; Semrau, Jeremy D

    2009-11-01

    Methane and nitrous oxide are both potent greenhouse gasses, with global warming potentials approximately 25 and 298 times that of carbon dioxide. A matrix of soil microcosms was constructed with landfill cover soils collected from the King Highway Landfill in Kalamazoo, Michigan and exposed to geochemical parameters known to affect methane consumption by methanotrophs while also examining their impact on biogenic nitrous oxide production. It was found that relatively dry soils (5% moisture content) along with 15 mg NH (4) (+) (kg soil)(-1) and 0.1 mg phenylacetylene(kg soil)(-1) provided the greatest stimulation of methane oxidation while minimizing nitrous oxide production. Microarray analyses of pmoA showed that the methanotrophic community structure was dominated by Type II organisms, but Type I genera were more evident with the addition of ammonia. When phenylacetylene was added in conjunction with ammonia, the methanotrophic community structure was more similar to that observed in the presence of no amendments. PCR analyses showed the presence of amoA from both ammonia-oxidizing bacteria and archaea, and that the presence of key genes associated with these cells was reduced with the addition of phenylacetylene. Messenger RNA analyses found transcripts of pmoA, but not of mmoX, nirK, norB, or amoA from either ammonia-oxidizing bacteria or archaea. Pure culture analyses showed that methanotrophs could produce significant amounts of nitrous oxide, particularly when expressing the particulate methane monooxygenase (pMMO). Collectively, these data suggest that methanotrophs expressing pMMO played a role in nitrous oxide production in these microcosms.

  14. Structural changes of noble metal catalysts during ignition and extinction of the partial oxidation of methane studied by advanced QEXAFS techniques

    DEFF Research Database (Denmark)

    Grunwaldt, Jan-Dierk; Beier, M.; Kimmerle, B.

    2009-01-01

    The dynamics of the ignition and extinction of the catalytic partial oxidation (CPO) of methane to hydrogen and carbon monoxide over Pt-Rh/Al2O3 and Pt/Al2O3 were studied in the subsecond timescale using quick-EXAFS with a novel cam-driven X-ray monochromator employing Si(111) and Si(311) crystals...... to discuss the potential and limitation of this technique in catalysis and related areas. With respect to the noble metal catalysed partial oxidation of methane, several interesting observations were made: structural changes during ignition were-independent of the chosen reaction conditions......-significantly faster than during the extinction of the reaction. The dynamic behavior of the catalysts was dependent on the flow conditions and the respective noble metal component(s). Higher reaction gas flow led to a faster ignition process. While the ignition over Pt-Rh/Al2O3 occurred at lower temperature than over...

  15. Visible-light-assisted SLCs template synthesis of sea anemone-like Pd/PANI nanocomposites with high electrocatalytic activity for methane oxidation in acidic medium

    Science.gov (United States)

    Tan, De-Xin; Wang, Yan-Li

    2018-03-01

    Sea anemone-like palladium (Pd)/polyaniline (PANI) nanocomposites were synthesized via visible-light-assisted swollen liquid crystals (SLCs) template method. The resulting samples were characterized by transmission electron microscopy (TEM), selected area electron diffraction (SAED), energy dispersive spectrometer (EDS), x-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), ultraviolet-visible (UV–vis) absorption spectroscopy and Fourier transform infrared (FT-IR) spectroscopy, respectively. The electrocatalytic properties of Pd/PANI nanocomposites modified glass carbon electrode (GCE) for methane oxidation were investigated by cycle voltammetry (CV) and chronoamperometry. Those dispersed sea anemone-like Pd/PANI nanocomposites had an average diameter of 320 nm. The obtained Pd nanoparticles with an average diameter of about 45 nm were uniformly distributed in PANI matrix. Sea anemone-like Pd/PANI nanocomposites exhibited excellent electrocatalytic activity and stability for oxidation of methane (CH4).

  16. Effect of Ca, Ce or K oxide addition on the activity of Ni/SiO{sub 2} catalysts for the methane decomposition reaction

    Energy Technology Data Exchange (ETDEWEB)

    Zapata, Beatriz; Torres-Garcia, Enelio [Instituto Mexicano del Petroleo, Programa de Procesos y Reactores, Eje C. 152, Mexico, D.F., C.P. 07730 (Mexico); Valenzuela, Miguel A.; Palacios, Jorge [Instituto Politecnico Nacional-ESIQIE, Lab. Catalisis y Materiales, Zacatenco, Mexico, D.F., C.P. 07738 (Mexico)

    2010-11-15

    To increase the activity and stability of Ni/SiO{sub 2} catalysts, a series of Ni-Ca, Ni-K and Ni-Ce promoted catalysts were prepared by successive impregnations. The textural properties, reducibility and catalytic performance in the methane decomposition reaction were investigated. The catalyst containing 30 wt.% Ni and 30 wt.% cerium oxide greatly increased the conversion of methane (90% of equilibrium value) and improved the stability, whereas the Ni-K and Ni-Ca were less active and stable than the Ni/SiO{sub 2} catalyst. The results suggest that Ce addition prevents the sintering of nickel particles during reduction process maintaining a random distribution between the silica and cerium oxide improving the distribution and migration of deposited carbon. (author)

  17. Ni modified ceramic anodes for direct-methane solid oxide fuel cells

    Science.gov (United States)

    Xiao, Guoliang; Chen, Fanglin

    2016-01-19

    In accordance with certain embodiments of the present disclosure, a method for fabricating a solid oxide fuel cell is described. The method includes synthesizing a composition having a perovskite present therein. The method further includes applying the composition on an electrolyte support to form an anode and applying Ni to the composition on the anode.

  18. Catalysis by Atomic-Sized Centers: Methane Activation for Partial Oxidation and Combustion

    Science.gov (United States)

    2015-07-21

    example, H adsorbed alone on an oxide surface will bind to oxygen to form a hydroxide . However, if a Lewis base (e.g. any electron donor) is...that on a gold surface, which is not surprising considering the bonding character between the cluster and metal surfaces. The high mobility verifies

  19. Co-existence of Anaerobic Ammonium Oxidation Bacteria and Denitrifying Anaerobic Methane Oxidation Bacteria in Sewage Sludge: Community Diversity and Seasonal Dynamics.

    Science.gov (United States)

    Xu, Sai; Lu, Wenjing; Mustafa, Muhammad Farooq; Caicedo, Luis Miguel; Guo, Hanwen; Fu, Xindi; Wang, Hongtao

    2017-11-01

    Anaerobic ammonium oxidation (ANAMMOX) and denitrifying anaerobic methane oxidation (DAMO) have been recently discovered as relevant processes in the carbon and nitrogen cycles of wastewater treatment plants. In this study, the seasonal dynamics of ANAMMOX and DAMO bacterial community structures and their abundance in sewage sludge collected from wastewater treatment plants were analysed. Results indicated that ANAMMOX and DAMO bacteria co-existed in sewage sludge in different seasons and their abundance was positively correlated (P bacteria in autumn and winter indicated that these seasons were the preferred time to favour the growth of ANAMMOX and DAMO bacteria. The community structure of ANNAMOX and DAMO bacteria could also shift with seasonal changes. The "Candidatus Brocadia" genus of ANAMMOX bacteria was mainly recovered in spring and summer, and an unknown cluster was primarily detected in autumn and winter. Similar patterns of seasonal variation in the community structure of DAMO bacteria were also observed. Group B was the dominant in spring and summer, whereas in autumn and winter, group A and group B presented almost the same proportion. The redundancy analysis revealed that pH and nitrate were the most significant factors affecting community structures of these two groups (P < 0.01). This study reported the diversity of ANAMMOX and DAMO in wastewater treatment plants that may be the basis for new nitrogen removal technologies.

  20. Characterization of Methane Degradation and Methane-Degrading Microbes in Alaska Coastal Water

    Energy Technology Data Exchange (ETDEWEB)

    Kirchman, David L. [Univ. of Delaware, Lewes, DE (United States)

    2012-03-29

    The net flux of methane from methane hydrates and other sources to the atmosphere depends on methane degradation as well as methane production and release from geological sources. The goal of this project was to examine methane-degrading archaea and organic carbon oxidizing bacteria in methane-rich and methane-poor sediments of the Beaufort Sea, Alaska. The Beaufort Sea system was sampled as part of a multi-disciplinary expedition (Methane in the Arctic Shelf or MIDAS) in September 2009. Microbial communities were examined by quantitative PCR analyses of 16S rRNA genes and key methane degradation genes (pmoA and mcrA involved in aerobic and anaerobic methane degradation, respectively), tag pyrosequencing of 16S rRNA genes to determine the taxonomic make up of microbes in these sediments, and sequencing of all microbial genes (metagenomes ). The taxonomic and functional make-up of the microbial communities varied with methane concentrations, with some data suggesting higher abundances of potential methane-oxidizing archaea in methane-rich sediments. Sequence analysis of PCR amplicons revealed that most of the mcrA genes were from the ANME-2 group of methane oxidizers. According to metagenomic data, genes involved in methane degradation and other degradation pathways changed with sediment depth along with sulfate and methane concentrations. Most importantly, sulfate reduction genes decreased with depth while the anaerobic methane degradation gene (mcrA) increased along with methane concentrations. The number of potential methane degradation genes (mcrA) was low and inconsistent with other data indicating the large impact of methane on these sediments. The data can be reconciled if a small number of potential methane-oxidizing archaea mediates a large flux of carbon in these sediments. Our study is the first to report metagenomic data from sediments dominated by ANME-2 archaea and is one of the few to examine the entire microbial assemblage potentially involved in

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

    Science.gov (United States)

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

    2014-12-01

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

  2. Axial Changes of Catalyst Structure and Temperature in a Fixed-Bed Microreactor During Noble Metal Catalysed Partial Oxidation of Methane

    DEFF Research Database (Denmark)

    Hannemann, S.; Grunwaldt, Jan-Dierk; Kimmerle, B.

