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

Warren, B.K.; Campbell, K.D.

Methane oxidative coupling studies were carried out in an atmospheric quartz reactor at temperatures between 700 and 800/degree/C. New catalysts prepared and studied included doped alkaline earth catalysts, lanthanide oxides, and proprietary catalysts. Neodymium oxide, Nd/sub 2/O/sub 3/, was found to be as active and selective as samarium oxide, Sm/sub 2/O/sub 3/, in contrast to literature reports. Proprietary Union Carbide catalysts (UCC-S:1) showed initial methane conversions and C/sub 2/ selectivities comparable to literature catalysts. Atypically low carbon dioxide to carbon monoxide ratios (typically ten times lower than those seen in the literature or other catalysts tested) and high ethylene tomore » ethane ratios (3 to 6 compared to typical literature ratios below 1) were obtained. These results are interesting because ethylene is more valuable than ethane and carbon monoxide is more valuable than carbon dioxide. With these UCC-S:1 catalysts, rapid deactivation was coupled with an observed shift in product ratios toward those more typical in the literature. Initial cases for process conceptualization studies were selected. The Comparison Case will consist of the conversion sequence from methane to synthesis gas to methanol to olefins to liquid hydrocarbon fuels. Case 1 will consist of the conversion of methane to ethylene and ethane. Case 2 will be the direct conversion of methane to C/sub 2/'s followed by conversion to liquid hydrocarbon fuels. 7 figs., 18 tabs.« less

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

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

Modeling and Design Optimization of Multifunctional Membrane Reactors for Direct Methane Aromatization

PubMed Central

Fouty, Nicholas J.; Carrasco, Juan C.; Lima, Fernando V.

2017-01-01

Due to the recent increase of natural gas production in the U.S., utilizing natural gas for higher-value chemicals has become imperative. Direct methane aromatization (DMA) is a promising process used to convert methane to benzene, but it is limited by low conversion of methane and rapid catalyst deactivation by coking. Past work has shown that membrane separation of the hydrogen produced in the DMA reactions can dramatically increase the methane conversion by shifting the equilibrium toward the products, but it also increases coke production. Oxygen introduction into the system has been shown to inhibit this coke production while not inhibiting the benzene production. This paper introduces a novel mathematical model and design to employ both methods in a multifunctional membrane reactor to push the DMA process into further viability. Multifunctional membrane reactors, in this case, are reactors where two different separations occur using two differently selective membranes, on which no systems studies have been found. The proposed multifunctional membrane design incorporates a hydrogen-selective membrane on the outer wall of the reaction zone, and an inner tube filled with airflow surrounded by an oxygen-selective membrane in the middle of the reactor. The design is shown to increase conversion via hydrogen removal by around 100%, and decrease coke production via oxygen addition by 10% when compared to a tubular reactor without any membranes. Optimization studies are performed to determine the best reactor design based on methane conversion, along with coke and benzene production. The obtained optimal design considers a small reactor (length = 25 cm, diameter of reaction tube = 0.7 cm) to subvert coke production and consumption of the product benzene as well as a high permeance (0.01 mol/s·m2·atm1/4) through the hydrogen-permeable membrane. This modeling and design approach sets the stage for guiding further development of multifunctional membrane reactor models and designs for natural gas utilization and other chemical reaction systems. PMID:28850068

A modeling approach to direct interspecies electron transfer process in anaerobic transformation of ethanol to methane.

PubMed

Liu, Yiwen; Zhang, Yaobin; Zhao, Zhiqiang; Ngo, Huu Hao; Guo, Wenshan; Zhou, Junliang; Peng, Lai; Ni, Bing-Jie

2017-01-01

Recent studies have shown that direct interspecies electron transfer (DIET) plays an important part in contributing to methane production from anaerobic digestion. However, so far anaerobic digestion models that have been proposed only consider two pathways for methane production, namely, acetoclastic methanogenesis and hydrogenotrophic methanogenesis, via indirect interspecies hydrogen transfer, which lacks an effective way for incorporating DIET into this paradigm. In this work, a new mathematical model is specifically developed to describe DIET process in anaerobic digestion through introducing extracellular electron transfer as a new pathway for methane production, taking anaerobic transformation of ethanol to methane as an example. The developed model was able to successfully predict experimental data on methane dynamics under different experimental conditions, supporting the validity of the developed model. Modeling predictions clearly demonstrated that DIET plays an important role in contributing to overall methane production (up to 33 %) and conductive material (i.e., carbon cloth) addition would significantly promote DIET through increasing ethanol conversion rate and methane production rate. The model developed in this work will potentially enhance our current understanding on syntrophic metabolism via DIET.

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

Bovine Host Genetic Variation Influences Rumen Microbial Methane Production with Best Selection Criterion for Low Methane Emitting and Efficiently Feed Converting Hosts Based on Metagenomic Gene Abundance

PubMed Central

Roehe, Rainer; Dewhurst, Richard J.; Duthie, Carol-Anne; Rooke, John A.; McKain, Nest; Ross, Dave W.; Hyslop, Jimmy J.; Waterhouse, Anthony; Freeman, Tom C.

2016-01-01

Methane produced by methanogenic archaea in ruminants contributes significantly to anthropogenic greenhouse gas emissions. The host genetic link controlling microbial methane production is unknown and appropriate genetic selection strategies are not developed. We used sire progeny group differences to estimate the host genetic influence on rumen microbial methane production in a factorial experiment consisting of crossbred breed types and diets. Rumen metagenomic profiling was undertaken to investigate links between microbial genes and methane emissions or feed conversion efficiency. Sire progeny groups differed significantly in their methane emissions measured in respiration chambers. Ranking of the sire progeny groups based on methane emissions or relative archaeal abundance was consistent overall and within diet, suggesting that archaeal abundance in ruminal digesta is under host genetic control and can be used to genetically select animals without measuring methane directly. In the metagenomic analysis of rumen contents, we identified 3970 microbial genes of which 20 and 49 genes were significantly associated with methane emissions and feed conversion efficiency respectively. These explained 81% and 86% of the respective variation and were clustered in distinct functional gene networks. Methanogenesis genes (e.g. mcrA and fmdB) were associated with methane emissions, whilst host-microbiome cross talk genes (e.g. TSTA3 and FucI) were associated with feed conversion efficiency. These results strengthen the idea that the host animal controls its own microbiota to a significant extent and open up the implementation of effective breeding strategies using rumen microbial gene abundance as a predictor for difficult-to-measure traits on a large number of hosts. Generally, the results provide a proof of principle to use the relative abundance of microbial genes in the gastrointestinal tract of different species to predict their influence on traits e.g. human metabolism, health and behaviour, as well as to understand the genetic link between host and microbiome. PMID:26891056

Bovine Host Genetic Variation Influences Rumen Microbial Methane Production with Best Selection Criterion for Low Methane Emitting and Efficiently Feed Converting Hosts Based on Metagenomic Gene Abundance.

PubMed

Roehe, Rainer; Dewhurst, Richard J; Duthie, Carol-Anne; Rooke, John A; McKain, Nest; Ross, Dave W; Hyslop, Jimmy J; Waterhouse, Anthony; Freeman, Tom C; Watson, Mick; Wallace, R John

2016-02-01

Methane produced by methanogenic archaea in ruminants contributes significantly to anthropogenic greenhouse gas emissions. The host genetic link controlling microbial methane production is unknown and appropriate genetic selection strategies are not developed. We used sire progeny group differences to estimate the host genetic influence on rumen microbial methane production in a factorial experiment consisting of crossbred breed types and diets. Rumen metagenomic profiling was undertaken to investigate links between microbial genes and methane emissions or feed conversion efficiency. Sire progeny groups differed significantly in their methane emissions measured in respiration chambers. Ranking of the sire progeny groups based on methane emissions or relative archaeal abundance was consistent overall and within diet, suggesting that archaeal abundance in ruminal digesta is under host genetic control and can be used to genetically select animals without measuring methane directly. In the metagenomic analysis of rumen contents, we identified 3970 microbial genes of which 20 and 49 genes were significantly associated with methane emissions and feed conversion efficiency respectively. These explained 81% and 86% of the respective variation and were clustered in distinct functional gene networks. Methanogenesis genes (e.g. mcrA and fmdB) were associated with methane emissions, whilst host-microbiome cross talk genes (e.g. TSTA3 and FucI) were associated with feed conversion efficiency. These results strengthen the idea that the host animal controls its own microbiota to a significant extent and open up the implementation of effective breeding strategies using rumen microbial gene abundance as a predictor for difficult-to-measure traits on a large number of hosts. Generally, the results provide a proof of principle to use the relative abundance of microbial genes in the gastrointestinal tract of different species to predict their influence on traits e.g. human metabolism, health and behaviour, as well as to understand the genetic link between host and microbiome.

Biocatalytic conversion of methane to methanol as a key step for development of methane-based biorefineries.

PubMed

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.

Biogenic coal-to-methane conversion efficiency decreases after repeated organic amendment

USGS Publications Warehouse

Davis, Katherine J.; Barnhart, Elliott P.; Fields, Matthew W.; Gerlach, Robin

2018-01-01

Addition of organic amendments to coal-containing systems can increase the rate and extent of biogenic methane production for 60–80 days before production slows or stops. Understanding the effect of repeated amendment additions on the rate and extent of enhanced coal-dependent methane production is important if biological coal-to-methane conversion is to be enhanced on a commercial scale. Microalgal biomass was added at a concentration of 0.1 g/L to microcosms with and without coal on days 0, 76, and 117. Rates of methane production were enhanced after the initial amendment but coal-containing treatments produced successively decreasing amounts of methane with each amendment. During the first amendment period, 113% of carbon added as amendment was recovered as methane, whereas in the second and third amendment periods, 39% and 32% of carbon added as amendment was recovered as methane, respectively. Additionally, algae-amended coal treatments produced ∼38% more methane than unamended coal treatments and ∼180% more methane than amended coal-free treatments after one amendment. However, a second amendment addition resulted in only an ∼25% increase in methane production for coal versus noncoal treatments and a third amendment addition resulted in similar methane production in both coal and noncoal treatments. Successive amendment additions appeared to result in a shift from coal-to-methane conversion to amendment-to-methane conversion. The reported results indicate that a better understanding is needed of the potential impacts and efficiencies of repeated stimulation for enhanced coal-to-methane conversion.

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

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

McCormick, R.L.

1995-12-31

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

Methodology to Collect Natural Gas from Methane Hydrate Deposits Using Sunlight: Design of Direct Sunlight Exposure System

NASA Astrophysics Data System (ADS)

Shimada, M.; Shimada, J.; Tsunashima, K.; Aoyama, C.

2017-12-01

Methane hydrate is anticipated to be the unconventional natural gas energy resource. Two types of methane hydrates are known to exist, based on the settings: "shallow" type and "sand layer" type. In comparison, shallow type is considered an advantage due to its high purity and the more simple exploration. However, not much development methods have been made in the area of extraction techniques. Currently, heating and depressurization are used as methods to collect sand layer methane hydrate, but these methods are still under examination and not yet to be implemented. This is probably because fossil fuel is used for the extraction process instead of natural energy. It is necessary to utilize natural energy instead of relying on fossil fuel. This is why sunlight is believed to be the most significant alternative. Solar power generation is commonly used to extract sunlight, but it is said that this process causes extreme energy loss since solar energy converted to electricity requires conversion to heat energy. A new method is contrived to accelerate the decomposition of methane hydrate with direct sunlight utilizing optical fibers. Authors will present details of this new method to collect methane hydrate with direct sunlight exposure.

Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature

PubMed Central

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

Genome-scale metabolic reconstructions and theoretical investigation of methane conversion in Methylomicrobium buryatense strain 5G(B1).

PubMed

de la Torre, Andrea; Metivier, Aisha; Chu, Frances; Laurens, Lieve M L; Beck, David A C; Pienkos, Philip T; Lidstrom, Mary E; Kalyuzhnaya, Marina G

2015-11-25

Methane-utilizing bacteria (methanotrophs) are capable of growth on methane and are attractive systems for bio-catalysis. However, the application of natural methanotrophic strains to large-scale production of value-added chemicals/biofuels requires a number of physiological and genetic alterations. An accurate metabolic model coupled with flux balance analysis can provide a solid interpretative framework for experimental data analyses and integration. A stoichiometric flux balance model of Methylomicrobium buryatense strain 5G(B1) was constructed and used for evaluating metabolic engineering strategies for biofuels and chemical production with a methanotrophic bacterium as the catalytic platform. The initial metabolic reconstruction was based on whole-genome predictions. Each metabolic step was manually verified, gapfilled, and modified in accordance with genome-wide expression data. The final model incorporates a total of 841 reactions (in 167 metabolic pathways). Of these, up to 400 reactions were recruited to produce 118 intracellular metabolites. The flux balance simulations suggest that only the transfer of electrons from methanol oxidation to methane oxidation steps can support measured growth and methane/oxygen consumption parameters, while the scenario employing NADH as a possible source of electrons for particulate methane monooxygenase cannot. Direct coupling between methane oxidation and methanol oxidation accounts for most of the membrane-associated methane monooxygenase activity. However the best fit to experimental results is achieved only after assuming that the efficiency of direct coupling depends on growth conditions and additional NADH input (about 0.1-0.2 mol of incremental NADH per one mol of methane oxidized). The additional input is proposed to cover loss of electrons through inefficiency and to sustain methane oxidation at perturbations or support uphill electron transfer. Finally, the model was used for testing the carbon conversion efficiency of different pathways for C1-utilization, including different variants of the ribulose monophosphate pathway and the serine cycle. We demonstrate that the metabolic model can provide an effective tool for predicting metabolic parameters for different nutrients and genetic perturbations, and as such, should be valuable for metabolic engineering of the central metabolism of M. buryatense strains.

Methane - fuel for the future

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

McGeer, P.; Durbin, E.

1982-01-01

The 20 invited papers presented at the world conference on alternative fuel entitled 'Methane - fuel for the future' form the basis of this book. Papers discuss: the availability of alternative fuels (natural gas, biomass conversion to methane, methane from coal conversion); technological adaptions for alternative fuels (e.g. natural gas fueled engines, methane and diesel engines); commercial experience with alternative fuel programs. (e.g. retailing of methane); and some national programs for alternative fuels. One paper has been abstracted separately.

The conversion of CO 2 to methanol on orthorhombic β-Mo 2C and Cu/β-Mo 2C catalysts: Mechanism for admetal induced change in the selectivity and activity

DOE PAGES

Posada-Pérez, Sergio; Ramírez, Pedro J.; Gutiérrez, Ramón A.; ...

2016-02-01

Here, the conversion of CO 2 into methanol catalyzed by β-Mo 2C and Cu/β-Mo 2C surfaces has been investigated by means of a combined experimental and theoretical study. Experiments have shown the direct activation and dissociation of the CO 2 molecule on bare β-Mo 2C, whereas on Cu/β-Mo 2C, CO 2 must be assisted by hydrogen for its conversion. Methane and CO are the main products on the clean surface and methanol production is lower. However, the deposition of Cu clusters avoids methane formation and increases methanol production even above that corresponding to a model of the technical catalyst. DFTmore » calculations on surface models of both possible C- and Mo-terminations corroborate the experimental observations. Calculations for the clean Mo-terminated surface reveal the existence of two possible routes for methane production (C + 4H → CH 4; CH 3O + 3H → CH 4 + H 2O) which are competitive with methanol synthesis, displaying slightly lower energy barriers. On the other hand, a model for Cu deposited clusters on the Mo-terminated surface points towards a new route for methanol and CO production avoiding methane formation. The new route is a direct consequence of the generation of a Mo 2C–Cu interface. The present experimental and theoretical results entail the interesting catalytic properties of Mo 2C as an active support of metallic nanoparticles, and also illustrate how the deposition of a metal can drastically change the activity and selectivity of a carbide substrate for CO 2 hydrogenation.« less

Enhanced coproduction of hydrogen and methane from cornstalks by a three-stage anaerobic fermentation process integrated with alkaline hydrolysis.

PubMed

Cheng, Xi-Yu; Liu, Chun-Zhao

2012-01-01

A three-stage anaerobic fermentation process including H(2) fermentation I, H(2) fermentation II, methane fermentation was developed for the coproduction of hydrogen and methane from cornstalks. Hydrogen production from cornstalks using direct microbial conversion by Clostridium thermocellum 7072 was markedly enhanced in the two-stage thermophilic hydrogen fermentation process integrated with alkaline treatment. The highest total hydrogen yield from cornstalks in the two-stage fermentation process reached 74.4 mL/g-cornstalk. The hydrogen fermentation effluents and alkaline hydrolyzate were further used for methane fermentation by anaerobic granular sludge, and the total methane yield reached 205.8 mL/g-cornstalk. The total energy recovery in the three-stage anaerobic fermentation process integrated with alkaline hydrolysis reached 70.0%. Copyright © 2011 Elsevier Ltd. All rights reserved.

Impact of cell design and operating conditions on the performances of SOFC fuelled with methane

NASA Astrophysics Data System (ADS)

Laurencin, J.; Lefebvre-Joud, F.; Delette, G.

An in-house-model has been developed to study the thermal and electrochemical behaviour of a planar SOFC fed directly with methane and incorporated in a boiler. The usual Ni-YSZ cermet has been considered for the anode material. It has been found that methane reforming into hydrogen occurs only at the cell inlet in a limited depth within the anode. A sensitivity analysis has allowed establishing that anode thicknesses higher than ∼400-500 μm are required to achieve both the optimal methane conversion and electrochemical performances. The direct internal reforming (DIR) mechanisms and the impact of operating conditions on temperature gradients and SOFC electrical efficiencies have been investigated considering the anode supported cell configuration. It has been shown that the temperature gradient is minimised in the autothermal mode of cell operation. Thermal equilibrium in the stack has been found to be strongly dependent on radiative heat losses with the stack envelope. Electrochemical performance and cell temperature maps have been established as a function of methane flow rates and cell voltages.

MnTiO3-driven low-temperature oxidative coupling of methane over TiO2-doped Mn2O3-Na2WO4/SiO2 catalyst

PubMed Central

Wang, Pengwei; Zhao, Guofeng; Wang, Yu; Lu, Yong

2017-01-01

Oxidative coupling of methane (OCM) is a promising method for the direct conversion of methane to ethene and ethane (C2 products). Among the catalysts reported previously, Mn2O3-Na2WO4/SiO2 showed the highest conversion and selectivity, but only at 800° to 900°C, which represents a substantial challenge for commercialization. We report a TiO2-doped Mn2O3-Na2WO4/SiO2 catalyst by using Ti-MWW zeolite as TiO2 dopant as well as SiO2 support, enabling OCM with 26% conversion and 76% C2-C3 selectivity at 720°C because of MnTiO3 formation. MnTiO3 triggers the low-temperature Mn2+↔Mn3+ cycle for O2 activation while working synergistically with Na2WO4 to selectively convert methane to C2-C3. We also prepared a practical Mn2O3-TiO2-Na2WO4/SiO2 catalyst in a ball mill. This catalyst can be transformed in situ into MnTiO3-Na2WO4/SiO2, yielding 22% conversion and 62% selectivity at 650°C. Our results will stimulate attempts to understand more fully the chemistry of MnTiO3-governed low-temperature activity, which might lead to commercial exploitation of a low-temperature OCM process. PMID:28630917

Methane-Powered Vehicles

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.

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

DOE PAGES

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

2016-10-10

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

Biogeochemistry: Hexadecane decay by methanogenesis

USGS Publications Warehouse

Anderson, Robert T.; Lovely, Derek R.

2000-01-01

The potential for the biological conversion of long-chain saturated hydrocarbons to methane under anaerobic conditions has been demonstrated by using an enrichment culture of bacteria to degrade pure-phase hexadecane1. The formation of methane in hydrocarbon-rich subsurface zones could be explained if a similar conversion of long-chain alkanes to methane were to take place in subsurface environments. If this process could be stimulated in the subsurface, it could be used to enhance hydrocarbon recovery from petroleum reserves1, 2. Parkes2, however, questions the environmental significance of the enrichment-culture results1 on the grounds that alkane conversion to methane is very slow and because sulphate-reducing and methanogenic bacteria might both be necessary for even this slow process to occur, restricting the conversion to specialized, unusual zones in sediments. Here we show that, on the contrary, subsurface bacteria can adapt to convert hexadecane to methane rapidly and in the absence of sulphate-reducing bacteria.

Analysis of Percent On-Cell Reformation of Methane in SOFC Stacks: Thermal, Electrical and Stress Analysis

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

Recknagle, Kurtis P.; Yokuda, Satoru T.; Jarboe, Daniel T.

2006-04-07

This report summarizes a parametric analysis performed to determine the effect of varying the percent on-cell reformation (OCR) of methane on the thermal and electrical performance for a generic, planar solid oxide fuel cell (SOFC) stack design. OCR of methane can be beneficial to an SOFC stack because the reaction (steam-methane reformation) is endothermic and can remove excess heat generated by the electrochemical reactions directly from the cell. The heat removed is proportional to the amount of methane reformed on the cell. Methane can be partially pre-reformed externally, then supplied to the stack, where rapid reaction kinetics on the anodemore » ensures complete conversion. Thus, the thermal load varies with methane concentration entering the stack, as does the coupled scalar distributions, including the temperature and electrical current density. The endotherm due to the reformation reaction can cause a temperature depression on the anode near the fuel inlet, resulting in large thermal gradients. This effect depends on factors that include methane concentration, local temperature, and stack geometry.« less

Methane Upgrading of Acetic Acid as a Model Compound for a Biomass-Derived Liquid over a Modified Zeolite Catalyst

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

Wang, Aiguo; Austin, Danielle; Karmakar, Abhoy

The technical feasibility of coaromatization of acetic acid derived from biomass and methane was investigated under mild reaction conditions (400 °C and 30 bar) over silver-, zinc-, and/or gallium-modified zeolite catalysts. On the basis of GC-MS, Micro-GC, and TGA analysis, more light aromatic hydrocarbons, less phenol formation, lower coke production, and higher methane conversion are observed over 5%Zn-1%Ga/ZSM-5 catalyst in comparison with catalytic performance over the other catalysts. Direct evidence of methane incorporation into aromatics over 5%Zn-1%Ga/ZSM-5 catalyst is witnessed in 1H, 2H, and 13C NMR spectra, revealing that the carbon from methane prefers to occupy the phenyl carbon sitesmore » and the benzylic carbon sites, and the hydrogen of methane favors the aromatic and benzylic substitutions of product molecules. In combination with the 13C NMR results for isotopically labeled acetic acid ( 13CH 3COOH and CH 3 13COOH), it can be seen that the methyl and carbonyl carbons of acetic acid are equally involved in the formation of ortho, meta and para carbons of the aromatics, whereas the phenyl carbons directly bonded with alkyl substituent groups and benzylic carbons are derived mainly from the carboxyl carbon of acetic acid. After various catalyst characterizations by using TEM, XRD, DRIFT, NH 3-TPD, and XPS, the excellent catalytic performance might be closely related to the highly dispersed zinc and gallium species on the zeolite support, moderate surface acidity, and an appropriate ratio of weak acidic sites to strong acidic sites as well as the fairly stable oxidation state during acetic acid conversion under a methane environment. Two mechanisms of the coaromatization of acetic acid and methane have also been proposed after consulting all the collected data in this study. In conclusion, the results reported in this paper could potentially lead to more cost-effective utilization of abundant natural gas and biomass.« less

Methane Upgrading of Acetic Acid as a Model Compound for a Biomass-Derived Liquid over a Modified Zeolite Catalyst

DOE PAGES

Wang, Aiguo; Austin, Danielle; Karmakar, Abhoy; ...

2017-04-19

The technical feasibility of coaromatization of acetic acid derived from biomass and methane was investigated under mild reaction conditions (400 °C and 30 bar) over silver-, zinc-, and/or gallium-modified zeolite catalysts. On the basis of GC-MS, Micro-GC, and TGA analysis, more light aromatic hydrocarbons, less phenol formation, lower coke production, and higher methane conversion are observed over 5%Zn-1%Ga/ZSM-5 catalyst in comparison with catalytic performance over the other catalysts. Direct evidence of methane incorporation into aromatics over 5%Zn-1%Ga/ZSM-5 catalyst is witnessed in 1H, 2H, and 13C NMR spectra, revealing that the carbon from methane prefers to occupy the phenyl carbon sitesmore » and the benzylic carbon sites, and the hydrogen of methane favors the aromatic and benzylic substitutions of product molecules. In combination with the 13C NMR results for isotopically labeled acetic acid ( 13CH 3COOH and CH 3 13COOH), it can be seen that the methyl and carbonyl carbons of acetic acid are equally involved in the formation of ortho, meta and para carbons of the aromatics, whereas the phenyl carbons directly bonded with alkyl substituent groups and benzylic carbons are derived mainly from the carboxyl carbon of acetic acid. After various catalyst characterizations by using TEM, XRD, DRIFT, NH 3-TPD, and XPS, the excellent catalytic performance might be closely related to the highly dispersed zinc and gallium species on the zeolite support, moderate surface acidity, and an appropriate ratio of weak acidic sites to strong acidic sites as well as the fairly stable oxidation state during acetic acid conversion under a methane environment. Two mechanisms of the coaromatization of acetic acid and methane have also been proposed after consulting all the collected data in this study. In conclusion, the results reported in this paper could potentially lead to more cost-effective utilization of abundant natural gas and biomass.« less

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

Detering, B.A.; Kong, P.C.; Thomas, C.P.

This paper describes the experimental demonstration of a process for direct conversion of methane to acetylene in a thermal plasma. The process utilizes a thermal plasma to dissociate methane and form an equilibrium mixture of acetylene followed by a supersonic expansion of the hot gas to preserve the produced acetylene in high yield. The high translational velocities and rapid cooling result in an overpopulation of atomic hydrogen which persists throughout the expansion process. The presence of atomic hydrogen shifts the equilibrium composition by inhibiting complete pyrolysis of methane and acetylene to solid carbon. This process has the potential to reducemore » the cost of producing acetylene from natural gas. Acetylene and hydrogen produced by this process could be used directly as industrial gases, building blocks for synthesis of industrial chemicals, or oligomerized to long chain liquid hydrocarbons for use as fuels. This process produces hydrogen and ultrafine carbon black in addition to acetylene.« less

Process Parameters for Successful Synthesis of Carbon Nanotubes by Chemical Vapor Deposition: Implications for Chemical Mechanisms and Life-cycle Assessment

NASA Astrophysics Data System (ADS)

Xue, Ke

Manufacturing of carbon nanotubes (CNTs) via chemical vapor deposition (CVD) calls for thermal treatment associated with gas-phase rearrangement and catalyst deposition to achieve high cost efficiency and limited influence on environmental impact. Taking advantage of higher degree of structure control and economical efficiency, catalytic chemical vapor deposition (CCVD) has currently become the most prevailing synthesis approach for the synthesis of large-scale pure CNTs in past years. Because the synthesis process of CNTs dominates the potential ecotoxic impacts, materials consumption, energy consumption and greenhouse gas emissions should be further limited to efficiently reduce life cycle ecotoxicity of carbon naotubes. However, efforts to reduce energy and material requirements in synthesis of CNTs by CCVD are hindered by a lack of mechanistic understanding. In this thesis, the effect of operating parameters, especially the temperature, carbon source concentration, and residence time on the synthesis were studied to improve the production efficiency in a different angle. Thus, implications on the choice of operating parameters could be provided to help the synthesis of carbon nanotubes. Here, we investigated the typical operating parameters in conditions that have yielded successful CNT production in the published academic literature of over seventy articles. The data were filtered by quality of the resultant product and deemed either "successful" or "unsuccessful" according to the authors. Furthermore, growth rate data were tabulated and used as performance metric for the process whenever possible. The data provided us an opportunity to prompt possible and common methods for practioners in the synthesis of CNTs and motivate routes to achieve energy and material minimization. The statistical analysis revealed that methane and ethylene often rely on thermal conversion process to form direct carbon precursor; further, methane and ethylene could not be the direct CNT precursors by themselves. Acetylene does not show an additional energy demand or thermal conversion in the synthesis, and it could be the direct CNT precursors by itself; or at least, it would be most easily to get access to carbon nanotube growth while minimizing synthesis temperature. In detail, methane employs more energy demand (Tavg=883°C) than ethylene (Tavg=766°C), which in turn demands more energy than acetylene (Tavg=710°C) to successfully synthesize carbon nanotubes. The distinction in energy demand could be the result of kinetic energy requirements by the thermal conversion process of methane and ethylene to form direct CNT precursors, and methane employs the highest activation demand among three hydrocarbons. Thus, these results support the hypothesis that methane and ethylene could be thermally converted to form acetylene before CNT incorporation. In addition, methane and ethylene show the demand for hydrogen in thermal conversion process before CNT incorporation; whereas, hydrogen does not contribute to the synthesis via acetylene before CNT incorporation, except the reduction of catalyst. At relatively low hydrogen concentration, this work suggests that hydrogen prompts growth of carbon nanotubes via methane and ethylene, probably by reducing the catalysts or participating thermal reactions. In addition, "polymerization-like formation mechanism" could be supported by the higher growth rate of CNTs via ethylene than acetylene. There could be an optimum residence time to maintain a relatively higher growth rate. At too low residence time, carbon source could not be accumulated, causing a waste of material; while too high residence time may cause the limitation of carbon source supplement and accumulation of byproducts. At last, high concentration of carbon source and hydrogen could cause more energy consumption, while it helps to achieve a high growth rate, due to the more presence of direct carbon precursor.

Characteristics of adapted hydrogenotrophic community during biomethanation.

PubMed

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.

Metabolic engineering of Methanosarcina acetivorans for lactate production from methane.

PubMed

McAnulty, Michael J; Poosarla, Venkata Giridhar; Li, Jine; Soo, Valerie W C; Zhu, Fayin; Wood, Thomas K

2017-04-01

We previously demonstrated anaerobic conversion of the greenhouse gas methane into acetate using an engineered archaeon that produces methyl-coenzyme M reductase (Mcr) from unculturable microorganisms from a microbial mat in the Black Sea to create the first culturable prokaryote that reverses methanogenesis and grows anaerobically on methane. In this work, we further engineered the same host with the goal of converting methane into butanol. Instead, we discovered a process for converting methane to a secreted valuable product, L-lactate, with sufficient optical purity for synthesizing the biodegradable plastic poly-lactic acid. We determined that the 3-hydroxybutyryl-CoA dehydrogenase (Hbd) from Clostridium acetobutylicum is responsible for lactate production. This work demonstrates the first metabolic engineering of a methanogen with a synthetic pathway; in effect, we produce a novel product (lactate) from a novel substrate (methane) by cloning the three genes for Mcr and one for Hbd. We further demonstrate the utility of anaerobic methane conversion with an increased lactate yield compared to aerobic methane conversion to lactate. Biotechnol. Bioeng. 2017;114: 852-861. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.

Dense ceramic membranes for converting methane to syngas

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

Balachandran, U.; Dusek, J.T.; Picciolo, J.J.

1995-07-01

Dense mixed-oxide ceramics capable of conducting both electrons and oxygen ions are promising materials for partial oxygenation of methane to syngas. We are particularly interested in an oxide based on the Sr-Fe-Co-O system. Dense ceramic membrane tubes have been fabricated by a plastic extrusion technique. The sintered tubes were then used to selectively transport oxygen from air through the membrane to make syngas without the use of external electrodes. The sintered tubes have operated for >1000 h, and methane conversion efficiencies of >98% have been observed. Mechanical properties, structural integrity of the tubes during reactor operation, results of methane conversion,more » selectivity of methane conversion products, oxygen permeation, and fabrication of multichannel configurations for large-scale production of syngas will be presented.« less

Clean fuels from biomass

NASA Technical Reports Server (NTRS)

Hsu, Y.-Y.

1976-01-01

The paper discusses the U.S. resources to provide fuels from agricultural products, the present status of conversion technology of clean fuels from biomass, and a system study directed to determine the energy budget, and environmental and socioeconomic impacts. Conversion processes are discussed relative to pyrolysis and anaerobic fermentation. Pyrolysis breaks the cellulose molecules to smaller molecules under high temperature in the absence of oxygen, wheras anaerobic fermentation is used to convert biomass to methane by means of bacteria. Cost optimization and energy utilization are also discussed.

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

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

Carbon Dioxide-Free Hydrogen Production with Integrated Hydrogen Separation and Storage.

PubMed

Dürr, Stefan; Müller, Michael; Jorschick, Holger; Helmin, Marta; Bösmann, Andreas; Palkovits, Regina; Wasserscheid, Peter

2017-01-10

An integration of CO 2 -free hydrogen generation through methane decomposition coupled with hydrogen/methane separation and chemical hydrogen storage through liquid organic hydrogen carrier (LOHC) systems is demonstrated. A potential, very interesting application is the upgrading of stranded gas, for example, gas from a remote gas field or associated gas from off-shore oil drilling. Stranded gas can be effectively converted in a catalytic process by methane decomposition into solid carbon and a hydrogen/methane mixture that can be directly fed to a hydrogenation unit to load a LOHC with hydrogen. This allows for a straight-forward separation of hydrogen from CH 4 and conversion of hydrogen to a hydrogen-rich LOHC material. Both, the hydrogen-rich LOHC material and the generated carbon on metal can easily be transported to destinations of further industrial use by established transport systems, like ships or trucks. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

Lebarbier Dagel, Vanessa M.; Li, J.; Taylor, Charles E.

This collaborative joint research project is in the area of advanced gasification and conversion, within the Chinese Academy of Sciences (CAS)-National Energy Technology Laboratory (NETL)-Pacific Northwest National Laboratory (PNNL) Memorandum of Understanding. The goal for this subtask is the development of advanced syngas conversion technologies. Two areas of investigation were evaluated: Sorption-Enhanced Synthetic Natural Gas Production from Syngas The conversion of synthetic gas (syngas) to synthetic natural gas (SNG) is typically catalyzed by nickel catalysts performed at moderate temperatures (275 to 325°C). The reaction is highly exothermic and substantial heat is liberated, which can lead to process thermal imbalance andmore » destruction of the catalyst. As a result, conversion per pass is typically limited, and substantial syngas recycle is employed. Commercial methanation catalysts and processes have been developed by Haldor Topsoe, and in some reports, they have indicated that there is a need and opportunity for thermally more robust methanation catalysts to allow for higher per-pass conversion in methanation units. SNG process requires the syngas feed with a higher H2/CO ratio than typically produced from gasification processes. Therefore, the water-gas shift reaction (WGS) will be required to tailor the H2/CO ratio. Integration with CO2 separation could potentially eliminate the need for a separate WGS unit, thereby integrating WGS, methanation, and CO2 capture into one single unit operation and, consequently, leading to improved process efficiency. The SNG process also has the benefit of producing a product stream with high CO2 concentrations, which makes CO2 separation more readily achievable. The use of either adsorbents or membranes that selectively separate the CO2 from the H2 and CO would shift the methanation reaction (by driving WGS for hydrogen production) and greatly improve the overall efficiency and economics of the process. The scope of this activity was to develop methods and enabling materials for syngas conversion to SNG with readily CO2 separation. Suitable methanation catalyst and CO2 sorbent materials were developed. Successful proof-of-concept for the combined reaction-sorption process was demonstrated, which culminated in a research publication. With successful demonstration, a decision was made to switch focus to an area of fuels research of more interest to all three research institutions (CAS-NETL-PNNL). Syngas-to-Hydrocarbon Fuels through Higher Alcohol Intermediates There are two types of processes in syngas conversion to fuels that are attracting R&D interest: 1) syngas conversion to mixed alcohols; and 2) syngas conversion to gasoline via the methanol-to-gasoline process developed by Exxon-Mobil in the 1970s. The focus of this task was to develop a one-step conversion technology by effectively incorporating both processes, which is expected to reduce the capital and operational cost associated with the conversion of coal-derived syngas to liquid fuels. It should be noted that this work did not further study the classic Fischer-Tropsch reaction pathway. Rather, we focused on the studies for unique catalyst pathways that involve the direct liquid fuel synthesis enabled by oxygenated intermediates. Recent advances made in the area of higher alcohol synthesis including the novel catalytic composite materials recently developed by CAS using base metal catalysts were used.« less

Batch conversion of methane to methanol using Methylosinus trichosporium OB3b as biocatalyst.

PubMed

Hwang, In Yeub; Hur, Dong Hoon; Lee, Jae Hoon; Park, Chang-Ho; Chang, In Seop; Lee, Jin Won; Lee, Eun Yeol

2015-03-01

Recently, methane has attracted much attention as an alternative carbon feedstock since it is the major component of abundant shale and natural gas. In this work, we produced methanol from methane using whole cells of Methylosinus trichosporium OB3b as the biocatalyst. M. trichosporium OB3b was cultured on NMS medium with a supply of 7:3 air/methane ratio at 30°C. The optimal concentrations of various methanol dehydrogenase inhibitors such as potassium phosphate and EDTA were determined to be 100 and 0.5 mM, respectively, for an efficient production of methanol. Sodium formate (40 mM) as a reducing power source was added to enhance the conversion efficiency. A productivity of 49.0 mg/l·h, titer of 0.393 g methanol/l, and conversion of 73.8% (mol methanol/mol methane) were obtained under the optimized batch condition.

Type and amount of organic amendments affect enhanced biogenic methane production from coal and microbial community structure

USGS Publications Warehouse

Davis, Katherine J.; Lu, Shipeng; Barnhart, Elliott P.; Parker, Albert E.; Fields, Matthew W.; Gerlach, Robin

2018-01-01

Slow rates of coal-to-methane conversion limit biogenic methane production from coalbeds. This study demonstrates that rates of coal-to-methane conversion can be increased by the addition of small amounts of organic amendments. Algae, cyanobacteria, yeast cells, and granulated yeast extract were tested at two concentrations (0.1 and 0.5 g/L), and similar increases in total methane produced and methane production rates were observed for all amendments at a given concentration. In 0.1 g/L amended systems, the amount of carbon converted to methane minus the amount produced in coal only systems exceeded the amount of carbon added in the form of amendment, suggesting enhanced coal-to-methane conversion through amendment addition. The amount of methane produced in the 0.5 g/L amended systems did not exceed the amount of carbon added. While the archaeal communities did not vary significantly, the bacterial populations appeared to be strongly influenced by the presence of coal when 0.1 g/L of amendment was added; at an amendment concentration of 0.5 g/L the bacterial community composition appeared to be affected most strongly by the amendment type. Overall, the results suggest that small amounts of amendment are not only sufficient but possibly advantageous if faster in situcoal-to-methane production is to be promoted.

Potential use and the energy conversion efficiency analysis of fermentation effluents from photo and dark fermentative bio-hydrogen production.

PubMed

Zhang, Zhiping; Li, Yameng; Zhang, Huan; He, Chao; Zhang, Quanguo

2017-12-01

Effluent of bio-hydrogen production system also can be adopted to produce methane for further fermentation, cogeneration of hydrogen and methane will significantly improve the energy conversion efficiency. Platanus Orientalis leaves were taken as the raw material for photo- and dark-fermentation bio-hydrogen production. The resulting concentrations of acetic, butyric, and propionic acids and ethanol in the photo- and dark-fermentation effluents were 2966mg/L and 624mg/L, 422mg/L and 1624mg/L, 1365mg/L and 558mg/L, and 866mg/L and 1352mg/L, respectively. Subsequently, we calculated the energy conversion efficiency according to the organic contents of the effluents and their energy output when used as raw material for methane production. The overall energy conversion efficiencies increased by 15.17% and 22.28%, respectively, when using the effluents of photo and dark fermentation. This two-step bio-hydrogen and methane production system can significantly improve the energy conversion efficiency of anaerobic biological treatment plants. Copyright © 2017. Published by Elsevier Ltd.

Raman studies of methane-ethane hydrate metastability.

PubMed

Ohno, Hiroshi; Strobel, Timothy A; Dec, Steven F; Sloan, E Dendy; Koh, Carolyn A

2009-03-05

The interconversion of methane-ethane hydrate from metastable to stable structures was studied using Raman spectroscopy. sI and sII hydrates were synthesized from methane-ethane gas mixtures of 65% or 93% methane in ethane and water, both with and without the kinetic hydrate inhibitor, poly(N-vinylcaprolactam). The observed faster structural conversion rate in the higher methane concentration atmosphere can be explained in terms of the differences in driving force (difference in chemical potential of water in sI and sII hydrates) and kinetics (mass transfer of gas and water rearrangement). The kinetic hydrate inhibitor increased the conversion rate at 65% methane in ethane (sI is thermodynamically stable) but retards the rate at 93% methane in ethane (sII is thermodynamically stable), implying there is a complex interaction between the polymer, water, and hydrate guests at crystal surfaces.

Kinetics of (reversible) internal reforming of methane in solid oxide fuel cells under stationary and APU conditions

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.

Methane Pyrolysis and Disposing Off Resulting Carbon

NASA Technical Reports Server (NTRS)

Sharma, P. K.; Rapp, D.; Rahotgi, N. K.

1999-01-01

Sabatier/Electrolysis (S/E) is a leading process for producing methane and oxygen for application to Mars ISPP. One significant problem with this process is that it produces an excess of methane for combustion with the amount of oxygen that is produced. Therefore, one must discard roughly half of the methane to obtain the proper stoichiometric methane/oxygen mixture for ascent from Mars. This is wasteful of hydrogen, which must be brought from Earth and is difficult to transport to Mars and store on Mars. To reduced the problem of transporting hydrogen to Mars, the S/E process can be augmented by another process which reduces overall hydrogen requirement. Three conceptual approaches for doing this are (1) recover hydrogen from the excess methane produced by the S/E process, (2) convert the methane to a higher hydrocarbon or other organic with a lower H/C ratio than methane, and (3) use a separate process (such as zirconia or reverse water gas shift reaction) to produce additional oxygen, thus utilizing all the methane produced by the Sabatier process. We report our results here on recovering hydrogen from the excess methane using pyrolysis of methane. Pyrolysis has the advantage that it produces almost pure hydrogen, and any unreacted methane can pass through the S/E process reactor. It has the disadvantage that disposing of the carbon produced by pyrolysis presents difficulties. Hydrogen may be obtained from methane by pyrolysis in the temperature range 10000-12000C. The main reaction products are hydrogen and carbon, though very small amounts of higher hydrocarbons, including aromatic hydrocarbons are formed. The conversion efficiency is about 95% at 12000C. One needs to distinguish between thermodynamic equilibrium conversion and conversion limited by kinetics in a finite reactor.

Reactions of C1 Building Blocks

NASA Astrophysics Data System (ADS)

Stöcker, Michael

The chapter “Reactions of C1 Building Blocks” covers the direct conversion of methane to aromatics, the methanol-to-hydrocarbons (MTHC) conversion with respect to gasoline (methanol to gasoline) and olefins (methanol to olefins, methanol-to-propene) as well as some combinations like the TIGAS and Mobil's olefin-to-gasoline and distillate processes. The main focus within this chapter will be on the industrial processes, especially concerning the MTHC reactions - including catalytic systems, reaction conditions, process - and to a minor extent related to the mechanistic aspects and kinetic considerations.

Enzyme-Embedded, Microstructural Reactors for Industrial Biocatalysis

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

Baker, Sarah E.; Knipe, J. M.; Oakdale, J.

In this project we explored enzyme-catalyzed methane conversion to methanol. Industrial biological approaches to methane conversion using whole organisms are predicted to be more energy efficient than chemical approaches, but are limited by mass transfer of the gas phase reactants, methane and oxygen, to the organisms. We demonstrated that 3D printing the enzyme particulate Methane Mono Oxygenase (pMMO) embedded in a polymer can improve the kinetics of methane to methanol conversion. This improvement was likely due to the ability to increase the surface area of the catalytic material using 3D printing. We also demonstrated the first continuous use of pMMOmore » in a flow-through reactor. In order to understand the fundamental kinetic properties of pMMO, we conducted an in-depth study of pMMO kinetics using analytical tools developed in our lab. Finally, we developed a new copolymer system that allowed tuning of the gas permeability of the biocatalytic material.« less

Catalytic conversion of methane to methanol using Cu-zeolites.

PubMed

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.

40 CFR 98.366 - Data reporting requirements.

Code of Federal Regulations, 2011 CFR

2011-07-01

... type). (11) Methane conversion factor used for each MMS component. (12) Average ambient temperature used to select each methane conversion factor. (13) N2O emissions (results of Equation JJ-13). (14) N... (CONTINUED) MANDATORY GREENHOUSE GAS REPORTING Manure Management § 98.366 Data reporting requirements. (a) In...

40 CFR 98.366 - Data reporting requirements.

Code of Federal Regulations, 2012 CFR

2012-07-01

... type). (11) Methane conversion factor used for each MMS component. (12) Average ambient temperature used to select each methane conversion factor. (13) N2O emissions (results of Equation JJ-13). (14) N... (CONTINUED) MANDATORY GREENHOUSE GAS REPORTING Manure Management § 98.366 Data reporting requirements. (a) In...

40 CFR 98.366 - Data reporting requirements.

Code of Federal Regulations, 2013 CFR

2013-07-01

... type). (11) Methane conversion factor used for each MMS component. (12) Average ambient temperature used to select each methane conversion factor. (13) N2O emissions (results of Equation JJ-13). (14) N... (CONTINUED) MANDATORY GREENHOUSE GAS REPORTING Manure Management § 98.366 Data reporting requirements. (a) In...

40 CFR 98.366 - Data reporting requirements.

Code of Federal Regulations, 2014 CFR

2014-07-01

... type). (11) Methane conversion factor used for each MMS component. (12) Average ambient temperature used to select each methane conversion factor. (13) N2O emissions (results of Equation JJ-13). (14) N... (CONTINUED) MANDATORY GREENHOUSE GAS REPORTING Manure Management § 98.366 Data reporting requirements. (a) In...

Production of Renewable Natural Gas from Waste Biomass

NASA Astrophysics Data System (ADS)

Kumar, Sachin; Suresh, S.; Arisutha, S.

2013-03-01

Biomass energy is expected to make a major contribution to the replacement of fossil fuels. Methane produced from biomass is referred to as bio-methane, green gas, bio-substitute natural gas or renewable natural gas (RNG) when it is used as a transport fuel. Research on upgrading of the cleaned producer gas to RNG is still ongoing. The present study deals with the conversion of woody biomass into fuels, RNG using gasifier. The various effects of parameters like temperature, pressure, and tar formation on conversion were also studied. The complete carbon conversion was observed at 480 °C and tar yield was significantly less. When biomass was gasified with and without catalyst at about 28 s residence time, ~75 % (w/w) and 88 % (w/w) carbon conversion for without and with catalyst was observed. The interest in RNG is growing; several initiatives to demonstrate the thermal-chemical conversion of biomass into methane and/or RNG are under development.

A novel process for volatile fatty acids production from syngas by integrating with mesophilic alkaline fermentation of waste activated sludge.

PubMed

Rao, Yue; Wan, Jingjing; Liu, Yafeng; Angelidaki, Irini; Zhang, Shicheng; Zhang, Yalei; Luo, Gang

2018-08-01

The present study proposed and demonstrated a novel process for the bioconversion of syngas (mainly CO and H 2 ) to valuable volatile fatty acids (VFA) by integrating with mesophilic alkaline fermentation of waste activated sludge (WAS). The results showed that although pH 9 was suitable for VFA production from WAS, 62.5% of the consumed CO was converted to methane due to the presence of hydrogenogenic pathway for CO conversion. The increase of pH from 9 to 9.5 inhibited the methane production from CO because of the possible presence of only acetogenic pathway for CO conversion. However, methane was still produced from H 2 contained in syngas through hydrogenotrophic methanogenesis, and around 32-34% of the consumed syngas was converted to methane. At both pH 9 and 9.5, methane was produced by hydrogenotrophic methanogens Methanobacteriales. Further increase of pH to 10 effectively inhibited methane production from syngas, and efficient VFA (mainly acetate with the concentration of around 135 mM) production by simultaneous conversion of syngas and WAS was achieved. High acetate concentrations (>150 mM) were shown to have serious negative effects on the conversion of syngas. The addition of syngas to the mesophilic alkaline fermentation of WAS at pH 10 not only resulted in the enrichment of some known bacteria related with syngas conversion, but also changed the microbial community compositions for the fermentation of WAS. Copyright © 2018 Elsevier Ltd. All rights reserved.

Transition metal sulfide loaded catalyst

DOEpatents

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.

Cobalt carbide nanoprisms for direct production of lower olefins from syngas

NASA Astrophysics Data System (ADS)

Zhong, Liangshu; Yu, Fei; An, Yunlei; Zhao, Yonghui; Sun, Yuhan; Li, Zhengjia; Lin, Tiejun; Lin, Yanjun; Qi, Xingzhen; Dai, Yuanyuan; Gu, Lin; Hu, Jinsong; Jin, Shifeng; Shen, Qun; Wang, Hui

2016-10-01

Lower olefins—generally referring to ethylene, propylene and butylene—are basic carbon-based building blocks that are widely used in the chemical industry, and are traditionally produced through thermal or catalytic cracking of a range of hydrocarbon feedstocks, such as naphtha, gas oil, condensates and light alkanes. With the rapid depletion of the limited petroleum reserves that serve as the source of these hydrocarbons, there is an urgent need for processes that can produce lower olefins from alternative feedstocks. The ‘Fischer-Tropsch to olefins’ (FTO) process has long offered a way of producing lower olefins directly from syngas—a mixture of hydrogen and carbon monoxide that is readily derived from coal, biomass and natural gas. But the hydrocarbons obtained with the FTO process typically follow the so-called Anderson-Schulz-Flory distribution, which is characterized by a maximum C2-C4 hydrocarbon fraction of about 56.7 per cent and an undesired methane fraction of about 29.2 per cent (refs 1, 10, 11, 12). Here we show that, under mild reaction conditions, cobalt carbide quadrangular nanoprisms catalyse the FTO conversion of syngas with high selectivity for the production of lower olefins (constituting around 60.8 per cent of the carbon products), while generating little methane (about 5.0 per cent), with the ratio of desired unsaturated hydrocarbons to less valuable saturated hydrocarbons amongst the C2-C4 products being as high as 30. Detailed catalyst characterization during the initial reaction stage and theoretical calculations indicate that preferentially exposed {101} and {020} facets play a pivotal role during syngas conversion, in that they favour olefin production and inhibit methane formation, and thereby render cobalt carbide nanoprisms a promising new catalyst system for directly converting syngas into lower olefins.

Methane combustion reactivity during the metal→metallic oxide transformation of Pd-Pt catalysts: Effect of oxygen pressure

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.

Transition metal sulfide loaded catalyst

DOEpatents

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.

Magnesium carbide synthesis from methane and magnesium oxide - a potential methodology for natural gas conversion to premium fuels and chemicals

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

Diaz, A.F.; Modestino, A.J.; Howard, J.B.

1995-12-31

Diversification of the raw materials base for manufacturing premium fuels and chemicals offers U.S. and international consumers economic and strategic benefits. Extensive reserves of natural gas in the world provide a valuable source of clean gaseous fuel and chemical feedstock. Assuming the availability of suitable conversion processes, natural gas offers the prospect of improving flexibility in liquid fuels and chemicals manufacture, and thus, the opportunity to complement, supplement, or displace petroleum-based production as economic and strategic considerations require. The composition of natural gas varies from reservoir to reservoir but the principal hydrocarbon constituent is always methane (CH{sub 4}). With itsmore » high hydrogen-to-carbon ratio, methane has the potential to produce hydrogen or hydrogen-rich products. However, methane is a very chemically stable molecule and, thus, is not readily transformed to other molecules or easily reformed to its elements (H{sub 2} and carbon). In many cases, further research is needed to augment selectivity to desired product(s), increase single-pass conversions, or improve economics (e.g. there have been estimates of $50/bbl or more for liquid products) before the full potential of these methodologies can be realized on a commercial scale. With the trade-off between gas conversion and product selectivity, a major challenge common to many of these technologies is to simultaneously achieve high methane single-pass conversions and high selectivity to desired products. Based on the results of the scoping runs, there appears to be strong indications that a breakthrough has finally been achieved in that synthesis of magnesium carbides from MgO and methane in the arc discharge reactor has been demonstrated.« less

Analysis of methane biodegradation by Methylosinus trichosporium OB3b

PubMed Central

Rodrigues, Andréa dos Santos; Salgado, Belkis Valdman e Andréa Medeiros

2009-01-01

The microbial oxidation of methane in the atmosphere is performed by methanotrophic bacteria that use methane as a unique source of carbon and energy. The objective of this work consisted of the investigation of the best conditions of methane biodegradation by methanotrophic bacteria Methylosinus trichosporium OB3b that oxidize it to carbon dioxide, and the use of these microorganisms in monitoring methods for methane. The results showed that M. trichosporium OB3b was capable to degrade methane in a more effective way with an initial microorganism concentration of 0.0700 g.L-1, temperature of 30ºC, pH 6.5 and using 1.79 mmol of methane. In these same conditions, there was no bacterial growth when 2.69 mmol of methane was used. The specific rate of microorganism growth, the conversion factor, the efficiency and the volumetric productivity, for the optimized conditions of biodegradation were, respectively, 0.0324 h-1, 0.6830 gcells/gCH4, 73.73% and 2.7732.10-3 gcells/L.h. The final product of methane microbiological degradation, carbon dioxide, was quantified through the use of a commercial electrode, and, through this, the grade of methane conversion in carbon dioxide was calculated. PMID:24031362

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

Yuan Zhang; Jin-hu Wu; Dong-ke Zhang

The cracking of oil refinery off-gas, simulated with a gas mixture containing methane (51%), ethylene (21.4%), ethane (21.1%), and propane (6.5%), over a coal char, petroleum coke, and quartz, respectively, has been studied in a fixed bed reactor. The experiments were performed at temperatures between 850 and 1000{sup o}C and at atmospheric pressure. The results show that the conversions of all species considered increased with increasing temperature. Ethane and propane completely decomposed over all three bed materials in the temperature range investigated. However, the higher initial conversion rates of methane and ethylene cracking at all temperatures were observed only overmore » the coal char and not on the petroleum coke and quartz, indicating a significant catalytic effect of the coal char on methane and ethylene cracking. Methane and ethylene conversions decreased with reaction time due to deactivation of the coal char by carbon deposition on the char surface and, in the later stage of a cracking experiment, became negative, suggesting that methane and ethylene had been formed during the cracking of ethane and propane. 16 refs., 13 figs., 2 tabs.« less

Catalytic conversion of light alkanes, Phase 3. Topical report, January 1990--December 1992

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

NONE

The mission of this work is to devise a new catalyst which can be used in the first simple, economic process to convert the light alkanes in natural gas to an alcohol-rich oxygenated product which can either be used as an environmentally friendly, high-performance liquid fuel, or a precursor to a liquid hydrocarbon transportation fuel. The authors have entered the proof-of-concept stage for converting isobutane to tert butyl alcohol in a practical process and are preparing to enter proof-of-concept of a propane to isopropyl alcohol process in the near future. Methane and ethane are more refractory and thus more difficultmore » to oxidize than the C{sub 3} and C{sub 4} hydrocarbons. Nonetheless, advances made in this area indicate that further research progress could achieve the goal of their direct conversion to alcohols. Progress in Phase 3 catalytic vapor phase methane and ethane oxidation over metals in regular oxidic lattices are the subject of this topical report.« less

Effect of process design and operating parameters on aerobic methane oxidation in municipal WWTPs.

PubMed

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.

Conversion of Amazon rainforest to agriculture alters community traits of methane-cycling organisms.

PubMed

Meyer, Kyle M; Klein, Ann M; Rodrigues, Jorge L M; Nüsslein, Klaus; Tringe, Susannah G; Mirza, Babur S; Tiedje, James M; Bohannan, Brendan J M

2017-03-01

Land use change is one of the greatest environmental impacts worldwide, especially to tropical forests. The Amazon rainforest has been subject to particularly high rates of land use change, primarily to cattle pasture. A commonly observed response to cattle pasture establishment in the Amazon is the conversion of soil from a methane sink in rainforest, to a methane source in pasture. However, it is not known how the microorganisms that mediate methane flux are altered by land use change. Here, we use the deepest metagenomic sequencing of Amazonian soil to date to investigate differences in methane-cycling microorganisms and their traits across rainforest and cattle pasture soils. We found that methane-cycling microorganisms responded to land use change, with the strongest responses exhibited by methane-consuming, rather than methane-producing, microorganisms. These responses included a reduction in the relative abundance of methanotrophs and a significant decrease in the abundance of genes encoding particulate methane monooxygenase. We also observed compositional changes to methanotroph and methanogen communities as well as changes to methanotroph life history strategies. Our observations suggest that methane-cycling microorganisms are vulnerable to land use change, and this vulnerability may underlie the response of methane flux to land use change in Amazon soils. © 2017 John Wiley & Sons Ltd.

Small Molecule Catalysts for Harvesting Methane Gas

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

Baker, S. E.; Ceron-Hernandez, M.; Oakdale, J.

As the average temperature of the earth increases the impact of these changes are becoming apparent. One of the most dramatic changes to the environment is the melting of arctic permafrost. The disappearance of the permafrost has resulted in release of streams of methane that was trapped in remote areas as gas hydrates in ice. Additionally, the use of fracking has also increased emission of methane. Currently, the methane is either lost to the atmosphere or flared. If these streams of methane could be brought to market, this would be an abundant source of revenue. A cheap conversion of gaseousmore » methane to a more convenient form for transport would be necessary to economical. Conversion of methane is a difficult reaction since the C-H bond is very stable (104 kcal/mole). At the industrial scale, the Fischer-Tropsch reaction can be used to convert gaseous methane to liquid methanol but is this method is impractical for these streams that have low pressures and are located in remote areas. Additionally, the Fischer-Tropsch reaction results in over oxidation of the methane leading to many products that would need to be separated.« less

Cation-exchanged zeolites for the selective oxidation of methane to methanol

DOE PAGES

Kulkarni, Ambarish R.; Zhao, Zhi-Jian; Siahrostami, Samira; ...

2017-10-19

Motivated by the increasing availability of cheap natural gas resources, considerable experimental and computational research efforts have focused on identifying selective catalysts for the direct conversion of methane to methanol. One promising class of catalysts are cation-exchanged zeolites, which have steadily increased in popularity over the past decade. Here, in this article, we first present a broad overview of this field from a conceptual perspective, and highlight the role of theory in developing a molecular-level understanding of the reaction. Next, by performing and analyzing a large database of density functional theory (DFT) calculations for a wide range of transition metalmore » cations, zeolite topologies and active site motifs, we present a unifying picture of the methane activation process in terms of active site stability, C–H bond activation and methanol extraction. Based on the trade-offs of active site stability and reactivity, we propose a framework for identifying new, promising active site motifs in these systems. Further, we show that the high methanol selectivity arises due to the strong binding nature of the C–H activation products. Lastly, using the atomistic and mechanistic insight obtained from these analyses, we summarize the key challenges and future strategies for improving the performance of cation-exchanged zeolites for this industrially relevant conversion.« less

Cation-exchanged zeolites for the selective oxidation of methane to methanol

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

Kulkarni, Ambarish R.; Zhao, Zhi-Jian; Siahrostami, Samira

Motivated by the increasing availability of cheap natural gas resources, considerable experimental and computational research efforts have focused on identifying selective catalysts for the direct conversion of methane to methanol. One promising class of catalysts are cation-exchanged zeolites, which have steadily increased in popularity over the past decade. Here, in this article, we first present a broad overview of this field from a conceptual perspective, and highlight the role of theory in developing a molecular-level understanding of the reaction. Next, by performing and analyzing a large database of density functional theory (DFT) calculations for a wide range of transition metalmore » cations, zeolite topologies and active site motifs, we present a unifying picture of the methane activation process in terms of active site stability, C–H bond activation and methanol extraction. Based on the trade-offs of active site stability and reactivity, we propose a framework for identifying new, promising active site motifs in these systems. Further, we show that the high methanol selectivity arises due to the strong binding nature of the C–H activation products. Lastly, using the atomistic and mechanistic insight obtained from these analyses, we summarize the key challenges and future strategies for improving the performance of cation-exchanged zeolites for this industrially relevant conversion.« less

Activation of methane by transition metal-substituted aluminophosphate molecular sieves

DOEpatents

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.

Theoretical Investigation of Methane Hydroxylation over Isoelectronic [FeO]2+- and [MnO]+-Exchanged Zeolites Activated by N2O.

PubMed

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.

Investigation of the characteristics of a compact steam reformer integrated with a water-gas shift reactor

NASA Astrophysics Data System (ADS)

Seo, Yong-Seog; Seo, Dong-Joo; Seo, Yu-Taek; Yoon, Wang-Lai

The objective of this study is to investigate numerically a compact steam methane reforming (SMR) system integrated with a water-gas shift (WGS) reactor. Separate numerical models are established for the combustion part, SMR and WGS reaction bed. The concentration of species at the exits of the SMR and WGS bed, and the temperatures in the WGS bed are in good agreement with the measured data. Heat transfer to the catalyst beds and the catalytic reactions in the SMR and WGS catalyst bed are investigated as a function of the operation parameters. The conversion of methane at the exit of the SMR catalyst bed is calculated to be 87%, and the carbon monoxide concentration at the outlet of the WGS bed is estimated to be 0.45%. The effects of the cooling heat flux at the outside wall of the system and steam-to-carbon (S/C) ratio are also examined. As the cooling heat flux increases, both the methane conversion and carbon monoxide content are reduced in the SMR bed, and the carbon monoxide conversion is improved in the WGS bed. Both methane conversion and carbon dioxide reduction increase with increasing steam-to-carbon ratio.

