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

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.

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.

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.

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.

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

USGS Publications Warehouse

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

2018-01-01

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

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

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

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.

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.

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

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

PubMed

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

2017-03-01

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

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

Plasma catalytic reforming of methane

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

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

1998-08-01

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

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.

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

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

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.

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.

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.

Renewable Natural Gas Clean-up Challenges and Applications

DTIC Science & Technology

2011-01-13

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

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

NASA Astrophysics Data System (ADS)

Khavarian, Mehrnoush; Mohamed, Abdul Rahman

2017-12-01

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

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.

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.

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

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.

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.

Dense ceramic membranes for converting methane to syngas

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

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

1995-07-01

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

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

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.

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

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

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.

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.

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%.

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

PubMed

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

2015-03-01

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

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

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.

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.

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.

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.

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

PubMed

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

2017-12-01

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

Raman studies of methane-ethane hydrate metastability.

PubMed

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

2009-03-05

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

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.

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.

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.

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

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.

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

Enzyme-Embedded, Microstructural Reactors for Industrial Biocatalysis

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

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

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

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.

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.

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.

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

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

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.

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

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.

Analysis of methane biodegradation by Methylosinus trichosporium OB3b

PubMed Central

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

2009-01-01

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

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

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

Anaerobic Digestion.

PubMed

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

2017-04-09

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

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.

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.

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.

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.

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

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

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.

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

Activation of methane by transition metal-substituted aluminophosphate molecular sieves

DOEpatents

Iton, Lennox E.; Maroni, Victor A.

1991-01-01

Aluminophosphate molecular sieves substituted with cobalt, manganese or iron and having the AlPO.sub.4 -34 or AlPO.sub.4 -5, or related AlPO.sub.4 structure activate methane starting at approximately 350.degree. C. Between 400.degree. and 500.degree. C. and at methane pressures .ltoreq.1 atmosphere the rate of methane conversion increases steadily with typical conversion efficiencies at 500.degree. C. approaching 50% and selectivity to the production of C.sub.2+ hydrocarbons approaching 100%. The activation mechanism is based on reduction of the transition metal(III) form of the molecular sieve to the transition metal(II) form with accompanying oxidative dehydrogenation of the methane. Reoxidation of the - transition metal(II) form to the transition metal(III) form can be done either chemically (e.g., using O.sub.2) or electrochemically.

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.

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.

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.

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.

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

PubMed Central

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

2016-01-01

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

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

PubMed

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

2016-02-01

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

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.

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

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.

Process for the conversion of carbonaceous feedstocks to particulate carbon and methanol

DOEpatents

Steinberg, Meyer; Grohse, Edward W.

1995-01-01

A process for the production of a pollutant-free particulate carbon (i.e., a substantially ash-, sulfur- and nitrogen-free carbon) from carbonaceous feedstocks. The basic process involves de-oxygenating one of the gas streams formed in a cyclic hydropyrolysis-methane pyrolysis process in order to improve conversion of the initial carbonaceous feedstock. De-oxygenation is effected by catalytically converting carbon monoxide, carbon dioxide, and hydrogen contained in one of the pyrolysis gas streams, preferably the latter, to a methanol co-product. There are thus produced two products whose use is known per se, viz., a substantially pollutant-free particulate carbon black and methanol. These products may be admixed in the form of a liquid slurry of carbon black in methanol.

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.

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

NASA Technical Reports Server (NTRS)

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

2017-01-01

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

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

NASA Technical Reports Server (NTRS)

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

1985-01-01

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

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.

The Reduction of Lunar Regolith by Carbothermal Processing Using Methane

NASA Technical Reports Server (NTRS)

Balasubramaniam, R.; Hegde, U.; Gokoglu, S.

2010-01-01

The processing of lunar regolith for the production of oxygen is a key component of the In-Situ Resource Utilization plans Currently being developed by NASA. In the carbothermal process, a portion of the surface of the regolith in a container is heated by exposure to a heat source so that a small zone of molten regolith is established. A continuous flow of methane is maintained over the molten regolith zone. In this paper, we discuss the development of a chemical conversion model of the carbothermal process to predict the rate of production of carbon monoxide. Our model is based on a mechanism where methane pyrolyzes when it comes in contact with the surface of the hot molten regolith to form solid carbon and hydrogen gas. Carbon is deposited on the surface of the melt, and hydrogen is released into the gas stream above the melt surface. We assume that the deposited carbon mixes in the molten regolith and reacts with metal oxides in a reduction reaction by which gaseous carbon monoxide is liberated. Carbon monoxide bubbles through the melt and is released into the gas stream. It is further processed downstream to ultimately produce oxygen.

The Reduction of Lunar Regolith by Carbothermal Processing Using Methane

NASA Technical Reports Server (NTRS)

Balasubramaniam, R.; Gokoglu, S. A.; Hegde, U.

2010-01-01

The processing of lunar regolith for the production of oxygen is a key component of the In-Situ Resource Utilization plans currently being developed by NASA. In the carbothermal process, a portion of the surface of the regolith in a container is heated by exposure to a heat source so that a small zone of molten regolith is established. A continuous flow of methane is maintained over the molten regolith zone. In this paper, we discuss the development of a chemical conversion model of the carbothermal process to predict the rate of production of carbon monoxide. Our model is based on a mechanism where methane pyrolyzes when it comes in contact with the surface of the hot molten regolith to form solid carbon and hydrogen gas. Carbon is deposited on the surface of the melt, and hydrogen is released into the gas stream above the melt surface. We assume that the deposited carbon mixes in the molten regolith and reacts with metal oxides in a reduction reaction by which gaseous carbon monoxide is liberated. Carbon monoxide bubbles through the melt and is released into the gas stream. It is further processed downstream to ultimately produce oxygen.

Sorption enhanced reaction process (SERP) for the production of hydrogen

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

Hufton, J.; Mayorga, S.; Gaffney, T.

1998-08-01

The novel Sorption Enhanced Reaction Process has the potential to decrease the cost of hydrogen production by steam methane reforming. Current effort for development of this technology has focused on adsorbent development, experimental process concept testing, and process development and design. A preferred CO{sub 2} adsorbent, K{sub 2}CO{sub 3} promoted hydrotalcite, satisfies all of the performance targets and it has been scaled up for process testing. A separate class of adsorbents has been identified which could potentially improve the performance of the H{sub 2}-SER process. Although this material exhibits improved CO{sub 2} adsorption capacity compared to the HTC adsorbent, itsmore » hydrothermal stability must be improved. Single-step process experiments (not cyclic) indicate that the H{sub 2}-SER reactor performance during the reaction step improves with decreasing pressure and increasing temperature and steam to methane ratio in the feed. Methane conversion in the H{sub 2}-SER reactor is higher than for a conventional catalyst-only reactor operated at similar temperature and pressure. The reactor effluent gas consists of 90+% H{sub 2}, balance CH{sub 4}, with only trace levels (< 50 ppm) of carbon oxides. A best-case process design (2.5 MMSCFD of 99.9+% H{sub 2}) based on the HTC adsorbent properties and a revised SER process cycle has been generated. Economic analysis of this design indicates the process has the potential to reduce the H{sub 2} product cost by 25--31% compared to conventional steam methane reforming.« less

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

PubMed Central

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

2013-01-01

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

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.

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

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.

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.

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

NASA Astrophysics Data System (ADS)

Pan, Wei

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

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.

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.

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

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.

Process for the conversion of carbonaceous feedstocks to particulate carbon and methanol

DOEpatents

Steinberg, M.; Grohse, E.W.

1995-06-27

A process is described for the production of a pollutant-free particulate carbon (i.e., a substantially ash-, sulfur- and nitrogen-free carbon) from carbonaceous feedstocks. The basic process involves de-oxygenating one of the gas streams formed in a cyclic hydropyrolysis-methane pyrolysis process in order to improve conversion of the initial carbonaceous feedstock. De-oxygenation is effected by catalytically converting carbon monoxide, carbon dioxide, and hydrogen contained in one of the pyrolysis gas streams, preferably the latter, to a methanol co-product. There are thus produced two products whose use is known per se, viz., a substantially pollutant-free particulate carbon black and methanol. These products may be admixed in the form of a liquid slurry of carbon black in methanol. 3 figs.

Determination of Chemical Kinetic Rate Constants of a Model for Carbothermal Processing of Lunar Regolith Simulant Using Methane

NASA Technical Reports Server (NTRS)

Balasubramaniam, R; Gokoglu, S.; Hegde, U.

2009-01-01

We have previously developed a chemical conversion model of the carbothermal processing of lunar regolith using methane to predict the rate of production of carbon monoxide. In this carbothermal process, gaseous methane is pyrolyzed as it flows over the hot surface of a molten zone of lunar regolith and is converted to carbon and hydrogen. Hydrogen is carried away by the exiting stream of gases and carbon is deposited on the melt surface. The deposited carbon mixes with the melt and reacts with the metal oxides in it to produce carbon monoxide that bubbles out of the melt. In our model, we assume that the flux of carbon deposited is equal to the product of the surface reaction rate constant gamma and the concentration of methane adjacent to the melt surface. Similarly, the rate of consumption of carbon per unit volume in the melt is equal to the product of the melt reaction rate constant k and the concentrations of carbon and metal oxide in the melt. In this paper, we describe our effort to determine gamma and k by comparison of the predictions from our model with test data obtained by ORBITEC (Orbital Technologies Corporation). The concentration of methane adjacent to the melt surface is a necessary input to the model. It is inferred from the test data by a mass balance of methane, adopting the usual assumptions of the continuously-stirred-tank-reactor model, whereby the average concentration of a given gaseous species equals its exit concentration. The reaction rates gamma and k have been determined by a non-linear least-squares fit to the test data for the production of carbon monoxide and the fraction of the incoming methane that is converted. The comparison of test data with our model predictions using the determined chemical kinetic rate constants provides a consistent interpretation of the process over the full range of temperatures, pressures, and methane flow rates used in the tests, thereby increasing our confidence to use the model for scale-up purposes.

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

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

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

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

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

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

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

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

PubMed

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

2017-05-01

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

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

DOE PAGES

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

2017-04-02

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

Methane production 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.

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.

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.

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.

Catalyst evaluation for high-purity H2 production by sorption-enhanced steam-methane reforming coupled to a Ca/Cu process

NASA Astrophysics Data System (ADS)

Navarro, M. V.; López, J. M.; García, T.; Grasa, G.; Murillo, R.

2017-09-01

The operational limits of a commercial nickel-based catalyst under the conditions of a sorption-enhanced steam-methane reforming process coupled to a Ca/Cu chemical loop are investigated for high-purity H2 production in a cyclic operation. The performance of the reforming catalyst is tested by means of a high number of oxidation-reduction-reforming cycles. After 100 oxidation-reduction cycles, this catalyst retains its exceptional reforming activity. The methane conversion values are close to the thermodynamic equilibrium under very demanding conditions: temperature between 500 °C - 700 °C and mass hourly space velocity of 8.8 kgCH4 h-1 kgcat-1. After 200 cycles, the sample shows reduction in its reforming activity in line with a lower dispersion of the Ni species. Sintering of Ni nanocrystals is evidenced during the oxidation-reduction multi-cycles. The performance of the catalyst after 200 oxidation-reduction cycles mixed with a CaO-based CO2 sorbent is studied under optimal conditions calculated for the sorption-enhanced reforming process coupled to a Ca/Cu cycle (temperature of 650 °C, steam/methane ratio of 4, sorbent/catalyst ratio of 4 and space velocity of 0.75 kgCH4 h-1 kgcat-1). Remarkably, an equilibrium value over 92 vol.% H2 concentration is achieved, highlighting this catalyst as a promising candidate for the next steps of the process development.

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.

Cobalt carbide nanoprisms for direct production of lower olefins from syngas

NASA Astrophysics Data System (ADS)

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

2016-10-01

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

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.

Efficient 1.6 Micron Laser Source for Methane DIAL

NASA Technical Reports Server (NTRS)

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

2013-01-01

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

Green plants as solar energy converters

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

Not Available

1976-06-01

A survey covers the potential of energy production from biomass and solid wastes; various processes for the combustion of wastes, such as the co-combustion of solid waste and sewage sludge at the St. Paul/Seneca Treatment Plant Sludge Incinerator; various biological processes for the conversion of solid wastes to fuel such as the Institute of Gas Technology 400 l. digestor for the biogasification of municipal solid waste and sewage solids to a methane-rich product gas; the use of industrial wastes for fuel, such as slash and mill residues used as fuel in lumber mills; the biogasification of animal wastes by usingmore » small-scale on-site digesters to produce methane gas for cooking and lighting; energy farming methods, such as growing giant California kelp, sargassum, and plankton as suitable feedstock for the production of methane, fertilizers, and food; problems, such as the possible alteration of the reflectivity of large areas of the earth's surface by rapidly growing plants raised for biomass; and benefits such as the reduction in air, water, and land pollution associated with the use of wastes and biomass grown especially for energy.« less

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

Code of Federal Regulations, 2013 CFR

2013-07-01

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

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

NASA Astrophysics Data System (ADS)

Endo, Ryosuke; Kitaya, Yoshiaki

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

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

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

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

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

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.

Optimization of semi-continuous anaerobic digestion of sugarcane straw co-digested with filter cake: Effects of macronutrients supplementation on conversion kinetics.