    2009-01-01

    The catalytic partial oxidation of methane (CPO) over flame-made 2.5%Rh-2.5%Pt/Al2O3 and 2.5%Rh/Al2O3 in 6%CH4/3%O-2/He shows the potential of in situ studies using miniaturized fixed-bed reactors, the importance of spatially resolved studies and its combination with infrared thermography and on-...

  3. Enrichment of sulfate reducing anaerobic methane oxidizing community dominated by ANME-1 from Ginsburg Mud Volcano (Gulf of Cadiz) sediment in a biotrickling filter.

    Science.gov (United States)

    Bhattarai, Susma; Cassarini, Chiara; Rene, Eldon R; Zhang, Yu; Esposito, Giovanni; Lens, Piet N L

    2018-07-01

    This study was performed to enrich anaerobic methane-oxidizing archaea (ANME) present in sediment from the Ginsburg Mud Volcano (Gulf of Cadiz) in a polyurethane foam packed biotrickling filter (BTF). The BTF was operated at 20 (±2) °C, ambient pressure with continuous supply of methane for 248 days. Sulfate reduction with simultaneous sulfide production (accumulating ∼7 mM) after 200 days of BTF operation evidenced anaerobic oxidation of methane (AOM) coupled to sulfate reduction. High-throughput sequence analysis of 16S rRNA genes showed that after 248 days of BTF operation, the ANME clades enriched to more than 50% of the archaeal sequences, including ANME-1b (40.3%) and ANME-2 (10.0%). Enrichment of the AOM community was beneficial to Desulfobacteraceae, which increased from 0.2% to 1.8%. Both the inoculum and the BTF enrichment contained large populations of anaerobic sulfur oxidizing bacteria, suggesting extensive sulfur cycling in the BTF. Copyright © 2018 Elsevier Ltd. All rights reserved.

  4. Thermochemical Properties of the Lattice Oxygen in W,Mn-Containing Mixed Oxide Catalysts for the Oxidative Coupling of Methane

    Science.gov (United States)

    Lomonosov, V. I.; Gordienko, Yu. A.; Sinev, M. Yu.; Rogov, V. A.; Sadykov, V. A.

    2018-03-01

    Mixed NaWMn/SiO2 oxide, samples containing individual components (Na, W, Mn) and their double combinations (Na-W, Na-Mn, W-Mn) supported on silica were studied by temperature programmed reduction (TPR) and desorption (TPD), and heat flow calorimetry during their reoxidation with molecular oxygen in pulse mode. The NaWMn/SiO2 mixed oxide was shown to contain two different types of reactive lattice oxygen. The weakly-bonded oxygen can be reversibly released from the oxide in a flow of inert gas in the temperature range of 575‒900°C, while the strongly-bonded oxygen can be removed during the reduction of the sample with hydrogen at 700-900°C. The measured thermal effect of oxygen consumption for these two oxygen forms are 185 and 350 kJ/mol, respectively. The amount of oxygen removed at reduction ( 443 μmol/g) considerably exceeded the amount desorbed in an inert gas flow ( 56 μmol/g). The obtained results suggest that the reversible oxygen desorption is due to the redox process in which manganese ions are involved, while during the temperature programmed reduction, mainly oxygen bonded with tungsten is removed.

  5. Carbon dioxide, methane and nitrous oxide fluxes from a fire chronosequence in subarctic boreal forests of Canada.

    Science.gov (United States)

    Köster, Egle; Köster, Kajar; Berninger, Frank; Aaltonen, Heidi; Zhou, Xuan; Pumpanen, Jukka

    2017-12-01

    Forest fires are one of the most important natural disturbances in boreal forests, and their occurrence and severity are expected to increase as a result of climate warming. A combination of factors induced by fire leads to a thawing of the near-surface permafrost layer in subarctic boreal forest. Earlier studies reported that an increase in the active layer thickness results in higher carbon dioxide (CO 2 ) and methane (CH 4 ) emissions. We studied changes in CO 2 , CH 4 and nitrous oxide (N 2 O) fluxes in this study, and the significance of several environmental factors that influence the greenhouse gas (GHG) fluxes at three forest sites that last had fires in 2012, 1990 and 1969, and we compared these to a control area that had no fire for at least 100years. The soils in our study acted as sources of CO 2 and N 2 O and sinks for CH 4 . The elapsed time since the last forest fire was the only factor that significantly influenced all studied GHG fluxes. Soil temperature affected the uptake of CH 4 , and the N 2 O fluxes were significantly influenced by nitrogen and carbon content of the soil, and by the active layer depth. Results of our study confirm that the impacts of a forest fire on GHGs last for a rather long period of time in boreal forests, and are influenced by the fire induced changes in the ecosystem. Copyright © 2017 Elsevier B.V. All rights reserved.

  6. Effects of ferric iron reduction and regeneration on nitrous oxide and methane emissions in a rice soil.

    Science.gov (United States)

    Huang, Bin; Yu, Kewei; Gambrell, Robert P

    2009-01-01

    A laboratory soil slurry experiment and an outdoor pot experiment were conducted to study effects of ferric iron (Fe(III)) reduction and regeneration on nitrous oxide (N(2)O) and methane (CH(4)) emissions in a rice (Oryza sativa L.) soil. The anoxic slurry experiment showed that enhancing microbial Fe(III) reduction by ferrihydrite amendment (40 mol Fe g(-1)) transitionally stimulated N(2)O production and lowered CH(4) production by 16% during an initial 33-day incubation. Increased regeneration of Fe(III) through a 4-day aeration period in the Fe-amended slurry compared to the control slurry reduced CH(4) emission by 30% in the subsequent 15-day anaerobic incubation. The pot experiment showed that ferrihydrite amendment (63 micromol Fe g(-1)) stimulated N(2)O fluxes in the days following flooding. The Fe amendment suppression on CH(4) emission was obscured in the early season but became significant upon reflooding in the mid- and late-seasons. As a result, seasonal CH(4) emission in Fe-amended pots was 26% lower than the control with a single 2-day drainage and 69% lower with a double 2-day drainage. The reduction in CH(4) emission upon reflooding from the Fe-amended pots was mainly attributed to the increased Fe(III) regeneration during drainage showing a mechanism of Fe(III) regeneration in mitigating CH(4) emission by short-term drainage in flooded soils.

  7. Tillage and Fertilizer Management Effects on Soil-Atmospheric Exchanges of Methane and Nitrous Oxide in a Corn Production System

    Directory of Open Access Journals (Sweden)

    Ermson Z. Nyakatawa

    2011-01-01

    Full Text Available Land application of poultry litter (PL presents an opportunity to improve soil productivity and disposal of poultry waste. We investigated methane (CH4 and nitrous oxide (N2O emissions from agricultural soil receiving PL and ammonium nitrate (AN fertilizers using surface (SA, soil incorporation (SI, and subsurface band (BA application methods in conventional (CT and no-tillage (NT systems on a Decatur silt loam soil in North Alabama. Plots under CT and NT were sinks of CH4 in spring, summer, and fall. In winter, the plots had net emissions of 3.32 and 4.24 g CH4 ha-1 day-1 in CT and NT systems, respectively. Plots which received AN were net emitters of CH4 and N2O, whereas plots which received PL were net sinks of CH4. Plots which received PL using SA or SI methods were net emitters of N2O, whereas under PL using BA application, the plots were net sinks of N2O. Our study indicates that using subsurface band application of PL was the most promising environmentally sustainable poultry waste application method for reducing CH4 and N2O emissions from agricultural soil in NT and CT corn production systems on the Decatur soil in north Alabama.

  8. Vertical and horizontal distribution of sediment nitrite-dependent methane-oxidizing organisms in a mesotrophic freshwater reservoir.

    Science.gov (United States)

    Long, Yan; Liu, Changbao; Lin, Hengliang; Li, Ningning; Guo, Qingwei; Xie, Shuguang

    2017-06-01

    In the present study, we investigated the spatial change of sediment nitrite-dependent anaerobic methane-oxidizing (n-damo) organisms in the mesotrophic freshwater Gaozhou Reservoir (6 different sampling locations and 2 sediment depths (0-5 cm, 5-10 cm)), one of the largest drinking water reservoirs in China. The abundance of sediment n-damo bacteria was quantified using quantitative polymerase chain reaction assay, while the richness, diversity, and composition of n-damo pmoA gene sequences were characterized using clone library analysis. Vertical and horizontal changes in sediment n-damo bacterial abundance occurred in Gaozhou Reservoir, with 1.37 × 10 5 to 8.24 × 10 5 n-damo 16S rRNA gene copies per gram of dry sediment. Considerable horizontal and vertical variations of n-damo pmoA gene diversity (Shannon index = 0.32-2.50) and composition also occurred in this reservoir. Various types of sediment n-damo pmoA genes existed in Gaozhou Reservoir. A small proportion of n-damo pmoA gene sequences (19.1%) were related to those recovered from "Candidatus Methylomirabilis oxyfera". Our results suggested that sediment n-damo pmoA gene diversity might be regulated by nitrite, while n-damo pmoA gene richness might be governed by multiple environmental factors, including total organic carbon, total phosphorus, nitrite, and total nitrogen.

