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.

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

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.

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

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.

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

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

Electricity from methane by reversing methanogenesis

PubMed Central

McAnulty, Michael J.; G. Poosarla, Venkata; Kim, Kyoung-Yeol; Jasso-Chávez, Ricardo; Logan, Bruce E.; Wood, Thomas K.

2017-01-01

Given our vast methane reserves and the difficulty in transporting methane without substantial leaks, the conversion of methane directly into electricity would be beneficial. Microbial fuel cells harness electrical power from a wide variety of substrates through biological means; however, the greenhouse gas methane has not been used with much success previously as a substrate in microbial fuel cells to generate electrical current. Here we construct a synthetic consortium consisting of: (i) an engineered archaeal strain to produce methyl-coenzyme M reductase from unculturable anaerobic methanotrophs for capturing methane and secreting acetate; (ii) micro-organisms from methane-acclimated sludge (including Paracoccus denitrificans) to facilitate electron transfer by providing electron shuttles (confirmed by replacing the sludge with humic acids), and (iii) Geobacter sulfurreducens to produce electrons from acetate, to create a microbial fuel cell that converts methane directly into significant electrical current. Notably, this methane microbial fuel cell operates at high Coulombic efficiency. PMID:28513579

Electricity from methane by reversing methanogenesis

NASA Astrophysics Data System (ADS)

McAnulty, Michael J.; G. Poosarla, Venkata; Kim, Kyoung-Yeol; Jasso-Chávez, Ricardo; Logan, Bruce E.; Wood, Thomas K.

2017-05-01

Given our vast methane reserves and the difficulty in transporting methane without substantial leaks, the conversion of methane directly into electricity would be beneficial. Microbial fuel cells harness electrical power from a wide variety of substrates through biological means; however, the greenhouse gas methane has not been used with much success previously as a substrate in microbial fuel cells to generate electrical current. Here we construct a synthetic consortium consisting of: (i) an engineered archaeal strain to produce methyl-coenzyme M reductase from unculturable anaerobic methanotrophs for capturing methane and secreting acetate; (ii) micro-organisms from methane-acclimated sludge (including Paracoccus denitrificans) to facilitate electron transfer by providing electron shuttles (confirmed by replacing the sludge with humic acids), and (iii) Geobacter sulfurreducens to produce electrons from acetate, to create a microbial fuel cell that converts methane directly into significant electrical current. Notably, this methane microbial fuel cell operates at high Coulombic efficiency.

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

NASA Astrophysics Data System (ADS)

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

2017-11-01

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

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

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

Shan, Junjun; Li, Mengwei; Allard, Lawrence F.

An efficient and direct method of catalytic conversion of methane to liquid methanol and other oxygenates would be of considerable practical value. However, it remains an unsolved problem in catalysis, as typically it involves expensive or corrosive oxidants or reaction media(5-8) that are not amenable to commercialization. Although methane can be directly converted to methanol using molecular oxygen under mild conditions in the gas phase, the process is either stoichiometric (and therefore requires a water extraction step) or is too slow and low-yielding to be practical. Methane could, in principle, also be transformed through direct oxidative carbonylation to acetic acid,more » which is commercially obtained through methane steam reforming, methanol synthesis, and subsequent methanol carbonylation on homogeneous catalysts. However, an effective catalyst for the direct carbonylation of methane to acetic acid, which might enable the economical small-scale utilization of natural gas that is currently flared or stranded, has not yet been reported. Here we show that mononuclear rhodium species, anchored on a zeolite or titanium dioxide support suspended in aqueous solution, catalyse the direct conversion of methane to methanol and acetic acid, using oxygen and carbon monoxide under mild conditions. Here, we find that the two products form through independent pathways, which allows us to tune the conversion: three-hour-long batch-reactor tests conducted at 150 degrees Celsius, using either the zeolitesupported or the titanium-dioxide-supported catalyst, yield around 22,000 micromoles of acetic acid per gram of catalyst, or around 230 micromoles of methanol per gram of catalyst, respectively, with selectivities of 60-100 per cent. Finally, we anticipate that these unusually high activities, despite still being too low for commercial application, may guide the development of optimized catalysts and practical processes for the direct conversion of methane to methanol, acetic acid and other useful chemicals.« less

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

DOE PAGES

Shan, Junjun; Li, Mengwei; Allard, Lawrence F.; ...

2017-11-30

An efficient and direct method of catalytic conversion of methane to liquid methanol and other oxygenates would be of considerable practical value. However, it remains an unsolved problem in catalysis, as typically it involves expensive or corrosive oxidants or reaction media(5-8) that are not amenable to commercialization. Although methane can be directly converted to methanol using molecular oxygen under mild conditions in the gas phase, the process is either stoichiometric (and therefore requires a water extraction step) or is too slow and low-yielding to be practical. Methane could, in principle, also be transformed through direct oxidative carbonylation to acetic acid,more » which is commercially obtained through methane steam reforming, methanol synthesis, and subsequent methanol carbonylation on homogeneous catalysts. However, an effective catalyst for the direct carbonylation of methane to acetic acid, which might enable the economical small-scale utilization of natural gas that is currently flared or stranded, has not yet been reported. Here we show that mononuclear rhodium species, anchored on a zeolite or titanium dioxide support suspended in aqueous solution, catalyse the direct conversion of methane to methanol and acetic acid, using oxygen and carbon monoxide under mild conditions. Here, we find that the two products form through independent pathways, which allows us to tune the conversion: three-hour-long batch-reactor tests conducted at 150 degrees Celsius, using either the zeolitesupported or the titanium-dioxide-supported catalyst, yield around 22,000 micromoles of acetic acid per gram of catalyst, or around 230 micromoles of methanol per gram of catalyst, respectively, with selectivities of 60-100 per cent. Finally, we anticipate that these unusually high activities, despite still being too low for commercial application, may guide the development of optimized catalysts and practical processes for the direct conversion of methane to methanol, acetic acid and other useful chemicals.« 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.

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.

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.

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

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.

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.

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.

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

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.

Method for the photocatalytic conversion of gas hydrates

DOEpatents

Taylor, Charles E.; Noceti, Richard P.; Bockrath, Bradley C.

2001-01-01

A method for converting methane hydrates to methanol, as well as hydrogen, through exposure to light. The process includes conversion of methane hydrates by light where a radical initiator has been added, and may be modified to include the conversion of methane hydrates with light where a photocatalyst doped by a suitable metal and an electron transfer agent to produce methanol and hydrogen. The present invention operates at temperatures below 0.degree. C., and allows for the direct conversion of methane contained within the hydrate in situ.

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.

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.

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.

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.

Photocatalytic conversion of methane to methanol

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

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

1995-12-31

A long-term goal of our research group is the exploration of novel pathways for the direct oxidation of methane to liquid fuels, chemicals, and intermediates. The use of three relatively abundant and inexpensive reactants, light, water, and methane, to produce methanol is attractive. The products of reaction, methanol and hydrogen, are both commercially desirable, methanol being used as is or converted to a variety of other chemicals, and the hydrogen could be utilized in petroleum and/or chemical manufacturing. Methane is produced as a by-product of coal gasification. Depending upon reactor design and operating conditions, up to 18% of total gasifiermore » product may be methane. In addition, there are vast proven reserves of geologic methane in the world. Unfortunately, a large fraction of these reserves are in regions where there is little local demand for methane and it is not economically feasible to transport it to a market. There is a global research effort under way in academia, industry, and government to find methods to convert methane to useful, more readily transportable and storable materials. Methanol, the initial product of methane oxidation, is a desirable product of conversion because it retains much of the original energy of the methane while satisfying transportation and storage requirements. Investigation of direct conversion of methane to transportation fuels has been an ongoing effort at PETC for over 10 years. One of the current areas of research is the conversion of methane to methanol, under mild conditions, using light, water, and a semiconductor photocatalyst. The use of three relatively abundant and inexpensive reactants, light, water, and methane, to produce methanol, is attractive. Research in the laboratory is directed toward applying the techniques developed for the photocatalytic splitting of the water and the photochemical conversion of methane.« less

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

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.

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.

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.

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

Mitigation of Humic Acid Inhibition in Anaerobic Digestion of Cellulose by Addition of Various Salts.

PubMed

Azman, Samet; Khadem, Ahmad F; Zeeman, Grietje; van Lier, Jules B; Plugge, Caroline M

2015-03-25

Humic compounds are inhibitory to the anaerobic hydrolysis of cellulosic biomass. In this study, the impact of salt addition to mitigate the inhibitory effects of humic compounds was investigated. The experiment was conducted using batch tests to monitor the anaerobic hydrolysis of cellulose in the presence of humic acid. Sodium, potassium, calcium, magnesium and iron salts were tested separately for their efficiency to mitigate humic acid inhibition. All experiments were done under mesophilic conditions (30 °C) and at pH 7. Methane production was monitored online, using the Automatic Methane Potential Test System. Methane production, soluble chemical oxygen demand and volatile fatty acid content of the samples were measured to calculate the hydrolysis efficiencies. Addition of magnesium, calcium and iron salts clearly mitigated the inhibitory effects of humic acid and hydrolysis efficiencies reached up to 75%, 65% and 72%, respectively, which were similar to control experiments. Conversely, potassium and sodium salts addition did not mitigate the inhibition and hydrolysis efficiencies were found to be less than 40%. Mitigation of humic acid inhibition via salt addition was also validated by inductively coupled plasma atomic emission spectroscopy analyses, which showed the binding capacity of different cations to humic acid.

Mitigation of Humic Acid Inhibition in Anaerobic Digestion of Cellulose by Addition of Various Salts

PubMed Central

Azman, Samet; Khadem, Ahmad F.; Zeeman, Grietje; van Lier, Jules B.; Plugge, Caroline M.

2015-01-01

Humic compounds are inhibitory to the anaerobic hydrolysis of cellulosic biomass. In this study, the impact of salt addition to mitigate the inhibitory effects of humic compounds was investigated. The experiment was conducted using batch tests to monitor the anaerobic hydrolysis of cellulose in the presence of humic acid. Sodium, potassium, calcium, magnesium and iron salts were tested separately for their efficiency to mitigate humic acid inhibition. All experiments were done under mesophilic conditions (30 °C) and at pH 7. Methane production was monitored online, using the Automatic Methane Potential Test System. Methane production, soluble chemical oxygen demand and volatile fatty acid content of the samples were measured to calculate the hydrolysis efficiencies. Addition of magnesium, calcium and iron salts clearly mitigated the inhibitory effects of humic acid and hydrolysis efficiencies reached up to 75%, 65% and 72%, respectively, which were similar to control experiments. Conversely, potassium and sodium salts addition did not mitigate the inhibition and hydrolysis efficiencies were found to be less than 40%. Mitigation of humic acid inhibition via salt addition was also validated by inductively coupled plasma atomic emission spectroscopy analyses, which showed the binding capacity of different cations to humic acid. PMID:28955013

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

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.

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.

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.

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.

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

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.

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

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.

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.

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.

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

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...

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.

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.

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.

Microwave-assisted direct synthesis of butene from high-selectivity methane

NASA Astrophysics Data System (ADS)

Lu, Yi-heng; Li, Kang; Lu, Yu-wei

2017-12-01

Methane was directly converted to butene liquid fuel by microwave-induced non-oxidative catalytic dehydrogenation under 0.1-0.2 MPa. The results show that, under microwave heating in a two-stage fixed-bed reactor, in which nickel powder and NiOx-MoOy/SiO2 are used as the catalyst, the methane-hydrogen mixture is used as the raw material, with no acetylene detected. The methane conversion is more than 73.2%, and the selectivity of methane to butene is 99.0%. Increasing the hydrogen/methane feed volume ratio increases methane conversion and selectivity. Gas chromatography/electron impact ionization/mass spectrometry chromatographic analysis showed that the liquid fuel produced by methane dehydrogenation oligomerization contained 89.44% of butene, and the rest was acetic acid, ethanol, butenol and butyric acid, and the content was 1.0-3.0 wt%.

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.

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.

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.

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.

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

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

Nanoceria Supported Single-Atom Platinum Catalysts for Direct Methane Conversion

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

Xie, Pengfei; Pu, Tiancheng; Nie, Anmin

Nanoceria-supported atomic Pt catalysts (denoted as Pt 1@CeO 2) have been synthesized and demonstrated with advanced catalytic performance for the non-oxidative, direct conversion of methane. These catalysts were synthesized by calcination of Pt-impregnated porous ceria nanoparticles at high temperature (ca. 1,000 °C), with the atomic dispersion of Pt characterized by combining aberra-tion-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption spec-troscopy (XAS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analyses. The Pt 1@CeO 2 catalysts exhibited much superior catalytic performance to its nanoparticulated counterpart, achieving 14.4% of methane conversion at 975 °C andmore » 74.6% selectivity toward C 2 products (ethane, ethylene and acetylene). Comparative studies of the Pt1@CeO 2 catalysts with different loadings as well as the nanoparticulated counterpart reveal the single-atom Pt to be the active sites for selective conversion of methane into C 2 hydrocarbons.« less

Nanoceria Supported Single-Atom Platinum Catalysts for Direct Methane Conversion

DOE PAGES

Xie, Pengfei; Pu, Tiancheng; Nie, Anmin; ...

2018-04-03

Nanoceria-supported atomic Pt catalysts (denoted as Pt 1@CeO 2) have been synthesized and demonstrated with advanced catalytic performance for the non-oxidative, direct conversion of methane. These catalysts were synthesized by calcination of Pt-impregnated porous ceria nanoparticles at high temperature (ca. 1,000 °C), with the atomic dispersion of Pt characterized by combining aberra-tion-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectroscopy (XPS), X-ray absorption spec-troscopy (XAS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analyses. The Pt 1@CeO 2 catalysts exhibited much superior catalytic performance to its nanoparticulated counterpart, achieving 14.4% of methane conversion at 975 °C andmore » 74.6% selectivity toward C 2 products (ethane, ethylene and acetylene). Comparative studies of the Pt1@CeO 2 catalysts with different loadings as well as the nanoparticulated counterpart reveal the single-atom Pt to be the active sites for selective conversion of methane into C 2 hydrocarbons.« less

Microwave-assisted direct synthesis of butene from high-selectivity methane

PubMed Central

Li, Kang; Lu, Yu-wei

2017-01-01

Methane was directly converted to butene liquid fuel by microwave-induced non-oxidative catalytic dehydrogenation under 0.1–0.2 MPa. The results show that, under microwave heating in a two-stage fixed-bed reactor, in which nickel powder and NiOx–MoOy/SiO2 are used as the catalyst, the methane–hydrogen mixture is used as the raw material, with no acetylene detected. The methane conversion is more than 73.2%, and the selectivity of methane to butene is 99.0%. Increasing the hydrogen/methane feed volume ratio increases methane conversion and selectivity. Gas chromatography/electron impact ionization/mass spectrometry chromatographic analysis showed that the liquid fuel produced by methane dehydrogenation oligomerization contained 89.44% of butene, and the rest was acetic acid, ethanol, butenol and butyric acid, and the content was 1.0–3.0 wt%. PMID:29308261

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.

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.

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

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.

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.

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

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.

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

Printable enzyme-embedded materials for methane to methanol conversion

DOE PAGES

Blanchette, Craig D.; Knipe, Jennifer M.; Stolaroff, Joshuah K.; ...

2016-06-15

An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas. The only selective catalysts for methane activation and conversion to methanol under mild conditions are methane monooxygenases (MMOs) found in methanotrophic bacteria; however, these enzymes are not amenable to standard enzyme immobilization approaches. Using particulate methane monooxygenase (pMMO), we create a biocatalytic polymer material that converts methane to methanol. We demonstrate embedding the material within a silicone lattice to create mechanically robust, gas-permeable membranes, and direct printing of micron-scalemore » structures with controlled geometry. Remarkably, the enzymes retain up to 100% activity in the polymer construct. The printed enzyme-embedded polymer motif is highly flexible for future development and should be useful in a wide range of applications, especially those involving gas–liquid reactions.« less

NREL Advancements in Methane Conversion Lead to Cleaner Air, Useful Products

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

2016-06-01

Researchers at NREL leveraged the recent on-site development of gas fermentation capabilities and novel genetic tools to directly convert methane to lactic acid using an engineered methanotrophic bacterium. The results provide proof-of-concept data for a gas-to-liquids bioprocess that concurrently produces fuels and chemicals from methane. NREL researchers developed genetic tools to express heterologous genes in methanotrophic organisms, which have historically been difficult to genetically engineer. Using these tools, researchers demonstrated microbial conversion of methane to lactate, a high-volume biochemical precursor predominantly utilized for the production of bioplastics. Methane biocatalysis offers a means to concurrently liquefy and upgrade natural gas andmore » renewable biogas, enabling their utilization in conventional transportation and industrial manufacturing infrastructure. Producing chemicals and fuels from methane expands the suite of products currently generated from biorefineries, municipalities, and agricultural operations, with the potential to increase revenue and significantly reduce greenhouse gas emissions.« less

Printable enzyme-embedded materials for methane to methanol conversion

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

Blanchette, Craig D.; Knipe, Jennifer M.; Stolaroff, Joshuah K.

An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas. The only selective catalysts for methane activation and conversion to methanol under mild conditions are methane monooxygenases (MMOs) found in methanotrophic bacteria; however, these enzymes are not amenable to standard enzyme immobilization approaches. Using particulate methane monooxygenase (pMMO), we create a biocatalytic polymer material that converts methane to methanol. We demonstrate embedding the material within a silicone lattice to create mechanically robust, gas-permeable membranes, and direct printing of micron-scalemore » structures with controlled geometry. Remarkably, the enzymes retain up to 100% activity in the polymer construct. The printed enzyme-embedded polymer motif is highly flexible for future development and should be useful in a wide range of applications, especially those involving gas–liquid reactions.« less

Printable enzyme-embedded materials for methane to methanol conversion

PubMed Central

Blanchette, Craig D.; Knipe, Jennifer M.; Stolaroff, Joshuah K.; DeOtte, Joshua R.; Oakdale, James S.; Maiti, Amitesh; Lenhardt, Jeremy M.; Sirajuddin, Sarah; Rosenzweig, Amy C.; Baker, Sarah E.

2016-01-01

An industrial process for the selective activation of methane under mild conditions would be highly valuable for controlling emissions to the environment and for utilizing vast new sources of natural gas. The only selective catalysts for methane activation and conversion to methanol under mild conditions are methane monooxygenases (MMOs) found in methanotrophic bacteria; however, these enzymes are not amenable to standard enzyme immobilization approaches. Using particulate methane monooxygenase (pMMO), we create a biocatalytic polymer material that converts methane to methanol. We demonstrate embedding the material within a silicone lattice to create mechanically robust, gas-permeable membranes, and direct printing of micron-scale structures with controlled geometry. Remarkably, the enzymes retain up to 100% activity in the polymer construct. The printed enzyme-embedded polymer motif is highly flexible for future development and should be useful in a wide range of applications, especially those involving gas–liquid reactions. PMID:27301270

High-rate two-phase process for the anaerobic degradation of cellulose, employing rumen microorganisms for an efficient acidogenesis

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

Gijzen, H.J.; Zwart, K.B.; Verhagen, F.J.M.

1988-04-05

A novel two-stage anaerobic process for the microbial conversion of cellulose into biogas has been developed. In the first phase, a mixed population of rumen bacteria and ciliates was used in the hydrolysis and fermentation of cellulose. The volatile fatty acids (VFA) produced in this acidogenic reactor were subsequently converted into biogas in a UASB-type methanogenic reactor. A stepwise increase of the loading rate from 11.9 to 25.8 g volatile solids/L reactor volume/day (g VS/L/day) did not affect the degradation efficiency in the acidogenic reactor, whereas the methanogenic reactor appeared to be overloaded at the highest loading rate. Cellulose digestionmore » was almost complete at all loading rates applied. The two-stage anaerobic process was also tested with a closed fluid circuit. In this instance total methane production was 0.438 L CH/sub 4//g VS added, which is equivalent to 98% of the theoretical value. The application of rumen microorganisms in combination with a high-rate methane reactor is proposed as a means of efficient anaerobic degradation of cellulosic residues to methane. Because this newly developed two-phase system is based on processes and microorganisms from the ruminant, it will be referred to as Rumen Derived Anaerobic Digestion (RUDAD)-process.« less

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

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.

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

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.

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

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.

Internal reforming of methane in solid oxide fuel cell systems

NASA Astrophysics Data System (ADS)

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

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

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.

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.

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.

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

Process simulation and comparison of biological conversion of syngas and hydrogen in biogas plants

NASA Astrophysics Data System (ADS)

Awais Salman, Chaudhary; Schwede, Sebastian; Thorin, Eva; Yan, Jinyue

2017-11-01

Organic waste is a good source of clean energy. However, different fractions of waste have to be utilized efficiently. One way is to find pathways to convert waste into useful products via various available processes (gasification, pyrolysis anaerobic digestion, etc.) and integrate them to increase the combined efficiency of the process. The syngas and hydrogen produced from the thermal conversion of biomass can be upgraded to biomethane via biological methanation. The current study presents the simulation model to predict the amount of biomethane produced by injecting the hydrogen and syngas. Hydrogen injection is modelled both in-situ and ex-situ while for syngas solely the ex-situ case has been studied. The results showed that 85% of the hydrogen conversion was achieved for the ex-situ reactor while 81% conversion rate was achieved for the in-situ reactor. The syngas could be converted completely in the bio-reactor. However, the addition of syngas resulted in an increase of carbon dioxide. Simulation of biomethanation of gas addition showed a biomethane concentration of 87% while for hydrogen addition an increase of 74% and 80% for in-situ and ex-situ addition respectively.

Integration of Power to Methane in a waste water treatment plant - A feasibility study.

PubMed

Patterson, Tim; Savvas, Savvas; Chong, Alex; Law, Ian; Dinsdale, Richard; Esteves, Sandra

2017-12-01

The integration of a biomethanation system within a wastewater treatment plant for conversion of CO 2 and H 2 to CH 4 has been studied. Results indicate that the CO 2 could be utilised to produce an additional 13,420m 3 /day of CH 4 , equivalent to approximately 133,826kWh of energy. The whole conversion process including electrolysis was found to have an energetic efficiency of 66.2%. The currently un-optimised biomethanation element of the process had a parasitic load of 19.9% of produced energy and strategies to reduce this to <5% are identified. The system could provide strategic benefits such as integrated management of electricity and gas networks, energy storage and maximising the deployment and efficiency of renewable energy assets. However, no policy or financial frameworks exist to attribute value to these increasingly important functions. Copyright © 2017 Elsevier Ltd. All rights reserved.

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.

Integrated solar thermochemical reaction system for steam methane reforming

DOE PAGES

Zheng, Feng; Diver, Rich; Caldwell, Dustin D.; ...

2015-06-05

Solar-aided upgrade of the energy content of fossil fuels, such as natural gas, can provide a near-term transition path towards a future solar-fuel economy and reduce carbon dioxide emission from fossil fuel consumption. Both steam and dry reforming a methane-containing fuel stream have been studied with concentrated solar power as the energy input to drive the highly endothermic reactions but the concept has not been demonstrated at a commercial scale. Under a current project with the U.S. Department of Energy, PNNL is developing an integrated solar thermochemical reaction system that combines solar concentrators with micro- and meso-channel reactors and heatmore » exchangers to accomplish more than 20% solar augment of methane higher heating value. The objective of our three-year project is to develop and prepare for commercialization such solar reforming system with a high enough efficiency to serve as the frontend of a conventional natural gas (or biogas) combined cycle power plant, producing power with a levelized cost of electricity less than 6¢/kWh, without subsidies, by the year 2020. In this paper, we present results from the first year of our project that demonstrated a solar-to-chemical energy conversion efficiency as high as 69% with a prototype reaction system.« less

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

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.

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.

Hemicellulose conversion by anaerobic digestion

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

Ghosh, S.; Henry, M.P.; Christopher, R.W.

1982-01-01

The digestibility of an aquatic biomass (water hyacinth), a land-based biomass (Coastal Bermuda grass), and a biomass-waste blend (a mixture of hyacinth, grass, MSW, and sludge) under various digestion conditions was studied. Anaerobic digestion of hemicellulose consists of the steps of enzymatic hydrolysis of hemicellulose to glucans, mannans, galactans, xylans, and arabans, and then to simple hexose and pentose sugars; production of C/sub 2/ and higher fatty acids from the simple sugars; conversion of higher fatty acids to acetate; and finally, production of methane and CO/sub 2/ from acetate, and CO/sub 2/ and hydrogen. The conversion of hemicellulose was highermore » under mesophilic conditions than those of cellulose or protein for all biomass test feeds, probably because the hemicellulose structure was more vulnerable to enzymatic attack than that of the lignocellulosic component. Cellulose conversion efficiencies at the mesophilic and thermophilic temperatures were about the same. However, hemicellulose was converted at a much lower efficiency than cellulose during thermophilic digestion - a situation that was the reverse of that observed at the mesophilic temperature. Cellulose was utilized in preference to hemicellulose during mesophilic digestion of nitrogen-supplemented Bermuda grass. It was speculated that Bermuda grass cellulose was converted at a higher efficiency than hemicellulose in the presence of external nitrogen because the metabolism of the breakdown product (glucose) of cellulose requires the least investment of enzymes and energy.« less

Renewable and high efficient syngas production from carbon dioxide and water through solar energy assisted electrolysis in eutectic molten salts

NASA Astrophysics Data System (ADS)

Wu, Hongjun; Liu, Yue; Ji, Deqiang; Li, Zhida; Yi, Guanlin; Yuan, Dandan; Wang, Baohui; Zhang, Zhonghai; Wang, Peng

2017-09-01

Over-reliance on non-renewable fossil fuel leads to steadily increasing concentration of atmospheric CO2, which has been implicated as a critical factor contributing to global warming. The efficient conversion of CO2 into useful product is highly sought after both in academic and industry. Herein, a novel conversion strategy is proposed to one-step transform CO2/H2O into syngas (CO/H2) in molten salt with electrolysis method. All the energy consumption in this system are contributed from sustainable energy sources: concentrated solar light heats molten salt and solar cell supplies electricity for electrolysis. The eutectic Li0.85Na0.61K0.54CO3/nLiOH molten electrolyte is rationally designed with low melting point (<450 °C). The synthesized syngas contains very desirable content of H2 and CO, with tuneable molar ratios (H2/CO) from 0.6 to 7.8, and with an efficient faradaic efficiency of ∼94.5%. The synthesis of syngas from CO2 with renewable energy at a such low electrolytic temperature not only alleviates heat loss, mitigates system corrosion, and heightens operational safety, but also decreases the generation of methane, thus increases the yield of syngas, which is a remarkable technological breakthrough and this work thus represents a stride in sustainable conversion of CO2 to value-added product.

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

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

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

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.

Effect of nitrogen-containing impurities on the activity of perovskitic catalysts for the catalytic combustion of methane.

PubMed

Buchneva, Olga; Gallo, Alessandro; Rossetti, Ilenia

2012-11-05

LaMnO(3), either pure or doped with 10 mol % Sr, has been prepared by flame pyrolysis in nanostructured form. Such catalysts have been tested for the catalytic flameless combustion of methane, achieving very high catalytic activity. The resistance toward poisoning by some model N-containing impurities has been checked in order to assess the possibility of operating the flameless catalytic combustion with biogas, possibly contaminated by S- or N-based compounds. This would be a significant improvement from the environmental point of view because the application of catalytic combustion to gas turbines would couple improved energy conversion efficiency and negligible noxious emissions, while the use of biogas would open the way to energy production from a renewable source by means of very efficient technologies. A different behavior has been observed for the two catalysts; namely, the undoped sample was more or less heavily poisoned, whereas the Sr-doped sample showed slightly increasing activity upon dosage of N-containing compounds. A possible reaction mechanism has been suggested, based on the initial oxidation of the organic backbone, with the formation of NO. The latter may adsorb more or less strongly depending on the availability of surface oxygen vacancies (i.e., depending on doping). Decomposition of NO may leave additional activated oxygen species on the surface, available for low-temperature methane oxidation and so improving the catalytic performance.

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

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.

Visible light active, nano-architectured metal oxide photo-catalysts for solar fuel applications

NASA Astrophysics Data System (ADS)

LaTempa, Thomas Joseph, Jr.