The conversion of community-derived wastes to methane in a high-rate digester. La conversion des dechets solides municipaux en methane dans un digesteur a rendement eleve

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

Biljetina, R.; Srivastava, V.J.; Punwani, D.V.

1988-01-01

The Institute of Gas Technology (IGT) has been operating a 4.5-m/sup 3/, anaerobic solids-concentrating digester at the Walt Disney World Resort Complex in Lake Buena Vista, Florida, since January 1984. This digester development work is part of a larger effort that provides effective community waste treatment and disposal options while recovering a valuable methane resources from these wastes. Excellent conversions to methane have been obtained in the digester during 4 years of uninterrupted operation. Data were collected on wastes from experimental municipal wastewater treatment applications, that is, water hyacinths were harvested from secondary wastewater treatment channels and combined with sludgemore » from primary clarifiers to maximize potential methane recoveries in the digester; wastes from agricultural operations, that is, sorghum was selected as a candidate because it represents both a potential energy crop, as well as a waste resource if only portions of the plant are converted after grain production; and wastes from municipal waste collection. Municipal solids waste (MSW) from a commercial resource recovery center was selected. 3 refs., 4 figs., 5 tabs.« less

Theoretical Insights into Direct Methane to Methanol Conversion over Supported Dicopper Oxo Nanoclusters

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

Theoretical Insights into Direct Methane to Methanol Conversion over Supported Dicopper Oxo Nanoclusters

DOE PAGES

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

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

PubMed Central

Lawton, Thomas J.; Rosenzweig, Amy C.

2017-01-01

Biological conversion of natural gas to liquids (Bio-GTL) represents an immense economic opportunity. In nature, aerobic methanotrophic bacteria and anaerobic archaea are able to selectively oxidize methane using methane monooxygenase (MMO) and methyl coenzyme M reductase (MCR) enzymes. Although significant progress has been made toward genetically manipulating these organisms for biotechnological applications, the enzymes themselves are slow, complex, and not recombinantly tractable in traditional industrial hosts. With turnover numbers of 0.16–13 s−1, these enzymes pose a considerable upstream problem in the biological production of fuels or chemicals from methane. Methane oxidation enzymes will need to be engineered to be faster to enable high volumetric productivities; however, efforts to do so and to engineer simpler enzymes have been minimally successful. Moreover, known methane-oxidizing enzymes have different expression levels, carbon and energy efficiencies, require auxiliary systems for biosynthesis and function, and vary considerably in terms of complexity and reductant requirements. The pros and cons of using each methane-oxidizing enzyme for Bio-GTL are considered in detail. The future for these enzymes is bright, but a renewed focus on studying them will be critical to the successful development of biological processes that utilize methane as a feedstock. PMID:27366961

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

PubMed

Lawton, Thomas J; Rosenzweig, Amy C

2016-08-03

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

Method for the photocatalytic conversion of methane

DOEpatents

Noceti, R.P.; Taylor, C.E.; D`Este, J.R.

1998-02-24

A method for converting methane to methanol is provided comprising subjecting the methane to visible light in the presence of a catalyst and an electron transfer agent. Another embodiment of the invention provides for a method for reacting methane and water to produce methanol and hydrogen comprising preparing a fluid containing methane, an electron transfer agent and a photolysis catalyst, and subjecting said fluid to visible light for an effective period of time. 3 figs.

Method for the photocatalytic conversion of methane

DOEpatents

Noceti, Richard P.; Taylor, Charles E.; D'Este, Joseph R.

1998-01-01

A method for converting methane to methanol is provided comprising subjecting the methane to visible light in the presence of a catalyst and an electron transfer agent. Another embodiment of the invention provides for a method for reacting methane and water to produce methanol and hydrogen comprising preparing a fluid containing methane, an electron transfer agent and a photolysis catalyst, and subjecting said fluid to visible light for an effective period of time.

Plasma conversion of methane into higher hydrocarbons at surfaces

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

Sackinger, W.M.; Kamath, V.A.

1995-12-31

Natural gas is widely abundant, is easily withdrawn from reservoirs, is commonly produced as an associated gas along with crude oil production, and is found in many geologic settings as a resource separate from oil. A much larger fraction of the natural gas may be produced from a gas reservoir, as compared with a crude oil reservoir. However, natural gas is normally transported by pipeline, and the energy throughput of such a pipeline is perhaps only 20% to 30% of the throughput of an oil pipeline of the same size and cost. Gas is difficult to transport in moderate quantitiesmore » at low cost, as it must either have a special pipeline or must be liquified into LNG, shipped in cryogenic LNG tankers, and regasified chemical stability of methane has made it difficult to convert it directly into conventional hydrocarbon fuel mixtures, and has also impeded its use as a feedstock for petrochemical production. Experiments are described in which a methane plasma is created, and the resulting methyl and hydrogen ions have been accelerated within a microchannel array so that they interact with neutral methane molecules on the inside surfaces of the microchannels. No catalysts are used, and the device operates at room temperature. Impact energies of the ions are in the range of 15 ev to greater than 100 ev, and the energy delivered in the interaction at the surfaces has caused the production of larger hydrocarbon molecules, such as C{sub 2}H{sub 2}, C{sub 2}H{sub 4}, and C{sub 2}H{sub 6}, along with C{sub 3}, C{sub 4}, C{sub 5}, C{sub 6}, C{sub 7}, and C{sub 8} molecules. Conversion effectiveness is greater at higher pressure, due to the increased ionic activity. The costs of production of the plasma conversion devices are projected to be quite low, and the technology appears to be commercially and economically feasible.« less

Hydrogen production from methane using oxygen-permeable ceramic membranes

NASA Astrophysics Data System (ADS)

Faraji, Sedigheh

Non-porous ceramic membranes with mixed ionic and electronic conductivity have received significant interest in membrane reactor systems for the conversion of methane and higher hydrocarbons to higher value products like hydrogen. However, hydrogen generation by this method has not yet been commercialized and suffers from low membrane stability, low membrane oxygen flux, high membrane fabrication costs, and high reaction temperature requirements. In this dissertation, hydrogen production from methane on two different types of ceramic membranes (dense SFC and BSCF) has been investigated. The focus of this research was on the effects of different parameters to improve hydrogen production in a membrane reactor. These parameters included operating temperature, type of catalyst, membrane material, membrane thickness, membrane preparation pH, and feed ratio. The role of the membrane in the conversion of methane and the interaction with a Pt/CeZrO2 catalyst has been studied. Pulse studies of reactants and products over physical mixtures of crushed membrane material and catalyst have clearly demonstrated that a synergy exists between the membrane and the catalyst under reaction conditions. The degree of catalyst/membrane interaction strongly impacts the conversion of methane and the catalyst performance. During thermogravimetric analysis, the onset temperature of oxygen release for BSCF was observed to be lower than that for SFC while the amount of oxygen release was significantly greater. Pulse injections of CO2 over crushed membranes at 800°C have shown more CO2 dissociation on the BSCF membrane than the SFC membrane, resulting in higher CO formation on the BSCF membrane. Similar to the CO2 pulses, when CO was injected on the samples at 800°C, CO2 production was higher on BSCF than SFC. It was found that hydrogen consumption on BSCF particles is 24 times higher than that on SFC particles. Furthermore, Raman spectroscopy and temperature programmed desorption studies of CO and CO2 showed a higher CO and CO2 adsorption (for temperatures ranging from room temperature to 600°C) on BSCF compared to the SFC membrane. CO2 reforming reactions on BSCF and SFC dense membranes in a membrane reactor showed higher methane conversion and H2/CO ratio on BSCF than SFC in the presence of the Pt/CeZrO2 catalyst. This high conversion and H2/CO ratio could be ascribed to higher CO, CO2, and H2 adsorption on BSCF than SFC, resulting in higher steam and CO2 reforming on the BSCF. The Pt-Ni/CeZrO2 catalyst exhibits promising performance for hydrogen production. Platinum enhances the reducibility of Ni/Al2O 3 and Ni/CeZrO2 catalysts resulting in improved catalysts for H2 production at moderate temperatures. TPR and Raman studies show an alloy formation in the Pt-Ni/Al2O3 catalyst. Further work is required to study the interaction between Pt and Ni in the bimetallic Pt-Ni/CeZrO2 and Pt-Ni/Al2O3 catalysts. Although the Pt-Ni/Al2O3 catalyst shows high methane conversion in the presence of the BSCF membrane at 800°C, the activity of this catalyst is low at 600°C. Pt-Ni/CeZrO2 bimetallic catalyst demonstrates superior performance compared to Pt-Ni/Al2O3 catalyst at 600°C. The thinner BSCF membrane (2.2 mm) demonstrates a higher methane conversion and H2:CO ratio than the thicker BSCF membrane (2.6 mm) because membrane oxygen flux is inversely proportional to thickness. Varying the pH of the precursor solution during membrane preparation has no significant effect on the oxygen flux or the reaction. The CH 4:CO2 feed ratio significantly affects the hydrogen production over the BSCF membrane. Altering the CH4:CO2 ratio has a direct impact on the oxygen flux, which in turn can influence the reaction pathway. These studies suggest that the Pt-Ni/CeZrO2 catalyst might be suitable for low-temperature hydrocarbon conversion reactions over thin BSCF ceramic membranes. Most importantly, the BSCF membrane can reduce the apparent activation energy of the CO2 reforming reaction by changing the reaction pathway to include more steam reforming.

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

DOE PAGES

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

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

NASA Astrophysics Data System (ADS)

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

2017-04-01

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

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

PubMed Central

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

2013-01-01

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

In situ high temperature MAS NMR study of the mechanisms of catalysis. Ethane aromatization on Zn-modified zeolite BEA.

PubMed

Arzumanov, Sergei S; Gabrienko, Anton A; Freude, Dieter; Stepanov, Alexander G

2009-04-01

Ethane conversion into aromatic hydrocarbons over Zn-modified zeolite BEA has been analyzed by high-temperature MAS NMR spectroscopy. Information about intermediates (Zn-ethyl species) and reaction products (mainly toluene and methane), which were formed under the conditions of a batch reactor, was obtained by (13)C MAS NMR. Kinetics of the reaction, which was monitored by (1)H MAS NMR in situ at the temperature of 573K, provided information about the reaction mechanism. Simulation of the experimental kinetics within the frames of the possible kinetic schemes of the reaction demonstrates that a large amount of methane evolved under ethane aromatization arises from the stage of direct ethane hydrogenolysis.

Carbon nanotubes accelerate methane production in pure cultures of methanogens and in a syntrophic coculture.

PubMed

Salvador, Andreia F; Martins, Gilberto; Melle-Franco, Manuel; Serpa, Ricardo; Stams, Alfons J M; Cavaleiro, Ana J; Pereira, M Alcina; Alves, M Madalena

2017-07-01

Carbon materials have been reported to facilitate direct interspecies electron transfer (DIET) between bacteria and methanogens improving methane production in anaerobic processes. In this work, the effect of increasing concentrations of carbon nanotubes (CNT) on the activity of pure cultures of methanogens and on typical fatty acid-degrading syntrophic methanogenic coculture was evaluated. CNT affected methane production by methanogenic cultures, although acceleration was higher for hydrogenotrophic methanogens than for acetoclastic methanogens or syntrophic coculture. Interestingly, the initial methane production rate (IMPR) by Methanobacterium formicicum cultures increased 17 times with 5 g·L -1 CNT. Butyrate conversion to methane by Syntrophomonas wolfei and Methanospirillum hungatei was enhanced (∼1.5 times) in the presence of CNT (5 g·L -1 ), but indications of DIET were not obtained. Increasing CNT concentrations resulted in more negative redox potentials in the anaerobic microcosms. Remarkably, without a reducing agent but in the presence of CNT, the IMPR was higher than in incubations with reducing agent. No growth was observed without reducing agent and without CNT. This finding is important to re-frame discussions and re-interpret data on the role of conductive materials as mediators of DIET in anaerobic communities. It also opens new challenges to improve methane production in engineered methanogenic processes. © 2017 The Authors. Environmental Microbiology published by Society for Applied Microbiology and John Wiley & Sons Ltd.

Monocopper active site for partial methane oxidation in Cu-exchanged 8MR zeolites

DOE PAGES

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

Postextraction Separation, On-Board Storage, and Catalytic Conversion of Methane in Natural Gas: A Review.

PubMed

Saha, Dipendu; Grappe, Hippolyte A; Chakraborty, Amlan; Orkoulas, Gerassimos

2016-10-12

In today's perspective, natural gas has gained considerable attention, due to its low emission, indigenous availability, and improvement in the extraction technology. Upon extraction, it undergoes several purification protocols including dehydration, sweetening, and inert rejection. Although purification is a commercially established technology, several drawbacks of the current process provide an essential impetus for developing newer separation protocols, most importantly, adsorption and membrane separation. This Review summarizes the needs of natural gas separation, gives an overview of the current technology, and provides a detailed discussion of the progress in research on separation and purification of natural gas including the benefits and drawbacks of each of the processes. The transportation sector is another growing sector of natural gas utilization, and it requires an efficient and safe on-board storage system. Compressed natural gas (CNG) and liquefied natural gas (LNG) are the most common forms in which natural gas can be stored. Adsorbed natural gas (ANG) is an alternate storage system of natural gas, which is advantageous as compared to CNG and LNG in terms of safety and also in terms of temperature and pressure requirements. This Review provides a detailed discussion on ANG along with computation predictions. The catalytic conversion of methane to different useful chemicals including syngas, methanol, formaldehyde, dimethyl ether, heavier hydrocarbons, aromatics, and hydrogen is also reviewed. Finally, direct utilization of methane onto fuel cells is also discussed.

Polarization of Light by Leaves and Plant Canopies

NASA Technical Reports Server (NTRS)

Vanderbilt, V. C.

2006-01-01

This talk will focus first on the information contained in the surface-scattered light from leaves, plant canopies and surface waters. This light is in general polarized and depends upon surface roughness. Thus, for example, - The surface reflection from shiny green leaves measured in the specular direction shows no chlorophyll absorption bands, no 'red edge.' - Conversely, the degree of linear polarization of such light displays marked variation with wavelength having local maxima in the chlorophyll absorption bands and an inverted red edge. - Plant canopies with shiny leaves distributed in angle like the area on a sphere, specularly reflect sunlight in the subsolar or specular direction- but also in every other view direction. - Canopies of green plants may appear white not green when viewed obliquely toward the sun. - In a light to moderate wind, the often blindingly bright glitter of sunlight off smooth water surfaces provides a strong, angularly narrow signature reflection characteristic of inundated vegetated areas that are big sources of atmospheric methane, a climatically important greenhouse gas. (Conversely, a blindingly bright glitter-type reflection is uncharacteristic of upland or wind ruffled open water areas that are poor sources of atmospheric methane.) Because some of these results may be 'head scratchers,' it's always important to properly calibrate ones instruments. Indeed, as the second portion of the talk will show, the characteristics of the light measuring instrument, particularly its entrance aperture, may affect the results and should be taken into account during across-instrument data comparisons.

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

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

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

DOE PAGES

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

Changes in soil carbon cycling accompanying conversion of row-crop fields to grazing dairy pastures

NASA Astrophysics Data System (ADS)

Thompson, A.; Kramer, M. G.; Hill, N.; Machmuller, M. B.; Cyle, K.

2011-12-01

Increasingly, the dairy industry in the eastern US is transitioning from total confinement dairy systems (TCD) toward pasture-based, management intensive grazing dairy (MiGD) systems. This transition is driven by the fact that MiGDs require substantially less operating capital and are more economically efficient than TCD systems. Consequently, the impact of this transition and shift in land-use practice on carbon dynamics may be considerable. Land-use in a Management intensive Grazing Dairy (MiGD) system is fundamentally different than conventional confinement dairies and conventional no-till pastures. The forage system involves rotational grazing at optimal digestibility, when the plants are immature (~20-days) and consequently protein-rich. MiGD cows spend >90% of their time in the field and deposit > 90% of their waste directly to the soil surface. Thus, little above ground plant residues are directly returned to the soil, but rather substantial C inputs derive from bovine manure. We sampled a MiGD-chronosequence of row-crop to MiGD conversion established in 2007 in eastern Georgia. All soils across the MiGD-chronosequence, all occur in relative (40 km) close proximity to one another, are deep, well-drained, fine and fine sandy loam Ultisols formed on Coastal Plain sediments. Prior to MiGD established, the soils were farmed for > 50 yrs using conventional tillage techniques. Our current sampling to 1m depths captures fields at 0, 2, 3, and 5 yrs since conversion. Total soil carbon (C) and the carbon concentration of the clay fraction increased following conversion, with the greatest increases occurring between 3 and 5 yrs since conversion. These C increases were limited to the upper 40cm of the soil, with minimal change occurring at depth. Characterization of the protein and ligand content of these soils via 13C NMR and chemolytic techniques as a function of soil particle density and size is in progress and will be presented along with estimates of carbon dioxide and methane fluxes across the MiGD chronosequence. Our broad goal is to quantify ruminal methane emissions and changes to soil C-stocks and stability associated with this land-use shift. Our preliminary data suggest such a land-use change will likely improve soil health and increase C-stocks. Balancing this against potential increases in methane emissions is a key knowledge gap for future southeastern U.S. C-cycling estimates.

Sorghums for methane production. Final report, April 1983 to March 1986

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

Hiler, E.A.; Miller, F.R.; Dominy, R.E.

1986-06-01

The objective of the research is to develop an integrated system for methane production utilizing high-energy sorghum as the feedstock. The report provides specifics of research activities in the sorghums-for-methane production program sponsored by Gas Research Institute and co-funded by Texas Agricultural Experiment Station. Emphasis is placed on third-year results in the report since first- and second-year results are given in earlier reports. Researchers in the program include plant geneticists, sorghum physiologists, chemists, agronomists, ruminant physiologists, agricultural and systems engineers, and agricultural economists. Major research emphasis is on genetic manipulation, physiology and production systems, harvesting, storage, processing and conversion systems,more » inhibitors, and economic and systems analyses. During the third year, increasing emphasis continued on the storage, processing, and conversion aspects of the program because of the critical importance of high efficiency and conversion to the economic implementation of the system.« less

Anaerobic digestion of water hyacinth and sludge

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

Biljetina, R.; Srivastava, V.J.; Chynoweth, D.P.

1986-01-01

The Institute of Gas Technology (IGT) has been operating an experimental test unit (ETU) at the Walt Disney World (WDW) wastewater treatment plant to demonstrate the conversion of water hyacinth and sludge to methane in a solids concentrating (SOLCON) digester. Results from 2 years to operation have confirmed earlier laboratory observations that this digester achieves higher methane yields and solids conversion than those observed in continuous stirred tank reactors. Methane yields as high as 0.49 m/sup 3/ kg/sup -1/ (7.9 SCF/lb) volatile solids added have been obtained during steady-state operation on a blend of water hyacinth and sludge. 9 refs.,more » 5 figs., 5 tabs.« less

Photoreduction of CO{sub 2} by TiO{sub 2} nanocomposites synthesized through reactive direct current magnetron sputter deposition.

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

Chen, L.; Graham, M. E.; Li, G.

The photoreduction of CO{sub 2} into methane provides a carbon-neutral energy alternative to fossil fuels, but its feasibility requires improvements in the photo-efficiency of materials tailored to this reaction. We hypothesize that mixed phase TiO{sub 2} nano-materials with high interfacial densities are extremely active photocatalysts well suited to solar fuel production by reducing CO{sub 2} to methane and shifting to visible light response. Mixed phase TiO{sub 2} films were synthesized by direct current (DC) magnetron sputtering and characterized by X-ray diffraction (XRD), atomic force microscope (AFM), scanning electron microscope (SEM) and transmission electron microscope (TEM). Bundles of anatase-rutile nano-columns havingmore » high densities of two kinds of interfaces (those among the bundles and those between the columns) are fabricated. Films sputtered at a low deposition angle showed the highest methane yield, compared to TiO{sub 2} fabricated under other sputtering conditions and commercial standard Degussa P25 under UV irradiation. The yield of methane could be significantly increased ({approx} 12% CO{sub 2} conversion) by increasing the CO{sub 2} to water ratio and temperature (< 100 C) as a combined effect. These films also displayed a light response strongly shifted into the visible range. This is explained by the creation of non-stoichiometric titania films having unique features that we can potentially tailor to the solar energy applications.« less

Development of a carbon formation reactor for carbon dioxide reduction

NASA Technical Reports Server (NTRS)

Noyes, G.

1985-01-01

Applied research, engineering development, and performance evaluation were conducted on a process for formation of dense carbon by pyrolysis of methane. Experimental research showed that dense (0.7 to 1.6 g/cc bulk density and 1.6 to 2.2 g/cc solid density) carbon can be produced by methane pyrolysis in quartzwool-packed quartz tubes at temperatrues of 1100 to 1300 C. This result supports the condensation theory of pyrolytic carbon formation from gaseous hydrocarbons. A full-scale Breadboard Carbon Formation Reactor (CFR) was designed, fabricated, and tested at 1100 to 1200 C with 380 to 2280 sccm input flows of methane. Single-pass conversion of methane to carbon ranged from 60 to 100 percent, with 89 percent average conversion. Performance was projected for an Advanced Carbon Reactor Subsystem (ACRS) which indicated that the ACRS is a viable option for management of metabolic carbon on long-duration space missions.

Steam conversion of liquefied petroleum gas and methane in microchannel reactor

NASA Astrophysics Data System (ADS)

Dimov, S. V.; Gasenko, O. A.; Fokin, M. I.; Kuznetsov, V. V.

2018-03-01

This study presents experimental results of steam conversion of liquefied petroleum gas and methane in annular catalytic reactor - heat exchanger. The steam reforming was done on the Rh/Al2O3 nanocatalyst with the heat applied through the microchannel gap from the outer wall. Concentrations of the products of chemical reactions in the outlet gas mixture are measured at different temperatures of reactor. The range of channel wall temperatures at which the ratio of hydrogen and carbon oxide in the outlet mixture grows substantially is determined. Data on the composition of liquefied petroleum gas conversion products for the ratio S/C = 5 was received for different GHVS.

Directly converting CO2 into a gasoline fuel

PubMed Central

Wei, Jian; Ge, Qingjie; Yao, Ruwei; Wen, Zhiyong; Fang, Chuanyan; Guo, Lisheng; Xu, Hengyong; Sun, Jian

2017-01-01

The direct production of liquid fuels from CO2 hydrogenation has attracted enormous interest for its significant roles in mitigating CO2 emissions and reducing dependence on petrochemicals. Here we report a highly efficient, stable and multifunctional Na–Fe3O4/HZSM-5 catalyst, which can directly convert CO2 to gasoline-range (C5–C11) hydrocarbons with selectivity up to 78% of all hydrocarbons while only 4% methane at a CO2 conversion of 22% under industrial relevant conditions. It is achieved by a multifunctional catalyst providing three types of active sites (Fe3O4, Fe5C2 and acid sites), which cooperatively catalyse a tandem reaction. More significantly, the appropriate proximity of three types of active sites plays a crucial role in the successive and synergetic catalytic conversion of CO2 to gasoline. The multifunctional catalyst, exhibiting a remarkable stability for 1,000 h on stream, definitely has the potential to be a promising industrial catalyst for CO2 utilization to liquid fuels. PMID:28462925

Directly converting CO2 into a gasoline fuel.

PubMed

Wei, Jian; Ge, Qingjie; Yao, Ruwei; Wen, Zhiyong; Fang, Chuanyan; Guo, Lisheng; Xu, Hengyong; Sun, Jian

2017-05-02

The direct production of liquid fuels from CO 2 hydrogenation has attracted enormous interest for its significant roles in mitigating CO 2 emissions and reducing dependence on petrochemicals. Here we report a highly efficient, stable and multifunctional Na-Fe 3 O 4 /HZSM-5 catalyst, which can directly convert CO 2 to gasoline-range (C 5 -C 11 ) hydrocarbons with selectivity up to 78% of all hydrocarbons while only 4% methane at a CO 2 conversion of 22% under industrial relevant conditions. It is achieved by a multifunctional catalyst providing three types of active sites (Fe 3 O 4 , Fe 5 C 2 and acid sites), which cooperatively catalyse a tandem reaction. More significantly, the appropriate proximity of three types of active sites plays a crucial role in the successive and synergetic catalytic conversion of CO 2 to gasoline. The multifunctional catalyst, exhibiting a remarkable stability for 1,000 h on stream, definitely has the potential to be a promising industrial catalyst for CO 2 utilization to liquid fuels.

Final Scientific/Technical Report for project “Increasing the Rate and Extent of Microbial Coal to Methane Conversion through Optimization of Microbial Activity, Thermodynamics, and Reactive Transport”

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

Efficient 1.6 Micron Laser Source for Methane DIAL

NASA Technical Reports Server (NTRS)

Shuman, Timothy; Burnham, Ralph; Nehrir, Amin R.; Ismail, Syed; Hair, Johnathan W.

2013-01-01

Methane is a potent greenhouse gas and on a per molecule basis has a warming influence 72 times that of carbon dioxide over a 20 year horizon. Therefore, it is important to look at near term radiative effects due to methane to develop mitigation strategies to counteract global warming trends via ground and airborne based measurements systems. These systems require the development of a time-resolved DIAL capability using a narrow-line laser source allowing observation of atmospheric methane on local, regional and global scales. In this work, a demonstrated and efficient nonlinear conversion scheme meeting the performance requirements of a deployable methane DIAL system is presented. By combining a single frequency 1064 nm pump source and a seeded KTP OPO more than 5 mJ of 1.6 µm pulse energy is generated with conversion efficiencies in excess of 20%. Even without active cavity control instrument limited linewidths (50 pm) were achieved with an estimated spectral purity of 95%. Tunable operation over 400 pm (limited by the tuning range of the seed laser) was also demonstrated. This source demonstrated the critical needs for a methane DIAL system motivating additional development of the technology.

40 CFR Table A-7 to Subpart A of... - Data Elements That Are Inputs to Emission Equations and for Which the Reporting Deadline Is March...

Code of Federal Regulations, 2013 CFR

2013-07-01

... mass balance equation. K 98.116(b) Only annual production by product from each EAF (No CEMS). K 98.116... contributed by methane. Y 98.256(f)(7) Only molar volume conversion factor. Y 98.256(f)(10) Only coke burn-off... methane in coking gas. Y 98.256(l)(5) Only molar volume conversion factor. Y 98.256(m)(3) Only total...

Application of methane fermentation technology into organic wastes in closed agricultural system

NASA Astrophysics Data System (ADS)

Endo, Ryosuke; Kitaya, Yoshiaki

Sustainable and recycling-based systems are required in space agriculture which takes place in an enclosed environment. Methane fermentation is one of the most major biomass conversion technologies, because (1) it provides a renewable energy source as biogas including methane, suitable for energy production, (2) the nutrient-rich solids left after digestion can be used as compost for agriculture. In this study, the effect of the application of methane fermentation technology into space agriculture on the material and energy cycle was investigated.

Pilot plant operation of a nonadiabatic methanation reactor. [15 refs. ; Raney nickel catalyst

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

Schehl, R.R.; Pennline, H.W.; Strakey, J.P.

The design and operation of a pilot plant scale hybrid methanation reactor is discussed. The hybrid methanator, utilizing a finned, Raney nickel coated insert, consolidates features of the tube-wall and hot-gas-recycle methanation reactors. Data are presented from four tests lasting from 3/sup 1///sub 2/ weeks to three months. Topics discussed include conversion, product yields, catalyst properties, and reactor temperature profiles. A one-dimensional mathematical model capable of explaining reactor performance trends is employed.

Catalytic Conversion of Cellulosic Biomass or Algal Biomass plus Methane to Drop in Hydrocarbon Fuels and Chemicals

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

Marker, Terry; Roberts, Michael; Linck, Martin

The goal of this Bioincubator Project was to improve the pyrolysis of biomass through the use of methane. Our initial concept was to use methane as a fluidizing gas with a hydrogen transfer catalyst. The results of the experiments did show that methane as a fluidizing gas, with a hydrogen transfer catalyst, does enhance catalytic pyrolysis over that which is achieved with an inert fluidizing gas. Using methane as a fluidizing gas, with a hydrogen transfer catalyst, consistently produced better products with lower oxygen content than the products produced when an inert gas was used. These improvements were also consistentmore » with the results obtained through pure component testing as well. However, the improvement was too small to justify any significant expense. The addition of hydrogen with a hydrogen transfer catalyst consistently showed a much greater, more significant effect than methane. This indicates that hydropyrolysis is a more effective approach to improved catalytic pyrolysis than methane addition. During the course of this project, another way to significantly increase biogenic liquid yields from pyrolysis through the use of methane was discovered. We discovered a remarkably stable CO2/steam reforming catalyst which directly makes a 2:1 H2/CO synthesis gas from the CO, CO2, methane, ethane and propane product gas from integrated hydropyrolysis and hydroconversion (IH2®). The biogenic synthesis gas can then be converted to liquid hydrocarbons using Fischer Tropsch. The hydrogen for the IH2 unit would then be provided through the use of added methane. By utilizing the biogenic gas to make liquids, 40% more biogenic liquid hydrocarbons can be made from wood, thereby increasing liquid yields from IH2 from 86GPT to 126GPT. It also simplifies the hydrogen plant since no CO or CO2 removal is required.« less

Catalyst for the methanation of carbon monoxide in sour gas

DOEpatents

Kustes, William A.; Hausberger, Arthur L.

1985-01-01

The invention involves the synergistic effect of the specific catalytic constituents on a specific series of carriers for the methanation of carbon monoxide in the presence of sulfur at relatively high temperatures and at low steam to gas ratios in the range of 0.2:1 or less. This effect was obtained with catalysts comprising the mixed sulfides and oxides of nickel and chromium supported on carriers comprising magnesium aluminate and magnesium silicate. Conversion of carbon monoxide to methane was in the range of from 40 to 80%. Tests of this combination of metal oxides and sulfides on other carriers and tests of other metal oxides and sulfides on the same carrier produced a much lower level of conversion.

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

Anaerobic co-digestion of steam-treated Quercus serrata chips and sewage sludge under mesophilic and thermophilic conditions.

PubMed

Wang, Feng; Hidaka, Taira; Sakurai, Kensuke; Tsumori, Jun

2014-08-01

The biodegradation of Quercus serrata chips was evaluated by anaerobic digestion under various steam explosion conditions. In continuous experiments, untreated chips (W₀) and chips steam-treated at less than 1.0 MPa (W₁) and 2.0 MPa (W₄) were co-digested with sewage sludge (S₁ and S₂) taken from two different wastewater treatment plants. The apparent methane yield of W₁ and W₄ co-digested with S₁ (thermophilic) was 261 dm(3)/kgVS (volatile solids) and 248 dm(3)/kgVS, respectively. The apparent methane yield of W₄ co-digested with S₂ was 258 dm(3)/kgVS (mesophilic) and 271 dm(3)/kgVS (thermophilic). Methane production was inhibited by W₀ due to components released during hydrolysis. The methane conversion ratio of pretreated chips obtained in batch experiments varied from 40.5% to 53.8% (mesophilic) and from 49.0% to 63.7% (thermophilic). The methane conversion ratio increased with decreasing acid-soluble lignin content in the chips. Copyright © 2014 Elsevier Ltd. All rights reserved.

Thermodynamic analysis on the CO2 conversion processes of methane dry reforming for hydrogen production and CO2 hydrogenation to dimethyl ether

NASA Astrophysics Data System (ADS)

He, Xinyi; Liu, Liping

2017-12-01

Based on the principle of Gibbs free energy minimization, the thermodynamic analysis on the CO2 conversion processes of dry reforming of methane for H2 and CO2 hydrogenation to dimethyl ether was carried out. The composition of the reaction system was determined on the basis of reaction mechanism. The effects of reaction temperature, pressure and raw material composition on the equilibrium conversion and the selectivity of products were analyzed. The results show that high temperature, low pressure, CO2/CH4 molar ratio of 1.0-1.5 and appropriate amount of oxygen are beneficial to the dry reforming of methane. For CO2 hydrogenation to dimethyl ether, low temperature, high pressure, the appropriate H2/CO2 and the proper CO addition in feed are favorable. The calculated results are compared with the relevant studies, indicating that industrial catalytic technology needs further improvement.

Direct catalytic conversion of methane and light hydrocarbon gases. Quarterly report No. 9, October 1--December 31, 1988

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

Consumption of methane by soils.

PubMed

Dueñas, C; Fernández, M C; Carretero, J; Pérez, M; Liger, E

1994-05-01

Measurements of the methane flux and methane concentration profiles in soil air are presented. The flux of methane from the soil is calculated by two methods: a) Direct by placing a static open chamber at the soil surface. b) Indirect, using the (222)Rn concentrations profile and the (222)Rn flux in the soil surface in parallel with the methane concentration ((222)Rn calibrated fluxes). The methane flux has been determined in two kinds of soils (sandy and loamy) in the surroundings of Málaga (SPAIN). The directly measured methane fluxes at all investigated sites is higher than methane fluxes derived from "Rn calibrated fluxes". Atmospheric methane is consumed by soils, mean direct flux to the atmosphere were - 0.33 g m(-2)yr-1. The direct methane flux is the same within the measuring error in sandy and loamy soils. The influence of the soil parameters on the methane flux indicates that microbial decomposition of methane is primarily controlled by the transport of methane.

Biogasification of Walt Disney World biomass waste blend. Final report, January 1982-December 1985

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

Biljetina, R.; Chynoweth, D.P.; Srivastava, V.J.

1986-10-01

The objective of the 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 operated 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 results in themore » production of methane and other useful products. The digester was operated as a non-mixed, solids concentrating digester to encourage higher solids and microorganism retention times. Data collected during six steady-state operating periods confirmed earlier laboratory observations that this digester consistently produces 15 to 25% higher methane yields and conversions when compared to conventional stirred-tank digester. Digester operation was evaluated at different loading rates, solids blend ratios and feed configurations. Results from the program have provided a data base for the design of larger conversion systems.« less

Cu-ZSM-5 catalyzed low-temperature hydrogen peroxide-induced methane-to-methanol conversion

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

Zhang, Yang; Li, Zhenglong; Allard, Jr., Lawrence Frederick

2017-01-01

We report that Cu-ZSM-5 is an effective catalyst for methane oxidation with hydrogen peroxide. We find that synthesis via ion-exchage and reaction conditions are important factors for the observed efficiency of Cu-ZSM-5.

Ammonium conversion and its feedback effect on methane oxidation of Methylosinus sporium.

PubMed

He, Ruo; Chen, Min; Ma, Ruo-Chan; Su, Yao; Zhang, Xuan

2017-04-01

Ammonium (NH 4 + ) is not only nitrogen source that can support methanotrophic growth, but also it can inhibit methane (CH 4 ) oxidation by competing with CH 4 for the active site of methane monooxygenase. NH 4 + conversion and its feedback effect on the growth and activity of methanotrophs were evaluated with Methylosinus sporium used as a model methanotroph. Nitrogen sources could affect the CH 4 -derived carbon distribution, which varied with incubation time and nitrogen concentrations. More CH 4 -derived carbon was incorporated into biomass in the media with NH 4 + -N, compared to nitrate-nitrogen (NO 3 - -N), as sole nitrogen source at the nitrogen concentrations of 10-18 mmol L -1 . Although ammonia (NH 3 ) oxidation activity of methanotrophs was considerably lower, only accounting for 0.01-0.06% of CH 4 oxidation activity in the experimental cultures, NH 4 + conversion could lead to the pH decrease and toxic intermediates accumulation in the their habits. Compared with NH 4 + , nitrite (NO 2 - ) accumulation in the NH 4 + conversion of methanotroph had stronger inhibition on its activity, especially the joint inhibition of NO 2 - accumulation and the pH decrease during the NH 4 + -N conversion. These results suggested that more attention should be paid to the feedback effects of NH 4 + conversion by methanotrophs to understand effects of NH 4 + on CH 4 oxidation in the environments. Copyright © 2017 The Society for Biotechnology, Japan. Published by Elsevier B.V. All rights reserved.

LanzaTech- Capturing Carbon. Fueling Growth.

ScienceCinema

NONE

2018-01-16

LanzaTech will design a gas fermentation system that will significantly improve the rate at which methane gas is delivered to a biocatalyst. Current gas fermentation processes are not cost effective compared to other gas-to-liquid technologies because they are too slow for large-scale production. If successful, LanzaTech's system will process large amounts of methane at a high rate, reducing the energy inputs and costs associated with methane conversion.

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

PubMed

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

2014-01-01

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

Potential for direct interspecies electron transfer in methanogenic wastewater digester aggregates.

PubMed

Morita, Masahiko; Malvankar, Nikhil S; Franks, Ashley E; Summers, Zarath M; Giloteaux, Ludovic; Rotaru, Amelia E; Rotaru, Camelia; Lovley, Derek R

2011-01-01

Mechanisms for electron transfer within microbial aggregates derived from an upflow anaerobic sludge blanket reactor converting brewery waste to methane were investigated in order to better understand the function of methanogenic consortia. The aggregates were electrically conductive, with conductivities 3-fold higher than the conductivities previously reported for dual-species aggregates of Geobacter species in which the two species appeared to exchange electrons via interspecies electron transfer. The temperature dependence response of the aggregate conductance was characteristic of the organic metallic-like conductance previously described for the conductive pili of Geobacter sulfurreducens and was inconsistent with electron conduction through minerals. Studies in which aggregates were incubated with high concentrations of potential electron donors demonstrated that the aggregates had no significant capacity for conversion of hydrogen to methane. The aggregates converted formate to methane but at rates too low to account for the rates at which that the aggregates syntrophically metabolized ethanol, an important component of the reactor influent. Geobacter species comprised 25% of 16S rRNA gene sequences recovered from the aggregates, suggesting that Geobacter species may have contributed to some but probably not all of the aggregate conductivity. Microorganisms most closely related to the acetate-utilizing Methanosaeta concilii accounted for more than 90% of the sequences that could be assigned to methane producers, consistent with the poor capacity for hydrogen and formate utilization. These results demonstrate for the first time that methanogenic wastewater aggregates can be electrically conductive and suggest that direct interspecies electron transfer could be an important mechanism for electron exchange in some methanogenic systems.

Effect of ferrihydrite biomineralization on methanogenesis in an anaerobic incubation from paddy soil

NASA Astrophysics Data System (ADS)

Zhuang, Li; Xu, Jielong; Tang, Jia; Zhou, Shungui

2015-05-01

Microbial reduction of Fe(III) can be one of the major factors controlling methane production from anaerobic sedimentary environments, such as paddy soils and wetlands. Although secondary iron mineralization following Fe(III) reduction is a process that occurs naturally over time, it has not yet been considered in methanogenic systems. This study performed a long-term anaerobic incubation of a paddy soil and ferrihydrite-supplemented soil cultures to investigate methanogenesis during ferrihydrite biomineralization. The results revealed that the long-term effect of ferrihydrite on methanogenesis may be enhancement rather than suppression documented in previous studies. During initial microbial ferrihydrite reduction, methanogenesis was suppressed; however, the secondary minerals of magnetite formation was simultaneous with facilitated methanogenesis in terms of average methane production rate and acetate utilization rate. In the phase of magnetite formation, microbial community analysis revealed a strong stimulation of the bacterial Geobacter, Bacillus, and Sedimentibacter and the archaeal Methanosarcina in the ferrihydrite-supplemented cultures. Direct electric syntrophy between Geobacter and Methanosarcina via conductive magnetite is the plausible mechanism for methanogenesis acceleration along with magnetite formation. Our data suggested that a change in iron mineralogy might affect the conversion of anaerobic organic matter to methane and might provide a fresh perspective on the mitigation of methane emissions from paddy soils by ferric iron fertilization.

Ammonia chemistry in a flameless jet

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

Zieba, Mariusz; Schuster, Anja; Scheffknecht, Guenter

2009-10-15

In this paper, the nitrogen chemistry in an ammonia (NH{sub 3}) doped flameless jet is investigated using a kinetic reactor network model. The reactor network model is used to explain the main differences in ammonia chemistry for methane (CH{sub 4})-containing fuels and methane-free fuels. The chemical pathways of nitrogen oxides (NO{sub x}) formation and destruction are identified using rate-of-production analysis. The results show that in the case of natural gas, ammonia reacts relatively late at fuel lean condition leading to high NO{sub x} emissions. In the pre-ignition zone, the ammonia chemistry is blocked due to the absence of free radicalsmore » which are consumed by methane-methyl radical (CH{sub 3}) conversion. In the case of methane-free gas, the ammonia reacted very rapidly and complete decomposition was reached in the fuel rich region of the jet. In this case the necessary radicals for the ammonia conversion are generated from hydrogen (H{sub 2}) oxidation. (author)« less

Method for in situ biological conversion of coal to methane

DOEpatents

Volkwein, Jon C.

1995-01-01

A method and apparatus are provided for the in situ biological conversion of coal to methane comprising culturing on a coal-containing substrate a consortium of microorganisms capable of degrading the coal into methane under suitable conditions. This consortium of microorganisms can be obtained from an underground cavity such as an abandoned mine which underwent a change from being supplied with sewage to where no sewage was present, since these conditions have favored the development of microorganisms capable of using coal as a carbon source and converting coal to methane. The consortium of microorganisms obtained from such abandoned coal mines can be isolated and introduced to hard-to-reach coal-containing substrates which lack such microorganisms and which would otherwise remain unrecoverable. The present invention comprises a significant advantage in that useable energy can be obtained from a number of abandoned mine sites or other areas wherein coal is no longer being recovered, and such energy can be obtained in a safe, efficient, and inexpensive manner.

How Does Poly(hydroxyalkanoate) Affect Methane Production from the Anaerobic Digestion of Waste-Activated Sludge?

PubMed

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.

Samaria-doped Ceria Modified Ni/YSZ Anode for Direct Methane Fuel in Tubular Solid Oxide Fuel Cells by Impregnation Method

NASA Astrophysics Data System (ADS)

Zhang, Long-shan; Gao, Jian-feng; Tian, Rui-fen; Xia, Chang-rong

2009-08-01

A porous NiO/yttria-stabilized zirconia anode substrate for tubular solid oxide fuel cells was prepared by gel casting technique. Nano-scale samaria-doped ceria (SDC) particles were formed onto the anode substrate to modify the anode microstructure by the impregnation of solution of Sm(NO3)3 and Ce(NO3)3. Electrochemical impedance spectroscopy, current-voltage and current-powder curves of the cells were measured using an electrochemical workstation. Scanning electron microcopy was used to observe the microstructure. The results indicate that the stability of the performance of the cell operated on humidified methane can be significantly improved by incorporating the nano-structured SDC particles, compared with the unmodified cell. This verifies that the coated SDC electrodes are very effective in suppressing catalytic carbon formation by blocking methane from approaching the Ni, which is catalytically active towards methane pyrolysis. In addition, it was found that a small amount of deposited carbon is beneficial to the performance of the anode. The cell showed a peak power density of 225 mW/cm2 when it was fed with H2 fuel at 700 °C, but the power density increased to 400 mW/cm2 when the fuel was switched from hydrogen to methane at the same flow rate. Methane conversion achieved about 90%, measured by gas chromatogram with a 10.0 mL/min flow rate of fuel at 700 °C. Although the carbon deposition was not suppressed absolutely, some deposited carbon was beneficial for performance improvement.

Genome-Scale Metabolic Reconstructions and Theoretical Investigation of Methane Conversion in Methylomicrobium buryatense Strain 5G(B1)

DOE PAGES

de la Torre, Andrea; Metivier, Aisha; Chu, Frances; ...

2015-11-25

Methane-utilizing bacteria (methanotrophs) are capable of growth on methane and are attractive systems for bio-catalysis. However, the application of natural methanotrophic strains to large-scale production of value-added chemicals/biofuels requires a number of physiological and genetic alterations. An accurate metabolic model coupled with flux balance analysis can provide a solid interpretative framework for experimental data analyses and integration.

Final technical report for the Center for Catalytic Hydrocarbon Functionalization (an EFRC)

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

Gunnoe, Thomas Brent

Greater than 95% of all materials produced by the chemical industry are derived from a small slate of simple hydrocarbons that are derived primarily from natural gas and petroleum, predominantly through oxygenation, C–C bond formation, halogenation or amination. Yet, current technologies for hydrocarbon conversion are typically high temperature, multi-step processes that are energy and capital intensive and result in excessive emissions (including carbon dioxide). The Center for Catalytic Hydrocarbon Functionalization (CCHF) brought together research teams with the broad coalition of skills and knowledge needed to make the fundamental advances in catalysis required for next-generation technologies to convert hydrocarbons (particularly lightmore » alkanes and methane) at high efficiency and low cost. Our new catalyst technologies offer many opportunities including enhanced utilization of natural gas in the transportation sector (via conversion to liquid fuels), more efficient generation of electricity from natural gas using direct methane fuel cells, reduced energy consumption and waste production for large petrochemical processes, and the preparation of high value molecules for use in biological/medical applications or the agricultural sector. The five year collaborative project accelerated fundamental understanding of catalyst design for the conversion of C–H bonds to functionalized products, essential to achieve the goals listed above, as evidenced by the publication of 134 manuscripts. Many of these fundamental advancements provide a foundation for potential commercialization, as evidenced by the submission of 11 patents from research support by the CCHF.« less

Hybrid bioinorganic approach to solar-to-chemical conversion.

PubMed

Nichols, Eva M; Gallagher, Joseph J; Liu, Chong; Su, Yude; Resasco, Joaquin; Yu, Yi; Sun, Yujie; Yang, Peidong; Chang, Michelle C Y; Chang, Christopher J

2015-09-15

Natural photosynthesis harnesses solar energy to convert CO2 and water to value-added chemical products for sustaining life. We present a hybrid bioinorganic approach to solar-to-chemical conversion in which sustainable electrical and/or solar input drives production of hydrogen from water splitting using biocompatible inorganic catalysts. The hydrogen is then used by living cells as a source of reducing equivalents for conversion of CO2 to the value-added chemical product methane. Using platinum or an earth-abundant substitute, α-NiS, as biocompatible hydrogen evolution reaction (HER) electrocatalysts and Methanosarcina barkeri as a biocatalyst for CO2 fixation, we demonstrate robust and efficient electrochemical CO2 to CH4 conversion at up to 86% overall Faradaic efficiency for ≥ 7 d. Introduction of indium phosphide photocathodes and titanium dioxide photoanodes affords a fully solar-driven system for methane generation from water and CO2, establishing that compatible inorganic and biological components can synergistically couple light-harvesting and catalytic functions for solar-to-chemical conversion.

Hybrid bioinorganic approach to solar-to-chemical conversion

PubMed Central

Nichols, Eva M.; Gallagher, Joseph J.; Liu, Chong; Su, Yude; Resasco, Joaquin; Yu, Yi; Sun, Yujie; Yang, Peidong; Chang, Michelle C. Y.; Chang, Christopher J.

2015-01-01

Natural photosynthesis harnesses solar energy to convert CO2 and water to value-added chemical products for sustaining life. We present a hybrid bioinorganic approach to solar-to-chemical conversion in which sustainable electrical and/or solar input drives production of hydrogen from water splitting using biocompatible inorganic catalysts. The hydrogen is then used by living cells as a source of reducing equivalents for conversion of CO2 to the value-added chemical product methane. Using platinum or an earth-abundant substitute, α-NiS, as biocompatible hydrogen evolution reaction (HER) electrocatalysts and Methanosarcina barkeri as a biocatalyst for CO2 fixation, we demonstrate robust and efficient electrochemical CO2 to CH4 conversion at up to 86% overall Faradaic efficiency for ≥7 d. Introduction of indium phosphide photocathodes and titanium dioxide photoanodes affords a fully solar-driven system for methane generation from water and CO2, establishing that compatible inorganic and biological components can synergistically couple light-harvesting and catalytic functions for solar-to-chemical conversion. PMID:26305947

Effect of bio-column composed of aged refuse on methane abatement--a novel configuration of biological oxidation in refuse landfill.

PubMed

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.

CATALYTIC OXIDATION OF METHANE AT LOW SPACE VELOCITIES.

DTIC Science & Technology

methane in airstream through an inhouse designed and fabricated stainless steel reactor. The reactor contained either Hopcalite , 5% V2O5 - 5% MoO3 on...plotted for each catalyst flow rate combination and the effect of space velocity on conversion at constant temperature is shown for the Hopcalite and

Evidence of sulfate-dependent anaerobic methane oxidation within an area impacted by coalbed methane-related gas migration

EPA Science Inventory

The rapid development of unconventional gas resources has been accompanied by an increase in public awareness regarding the potential effects of drilling operations on drinking water sources. Incidents have been reported involving blowouts (e.g., Converse County, WY; Lawrence Tow...

Feasibility of a peat biogasification process

NASA Astrophysics Data System (ADS)

Buivid, M. G.; Wise, D. L.; Rader, A. M.; McCarty, P. L.; Owen, W. F.

1980-07-01

The feasibility of a two-stage biogasification process for the conversion of peat reserves, the energy content of which in the United States is greater than that of uranium, shale oil or petroleum and natural gas combined, into pipeline-quality methane is investigated. Samples of wet-harvested reed-sedge peat were pretreated in alkaline and nonalkaline conditions in the presence and absence of oxidation in order to determine the most favorable conditions for the conversion of cellulosic and lignaceous fractions to water-soluble, fermentable compounds, and the resulting products were subjected to anaerobic fermentation to methane. Conversion efficiencies obtained reveal that up to 26% of the initial heat content of peat was converted to methane when alkaline heat pretreatment was employed. Analysis of the process parameters by a computer model to determine equipment sizes, mass and energy balances and costs indicates that for a 79,200 GJ/day plant the total capital requirement would be $323,000,000, annual operating costs would be $44,000,000 and average SNG cost would be $3.16/GJ, assuming a 90% stream factor with a delivered peat slurry costing $0.0033/kg.

Sludge accumulation and conversion to methane in a septic tank treating domestic wastewater or black water.

PubMed

Elmitwalli, Tarek

2013-01-01

Although the septic tank is the most applied on-site system for wastewater pre-treatment, limited research has been performed to determine sludge accumulation and biogas production in the tank. Therefore a dynamic mathematical model based on the Anaerobic Digestion Model No. 1 (ADM1) was developed for anaerobic digestion of the accumulated sludge in a septic tank treating domestic wastewater or black water. The results showed that influent chemical oxygen demand (COD) concentration and hydraulic retention time (HRT) of the tank mainly control the filling time with sludge, while operational temperature governs characteristics of the accumulated sludge and conversion to methane. For obtaining stable sludge and high conversion, the tank needs to be operated for a period more than a year without sludge wasting. Maximum conversion to methane in the tank is about 50 and 60% for domestic wastewater and black water, respectively. The required period for sludge wasting depends on the influent COD concentration and the HRT, while characteristics of the wasted sludge are affected by operational temperature followed by the influent COD concentration and the HRT. Sludge production from the tank ranges between 0.19 to 0.22 and 0.13 to 0.15 L/(person.d), for the domestic wastewater and black water, respectively.

Partial oxidation of methane by pulsed corona discharges

NASA Astrophysics Data System (ADS)

Hoeben, W. F. L. M.; Boekhoven, W.; Beckers, F. J. C. M.; van Heesch, E. J. M.; Pemen, A. J. M.

2014-09-01

Pulsed corona-induced partial oxidation of methane in humid oxygen or carbon dioxide atmospheres has been investigated for future fuel synthesis applications. The obtained product spectrum is wide, i.e. saturated, unsaturated and oxygen-functional hydrocarbons. The generally observed methane conversion levels are 6-20% at a conversion efficiency of about 100-250 nmol J-1. The main products are ethane, ethylene and acetylene. Higher saturated hydrocarbons up to C6 have been detected. The observed oxygen-functional hydrocarbons are methanol, ethanol and lower concentrations of aldehydes, ketones, dimethylether and methylformate. Methanol seems to be exclusively produced with CH4/O2 mixtures at a maximum production efficiency of 0.35 nmol J-1. CH4/CO2 mixtures appear to yield higher hydrocarbons. Carboxylic acids appear to be mainly present in the aqueous reactor phase, possibly together with higher molecular weight species.

Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol.

PubMed

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.

Biogasification of water hyacinth and sludge for methane production

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

Chynoweth, D.P.; Biljetina, R.; Srivastava, V.J.

1985-01-01

Research is in progress to determine the technical and economic feasibility of treatment of domestic sewage using primary settling and water hyacinth ponds and conversion of the organic products of this treatment (primary sludge and hyacinth) to substitute natural gas. This paper describes the status of the conversion component of this program which is centered on anaerobic digestion of hyacinth/sludge blends to methane. The results of several experiments conducted successfully in a large-scale experimental test unit located at the hyacinth treatment facility at Walt Disney are presented. 11 refs., 5 figs., 4 tabs.

Conversion of (Meth)acrylic acids to methane granular sludge: Initiation by specific anerobic microflora

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

Shtarkman, N.B.; Obraztova, A.Y.; Laurinavichyus, K.S.

1995-03-01

The role of a specific anaerobic microflora in the initiation of degradation of (meth)acrylic acids to methane by granular sludge from a UASB reactor was investigated. Associations of anaerobic bacteria isolated from the anaerobic sludge, which was used for a long time for treatment of wastewater from (meth)acrylate production, were able to realize the initial stage of (meth)acrylic acid decomposition, i.e., a conversion of acrylic and methacrylic acids to propionic and isobutyric acids, respectively. When added to granules, these association played a role of an {open_quotes}initiator{close_quotes} of the degradation process, which was then continued by the granular sludge microflora utilizingmore » propionate and isobutyrate. Some characteristics of the granules adapted to propionate or isobutyrate are presented. The rates of propionate and isobutyrate consumption by adapted granules is, respectively, 21 and 53 times higher than the values obtained for nonadapted granules. A combined use of {open_quotes}initiating{close_quotes} bacteria and adapted granules provided degradation of (meth)acrylic acids with a maximum methane yield. The possibility is discussed of employing the granules, which are adapted to short-chain fatty acids, and the {open_quotes}initiating{close_quotes} bacteria, which accomplish the initial steps of the organic material decomposition to lower fatty acids, for the conversion of various chemical compounds to methane. 10 refs., 3 figs., 2 tabs.« less

Uncertainty propagation in modeling of plasma-assisted hydrogen production from biogas

NASA Astrophysics Data System (ADS)

Zaherisarabi, Shadi; Venkattraman, Ayyaswamy

2016-10-01

With the growing concern of global warming and the resulting emphasis on decreasing greenhouse gas emissions, there is an ever-increasing need to utilize energy-production strategies that can decrease the burning of fossil fuels. In this context, hydrogen remains an attractive clean-energy fuel that can be oxidized to produce water as a by-product. In spite of being an abundant species, hydrogen is seldom found in a form that is directly usable for energy-production. While steam reforming of methane is one popular technique for hydrogen production, plasma-assisted conversion of biogas (carbon dioxide + methane) to hydrogen is an attractive alternative. Apart from producing hydrogen, the other advantage of using biogas as raw material is the fact that two potent greenhouse gases are consumed. In this regard, modeling is an important tool to understand and optimize plasma-assisted conversion of biogas. The primary goal of this work is to perform a comprehensive statistical study that quantifies the influence of uncertain rate constants thereby determining the key reaction pathways. A 0-D chemical kinetics solver in the OpenFOAM suite is used to perform a series of simulations to propagate the uncertainty in rate constants and the resulting mean and standard deviation of outcomes.

Methane on Titan: Photochemical-Meteorological-Hydrogeochemical Cycle

NASA Astrophysics Data System (ADS)

Atreya, S. K.; Niemann, H. B.; Owen, T. C.; Adams, E. Y.; Demick, J. E.; GCMS Team

2005-08-01

Photochemically driven destruction of methane in Titan's stratosphere leads to irreversible conversion to heavier hydrocarbons (1). The latter would largely condense out of the atmosphere (2). In the absence of recycling, Titan's methane would thus be destroyed in 10-100 million years (1). However, methane is key to the maintenance of Titan's nitrogen atmosphere. Without warming provided by CH4-generated hydrocarbon hazes in the stratosphere and pressure induced opacity in the infrared, particularly by H2-N2 and CH4-N2 collisions in the troposphere, the atmosphere would gradually diminish to tens of millibar pressure (3). Thus, the source-sink cycle of methane is crucial to the evolutionary history of Titan and its atmosphere. The GCMS measurements show that a ``methalogical" cycle with surface evaporation, cloud formation, followed by precipitation (rain) of methane exists. However, this ``closed" cycle does not recycle methane lost to heavy hydrocarbons. A source is required. Unlike the deep, hot, H2-rich interiors of the giant planets, Titan's interior is ill suited for thermochemical conversion of hydrocarbons back to methane. Instead we propose that serpentinization is an effective process for producing methane in Titan's interior (4). Hydration of ultramafic silicates, followed by reaction between the released H2 gas and CO2 or carbon grains can produce large quantities of CH4 at relatively mild (40-90oC) temperatures. Such thermal conditions are believed to exist below the purported water-ammonia ocean (5). Storage of methane produced via serpentinization can occur in form of clathrates. Evidence of outgassing from Titan's interior is provided by GCMS (6) and VIMS (7) data. (1) Wilson, Atreya, JGR 109, E06002, doi:10.1029/2003JE002181, 2004. (2) Wilson, Atreya, PSS 51, 1017, 2003. (3) Lorenz etal. Science 275, 642, 1997. (4) Owen etal. Phys. Uspekhi, in press. (5) Grasset, Pargamin, PSS 53, 371, 2005. (6) Niemann etal., Submitted to Nature, 2005. (7) Sotin etal., Nature 435, 786, 2005.

Methane uptake in urban forests and lawns

Treesearch

Peter M. Groffman; Richard V. Pouyat

2009-01-01

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

Conversion of MSW (municipal solids waste) to methane in the SOLCON (solids-concentrating) digester

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

Biljetina, R.; Srivastava, V.J.; Isaacson, H.R.

1988-01-01

The Institute of Gas Technology (IGT) has been operating a 1200- gallon, anaerobic solids-concentrating (SOLCON) digester at the Walt Disney World Resort Complex in Lake Buena Vista, Florida since January of 1984. This digester development work is part of a larger effort, sponsored by the Gas Research Institute (GRI) Southern California Edison, that provides effective community waste treatment and disposal options while recovering a valuable methane resource from these wastes. Excellent conversions to methane have been obtained in the SOLCON digester during 4 years of uninterrupted operation. Data were collected on: (1) Wastes from experimental municipal wastewater treatment applications. Watermore » hyacinths were harvested from secondary wastewater treatment channels and combined with sludge from primary clarifiers to maximize potential methane recoveries in the digester. (2) Wastes from agricultural operations. Sorghum was selected as a candidate because it represents both a potential energy crop, as well as, a waste resource if only portions of the plant are converted after grain production. (3) Wastes from municipal waste collection.« less

Bio-conversion of water hyacinths into methane gas, part 1

NASA Technical Reports Server (NTRS)

Wolverton, B. C.; Mcdonald, R. C.; Gordon, J.

1974-01-01

Bio-gas and methane production from the microbial anaerobic decomposition of water hyacinths (Eichhornia crassipes) (Mart) Solms was investigated. These experiments demonstrated the ability of water hyacinths to produce an average of 13.9 ml of methane gas per gram of wet plant weight. This study revealed that sample preparation had no significant effect on bio-gas and/or methane production. Pollution of water hyacinths by two toxic heavy materials, nickel and cadmium, increased the rate of methane production from 51.8 ml/day for non-contaminated plants incubated at 36 C to 81.0 ml/day for Ni-Cd contaminated plants incubated at the same temperature. The methane content of bio-gas evolved from the anaerobic decomposition of Ni-Cd contaminated plants was 91.1 percent as compared to 69.2 percent methane content of bio-gas collected from the fermentation of non-contaminated plants.

Transient studies of low temperature catalysts for methane conversion. Final report, [September 1992--March 1996

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

Wolf, E.E.

1996-09-30

The objective of this project is to use transient techniques to study gas surface interactions during the oxidative conversion of methane. Two groups of catalysts were studied: a double oxide of vanadium and phosphate or VPO, and double oxides of Ni, Co and Rh and lanthana. The objective of the studies involving the VPO catalyst was to understand gas-surface interactions leading to the formation of formaldehyde. In the second group of catalysts, involving metallo-oxides, the main objective was to study the gas-surface interactions that determine the selectivity to C{sub 2} hydrocarbons or synthesis gas. Transient techniques were used to studymore » the methane-surface interactions and the role of lattice oxygen. The selection of the double oxides was made on the hypothesis that the metal oxide would provide an increase interaction with methane whereas the phosphate or lanthanide would provide the sites for oxygen adsorption. The hypothesis behind this selection of catalysts was that increasing the methane interaction with the catalysts would lower the reaction temperature and thus increase the selectivity to the desired products over the total oxidation reaction. In both groups of catalysts the role of Li as a modifier of the selectivity was also studied in detail.« less

Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol

DOE PAGES

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

Single-site trinuclear copper oxygen clusters in mordenite for selective conversion of methane to methanol

PubMed Central

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

Treatment of gas from an in situ conversion process

DOEpatents

Diaz, Zaida [Katy, TX; Del Paggio, Alan Anthony [Spring, TX; Nair, Vijay [Katy, TX; Roes, Augustinus Wilhelmus Maria [Houston, TX

2011-12-06

A method of producing methane is described. The method includes providing formation fluid from a subsurface in situ conversion process. The formation fluid is separated to produce a liquid stream and a first gas stream. The first gas stream includes olefins. At least the olefins in the first gas stream are contacted with a hydrogen source in the presence of one or more catalysts and steam to produce a second gas stream. The second gas stream is contacted with a hydrogen source in the presence of one or more additional catalysts to produce a third gas stream. The third gas stream includes methane.

