Activation of methane by transition metal-substituted aluminophosphate molecular sieves
Iton, Lennox E.; Maroni, Victor A.
1991-01-01
Aluminophosphate molecular sieves substituted with cobalt, manganese or iron and having the AlPO.sub.4 -34 or AlPO.sub.4 -5, or related AlPO.sub.4 structure activate methane starting at approximately 350.degree. C. Between 400.degree. and 500.degree. C. and at methane pressures .ltoreq.1 atmosphere the rate of methane conversion increases steadily with typical conversion efficiencies at 500.degree. C. approaching 50% and selectivity to the production of C.sub.2+ hydrocarbons approaching 100%. The activation mechanism is based on reduction of the transition metal(III) form of the molecular sieve to the transition metal(II) form with accompanying oxidative dehydrogenation of the methane. Reoxidation of the - transition metal(II) form to the transition metal(III) form can be done either chemically (e.g., using O.sub.2) or electrochemically.
Nuchdang, Sasikarn; Khemkhao, Maneerat; Techkarnjanaruk, Somkiet; Phalakornkule, Chantaraporn
2015-05-01
The effect of inoculum sources on the anaerobic digestion of paragrass was investigated. Two types of sludge were used as the inoculums: an anaerobic sludge obtained from a domestic wastewater treatment plant (OS) and a sludge acclimated to fibrous substrates in raw palm oil mill effluent (AMC). Microbial activity assays showed that the AMC had hydrolytic and acetogenic activities two times greater than the activities of the OS. In addition, the production of methane from acetate by the AMC occurred without a lag phase, while it took 8 days for the OS to start producing methane from the same substrate. The biochemical methane potential after 80 days digestion was 316 ml STP/g VS(added) using the AMC, and 277 ml STP/g VS(added) using the OS. The methane potential of the paragrass was estimated to be 3337 Nm(3) CH4/ha a. Copyright © 2015 Elsevier Ltd. All rights reserved.
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.
Water-Gas Shift and Methane Reactivity on Reducible Perovskite-Type Oxides
2015-01-01
Comparative (electro)catalytic, structural, and spectroscopic studies in hydrogen electro-oxidation, the (inverse) water-gas shift reaction, and methane conversion on two representative mixed ionic–electronic conducting perovskite-type materials La0.6Sr0.4FeO3−δ (LSF) and SrTi0.7Fe0.3O3−δ (STF) were performed with the aim of eventually correlating (electro)catalytic activity and associated structural changes and to highlight intrinsic reactivity characteristics as a function of the reduction state. Starting from a strongly prereduced (vacancy-rich) initial state, only (inverse) water-gas shift activity has been observed on both materials beyond ca. 450 °C but no catalytic methane reforming or methane decomposition reactivity up to 600 °C. In contrast, when starting from the fully oxidized state, total methane oxidation to CO2 was observed on both materials. The catalytic performance of both perovskite-type oxides is thus strongly dependent on the degree/depth of reduction, on the associated reactivity of the remaining lattice oxygen, and on the reduction-induced oxygen vacancies. The latter are clearly more reactive toward water on LSF, and this higher reactivity is linked to the superior electrocatalytic performance of LSF in hydrogen oxidation. Combined electron microscopy, X-ray diffraction, and Raman measurements in turn also revealed altered surface and bulk structures and reactivities. PMID:26045733
NASA Astrophysics Data System (ADS)
Jung, Heon; Yoon, Wang Lai; Lee, Hotae; Park, Jong Soo; Shin, Jang Sik; La, Howon; Lee, Jong Dae
A palladium-washcoated metallic monolith catalyst is applied to the partial oxidation of methane to syngas. This catalyst is highly active at a gas hourly space velocity (GHSV) of 100,000 h -1. The compact partial oxidation (POX) reactor equipped with both 96 cc of the metallic monolith catalyst and an electrically-heated catalyst (EHC) has a start-up time of less than 1.5 min and a syngas generation capacity of 9.5 Nm 3 h -1. The POX reaction is sustained without the need for an external heater. With the stand-alone POX reactor, the methane conversion can be increased either by preheating the reactant mixture heat-exchanged with the product gas, or by supplying a larger amount of oxygen than is necessary for the reaction stoichiometry.
Giannini, Giuseppe; Marzi, Mauro; Marzo, Maria Di; Battistuzzi, Gianfranco; Pezzi, Riccardo; Brunetti, Tiziana; Cabri, Walter; Vesci, Loredana; Pisano, Claudio
2009-05-15
In order to gather further knowledge about the structural requirements on histone deacetylase inhibitors (HDACi), starting from the schematic model of the common pharmacophore that characterizes this class of molecules (surface recognition CAP group-connection unit-linker region-Zinc Binding Group), we designed and synthesized a series of hydroxamic acids containing a bis-(indolyl)methane moiety. HDAC inhibition profile and antiproliferative activity were evaluated.
NASA Astrophysics Data System (ADS)
Heeb, Norbert V.; Forss, Anna-Maria; Saxer, Christian J.; Wilhelm, Patrick
The US urban driving cycle (FTP-75) is widely used to estimate both the emissions under hot engine conditions as well as those associated with the cold start. Applying fast analysis techniques such as chemical ionization mass spectrometry (CI-MS) the warm-up behavior of individual vehicles can be monitored at a time resolution of 1 s. CI-MS has been used to investigate the emissions of methane, benzene and the alkyl benzene class of compounds. The amount of the emissions at cold start influence was deduced from the time-resolved emission data of four gasoline-driven vehicle classes representing the vehicle technology of the last two decades. Overall, the emissions of five EURO-0, 20 EURO-1, 18 EURO-2 and so far of six EURO-3 passenger cars were recorded. The test vehicles were selected from the currently operating Swiss car fleet based on the car sales statistics. The average methane, benzene and alkyl benzene cold start emissions are reported using both, the traditional bag method as well as the regression model. At room temperature a clear reduction of 94%, 81% and 85% was found for the methane, benzene and alkyl benzene cold start emissions from EURO-0 to EURO-3 technology, respectively.
NASA Astrophysics Data System (ADS)
Kanduč, Tjaša; Žigon, Stojan; Grassa, Fausto; Sedlar, Jerneja; Zadnik, Ivo; Zavšek, Simon
2016-04-01
Unconventional gas resources, including coal bed methane and shale gas, are a growing part of the global energy mix, which has changed the economic and strategic picture for gas consuming and producing countries, including the USA, China and Australia that, together are responsible for around half the currently recoverable unconventional gas resources. However, CBM production was often hindered by low permeability and mineralization in cleats and fractures, necessitating the development of cost effective horizontal drilling and completion techniques. Geochemical and isotopic monitoring of coalbed gases at excavation fields in Velenje Basin started in year 2000, with the aim to obtain better insights into the origin of coalbed gases. Results from active excavation fields in the mining areas Pesje and Preloge in the year period 2014-2015 are presented in this study. Composition and isotopic composition of coalbed gases were determined with mass - spectrometric methods. The chemical (methane, carbon dioxide, nitrogen) and isotopic composition of carbon in methane and carbon dioxide in the Velenje Basin vary and depend on the composition of the source of coalbed gas before excavation, advancement of the working face, depth of the longwall face, pre-mining activity and newly mined activity. The basic gas components determined in excavation fields are carbon dioxide and methane. Knowledge of the stable isotope geochemistry of coal bed and shale gas and the related production water is essential to determine not only gas origins but also the dominant methanogenic pathway in the case of microbial gas. Concentrations of methane at active excavation fields are changing from 1.8 to 63.9 %, concentrations of carbon dioxide are changing from 36.1 to 98.2% and CDMI (Carbon Dioxide Methane Index) index from 0.2 to 100 %. Isotopic composition of carbon dioxide is changing from -11.0 to -1.9‰ , isotopic composition of methane from -71.8 to -43.3‰ , isotopic composition of deuterium in methane from -343.9 to -223.1‰ , respectively. Further, these characteristics of methane have been compared with those observed in other coal sedimentary basins worldwide. The isotopic compositions of carbon and hydrogen in methane in the excavation fields show its biogenic origin, while a high Carbon Dioxide Methane Index (CDMI index) indicates the bacterial and endogenic origin of carbon dioxide.
Hwang, In Yeub; Lee, Seung Hwan; Choi, Yoo Seong; Park, Si Jae; Na, Jeong Geol; Chang, In Seop; Kim, Choongik; Kim, Hyun Cheol; Kim, Yong Hwan; Lee, Jin Won; Lee, Eun Yeol
2014-12-28
Methane is considered as a next-generation carbon feedstock owing to the vast reserves of natural and shale gas. Methane can be converted to methanol by various methods, which in turn can be used as a starting chemical for the production of value-added chemicals using existing chemical conversion processes. Methane monooxygenase is the key enzyme that catalyzes the addition of oxygen to methane. Methanotrophic bacteria can transform methane to methanol by inhibiting methanol dehydrogenase. In this paper, we review the recent progress made on the biocatalytic conversion of methane to methanol as a key step for methane-based refinery systems and discuss future prospects for this technology.
Yu, Hongguang; Wang, Qiaoying; Wang, Zhiwei; Sahinkaya, Erkan; Li, Yongli; Ma, Jinxing; Wu, Zhichao
2014-01-01
An anaerobic dynamic membrane digester (ADMD) was developed to digest waste sludge, and pyrosequencing was used to analyze the variations of the bacterial and archaeal communities during the start-up. Results showed that bacterial community richness decreased and then increased over time, while bacterial diversity remained almost the same during the start-up. Proteobacteria and Bacteroidetes were the major phyla. At the class level, Betaproteobacteria was the most abundant at the end of start-up, followed by Sphingobacteria. In the archaeal community, richness and diversity peaked at the end of the start-up stage. Principle component and cluster analyses demonstrated that archaeal consortia experienced a distinct shift and became stable after day 38. Methanomicrobiales and Methanosarcinales were the two predominant orders. Further investigations indicated that Methanolinea and Methanosaeta were responsible for methane production in the ADMD system. Hydrogenotrophic pathways might prevail over acetoclastic means for methanogenesis during the start-up, supported by specific methanogenic activity tests. PMID:24695488
30 CFR 57.22208 - Auxiliary fans (I-A, II-A, III, and V-A mines).
Code of Federal Regulations, 2010 CFR
2010-07-01
... NONMETAL MINES Safety Standards for Methane in Metal and Nonmetal Mines Ventilation § 57.22208 Auxiliary... which have been so designed that methane cannot enter the airway, shall be approved by MSHA under the...) Tests for methane shall be made at auxiliary fans before they are started. ...
30 CFR 57.22209 - Auxiliary fans (I-C mines).
Code of Federal Regulations, 2010 CFR
2010-07-01
... Standards for Methane in Metal and Nonmetal Mines Ventilation § 57.22209 Auxiliary fans (I-C mines.... Tests for methane shall be made at electric auxiliary fans before they are started. Such fans shall not be operated when air passing over or through them contains 0.5 percent or more methane. ...
30 CFR 57.22209 - Auxiliary fans (I-C mines).
Code of Federal Regulations, 2011 CFR
2011-07-01
... Standards for Methane in Metal and Nonmetal Mines Ventilation § 57.22209 Auxiliary fans (I-C mines.... Tests for methane shall be made at electric auxiliary fans before they are started. Such fans shall not be operated when air passing over or through them contains 0.5 percent or more methane. ...
Role of Megafauna and Frozen Soil in the Atmospheric CH4 Dynamics
Zimov, Sergey; Zimov, Nikita
2014-01-01
Modern wetlands are the world’s strongest methane source. But what was the role of this source in the past? An analysis of global 14C data for basal peat combined with modelling of wetland succession allowed us to reconstruct the dynamics of global wetland methane emission through time. These data show that the rise of atmospheric methane concentrations during the Pleistocene-Holocene transition was not connected with wetland expansion, but rather started substantially later, only 9 thousand years ago. Additionally, wetland expansion took place against the background of a decline in atmospheric methane concentration. The isotopic composition of methane varies according to source. Owing to ice sheet drilling programs past dynamics of atmospheric methane isotopic composition is now known. For example over the course of Pleistocene-Holocene transition atmospheric methane became depleted in the deuterium isotope, which indicated that the rise in methane concentrations was not connected with activation of the deuterium-rich gas clathrates. Modelling of the budget of the atmospheric methane and its isotopic composition allowed us to reconstruct the dynamics of all main methane sources. For the late Pleistocene, the largest methane source was megaherbivores, whose total biomass is estimated to have exceeded that of present-day humans and domestic animals. This corresponds with our independent estimates of herbivore density on the pastures of the late Pleistocene based on herbivore skeleton density in the permafrost. During deglaciation, the largest methane emissions originated from degrading frozen soils of the mammoth steppe biome. Methane from this source is unique, as it is depleted of all isotopes. We estimated that over the entire course of deglaciation (15,000 to 6,000 year before present), soils of the mammoth steppe released 300–550 Pg (1015 g) of methane. From current study we conclude that the Late Quaternary Extinction significantly affected the global methane cycle. PMID:24695117
Code of Federal Regulations, 2010 CFR
2010-07-01
... start-up, whichever date comes first. Each owner or operator shall either: (a) Reduce emissions of TOC (minus methane and ethane) by 98 weight-percent, or to a TOC (minus methane and ethane) concentration of...
Methane Explosion Mitigation in Coal Mines by Water Mist
NASA Astrophysics Data System (ADS)
Chikhradze, Nikoloz; Mataradze, Edgar; Chikhradze, Mikheil; Krauthammer, Ted; Mansurov, Zulkhair; Alyiev, Erhan
2017-12-01
Statistics shows that the majority of accidents with fatal outcome are caused by methane and/or coal dust explosion. This leads to assume that contemporary counter-explosion systems of various designs cannot be considered effective. Considering the growing threat of methane explosion in the coming years along with the development of deeper levels, the improvement of a system for protecting people in underground opening appears urgent. This paper focuses on technical solutions to be used in designing a protective system for minimizing the consequences of methane explosions in coalmines. The new protective system consists of three main modules: i) a high-speed shock wave suppression section; ii) a suppression section with a long-term action and iii) a system activating device. The shock wave suppressor contains a 200 litre volume water tank with a built-in gas generator and nozzles. It is activated after 12ms from the blast moment, the duration of discharge is 40 s. The suppression section with a long-term action contains a 2000 litre volume water tank, a high-pressure pump, a hydraulic accumulator, solenoid valves, and a system of pipes with built-in nozzles. It is activated after 4 s from the blast moment, the duration of discharge is 8 min. The activation device includes a detection block containing sensors, an emergency signal generation module, a signal transmission module, a signal receiving module and a power supply module. The system operates in a waiting mode and activates immediately upon the receipt of the start signal generated by the detector. The paper also addresses the preliminary results of the system prototype testing in the tunnel.
30 CFR 75.1913 - Starting aids.
Code of Federal Regulations, 2012 CFR
2012-07-01
... is taking place; or (3) Used in any area where 1.0 percent or greater concentration of methane is... fuel starting aids shall be used in accordance with recommendations provided by the starting aid... fuel starting aids shall be stored in metal enclosures that are used only for storage of starting aids...
30 CFR 75.1913 - Starting aids.
Code of Federal Regulations, 2010 CFR
2010-07-01
... is taking place; or (3) Used in any area where 1.0 percent or greater concentration of methane is... fuel starting aids shall be used in accordance with recommendations provided by the starting aid... fuel starting aids shall be stored in metal enclosures that are used only for storage of starting aids...
30 CFR 75.1913 - Starting aids.
Code of Federal Regulations, 2013 CFR
2013-07-01
... is taking place; or (3) Used in any area where 1.0 percent or greater concentration of methane is... fuel starting aids shall be used in accordance with recommendations provided by the starting aid... fuel starting aids shall be stored in metal enclosures that are used only for storage of starting aids...
30 CFR 75.1913 - Starting aids.
Code of Federal Regulations, 2011 CFR
2011-07-01
... is taking place; or (3) Used in any area where 1.0 percent or greater concentration of methane is... fuel starting aids shall be used in accordance with recommendations provided by the starting aid... fuel starting aids shall be stored in metal enclosures that are used only for storage of starting aids...
30 CFR 75.1913 - Starting aids.
Code of Federal Regulations, 2014 CFR
2014-07-01
... is taking place; or (3) Used in any area where 1.0 percent or greater concentration of methane is... fuel starting aids shall be used in accordance with recommendations provided by the starting aid... fuel starting aids shall be stored in metal enclosures that are used only for storage of starting aids...
Santos, M M O; van Elk, A G P; Romanel, C
2015-12-01
Solid waste disposal sites (SWDS) - especially landfills - are a significant source of methane, a greenhouse gas. Although having the potential to be captured and used as a fuel, most of the methane formed in SWDS is emitted to the atmosphere, mainly in developing countries. Methane emissions have to be estimated in national inventories. To help this task the Intergovernmental Panel on Climate Change (IPCC) has published three sets of guidelines. In addition, the Kyoto Protocol established the Clean Development Mechanism (CDM) to assist the developed countries to offset their own greenhouse gas emissions by assisting other countries to achieve sustainable development while reducing emissions. Based on methodologies provided by the IPCC regarding SWDS, the CDM Executive Board has issued a tool to be used by project developers for estimating baseline methane emissions in their project activities - on burning biogas from landfills or on preventing biomass to be landfilled and so avoiding methane emissions. Some inconsistencies in the first two IPCC guidelines have already been pointed out in an Annex of IPCC latest edition, although with hidden details. The CDM tool uses a model for methane estimation that takes on board parameters, factors and assumptions provided in the latest IPCC guidelines, while using in its core equation the one of the second IPCC edition with its shortcoming as well as allowing a misunderstanding of the time variable. Consequences of wrong ex-ante estimation of baseline emissions regarding CDM project activities can be of economical or environmental type. Example of the first type is the overestimation of 18% in an actual project on biogas from landfill in Brazil that harms its developers; of the second type, the overestimation of 35% in a project preventing municipal solid waste from being landfilled in China, which harms the environment, not for the project per se but for the undue generated carbon credits. In a simulated landfill - the same amount of waste for 20 years -, the error would be an overestimation of 25% if the CDM project activity starts from the very first year or an underestimation of 15% if it starts just after the landfill closure. Therefore, a correction in the tool to calculate emissions from landfills as adopted by the CDM Executive Board is needed. Moreover, in countries not using the latest IPCC guidelines, which provides clear formulas to prevent misunderstandings, inventory compilers can also benefit from this paper by having more accurate results in national GHG inventories related to solid waste disposal, especially when increasing amounts of waste are landfilled, which is the case of the developing countries. Copyright © 2015 Elsevier Ltd. All rights reserved.
30 CFR 57.22228 - Preshift examination (I-A, I-C, II-A, III, and V-A mines).
Code of Federal Regulations, 2014 CFR
2014-07-01
... the beginning of a shift following an idle shift, a competent person shall test the mine atmosphere... immediately follows another, a competent person shall test the mine atmosphere at each active working face for methane before work is started on that shift. (d) A competent person shall test the mine atmosphere at...
30 CFR 57.22228 - Preshift examination (I-A, I-C, II-A, III, and V-A mines).
Code of Federal Regulations, 2013 CFR
2013-07-01
... the beginning of a shift following an idle shift, a competent person shall test the mine atmosphere... immediately follows another, a competent person shall test the mine atmosphere at each active working face for methane before work is started on that shift. (d) A competent person shall test the mine atmosphere at...
30 CFR 57.22228 - Preshift examination (I-A, I-C, II-A, III, and V-A mines).
Code of Federal Regulations, 2012 CFR
2012-07-01
... the beginning of a shift following an idle shift, a competent person shall test the mine atmosphere... immediately follows another, a competent person shall test the mine atmosphere at each active working face for methane before work is started on that shift. (d) A competent person shall test the mine atmosphere at...
Research on soybean protein wastewater treatment by the integrated two-phase anaerobic reactor
Yu, Yaqin
2015-01-01
The start-up tests of treating soybean protein wastewater by the integrated two-phase anaerobic reactor were studied. The results showed that the soybean protein wastewater could be successfully processed around 30 days when running under the situation of dosing seed sludge with the influent of approximately 2000 mg/L and an HRT of 40 h. When the start-up was finished, the removal rate of COD by the reactor was about 80%. In the zone I, biogas mainly revealed carbon dioxide (CO2) and hydrogen (H2). Methane was the main component in the zone 2 which ranged from 53% to 59% with an average of 55%. The methane content in biogas increased from the zone I to II. It indicated that the methane-producing capacity of the anaerobic sludge increased. It was found that the uniquely designed two-phase integrated anaerobic reactor played a key role in treating soybean protein wastewater. The acidogenic fermentation bacteria dominated in the zone I, while methanogen became dominant in the zone II. It realized the relatively effective separation of hydrolysis acidification and methanogenesis process in the reactor, which was benefit to promote a more reasonable space distribution of the microbial communities in the reactor. There were some differences between the activities of the sludge in the two reaction zones of the integrated two-phase anaerobic reactor. The activity of protease was higher in the reaction zone I. And the coenzyme F420 in the reaction zone II was twice than that in the reaction zone I, which indicated that the activity of the methanogens was stronger in the reaction zone II. PMID:26288554
NASA Astrophysics Data System (ADS)
Dillon, A.; Penafiel, R.; Garzón, P. V.; Ochoa, V.
2015-12-01
Industrial processes to extract crude palm oil, generates large amounts of waste water. High concentrations of COD, ST, SV, NH4 + and low solubility of O2, make the treatment of these effluents starts with anaerobic processes. The anaerobic digestion process has several advantages over aerobic degradation: lower operating costs (not aeration), low sludge production, methane gas generation. The 4 stages of anaerobic digestion are: hydrolysis, acidogenic, acetogenesis and methanogenesis. Through the action of enzymes synthesized by microbial consortia are met. The products of each step to serve as reagents is conducted as follows. The organic load times and cell hydraulic retention, solids content, nutrient availability, pH and temperature are factors that influence directly in biodigesters. The objectives of this presentation is to; characterize the microbial inoculum and water (from palm oil wasted water) to be used in biodigestores, make specific methanogenic activity in bioassays, acclimatize the microorganisms to produce methane gas using basal mineral medium with acetate for the input power, and to determine the production of methane gas digesters high organic load.
M.R. Turetsky; C.C. Treat; M. Waldrop; J.M. Waddington; J.W. Harden; A.D. McGuire
2008-01-01
Growing season CH4 fluxes were monitored over a two year period following the start of ecosystem-scale manipulations of water table position and surface soil temperatures in a moderate rich fen in interior Alaska. The largest CH4 fluxes occurred in plots that received both flooding (raised water table position) and soil...
LaBarge, Nicole; Yilmazel, Yasemin Dilsad; Hong, Pei-Ying; Logan, Bruce E
2017-02-01
Microbial electrolysis cells (MECs) can generate methane by fixing carbon dioxide without using expensive catalysts, but the impact of acclimation procedures on subsequent performance has not been investigated. Granular activated carbon (GAC) was used to pre-enrich electrotrophic methanogenic communities, as GAC has been shown to stimulate direct transfer of electrons between different microbial species. MEC startup times using pre-acclimated GAC were improved compared to controls (without pre-acclimation or without GAC), and after three fed batch cycles methane generation rates were similar (P>0.4) for GAC acclimated to hydrogen (22±9.3nmolcm -3 d -1 ), methanol (25±9.7nmolcm -3 d -1 ), and a volatile fatty acid (VFA) mix (22±11nmolcm -3 d -1 ). However, MECs started with GAC but no pre-acclimation had lower methane generation rates (13±4.1nmolcm -3 d -1 ), and MECs without GAC had the lowest rates (0.7±0.8nmolcm -3 d -1 after cycle 2). Microbes previously found in methanogenic MECs, or previously shown to be capable of exocellular electron transfer, were enriched on the GAC. Pre-acclimation using GAC is therefore a simple approach to enrich electroactive communities, improve methane generation rates, and decrease startup times in MECs. Copyright © 2016 Elsevier B.V. All rights reserved.
Catalysis in high-temperature fuel cells.
Föger, K; Ahmed, K
2005-02-17
Catalysis plays a critical role in solid oxide fuel cell systems. The electrochemical reactions within the cell--oxygen dissociation on the cathode and electrochemical fuel combustion on the anode--are catalytic reactions. The fuels used in high-temperature fuel cells, for example, natural gas, propane, or liquid hydrocarbons, need to be preprocessed to a form suitable for conversion on the anode-sulfur removal and pre-reforming. The unconverted fuel (economic fuel utilization around 85%) is commonly combusted using a catalytic burner. Ceramic Fuel Cells Ltd. has developed anodes that in addition to having electrochemical activity also are reactive for internal steam reforming of methane. This can simplify fuel preprocessing, but its main advantage is thermal management of the fuel cell stack by endothermic heat removal. Using this approach, the objective of fuel preprocessing is to produce a methane-rich fuel stream but with all higher hydrocarbons removed. Sulfur removal can be achieved by absorption or hydro-desulfurization (HDS). Depending on the system configuration, hydrogen is also required for start-up and shutdown. Reactor operating parameters are strongly tied to fuel cell operational regimes, thus often limiting optimization of the catalytic reactors. In this paper we discuss operation of an authothermal reforming reactor for hydrogen generation for HDS and start-up/shutdown, and development of a pre-reformer for converting propane to a methane-rich fuel stream.
The effect of feed composition on anaerobic co-digestion of animal-processing by-products.
Hidalgo, D; Martín-Marroquín, J M; Corona, F
2018-06-15
Four streams and their mixtures have been considered for anaerobic co-digestion, all of them generated during pig carcasses processing or in related industrial activities: meat flour (MF), process water (PW), pig manure (PM) and glycerin (GL). Biochemical methane potential assays were conducted at 37 °C to evaluate the effects of the substrate mix ratio on methane generation and process behavior. The results show that the co-digestion of these products favors the anaerobic fermentation process when limiting the amount of meat flour in the mixture to co-digest, which should not exceed 10%. The ratio of other tested substrates is less critical, because different mixtures reach similar values of methane generation. The presence in the mixture of process water contributes to a quick start of the digester, something very interesting when operating an industrial reactor. The analysis of the fraction digested reveals that the four analyzed streams can be, a priori, suitable for agronomic valorization once digested. Copyright © 2017. Published by Elsevier Ltd.
NASA Astrophysics Data System (ADS)
Mastepanov, Mikhail; Christensen, Torben
2014-05-01
Methane emissions have been monitored by an automatic chamber method in Zackenberg valley, NE Greenland, since 2006 as a part of Greenland Ecosystem Monitoring (GEM) program. During most of the seasons the measurements were carried out from the time of snow melt (June-July) until freezing of the active layer (October-November). Several years of data, obtained by the same method, instrumentation and at exactly the same site, provided a unique opportunity for the analysis of interannual methane flux patterns and factors affecting their temporal variability. The start of the growing season emissions was found to be closely related to a date of snow melt at the site. Despite a large between year variability of this date (sometimes more than a month), methane emission started within a few days after, and was increasing for the next about 30 days. After this peak of emission, it slowly decreased and stayed more or less constant or slightly decreasing during the rest of the growing season (Mastepanov et al., Biogeosciences, 2013). During the soil freezing, a second peak of methane emission was found (Mastepanov et al., Nature, 2008); its amplitude varied a lot between the years, from almost undetectable to comparable with total growing season emissions. Analysis of the multiyear emission patterns (Mastepanov et al., Biogeosciences, 2013) led to hypotheses of different sources for the spring, summer and autumn methane emissions, and multiyear cycles of accumulation and release of these components to the atmosphere. For the further investigation of this it was decided to complement the monitoring system with a methane carbon isotope analyzer (Los Gatos Research, USA). The instrument was installed during 2013 field season and was successfully operating until the end of the measurement campaign (27 October). Detecting both 12C-CH4 and 13C-CH4 concentrations in real time (0.5 Hz) during automatic chamber closure (15 min), the instrument was providing data for determination of δ13C of the emitting methane (by a relation between 12C-CH4 and 13C-CH4 fluxes). Unfortunately, the beginning of the season was missed due to a delay in the instrument shipment; the summer fluxes were lower than any of the 7 previous years due to an exceptional drought; the autumn burst was not detected due to both exceptionally slow soil freezing and a low soil methane content. However, the data obtained from the most productive chambers confirm the feasibility of the chosen method and give good expectations for the following field campaign 2014.
40 CFR 86.004-2 - Definitions.
Code of Federal Regulations, 2012 CFR
2012-07-01
... (3) The AECD does not go beyond the requirements of engine starting. U.S.-directed production means...-duty diesel engines, for carbon monoxide, particulate, and oxides of nitrogen plus non-methane... non-methane hydrocarbons emission standards, a period of use of 10 years or 185,000 miles, whichever...
Liquid Oxygen/Liquid Methane Ascent Main Engine Technology Development
NASA Technical Reports Server (NTRS)
Robinson, Joel W.; Stephenson, David D.
2008-01-01
The National Aeronautics & Space Administration (NASA) has identified Liquid Oxygen (LO2)/Liquid Methane (LCH4) as a potential propellant combination for future space vehicles based upon the Exploration Systems Architecture Study (ESAS). The technology is estimated to have higher performance and lower overall systems mass compared to existing hypergolic propulsion systems. The current application considering this technology is the lunar ascent main engine (AME). AME is anticipated to be an expendable, pressure-fed engine to provide ascent from the moon at the completion of a 210 day lunar stay. The engine is expected to produce 5,500 lbf (24,465 N) thrust with variable inlet temperatures due to the cryogenic nature of the fuel and oxidizer. The primary technology risks include establishing reliable and robust ignition in vacuum conditions, maximizing specific impulse, developing rapid start capability for the descent abort, providing the capability for two starts and producing a total engine bum time over 500 seconds. This paper will highlight the efforts of the Marshall Space Flight Center (MSFC) in addressing risk reduction activities for this technology.
Co-digestion of domestic kitchen waste and night soil sludge in a full-scale sludge treatment plant.
Yoneyama, Y; Takeno, K
2002-01-01
A study was made on the domestic kitchen waste and night soil treatment performance of a full-scale sludge treatment plant. The sludge treatment at this plant was by thermophilic methane fermentation. The initial treatment, mesophilic to thermophilic fermentation, was able to be started up within a short time by adjusting the amount of influent waste. Thermophilic methane fermentation was carried out for five months (May-October) and the performance under a mean residual time of 22 days indicated a VTS decomposition of 42%, gas generation of 54-1,610 m3/day (average: 755 m3/day), and a mean methane concentration of 60%. The methane gas was used to generate power in the plant and the amount of power generated by methane gas was highest in October (average of 1,200 kWh/day). This was equivalent to about 7% of the power consumed at the entire sludge treatment plant. The BOD/NH4-N of the activated sludge influent water was lower, compared to a case where there is no recycle flow, due to the recycle flow from the methane fermentation process. There was, therefore, a tendency for an increase in the amount of methanol charged into the secondary denitrification tank. However, the quality of the effluent was satisfactory (BOD< 10 mg/L, SS< 5 mg/L, and T-N< 25 mg/L). Study results indicated that it was possible to implement a full-scale plant for recovering organic waste.
NASA Technical Reports Server (NTRS)
1982-01-01
Liquid methane is beginning to become an energy alternative to expensive oil as a power source for automotive vehicles. Methane is the principal component of natural gas, costs less than half as much as gasoline, and its emissions are a lot cleaner than from gasoline or diesel engines. Beech Aircraft Corporation's Boulder Division has designed and is producing a system for converting cars and trucks to liquid methane operation. Liquid methane (LM) is a cryogenic fuel which must be stored at a temperature of 260 degrees below zero Fahrenheit. The LM system includes an 18 gallon fuel tank in the trunk and simple "under the hood" carburetor conversion equipment. Optional twin-fuel system allows operator to use either LM or gasoline fuel. Boulder Division has started deliveries for 25 vehicle conversions and is furnishing a liquid methane refueling station. Beech is providing instruction for Northwest Natural Gas, for conversion of methane to liquid state.
Heritability of methane emissions from dairy cows over a lactation measured on commercial farms.
Pszczola, M; Rzewuska, K; Mucha, S; Strabel, T
2017-11-01
Methane emission is currently an important trait in studies on ruminants due to its environmental and economic impact. Recent studies were based on short-time measurements on individual cows. As methane emission is a longitudinal trait, it is important to investigate its changes over a full lactation. In this study, we aimed to estimate the heritability of the estimated methane emissions from dairy cows using Fourier-transform infrared spectroscopy during milking in an automated milking system by implementing the random regression method. The methane measurements were taken on 485 Polish Holstein-Friesian cows at 2 commercial farms located in western Poland. The overall daily estimated methane emission was 279 g/d. Genetic variance fluctuated over the course of lactation around the average level of 1,509 (g/d), with the highest level, 1,866 (g/d), at the end of the lactation. The permanent environment variance values started at 2,865 (g/d) and then dropped to around 846 (g/d) at 100 d in milk (DIM) to reach the level of 2,444 (g/d) at the end of lactation. The residual variance was estimated at 2,620 (g/d). The average repeatability was 0.25. The heritability level fluctuated over the course of lactation, starting at 0.23 (SE 0.12) and then increasing to its maximum value of 0.3 (SE 0.08) at 212 DIM and ending at the level of 0.27 (SE 0.12). Average heritability was 0.27 (average SE 0.09). We have shown that estimated methane emission is a heritable trait and that the heritability level changes over the course of lactation. The observed changes and low genetic correlations between distant DIM suggest that it may be important to consider the period in which methane phenotypes are collected.
Method for removal of methane from coalbeds
Pasini, III, Joseph; Overbey, Jr., William K.
1976-01-01
A method for removing methane gas from underground coalbeds prior to mining the coal which comprises drilling at least one borehole from the surface into the coalbed. The borehole is started at a slant rather than directly vertically, and as it descends, a gradual curve is followed until a horizontal position is reached where the desired portion of the coalbed is intersected. Approaching the coalbed in this manner and fracturing the coalbed in the major natural fraction direction cause release of large amounts of the trapped methane gas.
Code of Federal Regulations, 2011 CFR
2011-07-01
... production rate at which the affected facility will be operated, or 180 days after the initial start-up, whichever date comes first. Each owner or operator shall either: (a) Reduce emissions of TOC (less methane and ethane) by 98 weight-percent, or to a TOC (less methane and ethane) concentration of 20 ppmv, on a...
NASA Technical Reports Server (NTRS)
Melcher, J. C.; Morehead, Robert L.
2014-01-01
The Project Morpheus liquid oxygen (LOX) / liquid methane rocket engines demonstrated acousticcoupled combustion instabilities during sea-level ground-based testing at the NASA Johnson Space Center (JSC) and Stennis Space Center (SSC). High-amplitude, 1T, 1R, 1T1R (and higher order) modes appear to be triggered by injector conditions. The instability occurred during the Morpheus-specific engine ignition/start sequence, and did demonstrate the capability to propagate into mainstage. However, the instability was never observed to initiate during mainstage, even at low power levels. The Morpheus main engine is a JSC-designed 5,000 lbf-thrust, 4:1 throttling, pressure-fed cryogenic engine using an impinging element injector design. Two different engine designs, named HD4 and HD5, and two different builds of the HD4 engine all demonstrated similar instability characteristics. Through the analysis of more than 200 hot fire tests on the Morpheus vehicle and SSC test stand, a relationship between ignition stability and injector/chamber pressure was developed. The instability has the distinct characteristic of initiating at high relative injection pressure drop (dP) at low chamber pressure (Pc); i.e., instabilities initiated at high dP/Pc at low Pc during the start sequence. The high dP/Pc during start results during the injector /chamber chill-in, and is enhanced by hydraulic flip in the injector orifice elements. Because of the fixed mixture ratio of the existing engine design (the main valves share a common actuator), it is not currently possible to determine if LOX or methane injector dP/Pc were individual contributors (i.e., LOX and methane dP/Pc typically trend in the same direction within a given test). The instability demonstrated initiation characteristic of starting at or shortly after methane injector chillin. Colder methane (e.g., sub-cooled) at the injector inlet prior to engine start was much more likely to result in an instability. A secondary effect of LOX sub-cooling was also possibly observed; greater LOX sub- cooling improved stability. Some tests demonstrated a low-amplitude 1L-1T instability prior to LOX injector chill-in. The Morpheus main engine also demonstrated chug instabilities during some engine shutdown sequences on the flight vehicle and SSC test stand. The chug instability was also infrequently observed during the startup sequence. The chug instabilities predictably initiated at low dP/Pc at low Pc. The chug instabilities were always self-limiting; startup chug instabilities terminated during throttle-up and shutdown chug instabilities decayed by shutdown termination.
Development of an advanced Sabatier CO2 reduction subsystem
NASA Technical Reports Server (NTRS)
Kleiner, G. N.; Cusick, R. J.
1981-01-01
A preprototype Sabatier CO2 reduction subsystem was successfully designed, fabricated and tested. The lightweight, quick starting (less than 5 minutes) reactor utlizes a highly active and physically durable methanation catalyst composed of ruthenium on alumina. The use of this improved catalyst permits a simple, passively controlled reactor design with an average lean component H2/CO2 conversion efficiency of over 99% over a range of H2/CO2 molar ratios of 1.8 to 5 while operating with process flows equivalent to a crew size of up to five persons. The subsystem requires no heater operation after start-up even during simulated 55 minute lightside/39 minute darkside orbital operation.
Characteristics of adapted hydrogenotrophic community during biomethanation.
Rachbauer, Lydia; Beyer, Reinhard; Bochmann, Günther; Fuchs, Werner
2017-10-01
The results presented in this study were carried out as concomitant experiments during the start-up and operation of a biomethanation unit to evaluate the effect of process parameters on carbon conversion, product formation (methane and acetate) and community composition. For that, two different samples were withdrawn from a trickle-bed reactor with immobilized enrichment culture of hydrogenotrophic methanogens adapted from sewage sludge. One sample was taken from the recirculation liquid during start-up phase while the other was withdrawn directly from the carrier material in the reactor. Elevated acid levels especially during start-up were shown to affect the overall carbon conversion. This effect was also seen during the acid tolerance testing reported here. Final acid concentrations of 1.6±0.3g/L resulted in a reduced conversion ratio of only 46%. Without acid addition complete conversion of CO 2 in the headspace was achieved. However, maximum methane production of 0.55±0.02mmol after 4days of incubation was monitored at moderate initial acetate concentration of 0.4g/L. In both analyzed inoculation materials Methanobacterium species were by far the most dominant Archaea with 21.8% in the recirculation liquid during start-up and 84.8% in the enrichment culture immobilized on the carrier material. The microbial composition of the two analyzed samples is in accordance with the results obtained for the carbon conversion and product formation. With approximately 50% of Bacteroidetes and Firmicutes present during reactor start-up the acetic acid production significantly contributed to the overall carbon conversion. In contrast, methane was produced almost exclusively in trials representing continuous operation where acetogenic bacteria accounted only up to 17.5%. In summary, the acid accumulation monitored during reactor start-up of a biomethanation unit is most likely to result from the microbial composition present. Nevertheless, complete adaptation to hydrogenotrophic conditions was proven to alter the consortium and yield methane as main product alongside high carbon conversion of up to 70.5±1.8%. Copyright © 2017 Elsevier B.V. All rights reserved.
Simple Recipes for Prebiotic Soup: A High School or Undergraduate Chemistry Laboratory
NASA Astrophysics Data System (ADS)
Martinez-Meeler, Marisol; Aljinovic, Nika; Swain, Dorothy
2003-06-01
A lab activity demonstrating Stanley Miller‘s prebiotic soup experiments is described. This lab activity, which uses only simple, readily available materials and equipment, would be suitable for use in a high school or introductory college chemistry class. The activity starts by asking students to consider some of the debated issues surrounding research into the chemical origins of life on Earth. It continues by having the students set up a simple apparatus that sends an electrical spark through a mixture of methane, ammonia, and water. The experiment concludes (the following week) by having students analyze their reaction products and design their own variation on the experiment.
Modeling natural wetlands: A new global framework built on wetland observations
NASA Astrophysics Data System (ADS)
Matthews, E.; Romanski, J.; Olefeldt, D.
2015-12-01
Natural wetlands are the world's largest methane (CH4) source, and their distribution and CH4 fluxes are sensitive to interannual and longer-term climate variations. Wetland distributions used in wetland-CH4 models diverge widely, and these geographic differences contribute substantially to large variations in magnitude, seasonality and distribution of modeled methane fluxes. Modeling wetland type and distribution—closely tied to simulating CH4 emissions—is a high priority, particularly for studies of wetlands and CH4 dynamics under past and future climates. Methane-wetland models either prescribe or simulate methane-producing areas (aka wetlands) and both approaches result in predictable over- and under-estimates. 1) Monthly satellite-derived inundation data include flooded areas that are not wetlands (e.g., lakes, reservoirs, and rivers), and do not identify non-flooded wetlands. 2) Models simulating methane-producing areas overwhelmingly rely on modeled soil moisture, systematically over-estimating total global area, with regional over- and under-estimates, while schemes to model soil-moisture typically cannot account for positive water tables (i.e., flooding). Interestingly, while these distinct hydrological approaches to identify wetlands are complementary, merging them does not provide critical data needed to model wetlands for methane studies. We present a new integrated framework for modeling wetlands, and ultimately their methane emissions, that exploits the extensive body of data and information on wetlands. The foundation of the approach is an existing global gridded data set comprising all and only wetlands, including vegetation information. This data set is augmented with data inter alia on climate, inundation dynamics, soil type and soil carbon, permafrost, active-layer depth, growth form, and species composition. We investigate this enhanced wetland data set to identify which variables best explain occurrence and characteristics of observed wetland ecosystems. The novelty of the new approach is that it starts from what we know about wetlands, builds ecosystem-specific models from these observations, and avoids known biases in current hydrology-based approaches to wetland definition in methane models.
Methane emissions from different coastal wetlands in New England, US
NASA Astrophysics Data System (ADS)
Wang, F.; Tang, J.; Kroeger, K. D.; Gonneea, M. E.
2017-12-01
According to the IPCC, methane have 25 times warming effect than CO2, and natural wetlands contribute 20-39 % to the global emission of methane. Although most of these methane was from inland wetlands, there was still large uncertain in the methane emissions in coastal wetlands. In the past three years, we have investigated methane emissions in coastal wetlands in MA, USA. Contrary to previous assumptions, we have observed relative larger methane flux in some salt marshes than freshwater wetlands. We further detect the methane source, and found that plant activities played an important role in methane flux, for example, the growth of S. aterniflora, the dominate plants in salt marsh, could enhance methane emission, while in an fresh water wetland that was dominated by cattail, plant activity oxided methane and reduced total flux. Phragmite, an invasive plant at brackish marsh, have the highest methane flux among all coastal wetland investigated. This study indicated that coastal wetland could still emit relatively high amount of methane even under high water salinity condiations, and plant activity played an important role in methane flux, and this role was highly species-specific.
Formate oxidation-driven calcium carbonate precipitation by Methylocystis parvus OBBP.
Ganendra, Giovanni; De Muynck, Willem; Ho, Adrian; Arvaniti, Eleni Charalampous; Hosseinkhani, Baharak; Ramos, Jose Angel; Rahier, Hubert; Boon, Nico
2014-08-01
Microbially induced carbonate precipitation (MICP) applied in the construction industry poses several disadvantages such asammonia release to the air and nitric acid production. An alternative MICP from calcium formate by Methylocystis parvus OBBP is presented here to overcome these disadvantages. To induce calcium carbonate precipitation, M. parvus was incubated at different calcium formate concentrations and starting culture densities. Up to 91.4% ± 1.6% of the initial calcium was precipitated in the methane-amended cultures compared to 35.1% ± 11.9% when methane was not added. Because the bacteria could only utilize methane for growth, higher culture densities and subsequently calcium removals were exhibited in the cultures when methane was added. A higher calcium carbonate precipitate yield was obtained when higher culture densities were used but not necessarily when more calcium formate was added. This was mainly due to salt inhibition of the bacterial activity at a high calcium formate concentration. A maximum 0.67 ± 0.03 g of CaCO3 g of Ca(CHOOH)2(-1) calcium carbonate precipitate yield was obtained when a culture of 10(9) cells ml(-1) and 5 g of calcium formate liter(-)1 were used. Compared to the current strategy employing biogenic urea degradation as the basis for MICP, our approach presents significant improvements in the environmental sustainability of the application in the construction industry.
Formate Oxidation-Driven Calcium Carbonate Precipitation by Methylocystis parvus OBBP
Ganendra, Giovanni; De Muynck, Willem; Ho, Adrian; Arvaniti, Eleni Charalampous; Hosseinkhani, Baharak; Ramos, Jose Angel; Rahier, Hubert
2014-01-01
Microbially induced carbonate precipitation (MICP) applied in the construction industry poses several disadvantages such as ammonia release to the air and nitric acid production. An alternative MICP from calcium formate by Methylocystis parvus OBBP is presented here to overcome these disadvantages. To induce calcium carbonate precipitation, M. parvus was incubated at different calcium formate concentrations and starting culture densities. Up to 91.4% ± 1.6% of the initial calcium was precipitated in the methane-amended cultures compared to 35.1% ± 11.9% when methane was not added. Because the bacteria could only utilize methane for growth, higher culture densities and subsequently calcium removals were exhibited in the cultures when methane was added. A higher calcium carbonate precipitate yield was obtained when higher culture densities were used but not necessarily when more calcium formate was added. This was mainly due to salt inhibition of the bacterial activity at a high calcium formate concentration. A maximum 0.67 ± 0.03 g of CaCO3 g of Ca(CHOOH)2−1 calcium carbonate precipitate yield was obtained when a culture of 109 cells ml−1 and 5 g of calcium formate liter−1 were used. Compared to the current strategy employing biogenic urea degradation as the basis for MICP, our approach presents significant improvements in the environmental sustainability of the application in the construction industry. PMID:24837386
Saga of coal bed methane, Ignacio Blanco gas field, Colorado
DOE Office of Scientific and Technical Information (OSTI.GOV)
Boyce, B.C.; Harr, C.L.; Burch, L.C.
1989-09-01
Prior to the 1977 discovery of the Cedar Hill Basal Fruitland pool (the first officially designated coal-bed methane field in the western US) 28.5 bcf of gas had been produced from Fruitland Formation coal seams in the Ignacio Blanco Fruitland-Pictured Cliffs field, Northern San Juan basin, Colorado. The discovery well for the field, Southern Ute D-1, was drilled and completed in 1951 on the Ignacio anticline, La Plata County, Colorado. Initial completion was attempted in the Pictured Cliffs Sandstone. The well was plugged back after making water from the Pictured Cliffs and was completed in the lower coal-bearing section ofmore » the Fruitland Formation. The well produced 487,333 mcf of gas in nine years and was abandoned in 1959 due to water encroachment. Additionally, 52 similarly completed Ignacio anticline Fruitland wells were abandoned by the early 1970s due to the nemesis of If it's starting to kick water, you're through. Under today's coal-bed methane technology and economics, Amoco has twinned 12 of the abandoned wells, drilled five additional wells, and is successfully dewatering and producing adsorbed methane from previously depleted coal sections of the Ignacio structure. Field-wide drilling activity in 1988 exceeded all previous annual levels, with coal-seam degasification projects leading the resurgence. Drilling and completion forecasts for 1989 surpass 1988 levels by 50%.« less
NASA Technical Reports Server (NTRS)
Moore, Jeffrey
2012-01-01
Titan may have acquired its massive atmosphere relatively recently in solar system history. The warming sun may have been key to generating Titan's atmosphere over time, starting from a thin atmosphere with condensed surface volatiles like Triton, with increased luminosity releasing methane, and then large amounts of nitrogen (perhaps suddenly), into the atmosphere. This thick atmosphere, initially with much more methane than at present, resulted in global fluvial erosion that has over time retreated towards the poles with the removal of methane from the atmosphere. Basement rock, as manifested by bright, rough, ridges, scarps, crenulated blocks, or aligned massifs, mostly appears within 30 degrees of the equator. This landscape was intensely eroded by fluvial processes as evidenced by numerous valley systems, fan-like depositional features and regularly-spaced ridges (crenulated terrain). Much of this bedrock landscape, however, is mantled by dunes, suggesting that fluvial erosion no longer dominates in equatorial regions. High midlatitude regions on Titan exhibit dissected sedimentary plains at a number of localities, suggesting deposition (perhaps by sediment eroded from equatorial regions) followed by erosion. The polar regions are mainly dominated by deposits of fluvial and lacustrine sediment. Fluvial processes are active in polar areas as evidenced by alkane lakes and occasional cloud cover.
Reversing methanogenesis to capture methane for liquid biofuel precursors
DOE Office of Scientific and Technical Information (OSTI.GOV)
Soo, Valerie W. C.; McAnulty, Michael J.; Tripathi, Arti
Energy from remote methane reserves is transformative; however, unintended release of this potent greenhouse gas makes it imperative to convert methane efficiently into more readily transported biofuels. No pure microbial culture that grows on methane anaerobically has been isolated, despite that methane capture through anaerobic processes is more efficient than aerobic ones. Here we engineered the archaeal methanogen Methanosarcina acetivorans to grow anaerobically on methane as a pure culture and to convert methane into the biofuel precursor acetate. To capture methane, we cloned the enzyme methyl-coenzyme M reductase (Mcr) from an unculturable organism, anaerobic methanotrophic archaeal population 1 (ANME-1) frommore » a Black Sea mat, into M. acetivorans to effectively run methanogenesis in reverse. Starting with low-density inocula, M. acetivorans cells producing ANME-1 Mcr consumed up to 9 ± 1 % of methane (corresponding to 109 ± 12 µmol of methane) after 6 weeks of anaerobic growth on methane and utilized 10 mM FeCl 3 as an electron acceptor. Accordingly, increases in cell density and total protein were observed as cells grew on methane in a biofilm on solid FeCl 3. When incubated on methane for 5 days, high-densities of ANME-1 Mcr-producing M. acetivorans cells consumed 15 ± 2 % methane (corresponding to 143 ± 16 µmol of methane), and produced 10.3 ± 0.8 mM acetate (corresponding to 52 ± 4 µmol of acetate). We further confirmed the growth on methane and acetate production using 13C isotopic labeling of methane and bicarbonate coupled with nuclear magnetic resonance and gas chromatography/mass spectroscopy, as well as RNA sequencing. Lastly, we anticipate that our metabolically-engineered strain will provide insights into how methane is cycled in the environment by Archaea as well as will possibly be utilized to convert remote sources of methane into more easily transported biofuels via acetate.« less
Reversing methanogenesis to capture methane for liquid biofuel precursors
Soo, Valerie W. C.; McAnulty, Michael J.; Tripathi, Arti; ...
2016-01-14
Energy from remote methane reserves is transformative; however, unintended release of this potent greenhouse gas makes it imperative to convert methane efficiently into more readily transported biofuels. No pure microbial culture that grows on methane anaerobically has been isolated, despite that methane capture through anaerobic processes is more efficient than aerobic ones. Here we engineered the archaeal methanogen Methanosarcina acetivorans to grow anaerobically on methane as a pure culture and to convert methane into the biofuel precursor acetate. To capture methane, we cloned the enzyme methyl-coenzyme M reductase (Mcr) from an unculturable organism, anaerobic methanotrophic archaeal population 1 (ANME-1) frommore » a Black Sea mat, into M. acetivorans to effectively run methanogenesis in reverse. Starting with low-density inocula, M. acetivorans cells producing ANME-1 Mcr consumed up to 9 ± 1 % of methane (corresponding to 109 ± 12 µmol of methane) after 6 weeks of anaerobic growth on methane and utilized 10 mM FeCl 3 as an electron acceptor. Accordingly, increases in cell density and total protein were observed as cells grew on methane in a biofilm on solid FeCl 3. When incubated on methane for 5 days, high-densities of ANME-1 Mcr-producing M. acetivorans cells consumed 15 ± 2 % methane (corresponding to 143 ± 16 µmol of methane), and produced 10.3 ± 0.8 mM acetate (corresponding to 52 ± 4 µmol of acetate). We further confirmed the growth on methane and acetate production using 13C isotopic labeling of methane and bicarbonate coupled with nuclear magnetic resonance and gas chromatography/mass spectroscopy, as well as RNA sequencing. Lastly, we anticipate that our metabolically-engineered strain will provide insights into how methane is cycled in the environment by Archaea as well as will possibly be utilized to convert remote sources of methane into more easily transported biofuels via acetate.« less
Effect of process design and operating parameters on aerobic methane oxidation in municipal WWTPs.
Daelman, Matthijs R J; Van Eynde, Tamara; van Loosdrecht, Mark C M; Volcke, Eveline I P
2014-12-01
Methane is a potent greenhouse gas and its emission from municipal wastewater treatment plants (WWTPs) should be prevented. One way to do this is to promote the biological conversion of dissolved methane over stripping in aeration tanks. In this study, the well-established Activated Sludge Model n°1 (ASM1) and Benchmark Simulation Model n°1 (BSM1) were extended to study the influence of process design and operating parameters on biological methane oxidation. The aeration function used in BSM 1 was upgraded to more accurately describe gas-liquid transfer of oxygen and methane in aeration tanks equipped with subsurface aeration. Dissolved methane could be effectively removed in an aeration tank at an aeration rate that is in agreement with optimal effluent quality. Subsurface bubble aeration proved to be better than surface aeration, while a CSTR configuration was superior to plug flow conditions in avoiding methane emissions. The conversion of methane in the activated sludge tank benefits from higher methane concentrations in the WWTP's influent. Finally, if an activated sludge tank is aerated with methane containing off-gas, a limited amount of methane is absorbed and converted in the mixed liquor. This knowledge helps to stimulate the methane oxidizing capacity of activated sludge in order to abate methane emissions from wastewater treatment to the atmosphere. Copyright © 2014 Elsevier Ltd. All rights reserved.
Sancho Navarro, Silvia; Cimpoia, Ruxandra; Bruant, Guillaume; Guiot, Serge R
2016-01-01
Syngas generated by thermal gasification of biomass or coal can be steam reformed and purified into methane, which could be used locally for energy needs, or re-injected in the natural gas grid. As an alternative to chemical catalysis, the main components of the syngas (CO, CO2, and H2) can be used as substrates by a wide range of microorganisms, to be converted into gas biofuels, including methane. This study evaluates the carboxydotrophic (CO-consuming) methanogenic potential present in an anaerobic sludge from an upflow anaerobic sludge bed (UASB) reactor treating waste water, and elucidates the CO conversion routes to methane at 35 ± 3°C. Kinetic activity tests under CO at partial pressures (pCO) varying from 0.1 to 1.5 atm (0.09-1.31 mmol/L in the liquid phase) showed a significant carboxydotrophic activity potential for growing conditions on CO alone. A maximum methanogenic activity of 1 mmol CH4 per g of volatile suspended solid and per day was achieved at 0.2 atm of CO (0.17 mmol/L), and then the rate decreased with the amount of CO supplied. The intermediary metabolites such as acetate, H2, and propionate started to accumulate at higher CO concentrations. Inhibition experiments with 2-bromoethanesulfonic acid (BES), fluoroacetate, and vancomycin showed that in a mixed culture CO was converted mainly to acetate by acetogenic bacteria, which was further transformed to methane by acetoclastic methanogens, while direct methanogenic CO conversion was negligible. Methanogenesis was totally blocked at high pCO in the bottles (≥1 atm). However it was possible to achieve higher methanogenic potential under a 100% CO atmosphere after acclimation of the sludge to CO. This adaptation to high CO concentrations led to a shift in the archaeal population, then dominated by hydrogen-utilizing methanogens, which were able to take over acetoclastic methanogens, while syntrophic acetate oxidizing (SAO) bacteria oxidized acetate into CO2 and H2. The disaggregation of the granular sludge showed a negative impact on their methanogenic activity, confirming that the acetoclastic methanogens were the most sensitive to CO, and a contrario, the advantage of using granular sludge for further development toward large-scale methane production from CO-rich syngas.
Sancho Navarro, Silvia; Cimpoia, Ruxandra; Bruant, Guillaume; Guiot, Serge R.
2016-01-01
Syngas generated by thermal gasification of biomass or coal can be steam reformed and purified into methane, which could be used locally for energy needs, or re-injected in the natural gas grid. As an alternative to chemical catalysis, the main components of the syngas (CO, CO2, and H2) can be used as substrates by a wide range of microorganisms, to be converted into gas biofuels, including methane. This study evaluates the carboxydotrophic (CO-consuming) methanogenic potential present in an anaerobic sludge from an upflow anaerobic sludge bed (UASB) reactor treating waste water, and elucidates the CO conversion routes to methane at 35 ± 3°C. Kinetic activity tests under CO at partial pressures (pCO) varying from 0.1 to 1.5 atm (0.09–1.31 mmol/L in the liquid phase) showed a significant carboxydotrophic activity potential for growing conditions on CO alone. A maximum methanogenic activity of 1 mmol CH4 per g of volatile suspended solid and per day was achieved at 0.2 atm of CO (0.17 mmol/L), and then the rate decreased with the amount of CO supplied. The intermediary metabolites such as acetate, H2, and propionate started to accumulate at higher CO concentrations. Inhibition experiments with 2-bromoethanesulfonic acid (BES), fluoroacetate, and vancomycin showed that in a mixed culture CO was converted mainly to acetate by acetogenic bacteria, which was further transformed to methane by acetoclastic methanogens, while direct methanogenic CO conversion was negligible. Methanogenesis was totally blocked at high pCO in the bottles (≥1 atm). However it was possible to achieve higher methanogenic potential under a 100% CO atmosphere after acclimation of the sludge to CO. This adaptation to high CO concentrations led to a shift in the archaeal population, then dominated by hydrogen-utilizing methanogens, which were able to take over acetoclastic methanogens, while syntrophic acetate oxidizing (SAO) bacteria oxidized acetate into CO2 and H2. The disaggregation of the granular sludge showed a negative impact on their methanogenic activity, confirming that the acetoclastic methanogens were the most sensitive to CO, and a contrario, the advantage of using granular sludge for further development toward large-scale methane production from CO-rich syngas. PMID:27536280
Dynamics of Permafrost Associated Methane Hydrate in Response to Climate Change
NASA Astrophysics Data System (ADS)
You, K.; Flemings, P. B.
2014-12-01
The formation and melting of methane hydrate and ice are intertwined in permafrost regions. A shortage of methane supply leads to formation of hydrate only at depth, below the base of permafrost. We consider a system with the ground surface initially at 0 oC with neither ice nor hydrate present. We abruptly decrease the temperature from 0 to -10 oC to simulate the effect of marine regression/ global cooling. A low methane supply rate of 0.005 kg m-2 yr-1 from depth leads to distinct ice and hydrate layers: a 100 m continuous hydrate layer is present beneath 850 m at 80 k.y.. However, a high methane supply rate of 0.1 kg m-2 yr-1 leads to 50 m ice-bonded methane hydrate at the base of permafrost, and the hydrate layer distributes between the depth of 350 and 700 m at 80 k.y.. We apply our model to illuminate future melting of hydrate at Mallik, a known Arctic hydrate accumulation. We assume a 600 m thick ice saturated (average 90%) layer extending downward from the ground surface. We increase the surface temperature linearly from -6 to 0 oC for 300 yr and then keep the surface temperature at 0 oC to reflect future climate warming caused by doubling of CO2. Hydrate melting is initiated at the base of the hydrate layer after 15 k.y.. Methane gas starts to vent to the atmosphere at 38 k.y. with an average flux of ~ 0.35 g m-2 yr-1. If the 600 m thick average ice saturation is decreased to half (45%) (or to zero), methane gas starts to vent to the atmosphere at 29 k.y. (or at 20 k.y.) with the same average flux. These results are found by a newly-developed fully-coupled multiphase multicomponent fluid flow and heat transport model. Our thermodynamic equilibrium-based model emphasizes the role of salinity in both ice and hydrate dynamics.
Observations of mass fractionation of noble gases in synthetic methane hydrate
Hunt, Andrew G.; Pohlman, John; Stern, Laura A.; Ruppel, Carolyn D.; Moscati, Richard J.; Landis, Gary P.; Pinkston, John C.
2011-01-01
As a consequence of contemporary or longer term (since 15 ka) climate warming, gas hydrates in some settings are presently dissociating and releasing methane and other gases to the oceanatmosphere system. A key challenge in assessing the susceptibility of gas hydrates to warming climate is the lack of a technique able to distinguish between methane recently released from gas hydrates and methane emitted from leaky thermogenic reservoirs, shallow sublake and subseafloor sediments, coalbeds, and other sources. Carbon and deuterium stable isotopic data provide only a first-order characterization of methane sources, while gas hydrate can sequester any type of methane. Here, we investigate the possibility of exploiting the pattern of noble gas fractionation within the gas hydrate lattice to fingerprint methane released from gas hydrates. Starting with synthetic gas hydrate formed under careful laboratory conditions, we document complex noble gas fractionation patterns in the gases liberated during dissociation and explore the effects of aging and storage (e.g., in liquid nitrogen), as well as sampling and preservation procedures. The laboratory results confirm a unique noble gas fractionation pattern for gas hydrates, one that shows promise in evaluating modern natural gas seeps for a signature associated with gas hydrate dissociation.
The impact of compaction and leachate recirculation on waste degradation in simulated landfills.
Ko, Jae Hac; Yang, Fan; Xu, Qiyong
2016-07-01
This study investigated the impact of compaction and leachate recirculation on anaerobic degradation of municipal solid waste (MSW) at different methane formation phases. Two stainless steel lysimeters, C1 and C2, were constructed by equipping a hydraulic cylinder to apply pressure load (42kPs) on the MSW. When MSW started to produce methane, C1 was compacted, but C2 was compacted when the methane production rate declined from the peak generation rate. Methane production of C1was inhibited by the compaction and resulted in producing a total of 106L methane (44L/kgVS). However, the compaction in C2 promoted MSW degradation resulting in producing a total of 298L methane (125L/kgVS). The concentrations of volatile fatty acids and chemical oxygen demand showed temporary increases, when pressure load was applied. It was considered that the increased substrate accessibility within MSW by compaction could cause either the inhibition or the enhancement of methane production, depending the tolerability of methanogens on the acidic inhibition. Leachate recirculation also gave positive effects on methane generation from wet waste in the decelerated methanogenic phase by increasing mass transfer and the concentrations of volatile fatty acids. Copyright © 2016 Elsevier Ltd. All rights reserved.
NASA Technical Reports Server (NTRS)
Melcher, John C.; Morehead, Robert L.
2014-01-01
The project Morpheus liquid oxygen (LOX) / liquid methane (LCH4) main engine is a Johnson Space Center (JSC) designed 5,000 lbf-thrust, 4:1 throttling, pressure-fed cryogenic engine using an impinging element injector design. The engine met or exceeded all performance requirements without experiencing any in- ight failures, but the engine exhibited acoustic-coupled combustion instabilities during sea-level ground-based testing. First tangential (1T), rst radial (1R), 1T1R, and higher order modes were triggered by conditions during the Morpheus vehicle derived low chamber pressure startup sequence. The instability was never observed to initiate during mainstage, even at low power levels. Ground-interaction acoustics aggravated the instability in vehicle tests. Analysis of more than 200 hot re tests on the Morpheus vehicle and Stennis Space Center (SSC) test stand showed a relationship between ignition stability and injector/chamber pressure. The instability had the distinct characteristic of initiating at high relative injection pressure drop at low chamber pressure during the start sequence. Data analysis suggests that the two-phase density during engine start results in a high injection velocity, possibly triggering the instabilities predicted by the Hewitt stability curves. Engine ignition instability was successfully mitigated via a higher-chamber pressure start sequence (e.g., 50% power level vs 30%) and operational propellant start temperature limits that maintained \\cold LOX" and \\warm methane" at the engine inlet. The main engine successfully demonstrated 4:1 throttling without chugging during mainstage, but chug instabilities were observed during some engine shutdown sequences at low injector pressure drop, especially during vehicle landing.
Yap, S D; Astals, S; Jensen, P D; Batstone, D J; Tait, S
2017-06-01
Batch solid-phase anaerobic digestion is a technology for sustainable on-farm treatment of solid residues, but is an emerging technology that is yet to be optimised with respect to start-up and inoculation. In the present study, spent bedding from two piggeries (site A and B) were batch digested at total solids (TS) concentration of 5, 10 and 20% at mesophilic (37°C) and thermophilic (55°C) temperatures, without adding an external inoculum. The results showed that the indigenous microbial community present in spent bedding was able to recover the full methane potential of the bedding (140±5 and 227±6L CH 4 kgVS fed -1 for site A and B, respectively), but longer treatment times were required than for digestion with an added external inoculum. Nonetheless, at high solid loadings (i.e. TS level>10%), the digestion performance was affected by chemical inhibition due to ammonia and/or humic acid. Thermophilic temperatures did not influence digestion performance but did increase start-up failure risk. Further, inoculation of residues from the batch digestion to subsequent batch enhanced start-up and achieved full methane potential recovery of the bedding. Inoculation with liquid residue (leachate) was preferred over a solid residue, to preserve treatment capacity for fresh substrate. Overall, the study highlighted that indigenous microbial community in the solid manure residue was capable of recovering full methane potential and that solid-phase digestion was ultimately limited by chemical inhibition rather than lack of suitable microbial community. Copyright © 2017 Elsevier Ltd. All rights reserved.
Mechanistic insights into heterogeneous methane activation
Latimer, Allegra A.; Aljama, Hassan; Kakekhani, Arvin; ...
2017-01-11
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 tomore » 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.« less
Mechanistic insights into heterogeneous methane activation
DOE Office of Scientific and Technical Information (OSTI.GOV)
Latimer, Allegra A.; Aljama, Hassan; Kakekhani, Arvin
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 tomore » 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.« less
Copper enhances the activity and salt resistance of mixed methane-oxidizing communities.
van der Ha, David; Hoefman, Sven; Boeckx, Pascal; Verstraete, Willy; Boon, Nico
2010-08-01
Effluents of anaerobic digesters are an underestimated source of greenhouse gases, as they are often saturated with methane. A post-treatment with methane-oxidizing bacterial consortia could mitigate diffuse emissions at such sites. Semi-continuously fed stirred reactors were used as model systems to characterize the influence of the key parameters on the activity of these mixed methanotrophic communities. The addition of 140 mg L(-1) NH (4) (+) -N had no significant influence on the activity nor did a temperature increase from 28 degrees C to 35 degrees C. On the other hand, addition of 0.64 mg L(-1) of copper(II) increased the methane removal rate by a factor of 1.5 to 1.7 since the activity of particulate methane monooxygenase was enhanced. The influence of different concentrations of NaCl was also tested, as effluents of anaerobic digesters often contain salt levels up to 10 g NaCl L(-1). At a concentration of 11 g NaCl L(-1), almost no methane-oxidizing activity was observed in the reactors without copper addition. Yet, reactors with copper addition exhibited a sustained activity in the presence of NaCl. A colorimetric test based on naphthalene oxidation showed that soluble methane monooxygenase was inhibited by copper, suggesting that the particulate methane monooxygenase was the active enzyme and thus more salt resistant. The results obtained demonstrate that the treatment of methane-saturated effluents, even those with increased ammonium (up to 140 mg L(-1) NH (4) (+) -N) and salt levels, can be mitigated by implementation of methane-oxidizing microbial consortia.
A modeling study of methane hydrate decomposition in contact with the external surface of zeolites.
Smirnov, Konstantin S
2017-08-30
The behavior of methane hydrate (MH) enclosed between the (010) surfaces of the silicalite-1 zeolite was studied by means of molecular dynamics simulations at temperatures of 150 and 250 K. Calculations reveal that the interaction with the hydrophilic surface OH groups destabilizes the clathrate structure of hydrate. While MH mostly conserves the structure in the simulation at the low temperature, thermal motion at the high temperature breaks the fragilized cages of H-bonded water molecules, thus leading to the release of methane. The dissociation proceeds in a layer-by-layer manner starting from the outer parts of the MH slab until complete hydrate decomposition. The released CH 4 molecules are absorbed by the microporous solid, whereas water is retained at the surfaces of hydrophobic silicalite and forms a meniscus in the interlayer space. Methane uptake reaches 70% of the silicalite sorption capacity. The energy necessary for the endothermic MH dissociation is supplied by the exothermic methane absorption by the zeolite.
Zhou, Xu; Wang, Qilin; Jiang, Guangming
2015-04-01
Methane production from anaerobic digestion of waste activated sludge (WAS) is limited by the slow hydrolysis rate and/or poor methane potential of WAS. This study presents a novel pre-treatment strategy based on indigenous iron (in WAS) activated peroxidation to enhance methane production from WAS. Pre-treatment of WAS for 30 min at 50mg H2O2/g total solids (dry weight) and pH 2.0 (iron concentration in WAS was 7 mg/g TS) substantially enhanced WAS solubilization. Biochemical methane potential tests demonstrated that methane production was improved by 10% at a digestion time of 16d after incorporating the indigenous iron activated peroxidation pre-treatment. Model-based analysis indicated that indigenous iron activated peroxidation pre-treatment improved the methane potential by 13%, whereas the hydrolysis rate was not significantly affected. The economic analysis showed that the proposed pre-treatment method can save the cost by $112,000 per year in a treatment plant with a population equivalent of 300,000. Copyright © 2015 Elsevier Ltd. All rights reserved.
Microbial diversity and dynamics during methane production from municipal solid waste
DOE Office of Scientific and Technical Information (OSTI.GOV)
Bareither, Christopher A., E-mail: christopher.bareither@colostate.edu; Geological Engineering, University of Wisconsin-Madison, Madison, WI 53706; Wolfe, Georgia L., E-mail: gwolfe@wisc.edu
2013-10-15
Highlights: ► Similar bacterial communities developed following different start-up operation. ► Total methanogens in leachate during the decelerated methane phase reflected overall methane yield. ► Created correlations between methanogens, methane yield, and available substrate. ► Predominant bacteria identified with syntrophic polysaccharide degraders. ► Hydrogenotrophic methanogens were dominant in the methane generation process. - Abstract: The objectives of this study were to characterize development of bacterial and archaeal populations during biodegradation of municipal solid waste (MSW) and to link specific methanogens to methane generation. Experiments were conducted in three 0.61-m-diameter by 0.90-m-tall laboratory reactors to simulate MSW bioreactor landfills. Pyrosequencing ofmore » 16S rRNA genes was used to characterize microbial communities in both leachate and solid waste. Microbial assemblages in effluent leachate were similar between reactors during peak methane generation. Specific groups within the Bacteroidetes and Thermatogae phyla were present in all samples and were particularly abundant during peak methane generation. Microbial communities were not similar in leachate and solid fractions assayed at the end of reactor operation; solid waste contained a more abundant bacterial community of cellulose-degrading organisms (e.g., Firmicutes). Specific methanogen populations were assessed using quantitative polymerase chain reaction. Methanomicrobiales, Methanosarcinaceae, and Methanobacteriales were the predominant methanogens in all reactors, with Methanomicrobiales consistently the most abundant. Methanogen growth phases coincided with accelerated methane production, and cumulative methane yield increased with increasing total methanogen abundance. The difference in methanogen populations and corresponding methane yield is attributed to different initial cellulose and hemicellulose contents of the MSW. Higher initial cellulose and hemicellulose contents supported growth of larger methanogen populations that resulted in higher methane yield.« less
Production of Methane and Water from Crew Plastic Waste
NASA Technical Reports Server (NTRS)
Captain, Janine; Santiago, Eddie; Parrish, Clyde; Strayer, Richard F.; Garland, Jay L.
2008-01-01
Recycling is a technology that will be key to creating a self sustaining lunar outpost. The plastics used for food packaging provide a source of material that could be recycled to produce water and methane. The recycling of these plastics will require some additional resources that will affect the initial estimate of starting materials that will have to be transported from earth, mainly oxygen, energy and mass. These requirements will vary depending on the recycling conditions. The degredation products of these plastics will vary under different atmospheric conditions. An estimate of the the production rate of methane and water using typical ISRU processes along with the plastic recycling will be presented.
NASA Astrophysics Data System (ADS)
Hatzenpichler, R.; Connon, S. A.; Goudeau, D.; Malmstrom, R.; Woyke, T.; Orphan, V. J.
2015-12-01
Within the past few years, great progress has been made in tapping the genomes of individual cells separated from environmental samples. Unfortunately, however, most often these efforts have been target blind, as they did not pre-select for taxa of interest or focus on metabolically active cells that could be considered key species of the system at the time. This problem is particularly pronounced in low-turnover systems such as deep sea sediments. In an effort to tap the genetic potential hidden within functionally active cells, we have recently developed an approach for the in situ fluorescent tracking of protein synthesis in uncultured cells via bioorthogonal non-canonical amino acid-tagging (BONCAT). This technique depends on the incorporation of synthetic amino acids that carry chemically modifiable tags into newly made proteins, which later can be visualized via click chemistry-mediated fluorescence-labeling. BONCAT is thus able to specifically target proteins that have been expressed in reaction to an experimental condition. We are particularly interested in using BONCAT to understand the functional potential of slow-growing syntrophic consortia of anaerobic methanotrophic archaea and sulfate-reducing bacteria which together catalyze the anaerobic oxidation of methane (AOM) in marine methane seeps. In order to specifically target consortia that are active under varying environmental regimes, we are studying different subpopulations of these inter-domain consortia via a combination of BONCAT with rRNA-targeted FISH. We then couple the BONCAT-enabled staining of active consortia with their separation from inactive members of the community via fluorescence-activated cell-sorting (FACS) and metagenomic sequencing of individual consortia. Using this approach, we were able to identify previously unrecognized AOM-partnerships. By comparing the mini-metagenomes obtained from individual consortia with each other we are starting to gain a more hollistic understanding of the genetic similarities and niche-determining characteristics of a range of functional and taxonomic clades of AOM-consortia.
NASA Astrophysics Data System (ADS)
Qi, Wenjie; Ran, Jingyu; Zhang, Zhien; Niu, Juntian; Zhang, Peng; Fu, Lijuan; Hu, Bo; Li, Qilai
2018-03-01
Density functional theory combined with kinetic models were used to probe different kinetics consequences by which methane activation on different oxygen chemical potential surfaces as oxygen pressure increased. The metallic oxide → metal transformation temperature of Pd-Pt catalysts increased with the increase of the Pd content or/and O2 pressure. The methane conversion rate on Pt catalyst increased and then decreased to a constant value when increasing the O2 pressure, and Pd catalyst showed a poor activity performance in the case of low O2 pressure. Moreover, its activity increased as the oxygen chemical potential for O2 pressure increased in the range of 2.5-10 KPa. For metal clusters, the Csbnd H bond and Odbnd O bond activation steps occurred predominantly on *-* site pairs. The methane conversion rate was determined by O2 pressure because the adsorbed O atoms were rapidly consumed by other adsorbed species in this kinetic regime. As the O2 pressure increased, the metallic active sites for methane activation were decreased and there was no longer lack of adsorbed O atoms, resulting in the decrease of the methane conversion rate. Furthermore, when the metallic surfaces were completely covered by adsorbed oxygen atoms at higher oxygen chemical potentials, Pt catalyst showed a poor activity due to a high Csbnd H bond activation barrier on O*sbnd O*. In the case of high O2 pressure, Pd atoms preferred to segregate to the active surface of Pd-Pt catalysts, leading to the formation of PdO surfaces. The increase of Pd segregation promoted a subsequent increase in active sites and methane conversion rate. The PdO was much more active than metallic and O* saturated surfaces for methane activation, inferred from the theory and experimental study. Pd-rich bimetallic catalyst (75% molar Pd) showed a dual high methane combustion activity on O2-poor and O2-rich conditions.
Hunt, Andrew G.; Stern, Laura; Pohlman, John W.; Ruppel, Carolyn; Moscati, Richard J.; Landis, Gary P.
2013-01-01
As a consequence of contemporary or longer term (since 15 ka) climate warming, gas hydrates in some settings may presently be dissociating and releasing methane and other gases to the ocean-atmosphere system. A key challenge in assessing the impact of dissociating gas hydrates on global atmospheric methane is the lack of a technique able to distinguish between methane recently released from gas hydrates and methane emitted from leaky thermogenic reservoirs, shallow sediments (some newly thawed), coal beds, and other sources. Carbon and deuterium stable isotopic fractionation during methane formation provides a first-order constraint on the processes (microbial or thermogenic) of methane generation. However, because gas hydrate formation and dissociation do not cause significant isotopic fractionation, a stable isotope-based hydrate-source determination is not possible. Here, we investigate patterns of mass-dependent noble gas fractionation within the gas hydrate lattice to fingerprint methane released from gas hydrates. Starting with synthetic gas hydrate formed under laboratory conditions, we document complex noble gas fractionation patterns in the gases liberated during dissociation and explore the effects of aging and storage (e.g., in liquid nitrogen), as well as sampling and preservation procedures. The laboratory results confirm a unique noble gas fractionation pattern for gas hydrates, one that shows promise in evaluating modern natural gas seeps for a signature associated with gas hydrate dissociation.
Chemical markers of possible hot spots on Mars
NASA Astrophysics Data System (ADS)
Wong, Ah-San; Atreya, Sushil K.; Encrenaz, Thérèse
2003-04-01
Although there is no evidence of active volcanism on Mars today, ``localized'' outgassing sources, the hot spots, may not be ruled out. If outgassing does occur somewhere on Mars, water, carbon dioxide, sulfur species, methane, and to a lesser extent, halogens would be the likely molecules of outgassing, based on terrestrial analogs. The sulfur species, methane, and halogens have not been detected in the Martian atmosphere, but the observations were averaged over large areas, which could result in substantial dilution in abundances. If the interpretation of certain Mars Global Surveyor images indicating recent ground water seepage and surface runoff [Malin and Edgett, 2000] is correct, it may imply that Mars could still be active internally in some places from time to time, and outgassing of the abovementioned species may occur with or without the water seepage. Moreover, if the tentative detection of formaldehyde (CH2O) in the equatorial region of Mars [Korablev et al., 1993] is confirmed by future observations, it would imply at least local outgassing of methane, whose oxidation results in the formation of CH2O. Considering the possibility of outgassing from some localized hot spots, we have developed a one-dimensional photochemical model that includes methane (CH4), sulfur dioxide (SO2), and hydrogen sulfide (H2S), starting with their current ``global average'' upper limits of 0.02, 0.1, and 0.1 ppm at the surface, respectively, and then progressively increasing their abundances above possible hot spots. We find that the introduction of methane into the Martian atmosphere results in the formation of mainly formaldehyde, methyl alcohol (CH3OH), and ethane (C2H6), whereas the introduction of the sulfur species produces mainly sulfur monoxide (SO) and sulfuric acid (H2SO4). The effect of outgassed halogens on the Martian atmosphere is found to be negligible. Depending upon the flux of outgassed molecules from possible hot spots, some of these species and the resulting new molecules may be detectable locally, either by remote sensing or in situ measurements.
Yao, Yiqing; Luo, Yang; Li, Tian; Yang, Yingxue; Sheng, Hongmei; Virgo, Nolan; Xiang, Yun; Song, Yuan; Zhang, Hua; An, Lizhe
2014-01-01
Solid-state anaerobic digestion (SS-AD) was initially adopted for the treatment of municipal solid waste. Recently, SS-AD has been increasingly applied to treat lignocellulosic biomass, such as agricultural and forestry residues. However, studies on the SS-AD process are few. In this study, the process performance and methane yield from SS-AD of alkaline-pretreated poplar processing residues (PPRs) were investigated using the properties of soil, such as buffering capacity and nutritional requirements. The results showed that the lignocellulosic structures of the poplar sample were effectively changed by NaOH pretreatment, as indicated by scanning electron microscopy and Fourier transform infrared spectra analysis. The start-up was markedly hastened, and the process stability was enhanced. After NaOH pretreatment, the maximum methane yield (96.1 L/kg volatile solids (VS)) was obtained under a poplar processing residues-to-soil sample (P-to-S) ratio of 2.5:1, which was 29.9% and 36.1% higher than that of PPRs (74.0 L/kg VS) and that of experiments without NaOH pretreatment (70.6 L/kg VS), respectively. During steady state, the increase in the methane content of the experiment with a P-to-S ratio of 2.5:1 was 4.4 to 50.9% higher than that of the PPRs. Degradation of total solids and volatile solids ranged from 19.3 to 33.0% and from 34.9 to 45.9%, respectively. The maximum reductions of cellulose and hemicellulose were 52.6% and 42.9%, respectively, which were in accordance with the maximal methane yield. T 80 for the maximum methane yield for the experiments with NaOH pretreatment was 11.1% shorter than that for the PPRs. Pretreatment with NaOH and addition of soil led to a significant improvement in the process performance and the methane yield of SS-AD of PPRs. The changes in lignocellulosic structures induced by NaOH pretreatment led to an increase in methane yield. For the purpose of practical applications, SS-AD with soil addition is a convenient, economical, and practical technique.