Large-scale implementation of renewable energy sources such as solar requires the development of an efficient energy capture, conversion and storage scheme. Harnessing solar energy to create storable fuels, i.e., solar fuels, provides a unique strategy to meet this objective. In this regard, hydrogen generation through water photoelectrolysis and methane generation via the photocatalytic conversion of carbon dioxide and water vapor are investigated. The primary motivation of this work lies in the development of efficient, low cost materials for solar fuel applications. Metal oxide semiconductors such as n-type titanium dioxide (TiO 2) have generated significant interest in the scientific community due to their low cost, stability and high photocatalytic activity under band gap illumination. The implementation of nano-structured materials has significantly enhanced the conversion efficiency obtained with TiO2 in applications such as water photoelectrolysis. Despite these advancements, TiO2 has an inherently poor photoresponse due its wide band gap (3.0-3.2 eV), which accounts for ≈ 5% of the solar spectrum energy. Therefore, the primary objective of this work is to develop materials with a photocatalytic activity approaching that of TiO2, while shifting the photo-response to harness the visible light portion of the solar spectrum. Two differing approaches are evaluated in this work to meet this objective. Hematite (alpha-Fe2O3) has a band gap ≈ 2.2 eV, well suited for capturing solar energy, but suffers from intrinsically poor electrical characteristics. To overcome these limitations, iron oxide nanotubes were developed using a temperature controlled anodization technique. This provides greater control over the film morphology to create high aspect ratio nano-structures approximately 1-4 mum in length, sufficient to harness solar energy, with a wall thickness approaching 10 nm to improve the electrical characteristics for photocatalytic application. The performance of hematite nanotubes, formed after thermal annealing, were characterized using incident photon conversion efficiency measurements (IPCE). A maximum IPCE of 3.5% was obtained under partial bias conditions, with a photo-response extending to ≈ 600 nm. Alternatively, modification of a nano-structured material with an intrinsically poor photoresponse was evaluated. Amorphous tantalum oxide nanotubes were synthesized using an anodization technique, providing great control over the film morphology. Nanotubes of varying film thickness in the range of 240 nm -- 15 mum, and wall thickness as small as 7 nm were obtained. Subsequent crystallization and nitridation through thermal annealing in ammonia ambient was evaluated to create tantalum nitride (Ta3N5) nanotubes. Tantalum nitride has a band gap ≈ 2.1 eV, similar to that of hematite. Water photoelectrolysis performance was evaluated and a maximum IPCE of 5.3% was obtained under partial bias conditions, with a red shift in the photoresponse of ≈ 300 nm towards the visible relative to Ta2O5 nanotubes. Finally, the photocatalytic conversion of carbon dioxide and water vapor into hydrocarbons such as methane was evaluated for TiO2, alpha-Fe 2O3 and Ta3N5 nanotube arrays. A microwave assisted, solvothermal approach to load platinum nanoparticle catalysts within the nanotube structure is evaluated. Catalyst sensitization is necessary to achieve measurable yields for carbon dioxide reduction, and the composite nanotube photocatalysts were evaluated under simulated solar AM 1.5G conditions. Methane generation is achieved for TiO2 and Ta3N5 composite photocatalysts at the rate of 25 ppm / cm2-hr and 9 ppm / cm2-hr, respectively.

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.

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.

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.

Gasification of land-based biomass. Final report July 78-December 82

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

Chynoweth, D.P.; Jerger, D.E.; Conrad, J.R.

1983-06-01

The objective of this research was to develop efficient processes for conversion of land-based biomass to methane and other resources. One task was to determine the relative suitability of selected species or feedstocks for biological and thermal gasification processes. The second task was to narrow options for design and operation of the experimental test unit (ETU) on water hyacinth and sludge at Walt Disney World (WDW) and to provide a scientific base for understanding rate- and yield-limiting reactions for biogasification of these feedstocks, (separately and as blends).

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

Stimulation of the anaerobic digestion of the dry organic fraction of municipal solid waste (OFMSW) with carbon-based conductive materials.

PubMed

Dang, Yan; Sun, Dezhi; Woodard, Trevor L; Wang, Li-Ying; Nevin, Kelly P; Holmes, Dawn E

2017-08-01

Growth of bacterial and archaeal species capable of interspecies electron exchange was stimulated by addition of conductive materials (carbon cloth or granular activated carbon (GAC)) to anaerobic digesters treating dog food (a substitute for the dry-organic fraction of municipal solid waste (OFMSW)). Methane production (772-1428mmol vs <80mmol), volatile solids removal (78%-81% vs 54%-64%) and COD removal efficiencies (∼80% vs 20%-30%) were all significantly higher in reactors amended with GAC or carbon cloth than controls. OFMSW degradation was also significantly accelerated and VFA concentrations were substantially lower in reactors amended with conductive materials. These results suggest that both conductive materials (carbon cloth and GAC) can promote conversion of OFMSW to methane even in the presence of extremely high VFA concentrations (∼500mM). Copyright © 2017 Elsevier Ltd. All rights reserved.

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

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...

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

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

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.

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.

Associations among methane emission traits measured in the feedlot and in respiration chambers in Angus cattle bred to vary in feed efficiency.

PubMed

Herd, R M; Velazco, J I; Arthur, P F; Hegarty, R F

2016-11-01

The objective of the study was to evaluate associations among animal performance and methane emission traits under feedlot conditions and in respiration chambers in Angus cattle bred to vary in residual feed intake (RFI), which is a measure of feed efficiency. Fifty-nine cattle were tested for feedlot RFI, of which 41 had methane production recorded on an ad libitum grain-based ration in the feedlot, 59 on a restricted grain-based ration in respiration chambers, and 57 on a restricted roughage ration in respiration chambers. The cattle became older and heavier as they went through the different phases of the experiment, but their feed intake (expressed as DMI) and daily emission of enteric methane (methane production rate; MPR) did not increase proportionally, as feed offered was restricted in the respiration chamber tests. Methane emissions by individual animals relative to their DMI were calculated as methane yield (MY; MPR/DMI) and as 2 measures of residual methane production (RMP and RMP), which were calculated as the difference between measured MPR and that predicted from feed intake by 2 different equations. Within each test regime, MPR was positively correlated ( = 0.28 to 0.61) with DMI. Phenotypic correlations for MY, RMP, and RMP between the feedlot test and the restricted grain test ( = 0.40 to 0.43) and between the restricted grain test and the restricted roughage test were moderate ( = 0.36 to 0.41) and moderate to strong between the feedlot test and the restricted roughage test ( = 0.54 to 0.58). These results indicate that the rankings of animals for methane production relative to feed consumed are relatively stable over the 3 test phases. Feedlot feed conversion ratio and RFI were not correlated with MPR in the feedlot test and grain-based chamber test but were negatively correlated with MPR in the chamber roughage test ( = -0.31 and -0.37). Both were negatively correlated with MY and RMP in the feedlot test ( = -0.42 to -0.54) and subsequent chamber roughage test ( = -0.27 to -0.49). Midparent estimated breeding values for RFI tended to be negatively correlated with MY and RMP in the feedlot test ( = -0.27 and -0.27) and were negatively correlated with MY, RMP, and RMP in the chamber roughage test ( = -0.33 to -0.36). These results showed that in young growing cattle, lower RFI was associated with higher MY, RMP, and RMP but had no significant association with MPR.

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.

Treatment of natural rubber processing wastewater using a combination system of a two-stage up-flow anaerobic sludge blanket and down-flow hanging sponge system.

PubMed

Tanikawa, D; Syutsubo, K; Hatamoto, M; Fukuda, M; Takahashi, M; Choeisai, P K; Yamaguchi, T

2016-01-01

A pilot-scale experiment of natural rubber processing wastewater treatment was conducted using a combination system consisting of a two-stage up-flow anaerobic sludge blanket (UASB) and a down-flow hanging sponge (DHS) reactor for more than 10 months. The system achieved a chemical oxygen demand (COD) removal efficiency of 95.7% ± 1.3% at an organic loading rate of 0.8 kg COD/(m(3).d). Bacterial activity measurement of retained sludge from the UASB showed that sulfate-reducing bacteria (SRB), especially hydrogen-utilizing SRB, possessed high activity compared with methane-producing bacteria (MPB). Conversely, the acetate-utilizing activity of MPB was superior to SRB in the second stage of the reactor. The two-stage UASB-DHS system can reduce power consumption by 95% and excess sludge by 98%. In addition, it is possible to prevent emissions of greenhouse gases (GHG), such as methane, using this system. Furthermore, recovered methane from the two-stage UASB can completely cover the electricity needs for the operation of the two-stage UASB-DHS system, accounting for approximately 15% of the electricity used in the natural rubber manufacturing process.

Direct Conversion of Methane to Methanol on Ni-Ceria Surfaces: Metal-Support Interactions and Water-enabled Catalytic Conversion by Site Blocking

DOE PAGES

Lustemberg, Pablo G.; Palomino, Robert M.; Gutierrez, Ramon A.; ...

2018-05-28

The transformation of methane into methanol or higher alcohols at moderate temperature and pressure conditions is of great environmental interest and remains a challenge despite many efforts. Extended surfaces of metallic nickel are inactive for a direct CH 4 → CH 3OH conversion. This experimental and computational study provides clear evidence that low Ni loadings on a CeO 2(111) support can perform a direct catalytic cycle for the generation of methanol at low temperature using oxygen and water as reactants, with a higher selectivity than ever reported for ceria-based catalysts. On the basis of ambient pressure X-ray photoemission spectroscopy andmore » density functional theory calculations, we demonstrate that water plays a crucial role in blocking catalyst sites where methyl species could fully decompose, an essential factor for diminishing the production of CO and CO 2, and in generating sites on which methoxy species and ultimately methanol can form. In addition to water-site blocking, one needs the effects of metal-support interactions to bind and activate methane and water. Lastly, these findings should be considered when designing metal/oxide catalysts for converting methane to value-added chemicals and fuels.« less

Direct Conversion of Methane to Methanol on Ni-Ceria Surfaces: Metal-Support Interactions and Water-enabled Catalytic Conversion by Site Blocking

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

Lustemberg, Pablo G.; Palomino, Robert M.; Gutierrez, Ramon A.

The transformation of methane into methanol or higher alcohols at moderate temperature and pressure conditions is of great environmental interest and remains a challenge despite many efforts. Extended surfaces of metallic nickel are inactive for a direct CH 4 → CH 3OH conversion. This experimental and computational study provides clear evidence that low Ni loadings on a CeO 2(111) support can perform a direct catalytic cycle for the generation of methanol at low temperature using oxygen and water as reactants, with a higher selectivity than ever reported for ceria-based catalysts. On the basis of ambient pressure X-ray photoemission spectroscopy andmore » density functional theory calculations, we demonstrate that water plays a crucial role in blocking catalyst sites where methyl species could fully decompose, an essential factor for diminishing the production of CO and CO 2, and in generating sites on which methoxy species and ultimately methanol can form. In addition to water-site blocking, one needs the effects of metal-support interactions to bind and activate methane and water. Lastly, these findings should be considered when designing metal/oxide catalysts for converting methane to value-added chemicals and fuels.« less

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.

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.

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.

Continuous hydrogen and methane production from Agave tequilana bagasse hydrolysate by sequential process to maximize energy recovery efficiency.

PubMed

Montiel Corona, Virginia; Razo-Flores, Elías

2018-02-01

Continuous H 2 and CH 4 production in a two-stage process to increase energy recovery from agave bagasse enzymatic-hydrolysate was studied. In the first stage, the effect of organic loading rate (OLR) and stirring speed on volumetric hydrogen production rate (VHPR) was evaluated in a continuous stirred tank reactor (CSTR); by controlling the homoacetogenesis with the agitation speed and maintaining an OLR of 44 g COD/L-d, it was possible to reach a VHPR of 6 L H 2 /L-d, equivalent to 1.34 kJ/g bagasse. In the second stage, the effluent from CSTR was used as substrate to feed a UASB reactor for CH 4 production. Volumetric methane production rate (VMPR) of 6.4 L CH 4 /L-d was achieved with a high OLR (20 g COD/L-d) and short hydraulic retention time (HRT, 14 h), producing 225 mL CH 4 /g-bagasse equivalent to 7.88 kJ/g bagasse. The two-stage continuous process significantly increased energy conversion efficiency (56%) compared to one-stage hydrogen production (8.2%). Copyright © 2017 Elsevier Ltd. All rights reserved.

A novel atmospheric tritium sampling system

NASA Astrophysics Data System (ADS)

Qin, Lailai; Xia, Zhenghai; Gu, Shaozhong; Zhang, Dongxun; Bao, Guangliang; Han, Xingbo; Ma, Yuhua; Deng, Ke; Liu, Jiayu; Zhang, Qin; Ma, Zhaowei; Yang, Guo; Liu, Wei; Liu, Guimin

2018-06-01

The health hazard of tritium is related to its chemical form. Sampling different chemical forms of tritium simultaneously becomes significant. Here a novel atmospheric tritium sampling system (TS-212) was developed to collect the tritiated water (HTO), tritiated hydrogen (HT) and tritiated methane (CH3T) simultaneously. It consisted of an air inlet system, three parallel connected sampling channels, a hydrogen supply module, a methane supply module and a remote control system. It worked at air flow rate of 1 L/min to 5 L/min, with temperature of catalyst furnace at 200 °C for HT sampling and 400 °C for CH3T sampling. Conversion rates of both HT and CH3T to HTO were larger than 99%. The collecting efficiency of the two-stage trap sets for HTO was larger than 96% in 12 h working-time without being blocked. Therefore, the collected efficiencies of TS-212 are larger than 95% for tritium with different chemical forms in environment. Besides, the remote control system made sampling more intelligent, reducing the operator's work intensity. Based on the performance parameters described above, the TS-212 can be used to sample atmospheric tritium in different chemical forms.

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

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

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.

The combined effects of supplementing monensin and 3-nitrooxypropanol on methane emissions, growth rate, and feed conversion efficiency in beef cattle fed high forage and high grain diets.

PubMed

Vyas, Diwakar; Alemu, Aklilu W; McGinn, Sean M; Duval, Stephane M; Kindermann, Maik; Beauchemin, Karen A

2018-05-05

The study objective was to evaluate the combined effects of supplementing monensin (MON) and the methane (CH4) inhibitor 3-nitrooxypropanol (NOP) on enteric CH4 emissions, growth rate and feed conversion efficiency of backgrounding and finishing beef cattle. Two hundred and forty crossbred steers were used in a 238-d feeding study and fed a backgrounding diet for the first 105-d (backgrounding phase), transition diets for 28 d, followed by a finishing diet for 105-d (finishing phase). Treatments were: 1) Control (no additive); 2) MON (monensin supplemented at 33 mg/kg DM; 3) NOP (3-nitrooxypropanol supplemented at 200 mg/kg DM for backgrounding or 125 mg/kg DM for finishing phase); 4) MONOP (33 mg/kg DM MON supplemented with either 200 mg/kg DM or 125 mg/kg DM NOP). The experiment was a randomized complete block (weight: heavy and light) design with 2 (NOP) × 2 (MON) factorial arrangement of treatments using 24 pens (8 cattle/pen; 6 pens/treatment) at the main feedlot and 8 pens (6 cattle/pen; 2 pens/treatment) at the controlled environment building (CEB) feedlot. Five animals per treatment were moved to chambers for methane measurements during both phases. Data were analyzed using a Mixed procedure of SAS with pen as experimental unit (except CH4). Location (Main vs CEB) had no significant effect and was thus omitted from the final model. Overall, there were few interactions between MON and NOP indicating that the effects of the 2 compounds were independent. When cattle were fed the backgrounding diet, pen DMI was decreased by 7% while gain-to-feed ratio (G:F) was improved by 5% with NOP supplementation (P < 0.01). Similarly, MON improved G:F ratio by 4% (P < 0.01), but without affecting DMI. During the finishing phase, DMI tended (P = 0.06) to decrease by 5% with both MON (5%) and NOP (5%), while average daily gain tended (P = 0.08) to decrease by 3% with MON. Gain-to-feed ratio for finishing cattle was improved with NOP by 3% (P < 0.01); however, no effects were observed with MON. 3-Nitrooxypropanol decreased CH4 yield (g/kg DMI) by 42% and 37% with backgrounding and finishing diets (P ≤ 0.01), respectively, while MON did not lower CH4 yield. Overall, these results demonstrate efficacy of NOP in reducing enteric CH4 emissions and subsequently improving feed conversion efficiency in cattle fed high forage and high grain diets. Furthermore, effects of NOP did not depend upon whether MON was included in the diet.

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.

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.

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

Fe 2O 3–TiO 2 core–shell nanorod arrays for visible light photocatalytic applications

DOE PAGES

Yao, Kun; Basnet, Pradip; Sessions, Henry; ...

2015-11-11

By using the glancing angle deposition technique and post-deposition annealing, Fe 2O 3–TiO 2 core-shell nanorod arrays with specific crystalline states can be designed and fabricated. The Fe 2O 3–TiO 2 core-shell samples annealed at temperatures greater than 450°C formed α-Fe 2O 3 and anatase TiO 2, and showed higher catalytic efficiency for the degradation of methylene blue (MB) under visible light illumination when compared with pure anatase TiO 2 or α-Fe 2O 3 nanorod arrays. Solar conversion of carbon dioxide and water vapor in the presence of Fe 2O 3–TiO 2 core-shell nanorod arrays was also investigated. Carbon monoxide,more » hydrogen, methane, and methanol along with other hydrocarbons were produced after only several hours’ exposure under ambient sunlight. It was determined that the core-shell structure showed greater efficiency for solar CO 2 conversion than the pure TiO 2 nanorod arrays.« less

Improvement of the energy conversion efficiency of Chlorella pyrenoidosa biomass by a three-stage process comprising dark fermentation, photofermentation, and methanogenesis.

PubMed

Xia, Ao; Cheng, Jun; Ding, Lingkan; Lin, Richen; Huang, Rui; Zhou, Junhu; Cen, Kefa

2013-10-01

The effects of pre-treatment methods on saccharification and hydrogen fermentation of Chlorella pyrenoidosa biomass were investigated. When raw biomass and biomass pre-treated by steam heating, by microwave heating, and by ultrasonication were used as feedstock, the hydrogen yields were only 8.8-12.7 ml/g total volatile solids (TVS) during dark fermentation. When biomass was pre-treated by steam heating with diluted acid and by microwave heating with diluted acid, the dark hydrogen yields significantly increased to 75.6 ml/g TVS and 83.3 ml/g TVS, respectively. Steam heating with diluted acid is the preferred pre-treatment method of C. pyrenoidosa biomass to improve hydrogen yield during dark fermentation and photofermentation, which is followed by methanogenesis to increase energy conversion efficiency (ECE). A total hydrogen yield of 198.3 ml/g TVS and a methane yield of 186.2 ml/g TVS corresponding to an overall ECE of 34.0% were obtained through the three-stage process (dark fermentation, photofermentation, and methanogenesis). Copyright © 2013 Elsevier Ltd. All rights reserved.

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...

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.

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

PubMed

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

2017-10-01

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

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.

Methane, Black Carbon, and Ethane Emissions from Natural Gas Flares in the Bakken Shale, North Dakota.

PubMed

Gvakharia, Alexander; Kort, Eric A; Brandt, Adam; Peischl, Jeff; Ryerson, Thomas B; Schwarz, Joshua P; Smith, Mackenzie L; Sweeney, Colm

2017-05-02

Incomplete combustion during flaring can lead to production of black carbon (BC) and loss of methane and other pollutants to the atmosphere, impacting climate and air quality. However, few studies have measured flare efficiency in a real-world setting. We use airborne data of plume samples from 37 unique flares in the Bakken region of North Dakota in May 2014 to calculate emission factors for BC, methane, ethane, and combustion efficiency for methane and ethane. We find no clear relationship between emission factors and aircraft-level wind speed or between methane and BC emission factors. Observed median combustion efficiencies for methane and ethane are close to expected values for typical flares according to the US EPA (98%). However, we find that the efficiency distribution is skewed, exhibiting log-normal behavior. This suggests incomplete combustion from flares contributes almost 1/5 of the total field emissions of methane and ethane measured in the Bakken shale, more than double the expected value if 98% efficiency was representative. BC emission factors also have a skewed distribution, but we find lower emission values than previous studies. The direct observation for the first time of a heavy-tail emissions distribution from flares suggests the need to consider skewed distributions when assessing flare impacts globally.

Direct Measure of the Dense Methane Phase in Gas Shale Organic Porosity by Neutron Scattering

DOE PAGES

Eberle, Aaron P. R.; King, Hubert E.; Ravikovitch, Peter I.; ...

2016-08-30

Here, we report the first direct measurements of methane density in shale gas using small-angle neutron scattering. At a constant pressure, the density of methane in the inorganic pores is similar to the gas bulk density of the system conditions. Conversely, the methane density is 2.1 ± 0.2 times greater in the organic mesopores. Furthermore, classical density functional theory calculations show that this excess density in the organic pores persists to elevated temperatures, typical of shale gas reservoir conditions, providing new insight into the hydrocarbon storage mechanisms within these reservoirs.

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.

Producing methane, methanol and electricity from organic waste of fermentation reaction using novel microbes.

PubMed

Dhiman, Saurabh Sudha; Shrestha, Namita; David, Aditi; Basotra, Neha; Johnson, Glenn R; Chadha, Bhupinder S; Gadhamshetty, Venkataramana; Sani, Rajesh K

2018-06-01

Residual solid and liquid streams from the one-pot CRUDE (Conversion of Raw and Untreated Disposal into Ethanol) process were treated with two separate biochemical routes for renewable energy transformation. The solid residual stream was subjected to thermophilic anaerobic digestion (TAD), which produced 95 ± 7 L methane kg -1 volatile solid with an overall energy efficiency of 12.9 ± 1.7%. A methanotroph, Methyloferula sp., was deployed for oxidation of mixed TAD biogas into methanol. The residual liquid stream from CRUDE process was used in a Microbial Fuel Cell (MFC) to produce electricity. Material balance calculations confirmed the integration of biochemical routes (i.e. CRUDE, TAD, and MFC) for developing a sustainable approach of energy regeneration. The current work demonstrates the utilization of different residual streams originated after food waste processing to release minimal organic load to the environment. Copyright © 2018 Elsevier Ltd. All rights reserved.

The performance and microbial diversity of temperature-phased hyperthermophilic and thermophilic anaerobic digestion system fed with organic waste.

PubMed

Lee, M Y; Cheon, J H; Hidaka, T; Tsuno, H

2008-01-01

The objective of this study was to evaluate the performances and microbial diversities for development of the effective hyperthermophilic digester system that consists of a hyperthermophilic reactor and hyperthermophilic or thermophilic reactor in series. Lab-scale reactors were operated continuously fed with artificial kitchen garbage. The effect of temperature on the acidification step was firstly investigated. Results indicated that 20.8% of COD solubilization was achieved at 70 degrees C, with 12.6% at 80 degrees C. The average protein solubilization reached 31% at 80 degrees C. Methane conversion efficiency following the acidification was around 85% on average at 55 degrees C, but decreased with increasing temperature and methane gas was not produced over 73 degrees C. As well, bacteria affiliated with the methanogens dominated the population below 65 degrees C, while those affiliated with acidogens were predominant over 73 degrees C. These results indicated that the hyperthermophilic process has considerable benefits to treat wastewater or waste containing high concentration of protein.

Selective bio-oxidation of propane to acetone using methane-oxidizing Methylomonas sp. DH-1.

PubMed

Hur, Dong Hoon; Nguyen, Thu Thi; Kim, Donghyuk; Lee, Eun Yeol

2017-07-01

Propane is the major component of liquefied petroleum gas (LPG). Nowadays, the use of LPG is decreasing, and thus utilization of propane as a chemical feedstock is in need of development. An efficient biological conversion of propane to acetone using a methanotrophic whole cell as the biocatalyst was proposed and investigated. A bio-oxidation pathway of propane to acetone in Methylomonas sp. DH-1 was analyzed by gene expression profiling via RNA sequencing. Propane was oxidized to 2-propanol by particulate methane monooxygenase and subsequently to acetone by methanol dehydrogenases. Methylomonas sp. DH-1 was deficient in acetone-converting enzymes and thus accumulated acetone in the absence of any enzyme inhibition. The maximum accumulation, average productivity and specific productivity of acetone were 16.62 mM, 0.678 mM/h and 0.141 mmol/g cell/h, respectively, under the optimized conditions. Our study demonstrates a novel method for the bioconversion of propane to acetone using methanotrophs under mild reaction condition.

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

Long-term bio-H2 and bio-CH4 production from food waste in a continuous two-stage system: Energy efficiency and conversion pathways.

PubMed

Algapani, Dalal E; Qiao, Wei; di Pumpo, Francesca; Bianchi, David; Wandera, Simon M; Adani, Fabrizio; Dong, Renjie

2018-01-01

Anaerobic digestion is a well-established technology for treating organic waste, but it is still under challenge for food waste due to process stability problems. In this work, continuous H 2 and CH 4 production from canteen food waste (FW) in a two-stage system were successfully established by optimizing process parameters. The optimal hydraulic retention time was 5d for H 2 and 15d for CH 4 . Overall, around 59% of the total COD in FW was converted into H 2 (4%) and into CH 4 (55%). The fluctuations of FW characteristics did not significantly affect process performance. From the energy point view, the H 2 reactor contributed much less than the methane reactor to total energy balance, but it played a key role in maintaining the stability of anaerobic treatment of food waste. Microbial characterization indicated that methane formation was through syntrophic acetate oxidation combined with hydrogenotrophic methanogenesis pathway. Copyright © 2017. Published by Elsevier Ltd.

Filtration of Carbon Particulate Emissions from a Plasma Pyrolysis Assembly

NASA Technical Reports Server (NTRS)

Agui, Juan H.; Green, Robert; Vijayakumar, R.; Berger, Gordon; Greenwood, Zach; Abney, Morgan; Peterson, Elspeth

2016-01-01

NASA is investigating plasma pyrolysis as a candidate technology that will enable the recovery of hydrogen from the methane produced by the ISS Sabatier Reactor. The Plasma Pyrolysis Assembly (PPA) is the current prototype of this technology which converts the methane product from the Carbon Dioxide Reduction Assembly (CRA) to acetylene and hydrogen with 90% or greater conversion efficiency. 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. We discuss developmental work on several options for filtering out the carbon particulate emissions from the PPA exit gas stream. The filtration technologies and concepts investigated range from fibrous media to monolithic ceramic and sintered metal media. This paper describes the different developed filter prototypes and characterizes their performance from integrated testing at the Environmental Chamber (E-Chamber) at MSFC. In addition, characterization data on the generated carbon particulates, that help to define filter requirements, are also presented.

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

Electron string ion sources for carbon ion cancer therapy accelerators

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

Boytsov, A. Yu.; Donets, D. E.; Donets, E. D.

2015-08-15

The type of the Electron String Ion Sources (ESIS) is considered to be the appropriate one to produce pulsed C{sup 4+} and C{sup 6+} ion beams for cancer therapy accelerators. In fact, the new test ESIS Krion-6T already now provides more than 10{sup 10} C{sup 4+} ions per pulse and about 5 × 10{sup 9} C{sup 6+} ions per pulse. Such ion sources could be suitable to apply at synchrotrons. It has also been found that Krion-6T can provide more than 10{sup 11} C{sup 6+} ions per second at the 100 Hz repetition rate, and the repetition rate can bemore » increased at the same or larger ion output per second. This makes ESIS applicable at cyclotrons as well. ESIS can be also a suitable type of ion source to produce the {sup 11}C radioactive ion beams. A specialized cryogenic cell was experimentally tested at the Krion-2M ESIS for pulse injection of gaseous species into the electron string. It has been shown in experiments with stable methane that the total conversion efficiency of methane molecules to C{sup 4+} ions reached 5%÷10%. For cancer therapy with simultaneous irradiation and precise dose control (positron emission tomography) by means of {sup 11}C, transporting to the tumor with the primary accelerated {sup 11}C{sup 4+} beam, this efficiency is preliminarily considered to be large enough to produce the {sup 11}C{sup 4+} beam from radioactive methane and to inject this beam into synchrotrons.« less

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...

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

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

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

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

Microbial battery for efficient energy recovery.

PubMed

Xie, Xing; Ye, Meng; Hsu, Po-Chun; Liu, Nian; Criddle, Craig S; Cui, Yi

2013-10-01

By harnessing the oxidative power of microorganisms, energy can be recovered from reservoirs of less-concentrated organic matter, such as marine sediment, wastewater, and waste biomass. Left unmanaged, these reservoirs can become eutrophic dead zones and sites of greenhouse gas generation. Here, we introduce a unique means of energy recovery from these reservoirs-a microbial battery (MB) consisting of an anode colonized by microorganisms and a reoxidizable solid-state cathode. The MB has a single-chamber configuration and does not contain ion-exchange membranes. Bench-scale MB prototypes were constructed from commercially available materials using glucose or domestic wastewater as electron donor and silver oxide as a coupled solid-state oxidant electrode. The MB achieved an efficiency of electrical energy conversion of 49% based on the combustion enthalpy of the organic matter consumed or 44% based on the organic matter added. Electrochemical reoxidation of the solid-state electrode decreased net efficiency to about 30%. This net efficiency of energy recovery (unoptimized) is comparable to methane fermentation with combined heat and power.