Plasma catalytic reforming of methane

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

Bromberg, L.; Cohn, D.R.; Rabinovich, A.

1998-08-01

Thermal plasma technology can be efficiently used in the production of hydrogen and hydrogen-rich gases from methane and a variety of fuels. This paper describes progress in plasma reforming experiments and calculations of high temperature conversion of methane using heterogeneous processes. The thermal plasma is a highly energetic state of matter that is characterized by extremely high temperatures (several thousand degrees Celsius) and high degree of dissociation and substantial degree of ionization. The high temperatures accelerate the reactions involved in the reforming process. Hydrogen-rich gas (50% H{sub 2}, 17% CO and 33% N{sub 2}, for partial oxidation/water shifting) can bemore » efficiently made in compact plasma reformers. Experiments have been carried out in a small device (2--3 kW) and without the use of efficient heat regeneration. For partial oxidation/water shifting, it was determined that the specific energy consumption in the plasma reforming processes is 16 MJ/kg H{sub 2} with high conversion efficiencies. Larger plasmatrons, better reactor thermal insulation, efficient heat regeneration and improved plasma catalysis could also play a major role in specific energy consumption reduction and increasing the methane conversion. A system has been demonstrated for hydrogen production with low CO content ({approximately} 1.5%) with power densities of {approximately} 30 kW (H{sub 2} HHV)/liter of reactor, or {approximately} 10 m{sup 3}/hr H{sub 2} per liter of reactor. Power density should further increase with increased power and improved design.« less

Partial oxidative conversion of methane to methanol through selective inhibition of methanol dehydrogenase in methanotrophic consortium from landfill cover soil.

PubMed

Han, Ji-Sun; Ahn, Chang-Min; Mahanty, Biswanath; Kim, Chang-Gyun

2013-11-01

Using a methanotrophic consortium (that includes Methylosinus sporium NCIMB 11126, Methylosinus trichosporium OB3b, and Methylococcus capsulatus Bath) isolated from a landfill site, the potential for partial oxidation of methane into methanol through selective inhibition of methanol dehydrogenase (MDH) over soluble methane monooxygenase (sMMO) with some selected MDH inhibitors at varied concentration range, was evaluated in batch serum bottle and bioreactor experiments. Our result suggests that MDH activity could effectively be inhibited either at 40 mM of phosphate, 100 mM of NaCl, 40 mM of NH4Cl or 50 μM of EDTA with conversion ratios (moles of CH3OH produced per mole CH4 consumed) of 58, 80, 80, and 43 %, respectively. The difference between extent of inhibition in MDH activity and sMMO activity was significantly correlated (n = 6, p < 0.05) with resultant methane to methanol conversion ratio. In bioreactor study with 100 mM of NaCl, a maximum specific methanol production rate of 9 μmol/mg h was detected. A further insight with qPCR analysis of MDH and sMMO coding genes revealed that the gene copy number continued to increase along with biomass during reactor operation irrespective of presence or absence of inhibitor, and differential inhibition among two enzymes was rather the key for methanol production.

Starvation and recovery in the deep-sea methanotroph Methyloprofundus sedimenti.

PubMed

Tavormina, Patricia L; Kellermann, Matthias Y; Antony, Chakkiath Paul; Tocheva, Elitza I; Dalleska, Nathan F; Jensen, Ashley J; Valentine, David L; Hinrichs, Kai-Uwe; Jensen, Grant J; Dubilier, Nicole; Orphan, Victoria J

2017-01-01

In the deep ocean, the conversion of methane into derived carbon and energy drives the establishment of diverse faunal communities. Yet specific biological mechanisms underlying the introduction of methane-derived carbon into the food web remain poorly described, due to a lack of cultured representative deep-sea methanotrophic prokaryotes. Here, the response of the deep-sea aerobic methanotroph Methyloprofundus sedimenti to methane starvation and recovery was characterized. By combining lipid analysis, RNA analysis, and electron cryotomography, it was shown that M. sedimenti undergoes discrete cellular shifts in response to methane starvation, including changes in headgroup-specific fatty acid saturation levels, and reductions in cytoplasmic storage granules. Methane starvation is associated with a significant increase in the abundance of gene transcripts pertinent to methane oxidation. Methane reintroduction to starved cells stimulates a rapid, transient extracellular accumulation of methanol, revealing a way in which methane-derived carbon may be routed to community members. This study provides new understanding of methanotrophic responses to methane starvation and recovery, and lays the initial groundwork to develop Methyloprofundus as a model chemosynthesizing bacterium from the deep sea. © 2016 John Wiley & Sons Ltd.

All-fiber mid-infrared difference frequency generation source and its application to molecular dispersion spectroscopy

NASA Astrophysics Data System (ADS)

Krzempek, K.; Abramski, K. M.; Nikodem, M.

2017-09-01

A widely tunable, fully monolithic, mid-infrared difference frequency generation source and its application in the dispersion-spectroscopy-based laser trace gas detection of methane and ethane, near 2938 and 2998 cm-1, is presented. Utilizing a fiber pigtailed nonlinear crystal module radically simplified the optical setup, while maintaining a superb conversion efficiency of 20% W-1. Seeded directly from two laser diodes, the source delivered ~0.5 mW of tunable radiation, which was used in a chirped laser dispersion spectroscopy setup, enabling the highly sensitive detection of hydrocarbons.

Reaction pathways involved in CH4 conversion on Pd/Al2O3 catalysts : TAP as a powerful tool for the elucidation of the effective role of the metal/support interface

NASA Astrophysics Data System (ADS)

Granger, Pascal

2016-02-01

Temporal Analysis of Products (TAP) reactor offers an alternative to draw direct structure/activity relationships checked on Natural Gas-fuelled Vehicle (NGV) catalysts Determination of accurate kinetic constants for methane adsorption from single pulse experiments and subsequent investigation of sequential surface reactions from alternative CH4/O2 pulse experiments provides a straightforward visualization of the involvement of the metal/support interface on freshly-prepared catalysts and the loss of this effect on aged single palladium based catalysts.

Formation of Acetylene in the Reaction of Methane with Iron Carbide Cluster Anions FeC3- under High-Temperature Conditions.

PubMed

Li, Hai-Fang; Jiang, Li-Xue; Zhao, Yan-Xia; Liu, Qing-Yu; Zhang, Ting; He, Sheng-Gui

2018-03-01

The underlying mechanism for non-oxidative methane aromatization remains controversial owing to the lack of experimental evidence for the formation of the first C-C bond. For the first time, the elementary reaction of methane with atomic clusters (FeC 3 - ) under high-temperature conditions to produce C-C coupling products has been characterized by mass spectrometry. With the elevation of temperature from 300 K to 610 K, the production of acetylene, the important intermediate proposed in a monofunctional mechanism of methane aromatization, was significantly enhanced, which can be well-rationalized by quantum chemistry calculations. This study narrows the gap between gas-phase and condensed-phase studies on methane conversion and suggests that the monofunctional mechanism probably operates in non-oxidative methane aromatization. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

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

Alkanok, Gizem; Demirel, Burak, E-mail: burak.demirel@boun.edu.tr; Onay, Turgut T.

2014-01-15

Highlights: • Disposal of supermarket wastes in landfills may contribute to environmental pollution. • High methane yields can be obtained from supermarket wastes by anaerobic co-digestion. • Fruit and vegetable wastes or dairy products wastes could individually be handled by a two-stage anaerobic process. • Buffering capacity, trace metal and C/N ratio are essential for digestion of supermarket wastes. - Abstract: Fruit, vegetable, flower waste (FVFW), dairy products waste (DPW), meat waste (MW) and sugar waste (SW) obtained from a supermarket chain were anaerobically digested, in order to recover methane as a source of renewable energy. Batch mesophilic anaerobic reactorsmore » were run at total solids (TS) ratios of 5%, 8% and 10%. The highest methane yield of 0.44 L CH{sub 4}/g VS{sub added} was obtained from anaerobic digestion of wastes (FVFW + DPW + MW + SW) at 10% TS, with 66.4% of methane (CH{sub 4}) composition in biogas. Anaerobic digestion of mixed wastes at 5% and 8% TS provided slightly lower methane yields of 0.41 and 0.40 L CH{sub 4}/g VS{sub added}, respectively. When the wastes were digested alone without co-substrate addition, the highest methane yield of 0.40 L CH{sub 4}/g VS{sub added} was obtained from FVFW at 5% TS. Generally, although the volatile solids (VS) conversion percentages seemed low during the experiments, higher methane yields could be obtained from anaerobic digestion of supermarket wastes. A suitable carbon/nitrogen (C/N) ratio, proper adjustment of the buffering capacity and the addition of essential trace nutrients (such as Ni) could improve VS conversion and biogas production yields significantly.« less

Assessment of Methane Emissions – Impact of Using Natural Gas Engines in Unconventional Resource Development

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

Commercialization of waste gob gas and methane produced in conjunction with coal mining operations. Final report, August 1992--December 1993

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

Not Available

1993-12-01

The primary objectives of the project were to identify and evaluate existing processes for (1) using gas as a feedstock for production of marketable, value-added commodities, and (2) enriching contaminated gas to pipeline quality. The following gas conversion technologies were evaluated: (1) transformation to liquid fuels, (2) manufacture of methanol, (3) synthesis of mixed alcohols, and (4) conversion to ammonia and urea. All of these involved synthesis gas production prior to conversion to the desired end products. Most of the conversion technologies evaluated were found to be mature processes operating at a large scale. A drawback in all of themore » processes was the need to have a relatively pure feedstock, thereby requiring gas clean-up prior to conversion. Despite this requirement, the conversion technologies were preliminarily found to be marginally economic. However, the prohibitively high investment for a combined gas clean-up/conversion facility required that REI refocus the project to investigation of gas enrichment alternatives. Enrichment of a gas stream with only one contaminant is a relatively straightforward process (depending on the contaminant) using available technology. However, gob gas has a unique nature, being typically composed of from constituents. These components are: methane, nitrogen, oxygen, carbon dioxide and water vapor. Each of the four contaminants may be separated from the methane using existing technologies that have varying degrees of complexity and compatibility. However, the operating and cost effectiveness of the combined system is dependent on careful integration of the clean-up processes. REI is pursuing Phase 2 of this project for demonstration of a waste gas enrichment facility using the approach described above. This is expected to result in the validation of the commercial and technical viability of the facility, and the refinement of design parameters.« less

Clay enhancement of methane, low molecular weight hydrocarbon and halocarbon conversion by methanotrophic bacteria

DOEpatents

Apel, William A.; Dugan, Patrick R.

1995-01-01

An apparatus and method for increasing the rate of oxidation of toxic vapors by methanotrophic bacteria. The toxic vapors of interest are methane and trichloroethylene. The apparatus includes a gas phase bioreactor within a closed loop pumping system or a single pass system. The methanotrophic bacteria include Methylomonas methanica, Methylosinus trichosporium, and uncharacterized environmental enrichments.

Clay enhancement of methane, low molecular weight hydrocarbon and halocarbon conversion by methanotrophic bacteria

DOEpatents

Apel, William A.; Dugan, Patrick R.

1995-04-04

An apparatus and method for increasing the rate of oxidation of toxic vapors by methanotrophic bacteria. The toxic vapors of interest are methane and trichloroethylene. The apparatus includes a gas phase bioreactor within a closed loop pumping system or a single pass system. The methanotrophic bacteria include Methylomonas methanica, Methylosinus trichosporium, and uncharacterized environmental enrichments.

Renewable Natural Gas Clean-up Challenges and Applications

DTIC Science & Technology

2011-01-13

produced from digesters ─ Animal manure (dairy cows, swine) ─ Waste water treatment facilities > Methane from Landfills > RNG produced from...AGR used in process • Two stage + trim methanation reactor • Dehydration to achieve gas pipeline specifications ~ 70% conversion efficiency 21... digestion of agricultural waste for on-site electricity generation ─Altamont Landfill—Landfill gas (LFG) cleanup for production of liquefied natural gas

Biogas reforming over multi walled carbon nanotubes with Co-Mo/MgO nanoparticles

NASA Astrophysics Data System (ADS)

Khavarian, Mehrnoush; Mohamed, Abdul Rahman

2017-12-01

The utilization of biogas for the production of valuable chemicals is among the very important processes in the energy research field. The most suitable process for biogas reforming is dry reforming of methane. An obvious drawback is the variable composition of biogas rather than the stoichiometrically equimolar quantities of methane and carbon dioxide. Moreover, activating the methane and carbon dioxide molecules in the reforming reaction provides many challenges in exploring new concepts and opportunities for development of unique catalysts. In the present work, the catalytic activity behavior of Co-Mo-MgO/multi-walled carbon nanotubes (MWCNTs) nanocomposite in dry reforming was investigated with different CO2/CH4 feed ratio to evaluate the performance of this catalyst for biogas reforming reaction. It was found that conversions of methane and carbon dioxide were greatly influenced by the feed gas ratio. The CH4 and CO2 conversions are 83 % and 87 % at the reaction temperature of 825 °C, GHSV of 175 L/h.gcat and CO2/CH4 feed ratio of unity. The minimum carbon deposition rate is observed at the CO2/CH4 feed ratio of 0.6 which is 0.080 gc/gcat-h.

Bio-conversion of water hyacinths into methane gas. Part 1. [Effects of cadmium and nickel pollution

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

Wolverton, B.C.; Mcdonald, R.C.; Gordon, J.

1974-07-01

Bio-gas and methane production from the microbial anaerobic decomposition of water hyacinths (Eichhornia crassipes) (Mart) Solms was investigated. These experiments demonstrated the ability of water hyacinths to produce an average of 13.9 ml of methane gas per gram of wet plant weight. This study revealed that sample preparation had no significant effect on bio-gas and/or methane production. Pollution of water hyacinths by two toxic heavy materials, nickel and cadmium, increased the rate of methane production from 51.8 ml/day for non-contaminated plants incubated at 36 C to 81.0 ml/day for Ni-Cd contaminated plants incubated at the same temperature. The methane contentmore » of bio-gas evolved from the anaerobic decomposition of Ni-Cd contaminated plants was 91.1 percent as compared to 69.2 percent methane content of bio-gas collected from the fermentation of non-contaminated plants. (Author) (GRA)« less

Wood biodegradation in laboratory-scale landfills.

PubMed

Wang, Xiaoming; Padgett, Jennifer M; De la Cruz, Florentino B; Barlaz, Morton A

2011-08-15

The objective of this research was to characterize the anaerobic biodegradability of major wood products in municipal waste by measuring methane yields, decay rates, the extent of carbohydrate decomposition, carbon storage, and leachate toxicity. Tests were conducted in triplicate 8 L reactors operated to obtain maximum yields. Measured methane yields for red oak, eucalyptus, spruce, radiata pine, plywood (PW), oriented strand board (OSB) from hardwood (HW) and softwood (SW), particleboard (PB) and medium-density fiberboard (MDF) were 32.5, 0, 7.5, 0.5, 6.3, 84.5, 0, 5.6, and 4.6 mL CH(4) dry g(-1), respectively. The red oak, a HW, exhibited greater decomposition than either SW (spruce and radiata), a trend that was also measured for the OSB-HW relative to OSB-SW. However, the eucalyptus (HW) exhibited toxicity. Thus, wood species have unique methane yields that should be considered in the development of national inventories of methane production and carbon storage. The current assumption of uniform biodegradability is not appropriate. The ammonia release from urea formaldehyde as present in PB and MDF could contribute to ammonia in landfill leachate. Using the extent of carbon conversion measured in this research, 0-19.9%, predicted methane production from a wood mixture using the Intergovernmental Panel for Climate Change waste model is only 7.9% of that predicted using the 50% carbon conversion default.

Fiber Laser methane sensor with the function of self-diagnose

NASA Astrophysics Data System (ADS)

Li, Yan-fang; Wei, Yu-bin; Shang, Ying; Wang, Chang; Liu, Tong-yu

2012-02-01

Using the technology of tunable diode laser absorption spectroscopy and the technology of micro-electronics, a fiber laser methane sensor based on the microprocessor C8051F410 is given. In this paper, we use the DFB Laser as the light source of the sensor. By tuning temperature and driver current of the DFB laser, we can scan the laser over the methane absorption line, Based on the Beer-Lambert law, through detect the variation of the light power before and after the absorption we realize the methane detection. It makes the real-time and online detection of methane concentration to be true, and it has the advantages just as high accuracy, immunity to other gases , long calibration cycle and so on. The sensor has the function of adaptive gain and self-diagnose. By introducing digital potentiometers, the gain of the photoelectric conversion operational amplifier can be controlled by the microprocessor according to the light power. When the gain and the conversion voltage achieve the set value, then we can consider the sensor in a fault status, and then the software will alarm us to check the status of the probe. So we improved the dependence and the stability of the measured results. At last we give some analysis on the sensor according the field application and according the present working, we have a look of our next work in the distance.

Biomethanation of Syngas Using Anaerobic Sludge: Shift in the Catabolic Routes with the CO Partial Pressure Increase.

PubMed

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.

Biomethanation of Syngas Using Anaerobic Sludge: Shift in the Catabolic Routes with the CO Partial Pressure Increase

PubMed Central

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

Direct Internal Reformation and Mass Transport in the Solid Oxide Fuel Cell Anode: A Pore-Scale Lattice Boltzmann Study with Detailed Reaction Kinetics

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

Grew, Kyle N.; Joshi, Abhijit S.; Chiu, W. K. S.

2010-11-30

The solid oxide fuel cell (SOFC) allows the conversion of chemical energy that is stored in a given fuel, including light hydrocarbons, to electrical power. Hydrocarbon fuels, such as methane, are logistically favourable and provide high energy densities. However, the use of these fuels often results in a decreased efficiency and life. An improved understanding of the reactive flow in the SOFC anode can help address these issues. In this study, the transport and heterogeneous internal reformation of a methane based fuel is addressed. The effect of the SOFC anode's complex structure on transport and reactions is shown to exhibitmore » a complicated interplay between the local molar concentrations and the anode structure. Strong coupling between the phenomenological microstructures and local reformation reaction rates are recognised in this study, suggesting the extension to actual microstructures may provide new insights into the reformation processes.« less

Photoenhanced anaerobic digestion of organic acids

DOEpatents

Weaver, Paul F.

1990-01-01

A process is described for rapid conversion of organic acids and alcohols anaerobic digesters into hydrogen and carbon dioxide, the optimal precursor substrates for production of methane. The process includes addition of photosynthetic bacteria to the digester and exposure of the bacteria to radiant energy (e.g., solar energy). The process also increases the pH stability of the digester to prevent failure of the digester. Preferred substrates for photosynthetic bacteria are the organic acid and alcohol waste products of fermentative bacteria. In mixed culture with methanogenic bacteria or in defined co-culture with non-aceticlastic methanogenic bacteria, photosynthetic bacteria are capable of facilitating the conversion or organic acids and alcohols into methane with low levels of light energy input.

Ethane's 12C/13C Ratio in Titan: Implications for Methane Replenishment

NASA Technical Reports Server (NTRS)

Jennings, Donald E.; Nixon, C. A.; Romani, P. N.; Bjoraker, G. L.; Sada, P. V.; Lunsford, A. W.; Boyle, R. J.; Hesman, B. E.; McCabe, G. H.

2009-01-01

As the .main destination of carbon in the destruction of methane in the atmosphere of Titan, ethane provides information about the carbon isotopic composition of the reservoir from which methane is replenished. If the amount of methane entering the atmosphere is presently equal to the amount converted to ethane, the 12C/13C ratio in ethane should be close to the ratio in the reservoir. We have measured the 12C/13C ratio in ethane both with Cassini CIRS(exp 1) and from the ground and find that it is very close to the telluric standard and outer planet values (89), consistent with a primordial origin for the methane reservoir. The lower 12C/13C ratio measured for methane by Huygens GCMS (82.3) can be explained if the conversion of CH4 to CH3 (and C2H6) favors 12C over 13C with a carbon kinetic isotope effect of 1.08. The time required for the atmospheric methane to reach equilibrium, i.e., for replenishment to equal destruction, is approximately 5 methane atmospheric lifetimes.

Minimizing the formation of coke and methane on Co nanoparticles in steam reforming of biomass-derived oxygenates

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

Sun, Junming; Mei, Donghai; Karim, Ayman M.

2013-06-01

Fundamental understanding and control of chemical transformations are essential to the development of technically feasible and economically viable catalytic processes for efficient conversion of biomass to fuels and chemicals. Using an integrated experimental and theoretical approach, we report high hydrogen selectivity and catalyst durability of acetone steam reforming (ASR) on inert carbon supported Co nanoparticles. The observed catalytic performance is further elucidated on the basis of comprehensive first-principles calculations. Instead of being considered as an undesired intermediate prone for catalyst deactivation during bioethanol steam reforming (ESR), acetone is suggested as a key and desired intermediate in proposed two-stage ESR processmore » that leads to high hydrogen selectivity and low methane formation on Co-based catalysts. The significance of the present work also sheds a light on controlling the chemical transformations of key intermediates in biomass conversion such as ketones. We gratefully acknowledge the financial support from U. S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences, and the Laboratory directed research and development (LDRD) project of Pacific Northwest National Laboratory (PNNL). Computing time was granted by the William R. Wiley Environmental Molecular Sciences Laboratory (EMSL). The EMSL is a U.S. DOE national scientific user facility located at PNNL, and sponsored by the U.S. DOE’s Office of Biological and Environmental Research.« less

Animal health and greenhouse gas intensity: the paradox of periparturient parasitism.

PubMed

Houdijk, J G M; Tolkamp, B J; Rooke, J A; Hutchings, M R

2017-09-01

Here we provide the first known direct measurements of pathogen challenge impacts on greenhouse gas production, yield and intensity. Twin-rearing ewes were ad libitum fed pelleted lucerne from day -32 to 36 (day 0 is parturition), and repeatedly infected with 10,000 Teladorsagia circumcincta infective larvae (n=16), or sham-dosed with water (n=16). A third group of 16 ewes were fed at 80% of uninfected ewes' feed intake during lactation. Methane emissions were measured in respiration chambers (day 30-36) whilst total tract apparent nutrient digestibility around day 28 informed calculated manure methane and nitrous oxide emissions estimates. Periparturient parasitism reduced feed intake (-9%) and litter weight gain (-7%) and doubled maternal body weight loss. Parasitism reduced daily enteric methane production by 10%, did not affect the methane yield per unit of dry matter intake but increased the yield per unit of digestible organic matter intake by 14%. Parasitism did not affect the daily calculated manure methane and nitrous oxide production, but increased the manure methane and nitrous oxide yields per unit of dry matter intake by 16% and 4%, respectively, and per unit of digestible organic matter intake by 46% and 31%, respectively. Accounting for increased lucerne input for delayed weaning and maternal body weight loss compensation, parasitism increased the calculated greenhouse gas intensity per kg of lamb weight gain for enteric methane (+11%), manure methane (+32%) and nitrous oxide (+30%). Supplemented with the global warming potential associated with production of pelleted lucerne, we demonstrated that parasitism increased calculated global warming potential per kg of lamb weight gain by 16%, which was similar to the measured impact of parasitism on the feed conversion ratio. Thus, arising from a pathogen-induced feed efficiency reduction and modified greenhouse gas emissions, we demonstrated that ovine periparturient parasitism increases greenhouse gas intensity. This implies that ewe worm control can not only improve production efficiency but also reduce the environmental footprint of sheep production systems. Copyright © 2017 Australian Society for Parasitology. Published by Elsevier Ltd. All rights reserved.

Effects of sonication on co-precipitation synthesis and activity of copper manganese oxide catalyst to remove methane and sulphur dioxide gases.

PubMed

Yap, Yeow Hong; Lim, Mitchell S W; Lee, Zheng Yee; Lai, Kar Chiew; Jamaal, Muhamad Ashraf; Wong, Farng Hui; Ng, Hoon Kiat; Lim, Siew Shee; Tiong, T Joyce

2018-01-01

The utilisation of ultrasound in chemical preparation has been the focus of intense study in various fields, including materials science and engineering. This paper presents a novel method of synthesising the copper-manganese oxide (Hopcalite) catalyst that is used for the removal of volatile organic compounds and greenhouse gases like carbon monoxide. Several samples prepared under different conditions, with and without ultrasound, were subjected to a series of characterisation tests such as XRD, BET, FE-SEM, EDX, TPR-H 2 , TGA and FT-IR in order to establish their chemical and physical properties. A series of catalytic tests using a micro-reactor were subsequently performed on the samples in order to substantiate the aforementioned properties by analysing their ability to oxidise compressed natural gas (CNG), containing methane and sulphur dioxide. Results showed that ultrasonic irradiation of the catalyst led to observable alterations in its morphology: surfaces of the particles were noticeably smoothed and an increased in amorphicity was detected. Furthermore, ultrasonic irradiation has shown to enhance the catalytic activity of Hopcalite, achieving a higher conversion of methane relative to non-sonicated samples. Varying the ultrasonic intensity also produced appreciable effects, whereby an increase in intensity results in a higher conversion rate. The catalyst sonicated at the highest intensity of 29.7W/cm 2 has a methane conversion rate of 13.5% at 400°C, which was the highest among all the samples tested. Copyright © 2017 Elsevier B.V. All rights reserved.

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.

Microbial Ecology of Thermophilic Anaerobic Digestion. Final Report

DOE R&D Accomplishments Database

Zinder, Stephen H.

2000-04-15

This grant supported research on methanogenic archaea. The two major areas that were supported were conversion of acetic acid to methane and nitrogen fixation by Methanosarcina. Among the achievements of this research were the isolation of novel methanogenic cultures, elucidation of the pathways from acetate to methane, description of a specific DNA-binding complex in nitrogen fixing methanogens, and demonstration of an alternative nitrogenase in Methanosarcina.

Microwave Hydrogen Production from Methane

DTIC Science & Technology

2012-04-01

combustion NOx control of reciprocating engine exhaust and fuel cell application of biogas . Our target is to obtain the methane conversion efficiency...demonstration of MW technology removing and destroying hydrogen sulfide (H2S) and siloxanes from biogas produced by Sacramento Regional Wastewater...running on biogas and is currently conducting the field demonstration of the unit at Tollenaar Dairy in Elk Grove, CA. SMUD, California Air Resources

Anaerobic digestion of palm oil mill effluent (POME) using bio-methane potential (BMP) test

NASA Astrophysics Data System (ADS)

Aziz, Nur Izzah Hamna A.; Hanafiah, Marlia M.

2018-04-01

Biogas is a promising sustainable and renewable energy alternative to reduce the dependence on fossil fuel. In Malaysia, the conversion of palm oil mill effluent (POME) to bioenergy has recently been expanded due to its high potential in generating energy. However, without a proper treatment and management, POME could be harmful to environment because it emits greenhouse gas emissions into the atmosphere and could also pollutes the watercourses if discharge directly due to the high acidity and chemical oxygen demand (COD) content. Many initiatives have been taken by the government towards sustainable development. Therefore, more efforts need to be practiced to improve and upscale the technology for a better waste management. In this study, the anaerobic digestion of POME was carried out using Bio-methane potential (BMP) test in batch and laboratory scales. Physicochemical characteristics and the biogas production of POME were measured. The BMP test under mesophilic condition was conducted for 23 consecutive days to measure the biogas production. The POME produced 721.3 cm3 of biogas by using anaerobic sludge as inoculum. The results also found that the methane (CH4) and carbon dioxide (CO2) gases produced with 360.65 cm3 and 288.52 cm3, respectively.

Annual methane and nitrous oxide emissions from rice paddies and inland fish aquaculture wetlands in southeast China

NASA Astrophysics Data System (ADS)

Wu, Shuang; Hu, Zhiqiang; Hu, Tao; Chen, Jie; Yu, Kai; Zou, Jianwen; Liu, Shuwei

2018-02-01

Inland aquaculture ponds have been documented as important sources of atmospheric methane (CH4) and nitrous oxide (N2O), while their regional or global source strength remains unclear due to lack of direct flux measurements by covering more typical habitat-specific aquaculture environments. In this study, we compared the CH4 and N2O fluxes from rice paddies and nearby inland fish aquaculture wetlands that were converted from rice paddies in southeast China. Both CH4 and N2O fluxes were positively related to water temperature and sediment dissolved organic carbon, but negatively related to water dissolved oxygen concentration. More robust response of N2O fluxes to water mineral N was observed than to sediment mineral N. Annual CH4 and N2O fluxes from inland fish aquaculture averaged 0.51 mg m-2 h-1 and 54.78 μg m-2 h-1, amounting to 42.31 kg CH4 ha-1 and 2.99 kg N2O-N ha-1, respectively. The conversion of rice paddies to conventional fish aquaculture significantly reduced CH4 and N2O emissions by 23% and 66%, respectively. The emission factor for N2O was estimated to be 0.46% of total N input in the feed or 1.23 g N2O-N kg-1 aquaculture production. The estimate of sustained-flux global warming potential of annual CH4 and N2O emissions and the net economic profit suggested that such conversion of rice paddies to inland fish aquaculture would help to reconcile the dilemma for simultaneously achieving both low climatic impacts and high economic benefits in China. More solid direct field measurements from inland aquaculture are in urgent need to direct the overall budget of national or global CH4 and N2O fluxes.

7 CFR 1940.311 - Environmental assessments for Class I actions.

Code of Federal Regulations, 2013 CFR

2013-01-01

... designed for on-farm needs such as methane digestors and fuel alcohol production facilities; (5) Financial assistance for the conversion of more than 160 acres of pasture to agricultural production, but no more than 320 acres, provided that in a conversion to agricultural production no wetlands are affected, in which...

7 CFR 1940.311 - Environmental assessments for Class I actions.

Code of Federal Regulations, 2014 CFR

2014-01-01

... designed for on-farm needs such as methane digestors and fuel alcohol production facilities; (5) Financial assistance for the conversion of more than 160 acres of pasture to agricultural production, but no more than 320 acres, provided that in a conversion to agricultural production no wetlands are affected, in which...

7 CFR 1940.311 - Environmental assessments for Class I actions.

Code of Federal Regulations, 2012 CFR

2012-01-01

... designed for on-farm needs such as methane digestors and fuel alcohol production facilities; (5) Financial assistance for the conversion of more than 160 acres of pasture to agricultural production, but no more than 320 acres, provided that in a conversion to agricultural production no wetlands are affected, in which...

7 CFR 1940.311 - Environmental assessments for Class I actions.

Code of Federal Regulations, 2011 CFR

2011-01-01

... designed for on-farm needs such as methane digestors and fuel alcohol production facilities; (5) Financial assistance for the conversion of more than 160 acres of pasture to agricultural production, but no more than 320 acres, provided that in a conversion to agricultural production no wetlands are affected, in which...

Effects of Nickel and Cobalt on Kinetics of Methanol Conversion by Methanogenic Sludge as Assessed by On-Line CH4 Monitoring

PubMed Central

Gonzalez-Gil, Graciela; Kleerebezem, Robbert; Lettinga, Gatze

1999-01-01

When metals were added in a pulse mode to methylotrophic-methanogenic biomass, three methane production rate phases were recognized. Increased concentrations of Ni and Co accelerated the initial exponential and final arithmetic increases in the methane production rate and reduced the temporary decrease in the rate. When Ni and Co were added continuously, the temporary decrease phase was eliminated and the exponential production rate increased. We hypothesize that the temporary decrease in the methane production rate and the final arithmetic increase in the methane production rate were due to micronutrient limitations and that the precipitation-dissolution kinetics of metal sulfides may play a key role in the biovailability of these compounds. PMID:10103284

Effects of nickel and cobalt on kinetics of methanol conversion by methanogenic sludge as assessed by on-line CH4 monitoring.

PubMed

Gonzalez-Gil, G; Kleerebezem, R; Lettinga, G

1999-04-01

When metals were added in a pulse mode to methylotrophic-methanogenic biomass, three methane production rate phases were recognized. Increased concentrations of Ni and Co accelerated the initial exponential and final arithmetic increases in the methane production rate and reduced the temporary decrease in the rate. When Ni and Co were added continuously, the temporary decrease phase was eliminated and the exponential production rate increased. We hypothesize that the temporary decrease in the methane production rate and the final arithmetic increase in the methane production rate were due to micronutrient limitations and that the precipitation-dissolution kinetics of metal sulfides may play a key role in the biovailability of these compounds.

Fuelling the future: microbial engineering for the production of sustainable biofuels.

PubMed

Liao, James C; Mi, Luo; Pontrelli, Sammy; Luo, Shanshan

2016-04-01

Global climate change linked to the accumulation of greenhouse gases has caused concerns regarding the use of fossil fuels as the major energy source. To mitigate climate change while keeping energy supply sustainable, one solution is to rely on the ability of microorganisms to use renewable resources for biofuel synthesis. In this Review, we discuss how microorganisms can be explored for the production of next-generation biofuels, based on the ability of bacteria and fungi to use lignocellulose; through direct CO2 conversion by microalgae; using lithoautotrophs driven by solar electricity; or through the capacity of microorganisms to use methane generated from landfill. Furthermore, we discuss how to direct these substrates to the biosynthetic pathways of various fuel compounds and how to optimize biofuel production by engineering fuel pathways and central metabolism.

Temperature regulates methane production through the function centralization of microbial community in anaerobic digestion.

PubMed

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.

Comparison of methane production potential, biodegradability, and kinetics of different organic substrates.

PubMed

Li, Yeqing; Zhang, Ruihong; Liu, Guangqing; Chen, Chang; He, Yanfeng; Liu, Xiaoying

2013-12-01

The methane production potential, biodegradability, and kinetics of a wide range of organic substrates were determined using a unified and simple method. Results showed that feedstocks that contained high energy density and easily degradable substrates exhibited high methane production potential and biodegradability. Lignocellulosic biomass with high content of fibrous compositions had low methane yield and biodegradability. Feedstocks with high lignin content (≥ 15%, on a TS basis) had low first-order rate constant (0.05-0.06 1/d) compared to others. A negative linear correlation between lignin content and experimental methane yield (or biodegradability) was found for lignocellulosic and manure wastes. This could be used as a fast method to predict the methane production potential and biodegradability of fiber-rich substrates. The findings of this study provided a database for the conversion efficiency of different organic substrates and might be useful for applications of biomethane potential assay and anaerobic digestion in the future. Copyright © 2013 Elsevier Ltd. All rights reserved.

Template-Assisted Wet-Combustion Synthesis of Fibrous Nickel-Based Catalyst for Carbon Dioxide Methanation and Methane Steam Reforming.

PubMed

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.

Influence of operating pressure on the biological hydrogen methanation in trickle-bed reactors.

PubMed

Ullrich, Timo; Lindner, Jonas; Bär, Katharina; Mörs, Friedemann; Graf, Frank; Lemmer, Andreas

2018-01-01

In order to investigate the influence of pressures up to 9bar absolute on the productivity of trickle-bed reactors for biological methanation of hydrogen and carbon dioxide, experiments were carried out in a continuously operated experimental plant with three identical reactors. The pressure increase promises a longer residence time and improved mass transfer of H 2 due to higher gas partial pressures. The study covers effects of different pressures on important parameters like gas hourly space velocity, methane formation rate, conversion rates and product gas quality. The methane content of 64.13±3.81vol-% at 1.5bar could be increased up to 86.51±0.49vol-% by raising the pressure to 9bar. Methane formation rates of up to 4.28±0.26m 3 m -3 d -1 were achieved. Thus, pressure increase could significantly improve reactor performance. Copyright © 2017 Elsevier Ltd. All rights reserved.

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

PubMed

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.

2015-16 ENSO Drove Tropical Soil Moisture Dynamics and Methane Fluxes

NASA Astrophysics Data System (ADS)

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

2017-12-01

The El Niño/Southern Oscillation Event (ENSO) cycle drives large-scale climatic trends globally. Within the new world tropics, El Niño brings dryer weather than the counterpart La Niña. Atmospheric methane growth rates have shown extreme variability over the past three decades. One proposed driver is the proportion of tropical land surface saturated, affecting methane production or consumption. We measured methane flux bimonthly through the transition of 2015-16 ENSO. The date of measurement, across El Niño and La Niña within the typical "rainy" and "dry" seasons, to be the most significant driver of methane flux. Soil moisture varied across this time period, and regulated methane flux. During the strong El Niño, extreme dry soil conditions occurred in a typical "rainy" season month reducing soil moisture. Wetter than usual soil conditions appeared during the "rainy" season month of the moderate La Niña. The dry El Niño soils corresponded to greater methane consumption by tropical forest soils, and a reduced local atmospheric column methane concentration. Conversely, the wet La Niña soils had lower methane consumption and higher local atmospheric column methane concentrations. The ENSO cycle is a strong driver of tropical terrestrial and wetland soil moisture conditions, and can regulate global atmospheric methane dynamics.

In-Situ Quantification of Microbial Processes Controlling Methane Emissions From Rice Plants

NASA Astrophysics Data System (ADS)

Schroth, M. H.; Cho, R.; Zeyer, J. A.

2011-12-01

Methane is an important greenhouse gas contributing to global warming. Among other sources, rice (paddy) soils represent a major nonpoint source of biogenic methane. In flooded paddy soils methane is produced under anaerobic conditions. Conversely, methanotrophic microorganisms oxidize methane to carbon dioxide in the root zone of rice plants, thus reducing overall methane emissions to the atmosphere. We present a novel combination of methods to quantify methanogenesis and methane oxidation in paddy soils and to link methane turnover to net emissions of rice plants. To quantify methane turnover in the presence of high methane background concentrations, small-scale push-pull tests (PPTs) were conducted in paddy soils using stable isotope-labeled substrates. Deuterated acetate and 13-C bicarbonate were employed to discern and quantify acetoclastic and hydrogenotrophic methanogenesis, while 13-C methane was employed to quantify methane oxidation. During 2.5 hr-long PPTs, 140 mL of a test solution containing labeled substrates and nonreactive tracers (Ar, Br-) was injected into paddy soils of potted rice plants. After a short rest period, 480 mL of test solution/pore water mixture was extracted from the same location. Methane turnover was then computed from extraction-phase breakthrough curves of substrates and/or products, and nonreactive tracers. To link methane turnover to net emissions, methane emissions from paddy soils and rice plants were individually determined immediately preceding PPTs using static flux chambers. We will present results of a series of experiments conducted in four different potted rice plants. Preliminary results indicate substantial variability in methane turnover and net emission between different rice plants. The employed combination of methods appears to provide a robust means to quantitatively link methane turnover in paddy soils to net emissions from rice plants.

Methane drainage with horizontal boreholes in advance of longwall mining: an analysis. Final report

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

Gabello, D.P.; Felts, L.L.; Hayoz, F.P.

1981-05-01

The US Department of Energy (DOE) Morgantown Energy Technology Center has implemented a comprehensive program to demonstrate the technical and economic viability of coalbed methane as an energy resource. The program is directed toward solution of technical and institutional problems impeding the recovery and use of large quantities of methane contained in the nation's minable and unminable coalbeds. Conducted in direct support of the DOE Methane Recovery from Coalbeds Project, this study analyzes the economic aspects of a horizontal borehole methane recovery system integrated as part of a longwall mine operation. It establishes relationships between methane selling price and annualmore » mine production, methane production rate, and the methane drainage system capital investment. Results are encouraging, indicating that an annual coal production increase of approximately eight percent would offset all associated drainage costs over the range of methane production rates and capital investments considered.« less

Titan's surface-atmosphere system before and after Huygens

NASA Astrophysics Data System (ADS)

Lunine, Jonathan I.

2015-04-01

Speculation about the nature of Titan's surface-atmosphere interactions goes back to the discovery of methane in its atmosphere in 1943 but beginning in the early 1970's surface models began to grapple more quantitatively with the source of methane and its instability in the atmosphere. The role of molecular nitrogen in the atmosphere was first quantitatively considered at that time as well. The Voyager 1 flyby put a thick atmosphere of molecular nitrogen and methane on an observational footing, and made an atmospheric descent probe quite feasible. The measured high methane humidity made seas of methane and possibly other constituents an attractive possible source of methane and sink of its photolytic products, influencing the choice of instruments for a descent probe. At the time of Huygens' actual descent to the surface, global seas had been ruled out, and the Cassini Orbiter was just beginning to gather imaging and radar data of the surface. The fluvial nature of the Huygens landing site and presence of volatiles just below the surface were important discoveries of Huygens itself. Together with Cassini, Huygens painted a picture of a cryogenic desert with occasional violent methane rainstorms feeding streams that tumble pebbles of ice and organics downhill, the whole surrounded by dunes whose organic-rich particles are harvested from the chemical conversion of methane to more refractory compounds high in the atmosphere. And yet many mysteries remain. The large bodies of liquid methane are restricted to high latitudes. Most of the river valleys seen in Cassini radar data seem to run down to nowhere. And the ultimate source and replenishment of methane, although seemingly more strongly tied to the interior than before Cassini-Huygens, remain unresolved. Huygens gave us the only imaging of Titan's surface with a resolution good enough to follow fluvial processes all the way from the contextual geology, to channels, to the stream debris washed out into the plains. What would we see if we could image even just 10% of Titan at Huygens resolution? Conversely, what might we have concluded about Titan were only the Cassini Orbiter data available, without Huygens? It is clear that Huygens gave us one tantalizing look through the keyhole at a mysterious room, but to truly understand what was glimpsed will require a future mission to open wide the door.

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

PubMed

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

2015-01-06

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

Development of eye-safe lidar for aerosol measurements

NASA Technical Reports Server (NTRS)

Singh, Upendra N.; Wilderson, Thomas D.

1990-01-01

Research is summarized on the development of an eye safe Raman conversion system to carry out lidar measurements of aerosol and clouds from an airborne platform. Radiation is produced at the first Stokes wavelength of 1.54 micron in the eye safe infrared, when methane is used as the Raman-active medium, the pump source being a Nd:YAG laser at 1.064 micron. Results are presented for an experimental study of the dependence of the 1.54 micron first Stokes radiation on the focusing geometry, methane gas pressure, and pump energy. The specific new technique developed for optimizing the first Stokes generation involves retroreflecting the backward-generated first Stokes light back into the Raman cell as a seed Stokes beam which is then amplified in the temporal tail of the pump beam. Almost 20 percent conversion to 1.54 micron is obtained. Complete, assembled hardware for the Raman conversion system was delivered to the Goddard Space Flight Center for a successful GLOBE flight (1989) to measure aerosol backscatter around the Pacific basin.

High-strength fermentable wastewater reclamation through a sequential process of anaerobic fermentation followed by microalgae cultivation.

PubMed

Qi, Wenqiang; Chen, Taojing; Wang, Liang; Wu, Minghong; Zhao, Quanyu; Wei, Wei

2017-03-01

In this study, the sequential process of anaerobic fermentation followed by microalgae cultivation was evaluated from both nutrient and energy recovery standpoints. The effects of different fermentation type on the biogas generation, broth metabolites' composition, algal growth and nutrients' utilization, and energy conversion efficiencies for the whole processes were discussed. When the fermentation was designed to produce hydrogen-dominating biogas, the total energy conversion efficiency (TECE) of the sequential process was higher than that of the methane fermentation one. With the production of hydrogen in anaerobic fermentation, more organic carbon metabolites were left in the broth to support better algal growth with more efficient incorporation of ammonia nitrogen. By applying the sequential process, the heat value conversion efficiency (HVCE) for the wastewater could reach 41.2%, if methane was avoided in the fermentation biogas. The removal efficiencies of organic metabolites and NH 4 + -N in the better case were 100% and 98.3%, respectively. Copyright © 2016 Elsevier Ltd. All rights reserved.

Tri-reforming and combined reforming of methane for producing syngas with desired hydrogen/carbon monoxide ratios

NASA Astrophysics Data System (ADS)

Pan, Wei

This dissertation is an exploratory study of a new process concept for direct production of synthesis gas (CO + H2) with desired H 2/CO ratios (1.5--2.0) for methanol synthesis and F-T synthesis, using CO2 together with steam and unconverted O2 in flue gas from fossil fuel-fired electric power plants to react with methane or natural gas. This new process is called tri-reforming, referring to simultaneous CO2-steam-O2 reforming of methane or natural gas. This study included (1) The investigation of carbon formation in the tri-reforming process. For comparison, carbon formation in the combined reforming and CO2 reforming reaction was studied as well. (2) The effect of reaction conditions and feed compositions on equilibrium composition (e.g. H2/CO ratio) and equilibrium conversions in the tri-reforming process. (3) The role of catalysts in the tri-reforming process, especially the effect of catalysts on CO2 conversion in the presence of H 2O and O2. It was clearly evidenced from this study that CO in the product stream is probably the major source of carbon over Ni/Al2O3 in the equimolar CO2-CH4 reforming at 650°C and 1 atm. Addition of either O2 or H2O into the CO 2 reforming reaction system can suppress carbon formation. It was demonstrated that carbon-free operation can be achieved in the tri-reforming process. A thermodynamic comparison of tri-reforming with feed compositions of (H2O+CO2+0.5O2)/CH4 (mol ratio) = 1 showed that O2 improves equilibrium CH4 conversion, yet greatly decreases equilibrium CO2 conversion. H2O in tri-reforming has a significant effect on the H2/CO ratio in the products, while O2 has a minor effect. A kinetic study and catalytic performance tests indicated that the support in a supported catalyst has a significant role in enhancing CO2 conversion to CO in the presence of H2O and O2 in tri-reforming. The Ni/MgO catalyst showed superior performance with close to equilibrium CH4 and CO2 conversions at 850°C, 1 atm, and 32,000 ml/(h.gcat.). The apparent Activation energy for CH4 conversion over Ni/MgO was estimated to be 219 kJ/mol, which is higher than over Ni/Al2O 3 (69.1 kJ/mol) and Ni/MgO/CeZrO (67.4 kJ/mol). This may be attributed to less CH4 activation over Ni/MgO or to an experimental artifact caused by catalyst deactivation as reaction temperature decreases from 850°C to 750°C. With the decrease of temperature, Ni may be re-oxidized and form NiO-MgO solid solution in the presence of H2O, CO2, or O2. (Abstract shortened by UMI.)

Bioconversion of methane to lactate by an obligate methanotrophic bacterium

DOE PAGES

Henard, Calvin A.; Smith, Holly; Dowe, Nancy; ...

2016-02-23

Methane is the second most abundant greenhouse gas (GHG), with nearly 60% of emissions derived from anthropogenic sources. Microbial conversion of methane to fuels and value-added chemicals offers a means to reduce GHG emissions, while also valorizing this otherwise squandered high-volume, high-energy gas. However, to date, advances in methane biocatalysis have been constrained by the low-productivity and limited genetic tractability of natural methane-consuming microbes. Here, leveraging recent identification of a novel, tractable methanotrophic bacterium, Methylomicrobium buryatense, we demonstrate microbial biocatalysis of methane to lactate, an industrial platform chemical. Heterologous overexpression of a Lactobacillus helveticus L-lactate dehydrogenase in M. buryatense resultedmore » in an initial titer of 0.06 g lactate/L from methane. Cultivation in a 5 L continuously stirred tank bioreactor enabled production of 0.8 g lactate/L, representing a 13-fold improvement compared to the initial titer. The yields (0.05 g lactate/g methane) and productivity (0.008 g lactate/L/h) indicate the need and opportunity for future strain improvement. Additionally, real-time analysis of methane utilization implicated gas-to-liquid transfer and/or microbial methane consumption as process limitations. This work opens the door to develop an array of methanotrophic bacterial strain-engineering strategies currently employed for biocatalytic sugar upgrading to “green” chemicals and fuels.« less

Bioconversion of methane to lactate by an obligate methanotrophic bacterium

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

Henard, Calvin A.; Smith, Holly; Dowe, Nancy

Methane is the second most abundant greenhouse gas (GHG), with nearly 60% of emissions derived from anthropogenic sources. Microbial conversion of methane to fuels and value-added chemicals offers a means to reduce GHG emissions, while also valorizing this otherwise squandered high-volume, high-energy gas. However, to date, advances in methane biocatalysis have been constrained by the low-productivity and limited genetic tractability of natural methane-consuming microbes. Here, leveraging recent identification of a novel, tractable methanotrophic bacterium, Methylomicrobium buryatense, we demonstrate microbial biocatalysis of methane to lactate, an industrial platform chemical. Heterologous overexpression of a Lactobacillus helveticus L-lactate dehydrogenase in M. buryatense resultedmore » in an initial titer of 0.06 g lactate/L from methane. Cultivation in a 5 L continuously stirred tank bioreactor enabled production of 0.8 g lactate/L, representing a 13-fold improvement compared to the initial titer. The yields (0.05 g lactate/g methane) and productivity (0.008 g lactate/L/h) indicate the need and opportunity for future strain improvement. Additionally, real-time analysis of methane utilization implicated gas-to-liquid transfer and/or microbial methane consumption as process limitations. This work opens the door to develop an array of methanotrophic bacterial strain-engineering strategies currently employed for biocatalytic sugar upgrading to “green” chemicals and fuels.« less

Bioconversion of methane to lactate by an obligate methanotrophic bacterium

PubMed Central

Henard, Calvin A.; Smith, Holly; Dowe, Nancy; Kalyuzhnaya, Marina G.; Pienkos, Philip T.; Guarnieri, Michael T.

2016-01-01

Methane is the second most abundant greenhouse gas (GHG), with nearly 60% of emissions derived from anthropogenic sources. Microbial conversion of methane to fuels and value-added chemicals offers a means to reduce GHG emissions, while also valorizing this otherwise squandered high-volume, high-energy gas. However, to date, advances in methane biocatalysis have been constrained by the low-productivity and limited genetic tractability of natural methane-consuming microbes. Here, leveraging recent identification of a novel, tractable methanotrophic bacterium, Methylomicrobium buryatense, we demonstrate microbial biocatalysis of methane to lactate, an industrial platform chemical. Heterologous overexpression of a Lactobacillus helveticus L-lactate dehydrogenase in M. buryatense resulted in an initial titer of 0.06 g lactate/L from methane. Cultivation in a 5 L continuously stirred tank bioreactor enabled production of 0.8 g lactate/L, representing a 13-fold improvement compared to the initial titer. The yields (0.05 g lactate/g methane) and productivity (0.008 g lactate/L/h) indicate the need and opportunity for future strain improvement. Additionally, real-time analysis of methane utilization implicated gas-to-liquid transfer and/or microbial methane consumption as process limitations. This work opens the door to develop an array of methanotrophic bacterial strain-engineering strategies currently employed for biocatalytic sugar upgrading to “green” chemicals and fuels. PMID:26902345

Fractionation of carbon and hydrogen isotopes by methane-oxidizing bacteria

USGS Publications Warehouse

Coleman, D.D.; Risatti, J.B.; Schoell, M.

1981-01-01

Carbon isotopic analysis of methane has become a popular technique in the exploration for oil and gas because it can be used to differentiate between thermogenic and microbial gas and can sometimes be used for gas-source rock correlations. Methane-oxidizing bacteria, however, can significantly change the carbon isotopic composition of methane; the origin of gas that has been partially oxidized by these bacteria could therefore be misinterpreted. We cultured methane-oxidizing bacteria at two different temperatures and monitored the carbon and hydrogen isotopic compositions of the residual methane. The residual methane was enriched in both 13C and D. For both isotopic species, the enrichment at equivalent levels of conversion was greater at 26??C than at 11.5??C. The change in ??D relative to the change in ??13C was independent of temperature within the range studied. One culture exhibited a change in the fractionation pattern for carbon (but not for hydrogen) midway through the experiment, suggesting that bacterial oxidation of methane may occur via more than one pathway. The change in the ??D value for the residual methane was from 8 to 14 times greater than the change in the ??13C value, indicating that combined carbon and hydrogen isotopic analysis may be an effective way of identifying methane which has been subjected to partial oxidation by bacteria. ?? 1981.

Conversion of a wet waste feedstock to biocrude by hydrothermal processing in a continuous-flow reactor: grape pomace

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

Elliott, Douglas C.; Schmidt, Andrew J.; Hart, Todd R.

Wet waste feedstocks present an apt opportunity for biomass conversion to fuels by hydrothermal processing. In this study, grape pomace slurries from two varieties, Montepulciano and cabernet sauvignon, have been converted into a biocrude by hydrothermal liquefaction (HTL) in a bench-scale, continuous-flow reactor system. Carbon conversion to gravity-separable biocrude product up to 56 % was accomplished at relatively low temperature (350 C) in a pressurized (sub-critical liquid water) environment (20 MPa) when using grape pomace feedstock slurry with a 16.8 wt% concentration of dry solids processed at a liquid hourly space velocity of 2.1 h-1. Direct oil recovery was achievedmore » without the use of a solvent and biomass trace mineral components were removed by processing steps so that they did not cause processing difficulties. In addition, catalytic hydrothermal gasification (CHG) was effectively applied for HTL byproduct water cleanup using a Ru on C catalyst in a fixed bed producing a gas composed of methane and carbon dioxide from water soluble organics. Conversion of 99.8% of the chemical oxygen demand (COD) left in the aqueous phase was demonstrated. As a result, high conversion of grape pomace to liquid and gas fuel products was found with residual organic contamination in byproduct water reduced to <150 mg/kg COD.« less

Alternative Fuels Data Center

Science.gov Websites

vehicles altered to operate on propane, natural gas, methane gas, ethanol, or electricity are classified as information about vehicle conversion certification requirements, see the Alternative Fuels Data Center's

Biogasification of Walt Disney World biomass waste blend. Annual report Jan-Dec 82

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

Biljetina, R.; Chynoweth, D.P.; Janulis, J.

1983-05-01

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 facility (ETU) is being designed and installed at the Reedy Creek Wastewater Treatment Plant at Walt Disney World, Orlando, Florida. The facility will integrate a biomethanogenic conversion process with a waste-water treatment process employing water hyacinth ponds for secondary and tertiary treatment of sewage produced at Walt Disney World. The ETU will be capable of feeding 1-wet ton per day of water hyacinth-sludge blends to the digestion system for productionmore » of methane and other byproducts. The detailed design of the facility has been completed and procurement of equipment is in progress.« less

Microbially-Enhanced Coal Bed Methane: Strategies for Increased Biogenic Production

NASA Astrophysics Data System (ADS)

Davis, K.; Barhart, E. P.; Schweitzer, H. D.; Cunningham, A. B.; Gerlach, R.; Hiebert, R.; Fields, M. W.

2014-12-01

Coal is the largest fossil fuel resource in the United States. Most of this coal is deep in the subsurface making it costly and potentially dangerous to extract. However, in many of these deep coal seams, methane, the main component of natural gas, has been discovered and successfully harvested. Coal bed methane (CBM) currently accounts for approximately 7.5% of the natural gas produced in the U.S. Combustion of natural gas produces substantially less CO2 and toxic emissions (e.g. heavy metals) than combustion of coal or oil thereby making it a cleaner energy source. In the large coal seams of the Powder River Basin (PRB) in southeast Montana and northeast Wyoming, CBM is produced almost entirely by biogenic processes. The in situ conversion of coal to CBM by the native microbial community is of particular interest for present and future natural gas sources as it provides the potential to harvest energy from coal seams with lesser environmental impacts than mining and burning coal. Research at Montana State University has shown the potential for enhancing the subsurface microbial processes that produce CBM. Long-term batch enrichments have investigated the methane enhancement potential of yeast extract as well as algal and cyanobacterial biomass additions with increased methane production observed with all three additions when compared to no addition. Future work includes quantification of CBM enhancement and normalization of additions. This presentation addresses the options thus far investigated for increasing CBM production and the next steps for developing the enhanced in situ conversion of coal to CBM.

Hydrate kinetics study in the presence of nonaqueous liquid by nuclear magnetic resonance spectroscopy and imaging.

PubMed

Susilo, Robin; Moudrakovski, Igor L; Ripmeester, John A; Englezos, Peter

2006-12-28

The dynamics of methane hydrate growth and decomposition were studied by nuclear magnetic resonance (NMR) spectroscopy and imaging (MRI). Three well-known large molecule guest substances (LMGS) were used as structure H hydrate formers: 2,2-dimethylbutane (NH), methylcyclohexane (MCH), tert-butyl methyl ether (TBME). In addition, the impact of a non-hydrate former (n-heptane/nC7) was studied. The methane diffusion and hydrate growth were monitored by recording the 2H NMR spectra at 253 K and approximately 4.5 MPa for 20 h. The results revealed that methane diffuses faster in TBME and NH, slower in nC7, and slowest in MCH. The TBME system gives the fastest hydrate formation kinetics followed by NH, MCH, and nC7. The conversion of water into hydrate was also observed. The imaging study showed that TBME has a strong affinity toward ice, which is not the case for the NH and MCH systems. The degree of ice packing was also found to affect the LMGS distribution between ice particles. Highly packed ice increases the mass transfer resistance and hence limits the contact between LMGS and ice. It was also found that "temperature ramping" above the ice point improves the conversion significantly. Finally, hydrates were found to dissociate quickly within the first hour at atmospheric pressure and subsequently at a much slower rate. Methane dissolved in LMGS was also seen. The residual methane in hydrate phase and dissolved in LMGS phase explain the faster kinetics during hydrate re-formation.

Enzymes involved in the anaerobic oxidation of n-alkanes: from methane to long-chain paraffins

PubMed Central

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

Direct measurements of methane emissions from abandoned oil and gas wells in Pennsylvania

PubMed Central

Kang, Mary; Kanno, Cynthia M.; Reid, Matthew C.; Zhang, Xin; Mauzerall, Denise L.; Celia, Michael A.; Chen, Yuheng; Onstott, Tullis C.

2014-01-01

Abandoned oil and gas wells provide a potential pathway for subsurface migration and emissions of methane and other fluids to the atmosphere. Little is known about methane fluxes from the millions of abandoned wells that exist in the United States. Here, we report direct measurements of methane fluxes from abandoned oil and gas wells in Pennsylvania, using static flux chambers. A total of 42 and 52 direct measurements were made at wells and at locations near the wells (“controls”) in forested, wetland, grassland, and river areas in July, August, October 2013 and January 2014, respectively. The mean methane flow rates at these well locations were 0.27 kg/d/well, and the mean methane flow rate at the control locations was 4.5 × 10−6 kg/d/location. Three out of the 19 measured wells were high emitters that had methane flow rates that were three orders of magnitude larger than the median flow rate of 1.3 × 10−3 kg/d/well. Assuming the mean flow rate found here is representative of all abandoned wells in Pennsylvania, we scaled the methane emissions to be 4–7% of estimated total anthropogenic methane emissions in Pennsylvania. The presence of ethane, propane, and n-butane, along with the methane isotopic composition, indicate that the emitted methane is predominantly of thermogenic origin. These measurements show that methane emissions from abandoned oil and gas wells can be significant. The research required to quantify these emissions nationally should be undertaken so they can be accurately described and included in greenhouse gas emissions inventories. PMID:25489074

Direct measurements of methane emissions from abandoned oil and gas wells in Pennsylvania.

PubMed

Kang, Mary; Kanno, Cynthia M; Reid, Matthew C; Zhang, Xin; Mauzerall, Denise L; Celia, Michael A; Chen, Yuheng; Onstott, Tullis C

2014-12-23

Abandoned oil and gas wells provide a potential pathway for subsurface migration and emissions of methane and other fluids to the atmosphere. Little is known about methane fluxes from the millions of abandoned wells that exist in the United States. Here, we report direct measurements of methane fluxes from abandoned oil and gas wells in Pennsylvania, using static flux chambers. A total of 42 and 52 direct measurements were made at wells and at locations near the wells ("controls") in forested, wetland, grassland, and river areas in July, August, October 2013 and January 2014, respectively. The mean methane flow rates at these well locations were 0.27 kg/d/well, and the mean methane flow rate at the control locations was 4.5 × 10(-6) kg/d/location. Three out of the 19 measured wells were high emitters that had methane flow rates that were three orders of magnitude larger than the median flow rate of 1.3 × 10(-3) kg/d/well. Assuming the mean flow rate found here is representative of all abandoned wells in Pennsylvania, we scaled the methane emissions to be 4-7% of estimated total anthropogenic methane emissions in Pennsylvania. The presence of ethane, propane, and n-butane, along with the methane isotopic composition, indicate that the emitted methane is predominantly of thermogenic origin. These measurements show that methane emissions from abandoned oil and gas wells can be significant. The research required to quantify these emissions nationally should be undertaken so they can be accurately described and included in greenhouse gas emissions inventories.

Polarized electrode enhances biological direct interspecies electron transfer for methane production in upflow anaerobic bioelectrochemical reactor.

PubMed

Feng, Qing; Song, Young-Chae; Yoo, Kyuseon; Kuppanan, Nanthakumar; Subudhi, Sanjukta; Lal, Banwari

2018-08-01

The influence of polarized electrodes on the methane production, which depends on the sludge concentration, was investigated in upflow anaerobic bioelectrochemical (UABE) reactor. When the polarized electrode was placed in the bottom zone with a high sludge concentration, the methane production was 5.34 L/L.d, which was 53% higher than upflow anaerobic sludge blanket (UASB) reactor. However, the methane production was reduced to 4.34 L/L.d by placing the electrode in the upper zone of the UABE reactor with lower sludge concentration. In the UABE reactor, the methane production was mainly improved by the enhanced biological direct interspecies electron transfer (bDIET) pathway, and the methane production via the electrode was a minor fraction of less than 4% of total methane production. The polarized electrodes that placed in the bottom zone with a high sludge concentration enhance the bDIET for methane production in the UABE reactor and greatly improve the methane production. Copyright © 2018. Published by Elsevier Ltd.