  9. International IPCC workshop on methane and nitrous oxide: methods in national emissions inventories and options for control

    Energy Technology Data Exchange (ETDEWEB)

    Amstel, A.R. van (ed.)

    1993-07-01

    This workshop had two main objectives: to support the development of an internationally agreed methodology and reporting format for national emission inventories of greenhouse gases by mid 1993, as coordinated by the Science Working Group of the Intergovernmental Panel on Climate Change (IPCC) and the Organization for Economic Cooperation and Development (OECD); and the development of technical options for reduction of these greenhouse gases and the assessment of the socio-economic feasibility of these options. These proceedings contain the overview papers presented at the workshop, the background papers prepared for the working group sessions and the conclusions and recommendations of the working groups put forward during these sessions. 16 poster summaries are also included. During the workshop, 8 different sources of methane were discussed - oil and gas, coal mining, ruminants, animal waste, landfills and sewage treatments, combustion and industry, rice production and wetlands, and biomass burning - and 2 sources of nitrous oxide - agricultural soils and combustion and industry. All papers have been abstracted separately.

  10. Mitigating global warming potentials of methane and nitrous oxide gases from rice paddies under different irrigation regimes.

    Science.gov (United States)

    Ali, Muhammad Aslam; Hoque, M Anamul; Kim, Pil Joo

    2013-04-01

    A field experiment was conducted in Bangladesh Agricultural University Farm to investigate the mitigating effects of soil amendments such as calcium carbide, calcium silicate, phosphogypsum, and biochar with urea fertilizer on global warming potentials (GWPs) of methane (CH4) and nitrous oxide (N2O) gases during rice cultivation under continuous and intermittent irrigations. Among the amendments phosphogypsum and silicate fertilizer, being potential source of electron acceptors, decreased maximum level of seasonal CH4 flux by 25-27 % and 32-38 % in continuous and intermittent irrigations, respectively. Biochar and calcium carbide amendments, acting as nitrification inhibitors, decreased N2O emissions by 36-40 % and 26-30 % under continuous and intermittent irrigations, respectively. The total GWP of CH4 and N2O gases were decreased by 7-27 % and 6-34 % with calcium carbide, phosphogypsum, and silicate fertilizer amendments under continuous and intermittent irrigations, respectively. However, biochar amendments increased overall GWP of CH4 and N2O gases.

  11. Current advances in molecular methods for detection of nitrite-dependent anaerobic methane oxidizing bacteria in natural environments.

    Science.gov (United States)

    Chen, Jing; Dick, Richard; Lin, Jih-Gaw; Gu, Ji-Dong

    2016-12-01

    Nitrite-dependent anaerobic methane oxidation (n-damo) process uniquely links microbial nitrogen and carbon cycles. Research on n-damo bacteria progresses quickly with experimental evidences through enrichment cultures. Polymerase chain reaction (PCR)-based methods for detecting them in various natural ecosystems and engineered systems play a very important role in the discovery of their distribution, abundance, and biodiversity in the ecosystems. Important characteristics of n-damo enrichments were obtained and their key significance in microbial nitrogen and carbon cycles was investigated. The molecular methods currently used in detecting n-damo bacteria were comprehensively reviewed and discussed for their strengths and limitations in applications with a wide range of samples. The pmoA gene-based PCR primers for n-damo bacterial detection were evaluated and, in particular, several incorrectly stated PCR primer nucleotide sequences in the published papers were also pointed out to allow correct applications of the PCR primers in current and future investigations. Furthermore, this review also offers the future perspectives of n-damo bacteria based on current information and methods available for a better acquisition of new knowledge about this group of bacteria.

  12. Environmental evaluation of coexistence of denitrifying anaerobic methane-oxidizing archaea and bacteria in a paddy field.

    Science.gov (United States)

    Ding, Jing; Fu, Liang; Ding, Zhao-Wei; Lu, Yong-Ze; Cheng, Shuk H; Zeng, Raymond J

    2016-01-01

    The nitrate-dependent denitrifying anaerobic methane oxidation (DAMO) process, which is metabolized together by anaerobic methanotrophic archaea and NC10 phylum bacteria, is expected to be important for the global carbon and nitrogen cycles. However, there are little studies about the existence of this process and the functional microbes in environments. Therefore, the coexistence of DAMO archaea and bacteria in a paddy field was evaluated in this study. Next-generation sequencing showed that the two orders, Methanosarcinales and Nitrospirales, to which DAMO archaea and DAMO bacteria belong, were detected in the four soil samples. Then the in vitro experiments demonstrated both of nitrite- and nitrate-dependent DAMO activities, which confirmed the coexistence of DAMO archaea and DAMO bacteria. It was the first report about the coexistence of DAMO archaea and bacteria in a paddy field. Furthermore, anammox bacteria were detected in two of the four samples. The in vitro experiments did not show anammox activity in the initial period but showed low anammox activity after 20 days' enrichment. These results implicated that anammox bacteria may coexist with DAMO microorganisms in this field, but at a very low percentage.

  13. Supercritical water oxidation data acquisition testing. Final report, Volume II

    International Nuclear Information System (INIS)

    1996-11-01

    Supercritical Water Oxidation (SCWO) technology holds great promise for treating mixed wastes, in an environmentally safe and efficient manner. In the spring of 1994 the US Department of Energy (DOE), Idaho Operations Office awarded Stone ampersand Webster Engineering Corporation, of Boston Massachusetts and its sub-contractor MODAR, Inc. of Natick Massachusetts a Supercritical Water Oxidation Data Acquisition Testing (SCWODAT) program. The SCWODAT program was contracted through a Cooperative Agreement that was co-funded by the US Department of Energy and the Strategic Environmental Research and Development Program. The SCWODAT testing scope outlined by the DOE in the original Cooperative Agreement and amendments thereto was initiated in June 1994 and successfully completed in December 1995. The SCWODAT program provided further information and operational data on the effectiveness of treating both simulated mixed waste and typical Navy hazardous waste using the MODAR SCWO technology

  14. Experimental and Modeling Investigation of the Effectof H2S Addition to Methane on the Ignition and Oxidation at High Pressures

    DEFF Research Database (Denmark)

    Gersen, Sander; van Essen, Martijn; Darmeveil, Harry

    2017-01-01

    The autoignition and oxidation behavior of CH4/H2S mixtures has been studied experimentally in a rapid compression machine (RCM) and a high-pressure flow reactor. The RCM measurements show that the addition of 1% H2S to methane reduces the autoignition delay time by a factor of 2 at pressures....... A comparison of the flow reactordata to modeling predictions shows satisfactory agreement under stoichiometric conditions, while at very reducing conditions, the model underestimates the consumption of both H2S and CH4. Similar to the RCM experiments, the presence of H2S is predicted to promote oxidation...

  15. Evidence of syntrophic acetate oxidation by Spirochaetes during anaerobic methane production.

    Science.gov (United States)

    Lee, Sang-Hoon; Park, Jeong-Hoon; Kim, Sang-Hyoun; Yu, Byung Jo; Yoon, Jeong-Jun; Park, Hee-Deung

    2015-08-01

    To search for evidence of syntrophic acetate oxidation by cluster II Spirochaetes with hydrogenotrophic methanogens, batch reactors seeded with five different anaerobic sludge samples supplemented with acetate as the sole carbon source were operated anaerobically. The changes in abundance of the cluster II Spirochaetes, two groups of acetoclastic methanogens (Methanosaetaceae and Methanosarcinaceae), and two groups of hydrogenotrophic methanogens (Methanomicrobiales and Methanobacteriales) in the reactors were assessed using qPCR targeting the 16S rRNA genes of each group. Increase in the cluster II Spirochaetes (9.0±0.4-fold) was positively correlated with increase in hydrogenotrophic methanogens, especially Methanomicrobiales (5.6±1.0-fold), but not with acetoclastic methanogens. In addition, the activity of the cluster II Spirochaetes decreased (4.6±0.1-fold) in response to high hydrogen partial pressure, but their activity was restored after consumption of hydrogen by the hydrogenotrophic methanogens. These results strongly suggest that the cluster II Spirochaetes are involved in syntrophic acetate oxidation in anaerobic digesters. Copyright © 2015 Elsevier Ltd. All rights reserved.