Microbial battery for efficient energy recovery

PubMed Central

Xie, Xing; Ye, Meng; Hsu, Po-Chun; Liu, Nian; Criddle, Craig S.; Cui, Yi

2013-01-01

By harnessing the oxidative power of microorganisms, energy can be recovered from reservoirs of less-concentrated organic matter, such as marine sediment, wastewater, and waste biomass. Left unmanaged, these reservoirs can become eutrophic dead zones and sites of greenhouse gas generation. Here, we introduce a unique means of energy recovery from these reservoirs—a microbial battery (MB) consisting of an anode colonized by microorganisms and a reoxidizable solid-state cathode. The MB has a single-chamber configuration and does not contain ion-exchange membranes. Bench-scale MB prototypes were constructed from commercially available materials using glucose or domestic wastewater as electron donor and silver oxide as a coupled solid-state oxidant electrode. The MB achieved an efficiency of electrical energy conversion of 49% based on the combustion enthalpy of the organic matter consumed or 44% based on the organic matter added. Electrochemical reoxidation of the solid-state electrode decreased net efficiency to about 30%. This net efficiency of energy recovery (unoptimized) is comparable to methane fermentation with combined heat and power. PMID:24043800

Application of polyimide membranes for biogas purification and enrichment.

PubMed

Harasimowicz, M; Orluk, P; Zakrzewska-Trznadel, G; Chmielewski, A G

2007-06-18

Biogas is a clean environment friendly fuel that is produced by bacterial conversion of organic matter under anaerobic (oxygen-free) conditions. Raw biogas contains about 55-65% methane (CH(4)), 30-45% carbon dioxide (CO(2)), traces of hydrogen sulphide (H(2)S) and fractions of water vapour. Pure methane has a calorific value of 9100 kcal/m(3) at 15.5 degrees C and 1 atm; the calorific value of biogas varies from 4800 to 6900 kcal/m(3). To achieve the standard composition of the biogas and calorific value of 5500 kcal/m(3) the treatment techniques like absorption or membrane separation should be applied. In the paper the results of the tests of the CH(4) enrichment in simulated biogas mixture consisted of methane, carbon dioxide and hydrogen sulphide were presented. It was showed that using the capillary module with polyimide membranes it was possible to achieve the enrichment of CH(4) from the concentrations of 55-85% up to 91-94.4%. The membrane material was resistant to the small concentrations of sour gases and assured the reduction of H(2)S and water vapour concentrations, as well. The required enrichment was achieved in the single module, however to prevent CH(4) losses the multistage or hybrid systems should be used to improve process efficiency.

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

Anaerobic digestion performance of sweet potato vine and animal manure under wet, semi-dry, and dry conditions.

PubMed

Zhang, Enlan; Li, Jiajia; Zhang, Keqiang; Wang, Feng; Yang, Houhua; Zhi, Suli; Liu, Guangqing

2018-03-22

Sweet potato vine (SPV) is an abundant agricultural waste, which is easy to obtain at low cost and has the potential to produce clean energy via anaerobic digestion (AD). The main objectives of this study were to reveal methane production and process stability of SPV and the mixtures with animal manure under various total solid conditions, to verify synergetic effect in co-digestion of SPV and manure in AD systems, and to determine the kinetics characteristics during the full AD process. The results showed that SPV was desirable feedstock for AD with 200.22 mL/g VS added of methane yield in wet anaerobic digestion and 12.20 L methane /L working volume in dry anaerobic digestion (D-AD). Synergistic effects were found in semi-dry anaerobic digestion and D-AD with each two mixing feedstock. In contrast with SPV mono-digestion, co-digestion with manure increased methane yield within the range of 14.34-49.11% in different AD digesters. The values of final volatile fatty acids to total alkalinity (TA) were below 0.4 and the values of final pH were within the range of 7.4-8.2 in all the reactors, which supported a positive relationship between carbohydrate hydrolysis and methanogenesis during AD process. The mathematical modified first order model was applied to estimate substrate biodegradability and methane production potential well with conversion constant ranged from 0.0003 to 0.0953 1/day, which indicated that co-digestion increased hydrolysis efficiency and metabolic activity. This work provides useful information to improve the utilization and stability of digestion using SPV and livestock or poultry manure as substrates.

Anaerobic co-digestion of sugarcane press mud with vinasse on methane yield.

PubMed

López González, Lisbet Mailin; Pereda Reyes, Ileana; Romero Romero, Osvaldo

2017-10-01

The conversion efficiency of high solids waste digestion as sugarcane press mud (P) may be limited due to hydrolysis step. The option of co-digestion with vinasse, main liquid waste generated from ethanol production, was investigated under batch regime at mesophilic conditions (37.5±1°C) and the best mixture was evaluated under semicontinuous regime in stirred-tank reactors. The maximum values for methane yield in batch tests were for V 75 /P 25 and V 50 /P 50 mixtures (on basis of the chemical oxygen demand (COD) percentage added in the mixture), with an average value of 246NmL CH 4 g -1 COD fed , which was 13% higher than that of press mud alone. A highest methane production rate of 69.6NmL CH 4 g -1 COD fed -1 d -1 was obtained for the mixtureV 75 /P 25 . During the experiment carried out in CSTR reactors, the organic loading rate (OLR) was increased from 0.5 up to 2.2gVSL -1 d -1 . Methane yields of 365L CH 4 kg -1 VS and biogas productivities of 1.6LL -1 were obtained in co-digestion, which was 64% higher in comparison to mono-digestion. The performance of the process in mono-digestion was less stable than in co-digestion, with a significant fall of methane yield to 1.8kgVSm -3 d -1 , and a partial inhibition of the methanogenic archaeas when the OLR was increased up to 2.2kgVSm -3 d -1 . The co-digestion of vinasse with press mud is a good option for the treatment of streams at the alcohol-sugar industry. Copyright © 2017 Elsevier Ltd. All rights reserved.

Effect of feeding of blend of essential oils on methane production, growth, and nutrient utilization in growing buffaloes

PubMed Central

2018-01-01

Objective An experiment was conducted to study the effect of a blend of essential oils (BEO) on enteric methane emission and growth performance of buffaloes (Bubalus bubalis). Methods Twenty one growing male buffaloes (average body weight of 279±9.3 kg) were divided in to three groups. The animals of all the three groups were fed on a ration consisting of wheat straw and concentrate mixture targeting 500 g daily live weight gain. The three dietary groups were; Group 1, control without additive; Group 2 and 3, supplemented with BEO at 0.15 and 0.30 mL/kg of dry matter intake (DMI), respectively. Results During six months feeding trial, the intake and digestibility of dry matter and nutrients (organic matter, crude protein, ether extract, neutral detergent fibre, and acid detergent fibre) were similar in all the groups. The average body weight gain was tended to improve (p = 0.084) in Group 2 and Group 3 as compared to control animals. Feeding of BEO did not affect feed conversion efficiency of the animals. The calves of all the three groups were in positive nitrogen balance with no difference in nitrogen metabolism. During respiration chamber studies the methane production (L/kg DMI and L/kg digestible dry matter intake was significantly (p<0.001) lower in Group 2 and Group 3 as compared to control animals. Conclusion The results indicated that the BEO tested in the present study have shown potential to reduce enteric methane production without compromising the nutrient utilization and animal performance and could be further explored for its use as feed additive to mitigate enteric methane production in livestock. PMID:28231698

More feed efficient sheep produce less methane and carbon dioxide when eating high-quality pellets.

PubMed

Paganoni, B; Rose, G; Macleay, C; Jones, C; Brown, D J; Kearney, G; Ferguson, M; Thompson, A N

2017-09-01

The Australian sheep industry aims to increase the efficiency of sheep production by decreasing the amount of feed eaten by sheep. Also, feed intake is related to methane production, and more efficient (low residual feed intake) animals eat less than expected. So we tested the hypothesis that more efficient sheep produce less methane by investigating the genetic correlations between feed intake, residual feed intake, methane, carbon dioxide, and oxygen. Feed intake, methane, oxygen, and carbon dioxide were measured on Merino ewes at postweaning (1,866 at 223 d old), hogget (1,010 sheep at 607 d old), and adult ages (444 sheep at 1,080 d old). Sheep were fed a high-energy grower pellet ad libitum for 35 d. Individual feed intake was measured using automated feeders. Methane was measured using portable accumulation chambers up to 3 times during this feed intake period. Heritabilities and phenotypic and genotypic correlations between traits were estimated using ASReml. Oxygen (range 0.10 to 0.20) and carbon dioxide (range 0.08 to 0.28) were generally more heritable than methane (range 0.11 to 0.14). Selecting to decrease feed intake or residual feed intake will decrease methane (genetic correlation [] range 0.76 to 0.90) and carbon dioxide ( range 0.65 to 0.96). Selecting to decrease intake ( range 0.64 to 0.78) and methane ( range 0.81 to 0.86) in sheep at postweaning age would also decrease intake and methane in hoggets and adults. Furthermore, selecting for lower residual feed intake ( = 0.75) and carbon dioxide ( = 0.90) in hoggets would also decrease these traits in adults. Similarly, selecting for higher oxygen ( = 0.69) in hoggets would also increase this trait in adults. Given these results, the hypothesis that making sheep more feed efficient will decrease their methane production can be accepted. In addition, carbon dioxide is a good indicator trait for feed intake because it has the highest heritability of the gas traits measured; is cheaper, faster, and easier to measure than feed intake and has strong phenotypic and genetic correlations with feed intake. Furthermore, selection for feed intake, feed efficiency, methane, and carbon dioxide can be done early in sheep at postweaning age or hoggets. This early selection reduces the generation interval for breeding, thereby increasing response to selection.

Ceramic membranes with mixed conductivity and their application

NASA Astrophysics Data System (ADS)

Kozhevnikov, V. L.; Leonidov, I. A.; Patrakeev, M. V.

2013-08-01

Data on the catalytic reactors with ceramic membranes possessing mixed oxygen ion and electronic conductivity that make it possible to integrate the processes of oxygen separation and oxidation are analyzed and generalized. The development of this approach is of interest for the design of energy efficient and environmentally friendly processes for processing natural gas and other raw materials. The general issues concerning the primary processing of light alkanes in reactors with oxygen separating membranes are expounded and general demands to the membrane materials are discussed. Particular attention is paid to the process of oxidative conversion of methane to synthesis gas. The bibliography includes 110 references.

Solution combustion synthesis of metal oxide nanomaterials for energy storage and conversion.

PubMed

Li, Fa-tang; Ran, Jingrun; Jaroniec, Mietek; Qiao, Shi Zhang

2015-11-14

The design and synthesis of metal oxide nanomaterials is one of the key steps for achieving highly efficient energy conversion and storage on an industrial scale. Solution combustion synthesis (SCS) is a time- and energy-saving method as compared with other routes, especially for the preparation of complex oxides which can be easily adapted for scale-up applications. This review summarizes the synthesis of various metal oxide nanomaterials and their applications for energy conversion and storage, including lithium-ion batteries, supercapacitors, hydrogen and methane production, fuel cells and solar cells. In particular, some novel concepts such as reverse support combustion, self-combustion of ionic liquids, and creation of oxygen vacancies are presented. SCS has some unique advantages such as its capability for in situ doping of oxides and construction of heterojunctions. The well-developed porosity and large specific surface area caused by gas evolution during the combustion process endow the resulting materials with exceptional properties. The relationship between the structural properties of the metal oxides studied and their performance is discussed. Finally, the conclusions and perspectives are briefly presented.

Solution combustion synthesis of metal oxide nanomaterials for energy storage and conversion

NASA Astrophysics Data System (ADS)

Li, Fa-Tang; Ran, Jingrun; Jaroniec, Mietek; Qiao, Shi Zhang

2015-10-01

The design and synthesis of metal oxide nanomaterials is one of the key steps for achieving highly efficient energy conversion and storage on an industrial scale. Solution combustion synthesis (SCS) is a time- and energy-saving method as compared with other routes, especially for the preparation of complex oxides which can be easily adapted for scale-up applications. This review summarizes the synthesis of various metal oxide nanomaterials and their applications for energy conversion and storage, including lithium-ion batteries, supercapacitors, hydrogen and methane production, fuel cells and solar cells. In particular, some novel concepts such as reverse support combustion, self-combustion of ionic liquids, and creation of oxygen vacancies are presented. SCS has some unique advantages such as its capability for in situ doping of oxides and construction of heterojunctions. The well-developed porosity and large specific surface area caused by gas evolution during the combustion process endow the resulting materials with exceptional properties. The relationship between the structural properties of the metal oxides studied and their performance is discussed. Finally, the conclusions and perspectives are briefly presented.

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.

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.

Methane biofiltration using autoclaved aerated concrete as the carrier material.

PubMed

Ganendra, Giovanni; Mercado-Garcia, Daniel; Hernandez-Sanabria, Emma; Boeckx, Pascal; Ho, Adrian; Boon, Nico

2015-09-01

The methane removal capacity of mixed methane-oxidizing bacteria (MOB) culture in a biofilter setup using autoclaved aerated concrete (AAC) as a highly porous carrier material was tested. Batch experiment was performed to optimize MOB immobilization on AAC specimens where optimum methane removal was obtained when calcium chloride was not added during bacterial inoculation step and 10-mm-thick AAC specimens were used. The immobilized MOB could remove methane at low concentration (~1000 ppmv) in a biofilter setup for 127 days at average removal efficiency (RE) of 28.7 %. Unlike a plug flow reactor, increasing the total volume of the filter by adding a biofilter in series did not result in higher total RE. MOB also exhibited a higher abundance at the bottom of the filter, in proximity with the methane gas inlet where a high methane concentration was found. Overall, an efficient methane biofilter performance could be obtained using AAC as the carrier material.

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.

Principal Factors for High Performance of Odor and Methane degrading Biocover using Network Analysis

NASA Astrophysics Data System (ADS)

Jung, H.; Yun, J.; O, G. C.; Ryu, H. W.; Jeon, J. M.; Cho, K. S.

2016-12-01

Methane is 25 times more powerful greenhouse gas than carbon dioxide and plays an important role in global warming. Landfills are one of the biggest methane sources and have emitted 37% of anthropogenic methane in Korea. Applying biocovers in landfills is known to be efficient for the simultaneous mitigation of methane as well as odor which occurs severe civil claims. In this study, three pilot-scale biocovers (2.5mx5mx1m) were constructed in a sanitary landfill at Gwangyang, Korea to establish the optimal operational conditions of biocover. All biocovers are filled with soil, EG microbial agent, food waste compost, and perlite with different combination. Pilot-scale biocovers have been operated since January in this year for simultaneous removal of odor and methane. The concentrations of methane and odors such as ammonia, H2S, methyl mercaptane, methylsulfide, dimetyl disulfide, i-valeraldehyde, and styrene were measured at the inlet and outlet of biocovers each month using GC and HPLC for removal performance evaluation. The biocover with highest removal efficiency eliminated 98.4% of odor and 100.0% of methane. All removal efficiencies of odor measured during experiment are in 81.1 98.4% range, and those of methane are in 3.6 100.0%. Three months later after biocover construction, all biocovers with mixed packing material showed better methane degradation performance than the biocovers packed only with soil. The packing materials of biocovers were sampled during winter (January), spring (April) and summer (July), and their microbial communities were examined based on 16S rDNA using 454 pyrosequencing to detect microbial factors that affects the removal efficiency. Methanotrophs which are known as methane-degradable bacteria take 10 25% of microbial community in biocovers, and most of those found in biocovers are type methanothrophs. Network analysis is performed and principal factors for performance improvement of biocovers are derived. Based on this study, well-designed biocovers will be newly set up in the operational landfill with the consideration of derived principal factors for high efficiency. This research was supported by the Korea Ministry of Environment as a "Converging Technology Project (2015001640003)".

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.

Countercurrent extraction of soluble sugars from almond hulls and assessment of the bioenergy potential.

PubMed

Holtman, Kevin M; Offeman, Richard D; Franqui-Villanueva, Diana; Bayati, Andre K; Orts, William J

2015-03-11

Almond hulls contain considerable proportions (37% by dry weight) of water-soluble, fermentable sugars (sucrose, glucose, and fructose), which can be extracted for industrial purposes. The maximum optimal solids loading was determined to be 20% for sugar extraction, and the addition of 0.5% (w/v) pectinase aided in maintaining a sufficient free water volume for sugar recovery. A laboratory countercurrent extraction experiment utilizing a 1 h steep followed by three extraction (wash) stages produced a high-concentration (131 g/L fermentable sugar) syrup. Overall, sugar recovery efficiency was 88%. The inner stage washing efficiencies were compatible with solution equilibrium calculations, indicating that efficiency was high. The concentrated sugar syrup was fermented to ethanol at high efficiency (86% conversion), and ethanol concentrations in the broth were 7.4% (v/v). Thin stillage contained 233 g SCOD/L, which was converted to biomethane at an efficiency of 90% with a biomethane potential of 297 mL/g SCODdestroyed. Overall, results suggested that a minima of 49 gal (185 L) ethanol and 75 m(3) methane/t hulls (dry whole hull basis) are achievable.

Self-Cleaning Boudouard Reactor for Full Oxygen Recovery from CO2 Project

NASA Technical Reports Server (NTRS)

Zeitlin, Nancy; Muscatello, Anthony

2015-01-01

Oxygen recovery from respiratory CO2 is an important aspect of human spaceflight. Methods exist to sequester the CO2, but production of oxygen needs further development. The current ISS Carbon Dioxide Reduction System (CRS) uses the Sabatier reaction to produce water (and ultimately breathing air). Oxygen recovery is limited to 50% because half of the hydrogen used in the Sabatier reactor is lost as methane, which is vented overboard. The Bosch reaction is the only real alternative to the Sabatier reaction, but in the last reaction in the cycle (Boudouard) the resulting carbon buildup will eventually foul the nickel or iron catalyst, reducing reactor life and increasing consumables. To minimize this fouling, find a use for this waste product, and increase efficiency, we propose testing various self-cleaning catalyst designs in an existing MSFC Boudouard reaction test bed and to determine which one is the most reliable in conversion and lack of fouling. Challenges include mechanical reliability of the cleaning method and maintaining high conversion efficiency with lower catalyst surface area. The above chemical reactions are well understood, but planned implementations are novel (TRL 2) and haven't been investigated at any level.

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

Macroalgae for CO 2 Capture and Renewable Energy - A Pilot Project

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

Wiley, Kristine

2011-01-31

The objective of this project was to demonstrate, at a pilot scale, the beneficial use of carbon dioxide (CO 2) through a technology designed to capture CO 2 from fossil-fuel fired power plant stack gas, generating macroalgae and converting the macroalgae at high efficiency to renewable methane that can be utilized in the power plant or introduced into a natural gas pipeline. The proposed pilot plant would demonstrate the cost-effectiveness and CO 2/ NO x flue-gas removal efficiency of an innovative algal scrubber technology where seaweeds are grown out of water on specially-designed supporting structures contained within greenhouses where themore » plants are constantly bathed by recycled nutrient sprays enriched by flue gas constituents. The work described in this document addresses Phase 1 of the project only. The scope of work for Phase 1 includes the completion of a preliminary design package; the collection of additional experimental data to support the preliminary and detailed design for a pilot scale utilization of CO 2 to cultivate macroalage and to process that algae to produce methane; and a technological and economic analysis to evaluate the potential of the system. Selection criteria for macroalgae that could survive the elevated temperatures and potential periodic desiccation of near desert project sites were identified. Samples of the selected macroalgae species were obtained and then subjected to anaerobic digestion to determine conversions and potential methane yields. A Process Design Package (PDP) was assembled that included process design, process flow diagram, material balance, instrumentation, and equipment list, sizes, and cost for the Phase 2 pilot plant. Preliminary economic assessments were performed under the various assumptions made, which are purposely conservative. Based on the results, additional development work should be conducted to delineate the areas for improving efficiency, reducing contingencies, and reducing overall costs.« 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.

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

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.

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.

Methane production from a field-scale biofilter designed for desulfurization of biogas stream.

PubMed

Pirolli, Mateus; da Silva, Márcio Luís Busi; Mezzari, Melissa Paola; Michelon, William; Prandini, Jean Michel; Moreira Soares, Hugo

2016-07-15

The development of a simple and low maintenance field-scale biotrickling filter (BTF) for desulfurization of swine wastewater-derived biogas stream that was also capable of increasing biomethane concentrations was investigated. BTF was continuously fed with wastewater effluent from an air sparged nitrification-denitrification bioreactor installed downgradient from an UASB-type digester. BTF maximum removal efficiency (RE) of 99.8% was achieved with a maximum elimination capacity (EC) of 1,509 g H2S m(-3) h(-1). Average EC obtained with inlet biogas flow rates of 0.024, 0.036 and 0.048 m(3) h(-1) was 718, 1,013 and 438 g H2S m(-3) h(-1), respectively. SO4(-2) and S(0) were the major metabolites produced from biological conversion of H2S. Additionally to the satisfactory biodesulfurization capacity, an average increase in methane concentration of ≅ 3.8 ± 1.68 g m(-3) was measured in the filtered gas stream throughout 200 days of BTF operation. RT-PCR analyses of archaea communities in the biofilm confirmed dominance of hydrogenotrophic methanogens thus corroborating with the observed strong correlation between CO2 removal and CH4 production. Among the three major archaea orders investigated (i.e., Methanosarcinales, Methanobacteriales, and Methanomicrobiales), Methanobacteriales were encountered at highest concentrations (1.9 × 10(11) gene copies mL(-1)). The proposed BTF was robust efficiently removing H2S from biogas stream while concomitantly enhancing the concentration of valuable methane as source of renewable fuel. Copyright © 2016 Elsevier Ltd. All rights reserved.

Learning reduced kinetic Monte Carlo models of complex chemistry from molecular dynamics

DOE PAGES

Yang, Qian; Sing-Long, Carlos A.; Reed, Evan J.

2017-06-19

Here, we propose a novel statistical learning framework for automatically and efficiently building reduced kinetic Monte Carlo (KMC) models of large-scale elementary reaction networks from data generated by a single or few molecular dynamics simulations (MD). Existing approaches for identifying species and reactions from molecular dynamics typically use bond length and duration criteria, where bond duration is a fixed parameter motivated by an understanding of bond vibrational frequencies. Conversely, we show that for highly reactive systems, bond duration should be a model parameter that is chosen to maximize the predictive power of the resulting statistical model. We demonstrate our methodmore » on a high temperature, high pressure system of reacting liquid methane, and show that the learned KMC model is able to extrapolate more than an order of magnitude in time for key molecules. Additionally, our KMC model of elementary reactions enables us to isolate the most important set of reactions governing the behavior of key molecules found in the MD simulation. We develop a new data-driven algorithm to reduce the chemical reaction network which can be solved either as an integer program or efficiently using L1 regularization, and compare our results with simple count-based reduction. For our liquid methane system, we discover that rare reactions do not play a significant role in the system, and find that less than 7% of the approximately 2000 reactions observed from molecular dynamics are necessary to reproduce the molecular concentration over time of methane. Furthermore, we describe a framework in this work that paves the way towards a genomic approach to studying complex chemical systems, where expensive MD simulation data can be reused to contribute to an increasingly large and accurate genome of elementary reactions and rates.« 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.

Effect of methane partial pressure on the performance of a membrane biofilm reactor coupling methane-dependent denitrification and anammox.

PubMed

Cai, Chen; Hu, Shihu; Chen, Xueming; Ni, Bing-Jie; Pu, Jiaoyang; Yuan, Zhiguo

2018-10-15

Complete nitrogen removal has recently been demonstrated by integrating anaerobic ammonium oxidation (anammox) and denitrifying anaerobic methane oxidation (DAMO) processes. In this work, the effect of methane partial pressure on the performance of a membrane biofilm reactor (MBfR) consisting of DAMO and anammox microorganisms was evaluated. The activities of DAMO archaea and DAMO bacteria in the biofilm increased significantly with increased methane partial pressure, from 367 ± 9 and 58 ± 22 mg-N L -1 d -1 to 580 ± 12 and 222 ± 22 mg-N L -1 d -1 , respectively, while the activity of anammox bacteria only increased slightly, when the methane partial pressure was elevated from 0.24 to 1.39 atm in the short-term batch tests. The results were supported by a long-term (seven weeks) continuous test, when the methane partial pressure was dropped from 1.39 to 0.78 atm. The methane utilization efficiency was always above 96% during both short-term and long-term tests. Taken together, nitrogen removal rate (especially the nitrate reduction rate by DAMO archaea) and methane utilization efficiency could be maintained at high levels in a broad range of methane partial pressure (0.24-1.39 atm in this study). In addition, a previously established DAMO/anammox biofilm model was used to analyze the experimental data. The observed impacts of methane partial pressure on biofilm activity were well explained by the modeling results. These results suggest that methane partial pressure can potentially be used as a manipulated variable to control reaction rates, ultimately to maintain high nitrogen removal efficiency, according to nitrogen loading rate. Copyright © 2018 Elsevier B.V. All rights reserved.

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.

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

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.

Mitigation of methane emission from an old unlined landfill in Klintholm, Denmark using a passive biocover system

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

Scheutz, Charlotte; Pedersen, Rasmus Broe; Petersen, Per Haugsted

Highlights: • An innovative biocover system was constructed on a landfill cell to mitigate the methane emission. • The biocover system had a mitigation efficiently of typically 80%. • The system also worked efficiently at ambient temperatures below freezing. • A whole landfill emission measurement tool was required to document the biocover system efficiency. - Abstract: Methane generated at landfills contributes to global warming and can be mitigated by biocover systems relying on microbial methane oxidation. As part of a closure plan for an old unlined landfill without any gas management measures, an innovative biocover system was established. The systemmore » was designed based on a conceptual model of the gas emission patterns established through an initial baseline study. The study included construction of gas collection trenches along the slopes of the landfill where the majority of the methane emissions occurred. Local compost materials were tested as to their usefulness as bioactive methane oxidizing material and a suitable compost mixture was selected. Whole site methane emission quantifications based on combined tracer release and downwind measurements in combination with several local experimental activities (gas composition within biocover layers, flux chamber based emission measurements and logging of compost temperatures) proved that the biocover system had an average mitigation efficiency of approximately 80%. The study showed that the system also had a high efficiency during winter periods with temperatures below freezing. An economic analysis indicated that the mitigation costs of the biocover system were competitive to other existing greenhouse gas mitigation options.« less

Temperature-phased anaerobic digestion of food waste: A comparison with single-stage digestions based on performance and energy balance.

PubMed

Xiao, Benyi; Qin, Yu; Zhang, Wenzhe; Wu, Jing; Qiang, Hong; Liu, Junxin; Li, Yu-You

2018-02-01

The temperature-phased anaerobic digestion (TPAD) of food waste was studied for the purpose of comparing with single-stage mesophilic and thermophilic anaerobic digestion. The biogas and methane yields in the TPAD during the steady period were 0.759 ± 0.115 L/g added VS and 0.454 ± 0.201 L/g added VS, which were lower than those in the two single-stage anaerobic digestion. The improper sludge retention time may be the reason for the lower biogas and methane production in TPAD. The removal of volatile solids in the TPAD was 78.55 ± 4.59% and the lowest among the three anaerobic digestion processes. The reaction ratios of the four anaerobic digestion steps in the TPAD were all lower than those in the two single-stage anaerobic digestion. The energy conversion efficiency of the degraded substrate in the TPAD was similar with those in single-stage mesophilic and thermophilic anaerobic digestion systems. Copyright © 2017 Elsevier Ltd. All rights reserved.

Methanogenic degradation of toilet-paper cellulose upon sewage treatment in an anaerobic membrane bioreactor at room temperature.

PubMed

Chen, Rong; Nie, Yulun; Kato, Hiroyuki; Wu, Jiang; Utashiro, Tetsuya; Lu, Jianbo; Yue, Shangchao; Jiang, Hongyu; Zhang, Lu; Li, Yu-You

2017-03-01

Toilet-paper cellulose with rich but refractory carbon sources, are the main insoluble COD fractions in sewage. An anaerobic membrane bioreactor (AnMBR) was configured for sewage treatment at room temperature and its performance on methanogenic degradation of toilet paper was highlighted. The results showed, high organic removal (95%), high methane conversion (90%) and low sludge yield (0.08gVSS/gCOD) were achieved in the AnMBR. Toilet-paper cellulose was fully biodegraded without accumulation in the mixed liquor and membrane cake layer. Bioconversion efficiency of toilet paper approached 100% under a high organic loading rate (OLR) of 2.02gCOD/L/d and it could provide around 26% of total methane generation at most of OLRs. Long sludge retention time and co-digestion of insoluble/soluble COD fractions achieving mutualism of functional microorganisms, contributed to biodegradation of toilet-paper cellulose. Therefore the AnMBR successfully implemented simultaneously methanogenic bioconversion of toilet-paper cellulose and soluble COD in sewage at room temperature. Copyright © 2016 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.

Modeling and comparative assessment of bubbling fluidized bed gasification system for syngas production - a gateway for a cleaner future in Pakistan.