Optimal Design of Biomass Utilization System for Rural Area Includes Technical and Economic Dimensions

NASA Astrophysics Data System (ADS)

Morioka, Yasuki; Nakata, Toshihiko

In order to design optimal biomass utilization system for rural area, OMNIBUS (The Optimization Model for Neo-Integrated Biomass Utilization System) has been developed. OMNIBUS can derive the optimal system configuration to meet different objective function, such as current account balance, amount of biomass energy supply, and CO2 emission. Most of biomass resources in a focused region e.g. wood biomass, livestock biomass, and crop residues are considered in the model. Conversion technologies considered are energy utilization technologies e.g. direct combustion and methane fermentation, and material utilization technologies e.g. composting and carbonization. Case study in Miyakojima, Okinawa prefecture, has been carried out for several objective functions and constraint conditions. Considering economics of the utilization system as a priority requirement, composting and combustion heat utilization are mainly chosen in the optimal system configuration. However gasification power plant and methane fermentation are included in optimal solutions, only when both biomass energy utilization and CO2 reduction have been set as higher priorities. External benefit of CO2 reduction has large impacts on the system configuration. Provided marginal external benefit of more than 50,000 JPY/t-C, external benefit becomes greater than the revenue from electricity and compost etc. Considering technological learning in the future, expensive technologies such as gasification power plant and methane fermentation will have economic feasibility as well as market competitiveness.

Alkane Oxidation: Methane Monooxygenases, Related Enzymes, and Their Biomimetics.

PubMed

Wang, Vincent C-C; Maji, Suman; Chen, Peter P-Y; Lee, Hung Kay; Yu, Steve S-F; Chan, Sunney I

2017-07-12

Methane monooxygenases (MMOs) mediate the facile conversion of methane into methanol in methanotrophic bacteria with high efficiency under ambient conditions. Because the selective oxidation of methane is extremely challenging, there is considerable interest in understanding how these enzymes carry out this difficult chemistry. The impetus of these efforts is to learn from the microbes to develop a biomimetic catalyst to accomplish the same chemical transformation. Here, we review the progress made over the past two to three decades toward delineating the structures and functions of the catalytic sites in two MMOs: soluble methane monooxygenase (sMMO) and particulate methane monooxygenase (pMMO). sMMO is a water-soluble three-component protein complex consisting of a hydroxylase with a nonheme diiron catalytic site; pMMO is a membrane-bound metalloenzyme with a unique tricopper cluster as the site of hydroxylation. The metal cluster in each of these MMOs harnesses O 2 to functionalize the C-H bond using different chemistry. We highlight some of the common basic principles that they share. Finally, the development of functional models of the catalytic sites of MMOs is described. These efforts have culminated in the first successful biomimetic catalyst capable of efficient methane oxidation without overoxidation at room temperature.

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.

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

PubMed Central

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

2013-01-01

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

Evaluating biochemical methane production from brewer's spent yeast.

PubMed

Sosa-Hernández, Ornella; Parameswaran, Prathap; Alemán-Nava, Gibrán Sidney; Torres, César I; Parra-Saldívar, Roberto

2016-09-01

Anaerobic digestion treatment of brewer's spent yeast (SY) is a viable option for bioenergy capture. The biochemical methane potential (BMP) assay was performed with three different samples (SY1, SY2, and SY3) and SY1 dilutions (75, 50, and 25 % on a v/v basis). Gompertz-equation parameters denoted slow degradability of SY1 with methane production rates of 14.59-4.63 mL/day and lag phases of 10.72-19.7 days. Performance and kinetic parameters were obtained with the Gompertz equation and the first-order hydrolysis model with SY2 and SY3 diluted 25 % and SY1 50 %. A SY2 25 % gave a 17 % of TCOD conversion to methane as well as shorter lag phase (<1 day). Average estimated hydrolysis constant for SY was 0.0141 (±0.003) day(-1), and SY2 25 % was more appropriate for faster methane production. Methane capture and biogas composition were dependent upon the SY source, and co-digestion (or dilution) can be advantageous.

Direct Quantification of Methane Emissions Across the Supply Chain: Identification of Mitigation Targets

NASA Astrophysics Data System (ADS)

Darzi, M.; Johnson, D.; Heltzel, R.; Clark, N.

2017-12-01

Researchers at West Virginia University's Center for Alternative Fuels, Engines, and Emissions have recently participated in a variety of studies targeted at direction quantification of methane emissions from across the natural gas supply chain. These studies included assessing methane emissions from heavy-duty vehicles and their fuel stations, active unconventional well sites - during both development and production, natural gas compression and storage facilities, natural gas engines - both large and small, two- and four-stroke, and low-throughput equipment associated with coal bed methane wells. Engine emissions were sampled using conventional instruments such as Fourier transform infrared spectrometers and heated flame ionization detection analyzers. However, to accurately quantify a wide range of other sources beyond the tailpipe (both leaks and losses), a full flow sampling system was developed, which included an integrated cavity-enhanced absorption spectrometer. Through these direct quantification efforts and analysis major sources of methane emissions were identified. Technological solutions and best practices exist or could be developed to reduce methane emissions by focusing on the "lowest-hanging fruit." For example, engine crankcases from across the supply chain should employ vent mitigation systems to reduce methane and other emissions. An overview of the direct quantification system and various campaign measurements results will be presented along with the identification of other targets for additional mitigation.

Evidence of sulfate-dependent anaerobic methane oxidation ...

EPA Pesticide Factsheets

The rapid development of unconventional gas resources has been accompanied by an increase in public awareness regarding the potential effects of drilling operations on drinking water sources. Incidents have been reported involving blowouts (e.g., Converse County, WY; Lawrence Township, PA; Aliso Canyon, CA) and home/property explosions (e.g., Bainbridge Township, OH; Dimock, PA; Huerfano County, CO) caused by methane migration in the subsurface within areas of natural gas development. We evaluated water quality characteristics in the northern Raton Basin of Colorado and documented the response of the Poison Canyon aquifer system several years after upward migration of methane gas occurred from the deeper Vermejo Formation coalbed production zone. Results show persistent secondary water quality impacts related to the biodegradation of methane. We identify four distinct characteristics of groundwater methane attenuation in the Poison Canyon aquifer: (i) consumption of methane and sulfate and production of sulfide and bicarbonate, (ii) methane loss coupled to production of higher-molecular-weight (C2+) gaseous hydrocarbons, (iii) patterns of 13C enrichment and depletion in methane and dissolved inorganic carbon, and (iv) a systematic shift in sulfur and oxygen isotope ratios of sulfate, indicative of microbial sulfate reduction. We also show that the biogeochemical response of the aquifer system has not mobilized naturally occurring trace metals, including arsenic,

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.

High performance biological methanation in a thermophilic anaerobic trickle bed reactor.

PubMed

Strübing, Dietmar; Huber, Bettina; Lebuhn, Michael; Drewes, Jörg E; Koch, Konrad

2017-12-01

In order to enhance energy efficiency of biological methanation of CO 2 and H 2 , this study investigated the performance of a thermophilic (55°C) anaerobic trickle bed reactor (ATBR) (58.1L) at ambient pressure. With a methane production rate of up to 15.4m 3 CH4 /(m 3 trickle bed ·d) at methane concentrations above 98%, the ATBR can easily compete with the performance of other mixed culture methanation reactors. Control of pH and nutrient supply turned out to be crucial for stable operation and was affected significantly by dilution due to metabolic water production, especially during demand-orientated operation. Considering practical applications, inoculation with digested sludge, containing a diverse biocenosis, showed high adaptive capacity due to intrinsic biological diversity. However, no macroscopic biofilm formation was observed at thermophilic conditions even after 313days of operation. The applied approach illustrates the high potential of thermophilic ATBRs as a very efficient energy conversion and storage technology. Copyright © 2017 Elsevier Ltd. All rights reserved.

Evaluating the influences of mixing strategies on the Biochemical Methane Potential test.

PubMed

Wang, Bing; Björn, Annika; Strömberg, Sten; Nges, Ivo Achu; Nistor, Mihaela; Liu, Jing

2017-01-01

Mixing plays an important role in the Biochemical Methane Potential (BMP) test, but only limited efforts have been put into it. In this study, various mixing strategies were applied to evaluate the influences on the BMP test, i.e., no mixing, shaking in water bath, shake manually once per day (SKM), automated unidirectional and bidirectional mixing. The results show that the effects of mixing are prominent for the most viscous substrate investigated, as both the highest methane production and highest maximal daily methane production were obtained at the highest mixing intensity. However, the organic removal efficiencies were not affected, which might offer evidence that mixing helps the release of gases trapped in digester liquid. Moreover, mixing is required for improved methane production when the digester content is viscous, conversely, mixing is unnecessary or SKM might be sufficient for the BMP test if the digester content is quite dilute or the substrate is easily degraded. Copyright © 2016 Elsevier Ltd. All rights reserved.

A new method of two-phase anaerobic digestion for fruit and vegetable waste treatment.

PubMed

Wu, Yuanyuan; Wang, Cuiping; Liu, Xiaoji; Ma, Hailing; Wu, Jing; Zuo, Jiane; Wang, Kaijun

2016-07-01

A novel method of two-phase anaerobic digestion where the acid reactor is operated at low pH 4.0 was proposed and investigated. A completely stirred tank acid reactor and an up-flow anaerobic sludge bed methane reactor were operated to examine the possibility of efficient degradation of lactate and to identify their optimal operating conditions. Lactate with an average concentration of 14.8g/L was the dominant fermentative product and Lactobacillus was the predominant microorganism in the acid reactor. The effluent from the acid reactor was efficiently degraded in the methane reactor and the average methane yield was 261.4ml/gCOD removed. Organisms of Methanosaeta were the predominant methanogen in granular sludge of methane reactor, however, after acclimation hydrogenotrophic methanogens enriched, which benefited for the conversion of lactate to acetate. The two-phase AD system exhibited a low hydraulic retention time of 3.56days and high methane yield of 348.5ml/g VS removed. Copyright © 2016 Elsevier Ltd. All rights reserved.

Determination of the isotopic composition of atmospheric methane and its application in the Antarctic

NASA Technical Reports Server (NTRS)

Lowe, David C.; Brenninkmeijer, Carl A. M.; Tyler, Stanley C.; Dlugkencky, Edward J.

1991-01-01

A procedure for establishing the C-13/C-12 ratio and the C-14 abundance in the atmospheric methane is discussed. The method involves air sample collection, measurement of the methane mixing ratio by gas chromotography followed by quantitative conversion of the methane in the air samples to CO2 and H2O, and analysis of the resulting CO2 for the C-13/C-12 ratio by stable isotope ratio mass spectrometry and measurement of C-14 content by accelerator mass spectrometry. The carbon isotropic composition of methane in air collected at Baring Head, New Zealand, and in air collected on aircraft flights between New Zealand and Antarctica is determined by the method, and no gradient in the composition between Baring Head and the South Pole station is found. As the technique is refined, and more data is gathered, small seasonal and long-term variations in C-13 are expected to be resolved.

Catalysts for conversion of methane to higher hydrocarbons

DOEpatents

Siriwardane, Ranjani V.

1993-01-01

Catalysts for converting methane to higher hydrocarbons such as ethane and ethylene in the presence of oxygen at temperatures in the range of about 700.degree. to 900.degree. C. are described. These catalysts comprise calcium oxide or gadolinium oxide respectively promoted with about 0.025-0.4 mole and about 0.1-0.7 mole sodium pyrophosphate. A preferred reaction temperature in a range of about 800.degree. to 850.degree. C. with a preferred oxygen-to-methane ratio of about 2:1 provides an essentially constant C.sub.2 hydrocarbon yield in the range of about 12 to 19 percent over a period of time greater than about 20 hours.

Artificial photosynthesis: biomimetic approaches to solar energy conversion and storage.

PubMed

Kalyanasundaram, K; Graetzel, M

2010-06-01

Using sun as the energy source, natural photosynthesis carries out a number of useful reactions such as oxidation of water to molecular oxygen and fixation of CO(2) in the form of sugars. These are achieved through a series of light-induced multi-electron-transfer reactions involving chlorophylls in a special arrangement and several other species including specific enzymes. Artificial photosynthesis attempts to reconstruct these key processes in simpler model systems such that solar energy and abundant natural resources can be used to generate high energy fuels and restrict the amount of CO(2) in the atmosphere. Details of few model catalytic systems that lead to clean oxidation of water to H(2) and O(2), photoelectrochemical solar cells for the direct conversion of sunlight to electricity, solar cells for total decomposition of water and catalytic systems for fixation of CO(2) to fuels such as methanol and methane are reviewed here. Copyright 2010 Elsevier Ltd. All rights reserved.

Biological conversion of biogas to methanol using methanotrophs isolated from solid-state anaerobic digestate.

PubMed

Sheets, Johnathon P; Ge, Xumeng; Li, Yueh-Fen; Yu, Zhongtang; Li, Yebo

2016-02-01

The aim of this work was to isolate methanotrophs (methane oxidizing bacteria) that can directly convert biogas produced at a commercial anaerobic digestion (AD) facility to methanol. A methanotrophic bacterium was isolated from solid-state anaerobic digestate. The isolate had characteristics comparable to obligate methanotrophs from the genus Methylocaldum. This newly isolated methanotroph grew on biogas or purified CH4 and successfully converted biogas from AD to methanol. Methanol production was achieved using several methanol dehydrogenase (MDH) inhibitors and formate as an electron donor. The isolate also produced methanol using phosphate with no electron donor or using formate with no MDH inhibitor. The maximum methanol concentration (0.43±0.00gL(-1)) and 48-h CH4 to methanol conversion (25.5±1.1%) were achieved using biogas as substrate and a growth medium containing 50mM phosphate and 80mM formate. Copyright © 2015 Elsevier Ltd. All rights reserved.

Livestock waste-to-bioenergy generation opportunities.

PubMed

Cantrell, Keri B; Ducey, Thomas; Ro, Kyoung S; Hunt, Patrick G

2008-11-01

The use of biological and thermochemical conversion (TCC) technologies in livestock waste-to-bioenergy treatments can provide livestock operators with multiple value-added, renewable energy products. These products can meet heating and power needs or serve as transportation fuels. The primary objective of this work is to present established and emerging energy conversion opportunities that can transform the treatment of livestock waste from a liability to a profit center. While biological production of methanol and hydrogen are in early research stages, anaerobic digestion is an established method of generating between 0.1 to 1.3m3m(-3)d(-1) of methane-rich biogas. The TCC processes of pyrolysis, direct liquefaction, and gasification can convert waste into gaseous fuels, combustible oils, and charcoal. Integration of biological and thermal-based conversion technologies in a farm-scale hybrid design by combining an algal CO2-fixation treatment requiring less than 27,000m2 of treatment area with the energy recovery component of wet gasification can drastically reduce CO2 emissions and efficiently recycle nutrients. These designs have the potential to make future large scale confined animal feeding operations sustainable and environmentally benign while generating on-farm renewable energy.

The Mars Methane Analogue Mission (M3): Results of the 2011 Field Deployment

NASA Astrophysics Data System (ADS)

Cloutis, E. A.; Whyte, L.; Qadi, A.; Bell, J. F.; Berard, G.; Boivin, A.; Ellery, A.; Haddad, E.; Jamroz, W.; Kruzelecky, R.; Mann, P.; Olsen, K.; Perrot, M.; Popa, D.; Rhind, T.; Samson, C.; Sharma, R.; Stromberg, J.; Strong, K.; Tremblay, A.; Wilhelm, R.; Wing, B.; Wong, B.

2012-03-01

The M3 mission simulated a rover mission to Mars to search for sources of methane. The 2011 campaign found that methane plumes from serpentinite are very localized and target selection based on imagery is preferred over direct methane detection.

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

Bio-energy conversion performance, biodegradability, and kinetic analysis of different fruit residues during discontinuous anaerobic digestion.

PubMed

Zhao, Chen; Yan, Hu; Liu, Yan; Huang, Yan; Zhang, Ruihong; Chen, Chang; Liu, Guangqing

2016-06-01

Huge amounts of fruit residues are produced and abandoned annually. The high moisture and organic contents of these residues makes them a big problem to the environment. Conversely, they are a potential resource to the world. Anaerobic digestion is a good way to utilize these organic wastes. In this study, the biomethane conversion performances of a large number of fruit residues were determined and compared using batch anaerobic digestion, a reliable and easily accessible method. The results showed that some fruit residues containing high contents of lipids and carbohydrates, such as loquat peels and rambutan seeds, were well fit for anaerobic digestion. Contrarily, residues with high lignin content were strongly recommended not to be used as a single substrate for methane production. Multiple linear regression model was adopted to simulate the correlation between the organic component of these fruit residues and their experimental methane yield, through which the experimental methane yield could probably be predicted for any other fruit residues. Four kinetic models were used to predict the batch anaerobic digestion process of different fruit residues. It was shown that the modified Gompertz and Cone models were better fit for the fruit residues compared to the first-order and Fitzhugh models. The first findings of this study could provide useful reference and guidance for future studies regarding the applications and potential utilization of fruit residues. Copyright © 2016 Elsevier Ltd. All rights reserved.

40 CFR Table A-7 to Subpart A of... - Data Elements That Are Inputs to Emission Equations and for Which the Reporting Deadline Is March...

Code of Federal Regulations, 2014 CFR

2014-07-01

....116(b) Only annual production by product from each EAF (No CEMS). K 98.116(e)(4) All. K 98.116(e)(5... factor if using Eq. Y-3. Y 98.256(e)(10) Only fraction of carbon in the flare gas contributed by methane... methane in coking gas. Y 98.256(l)(5) Only molar volume conversion factor. Y 98.256(m)(3) Only total...

Project identification for methane reduction options

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

Kerr, T.

1996-12-31

This paper discusses efforts directed at reduction in emission of methane to the atmosphere. Methane is a potent greenhouse gas, which on a 20 year timeframe may present a similar problem to carbon dioxide. In addition, methane causes additional problems in the form of smog and its longer atmospheric lifetime. The author discusses strategies for reducing methane emission from several major sources. This includes landfill methane recovery, coalbed methane recovery, livestock methane reduction - in the form of ruminant methane reduction and manure methane recovery. The author presents examples of projects which have implemented these ideas, the economics of themore » projects, and additional gains which come from the projects.« less

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

PubMed

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

2014-08-19

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

Selective anaerobic oxidation of methane enables direct synthesis of methanol.

PubMed

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.

Phosphoketolase overexpression increases biomass and lipid yield from methane in an obligate methanotrophic biocatalyst

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

Henard, Calvin A.; Smith, Holly K.; Guarnieri, Michael T.

Microbial conversion of methane to high-value bio-based chemicals and materials offers a path to mitigate GHG emissions and valorize this abundant-yet -underutilized carbon source. In addition to fermentation optimization strategies, rational methanotrophic bacterial strain engineering offers a means to reach industrially relevant titers, carbon yields, and productivities of target products. The phosphoketolase pathway functions in heterofermentative bacteria where carbon flux through two sugar catabolic pathways to mixed acids (lactic acid and acetic acid) increases cellular ATP production. Importantly, this pathway also serves as an alternative route to produce acetyl-CoA that bypasses the CO 2 lost through pyruvate decarboxylation in themore » Embden-Meyerhof-Parnas pathway. Thus, the phosphoketolase pathway can be leveraged for carbon efficient biocatalysis to acetyl-CoA-derived intermediates and products. Here, we show that the industrially promising methane biocatalyst, Methylomicrobium buryatense, encodes two phosphoketolase isoforms that are expressed in methanol- and methane-grown cells. Overexpression of the PktB isoform led to a 2-fold increase in intracellular acetyl-CoA concentration, and a 2.6-fold yield enhancement from methane to microbial biomass and lipids compared to wild-type, increasing the potential for methanotroph lipid-based fuel production. Off-gas analysis and metabolite profiling indicated that global metabolic rearrangements, including significant increases in post-translational protein acetylation and gene expression of the tetrahydromethanopterin-linked pathway, along with decreases in several excreted products, coincided with the superior biomass and lipid yield observed in the engineered strain. Further, these data suggest that phosphoketolase may play a key regulatory role in methanotrophic bacterial metabolism. As a result, given that acetyl-CoA is a key intermediate in several biosynthetic pathways, phosphoketolase overexpression offers a viable strategy to enhance the economics of an array of biological methane conversion processes.« less

Phosphoketolase overexpression increases biomass and lipid yield from methane in an obligate methanotrophic biocatalyst.

PubMed

Henard, Calvin A; Smith, Holly K; Guarnieri, Michael T

2017-05-01

Microbial conversion of methane to high-value bio-based fuels, chemicals, and materials offers a path to mitigate GHG emissions and valorize this abundant-yet -underutilized carbon source. In addition to fermentation optimization strategies, rational methanotrophic bacterial strain engineering offers a means to reach industrially relevant titers, carbon yields, and productivities of target products. The phosphoketolase pathway functions in heterofermentative bacteria where carbon flux through two sugar catabolic pathways to mixed acids (lactic acid and acetic acid) increases cellular ATP production. Importantly, this pathway also serves as an alternative route to produce acetyl-CoA that bypasses the CO 2 lost through pyruvate decarboxylation in the Embden-Meyerhof-Parnas pathway. Thus, the phosphoketolase pathway can be leveraged for carbon efficient biocatalysis to acetyl-CoA-derived intermediates and products. Here, we show that the industrially promising methane biocatalyst, Methylomicrobium buryatense, encodes two phosphoketolase isoforms that are expressed in methanol- and methane-grown cells. Overexpression of the PktB isoform led to a 2-fold increase in intracellular acetyl-CoA concentration, and a 2.6-fold yield enhancement from methane to microbial biomass and lipids compared to wild-type, increasing the potential for methanotroph lipid-based fuel production. Off-gas analysis and metabolite profiling indicated that global metabolic rearrangements, including significant increases in post-translational protein acetylation and gene expression of the tetrahydromethanopterin-linked pathway, along with decreases in several excreted products, coincided with the superior biomass and lipid yield observed in the engineered strain. Further, these data suggest that phosphoketolase may play a key regulatory role in methanotrophic bacterial metabolism. Given that acetyl-CoA is a key intermediate in several biosynthetic pathways, phosphoketolase overexpression offers a viable strategy to enhance the economics of an array of biological methane conversion processes. Copyright © 2017. Published by Elsevier Inc.

Phosphoketolase overexpression increases biomass and lipid yield from methane in an obligate methanotrophic biocatalyst

DOE PAGES

Henard, Calvin A.; Smith, Holly K.; Guarnieri, Michael T.

2017-04-02

Microbial conversion of methane to high-value bio-based chemicals and materials offers a path to mitigate GHG emissions and valorize this abundant-yet -underutilized carbon source. In addition to fermentation optimization strategies, rational methanotrophic bacterial strain engineering offers a means to reach industrially relevant titers, carbon yields, and productivities of target products. The phosphoketolase pathway functions in heterofermentative bacteria where carbon flux through two sugar catabolic pathways to mixed acids (lactic acid and acetic acid) increases cellular ATP production. Importantly, this pathway also serves as an alternative route to produce acetyl-CoA that bypasses the CO 2 lost through pyruvate decarboxylation in themore » Embden-Meyerhof-Parnas pathway. Thus, the phosphoketolase pathway can be leveraged for carbon efficient biocatalysis to acetyl-CoA-derived intermediates and products. Here, we show that the industrially promising methane biocatalyst, Methylomicrobium buryatense, encodes two phosphoketolase isoforms that are expressed in methanol- and methane-grown cells. Overexpression of the PktB isoform led to a 2-fold increase in intracellular acetyl-CoA concentration, and a 2.6-fold yield enhancement from methane to microbial biomass and lipids compared to wild-type, increasing the potential for methanotroph lipid-based fuel production. Off-gas analysis and metabolite profiling indicated that global metabolic rearrangements, including significant increases in post-translational protein acetylation and gene expression of the tetrahydromethanopterin-linked pathway, along with decreases in several excreted products, coincided with the superior biomass and lipid yield observed in the engineered strain. Further, these data suggest that phosphoketolase may play a key regulatory role in methanotrophic bacterial metabolism. As a result, given that acetyl-CoA is a key intermediate in several biosynthetic pathways, phosphoketolase overexpression offers a viable strategy to enhance the economics of an array of biological methane conversion processes.« less

Methane production by anaerobic digestion of Bermuda grass

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

Klass, D.L.; Ghosh, S.

1979-01-01

Bermuda grass (Cynodon dactylon) is one of the high-yield warm-season grasses that has been suggested as a promising raw material for conversion to methane. Experimental work performed with laboratory digesters to study the anaerobic digestion of Coastal Bermuda grass harvested in Louisiana and having a C/N ratio of 24 is described. Methane yields of about 1.9 SCF/lb of volatile solids( VS) added were observed under conventional mesophilic high-rate conditions. When supplemental nitrogen additions were made, the yields increased up to 3.5 SCF/lb of VS added indicating that the nitrogen content of the grass examined was insufficient to sustain high-rate digestionmore » at the higher yield level. Thermophilic digestion with supplemental nitrogen additions afforded methane yields of about 2.7 SCF/lb VS added. Carbon and energy balances were calculated and the relative biodegradabilities of the organics were estimated.« less

Mars Atmospheric Conversion to Methane and Water: An Engineering Model of the Sabatier Reactor with Characterization of Ru/Al2O3 for Long Duration Use on Mars

NASA Technical Reports Server (NTRS)

Meier, Anne J.; Shah, Malay; Petersen, Elspeth; Hintze, Paul; Muscatello, Tony

2017-01-01

The Atmospheric Processing Module (APM) is a Mars In-Situ Resource Utilization (ISRU) technology designed to demonstrate conversion of the Martian atmosphere into methane and water. The Martian atmosphere consists of approximately 95 carbon dioxide (CO2) and residual argon and nitrogen. APM utilizes cryocoolers for CO2 acquisition from a simulated Martian atmosphere and pressure. The captured CO2 is sublimated and pressurized as a feedstock into the Sabatier reactor, which converts CO2 and hydrogen to methane and water. The Sabatier reaction occurs over a packed bed reactor filled with Ru/Al2O3 pellets. The long duration use of the APM system and catalyst was investigated for future scaling and failure limits. Failure of the catalyst was detected by gas chromatography and temperature sensors on the system. Following this, characterization and experimentation with the catalyst was carried out with analysis including x-ray photoelectron spectroscopy and scanning electron microscopy with elemental dispersive spectroscopy. This paper will discuss results of the catalyst performance, the overall APM Sabatier approach, as well as intrinsic catalyst considerations of the Sabatier reactor performance incorporated into a chemical model.

Initial development and performance evaluation of a process for formation of dense carbon by pyrolysis of methane

NASA Technical Reports Server (NTRS)

Noyes, G. P.; Cusick, R. J.

1985-01-01

The three steps in pyrolytic carbon formation are: (1) gaseous hydrocarbon polymerization and aromatic formation; (2) gas-phase condensation and surface adsorption/impingement of polyaromatic hydrocarbon; and (3) final dehydration to carbon. The structure of the carbon in the various stages of formation is examined. The apparatuses and experimental procedures for the pyrolysis of methane in a 60 cm long quartz reactor tube at temperatures ranging from 1400-1600 K are described. The percentage of carbon converted and its density are calculated and tabularly presented. The results reveal that dense carbon formation is maximized and soot eliminated by this procedure. It is observed that conversion efficiency depends on the composition of the inlet gas and conversion increases with increasing temperature. Based on the experimental data a three-man carbon reactor subsystem (CRS) is developed; the functions of the Sabatier Methanation Reactor, two carbon formation reactors and fluid handling components of the CRS are analyzed. The CRS forms 16 kg of carbon at a rate of 0.8 kg/day for 20 days in a two percent volume density quartz wool packing at temperature of 1500-1600 K.

Direct catalytic conversion of methane and light hydrocarbon gases. Quarterly report No. 10, January 1--March 31, 1989

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. In this reporting period, we have utilized samples of magnesia differing in their pretreatment temperature. Both the hydrido-ruthenium complex H{sub 4}Ru{sub 4}(CO){sub 12} and its reaction product with triethyl aluminum were reacted with these samples. The two ruthenium clusters are expected to react with the magnesia surface in different ways: by deprotonation of the hydride through an acid-base reaction with the basic surface, or by hydrolysis ofmore » the aluminum-carbon bond of the triethyl aluminum adduct. The concentration of hydroxyl groups on the magnesia surface able to hydrolyze the aluminum-carbon bond for immobilation should vary depending on the temperature of the pretreatment; the concentration of basic sites which can deprotonate the cluster should also vary with temperature. These differences were borne out by the experiment. We also compared the activity of two batches of AlRu{sub 4}/MgO which had been synthesized at different times in the project. Both batches had approximately the same activity, but the newer batch had greater selectivity for C{sub 6+} hydrocarbons.« less

Aerobic methane production in surface waters of the Gulf of Mexico

NASA Astrophysics Data System (ADS)

Finke, N.; Crespo-Medina, M.; Schweers, J.; Joye, S. B.

2011-12-01

Near surface water of the global oceans often show elevated methane concentrations compared to the water column below with concentrations in supersaturation in regard to the atmosphere (Lamontagne et al. 1973), resulting in a source of this potent greenhouse gas to the atmosphere. The mechanisms leading to methane supersaturation in surface waters remains unclear. Incubations with Trichodesmium-containing Pacific surface water suggested methylphosphonate as potential methane precursor under phosphate limiting conditions (Karl et al. 2008), whereas in phosphate rich Arctic surface waters, DMSP addition stimulated methane production (Damm et al. 2010). Surface waters of the Gulf of Mexico typically exhibit a methane maximum that is conincident with the deep chlorophyll maximum, below the depths where Trichodesmium is abundant. Addition of methylphosphonate, dimethylsulfoniopropionate (DMSP) or methane thiol (MeSH), the proposed methane precursor in DMSP conversion to methane, to oxic sea water did not affect methane production within the chlorophyll maximum at most stations, whereas methyl phosphonate addition stimulated methane production in the surface water and proposed deep Trichodesmium horizon. Pre-filtration of the water through a 10 μm sieve, which eliminated Trichodesmium, or through a 1.2 μm filter, which eliminated additional cyanobacteria such as Synechococcus, did not reduce methane production. Under dark oxic and dark anoxic conditions, however, methane production was reduced 5 and 7-20 fold, respectively, indicating that anerobic methane production in anoxic microniches is not responsible for the methane production. The reduction of methane production under dark conditions suggests that methane production is, in some yet unrecognized way, linked to phototrophic metabolism. Cyanobacteria are likely not responsible for the observed aerobic methane production in the surface waters of the Gulf of Mexico and while methylphosphonate is a potential precursor in the surface waters, the precursor and methanism of methane production within the coincident deep chlorophyll/methane maximum remains unknown. Lamontagne R, Swinnert J, Linnenbo V, Smith WD (1973) Methane concentrations in various marine environments. Journal of Geophysical Research 78, 5317-5324 Karl DM et al. (2008) Aerobic production of methane in the sea. Nature Geosciences 1, 473-478 Damm E et al. (2010) Methane production in aerobic oligotrophic surface water in the central Arctic Ocean. Biogeosciences 7, 1099-1108

Enhanced activity and stability of La-doped CeO2 monolithic catalysts for lean-oxygen methane combustion.

PubMed

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.

Reducing the environmental impact of methane emissions from dairy farms by anaerobic digestion of cattle waste.

PubMed

Marañón, E; Salter, A M; Castrillón, L; Heaven, S; Fernández-Nava, Y

2011-08-01

Four dairy cattle farms considered representative of Northern Spain milk production were studied. Cattle waste was characterised and energy consumption in the farms was inventoried. Methane emissions due to slurry/manure management and fuel consumption on the farms were calculated. The possibility of applying anaerobic digestion to the slurry to minimise emissions and of using the biogas produced to replace fossil fuels on the farm was considered. Methane emissions due to slurry management (storage and use as fertiliser) ranged from 34 to 66kg CH(4)cow(-1)year(-1) for dairy cows and from 13 to 25kg CH(4)cow(-1)year(-1) for suckler calves. Cattle on these farms are housed for most of the year, and the contribution from emissions from manure dropped in pastures is insignificant due to the very low methane conversion factors. If anaerobic digestion were implemented on the farms, the potential GHG emissions savings per livestock unit would range from 978 to 1776kg CO(2)eq year(-1), with the main savings due to avoided methane emissions during slurry management. The methane produced would be sufficient to supply digester heating needs (35-55% of the total methane produced) and on-farm fuel energy requirements. Copyright © 2011 Elsevier Ltd. All rights reserved.

Temperature dependence of bioelectrochemical CO2 conversion and methane production with a mixed-culture biocathode.

PubMed

Yang, Hou-Yun; Bao, Bai-Ling; Liu, Jing; Qin, Yuan; Wang, Yi-Ran; Su, Kui-Zu; Han, Jun-Cheng; Mu, Yang

2018-02-01

This study evaluated the effect of temperature on methane production by CO 2 reduction during microbial electrosynthesis (MES) with a mixed-culture biocathode. Reactor performance, in terms of the amount and rate of methane production, current density, and coulombic efficiency, was compared at different temperatures. The microbial properties of the biocathode at each temperature were also analyzed by 16S rRNA gene sequencing. The results showed that the optimum temperature for methane production from CO 2 reduction in MES with a mixed-culture cathode was 50°C, with the highest amount and rate of methane production of 2.06±0.13mmol and 0.094±0.01mmolh -1 , respectively. In the mixed-culture biocathode MES, the coulombic efficiency of methane formation was within a range of 19.15±2.31% to 73.94±2.18% due to by-product formation at the cathode, including volatile fatty acids and hydrogen. Microbial analysis demonstrated that temperature had an impact on the diversity of microbial communities in the biofilm that formed on the MES cathode. Specifically, the hydrogenotrophic methanogen Methanobacterium became the predominant archaea for methane production from CO 2 reduction, while the abundance of the aceticlastic methanogen Methanosaeta decreased with increased temperature. Copyright © 2017. Published by Elsevier B.V.

Microbial minorities modulate methane consumption through niche partitioning

PubMed Central

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.

PubMed

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.

Mechanistic insights into heterogeneous methane activation

DOE PAGES

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

Molecular Simulation of the Phase Diagram of Methane Hydrate: Free Energy Calculations, Direct Coexistence Method, and Hyperparallel Tempering.

PubMed

Jin, Dongliang; Coasne, Benoit

2017-10-24

Different molecular simulation strategies are used to assess the stability of methane hydrate under various temperature and pressure conditions. First, using two water molecular models, free energy calculations consisting of the Einstein molecule approach in combination with semigrand Monte Carlo simulations are used to determine the pressure-temperature phase diagram of methane hydrate. With these calculations, we also estimate the chemical potentials of water and methane and methane occupancy at coexistence. Second, we also consider two other advanced molecular simulation techniques that allow probing the phase diagram of methane hydrate: the direct coexistence method in the Grand Canonical ensemble and the hyperparallel tempering Monte Carlo method. These two direct techniques are found to provide stability conditions that are consistent with the pressure-temperature phase diagram obtained using rigorous free energy calculations. The phase diagram obtained in this work, which is found to be consistent with previous simulation studies, is close to its experimental counterpart provided the TIP4P/Ice model is used to describe the water molecule.

Methane and Nitrous Oxide Emissions Reduced Following Conversion of Rice Paddies to Inland Crab-Fish Aquaculture in Southeast China.

PubMed

Liu, Shuwei; Hu, Zhiqiang; Wu, Shuang; Li, Shuqing; Li, Zhaofu; Zou, Jianwen

2016-01-19

Aquaculture is an important source of atmospheric methane (CH4) and nitrous oxide (N2O), while few direct flux measurements are available for their regional and global source strength estimates. A parallel field experiment was performed to measure annual CH4 and N2O fluxes from rice paddies and rice paddy-converted inland crab-fish aquaculture wetlands in southeast China. Besides N2O fluxes dependent on water/sediment mineral N and CH4 fluxes related to water chemical oxygen demand, both CH4 and N2O fluxes from aquaculture were related to water/sediment temperature, sediment dissolved organic carbon, and water dissolved oxygen concentration. Annual CH4 and N2O fluxes from inland aquaculture averaged 0.37 mg m(-2) h(-1) and 48.1 μg m(-2) h(-1), yielding 32.57 kg ha(-1) and 2.69 kg N2O-N ha(-1), respectively. The conversion of rice paddies to aquaculture significantly reduced CH4 and N2O emissions by 48% and 56%, respectively. The emission factor for N2O was estimated to be 0.66% of total N input in the feed or 1.64 g N2O-N kg(-1) aquaculture production in aquaculture. The conversion of rice paddies to inland aquaculture would benefit for reconciling greenhouse gas mitigation and agricultural income increase as far as global warming potentials and net ecosystem economic profits are of concomitant concern. Some agricultural practices such as better aeration and feeding, and fallow season dredging would help to lower CH4 and N2O emissions from inland aquaculture. More field measurements from inland aquaculture are highly needed to gain an insight into national and global accounting of CH4 and N2O emissions.

Chemical Aspects of Astrophysically Observed Extraterrestrial Methanol, Hydrocarbon Derivatives, and Ions.

PubMed

Olah, George A; Mathew, Thomas; Prakash, G K Surya; Rasul, Golam

2016-02-10

Astrophysically observed extraterrestrial molecular matter contains, besides hydrogen and water, methane and methanol as the most abundant species. Feasible pathways and chemical aspects of their formation as well as of derived hydrocarbon homologues and their ions (carbocations and carbanions) are discussed on the basis of observed similarities with our studied terrestrial chemistry. The preferred pathway for converting extraterrestrial methane according to Ali et al. is based on CH5(+) and Olah's related nonclassical carbonium ion chemistry. On the basis of the observed higher reactivity of methanol compared with methane in various chemical reactions, a feasible new pathway is proposed for the conversion of extraterrestrial methanol to hydrocarbons, their derivatives, and carbocations together with a possible connection with methonium ion-based chemistry.

Development of a Hydrogasification Process for Co-Production of Substitute Natural Gas (SNG) and Electric Power from Western Coals-Phase I

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

Raymond Hobbs

2007-05-31

The Advanced Hydrogasification Process (AHP)--conversion of coal to methane--is being developed through NETL with a DOE Grant and has successfully completed its first phase of development. The results so far are encouraging and have led to commitment by DOE/NETL to begin a second phase--bench scale reactor vessel testing, expanded engineering analysis and economic perspective review. During the next decade new means of generating electricity, and other forms of energy, will be introduced. The members of the AHP Team envision a need for expanded sources of natural gas or substitutes for natural gas, to fuel power generating plants. The initial workmore » the team has completed on a process to use hydrogen to convert coal to methane (pipeline ready gas) shows promising potential. The Team has intentionally slanted its efforts toward the needs of US electric utilities, particularly on fuels that can be used near urban centers where the greatest need for new electric generation is found. The process, as it has evolved, would produce methane from coal by adding hydrogen. The process appears to be efficient using western coals for conversion to a highly sought after fuel with significantly reduced CO{sub 2} emissions. Utilities have a natural interest in the preservation of their industry, which will require a dramatic reduction in stack emissions and an increase in sustainable technologies. Utilities tend to rank long-term stable supplies of fuel higher than most industries and are willing to trade some ratio of cost for stability. The need for sustainability, stability and environmentally compatible production are key drivers in the formation and progression of the AHP development. In Phase II, the team will add a focus on water conservation to determine how the basic gasification process can be best integrated with all the plant components to minimize water consumption during SNG production. The process allows for several CO{sub 2} reduction options including consumption of the CO{sub 2} in the original process as converted to methane. The process could under another option avoid emissions following the conversion to SNG through an adjunct algae conversion process. The algae would then be converted to fuels or other products. An additional application of the algae process at the end use natural gas fired plant could further reduce emissions. The APS team fully recognizes the competition facing the process from natural gas and imported liquid natural gas. While we expect those resources to set the price for methane in the near-term, the team's work to date indicates that the AHP process can be commercially competitive, with the added benefit of assuring long-term energy supplies from North American resources. Conversion of coal to a more readily transportable fuel that can be employed near load centers with an overall reduction of greenhouses gases is edging closer to reality.« less

Bioassay for estimating the biogenic methane-generating potential of coal samples

USGS Publications Warehouse

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.

Fast Optimization of LiMgMnOx/La2O3 Catalysts for the Oxidative Coupling of Methane.

PubMed

Li, Zhinian; He, Lei; Wang, Shenliang; Yi, Wuzhong; Zou, Shihui; Xiao, Liping; Fan, Jie

2017-01-09

The development of efficient catalyst for oxidative coupling of methane (OCM) reaction represents a grand challenge in direct conversion of methane into other useful products. Here, we reported that a newly developed combinatorial approach can be used for ultrafast optimization of La 2 O 3 -based multicomponent metal oxide catalysts in OCM reaction. This new approach integrated inkjet printing assisted synthesis (IJP-A) with multidimensional group testing strategy (m-GT) tactfully takes the place of conventionally high-throughput synthesis-and-screen experiment. Just within a week, 2048 formulated LiMgMnO x -La 2 O 3 catalysts in a 64·8·8·8·8 = 262 144 compositional space were fabricated by IJP-A in a four-round synthesis-and-screen process, and an optimized formulation has been successfully identified through only 4·8 = 32 times of tests via m-GT screening strategy. The screening process identifies the most promising ternary composition region is Li 0-0.48 Mg 0-6.54 Mn 0-0.62 -La 100 O x with an external C 2 yield of 10.87% at 700 °C. The yield of C 2 is two times as high as the pure nano-La 2 O 3 . The good performance of the optimized catalyst formulation has been validated by the manual preparation, which further prove the effectiveness of the new combinatorial methodology in fast discovery of heterogeneous catalyst.

Application of a rotating impeller anode in a bioelectrochemical anaerobic digestion reactor for methane production from high-strength food waste.

PubMed

Park, Jungyu; Lee, Beom; Shin, Wonbeom; Jo, Sangyeol; Jun, Hangbae

2018-07-01

In this study, a practical bioelectrochemical anaerobic digestion (BEAD) reactor equipped with a rotating STS304 impeller was tested to verify its methane production performance. Methane production in the BEAD reactor was possible without accumulation of volatile fatty acids (VFAs) and decreases in pH at high organic loading rates (OLRs) up to 6 kg-COD/m 3 ·d (COD: chemical oxygen demand). Methane production in a BEAD-O (open circuit) reactor was inhibited at OLRs above 4 kg-COD/m 3 ·d; however, the performance could be recovered bioelectrochemically by supplying voltage. The population density of hydrogenotrophic methanogens increased to 73.3% in the BEAD-C (closed circuit) reactor, even at high OLRs, through the removal of VFAs and conversion of hydrogen to methane. The energy efficiency in the BEAD-C reactor was 85.6%, indicating that the commercialization of BEAD reactors equipped with rotating STS304 impeller electrodes is possible. Copyright © 2018 Elsevier Ltd. All rights reserved.

Biocatalytic methanation of hydrogen and carbon dioxide in an anaerobic three-phase system.

PubMed

Burkhardt, M; Koschack, T; Busch, G

2015-02-01

A new type of anaerobic trickle-bed reactor was used for biocatalytic methanation of hydrogen and carbon dioxide under mesophilic temperatures and ambient pressure in a continuous process. The conversion of gaseous substrates through immobilized hydrogenotrophic methanogenic archaea in a biofilm is a unique feature of this type of reactor. Due to the formation of a three-phase system on the carrier surface and operation as a plug flow reactor without gas recirculation, a complete reaction could be observed. With a methane concentration higher than c(CH4) = 98%, the product gas exhibits a very high quality. A specific methane production of P(CH4) = 1.49 Nm(3)/(m(3)(SV) d) was achieved at a hydraulic loading rate of LR(H2) = 6.0 Nm(3)/(m(3)(SV) d). The relation between trickle flow through the reactor and productivity could be shown. An application for methane enrichment in combination with biogas facilities as a source of carbon dioxide has also been positively proven. Copyright © 2014 Elsevier Ltd. All rights reserved.

IR Studies of the Spin-Nuclear Conversion in the Vicinity of alpha α - beta β - Transition in Cryodeposited Methane Films

NASA Astrophysics Data System (ADS)

Drobyshev, A.; Aldiyarov, A.; Sokolov, D.; Shinbayeva, A.

2017-06-01

Solid methane belongs to a group of crystals containing hydrogen atoms, whose macroscopic properties are greatly influenced by the spin interaction of hydrogen nuclei. In particular, the methane molecule, which has four protons with spin I=1/2, has three total spin modifications: para-, ortho- and meta-states with three values of the total spin moments of 0, 1 and 2, respectively. Equilibrium concentrations of these modifications and relaxation times are dependent on the temperature, affecting the observed thermal properties of solid methane, such as thermal conductivity, specific heat, thermal expansion. In this paper, we attempt to explain the peculiarities of thin film growth of methane at cryogenic temperatures from the viewpoint of spin-nuclear transformations. Our observations of absorption intensity at a frequency corresponding to 1/2 of the absorption band amplitude of deformation vibrations record a step-like change in the position of the absorption band during the sample deposition process. The observed phenomenon, in our opinion, is the demonstration of spin transformations during deposition.

Insight into the role of facultative bacteria stimulated by micro-aeration in continuous bioreactors converting LCFA to methane.

PubMed

Duarte, Maria Salomé; Silva, Sérgio A; Salvador, Andreia F; Cavaleiro, Ana Júlia; Stams, Alfons J M; Alves, Maria Madalena; Pereira, Maria Alcina

2018-05-15

Conversion of unsaturated long chain fatty acids (LCFA) to methane in continuous bioreactors is not fully understood. Palmitate (C16:0) often accumulates during oleate (C18:1) biodegradation in methanogenic bioreactors, and the reason why this happens and which microorganisms catalyze this reaction remains unknown. Facultative anaerobic bacteria are frequently found in continuous reactors operated at high LCFA loads, but their function is unclear. To get more insight on the role of these bacteria, LCFA conversion was studied under microaerophilic conditions. For that, we compared bioreactors treating oleate-based wastewater (organic loading rates of 1 and 3 kg COD m-3 d-1), operated under different redox conditions (strictly anaerobic-AnR, -350 mV; microaerophilic-MaR, -250 mV). At the higher load, palmitate accumulated 7 times more in the MaR, where facultative anaerobes were more abundant, and only the biomass from this reactor could recover the methanogenic activity after a transient inhibition. In a second experiment, the abundance of facultative anaerobic bacteria, particularly Pseudomonas spp. (from which two strains were isolated), was strongly correlated (p<0.05) with palmitate-to-total LCFA percentage in the biofilm formed in a continuous plug flow reactor fed with very high loads of oleate. This work strongly suggests that micro-aeration stimulates the development of facultative bacteria that are critical for achieving LCFA conversion to methane in continuous bioreactors. Microbial networks and interactions of facultative and strict anaerobes in microbial communities should be considered in future studies.

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

Stapleton, J.

Apple pomace, the solid residue from juice production, is a solid waste problem in the Hudson Valley. This study investigates possibilities for converting it to a resource. The characteristics of the region's apple growing and processing industries are examined at length, including their potential for converting waste biomass. The properties of apple pomace are described. From interviews with Hudson Valley apple processors the following information is presented: quantities of pomace produced; seasonality of production; disposal procedures, costs, and revenues; trends in juice production; and attitudes toward alternatives. Literature research resulted in a list of more than 25 end uses formore » apple pomace of which eight were selected for analysis. Landfilling, landspreading, composting, animal feed, direct burning, gasification, anaerobic digestion (methane generation), and fermentation (ethanol production) were analyzed with regard to technical availability, regulatory and environmental impact, attitudes toward end use, and energetic and economic feasibility (See Table 19). The study recommends (1) a pilot anaerobic digestion plant be set up, (2) the possibility of extracting methane from the Marlborough landfill be investigated, (3) a study of the mid-Hudson waste conversion potential be conducted, and (4) an education program in alternative waste management be carried out for the region's industrial and agricultural managers.« less

Microbial Physiology of the Conversion of Residual Oil to Methane: A Protein Prospective

NASA Astrophysics Data System (ADS)

Morris, Brandon E. L.; Bastida-Lopez, Felipe; von Bergen, Martin; Richnow, Hans-Hermann; Suflita, Joseph M.

2010-05-01

Traditional petroleum recovery techniques are unable to extract the majority of oil in most petroliferous deposits. The recovery of even a fraction of residual hydrocarbon in conventional reserves could represent a substantive energy supply. To this end, the microbial conversion of residual oil to methane has gained increasing relevance in recent years [1,2]. Worldwide demand for methane is expected to increase through 2030 [3], as it is a cleaner-burning alternative to traditional fuels [4]. To investigate the microbial physiology of hydrocarbon-decomposition and ultimate methanogenesis, we initiated a two-pronged approach. First, a model alkane-degrading sulfate-reducing bacterium, Desulfoglaeba alkanexedens, was used to interrogate the predominant metabolic pathway(s) differentially expressed during growth on either n-decane or butyrate. A total of 81 proteins were differentially expressed during bacterial growth on butyrate, while 100 proteins were unique to the alkane-grown condition. Proteins related to alkylsuccinate synthase, or the homologous 1-methyl alkylsuccinate synthase, were identified only in the presence of the hydrocarbon. Secondly, we used a newly developed stable isotope probing technique [5] targeted towards proteins to monitor the flux of carbon through a residual oil-degrading bacterial consortium enriched from a gas-condensate contaminated aquifer [1]. Combined carbon and hydrogen stable isotope fractionation identified acetoclastic methanogenesis as the dominant process in this system. Such findings agree with the previous clone library characterization of the consortium. Furthermore, hydrocarbon activation was determined to be the rate-limiting process during the net conversion of residual oil to methane. References 1. Gieg, L.M., K.E. Duncan, and J.M. Suflita, Bioenegy production via microbial conversion of residual oil to natural gas. Appl Environ Micro, 2008. 74(10): p. 3022-3029. 2. Jones, D.M., et al., Crude-oil biodegradation via methanogenesis in subsurface petroleum reserviors. Nature, 2008. 451: p. 176-180. 3. US-DOE, E.I.A., International Energy Outlook 2009. 2009, United States Department of Energy: Washington D.C. 4. DeLuchi, M.A., Emissions of greenhouse gases from the use of transportation fuels and electricity, US-DoE, Editor. 1991, Center for Transportation Research, Argonne National Laboratory: Chicago, Illinois. 5. Jehmlich, N., et al., Protein-based stable isotope probing (Protein-SIP) reveals active species within anoxic mixed cultures. ISME, 2008. 2: p. 1122-1133.

Enzymes and microorganisms in food industry waste processing and conversion to useful products: a review of the literature

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

Carroad, P.A.; Wilke, C.R.

1976-12-01

Bioconversion of food processing wastes is receiving increased attention with the realization that waste components represent an available and utilizable resource for conversion to useful products. Liquid wastes are characterized as dilute streams containing sugars, starches, proteins, and fats. Solid wastes are generally cellulosic, but may contain other biopolymers. The greatest potential for economic bioconversion is represented by processes to convert cellulose to glucose, glucose to alcohol and protein, starch to invert sugar, and dilute waste streams to methane by anaerobic digestion. Microbial or enzymatic processes to accomplish these conversions are described.

Utilization of coal mine methane for methanol and SCP production. Topical report, May 5, 1995--March 4, 1996

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

NONE

1998-12-31

The feasibility of utilizing a biological process to reduce methane emissions from coal mines and to produce valuable single cell protein (SCP) and/or methanol as a product has been demonstrated. The quantities of coal mine methane from vent gas, gob wells, premining wells and abandoned mines have been determined in order to define the potential for utilizing mine gases as a resource. It is estimated that 300 MMCFD of methane is produced in the United States at a typical concentration of 0.2-0.6 percent in ventilation air. Of this total, almost 20 percent is produced from the four Jim Walter Resourcesmore » (JWR) mines, which are located in very gassy coal seams. Worldwide vent gas production is estimated at 1 BCFD. Gob gas methane production in the U.S. is estimated to be 38 MMCFD. Very little gob gas is produced outside the U.S. In addition, it is estimated that abandoned mines may generate as much as 90 MMCFD of methane. In order to make a significant impact on coal mine methane emissions, technology which is able to utilize dilute vent gases as a resource must be developed. Purification of the methane from the vent gases would be very expensive and impractical. Therefore, the process application must be able to use a dilute methane stream. Biological conversion of this dilute methane (as well as the more concentrated gob gases) to produce single cell protein (SCP) and/or methanol has been demonstrated in the Bioengineering Resources, Inc. (BRI) laboratories. SCP is used as an animal feed supplement, which commands a high price, about $0.11 per pound.« less

Methane Recovery from Animal Manures The Current Opportunities Casebook

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

Lusk, P.

1998-09-22

Growth and concentration of the livestock industry create opportunities for the proper disposal of the large quantities of manures generated at dairy, swine, and poultry farms. Pollutants from unmanaged livestock wastes can degrade the environment, and methane emitted from decomposing manure may contribute to global climate change. One management system not only helps prevent pollution but can also convert a manure problem into a new profit center. Economic evaluations and case studies of operating systems indicate that the anaerobic digestion of livestock manures is a commercially viable conversion technology with considerable potential for providing profitable coproducts, including a cost-effective renewablemore » fuel for livestock production operations. This casebook examines some of the current opportunities for recovering methane from anaerobic digestion animal manures.« less

Effect of Sodium Dodecyl Sulfate Surfactant on Methane Hydrate Formation: A Molecular Dynamics Study.

PubMed

Choudhary, Nilesh; Hande, Vrushali R; Roy, Sudip; Chakrabarty, Suman; Kumar, Rajnish

2018-06-28

In experimental studies, it has been observed that the presence of sodium dodecyl sulfate (SDS) significantly increases the kinetics of hydrate formation and the final water-to-hydrate conversion ratio. In this study, we intend to understand the molecular mechanism behind the effect of SDS on the formation of methane hydrate through molecular dynamics simulation. Hydrate formation conditions similar to that of laboratory experiments were chosen to study hydrate growth kinetics in 1 wt % SDS solution. We also investigate the effect of interactions with isolated SDS molecules on methane hydrate growth. It was observed that the hydrophobic tail part of the SDS molecule favorably interacts with the growing hydrate surface and may occupy the partial hydrate cages while the head groups remain exposed to water.

The use of renewable energy in the form of methane via electrolytic hydrogen generation using carbon dioxide as the feedstock

NASA Astrophysics Data System (ADS)

Hashimoto, Koji; Kumagai, Naokazu; Izumiya, Koichi; Takano, Hiroyuki; Shinomiya, Hiroyuki; Sasaki, Yusuke; Yoshida, Tetsuya; Kato, Zenta

2016-12-01

The history reveals the continuous increase in world energy consumption and carbon emissions. For prevention of intolerable global warming and complete exhaustion of fossil fuels we need complete conversion from fossil fuel consumption to renewable energy. We have been performing the research and development of global carbon dioxide recycling for more than 25 years to supply renewable energy to the world in the form of methane produced by the reaction of carbon dioxide captured from chimney with hydrogen generated electrolytically using electricity generated by renewable energy. We created the cathode and anode for electrolytic hydrogen generation and the catalyst for carbon dioxide methanation by the reaction with hydrogen. The methane formation from renewable energy will be the most convenient and efficient key technology for the use of renewable energy by storage of intermittent and fluctuating electricity generated from renewable energy and by regeneration of stable electricity. Domestic and international cooperation of companies for industrialization is in progress.

Enhancing ethanol production from thermophilic and mesophilic solid digestate using ozone combined with aqueous ammonia pretreatment.

PubMed

Wang, Dianlong; Xi, Jiang; Ai, Ping; Yu, Liang; Zhai, Hong; Yan, Shuiping; Zhang, Yanlin

2016-05-01

Pretreatment with ozone combined with aqueous ammonia was used to recover residual organic carbon from recalcitrant solid digestate for ethanol production after anaerobic digestion (AD) of rice straw. Methane yield of AD at mesophilic and thermophilic conditions, and ethanol production of solid digestate were investigated. The results showed that the methane yield at thermophilic temperature was 72.2% higher than that at mesophilic temperature under the same conditions of 24days and 17% solid concentration. And also the ethanol production efficiency of solid digestate after thermophilic process was 24.3% higher than that of solid digestate after mesophilic process. In this study, the optimal conditions for integrated methane and ethanol processes were determined as 55°C, 17% solid concentration and 24days. 58.6% of glucose conversion, 142.8g/kg of methane yield and 65.2g/kg of ethanol yield were achieved, and the highest net energy balance was calculated as 6416kJ/kg. Copyright © 2016 Elsevier Ltd. All rights reserved.

Enhanced methane yield by co-digestion of sewage sludge with micro-algae and catering waste leachate.

PubMed

2018-04-04

The co-digestion of different wastes is a promising concept to improve methane generation during anaerobic process. However, the anaerobic co-digestion of catering waste leachate with algal biomass and sewage sludge has not been studied to date. This work investigated the methane generation by the anaerobic co-digestion of different mixtures of catering waste leachate, micro-algal biomass, and sewage sludge. Co-digestion of waste mixture containing equal ratios of three substrates had 39.31% higher methane yield than anaerobic digestion of raw sludge. This was possibly due to a proliferation of methanogens during the co-digestion period induced by multi-phase digestion of different wastes with different degrees of digestibility. Therefore, co-digestion of catering waste leachate, micro-algal biomass, and sewage sludge appears to be an efficient technology for energy conversion from waste resources. The scientific application of this co-digestion technology with these three substrates may play a role in solving important environmental issues of waste management.

Methane utilization in Methylomicrobium alcaliphilum 20ZR: a systems approach.

PubMed

Akberdin, Ilya R; Thompson, Merlin; Hamilton, Richard; Desai, Nalini; Alexander, Danny; Henard, Calvin A; Guarnieri, Michael T; Kalyuzhnaya, Marina G

2018-02-06

Biological methane utilization, one of the main sinks of the greenhouse gas in nature, represents an attractive platform for production of fuels and value-added chemicals. Despite the progress made in our understanding of the individual parts of methane utilization, our knowledge of how the whole-cell metabolic network is organized and coordinated is limited. Attractive growth and methane-conversion rates, a complete and expert-annotated genome sequence, as well as large enzymatic, 13 C-labeling, and transcriptomic datasets make Methylomicrobium alcaliphilum 20Z R an exceptional model system for investigating methane utilization networks. Here we present a comprehensive metabolic framework of methane and methanol utilization in M. alcaliphilum 20Z R . A set of novel metabolic reactions governing carbon distribution across central pathways in methanotrophic bacteria was predicted by in-silico simulations and confirmed by global non-targeted metabolomics and enzymatic evidences. Our data highlight the importance of substitution of ATP-linked steps with PPi-dependent reactions and support the presence of a carbon shunt from acetyl-CoA to the pentose-phosphate pathway and highly branched TCA cycle. The diverged TCA reactions promote balance between anabolic reactions and redox demands. The computational framework of C 1 -metabolism in methanotrophic bacteria can represent an efficient tool for metabolic engineering or ecosystem modeling.

Methane production and hydrolysis kinetics in the anaerobic degradation of wastewater screenings.

PubMed

Cadavid-Rodríguez, L S; Horan, N

2013-01-01

Anaerobic biodegradability and hydrolysis rates of wastewater screenings were determined using the biochemical methane potential test at 37 °C. The extent and rate of screenings conversion to methane of this complex and particulate substrate were investigated and since two stages of hydrolysis were identified, corresponding to the different types of materials in screenings, a linear and non-linear model was used. No accumulation of intermediary products was observed and so it was possible to use the methane production rate and a linear model to estimate the hydrolysis rate in the first phase of hydrolysis. The measured values of 0.061-0.127 d(-1) are in the range reported for other comparable organic wastes. It was also observed that the inoculum-to-substrate ratio has a large impact on methane production rate of screenings. The difference in biodegradation rates from the materials in screenings and the overall hydrolysis could be represented by the modified Gompertz non-linear model which was able to describe the methane production rate of screenings with a high confidence. Screenings were found to have 52% biodegradability on average and this shows the potential for volatile solids destruction. A two-stage process with an improved hydrolysis rate is proposed to ensure that the full potential of the material is exploited.

Methane oxidation at a surface-sealed boreal landfill.

PubMed

Einola, Juha; Sormunen, Kai; Lensu, Anssi; Leiskallio, Antti; Ettala, Matti; Rintala, Jukka

2009-07-01

Methane oxidation was studied at a closed boreal landfill (area 3.9 ha, amount of deposited waste 200,000 tonnes) equipped with a passive gas collection and distribution system and a methane oxidative top soil cover integrated in a European Union landfill directive-compliant, multilayer final cover. Gas wells and distribution pipes with valves were installed to direct landfill gas through the water impermeable layer into the top soil cover. Mean methane emissions at the 25 measuring points at four measurement times (October 2005-June 2006) were 0.86-6.2 m(3) ha(-1) h(-1). Conservative estimates indicated that at least 25% of the methane flux entering the soil cover at the measuring points was oxidized in October and February, and at least 46% in June. At each measurement time, 1-3 points showed significantly higher methane fluxes into the soil cover (20-135 m(3) ha(-1) h(-1)) and methane emissions (6-135 m(3) ha(-1) h(-1)) compared to the other points (< 20 m(3) ha(-1) h(-1) and < 10 m(3) ha(-1) h(-1), respectively). These points of methane overload had a high impact on the mean methane oxidation at the measuring points, resulting in zero mean oxidation at one measurement time (November). However, it was found that by adjusting the valves in the gas distribution pipes the occurrence of methane overload can be to some extent moderated which may increase methane oxidation. Overall, the investigated landfill gas treatment concept may be a feasible option for reducing methane emissions at landfills where a water impermeable cover system is used.