Dekas, Anne E; Connon, Stephanie A; Chadwick, Grayson L; Trembath-Reichert, Elizabeth; Orphan, Victoria J
2016-01-01
To characterize the activity and interactions of methanotrophic archaea (ANME) and Deltaproteobacteria at a methane-seeping mud volcano, we used two complimentary measures of microbial activity: a community-level analysis of the transcription of four genes (16S rRNA, methyl coenzyme M reductase A (mcrA), adenosine-5′-phosphosulfate reductase α-subunit (aprA), dinitrogenase reductase (nifH)), and a single-cell-level analysis of anabolic activity using fluorescence in situ hybridization coupled to nanoscale secondary ion mass spectrometry (FISH-NanoSIMS). Transcript analysis revealed that members of the deltaproteobacterial groups Desulfosarcina/Desulfococcus (DSS) and Desulfobulbaceae (DSB) exhibit increased rRNA expression in incubations with methane, suggestive of ANME-coupled activity. Direct analysis of anabolic activity in DSS cells in consortia with ANME by FISH-NanoSIMS confirmed their dependence on methanotrophy, with no 15NH4+ assimilation detected without methane. In contrast, DSS and DSB cells found physically independent of ANME (i.e., single cells) were anabolically active in incubations both with and without methane. These single cells therefore comprise an active ‘free-living' population, and are not dependent on methane or ANME activity. We investigated the possibility of N2 fixation by seep Deltaproteobacteria and detected nifH transcripts closely related to those of cultured diazotrophic Deltaproteobacteria. However, nifH expression was methane-dependent. 15N2 incorporation was not observed in single DSS cells, but was detected in single DSB cells. Interestingly, 15N2 incorporation in single DSB cells was methane-dependent, raising the possibility that DSB cells acquired reduced 15N products from diazotrophic ANME while spatially coupled, and then subsequently dissociated. With this combined data set we address several outstanding questions in methane seep microbial ecosystems and highlight the benefit of measuring microbial activity in the context of spatial associations. PMID:26394007
Dekas, Anne E.; Connon, Stephanie A.; Chadwick, Grayson L.; ...
2015-09-22
To characterize the activity and interactions of methanotrophic archaea (ANME) and Deltaproteo-bacteria at a methane-seeping mud volcano, we used two complimentary measures of microbial activity: a community-level analysis of the transcription of four genes (16S rRNA, methyl coenzyme M reductase A (mcrA), adenosine-5'-phosphosulfate reductase α-subunit (aprA), dinitrogenase reductase (nifH)), and a single-cell-level analysis of anabolic activity using fluorescence in situ hybridization coupled to nanoscale secondary ion mass spectrometry (FISH-NanoSIMS). Transcript analysis revealed that members of the deltaproteobacterial groups Desulfosarcina/Desulfococcus (DSS) and Desulfobulbaceae (DSB) exhibit increased rRNA expression in incubations with methane, suggestive of ANME-coupled activity. Direct analysis of anabolic activity in DSS cells in consortia with ANME by FISH-NanoSIMS confirmed their dependence on methanotrophy, with no 15NHmore » $$+\\atop{4}$$ assimilation detected without methane. In contrast, DSS and DSB cells found physically independent of ANME (i.e., single cells) were anabolically active in incubations both with and without methane. These single cells therefore comprise an active ‘free-living’ population, and are not dependent on methane or ANME activity. We investigated the possibility of N 2 fixation by seep Deltaproteobacteria and detected nifH transcripts closely related to those of cultured diazotrophic Deltaproteobacteria. However, nifH expression was methane-dependent. 15N 2 incorporation was not observed in single DSS cells, but was detected in single DSB cells. Interestingly, 15N 2 incorporation in single DSB cells was methane-dependent, raising the possibility that DSB cells acquired reduced 15N products from diazotrophic ANME while spatially coupled, and then subsequently dissociated. In conclusion, with this combined data set we address several outstanding questions in methane seep microbial ecosystems and highlight the benefit of measuring microbial activity in the context of spatial associations.« less
Methanosarcina plays a main role during methanogenesis of high-solids food waste and cardboard.
Capson-Tojo, Gabriel; Trably, Eric; Rouez, Maxime; Crest, Marion; Bernet, Nicolas; Steyer, Jean-Philippe; Delgenès, Jean-Philippe; Escudié, Renaud
2018-04-07
Anaerobic digestion of food waste is a complex process often hindered by high concentrations of volatile fatty acids and ammonia. Methanogenic archaea are more sensitive to these inhibitors than bacteria and thus the structure of their community is critical to avoid reactor acidification. In this study, the performances of three different inocula were compared using batch digestion tests of food waste and cardboard mixtures. Particular attention was paid to the archaeal communities in the inocula and after digestion. While the tests started with inocula rich in Methanosarcina led to efficient methane production, VFAs accumulated in the reactors where inocula initially were poor in this archaea and no methane was produced. In addition, higher substrate loads were tolerated when greater proportions of Methanosarcina were initially present in the inoculum. Independently of the inoculum origin, Methanosarcina were the dominant methanogens in the digestates from the experiments that efficiently produced methane. These results suggest that the initial archaeal composition of the inoculum is crucial during reactor start-up to achieve stable anaerobic digestion at high concentrations of ammonia and organic acids. Copyright © 2018 Elsevier Ltd. All rights reserved.
From Animal Waste to Energy; A Study of Methane Gas converted to Energy.
NASA Astrophysics Data System (ADS)
Weiss, S.
2016-12-01
Does animal waste produce enough harvestable energy to power a household, and if so, what animal's waste can produce the most methane that is usable. What can we power using this methane and how can we power these appliances within an average household using the produced methane from animal waste. The waste product from animals is readily available all over the world, including third world countries. Using animal waste to produce green energy would allow low cost energy sources and give independence from fossil fuels. But which animal produces the most methane and how hard is it to harvest? Before starting this experiment I knew that some cow farms in the northern part of the Central California basin were using some of the methane from the waste to power their machinery as a safer, cheaper and greener source through the harnessed methane gas in a digester. The fermentation process would occur in the digester producing methane gasses as a side product. Methane that is collected can later be burned for energy. I have done a lot of research on this experiment and found that many different farm and ranch animals produce methane, but it was unclear which produced the most. I decided to focus my study on the waste from cows, horses, pig and dogs to try to find the most efficient and strongest source of methane from animal waste. I produced an affordable methane digester from plastic containers with a valve to attach a hose. By putting in the waste product and letting it ferment with water, I was able to produce and capture methane, then measure the amount with a Gaslab meter. By showing that it is possible to create energy with this simple digester, it could reduce pollution and make green energy easily available to communities all over the world. Eventually this could result into our sewer systems converting waste to energy, producing an energy source right in your home.
Co-aromatization of olefin and methane over Ag-Ga/ZSM-5 catalyst at low temperature
DOE Office of Scientific and Technical Information (OSTI.GOV)
He, Peng; Gatip, Richard; Yung, Matthew
The massive exploitation of shale gas in the past decade has boosted the production of natural gas and reduced its price dramatically. The methane activation and following conversion into more valuable fuels and chemicals have thus become more and more attractive, while the introduction of hydrocarbons to enhance the methane activation at mild conditions represents a promising approach. In the present work, the co-aromatization of methane with propylene has been studied at 400 °C. The presence of methane would increase the toluene to benzene ratio as well as the average carbon number of the formed liquid aromatic products compared tomore » its propylene alone counterpart. Among the gas products, the formations of C 3H 8, C 4H 8 and C 4H 10 also get promoted when methane is present. The incorporation of methane into the product molecules is also directly evidenced by the 1H, 2D and 13C NMR spectroscopy of the liquid products obtained from the reaction between propylene (or styrene) and isotope labelled methane. Hydrogen from methane would contribute a large portion of the hydrogen in the product molecules, while the benzylic and aromatic hydrogen sites are favored compared with those on the alkyl side chains. The activation of methane is also observed in the DRIFT spectra when deuterium enriched methane is engaged as the methane source and evidenced by the escalated exothermic feature when olefin aromatization takes place under methane environment. The excellent catalytic performance of Ag-Ga/ZSM-5 might be because of the better dispersion of Ag and Ga on the ZSM-5 surface and moderate amount of strong Brosted and Lewis surface acid sites. All the observations suggest that methane might be activated nonoxidatively and converted into aromatics if suitable catalyst is charged under the assistance of co-existing olefin. In conclusion, the reported synergetic effect could potentially lead to the more economic utilization of abundant natural gas and petrochemical intermediates.« less
Co-aromatization of olefin and methane over Ag-Ga/ZSM-5 catalyst at low temperature
He, Peng; Gatip, Richard; Yung, Matthew; ...
2017-04-22
The massive exploitation of shale gas in the past decade has boosted the production of natural gas and reduced its price dramatically. The methane activation and following conversion into more valuable fuels and chemicals have thus become more and more attractive, while the introduction of hydrocarbons to enhance the methane activation at mild conditions represents a promising approach. In the present work, the co-aromatization of methane with propylene has been studied at 400 °C. The presence of methane would increase the toluene to benzene ratio as well as the average carbon number of the formed liquid aromatic products compared tomore » its propylene alone counterpart. Among the gas products, the formations of C 3H 8, C 4H 8 and C 4H 10 also get promoted when methane is present. The incorporation of methane into the product molecules is also directly evidenced by the 1H, 2D and 13C NMR spectroscopy of the liquid products obtained from the reaction between propylene (or styrene) and isotope labelled methane. Hydrogen from methane would contribute a large portion of the hydrogen in the product molecules, while the benzylic and aromatic hydrogen sites are favored compared with those on the alkyl side chains. The activation of methane is also observed in the DRIFT spectra when deuterium enriched methane is engaged as the methane source and evidenced by the escalated exothermic feature when olefin aromatization takes place under methane environment. The excellent catalytic performance of Ag-Ga/ZSM-5 might be because of the better dispersion of Ag and Ga on the ZSM-5 surface and moderate amount of strong Brosted and Lewis surface acid sites. All the observations suggest that methane might be activated nonoxidatively and converted into aromatics if suitable catalyst is charged under the assistance of co-existing olefin. In conclusion, the reported synergetic effect could potentially lead to the more economic utilization of abundant natural gas and petrochemical intermediates.« less
Activities That Reduce Global Anthropogenic Methane Emissions Grant - Closed Announcement FY 2012
Grant to fund eligible projects for activities that advance near-term, cost-effective methane abatement or recovery and use as a clean energy source, and support the goals of of theGlobal Methane Initiative.
Distribution and Rate of Methane Oxidation in Sediments of the Florida Everglades †
King, Gary M.; Roslev, Peter; Skovgaard, Henrik
1990-01-01
Rates of methane emission from intact cores were measured during anoxic dark and oxic light and dark incubations. Rates of methane oxidation were calculated on the basis of oxic incubations by using the anoxic emissions as an estimate of the maximum potential flux. This technique indicated that methane oxidation consumed up to 91% of the maximum potential flux in peat sediments but that oxidation was negligible in marl sediments. Oxygen microprofiles determined for intact cores were comparable to profiles measured in situ. Thus, the laboratory incubations appeared to provide a reasonable approximation of in situ activities. This was further supported by the agreement between measured methane fluxes and fluxes predicted on the basis of methane profiles determined by in situ sampling of pore water. Methane emissions from peat sediments, oxygen concentrations and penetration depths, and methane concentration profiles were all sensitive to light-dark shifts as determined by a combination of field and laboratory analyses. Methane emissions were lower and oxygen concentrations and penetration depths were higher under illuminated than under dark conditions; the profiles of methane concentration changed in correspondence to the changes in oxygen profiles, but the estimated flux of methane into the oxic zone changed negligibly. Sediment-free, root-associated methane oxidation showed a pattern similar to that for methane oxidation in the core analyses: no oxidation was detected for roots growing in marl sediment, even for roots of Cladium jamaicense, which had the highest activity for samples from peat sediments. The magnitude of the root-associated oxidation rates indicated that belowground plant surfaces may not markedly increase the total capacity for methane consumption. However, the data collectively support the notion that the distribution and activity of methane oxidation have a major impact on the magnitude of atmospheric fluxes from the Everglades. PMID:16348299
Rain increases methane production and methane oxidation in a boreal thermokarst bog
NASA Astrophysics Data System (ADS)
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 thermokarst bogs to energy and oxygen inputs from rain, and have implications for how boreal wetland methane emissions may respond in the future to altered precipitation patterns. Advective delivery of energy and oxygen to wetland subsoils via rainwater is not currently a mechanism included in bottom-up wetland methane models.
CO2 Injection Into CH4 Hydrate Reservoirs: Quantifying Controls of Micro-Scale Processes
NASA Astrophysics Data System (ADS)
Bigalke, N. K.; Deusner, C.; Kossel, E.; Haeckel, M.
2014-12-01
The exchangeability of methane for carbon dioxide in gas hydrates opens the possibility of producing emission-neutral hydrocarbon energy. Recent field tests have shown that the production of natural gas from gas hydrates is feasible via injection of carbon dioxide into sandy, methane-hydrate-bearing sediment strata. Industrial-scale application of this method requires identification of thermo- and fluid-dynamic as well as kinetic controls on methane yield from and carbon dioxide retention within the reservoir. Extraction of gas via injection of carbon dioxide into the hydrate reservoir triggers a number of macroscopic effects, which are revealed for example by changes of the hydraulic conductivity and geomechanical stability. Thus far, due to analytical limitations, localized reactions and fluid-flow phenomena held responsible for these effects remain unresolved on the microscale (1 µm - 1 mm) and at near-natural reservoir conditions. We address this deficit by showing results from high-resolution, two-dimensional Raman spectroscopy mappings of an artificial hydrate reservoir during carbon dioxide injection under realistic reservoir conditions. The experiments allow us to resolve hydrate conversion rate and efficiency as well as activation of fluid pathways in space and time and their effect on methane yield, carbon-dioxide retention and hydraulic conductivity of the reservoir. We hypothesize that the conversion of single hydrate grains is a diffusion-controlled process which starts at the grain surface before continuing into the grain interior and show that the conversion can be modeled simply by using published permeation coefficients for CO2 and CH4 in hydrate and grain size as only input parameters.
DOE Office of Scientific and Technical Information (OSTI.GOV)
NONE
1998-12-31
Research in the initial grant period focused on computational studies relevant to the selective activation of methane, the prime component of natural gas. Reaction coordinates for methane activation by experimental models were delineated, as well as the bonding and structure of complexes that effect this important reaction. This research, highlighted in the following sections, also provided the impetus for further development, and application of methods for modeling metal-containing catalysts. Sections of the report describe the following: methane activation by multiple-bonded transition metal complexes; computational lanthanide chemistry; and methane activation by non-imido, multiple-bonded ligands.
Siljanen, Henri M. P.; Saari, Anne; Bodrossy, Levente; Martikainen, Pertti J.
2012-01-01
Methane is the second most abundant greenhouse gas in the atmosphere. A major part of the total methane emissions from lake ecosystems is emitted from littoral wetlands. Methane emissions are significantly reduced by methanotrophs, as they use methane as their sole energy and carbon source. Methanotrophic activity can be either activated or inhibited by nitrogen. However, the effects of nitrogen on methanotrophs in littoral wetlands are unknown. Here we report how nitrogen loading in situ affected the function and diversity of methanotrophs in a boreal littoral wetland. Methanotrophic community composition and functional diversity were analyzed with a particulate methane monooxygenase (pmoA) gene targeted microarray. Nitrogen load had no effects on methane oxidation potential and methane fluxes. Nitrogen load activated pmoA gene transcription of type I (Methylobacter, Methylomonas, and LW21-freshwater phylotypes) methanotrophs, but decreased the relative abundance of type II (Methylocystis, Methylosinus trichosporium, and Methylosinus phylotypes) methanotrophs. Hence, the overall activity of a methanotroph community in littoral wetlands is not affected by nitrogen leached from the catchment area. PMID:22363324
Liu, Zongyuan; Grinter, David C.; Lustemberg, Pablo G.; ...
2016-05-04
Ni-CeO 2 is a highly efficient, stable and non-expensive catalyst for methane dry reforming at relative low temperatures (700 K). The active phase of the catalyst consists of small nanoparticles of nickel dispersed on partially reduced ceria. Experiments of ambient pressure XPS indicate that methane dissociates on Ni/CeO 2 at temperatures as low as 300 K, generating CH x and CO x species on the surface of the catalyst. Strong metal–support interactions activate Ni for the dissociation of methane. The results of density-functional calculations show a drop in the effective barrier for methane activation from 0.9 eV on Ni(111) tomore » only 0.15 eV on Ni/CeO 2–x(111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CH x or C species are detected in the C1s XPS region. As a result, the reforming of methane proceeds in a clean and efficient way.« less
Coalbed Methane Outreach Program
Coalbed Methane Outreach Program, voluntary program seeking to reduce methane emissions from coal mining activities. CMOP promotes profitable recovery/use of coal mine methane (CMM), addressing barriers to using CMM instead of emitting it to atmosphere.
Termites Facilitate Methane Oxidation and Shape the Methanotrophic Community
Erens, Hans; Mujinya, Basile Bazirake; Boeckx, Pascal; Baert, Geert; Schneider, Bellinda; Frenzel, Peter; Van Ranst, Eric
2013-01-01
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. PMID:24038691
Termites facilitate methane oxidation and shape the methanotrophic community.
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.
Evolution of microorganisms in thermophilic-dry anaerobic digestion.
Montero, B; Garcia-Morales, J L; Sales, D; Solera, R
2008-05-01
Microbial population dynamics were studied during the start-up and stabilization periods in thermophilic-dry anaerobic digestion at lab-scale. The experimental protocol was defined to quantify Eubacteria and Archaea using Fluorescent in situ hybridization (FISH) in a continuously stirred tank reactor (CSTR), without recycling solids. The reactor was subjected to a programme of steady-state operation over a range of the retention times from 40 to 25 days, with an organic loading rate between 4.42 and 7.50 kg volatile solid/m3/day. Changes in microbial concentrations were linked to traditional performance parameters such as biogas production and VS removal. The relations of Eubacteria:Archaea and H2-utilising methanogens:acetate-utilising methanogens were 88:12 and 11:1, respectively, during start-up stage. Hydrogenotrophic methanogens, although important in the initial phase of the reactor start-up, were displaced by acetoclastic methanogens at steady-state, thus their relation were 7:32, respectively. The methane yield coefficient, the methane content in the biogas and VS removal were stabilized around 0.30 LCH4/gCOD, 50% and 80%, respectively. Methanogenic population correlated well with performance measurements.
NASA Astrophysics Data System (ADS)
Weiss, S.
2015-12-01
The waste product from animals is readily available all over the world, including third world countries. Using animal waste to produce green energy would allow low cost energy sources and give independence from fossil fuels. But which animal produces the most methane and how hard is it to harvest? Before starting this experiment I knew that some cow farms in the northern part of the Central California basin were using some of the methane from the waste to power their machinery as a safer, cheaper and greener source through the harnessed methane gas in a digester. The fermentation process would occur in the digester producing methane gasses as a side product. Methane that is collected can later be burned for energy. I have done a lot of research on this experiment and found that many different farm and ranch animals produce methane, but it was unclear which produced the most. I decided to focus my study on the waste from cows, horses, pig and dogs to try to find the most efficient and strongest source of methane from animal waste. I produced an affordable methane digester from plastic containers with a valve to attach a hose. By putting in the waste product and letting it ferment with water, I was able to produce and capture methane, then measure the amount with a Gaslab meter. By showing that it is possible to create energy with this simple digester, it could reduce pollution and make green energy easily available to communities all over the world. Eventually this could result into our sewer systems converting waste to energy, producing an energy source right in your home.
NASA Astrophysics Data System (ADS)
Yuliusman; Afdhol, M. K.; Sanal, Alristo
2018-03-01
Carbon monoxide and methane gas are widely present in oil refineries. Off-potential gas is used as raw material for the petrochemical industry. In order for this off-gas to be utilized, carbon monoxide and methane must be removed from off-gas. This study aims to adsorb carbon monoxide and methane using activated carbon of palm shells and commercial activated carbon simultaneously. This research was conducted in 2 stages: 1) Preparation and characterization of activated carbon, 2) Carbon monoxide and methane adsorption test. The activation experiments using carbon dioxide at a flow rate of 150 ml/min yielded a surface area of 978.29 m2/g, Nitrogen at flow rate 150 ml/min yielded surface area 1241.48 m2/g, and carbon dioxide and nitrogen at a flow rate 200 ml/min yielded a surface area 300.37 m2/g. Adsorption of carbon monoxide and methane on activated carbon of palm shell systems yielded results in the amount of 0.5485 mg/g and 0.0649 mg/g and using commercial activated carbon yielded results in the amount of 0.5480 mg/g and 0.0650 mg/g
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.
Biey, E M; Musibono, E D; Verstraete, W
2003-01-01
Vegetable fruit garden wastes were treated anaerobically using a multistage Dranco system. The digesters were composed of three 50 L vessels kept in mesophilic conditions. They were operating at 14.5-17% TS. By controlling the pH in the system, the start-up for biogas production was shortened to 60 days. The pH correction was a buffering which enhanced methanogenic activity in the digesters. With a loading rate of 4.1 kg VS/m3 reactor/day, the production of biogas was 5 m3/m3 reactor/ day, and 60-70% methane content. This allowed making a multisystem by starting every 3 weeks with new vessels in order to maintain biogas production, to be used in industries or in local communities in low-tech countries. The designed model was started in Kinshasa (Congo) where a project is expected to treat one ton of solid waste on a daily basis, for a production of 100 m3 biogas. This cost effectiveness of the system is demonstrated and presents the opportunity for biowaste treatment coupled with environmental protection and substantial energy recovery.
NASA Astrophysics Data System (ADS)
Houweling, S.; Pandey, S.; Segers, A.
2017-12-01
Methane is regarded as a suitable target for short-term climate mitigation, because of its relatively short atmospheric residence time compared to carbon dioxide and other long-lived greenhouse gases. However, to build climate policy on methane is complicated because of the uncertainties in its emission budget, reflected in the difficulty to predict its global growth rate. Several different and conflicting scenarios have been proposed in high profile journals to explain its recent evolution in the atmosphere. Since the early 2000s atmospheric methane is being measured by Earth orbiting satellites. Missions such as SCIAMACHY and GOSAT have largely increased the number of atmospheric methane measurements that are available for the quantification its emissions using inverse modelling techniques. In this presentation, we address the question what has been the role of satellite data in the discussion about the causes of the varying growth rate of methane, and what are the remaining limitations. This is the time when space borne remote sensing of methane is transitioning from exploratory scientific missions to monitoring missions, starting with the preoperational mission S5p TROPOMI to be launched in September 2017. In the meantime, also inverse modelling techniques are prepared for operational use in support of COP21 agreement to reduce greenhouse gas emissions. These developments bring new opportunities and challenges, which will be discussed.
Development of a preprototype sabatier CO2 reduction subsystem
NASA Technical Reports Server (NTRS)
Kleiner, G. N.; Birbara, P.
1980-01-01
A preoprototype Sabatier CO2 Reduction Subsystem was successfully designed, fabricated and tested. The lightweight, quick starting reactor utilizes a highly active and physically durable methanation catalyst composed of ruthenium on alumina. The use of this improved catalyst permits a single straight through plug flow design with an average lean component H2/CO2 conversion efficiency of over 99% over a range of H2/CO2 molar ratios of 1.8 to 5 while operating with flows equivalent to a crew size of one person steadystate to 3 persons cyclical (equivalent to 5 persons steady state). The reactor requires no heater operation after start-up even during simulated 55 minute lightside/39 minute darkside orbital operation over the above range of molar ratios and crew loadings. The subsystem's operation and performance is controlled by a microprocessor and displayed on a nineteen inch multi-colored cathode ray tube.
Development of a preprototype Sabatier CO2 reduction subsystem
NASA Technical Reports Server (NTRS)
Kleiner, G. N.; Birbara, P.
1981-01-01
A lightweight, quick starting reactor utilizes a highly active and physically durable methanation catalyst composed of ruthenium on alumina. The use of this improved catalyst permits a single straight through plug flow design with an average lean component H2/CO2 conversion efficiency of over 99% over a range of H2/CO2 molar ratios of 1.8 to 5 while operating with flows equivalent to a crew size of one person steadystate to 3 persons cyclical. The reactor requires no heater operation after start-up even during simulated 55 minute lightside/39 minute darkside orbital operation over the above range of molar ratios and crew loadings. Subsystem performance was proven by parametric testing and endurance testing over a wide range of crew sizes and metabolic loadings. The subsystem's operation and performance is controlled by a microprocessor and displayed on a nineteen inch multi-colored cathode ray tube.
Novel microbial communities of the Haakon Mosby mud volcano and their role as a methane sink.
Niemann, Helge; Lösekann, Tina; de Beer, Dirk; Elvert, Marcus; Nadalig, Thierry; Knittel, Katrin; Amann, Rudolf; Sauter, Eberhard J; Schlüter, Michael; Klages, Michael; Foucher, Jean Paul; Boetius, Antje
2006-10-19
Mud volcanism is an important natural source of the greenhouse gas methane to the hydrosphere and atmosphere. Recent investigations show that the number of active submarine mud volcanoes might be much higher than anticipated (for example, see refs 3-5), and that gas emitted from deep-sea seeps might reach the upper mixed ocean. Unfortunately, global methane emission from active submarine mud volcanoes cannot be quantified because their number and gas release are unknown. It is also unclear how efficiently methane-oxidizing microorganisms remove methane. Here we investigate the methane-emitting Haakon Mosby Mud Volcano (HMMV, Barents Sea, 72 degrees N, 14 degrees 44' E; 1,250 m water depth) to provide quantitative estimates of the in situ composition, distribution and activity of methanotrophs in relation to gas emission. The HMMV hosts three key communities: aerobic methanotrophic bacteria (Methylococcales), anaerobic methanotrophic archaea (ANME-2) thriving below siboglinid tubeworms, and a previously undescribed clade of archaea (ANME-3) associated with bacterial mats. We found that the upward flow of sulphate- and oxygen-free mud volcano fluids restricts the availability of these electron acceptors for methane oxidation, and hence the habitat range of methanotrophs. This mechanism limits the capacity of the microbial methane filter at active marine mud volcanoes to <40% of the total flux.
A case study of methane gas migration through sealed mine GOB into active mine workings
DOE Office of Scientific and Technical Information (OSTI.GOV)
Garcia, F.; McCall, F.E.; Trevits, M.A.
1995-12-31
The U.S. Bureau of Mines investigated the influence of atmospheric pressure changes on methane gas migration through mine seals at a mine site located in the Pittsburgh Coalbed. The mine gained access to a coal reserve through part of an abandoned mine and constructed nine seals to isolate the extensive old workings from the active mine area. Underground problems were experienced when atmospheric pressure fell, causing methane gas to migrate around the seals and into the active workings. During mining operations, methane gas levels exceeded legal limits and coal production was halted until the ventilation system could be improved. Whenmore » mining resumed with increased air flow, methane gas concentrations occasionally exceeded the legal limits and production had to be halted until the methane level fell within the mandated limit. To assist the ventilation system, a pressure relief borehole located in the abandoned workings near the mine seals was proposed. Preliminary estimates by a gob gas simulator (computer model) suggested that a 0.76 m (2.5 ft) diameter pressure relief borehole with an exhaust fan would be necessary to remove enough methane from the abandoned area so that the ventilation system could dilute the gas in the active workings. However, by monitoring methane gas emissions and seal pressure, during periods of low atmospheric pressure, the amount of methane gas that migrated into the active mine workings was calculated. Researchers then determined that a relief borehole, 20.3 cm (8-in) with an exhaust fan could remove at least twice the maximum measured volume of migrating methane gas. Because gas concentrations in the abandoned workings could potentially reach explosive limits, it was proposed that the mine eliminate the exhaust fan. Installation of the recommended borehole and enlarging two other ventilation boreholes located In the abandoned area reduced methane gas leakage through the seals by at least 63%.« less
Ion-Molecule Reactions and Chemical Composition of Emanated from Herculane Spa Geothermal Sources
Cosma, Constantin; Suciu, Ioan; Jäntschi, Lorentz; Bolboacă, Sorana D.
2008-01-01
The paper presents a chemical composition analysis of the gases emanated from geothermal sources in the Herculane Spa area (Romania). The upper homologues of methane have been identified in these gases. An ion-molecule reaction mechanism could be implicated in the formation of the upper homologues of methane. The CH4+ ions that appear under the action of radiation are the starting point of these reactions. The presence of hydrogen in the emanated gases may be also a result of these reactions. PMID:19325844
Temperature-Induced Increase in Methane Release from Peat Bogs: A Mesocosm Experiment
van Winden, Julia F.; Reichart, Gert-Jan; McNamara, Niall P.; Benthien, Albert; Damsté, Jaap S. Sinninghe.
2012-01-01
Peat bogs are primarily situated at mid to high latitudes and future climatic change projections indicate that these areas may become increasingly wetter and warmer. Methane emissions from peat bogs are reduced by symbiotic methane oxidizing bacteria (methanotrophs). Higher temperatures and increasing water levels will enhance methane production, but also methane oxidation. To unravel the temperature effect on methane and carbon cycling, a set of mesocosm experiments were executed, where intact peat cores containing actively growing Sphagnum were incubated at 5, 10, 15, 20, and 25°C. After two months of incubation, methane flux measurements indicated that, at increasing temperatures, methanotrophs are not able to fully compensate for the increasing methane production by methanogens. Net methane fluxes showed a strong temperature-dependence, with higher methane fluxes at higher temperatures. After removal of Sphagnum, methane fluxes were higher, increasing with increasing temperature. This indicates that the methanotrophs associated with Sphagnum plants play an important role in limiting the net methane flux from peat. Methanotrophs appear to consume almost all methane transported through diffusion between 5 and 15°C. Still, even though methane consumption increased with increasing temperature, the higher fluxes from the methane producing microbes could not be balanced by methanotrophic activity. The efficiency of the Sphagnum-methanotroph consortium as a filter for methane escape thus decreases with increasing temperature. Whereas 98% of the produced methane is retained at 5°C, this drops to approximately 50% at 25°C. This implies that warming at the mid to high latitudes may be enhanced through increased methane release from peat bogs. PMID:22768100
Monocopper active site for partial methane oxidation in Cu-exchanged 8MR zeolites
Kulkarni, Ambarish R.; Zhao, Zhi -Jian; Siahrostami, Samira; ...
2016-08-17
Direct conversion of methane to methanol using oxygen is experiencing renewed interest owing to the availability of new natural gas resources. Copper-exchanged zeolites such as mordenite and ZSM-5 have shown encouraging results, and di- and tri-copper species have been suggested as active sites. Recently, small eight-membered ring (8MR) zeolites including SSZ-13, -16, and -39 have been shown to be active for methane oxidation, but the active sites and reaction mechanisms in these 8MR zeolites are not known. In this work, we use density functional theory (DFT) calculations to systematically evaluate monocopper species as active sites for the partial methane oxidationmore » reaction in Cu-exchanged SSZ-13. On the basis of kinetic and thermodynamic arguments, we suggest that [Cu IIOH] + species in the 8MR are responsible for the experimentally observed activity. Furthermore, our results successfully explain the available spectroscopic data and experimental observations including (i) the necessity of water for methanol extraction and (ii) the effect of Si/Al ratio on the catalyst activity. Monocopper species have not yet been suggested as an active site for the partial methane oxidation reaction, and our results suggest that [Cu IIOH] + active site may provide complementary routes for methane activation in zeolites in addition to the known [Cu–O–Cu] 2+ and Cu 3O 3 motifs.« less
Methane Recycling During Burial of Methane Hydrate-Bearing Sediments
NASA Astrophysics Data System (ADS)
You, K.; Flemings, P. B.
2017-12-01
We quantitatively investigate the integral processes of methane hydrate formation from local microbial methane generation, burial of methane hydrate with sedimentation, and methane recycling at the base of the hydrate stability zone (BHSZ) with a multiphase multicomponent numerical model. Methane recycling happens in cycles, and there is not a steady state. Each cycle starts with free gas accumulation from hydrate dissociation below the BHSZ. This free gas flows upward under buoyancy, elevates the hydrate saturation and capillary entry pressure at the BHSZ, and this prevents more free gas flowing in. Later as this layer with elevated hydrate saturation is buried and dissociated, the large amount of free gas newly released and accumulated below rapidly intrudes into the hydrate stability zone, drives rapid hydrate formation and creates three-phase (gas, liquid and hydrate) equilibrium above the BHSZ. The gas front retreats to below the BHSZ until all the free gas is depleted. The shallowest depth that the free gas reaches in one cycle moves toward seafloor as more and more methane is accumulated to the BHSZ with time. More methane is stored above the BHSZ in the form of concentrated hydrate in sediments with relatively uniform pore throat, and/or with greater compressibility. It is more difficult to initiate methane recycling in passive continental margins where the sedimentation rate is low, and in sediments with low organic matter content and/or methanogenesis reaction rate. The presence of a permeable layer can store methane for significant periods of time without recycling. In a 2D system where the seafloor dips rapidly, the updip gas flow along the BHSZ transports more methane toward topographic highs where methane gas and elevated hydrate saturation intrude deeper into the hydrate stability zone within one cycle. This could lead to intermittent gas venting at seafloor at the topographic highs. This study provides insights on many phenomenon associated with methane recycling, such as the formation of free gas zone, concentrated hydrate zone, bottom simulating reflector, and overpressured zone around the BHSZ, and gas venting at seafloor.
Printable enzyme-embedded materials for methane to methanol conversion
Blanchette, Craig D.; Knipe, Jennifer M.; Stolaroff, Joshuah K.; ...
2016-06-15
An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas. The only selective catalysts for methane activation and conversion to methanol under mild conditions are methane monooxygenases (MMOs) found in methanotrophic bacteria; however, these enzymes are not amenable to standard enzyme immobilization approaches. Using particulate methane monooxygenase (pMMO), we create a biocatalytic polymer material that converts methane to methanol. We demonstrate embedding the material within a silicone lattice to create mechanically robust, gas-permeable membranes, and direct printing of micron-scalemore » structures with controlled geometry. Remarkably, the enzymes retain up to 100% activity in the polymer construct. The printed enzyme-embedded polymer motif is highly flexible for future development and should be useful in a wide range of applications, especially those involving gas–liquid reactions.« less
Printable enzyme-embedded materials for methane to methanol conversion
DOE Office of Scientific and Technical Information (OSTI.GOV)
Blanchette, Craig D.; Knipe, Jennifer M.; Stolaroff, Joshuah K.
An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas. The only selective catalysts for methane activation and conversion to methanol under mild conditions are methane monooxygenases (MMOs) found in methanotrophic bacteria; however, these enzymes are not amenable to standard enzyme immobilization approaches. Using particulate methane monooxygenase (pMMO), we create a biocatalytic polymer material that converts methane to methanol. We demonstrate embedding the material within a silicone lattice to create mechanically robust, gas-permeable membranes, and direct printing of micron-scalemore » structures with controlled geometry. Remarkably, the enzymes retain up to 100% activity in the polymer construct. The printed enzyme-embedded polymer motif is highly flexible for future development and should be useful in a wide range of applications, especially those involving gas–liquid reactions.« less
Printable enzyme-embedded materials for methane to methanol conversion
Blanchette, Craig D.; Knipe, Jennifer M.; Stolaroff, Joshuah K.; DeOtte, Joshua R.; Oakdale, James S.; Maiti, Amitesh; Lenhardt, Jeremy M.; Sirajuddin, Sarah; Rosenzweig, Amy C.; Baker, Sarah E.
2016-01-01
An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas. The only selective catalysts for methane activation and conversion to methanol under mild conditions are methane monooxygenases (MMOs) found in methanotrophic bacteria; however, these enzymes are not amenable to standard enzyme immobilization approaches. Using particulate methane monooxygenase (pMMO), we create a biocatalytic polymer material that converts methane to methanol. We demonstrate embedding the material within a silicone lattice to create mechanically robust, gas-permeable membranes, and direct printing of micron-scale structures with controlled geometry. Remarkably, the enzymes retain up to 100% activity in the polymer construct. The printed enzyme-embedded polymer motif is highly flexible for future development and should be useful in a wide range of applications, especially those involving gas–liquid reactions. PMID:27301270
Natural gas storage with activated carbon from a bituminous coal
Sun, Jielun; Rood, M.J.; Rostam-Abadi, M.; Lizzio, A.A.
1996-01-01
Granular activated carbons ( -20 + 100 mesh; 0.149-0.84 mm) were produced by physical activation and chemical activation with KOH from an Illinois bituminous coal (IBC-106) for natural gas storage. The products were characterized by BET surface area, micropore volume, bulk density, and methane adsorption capacities. Volumetric methane adsorption capacities (Vm/Vs) of some of the granular carbons produced by physical activation are about 70 cm3/cm3 which is comparable to that of BPL, a commercial activated carbon. Vm/Vs values above 100 cm3/cm3 are obtainable by grinding the granular products to - 325 mesh (<0.044 mm). The increase in Vm/Vs is due to the increase in bulk density of the carbons. Volumetric methane adsorption capacity increases with increasing pore surface area and micropore volume when normalizing with respect to sample bulk volume. Compared with steam-activated carbons, granular carbons produced by KOH activation have higher micropore volume and higher methane adsorption capacities (g/g). Their volumetric methane adsorption capacities are lower due to their lower bulk densities. Copyright ?? 1996 Elsevier Science Ltd.
Fugitive greenhouse gas emissions from shale gas activities - a case study of Dish, TX
NASA Astrophysics Data System (ADS)
Khan, A.; Roscoe, B.; Lary, D.; Schaefer, D.; Tao, L.; Sun, K.; Brian, A.; DiGangi, J.; Miller, D. J.; Zondlo, M. A.
2012-12-01
We evaluate new findings on aerial (horizontal and vertical) mapping of methane emissions in the atmospheric boundary layer region to help study fugitive methane emissions from extraction, transmission, and storage of natural gas and oil in Dish, Texas. Dish is located in the Barnett Shale which has seen explosive development of hydraulic fracking activities in recent years. The aerial measurements were performed with a new laser-based methane sensor developed specifically for an unmanned aerial vehicle (UAV). The vertical cavity surface emitting laser (VCSEL) methane sensor, with a mass of 2.5 kg and a precision of < 20 ppbv methane at 1 Hz, was flown on the UT-Dallas ARC Payload Master electronic aircraft at two sites in Texas: one representative of urban emissions of the Dallas-Fort Worth area in Richardson, Texas and another in Dish, Texas, closer to gas and oil activities. Methane mixing ratios at Dish were ubiquitously in the 3.5 - 4 ppmv range which was 1.5 - 2 ppmv higher than methane levels immediately downwind of Dallas. During the flight measurements at Dish, narrow methane plumes exceeding 20 ppmv were frequently observed at altitudes from the surface to 130 m above the ground. Based on the wind speed at the sampling location, the horizontal widths of large methane plumes were of the order of 100 m. The locations of the large methane plumes were variable in space and time over a ~ 1 km2 area sampled from the UAV. Spatial mapping over larger scales (10 km) by ground-based measurements showed similar methane levels as the UAV measurements. To corroborate our measurements, alkane and other hydrocarbon mixing ratios from an on-site TCEQ environmental monitoring station were analyzed and correlated with methane measurements to fingerprint the methane source. We show that fugitive methane emissions at Dish are a significant cause of the large and ubiquitous methane levels on the 1-10 km scale.
Federal Register 2010, 2011, 2012, 2013, 2014
2012-01-27
... Activities; Proposed Collection; Comment Request; Reporting Under EPA's Landfill Methane Outreach Program...; and other landfill gas energy stakeholders. Title: Reporting Under EPA's Landfill Methane Outreach... Landfill Methane Outreach Program (LMOP), created by EPA as part of the Climate Change Action Plan, is a...
Snowball Earth termination by destabilization of equatorial permafrost methane clathrate.
Kennedy, Martin; Mrofka, David; von der Borch, Chris
2008-05-29
The start of the Ediacaran period is defined by one of the most severe climate change events recorded in Earth history--the recovery from the Marinoan 'snowball' ice age, approximately 635 Myr ago (ref. 1). Marinoan glacial-marine deposits occur at equatorial palaeolatitudes, and are sharply overlain by a thin interval of carbonate that preserves marine carbon and sulphur isotopic excursions of about -5 and +15 parts per thousand, respectively; these deposits are thought to record widespread oceanic carbonate precipitation during postglacial sea level rise. This abrupt transition records a climate system in profound disequilibrium and contrasts sharply with the cyclical stratigraphic signal imparted by the balanced feedbacks modulating Phanerozoic deglaciation. Hypotheses accounting for the abruptness of deglaciation include ice albedo feedback, deep-ocean out-gassing during post-glacial oceanic overturn or methane hydrate destabilization. Here we report the broadest range of oxygen isotope values yet measured in marine sediments (-25 per thousand to +12 per thousand) in methane seeps in Marinoan deglacial sediments underlying the cap carbonate. This range of values is likely to be the result of mixing between ice-sheet-derived meteoric waters and clathrate-derived fluids during the flushing and destabilization of a clathrate field by glacial meltwater. The equatorial palaeolatitude implies a highly volatile shelf permafrost pool that is an order of magnitude larger than that of the present day. A pool of this size could have provided a massive biogeochemical feedback capable of triggering deglaciation and accounting for the global postglacial marine carbon and sulphur isotopic excursions, abrupt unidirectional warming, cap carbonate deposition, and a marine oxygen crisis. Our findings suggest that methane released from low-latitude permafrost clathrates therefore acted as a trigger and/or strong positive feedback for deglaciation and warming. Methane hydrate destabilization is increasingly suspected as an important positive feedback to climate change that coincides with critical boundaries in the geological record and may represent one particularly important mechanism active during conditions of strong climate forcing.
Arctic Methane: the View from Space
NASA Astrophysics Data System (ADS)
Leifer, I.; Yurganov, L.; Xiong, X.
2014-12-01
Global increase of methane that started in 2007-2008 after a decade of stability requires investigation and explanation. Recent Arctic warming has stimulated speculation about dissociation of Arctic Ocean methane hydrates providing a potentially important new climatic positive feedback. Satellite thermal infrared (TIR) data do not require sunlight, providing key advantages for Arctic data collection compared to shortwave infrared spectroscopy. The US Atmospheric IR Sounder (AIRS) has been delivering CH4 tropospheric data since 2002; NOAA CH4 retrievals from the European Infrared Atmospheric Sounding Interferometer (IASI) radiation data are available since 2008 and analyzed here since 2009. Accuracy of TIR satellite retrievals, especially for the lower troposphere, diminishes for a cold, underlying surface. In this analysis the dependence is parameterized using the Thermal Contrast (a difference between surface temperature and air temperature at the altitude of 4 km, defined THC). A correction function was applied to CH4 data based on a data-derived relationship between THC and retrieved CH4 for areas with positive THC (in other words, without temperature inversions). The seasonal cycles of the adjusted low tropospheric data are in agreement with the surface in situ measurements. Instantaneous IASI retrievals exhibit less variability than AIRS v6 data. Maximum positive deviation of methane concentration measured by IASI for the study period was found for Baffin Bay in November-December, 2013 (Figure). It was concluded that the methane anomaly could indicate both coastal and off-shore emissions. Off-shore data were spatially consistent with a hydrate dissociation mechanisms, active for water depths below the hydrate stability zone top at ~300 m. These are hypothesized to dissociate during seasonal temperature maximum in the bottom layer of the ocean, which occurs in fall. IASI data may be considered as a reliable source of information about Arctic CH4 for conditions of sufficiently high atmospheric vertical thermal contrast. Figure caption. Standard adjusted NOAA/IASI retrievals of 0-4 km mean methane concentration over areas with positive THC. Black points are for the entire Baffin Bay, red points are for locations with seawater depth below 300 m. Blue line is the all-Arctic mean.
Experimental and modeling study on decomposition kinetics of methane hydrates in different media.
Liang, Minyan; Chen, Guangjin; Sun, Changyu; Yan, Lijun; Liu, Jiang; Ma, Qinglan
2005-10-13
The decomposition kinetic behaviors of methane hydrates formed in 5 cm3 porous wet activated carbon were studied experimentally in a closed system in the temperature range of 275.8-264.4 K. The decomposition rates of methane hydrates formed from 5 cm3 of pure free water and an aqueous solution of 650 g x m(-3) sodium dodecyl sulfate (SDS) were also measured for comparison. The decomposition rates of methane hydrates in seven different cases were compared. The results showed that the methane hydrates dissociate more rapidly in porous activated carbon than in free systems. A mathematical model was developed for describing the decomposition kinetic behavior of methane hydrates below ice point based on an ice-shielding mechanism in which a porous ice layer was assumed to be formed during the decomposition of hydrate, and the diffusion of methane molecules through it was assumed to be one of the control steps. The parameters of the model were determined by correlating the decomposition rate data, and the activation energies were further determined with respect to three different media. The model was found to well describe the decomposition kinetic behavior of methane hydrate in different media.
NASA Astrophysics Data System (ADS)
Ebrahimi, Ali; Or, Dani
2017-05-01
The sensitivity of polar regions to raising global temperatures is reflected in rapidly changing hydrological processes associated with pronounced seasonal thawing of permafrost soil and increased biological activity. Of particular concern is the potential release of large amounts of soil carbon and stimulation of other soil-borne greenhouse gas emissions such as methane. Soil methanotrophic and methanogenic microbial communities rapidly adjust their activity and spatial organization in response to permafrost thawing and other environmental factors. Soil structural elements such as aggregates and layering affect oxygen and nutrient diffusion processes thereby contributing to methanogenic activity within temporal anoxic niches (hot spots). We developed a mechanistic individual-based model to quantify microbial activity dynamics in soil pore networks considering transport processes and enzymatic activity associated with methane production in soil. The model was upscaled from single aggregates to the soil profile where freezing/thawing provides macroscopic boundary conditions for microbial activity at different soil depths. The model distinguishes microbial activity in aerate bulk soil from aggregates (or submerged profile) for resolving methane production and oxidation rates. Methane transport pathways by diffusion and ebullition of bubbles vary with hydration dynamics. The model links seasonal thermal and hydrologic dynamics with evolution of microbial community composition and function affecting net methane emissions in good agreement with experimental data. The mechanistic model enables systematic evaluation of key controlling factors in thawing permafrost and microbial response (e.g., nutrient availability and enzyme activity) on long-term methane emissions and carbon decomposition rates in the rapidly changing polar regions.
Karacan, C. Özgen
2015-01-01
The Black Warrior Basin of Alabama is one of the most important coal mining and coalbed methane production areas in the United States. Methane control efforts through degasification that started almost 25 years ago for the sole purpose of ensuring mining safety resulted in more than 5000 coalbed methane wells distributed within various fields throughout the basin. The wells are completed mostly in the Pratt, Mary Lee, and Black Creek coal groups of the Upper Pottsville formation and present a unique opportunity to understand methane reservoir properties of these coals and to improve their degasification performances. The Brookwood and Oak Grove fields in the Black Warrior Basin are probably two of the most important fields in the basin due to current longwall coal mining activities. In this work, methane and water productions of 92 vertical wellbores drilled, some completed 20 years ago, over a current large coal mine district located in these two fields, were analyzed by history matching techniques. The boreholes were completed at the Mary Lee coal group, or at combinations of the Pratt, Mary Lee, and Black Creek groups. History matching models were prepared and performed according to properties of each coal group. Decline curve analyses showed that effective exponential decline rates of the wells were between 2% and 25% per year. Results of production history matching showed, although they varied by coal group, that pressure decreased as much as 80% to nearly 25 psi in some areas and resulted in corresponding decreases in methane content. Water saturation in coals decreased from 100% to between 20 and 80%, improving gas relative permeabilities to as much as 0.8. As a result of primary depletion, permeability of coal seams increased between 10 and 40% compared to their original permeability, which varied between 1 and 10 md depending on depth and coal seam. These results not only can be used for diagnostic and interpretation purposes, but can be used as parameter distributions in probabilistic simulations, as illustrated in the last section of this paper. They can also be used in conjunction with spatial modeling and geological considerations to calculate potential methane emissions in operating mines. PMID:26191096
Electrical properties of polycrystalline methane hydrate
Du Frane, W. L.; Stern, L.A.; Weitemeyer, K.A.; Constable, S.; Pinkston, J.C.; Roberts, J.J.
2011-01-01
Electromagnetic (EM) remote-sensing techniques are demonstrated to be sensitive to gas hydrate concentration and distribution and complement other resource assessment techniques, particularly seismic methods. To fully utilize EM results requires knowledge of the electrical properties of individual phases and mixing relations, yet little is known about the electrical properties of gas hydrates. We developed a pressure cell to synthesize gas hydrate while simultaneously measuring in situ frequency-dependent electrical conductivity (σ). Synthesis of methane (CH4) hydrate was verified by thermal monitoring and by post run cryogenic scanning electron microscope imaging. Impedance spectra (20 Hz to 2 MHz) were collected before and after synthesis of polycrystalline CH4 hydrate from polycrystalline ice and used to calculate σ. We determined the σ of CH4 hydrate to be 5 × 10−5 S/m at 0°C with activation energy (Ea) of 30.6 kJ/mol (−15 to 15°C). After dissociation back into ice, σ measurements of samples increased by a factor of ~4 and Ea increased by ~50%, similar to the starting ice samples.
Cai, Chen; Hu, Shihu; Chen, Xueming; Ni, Bing-Jie; Pu, Jiaoyang; Yuan, Zhiguo
2018-10-15
Complete nitrogen removal has recently been demonstrated by integrating anaerobic ammonium oxidation (anammox) and denitrifying anaerobic methane oxidation (DAMO) processes. In this work, the effect of methane partial pressure on the performance of a membrane biofilm reactor (MBfR) consisting of DAMO and anammox microorganisms was evaluated. The activities of DAMO archaea and DAMO bacteria in the biofilm increased significantly with increased methane partial pressure, from 367 ± 9 and 58 ± 22 mg-N L -1 d -1 to 580 ± 12 and 222 ± 22 mg-N L -1 d -1 , respectively, while the activity of anammox bacteria only increased slightly, when the methane partial pressure was elevated from 0.24 to 1.39 atm in the short-term batch tests. The results were supported by a long-term (seven weeks) continuous test, when the methane partial pressure was dropped from 1.39 to 0.78 atm. The methane utilization efficiency was always above 96% during both short-term and long-term tests. Taken together, nitrogen removal rate (especially the nitrate reduction rate by DAMO archaea) and methane utilization efficiency could be maintained at high levels in a broad range of methane partial pressure (0.24-1.39 atm in this study). In addition, a previously established DAMO/anammox biofilm model was used to analyze the experimental data. The observed impacts of methane partial pressure on biofilm activity were well explained by the modeling results. These results suggest that methane partial pressure can potentially be used as a manipulated variable to control reaction rates, ultimately to maintain high nitrogen removal efficiency, according to nitrogen loading rate. Copyright © 2018 Elsevier B.V. All rights reserved.
Bioassay for estimating the biogenic methane-generating potential of coal samples
Jones, Elizabeth J.P.; Voytek, Mary A.; Warwick, Peter D.; Corum, Margo D.; Cohn, Alexander G.; Bunnell, Joseph E.; Clark, Arthur C.; Orem, William H.
2008-01-01
Generation of secondary biogenic methane in coal beds is likely controlled by a combination of factors such as the bioavailability of coal carbon, the presence of a microbial community to convert coal carbon to methane, and an environment supporting microbial growth and methanogenesis. A set of treatments and controls was developed to bioassay the bioavailability of coal for conversion to methane under defined laboratory conditions. Treatments included adding a well-characterized consortium of bacteria and methanogens (enriched from modern wetland sediments) and providing conditions to support endemic microbial activity. The contribution of desorbed methane in the bioassays was determined in treatments with bromoethane sulfonic acid, an inhibitor of microbial methanogenesis. The bioassay compared 16 subbituminous coal samples collected from beds in Texas (TX), Wyoming (WY), and Alaska (AK), and two bituminous coal samples from Pennsylvania (PA). New biogenic methane was observed in several samples of subbituminous coal with the microbial consortium added, but endemic activity was less commonly observed. The highest methane generation [80 µmol methane/g coal (56 scf/ton or 1.75 cm3/g)] was from a south TX coal sample that was collected from a non-gas-producing well. Subbituminous coals from the Powder River Basin, WY and North Slope Borough, AK contained more sorbed (original) methane than the TX coal sample and generated 0–23 µmol/g (up to 16 scf/ton or 0.5 cm3/g) new biogenic methane in the bioassay. Standard indicators of thermal maturity such as burial depth, nitrogen content, and calorific value did not explain differences in biogenic methane among subbituminous coal samples. No original methane was observed in two bituminous samples from PA, nor was any new methane generated in bioassays of these samples. The bioassay offers a new tool for assessing the potential of coal for biogenic methane generation, and provides a platform for studying the mechanisms involved in this economically important activity.
Pilot-scale testing of a leachbed for anaerobic digestion of livestock residues on-farm.
Yap, S D; Astals, S; Jensen, P D; Batstone, D J; Tait, S
2016-04-01
A leachbed is a relatively simple anaerobic digester suitable for high-solids residues and on-farm applications. However, performance characteristics and optimal configuration of leachbeds are not well-understood. In this study, two 200 L pilot-scale leachbeds fed with spent straw bedding from pigs/swine (methane potential, B0 = 195-218 L CH4 kg(-1) VS fed) were used to assess the effects of leachate recirculation mode (trickling vs. flood-and-drain) on the digestion performance. Results showed comparable substrate solubilisation extents (30-45% of total chemical oxygen demand fed) and methane conversion (50% of the B0) for the trickling and flood-and-drain modes, indicating that digestion performance was insensitive to the mode of leachate flow. However, the flood-and-drain leachbed mobilised more particulates into the leachate than the trickling leachbed, an undesirable outcome, because these particulates were mostly non-biodegradable. Inoculation with solid residues from a previous leachbed (inoculum-to-substrate ratio of 0.22 on a VS basis) hastened the leachbed start-up, but methane recovery remained at 50% of the B0 regardless of the leachate recirculation mode. Post-digestion testing indicated that the leachbeds may have been limited by microbial activity/inhibition. The high residual methane potential of leachate from the trickling (residual Bo = 732 ± 7 L CH4 kg(-1) VS fed) and flood-and-drain leachbeds (582 ± 8 L CH4 kg(-1) VS fed) indicated an opportunity for further processing of leachate via a separate methanogenic step. Overall, a trickling leachbed appeared to be more favourable than the flood-and-drain leachbed for treating spent bedding at farm-scale due to easier operation. Copyright © 2016 Elsevier Ltd. All rights reserved.
Federal Register 2010, 2011, 2012, 2013, 2014
2012-04-24
... Activities; Submission to OMB for Review and Approval; Comment Request; Landfill Methane Outreach Program... the electronic docket, go to www.regulations.gov . Title: Landfill Methane Outreach Program (Renewal... consolidated in 40 CFR part 9. Abstract: The Landfill Methane Outreach Program (LMOP), created by EPA as part...
Farrokhzadeh, Hasti; Hettiaratchi, J Patrick A; Jayasinghe, Poornima; Kumar, Sunil
2017-09-01
Aiming to improve conventional methane biofilter performance, a multiple-level aeration biofilter design is proposed. Laboratory flow-through column experiments were conducted to evaluate three actively-aerated methane biofilter configurations. Columns were aerated at one, two, and three levels of the bed depth, with air introduced at flow rates calculated from methane oxidation reaction stoichiometry. Inlet methane loading rates were increased in five stages between 6 and 18mL/min. The effects of methane feeding rate, levels of aeration, and residence time on methane oxidation rates were determined. Samples collected after completion of flow-through experiments were used to determine methane oxidation kinetic parameters, V max , K m , and methanotrophic community distribution across biofilter columns. Results obtained from mixed variances analysis and response surfaces, as well as methanotrophic activity data, suggested that, biofilter column with two aeration levels has the most even performance over time, maintaining 85.1% average oxidation efficiency over 95days of experiments. Copyright © 2017 Elsevier Ltd. All rights reserved.
Dai, Xiaohu; Li, Xiaoshuai; Zhang, Dong; Chen, Yinguang; Dai, Lingling
2016-09-01
It is necessary to find an appropriate strategy to simultaneously enhance the methane production and methane content in biogas from waste activated sludge (WAS) and grass co-digestion. In this study an efficient strategy, i.e., adjusting the initial pH 12 and C/N ratio 17/1, for simultaneous enhancement of methane production and methane content in biogas from WAS and perennial ryegrass co-digestion was reported. Experimental results indicated that the maximal methane production was 310mL/gVSadd at the optimum conditions after 30-d anaerobic digestion, which was, respectively, about 1.5- and 3.8-fold of the sole WAS and sole perennial ryegrass anaerobic digestion. Meanwhile, the methane content in biogas was about 74%, which was much higher than that of sole WAS (64%) or sole perennial ryegrass (54%) anaerobic digestion. Copyright © 2016 Elsevier Ltd. All rights reserved.
Evidence for methane in Martian meteorites
Blamey, Nigel J. F.; Parnell, John; McMahon, Sean; Mark, Darren F.; Tomkinson, Tim; Lee, Martin; Shivak, Jared; Izawa, Matthew R. M.; Banerjee, Neil R.; Flemming, Roberta L.
2015-01-01
The putative occurrence of methane in the Martian atmosphere has had a major influence on the exploration of Mars, especially by the implication of active biology. The occurrence has not been borne out by measurements of atmosphere by the MSL rover Curiosity but, as on Earth, methane on Mars is most likely in the subsurface of the crust. Serpentinization of olivine-bearing rocks, to yield hydrogen that may further react with carbon-bearing species, has been widely invoked as a source of methane on Mars, but this possibility has not hitherto been tested. Here we show that some Martian meteorites, representing basic igneous rocks, liberate a methane-rich volatile component on crushing. The occurrence of methane in Martian rock samples adds strong weight to models whereby any life on Mars is/was likely to be resident in a subsurface habitat, where methane could be a source of energy and carbon for microbial activity. PMID:26079798
Variations in Gas and Water Pulses at an Arctic Seep: Fluid Sources and Methane Transport
NASA Astrophysics Data System (ADS)
Hong, W.-L.; Torres, M. E.; Portnov, A.; Waage, M.; Haley, B.; Lepland, A.
2018-05-01
Methane fluxes into the oceans are largely dependent on the methane phase as it migrates upward through the sediments. Here we document decoupled methane transport by gaseous and aqueous phases in Storfjordrenna (offshore Svalbard) and propose a three-stage evolution model for active seepage in the region where gas hydrates are present in the shallow subsurface. In a preactive seepage stage, solute diffusion is the primary transport mechanism for methane in the dissolved phase. Fluids containing dissolved methane have high 87Sr/86Sr ratios due to silicate weathering in the microbial methanogenesis zone. During the active seepage stage, migration of gaseous methane results in near-seafloor gas hydrate formation and vigorous seafloor gas discharge with a thermogenic fingerprint. In the postactive seepage stage, the high concentration of dissolved lithium points to the contribution of a deeper-sourced aqueous fluid, which we postulate advects upward following cessation of gas discharge.
Evidence for methane in Martian meteorites.
Blamey, Nigel J F; Parnell, John; McMahon, Sean; Mark, Darren F; Tomkinson, Tim; Lee, Martin; Shivak, Jared; Izawa, Matthew R M; Banerjee, Neil R; Flemming, Roberta L
2015-06-16
The putative occurrence of methane in the Martian atmosphere has had a major influence on the exploration of Mars, especially by the implication of active biology. The occurrence has not been borne out by measurements of atmosphere by the MSL rover Curiosity but, as on Earth, methane on Mars is most likely in the subsurface of the crust. Serpentinization of olivine-bearing rocks, to yield hydrogen that may further react with carbon-bearing species, has been widely invoked as a source of methane on Mars, but this possibility has not hitherto been tested. Here we show that some Martian meteorites, representing basic igneous rocks, liberate a methane-rich volatile component on crushing. The occurrence of methane in Martian rock samples adds strong weight to models whereby any life on Mars is/was likely to be resident in a subsurface habitat, where methane could be a source of energy and carbon for microbial activity.
Metabolic stratification driven by surface and subsurface interactions in a terrestrial mud volcano.
Cheng, Ting-Wen; Chang, Yung-Hsin; Tang, Sen-Lin; Tseng, Ching-Hung; Chiang, Pei-Wen; Chang, Kai-Ti; Sun, Chih-Hsien; Chen, Yue-Gau; Kuo, Hung-Chi; Wang, Chun-Ho; Chu, Pao-Hsuan; Song, Sheng-Rong; Wang, Pei-Ling; Lin, Li-Hung
2012-12-01
Terrestrial mud volcanism represents the prominent surface geological feature, where fluids and hydrocarbons are discharged along deeply rooted structures in tectonically active regimes. Terrestrial mud volcanoes (MVs) directly emit the major gas phase, methane, into the atmosphere, making them important sources of greenhouse gases over geological time. Quantification of methane emission would require detailed insights into the capacity and efficiency of microbial metabolisms either consuming or producing methane in the subsurface, and establishment of the linkage between these methane-related metabolisms and other microbial or abiotic processes. Here we conducted geochemical, microbiological and genetic analyses of sediments, gases, and pore and surface fluids to characterize fluid processes, community assemblages, functions and activities in a methane-emitting MV of southwestern Taiwan. Multiple lines of evidence suggest that aerobic/anaerobic methane oxidation, sulfate reduction and methanogenesis are active and compartmentalized into discrete, stratified niches, resembling those in marine settings. Surface evaporation and oxidation of sulfide minerals are required to account for the enhanced levels of sulfate that fuels subsurface sulfate reduction and anaerobic methanotrophy. Methane flux generated by in situ methanogenesis appears to alter the isotopic compositions and abundances of thermogenic methane migrating from deep sources, and to exceed the capacity of microbial consumption. This metabolic stratification is sustained by chemical disequilibria induced by the mixing between upward, anoxic, methane-rich fluids and downward, oxic, sulfate-rich fluids.
Metabolic stratification driven by surface and subsurface interactions in a terrestrial mud volcano
Cheng, Ting-Wen; Chang, Yung-Hsin; Tang, Sen-Lin; Tseng, Ching-Hung; Chiang, Pei-Wen; Chang, Kai-Ti; Sun, Chih-Hsien; Chen, Yue-Gau; Kuo, Hung-Chi; Wang, Chun-Ho; Chu, Pao-Hsuan; Song, Sheng-Rong; Wang, Pei-Ling; Lin, Li-Hung
2012-01-01
Terrestrial mud volcanism represents the prominent surface geological feature, where fluids and hydrocarbons are discharged along deeply rooted structures in tectonically active regimes. Terrestrial mud volcanoes (MVs) directly emit the major gas phase, methane, into the atmosphere, making them important sources of greenhouse gases over geological time. Quantification of methane emission would require detailed insights into the capacity and efficiency of microbial metabolisms either consuming or producing methane in the subsurface, and establishment of the linkage between these methane-related metabolisms and other microbial or abiotic processes. Here we conducted geochemical, microbiological and genetic analyses of sediments, gases, and pore and surface fluids to characterize fluid processes, community assemblages, functions and activities in a methane-emitting MV of southwestern Taiwan. Multiple lines of evidence suggest that aerobic/anaerobic methane oxidation, sulfate reduction and methanogenesis are active and compartmentalized into discrete, stratified niches, resembling those in marine settings. Surface evaporation and oxidation of sulfide minerals are required to account for the enhanced levels of sulfate that fuels subsurface sulfate reduction and anaerobic methanotrophy. Methane flux generated by in situ methanogenesis appears to alter the isotopic compositions and abundances of thermogenic methane migrating from deep sources, and to exceed the capacity of microbial consumption. This metabolic stratification is sustained by chemical disequilibria induced by the mixing between upward, anoxic, methane-rich fluids and downward, oxic, sulfate-rich fluids. PMID:22739492
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.
Hao, Liping; Lü, Fan; Mazéas, Laurent; Desmond-Le Quéméner, Elie; Madigou, Céline; Guenne, Angéline; Shao, Liming; Bouchez, Théodore; He, Pinjing
2015-02-01
Ammonia inhibition represents a major operational issue for anaerobic digestion. In order to refine our understanding of the terminal catabolic steps in thermophilic anaerobic digestion under ammonia stress, we studied batch thermophilic acetate fed experiments at low (0.26 g L(-1)) and high (7.00 g L(-1)) Total Ammonia Nitrogen concentrations (TAN). Although methane production started immediately for all incubations and resulted in methane yields close to stoichiometric expectations, a 62-72% decrease of methanogenic rate was observed throughout the incubation at 7.00 g L(-1) of TAN compared to 0.26 g L(-1). Stable Isotope Probing analysis of active microbial communities in (13)C-acetate fed experiments coupled to automated ribosomal intergenic spacer analysis and 16S rDNA pyrotag sequencing confirmed that microbial communities were similar for both TAN conditions. At both TAN levels, the (13)C-labeled bacterial community was mainly affiliated to Clostridia-relatives, with OPB54 bacteria being the most abundant sequence in the heavy DNA 16S rDNA pyrotag library. Sequences closely related to Methanosarcina thermophila were also abundantly retrieved in the heavy DNA fractions, showing that this methanogen was still actively assimilating labeled carbon from acetate at free ammonia nitrogen concentrations up to 916 mg L(-1). Stable isotopic signature analysis of biogas, measured in unlabeled acetate fed experiments that were conducted in parallel, confirmed that acetoclastic methanogenic pathway was dominant at both ammonia concentrations. Our work demonstrates that, besides the syntrophic acetate oxidation pathway, acetoclastic methanogenesis catalyzed by Methanosarcina can also play a major role in methane production at high ammonia levels. Copyright © 2014 Elsevier Ltd. All rights reserved.
NASA Astrophysics Data System (ADS)
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 sources, Atmospheric Environment, 110, 151-162, doi.org/10.1016/j.atmosenv.2015.03.029.
Suwannoppadol, Suwat; Ho, Goen; Cord-Ruwisch, Ralf
2012-12-01
Sodium toxicity is a common problem causing inhibition of anaerobic digestion, and digesters treating highly concentrated wastes, such as food and municipal solid waste, and concentrated animal manure, are likely to suffer from partial or complete inhibition of methane-producing consortia, including methanogens. When grass clippings were added at the onset of anaerobic digestion of acetate containing a sodium concentration of 7.8 gNa(+)/L, a total methane production about 8L/L was obtained, whereas no methane was produced in the absence of grass leaves. In an attempt to narrow down which components of grass leaves caused decrease of sodium toxicity, different hypotheses were tested. Results revealed that betaine could be a significant compound in grass leaves causing reduction to sodium inhibition. Copyright © 2012 Elsevier Ltd. All rights reserved.
NASA Astrophysics Data System (ADS)
Ebrahimi, Ali; Or, Dani
2017-04-01
The sensitivity of the Earth's polar regions to raising global temperatures is reflected in rapidly changing hydrological processes with pronounced seasonal thawing of permafrost soil and increased biological activity. Of particular concern is the potential release of large amounts of soil carbon and the stimulation of other soil-borne GHG emissions such as methane. Soil methanotrophic and methanogenic microbial communities rapidly adjust their activity and spatial organization in response to permafrost thawing and a host of other environmental factors. Soil structural elements such as aggregates and layering and hydration status affect oxygen and nutrient diffusion processes thereby contributing to methanogenic activity within temporal anoxic niches (hotspots or hot-layers). We developed a mechanistic individual based model to quantify microbial activity dynamics within soil pore networks considering, hydration, temperature, transport processes and enzymatic activity associated with methane production in soil. The model was the upscaled from single aggregates (or hotspots) to quantifying emissions from soil profiles in which freezing/thawing processes provide macroscopic boundary conditions for microbial activity at different soil depths. The model distinguishes microbial activity in aerate bulk soil from aggregates (or submerged parts of the profile) for resolving methane production and oxidation rates. Methane transport pathways through soil by diffusion and ebullition of bubbles vary with hydration dynamics and affect emission patterns. The model links seasonal thermal and hydrologic dynamics with evolution of microbial community composition and function affecting net methane emissions in good agreement with experimental data. The mechanistic model enables systematic evaluation of key controlling factors in thawing permafrost and microbial response (e.g., nutrient availability, enzyme activity, PH) on long term methane emissions and carbon decomposition rates in the rapidly changing polar regions.
Synthesis of Titanium Oxycarbide from Titanium Slag by Methane-Containing Gas
NASA Astrophysics Data System (ADS)
Dang, Jie; Fatollahi-Fard, Farzin; Pistorius, Petrus Christiaan; Chou, Kuo-Chih
2018-02-01
In this study, reaction steps of a process for synthesis of titanium oxycarbide from titanium slag were demonstrated. This process involves the reduction of titanium slag by a methane-hydrogen-argon mixture at 1473 K (1200 °C) and the leaching of the reduced products by hydrofluoric acid near room temperature to remove the main impurity (Fe3Si). Some iron was formed by disproportionation of the main M3O5 phase before gaseous reduction started. Upon reduction, more iron formed first, followed by reduction of titanium dioxide to suboxides and eventually oxycarbide.
Karska-Wysocki, B; Mamet-Bratley, M D; Verly, W G
1976-01-01
After treatment with methyl or ethyl methane sulfonate, T7 amber mutants display a reduced capacity for recombination. Moreover, alkylation reduces recombination frequency involving markers on the right-hand side of the genetic map more than it reduces recombination frequency involving markers on the left-hand side. We interpret this to mean that alkylation can stop DNA injection at any point along the DNA molecule, and that T7 phage injects its DNA in a unique fashion starting from the end carrying the genes for early proteins. PMID:183007
A cryptic sulfur cycle driven by iron in the methane zone of marine sediment (Aarhus Bay, Denmark)
NASA Astrophysics Data System (ADS)
Holmkvist, Lars; Ferdelman, Timothy G.; Jørgensen, Bo Barker
2011-06-01
Sulfate reduction and sulfur-iron geochemistry were studied in 5-6 m deep gravity cores of Holocene mud from Aarhus Bay (Denmark). A goal was to understand whether sulfate is generated by re-oxidation of sulfide throughout the sulfate and methane zones, which might explain the abundance of active sulfate reducers deep below the main sulfate zone. Sulfate penetrated down to 130 cm where methane started to build up and where the concentration of free sulfide peaked at 5.5 mM. Below this sulfate-methane transition, sulfide diffused downwards to a sulfidization front at 520 cm depth, below which dissolved iron, Fe 2+, accumulated in the pore water. Sulfate reduction rates measured by 35S-tracer incubations in the sulfate zone were high due to high concentrations of reactive organic matter. Within the sulfate-methane transition, sulfate reduction was distinctly stimulated by the anaerobic oxidation of methane. In the methane zone below, sulfate remained at positive "background" concentrations of <0.5 mM down to the sulfidization front. Sulfate reduction decreased steeply to rates which at 300-500 cm depth were 0.2-1 pmol SO 42- cm -3 d -1, i.e., 4-5 orders of magnitude lower than rates measured near the sediment surface. The turn-over time of sulfate increased from 3 years at 12 cm depth to 100-1000 years down in the methane zone. Sulfate reduction in the methane zone accounted for only 0.1% of sulfate reduction in the entire sediment column and was apparently limited by the low pore water concentration of sulfate and the low availability of organic substrates. Amendment of the sediment with both sulfate and organic substrates immediately caused a 10- to 40-fold higher, "potential sulfate reduction" which showed that a physiologically intact community of sulfate reducing bacteria was present. The "background" sulfate concentration appears to be generated from the reaction of downwards diffusing sulfide with deeply buried Fe(III) species, such as poorly-reactive iron oxides or iron bound in reactive silicates. The oxidation of sulfide to sulfate in the sulfidic sediment may involve the formation of elemental sulfur and thiosulfate and their further disproportionation to sulfide and sulfate. The net reaction of sulfide and Fe(III) to form pyrite requires an additional oxidant, irrespective of the formation of sulfate. This could be CO 2 which is reduced with H 2 to methane. The methane subsequently diffuses upwards to become re-oxidized at the sulfate-methane transition and thereby removes excess reducing power and enables the formation of excess sulfate. We show here how the combination of these well-established sulfur-iron-carbon reactions may lead to the deep formation of sulfate and drive a cryptic sulfur cycle. The iron-rich post-glacial sediments underlying Holocene marine mud stimulate the strong sub-surface sulfide reoxidation observed in Aarhus Bay and are a result of the glacial to interglacial history of the Baltic Sea area. Yet, processes similar to the ones described here probably occur widespread in marine sediments, in particular along the ocean margins.
Methane oxidation coupled to oxygenic photosynthesis in anoxic waters
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
Recent decreases in fossil-fuel emissions of ethane and methane derived from firn air.
Aydin, Murat; Verhulst, Kristal R; Saltzman, Eric S; Battle, Mark O; Montzka, Stephen A; Blake, Donald R; Tang, Qi; Prather, Michael J
2011-08-10
Methane and ethane are the most abundant hydrocarbons in the atmosphere and they affect both atmospheric chemistry and climate. Both gases are emitted from fossil fuels and biomass burning, whereas methane (CH(4)) alone has large sources from wetlands, agriculture, landfills and waste water. Here we use measurements in firn (perennial snowpack) air from Greenland and Antarctica to reconstruct the atmospheric variability of ethane (C(2)H(6)) during the twentieth century. Ethane levels rose from early in the century until the 1980s, when the trend reversed, with a period of decline over the next 20 years. We find that this variability was primarily driven by changes in ethane emissions from fossil fuels; these emissions peaked in the 1960s and 1970s at 14-16 teragrams per year (1 Tg = 10(12) g) and dropped to 8-10 Tg yr(-1) by the turn of the century. The reduction in fossil-fuel sources is probably related to changes in light hydrocarbon emissions associated with petroleum production and use. The ethane-based fossil-fuel emission history is strikingly different from bottom-up estimates of methane emissions from fossil-fuel use, and implies that the fossil-fuel source of methane started to decline in the 1980s and probably caused the late twentieth century slow-down in the growth rate of atmospheric methane.
Mars Methane highs unrelated to comets
NASA Astrophysics Data System (ADS)
Roos-Serote, Maarten; Atreya, Sushil K.; Webster, Chris; Mahaffy, Paul
2016-10-01
Until the Curiosity Rover arrived at Mars, all measurements of methane were done by remote sensing, either from Earth or from orbiting spacecraft, using a variety of different instruments and under different observing conditions. The Curiosity Rover's Sample Analysis at Mars (SAM) / Tunable Laser Spectrometer (TLS) has carried out systematic measurements of martian methane from Gale crater for two consecutive martian years (31 - 33, starting in October 2012). Meteoric material interacts with the martian atmosphere when Mars passes through a meteoroid stream left behind by cometary bodies orbiting the Sun. Predictions show that 33 such events are likely to occur during the martian year. It has been suggested that the organics present in this material trigger the formation of methane in the atmosphere, and thus these events could possibly be an explanation for the observed variations in the methane abundance. In a recent paper, Fries et al. [2016] argued that all measurements of high methane concentrations are within 16 days of a predicted meteor shower event, and that as such there is a correlation. We present a new analysis including seven new data points that were not available previously. All these new measurements show low methane values. Some of the new measurements were deliberately taken at the same Ls when high values of methane were measured in the previous martian year, showing that the high methane measurements are likely not seasonal, as would be expected if they were connected to meteor shower events. In our analysis we take into account all the predicted meteor events and search for any correlation drawn between these events and the level of methane in the atmosphere. We conclude that whether we consider individual data points, apply statistical analysis, or consider different time spans between measurements and the occurrence of meteor events, or possible supply of organic material from comets, there is no evidence for such a correlation in the available data.
NASA Astrophysics Data System (ADS)
Römer, Miriam; Riedel, Michael; Scherwath, Martin; Heesemann, Martin; Spence, George D.
2016-09-01
Long-term monitoring over 1 year revealed high temporal variability of gas emissions at a cold seep in 1250 m water depth offshore Vancouver Island, British Columbia. Data from the North East Pacific Time series Underwater Networked Experiment observatory operated by Ocean Networks Canada were used. The site is equipped with a 260 kHz Imagenex sonar collecting hourly data, conductivity-temperature-depth sensors, bottom pressure recorders, current meter, and an ocean bottom seismograph. This enables correlation of the data and analyzing trigger mechanisms and regulating criteria of gas discharge activity. Three periods of gas emission activity were observed: (a) short activity phases of few hours lasting several months, (b) alternating activity and inactivity of up to several day-long phases each, and (c) a period of several weeks of permanent activity. These periods can neither be explained by oceanographic conditions nor initiated by earthquakes. However, we found a clear correlation of gas emission with bottom pressure changes controlled by tides. Gas bubbles start emanating during decreasing tidal pressure. Tidally induced pressure changes also influence the subbottom fluid system by shifting the methane solubility resulting in exsolution of gas during falling tides. These pressure changes affect the equilibrium of forces allowing free gas in sediments to emanate into the water column at decreased hydrostatic load. We propose a model for the fluid system at the seep, fueled by a constant subsurface methane flux and a frequent tidally controlled discharge of gas bubbles into the ocean, transferable to other gas emission sites in the world's oceans.
Thinking Like a Wildcatter: Prospecting for Methane in Arabia Terra, Mars
NASA Technical Reports Server (NTRS)
Allen, C. C.; Oehler, D. Z.
2005-01-01
Methane has been detected in the martian atmosphere at a concentration of approximately 10 ppb. The lifetime of such methane against decomposition by solar radiation is approximately 300 years, strongly suggesting that methane is currently being released to the atmosphere. By analogy to Earth, possible methane sources on Mars include active volcanism, hot springs, frozen methane clathrates, thermally-matured sedimentary organic matter, and extant microbial metabolism. The discovery of any one of these sources would revolutionize our understanding of Mars.
Temporal variation of aerobic methane oxidation over a tidal cycle in a wetland of northern Taiwan.
NASA Astrophysics Data System (ADS)
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 methanotrophy could be modulated to reach peak activity once the influence of saline water is reduced to a low level.
Grundner, Sebastian; Markovits, Monica A C; Li, Guanna; Tromp, Moniek; Pidko, Evgeny A; Hensen, Emiel J M; Jentys, Andreas; Sanchez-Sanchez, Maricruz; Lercher, Johannes A
2015-06-25
Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon-hydrogen bonds in methane and its subsequent transformation to methanol. The similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towards methanol, in both the enzyme system and copper-exchanged mordenite.
Changes in deep-sea carbonate-hosted microbial communities associated with high and low methane flux
NASA Astrophysics Data System (ADS)
Case, D. H.; Steele, J. A.; Chadwick, G.; Mendoza, G. F.; Levin, L. A.; Orphan, V. J.