  16. Profitability expertise of rural methanization projects; Expertise de la rentabilite des projets de methanisation rurale. Rapport final

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    2010-02-15

    The main objectives of this study were to analyze the profitability of projects of methanization, and to identify factors which curb or favour their profitability. It is based on a detailed analysis of the investment and of the profitability of 50 sites of different sizes and at different stages of progress (from the feasibility study to few months of operation), and also of experiences in three neighbour countries (Germany, Switzerland and Belgium). First, the study highlights the importance of investment costs in the biogas production global cost, notably with respect to current German prices. Then, it comments the impact of subsidies on facility profitability. It proposes ways to improve public support to the different energetic vectors produced from biogas: electricity, biomethane, and heat

  17. A robust NiO-Sm0.2Ce0.8O1.9 anode for direct-methane solid oxide fuel cell

    KAUST Repository

    Tian, Dong

    2015-07-02

    In order to directly use methane without a reforming process, NiO-Sm0.2Ce0.8O1.9 (NiO-SDC) nanocomposite anode are successfully synthesized via a one-pot, surfactant-assisted co-assembly approach for direct-methane solid oxide fuel cells. Both NiO with cubic phase and SDC with fluorite phase are obtained at 550 °C. Both NiO nanoparticles and SDC nanoparticles are highly monodispersed in size with nearly spherical shapes. Based on the as-synthesized NiO-SDC, two kinds of single cells with different micro/macro-porous structure are successfully fabricated. As a result, the cell performance was improved by 40%-45% with the new double-pore NiO-SDC anode relative to the cell performance with the conventional NiO-SDC anode due to a wider triple-phase-boundary (TPB) area. In addition, no significant degradation of the cell performance was observed after 60 hours, which means an increasing of long term stability. Therefore, the as-synthesized NiO-SDC nanocomposite is a promising anode for direct-methane solid oxide fuel cells.

  18. Integrated Science Assessment (ISA) for Sulfur Oxides – Health Criteria (Final Report, Sep 2008)

    Science.gov (United States)

    EPA announced the availability of the final report, Integrated Science Assessment (ISA) for Sulfur Oxides – Health Criteria final assessment. This report represents a concise synthesis and evaluation of the most policy-relevant science and will ultimately provide the scien...

  19. Electronic Effects on Room-Temperature, Gas-Phase C-H Bond Activations by Cluster Oxides and Metal Carbides: The Methane Challenge.

    Science.gov (United States)

    Schwarz, Helmut; Shaik, Sason; Li, Jilai

    2017-12-06

    This Perspective discusses a story of one molecule (methane), a few metal-oxide cationic clusters (MOCCs), dopants, metal-carbide cations, oriented-electric fields (OEFs), and a dizzying mechanistic landscape of methane activation! One mechanism is hydrogen atom transfer (HAT), which occurs whenever the MOCC possesses a localized oxyl radical (M-O • ). Whenever the radical is delocalized, e.g., in [MgO] n •+ the HAT barrier increases due to the penalty of radical localization. Adding a dopant (Ga 2 O 3 ) to [MgO] 2 •+ localizes the radical and HAT transpires. Whenever the radical is located on the metal centers as in [Al 2 O 2 ] •+ the mechanism crosses over to proton-coupled electron transfer (PCET), wherein the positive Al center acts as a Lewis acid that coordinates the methane molecule, while one of the bridging oxygen atoms abstracts a proton, and the negatively charged CH 3 moiety relocates to the metal fragment. We provide a diagnostic plot of barriers vs reactants' distortion energies, which allows the chemist to distinguish HAT from PCET. Thus, doping of [MgO] 2 •+ by Al 2 O 3 enables HAT and PCET to compete. Similarly, [ZnO] •+ activates methane by PCET generating many products. Adding a CH 3 CN ligand to form [(CH 3 CN)ZnO] •+ leads to a single HAT product. The CH 3 CN dipole acts as an OEF that switches off PCET. [MC] + cations (M = Au, Cu) act by different mechanisms, dictated by the M + -C bond covalence. For example, Cu + , which bonds the carbon atom mostly electrostatically, performs coupling of C to methane to yield ethylene, in a single almost barrier-free step, with an unprecedented atomic choreography catalyzed by the OEF of Cu + .

  20. Anaerobic oxidation of methane (AOM) in marine sediments from the Skagerrak (Denmark): I. Geochemical and microbiological analyses

    DEFF Research Database (Denmark)

    Knab, Nina J.; Cragg, Barry A.; Borowski, Christian

    2008-01-01

    as a methane barrier for this upward diffusing methane. To investigate the regulation of AOM and sulfate reduction rates (SRR) and the controls on the efficiency of methane consumption, pore water concentrations, and microbial rates of AOM, sulfate reduction and methanogenesis were determined in three gravity...... cores collected along the slope of the Norwegian Trench in the Skagerrak. SRR occurred in two distinct peaks, at the sediment surface and the SMTZ, the latter often exceeding the peak AOM rates that occurred at the bottom of the SMTZ. Highest rates of both AOM and SRR were observed in a core from...

  1. Effect of land use change on methane oxidation in temperate forest and grassland soils

    Energy Technology Data Exchange (ETDEWEB)

    Ojima, D.S.; Valentine, D.W.; Mosier, A.R.; Parton, W.J.; Schimel, D.S. (Colorado State University, Fort Collins, CO (USA). Natural Resources Ecology Lab.)

    Evidence is accumulating that land use changes and other human activity during the past 100 to 200 years have contributed to decreased CH[sub 4] oxidation in the soil. Increased N additions to temperate forest soils in the northeastern United States decreased CH[sub 4] uptake by 30 to 60%, and increased N fertilization and conversion to cropland in temperate grasslands decreased CH[sub 4] uptake by 30 to 75%. Using these data, a series of calculations were made to estimate the impact of land use and management changes which have altered soil, the CH[sub 4] sink in temperate forest and grassland ecosystems. As the atmospheric mixing ratio of CH[sub 4] has increased during the past 150 y, the temperate CH[sub 4] sink has risen from approximately 8 Tg y[sup -1] to 27 Tg y[sup -1], assuming no loss of land cover to cropland conversion. The net effect of intensive land cover changes and extensive chronic disturbance (i.e., increased atmospheric N deposition) to these ecosystems have resulted in about 30% reduction in the CH[sub 4] budget even more as atmospheric CH[sub 4] concentrations increase and as a result of further disturbance to other biomes. Without accounting for this approximately 20 Tg y[sup -1] temperate soil sink, the atmospheric CH[sub 4] concentration would be increasing about 1.5 times the current rate. 39 refs., 2 figs., 1 tab.

  2. Methane and Nitrous Oxide Emissions Reduced Following Conversion of Rice Paddies to Inland Crab-Fish Aquaculture in Southeast China.

    Science.gov (United States)

    Liu, Shuwei; Hu, Zhiqiang; Wu, Shuang; Li, Shuqing; Li, Zhaofu; Zou, Jianwen

    2016-01-19

    Aquaculture is an important source of atmospheric methane (CH4) and nitrous oxide (N2O), while few direct flux measurements are available for their regional and global source strength estimates. A parallel field experiment was performed to measure annual CH4 and N2O fluxes from rice paddies and rice paddy-converted inland crab-fish aquaculture wetlands in southeast China. Besides N2O fluxes dependent on water/sediment mineral N and CH4 fluxes related to water chemical oxygen demand, both CH4 and N2O fluxes from aquaculture were related to water/sediment temperature, sediment dissolved organic carbon, and water dissolved oxygen concentration. Annual CH4 and N2O fluxes from inland aquaculture averaged 0.37 mg m(-2) h(-1) and 48.1 μg m(-2) h(-1), yielding 32.57 kg ha(-1) and 2.69 kg N2O-N ha(-1), respectively. The conversion of rice paddies to aquaculture significantly reduced CH4 and N2O emissions by 48% and 56%, respectively. The emission factor for N2O was estimated to be 0.66% of total N input in the feed or 1.64 g N2O-N kg(-1) aquaculture production in aquaculture. The conversion of rice paddies to inland aquaculture would benefit for reconciling greenhouse gas mitigation and agricultural income increase as far as global warming potentials and net ecosystem economic profits are of concomitant concern. Some agricultural practices such as better aeration and feeding, and fallow season dredging would help to lower CH4 and N2O emissions from inland aquaculture. More field measurements from inland aquaculture are highly needed to gain an insight into national and global accounting of CH4 and N2O emissions.

  3. Annual methane and nitrous oxide emissions from rice paddies and inland fish aquaculture wetlands in southeast China

    Science.gov (United States)

    Wu, Shuang; Hu, Zhiqiang; Hu, Tao; Chen, Jie; Yu, Kai; Zou, Jianwen; Liu, Shuwei

    2018-02-01

    Inland aquaculture ponds have been documented as important sources of atmospheric methane (CH4) and nitrous oxide (N2O), while their regional or global source strength remains unclear due to lack of direct flux measurements by covering more typical habitat-specific aquaculture environments. In this study, we compared the CH4 and N2O fluxes from rice paddies and nearby inland fish aquaculture wetlands that were converted from rice paddies in southeast China. Both CH4 and N2O fluxes were positively related to water temperature and sediment dissolved organic carbon, but negatively related to water dissolved oxygen concentration. More robust response of N2O fluxes to water mineral N was observed than to sediment mineral N. Annual CH4 and N2O fluxes from inland fish aquaculture averaged 0.51 mg m-2 h-1 and 54.78 μg m-2 h-1, amounting to 42.31 kg CH4 ha-1 and 2.99 kg N2O-N ha-1, respectively. The conversion of rice paddies to conventional fish aquaculture significantly reduced CH4 and N2O emissions by 23% and 66%, respectively. The emission factor for N2O was estimated to be 0.46% of total N input in the feed or 1.23 g N2O-N kg-1 aquaculture production. The estimate of sustained-flux global warming potential of annual CH4 and N2O emissions and the net economic profit suggested that such conversion of rice paddies to inland fish aquaculture would help to reconcile the dilemma for simultaneously achieving both low climatic impacts and high economic benefits in China. More solid direct field measurements from inland aquaculture are in urgent need to direct the overall budget of national or global CH4 and N2O fluxes.