PubMed

Shehzad, Areeb; Bashir, Mohammed J K; Horttanainen, Mika; Manttari, Mika; Havukainen, Jouni; Abbas, Ghulam

2017-06-19

The present study explores the potential of MSW gasification for exergy analysis and has been recently given a premier attention in a region like Pakistan where the urbanization is rapidly growing and resources are few. The plant capacity was set at 50 MW based on reference data available and the total exergetic efficiency was recorded to be 31.5 MW. The largest irreversibility distribution appears in the gasifier followed by methanation unit and CO 2 capture. The effect of process temperature, equivalence ratio and MSW moisture content was explored for inspecting the variations in syngas composition, lower heating value, carbon conversion efficiency and cold gas efficiency. Special attention of the paper is paid to the comparative assessment of MSW gasification products in four regions, namely Pakistan, USA, UAE and Thailand. This extended study gave an insight into the spectrum of socioeconomic conditions with varying MSW compositions in order to explain the effect of MSW composition variance on the gasification products.

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.

Development of an advanced Sabatier CO2 reduction subsystem

NASA Technical Reports Server (NTRS)

Kleiner, G. N.; Cusick, R. J.

1981-01-01

A preprototype Sabatier CO2 reduction subsystem was successfully designed, fabricated and tested. The lightweight, quick starting (less than 5 minutes) reactor utlizes a highly active and physically durable methanation catalyst composed of ruthenium on alumina. The use of this improved catalyst permits a simple, passively controlled reactor design with an average lean component H2/CO2 conversion efficiency of over 99% over a range of H2/CO2 molar ratios of 1.8 to 5 while operating with process flows equivalent to a crew size of up to five persons. The subsystem requires no heater operation after start-up even during simulated 55 minute lightside/39 minute darkside orbital operation.

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.

Compact, Lightweight Adsorber and Sabatier Reactor for CO2 Capture and Reduction for Consumable and Propellant Production

NASA Technical Reports Server (NTRS)

Junaedi, Christian; Hawley, Kyle; Walsh, Dennis; Roychoudhury, Subir; Busby, Stacy A.; Abney, Morgan B.; Perry, Jay L.; Knox, James C.

2012-01-01

The utilization of CO2 to produce (or recycle) life support consumables, such as O2 and H2O, and to generate propellant fuels is an important aspect of NASA's concept for future, long duration planetary exploration. One potential approach is to capture and use CO2 from the Martian atmosphere to generate the consumables and propellant fuels. Precision Combustion, Inc. (PCI), with support from NASA, continues to develop its regenerable adsorber technology for capturing CO2 from gaseous atmospheres (for cabin atmosphere revitalization and in-situ resource utilization applications) and its Sabatier reactor for converting CO2 to methane and water. Both technologies are based on PCI's Microlith(R) substrates and have been demonstrated to reduce size, weight, and power consumption during CO2 capture and methanation process. For adsorber applications, the Microlith substrates offer a unique resistive heating capability that shows potential for short regeneration time and reduced power requirements compared to conventional systems. For the Sabatier applications, the combination of the Microlith substrates and durable catalyst coating permits efficient CO2 methanation that favors high reactant conversion, high selectivity, and durability. Results from performance testing at various operating conditions will be presented. An effort to optimize the Sabatier reactor and to develop a bench-top Sabatier Development Unit (SDU) will be discussed.

Effect of the anode feeding composition on the performance of a continuous-flow methane-producing microbial electrolysis cell.

PubMed

Zeppilli, Marco; Villano, Marianna; Aulenta, Federico; Lampis, Silvia; Vallini, Giovanni; Majone, Mauro

2015-05-01

A methane-producing microbial electrolysis cell (MEC) was continuously fed at the anode with a synthetic solution of soluble organic compounds simulating the composition of the soluble fraction of a municipal wastewater. The MEC performance was assessed at different anode potentials in terms of chemical oxygen demand (COD) removal efficiency, methane production, and energy efficiency. As a main result, about 72-80% of the removed substrate was converted into current at the anode, and about 84-86% of the current was converted into methane at the cathode. Moreover, even though both COD removed and methane production slightly decreased as the applied anode potential decreased, the energy efficiency (i.e., the energy recovered as methane with respect to the energy input into the system) increased from 54 to 63%. Denaturing gradient gel electrophoresis (DGGE) analyses revealed a high diversity in the anodic bacterial community with the presence of both fermentative (Proteiniphilum acetatigenes and Petrimonas sulphurifila) and aerobic (Rhodococcus qingshengii) microorganisms, whereas only two microorganisms (Methanobrevibacter arboriphilus and Methanosarcina mazei), both assignable to methanogens, were observed in the cathodic community.

A full scale worm reactor for efficient sludge reduction by predation in a wastewater treatment plant.

PubMed

Tamis, J; van Schouwenburg, G; Kleerebezem, R; van Loosdrecht, M C M

2011-11-15

Sludge predation can be an effective solution to reduce sludge production at a wastewater treatment plant. Oligochaete worms are the natural consumers of biomass in benthic layers in ecosystems. In this study the results of secondary sludge degradation by the aquatic Oligochaete worm Aulophorus furcatus in a 125 m(3) reactor and further sludge conversion in an anaerobic tank are presented. The system was operated over a period of 4 years at WWTP Wolvega, the Netherlands and was fed with secondary sludge from a low loaded activated sludge process. It was possible to maintain a stable and active population of the aquatic worm species A. furcatus during the full period. Under optimal conditions a sludge conversion of 150-200 kg TSS/d or 1.2-1.6 kg TSS/m(3)/d was established in the worm reactor. The worms grew as a biofilm on carrier material in the reactor. The surface specific conversion rate reached 140-180 g TSS/m(2)d and the worm biomass specific conversion rate was 0.5-1 g TSS sludge/g dry weight worms per day. The sludge reduction under optimal conditions in the worm reactor was 30-40%. The degradation by worms was an order of magnitude larger than the endogenous conversion rate of the secondary sludge. Effluent sludge from the worm reactor was stored in an anaerobic tank where methanogenic processes became apparent. It appeared that besides reducing the sludge amount, the worms' activity increased anaerobic digestibility, allowing for future optimisation of the total system by maximising sludge reduction and methane formation. In the whole system it was possible to reduce the amount of sludge by at least 65% on TSS basis. This is a much better total conversion than reported for anaerobic biodegradability of secondary sludge of 20-30% efficiency in terms of TSS reduction. Copyright © 2011 Elsevier Ltd. All rights reserved.

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.

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

Photosynthesis of organic compounds in the atmosphere of Jupiter

NASA Technical Reports Server (NTRS)

Ferris, J. P.; Chen, C. T.

1975-01-01

An efficient conversion of CH4 to hydrocarbons and HCN takes place when NH3 is photolysed in the presence of CH4, H2, and He using a 184.9 nm light source. The extent of NH3 decomposition after a 1 hr exposure was determined spectrophotometrically; CH4, N2, and C2 and C3 hydrocarbons were detected and analyzed by mass spectrometry. Photolysis of one molar equivalent of NH3 results in the loss of 0.84 molar equivalent of CH4, which apparently reacts with hot hydrogen atoms produced by photolysis. The 8% of the NH3 which is not converted to N2 probably is converted to organic amines and nitrile derivatives. The results indicate that NH3 photolysis is a highly probable mechanism for the conversion of methane to more complex hydrocarbons in the upper atmosphere of Jupiter, and predict the occurrence of HCN, NH2NH2, and higher hydrocarbons in the Jovian atmosphere above the NH3 clouds.

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.

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.

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.

Energy efficiency analysis: biomass-to-wheel efficiency related with biofuels production, fuel distribution, and powertrain systems.

PubMed

Huang, Wei-Dong; Zhang, Y-H Percival

2011-01-01

Energy efficiency analysis for different biomass-utilization scenarios would help make more informed decisions for developing future biomass-based transportation systems. Diverse biofuels produced from biomass include cellulosic ethanol, butanol, fatty acid ethyl esters, methane, hydrogen, methanol, dimethyether, Fischer-Tropsch diesel, and bioelectricity; the respective powertrain systems include internal combustion engine (ICE) vehicles, hybrid electric vehicles based on gasoline or diesel ICEs, hydrogen fuel cell vehicles, sugar fuel cell vehicles (SFCV), and battery electric vehicles (BEV). We conducted a simple, straightforward, and transparent biomass-to-wheel (BTW) analysis including three separate conversion elements--biomass-to-fuel conversion, fuel transport and distribution, and respective powertrain systems. BTW efficiency is a ratio of the kinetic energy of an automobile's wheels to the chemical energy of delivered biomass just before entering biorefineries. Up to 13 scenarios were analyzed and compared to a base line case--corn ethanol/ICE. This analysis suggests that BEV, whose electricity is generated from stationary fuel cells, and SFCV, based on a hydrogen fuel cell vehicle with an on-board sugar-to-hydrogen bioreformer, would have the highest BTW efficiencies, nearly four times that of ethanol-ICE. In the long term, a small fraction of the annual US biomass (e.g., 7.1%, or 700 million tons of biomass) would be sufficient to meet 100% of light-duty passenger vehicle fuel needs (i.e., 150 billion gallons of gasoline/ethanol per year), through up to four-fold enhanced BTW efficiencies by using SFCV or BEV. SFCV would have several advantages over BEV: much higher energy storage densities, faster refilling rates, better safety, and less environmental burdens.

Energy Efficiency Analysis: Biomass-to-Wheel Efficiency Related with Biofuels Production, Fuel Distribution, and Powertrain Systems

PubMed Central

Huang, Wei-Dong; Zhang, Y-H Percival

2011-01-01

Background Energy efficiency analysis for different biomass-utilization scenarios would help make more informed decisions for developing future biomass-based transportation systems. Diverse biofuels produced from biomass include cellulosic ethanol, butanol, fatty acid ethyl esters, methane, hydrogen, methanol, dimethyether, Fischer-Tropsch diesel, and bioelectricity; the respective powertrain systems include internal combustion engine (ICE) vehicles, hybrid electric vehicles based on gasoline or diesel ICEs, hydrogen fuel cell vehicles, sugar fuel cell vehicles (SFCV), and battery electric vehicles (BEV). Methodology/Principal Findings We conducted a simple, straightforward, and transparent biomass-to-wheel (BTW) analysis including three separate conversion elements -- biomass-to-fuel conversion, fuel transport and distribution, and respective powertrain systems. BTW efficiency is a ratio of the kinetic energy of an automobile's wheels to the chemical energy of delivered biomass just before entering biorefineries. Up to 13 scenarios were analyzed and compared to a base line case – corn ethanol/ICE. This analysis suggests that BEV, whose electricity is generated from stationary fuel cells, and SFCV, based on a hydrogen fuel cell vehicle with an on-board sugar-to-hydrogen bioreformer, would have the highest BTW efficiencies, nearly four times that of ethanol-ICE. Significance In the long term, a small fraction of the annual US biomass (e.g., 7.1%, or 700 million tons of biomass) would be sufficient to meet 100% of light-duty passenger vehicle fuel needs (i.e., 150 billion gallons of gasoline/ethanol per year), through up to four-fold enhanced BTW efficiencies by using SFCV or BEV. SFCV would have several advantages over BEV: much higher energy storage densities, faster refilling rates, better safety, and less environmental burdens. PMID:21765941

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.

Trace Gas Measurements on Mars and Earth Using Optical Parametric Generation

NASA Technical Reports Server (NTRS)

Numata, Kenji; Haris, Riris; Li, Steve; Sun, Xiaoli; Abshire, James Brice

2010-01-01

Trace gases and their isotopic ratios in planetary atmospheres offer important but subtle clues as to the origins of a planet's atmosphere, hydrology, geology, and potential for biology. An orbiting laser remote sensing instrument is capable of measuring trace gases on a global scale with unprecedented accuracy, and higher spatial resolution that can be obtained by passive instruments. We have developed an active sensing instrument for the remote measurement of trace gases in planetary atmospheres (including Earth). The technique uses widely tunable, seeded optical parametric generation (OPG) to measure methane, CO2, water vapor, and other trace gases in the near and mid-infrared spectral regions. Methane is a strong greenhouse gas on Earth and it is also a potential biogenic marker on Mars and other planets. Methane in the Earth's atmosphere survives for a shorter time than CO2 but its impact on climate change can be larger than CO2. Methane levels have remained relatively constant over the last decade around 1.78 parts per million (ppm) but recent observations indicate that methane levels may be on the rise. Increasing methane concentrations may trigger a positive feedback loop and a subsequent runaway greenhouse effect, where increasing temperatures result in increasing methane levels. The NRC Decadal Survey recognized the importance of global observations of greenhouse gases and called for simultaneous CH4, CO, and CO2 measurements but also underlined the technological limitations for these observations. For Mars, methane measurements are of great interest because of its potential as a strong biogenic marker. A remote sensing instrument that can measure day and night over all seasons and latitudes can identify and localize sources of biogenic gas plumes produced by subsurface chemistry or biology, and aid in the search for extra-terrestrial life. It can identify the dynamics of methane generation over time and latitude and identify future lander mission sites for more detailed in-situ analysis. In this paper we report on remote sensing measurements of methane using a high peak power, widely tunable optical parametric generator (OPG) operating at 3.3 micron and 1.65 micron. The OPG is pumped by a passively q-switched single frequency laser (3ns, 5KHz, 50uJ) and seeded by a diode laser. The spectral width of both signal and idler of seeded OPG is nearly Fourier transform limited. The output of seeded OPG is single frequency with high spectral purity and is widely tunable. Both 1650 nm and 3300 nm can be generated with a conversion efficiency of more than 30%. We have demonstrated detection of methane at 3274 nm and 1650 nm in a cell and also performed open path atmospheric measurements of methane at the same wavelengths. Finally, we were able to demonstrate simultaneous detection of methane at 3270.4 nm and CO2 at 1578.2 nm. In this paper we will discuss the OPG performance and atmospheric open path measurement results.

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

Ultrasonic sludge disintegration for enhanced methane production in anaerobic digestion: effects of sludge hydrolysis efficiency and hydraulic retention time.

PubMed

Kim, Dong-Jin; Lee, Jonghak

2012-01-01

Hydrolysis of waste activated sludge (WAS) has been regarded as the rate limiting step of anaerobic sludge digestion. Therefore, in this study, the effect of ultrasound and hydraulic residence time during sludge hydrolysis was investigated with the goal of enhancing methane production from anaerobic digestion (AD). WAS was ultrasonically disintegrated for hydrolysis, and it was semi-continuously fed to an anaerobic digesters at various hydraulic retention times (HRTs). The results of these experiments showed that the solids and chemical oxygen demand (COD) removal efficiencies when using ultrasonically disintegrated sludge were higher during AD than the control sludge. The longer the HRT, the higher the removal efficiencies of solids and COD, while methane production increased with lower HRT. Sludge with 30% hydrolysis produced 7 × more methane production than the control sludge. The highest methane yields were 0.350 m(3)/kg volatile solids (VS)(add) and 0.301 m(3)/kg COD(con) for 16 and 30% hydrolyzed sludge, respectively. In addition, we found that excess ultrasound irradiation may inhibit AD since the 50% hydrolyzed sludge produced lower methane yields than 16 and 30% hydrolyzed sludge.

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.

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

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.

Reversing methanogenesis to capture methane for liquid biofuel precursors

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

Soo, Valerie W. C.; McAnulty, Michael J.; Tripathi, Arti

Energy from remote methane reserves is transformative; however, unintended release of this potent greenhouse gas makes it imperative to convert methane efficiently into more readily transported biofuels. No pure microbial culture that grows on methane anaerobically has been isolated, despite that methane capture through anaerobic processes is more efficient than aerobic ones. Here we engineered the archaeal methanogen Methanosarcina acetivorans to grow anaerobically on methane as a pure culture and to convert methane into the biofuel precursor acetate. To capture methane, we cloned the enzyme methyl-coenzyme M reductase (Mcr) from an unculturable organism, anaerobic methanotrophic archaeal population 1 (ANME-1) frommore » a Black Sea mat, into M. acetivorans to effectively run methanogenesis in reverse. Starting with low-density inocula, M. acetivorans cells producing ANME-1 Mcr consumed up to 9 ± 1 % of methane (corresponding to 109 ± 12 µmol of methane) after 6 weeks of anaerobic growth on methane and utilized 10 mM FeCl 3 as an electron acceptor. Accordingly, increases in cell density and total protein were observed as cells grew on methane in a biofilm on solid FeCl 3. When incubated on methane for 5 days, high-densities of ANME-1 Mcr-producing M. acetivorans cells consumed 15 ± 2 % methane (corresponding to 143 ± 16 µmol of methane), and produced 10.3 ± 0.8 mM acetate (corresponding to 52 ± 4 µmol of acetate). We further confirmed the growth on methane and acetate production using 13C isotopic labeling of methane and bicarbonate coupled with nuclear magnetic resonance and gas chromatography/mass spectroscopy, as well as RNA sequencing. Lastly, we anticipate that our metabolically-engineered strain will provide insights into how methane is cycled in the environment by Archaea as well as will possibly be utilized to convert remote sources of methane into more easily transported biofuels via acetate.« less

Reversing methanogenesis to capture methane for liquid biofuel precursors

DOE PAGES

Soo, Valerie W. C.; McAnulty, Michael J.; Tripathi, Arti; ...

2016-01-14

Energy from remote methane reserves is transformative; however, unintended release of this potent greenhouse gas makes it imperative to convert methane efficiently into more readily transported biofuels. No pure microbial culture that grows on methane anaerobically has been isolated, despite that methane capture through anaerobic processes is more efficient than aerobic ones. Here we engineered the archaeal methanogen Methanosarcina acetivorans to grow anaerobically on methane as a pure culture and to convert methane into the biofuel precursor acetate. To capture methane, we cloned the enzyme methyl-coenzyme M reductase (Mcr) from an unculturable organism, anaerobic methanotrophic archaeal population 1 (ANME-1) frommore » a Black Sea mat, into M. acetivorans to effectively run methanogenesis in reverse. Starting with low-density inocula, M. acetivorans cells producing ANME-1 Mcr consumed up to 9 ± 1 % of methane (corresponding to 109 ± 12 µmol of methane) after 6 weeks of anaerobic growth on methane and utilized 10 mM FeCl 3 as an electron acceptor. Accordingly, increases in cell density and total protein were observed as cells grew on methane in a biofilm on solid FeCl 3. When incubated on methane for 5 days, high-densities of ANME-1 Mcr-producing M. acetivorans cells consumed 15 ± 2 % methane (corresponding to 143 ± 16 µmol of methane), and produced 10.3 ± 0.8 mM acetate (corresponding to 52 ± 4 µmol of acetate). We further confirmed the growth on methane and acetate production using 13C isotopic labeling of methane and bicarbonate coupled with nuclear magnetic resonance and gas chromatography/mass spectroscopy, as well as RNA sequencing. Lastly, we anticipate that our metabolically-engineered strain will provide insights into how methane is cycled in the environment by Archaea as well as will possibly be utilized to convert remote sources of methane into more easily transported biofuels via acetate.« less

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.

Recent Advances in the Synthesis, Characterization and Application of Zn+-containing Heterogeneous Catalysts.

PubMed

Chen, Guangbo; Zhao, Yufei; Shang, Lu; Waterhouse, Geoffrey I N; Kang, Xiaofeng; Wu, Li-Zhu; Tung, Chen-Ho; Zhang, Tierui

2016-07-01

Monovalent Zn + (3d 10 4s 1 ) systems possess a special electronic structure that can be exploited in heterogeneous catalysis and photocatalysis, though it remains challenge to synthesize Zn + -containing materials. By careful design, Zn + -related species can be synthesized in zeolite and layered double hydroxide systems, which in turn exhibit excellent catalytic potential in methane, CO and CO 2 activation. Furthermore, by utilizing advanced characterization tools, including electron spin resonance, X-ray absorption fine structure and density functional theory calculations, the formation mechanism of the Zn + species and their structure-performance relationships can be understood. Such advanced characterization tools guide the rational design of high-performance Zn + -containing catalysts for efficient energy conversion.

Recent Advances in the Synthesis, Characterization and Application of Zn+‐containing Heterogeneous Catalysts

PubMed Central

Chen, Guangbo; Zhao, Yufei; Shang, Lu; Waterhouse, Geoffrey I. N.; Kang, Xiaofeng; Wu, Li‐Zhu; Tung, Chen‐Ho

2016-01-01

Monovalent Zn+ (3d104s1) systems possess a special electronic structure that can be exploited in heterogeneous catalysis and photocatalysis, though it remains challenge to synthesize Zn+‐containing materials. By careful design, Zn+‐related species can be synthesized in zeolite and layered double hydroxide systems, which in turn exhibit excellent catalytic potential in methane, CO and CO2 activation. Furthermore, by utilizing advanced characterization tools, including electron spin resonance, X‐ray absorption fine structure and density functional theory calculations, the formation mechanism of the Zn+ species and their structure‐performance relationships can be understood. Such advanced characterization tools guide the rational design of high‐performance Zn+‐containing catalysts for efficient energy conversion. PMID:27818902

Conversion of wastes into bioelectricity and chemicals by using microbial electrochemical technologies.

PubMed

Logan, Bruce E; Rabaey, Korneel

2012-08-10

Waste biomass is a cheap and relatively abundant source of electrons for microbes capable of producing electrical current outside the cell. Rapidly developing microbial electrochemical technologies, such as microbial fuel cells, are part of a diverse platform of future sustainable energy and chemical production technologies. We review the key advances that will enable the use of exoelectrogenic microorganisms to generate biofuels, hydrogen gas, methane, and other valuable inorganic and organic chemicals. Moreover, we examine the key challenges for implementing these systems and compare them to similar renewable energy technologies. Although commercial development is already underway in several different applications, ranging from wastewater treatment to industrial chemical production, further research is needed regarding efficiency, scalability, system lifetimes, and reliability.

Quantifying Methane Abatement Efficiency at Three Municipal Solid Waste Landfills; Final Report

EPA Science Inventory

Measurements were conducted at three municipal solid waste landfills to compare fugitive methane emissions from the landfill cells to the quantity of collected gas (i.e., gas collection efficiency). The measurements were conducted over a multi-week sampling campaign using EPA Oth...

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

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

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.

Potential impact of salinity on methane production from food waste anaerobic digestion.

PubMed

Zhao, Jianwei; Liu, Yiwen; Wang, Dongbo; Chen, Fei; Li, Xiaoming; Zeng, Guangming; Yang, Qi

2017-09-01

Previous studies have demonstrated that the presence of sodium chloride (NaCl) inhibited the production of methane from food waste anaerobic digestion. However, the details of how NaCl affects methane production from food waste remain unknown by now and the efficient approach to mitigate the impact of NaCl on methane production was seldom reported. In this paper, the details of how NaCl affects methane production was first investigated via a series of batch experiments. Experimental results showed the effect of NaCl on methane production was dosage dependent. Low level of NaCl improved the hydrolysis and acidification but inhibited the process of methanogenesis whereas high level of NaCl inhibit both steps of acidification and methanogenesis. Then an efficient approach, i.e. co-digestion of food waste and waste activated sludge, to mitigate the impact of NaCl on methane production was reported. Finally, the mechanisms of how co-digestion mitigates the effect on methane production caused by NaCl in co-digestion system were revealed. These findings obtained in this work might be of great importance for the operation of methane recovery from food waste in the presence of NaCl. Copyright © 2017 Elsevier Ltd. All rights reserved.

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

Dry reforming of methane on a highly-active Ni-CeO 2 catalyst: Effects of metal-support interactions on C–H bond breaking

DOE PAGES

Liu, Zongyuan; Grinter, David C.; Lustemberg, Pablo G.; ...

2016-05-04

Ni-CeO 2 is a highly efficient, stable and non-expensive catalyst for methane dry reforming at relative low temperatures (700 K). The active phase of the catalyst consists of small nanoparticles of nickel dispersed on partially reduced ceria. Experiments of ambient pressure XPS indicate that methane dissociates on Ni/CeO 2 at temperatures as low as 300 K, generating CH x and CO x species on the surface of the catalyst. Strong metal–support interactions activate Ni for the dissociation of methane. The results of density-functional calculations show a drop in the effective barrier for methane activation from 0.9 eV on Ni(111) tomore » only 0.15 eV on Ni/CeO 2–x(111). At 700 K, under methane dry reforming conditions, no signals for adsorbed CH x or C species are detected in the C1s XPS region. As a result, the reforming of methane proceeds in a clean and efficient way.« less

Assessment of different pre-treatment methods for the removal of limonene in citrus waste and their effect on methane potential and methane production rate.

PubMed

Ruiz, Begoña; de Benito, Amparo; Rivera, José Daniel; Flotats, Xavier

2016-12-01

The objective of this study was to assess the limonene removal efficiency of three pre-treatment methods when applied to citrus waste and to evaluate their effects on the biochemical methane potential and the methane production rate using batch anaerobic tests. The methods tested were based on removal (biological pretreatment by fungi) or recovery (steam distillation and ethanol extraction) of limonene. All the treatments decreased the concentration of limonene in orange peel, with average efficiencies of 22%, 44% and 100% for the biological treatment, steam distillation and ethanol extraction, respectively. By-products from limonene biodegradation by fungi exhibited an inhibitory effect also, not making interesting the biological pretreatment. The methane potential and production rate of the treated orange peel increased significantly after applying the recovery strategies, which separated and recovered simultaneously other inhibitory components of the citrus essential oil. Apart from the high recovery efficiency of the ethanol extraction process, it presented a favourable energy balance. © The Author(s) 2016.

Methods for applying microchannels to separate methane using liquid absorbents, especially ionic liquid absorbents from a mixture comprising methane and nitrogen

DOEpatents

Tonkovich, Anna Lee Y [Dublin, OH; Litt, Robert D [Westerville, OH; Dongming, Qiu [Dublin, OH; Silva, Laura J [Plain City, OH; Lamont, Micheal Jay [Plain City, OH; Fanelli, Maddalena [Plain City, OH; Simmons, Wayne W [Plain city, OH; Perry, Steven [Galloway, OH

2011-10-04

Methods of using microchannel separation systems including absorbents to improve thermal efficiency and reduce parasitic power loss. Energy is typically added to desorb methane and then energy or heat is removed to absorb methane using a working solution. The working solution or absorbent may comprise an ionic liquid, or other fluids that demonstrate a difference in affinity between methane and nitrogen in a solution.

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.

Factors influencing the stable carbon isotopic signature of methane from combustion and biomass burning

NASA Astrophysics Data System (ADS)

Chanton, Jeffrey P.; Rutkowski, Christine M.; Schwartz, Candace C.; Ward, Darold E.; Boring, Lindsay

2000-01-01

Factors controlling the δ13C of methane released by combustion include the combustion efficiency of the fire and the δ13C of the fuel. Smoldering fires produced 13C-depleted methane relative to hot, flaming fires in controlled forest and grassland burns and within a wood stove. Pine forest burns in the southeastern United States produced methane which ranged from -21 to -30‰, while African grassland burns varied from -17 to -26‰, depending upon combustion phase. African woodland burns produced methane at -30‰. In forest burns in the southeastern United States, the δ13C of methane released with smoldering was significantly 13C depleted relative to methane released under hot flaming conditions. Methane released with smoldering was depleted by 2-3‰ relative to the fuel δ13C, but this difference was not significant. The δ13C of methane produced in a variety of wood stove conditions varied from -9 to -25‰ and also depended upon combustion efficiency. Similar results were found for methane produced by gasoline automobile engines, where the δ13C of methane varied from -9 to -22‰. For combustion occurring within the confining chamber of a wood stove or engine the δ13C of methane was clearly 13C enriched relative to the δ13C of the fuel, possibly because of preferential combustion of 12CH4 in the gas phase. Significant quantities of ethylene (up to 25 to 50% of methane concentrations) were produced in southeastern U.S. forest fires, which may have consequences for physiological and reproductive responses of plants in the ecosystem. Methane production in these fires varied from 0.2 to 8.5% of the carbon dioxide production.

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

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

NASA Astrophysics Data System (ADS)

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

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

Evaluating 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.

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

PubMed

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

2011-03-01

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

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.

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.

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.

40 CFR 63.1426 - Process vent requirements for determining organic HAP concentration, control efficiency, and...

Code of Federal Regulations, 2014 CFR

2014-07-01

... Production § 63.1426 Process vent requirements for determining organic HAP concentration, control efficiency..., total organic HAP, or as TOC minus methane and ethane according to the procedures specified. When... methane and ethane) concentrations in all process vent streams and primary and secondary fuels introduced...

40 CFR 60.565 - Reporting and recordkeeping requirements.

Code of Federal Regulations, 2014 CFR

2014-07-01

... emission control efficiency of a combustion device or the outlet concentration of TOC (minus methane and... performance test period, and (ii) The percent reduction of TOC (minus methane and ethane) achieved by the incinerator, the concentration of TOC (minus methane and ethane) (ppmv, by compound) at the outlet of the...

Relationship between selection for feed efficiency and methane production

USDA-ARS?s Scientific Manuscript database

Enteric methane is a product of fermentation in the gastro-intestinal tract of ruminants. A group of archaea bacteria collectively called “methanogens” are responsible for the synthesis of methane. In ruminants, the methanogens grow in the reticulum-rumen complex and in the cecum. Most of the met...