Effects of Land-Use Conversion from Double Rice Cropping to Vegetables on Methane and Nitrous Oxide Fluxes in Southern China

PubMed Central

Yuan, Ye; Dai, Xiaoqin; Wang, Huimin; Xu, Ming; Fu, Xiaoli; Yang, Fengting

2016-01-01

Compared with CO2, methane (CH4) and nitrous oxide (N2O) are potent greenhouse gases in terms of their global warming potentials. Previous studies have indicated that land-use conversion has a significant impact on greenhouse gas emissions. However, little is known regarding the impact of converting rice (Oryza sativa L.) to vegetable fields, an increasing trend in land-use change in southern China, on CH4 and N2O fluxes. The effects of converting double rice cropping to vegetables on CH4 and N2O fluxes were examined using a static chamber method in southern China from July 2012 to July 2013. The results indicate that CH4 fluxes could reach 31.6 mg C m−2 h−1 under rice before land conversion. The cumulative CH4 emissions for fertilized and unfertilized rice were 348.9 and 321.0 kg C ha−1 yr−1, respectively. After the land conversion, the cumulative CH4 emissions were −0.4 and 1.4 kg C ha−1 yr−1 for the fertilized and unfertilized vegetable fields, respectively. Similarly, the cumulative N2O fluxes under rice were 1.27 and 0.56 kg N ha−1 yr−1 for the fertilized and unfertilized treatments before the land conversion and 19.2 and 8.5 kg N ha−1 yr−1, respectively, after the land conversion. By combining the global warming potentials (GWPs) of both gases, the overall land-use conversion effect was minor (P = 0.36) with fertilization, but the conversion reduced GWP by 63% when rice and vegetables were not fertilized. Increase in CH4 emissions increased GWP under rice compared with vegetables with non-fertilization, but increased N2O emissions compensated for similar GWPs with fertilization under rice and vegetables. PMID:27195497

Effects of Land-Use Conversion from Double Rice Cropping to Vegetables on Methane and Nitrous Oxide Fluxes in Southern China.

PubMed

Yuan, Ye; Dai, Xiaoqin; Wang, Huimin; Xu, Ming; Fu, Xiaoli; Yang, Fengting

2016-01-01

Compared with CO2, methane (CH4) and nitrous oxide (N2O) are potent greenhouse gases in terms of their global warming potentials. Previous studies have indicated that land-use conversion has a significant impact on greenhouse gas emissions. However, little is known regarding the impact of converting rice (Oryza sativa L.) to vegetable fields, an increasing trend in land-use change in southern China, on CH4 and N2O fluxes. The effects of converting double rice cropping to vegetables on CH4 and N2O fluxes were examined using a static chamber method in southern China from July 2012 to July 2013. The results indicate that CH4 fluxes could reach 31.6 mg C m-2 h-1 under rice before land conversion. The cumulative CH4 emissions for fertilized and unfertilized rice were 348.9 and 321.0 kg C ha-1 yr-1, respectively. After the land conversion, the cumulative CH4 emissions were -0.4 and 1.4 kg C ha-1 yr-1 for the fertilized and unfertilized vegetable fields, respectively. Similarly, the cumulative N2O fluxes under rice were 1.27 and 0.56 kg N ha-1 yr-1 for the fertilized and unfertilized treatments before the land conversion and 19.2 and 8.5 kg N ha-1 yr-1, respectively, after the land conversion. By combining the global warming potentials (GWPs) of both gases, the overall land-use conversion effect was minor (P = 0.36) with fertilization, but the conversion reduced GWP by 63% when rice and vegetables were not fertilized. Increase in CH4 emissions increased GWP under rice compared with vegetables with non-fertilization, but increased N2O emissions compensated for similar GWPs with fertilization under rice and vegetables.

Method for removal of methane from coalbeds

DOEpatents

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.

40 CFR 98.356 - Data reporting requirements.

Code of Federal Regulations, 2014 CFR

2014-07-01

...) Maximum CH4 production potential (B0) used as an input to Equation II-1 or II-2 of this subpart, from Table II-1 to this subpart. (4) Methane conversion factor (MCF) used as an input to Equation II-1 or II...

40 CFR 98.356 - Data reporting requirements.

Code of Federal Regulations, 2011 CFR

2011-07-01

...) Maximum CH4 production potential (B0) used as an input to Equation II-1 or II-2 of this subpart. (4) Methane conversion factor (MCF) used as an input to Equation II-1 or II-2 of this subpart. (5) Annual mass...

40 CFR 98.356 - Data reporting requirements.

Code of Federal Regulations, 2012 CFR

2012-07-01

...) Maximum CH4 production potential (B0) used as an input to Equation II-1 or II-2 of this subpart, from Table II-1 to this subpart. (4) Methane conversion factor (MCF) used as an input to Equation II-1 or II...

40 CFR 98.356 - Data reporting requirements.

Code of Federal Regulations, 2013 CFR

2013-07-01

...) Maximum CH4 production potential (B0) used as an input to Equation II-1 or II-2 of this subpart, from Table II-1 to this subpart. (4) Methane conversion factor (MCF) used as an input to Equation II-1 or II...

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

PubMed Central

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

2017-01-01

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

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

PubMed

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

2017-01-01

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

Review on dry reforming of methane, a potentially more environmentally-friendly approach to the increasing natural gas exploitation

PubMed Central

Lavoie, Jean-Michel

2014-01-01

With the actual growth of the natural gas industry in the US as well as the potential and availability of this non-renewable carbon source worldwide, reforming of methane gas is getting increasing attention. Methane can be used for the production of heat or electricity, as well, it can be converted to syngas, a building block that could lead to the production of liquid fuels and chemicals, a very promising pathway in light of the increasing price of oil. Amongst the different reforming techniques, dry reforming could represent a very interesting approach both to valorize a cheap source or carbon (CO2) as well as to reduce the overall carbon footprint of the increasing worldwide fossil-based methane consumption. In this short review, attention will be given to the thermodynamics of dry reforming followed by an investigation on dry reforming using heterogeneous catalyst by focusing on the most popular elements used in literature for dry reforming. Attention will as well be given to other emerging techniques that may allow countering at one point the high thermodynamic penalties that accompanies conversion of methane using carbon dioxide. PMID:25426488

Thermochemical Pretreatment for Anaerobic Digestion of Sorted Waste

NASA Astrophysics Data System (ADS)

Hao, W.; Hongtao, W.

2008-02-01

The effect of alkaline hydrothermal pre-treatment for anaerobic digestion of mechanically-sorted municipal solid waste (MSW) and source-sorted waste was studied. Waste was hydrothermally pre-treated in dilute alkali solution. Hydrolysis product was incubated in 500 ml saline bottle to determine methane potential (MP) under mesospheric anaerobic conditions. Optimum reaction condition obtained in the study is 170 °C at the dose of 4 g NaOH/100 g solid for one hour. Soluble COD was 13936 mg/L and methane yield was 164 ml/g VS for 6 days incubation at optimum conditions. More than 50% biogas increase was achieved over the control, and methane conversion ratio on carbon basis was enhanced to 30.6%. The digestion period was less than 6 days when pre-treatment temperature was above 130 °C. The organic part of sorted waste is mainly constituted of kitchen garbage and leaf. Model kitchen garbage was completely liquidized at 130 °C for one hour and the methane yield was 276 ml/g VS. Addition of alkali enhance hydroxylation rate and methane yield slightly. The biogas potential of leaf could be observed by pre-treatment above 150 °C under alkaline condition.

Dry Reforming of Methane in a Gliding Arc Plasmatron: Towards a Better Understanding of the Plasma Chemistry.

PubMed

Cleiren, Emelie; Heijkers, Stijn; Ramakers, Marleen; Bogaerts, Annemie

2017-10-23

Dry reforming of methane (DRM) in a gliding arc plasmatron is studied for different CH 4 fractions in the mixture. The CO 2 and CH 4 conversions reach their highest values of approximately 18 and 10 %, respectively, at 25 % CH 4 in the gas mixture, corresponding to an overall energy cost of 10 kJ L -1 (or 2.5 eV per molecule) and an energy efficiency of 66 %. CO and H 2 are the major products, with the formation of smaller fractions of C 2 H x (x=2, 4, or 6) compounds and H 2 O. A chemical kinetics model is used to investigate the underlying chemical processes. The calculated CO 2 and CH 4 conversion and the energy efficiency are in good agreement with the experimental data. The model calculations reveal that the reaction of CO 2 (mainly at vibrationally excited levels) with H radicals is mainly responsible for the CO 2 conversion, especially at higher CH 4 fractions in the mixture, which explains why the CO 2 conversion increases with increasing CH 4 fraction. The main process responsible for CH 4 conversion is the reaction with OH radicals. The excellent energy efficiency can be explained by the non-equilibrium character of the plasma, in which the electrons mainly activate the gas molecules, and by the important role of the vibrational kinetics of CO 2 . The results demonstrate that a gliding arc plasmatron is very promising for DRM. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Dry reforming of methane via plasma-catalysis: influence of the catalyst nature supported on alumina in a packed-bed DBD configuration

NASA Astrophysics Data System (ADS)

Brune, L.; Ozkan, A.; Genty, E.; Visart de Bocarmé, T.; Reniers, F.

2018-06-01

These days, the consideration of CO2 as a feedstock has become the subject of more interest. The reutilization of CO2 is already possible via cold plasma techniques operating at atmospheric pressure. A promising technology is the dielectric barrier discharge (DBD). In most cases DBDs exhibit a low energy efficiency for CO2 conversion. However, several routes can be used to increase this efficiency and hence, the product formation. One of these routes is the packed-bed DBD configuration with porous beads inside the gap of the DBD, which also allows the coupling of plasma with catalysis. Catalysts can be introduced in such a configuration to exploit the synergistic effect between plasma and catalytically active surfaces, leading to a more efficient process. In this article, the dry reforming of methane (DRM) is studied, which aims to convert both CO2 and CH4, another greenhouse gas, at the same time. The conversions and energy costs of the DRM process are investigated and compared in both the packed-bed DBD configurations containing catalysts (Co, Cu or Ni) and the classical DBD. The change in filamentary behavior is studied in detail and correlated with the obtained conversions using gas chromatography, mass spectrometry and using an oscilloscope. A characterization of the catalysts on the beads is also carried out. Both the CO2 and CH4 conversions are clearly increased with the plasma-catalysis. Moreover, CH4 conversions as high as 90% can be obtained in certain conditions with copper catalysts.

Porous Silica Sol-Gel Glasses Containing Reactive V2O5 Groups

NASA Technical Reports Server (NTRS)

Stiegman, Albert E.

1995-01-01

Porous silica sol-gel glasses into which reactive vanadium oxide functional groups incorporated exhibit number of unique characteristics. Because they bind molecules of some species both reversibly and selectively, useful as chemical sensors or indicators or as scrubbers to remove toxic or hazardous contaminants. Materials also oxidize methane gas photochemically: suggests they're useful as catalysts for conversion of methane to alcohol and for oxidation of hydrocarbons in general. By incorporating various amounts of other metals into silica sol-gel glasses, possible to synthesize new materials with broad range of new characteristics.

Study on potency of municipal solid waste conversion into renewable energy by thermal incineration and bioconversion: case study of Medan city

NASA Astrophysics Data System (ADS)

Sarah, Maya; Misran, Erni

2018-03-01

Municipal solid waste (MSW) in Medan City is facing problems either with the quantity and management of MSW. Local authority only dumped approximately 73.9% MSW in the landfill over the years. Spontaneous phenomena of methane formation in dumping site indicates the potency of MSW conversion into energy by biochemical conversion. On the contrary, the presence of plastics, woods, papers, etc. in the MSW show the potency of MSW to be treated by thermal conversion. Both thermal incineration and anaerobic digestion may convert MSW Medan City into energy. This study evaluates potency of MSW conversion into renewable energy using proximate and ultimate analysis. Overall, MSW of Medan City has the opportunities to be converted into energy by both thermal and biochemical conversion with a special requirement such as pre-dry the MSW prior incineration process and degrade organic MSW in a bioreactor.

Granular Carbon-Based Electrodes as Cathodes in Methane-Producing Bioelectrochemical Systems

PubMed Central

Liu, Dandan; Roca-Puigros, Marta; Geppert, Florian; Caizán-Juanarena, Leire; Na Ayudthaya, Susakul P.; Buisman, Cees; ter Heijne, Annemiek

2018-01-01

Methane-producing bioelectrochemical systems generate methane by using microorganisms to reduce carbon dioxide at the cathode with external electricity supply. This technology provides an innovative approach for renewable electricity conversion and storage. Two key factors that need further attention are production of methane at high rate, and stable performance under intermittent electricity supply. To study these key factors, we have used two electrode materials: granular activated carbon (GAC) and graphite granules (GG). Under galvanostatic control, the biocathodes achieved methane production rates of around 65 L CH4/m2catproj/d at 35 A/m2catproj, which is 3.8 times higher than reported so far. We also operated all biocathodes with intermittent current supply (time-ON/time-OFF: 4–2′, 3–3′, 2–4′). Current-to-methane efficiencies of all biocathodes were stable around 60% at 10 A/m2catproj and slightly decreased with increasing OFF time at 35 A/m2catproj, but original performance of all biocathodes was recovered soon after intermittent operation. Interestingly, the GAC biocathodes had a lower overpotential than the GG biocathodes, with methane generation occurring at −0.52 V vs. Ag/AgCl for GAC and at −0.92 V for GG at a current density of 10 A/m2catproj. 16S rRNA gene analysis showed that Methanobacterium was the dominant methanogen and that the GAC biocathodes experienced a higher abundance of proteobacteria than the GG biocathodes. Both cathode materials show promise for the practical application of methane-producing BESs. PMID:29946543

Methane production by anaerobic digestion of Bermuda grass

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

Klass, D.L.; Ghosh, S.

1981-01-01

Bermuda grass (Cynodon dactylon) is one of the high-yield warm-season grasses that has been suggested as a promising raw material for conversion to methane. Experimental work performed with laboratory digesters to study the anaerobic digestion of Coastal Bermuda grass harvested in Louisiana and having a C/N ratio of 24 is described. Methane yields of about 1.9 SCF/lb of volatile solids (VS) added were observed under conventional mesophilic high-rate conditions. When supplemental nitrogen additions were made, the methane yields increased. This observation along with the compositional data compiled on the grass used in this work indicated that the nitrogen content ofmore » the unsupplemented grass was insufficient to sustain high-rate digestion at the higher yield level. However, as the C/N ratio was reduced by addition of ammonium chloride, the methane yield continually increased up to 3.5 SCF/lb added at the lowest C/N ratio examined (6.3) even after relatively high concentrations of ammonium nitrogen were measured in the effluent. It appears that the added nutrient had a stimulatory effect on methane production above the point where nitrogen was not limiting. Thermophilic digestion with supplemental nitrogen additions afforded methane yields of about 2.7 SCF/lb VS added. Carbon and energy balances were calculated and the relative biodegradabilities of the organics were estimated. It was concluded from this work that Coastal Bermuda grass can be converted to high-methane gas under conventional anaerobic digestion conditions. The performance of the particular lot of grass studied was substantially improved by supplemental nitrogen additions. (Refs. 12).« less

Fast start-up reactor for partial oxidation of methane with electrically-heated metallic monolith catalyst

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.

Visible-light-driven methane formation from CO2 with a molecular iron catalyst.

PubMed

Rao, Heng; Schmidt, Luciana C; Bonin, Julien; Robert, Marc

2017-08-03

Converting CO 2 into fuel or chemical feedstock compounds could in principle reduce fossil fuel consumption and climate-changing CO 2 emissions. One strategy aims for electrochemical conversions powered by electricity from renewable sources, but photochemical approaches driven by sunlight are also conceivable. A considerable challenge in both approaches is the development of efficient and selective catalysts, ideally based on cheap and Earth-abundant elements rather than expensive precious metals. Of the molecular photo- and electrocatalysts reported, only a few catalysts are stable and selective for CO 2 reduction; moreover, these catalysts produce primarily CO or HCOOH, and catalysts capable of generating even low to moderate yields of highly reduced hydrocarbons remain rare. Here we show that an iron tetraphenylporphyrin complex functionalized with trimethylammonio groups, which is the most efficient and selective molecular electro- catalyst for converting CO 2 to CO known, can also catalyse the eight-electron reduction of CO 2 to methane upon visible light irradiation at ambient temperature and pressure. We find that the catalytic system, operated in an acetonitrile solution containing a photosensitizer and sacrificial electron donor, operates stably over several days. CO is the main product of the direct CO 2 photoreduction reaction, but a two-pot procedure that first reduces CO 2 and then reduces CO generates methane with a selectivity of up to 82 per cent and a quantum yield (light-to-product efficiency) of 0.18 per cent. However, we anticipate that the operating principles of our system may aid the development of other molecular catalysts for the production of solar fuels from CO 2 under mild conditions.

Visible-light-driven methane formation from CO2 with a molecular iron catalyst

NASA Astrophysics Data System (ADS)

Rao, Heng; Schmidt, Luciana C.; Bonin, Julien; Robert, Marc

2017-08-01

Converting CO2 into fuel or chemical feedstock compounds could in principle reduce fossil fuel consumption and climate-changing CO2 emissions. One strategy aims for electrochemical conversions powered by electricity from renewable sources, but photochemical approaches driven by sunlight are also conceivable. A considerable challenge in both approaches is the development of efficient and selective catalysts, ideally based on cheap and Earth-abundant elements rather than expensive precious metals. Of the molecular photo- and electrocatalysts reported, only a few catalysts are stable and selective for CO2 reduction; moreover, these catalysts produce primarily CO or HCOOH, and catalysts capable of generating even low to moderate yields of highly reduced hydrocarbons remain rare. Here we show that an iron tetraphenylporphyrin complex functionalized with trimethylammonio groups, which is the most efficient and selective molecular electro- catalyst for converting CO2 to CO known, can also catalyse the eight-electron reduction of CO2 to methane upon visible light irradiation at ambient temperature and pressure. We find that the catalytic system, operated in an acetonitrile solution containing a photosensitizer and sacrificial electron donor, operates stably over several days. CO is the main product of the direct CO2 photoreduction reaction, but a two-pot procedure that first reduces CO2 and then reduces CO generates methane with a selectivity of up to 82 per cent and a quantum yield (light-to-product efficiency) of 0.18 per cent. However, we anticipate that the operating principles of our system may aid the development of other molecular catalysts for the production of solar fuels from CO2 under mild conditions.

Methane Production by Microbial Mats Under Low Sulfate Concentrations

NASA Technical Reports Server (NTRS)

Bebout, Brad M.; Hoehler, Tori M.; Thamdrup, Bo; Albert, Dan; Carpenter, Steven P.; Hogan, Mary; Turk, Kendra; DesMarais, David J.

2003-01-01

Cyanobacterial mats collected in hypersaline salterns were incubated in a greenhouse under low sulfate concentrations ([SO4]) and examined for their primary productivity and emissions of methane and other major carbon species. Atmospheric greenhouse warming by gases such as carbon dioxide and methane must have been greater during the Archean than today in order to account for a record of moderate to warm paleoclemates, despite a less luminous early sun. It has been suggested that decreased levels of oxygen and sulfate in Archean oceans could have significantly stimulated microbial methanogenesis relative to present marine rates, with a resultant increase in the relative importance of methane in maintaining the early greenhouse. We maintained modern microbial mats, models of ancient coastal marine communities, in artificial brine mixtures containing both modern [SO4=] (ca. 70 mM) and "Archean" [SO4] (less than 0.2 mM). At low [SO4], primary production in the mats was essentially unaffected, while rates of sulfate reduction decreased by a factor of three, and methane fluxes increased by up to ten-fold. However, remineralization by methanogenesis still amounted to less than 0.4 % of the total carbon released by the mats. The relatively low efficiency of conversion of photosynthate to methane is suggested to reflect the particular geometry and chemical microenvironment of hypersaline cyanobacterial mats. Therefore, such mats w-ere probably relatively weak net sources of methane throughout their 3.5 Ga history, even during periods of low- environmental levels oxygen and sulfate.

Experimental comparison of MCFC performance using three different biogas types and methane

NASA Astrophysics Data System (ADS)

Bove, Roberto; Lunghi, Piero

Biogas recovery is an environmentally friendly and cost-effective practice that is getting consensus in both the scientific and industrial community, as the growing number of projects demonstrate. The use of fuel cells as energy conversion systems increases the conversion efficiency, as well as the environmental benefits. Molten carbonate fuel cells (MCFC) operate at a temperature of about 650 °C, thus presenting a high fuel flexibility, compared to low temperature fuel cells. Aim of the present study is to compare the performance of an MCFC single cell, fuelled with different biogas types as well as methane. The biogases considered are derived from the following processes: (1) steam gasification in an entrained flow gasifier; (2) steam gasification in a duel interconnect fluidized bed gasifier; (3) biogas from an anaerobic digestion process. The performances are evaluated for different fuel utilization and current densities. The results are an essential starting point for a complete system design and demonstration.

Combined Ceria Reduction and Methane Reforming in a Solar-Driven Particle-Transport Reactor.

PubMed

Welte, Michael; Warren, Kent; Scheffe, Jonathan R; Steinfeld, Aldo

2017-09-20

We report on the experimental performance of a solar aerosol reactor for carrying out the combined thermochemical reduction of CeO 2 and reforming of CH 4 using concentrated radiation as the source of process heat. The 2 kW th solar reactor prototype utilizes a cavity receiver enclosing a vertical Al 2 O 3 tube which contains a downward gravity-driven particle flow of ceria particles, either co-current or counter-current to a CH 4 flow. Experimentation under a peak radiative flux of 2264 suns yielded methane conversions up to 89% at 1300 °C for residence times under 1 s. The maximum extent of ceria reduction, given by the nonstoichiometry δ (CeO 2-δ ), was 0.25. The solar-to-fuel energy conversion efficiency reached 12%. The syngas produced had a H 2 :CO molar ratio of 2, and its calorific value was solar-upgraded by 24% over that of the CH 4 reformed.

Combined Ceria Reduction and Methane Reforming in a Solar-Driven Particle-Transport Reactor

PubMed Central

2017-01-01

We report on the experimental performance of a solar aerosol reactor for carrying out the combined thermochemical reduction of CeO2 and reforming of CH4 using concentrated radiation as the source of process heat. The 2 kWth solar reactor prototype utilizes a cavity receiver enclosing a vertical Al2O3 tube which contains a downward gravity-driven particle flow of ceria particles, either co-current or counter-current to a CH4 flow. Experimentation under a peak radiative flux of 2264 suns yielded methane conversions up to 89% at 1300 °C for residence times under 1 s. The maximum extent of ceria reduction, given by the nonstoichiometry δ (CeO2−δ), was 0.25. The solar-to-fuel energy conversion efficiency reached 12%. The syngas produced had a H2:CO molar ratio of 2, and its calorific value was solar-upgraded by 24% over that of the CH4 reformed. PMID:28966440

Numerical simulations to assess the tracer dilution method for measurement of landfill methane emissions.

PubMed

Taylor, Diane M; Chow, Fotini K; Delkash, Madjid; Imhoff, Paul T

2016-10-01

Landfills are a significant contributor to anthropogenic methane emissions, but measuring these emissions can be challenging. This work uses numerical simulations to assess the accuracy of the tracer dilution method, which is used to estimate landfill emissions. Atmospheric dispersion simulations with the Weather Research and Forecast model (WRF) are run over Sandtown Landfill in Delaware, USA, using observation data to validate the meteorological model output. A steady landfill methane emissions rate is used in the model, and methane and tracer gas concentrations are collected along various transects downwind from the landfill for use in the tracer dilution method. The calculated methane emissions are compared to the methane emissions rate used in the model to find the percent error of the tracer dilution method for each simulation. The roles of different factors are examined: measurement distance from the landfill, transect angle relative to the wind direction, speed of the transect vehicle, tracer placement relative to the hot spot of methane emissions, complexity of topography, and wind direction. Results show that percent error generally decreases with distance from the landfill, where the tracer and methane plumes become well mixed. Tracer placement has the largest effect on percent error, and topography and wind direction both have significant effects, with measurement errors ranging from -12% to 42% over all simulations. Transect angle and transect speed have small to negligible effects on the accuracy of the tracer dilution method. These tracer dilution method simulations provide insight into measurement errors that might occur in the field, enhance understanding of the method's limitations, and aid interpretation of field data. Copyright © 2016 Elsevier Ltd. All rights reserved.

How much do direct livestock emissions actually contribute to global warming?

PubMed

Reisinger, Andy; Clark, Harry

2018-04-01

Agriculture directly contributes about 10%-12% of current global anthropogenic greenhouse gas emissions, mostly from livestock. However, such percentage estimates are based on global warming potentials (GWPs), which do not measure the actual warming caused by emissions and ignore the fact that methane does not accumulate in the atmosphere in the same way as CO 2 . Here, we employ a simple carbon cycle-climate model, historical estimates and future projections of livestock emissions to infer the fraction of actual warming that is attributable to direct livestock non-CO 2 emissions now and in future, and to CO 2 from pasture conversions, without relying on GWPs. We find that direct livestock non-CO 2 emissions caused about 19% of the total modelled warming of 0.81°C from all anthropogenic sources in 2010. CO 2 from pasture conversions contributed at least another 0.03°C, bringing the warming directly attributable to livestock to 23% of the total warming in 2010. The significance of direct livestock emissions to future warming depends strongly on global actions to reduce emissions from other sectors. Direct non-CO 2 livestock emissions would contribute only about 5% of the warming in 2100 if emissions from other sectors increase unabated, but could constitute as much as 18% (0.27°C) of the warming in 2100 if global CO 2 emissions from other sectors are reduced to near or below zero by 2100, consistent with the goal of limiting warming to well below 2°C. These estimates constitute a lower bound since indirect emissions linked to livestock feed production and supply chains were not included. Our estimates demonstrate that expanding the mitigation potential and realizing substantial reductions of direct livestock non-CO 2 emissions through demand and supply side measures can make an important contribution to achieve the stringent mitigation goals set out in the Paris Agreement, including by increasing the carbon budget consistent with the 1.5°C goal. © 2017 John Wiley & Sons Ltd.

Renewable energy: energy from agricultural products

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

Not Available

1984-06-01

This study discusses major issues concerning fuels derived from agricultural products. Agricultural products, particularly sugarcane and corn, are currently meeting major energy needs in Florida. Recent figures indicate that about 10% of the gasoline sold in Florida is ethanol enriched. This gasohol contains a 10% mix of ethanol, which is generally produced from corn or sugarcane molasses. Sugarcane residues (bagasse) also supply most of the fuel to power Florida's large sugar processing industry. These products have the potential to play an expanded role in Florida's energy future. Principle areas of interest are: Growing crops such as napier grass or harvestingmore » water hyacinths to produce methane that can be substituted for natural gas; expanded use of sugar, starch, and industrial and agricultural wastes as raw materials for ethanol production; improved efficiency in conversion processes such as anaerobic digestion and fermentation. The Institute of Food and Agricultural Sciences at the University of Florida plays a leading national role in energy crops research, while Walt Disney World is using a demonstration project to convert water hyacinths into methane. Increased use of fuels produced from agricultural products depends largely on their costs compared to other fuels. Ethanol is currently attractive because of federal and state tax incentives. The growth potential of ethanol and methane is enhanced by the ease with which they can be blended with fossil fuels and thereby utilize the current energy distribution system. Neither ethanol nor methane appear able to compete in the free market for mass distribution at present, although studies indicate that genetic engineering and more efficient conversion processes may lower prices to cost effective levels. These fuels will be most cost effective in cases where waste products are utilized and the fuel is used close to the site of production.« less

Renewable energy: energy from agricultural products

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

Not Available

1984-06-01

This report discusses the major issues concerning fuels derived from agricultural products. Agricultural products, particularly sugarcane and corn, are currently meeting major energy needs in Florida. Recent figures indicate that about 10 percent of the gasoline sold in Florida is ethanol enriched. This gasohol contains a 10 percent mix of ethanol, which is generally produced from corn or sugarcane molasses. Sugarcane residues (bagasse) also supply most of the fuel to power Florida's large sugar processing industry. These products have the potential to play an expanded role in Florida's energy future. Principle areas of interest are: growing crops such as napiermore » grass or harvesting water hyacinths to produce methane that can be substituted for natural gas; expanded use of sugar, starch, and industrial and agricultural wastes as raw materials for ethanol production; and improved efficiency in conversion processes such as anaerobic digestion and fermentation. The Institute of Food and Agricultural Sciences at the University of Florida plays a leading national role in energy crops research, while Walt Disney World is using a demonstration project to convert water hyacinths into methane. Increased use of fuels produced from agricultural products depends largely on their costs compared to other fuels. Ethanol is currently attractive because of federal and state tax incentives. The growth potential of ethanol and methane is enhanced by the ease with which they can be blended with fossil fuels and thereby utilize the current energy distribution system. Neither ethanol nor methane appear able to compete in the free market for mass distribution at present, although studies indicate that genetic engineering and more efficient conversion processes may lower prices to cost effective levels. These fuels will be most cost effective in cases where waste products are utilized and the fuel is used close to the site of production.« less

Low-temperature superacid catalysis: Reactions of n - butane and propane catalyzed by iron- and manganese-promoted sulfated zirconia

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

Tsz-Keung, Cheung; d`Itri, J.L.; Lange, F.C.

1995-12-31

The primary goal of this project is to evaluate the potential value of solid superacid catalysts of the sulfated zirconia type for light hydrocarbon conversion. The key experiments catalytic testing of the performance of such catalysts in a flow reactor fed with streams containing, for example, n-butane or propane. Fe- and Mn-promoted sulfated zirconia was used to catalyze the conversion of n-butane at atmospheric pressure, 225-450{degrees}C, and n-butane partial pressures in the range of 0.0025-0.01 atm. At temperatures <225{degrees}C, these reactions were accompanied by cracking; at temperatures >350{degrees}C, cracking and isomerization occurred. Catalyst deactivation, resulting at least in part frommore » coke formation, was rapid. The primary cracking products were methane, ethane, ethylene, and propylene. The observation of these products along with an ethane/ethylene molar ratio of nearly 1 at 450{degrees}C is consistent with cracking occurring, at least in part, by the Haag-Dessau mechanism, whereby the strongly acidic catalyst protonates n-butane to give carbonium ions. The rate of methane formation from n-butane cracking catalyzed by Fe- and Mn-promoted sulfated zirconia at 450{degrees}C was about 3 x 10{sup -8} mol/(g of catalyst {center_dot}s). The observation of butanes, pentanes, and methane as products is consistent with Olah superacid chemistry, whereby propane is first protonated by a very strong acid to form a carbonium ion. The carbonium ion then decomposes into methane and an ethyl cation which undergoes oligocondensation reactions with propane to form higher molecular weight alkanes. The results are consistent with the identification of iron- and manganese-promoted sulfated zirconia as a superacid.« less

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

NASA Astrophysics Data System (ADS)

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

2003-11-01

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

Assessment of anaerobic biodegradability of five different solid organic wastes

NASA Astrophysics Data System (ADS)

Kristanto, Gabriel Andari; Asaloei, Huinny

2017-03-01

The concept of waste to energy emerges as an alternative solution to increasing waste generation and energy crisis. In the waste to energy concept, waste will be used to produce renewable energy through thermochemical, biochemical, and physiochemical processes. In an anaerobic digester, organic matter brake-down due to anaerobic bacteria produces methane gas as energy source. The organic waste break-down is affected by various characteristics of waste components, such as organic matter content (C, N, O, H, P), solid contents (TS and VS), nutrients ratio (C/N), and pH. This research aims to analyze biodegradability and potential methane production (CH4) from organic waste largely available in Indonesia. Five solid wastes comprised of fecal sludge, cow rumen, goat farm waste, traditional market waste, and tofu dregs were analyzed which showed tofu dregs as waste with the highest rate of biodegradability compared to others since the tofu dregs do not contain any inhibitor which is lignin, have 2.7%VS, 14 C/N ratios and 97.3% organic matter. The highest cumulative methane production known as Biochemical Methane Potential was achieved by tofu dregs with volume of 77 ml during 30-day experiment which then followed by cow rumen, goat farm waste, and traditional market waste. Subsequently, methane productions were calculated through percentage of COD reduction, which showed the efficiency of 99.1% that indicates complete conversion of the high organic matter into methane.

Methane utilization in Methylomicrobium alcaliphilum 20Z R: a systems approach

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

Akberdin, Ilya R.; Thompson, Merlin; Hamilton, Richard

Biological methane utilization, one of the main sinks of the greenhouse gas in nature, represents an attractive platform for production of fuels and value-added chemicals. Despite the progress made in our understanding of the individual parts of methane utilization, our knowledge of how the whole-cell metabolic network is organized and coordinated is limited. Attractive growth and methane-conversion rates, a complete and expert-annotated genome sequence, as well as large enzymatic, 13C-labeling, and transcriptomic datasets make Methylomicrobium alcaliphilum 20Z R an exceptional model system for investigating methane utilization networks. Here we present a comprehensive metabolic framework of methane and methanol utilization inmore » M. alcaliphilum 20Z R. A set of novel metabolic reactions governing carbon distribution across central pathways in methanotrophic bacteria was predicted by in-silico simulations and confirmed by global non-targeted metabolomics and enzymatic evidences. Our data highlight the importance of substitution of ATP-linked steps with PPi-dependent reactions and support the presence of a carbon shunt from acetyl-CoA to the pentose-phosphate pathway and highly branched TCA cycle. The diverged TCA reactions promote balance between anabolic reactions and redox demands. As a result, the computational framework of C 1-metabolism in methanotrophic bacteria can represent an efficient tool for metabolic engineering or ecosystem modeling.« less

Methane utilization in Methylomicrobium alcaliphilum 20Z R: a systems approach

DOE PAGES

Akberdin, Ilya R.; Thompson, Merlin; Hamilton, Richard; ...

2018-02-06

Biological methane utilization, one of the main sinks of the greenhouse gas in nature, represents an attractive platform for production of fuels and value-added chemicals. Despite the progress made in our understanding of the individual parts of methane utilization, our knowledge of how the whole-cell metabolic network is organized and coordinated is limited. Attractive growth and methane-conversion rates, a complete and expert-annotated genome sequence, as well as large enzymatic, 13C-labeling, and transcriptomic datasets make Methylomicrobium alcaliphilum 20Z R an exceptional model system for investigating methane utilization networks. Here we present a comprehensive metabolic framework of methane and methanol utilization inmore » M. alcaliphilum 20Z R. A set of novel metabolic reactions governing carbon distribution across central pathways in methanotrophic bacteria was predicted by in-silico simulations and confirmed by global non-targeted metabolomics and enzymatic evidences. Our data highlight the importance of substitution of ATP-linked steps with PPi-dependent reactions and support the presence of a carbon shunt from acetyl-CoA to the pentose-phosphate pathway and highly branched TCA cycle. The diverged TCA reactions promote balance between anabolic reactions and redox demands. As a result, the computational framework of C 1-metabolism in methanotrophic bacteria can represent an efficient tool for metabolic engineering or ecosystem modeling.« less

Microbial electricity generation in rice paddy fields: recent advances and perspectives in rhizosphere microbial fuel cells.

PubMed

Kouzuma, Atsushi; Kaku, Nobuo; Watanabe, Kazuya

2014-12-01

Microbial fuel cells (MFCs) are devices that use living microbes for the conversion of organic matter into electricity. MFC systems can be applied to the generation of electricity at water/sediment interfaces in the environment, such as bay areas, wetlands, and rice paddy fields. Using these systems, electricity generation in paddy fields as high as ∼80 mW m(-2) (based on the projected anode area) has been demonstrated, and evidence suggests that rhizosphere microbes preferentially utilize organic exudates from rice roots for generating electricity. Phylogenetic and metagenomic analyses have been conducted to identify the microbial species and catabolic pathways that are involved in the conversion of root exudates into electricity, suggesting the importance of syntrophic interactions. In parallel, pot cultures of rice and other aquatic plants have been used for rhizosphere MFC experiments under controlled laboratory conditions. The findings from these studies have demonstrated the potential of electricity generation for mitigating methane emission from the rhizosphere. Notably, however, the presence of large amounts of organics in the rhizosphere drastically reduces the effect of electricity generation on methane production. Further studies are necessary to evaluate the potential of these systems for mitigating methane emission from rice paddy fields. We suggest that paddy-field MFCs represent a promising approach for harvesting latent energy of the natural world.

An Overview of Power, Energy Storage, and Conversion Efforts for 2014 SBIR Phases I and II

NASA Technical Reports Server (NTRS)

Nguyen, Hung D.; Steele, Gynelle C.

2016-01-01

Technological innovation is the overall focus of NASA's Small Business Innovation Research (SBIR) program. The program invests in the development of innovative concepts and technologies to help NASA's mission directorates address critical research and development needs for agency projects. NASA's Small Business Innovation Research (SBIR) program focuses on technological innovation by investing in development of innovative concepts and technologies to help NASA mission directorates address critical research needs for Agency programs. This report highlights 15 of the innovative SBIR 2014 Phase I and II projects that focus on one of NASA Glenn Research Center's six core competencies-Power, Energy Storage and Conversion. The technologies cover a wide spectrum of applications such as high-radiation-tolerant ceramic voltage isolators, development of hermetic sealing glasses for solid oxide fuel cells, rechargeable lithium metal cells, high-efficiency direct methane solid oxide fuel cell systems, Li metal protection for high-energy space batteries, isolated bidirectional direct current converters for distributed battery energy applications, and high-efficiency rad-hard ultrathin Si photovoltaic cell technology for space. Each article describes an innovation and technical objective and highlights NASA commercial and industrial applications. This report provides an opportunity for NASA engineers, researchers, and program managers to learn how NASA SBIR technologies could help their programs and projects, and lead to collaborations and partnerships between the small SBIR companies and NASA that would benefit both.

Synthesis and characterization of Cu-Zn/TiO2 for the photocatalytic conversion of CO2 to methane.

PubMed

Rana, Adeem Ghaffar; Ahmad, Waqar; Al-Matar, Ali; Shawabkeh, Reyad; Aslam, Zaheer

2017-05-01

Different Cu-Zn/TiO 2 catalysts were synthesized by using the wet impregnation method. The prepared catalysts were used for the conversion of CO 2 into methane by photocatalysis. Various characterization techniques were used to observe the surface morphology, crystalline phase, Brunauer-Emmett-Teller (BET) surface area, presence of impregnated Cu and Zn, and functional group. Scanning electron microscope analysis showed spherical morphology, and slight agglomeration of catalyst particles was observed. BET analysis revealed that the surface area of the catalyst was decreased from 10 to 8.5 m 2 /g after impregnation of Cu and Zn over TiO 2 support. Synergetic effect of Cu and Zn over TiO 2 support (Cu 2.6 /TiO 2 , Zn 0.5 /TiO 2 and Cu 2.6 -Zn 0.5 /TiO 2 ) and the effects of Cu loading (0, 1.8, 2.1, 2.6 and 2.9 wt%) were also investigated at different feed molar ratios of H 2 /CO 2 (2:1 and 4:1). The Cu 2.6 -Zn 0.5 /TiO 2 catalyst showed a maximum conversion of 14.3% at a feed molar ratio of 4. The addition of Zn over the catalyst surface increased the conversion of CO 2 from 10% to 14.3% which might be due to synergy of Cu and Zn over TiO 2 support.

Chemical Processing in High-Pressure Aqueous Environments. 9. Process Development for Catalytic Gasification of Algae Feedstocks

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

Elliott, Douglas C.; Hart, Todd R.; Neuenschwander, Gary G.

Through the use of a metal catalyst, gasification of wet algae slurries can be accomplished with high levels of carbon conversion to gas at relatively low temperature (350 C). In a pressurized-water environment (20 MPa), near-total conversion of the organic structure of the algae to gases has been achieved in the presence of a supported ruthenium metal catalyst. The process is essentially steam reforming, as there is no added oxidizer or reagent other than water. In addition, the gas produced is a medium-heating value gas due to the synthesis of high levels of methane, as dictated by thermodynamic equilibrium. Asmore » opposed to earlier work, biomass trace components were removed by processing steps so that they did not cause processing difficulties in the fixed catalyst bed tubular reactor system. As a result, the algae feedstocks, even those with high ash contents, were much more reliably processed. High conversions were obtained even with high slurry concentrations. Consistent catalyst operation in these short-term tests suggested good stability and minimal poisoning effects. High methane content in the product gas was noted with significant carbon dioxide captured in the aqueous byproduct in combination with alkali constituents and the ammonia byproduct derived from proteins in the algae. High conversion of algae to gas products was found with low levels of byproduct water contamination and low to moderate loss of carbon in the mineral separation step.« less

Conversion of Cn-Unsaturated into Cn-2-Saturated LCFA Can Occur Uncoupled from Methanogenesis in Anaerobic Bioreactors.

PubMed

Cavaleiro, Ana J; Pereira, Maria Alcina; Guedes, Ana P; Stams, Alfons J M; Alves, M Madalena; Sousa, Diana Z

2016-03-15

Fat, oils, and grease present in complex wastewater can be readily converted to methane, but the energy potential of these compounds is not always recyclable, due to incomplete degradation of long chain fatty acids (LCFA) released during lipids hydrolysis. Oleate (C18:1) is generally the dominant LCFA in lipid-containing wastewater, and its conversion in anaerobic bioreactors results in palmitate (C16:0) accumulation. The reason why oleate is continuously converted to palmitate without further degradation via β-oxidation is still unknown. In this work, the influence of methanogenic activity in the initial conversion steps of unsaturated LCFA was studied in 10 bioreactors continuously operated with saturated or unsaturated C16- and C18-LCFA, in the presence or absence of the methanogenic inhibitor bromoethanesulfonate (BrES). Saturated Cn-2-LCFA accumulated both in the presence and absence of BrES during the degradation of unsaturated Cn-LCFA, and represented more than 50% of total LCFA. In the presence of BrES further conversion of saturated intermediates did not proceed, not even when prolonged batch incubation was applied. As the initial steps of unsaturated LCFA degradation proceed uncoupled from methanogenesis, accumulation of saturated LCFA can be expected. Analysis of the active microbial communities suggests a role for facultative anaerobic bacteria in the initial steps of unsaturated LCFA biodegradation. Understanding this role is now imperative to optimize methane production from LCFA.

Toward estimation of origin of methane at ancient seeps — Carbon isotopes of seep carbonates, lipid biomarkers, and adsorbed gas

NASA Astrophysics Data System (ADS)

Miyajima, Yusuke; Watanabe, Yumiko; Ijiri, Akira; Goto, Akiko; Jenkins, Robert; Hasegawa, Takashi; Sakai, Saburo; Matsumoto, Ryo

2017-04-01

Methane is generated mainly by microbial or thermal degradation of organic matter, and the origin of methane can be estimated based on its stable carbon isotopic signature. Seafloor seepages of methane-charged fluids have been a major source of methane to the ocean, and knowing the origin of methane at the methane seeps can provide valuable insights into the subsurface fluid circulation and biogeochemical processes. Methane seeps in the geological past are archived as authigenic methane-derived carbonate rocks, which precipitate via an alkalinity increase facilitated by microbially mediated anaerobic oxidation of methane. Here we attempted to estimate origins of methane at ancient seeps, based on several proxies preserved within the seep carbonates. We examined methane-seep carbonate rocks in the Japan Sea region, collected from lower Miocene to middle Pleistocene sediments at 11 sites on land, and also carbonate nodules collected from the seafloor off Joetsu, where thermogenic methane is seeping. Carbon isotopic compositions of the carbonates and lipid biomarkers of methane-oxidizing archaea within them were analyzed. In order to directly know original isotopic signatures of methane, we also attempted to extract adsorbed methane through acid dissolution of the powdered carbonates. Early-diagenetic carbonate phases show various δ13C values between -64.7 and -4.7‰ vs. VPDB, suggesting either biogenic or thermogenic, or both origins of methane. A lipid biomarker pentamethylicosane (PMI) extracted from the ancient carbonates has δ13C values mostly lower than -100‰ , whereas that from the modern methane-derived carbonate nodule has a higher value (-80‰ ). The δ13C values of the seeping methane (-36‰ ) and PMI in the modern Joetsu seep carbonate shows an offset of -44‰ . If this carbon isotope offset was similar at the ancient seeps, the δ13C values of PMI indicate that methane at ancient seeps in the Japan Sea region was biogenic in origin, with δ13C values lower than -50‰ . Acid dissolution of the Miocene to Pliocene carbonates released methane with δ13C values mostly around or higher than -50‰ , which conflicts with the estimation based on biomarkers. Moreover, the Pleistocene and modern samples released only trace amounts of methane. It is thus highly possible that the extracted methane was mostly adsorbed on the carbonates within zones of thermogenic generation of hydrocarbons during burial. In conclusion, we can roughly estimate origins of methane at ancient seeps based on δ13C values of carbonates and biomarkers. However, in order to directly analyze methane contained in ancient seepage fluids, exploration of gas or fluid inclusions trapped within carbonate crystals is necessary.

Environmental impacts on the diversity of methane-cycling microbes and their resultant function

PubMed Central

Aronson, Emma L.; Allison, Steven D.; Helliker, Brent R.

2013-01-01

Methane is an important anthropogenic greenhouse gas that is produced and consumed in soils by microorganisms responding to micro-environmental conditions. Current estimates show that soil consumption accounts for 5–15% of methane removed from the atmosphere on an annual basis. Recent variability in atmospheric methane concentrations has called into question the reliability of estimates of methane consumption and calls for novel approaches in order to predict future atmospheric methane trends. This review synthesizes the environmental and climatic factors influencing the consumption of methane from the atmosphere by non-wetland, terrestrial soil microorganisms. In particular, we focus on published efforts to connect community composition and diversity of methane-cycling microbial communities to observed rates of methane flux. We find abundant evidence for direct connections between shifts in the methane-cycling microbial community, due to climate and environmental changes, and observed methane flux levels. These responses vary by ecosystem and associated vegetation type. This information will be useful in process-based models of ecosystem methane flux responses to shifts in environmental and climatic parameters. PMID:23966984

Reacting Flow in the Entrance to a Channel with Surface and Gas-Phase Kinetics

NASA Astrophysics Data System (ADS)

Mikolaitis, David; Griffen, Patrick

2006-11-01

In many catalytic reactors the conversion process is most intense at the very beginning of the channel where the flow is not yet fully developed; hence there will be important interactions between the developing flow field and reaction. To study this problem we have written an object-oriented code for the analysis of reacting flow in the entrance of a channel where both surface reaction and gas-phase reaction are modeled with detailed kinetics. Fluid mechanical momentum and energy equations are modeled by parabolic ``boundary layer''-type equations where streamwise gradient terms are small and the pressure is constant in the transverse direction. Transport properties are modeled with mixture-averaging and the chemical kinetic sources terms are evaluated using Cantera. Numerical integration is done with Matlab using the function pdepe. Calculations were completed using mixtures of methane and air flowing through a channel with platinum walls held at a fixed temperature. GRI-Mech 3.0 was used to describe the gas-phase chemistry and Deutchmann's methane-air-platinum model was used for the surface chemistry. Ignition in the gas phase is predicted for high enough wall temperatures. A hot spot forms away from the walls just before ignition that is fed by radicals produced at the surface.

Exposure to polystyrene nanoplastic leads to inhibition of anaerobic digestion system.

PubMed

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.

Characterisation of water hyacinth with microwave-heated alkali pretreatment for enhanced enzymatic digestibility and hydrogen/methane fermentation.

PubMed

Lin, Richen; Cheng, Jun; Song, Wenlu; Ding, Lingkan; Xie, Binfei; Zhou, Junhu; Cen, Kefa

2015-04-01

Microwave-heated alkali pretreatment (MAP) was investigated to improve enzymatic digestibility and H2/CH4 production from water hyacinth. SEM revealed that MAP deconstructed the lignocellulose matrix and swelled the surfaces of water hyacinth. XRD indicated that MAP decreased the crystallinity index from 16.0 to 13.0 because of cellulose amorphisation. FTIR indicated that MAP effectively destroyed the lignin structure and disrupted the crystalline cellulose to reduce crystallinity. The reducing sugar yield of 0.296 g/gTVS was achieved at optimal hydrolysis conditions (microwave temperature = 190°C, time = 10 min, and cellulase dosage = 5 wt%). The sequentially fermentative hydrogen and methane yields from water hyacinth with MAP and enzymatic hydrolysis were increased to 63.9 and 172.5 mL/gTVS, respectively. The energy conversion efficiency (40.0%) in the two-stage hydrogen and methane cogeneration was lower than that (49.5%) in the one-stage methane production (237.4 mL/gTVS) from water hyacinth with MAP and enzymatic hydrolysis. Copyright © 2015 Elsevier Ltd. All rights reserved.

Oxidative coupling of methane using inorganic membrane reactor

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

Ma, Y.H.; Moser, W.R.; Dixon, A.G.

1995-12-31

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

Attribution of changes in global wetland methane emissions from pre-industrial to present using CLM4.5-BGC

DOE PAGES

Paudel, Rajendra; Mahowald, Natalie M.; Hess, Peter G. M.; ...

2016-03-10

An understanding of potential factors controlling methane emissions from natural wetlands is important to accurately project future atmospheric methane concentrations. Here, we examine the relative contributions of climatic and environmental factors, such as precipitation, temperature, atmospheric CO 2 concentration, nitrogen deposition, wetland inundation extent, and land-use and land-cover change, on changes in wetland methane emissions from preindustrial to present day (i.e., 1850-2005). We apply a mechanistic methane biogeochemical model integrated in the Community Land Model version 4.5 (CLM4.5), the land component of the Community Earth System Model. The methane model explicitly simulates methane production, oxidation, ebullition, transport through aerenchyma ofmore » plants, and aqueous and gaseous diffusion. We conduct a suite of model simulations from 1850 to 2005, with all changes in environmental factors included, and sensitivity studies isolating each factor. Globally, we estimate that preindustrial methane emissions were higher by 10% than present-day emissions from natural wetlands, with emissions changes from preindustrial to the present of +15%, -41%, and -11% for the high latitudes, temperate regions, and tropics, respectively. The most important change is due to the estimated change in wetland extent, due to the conversion of wetland areas to drylands by humans. This effect alone leads to higher preindustrial global methane fluxes by 33% relative to the present, with the largest change in temperate regions (+80%). These increases were partially offset by lower preindustrial emissions due to lower CO 2 levels (10%), shifts in precipitation (7%), lower nitrogen deposition (3%), and changes in land-use and land-cover (2%). Cooler temperatures in the preindustrial regions resulted in our simulations in an increase in global methane emissions of 6% relative to present day. Much of the sensitivity to these perturbations is mediated in the model by changes in methane substrate production and the areal extent of wetlands. The detrended interannual variability of high-latitude methane emissions is explained by the variation in substrate production and wetland inundation extent, whereas the tropical emission variability is explained by both of those variables and precipitation.« less

Attribution of changes in global wetland methane emissions from pre-industrial to present using CLM4.5-BGC

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

Paudel, Rajendra; Mahowald, Natalie M.; Hess, Peter G. M.

An understanding of potential factors controlling methane emissions from natural wetlands is important to accurately project future atmospheric methane concentrations. Here, we examine the relative contributions of climatic and environmental factors, such as precipitation, temperature, atmospheric CO 2 concentration, nitrogen deposition, wetland inundation extent, and land-use and land-cover change, on changes in wetland methane emissions from preindustrial to present day (i.e., 1850-2005). We apply a mechanistic methane biogeochemical model integrated in the Community Land Model version 4.5 (CLM4.5), the land component of the Community Earth System Model. The methane model explicitly simulates methane production, oxidation, ebullition, transport through aerenchyma ofmore » plants, and aqueous and gaseous diffusion. We conduct a suite of model simulations from 1850 to 2005, with all changes in environmental factors included, and sensitivity studies isolating each factor. Globally, we estimate that preindustrial methane emissions were higher by 10% than present-day emissions from natural wetlands, with emissions changes from preindustrial to the present of +15%, -41%, and -11% for the high latitudes, temperate regions, and tropics, respectively. The most important change is due to the estimated change in wetland extent, due to the conversion of wetland areas to drylands by humans. This effect alone leads to higher preindustrial global methane fluxes by 33% relative to the present, with the largest change in temperate regions (+80%). These increases were partially offset by lower preindustrial emissions due to lower CO 2 levels (10%), shifts in precipitation (7%), lower nitrogen deposition (3%), and changes in land-use and land-cover (2%). Cooler temperatures in the preindustrial regions resulted in our simulations in an increase in global methane emissions of 6% relative to present day. Much of the sensitivity to these perturbations is mediated in the model by changes in methane substrate production and the areal extent of wetlands. The detrended interannual variability of high-latitude methane emissions is explained by the variation in substrate production and wetland inundation extent, whereas the tropical emission variability is explained by both of those variables and precipitation.« less

On-site manufacture of propellant oxygen from lunar resources

NASA Technical Reports Server (NTRS)

Rosenberg, Sanders D.

1992-01-01

The Aerojet Carbothermal Process for the manufacture of oxygen from lunar resources has three essential steps: the reduction of silicate with methane to form carbon monoxide and hydrogen; the reduction of carbon monoxide with hydrogen to form methane and water; and the electrolysis of water to form oxygen and hydrogen. This cyclic process does not depend upon the presence of water or water precursors in the lunar materials; it will produce oxygen from silicates regardless of their precise composition and fine structure. Research on the first step of the process was initiated by determining some of the operating conditions required to reduce igneous rock with carbon and silicon carbide. The initial phase of research on the second step is completed; quantitative conversion of carbon monoxide and hydrogen to methane and water was achieved with a nickel-on-kieselguhr catalyst. The equipment used in and the results obtained from these process studies are reported in detail.

A trimodal porous carbon as an effective catalyst for hydrogen production by methane decomposition.

PubMed

Shen, Yi; Lua, Aik Chong

2016-01-15

A new type of porous carbon with an interconnected trimodal pore system is synthesized by a nanocasting method using nanoparticulated bimodal micro-mesoporous silica particles as the template. The synthesized template and carbon material are characterized using transmission electron microscopy (TEM), field emission electron scanning microscopy (FESEM) and nitrogen adsorption-desorption test. The synthesized carbon material has an extremely high surface area, a large pore volume and an interconnected pore structure, which could provide abundant active sites and space for chemical reactions and minimize the diffusion resistance of the reactants. The resulting carbon is used as the catalyst for hydrogen production by the thermal decomposition of methane. The catalytic results show that the as-synthesized carbon in this study produces much higher methane conversion and hydrogen yield than the commercial carbon materials. Copyright © 2015 Elsevier Inc. All rights reserved.

New approach to control the methanogenic reactor of a two-phase anaerobic digestion system.

PubMed

von Sachs, Jürgen; Meyer, Ulrich; Rys, Paul; Feitkenhauer, Heiko

2003-03-01

A new control strategy for the methanogenic reactor of a two-phase anaerobic digestion system has been developed and successfully tested on the laboratory scale. The control strategy serves the purpose to detect inhibitory effects and to achieve good conversion. The concept is based on the idea that volatile fatty acids (VFA) can be measured in the influent of the methanogenic reactor by means of titration. Thus, information on the output (methane production) and input of the methanogenic reactor is available, and a (carbon) mass balance can be obtained. The control algorithm comprises a proportional/integral structure with the ratio of (a) the methane production rate measured online and (b) a maximum methane production rate expected (derived from the stoichiometry) as a control variable. The manipulated variable is the volumetric feed rate. Results are shown for an experiment with VFA (feed) concentration ramps and for experiments with sodium chloride as inhibitor.

Effect of Catalytic Cylinders on Autothermal Reforming of Methane for Hydrogen Production in a Microchamber Reactor

PubMed Central

Yan, Yunfei; Guo, Hongliang; Zhang, Li; Zhu, Junchen; Yang, Zhongqing; Tang, Qiang; Ji, Xin

2014-01-01

A new multicylinder microchamber reactor is designed on autothermal reforming of methane for hydrogen production, and its performance and thermal behavior, that is, based on the reaction mechanism, is numerically investigated by varying the cylinder radius, cylinder spacing, and cylinder layout. The results show that larger cylinder radius can promote reforming reaction; the mass fraction of methane decreased from 26% to 21% with cylinder radius from 0.25 mm to 0.75 mm; compact cylinder spacing corresponds to more catalytic surface and the time to steady state is decreased from 40 s to 20 s; alteration of staggered and aligned cylinder layout at constant inlet flow rates does not result in significant difference in reactor performance and it can be neglected. The results provide an indication and optimize performance of reactor; it achieves higher conversion compared with other reforming reactors. PMID:25097877

Raman and FTIR spectroscopy of methane in olivine

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Thermodynamic equilibrium calculations of dimethyl ether steam reforming and dimethyl ether hydrolysis

NASA Astrophysics Data System (ADS)

Semelsberger, Troy A.; Borup, Rodney L.

The production of a hydrogen-rich fuel-cell feed by dimethyl ether (DME) steam reforming was investigated using calculations of thermodynamic equilibrium as a function of steam-to-carbon ratio (0.00-4.00), temperature (100-600 °C), pressure (1-5 atm), and product species. Species considered were acetone, acetylene, carbon dioxide, carbon monoxide, dimethyl ether, ethane, ethanol, ethylene, formaldehyde, formic acid, hydrogen, isopropanol, methane, methanol, methyl-ethyl ether, n-propanol and water. Thermodynamic equilibrium calculations of DME steam reforming indicate complete conversion of dimethyl ether to hydrogen, carbon monoxide and carbon dioxide at temperatures greater than 200 °C and steam-to-carbon ratios greater than 1.25 at atmospheric pressure ( P = 1 atm). Increasing the operating pressure shifts the equilibrium toward the reactants; increasing the pressure from 1 to 5 atm decreases the conversion of dimethyl ether from 99.5 to 76.2%. The trend of thermodynamically stable products in decreasing mole fraction is methane, ethane, isopropyl alcohol, acetone, n-propanol, ethylene, ethanol, methyl-ethyl ether and methanol-formaldehyde, formic acid, and acetylene were not observed. Based on the equilibrium calculations, the optimal processing conditions for dimethyl ether steam reforming occur at a steam-to-carbon ratio of 1.50, a pressure of 1 atm, and a temperature of 200 °C. These thermodynamic equilibrium calculations show dimethyl ether processed with steam will produce hydrogen-rich fuel-cell feeds—with hydrogen concentrations exceeding 70%. The conversion of dimethyl ether via hydrolysis (considering methanol as the only product) is limited by thermodynamic equilibrium. Equilibrium conversion increases with temperature and steam-to-carbon ratio. A maximum dimethyl ether conversion of 62% is achieved at a steam-to-carbon ratio of 5.00 and a processing temperature of 600 °C.

Confinement Effects on Carbon Dioxide Methanation: A Novel Mechanism for Abiotic Methane Formation

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

Le, Thu; Striolo, Alberto; Turner, C. Heath

An important scientific debate focuses on the possibility of abiotic synthesis of hydrocarbons during oceanic crust-seawater interactions. While on-site measurements near hydrothermal vents support this possibility, laboratory studies have provided data that are in some cases contradictory. At conditions relevant for sub-surface environments it has been shown that classic thermodynamics favour the production of CO 2 from CH 4, while abiotic methane synthesis would require the opposite. However, confinement effects are known to alter reaction equilibria. This report shows that indeed thermodynamic equilibrium can be shifted towards methane production, suggesting that thermal hydrocarbon synthesis near hydrothermal vents and deeper inmore » the magma-hydrothermal system is possible. We report reactive ensemble Monte Carlo simulations for the CO 2 methanation reaction. We compare the predicted equilibrium composition in the bulk gaseous phase to that expected in the presence of confinement. In the bulk phase we obtain excellent agreement with classic thermodynamic expectations. When the reactants can exchange between bulk and a confined phase our results show strong dependency of the reaction equilibrium conversions, X CO2, on nanopore size, nanopore chemistry, and nanopore morphology. Some physical conditions that could shift significantly the equilibrium composition of the reactive system with respect to bulk observations are discussed.« less

Confinement Effects on Carbon Dioxide Methanation: A Novel Mechanism for Abiotic Methane Formation

DOE PAGES

Le, Thu; Striolo, Alberto; Turner, C. Heath; ...