PubMed

Janke, Leandro; Weinrich, Sören; Leite, Athaydes F; Schüch, Andrea; Nikolausz, Marcell; Nelles, Michael; Stinner, Walter

2017-12-01

Anaerobic digestion of sugarcane straw co-digested with sugarcane filter cake was investigated with a special focus on macronutrients supplementation for an optimized conversion process. Experimental data from batch tests and a semi-continuous experiment operated in different supplementation phases were used for modeling the conversion kinetics based on continuous stirred-tank reactors. The semi-continuous experiment showed an overall decrease in the performance along the inoculum washout from the reactors. By supplementing nitrogen alone or in combination to phosphorus and sulfur the specific methane production significantly increased (P<0.05) by 17% and 44%, respectively. Although the two-pool one-step model has fitted well to the batch experimental data (R 2 >0.99), the use of the depicted kinetics did not provide a good estimation for process simulation of the semi-continuous process (in any supplementation phase), possibly due to the different feeding modes and inoculum source, activity and adaptation. Copyright © 2017 Elsevier Ltd. All rights reserved.

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.

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

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

Doan, Hieu A.; Li, Zhanyong; Farha, Omar K.

In this study, the prospect of using copper oxide nanoclusters grown by atomic layer deposition on a porphyrin support for selective oxidation of methane to methanol was examined by means of density functional theory (DFT) calculations. Ab initio thermodynamic analysis indicates that an active site in the form of Cu(μ-O)Cu can be stabilized by activation in O2 at 465K. Furthermore, a moderate methane activation energy barrier (Ea=54kJ/mol) is predicted, and the hydrogen abstraction activity of the active site could be attributed to the radical character of the bridging oxygen. Methanol extraction in this system is limited by a thermodynamic barriermore » to desorption of ΔG=57kJ/mol at 473K; however, desorption can be facilitated by the addition of water in a “stepped conversion” process. Overall, our results indicate similar activity between porphyrin-supported copper oxide nanoclusters and existing Cu-exchanged zeolites and provide a computational proof-of-concept for utilizing functionalized organic linkers in metal-organic frameworks (MOFs) for selective oxidation of methane to methanol.« less

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

DOE PAGES

Doan, Hieu A.; Li, Zhanyong; Farha, Omar K.; ...

2018-04-08

In this study, the prospect of using copper oxide nanoclusters grown by atomic layer deposition on a porphyrin support for selective oxidation of methane to methanol was examined by means of density functional theory (DFT) calculations. Ab initio thermodynamic analysis indicates that an active site in the form of Cu(μ-O)Cu can be stabilized by activation in O2 at 465K. Furthermore, a moderate methane activation energy barrier (Ea=54kJ/mol) is predicted, and the hydrogen abstraction activity of the active site could be attributed to the radical character of the bridging oxygen. Methanol extraction in this system is limited by a thermodynamic barriermore » to desorption of ΔG=57kJ/mol at 473K; however, desorption can be facilitated by the addition of water in a “stepped conversion” process. Overall, our results indicate similar activity between porphyrin-supported copper oxide nanoclusters and existing Cu-exchanged zeolites and provide a computational proof-of-concept for utilizing functionalized organic linkers in metal-organic frameworks (MOFs) for selective oxidation of methane to methanol.« less

Press fluid pre-treatment optimisation of the integrated generation of solid fuel and biogas from biomass (IFBB) process approach.

PubMed

Corton, John; Toop, Trisha; Walker, Jonathan; Donnison, Iain S; Fraser, Mariecia D

2014-10-01

The integrated generation of solid fuel and biogas from biomass (IFBB) system is an innovative approach to maximising energy conversion from low input high diversity (LIHD) biomass. In this system water pre-treated and ensiled LIHD biomass is pressed. The press fluid is anaerobically digested to produce methane that is used to power the process. The fibrous fraction is densified and then sold as a combustion fuel. Two process options designed to concentrate the press fluid were assessed to ascertain their influence on productivity in an IFBB like system: sedimentation and the omission of pre-treatment water. By concentrating press fluid and not adding water during processing, energy production from methane was increased by 75% per unit time and solid fuel productivity increased by 80% per unit of fluid produced. The additional energy requirements for pressing more biomass in order to generate equal volumes of feedstock were accounted for in these calculations. Copyright © 2014 Elsevier Ltd. All rights reserved.

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

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

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

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

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

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

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

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

2017-01-01

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

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.

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

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

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.

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.

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.

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.

Ammonia chemistry in a flameless jet

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

Zieba, Mariusz; Schuster, Anja; Scheffknecht, Guenter

2009-10-15

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

Method for in situ biological conversion of coal to methane

DOEpatents

Volkwein, Jon C.

1995-01-01

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

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

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.

Carbothermal Processing of Lunar Regolith Using Methane

NASA Technical Reports Server (NTRS)

Balasubramaniam, R.; Hegde, U.; Gokoglu, S.

2009-01-01

The processing of lunar regolith for the production of oxygen is a key component of the In-Situ Resource Utilization plans currently being developed by NASA. Among various candidate processes, the modeling of oxygen production by hydrogen reduction, molten salt electrolysis, and carbothermal processing are presently being pursued. In the carbothermal process, a portion of the surface of the regolith in a container is heated by exposure to a heat source such as a laser beam or a concentrated solar heat flux, so that a small zone of molten regolith is established. The molten zone is surrounded by solid regolith particles that are poor conductors of heat. A continuous flow of methane is maintained over the molten regolith zone. Our model is based on a mechanism where methane pyrolyzes when it comes in contact with the surface of the hot molten regolith to form solid carbon and hydrogen gas. Carbon is deposited on the surface of the melt, and hydrogen is released into the gas stream above the melt surface. We assume that the deposited carbon mixes in the molten regolith and reacts with metal oxides in a reduction reaction by which gaseous carbon monoxide is liberated. Carbon monoxide bubbles through the melt and is released into the gas stream. Oxygen is produced subsequently by (catalytically) processing the carbon monoxide downstream. In this paper, we discuss the development of a chemical conversion model of the carbothermal process to predict the rate of production of carbon monoxide.

Carbothermal Processing of Lunar Regolith Using Methane

NASA Technical Reports Server (NTRS)

Balasubramaniam, R.; Hegde, U.; Gokoglu, S.

2008-01-01

The processing of lunar regolith for the production of oxygen is a key component of the In-Situ Resource Utilization plans currently being developed by NASA. Among various candidate processes, the modeling of oxygen production by hydrogen reduction, molten salt electrolysis, and carbothermal processing are presently being pursued. In the carbothermal process, a portion of the surface of the regolith in a container is heated by exposure to a heat source such as a laser beam or a concentrated solar heat flux, so that a small zone of molten regolith is established. The molten zone is surrounded by solid regolith particles that are poor conductors of heat. A continuous flow of methane is maintained over the molten regolith zone. Our model is based on a mechanism where methane pyrolyzes when it comes in contact with the surface of the hot molten regolith to form solid carbon and hydrogen gas. Carbon is deposited on the surface of the melt, and hydrogen is released into the gas stream above the melt surface. We assume that the deposited carbon mixes in the molten regolith and reacts with metal oxides in a reduction reaction by which gaseous carbon monoxide is liberated. Carbon monoxide bubbles through the melt and is released into the gas stream. Oxygen is produced subsequently by (catalytically) processing the carbon monoxide downstream. In this paper, we discuss the development of a chemical conversion model of the carbothermal process to predict the rate of production of carbon monoxide.

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.

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.

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.

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.

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.

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.

Hybrid bioinorganic approach to solar-to-chemical conversion.

PubMed

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

2015-09-15

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

Hybrid bioinorganic approach to solar-to-chemical conversion

PubMed Central

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

2015-01-01

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

Control of GHG emission at the microbial community level.

PubMed

Insam, H; Wett, B

2008-01-01

All organic material eventually is decomposed by microorganisms, and considerable amounts of C and N end up as gaseous metabolites. The emissions of greenhouse relevant gases like carbon dioxide, methane and nitrous oxides largely depend on physico-chemical conditions like substrate quality or the redox potential of the habitat. Manipulating these conditions has a great potential for reducing greenhouse gas emissions. Such options are known from farm and waste management, as well as from wastewater treatment. In this paper examples are given how greenhouse gas production might be reduced by regulating microbial processes. Biogas production from manure, organic wastes, and landfills are given as examples how methanisation may be used to save fossil fuel. Methane oxidation, on the other hand, might alleviate the problem of methane already produced, or the conversion of aerobic wastewater treatment to anaerobic nitrogen elimination through the anaerobic ammonium oxidation process might reduce N2O release to the atmosphere. Changing the diet of ruminants, altering soil water potentials or a change of waste collection systems are other measures that affect microbial activities and that might contribute to a reduction of carbon dioxide equivalents being emitted to the atmosphere.

Anaerobic co-digestion of livestock and vegetable processing wastes: fibre degradation and digestate stability.

PubMed

Molinuevo-Salces, Beatriz; Gómez, Xiomar; Morán, Antonio; García-González, Mari Cruz

2013-06-01

Anaerobic digestion of livestock wastes (swine manure (SM) and poultry litter (PL)) and vegetable processing wastes (VPW) mixtures was evaluated in terms of methane yield, volatile solids removal and lignocellulosic material degradation. Batch experiments were performed with 2% VS (volatile solids) to ensure complete conversion of TVFAs (total volatile fatty acids) and to avoid ammonia inhibition. Experimental methane yields obtained for the mixtures resulted in higher values than those obtained from the sum of the methane yields from the individual components. VPW addition to livestock wastes before anaerobic digestion also resulted in improved VS elimination. In SM-VPW co-digestions, CH4 yield increased from 111 to 244 mL CH4 g VS added(-1), and the percentage of VS removed increased from 50% to 86%. For PL-VPW co-digestions, the corresponding values were increased from 158 to 223 mL CH4 g VS added(-1) and from 70% to 92% VS removed. Hemicelluloses and more than 50% of cellulose were degraded during anaerobic digestion. Thermal analyses indicated that the stabilization of the wastes during anaerobic digestion resulted in significantly less energy being released by digestate samples than fresh samples. Copyright © 2013 Elsevier Ltd. All rights reserved.

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.

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.

Microbial fuel cells: Running on gas

NASA Astrophysics Data System (ADS)

Ren, Zhiyong Jason

2017-06-01

Methane is an abundant energy source that is used for power generation in thermal power plants via combustion, but direct conversion to electricity in fuel cells remains challenging. Now, a microbial fuel cell is demonstrated to efficiently convert methane directly to current by careful selection of a consortium of microorganisms.

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.

Partial oxidation of methane by pulsed corona discharges

NASA Astrophysics Data System (ADS)

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

2014-09-01

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

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

PubMed

Grundner, Sebastian; Markovits, Monica A C; Li, Guanna; Tromp, Moniek; Pidko, Evgeny A; Hensen, Emiel J M; Jentys, Andreas; Sanchez-Sanchez, Maricruz; Lercher, Johannes A

2015-06-25

Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon-hydrogen bonds in methane and its subsequent transformation to methanol. The similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towards methanol, in both the enzyme system and copper-exchanged mordenite.

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.

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).

Giant seafloor craters formed by hydrate-controlled large-scale methane expulsion from the Arctic seafloor after ice sheet retreat

NASA Astrophysics Data System (ADS)

Andreassen, K.; Hubbard, A.; Patton, H.; Vadakkepuliyambatta, S.; Winsborrow, M.; Plaza-Faverola, A. A.; Serov, P.

2017-12-01

Large-scale methane releases from thawing Arctic gas hydrates is a major concern, yet the processes and fluxes involved remain elusive. We present geophysical data indicating two contrasting processes of natural methane emissions from the seafloor of the northern Barents Sea, Polar North Atlantic. Abundant gas flares, acoustically imaged in the water column reveal slow, gradual release of methane bubbles, a process that is commonly documented from nearby areas, elsewhere in the Arctic and along continental margins worldwide. Conversely, giant craters across the study area indicate a very different process. We propose that these are blow-out craters, formed through large-scale, abrupt methane expulsion induced when gas hydrates destabilized after the Barents Sea Ice Sheet retreated from the area. The data reveal over 100 giant seafloor craters within an area of 440 km2. These are up to 1000 m in diameter, 30 m deep and with a semi-circular to elliptical shape. We also identified numerous large seafloor mounds, which we infer to have formed by the expansion of gas hydrate accumulations within the shallow subsurface, so-called gas hydrate pingos. These are up to 1100 m wide and 20 m high. Smaller craters and mounds < 200 m wide and with varying relief are abundant across the study site. The empirical observations and analyses are combined with numerical modelling of ice sheet, isostatic and gas hydrate evolution and indicate that during glaciation, natural gas migrating from underlying hydrocarbon reservoirs was stored as subglacial gas hydrates. On ice sheet retreat, methane from these hydrate reservoirs and underlying free gas built up and abruptly released, forming the giant mounds and craters observed in the study area today. Petroleum basins are abundant beneath formerly and presently glaciated regions. We infer that episodes of subglacial sequestration of gas hydrates and underlying free gas and subsequent abrupt expulsions were common and widespread throughout Quaternary glacial cycles. The presented conceptual model for the evolution of giant craters can also serve as an analogue for future destabilization of glacially influenced hydrate reservoirs.

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.

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.

Nitrous oxide and methane emissions from different treatment processes in full-scale municipal wastewater treatment plants.