40 CFR 60.565 - Reporting and recordkeeping requirements.

Code of Federal Regulations, 2010 CFR

2010-07-01

... emission control efficiency of a combustion device or the outlet concentration of TOC (minus methane and... performance test period, and (ii) The percent reduction of TOC (minus methane and ethane) achieved by the incinerator, the concentration of TOC (minus methane and ethane) (ppmv, by compound) at the outlet of the...

40 CFR 60.565 - Reporting and recordkeeping requirements.

Code of Federal Regulations, 2012 CFR

2012-07-01

... emission control efficiency of a combustion device or the outlet concentration of TOC (minus methane and... performance test period, and (ii) The percent reduction of TOC (minus methane and ethane) achieved by the incinerator, the concentration of TOC (minus methane and ethane) (ppmv, by compound) at the outlet of the...

40 CFR 60.565 - Reporting and recordkeeping requirements.

Code of Federal Regulations, 2011 CFR

2011-07-01

... emission control efficiency of a combustion device or the outlet concentration of TOC (minus methane and... performance test period, and (ii) The percent reduction of TOC (minus methane and ethane) achieved by the incinerator, the concentration of TOC (minus methane and ethane) (ppmv, by compound) at the outlet of the...

40 CFR 60.565 - Reporting and recordkeeping requirements.

Code of Federal Regulations, 2013 CFR

2013-07-01

... emission control efficiency of a combustion device or the outlet concentration of TOC (minus methane and... performance test period, and (ii) The percent reduction of TOC (minus methane and ethane) achieved by the incinerator, the concentration of TOC (minus methane and ethane) (ppmv, by compound) at the outlet of the...

Methane biofiltration in the presence of ethanol vapor under steady and transient state conditions: an experimental study.

PubMed

Ferdowsi, Milad; Ramirez, Antonio Avalos; Jones, Joseph Peter; Heitz, Michèle

2017-09-01

Methane (CH 4 ) removal in the presence of ethanol vapors was performed by a stone-based bed and a hybrid packing biofilter in parallel. In the absence of ethanol, a methane removal efficiency of 55 ± 1% was obtained for both biofilters under similar CH 4 inlet load (IL) of 13 ± 0.5 g CH4  m -3  h -1 and an empty bed residence time (EBRT) of 6 min. The results proved the key role of the bottom section in both biofilters for simultaneous removal of CH 4 and ethanol. Ethanol vapor was completely eliminated in the bottom sections for an ethanol IL variation between 1 and 11 g ethanol  m -3  h -1 . Ethanol absorption and accumulation in the biofilm phase as well as ethanol conversion to CO 2 contributed to ethanol removal efficiency of 100%. In the presence of ethanol vapor, CO 2 productions in the bottom section increased almost fourfold in both biofilters. The ethanol concentration in the leachate of the biofilter exceeding 2200 g ethanol  m -3 leachate in both biofilters demonstrated the excess accumulation of ethanol in the biofilm phase. The biofilters responded quickly to an ethanol shock load followed by a starvation with 20% decrease of their performance. The return to normal operations in both biofilters after the transient conditions took less than 5 days. Unlike the hybrid packing biofilter, excess pressure drop (up to 1.9 cmH 2 O m -1 ) was an important concern for the stone bed biofilter. The biomass accumulation in the bottom section of the stone bed biofilter contributed to 80% of the total pressure drop. However, the 14-day starvation reduced the pressure drop to 0.25 cmH 2 O m -1 .

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...

Evaluation of the impact of organic material on the anaerobic methane and ammonium removal in a membrane aerated biofilm reactor (MABR) based on the multispecies biofilm modeling.

PubMed

Wu, Jun; Zhang, Yue

2017-01-01

The simultaneous nitrogen and methane removal by the combined nitritation, anaerobic ammonium oxidation (anammox), and nitrite dependent anaerobic methane oxidation (n-damo) processes in the membrane aerated biofilm reactor (MABR) offers clear advantages in term of energy saving and greenhouse gas emission mitigation. The rejected water from sludge digestion usually contained high ammonium, COD, and dissolved methane. The impact of influent COD on the anaerobic methane and ammonium removal in an MABR was evaluated in the model based study. The results indicated that the influent COD did not reduce the methane and ammonium removal efficiency at C/N ratio (influent COD/NH 4 + -N) less than 0.1. At high C/N ratio, the oxygen transfer coefficient needed to be increased to achieve high methane and nitrogen removal. Substrate flux analysis indicated that heterotrophic denitrification in the outside layer of biofilm reduced the impact of influent COD. Heterotrophic growth needed to be limited at the outside layer by using NO 3 - as electron acceptor; otherwise, the heterotrophic bacteria would compete NO 2 - and space with anammox and n-damo bacteria in the inner layers and reduce the nitrogen and methane removal efficiency.

Significance of dissolved methane in effluents of anaerobically ...

EPA Pesticide Factsheets

The need for energy efficient Domestic Wastewater (DWW) treatment is increasing annually with population growth and expanding global energy demand. Anaerobic treatment of low strength DWW produces methane which can be used to as an energy product. Temperature sensitivity, low removal efficiencies (Chemical Oxygen Demand (COD), Suspended Solids (SS), and Nutrients), alkalinity demand, and potential greenhouse gas (GHG) emissions have limited its application to warmer climates. Although well designed anaerobic Membrane Bioreactors (AnMBRs) are able to effectively treat DWW at psychrophilic temperatures (10–30 °C), lower temperatures increase methane solubility leading to increased energy losses in the form of dissolved methane in the effluent. Estimates of dissolved methane losses are typically based on concentrations calculated using Henry's Law but advection limitations can lead to supersaturation of methane between 1.34 and 6.9 times equilibrium concentrations and 11–100% of generated methane being lost in the effluent. In well mixed systems such as AnMBRs which use biogas sparging to control membrane fouling, actual concentrations approach equilibrium values. Non-porous membranes have been used to recover up to 92.6% of dissolved methane and well suited for degassing effluents of Upflow Anaerobic Sludge Blanket (UASB) reactors which have considerable solids and organic contents and can cause pore wetting and clogging in microporous membrane modules. Micro

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.

Improvement of gaseous energy recovery from sugarcane bagasse by dark fermentation followed by biomethanation process.

PubMed

Kumari, Sinu; Das, Debabrata

2015-10-01

The aim of the present study was to enhance the gaseous energy recovery from sugarcane bagasse. The two stage (biohydrogen and biomethanation) batch process was considered under mesophilic condition. Alkali pretreatment (ALP) was used to remove lignin from sugarcane bagasse. This enhanced the enzymatic digestibility of bagasse to a great extent. The maximum lignin removal of 60% w/w was achieved at 0.25 N NaOH concentration (50°C, 30 min). The enzymatic hydrolysis efficiency was increased to about 2.6-folds with alkali pretreated sugarcane bagasse as compared to untreated one. The maximum hydrogen and methane yields from the treated sugarcane bagasse by biohydrogen and biomethanation processes were 93.4 mL/g-VS and 221.8 mL/g-VS respectively. This process resulted in significant increase in energy conversion efficiency (44.8%) as compared to single stage hydrogen production process (5.4%). Copyright © 2015 Elsevier Ltd. All rights reserved.

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.

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.

Improving methane production from digested manure biofibers by mechanical and thermal alkaline pretreatment.

PubMed

Tsapekos, P; Kougias, Panagiotis G; Frison, A; Raga, R; Angelidaki, I

2016-09-01

Animal manure digestion is associated with limited methane production, due to the high content in fibers, which are hardly degradable lignocellulosic compounds. In this study, different mechanical and thermal alkaline pretreatment methods were applied to partially degradable fibers, separated from the effluent stream of biogas reactors. Batch and continuous experiments were conducted to evaluate the efficiency of these pretreatments. In batch experiments, the mechanical pretreatment improved the degradability up to 45%. Even higher efficiency was shown by applying thermal alkaline pretreatments, enhancing fibers degradability by more than 4-fold. In continuous experiments, the thermal alkaline pretreatment, using 6% NaOH at 55°C was proven to be the most efficient pretreatment method as the methane production was increased by 26%. The findings demonstrated that the methane production of the biogas plants can be increased by further exploiting the fraction of the digested manure fibers which are discarded in the post-storage tank. Copyright © 2016 Elsevier Ltd. All rights reserved.

Natural Gas STAR Program

EPA Pesticide Factsheets

EPA’s Voluntary Methane Programs encourage oil and natural gas companies to adopt cost-effective technologies and practices that improve operational efficiency and reduce emissions of methane, a potent greenhouse gas.

40 CFR 60.614 - Test methods and procedures.

Code of Federal Regulations, 2012 CFR

2012-07-01

... or TOC (less methane and ethane) reduction efficiency shall be prior to the inlet of the control... TOC (minus methane and ethane), dry basis, ppm by volume. %O2d=Concentration of O2, dry basis, percent.... (ii) The emission reduction (R) of TOC (minus methane and ethane) shall be determined using the...

40 CFR 60.664 - Test methods and procedures.

Code of Federal Regulations, 2012 CFR

2012-07-01

... (less methane and ethane) reduction efficiency shall be prior to the inlet of the control device and... methane and ethane), dry basis, ppm by volume. %O2d=Concentration of O2, dry basis, percent by volume. (4... emission reduction (R) of TOC (minus methane and ethane) shall be determined using the following equation...

Anaerobic digestion of thermal-alkaline-pretreated cephalosporin bacterial residues for methane production.

PubMed

Li, Guixia; Zhong, Weizhang; Wang, Rui; Chen, Jiaqi; Li, Zaixing

2017-08-01

Optimum anaerobic conditions of cephalosporin bacterial residues after thermal-alkaline pretreatment were determined by orthogonal experiments. And through biochemical methane potential tests (BMPs) for cephalosporin bacterial residues, the ability for bacterial degradation of cephalosporin was also evaluated. The thermal-alkaline pretreatment with the optimum values of 6% NaOH at 105 °C for 15 min significantly improved digestion performance. With the thermal-alkaline pretreatment, the specific methane yield of the pretreated cephalosporin bacterial residue increased by 254.79% compared with that of the un-pretreated cephalosporin bacterial residue. The results showed that anaerobic digestion of thermal-alkaline-pretreated cephalosporin bacterial residues could be one of the options for efficient methane production and waste treatment. This work investigates the thermal-alkaline pretreatment of cephalosporin bacterial residues, which can increase their methane yield by 254.79% compared with no pretreatment. The digestion performance is significantly improved under the condition of 6% NaOH at 105 °C for 15 min. The results show that anaerobic digestion of thermal-alkaline-pretreated cephalosporin bacterial residues could be one of the options for efficient methane production and waste treatment.

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

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.

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

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

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.

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.

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.

Plasma technology - a novel solution for CO2 conversion?

PubMed

Snoeckx, Ramses; Bogaerts, Annemie

2017-10-02

CO 2 conversion into value-added chemicals and fuels is considered as one of the great challenges of the 21st century. Due to the limitations of the traditional thermal approaches, several novel technologies are being developed. One promising approach in this field, which has received little attention to date, is plasma technology. Its advantages include mild operating conditions, easy upscaling, and gas activation by energetic electrons instead of heat. This allows thermodynamically difficult reactions, such as CO 2 splitting and the dry reformation of methane, to occur with reasonable energy cost. In this review, after exploring the traditional thermal approaches, we have provided a brief overview of the fierce competition between various novel approaches in a quest to find the most effective and efficient CO 2 conversion technology. This is needed to critically assess whether plasma technology can be successful in an already crowded arena. The following questions need to be answered in this regard: are there key advantages to using plasma technology over other novel approaches, and if so, what is the flip side to the use of this technology? Can plasma technology be successful on its own, or can synergies be achieved by combining it with other technologies? To answer these specific questions and to evaluate the potentials and limitations of plasma technology in general, this review presents the current state-of-the-art and a critical assessment of plasma-based CO 2 conversion, as well as the future challenges for its practical implementation.

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

PubMed

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

2018-05-01

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

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

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.

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

Seeking key microorganisms for enhancing methane production in anaerobic digestion of waste sewage sludge.

PubMed

Mustapha, Nurul Asyifah; Hu, Anyi; Yu, Chang-Ping; Sharuddin, Siti Suhailah; Ramli, Norhayati; Shirai, Yoshihito; Maeda, Toshinari

2018-06-01

Efficient approaches for the utilization of waste sewage sludge have been widely studied. One of them is to use it for the bioenergy production, specifically methane gas which is well-known to be driven by complex bacterial interactions during the anaerobic digestion process. Therefore, it is important to understand not only microorganisms for producing methane but also those for controlling or regulating the process. In this study, azithromycin analogs belonging to macrolide, ketolide, and lincosamide groups were applied to investigate the mechanisms and dynamics of bacterial community in waste sewage sludge for methane production. The stages of anaerobic digestion process were evaluated by measuring the production of intermediate substrates, such as protease activity, organic acids, the quantification of bacteria and archaea, and its community dynamics. All azithromycin analogs used in this study achieved a high methane production compared to the control sample without any antibiotic due to the efficient hydrolysis process and the presence of important fermentative bacteria and archaea responsible in the methanogenesis stage. The key microorganisms contributing to the methane production may be Clostridia, Cladilinea, Planctomycetes, and Alphaproteobacteria as an accelerator whereas Nitrosomonadaceae and Nitrospiraceae may be suppressors for methane production. In conclusion, the utilization of antibiotic analogs of macrolide, ketolide, and lincosamide groups has a promising ability in finding the essential microorganisms and improving the methane production using waste sewage sludge.

Methanosarcinaceae and Acetate-Oxidizing Pathways Dominate in High-Rate Thermophilic Anaerobic Digestion of Waste-Activated Sludge

PubMed Central

Ho, Dang P.; Jensen, Paul D.

2013-01-01

This study investigated the process of high-rate, high-temperature methanogenesis to enable very-high-volume loading during anaerobic digestion of waste-activated sludge. Reducing the hydraulic retention time (HRT) from 15 to 20 days in mesophilic digestion down to 3 days was achievable at a thermophilic temperature (55°C) with stable digester performance and methanogenic activity. A volatile solids (VS) destruction efficiency of 33 to 35% was achieved on waste-activated sludge, comparable to that obtained via mesophilic processes with low organic acid levels (<200 mg/liter chemical oxygen demand [COD]). Methane yield (VS basis) was 150 to 180 liters of CH4/kg of VSadded. According to 16S rRNA pyrotag sequencing and fluorescence in situ hybridization (FISH), the methanogenic community was dominated by members of the Methanosarcinaceae, which have a high level of metabolic capability, including acetoclastic and hydrogenotrophic methanogenesis. Loss of function at an HRT of 2 days was accompanied by a loss of the methanogens, according to pyrotag sequencing. The two acetate conversion pathways, namely, acetoclastic methanogenesis and syntrophic acetate oxidation, were quantified by stable carbon isotope ratio mass spectrometry. The results showed that the majority of methane was generated by nonacetoclastic pathways, both in the reactors and in off-line batch tests, confirming that syntrophic acetate oxidation is a key pathway at elevated temperatures. The proportion of methane due to acetate cleavage increased later in the batch, and it is likely that stable oxidation in the continuous reactor was maintained by application of the consistently low retention time. PMID:23956388

Comparison of various microbial inocula for the efficient anaerobic digestion of Laminaria hyperborea.

PubMed

Sutherland, Alastair D; Varela, Joao C

2014-01-23

The hydrolysis of seaweed polysaccharides is the rate limiting step in anaerobic digestion (AD) of seaweeds. Seven different microbial inocula and a mixture of these (inoculum 8) were therefore compared in triplicate, each grown over four weeks in static culture for the ability to degrade Laminaria hyperborea seaweed and produce methane through AD. All the inocula could degrade L. hyperborea and produce methane to some extent. However, an inoculum of slurry from a human sewage anaerobic digester, one of rumen contents from seaweed-eating North Ronaldsay sheep and inoculum 8 used most seaweed volatile solids (VS) (means ranged between 59 and 68% used), suggesting that these each had efficient seaweed polysaccharide digesting bacteria. The human sewage inoculum, an inoculum of anaerobic marine mud mixed with rotting seaweed and inoculum 8 all developed to give higher volumes of methane (means between 41 and 62.5 ml g-1 of seaweed VS by week four) ,compared to other inocula (means between 3.5 and 27.5 ml g-1 VS). Inoculum 8 also gave the highest acetate production (6.5 mmol g-1 VS) in a single-stage fermenter AD system and produced most methane (8.4 mL mmol acetate-1) in phase II of a two-stage AD system. Overall inoculum 8 was found to be the most efficient inoculum for AD of seaweed. The study therefore showed that selection and inclusion of efficient polysaccharide hydrolysing bacteria and methanogenic archaea in an inoculum offer increased methane productivity in AD of L. hyperborea. This inoculum will now being tested in larger scale (10L) continuously stirred reactors optimised for feed rate and retention time to determine maximum methane production under single-stage and two-stage AD systems.

Comparison of various microbial inocula for the efficient anaerobic digestion of Laminaria hyperborea

PubMed Central

2014-01-01

Background The hydrolysis of seaweed polysaccharides is the rate limiting step in anaerobic digestion (AD) of seaweeds. Seven different microbial inocula and a mixture of these (inoculum 8) were therefore compared in triplicate, each grown over four weeks in static culture for the ability to degrade Laminaria hyperborea seaweed and produce methane through AD. Results All the inocula could degrade L. hyperborea and produce methane to some extent. However, an inoculum of slurry from a human sewage anaerobic digester, one of rumen contents from seaweed-eating North Ronaldsay sheep and inoculum 8 used most seaweed volatile solids (VS) (means ranged between 59 and 68% used), suggesting that these each had efficient seaweed polysaccharide digesting bacteria. The human sewage inoculum, an inoculum of anaerobic marine mud mixed with rotting seaweed and inoculum 8 all developed to give higher volumes of methane (means between 41 and 62.5 ml g-1 of seaweed VS by week four) ,compared to other inocula (means between 3.5 and 27.5 ml g-1 VS). Inoculum 8 also gave the highest acetate production (6.5 mmol g-1 VS) in a single-stage fermenter AD system and produced most methane (8.4 mL mmol acetate-1) in phase II of a two-stage AD system. Conclusions Overall inoculum 8 was found to be the most efficient inoculum for AD of seaweed. The study therefore showed that selection and inclusion of efficient polysaccharide hydrolysing bacteria and methanogenic archaea in an inoculum offer increased methane productivity in AD of L. hyperborea. This inoculum will now being tested in larger scale (10L) continuously stirred reactors optimised for feed rate and retention time to determine maximum methane production under single-stage and two-stage AD systems. PMID:24456825

The effect of harvest time, dry matter content and mechanical pretreatments on anaerobic digestion and enzymatic hydrolysis of miscanthus.

PubMed

Frydendal-Nielsen, Susanne; Hjorth, Maibritt; Baby, Sanmohan; Felby, Claus; Jørgensen, Uffe; Gislum, René

2016-10-01

Miscanthus x giganteus was harvested as both green and mature biomass and the dry matter content of the driest harvest was artificially decreased by adding water in two subsamples, giving a total of five dry matter contents. All five biomass types were mechanically pretreated by roller-milling, extrusion or grinding and accumulated methane production and enzymatically-accessible sugars were measured. Accumulated methane production was studied using sigmoid curves that allowed comparison among the treatments of the rate of the methane production and ultimate methane yield. The green biomass gave the highest methane yield and highest levels of enzymatically-accessible cellulose. The driest biomass gave the best effect from extrusion but with the highest energy consumption, whereas roller-milling was most efficient on wet biomass. The addition of water to the last harvest improved the effect of roller-milling and equalled extrusion of the samples in efficiency. Copyright © 2016 Elsevier Ltd. All rights reserved.

RNAi Knock-Down of LHCBM1, 2 and 3 Increases Photosynthetic H2 Production Efficiency of the Green Alga Chlamydomonas reinhardtii

PubMed Central

Oey, Melanie; Ross, Ian L.; Stephens, Evan; Steinbeck, Janina; Wolf, Juliane; Radzun, Khairul Adzfa; Kügler, Johannes; Ringsmuth, Andrew K.; Kruse, Olaf; Hankamer, Ben

2013-01-01

Single cell green algae (microalgae) are rapidly emerging as a platform for the production of sustainable fuels. Solar-driven H2 production from H2O theoretically provides the highest-efficiency route to fuel production in microalgae. This is because the H2-producing hydrogenase (HYDA) is directly coupled to the photosynthetic electron transport chain, thereby eliminating downstream energetic losses associated with the synthesis of carbohydrate and oils (feedstocks for methane, ethanol and oil-based fuels). Here we report the simultaneous knock-down of three light-harvesting complex proteins (LHCMB1, 2 and 3) in the high H2-producing Chlamydomonas reinhardtii mutant Stm6Glc4 using an RNAi triple knock-down strategy. The resultant Stm6Glc4L01 mutant exhibited a light green phenotype, reduced expression of LHCBM1 (20.6% ±0.27%), LHCBM2 (81.2% ±0.037%) and LHCBM3 (41.4% ±0.05%) compared to 100% control levels, and improved light to H2 (180%) and biomass (165%) conversion efficiencies. The improved H2 production efficiency was achieved at increased solar flux densities (450 instead of ∼100 µE m−2 s−1) and high cell densities which are best suited for microalgae production as light is ideally the limiting factor. Our data suggests that the overall improved photon-to-H2 conversion efficiency is due to: 1) reduced loss of absorbed energy by non-photochemical quenching (fluorescence and heat losses) near the photobioreactor surface; 2) improved light distribution in the reactor; 3) reduced photoinhibition; 4) early onset of HYDA expression and 5) reduction of O2-induced inhibition of HYDA. The Stm6Glc4L01 phenotype therefore provides important insights for the development of high-efficiency photobiological H2 production systems. PMID:23613840

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.

An introduction of CO₂ conversion by dry reforming with methane and new route of low-temperature methanol synthesis.

PubMed

Shi, Lei; Yang, Guohui; Tao, Kai; Yoneyama, Yoshiharu; Tan, Yisheng; Tsubaki, Noritatsu

2013-08-20

Carbon dioxide is one of the highest contributors to the greenhouse effect, as well as a cheap and nontoxic building block for single carbon source chemistry. As such, CO₂ conversion is one of most important research areas in energy and environment sciences, as well as in catalysis technology. For chemical conversion of CO₂, natural gas (mainly CH₄) is a promising counterpart molecule to the CO₂-related reaction, due to its high availability and low price. More importantly, being able to convert CH₄ to useful fuels and molecules is advantageous, because it is also a kind of "greenhouse effect" gas, and can be an energy alternative to petroleum oil. In this Account, we discuss our development of efficient catalysts with precisely designed nanostructure for CO₂ reforming of CH₄ to produce syngas (mixture of CO and H₂), which can then be converted to many chemicals and energy products. This new production flow can establish a GTL (gas-to-liquid) industry, being currently pushed by the shale gas revolution. From the viewpoint of GTL industry, developing a catalyst for CO₂ reforming of CH₄ is a challenge, because they need a very high production rate to make the huge GTL methane reformer as small as possible. In addition, since both CO₂ and CH₄ give off carbon deposits that deactivate non-precious metallic catalysts very quickly, the total design of catalyst support and supported metallic nanoparticles is necessary. We present a simple but useful method to prepare bimodal catalyst support, where small pores are formed inside large ones during the self-organization of nanoparticles from solution. Large pores enhance the mass transfer rate, while small pores provide large surface areas to disperse active metallic nanoparticles. More importantly, building materials for small pores can also be used as promoters or cocatalysts to further enhance the total activity and stability. Produced syngas from methane reforming is generally catalytically converted in situ via one of two main routes. The first is to use Fischer-Tropsch synthesis (FTS), a process that catalytically converts syngas to hydrocarbons of varying molecular weights. The second is methanol synthesis. The latter has better atomic economy, since the oxygen atom in CO is included in the product and CO₂ can be blended into syngas as a reactant. However, production of methanol is very inefficient in this reaction: only 10-15% one-pass conversion typically at 5.0-10.0 MPa and 523-573 K, due to the severe thermodynamic limitations of this exothermal reaction (CO + 2H₂ = CH₃OH). In this Account, we propose and develop a new route of low-temperature methanol synthesis from CO₂-containing syngas only by adding alcohols, including methanol itself. These alcohols act as homogeneous cocatalysts and the solvent, realizing 70-100% one-pass conversion at only 5.0 MPa and 443 K. The key step is the reaction of the adsorbed formate species with alcohols to yield ester species at low temperatures, followed by the hydrogenation of ester by hydrogen atoms on metallic Cu. This changes the normal reaction path of conventional, high-temperature methanol synthesis from formate via methoxy to methanol.

Nitrogen oxides and methane treatment by non-thermal plasma

NASA Astrophysics Data System (ADS)

Alva, E.; Pacheco, M.; Colín, A.; Sánchez, V.; Pacheco, J.; Valdivia, R.; Soria, G.

2015-03-01

Non thermal plasma was used to treat nitrogen oxides (NOx) and methane (CH4), since they are important constituents of hydrocarbon combustion emissions processes and, both gases, play a key role in the formation of tropospheric ozone. These gases are involved in environmental problems like acid rain and some diseases such as bronchitis and pneumonia. In the case of methane is widely known its importance in the global climate change, and currently accounts for 30% of global warming. There is a growing concern for methane leaks, associated with a rapid expansion of unconventional oil and gas extraction techniques as well as a large-scale methane release from Arctic because of ice melting and the subsequent methane production of decaying organic matter. Therefore, methane mitigation is a key to avoid dangerous levels of global warming. The research, here reported, deals about the generation of non-thermal plasma with a double dielectric barrier (2DBD) at atmospheric pressure with alternating current (AC) for NOx and CH4 treatment. The degradation efficiencies and their respective power consumption for different reactor configurations (cylindrical and planar) are also reported. Qualitative and quantitative analysis of gases degradation are reported before and after treatment with cold plasma. Experimental and theoretical results are compared obtaining good removal efficiencies, superior to 90% and to 20% respectively for NOx and CH4.

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.

Anaerobic biodegradation of aircraft deicing fluid in UASB reactors.

PubMed

Tham, P T Pham thi; Kennedy, K J Kevin J

2004-05-01

A central composite design was employed to methodically investigate anaerobic treatment of aircraft deicing fluid (ADF) in bench-scale Upflow Anaerobic Sludge Blanket (UASB) reactors. A total of 23 runs at 17 different operating conditions (0.8% 1.6% ADF (6000-12,000mg/L COD), 12-56h HRT, and 18-36gVSS/L) were conducted in continuous mode. The development of four empirical models describing process responses (i.e. COD removal efficiency, biomass-specific acetoclastic activity, methane production rate, and methane production potential) as functions of ADF concentration, hydraulic retention time, and biomass concentration is presented. Model verification indicated that predicted responses (COD removal efficiencies, biomass-specific acetoclastic activity, and methane production rates and potential) were in good agreement with experimental results. Biomass-specific acetoclastic activity was improved two-fold from 0.23gCOD/gVSS/d for inoculum to a maximum of 0.55gCOD/gVSS/d during ADF treatment in UASB reactors. For the design window, COD removal efficiencies were higher than 90%. The predicted methane production potentials were close to theoretical values, and methane production rates increased as the organic loading rate is increased. ADF toxicity effects were evident for 1.6% ADF at medium organic loadings (SOLR above 0.5gCOD/gVSS/d). In contrast, good reactor stability and excellent COD removal efficiencies were achieved at 1.2% ADF for reactor loadings approaching that of highly loaded systems (0.73gCOD/gVSS/d).

Methane production by anaerobic digestion of water hyacinth (Eichhornia crassipes)

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

Klass, D.L.; Ghosh, S.

1980-01-01

Water hyacinth under conventional high-rate digestion conditions exhibited higher methane yields and energy recovery efficiencies when grown in sewage-fed lagoons as compared to the corresponding values obtained with water hyacinth grown in a fresh-water pond. Mesophilic digestion provided the highest feed energy recovered in the product gas as methane while thermophilic digestion, when operated at sufficiently high loading rates and reduced detention times, gave the highest specific methane production rates. Methane yields, volatile solids reduction, and energy recovery as methane for the sewage-grown water hyacinth were in the same range as those observed for other biomass substrates when digested undermore » similar conditions.« 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.

On the relevance of the methane oxidation cycle to ozone hole chemistry

NASA Technical Reports Server (NTRS)

Mueller, Rolf; Crutzen, Paul J.