2017-08-21

An important scientific debate focuses on the possibility of abiotic synthesis of hydrocarbons during oceanic crust-seawater interactions. While on-site measurements near hydrothermal vents support this possibility, laboratory studies have provided data that are in some cases contradictory. At conditions relevant for sub-surface environments it has been shown that classic thermodynamics favour the production of CO 2 from CH 4, while abiotic methane synthesis would require the opposite. However, confinement effects are known to alter reaction equilibria. This report shows that indeed thermodynamic equilibrium can be shifted towards methane production, suggesting that thermal hydrocarbon synthesis near hydrothermal vents and deeper inmore » the magma-hydrothermal system is possible. We report reactive ensemble Monte Carlo simulations for the CO 2 methanation reaction. We compare the predicted equilibrium composition in the bulk gaseous phase to that expected in the presence of confinement. In the bulk phase we obtain excellent agreement with classic thermodynamic expectations. When the reactants can exchange between bulk and a confined phase our results show strong dependency of the reaction equilibrium conversions, X CO2, on nanopore size, nanopore chemistry, and nanopore morphology. Some physical conditions that could shift significantly the equilibrium composition of the reactive system with respect to bulk observations are discussed.« less

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

DOE PAGES

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

2016-05-02

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

The hunt for the most-wanted chemolithoautotrophic spookmicrobes

PubMed Central

2018-01-01

ABSTRACT Microorganisms are the drivers of biogeochemical methane and nitrogen cycles. Essential roles of chemolithoautotrophic microorganisms in these cycles were predicted long before their identification. Dedicated enrichment procedures, metagenomics surveys and single-cell technologies have enabled the identification of several new groups of most-wanted spookmicrobes, including novel methoxydotrophic methanogens that produce methane from methylated coal compounds and acetoclastic ‘Candidatus Methanothrix paradoxum’, which is active in oxic soils. The resultant energy-rich methane can be oxidized via a suite of electron acceptors. Recently, ‘Candidatus Methanoperedens nitroreducens’ ANME-2d archaea and ‘Candidatus Methylomirabilis oxyfera’ bacteria were enriched on nitrate and nitrite under anoxic conditions with methane as an electron donor. Although ‘Candidatus Methanoperedens nitroreducens’ and other ANME archaea can use iron citrate as an electron acceptor in batch experiments, the quest for anaerobic methane oxidizers that grow via iron reduction continues. In recent years, the nitrogen cycle has been expanded by the discovery of various ammonium-oxidizing prokaryotes, including ammonium-oxidizing archaea, versatile anaerobic ammonium-oxidizing (anammox) bacteria and complete ammonium-oxidizing (comammox) Nitrospira bacteria. Several biogeochemical studies have indicated that ammonium conversion occurs under iron-reducing conditions, but thus far no microorganism has been identified. Ultimately, iron-reducing and sulfate-dependent ammonium-oxidizing microorganisms await discovery. PMID:29873717

Treatment of corn ethanol distillery wastewater using two-stage anaerobic digestion.

PubMed

Ráduly, B; Gyenge, L; Szilveszter, Sz; Kedves, A; Crognale, S

In this study the mesophilic two-stage anaerobic digestion (AD) of corn bioethanol distillery wastewater is investigated in laboratory-scale reactors. Two-stage AD technology separates the different sub-processes of the AD in two distinct reactors, enabling the use of optimal conditions for the different microbial consortia involved in the different process phases, and thus allowing for higher applicable organic loading rates (OLRs), shorter hydraulic retention times (HRTs) and better conversion rates of the organic matter, as well as higher methane content of the produced biogas. In our experiments the reactors have been operated in semi-continuous phase-separated mode. A specific methane production of 1,092 mL/(L·d) has been reached at an OLR of 6.5 g TCOD/(L·d) (TCOD: total chemical oxygen demand) and a total HRT of 21 days (5.7 days in the first-stage, and 15.3 days in the second-stage reactor). Nonetheless the methane concentration in the second-stage reactor was very high (78.9%); the two-stage AD outperformed the reference single-stage AD (conducted at the same reactor loading rate and retention time) by only a small margin in terms of volumetric methane production rate. This makes questionable whether the higher methane content of the biogas counterbalances the added complexity of the two-stage digestion.

Evaluation on direct interspecies electron transfer in anaerobic sludge digestion of microbial electrolysis cell.

PubMed

Zhao, Zisheng; Zhang, Yaobin; Quan, Xie; Zhao, Huimin

2016-01-01

Increase of methanogenesis in methane-producing microbial electrolysis cells (MECs) is frequently believed as a result of cathodic reduction of CO2. Recent studies indicated that this electromethanogenesis only accounted for a little part of methane production during anaerobic sludge digestion. Instead, direct interspecies electron transfer (DIET) possibly plays an important role in methane production. In this study, anaerobic digestion of sludge were investigated in a single-chamber MEC reactor, a carbon-felt supplemented reactor and a common anaerobic reactor to evaluate the effects of DIET on the sludge digestion. The results showed that adding carbon felt into the reactor increased 12.9% of methane production and 17.2% of sludge reduction. Imposing a voltage on the carbon felt further improved the digestion. Current calculation showed that the cathodic reduction only contributed to 27.5% of increased methane production. Microbial analysis indicated that DIET played an important role in the anaerobic sludge digestion in the MEC. Copyright © 2015 Elsevier Ltd. All rights reserved.

Direct measurement of methane hydrate composition along the hydrate equilibrium boundary

USGS Publications Warehouse

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

2005-01-01

The composition of methane hydrate, namely nW for CH 4??nWH2O, was directly measured along the hydrate equilibrium boundary under conditions of excess methane gas. Pressure and temperature conditions ranged from 1.9 to 9.7 MPa and 263 to 285 K. Within experimental error, there is no change in hydrate composition with increasing pressure along the equilibrium boundary, but nW may show a slight systematic decrease away from this boundary. A hydrate stoichiometry of n W = 5.81-6.10 H2O describes the entire range of measured values, with an average composition of CH4??5.99(??0.07) H2O along the equilibrium boundary. These results, consistent with previously measured values, are discussed with respect to the widely ranging values obtained by thermodynamic analysis. The relatively constant composition of methane hydrate over the geologically relevant pressure and temperature range investigated suggests that in situ methane hydrate compositions may be estimated with some confidence. ?? 2005 American Chemical Society.

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

PubMed Central

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

Iron oxides alter methanogenic pathways of acetate in production water of high-temperature petroleum reservoir.

PubMed

Pan, Pan; Hong, Bo; Mbadinga, Serge Maurice; Wang, Li-Ying; Liu, Jin-Feng; Yang, Shi-Zhong; Gu, Ji-Dong; Mu, Bo-Zhong

2017-09-01

Acetate is a key intermediate in anaerobic crude oil biodegradation and also a precursor for methanogenesis in petroleum reservoirs. The impact of iron oxides, viz. β-FeOOH (akaganéite) and magnetite (Fe 3 O 4 ), on the methanogenic acetate metabolism in production water of a high-temperature petroleum reservoir was investigated. Methane production was observed in all the treatments amended with acetate. In the microcosms amended with acetate solely about 30% of the acetate utilized was converted to methane, whereas methane production was stimulated in the presence of magnetite (Fe 3 O 4 ) resulting in a 48.34% conversion to methane. Methane production in acetate-amended, β-FeOOH (akaganéite)-supplemented microcosms was much faster and acetate consumption was greatly improved compared to the other conditions in which the stoichiometric expected amounts of methane were not produced. Microbial community analysis showed that Thermacetogenium spp. (known syntrophic acetate oxidizers) and hydrogenotrophic methanogens closely related to Methanothermobacter spp. were enriched in acetate and acetate/magnetite (Fe 3 O 4 ) microcosms suggesting that methanogenic acetate metabolism was through hydrogenotrophic methanogenesis fueled by syntrophic acetate oxidizers. The acetate/β-FeOOH (akaganéite) microcosms, however, differed by the dominance of archaea closely related to the acetoclastic Methanosaeta thermophila. These observations suggest that supplementation of β-FeOOH (akaganéite) accelerated the production of methane further, driven the alteration of the methanogenic community, and changed the pathway of acetate methanogenesis from hydrogenotrophic methanogenesis fueled by syntrophic acetate oxidizers to acetoclastic.

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

PubMed

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.

Bioelectrochemical approach for control of methane emission from wetlands.

PubMed

Liu, Shentan; Feng, Xiaojuan; Li, Xianning

2017-10-01

To harvest electricity and mitigate methane emissions from wetlands, a novel microbial fuel cell coupled constructed wetland (MFC-CW) was assembled with an anode placing in the rhizosphere and a cathode on the water surface. Plant-mediated methane accounted for 71-82% of the total methane fluxes. The bioanode served as an inexhaustible source of electron acceptors and resulted in reduced substantial methane emissions owing to electricigens outcompeting methanogens for carbon and electrons when substrate was deficient. However, when supplying sufficient organic carbon, both electricity and methane increased, indicating that electrogenesis and methanogenesis could co-exist in harmony. Direct methane emission (diffusion/ebullition) and plant-mediated methane emission were affected by operating conditions. Methanogenesis was significantly suppressed (∼98%) at HRT of 96h and with external resistance of 200Ω, accompanied with improved coulombic efficiency of 14.9% and current density of 187mA/m 2 . Contrarily, change of electrode polarity in the rhizosphere led to more methane efflux. Copyright © 2017 Elsevier Ltd. All rights reserved.

Measured temperature and pressure dependence of Vp and Vs in compacted, polycrystalline sI methane and sII methane-ethane hydrate

USGS Publications Warehouse

Helgerud, M.B.; Waite, W.F.; Kirby, S.H.; Nur, A.

2003-01-01

We report on compressional- and shear-wave-speed measurements made on compacted polycrystalline sI methane and sII methane-ethane hydrate. The gas hydrate samples are synthesized directly in the measurement apparatus by warming granulated ice to 17??C in the presence of a clathrate-forming gas at high pressure (methane for sI, 90.2% methane, 9.8% ethane for sII). Porosity is eliminated after hydrate synthesis by compacting the sample in the synthesis pressure vessel between a hydraulic ram and a fixed end-plug, both containing shear-wave transducers. Wave-speed measurements are made between -20 and 15??C and 0 to 105 MPa applied piston pressure.

Direct use of methane in coal liquefaction

DOEpatents

Sundaram, Muthu S.; Steinberg, Meyer

1987-01-01

This invention relates to a process for converting solid carbonaceous material, such as coal, to liquid and gaseous hydrocarbons utilizing methane, generally at a residence time of about 20-120 minutes at a temperature of 250.degree.-750.degree. C., preferably 350.degree.-450.degree. C., pressurized up to 6000 psi, and preferably in the 1000-2500 psi range, preferably directly utilizing methane 50-100% by volume in a mix of methane and hydrogen. A hydrogen donor solvent or liquid vehicle such as tetralin, tetrahydroquinoline, piperidine, and pyrolidine may be used in a slurry mix where the solvent feed is 0-100% by weight of the coal or carbonaceous feed. Carbonaceous feed material can either be natural, such as coal, wood, oil shale, petroleum, tar sands, etc., or man-made residual oils, tars, and heavy hydrocarbon residues from other processing systems.

Application of optimized alkaline pretreatment for enhancing the anaerobic digestion of different sunflower stalks varieties.

PubMed

Monlau, Florian; Aemig, Quentin; Barakat, Abdellatif; Steyer, Jean-Philippe; Carrère, Hélène

2013-01-01

The use of lignocellulosic residues such as sunflower stalks (SS) for the production of bioenergy such as methane is a promising alternative to fossil fuels. However, their recalcitrant structure justifies the use of pretreatment to enhance the accessibility of holocelluloses and their further conversion into methane. First, different conditions of alkaline pretreatment (i.e. duration and NaOH concentration (g/100 g TS) at a fixed temperature of 55 degrees C) were tested to enhance the methane potential of the stalks of the Serin sunflower (193 mL of methane per gram of volatile solids (VS)). The greatest improvement to the methane potential (262 mL CH4 g(-1) VS) was observed at 55 degrees C, 24 h, 4 g NaOH/100 g TS. Fourier Transform Infrared spectra highlighted an accumulation of lignin in the digestate and the degradation of holocelluloses during the anaerobic process, both for pretreated and untreated SS. In a second stage, this optimum condition for alkaline pretreatment (55 degrees C, 24 h, 4 g NaOH/100 g TS) was applied to the stalks of three other varieties of sunflower. Alkaline pretreatment was effective in the delignification of the stalks of the different sunflower varieties, with lignin reduction varying from 23.3% to 36.3% VS. This reduction of lignin was concomitant with the enhancement of methane potential as compared to that of raw SS, with an increase ranging from 29% to 44% for the different SS.

Extreme methane emissions from a Swiss hydropower reservoir: contribution from bubbling sediments.

PubMed

Delsontro, Tonya; McGinnis, Daniel F; Sobek, Sebastian; Ostrovsky, Ilia; Wehrli, Bernhard

2010-04-01

Methane emission pathways and their importance were quantified during a yearlong survey of a temperate hydropower reservoir. Measurements using gas traps indicated very high ebullition rates, but due to the stochastic nature of ebullition a mass balance approach was crucial to deduce system-wide methane sources and losses. Methane diffusion from the sediment was generally low and seasonally stable and did not account for the high concentration of dissolved methane measured in the reservoir discharge. A strong positive correlation between water temperature and the observed dissolved methane concentration enabled us to quantify the dissolved methane addition from bubble dissolution using a system-wide mass balance. Finally, knowing the contribution due to bubble dissolution, we used a bubble model to estimate bubble emission directly to the atmosphere. Our results indicated that the total methane emission from Lake Wohlen was on average >150 mg CH(4) m(-2) d(-1), which is the highest ever documented for a midlatitude reservoir. The substantial temperature-dependent methane emissions discovered in this 90-year-old reservoir indicate that temperate water bodies can be an important but overlooked methane source.

Co-digestion of polylactide and kitchen garbage in hyperthermophilic and thermophilic continuous anaerobic process.

PubMed

Wang, Feng; Hidaka, Taira; Tsuno, Hiroshi; Tsubota, Jun

2012-05-01

Two series of two-phase anaerobic systems, consisting of a hyperthermophilic (80°C) reactor and a thermophilic (55°C) reactor, fed with a mixture of kitchen garbage (KG) and polylactide (PLA), was compared with a single-phase thermophilic reactor for the overall performance. The result indicated that ammonia addition under hyperthermophilic condition promoted the transformation of PLA particles to lactic acid. The systems with hyperthermophilic treatment had advantages on PLA transformation and methane conversion ratio to the control system. Under the organic loading rate (OLR) of 10.3 g COD/(L day), the PLA transformation ratios of the two-phase systems were 82.0% and 85.2%, respectively, higher than that of the control system (63.5%). The methane conversion ratios of the two-phase systems were 82.9% and 80.8%, respectively, higher than 70.1% of the control system. The microbial community analysis indicated that hyperthermophilic treatment is easily installed to traditional thermophilic anaerobic digestion plants without inoculation of special bacteria. Copyright © 2012 Elsevier Ltd. All rights reserved.

Oxidative coupling of methane over a Sr-promoted La{sub 2}O{sub 3} catalyst supported on a low surface area porous catalyst carrier

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

Choudhary, V.R.; Uphade, B.S.; Mulla, S.A.R.

1997-09-01

Oxidative coupling of methane (OCM) to higher hydrocarbons over Sr-promoted La{sub 2}O{sub 3} supported on commercial low surface area porous catalyst carriers at 800 and 850 C and a space velocity of 102,000 cm{sup 3}/g{center_dot}h has been thoroughly investigated. Effects of support, catalyst particle size, linear gas velocity, Sr/La ratio, CH{sub 4}/O{sub 2} ratio in the feed, and catalyst dilution by inert solid particles on the conversion, yield, or selectivity and product ratios (C{sub 2}H{sub 4}/C{sub 2}H{sub 6} and CO/CO{sub 2}) in the OCM process have been studied. The catalysts have been characterized for their basicity, acidity, and oxygen chemisorptionmore » by the TPD of CO{sub 2}, ammonia, and oxygen, respectively, from 50 to 950 C and also characterized for their surface area. The supported catalysts showed better performance than the unsupported one. The best OCM results (obtained over Sr-La{sub 2}O{sub 3}/SA-5205 with a Sr/La ratio of 0.3 at a space velocity of 102,000 cm{sup 3}/g{center_dot}h) are 30.1% CH{sub 4} conversion with 65.6% selectivity for C{sub 2+} (or 19.7% C{sub 2+}-yield) at 850 C (CH{sub 4}/O{sub 2} = 16.0). The basicity is strongly influenced by the Sr/La ratio; the supported catalysts showed the best performance for their Sr/La ratio of about 0.3. The methane/O{sub 2} ratio also showed a strong influence for their Sr/La ratio of about 0.3. The methane/O{sub 2} ratio also showed a strong influence on the OCM process. However, the influence of linear gas velocity and particle size is found to be small; it results mainly from the temperature gradient in the catalyst. The catalyst dilution has beneficial effects for achieving a higher C{sub 2}H{sub 4}/C{sub 2}H{sub 6} ratio and also for reducing the hazardous nature of the OCM process because of the coupling of the exothermic oxidative conversion reactions and the endothermic thermal cracking reactions and also due to the increased heat transfer area.« less

Methane Conversion to Ethylene and Aromatics on PtSn Catalysts

DOE PAGES

Gerceker, Duygu; Motagamwala, Ali Hussain; Rivera-Dones, Keishla R.; ...

2017-02-03

Pt and PtSn catalysts supported on SiO 2 and H-ZSM-5 were studied for methane conversion under nonoxidative conditions. Addition of Sn to Pt/SiO 2 increased the turnover frequency for production of ethylene by a factor of 3, and pretreatment of the catalyst at 1123 K reduced the extent of coke formation. Pt and PtSn catalysts supported on H-ZSM-5 zeolite were prepared to improve the activity and selectivity to non-coke products. Ethylene formation rates were 20 times faster over a PtSn(1:3)/H-ZSM-5 catalyst with SiO 2:Al 2O 3 = 280 in comparison to those over PtSn(3:1)/SiO 2. H-ZSM-5-supported catalysts were also activemore » for the formation of aromatics, and the rates of benzene and naphthalene formation were increased by using more acidic H-ZSM-5 supports. These catalysts operate through a bifunctional mechanism, in which ethylene is first produced on highly dispersed PtSn nanoparticles and then is subsequently converted to benzene and naphthalene on Brønsted acid sites within the zeolite support. The most active and stable PtSn catalyst forms carbon products at a rate, 2.5 mmol of C/((mol of Pt) s), which is comparable to that of state-of-the-art Mo/H-ZSM-5 catalysts with same metal loading operated under similar conditions (1.8 mmol of C/((mol of Mo) s)). Scanning transmission electron microscopy measurements suggest the presence of smaller Pt nanoparticles on H-ZSM-5-supported catalysts, in comparison to SiO 2-supported catalysts, as a possible source of their high activity. As a result, a microkinetic model of methane conversion on Pt and PtSn surfaces, built using results from density functional theory calculations, predicts higher coupling rates on bimetallic and stepped surfaces, supporting the experimental observations that relate the high catalytic activity to small PtSn particles.« 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.

Catalytic aromatization of methane.

PubMed

Spivey, James J; Hutchings, Graham

2014-02-07

Recent developments in natural gas production technology have led to lower prices for methane and renewed interest in converting methane to higher value products. Processes such as those based on syngas from methane reforming are being investigated. Another option is methane aromatization, which produces benzene and hydrogen: 6CH4(g) → C6H6(g) + 9H2(g) ΔG°(r) = +433 kJ mol(-1) ΔH°(r) = +531 kJ mol(-1). Thermodynamic calculations for this reaction show that benzene formation is insignificant below ∼600 °C, and that the formation of solid carbon [C(s)] is thermodynamically favored at temperatures above ∼300 °C. Benzene formation is insignificant at all temperatures up to 1000 °C when C(s) is included in the calculation of equilibrium composition. Interestingly, the thermodynamic limitation on benzene formation can be minimized by the addition of alkanes/alkenes to the methane feed. By far the most widely studied catalysts for this reaction are Mo/HZSM-5 and Mo/MCM-22. Benzene selectivities are generally between 60 and 80% at methane conversions of ∼10%, corresponding to net benzene yields of less than 10%. Major byproducts include lower molecular weight hydrocarbons and higher molecular weight substituted aromatics. However, carbon formation is inevitable, but the experimental findings show this can be kinetically limited by the use of H2 or oxidants in the feed, including CO2 or steam. A number of reactor configurations involving regeneration of the carbon-containing catalyst have been developed with the goal of minimizing the cost of regeneration of the catalyst once deactivated by carbon deposition. In this tutorial review we discuss the thermodynamics of this process, the catalysts used and the potential reactor configurations that can be applied.

Hydrocarbon-Rich Groundwater above Shale-Gas Formations: A Karoo Basin Case Study.

PubMed

Eymold, William K; Swana, Kelley; Moore, Myles T; Whyte, Colin J; Harkness, Jennifer S; Talma, Siep; Murray, Ricky; Moortgat, Joachim B; Miller, Jodie; Vengosh, Avner; Darrah, Thomas H

2018-03-01

Horizontal drilling and hydraulic fracturing have enhanced unconventional hydrocarbon recovery but raised environmental concerns related to water quality. Because most basins targeted for shale-gas development in the USA have histories of both active and legacy petroleum extraction, confusion about the hydrogeological context of naturally occurring methane in shallow aquifers overlying shales remains. The Karoo Basin, located in South Africa, provides a near-pristine setting to evaluate these processes, without a history of conventional or unconventional energy extraction. We conducted a comprehensive pre-industrial evaluation of water quality and gas geochemistry in 22 groundwater samples across the Karoo Basin, including dissolved ions, water isotopes, hydrocarbon molecular and isotopic composition, and noble gases. Methane-rich samples were associated with high-salinity, NaCl-type groundwater and elevated levels of ethane, 4 He, and other noble gases produced by radioactive decay. This endmember displayed less negative δ 13 C-CH 4 and evidence of mixing between thermogenic natural gases and hydrogenotrophic methane. Atmospheric noble gases in the methane-rich samples record a history of fractionation during gas-phase migration from source rocks to shallow aquifers. Conversely, methane-poor samples have a paucity of ethane and 4 He, near saturation levels of atmospheric noble gases, and more negative δ 13 C-CH 4 ; methane in these samples is biogenic and produced by a mixture of hydrogenotrophic and acetoclastic sources. These geochemical observations are consistent with other basins targeted for unconventional energy extraction in the USA and contribute to a growing data base of naturally occurring methane in shallow aquifers globally, which provide a framework for evaluating environmental concerns related to unconventional energy development (e.g., stray gas). © 2018, National Ground Water Association.

Microbial Energy Conversion

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

Buckley, Merry; Wall, Judy D.

2006-10-01

The American Academy of Microbiology convened a colloquium March 10-12, 2006, in San Francisco, California, to discuss the production of energy fuels by microbial conversions. The status of research into various microbial energy technologies, the advantages and disadvantages of each of these approaches, research needs in the field, and education and training issues were examined, with the goal of identifying routes for producing biofuels that would both decrease the need for fossil fuels and reduce greenhouse gas emissions. Currently, the choices for providing energy are limited. Policy makers and the research community must begin to pursue a broader array ofmore » potential energy technologies. A diverse energy portfolio that includes an assortment of microbial energy choices will allow communities and consumers to select the best energy solution for their own particular needs. Funding agencies and governments alike need to prepare for future energy needs by investing both in the microbial energy technologies that work today and in the untested technologies that will serve the world’s needs tomorrow. More mature bioprocesses, such as ethanol production from starchy materials and methane from waste digestors, will find applications in the short term. However, innovative techniques for liquid fuel or biohydrogen production are among the longer term possibilities that should also be vigorously explored, starting now. Microorganisms can help meet human energy needs in any of a number of ways. In their most obvious role in energy conversion, microorganisms can generate fuels, including ethanol, hydrogen, methane, lipids, and butanol, which can be burned to produce energy. Alternatively, bacteria can be put to use in microbial fuel cells, where they carry out the direct conversion of biomass into electricity. Microorganisms may also be used some day to make oil and natural gas technologies more efficient by sequestering carbon or by assisting in the recovery of oil and natural gas from the subsurface. The participants discussed--key microbial conversion paths; overarching research issues; current funding models and microbial energy research; education, training, interdisciplinary cooperation and communication. Their recommendations are--Cellulose and lignocellulose are the preferred substrates for producing liquid transportation fuels, of which ethanol is the most commonly considered example. Generating fuels from these materials is still difficult and costly. A number of challenges need to be met in order to make the conversion of cellulose and lignocellulose to transportation fuels more cost-competitive. The design of hydrogen-producing bioreactors must be improved in order to more effectively manage hydrogen removal, oxygen exclusion, and, in the case of photobioreactors, to capture light energy more efficiently. Methane production may be optimized by fine-tuning methanogenic microbial communities. The ability to transfer electrons to an anode in a microbial fuel cell is probably very broadly distributed in the bacterial world. The scientific community needs a larger inventory of cultivated microorganisms from which to draw for energy conversion development. New and unusual organisms for manufacturing fuels and for use in fuel cells can be discovered using bioprospecting techniques. Particular emphasis should be placed on finding microbes, microbial communities, and enzymes that can enhance the conversion of lignocellulosic biomass to usable sugars. Many of the microbial processes critical to energy conversion are carried out by complex communities of organisms, and there is a need to better understand the community interactions that make these transformations possible. Better understanding of microbial community structure, robustness, networks, homeostasis, and cell-to-cell signaling is also needed. A better understanding of the basic enzymology of microorganisms is needed in order to move forward more quickly with microbial energy production. Research should focus on the actions of enzymes and enzyme complexes within the context of the whole cell, how they’re regulated, where they’re placed, and what they interact with. Better modeling tools are needed to facilitate progress in microbial energy transformations. Models of metabolic dynamics, including levels of reductants and regulation of electron flow need to be improved. Global techno-economic models of microbial energy conversion systems, which seek to simultaneously describe the resource flows into and out of a system as well as its economics, are needed and should be made publicly available on the internet. Finally, more emphasis needs to be placed on multidisciplinary education and training and on cooperation between disciplines in order to make the most of microbial energy conversion technologies and to meet the research needs of the future.« less

Lignocellulose-derived thin stillage composition and efficient biological treatment with a high-rate hybrid anaerobic bioreactor system.

PubMed

Oosterkamp, Margreet J; Méndez-García, Celia; Kim, Chang-H; Bauer, Stefan; Ibáñez, Ana B; Zimmerman, Sabrina; Hong, Pei-Ying; Cann, Isaac K; Mackie, Roderick I

2016-01-01

This study aims to chemically characterize thin stillage derived from lignocellulosic biomass distillation residues in terms of organic strength, nutrient, and mineral content. The feasibility of performing anaerobic digestion on these stillages at mesophilic (40 °C) and thermophilic (55 °C) temperatures to produce methane was demonstrated. The microbial communities involved were further characterized. Energy and sugar cane stillage have a high chemical oxygen demand (COD of 43 and 30 g/L, respectively) and low pH (pH 4.3). Furthermore, the acetate concentration in sugar cane stillage was high (45 mM) but was not detected in energy cane stillage. There was also a high amount of lactate in both types of stillage (35-37 mM). The amount of sugars was 200 times higher in energy cane stillage compared to sugar cane stillage. Although there was a high concentration of sulfate (18 and 23 mM in sugar and energy cane stillage, respectively), both thin stillages were efficiently digested anaerobically with high COD removal under mesophilic and thermophilic temperature conditions and with an organic loading rate of 15-21 g COD/L/d. The methane production rate was 0.2 L/g COD, with a methane percentage of 60 and 64, and 92 and 94 % soluble COD removed, respectively, by the mesophilic and thermophilic reactors. Although both treatment processes were equally efficient, there were different microbial communities involved possibly arising from the differences in the composition of energy cane and sugar cane stillage. There was more acetic acid in sugar cane stillage which may have promoted the occurrence of aceticlastic methanogens to perform a direct conversion of acetate to methane in reactors treating sugar cane stillage. Results showed that thin stillage contains easily degradable compounds suitable for anaerobic digestion and that hybrid reactors can efficiently convert thin stillage to methane under mesophilic and thermophilic conditions. Furthermore, we found that optimal conditions for biological treatment of thin stillage were similar for both mesophilic and thermophilic reactors. Bar-coded pyrosequencing of the 16S rRNA gene identified different microbial communities in mesophilic and thermophilic reactors and these differences in the microbial communities could be linked to the composition of the thin stillage.

Rapid solar-thermal decarbonization of methane

NASA Astrophysics Data System (ADS)

Dahl, Jaimee Kristen

Due to the ever-increasing demand for energy and the concern over the environmental impact of continuing to produce energy using current methods, there is interest in developing a hydrogen economy. Hydrogen is a desirable energy source because it is abundant in nature and burns cleanly. One method for producing hydrogen is to utilize a renewable energy source to obtain high enough temperatures to decompose a fossil fuel into its elements. This thesis work is directed at developing a solar-thermal aerosol flow reactor to dissociate methane to carbon black and hydrogen. The technology is intended as a "bridge" between current hydrogen production methods, such as conventional steam-methane reformers, and future "zero emission" technology for producing hydrogen, such as dissociating water using a renewable heating source. A solar furnace is used to heat a reactor to temperatures in excess of 2000 K. The final reactor design studied consists of three concentric vertical tubes---an outer quartz protection tube, a middle solid graphite heating tube, and an inner porous graphite reaction tube. A "fluid-wall" is created on the inside wall of the porous reaction tube in order to prevent deposition of the carbon black co-product on the reactor tube wall. The amorphous carbon black produced aids in heating the gas stream by absorbing radiation from the reactor wall. Conversions of 90% are obtained at a reactor wall temperature of 2100 K and an average residence time of 0.01 s. Computer modeling is also performed to study the gas flow and temperature profiles in the reactor as well as the kinetics of the methane dissociation reaction. The simulations indicate that there is little flow of the fluid-wall gas through the porous wall in the hot zone region, but this can be remedied by increasing the inlet temperature of the fluid-wall gas and/or increasing the tube permeability only in the hot zone region of the wall. The following expression describes the kinetics of methane dissociation in a solar-thermal fluid-wall reactor: dXdt=5.8x108 exp-155,600RT 1-X 7.2s-1. The experimental and theoretical work reported in this thesis is the groundwork that will be utilized in scaling up the reactor to produce hydrogen in distributed or centralized facilities.

Direct use of methane in coal liquefaction

DOEpatents

Sundaram, M.S.; Steinberg, M.

1985-06-19

This invention relates to a process for converting solid carbonaceous material, such as coal, to liquid and gaseous hydrocarbons utilizing methane, generally at a residence time of about 20 to 120 minutes at a temperature of 250 to 750/sup 0/C, preferably 350 to 450/sup 0/C, pressurized up to 6000 psi, and preferably in the 1000 to 2500 psi range, preferably directly utilizing methane 50 to 100% by volume in a mix of methane and hydrogen. A hydrogen donor solvent or liquid vehicle such as tetralin, tetrahydroquinoline, piperidine, and pyrolidine may be used in a slurry mix where the solvent feed is 0 to 100% by weight of the coal or carbonaceous feed. Carbonaceous feed material can either be natural, such as coal, wood, oil shale, petroleum, tar sands, etc., or man-made residual oils, tars, and heavy hydrocarbon residues from other processing systems. 1 fig.

Methane clumped isotopes: Progress and potential for a new isotopic tracer

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

Douglas, Peter M. J.; Stolper, Daniel A.; Eiler, John M.

The isotopic composition of methane is of longstanding geochemical interest, with important implications for understanding hydrocarbon systems, atmospheric greenhouse gas concentrations, the global carbon cycle, and life in extreme environments. Recent analytical developments focusing on multiply substituted isotopologues (‘clumped isotopes’) are opening a potentially valuable new window into methane geochemistry. When methane forms in internal isotopic equilibrium, clumped isotopes can provide a direct record of formation temperature, making this property particularly valuable for identifying different methane origins. However, it has also become clear that in certain settings methane clumped isotope measurements record kinetic rather than equilibrium isotope effects. Here wemore » present a substantially expanded dataset of methane clumped isotope analyses, and provide a synthesis of the current interpretive framework for this parameter. We review different processes affecting methane clumped isotope compositions, describe the relationships between conventional isotope and clumped isotope data, and summarize the types of information that this measurement can provide in different Earth and planetary environments.« less

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

Cyclic process for producing methane with catalyst regeneration

DOEpatents

Frost, Albert C.; Risch, Alan P.

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. For practical commercial operations utilizing the two-step process of the invention of a cyclic basis, nickel, cobalt, ruthenium, thenium and alloys thereof are especially prepared for use in a metal state, with CO disproportionation being carried out at temperatures up to about 350.degree. C. and with the conversion of active surface carbon to methane being carried out by reaction with steam. The catalyst is employed in such cyclic operations without the necessity for employing a regeneration step as part of each processing cycle. Inactive carbon or coke that tends to form on the catalyst over the course of continuous operations utilizing such cyclic process is effectively and advantageously removed, on a periodic basis, in place of conventional burn off with an inert stream containing a low concentration of oxygen.

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.

Methane Emissions from Upland Forests

NASA Astrophysics Data System (ADS)

Megonigal, Patrick; Pitz, Scott; Wang, Zhi-Ping

2016-04-01

Global budgets ascribe 4-10% of atmospheric methane sinks to upland soils and assume that soils are the sole surface for methane exchange between upland forests and the atmosphere. The dogma that upland forests are uniformly atmospheric methane sinks was challenged a decade ago by the discovery of abiotic methane production from plant tissue. Subsequently a variety of relatively cryptic microbial and non-microbial methane sources have been proposed that have the potential to emit methane in upland forests. Despite the accumulating evidence of potential methane sources, there are few data demonstrating actual emissions of methane from a plant surface in an upland forest. We report direct observations of methane emissions from upland tree stems in two temperate forests. Stem methane emissions were observed from several tree species that dominate a forest located on the mid-Atlantic coast of North America (Maryland, USA). Stem emissions occurred throughout the growing season while soils adjacent to the trees simultaneously consumed methane. Scaling fluxes by stem surface area suggested the forest was a net methane source during a wet period in June, and that stem emissions offset 5% of the soil methane sink on an annual basis. High frequency measurements revealed diurnal cycles in stem methane emission rates, pointing to soils as the methane source and transpiration as the most likely pathway for gas transport. Similar observations were made in an upland forest in Beijing, China. However, in this case the evidence suggested the methane was not produced in soils, but in the heartwood by microbial or non-microbial processes. These data challenge the concept that forests are uniform sinks of methane, and suggest that upland forests are smaller methane sinks than previously estimated due to stem emissions. Tree emissions may be particularly important in upland tropical forests characterized by high rainfall and transpiration.

Microcanonical molecular simulations of methane hydrate nucleation and growth: evidence that direct nucleation to sI hydrate is among the multiple nucleation pathways.

PubMed

Zhang, Zhengcai; Walsh, Matthew R; Guo, Guang-Jun

2015-04-14

The results of six high-precision constant energy molecular dynamics (MD) simulations initiated from methane-water systems equilibrated at 80 MPa and 250 K indicate that methane hydrates can nucleate via multiple pathways. Five trajectories nucleate to an amorphous solid. One trajectory nucleates to a structure-I hydrate template with long-range order which spans the simulation box across periodic boundaries despite the presence of several defects. While experimental and simulation data for hydrate nucleation with different time- and length-scales suggest that there may exist multiple pathways for nucleation, including metastable intermediates and the direct formation of the globally-stable phase, this work provides the most compelling evidence that direct formation to the globally stable crystalline phase is one of the multiple pathways available for hydrate nucleation.

Anaerobic digestion of selected Italian agricultural and industrial residues (grape seeds and leather dust): combined methane production and digestate characterization.

PubMed

Caramiello, C; Lancellotti, I; Righi, F; Tatàno, F; Taurino, R; Barbieri, L

2013-01-01

A combined experimental evaluation of methane production (obtained by anaerobic digestion) and detailed digestate characterization (with physical-chemical, thermo-gravimetric and mineralogical approaches) was conducted on two organic substrates, which are specific to Italy (at regional and national levels). One of the substrates was grape seeds, which have an agricultural origin, whereas the other substrate was vegetable-tanned leather dust, which has an industrial origin. Under the assumed experimental conditions of the performed lab-scale test series, the grape seed substrate exhibited a resulting net methane production of 175.0 NmL g volatile solids (VS)(-1); hence, it can be considered as a potential energy source via anaerobic digestion. Conversely, the net methane production obtained from the anaerobic digestion of the vegetable-tanned leather dust substrate was limited to 16.1 NmL gVS(-1). A detailed characterization of the obtained digestates showed that there were both nitrogen-containing compounds and complex organic compounds present in the digestate that was obtained from the mixture of leather dust and inoculum. As a general perspective of this experimental study, the application of diversified characterization analyzes could facilitate (1) a better understanding of the main properties of the obtained digestates to evaluate their potential valorization, and (2) a combination of the digestate characteristics with the corresponding methane productions to comprehensively evaluate the bioconversion process.

Water-Gas Shift and Methane Reactivity on Reducible Perovskite-Type Oxides

PubMed Central

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

Stable isotope tracing of anaerobic methane oxidation in the gassy sediments of Eckernfoerde Bay, German Baltic Sea

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

Martens, C.S.; Albert, D.B.; Alperin, M.J.

Methane concentrations in the pore waters of Eckernfoerde Bay in the German Baltic Sea generally reach gas bubble saturation values within the upper meter of the sediment column. The depth at which saturation occurs is controlled by a balance between rates of methane production, consumption (oxidation), and transport. The relative importance of anaerobic methane oxidation (AMO) in controlling dissolved and gas bubble methane distributions in the bay's sediments is indirectly revealed through methane concentration versus depth profiles, depth variations in the stable C and H isotope composition of methane, and the C isotope composition of total dissolved inorganic carbon ({Sigma}CO{submore » 2}). Direct radiotracer measurements indicate that AMO rates of over 15 mM/yr are focused at the base of the sulfate reduction zone. Diagenetic equations that describe the depth destructions of the {delta}{sup 13}C and {delta}D values of methane reproduce isotopic shifts observed throughout the methane oxidation zone and are best fit with kinetic isotope fractionation factors of 1.012 {+-} 0.001 and 1.120 {plus{underscore}minus} 0.020 respectively.« less

Probing methane hydrate nucleation through the forward flux sampling method.

PubMed

Bi, Yuanfei; Li, Tianshu

2014-11-26

Understanding the nucleation of hydrate is the key to developing effective strategies for controlling methane hydrate formation. Here we present a computational study of methane hydrate nucleation, by combining the forward flux sampling (FFS) method and the coarse-grained water model mW. To facilitate the application of FFS in studying the formation of methane hydrate, we developed an effective order parameter λ on the basis of the topological analysis of the tetrahedral network. The order parameter capitalizes the signature of hydrate structure, i.e., polyhedral cages, and is capable of efficiently distinguishing hydrate from ice and liquid water while allowing the formation of different hydrate phases, i.e., sI, sII, and amorphous. Integration of the order parameter λ with FFS allows explicitly computing hydrate nucleation rates and obtaining an ensemble of nucleation trajectories under conditions where spontaneous hydrate nucleation becomes too slow to occur in direct simulation. The convergence of the obtained hydrate nucleation rate was found to depend crucially on the convergence of the spatial distribution for the spontaneously formed hydrate seeds obtained from the initial sampling of FFS. The validity of the approach is also verified by the agreement between the calculated nucleation rate and that inferred from the direct simulation. Analyzing the obtained large ensemble of hydrate nucleation trajectories, we show hydrate formation at 220 K and 500 bar is initiated by the nucleation events occurring in the vicinity of water-methane interface, and facilitated by a gradual transition from amorphous to crystalline structure. The latter provides the direct support to the proposed two-step nucleation mechanism of methane hydrate.

NOTE: Laboratory Studies of Catalysis of CO to Organics on Grain Analogs

NASA Astrophysics Data System (ADS)

Ferrante, R. F.; Moore, M. H.; Nuth, J. A.; Smith, T.

2000-05-01

Experiments simulating heterogeneous conversion of H 2 and CO into simple hydrocarbons in astrophysical environments have been performed, utilizing realistic cosmic grain analogs of Fe-doped silicates as Fischer-Tropsch-Type catalysts. Catalysis was studied for temperatures from 470-670 K and reactant gas mixtures of H 2/CO with a ratio of 2-100. The total gas pressure was near 0.5 bar. Maximum conversion rates of a few percentage points were achieved over a 3-h time period. Major products were methane, ethane, ethylene, carbon dioxide, and water. Products were identified by IR spectroscopy.

Emerging Methane Sources: A Bang or Whimper? (Invited)

NASA Astrophysics Data System (ADS)

Harriss, R. C.

2013-12-01

In this presentation we examine two emerging methane emission sources that may further accelerate climate change in the 21st century: 1) Will fugitive methane emissions associated with the development of unconventional natural gas resources pose a significant threat of accelerating climate change? 2) Will continued warming of Arctic regions destabilize permafrost and methane hydrates rapidly increasing global atmospheric methane that results in a catastrophic climate change emergency? These risks are currently described in two different guises, with unconventional gas as persistent and gradually unfolding threat and Arctic rapid warming and release of methane as a low-probability event that could in an instant change everything. Current research is far from answering the question of whether these emerging methane sources will lead to a climate change bang or whimper. Both issues reflect the need to understand complex environmental and engineered systems as they interact with social and economic forces. While the evolution of energy systems favors methane as a contemporary transition fuel, researchers and practitioners need to address the fugitive methane leakage, reliability, and safety of natural gas systems. The concept of a methane bridge as a viable direction to decarbonization is appealing; it's just not as big or fast a step as many scientists want.

Methane emission during municipal wastewater treatment.

PubMed

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.

Perovskite nanocomposites as effective CO2-splitting agents in a cyclic redox scheme

PubMed Central

Zhang, Junshe; Haribal, Vasudev; Li, Fanxing

2017-01-01

We report iron-containing mixed-oxide nanocomposites as highly effective redox materials for thermochemical CO2 splitting and methane partial oxidation in a cyclic redox scheme, where methane was introduced as an oxygen “sink” to promote the reduction of the redox materials followed by reoxidation through CO2 splitting. Up to 96% syngas selectivity in the methane partial oxidation step and close to complete conversion of CO2 to CO in the CO2-splitting step were achieved at 900° to 980°C with good redox stability. The productivity and production rate of CO in the CO2-splitting step were about seven times higher than those in state-of-the-art solar-thermal CO2-splitting processes, which are carried out at significantly higher temperatures. The proposed approach can potentially be applied for acetic acid synthesis with up to 84% reduction in CO2 emission when compared to state-of-the-art processes. PMID:28875171

The effect of a combined biological and thermo-mechanical pretreatment of wheat straw on energy yields in coupled ethanol and methane generation.

PubMed

Theuretzbacher, Franz; Blomqvist, Johanna; Lizasoain, Javier; Klietz, Lena; Potthast, Antje; Horn, Svein Jarle; Nilsen, Paal J; Gronauer, Andreas; Passoth, Volkmar; Bauer, Alexander

2015-10-01

Ethanol and biogas are energy carriers that could contribute to a future energy system independent of fossil fuels. Straw is a favorable bioenergy substrate as it does not compete with food or feed production. As straw is very resistant to microbial degradation, it requires a pretreatment to insure efficient conversion to ethanol and/or methane. This study investigates the effect of combining biological pretreatment and steam explosion on ethanol and methane yields in order to improve the coupled generation process. Results show that the temperature of the steam explosion pretreatment has a particularly strong effect on possible ethanol yields, whereas combination with the biological pretreatment showed no difference in overall energy yield. The highest overall energy output was found to be 10.86 MJ kg VS(-1) using a combined biological and steam explosion pretreatment at a temperature of 200°C. Copyright © 2015 Elsevier Ltd. All rights reserved.

Promotional Effects of In on Non-Oxidative Methane Transformation Over Mo-ZSM-5

DOE PAGES

Zhang, Yang; Kidder, Michelle; Ruther, Rose E.; ...

2016-08-16

In this paper, we present a new class of catalysts, InMo-ZSM- 5, which can be prepared by indium impregnation of Mo-ZSM- 5. The incorporation of indium dramatically decreases coke formation during methane dehydroaromatization. The benzene and C 2 hydrocarbons selectivity among total hydrocarbons over InMo-ZSM- 5 remains comparable to that of Mo-ZSM- 5 despite reduced methane conversion due to decreased coke formation. We found 1 wt% indium to be optimal loading for reducing coke selectivity to half that of Mo-ZSM- 5. Characterization methods were not helpful in discerning the interaction of In with Mo but experiments with bimetallic 1In2Mo-ZSM- 5more » and mechanical mixture 1In+2Mo-ZSM- 5 suggest that In and Mo need to be in close proximity to suppress coke formation. Finally, this is supported by temperature programmed reduction experiments which show that In incorporation leads to lower Mo reduction temperature in In2Mo-ZMS- 5.« less

Hydrogen and carbon nanotube production via catalytic decomposition of methane

NASA Astrophysics Data System (ADS)

Deniz, Cansu; Karatepe, Nilgün

2013-09-01

The future energy demand is expected to increase significantly due to an increasing world population and demands for higher standards of living and better air quality. Hydrogen is considered as an energy carrier because of its high conversion efficiency and low pollutant emissions. It can be produced from various sources and transformed into electricity and other energy forms with a low pollution. The catalytic decomposition of hydrocarbon has been seen as a really useful method for production of pure hydrogen and for the environmental concern. The objective of this study was to assess the impact of catalyst composition and processing parameters on COx-free hydrogen production and to produce an available solid form of co-product carbon as carbon nanotubes via catalytic decomposition of methane. The optimum experimental conditions for methane decomposition have been investigated. Fe, Co and Ni are used as catalysts (nano materials) over different substrates as SiO2 and MgO to produce hydrogen at optimum temperatures.

Effects of enzymatic hydrolysis and ultrasounds pretreatments on corn cob and vine trimming shoots for biogas production.

PubMed

Pérez-Rodríguez, N; García-Bernet, D; Domínguez, J M

2016-12-01

Due to their lignocellulosic nature, corn cob and vine trimming shoots (VTS) could be valorized by anaerobic digestion for biogas production. To enhance the digestibility of substrates, pretreatments of lignocellulosic materials are recommended. The effect of enzymatic hydrolysis, ultrasounds pretreatments (US) and the combination of both was assayed in lignocellulosic composition, methane, and biogas yields. The pretreatments leaded to a reduction in lignin and an increase in neutral detergent soluble compounds making corn cob and VTS more amendable for biogas conversion. The US were negative for biogas production from both substrates and in particular strongly detrimental for VTS. On the opposite side, the enzymatic hydrolysis was certainly beneficial increasing 59.8% and 14.6% the methane production from VTS and corn cob, respectively. The prior application of US did not potentiate (or not sufficiently) the improvement in the methane production reflected by the enzymatic hydrolysis pretreatment of VTS and corn cob. Copyright © 2016 Elsevier Ltd. All rights reserved.

New Ni-based quaternary disk-shaped catalysts for low-temperature CO2 methanation: Fabrication, characterization, and performance.

PubMed

Moon, Dea Hyun; Lee, Sang Moon; Ahn, Jeong Yoon; Nguyen, Dinh Duc; Kim, Sung Su; Chang, Soon Woong

2018-07-15

Ni-based quaternary disk catalysts were manufactured for low-temperature CO 2 methanation reactions, and the reaction activity was examined with respect to the thermal treatment conditions. By applying varying reduction and combustion treatments, the same catalysts were compared, and the Ni oxidation conditions and physical features were confirmed through X-Ray diffraction, scanning electron microscopy, and energy dispersive X-ray analyses. In addition, oxygen adsorption/desorption changes were measured by temperature-programmed reduction after pre-treating with oxygen and hydrogen. The reduction treatment catalyst showed a conversion of 20% at 280 °C, and the 70% calcined catalyst did not form a NiO crystalloid. The activation of the catalyst increased because of NiO movement on the catalyst surface, which enabled easy transformation to metallic Ni. The prepared catalyst is a highly reactive, yet stable, candidate for practical catalytic CO 2 methanation. Copyright © 2018 Elsevier Ltd. All rights reserved.

Thermo-electrochemical production of compressed hydrogen from methane with near-zero energy loss

NASA Astrophysics Data System (ADS)

Malerød-Fjeld, Harald; Clark, Daniel; Yuste-Tirados, Irene; Zanón, Raquel; Catalán-Martinez, David; Beeaff, Dustin; Morejudo, Selene H.; Vestre, Per K.; Norby, Truls; Haugsrud, Reidar; Serra, José M.; Kjølseth, Christian

2017-11-01

Conventional production of hydrogen requires large industrial plants to minimize energy losses and capital costs associated with steam reforming, water-gas shift, product separation and compression. Here we present a protonic membrane reformer (PMR) that produces high-purity hydrogen from steam methane reforming in a single-stage process with near-zero energy loss. We use a BaZrO3-based proton-conducting electrolyte deposited as a dense film on a porous Ni composite electrode with dual function as a reforming catalyst. At 800 °C, we achieve full methane conversion by removing 99% of the formed hydrogen, which is simultaneously compressed electrochemically up to 50 bar. A thermally balanced operation regime is achieved by coupling several thermo-chemical processes. Modelling of a small-scale (10 kg H2 day-1) hydrogen plant reveals an overall energy efficiency of >87%. The results suggest that future declining electricity prices could make PMRs a competitive alternative for industrial-scale hydrogen plants integrating CO2 capture.

Characterization of Carbon Particulates in the Exit Flow of a Plasma Pyrolysis Assembly (PPA) Reactor

NASA Technical Reports Server (NTRS)

Green, Robert D.; Meyer, Marit E.; Agui, Juan H.; Berger, Gordon M.; Vijayakumar, R.; Abney, Morgan B.; Greenwood, Zachary

2015-01-01

The ISS presently recovers oxygen from crew respiration via a Carbon Dioxide Reduction Assembly (CRA) that utilizes the Sabatier chemical process to reduce captured carbon dioxide to methane (CH4) and water. In order to recover more of the hydrogen from the methane and increase oxygen recovery, NASA Marshall Space Flight Center (MSFC) is investigating a technology, plasma pyrolysis, to convert the methane to acetylene. The Plasma Pyrolysis Assembly (or PPA), achieves 90% or greater conversion efficiency, but a small amount of solid carbon particulates are generated as a side product and must be filtered before the acetylene is removed and the hydrogen-rich gas stream is recycled back to the CRA. In this work, we present the experimental results of an initial characterization of the carbon particulates in the PPA exit gas stream. We also present several potential options to remove these carbon particulates via carbon traps and filters to minimize resupply mass and required downtime for regeneration.

Direct conversion of CO2 into liquid fuels with high selectivity over a bifunctional catalyst.

PubMed

Gao, Peng; Li, Shenggang; Bu, Xianni; Dang, Shanshan; Liu, Ziyu; Wang, Hui; Zhong, Liangshu; Qiu, Minghuang; Yang, Chengguang; Cai, Jun; Wei, Wei; Sun, Yuhan

2017-10-01

Although considerable progress has been made in carbon dioxide (CO 2 ) hydrogenation to various C 1 chemicals, it is still a great challenge to synthesize value-added products with two or more carbons, such as gasoline, directly from CO 2 because of the extreme inertness of CO 2 and a high C-C coupling barrier. Here we present a bifunctional catalyst composed of reducible indium oxides (In 2 O 3 ) and zeolites that yields a high selectivity to gasoline-range hydrocarbons (78.6%) with a very low methane selectivity (1%). The oxygen vacancies on the In 2 O 3 surfaces activate CO 2 and hydrogen to form methanol, and C-C coupling subsequently occurs inside zeolite pores to produce gasoline-range hydrocarbons with a high octane number. The proximity of these two components plays a crucial role in suppressing the undesired reverse water gas shift reaction and giving a high selectivity for gasoline-range hydrocarbons. Moreover, the pellet catalyst exhibits a much better performance during an industry-relevant test, which suggests promising prospects for industrial applications.

Performance and microbial community analysis of the anaerobic reactor with coke oven gas biomethanation and in situ biogas upgrading.

PubMed

Wang, Wen; Xie, Li; Luo, Gang; Zhou, Qi; Angelidaki, Irini

2013-10-01

A new method for simultaneous coke oven gas (COG) biomethanation and in situ biogas upgrading in anaerobic reactor was developed in this study. The simulated coke oven gas (SCOG) (92% H2 and 8% CO) was injected directly into the anaerobic reactor treating sewage sludge through hollow fiber membrane (HFM). With pH control at 8.0, the added H2 and CO were fully consumed and no negative effects on the anaerobic degradation of sewage sludge were observed. The maximum CH4 content in the biogas was 99%. The addition of SCOG resulted in enrichment and dominance of homoacetogenetic genus Treponema and hydrogenotrophic genus Methanoculleus in the liquid, which indicated that H2 were converted to methane by both direct (hydrogenotrophic methanogenesis) and indirect (homoacetogenesis+aceticlastic methanogenesis) pathways in the liquid. However, the aceticlasitic genus Methanosaeta was dominant for archaea in the biofilm on the HFM, which indicated indirect (homoacetogenesis+aceticlastic methanogenesis) H2 conversion pathway on the biofilm. Copyright © 2013 Elsevier Ltd. All rights reserved.

Direct methane solid oxide fuel cells and their related applications

NASA Astrophysics Data System (ADS)

Lin, Yuanbo

Solid oxide fuel cells (SOFCs), renowned for their high electrical generation efficiency with low pollutant production, are promising for reducing global energy and environmental concerns. However, there are major barriers for SOFC commercialization. A primary challenge is reducing the capital cost of SOFC power plants to levels that can compete with other generation methods. While the focus of this thesis research was on operation of SOFCs directly with methane fuel, the underlying motivation was to make SOFCs more competitive by reducing their cost. This can be achieved by making SOFCs that reduce the size and complexity of the required "balance of plant". Firstly, direct operation of SOFCs on methane is desirable since it can eliminate the external reformer. However, effective means must be found to suppress deleterious anode coking in methane. In this thesis, the operating conditions under which SOFCs can operate stably and without anode coking were investigated in detail, and the underlying mechanisms of coking and degradation were determined. Furthermore, a novel design utilizing an inert anode barrier layer was developed and shown to substantially improve stability against coking. Secondly, the direct methane SOFCs were investigated for use as electrochemical partial oxidation (EPOx) reactors that can co-generate electricity and synthesis gas (CO+H2) from methane. The results indicated that conventional SOFCs work quite well as methane partial oxidation reactors, producing syngas at relatively high rates. While this approach would not decrease the cost of SOFC power plant, it would improve prospects for commercialization by increasing the value of the power plant, because two products, electricity and syngas, can be sold. Thirdly, SOFCs utilizing thin (La,Sr)(Ga,Mg)O3 electrolytes were demonstrated. This highly conductive material allows lower SOFC operation temperature, leading to the use of lower-cost materials for sealing, interconnection, and balance of plant. Deleterious electrolyte/electrode reactions and electrolyte La loss were avoided during high-temperature co-firing by using thin La-doped ceria barrier layers, allowing very high power densities at moderate operating temperatures. (La,Sr)(Ga,Mg)O3-(La,Sr)(Fe,Co)O3 composite cathodes were investigated and optimal processing parameters that yield low interfacial polarization resistance at intermediate temperature were determined.

Anaerobic Digestion.

PubMed

Liebetrau, Jan; Sträuber, Heike; Kretzschmar, Jörg; Denysenko, Velina; Nelles, Michael

2017-04-09

The term anaerobic digestion usually refers to the microbial conversion of organic material to biogas, which mainly consists of methane and carbon dioxide. The technical application of the naturally-occurring process is used to provide a renewable energy carrier and - as the substrate is often waste material - to reduce the organic matter content of the substrate prior to disposal.Applications can be found in sewage sludge treatment, the treatment of industrial and municipal solid wastes and wastewaters (including landfill gas utilization), and the conversion of agricultural residues and energy crops.For biorefinery concepts, the anaerobic digestion (AD) process is, on the one hand, an option to treat organic residues from other production processes. Concomitant effects are the reduction of organic carbon within the treated substance, the conversion of nitrogen and sulfur components, and the production of an energy-rich gas - the biogas. On the other hand, the multistep conversion of complex organic material offers the possibility of interrupting the conversion chain and locking out intermediates for utilization as basic material within the chemical industry.

Anaerobic digestion of municipal solid waste: Utility of process residues as a soil amendment

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

Rivard, C.J.; Nagle, N.J.; Kay, B.D.

1995-12-31

Tuna processing wastes (sludges high in fat, oil, and grease [FOG]) and municipal solid waste (MSW) generated on Tutuila Island, American Samoa, represent an ongoing disposal challenge. The biological conversion of the organic fraction of these wastes to useful products, including methane and fertilizer-grade residue, through anaerobic high-solids digestion is currently in scale-up development. The suitability of the anaerobic digestion residues as a soil amendment was evaluated through extensive chemical analysis and greenhouse studies using corn as an indicator crop. Additionally, native Samoan soil was used to evaluate the specific application rates for the compost. Experiments established that anaerobic residuesmore » increase crop yields in direct proportion to increases in the application rate. Additionally, nutrient saturation was not demonstrated within the range of application rates evaluated for the Samoan soil. Beyond nutrient supplementation, organic residue amendment to Samoan soil imparts enhanced water and nutrient-binding capacities.« less

A review on bio-electrochemical systems (BESs) for the syngas and value added biochemicals production.

PubMed

Kumar, Gopalakrishnan; Saratale, Rijuta Ganesh; Kadier, Abudukeremu; Sivagurunathan, Periyasamy; Zhen, Guangyin; Kim, Sang-Hyoun; Saratale, Ganesh Dattatraya

2017-06-01

Bio-electrochemical systems (BESs) are the microbial systems which are employed to produce electricity directly from organic wastes along with some valuable chemicals production such as medium chain fatty acids; acetate, butyrate and alcohols. In this review, recent updates about value-added chemicals production concomitantly with the production of gaseous fuels like hydrogen and methane which are considered as cleaner for the environment have been addressed. Additionally, the bottlenecks associated with the conversion rates, lower yields and other aspects have been mentioned. In spite of its infant stage development, this would be the future trend of energy, biochemicals and electricity production in greener and cleaner pathway with the win-win situation of organic waste remediation. Henceforth, this review intends to summarise and foster the progress made in the BESs and discusses its challenges and outlook on future research advances. Copyright © 2017 Elsevier Ltd. All rights reserved.

Development of methane conversion factor models for Zebu beef cattle fed low-quality crop residues and by-products in tropical regions.

PubMed

Kaewpila, Chatchai; Sommart, Kritapon

2016-10-01

The enteric methane conversion factor ( Y m ) is an important country-specific value for the provision of precise enteric methane emissions inventory reports. The objectives of this meta-analysis were to develop and evaluate the empirical Y m models for the national level and the farm level for tropical developing countries according to the IPCC's categorization. We used datasets derived from 18 in vivo feeding experiments from 1999 to 2015 of Zebu beef cattle breeds fed low-quality crop residues and by-products. We found that the observed Y m value was 8.2% gross energy (GE) intake (~120 g methane emission head -1  day -1 ) and ranged from 4.8% to 13.7% GE intake. The IPCC default model (tier 2, Y m  = 6.5% ± 1.0% GE intake) underestimated the Y m values by up to 26.1% compared with its refinement of 8.4% ± 0.4% GE intake for the national-level estimate. Both the IPCC default model and the refined model performed worse in predicting Y m trends at the farm level (root mean square prediction error [MSPE] = 15.1%-23.1%, concordance correlation coefficient [CCC] = 0.16-0.18, R 2  = .32). Seven of the extant Y m models based on a linear regression approach also showed inaccurately estimated Y m values (root MSPE = 16.2%-36.0%, CCC = 0.02-0.27, R 2  < .37). However, one of the developed models, which related to the complexity of the energy use efficiencies of the diet consumed to Y m , showed adequate accuracy at the farm level (root MSPE = 9.1%, CCC = 0.75, R 2  = .67). Our results thus suggest a new Y m model and future challenges for estimating Zebu beef cattle production in tropical developing countries.

Enhancing methane production from food waste fermentate using biochar: the added value of electrochemical testing in pre-selecting the most effective type of biochar.

PubMed

Cruz Viggi, Carolina; Simonetti, Serena; Palma, Enza; Pagliaccia, Pamela; Braguglia, Camilla; Fazi, Stefano; Baronti, Silvia; Navarra, Maria Assunta; Pettiti, Ida; Koch, Christin; Harnisch, Falk; Aulenta, Federico

2017-01-01

Recent studies have suggested that addition of electrically conductive biochar particles is an effective strategy to improve the methanogenic conversion of waste organic substrates, by promoting syntrophic associations between acetogenic and methanogenic organisms based on interspecies electron transfer processes. However, the underlying fundamentals of the process are still largely speculative and, therefore, a priori identification, screening, and even design of suitable biochar materials for a given biotechnological process are not yet possible. Here, three charcoal-like products (i.e., biochars) obtained from the pyrolysis of different lignocellulosic materials, (i.e., wheat bran pellets, coppiced woodlands, and orchard pruning) were tested for their capacity to enhance methane production from a food waste fermentate. In all biochar-supplemented (25 g/L) batch experiments, the complete methanogenic conversion of fermentate volatile fatty acids proceeded at a rate that was up to 5 times higher than that observed in the unamended (or sand-supplemented) controls. Fluorescent in situ hybridization analysis coupled with confocal laser scanning microscopy revealed an intimate association between archaea and bacteria around the biochar particles and provided a clear indication that biochar also shaped the composition of the microbial consortium. Based on the application of a suite of physico-chemical and electrochemical characterization techniques, we demonstrated that the positive effect of biochar is directly related to the electron-donating capacity (EDC) of the material, but is independent of its bulk electrical conductivity and specific surface area. The latter properties were all previously hypothesized to play a major role in the biochar-mediated interspecies electron transfer process in methanogenic consortia. Collectively, these results of this study suggest that for biochar addition in anaerobic digester operation, the screening and identification of the most suitable biochar material should be based on EDC determination, via simple electrochemical tests.