2012-12-01
Methane seeps on continental shelves are rich in authigenic carbonates built of methane-derived carbon. These authigenic carbonates are home to micro- and macroscopic communities whose compositions are thus far poorly constrained but are known to broadly depend on local methane flux. The formation of authigenic carbonates is itself a result of microbial metabolic activity, as associations of anaerobic methane oxidizing archaea (ANME) and sulfate reducing bacteria (SRB) in the sediment subsurface increase both dissolved inorganic carbon (DIC) and alkalinity in pore waters. This 1:1 increase in DIC and alkalinity promotes the precipitation of authigenic carbonates. In this study, we performed in situ manipulations to test the response of micro- and macrofaunal communities to a change in methane flux. Methane-derived authigenic carbonates from two locations at Hydrate Ridge, OR, USA (depth range 595-604 mbsl), were transplanted from "active" cold seep sites (high methane flux) to "inactive" background sites (low methane flux), and vise versa, for one year. Community diversity surveys using T-RFLP and 16S rRNA clone libraries revealed how both bacterial and archaeal assemblages respond to this change in local environment, specifically demonstrating reproducible shifts in different ANME groups (ANME-1 vs. ANME-2). Animal assemblage composition also shifted during transplantation; gastropod representation increased (relative to control rocks) when substrates were moved from inactive to active sites and polychaete, crustacean and echinoderm representation increased when substrates were moved from active to inactive sites. Combined with organic and inorganic carbon δ13C measurements and mineralogy, this unique in situ experiment demonstrates that authigenic carbonates are viable habitats, hosting microbial and macrofaunal communities capable of responding to changes in external environment over relatively short time periods.
Reumer, Max; Harnisz, Monika; Lee, Hyo Jung; Reim, Andreas; Grunert, Oliver; Putkinen, Anuliina; Fritze, Hannu; Bodelier, Paul L E; Ho, Adrian
2018-02-01
Ombrotrophic peatlands are a recognized global carbon reservoir. Without restoration and peat regrowth, harvested peatlands are dramatically altered, impairing their carbon sink function, with consequences for methane turnover. Previous studies determined the impact of commercial mining on the physicochemical properties of peat and the effects on methane turnover. However, the response of the underlying microbial communities catalyzing methane production and oxidation have so far received little attention. We hypothesize that with the return of Sphagnum spp. postharvest, methane turnover potential and the corresponding microbial communities will converge in a natural and restored peatland. To address our hypothesis, we determined the potential methane production and oxidation rates in natural (as a reference), actively mined, abandoned, and restored peatlands over two consecutive years. In all sites, the methanogenic and methanotrophic population sizes were enumerated using quantitative PCR (qPCR) assays targeting the mcrA and pmoA genes, respectively. Shifts in the community composition were determined using Illumina MiSeq sequencing of the mcrA gene and a pmoA -based terminal restriction fragment length polymorphism (t-RFLP) analysis, complemented by cloning and sequence analysis of the mmoX gene. Peat mining adversely affected methane turnover potential, but the rates recovered in the restored site. The recovery in potential activity was reflected in the methanogenic and methanotrophic abundances. However, the microbial community composition was altered, being more pronounced for the methanotrophs. Overall, we observed a lag between the recovery of the methanogenic/methanotrophic activity and the return of the corresponding microbial communities, suggesting that a longer duration (>15 years) is needed to reverse mining-induced effects on the methane-cycling microbial communities. IMPORTANCE Ombrotrophic peatlands are a crucial carbon sink, but this environment is also a source of methane, an important greenhouse gas. Methane emission in peatlands is regulated by methane production and oxidation catalyzed by methanogens and methanotrophs, respectively. Methane-cycling microbial communities have been documented in natural peatlands. However, less is known of their response to peat mining and of the recovery of the community after restoration. Mining exerts an adverse impact on potential methane production and oxidation rates and on methanogenic and methanotrophic population abundances. Peat mining also induced a shift in the methane-cycling microbial community composition. Nevertheless, with the return of Sphagnum spp. in the restored site after 15 years, methanogenic and methanotrophic activity and population abundance recovered well. The recovery, however, was not fully reflected in the community composition, suggesting that >15 years are needed to reverse mining-induced effects. Copyright © 2018 American Society for Microbiology.
Nkemka, Valentine Nkongndem; Hao, Xiying
2018-04-01
The present laboratory study evaluated the sequential leach bed dry anaerobic digestion (DAD) of paunch under psychrophilic (22°C) and mesophilic (40°C) temperatures. Three leach bed reactors were operated under the mesophilic temperature in sequence at a solid retention time (SRT) of 40d with a new batch started 27d into the run of the previous one. A total of six batches were operated for 135d. The results showed that the mesophilic DAD of paunch was efficient, reaching methane yields of 126.9-212.1mLg -1 volatile solid (VS) and a VS reduction of 32.9-55.5%. The average daily methane production rate increased from 334.3mLd -1 to 571.4mLd -1 and 825.7mLd -1 when one, two and three leach bed reactors were in operation, respectively. The psychrophilic DAD of paunch was operated under a SRT of 100d and a total of three batches were performed in sequence for 300d with each batch starting after completion of the previous one. Improvements in the methane yield from 93.9 to 107.3 and 148.3mLg -1 VS and VS reductions of 24.8, 30.2 and 38.6% were obtained in the consecutive runs, indicating the adaptation of anaerobic microbes from mesophilic to psychrophilic temperatures. In addition, it took three runs for anaerobic microbes to reduce the volatile fatty acid accumulation observed in the first and second trials. This study demonstrates the potential of renewable energy recovery from paunch under psychrophilic and mesophilic temperatures. Crown Copyright © 2016. Published by Elsevier Ltd. All rights reserved.
In 't Zandt, Michiel H; Beckmann, Sabrina; Rijkers, Ruud; Jetten, Mike S M; Manefield, Mike; Welte, Cornelia U
2017-09-19
Coal mining is responsible for 11% of total anthropogenic methane emission thereby contributing considerably to climate change. Attempts to harvest coalbed methane for energy production are challenged by relatively low methane concentrations. In this study, we investigated whether nutrient and acetate amendment of a non-producing sub-bituminous coal well could transform the system to a methane source. We tracked cell counts, methane production, acetate concentration and geochemical parameters for 25 months in one amended and one unamended coal well in Australia. Additionally, the microbial community was analysed with 16S rRNA gene amplicon sequencing at 17 and 25 months after amendment and complemented by metagenome sequencing at 25 months. We found that cell numbers increased rapidly from 3.0 × 10 4 cells ml -1 to 9.9 × 10 7 in the first 7 months after amendment. However, acetate depletion with concomitant methane production started only after 12-19 months. The microbial community was dominated by complex organic compound degraders (Anaerolineaceae, Rhodocyclaceae and Geobacter spp.), acetoclastic methanogens (Methanothrix spp.) and fungi (Agaricomycetes). Even though the microbial community had the functional potential to convert coal to methane, we observed no indication that coal was actually converted within the time frame of the study. Our results suggest that even though nutrient and acetate amendment stimulated relevant microbial species, it is not a sustainable way to transform non-producing coal wells into bioenergy factories. © 2017 The Authors. Microbial Biotechnology published by John Wiley & Sons Ltd and Society for Applied Microbiology.
NASA Astrophysics Data System (ADS)
Takano, Hiroyuki; Izumiya, Koichi; Kumagai, Naokazu; Hashimoto, Koji
2011-07-01
The active catalysts for methane formation from the gas mixture of CO 2 + 4H 2 with almost 100% methane selectivity were prepared by reduction of the oxide mixture of NiO and ZrO 2 prepared by calcination of aqueous ZrO 2 sol with Sm(NO 3) 3 and Ni(NO 3) 2. The 50 at%Ni-50 at%(Zr-Sm oxide) catalyst consisting of 50 at%Ni-50 at%(Zr + Sm) with Zr/Sm = 5 calcined at 650 or 800 °C showed the highest activity for methanation. The active catalysts were Ni supported on tetragonal ZrO 2, and the activity for methanation increased by an increase in inclusion of Sm 3+ ions substituting Zr 4+ ions in the tetragonal ZrO 2 lattice as a result of an increase in calcination temperature. However, the increase in calcination temperature decreased BET surface area, metal dispersion and hydrogen uptake due to grain growth. Thus, the optimum calcination temperature existed.
Catalytic conversion of methane to methanol using Cu-zeolites.
Alayon, Evalyn Mae C; Nachtegaal, Maarten; Ranocchiari, Marco; van Bokhoven, Jeroen A
2012-01-01
The conversion of methane to value-added liquid chemicals is a promising answer to the imminent demand for fuels and chemical synthesis materials in the advent of a dwindling petroleum supply. Current technology requires high energy input for the synthesis gas production, and is characterized by low overall selectivity, which calls for alternative reaction routes. The limitation to achieve high selectivity is the high C-H bond strength of methane. High-temperature reaction systems favor gas-phase radical reactions and total oxidation. This suggests that the catalysts for methane activation should be active at low temperatures. The enzymatic-inspired metal-exchanged zeolite systems apparently fulfill this need, however, methanol yield is low and a catalytic process cannot yet be established. Homogeneous and heterogeneous catalytic systems have been described which stabilize the intermediate formed after the first C-H activation. The understanding of the reaction mechanism and the determination of the active metal sites are important for formulating strategies for the upgrade of methane conversion catalytic technologies.
Wang, Qilin; Sun, Jing; Zhang, Chang; Xie, Guo-Jun; Zhou, Xu; Qian, Jin; Yang, Guojing; Zeng, Guangming; Liu, Yiqi; Wang, Dongbo
2016-01-21
Anaerobic sludge digestion is the main technology for sludge reduction and stabilization prior to sludge disposal. Nevertheless, methane production from anaerobic digestion of waste activated sludge (WAS) is often restricted by the poor biochemical methane potential and slow hydrolysis rate of WAS. This work systematically investigated the effect of PHA levels of WAS on anaerobic methane production, using both experimental and mathematical modeling approaches. Biochemical methane potential tests showed that methane production increased with increased PHA levels in WAS. Model-based analysis suggested that the PHA-based method enhanced methane production by improving biochemical methane potential of WAS, with the highest enhancement being around 40% (from 192 to 274 L CH4/kg VS added; VS: volatile solid) when the PHA levels increased from 21 to 143 mg/g VS. In contrast, the hydrolysis rate (approximately 0.10 d(-1)) was not significantly affected by the PHA levels. Economic analysis suggested that the PHA-based method could save $1.2/PE/y (PE: population equivalent) in a typical wastewater treatment plant (WWTP). The PHA-based method can be easily integrated into the current WWTP to enhance methane production, thereby providing a strong support to the on-going paradigm shift in wastewater management from pollutant removal to resource recovery.
Liu, Yiwen; Wang, Qilin; Zhang, Yaobin; Ni, Bing-Jie
2015-02-05
Anaerobic digestion has been widely applied for waste activated sludge (WAS) treatment. However, methane production from anaerobic digestion of WAS is usually limited by the slow hydrolysis rate and/or poor biochemical methane potential of WAS. This work systematically studied the effects of three different types of zero valent iron (i.e., iron powder, clean scrap and rusty scrap) on methane production from WAS in anaerobic digestion, by using both experimental and mathematical approaches. The results demonstrated that both the clean and the rusty iron scrap were more effective than the iron powder for improving methane production from WAS. Model-based analysis showed that ZVI addition significantly enhanced methane production from WAS through improving the biochemical methane potential of WAS rather than its hydrolysis rate. Economic analysis indicated that the ZVI-based technology for enhancing methane production from WAS is economically attractive, particularly considering that iron scrap can be freely acquired from industrial waste. Based on these results, the ZVI-based anaerobic digestion process of this work could be easily integrated with the conventional chemical phosphorus removal process in wastewater treatment plant to form a cost-effective and environment-friendly approach, enabling maximum resource recovery/reuse while achieving enhanced methane production in wastewater treatment system.
Liu, Yiwen; Wang, Qilin; Zhang, Yaobin; Ni, Bing-Jie
2015-01-01
Anaerobic digestion has been widely applied for waste activated sludge (WAS) treatment. However, methane production from anaerobic digestion of WAS is usually limited by the slow hydrolysis rate and/or poor biochemical methane potential of WAS. This work systematically studied the effects of three different types of zero valent iron (i.e., iron powder, clean scrap and rusty scrap) on methane production from WAS in anaerobic digestion, by using both experimental and mathematical approaches. The results demonstrated that both the clean and the rusty iron scrap were more effective than the iron powder for improving methane production from WAS. Model-based analysis showed that ZVI addition significantly enhanced methane production from WAS through improving the biochemical methane potential of WAS rather than its hydrolysis rate. Economic analysis indicated that the ZVI-based technology for enhancing methane production from WAS is economically attractive, particularly considering that iron scrap can be freely acquired from industrial waste. Based on these results, the ZVI-based anaerobic digestion process of this work could be easily integrated with the conventional chemical phosphorus removal process in wastewater treatment plant to form a cost-effective and environment-friendly approach, enabling maximum resource recovery/reuse while achieving enhanced methane production in wastewater treatment system. PMID:25652244
Wang, Qilin; Sun, Jing; Zhang, Chang; Xie, Guo-Jun; Zhou, Xu; Qian, Jin; Yang, Guojing; Zeng, Guangming; Liu, Yiqi; Wang, Dongbo
2016-01-01
Anaerobic sludge digestion is the main technology for sludge reduction and stabilization prior to sludge disposal. Nevertheless, methane production from anaerobic digestion of waste activated sludge (WAS) is often restricted by the poor biochemical methane potential and slow hydrolysis rate of WAS. This work systematically investigated the effect of PHA levels of WAS on anaerobic methane production, using both experimental and mathematical modeling approaches. Biochemical methane potential tests showed that methane production increased with increased PHA levels in WAS. Model-based analysis suggested that the PHA-based method enhanced methane production by improving biochemical methane potential of WAS, with the highest enhancement being around 40% (from 192 to 274 L CH4/kg VS added; VS: volatile solid) when the PHA levels increased from 21 to 143 mg/g VS. In contrast, the hydrolysis rate (approximately 0.10 d−1) was not significantly affected by the PHA levels. Economic analysis suggested that the PHA-based method could save $1.2/PE/y (PE: population equivalent) in a typical wastewater treatment plant (WWTP). The PHA-based method can be easily integrated into the current WWTP to enhance methane production, thereby providing a strong support to the on-going paradigm shift in wastewater management from pollutant removal to resource recovery. PMID:26791952
NASA Astrophysics Data System (ADS)
Liu, Yiwen; Wang, Qilin; Zhang, Yaobin; Ni, Bing-Jie
2015-02-01
Anaerobic digestion has been widely applied for waste activated sludge (WAS) treatment. However, methane production from anaerobic digestion of WAS is usually limited by the slow hydrolysis rate and/or poor biochemical methane potential of WAS. This work systematically studied the effects of three different types of zero valent iron (i.e., iron powder, clean scrap and rusty scrap) on methane production from WAS in anaerobic digestion, by using both experimental and mathematical approaches. The results demonstrated that both the clean and the rusty iron scrap were more effective than the iron powder for improving methane production from WAS. Model-based analysis showed that ZVI addition significantly enhanced methane production from WAS through improving the biochemical methane potential of WAS rather than its hydrolysis rate. Economic analysis indicated that the ZVI-based technology for enhancing methane production from WAS is economically attractive, particularly considering that iron scrap can be freely acquired from industrial waste. Based on these results, the ZVI-based anaerobic digestion process of this work could be easily integrated with the conventional chemical phosphorus removal process in wastewater treatment plant to form a cost-effective and environment-friendly approach, enabling maximum resource recovery/reuse while achieving enhanced methane production in wastewater treatment system.
NASA Astrophysics Data System (ADS)
Wang, Qilin; Sun, Jing; Zhang, Chang; Xie, Guo-Jun; Zhou, Xu; Qian, Jin; Yang, Guojing; Zeng, Guangming; Liu, Yiqi; Wang, Dongbo
2016-01-01
Anaerobic sludge digestion is the main technology for sludge reduction and stabilization prior to sludge disposal. Nevertheless, methane production from anaerobic digestion of waste activated sludge (WAS) is often restricted by the poor biochemical methane potential and slow hydrolysis rate of WAS. This work systematically investigated the effect of PHA levels of WAS on anaerobic methane production, using both experimental and mathematical modeling approaches. Biochemical methane potential tests showed that methane production increased with increased PHA levels in WAS. Model-based analysis suggested that the PHA-based method enhanced methane production by improving biochemical methane potential of WAS, with the highest enhancement being around 40% (from 192 to 274 L CH4/kg VS added; VS: volatile solid) when the PHA levels increased from 21 to 143 mg/g VS. In contrast, the hydrolysis rate (approximately 0.10 d-1) was not significantly affected by the PHA levels. Economic analysis suggested that the PHA-based method could save $1.2/PE/y (PE: population equivalent) in a typical wastewater treatment plant (WWTP). The PHA-based method can be easily integrated into the current WWTP to enhance methane production, thereby providing a strong support to the on-going paradigm shift in wastewater management from pollutant removal to resource recovery.
Influence of trace substances on methanation catalysts used in dynamic biogas upgrading.
Jürgensen, Lars; Ehimen, Ehiaze Augustine; Born, Jens; Holm-Nielsen, Jens Bo; Rooney, David
2015-02-01
The aim of this work was to study the possible deactivation effects of biogas trace ammonia concentrations on methanation catalysts. It was found that small amounts of ammonia led to a slight decrease in the catalyst activity. A decrease in the catalyst deactivation by carbon formation was also observed, with ammonia absorbed on the active catalyst sites. This was via a suppression of the carbon formation and deposition on the catalyst, since it requires a higher number of active sites than for the methanation of carbon oxides. From the paper findings, no special pretreatment for ammonia removal from the biogas fed to a methanation process is required. Copyright © 2014 Elsevier Ltd. All rights reserved.
Exposure to polystyrene nanoplastic leads to inhibition of anaerobic digestion system.
Fu, Shan-Fei; Ding, Jian-Nan; Zhang, Yun; Li, Yi-Fei; Zhu, Rong; Yuan, Xian-Zheng; Zou, Hua
2018-06-01
In this study, impacts of nanoplastic on the pure and mixed anaerobic digestion systems were investigated. Results showed the growth and metabolism of Acetobacteroides hydrogenigenes were partly inhibited by nanoplastic existed in the pure anaerobic digestion system. The anaerobic digestion of sewage sludge was also obviously inhibited by nanoplastic existed in the mixed anaerobic digestion system. Both the methane yield and methane production rate of the mixed anaerobic digestion system showed negative correlation with the nanoplastic concentration. Compared with anaerobic digestion system without nanoplastic, methane yield and maximum daily methane yield at the nanoplastic concentration of 0.2g/L decreased for 14.4% and 40.7%, respectively. In addition, the start-up of mixed anaerobic digestion system was prolonged by addition of nanoplastic. Microbial community structure analysis indicated the microbial community structures were also affected by nanoplastic existed in the system. At the nanoplastic concentration of 0.2g/L, the relative abundances of family Cloacamonaceae, Porphyromonadaceae, Anaerolinaceae and Gracilibacteraceae decreased partly. Conversely, the relative abundances of family Anaerolinaceae, Clostridiaceae, Geobacteraceae, Dethiosulfovibrionaceae and Desulfobulbaceae improved partly. Copyright © 2017 Elsevier B.V. All rights reserved.
NASA Technical Reports Server (NTRS)
Khalil, M. A. K.; Rasmussen, R. A.; Moraes, F.
1993-01-01
Between 1979 and 1992 we took some 120,000 measurements of atmospheric methane at Cape Meares on the Oregon coast. The site is representative of methane concentrations in the northern latitudes (from 30 deg N to 90 deg N). The average concentration during the experiment was 1698 parts per billion by volume (ppbv). Methane concentration increased by 190 ppbv (or 11.9 percent) during the 13-year span of the experiment. The rate of increase was about 20 +/- 4 ppbv/yr in the first 2 yr and 10 +/- 2 ppbv/yr in the last 2 yr of the experiment, suggesting a substantial decline in the trend at northern middle and high latitudes. Prominent seasonal cycles were observed. During the year, the concentration stays more or less constant until May and then starts falling, reaching lowest levels in July and August, then rises rapidly to nearly maximum concentrations in October. Interannual variations with small amplitudes of 2-3 ppbv occur with periods of 1.4 and 6.5 yr.
Motte, J-C; Escudié, R; Bernet, N; Delgenes, J-P; Steyer, J-P; Dumas, C
2013-09-01
Among all the process parameters of solid-state anaerobic digestion (SS-AD), total solid content (TS), inoculation (S/X ratio) and size of the organic solid particles can be optimized to improve methane yield and process stability. To evaluate the effects of each parameter and their interactions on methane production, a three level Box-Behnken experimental design was implemented in SS-AD batch tests degrading wheat straw by adjusting: TS content from 15% to 25%, S/X ratio (in volatile solids) between 28 and 47 and particle size with a mean diameter ranging from 0.1 to 1.4mm. A dynamic analysis of the methane production indicates that the S/X ratio has only an effect during the start-up phase of the SS-AD. During the growing phase, TS content becomes the main parameter governing the methane production and its strong interaction with the particle size suggests the important role of water compartmentation on SS-AD. Copyright © 2013 Elsevier Ltd. All rights reserved.
An optimizing start-up strategy for a bio-methanator.
Sbarciog, Mihaela; Loccufier, Mia; Vande Wouwer, Alain
2012-05-01
This paper presents an optimizing start-up strategy for a bio-methanator. The goal of the control strategy is to maximize the outflow rate of methane in anaerobic digestion processes, which can be described by a two-population model. The methodology relies on a thorough analysis of the system dynamics and involves the solution of two optimization problems: steady-state optimization for determining the optimal operating point and transient optimization. The latter is a classical optimal control problem, which can be solved using the maximum principle of Pontryagin. The proposed control law is of the bang-bang type. The process is driven from an initial state to a small neighborhood of the optimal steady state by switching the manipulated variable (dilution rate) from the minimum to the maximum value at a certain time instant. Then the dilution rate is set to the optimal value and the system settles down in the optimal steady state. This control law ensures the convergence of the system to the optimal steady state and substantially increases its stability region. The region of attraction of the steady state corresponding to maximum production of methane is considerably enlarged. In some cases, which are related to the possibility of selecting the minimum dilution rate below a certain level, the stability region of the optimal steady state equals the interior of the state space. Aside its efficiency, which is evaluated not only in terms of biogas production but also from the perspective of treatment of the organic load, the strategy is also characterized by simplicity, being thus appropriate for implementation in real-life systems. Another important advantage is its generality: this technique may be applied to any anaerobic digestion process, for which the acidogenesis and methanogenesis are, respectively, characterized by Monod and Haldane kinetics.
The radical mechanism of biological methane synthesis by methyl-coenzyme M reductase
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wongnate, T.; Sliwa, D.; Ginovska, B.
2016-05-19
Methyl-coenzyme M reductase (MCR), the rate-limiting enzyme in methanogenesis and anaerobic methane oxidation, is responsible for the production of over one billion tons of methane per year. The mechanism of methane synthesis is unknown, with the two leading proposals involving either a methyl-nickel(III) (Mechanism I) or methyl radical/Ni(II)-thiolate (Mechanism II) intermediate(s). When the reaction between the active Ni(I) enzyme with substrates was studied by transient kinetic, spectroscopic and computational methods, formation of an EPR-silent Ni(II)-thiolate intermediate was positively identified by magnetic circular dichroism spectroscopy. There was no evidence for an EPR-active methyl-Ni(III) species. Temperature-dependent transient kinetic studies revealed that themore » activation energy for the initial catalytic step closely matched the value computed by density functional theory for Mechanism II. Thus, our results demonstrate that biological methane synthesis occurs by generation of a methyl radical.« less
Selective anaerobic oxidation of methane enables direct synthesis of methanol.
Sushkevich, Vitaly L; Palagin, Dennis; Ranocchiari, Marco; van Bokhoven, Jeroen A
2017-05-05
Direct functionalization of methane in natural gas remains a key challenge. We present a direct stepwise method for converting methane into methanol with high selectivity (~97%) over a copper-containing zeolite, based on partial oxidation with water. The activation in helium at 673 kelvin (K), followed by consecutive catalyst exposures to 7 bars of methane and then water at 473 K, consistently produced 0.204 mole of CH 3 OH per mole of copper in zeolite. Isotopic labeling confirmed water as the source of oxygen to regenerate the zeolite active centers and renders methanol desorption energetically favorable. On the basis of in situ x-ray absorption spectroscopy, infrared spectroscopy, and density functional theory calculations, we propose a mechanism involving methane oxidation at Cu II oxide active centers, followed by Cu I reoxidation by water with concurrent formation of hydrogen. Copyright © 2017, American Association for the Advancement of Science.
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.
Zhu, Wenjun; Jin, Jianhui; Chen, Xiao; Li, Chuang; Wang, Tonghua; Tsang, Chi-Wing; Liang, Changhai
2018-02-01
Effective utilization of coal bed methane is very significant for energy utilization and environment protection. Catalytic combustion of methane is a promising way to eliminate trace amounts of oxygen in the coal bed methane and the key to this technology is the development of high-efficiency catalysts. Herein, we report a series of Ce 1-x La x O 2-δ (x = 0-0.8) monolithic catalysts for the catalytic combustion of methane, which are prepared by citric acid method. The structural characterization shows that the substitution of La enhance the oxygen vacancy concentration and reducibility of the supports and promote the migration of the surface oxygen, as a result improve the catalytic activity of CeO 2 . M-Ce 0.8 La 0.2 O 2-δ (monolithic catalyst, Ce 0.8 La 0.2 O 2-δ coated on cordierite honeycomb) exhibits outstanding activity for methane combustion, and the temperature for 10 and 90% methane conversion are 495 and 580 °C, respectively. Additionally, Ce 0.8 La 0.2 O 2-δ monolithic catalyst presents excellent stability at high temperature. These Ce 1-x La x O 2-δ monolithic materials with a small amount of La incorporation therefore show promises as highly efficient solid solution catalysts for lean-oxygen methane combustion. Graphical abstract ᅟ.
Methane emission from flooded soils - from microorganisms to the atmosphere
NASA Astrophysics Data System (ADS)
Conrad, Ralf
2016-04-01
Methane is an important greenhouse gas that is affected by anthropogenic activity. The annual budget of atmospheric methane, which is about 600 million tons, is by more than 75% produced by methanogenic archaea. These archaea are the end-members of a microbial community that degrades organic matter under anaerobic conditions. Flooded rice fields constitute a major source (about 10%) of atmospheric methane. After flooding of soil, anaerobic processes are initiated, finally resulting in the disproportionation of organic matter to carbon dioxide and methane. This process occurs in the bulk soil, on decaying organic debris and in the rhizosphere. The produced methane is mostly ventilated through the plant vascular system into the atmosphere. This system also allows the diffusion of oxygen into the rizosphere, where part of the produced methane is oxidized by aerobic methanotrophic bacteria. More than 50% of the methane production is derived from plant photosynthetic products and is formed on the root surface. Methanocellales are an important group of methanogenic archaea colonizing rice roots. Soils lacking this group seem to result in reduced root colonization and methane production. In rice soil methane is produced by two major paths of methanogenesis, the hydrogenotrophic one reducing carbon dioxide to methane, and the aceticlastic one disproportionating acetate to methane and carbon dioxide. Theoretically, at least two third of the methane should be produced by aceticlastic and the rest by hydrogenotrophic methanogenesis. In nature, however, the exact contribution of the two paths can vary from zero to 100%. Several environmental factors, such as temperature and quality of organic matter affect the path of methane production. The impact of these factors on the composition and activity of the environmental methanogenic microbial community will be discussed.
Biochemical methane potential (BMP) of artichoke waste: the inoculum effect.
Fabbri, Andrea; Serranti, Silvia; Bonifazi, Giuseppe
2014-03-01
The aim of this work was to investigate anaerobic digestibility of artichoke waste resulting from industrial transformation. A series of batch anaerobic digestion tests was performed in order to evaluate the biochemical methane potential of the matrix in respect of the process. A comparison of the different performances of the laboratory-scale reactors operating in mesophilic conditions and utilizing three different values of the inoculum/substrate ratio was carried out. The best performance was achieved with an inoculum/substrate ratio of 2. Artichoke-processing byproducts showed a classical organic waste decomposition behaviour: a fast start-up phase, an acclimation stage, and a final stabilization phase. Following this approach, artichoke waste reached chemical oxygen demand removal of about 90% in 40 days. The high methane yield (average 408.62 mL CH4 gvs (-1) voltatile solids), makes artichoke waste a good product to be utilized in anaerobic digestion plants for biogas production.
Mahajan, Devinder; Servio, Phillip; Jones, Keith W.; Feng, Huan; Winters, William J.; Taylor, C.E.; Kwwan, J.T.
2004-01-01
We have presented a summary of measurements on the physical properties of sediments relevant to methane hydrate recovery. The data includes not only geotechnical determinations, but also the CMT data that gives porosity values and pathways through the sediment material. The results show that CMT techniques can be used to study sediment properties on a micrometer-size scale. Since the technique is non-destructive, changes in the sediment microstructures as a function of pressure and temperature can be measured. It is also feasible to look at formation of methane hydrates in the sediment structure as has already been demonstrated [7–9]. A longer term challenge is to start from the microscale data and calculate the macroscopic quantities shown in Table 2. We also note that the CMT measurements help in identification of different minerals found in the sediments. This feature of CMT was not exploited in this survey.
Binding of methane to activated mineral surfaces - a methane sink on Mars?
NASA Astrophysics Data System (ADS)
Nørnberg, P.; Knak Jensen, S. J.; Skibsted, J.; Jakobsen, H. J.; ten Kate, I. L.; Gunnlaugsson, H. P.; Merrison, J. P.; Finster, K.; Bak, Ebbe; Iversen, J. J.; Kondrup, J. C.
2015-10-01
Tumbling experiments that simulate the wind erosion of quartz grains in an atmosphere of 13 C-enriched methane are reported. The eroded grains are analyzed by 13C and 29 Si solid-state NMR techniques after several months of tumbling. The analysis shows that methane has reacted with the eroded surface to form covalent Si-CH3 bonds, which stay intact for temperatures up to at least 250oC. These findings offer a model for a methane sink that might explain the fast disappearance of methane on Mars.
NASA Astrophysics Data System (ADS)
Alden, C. B.; Coburn, S.; Wright, R.; Baumann, E.; Cossel, K.; Sweeney, C.; Ghosh, S.; Newbury, N.; Prasad, K.; Coddington, I.; Rieker, G. B.
2017-12-01
Advances in natural gas extraction technology have led to increased US production and transport activity, and as a consequence, an increased need for monitoring of methane leaks. Current leak detection methods provide time snapshots, and not continuous, time-varying estimates of emissions. Most approaches also require specific atmospheric conditions, operators, or the use of a tracer gas, requiring site access. Given known intermittency in fugitive methane emissions, continuous monitoring is a critical need for emissions mitigation. We present a novel leak detection method that employs dual frequency comb spectrometry to offer continuous, autonomous, leak detection and quantification over square-km scale areas. The spectrometer is situated in a field of natural gas pads, and a series of retroreflectors around the field direct light back to a detector. The laser light spans 1620-1680 nm with 0.002 nm line spacing, measuring thousands of individual absorption features from multiple species. The result is high-stability trace gas (here CH4, CO2, and H2O) measurements over long (1 km+) open paths through the atmosphere. Measurements are used in an atmospheric inversion to estimate the time variability of emissions at each location of interest. Importantly, the measurement framework and inversion solve explicitly for background concentrations, which vary rapidly in fields of active oil and gas production. We present the results of controlled-leak field tests in rural Colorado. We demonstrate the ability to locate and size a leak located 1 km away from the spectrometer and varying in strength from 1.5 to 7.7 g/min, resulting in mean atmospheric enhancements of 20 ppb. The inversion correctly identifies when the leak turned on and off over a 24-hour period, and determines the mean leak strength to within 10% of the true controlled rate. We further demonstrate the ability of the system to correctly locate and size the start and end of simultaneous 2.7 to 4.8 g/min leaks from 2 sources in a field of 5 potential leak locations. Finally, we present the results of leak-detection tests in active oil and gas fields in the Denver Julesburg Basin, where background methane is complex.
Pedersen, Karsten
2013-01-01
It was previously concluded that opposing gradients of sulphate and methane, observations of 16S ribosomal DNA sequences displaying great similarity to those of anaerobic methane-oxidizing Archaea and a peak in sulphide concentration in groundwater from a depth of 250–350 m in Olkiluoto, Finland, indicated proper conditions for methane oxidation with sulphate. In the present research, pressure-resistant, gas-tight circulating systems were constructed to enable the investigation of attached and unattached anaerobic microbial populations from a depth of 327 m in Olkiluoto under in situ pressure (2.4 MPa), diversity, dissolved gas and chemistry conditions. Three parallel flow cell cabinets were configured to allow observation of the influence on microbial metabolic activity of 11 mℳ methane, 11 mℳ methane plus 10 mℳ H2 or 2.1 mℳ O2 plus 7.9 mℳ N2 (that is, air). The concentrations of these gases and of organic acids and carbon, sulphur chemistry, pH and Eh, ATP, numbers of cultivable micro-organisms, and total numbers of cells and bacteriophages were subsequently recorded under batch conditions for 105 days. The system containing H2 and methane displayed microbial reduction of 0.7 mℳ sulphate to sulphide, whereas the system containing only methane resulted in 0.2 mℳ reduced sulphate. The system containing added air became inhibited and displayed no signs of microbial activity. Added H2 and methane induced increasing numbers of lysogenic bacteriophages per cell. It appears likely that a microbial anaerobic methane-oxidizing process coupled to acetate formation and sulphate reduction may be ongoing in aquifers at a depth of 250–350 m in Olkiluoto. PMID:23235288
Grundner, Sebastian; Markovits, Monica A. C.; Li, Guanna; ...
2015-06-25
Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane and its subsequent transformation to methanol. In conclusion, the similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towardsmore » methanol, in both the enzyme system and copper-exchanged mordenite.« less
Grundner, Sebastian; Markovits, Monica A.C.; Li, Guanna; Tromp, Moniek; Pidko, Evgeny A.; Hensen, Emiel J.M.; Jentys, Andreas; Sanchez-Sanchez, Maricruz; Lercher, Johannes A.
2015-01-01
Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane and its subsequent transformation to methanol. The similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towards methanol, in both the enzyme system and copper-exchanged mordenite. PMID:26109507
A Possible Sink for Methane on Mars
NASA Astrophysics Data System (ADS)
Nørnberg, P.; Jensen, S. J. K.; Skibsted, J.; Jakobsen, H. J.; ten Kate, I. L.; Gunnlaugsson, H. P.; Merrison, J. P.; Finster, K.; Bak, E.; Iversen, J. J.; Kondrup, J. C.
2014-07-01
Mechanical simulated wind activation of mineral surfaces act as a trap for Methane through formation of covalent Si-C bonds stable up to temperatures above 250 C. This mechanism is proposed as a Methane sink on Mars.
Solubility of crude oil in methane as a function of pressure and temperature
Price, L.C.; Wenger, L.M.; Ging, T.; Blount, C.W.
1983-01-01
The solubility of a 44?? API (0.806 sp. gr.) whole crude oil has been measured in methane with water present at temperatures of 50 to 250??C and pressures of 740 to 14,852 psi, as have the solubilities of two high molecular weight petroleum distillation fractions at temperatures of 50 to 250??C and pressures of 4482 to 25,266 psi. Both increases in pressure and temperature increase the solubility of crude oil and petroleum distillation fractions in methane, the effect of pressure being greater than that of temperature. Unexpectedly high solubility levels (0.5-1.5 grams of oil per liter of methane-at laboratory temperature and pressure) were measured at moderate conditions (50-200??C and 5076-14504 psi). Similar results were found for the petroleum distillation fractions, one of which was the highest molecular weight material of petroleum (material boiling above 266??C at 6 microns pressure). Unexpectedly mild conditions (100??C and 15,200 psi; 200??C and 7513 psi) resulted in cosolubility of crude oil and methane. Under these conditions, samples of the gas-rich phase gave solubility values of 4 to 5 g/l, or greater. Qualitative analyses of the crude-oil solute samples showed that at low pressure and temperature equilibration conditions, the solute condensate would be enriched in C5-C15 range hydrocarbons and in saturated hydrocarbons in the C15+ fraction. With increases in temperature and especially pressure, these tendencies were reversed, and the solute condensate became identical to the starting crude oil. The data of this study, compared to that of previous studies, shows that methane, with water present, has a much greater carrying capacity for crude oil than in dry systems. The presence of water also drastically lowers the temperature and pressure conditions required for cosolubility. The data of this and/or previous studies demonstrate that the addition of carbon dioxide, ethane, propane, or butane to methane also has a strong positive effect on crude oil solubility, as does the presence of fine grained rocks. The n-paraffin distributions (as well as the overall composition) of the solute condensates are controlled by the temperature and pressure of solution and exsolution, as well as by the composition of the original starting material. It appears quite possible that primary migration by gaseous solution could 'strip' a source rock of crude-oil like components leaving behind a bitumen totally unlike the migrated crude oil. The data of this study demonstrate previous criticisms of primary petroleum migration by gas solution are invalid; that primary migration by gaseous solution cannot occur because methane cannot dissolve sufficient volumes of crude oil or cannot dissolve the highest molecular weight components of petroleum (tars and asphaltenes). ?? 1983.
Lee, C; Araujo, R C; Koenig, K M; Beauchemin, K A
2017-08-01
A finishing feedlot study was conducted with beef steers to determine effects of encapsulated nitrate (EN) on growth performance, carcass characteristics, methane production, and nitrate (NO) residues in tissues. The 132 crossbred steers were backgrounded in a feedlot for 91 d and transitioned for 28 days to the high-concentrate diets evaluated in the present study, maintaining the treatment and pen assignments designated at the start of the backgrounding period. The steers were initially assigned to 22 pens (6 animals per pen) in a randomized complete block design with BW (18 pens) and animals designated for methane measurement (4 pens) as blocking factors. Five animals in each pen designated for methane measurement (total of 20 animals) were monitored for methane emissions in respiratory chambers twice during the experiment. Pens received 3 dietary treatments (7 pens each): Control, a finishing diet supplemented with urea; 1.25% EN, control diet supplemented with 1.25% encapsulated NO in dietary DM that partially replaced urea; and 2.5% EN, control diet supplemented with 2.5% EN (DM basis) fully replacing urea. The final pen designated only for methane measurement received a fourth dietary treatment, 2.3% UEN, the control diet supplemented with unencapsulated NO (UEN) fully replacing urea. The cattle weighed 449 ± SD 32 kg at the start of the 150-d finishing period. The 2.5% EN diet decreased ( < 0.01) DMI compared with Control and 1.25% EN diets. Feeding EN tended to increase ( = 0.092) ADG compared with Control, and G:F was improved ( < 0.01) for EN compared with Control. No differences in methane production (g/d) and yield (g/kg DMI) were observed among treatments. Inclusion of EN in the diets increased ( ≤ 0.03) sorting in favor of large and medium particles and against small and fine particles. Plasma NO and NO concentrations were elevated ( < 0.01) with EN in a dose-response manner, but total blood methemoglobin levels for all treatments were low, below the detection limit. Feeding EN increased ( < 0.01) NO concentrations of samples from muscle, fat, liver, and kidney; NO concentrations of these tissues were similar between 1.25% EN and 2.3% UEN. In conclusion, inclusion of 2.5% EN in a finishing diet (DM basis; about 2% NO) did not cause NO toxicity or any health problems in the long term. In comparison with supplemental urea, feeding EN improved feed efficiency despite increases in sorting against dietary EN.
Anaerobic oxidation of methane in the Concepción Methane Seep Area, Chilean continental margin
NASA Astrophysics Data System (ADS)
Steeb, P.; Linke, P.; Scholz, F.; Schmidt, M.; Liebetrau, V.; Treude, T.
2012-04-01
Within subduction zones of active continental margins, large amounts of methane can be mobilized by dewatering processes and transported to the seafloor along migration pathways. A recently discovered seep area located off Concepción (Chile) at water depth between 600 to 1100 mbsl is characterized by active methane vent sites as well as massive carbonates boulders and plates which probably are related to methane seepage in the past. During the SO210 research expedition "Chiflux" (Sept-Oct 2010), sediment from the Concepción Methane Seep Area (CSMA) at the fore arc of the Chilean margin was sampled to study microbial activity related to methane seepage. We sampled surface sediments (0-30cm) from sulfur bacteria mats, as well as clam, pogonophoran, and tubeworm fields with push cores and a TV-guided multicorer system. Anaerobic oxidation of methane (AOM) and sulfate reduction rates were determined using ex-situ radioisotope tracer techniques. Additionally, porewater chemistry of retrieved cores as well as isotopic composition and age record of surrounding authigenic carbonates were analyzed. The shallowest sulfate-methane-transition zone (SMTZ) was identified at 4 cm sediment depth hinting to locally strong fluid fluxes. However, a lack of Cl- anomalies in porewater profiles indicates a shallow source of these fluids, which is supported by the biogenic origin of the methane (δ13C -70‰ PDB). Sulfide and alkalinity was relatively high (up to 20 mM and 40 mEq, respectively). Rates of AOM and sulfate reduction within this area reached magnitudes typical for seeps with variation between different habitat types, indicating a diverse methane supply, which is affecting the depths of the SMTZ. Rates were highest at sulfur a bacteria mats (20 mmol m-2 d-1) followed by a large field of dead clams, a pogonophoran field, a black sediment spot, and a carbonate rich clam field. Lowest rates (0.2 mmol m-2 d-1) were measured in close vicinity to these hot spots. Abundant massive carbonate blocks and plates hint to a very old seep system with a probably much higher activity in the past. The U-Th age record of these authigenic carbonates reach back to periods of venting activity with more than 150 ka ago. Carbon isotopic signatures of authigenic carbonates (δ13C -50 to -40‰ PDB) suggest a biogenic carbon source (i.e. methane), also in the past. We found several indications for the impact of recent earthquakes within the seep area (cracks, shifted seafloor), which could be an important mechanism for the triggering of new seepage activity, change in fluid expulsion rates and colonization patterns of the cold seep fauna.
Zhao, Zhi -Jian; Kulkarni, Ambarish; Vilella, Laia; ...
2016-05-02
Selective oxidation of methane to methanol is one of the most difficult chemical processes to perform. A potential group of catalysts to achieve CH 4 partial oxidation are Cu-exchanged zeolites mimicking the active structure of the enzyme methane monooxygenase. However, the details of this conversion, including the structure of the active site, are still under debate. In this contribution, periodic density functional theory (DFT) methods were employed to explore the molecular features of the selective oxidation of methane to methanol catalyzed by Cu-exchanged mordenite (Cu-MOR). We focused on two types of previously suggested active species, CuOCu and CuOOCu. Our calculationsmore » indicate that the formation of CuOCu is more feasible than that of CuOOCu. In addition, a much lower C–H dissociation barrier is located on the former active site, indicating that C–H bond activation is easily achieved with CuOCu. We calculated the energy barriers of all elementary steps for the entire process, including catalyst activation, CH 4 activation, and CH 3OH desorption. Finally, our calculations are in agreement with experimental observations and present the first theoretical study examining the entire process of selective oxidation of methane to methanol.« less
NASA Technical Reports Server (NTRS)
Petersen, Elspeth M.; Meier, Anne J.; Tessonnier, Jean-Philippe
2018-01-01
Overarching Purpose: To design a carbon dioxide methanation/Sabatier reaction catalyst able to withstand variable conditions including fluctuations in bed temperature and feed flow rates for 480 days of remote operation to produce seven tons of methane. Current Study Purpose: Examine supported Ruthenium as a carbon dioxide methanation catalyst to determine the effects support properties have on the active phase by studying activity and selectivity. Objective: The remote operation of the Mars ISRU (In Situ Resources Utilization) lander to produce rocket fuel prior to crew arrival on the planet to power an ascent vehicle. Constraints: Long-term operation (480 days); Variable conditions: Feed gas flow rates, Feed gas flow ratios, Reactor bed temperature.
Malinverno, A.; Pohlman, J.W.
2011-01-01
The sulfate-methane transition (SMT), a biogeochemical zone where sulfate and methane are metabolized, is commonly observed at shallow depths (1-30 mbsf) in methane-bearing marine sediments. Two processes consume sulfate at and above the SMT, anaerobic oxidation of methane (AOM) and organoclastic sulfate reduction (OSR). Differentiating the relative contribution of each process is critical to estimate methane flux into the SMT, which, in turn, is necessary to predict deeper occurrences of gas hydrates in continental margin sediments. To evaluate the relative importance of these two sulfate reduction pathways, we developed a diagenetic model to compute the pore water concentrations of sulfate, methane, and dissolved inorganic carbon (DIC). By separately tracking DIC containing 12C and 13C, the model also computes ??13C-DIC values. The model reproduces common observations from methane-rich sediments: a well-defined SMT with no methane above and no sulfate below and a ??13C-DIC minimum at the SMT. The model also highlights the role of upward diffusing 13C-enriched DIC in contributing to the carbon isotope mass balance of DIC. A combination of OSR and AOM, each consuming similar amounts of sulfate, matches observations from Site U1325 (Integrated Ocean Drilling Program Expedition 311, northern Cascadia margin). Without AOM, methane diffuses above the SMT, which contradicts existing field data. The modeling results are generalized with a dimensional analysis to the range of SMT depths and sedimentation rates typical of continental margins. The modeling shows that AOM must be active to establish an SMT wherein methane is quantitatively consumed and the ??13C-DIC minimum occurs. The presence of an SMT generally requires active AOM. Copyright 2011 by the American Geophysical Union.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Holdridge, D. J.
Global Warming and Methane--Global warming, an increase in Earth's near-surface temperature, is believed to result from the buildup of what scientists refer to as ''greenhouse gases.'' These gases include water vapor, carbon dioxide, methane, nitrous oxide, ozone, perfluorocarbons, hydrofluoro-carbons, and sulfur hexafluoride. Greenhouse gases can absorb outgoing infrared (heat) radiation and re-emit it back to Earth, warming the surface. Thus, these gases act like the glass of a greenhouse enclosure, trapping infrared radiation inside and warming the space. One of the more important greenhouse gases is the naturally occurring hydrocarbon methane. Methane, a primary component of natural gas, is themore » second most important contributor to the greenhouse effect (after carbon dioxide). Natural sources of methane include wetlands, fossil sources, termites, oceans, fresh-waters, and non-wetland soils. Methane is also produced by human-related (or anthropogenic) activities such as fossil fuel production, coal mining, rice cultivation, biomass burning, water treatment facilities, waste management operations and landfills, and domesticated livestock operations (Figure 1). These anthropogenic activities account for approximately 70% of the methane emissions to the atmosphere. Methane is removed naturally from the atmosphere in three ways. These methods, commonly referred to as sinks, are oxidation by chemical reaction with tropospheric hydroxyl ion, oxidation within the stratosphere, and microbial uptake by soils. In spite of their important role in removing excess methane from the atmosphere, the sinks cannot keep up with global methane production. Methane concentrations in the atmosphere have increased by 145% since 1800. Increases in atmospheric methane roughly parallel world population growth, pointing to anthropogenic sources as the cause (Figure 2). Increases in the methane concentration reduce Earth's natural cooling efficiency by trapping more of the outgoing terrestrial infrared radiation, increasing the near-surface temperature.« less
Global tropospheric methane: An indication of atmosphere-biosphere-climate interactions?
NASA Technical Reports Server (NTRS)
Harriss, Robert C.; Sebacher, Daniel I.; Bartlett, Karen B.
1985-01-01
Methane is an important atmospheric gas with potentially critical roles in both photochemical and radiation transfer processes. A major natural source of atmospheric methane involves anaerobic fermentation of organic materials in wetland soils and sediments. A data base of field measurements of atmospheric methane was used in the development of a global methane emissions inventory. Calculations support the following hypotheses: (1) Human activities currently produce methane at a rate approximately equal to natural resources (these rapidly increasing anthropogenic sources can explain most of the recent increase observed in tropospheric methane); and (2) Prior to 200 B.P. (before the present), the influence of climate on wetland extent and distribution was probably a dominant factor controlling global biogenic methane emissions to the atmosphere.
Lustemberg, Pablo G.; Ramírez, Pedro J.; Liu, Zongyuan; ...
2016-10-27
The results of core-level photoemission indicate that Ni-CeO 2(111) surfaces with small or medium coverages of nickel are able to activate methane at 300 K, producing adsorbed CH x and CO x (x = 2, 3) groups. Calculations based on density functional theory predict a relatively low activation energy of 0.6–0.7 eV for the cleavage of the first C–H bond in the adsorbed methane molecule. Ni and O centers of ceria work in a cooperative way in the dissociation of the C–H bond at room temperature, where a low Ni loading is crucial for the catalyst activity and stability. Themore » strong electronic perturbations in the Ni nanoparticles produced by the ceria supports of varying natures, such as stoichiometric and reduced, result in a drastic change in their chemical properties toward methane adsorption and dissociation as well as the dry reforming of methane reaction. Lastly, the coverage of Ni has a drastic effect on the ability of the system to dissociate methane and catalyze the dry re-forming process.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lustemberg, Pablo G.; Ramírez, Pedro J.; Liu, Zongyuan
The results of core-level photoemission indicate that Ni-CeO 2(111) surfaces with small or medium coverages of nickel are able to activate methane at 300 K, producing adsorbed CH x and CO x (x = 2, 3) groups. Calculations based on density functional theory predict a relatively low activation energy of 0.6–0.7 eV for the cleavage of the first C–H bond in the adsorbed methane molecule. Ni and O centers of ceria work in a cooperative way in the dissociation of the C–H bond at room temperature, where a low Ni loading is crucial for the catalyst activity and stability. Themore » strong electronic perturbations in the Ni nanoparticles produced by the ceria supports of varying natures, such as stoichiometric and reduced, result in a drastic change in their chemical properties toward methane adsorption and dissociation as well as the dry reforming of methane reaction. Lastly, the coverage of Ni has a drastic effect on the ability of the system to dissociate methane and catalyze the dry re-forming process.« less
NASA Astrophysics Data System (ADS)
Zheng, Y.; Huang, R.; Wang, B. Z.; Bodelier, P. L. E.; Jia, Z. J.
2014-06-01
Pure culture studies have demonstrated that methanotrophs and ammonia oxidizers can both carry out the oxidation of methane and ammonia. However, the expected interactions resulting from these similarities are poorly understood, especially in complex, natural environments. Using DNA-based stable isotope probing and pyrosequencing of 16S rRNA and functional genes, we report on biogeochemical and molecular evidence for growth stimulation of methanotrophic communities by ammonium fertilization, and that methane modulates nitrogen cycling by competitive inhibition of nitrifying communities in a rice paddy soil. Pairwise comparison between microcosms amended with CH4, CH4+Urea, and Urea indicated that urea fertilization stimulated methane oxidation activity 6-fold during a 19-day incubation period, while ammonia oxidation activity was significantly suppressed in the presence of CH4. Pyrosequencing of the total 16S rRNA genes revealed that urea amendment resulted in rapid growth of Methylosarcina-like MOB, and nitrifying communities appeared to be partially inhibited by methane. High-throughput sequencing of the 13C-labeled DNA further revealed that methane amendment resulted in clear growth of Methylosarcina-related MOB while methane plus urea led to an equal increase in Methylosarcina and Methylobacter-related type Ia MOB, indicating the differential growth requirements of representatives of these genera. An increase in 13C assimilation by microorganisms related to methanol oxidizers clearly indicated carbon transfer from methane oxidation to other soil microbes, which was enhanced by urea addition. The active growth of type Ia methanotrops was significantly stimulated by urea amendment, and the pronounced growth of methanol-oxidizing bacteria occurred in CH4-treated microcosms only upon urea amendment. Methane addition partially inhibited the growth of Nitrosospira and Nitrosomonas in urea-amended microcosms, as well as growth of nitrite-oxidizing bacteria. These results suggest that type I methanotrophs can outcompete type II methane oxidizers in nitrogen-rich environments, rendering the interactions among methane and ammonia oxidizers more complicated than previously appreciated.
Anaerobic methanotrophic communities thrive in deep submarine permafrost.
Winkel, Matthias; Mitzscherling, Julia; Overduin, Pier P; Horn, Fabian; Winterfeld, Maria; Rijkers, Ruud; Grigoriev, Mikhail N; Knoblauch, Christian; Mangelsdorf, Kai; Wagner, Dirk; Liebner, Susanne
2018-01-22
Thawing submarine permafrost is a source of methane to the subsurface biosphere. Methane oxidation in submarine permafrost sediments has been proposed, but the responsible microorganisms remain uncharacterized. We analyzed archaeal communities and identified distinct anaerobic methanotrophic assemblages of marine and terrestrial origin (ANME-2a/b, ANME-2d) both in frozen and completely thawed submarine permafrost sediments. Besides archaea potentially involved in anaerobic oxidation of methane (AOM) we found a large diversity of archaea mainly belonging to Bathyarchaeota, Thaumarchaeota, and Euryarchaeota. Methane concentrations and δ 13 C-methane signatures distinguish horizons of potential AOM coupled either to sulfate reduction in a sulfate-methane transition zone (SMTZ) or to the reduction of other electron acceptors, such as iron, manganese or nitrate. Analysis of functional marker genes (mcrA) and fluorescence in situ hybridization (FISH) corroborate potential activity of AOM communities in submarine permafrost sediments at low temperatures. Modeled potential AOM consumes 72-100% of submarine permafrost methane and up to 1.2 Tg of carbon per year for the total expected area of submarine permafrost. This is comparable with AOM habitats such as cold seeps. We thus propose that AOM is active where submarine permafrost thaws, which should be included in global methane budgets.
Aoki, Masataka; Ehara, Masayuki; Saito, Yumi; Yoshioka, Hideyoshi; Miyazaki, Masayuki; Saito, Yayoi; Miyashita, Ai; Kawakami, Shuji; Yamaguchi, Takashi; Ohashi, Akiyoshi; Nunoura, Takuro; Takai, Ken; Imachi, Hiroyuki
2014-01-01
Anaerobic oxidation of methane (AOM) in marine sediments is an important global methane sink, but the physiological characteristics of AOM-associated microorganisms remain poorly understood. Here we report the cultivation of an AOM microbial community from deep-sea methane-seep sediment using a continuous-flow bioreactor with polyurethane sponges, called the down-flow hanging sponge (DHS) bioreactor. We anaerobically incubated deep-sea methane-seep sediment collected from the Nankai Trough, Japan, for 2,013 days in the bioreactor at 10°C. Following incubation, an active AOM activity was confirmed by a tracer experiment using 13C-labeled methane. Phylogenetic analyses demonstrated that phylogenetically diverse Archaea and Bacteria grew in the bioreactor. After 2,013 days of incubation, the predominant archaeal components were anaerobic methanotroph (ANME)-2a, Deep-Sea Archaeal Group, and Marine Benthic Group-D, and Gammaproteobacteria was the dominant bacterial lineage. Fluorescence in situ hybridization analysis showed that ANME-1 and -2a, and most ANME-2c cells occurred without close physical interaction with potential bacterial partners. Our data demonstrate that the DHS bioreactor system is a useful system for cultivating fastidious methane-seep-associated sedimentary microorganisms. PMID:25141130
NASA Astrophysics Data System (ADS)
Leifer, I.; Culling, D.; Schneising, O.; Bovensmann, H.; Buchwitz, M.; Burrows, J. P.
2012-12-01
A ground-based, transcontinental (Florida to California - i.e., satellite-scale) survey was conducted to understand better the role of fossil fuel industrial (FFI) fugitive emissions of the potent greenhouse gas, methane. Data were collected by flame ion detection gas chromatography (Fall 2010) and by a cavity ring-down sensor (Winter 2012) from a nearly continuously moving recreational vehicle, allowing 24/7 data collection. Nocturnal methane measurements for similar sources tended to be higher compared to daytime values, sometime significantly, due to day/night meteorological differences. Data revealed strong and persistent FFI methane sources associated with refining, a presumed major pipeline leak, and several minor pipeline leaks, a coal loading plant, and areas of active petroleum production. Data showed FFI source emissions were highly transient and heterogeneous; however, integrated over these large-scale facilities, methane signatures overwhelmed that of other sources, creating clearly identifiable plumes that were well elevated above ambient. The highest methane concentration recorded was 39 ppm at an active central valley California production field, while desert values were as low as 1.80 ppm. Surface methane data show similar trends with strong emissions correlated with FFI on large (4° bin) scales and positive methane anomalies centered on the Gulf Coast area of Houston, home to most of US refining capacity. Comparison with SCIAMACHY and GOSAT satellite data show agreement with surface data in the large-scale methane spatial patterns. Positive satellite methane anomalies in the southeast and Mexico largely correlated with methane anthropogenic and wetland inventory models suggests most strong ground methane anomalies in the Gulf of Mexico region were related to dominant FFI input for most seasons. Wind advection played a role, in some cases confounding a clear relationship. Results are consistent with a non-negligible underestimation of the FFI contribution to global methane budgets.; In situ methane concentrations during transcontinental survey Fall 2010.
Observed variations of methane on Mars unexplained by known atmospheric chemistry and physics.
Lefèvre, Franck; Forget, François
2009-08-06
The detection of methane on Mars has revived the possibility of past or extant life on this planet, despite the fact that an abiogenic origin is thought to be equally plausible. An intriguing aspect of the recent observations of methane on Mars is that methane concentrations appear to be locally enhanced and change with the seasons. However, methane has a photochemical lifetime of several centuries, and is therefore expected to have a spatially uniform distribution on the planet. Here we use a global climate model of Mars with coupled chemistry to examine the implications of the recently observed variations of Martian methane for our understanding of the chemistry of methane. We find that photochemistry as currently understood does not produce measurable variations in methane concentrations, even in the case of a current, local and episodic methane release. In contrast, we find that the condensation-sublimation cycle of Mars' carbon dioxide atmosphere can generate large-scale methane variations differing from those observed. In order to reproduce local methane enhancements similar to those recently reported, we show that an atmospheric lifetime of less than 200 days is necessary, even if a local source of methane is only active around the time of the observation itself. This implies an unidentified methane loss process that is 600 times faster than predicted by standard photochemistry. The existence of such a fast loss in the Martian atmosphere is difficult to reconcile with the observed distribution of other trace gas species. In the case of a destruction mechanism only active at the surface of Mars, destruction of methane must occur with an even shorter timescale of the order of approximately 1 hour to explain the observations. If recent observations of spatial and temporal variations of methane are confirmed, this would suggest an extraordinarily harsh environment for the survival of organics on the planet.
NASA Astrophysics Data System (ADS)
Graw, M. F.; Pohlman, J.; Treude, T.; Ruppel, C. D.; Colwell, F. S.
2016-12-01
Methane seeps are dynamic environments on continental margins where subsurface methane reaches the ocean. Microbial communities play a critical role in carbon cycling within seep sediments via organic carbon degradation, methane production, and anaerobic oxidation of methane (AOM), which consumes 20-80% of methane in seep sediments. However, biogeochemical controls on microbial community structure at seeps on a margin-wide scale remain unclear. The passive US Atlantic Margin (USAM) has been identified as a region of active methane seepage. Passive margin seeps have traditionally been understudied relative to seeps on active margins. Passive margins exhibit large cross-margin variability in organic carbon deposition and are anticipated to have divergent seep dynamics from active margins. Thus, the USAM offers a unique opportunity to investigate controls on microbial communities in seep sediments. We undertook analysis of microbial communities inhabiting seep sediments at 6 biogeochemically distinct sites along the USAM. Microbiological samples were co-located with measurements of sediment geochemistry and AOM and sulfate reduction rates. Illumina sequencing of the 16S rRNA gene, using both universal (83 samples) and archaeal-specific (64 samples) primers, and the mcrA gene (18 samples) identified 44 bacterial phyla and 7 archaeal phyla. Seeps in canyons and on open slope, likely representing high and low organic content sediments, hosted distinct communities; the former was dominated by ammonia-oxidizing Marine Group I Thaumarchaeota and the latter by mixotrophic Hadesarchaeota. Seep stability also impacted microbial community structure, and in particular the establishment of an AOM community rather than a Bathyarchaeota-dominated community. These findings contribute to understanding how microbial communities are structured within methane seep sediments and pave the way for investigating broad differences in carbon cycling between seeps on passive and active margins.
A Novel Study of Methane-Rich Gas Reforming to Syngas and Its Kinetics over Semicoke Catalyst
Zhang, Guojie; Su, Aiting; Qu, Jiangwen; Du, Yannian
2014-01-01
A small-size gasification unit is improved through process optimization to simulate industrial United Gas Improvement Company gasification. It finds that the reaction temperature has important impacts on semicoke catalyzed methane gas mixture. The addition of water vapor can enhance the catalytic activity of reforming, which is due to the fact that addition of water vapor not only removes carbon deposit produced in the reforming and gasification reaction processes, but also participates in gasification reaction with semicoke to generate some active oxygen-containing functional groups. The active oxygen-containing functional groups provide active sites for carbon dioxide reforming of methane, promoting the reforming reaction. It also finds that the addition of different proportions of methane-rich gas can yield synthesis gas with different H2/CO ratio. The kinetics study shows that the semicoke can reduce the activation energy of the reforming reaction and promote the occurrence of the reforming reaction. The kinetics model of methane reforming under the conditions of steam gasification over semicoke is as follows: k-=5.02×103·pCH40.71·pH20.26·exp(−74200/RT). PMID:24959620
Low upper limit to methane abundance on Mars.
Webster, Christopher R; Mahaffy, Paul R; Atreya, Sushil K; Flesch, Gregory J; Farley, Kenneth A
2013-10-18
By analogy with Earth, methane in the Martian atmosphere is a potential signature of ongoing or past biological activity. During the past decade, Earth-based telescopic observations reported "plumes" of methane of tens of parts per billion by volume (ppbv), and those from Mars orbit showed localized patches, prompting speculation of sources from subsurface bacteria or nonbiological sources. From in situ measurements made with the Tunable Laser Spectrometer (TLS) on Curiosity using a distinctive spectral pattern specific to methane, we report no detection of atmospheric methane with a measured value of 0.18 ± 0.67 ppbv corresponding to an upper limit of only 1.3 ppbv (95% confidence level), which reduces the probability of current methanogenic microbial activity on Mars and limits the recent contribution from extraplanetary and geologic sources.
Survey of Constellation-Era LOX/Methane Development Activities and Future Development Needs
NASA Technical Reports Server (NTRS)
Marshall, William M.; Stiegemeier, Benjamin; Greene, Sandra Elam; Hurlbert, Eric A.
2017-01-01
NASA formed the Constellation Program in 2005 to achieve the objectives of maintaining American presence in low-Earth orbit, returning to the moon for purposes of establishing an outpost, and laying the foundation to explore Mars and beyond in the first half of the 21st century. The Exploration Technology Development Program (ETDP) was formulated to address the technology needs to address Constellation architecture decisions. The Propellants and Cryogenic Advanced Development (PCAD) project was tasked with risk mitigation of specific propulsion related technologies to support ETDP. Propulsion systems were identified as critical technologies owing to the high gear-ratio of lunar Mars landers Cryogenic propellants offer performance advantage over storables (NTOMMH) Mass savings translate to greater payload capacity In-situ production of propellant an attractive feature; methane and oxygen identified as possible Martian in-situ propellants New technologies were required to meet more difficult missions High performance LOX/LH2 deep throttle descent engines High performance LOX/LCH4 ascent main and reaction control system (RCS) engines The PCAD project sought to provide those technologies through Reliable ignition pulse RCS Fast start High efficiency engines Stable deep throttling.
Aghayan, M; Potemkin, D I; Rubio-Marcos, F; Uskov, S I; Snytnikov, P V; Hussainova, I
2017-12-20
Efficient capture and recycling of CO 2 enable not only prevention of global warming but also the supply of useful low-carbon fuels. The catalytic conversion of CO 2 into an organic compound is a promising recycling approach which opens new concepts and opportunities for catalytic and industrial development. Here we report about template-assisted wet-combustion synthesis of a one-dimensional nickel-based catalyst for carbon dioxide methanation and methane steam reforming. Because of a high temperature achieved in a short time during reaction and a large amount of evolved gases, the wet-combustion synthesis yields homogeneously precipitated nanoparticles of NiO with average particle size of 4 nm on alumina nanofibers covered with a NiAl 2 O 4 nanolayer. The as-synthesized core-shell structured fibers exhibit outstanding activity in steam reforming of methane and sufficient activity in carbon dioxide methanation with 100% selectivity toward methane formation. The as-synthesized catalyst shows stable operation under the reaction conditions for at least 50 h.
[Sources of Methane in the Boreal Region
NASA Technical Reports Server (NTRS)
1998-01-01
In determining the global methane budget the sources of methane must be balanced with the sinks and atmospheric inventory. The approximate contribution of the different methane sources to the budget has been establish showing the major terrestrial inputs as rice, wetlands, bogs, fens, and tundra. Measurements and modeling of production in these sources suggest that temperature, water table height and saturation along with substratum composition are important in controlling methane production and emission. The isotopic budget of 13 C and D/H in methane can be used as a tool to clarify the global budget. This approach has achieved success at constraining the inputs. Studies using the isotopic approach place constraints on global methane production from different sources. Also, the relation between the two biogenic production pathways, acetate fermentation and CO2 reduction, and the effect of substratum composition can be made using isotope measurements shows the relation between the different biogenic, thermogenic and anthropogenic sources of methane as a function of the carbon and hydrogen isotope values for each source and the atmosphere, tropospheric composition. Methane emissions from ponds and fens are a significant source in the methane budget of the boreal region. An initial study in 1993 and 1994 on the isotopic composition of this methane source and the isotopic composition in relation to oxidation of methane at the sediment surface of the ponds or fen was conducted as part of our BOREAS project. The isotopic composition of methane emitted by saturated anoxic sediment is dependent on the sediment composition and geochemistry, but will be influenced by in situ oxidation, in part, a function of rooted plant activity. The influence of oxidation mediated by rooted plant activities on the isotopic composition of methane is not well known and will depend on the plant type, sediment temperature, and numerous other variables. Information on this isotopic composition is important in both understanding the bio-geochemistry of the system and also in determining the regional and global inputs for the methane isotope budget. In determining the destruction of methane for balancing the atmospheric methane budget soil oxidation must be considered.
Dry/Wet Cycles Change the Activity and Population Dynamics of Methanotrophs in Rice Field Soil
Ma, Ke; Conrad, Ralf
2013-01-01
The methanotrophs in rice field soil are crucial in regulating the emission of methane. Drainage substantially reduces methane emission from rice fields. However, it is poorly understood how drainage affects microbial methane oxidation. Therefore, we analyzed the dynamics of methane oxidation rates, composition (using terminal restriction fragment length polymorphism [T-RFLP]), and abundance (using quantitative PCR [qPCR]) of methanotroph pmoA genes (encoding a subunit of particulate methane monooxygenase) and their transcripts over the season and in response to alternate dry/wet cycles in planted paddy field microcosms. In situ methane oxidation accounted for less than 15% of total methane production but was enhanced by intermittent drainage. The dry/wet alternations resulted in distinct effects on the methanotrophic communities in different soil compartments (bulk soil, rhizosphere soil, surface soil). The methanotrophic communities of the different soil compartments also showed distinct seasonal dynamics. In bulk soil, potential methanotrophic activity and transcription of pmoA were relatively low but were significantly stimulated by drainage. In contrast, however, in the rhizosphere and surface soils, potential methanotrophic activity and pmoA transcription were relatively high but decreased after drainage events and resumed after reflooding. While type II methanotrophs dominated the communities in the bulk soil and rhizosphere soil compartments (and to a lesser extent also in the surface soil), it was the pmoA of type I methanotrophs that was mainly transcribed under flooded conditions. Drainage affected the composition of the methanotrophic community only minimally but strongly affected metabolically active methanotrophs. Our study revealed dramatic dynamics in the abundance, composition, and activity of the various type I and type II methanotrophs on both a seasonal and a spatial scale and showed strong effects of dry/wet alternation cycles, which enhanced the attenuation of methane flux into the atmosphere. PMID:23770899
Zuo, Zhijun; Ramírez, Pedro J.; Senanayake, Sanjaya D.; ...
2016-10-10
Here, an inverse CeO 2/Cu 2O/Cu(111) catalyst is able to activate methane at room temperature producing C, CH x fragments and CO x species on the oxide surface. The addition of water to the system leads to a drastic change in the selectivity of methane activation yielding only adsorbed CH x fragments. At a temperature of 450 K, in the presence of water, a CH 4 → CH 3OH catalytic transformation occurs with a high selectivity. OH groups formed by the dissociation of water saturate the catalyst surface, removing sites that could decompose CH x fragments, and generating centers onmore » which methane can directly interact to yield methanol.« less
The effects and mechanism of action of methane on ileal motor function.
Park, Y M; Lee, Y J; Hussain, Z; Lee, Y H; Park, H
2017-09-01
Methane has been associated with constipation-predominant irritable bowel syndrome, slowing intestinal transit time by augmenting contractile activity. However, the precise mechanism underlying this effect remains unclear. Therefore, we investigated the mechanisms underlying the effect of methane on contractile activity, and whether such effects are mediated by nerve impulses or muscular contraction. We connected guinea pig ileal muscle strips to a force/tension transducer and measured amplitudes of contraction in response to electrical field stimulation (EFS; 1, 2, 8, 16 Hz) following methane infusion in the presence of tetradotoxin (TTX), atropine, guanethidine, or GR 113808. We then performed calcium imaging using Oregon Green 488 BAPTA-1 AM in order to visualize changes in calcium fluorescence in response to EFS following methane infusion in the presence of TTX, atropine, or a high K + solution. Methane significantly increased amplitudes of contraction (P<.05), while treatment with TTX abolished such contraction. Methane-induced increases in amplitude were inhibited when lower-frequency (1, 2 Hz) EFS was applied following atropine infusion (P<.05). Neither guanethidine nor GR 113808 significantly altered contraction amplitudes. Methane significantly increased calcium fluorescence, while this increase was attenuated following atropine infusion (P<.05). Although calcium fluorescence was increased by the high K + solution under pretreatment with TTX, the intensity of fluorescence remained unchanged after methane infusion. The actions of methane on the intestine are influenced by the cholinergic pathway of the enteric nervous system. Our findings support the classification of methane as a gasotransmitter. © 2017 John Wiley & Sons Ltd.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Varghese, Jithin J.; Mushrif, Samir H., E-mail: shmushrif@ntu.edu.sg
Small metal clusters exhibit unique size and morphology dependent catalytic activity. The search for alternate minimum energy pathways and catalysts to transform methane to more useful chemicals and carbon nanomaterials led us to investigate collision induced dissociation of methane on small Cu clusters. We report here for the first time, the free energy barriers for the collision induced activation, dissociation, and coupling of methane on small Cu clusters (Cu{sub n} where n = 2–12) using ab initio molecular dynamics and metadynamics simulations. The collision induced activation of the stretching and bending vibrations of methane significantly reduces the free energy barriermore » for its dissociation. Increase in the cluster size reduces the barrier for dissociation of methane due to the corresponding increase in delocalisation of electron density within the cluster, as demonstrated using the electron localisation function topology analysis. This enables higher probability of favourable alignment of the C–H stretching vibration of methane towards regions of high electron density within the cluster and makes higher number of sites available for the chemisorption of CH{sub 3} and H upon dissociation. These characteristics contribute in lowering the barrier for dissociation of methane. Distortion and reorganisation of cluster geometry due to high temperature collision dynamics disturb electron delocalisation within them and increase the barrier for dissociation. Coupling reactions of CH{sub x} (x = 1–3) species and recombination of H with CH{sub x} have free energy barriers significantly lower than complete dehydrogenation of methane to carbon. Thus, competition favours the former reactions at high hydrogen saturation on the clusters.« less
NASA Astrophysics Data System (ADS)
Spaendonk, Vincent Van
Past research has shown unusual activity of the (1 x 1)Pt(110) surface to break carbon-carbon and carbon -oxygen bonds. Methane formation from ethylene or ethane has been reported for supported platinum catalysts. A model for the methane formation on (1 x 1)Pt(110), was proposed by Yagasaki. In this study, the mechanism of methane formation has been further investigated, and Yagasaki's model tested, by studying the decomposition of ethylene and methanol on the stepped surfaces Pt(511) and Pt(331) with Temperature Programmed Desorption. The experiments have been carried out in a Ultra High Vacuum system, equipped with a mass spectrometer, LEED and AES. Hydrogen and carbon monoxide desorption show that on Pt(511) different adsorption sites are available than on Pt(331). Ethylene decomposition on Pt(511) leads to small amounts of methane formation compared to (1 x 1)Pt(110). The metastable (1 x 1) phase of Pt(511) is 2-3 times more active than the stable (hex) phase. When ^{13}C_2H _4 is used, ^{13 }CH_4 is not detected. Methane formation is not seen on the Pt(331) surface. Arguments are given why Pt(511) is a superior model for supported catalysts compared to (1 x 1)Pt(110). The carbon-oxygen bond of methanol is not broken on either Pt(511) or Pt(331), whether the surface is clean or covered with oxygen. Hydrogen saturating the surface, prevents the chemisorption of ethylene and the formation of methane. Postadsorption of hydrogen does not lead to an increase in methane formation. Coadsorption of ethylene with carbon monoxide shows a maximum methane formation at 0.3 L carbon monoxide exposure. Poison experiments with 'oxide' and carbon indicate that the active site for methane formation is located at the step. The amount of carbon deposited during ethylene decomposition, increases in the order (1 x 1)Pt(511) to (hex)Pt(511) to Pt(331). This is also the order for decreasing methane activity. In a new model, it is proposed that in order to be active for methane formation, a surface has to prevent the polymerization of single carbon species to inactive graphite. The model predicts that surfaces with large enough (111) terraces have higher diffusion rates and allow the single carbon species to convert to graphite before the species can be hydrogenated.
Microbial oxidation as a methane sink beneath the West Antarctic Ice Sheet
NASA Astrophysics Data System (ADS)
Michaud, Alexander B.; Dore, John E.; Achberger, Amanda M.; Christner, Brent C.; Mitchell, Andrew C.; Skidmore, Mark L.; Vick-Majors, Trista J.; Priscu, John C.
2017-08-01
Aquatic habitats beneath ice masses contain active microbial ecosystems capable of cycling important greenhouse gases, such as methane (CH4). A large methane reservoir is thought to exist beneath the West Antarctic Ice Sheet, but its quantity, source and ultimate fate are poorly understood. For instance, O2 supplied by basal melting should result in conditions favourable for aerobic methane oxidation. Here we use measurements of methane concentrations and stable isotope compositions along with genomic analyses to assess the sources and cycling of methane in Subglacial Lake Whillans (SLW) in West Antarctica. We show that sub-ice-sheet methane is produced through the biological reduction of CO2 using H2. This methane pool is subsequently consumed by aerobic, bacterial methane oxidation at the SLW sediment-water interface. Bacterial oxidation consumes >99% of the methane and represents a significant methane sink, and source of biomass carbon and metabolic energy to the surficial SLW sediments. We conclude that aerobic methanotrophy may mitigate the release of methane to the atmosphere upon subglacial water drainage to ice sheet margins and during periods of deglaciation.
Historical methane hydrate project review
Collett, Timothy; Bahk, Jang-Jun; Frye, Matt; Goldberg, Dave; Husebo, Jarle; Koh, Carolyn; Malone, Mitch; Shipp, Craig; Torres, Marta
2013-01-01
In 1995, U.S. Geological Survey made the first systematic assessment of the volume of natural gas stored in the hydrate accumulations of the United States. That study, along with numerous other studies, has shown that the amount of gas stored as methane hydrates in the world greatly exceeds the volume of known conventional gas resources. However, gas hydrates represent both a scientific and technical challenge and much remains to be learned about their characteristics and occurrence in nature. Methane hydrate research in recent years has mostly focused on: (1) documenting the geologic parameters that control the occurrence and stability of gas hydrates in nature, (2) assessing the volume of natural gas stored within various gas hydrate accumulations, (3) analyzing the production response and characteristics of methane hydrates, (4) identifying and predicting natural and induced environmental and climate impacts of natural gas hydrates, and (5) analyzing the effects of methane hydrate on drilling safety.Methane hydrates are naturally occurring crystalline substances composed of water and gas, in which a solid water-‐lattice holds gas molecules in a cage-‐like structure. The gas and water becomes a solid under specific temperature and pressure conditions within the Earth, called the hydrate stability zone. Other factors that control the presence of methane hydrate in nature include the source of the gas included within the hydrates, the physical and chemical controls on the migration of gas with a sedimentary basin containing methane hydrates, the availability of the water also included in the hydrate structure, and the presence of a suitable host sediment or “reservoir”. The geologic controls on the occurrence of gas hydrates have become collectively known as the “methane hydrate petroleum system”, which has become the focus of numerous hydrate research programs.Recognizing the importance of methane hydrate research and the need for a coordinated effort, the U.S. Congress enacted Public Law 106-‐193, the Methane Hydrate Research and Development Act of 2000. This Act called for the Secretary of Energy to begin a methane hydrate research and development program in consultation with other U.S. federal agencies. At the same time a new methane hydrate research program had been launched in Japan by the Ministry of International Trade and Industry to develop plans for a methane hydrate exploratory drilling project in the Nankai Trough. Since this early start we have seen other countries including India, China, Canada, and the Republic of Korea establish large gas hydrate research and development programs. These national led efforts have also included the investment in a long list of important scientific research drilling expeditions and production test studies that have provided a wealth of information on the occurrence of methane hydrate in nature. The most notable expeditions and projects have including the following:-‐Ocean Drilling Program Leg 164 (1995)-‐Japan Nankai Trough Project (1999-‐2000)-‐Ocean Drilling Program Leg 204 (2004)-‐Japan Tokai-‐oki to Kumano-‐nada Project (2004)-‐Gulf of Mexico JIP Leg I (2005)-‐Integrated Ocean Drilling Program Expedition 311 (2005)-‐Malaysia Gumusut-‐Kakap Project (2006)-‐India NGHP Expedition 01 (2006)-‐China GMGS Expedition 01 (2007)-‐Republic of Korea UBGH Expedition 01 (2007)-‐Gulf of Mexico JIP Leg II (2009)-‐Republic of Korea UBGH Expedition 02 (2010)-‐MH-‐21 Nankai Trough Pre-‐Production Expedition (2012-‐2013)-‐Mallik Gas Hydrate Testing Projects (1998/2002/2007-‐2008)-‐Alaska Mount Elbert Stratigraphic Test Well (2007)-‐Alaska Iġnik Sikumi Methane Hydrate Production Test Well (2011-‐2012)Research coring and seismic programs carried out by the Ocean Drilling Program (ODP) and Integrated Ocean Drilling Program (IODP), starting with the ODP Leg 164 drilling of the Blake Ridge in the Atlantic Ocean in 1995, have also contributed greatly to our understanding of the geologic controls on the formation, occurrence, and stability of gas hydrates in marine environments. For the most part methane hydrate research expeditions carried out by the ODP and IODP provided the foundation for our scientific understanding of gas hydrates. The methane hydrate research efforts under ODP-‐IODP have mostly dealt with the assessment of the geologic controls on the occurrence of gas hydrate, with a specific goal to study the role methane hydrates may play in the global carbon cycle.Over the last 10 years, national led methane hydrate research programs, along with industry interest have led to the development and execution of major methane hydrate production field test programs. Two of the most important production field testing programs have been conducted at the Mallik site in the Mackenzie River Delta of Canada and in the Eileen methane hydrate accumulation on the North Slope of Alaska. Most recently we have also seen the completion of the world’s first marine methane hydrate production test in the Nankai Trough in the offshore of Japan. Industry interest in gas hydrates has also included important projects that have dealt with the assessment of geologic hazards associated with the presence of hydrates.The scientific drilling and associated coring, logging, and borehole monitoring technologies developed in the long list of methane hydrate related field studies are one of the most important developments and contributions associated with methane hydrate research and development activities. Methane hydrate drilling has been conducted from advanced scientific drilling platforms like the JOIDES Resolution and the D/V Chikyu, which feature highly advanced integrated core laboratories and borehole logging capabilities. Hydrate research drilling has also included the use of a wide array of industry, geotechnical and multi-‐service ships. All of which have been effectively used to collect invaluable geologic and engineering data on the occurrence of methane hydrates throughout the world. Technologies designed specifically for the collection and analysis of undisturbed methane hydrate samples have included the development of a host of pressure core systems and associated specialty laboratory apparatus. The study and use of both wireline conveyed and logging-‐while-‐drilling technologies have also contributed greatly to our understanding of the in-‐situ nature of hydrate-‐bearing sediments. Recent developments in borehole instrumentation specifically designed to monitor changes associated with hydrates in nature through time or to evaluate the response of hydrate accumulations to production have also contributed greatly to our understanding of the complex nature and evolution of methane hydrate systems.Our understanding of how methane hydrates occur and behave in nature is still growing and evolving – we do not yet know if methane hydrates can be economically produced, nor do we know fully the role of hydrates as an agent of climate change or as a geologic hazard. But it is known for certain that scientific drilling has contributed greatly to our understanding of hydrates in nature and will continue to be a critical source of the information to advance our understanding of methane hydrates.