1994-01-01

High concentrations of active chlorine are clearly responsible for the observed ozone depletion during the Antarctic polar spring. However, the mechanism behind the activation of chlorine from the reservoirs species HCl and ClONO2 and the maintenance of extremely high levels of active chlorine after polar sunrise is less well understood. Here, we focus on the influence of the methane oxidation cycle on 'ozone hole' chemistry through its effect on HOx and ClOx radicals. We demonstrate the great potential importance of the heterogeneous reaction HCl + HOCl yields Cl2 + H2O and the gasphase reaction ClO + CH3O2 yields ClOO + CH3O under sunlight conditions in polar spring. Under these conditions, the heterogeneous reaction is the main sink for HOx radicals. Through this channel, the HCl reservoir may be almost completely depleted. The gas phase reaction may control the levels of the CH3O2 radical, provided that high levels of ClO exist. Otherwise this radical initiates a sequence of reactions leading to a considerable loss of active chlorine. Moreover, the production of HOx radicals is reduced, and thereby the efficiency of the heterogeneous reaction limited. The two reactions together may accomplish the complete conversion of HCl into active chlorine, thereby leading to a rapid destruction of ozone.

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.

In vitro-in vivo study on the effects of plant compounds on rumen fermentation, microbial abundances and methane emissions in goats.

PubMed

Martínez-Fernández, G; Abecia, L; Martín-García, A I; Ramos-Morales, E; Hervás, G; Molina-Alcaide, E; Yáñez-Ruiz, D R

2013-12-01

Two in vitro and one in vivo experiments were conducted to investigate the effects of a selection of plant compounds on rumen fermentation, microbial concentration and methane emissions in goats. Treatments were: control (no additive), carvacrol (CAR), cinnamaldehyde (CIN), eugenol (EUG), propyl propane thiosulfinate (PTS), propyl propane thiosulfonate (PTSO), diallyl disulfide (DDS), a mixture (40 : 60) of PTS and PTSO (PTS+PTSO), and bromochloromethane (BCM) as positive control with proven antimethanogenic effectiveness. Four doses (40, 80, 160 and 320 µl/l) of the different compounds were incubated in vitro for 24 h in diluted rumen fluid from goats using two diets differing in starch and protein source within the concentrate (Experiment 1).The total gas production was linearly decreased (P<0.012) by all compounds, with the exception of EUG and PTS+PTSO (P≥ 0.366). Total volatile fatty-acid (VFA) concentration decreased (P≤ 0.018) only with PTS, PTSO and CAR, whereas the acetate:propionate ratio decreased (P≤ 0.002) with PTS, PTSO and BCM, and a tendency (P=0.064) was observed for DDS. On the basis of results from Experiment 1, two doses of PTS, CAR, CIN, BCM (160 and 320 µl/l), PTSO (40 and 160 µl/l) and DDS (80 and 320 µl/l) were further tested in vitro for 72 h (Experiment 2). The gas production kinetics were affected (P≤ 0.045) by all compounds, and digested NDF (DNDF) after 72 h of incubation was only linearly decreased (P≤ 0.004) by CAR and PTS. The addition of all compounds linearly decreased (P≤ 0.009) methane production, although the greatest reductions were observed for PTS (up to 96%), DDS (62%) and BCM (95%). No diet-dose interaction was observed. To further test the results obtained in vitro, two groups of 16 adult non-pregnant goats were used to study in vivo the effect of adding PTS (50, 100 and 200 mg/l rumen content per day) and BCM (50, 100 and 160 mg/l rumen content per day) during the 9 days on methane emissions (Experiment 3). The addition of PTS and BCM resulted in linear reductions (33% and 64%, respectively, P≤ 0.002) of methane production per unit of dry matter intake, which were lower than the maximum inhibition observed in vitro (87% and 96%, respectively). We conclude that applying the same doses in vivo as in vitro resulted in a proportional lower extent of methane decrease, and that PTS at 200 mg/l rumen content per day has the potential to reduce methane emissions in goats. Whether the reduction in methane emission observed in vivo persists over longer periods of treatments and improves feed conversion efficiency requires further research.

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.

Density-Functional Theory with Dispersion-Correcting Potentials for Methane: Bridging the Efficiency and Accuracy Gap between High-Level Wave Function and Classical Molecular Mechanics Methods.

PubMed

Torres, Edmanuel; DiLabio, Gino A

2013-08-13

Large clusters of noncovalently bonded molecules can only be efficiently modeled by classical mechanics simulations. One prominent challenge associated with this approach is obtaining force-field parameters that accurately describe noncovalent interactions. High-level correlated wave function methods, such as CCSD(T), are capable of correctly predicting noncovalent interactions, and are widely used to produce reference data. However, high-level correlated methods are generally too computationally costly to generate the critical reference data required for good force-field parameter development. In this work we present an approach to generate Lennard-Jones force-field parameters to accurately account for noncovalent interactions. We propose the use of a computational step that is intermediate to CCSD(T) and classical molecular mechanics, that can bridge the accuracy and computational efficiency gap between them, and demonstrate the efficacy of our approach with methane clusters. On the basis of CCSD(T)-level binding energy data for a small set of methane clusters, we develop methane-specific, atom-centered, dispersion-correcting potentials (DCPs) for use with the PBE0 density-functional and 6-31+G(d,p) basis sets. We then use the PBE0-DCP approach to compute a detailed map of the interaction forces associated with the removal of a single methane molecule from a cluster of eight methane molecules and use this map to optimize the Lennard-Jones parameters for methane. The quality of the binding energies obtained by the Lennard-Jones parameters we obtained is assessed on a set of methane clusters containing from 2 to 40 molecules. Our Lennard-Jones parameters, used in combination with the intramolecular parameters of the CHARMM force field, are found to closely reproduce the results of our dispersion-corrected density-functional calculations. The approach outlined can be used to develop Lennard-Jones parameters for any kind of molecular system.

Biogas production of Chicken Manure by Two-stage fermentation process

NASA Astrophysics Data System (ADS)

Liu, Xin Yuan; Wang, Jing Jing; Nie, Jia Min; Wu, Nan; Yang, Fang; Yang, Ren Jie

2018-06-01

This paper performs a batch experiment for pre-acidification treatment and methane production from chicken manure by the two-stage anaerobic fermentation process. Results shows that the acetate was the main component in volatile fatty acids produced at the end of pre-acidification stage, accounting for 68% of the total amount. The daily biogas production experienced three peak period in methane production stage, and the methane content reached 60% in the second period and then slowly reduced to 44.5% in the third period. The cumulative methane production was fitted by modified Gompertz equation, and the kinetic parameters of the methane production potential, the maximum methane production rate and lag phase time were 345.2 ml, 0.948 ml/h and 343.5 h, respectively. The methane yield of 183 ml-CH4/g-VSremoved during the methane production stage and VS removal efficiency of 52.7% for the whole fermentation process were achieved.

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

A review on hydrothermal pre-treatment technologies and environmental profiles of algal biomass processing.

PubMed

Patel, Bhavish; Guo, Miao; Izadpanah, Arash; Shah, Nilay; Hellgardt, Klaus

2016-01-01

The need for efficient and clean biomass conversion technologies has propelled Hydrothermal (HT) processing as a promising treatment option for biofuel production. This manuscript discussed its application for pre-treatment of microalgae biomass to solid (biochar), liquid (biocrude and biodiesel) and gaseous (hydrogen and methane) products via Hydrothermal Carbonisation (HTC), Hydrothermal Liquefaction (HTL) and Supercritical Water Gasification (SCWG) as well as the utility of HT water as an extraction medium and HT Hydrotreatment (HDT) of algal biocrude. In addition, the Solar Energy Retained in Fuel (SERF) using HT technologies is calculated and compared with benchmark biofuel. Lastly, the Life Cycle Assessment (LCA) discusses the limitation of the current state of art as well as introduction to new potential input categories to obtain a detailed environmental profile. Copyright © 2015 Elsevier Ltd. All rights reserved.

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

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.

Influence of methane emissions and vehicle efficiency on the climate implications of heavy-duty natural gas trucks.

PubMed

Camuzeaux, Jonathan R; Alvarez, Ramón A; Brooks, Susanne A; Browne, Joshua B; Sterner, Thomas

2015-06-02

While natural gas produces lower carbon dioxide emissions than diesel during combustion, if enough methane is emitted across the fuel cycle, then switching a heavy-duty truck fleet from diesel to natural gas can produce net climate damages (more radiative forcing) for decades. Using the Technology Warming Potential methodology, we assess the climate implications of a diesel to natural gas switch in heavy-duty trucks. We consider spark ignition (SI) and high-pressure direct injection (HPDI) natural gas engines and compressed and liquefied natural gas. Given uncertainty surrounding several key assumptions and the potential for technology to evolve, results are evaluated for a range of inputs for well-to-pump natural gas loss rates, vehicle efficiency, and pump-to-wheels (in-use) methane emissions. Using reference case assumptions reflecting currently available data, we find that converting heavy-duty truck fleets leads to damages to the climate for several decades: around 70-90 years for the SI cases, and 50 years for the more efficient HPDI. Our range of results indicates that these fuel switches have the potential to produce climate benefits on all time frames, but combinations of significant well-to-wheels methane emissions reductions and natural gas vehicle efficiency improvements would be required.

Engineering Methane and Carbon Dioxide Pathways to Turn Renewable Biogas into Higher-Value Chemicals

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

Greenfield, Derek; Helman, Noah; Clarke, Elizabeth

The United States has a critical need for green manufacturing technologies that can produce a wide range of renewable products at low cost. Industrial Microbes develops biological processes that produce renewable chemicals from organic waste streams. The target chemical for this Phase I project is used to make paints, coatings, and polymers for a multi-billion-dollar market. In addition to the benefits from its green process, the company estimates that the new manufacturing process described here will result in 20-40% cost savings when used at commercial scale. This is possible because the company’s process utilizes waste biogas, an inexpensive feedstock, andmore » is highly efficient: the only byproduct is clean water. For this Phase I project, Industrial Microbes successfully built an enzyme pathway that solves the most difficult challenges of converting biogas into the target chemical. These challenges include the conversion of methane into soluble methanol; the identification of highly-active enzymes; and the production of the target chemical. The company has also completed proof-of-concept by demonstrating that its production strain can utilize raw biogas from a wastewater treatment plant. Achieving these goals required several breakthroughs in transferring enzymes from exotic microorganisms into a commercial one, used commonly for industrial-scale production. In Phase II, Industrial Microbes will work toward commercializing this process by improving carbon efficiency and speed of chemical production. Organic waste streams such as biogas are an underutilized source of renewable carbon and energy; efficient use of such waste streams will reduce the United States’ reliance on petroleum and lower greenhouse gas emissions. The process described here is one of few industrial processes that can convert biogas into commodity products, rather than burning it for energy. If renewable products can be made from biogas economically, companies and governments will find it attractive to collect organic waste streams for biogas production. This can prevent waste from ending up in landfills, where it breaks down into the greenhouse gases methane and carbon dioxide: landfills emit the equivalent greenhouse gases of 35 million cars every year. New uses of biogas will also help lower costs for making carbon-neutral biofuels, since biofuel production also generates waste that can be turned into biogas.« less

Designing and implementing science-based methane policies

NASA Astrophysics Data System (ADS)

George, F.

2017-12-01

The phenomenal growth in shale gas production across the U.S. has significantly improved the energy security and economic prospects of the country. Natural gas is a "versatile" fuel that has application in every major end-use sector of the economy, both as a fuel and a feedstock. Natural gas has also played a significant role in reducing CO2 emissions from the power sector by displacing more carbon intensive fossil fuels. However, emissions of natural gas (predominantly methane) from the wellhead to the burner tip can erode this environmental benefit. Preserving the many benefits of America's natural gas resources requires smart, science-based policies to optimize the energy delivery efficiency of the natural gas supply chain and ensure that natural gas remains a key pillar in our transition to a low-carbon economy. Southwestern Energy (SWN) is the third largest natural gas producer in the United States. Over the last several years, SWN has participated in a number of scientific studies with regulatory agencies, academia and non-governmental entities that have led to over a dozen peer-reviewed papers on methane emissions from oil and gas operations. This presentation will review how our participation in these studies has informed our internal policies and procedures, as well as our external programs, including the ONE Future coalition (ONE Future). In particular, the presentation will highlight the impact of such studies on our Leak Detection and Repair (LDAR) program, designing new methane research and on the ONE Future initiatives - all with the focus of improving the delivery efficiency of oil and gas operations. Our experience supports continued research in the detection and mitigation of methane emissions, with emphasis on longer duration characterization of methane emissions from oil and gas facilities and further development of cost-effective methane detection and mitigation techniques. We conclude from our scientific and operational experiences that a performance-based methane mitigation policy like the ONE Future will lead to more operationally efficient and cost-effective reductions in methane emissions from the natural gas supply chain.

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.

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.

Importance of storage time in mesophilic anaerobic digestion of food waste.

PubMed

Lü, Fan; Xu, Xian; Shao, Liming; He, Pinjing

2016-07-01

Storage was used as a pretreatment to enhance the methanization performance of mesophilic anaerobic digestion of food waste. Food wastes were separately stored for 0, 1, 2, 3, 4, 5, 7, and 12days, and then fed into a methanogenic reactor for a biochemical methane potential (BMP) test lasting up to 60days. Relative to the methane production of food waste stored for 0-1day (285-308mL/g-added volatile solids (VSadded)), that after 2-4days and after 5-12days of storage increased to 418-530 and 618-696mL/g-VSadded, respectively. The efficiency of hydrolysis and acidification of pre-stored food waste in the methanization reactors increased with storage time. The characteristics of stored waste suggest that methane production was not correlated with the total hydrolysis efficiency of organics in pre-stored food waste but was positively correlated with the storage time and acidification level of the waste. From the results, we recommend 5-7days of storage of food waste in anaerobic digestion treatment plants. Copyright © 2016. Published by Elsevier B.V.

Effects of granular activated carbon on methane removal performance and methanotrophic community of a lab-scale bioreactor.

PubMed

Lee, Eun-Hee; Choi, Sun-Ah; Yi, Taewoo; Kim, Tae Gwan; Lee, Sang-Don; Cho, Kyung-Suk

2015-01-01

Two identical lab-scale bioreactor systems were operated to examine the effects of granular activated carbon (GAC) on methane removal performance and methanotrophic community. Both bioreactor systems removed methane completely at a CH4 loading rate of 71.2 g-CH4·d(-1) for 17 days. However, the methane removal efficiency declined to 88% in the bioreactor without GAC, while the bioreactor amended with GAC showed greater methane removal efficiency of 97% at a CH4 loading rate of 107.5 g-CH4·d(-1). Although quantitative real-time PCR showed that methanotrophic populations were similar levels of 5-10 × 10(8) pmoA gene copy number·VSS(-1) in both systems, GAC addition changed the methanotrophic community composition of the bioreactor systems. Microarray assay revealed that GAC enhanced the type I methanotrophic genera including Methylobacter, Methylomicrobium, and Methylomonas of the system, which suggests that GAC probably provided a favorable environment for type I methanotrophs. These results indicated that GAC is a promising support material in bioreactor systems for CH4 mitigation.

A balanced microbiota efficiently produces methane in a novel high-rate horizontal anaerobic reactor for the treatment of swine wastewater.

PubMed

Duda, Rose Maria; da Silva Vantini, Juliana; Martins, Larissa Scattolin; de Mello Varani, Alessandro; Lemos, Manoel Victor Franco; Ferro, Maria Inês Tiraboschi; de Oliveira, Roberto Alves

2015-12-01

A novel combination of structurally simple, high-rate horizontal anaerobic reactors installed in series was used to treat swine wastewater. The reactors maintained stable pH, alkalinity, and volatile acid levels. Removed chemical oxygen demand (COD) represented 68% of the total, and the average specific methane production was 0.30L CH4 (g removed CODtot)(-1). In addition, next-generation sequencing and quantitative real-time PCR analyses were used to explore the methane-producing Archaea and microbial diversity. At least 94% of the sludge diversity belong to the Bacteria and Archaea, indicating a good balance of microorganisms. Among the Bacteria the Proteobacteria, Bacteroidetes and Firmicutes were the most prevalent phyla. Interestingly, up to 12% of the sludge diversity belongs to methane-producing orders, such as Methanosarcinales, Methanobacteriales and Methanomicrobiales. In summary, this system can efficiently produce methane and this is the first time that horizontal anaerobic reactors have been evaluated for the treatment of swine wastewater. Copyright © 2015 Elsevier Ltd. All rights reserved.

Methane storage in metal-organic frameworks.

PubMed

He, Yabing; Zhou, Wei; Qian, Guodong; Chen, Banglin

2014-08-21

Natural gas (NG), whose main component is methane, is an attractive fuel for vehicular applications. Realization of safe, cheap and convenient means and materials for high-capacity methane storage can significantly facilitate the implementation of natural gas fuelled vehicles. The physisorption based process involving porous materials offers an efficient storage methodology and the emerging porous metal-organic frameworks have been explored as potential candidates because of their extraordinarily high porosities, tunable pore/cage sizes and easily immobilized functional sites. In this view, we provide an overview of the current status of metal-organic frameworks for methane storage.

75 FR 29338 - Energy Efficiency of Natural Gas Infrastructure and Operations Conference; Final Notice of Public...

Federal Register 2010, 2011, 2012, 2013, 2014

2010-05-25

... recovery projects and issues associated with fugitive methane. Bruce Hedman, ICF International, on behalf... associated with fugitive methane. Richard D. Murphy, S.V.P. Energy Solutions Services, National Grid, on...

Catalytic Tar Reduction for Assistance in Thermal Conversion of Space Waste for Energy Production

NASA Technical Reports Server (NTRS)

Caraccio, Anne Joan; Devor, Robert William; Hintze, Paul E.; Muscatello, Anthony C.; Nur, Mononita

2014-01-01

The Trash to Gas (TtG) project investigates technologies for converting waste generated during spaceflight into various resources. One of these technologies was gasification, which employed a downdraft reactor designed and manufactured at NASA's Kennedy Space Center (KSC) for the conversion of simulated space trash to carbon dioxide. The carbon dioxide would then be converted to methane for propulsion and water for life support systems. A minor byproduct of gasification includes large hydrocarbons, also known as tars. Tars are unwanted byproducts that add contamination to the product stream, clog the reactor and cause complications in analysis instrumentation. The objective of this research was to perform reduction studies of a mock tar using select catalysts and choose the most effective for primary treatment within the KSC downdraft gasification reactor. Because the KSC reactor is operated at temperatures below typical gasification reactors, this study evaluates catalyst performance below recommended catalytic operating temperatures. The tar reduction experimentation was observed by passing a model tar vapor stream over the catalysts at similar conditions to that of the KSC reactor. Reduction in tar was determined using gas chromatography. Tar reduction efficiency and catalyst performances were evaluated at different temperatures.

Ecophysiology of syntrophic communities that degrade saturated and unsaturated long-chain fatty acids.

PubMed

Sousa, Diana Z; Smidt, Hauke; Alves, Maria M; Stams, Alfons J M

2009-06-01

Syntrophic relationships are the key for biodegradation in methanogenic environments. We review the ecological and physiological features of syntrophic communities involved in the degradation of saturated and unsaturated long-chain fatty acids (LCFA), as well as their potential application to convert lipids/fats containing waste to biogas. Presently, about 14 species have been described with the ability to grow on fatty acids in syntrophy with methanogens, all belonging to the families Syntrophomonadaceae and Syntrophaceae. The principle pathway of LCFA degradation is through beta-oxidation, but the initial steps in the conversion of unsaturated LCFA are unclear. Communities enriched on unsaturated LCFA also degrade saturated LCFA, but the opposite generally is not the case. For efficient methane formation, the physical and inhibitory effects of LCFA on methanogenesis need to be considered. LCFA adsorbs strongly to biomass, which causes encapsulation of active syntrophic communities and hampers diffusion of substrate and products in and out of the biomass. Quantification of archaea by real-time PCR analysis suggests that potential LCFA inhibitory effect towards methanogens might be reversible. Rather, the conversion of adsorbed LCFA in batch assays was shown to result in a significant increase of archaeal cell numbers in anaerobic sludge samples.

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...

Engineering of Methane Metabolism in Pichia Pastoris Through Methane Monooxygenase Expression

NASA Technical Reports Server (NTRS)

Fleury, Samantha T.; Neff, Lily S.; Galazka, Jonathan M.

2017-01-01

Exploration of the solar system is constrained by the cost of moving mass off Earth. Producing materials in situ will reduce the mass that must be delivered from earth. CO2 is abundant on Mars and manned spacecraft. On the ISS, NASA reacts excess CO2 with H2 to generate CH4 and H2O using the Sabatier System. The resulting water is recovered into the ISS, but the methane is vented to space. Thus, there is a capability need for systems that convert methane into valuable materials. Methanotrophic bacteria consume methane but these are poor synthetic biology platforms. Thus, there is a knowledge gap in utilizing methane in a robust and flexible synthetic biology platform. The yeast Pichia pastoris is a refined microbial factory that is used widely by industry because it efficiently secretes products. Pichia could produce a variety of useful products in space. Pichia does not consume methane but robustly consumes methanol, which is one enzymatic step removed from methane. Our goal is to engineer Pichia to consume methane thereby creating a powerful methane-consuming microbial factory.

Anaerobic methane oxidation in low-organic content methane seep sediments

USGS Publications Warehouse

Pohlman, John W.; Riedel, Michael; Bauer, James E.; Canuel, Elizabeth A.; Paull, Charles K.; Lapham, Laura; Grabowski, Kenneth S.; Coffin, Richard B.; Spence, George D.

2013-01-01

Sulfate-dependent anaerobic oxidation of methane (AOM) is the key sedimentary microbial process limiting methane emissions from marine sediments and methane seeps. In this study, we investigate how the presence of low-organic content sediment influences the capacity and efficiency of AOM at Bullseye vent, a gas hydrate-bearing cold seep offshore of Vancouver Island, Canada. The upper 8 m of sediment contains 14C. A fossil origin for the DIC precludes remineralization of non-fossil OM present within the sulfate zone as a significant contributor to pore water DIC, suggesting that nearly all sulfate is available for anaerobic oxidation of fossil seep methane. Methane flux from the SMT to the sediment water interface in a diffusion-dominated flux region of Bullseye vent was, on average, 96% less than at an OM-rich seep in the Gulf of Mexico with a similar methane flux regime. Evidence for enhanced methane oxidation capacity within OM-poor sediments has implications for assessing how climate-sensitive reservoirs of sedimentary methane (e.g., gas hydrate) will respond to ocean warming, particularly along glacially-influenced mid and high latitude continental margins.

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.

Chemical recycling of carbon dioxide to methanol and dimethyl ether: from greenhouse gas to renewable, environmentally carbon neutral fuels and synthetic hydrocarbons.

PubMed

Olah, George A; Goeppert, Alain; Prakash, G K Surya

2009-01-16

Nature's photosynthesis uses the sun's energy with chlorophyll in plants as a catalyst to recycle carbon dioxide and water into new plant life. Only given sufficient geological time can new fossil fuels be formed naturally. In contrast, chemical recycling of carbon dioxide from natural and industrial sources as well as varied human activities or even from the air itself to methanol or dimethyl ether (DME) and their varied products can be achieved via its capture and subsequent reductive hydrogenative conversion. The present Perspective reviews this new approach and our research in the field over the last 15 years. Carbon recycling represents a significant aspect of our proposed Methanol Economy. Any available energy source (alternative energies such as solar, wind, geothermal, and atomic energy) can be used for the production of needed hydrogen and chemical conversion of CO(2). Improved new methods for the efficient reductive conversion of CO(2) to methanol and/or DME that we have developed include bireforming with methane and ways of catalytic or electrochemical conversions. Liquid methanol is preferable to highly volatile and potentially explosive hydrogen for energy storage and transportation. Together with the derived DME, they are excellent transportation fuels for internal combustion engines (ICE) and fuel cells as well as convenient starting materials for synthetic hydrocarbons and their varied products. Carbon dioxide thus can be chemically transformed from a detrimental greenhouse gas causing global warming into a valuable, renewable and inexhaustible carbon source of the future allowing environmentally neutral use of carbon fuels and derived hydrocarbon products.

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.

Mitigation of methane emission from an old unlined landfill in Klintholm, Denmark using a passive biocover system.

PubMed

Scheutz, Charlotte; Pedersen, Rasmus Broe; Petersen, Per Haugsted; Jørgensen, Jørgen Henrik Bjerre; Ucendo, Inmaculada Maria Buendia; Mønster, Jacob G; Samuelsson, Jerker; Kjeldsen, Peter

2014-07-01

Methane generated at landfills contributes to global warming and can be mitigated by biocover systems relying on microbial methane oxidation. As part of a closure plan for an old unlined landfill without any gas management measures, an innovative biocover system was established. The system was designed based on a conceptual model of the gas emission patterns established through an initial baseline study. The study included construction of gas collection trenches along the slopes of the landfill where the majority of the methane emissions occurred. Local compost materials were tested as to their usefulness as bioactive methane oxidizing material and a suitable compost mixture was selected. Whole site methane emission quantifications based on combined tracer release and downwind measurements in combination with several local experimental activities (gas composition within biocover layers, flux chamber based emission measurements and logging of compost temperatures) proved that the biocover system had an average mitigation efficiency of approximately 80%. The study showed that the system also had a high efficiency during winter periods with temperatures below freezing. An economic analysis indicated that the mitigation costs of the biocover system were competitive to other existing greenhouse gas mitigation options. Copyright © 2014 Elsevier Ltd. All rights reserved.

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.

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

Makundi, W.; Sathaye, J.; Fearnside, P.M.

Deforestation in Brazilian Amazonia in 1990 was releasing approximately 281--282 X 10{sup 6} metric tons (MT) of carbon on conversion to a landscape of agriculture, productive pasture, degraded pasture, secondary forest and regenerated forest in the proportions corresponding to the equilibrium condition implied by current land-use patterns. Emissions are expressed as ``committed carbon,`` or the carbon released over a period of years as the carbon stock in each hectare deforested approaches a new equilibrium in the landscape that replaces the original forest. To the extent that deforestation rates have remained constant, current releases from the areas deforested in previous yearsmore » will be equal to the future releases from the areas being cleared now. Considering the quantities of carbon dioxide, carbon monoxide, methane, nitrous oxide, NO{sub x} and non-methane hydrocarbons released raises the impact by 22--37%. The relative impact on the greenhouse effect of each gas is based on the Intergovernmental Panel on Climate Change (IPCC) calculations over a 20-year time period (including indirect effects). The six gases considered have a combined global warming impact equivalent to 343 to 386 million MT of C0{sub 2}-equivalent carbon, depending on assumptions regarding the release of methane and other gases from the various sources such as burning and termites. These emissions represent 7--8 times the 50 million MT annual carbon release from Brazil`s use of fossil fuels, but bring little benefit to the country. Stopping deforestation in Brazil would prevent as much greenhouse emission as tripling the fuel efficiency of all the automobiles in the world. The relatively cheap measures needed to contain deforestation, together with the many complementary benefits of doing so, make this the first priority for funds intended to slow global warming.« less

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

Makundi, W.; Sathaye, J.; Fearnside, P.M.

Deforestation in Brazilian Amazonia in 1990 was releasing approximately 281--282 X 10{sup 6} metric tons (MT) of carbon on conversion to a landscape of agriculture, productive pasture, degraded pasture, secondary forest and regenerated forest in the proportions corresponding to the equilibrium condition implied by current land-use patterns. Emissions are expressed as committed carbon,'' or the carbon released over a period of years as the carbon stock in each hectare deforested approaches a new equilibrium in the landscape that replaces the original forest. To the extent that deforestation rates have remained constant, current releases from the areas deforested in previous yearsmore » will be equal to the future releases from the areas being cleared now. Considering the quantities of carbon dioxide, carbon monoxide, methane, nitrous oxide, NO{sub x} and non-methane hydrocarbons released raises the impact by 22--37%. The relative impact on the greenhouse effect of each gas is based on the Intergovernmental Panel on Climate Change (IPCC) calculations over a 20-year time period (including indirect effects). The six gases considered have a combined global warming impact equivalent to 343 to 386 million MT of C0{sub 2}-equivalent carbon, depending on assumptions regarding the release of methane and other gases from the various sources such as burning and termites. These emissions represent 7--8 times the 50 million MT annual carbon release from Brazil's use of fossil fuels, but bring little benefit to the country. Stopping deforestation in Brazil would prevent as much greenhouse emission as tripling the fuel efficiency of all the automobiles in the world. The relatively cheap measures needed to contain deforestation, together with the many complementary benefits of doing so, make this the first priority for funds intended to slow global warming.« less

Co-digestion of agricultural and municipal waste to produce energy and soil amendment.