PubMed

Rena, Y G; Wang, J H; Li, H F; Zhang, J; Qi, P Y; Hu, Z

2013-01-01

Nitrous oxide (N2O) and methane (CH4) are two important greenhouse gases (GHG) emitted from biological nutrient removal (BNR) processes in municipal wastewater treatment plants (WWTP). In this study, three typical biological wastewater treatment processes were studied in WWTP of Northern China: pre-anaerobic carrousel oxidation ditch (A+OD) process, pre-anoxic anaerobic-anoxic-oxic (A-A/ A/O) process and reverse anaerobic-anoxic-oxic (r-A/ A/O) process. The N2O and CH4 emissions from these three different processes were measured in every processing unit of each WWTP. Results showed that N2O and CH4 were mainly discharged during the nitrification/denitrification process and the anaerobic/anoxic treatment process, respectively and the amounts of their formation and release were significantly influenced by different BNR processes implemented in these WWTP. The N2O conversion ratio of r-A/ A/O process was the lowest among the three WWTP, which were 10.9% and 18.6% lower than that of A-A/A/O process and A+OD process, respectively. Similarly, the CH4 conversion ratio of r-A/ A/O process was the lowest among the three WWTP, which were 89. I% and 80.8% lower than that of A-A/ A/O process and A+OD process, respectively. The factors influencing N2O and CH4 formation and emission in the three WWTP were investigated to explain the difference between these processes. The nitrite concentration and oxidation-reduction potential (ORP) value were found to be the dominant influencing factors affecting N2O and CH4 production, respectively. The flow-based emission factors of N2O and CH4 of the WWTP were figured out for better quantification of GHG emissions and further technical assessments of mitigation options.

Methane uptake in urban forests and lawns

Treesearch

Peter M. Groffman; Richard V. Pouyat

2009-01-01

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

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

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

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

1988-01-01

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

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

NASA Technical Reports Server (NTRS)

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

1974-01-01

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

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.

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

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

Wolf, E.E.

1996-09-30

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

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

DOE PAGES

Grundner, Sebastian; Markovits, Monica A. C.; Li, Guanna; ...

2015-06-25

Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane and its subsequent transformation to methanol. In conclusion, the similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towardsmore » methanol, in both the enzyme system and copper-exchanged mordenite.« less

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

PubMed Central

Grundner, Sebastian; Markovits, Monica A.C.; Li, Guanna; Tromp, Moniek; Pidko, Evgeny A.; Hensen, Emiel J.M.; Jentys, Andreas; Sanchez-Sanchez, Maricruz; Lercher, Johannes A.

2015-01-01

Copper-exchanged zeolites with mordenite structure mimic the nuclearity and reactivity of active sites in particulate methane monooxygenase, which are enzymes able to selectively oxidize methane to methanol. Here we show that the mordenite micropores provide a perfect confined environment for the highly selective stabilization of trinuclear copper-oxo clusters that exhibit a high reactivity towards activation of carbon–hydrogen bonds in methane and its subsequent transformation to methanol. The similarity with the enzymatic systems is also implied from the similarity of the reversible rearrangements of the trinuclear clusters occurring during the selective transformations of methane along the reaction path towards methanol, in both the enzyme system and copper-exchanged mordenite. PMID:26109507

Agriculture's impact on microbial diversity and associated fluxes of carbon dioxide and methane

PubMed Central

Levine, Uri Y; Teal, Tracy K; Robertson, G Philip; Schmidt, Thomas M

2011-01-01

Agriculture has marked impacts on the production of carbon dioxide (CO2) and consumption of methane (CH4) by microbial communities in upland soils—Earth's largest biological sink for atmospheric CH4. To determine whether the diversity of microbes that catalyze the flux of these greenhouse gases is related to the magnitude and stability of these ecosystem-level processes, we conducted molecular surveys of CH4-oxidizing bacteria (methanotrophs) and total bacterial diversity across a range of land uses and measured the in situ flux of CH4 and CO2 at a site in the upper United States Midwest. Conversion of native lands to row-crop agriculture led to a sevenfold reduction in CH4 consumption and a proportionate decrease in methanotroph diversity. Sites with the greatest stability in CH4 consumption harbored the most methanotroph diversity. In fields abandoned from agriculture, the rate of CH4 consumption increased with time along with the diversity of methanotrophs. Conversely, estimates of total bacterial diversity in soil were not related to the rate or stability of CO2 emission. These combined results are consistent with the expectation that microbial diversity is a better predictor of the magnitude and stability of processes catalyzed by organisms with highly specialized metabolisms, like CH4 oxidation, as compared with processes driven by widely distributed metabolic processes, like CO2 production in heterotrophs. The data also suggest that managing lands to conserve or restore methanotroph diversity could mitigate the atmospheric concentrations of this potent greenhouse gas. PMID:21490688

Catalyst and process for converting synthesis gas to liquid motor fuels

DOEpatents

Coughlin, Peter K.

1987-01-01

The addition of an inert metal component, such as gold, silver or copper, to a Fischer-Tropsch catalyst comprising cobalt enables said catalyst to convert synthesis gas to liquid motor fuels at about 240.degree.-370.degree. C. with advantageously reduced selectivity of said cobalt for methane in said conversion. The catalyst composition can advantageously include a support component, such as a molecular sieve, co-catalyst/support component or a combination of such support components.

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

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.

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.

Preparation of Pd supported on La(Sr)-Mn-O Perovskite by microwave Irradiation Method and Its Catalytic Performances for the Methane Combustion

PubMed Central

Wang, Wei; Yuan, Fulong; Niu, Xiaoyu; Zhu, Yujun

2016-01-01

In this work, a series of palladium supported on the La0.8Sr0.2MnO3.15 perovskite catalysts (Pd/LSM-x) with different Pd loading were prepared by microwave irradiation processing plus incipient wetness impregnation method and characterized by XRD, TEM, H2-TPR and XPS. These catalysts were evaluated on the lean CH4 combustion. The results show that the Pd/LSM-x samples prepared by microwave irradiation processing possess relative higher surface areas than LSM catalyst. The addition of Pd to the LSM leads to the increase in the oxygen vacancy content and the enhancement in the mobility of lattice oxygen which play an important role on the methane combustion. The Pd/LSM-3 catalysts with 4.2wt% Pd loading exhibited the best performance for CH4 combustion that temperature for 10% and 90% of CH4 conversion is 315 and 520 °C. PMID:26781628

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.

Conversion of crude oil to methane by a microbial consortium enriched from oil reservoir production waters

PubMed Central

Berdugo-Clavijo, Carolina; Gieg, Lisa M.

2014-01-01

The methanogenic biodegradation of crude oil is an important process occurring in petroleum reservoirs and other oil-containing environments such as contaminated aquifers. In this process, syntrophic bacteria degrade hydrocarbon substrates to products such as acetate, and/or H2 and CO2 that are then used by methanogens to produce methane in a thermodynamically dependent manner. We enriched a methanogenic crude oil-degrading consortium from production waters sampled from a low temperature heavy oil reservoir. Alkylsuccinates indicative of fumarate addition to C5 and C6 n-alkanes were identified in the culture (above levels found in controls), corresponding to the detection of an alkyl succinate synthase encoding gene (assA/masA) in the culture. In addition, the enrichment culture was tested for its ability to produce methane from residual oil in a sandstone-packed column system simulating a mature field. Methane production rates of up to 5.8 μmol CH4/g of oil/day were measured in the column system. Amounts of produced methane were in relatively good agreement with hydrocarbon loss showing depletion of more than 50% of saturate and aromatic hydrocarbons. Microbial community analysis revealed that the enrichment culture was dominated by members of the genus Smithella, Methanosaeta, and Methanoculleus. However, a shift in microbial community occurred following incubation of the enrichment in the sandstone columns. Here, Methanobacterium sp. were most abundant, as were bacterial members of the genus Pseudomonas and other known biofilm forming organisms. Our findings show that microorganisms enriched from petroleum reservoir waters can bioconvert crude oil components to methane both planktonically and in sandstone-packed columns as test systems. Further, the results suggest that different organisms may contribute to oil biodegradation within different phases (e.g., planktonic vs. sessile) within a subsurface crude oil reservoir. PMID:24829563

Anaerobic microbial redox processes in a landfill leachate contaminated aquifer (Grindsted, Denmark)

NASA Astrophysics Data System (ADS)

Ludvigsen, L.; Albrechtsen, H.-J.; Heron, G.; Bjerg, P. L.; Christensen, T. H.

1998-10-01

The distribution of anaerobic microbial redox processes was investigated along a 305 m long transect of a shallow landfill-leachate polluted aquifer. By unamended bioassays containing sediment and groundwater, 37 samples were investigated with respect to methane production, sulfate, iron, and manganese reduction, and denitrification. Methane production was restricted to the most reduced part of the plume with rates of 0.003-0.055 nmol CH 4/g dry weight/day. Sulfate reduction was observed at rates of maximum 1.8 nmol SO 42-/g dry weight/day along with methane production in the plume, but sulfate reduction was also observed further downgradient of the landfill. Iron reduction at rates of 5-19 nmol Fe(II)/g dry weight/day was observed in only a few samples, but this may be related to a high detection limit for the iron reducing bioassay. Manganese reduction at rates of maximum 2.4 nmol Mn(II)/g dry weight/day and denitrification at rates of 0.2-37 nmol N 2O-N/g dry weight/day were observed in the less reduced part of the plume. All the redox processes were microbial processes. In many cases, several redox processes took place simultaneously, but in all samples one process dominated accounting for more than 70% of the equivalent carbon conversion. The bioassays showed that the redox zones in the plume identified from the groundwater composition (e.g. as methanogenic and sulfate reducing) locally hosted also other redox processes (e.g. iron reduction). This may have implications for the potential of the redox zone to degrade trace amounts of organic chemicals and suggests that unamended bioassays may be an important supplement to other approaches in characterizing the redox processes in an anaerobic plume.

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.

Photodissociation of cyanoacetylene: Application to the atmospheric chemistry of Titan

NASA Technical Reports Server (NTRS)

Clarke, David W.; Ferris, James P.

1995-01-01

The quantum yield and reaction threshold for the photochemical dissociation of cyanoacetylene into a hydrogen atom and the cyanoethynyl radical have been determined. The quantum yield at 185 nm is approximately 0.09. The threshold is approximately 240 nm. Combination of this data with literature values shows that production of excited-state cyanoacetylene is the major primary process resulting from irradiation between 185 and 254 nm. Also determined are the relative rate constants for the abstraction of a hydrogen atom from hydrogen, methane, and ethane by the cyanoethynyl radical (k(H2):k(CH4):k(C2H6) = 1:9.3:63). Implications of these results for the proposal that hydrogen abstraction plays an important role in the conversion of methane to ethane and in the protection of unsaturated compounds from photoconsumption in the atmosphere of Titan are discussed.

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

NASA Astrophysics Data System (ADS)

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

2015-05-01

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

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.

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

Applications of de-oiled microalgal biomass towards development of sustainable biorefinery.

PubMed

Maurya, Rahulkumar; Paliwal, Chetan; Ghosh, Tonmoy; Pancha, Imran; Chokshi, Kaumeel; Mitra, Madhusree; Ghosh, Arup; Mishra, Sandhya

2016-08-01

In view of commercialization of microalgal biofuel, the de-oiled microalgal biomass (DMB) is a surplus by-product in the biorefinery process that needs to be exploited to make the process economically attractive and feasible. This DMB, rich in carbohydrates, proteins, and minerals, can be used as feed, fertilizer, and substrate for the production of bioethanol/bio-methane. Further, thermo-chemical conversion of DMB results into fuels and industrially important chemicals. Future prospects of DMB also lie with its conversion into novel biomaterials like nanoparticles and carbon-dot which have biomedical importance. The lowest valued application of DMB is to use it for adsorption of dyes and heavy metals from industrial effluents. This study reviews how DMB can be utilized for different applications and in the generation of valuable co-products. The value addition of DMB would thereby improve the overall cost economics of the microalgal bio-refinery. Copyright © 2016 Elsevier Ltd. All rights reserved.

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.

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.