Bornemann, Maren; Bussmann, Ingeborg; Tichy, Lucas; Deutzmann, Jörg; Schink, Bernhard; Pester, Michael
2016-08-01
Methane emissions from freshwater environments contribute substantially to global warming but are under strong control of aerobic methane-oxidizing bacteria. Recently discovered methane seeps (pockmarks) in freshwater lake sediments have the potential to bypass this control by their strong outgassing activity. Whether this is counteracted by pelagic methanotrophs is not well understood yet. We used a (3)H-CH4-radiotracer technique and pmoA-based molecular approaches to assess the activity, abundance and community structure of pelagic methanotrophs above active pockmarks in deep oligotrophic Lake Constance. Above profundal pockmarks, methane oxidation rates (up to 458 nmol CH4 l(-1) d(-1)) exceeded those of the surrounding water column by two orders of magnitude and coincided with maximum methanotroph abundances of 0.6% of the microbial community. Phylogenetic analysis indicated a dominance of members of the Methylococcaceae in the water column of both, pockmark and reference sites, with most of the retrieved sequences being associated with a water-column specific clade. Communities at pockmark and reference locations also differed in parts, which was likely caused by entrainment of sediment-hosted methanotrophs at pockmark sites. Our results show that the release of seep-derived methane to the atmosphere is counteracted by a distinct methanotrophic community with a pronounced activity throughout bottom waters. © FEMS 2016. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.
Diversity and potential activity of methanotrophs in high methane-emitting permafrost thaw ponds
Vincent, Warwick F.; Comte, Jérôme; Matveev, Alex; Lovejoy, Connie
2017-01-01
Lakes and ponds derived from thawing permafrost are strong emitters of carbon dioxide and methane to the atmosphere, but little is known about the methane oxidation processes in these waters. Here we investigated the distribution and potential activity of aerobic methanotrophic bacteria in thaw ponds in two types of eroding permafrost landscapes in subarctic Québec: peatlands and mineral soils. We hypothesized that methanotrophic community composition and potential activity differ regionally as a function of the landscape type and permafrost degradation stage, and locally as a function of depth-dependent oxygen conditions. Our analysis of pmoA transcripts by Illumina amplicon sequencing and quantitative PCR showed that the communities were composed of diverse and potentially active lineages. Type I methanotrophs, particularly Methylobacter, dominated all communities, however there was a clear taxonomic separation between the two landscape types, consistent with environmental control of community structure. In contrast, methanotrophic potential activity, measured by pmoA transcript concentrations, did not vary with landscape type, but correlated with conductivity, phosphorus and total suspended solids. Methanotrophic potential activity was also detected in low-oxygen bottom waters, where it was inversely correlated with methane concentrations, suggesting methane depletion by methanotrophs. Methanotrophs were present and potentially active throughout the water column regardless of oxygen concentration, and may therefore be resilient to future mixing and oxygenation regimes in the warming subarctic. PMID:29182670
Diversity and potential activity of methanotrophs in high methane-emitting permafrost thaw ponds.
Crevecoeur, Sophie; Vincent, Warwick F; Comte, Jérôme; Matveev, Alex; Lovejoy, Connie
2017-01-01
Lakes and ponds derived from thawing permafrost are strong emitters of carbon dioxide and methane to the atmosphere, but little is known about the methane oxidation processes in these waters. Here we investigated the distribution and potential activity of aerobic methanotrophic bacteria in thaw ponds in two types of eroding permafrost landscapes in subarctic Québec: peatlands and mineral soils. We hypothesized that methanotrophic community composition and potential activity differ regionally as a function of the landscape type and permafrost degradation stage, and locally as a function of depth-dependent oxygen conditions. Our analysis of pmoA transcripts by Illumina amplicon sequencing and quantitative PCR showed that the communities were composed of diverse and potentially active lineages. Type I methanotrophs, particularly Methylobacter, dominated all communities, however there was a clear taxonomic separation between the two landscape types, consistent with environmental control of community structure. In contrast, methanotrophic potential activity, measured by pmoA transcript concentrations, did not vary with landscape type, but correlated with conductivity, phosphorus and total suspended solids. Methanotrophic potential activity was also detected in low-oxygen bottom waters, where it was inversely correlated with methane concentrations, suggesting methane depletion by methanotrophs. Methanotrophs were present and potentially active throughout the water column regardless of oxygen concentration, and may therefore be resilient to future mixing and oxygenation regimes in the warming subarctic.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Rogers, Jessica L.; Mangarella, Michael C.; D’Amico, Andrew D.
In this paper, the Pechini synthesis was used to prepare nickel aluminate catalysts with the compositions NiAl 4O 7, NiAl 2O 4, and Ni 2Al 2O 5. The samples have been characterized by N 2 physisorption, temperature-programmed reduction (TPR), temperature-programmed oxidation (TPO), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and X-ray absorption spectroscopy (XAS). Characterization results indicate unique structural properties and excellent regeneration potential of nickel aluminates. Prepared samples were tested when unreduced and reduced prior to reaction for methane dry reforming and methane steam reforming reactivity. NiAl 2O 4 in the reduced and unreduced statemore » as well as NiAl 4O 7 in the reduced state are active and stable for methane dry reforming due to the presence of 4-fold coordinated oxidized nickel. The limited amount of metallic nickel in these samples minimizes carbon deposition. Finally, on the other hand, the presence of metallic nickel is required for methane steam reforming. Ni 2Al 2O 5 in the reduced and unreduced states and NiAl 2O 4 in the reduced state are found to be active for methane steam reforming due to the presence of sufficiently small nickel nanoparticles that catalyze the reaction without accumulating carbonaceous deposits.« less
Rogers, Jessica L.; Mangarella, Michael C.; D’Amico, Andrew D.; ...
2016-07-20
In this paper, the Pechini synthesis was used to prepare nickel aluminate catalysts with the compositions NiAl 4O 7, NiAl 2O 4, and Ni 2Al 2O 5. The samples have been characterized by N 2 physisorption, temperature-programmed reduction (TPR), temperature-programmed oxidation (TPO), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and X-ray absorption spectroscopy (XAS). Characterization results indicate unique structural properties and excellent regeneration potential of nickel aluminates. Prepared samples were tested when unreduced and reduced prior to reaction for methane dry reforming and methane steam reforming reactivity. NiAl 2O 4 in the reduced and unreduced statemore » as well as NiAl 4O 7 in the reduced state are active and stable for methane dry reforming due to the presence of 4-fold coordinated oxidized nickel. The limited amount of metallic nickel in these samples minimizes carbon deposition. Finally, on the other hand, the presence of metallic nickel is required for methane steam reforming. Ni 2Al 2O 5 in the reduced and unreduced states and NiAl 2O 4 in the reduced state are found to be active for methane steam reforming due to the presence of sufficiently small nickel nanoparticles that catalyze the reaction without accumulating carbonaceous deposits.« less
Lu, Xueqin; Zhen, Guangyin; Liu, Yuan; Hojo, Toshimasa; Estrada, Adriana Ledezma; Li, Yu-You
2014-10-01
Long-term experiments herein were conducted to investigate the effect of cefalexin (CLX) on methane production during waste activated sludge (WAS) anaerobic digestion. CLX exhibited a considerable inhibition in methane production during the initial 25 days while the negative effect attenuated subsequently and methane production recovered depending on CLX doses used (600 and 1000 mg/L). The highest methane yield reached 450 mL at 1000 mg-CLX/L after 157 days of digestion, 63.8% higher than CLX-free one. Stimulated excretion of extracellular polymeric substances (EPS) by CLX served as microbial protecting layers, creating a suitable environment for microbes' growth and fermentation. Further examination via ultraviolet visible (UV-Vis) spectra also verified the elevated slime EPS, LB-EPS and TB-EPS indicated by UV-254 in the presence of CLX. Unlike the commonly accepted adverse effect, this study demonstrated the beneficial role of CLX in methane production, providing new insights into its true environmental impacts. Copyright © 2014 Elsevier Ltd. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Lidstrom, Mary E.; Chistoserdova, Ludmila; Kalyuzhnaya, Marina G.
2014-08-07
The research conducted as part of this project contributes significantly to the understanding of the microbes and their activities involved in methane metabolism in freshwater lake sediments and in the environment in a more global sense. Significant new insights have been gained into the identity of the species that are most active in methane oxidation. New concepts have been developed based on the new data on how these organisms metabolize methane, impacting not only environmental microbiology but also biotechnology, including biotechnology of next generation biofuels. Novel approaches have been developed for studying functional microbial communities, via holistic approaches, such asmore » metagenomics, metatrancriptomics and metabolite analysis. As a result, a novel outlook has been obtained at how such communities operate in nature. Understanding methane-oxidizing communities in lakes and other environments is of significant benefit to the public, in terms of methane emission mitigation and in terms of potential biotechnological applications.« less
Methane Seep Carbonates Host Distinct, Diverse, and Dynamic Microbial Assemblages
Pasulka, Alexis L.; Marlow, Jeffrey J.; Grupe, Benjamin M.; Levin, Lisa A.
2015-01-01
ABSTRACT Marine methane seeps are globally distributed geologic features in which reduced fluids, including methane, are advected upward from the subsurface. As a result of alkalinity generation during sulfate-coupled methane oxidation, authigenic carbonates form slabs, nodules, and extensive pavements. These carbonates shape the landscape within methane seeps, persist long after methane flux is diminished, and in some cases are incorporated into the geologic record. In this study, microbial assemblages from 134 native and experimental samples across 5,500 km, representing a range of habitat substrates (carbonate nodules and slabs, sediment, bottom water, and wood) and seepage conditions (active and low activity), were analyzed to address two fundamental questions of seep microbial ecology: (i) whether carbonates host distinct microbial assemblages and (ii) how sensitive microbial assemblages are to habitat substrate type and temporal shifts in methane seepage flux. Through massively parallel 16S rRNA gene sequencing and statistical analysis, native carbonates are shown to be reservoirs of distinct and highly diverse seep microbial assemblages. Unique coupled transplantation and colonization experiments on the seafloor demonstrated that carbonate-associated microbial assemblages are resilient to seep quiescence and reactive to seep activation over 13 months. Various rates of response to simulated seep quiescence and activation are observed among similar phylogenies (e.g., Chloroflexi operational taxonomic units) and similar metabolisms (e.g., putative S oxidizers), demonstrating the wide range of microbial sensitivity to changes in seepage flux. These results imply that carbonates do not passively record a time-integrated history of seep microorganisms but rather host distinct, diverse, and dynamic microbial assemblages. PMID:26695630
Freshwater bacteria release methane as a byproduct of phosphorus acquisition.
Yao, Mengyin; Henny, Cynthia; Maresca, Julia A
2016-09-30
Freshwater lakes emit large amounts of methane, some of which is produced in oxic surface waters. Two potential pathways for aerobic methane production exist: methanogenesis in oxygenated water, which has been observed in some lakes, or demethylation of small organic molecules. Although methane is produced via demethylation in oxic marine environments, this mechanism of methane release has not yet been demonstrated in freshwater systems. Genes related to the C-P lyase pathway, which cleaves C-P bonds in phosphonate compounds, were found in a metagenomic survey of the surface water of Lake Matano, which is chronically P-starved and methane-rich. We demonstrate that four bacterial isolates from Lake Matano obtain P from methylphosphonate and release methane, and that this activity is repressed by phosphate. We further demonstrate that expression of phnJ, which encodes the enzyme that releases methane, is higher in the presence of methylphosphonate and lower when both methylphosphonate and phosphate are added. This gene is also found in most of the metagenomic data sets from freshwater environments. These experiments link methylphosphonate degradation and methane production with gene expression and phosphate availability in freshwater organisms, and suggest that some of the excess methane in the Lake Matano surface water, and in other methane-rich lakes, may be produced by P-starved bacteria. Methane is an important greenhouse gas, and contributes substantially to global warming. Although freshwater environments are known to release methane into the atmosphere, estimates of the amount of methane emitted by freshwater lakes vary from 8 to 73 Tg per year. Methane emissions are difficult to predict in part because the source of the methane can vary: it is the end product of the energy-conserving pathway in methanogenic archaea, which predominantly live in anoxic sediments or waters, but have also been identified in some oxic freshwater environments. More recently, methane release from small organic molecules has been observed in oxic marine environments. Here we show that demethylation of methylphosphonate may also contribute to methane release from lakes, and that phosphate can repress this activity. Since lakes are typically phosphorus-limited, some methane release in these environments may be a byproduct of phosphorus metabolism, rather than carbon or energy metabolism. Methane emissions from lakes are currently predicted using primary production, eutrophication status, extent of anoxia, and the shape and size of the lake; to improve prediction of methane emissions, phosphorus availability and sources may also need to be included in these models. Copyright © 2016, American Society for Microbiology. All Rights Reserved.
Deutzmann, Jörg S.; Wörner, Susanne; Schink, Bernhard
2011-01-01
The activity and community structure of aerobic methanotrophic communities were investigated at methane seeps (pockmarks) in the littoral and profundal zones of an oligotrophic freshwater lake (Lake Constance, Germany). Measurements of potential methane oxidation rates showed that sediments inside littoral pockmarks are hot spots of methane oxidation. Potential methane oxidation rates at littoral pockmark sites exceeded the rates of the surrounding sediment by 2 orders of magnitude. Terminal restriction fragment length polymorphism (T-RFLP) analysis of the pmoA gene revealed major differences in the methanotrophic community composition between littoral pockmarks and the surrounding sediments. Clone library analysis confirmed that one distinct Methylobacter-related group dominates the community at littoral pockmarks. In profundal sediments, the differences between pockmarks and surrounding sediments were found to be less pronounced. PMID:21335392
Biogas Production from Citrus Waste by Membrane Bioreactor
Wikandari, Rachma; Millati, Ria; Cahyanto, Muhammad Nur; Taherzadeh, Mohammad J.
2014-01-01
Rapid acidification and inhibition by d-limonene are major challenges of biogas production from citrus waste. As limonene is a hydrophobic chemical, this challenge was encountered using hydrophilic polyvinylidine difluoride (PVDF) membranes in a biogas reactor. The more sensitive methane-producing archaea were encapsulated in the membranes, while freely suspended digesting bacteria were present in the culture as well. In this membrane bioreactor (MBR), the free digesting bacteria digested the citrus wastes and produced soluble compounds, which could pass through the membrane and converted to biogas by the encapsulated cell. As a control experiment, similar digestions were carried out in bioreactors containing the identical amount of just free cells. The experiments were carried out in thermophilic conditions at 55 °C, and hydraulic retention time of 30 days. The organic loading rate (OLR) was started with 0.3 kg VS/m3/day and gradually increased to 3 kg VS/m3/day. The results show that at the highest OLR, MBR was successful to produce methane at 0.33 Nm3/kg VS, while the traditional free cell reactor reduced its methane production to 0.05 Nm3/kg VS. Approximately 73% of the theoretical methane yield was achieved using the membrane bioreactor. PMID:25167328
Photosynthesis in Hydrogen-Dominated Atmospheres
Bains, William; Seager, Sara; Zsom, Andras
2014-01-01
The diversity of extrasolar planets discovered in the last decade shows that we should not be constrained to look for life in environments similar to early or present-day Earth. Super-Earth exoplanets are being discovered with increasing frequency, and some will be able to retain a stable, hydrogen-dominated atmosphere. We explore the possibilities for photosynthesis on a rocky planet with a thin H2-dominated atmosphere. If a rocky, H2-dominated planet harbors life, then that life is likely to convert atmospheric carbon into methane. Outgassing may also build an atmosphere in which methane is the principal carbon species. We describe the possible chemical routes for photosynthesis starting from methane and show that less energy and lower energy photons could drive CH4-based photosynthesis as compared with CO2-based photosynthesis. We find that a by-product biosignature gas is likely to be H2, which is not distinct from the hydrogen already present in the environment. Ammonia is a potential biosignature gas of hydrogenic photosynthesis that is unlikely to be generated abiologically. We suggest that the evolution of methane-based photosynthesis is at least as likely as the evolution of anoxygenic photosynthesis on Earth and may support the evolution of complex life. PMID:25411926
Photosynthesis in hydrogen-dominated atmospheres.
Bains, William; Seager, Sara; Zsom, Andras
2014-11-18
The diversity of extrasolar planets discovered in the last decade shows that we should not be constrained to look for life in environments similar to early or present-day Earth. Super-Earth exoplanets are being discovered with increasing frequency, and some will be able to retain a stable, hydrogen-dominated atmosphere. We explore the possibilities for photosynthesis on a rocky planet with a thin H2-dominated atmosphere. If a rocky, H2-dominated planet harbors life, then that life is likely to convert atmospheric carbon into methane. Outgassing may also build an atmosphere in which methane is the principal carbon species. We describe the possible chemical routes for photosynthesis starting from methane and show that less energy and lower energy photons could drive CH4-based photosynthesis as compared with CO2-based photosynthesis. We find that a by-product biosignature gas is likely to be H2, which is not distinct from the hydrogen already present in the environment. Ammonia is a potential biosignature gas of hydrogenic photosynthesis that is unlikely to be generated abiologically. We suggest that the evolution of methane-based photosynthesis is at least as likely as the evolution of anoxygenic photosynthesis on Earth and may support the evolution of complex life.
Big Soda Lake (Nevada). 3. Pelagic methanogenesis and anaerobic methane oxidation
Iversen, Niels; Oremland, Ronald S.; Klug, Michael J.
1987-01-01
In situ rates of methanogenesis and methane oxidation were measured in meromictic Big Soda Lake. Methane production was measured by the accumulation of methane in the headspaces of anaerobically sealed water samples; radiotracer was used to follow methane oxidation. Nearly all the methane oxidation occurred in the anoxic zones of the lake. Rates of anaerobic oxidation exceeded production at all depths studied in both the mixolimnion (2–6 vs. 0.1–1 nmol liter−1 d−1) and monimolimnion (49–85 vs. 1.6–12 nmol liter−1 d−1) of the lake. Thus, a net consumption of methane equivalent to 1.36 mmol m−2 d−1 occurred in the anoxic water column. Anaerobic methane oxidation had a first-order rate constant of 8.1±0.5 × 10−4 d−1, and activity was eliminated by filter sterilization. However, in situ methane oxidation was of insufficient magnitude to cause a noticeable decrease of ambient dissolved methane levels over an incubation period of 97 h.
The effects of acid deposition on sulfate reduction and methane production in peatlands
NASA Technical Reports Server (NTRS)
Murray, Georgia L.; Hines, Mark E.; Bayley, Suzanne E.
1992-01-01
Peatlands, as fens and bods, make up a large percentage of northern latitude terrestrial environments. They are organic rich and support an active community of anaerobic bacteria, such as methanogenic and sulfate-reducing bacteria. The end products of these microbial activities, methane and hydrogen sulfide, are important components in the global biogeochemical cycles of carbon and sulfur. Since these two bacterial groups compete for nutritional substrates, increases in sulfate deposition due to acid rain potentially can disrupt the balance between these processes leading to a decrease in methane production and emission. This is significant because methane is a potent greenhouse gas that effects the global heat balance. A section of Mire 239 in the Experimental Lakes Area, in Northwestern Ontario, was artificially acidified and rates of sulfate reduction and methane production were measured with depth. Preliminary results suggested that methane production was not affected immediately after acidification. However, concentrations of dissolved methane decreased and dissolved sulfide increased greatly after acidification and both took several days to recover. The exact mechanism for the decrease in methane was not determined. Analyses are under way which will be used to determine rates of sulfate reduction. These results will be available by Spring and will be discussed.
2013-07-01
throughout the observation period. A 0.25-ml Pressure-Lok gas -tight syringe with a side-ported needle was used to take 0.1 ml headspace samples during...33. Biodegradation of methane, VC and a methane+VC mixture by methane enrichment cultures derived from Carver well RB63I. These results indicate that...VC and a methane+VC mixture by methane enrichment cultures derived from Carver well RB63I. These results are a repeat of the experiment depicted in
NASA Astrophysics Data System (ADS)
Lee, Y. M.; Lee, D. H.; Hwang, K.; Hong, S. G.; Jin, Y. K.
2016-12-01
The prokaryotic microorganisms inhabiting Mud Volcanoes (MVs) play an important role for mitigation of methane (CH4) emission. Despite the identification of active MVs in the continental slope of the Canadian Beaufort Sea, little is known about the distribution and functions of prokaryotic community in this region. Hence, we investigated the prokaryotic diversity of four sediment cores (three from the active MVs and one from a non-methane influenced reference site) of the Canadian Beaufort Sea using 454-pyrosequencing of 16S rRNA genes as the first step to understand the prokaryotic roles in controlling outgassing methane. Bacterial and archaeal communities of MVs were distinctive from those of the reference site, and the communities of MVs were similar to each other at deeper depth levels. Chloroflexi, Actinobacteria, unclassified bacterial groups, and MCG_c of Crenarchaeota were predominant in the MVs, while Firmicutes, Deltaproteobacteria, and unclassified class of Thaumarchaeota were dominant in reference site. The relative abundance of dominant bacterial groups varied at sulfate-methane transition zone (SMTZ) of individual MVs. However, certain microbial taxa such as members of SAGMEG_o or Methanosarcinales of Euryarcheaota and Dehalococcoidales of Chloroflexi were predominant at SMTZs. Since they are not the classical representative taxa known to be involved in anaerobic oxidation of methane, their dominance implicates that they could be playing important roles in methane cycling using unrevealed mechanisms. We will further perform the phylogenetic and network analyses to infer mechanisms and interactions of dominant operational taxonomic units in controlling methane flux.
High rates of anaerobic oxidation of methane, ethane and propane coupled to thiosulphate reduction.
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.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Myers, Greg
This final report document summarizes the activities undertaken and the output from three primary deliverables generated during this project. This fifteen month effort comprised numerous key steps including the creation of an international methane hydrate science team, determining and reporting the current state of marine methane hydrate research, convening an international workshop to collect the ideas needed to write a comprehensive Marine Methane Hydrate Field Research Plan and the development and publication of that plan. The following documents represent the primary deliverables of this project and are discussed in summary level detail in this final report: Historical Methane Hydrate Projectmore » Review Report; Methane Hydrate Workshop Report; Topical Report: Marine Methane Hydrate Field Research Plan; and Final Scientific/Technical Report.« less
Martian methane plume models for defining Mars rover methane source search strategies
NASA Astrophysics Data System (ADS)
Nicol, Christopher; Ellery, Alex; Lynch, Brian; Cloutis, Ed
2018-07-01
The detection of atmospheric methane on Mars implies an active methane source. This introduces the possibility of a biotic source with the implied need to determine whether the methane is indeed biotic in nature or geologically generated. There is a clear need for robotic algorithms which are capable of manoeuvring a rover through a methane plume on Mars to locate its source. We explore aspects of Mars methane plume modelling to reveal complex dynamics characterized by advection and diffusion. A statistical analysis of the plume model has been performed and compared to analyses of terrestrial plume models. Finally, we consider a robotic search strategy to find a methane plume source. We find that gradient-based techniques are ineffective, but that more sophisticated model-based search strategies are unlikely to be available in near-term rover missions.
Microbial Methane Oxidation Rates in Guandu Wetland of northern Taiwan
NASA Astrophysics Data System (ADS)
Yu, Zih-Huei; Wang, Pei-Ling; Lin, Li-Hung
2016-04-01
Wetland is one of the major sources of atmospheric methane. The exact magnitude of methane emission is essentially controlled by microbial processes. Besides of methanogenesis, methanotrophy oxidizes methane with the reduction of various electron acceptors under oxic or anoxic conditions. The interplay of these microbial activities determines the final methane flux under different circumstances. In a tidal wetland, the cyclic flooding and recession of tide render oxygen and sulfate the dominant electron acceptors for methane oxidation. However, the details have not been fully examined, especially for the linkage between potential methane oxidation rates and in situ condition. In this study, a sub-tropical wetland in northern Taiwan, Guandu, was chosen to examine the tidal effect on microbial methane regulation. Several sediment cores were retrieved during high tide and low tide period and their geochemical profiles were characterized to demonstrate in situ microbial activities. Incubation experiments were conducted to estimate potential aerobic and anaerobic methane oxidation rates in surface and core sediments. Sediment cores collected in high tide and low tide period showed different geochemical characteristics, owning to tidal inundation. Chloride and sulfate concentration were lower during low tide period. A spike of enhanced sulfate at middle depth intervals was sandwiched by two sulfate depleted zones above and underneath. Methane was accumulated significantly with two methane depletion zones nearly mirroring the sulfate spike zone identified. During the high tide period, sulfate decreased slightly with depth with methane production inhibited at shallow depths. However, a methane consumption zone still occurred near the surface. Potential aerobic methane oxidation rates were estimated between 0.7 to 1.1 μmole/g/d, showing no difference between the samples collected at high tide or low tide period. However, a lag phase was widely observed and the lag phase lasted over a longer period of time for the samples collected in high tide period. It seems that aerobic methanotrophs needed a longer period of time to recovery and/or had low activities, since they had been suppressed by low oxygen concentration during high tide period. The rates of anaerobic methane oxidation ranged between 1.5 and 4.0 nmole/g/d for samples collected at high tide period, whereas lower rates ranging from 0.2 to 2.0 nmole/g/d were observed for samples at low tide period. The addition of basal salt solution apparently stimulated methane consumption significantly. Based on the field observation and laboratory incubations, our results indicated a dynamic shift of metabolic zonation in tidally influenced wetlands. Aerobic methanotrophy appears to outpace anaerobic methanotrophy by orders of magnitude regardless of tidal inundation. This together with methanogenesis regulated by the availability of sulfate and organic degradation plays a major role in controlling methane emission. While anaerobic methanotrophy is relatively minor in methane cycling, its linkage with the sulfate availability modulates the coupling of carbon and sulfur turnover under anoxic conditions.
NASA Astrophysics Data System (ADS)
Seabrook, S.; Thurber, A. R.; Embley, R. W.; Raineault, N.; Baumberger, T.; Merle, S. G.
2016-12-01
Methane seeps provide biogeochemical and microbial heterogeneity in deep-sea habitats. In June of 2016 the E/V Nautilus, exploring for methane seeps along the Cascadia continental margin, discovered over 450 bubble streams, indicative of active seepage, and collected biological samples at 6 of the resulting newly discovered seeps. These seeps covered a range of depths, latitudes, habitat types and biogeochemical environments and included: Juan de Fuca (150m), Astoria canyon (800m and 500m), Nehalem Bank (185m), Heceta SW (1200m), SW Coquille Bank (600m), and Klamath Knoll seep (700m). Geologic environment types included continental shelf, canyons and slopes, and these sites spanned the zone of hydrate stability and the Oxygen Minimum Zone. A range of seep-specific habitat were found and sampled including: reduced sediments, microbial mats, methane hydrates, clam beds (Calyptogena spp.), Siboglinidae tubeworm assemblages and sparse assemblages of stalked barnacles. Here, we present an initial characterization of the microbial communities collected via push cores by a remotely operated vehicle (ROV) at the six aforementioned sites. With high throughput amplicon sequencing of the V4-V5 region of the 16S rRNA gene, we characterize the diversity and microbial composition of the seep sites sampled. This characterization is furthered with digital drop PCR of the pmoA gene (involved with aerobic methanotrophy) to allow for a comparison of the community composition with functional gene abundance of critical microbial processes. These data will be placed in the greater biogeochemical context of the region, including direct comparison with paired gas-tight sampling at key locations. The results of these analyses will provide the first microbial description of this broad range of seep ecosystems along the Cascadia Margin adding to our overall understanding of microbial diversity, the dominant physiological processes at seep ecosystems, and the connection between community structure, function and biogeochemistry in habitats which we are just starting to appreciate for their ubiquity in marine environments.
Feng, L Y; Yang, L Q; Zhang, L X; Chen, H L; Chen, J
2013-01-01
Sludge with low organic content always results in an unsatisfactory performance, even failure of anaerobic digestion. The alkaline pretreatment effect on anaerobic digestion of sludge with low organic content has seldom been studied although it gives many benefits for sludge with high organic content. In this study the influence of alkaline pretreatment (pH 10, an effective alkaline pH) on the solubilization and methane production from waste activated sludge (WAS) with low organic content was investigated. Results from biochemical methane potential (BMP) experiments showed that anaerobic biodegradability of WAS was greatly improved by alkaline pretreatment at pH 10. Methane production from the current WAS under conditions of pretreatment time 4 h and digestion time 15 d was 139.6 mL/g VS (volatile solids), much higher than that from the unpretreated WAS with digestion time of 20 d (75.2 mL/g VS). Also, the solubilization of WAS was significantly accelerated by alkaline pretreatment. Mechanism exploration indicated that the general activities of anaerobic microorganisms, specific activities of key enzymes and the amounts of methanogens were enhanced by alkaline pretreatment at pH 10, showing good agreement with methane production.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Polk, A. C.; Gibson, C. M.; Shoemaker, N. T.
2013-05-24
This paper presents experimental analyses of the ignition delay (ID) behavior for diesel-ignited propane and diesel-ignited methane dual fuel combustion. Two sets of experiments were performed at a constant speed (1800 rev/min) using a 4-cylinder direct injection diesel engine with the stock ECU and a wastegated turbocharger. First, the effects of fuel-air equivalence ratios (© pilot ¼ 0.2-0.6 and © overall ¼ 0.2-0.9) on IDs were quantified. Second, the effects of gaseous fuel percent energy substitution (PES) and brake mean effective pressure (BMEP) (from 2.5 to 10 bar) on IDs were investigated. With constant © pilot (> 0.5), increasing ©more » overall with propane initially decreased ID but eventually led to premature propane autoignition; however, the corresponding effects with methane were relatively minor. Cyclic variations in the start of combustion (SOC) increased with increasing © overall (at constant © pilot), more significantly for propane than for methane. With increasing PES at constant BMEP, the ID showed a nonlinear (initially increasing and later decreasing) trend at low BMEPs for propane but a linearly decreasing trend at high BMEPs. For methane, increasing PES only increased IDs at all BMEPs. At low BMEPs, increasing PES led to significantly higher cyclic SOC variations and SOC advancement for both propane and methane. Finally, the engine ignition delay (EID) was also shown to be a useful metric to understand the influence of ID on dual fuel combustion.« less
NASA Astrophysics Data System (ADS)
Ji, Zhong-Min; Chen, Zhi-Jian; Pan, Jie-Nan; Niu, Qing-He
2017-12-01
As the world's largest coal producer and consumer, China accounts for a relatively high proportion of methane emissions from coal mines. Several estimation methods had been established for the coal mine methane (CMM) emission. However, with large regional differences, various reservoir formation types of coalbed methane (CBM) and due to the complicated geological conditions in China, these methods may be deficient or unsuitable for all the mining areas (e.g. Jiaozuo mining area). By combing the CMM emission characteristics and considering the actual situation of methane emissions from underground coal mine, we found that the methane pre-drainage is a crucial reason creating inaccurate evaluating results for most estimation methods. What makes it so essential is the extensive pre-drainage quantity and its irrelevance with annual coal production. Accordingly, the methane releases were divided into two categories: methane pre-drainage and methane release during mining. On this basis, a pioneering method for estimating CMM emissions was proposed. Taking the Yanma coal mine in the Jiaozuo mining area as a study case, the evaluation method of the pre-drainage methane quantity was established after the correlation analysis between the pre-drainage rate and time. Thereafter, the mining activity influence factor (MAIF) was first introduced to reflect the methane release from the coal and rock seams around where affected by mining activity, and the buried depth was adopted as the predictor of the estimation for future methane emissions. It was verified in the six coal mines of Jiaozuo coalfield (2011) that the new estimation method has the minimum errors of 12.11%, 9.23%, 5.77%, -5.20%, -8.75% and 4.92% respectively comparing with other methods. This paper gives a further insight and proposes a more accurate evaluation method for the CMM emissions, especially for the coal seams with low permeability and strong tectonic deformation in methane outburst coal mines.
Heterogeneous Nucleation of Methane Hydrate in a Water-Decane-Methane Emulsion
NASA Astrophysics Data System (ADS)
Shestakov, V. A.; Kosyakov, V. I.; Manakov, A. Yu.; Stoporev, A. S.; Grachev, E. V.
2018-07-01
Heterogeneous nucleation in disperse systems with metastable disperse phases plays an important role in the mechanisms of environmental and technological processes. The effect the concentration and activity of particles that initiate the formation of a new phase have on nucleation processes in such systems is considered. An approach is proposed that allows construction of a spectrum of particle activity characterizing the features of nucleation in a sample, based on the fraction of crystallized droplets depending on the level of supercooling and the use of Weibull's distribution. The proposed method is used to describe experimental data on the heterogeneous nucleation of methane hydrate in an emulsion in a water-decane-methane system.
Methanation of gas streams containing carbon monoxide and hydrogen
Frost, Albert C.
1983-01-01
Carbon monoxide-containing gas streams having a relatively high concentration of hydrogen are pretreated so as to remove the hydrogen in a recoverable form for use in the second step of a cyclic, essentially two-step process for the production of methane. The thus-treated streams are then passed over a catalyst to deposit a surface layer of active surface carbon thereon essentially without the formation of inactive coke. This active carbon is reacted with said hydrogen removed from the feed gas stream to form methane. The utilization of the CO in the feed gas stream is appreciably increased, enhancing the overall process for the production of relatively pure, low-cost methane from CO-containing waste gas streams.
Method of making improved gas storage carbon with enhanced thermal conductivity
Burchell, Timothy D [Oak Ridge, TN; Rogers, Michael R [Knoxville, TN
2002-11-05
A method of making an adsorbent carbon fiber based monolith having improved methane gas storage capabilities is disclosed. Additionally, the monolithic nature of the storage carbon allows it to exhibit greater thermal conductivity than conventional granular activated carbon or powdered activated carbon storage beds. The storage of methane gas is achieved through the process of physical adsorption in the micropores that are developed in the structure of the adsorbent monolith. The disclosed monolith is capable of storing greater than 150 V/V of methane [i.e., >150 STP (101.325 KPa, 298K) volumes of methane per unit volume of storage vessel internal volume] at a pressure of 3.5 MPa (500 psi).
DOE Office of Scientific and Technical Information (OSTI.GOV)
Doan, Hieu A.; Li, Zhanyong; Farha, Omar K.
In this study, the prospect of using copper oxide nanoclusters grown by atomic layer deposition on a porphyrin support for selective oxidation of methane to methanol was examined by means of density functional theory (DFT) calculations. Ab initio thermodynamic analysis indicates that an active site in the form of Cu(μ-O)Cu can be stabilized by activation in O2 at 465K. Furthermore, a moderate methane activation energy barrier (Ea=54kJ/mol) is predicted, and the hydrogen abstraction activity of the active site could be attributed to the radical character of the bridging oxygen. Methanol extraction in this system is limited by a thermodynamic barriermore » to desorption of ΔG=57kJ/mol at 473K; however, desorption can be facilitated by the addition of water in a “stepped conversion” process. Overall, our results indicate similar activity between porphyrin-supported copper oxide nanoclusters and existing Cu-exchanged zeolites and provide a computational proof-of-concept for utilizing functionalized organic linkers in metal-organic frameworks (MOFs) for selective oxidation of methane to methanol.« less
Doan, Hieu A.; Li, Zhanyong; Farha, Omar K.; ...
2018-04-08
In this study, the prospect of using copper oxide nanoclusters grown by atomic layer deposition on a porphyrin support for selective oxidation of methane to methanol was examined by means of density functional theory (DFT) calculations. Ab initio thermodynamic analysis indicates that an active site in the form of Cu(μ-O)Cu can be stabilized by activation in O2 at 465K. Furthermore, a moderate methane activation energy barrier (Ea=54kJ/mol) is predicted, and the hydrogen abstraction activity of the active site could be attributed to the radical character of the bridging oxygen. Methanol extraction in this system is limited by a thermodynamic barriermore » to desorption of ΔG=57kJ/mol at 473K; however, desorption can be facilitated by the addition of water in a “stepped conversion” process. Overall, our results indicate similar activity between porphyrin-supported copper oxide nanoclusters and existing Cu-exchanged zeolites and provide a computational proof-of-concept for utilizing functionalized organic linkers in metal-organic frameworks (MOFs) for selective oxidation of methane to methanol.« less
Hammond, K J; Humphries, D J; Crompton, L A; Kirton, P; Reynolds, C K
2015-11-01
Changes in diet carbohydrate amount and type (i.e., starch vs. fiber) and dietary oil supplements can affect ruminant methane emissions. Our objectives were to measure methane emissions, whole-tract digestibility, and energy and nitrogen utilization from growing dairy cattle at 2 body weight (BW) ranges, fed diets containing either high maize silage (MS) or high grass silage (GS), without or with supplemental oil from extruded linseed (ELS). Four Holstein-Friesian heifers aged 13 mo (BW range from start to finish of 382 to 526 kg) were used in experiment 1, whereas 4 lighter heifers aged 12 mo (BW range from start to finish of 292 to 419 kg) were used in experiment 2. Diets were fed as total mixed rations with forage dry matter (DM) containing high MS or high GS and concentrates in proportions (forage:concentrate, DM basis) of either 75:25 (experiment 1) or 60:40 (experiment 2), respectively. Diets were supplemented without or with ELS (Lintec, BOCM Pauls Ltd., Wherstead, UK; 260 g of oil/kg of DM) at 6% of ration DM. Each experiment was a 4 × 4 Latin square design with 33-d periods, with measurements during d 29 to 33 while animals were housed in respiration chambers. Heifers fed MS at a heavier BW (experiment 1) emitted 20% less methane per unit of DM intake (yield) compared with GS (21.4 vs. 26.6, respectively). However, when repeated with heifers of a lower BW (experiment 2), methane yield did not differ between the 2 diets (26.6g/kg of DM intake). Differences in heifer BW had no overall effect on methane emissions, except when expressed as grams per kilogram of digestible organic matter (OMD) intake (32.4 vs. 36.6, heavy vs. light heifers). Heavier heifers fed MS in experiment 1 had a greater DM intake (9.4kg/d) and lower OMD (755 g/kg), but no difference in N utilization (31% of N intake) compared with heifers fed GS (7.9 kg/d and 799 g/kg, respectively). Tissue energy retention was nearly double for heifers fed MS compared with GS in experiment 1 (15 vs. 8% of energy intake, respectively). Heifers fed MS in experiment 2 had similar DM intake (7.2 kg/d) and retention of energy (5% of intake energy) and N (28% of N intake), compared with GS-fed heifers, but OMD was lower (741 vs. 765 g/kg, respectively). No effect of ELS was noted on any of the variables measured, irrespective of animal BW, and this was likely due to the relatively low amount of supplemental oil provided. Differences in heifer BW did not markedly influence dietary effects on methane emissions. Differences in methane yield were attributable to differences in dietary starch and fiber composition associated with forage type and source. Copyright © 2015 American Dairy Science Association. Published by Elsevier Inc. All rights reserved.
Root biomass as a major means of affecting methane emissions
USDA-ARS?s Scientific Manuscript database
Human activities are contributing to greenhouse gas emissions. Methane, the second most abundant greenhouse gas, is ~25 times more potent in global warming potential than carbon dioxide, and 7-17% of atmospheric methane comes from paddy rice fields. The purpose of the study was to investigate gene...
75 FR 12796 - Petitions for Modification
Federal Register 2010, 2011, 2012, 2013, 2014
2010-03-17
... to continuously monitor methane, oxygen and carbon monoxide concentrations at the specified... activated for the following initial levels: (1) Oxygen: 19.4%; (2) Methane: 1.5%; (3) Carbon Monoxide: 8 ppm...: 19.0%: (2) Methane: 2.0%; and (3) Carbon Monoxide: 13 ppm; (d) if an AMS sensor indicates an alert...
Federal Register 2010, 2011, 2012, 2013, 2014
2013-02-19
... monitoring, accumulated refuse, surface methane monitoring, and collection and control system exceedances... included a burden item for Agency review of surface methane monitoring reports. Respondents, however, are... adjusted the calculations to exclude any Agency burden associated with surface methane monitoring. We have...
The key nickel enzyme of methanogenesis catalyses the anaerobic oxidation of methane.
Scheller, Silvan; Goenrich, Meike; Boecher, Reinhard; Thauer, Rudolf K; Jaun, Bernhard
2010-06-03
Large amounts (estimates range from 70 Tg per year to 300 Tg per year) of the potent greenhouse gas methane are oxidized to carbon dioxide in marine sediments by communities of methanotrophic archaea and sulphate-reducing bacteria, and thus are prevented from escaping into the atmosphere. Indirect evidence indicates that the anaerobic oxidation of methane might proceed as the reverse of archaeal methanogenesis from carbon dioxide with the nickel-containing methyl-coenzyme M reductase (MCR) as the methane-activating enzyme. However, experiments showing that MCR can catalyse the endergonic back reaction have been lacking. Here we report that purified MCR from Methanothermobacter marburgensis converts methane into methyl-coenzyme M under equilibrium conditions with apparent V(max) (maximum rate) and K(m) (Michaelis constant) values consistent with the observed in vivo kinetics of the anaerobic oxidation of methane with sulphate. This result supports the hypothesis of 'reverse methanogenesis' and is paramount to understanding the still-unknown mechanism of the last step of methanogenesis. The ability of MCR to cleave the particularly strong C-H bond of methane without the involvement of highly reactive oxygen-derived intermediates is directly relevant to catalytic C-H activation, currently an area of great interest in chemistry.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Mayernick, Adam D.; Janik, Michael J.
2010-12-24
Palladium/ceria exhibits unique catalytic activity for hydrocarbon oxidation; however, the chemical and structural properties of active sites on the palladium–ceria surface are difficult to characterize. Strong interactions between palladium and the ceria support stabilize oxidized Pd δ+ species, which may contribute to the significant activity of Pd/ceria for methane oxidation. We present a density functional theory (DFT + U) investigation into methane oxidation over Pd/ceria and quantify the activity of the Pd xCe 1-xO 2(1 1 1) mixed oxide surface in comparison with the PdO(1 0 0) and Pd(1 1 1) surfaces. The methane activation barrier is lowest over themore » Pd xCe 1-xO 2(1 1 1) surface, even lower than over the Pd(1 1 1) surface or low coordinated stepped or kinked Pd sites. Subsequent reaction steps in complete oxidation, including product desorption and vacancy refilling, are considered to substantiate that methane activation remains the rate-limiting step despite the low barrier over Pd xCe 1-xO 2(1 1 1). The low barrier over the Pd xCe 1-xO 2(1 1 1) surface demonstrates that mixed ceria-noble metal oxides offer the potential for improved hydrocarbon oxidation performance with respect to dispersed noble metal particles on ceria.« less
Methane oxidation on Pd–Ceria: A DFT study of the mechanism over PdxCe1-xO2, Pd, and PdO
DOE Office of Scientific and Technical Information (OSTI.GOV)
Mayernick, Adam D.; Janik, Michael J.
2011-02-14
Palladium/ceria exhibits unique catalytic activity for hydrocarbon oxidation; however, the chemical and structural properties of active sites on the palladium–ceria surface are difficult to characterize. Strong interactions between palladium and the ceria support stabilize oxidized Pdδ+ species, which may contribute to the significant activity of Pd/ceria for methane oxidation. We present a density functional theory (DFT + U) investigation into methane oxidation over Pd/ceria and quantify the activity of the Pd xCe 1-xO 2(1 1 1) mixed oxide surface in comparison with the PdO(1 0 0) and Pd(1 1 1) surfaces. The methane activation barrier is lowest over the Pdmore » xCe 1-xO 2(1 1 1) surface, even lower than over the Pd(1 1 1) surface or low coordinated stepped or kinked Pd sites. Subsequent reaction steps in complete oxidation, including product desorption and vacancy refilling, are considered to substantiate that methane activation remains the rate-limiting step despite the low barrier over Pd xCe 1-xO 2(1 1 1). The low barrier over the Pd xCe 1-xO 2(1 1 1) surface demonstrates that mixed ceria-noble metal oxides offer the potential for improved hydrocarbon oxidation performance with respect to dispersed noble metal particles on ceria.« less
NASA Astrophysics Data System (ADS)
Yamazaki, T.; Nakano, Y.; Monoe, D.; Oomi, T.; Doi, T.; Nakata, K.; Fukushima, T.
2005-05-01
Natural methane hydrate has been scientifically studied as a carbon reservoir globally. However, in Japan, the potential for energy resource has been industrially highlighted. There is less domestic oil and natural gas resources in Japan, but many potential deposition areas for methane hydrate in ocean around Japan are the reasons. Less CO2 discharge from methane compared with coal, oil and conventional natural gas when the same calorie value we get is considered as the advantage for energy resource. However, because methane hydrate distributes in shallower sediment layer in ocean floor, accidental leakage of methane may occur while we utilize methane hydrate. Methane itself has 21-times impact on the greenhouse effect, if it reaches the atmosphere. Therefore, it is necessary to estimate the behavior in the environment after the leakage, if we want to use methane hydrate as energy resource. The mass balance after leakage of methane on seafloor and in water column is numerically studied through the analyses of methane emissions from natural cold seepages and hydrothermal activities in this research. The outline structure of mass balance ecosystem model creating is introduced and some preliminary examination results from the test calculation are discussed.
Wang, Xuemei; Li, Zifu; Bai, Xue; Zhou, Xiaoqin; Cheng, Sikun; Gao, Ruiling; Sun, Jiachen
2018-02-01
Based on continuous anaerobic co-digestion of cow manure with available carbon slowly released corn straw, the effect of adding available carbon quickly released fruit and vegetable waste (FVW) was explored, meanwhile microbial community variation was studied in this study. When the FVW added was 5% and 1%, the methane production of the cow manure and corn straw was improved, and the start-up process was shortened. With higher proportion of FVW to 5%, the performance was superior with a mean methane yield increase of 22.4%, and a greater variation of bacterial communities was observed. FVW enhanced the variation of the bacterial communities. The microbial community structure changed during fermentation and showed a trend toward a diverse and balance system. Therefore, the available carbon quickly released FVW was helpful to improve the anaerobic co-digestion of the cow manure and available carbon slowly released corn straw. Copyright © 2017 Elsevier Ltd. All rights reserved.
Martian Methane From a Cometary Source: A Hypothesis
NASA Technical Reports Server (NTRS)
Fries, M.; Christou, A.; Archer, D.; Conrad, P.; Cooke, W.; Eigenbrode, J.; ten Kate, I. L.; Matney, M.; Niles, P.; Sykes, M.;
2016-01-01
In recent years, methane in the martian atmosphere has been detected by Earth-based spectroscopy, the Planetary Fourier Spectrometer on the ESA Mars Express mission, and the NASA Mars Science Laboratory. The methane's origin remains a mystery, with proposed sources including volcanism, exogenous sources like impacts and interplanetary dust, aqueous alteration of olivine in the presence of carbonaceous material, release from ancient deposits of methane clathrates, and/or biological activity. An additional potential source exists: meteor showers from the emission of large comet dust particles could generate martian methane via UV pyrolysis of carbon-rich infall material. We find a correlation between the dates of Mars/cometary orbit encounters and detections of methane on Mars. We hypothesize that cometary debris falls onto Mars during these interactions, generating methane via UV photolysis.
Understanding complete oxidation of methane on spinel oxides at a molecular level
Tao, Franklin Feng; Shan, Jun-jun; Nguyen, Luan; ...
2015-08-04
It is crucial to develop a catalyst made of earth-abundant elements highly active for a complete oxidation of methane at a relatively low temperature. NiCo 2O 4 consisting of earth-abundant elements which can completely oxidize methane in the temperature range of 350-550 °C. Being a cost-effective catalyst, NiCo 2O 4 exhibits activity higher than precious-metal-based catalysts. Here we report that the higher catalytic activity at the relatively low temperature results from the integration of nickel cations, cobalt cations and surface lattice oxygen atoms/oxygen vacancies at the atomic scale. Finally, in situ studies of complete oxidation of methane on NiCo 2Omore » 4 and theoretical simulations show that methane dissociates to methyl on nickel cations and then couple with surface lattice oxygen atoms to form -CH 3O with a following dehydrogenation to -CH 2O; a following oxidative dehydrogenation forms CHO; CHO is transformed to product molecules through two different sub-pathways including dehydrogenation of OCHO and CO oxidation.« less
Effect of packing material on methane activation in a dielectric barrier discharge reactor
DOE Office of Scientific and Technical Information (OSTI.GOV)
Jo, Sungkwon; Hoon Lee, Dae; Seok Kang, Woo
2013-12-15
The conversion of methane is measured in a planar-type dielectric barrier discharge reactor using γ-Al{sub 2}O{sub 3} (sphere), α-Al{sub 2}O{sub 3} (sphere), and γ-Al{sub 2}O{sub 3} (16–20 mesh). Investigations on the surface properties and shape of the three packing materials clearly indicate that methane activation is considerably affected by the material used. Capacitances inside the discharge gap are estimated from charge–voltage plots, and a comparison of the generated and transferred charges for different packing conditions show that the difference in surface properties between γ- and α-phase Al{sub 2}O{sub 3} affects the discharge characteristics. Moreover, all packing conditions show different chargemore » characteristics that are related to the electron density. Finally, the packing material's shape affects the local electron temperature, which is strongly related to methane conversion. The combined results indicate that both microscale and macroscale variations in a packing material affect the discharge characteristics, and a packing material should be considered carefully for effective methane activation.« less
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.
Lee, Jung-Yeol; Lee, Sang-Hoon; Park, Hee-Deung
2016-04-01
Direct interspecies electron transfer (DIET) via conductive materials can provide significant benefits to anaerobic methane formation in terms of production amount and rate. Although granular activated carbon (GAC) demonstrated its applicability in facilitating DIET in methanogenesis, DIET in continuous flow anaerobic reactors has not been verified. Here, evidences of DIET via GAC were explored. The reactor supplemented with GAC showed 1.8-fold higher methane production rate than that without GAC (35.7 versus 20.1±7.1mL-CH4/d). Around 34% of methane formation was attributed to the biomass attached to GAC. Pyrosequencing of 16S rRNA gene demonstrated the enrichment of exoelectrogens (e.g. Geobacter) and hydrogenotrophic methanogens (e.g. Methanospirillum and Methanolinea) from the biomass attached to GAC. Furthermore, anodic and cathodic currents generation was observed in an electrochemical cell containing GAC biomass. Taken together, GAC supplementation created an environment for enriching the microorganisms involved in DIET, which increased the methane production rate. Copyright © 2016 Elsevier Ltd. All rights reserved.
Trees as methane sources: A case study of West Siberian South taiga
NASA Astrophysics Data System (ADS)
Churkina, A. I.; Mochenov, S. Yu; Sabrekov, S. F.; Glagolev, M. V.; Il’yasov, D. V.; Terentieva, I. E.; Maksyutov, S. S.
2018-03-01
Within this study, we were measuring methane emission from the tree trunks, leaves and branches in the seasonally flooded forest and in the forested bogs (pine-shrub-sphagnum ecosystems or “ryams”) in south taiga zone of Western Siberia. Our results suggest that the tree trunks may act as a methane conductor from the soil to the atmosphere bypassing the methanotrophically active zones of soil. The tree methane flux depends on a trunk diameter and an ecosystem type. The average methane emission from tree trunks was 0.0061±0.0003 mg CH4·m-2·h-1 per unit of ground area. The methane emission from branches and leaves was zero.
NASA Astrophysics Data System (ADS)
Biddle, J. F.; Turich, C.; Brantley, S.; Bruns, M.
2002-12-01
Wetlands produce between 55 and 150 Tg of methane per year, or ~70% of all natural methane, and 20% of total methane (natural and anthropogenic). Understanding inputs to the global methane cycle depends on integrated in situ study of the sources and sinks of methane, as well as the rate and magnitude of methane production and consumption. Bear Meadows Natural Area in central Pennsylvania (N 40° 43.796' W 077° 45.310; 554 m elevation) contains an acidic, methane-producing, peaty bog with vegetation that is typical of wetlands at higher latitudes. In this four year study conducted within a cross-disciplinary training course offered by the NSF-IGERT Biogeochemical Research Initiative in Education (BRIE) program at Penn State University, graduate students applied a combination of geochemical and microbiological techniques to explore microbial diversity and activity in Bear Meadows sediments. The methane flux at the peat:water interface was highly variable, from 0.01 to over 3000 umol/m2/min in both sphagnum and sedge vegetation. The methane released from the bog had a carbon isotopic composition of -60 %o, typical of biogenic methane. Analysis of peat pore waters showed that the most methane was produced 30 cm below the peat:water interface, with a broad peak of methane in pore waters from 20-40 cm. At 21 cm below the peat:water interface, profiles of Archaeal 16S-23S ribosomal RNA spacer regions revealed the presence of populations having 92% similarity to 16S rRNA sequences of Methanoculleus marisnigri. Phospholipid fatty acids (PLFA) and compound specific isotope analysis revealed other biological controls on the methane cycle. PLFAs typical of methanotrophic bacteria were also present within peat cores from 20-30 cm below the water interface. The depleted carbon isotopic composition of these biomarkers (C16:1 and C18:1 fatty acids) was - 31.4 %o and - 33.8%o, indicative of methane oxidation. The presence of biomarkers of methane oxidizing bacteria within the zone of methane production may indicate that there is temporal or spatial heterogeneity in oxygen concentration within the peat. This interdisciplinary approach helped define specific ecological niches where novel methanogens and methane oxidizers may be active in a typical northern wetland. Through BRIE, on-going studies of the Bear Meadows wetland will focus on detecting other potentially novel aerobic and anaerobic microbes, and determining the biological influence on methane release to the atmosphere.
Bio-methane from an-aerobic digestion using activated carbon adsorption.
Farooq, Muhammad; Bell, Alexandra H; Almustapha, M N; Andresen, John M
2017-08-01
There is an increasing global demand for carbon-neutral bio-methane from an-aerobic digestion (AD) to be injected into national gas grids. Bio-gas, a methane -rich energy gas, is produced by microbial decomposition of organic matter through an-aerobic conditions where the presence of carbon dioxide and hydrogen sulphide affects its performance. Although the microbiological process in the AD can be tailored to enhance the bio-gas composition, physical treatment is needed to convert the bio-gas into bio-methane. Water washing is the most common method for upgrading bio-gas for bio-methane production, but its large use of water is challenging towards industrial scale-up. Hence, the present study focuses on scale-up comparison of water washing with activated-carbon adsorption using HYSYS and Aspen Process Economic Analyzer. The models show that for plants processing less than 500 m 3 /h water scrubbing was cost effective compared with activated carbon. However, against current fossil natural-gas cost of about 1 p/kWh in the UK both relied heavily on governmental subsidies to become economically feasible. For plants operating at 1000 m 3 /hr, the treatment costs were reduced to below 1.5 p/kWh for water scrubbing and 0.9 p/kWh for activated carbon where the main benefits of activated carbon were lower capital and operating costs and virtually no water losses. It is envisioned that this method can significantly aid the production of sustainable bio-methane. Copyright © 2017 Elsevier Ltd. All rights reserved.
NASA Astrophysics Data System (ADS)
Rapp, M.; Ehret, G.; Fix, A.; Wirth, M.; Amediek, A.; Kiemle, C.; Quatrevalet, M.; Butz, A.; Roiger, A.; Joeckel, P.
2017-12-01
For meeting the goals of the Paris agreement it is highly desirable to obtain objective global information on anthropogenic greenhouse gas emission rates. A promising approach for a space based observation system is the combination of active and passive remote sensing from satellites in Low Earth Orbit (LEO). While LIDAR techniques have the potential to yield low bias observations which are independent of solar illumination and hence also work during night and at polar winter latitudes, spectroscopic observations of scattered sunlight are suitable for imaging atmospheric concentrations at high spatial resolution. This presentation reviews progress and plans of work conducted at the German Aerospace Center (DLR). Regarding active remote sensing, DLR has developed the airborne Integrated Path Differential Absorption (IPDA)-Lidar CHARM-F (CO2 and CH4 Remote Monitoring—Flugzeug) for the quantification of carbon dioxide and methane column mixing ratios. CHARM-F has been deployed in an initial airborne field campaign in spring 2015 and results of strong anthropogenic sources detected during these flights will be presented. In addition, DLR is in the process of preparing an international airborne campaign (CoMet - Carbon Dioxide and Methane Mission for HALO) for April 2018 which will be supported by various in-situ, ground based, and modelling activities. These airborne field campaigns are important steps towards the German-French satellite mission MERLIN which also utilizes an IPDA-LIDAR. Also, DLR has started to further investigate concepts for a future space borne IPDA-Lidar for the quantification of strong anthropogenic CO2 point sources. Jointly with the latter, DLR is currently further studying the concept of a passive spectrometer for the observation of CO2 point emissions.
NASA Astrophysics Data System (ADS)
Krueger, Martin; Mazzini, Adriano; Scheeder, Georg; Blumenberg, Martin
2017-04-01
The Lusi eruption represents one of the largest ongoing sedimentary hosted geothermal systems, which started in 2006 following an earthquake on Java Island. Since then it has been continuously producing hot and hydrocarbon rich mud from a central crater with peaks reaching 180.000 m3 per day. Numerous investigations focused on the study of microbial communities which thrive at offshore methane and oil seeps and mud volcanoes, however very little has been done on onshore seeping structures. Lusi represents a unique opportunity to complete a comprehensive study of onshore microbial communities fed by the seepage of CH4 as well as of liquid hydrocarbons originating from one or more km below the surface. While the source of the methane at Lusi is unambiuous, the origin of the seeping oil is still discussed. Both, source and maturity estimates from biomarkers, are in favor of a type II/III organic matter source. Likely the oils were formed from the studied black shales (deeper Ngimbang Fm.) which contained a Type III component in the Type II predominated organic matter. In all samples large numbers of active microorganisms were present. Rates for aerobic methane oxidation were high, as was the potential of the microbial communities to degrade different hydrocarbons. The data suggests a transition of microbial populations from an anaerobic, hydrocarbon-driven metabolism in fresher samples from center or from small seeps to more generalistic, aerobic microbial communities in older, more consolidated sediments. Ongoing microbial activity in crater sediment samples under high temperatures (80-95C) indicate a deep origin of the involved microorganisms. First results of molecular analyses of the microbial community compositions confirm the above findings. This study represents an initial step to better understand onshore seepage systems and provides an ideal analogue for comparison with the better investigated offshore structures.
Surface modification processes during methane decomposition on Cu-promoted Ni–ZrO2 catalysts
Wolfbeisser, Astrid; Klötzer, Bernhard; Mayr, Lukas; Rameshan, Raffael; Zemlyanov, Dmitry; Bernardi, Johannes; Rupprechter, Günther
2015-01-01
The surface chemistry of methane on Ni–ZrO2 and bimetallic CuNi–ZrO2 catalysts and the stability of the CuNi alloy under reaction conditions of methane decomposition were investigated by combining reactivity measurements and in situ synchrotron-based near-ambient pressure XPS. Cu was selected as an exemplary promoter for modifying the reactivity of Ni and enhancing the resistance against coke formation. We observed an activation process occurring in methane between 650 and 735 K with the exact temperature depending on the composition which resulted in an irreversible modification of the catalytic performance of the bimetallic catalysts towards a Ni-like behaviour. The sudden increase in catalytic activity could be explained by an increase in the concentration of reduced Ni atoms at the catalyst surface in the active state, likely as a consequence of the interaction with methane. Cu addition to Ni improved the desired resistance against carbon deposition by lowering the amount of coke formed. As a key conclusion, the CuNi alloy shows limited stability under relevant reaction conditions. This system is stable only in a limited range of temperature up to ~700 K in methane. Beyond this temperature, segregation of Ni species causes a fast increase in methane decomposition rate. In view of the applicability of this system, a detailed understanding of the stability and surface composition of the bimetallic phases present and the influence of the Cu promoter on the surface chemistry under relevant reaction conditions are essential. PMID:25815163
Light-Dependent Aerobic Methane Oxidation Reduces Methane Emissions from Seasonally Stratified Lakes
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
Martian Atmospheric Methane Plumes from Meteor Shower Infall: A Hypothesis
NASA Technical Reports Server (NTRS)
Fries, M.; Christou, A.; Archer, D.; Conrad, P.; Cooke, W.; Eigenbrode, J.; ten Kate, I. L.; Matney, M.; Niles, P.; Sykes, M.
2016-01-01
Methane plumes in the martian atmosphere have been detected using Earth-based spectroscopy, the Planetary Fourier Spectrometer on the ESA Mars Express mission, and the NASA Mars Science Laboratory. The methane's origin remains a mystery, with proposed sources including volcanism, exogenous sources like impacts and interplanetary dust, aqueous alteration of olivine in the presence of carbonaceous material, release from ancient deposits of methane clathrates, and/or biological activity. To date, none of these phenomena have been found to reliably correlate with the detection of methane plumes. An additional source exists, however: meteor showers could generate martian methane via UV pyrolysis of carbon-rich infall material. We find a correlation between the dates of Mars/cometary orbit encounters and detections of methane on Mars. We hypothesize that cometary debris falls onto Mars during these interactions, depositing freshly disaggregated meteor shower material in a regional concentration. The material generates methane via UV photolysis, resulting in a localized "plume" of short-lived methane.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wilson, R.B. Jr.; Posin, B.M.; Chan, Yee Wai
The goal of this research is to develop catalysts that directly convert methane and light hydrocarbons to intermediates that later can be converted to either liquid fuels or value-added chemicals, as economics dictate. During this reporting period, we completed our IR spectroscopic examination of the Ru{sub 4}/MgO and FeRu{sub 3}/MgO systems under nitrogen and methane by examining FeRu{sub 3}/MgO under methane. This system behaved quite differently than the same system under nitrogen. Under methane, only one very broad peak is observed at room temperature. Upon heating, the catalyst transformed so that by 300{degrees}C, the spectrum of FeRu{sub 3}/MgO under methanemore » was the same as that of Ru{sub 4}/MgO. This suggests that methane promotes the segregation of the metals in the mixed metal system. The differences in catalytic activity between the FeRu{sub 3}/MgO and Ru{sub 4}/MgO systems may then be due to the presence of IR transparent species such as iron ions which cause different nucleation in the ruthenium clusters. We examined several systems for activity in the methane dehydrogenation reaction. Focusing on systems which produce C{sub 6} hydrocarbons since this is the most useful product. These systems all displayed low activity so that the amount of hydrocarbon product is very low. Some C{sub 6} hydrocarbon is observed over zeolite supports, but its production ceases after the first few hours of reaction. We prepared a new system, Ru{sub 4} supported on carbon, and examined its reactivity. Its activity was very low and in fact the carbon support had the same level of activity. We synthesized four new systems for examination as catalysts in the partial oxidation of methane. Three of these (PtTSPC/MgO, PtTSPC and PdTSPC on carbon) are analogs of PdTSPC/MgO. This system is of interest because we have observed the production of ethane from methane oxidation over PdTSPC/MgO at relatively low temperatures and we wished to explore its generality among close analogs.« less
Methane contamination of drinking water accompanying gas-well drilling and hydraulic fracturing
Osborn, Stephen G.; Vengosh, Avner; Warner, Nathaniel R.; Jackson, Robert B.
2011-01-01
Directional drilling and hydraulic-fracturing technologies are dramatically increasing natural-gas extraction. In aquifers overlying the Marcellus and Utica shale formations of northeastern Pennsylvania and upstate New York, we document systematic evidence for methane contamination of drinking water associated with shale-gas extraction. In active gas-extraction areas (one or more gas wells within 1 km), average and maximum methane concentrations in drinking-water wells increased with proximity to the nearest gas well and were 19.2 and 64 mg CH4 L-1 (n = 26), a potential explosion hazard; in contrast, dissolved methane samples in neighboring nonextraction sites (no gas wells within 1 km) within similar geologic formations and hydrogeologic regimes averaged only 1.1 mg L-1 (P < 0.05; n = 34). Average δ13C-CH4 values of dissolved methane in shallow groundwater were significantly less negative for active than for nonactive sites (-37 ± 7‰ and -54 ± 11‰, respectively; P < 0.0001). These δ13C-CH4 data, coupled with the ratios of methane-to-higher-chain hydrocarbons, and δ2H-CH4 values, are consistent with deeper thermogenic methane sources such as the Marcellus and Utica shales at the active sites and matched gas geochemistry from gas wells nearby. In contrast, lower-concentration samples from shallow groundwater at nonactive sites had isotopic signatures reflecting a more biogenic or mixed biogenic/thermogenic methane source. We found no evidence for contamination of drinking-water samples with deep saline brines or fracturing fluids. We conclude that greater stewardship, data, and—possibly—regulation are needed to ensure the sustainable future of shale-gas extraction and to improve public confidence in its use. PMID:21555547
Synthesis of single-site copper catalysts for methane partial oxidation
Grundner, S.; Luo, W.; Sanchez-Sanchez, M.; ...
2015-12-24
Cu-Exchanged zeolites are known as active materials for methane oxidation to methanol. However, understanding of the formation of Cu active species during synthesis, dehydration and activation is fragmented and rudimentary. We show here how a synthesis protocol guided by insight in the ion exchange elementary steps leads to highly uniform Cu species in mordenite (MOR).
Federal Register 2010, 2011, 2012, 2013, 2014
2012-08-08
... for OMB Review; Comment Request; Notification of Methane Detected in Underground Metal and Nonmetal... of Methane Detected in Underground Metal and Nonmetal Mine Atmospheres,'' to the Office of Management... following events occur: There is an outburst that results in 0.25 percent or more methane in the mine...
Freshwater wetland sediments support substantial rates of anaerobic oxidation of methane (AOM)
NASA Astrophysics Data System (ADS)
Segarra, K. E.; Samarkin, V.; Schubotz, F.; Yoshinaga, M. Y.; Hinrichs, K.; Joye, S. B.
2012-12-01
Freshwater wetlands are characterized by high rates of methanogenesis and are the single largest source of atmospheric methane. Anaerobic oxidation of methane (AOM), a previously underappreciated process in these systems, may be an important component in freshwater methane budgets. Here we report some of the first direct measurements of AOM in wetland sediments. We examined seasonal methane cycling within three freshwater wetlands (two peat wetlands and one tidal, freshwater creekbank) along the eastern coast of the US. Rates of AOM were high (up to 286 nmol per cubic cm per day) and varied on a seasonal basis. Despite low sulfate concentrations, rates of sulfate reduction were sufficient to support all the observed AOM activity, though rates of these two processes were not correlated. This study highlights the importance of AOM in freshwater sediments, where this process, in conjunction with sulfate reduction, may control emissions of methane to the atmosphere through competitive interactions with methanogens and the consumption of large fractions of the methane produced from acetate and hydrogen. The zone of maximum AOM activity was marked by enriched stable carbon isotopic signatures (δ13C) of methane and depleted signatures of DIC. However, the δ13C of archaeal and bacterial lipids were not indicative of methanotrophy. Studies that evaluate the role of AOM in wetlands using lipid and isotope-based approaches may therefore underestimate its importance.
Xu, Fuli; Liang, Yinli; Zhang, Chenge; Du, Sheni; Chen, Zhijie
2004-07-01
This paper studied the effect of fertilization on cucumber growth and yield, soil microbial biomass and soil enzyme activities in sunlight greenhouse in Loess Plateau. The results indicated that the growth and yield of cucumber were increased with application of manure and methane. Foliage application reduced the application rate of NP and manure. Fertilization had an obvious effect on the biological characteristics of soil in sunlight greenhouse. The number of bacteria was increased by manure and foliage fertilization, and that of fungi was increased by NP and methane fertilization but decreased by manure fertilization. Fertilization with manure, NP and methane also remarkably increased the number of actinomyces and the activities of urease, phosphatase and sucrase in soil. The activities of soil urease and phosphatase were increased by fertilization of manure, but little effect was found with fertilization of NP and methane.
NASA Astrophysics Data System (ADS)
Rella, Chris; Winkler, Renato; Sweeney, Colm; Karion, Anna; Petron, Gabrielle; Crosson, Eric
2014-05-01
Fugitive emissions of methane into the atmosphere are a major concern facing the natural gas production industry. Because methane is more energy-rich than coal per kg of carbon dioxide emitted into the atmosphere, it represents an attractive alternative to coal for electricity generation, provided that the fugitive emissions of methane are kept under control. A key step in assessing these emissions in a given region is partitioning the observed methane emissions between natural gas fugitive emissions and other sources of methane, such as from landfills or agricultural activities. One effective method for assessing the contribution of these different sources is stable isotope analysis, using the isotopic carbon signature to distinguish between natural gas and landfills or ruminants. We present measurements of methane using a mobile spectroscopic stable isotope analyzer based on cavity ringdown spectroscopy, in three intense natural gas producing regions of the United States: the Denver-Julesburg basin in Colorado, the Uintah basin in Utah, and the Barnett Shale in Texas. Performance of the CRDS isotope analyzer is presented, including precision, calibration, stability, and the potential for measurement bias due to other atmospheric constituents. Mobile isotope measurements of individual sources and in the nocturnal boundary layer have been combined to establish the fraction of the observed methane emissions that can be attributed to natural gas activities. The fraction of total methane emissions in the Denver-Julesburg basin attributed to natural gas emissions is 78 +/- 13%. In the Uinta basin, which has no other significant sources of methane, the fraction is 96% +/- 15%. In addition, results from the Barnett shale are presented, which includes a major urban center (Dallas / Ft. Worth). Methane emissions in this region are spatially highly heterogeneous. Spatially-resolved isotope and concentration measurements are interpreted using a simple emissions model to arrive at an overall isotope ratio for the region.
Methane-Stimulated Benthic Marine Nitrogen Fixation at Deep-Sea Methane Seeps
NASA Astrophysics Data System (ADS)
Dekas, A. E.; Orphan, V.
2011-12-01
Biological nitrogen fixation (the conversion of N2 to NH3) is a critical process in the oceans, counteracting the production of N2 gas by dissimilatory bacterial metabolisms and providing a source of bioavailable nitrogen to many nitrogen-limited ecosystems. Although current measurements of N2 production and consumption in the oceans indicate that the nitrogen cycle is not balanced, recent findings on the limits of nitrogen fixation suggest that the perceived imbalance is an artifact of an incomplete assessment of marine diazotrophy. One currently poorly studied and potentially underappreciated habitat for diazotrophic organisms is the sediments of the deep-sea. In the present study we investigate the distribution and magnitude of benthic marine diazotrophy at several active deep-sea methane seeps (Mound 12, Costa Rica; Eel River Basin, CA, USA; Hydrate Ridge, OR, USA; and Monterey Canyon, CA, USA). Using 15N2 and 15NH4 sediment incubation experiments followed by single-cell (FISH-NanoSIMS) and bulk isotopic analysis (EA-IRMS), we observed total protein synthesis (15N uptake from 15NH4) and nitrogen fixation (15N update from 15N2). The highest rates of nitrogen fixation observed in the methane seep sediment incubation experiments were over an order of magnitude greater than those previously published from non-seep deep-sea sediments (Hartwig and Stanley, Deep-Sea Research, 1978, 25:411-417). However, methane seep diazotrophy appears to be highly spatially variable, with sediments exhibiting no nitrogen fixation originating only centimeters away from sediments actively incorporating 15N from 15N2. The greatest spatial variability in diazotrophy was observed with depth in the sediment, and corresponded to steep gradients in sulfate and methane. The maximum rates of nitrogen fixation were observed within the methane-sulfate transition zone, where organisms mediating the anaerobic oxidation of methane are typically in high abundance. Additionally, incubation experiments without added methane were observed to have little to no nitrogen fixation activity. In previous work, we demonstrated the capability of uncultured methanotrophic archaea (ANME-2) to fix nitrogen when associated with sulfate reducing bacterial symbionts. These new results suggest that these microbes may be the dominant nitrogen-fixing organisms in methane seep sediment. Intriguingly, characterization of the diversity of nifH genes from our sediment incubations as well as published nifH sequences reported from other seep habitats suggest the potential for other diazotrophic microorganisms in addition to the ANME-2 archaea. To further explore this possibility, FISH-NanoSIMS analyses were conducted on two dominant free-living sulfate-reducing lineages from seep incubations demonstrating nitrogen fixation activity. Preliminary results from this analysis suggest that single cells belonging to the Desulfobulbaceae may also be involved in nitrogen fixation in methane seeps. Despite this demonstrated potential, the extent of methane-independent diazotrophy by non-ANME diazotrophs appears to be low within the methane seep environment. Further studies are necessary to assess the greater diversity and activity of diazotrophs in other deep-sea sedimentary habitats.
Methane distribution and oxidation around the Lena Delta in summer 2013
NASA Astrophysics Data System (ADS)
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) < 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 postulate the presence of a riverine methanotrophic population that is limited by sub-optimal temperatures and substrate concentrations and a polar methanotrophic population that is well adapted to the cold and methane-poor polar environment but limited by a lack of nitrogen. The diffusive methane flux into the atmosphere ranged from 4 to 163 µmol m2 d-1 (median 24). The diffusive methane flux accounted for a loss of 8 % of the total methane inventory of the investigated area, whereas the methanotrophic bacteria consumed only 1 % of this methane inventory. Our results underscore the importance of measuring the methane oxidation activities in polar estuaries, and they indicate a population-level differentiation between riverine and polar water methanotrophs.
Theoretical study on the gas-phase reaction mechanism between palladium monoxide and methane.
Yang, Hua-Qing; Hu, Chang-Wei; Gao, Chao; Yang, Meng-Yao; Li, Fang-Ming; Li, Cai-Qin; Li, Xiang-Yuan
2011-12-01
The gas-phase reaction mechanism between palladium monoxide and methane has been theoretically investigated on the singlet and triplet state potential energy surfaces (PESs) at the CCSD(T)/AVTZ//B3LYP/6-311+G(2d, 2p), SDD level. The major reaction channel leads to the products PdCH(2) + H(2)O, whereas the minor channel results in the products Pd + CH(3)OH, CH(2)OPd + H(2), and PdOH + CH(3). The minimum energy reaction pathway for the formation of main products (PdCH(2) + H(2)O), involving one spin inversion, prefers to start at the triplet state PES and afterward proceed along the singlet state PES, where both CH(3)PdOH and CH(3)Pd(O)H are the critical intermediates. Furthermore, the rate-determining step is RS-CH(3) PdOH → RS-2-TS1cb → RS-CH(2)Pd(H)OH with the rate constant of k = 1.48 × 10(12) exp(-93,930/RT). For the first C-H bond cleavage, both the activation strain ΔE(≠)(strain) and the stabilizing interaction ΔE(≠)(int) affect the activation energy ΔE(≠), with ΔE(≠)(int) in favor of the direct oxidative insertion. On the other hand, in the PdCH(2) + H(2) O reaction, the main products are Pd + CH(3)OH, and CH(3)PdOH is the energetically preferred intermediate. In the CH(2)OPd + H(2) reaction, the main products are Pd + CH(3)OH with the energetically preferred intermediate H(2)PdOCH(2). In the Pd + CH(3)OH reaction, the main products are CH(2)OPd + H(2), and H(2)PdOCH(2) is the energetically predominant intermediate. The intermediates, PdCH(2), H(2) PdCO, and t-HPdCHO are energetically preferred in the PdC + H(2), PdCO + H(2), and H(2)Pd + CO reactions, respectively. Besides, PdO toward methane activation exhibits higher reaction efficiency than the atom Pd and its first-row congener NiO. Copyright © 2011 Wiley Periodicals, Inc.
Activity and diversity of aerobic methanotrophs in a coastal marine oxygen minimum zone
NASA Astrophysics Data System (ADS)
Padilla, C. C.; Bristow, L. A.; Sarode, N. D.; Garcia-Robledo, E.; Girguis, P. R.; Thamdrup, B.; Stewart, F. J.
2016-02-01
The pelagic ocean is a sink for the potent greenhouse gas methane, with methane consumption regulated primarily by aerobic methane-oxidizing bacteria (MOB). Marine oxygen minimum zones (OMZs) contain the largest pool of pelagic methane in the oceans but remain largely unexplored for their potential to harbor MOB communities and contribute to methane cycling. Here, we present meta-omic and geochemical evidence that aerobic MOB are present and active in a coastal OMZ, in Golfo Dulce, Costa Rica. Oxygen concentrations were < 50 nM below 85 m, and sulfide accumulated below 140 m, with methane concentrations ranging from trace levels above the oxycline to 78 nM at 180 m. The upper OMZ (90 m) was characterized by an abundant MOB and methylotroph community representing diverse lineages of the Methylophilaceae, Methylophaga, and Methylococcales. Of these, Type I methanotrophs of the Order Methylococcales dominated , representing >5% of total 16S rRNA genes and >19% of 16S rRNA transcripts. This peak in ribosomal abundance and activity was affiliated with methane oxidation rates of 2.6 ± 0.7 nM d-1, measured in seawater incubations with estimated O2 concentrations of 50 nM. Rates fell to zero with the addition of acetylene, an inhibitor of aerobic methanotrophy. In contrast, methane oxidation was below detection at lower depths in the OMZ (100 m and 120 m). Metatranscriptome sequencing indicated a peak at 90 m in the expression of pathways essential to Methylococcales, including aerobic methanotrophy and the RuMP pathway of carbon assimilation, as well as the serine pathway of Type II methanotrophs. Preliminary analysis of single-cell genomes suggests distinct adaptations by Methylococcales from the Golfo Dulce, helping explain the persistence of putative aerobic methanotrophs under very low oxygen in this OMZ. Taken together, these data suggest the boundary layers of OMZs, despite extreme oxygen depletion, are a niche for aerobic MOBs and therefore potentially important zones of pelagic methane loss.
Liu, Yiwen; Ni, Bing-Jie; Sharma, Keshab R; Yuan, Zhiguo
2015-08-15
Recent studies have shown that sewer systems produce and emit a significant amount of methane. Methanogens produce methane under anaerobic conditions in sewer biofilms and sediments, and the stratification of methanogens and sulfate-reducing bacteria may explain the simultaneous production of methane and sulfide in sewers. No significant methane sinks or methanotrophic activities have been identified in sewers to date. Therefore, most of the methane would be emitted at the interface between sewage and atmosphere in gravity sewers, pumping stations, and inlets of wastewater treatment plants, although oxidation of methane in the aeration basin of a wastewater treatment plant has been reported recently. Online measurements have also revealed highly dynamic temporal and spatial variations in methane production caused by factors such as hydraulic retention time, area-to-volume ratio, temperature, and concentration of organic matter in sewage. Both mechanistic and empirical models have been proposed to predict methane production in sewers. Due to the sensitivity of methanogens to environmental conditions, most of the chemicals effective in controlling sulfide in sewers also suppress or diminish methane production. In this paper, we review the recent studies on methane emission from sewers, including the production mechanisms, quantification, modeling, and mitigation. Copyright © 2015 Elsevier B.V. All rights reserved.