  4. Warming of subarctic tundra increases emissions of all three important greenhouse gases - carbon dioxide, methane, and nitrous oxide.

    Science.gov (United States)

    Voigt, Carolina; Lamprecht, Richard E; Marushchak, Maija E; Lind, Saara E; Novakovskiy, Alexander; Aurela, Mika; Martikainen, Pertti J; Biasi, Christina

    2017-08-01

    Rapidly rising temperatures in the Arctic might cause a greater release of greenhouse gases (GHGs) to the atmosphere. To study the effect of warming on GHG dynamics, we deployed open-top chambers in a subarctic tundra site in Northeast European Russia. We determined carbon dioxide (CO 2 ), methane (CH 4 ), and nitrous oxide (N 2 O) fluxes as well as the concentration of those gases, inorganic nitrogen (N) and dissolved organic carbon (DOC) along the soil profile. Studied tundra surfaces ranged from mineral to organic soils and from vegetated to unvegetated areas. As a result of air warming, the seasonal GHG budget of the vegetated tundra surfaces shifted from a GHG sink of -300 to -198 g CO 2 -eq m -2 to a source of 105 to 144 g CO 2 -eq m -2 . At bare peat surfaces, we observed increased release of all three GHGs. While the positive warming response was dominated by CO 2 , we provide here the first in situ evidence of increasing N 2 O emissions from tundra soils with warming. Warming promoted N 2 O release not only from bare peat, previously identified as a strong N 2 O source, but also from the abundant, vegetated peat surfaces that do not emit N 2 O under present climate. At these surfaces, elevated temperatures had an adverse effect on plant growth, resulting in lower plant N uptake and, consequently, better N availability for soil microbes. Although the warming was limited to the soil surface and did not alter thaw depth, it increased concentrations of DOC, CO 2, and CH 4 in the soil down to the permafrost table. This can be attributed to downward DOC leaching, fueling microbial activity at depth. Taken together, our results emphasize the tight linkages between plant and soil processes, and different soil layers, which need to be taken into account when predicting the climate change feedback of the Arctic. © 2016 John Wiley & Sons Ltd.

  5. Nitrous oxide, carbon dioxide and methane emissions from irrigated cropping systems as influenced by legumes, manure and fertilizer

    Energy Technology Data Exchange (ETDEWEB)

    Ellert, B.H.; Janzen, H.H. [Agriculture and Agri-Food Canada, Lethbridge, AB (Canada)

    2008-04-15

    Irrigated crops in Alberta require higher inputs of nitrogen (N) than rainfed crops. The aim of the study was to determine emissions of nitrous oxide (N{sub 2}O) from the soils of irrigated cropping systems that used inorganic fertilizer N at a site in Alberta. The study measured carbon dioxide (CO{sub 2}) and methane (CH{sub 4}) levels in order to determine net greenhouse gas (GHG) emissions. The exchange of gases between the atmosphere and soil in selected treatments was measured in order to compare the effects of contrasting N inputs. Fluxes were measured bi-weekly from spring 2001 to spring 2004. The time period included annual and perennial legume crops; the termination of a perennial forage crop; manure application; and 2 growing seasons of test crops. Soil surface fluxes were measured using PVC chambers equipped with thermocouples. Gas samples were measured using gas chromatography. A linear least squares method was used to calculate gas concentrations. Results showed that soil CO{sub 2} and N{sub 2}O production rates were intertwined after legume production or manure application, but decoupled during early spring bursts of N{sub 2}O production. Higher soil CO{sub 2} emissions with alfalfa and manure-amended soils suggested that soil oxygen consumption during high CO{sub 2} emission periods may promote N{sub 2}O emissions. Appreciable proportions of N{sub 2}O were emitted outside the growing season. Results suggested that N{sub 2}O leakage is an inevitable hazard of crop production. The study highlighted the importance of understanding and quantifying N{sub 2}O emissions from intensive cropping systems. 22 refs., 4 tabs., 6 figs.

  6. Temperate mangrove and salt marsh sediments are a small methane and nitrous oxide source but important carbon store

    Science.gov (United States)

    Livesley, Stephen J.; Andrusiak, Sascha M.

    2012-01-01

    Tidal saline wetlands (TSW), such as mangrove and salt marsh systems, provide many valuable ecosystem services, but continue to suffer disturbance, degradation and deforestation. Tropical mangroves perform a critical role in the exchange and storage of terrestrial-marine carbon but can function as a source of methane (CH 4) and nitrous oxide (N 2O). However, little is known of biogeochemical processes in temperate mangrove and salt marsh systems in the southern hemisphere. In this study, the soil/sediment exchange of CO 2, CH 4 and N 2O was measured seasonally along a natural transition from melaleuca woodland, salt marsh and into mangroves along the Mornington Peninsula edge of Westernport Bay, Victoria, Australia. Soil/sediment physiochemical properties and sediment C density were measured concurrently. The melaleuca woodland soil was a constant CH 4 sink of approximately -25 μg C m -2 h -1 but along the transect this rapidly switched to a weak CH 4 source (mangrove sediments where emissions of up to 375 μg C m -2 h -1 were measured in summer. Sediment CH 4 exchange correlated with salinity, pneumatophore number and the redox potential of sediment water at depth. All three ecosystems were a small N 2O source of ecosystem and season along with soil temperature and salinity. Sediment C density was significantly greater in the salt marsh than the mangrove. Salt marsh sediment C density was 168 Mg C ha -1 which is comparable with that measured globally, whereas the mangrove sediment C density of 145 Mg C ha -1 is among the lowest reported. Contrary to global patterns in terrestrial soil C content and salt marsh sediment C content, data from our study indicate that mangrove sediments from a cooler, drier temperate latitude may store less C than mangroves in warmer and wetter tropical latitudes. Understanding both C storage and the greenhouse gas balance of TSWs will help us to better value these vulnerable ecosystems and manage them accordingly.

  7. Final report on the oxidation of energetic materials in supercritical water. Final Air Force report

    Energy Technology Data Exchange (ETDEWEB)

    Buelow, S.J.; Allen, D.; Anderson, G.K. [and others

    1995-04-03

    The objective of this project was to determine the suitability of oxidation in supercritical fluids (SCO), particularly water (SCWO), for disposal of propellants, explosives, and pyrotechnics (PEPs). The SCO studies of PEPs addressed the following issues: The efficiency of destruction of the substrate. The products of destruction contained in the effluents. Whether the process can be conducted safely on a large scale. Whether energy recovery from the process is economically practicable. The information essential for process development and equipment design was also investigated, including issues such as practical throughput of explosives through a SCWO reactor, reactor materials and corrosion, and models for process design and optimization.

  8. Controls on gross fluxes of nitrous oxide and methane from an active agricultural ecosystem

    Science.gov (United States)

    Yang, W. H.; Silver, W. L.

    2013-12-01

    Agricultural soils can be a significant source of greenhouse gas emissions. Most research on the dynamics of these gases measure net fluxes across the soil-atmosphere interface. This approach limits our ability to determine driving variables because production and consumption processes occur simultaneously, and may be controlled by different factors. We used the trace gas stable isotope pool dilution technique to simultaneously measure field rates of gross production and consumption of N2O and CH4 during the growing season in a corn field located in the Sacramento-San Joaquin Delta, California. We also measured net nitrogen (N) mineralization and nitrification rates, soil temperature, soil moisture, and soil carbon dioxide (CO2) emissions to explore their role as drivers of greenhouse gas fluxes. Across five sampling dates spanning from seeding to senescence, net N2O fluxes ranged from 0 - 4.5 mg N m-2 d-1 and averaged 1.6 × 0.2 mg N m-2 d-1 (n = 112). Gross N2O production ranged from 0.09 - 6.6 mg N m-2 d-1 and gross N2O reduction rates ranged from 0.00 - 0.95 mg N m-2 d-1. The N2O yield averaged 0.68 × 0.02 (n = 40). At peak growth (days after seeding 59 and 94), 89 % of the variability in gross N2O production rates was predicted by the combination of soil moisture, soil temperature, net N mineralization, and CO2 emissions (n = 15, p seeding 11, 24, and 171), gross N2O production was most strongly correlated with soil temperature (R2 = 0.20, n = 24, p = 0.03), and gross N2O reduction rates were best predicted by CO2 emissions (R2 = 0.80, n =24, p production in 36 out of 37 measurements. Gross CH4 production reached as high as 5.4 mg C m-2 d-1 with rates trending higher throughout the growing season. Gross CH4 production rates were marginally significantly higher in rows than in inter-rows (p = 0.10). Gross CH4 oxidation did not differ significantly among sampling dates (Figure 2b), averaging 1.1 × 0.2 mg C m-2 d-1 across all measurements (n = 37). However

  9. Mitigation of methane emissions in a pilot-scale biocover system at the AV Miljø Landfill, Denmark: 2. Methane oxidation

    DEFF Research Database (Denmark)

    Scheutz, Charlotte; Cassini, Filippo; De Schoenmaeker, Jan

    2017-01-01

    resulting in overloaded areas causing CH4 emission hot spot areas in the biocover surface. The whole biocover CH4 oxidation efficiency was determined by measuring the CH4 inlet load and CH4 surface fluxes. In addition, CH4 oxidation was determined for single points in the biocover using two different...... oxidation rates -0.06 and 40gm2d-1. The study also revealed that the compost respiration contributed significantly to the measured CO2 surface emission, and that the contribution of the compost respiration decreased significantly with time probably due to further maturation of the compost material....