Interaction of Microbial and Abiotic Processes in Soil Leading to the (Bio)Conversion and Ultimate Attenuation of New Insensitive Munitions Compounds

DTIC Science & Technology

2016-12-30

Toxicity is expressed as percentage of toxicant- free activity 125 Figure 4.12-1. Panel A: (Bio)transformation pathways of DNAN in anaerobic incubations...O-demethylation of the methoxy group was confirmed by formation of formaldehye. Cell free extracts of the Bacillus culture yielded formation of 2...periodically until the production of methane became constant in the toxicant- free controls. The maximum specific methanogenic activity of the

Investigation of Redox Metal Oxides for Carbonaceous Fuel Conversion and CO2 Capture

NASA Astrophysics Data System (ADS)

Galinsky, Nathan Lee

The chemical looping combustion (CLC) process uses metal oxides, also referred to as oxygen carriers, in a redox scheme for conversion of carbonaceous fuels into a concentrated stream of CO2 and steam while also producing heat and electricity. The unique redox scheme of CLC allows CO2 capture with minimal energy penalty. The CLC process performance greatly depends on the oxygen carrier that is chosen. To date, more than 1000 oxygen carriers have been developed for chemical-looping processes using metal oxides containing first-row transition metals. Oxygen carriers are typically mixed with an inert ceramic support to improve their overall mechanical stability and recyclability. This study focuses on design of (i) iron oxide oxygen carriers for conversion of gaseous carbonaceous fuels and (ii) development of perovskite CaMnO 3-d with improved stability and redox properties for conversion of solid fuels. Iron oxide is cheap and environmentally benign. However, it suffers from low activity with carbonaceous fuels due partially to the low ionic conductivity of iron oxides. In order to address the low activity of iron-oxide-based oxygen carriers, support addition has been shown to lower the energy barrier of oxygen anion transport within the oxygen carrier. This work adds a mixed-ionic-and-electronic-conductor (MIEC) support to iron oxide to help facilitate O2- transport inside the lattice of iron oxide. The MIEC-supported iron oxide is compared to commonly used supports including TiO2 and Al2O 3 and the pure ionic conductor support yttria-stabilized zirconia (YSZ) for conversion of different carbonaceous fuels and hydrogen. Results show that the MIEC-supported iron oxide exhibits up to 70 times higher activity than non-MIEC-supported iron oxides for methane conversion. The MIEC supported iron oxide also shows good recyclability with only minor agglomeration and carbon formation observed. The effect of support-iron oxide synergies is further investigated to understand other physical and chemical properties that lead to highly active and recyclable oxygen carriers. Perovskite and fluorite-structured MIEC supports are tested for conversion of methane. The perovskite supported iron oxides exhibit higher activity and stability resulting from the high mixed conductivity of the support. Fluorite-structured CeO2 oxygen carriers deactivated by 75% after 10 redox cycles. This deactivation was attributed to agglomeration of iron oxide. The agglomeration was determined to occur due to Fe x+ transport during the oxidation step leading to high content of Fe on the surface of the oxygen carrier. Besides the MIEC supports, inert MgAl2O4 supported iron oxide is observed to activate in methane. The activation is attributed to carbon formation causing physical degradation of the oxygen carrier and leading to higher surface area and porosity. To achieve high activity with solid fuels, chemical looping with oxygen uncoupling (CLOU) is commonly used. This process uses oxygen carriers with high PO2 that allows the oxygen carrier to release a portion of their lattice oxygen as gaseous oxygen. In turn, the gaseous oxygen can react with solid fuel particles at a higher rate than the lattice oxygen. CaMnO 3 perovskite oxygen carriers offer high potential for CLOU. However, pure CaMnO3 suffers from long-term recyclability and sulfur poisoning. Addition of A-site (Ba and Sr) and B-site (Fe, Ni, Co, Al, and V) dopants are used to improve the performance of the base CaMnO3 oxygen carrier. Sr (A-site) and Fe (B-site) exhibit high compatibility with the base perovskite structure. Both dopants observe oxygen uncoupling properties up to 200°C below that of pure CaMnO3. Additionally, the doped structures also exhibit higher stability at high temperatures (>1000°C) and during redox cycles. The doped oxygen carriers also demonstrate significantly improved activity for coal char conversion.

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.

Implementation and process analysis of pilot scale multi-phase anaerobic fermentation and digestion of faecal sludge in Ghana

PubMed Central

Shih, Justin; Fanyin-Martin, Ato; Taher, Edris; Chandran, Kartik

2017-01-01

Background.  In Ghana, faecal sludge (FS) from on-site sanitation facilities is often discharged untreated into the environment, leading to significant insults to environmental and human health. Anaerobic digestion offers an attractive pathway for FS treatment with the concomitant production of energy in the form of methane. Another innovative option includes separating digestion into acidogenesis (production of volatile fatty acids (VFA)) and methanogenesis (production of methane), which could ultimately facilitate the production of an array of biofuels and biochemicals from the VFA. This work describes the development, implementation and modeling based analysis of a novel multiphase anaerobic fermentation-digestion process aimed at FS treatment in Kumasi, Ghana.  Methods.  A pilot-scale anaerobic fermentation process was implemented at the Kumasi Metropolitan Assembly’s Oti Sanitary Landfill Site at Adanse Dompoase.  The process consisted of six 10 m reactors in series, which were inoculated with bovine rumen and fed with fecal sludge obtained from public toilets.  The performance of the fermentation process was characterized in terms of both aqueous and gaseous variables representing the conversion of influent organic carbon to VFA as well as CH 4.  Using the operating data, the first-ever process model for FS fermentation and digestion was developed and calibrated, based on the activated sludge model framework. Results and Conclusions.  This work represents one of the first systematic efforts at integrated FS characterization and process modeling to enable anaerobic fermentation and digestion of FS. It is shown that owing to pre-fermentation of FS in public septage holding tanks, one could employ significantly smaller digesters (lower capital costs) or increased loading capabilities for FS conversion to biogas or VFA. Further, using the first-ever calibrated process model for FS fermentation and digestion presented herein, we expect improved and more mechanistically informed development and application of different process designs and configurations for global FS management practice. PMID:29528044

Implementation and process analysis of pilot scale multi-phase anaerobic fermentation and digestion of faecal sludge in Ghana.

PubMed

Shih, Justin; Fanyin-Martin, Ato; Taher, Edris; Chandran, Kartik

2017-11-06

Background.  In Ghana, faecal sludge (FS) from on-site sanitation facilities is often discharged untreated into the environment, leading to significant insults to environmental and human health. Anaerobic digestion offers an attractive pathway for FS treatment with the concomitant production of energy in the form of methane. Another innovative option includes separating digestion into acidogenesis (production of volatile fatty acids (VFA)) and methanogenesis (production of methane), which could ultimately facilitate the production of an array of biofuels and biochemicals from the VFA. This work describes the development, implementation and modeling based analysis of a novel multiphase anaerobic fermentation-digestion process aimed at FS treatment in Kumasi, Ghana.  Methods.  A pilot-scale anaerobic fermentation process was implemented at the Kumasi Metropolitan Assembly's Oti Sanitary Landfill Site at Adanse Dompoase.  The process consisted of six 10 m reactors in series, which were inoculated with bovine rumen and fed with fecal sludge obtained from public toilets.  The performance of the fermentation process was characterized in terms of both aqueous and gaseous variables representing the conversion of influent organic carbon to VFA as well as CH 4 .  Using the operating data, the first-ever process model for FS fermentation and digestion was developed and calibrated, based on the activated sludge model framework. Results and Conclusions.  This work represents one of the first systematic efforts at integrated FS characterization and process modeling to enable anaerobic fermentation and digestion of FS. It is shown that owing to pre-fermentation of FS in public septage holding tanks, one could employ significantly smaller digesters (lower capital costs) or increased loading capabilities for FS conversion to biogas or VFA. Further, using the first-ever calibrated process model for FS fermentation and digestion presented herein, we expect improved and more mechanistically informed development and application of different process designs and configurations for global FS management practice.

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.

Catalyst and process development for synthesis gas conversion to isobutylene. Final report, September 1, 1990--January 31, 1994

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

Anthony, R.G.; Akgerman, A.

1994-05-06

Previous work on isosynthesis (conversion of synthesis gas to isobutane and isobutylene) was performed at very low conversions or extreme process conditions. The objectives of this research were (1) determine the optimum process conditions for isosynthesis; (2) determine the optimum catalyst preparation method and catalyst composition/properties for isosynthesis; (3) determine the kinetics for the best catalyst; (4) develop reactor models for trickle bed, slurry, and fixed bed reactors; and (5) simulate the performance of fixed bed trickle flow reactors, slurry flow reactors, and fixed bed gas phase reactors for isosynthesis. More improvement in catalyst activity and selectivity is needed beforemore » isosynthesis can become a commercially feasible (stand-alone) process. Catalysts prepared by the precipitation method show the most promise for future development as compared with those prepared hydrothermally, by calcining zirconyl nitrate, or by a modified sol-gel method. For current catalysts the high temperatures (>673 K) required for activity also cause the production of methane (because of thermodynamics). A catalyst with higher activity at lower temperatures would magnify the unique selectivity of zirconia for isobutylene. Perhaps with a more active catalyst and acidification, oxygenate production could be limited at lower temperatures. Pressures above 50 atm cause an undesirable shift in product distribution toward heavier hydrocarbons. A model was developed that can predict carbon monoxide conversion an product distribution. The rate equation for carbon monoxide conversion contains only a rate constant and an adsorption equilibrium constant. The product distribution was predicted using a simple ratio of the rate of CO conversion. This report is divided into Introduction, Experimental, and Results and Discussion sections.« less

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.

PEaCH4 v.2.0: A modelling platform to predict early diagenetic processes in marine sediments with a focus on biogenic methane - Case study: Offshore Namibia

NASA Astrophysics Data System (ADS)

Arning, Esther T.; Häußler, Steffen; van Berk, Wolfgang; Schulz, Hans-Martin

2016-07-01

The modelling of early diagenetic processes in marine sediments is of interest in marine science, and in the oil and gas industry, here, especially with respect to methane occurrence and gas hydrate formation as resources. Early diagenesis in marine sediments evolves from a complex web of intertwining (bio)geochemical reactions. It comprises microbially catalysed reactions and inorganic mineral-water-gas interactions. A model that will describe and consider all of these reactions has to be complex. However, it should be user-friendly, as well as to be applicable for a broad community and not only for experts in the field of marine chemistry. The presented modelling platform PeaCH4 v.2.0 combines both aspects, and is Microsoft Excel©-based. The modelling tool is PHREEQC (version 2), a computer programme for speciation, batch-reaction, one-dimensional transport, and inverse geochemical calculations. The conceptual PEaCH4 model is based on the conversion of sediment-bound degradable organic matter. PEaCH4 v.2.0 was developed to quantify and predict early diagenetic processes in marine sediments with the focus on biogenic methane formation and its phase behaviour, and allows carbon mass balancing. In regard to the irreversible degradation of organic matter, it comprises a "reaction model" and a "kinetic model" to predict methane formation. Both approaches differ in their calculations and outputs as the "kinetic model" considers the modelling time to integrate temperature dependent biogenic methane formation in its calculations, whereas the "reaction model" simply relies on default organic matter degradation. With regard to the inorganic mineral-water-gas interactions, which are triggered by irreversible degradation of organic matter, PEaCH4 v.2.0 is based on chemical equilibrium thermodynamics, appropriate mass-action laws, and their temperature dependent equilibrium constants. The programme is exemplarily presented with the example of upwelling sediments off Namibia, ODP Leg 175, Site 1082. The application demonstrates that the modelling platform PEaCH4 v.2.0 provides a user-friendly, but complex scientific tool that delivers retraceable information about early diagenetic processes and products in marine sediments.

Process for the production of ethylene and other hydrocarbons from coal

DOEpatents

Steinberg, M.; Fallon, P.

1984-02-15

The subject invention comprises the steps of first reacting particulate coal with methane at a temperature in the approximate range of 500/sup 0/C to 1100/sup 0/C and at a partial pressure of methane of less than about 200 psig for a period of less than 10 seconds. More preferably, the method of the subject invention is carried out at a temperature of approximately 850/sup 0/C to 1000/sup 0/C and a pressure of 50 psig for a period of approximately 1.5 seconds. Surprisingly, it has been found that in the practice of the subject invention not only are commercially significant quantities of ethylene produced, namely yields in excess of 10% (percent carbon converted to product), along with economically significant quantities of-benzene and light oils, namely toluene and xylene, but also that there is little, if any, net consumption of methane in the reaction and possibly even a small net production. Since it is apparent that the carbonaceous solids or char remaining after the reaction is carried out may be burned to provide the necessary energy to carry out the process of the subject invention, it is apparent that the subject invention advantageously provides a method for the conversion of coal to economically significant quantities of ethylene, benzene and light oils while requiring only coal and, possibly, small amounts of make-up methane. Other objects and advantages of the subject invention will be apparent to those skilled in the art from a consideration of the attached drawings, the detailed description of the invention, and the experimental examples set forth below.

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.

Microbial Ecology of Thermophilic Anaerobic Digestion. Final Report

DOE R&D Accomplishments Database

Zinder, Stephen H.

2000-04-15

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

Microwave Hydrogen Production from Methane

DTIC Science & Technology

2012-04-01

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

Fair Oaks Dairy Farms Cellulosic Ethanol Technology Review Summary

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

Andrew Wold; Robert Divers

2011-06-23

At Fair Oaks Dairy, dried manure solids (''DMS'') are currently used as a low value compost. United Power was engaged to evaluate the feasibility of processing these DMS into ethanol utilizing commercially available cellulosic biofuels conversion platforms. The Fair Oaks Dairy group is transitioning their traditional ''manure to methane'' mesophilic anaerobic digester platform to an integrated bio-refinery centered upon thermophilic digestion. Presently, the Digested Manure Solids (DMS) are used as a low value soil amendment (compost). United Power evaluated the feasibility of processing DMS into higher value ethanol utilizing commercially available cellulosic biofuels conversion platforms. DMS was analyzed and overmore » 100 potential technology providers were reviewed and evaluated. DMS contains enough carbon to be suitable as a biomass feedstock for conversion into ethanol by gasification technology, or as part of a conversion process that would include combined heat and power. In the first process, 100% of the feedstock is converted into ethanol. In the second process, the feedstock is combusted to provide heat to generate electrical power supporting other processes. Of the 100 technology vendors evaluated, a short list of nine technology providers was developed. From this, two vendors were selected as finalists (one was an enzymatic platform and one was a gasification platform). Their selection was based upon the technical feasibility of their systems, engineering expertise, experience in commercial or pilot scale operations, the ability or willingness to integrate the system into the Fair Oaks Biorefinery, the know-how or experience in producing bio-ethanol, and a clear path to commercial development.« less

Synthesis gas production by mixed conducting membranes with integrated conversion into liquid products

DOEpatents

Nataraj, Shankar; Russek, Steven Lee; Dyer, Paul Nigel

2000-01-01

Natural gas or other methane-containing feed gas is converted to a C.sub.5 -C.sub.19 hydrocarbon liquid in an integrated system comprising an oxygenative synthesis gas generator, a non-oxygenative synthesis gas generator, and a hydrocarbon synthesis process such as the Fischer-Tropsch process. The oxygenative synthesis gas generator is a mixed conducting membrane reactor system and the non-oxygenative synthesis gas generator is preferably a heat exchange reformer wherein heat is provided by hot synthesis gas product from the mixed conducting membrane reactor system. Offgas and water from the Fischer-Tropsch process can be recycled to the synthesis gas generation system individually or in combination.