Chawanakul, Sansanee; Chaiprasert, Pawinee; Towprayoon, Sirintornthep; Tanticharoen, Morakot
2009-01-01
Potential of methane production and trophic microbial activities at rhizospheric soil during rice cv. Supanbunri 1 cultivation were determined by laboratory anaerobic diluents vials. The methane production was higher from rhizospheric than non-rhizospheric soil, with the noticeable peaks during reproductive phase (RP) than vegetative phase (VP). Glucose, ethanol and acetate were the dominant available substrates found in rhizospheric soil during methane production at both phases. The predominance activities of trophic microbial consortium in methanogenesis, namely fermentative bacteria (FB), acetogenic bacteria (AGB), acetate utilizing bacteria (AB) and acetoclastic methanogens (AM) were also determined. At RP, these microbial groups were enhanced in the higher of methane production than VP. This correlates with our finding that methane production was greater at the rhizospheric soil with the noticeable peaks during RP (1,150 +/- 60 nmol g dw(-1) d(-1)) compared with VP (510 +/- 30 nmol g dw(-1) d(-1)). The high number of AM showed the abundant (1.1x10(4) cell g dw(-1)) with its high activity at RP, compared to the less activity with AM number at VP (9.8x10(2) cell g dw(-1)). Levels of AM are low in the total microbial population, being less than 1% of AB. These evidences revealed that the microbial consortium of these two phases were different.
Bomberg, Malin; Nyyssönen, Mari; Pitkänen, Petteri; Lehtinen, Anne; Itävaara, Merja
2015-01-01
Active microbial communities of deep crystalline bedrock fracture water were investigated from seven different boreholes in Olkiluoto (Western Finland) using bacterial and archaeal 16S rRNA, dsrB, and mcrA gene transcript targeted 454 pyrosequencing. Over a depth range of 296–798 m below ground surface the microbial communities changed according to depth, salinity gradient, and sulphate and methane concentrations. The highest bacterial diversity was observed in the sulphate-methane mixing zone (SMMZ) at 250–350 m depth, whereas archaeal diversity was highest in the lowest boundaries of the SMMZ. Sulphide-oxidizing ε-proteobacteria (Sulfurimonas sp.) dominated in the SMMZ and γ-proteobacteria (Pseudomonas spp.) below the SMMZ. The active archaeal communities consisted mostly of ANME-2D and Thermoplasmatales groups, although Methermicoccaceae, Methanobacteriaceae, and Thermoplasmatales (SAGMEG, TMG) were more common at 415–559 m depth. Typical indicator microorganisms for sulphate-methane transition zones in marine sediments, such as ANME-1 archaea, α-, β- and δ-proteobacteria, JS1, Actinomycetes, Planctomycetes, Chloroflexi, and MBGB Crenarchaeota were detected at specific depths. DsrB genes were most numerous and most actively transcribed in the SMMZ while the mcrA gene concentration was highest in the deep methane rich groundwater. Our results demonstrate that active and highly diverse but sparse and stratified microbial communities inhabit the Fennoscandian deep bedrock ecosystems. PMID:26425566
Fine-Scale Community Structure Analysis of ANME in Nyegga Sediments with High and Low Methane Flux
Roalkvam, Irene; Dahle, Håkon; Chen, Yifeng; Jørgensen, Steffen Leth; Haflidason, Haflidi; Steen, Ida Helene
2012-01-01
To obtain knowledge on how regional variations in methane seepage rates influence the stratification, abundance, and diversity of anaerobic methanotrophs (ANME), we analyzed the vertical microbial stratification in a gravity core from a methane micro-seeping area at Nyegga by using 454-pyrosequencing of 16S rRNA gene tagged amplicons and quantitative PCR. These data were compared with previously obtained data from the more active G11 pockmark, characterized by higher methane flux. A down core stratification and high relative abundance of ANME were observed in both cores, with transition from an ANME-2a/b dominated community in low-sulfide and low methane horizons to ANME-1 dominance in horizons near the sulfate-methane transition zone. The stratification was over a wider spatial region and at greater depth in the core with lower methane flux, and the total 16S rRNA copy numbers were two orders of magnitude lower than in the sediments at G11 pockmark. A fine-scale view into the ANME communities at each location was achieved through operational taxonomical units (OTU) clustering of ANME-affiliated sequences. The majority of ANME-1 sequences from both sampling sites clustered within one OTU, while ANME-2a/b sequences were represented in unique OTUs. We suggest that free-living ANME-1 is the most abundant taxon in Nyegga cold seeps, and also the main consumer of methane. The observation of specific ANME-2a/b OTUs at each location could reflect that organisms within this clade are adapted to different geochemical settings, perhaps due to differences in methane affinity. Given that the ANME-2a/b population could be sustained in less active seepage areas, this subgroup could be potential seed populations in newly developed methane-enriched environments. PMID:22715336
Mustapha, Nurul Asyifah; Sakai, Kenji; Shirai, Yoshihito; Maeda, Toshinari
2016-11-01
Anaerobic digestion is an effective method for reducing the by-product of waste-activated sludge (WAS) from wastewater treatment plants and for producing bioenergy from WAS. However, only a limited number of studies have attempted to improve anaerobic digestion by targeting the microbial interactions in WAS. In this study, we examined whether different antibiotics positively, negatively, or neutrally influence methane fermentation by evaluating changes in the microbial community and functions in WAS. Addition of azithromycin promoted the microbial communities related to the acidogenic and acetogenic stages, and a high concentration of soluble proteins and a high activity of methanogens were detected. Chloramphenicol inhibited methane production but did not affect the bacteria that contribute to the hydrolysis, acidogenesis, and acetogenesis digestion stages. The addition of kanamycin, which exhibits the same methane productivity as a control (antibiotic-free WAS), did not affect all of the microbial communities during anaerobic digestion. This study demonstrates the simultaneous functions and interactions of diverse bacteria and methanogenic Archaea in different stages of the anaerobic digestion of WAS. The ratio of Caldilinea, Methanosarcina, and Clostridium may correspond closely to the trend of methane production in each antibiotic. The changes in microbial activities and function by antibiotics facilitate a better understanding of bioenergy production.
Chemical identifications of possible martian hot spots
NASA Astrophysics Data System (ADS)
Wong, A. S.; Atreya, S. K.; Renno, N. O.
2003-04-01
If the interpretation of certain Mars Global Surveyor images indicating recent ground water seepage and surface runoff (1) is correct, it may imply that Mars can still be active internally in some places from time to time, and outgassing of certain molecules from the interior could occur with or without the water seepage. Although there is no evidence of active volcanism on Mars today, ``localized'' outgassing sources, the ``hot spots'', may not be ruled out. If outgassing does occur somewhere on Mars, water, carbon dioxide, sulfur species, methane, and to a lesser extent, halogens, would be the likely molecules of outgassing, based on the terrestrial analogs. The sulfur species, methane and halogens have not been detected in the ``global'' observations of Mars. Considering the possibility of outgassing from some localized hot spots, we have developed a one-dimensional photochemical model (2) that includes methane (CH_4), sulfur dioxide (SO_2) and hydrogen sulfide (H_2S), starting with their current ``global average'' upper limits of, respectively, 0.02, 0.1 and 0.1 ppm at the surface, and then progressively increasing their abundances above possible hot spots. Halogens are neglected as they are a minor product of the terrestrial outgassing sources. We find that the introduction of methane into the martian atmosphere results in the formation of mainly formaldehyde, methyl alcohol (CH_3OH) and ethane (C_2H_6), whereas the introduction of the sulfur species produces mainly sulfur monoxide (SO) and sulfuric acid (H_2SO_4). In a relatively short time of an hour, ordinary convective processes alone can reduce the mixing ratios of outgassed species by factors of 10^4 -- 10^5 approximately 50 km from the source, and the time for spreading the source material more or less uniformly over the planet (with corresponding dilution factor of ˜10^8) would be approximately one year. Depending upon the flux of the outgassed molecules from possible hot spots, some of these species, especially CH_4, SO_2, H_2S, and perhaps CH_2O, may be detectable locally, either by remote sensing or in situ measurements. References: (1) Malin, M. C. and K. S. Edgett, Science 288, 2330, 2000; (2) Wong, A. S., S. K. Atreya, and Th. Encrenaz, J. Geophys. Res., in press, 2003.
Oxygen-Promoted Methane Activation on Copper
Niu, Tianchao; Jiang, Zhao; Zhu, Yaguang; ...
2017-11-01
The role of oxygen in the activation of C–H bonds in methane on clean and oxygen-precovered Cu(111) and Cu 2O(111) surfaces was studied with combined in situ near-ambient-pressure scanning tunneling microscopy and X-ray photoelectron spectroscopy. Activation of methane at 300 K and “moderate pressures” was only observed on oxygen-precovered Cu(111) surfaces. Density functional theory calculations reveal that the lowest activation energy barrier of C–H on Cu(111) in the presence of chemisorbed oxygen is related to a two-active-site, four-centered mechanism, which stabilizes the required transition-state intermediate by dipole–dipole attraction of O–H and Cu–CH 3 species. Furthermore, the C–H bond activation barriersmore » on Cu 2O(111) surfaces are large due to the weak stabilization of H and CH 3 fragments.« less
Oxygen-Promoted Methane Activation on Copper
DOE Office of Scientific and Technical Information (OSTI.GOV)
Niu, Tianchao; Jiang, Zhao; Zhu, Yaguang
The role of oxygen in the activation of C–H bonds in methane on clean and oxygen-precovered Cu(111) and Cu 2O(111) surfaces was studied with combined in situ near-ambient-pressure scanning tunneling microscopy and X-ray photoelectron spectroscopy. Activation of methane at 300 K and “moderate pressures” was only observed on oxygen-precovered Cu(111) surfaces. Density functional theory calculations reveal that the lowest activation energy barrier of C–H on Cu(111) in the presence of chemisorbed oxygen is related to a two-active-site, four-centered mechanism, which stabilizes the required transition-state intermediate by dipole–dipole attraction of O–H and Cu–CH 3 species. Furthermore, the C–H bond activation barriersmore » on Cu 2O(111) surfaces are large due to the weak stabilization of H and CH 3 fragments.« less
Hurtado, Paloma; Ordóñez, Salvador; Vega, Aurelio; Díez, Fernando V
2004-05-01
The performance of different commercially available catalysts (supported Pd, Pt, Rh, bimetallic Pd-Pt, and Cr-Cu-Ti oxide catalyst) for the oxidation of methane, alone and in presence of ammonia and hydrogen sulphide is studied in this work. Catalysts performance was evaluated both in terms of activity and resistance to poisoning. The main conclusions are that supported Pd and Rh, present the highest activities for methane oxidation, both alone and in presence of ammonia, whereas they are severely poisoned in presence of H2S. Pt and Cr-Cu-Ti are less active but more sulphur resistant, but their activity is lower than the residual activity of sulphur-deactivated Pd and Rh catalysts. The Pd-Pt catalyst exhibits low activity and it is quickly deactivated in presence of hydrogen sulphide.
Microbial minorities modulate methane consumption through niche partitioning
Bodelier, Paul LE; Meima-Franke, Marion; Hordijk, Cornelis A; Steenbergh, Anne K; Hefting, Mariet M; Bodrossy, Levente; von Bergen, Martin; Seifert, Jana
2013-01-01
Microbes catalyze all major geochemical cycles on earth. However, the role of microbial traits and community composition in biogeochemical cycles is still poorly understood mainly due to the inability to assess the community members that are actually performing biogeochemical conversions in complex environmental samples. Here we applied a polyphasic approach to assess the role of microbial community composition in modulating methane emission from a riparian floodplain. We show that the dynamics and intensity of methane consumption in riparian wetlands coincide with relative abundance and activity of specific subgroups of methane-oxidizing bacteria (MOB), which can be considered as a minor component of the microbial community in this ecosystem. Microarray-based community composition analyses demonstrated linear relationships of MOB diversity parameters and in vitro methane consumption. Incubations using intact cores in combination with stable isotope labeling of lipids and proteins corroborated the correlative evidence from in vitro incubations demonstrating γ-proteobacterial MOB subgroups to be responsible for methane oxidation. The results obtained within the riparian flooding gradient collectively demonstrate that niche partitioning of MOB within a community comprised of a very limited amount of active species modulates methane consumption and emission from this wetland. The implications of the results obtained for biodiversity–ecosystem functioning are discussed with special reference to the role of spatial and temporal heterogeneity and functional redundancy. PMID:23788331
Microbial minorities modulate methane consumption through niche partitioning.
Bodelier, Paul L E; Meima-Franke, Marion; Hordijk, Cornelis A; Steenbergh, Anne K; Hefting, Mariet M; Bodrossy, Levente; von Bergen, Martin; Seifert, Jana
2013-11-01
Microbes catalyze all major geochemical cycles on earth. However, the role of microbial traits and community composition in biogeochemical cycles is still poorly understood mainly due to the inability to assess the community members that are actually performing biogeochemical conversions in complex environmental samples. Here we applied a polyphasic approach to assess the role of microbial community composition in modulating methane emission from a riparian floodplain. We show that the dynamics and intensity of methane consumption in riparian wetlands coincide with relative abundance and activity of specific subgroups of methane-oxidizing bacteria (MOB), which can be considered as a minor component of the microbial community in this ecosystem. Microarray-based community composition analyses demonstrated linear relationships of MOB diversity parameters and in vitro methane consumption. Incubations using intact cores in combination with stable isotope labeling of lipids and proteins corroborated the correlative evidence from in vitro incubations demonstrating γ-proteobacterial MOB subgroups to be responsible for methane oxidation. The results obtained within the riparian flooding gradient collectively demonstrate that niche partitioning of MOB within a community comprised of a very limited amount of active species modulates methane consumption and emission from this wetland. The implications of the results obtained for biodiversity-ecosystem functioning are discussed with special reference to the role of spatial and temporal heterogeneity and functional redundancy.
Upward revision of global fossil fuel methane emissions based on isotope database.
Schwietzke, Stefan; Sherwood, Owen A; Bruhwiler, Lori M P; Miller, John B; Etiope, Giuseppe; Dlugokencky, Edward J; Michel, Sylvia Englund; Arling, Victoria A; Vaughn, Bruce H; White, James W C; Tans, Pieter P
2016-10-06
Methane has the second-largest global radiative forcing impact of anthropogenic greenhouse gases after carbon dioxide, but our understanding of the global atmospheric methane budget is incomplete. The global fossil fuel industry (production and usage of natural gas, oil and coal) is thought to contribute 15 to 22 per cent of methane emissions to the total atmospheric methane budget. However, questions remain regarding methane emission trends as a result of fossil fuel industrial activity and the contribution to total methane emissions of sources from the fossil fuel industry and from natural geological seepage, which are often co-located. Here we re-evaluate the global methane budget and the contribution of the fossil fuel industry to methane emissions based on long-term global methane and methane carbon isotope records. We compile the largest isotopic methane source signature database so far, including fossil fuel, microbial and biomass-burning methane emission sources. We find that total fossil fuel methane emissions (fossil fuel industry plus natural geological seepage) are not increasing over time, but are 60 to 110 per cent greater than current estimates owing to large revisions in isotope source signatures. We show that this is consistent with the observed global latitudinal methane gradient. After accounting for natural geological methane seepage, we find that methane emissions from natural gas, oil and coal production and their usage are 20 to 60 per cent greater than inventories. Our findings imply a greater potential for the fossil fuel industry to mitigate anthropogenic climate forcing, but we also find that methane emissions from natural gas as a fraction of production have declined from approximately 8 per cent to approximately 2 per cent over the past three decades.
Transition metal sulfide loaded catalyst
Maroni, Victor A.; Iton, Lennox E.; Pasterczyk, James W.; Winterer, Markus; Krause, Theodore R.
1994-01-01
A zeolite based catalyst for activation and conversion of methane. A zeolite support includes a transition metal (Mo, Cr or W) sulfide disposed within the micropores of the zeolite. The catalyst allows activation and conversion of methane to C.sub.2 + hydrocarbons in a reducing atmosphere, thereby avoiding formation of oxides of carbon.
30 CFR 57.22206 - Main ventilation failure (I-A, II-A, III, and V-A mines).
Code of Federal Regulations, 2010 CFR
2010-07-01
... AND NONMETAL MINES Safety Standards for Methane in Metal and Nonmetal Mines Ventilation § 57.22206..., tests for methane shall be conducted in affected active workings until normal air flow has resumed. (b... less than 1.0 percent methane. Persons other than examiners shall not reenter a Subcategory II-A mine...
Commercial-scale utilization of greenhouse residues.
Maroušek, Josef; Kondo, Yoshikazu; Ueno, Masami; Kawamitsu, Yoshinobu
2013-01-01
Development of techniques utilizing waste without any additional energy or rare catalysts is a starting point for becoming sustainable. In the present work, the complex utilization of greenhouse residues was studied on a commercial scale. Only the energy produced by the process (8%) was used to run the technology, thanks to multilevel heat recuperation and high methane yields (over 340 m(3) volatile solid t(-1) ). Manifestations of labile carbon in relation to available nitrogen, methane yields, and the formation of inhibitors were investigated in detail. The results sweep away many false beliefs about the ratios of carbon to nitrogen and highlight the role of the availability of carbon in phytomass utilization. © 2013 International Union of Biochemistry and Molecular Biology, Inc.
Clumped isotopologue constraints on the origin of methane at seafloor hot springs
NASA Astrophysics Data System (ADS)
Wang, David T.; Reeves, Eoghan P.; McDermott, Jill M.; Seewald, Jeffrey S.; Ono, Shuhei
2018-02-01
Hot-spring fluids emanating from deep-sea vents hosted in unsedimented ultramafic and mafic rock commonly contain high concentrations of methane. Multiple hypotheses have been proposed for the origin(s) of this methane, ranging from synthesis via reduction of aqueous inorganic carbon (∑CO2) during active fluid circulation to leaching of methane-rich fluid inclusions from plutonic rocks of the oceanic crust. To further resolve the process(es) responsible for methane generation in these systems, we determined the relative abundances of several methane isotopologues (including 13CH3D, a "clumped" isotopologue containing two rare isotope substitutions) in hot-spring source fluids sampled from four geochemically-distinct hydrothermal vent fields (Rainbow, Von Damm, Lost City, and Lucky Strike). Apparent equilibrium temperatures retrieved from methane clumped isotopologue analyses average 310-42+53 °C, with no apparent relation to the wide range of fluid temperatures (96-370 °C) and chemical compositions (pH, [H2], [∑CO2], [CH4]) represented. Combined with very similar bulk stable isotope ratios (13C/12C and D/H) of methane across the suite of hydrothermal fluids, all available geochemical and isotopic data suggest a common mechanism of methane generation at depth that is disconnected from active fluid circulation. Attainment of equilibrium amongst methane isotopologues at temperatures of ca. 270-360 °C is compatible with the thermodynamically-favorable reduction of CO2 to CH4 at temperatures at or below ca. 400 °C under redox conditions characterizing intrusive rocks derived from sub-ridge melts. Collectively, the observations support a model where methane-rich aqueous fluids, known to be trapped in rocks of the oceanic lithosphere, are liberated from host rocks during hydrothermal circulation and perhaps represent the major source of methane venting with thermal waters at unsedimented hydrothermal fields. The results also provide further evidence that water-rock reactions occurring at temperatures lower than 200 °C do not contribute significantly to the quantities of methane venting at mid-ocean ridge hot springs.
Rainfall, Plant Communities and Methane Fluxes in the Ka`au Crater Wetland, Oahu, Hawaii
NASA Astrophysics Data System (ADS)
Grand, M.; Gaidos, E.
2003-12-01
Tropical wetlands constitute a major source of methane, an atmospheric greenhouse gas. Net methane emission in freshwater settings is the result of organic matter decomposition under anaerobic conditions modulated by aerobic methane oxidation and is thus also an indicator of wetland ecosystem processes. This study is monitoring the methane flux from the Ka`au crater wetland on the island of Oahu (Hawaii) and correlating it with environmental parameters such as precipitation and sunlight. We are obtaining precipitation, Photosynthetic Active Radiation (PAR), and water table level data with data loggers and are correlating these data with static chamber methane flux measurements and measurements of soil methane production potential. Additionally, our research is studying the effects of changes in vegetation type, i.e., of the invasive strawberry guava tree (Psidium Cattleianum) on the wetland methane emissions. Changes in soil chemistry and in the transport of gases by roots that accompany such vegetation change are a potential driver of methane flux modifications that have not been previously examined. Strawberry guava forms dense mats of surface roots that may change soil gas exchange and prolific fruiting may raise the soil organic content. We collected soil samples along a 30 meter transect that extends through two vegetation patterns; the strawberry guava canopy and the sedge meadow (Cladium Leptostachyum). Samples were incubated for 24 hours to estimate their methane generation potential. Our preliminary results show that methane generation potential is greater under the strawberry guava canopy. However, 2 of the 15 samples collected in the sedge meadow section of the transect did not match this pattern. Soil organic carbon content is slightly higher in the strawberry guava than in the sedge. We recorded a 90% decrease in methane generation potential in sedge meadow soils during a dry period relative to a wet period 2 months earlier. We propose that this change reflects a difference in the relative activity of microorganisms in the oxic and anoxic parts of the soil column. We will use environmental molecular technique to compare the microbial community component responsible for the production of methane in the different wetland soils.
NASA Astrophysics Data System (ADS)
Rella, C.; Jacobson, G. A.; Crosson, E.; Sweeney, C.; Karion, A.; Petron, G.
2012-12-01
Fugitive emissions of methane into the atmosphere are a major concern facing the natural gas production industry. Given that the global warming potential of methane is many times greater than that of carbon dioxide (Forster et al. 2007), the importance of quantifying methane emissions becomes clear. Companion presentations at this meeting describe efforts to quantify the overall methane emissions in two separate gas producing areas in Colorado and Utah during intensive field campaigns undertaken in 2012. A key step in the process of assessing the emissions arising from natural gas production activities is partitioning the observed methane emissions between natural gas fugitive emissions and other sources of methane, such as from landfills or agricultural activities. One method for assessing the contribution of these different sources is stable isotope analysis. In particular, the δ13CH4 signature of natural gas (-37 permil) is significantly different that the signature of other significant sources of methane, such as landfills or ruminants (-50 to -70 permil). In this paper we present measurements of δ13CH4 in Colorado in Weld County, a region of intense natural gas production, using a mobile δ13CH4¬ analyzer capable of high-precision measurements of the stable isotope ratio of methane at ambient levels. This analyzer was used to make stable isotope measurements at a fixed location near the center of the gas producing region, from which an overall isotope ratio for the regional emissions is determined. In addition, mobile measurements in the nocturnal boundary layer have been made, over a total distance of 150 km throughout Weld County, allowing spatially resolved measurements of this isotope signature. Finally, this analyzer was used to quantify the isotopic signature of those individual sources (natural gas fugitive emissions, concentrated animal feeding operations, and landfills) that constitute the majority of methane emissions in this region, by making measurements of the isotope ratio directly in the downwind plume from each source. These data are combined to establish the fraction of the observed methane emissions that can be attributed to natural gas activities in the region. The results are compared to inventories as well as other measurement techniques, and the uncertainty of the measurement is estimated.
NASA Technical Reports Server (NTRS)
Brabbs, T. A.; Robertson, T. F.
1986-01-01
Ignition delay data were recorded for three methane-oxygen-argon mixtures (phi = 0.5, 1.0, 2.0) for the temperature range 1500 to 1920 K. Quiet pressure trances enabled us to obtain delay times for the start of the experimental pressure rise. These times were in good agreement with those obtained from the flame band emission at 3700 A. The data correlated well with the oxygen and methane dependence of Lifshitz, but showed a much stronger temperature dependence (phi = 0.5 delta E = 51.9, phi = 1.0 delta = 58.8, phi = 2.0 delta E = 58.7 Kcal). The effect of probe location on the delay time measurement was studied. It appears that the probe located 83 mm from the reflecting surface measured delay times which may not be related to the initial temperature and pressure. It was estimated that for a probe located 7 mm from the reflecting surface, the measured delay time would be about 10 microseconds too short, and it was suggested that delay times less than 100 microsecond should not be used. The ignition period was defined as the time interval between start of the experimental pressure rise and 50 percent of the ignition pressure. This time interval was measured for three gas mixtures and found to be similar (40 to 60 micro sec) for phi = 1.0 and 0.5 but much longer (100 to 120) microsecond for phi = 2.0. It was suggested that the ignition period would be very useful to the kinetic modeler in judging the agreement between experimental and calculated delay times.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Welsch, Ralph, E-mail: rwelsch@uni-bielefeld.de; Manthe, Uwe, E-mail: uwe.manthe@uni-bielefeld.de
2015-02-14
Initial state-selected reaction probabilities of the H + CH{sub 4} → H{sub 2} + CH{sub 3} reaction are calculated in full and reduced dimensionality on a recent neural network potential [X. Xu, J. Chen, and D. H. Zhang, Chin. J. Chem. Phys. 27, 373 (2014)]. The quantum dynamics calculation employs the quantum transition state concept and the multi-layer multi-configurational time-dependent Hartree approach and rigorously studies the reaction for vanishing total angular momentum (J = 0). The calculations investigate the accuracy of the neutral network potential and study the effect resulting from a reduced-dimensional treatment. Very good agreement is found betweenmore » the present results obtained on the neural network potential and previous results obtained on a Shepard interpolated potential energy surface. The reduced-dimensional calculations only consider motion in eight degrees of freedom and retain the C{sub 3v} symmetry of the methyl fragment. Considering reaction starting from the vibrational ground state of methane, the reaction probabilities calculated in reduced dimensionality are moderately shifted in energy compared to the full-dimensional ones but otherwise agree rather well. Similar agreement is also found if reaction probabilities averaged over similar types of vibrational excitation of the methane reactant are considered. In contrast, significant differences between reduced and full-dimensional results are found for reaction probabilities starting specifically from symmetric stretching, asymmetric (f{sub 2}-symmetric) stretching, or e-symmetric bending excited states of methane.« less
Greenhouse Gas Fluxes at the Tablelands, NL, Canada: A Site of Active Serpentinization
NASA Astrophysics Data System (ADS)
Morrill, P. L.; Morrissey, L. S.; Cumming, E.
2016-12-01
Active sites of serpentinization have been proposed as sites for carbon capture and storage (CCS) projects. However, in addition to their ability to convert carbon dioxide to carbonate rock, sites of serpentinization also have the potential release methane, which is a more power greenhouse gas than carbon dioxide. Very little is known about the natural flux of carbon dioxide sequestered and methane released into the atmosphere from active sites of serpentinization. In this study we measured carbon dioxide, methane, and nitrous oxide gas fluxes at a pool of ultra-basic water discharging from serpentinized rock in Winterhouse Canyon, Gros Morne, Newfoundland. We found that the flux of methane released was 4.6 x 10-7 mol/m2/min and the carbon dioxide sequestered was 1.9 x 10-5 mol/m2/min, while the concentrations of nitrous oxide showed little change. Based on these fluxes we calculated predictive climate change parameters such as net radiative forcing and global warming potential which predicted that despite the methane being released the site still had an overall long-term atmospheric cooling effect based on the natural rate of carbon dioxide sequestration.
Bimetallo-radical carbon-hydrogen bond activation of methanol and methane.
Cui, Weihong; Zhang, X Peter; Wayland, Bradford B
2003-04-30
Carbon-hydrogen bond cleavage reactions of CH3OH and CH4 by a dirhodium(II) diporphyrin complex with a m-xylyl tether (.Rh(m-xylyl)Rh.(1)) are reported. Kinetic-mechanistic studies show that the substrate reactions are bimolecular and occur through the use of two Rh(II) centers in the molecular unit of 1. Second-order rate constants (T = 296 K) for the reactions of 1 with methanol (k(CH3OH) = 1.45 x 10-2 M-1 s-1) and methane (k(CH4) = 0.105 M-1 s-1) show a clear kinetic preference for the methane activation process. The methanol and methane reactions with 1 have large kinetic isotope effects (k(CH3OH)/k(CD3OD) = 9.7 +/- 0.8, k(CH4)/k(CD4) = 10.8 +/- 1.0, T = 296 K), consistent with a rate-limiting step of C-H bond homolysis through a linear transition state. Activation parameters for reaction of 1 with methanol (DeltaH = 15.6 +/- 1.0 kcal mol-1; DeltaS = -14 +/- 5 cal K-1 mol-1) and methane (DeltaH = 9.8 +/- 0.5 kcal mol-1; DeltaS = -30 +/- 3 cal K-1 mol-1) are reported.
Study of Methanogenesis while Bioutilisation of Plant Residuals
NASA Astrophysics Data System (ADS)
Ilyin, V. K.; Korniushenkova, I. N.; Starkova, L. V.; Lauriniavichius, K. S.
respect principals of planet ecology, and compatibility with other habitability systems. For these purpose the waste management technologies, relevant to application of the biodegradation properties of bacteria are of great value. Biological treatment method is based upon the biodegradation of organic substances by various microorganisms. vegetable non-edible residual, using artificial inoculum; to study peculiarities of biogas, possibilities to optimize or to reduce the share of methane. fermentation. The biogas production achieved 46 l per 1 kg of substrate. The microbial studies of biodegradation process revealed following peculiarities: (i)gradual quantitative increasing of Lactobacillus sp. (from 103 to 105 colony forming units (CFU) per ml); (ii)activation of Clostridia sp. (from 102 to 104 CFU/ml); (iii) elimination of aerobic conventional pathogens (Enterobacteriaceae sp., Protea sp., staphylococci). methane content measures revealed traces 0.1-0.4%. granules, the amount of methane in biogas reached 80-90%. biodegradation of vegetable wastes. This inoculum consists of active sludge adapted to wastes mixed with excretes of insects which consume plant wastes. Using this inoculum the biodegradation process takes less time, then that using active sludge. Regulation of methane concentration from traces to 90% may be achieved by adding of methane reactor to the plant digester.
Methane Leak Rates from Natural Gas Wells in Norther California
NASA Astrophysics Data System (ADS)
Cui, Y.; Yoon, S.; Chen, Y.; Falk, M.; Kuwayama, T.; Croes, B. E.; Herner, J.; Vijayan, A.
2017-12-01
Methane is a potent greenhouse gas (GHG) and is the second most prevalent GHG emitted in California from human activities. As part of a comprehensive effort to reduce GHG emissions and meet the statewide climate goals, California has proposed a Short Lived Climate Pollutant (SLCP) Strategy that includes a 40% reduction of methane emissions from 2013 levels by 2030, with goals to reduce oil and gas related emissions and capture methane emissions from dairy operations and organic waste. There is growing evidence in the recent scientific literature suggesting that methane emissions can come from every stage of the oil and gas supply chain. During oil and gas production operations, studies reported that a small number of oil and gas wells made up a large fraction of total methane emissions from the wells. In such a fat-tail distribution, the mean methane leak rate from wells is orders of magnitude larger than the median, which indicates the presence of super emitter sources. However, since the super emitters are often positioned as outliers in a fat-tail distribution and do not always behave consistently, measuring their leak rates is challenging, but critical to quantify their impacts and identify potential mitigation opportunities. This presentation will discuss of methane leak rates measured from natural gas wells in Northern California for different well operations: active, idle, and plugged. The leak rates demonstrated fat-tail distributions, and the mean leak rates for each well operation status were an order of magnitude higher than the median leak rates. It was also observed that roughly 20% of wells contributed more than 80% of methane emissions. Further data collection is needed with a larger number of samples to better understand the relationship between the leak rates and well operation status. Such measurements could help improve the estimate of methane emissions from natural gas wells and inform methane reduction policies and programs in California.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Miller, Benjamin L.; Arntzen, Evan V.; Goldman, Amy E.
The United States is home to more than 87,000 dams, 2,198 of which are actively used for hydropower production. With the December 2015 consensus adoption of the United Nations Framework Convention on Climate Change’s Paris Agreement, it is imperative for the U.S. to accurately quantify greenhouse gas fluxes from its hydropower reservoirs. Methane ebullition, or methane bubbles originating from river or lake sediments, can account for nearly all of a reservoir’s methane emissions to the atmosphere. However, methane ebullition in hydropower reservoirs has been studied in only three temperate locations, none of which are in the United States. This studymore » measures high ebullitive methane fluxes from two hydropower reservoirs in eastern Washington, synthesizes the known information about methane ebullition from tropical, boreal, and temperate hydropower reservoirs, and investigates the implications for U.S. hydropower management and growth.« less
Three-Dimensional Model Synthesis of the Global Methane Cycle
NASA Technical Reports Server (NTRS)
Fung, I.; Prather, M.; John, J.; Lerner, J.; Matthews, E.
1991-01-01
A synthesis of the global methane cycle is presented to attempt to generate an accurate global methane budget. Methane-flux measurements, energy data, and agricultural statistics are merged with databases of land-surface characteristics and anthropogenic activities. The sources and sinks of methane are estimated based on atmospheric methane composition and variations, and a global 3D transport model simulates the corresponding atmospheric responses. The geographic and seasonal variations of candidate budgets are compared with observational data, and the available observations are used to constrain the plausible methane budgets. The preferred budget includes annual destruction rates and annual emissions for various sources. The lack of direct flux measurements in the regions of many of these fluxes makes the unique determination of each term impossible. OH oxidation is found to be the largest single term, although more measurements of this and other terms are recommended.
Costa, J C; Gonçalves, P R; Nobre, A; Alves, M M
2012-06-01
Biochemical methane potential of four species of Ulva and Gracilaria genus was assessed in batch assays at mesophilic temperature. The results indicate a higher specific methane production (per volatile solids) for one of the Ulva sp. compared with other macroalgae and for tests running with 2.5% of total solids (196±9 L CH(4) kg(-1)VS). Considering that macroalgae can potentially be a post treatment of municipal wastewater for nutrients removal, co-digestion of macroalgae with waste activated sludge (WAS) was assessed. The co-digestion of macroalgae (15%) with WAS (85%) is feasible at a rate of methane production 26% higher than WAS alone without decreasing the overall biodegradability of the substrate (42-45% methane yield). The use of anoxic marine sediment as inoculum had no positive effect on the methane production in batch assays. The limiting step of the overall anaerobic digestion process was the hydrolysis. Copyright © 2012 Elsevier Ltd. All rights reserved.
Interactions of Methylotrophs with Plants and Other Heterotrophic Bacteria
Iguchi, Hiroyuki; Yurimoto, Hiroya; Sakai, Yasuyoshi
2015-01-01
Methylotrophs, which can utilize methane and/or methanol as sole carbon and energy sources, are key players in the carbon cycle between methane and CO2, the two most important greenhouse gases. This review describes the relationships between methylotrophs and plants, and between methanotrophs (methane-utilizers, a subset of methylotrophs) and heterotrophic bacteria. Some plants emit methane and methanol from their leaves, and provide methylotrophs with habitats. Methanol-utilizing methylotrophs in the genus Methylobacterium are abundant in the phyllosphere and have the ability to promote the growth of some plants. Methanotrophs also inhabit the phyllosphere, and methanotrophs with high methane oxidation activities have been found on aquatic plants. Both plant and environmental factors are involved in shaping the methylotroph community on plants. Methanotrophic activity can be enhanced by heterotrophic bacteria that provide growth factors (e.g., cobalamin). Information regarding the biological interaction of methylotrophs with other organisms will facilitate a better understanding of the carbon cycle that is driven by methylotrophs. PMID:27682083
Kim, Jaai; Kim, Hakchan; Baek, Gahyun; Lee, Changsoo
2017-02-01
Proper management of spent coffee grounds has become a challenging problem as the production of this waste residue has increased rapidly worldwide. This study investigated the feasibility of the anaerobic co-digestion of spent coffee ground with various organic wastes, i.e., food waste, Ulva, waste activated sludge, and whey, for biomethanation. The effect of co-digestion was evaluated for each tested co-substrate in batch biochemical methane potential tests by varying the substrate mixing ratio. Co-digestion with waste activated sludge had an apparent negative effect on both the yield and production rate of methane. Meanwhile, the other co-substrates enhanced the reaction rate while maintaining methane production at a comparable or higher level to that of the mono-digestion of spent coffee ground. The reaction rate increased with the proportion of co-substrates without a significant loss in methanation potential. These results suggest the potential to reduce the reaction time and thus the reactor capacity without compromising methane production. Copyright © 2016 Elsevier Ltd. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Presto, Albert A
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 PAmore » 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.« less
Toxic effects of butyl elastomers on aerobic methane oxidation
NASA Astrophysics Data System (ADS)
Niemann, Helge; Steinle, Lea I.; Blees, Jan H.; Krause, Stefan; Bussmann, Ingeborg; Lehmann, Moritz F.; Treude, Tina
2013-04-01
Large quantities of the potent greenhouse gas methane are liberated into the water column of marine and lacustrine environments where it may be consumed by aerobic methane oxidising bacteria before reaching the atmosphere.The reliable quantification of aerobic methane oxidation (MOx) rates is consequently of paramount importance for estimating methane budgets and to understand the controls on water column methane cycling. A widely used set of methods for measuring MOx rates is based on the incubation of water samples during which the consumption of methane is monitored, for instance with radio-tracer assays. Typically, incubation vessels are sealed with butyl rubber stoppers because these elastomers are essentially impermeable for gases at the relevant time scales. We tested the effect of different stopper materials (unmodified- and halogenated butyl rubber) on MOx activity in environmental samples and in cultures of methane oxidising bacteria. MOx rates in samples sealed with unmodified butyl rubber were > 75% lower compared to parallel incubations with halogenated butyl rubber seals, suggesting inhibiting/toxic effects associated with the use of unmodified butyl elastomers. To further explore the cause of these effects, we analysed aqueous extracts of the different stoppers. Halogenated butyl rubber stoppers appeared to bleed off comparably little amounts of organics. In stark contrast, extracts of unmodified butyl rubber were contaminated with various organic compounds including potential bactericides such as benzyltoluenes, phenylalkanes and benzuothiazoles. We also found tetramethylthiourea, a scavenger of active oxygen species, which may inhibit the MOx pathway.
Hanson, R S; Hanson, T E
1996-01-01
Methane-utilizing bacteria (methanotrophs) are a diverse group of gram-negative bacteria that are related to other members of the Proteobacteria. These bacteria are classified into three groups based on the pathways used for assimilation of formaldehyde, the major source of cell carbon, and other physiological and morphological features. The type I and type X methanotrophs are found within the gamma subdivision of the Proteobacteria and employ the ribulose monophosphate pathway for formaldehyde assimilation, whereas type II methanotrophs, which employ the serine pathway for formaldehyde assimilation, form a coherent cluster within the beta subdivision of the Proteobacteria. Methanotrophic bacteria are ubiquitous. The growth of type II bacteria appears to be favored in environments that contain relatively high levels of methane, low levels of dissolved oxygen, and limiting concentrations of combined nitrogen and/or copper. Type I methanotrophs appear to be dominant in environments in which methane is limiting and combined nitrogen and copper levels are relatively high. These bacteria serve as biofilters for the oxidation of methane produced in anaerobic environments, and when oxygen is present in soils, atmospheric methane is oxidized. Their activities in nature are greatly influenced by agricultural practices and other human activities. Recent evidence indicates that naturally occurring, uncultured methanotrophs represent new genera. Methanotrophs that are capable of oxidizing methane at atmospheric levels exhibit methane oxidation kinetics different from those of methanotrophs available in pure cultures. A limited number of methanotrophs have the genetic capacity to synthesize a soluble methane monooxygenase which catalyzes the rapid oxidation of environmental pollutants including trichloroethylene. PMID:8801441
Methane emission during municipal wastewater treatment.
Daelman, Matthijs R J; van Voorthuizen, Ellen M; van Dongen, Udo G J M; Volcke, Eveline I P; van Loosdrecht, Mark C M
2012-07-01
Municipal wastewater treatment plants emit methane. Since methane is a potent greenhouse gas that contributes to climate change, the abatement of the emission is necessary to achieve a more sustainable urban water management. This requires thorough knowledge of the amount of methane that is emitted from a plant, but also of the possible sources and sinks of methane on the plant. In this study, the methane emission from a full-scale municipal wastewater facility with sludge digestion was evaluated during one year. At this plant the contribution of methane emissions to the greenhouse gas footprint were slightly higher than the CO₂ emissions related to direct and indirect fossil fuel consumption for energy requirements. By setting up mass balances over the different unit processes, it could be established that three quarters of the total methane emission originated from the anaerobic digestion of primary and secondary sludge. This amount exceeded the carbon dioxide emission that was avoided by utilizing the biogas. About 80% of the methane entering the activated sludge reactor was biologically oxidized. This knowledge led to the identification of possible measures for the abatement of the methane emission. Copyright © 2012 Elsevier Ltd. All rights reserved.
Root-Associated Methane Oxidation and Methanogenesis: Key Determinants of Wetland Methane Emissions
NASA Technical Reports Server (NTRS)
King, G. M.
1997-01-01
During the award period, we have assessed the extent and controls of methane oxidation in north temperate wetlands. It is evident that wetlands have been a major global source of atmospheric methane in the past, and are so at present. It is also evident that microbial methane oxidation consumes a variable fraction of total wetland methane production, perhaps 10%-90%. Methane oxidation is thus a potentially important control of wetland methane emission. Our efforts have been designed to determine the extent of the process, its controls, and possible relationships to changes that might be expected in wetlands as a consequence of anthropogenic or climate-related disturbances. Current work, has emphasized controls of methane oxidation associated with rooted aquatic plants. As for the sediment-water interface, we have observed that oxygen availability is a primary limiting factor. Our conclusion is based on several different lines of evidence obtained from in vitro and in situ analyses. First, we have measured the kinetics of methane oxidation by intact plant roots harboring methane-oxidizing bacteria, as well as the kinetics of the methanotrophs themselves. Values for the half-saturation constant (apparent K(sub m)) are approximately 5 microns. These values are roughly equivalent to, or much less than porewater methane concentrations, indicating that uptake is likely saturated with respect to methane, and that some other parameter must limit activity. Methane concentrations in the lacunar spaces at the base of plant stems are also comparable to the half-saturation constants (when expressed as equivalent dissolved concentrations), providing further support for limitation of uptake by parameters other than methane.
Methane fluxes and inventories in the accretionary prism of southwestern Taiwan
NASA Astrophysics Data System (ADS)
Lin, L. H.; Chen, N. C.; Yang, T. F.; Hong, W. L.; Chen, H. W.; Chen, H. C.; Hu, C. Y.; Huang, Y. C.; Lin, S.; Su, C. C.; Liao, W. Z.; Sun, C. H.; Wang, P. L.; Yang, T.; Jiang, S. Y.; Liu, C. S.; Wang, Y.; Chung, S. H.
2017-12-01
Sediments distributed across marine and terrestrial realms represent the largest methane reservoir on Earth. The degassing of methane facilitated through either geological structures or perturbation would contribute significantly to global climatic fluctuation and elemental cycling. The exact fluxes and processes governing methane production, consumption and transport in a geological system remain largely unknown in part due to the limited coverage and access of samples. In this study, more than 200 sediment cores were collected from offshore and onshore southwestern Taiwan and analyzed for their gas and aqueous geochemistry. These data combined with published data and existing parameters of subduction system were used to calculate methane fluxes across different geochemical transitions and to develop scenarios of mass balance to constrain deep microbial and thermogenic methane production rates within the Taiwanese accretionary prism. The results showed that high methane fluxes tend to be associated with structural features, suggesting a strong structural control on methane transport. A significant portion of ascending methane (>50%) was consumed by anaerobic oxidation of methane at most sites. Gas compositions and isotopes revealed a transition from the predominance of microbial methane in the passive margin to thermogenic methane at the upper slope of the active margin and onshore mud volcanoes. Methane production and consumption at shallow depths were nearly offset with a small fraction of residual methane discharged into seawater or the atmosphere. The flux imbalance arose primarily from the deep microbial and thermogenic production and could be likely accounted for by the sequestration of methane into hydrate forms, and clay absorption.
Prospecting for Methane in Arabia Terra, Mars - First Results
NASA Technical Reports Server (NTRS)
Allen, Carlton C.; Oehler, Dotoyhy Z.; Venechuk, Elizabeth M.
2006-01-01
Methane has been measured in the Martian atmosphere at concentrations of approx. 10 ppb. Since the photochemical lifetime of this gas is approx. 300 years, it is likely that methane is currently being released from the surface. Possible sources for the methane include 1) hydrothermal activity, 2) serpentinization of basalts and other water-rock interactions, 3) thermal maturation of sedimentary organic matter, and 4) metabolism of living bacteria. Any such discovery would revolutionize our understanding of Mars. Longitudinal variations in methane concentration, as measured by the Planetary Fourier Spectrometer (PFS) on Mars Express, show the highest values over Arabia Terra, Elysium Planum, and Arcadia-Memnonia, suggesting localized areas of methane release. We are using orbital data and methodologies derived from petroleum exploration in an attempt to locate these release points.
De Vrieze, Jo; Christiaens, Marlies E R; Walraedt, Diego; Devooght, Arno; Ijaz, Umer Zeeshan; Boon, Nico
2017-03-15
Anaerobic digestion of high-salinity wastewaters often results in process inhibition due to the susceptibility of the methanogenic archaea. The ability of the microbial community to deal with increased salinity levels is of high importance to ensure process perseverance or recovery after failure. The exact strategy of the microbial community to ensure process endurance is, however, often unknown. In this study, we investigated how the microbial community is able to recover process performance following a disturbance through the application of high-salinity molasses wastewater. After a stable start-up, methane production quickly decreased from 625 ± 17 to 232 ± 35 mL CH 4 L -1 d -1 with a simultaneous accumulation in volatile fatty acids up to 20.5 ± 1.4 g COD L -1 , indicating severe process disturbance. A shift in feedstock from molasses wastewater to waste activated sludge resulted in complete process recovery. However, the bacterial and archaeal communities did not return to their original composition as before the disturbance, despite similar process conditions. Microbial community diversity was recovered to similar levels as before disturbance, which indicates that the metabolic potential of the community was maintained. A mild increase in ammonia concentration after process recovery did not influence methane production, indicating a well-balanced microbial community. Hence, given the change in community composition following recovery after salinity disturbance, it can be assumed that microbial community redundancy was the major strategy to ensure the continuation of methane production, without loss of functionality or metabolic flexibility. Copyright © 2017 The Authors. Published by Elsevier Ltd.. All rights reserved.
Understanding trends in C-H bond activation in heterogeneous catalysis.
Latimer, Allegra A; Kulkarni, Ambarish R; Aljama, Hassan; Montoya, Joseph H; Yoo, Jong Suk; Tsai, Charlie; Abild-Pedersen, Frank; Studt, Felix; Nørskov, Jens K
2017-02-01
While the search for catalysts capable of directly converting methane to higher value commodity chemicals and liquid fuels has been active for over a century, a viable industrial process for selective methane activation has yet to be developed. Electronic structure calculations are playing an increasingly relevant role in this search, but large-scale materials screening efforts are hindered by computationally expensive transition state barrier calculations. The purpose of the present letter is twofold. First, we show that, for the wide range of catalysts that proceed via a radical intermediate, a unifying framework for predicting C-H activation barriers using a single universal descriptor can be established. Second, we combine this scaling approach with a thermodynamic analysis of active site formation to provide a map of methane activation rates. Our model successfully rationalizes the available empirical data and lays the foundation for future catalyst design strategies that transcend different catalyst classes.
Understanding trends in C–H bond activation in heterogeneous catalysis
Latimer, Allegra A.; Kulkarni, Ambarish R.; Aljama, Hassan; ...
2016-10-10
While the search for catalysts capable of directly converting methane to higher value commodity chemicals and liquid fuels has been active for over a century, a viable industrial process for selective methane activation has yet to be developed1. Electronic structure calculations are playing an increasingly relevant role in this search, but large-scale materials screening efforts are hindered by computationally expensive transition state barrier calculations. The purpose of the present letter is twofold. First, we show that, for the wide range of catalysts that proceed via a radical intermediate, a unifying framework for predicting C–H activation barriers using a single universalmore » descriptor can be established. Second, we combine this scaling approach with a thermodynamic analysis of active site formation to provide a map of methane activation rates. Lastly, our model successfully rationalizes the available empirical data and lays the foundation for future catalyst design strategies that transcend different catalyst classes.« less
Understanding trends in C-H bond activation in heterogeneous catalysis
NASA Astrophysics Data System (ADS)
Latimer, Allegra A.; Kulkarni, Ambarish R.; Aljama, Hassan; Montoya, Joseph H.; Yoo, Jong Suk; Tsai, Charlie; Abild-Pedersen, Frank; Studt, Felix; Nørskov, Jens K.
2017-02-01
While the search for catalysts capable of directly converting methane to higher value commodity chemicals and liquid fuels has been active for over a century, a viable industrial process for selective methane activation has yet to be developed. Electronic structure calculations are playing an increasingly relevant role in this search, but large-scale materials screening efforts are hindered by computationally expensive transition state barrier calculations. The purpose of the present letter is twofold. First, we show that, for the wide range of catalysts that proceed via a radical intermediate, a unifying framework for predicting C-H activation barriers using a single universal descriptor can be established. Second, we combine this scaling approach with a thermodynamic analysis of active site formation to provide a map of methane activation rates. Our model successfully rationalizes the available empirical data and lays the foundation for future catalyst design strategies that transcend different catalyst classes.
Li, Xiaolan; Xu, Xueqin; Huang, Shansong; Zhou, Yun; Jia, Haijiang
2017-10-01
Methane production from waste activated sludge (WAS) anaerobic digestion is always low due to slow hydrolysis rate and inappropriate ratio of carbon to nitrogen (C/N). In this work, a novel approach, i.e., co-digestion of WAS and tobacco waste (TW) using ozone pretreatment, to greatly enhance the production of methane is reported. Experimental results showed the optimal C/N and ozone dosage for methane production was 24:1 and 90 mg/g suspended solids, and the corresponding methane production was 203.6 mL/g volatile suspended solids, which was 1.3-fold that in mono-WAS digestion. Further investigation showed the co-digestion of WAS and TW was beneficial to the consumptions of protein and cellulose; also, the presence of ozone enhanced the disruption of organic substrates and production of short chain fatty acids, which provided sufficient digestion substrates for methane generation. Analysis of microbial community structure suggested that members of the phyla Bacteroidetes and Firmicutes were the dominant species when ozone pretreatment was applied. The findings obtained in this work might be of great importance for the treatment of WAS and TW.
Isotopic constraints on methane's global sources and ENSO-dependence
NASA Astrophysics Data System (ADS)
Schaefer, Hinrich; Mikaloff Fletcher, Sara; Veidt, Cora; Lassey, Keith; Brailsford, Gordon; Bromley, Tony; Dlugokencky, Ed; Englund Michel, Sylvia; Miller, John; Levin, Ingeborg; Lowe, Dave; Martin, Ross; Vaughn, Bruce; White, James; Nichol, Sylvia
2017-04-01
Atmospheric levels of the potent greenhouse gas methane (CH4) have been rising since the industrial revolution, except for a plateau during the early 2000s. Stable carbon isotopes in methane (delta-13CH4) provide constraints on the budget changes associated with the plateau's onset and its end. We present a reconstruction of annual global delta-13CH4 averages based on a global network of stations, whose trends are indicative of global methane source and sink activity. A box model analysis shows that from the mid-1990s methane emissions with the characteristic thermogenic delta-13CH4 signature reduced, implying persistently lower emissions from fossil fuel productions as the cause of the plateau. However, variations in hydroxyl, the main CH4 sink, provide an equably plausible explanation for the plateau onset that may also account for strong variability in emission-vs-removal rates during the plateau period. In contrast, the renewed CH4 rise since 2006 can only be explained by increasing emissions with a biogenic isotope signature, i.e. agriculture or wetlands. We present correlation studies that test whether ENSO activity controls atmospheric delta-13CH4, and by extension methane levels, through tropical wetland emissions.
Transition metal sulfide loaded catalyst
Maroni, V.A.; Iton, L.E.; Pasterczyk, J.W.; Winterer, M.; Krause, T.R.
1994-04-26
A zeolite-based catalyst is described for activation and conversion of methane. A zeolite support includes a transition metal (Mo, Cr or W) sulfide disposed within the micropores of the zeolite. The catalyst allows activation and conversion of methane to C[sub 2]+ hydrocarbons in a reducing atmosphere, thereby avoiding formation of oxides of carbon.
Controls on tree species stem transport and emission of methane from tropical peatlands
NASA Astrophysics Data System (ADS)
Van Haren, J. L. M.; Cadillo-Quiroz, H.
2016-12-01
Methane emissions from wetlands dominate the global budget and are most likely responsible for the annual variability in emissions. Methane is produced and consumed by microbial activity and then transported to the atmosphere. Plants have been shown to facilitate the transport of methane to significant amounts, but broad surveys across multiple sites have been lacking. We present data collected from multiple peatland and wetland sites south of Iquitos Peru and varzea sites from Santarem Brazil and compare our results to the limited literature of tree stem fluxes. The survey suggests that methane stem emissions might be conserved at the genera level, but not the family level. Large emitters exist in the Aracaceae, Euphorbiaceae, and Sapotaceae, however, other genera within the same families do not emit any methane. Certain genera are consistent pan-tropical methane emitters. The methane emission from the stems decreases generally with height, suggesting a diffusion constrained stem flux. Further constraints on the methane emissions from tree stems involve soil methane concentration and wood density, which is likely an indicator for stem conductivity. Diurnal cycles, flooding level and tree leaves appear to have less of an influence on the tree methane emissions though flooding can lead to a translocation of emissions up the stem to above the flooding level. Methane emissions and the plant transport pathways appear to be constrained at the genera level within wetlands.
Marlow, Jeffrey J; Kumar, Amit; Enalls, Brandon C; Reynard, Linda M; Tuross, Noreen; Stephanopoulos, Gregory; Girguis, Peter
2018-06-01
Harnessing the metabolic potential of uncultured microbial communities is a compelling opportunity for the biotechnology industry, an approach that would vastly expand the portfolio of usable feedstocks. Methane is particularly promising because it is abundant and energy-rich, yet the most efficient methane-activating metabolic pathways involve mixed communities of anaerobic methanotrophic archaea and sulfate reducing bacteria. These communities oxidize methane at high catabolic efficiency and produce chemically reduced by-products at a comparable rate and in near-stoichiometric proportion to methane consumption. These reduced compounds can be used for feedstock and downstream chemical production, and at the production rates observed in situ they are an appealing, cost-effective prospect. Notably, the microbial constituents responsible for this bioconversion are most prominent in select deep-sea sediments, and while they can be kept active at surface pressures, they have not yet been cultured in the lab. In an industrial capacity, deep-sea sediments could be periodically recovered and replenished, but the associated technical challenges and substantial costs make this an untenable approach for full-scale operations. In this study, we present a novel method for incorporating methanotrophic communities into bioindustrial processes through abstraction onto low mass, easily transportable carbon cloth artificial substrates. Using Gulf of Mexico methane seep sediment as inoculum, optimal physicochemical parameters were established for methane-oxidizing, sulfide-generating mesocosm incubations. Metabolic activity required >∼40% seawater salinity, peaking at 100% salinity and 35 °C. Microbial communities were successfully transferred to a carbon cloth substrate, and rates of methane-dependent sulfide production increased more than threefold per unit volume. Phylogenetic analyses indicated that carbon cloth-based communities were substantially streamlined and were dominated by Desulfotomaculum geothermicum. Fluorescence in situ hybridization microscopy with carbon cloth fibers revealed a novel spatial arrangement of anaerobic methanotrophs and sulfate reducing bacteria suggestive of an electronic coupling enabled by the artificial substrate. This system: 1) enables a more targeted manipulation of methane-activating microbial communities using a low-mass and sediment-free substrate; 2) holds promise for the simultaneous consumption of a strong greenhouse gas and the generation of usable downstream products; and 3) furthers the broader adoption of uncultured, mixed microbial communities for biotechnological use. © 2018 The Authors. Biotechnology and Bioengineering Published by Wiley Periodicals Inc.
Methane from shallow seep areas of the NW Svalbard Arctic margin does not reach the sea surface
NASA Astrophysics Data System (ADS)
Silyakova, Anna; Greinert, Jens; Jansson, Pär; Ferré, Bénédicte
2015-04-01
Methane, an important greenhouse gas, leaks from large areas of the Arctic Ocean floor. One overall question is how much methane passes from the seabed through the water column, potentially reaching the atmosphere. Transport of methane from the ocean floor into and through the water column depends on many factors such as distribution of gas seeps, microbial methane oxidation, and ambient oceanographic conditions, which may trigger a change in seep activity. From June-July 2014 we investigated dissolved methane in the water column emanating from the "Prins Karls Forland seeps" area offshore the NW Svalbard Arctic margin. Measurements of the spatial variability of dissolved methane in the water column included 65 CTD stations located in a grid covering an area of 30 by 15 km. We repeated an oceanographic transect twice in a week for time lapse studies, thus documenting significant temporal variability in dissolved methane above one shallow seep site (~100 m water depth). Analysis of both nutrient concentrations and dissolved methane in water samples from the same transect, reveal striking similarities in spatial patterns of both dissolved methane and nutrients indicating that microbial community is involved in methane cycling above the gas seepage. Our preliminary results suggest that although methane release can increase in a week's time, providing twice as much dissolved gas to the water column, no methane from a seep reaches the sea surface. Instead it spreads horizontally under the pycnocline. Yet microbial communities react rapidly to the methane supply above gas seepage areas and may also have an important role as an effective filter, hindering methane release from the ocean to the atmosphere during rapid methane ebullition. This study is funded by CAGE (Centre for Arctic Gas Hydrate, Environment and Climate), Norwegian Research Council grant no. 223259.
30 CFR 22.4 - Application procedures and requirements.
Code of Federal Regulations, 2010 CFR
2010-07-01
..., EVALUATION, AND APPROVAL OF MINING PRODUCTS PORTABLE METHANE DETECTORS § 22.4 Application procedures and requirements. (a) Before MSHA will undertake an active investigation leading to approval of any methane...
Generation of methane from paddy fields and cattle in India, and its reduction at source
NASA Astrophysics Data System (ADS)
Bandyopadhyay, T. K.; Goyal, P.; Singh, M. P.
Methane (CH4) is a saturated organic gas. About 500 Tg yr -1 methane is generated globally. It is evident that 70% of the total emission have anthropogenic sources. The paddy fields contribute a significant portion of the total methane generated. About 20% of the total methane is generated from the paddy fields. In India, methane efflux rate is negative to 49 mg m -2 hr -1. The mean CH4 flux from Indian paddy fields is calculated to be 4.0 Tgyr -1. Livestock, and in particular ruminants are one of the important sources of methane emission on a global scale. There are two sources of methane emission from live stock: (1) from digestive process of ruminants, (2) from animal wastes. The estimated value of methane emission from digestive process of ruminants in India accounts for 6.47 Tgyr -1, and animal wastes accounts for 1.60 Tgyr -1. Total generation of methane from animals in India is about 8.0 Tg yr -1 . In paddy fields the key of controlling methane emission lies in the control of irrigation water. The methane emission can be decreased drastically if the field is under dry conditions for a few days at the end of tillering. In the case of livestock, reduction of methane emission can be done by (1) increasing the intake of the animal, (2) modifying the composition of the diet, (3) eliminating protozoa in rumen, (4) improving fibre digestion efficiency and (5) inhibiting activity of methanogenic bacteria.
Deep-biosphere methane production stimulated by geofluids in the Nankai accretionary complex
Kubo, Yusuke; Hoshino, Tatsuhiko; Sakai, Sanae; Arnold, Gail L.; Case, David H.; Lever, Mark A.; Morita, Sumito; Nakamura, Ko-ichi
2018-01-01
Microbial life inhabiting subseafloor sediments plays an important role in Earth’s carbon cycle. However, the impact of geodynamic processes on the distributions and carbon-cycling activities of subseafloor life remains poorly constrained. We explore a submarine mud volcano of the Nankai accretionary complex by drilling down to 200 m below the summit. Stable isotopic compositions of water and carbon compounds, including clumped methane isotopologues, suggest that ~90% of methane is microbially produced at 16° to 30°C and 300 to 900 m below seafloor, corresponding to the basin bottom, where fluids in the accretionary prism are supplied via megasplay faults. Radiotracer experiments showed that relatively small microbial populations in deep mud volcano sediments (102 to 103 cells cm−3) include highly active hydrogenotrophic methanogens and acetogens. Our findings indicate that subduction-associated fluid migration has stimulated microbial activity in the mud reservoir and that mud volcanoes may contribute more substantially to the methane budget than previously estimated. PMID:29928689
2016-01-01
The direct catalytic conversion of methane to liquid oxygenated compounds, such as methanol or dimethyl ether, at low temperature using molecular oxygen is a grand challenge in C–H activation that has never been met with synthetic, heterogeneous catalysts. We report the first demonstration of direct, catalytic oxidation of methane into methanol with molecular oxygen over copper-exchanged zeolites at low reaction temperatures (483–498 K). Reaction kinetics studies show sustained catalytic activity and high selectivity for a variety of commercially available zeolite topologies under mild conditions (e.g., 483 K and atmospheric pressure). Transient and steady state measurements with isotopically labeled molecules confirm catalytic turnover. The catalytic rates and apparent activation energies are affected by the zeolite topology, with caged-based zeolites (e.g., Cu-SSZ-13) showing the highest rates. Although the reaction rates are low, the discovery of catalytic sites in copper-exchanged zeolites will accelerate the development of strategies to directly oxidize methane into methanol under mild conditions. PMID:27413787
Nguyen, Minh Tuan; Mohd Yasin, Nazlina Haiza; Miyazaki, Toshiki; Maeda, Toshinari
2014-12-01
The management of waste activated sludge (WAS) recycling is a concern that affects the development of the future low-carbon society, particularly sludge reduction and biomass utilization. In this study, we investigated the effect of removing extracellular polymeric substances (EPS), which play important roles in the adhesion and flocculation of WAS, on increased sludge disintegration, thereby enhancing sludge reduction and methane production by anaerobic digestion. EPS removal from WAS by ethylenediaminetetraacetic acid (EDTA) significantly enhanced sludge reduction, i.e., 49 ± 5% compared with 27 ± 1% of the control at the end the digestion process. Methane production was also improved in WAS without EPS by 8881 ± 109 CH4 μmol g(-1) dry-weight of sludge. Microbial activity was determined by denaturing gradient gel electrophoresis and real-time polymerase chain reaction, which showed that the hydrolysis and acetogenesis stages were enhanced by pretreatment with 2% EDTA, with a larger methanogenic community and better methane production. Copyright © 2014 Elsevier Ltd. All rights reserved.
Tracking Dissolved Methane Concentrations near Active Seeps and Gas Hydrates: Sea of Japan.
NASA Astrophysics Data System (ADS)
Snyder, G. T.; Aoki, S.; Matsumoto, R.; Tomaru, H.; Owari, S.; Nakajima, R.; Doolittle, D. F.; Brant, B.
2015-12-01
A number of regions in the Sea of Japan are known for active gas venting and for gas hydrate exposures on the sea floor. In this investigation we employed several gas sensors mounted on a ROV in order to determine the concentrations of dissolved methane in the water near these sites. Methane concentrations were determined during two-second intervals throughout each ROV deployment during the cruise. The methane sensor deployments were coupled with seawater sampling using Niskin bottles. Dissolved gas concentrations were later measured using gas chromatography in order to compare with the sensor results taken at the same time. The observed maximum dissolved methane concentrations were much lower than saturation values, even when the ROV manipulators were in contact with gas hydrate. Nonetheless, dissolved concentrations did reach several thousands of nmol/L near gas hydrate exposures and gas bubbles, more than two orders of magnitude over the instrumental detection limits. Most of the sensors tested were able to detect dissolved methane concentrations as low as 10 nmol/L which permitted detection when the ROV approached methane plume sites, even from several tens of meters above the sea floor. Despite the low detection limits, the methane sensors showed variable response times when returning to low-background seawater (~5nM). For some of the sensors, the response time necessary to return to background values occurred in a matter of minutes, while for others it took several hours. Response time, as well as detection limit, should be an important consideration when selecting methane sensors for ROV or AUV investigations. This research was made possible, in part, through funding provided by the Japanese Ministry of Economy, Trade and Industry (METI).
DOE Office of Scientific and Technical Information (OSTI.GOV)
Rodriguez, Jose A.; Liu, Zongyuan; Lustemberg, Pablo
Studies with a series of M-CeO 2(111) {M= Co, Ni, Cu} surfaces indicate that metal-oxide interactions can play a very important role for the activation of methane and its reforming with CO 2 at relatively low temperatures (600-700 K). Among the systems examined, Co-CeO 2(111) exhibits the best performance and Cu-CeO 2(111) has negligible activity. Experiments using ambient pressure XPS indicate that methane dissociates on Co-CeO2(111), at temperatures as low as 300 K, generating CH x and CO x species on the catalyst surface. The results of density-functional calculations show a reduction in the methane activation barrier from 1.07 eVmore » on Co(0001) to 0.87 eV on Co 2+/CeO 2(111), and to only 0.05 eV on Co 0/CeO 2-x(111). At 700 K, under methane dry reforming conditions, CO 2 dissociates on the oxide surface and a catalytic cycle is established without coke deposition. In conclusion, a significant part of the CH x formed on the Co 0/CeO 2-x (111) catalyst recombines to yield ethane or ethylene.« less
Rodriguez, Jose A.; Liu, Zongyuan; Lustemberg, Pablo; ...
2017-08-16
Studies with a series of M-CeO 2(111) {M= Co, Ni, Cu} surfaces indicate that metal-oxide interactions can play a very important role for the activation of methane and its reforming with CO 2 at relatively low temperatures (600-700 K). Among the systems examined, Co-CeO 2(111) exhibits the best performance and Cu-CeO 2(111) has negligible activity. Experiments using ambient pressure XPS indicate that methane dissociates on Co-CeO2(111), at temperatures as low as 300 K, generating CH x and CO x species on the catalyst surface. The results of density-functional calculations show a reduction in the methane activation barrier from 1.07 eVmore » on Co(0001) to 0.87 eV on Co 2+/CeO 2(111), and to only 0.05 eV on Co 0/CeO 2-x(111). At 700 K, under methane dry reforming conditions, CO 2 dissociates on the oxide surface and a catalytic cycle is established without coke deposition. In conclusion, a significant part of the CH x formed on the Co 0/CeO 2-x (111) catalyst recombines to yield ethane or ethylene.« less
Evaluation of the effects of low energetic microwave irradiation on anaerobic digestion.
Bastiaens, Bert; Van den Broeck, Rob; Appels, Lise; Dewil, Raf
2017-11-01
The present study investigates the effects of microwave irradiation on the performance of anaerobic digestion processes. A first set of experiments is performed to distinguish the upper limit of the applied energy levels. Secondly, the effects of these treatments on the performance of the digestion process are evaluated in 3 experimental setups: (i) monitoring the acetic acid degradation, (ii) performing a biological methane potential (BMP) assay and (iii) conducting a specific methanogenic activity (SMA) test. The solubilisation experiment reveals a limited degree of disintegration of anaerobic biomass up to a microwave treatment of 10000 kJ/kg TS. Above this threshold value the soluble COD level started to rise, with up to 350% at 30000 kJ/kg TS regardless of the microwave output power. Because solubilisation of the biomass increases the easily degradable content, this would lead to false observations regarding increased activity. Therefore, solubilisation is minimized by limiting the microwave treatment to a maximum of 6000 kJ/kg TS during the second part of the experiments. Monitoring the degradation of acetic acid after a low intensity microwave treatment, reveals that microwave irradiation shortens the lag phase, e.g., from 21 to 3 h after a microwave treatment of 1000 kJ/kg TS at 100 W. However most treatments also result in a decrease of the maximum degradation and of the degradation rate of acetic acid. BMP assays are performed to evaluate the activity and performance of the entire anaerobic community. Every treatment results in a decreased biogas production potential and decreased biogas production rate. Moreover, each treatment induced an increase of the lag phase. The SMA experiments show no influence of the microwave irradiation in terms of biogas or methane production. Copyright © 2017 Elsevier Ltd. All rights reserved.
Light-induced diurnal pattern of methane exchange in a boreal forest
NASA Astrophysics Data System (ADS)
Sundqvist, Elin; Crill, Patrick; Mölder, Meelis; Vestin, Patrik; Lindroth, Anders
2013-04-01
Boreal forests represents one third of the Earth's forested land surface area and is a net sink of methane and an important component of the atmospheric methane budget. Methane is oxidized in well-aerated forest soils whereas ponds and bog soils are sources of methane. Besides the microbial processes in the soil also forest vegetation might contribute to methane exchange. Due to a recent finding of methane consumption by boreal plants that correlated with photosynthetic active radiation (PAR), we investigate the impact of PAR on soil methane exchange at vegetated plots on the forest floor. The study site, Norunda in central Sweden, is a 120 years old boreal forest stand, dominated by Scots pine and Norway spruce. We used continuous chamber measurements in combination with a high precision laser gas analyzer (Los Gatos Research), to measure the methane exchange at four different plots in July-November 2009, and April-June 2010. The ground vegetation consisted almost entirely of mosses and blueberry-shrubs. Two of the plots acted as stable sinks of methane whereas the other two plots shifted from sinks to sources during very wet periods. The preliminary results show a clear diurnal pattern of the methane exchange during the growing season, which cannot be explained by temperature. The highest consumption occurs at high PAR levels. The amplitude of the diurnal methane exchange during the growing season is in the order of 10 μmol m-2 h-1. This indicates that besides methane oxidation by methanotrophs in the soil there is an additional removal of methane at soil level by a process related to ground vegetation.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Nix, Andrew; Johnson, Derek; Heltzel, Robert
Researchers at the Center for Alternative Fuels, Engines, and Emissions (CAFEE) completed a multi-year program under DE-FE0013689 entitled, “Assessing Fugitive Methane Emissions Impact Using Natural Gas Engines in Unconventional Resource Development.” When drilling activity was high and industry sought to lower operating costs and reduce emissions they began investing in dual fuel and dedicated natural gas engines to power unconventional well equipment. From a review of literature we determined that the prime-movers (or major fuel consumers) of unconventional well development were the service trucks (trucking), horizontal drilling rig (drilling) engines, and hydraulic stimulation pump (fracturing) engines. Based on early findingsmore » from on-road studies we assessed that conversion of prime movers to operate on natural gas could contribute to methane emissions associated with unconventional wells. As such, we collected significant in-use activity data from service trucks and in-use activity, fuel consumption, and gaseous emissions data from drilling and fracturing engines. Our findings confirmed that conversion of the prime movers to operate as dual fuel or dedicated natural gas – created an additional source of methane emissions. While some gaseous emissions were decreased from implementation of these technologies – methane and CO 2 equivalent emissions tended to increase, especially for non-road engines. The increases were highest for dual fuel engines due to methane slip from the exhaust and engine crankcase. Dedicated natural gas engines tended to have lower exhaust methane emissions but higher CO 2 emissions due to lower efficiency. Therefore, investing in currently available natural gas technologies for prime movers will increase the greenhouse gas footprint of the unconventional well development industry.« less
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.
Choi, Kwang-Soon; Kondaveeti, Sanath; Min, Booki
2017-12-01
Microbial electrolysis cells (MECs) at various cell voltages (0.5, 0.7 1.0 and 1.5V) were operated in anaerobic fermentation. During the start-up period, the cathode potential decreased from -0.63 to -1.01V, and CH 4 generation increased from 168 to 199ml. At an applied voltage of 1.0V, the highest methane yields of 408.3ml CH 4 /g COD glucose was obtained, which was 30.3% higher than in the control tests (313.4ml CH 4 /g COD glucose). The average current of 5.1mA was generated at 1.0V at which the maximum methane yield was obtained. The other average currents were 1.42, 3.02, 0.53mA at 0.5, 0.7, and 1.5V, respectively. Cyclic voltammetry and EIS analysis revealed that enhanced reduction currents were present at all cell voltages with biocatalyzed cathode electrodes (no reduction without biofilm), and the highest value was obtained with 1V external voltage. Copyright © 2017 Elsevier Ltd. All rights reserved.
Cashman, Sarah; Ma, Xin; Mosley, Janet; Garland, Jay; Crone, Brian; Xue, Xiaobo
2018-04-01
This study calculated the energy and greenhouse gas life cycle and cost profiles of transitional aerobic membrane bioreactors (AeMBR) and anaerobic membrane bioreactors (AnMBR). Membrane bioreactors (MBR) represent a promising technology for decentralized wastewater treatment and can produce recycled water to displace potable water. Energy recovery is possible with methane generated from AnMBRs. Scenarios for these technologies were investigated for different scale systems serving various population densities under a number of climate conditions with multiple methane recovery options. When incorporating the displacement of drinking water, AeMBRs started to realize net energy benefits at the 1 million gallons per day (MGD) scale and mesophilic AnMBRs at the 5 MGD scale. For all scales, the psychrophilic AnMBR resulted in net energy benefits. This study provides insights into key performance characteristics needed before an informed decision can be made for a community to transition towards the adoption of MBR technologies. Copyright © 2018. Published by Elsevier Ltd.
Dong, Ming; Gonzalez, Tara D; Klems, Meghan M; Steinberg, Lisa M; Chen, Wilfred; Papoutsakis, Eleftherios T; Bahnson, Brian J
2017-09-01
Methanol:coenzyme M methyltransferase is an enzyme complex composed of three subunits, MtaA, MtaB, and MtaC, found in methanogenic archaea and is needed for their growth on methanol ultimately producing methane. MtaABC catalyzes the energetically favorable methyl transfer from methanol to coenzyme M to form methyl coenzyme M. Here we demonstrate that this important reaction for possible production of methanol from the anaerobic oxidation of methane can be reversed in vitro. To this effect, we have expressed and purified the Methanosarcina barkeri MtaABC enzyme, and developed an in vitro functional assay that demonstrates MtaABC can catalyze the energetically unfavorable (ΔG° = 27 kJ/mol) reverse reaction starting from methyl coenzyme M and generating methanol as a product. Demonstration of an in vitro ability of MtaABC to produce methanol may ultimately enable the anaerobic oxidation of methane to produce methanol and from methanol alternative fuel or fuel-precursor molecules. © 2017 American Institute of Chemical Engineers Biotechnol. Prog., 33:1243-1249, 2017. © 2017 American Institute of Chemical Engineers.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Okolie, Chukwuemeka; Belhseine, Yasmeen F.; Lyu, Yimeng
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 acidicmore » NiO clusters and the redox-active CZ support, which also stabilizes the small NiO clusters.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Okolie, Chukwuemeka; Belhseine, Yasmeen F.; Lyu, Yimeng
Here, the conversion of methane into alcohols under moderate reaction conditions 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 convert methane to methanol and ethanol in a single, steady-state process at 723 K using O 2 as an abundantly available oxidant. The presence of steam is required to obtain alcohols rather than CO 2 as the product of catalytic combustion. The unusual activity of this catalyst is attributed to themore » synergy between the small Lewis acidic NiO clusters and the redox-active CZ support, which also stabilizes the small NiO clusters.« less
Okolie, Chukwuemeka; Belhseine, Yasmeen F.; Lyu, Yimeng; ...
2017-08-08
Here, the conversion of methane into alcohols under moderate reaction conditions 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 convert methane to methanol and ethanol in a single, steady-state process at 723 K using O 2 as an abundantly available oxidant. The presence of steam is required to obtain alcohols rather than CO 2 as the product of catalytic combustion. The unusual activity of this catalyst is attributed to themore » synergy between the small Lewis acidic NiO clusters and the redox-active CZ support, which also stabilizes the small NiO clusters.« less
ELECTROCHEMISTRY AND ON-CELL REFORMATION MODELING FOR SOLID OXIDE FUEL CELL STACKS
DOE Office of Scientific and Technical Information (OSTI.GOV)
Recknagle, Kurtis P.; Jarboe, Daniel T.; Johnson, Kenneth I.
2007-01-16
ABSTRACT Providing adequate and efficient cooling schemes for solid-oxide-fuel-cell (SOFC) stacks continues to be a challenge coincident with the development of larger, more powerful stacks. The endothermic steam-methane reformation reaction can provide cooling and improved system efficiency when performed directly on the electrochemically active anode. Rapid kinetics of the endothermic reaction typically causes a localized temperature depression on the anode near the fuel inlet. It is desirable to extend the endothermic effect over more of the cell area and mitigate the associated differences in temperature on the cell to alleviate subsequent thermal stresses. In this study, modeling tools validated formore » the prediction of fuel use, on-cell methane reforming, and the distribution of temperature within SOFC stacks, are employed to provide direction for modifying the catalytic activity of anode materials to control the methane conversion rate. Improvements in thermal management that can be achieved through on-cell reforming is predicted and discussed. Two operating scenarios are considered: one in which the methane fuel is fully pre-reformed, and another in which a substantial percentage of the methane is reformed on-cell. For the latter, a range of catalytic activity is considered and the predicted thermal effects on the cell are presented. Simulations of the cell electrochemical and thermal performance with and without on-cell reforming, including structural analyses, show a substantial decrease in thermal stresses for an on-cell reforming case with slowed methane conversion.« less
Wang, Ruobing; Sun, Qinglei; Xia, Fangzhou; Chen, Zeli; Wu, Jiangchun; Zhang, Yuelu; Xu, Jiajun; Liu, Lin
2017-06-01
Secondary degeneration is a common event in traumatic central nervous system disorders, which involves neuronal apoptosis and mitochondrial dysfunction. Exogenous methane exerts the therapeutic effects in many organ injury. Our study aims to investigate the potential neuroprotection of methane in a rat model of optic nerve crush (ONC). Adult male Sprague-Dawley rats were subjected to ONC and administrated intraperitoneally with methane-saturated or normal saline (10 ml/kg) once per day for one week after ONC. The retinal ganglion cells (RGCs) density was assessed by hematoxylin and eosin staining and Fluoro-Gold retrogradely labeling. Visual function was evaluated by flash visual evoked potentials (FVEP). The retinal apoptosis was measured by terminal-deoxy-transferase-mediated dUTP nick end labeling (TUNEL) assay and the expression of apoptosis-related factors, such as phosphorylated Bcl-2-associated death promoter (pBAD), phosphorylated glycogen synthase kinase-3β (pGSK-3β), Bcl-2 associated X protein (Bax) and Bcl-2 extra large (Bcl-xL). Retinal mitochondrial function was assessed by the mRNA expressions of peroxisome proliferator-activated receptor gamma coactivator-1α (PGC-1α), nuclear respiratory factor 1 (NRF1) and mitochondrial transcription factor A (TFAM), the mitochondrial DNA (mtDNA) copy number, citrate synthase activity and ATP content. Methane treatment significantly improved the RGC loss and visual dysfunction following ONC. As expected, methane also remarkably inhibited the retinal neural apoptosis, such as the fewer TUNEL-positive cells in ganglion cell layer, accompanied by the up-regulations of anti-apoptotic factors (pGSK-3β, pBAD, Bcl-xL) and the down-regulation of pro-apoptotic factor (Bax). Furthermore, methane treatment suppressed up-regulations of critical mitochondrial components (PGC-1α, NRF1 and TFAM) mRNA and mtDNA copy number, as well as improved the reduction of functional mitochondria markers, including citrate synthase activity and ATP content, in retinas with ONC. Taken together, methane treatment promotes RGC survival and limits retinal mitochondrial dysfunction against ONC insult. Methane can be a potential neuroprotective agent for traumatic and glaucomatous neurodegeneration. Copyright © 2017. Published by Elsevier Ltd.