Organics in hydrothermal fluids from ultramafics on the Mid-Atlantic Ridge (MAR) - Abiogenic and/or biogenic origin?

NASA Astrophysics Data System (ADS)

Charlou, J.; Donval, J.; Fouquet, Y.; Jean-Baptiste, P.; Dehairs, F.; Holm, N.; Godfroy, A.

2005-12-01

Between 12°N and the Azores Triple Junction along the MAR, CH4 anomalies over axial ultramafic sites are common and point to the association of high or low temperature hydrothermal activity and mantle degassing indicative of ongoing serpentinization process. The general occurrence of isotopically-heavy methane shows the possible abiogenic synthesis of hydrocarbons in hydrothermal systems. The abiogenic formation of CH4 and more complex organic compounds is related to the process of serpentinization of mantellic rocks. Three sites (Logachev, 14°45'N; Rainbow, 36°14'N; Lost City Field, 30°N) are known on the MAR. New fresh fluids were recently sampled at Rainbow and Lost City by the French ROV-Victor during EXOMAR cruise (July 24 to August 28, 2005). The Rainbow and Lost City fluids issued from contrasted ultramafic environments are both enriched in H2, CH4 and hydrocarbons. Hydrogen gas represents more than 40 per cent total gas volume extracted from fluids. SPME (Solid Phase Micro-Extraction) and SBSE (Stir-Bar Sorptive Extraction) extraction techniques were used on board for organic recovery and the analysis was performed on shore by direct GC/MS or by Thermo-Desorption/GC/MS. The hydration of olivine and pyroxen minerals with conversion of Fe(II) to Fe(III) in magnetite during serpentinization leads to production of H2 and conversion of dissolved CO2 to reduced-C species including methane, ethane, propane. In addition heavier straight chain hydrocarbons as alcohols, aldehydes, ketones, aromatics, and cyclic compounds are identified at Rainbow. These compounds may be generated in ultramafic rocks through catalytic reactions (Fischer-Tropsch type reactions), but a biogenic contribution cannot be excluded. Abiogenic organic compounds may be produced from crystalline basement, from volcanic structures, from riftogenic zones and probably from sedimented margins.

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

PubMed

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.

Methane flux from coastal salt marshes

NASA Technical Reports Server (NTRS)

Bartlett, K. B.; Harriss, R. C.; Sebacher, D. I.

1985-01-01

It is thought that biological methanogenesis in natural and agricultural wetlands and enteric fermentation in animals are the dominant sources of global tropospheric methane. It is pointed out that the anaerobic soils and sediments, where methanogenesis occurs, predominate in coastal marine wetlands. Coastal marine wetlands are generally believed to be approximately equal in area to freshwater wetlands. For this reason, coastal marine wetlands may be a globally significant source of atmospheric methane. The present investigation is concerned with the results of a study of direct measurements of methane fluxes to the atmosphere from salt marsh soils and of indirect determinations of fluxes from tidal creek waters. In addition, measurements of methane distributions in coastal marine wetland sediments and water are presented. The results of the investigation suggest that marine wetlands provide only a minor contribution to atmospheric methane on a global scale.

Preparation of a Ni-MgO-Al2O3 catalyst with high activity and resistance to potassium poisoning during direct internal reforming of methane in molten carbonate fuel cells

NASA Astrophysics Data System (ADS)

Jang, Won-Jun; Jung, You-Shick; Shim, Jae-Oh; Roh, Hyun-Seog; Yoon, Wang Lai

2018-02-01

Steam reforming of methane (SRM) is conducted using a series of Ni-MgO-Al2O3 catalysts for direct internal reforming (DIR) in molten carbonate fuel cells (MCFCs). Ni-MgO-Al2O3 catalysts are prepared by the homogeneous precipitation method with a variety of MgO loading amounts ranging from 3 to 15 wt%. In addition, each precursor concentrations are systemically changed (Ni: 1.2-4.8 mol L-1; Mg: 0.3-1.2 mol L-1; Al: 0.4-1.6 mol L-1) at the optimized composition (10 wt% MgO). The effects of MgO loading and precursor concentration on the catalytic performance and resistance against poisoning of the catalyst by potassium (K) are investigated. The Ni-MgO-Al2O3 catalyst with 10 wt% MgO and the original precursor concentration (Ni: 1.2 mol L-1; Mg: 0.3 mol L-1; Al: 0.4 mol L-1) exhibits the highest CH4 conversion and resistance against K poisoning even at the extremely high gas space velocity (GHSV) of 1,512,000 h-1. Excellent SRM performance of the Ni-MgO-Al2O3 catalyst is attributed to strong metal (Ni) to alumina support interaction (SMSI) when magnesium oxide (MgO) is co-precipitated with the Ni-Al2O3. The enhanced interaction of the Ni with MgO-Al2O3 support is found to protect the active Ni species against K poisoning.

Direct multitrait selection realizes the highest genetic response for ratio traits.

PubMed

Zetouni, L; Henryon, M; Kargo, M; Lassen, J

2017-05-01

For a number of traits the phenotype considered to be the goal trait is a combination of 2 or more traits, like methane (CH) emission (CH/kg of milk). Direct selection on CH4 emission defined as a ratio is problematic, because it is uncertain whether the improvement comes from an improvement in milk yield, a decrease in CH emission or both. The goal was to test different strategies on selecting for 2 antagonistic traits- improving milk yield while decreasing methane emissions. The hypothesis was that to maximize genetic gain for a ratio trait, the best approach is to select directly for the component traits rather than using a ratio trait or a trait where 1 trait is corrected for the other as the selection criteria. Stochastic simulation was used to mimic a dairy cattle population. Three scenarios were tested, which differed in selection criteria but all selecting for increased milk yield: 1) selection based on a multitrait approach using the correlation structure between the 2 traits, 2) the ratio of methane to milk and 3) gross methane phenotypically corrected for milk. Four correlation sets were tested in all scenarios, to access robustness of the results. An average genetic gain of 66 kg of milk per yr was obtained in all scenarios, but scenario 1 had the best response for decreased methane emissions, with a genetic gain of 24.8 l/yr, while scenarios 2 and 3 had genetic gains of 27.1 and 27.3 kg/yr. The results found were persistent across correlation sets. These results confirm the hypothesis that to obtain the highest genetic gain a multitrait selection is a better approach than selecting for the ratio directly. The results are exemplified for a methane and milk scenario but can be generalized to other situations where combined traits need to be improved.

Development of Carbon and Sulphur Tolerant Anodes of Solid Oxide Fuel Cells

DTIC Science & Technology

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

Analysis of biomass and waste gasification lean syngases combustion for power generation using spark ignition engines.

PubMed

Marculescu, Cosmin; Cenuşă, Victor; Alexe, Florin

2016-01-01

The paper presents a study for food processing industry waste to energy conversion using gasification and internal combustion engine for power generation. The biomass we used consisted in bones and meat residues sampled directly from the industrial line, characterised by high water content, about 42% in mass, and potential health risks. Using the feedstock properties, experimentally determined, two air-gasification process configurations were assessed and numerically modelled to quantify the effects on produced syngas properties. The study also focused on drying stage integration within the conversion chain: either external or integrated into the gasifier. To comply with environmental regulations on feedstock to syngas conversion both solutions were developed in a closed system using a modified down-draft gasifier that integrates the pyrolysis, gasification and partial oxidation stages. Good quality syngas with up to 19.1% - CO; 17% - H2; and 1.6% - CH4 can be produced. The syngas lower heating value may vary from 4.0 MJ/Nm(3) to 6.7 MJ/Nm(3) depending on process configuration. The influence of syngas fuel properties on spark ignition engines performances was studied in comparison to the natural gas (methane) and digestion biogas. In order to keep H2 molar quota below the detonation value of ⩽4% for the engines using syngas, characterised by higher hydrogen fraction, the air excess ratio in the combustion process must be increased to [2.2-2.8]. The results in this paper represent valuable data required by the design of waste to energy conversion chains with intermediate gas fuel production. The data is suitable for Otto engines characterised by power output below 1 MW, designed for natural gas consumption and fuelled with low calorific value gas fuels. Copyright © 2015 Elsevier Ltd. All rights reserved.

A comparison of methane emissions following rice paddies conversion to crab-fish farming wetlands in southeast China.

PubMed

Hu, Zhiqiang; Wu, Shuang; Ji, Cheng; Zou, Jianwen; Zhou, Quansuo; Liu, Shuwei

2016-01-01

Rice paddies and aquaculture wetlands are typical agricultural wetlands that constitute one of the important sources of atmospheric methane (CH4). Traditional transplanted rice paddies have been experiencing conversion to pond aquaculture wetlands for pursuing higher economic benefits over the past decades in southeast China. A parallel field experiment was carried out to compare CH4 emissions from a transplanted rice paddy and its converted crab-fish farming wetland in southeast China. Over the rice-growing season, CH4 fluxes averaged 1.86 mg m(-2) h(-1) from rice paddies, and 1.14 and 0.50 mg m(-2) h(-1) for the treatments with or without aquatic vegetation present in the crab-fish farming wetlands, respectively. When averaged across the treatments, seasonal CH4 emissions from crab-fish framing wetlands were 52% lower than those from rice paddies. The CH4 fluxes were negatively related to water dissolved oxygen (DO) concentration but positively related to soil/sediment dissolved organic carbon (DOC) content in crab-fish farming wetlands. Dependence of CH4 fluxes on DO or DOC was intensified by the aquatic vegetation presence. By extrapolating the present CH4 emission rate with the current rice paddy-converted aquaculture cultivation area, the seasonal CH4 emissions from inland aquaculture wetlands during the critical farming stage (20 June to 18 October) were estimated to be 33.6 Gg ha(-1) in southeast China in 2012. Rice paddies conversion to crab-fish farming wetlands might have reduced CH4 emissions by 22-54% in mainland China. Results of this study suggest that the conversion of transplanted rice paddies to crab-fish aquaculture wetlands for higher economic benefits would also lead to a lower ecosystem CH4 release rate.

40 CFR 86.094-2 - Definitions.

Code of Federal Regulations, 2013 CFR

2013-07-01

... methane. Non-Methane Hydrocarbon Equivalent means the sum of the carbon mass emissions of non-oxygenated... Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF... Loaded Vehicle Weight means the numerical average of vehicle curb weight and GVWR. Bi-directional control...

40 CFR 86.094-2 - Definitions.

Code of Federal Regulations, 2012 CFR

2012-07-01

... methane. Non-Methane Hydrocarbon Equivalent means the sum of the carbon mass emissions of non-oxygenated... Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF... Loaded Vehicle Weight means the numerical average of vehicle curb weight and GVWR. Bi-directional control...

40 CFR 86.094-2 - Definitions.

Code of Federal Regulations, 2011 CFR

2011-07-01

... methane. Non-Methane Hydrocarbon Equivalent means the sum of the carbon mass emissions of non-oxygenated... Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF... Loaded Vehicle Weight means the numerical average of vehicle curb weight and GVWR. Bi-directional control...

40 CFR 86.094-2 - Definitions.

Code of Federal Regulations, 2010 CFR

2010-07-01

... methane. Non-Methane Hydrocarbon Equivalent means the sum of the carbon mass emissions of non-oxygenated... Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF... Loaded Vehicle Weight means the numerical average of vehicle curb weight and GVWR. Bi-directional control...

40 CFR 86.094-2 - Definitions.

Code of Federal Regulations, 2014 CFR

2014-07-01

... methane. Non-Methane Hydrocarbon Equivalent means the sum of the carbon mass emissions of non-oxygenated... Protection of Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF... Loaded Vehicle Weight means the numerical average of vehicle curb weight and GVWR. Bi-directional control...

The Atmospheres of Directly Imaged Planets: Where Has All the Methane Gone?

NASA Technical Reports Server (NTRS)

Marley, Mark S.; Zahnle, Kevin

2014-01-01

Methane and ammonia both first appear at lower effective temperatures in brown dwarf atmospheres than equilibrium chemistry models would suggest. This has traditionally been understood as a consequence of vertical mixing timescales being shorter than chemical equilibration timescales in brown dwarf photospheres. Indeed the eddy diffusivity, a variable accounting for the vigor of vertical mixing, has become a standard part of the description of brown dwarf atmosphere models, along with Teff and log g. While some models have suggested that methane is less favored at lower gravity, the almost complete absence of methane in the atmospheres of directly imaged planets, such as those orbiting HR 8799, even at effective temperatures where methane is readily apparent in brown dwarf spectra, has been puzzling. To better understand the paucity of methane in low gravity atmospheres we have revisited the problem of methane chemistry and mixing. We employed a 1-D atmospheric chemistry code augmented with an updated and complete network of the chemical reactions that link CO to CH4. We find the methane abundance at altitudes at or above the effective photosphere is a strong function of surface gravity because higher g shifts the p-T structure to higher pressures (i.e., a given optical depth is proportional to p/g, a relation mitigated somewhat by pressure broadening). Thus quenching in more massive brown dwarfs occurs at a lower temperature and higher pressure, both favoring CH4. We predict that in the lowest mass young giant planets, methane will appear very late, at effective temperatures as low as 600 K rather than the 1200 K seen among field brown dwarfs. This methane deficiency has important implications for the interpretation of spectra as well as methane-based planetary companion searches, such as the NICI survey. The GPI and SPHERE surveys will test these ideas and probe atmospheric chemistry and composition in an entire new range of parameter space. A caveat is that these calculations presume that the C to O ratio is comfortably less than one; the behavior is quite different if C and O are equally abundant, and of course CH4 is always present if C exceeds O.

α-Fluoro-α-nitro(phenylsulfonyl)methane as a fluoromethyl pronucleophile: Efficient stereoselective Michael addition to chalcones

PubMed Central

Prakash, G. K. Surya; Wang, Fang; Stewart, Timothy; Mathew, Thomas; Olah, George A.

2009-01-01

Highly efficient stereoselective 1,4-addition of racemic α-fluoro-α-nitro(phenylsulfonyl)methane (FNSM) as a fluoromethyl pronucleophile to α,β-unsaturated ketones using a wide range of chiral organobifunctional catalysts under moderate conditions in the absence of an additional base has been achieved. A series of catalysts was screened for the enantioselective addition of FNSM to chalcones and the catalysts CN I, CD I, QN I-IV, and QD I were found to enable this reaction, successfully providing exclusive 1,4-addition products stereoselectively in high yields (conversion, diastereomeric ratio, and enantiomeric excess). Studies involving a model reaction and systematic analysis of the absolute configuration support the suggested mechanism. PMID:19237559

Catalysis by Dust Grains in the Solar Nebula

NASA Technical Reports Server (NTRS)

Kress, Monika E.; Tielens, Alexander G. G. M.

1996-01-01

In order to determine whether grain-catalyzed reactions played an important role in the chemistry of the solar nebula, we have applied our time-dependent model of methane formation via Fischer-Tropsch catalysis to pressures from 10(exp -5) to 1 bar and temperatures from 450 to 650 K. Under these physical conditions, the reaction 3H2 + CO yields CH4 + H2O is readily catalyzed by an iron or nickel surface, whereas the same reaction is kinetically inhibited in the gas phase. Our model results indicate that under certain nebular conditions, conversion of CO to methane could be extremely efficient in the presence of iron-nickel dust grains over timescales very short compared to the lifetime of the solar nebula.

Ferrimagnetic Iron Sulfide Formation and Methane Venting Across the Paleocene-Eocene Thermal Maximum in Shallow Marine Sediments, Ancient West Siberian Sea

NASA Astrophysics Data System (ADS)

Rudmin, Maxim; Roberts, Andrew P.; Horng, Chorng-Shern; Mazurov, Aleksey; Savinova, Olesya; Ruban, Aleksey; Kashapov, Roman; Veklich, Maxim

2018-01-01

Authigenesis of ferrimagnetic iron sulfide minerals (greigite and monoclinic pyrrhotite) occurred across the Paleocene-Eocene Thermal Maximum (PETM) within the Bakchar oolitic ironstone in southeastern Western Siberia. Co-occurrence of these minerals is associated with diagenetic environments that support anaerobic oxidation of methane, which has been validated by methane fluid inclusion analysis in the studied sediments. In modern settings, such ferrimagnetic iron sulfide formation is linked to upward methane diffusion in the presence of minor dissolved sulfide ions. The PETM was the most extreme Cenozoic global warming event and massive methane mobilization has been proposed as a major contributor to the globally observed warming and carbon isotope excursion associated with the PETM. The studied sediments provide rare direct evidence for methane mobilization during the PETM. Magnetic iron sulfide formation associated with methanogenesis in the studied sediments can be explained by enhanced local carbon burial across the PETM. While there is no strong evidence to link local methane venting with more widespread methane mobilization and global warming, the magnetic, petrographic, and geochemical approach used here is applicable to identifying authigenic minerals that provide telltale signatures of methane mobility that can be used to assess methane formation and mobilization through the PETM and other hyperthermal climatic events.

Effective conversion of biomass tar into fuel gases in a microwave reactor

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

Anis, Samsudin, E-mail: samsudin-anis@yahoo.com; Zainal, Z. A., E-mail: mezainal@usm.my

2016-06-03

This work deals with conversion of naphthalene (C{sub 10}H{sub 8}) as a biomass tar model compound by means of thermal and catalytic treatments. A modified microwave oven with a maximum output power of 700 W was used as the experimental reactor. Experiments were performed in a wide temperature range of 450-1200°C at a predetermined residence time of 0.24-0.5 s. Dolomite and Y-zeolite were applied to convert naphthalene catalytically into useful gases. Experimental results on naphthalene conversion showed that conversion efficiency and yield of gases increased significantly with the increase of temperature. More than 90% naphthalene conversion efficiency was achieved bymore » thermal treatment at 1200°C and 0.5 s. Nevertheless, this treatment was unfavorable for fuel gases production. The main product of this treatment was soot. Catalytic treatment provided different results with that of thermal treatment in which fuel gases formation was found to be the important product of naphthalene conversion. At a high temperature of 900°C, dolomite had better conversion activity where almost 40 wt.% of naphthalene could be converted into hydrogen, methane and other hydrocarbon gases.« less

Effects of an applied voltage on direct interspecies electron transfer via conductive materials for methane production.

PubMed

Lee, Jung-Yeol; Park, Jeong-Hoon; Park, Hee-Deung

2017-10-01

Direct interspecies electron transfer (DIET) between exoelectrogenic bacteria and methanogenic archaea via conductive materials is reported as an efficient method to produce methane in anaerobic organic waste digestion. A voltage can be applied to the conductive materials to accelerate the DIET between two groups of microorganisms to produce methane. To evaluate this hypothesis, two sets of anaerobic serum bottles with and without applied voltage were used with a pair of graphite rods as conductive materials to facilitate DIET. Initially, the methane production rate was similar between the two sets of serum bottles, and later the serum bottles with an applied voltage of 0.39V showed a 168% higher methane production rate than serum bottles without an applied voltage. In cyclic voltammograms, the characteristic redox peaks for hydrogen and acetate oxidation were identified in the serum bottles with an applied voltage. In the microbial community analyses, hydrogenotrophic methanogens (e.g. Methanobacterium) were observed to be abundant in serum bottles with an applied voltage, while methanogens utilizing carbon dioxide (e.g., Methanosaeta and Methanosarcina) were dominant in serum bottles without an applied voltage. Taken together, the applied voltage on conductive materials might not be effective to promote DIET in methane production. Instead, it appeared to generate a condition for hydrogenotrophic methanogenesis. Copyright © 2017 Elsevier Ltd. All rights reserved.

Sediment characteristics and microbial communities associated with methane production in a eutrophic reservoir

EPA Science Inventory

Methane (CH4), a potent greenhouse gas, is known to be produced and emitted from freshwater systems. Recently, extensive efforts have been directed toward quantifyingmethane emissions fromthese ecosystems, while additional research has focused on factors that may influence emissi...

The effects of the forage-to-concentrate ratio on the conversion of digestible energy to metabolizable energy in growing beef steers

USDA-ARS?s Scientific Manuscript database

The net energy of a feed, required for beef cattle growth models, is often determined from metabolizable energy using cubic equations established by Garrett (1980). For the determination of these equations, ME was estimated using a fixed efficiency of 82% of the digestible energy. However, methane e...

Methane to methanol conversion induced by thorium oxide through the CH3Th(O)H intermediate in solid argon.

PubMed

Gong, Yu; Andrews, Lester; Jackson, Virgil E; Dixon, David A

2012-10-15

Reactions of ThO molecules and CH(4) have been investigated in solid argon near 4 K. The CH(3)Th(O)H molecule is produced when the sample is exposed to UV irradiation. Identification of this new intermediate is substantiated by observation of the Th═O and Th-H stretching vibrational modes with isotopic substitution via matrix infrared spectroscopy, and the assignments are supported by electronic structure frequency calculations. Methanol absorptions increase together with formation of the CH(3)Th(O)H molecule, suggesting a methane to methanol conversion induced by thorium oxide proceeding through the CH(3)Th(O)H intermediate. The formation of CH(3)Th(O)H from ThO + CH(4) is exothermic (ΔH(rxn) = -11 kcal/mol) with an energy barrier of 30 kcal/mol at the CCSD(T)//B3LYP level. Decomposition of this intermediate to form methanol involves spin crossing, and the overall reaction from the intermediate is endothermic by 127 kcal/mol. There is no activation energy for the reaction of thorium atoms with methanol to give CH(3)Th(O)H, as observed in separate experiments with Th and CH(3)OH.

Environmental change and the conversion of permanently frozen ground to wetlands

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

Much of the land around the arctic is permanently frozen, even in the summer. However, because the world is getting warmer, this frozen ground, known as permafrost, is thawing. When permafrost thaws, the ground collapses and sinks, and often a wetland forms within the collapsed area. This conversion of a permanently frozen landscape to a wetland changes the exchange of greenhouse gases between the land and atmosphere, which can, in turn, impact global temperatures and environmental conditions. Wetlands pull carbon dioxide out of the atmosphere because they support the growth of many plants. This uptake of atmospheric carbon dioxide by wetlands helps reduce global warming. However, wetlands also release methane into the atmosphere, which is a potent greenhouse gas — more potent than carbon dioxide. The net effect on global temperatures and environmental conditions depends on the balance between wetland uptake of atmospheric carbon dioxide and release of methane. We are measuring the exchange of these two greenhouse gases between the land and atmosphere in a wetland that formed after permafrost thawed so we can know how global temperatures and environmental conditions will change as northern landscapes continue to thaw.

Development of compact fuel processor for 2 kW class residential PEMFCs

NASA Astrophysics Data System (ADS)

Seo, Yu Taek; Seo, Dong Joo; Jeong, Jin Hyeok; Yoon, Wang Lai

Korea Institute of Energy Research (KIER) has been developing a novel fuel processing system to provide hydrogen rich gas to residential polymer electrolyte membrane fuel cells (PEMFCs) cogeneration system. For the effective design of a compact hydrogen production system, the unit processes of steam reforming, high and low temperature water gas shift, steam generator and internal heat exchangers are thermally and physically integrated into a packaged hardware system. Several prototypes are under development and the prototype I fuel processor showed thermal efficiency of 73% as a HHV basis with methane conversion of 81%. Recently tested prototype II has been shown the improved performance of thermal efficiency of 76% with methane conversion of 83%. In both prototypes, two-stage PrOx reactors reduce CO concentration less than 10 ppm, which is the prerequisite CO limit condition of product gas for the PEMFCs stack. After confirming the initial performance of prototype I fuel processor, it is coupled with PEMFC single cell to test the durability and demonstrated that the fuel processor is operated for 3 days successfully without any failure of fuel cell voltage. Prototype II fuel processor also showed stable performance during the durability test.

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

NASA Astrophysics Data System (ADS)

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

2015-12-01

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

Flux balance analysis indicates that methane is the lowest cost feedstock for microbial cell factories

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

Comer, Austin D.; Long, Matthew R.; Reed, Jennifer L.

The low cost of natural gas has driven significant interest in using C 1 carbon sources (e.g. methane, methanol, CO, syngas) as feedstocks for producing liquid transportation fuels and commodity chemicals. Given the large contribution of sugar and lignocellulosic feedstocks to biorefinery operating costs, natural gas and other C 1 sources may provide an economic advantage. To assess the relative costs of these feedstocks, we performed flux balance analysis on genome-scale metabolic models to calculate the maximum theoretical yields of chemical products from methane, methanol, acetate, and glucose. Yield calculations were performed for every metabolite (as a proxy for desiredmore » products) in the genome-scale metabolic models of three organisms: Escherichia coli (bacterium), Saccharomyces cerevisiae (yeast), and Synechococcus sp. PCC 7002 (cyanobacterium). The calculated theoretical yields and current feedstock prices provided inputs to create comparative feedstock cost surfaces. Our analysis shows that, at current market prices, methane feedstock costs are consistently lower than glucose when used as a carbon and energy source for microbial chemical production. Conversely, methanol is costlier than glucose under almost all price scenarios. Acetate feedstock costs could be less than glucose given efficient acetate production from low-cost syngas using nascent biological gas to liquids (BIO-GTL) technologies. Furthermore, our analysis suggests that research should focus on overcoming the technical challenges of methane assimilation and/or yield of acetate via BIO-GTL to take advantage of low-cost natural gas rather than using methanol as a feedstock.« less

Effect of influent COD/SO4(2-) ratios on UASB treatment of a synthetic sulfate-containing wastewater.

PubMed

Hu, Yong; Jing, Zhaoqian; Sudo, Yuta; Niu, Qigui; Du, Jingru; Wu, Jiang; Li, Yu-You

2015-07-01

The effect of the chemical oxygen demand/sulfate (COD/SO4(2-)) ratio on the anaerobic treatment of synthetic chemical wastewater containing acetate, ethanol, and sulfate, was investigated using a UASB reactor. The experimental results show that at a COD/SO4(2-) ratio of 20 and a COD loading rate of 25.2gCODL(-1)d(-1), a COD removal of as high as 87.8% was maintained. At a COD/SO4(2-) ratio of 0.5 (sulfate concentration 6000mgL(-1)), however, the COD removal was 79.2% and the methane yield was 0.20LCH4gCOD(-1). The conversion of influent COD to methane dropped from 80.5% to 54.4% as the COD/SO4(2-) ratio decreased from 20 to 0.5. At all the COD/SO4(2-) ratios applied, over 79.4% of the total electron flow was utilized by methane-producing archaea (MPA), indicating that methane fermentation was the predominant reaction. The majority of the methane was produced by acetoclastic MPA at high COD/SO4(2-) ratios and both acetoclastic and hydrogenthrophic MPA at low COD/SO4(2-) ratios. Only at low COD/SO4(2-) ratios were SRB species such as Desulfovibrio found to play a key role in ethanol degradation, whereas all the SRB species were found to be incomplete oxidizers at both high and low COD/SO4(2-) ratios. Copyright © 2015 Elsevier Ltd. All rights reserved.

Flux balance analysis indicates that methane is the lowest cost feedstock for microbial cell factories

DOE PAGES

Comer, Austin D.; Long, Matthew R.; Reed, Jennifer L.; ...

2017-07-10

The low cost of natural gas has driven significant interest in using C 1 carbon sources (e.g. methane, methanol, CO, syngas) as feedstocks for producing liquid transportation fuels and commodity chemicals. Given the large contribution of sugar and lignocellulosic feedstocks to biorefinery operating costs, natural gas and other C 1 sources may provide an economic advantage. To assess the relative costs of these feedstocks, we performed flux balance analysis on genome-scale metabolic models to calculate the maximum theoretical yields of chemical products from methane, methanol, acetate, and glucose. Yield calculations were performed for every metabolite (as a proxy for desiredmore » products) in the genome-scale metabolic models of three organisms: Escherichia coli (bacterium), Saccharomyces cerevisiae (yeast), and Synechococcus sp. PCC 7002 (cyanobacterium). The calculated theoretical yields and current feedstock prices provided inputs to create comparative feedstock cost surfaces. Our analysis shows that, at current market prices, methane feedstock costs are consistently lower than glucose when used as a carbon and energy source for microbial chemical production. Conversely, methanol is costlier than glucose under almost all price scenarios. Acetate feedstock costs could be less than glucose given efficient acetate production from low-cost syngas using nascent biological gas to liquids (BIO-GTL) technologies. Furthermore, our analysis suggests that research should focus on overcoming the technical challenges of methane assimilation and/or yield of acetate via BIO-GTL to take advantage of low-cost natural gas rather than using methanol as a feedstock.« less

Performance of a passively vented field-scale biofilter for the microbial oxidation of landfill methane.

PubMed

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.

Rain, winds and haze during the Huygens probe's descent to Titan's surface

USGS Publications Warehouse

Tomasko, M.G.; Archinal, B.; Becker, T.; Bezard, B.; Bushroe, M.; Combes, M.; Cook, D.; Coustenis, A.; De Bergh, C.; Dafoe, L.E.; Doose, L.; Doute, S.; Eibl, A.; Engel, S.; Gliem, F.; Grieger, B.; Holso, K.; Howington-Kraus, E.; Karkoschka, E.; Keller, H.U.; Kirk, R.; Kramm, R.; Kuppers, M.; Lanagan, P.; Lellouch, E.; Lemmon, M.; Lunine, J.; McFarlane, E.; Moores, J.; Prout, G.M.; Rizk, B.; Rosiek, M.; Rueffer, P.; Schroder, S.E.; Schmitt, B.; See, C.; Smith, P.; Soderblom, L.; Thomas, N.; West, R.

2005-01-01

The irreversible conversion of methane into higher hydrocarbons in Titan's stratosphere implies a surface or subsurface methane reservoir. Recent measurements from the cameras aboard the Cassini orbiter fail to see a global reservoir, but the methane and smog in Titan's atmosphere impedes the search for hydrocarbons on the surface. Here we report spectra and high-resolution images obtained by the Huygens Probe Descent Imager/Spectral Radiometer instrument in Titan's atmosphere. Although these images do not show liquid hydrocarbon pools on the surface, they do reveal the traces of once flowing liquid. Surprisingly like Earth, the brighter highland regions show complex systems draining into flat, dark lowlands. Images taken after landing are of a dry riverbed. The infrared reflectance spectrum measured for the surface is unlike any other in the Solar System; there is a red slope in the optical range that is consistent with an organic material such as tholins, and absorption from water ice is seen. However, a blue slope in the near-infrared suggests another, unknown constituent. The number density of haze particles increases by a factor of just a few from an altitude of 150 km to the surface, with no clear space below the tropopause. The methane relative humidity near the surface is 50 per cent. ?? 2005 Nature Publishing Group.

Creating Methane from Plastics: Recycling at a Lunar Outpost

NASA Technical Reports Server (NTRS)

Captain, Janine; Santiago, Eddie; Wheeler, Ray; Strayer, RIchard; Garland, Jay; Parrish, Clyde

2010-01-01

The high cost of re-supply from Earth demands resources to be utilized to the fullest extent for exploration missions. Recycling is a key technology that maximizes the available resources by converting waste products into useful commodities. One example of this is to convert crew member waste such as plastic packaging, food scraps, and human waste, into fuel. The ability to refuel on the lunar surface would reduce the vehicle mass during launch and provide excess payload capability. The goal of this project is to determine the feasibility of recycling waste into methane on the lunar outpost by performing engineering assessments and lab demonstrations of the technology. The first goal of the project was to determine how recycling could influence lunar exploration. Table I shows an estimation of the typical dried waste stream generated each day for a crew of four. Packaging waste accounts for nearly 86% of the dry waste stream and is a significant source of carbon on the lunar surface. This is important because methane (CH4) can be used as fuel and no other source of carbon is available on the lunar surface. With the initial assessment indicating there is sufficient resources in the waste stream to provide refueling capabilities, the project was designed to examine the conversion of plastics into methane.

Simultaneous hydrogen utilization and in situ biogas upgrading in an anaerobic reactor.

PubMed

Luo, Gang; Johansson, Sara; Boe, Kanokwan; Xie, Li; Zhou, Qi; Angelidaki, Irini

2012-04-01

The possibility of converting hydrogen to methane and simultaneous upgrading of biogas was investigated in both batch tests and fully mixed biogas reactor, simultaneously fed with manure and hydrogen. Batch experiments showed that hydrogen could be converted to methane by hydrogenotrophic methanogenesis with conversion of more than 90% of the consumed hydrogen to methane. The hydrogen consumption rates were affected by both P(H₂) (hydrogen partial pressure) and mixing intensity. Inhibition of propionate and butyrate degradation by hydrogen (1 atm) was only observed under high mixing intensity (shaking speed 300 rpm). Continuous addition of hydrogen (flow rate of 28.6 mL/(L/h)) to an anaerobic reactor fed with manure, showed that more than 80% of the hydrogen was utilized. The propionate and butyrate level in the reactor was not significantly affected by the hydrogen addition. The methane production rate of the reactor with H₂ addition was 22% higher, compared to the control reactor only fed with manure. The CO₂ content in the produced biogas was only 15%, while it was 38% in the control reactor. However, the addition of hydrogen resulted in increase of pH (from 8.0 to 8.3) due to the consumption of bicarbonate, which subsequently caused slight inhibition of methanogenesis. Copyright © 2011 Wiley Periodicals, Inc.

Structured catalyst bed and method for conversion of feed materials to chemical products and liquid fuels

DOEpatents

Wang, Yong , Liu; Wei, [Richland, WA

2012-01-24

The present invention is a structured monolith reactor and method that provides for controlled Fischer-Tropsch (FT) synthesis. The invention controls mass transport limitations leading to higher CO conversion and lower methane selectivity. Over 95 wt % of the total product liquid hydrocarbons obtained from the monolithic catalyst are in the carbon range of C.sub.5-C.sub.18. The reactor controls readsorption of olefins leading to desired products with a preselected chain length distribution and enhanced overall reaction rate. And, liquid product analysis shows readsorption of olefins is reduced, achieving a narrower FT product distribution.

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...

Abundant carbon substrates drive extremely high sulfate reduction rates and methane fluxes in Prairie Pothole Wetlands.

PubMed

Dalcin Martins, Paula; Hoyt, David W; Bansal, Sheel; Mills, Christopher T; Tfaily, Malak; Tangen, Brian A; Finocchiaro, Raymond G; Johnston, Michael D; McAdams, Brandon C; Solensky, Matthew J; Smith, Garrett J; Chin, Yu-Ping; Wilkins, Michael J

2017-08-01

Inland waters are increasingly recognized as critical sites of methane emissions to the atmosphere, but the biogeochemical reactions driving such fluxes are less well understood. The Prairie Pothole Region (PPR) of North America is one of the largest wetland complexes in the world, containing millions of small, shallow wetlands. The sediment pore waters of PPR wetlands contain some of the highest concentrations of dissolved organic carbon (DOC) and sulfur species ever recorded in terrestrial aquatic environments. Using a suite of geochemical and microbiological analyses, we measured the impact of sedimentary carbon and sulfur transformations in these wetlands on methane fluxes to the atmosphere. This research represents the first study of coupled geochemistry and microbiology within the PPR and demonstrates how the conversion of abundant labile DOC pools into methane results in some of the highest fluxes of this greenhouse gas to the atmosphere ever reported. Abundant DOC and sulfate additionally supported some of the highest sulfate reduction rates ever measured in terrestrial aquatic environments, which we infer to account for a large fraction of carbon mineralization in this system. Methane accumulations in zones of active sulfate reduction may be due to either the transport of free methane gas from deeper locations or the co-occurrence of methanogenesis and sulfate reduction. If both respiratory processes are concurrent, any competitive inhibition of methanogenesis by sulfate-reducing bacteria may be lessened by the presence of large labile DOC pools that yield noncompetitive substrates such as methanol. Our results reveal some of the underlying mechanisms that make PPR wetlands biogeochemical hotspots, which ultimately leads to their critical, but poorly recognized role in regional greenhouse gas emissions. © 2017 John Wiley & Sons Ltd.

Abundant carbon substrates drive extremely high sulfate reduction rates and methane fluxes in Prairie Pothole Wetlands

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

Dalcin Martins, Paula; Hoyt, David W.; Bansal, Sheel

Inland waters are increasingly recognized as critical sites of methane emissions to the atmosphere, but the biogeochemical reactions driving such fluxes are less well understood. The Prairie Pothole Region (PPR) of North America is one of the largest wetland complexes in the world, containing millions of small, shallow wetlands. The sediment pore waters of PPR wetlands contain some of the highest concentrations of dissolved organic carbon (DOC) and sulfur species ever recorded in terrestrial aquatic environments. Using a suite of geochemical and microbiological analyses we measured the impact of sedimentary carbon and sulfur transformations in these wetlands on methane fluxesmore » to the atmosphere. This research represents the first study of coupled geochemistry and microbiology within the PPR, and demonstrates how the conversion of abundant labile DOC pools into methane results in some of the highest fluxes of this greenhouse gas to the atmosphere ever reported. Abundant DOC and sulfate additionally supported some of the highest sulfate reduction rates ever measured in terrestrial aquatic environments, which we infer to account for a large fraction of carbon mineralization in this system. Methane accumulations in zones of active sulfate reduction may be due to either the transport of free methane gas from deeper locations, or the co-occurrence of methanogenesis and sulfate reduction. If both respiratory processes are concurrent, any competitive inhibition of methanogenesis by sulfate-reducing bacteria may be lessened by the presence of large labile DOC pools that yield non-competitive substrates such as methanol. Our results reveal some of the underlying mechanisms that make PPR wetlands biogeochemical hotspots, which ultimately leads to their critical, but poorly recognized role in regional greenhouse gas emissions.« less

Abundant carbon substrates drive extremely high sulfate reduction rates and methane fluxes in Prairie Pothole Wetlands

USGS Publications Warehouse

Martins, Paula; Hoyt, David W.; Bansal, Sheel; Mills, Christopher T.; Tfaily, Malak; Tangen, Brian; Finocchiaro, Raymond; Johnston, Michael D.; McAdams, Brandon C.; Solensky, Matthew J.; Smith, Garrett J.; Chin, Yu-Ping; Wilkins, Michael J.

2017-01-01

Inland waters are increasingly recognized as critical sites of methane emissions to the atmosphere, but the biogeochemical reactions driving such fluxes are less well understood. The Prairie Pothole Region (PPR) of North America is one of the largest wetland complexes in the world, containing millions of small, shallow wetlands. The sediment pore waters of PPR wetlands contain some of the highest concentrations of dissolved organic carbon (DOC) and sulfur species ever recorded in terrestrial aquatic environments. Using a suite of geochemical and microbiological analyses, we measured the impact of sedimentary carbon and sulfur transformations in these wetlands on methane fluxes to the atmosphere. This research represents the first study of coupled geochemistry and microbiology within the PPR and demonstrates how the conversion of abundant labile DOC pools into methane results in some of the highest fluxes of this greenhouse gas to the atmosphere ever reported. Abundant DOC and sulfate additionally supported some of the highest sulfate reduction rates ever measured in terrestrial aquatic environments, which we infer to account for a large fraction of carbon mineralization in this system. Methane accumulations in zones of active sulfate reduction may be due to either the transport of free methane gas from deeper locations or the co-occurrence of methanogenesis and sulfate reduction. If both respiratory processes are concurrent, any competitive inhibition of methanogenesis by sulfate-reducing bacteria may be lessened by the presence of large labile DOC pools that yield noncompetitive substrates such as methanol. Our results reveal some of the underlying mechanisms that make PPR wetlands biogeochemical hotspots, which ultimately leads to their critical, but poorly recognized role in regional greenhouse gas emissions.

Catalytic co-aromatization of ethanol and methane

DOE PAGES

Wang, Aiguo; He, Peng; Yung, Matthew; ...

2016-06-06

This study demonstrates the technical feasibility of simultaneously converting ethanol and methane into liquid hydrocarbons at mild reaction conditions (400 °C and 1 atm) over silver and/or zinc modified zeolite catalysts. After GC-MS analysis, it is worth noting that aromatics are the major compounds contained in the liquid product collected from the run when 1%Ag/ZSM-5, particularly after H 2 pretreatment, is charged. Compared to the performance exhibited from the run with pure HZSM-5 support engaged, Ag addition into the HZSM-5 framework favors aromatics formation, which might be closely associated with better Ag dispersion and more abundance of strong surface acidicmore » sites where aromatization might take place while Zn loading exerts a detrimental effect on the production of aromatics but promotes the ether generation possibly through dehydration reaction. Referred to that from its N 2 counterpart, the increased aromatics formation of the collected liquid product when methane is present indicates that methane existence might facilitate ethanol aromatization. Moreover, combined with the increased carbon number in the formed aromatics from CH 4 run when H 2 run is referred and zero liquid formation from CH 4-alone test as well as more prominent endothermic feature of methane run and more importantly the notably increased 13C signals in 13C NMR spectra of the liquid product collected during ethanol conversion under 13CH 4 environment, all the observations suggest that methane might be activated nonoxidatively and converted into higher hydrocarbons, preferentially into aromatics if suitable catalyst is charged under the assistance of co-existing oxygenated hydrocarbon. Lastly, the reported synergetic effect could potentially lead to the more economic utilization of abundant natural gas and cellulosic ethanol.« less

Potential for cometabolic biodegradation of 1,4-dioxane in aquifers with methane or ethane as primary substrates.

PubMed

Hatzinger, Paul B; Banerjee, Rahul; Rezes, Rachael; Streger, Sheryl H; McClay, Kevin; Schaefer, Charles E

2017-12-01

The objective of this research was to evaluate the potential for two gases, methane and ethane, to stimulate the biological degradation of 1,4-dioxane (1,4-D) in groundwater aquifers via aerobic cometabolism. Experiments with aquifer microcosms, enrichment cultures from aquifers, mesophilic pure cultures, and purified enzyme (soluble methane monooxygenase; sMMO) were conducted. During an aquifer microcosm study, ethane was observed to stimulate the aerobic biodegradation of 1,4-D. An ethane-oxidizing enrichment culture from these samples, and a pure culture capable of growing on ethane (Mycobacterium sphagni ENV482) that was isolated from a different aquifer also biodegraded 1,4-D. Unlike ethane, methane was not observed to appreciably stimulate the biodegradation of 1,4-D in aquifer microcosms or in methane-oxidizing mixed cultures enriched from two different aquifers. Three different pure cultures of mesophilic methanotrophs also did not degrade 1,4-D, although each rapidly oxidized 1,1,2-trichloroethene (TCE). Subsequent studies showed that 1,4-D is not a substrate for purified sMMO enzyme from Methylosinus trichosporium OB3b, at least not at the concentrations evaluated, which significantly exceeded those typically observed at contaminated sites. Thus, our data indicate that ethane, which is a common daughter product of the biotic or abiotic reductive dechlorination of chlorinated ethanes and ethenes, may serve as a substrate to enhance 1,4-D degradation in aquifers, particularly in zones where these products mix with aerobic groundwater. It may also be possible to stimulate 1,4-D biodegradation in an aerobic aquifer through addition of ethane gas. Conversely, our results suggest that methane may have limited importance in natural attenuation or for enhancing biodegradation of 1,4-D in groundwater environments.

Methane fluxes from tropical coastal lagoons surrounded bymangroves, Yucatán, Mexico

USGS Publications Warehouse

Chuang, Pei-Chuan; Young, Megan B.; Dale, Andrew W.; Miller, Laurence G.; Herrera-Silveira, Jorge A; Paytan, Adina

2017-01-01

Methane concentrations in the water column and emissions to the atmosphere were determined for three tropical coastal lagoons surrounded by mangrove forests on the Yucatán Peninsula, Mexico. Surface water dissolved methane was sampled at different seasons over a period of 2 years in areas representing a wide range of salinities and anthropogenic impacts. The highest surface water methane concentrations (up to 8378 nM) were measured in a polluted canal associated with Terminos Lagoon. In Chelem Lagoon, methane concentrations were typically lower, except in the polluted harbor area (1796 nM). In the relatively pristine Celestún Lagoon, surface water methane concentrations ranged from 41 to 2551 nM. Methane concentrations were negatively correlated with salinity in Celestún, while in Chelem and Terminos high methane concentrations were associated with areas of known pollution inputs, irrespective of salinity. The diffusive methane flux from surface lagoon water to the atmosphere ranged from 0.0023 to 15 mmol CH4 m−2 d−1. Flux chamber measurements revealed that direct methane release as ebullition was up to 3 orders of magnitude greater than measured diffusive flux. Coastal mangrove lagoons may therefore be an important natural source of methane to the atmosphere despite their relatively high salinity. Pollution inputs are likely to substantially enhance this flux. Additional statistically rigorous data collected globally are needed to better consider methane fluxes from mangrove-surrounded coastal areas in response to sea level changes and anthropogenic pollution in order to refine projections of future atmospheric methane budgets.

Microbial methane production in oxygenated water column of an oligotrophic lake

PubMed Central

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

Methane fluxes from tropical coastal lagoons surrounded by mangroves, Yucatán, Mexico

NASA Astrophysics Data System (ADS)

Chuang, P.-C.; Young, M. B.; Dale, A. W.; Miller, L. G.; Herrera-Silveira, J. A.; Paytan, A.

2017-05-01

Methane concentrations in the water column and emissions to the atmosphere were determined for three tropical coastal lagoons surrounded by mangrove forests on the Yucatán Peninsula, Mexico. Surface water dissolved methane was sampled at different seasons over a period of 2 years in areas representing a wide range of salinities and anthropogenic impacts. The highest surface water methane concentrations (up to 8378 nM) were measured in a polluted canal associated with Terminos Lagoon. In Chelem Lagoon, methane concentrations were typically lower, except in the polluted harbor area (1796 nM). In the relatively pristine Celestún Lagoon, surface water methane concentrations ranged from 41 to 2551 nM. Methane concentrations were negatively correlated with salinity in Celestún, while in Chelem and Terminos high methane concentrations were associated with areas of known pollution inputs, irrespective of salinity. The diffusive methane flux from surface lagoon water to the atmosphere ranged from 0.0023 to 15 mmol CH4 m-2 d-1. Flux chamber measurements revealed that direct methane release as ebullition was up to 3 orders of magnitude greater than measured diffusive flux. Coastal mangrove lagoons may therefore be an important natural source of methane to the atmosphere despite their relatively high salinity. Pollution inputs are likely to substantially enhance this flux. Additional statistically rigorous data collected globally are needed to better consider methane fluxes from mangrove-surrounded coastal areas in response to sea level changes and anthropogenic pollution in order to refine projections of future atmospheric methane budgets.

40 CFR 86.004-2 - Definitions.

Code of Federal Regulations, 2013 CFR

2013-07-01

... or a fire truck. Fire truck has the meaning given in § 86.1803. U.S.-directed production means the...-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...

40 CFR 86.004-2 - Definitions.

Code of Federal Regulations, 2014 CFR

2014-07-01

... or a fire truck. Fire truck has the meaning given in § 86.1803. U.S.-directed production means the...-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...

30 CFR 75.351 - Atmospheric monitoring systems.

Code of Federal Regulations, 2010 CFR

2010-07-01

... and type of AMS sensor at each location, and the intended air flow direction at these locations. This... methane concentration at any sensor reaches the alert level as specified in § 75.351(i). These signals... carbon monoxide, smoke, or methane concentration at any sensor reaches the alarm level as specified in...

30 CFR 75.351 - Atmospheric monitoring systems.

Code of Federal Regulations, 2011 CFR

2011-07-01

... and type of AMS sensor at each location, and the intended air flow direction at these locations. This... methane concentration at any sensor reaches the alert level as specified in § 75.351(i). These signals... carbon monoxide, smoke, or methane concentration at any sensor reaches the alarm level as specified in...

Liquid methane gelled with methanol and water reduces rate of nitrogen absorption

NASA Technical Reports Server (NTRS)

Vanderwall, E. M.

1972-01-01

Dilution of gelant vapor with inert carrier gas accomplishes gelation. Mixture is injected through heated tube and orifice into liquid methane for immediate condensation within bulk of liquid. Direct dispersion of particles in liquid avoids condensation on walls of vessel and eliminates additional mixing.

Quantifying the loss of methane through secondary gas mass transport (or 'slip') from a micro-porous membrane contactor applied to biogas upgrading.

PubMed

McLeod, Andrew; Jefferson, Bruce; McAdam, Ewan J

2013-07-01

Secondary gas transport during the separation of a binary gas with a micro-porous hollow fibre membrane contactor (HMFC) has been studied for biogas upgrading. In this application, the loss or 'slip' of the secondary gas (methane) during separation is a known concern, specifically since methane possesses the intrinsic calorific value. Deionised (DI) water was initially used as the physical solvent. Under these conditions, carbon dioxide (CO2) and methane (CH4) absorption were dependent upon liquid velocity (V(L)). Whilst the highest CO2 flux was recorded at high V(L), selectivity towards CO2 declined due to low residence times and a diminished gas-side partial pressure, and resulted in slip of approximately 5.2% of the inlet methane. Sodium hydroxide was subsequently used as a comparative chemical absorption solvent. Under these conditions, CO2 mass transfer increased by increasing gas velocity (VG) which is attributed to the excess of reactive hydroxide ions present in the solvent, and the fast conversion of dissolved CO2 to carbonate species reinitiating the concentration gradient at the gas-liquid interface. At high gas velocities, CH4 slip was reduced to 0.1% under chemical conditions. Methane slip is therefore dependent upon whether the process is gas phase or liquid phase controlled, since methane mass transport can be adequately described by Henry's law within both physical and chemical solvents. The addition of an electrolyte was found to further retard CH4 absorption via the salting out effect. However, their applicability to physical solvents is limited since electrolytic concentration similarly impinges upon the solvents' capacity for CO2. This study illustrates the significance of secondary gas mass transport, and furthermore demonstrates that gas-phase controlled systems are recommended where greater selectivity is required. Copyright © 2013 Elsevier Ltd. All rights reserved.

Source Attribution of Methane Emissions in Northeastern Colorado Using Ammonia to Methane Emission Ratios

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.

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.

Mission analysis for the federal fuels from biomass program. Volume IV. Termochemical conversion of biomass to fuels and chemicals

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

Kohan, S.M.; Barkhordar, P.M.

1979-01-01

The thermochemical conversion of biomass feedstocks generally denotes technologies that use elevated temperatures to convert the fixed carbon content of biomass materials to produce other, more useful energy forms. Examples are combustion to produce heat, steam, electricity, or combinations of these; pyrolysis to produce gas (low- or intermediate-Btu), pyrolytic liquids and chemicals, and char; gasification to produce low or intermediate Btu gas (and, from IBG, additional products such as SNG, ammonia, methanol, or Fischer-Tropsch liquids); and liquefaction to produce heavy fuel oil or, with upgrading, lighter-boiling liquid products such as distillates, light fuel oils, or gasoline. This section discusses themore » selection of the feedstock used in the analysis of thermochemical conversion technologies. The following sections present detailed technical and economic evaluations of biomass conversion to electricity and steam by combustion, SNG by gasification and methanation, methanol by gasification and synthesis, oil by catalytic liquefaction, oil and char by pyrolysis, and ammonia by gasification and synthesis. The conversion options were reviewed with DOE for approval at the start of the project.« less

Electrohydrolysis pretreatment for enhanced methane production from lignocellulose waste pulp and paper mill sludge and its kinetics.

PubMed

Veluchamy, C; Raju, V Wilson; Kalamdhad, Ajay S

2018-03-01

A novel electrohydrolysis pretreatment enhances methane production from lignocellulose material during anaerobic digestion. A biochemical methane potential assay was carried out to determine the effect of direct current and the efficacy of electrohydrolysis pretreatment on biogas production. Methane yield was increased by 13.8%, to 301 ± 3 mL CH 4 /g VS, when lignocellulosic waste was pretreated with electrohydrolysis. A net energy gain of 13,224 kJ was realized after electrohydrolysis pretreatment, which was 1.51 times higher than reported for thermal pretreatment. In addition, two kinetic models were used, including the modified Gompertz model to reproduce the experimental data. These finding support the potential for increased methane recovery from lignocellulosic waste using electrohydrolysis as a pretreatment. Copyright © 2017 Elsevier Ltd. All rights reserved.

Microscopic Origin of Strain Hardening in Methane Hydrate

PubMed Central

Jia, Jihui; Liang, Yunfeng; Tsuji, Takeshi; Murata, Sumihiko; Matsuoka, Toshifumi

2016-01-01

It has been reported for a long time that methane hydrate presents strain hardening, whereas the strength of normal ice weakens with increasing strain after an ultimate strength. However, the microscopic origin of these differences is not known. Here, we investigated the mechanical characteristics of methane hydrate and normal ice by compressive deformation test using molecular dynamics simulations. It is shown that methane hydrate exhibits strain hardening only if the hydrate is confined to a certain finite cross-sectional area that is normal to the compression direction. For normal ice, it does not present strain hardening under the same conditions. We show that hydrate guest methane molecules exhibit no long-distance diffusion when confined to a finite-size area. They appear to serve as non-deformable units that prevent hydrate structure failure, and thus are responsible for the strain-hardening phenomenon. PMID:27009239

Effect of structural promoters on Fe-based Fischer-Tropsch synthesis of biomass derived syngas

Treesearch

Pratibha Sharma; Thomas Elder; Leslie H. Groom; James J. Spivey

2014-01-01

Biomass gasification and subsequent conversion of this syngas to liquid hydrocarbons using Fischer–Tropsch (F–T) synthesis is a promising source of hydrocarbon fuels. However, biomass-derived syngas is different from syngas obtained from other sources such as steam reforming of methane. Specifically the H2/CO ratio is less than 1/1 and the CO

Shock synthesis of amino acids in simulated primitive environments.

NASA Technical Reports Server (NTRS)

Bar-Nun, A.; Bar-Nun, N.; Bauer, S. H.; Sagan, C.

1971-01-01

A single pulse shock tube of a uniform bore was used in the experiments. The reaction mixture consisted of 3.3 per cent methane, 11 per cent ethane, and 5.6 per cent ammonia, diluted with ultra-pure argon. The formation of glycine, alanine, valine, and leucine under conditions of shock heating was observed. Thermodynamic relations are discussed together with questions of conversion efficiency.

Efficient gas-separation process to upgrade dilute methane stream for use as fuel

DOEpatents

Wijmans, Johannes G [Menlo Park, CA; Merkel, Timothy C [Menlo Park, CA; Lin, Haiqing [Mountain View, CA; Thompson, Scott [Brecksville, OH; Daniels, Ramin [San Jose, CA

2012-03-06

A membrane-based gas separation process for treating gas streams that contain methane in low concentrations. The invention involves flowing the stream to be treated across the feed side of a membrane and flowing a sweep gas stream, usually air, across the permeate side. Carbon dioxide permeates the membrane preferentially and is picked up in the sweep air stream on the permeate side; oxygen permeates in the other direction and is picked up in the methane-containing stream. The resulting residue stream is enriched in methane as well as oxygen and has an EMC value enabling it to be either flared or combusted by mixing with ordinary air.

Carbon kinetic isotope effect in the reaction of CH4 with HO

NASA Technical Reports Server (NTRS)

Davidson, J. A.; Cantrell, C. A.; Tyler, S. C.; Shetter, R. E.; Cicerone, R. J.

1987-01-01

The carbon kinetic isotope effect in the CH4 + HO reaction is measured experimentally and the use of carbon isotope ratios to diagnose atmospheric methane is examined. The chemical, photolysis, and analytical experimental conditions and procedures are described. It is determined that the CH4 + HO reaction has a carbon kinetic isotope effect of 1.010 + or 0.007 for k(12)k(13) (rate constants ratio) at 297 + or - 3 K. This value is compared with the data of Rust and Stevens (1980). Causes for the poor correlation between the data at high methane conversions are discussed. It is supposed that the difference between the k(12) and k(13) values is due to a difference in the activation energy of the two reactions.

Co-generation of biohydrogen and biomethane through two-stage batch co-fermentation of macro- and micro-algal biomass.

PubMed

Ding, Lingkan; Cheng, Jun; Xia, Ao; Jacob, Amita; Voelklein, Markus; Murphy, Jerry D

2016-10-01

Aquatic micro-algae can be used as feedstocks for gaseous biofuel production via biological fermentation. However, micro-algae usually have low C/N ratios, which are not advantageous for fermentation. In this study, carbon-rich macro-algae (Laminaria digitata) mixed with nitrogen-rich micro-algae (Chlorella pyrenoidosa and Nannochloropsis oceanica) were used to maintain a suitable C/N ratio of 20 for a two-stage process combining hydrogen and methane fermentation. Co-fermentation of L. digitata and micro-algae facilitated hydrolysis and acidogenesis, resulting in hydrogen yields of 94.5-97.0mL/gVS; these values were 15.5-18.5% higher than mono-fermentation using L. digitata. Through the second stage of methane co-fermentation, a large portion of energy remaining in the hydrogenogenic effluents was recovered in the form of biomethane. The two-stage batch co-fermentation markedly increased the energy conversion efficiencies (ECEs) from 4.6-6.6% during the hydrogen fermentation to 57.0-70.9% in the combined hydrogen and methane production. Copyright © 2016 Elsevier Ltd. All rights reserved.

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

NASA Technical Reports Server (NTRS)

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

1980-01-01

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

Microbial ecology of anaerobic digesters: the key players of anaerobiosis.

PubMed

Ali Shah, Fayyaz; Mahmood, Qaisar; Maroof Shah, Mohammad; Pervez, Arshid; Ahmad Asad, Saeed

2014-01-01

Anaerobic digestion is the method of wastes treatment aimed at a reduction of their hazardous effects on the biosphere. The mutualistic behavior of various anaerobic microorganisms results in the decomposition of complex organic substances into simple, chemically stabilized compounds, mainly methane and CO2. The conversions of complex organic compounds to CH4 and CO2 are possible due to the cooperation of four different groups of microorganisms, that is, fermentative, syntrophic, acetogenic, and methanogenic bacteria. Microbes adopt various pathways to evade from the unfavorable conditions in the anaerobic digester like competition between sulfate reducing bacteria (SRB) and methane forming bacteria for the same substrate. Methanosarcina are able to use both acetoclastic and hydrogenotrophic pathways for methane production. This review highlights the cellulosic microorganisms, structure of cellulose, inoculum to substrate ratio, and source of inoculum and its effect on methanogenesis. The molecular techniques such as DGGE (denaturing gradient gel electrophoresis) utilized for dynamic changes in microbial communities and FISH (fluorescent in situ hybridization) that deal with taxonomy and interaction and distribution of tropic groups used are also discussed.

Microbial Ecology of Anaerobic Digesters: The Key Players of Anaerobiosis

PubMed Central

Ali Shah, Fayyaz; Mahmood, Qaisar; Maroof Shah, Mohammad; Pervez, Arshid; Ahmad Asad, Saeed

2014-01-01

Anaerobic digestion is the method of wastes treatment aimed at a reduction of their hazardous effects on the biosphere. The mutualistic behavior of various anaerobic microorganisms results in the decomposition of complex organic substances into simple, chemically stabilized compounds, mainly methane and CO2. The conversions of complex organic compounds to CH4 and CO2 are possible due to the cooperation of four different groups of microorganisms, that is, fermentative, syntrophic, acetogenic, and methanogenic bacteria. Microbes adopt various pathways to evade from the unfavorable conditions in the anaerobic digester like competition between sulfate reducing bacteria (SRB) and methane forming bacteria for the same substrate. Methanosarcina are able to use both acetoclastic and hydrogenotrophic pathways for methane production. This review highlights the cellulosic microorganisms, structure of cellulose, inoculum to substrate ratio, and source of inoculum and its effect on methanogenesis. The molecular techniques such as DGGE (denaturing gradient gel electrophoresis) utilized for dynamic changes in microbial communities and FISH (fluorescent in situ hybridization) that deal with taxonomy and interaction and distribution of tropic groups used are also discussed. PMID:24701142

High reactivity of nanosized niobium oxide cluster cations in methane activation: A comparison with vanadium oxides

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

Ding, Xun-Lei, E-mail: dingxl@ncepu.edu.cn, E-mail: chemzyx@iccas.ac.cn; Wang, Dan; Wu, Xiao-Nan

2015-09-28

The reactions between methane and niobium oxide cluster cations were studied and compared to those employing vanadium oxides. Hydrogen atom abstraction (HAA) reactions were identified over stoichiometric (Nb{sub 2}O{sub 5}){sub N}{sup +} clusters for N as large as 14 with a time-of-flight mass spectrometer. The reactivity of (Nb{sub 2}O{sub 5}){sub N}{sup +} clusters decreases as the N increases, and it is higher than that of (V {sub 2}O{sub 5}){sub N}{sup +} for N ≥ 4. Theoretical studies were conducted on (Nb{sub 2}O{sub 5}){sub N}{sup +} (N = 2–6) by density functional calculations. HAA reactions on these clusters are all favorablemore » thermodynamically and kinetically. The difference of the reactivity with respect to the cluster size and metal type (Nb vs V) was attributed to thermodynamics, kinetics, the electron capture ability, and the distribution of the unpaired spin density. Nanosized Nb oxide clusters show higher HAA reactivity than V oxides, indicating that niobia may serve as promising catalysts for practical methane conversion.« less

Green plants as solar energy converters

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

Not Available

1976-06-01

A survey covers the potential of energy production from biomass and solid wastes; various processes for the combustion of wastes, such as the co-combustion of solid waste and sewage sludge at the St. Paul/Seneca Treatment Plant Sludge Incinerator; various biological processes for the conversion of solid wastes to fuel such as the Institute of Gas Technology 400 l. digestor for the biogasification of municipal solid waste and sewage solids to a methane-rich product gas; the use of industrial wastes for fuel, such as slash and mill residues used as fuel in lumber mills; the biogasification of animal wastes by usingmore » small-scale on-site digesters to produce methane gas for cooking and lighting; energy farming methods, such as growing giant California kelp, sargassum, and plankton as suitable feedstock for the production of methane, fertilizers, and food; problems, such as the possible alteration of the reflectivity of large areas of the earth's surface by rapidly growing plants raised for biomass; and benefits such as the reduction in air, water, and land pollution associated with the use of wastes and biomass grown especially for energy.« less

Metagenomic insight into methanogenic reactors promoting direct interspecies electron transfer via granular activated carbon.