PubMed

Macias-Corral, Maritza A; Samani, Zohrab A; Hanson, Adrian T; Funk, Paul A

2017-09-01

In agriculture, manure and cotton gin waste are major environmental liabilities. Likewise, grass is an important organic component of municipal waste. These wastes were combined and used as substrates in a two-phase, pilot-scale anaerobic digester to evaluate the potential for biogas (methane) production, waste minimisation, and the digestate value as soil amendment. The anaerobic digestion process did not show signs of inhibition. Biogas production increased during the first 2 weeks of operation, when chemical oxygen demand and volatile fatty acid concentrations and the organic loading rate to the system were high. Chemical oxygen demand from the anaerobic columns remained relatively steady after the first week of operation, even at high organic loading rates. The experiment lasted about 1 month and produced 96.5 m 3 of biogas (68 m 3 of CH 4 ) per tonne of waste. In terms of chemical oxygen demand to methane conversion efficiency, the system generated 62% of the theoretical methane production; the chemical oxygen demand/volatile solids degradation rate was 62%, compared with the theoretical 66%. The results showed that co-digestion and subsequent digestate composting resulted in about 60% and 75% mass and volume reductions, respectively. Digestate analysis showed that it can be used as a high nutrient content soil amendment. The digestate met Class A faecal coliform standards (highest quality) established in the United States for biosolids. Digestion and subsequent composting concentrated the digestate nitrogen, phosphorus, and potassium content by 37%, 24%, and 317%, respectively. Multi-substrate co-digestion is a practical alternative for agricultural waste management, minimisation of landfill disposal, and it also results in the production of valuable products.

Dry anaerobic digestion of food waste and cardboard at different substrate loads, solid contents and co-digestion proportions.

PubMed

Capson-Tojo, Gabriel; Trably, Eric; Rouez, Maxime; Crest, Marion; Steyer, Jean-Philippe; Delgenès, Jean-Philippe; Escudié, Renaud

2017-06-01

The increasing food waste production calls for developing efficient technologies for its treatment. Anaerobic processes provide an effective waste valorization. The influence of the initial substrate load on the performance of batch dry anaerobic co-digestion reactors treating food waste and cardboard was investigated. The load was varied by modifying the substrate to inoculum ratio (S/X), the total solids content and the co-digestion proportions. The results showed that the S/X was a crucial parameter. Within the tested values (0.25, 1 and 4gVS·gVS -1 ), only the reactors working at 0.25 produced methane. Methanosarcina was the main archaea, indicating its importance for efficient methanogenesis. Acidogenic fermentation was predominant at higher S/X, producing hydrogen and other metabolites. Higher substrate conversions (≤48%) and hydrogen yields (≤62mL·gVS -1 ) were achieved at low loads. This study suggests that different value-added compounds can be produced in dry conditions, with the initial substrate load as easy-to-control operational parameter. Copyright © 2017 Elsevier Ltd. All rights reserved.

Design of an integrated fuel processor for residential PEMFCs applications

NASA Astrophysics Data System (ADS)

Seo, Yu Taek; Seo, Dong Joo; Jeong, Jin Hyeok; Yoon, Wang Lai

KIER has been developing a novel fuel processing system to provide hydrogen rich gas to residential PEMFCs system. For the effective design of a compact hydrogen production system, each unit process for steam reforming and water gas shift, has a steam generator and internal heat exchangers which are thermally and physically integrated into a single packaged hardware system. The newly designed fuel processor (prototype II) showed a thermal efficiency of 78% as a HHV basis with methane conversion of 89%. The preferential oxidation unit with two staged cascade reactors, reduces, the CO concentration to below 10 ppm without complicated temperature control hardware, which is the prerequisite CO limit for the PEMFC stack. After we achieve the initial performance of the fuel processor, partial load operation was carried out to test the performance and reliability of the fuel processor at various loads. The stability of the fuel processor was also demonstrated for three successive days with a stable composition of product gas and thermal efficiency. The CO concentration remained below 10 ppm during the test period and confirmed the stable performance of the two-stage PrOx reactors.

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

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.

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.

Anaerobic digestion of grass: the effect of temperature applied during the storage of substrate on the methane production.

PubMed

Míchal, Pavel; Švehla, Pavel; Plachý, Vladimír; Tlustoš, Pavel

2017-07-01

Within this research, biogas production, representation of methane in biogas and volatile solids (VSs) removal efficiency were compared using batch tests performed with the samples of intensively and extensively planted grasses originating from public areas. Before the batch tests, the samples were stored at different temperatures achievable on biogas plants applying trigeneration strategy (-18°C, +3°C, +18°C and +35°C). Specific methane production from intensively planted grasses was relatively high (0.33-0.41 m 3 /kg VS) compared to extensively planted grasses (0.20-0.33 m 3 /kg VS). VSs removal efficiency reached 59.8-68.8% for intensively planted grasses and 34.6-56.5% for extensively planted grasses. Freezing the intensively planted grasses at -18°C proved to be an effective thermal pretreatment leading to high biogas production (0.61 m 3 /kg total solid (TS)), high representation of methane (64.0%) in biogas and good VSs removal efficiency (68.8%). The results of this research suggest that public areas or sport parks seem to be available, cheap and at the same time very effective feedstock for biogas production.

An innovative sewage sludge reduction by using a combined mesophilic anaerobic and thermophilic aerobic process with thermal-alkaline treatment and sludge recirculation.

PubMed

Cho, Hyun Uk; Park, Sang Kyu; Ha, Jeong Hyub; Park, Jong Moon

2013-11-15

Lab-scale High Efficiency Digestion (HED) systems containing a Mesophilic Anaerobic Reactor (MAR), Thermophilic Aerobic Reactor (TAR), liquid/solid separation unit, and thermal-alkaline treatment were developed to evaluate the efficiencies of sludge reduction and methane production. The HED process was divided into three phases to examine the influence of sludge pretreatment and pretreated sludge recirculation using TCOD and VSS reduction, COD solubilization, and methane production. The VSS removal with a solid/liquid separation unit, sludge recirculation, and thermal-alkaline treatment drastically increased up to 95% compared to the feed concentration. In addition, the results of COD solubilization and VSS/TSS showed that the solubilization of cells and organic matters by the thermal-alkaline treatment was highly increased, which was also consistent with the SEM images. In particular, the methane production rate increased 24-fold when the feed sludge and recirculated sludge were pretreated together. Collectively, the HED experiments performed with sludge recirculation and thermal-alkaline treatment demonstrated that the HED systems can be successfully employed for highly efficient sewage sludge reduction and methane gas production. Copyright © 2013 Elsevier Ltd. All rights reserved.

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

Aerated biofilters with multiple-level air injection configurations to enhance biological treatment of methane emissions.

PubMed

Farrokhzadeh, Hasti; Hettiaratchi, J Patrick A; Jayasinghe, Poornima; Kumar, Sunil

2017-09-01

Aiming to improve conventional methane biofilter performance, a multiple-level aeration biofilter design is proposed. Laboratory flow-through column experiments were conducted to evaluate three actively-aerated methane biofilter configurations. Columns were aerated at one, two, and three levels of the bed depth, with air introduced at flow rates calculated from methane oxidation reaction stoichiometry. Inlet methane loading rates were increased in five stages between 6 and 18mL/min. The effects of methane feeding rate, levels of aeration, and residence time on methane oxidation rates were determined. Samples collected after completion of flow-through experiments were used to determine methane oxidation kinetic parameters, V max , K m , and methanotrophic community distribution across biofilter columns. Results obtained from mixed variances analysis and response surfaces, as well as methanotrophic activity data, suggested that, biofilter column with two aeration levels has the most even performance over time, maintaining 85.1% average oxidation efficiency over 95days of experiments. Copyright © 2017 Elsevier Ltd. All rights reserved.

Simultaneous enhancement of methane production and methane content in biogas from waste activated sludge and perennial ryegrass anaerobic co-digestion: The effects of pH and C/N ratio.

PubMed

Dai, Xiaohu; Li, Xiaoshuai; Zhang, Dong; Chen, Yinguang; Dai, Lingling

2016-09-01

It is necessary to find an appropriate strategy to simultaneously enhance the methane production and methane content in biogas from waste activated sludge (WAS) and grass co-digestion. In this study an efficient strategy, i.e., adjusting the initial pH 12 and C/N ratio 17/1, for simultaneous enhancement of methane production and methane content in biogas from WAS and perennial ryegrass co-digestion was reported. Experimental results indicated that the maximal methane production was 310mL/gVSadd at the optimum conditions after 30-d anaerobic digestion, which was, respectively, about 1.5- and 3.8-fold of the sole WAS and sole perennial ryegrass anaerobic digestion. Meanwhile, the methane content in biogas was about 74%, which was much higher than that of sole WAS (64%) or sole perennial ryegrass (54%) anaerobic digestion. Copyright © 2016 Elsevier Ltd. All rights reserved.

Significance of dissolved methane in effluents of anaerobically treated low strength wastewater and potential for recovery as an energy product: A review.

PubMed

Crone, Brian C; Garland, Jay L; Sorial, George A; Vane, Leland M

2016-11-01

The need for energy efficient Domestic Wastewater (DWW) treatment is increasing annually with population growth and expanding global energy demand. Anaerobic treatment of low strength DWW produces methane which can be used to as an energy product. Temperature sensitivity, low removal efficiencies (Chemical Oxygen Demand (COD), Suspended Solids (SS), and Nutrients), alkalinity demand, and potential greenhouse gas (GHG) emissions have limited its application to warmer climates. Although well designed anaerobic Membrane Bioreactors (AnMBRs) are able to effectively treat DWW at psychrophilic temperatures (10-30 °C), lower temperatures increase methane solubility leading to increased energy losses in the form of dissolved methane in the effluent. Estimates of dissolved methane losses are typically based on concentrations calculated using Henry's Law but advection limitations can lead to supersaturation of methane between 1.34 and 6.9 times equilibrium concentrations and 11-100% of generated methane being lost in the effluent. In well mixed systems such as AnMBRs which use biogas sparging to control membrane fouling, actual concentrations approach equilibrium values. Non-porous membranes have been used to recover up to 92.6% of dissolved methane and well suited for degassing effluents of Upflow Anaerobic Sludge Blanket (UASB) reactors which have considerable solids and organic contents and can cause pore wetting and clogging in microporous membrane modules. Microporous membranes can recover up to 98.9% of dissolved methane in AnMBR effluents which have low COD and SS concentrations. Sequential Down-flow Hanging Sponge (DHS) reactors have been used to recover between 57 and 88% of dissolved methane from Upflow Anaerobic Sludge Blanket (UASB) reactor effluent at concentrations of greater than 30% and oxidize the rest for a 99% removal of total dissolved methane. They can also remove 90% of suspended solids and COD in UASB effluents and produce a high quality effluent. In situ degassing can increase process stability, COD removal, biomass retention, and headspace methane concentrations. A model for estimating energy consumption associated with membrane-based dissolved methane recovery predicts that recovered dissolved and headspace methane may provide all the energy required for operation of an anaerobic system treating DWW at psychrophilic temperatures. Copyright © 2016 Elsevier Ltd. All rights reserved.

An Eco-Friendly Improved Protocol for the Synthesis of Bis(3-indolyl)methanes Using Poly(4-vinylpyridinium)hydrogen Sulfate as Efficient, Heterogeneous, and Recyclable Solid Acid Catalyst

PubMed Central

Banothu, Janardhan; Gali, Rajitha; Velpula, Ravibabu; Bavantula, Rajitha; Crooks, Peter A.

2013-01-01

Highly efficient and eco-friendly protocol for the synthesis of bis(3-indolyl)methanes by the electrophilic substitution reaction of indole with aldehydes catalyzed by poly(4-vinylpyridinium)hydrogen sulfate was described. Excellent yields, shorter reaction times, simple work-up procedure, avoiding hazardous organic solvents, and reusability of the catalyst are the most obvious advantages of this method. PMID:24052864

Trace-gas metabolic versatility of the facultative methanotroph Methylocella silvestris.

PubMed

Crombie, Andrew T; Murrell, J Colin

2014-06-05

The climate-active gas methane is generated both by biological processes and by thermogenic decomposition of fossil organic material, which forms methane and short-chain alkanes, principally ethane, propane and butane. In addition to natural sources, environments are exposed to anthropogenic inputs of all these gases from oil and gas extraction and distribution. The gases provide carbon and/or energy for a diverse range of microorganisms that can metabolize them in both anoxic and oxic zones. Aerobic methanotrophs, which can assimilate methane, have been considered to be entirely distinct from utilizers of short-chain alkanes, and studies of environments exposed to mixtures of methane and multi-carbon alkanes have assumed that disparate groups of microorganisms are responsible for the metabolism of these gases. Here we describe the mechanism by which a single bacterial strain, Methylocella silvestris, can use methane or propane as a carbon and energy source, documenting a methanotroph that can utilize a short-chain alkane as an alternative to methane. Furthermore, during growth on a mixture of these gases, efficient consumption of both gases occurred at the same time. Two soluble di-iron centre monooxygenase (SDIMO) gene clusters were identified and were found to be differentially expressed during bacterial growth on these gases, although both were required for efficient propane utilization. This report of a methanotroph expressing an additional SDIMO that seems to be uniquely involved in short-chain alkane metabolism suggests that such metabolic flexibility may be important in many environments where methane and short-chain alkanes co-occur.

Sequential hydrogen and methane coproduction from sugary wastewater treatment by "CSTRHyd-UASBMet" system

NASA Astrophysics Data System (ADS)

Hao, Ping

2017-10-01

Potentiality of sequential hydrogen bioproduction from sugary wastewater treatment was investigated using continuous stirred tank reactor (CSTR) for various substrate COD concentrations and HRTs. At optimum substrate concentration of 6 g COD/L, hydrogen could be efficiently produced from CSTR with the highest production rate of 3.00 (±0.04) L/L reactor d at HRT of 6 h. The up flow anaerobic sludge bed (UASB) reactor was used for continuous methane bioproduction from the effluents of hydrogen bioproduction. At optimal HRT 12 h, methane could be produced with a production rate of 2.27 (±0.08) L/L reactor d and the COD removal efficiency reached up to the maximum 82.3%.

Alternate aircraft fuels: Prospects and operational implications

NASA Technical Reports Server (NTRS)

Witcofski, R. D.

1977-01-01

The potential use of coal-derived aviation fuels was assessed. The studies addressed the prices and thermal efficiencies associated with the production of coal-derived aviation kerosene, liquid methane and liquid hydrogen and the air terminal requirements and subsonic transport performance when utilizing liquid hydrogen. The fuel production studies indicated that liquid methane can be produced at a lower price and with a higher thermal efficiency than aviation kerosene or liquid hydrogen. Ground facilities of liquefaction, storage, distribution and refueling of liquid hydrogen fueled aircraft at airports appear technically feasibile. The aircraft studies indicate modest onboard energy savings for hydrogen compared to conventional fuels. Liquid hydrogen was found to be superior to both aviation kerosene and liquid methane from the standpoint of aircraft engine emissions.

Temperature-Induced Increase in Methane Release from Peat Bogs: A Mesocosm Experiment

PubMed Central

van Winden, Julia F.; Reichart, Gert-Jan; McNamara, Niall P.; Benthien, Albert; Damsté, Jaap S. Sinninghe.

2012-01-01

Peat bogs are primarily situated at mid to high latitudes and future climatic change projections indicate that these areas may become increasingly wetter and warmer. Methane emissions from peat bogs are reduced by symbiotic methane oxidizing bacteria (methanotrophs). Higher temperatures and increasing water levels will enhance methane production, but also methane oxidation. To unravel the temperature effect on methane and carbon cycling, a set of mesocosm experiments were executed, where intact peat cores containing actively growing Sphagnum were incubated at 5, 10, 15, 20, and 25°C. After two months of incubation, methane flux measurements indicated that, at increasing temperatures, methanotrophs are not able to fully compensate for the increasing methane production by methanogens. Net methane fluxes showed a strong temperature-dependence, with higher methane fluxes at higher temperatures. After removal of Sphagnum, methane fluxes were higher, increasing with increasing temperature. This indicates that the methanotrophs associated with Sphagnum plants play an important role in limiting the net methane flux from peat. Methanotrophs appear to consume almost all methane transported through diffusion between 5 and 15°C. Still, even though methane consumption increased with increasing temperature, the higher fluxes from the methane producing microbes could not be balanced by methanotrophic activity. The efficiency of the Sphagnum-methanotroph consortium as a filter for methane escape thus decreases with increasing temperature. Whereas 98% of the produced methane is retained at 5°C, this drops to approximately 50% at 25°C. This implies that warming at the mid to high latitudes may be enhanced through increased methane release from peat bogs. PMID:22768100

Incentives for methane mitigation and energy-efficiency improvements in the case of Ukraine's natural gas transmission system

NASA Astrophysics Data System (ADS)

Roshchanka, Volha; Evans, Meredydd

2014-06-01

Reducing methane losses is a concern for climate change policy and energy policy. The energy sector is the major source of anthropogenic methane emissions into the atmosphere in Ukraine. Reducing methane emissions and avoiding combustion can be very cost-effective, but various barriers prevent such energy-efficiency measures from taking place. To date, few examples of industry-wide improvements exist. One example of substantial investments into upgrading natural gas transmission system comes from Ukraine's natural gas transmission company, Ukrtransgaz. The company's investments into system upgrades, along with a 34% fall in throughput, resulted in reduction of Ukrtransgaz system's own consumption of natural gas by 68% in 2011 compared to the level in 2005. Evaluating reductions in methane emissions is challenging because of lack of accurate data and gaps in accounting methodologies. At the same time, Ukraine's transmission system has undergone improvements that, at the very least, have contained methane emissions, if not substantially reduced them. In this paper, we describe recent developments in Ukraine's natural gas transmission system and analyze the incentives that forced the sector to pay close attention to its methane losses. Ukraine is one of the most energy-intensive countries, among the largest natural gas consumers in the world, and a significant emitter of methane. The country is also dependent on imports of natural gas. A combination of several factors has created conditions for successful reductions in methane emissions and combustion. These factors include: an eightfold increase in the price of imported natural gas; comprehensive domestic environmental and energy policies, such as the Laws of Ukraine on Protecting the Natural Environment and on Air Protection; policies aimed at integration with European Union's energy market and accession to the Energy Community Treaty; and the country's participation in international cooperation on environment, such as through the Joint Implementation mechanism and the voluntary Global Methane Initiative. Learning about such case studies can help policymakers and sustainability professionals design better policies elsewhere.

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.

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

Effects of thermal pretreatment and catalyst on biomass gasification efficiency and syngas composition

DOE PAGES

Cheah, Singfoong; Jablonski, Whitney S.; Olstad, Jessica L.; ...

2016-09-16

This work explores the combined effects of thermal pretreatment and using a catalyst in situ on gasification carbon conversion efficiency, as well as product gas and tar content and compositions. To compare the effects of thermal pretreatment, pelletized and ground oak with three different levels of thermal pretreatment were gasified in a fluidized bed reactor. The pretreatments applied to the oak were (1) pelletization, (2) drying at 180 °C in air, and (3) torrefaction at 270 °C in nitrogen. The oak dried at 180 °C produced syngas of similar quality and approximately the same amount of char as untreated oak.more » Torrefaction at 270 °C resulted in syngas with a higher hydrogen to CO ratio, lower methane, and less than half of the total tar -- all of which are desirable properties in terms of product gas quality. However, the oak torrefied at 270 °C also produced more than two times the amount of char as the untreated, pelletized oak. To determine the effect of catalyst, a series of experiments were conducted using olivine impregnated with nickel and cerium as the fluidized bed material in the gasifier. These tests showed that modified olivine can improve hydrogen production and reduce methane and tar levels in the syngas. The result was observed for both treated and untreated oak; although the effect was more substantial for untreated oak, for which the use of modified olivine reduced tar concentrations in the product gas by 60%, with a larger reduction in heavier tars than lighter tars. Furthermore, this result is important because reduction in heavier tar plays a more important role in benefitting downstream operations.« less

Single Spatial-Mode Room-Temperature-Operated 3.0 to 3.4 micrometer Diode Lasers

NASA Technical Reports Server (NTRS)

Frez, Clifford F.; Soibel, Alexander; Belenky, Gregory; Shterengas, Leon; Kipshidze, Gela

2010-01-01

Compact, highly efficient, 3.0 to 3.4 m light emitters are in demand for spectroscopic analysis and identification of chemical substances (including methane and formaldehyde), infrared countermeasures technologies, and development of advanced infrared scene projectors. The need for these light emitters can be currently addressed either by bulky solid-state light emitters with limited power conversion efficiency, or cooled Interband Cascade (IC) semiconductor lasers. Researchers here have developed a breakthrough approach to fabrication of diode mid-IR lasers that have several advantages over IC lasers used for the Mars 2009 mission. This breakthrough is due to a novel design utilizing the strain-engineered quantum-well (QW) active region and quinternary barriers, and due to optimization of device material composition and growth conditions (growth temperatures and rates). However, in their present form, these GaSb-based laser diodes cannot be directly used as a part of sensor systems. The device spectrum is too broad to perform spectroscopic analysis of gas species, and operating currents and voltages are too high. In the current work, the emitters were fabricated as narrow-ridge waveguide index-guided lasers rather than broad stripe-gain guided multimode Fabry-Perot (FP) lasers as was done previously. These narrow-ridge waveguide mid-IR lasers exhibit much lower power consumptions, and can operate in a single spatial mode that is necessary for demonstration of single-mode distributed feedback (DBF) devices for spectroscopic applications. These lasers will enable a new generation of compact, tunable diode laser spectrometers with lower power consumption, reduced complexity, and significantly reduced development costs. These lasers can be used for the detection of HCN, C2H2, methane, and ethane.

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.

Development of a preprototype sabatier CO2 reduction subsystem

NASA Technical Reports Server (NTRS)

Kleiner, G. N.; Birbara, P.

1980-01-01

A preoprototype Sabatier CO2 Reduction Subsystem was successfully designed, fabricated and tested. The lightweight, quick starting reactor utilizes a highly active and physically durable methanation catalyst composed of ruthenium on alumina. The use of this improved catalyst permits a single straight through plug flow design with an average lean component H2/CO2 conversion efficiency of over 99% over a range of H2/CO2 molar ratios of 1.8 to 5 while operating with flows equivalent to a crew size of one person steadystate to 3 persons cyclical (equivalent to 5 persons steady state). The reactor requires no heater operation after start-up even during simulated 55 minute lightside/39 minute darkside orbital operation over the above range of molar ratios and crew loadings. The subsystem's operation and performance is controlled by a microprocessor and displayed on a nineteen inch multi-colored cathode ray tube.

Effect of biological pretreatments in enhancing corn straw biogas production.

PubMed

Zhong, Weizhang; Zhang, Zhongzhi; Luo, Yijing; Sun, Shanshan; Qiao, Wei; Xiao, Meng

2011-12-01

A biological pretreatment with new complex microbial agents was used to pretreat corn straw at ambient temperature (about 20°C) to improve its biodegradability and anaerobic biogas production. A complex microbial agent dose of 0.01% (w/w) and pretreatment time of 15 days were appropriate for biological pretreatment. These treatment conditions resulted in 33.07% more total biogas yield, 75.57% more methane yield, and 34.6% shorter technical digestion time compared with the untreated sample. Analyses of chemical compositions showed 5.81-25.10% reductions in total lignin, cellulose, and hemicellulose contents, and 27.19-80.71% increases in hot-water extractives; these changes contributed to the enhancement of biogas production. Biological pretreatment could be an effective method for improving biodegradability and enhancing the highly efficient biological conversion of corn straw into bioenergy. Copyright © 2011 Elsevier Ltd. All rights reserved.

Development of a preprototype Sabatier CO2 reduction subsystem

NASA Technical Reports Server (NTRS)

Kleiner, G. N.; Birbara, P.

1981-01-01

A lightweight, quick starting reactor utilizes a highly active and physically durable methanation catalyst composed of ruthenium on alumina. The use of this improved catalyst permits a single straight through plug flow design with an average lean component H2/CO2 conversion efficiency of over 99% over a range of H2/CO2 molar ratios of 1.8 to 5 while operating with flows equivalent to a crew size of one person steadystate to 3 persons cyclical. The reactor requires no heater operation after start-up even during simulated 55 minute lightside/39 minute darkside orbital operation over the above range of molar ratios and crew loadings. Subsystem performance was proven by parametric testing and endurance testing over a wide range of crew sizes and metabolic loadings. The subsystem's operation and performance is controlled by a microprocessor and displayed on a nineteen inch multi-colored cathode ray tube.

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.

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

EPA Science Inventory

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

Enhancing biogas production of corn stover by fast pyrolysis pretreatment.

PubMed

Wang, Fang; Zhang, Deli; Wu, Houkai; Yi, Weiming; Fu, Peng; Li, Yongjun; Li, Zhihe

2016-10-01

A new thermo-chemical pretreatment by a lower temperature fast pyrolysis (LTFP) was applied to promote anaerobic digestion (AD) efficiency of corn stover (CS). The pretreatment experiment was performed by a fluidized bed pyrolysis reactor at 180, 200 and 220°C with a carrier gas flow rate of 4 and 3m(3)/h. The components characteristics, Scanning Electron Microscope (SEM) images and Crystal Intensity (CrI) of the pretreated CS were tested to explore effectiveness of the pretreatment. The results showed that the cumulative methane production at 180°C for 4 and 3m(3)/h were 199.8 and 200.3mL/g TS, respectively. As compared to the untreated CS, the LTFP pretreatment significantly (a<0.05) increased the methane production by 18.07% and 18.33%, respectively. Methane production was well fitted by the Gompertz models, and the maximum methane potential and AD efficiency was obtained at 180°C for 3m(3)/h. Copyright © 2016 Elsevier Ltd. All rights reserved.

Rerouting Cellular Electron Flux To Increase the Rate of Biological Methane Production

PubMed Central

Catlett, Jennie L.; Ortiz, Alicia M.

2015-01-01

Methanogens are anaerobic archaea that grow by producing methane, a gas that is both an efficient renewable fuel and a potent greenhouse gas. We observed that overexpression of the cytoplasmic heterodisulfide reductase enzyme HdrABC increased the rate of methane production from methanol by 30% without affecting the growth rate relative to the parent strain. Hdr enzymes are essential in all known methane-producing archaea. They function as the terminal oxidases in the methanogen electron transport system by reducing the coenzyme M (2-mercaptoethane sulfonate) and coenzyme B (7-mercaptoheptanoylthreonine sulfonate) heterodisulfide, CoM-S-S-CoB, to regenerate the thiol-coenzymes for reuse. In Methanosarcina acetivorans, HdrABC expression caused an increased rate of methanogenesis and a decrease in metabolic efficiency on methylotrophic substrates. When acetate was the sole carbon and energy source, neither deletion nor overexpression of HdrABC had an effect on growth or methane production rates. These results suggest that in cells grown on methylated substrates, the cell compensates for energy losses due to expression of HdrABC with an increased rate of substrate turnover and that HdrABC lacks the appropriate electron donor in acetate-grown cells. PMID:26162885

Some advantages of methane in an aircraft gas turbine

NASA Technical Reports Server (NTRS)

Graham, R. W.; Glassman, A. J.

1980-01-01

Liquid methane, which can be manufactured from any of the hydrocarbon sources such as coal, shale biomass, and organic waste considered as a petroleum replacement for aircraft fuels. A simple cycle analysis is carried out for a turboprop engine flying a Mach 0.8 and 10, 688 meters (35,000 ft.) altitude. Cycle performance comparisions are rendered for four cases in which the turbine cooling air is cooled or not cooled by the methane fuel. The advantages and disadvantages of involving the fuel in the turbine cooling system are discussed. Methane combustion characteristics are appreciably different from Jet A and will require different combustor designs. Although a number of similar difficult technical problems exist, a highly fuel efficient turboprop engine burning methane appear to be feasible.

Increasing conversion efficiency of two-step photon up-conversion solar cell with a voltage booster hetero-interface.

PubMed

Asahi, Shigeo; Kusaki, Kazuki; Harada, Yukihiro; Kita, Takashi

2018-01-17

Development of high-efficiency solar cells is one of the attractive challenges in renewable energy technologies. Photon up-conversion can reduce the transmission loss and is one of the promising concepts which improve conversion efficiency. Here we present an analysis of the conversion efficiency, which can be increased by up-conversion in a single-junction solar cell with a hetero-interface that boosts the output voltage. We confirm that an increase in the quasi-Fermi gap and substantial photocurrent generation result in a high conversion efficiency.

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

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

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.

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

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

An investigation of anaerobic methane oxidation by consortia of methanotrophic archaea and bacterial partners using nanoSIMS and process-based modeling

NASA Astrophysics Data System (ADS)

Shi, Y.; Kempes, C.; Chadwick, G.; McGlynn, S.; He, X.; Orphan, V. J.; Meile, C. D.

2016-02-01

The anaerobic oxidation of methane in marine sediments plays an important role in the global methane cycle. Mediated by a microbial consortium consisting of archaea and bacteria, it is estimated that almost 80% of all the methane that arises from marine sediments is oxidized anaerobically by this process (Reeburgh 2007, Chemical Reviews 107, 486-513). We used reactive transport modeling to compare and contrast potential mechanisms of methane oxidation. This included acetate, hydrogen, formate, and disulfide acting as intermediates that are exchanged between archaea and bacteria. Moreover, we investigated electron transport through nanowires, facilitating the electron exchange between the microbial partners. It was shown that reaction kinetics, transport intensities, and energetic considerations all could decisively impact the overall rate of methane consumption. Informed by observed microbial cell distribution, we applied the model to a range of spatial distribution patterns of archaea and bacteria. We found that a consortium with evenly distributed archaeal and bacterial cells has the potential to more efficiently oxidize methane, because the vicinity of bacteria and archaea counteracts the build up of products and therefore prevents the thermodynamic shutdown of microbial metabolism. Single cell stable isotope enrichment in archaeal-bacterial consortia observed by nanoSIMS revealed rather uniform levels of anabolic activity within consortia with different spatial distribution patterns. Comparison to model simulation illustrates that efficient exchange is necessary to reproduce such observations and prevent conditions that are energetically unfavorable for methane oxidation to take place. Model simulations indicate that a recently described mechanism of direct interspecies electron transport between the methanotrophic archaea and its bacterial partner through a conductive matrix (McGlynn et al. 2015, Nature, 10.1038/nature15512) is consistent with observations.