NASA Astrophysics Data System (ADS)
Douglas, P. M.; Stolper, D. A.; Eiler, J. M.; Sessions, A. L.; Walter Anthony, K. M.
2014-12-01
Natural methane emissions from the Arctic present an important potential feedback to global warming. Arctic methane emissions may come from either active microbial sources or from deep fossil reservoirs released by the thawing of permafrost and melting of glaciers. It is often difficult to distinguish between and quantify contributions from these methane sources based on stable isotope data. Analyses of methane clumped isotopes (isotopologues with two or more rare isotopes such as 13CH3D) can complement traditional stable isotope-based classifications of methane sources. This is because clumped isotope abundances (for isotopically equilibrated systems) are a function of temperature and can be used to identify pathways of methane generation. Additionally, distinctive effects of mixing on clumped isotope abundances make this analysis valuable for determining the origins of mixed gasses. We find large variability in clumped isotope compositions of methane from seeps in several lakes, including thermokarst lakes, across Alaska. At Lake Sukok in northern Alaska we observe the emission of dominantly thermogenic methane, with a formation temperature of at least 100° C. At several other lakes we find evidence for mixing between thermogenic methane and biogenic methane that forms in low-temperature isotopic equilibrium. For example, at Eyak Lake in southeastern Alaska, analysis of three methane samples results in a distinctive isotopic mixing line between a high-temperature end-member that formed between 100-170° C, and a biogenic end-member that formed in isotopic equilibrium between 0-20° C. In this respect, biogenic methane in these lakes resembles observations from marine gas seeps, oil degradation, and sub-surface aquifers. Interestingly, at Goldstream Lake in interior Alaska, methane with strongly depleted clumped-isotope abundances, indicative of disequilibrium gas formation, is found, similar to observations from methanogen culture experiments.
Reducing Open Cell Landfill Methane Emissions with a Bioactive Alternative Daily
DOE Office of Scientific and Technical Information (OSTI.GOV)
Helene Hilger; James Oliver; Jean Bogner
2009-03-31
Methane and carbon dioxide are formed in landfills as wastes degrade. Molecule-for-molecule, methane is about 20 times more potent than carbon dioxide at trapping heat in the earth's atmosphere, and thus, it is the methane emissions from landfills that are scrutinized. For example, if emissions composed of 60% methane and 40% carbon dioxide were changed to a mix that was 40% methane and 60% carbon dioxide, a 30% reduction in the landfill's global warming potential would result. A 10% methane, 90% carbon dioxide ratio will result in a 75% reduction in global warming potential compared to the baseline. Gas collectionmore » from a closed landfill can reduce emissions, and it is sometimes combined with a biocover, an engineered system where methane oxidizing bacteria living in a medium such as compost, convert landfill methane to carbon dioxide and water. Although methane oxidizing bacteria merely convert one greenhouse gas (methane) to another (carbon dioxide), this conversion can offer significant reductions in the overall greenhouse gas contribution, or global warming potential, associated with the landfill. What has not been addressed to date is the fact that methane can also escape from a landfill when the active cell is being filled with waste. Federal regulations require that newly deposited solid waste to be covered daily with a 6 in layer of soil or an alternative daily cover (ADC), such as a canvas tarp. The aim of this study was to assess the feasibility of immobilizing methane oxidizing bacteria into a tarp-like matrix that could be used for alternative daily cover at open landfill cells to prevent methane emissions. A unique method of isolating methanotrophs from landfill cover soil was used to create a liquid culture of mixed methanotrophs. A variety of prospective immobilization techniques were used to affix the bacteria in a tarp-like matrix. Both gel encapsulation of methanotrophs and gels with liquid cores containing methanotrophs were readily made but prone to rapid desiccation. Bacterial adsorption onto foam padding, natural sponge, and geotextile was successful. The most important factor for success appeared to be water holding capacity. Prototype biotarps made with geotextiles plus adsorbed methane oxidizing bacteria were tested for their responses to temperature, intermittent starvation, and washing (to simulate rainfall). The prototypes were mesophilic, and methane oxidation activity remained strong after one cycle of starvation but then declined with repeated cycles. Many of the cells detached with vigorous washing, but at least 30% appeared resistant to sloughing. While laboratory landfill simulations showed that four-layer composite biotarps made with two different types of geotextile could remove up to 50% of influent methane introduced at a flux rate of 22 g m{sup -2} d{sup -1}, field experiments did not yield high activity levels. Tests revealed that there were high hour-to-hour flux variations in the field, which, together with frequent rainfall events, confounded the field testing. Overall, the findings suggest that a methanotroph embedded biotarp appears to be a feasible strategy to mitigate methane emission from landfill cells, although the performance of field-tested biotarps was not robust here. Tarps will likely be best suited for spring and summer use, although the methane oxidizer population may be able to shift and adapt to lower temperatures. The starvation cycling of the tarp may require the capacity for intermittent reinoculation of the cells, although it is also possible that a subpopulation will adapt to the cycling and become dominant. Rainfall is not expected to be a major factor, because a baseline biofilm will be present to repopulate the tarp. If strong performance can be achieved and documented, the biotarp concept could be extended to include interception of other compounds beyond methane, such as volatile aromatic hydrocarbons and chlorinated solvents.« less
Applications for activated carbons from waste tires: Natural gas storage and air pollution control
Brady, T.A.; Rostam-Abadi, M.; Rood, M.J.
1996-01-01
Natural gas storage for natural gas vehicles and the separation and removal of gaseous contaminants from gas streams represent two emerging applications for carbon adsorbents. A possible precursor for such adsorbents is waste tires. In this study, activated carbon has been developed from waste tires and tested for its methane storage capacity and SO2 removal from a simulated flue-gas. Tire-derived carbons exhibit methane adsorption capacities (g/g) within 10% of a relatively expensive commercial activated carbon; however, their methane storage capacities (Vm/Vs) are almost 60% lower. The unactivated tire char exhibits SO2 adsorption kinetics similar to a commercial carbon used for flue-gas clean-up. Copyright ?? 1996 Elsevier Science Ltd.
Catalysis of carbon monoxide methanation by deep sea manganate minerals
NASA Technical Reports Server (NTRS)
Cabrera, A. L.; Maple, M. B.; Arrhenius, G.
1990-01-01
The catalytic activity of deep sea manganese nodule minerals for the methanation of carbon monoxide was measured with a microcatalytic technique between 200 and 460 degrees C. The manganate minerals were activated at 248 degrees C by immersion into a stream of hydrogen in which pulses of carbon monoxide were injected. Activation energies for the methanation reaction and hydrogen desorption from the manganate minerals were obtained and compared with those of pure nickel. Similar energy values indicate that the activity of the nodule materials for the reaction appears to be related to the amount of reducible transition metals present in the samples (ca. 11 wt.-%). Since the activity of the nodule minerals per gram is comparable to that of pure nickel, most of the transition metal ions located between manganese oxide layers appear to be exposed and available to catalyze the reaction.
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.
Ünal, Burcu; Perry, Verlin Ryan; Sheth, Mili; Gomez-Alvarez, Vicente; Chin, Kuk-Jeong; Nüsslein, Klaus
2012-01-01
Microbial methane from coal beds accounts for a significant and growing percentage of natural gas worldwide. Our knowledge of physical and geochemical factors regulating methanogenesis is still in its infancy. We hypothesized that in these closed systems, trace elements (as micronutrients) are a limiting factor for methanogenic growth and activity. Trace elements are essential components of enzymes or cofactors of metabolic pathways associated with methanogenesis. This study examined the effects of eight trace elements (iron, nickel, cobalt, molybdenum, zinc, manganese, boron, and copper) on methane production, on mcrA transcript levels, and on methanogenic community structure in enrichment cultures obtained from coal bed methane (CBM) well produced water samples from the Powder River Basin, Wyoming. Methane production was shown to be limited both by a lack of additional trace elements as well as by the addition of an overly concentrated trace element mixture. Addition of trace elements at concentrations optimized for standard media enhanced methane production by 37%. After 7 days of incubation, the levels of mcrA transcripts in enrichment cultures with trace element amendment were much higher than in cultures without amendment. Transcript levels of mcrA correlated positively with elevated rates of methane production in supplemented enrichments (R2 = 0.95). Metabolically active methanogens, identified by clone sequences of mcrA mRNA retrieved from enrichment cultures, were closely related to Methanobacterium subterraneum and Methanobacterium formicicum. Enrichment cultures were dominated by M. subterraneum and had slightly higher predicted methanogenic richness, but less diversity than enrichment cultures without amendments. These results suggest that varying concentrations of trace elements in produced water from different subsurface coal wells may cause changing levels of CBM production and alter the composition of the active methanogenic community. PMID:22590465
Clathrate hydrates as possible source of episodic methane releases on Mars
NASA Astrophysics Data System (ADS)
Karatekin, Özgür; Gloesener, Elodie; Temel, Orkun
2017-04-01
Methane has been shown to vary with location and time in the Martian atmosphere, with abundances of up to tens of parts-per-billion by volume (ppbv). Since methane is short-lived on geological time scales, its presence implies the existence of an active, current source of methane that is yet to be understood. In this study we investigate the destabilization of subsurface reservoirs of clathrate hydrates as a possible geological source of methane. Clathrate hydrates are crystalline compounds constituted by cages of hydrogen-bonded water molecules, inside of which guest gas molecules are trapped. We show the present-day maps of methane clathrate stability zones, in particular in the vicinity of Gale Crater where the Sample Analysis at Mars (SAM) suite on the Curiosity rover has made in situ measurements of atmospheric methane, during more than 3 years. Curiosity has observed spikes of elevated methane levels of 7 ppbv on four sequential observations over a 2-month period. The possibility of episodic releases consistent with curiosity observations from a subsurface clathrate source, is investigated using a gas transport through porous Martian regolith considering different depths of reservoirs. Transport of the released methane spike into the atmosphere is simulated using the PlanetWRF model.
Mobility and persistence of methane in groundwater in a controlled-release field experiment
NASA Astrophysics Data System (ADS)
Cahill, Aaron G.; Steelman, Colby M.; Forde, Olenka; Kuloyo, Olukayode; Emil Ruff, S.; Mayer, Bernhard; Ulrich Mayer, K.; Strous, Marc; Cathryn Ryan, M.; Cherry, John A.; Parker, Beth L.
2017-03-01
Expansion of shale gas extraction has fuelled global concern about the potential impact of fugitive methane on groundwater and climate. Although methane leakage from wells is well documented, the consequences on groundwater remain sparsely studied and are thought by some to be minor. Here we present the results of a 72-day methane gas injection experiment into a shallow, flat-lying sand aquifer. In our experiment, although a significant fraction of methane vented to the atmosphere, an equal portion remained in the groundwater. We find that methane migration in the aquifer was governed by subtle grain-scale bedding that impeded buoyant free-phase gas flow and led to episodic releases of free-phase gas. The result was lateral migration of gas beyond that expected by groundwater advection alone. Methane persisted in the groundwater zone despite active growth of methanotrophic bacteria, although much of the methane that vented into the vadose zone was oxidized. Our findings demonstrate that even small-volume releases of methane gas can cause extensive and persistent free phase and solute plumes emanating from leaks that are detectable only by contaminant hydrogeology monitoring at high resolution.
Evidence of Methane Outgassing During MIS3 in the Bering Sea
NASA Astrophysics Data System (ADS)
Cook, M. S.; Keigwin, L. D.
2005-12-01
There are multiple negative excursions in planktonic and benthic foraminifer δ13C in a core from 1467m in the southeast Bering Sea. These excursions occur episodically during the last glacial period, and may coincide with Dansgaard-Oeschger (D-O) events. Measured foraminifer δ13C during the excursions is as low as -14‰ and are probably the result of overgrowths of diagenetic calcium carbonate. We estimate overgrowth δ13C is -23‰, and hypothesize that the occurrence of overgrowths is associated with anaerobic oxidation of biogenic methane. The likely pressure and temperature conditions at this site and during the last glacial period were well within the zone of methane-hydrate stability, so the source of methane is probably not from destabilization of methane hydrate at this depth. The methane may have originated from increased in-situ methanogenesis resulting from greater burial of organic carbon, or from destabilization of methane hydrate at shallower sites near the methane-hydrate stability threshold. Both these scenarios could be active, consistent with the ``Clathrate Gun Hypothesis'' (Kennett et al., 2003), in which there is widespread destabilization of marine methane hydrates during D-O events, where methane gas both is oxidized within the water column and escapes to the atmosphere.
Characterisation of methane isotope composition over the Silesian Coal Basin, Poland.
NASA Astrophysics Data System (ADS)
Necki, Jaroslaw; Zimnoch, Miroslaw; Jasek, Alina; Chmura, Lukasz; Galkowski, Michal; Wolkowicz, Wojciech
2017-04-01
Methane emissions from Silesian Coal Basin (SCB), one of European regions associated with coal excavation industry constitute an important component of the continental anthropogenic flux of this gas into the atmosphere. It is estimated by different methodology that SCB is responsible for between 450 - 1350 Gg CH4 of atmospheric methane releases annually, making it one of the most significant sources of this gas in Europe. In this region, active or restructuring coal mining methane emissions may lead to elevated concentrations of this gas in near-ground atmosphere. Observed methane mixing ratio in pbl during nighttime over the specific areas of SCB is elevated by up to 50ppm with carbon isotope source ratio -46‰ to -52‰ with occasionally lighter methane (-58) form particular coal beds. Numbers were derived from direct measurement of samples taken from ventilation shafts (concentration 1.5% to 4% of CH4, subsequently diluted to 2ppm with zero air and measured by Picarro CRDS analyzer). Measurements of CH4 mixing ratios and isotopic composition were performed along latitudinal transects (ca. 50oN), typically extending from ca. 15oE to 20oE, covering the Upper Silesia and bordering regions on the public roads in vicinity of the mine ventilation shafts. Apart from CH4 emissions associated with coal production, other sources of anthropogenic methane are also active over SCB. These include city gas networks leakages that enrich the air by up to 5ppm (in the city centers, carbon isotope ratio on average -52). Most of the numerous landfills, not yet equipped with appropriate CH4 uptake installations, also contribute to substantial anthropogenic flux of this gas to the atmosphere. Values of methane mixing ratio recorded during the in-situ measurements close to the landfill sites reached 15ppm (with carbon isotope ratio -56‰ to -60). The transects of methane concentration over Silesian area, assisted by analysis of its stable isotopic composition has been performed in all of the locations where active and closed mining shafts are positioned, and most of the landfills and cities under the different meteorological and synoptic conditions to provide a base for efficient future verification of methane inventory over SCB. Project will be continued with MEMO2 ITN H2020.
Methanotrophs and methanogens in masonry
Kussmaul; Wilimzig; Bock
1998-11-01
Methanotrophs were present in 48 of 225 stone samples which were removed from 19 historical buildings in Germany and Italy. The average cell number of methanotrophs was 20 CFU per g of stone, and their activities ranged between 11 and 42 pmol of CH4 g of stone-1 day-1. Twelve strains of methane-oxidizing bacteria were isolated. They belonged to the type II methanotrophs of the genera Methylocystis, Methylosinus, and Methylobacterium. In masonry, growth substrates like methane or methanol are available in very low concentrations. To determine if methane could be produced by the stone at rates sufficient to support growth of methanotrophs, methane production by stone samples under nonoxic conditions was examined. Methane production of 0.07 to 215 nmol of CH4 g of stone-1 day-1 was detected in 23 of 47 stone samples examined. This indicated the presence of the so-called "mini-methane"-producing bacteria and/or methanogenic archaea. Methanotrophs occurred in nearly all samples which showed methane production. This finding indicated that methanotrophs depend on biogenic methane production in or on stone surfaces of historical buildings.
Methane on Mars: Measurements and Possible Origins
NASA Technical Reports Server (NTRS)
Mumma, Michael J.; Villanueva, Geronimo L.; Novak, Robert E.; Radeva, Yana L.; Kaufl, H. Ulrich; Tokunaga, Alan; Encrenaz, Therese; Hartogh, Paul
2011-01-01
The presence of abundant methane in Earth's atmosphere (1.6 parts per million) requires sources other than atmospheric chemistry. Living systems produce more than 90% of Earth's atmospheric methane; the balance is of geochemical origin. On Mars, methane has been sought for nearly 40 years because of its potential biological significance, but it was detected only recently [1-5]. Its distribution on the planet is found to be patchy and to vary with time [1,2,4,5], suggesting that methane is released recently from the subsurface in localized areas, and is then rapidly destroyed [1,6]. Before 2000, searchers obtained sensitive upper limits for methane by averaging over much of Mars' dayside hemisphere, using data acquired by Marsorbiting spacecraft (Mariner 9) and Earth-based observatories (Kitt Peak National Observatory, Canada- France-Hawaii Telescope, Infrared Space Observatory). These negative findings suggested that methane should be searched at higher spatial resolution since the local abundance could be significantly larger at active sites. Since 2001, searches for methane have emphasized spatial mapping from terrestrial observatories and from Mars orbit (Mars Express).
Long-term effect of ZnO nanoparticles on waste activated sludge anaerobic digestion.
Mu, Hui; Chen, Yinguang
2011-11-01
The increasing use of zinc oxide nanoparticles (ZnO NPs) raises concerns about their environmental impacts, but the potential effect of ZnO NPs on sludge anaerobic digestion remains unknown. In this paper, long-term exposure experiments were carried out to investigate the influence of ZnO NPs on methane production during waste activated sludge (WAS) anaerobic digestion. The presence of 1 mg/g-TSS of ZnO NPs did not affect methane production, but 30 and 150 mg/g-TSS of ZnO NPs induced 18.3% and 75.1% of inhibition respectively, which showed that the impact of ZnO NPs on methane production was dosage dependant. Then, the mechanisms of ZnO NPs affecting sludge anaerobic digestion were investigated. It was found that the toxic effect of ZnO NPs on methane production was mainly due to the release of Zn(2+) from ZnO NPs, which may cause the inhibitory effects on the hydrolysis and methanation steps of sludge anaerobic digestion. Further investigations with enzyme and fluorescence in situ hybridization (FISH) assays indicated that higher concentration of ZnO NPs decreased the activities of protease and coenzyme F(420), and the abundance of methanogenesis Archaea. Copyright © 2011 Elsevier Ltd. All rights reserved.
Could Methane Oxidation in Lakes Be Enhanced by Eutrophication?
NASA Astrophysics Data System (ADS)
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.
Gebert, J; Gröngröft, A
2006-01-01
An upflow biofilter system was operated on a passively vented landfill for the treatment of residual landfill methane. Biofilter methane emissions as a basis for determining methane removal rates were assessed by manual and automated chamber measurements, by measuring methane concentrations in the top layer gaseous phase in combination with gas flow rates, and by evaluating the methane load in the reverse gas flow following the change of landfill gas flux direction as governed by the course of barometric pressure. Methane removal rates were very high with maximum values of 80 g h(-1) m(-3). For the observed cases, the limit of biofilter methane oxidation capacity was not reached and absolute removal rates were thus linearly correlated to the amount of methane entering the filter. The analysis of methane loads flowing back from the biofilter following phases of longer, continuous and non-oscillating landfill gas emission, however, revealed that in these situations biofilter performance is restricted by deficient oxygen supply. At the oxygen-restricted capacity limit, removal rates are influenced by temperature (positively), methane influx (negatively) and flow rate (negatively) as a measure for the displacement of oxygen. These situations, however, account for only 12% of all emission phases. The investigated biofilter capacity, as derived from laboratory analyses of methanotrophic activities, is sufficient to oxidise 62% of the methane load emitted annually. Field and laboratory data provide a stable basis for the dimensioning of filters in future applications.
Federal Register 2010, 2011, 2012, 2013, 2014
2011-07-26
... for reducing methane emissions. By joining, Natural Gas STAR partners agree to implement cost-effective technologies and practices to reduce methane emissions, which will save money, improve operational...
Microbial methane production in oxygenated water column of an oligotrophic lake
Grossart, Hans-Peter; Frindte, Katharina; Dziallas, Claudia; Eckert, Werner; Tang, Kam W.
2011-01-01
The prevailing paradigm in aquatic science is that microbial methanogenesis happens primarily in anoxic environments. Here, we used multiple complementary approaches to show that microbial methane production could and did occur in the well-oxygenated water column of an oligotrophic lake (Lake Stechlin, Germany). Oversaturation of methane was repeatedly recorded in the well-oxygenated upper 10 m of the water column, and the methane maxima coincided with oxygen oversaturation at 6 m. Laboratory incubations of unamended epilimnetic lake water and inoculations of photoautotrophs with a lake-enrichment culture both led to methane production even in the presence of oxygen, and the production was not affected by the addition of inorganic phosphate or methylated compounds. Methane production was also detected by in-lake incubations of lake water, and the highest production rate was 1.8–2.4 nM⋅h−1 at 6 m, which could explain 33–44% of the observed ambient methane accumulation in the same month. Temporal and spatial uncoupling between methanogenesis and methanotrophy was supported by field and laboratory measurements, which also helped explain the oversaturation of methane in the upper water column. Potentially methanogenic Archaea were detected in situ in the oxygenated, methane-rich epilimnion, and their attachment to photoautotrophs might allow for anaerobic growth and direct transfer of substrates for methane production. Specific PCR on mRNA of the methyl coenzyme M reductase A gene revealed active methanogenesis. Microbial methane production in oxygenated water represents a hitherto overlooked source of methane and can be important for carbon cycling in the aquatic environments and water to air methane flux. PMID:22089233
Vigneron, Adrien; Bishop, Andrew; Alsop, Eric B.; Hull, Kellie; Rhodes, Ileana; Hendricks, Robert; Head, Ian M.; Tsesmetzis, Nicolas
2017-01-01
The Pennsylvania region hosts numerous oil and gas reservoirs and the presence of hydrocarbons in groundwater has been locally observed. However, these methane-containing freshwater ecosystems remain poorly explored despite their potential importance in the carbon cycle. Methane isotope analysis and analysis of low molecular weight hydrocarbon gases from 18 water wells indicated that active methane cycling may be occurring in methane-containing groundwater from the Pennsylvania region. Consistent with this observation, multigenic qPCR and gene sequencing (16S rRNA genes, mcrA, and pmoA genes) indicated abundant populations of methanogens, ANME-2d (average of 1.54 × 104 mcrA gene per milliliter of water) and bacteria associated with methane oxidation (NC10, aerobic methanotrophs, methylotrophs; average of 2.52 × 103 pmoA gene per milliliter of water). Methane cycling therefore likely represents an important process in these hydrocarbon-containing aquifers. The microbial taxa and functional genes identified and geochemical data suggested that (i) methane present is at least in part due to methanogens identified in situ; (ii) Potential for aerobic and anaerobic methane oxidation is important in groundwater with the presence of lineages associated with both anaerobic an aerobic methanotrophy; (iii) the dominant methane oxidation process (aerobic or anaerobic) can vary according to prevailing conditions (oxic or anoxic) in the aquifers; (iv) the methane cycle is closely associated with the nitrogen cycle in groundwater methane seeps with methane and/or methanol oxidation coupled to denitrification or nitrate and nitrite reduction. PMID:28424678
Methodology of Estimation of Methane Emissions from Coal Mines in Poland
NASA Astrophysics Data System (ADS)
Patyńska, Renata
2014-03-01
Based on a literature review concerning methane emissions in Poland, it was stated in 2009 that the National Greenhouse Inventory 2007 [13] was published. It was prepared firstly to meet Poland's obligations resulting from point 3.1 Decision no. 280/2004/WE of the European Parliament and of the Council of 11 February 2004, concerning a mechanism for monitoring community greenhouse gas emissions and for implementing the Kyoto Protocol and secondly, for the United Nations Framework Convention on Climate Change (UNFCCC) and Kyoto Protocol. The National Greenhouse Inventory states that there are no detailed data concerning methane emissions in collieries in the Polish mining industry. That is why the methane emission in the methane coal mines of Górnośląskie Zagłębie Węglowe - GZW (Upper Silesian Coal Basin - USCB) in Poland was meticulously studied and evaluated. The applied methodology for estimating methane emission from the GZW coal mining system was used for the four basic sources of its emission. Methane emission during the mining and post-mining process. Such an approach resulted from the IPCC guidelines of 2006 [10]. Updating the proposed methods (IPCC2006) of estimating the methane emissions of hard coal mines (active and abandoned ones) in Poland, assumes that the methane emission factor (EF) is calculated based on methane coal mine output and actual values of absolute methane content. The result of verifying the method of estimating methane emission during the mining process for Polish coal mines is the equation of methane emission factor EF.
High-temperature catalyst for catalytic combustion and decomposition
NASA Technical Reports Server (NTRS)
Mays, Jeffrey A. (Inventor); Lohner, Kevin A. (Inventor); Sevener, Kathleen M. (Inventor); Jensen, Jeff J. (Inventor)
2005-01-01
A robust, high temperature mixed metal oxide catalyst for propellant composition, including high concentration hydrogen peroxide, and catalytic combustion, including methane air mixtures. The uses include target, space, and on-orbit propulsion systems and low-emission terrestrial power and gas generation. The catalyst system requires no special preheat apparatus or special sequencing to meet start-up requirements, enabling a fast overall response time. Start-up transients of less than 1 second have been demonstrated with catalyst bed and propellant temperatures as low as 50 degrees Fahrenheit. The catalyst system has consistently demonstrated high decomposition effeciency, extremely low decomposition roughness, and long operating life on multiple test particles.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ganesh, Rangaraj; Torrijos, Michel, E-mail: michel.torrijos@supagro.inra.fr; Sousbie, Philippe
Highlights: • Single-phase and two-phase systems were compared for fruit and vegetable waste digestion. • Single-phase digestion produced a methane yield of 0.45 m{sup 3} CH{sub 4}/kg VS and 83% VS removal. • Substrate solubilization was high in acidification conditions at 7.0 kg VS/m{sup 3} d and pH 5.5–6.2. • Energy yield was lower by 33% for two-phase system compared to the single-phase system. • Simple and straight-forward operation favored single phase process over two-phase process. - Abstract: Single-phase and two-phase digestion of fruit and vegetable waste were studied to compare reactor start-up, reactor stability and performance (methane yield, volatilemore » solids reduction and energy yield). The single-phase reactor (SPR) was a conventional reactor operated at a low loading rate (maximum of 3.5 kg VS/m{sup 3} d), while the two-phase system consisted of an acidification reactor (TPAR) and a methanogenic reactor (TPMR). The TPAR was inoculated with methanogenic sludge similar to the SPR, but was operated with step-wise increase in the loading rate and with total recirculation of reactor solids to convert it into acidification sludge. Before each feeding, part of the sludge from TPAR was centrifuged, the centrifuge liquid (solubilized products) was fed to the TPMR and centrifuged solids were recycled back to the reactor. Single-phase digestion produced a methane yield of 0.45 m{sup 3} CH{sub 4}/kg VS fed and VS removal of 83%. The TPAR shifted to acidification mode at an OLR of 10.0 kg VS/m{sup 3} d and then achieved stable performance at 7.0 kg VS/m{sup 3} d and pH 5.5–6.2, with very high substrate solubilization rate and a methane yield of 0.30 m{sup 3} CH{sub 4}/kg COD fed. The two-phase process was capable of high VS reduction, but material and energy balance showed that the single-phase process was superior in terms of volumetric methane production and energy yield by 33%. The lower energy yield of the two-phase system was due to the loss of energy during hydrolysis in the TPAR and the deficit in methane production in the TPMR attributed to COD loss due to biomass synthesis and adsorption of hard COD onto the flocs. These results including the complicated operational procedure of the two-phase process and the economic factors suggested that the single-phase process could be the preferred system for FVW.« less
NASA Astrophysics Data System (ADS)
Orphan, V. J.; McGlynn, S.; Chadwick, G.; Dekas, A.; Green-Saxena, A.
2013-12-01
Sulfate-coupled anaerobic oxidation of methane is catalysed through symbiotic associations between archaea and sulphate-reducing bacteria and represents the dominant sink for methane in the oceans. These methane-oxidizing symbiotic consortia form well-structured multi-celled aggregations in marine methane seeps, where close spatial proximity is believed to be essential for efficient exchange of substrates between syntrophic partners. The nature of this interspecies metabolic relationship is still unknown however there are a number of hypotheses regarding the electron carrying intermediate and ecophysiology of the partners, each of which should be affected by, and influence, the spatial arrangement of archaeal and bacterial cells within aggregates. To advance our understanding of the role of spatial structure within naturally occurring environmental consortia, we are using spatial statistical methods combined with fluorescence in situ hybridization and high-resolution nanoscale secondary ion mass spectrometry (FISH-nanoSIMS) to quantify the effect of spatial organization and intra- and inter-species interactions on cell-specific microbial activity within these diverse archaeal-bacterial partnerships.
DISCOVERY OF FOG AT THE SOUTH POLE OF TITAN
DOE Office of Scientific and Technical Information (OSTI.GOV)
Brown, M. E.; Smith, A. L.; Chen, C.
2009-11-20
While Saturn's moon Titan appears to support an active methane hydrological cycle, no direct evidence for surface-atmosphere exchange has yet appeared. The indirect evidence, while compelling, could be misleading. It is possible, for example, that the identified lake features could be filled with ethane, an involatile long-term residue of atmospheric photolysis; the apparent stream and channel features could be ancient remnants of a previous climate; and the tropospheric methane clouds, while frequent, could cause no rain to reach the surface. We report here the detection of fog at the south pole of Titan during late summer using observations from themore » VIMS instrument on board the Cassini spacecraft. While terrestrial fog can form from a variety of causes, most of these processes are inoperable on Titan. Fog on Titan can only be caused by evaporation of nearly pure liquid methane; the detection of fog provides the first direct link between surface and atmospheric methane. Based on the detections presented here, liquid methane appears widespread at the south pole of Titan in late southern summer, and the hydrological cycle on Titan is currently active.« less
Lee, Eun-Hee; Choi, Sun-Ah; Yi, Taewoo; Kim, Tae Gwan; Lee, Sang-Don; Cho, Kyung-Suk
2015-01-01
Two identical lab-scale bioreactor systems were operated to examine the effects of granular activated carbon (GAC) on methane removal performance and methanotrophic community. Both bioreactor systems removed methane completely at a CH4 loading rate of 71.2 g-CH4·d(-1) for 17 days. However, the methane removal efficiency declined to 88% in the bioreactor without GAC, while the bioreactor amended with GAC showed greater methane removal efficiency of 97% at a CH4 loading rate of 107.5 g-CH4·d(-1). Although quantitative real-time PCR showed that methanotrophic populations were similar levels of 5-10 × 10(8) pmoA gene copy number·VSS(-1) in both systems, GAC addition changed the methanotrophic community composition of the bioreactor systems. Microarray assay revealed that GAC enhanced the type I methanotrophic genera including Methylobacter, Methylomicrobium, and Methylomonas of the system, which suggests that GAC probably provided a favorable environment for type I methanotrophs. These results indicated that GAC is a promising support material in bioreactor systems for CH4 mitigation.
The Methane to Markets Coal Mine Methane Subcommittee meeting
DOE Office of Scientific and Technical Information (OSTI.GOV)
NONE
2008-07-01
The presentations (overheads/viewgraphs) include: a report from the Administrative Support Group; strategy updates from Australia, India, Italy, Mexico, Nigeria, Poland and the USA; coal mine methane update and IEA's strategy and activities; the power of VAM - technology application update; the emissions trading market; the voluntary emissions reduction market - creating profitable CMM projects in the USA; an Italian perspective towards a zero emission strategies; and the wrap-up and summary.
JPRS Report. Science & Technology: Japan
1987-07-16
methane. So, it has been proved that seawater containing methane and sulfur, which oozed out at this point from underground, grew bacteria, a food ...activity was measured by dispersing glass powder at the seabed and the speed of extinction due to food poisoning was also measured by leaving dead...solar light is very small due to the scarcity of food . However, a special ecosystem nourished with bacteria, which eat methane and inorganic compounds
Rice cultivation and methane emission: Documentation of distributed geographic data sets
NASA Technical Reports Server (NTRS)
Matthews, Elaine; John, Jasmin; Fung, Inez
1994-01-01
High-resolution global data bases on the geographic and seasonal distribution of rice cultivation and associated methane emission, compiled by Matthews et al., were archived for public use. In addition to the primary data sets identifying location, seasonality, and methane emission from rice cultivation, a series of supporting data sets is included, allowing users not only to replicate the work of Matthews et al. but to investigate alternative cultivation and emission scenarios. The suite of databases provided, at 1 latitude by 1 longitude resolution for the globe, includes (1) locations of rice cultivation, (2) monthly arrays of actively growing rice areas, (3) countries and political subdivisions, and (4) monthly arrays of methane emission from rice cultivation. Ancillary data include (1) a listing, by country, of harvested rice areas and seasonal distribution of crop cycles and (2) country names and codes. Summary tables of zonal/monthly distributions of actively growing rice areas and of methane emissions are presented. Users should consult original publications for complete discussion of the data bases. This short paper is designed only to document formats of the distributed information and briefly describe the contents of the data sets and their initial application to evaluating the role of rice cultivation in the methane budget.
van der Ha, David; Vanwonterghem, Inka; Hoefman, Sven; De Vos, Paul; Boon, Nico
2013-03-01
Due to the increasing atmospheric concentration of the greenhouse gas methane, more knowledge is needed on the management of methanotrophic communities. While most studies have focused on the characteristics of the methane-oxidizing bacteria (MOB), less is known about their interactions with the associated heterotrophs. Interpretative tools based on denaturing gradient gel electrophoresis allowed to evaluate the influence of copper-an important enzymatic regulator for MOB-on the activity and composition of the bacterial community. Over 30 days, enrichments with 0.1, 1.0 and 10 μM Cu(2+) respectively, showed comparable methane oxidation activities. The different copper concentrations did not create major shifts in the methanotrophic communities, as a Methylomonas sp. was able to establish dominance at all different copper concentrations by switching between both known methane monooxygenases. The associated heterotrophic communities showed continuous shifts, but over time all cultures evolved to a comparable composition, independent of the copper concentration. This indicates that the MOB selected for certain heterotrophs, possibly fulfilling vital processes such as removal of toxic compounds. The presence of a large heterotrophic food web indirectly depending on methane as sole carbon and energy source was confirmed by a clone library wherein MOB only formed a minority of the identified species.
Assessing the Efficacy of the Aerobic Methanotrophic Biofilter in Methane Hydrate Environments
DOE Office of Scientific and Technical Information (OSTI.GOV)
Valentine, David
2012-09-30
In October 2008 the University of California at Santa Barbara (UCSB) initiated investigations of water column methane oxidation in methane hydrate environments, through a project funded by the National Energy Technology Laboratory (NETL) entitled: assessing the efficacy of the aerobic methanotrophic biofilter in methane hydrate environments. This Final Report describes the scientific advances and discoveries made under this award as well as the importance of these discoveries in the broader context of the research area. Benthic microbial mats inhabit the sea floor in areas where reduced chemicals such as sulfide reach the more oxidizing water that overlies the sediment. Wemore » set out to investigate the role that methanotrophs play in such mats at locations where methane reaches the sea floor along with sulfide. Mats were sampled from several seep environments and multiple sets were grown in-situ at a hydrocarbon seep in the Santa Barbara Basin. Mats grown in-situ were returned to the laboratory and used to perform stable isotope probing experiments in which they were treated with 13C-enriched methane. The microbial community was analyzed, demonstrating that three or more microbial groups became enriched in methane?s carbon: methanotrophs that presumably utilize methane directly, methylotrophs that presumably consume methanol excreted by the methanotrophs, and sulfide oxidizers that presumably consume carbon dioxide released by the methanotrophs and methylotrophs. Methanotrophs reached high relative abundance in mats grown on methane, but other bacterial processes include sulfide oxidation appeared to dominate mats, indicating that methanotrophy is not a dominant process in sustaining these benthic mats, but rather a secondary function modulated by methane availability. Methane that escapes the sediment in the deep ocean typically dissolved into the overlying water where it is available to methanotrophic bacteria. We set out to better understand the efficacy of this process as a biofilter by studying the distribution of methane oxidation and disposition of methanotrophic populations in the Pacific Ocean. We investigated several environments including the basins offshore California, the continental margin off Central America, and the shallow waters around gas seeps. We succeeded in identifying the distributions of activity in these environments, identified potential physical and chemical controls on methanotrophic activity, we further revealed details about the methanotrophic communities active in these settings, and we developed new approaches to study methanotrophic communities. These findings should improve our capacity to predict the methanotrophic response in ocean waters, and further our ability to generate specific hypotheses as to the ecology and efficacy of pelagic methanotrophic communites. The discharge of methane and other hydrocarbons to Gulf of Mexico that followed the sinking of the Deepwater Horizon provided a unique opportunity to study the methanotorphic biofilter in the deep ocean environment. We set out to understand the consumption of methane and the bloom of methanotrophs resulting from this event, as a window into the regional scale release of gas hydrate under rapid warming scenarios. We found that other hydrocarbon gases, notably propane and ethane, were preferred for consumption over methane, but that methane consumption accelerated rapidly and drove the depletion of methane within a matter of months after initial release. These results revealed the identity of the responsible community, and point to the importance of the seed population in determining the rate at which a methanotrophic community is able to respond to an input of methane. Collectively, these results provide a significant advance in our understanding of the marine methanotrohic biofilter, and further provide direction and context for future investigations of this important phenomenon. This project has resulted in fourteen publications to date, with five more circulating in draft form, and several others planned.« less
NASA Astrophysics Data System (ADS)
Rella, Chris; Jacobson, Gloria; Crosson, Eric; Karion, Anna; Petron, Gabrielle; Sweeney, Colm
2013-04-01
Fugitive emissions of methane into the atmosphere are a major concern facing the natural gas production industry. Because methane is more energy-rich than coal per kg of CO2 emitted into the atmosphere, it represents an attractive alternative to coal for electricity generation. However, given that the global warming potential of methane is many times greater than that of carbon dioxide (Solomon et al. 2007), the importance of quantifying the fugitive emissions of methane throughout the natural gas production and distribution process becomes clear (Howarth et al. 2011). A key step in the process of assessing the emissions arising from natural gas production activities is partitioning the observed methane emissions between natural gas fugitive emissions and other sources of methane, such as from landfills or agricultural activities. One effective method for assessing the contribution of these different sources is stable isotope analysis. In particular, the 13CH4 signature of natural gas (-35 to -40 permil) is significantly different that the signature of other significant sources of methane, such as landfills or ruminants (-45 to -70 permil). In this paper we present measurements of mobile field 13CH4 using a spectroscopic stable isotope analyzer based on cavity ringdown spectroscopy, in two intense natural gas producing regions of the United States: the Denver-Julesburg basin in Colorado, and the Uintah basin in Utah. Mobile isotope measurements in the nocturnal boundary layer have been made, over a total path of 100s of km throughout the regions, allowing spatially resolved measurements of the regional isotope signature. Secondly, this analyzer was used to quantify the isotopic signature of those individual sources (natural gas fugitive emissions, concentrated animal feeding operations, and landfills) that constitute the majority of methane emissions in these regions, by making measurements of the isotope ratio directly in the downwind plume from each source. These data are combined to establish the fraction of the observed methane emissions that can be attributed to natural gas activities in the regions. The fraction of total methane emissions in the Denver-Julesburg basin that can be attributed to natural gas fugitive emissions has been determined to be 71 +/- 9%. References: 1. S. Solomon, D. Qin, M. Manning, Z. Chen, M. Marquis, K.B. Averyt, M.Tignor and H.L. Miller (eds.). IPCC, 2007: Climate Change 2007: The Physical Science Basis of the Fourth Assessment Report. Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA. 2. R.W. Howarth, R. Santoro, and A. Ingraffea. "Methane and the greenhouse-gas footprint of natural gas from shale formations." Climate Change, 106, 679 (2011).
NASA Astrophysics Data System (ADS)
Rella, C.; Crosson, E.; Petron, G.; Sweeney, C.; Karion, A.
2013-12-01
Fugitive emissions of methane into the atmosphere are a major concern facing the natural gas production industry. Because methane is more energy-rich than coal per kg of CO2 emitted into the atmosphere, it represents an attractive alternative to coal for electricity generation, provided that the fugitive emissions of methane are kept under control. A key step in assessing these emissions in a given region is partitioning the observed methane emissions between natural gas fugitive emissions and other sources of methane, such as from landfills or agricultural activities. One effective method for assessing the contribution of these different sources is stable isotope analysis, using the δ13CH4 signature to distinguish between natural gas and landfills or ruminants. We present measurements of mobile field δ13CH4 using a spectroscopic stable isotope analyzer based on cavity ringdown spectroscopy, in three intense natural gas producing regions of the United States: the Denver-Julesburg basin in Colorado, the Uintah basin in Utah, and the Barnett Shale in Texas. Mobile isotope measurements of individual sources and in the nocturnal boundary layer have been combined to establish the fraction of the observed methane emissions that can be attributed to natural gas activities. The fraction of total methane emissions in the Denver-Julesburg basin attributed to natural gas emissions is 78 +/- 13%. In the Uinta basin, which has no other significant sources of methane, the fraction is 96% +/- 15%. In addition, results from the Barnett shale are presented, which includes a major urban center (Dallas / Ft. Worth). Methane emissions in this region are spatially highly heterogeneous. Spatially-resolved isotope and concentration measurements are interpreted using a simple emissions model to arrive at an overall isotope ratio for the region. (left panel) Distribution of oil and gas well pads (yellow) and landfills (blue) in the Dallas / Ft. Worth area. Mobile nocturnal measurements of methane are shown in red, indicating a strong degree of source heterogeneity. (right panel) Histogram of individual isotopic source signatures, showing distinct signatures for landfills (red) and oil and gas sources (green).
Feasibility Assessment of CO2 Sequestration and Enhanced Recovery in Gas Shale Reservoirs
NASA Astrophysics Data System (ADS)
Vermylen, J. P.; Hagin, P. N.; Zoback, M. D.
2008-12-01
CO2 sequestration and enhanced methane recovery may be feasible in unconventional, organic-rich, gas shale reservoirs in which the methane is stored as an adsorbed phase. Previous studies have shown that organic-rich, Appalachian Devonian shales adsorb approximately five times more carbon dioxide than methane at reservoir conditions. However, the enhanced recovery and sequestration concept has not yet been tested for gas shale reservoirs under realistic flow and production conditions. Using the lessons learned from previous studies on enhanced coalbed methane (ECBM) as a starting point, we are conducting laboratory experiments, reservoir modeling, and fluid flow simulations to test the feasibility of sequestration and enhanced recovery in gas shales. Our laboratory work investigates both adsorption and mechanical properties of shale samples to use as inputs for fluid flow simulation. Static and dynamic mechanical properties of shale samples are measured using a triaxial press under realistic reservoir conditions with varying gas saturations and compositions. Adsorption is simultaneously measured using standard, static, volumetric techniques. Permeability is measured using pulse decay methods calibrated to standard Darcy flow measurements. Fluid flow simulations are conducted using the reservoir simulator GEM that has successfully modeled enhanced recovery in coal. The results of the flow simulation are combined with the laboratory results to determine if enhanced recovery and CO2 sequestration is feasible in gas shale reservoirs.
Marlow, Jeffrey J.; Skennerton, Connor T.; Li, Zhou; Chourey, Karuna; Hettich, Robert L.; Pan, Chongle; Orphan, Victoria J.
2016-01-01
Marine methane seep habitats represent an important control on the global flux of methane. Nucleotide-based meta-omics studies outline community-wide metabolic potential, but expression patterns of environmentally relevant proteins are poorly characterized. Proteomic stable isotope probing (proteomic SIP) provides additional information by characterizing phylogenetically specific, functionally relevant activity in mixed microbial communities, offering enhanced detection through system-wide product integration. Here we applied proteomic SIP to 15NH4+ and CH4 amended seep sediment microcosms in an attempt to track protein synthesis of slow-growing, low-energy microbial systems. Across all samples, 3495 unique proteins were identified, 11% of which were 15N-labeled. Consistent with the dominant anaerobic oxidation of methane (AOM) activity commonly observed in anoxic seep sediments, proteins associated with sulfate reduction and reverse methanogenesis—including the ANME-2 associated methylenetetrahydromethanopterin reductase (Mer)—were all observed to be actively synthesized (15N-enriched). Conversely, proteins affiliated with putative aerobic sulfur-oxidizing epsilon- and gammaproteobacteria showed a marked decrease over time in our anoxic sediment incubations. The abundance and phylogenetic range of 15N-enriched methyl-coenzyme M reductase (Mcr) orthologs, many of which exhibited novel post-translational modifications, suggests that seep sediments provide niches for multiple organisms performing analogous metabolisms. In addition, 26 proteins of unknown function were consistently detected and actively expressed under conditions supporting AOM, suggesting that they play important roles in methane seep ecosystems. Stable isotope probing in environmental proteomics experiments provides a mechanism to determine protein durability and evaluate lineage-specific responses in complex microbial communities placed under environmentally relevant conditions. Our work here demonstrates the active synthesis of a metabolically specific minority of enzymes, revealing the surprising longevity of most proteins over the course of an extended incubation experiment in an established, slow-growing, methane-impacted environmental system. PMID:27199908
Zhang, Yong; Zhao, Hua-de; Zhai, Wei-dong; Zang, Kun-peng; Wang, Ju-ying
2014-04-15
The distributions of dissolved methane in the central Bohai Sea were investigated in November 2011, May 2012, July 2012, and August 2012. Methane concentration in surface seawater, determined using an underway measurement system combined with wavelength-scanned cavity ring-down spectroscopy, showed marked spatiotemporal variations with saturation ratio from 107% to 1193%. The central Bohai Sea was thus a source of atmospheric methane during the survey periods. Several episodic oil and gas spill events increased surface methane concentration by up to 4.7 times and raised the local methane outgassing rate by up to 14.6 times. This study demonstrated a method to detect seafloor CH4 leakages at the sea surface, which may have applicability in many shallow sea areas with oil and gas exploration activities around the world. Copyright © 2014 Elsevier Ltd. All rights reserved.
Influence of headspace flushing on methane production in Biochemical Methane Potential (BMP) tests.
Koch, Konrad; Bajón Fernández, Yadira; Drewes, Jörg E
2015-06-01
The influence of headspace flushing on the specific methane (CH4) production of blank samples with just inoculum in Biochemical Methane Potential (BMP) tests was studied. The three most common ways were applied: flushing with nitrogen (N2) gas, flushing with a mixture of N2 and CO2 (80/20 v/v), and no flushing. The results revealed that removing the oxygen is crucial to avoid aerobic respiration, which caused both hindered activity of methanogens and loss of methane potential. Furthermore it was demonstrated that 20% of CO2 in the flush gas increased significantly the methane production by over 20% compared to the flushing with pure N2. In order to mimic the same headspace conditions as in full-scale treatment plants, using a flush gas with a similar CO2 concentration as the expected biogas is suggested. Copyright © 2015 Elsevier Ltd. All rights reserved.
Federal Register 2010, 2011, 2012, 2013, 2014
2012-06-21
... dust and explosive methane gas are present. Diesel equipment operating in underground coal mines also..., such as cabs or canopies, methane monitors, brakes and lights. Sampling of diesel exhaust emissions is...
Federal Register 2010, 2011, 2012, 2013, 2014
2011-12-27
... operation and maintenance of this equipment. These standards rely on the capture and reduction of methane, carbon dioxide, and non-methane organic gas compound emissions by combustion devices (boilers, internal...
DOE Office of Scientific and Technical Information (OSTI.GOV)
Ikuno, Takaaki; Zheng, Jian; Vjunov, Aleksei
The catalyzed conversion of shale gas-derived light hydrocarbons, e.g. methane to methanol, for further application as automotive fuels and/or bulk chemicals is especially attractive in light of improved methods of hydrocarbon extraction. MOF based catalysts have previously been demonstrated to be active for a range of catalytic reactions. In this work we used Cu-NU1000 as a methane-to-methanol oxidation catalyst. In addition to product studies, in-situ X-ray Absorption Spectroscopic (XAS) experiments are performed under catalytic conditions in order to follow the modification of the Cu-species and directly probe the structure/activity properties of the Cu-NU1000 system. The insights reported herein serve asmore » a first look at metal-organic framework materials as catalysts for methane oxidation and be the basis for development of the subsequent generations of materials.« less
Adsorbed Natural Gas Storage in Optimized High Surface Area Microporous Carbon
NASA Astrophysics Data System (ADS)
Romanos, Jimmy; Rash, Tyler; Nordwald, Erik; Shocklee, Joshua Shawn; Wexler, Carlos; Pfeifer, Peter
2011-03-01
Adsorbed natural gas (ANG) is an attractive alternative technology to compressed natural gas (CNG) or liquefied natural gas (LNG) for the efficient storage of natural gas, in particular for vehicular applications. In adsorbants engineered to have pores of a few molecular diameters, a strong van der Walls force allows reversible physisorption of methane at low pressures and room temperature. Activated carbons were optimized for storage by varying KOH:C ratio and activation temperature. We also consider the effect of mechanical compression of powders to further enhance the volumetric storage capacity. We will present standard porous material characterization (BET surface area and pore-size distribution from subcritical N2 adsorption) and methane isotherms up to 250 bar at 293K. At sufficiently high pressure, specific surface area, methane binding energy and film density can be extracted from supercritical methane adsorption isotherms. Research supported by the California Energy Commission (500-08-022).
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.
Alqaralleh, Rania Mona; Kennedy, Kevin; Delatolla, Robert; Sartaj, Majid
2016-12-01
Renewable energy and clean environment are two crucial requirements for our modern world. Low cost, energy production and limited environmental impact make anaerobic digestion (AD) a promising technology for stabilizing organic waste and in particular, sewage waste. The anaerobic co-digestion of thickened waste activated sludge (TWAS) and sewage treatment plant trapped fat, oil and grease (FOG) using different FOG-TWAS mixtures (20, 40, 60 and 80% of FOG based on total volatile solids (TVS)) were investigated in this study using both thermophilic (55 ± 1 °C) and two stages hyper-thermophilic/thermophilic (70 ± 1 °C and 55 ± 1 °C) anaerobic co-digestion. The hyper-thermophilic co-digestion approach as a part of the co-digestion process has been shown to be very useful in improving the methane production. During hyper-thermophilic biochemical methane potential (BMP) assay testing the sample with 60% FOG (based on TVS) has been shown to significantly increase the maximum methane production to 673.1 ± 14.0 ml of methane as compared to 316.4 ± 14.3 ml of methane for the control sample. This represents a 112.7% increase in methane production compared to the control sample considered in this paper. These results signify the importance of hyper-thermophilic digestion to the co-digestion of TWAS-FOG field. Copyright © 2016 Elsevier Ltd. All rights reserved.
Barnhart, Elliott P.; Davis, Katherine J.; Varonka, Matthew; Orem, William H.; Cunningham, Alfred B.; Ramsay, Bradley D.; Fields, Matthew W.
2017-01-01
Many coal beds contain microbial communities that can convert coal to natural gas (coalbed methane). Native microorganisms were obtained from Powder River Basin (PRB) coal seams with a diffusive microbial sampler placed downhole and used as an inoculum for enrichments with different nutrients to investigate microbially-enhanced coalbed methane production (MECoM). Coal-dependent methanogenesis more than doubled when yeast extract (YE) and several less complex components (proteins and amino acids) were added to the laboratory microcosms. Stimulated coal-dependent methanogenesis with peptone was 86% of that with YE while glutamate-stimulated activity was 65% of that with YE, and a vitamin mix had only 33% of the YE stimulated activity. For field application of MECoM, there is interest in identifying cost-effective alternatives to YE and other expensive nutrients. In laboratory studies, adding algal extract (AE) with lipids removed stimulated coal-dependent methanogenesis and the activity was 60% of that with YE at 27 d and almost 90% of YE activity at 1406 d. Analysis of British Thermal Unit (BTU) content of coal (a measure of potential energy yield) from long-term incubations indicated > 99.5% of BTU content remained after coalbed methane (CBM) stimulation with either AE or YE. Thus, the coal resource remains largely unchanged following stimulated microbial methane production. Algal CBM stimulation could lead to technologies that utilize coupled biological systems (photosynthesis and methane production) that sustainably enhance CBM production and generate algal biofuels while also sequestering carbon dioxide (CO2).
Ho, Adrian; Reim, Andreas; Kim, Sang Yoon; Meima-Franke, Marion; Termorshuizen, Aad; de Boer, Wietse; van der Putten, Wim H; Bodelier, Paul L E
2015-10-01
Intensification of agriculture to meet the global food, feed, and bioenergy demand entail increasing re-investment of carbon compounds (residues) into agro-systems to prevent decline of soil quality and fertility. However, agricultural intensification decreases soil methane uptake, reducing, and even causing the loss of the methane sink function. In contrast to wetland agricultural soils (rice paddies), the methanotrophic potential in well-aerated agricultural soils have received little attention, presumably due to the anticipated low or negligible methane uptake capacity in these soils. Consequently, a detailed study verifying or refuting this assumption is still lacking. Exemplifying a typical agricultural practice, we determined the impact of bio-based residue application on soil methane flux, and determined the methanotrophic potential, including a qualitative (diagnostic microarray) and quantitative (group-specific qPCR assays) analysis of the methanotrophic community after residue amendments over 2 months. Unexpectedly, after amendments with specific residues, we detected a significant transient stimulation of methane uptake confirmed by both the methane flux measurements and methane oxidation assay. This stimulation was apparently a result of induced cell-specific activity, rather than growth of the methanotroph population. Although transient, the heightened methane uptake offsets up to 16% of total gaseous CO2 emitted during the incubation. The methanotrophic community, predominantly comprised of Methylosinus may facilitate methane oxidation in the agricultural soils. While agricultural soils are generally regarded as a net methane source or a relatively weak methane sink, our results show that methane oxidation rate can be stimulated, leading to higher soil methane uptake. Hence, even if agriculture exerts an adverse impact on soil methane uptake, implementing carefully designed management strategies (e.g. repeated application of specific residues) may compensate for the loss of the methane sink function following land-use change. © 2015 John Wiley & Sons Ltd.
NASA Astrophysics Data System (ADS)
Dekas, A. E.; Connon, S. A.; Chadwick, G.; Orphan, V. J.
2012-12-01
Methane seep microbial ecosystems are phylogenetically diverse and physiologically complex, and require culture-independent techniques to accurately investigate metabolic activity. In the present study we combine an RNA analysis of four key microbial genes with FISH-NanoSIMS analysis of single cells to determine the diversity of nitrogen fixing microorganisms (diazotrophs) present at a deep-sea methane-seeping site, as well as investigate the methane-dependency of a variety of community members. Recently, methane-dependent nitrogen fixation was observed in Mound 12 Costa Rica sediments, and was spatially correlated with the abundance of aggregates of anaerobic methanotrophic archaea (ANME) and sulfate reducing bacterial symbionts (SRB). Combined with the detection of 15N uptake from 15N2 in these aggregates, this suggested that the ANME-SRB aggregates are the primary diazotrophs in seep sediment. However, the diversity of dinitrogenase reductase (nifH) sequences recovered from several deep-sea locales, including Mound 12, suggests a greater diversity of diazotrophs in marine sediment. To investigate the activity of these potential diazotrophs in Mound 12 sediment, we investigated a suite of RNA transcripts in 15N2 incubations in both the presence and absence of methane: nifH, bacterial 16S rRNA, methyl coenzyme M reductase A (mcrA), and adenosine-5'-phosposulfate reductase alpha subunit (aprA). No nifH transcripts were recovered in incubations without methane, consistent with previous measurements lacking 15N2 uptake in the same sediments. The activity of the bacterial community in general, assessed by variable transcription, was also greatly affected by the presence or absence of methane. Single-cell fluorescence in situ hybridization coupled to nanoscale secondary ion mass spectrometry (FISH-NanoSIMS) was employed to confirm diazotrophic activity (15N2 uptake) and protein synthesis (15NH4+ uptake) of particular species implicated as ecologically important by the pattern of transcripts recovered in the mesocosm experiments. This analysis revealed 15N enrichment in free-living (i.e. non-ANME associated) members of the Desulfobulbaceae in 15N2 incubations with methane, while free-living Desulfosarcina/Desulfococcus cells, as well as nearly 40 unidentified DAPI-stained cells, were not 15N enriched. However, further NanoSIMS analyses of DSB in a variety of incubation conditions suggests that this enrichment may be due to N sharing between the ANME and DSB while in tight physical association, and then subsequent dissociation, rather than nitrogen fixation by the DSB. If true, this is an excellent example of the potential pitfalls of single cell stable isotope labeling experiments, and potential false positives due to the recycling of labeled material between (even transiently) closely associated symbionts. This work highlights both the utility of transcript analysis as a hypothesis-generator for direct analyses of microbial activity via stable isotope labeling, as well as the need to contextualize labeling experiments with investigations of microbial community structure.
Wang, Dongbo; Zhao, Jianwei; Zeng, Guangming; Chen, Yinguang; Bond, Philip L; Li, Xiaoming
2015-10-20
Recent studies demonstrate that, besides being used for production of biodegradable plastics, poly(hydroxyalkanoate) (PHA) that is accumulated in heterotrophic microorganisms during wastewater treatment has another novel application direction, i.e., being utilized for enhancing methane yield during the anaerobic digestion of waste-activated sludge (WAS). To date, however, the underlying mechanism of how PHA affects methane production remains largely unknown, and this limits optimization and application of the strategy. This study therefore aims to fill this knowledge gap. Experimental results showed that with the increase of sludge PHA levels from 21 to 184 mg/g of volatile suspended solids (VSS) the methane yield linearly increased from 168.0 to 246.1 mL/g of VSS (R(2) = 0.9834). Compared with protein and carbohydrate (the main components of a cell), PHA exhibited a higher biochemical methane potential on a unit VSS basis. It was also found that the increased PHA not only enhanced cell disruption of PHA cells but also benefited the soluble protein conversion of both PHA- and non-PHA cells. Moreover, the reactor fed with higher PHA sludge showed greater sludge hydrolysis and acidification than those fed with the lower PHA sludges. Further investigations using fluorescence in situ hybridization and enzyme analysis revealed that the increased PHA enhanced the abundance of methanogenic Archaea and increased the activities of protease, acetate kinase, and coenzyme F420, which were consistent with the observed methane yield. This work provides insights into PHA-involved WAS digestion systems and may have important implications for future operation of wastewater treatment plants.
NASA Astrophysics Data System (ADS)
Treude, T.; Krause, S.; Bertics, V. J.; Steinle, L.; Niemann, H.; Liebetrau, V.; Feseker, T.; Burwicz, E.; Krastel, S.; Berndt, C.
2014-12-01
In 2008, a large area with several hundred methane plumes was discovered along the West Spitsbergen continental margin at water depths between 150 and 400 m (Westbrook et al. 2009, GRL 36, doi:10.1029/2009GL039191). Many of the observed plumes were located at the boundary of gas hydrate stability (~400 m water depth). It was speculated that the methane escape at this depth was correlated with gas hydrate destabilization caused by recent increases in water temperatures recorded in this region. In a later study, geochemical analyses of authigenic carbonates and modeling of heat flow data combined with seasonal changes in water temperature demonstrated that the methane seeps were active already prior to industrial warming but that the gas hydrate system nevertheless reacts very sensitive to even seasonal temperature changes (Berndt et al. 2014, Science 343: 284-287). Here, we report about a methane seep site at the gas hydrate stability boundary (394 m water depth) that features unusual geochemical profiles indicative for non-steady state conditions. Sediment was recovered with a gravity corer (core length 210 cm) and samples were analyzed to study porewater geochemistry, methane concentration, authigenic carbonates, and microbial activity. Porewater profiles revealed two zones of sulfate-methane transition at 50 and 200 cm sediment depth. The twin zones were confirmed by a double peaking in sulfide, total alkalinity, anaerobic oxidation of methane, and sulfate reduction. δ18O values sharply increased from around -2.8 ‰ between 0 and 126 cm to -1.2 ‰ below 126 cm sediment depth. While U/Th isotope measurements of authigenic seep carbonates that were collected from different depths of the core illustrated that methane seepage must be occurring at this site since at least 3000 years, the biogeochemical profiles suggest that methane flux must have been altered recently. By applying a multi-phase reaction-transport model using known initial parameters from the study site (e.g. water depth, temperature profile, salinity, and sediment surface concentrations of CH4, SO4, DIC, and POC) were able to show that the observed twin sulfate-methane transition zones are an ephemeral phenomenon occurring during increase of methane production in the sediment, which can be introduced by, e.g., gas hydrate dissociation.
NASA Astrophysics Data System (ADS)
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. Collectively, our results provided evidence for the possible decoupling of AOM and SR under in situconditions. This decoupling appears to be widespread in methane-rich marine sediment, motivating a wide variety of future research endeavors.
Moritz, Anja; Hélie, Jean-Francois; Pinti, Daniele L; Larocque, Marie; Barnetche, Diogo; Retailleau, Sophie; Lefebvre, René; Gélinas, Yves
2015-04-07
Hydraulic fracturing is becoming an important technique worldwide to recover hydrocarbons from unconventional sources such as shale gas. In Quebec (Canada), the Utica Shale has been identified as having unconventional gas production potential. However, there has been a moratorium on shale gas exploration since 2010. The work reported here was aimed at defining baseline concentrations of methane in shallow aquifers of the St. Lawrence Lowlands and its sources using δ(13)C methane signatures. Since this study was performed prior to large-scale fracturing activities, it provides background data prior to the eventual exploitation of shale gas through hydraulic fracturing. Groundwater was sampled from private (n = 81), municipal (n = 34), and observation (n = 15) wells between August 2012 and May 2013. Methane was detected in 80% of the wells with an average concentration of 3.8 ± 8.8 mg/L, and a range of <0.0006 to 45.9 mg/L. Methane concentrations were linked to groundwater chemistry and distance to the major faults in the studied area. The methane δ(1)(3)C signature of 19 samples was > -50‰, indicating a potential thermogenic source. Localized areas of high methane concentrations from predominantly biogenic sources were found throughout the study area. In several samples, mixing, migration, and oxidation processes likely affected the chemical and isotopic composition of the gases, making it difficult to pinpoint their origin. Energy companies should respect a safe distance from major natural faults in the bedrock when planning the localization of hydraulic fracturation activities to minimize the risk of contaminating the surrounding groundwater since natural faults are likely to be a preferential migration pathway for methane.
Liu, Lin; Sun, Qinglei; Wang, Ruobing; Chen, Zeli; Wu, Jiangchun; Xia, Fangzhou; Fan, Xian-Qun
2016-09-01
Retinal ischemia/reperfusion injury (IRI) may cause incurable visual impairment due to neural regeneration limits. Methane was shown to exert a protective effect against IRI in many organs. This study aims to explore the possible protective effects of methane-rich saline against retinal IRI in rat. Retinal IRI was performed on the right eyes of male Sprague-Dawley rats, which were immediately injected intraperitoneally with methane-saturated saline (25ml/kg). At one week after surgery, the number of retinal ganglion cells (RGCs), total retinal thickness, visual function were measured by hematoxylin and eosin staining, FluoroGold anterograde labeling and flash visual evoked potentials. The levels of 8-hydroxy-2-deoxyguanosine (8-OHdG), 4-Hydroxy-2-nonenal (4-HNE), malondialdehyde (MDA), superoxide dismutase (SOD), catalase (CAT), glutathione peroxidase (GPx), caspase-3, caspase-9, B cell lymphoma/leukemia-2 (Bcl-2) and Bcl-2 associated X protein (Bax) in retinas were assessed by immunofluorescence staining, enzyme-linked immunosorbent assay and quantitative polymerase chain reaction. As expected, methane treatment significantly improved the retinal IRI-induced RGC loss, total retinal layer thinning and visual dysfunction. Moreover, methane treatment significantly reduced the levels of oxidative stress biomarkers (8-OHdG, 4-HNE, MDA) and increased the antioxidant enzyme activities (SOD, CAT, GPx) in the retinas with IRI. Meanwhile, methane treatment significantly increased the anti-apoptotic gene (Bcl-2) expression and decreased the pro-apoptotic gene (Bax) expression, accompanied by the suppression of caspase-3 and caspase-9 activity. Thus, these data demonstrated that methane can exert a neuroprotective role against retinal IRI through anti-oxidative and anti-apoptotic pathways. Copyright © 2016. Published by Elsevier B.V.
Non-Detection of Methane in the Mars Atmosphere by the Curiosity Rover
NASA Technical Reports Server (NTRS)
Webster, Chris R.; Mahaffy, Paul R.; Atreya, Sushil K.; Flesch, Gregory J.; Farley, Kenneth A.
2014-01-01
By analogy with Earth, methane in the atmosphere of Mars is a potential signature of ongoing or past biological activity on the planet. During the last decade, Earth-based telescopic and Mars orbit remote sensing instruments have reported significant abundances of methane in the Martian atmosphere ranging from several to tens of parts-per-billion by volume (ppbv). Observations from Earth showed plumes of methane with variations on timescales much faster than expected and inconsistent with localized patches seen from orbit, prompting speculation of sources from sub-surface methanogen bacteria, geological water-rock reactions or infall from comets, micro-meteorites or interplanetary dust. From measurements on NASAs Curiosity Rover that landed near Gale Crater on 5th August 2012, we here report no definitive detection of methane in the near-surface Martian atmosphere. Our in situ measurements were made using the Tunable Laser Spectrometer (TLS) in the Sample Analysis at Mars (SAM) instrument suite6 that made three separate searches on Martian sols 79, 81 and 106 after landing. The measured mean value of 0.39 plus or minus 1.4 ppbv corresponds to an upper limit for methane abundance of 2.7 ppbv at the 95 confidence level. This result is in disagreement with both the remote sensing spacecraft observations taken at lower sensitivity and the telescopic observations that relied on subtraction of a very large contribution from terrestrial methane in the intervening observation path. Since the expected lifetime of methane in the Martian atmosphere is hundreds of years, our results question earlier observations and set a low upper limit on the present day abundance, reducing the probability of significant current methanogenic microbial activity on Mars.
NASA Astrophysics Data System (ADS)
Bar Or, I.; Ben-Dov, E.; Kushmaro, A.; Eckert, W.; Sivan, O.
2014-06-01
Microbial methane oxidation process (methanotrophy) is the primary control on the emission of the greenhouse gas methane (CH4) to the atmosphere. In terrestrial environments, aerobic methanotrophic bacteria are mainly responsible for oxidizing the methane. In marine sediments the coupling of the anaerobic oxidation of methane (AOM) with sulfate reduction, often by a consortium of anaerobic methanotrophic archaea (ANME) and sulfate reducing bacteria, was found to consume almost all the upward diffusing methane. Recently, we showed geochemical evidence for AOM driven by iron reduction in Lake Kinneret (LK) (Israel) deep sediments and suggested that this process can be an important global methane sink. The goal of the present study was to link the geochemical gradients found in the porewater (chemical and isotope profiles) with possible changes in microbial community structure. Specifically, we examined the possible shift in the microbial community in the deep iron-driven AOM zone and its similarity to known sulfate driven AOM populations. Screening of archaeal 16S rRNA gene sequences revealed Thaumarchaeota and Euryarchaeota as the dominant phyla in the sediment. Thaumarchaeota, which belongs to the family of copper containing membrane-bound monooxgenases, increased with depth while Euryarchaeota decreased. This may indicate the involvement of Thaumarchaeota, which were discovered to be ammonia oxidizers but whose activity could also be linked to methane, in AOM in the deep sediment. ANMEs sequences were not found in the clone libraries, suggesting that iron-driven AOM is not through sulfate. Bacterial 16S rRNA sequences displayed shifts in community diversity with depth. Proteobacteria and Chloroflexi increased with depth, which could be connected with their different dissimilatory anaerobic processes. The observed changes in microbial community structure suggest possible direct and indirect mechanisms for iron-driven AOM in deep sediments.
Wei, Shiping; Cui, Hongpeng; Zhu, Youhai; Lu, Zhenquan; Pang, Shouji; Zhang, Shuai; Dong, Hailiang; Su, Xin
2018-05-01
Permafrost thaw can bring negative consequences in terms of ecosystems, resulting in permafrost collapse, waterlogging, thermokarst lake development, and species composition changes. Little is known about how permafrost thaw influences microbial community shifts and their activities. Here, we show that the dominant archaeal community shifts from Methanomicrobiales to Methanosarcinales in response to the permafrost thaw, and the increase in methane emission is found to be associated with the methanogenic archaea, which rapidly bloom with nearly tenfold increase in total number. The mcrA gene clone libraries analyses indicate that Methanocellales/Rice Cluster I was predominant both in the original permafrost and in the thawed permafrost. However, only species belonging to Methanosarcinales showed higher transcriptional activities in the thawed permafrost, indicating a shift of methanogens from hydrogenotrophic to partly acetoclastic methane-generating metabolic processes. In addition, data also show the soil texture and features change as a result of microbial reproduction and activity induced by this permafrost thaw. Those data indicate that microbial ecology under warming permafrost has potential impacts on ecosystem and methane emissions.
Miller, Benjamin L; Arntzen, Evan V; Goldman, Amy E; Richmond, Marshall C
2017-10-01
The United States is home to 2198 dams actively used for hydropower production. With the December 2015 consensus adoption of the United Nations Framework Convention on Climate Change Paris Agreement, it is important to accurately quantify anthropogenic greenhouse gas emissions. Methane ebullition, or methane bubbles originating from river or lake sediments, has been shown to account for nearly all methane emissions from tropical hydropower reservoirs to the atmosphere. However, distinct ebullitive methane fluxes have been studied in comparatively few temperate hydropower reservoirs globally. This study measures ebullitive and diffusive methane fluxes from two eastern Washington reservoirs, and synthesizes existing studies of methane ebullition in temperate, boreal, and tropical hydropower reservoirs. Ebullition comprises nearly all methane emissions (>97%) from this study's two eastern Washington hydropower reservoirs to the atmosphere. Summer methane ebullition from these reservoirs was higher than ebullition in six southeastern U.S. hydropower reservoirs, however it was similar to temperate reservoirs in other parts of the world. Our literature synthesis suggests that methane ebullition from temperate hydropower reservoirs can be seasonally elevated compared to tropical climates, however annual emissions are likely to be higher within tropical climates, emphasizing the possible range of methane ebullition fluxes and the need for the further study of temperate reservoirs. Possible future changes to the Intergovernmental Panel on Climate Change and UNFCCC guidelines for national greenhouse gas inventories highlights the need for accurate assessment of reservoir emissions.
NASA Astrophysics Data System (ADS)
Miller, Benjamin L.; Arntzen, Evan V.; Goldman, Amy E.; Richmond, Marshall C.
2017-10-01
The United States is home to 2198 dams actively used for hydropower production. With the December 2015 consensus adoption of the United Nations Framework Convention on Climate Change Paris Agreement, it is important to accurately quantify anthropogenic greenhouse gas emissions. Methane ebullition, or methane bubbles originating from river or lake sediments, has been shown to account for nearly all methane emissions from tropical hydropower reservoirs to the atmosphere. However, distinct ebullitive methane fluxes have been studied in comparatively few temperate hydropower reservoirs globally. This study measures ebullitive and diffusive methane fluxes from two eastern Washington reservoirs, and synthesizes existing studies of methane ebullition in temperate, boreal, and tropical hydropower reservoirs. Ebullition comprises nearly all methane emissions (>97%) from this study's two eastern Washington hydropower reservoirs to the atmosphere. Summer methane ebullition from these reservoirs was higher than ebullition in six southeastern U.S. hydropower reservoirs, however it was similar to temperate reservoirs in other parts of the world. Our literature synthesis suggests that methane ebullition from temperate hydropower reservoirs can be seasonally elevated compared to tropical climates, however annual emissions are likely to be higher within tropical climates, emphasizing the possible range of methane ebullition fluxes and the need for the further study of temperate reservoirs. Possible future changes to the Intergovernmental Panel on Climate Change and UNFCCC guidelines for national greenhouse gas inventories highlights the need for accurate assessment of reservoir emissions.
Enzymes involved in the anaerobic oxidation of n-alkanes: from methane to long-chain paraffins
Callaghan, Amy V.
2013-01-01
Anaerobic microorganisms play key roles in the biogeochemical cycling of methane and non-methane alkanes. To date, there appear to be at least three proposed mechanisms of anaerobic methane oxidation (AOM). The first pathway is mediated by consortia of archaeal anaerobic methane oxidizers and sulfate-reducing bacteria (SRB) via “reverse methanogenesis” and is catalyzed by a homolog of methyl-coenzyme M reductase. The second pathway is also mediated by anaerobic methane oxidizers and SRB, wherein the archaeal members catalyze both methane oxidation and sulfate reduction and zero-valent sulfur is a key intermediate. The third AOM mechanism is a nitrite-dependent, “intra-aerobic” pathway described for the denitrifying bacterium, ‘Candidatus Methylomirabilis oxyfera.’ It is hypothesized that AOM proceeds via reduction of nitrite to nitric oxide, followed by the conversion of two nitric oxide molecules to dinitrogen and molecular oxygen. The latter can be used to functionalize the methane via a particulate methane monooxygenase. With respect to non-methane alkanes, there also appear to be novel mechanisms of activation. The most well-described pathway is the addition of non-methane alkanes across the double bond of fumarate to form alkyl-substituted succinates via the putative glycyl radical enzyme, alkylsuccinate synthase (also known as methylalkylsuccinate synthase). Other proposed mechanisms include anaerobic hydroxylation via ethylbenzene dehydrogenase-like enzymes and an “intra-aerobic” denitrification pathway similar to that described for ‘Methylomirabilis oxyfera.’ PMID:23717304
NASA Technical Reports Server (NTRS)
Socki, Richard A.; Niles, Paul B.; Gibson, Everett K., Jr.; Romanek, Christopher S.; Zhang, Chuanlun L.; Bissada, Kadry K.
2008-01-01
The recent detection of methane in the Martian atmosphere and the possibility that its origin could be attributed to biological activity, have highlighted the importance of understanding the mechanisms of methane formation and its usefulness as a biomarker. Much debate has centered on the source of the methane in hydrothermal fluids, whether it is formed biologically by microorganisms, diagenetically through the decomposition of sedimentary organic matter, or inorganically via reduction of CO2 at high temperatures. Ongoing research has now shown that much of the methane present in sea-floor hydrothermal systems is probably formed through inorganic CO2 reduction processes at very high temperatures (greater than 400 C). Experimental results have indicated that methane might form inorganically at temperatures lower still, however these results remain controversial. Currently, methane in continental hydrothermal systems is thought to be formed mainly through the breakdown of sedimentary organic matter and carbon isotope equilibrium between CO2 and CH4 is thought to be rarely present if at all. Based on isotopic measurements of CO2 and CH4 in two continental hydrothermal systems, we suggest that carbon isotope equilibration exists at temperatures as low as 155 C. This would indicate that methane is forming through abiotic CO2 reduction at lower temperatures than previously thought and could bolster arguments for an abiotic origin of the methane detected in the martian atmosphere.
Biogeochemical Carbon Cycling in Ultrabasic Reducing Springs in Sonoma County, CA
NASA Astrophysics Data System (ADS)
Cotton, J. M.; Morrill, P.; Johnson, O.; Nealson, K. H.; Sherwood Lollar, B.; Eigenbrode, J.; Fogel, M.
2006-12-01
Dissolved gases in the ultrabasic spring waters from The Cedars in Sonoma County, CA were analyzed for concentrations and carbon and hydrogen isotopic ratios in order to determine the geobiological processes occurring in this extreme environment of unknown biological activity. The ultrabasic, highly reducing conditions unique to these springs result from local serpentinization. Gases bubbling from the springs are mainly composed of methane, hydrogen, and nitrogen. Serpentinization is a process characteristic of early Earth, Mars and Titan that is thought to produce abiogenic hydrocarbons as well as provide geochemical energy for chemolithotrophic life. Methane, CO2, hydrogen and nitrogen were detected in the aqueous phases. Earlier work indicated that the primary source of the methane in the free gases bubbling from the springs was associated with microbial fermentation a suspected source of the dissolved methane. Here we report, a negative, linear correlation between concentrations of CO2 and methane that is an indicator of microbial anaerobic methane oxidation taking place in the ultrabasic waters. Furthermore, as the concentrations of methane decrease, the concentration of CO2 increases and both reactant and product become 13C-enriched. These observations are consistent with microbial oxidation of methane, suggesting a biogeochemical carbon cycle exists in these springs. We hypothesize that one group of microbes is breaking down organic matter by a process of fermentation to produce methane and CO2. The CO2 dissolves in the basic springs, while most of the methane escapes solution. The residual dissolved methane undergoes a conversion to CO2 by anaerobic methane oxidation.
Hypotheses for a Near-Surface Reservoir of Methane and Its Release on Mars
NASA Astrophysics Data System (ADS)
Hu, R.; Bloom, A. A.; Gao, P.; Miller, C. E.; Yung, Y. L.
2015-12-01
The Curiosity rover recently detected a background of 0.7 ppb and spikes of 7 ppb of methane on Mars. This in situ measurement reorients our understanding of the Martian environment and its potential for life, as the current theories do not entail any active source or sink of methane. In particular, the 10-fold elevation during the southern winter indicates episodic sources of methane that are yet to be discovered. Using the temperature and humidity measurements from the rover, we find that perchlorate salts in the regolith deliquesce to form liquid solutions, and deliquescence progresses to deeper subsurface in the season of the methane spikes. We therefore formulate the following three testable hypotheses as an attempt to explain the apparent variability of the atmospheric methane abundance. The first scenario is that the regolith in Gale Crater adsorbs methane when dry and releases this methane to the atmosphere upon deliquescence. The adsorption energy needs to be 36 kJ mol-1 to explain the magnitude of the methane spikes, higher than laboratory measurements. The second scenario is that microorganisms exist and convert organic matter in the soil to methane when they are in liquid solutions. This scenario does not require regolith adsorption. The third scenario is that deep subsurface aquifers sealed by ice or clathrate produce bursts of methane as a result of freezing and thawing of the permafrost, as the terrestrial arctic tundra. Continued monitoring of methane by Curiosity will test the existence of the near-surface reservoir and its exchange with the atmosphere.
Molecular dynamics simulations of methane hydrate decomposition.
Myshakin, Evgeniy M; Jiang, Hao; Warzinski, Robert P; Jordan, Kenneth D
2009-03-12
Molecular dynamics simulations have been carried out to study decomposition of methane hydrate at different cage occupancies. The decomposition rate is found to depend sensitively on the hydration number. The rate of the destruction of the cages displays Arrhenius behavior, consistent with an activated mechanism. During the simulations, reversible formation of partial water cages around methane molecules in the liquid was observed at the interface at temperatures above the computed hydrate decomposition temperature.
Development of Carbon and Sulphur Tolerant Anodes of Solid Oxide Fuel Cells
2010-01-14
LSCM/YSZ) composite anode is investigated in detail for the direct utilization of ethanol and methane (the main component of natural gas) in SOFCs...Impregnation of Pd nanoparticles significantly promotes the electrocatalytic activity of LSCM/YSZ composite anodes for the ethanol and methane... electrooxidation reaction. At 800°C, the electrode polarization resistance for the methane oxidation is reduced by a factor of 3 after impregnation of 0.10
Limitations of microbial hydrocarbon degradation at the Amon mud volcano (Nile deep-sea fan)
NASA Astrophysics Data System (ADS)
Felden, J.; Lichtschlag, A.; Wenzhöfer, F.; de Beer, D.; Feseker, T.; Pop Ristova, P.; de Lange, G.; Boetius, A.