  10. Phytoremediation of Atmospheric Methane

    Science.gov (United States)

    2013-04-15

    REPORT Phytoremediation of Atmospheric Methane 14. ABSTRACT 16. SECURITY CLASSIFICATION OF: We have transformed a plant, Arabidopsis thaliana, with the...298 (Rev 8/98) Prescribed by ANSI Std. Z39.18 - 31-Mar-2012 Phytoremediation of Atmospheric Methane Report Title ABSTRACT We have transformed a...DD882) Scientific Progress See attachment Technology Transfer 1    Final Report for DARPA project W911NF1010027  Phytoremediation  of Atmospheric

  11. European strategies benchmark of biogas production and valorization industries and French methanation industry forward-looking statements. Final report

    International Nuclear Information System (INIS)

    Bastide, Guillaume; Thual, Julien; Theobald, Olivier; Bardinal, Marc; Johansson, Hannele; Piccinini, Sergio; Maggioni, Lorenzo; Al Seadi, Teodorita; Holm-Nielsen, Jens Bo; Da Costa Gomez, Claudius; Fricke, Klaus; Collins, David; Dumont, Mathieu; Onno, Jean-Marc; Guerin, Bertrand; Ollivier, Denis; Pessiot, Carine; Charlot, Marie-Laure; Molinie, Lea; Vizy, Pascale; Krembel, David; Lamy, Jean-Michel; Ingremeau, Claire; Lukehurst, Clare

    2015-06-01

    In France, the biogas sector is developing. Currently two incentive programs for this sector have been set up: the Energy Methane Nitrogen Autonomy (EMAA) Plan and the call for projects '1500 biogas plants'. The information gathering about measures applied in the historical countries and in countries whose development is supported nowadays, is necessary for decision making and the development of national support strategy. The first part of this report presents the European state of development of biogas plants (28 countries of the European Union and Switzerland) and lists the actions implemented by each country. It details the situation in five countries: Germany, Italy, the Netherlands, the United Kingdom, and Sweden. The second part presents 20 detailed measures selected among the 30 measures identified during the benchmark phase. The three scenarios for the French sector until 2030 are composed of a socio-economic context, a package of measures, and a quantified simulation by category and by type of biogas recovery. (authors)

  12. Methane, nitrous oxide and ammonia emissions from pigs housed on litter and from stockpiling of spent litter

    KAUST Repository

    Phillips, F. A.; Wiedemann, S. G.; Naylor, T. A.; McGahan, E. J.; Warren, B. R.; Murphy, C. M.; Parkes, Stephen; Wilson, J.

    2016-01-01

    Mitigation of agricultural greenhouse gas emissions is a target area for the Australian Government and the pork industry. The present study measured methane (CH4), nitrous oxide (N2O) and ammonia (NH3) from a deep-litter piggery and litter stockpile over two trials in southern New South Wales, to compare emissions from housing pigs on deep litter with those of pigs from conventional housing with uncovered anaerobic effluent-treatment ponds. Emissions were measured using open-path Fourier transform infrared spectrometry, in conjunction with a backward Lagrangian stochastic model. Manure excretion was determined by mass balance and emission factors (EFs) were developed to report emissions relative to volatile solids and nitrogen (N) input. Nitrous oxide emissions per animal unit (1 AU ≤ 500 kg liveweight) from deep-litter sheds were negligible in winter, and 8.4 g/AU.day in summer. Ammonia emissions were 39.1 in winter and 52.2 g/AU.day in summer, while CH4 emissions were 16.1 and 21.6 g/AU.day in winter and summer respectively. Emission factors averaged from summer and winter emissions showed a CH4 conversion factor of 3.6%, an NH3-N EF of 10% and a N2O-N EF of 0.01 kg N2O-N/kg N excreted. For the litter stockpile, the simple average of summer and winter showed an EF for NH3-N of 14%, and a N2O-N EF of 0.02 kg N2O-N/kg-N of spent litter added to the stockpile. We observed a 66% and 80% decrease in emissions from the manure excreted in litter-based housing with litter stockpiling or without litter stockpiling, compared with conventional housing with an uncovered anaerobic effluent-treatment pond. This provides a sound basis for mitigation strategies that utilise litter-based housing as an alternative to conventional housing with uncovered anaerobic effluent-treatment ponds. © CSIRO 2016.

  13. Methane, nitrous oxide and ammonia emissions from pigs housed on litter and from stockpiling of spent litter

    KAUST Repository

    Phillips, F. A.

    2016-05-05

    Mitigation of agricultural greenhouse gas emissions is a target area for the Australian Government and the pork industry. The present study measured methane (CH4), nitrous oxide (N2O) and ammonia (NH3) from a deep-litter piggery and litter stockpile over two trials in southern New South Wales, to compare emissions from housing pigs on deep litter with those of pigs from conventional housing with uncovered anaerobic effluent-treatment ponds. Emissions were measured using open-path Fourier transform infrared spectrometry, in conjunction with a backward Lagrangian stochastic model. Manure excretion was determined by mass balance and emission factors (EFs) were developed to report emissions relative to volatile solids and nitrogen (N) input. Nitrous oxide emissions per animal unit (1 AU ≤ 500 kg liveweight) from deep-litter sheds were negligible in winter, and 8.4 g/AU.day in summer. Ammonia emissions were 39.1 in winter and 52.2 g/AU.day in summer, while CH4 emissions were 16.1 and 21.6 g/AU.day in winter and summer respectively. Emission factors averaged from summer and winter emissions showed a CH4 conversion factor of 3.6%, an NH3-N EF of 10% and a N2O-N EF of 0.01 kg N2O-N/kg N excreted. For the litter stockpile, the simple average of summer and winter showed an EF for NH3-N of 14%, and a N2O-N EF of 0.02 kg N2O-N/kg-N of spent litter added to the stockpile. We observed a 66% and 80% decrease in emissions from the manure excreted in litter-based housing with litter stockpiling or without litter stockpiling, compared with conventional housing with an uncovered anaerobic effluent-treatment pond. This provides a sound basis for mitigation strategies that utilise litter-based housing as an alternative to conventional housing with uncovered anaerobic effluent-treatment ponds. © CSIRO 2016.

  14. Direct Partial Oxidations Using Molecular Oxygen - Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Kemp, Richard [Univ. of New Mexico, Albuquerque, NM (United States)

    2017-11-01

    In 2006, Richard A. Kemp (University of New Mexico) and Karen I. Goldberg (University of Washington) formed a team and began to investigate new strategies to accomplish direct selective aerobic oxidations, with a particular emphasis on the epoxidation of propylene and higher olefins. This DOE-BES funded project was renewed twice and concluded after a no-cost extension earlier this year. Multiple novel strategies involving homogeneous catalyst systems were initiated and investigated during the award. Important fundamental understanding and insight concerning requirements for promotion of aerobic olefin epoxidation was generated. During the tenure of this project, new knowledge was generated concerning the synthesis, characterization and aerobic reactivity of metal hydrides and hydroxides. Key results describing synthetic strategies and optimization of the preparation of mononuclear late metal hydrides were published. The team reported the first example of O2 insertion into a Pd-H bond, a reaction which had been proposed in the literature but never previously observed. Our experimental investigation of the mechanism was later followed by computational work, and a description of what is now referred to as the Hydrogen Atom Abstraction (HAA) pathway for this reaction has been widely accepted in the community. After investigation of many other late metal hydrides, both experimentally and computationally, the team put together a chapter that included a description of key contributing factors that allow reaction by the HAA mechanism. A brief sampling of other classic papers from our project include hydrogenolysis reactions of late metal hydroxide and alkoxide complexes, the synthesis of nickel-hydrides, and the involvement of hemilabile ligands in promoting new reaction pathways.