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.

Abundant carbon substrates drive extremely high sulfate reduction rates and methane fluxes in Prairie Pothole Wetlands.

PubMed

Dalcin Martins, Paula; Hoyt, David W; Bansal, Sheel; Mills, Christopher T; Tfaily, Malak; Tangen, Brian A; Finocchiaro, Raymond G; Johnston, Michael D; McAdams, Brandon C; Solensky, Matthew J; Smith, Garrett J; Chin, Yu-Ping; Wilkins, Michael J

2017-08-01

Inland waters are increasingly recognized as critical sites of methane emissions to the atmosphere, but the biogeochemical reactions driving such fluxes are less well understood. The Prairie Pothole Region (PPR) of North America is one of the largest wetland complexes in the world, containing millions of small, shallow wetlands. The sediment pore waters of PPR wetlands contain some of the highest concentrations of dissolved organic carbon (DOC) and sulfur species ever recorded in terrestrial aquatic environments. Using a suite of geochemical and microbiological analyses, we measured the impact of sedimentary carbon and sulfur transformations in these wetlands on methane fluxes to the atmosphere. This research represents the first study of coupled geochemistry and microbiology within the PPR and demonstrates how the conversion of abundant labile DOC pools into methane results in some of the highest fluxes of this greenhouse gas to the atmosphere ever reported. Abundant DOC and sulfate additionally supported some of the highest sulfate reduction rates ever measured in terrestrial aquatic environments, which we infer to account for a large fraction of carbon mineralization in this system. Methane accumulations in zones of active sulfate reduction may be due to either the transport of free methane gas from deeper locations or the co-occurrence of methanogenesis and sulfate reduction. If both respiratory processes are concurrent, any competitive inhibition of methanogenesis by sulfate-reducing bacteria may be lessened by the presence of large labile DOC pools that yield noncompetitive substrates such as methanol. Our results reveal some of the underlying mechanisms that make PPR wetlands biogeochemical hotspots, which ultimately leads to their critical, but poorly recognized role in regional greenhouse gas emissions. © 2017 John Wiley & Sons Ltd.

Abundant carbon substrates drive extremely high sulfate reduction rates and methane fluxes in Prairie Pothole Wetlands

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

Dalcin Martins, Paula; Hoyt, David W.; Bansal, Sheel

Inland waters are increasingly recognized as critical sites of methane emissions to the atmosphere, but the biogeochemical reactions driving such fluxes are less well understood. The Prairie Pothole Region (PPR) of North America is one of the largest wetland complexes in the world, containing millions of small, shallow wetlands. The sediment pore waters of PPR wetlands contain some of the highest concentrations of dissolved organic carbon (DOC) and sulfur species ever recorded in terrestrial aquatic environments. Using a suite of geochemical and microbiological analyses we measured the impact of sedimentary carbon and sulfur transformations in these wetlands on methane fluxesmore » to the atmosphere. This research represents the first study of coupled geochemistry and microbiology within the PPR, and demonstrates how the conversion of abundant labile DOC pools into methane results in some of the highest fluxes of this greenhouse gas to the atmosphere ever reported. Abundant DOC and sulfate additionally supported some of the highest sulfate reduction rates ever measured in terrestrial aquatic environments, which we infer to account for a large fraction of carbon mineralization in this system. Methane accumulations in zones of active sulfate reduction may be due to either the transport of free methane gas from deeper locations, or the co-occurrence of methanogenesis and sulfate reduction. If both respiratory processes are concurrent, any competitive inhibition of methanogenesis by sulfate-reducing bacteria may be lessened by the presence of large labile DOC pools that yield non-competitive substrates such as methanol. Our results reveal some of the underlying mechanisms that make PPR wetlands biogeochemical hotspots, which ultimately leads to their critical, but poorly recognized role in regional greenhouse gas emissions.« less

Abundant carbon substrates drive extremely high sulfate reduction rates and methane fluxes in Prairie Pothole Wetlands

USGS Publications Warehouse

Martins, Paula; Hoyt, David W.; Bansal, Sheel; Mills, Christopher T.; Tfaily, Malak; Tangen, Brian; Finocchiaro, Raymond; Johnston, Michael D.; McAdams, Brandon C.; Solensky, Matthew J.; Smith, Garrett J.; Chin, Yu-Ping; Wilkins, Michael J.

2017-01-01

Inland waters are increasingly recognized as critical sites of methane emissions to the atmosphere, but the biogeochemical reactions driving such fluxes are less well understood. The Prairie Pothole Region (PPR) of North America is one of the largest wetland complexes in the world, containing millions of small, shallow wetlands. The sediment pore waters of PPR wetlands contain some of the highest concentrations of dissolved organic carbon (DOC) and sulfur species ever recorded in terrestrial aquatic environments. Using a suite of geochemical and microbiological analyses, we measured the impact of sedimentary carbon and sulfur transformations in these wetlands on methane fluxes to the atmosphere. This research represents the first study of coupled geochemistry and microbiology within the PPR and demonstrates how the conversion of abundant labile DOC pools into methane results in some of the highest fluxes of this greenhouse gas to the atmosphere ever reported. Abundant DOC and sulfate additionally supported some of the highest sulfate reduction rates ever measured in terrestrial aquatic environments, which we infer to account for a large fraction of carbon mineralization in this system. Methane accumulations in zones of active sulfate reduction may be due to either the transport of free methane gas from deeper locations or the co-occurrence of methanogenesis and sulfate reduction. If both respiratory processes are concurrent, any competitive inhibition of methanogenesis by sulfate-reducing bacteria may be lessened by the presence of large labile DOC pools that yield noncompetitive substrates such as methanol. Our results reveal some of the underlying mechanisms that make PPR wetlands biogeochemical hotspots, which ultimately leads to their critical, but poorly recognized role in regional greenhouse gas emissions.

An Effective Method to Detect Volatile Intermediates Generated in the Bioconversion of Coal to Methane by Gas Chromatography-Mass Spectrometry after In-Situ Extraction Using Headspace Solid-Phase Micro-Extraction under Strict Anaerobic Conditions.

PubMed

Liu, Jianmin; Wang, Baoyu; Tai, Chao; Wu, Li; Zhao, Han; Guan, Jiadong; Chen, Linyong

2016-01-01

Bioconversion of coal to methane has gained increased attention in recent decades because of its economic and environmental advantages. However, the mechanism of this process is difficult to study in depth, partly because of difficulties associated with the analysis of intermediates generated in coal bioconversion. In this investigation, we report on an effective method to analyze volatile intermediates generated in the bioconversion of coal under strict anaerobic conditions. We conduct in-situ extraction of intermediates using headspace solid-phase micro-extraction followed by detection by gas chromatography-mass spectrometry. Bioconversion simulation equipment was modified and combined with a solid-phase micro-extraction device. In-situ extraction could be achieved by using the combined units, to avoid a breakdown in anaerobic conditions and to maintain the experiment continuity. More than 30 intermediates were identified qualitatively in the conversion process, and the variation in trends of some typical intermediates has been discussed. Volatile organic acids (C2-C7) were chosen for a quantitative study of the intermediates because of their importance during coal bioconversion to methane. Fiber coating, extraction time, and solution acidity were optimized in the solid-phase micro-extraction procedure. The pressure was enhanced during the bioconversion process to investigate the influence of headspace pressure on analyte extraction. The detection limits of the method ranged from 0.0006 to 0.02 mmol/L for the volatile organic acids and the relative standard deviations were between 4.6% and 11.5%. The volatile organic acids (C2-C7) generated in the bioconversion process were 0.01-1.15 mmol/L with a recovery range from 80% to 105%. The developed method is useful for further in-depth research on the bioconversion of coal to methane.

An Effective Method to Detect Volatile Intermediates Generated in the Bioconversion of Coal to Methane by Gas Chromatography-Mass Spectrometry after In-Situ Extraction Using Headspace Solid-Phase Micro-Extraction under Strict Anaerobic Conditions

PubMed Central

Liu, Jianmin; Wang, Baoyu; Tai, Chao; Wu, Li; Zhao, Han; Guan, Jiadong; Chen, Linyong

2016-01-01

Bioconversion of coal to methane has gained increased attention in recent decades because of its economic and environmental advantages. However, the mechanism of this process is difficult to study in depth, partly because of difficulties associated with the analysis of intermediates generated in coal bioconversion. In this investigation, we report on an effective method to analyze volatile intermediates generated in the bioconversion of coal under strict anaerobic conditions. We conduct in-situ extraction of intermediates using headspace solid-phase micro-extraction followed by detection by gas chromatography-mass spectrometry. Bioconversion simulation equipment was modified and combined with a solid-phase micro-extraction device. In-situ extraction could be achieved by using the combined units, to avoid a breakdown in anaerobic conditions and to maintain the experiment continuity. More than 30 intermediates were identified qualitatively in the conversion process, and the variation in trends of some typical intermediates has been discussed. Volatile organic acids (C2–C7) were chosen for a quantitative study of the intermediates because of their importance during coal bioconversion to methane. Fiber coating, extraction time, and solution acidity were optimized in the solid-phase micro-extraction procedure. The pressure was enhanced during the bioconversion process to investigate the influence of headspace pressure on analyte extraction. The detection limits of the method ranged from 0.0006 to 0.02 mmol/L for the volatile organic acids and the relative standard deviations were between 4.6% and 11.5%. The volatile organic acids (C2–C7) generated in the bioconversion process were 0.01–1.15 mmol/L with a recovery range from 80% to 105%. The developed method is useful for further in-depth research on the bioconversion of coal to methane. PMID:27695055

An Overview of Natural Gas Conversion Technologies for Co-Production of Hydrogen and Value-Added Solid Carbon Products

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

Dagle, Robert A.; Dagle, Vanessa; Bearden, Mark D.

This report was prepared in response to the U.S. Department of Energy Fuel Cell Technologies Office Congressional Appropriation language to support research on carbon-free production of hydrogen using new chemical processes that utilize natural gas to produce solid carbon and hydrogen. The U.S. produces 9-10 million tons of hydrogen annually with more than 95% of the hydrogen produced by steam-methane reforming (SMR) of natural gas. SMR is attractive because of its high hydrogen yield; but it also converts the carbon to carbon dioxide. Non-oxidative thermal decomposition of methane to carbon and hydrogen is an alternative to SMR and produces COmore » 2-free hydrogen. The produced carbon can be sold as a co-product, thus providing economic credit that reduces the delivered net cost of hydrogen. The combination of producing hydrogen with potentially valuable carbon byproducts has market value in that this allows greater flexibility to match the market prices of hydrogen and carbon. That is, the higher value product can subsidize the other in pricing decisions. In this report we highlight the relevant technologies reported in the literature—primarily thermochemical and plasma conversion processes—and recent research progress and commercial activities. Longstanding technical challenges include the high energetic requirements (e.g., high temperatures and/or electricity requirements) necessary for methane activation and, for some catalytic processes, the separation of solid carbon product from the spent catalyst. We assess current and new carbon product markets that could be served given technological advances, and we discuss technical barriers and potential areas of research to address these needs. We provide preliminary economic analysis for these processes and compare to other emerging (e.g., electrolysis) and conventional (e.g., SMR) processes for hydrogen production. The overarching conclusion of this study is that the cost of hydrogen can be potentially reduced to target levels of $2/kg with the co-production and sale of a sufficiently high-value carbon product. Technological advances are required to understand the reaction conditions and design reactor systems that can achieve high yields of the select carbon products and segregate or separate the high-value carbon products, and optimize the production process for both hydrogen and carbon.« less

Ethanol dehydration to ethylene in a stratified autothermal millisecond reactor.

PubMed

Skinner, Michael J; Michor, Edward L; Fan, Wei; Tsapatsis, Michael; Bhan, Aditya; Schmidt, Lanny D

2011-08-22

The concurrent decomposition and deoxygenation of ethanol was accomplished in a stratified reactor with 50-80 ms contact times. The stratified reactor comprised an upstream oxidation zone that contained Pt-coated Al(2)O(3) beads and a downstream dehydration zone consisting of H-ZSM-5 zeolite films deposited on Al(2)O(3) monoliths. Ethanol conversion, product selectivity, and reactor temperature profiles were measured for a range of fuel:oxygen ratios for two autothermal reactor configurations using two different sacrificial fuel mixtures: a parallel hydrogen-ethanol feed system and a series methane-ethanol feed system. Increasing the amount of oxygen relative to the fuel resulted in a monotonic increase in ethanol conversion in both reaction zones. The majority of the converted carbon was in the form of ethylene, where the ethanol carbon-carbon bonds stayed intact while the oxygen was removed. Over 90% yield of ethylene was achieved by using methane as a sacrificial fuel. These results demonstrate that noble metals can be successfully paired with zeolites to create a stratified autothermal reactor capable of removing oxygen from biomass model compounds in a compact, continuous flow system that can be configured to have multiple feed inputs, depending on process restrictions. Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

PubMed

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

2013-12-01

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

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

PubMed

Aghayan, M; Potemkin, D I; Rubio-Marcos, F; Uskov, S I; Snytnikov, P V; Hussainova, I

2017-12-20

Efficient capture and recycling of CO 2 enable not only prevention of global warming but also the supply of useful low-carbon fuels. The catalytic conversion of CO 2 into an organic compound is a promising recycling approach which opens new concepts and opportunities for catalytic and industrial development. Here we report about template-assisted wet-combustion synthesis of a one-dimensional nickel-based catalyst for carbon dioxide methanation and methane steam reforming. Because of a high temperature achieved in a short time during reaction and a large amount of evolved gases, the wet-combustion synthesis yields homogeneously precipitated nanoparticles of NiO with average particle size of 4 nm on alumina nanofibers covered with a NiAl 2 O 4 nanolayer. The as-synthesized core-shell structured fibers exhibit outstanding activity in steam reforming of methane and sufficient activity in carbon dioxide methanation with 100% selectivity toward methane formation. The as-synthesized catalyst shows stable operation under the reaction conditions for at least 50 h.