2013-05-01
The Amon mud volcano (MV), located at 1250 m water depth on the Nile deep-sea fan, is known for its active emission of methane and non-methane hydrocarbons into the hydrosphere. Previous investigations showed a low efficiency of hydrocarbon-degrading anaerobic microbial communities inhabiting the Amon MV center in the presence of sulfate and hydrocarbons in the seeping subsurface fluids. By comparing spatial and temporal patterns of in situ biogeochemical fluxes, temperature gradients, pore water composition, and microbial activities over 3 yr, we investigated why the activity of anaerobic hydrocarbon degraders can be low despite high energy supplies. We found that the central dome of the Amon MV, as well as a lateral mud flow at its base, showed signs of recent exposure of hot subsurface muds lacking active hydrocarbon degrading communities. In these highly disturbed areas, anaerobic degradation of methane was less than 2% of the methane flux. Rather high oxygen consumption rates compared to low sulfide production suggest a faster development of more rapidly growing aerobic hydrocarbon degraders in highly disturbed areas. In contrast, the more stabilized muds surrounding the central gas and fluid conduits hosted active anaerobic hydrocarbon-degrading microbial communities. The low microbial activity in the hydrocarbon-vented areas of Amon MV is thus a consequence of kinetic limitations by heat and mud expulsion, whereas most of the outer MV area is limited by hydrocarbon transport.
Potential impact of salinity on methane production from food waste anaerobic digestion.
Zhao, Jianwei; Liu, Yiwen; Wang, Dongbo; Chen, Fei; Li, Xiaoming; Zeng, Guangming; Yang, Qi
2017-09-01
Previous studies have demonstrated that the presence of sodium chloride (NaCl) inhibited the production of methane from food waste anaerobic digestion. However, the details of how NaCl affects methane production from food waste remain unknown by now and the efficient approach to mitigate the impact of NaCl on methane production was seldom reported. In this paper, the details of how NaCl affects methane production was first investigated via a series of batch experiments. Experimental results showed the effect of NaCl on methane production was dosage dependent. Low level of NaCl improved the hydrolysis and acidification but inhibited the process of methanogenesis whereas high level of NaCl inhibit both steps of acidification and methanogenesis. Then an efficient approach, i.e. co-digestion of food waste and waste activated sludge, to mitigate the impact of NaCl on methane production was reported. Finally, the mechanisms of how co-digestion mitigates the effect on methane production caused by NaCl in co-digestion system were revealed. These findings obtained in this work might be of great importance for the operation of methane recovery from food waste in the presence of NaCl. Copyright © 2017 Elsevier Ltd. All rights reserved.
NASA Astrophysics Data System (ADS)
Eilerman, S. J.; Neuman, J. A.; Peischl, J.; Aikin, K. C.; Ryerson, T. B.; Perring, A. E.; Robinson, E. S.; Holloway, M.; Trainer, M.
2015-12-01
Due to recent advances in extraction technology, oil and natural gas extraction and processing in the Denver-Julesburg basin has increased substantially in the past decade. Northeastern Colorado is also home to over 250 concentrated animal feeding operations (CAFOs), capable of hosting over 2 million head of ruminant livestock (cattle and sheep). Because of methane's high Global Warming Potential, quantification and attribution of methane emissions from oil and gas development and agricultural activity are important for guiding greenhouse gas emission policy. However, due to the co-location of these different sources, top-down measurements of methane are often unable to attribute emissions to a specific source or sector. In this work, we evaluate the ammonia:methane emission ratio directly downwind of CAFOs using a mobile laboratory. Several CAFOs were chosen for periodic study over a 12-month period to identify diurnal and seasonal variation in the emission ratio as well as differences due to livestock type. Using this knowledge of the agricultural ammonia:methane emission ratio, aircraft measurements of ammonia and methane over oil and gas basins in the western US during the Shale Oil and Natural Gas Nexus (SONGNEX) field campaign in March and April 2015 can be used for source attribution of methane emissions.
Effects of Environmental Conditions on an Urban Wetland's Methane Fluxes
NASA Astrophysics Data System (ADS)
Naor Azrieli, L.; Morin, T. H.; Bohrer, G.; Schafer, K. V.; Brooker, M.; Mitsch, W. J.
2013-12-01
Methane emissions from wetlands are the largest natural source of uncertainty in the global methane (CH4) budget. Wetlands are highly productive ecosystems with a large carbon sequestration potential. While wetlands are a net sink for carbon dioxide, they also release methane, a potent greenhouse gas. To effectively develop wetland management techniques, it is important to properly calculate the carbon budget of wetlands by understand the driving factors of methane fluxes. We constructed an eddy flux covariance system in the Olentangy River Wetland Research Park, a series of created and restored wetland in Columbus Ohio. Through the use of high frequency open path infrared gas analyzer (IRGA) sensors, we have continuously monitored the methane fluxes associated with the wetland since May 2011. To account for the heterogeneous landscape surrounding the tower, a footprint analysis was used to isolate data originating from within the wetland. Continuous measurements of the meteorological and environmental conditions at the wetlands coinciding with the flux measurements allow the interactions between methane fluxes and the climate and ecological forcing to be studied. The wintertime daily cycle of methane peaks around midday indicating a typical diurnal pattern in cold months. In the summer, the peak shifts to earlier in the day and also includes a daily peak occurring at approximately 10 AM. We believe this peak is associated with the onset of photosynthesis in Typha latifolia flushing methane from the plant's air filled tissue. Correlations with methane fluxes include latent heat flux, soil temperature, and incoming radiation. The connection to radiation may be further evidence of plant activity as a driver of methane fluxes. Higher methane fluxes corresponding with higher soil temperature indicates that warmer days stimulate the methanogenic consortium. Further analysis will focus on separating the methane fluxes into emissions from different terrain types within the wetland.
Willis, Joshua J.; Gallo, Alessandro; Sokaras, Dimosthenis; ...
2017-10-09
To limit further rising levels in methane emissions from stationary and mobile sources and to enable promising technologies based on methane, the development of efficient combustion catalysts that completely oxidize CH 4 to CO 2 and H 2O at low temperatures in the presence of high steam concentrations is required. Palladium is widely considered as one of the most promising materials for this reaction, and a better understanding of the factors affecting its activity and stability is crucial to design even more improved catalysts that efficiently utilize this precious metal. Here we report a study of the effect of threemore » important variables (particle size, support, and reaction conditions including water) on the activity of supported Pd catalysts. We use uniform palladium nanocrystals as catalyst precursors to prepare a library of well-defined catalysts to systematically describe structure–property relationships with help from theory and in situ X-ray absorption spectroscopy. With this approach, we confirm that PdO is the most active phase and that small differences in reaction rates as a function of size are likely due to variations in the surface crystal structure. We further demonstrate that the support exerts a limited influence on the PdO activity, with inert (SiO 2), acidic (Al 2O 3), and redox-active (Ce 0.8Zr 0.2O 2) supports providing similar rates, while basic (MgO) supports show remarkably lower activity. Finally, we show that the introduction of steam leads to a considerable decrease in rates that is due to coverage effects, rather than structural and/or phase changes. Altogether, the data suggest that to further increase the activity and stability of Pd-based catalysts for methane combustion, increasing the surface area of supported PdO phases while avoiding strong adsorption of water on the catalytic surfaces is required. Furthermore, this study clarifies contrasting reports in the literature about the active phase and stability of Pd-based materials for methane combustion.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Willis, Joshua J.; Gallo, Alessandro; Sokaras, Dimosthenis
To limit further rising levels in methane emissions from stationary and mobile sources and to enable promising technologies based on methane, the development of efficient combustion catalysts that completely oxidize CH 4 to CO 2 and H 2O at low temperatures in the presence of high steam concentrations is required. Palladium is widely considered as one of the most promising materials for this reaction, and a better understanding of the factors affecting its activity and stability is crucial to design even more improved catalysts that efficiently utilize this precious metal. Here we report a study of the effect of threemore » important variables (particle size, support, and reaction conditions including water) on the activity of supported Pd catalysts. We use uniform palladium nanocrystals as catalyst precursors to prepare a library of well-defined catalysts to systematically describe structure–property relationships with help from theory and in situ X-ray absorption spectroscopy. With this approach, we confirm that PdO is the most active phase and that small differences in reaction rates as a function of size are likely due to variations in the surface crystal structure. We further demonstrate that the support exerts a limited influence on the PdO activity, with inert (SiO 2), acidic (Al 2O 3), and redox-active (Ce 0.8Zr 0.2O 2) supports providing similar rates, while basic (MgO) supports show remarkably lower activity. Finally, we show that the introduction of steam leads to a considerable decrease in rates that is due to coverage effects, rather than structural and/or phase changes. Altogether, the data suggest that to further increase the activity and stability of Pd-based catalysts for methane combustion, increasing the surface area of supported PdO phases while avoiding strong adsorption of water on the catalytic surfaces is required. Furthermore, this study clarifies contrasting reports in the literature about the active phase and stability of Pd-based materials for methane combustion.« less
Geochemical evidences of methane hydrate dissociation in Alaskan Beaufort Margin during Holocene
NASA Astrophysics Data System (ADS)
Uchida, M.; Rella, S.; Kubota, Y.; Kumata, H.; Mantoku, K.; Nishino, S.; Itoh, M.
2017-12-01
Alaskan Beaufort margin bear large abundances of sub-sea and permafrost methane hydrate[Ruppel, 2016]. During the Last Glacial, previous reported direct and indirect evidences accumulated from geochemical data from marginal sea sediment suggests that methane episodically released from hydrate trapped in the seafloor sediments[Kennett et al., 2000; Uchida et al., 2006, 2008; Cook et al, 2011]. Here we analyzed stable isotopes of foraminifera and molecular marker derived from the activity of methanotrophic bacteria from piston cores collected by the 2010 R/V Mirai cruise in Alaskan Beaufort Margin. Our data showed highly depleted 13C compositions of benthic foraminifera, suggesting indirect records of enhanced incorporation of 13C-depleted CO2 formed by methanotrophic process that use 12C-enriched methane as their main source of carbon. This is the first evidence of methane hydrate dissociation in Alaskan margin. Here we discussed timing of signals of methane dissociation with variability of sea ice and intermediate Atlantic water temperature. The dissociation of methane hydrate in the Alaskan Margin may be modulated by Atlantic warm intermediate water warming. Our results suggest that Arctic marginal regions bearing large amount methane hydrate may be a profound effect on future warming climate changes.
NMR study of methane + ethane structure I hydrate decomposition.
Dec, Steven F; Bowler, Kristen E; Stadterman, Laura L; Koh, Carolyn A; Sloan, E Dendy
2007-05-24
The thermally activated decomposition of methane + ethane structure I hydrate was studied with use of 13C magic-angle spinning (MAS) NMR as a function of composition and temperature. The observed higher decomposition rate of large sI cages initially filled with ethane gas can be described in terms of a model where a distribution of sI unit cells exists such that a particular unit cell contains zero, one, or two methane molecules in the unit cell; this distribution of unit cells is combined to form the observed equilibrium composition. In this model, unit cells with zero methane molecules are the least stable and decompose more rapidly than those populated with one or two methane molecules leading to the observed overall faster decomposition rate of the large cages containing ethane molecules.
Controls on Methane Occurrences in Aquifers Overlying the Eagle Ford Shale Play, South Texas.
Nicot, Jean-Philippe; Larson, Toti; Darvari, Roxana; Mickler, Patrick; Uhlman, Kristine; Costley, Ruth
2017-07-01
Assessing natural vs. anthropogenic sources of methane in drinking water aquifers is a critical issue in areas of shale oil and gas production. The objective of this study was to determine controls on methane occurrences in aquifers in the Eagle Ford Shale play footprint. A total of 110 water wells were tested for dissolved light alkanes, isotopes of methane, and major ions, mostly in the eastern section of the play. Multiple aquifers were sampled with approximately 47 samples from the Carrizo-Wilcox Aquifer (250-1200 m depth range) and Queen City-Sparta Aquifer (150-900 m depth range) and 63 samples from other shallow aquifers but mostly from the Catahoula Formation (depth <150 m). Besides three shallow wells with unambiguously microbial methane, only deeper wells show significant dissolved methane (22 samples >1 mg/L, 10 samples >10 mg/L). No dissolved methane samples exhibit thermogenic characteristics that would link them unequivocally to oil and gas sourced from the Eagle Ford Shale. In particular, the well water samples contain very little or no ethane and propane (C1/C2+C3 molar ratio >453), unlike what would be expected in an oil province, but they also display relatively heavier δ 13 C methane (>-55‰) and δD methane (>-180‰). Samples from the deeper Carrizo and Queen City aquifers are consistent with microbial methane sourced from syndepositional organic matter mixed with thermogenic methane input, most likely originating from deeper oil reservoirs and migrating through fault zones. Active oxidation of methane pushes δ 13 C methane and δD methane toward heavier values, whereas the thermogenic gas component is enriched with methane owing to a long migration path resulting in a higher C1/C2+C3 ratio than in the local reservoirs. © 2017, National Ground Water Association.
Lloyd, Karen G.; Albert, Daniel B.; Biddle, Jennifer F.; Chanton, Jeffrey P.; Pizarro, Oscar; Teske, Andreas
2010-01-01
Background Subsurface fluids from deep-sea hydrocarbon seeps undergo methane- and sulfur-cycling microbial transformations near the sediment surface. Hydrocarbon seep habitats are naturally patchy, with a mosaic of active seep sediments and non-seep sediments. Microbial community shifts and changing activity patterns on small spatial scales from seep to non-seep sediment remain to be examined in a comprehensive habitat study. Methodology/Principal Findings We conducted a transect of biogeochemical measurements and gene expression related to methane- and sulfur-cycling at different sediment depths across a broad Beggiatoa spp. mat at Mississippi Canyon 118 (MC118) in the Gulf of Mexico. High process rates within the mat (∼400 cm and ∼10 cm from the mat's edge) contrasted with sharply diminished activity at ∼50 cm outside the mat, as shown by sulfate and methane concentration profiles, radiotracer rates of sulfate reduction and methane oxidation, and stable carbon isotopes. Likewise, 16S ribosomal rRNA, dsrAB (dissimilatory sulfite reductase) and mcrA (methyl coenzyme M reductase) mRNA transcripts of sulfate-reducing bacteria (Desulfobacteraceae and Desulfobulbaceae) and methane-cycling archaea (ANME-1 and ANME-2) were prevalent at the sediment surface under the mat and at its edge. Outside the mat at the surface, 16S rRNA sequences indicated mostly aerobes commonly found in seawater. The seep-related communities persisted at 12–20 cm depth inside and outside the mat. 16S rRNA transcripts and V6-tags reveal that bacterial and archaeal diversity underneath the mat are similar to each other, in contrast to oxic or microoxic habitats that have higher bacterial diversity. Conclusions/Significance The visual patchiness of microbial mats reflects sharp discontinuities in microbial community structure and activity over sub-meter spatial scales; these discontinuities have to be taken into account in geochemical and microbiological inventories of seep environments. In contrast, 12–20 cm deep in the sediments microbial communities performing methane-cycling and sulfate reduction persist at lower metabolic rates regardless of mat cover, and may increase activity rapidly when subsurface flow changes. PMID:20090951
Effect of magnetite powder on anaerobic co-digestion of pig manure and wheat straw.
Wang, Yanzi; Ren, Guangxin; Zhang, Tong; Zou, Shuzhen; Mao, Chunlan; Wang, Xiaojiao
2017-08-01
This study investigated the effects of different amounts of magnetite powder (i.e., 0g, 1.5g, 3g, 4.5g, 6g) on the anaerobic co-digestion of pig manure (PM) and wheat straw (WS). The variations in pH, alkalinity, cellulase activity (CEA), dehydrogenase activity (DHA) and methane production, were analyzed by phases. Correlation of the activities of the two enzymes with methane production was also analyzed, and the Gompertz model was used to evaluate the efficiency of anaerobic digestion (AD) with the addition of magnetite powder. The results showed that magnetite powder had significant effects on the anaerobic co-digestion of PM and WS. The maximum total methane production with the addition of 3g of magnetite powder was 195mL/g total solids (TS), an increase of 72.1%. The CEA and DHA increased with magnetite powder in the ranges of 1.5-4.5g, 1.5-6g, respectively, while the methane production showed a better correlation with DHA than with CEA. Using the Gompertz model, the efficiency of AD was optimal when adding 3g magnetite powder, with higher methane production potential (206mL/g TS), shorter lag-phase time (14.9d) and shorter AD period (44d). Copyright © 2017 Elsevier Ltd. All rights reserved.
Effect of humic acid in leachate on specific methanogenic activity of anaerobic granular sludge.
Guo, Mengfei; Xian, Ping; Yang, Longhui; Liu, Xi; Zhan, Longhui; Bu, Guanghui
2015-01-01
In order to find out the effects of humic acid (HA) in anaerobic-treated landfill leachate on granular sludge, the anaerobic biodegradability of HA as well as the influences of HA on the total cumulative methane production, the anaerobic methanization process and the specific methanogenic activity (SMA) of granular sludge are studied in this paper. Experimental results show that as a non-biodegradable organic pollutant, HA is also difficult to be decomposed by microbes in the anaerobic reaction process. Presence of HA and changes in the concentration have no significant influences on the total cumulative methane production and the anaerobic methanization process of granular sludge. Besides, the total cumulative methane production cannot reflect the inhibition of toxics on the methanogenic activity of granular sludge on the premise of sufficient reaction time. Results also show that HA plays a promoting role on SMA of granular sludge. Without buffering agent the SMA value increased by 19.2% on average due to the buffering and regulating ability of HA, while with buffering agent the SMA value increased by 5.4% on average due to the retaining effect of HA on the morphology of the sludge particles. However, in the presence of leachate the SMA value decreased by 27.6% on average, because the toxic effect of the toxics in the leachate on granular sludge is much larger than the promoting effect of HA.
NASA Astrophysics Data System (ADS)
Oi, T.; Akiba, F.; Matsumoto, R.; Kakuwa, Y.
2016-12-01
Gas hydrates were collected at several sites off Joetsu which presented anomalous seismic structures. "Gas chimneys", major host structures for shallow gas hydrates, were recognized ROV off Joetsu in eastern margin of the Japan Sea, as were a number of active methane seeps. The assemblage components and carbon isotope of benthic foraminifera, which are ubiquitous in global marine settings, can indicate methane seep environments (Akimoto et al., 1994; Bhaumik and Gupta, 2007). Preliminary work by Oi et al. (2015) documented the obvious occurrences of methane related foraminifera, Rutherfordoides sp., in three core sediments recovered from Umitaka Spur, west Oki Trough and north Mogami Trough in the eastern margin of the Japan Sea, and found them to comprise the early part of the MIS 2, calculated to 28-25ka. These records suggest that active methane seep events might occur at the same time during early MIS 2, but were confined within the last 100ka. In this study, we analyzed benthic foraminiferal fossils from drilling core J04RB (core length 122 m; one of the gas hydrate bearing sites at a southern part of the Joetsu Knoll) in order to document methane seep events during the last 500ka. Firstly, we estimated sedimentation ages from diatom biostratigraphy and identification of Aso-1 tephra. Based on diatom components, we recognized a boundary between NPD (Neogene North Pacific diatom Zonations) 12 and NPD11, estimated at 300 ka (MIS8/9; Yanagisawa and Akiba, 1998). The bottom age was estimated to almost 530-560 ka (around MIS14) especially from the alternation with warm and cold diatom zones (Akiba et al., 2014). Secondary, we could suppose the paleoenvironments from benthic foraminifera as below. 1. The rare benthic foraminifera during the cold stages (MIS8, MIS10, and MIS12) indicate anoxic bottom conditions characteristic of falling sea level, just as with MIS 2. 2. We recognized the continuous distributions of tiny methane related specimens of Rutherfordoides sp. during MIS10. In order to confirm new records of active methane seep events in the Joetsu Knoll, we need to measure isotope records of this species. This study was conducted under the commission from AIST as a part of the methane hydrate research project of METI (the Ministry of Economy, Trade and Industry, Japan).
Jensen, Michael P; Wick, Douglas D; Reinartz, Stefan; White, Peter S; Templeton, Joseph L; Goldberg, Karen I
2003-07-16
Reductive elimination of methane occurs upon solution thermolysis of kappa(3)-Tp(Me)2Pt(IV)(CH(3))(2)H (1, Tp(Me)2 = hydridotris(3,5-dimethylpyrazolyl)borate). The platinum product of this reaction is determined by the solvent. C-D bond activation occurs after methane elimination in benzene-d(6), to yield kappa(3)-Tp(Me)2Pt(IV)(CH(3))(C(6)D(5))D (2-d(6)), which undergoes a second reductive elimination/oxidative addition reaction to yield isotopically labeled methane and kappa(3)-Tp(Me)2Pt(IV)(C(6)D(5))(2)D (3-d(11)). In contrast, kappa(2)-Tp(Me)2Pt(II)(CH(3))(NCCD(3)) (4) was obtained in the presence of acetonitrile-d(3), after elimination of methane from 1. Reductive elimination of methane from these Pt(IV) complexes follows first-order kinetics, and the observed reaction rates are nearly independent of solvent. Virtually identical activation parameters (DeltaH(++)(obs) = 35.0 +/- 1.1 kcal/mol, DeltaS(++)(obs) = 13 +/- 3 eu) were measured for the reductive elimination of methane from 1 in both benzene-d(6) and toluene-d(8). A lower energy process (DeltaH(++)(scr) = 26 +/- 1 kcal/mol, DeltaS(++)(scr) = 1 +/- 4 eu) scrambles hydrogen atoms of 1 between the methyl and hydride positions, as confirmed by monitoring the equilibration of kappa(3)-Tp(Me)()2Pt(IV)(CH(3))(2)D (1-d(1)()) with its scrambled isotopomer, kappa(3)-Tp(Me)2Pt(IV)(CH(3))(CH(2)D)H (1-d(1'). The sigma-methane complex kappa(2)-Tp(Me)2Pt(II)(CH(3))(CH(4)) is proposed as a common intermediate in both the scrambling and reductive elimination processes. Kinetic results are consistent with rate-determining dissociative loss of methane from this intermediate to produce the coordinatively unsaturated intermediate [Tp(Me)2Pt(II)(CH(3))], which reacts rapidly with solvent. The difference in activation enthalpies for the H/D scrambling and C-H reductive elimination provides a lower limit for the binding enthalpy of methane to [Tp(Me)2Pt(II)(CH(3))] of 9 +/- 2 kcal/mol.
Methanotrophs and Methanogens in Masonry
Kussmaul, Martin; Wilimzig, Markus; Bock, Eberhard
1998-01-01
Methanotrophs were present in 48 of 225 stone samples which were removed from 19 historical buildings in Germany and Italy. The average cell number of methanotrophs was 20 CFU per g of stone, and their activities ranged between 11 and 42 pmol of CH4 g of stone−1 day−1. Twelve strains of methane-oxidizing bacteria were isolated. They belonged to the type II methanotrophs of the genera Methylocystis, Methylosinus, and Methylobacterium. In masonry, growth substrates like methane or methanol are available in very low concentrations. To determine if methane could be produced by the stone at rates sufficient to support growth of methanotrophs, methane production by stone samples under nonoxic conditions was examined. Methane production of 0.07 to 215 nmol of CH4 g of stone−1 day−1 was detected in 23 of 47 stone samples examined. This indicated the presence of the so-called “mini-methane”-producing bacteria and/or methanogenic archaea. Methanotrophs occurred in nearly all samples which showed methane production. This finding indicated that methanotrophs depend on biogenic methane production in or on stone surfaces of historical buildings. PMID:9797318
Biologically derived fertilizer: A multifaceted bio-tool in methane mitigation.
Singh, Jay Shankar; Strong, P J
2016-02-01
Methane emissions are affected by agricultural practices. Agriculture has increased in scale and intensity because of greater food, feed and energy demands. The application of chemical fertilizers in agriculture, particularly in paddy fields, has contributed to increased atmospheric methane emissions. Using organic fertilizers may improve crop yields and the methane sink potential within agricultural systems, which may be further improved when combined with beneficial microbes (i.e. biofertilizers) that improve the activity of methane oxidizing bacteria such as methanotrophs. Biofertilizers may be an effective tool for agriculture that is environmentally beneficial compared to conventional inorganic fertilizers. This review highlights and discusses the interplay between ammonia and methane oxidizing bacteria, the potential interactions of microbial communities with microbially-enriched organic amendments and the possible role of these biofertilizers in augmenting the methane sink potential of soils. It is suggested that biofertilizer applications should not only be investigated in terms of sustainable agriculture productivity and environmental management, but also in terms of their effects on methanogen and methanotroph populations. Copyright © 2015 Elsevier Inc. All rights reserved.
NASA Astrophysics Data System (ADS)
Davies, A. G.; Sotin, C.; Choukroun, M.; Matson, D. L.; Johnson, T. V.
2013-09-01
As previously noted [1-3], Titan may have an upper crust rich in methane clathrates which would have formed early in Titan's history [2, 3]. With an estimated mass of ~2 x 1017 kg, methane is a major component of Titan's atmosphere. The abundance of methane, which photo-dissociates under the influence of solar UV, and the presence of 40Ar require replenishment of these atmospheric components over geologic timescales. One possibility is that volcanic processes release these gases from Titan's interior, although so far there is no conclusive evidence of ongoing volcanic activity: no "smoking gun" has been observed. Still, some process has recently supplied a considerable amount of methane to Titan's atmosphere. We have been investigating the emplacement of proposed "cryolavas" of varying composition to, firstly, examine how such a volcanic process behaves thermally in order to determine event detectability via remote sensing, and, secondly, to model the penetration of the thermal wave into a methane-rich substrate. Destabilisation of clathrates would release methane into the atmosphere and liberate trapped argon.
Biogasification of Walt Disney World biomass waste blend. Annual report, January-December 1983
DOE Office of Scientific and Technical Information (OSTI.GOV)
Biljetina, R.; Chynoweth, D.P.; Janulis, J.
1984-09-01
The objective of this research is to develop efficient processes for conversion of biomass-waste blends to methane and other resources. To evaluate the technical and economic feasibility, an experimental test unit (ETU) was designed and installed at the Reedy Creek Wastewater Treatment Plant at Walt Disney World in Lake Buena Vista, Florida. The facility integrates a biomethanogenic conversion process with a wastewater treatment process employing water hyacinth ponds for secondary and tertiary treatment of sewage. Harvested water hyacinth is subsequently combined with sludge from the primary wastewater clarifier and fed at 1-wet-ton per day to the ETU digester. This resultsmore » in the production of methane and other useful byproducts. Design, procurement of equipment, and installation has been completed. Start-up of the ETU is in progress.« less
Mahyuddin, M Haris; Shiota, Yoshihito; Staykov, Aleksandar; Yoshizawa, Kazunari
2017-09-05
While the most likely structure of the active site in iron-containing zeolites has been recently identified as [FeO] 2+ (Snyder et al. Nature 2016, 536, 317-321), the mechanism for the direct conversion of methane to methanol over this active species is still debatable between the direct-radical-rebound or nonradical (concerted) mechanism. Using density functional theory on periodic systems, we calculated the two reaction mechanisms over two d 4 isoelectronic systems, [FeO] 2+ and [MnO] + zeolites. We found that [FeO] 2+ zeolites favor the direct-radical-rebound mechanism with low CH 4 activation energies, while [MnO] + zeolites prefer the nonradical mechanism with higher CH 4 activation energies. These contrasts, despite their isoelectronic structures, are mainly due to the differences in the metal coordination number and O α (oxo) spin density. Moreover, molecular orbital analyses suggest that the zeolite steric hindrance further degrades the reactivity of [MnO] + zeolites toward methane. Two types of zeolite frameworks, i.e., medium-pore ZSM-5 (MFI framework) and small-pore SSZ-39 (AEI framework) zeolites, were evaluated, but no significant differences in the reactivity were found. The rate-determining reaction step is found to be methanol desorption instead of methane activation. Careful examination of the most stable sites hosting the active species and calculation for N 2 O decomposition over [Fe] 2+ -MFI and -AEI zeolites were also performed.
Chu, Kung-Hui; Alvarez-Cohen, Lisa
1999-01-01
In this study we evaluated specific and nonspecific toxic effects of aeration and trichloroethylene (TCE) oxidation on methanotrophic bacteria grown with different nitrogen sources (nitrate, ammonia, and molecular nitrogen). The specific toxic effects, exerted directly on soluble methane monooxygenase (sMMO), were evaluated by comparing changes in methane uptake rates and naphthalene oxidation rates following aeration and/or TCE oxidation. Nonspecific toxic effects, defined as general cellular damage, were examined by using a combination of epifluorescent cellular stains to measure viable cell numbers based on respiratory activity and measuring formate oxidation activities following aeration and TCE transformation. Our results suggest that aeration damages predominantly sMMO rather than other general cellular components, whereas TCE oxidation exerts a broad range of toxic effects that damage both specific and nonspecific cellular functions. TCE oxidation caused sMMO-catalyzed activity and respiratory activity to decrease linearly with the amount of substrate degraded. Severe TCE oxidation toxicity resulted in total cessation of the methane, naphthalene, and formate oxidation activities and a 95% decrease in the respiratory activity of methanotrophs. The failure of cells to recover even after 7 days of incubation with methane suggests that cellular recovery following severe TCE product toxicity is not always possible. Our evidence suggests that generation of greater amounts of sMMO per cell due to nitrogen fixation may be responsible for enhanced TCE oxidation activities of nitrogen-fixing methanotrophs rather than enzymatic protection mechanisms associated with the nitrogenase enzymes. PMID:9925614
Limitations of microbial hydrocarbon degradation at the Amon Mud Volcano (Nile Deep Sea Fan)
NASA Astrophysics Data System (ADS)
Felden, J.; Lichtschlag, A.; Wenzhöfer, F.; de Beer, D.; Feseker, T.; Pop Ristova, P.; de Lange, G.; Boetius, A.
2013-01-01
The Amon mud volcano (MV), located at 1250 m water depth on the Nile Deep Sea Fan, is known for its active emission of methane and non-methane hydrocarbons into the hydrosphere. Previous investigations showed a low efficiency of hydrocarbon-degrading anaerobic microbial communities inhabiting the Amon MV center in the presence of sulphate and hydrocarbons in the seeping subsurface fluids. By comparing spatial and temporal patterns of in situ biogeochemical fluxes, temperature gradients, pore water composition and microbial activities over three years, we investigated why the activity of anaerobic hydrocarbon degraders can be low despite high energy supplies. We found that the central dome of the Amon MV, as well as a lateral mud flow at its base, showed signs of recent exposure of hot subsurface muds lacking active hydrocarbon degrading communities. In these highly disturbed areas, anaerobic degradation of methane was less than 2% of the methane flux. Rather high oxygen consumption rates compared to low sulphide production suggest a faster development of more rapidly growing aerobic hydrocarbon degraders in highly disturbed areas. In contrast, the more stabilized muds surrounding the central gas and fluid conduits hosted active anaerobic hydrocarbon-degrading microbial communities. Furthermore, within three years, cell numbers and hydrocarbon degrading activity increased at the gas-seeping sites. The low microbial activity in the hydrocarbon-vented areas of Amon mud volcano is thus a consequence of kinetic limitations by heat and mud expulsion, whereas most of the outer mud volcano area is limited by hydrocarbon transport.
Reactivation of Deep Subsurface Microbial Community in Response to Methane or Methanol Amendment
Rajala, Pauliina; Bomberg, Malin
2017-01-01
Microbial communities in deep subsurface environments comprise a large portion of Earth’s biomass, but the microbial activity in these habitats is largely unknown. Here, we studied how microorganisms from two isolated groundwater fractures at 180 and 500 m depths of the Outokumpu Deep Drillhole (Finland) responded to methane or methanol amendment, in the presence or absence of sulfate as an additional electron acceptor. Methane is a plausible intermediate in the deep subsurface carbon cycle, and electron acceptors such as sulfate are critical components for oxidation processes. In fact, the majority of the available carbon in the Outokumpu deep biosphere is present as methane. Methanol is an intermediate of methane oxidation, but may also be produced through degradation of organic matter. The fracture fluid samples were incubated in vitro with methane or methanol in the presence or absence of sulfate as electron acceptor. The metabolic response of microbial communities was measured by staining the microbial cells with fluorescent redox sensitive dye combined with flow cytometry, and DNA or cDNA-derived amplicon sequencing. The microbial community of the fracture zone at the 180 m depth was originally considerably more respiratory active and 10-fold more numerous (105 cells ml-1 at 180 m depth and 104 cells ml-1 at 500 m depth) than the community of the fracture zone at the 500 m. However, the dormant microbial community at the 500 m depth rapidly reactivated their transcription and respiration systems in the presence of methane or methanol, whereas in the shallower fracture zone only a small sub-population was able to utilize the newly available carbon source. In addition, the composition of substrate activated microbial communities differed at both depths from original microbial communities. The results demonstrate that OTUs representing minor groups of the total microbial communities play an important role when microbial communities face changes in environmental conditions. PMID:28367144
SPaMOB eat atmospheric methane in Antarctica
NASA Astrophysics Data System (ADS)
Lau, C. Y. M.; Edwards, C. R.; Onstott, T. C.
2016-12-01
The diverse and endemic soil microorganisms that have adapted to the hostile environments in Antarctica are facing challenges due to climate change. The seasonally thawed active layer would exhibit greater daily and/or seasonal temperature variations and different soil moisture regimes, which would cause compositional shifts in these microbial communities. Our preliminary data reveal that Antarctic cryosols from the Taylor Dry Valley are capable of oxidizing methane at atmospheric concentration ( 2 ppmv) at significantly higher rates than the acidic mineral cryosols from the Canadian High Arctic (N 79°) [The ISME J (2015) 9: 1880-1891]. Understanding of this understudied behavior for these active layer cryosols is important for determining the potential methane feedback responses in the Antarctic region. We therefore investigate the biodiversity and genome-wide adaptation of the responsible Southern Polar atmospheric methane-oxidizing bacteria (SPaMOB) in these cryosols. Methane consumption at atmospheric concentration at 4 and 10°C was monitored over a period of four weeks. Two cryosol samples that oxidized methane at both temperatures were selected for molecular analyses. PCR-cloning and sequencing of pmoA (particulate methane monooxygenase beta subunit), the marker gene of methane oxidation, revealed that the SPaMOB in alkaline Antarctic cryosols are closely related to Upland Soil Cluster γ (USCγ), whereas the high Canadian Arctic cryosols contain predominantly USCa-like phylotypes. Four metagenomic libraries were prepared from total DNA and sequenced (2x100bp, Illumina). Quality-filtered reads (avg. 20 M reads per library) were de novo assembled and annotated. A 42.8 kb-long contig containing the pmoCBAcluster was successfully assembled. The pmoA gene is closely related to our USCγ clone sequences. In addition to pmo genes, the presence of genes for conversion of methanol to formaldehyde, production of formate and eventually CO2 indicates SPaMOB's ability of complete methane oxidation. Carbon assimilation pathway is suggested by the presence of genes involved in serine synthesis, serine cycle and tricarboxylic acid cycle. This study provides the first genetic basis for a possible role of Antarctica as a current and future methane sink.
NASA Astrophysics Data System (ADS)
Li, Jiwei; Peng, Xiaotong; Bai, Shijie; Chen, Zhiyan; Van Nostrand, Joy D.
2018-02-01
Authigenic carbonates are one type of conspicuous manifestation in seep environments that can provide long-term archives of past seepage activity and methane cycling in the oceans. Comprehensive investigations of the microbial community functional structure and their roles in the process of carbonate formation are, however, lacking. In this study, the mineralogical, geochemical, and microbial functional composition were examined in seep carbonate deposits collected from the west slope of the northern section of the Okinawa Trough (OT). The aim of this work was to explore the correspondence between the mineralogical phases and microbial metabolism during carbonate deposit formation. The mineralogical analyses indicated that authigenic carbonate minerals (aragonite, magnesium-rich calcite, dolomite, ankerite and siderite) and iron-bearing minerals (limonite, chlorite, and biotite) were present in these carbonate samples. The carbon and oxygen isotopic values of the carbonate samples varied between -51.1‰ to -4.7‰ and -4.8‰ to 3.7‰, respectively. A negative linear correlation between carbon and oxygen isotopic compositions was found, indicating a mixture of methane-derived diagenetic (low δ13C/high 18O) carbonates and detrital origin (high δ13C/low 18O) carbonates at the OT. GeoChip analyses suggested that various metabolic activities of microorganisms, including methanogenesis, methane oxidation, sulfite oxidation, sulfate reduction, and metal biotransformations, all occurred during the formation process. On the basis of these findings, the following model for the methane cycle and seep carbonate deposit formation in the sediment column at the OT is proposed: (1) in the upper oxidizing zone, aerobic methane oxidation was the main way of methane consumption; (2) in the sulfate methane transition zone, sulfate-dependent AOM (anaerobic oxidation of methane) consumes methane, and authigenic minerals such as aragonite, magnesium-calcite, and sulfide minerals precipitate; (3) in the underlying sulfate depleted zone, the presence of iron-oxides supplied by hydrothermal fluids and terrestrial inputs created thermodynamically favorable conditions for Fe-dependent AOM to consume methane, and dolomite and siderite/ankerite precipitate in this zone.
Methyl-sulfonyl-methane (MSM)-induced acute angle closure.
Hwang, Jeremy C; Khine, Kay T; Lee, Jennifer C; Boyer, David S; Francis, Brian A
2015-01-01
To report the first case of presumed bilateral acute angle closure (AAC) secondary to ingestion of the dietary supplement, methyl-sulfonyl-methane (MSM). A 35-year-old woman presented with bilateral AAC 1 week after starting multiple dietary supplements, one of which contained MSM. Ultrasound biomicroscopy demonstrated bilateral anterior rotation of the iris-lens diaphragm, ciliary body edema, and choroidal effusion. Four days after discontinuation of the supplements, her angle closure and uveal effusion resolved, and her best-corrected vision recovered to 20/20 bilaterally. Sulfa-based drugs have been reported to cause AAC, choroidal effusion, and ciliary body edema. In our patient, the coincidence of bilateral AAC with choroidal and ciliary body effusion that began 1 week after starting dietary supplements was suspicious for drug-induced AAC. The dietary supplement Basic Detox Nutrients contains MSM, the only constituent in the patient's medication list with a sulfonyl moiety. Given the similarities in chemical structure and clinical presentation, we postulate that MSM induces AAC in a manner similar to mechanisms previously described for other sulfa-based drugs. As MSM continues to be used and studied for its anti-inflammatory and antioxidative properties, investigators and marketers will need to be cognizant of its potential to cause AAC and provide proper warning to consumers.
Li, Yangyang; Jin, Yiying; Borrion, Aiduan; Li, Jinhui
2018-03-01
Information on the anaerobic digestion (AD) of food waste (FW) with different waste cooking oil contents is limited in terms of the effect of the initial substrate concentrations. In this work, batch tests were performed to evaluate the combined effects of waste cooking oil content (33-53%) and feed/inoculum (F/I) ratios (0.5-1.2) on biogas/methane yield, process stability parameters and organics reduction during the FW AD. Both waste cooking oil and the inoculation ratios were found to affect digestion parameters during the AD process start-up and the F/I ratio was the predominant factor affecting AD after the start-up phase. The possible inhibition due to acidification caused by volatile fatty acids accumulation, low pH values and long-chain fatty acids was reversible. The characteristics of the final digestate indicated a stable anaerobic system, whereas samples with F/I ratios ranging from 0.8 to 1.2 display higher propionic and valeric acid contents and high amounts of total ammonia nitrogen and free ammonia nitrogen. Overall, F/I ratios higher than 0.70 caused inhibition and resulted in low biogas/methane yields from the FW. Copyright © 2018 Elsevier Ltd. All rights reserved.
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 13C-depleted isotopic signatures of dissolved inorganic carbon. The anaerobic conversion of methane to CO2 was confirmed in a 13C-labeling experiment. Methane fueled a vital microbial community with cell numbers of up to 4 × 109 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. PMID:22207865
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.
Surface Protonics Promotes Catalysis
Manabe, R.; Okada, S.; Inagaki, R.; Oshima, K.; Ogo, S.; Sekine, Y.
2016-01-01
Catalytic steam reforming of methane for hydrogen production proceeds even at 473 K over 1 wt% Pd/CeO2 catalyst in an electric field, thanks to the surface protonics. Kinetic analyses demonstrated the synergetic effect between catalytic reaction and electric field, revealing strengthened water pressure dependence of the reaction rate when applying an electric field, with one-third the apparent activation energy at the lower reaction temperature range. Operando–IR measurements revealed that proton conduction via adsorbed water on the catalyst surface occurred during electric field application. Methane was activated by proton collision at the Pd–CeO2 interface, based on the inverse kinetic isotope effect. Proton conduction on the catalyst surface plays an important role in methane activation at low temperature. This report is the first describing promotion of the catalytic reaction by surface protonics. PMID:27905505
NASA Astrophysics Data System (ADS)
Lamarche-Gagnon, G.; Wadham, J.; Beaton, A.; Fietzek, P.; Stanley, K. M.; Tedstone, A.; Sherwood Lollar, B.; Lacrampe Couloume, G.; Telling, J.; Liz, B.; Hawkings, J.; Kohler, T. J.; Zarsky, J. D.; Stibal, M.; Mowlem, M. C.
2016-12-01
Both past and present ice sheets have been proposed to cap large quantities of methane (CH4), on orders of magnitude significant enough to impact global greenhouse gas concentrations during periods of rapid ice retreat. However, to date most evidence for sub-ice sheet methane has been indirect, derived from calculations of the methanogenic potential of basal-ice microbial communities and biogeochemical models; field-based empirical measurements are lacking from large ice sheet catchments. Here, we present the first continuous, in situ record of dissolved methane export from a large catchment of the Greenland Ice Sheet (GrIS) in South West Greenland from May-July 2015. Our results indicate that glacial runoff was continuously supersaturated with methane over the observation period (dissolved CH4 concentrations of 30-700 nM), with total methane flux rising as subglacial discharge increased. Periodic subglacial drainage events, characterised by rapid changes (i.e. pulses) in meltwater hydrochemistry, also coincided with a rise in methane concentrations. We argue that these are likely indicative of the flushing of subglacial reservoirs of CH4 beneath the ice sheet. Total methane export was relatively modest when compared to global methane budgets, but too high to be explained by previously determined methanogenic rates from Greenland basal ice. Discrepancies between estimated Greenland methane reserves and observed fluxes stress the need to further investigate GrIS methane fluxes and sources, and suggest a more biogeochemically active subglacial environment than previously considered. Results indicate that future warming, and a coincident increase in ice melt rates, would likely make the GrIS, and by extension the Antarctic Ice Sheet, more significant sources of atmospheric methane, consequently acting as a positive feedback to a warming climate.
Wireless device for activation of an underground shock wave absorber
NASA Astrophysics Data System (ADS)
Chikhradze, M.; Akhvlediani, I.; Bochorishvili, N.; Mataradze, E.
2011-10-01
The paper describes the mechanism and design of the wireless device for activation of energy absorber for localization of blast energy in underground openings. The statistics shows that the greatest share of accidents with fatal results associate with explosions in coal mines due to aero-methane and/or air-coal media explosion. The other significant problem is terrorist or accidental explosions in underground structures. At present there are different protective systems to reduce the blast energy. One of the main parts of protective Systems is blast Identification and Registration Module. The works conducted at G. Tsulukidze Mining Institute of Georgia enabled to construct the wireless system of explosion detection and mitigation of shock waves. The system is based on the constant control on overpressure. The experimental research continues to fulfill the system based on both threats, on the constant control on overpressure and flame parameters, especially in underground structures and coal mines. Reaching the threshold value of any of those parameters, the system immediately starts the activation. The absorber contains a pyrotechnic device ensuring the discharge of dispersed water. The operational parameters of wireless device and activation mechanisms of pyrotechnic element of shock wave absorber are discussed in the paper.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Barnhart, Elliott P.; Davis, Katherine J.; Varonka, Matthew
Many coal beds contain microbial communities that can convert coal to natural gas (coalbed methane). Native microorganisms were obtained from Powder River Basin (PRB) coal seams with a diffusive microbial sampler placed downhole and used as an inoculum for enrichments with different nutrients to investigate microbially-enhanced coalbed methane production (MECoM). Coal-dependent methanogenesis more than doubled when yeast extract (YE) and several less complex components (proteins and amino acids) were added to the laboratory microcosms. Stimulated coal-dependent methanogenesis with peptone was 86% of that with YE while glutamate-stimulated activity was 65% of that with YE, and a vitamin mix had onlymore » 33% of the YE stimulated activity. For field application of MECoM, there is interest in identifying cost-effective alternatives to YE and other expensive nutrients. In laboratory studies, adding algal extract (AE) with lipids removed stimulated coal-dependent methanogenesis and the activity was 60% of that with YE at 27 d and almost 90% of YE activity at 1406 d. Analysis of British Thermal Unit (BTU) content of coal (a measure of potential energy yield) from long-term incubations indicated > 99.5% of BTU content remained after coalbed methane (CBM) stimulation with either AE or YE. Thus, the coal resource remains largely unchanged following stimulated microbial methane production. Algal CBM stimulation could lead to technologies that utilize coupled biological systems (photosynthesis and methane production) that sustainably enhance CBM production and generate algal biofuels while also sequestering carbon dioxide (CO 2).« less
Barnhart, Elliott P.; Davis, Katherine J.; Varonka, Matthew; ...
2017-01-05
Many coal beds contain microbial communities that can convert coal to natural gas (coalbed methane). Native microorganisms were obtained from Powder River Basin (PRB) coal seams with a diffusive microbial sampler placed downhole and used as an inoculum for enrichments with different nutrients to investigate microbially-enhanced coalbed methane production (MECoM). Coal-dependent methanogenesis more than doubled when yeast extract (YE) and several less complex components (proteins and amino acids) were added to the laboratory microcosms. Stimulated coal-dependent methanogenesis with peptone was 86% of that with YE while glutamate-stimulated activity was 65% of that with YE, and a vitamin mix had onlymore » 33% of the YE stimulated activity. For field application of MECoM, there is interest in identifying cost-effective alternatives to YE and other expensive nutrients. In laboratory studies, adding algal extract (AE) with lipids removed stimulated coal-dependent methanogenesis and the activity was 60% of that with YE at 27 d and almost 90% of YE activity at 1406 d. Analysis of British Thermal Unit (BTU) content of coal (a measure of potential energy yield) from long-term incubations indicated > 99.5% of BTU content remained after coalbed methane (CBM) stimulation with either AE or YE. Thus, the coal resource remains largely unchanged following stimulated microbial methane production. Algal CBM stimulation could lead to technologies that utilize coupled biological systems (photosynthesis and methane production) that sustainably enhance CBM production and generate algal biofuels while also sequestering carbon dioxide (CO 2).« less
Microbial production and oxidation of methane in deep subsurface
NASA Astrophysics Data System (ADS)
Kotelnikova, Svetlana
2002-10-01
The goal of this review is to summarize present studies on microbial production and oxidation of methane in the deep subterranean environments. Methane is a long-living gas causing the "greenhouse" effect in the planet's atmosphere. Earlier, the deep "organic carbon poor" subsurface was not considered as a source of "biogenic" methane. Evidence of active methanogenesis and presence of viable methanogens including autotrophic organisms were obtained for some subsurface environments including water-flooded oil-fields, deep sandy aquifers, deep sea hydrothermal vents, the deep sediments and granitic groundwater at depths of 10 to 2000 m below sea level. As a rule, the deep subterranean microbial populations dwell at more or less oligotrophic conditions. Molecular hydrogen has been found in a variety of subsurface environments, where its concentrations were significantly higher than in the tested surface aquatic environments. Chemolithoautotrophic microorganisms from deep aquifers that could grow on hydrogen and carbon dioxide can act as primary producers of organic carbon, initiating heterotrophic food chains in the deep subterranean environments independent of photosynthesis. "Biogenic" methane has been found all over the world. On the basis of documented occurrences, gases in reservoirs and older sediments are similar and have the isotopic character of methane derived from CO 2 reduction. Groundwater representing the methanogenic end member are characterized by a relative depletion of dissolved organic carbon (DOC) in combination with an enrichment in 13C in inorganic carbon, which is consistent with the preferential reduction of 12CO 2 by autotrophic methanogens or acetogens. The isotopic composition of methane formed via CO 2 reduction is controlled by the δ13C of the original CO 2 substrate. Literature data shows that CH 4 as heavy as -40‰ or -50‰ can be produced by the microbial reduction of isotopically heavy CO 2. Produced methane may be oxidized microbially to carbon dioxide. Microbial methane oxidation is a biogeochemical process that limits the release of methane, a greenhouse gas from anaerobic environments. Anaerobic methane oxidation plays an important role in marine sediments. Similar processes may take place in deep subsurface and thus fuel the deep microbial community. Organisms or consortia responsible for anaerobic methane oxidation have not yet been cultured, although diverse aerobic methanotrophs have been isolated from a variety of underground niches. The presence of aerobic methanotrophs in the anoxic subsurface remains to be explained. The presence of methane in the deep subsurface have been shown all over the world. The flux of gases between the deep subsurface and the atmosphere is driven by the concentration gradient from depth to the atmosphere. However, methane is consumed by methanotrophs on the way of its evolution in oxidized environments and is transformed to organic form, available for further microbial processing. When the impact of subsurface environments to global warming is estimated, it is necessary to take into account the activity of methane-producing Archaea and methane-oxidizing biofilters in groundwater. Microbial production and oxidation of methane is involved in the carbon cycle in the deep subsurface environments.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Wilmer, CE; Farha, OK; Yildirim, T
We have synthesized and characterized a new metal-organic framework (MOF) material, NU-125, that, in the single-crystal limit, achieves a methane storage density at 58 bar (840 psi) and 298 K corresponding to 86% of that obtained with compressed natural gas tanks (CNG) used in vehicles today, when the latter are pressurized to 248 bar (3600 psi). More importantly, the deliverable capacity (58 bar to 5.8 bar) for NU-125 is 67% of the deliverable capacity of a CNG tank that starts at 248 bar. (For crystalline granules or powders, particle packing inefficiencies will yield densities and deliverable capacities lower than 86%more » and 67% of high-pressure CNG.) This material was synthesized in high yield on a gram-scale in a single-batch synthesis. Methane adsorption isotherms were measured over a wide pressure range (0.1-58 bar) and repeated over twelve cycles on the same sample, which showed no detectable degradation. Adsorption of CO2 and H-2 over a broad range of pressures and temperatures are also reported and agree with our computational findings.« less
Albertson, John D; Harvey, Tierney; Foderaro, Greg; Zhu, Pingping; Zhou, Xiaochi; Ferrari, Silvia; Amin, M Shahrooz; Modrak, Mark; Brantley, Halley; Thoma, Eben D
2016-03-01
This paper addresses the need for surveillance of fugitive methane emissions over broad geographical regions. Most existing techniques suffer from being either extensive (but qualitative) or quantitative (but intensive with poor scalability). A total of two novel advancements are made here. First, a recursive Bayesian method is presented for probabilistically characterizing fugitive point-sources from mobile sensor data. This approach is made possible by a new cross-plume integrated dispersion formulation that overcomes much of the need for time-averaging concentration data. The method is tested here against a limited data set of controlled methane release and shown to perform well. We then present an information-theoretic approach to plan the paths of the sensor-equipped vehicle, where the path is chosen so as to maximize expected reduction in integrated target source rate uncertainty in the region, subject to given starting and ending positions and prevailing meteorological conditions. The information-driven sensor path planning algorithm is tested and shown to provide robust results across a wide range of conditions. An overall system concept is presented for optionally piggybacking of these techniques onto normal industry maintenance operations using sensor-equipped work trucks.
Enhanced carbon monoxide utilization in methanation process
Elek, Louis F.; Frost, Albert C.
1984-01-01
Carbon monoxide - containing gas streams are passed over a catalyst to deposit a surface layer of active surface carbon thereon essentially without the formation of inactive coke. The active carbon is subsequently reacted with steam or hydrogen to form methane. Surprisingly, hydrogen and water vapor present in the feed gas do not adversely affect CO utilization significantly, and such hydrogen actually results in a significant increase in CO utilization.
Zhang, Yaobin; Feng, Yinghong; Quan, Xie
2015-04-01
Heat or alkali pretreatment is the effective method to improve hydrolysis of waste sludge and then enhance anaerobic sludge digestion. However the pretreatment may inactivate the methanogens in the sludge. In the present work, zero-valent iron (ZVI) was used to enhance the methanogenic activity in anaerobic sludge digester under two methanogens-suppressing conditions, i.e. heat-pretreatment and alkali condition respectively. With the addition of ZVI, the lag time of methane production was shortened, and the methane yield increased by 91.5% compared to the control group. The consumption of VFA was accelerated by ZVI, especially for acetate, indicating that the acetoclastic methanogenesis was enhanced. In the alkali-condition experiment, the hydrogen produced decreased from 27.6 to 18.8 mL when increasing the ZVI dosage from 0 to 10 g/L. Correspondingly, the methane yield increased from 1.9 to 32.2 mL, which meant that the H2-utilizing methanogenes was enriched. These results suggested that the addition of ZVI into anaerobic digestion of sludge after pretreated by the heat or alkali process could efficiently recover the methanogenic activity and increase the methane production and sludge reduction. Copyright © 2015 Elsevier Ltd. All rights reserved.
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 + .
Study of methanogenesis during bioutilization of plant residuals
NASA Astrophysics Data System (ADS)
Ilyin, V. K.; Korniushenkova, I. N.; Starkova, L. V.; Lauriniavichius, K. S.
2005-02-01
The waste management strategy for the future should meet the benefits of human safety, respect principles of planet ecology, and compatibility with other habitability systems. For these purposes waste management technologies relevant to application of the biodegradation properties of bacteria are of great value. Biological treatment method is based on the biodegradation of organic substances by various microorganisms. The objectives of our study were: to evaluate the effectiveness of microbial biodegradation of vegetable non-edible residual, using artificial inoculum, and to study the peculiarities of biogas, and possibilities of optimizing or reducing the share of methane. The diminution rate of organic gained 76% from initial mass within 9 days of fermentation. The biogas production achieved 46 l/kg of substrate. The microbial studies of biodegradation process revealed the following peculiarities: (i) gradual quantitative increase of Lactobacillus sp. (from 103 to 105 colony-forming units (CFU) per ml); (ii) activation of Clostridia sp. (from 102 to 10 4 CFU/ml); and (iii) elimination of aerobic conventional pathogens (Enterobacteriaceae, Protea sp., Staphylococci). Chromatography analysis revealed the constant presence of carbon dioxide (up to 90.9%). The methane content measures revealed traces 0.1-0.4%. However, when we optimized the methane production in "boiling layer" using methanogenic granules, the amount of methane in biogas reached 80-90%. Based on the results obtained the artificial inoculum was created which was capable of initiating biodegradation of vegetable wastes. This inoculum consisted of active sludge adapted to wastes mixed with excretea of insects which consume plant wastes. Using this inoculum the biodegradation process takes less time than that using active sludge. Regulation of methane concentration from traces to 90% may be achieved by adding methane reactor to the plant digester.
Lightning generation in Titan due to the electrical self-polarization properties of Methane
NASA Astrophysics Data System (ADS)
Quintero, A.; Falcón, N.
2009-05-01
We describe an electrical charge process in Titan's thunderclouds, due to the self-polarization properties or pyroelectricity of methane, which increases the internal electric field in thunderclouds and facilitates the charge generation and separation processes. Microphysics that generates lightning flashes is associated with the physical and chemical properties of the local atmosphere, so methane could be the principal agent of the electrical activity because of its great concentration in Titan's atmosphere. Besides, Titan's electrical activity should not be very influenced by Saturn's magnetosphere because lightning occurs at very low altitude above Titan's surface, compared with the greater distance of Saturn's magnetosphere and Titan's troposphere. Using an electrostatic treatment, we calculate the internal electric field of Titan's thunderclouds due to methane's pyroelectrical properties, 7.05×10^11 Vm^-1; and using the telluric capacitor approximation for thunderclouds, we calculate the total charge obtained for a typical Titan thundercloud, 2.67×10^9 C. However, it is not right to use an electrostatic treatment because charge times are very fast due to the large methane concentration in Titan's clouds and the life time of thunderclouds is very low (around 2 hours). We consider a time dependent mechanism, employing common Earth atmospheric approaches, because of the similitude in chemical composition of both atmospheres (mainly nitrogen), so the typical charge of a thundercloud in Titan should reach between 20 C to 40 C, like on Earth. We obtain that lightning occurs with a frequency between 2 and 6 KHz. In Titan's atmosphere, methane concentration is higher than on Earth, and atmospheric electrical activity is stronger, so this model could be consistent with the observed phenomenology.
NASA Astrophysics Data System (ADS)
Sonderfeld, Hannah; Boesch, Hartmut; Jeanjean, Antoine P. R.; Riddick, Stuart N.; Allen, Grant; Ars, Sebastien; Davies, Stewart; Harris, Neil; Humpage, Neil; Leigh, Roland; Pitt, Joseph
2017-04-01
Globally, the waste sector contributes to nearly a fifth of anthropogenic methane (CH4) emitted to the atmosphere and is the second largest source of methane in the UK. In recent years great improvements to reduce those emissions have been achieved by installation of methane recovery systems at landfill sites and subsequently methane emissions reported in national emission inventories have been reduced. Nevertheless, methane emissions of landfills remain uncertain and quantification of emission fluxes is essential to verify reported emission inventories and to monitor changes in emissions. We are presenting data from the deployment of an in situ FTIR (Fourier Transform Infrared Spectrometer, Ecotech) for continuous and simultaneous sampling of CO2, CH4, N2O and CO with high time resolution of the order of minutes. During a two week field campaign at an operational landfill site in Eastern England in August 2014, measurements were taken within a radius of 320 m of the uncovered and active area of the landfill, which was still filled with new incoming waste. We have applied a computation fluid dynamics (CFD) model, constrained with local wind measurements and a detailed topographic map of the landfill site, to the in situ concentration data to calculate CH4 fluxes of the active site. A mean daytime flux of 0.83 mg m-2 s-1 (53.26 kg h-1) was calculated for the area of the active site. An additional source area was identified and incorporated into the CFD model, which resulted in higher total methane emissions of 75.97 kg h-1 for the combined emission areas. Our method of combining a CFD model to in situ data, in medium proximity of the source area, allows to distinguish between different emission areas and thereby provide more detailed information compared to bulk emission approaches.
Marlow, Jeffery; Skennerton, Connor T.; Li, Zhou; ...
2016-04-29
Marine methane seep habitats represent an important control on the global flux of methane between the subsurface and water column reservoirs. Meta-omics studies have begun to outline community-wide metabolic potential, but expression patterns of proteins that enact sulfate-mediated anaerobic methane oxidation in seeps are poorly characterized. Proteomic stable isotope probing (proteomic SIP) offers an additional layer of information for characterizing phylogenetically specific, functionally relevant activity in mixed microbial communities. Here we applied proteomic SIP to 15NH4+ and CH4 amended seep sediment microcosms in an attempt to track the protein synthesis of slow-growing, low-energy microbial systems. Across all samples, 3495 proteinsmore » were identified, 21% of which were 15N-labeled. We observed active synthesis (15N enrichment) of all proteins believed to be involved in sulfate reduction and reverse methanogenesis including methylenetetrahydromethanopterin reductase (Mer). The abundance and phylogenetic range of methyl-coenzyme M reductase (Mcr) orthologs produced during incubation experiments suggests that seeps provide sufficient niches for multiple organisms performing analogous metabolisms. Twenty-eight previously unreported post-translational modifications of McrA were measured, indicating dynamic enzymatic machinery and offering a dimension of functional diversity beyond gene-dictated sequence. RNA polymerase associated with putative sulfur-oxidizing Epsilonproteobacteria and aerobic Gammaproteobacteria were more abundant among pre-incubation proteins, suggesting diminished metabolic activity in long-term anoxic, sulfidic experimental incubations. Twenty-six proteins of unknown function were detected in all proteomic experiments and actively expressed in labeled experiments, suggesting that they play important roles in methane seep ecosystems. The addition of stable isotope probing to environmental proteomics experiments provides a mechanism to begin to assess the degree to which diagnostic meatbolic proteins are long-lived or acively synthesized in complex, slow-growing microbial communities. Our work here demonstrates that sediment-hosted microbial assemblages in marine methane seeps are dynamic, heterogeneous systems with broad functional diversity.« less
Methane Ebullition During Simulated Lake Expansion and Permafrost Degradation
NASA Astrophysics Data System (ADS)
Mazéas, O.; von Fischer, J. C.; Whelan, M.; Rhew, R.
2007-12-01
Methane, a potent greenhouse gas, is emitted by Arctic tundra and lakes. Ebullition, or bubbling, of methane from Arctic lakes has been shown to be a major transport mechanism from the sediment to the atmosphere, and ebullition rates are greatest near the edges of the lakes where active erosion is occurring. In regions of continuous permafrost, Arctic lakes have been expanding in recent decades, attributed to permafrost melting and development of thermokarst. Lake expansion occurs when the margins erode into water, supplying large amounts of organic rich material to the sediment-water interface. This allows carbon that was previously stored in the soil (active layer and permafrost) to become bioavailable and subject to decomposition. An increase in Arctic methane emissions as a result of permafrost thawing and lake expansion would constitute a positive feedback to Arctic warming. In order to better understand these processes, an experiment was initiated in July 2007 at the Barrow Environmental Observatory, Barrow, AK. Different layers of locally collected tundra soil were placed into incubation chambers at the bottom of a shallow (about 1 m deep) lake. Each experimental chamber consists of a bucket fixed underneath an inverted funnel, with a sampling port on top to capture and collect the emitted gases. Gas samples are analyzed for methane and carbon dioxide concentrations, as well as relevant isotopic compositions. Gas sampling has occurred at frequent intervals during the late summer and will continue through the early winter. Three replicates of each layer (active layer, seasonally frozen active layer and permafrost) were incubated, as well as an empty control chamber. An additional chamber containing thawed permafrost and cellulose-rich sawdust was placed for comparison, as cellulose is a major component of plant tissue and the fermentation of the cellulose should yield substrates for methanogenesis. Total production of methane versus organic carbon content of initial sample, kinetics of ebullition, and relative potential emissions from each tundra layer will be assessed.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Marlow, Jeffery; Skennerton, Connor T.; Li, Zhou
Marine methane seep habitats represent an important control on the global flux of methane between the subsurface and water column reservoirs. Meta-omics studies have begun to outline community-wide metabolic potential, but expression patterns of proteins that enact sulfate-mediated anaerobic methane oxidation in seeps are poorly characterized. Proteomic stable isotope probing (proteomic SIP) offers an additional layer of information for characterizing phylogenetically specific, functionally relevant activity in mixed microbial communities. Here we applied proteomic SIP to 15NH4+ and CH4 amended seep sediment microcosms in an attempt to track the protein synthesis of slow-growing, low-energy microbial systems. Across all samples, 3495 proteinsmore » were identified, 21% of which were 15N-labeled. We observed active synthesis (15N enrichment) of all proteins believed to be involved in sulfate reduction and reverse methanogenesis including methylenetetrahydromethanopterin reductase (Mer). The abundance and phylogenetic range of methyl-coenzyme M reductase (Mcr) orthologs produced during incubation experiments suggests that seeps provide sufficient niches for multiple organisms performing analogous metabolisms. Twenty-eight previously unreported post-translational modifications of McrA were measured, indicating dynamic enzymatic machinery and offering a dimension of functional diversity beyond gene-dictated sequence. RNA polymerase associated with putative sulfur-oxidizing Epsilonproteobacteria and aerobic Gammaproteobacteria were more abundant among pre-incubation proteins, suggesting diminished metabolic activity in long-term anoxic, sulfidic experimental incubations. Twenty-six proteins of unknown function were detected in all proteomic experiments and actively expressed in labeled experiments, suggesting that they play important roles in methane seep ecosystems. The addition of stable isotope probing to environmental proteomics experiments provides a mechanism to begin to assess the degree to which diagnostic meatbolic proteins are long-lived or acively synthesized in complex, slow-growing microbial communities. Our work here demonstrates that sediment-hosted microbial assemblages in marine methane seeps are dynamic, heterogeneous systems with broad functional diversity.« less
H2S-mediated thermal and photochemical methane activation.
Baltrusaitis, Jonas; de Graaf, Coen; Broer, Ria; Patterson, Eric V
2013-12-02
Sustainable, low-temperature methods for natural gas activation are critical in addressing current and foreseeable energy and hydrocarbon feedstock needs. Large portions of natural gas resources are still too expensive to process due to their high content of hydrogen sulfide gas (H2S) mixed with methane, deemed altogether as sub-quality or "sour" gas. We propose a unique method of activation to form a mixture of sulfur-containing hydrocarbon intermediates, CH3SH and CH3SCH3 , and an energy carrier such as H2. For this purpose, we investigated the H2S-mediated methane activation to form a reactive CH3SH species by means of direct photolysis of sub-quality natural gas. Photoexcitation of hydrogen sulfide in the CH4 + H2S complex resulted in a barrierless relaxation by a conical intersection to form a ground-state CH3SH + H2 complex. The resulting CH3SH could further be coupled over acidic catalysts to form higher hydrocarbons, and the resulting H2 used as a fuel. This process is very different from conventional thermal or radical-based processes and can be driven photolytically at low temperatures, with enhanced control over the conditions currently used in industrial oxidative natural gas activation. Finally, the proposed process is CO2 neutral, as opposed to the current industrial steam methane reforming (SMR). Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
NASA Astrophysics Data System (ADS)
Baker, A. K.; Rauthe-Schöch, A.; Schuck, T. J.; van Velthoven, P. F.; Slemr, F.; Brenninkmeijer, C. A.
2010-12-01
A large fraction of methane sources are anthropogenic, and include fossil fuel use, biomass/biofuel burning, agriculture and waste treatment. Recently, much attention regarding emissions of greenhouse gases has focused on large, developing nations, as their emissions are expected to rise rapidly over the coming decades. As the second most populous country in the world, and one of the fastest growing economies, India has been of particular interest. Arguably the most important feature of meteorology in India is the Asian summer monsoon. During the monsoon period there exists persistent deep convection over Southern Asia, and the composition of convected air masses is strongly influenced by emissions from India. This ultimately results in a well-mixed air parcel containing air from India being transported to the upper troposphere. Over the course of the 2008 monsoon period the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) passenger aircraft conducted monthly measurement flights which probed this outflow. Data collected during these flights provides a unique opportunity to examine sources of atmospheric species in India. Here we use measurements of methane (CH4), carbon monoxide (CO) and ethane (C2H6) from whole air samples collected during CARIBIC flights to estimate emissions of methane and to quantify those emissions related to flooding during the monsoon. Methane data from the monsoon period show enhancements inside the monsoon plume, which increase as the monsoon progresses. Using emission data for CO and ΔCH4/ΔCO derived from CARIBIC measurements, we estimate total methane emissions to be ~40 Tg yr-1. Relationships of methane to ethane, which shares the bulk of its sources with methane but lacks a biological component, are further used to estimate the fraction of “extra” emissions from biological activity related to increased monsoon rains. This additional methane is a considerable fraction of total methane emissions. As emissions from rice paddies, which are not restricted to the monsoon season, are estimated to be 4±2 Tg yr-1, we expect that the additional methane emitted during the monsoon season is a product of anaerobic microbial activity related to persistent and widespread flooding during the monsoon, although the exact sources cannot be identified from our data.
Methane occurrence in groundwater of south-central New York State, 2012: summary of findings
Heisig, Paul M.; Scott, Tia-Marie
2013-01-01
A survey of methane in groundwater was undertaken to document methane occurrence on the basis of hydrogeologic setting within a glaciated 1,810-square-mile area of south-central New York that has not seen shale-gas resource development. The adjacent region in northeastern Pennsylvania has undergone shale-gas resource development from the Marcellus Shale. Well construction and subsurface data were required for each well sampled so that the local hydrogeologic setting could be classified. All wells were also at least 1 mile from any known gas well (active, exploratory, or abandoned). Sixty-six domestic wells and similar purposed supply wells were sampled during summer 2012. Field water-quality characteristics (pH, specific conductance, dissolved oxygen, and temperature) were measured at each well, and samples were collected and analyzed for dissolved gases, including methane and short-chain hydrocarbons. Carbon and hydrogen isotopic ratios of methane were measured in 21 samples that had at least 0.3 milligram per liter (mg/L) methane.
Lin, Qiang; De Vrieze, Jo; He, Guihua; Li, Xiangzhen; Li, Jiabao
2016-09-01
Temperature is crucial for the performance of anaerobic digestion process. In this study of anaerobic digestion of swine manure, the relationship between the microbial gene expression and methane production at different temperatures (25-55°C) was revealed through metatranscriptomic analysis. Daily methane production and total biogas production increased with temperature up to 50°C, but decreased at 55°C. The functional gene expression showed great variation at different temperatures. The function centralization (opposite to alpha-diversity), assessed by the least proportions of functional pathways contributing for at least 50% of total reads positively correlated to methane production. Temperature regulated methane production probably through reducing the diversity of functional pathways, but enhancing central functional pathways, so that most of cellular activities and resource were invested in methanogenesis and related pathways, enhancing the efficiency of conversion of substrates to methane. This research demonstrated the importance of function centralization for efficient system functioning. Copyright © 2016 Elsevier Ltd. All rights reserved.
Methanogenesis in oxygenated soils is a substantial fraction of wetland methane emissions
DOE Office of Scientific and Technical Information (OSTI.GOV)
Angle, Jordan C.; Morin, Timothy H.; Solden, Lindsey M.
The current paradigm, widely incorporated in soil biogeochemical models, is that microbial methanogenesis can only occur in anoxic habitats. In contrast, here we show clear geochemical and biological evidence for methane production in well-oxygenated soils of a freshwater wetland. A comparison of oxic to anoxic soils reveal up to ten times greater methane production and nine times more methanogenesis activity in oxygenated soils. Metagenomic and metatranscriptomic sequencing recover the first near-complete genomes for a novel methanogen species, and show acetoclastic production from this organism was the dominant methanogenesis pathway in oxygenated soils. This organism, Candidatus Methanothrix paradoxum, is prevalent acrossmore » methane emitting ecosystems, suggesting a global significance. Moreover, in this wetland, we estimate that up to 80% of methane fluxes could be attributed to methanogenesis in oxygenated soils. Together, our findings challenge a widely held assumption about methanogenesis, with significant ramifications for global methane estimates and Earth system modeling.« less
Methanogenesis in oxygenated soils is a substantial fraction of wetland methane emissions
DOE Office of Scientific and Technical Information (OSTI.GOV)
Angle, Jordan C.; Morin, Timothy H.; Solden, Lindsey M.
The current paradigm, widely incorporated in soil biogeochemical models, is that microbial methanogenesis can only occur in anoxic habitats1-4. In contrast, here porewater and greenhouse-gas flux measurements show clear evidence for methane production in well-oxygenated soils from a freshwater wetland. A comparison of oxic to anoxic soils revealed up to ten times greater methane production and nine times more methanogenesis activity in oxygenated soils. Metagenomic and metatranscriptomic sequencing recovered the first near complete genomes for a novel methanogen species, and showed acetoclastic production from this organism was the dominant methanogenesis pathway in oxygenated soils. This organism, Candidatus Methanosaeta oxydurans, ismore » prevalent across methane emitting ecosystems, suggesting a global significance. Moreover, in this wetland, we estimated that a dominant fraction of methane fluxes could be attributed to methanogenesis in oxygenated soils. Together our findings challenge a widely-held assumption about methanogenesis, with significant ramifications for global methane estimates and Earth system modeling.« less
QENS study of methane diffusion in Mo/H-ZSM-5 used for the methane dehydroaromatisation reaction
NASA Astrophysics Data System (ADS)
Silverwood, Ian P.; Arán, Miren Agote; González, Ines Lezcano; Kroner, Anna; Beale, Andrew M.
2018-05-01
There is commercial interest in understanding the deactivation of Mo loaded H-ZSM-5 catalyst by coke fouling during the methane dehydroaromatization reaction (MDA). The effect of coke on methane diffusion inside the zeolite pores was studied by quasielastic neutron scattering (QENS) measurements on Mo/H-ZSM-5 samples reacted with methane for 0, 7, 25 and 60 min. Catalytic activity of the samples followed by mass spectrometry indicate that the induction period in which Mo species are carburized lasts for ˜9 min; after this period the material shows selectivity to aromatics. Characterization by TGA and N2 physisorption suggest that practically no carbon is deposited during the induction period. The ˜2 wt % of coke formed after one hour of reaction has a negligible effect in the zeolite crystal structurebut a small effect on the micropore volume. The QENS studies show that the methane transport by jump diffusion is however not measurably affected by the accumulated coke in the samples.
Ice-sheet-driven methane storage and release in the Arctic
Portnov, Alexey; Vadakkepuliyambatta, Sunil; Mienert, Jürgen; Hubbard, Alun
2016-01-01
It is established that late-twentieth and twenty-first century ocean warming has forced dissociation of gas hydrates with concomitant seabed methane release. However, recent dating of methane expulsion sites suggests that gas release has been ongoing over many millennia. Here we synthesize observations of ∼1,900 fluid escape features—pockmarks and active gas flares—across a previously glaciated Arctic margin with ice-sheet thermomechanical and gas hydrate stability zone modelling. Our results indicate that even under conservative estimates of ice thickness with temperate subglacial conditions, a 500-m thick gas hydrate stability zone—which could serve as a methane sink—existed beneath the ice sheet. Moreover, we reveal that in water depths 150–520 m methane release also persisted through a 20-km-wide window between the subsea and subglacial gas hydrate stability zone. This window expanded in response to post-glacial climate warming and deglaciation thereby opening the Arctic shelf for methane release. PMID:26739497
Methanogenesis in oxygenated soils is a substantial fraction of wetland methane emissions
Angle, Jordan C.; Morin, Timothy H.; Solden, Lindsey M.; ...
2017-11-16
The current paradigm, widely incorporated in soil biogeochemical models, is that microbial methanogenesis can only occur in anoxic habitats. In contrast, here we show clear geochemical and biological evidence for methane production in well-oxygenated soils of a freshwater wetland. A comparison of oxic to anoxic soils reveal up to ten times greater methane production and nine times more methanogenesis activity in oxygenated soils. Metagenomic and metatranscriptomic sequencing recover the first near-complete genomes for a novel methanogen species, and show acetoclastic production from this organism was the dominant methanogenesis pathway in oxygenated soils. This organism, Candidatus Methanothrix paradoxum, is prevalent acrossmore » methane emitting ecosystems, suggesting a global significance. Moreover, in this wetland, we estimate that up to 80% of methane fluxes could be attributed to methanogenesis in oxygenated soils. Together, our findings challenge a widely held assumption about methanogenesis, with significant ramifications for global methane estimates and Earth system modeling.« less
NASA Astrophysics Data System (ADS)
Lorenson, T. D.; Collett, T. S.; Ignik Sikumi, S.
2012-12-01
Hydrocarbon gases, nitrogen, carbon dioxide and water were collected from production streams at the Ignik Sikumi gas hydrate production test well (TD, 791.6 m), drilled on the Alaska North Slope. The well was drilled to test the feasibility of producing methane by carbon dioxide injection that replaces methane in the solid gas hydrate. The Ignik Sikumi well penetrated a stratigraphically-bounded prospect within the Eileen gas hydrate accumulation. Regionally, the Eileen gas hydrate accumulation overlies the more deeply buried Prudhoe Bay, Milne Point, and Kuparuk River oil fields and is restricted to the up-dip portion of a series of nearshore deltaic sandstone reservoirs in the Sagavanirktok Formation. Hydrate-bearing sandstones penetrated by Ignik Sikumi well occur in three primary horizons; an upper zone, ("E" sand, 579.7 - 597.4 m) containing 17.7 meters of gas hydrate-bearing sands, a middle zone ("D" sand, 628.2 - 648.6 m) with 20.4 m of gas hydrate-bearing sands and a lower zone ("C" sand, 678.8 - 710.8 m), containing 32 m of gas hydrate-bearing sands with neutron porosity log-interpreted average gas hydrate saturations of 58, 76 and 81% respectively. A known volume mixture of 77% nitrogen and 23% carbon dioxide was injected into an isolated section of the upper part of the "C" sand to start the test. Production flow-back part of the test occurred in three stages each followed by a period of shut-in: (1) unassisted flowback; (2) pumping above native methane gas hydrate stability conditions; and (3) pumping below the native methane gas hydrate stability conditions. Methane production occurred immediately after commencing unassisted flowback. Methane concentration increased from 0 to 40% while nitrogen and carbon dioxide concentrations decreased to 48 and 12% respectively. Pumping above the hydrate stability phase boundary produced gas with a methane concentration climbing above 80% while the carbon dioxide and nitrogen concentrations fell to 2 and 18% respectively. Pumping below the gas hydrate stability phase boundary occurred in two periods with the composition of the produced gases continually increasing in methane reaching an excess of 96%, along with carbon dioxide decreasing to <1% and nitrogen to ~3%. The isotopic composition of all the gases was monitored. Methane carbon and hydrogen isotopic compositions remained stable throughout the test, while the carbon dioxide carbon became isotopically heavier. Nitrogen isotopic composition remained stable or became slightly isotopically depleted at the later phase of the test. These results imply that the produced methane was not isotopically fractionated, whereas carbon dioxide was fractionated becoming isotopically heavier at the end of each production phase. In addition, water samples were analyzed during the production phase documenting an increase in salinity.
Trichloroethylene Biodegradation by a Methane-Oxidizing Bacterium †
Little, C. Deane; Palumbo, Anthony V.; Herbes, Stephen E.; Lidstrom, Mary E.; Tyndall, Richard L.; Gilmer, Penny J.
1988-01-01
Trichloroethylene (TCE), a common groundwater contaminant, is a suspected carcinogen that is highly resistant to aerobic biodegradation. An aerobic, methane-oxidizing bacterium was isolated that degrades TCE in pure culture at concentrations commonly observed in contaminated groundwater. Strain 46-1, a type I methanotrophic bacterium, degraded TCE if grown on methane or methanol, producing CO2 and water-soluble products. Gas chromatography and 14C radiotracer techniques were used to determine the rate, methane dependence, and mechanism of TCE biodegradation. TCE biodegradation by strain 46-1 appears to be a cometabolic process that occurs when the organism is actively metabolizing a suitable growth substrate such as methane or methanol. It is proposed that TCE biodegradation by methanotrophs occurs by formation of TCE epoxide, which breaks down spontaneously in water to form dichloroacetic and glyoxylic acids and one-carbon products. Images PMID:16347616
Methane in the lunar exosphere: Implications for solar wind carbon escape
NASA Astrophysics Data System (ADS)
Hodges, R. Richard
2016-07-01
A positive identification of methane in the lunar exosphere has been made in data from the neutral mass spectrometer on the Lunar Atmosphere and Dust Environment Explorer (LADEE) spacecraft. Like argon-40, methane is adsorbed on the lunar surface during nighttime. However, higher activation energies for methane delay its desorption at sunrise by about an hour local time, creating a postsunrise bulge with peak concentration of approximately 400-450 molecules cm-3 at a reference altitude of 12 km, which is just above the highest topographic feature on the Moon. The rate of escape of carbon as methane derived from the LADEE data is estimated to be in the range 1.5-4.5 × 1021 s-1. A lower bound for solar carbon escape derived separately from Apollo sample analyses is 3.4 × 1021 s-1.