  15. Modification of MWCNT@TiO{sub 2} core–shell nanocomposites with transition metal oxide dopants for photoreduction of carbon dioxide into methane

    Energy Technology Data Exchange (ETDEWEB)

    Gui, Meei Mei [Low Carbon Economy (LCE) Group, Chemical Engineering Discipline, School of Engineering, Monash University, Jalan Lagoon Selatan, 46150 Bandar Sunway, Selangor (Malaysia); Chai, Siang-Piao, E-mail: chai.siang.piao@monash.edu [Low Carbon Economy (LCE) Group, Chemical Engineering Discipline, School of Engineering, Monash University, Jalan Lagoon Selatan, 46150 Bandar Sunway, Selangor (Malaysia); Mohamed, Abdul Rahman [Low Carbon Economy (LCE) Group, School of Chemical Engineering, Universiti Sains Malaysia, Engineering Campus, Seri Ampangan, 14300 Nibong Tebal, Pulau Pinang (Malaysia)

    2014-11-15

    Graphical abstract: - Highlights: • Metal oxide-doped MWCNT@TiO{sub 2} core–shell nanocomposites were prepared. • Red-shift of absorption band positions was observed in CuO- and Fe{sub 2}O{sub 3}-MWCNT@TiO{sub 2}. • Total methane formation of 0.93 μmol/g-catalyst was achieved using CuO-MWCNT@TiO{sub 2}. - Abstract: Titanium dioxide (TiO{sub 2}) doped with visible-light-responsive metal oxides has been widely reported for improving the visible light absorption performance of TiO{sub 2} and its photocatalytic activity. The metal oxides could function as ‘charge-carrier traps’ that transport electrons from TiO{sub 2} through the heterojunction of the TiO{sub 2}-metal oxides. In this work, the common transition metal oxides, i.e. FeO{sub x}, CuO{sub x}, NiO, CoO{sub x} and ZnO, were doped onto MWCNT@TiO{sub 2} core–shell nanocomposites. The effects of the metal oxide dopants on the photoactivity of the core–shell nanocomposites on CO{sub 2} reduction were studied. Characterization with diffuse-reflectance UV–vis showed significant improvement on visible light absorption after doping MWCNT@TiO{sub 2} with CuO{sub x}, FeO{sub x} and CoO{sub x} with the adsorption band-edge position red-shifted into the wavelength range of 480–630 nm. CuO-MWCNT@TiO{sub 2} appeared to be the most active one among all the studied photocatalysts, achieving a total methane formation of 0.93 μmol/g-catalyst.

  16. Effects of sonication on co-precipitation synthesis and activity of copper manganese oxide catalyst to remove methane and sulphur dioxide gases.

    Science.gov (United States)

    Yap, Yeow Hong; Lim, Mitchell S W; Lee, Zheng Yee; Lai, Kar Chiew; Jamaal, Muhamad Ashraf; Wong, Farng Hui; Ng, Hoon Kiat; Lim, Siew Shee; Tiong, T Joyce

    2018-01-01

    The utilisation of ultrasound in chemical preparation has been the focus of intense study in various fields, including materials science and engineering. This paper presents a novel method of synthesising the copper-manganese oxide (Hopcalite) catalyst that is used for the removal of volatile organic compounds and greenhouse gases like carbon monoxide. Several samples prepared under different conditions, with and without ultrasound, were subjected to a series of characterisation tests such as XRD, BET, FE-SEM, EDX, TPR-H 2 , TGA and FT-IR in order to establish their chemical and physical properties. A series of catalytic tests using a micro-reactor were subsequently performed on the samples in order to substantiate the aforementioned properties by analysing their ability to oxidise compressed natural gas (CNG), containing methane and sulphur dioxide. Results showed that ultrasonic irradiation of the catalyst led to observable alterations in its morphology: surfaces of the particles were noticeably smoothed and an increased in amorphicity was detected. Furthermore, ultrasonic irradiation has shown to enhance the catalytic activity of Hopcalite, achieving a higher conversion of methane relative to non-sonicated samples. Varying the ultrasonic intensity also produced appreciable effects, whereby an increase in intensity results in a higher conversion rate. The catalyst sonicated at the highest intensity of 29.7W/cm 2 has a methane conversion rate of 13.5% at 400°C, which was the highest among all the samples tested. Copyright © 2017 Elsevier B.V. All rights reserved.

  17. Investigation of the effects of high-energy proton-beam irradiation on metal-oxide surfaces by using methane adsorption isotherms

    International Nuclear Information System (INIS)

    Kim, Euikwoun; Lee, Junggil; Kim, Jaeyong; Kim, Kyeryung

    2012-01-01

    The creation of possible local defects on metal-oxide surfaces due to irradiation with a high-energy proton beam was investigated by using a series of gas adsorption isotherms for methane (CH 4 ) on a MgO powder surface. After a MgO powder surface having only a (100) surface had been irradiated with a 35-MeV proton beam, the second atomic layer of methane had completely disappeared while two distinct atomic layers were found in a layer-by-layer fashion on the surfaces of unirradiated samples. This subtle modification of the surface is evidenced by a change of the contrasts in the morphologies measured a using a transmission electron microscopy. Combined results obtained from an electron microscopy and methane adsorption isotherms strongly suggest that the high-energy proton-beam irradiation induced a local surface modification by imparting kinetic energy to the sample. The calculation of the 2-dimensional compressibility values, which are responsible for the formation of the atomic layers, confirmed the surface modification after irradiating surface-clean MgO powders with a proton beam.

  18. Nitrogen-fixing methane-utilizing bacteria

    NARCIS (Netherlands)

    Bont, de J.A.M.

    1976-01-01

    Methane occurs abundantly in nature. In the presence of oxygen this gas may be metabolized by bacteria that are able to use it as carbon and energy source. Several types of bacteria involved in the oxidation of methane have been described in literature. Methane-utilizing bacteria have in

  19. Methylocella palustris gen. nov., sp. nov., a new methane-oxidizing acidophilic bacterium from peat bogs, representing a novel subtype of serine-pathway methanotrophs.

    Science.gov (United States)

    Dedysh, S N; Liesack, W; Khmelenina, V N; Suzina, N E; Trotsenko, Y A; Semrau, J D; Bares, A M; Panikov, N S; Tiedje, J M

    2000-05-01

    A new genus, Methylocella, and a new species, Methylocella palustris, are proposed for three strains of methane-oxidizing bacteria isolated from acidic Sphagnum peat bogs. These bacteria are aerobic, Gram-negative, colourless, non-motile, straight and curved rods that utilize the serine pathway for carbon assimilation, multiply by normal cell division and contain intracellular poly-beta-hydroxybutyrate granules (one at each pole). These strains use methane and methanol as sole sources of carbon and energy and are moderately acidophilic organisms with growth between pH 4.5 and pH 7.0, the optimum being at pH 5.0-5.5. The temperature range for growth is 10-28 degrees C with the optimum at 15-20 degrees C. The intracytoplasmic membrane system is different from those of type I and II methanotrophs. Cells contain an extensive periplasmic space and a vesicular membrane system connected to the cytoplasmic membrane. The strains grew only on media with a low salt content (0.2-0.5 g l(-1)). All three strains were found to possess soluble methane monooxygenase and are able to fix atmospheric nitrogen via an oxygen-sensitive nitrogenase. No products were observed in a PCR with particulate methane monooxygenase-targeted primers; hybridization with a pmoA probe was also negative. The major phospholipid fatty acids are 18:1 acids. The G+C content of the DNA is 61.2 mol%. The three strains share identical 16S rRNA gene sequences and represent a novel lineage of methane-oxidizing bacteria within the alpha-subclass of the class Proteobacteria and are only moderately related to type II methanotrophs of the Methylocystis-Methylosinus group. The three strains are most closely related to the acidophilic heterotrophic bacterium Beijerinckia indica subsp. indica (96.5% 16S rDNA sequence similarity). Collectively, these strains comprise a new species and genus Methylocella palustris gen. nov., sp. nov.; strain KT (= ATCC 700799T) is the type strain.

  20. Effects of straw incorporation along with microbial inoculant on methane and nitrous oxide emissions from rice fields

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Gang; Yu, Haiyang [State Key Laboratory of Soil and Sustainable Agriculture, Institute of Soil Science, Chinese Academy of Sciences, No. 71 East Beijing Road, Nanjing 210008 (China); University of Chinese Academy of Sciences, Beijing 100049 (China); Ma, Jing [State Key Laboratory of Soil and Sustainable Agriculture, Institute of Soil Science, Chinese Academy of Sciences, No. 71 East Beijing Road, Nanjing 210008 (China); Xu, Hua, E-mail: hxu@issas.ac.cn [State Key Laboratory of Soil and Sustainable Agriculture, Institute of Soil Science, Chinese Academy of Sciences, No. 71 East Beijing Road, Nanjing 210008 (China); Wu, Qinyan; Yang, Jinghui; Zhuang, Yiqing [Zhenjiang Institute of Agricultural Science of Hilly Regions in Jiangsu, Jurong 212400 (China)