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

PubMed

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

2018-01-01

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

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.

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.

On the Edge of Research and Technological Application: A Critical Review of Electromethanogenesis

PubMed Central

Blasco-Gómez, Ramiro; Batlle-Vilanova, Pau; Villano, Marianna; Balaguer, Maria Dolors; Colprim, Jesús; Puig, Sebastià

2017-01-01

The conversion of electrical current into methane (electromethanogenesis) by microbes represents one of the most promising applications of bioelectrochemical systems (BES). Electromethanogenesis provides a novel approach to waste treatment, carbon dioxide fixation and renewable energy storage into a chemically stable compound, such as methane. This has become an important area of research since it was first described, attracting different research groups worldwide. Basics of the process such as microorganisms involved and main reactions are now much better understood, and recent advances in BES configuration and electrode materials in lab-scale enhance the interest in this technology. However, there are still some gaps that need to be filled to move towards its application. Side reactions or scaling-up issues are clearly among the main challenges that need to be overcome to its further development. This review summarizes the recent advances made in the field of electromethanogenesis to address the main future challenges and opportunities of this novel process. In addition, the present fundamental knowledge is critically reviewed and some insights are provided to identify potential niche applications and help researchers to overcome current technological boundaries. PMID:28425974

On the Edge of Research and Technological Application: A Critical Review of Electromethanogenesis.

PubMed

Blasco-Gómez, Ramiro; Batlle-Vilanova, Pau; Villano, Marianna; Balaguer, Maria Dolors; Colprim, Jesús; Puig, Sebastià

2017-04-20

The conversion of electrical current into methane (electromethanogenesis) by microbes represents one of the most promising applications of bioelectrochemical systems (BES). Electromethanogenesis provides a novel approach to waste treatment, carbon dioxide fixation and renewable energy storage into a chemically stable compound, such as methane. This has become an important area of research since it was first described, attracting different research groups worldwide. Basics of the process such as microorganisms involved and main reactions are now much better understood, and recent advances in BES configuration and electrode materials in lab-scale enhance the interest in this technology. However, there are still some gaps that need to be filled to move towards its application. Side reactions or scaling-up issues are clearly among the main challenges that need to be overcome to its further development. This review summarizes the recent advances made in the field of electromethanogenesis to address the main future challenges and opportunities of this novel process. In addition, the present fundamental knowledge is critically reviewed and some insights are provided to identify potential niche applications and help researchers to overcome current technological boundaries.

H2-rich fluids from serpentinization: Geochemical and biotic implications

PubMed Central

Sleep, N. H.; Meibom, A.; Fridriksson, Th.; Coleman, R. G.; Bird, D. K.

2004-01-01

Metamorphic hydration and oxidation of ultramafic rocks produces serpentinites, composed of serpentine group minerals and varying amounts of brucite, magnetite, and/or FeNi alloys. These minerals buffer metamorphic fluids to extremely reducing conditions that are capable of producing hydrogen gas. Awaruite, FeNi3, forms early in this process when the serpentinite minerals are Fe-rich. Olivine with the current mantle Fe/Mg ratio was oxidized during serpentinization after the Moon-forming impact. This process formed some of the ferric iron in the Earth's mantle. For the rest of Earth's history, serpentinites covered only a small fraction of the Earth's surface but were an important prebiotic and biotic environment. Extant methanogens react H2 with CO2 to form methane. This is a likely habitable environment on large silicate planets. The catalytic properties of FeNi3 allow complex organic compounds to form within serpentinite and, when mixed with atmospherically produced complex organic matter and waters that circulated through basalts, constitutes an attractive prebiotic substrate. Conversely, inorganic catalysis of methane by FeNi3 competes with nascent and extant life. PMID:15326313

Kinetics and advanced digester design for anaerobic digestion of water hyacinth and primary sludge

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

Chynoweth, D.P.; Dolenc, D.A.; Ghosh, S.

1982-01-01

A research program centered around a facility located at Walt Disney World (WDW) is in progress to evaluate the use of water hyacinth (WH) for secondary and tertiary wastewater treatment, to optimize growth of WH under these conditions, and to convert the resultant primary sludge (PS) and WH to methane via anaerobic digestion. This article describes the status of the biogasification component of this program, which includes baseline and advanced digestion experiments with individual feeds and blends and the design of an experimental test unit (ETU) to be installed at WDW. Experiments with several blends demonstrated that methane yields canmore » be predicted from the fractional content and methane yield of each component. The process was found to adhere to the Monod kinetic model for microbial growth, and associated kinetic parameters were developed for various feed combinations. A novel upflow digester is achieving significantly higher conversion than a stirred-tank digester. Of several pretreatment techniques used, only alkaline treatment resulted in increased biodegradability. A larger scale (4.5 m/sup 3/) experimental test unit is being designed for installation at WDW in 1982. 13 figures, 4 tables.« less

An improved light hydrocarbon analysis system. Interim report

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

Lamontagne, R.A.

1982-05-11

A system for extracting and measuring ambient levels of C1-C4 hydrocarbons and carbon monoxide (CO) in seawater is described. The analytical instrument is a gas chromatograph with flame ionization detectors that incorporates a catalytic conversion of CO to CH4 (methane). The samples are concentrated prior to introduction to the chromatographic system. The volatile hydrocarbons are extracted from the seawater by the use of a helium flow stream and concentrated on dry ice-acetone cold traps. Air samples can be processed in a similar way.

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

Quantifying the loss of methane through secondary gas mass transport (or 'slip') from a micro-porous membrane contactor applied to biogas upgrading.

PubMed

McLeod, Andrew; Jefferson, Bruce; McAdam, Ewan J

2013-07-01

Secondary gas transport during the separation of a binary gas with a micro-porous hollow fibre membrane contactor (HMFC) has been studied for biogas upgrading. In this application, the loss or 'slip' of the secondary gas (methane) during separation is a known concern, specifically since methane possesses the intrinsic calorific value. Deionised (DI) water was initially used as the physical solvent. Under these conditions, carbon dioxide (CO2) and methane (CH4) absorption were dependent upon liquid velocity (V(L)). Whilst the highest CO2 flux was recorded at high V(L), selectivity towards CO2 declined due to low residence times and a diminished gas-side partial pressure, and resulted in slip of approximately 5.2% of the inlet methane. Sodium hydroxide was subsequently used as a comparative chemical absorption solvent. Under these conditions, CO2 mass transfer increased by increasing gas velocity (VG) which is attributed to the excess of reactive hydroxide ions present in the solvent, and the fast conversion of dissolved CO2 to carbonate species reinitiating the concentration gradient at the gas-liquid interface. At high gas velocities, CH4 slip was reduced to 0.1% under chemical conditions. Methane slip is therefore dependent upon whether the process is gas phase or liquid phase controlled, since methane mass transport can be adequately described by Henry's law within both physical and chemical solvents. The addition of an electrolyte was found to further retard CH4 absorption via the salting out effect. However, their applicability to physical solvents is limited since electrolytic concentration similarly impinges upon the solvents' capacity for CO2. This study illustrates the significance of secondary gas mass transport, and furthermore demonstrates that gas-phase controlled systems are recommended where greater selectivity is required. Copyright © 2013 Elsevier Ltd. All rights reserved.

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.

Process for separating nitrogen from methane using microchannel process technology

DOEpatents

Tonkovich, Anna Lee [Marysville, OH; Qiu, Dongming [Dublin, OH; Dritz, Terence Andrew [Worthington, OH; Neagle, Paul [Westerville, OH; Litt, Robert Dwayne [Westerville, OH; Arora, Ravi [Dublin, OH; Lamont, Michael Jay [Hilliard, OH; Pagnotto, Kristina M [Cincinnati, OH

2007-07-31

The disclosed invention relates to a process for separating methane or nitrogen from a fluid mixture comprising methane and nitrogen, the process comprising: (A) flowing the fluid mixture into a microchannel separator, the microchannel separator comprising a plurality of process microchannels containing a sorption medium, the fluid mixture being maintained in the microchannel separator until at least part of the methane or nitrogen is sorbed by the sorption medium, and removing non-sorbed parts of the fluid mixture from the microchannel separator; and (B) desorbing the methane or nitrogen from the sorption medium and removing the desorbed methane or nitrogen from the microchannel separator. The process is suitable for upgrading methane from coal mines, landfills, and other sub-quality sources.

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.

Superacid Catalyzed Coal Conversion Chemistry. 1st and 2nd Quarterly Technical Progress Reports, September 1, 1983-March 30, 1984.

DOE R&D Accomplishments Database

Olah, G. A.

1984-01-01

In our laboratories we have previously developed a mild coal conversion process. This involves the use of a superacid system consisting of HF and BF{sub 3} in presence of hydrogen and/or a hydrogen donor solvent. In order to understand the chemistry involved in the process of depolymerization of coal by the HF:BF{sub 3}:H{sub 2} system we are carrying out a systematic study of a number of coal model compounds. The model compounds selected for present study have two benzene rings connected with various bridging units such as alkylidene, ether, sulfide etc. From studies so far carried out it appears that high pyridine extractibilities achieved by treating coal at temperature below 100 degrees C results from the cleavage of bridges such as present in bibenzyl, diphenyl methane, dibenzyl ether, dibenzyl sulfide etc. On the other hand the increased cyclohexane extractibility and distillability observed at relatively higher temperatures and hydrogen pressures reflects the hydrogenation and cleavage of the aromatic backbone in coal structure similar to what is seen in the conversion of model compounds such as biphenyl, diphenyl ether, diphenyl sulfide, anthracene, etc.

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

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

PubMed

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

2006-12-28

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

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

PubMed Central

Callaghan, Amy V.

2013-01-01

Anaerobic microorganisms play key roles in the biogeochemical cycling of methane and non-methane alkanes. To date, there appear to be at least three proposed mechanisms of anaerobic methane oxidation (AOM). The first pathway is mediated by consortia of archaeal anaerobic methane oxidizers and sulfate-reducing bacteria (SRB) via “reverse methanogenesis” and is catalyzed by a homolog of methyl-coenzyme M reductase. The second pathway is also mediated by anaerobic methane oxidizers and SRB, wherein the archaeal members catalyze both methane oxidation and sulfate reduction and zero-valent sulfur is a key intermediate. The third AOM mechanism is a nitrite-dependent, “intra-aerobic” pathway described for the denitrifying bacterium, ‘Candidatus Methylomirabilis oxyfera.’ It is hypothesized that AOM proceeds via reduction of nitrite to nitric oxide, followed by the conversion of two nitric oxide molecules to dinitrogen and molecular oxygen. The latter can be used to functionalize the methane via a particulate methane monooxygenase. With respect to non-methane alkanes, there also appear to be novel mechanisms of activation. The most well-described pathway is the addition of non-methane alkanes across the double bond of fumarate to form alkyl-substituted succinates via the putative glycyl radical enzyme, alkylsuccinate synthase (also known as methylalkylsuccinate synthase). Other proposed mechanisms include anaerobic hydroxylation via ethylbenzene dehydrogenase-like enzymes and an “intra-aerobic” denitrification pathway similar to that described for ‘Methylomirabilis oxyfera.’ PMID:23717304

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.

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.