Carbon and energy footprint of the hydrate-based biogas upgrading process integrated with CO2 valorization.

PubMed

Castellani, Beatrice; Rinaldi, Sara; Bonamente, Emanuele; Nicolini, Andrea; Rossi, Federico; Cotana, Franco

2018-02-15

The present paper aims at assessing the carbon and energy footprint of an energy process, in which the energy excess from intermittent renewable sources is used to produce hydrogen which reacts with the CO 2 previously separated from an innovative biogas upgrading process. The process integrates a hydrate-based biogas upgrading section and a CO 2 methanation section, to produce biomethane from the biogas enrichment and synthetic methane from the CO 2 methanation. Clathrate hydrates are crystalline compounds, formed by gas enclathrated in cages of water molecules and are applied to the selective separation of CO 2 from biogas mixtures. Data from the experimental setup were analyzed in order to evaluate the green-house gas emissions (carbon footprint CF) and the primary energy consumption (energy footprint EF) associated to the two sections of the process. The biosynthetic methane production during a single-stage process was 0.962Nm 3 , obtained mixing 0.830Nm 3 of methane-enriched biogas and 0.132Nm 3 of synthetic methane. The final volume composition was: 73.82% CH 4 , 19.47% CO 2 , 0.67% H 2 , 1.98% O 2 , 4.06% N 2 and the energy content was 28.0MJ/Nm 3 . The functional unit is the unitary amount of produced biosynthetic methane in Nm 3 . Carbon and energy footprints are 0.7081kgCO 2eq /Nm 3 and 28.55MJ/Nm 3 , respectively, when the electric energy required by the process is provided by photovoltaic panels. In this scenario, the overall energy efficiency is about 0.82, higher than the worldwide average energy efficiency for fossil methane, which is 0.75. Copyright © 2017 Elsevier B.V. All rights reserved.

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

Stable acetate production in extreme-thermophilic (70°C) mixed culture fermentation by selective enrichment of hydrogenotrophic methanogens

NASA Astrophysics Data System (ADS)

Zhang, Fang; Zhang, Yan; Ding, Jing; Dai, Kun; van Loosdrecht, Mark C. M.; Zeng, Raymond J.

2014-06-01

The control of metabolite production is difficult in mixed culture fermentation. This is particularly related to hydrogen inhibition. In this work, hydrogenotrophic methanogens were selectively enriched to reduce the hydrogen partial pressure and to realize efficient acetate production in extreme-thermophilic (70°C) mixed culture fermentation. The continuous stirred tank reactor (CSTR) was stable operated during 100 days, in which acetate accounted for more than 90% of metabolites in liquid solutions. The yields of acetate, methane and biomass in CSTR were 1.5 +/- 0.06, 1.0 +/- 0.13 and 0.4 +/- 0.05 mol/mol glucose, respectively, close to the theoretical expected values. The CSTR effluent was stable and no further conversion occurred when incubated for 14 days in a batch reactor. In fed-batch experiments, acetate could be produced up to 34.4 g/L, significantly higher than observed in common hydrogen producing fermentations. Acetate also accounted for more than 90% of soluble products formed in these fed-batch fermentations. The microbial community analysis revealed hydrogenotrophic methanogens (mainly Methanothermobacter thermautotrophicus and Methanobacterium thermoaggregans) as 98% of Archaea, confirming that high temperature will select hydrogenotrophic methanogens over aceticlastic methanogens effectively. This work demonstrated a potential application to effectively produce acetate as a value chemical and methane as an energy gas together via mixed culture fermentation.

Stable acetate production in extreme-thermophilic (70°C) mixed culture fermentation by selective enrichment of hydrogenotrophic methanogens

PubMed Central

Zhang, Fang; Zhang, Yan; Ding, Jing; Dai, Kun; van Loosdrecht, Mark C. M.; Zeng, Raymond J.

2014-01-01

The control of metabolite production is difficult in mixed culture fermentation. This is particularly related to hydrogen inhibition. In this work, hydrogenotrophic methanogens were selectively enriched to reduce the hydrogen partial pressure and to realize efficient acetate production in extreme-thermophilic (70°C) mixed culture fermentation. The continuous stirred tank reactor (CSTR) was stable operated during 100 days, in which acetate accounted for more than 90% of metabolites in liquid solutions. The yields of acetate, methane and biomass in CSTR were 1.5 ± 0.06, 1.0 ± 0.13 and 0.4 ± 0.05 mol/mol glucose, respectively, close to the theoretical expected values. The CSTR effluent was stable and no further conversion occurred when incubated for 14 days in a batch reactor. In fed-batch experiments, acetate could be produced up to 34.4 g/L, significantly higher than observed in common hydrogen producing fermentations. Acetate also accounted for more than 90% of soluble products formed in these fed-batch fermentations. The microbial community analysis revealed hydrogenotrophic methanogens (mainly Methanothermobacter thermautotrophicus and Methanobacterium thermoaggregans) as 98% of Archaea, confirming that high temperature will select hydrogenotrophic methanogens over aceticlastic methanogens effectively. This work demonstrated a potential application to effectively produce acetate as a value chemical and methane as an energy gas together via mixed culture fermentation. PMID:24920064

Recovery and biological oxidation of dissolved methane in effluent from UASB treatment of municipal sewage using a two-stage closed downflow hanging sponge system.

PubMed

Matsuura, Norihisa; Hatamoto, Masashi; Sumino, Haruhiko; Syutsubo, Kazuaki; Yamaguchi, Takashi; Ohashi, Akiyoshi

2015-03-15

A two-stage closed downflow hanging sponge (DHS) reactor was used as a post-treatment to prevent methane being emitted from upflow anaerobic sludge blanket (UASB) effluents containing unrecovered dissolved methane. The performance of the closed DHS reactor was evaluated using real municipal sewage at ambient temperatures (10-28 °C) for one year. The first stage of the closed DHS reactor was intended to recover dissolved methane from the UASB effluent and produce a burnable gas with a methane concentration greater than 30%, and its recovery efficiency was 57-88%, although the amount of dissolved methane in the UASB effluent fluctuated in the range of 46-68 % of methane production greatly depending on the temperature. The residual methane was oxidized and the remaining organic carbon was removed in the second closed DHS reactor, and this reactor performed very well, removing more than 99% of the dissolved methane during the experimental period. The rate at which air was supplied to the DHS reactor was found to be one of the most important operating parameters. Microbial community analysis revealed that seasonal changes in the methane-oxidizing bacteria were key to preventing methane emissions. Copyright © 2014 Elsevier Ltd. All rights reserved.

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.

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

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

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.

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.

Wide area methane emissions mapping with airborne IPDA lidar

NASA Astrophysics Data System (ADS)

Bartholomew, Jarett; Lyman, Philip; Weimer, Carl; Tandy, William

2017-08-01

Methane emissions from natural gas production, storage, and transportation are potential sources of greenhouse gas emissions. Methane leaks also constitute revenue loss potential from operations. Since 2013, Ball Aerospace has been developing advanced airborne sensors using integrated path differential absorption (IPDA) LIDAR instrumentation to identify methane, propane, and longer-chain alkanes in the lowest region of the atmosphere. Additional funding has come from the U.S. Department of Transportation, Pipeline and Hazardous Materials Administration (PHMSA) to upgrade instrumentation to a broader swath coverage of up to 400 meters while maintaining high spatial sampling resolution and geolocation accuracy. Wide area coverage allows efficient mapping of emissions from gathering and distribution networks, processing facilities, landfills, natural seeps, and other distributed methane sources. This paper summarizes the benefits of advanced instrumentation for aerial methane emission mapping, describes the operating characteristics and design of this upgraded IPDA instrumentation, and reviews technical challenges encountered during development and deployment.

New Frontiers in Synthetic Biology for Spaceflight

NASA Technical Reports Server (NTRS)

Galazka, Jonathan M.

2017-01-01

Exploration of the solar system is constrained by the cost of moving mass off Earth. Producing materials in situ will reduce the mass that must be delivered from earth. CO2 is abundant on Mars and manned spacecraft. On the ISS, NASA reacts excess CO2 with H2 to generate CH4 and H2O using the Sabatier System. The resulting water is recovered into the ISS, but the methane is vented to space. Thus, there is a capability need for systems that convert methane into valuable materials. Methanotrophic bacteria consume methane but these are poor synthetic biology platforms. Thus, there is a knowledge gap in utilizing methane in a robust and flexible synthetic biology platform. The yeast Pichia pastoris is a refined microbial factory that is used widely by industry because it efficiently secretes products. Pichia could produce a variety of useful products in space. Pichia does not consume methane but robustly consumes methanol, which is one enzymatic step removed from methane. Our goal is to engineer Pichia to consume methane thereby creating a powerful methane-consuming microbial factory.

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.

Generation of methane from paddy fields and cattle in India, and its reduction at source

NASA Astrophysics Data System (ADS)

Bandyopadhyay, T. K.; Goyal, P.; Singh, M. P.

Methane (CH4) is a saturated organic gas. About 500 Tg yr -1 methane is generated globally. It is evident that 70% of the total emission have anthropogenic sources. The paddy fields contribute a significant portion of the total methane generated. About 20% of the total methane is generated from the paddy fields. In India, methane efflux rate is negative to 49 mg m -2 hr -1. The mean CH4 flux from Indian paddy fields is calculated to be 4.0 Tgyr -1. Livestock, and in particular ruminants are one of the important sources of methane emission on a global scale. There are two sources of methane emission from live stock: (1) from digestive process of ruminants, (2) from animal wastes. The estimated value of methane emission from digestive process of ruminants in India accounts for 6.47 Tgyr -1, and animal wastes accounts for 1.60 Tgyr -1. Total generation of methane from animals in India is about 8.0 Tg yr -1 . In paddy fields the key of controlling methane emission lies in the control of irrigation water. The methane emission can be decreased drastically if the field is under dry conditions for a few days at the end of tillering. In the case of livestock, reduction of methane emission can be done by (1) increasing the intake of the animal, (2) modifying the composition of the diet, (3) eliminating protozoa in rumen, (4) improving fibre digestion efficiency and (5) inhibiting activity of methanogenic bacteria.

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.

Anaerobic Biodegradation of Soybean Biodiesel and Diesel ...

EPA Pesticide Factsheets

Biotransformation of soybean biodiesel and the inhibitory effect of petrodiesel were studied under methanogenic conditions. Biodiesel removal efficiency of more than 95% was achieved in a chemostat with influent biodiesel concentrations up to 2.45 g/L. The kinetics of anaerobic biodegradation of soybean biodiesel B100 (biodiesel only) with different petrodiesel loads were studied using biomass pre-acclimated to B100 and B80 (80% biodiesel and 20 petrodiesel). The results indicated that the biodiesel fraction of the blend could be effectively biodegraded, whereas petrodiesel was not biodegraded at all under methanogenic conditions. The presence of petrodiesel in blends with biodiesel had a greater inhibitory effect on the rate of biodegradation than the biodegradation efficiency (defined as the efficiency of methane production). Both the biodegradation rate coefficient and the methane production efficiency increased almost linearly with the increasing fraction of biodiesel. With the increasing fraction of petrodiesel, the biodegradation rate and efficiency were correlated with the concentration of soluble FAMEs in the water. The objective of this study was to investigate the anaerobic biodegradation of soybean biodiesel blends under methanogenic conditions. Biological methane potential (BMP) tests were conducted in serum bottles to determine the anaerobic biodegradation kinetics of biodiesel in the absence and presence of different concentrations of petrod

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.

40 CFR 63.1426 - Process vent requirements for determining organic HAP concentration, control efficiency, and...

Code of Federal Regulations, 2011 CFR

2011-07-01

... National Emission Standards for Hazardous Air Pollutant Emissions for Polyether Polyols Production § 63... percent reduction may be measured as total epoxide, total organic HAP, or as TOC minus methane and ethane... TOC (minus methane and ethane) concentrations in all process vent streams and primary and secondary...

40 CFR 63.1426 - Process vent requirements for determining organic HAP concentration, control efficiency, and...

Code of Federal Regulations, 2012 CFR

2012-07-01

... National Emission Standards for Hazardous Air Pollutant Emissions for Polyether Polyols Production § 63... percent reduction may be measured as total epoxide, total organic HAP, or as TOC minus methane and ethane... TOC (minus methane and ethane) concentrations in all process vent streams and primary and secondary...

Berkeley Lab - Lawrence Berkeley National Laboratory

Science.gov Websites

nanoparticles that could make solar panels more efficient by converting light usually missed by solar cells into of Methane's Increasing Greenhouse Effect A Berkeley Lab research team tracked a rise in the warming effect of methane - one of the most important greenhouse gases for the Earth's atmosphere - over a 10

Significance of dissolved methane in effluents of anaerobically treated low strength wastewater and potential for recovery as an energy product: A review

EPA Science Inventory

The need for energy efficient Domestic Wastewater (DWW) treatment is increasing annually with population growth and expanding global energy demand. Anaerobic treatment of low strength DWW produces methane which can be used to as an energy product. Temperature sensitivity, low rem...

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.

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

Tailoring gas-phase CO2 electroreduction selectivity to hydrocarbons at Cu nanoparticles

NASA Astrophysics Data System (ADS)

Merino-Garcia, I.; Albo, J.; Irabien, A.

2018-01-01

Copper-based surfaces appear as the most active catalysts for CO2 electroreduction to hydrocarbons, even though formation rates and efficiencies still need to be improved. The aim of the present work is to evaluate the continuous gas-phase CO2 electroreduction to hydrocarbons (i.e. ethylene and methane) at copper nanoparticulated-based surfaces, paying attention to particle size influence (ranging from 25-80 nm) on reaction productivity, selectivity, and Faraday efficiency (FE) for CO2 conversion. The effect of the current density and the presence of a microporous layer within the working electrode are then evaluated. Copper-based gas diffusion electrodes are prepared by airbrushing the catalytic ink onto carbon supports, which are then coupled to a cation exchange membrane (Nafion) in a membrane electrode assembly. The results show that the use of smaller copper nanoparticles (25 nm) leads to a higher ethylene production (1148 μmol m-2 s-1) with a remarkable high FE (92.8%), at the same time, diminishing the competitive hydrogen evolution reaction in terms of FE. This work demonstrates the importance of nanoparticle size on reaction selectivity, which may be of help to design enhanced electrocatalytic materials for CO2 valorization to hydrocarbons.

The use of gaseous fuels mixtures for SI engines propulsion

NASA Astrophysics Data System (ADS)

Flekiewicz, M.; Kubica, G.

2016-09-01

Paper presents results of SI engine tests, carried on for different gaseous fuels. Carried out analysis made it possible to define correlation between fuel composition and engine operating parameters. Tests covered various gaseous mixtures: of methane and hydrogen and LPG with DME featuring different shares. The first group, considered as low carbon content fuels can be characterized by low CO2 emissions. Flammability of hydrogen added in those mixtures realizes the function of combustion process activator. That is why hydrogen addition improves the energy conversion by about 3%. The second group of fuels is constituted by LPG and DME mixtures. DME mixes perfectly with LPG, and differently than in case of other hydrocarbon fuels consists also of oxygen makes the stoichiometric mixture less oxygen demanding. In case of this fuel an improvement in engine volumetric and overall engine efficiency has been noticed, when compared to LPG. For the 11% DME share in the mixture an improvement of 2% in the efficiency has been noticed. During the tests standard CNG/LPG feeding systems have been used, what underlines utility value of the research. The stand tests results have been followed by combustion process simulation including exhaust forming and charge exchange.

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.

Mobile sensing of point-source fugitive methane emissions using Bayesian inference: the determination of the likelihood function

NASA Astrophysics Data System (ADS)

Zhou, X.; Albertson, J. D.

2016-12-01

Natural gas is considered as a bridge fuel towards clean energy due to its potential lower greenhouse gas emission comparing with other fossil fuels. Despite numerous efforts, an efficient and cost-effective approach to monitor fugitive methane emissions along the natural gas production-supply chain has not been developed yet. Recently, mobile methane measurement has been introduced which applies a Bayesian approach to probabilistically infer methane emission rates and update estimates recursively when new measurements become available. However, the likelihood function, especially the error term which determines the shape of the estimate uncertainty, is not rigorously defined and evaluated with field data. To address this issue, we performed a series of near-source (< 30 m) controlled methane release experiments using a specialized vehicle mounted with fast response methane analyzers and a GPS unit. Methane concentrations were measured at two different heights along mobile traversals downwind of the sources, and concurrent wind and temperature data are recorded by nearby 3-D sonic anemometers. With known methane release rates, the measurements were used to determine the functional form and the parameterization of the likelihood function in the Bayesian inference scheme under different meteorological conditions.

Effects of exogenous aerobic bacteria on methane production and biodegradation of municipal solid waste in bioreactors.

PubMed

Ge, Sai; Liu, Lei; Xue, Qiang; Yuan, Zhiming

2016-09-01

Landfill is the most common and efficient ways of municipal solid waste (MSW) disposal and the landfill biogas, mostly methane, is currently utilized to generate electricity and heat. The aim of this work is to study the effects and the role of exogenous aerobic bacteria mixture (EABM) on methane production and biodegradation of MSW in bioreactors. The results showed that the addition of EABM could effectively enhance hydrolysis and acidogenesis processes of MSW degradation, resulting in 63.95% reduction of volatile solid (VS), the highest methane production rate (89.83Lkg(-1) organic matter) ever recorded and a threefold increase in accumulative methane production (362.9L) than the control (127.1L). In addition, it is demonstrated that white-rot fungi (WRF) might further promote the methane production through highly decomposing lignin, but the lower pH value in leachate and longer acidogenesis duration may cause methane production reduced. The data demonstrated that methane production and biodegradation of MSW in bioreactors could be significantly enhanced by EABM via enhanced hydrolysis and acidogenesis processes, and the results are of great economic importance for the future design and management of landfill. Copyright © 2015 Elsevier Ltd. All rights reserved.

Ecological conversion efficiency and its influencers in twelve species of fish in the Yellow Sea Ecosystem

NASA Astrophysics Data System (ADS)

Tang, Qisheng; Guo, Xuewu; Sun, Yao; Zhang, Bo

2007-09-01

The ecological conversion efficiencies in twelve species of fish in the Yellow Sea Ecosystem, i.e., anchovy ( Engraulis japonicus), rednose anchovy ( Thrissa kammalensis), chub mackerel ( Scomber japonicus), halfbeak ( Hyporhamphus sajori), gizzard shad ( Konosirus punctatus), sand lance ( Ammodytes personatus), red seabream ( Pagrus major), black porgy ( Acanthopagrus schlegeli), black rockfish ( Sebastes schlegeli), finespot goby ( Chaeturichthys stigmatias), tiger puffer ( Takifugu rubripes), and fat greenling ( Hexagrammos otakii), were estimated through experiments conducted either in situ or in a laboratory. The ecological conversion efficiencies were significantly different among these species. As indicated, the food conversion efficiencies and the energy conversion efficiencies varied from 12.9% to 42.1% and from 12.7% to 43.0%, respectively. Water temperature and ration level are the main factors influencing the ecological conversion efficiencies of marine fish. The higher conversion efficiency of a given species in a natural ecosystem is acquired only under the moderate environment conditions. A negative relationship between ecological conversion efficiency and trophic level among ten species was observed. Such a relationship indicates that the ecological efficiency in the upper trophic levels would increase after fishing down marine food web in the Yellow Sea ecosystem.

Dynamics of the microbial community during continuous methane fermentation in continuously stirred tank reactors.

PubMed

Tang, Yue-Qin; Shigematsu, Toru; Morimura, Shigeru; Kida, Kenji

2015-04-01

Methane fermentation is an attractive technology for the treatment of organic wastes and wastewaters. However, the process is difficult to control, and treatment rates and digestion efficiency require further optimization. Understanding the microbiology mechanisms of methane fermentation is of fundamental importance to improving this process. In this review, we summarize the dynamics of microbial communities in methane fermentation chemostats that are operated using completely stirred tank reactors (CSTRs). Each chemostat was supplied with one substrate as the sole carbon source. The substrates include acetate, propionate, butyrate, long-chain fatty acids, glycerol, protein, glucose, and starch. These carbon sources are general substrates and intermediates of methane fermentation. The factors that affect the structure of the microbial community are discussed. The carbon source, the final product, and the operation conditions appear to be the main factors that affect methane fermentation and determine the structure of the microbial community. Understanding the structure of the microbial community during methane fermentation will guide the design and operation of practical wastewater treatments. Copyright © 2014 The Society for Biotechnology, Japan. Published by Elsevier B.V. All rights reserved.

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.

Dry anaerobic co-digestion of cow dung with pig manure for methane production.

PubMed

Li, Jianzheng; Jha, Ajay Kumar; Bajracharya, Tri Ratna

2014-07-01

The performance of dry anaerobic digestions of cow dung, pig manure, and their mixtures into different ratios were evaluated at 35 ± 1 °C in single-stage batch reactors for 63 days. The specific methane yields were 0.33, 0.37, 0.40, 0.38, 0.36, and 0.35 LCH4/gVSr for cow dung to pig manure ratios of 1:0, 4:1, 3:2, 2:3, 1:4, and 0:1, respectively, while volatile solid (VS) and chemical oxygen demand (COD) removal efficiencies were 48.59, 50.79, 53.20, 47.73, 46.10, and 44.88 % and 55.44, 57.96, 60.32, 56.96, 53.32, and 50.86 %, respectively. The experimental results demonstrated that the co-digestions resulted in 5.10-18.01 % higher methane yields, 2.03-12.95 % greater VS removals, 2.98-12.52 % greater COD degradation and so had positive synergism. The various mixtures of pig manure with cow dung might persuade a better nutrient balance and dilution of high ammonia concentration in pig manure and therefore enhanced digester performance efficiency and higher biogas yields. The dry co-digestion of 60 % cow dung and 40 % pig manure achieved the highest methane yield and the greatest organic materials removal efficiency than other mixtures and controls.

Performance evaluation of an anaerobic/aerobic landfill-based digester using yard waste for energy and compost production

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

Yazdani, Ramin, E-mail: ryazdani@sbcglobal.net; Civil and Environmental Engineering, University of California, One Shields Avenue, Ghausi Hall, Davis, CA 95616; Barlaz, Morton A., E-mail: barlaz@eos.ncsu.edu

2012-05-15

Highlights: Black-Right-Pointing-Pointer Biochemical methane potential decreased by 83% during the two-stage operation. Black-Right-Pointing-Pointer Net energy produced was 84.3 MWh or 46 kWh per million metric tons (Mg). Black-Right-Pointing-Pointer The average removal efficiency of volatile organic compounds (VOCs) was 96-99%. Black-Right-Pointing-Pointer The average removal efficiency of non-methane organic compounds (NMOCs) was 68-99%. Black-Right-Pointing-Pointer The two-stage batch digester proved to be simple to operate and cost-effective. - Abstract: The objective of this study was to evaluate a new alternative for yard waste management by constructing, operating and monitoring a landfill-based two-stage batch digester (anaerobic/aerobic) with the recovery of energy and compost. Themore » system was initially operated under anaerobic conditions for 366 days, after which the yard waste was aerated for an additional 191 days. Off gas generated from the aerobic stage was treated by biofilters. Net energy recovery was 84.3 MWh, or 46 kWh per million metric tons of wet waste (as received), and the biochemical methane potential of the treated waste decreased by 83% during the two-stage operation. The average removal efficiencies of volatile organic compounds and non-methane organic compounds in the biofilters were 96-99% and 68-99%, respectively.« less

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 Sensitivity to Perturbations in Tropospheric Oxidizing Capacity

NASA Technical Reports Server (NTRS)

Yegorova, Elena; Duncan, Bryan

2011-01-01

Methane is an important greenhouse gas and has a 25 times greater global warming potential than CO2 on a century timescale. Yet there are considerable uncertainties in the magnitude and variability of its sources and sinks. The response of the coupled non-linear methane-carbon monoxide-hydroxyl radical (OH) system is important in determining the tropospheric oxidizing capacity. Using the NASA Goddard Earth Observing System, Version 5 (GEOS-5) chemistry climate model, we study the response of methane to perturbations of OH and wetland emissions. We use a computationally-efficient option of the GEOS-5 CCM that includes an OH parameterization that accurately represents OH predicted by a full chemical mechanism. The OH parameterization allows for studying non-linear CH4-CO-OH feedbacks in computationally fast sensitivity experiments. We compare our results with surface observations (GMD) and discuss the range of uncertainty in OH and wetland emissions required to bring modeling results in better agreement with surface observations. Our results can be used to improve projections of methane emissions and methane growth.

Anaerobic co-digestion of acetate-rich with lignin-rich wastewater and the effect of hydrotalcite addition.

PubMed

Rodriguez-Chiang, Lourdes; Llorca, Jordi; Dahl, Olli

2016-10-01

The methane potential and biodegradability of different ratios of acetate and lignin-rich effluents from a neutral sulfite semi-chemical (NSSC) pulp mill were investigated. Results showed ultimate methane yields up to 333±5mLCH4/gCOD when only acetate-rich substrate was added and subsequently lower methane potentials of 192±4mLCH4/gCOD when the lignin fraction was increased. The presence of lignin showed a linear decay in methane production, resulting in a 41% decrease in methane when the lignin-rich feed had a 30% increase. A negative linear correlation between lignin content and biodegradability was also observed. Furthermore, the effect of hydrotalcite (HT) addition was evaluated and showed increase in methane potential of up to 8%, a faster production rate and higher soluble lignin removal (7-12% higher). Chemical oxygen demand (COD) removal efficiencies between 64 and 83% were obtained for all samples. Copyright © 2016 Elsevier Ltd. All rights reserved.

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

Oceanic methane hydrate: The character of the Blake Ridge hydrate stability zone, and the potential for methane extraction

USGS Publications Warehouse

Max, M.D.; Dillon, William P.

1998-01-01

Oceanic methane hydrates are mineral deposits formed from a crystalline 'ice' of methane and water in sea-floor sediments (buried to less than about 1 km) in water depths greater than about 500 m; economic hydrate deposits are probably restricted to water depths of between 1.5 km and 4 km. Gas hydrates increase a sediment's strength both by 'freezing' the sediment and by filling the pore spaces in a manner similar to water-ice in permafrost. Concentrated hydrate deposits may be underlain by significant volumes of methane gas, and these localities are the most favourable sites for methane gas extraction operations. Seismic reflection records indicate that trapped gas may blow-out naturally, causing large-scale seafloor collapse. In this paper, we consider both the physical properties and the structural integrity of the hydrate stability zone and the associated free gas deposits, with special reference to the Blake Ridge area, SE US offshore, in order to help establish a suitable framework for the safe, efficient, and economic recovery of methane from oceanic gas hydrates. We also consider the potential effects of the extraction of methane from hydrate (such as induced sea-floor faulting, gas venting, and gas-pocket collapse). We assess the ambient pressure effect on the production of methane by hydrate dissociation, and attempt to predict the likelihood of spontaneous gas flow in a production situation.Oceanic methane hydrates are mineral sits formed from a crystalline `ice' of methane and water in sea-floor sediments (buried to less than about 1 km) in water depths greater than about 500 m; economic hydrate deposits are probably restricted to water depths of between 1.5 km and 4 km. Gas hydrates increase a sediment's strength both by `freezing' the sediment and by filling the pore spaces in a manner similar to water-ice in permafrost. Concentrated hydrate deposits may be underlain by significant volumes of methane gas, and these localities are the most favourable sites for methane gas extraction operations. Seismic reflection records indicate that trapped gas may blow-out naturally, causing large-scale seafloor collapse. In this paper, we consider both the physical properties and the structural integrity of the hydrate stability zone and the associated free gas deposits, with special reference to the Blake Ridge area, SE US offshore, in order to help establish a suitable framework for the safe, efficient, and economic recovery of methane from oceanic gas hydrates. We also consider the potential effects of the extraction of methane from hydrate (such as induced sea-floor faulting, gas venting, and gas-pocket collapse). We assess the ambient pressure effect on the production of methane by hydrate dissociation, and attempt to predict the likelihood of spontaneous gas flow in a production situation.

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

NASA Technical Reports Server (NTRS)

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

2015-01-01

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

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

NASA Technical Reports Server (NTRS)

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

2016-01-01

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

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.

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

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

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.