    2015-06-15

    Incorporation of straw together with microbial inoculant (a microorganism agent, accelerating straw decomposition) is being increasingly adopted in rice cultivation, thus its effect on greenhouse gas (GHG) emissions merits serious attention. A 3-year field experiment was conducted from 2010 to 2012 to investigate combined effect of straw and microbial inoculant on methane (CH{sub 4}) and nitrous oxide (N{sub 2}O) emissions, global warming potential (GWP) and greenhouse gas intensity (GHGI) in a rice field in Jurong, Jiangsu Province, China. The experiment was designed to have treatment NPK (N, P and K fertilizers only), treatment NPKS (NPK plus wheat straw), treatment NPKSR (NPKS plus Ruilaite microbial inoculant) and treatment NPKSJ (NPKS plus Jinkuizi microbial inoculant). Results show that compared to NPK, NPKS increased seasonal CH{sub 4} emission by 280–1370%, while decreasing N{sub 2}O emission by 7–13%. When compared with NPKS, NPKSR and NPKSJ increased seasonal CH{sub 4} emission by 7–13% and 6–12%, respectively, whereas reduced N{sub 2}O emission by 10–27% and 9–24%, respectively. The higher CH{sub 4} emission could be attributed to the higher soil CH{sub 4} production potential triggered by the combined application of straw and microbial inoculant, and the lower N{sub 2}O emission to the decreased inorganic N content. As a whole, the benefit of lower N{sub 2}O emission was completely offset by increased CH{sub 4} emission, resulting in a higher GWP for NPKSR (5–12%) and NPKSJ (5–11%) relative to NPKS. Due to NPKSR and NPKSJ increased rice grain yield by 3–6% and 2–4% compared to NPKS, the GHGI values for NPKS, NPKSR and NPKSJ were comparable. These findings suggest that incorporating straw together with microbial inoculant would not influence the radiative forcing of rice production in the terms of per unit of rice grain yield relative to the incorporation of straw alone. - Highlights: • This paper presents 3-year measurements of CH

  1. Street-level emissions of methane and nitrous oxide from the wastewater collection system in Cincinnati, Ohio.

    Science.gov (United States)

    Fries, Anastasia E; Schifman, Laura A; Shuster, William D; Townsend-Small, Amy

    2018-05-01

    Recent studies have indicated that urban streets can be hotspots for emissions of methane (CH 4 ) from leaky natural gas lines, particularly in cities with older natural gas distribution systems. The objective of the current study was to determine whether leaking sewer pipes could also be a source of street-level CH 4 as well as nitrous oxide (N 2 O) in Cincinnati, Ohio, a city with a relatively new gas pipeline network. To do this, we measured the carbon (δ 13 C) and hydrogen (δ 2 H) stable isotopic composition of CH 4 to distinguish between biogenic CH 4 from sewer gas and thermogenic CH 4 from leaking natural gas pipelines and measured CH 4 and N 2 O flux rates and concentrations at sites from a previous study of street-level CH 4 enhancements (77 out of 104 sites) as well as additional sites found through surveying sewer grates and utility manholes (27 out of 104 sites). The average isotopic signatures for δ 13 C-CH 4 and δ 2 H-CH 4 were -48.5‰ ± 6.0‰ and -302‰ ± 142‰. The measured flux rates ranged from 0.0 to 282.5 mg CH 4 day -1 and 0.0-14.1 mg N 2 O day -1 (n = 43). The average CH 4 and N 2 O concentrations measured in our study were 4.0 ± 7.6 ppm and 392 ± 158 ppb, respectively (n = 104). 72% of sites where fluxes were measured were a source of biogenic CH 4 . Overall, 47% of the sampled sites had biogenic CH 4 , while only 13% of our sites had solely thermogenic CH 4 . The other sites were either a source of both biogenic and thermogenic CH 4 (13%), and a relatively large portion of sites had an unresolved source (29%). Overall, this survey of emissions across a large urban area indicates that production and emission of biogenic CH 4 and N 2 O is considerable, although CH 4 fluxes are lower than those reported for cities with leaky natural gas distribution systems. Copyright © 2018 Elsevier Ltd. All rights reserved.

  2. Critical Surface Parameters for the Oxidative Coupling of Methane over the Mn-Na-W/SiO2 Catalyst.

    Science.gov (United States)

    Hayek, Naseem S; Lucas, Nishita S; Warwar Damouny, Christine; Gazit, Oz M

    2017-11-22

    The work here presents a thorough evaluation of the effect of Mn-Na-W/SiO 2 catalyst surface parameters on its performance in the oxidative coupling of methane (OCM). To do so, we used microporous dealuminated β-zeolite (Zeo), or mesoporous SBA-15 (SBA), or macroporous fumed silica (Fum) as precursors for catalyst preparation, together with Mn nitrate, Mn acetate and Na 2 WO 4 . Characterizing the catalysts by inductively coupled plasma-optical emission spectroscopy, N 2 physisorption, X-ray diffraction, high-resolution scanning electron microscopy-energy-dispersive spectroscopy, X-ray photoelectron spectroscopy, and catalytic testing enabled us to identify critical surface parameters that govern the activity and C 2 selectivity of the Mn-Na-W/SiO 2 catalyst. Although the current paradigm views the phase transition of silica to α-cristobalite as the critical step in obtaining dispersed and stable metal sites, we show that the choice of precursors is equally or even more important with respect to tailoring the right surface properties. Specifically, the SBA-based catalyst, characterized by relatively closed surface porosity, demonstrated low activity and low C 2 selectivity. By contrast, for the same composition, the Zeo-based catalyst showed an open surface pore structure, which translated up to fourfold higher activity and enhanced selectivity. By varying the overall composition of the Zeo catalysts, we show that reducing the overall W concentration reduces the size of the Na 2 WO 4 species and increases the catalytic activity linearly as much as fivefold higher than the SBA catalyst. This linear dependence correlates well to the number of interfaces between the Na 2 WO 4 and Mn 2 O 3 species. Our results combined with prior studies lead us to single out the interface between Na 2 WO 4 and Mn 2 O 3 as the most probable active site for OCM using this catalyst. Synergistic interactions between the various precursors used and the phase transition are discussed in

  3. Changes of soil carbon dioxide, methane, and nitrous oxide fluxes in relation to land use/cover management.

    Science.gov (United States)

    Kooch, Yahya; Moghimian, Negar; Bayranvand, Mohammad; Alberti, Giorgio

    2016-06-01

    Conversions of land use/cover are associated with changes in soil properties and biogeochemical cycling, with implications for carbon (C), nitrogen (N), and trace gas fluxes. In an attempt to provide a comprehensive evaluation of the significance of different land uses (Alnus subcordata plantation, Taxodium distichum plantation, agriculture, and deforested areas) on soil features and on the dynamics of greenhouse gas (GHG) fluxes at local scale, this study was carried out in Mazandaran province, northern Iran. Sixteen samples per land use, from the top 10 cm of soil, were taken, from which bulk density, texture, water content, pH, organic C, total N, microbial biomass of C and N, and earthworm density/biomass were determined. In addition, the seasonal changes in the fluxes of carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) were monitored over a year. Our results indicated that the different land uses were different in terms of soil properties and GHG fluxes. Even though the amount of the GHG varied widely during the year, the highest CO2 and CH4 fluxes (0.32 mg CO2 m(-2) day(-1) and 0.11 mg CH4 m(-2) day(-1), respectively) were recorded in the deforested areas. N2O flux was higher in Alnus plantation (0.18 mg N2O m(-2) day(-1)) and deforested areas (0.17 mg N2O m(-2) day(-1)) than at agriculture site (0.05 mg N2O m(-2) day(-1)) and Taxodium plantation (0.03 mg N2O m(-2) day(-1)). This study demonstrated strong impacts of land use change on soil-atmosphere trace gas exchanges and provides useful observational constraints for top-down and bottom-up biogeochemistry models.

  4. Temporal and spatial variations of soil carbon dioxide, methane, and nitrous oxide fluxes in a Southeast Asian tropical rainforest

    Science.gov (United States)

    Itoh, M.; Kosugi, Y.; Takanashi, S.; Hayashi, Y.; Kanemitsu, S.; Osaka, K.; Tani, M.; Nik, A. R.

    2010-09-01

    To clarify the factors controlling temporal and spatial variations of soil carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) fluxes, we investigated these gas fluxes and environmental factors in a tropical rainforest in Peninsular Malaysia. Temporal variation of CO2 flux in a 2-ha plot was positively related to soil water condition and rainfall history. Spatially, CO2 flux was negatively related to soil water condition. When CO2 flux hotspots were included, no other environmental factors such as soil C or N concentrations showed any significant correlation. Although the larger area sampled in the present study complicates explanations of spatial variation of CO2 flux, our results support a previously reported bipolar relationship between the temporal and spatial patterns of CO2 flux and soil water condition observed at the study site in a smaller study plot. Flux of CH4 was usually negative with little variation, resulting in the soil at our study site functioning as a CH4 sink. Both temporal and spatial variations of CH4 flux were positively related to the soil water condition. Soil N concentration was also related to the spatial distribution of CH4 flux. Some hotspots were observed, probably due to CH4 production by termites, and these hotspots obscured the relationship between both temporal and spatial variations of CH4 flux and environmental factors. Temporal variation of N2O flux and soil N2O concentration was large and significantly related to the soil water condition, or in a strict sense, to rainfall history. Thus, the rainfall pattern controlled wet season N2O production in soil and its soil surface flux. Spatially, large N2O emissions were detected in wet periods at wetter and anaerobic locations, and were thus determined by soil physical properties. Our results showed that, even in Southeast Asian rainforests where distinct dry and wet seasons do not exist, variation in the soil water condition related to rainfall history controlled the