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,

Development of optimal enzymatic and microbial conversion systems for biofuel production

NASA Astrophysics Data System (ADS)

Aramrueang, Natthiporn

The increase in demand for fuels, along with the concerns over the depletion of fossil fuels and the environmental problems associated with the use of the petroleum-based fuels, has driven the exploitation of clean and renewable energy. Through a collaboration project with Mendota Bioenergy LLC to produce advanced biofuel from sugar beet and other locally grown crops in the Central Valley of California through demonstration and commercial-scale biorefineries, the present study focused on the investigation of selected potential biomass as biofuel feedstock and development of bioconversion systems for sustainable biofuel production. For an efficient biomass-to-biofuel conversion process, three important steps, which are central to this research, must be considered: feedstock characterization, enzymatic hydrolysis of the feedstock, and the bioconversion process. The first part of the research focused on the characterization of various lignocellulosic biomass as feedstocks and investigated their potential ethanol yields. Physical characteristics and chemical composition were analyzed for four sugar beet varieties, three melon varieties, tomato, Jose tall wheatgrass, wheat hay, and wheat straw. Melons and tomato are those products discarded by the growers or processors due to poor quality. The mass-based ethanol potential of each feedstock was determined based on the composition. The high sugar-containing feedstocks are sugar beet roots, melons, and tomato, containing 72%, 63%, and 42% average soluble sugars on a dry basis, respectively. Thus, for these crops, the soluble sugars are the main substrate for ethanol production. The potential ethanol yields, on average, for sugar beet roots, melons, and tomato are 591, 526, and 448 L ethanol/metric ton dry basis (d.b.), respectively. Lignocellulosic biomass, including Jose Tall wheatgrass and wheat straw, are composed primarily of cellulose (27-39% d.b.) and hemicellulose (26-30% d.b.). The ethanol yields from these materials can range from 470 to 533 L ethanol/metric ton (d.b.) Sugar beet leaves contain nearly equal amounts of cellulose (13%), hemicellulose (16%), and pectin (17%). The potential ethanol yield of sugar beet leaves is 340 L ethanol/metric ton (d.b.). As remaining unused in great quantities during the production of sugar beet as a sugar and energy crop, sugar beet leaves was studied as a potential feedstock for the production of biofuel and valuable products. The enzymatic hydrolysis of sugar beet leaves was optimized for fermentable sugar production. Optimization of enzyme usage was performed to make the biorefinery process more cost- and energy-effective. In this research, response surface methodology was used to study the effects of enzyme loadings during the hydrolysis of sugar beet leaves at 10% total solids content, using a mix of cellulases, hemicellulases, and pectinases. The effects of enzyme loadings were studied with a five-level rotatable central composite design for maximum conversion of sugar beet leaves to fermentable sugars. The last part of this study investigated biogas production through the anaerobic digestion of microalgae as they have received much attention as another potential biofuel feedstock. Anaerobic digestion of Spirulina ( Arthrospira platensis) was conducted in batch reactors for the study of the kinetics and, in continuous stirred tank reactors (CSTR), for the study of the two important operating parameters: hydraulic retention time (HRT) and organic loading rate (OLR). The kinetics study on methane production from batch experiments shows first order kinetics and a reaction rate constant of 0.382 d-1. The maximum biogas and methane yields for Spirulina are 0.514 L/gVS and 0.360 L CH4/gVS, respectively. The methane content of the biogas is 68%. During the continuous anaerobic digestion in CSTR for OLR in the range of 1.0-4.0 gVS/L/d, biogas and methane yields are in the ranges of 0.276-0.502 L/ gVS and 0.163-0.342 L CH4/gVS, respectively. Methane content is 59-70% of the biogas. Methane yield decreases with an increase in OLR and a decrease in HRT. The maximum methane production is 0.342 L CH4/gVS at OLR of 1.0 gVS/L d and 25d-HRT, achieving 94% of the maximum yield produced by batch digestion. Ammonia inhibition and the accumulation of volatile fatty acids (VFA) were observed at high OLR. According to the results from the continuous digestion of Spirulina, the recommended HRT should be sufficient at least 15d, with the OLRmax of 2.0 gVS/L to prevent ammonia inhibition at higher feed concentrations. The OLR can be increased when the digester is operated at longer HRT since a long HRT provides a more stable operation. A mathematical model, based on the kinetics study from the batch process, was developed for the prediction of methane production during a continuous digestion process, in relation to HRT. Further improvement of the model may have to include the effects of ammonia inhibition and low solids retention time (SRT) to overcome these limitations. (Abstract shortened by UMI.).

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

PubMed

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

2017-12-01

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

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

PubMed

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

2017-01-01

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

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

PubMed

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

2016-07-01

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

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

NASA Technical Reports Server (NTRS)

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

1991-01-01

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

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.

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

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.

Methane/nitrogen separation process

DOEpatents

Baker, R.W.; Lokhandwala, K.A.; Pinnau, I.; Segelke, S.

1997-09-23

A membrane separation process is described for treating a gas stream containing methane and nitrogen, for example, natural gas. The separation process works by preferentially permeating methane and rejecting nitrogen. The authors have found that the process is able to meet natural gas pipeline specifications for nitrogen, with acceptably small methane loss, so long as the membrane can exhibit a methane/nitrogen selectivity of about 4, 5 or more. This selectivity can be achieved with some rubbery and super-glassy membranes at low temperatures. The process can also be used for separating ethylene from nitrogen. 11 figs.

Methane/nitrogen separation process

DOEpatents

Baker, Richard W.; Lokhandwala, Kaaeid A.; Pinnau, Ingo; Segelke, Scott

1997-01-01

A membrane separation process for treating a gas stream containing methane and nitrogen, for example, natural gas. The separation process works by preferentially permeating methane and rejecting nitrogen. We have found that the process is able to meet natural gas pipeline specifications for nitrogen, with acceptably small methane loss, so long as the membrane can exhibit a methane/nitrogen selectivity of about 4, 5 or more. This selectivity can be achieved with some rubbery and super-glassy membranes at low temperatures. The process can also be used for separating ethylene from nitrogen.

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.

Inverse Modeling of Tropospheric Methane Constrained by 13C Isotope in Methane

NASA Astrophysics Data System (ADS)

Mikaloff Fletcher, S. E.; Tans, P. P.; Bruhwiler, L. M.

2001-12-01

Understanding the budget of methane is crucial to predicting climate change and managing earth's carbon reservoirs. Methane is responsible for approximately 15% of the anthropogenic greenhouse forcing and has a large impact on the oxidative capacity of Earth's atmosphere due to its reaction with hydroxyl radical. At present, many of the sources and sinks of methane are poorly understood, due in part to the large spatial and temporal variability of the methane flux. Model calculations of methane mixing ratios using most process-based source estimates typically over-predict the inter-hemispheric gradient of atmospheric methane. Inverse models, which estimate trace gas budgets by using observations of atmospheric mixing ratios and transport models to estimate sources and sinks, have been used to incorporate features of the atmospheric observations into methane budgets. While inverse models of methane generally tend to find a decrease in northern hemisphere sources and an increase in southern hemisphere sources relative to process-based estimates,no inverse study has definitively associated the inter-hemispheric gradient difference with a specific source process or group of processes. In this presentation, observations of isotopic ratios of 13C in methane and isotopic signatures of methane source processes are used in conjunction with an inverse model of methane to further constrain the source estimates of methane. In order to investigate the advantages of incorporating 13C, the TM3 three-dimensional transport model was used. The methane and carbon dioxide measurements used are from a cooperative international effort, the Cooperative Air Sampling Network, lead by the Climate Monitoring Diagnostics Laboratory (CMDL) at the National Oceanic and Atmospheric Administration (NOAA). Experiments using model calculations based on process-based source estimates show that the inter-hemispheric gradient of δ 13CH4 is not reproduced by these source estimates, showing that the addition of observations of δ 13CH4 should provide unique insight into the methane problem.

Preliminary System Analysis of In Situ Resource Utilization for Mars Human Exploration

NASA Technical Reports Server (NTRS)

Rapp, Donald; Andringa, Jason; Easter, Robert; Smith, Jeffrey H .; Wilson, Thomas; Clark, D. Larry; Payne, Kevin

2005-01-01

We carried out a system analysis of processes for utilization of Mars resources to support human exploration of Mars by production of propellants from indigenous resources. Seven ISRU processes were analyzed to determine mass. power and propellant storage volume requirements. The major elements of each process include C02 acquisition, chemical conversion, and storage of propellants. Based on a figure of merit (the ratio of the mass of propellants that must be brought from Earth in a non-ISRU mission to the mass of the ISRU system. tanks and feedstocks that must be brought from Earth for a ISRU mission) the most attractive process (by far); is one where indigenous Mars water is accessible and this is processed via Sabatier/Electrolysis to methane and oxygen. These processes are technically relatively mature. Other processes with positive leverage involve reverse water gas shift and solid oxide electrolysis.

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.

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

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.

Swarm intelligence for multi-objective optimization of synthesis gas production

NASA Astrophysics Data System (ADS)

Ganesan, T.; Vasant, P.; Elamvazuthi, I.; Ku Shaari, Ku Zilati

2012-11-01

In the chemical industry, the production of methanol, ammonia, hydrogen and higher hydrocarbons require synthesis gas (or syn gas). The main three syn gas production methods are carbon dioxide reforming (CRM), steam reforming (SRM) and partial-oxidation of methane (POM). In this work, multi-objective (MO) optimization of the combined CRM and POM was carried out. The empirical model and the MO problem formulation for this combined process were obtained from previous works. The central objectives considered in this problem are methane conversion, carbon monoxide selectivity and the hydrogen to carbon monoxide ratio. The MO nature of the problem was tackled using the Normal Boundary Intersection (NBI) method. Two techniques (Gravitational Search Algorithm (GSA) and Particle Swarm Optimization (PSO)) were then applied in conjunction with the NBI method. The performance of the two algorithms and the quality of the solutions were gauged by using two performance metrics. Comparative studies and results analysis were then carried out on the optimization results.

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...

[In situ Raman spectroscopic observation of micro-processes of methane hydrate formation and dissociation].

PubMed

Liu, Chang-Ling; Ye, Yu-Guang; Meng, Qing-Guo; Lü, Wan-Jun; Wang, Fei-Fei

2011-06-01

Micro laser Raman spectroscopic technique was used for in situ observation of the micro-processes of methane hydrate formed and decomposed in a high pressure transparent capillary. The changes in clathrate structure of methane hydrate were investigated during these processes. The results show that, during hydrate formation, the Raman peak (2 917 cm(-1)) of methane gas gradually splits into two peaks (2 905 and 2 915 cm(-1)) representing large and small cages, respectively, suggesting that the dissolved methane molecules go into two different chemical environments. In the meantime, the hydrogen bonds interaction is strengthened because water is changing from liquid to solid state gradually. As a result, the O-H stretching vibrations of water shift to lower wavenumber. During the decomposition process of methane hydrates, the Raman peaks of the methane molecules both in the large and small cages gradually clear up, and finally turn into a single peak of methane gas. The experimental results show that laser Raman spectroscopy can accurately demonstrate some relevant information of hydrate crystal structure changes during the formation and dissociation processes of methane hydrate.

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.

Enhancing methane production from food waste fermentate using biochar: the added value of electrochemical testing in pre-selecting the most effective type of biochar.

PubMed

Cruz Viggi, Carolina; Simonetti, Serena; Palma, Enza; Pagliaccia, Pamela; Braguglia, Camilla; Fazi, Stefano; Baronti, Silvia; Navarra, Maria Assunta; Pettiti, Ida; Koch, Christin; Harnisch, Falk; Aulenta, Federico

2017-01-01

Recent studies have suggested that addition of electrically conductive biochar particles is an effective strategy to improve the methanogenic conversion of waste organic substrates, by promoting syntrophic associations between acetogenic and methanogenic organisms based on interspecies electron transfer processes. However, the underlying fundamentals of the process are still largely speculative and, therefore, a priori identification, screening, and even design of suitable biochar materials for a given biotechnological process are not yet possible. Here, three charcoal-like products (i.e., biochars) obtained from the pyrolysis of different lignocellulosic materials, (i.e., wheat bran pellets, coppiced woodlands, and orchard pruning) were tested for their capacity to enhance methane production from a food waste fermentate. In all biochar-supplemented (25 g/L) batch experiments, the complete methanogenic conversion of fermentate volatile fatty acids proceeded at a rate that was up to 5 times higher than that observed in the unamended (or sand-supplemented) controls. Fluorescent in situ hybridization analysis coupled with confocal laser scanning microscopy revealed an intimate association between archaea and bacteria around the biochar particles and provided a clear indication that biochar also shaped the composition of the microbial consortium. Based on the application of a suite of physico-chemical and electrochemical characterization techniques, we demonstrated that the positive effect of biochar is directly related to the electron-donating capacity (EDC) of the material, but is independent of its bulk electrical conductivity and specific surface area. The latter properties were all previously hypothesized to play a major role in the biochar-mediated interspecies electron transfer process in methanogenic consortia. Collectively, these results of this study suggest that for biochar addition in anaerobic digester operation, the screening and identification of the most suitable biochar material should be based on EDC determination, via simple electrochemical tests.

Fifteenth symposium on biotechnology for fuels and chemicals: Program and abstracts

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

Not Available

1993-07-01

This collection contains 173 abstracts from presented papers and poster sessions. The five sessions of the conference were on the subjects of: (1) Thermal, Chemical, and Biological Processing, (2) Applied Biological Research, (3) Bioprocessing Research (4), Process Economics and Commercialization, and (5) Environmental Biotechnology. Examples of specific topics in the first session include the kinetics of ripening cheese, microbial liquefaction of lignite, and wheat as a feedstock for fuel ethanol. Typical topics in the second session were synergism studies of bacterial and fungal celluloses, conversion of inulin from jerusalem artichokes to sorbitol and ethanol by saccharomyces cerevisiae, and microbial conversionmore » of high rank coals to methane. The third session entertained topics such as hydrodynamic modeling of a liquid fluidized bed bioreactor for coal biosolubilization, aqueous biphasic systems for biological particle partitioning, and arabinose utilization by xylose-fermenting yeast and fungi. The fourth session included such topics as silage processing of forage biomass to alcohol fuels, economics of molasses to ethanol in India, and production of lactic acid from renewable resources. the final session contained papers on such subjects as bioluminescent detection of contaminants in soils, characterization of petroleum contaminated soils in coral atolls in the south Pacific, and landfill management for methane generation and emission control.« less

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.

AO13. High energy, low methane syngas from low-rank coals for coal-to-liquids production

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

Lucero, Andrew; Goyal, Amit; McCabe, Kevin

2015-06-30

An experimental program was undertaken to develop and demonstrate novel steam reforming catalysts for converting tars, C2+ hydrocarbons, and methane under high temperature and sulfur environments at lab scale. Several catalysts were developed and synthesized along with some catalysts based on recipes found in the literature. Of these, two had good resistance at 90 ppm H 2S with one almost not affected at all. Higher concentrations of H 2S did affect methane conversion across the catalyst, but performance was fairly stable for up to 200 hours. Based on the results of the experimental program, a techno-economic analysis was developed formore » IGCC and CTL applications and compared to DOE reference cases to examine the effects of the new technology. In the IGCC cases, the reformer/POX system produces nearly the same amount of electricity for nearly the same cost, however, the reformers/POX case sequesters a higher percentage of the carbon when compared to IGCC alone. For the CTL case the economics of the new process were nearly identical to the CTL case, but due to improved yields, the greenhouse gas emissions for a given production of fuels was approximately 50% less than the baseline case.« less

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.