PubMed

Park, Jeong-Hoon; Park, Jong-Hun; Je Seong, Hoon; Sul, Woo Jun; Jin, Kang-Hyun; Park, Hee-Deung

2018-07-01

To provide insight into direct interspecies electron transfer via granular activated carbon (GAC), the effect of GAC supplementation on anaerobic digestion was evaluated. Compared to control samples, the GAC supplementation increased the total amount of methane production and its production rate by 31% and 72%, respectively. 16S rDNA sequencing analysis revealed a shift in the archaeal community composition; the Methanosarcina proportion decreased 17%, while the Methanosaeta proportion increased 5.6%. Metagenomic analyses based on shotgun sequencing demonstrated that the abundance of pilA and omcS genes belonging to Geobacter species decreased 69.4% and 29.4%, respectively. Furthermore, the analyses suggested a carbon dioxide reduction pathway rather than an acetate decarboxylation pathway for methane formation. Taken together, these results suggest that GAC improved methane production performance by shifting the microbial community and altering functional genes associated with direct interspecies electron transfer via conductive materials. Copyright © 2018 Elsevier Ltd. All rights reserved.

The phase transformation of methane caused by pressure change during its rising from seepage, revealed by video　observation　and acoustic reflection data

NASA Astrophysics Data System (ADS)

Aoyama, D.; Aoyama, C.

2014-12-01

The plume comes out to the surface of the water, and methane is released for low water temperature and low temperature in the Arctic Ocean by the atmosphere. Methane released by the atmosphere is combined with oxygen and becomes carbon dioxide and the water, and the greenhouse effect is higher in 20 times than carbon dioxide. If quantity of the　methane　plume is quantified, I may estimate the quantity of existing methane underground and can estimate the scale of methane melting into it in seawater. The　methane　plume solved in seawater is one element of the carbon cycle. It is important that I elucidate this element in thinking about the carbon cycle of the wide sense.　However, there is not the report that I showed quantitatively how much methane melts into it in seawater a year from the methane plume. Therefore, in this article, I identified an aspect of gush methane as it by the sound data with the fishfinder and by a gush picture of the methane plume. With that in mind, I quantified the quantity of the methane plume. As a result, the following things became clear. The methane hydrate grain to gush out from a gush mouth is a solid at the bottom of the sea direct top. In this sea area, methane of 7.7*104m3 per unit area gushes out. In addition, the sea area where 6.3*106m3 gushed out existed.

Multi-scale monitoring of a marine geologic methane source in the Santa Barbara Channel using imaging spectrometry, ARCTAS-CARB in situ sampling and coastal hourly total hydrocarbon measurements

NASA Astrophysics Data System (ADS)

Bradley, E. S.; Leifer, I.; Roberts, D.; Dennison, P. E.; Margolis, J.; Moritsch, M.; Diskin, G. S.; Sachse, G. W.

2009-12-01

The Coal Oil Point (COP) hydrocarbon seep field off the coast of Santa Barbara, CA is one of the most active and best-studied marine geologic methane sources in the world and contributes to elevated terrestrial methane concentrations downwind. In this study, we investigate the spatiotemporal variability of this local source and the influence of meteorological conditions on transport and concentration. A methane plume emanating from Trilogy Seep was mapped with the Airborne Visible Infrared Imaging Spectrometer at a 7.5 m resolution with a short-wave infrared band ratio technique. This structure agrees with the local wind speed and direction and is orthogonal to the surface currents. ARCTAS-CARB aircraft in situ sampling of lower-troposphere methane is compared to sub-hour total hydrocarbon concentration (THC) measurements from the Santa Barbara Air Pollution Control District (SBAPCD) station located near COP. Hourly SBAPCD THC values from 1980-2008 demonstrate a decrease in seep source strength until the late 1990s, followed by a consistent increase. The occurrence of elevated SBAPCD THC values for onshore wind conditions as well as numerous positive outliers as high as 17 ppm suggests that seep field emissions are both quasi-steady state and transient, direct (bubble) and diffuse (outgassing). As demonstrated for the COP seeps, the combination of imaging spectrometry, aircraft in situ sampling, and ground-based monitoring provides a powerful approach for understanding local methane sources and transport processes.

Regimes of an atmospheric pressure nanosecond repetitively pulsed discharge for methane partial oxidation

NASA Astrophysics Data System (ADS)

Maqueo, P. D. G.; Maier, M.; Evans, M. D. G.; Coulombe, S.; Bergthorson, J. M.

2018-04-01

The operation of a nanosecond repetitively pulsed discharge for partial oxidation of CH4 is characterized at atmospheric pressure and room temperature. Two regimes are observed: diffuse and filamentary. The first is a low power regime, characterized by low rotational temperatures around 400 K. The second is much more energetic with rotational temperatures close to 600 K. Both have vibrational temperatures of at least 10 times their rotational temperatures. The average electron number density was determined to be 8.9×1015 and 4.0×1017 cm-3, respectively, showing an increase in the ionization fraction in the more powerful filamentary regime. Results of CH4 conversion to H2, CO, CO2 and C2H6 are presented for the filamentary regime, while the diffuse regime shows no measurable conversion ability. As expected, oxidative mixtures show higher conversion ability than pure CH4. A maximum conversion efficiency of 26.3% and a maximum energy efficiency of 19.7% were reached for the oxidative mixtures.

Determination of Chemical Kinetic Rate Constants of a Model for Carbothermal Processing of Lunar Regolith Simulant Using Methane

NASA Technical Reports Server (NTRS)

Balasubramaniam, R; Gokoglu, S.; Hegde, U.

2009-01-01

We have previously developed a chemical conversion model of the carbothermal processing of lunar regolith using methane to predict the rate of production of carbon monoxide. In this carbothermal process, gaseous methane is pyrolyzed as it flows over the hot surface of a molten zone of lunar regolith and is converted to carbon and hydrogen. Hydrogen is carried away by the exiting stream of gases and carbon is deposited on the melt surface. The deposited carbon mixes with the melt and reacts with the metal oxides in it to produce carbon monoxide that bubbles out of the melt. In our model, we assume that the flux of carbon deposited is equal to the product of the surface reaction rate constant gamma and the concentration of methane adjacent to the melt surface. Similarly, the rate of consumption of carbon per unit volume in the melt is equal to the product of the melt reaction rate constant k and the concentrations of carbon and metal oxide in the melt. In this paper, we describe our effort to determine gamma and k by comparison of the predictions from our model with test data obtained by ORBITEC (Orbital Technologies Corporation). The concentration of methane adjacent to the melt surface is a necessary input to the model. It is inferred from the test data by a mass balance of methane, adopting the usual assumptions of the continuously-stirred-tank-reactor model, whereby the average concentration of a given gaseous species equals its exit concentration. The reaction rates gamma and k have been determined by a non-linear least-squares fit to the test data for the production of carbon monoxide and the fraction of the incoming methane that is converted. The comparison of test data with our model predictions using the determined chemical kinetic rate constants provides a consistent interpretation of the process over the full range of temperatures, pressures, and methane flow rates used in the tests, thereby increasing our confidence to use the model for scale-up purposes.

Open-path spectroscopic methane detection using a broadband monolithic distributed feedback-quantum cascade laser array.

PubMed

Michel, Anna P M; Kapit, Jason; Witinski, Mark F; Blanchard, Romain

2017-04-10

Methane is a powerful greenhouse gas that has both natural and anthropogenic sources. The ability to measure methane using an integrated path length approach such as an open/long-path length sensor would be beneficial in several environments for examining anthropogenic and natural sources, including tundra landscapes, rivers, lakes, landfills, estuaries, fracking sites, pipelines, and agricultural sites. Here a broadband monolithic distributed feedback-quantum cascade laser array was utilized as the source for an open-path methane sensor. Two telescopes were utilized for the launch (laser source) and receiver (detector) in a bistatic configuration for methane sensing across a 50 m path length. Direct-absorption spectroscopy was utilized with intrapulse tuning. Ambient methane levels were detectable, and an instrument precision of 70 ppb with 100 s averaging and 90 ppb with 10 s averaging was achieved. The sensor system was designed to work "off the grid" and utilizes batteries that are rechargeable with solar panels and wind turbines.

Indirect chemical effects of methane on climate warming

NASA Astrophysics Data System (ADS)

Lelieveld, Jos; Crutzen, Paul J.

1992-01-01

METHANE concentrations in the atmosphere have increased from about 0.75 to 1.7 p.p.m.v. since pre-industrial times1,2. The current annual rate of increase of about 0.8% yr-1 (ref. 2) is due to increases in industrial and agricultural emissions. This increase in atmospheric methane concentrations not only influences the climate directly, but also indirectly through chemical reactions. Here we show that the climate effects of methane's atmospheric chemistry have previously been overestimated, notably by the Inter-governmental Panel on Climate Change (IPCC)3, largely owing to neglect of the height dependence of certain atmospheric radiative processes. Using available estimates of fossil-fuel-related leaks of methane, our results show that switching from coal and oil to natural gas as an energy source would reduce climate warming. A significant fraction of methane emissions cannot, however, be accounted for by known sources; should leakages from gas production and distribution be underestimated for some countries, then it might be unwise to switch to using natural gas.

Exploring the metabolic potential of microbial communities in ultra-basic, reducing springs at The Cedars, CA, USA: Experimental evidence of microbial methanogenesis and heterotrophic acetogenesis

NASA Astrophysics Data System (ADS)

Kohl, Lukas; Cumming, Emily; Cox, Alison; Rietze, Amanda; Morrissey, Liam; Lang, Susan Q.; Richter, Andreas; Suzuki, Shino; Nealson, Kenneth H.; Morrill, Penny L.

2016-04-01

Present-day serpentinization generates groundwaters with conditions (pH > 11, Eh < -550 mV) favorable for the microbial and abiotic production of organic compounds from inorganic precursors. Elevated concentrations of methane, C2-C6 alkanes, acetate, and formate have been detected at these sites, but the microbial or abiotic origin of these compounds remains unclear. While geochemical data indicate that methane at most sites of present-day serpentinization is abiogenic, the stable carbon, hydrogen, and clumped isotope data as well as the hydrocarbon gas composition from The Cedars, CA, USA, are consistent with a microbial origin for methane. However, there is no direct evidence of methanogenesis at this site of serpentinization. We report on laboratory experiments in which the microbial communities in fluids and sediments from The Cedars were incubated with 13C labeled substrates. Increasing methane concentrations and the incorporation of 13C into methane in live experiments, but not in killed controls, demonstrated that methanogens converted methanol, formate, acetate (methyl group), and bicarbonate to methane. The apparent fractionation between methane and potential substrates (α13CCH4-CO2(g) = 1.059 to 1.105, α13CCH4-acetate = 1.042 to 1.119) indicated that methanogenesis was dominated by the carbonate reduction pathway. Increasing concentrations of volatile organic acid anions indicated microbial acetogenesis. α13CCO2(g)-acetate values (0.999 to 1.000), however, were inconsistent with autotrophic acetogenesis, thus suggesting that acetate was produced through fermentation. This is the first study to show direct evidence of microbial methanogenesis and acetogenesis by the native microbial community at a site of present-day serpentinization.

Trade Study of Five In-Situ Propellant Production System for a Mars Sample Return Mission

NASA Technical Reports Server (NTRS)

Green, S. T.; Deffenbaugh, D. M.; Miller, M. A.

1999-01-01

One of the goals of NASA''s HEDS enterprise is to establish a long-term human presence on Mars at a fraction of the cost of employing today''s technology. The most direct method of reducing mission cost is to reduce the launch mass of the spacecraft. If the propellants for the return phase of the mission are produced on Mars, the total spacecraft mass could be reduced significantly. An interim goal is a Mars Sample Return (MSR) mission, which is proposed to demonstrate the feasibility of in-situ propellant production (ISPP). Five candidate ISPP systems for producing two fuels and oxygen from the Martian atmosphere are considered in this design trade-off study:(1) Zirconia cell with methanol synthesis, (2) Reverse water gas shift (RWGS) with water electrolysis and methanol synthesis, (3) Sabatier process for methane production with water electrolysis, (4) Sabatier process with water electrolysis and partial methane pyrolysis, and (5) Sabatier/RWGS combination with water electrolysis. These systems have been the subject of numerous previous analytical studies and laboratory demonstrations. In this investigation, the systems are objectively compared on the basis of thermochemical performance models using a commonly used chemical plant analysis software package. The realistic effects of incomplete chemical conversion and gas phase separator performance are included in these models. This study focuses on the chemical processing and product separation subsystems. The CO2 compression upstream of the chemical plane and the liquefaction/storage components are not included here.

Structure, microstructure, and size dependent catalytic properties of nanostructured ruthenium dioxide

NASA Astrophysics Data System (ADS)

Nowakowski, Pawel; Dallas, Jean-Pierre; Villain, Sylvie; Kopia, Agnieszka; Gavarri, Jean-Raymond

2008-05-01

Nanostructured powders of ruthenium dioxide RuO 2 were synthesized via a sol gel route involving acidic solutions with pH varying between 0.4 and 4.5. The RuO 2 nanopowders were characterized by X-ray diffraction, scanning and transmission electron microscopy (SEM and TEM). Rietveld refinement of mean crystal structure was performed on RuO 2 nanopowders and crystallized standard RuO 2 sample. Crystallite sizes measured from X-ray diffraction profiles and TEM analysis varied in the range of 4-10 nm, with a minimum of crystallite dimension for pH=1.5. A good agreement between crystallite sizes calculated from Williamson Hall approach of X-ray data and from direct TEM observations was obtained. The tetragonal crystal cell parameter (a) and cell volumes of nanostructured samples were characterized by values greater than the values of standard RuO 2 sample. In addition, the [Ru-O 6] oxygen octahedrons of rutile structure also depended on crystal size. Catalytic conversion of methane by these RuO 2 nanostructured catalysts was studied as a function of pH, catalytic interaction time, air methane composition, and catalysis temperature, by the way of Fourier transform infrared (FTIR) spectroscopy coupled to homemade catalytic cell. The catalytic efficiency defined as FTIR absorption band intensities I(CO 2) was maximum for sample prepared at pH=1.5, and mainly correlated to crystallite dimensions. No significant catalytic effect was observed from sintered RuO 2 samples.

Modeling a solar-heated anaerobic digester for the developing world using system dynamics

NASA Astrophysics Data System (ADS)

Bentley, Johanna Lynn

Much of the developing world lacks access to a dependable source of energy. Agricultural societies such as Mozambique and Papua New Guinea could sustain a reliable energy source through the microbacterial decomposition of animal and crop waste. Anaerobic digestion produces methane, which can be used directly for heating, cooking, and lighting. Adding a solar component to the digester provides a catalyst for bacteria activity, accelerating digestion and increasing biogas production. Using methane decreases the amount of energy expended by collecting and preparing firewood, eliminates hazardous health effects linked to inhalation of particles, and provides energy close to where it is needed. The purpose of this work is two fold: initial efforts focus on the development and validation of a computer-based system dynamics model that combines elements of the anaerobic digestion process in order to predict methane output; second, the model is flexed to explore how the addition of a solar component increases robustness of the design, examines predicted biogas generation as a function of varying input conditions, and determines how best to configure such systems for use in varying developing world environments. Therefore, the central components of the system: solar insolation, waste feedstock, bacteria population and consumption rates, and biogas production are related both conceptually and mathematically through a serious of equations, conversions, and a causal loop and feedback diagram. Given contextual constraints and initial assumptions for both locations, it was determined that solar insolation and subsequent digester temperature control, amount of waste, and extreme weather patterns had the most significant impact on the system as a whole. Model behavior was both reproducible and comparable to that demonstrated in existing experimental systems. This tool can thus be flexed to fit specific contexts within the developing world to improve the standard of living of many people, without significantly altering everyday activities.

Seasonal methane and nitrous oxide emissions of several rice cultivars in direct-seeded systems

USDA-ARS?s Scientific Manuscript database

Understanding cultivar effects on field greenhouse gas (GHG) emissions in rice (Oryza sativa L.) systems is needed to improve the accuracy of predictive models used for estimating GHG emissions and determine to what extent choice of cultivar may have on GHG mitigation. We compared methane (CH4) and...

Sedimentary Rocks and Methane - Southwest Arabia Terra

NASA Technical Reports Server (NTRS)

Allen, Carlton C.; Oehler, Dorothy Z.; Venechuk, Elizabeth M.

2006-01-01

We propose to land the Mars Science Laboratory in southwest Arabia Terra to study two key aspects of martian history the extensive record of sedimentary rocks and the continuing release of methane. The results of this exploration will directly address the MSL Scientific Objectives regarding biological potential, geology and geochemistry, and past habitability.

Methane fugitive emissions quantification using the novel 'plume camera' (spatial correlation) method

NASA Astrophysics Data System (ADS)

Crosson, E.; Rella, C.

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, the importance of quantifying methane emissions becomes clear. The rapidly increasing reliance on shale gas (or other unconventional sources) is only intensifying the interest in fugitive methane releases. Natural gas (which is predominantly methane) is an attractive energy source, as it emits 40% less carbon dioxide per Joule of energy generated than coal. However, if just a small percentage of the natural gas consumed is lost due to fugitive emissions during production, processing, or transport, this global warming benefit is lost (Howarth et al. 2012). It is therefore imperative, as production of natural gas increases, that the fugitive emissions of methane are quantified accurately. Traditional direct measurement techniques often involve physical access of the leak itself to quantify the emissions rate, and are generally require painstaking effort to first find the leak and then quantify the emissions rate. With over half a million natural gas producing wells in the U.S. (U.S. Energy Information Administration), not including the associated processing, storage, and transport facilities, and with each facility having hundreds or even thousands of fittings that can potentially leak, the need is clear to develop methodologies that can provide a rapid and accurate assessment of the total emissions rate on a per-well head basis. In this paper we present a novel method for emissions quantification which uses a 'plume camera' with three 'pixels' to quantify emissions using direct measurements of methane concentration in the downwind plume. By analyzing the spatial correlation between the pixels, the spatial extent of the instantaneous plume can be inferred. This information, when combined with the wind speed through the measurement plane, provides a direct measurement of the emission rate. One example of this method is shown in Fig. 1. This method is simple to deploy, does not require an accurate model of atmospheric transport or knowledge of the distance to the emission source or its spatial distribution. Accurate measurements of the emissions can be made with just a few minutes of data collection. Results of controlled release methane experiments are presented, and the strengths and limitations of the methodology are discussed. REFERENCES R. Howarth, R. Santoro, and A. Ingraffea (2011): "Methane and the greenhouse-gas footprint of natural gas from shale formations," Climatic Change 106, 679 - 690. Fig 1: Spatial correlation analysis for two measurement points (or pixels) distributed vertically (A and B) or horizontally (A and C), for measurements at a distance of 21 meters from a methane point source of 650 sccm. The emission rate recovered from this analysis was 496 ± 160 sccm of CH4. The total measurement time was 30 minutes.

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

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Direct-Conversion Molecular Breast Imaging of Invasive Breast Cancer: Imaging Features, Extent of Invasive Disease, and Comparison Between Invasive Ductal and Lobular Histology.

PubMed

Conners, Amy Lynn; Jones, Katie N; Hruska, Carrie B; Geske, Jennifer R; Boughey, Judy C; Rhodes, Deborah J

2015-09-01

The purposes of this study were to compare the tumor appearance of invasive breast cancer on direct-conversion molecular breast imaging using a standardized lexicon and to determine how often direct-conversion molecular breast imaging identifies all known invasive tumor foci in the breast, and whether this differs for invasive ductal versus lobular histologic profiles. Patients with prior invasive breast cancer and concurrent direct-conversion molecular breast imaging examinations were retrospectively reviewed. Blinded review of direct-conversion molecular breast imaging examinations was performed by one of two radiologists, according to a validated lexicon. Direct-conversion molecular breast imaging findings were matched with lesions described on the pathology report to exclude benign reasons for direct-conversion molecular breast imaging findings and to document direct-conversion molecular breast imaging-occult tumor foci. Associations between direct-conversion molecular breast imaging findings and tumor histologic profiles were examined using chi-square tests. In 286 patients, 390 invasive tumor foci were present in 294 breasts. A corresponding direct-conversion molecular breast imaging finding was present for 341 of 390 (87%) tumor foci described on the pathology report. Invasive ductal carcinoma (IDC) tumor foci were more likely to be a mass (40% IDC vs 15% invasive lobular carcinoma [ILC]; p < 0.001) and to have marked intensity than were ILC foci (63% IDC vs 32% ILC; p < 0.001). Direct-conversion molecular breast imaging correctly revealed all pathology-proven foci of invasive disease in 79.8% of cases and was more likely to do so for IDC than for ILC (86.1% vs 56.7%; p < 0.0001). Overall, direct-conversion molecular breast imaging showed all known invasive foci in 249 of 286 (87%) patients. Direct-conversion molecular breast imaging features of invasive cancer, including lesion type and intensity, differ by histologic subtype. Direct-conversion molecular breast imaging is less likely to show all foci of ILC compared with IDC.

Model for estimating enteric methane emissions from United States dairy and feedlot cattle.

PubMed

Kebreab, E; Johnson, K A; Archibeque, S L; Pape, D; Wirth, T

2008-10-01

Methane production from enteric fermentation in cattle is one of the major sources of anthropogenic greenhouse gas emission in the United States and worldwide. National estimates of methane emissions rely on mathematical models such as the one recommended by the Intergovernmental Panel for Climate Change (IPCC). Models used for prediction of methane emissions from cattle range from empirical to mechanistic with varying input requirements. Two empirical and 2 mechanistic models (COWPOLL and MOLLY) were evaluated for their prediction ability using individual cattle measurements. Model selection was based on mean square prediction error (MSPE), concordance correlation coefficient, and residuals vs. predicted values analyses. In dairy cattle, COWPOLL had the lowest root MSPE and greatest accuracy and precision of predicting methane emissions (correlation coefficient estimate = 0.75). The model simulated differences in diet more accurately than the other models, and the residuals vs. predicted value analysis showed no mean bias (P = 0.71). In feedlot cattle, MOLLY had the lowest root MSPE with almost all errors from random sources (correlation coefficient estimate = 0.69). The IPCC model also had good agreement with observed values, and no significant mean (P = 0.74) or linear bias (P = 0.11) was detected when residuals were plotted against predicted values. A fixed methane conversion factor (Ym) might be an easier alternative to diet-dependent variable Ym. Based on the results, the 2 mechanistic models were used to simulate methane emissions from representative US diets and were compared with the IPCC model. The average Ym in dairy cows was 5.63% of GE (range 3.78 to 7.43%) compared with 6.5% +/- 1% recommended by IPCC. In feedlot cattle, the average Ym was 3.88% (range 3.36 to 4.56%) compared with 3% +/- 1% recommended by IPCC. Based on our simulations, using IPCC values can result in an overestimate of about 12.5% and underestimate of emissions by about 9.8% for dairy and feedlot cattle, respectively. In addition to providing improved estimates of emissions based on diets, mechanistic models can be used to assess mitigation options such as changing source of carbohydrate or addition of fat to decrease methane, which is not possible with empirical models. We recommend national inventories use diet-specific Ym values predicted by mechanistic models to estimate methane emissions from cattle.

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

Pig feeding strategy coupled with effluent management - fresh or stored slurry, solid phase separation - on methane potential and methane conversion factors during storage

NASA Astrophysics Data System (ADS)

Jarret, Guillaume; Martinez, José; Dourmad, Jean-Yves

2011-11-01

In the guideline for the determination of methane (CH 4) emission from animal manure (IPCC) the amount of CH 4 emitted is generally calculated according to an equation combining the amount of organic matter (OM) or volatile solids excreted, the ultimate CH 4 potential ( B0) of excreta and a system-specific methane conversion factor (MCF, %) that reflects the portion of B0 that is really converted into CH 4. The objective of the present study was to investigate the effect of the modification of dietary crude protein and fibre levels on B0 of pig slurry and on subsequent MCF according to different strategies of slurry management. Five experimental diets differing mainly in their crude protein and fibre content were compared. Two types of measurement of CH 4 emission were performed. The first was the measurement of B0 of slurry using biomethanogene potential (BMP) test. The second consisted in a storage simulation, which was performed on different kinds of effluents: fresh slurry (FSl), stored slurry (SSl), and faeces mixed with water (FaW). The type of diet and the type of effluent affected ( P < 0.001) CH 4 production after 30, 50 and 100 days. Moreover, the interaction between type of effluent and type of diet was significant for CH 4 emission and for MCF. CH 4 production was the highest for BMP, the average production of CH 4 during storage from FaW, FSl and SSl samples representing 77%, 58% and 64% of the B0 value. The dynamic of CH 4 production during BMP tests was rather similar for all dietary treatments whereas it differed for storage simulation studies with significant effects of dietary CP and fibre contents. The results from this study indicate that the type of diet has a significant but rather limited effect on B0 value of effluent. The effect of diet is much more marked on MCF, with lower values for high protein diets, and higher values for high fibre diets. MCF is also affected by manure management, the values measured on separated faeces from urine being much higher than for slurry.

Methane production in the sulfate-depleted sediments of two marine basins

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

Kuivila, K.M.; Murray, J.W.; Devol, A.H.

1990-02-01

Rates of methane production via both acetate fermentation and CO{sub 2} reduction were directly measured with radiotracer techniques in the sulfate-depleted sediments of Saanich and Princess Louisa Inlets. Comparison of measured and modeled rates suggests that these two pathways account for the majority of methane produced below the sulfate reduction zone in the sediments of both basins. Methane production via CO{sub 2} reduction was slightly more important than acetate fermentation with 57-58% of the methane in Saanich Inlet and 52-57% in Princess Louisa Inlet being produced from bicarbonate. The results from Saanich Inlet, a seasonally anoxic basin, are compared withmore » Princess Louisa Inlet, with a permanently oxic hypolimnion. Although the two basins have comparable organic-carbon rain rates, the rates of methanogenesis are much lower in Princess Louisa Inlet. This decrease in methane production can be attributed to the consumption of organic carbon via aerobic respiration occurring in the surface sediments of Princess Louisa Inlet, thereby decreasing the actual input of organic carbon to the zone of methane production. The relative importance of CO{sub 2} reduction and acetate fermentation in the production of methane was the same in both basins, suggesting that prior aerobic degradation of the organic matter has little influence on the pathways of methane production. The results from this study in the two marine systems (high sulfate) are also compared to published studies in freshwater environments (low sulfate) where acetate fermentation is the predominant pathway of methane production.« less

Relationships between CH4 emission, biomass, and CO2 exchange in a subtropical grassland

NASA Technical Reports Server (NTRS)

Whiting, Gary J.; Chanton, Jeffrey P.; Happell, James D.; Bartlett, David S.

1991-01-01

Methane flux was linearly correlated with plant biomass (r = 0.97, n = 6 and r = 0.95, n = 8) at two locations in a Florida Everglades Cladium marsh. One location, which had burned 4 months previously, exhibited a greater increase in methane flux as a function of biomass relative to sites at an unburned location. However, methane flux data from both sites fit a single regression (r = 0.94, n = 14) when plotted against net CO2 exchange suggesting that either methanogenesis in Everglades marl sediments is fueled by root exudation below ground, or that factors which enhance photosynthetic production and plant growth are also correlated with methane production and flux in this oligotrophic environment. The data presented are the first to show a direct relationship between spatial variability in plant biomass, net ecosystem production, and methane emission in a natural wetland.

Remote detection of methane with a 1.66-microm diode laser.

PubMed

Uehara, K; Tai, H

1992-02-20

High-sensitivity real-time remote detection of methane in air with a 1.66-microm distributed-feedback diode laser operating at room temperature is demonstrated by laboratory simulations. The laser current was modulated at a high frequency of ~5 MHz, and the laser-center frequency was locked onto a methane-absorption line. The laser light directed toward the probed region was received after one-way transmission or further reflection from a topographic target. The methane absorption was detected by the second-harmonic component in the optical-power variation. The minimum-detectable concentration-path-length product in the transmission scheme was 0.3 part in 10(6) m for a signal averaging time of 1.3 s. In the reflection scheme, the amount of methane could be measured from the ratio of the fundamental and second-harmonic signal intensities independently of the received power.

Methanogens: Methane Producers of the Rumen and Mitigation Strategies

PubMed Central

Hook, Sarah E.; Wright, André-Denis G.; McBride, Brian W.

2010-01-01

Methanogens are the only known microorganisms capable of methane production, making them of interest when investigating methane abatement strategies. A number of experiments have been conducted to study the methanogen population in the rumen of cattle and sheep, as well as the relationship that methanogens have with other microorganisms. The rumen methanogen species differ depending on diet and geographical location of the host, as does methanogenesis, which can be reduced by modifying dietary composition, or by supplementation of monensin, lipids, organic acids, or plant compounds within the diet. Other methane abatement strategies that have been investigated are defaunation and vaccines. These mitigation methods target the methanogen population of the rumen directly or indirectly, resulting in varying degrees of efficacy. This paper describes the methanogens identified in the rumens of cattle and sheep, as well as a number of methane mitigation strategies that have been effective in vivo. PMID:21253540

Metabolic stratification driven by surface and subsurface interactions in a terrestrial mud volcano.

PubMed

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

PubMed Central

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

Computer simulations of adsorption and diffusion for binary mixtures of methane and hydrogen in titanosilicates.

PubMed

Mitchell, Martha C; Gallo, Marco; Nenoff, Tina M

2004-07-22

Equilibrium molecular dynamics (MD) simulations of equimolar mixtures of hydrogen and methane were performed in three different titanosilicates: naturally occurring zorite and two synthetic titanosilicates, ETS-4 and ETS-10. In addition, single-component MD simulations and adsorption isotherms generated using grand canonical Monte Carlo simulations were performed to support the mixture simulations. The goal of this study was to determine the best membrane material to carry out hydrogen/methane separations. ETS-10 has a three-dimensional pore network. ETS-4 and zorite have two-dimensional pore networks. The simulations carried out in this study show that the increased porosity of ETS-10 results in self-diffusion coefficients for both hydrogen and methane that are higher in ETS-10 than in either ETS-4 or zorite. Methane only showed appreciable displacement in ETS-10. The ability of the methane molecules to move in all three directions in ETS-10 was demonstrated by the high degree of isotropy shown in the values of the x, y, and z components of the self-diffusion coefficient for methane in ETS-10. From our simulations we conclude that ETS-10 would be better suited for fast industrial separations of hydrogen and methane. However, the separation would not result in a pure hydrogen stream. In contrast, ETS-4 and zorite would act as true molecular sieves for separations of hydrogen and methane, as the methane would not move through membranes made of these materials. This was indicated by the near-zero self-diffusion coefficient of methane in ETS-4 and zorite.

Computer simulations of adsorption and diffusion for binary mixtures of methane and hydrogen in titanosilicates

NASA Astrophysics Data System (ADS)

Mitchell, Martha C.; Gallo, Marco; Nenoff, Tina M.

2004-07-01

Equilibrium molecular dynamics (MD) simulations of equimolar mixtures of hydrogen and methane were performed in three different titanosilicates: naturally occurring zorite and two synthetic titanosilicates, ETS-4 and ETS-10. In addition, single-component MD simulations and adsorption isotherms generated using grand canonical Monte Carlo simulations were performed to support the mixture simulations. The goal of this study was to determine the best membrane material to carry out hydrogen/methane separations. ETS-10 has a three-dimensional pore network. ETS-4 and zorite have two-dimensional pore networks. The simulations carried out in this study show that the increased porosity of ETS-10 results in self-diffusion coefficients for both hydrogen and methane that are higher in ETS-10 than in either ETS-4 or zorite. Methane only showed appreciable displacement in ETS-10. The ability of the methane molecules to move in all three directions in ETS-10 was demonstrated by the high degree of isotropy shown in the values of the x, y, and z components of the self-diffusion coefficient for methane in ETS-10. From our simulations we conclude that ETS-10 would be better suited for fast industrial separations of hydrogen and methane. However, the separation would not result in a pure hydrogen stream. In contrast, ETS-4 and zorite would act as true molecular sieves for separations of hydrogen and methane, as the methane would not move through membranes made of these materials. This was indicated by the near-zero self-diffusion coefficient of methane in ETS-4 and zorite.

The interaction of climate change and methane hydrates

USGS Publications Warehouse

Ruppel, Carolyn D.; Kessler, John D.

2017-01-01

Gas hydrate, a frozen, naturally-occurring, and highly-concentrated form of methane, sequesters significant carbon in the global system and is stable only over a range of low-temperature and moderate-pressure conditions. Gas hydrate is widespread in the sediments of marine continental margins and permafrost areas, locations where ocean and atmospheric warming may perturb the hydrate stability field and lead to release of the sequestered methane into the overlying sediments and soils. Methane and methane-derived carbon that escape from sediments and soils and reach the atmosphere could exacerbate greenhouse warming. The synergy between warming climate and gas hydrate dissociation feeds a popular perception that global warming could drive catastrophic methane releases from the contemporary gas hydrate reservoir. Appropriate evaluation of the two sides of the climate-methane hydrate synergy requires assessing direct and indirect observational data related to gas hydrate dissociation phenomena and numerical models that track the interaction of gas hydrates/methane with the ocean and/or atmosphere. Methane hydrate is likely undergoing dissociation now on global upper continental slopes and on continental shelves that ring the Arctic Ocean. Many factors—the depth of the gas hydrates in sediments, strong sediment and water column sinks, and the inability of bubbles emitted at the seafloor to deliver methane to the sea-air interface in most cases—mitigate the impact of gas hydrate dissociation on atmospheric greenhouse gas concentrations though. There is no conclusive proof that hydrate-derived methane is reaching the atmosphere now, but more observational data and improved numerical models will better characterize the climate-hydrate synergy in the future.

The interaction of climate change and methane hydrates

NASA Astrophysics Data System (ADS)

Ruppel, Carolyn D.; Kessler, John D.

2017-03-01

Gas hydrate, a frozen, naturally-occurring, and highly-concentrated form of methane, sequesters significant carbon in the global system and is stable only over a range of low-temperature and moderate-pressure conditions. Gas hydrate is widespread in the sediments of marine continental margins and permafrost areas, locations where ocean and atmospheric warming may perturb the hydrate stability field and lead to release of the sequestered methane into the overlying sediments and soils. Methane and methane-derived carbon that escape from sediments and soils and reach the atmosphere could exacerbate greenhouse warming. The synergy between warming climate and gas hydrate dissociation feeds a popular perception that global warming could drive catastrophic methane releases from the contemporary gas hydrate reservoir. Appropriate evaluation of the two sides of the climate-methane hydrate synergy requires assessing direct and indirect observational data related to gas hydrate dissociation phenomena and numerical models that track the interaction of gas hydrates/methane with the ocean and/or atmosphere. Methane hydrate is likely undergoing dissociation now on global upper continental slopes and on continental shelves that ring the Arctic Ocean. Many factors—the depth of the gas hydrates in sediments, strong sediment and water column sinks, and the inability of bubbles emitted at the seafloor to deliver methane to the sea-air interface in most cases—mitigate the impact of gas hydrate dissociation on atmospheric greenhouse gas concentrations though. There is no conclusive proof that hydrate-derived methane is reaching the atmosphere now, but more observational data and improved numerical models will better characterize the climate-hydrate synergy in the future.

The interaction of climate change and methane hydrates

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

Ruppel, Carolyn D.; Kessler, John D.

Gas hydrate, a frozen, naturally-occurring, and highly-concentrated form of methane, sequesters significant carbon in the global system and is stable only over a range of low-temperature and moderate-pressure conditions. Gas hydrate is widespread in the sediments of marine continental margins and permafrost areas, locations where ocean and atmospheric warming may perturb the hydrate stability field and lead to release of the sequestered methane into the overlying sediments and soils. Methane and methane-derived carbon that escape from sediments and soils and reach the atmosphere could exacerbate greenhouse warming. The synergy between warming climate and gas hydrate dissociation feeds a popular perceptionmore » that global warming could drive catastrophic methane releases from the contemporary gas hydrate reservoir. Appropriate evaluation of the two sides of the climate-methane hydrate synergy requires assessing direct and indirect observational data related to gas hydrate dissociation phenomena and numerical models that track the interaction of gas hydrates/methane with the ocean and/or atmosphere. Methane hydrate is likely undergoing dissociation now on global upper continental slopes and on continental shelves that ring the Arctic Ocean. Many factors—the depth of the gas hydrates in sediments, strong sediment and water column sinks, and the inability of bubbles emitted at the seafloor to deliver methane to the sea-air interface in most cases—mitigate the impact of gas hydrate dissociation on atmospheric greenhouse gas concentrations though. There is no conclusive proof that hydrate-derived methane is reaching the atmosphere now, but more observational data and improved numerical models will better characterize the climate-hydrate synergy in the future.« less

The interaction of climate change and methane hydrates

DOE PAGES

Ruppel, Carolyn D.; Kessler, John D.

2016-12-14

Gas hydrate, a frozen, naturally-occurring, and highly-concentrated form of methane, sequesters significant carbon in the global system and is stable only over a range of low-temperature and moderate-pressure conditions. Gas hydrate is widespread in the sediments of marine continental margins and permafrost areas, locations where ocean and atmospheric warming may perturb the hydrate stability field and lead to release of the sequestered methane into the overlying sediments and soils. Methane and methane-derived carbon that escape from sediments and soils and reach the atmosphere could exacerbate greenhouse warming. The synergy between warming climate and gas hydrate dissociation feeds a popular perceptionmore » that global warming could drive catastrophic methane releases from the contemporary gas hydrate reservoir. Appropriate evaluation of the two sides of the climate-methane hydrate synergy requires assessing direct and indirect observational data related to gas hydrate dissociation phenomena and numerical models that track the interaction of gas hydrates/methane with the ocean and/or atmosphere. Methane hydrate is likely undergoing dissociation now on global upper continental slopes and on continental shelves that ring the Arctic Ocean. Many factors—the depth of the gas hydrates in sediments, strong sediment and water column sinks, and the inability of bubbles emitted at the seafloor to deliver methane to the sea-air interface in most cases—mitigate the impact of gas hydrate dissociation on atmospheric greenhouse gas concentrations though. There is no conclusive proof that hydrate-derived methane is reaching the atmosphere now, but more observational data and improved numerical models will better characterize the climate-hydrate synergy in the future.« less

The FISH-SIMS Approach: Isotopic Imprints of Methane in Diverse Microbial Assemblages

NASA Astrophysics Data System (ADS)

Orphan, V. J.; House, C. H.; Hinrichs, K.; McKeegan, K. D.; Paull, C.; Ussler, W.; DeLong, E. F.

2001-12-01

One of the more important biogeochemical processes influencing carbon turnover in continental margin environments and cold seeps is the anaerobic oxidation of methane (AOM). Although there is convincing biogeochemical evidence for archaeal/sulfate-reducer cooperative involvement in AOM, methane-consuming anaerobic microorganisms have eluded identification until only very recently. Parallel phylogenetic gene surveys and isotopic determination of lipid biomarkers in methane-rich seep sediments suggested that diverse archaeal and bacterial assemblages are involved in AOM. Specifically, a novel clade of Archaea related to known methanogens (ANME-1 group), as well as microorganisms affiliated with the Methanosarcinales (ANME-2 group) and their syntrophic sulfate-reducing bacterial partner affiliated with the Desulfosarcina, have been identified as likely candidate methane-oxidizing microorganisms. Both 16S rDNA and lipid analyses provide only circumstantial evidence linking these specific groups to AOM, however, because they are based on bulk analyses of whole sediments, rather than on the level of single microorganisms. In this study, we provide the first concrete evidence directly linking two distinct groups of Archaea, the uncultured consortium archaeal ANME-2/ bacterial Desulfosarcina spp. and the archaeal ANME-1 to methane consumption in anoxic marine sediments. Using a novel approach combining fluorescent in situ hybridization (FISH) and secondary ion mass spectrometry (SIMS), we identified aggregations of ANME-2/ Desulfosarcina and single cells and aggregates of ANME-1 from methane seep sediments and directly determined the carbon stable isotopic composition for the individual cells and cell aggregates. Both archaeal groups ANME-1 and ANME-2 displayed isotopic signatures suggestive of methane assimilation, with extreme 13C depletion (down to -97 per mil). In comparison, the carbon isotopic composition of microorganisms from the same sample not targeted with either the archaeal ANME-1 or ANME-2 specific rRNA probe sets had 13C values averaging -30 per mil. Interestingly, large bacterial filaments resembling sulfide-oxidizing Beggiatoa were slightly more depleted in 13C (approx. -50 per mil), and may signify ecosystem-wide incorporation of methane-derived endproducts. The combined application of FISH and SIMS serves as a new useful tool in geomicrobiology for deciphering the metabolic function of environmental microorganisms in situ.

Methane flux and carbon isotope composition correlate to shifting plant and microbial communities along a permafrost thaw gradient

NASA Astrophysics Data System (ADS)

McCalley, C. K.; Mondav, R.; Chanton, J.; Crill, P. M.; Hodgkins, S. B.; Kim, E.; Rich, V. I.; Wehr, R.; Woodcroft, B. J.; Tyson, G. W.; Saleska, S. R.

2012-12-01

Methane flux from high latitude wetlands is a critical component of the global carbon budget and is highly sensitive to climate change, with observed and predicted increases as permafrost thaws. Microorganisms mediate wetland methane cycling, but connections between ecosystem-scale flux and underlying microbial dynamics are poorly understood. To address this gap we used isotopic (laser absorption spectrometry) and molecular (16S rRNA gene amplicon sequencing) techniques in a high latitude (68° N) wetland to investigate the relationship between microbial community composition and methane emissions across a permafrost thaw gradient. The transition from permafrost dominated, well drained palsas, through intermediate thaw sites dominated by Sphagnum spp., to wet sites with no underlying permafrost dominated by Eriophorum angustifolium is associated with substantial increases in methane emission. Across this thaw progression the carbon isotopic composition of emitted methane increased from -79.5 ‰ in the intermediate-thawing site to -66.4 ‰ in the thawed site, indicating a relative shift from CO2-reductive towards acetoclastic methanogenesis. Increases in methane flux under thaw were correlated with increasing abundance of methane-producing archaeal clades and increases in methane isotopic composition were associated with shifts in the archaeal community. While CO2 reducing methanogens were found throughout thawing and thawed sites, methanogens of the Methanosarcina (the order of Archaea that contains all known acetoclastic methanogens) were most associated with the fully thawed site. These results directly link microbial community composition to ecosystem scale changes in the magnitude and isotopic composition of methane emissions under permafrost thaw. If isotopic shifts of this magnitude are characteristic of methane dynamics under permafrost loss they should also become detectable in global atmospheric methane observations, providing a global scale tracer of shifting microbial communities associated with permafrost thaw.

Production of H2 from aluminium/water reaction and its potential for CO2 methanation

NASA Astrophysics Data System (ADS)

Khai Phung, Khor; Sethupathi, Sumathi; Siang Piao, Chai

2018-04-01

Carbon dioxide (CO2) is a natural gas that presents in excess in the atmosphere. Owing to its ability to cause global warming, capturing and conversion of CO2 have attracted much attention worldwide. CO2 methanation using hydrogen (H2) is believed to be a promising route for CO2 removal. In the present work, H2 is produced using aluminum-water reaction and tested for its ability to convert CO2 to methane (CH4). Different type of water i.e. tap water, distilled water, deionized water and ultrapure water, concentration of sodium hydroxide (NaOH) (0.2 M to 1.0 M) and particle size of aluminum (45 m to 500 μm) were varied as parameter study. It was found that the highest yield of H2 was obtained using distilled water, 1.0 M of NaOH and 45μm particle size of aluminium. However, the highest yield of methane was achieved using a moderate and progressive H2 production (distilled water, 0.6 M of NaOH and 45 μm particle size of aluminium) which allowed sufficient time for H2 to react with CO2. It was concluded that 1130 ml of H2 can produce about 560 ppm of CH4 within 25 min of batch reaction using nickel catalyst.

Effect of aerobic pre-treatment on hydrogen and methane production in a two-stage anaerobic digestion process using food waste with different compositions.

PubMed

Rafieenia, Razieh; Girotto, Francesca; Peng, Wei; Cossu, Raffaello; Pivato, Alberto; Raga, Roberto; Lavagnolo, Maria Cristina

2017-01-01

Aerobic pre-treatment was applied prior to two-stage anaerobic digestion process. Three different food wastes samples, namely carbohydrate rich, protein rich and lipid rich, were prepared as substrates. Effect of aerobic pre-treatment on hydrogen and methane production was studied. Pre-aeration of substrates showed no positive impact on hydrogen production in the first stage. All three categories of pre-aerated food wastes produced less hydrogen compared to samples without pre-aeration. In the second stage, methane production increased for aerated protein rich and carbohydrate rich samples. In addition, the lag phase for carbohydrate rich substrate was shorter for aerated samples. Aerated protein rich substrate yielded the best results among substrates for methane production, with a cumulative production of approximately 351ml/gVS. With regard to non-aerated substrates, lipid rich was the best substrate for CH 4 production (263ml/gVS). Pre-aerated P substrate was the best in terms of total energy generation which amounted to 9.64kJ/gVS. This study revealed aerobic pre-treatment to be a promising option for use in achieving enhanced substrate conversion efficiencies and CH 4 production in a two-stage AD process, particularly when the substrate contains high amounts of proteins. Copyright © 2016 Elsevier Ltd. All rights reserved.

Uptake and effect of rare earth elements on gene expression in Methylosinus trichosporium OB3b

DOE PAGES

Gu, Wenyu; Farhan Ul Haque, Muhammad; DiSpirito, Alan A.; ...

2016-05-12

It is well-known that M. trichosporium OB3b has two forms of methane monooxygenase responsible for the initial conversion of methane to methanol, a cytoplasmic (soluble) methane monooxygenase (sMMO) and a membrane-associated (particulate) methane monooxygenase (pMMO) and that copper strongly regulates expression of these alternative forms of MMO. More recently, it has been discovered that M. trichosporium OB3b has multiple types of the methanol dehydrogenase (MeDH), i.e. the Mxa-MeDH and Xox-MeDH, and the expression of these two forms is regulated by the availability of the rare earth element, cerium. Here we extend these studies and show that lanthanum, praseodymium, neodymium andmore » samarium also regulate expression of alternative forms of MeDH. The effect of these rare earth elements on MeDH expression, however, was only observed in the absence of copper. Further, a mutant of M. trichosporium OB3b where the Mxa-MeDH was knocked out was able to grow in the presence of lanthanum, praseodymium and neodymium, but was not able to grow in the presence of samarium. In conclusion, collectively these data suggest that multiple levels of gene regulation by metals exist in M. trichosporium OB3b but that copper overrides the effect of other metals by an as yet unknown mechanism.« less

Trash-to-Gas: Using Waste Products to Minimize Logistical Mass During Long Duration Space Missions

NASA Technical Reports Server (NTRS)

Hintze, Paul E.; Caraccio, A. J.; Anthony, S. M.; Tsoras, A. N.; Devor, Robert; Captain, James G.; Nur, Mononita

2013-01-01

Just as waste-to-energy processes utilizing municipal landftll and biomass wastes are finding increased terrestrial uses, the Trash-to-Gas (TtG) project seeks to convert waste generated during spaceflight into high value commodities. These include methane for propulsion and water for life support in addition to a variety of other gasses. TtG is part of the Logistic Reduction and Repurposing (LRR) project under the NASA Advanced Exploration Systems Program. The LRR project will enable a largely mission-independent approach to minimize logistics contributions to total mission architecture mass. LRR includes technologies that reduce the amount of consumables that need to be sent to space, repurpose items sent to space, or convert wastes to commodities. Currently, waste generated on the International Space Station is stored inside a logistic module which is de-orbited into Earth's atmosphere for destruction. The waste consists of food packaging, food, clothing and other items. This paper will discuss current results on incineration as a waste processing method. Incineration is part of a two step process to produce methane from waste: first the waste is converted to carbon oxides; second, the carbon oxides are fed to a Sabatier reactor where they are converted to methane. The quantities of carbon dioxide, carbon monoxide, methane and water were measured under the different thermal degradation conditions. The overall carbon conversion efficiency and water recovery are discussed

Trash-to-Gas: Using Waste Products to Minimize Logistical Mass During Long Duration Space Missions

NASA Technical Reports Server (NTRS)

Hintze, Paul. E.; Caraccio, Anne J.; Anthony, Stephen M.; Tsoras, Alexandra N.; Nur, Monoita; Devor, Robert; Captain, James G.

2013-01-01

Just as waste-to-energy processes utilizing municipal landftll and biomass wastes are finding increased terrestrial uses, the Trash-to-Gas (TtG) project seeks to convert waste generated during spaceflight into high value commodities. These include methane for propulsion and water for life support in addition to a variety of other gasses. TtG is part of the Logistic Reduction and Repurposing (LRR) project under the NASA Advanced Exploration Systems Program. The LRR project will enable a largely mission-independent approach to minimize logistics contributions to total mission architecture mass. LRR includes technologies that reduce the amount of consumables that need to be sent to space, repurpose items sent to space, or convert wastes to commodities. Currently, waste generated on the International Space Station is stored inside a logistic module which is de-orbited into Earth's atmosphere for destruction. The waste consists of food packaging, food, clothing and other items. This paper will discuss current results on incineration as a waste processing method. Incineration is part of a two step process to produce methane from waste: first the waste is converted to carbon oxides; second, the carbon oxides are fed to a Sabatier reactor where they are converted to methane. The quantities of carbon dioxide, carbon monoxide, methane and water were measured under the different thermal degradation conditions. The overall carbon conversion efficiency and water recovery are discussed.

Formate-Dependent Microbial Conversion of CO2 and the Dominant Pathways of Methanogenesis in Production Water of High-temperature Oil Reservoirs Amended with Bicarbonate.

PubMed

Yang, Guang-Chao; Zhou, Lei; Mbadinga, Serge M; Liu, Jin-Feng; Yang, Shi-Zhong; Gu, Ji-Dong; Mu, Bo-Zhong

2016-01-01

CO2 sequestration in deep-subsurface formations including oil reservoirs is a potential measure to reduce the CO2 concentration in the atmosphere. However, the fate of the CO2 and the ecological influences in carbon dioxide capture and storage (CDCS) facilities is not understood clearly. In the current study, the fate of CO2 (in bicarbonate form; 0∼90 mM) with 10 mM of formate as electron donor and carbon source was investigated with high-temperature production water from oilfield in China. The isotope data showed that bicarbonate could be reduced to methane by methanogens and major pathway of methanogenesis could be syntrophic formate oxidation coupled with CO2 reduction and formate methanogenesis under the anaerobic conditions. The bicarbonate addition induced the shift of microbial community. Addition of bicarbonate and formate was associated with a decrease of Methanosarcinales, but promotion of Methanobacteriales in all treatments. Thermodesulfovibrio was the major group in all the samples and Thermacetogenium dominated in the high bicarbonate treatments. The results indicated that CO2 from CDCS could be transformed to methane and the possibility of microbial CO2 conversion for enhanced microbial energy recovery in oil reservoirs.

Formate-Dependent Microbial Conversion of CO2 and the Dominant Pathways of Methanogenesis in Production Water of High-temperature Oil Reservoirs Amended with Bicarbonate

PubMed Central

Yang, Guang-Chao; Zhou, Lei; Mbadinga, Serge M.; Liu, Jin-Feng; Yang, Shi-Zhong; Gu, Ji-Dong; Mu, Bo-Zhong

2016-01-01

CO2 sequestration in deep-subsurface formations including oil reservoirs is a potential measure to reduce the CO2 concentration in the atmosphere. However, the fate of the CO2 and the ecological influences in carbon dioxide capture and storage (CDCS) facilities is not understood clearly. In the current study, the fate of CO2 (in bicarbonate form; 0∼90 mM) with 10 mM of formate as electron donor and carbon source was investigated with high-temperature production water from oilfield in China. The isotope data showed that bicarbonate could be reduced to methane by methanogens and major pathway of methanogenesis could be syntrophic formate oxidation coupled with CO2 reduction and formate methanogenesis under the anaerobic conditions. The bicarbonate addition induced the shift of microbial community. Addition of bicarbonate and formate was associated with a decrease of Methanosarcinales, but promotion of Methanobacteriales in all treatments. Thermodesulfovibrio was the major group in all the samples and Thermacetogenium dominated in the high bicarbonate treatments. The results indicated that CO2 from CDCS could be transformed to methane and the possibility of microbial CO2 conversion for enhanced microbial energy recovery in oil reservoirs. PMID:27047478

Methane uptake in urban forests and lawns.

PubMed

Groffman, Peter M; Pouyat, Richard V

2009-07-15

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

Ethanol dehydration to ethylene in a stratified autothermal millisecond reactor.

PubMed

Skinner, Michael J; Michor, Edward L; Fan, Wei; Tsapatsis, Michael; Bhan, Aditya; Schmidt, Lanny D

2011-08-22

The concurrent decomposition and deoxygenation of ethanol was accomplished in a stratified reactor with 50-80 ms contact times. The stratified reactor comprised an upstream oxidation zone that contained Pt-coated Al(2)O(3) beads and a downstream dehydration zone consisting of H-ZSM-5 zeolite films deposited on Al(2)O(3) monoliths. Ethanol conversion, product selectivity, and reactor temperature profiles were measured for a range of fuel:oxygen ratios for two autothermal reactor configurations using two different sacrificial fuel mixtures: a parallel hydrogen-ethanol feed system and a series methane-ethanol feed system. Increasing the amount of oxygen relative to the fuel resulted in a monotonic increase in ethanol conversion in both reaction zones. The majority of the converted carbon was in the form of ethylene, where the ethanol carbon-carbon bonds stayed intact while the oxygen was removed. Over 90% yield of ethylene was achieved by using methane as a sacrificial fuel. These results demonstrate that noble metals can be successfully paired with zeolites to create a stratified autothermal reactor capable of removing oxygen from biomass model compounds in a compact, continuous flow system that can be configured to have multiple feed inputs, depending on process restrictions. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The Effect of Copper Addition on the Activity and Stability of Iron-Based CO₂ Hydrogenation Catalysts.

PubMed

Bradley, Matthew J; Ananth, Ramagopal; Willauer, Heather D; Baldwin, Jeffrey W; Hardy, Dennis R; Williams, Frederick W

2017-09-20

Iron-based CO₂ catalysts have shown promise as a viable route to the production of olefins from CO₂ and H₂ gas. However, these catalysts can suffer from low conversion and high methane selectivity, as well as being particularly vulnerable to water produced during the reaction. In an effort to improve both the activity and durability of iron-based catalysts on an alumina support, copper (10-30%) has been added to the catalyst matrix. In this paper, the effects of copper addition on the catalyst activity and morphology are examined. The addition of 10% copper significantly increases the CO₂ conversion, and decreases methane and carbon monoxide selectivity, without significantly altering the crystallinity and structure of the catalyst itself. The FeCu/K catalysts form an inverse spinel crystal phase that is independent of copper content and a metallic phase that increases in abundance with copper loading (>10% Cu). At higher loadings, copper separates from the iron oxide phase and produces metallic copper as shown by SEM-EDS. An addition of copper appears to increase the rate of the Fischer-Tropsch reaction step, as shown by modeling of the chemical kinetics and the inter- and intra-particle transport of mass and energy.

Clumped isotope effects during OH and Cl oxidation of methane

NASA Astrophysics Data System (ADS)

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

2017-01-01

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

The key nickel enzyme of methanogenesis catalyses the anaerobic oxidation of methane.

PubMed

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.

Modeling of Methane Migration in Shallow Aquifers from Shale Gas Well Drilling.

PubMed

Zhang, Liwei; Soeder, Daniel J

2016-05-01

The vertical portion of a shale gas well, known as the "tophole" is often drilled using an air-hammer bit that may introduce pressures as high as 2400 kPa (350 psi) into groundwater while penetrating shallow aquifers. A 3-D TOUGH2 model was used to simulate the flow of groundwater under the high hydraulic heads that may be imposed by such trapped compressed air, based on an observed case in West Virginia (USA) in 2012. The model realizations show that high-pressure air trapped in aquifers may cause groundwater to surge away from the drill site at observable velocities. If dissolved methane is present within the aquifer, the methane can be entrained and transported to a maximum distance of 10.6 m per day. Results from this study suggest that one cause of the reported increase in methane concentrations in groundwater near shale gas production wells may be the transport of pre-existing methane via groundwater surges induced by air drilling, not necessarily direct natural gas leakage from the unconventional gas reservoir. The primary transport mechanisms are advective transport of dissolved methane with water flow, and diffusive transport of dissolved methane. © 2015, National Ground Water Association.

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

USDA-ARS?s Scientific Manuscript database

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

Nanoplasmonic Catalysis for Synthetic Fuel Production

DTIC Science & Technology

2010-02-22

understanding of the basic mechanism underlying this enhancement with the ultimate goal of producing synthetic fuels, such as hydrogen , methane and...of producing synthetic fuels, such as hydrogen , methane and methanol using visible illumination. Objectives: - Fabricate arrays of metal...in our energy infrastructure. For photocatalysis , this area is especially exciting because it presents a possible route to direct solar-to-fuel

Integrated metagenomic analysis of the rumen microbiome of cattle reveals key biological mechanisms associated with methane traits.

PubMed

Wang, Haiying; Zheng, Huiru; Browne, Fiona; Roehe, Rainer; Dewhurst, Richard J; Engel, Felix; Hemmje, Matthias; Lu, Xiangwu; Walsh, Paul

2017-07-15

Methane is one of the major contributors to global warming. The rumen microbiota is directly involved in methane production in cattle. The link between variation in rumen microbial communities and host genetics has important applications and implications in bioscience. Having the potential to reveal the full extent of microbial gene diversity and complex microbial interactions, integrated metagenomics and network analysis holds great promise in this endeavour. This study investigates the rumen microbial community in cattle through the integration of metagenomic and network-based approaches. Based on the relative abundance of 1570 microbial genes identified in a metagenomics analysis, the co-abundance network was constructed and functional modules of microbial genes were identified. One of the main contributions is to develop a random matrix theory-based approach to automatically determining the correlation threshold used to construct the co-abundance network. The resulting network, consisting of 549 microbial genes and 3349 connections, exhibits a clear modular structure with certain trait-specific genes highly over-represented in modules. More specifically, all the 20 genes previously identified to be associated with methane emissions are found in a module (hypergeometric test, p<10 -11 ). One third of genes are involved in methane metabolism pathways. The further examination of abundance profiles across 8 samples of genes highlights that the revealed pattern of metagenomics abundance has a strong association with methane emissions. Furthermore, the module is significantly enriched with microbial genes encoding enzymes that are directly involved in methanogenesis (hypergeometric test, p<10 -9 ). Copyright © 2017 Elsevier Inc. All rights reserved.

Analysis of Ignition Behavior in a Turbocharged Direct Injection Dual Fuel Engine Using Propane and Methane as Primary Fuels

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

A process concept for the production of benzene-ethylene-SNG from coal using flash hydropyrolysis technology

NASA Astrophysics Data System (ADS)

Greene, M. I.; Ladelfa, C. J.; Bivacca, S. J.

1980-05-01

Flash hydropyrolysis (FHP) of coal is an emerging technology for the direct production of methane, ethane and BTX in a single-stage, high throughput reactor. The FHP technique involves the short residence time (1-2 seconds), rapid heatup of coal in a dilute-phase, transport reactor. When integrated into an overall, grass-roots conversion complex, the FHP technique can be utilized to generate a product consisting of SNG, ethylene/propylene, benzene and Fischer-Tropsch-based alcohols. This paper summarizes the process engineering and economics of conceptualized facility based on an FHP reactor operation with a lignitic coal. The plant is hypothetically sited near the extensive lignite fields located in the Texas region of the United States. Utilizing utility-financing methods for the costing of SNG, and selling the chemicals cogenerated at petrochemical market prices, the 20-year average SNG cost has been computed to vary between $3-4/MM Btu, depending upon the coal costs, interest rates, debt/equity ratio, coproduct chemicals prices, etc.

Comparison of complex effluent treatability in different bench scale microbial electrolysis cells.

PubMed

Ullery, Mark L; Logan, Bruce E

2014-10-01

A range of wastewaters and substrates were examined using mini microbial electrolysis cells (mini MECs) to see if they could be used to predict the performance of larger-scale cube MECs. COD removals and coulombic efficiencies corresponded well between the two reactor designs for individual samples, with 66-92% of COD removed for all samples. Current generation was consistent between the reactor types for acetate (AC) and fermentation effluent (FE) samples, but less consistent with industrial (IW) and domestic wastewaters (DW). Hydrogen was recovered from all samples in cube MECs, but gas composition and volume varied significantly between samples. Evidence for direct conversion of substrate to methane was observed with two of the industrial wastewater samples (IW-1 and IW-3). Overall, mini MECs provided organic treatment data that corresponded well with larger scale reactor results, and therefore it was concluded that they can be a useful platform for screening wastewater sources. Copyright © 2014 Elsevier Ltd. All rights reserved.