Methane Recovery from Gaseous Mixtures Using Carbonaceous Adsorbents
NASA Astrophysics Data System (ADS)
Buczek, Bronisław
2016-06-01
Methane recovery from gaseous mixtures has both economical and ecological aspect. Methane from different waste gases like mine gases, nitrogenated natural gases and biogases can be treated as local source for production electric and heat energy. Also occurs the problem of atmosphere pollution with methane that shows over 20 times more harmful environmental effect in comparison to carbon dioxide. One of the ways utilisation such gases is enrichment of methane in the PSA technique, which requires appropriate adsorbents. Active carbons and carbon molecular sieve produced by industry and obtained in laboratory scale were examined as adsorbent for methane recuperation. Porous structure of adsorbents was investigated using densimetry measurements and adsorption of argon at 77.5K. On the basis of adsorption data, the Dubinin-Radushkevich equation parameters, micropore volume (Wo) and characteristics of energy adsorption (Eo) as well as area micropores (Smi) and BET area (SBET) were determined. The usability of adsorbents in enrichment of the methane was evaluated in the test, which simulate the basic stages of PSA process: a) adsorbent degassing, b) pressure raise in column by feed gas, c) cocurrent desorption with analysis of out flowing gas. The composition of gas phase was accepted as the criterion of the suitability of adsorbent for methane separation from gaseous mixtures. The relationship between methane recovery from gas mixture and texture parameters of adsorbents was found.
ECOS E-MATRIX Methane and Volatile Organic Carbon (VOC) Emissions Best Practices Database
DOE Office of Scientific and Technical Information (OSTI.GOV)
Parisien, Lia
2016-01-31
This final scientific/technical report on the ECOS e-MATRIX Methane and Volatile Organic Carbon (VOC) Emissions Best Practices Database provides a disclaimer and acknowledgement, table of contents, executive summary, description of project activities, and briefing/technical presentation link.
Evidence of active methanogen communities in shallow sediments of the sonora margin cold seeps.
Vigneron, Adrien; L'Haridon, Stéphane; Godfroy, Anne; Roussel, Erwan G; Cragg, Barry A; Parkes, R John; Toffin, Laurent
2015-05-15
In the Sonora Margin cold seep ecosystems (Gulf of California), sediments underlying microbial mats harbor high biogenic methane concentrations, fueling various microbial communities, such as abundant lineages of anaerobic methanotrophs (ANME). However, the biodiversity, distribution, and metabolism of the microorganisms producing this methane remain poorly understood. In this study, measurements of methanogenesis using radiolabeled dimethylamine, bicarbonate, and acetate showed that biogenic methane production in these sediments was mainly dominated by methylotrophic methanogenesis, while the proportion of autotrophic methanogenesis increased with depth. Congruently, methane production and methanogenic Archaea were detected in culture enrichments amended with trimethylamine and bicarbonate. Analyses of denaturing gradient gel electrophoresis (DGGE) fingerprinting and reverse-transcribed PCR-amplified 16S rRNA sequences retrieved from these enrichments revealed the presence of active methylotrophic Methanococcoides burtonii relatives and several new autotrophic Methanogenium lineages, confirming the cooccurrence of Methanosarcinales and Methanomicrobiales methanogens with abundant ANME populations in the sediments of the Sonora Margin cold seeps. Copyright © 2015, American Society for Microbiology. All Rights Reserved.
Process for producing methane from gas streams containing carbon monoxide and hydrogen
Frost, Albert C.
1980-01-01
Carbon monoxide-containing gas streams are passed over a catalyst capable of catalyzing the disproportionation of carbon monoxide so as to deposit a surface layer of active surface carbon on the catalyst essentially without formation of inactive coke thereon. The surface layer is contacted with steam and is thus converted to methane and CO.sub.2, from which a relatively pure methane product may be obtained. While carbon monoxide-containing gas streams having hydrogen or water present therein can be used only the carbon monoxide available after reaction with said hydrogen or water is decomposed to form said active surface carbon. Although hydrogen or water will be converted, partially or completely, to methane that can be utilized in a combustion zone to generate heat for steam production or other energy recovery purposes, said hydrogen is selectively removed from a CO--H.sub.2 -containing feed stream by partial oxidation thereof prior to disproportionation of the CO content of said stream.
Investigations of Methane Production in Hypersaline Environments
NASA Technical Reports Server (NTRS)
Bebout, Brad M.
2015-01-01
The recent reports of methane in the atmosphere of Mars, as well as the findings of hypersaline paleo-environments on that planet, have underscored the need to evaluate the importance of biological (as opposed to geological) trace gas production and consumption. Methane in the atmosphere of Mars may be an indication of life but might also be a consequence of geologic activity and/or the thermal alteration of ancient organic matter. Hypersaline environments have now been reported to be extremely likely in several locations in our solar system, including: Mars, Europa, and Enceladus. Modern hypersaline microbial mat communities, (thought to be analogous to those present on the early Earth at a period of time when Mars was experiencing very similar environmental conditions), have been shown to produce methane. However, very little is known about the physical and/or biological controls imposed upon the rates at which methane, and other important trace gases, are produced and consumed in these environments. We describe here the results of our investigations of methane production in hypersaline environments, including field sites in Chile, Baja California Mexico, California, USA and the United Arab Emirates. We have measured high concentrations of methane in bubbles of gas produced both in the sediments underlying microbial mats, as well as in areas not colonized by microbial mats in the Guerrero Negro hypersaline ecosystem, Baja California Mexico, in Chile, and in salt ponds on the San Francisco Bay. The carbon isotopic (d13C) composition of the methane in the bubbles exhibited an extremely wide range of values, (ca. -75 per mille ca. -25 per mille). The hydrogen isotopic composition of the methane (d2H) ranged from -60 to -30per mille and -450 to -350per mille. These isotopic values are outside of the range of values normally considered to be biogenic, however incubations of the sediments in contact with these gas bubbles reveals that the methane is indeed being produced by these sediments. Substrate limitation of methanogenesis in these environments, and not methane oxidation, would explain the isotopic values of the methane in these environments. Incubations with both isotopically labeled and unlabeled putative substrates for methanogenesis have shown that the substrates most important for methanogenesis in these environments are the so-called non-competitive substrates, e.g., methylamines, dimethylsulfide, and methanol. Acetate and bicarbonate appear not to be important substrates for methanogens in these environments. Extraction of DNA and analysis of a gene used for methane production (mcrA) has revealed that the community composition of methanogens is consistent with organisms known to use non-competitive substrates. Our work has shown that hypersaline environments have the potential to both produce and preserve methane for analysis, e.g., by capable rovers. Our work expends the range of methane isotopic values now known to be produced by active methanogenesis
NASA Astrophysics Data System (ADS)
Watkins, B. E.; Droege, M. W.; Taylor, R. T.; Satcher, J. H.
1992-06-01
Methane monooxygenase (MMO) is an enzyme found in methanotrophs that catalyses the selective oxidation of methane to methanol. MMO is protein complex one component of which is a binuclear metal center containing oxygenase. We have completed one round of a design/synthesis/evaluation cycle in the development of coordination complexes that mimic the structure/function of the MMO active site. One of these, a binuclear, coordinately-asymmetric copper complex, is capable of oxidizing cyclohexane to a mixture of cyclohexanol and cyclohexanone in the presence of hydrogen peroxide.
Nonlinear effects of stretch on the flame front propagation
DOE Office of Scientific and Technical Information (OSTI.GOV)
Halter, F.; Tahtouh, T.; Mounaim-Rousselle, C.
2010-10-15
In all experimental configurations, the flames are affected by stretch (curvature and/or strain rate). To obtain the unstretched flame speed, independent of the experimental configuration, the measured flame speed needs to be corrected. Usually, a linear relationship linking the flame speed to stretch is used. However, this linear relation is the result of several assumptions, which may be incorrected. The present study aims at evaluating the error in the laminar burning speed evaluation induced by using the traditional linear methodology. Experiments were performed in a closed vessel at atmospheric pressure for two different mixtures: methane/air and iso-octane/air. The initial temperaturesmore » were respectively 300 K and 400 K for methane and iso-octane. Both methodologies (linear and nonlinear) are applied and results in terms of laminar speed and burned gas Markstein length are compared. Methane and iso-octane were chosen because they present opposite evolutions in their Markstein length when the equivalence ratio is increased. The error induced by the linear methodology is evaluated, taking the nonlinear methodology as the reference. It is observed that the use of the linear methodology starts to induce substantial errors after an equivalence ratio of 1.1 for methane/air mixtures and before an equivalence ratio of 1 for iso-octane/air mixtures. One solution to increase the accuracy of the linear methodology for these critical cases consists in reducing the number of points used in the linear methodology by increasing the initial flame radius used. (author)« less
Grumpe, Arne; Becker, Adrian; Wöhler, Christian
2018-01-01
Simple Summary Methane (CH4) is common on Earth but its natural sources are not well-characterized. We investigated concentrations of CH4 and its stable carbon isotope (δ13C-CH4) within a red wood-ant (RWA; Formica polyctena) nest in the Neuwied Basin, a part of the East Eifel Volcanic Field (EEVF), and tested for associations between methane concentration and RWA activity patterns, earthquakes, and earth tides. Methane degassing was not synchronized with earth tides, nor was it influenced by a micro-earthquake or RWA activity. Elevated CH4 concentrations in nest gas appear to result from a combination of microbial activity and fault-related emissions. The latter could result from micro-seepage of methane derived from low-temperature gas-water-rock reactions that subsequently moves via fault networks through the RWA nest or from overlapping micro-seepage of magmatic CH4 from the Eifel plume. Given the abundance of RWA nests on the landscape, their role as sources of microbial CH4 and biological indicators for abiotically-derived CH4 should be included in estimations of methane emissions that are contributing to climatic change. Abstract We measured methane (CH4) and stable carbon isotope of methane (δ13C-CH4) concentrations in ambient air and within a red wood-ant (RWA; Formica polyctena) nest in the Neuwied Basin (Germany) using high-resolution in-situ sampling to detect microbial, thermogenic, and abiotic fault-related micro-seepage of CH4. Methane degassing from RWA nests was not synchronized with earth tides, nor was it influenced by micro-earthquake degassing or concomitantly measured RWA activity. Two δ13C-CH4 signatures were identified in nest gas: −69‰ and −37‰. The lower peak was attributed to microbial decomposition of organic matter within the RWA nest, in line with previous observations that RWA nests are hot-spots of microbial CH4. The higher peak has not been reported in previous studies. We attribute this peak to fault-related CH4 emissions moving via fault networks into the RWA nest, which could originate either from thermogenic or abiotic CH4 formation. Sources of these micro-seepages could be Devonian schists, iron-bearing “Klerf Schichten”, or overlapping micro-seepage of magmatic CH4 from the Eifel plume. Given the abundance of RWA nests on the landscape, their role as sources of microbial CH4 and biological indicators for abiotically-derived CH4 should be included in estimation of methane emissions that are contributing to climatic change. PMID:29597318
NASA Astrophysics Data System (ADS)
Timmermann, H.; Sawady, W.; Reimert, R.; Ivers-Tiffée, E.
The internal reforming of methane in a solid oxide fuel cell (SOFC) is investigated and modeled for flow conditions relevant to operation. To this end, measurements are performed on anode-supported cells (ASC), thereby varying gas composition (y CO = 4-15%, yH2 = 5 - 17 % , yCO2 = 6 - 18 % , yH2O = 2 - 30 % , yCH4 = 0.1 - 20 %) and temperature (600-850 °C). In this way, operating conditions for both stationary applications (methane-rich pre-reformate) as well as for auxiliary power unit (APU) applications (diesel-POX reformate) are represented. The reforming reaction is monitored in five different positions alongside the anodic gas channel by means of gas chromatography. It is shown that methane is converted in the flow field for methane-rich gas compositions, whereas under operation with diesel reformate the direction of the reaction is reversed for temperatures below 675 °C, i.e. (exothermic) methanation occurs along the anode. Using a reaction model, a rate equation for reforming could be derived which is also valid in the case of methanation. By introducing this equation into the reaction model the methane conversion along a catalytically active Ni-YSZ cermet SOFC anode can be simulated for the operating conditions specified above.
Baseline study of methane emission from anaerobic ponds of palm oil mill effluent treatment.
Yacob, Shahrakbah; Ali Hassan, Mohd; Shirai, Yoshihito; Wakisaka, Minato; Subash, Sunderaj
2006-07-31
The world currently obtains its energy from the fossil fuels such as oil, natural gas and coal. However, the international crisis in the Middle East, rapid depletion of fossil fuel reserves as well as climate change have driven the world towards renewable energy sources which are abundant, untapped and environmentally friendly. Malaysia has abundant biomass resources generated from the agricultural industry particularly the large commodity, palm oil. This paper will focus on palm oil mill effluent (POME) as the source of renewable energy from the generation of methane and establish the current methane emission from the anaerobic treatment facility. The emission was measured from two anaerobic ponds in Felda Serting Palm Oil Mill for 52 weeks. The results showed that the methane content was between 35.0% and 70.0% and biogas flow rate ranged between 0.5 and 2.4 L/min/m(2). Total methane emission per anaerobic pond was 1043.1 kg/day. The total methane emission calculated from the two equations derived from relationships between methane emission and total carbon removal and POME discharged were comparable with field measurement. This study also revealed that anaerobic pond system is more efficient than open digesting tank system for POME treatment. Two main factors affecting the methane emission were mill activities and oil palm seasonal cropping.
NASA Astrophysics Data System (ADS)
Laurila, T. J.; Aurela, M.; Hatakka, J.; Aalto, T.; Lohila, A.; Asmi, E.; Kondratyev, V.; Ivakhov, V.; Reshetnikov, A.; Makshtas, A. P.; Dlugokencky, E. J.; Uttal, T.
2013-12-01
Arctic and Boreal regions are important in the global methane budget mainly because emissions are large from the extensive wetlands. Recently the potential for increased emissions from methane hydrates under sediments at the bottom of the Arctic Ocean has been recognized. Resource exploitation in the Arctic is expanding and includes gas and oil drilling. Together with climate warming, we may expect changes in methane emissions from high northern latitudes. The main tools to probe the effect of this development on atmospheric methane are atmospheric methane observations and local emission measurements by micrometeorological and chamber methods. To better understand emissions at small and large scales, so called supersites have been introduced. At these sites, both atmospheric concentrations and emissions from representative ecosystems, together with suite of other environmental information, are measured continuously. We are running two of these supersites: Pallas-Sodankylä in northern Finland and Tiksi in Siberia on the coast of the Laptev Sea. In spite of the fact that both sites are north of the Arctic Circle, environmental conditions differ very much. In northern Scandinavia, climate is relatively marine, and wetland methane emissions are active throughout the year. In continental Tiksi the active layer is 30-80 cm and methane emissions cease during the coldest months when soil temperature is close to -20°C. Air mass advection is either from continental Siberia or from the Siberian seas. Forest and tundra fires are relatively common. At Pallas, advection is from the forested boreal and industrialized areas of Europe or the Norwegian or Barents Sea. In this presentation, we show seasonal variations of atmospheric methane concentrations at World Meteorological Organization - Global Atmosphere Watch sites: Pallas-Sodankylä and Tiksi. Source areas have been analyzed by trajectories. The main sources of methane in Tiksi were wetlands and the Laptev Sea, which is oversaturated regarding methane. Concentrations and their variability were high in June-October due to terrestrial and marine emissions. Sea ice restricts marine emissions very much. Interesting periods were when the sea froze in October and when the ice melted in early July. Seasonal pattern of tundra methane emissions will be presented including growing season onset in June-July, high season in August and late season emission rates extending to winter. These will be compared to emission rates at typical northern boreal fens of the Pallas-Sodankylä site. It is expected that the Tiksi and Pallas-Sodakyla site will form the foundation for further pan-Arctic comparisons between the observatories in the IASOA consortium (www.iasoa.org).
Wang, Liping; Yao, Ying; He, Rong; Meng, Yan; Li, Na; Zhang, Dan; Xu, Jiajun; Chen, Ouyang; Cui, Jin; Bian, Jinjun; Zhang, Yan; Chen, Guozhong; Deng, Xiaoming
2017-02-01
Methane is reported to have antioxidant, anti-inflammatory and anti-apoptotic properties. We investigated the potential neuroprotective effects of methane-rich saline (MS) on spinal cord ischemia-reperfusion injury and determined that its therapeutic benefits are associated with the activation of nuclear factor erythroid 2-related factor 2 (Nrf2). Rats received 9min of spinal cord ischemia induced by occlusion of the descending thoracic aorta plus systemic hypotension followed by a single MS treatment (10ml/kg, ip) and 72h reperfusion. MS treatment attenuated motor sensory deficits and produced high concentrations of methane in spinal cords during reperfusion, which increased Nrf2 expression and transcriptional activity in neurons, microglia and astrocytes in the ventral, intermediate and dorsal gray matter of lumbar segments. Heme oxygenase-1, superoxide dismutase, catalase and glutathione were upregulated; and glutathione disulfide, superoxide, hydrogen peroxide, malondialdehyde, 8-hydroxy-2-deoxyguanosine and 3-nitrotyrosine were downregulated in MS-treated spinal cords. MS treatment reduced neuronal apoptosis in gray matter zones, which was consistent with the suppression of cytochrome c release to the cytosol from the mitochondria and the activation of caspase-9 and -3. Throughout the gray matter, the activation of microglia and astrocytes was inhibited; the nuclear accumulation of phosphorylated nuclear factor-kappa B p65 was reduced; and tumor necrosis factor α, interleukin 1β, chemokine (C-X-C motif) ligand 1, intercellular adhesion molecule 1 and myeloperoxidase were decreased. MS treatment attenuated blood-spinal cord barrier dysfunction by preventing the expression and activity of matrix metallopeptidase-9 and disrupting tight junction proteins. Consecutive intrathecal injection of specific siRNAs targeting Nrf2 at 24-h intervals 3 days before ischemia reduced the beneficial effects of MS. Our data indicate that MS treatment prevents IR-induced spinal cord damage via antioxidant, anti-inflammatory and anti-apoptotic activities that involve the activation of Nrf2 signaling. Thus, methane may serve as a novel promising therapeutic agent for treating ischemic spinal cord injury. Copyright © 2016 Elsevier Inc. All rights reserved.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Grunwaldt, Jan-Dierk; Baiker, Alfons
2007-02-02
x-ray absorption spectroscopy is a well-suited technique to uncover the structure of heterogeneous catalysts under reaction conditions. Different aspects of in situ cell design suitable for dynamic and catalytic studies are discussed. In addition, criteria are presented that allow estimating the influence external and internal mass transfer. Starting with studies on gas-solid reactions, including structure-activity relationships, this concept is extended to liquid-solid reactions, reactions at high pressure and in supercritical fluids. The following examples are discussed in more detail: partial oxidation of methane over Pt-Rh/Al2O3, reduction of a Cu/ZnO catalyst, alcohol oxidation over Bi-promoted Pd/Al2O3 in liquid phase and overmore » Pd/Al2O3 in supercritical CO2, and batch reactions (e.g. CO2-fixation over zinc-based catalysts)« less
Dissolved methane in groundwater, Upper Delaware River Basin, Pennsylvania and New York, 2007-12
Kappel, William M.
2013-01-01
The prospect of natural gas development from the Marcellus and Utica Shales has raised concerns about freshwater aquifers being vulnerable to contamination. Well owners are asking questions about subsurface methane, such as, “Does my well water have methane and is it safe to drink the water?” and “Is my well system at risk of an explosion hazard associated with a combustible gas like methane in groundwater?” This newfound awareness of methane contamination of water wells by stray gas migration is based upon studies such as Molofsky and others (2011) who document the widespread natural occurrence of methane in drinking-water wells in Susquehanna County, Pennsylvania. In the same county, Osborn and others (2011) identified elevated methane concentrations in selected drinking-water wells in the vicinity of Marcellus Shale gas-development activities, although pre-development groundwater samples were not available for comparison. A compilation of dissolved methane concentrations in groundwater for New York State was published by Kappel and Nystrom (2012). Recent work documenting the occurrence and distribution of methane in groundwater was completed in southern Sullivan County, Pennsylvania (Sloto, 2013). Additional work is ongoing with respect to monitoring for stray gases in groundwater (Jackson and others, 2013). These studies and their results indicate the importance of collecting baseline or pre-development data. While such data are being collected in some areas, published data on methane in groundwater are sparse in the Upper Delaware River Basin of Pennsylvania, New York, and New Jersey. To manage drinking-water resources in areas of gas-well drilling and hydraulic fracturing in the Upper Delaware River Basin, the natural occurrence of methane in the tri-state aquifers needs to be documented. The purpose of this report is to present data on dissolved methane concentrations in the groundwater in the Upper Delaware River Basin. The scope is restricted to data for Pennsylvania and New York, no U.S. Geological Survey (USGS) methane analyses are presently available for northwestern New Jersey.
NASA Astrophysics Data System (ADS)
Pum, Lisa; Reichenauer, Thomas; Germida, Jim
2015-04-01
Anthropogenic activities create a number of significant greenhouse gases and thus potentially contribute to global warming. Methane production is significant in some agricultural production systems and from wetlands. In soil, methane can be oxidised by methanotrophic bacteria. However, little is known about methane production and oxidation in oil sand reclamation covers. The purpose of this study was to investigate methane production and oxidation potential of tailing sands and six different reclamation layers of oil sands mining sites in Alberta, Canada. Methane production and oxidation potential were investigated in laboratory scale microcosms through continuous headspace analysis using gas chromatography. Samples from a reclamation layer were collected at the Canadian Natural Resources Limited (CNRL) reclamation site at depths of 0-10 cm, 10-20 cm and 20-40 cm in October 2014. In addition, tailing sands provided by Suncor Energy Inc. and soil from a CNRL wetland were studied for methane production. Samples were dried, crushed and sieved to 4 mm, packed into serum bottle microcosms and monitored for eight weeks. Methane production potential was assessed by providing an anoxic environment and by adjusting the samples to a moisture holding capacity of 100 %. Methane oxidation potential was examined by an initial application of 2 vol % methane to the microcosms and by adjusting the samples to a moisture holding capacity of 50 %. Microcosm headspace gas was analysed for methane, carbon dioxide, nitrous oxide and oxygen. All experiments were carried out in triplicates, including controls. SF6 and Helium were used as internal standards to detect potential leaks. Our results show differences for methane production potential between the soil depths, tailing sands and wetlands. Moreover, there were differences in the methane oxidation potential of substrate from the three depths investigated and between the reclamation layers. In conclusion, the present study shows that reclamation layers for oil sands mining sites in Alberta, Canada have the potential to oxidize on-site produced methane emissions to the less harmful greenhouse gas carbon dioxide. Such oxidation might mitigate impacts of methane production from these sites.
NASA Astrophysics Data System (ADS)
Leonte, Mihai; Kessler, John D.; Kellermann, Matthias Y.; Arrington, Eleanor C.; Valentine, David L.; Sylva, Sean P.
2017-05-01
Aerobic oxidation is an important methane sink in seawater overlying gas seeps. Recent surveys have identified active methane seeps in the waters of Hudson Canyon, US Atlantic Margin near the updip limit of methane clathrate hydrate stability. The close proximity of these seeps to the upper stability limit of methane hydrates suggests that changing bottom water temperatures may influence the release rate of methane into the overlying water column. In order to assess the significance of aerobic methane oxidation in limiting the atmospheric expression of methane released from Hudson Canyon, the total extent of methane oxidized along with integrated oxidation rates were quantified. These calculations were performed by combining the measurements of the natural levels of methane concentrations, stable carbon isotopes, and water current velocities into kinetic isotope models yielding rates ranging from 22.8 ± 17 to 116 ± 76 nM/day with an average of 62.7 ± 37 nM/day. Furthermore, an average of 63% of methane released into the water column from an average depth of 515 m was oxidized before leaving this relatively small study area (6.5 km2). Results from the kinetic isotope model were compared to previously-published but concurrently-sampled ex situ measurements of oxidation potential performed using 13C-labeled methane. Ex situ rates were substantially lower, ranging from 0.1 to 22.5 nM/day with an average of 5.6 ± 2.3 nM/day, the discrepancy likely due to the inherent differences between these two techniques. Collectively, the results reveal exceptionally-rapid methane oxidation, with turnover times for methane as low as 0.3-3.7 days, indicating that methane released to the water column is removed quantitatively within the greater extent of Hudson Canyon. The red line represents the original Rayleigh model output, Eq. (1), detailed in the text. The red line represents the original Rayleigh model output, Eq. (1), detailed in the text.
Origin of lipid biomarkers in mud volcanoes from the Alboran Sea, western Mediterranean
NASA Astrophysics Data System (ADS)
López-Rodríguez, C.; Stadnitskaia, A.; De Lange, G. J.; Martínez-Ruíz, F.; Comas, M.; Sinninghe Damsté, J. S.
2013-11-01
Mud volcanoes (MVs) are the most prominent indicators of active methane/hydrocarbon venting at the seafloor on both passive and active continental margins. Their occurrence in the Western Mediterranean is patent at the West Alboran Basin, where numerous MVs develop overlaying a major sedimentary depocenter containing overpressured shales. Although some of these MVs have been studied, the detailed biogeochemistry of expelled mud so far has not been examined in detail. This work provides the first results on the composition and origin of organic matter, Anaerobic Oxidation of Methane (AOM) processes and general characteristics on MV dynamics using lipid biomarkers as the main tool. Lipid biomarker analysis was performed on MV expelled material (mud breccias) and interbedded hemipelagic sediments from Perejil, Kalinin and Schneider's Heart MVs located in the northwest margin of the Alboran Sea. The n-alkane-distributions and n-alkane-derived indices (CPI and ACL), in combination with the epimerization degree of hopanes (22S/(22S + 22R)) indicate that all studied mud breccia have a similar biomarker composition consisting of mainly thermally immature organic matter with an admixture of petroleum-derived compounds. This concordant composition indicates that common source strata must feed all three studied MVs. The past or present AOM activity was established using lipid biomarkers specific for anaerobic methanotropic archaea (irregular isoprenoids and DGDs) and the depleted carbon isotope composition (δ13C) of crocetane/phytane. The presence of these lipid biomarkers, together with the low amounts of detected GDGTs, is consistent with the dominance of anaerobic methanotrophs of the ANME-2 over ANME-1, at least in mud breccia from Perejil MVs. In contrast, the scarce presence or lack of these AOM-related lipid biomarkers in sediments from Kalinin and Schneider's Heart MVs, suggest no recent active methane seepage has occurred at these sites. Moreover, the observed methane concentrations support the current activity of Perejil MV, and the very low methane seepage activity in Kalinin and Schneider's Heart MVs.
Anaerobic biodegradation of aircraft deicing fluid in UASB reactors.
Tham, P T Pham thi; Kennedy, K J Kevin J
2004-05-01
A central composite design was employed to methodically investigate anaerobic treatment of aircraft deicing fluid (ADF) in bench-scale Upflow Anaerobic Sludge Blanket (UASB) reactors. A total of 23 runs at 17 different operating conditions (0.8% 1.6% ADF (6000-12,000mg/L COD), 12-56h HRT, and 18-36gVSS/L) were conducted in continuous mode. The development of four empirical models describing process responses (i.e. COD removal efficiency, biomass-specific acetoclastic activity, methane production rate, and methane production potential) as functions of ADF concentration, hydraulic retention time, and biomass concentration is presented. Model verification indicated that predicted responses (COD removal efficiencies, biomass-specific acetoclastic activity, and methane production rates and potential) were in good agreement with experimental results. Biomass-specific acetoclastic activity was improved two-fold from 0.23gCOD/gVSS/d for inoculum to a maximum of 0.55gCOD/gVSS/d during ADF treatment in UASB reactors. For the design window, COD removal efficiencies were higher than 90%. The predicted methane production potentials were close to theoretical values, and methane production rates increased as the organic loading rate is increased. ADF toxicity effects were evident for 1.6% ADF at medium organic loadings (SOLR above 0.5gCOD/gVSS/d). In contrast, good reactor stability and excellent COD removal efficiencies were achieved at 1.2% ADF for reactor loadings approaching that of highly loaded systems (0.73gCOD/gVSS/d).
Anaerobic Oxidation of Methane Coupled to Nitrite Reduction by Halophilic Marine NC10 Bacteria.
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.
Enhanced catalyst stability for cyclic co methanation operations
Risch, Alan P.; Rabo, Jule A.
1983-01-01
Carbon monoxide-containing gas streams are passed over a catalyst to deposit a surface layer of active surface carbon thereon essentially without the formation of inactive coke. The active carbon is thereafter reacted with steam or hydrogen to form methane. Enhanced catalyst stability for long term, cyclic operation is obtained by the incorporation of an alkali or alkaline earth dopant in a silica binding agent added to the catalyst-support additive composition.
Product selectivity in plasmonic photocatalysis for carbon dioxide hydrogenation.
Zhang, Xiao; Li, Xueqian; Zhang, Du; Su, Neil Qiang; Yang, Weitao; Everitt, Henry O; Liu, Jie
2017-02-23
Photocatalysis has not found widespread industrial adoption, in spite of decades of active research, because the challenges associated with catalyst illumination and turnover outweigh the touted advantages of replacing heat with light. A demonstration that light can control product selectivity in complex chemical reactions could prove to be transformative. Here, we show how the recently demonstrated plasmonic behaviour of rhodium nanoparticles profoundly improves their already excellent catalytic properties by simultaneously reducing the activation energy and selectively producing a desired but kinetically unfavourable product for the important carbon dioxide hydrogenation reaction. Methane is almost exclusively produced when rhodium nanoparticles are mildly illuminated as hot electrons are injected into the anti-bonding orbital of a critical intermediate, while carbon monoxide and methane are equally produced without illumination. The reduced activation energy and super-linear dependence on light intensity cause the unheated photocatalytic methane production rate to exceed the thermocatalytic rate at 350 °C.
Product selectivity in plasmonic photocatalysis for carbon dioxide hydrogenation
Zhang, Xiao; Li, Xueqian; Zhang, Du; Su, Neil Qiang; Yang, Weitao; Everitt, Henry O.; Liu, Jie
2017-01-01
Photocatalysis has not found widespread industrial adoption, in spite of decades of active research, because the challenges associated with catalyst illumination and turnover outweigh the touted advantages of replacing heat with light. A demonstration that light can control product selectivity in complex chemical reactions could prove to be transformative. Here, we show how the recently demonstrated plasmonic behaviour of rhodium nanoparticles profoundly improves their already excellent catalytic properties by simultaneously reducing the activation energy and selectively producing a desired but kinetically unfavourable product for the important carbon dioxide hydrogenation reaction. Methane is almost exclusively produced when rhodium nanoparticles are mildly illuminated as hot electrons are injected into the anti-bonding orbital of a critical intermediate, while carbon monoxide and methane are equally produced without illumination. The reduced activation energy and super-linear dependence on light intensity cause the unheated photocatalytic methane production rate to exceed the thermocatalytic rate at 350 °C. PMID:28230100
Methane emission and consumption at a North Sea gas seep (Tommeliten area)
NASA Astrophysics Data System (ADS)
Niemann, H.; Elvert, M.; Hovland, M.; Orcutt, B.; Judd, A.; Suck, I.; Gutt, J.; Joye, S.; Damm, E.; Finster, K.; Boetius, A.
2005-11-01
The North Sea hosts large coal, oil and gas reservoirs of commercial value. Natural leakage pathways of subsurface gas to the hydrosphere have been recognized during geological surveys (Hovland and Judd, 1988). The Tommeliten seepage area is part of the Greater Ekofisk area, which is situated above the Tommeliten Delta salt diapir in the central North Sea. In this study, we report of an active seep site (56°29.90'N, 2°59.80'E) located in the Tommeliten area, Norwegian Block 1/9, at 75 m water depth. Here, cracks in a buried marl horizon allow methane to migrate into overlying clay-silt and sandy sediments. Hydroacoustic sediment echosounding showed several venting spots coinciding with the apex of marl domes where methane is released into the water column and potentially to the atmosphere during deep mixing situations. In the vicinity of the gas seeps, sea floor observations showed small mats of giant sulphide-oxidizing bacteria above patches of black sediments and carbonate crusts, which are exposed 10 to 50 cm above seafloor forming small reefs. These Methane-Derived Authigenic Carbonates (MDACs) contain 13C-depleted, archaeal lipids indicating previous gas seepage and AOM activity. High amounts of sn2-hydroxyarchaeol relative to archaeol and low abundances of biphytanes in the crusts give evidence that ANaerobic MEthane-oxidising archaea (ANME) of the phylogenetic cluster ANME-2 were the potential mediators of Anaerobic Oxidation of Methane (AOM) at the time of carbonate formation. Small pieces of MDACs were also found subsurface at about 1.7 m sediment depth, associated with the Sulphate-Methane Transition Zone (SMTZ). The SMTZ of Tommeliten is characterized by elevated AOM and Sulphate Reduction (SR) rates, increased concentrations of 13C-depleted tetraether derived biphytanes, and specific bacterial Fatty Acids (FA). Further biomarker and 16S rDNA based analyses give evidence that AOM at the Tommeliten SMTZ is mediated by archaea belonging to the ANME-1b group and Sulphate Reducing Bacteria (SRB) most likely belonging to the Seep-SRB1 cluster. The zone of active methane consumption was restricted to a distinct horizon of about 20 cm. Concentrations of 13C-depleted lipid biomarkers (e.g. 500 ng g-dw-1 biphythanes, 140 ng g-dw-1 fatty acid ai-C15:0), cell numbers (1.5x108 cells cm-3), AOM and SR rates (3 nmol cm-3 d-1 in the SMTZ are 2-3 orders of magnitude lower compared to AOM zones of highly active cold seeps such as Hydrate Ridge or the Gulf of Mexico.
Wang, Xiao; Duan, Xu; Chen, Jianguang; Fang, Kuo; Feng, Leiyu; Yan, Yuanyuan; Zhou, Qi
2016-01-01
In this study the effect of volatile to total solids (VS/TS) on anaerobic digestion of waste activated sludge (WAS) pretreated by alkaline, thermal and thermal-alkaline strategies was studied. Experimental results showed that the production of methane from sludge was increased with VS/TS. When anaerobic digesters were fed with sludge pretreated by the thermal-alkaline method, the average methane yield was improved from 2.8 L/d at VS/TS 0.35 to 4.7 L/d at VS/TS 0.56. Also, the efficiency of VS reduction during sludge anaerobic digestion varied between 18.9% and 45.6%, and increased gradually with VS/TS. Mechanism investigation of VS/TS on WAS anaerobic digestion suggested that the general activities of anaerobic microorganisms, activities of key enzymes related to sludge hydrolysis, acidification and methanogenesis, and the ratio of Archaea to Bacteria were all increased with VS/TS, showing good agreement with methane production.
Methane Seepage on Mars: Where to Look and Why
NASA Astrophysics Data System (ADS)
Oehler, Dorothy Z.; Etiope, Giuseppe
2017-12-01
Methane on Mars is a topic of special interest because of its potential association with microbial life. The variable detections of methane by the Curiosity rover, orbiters, and terrestrial telescopes, coupled with methane's short lifetime in the martian atmosphere, may imply an active gas source in the planet's subsurface, with migration and surface emission processes similar to those known on Earth as "gas seepage." Here, we review the variety of subsurface processes that could result in methane seepage on Mars. Such methane could originate from abiotic chemical reactions, thermogenic alteration of abiotic or biotic organic matter, and ancient or extant microbial metabolism. These processes can occur over a wide range of temperatures, in both sedimentary and igneous rocks, and together they enhance the possibility that significant amounts of methane could have formed on early Mars. Methane seepage to the surface would occur preferentially along faults and fractures, through focused macro-seeps and/or diffuse microseepage exhalations. Our work highlights the types of features on Mars that could be associated with methane release, including mud-volcano-like mounds in Acidalia or Utopia; proposed ancient springs in Gusev Crater, Arabia Terra, and Valles Marineris; and rims of large impact craters. These could have been locations of past macro-seeps and may still emit methane today. Microseepage could occur through faults along the dichotomy or fractures such as those at Nili Fossae, Cerberus Fossae, the Argyre impact, and those produced in serpentinized rocks. Martian microseepage would be extremely difficult to detect remotely yet could constitute a significant gas source. We emphasize that the most definitive detection of methane seepage from different release candidates would be best provided by measurements performed in the ground or at the ground-atmosphere interface by landers or rovers and that the technology for such detection is currently available.
Ground and Airborne Methane Measurements Using Optical Parametric Amplifiers
NASA Technical Reports Server (NTRS)
Numata, Kenji; Riris, Haris; Li, Steve; Wu, Stewart; Kawa, Stephan R.; Abshire, James Brice; Dawsey, Martha; Ramanathan, Anand
2011-01-01
We report on ground and airborne methane measurements with an active sensing instrument using widely tunable, seeded optical parametric generation (OPG). The technique has been used to measure methane, CO2, water vapor, and other trace gases in the near and mid-infrared spectral regions. Methane is a strong greenhouse gas on Earth and it is also a potential biogenic marker on Mars and other planetary bodies. Methane in the Earth's atmosphere survives for a shorter time than CO2 but its impact on climate change can be larger than CO2. Carbon and methane emissions from land are expected to increase as permafrost melts exposing millennial-age carbon stocks to respiration (aerobic-CO2 and anaerobic-CH4) and fires. Methane emissions from c1athrates in the Arctic Ocean and on land are also likely to respond to climate warming. However, there is considerable uncertainty in present Arctic flux levels, as well as how fluxes will change with the changing environment. For Mars, methane measurements are of great interest because of its potential as a strong biogenic marker. A remote sensing instrument that can measure day and night over all seasons and latitudes can localize sources of biogenic gas plumes produced by subsurface chemistry or biology, and aid in the search for extra-terrestrial life. In this paper we report on remote sensing measurements of methane using a high peak power, widely tunable optical parametric generator (OPG) operating at 3.3 micrometers and 1.65 micrometers. We have demonstrated detection of methane at 3.3 micrometers and 1650 nanometers in an open path and compared them to accepted standards. We also report on preliminary airborne demonstration of methane measurements at 1.65 micrometers.
Schwach, Pierre; Pan, Xiulian; Bao, Xinhe
2017-07-12
The quest for an efficient process to convert methane efficiently to fuels and high value-added chemicals such as olefins and aromatics is motivated by their increasing demands and recently discovered large reserves and resources of methane. Direct conversion to these chemicals can be realized either oxidatively via oxidative coupling of methane (OCM) or nonoxidatively via methane dehydroaromatization (MDA), which have been under intensive investigation for decades. While industrial applications are still limited by their low yield (selectivity) and stability issues, innovations in new catalysts and concepts are needed. The newly emerging strategy using iron single sites to catalyze methane conversion to olefins, aromatics, and hydrogen (MTOAH) attracted much attention when it was reported. Because the challenge lies in controlled dehydrogenation of the highly stable CH 4 and selective C-C coupling, we focus mainly on the fundamentals of C-H activation and analyze the reaction pathways toward selective routes of OCM, MDA, and MTOAH. With this, we intend to provide some insights into their reaction mechanisms and implications for future development of highly selective catalysts for direct conversion of methane to high value-added chemicals.
Hydrogen generator, via catalytic partial oxidation of methane for fuel cells
NASA Astrophysics Data System (ADS)
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.
Evaluating host-associated sources of marine methane supersaturation
NASA Astrophysics Data System (ADS)
Blanton, J. M.; Pieper, L. M.; Allen, E. E.
2013-12-01
Methane can be found in surface ocean waters at levels from 5% to 75% greater than expected from exchange with the atmosphere. Because oceanic emissions account for up to 4% of the planet's annual methane inventory, understanding marine sources and sinks is relevant to global greenhouse gas budgets. These methane levels are presumed to result from the activity of microorganisms in the water column, yet this presents a paradox: how can biotic methanogensis, primarily understood as an anaerobic process, take place in oxic waters? One working theory is that methanogens find safe harbor in the gastrointestinal tracts of marine animals. We investigate the possibility that microbial communities within fish, and the fecal material they produce, contribute to in-situ methane production in the open ocean. Using genetic markers, we test the GI tracts of benthic and pelagic marine teleosts for the presence of methanogenic organisms and for components of the methanogenesis pathway. Our results indicate that methanogens may be present in fish, but in low numbers. This work sets the scene for measurement of methane production rates from these gut-associated communities in order to elucidate their contribution to oceanic methane supersaturation.
NASA Astrophysics Data System (ADS)
Omara, M.; Subramanian, R.; Sullivan, M.; Robinson, A. L.; Presto, A. A.
2014-12-01
The Marcellus Shale is the most expansive shale gas reserve in play in the United States, representing an estimated 17 to 29 % of the total domestic shale gas reserves. The rapid and extensive development of this shale gas reserve in the past decade has stimulated significant interest and debate over the climate and environmental impacts associated with fugitive releases of methane and other pollutants, including volatile organic compounds. However, the nature and magnitude of these pollutant emissions remain poorly characterized. This study utilizes the tracer release technique to characterize total fugitive methane release rates from natural gas facilities in southwestern Pennsylvania and West Virginia that are at different stages of development, including well completion flowbacks and active production. Real-time downwind concentrations of methane and two tracer gases (acetylene and nitrous oxide) released onsite at known flow rates were measured using a quantum cascade tunable infrared laser differential absorption spectrometer (QC-TILDAS, Aerodyne, Billerica, MA) and a cavity ring down spectrometer (Model G2203, Picarro, Santa Clara, CA). Evacuated Silonite canisters were used to sample ambient air during downwind transects of methane and tracer plumes to assess volatile organic compounds (VOCs). A gas chromatograph with a flame ionization detector was used to quantify VOCs following the EPA Method TO-14A. A preliminary assessment of fugitive emissions from actively producing sites indicated that methane leak rates ranged from approximately 1.8 to 6.2 SCFM, possibly reflecting differences in facility age and installed emissions control technology. A detailed comparison of methane leak rates and VOCs emissions with recent published literature for other US shale gas plays will also be discussed.
NASA Astrophysics Data System (ADS)
Orcutt, B.; Meile, C.
2008-11-01
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.
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.
Alain, Karine; Holler, Thomas; Musat, Florin; Elvert, Marcus; Treude, Tina; Krüger, Martin
2006-04-01
Paclele Mici is a terrestrial mud volcano field located in the Carpathian Mountains (Romania), where thermal alteration of sedimentary organic compounds leads to methane, higher hydrocarbons and other petroleum compounds that are continuously released into the environment. The hydrocarbons represent potential substrates for microorganisms. We studied lipid biomarkers, stable isotope ratios, the effect of substrate (methane, other organic compounds) addition and 16S rRNA genes to gain insights into the hitherto unknown microbial community at this site. Quantitative real-time polymerase chain reaction analysis demonstrated that bacteria were much more abundant than archaea. Phylogenetic analyses of 16S rDNA clone sequences indicated the presence of bacterial and archaeal lineages generally associated with the methane cycle (methanogens, aerobic and anaerobic methanotrophs), the sulfur cycle (sulfate reducers), and groups linked to the anaerobic degradation of alkanes or aromatic hydrocarbons. The presence of sulfate reducers, methanogens and methanotrophs in this habitat was also confirmed by concurrent surveys of lipid biomarkers and their isotopic signatures. Incubation experiments with several common and complex substrates revealed the potential of the indigenous microbial community for sulfate reduction, methanogenesis and aerobic methanotrophy. Additionally, consistently to the detection of methane-oxidizing archaea (ANME) and 13C-depleted archaeal lipids, a weak but significant activity of anaerobic methane oxidation was measured by radiotracer techniques and in vitro. This survey is the first to report the presence and activity of ANME in a terrestrial environment.
Anaerobic oxidation of methane coupled to thiosulfate reduction in a biotrickling filter.
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.
Li, Huishu; Carlson, Kenneth H
2014-01-01
Public concerns over potential environmental contamination associated with oil and gas well drilling and fracturing in the Wattenberg field in northeast Colorado are increasing. One of the issues of concern is the migration of oil, gas, or produced water to a groundwater aquifer resulting in contamination of drinking water. Since methane is the major component of natural gas and it can be dissolved and transported with groundwater, stray gas in aquifers has elicited attention. The initial step toward understanding the environmental impacts of oil and gas activities, such as well drilling and fracturing, is to determine the occurrence, where it is and where it came from. In this study, groundwater methane data that has been collected in response to a relatively new regulation in Colorado is analyzed. Dissolved methane was detected in 78% of groundwater wells with an average concentration of 4.0 mg/L and a range of 0-37.1 mg/L. Greater than 95% of the methane found in groundwater wells was classified as having a microbial origin, and there was minimal overlap between the C and H isotopic characterization of the produced gas and dissolved methane measured in the aquifer. Neither density of oil/gas wells nor distance to oil/gas wells had a significant impact on methane concentration suggesting other important factors were influencing methane generation and distribution. Thermogenic methane was detected in two aquifer wells indicating a potential contamination pathway from the producing formation, but microbial-origin gas was by far the predominant source of dissolved methane in the Wattenberg field.
NASA Astrophysics Data System (ADS)
Hu, Yu; Chen, Linying; Feng, Dong; Liang, Qianyong; Xia, Zhen; Chen, Duofu
2017-05-01
Sediments at marine methane seep sites provide potential archives of past fluid flow that serve to explore seepage activities over time. Three gravity cores (D-8, D-F, and D-7) were collected from seep sites on the northern slope of the South China Sea where gas hydrates were drilled in the subsurface. Various carbon and sulfur contents, δ13C values of total inorganic carbon (δ13CTIC), δ34S values of chromium reducible sulfur (δ34SCRS), trace element contents, grain size, and AMS 14C dating of planktonic Foraminifera in the sediments were determined to explore the availability of related proxies at seeps and to trace past methane seepage activities. Evidence for the presence of methane seepage and consequently anaerobic oxidation of methane comes from the occurrence of 13C-depleted authigenic carbonate nodules (δ13C values as low as -49‰) discovered at an interval of 150-200 cm in core D-7. This finding is supported by high S/C ratios and molybdenum enrichment in the same interval. However, low contents of CRS and negative δ34SCRS values are present. It is suggested to reflect a transient methane seepage event, which continued for about 1 ka based on the 14C ages. Cores D-8 and D-F have δ13CTIC values close to zero, low S/C ratios and CRS contents, negative δ34SCRS values, and no trace element enrichment, suggesting a negligible impact of methane-seepage on the sediments. The negative δ34SCRS values of the studied seep-impacted and background sediments suggest that the application of δ34SCRS alone as a proxy to identify AOM-related process may be insufficient. Sediment carbon-sulfur-trace element systematics and 14C ages used here have the potential to be a promising tool to recognize transient methane seepages and constrain their timescales.
Amha, Yamrot M; Sinha, Pooja; Lagman, Jewls; Gregori, Matt; Smith, Adam L
2017-10-15
Despite growing interest in co-digestion and demonstrated process improvements (e.g., enhanced stability and biogas production), few studies have evaluated how co-digestion impacts the anaerobic digestion (AD) microbiome. Three sequential bench-scale respirometry experiments were conducted at thermophilic temperature (50 °C) with various combinations of primary sludge (PS); thickened waste activated sludge (TWAS); fats, oils, and grease (FOG); and food waste (FW). Two additional runs were then performed to evaluate microbial inhibition at higher organic fractions of FOG (30-60% volatile solids loading (VSL; v/v)). Co-digestion of PS, TWAS, FOG, and FW resulted in a 26% increase in methane production relative to digestion of PS and TWAS. A substantial lag time was observed in biogas production for vessels with FOG addition that decreased by more than half in later runs, likely due to adaptation of the microbial community. 30% FOG with 10% FW showed the highest increase in methane production, increasing 53% compared to digestion of PS and TWAS. FOG addition above 50% VSL was found to be inhibitory with and without FW addition and resulted in volatile fatty acid (VFA) accumulation. Methane production was linked with high relative activity and abundance of syntrophic fatty-acid oxidizers alongside hydrogenotrophic methanogens, signaling the importance of interspecies interactions in AD. Specifically, relative activity of Syntrophomonas was significantly correlated with methane production. Further, methane production increased over subsequent runs along with methyl coenzyme M reductase (mcrA) gene expression, a functional gene in methanogens, suggesting temporal adaptation of the microbial community to co-digestion substrate mixtures. The study demonstrated the benefits of co-digestion in terms of performance enhancement and enrichment of key active microbial populations. Copyright © 2017 Elsevier Ltd. All rights reserved.
NASA Astrophysics Data System (ADS)
DongHun, Lee; YoungKeun, Jin; JungHyun, Kim; Heldge, Niemann; JongKu, Gal; BoHyung, Choi
2016-04-01
Based on the water column acoustic anomalies related to active methane (CH4) venting, numerous active Mud Volcanoes (MVs) were recently identified at ~282, ~420, and ~740 m water depths on the continental slope of the Canadian Beaufort Sea (Paull et al., 2015). While geophysical aspects such as the multibeam bathymetric mapping are thoroughly investigated, biogeochemical processes controlling outgassing CH4 at the active MVs are not well constrained. Here, we investigated three sediment cores from the active MVs and one sediment core from a non-methane influenced reference site recovered during the ARA-05C expedition with the R/V ARAON in 2014. We analyzed lipid biomarkers and their stable carbon isotopic values (δ13C) in order to determine key biogeochemical processes involved in CH4 cycling in the MV sediments. Downcore CH4 and sulphate (SO42-) concentration measurements revealed a distinct sulfate-methane transition zone (SMTZ) at the shallow sections of the cores (15 - 45 cm below seafloor (cm bsf) at 282 m MV, 420 m MV, and 740 m MV). The most abundant diagnostic lipid biomarkers in the SMTZ were sn-2-hydroxyarchaeol (-94‰) and archaeol (-66‰) with the sn-2-hydroxyarchaeol: archaeol ratio of 1.1 to 5, indicating the presence of ANME-2 or -3. However, we also found substantial amounts of monocyclic biphytane-1 (BP-1, -118‰), which is rather indicative for ANME-1. Nevertheless, the concentration of sn-2-hydroxyarchaeol was 2-fold higher than any other archaeal lipids, suggesting a predominant ANME-2 or -3 rather than ANME-1 as a driving force for the anaerobic methane oxidation (AOM) in these systems. We will further investigate the microbial community at the active MVs using nucleic acid (RNA and DNA) sequence analyses in near future. Our study provides first biogeochemical data set of the active MVs in the Canadian Beaufort Sea, which helps to better understand CH4 cycling mediated in these systems. Reference Paull, C.K., et al. (2015), Active mud volcanoes on the continental slope of the Canadian Beaufort Sea. Geochemistry, Geophysics, Geosystems 16, doi:10.1002/2015GC005928.
METHANE EMISSIONS FROM THE NATURAL GAS INDUSTRY VOLUME 5: ACTIVITY FACTORS
The 15-volume report summarizes the results of a comprehensive program to quantify methane (CH4) emissions from the U.S. natural gas industry for the base year. The objective was to determine CH4 emissions from the wellhead and ending downstream at the customer's meter. The accur...
Performance and Stability Analyses of Rocket Thrust Chambers with Oxygen/Methane Propellants
NASA Technical Reports Server (NTRS)
Hulka, James R.; Jones, Gregg W.
2010-01-01
Liquid rocket engines using oxygen and methane propellants are being considered by the National Aeronautics and Space Administration (NASA) for future in-space vehicles. This propellant combination has not been previously used in flight-qualified engine systems developed by NASA, so limited test data and analysis results are available at this stage of early development. As part of activities for the Propulsion and Cryogenic Advanced Development (PCAD) project funded under the Exploration Technology Development Program, the NASA Marshall Space Flight Center (MSFC) has been evaluating capability to model combustion performance and stability for oxygen and methane propellants. This activity has been proceeding for about two years and this paper is a summary of results to date. Hot-fire test results of oxygen/methane propellant rocket engine combustion devices for the modeling investigations have come from several sources, including multi-element injector tests with gaseous methane from the 1980s, single element tests with gaseous methane funded through the Constellation University Institutes Program, and multi-element injector tests with both gaseous and liquid methane conducted at the NASA MSFC funded by PCAD. For the latter, test results of both impinging and coaxial element injectors using liquid oxygen and liquid methane propellants are included. Configurations were modeled with two one-dimensional liquid rocket combustion analysis codes, the Rocket Combustor Interactive Design and Analysis code and the Coaxial Injector Combustion Model. Special effort was focused on how these codes can be used to model combustion and performance with oxygen/methane propellants a priori, and what anchoring or calibrating features need to be applied, improved or developed in the future. Low frequency combustion instability (chug) occurred, with frequencies ranging from 150 to 250 Hz, with several multi-element injectors with liquid/liquid propellants, and was modeled using techniques from Wenzel and Szuch. High-frequency combustion instability also occurred at the first tangential (1T) mode, at about 4500 Hz, with several multi-element injectors with liquid/liquid propellants. Analyses of the transverse mode instability were conducted by evaluating injector resonances and empirical methods developed by Hewitt.
NASA Astrophysics Data System (ADS)
Silyakova, A.; Jansson, P.; Serov, P.; Graves, C. A.; Niemann, H.; Grundger, F.; Ferre, B.; Mienert, J.
2016-02-01
The area west of Prins Karls Forland (PKF, West Spitsbergen) in the Arctic Ocean, restricted to 90 m water depth, is known for a large amount of shallow active gas flares. Gas flares are streams of bubbles that contain mostly methane, which is a potent greenhouse gas. The important questions for many areas with discovered gas flares are: Does this gas reach the atmosphere? What controls the vertical and horizontal distribution of dissolved methane away from the source on the seafloor? Is all dissolved methane detected above gas flares released from those flares or does it partially originate from other areas (eg. Storfjorden, or area of deeper flares on the PKF slope)? The present study is based on two repeated oceanographic surveys conducted in the summers of 2014 and 2015. During the surveys, we sampled 64 CTD stations in a grid above a 30 x 15 km area with active methane flares. Vertical profiles of temperature (T) and salinity (S), as well as TS diagrams indicate very different oceanographic settings during the two surveys. Warm and saline Atlantic waters originating from the West Spitsbergen Current prevailed during the 2014 campaign. In 2015, in contrast, waters were distinctly less saline and cooler. These waters originate from the East-Spitsbergen current that flows northwards over the shelf from the Barents Sea around the southern tip of Spitsbergen. The water mass was furthermore influenced by local sources from the fjords. In both years, we observed strong vertical gradients in the distribution of dissolved methane in the water column above gas flares, with only 4% methane concentrations at the sea surface when compared to bottom waters. However, the circulation of the dominant water masses mainly controlled the horizontal distribution of methane in the water column in the specific year. We discuss oceanographic processes and mechanisms responsible for methane transport and transformation in the study area. This study is funded by CAGE (Centre for Arctic Gas Hydrate, Environment and Climate), Norwegian Research Council grant no. 223259.
MERLIN: a Franco-German LIDAR space mission for atmospheric methane
NASA Astrophysics Data System (ADS)
Bousquet, P.; Ehret, G.; Pierangelo, C.; Marshall, J.; Bacour, C.; Chevallier, F.; Gibert, F.; Armante, R.; Crevoisier, C. D.; Edouart, D.; Esteve, F.; Julien, E.; Kiemle, C.; Alpers, M.; Millet, B.
2017-12-01
The Methane Remote Sensing Lidar Mission (MERLIN), currently in phase C, is a joint cooperation between France and Germany on the development, launch and operation of a space LIDAR dedicated to the retrieval of total weighted methane (CH4) atmospheric columns. Atmospheric methane is the second most potent anthropogenic greenhouse gas, contributing 20% to climate radiative forcing but also plying an important role in atmospheric chemistry as a precursor of tropospheric ozone and low-stratosphere water vapour. Its short lifetime ( 9 years) and the nature and variety of its anthropogenic sources also offer interesting mitigation options in regards to the 2° objective of the Paris agreement. For the first time, measurements of atmospheric composition will be performed from space thanks to an IPDA (Integrated Path Differential Absorption) LIDAR (Light Detecting And Ranging), with a precision (target ±27 ppb for a 50km aggregation along the trace) and accuracy (target <3.7 ppb at 68%) sufficient to significantly reduce the uncertainties on methane emissions. The very low targeted systematic error target is particularly ambitious compared to current passive methane space mission. It is achievable because of the differential active measurements of MERLIN, which guarantees almost no contamination by aerosols or water vapour cross-sensitivity. As an active mission, MERLIN will deliver global methane weighted columns (XCH4) for all seasons and all latitudes, day and night Here, we recall the MERLIN objectives and mission characteristics. We also propose an end-to-end error analysis, from the causes of random and systematic errors of the instrument, of the platform and of the data treatment, to the error on methane emissions. To do so, we propose an OSSE analysis (observing system simulation experiment) to estimate the uncertainty reduction on methane emissions brought by MERLIN XCH4. The originality of our inversion system is to transfer both random and systematic errors from the observation space to the flux space, thus providing more realistic error reductions than usually provided in OSSE only using the random part of errors. Uncertainty reductions are presented using two different atmospheric transport models, TM3 and LMDZ, and compared with error reduction achieved with the GOSAT passive mission.
Sources and sinks of methane beneath polar ice
NASA Astrophysics Data System (ADS)
Priscu, J. C.; Adams, H. E.; Hand, K. P.; Dore, J. E.; Matheus-Carnevali, P.; Michaud, A. B.; Murray, A. E.; Skidmore, M. L.; Vick-Majors, T.
2014-12-01
Several icy moons of the outer solar system carry subsurface oceans containing many times the volume of liquid water on Earth and may provide the greatest volume of habitable space in our solar system. Functional sub-ice polar ecosystems on Earth provide compelling models for the habitability of extraterrestrial sub-ice oceans. A key feature of sub-ice environments is that most of them receive little to no solar energy. Consequently, organisms inhabiting these environments must rely on chemical energy to assimilate either carbon dioxide or organic molecules to support their metabolism. Methane can be utilized by certain bacteria as both a carbon and energy source. Isotopic data show that methane in Earth's polar lakes is derived from both biogenic and thermogenic sources. Thermogenic sources of methane in the thermokarst lakes of the north slope of Alaska yield supersaturated water columns during winter ice cover that support active populations of methanotrophs during the polar night. Methane in the permanently ice-covered lakes of the McMurdo Dry Valleys, Antarctica varies widely in concentration and is produced either by contemporary methanogenesis or is a relic from subglacial flow. Rate measurements revealed that microbial methane oxidation occurs beneath the ice in both the arctic and Antarctic lakes. The first samples collected from an Antarctic subglacial environment beneath 800 m of ice (Subglacial Lake Whillans) revealed an active microbial ecosystem that has been isolated from the atmosphere for many thousands of years. The sediments of Lake Whillans contained high levels of methane with an isotopic signature that indicates it was produced via methanogenesis. The source of this methane appears to be from the decomposition of organic carbon deposited when this region of Antarctica was covered by the sea. Collectively, data from these sub-ice environments show that methane transformations play a key role in microbial community metabolism. The discovery of functional microbial ecosystems in Earth's sub-ice aquatic environments together with what we know about the geochemistry of extraterrestrial ice-covered water worlds provide a compelling case that sub-ice oceans, such as those on Europa and Enceladus, may support microbial life.
Zheng, Xiong; Wu, Lijuan; Chen, Yinguang; Su, Yinglong; Wan, Rui; Liu, Kun; Huang, Haining
2015-01-01
Anaerobic co-digestion of primary and excess sludge is regarded as an efficient way to reuse sludge organic matter to produce methane. In this study, short-term and long-term exposure experiments were conducted to investigate the possible effects of titanium dioxide (TiO2) and zinc oxide (ZnO) nanoparticles (NPs) on methane production from anaerobic co-digestion of primary and excess sludge. The data showed that TiO2 NPs had no measurable impact on methane production, even at a high concentration (150 mg/g total suspended solids (TSS)). However, short-term (8 days) exposure to 30 or 150 mg/g-TSS of ZnO NPs significantly decreased methane production. More importantly, these negative effects of ZnO NPs on anaerobic sludge co-digestion were not alleviated by increasing the adaptation time to 105 days. Further studies indicated that the presence of ZnO NPs substantially decreased the abundance of methanogenic archaea, which reduced methane production. Meanwhile, the activities of some key enzymes involved in methane production, such as protease, acetate kinase, and coenzyme F420, were remarkably inhibited by the presence of ZnO NPs, which was also an important reason for the decreased methane production. These results provide a better understanding of the potential risks of TiO2 and ZnO NPs to methane production from anaerobic sludge co-digestion.
DOE Office of Scientific and Technical Information (OSTI.GOV)
Fields, Matthew
Currently, coal bed methane (CBM) wells have a limited lifetime since the rate of methane removal via the installed wells is much faster than the in situ methane production rates. Along with water issues created by large amounts of CBM production water, the short life span of CBM wells is a huge deterrent to the environmental and economic feasibility of CBM production. The process of biogenic methanogenesis can be enhanced via the stimulation of the associated microbial communities that can convert the organic fractions of coal to methane. This process is termed Microbially-Enhanced Coal Bed Methane (MECBM). However, the ratesmore » of methane production are still limited and long incubation times are necessary. We hypothesized that the elucidation of chemical and biological parameters that limited MECBM together with thermodynamic considerations would inform strategies to optimize the process under flow conditions. We incorporated microbiological, physicochemical, and engineering processes to develop a more sustainable CBM production scheme with native coal and native microorganisms. The proposed combination of microbial ecology and physiology as well as optimized engineering principles minimized key constraints that impact microbial coal conversion to methane under environmentally relevant conditions. The combined approach for bench-scale tests resulted in more effective and less environmentally burdensome coal-dependent methane production with the potential for H 2O and CO 2 management.« less
Methane Production and Methanogenic Archaea in the Digestive Tracts of Millipedes (Diplopoda)
Šustr, Vladimír; Chroňáková, Alica; Semanová, Stanislava; Tajovský, Karel; Šimek, Miloslav
2014-01-01
Methane production by intestinal methanogenic Archaea and their community structure were compared among phylogenetic lineages of millipedes. Tropical and temperate millipedes of 35 species and 17 families were investigated. Species that emitted methane were mostly in the juliform orders Julida, Spirobolida, and Spirostreptida. The irregular phylogenetic distribution of methane production correlated with the presence of the methanogen-specific mcrA gene. The study brings the first detailed survey of methanogens’ diversity in the digestive tract of millipedes. Sequences related to Methanosarcinales, Methanobacteriales, Methanomicrobiales and some unclassified Archaea were detected using molecular profiling (DGGE). The differences in substrate preferences of the main lineages of methanogenic Archaea found in different millipede orders indicate that the composition of methanogen communities may reflect the differences in available substrates for methanogenesis or the presence of symbiotic protozoa in the digestive tract. We conclude that differences in methane production in the millipede gut reflect differences in the activity and proliferation of intestinal methanogens rather than an absolute inability of some millipede taxa to host methanogens. This inference was supported by the general presence of methanogenic activity in millipede faecal pellets and the presence of the 16S rRNA gene of methanogens in all tested taxa in the two main groups of millipedes, the Helminthophora and the Pentazonia. PMID:25028969
Hatzenpichler, Roland; Connon, Stephanie A.; Goudeau, Danielle; Malmstrom, Rex R.; Woyke, Tanja; Orphan, Victoria J.
2016-01-01
To understand the biogeochemical roles of microorganisms in the environment, it is important to determine when and under which conditions they are metabolically active. Bioorthogonal noncanonical amino acid tagging (BONCAT) can reveal active cells by tracking the incorporation of synthetic amino acids into newly synthesized proteins. The phylogenetic identity of translationally active cells can be determined by combining BONCAT with rRNA-targeted fluorescence in situ hybridization (BONCAT-FISH). In theory, BONCAT-labeled cells could be isolated with fluorescence-activated cell sorting (BONCAT-FACS) for subsequent genetic analyses. Here, in the first application, to our knowledge, of BONCAT-FISH and BONCAT-FACS within an environmental context, we probe the translational activity of microbial consortia catalyzing the anaerobic oxidation of methane (AOM), a dominant sink of methane in the ocean. These consortia, which typically are composed of anaerobic methane-oxidizing archaea (ANME) and sulfate-reducing bacteria, have been difficult to study due to their slow in situ growth rates, and fundamental questions remain about their ecology and diversity of interactions occurring between ANME and associated partners. Our activity-correlated analyses of >16,400 microbial aggregates provide the first evidence, to our knowledge, that AOM consortia affiliated with all five major ANME clades are concurrently active under controlled conditions. Surprisingly, sorting of individual BONCAT-labeled consortia followed by whole-genome amplification and 16S rRNA gene sequencing revealed previously unrecognized interactions of ANME with members of the poorly understood phylum Verrucomicrobia. This finding, together with our observation that ANME-associated Verrucomicrobia are found in a variety of geographically distinct methane seep environments, suggests a broader range of symbiotic relationships within AOM consortia than previously thought. PMID:27357680
Hatzenpichler, Roland; Connon, Stephanie A.; Goudeau, Danielle; ...
2016-06-28
To understand the biogeochemical roles of microorganisms in the environment, it is important to determine when and under which conditions they are metabolically active. Bioorthogonal noncanonical amino acid tagging (BONCAT) can reveal active cells by tracking the incorporation of synthetic amino acids into newly synthesized proteins. The phylogenetic identity of translationally active cells can be determined by combining BONCAT with rRNA-targeted fluorescence in situ hybridization (BONCAT-FISH). In theory, BONCAT-labeled cells could be isolated with fluorescence-activated cell sorting (BONCAT-FACS) for subsequent genetic analyses. Here, in the first application, to our knowledge, of BONCAT-FISH and BONCAT-FACS within an environmental context, we probemore » the translational activity of microbial consortia catalyzing the anaerobic oxidation of methane (AOM), a dominant sink of methane in the ocean. These consortia, which typically are composed of anaerobic methane-oxidizing archaea (ANME) and sulfate-reducing bacteria, have been difficult to study due to their slow in situ growth rates, and fundamental questions remain about their ecology and diversity of interactions occurring between ANME and associated partners. Our activity-correlated analyses of > 16,400 microbial aggregates provide the first evidence, to our knowledge, that AOM consortia affiliated with all five major ANME clades are concurrently active under controlled conditions. Surprisingly, sorting of individual BONCAT-labeled consortia followed by whole-genome amplification and 16S rRNA gene sequencing revealed previously unrecognized interactions of ANME with members of the poorly understood phylum Verrucomicrobia. This finding, together with our observation that ANME-associated Verrucomicrobia are found in a variety of geographically distinct methane seep environments, suggests a broader range of symbiotic relationships within AOM consortia than previously thought.« less
DOE Office of Scientific and Technical Information (OSTI.GOV)
Hatzenpichler, Roland; Connon, Stephanie A.; Goudeau, Danielle
To understand the biogeochemical roles of microorganisms in the environment, it is important to determine when and under which conditions they are metabolically active. Bioorthogonal noncanonical amino acid tagging (BONCAT) can reveal active cells by tracking the incorporation of synthetic amino acids into newly synthesized proteins. The phylogenetic identity of translationally active cells can be determined by combining BONCAT with rRNA-targeted fluorescence in situ hybridization (BONCAT-FISH). In theory, BONCAT-labeled cells could be isolated with fluorescence-activated cell sorting (BONCAT-FACS) for subsequent genetic analyses. Here, in the first application, to our knowledge, of BONCAT-FISH and BONCAT-FACS within an environmental context, we probemore » the translational activity of microbial consortia catalyzing the anaerobic oxidation of methane (AOM), a dominant sink of methane in the ocean. These consortia, which typically are composed of anaerobic methane-oxidizing archaea (ANME) and sulfate-reducing bacteria, have been difficult to study due to their slow in situ growth rates, and fundamental questions remain about their ecology and diversity of interactions occurring between ANME and associated partners. Our activity-correlated analyses of > 16,400 microbial aggregates provide the first evidence, to our knowledge, that AOM consortia affiliated with all five major ANME clades are concurrently active under controlled conditions. Surprisingly, sorting of individual BONCAT-labeled consortia followed by whole-genome amplification and 16S rRNA gene sequencing revealed previously unrecognized interactions of ANME with members of the poorly understood phylum Verrucomicrobia. This finding, together with our observation that ANME-associated Verrucomicrobia are found in a variety of geographically distinct methane seep environments, suggests a broader range of symbiotic relationships within AOM consortia than previously thought.« less
H2S mediated thermal and photochemical methane activation
Baltrusaitis, Jonas; de Graaf, Coen; Broer, Ria; Patterson, Eric
2013-01-01
Sustainable, low temperature methods of natural gas activation are critical in addressing current and foreseeable energy and hydrocarbon feedstock needs. Large portions of natural gas resources are still too expensive to process due to their high content of hydrogen sulfide gas (H2S) in mixture with methane, CH4, altogether deemed as sub-quality or “sour” gas. We propose a unique method for activating this “sour” gas to form a mixture of sulfur-containing hydrocarbon intermediates, CH3SH and CH3SCH3, and an energy carrier, such as H2. For this purpose, we computationally investigated H2S mediated methane activation to form a reactive CH3SH species via direct photolysis of sub-quality natural gas. Photoexcitation of hydrogen sulfide in the CH4+H2S complex results in a barrier-less relaxation via a conical intersection to form a ground state CH3SH+H2 complex. The resulting CH3SH can further be heterogeneously coupled over acidic catalysts to form higher hydrocarbons while the H2 can be used as a fuel. This process is very different from a conventional thermal or radical-based processes and can be driven photolytically at low temperatures, with enhanced controllability over the process conditions currently used in industrial oxidative natural gas activation. Finally, the proposed process is CO2 neutral, as opposed to the currently industrially used methane steam reforming (SMR). PMID:24150813
NASA Astrophysics Data System (ADS)
Li, X.; Omara, M.; Adams, P. J.; Presto, A. A.
2017-12-01
Methane is the second most powerful greenhouse gas after Carbon Dioxide. The natural gas production and distribution accounts for 23% of the total anthropogenic methane emissions in the United States. The boost of natural gas production in U.S. in recent years poses a potential concern of increased methane emissions from natural gas production and distribution. The Emission Database for Global Atmospheric Research (Edgar) v4.2 and the EPA Greenhouse Gas Inventory (GHGI) are currently the most commonly used methane emission inventories. However, recent studies suggested that both Edgar v4.2 and the EPA GHGI largely underestimated the methane emission from natural gas production and distribution in U.S. constrained by both ground and satellite measurements. In this work, we built a gridded (0.1° Latitude ×0.1° Longitude) methane emission inventory of natural gas production and distribution over the contiguous U.S. using emission factors measured by our mobile lab in the Marcellus Shale, the Denver-Julesburg Basin, and the Uintah Basin, and emission factors reported from other recent field studies for other natural gas production regions. The activity data (well location and count) are mostly obtained from the Drillinginfo, the EPA Greenhouse Gas Reporting Program (GHGRP) and the U.S. Energy Information Administration (EIA). Results show that the methane emission from natural gas production and distribution estimated by our inventory is about 20% higher than the EPA GHGI, and in some major natural gas production regions, methane emissions estimated by the EPA GHGI are significantly lower than our inventory. For example, in the Marcellus Shale, our estimated annual methane emission in 2015 is 600 Gg higher than the EPA GHGI. We also ran the GEOS-Chem methane simulation to estimate the methane concentration in the atmosphere with our built inventory, the EPA GHGI and the Edgar v4.2 over the nested North American Domain. These simulation results showed differences in some major gas production regions. The simulated methane concentrations will be compared with the GOSAT satellite data to explore whether our built inventory could potentially improve the prediction of regional methane concentrations in the atmosphere.
From micelles to bicelles: Effect of the membrane on particulate methane monooxygenase activity.
Ro, Soo Y; Ross, Matthew O; Deng, Yue Wen; Batelu, Sharon; Lawton, Thomas J; Hurley, Joseph D; Stemmler, Timothy L; Hoffman, Brian M; Rosenzweig, Amy C
2018-05-08
Particulate methane monooxygenase (pMMO) is a copper-dependent, integral membrane metalloenzyme that converts methane to methanol in methanotrophic bacteria. Studies of isolated pMMO have been hindered by loss of enzymatic activity upon its removal from the native membrane. To characterize pMMO in a membrane-like environment, we reconstituted pMMOs from Methylococcus ( Mcc. ) capsulatus (Bath) and Methylomicrobium ( Mm. ) alcaliphilum 20Z into bicelles. Reconstitution into bicelles recovers methane oxidation activity lost upon detergent solubilization and purification without substantial alterations to copper content or copper electronic structure as observed by electron paramagnetic resonance (EPR) spectroscopy.. These findings suggest that loss of pMMO activity upon isolation is due to removal from the membranes rather than caused by loss of the catalytic copper ions. A 2.7 Å resolution crystal structure of pMMO from Mm. alcaliphilum 20Z revealed a mononuclear copper center in the PmoB subunit and indicated that the transmembrane PmoC subunit may be conformationally flexible. Finally, results from extended X-ray absorption fine structure (EXAFS) analysis of pMMO from Mm. alcaliphilum 20Z were consistent with the observed monocopper center in the PmoB subunit. These results underscore the importance of studying membrane proteins in a membrane-like environment, and provide valuable insight into pMMO function. Published under license by The American Society for Biochemistry and Molecular Biology, Inc.
NASA Astrophysics Data System (ADS)
Naudts, L.; Khlystov, O.; Khabuev, A.; Seminskiy, I.; Casier, R.; Cuylaerts, M.; 'chenko, P., General; Synaeve, J.; Vlamynck, N.; de Batist, M. A.; Grachev, M. A.
2009-12-01
Lake Baikal is a large rift lake in Southern Siberia (Russian Federation). It occupies the three central depressions of the Baikal Rift Zone (BRZ): i.e. the Southern, Central and Northern Baikal Basins. Rifting started ca. 30 Ma ago and is still active with a present-day average extension rate of about 4 mm/yr. With a depth of 1637 m, Lake Baikal is the deepest lake in the World. It also holds 20 % of the world’s liquid surface fresh water, which makes it the largest lake in the World in terms of volume. Lake Baikal is also the only freshwater lake in the World with demonstrated occurrences of gas hydrates in its sedimentary infill. Methane hydrates are stable at water depths below 375 m. The presence of hydrates in the sedimentary infill is evidenced by a widespread BSR. Hydrates have also been encountered locally, in the near-bottom sediments of mud-volcano-like structures. In the summer of 2009, the lake floor has been mapped with multibeam swath bathymetry for the first time during a two-month-long survey with RV Titov. Swath bathymetry data were acquired with RCMG’s mobile 50 kHz SeaBeam 1050 multibeam system. In total 12600 km of echosounder tracks were sailed covering 15000 km2, including the Academician Ridge Accommodation Zone, the Central Baikal Basin, the Selenga Delta Accommodation Zone en the South Baikal Basin. In general, the lake floor was mapped starting from water depths of about -200 m to -1637 m, with an average survey depth of -1000 m. The new bathymetric data image the lake-floor morphology in unprecedented detail, revealing many small- and large-scall morphosedimentary, morphostructural and fluid-flow-related features, many of which were hitherto unknown. Known mud-volcano provinces in the Southern and Central Baikal Basins (i.e. the Posolsky Bank mud-volcano province, the Kukuy Canyon mud volcano province and the Olkhon Gate mud-volcano province) were mapped in detail, and several new, often isolated, mud-volcano-like structures were discovered. In addition, different possible fluid-flow features were identified in front of the Selenga Delta. Also the gas-hydrate-bearing areas around the oil seeps of Gorevoi Utes and the methane seeps of Goloustnoye have been mapped in detail, revealing that these hydrate occurrences are not associated with mud-volcano-like structures. The multibeam mapping survey coincided with the 2nd season of exploration of the lake floor by manned MIR submersibles (http://baikalfund.ru/eng/projects/expedition/index.wbp). Several of the MIR dives focused on features imaged by the new bathymetry data, such as gas-hydrate occurrences at methane seeps and oil seeps and in the mud-volcano-like structures, and gas seeps and fluid-flow phenomena along active fault scarps. The multibeam mapping survey was conducted in the framework of SBRAS project 17.8 and FWO Flanders project 1.5.198.09.
Sources, extent and history of methane seepage on the continental shelf off northern Norway
NASA Astrophysics Data System (ADS)
Sauer, Simone; Lepland, Aivo; Chand, Shyam; Schubert, Carsten J.; Eichinger, Florian; Knies, Jochen
2014-05-01
Active natural hydrocarbon gas seepage was recently discovered in the Hola area on the continental shelf off Vesterålen, northern Norway. We conducted acoustic and geochemical investigations to assess the modern and past extent, source and pathways of the gas seepage . Water column echosounder surveys showed bubble plumes up to several tens of metres above the seafloor. Analyses of dissolved methane in the water column indicated slightly elevated concentrations (50 nM) close to the seafloor. To identify fluxes and origin of methane in the sediments we analysed sediment pore water chemistry, the isotopic composition of methane and of dissolved inorganic carbon (d13CCH4, d2HCH4, d13CDIC) in three closely spaced (
BOREAS TE-1 CH4 Flux Data Over The SSA-OA
NASA Technical Reports Server (NTRS)
Anderson, Darwin; Papagno, Andrea; Hall, Forrest G. (Editor); Newcomer, Jeffrey A. (Editor)
2000-01-01
The BOREAS TE-1 team collected various data to characterize the soil-plant systems in the BOREAS SSA. Particular emphasis was placed on nutrient biochemistry, the stores and transfers of organic carbon, and how the characteristics were related to measured methane fluxes. The overall transect in the Prince Albert National Park (Saskatchewan, Canada) included the major plant communities and related soils that occurred in that section of the boreal forest. Soil physical, chemical, and biological measurements along the transect were used to characterize the static environment, which allowed them to be related to methane fluxes. Chamber techniques were used to provide a measure of methane production/uptake. Chamber measurements coupled with flask sampling were used to determine the seasonality of methane fluxes. This particular data set contains methane flux and soil profile methane concentration values from the SSA-OA site. The data were collected from 29-May to 17-Sep-1994. The data are stored in tabular ASCII files. The data files are available on a CD-ROM (see document number 20010000884), or from the Oak Ridge National Laboratory (ORNL) Distributed Active Archive Center (DAAC).
NASA Astrophysics Data System (ADS)
Cao, Y.; Cervone, G.; Barkley, Z.; Lauvaux, T.; Deng, A.; Miles, N.; Richardson, S.
2016-12-01
Fugitive methane emission rates for the Marcellus shale area are estimated using a genetic algorithm that finds optimal weights to minimize the error between simulated and observed concentrations. The overall goal is to understand the relative contribution of methane due to Shale gas extraction. Methane sensors were installed on four towers located in northeastern Pennsylvania to measure atmospheric concentrations since May 2015. Inverse Lagrangian dispersion model runs are performed from each of these tower locations for each hour of 2015. Simulated methane concentrations at each of the four towers are computed by multiplying the resulting footprints from the atmospheric simulations by thousands of emission sources grouped into 11 classes. The emission sources were identified using GIS techniques, and include conventional and unconventional wells, different types of compressor stations, pipelines, landfills, farming and wetlands. Initial estimates for each source are calculated based on emission factors from EPA and few regional studies. A genetic algorithm is then used to identify optimal emission rates for the 11 classes of methane emissions and to explore extreme events and spatial and temporal structures in the emissions associated with natural gas activities.
A post-Cassini view of Titan's methane-based hydrologic cycle
NASA Astrophysics Data System (ADS)
Hayes, Alexander G.; Lorenz, Ralph D.; Lunine, Jonathan I.
2018-05-01
The methane-based hydrologic cycle on Saturn's largest moon, Titan, is an extreme analogue to Earth's water cycle. Titan is the only planetary body in the Solar System, other than Earth, that is known to have an active hydrologic cycle. With a surface pressure of 1.5 bar and temperatures of 90 to 95 K, methane and ethane condense out of a nitrogen-based atmosphere and flow as liquids on the moon's surface. Exchange processes between atmospheric, surface and subsurface reservoirs produce methane and ethane cloud systems, as well as erosional and depositional landscapes that have strikingly similar forms to their terrestrial counterparts. Over its 13-year exploration of the Saturn system, the Cassini-Huygens mission revealed that Titan's hydrocarbon-based hydrology is driven by nested methane cycles that operate over a range of timescales, including geologic, orbital (for example, Croll-Milankovitch cycles), seasonal and that of a single convective storm. In this Review Article, we describe the dominant exchange processes that operate over these timescales and present a post-Cassini view of Titan's methane-based hydrologic system.