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

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

H2-rich fluids from serpentinization: geochemical and biotic implications.

PubMed

Sleep, N H; Meibom, A; Fridriksson, Th; Coleman, R G; Bird, D K

2004-08-31

Metamorphic hydration and oxidation of ultramafic rocks produces serpentinites, composed of serpentine group minerals and varying amounts of brucite, magnetite, and/or FeNi alloys. These minerals buffer metamorphic fluids to extremely reducing conditions that are capable of producing hydrogen gas. Awaruite, FeNi3, forms early in this process when the serpentinite minerals are Fe-rich. Olivine with the current mantle Fe/Mg ratio was oxidized during serpentinization after the Moon-forming impact. This process formed some of the ferric iron in the Earth's mantle. For the rest of Earth's history, serpentinites covered only a small fraction of the Earth's surface but were an important prebiotic and biotic environment. Extant methanogens react H2 with CO2 to form methane. This is a likely habitable environment on large silicate planets. The catalytic properties of FeNi3 allow complex organic compounds to form within serpentinite and, when mixed with atmospherically produced complex organic matter and waters that circulated through basalts, constitutes an attractive prebiotic substrate. Conversely, inorganic catalysis of methane by FeNi3 competes with nascent and extant life. Copyright 2004 The National Academy of Sciencs of the USA

Physical Pretreatment Methods for Improving Microalgae Anaerobic Biodegradability.

PubMed

Córdova, Olivia; Passos, Fabiana; Chamy, Rolando

2018-05-01

Microalgae may be a potential feedstock for biogas production through anaerobic digestion. However, this process is limited by the hydrolytic stage, due to the complex and resistant microalgae cell wall components. This fact hinders biomass conversion into biogas, demanding the application of pretreatment techniques for inducing cell damage and/or lysis and organic matter solubilisation. In this study, sonication, thermal, ultrasound, homogeneizer, hydrothermal and steam explosion pretreatments were evaluated in different conditions for comparing their effects on anaerobic digestion performance in batch reactors. The results showed that the highest biomass solubilisation values were reached for steam explosion (65-73%) and ultrasound (33-57%). In fact, only applied energies higher than 220 W or temperatures higher than 80 °C induced cell wall lysis in C. sorokiniana. Nonetheless, the highest methane yields were not correlated to biogas production. Thermal hydrolysis and steam explosion showed lower methane yields in respect to non-pretreated biomass, suggesting the presence of toxic compounds that inhibited the biological process. Accordingly, these pretreatment techniques led to a negative energy balance. The best pretreatment method among the ones evaluated was thermal pretreatment, with four times more energy produced that demanded.

Aerobic methane production in surface waters of the Gulf of Mexico

NASA Astrophysics Data System (ADS)

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

2011-12-01

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

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

PubMed

Zhu, Wenjun; Jin, Jianhui; Chen, Xiao; Li, Chuang; Wang, Tonghua; Tsang, Chi-Wing; Liang, Changhai

2018-02-01

Effective utilization of coal bed methane is very significant for energy utilization and environment protection. Catalytic combustion of methane is a promising way to eliminate trace amounts of oxygen in the coal bed methane and the key to this technology is the development of high-efficiency catalysts. Herein, we report a series of Ce 1-x La x O 2-δ (x = 0-0.8) monolithic catalysts for the catalytic combustion of methane, which are prepared by citric acid method. The structural characterization shows that the substitution of La enhance the oxygen vacancy concentration and reducibility of the supports and promote the migration of the surface oxygen, as a result improve the catalytic activity of CeO 2 . M-Ce 0.8 La 0.2 O 2-δ (monolithic catalyst, Ce 0.8 La 0.2 O 2-δ coated on cordierite honeycomb) exhibits outstanding activity for methane combustion, and the temperature for 10 and 90% methane conversion are 495 and 580 °C, respectively. Additionally, Ce 0.8 La 0.2 O 2-δ monolithic catalyst presents excellent stability at high temperature. These Ce 1-x La x O 2-δ monolithic materials with a small amount of La incorporation therefore show promises as highly efficient solid solution catalysts for lean-oxygen methane combustion. Graphical abstract ᅟ.

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

PubMed

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

2011-08-01

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

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

PubMed

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

2018-02-01

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

Microbial minorities modulate methane consumption through niche partitioning

PubMed Central

Bodelier, Paul LE; Meima-Franke, Marion; Hordijk, Cornelis A; Steenbergh, Anne K; Hefting, Mariet M; Bodrossy, Levente; von Bergen, Martin; Seifert, Jana

2013-01-01

Microbes catalyze all major geochemical cycles on earth. However, the role of microbial traits and community composition in biogeochemical cycles is still poorly understood mainly due to the inability to assess the community members that are actually performing biogeochemical conversions in complex environmental samples. Here we applied a polyphasic approach to assess the role of microbial community composition in modulating methane emission from a riparian floodplain. We show that the dynamics and intensity of methane consumption in riparian wetlands coincide with relative abundance and activity of specific subgroups of methane-oxidizing bacteria (MOB), which can be considered as a minor component of the microbial community in this ecosystem. Microarray-based community composition analyses demonstrated linear relationships of MOB diversity parameters and in vitro methane consumption. Incubations using intact cores in combination with stable isotope labeling of lipids and proteins corroborated the correlative evidence from in vitro incubations demonstrating γ-proteobacterial MOB subgroups to be responsible for methane oxidation. The results obtained within the riparian flooding gradient collectively demonstrate that niche partitioning of MOB within a community comprised of a very limited amount of active species modulates methane consumption and emission from this wetland. The implications of the results obtained for biodiversity–ecosystem functioning are discussed with special reference to the role of spatial and temporal heterogeneity and functional redundancy. PMID:23788331

Microbial minorities modulate methane consumption through niche partitioning.

PubMed

Bodelier, Paul L E; Meima-Franke, Marion; Hordijk, Cornelis A; Steenbergh, Anne K; Hefting, Mariet M; Bodrossy, Levente; von Bergen, Martin; Seifert, Jana

2013-11-01

Microbes catalyze all major geochemical cycles on earth. However, the role of microbial traits and community composition in biogeochemical cycles is still poorly understood mainly due to the inability to assess the community members that are actually performing biogeochemical conversions in complex environmental samples. Here we applied a polyphasic approach to assess the role of microbial community composition in modulating methane emission from a riparian floodplain. We show that the dynamics and intensity of methane consumption in riparian wetlands coincide with relative abundance and activity of specific subgroups of methane-oxidizing bacteria (MOB), which can be considered as a minor component of the microbial community in this ecosystem. Microarray-based community composition analyses demonstrated linear relationships of MOB diversity parameters and in vitro methane consumption. Incubations using intact cores in combination with stable isotope labeling of lipids and proteins corroborated the correlative evidence from in vitro incubations demonstrating γ-proteobacterial MOB subgroups to be responsible for methane oxidation. The results obtained within the riparian flooding gradient collectively demonstrate that niche partitioning of MOB within a community comprised of a very limited amount of active species modulates methane consumption and emission from this wetland. The implications of the results obtained for biodiversity-ecosystem functioning are discussed with special reference to the role of spatial and temporal heterogeneity and functional redundancy.

Mechanistic insights into heterogeneous methane activation

DOE PAGES

Latimer, Allegra A.; Aljama, Hassan; Kakekhani, Arvin; ...

2017-01-11

While natural gas is an abundant chemical fuel, its low volumetric energy density has prompted a search for catalysts able to transform methane into more useful chemicals. This search has often been aided through the use of transition state (TS) scaling relationships, which estimate methane activation TS energies as a linear function of a more easily calculated descriptor, such as final state energy, thus avoiding tedious TS energy calculations. It has been shown that methane can be activated via a radical or surface-stabilized pathway, both of which possess a unique TS scaling relationship. Herein, we present a simple model tomore » aid in the prediction of methane activation barriers on heterogeneous catalysts. Analogous to the universal radical TS scaling relationship introduced in a previous publication, we show that a universal TS scaling relationship that transcends catalysts classes also seems to exist for surface-stabilized methane activation if the relevant final state energy is used. We demonstrate that this scaling relationship holds for several reducible and irreducible oxides, promoted metals, and sulfides. By combining the universal scaling relationships for both radical and surface-stabilized methane activation pathways, we show that catalyst reactivity must be considered in addition to catalyst geometry to obtain an accurate estimation for the TS energy. Here, this model can yield fast and accurate predictions of methane activation barriers on a wide range of catalysts, thus accelerating the discovery of more active catalysts for methane conversion.« less

Mechanistic insights into heterogeneous methane activation

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

Latimer, Allegra A.; Aljama, Hassan; Kakekhani, Arvin

While natural gas is an abundant chemical fuel, its low volumetric energy density has prompted a search for catalysts able to transform methane into more useful chemicals. This search has often been aided through the use of transition state (TS) scaling relationships, which estimate methane activation TS energies as a linear function of a more easily calculated descriptor, such as final state energy, thus avoiding tedious TS energy calculations. It has been shown that methane can be activated via a radical or surface-stabilized pathway, both of which possess a unique TS scaling relationship. Herein, we present a simple model tomore » aid in the prediction of methane activation barriers on heterogeneous catalysts. Analogous to the universal radical TS scaling relationship introduced in a previous publication, we show that a universal TS scaling relationship that transcends catalysts classes also seems to exist for surface-stabilized methane activation if the relevant final state energy is used. We demonstrate that this scaling relationship holds for several reducible and irreducible oxides, promoted metals, and sulfides. By combining the universal scaling relationships for both radical and surface-stabilized methane activation pathways, we show that catalyst reactivity must be considered in addition to catalyst geometry to obtain an accurate estimation for the TS energy. Here, this model can yield fast and accurate predictions of methane activation barriers on a wide range of catalysts, thus accelerating the discovery of more active catalysts for methane conversion.« less

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

Analysis of biomass and waste gasification lean syngases combustion for power generation using spark ignition engines.

PubMed

Marculescu, Cosmin; Cenuşă, Victor; Alexe, Florin

2016-01-01

The paper presents a study for food processing industry waste to energy conversion using gasification and internal combustion engine for power generation. The biomass we used consisted in bones and meat residues sampled directly from the industrial line, characterised by high water content, about 42% in mass, and potential health risks. Using the feedstock properties, experimentally determined, two air-gasification process configurations were assessed and numerically modelled to quantify the effects on produced syngas properties. The study also focused on drying stage integration within the conversion chain: either external or integrated into the gasifier. To comply with environmental regulations on feedstock to syngas conversion both solutions were developed in a closed system using a modified down-draft gasifier that integrates the pyrolysis, gasification and partial oxidation stages. Good quality syngas with up to 19.1% - CO; 17% - H2; and 1.6% - CH4 can be produced. The syngas lower heating value may vary from 4.0 MJ/Nm(3) to 6.7 MJ/Nm(3) depending on process configuration. The influence of syngas fuel properties on spark ignition engines performances was studied in comparison to the natural gas (methane) and digestion biogas. In order to keep H2 molar quota below the detonation value of ⩽4% for the engines using syngas, characterised by higher hydrogen fraction, the air excess ratio in the combustion process must be increased to [2.2-2.8]. The results in this paper represent valuable data required by the design of waste to energy conversion chains with intermediate gas fuel production. The data is suitable for Otto engines characterised by power output below 1 MW, designed for natural gas consumption and fuelled with low calorific value gas fuels. Copyright © 2015 Elsevier Ltd. All rights reserved.

Tree-mediated methane emissions from tropical and temperate peatlands.

NASA Astrophysics Data System (ADS)

Pangala, S. R.; Gauci, V.; Hornibrook, E. R. C.; Gowing, D. J.

2012-04-01

Methane production and transport processes in peatlands are fairly well understood, but growing evidence for emission of methane through trees has highlighted the need to revisit methane transport processes. In wetland trees, morphological adaptations such as development of hypertrophied lenticels, aerenchyma and adventitious roots in response to soil anoxia mediates gas transport, transporting both oxygen from the atmosphere to oxygen-deprived roots and soil-produced methane from the root-zone to the atmosphere. Although, tree-mediated methane emissions from temperate tree species have been confirmed, methane emissions from tropical tree species and processes that control tree-mediated methane emissions remain unclear. This study explains the role of trees in transporting soil-produced methane to the atmosphere and uncovers the principal mechanisms of tree-mediated methane emissions. Methane emissions from eight tropical tree species and two temperate tree species were studied in situ. The mechanisms and controls on tree-mediated methane emissions were investigated using three year old common alder (Alnus glutinosa; 50 trees) grown under two artificially controlled water-table positions. Methane fluxes from whole mesocosms, the soil surface and tree stems were measured using static closed chambers. Both temperate and tropical tree species released significant quantities of methane, with tropical trees dominating ecosystem level methane fluxes. In temperate peatlands, both the methane gas transport mechanism and quantity of methane emitted from stems is tree-species dependent. In Alnus glutinosa, no correlations were observed between stomatal behaviour and tree-mediated methane emissions, however, stem methane emissions were positively correlated with both stem lenticel density and dissolved soil methane concentration. In Alnus glutinosa, no emissions were observed from leaf surfaces. The results demonstrate that exclusion of tree-mediated methane emissions from flux measurement campaigns in forested peatlands will lead to an underestimation of ecosystem-wide methane emissions.

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

PubMed

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

2016-02-10

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

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.

Electric measurements of PV heterojunction structures a-SiC/c-Si

NASA Astrophysics Data System (ADS)

Perný, Milan; Šály, Vladimír; Janíček, František; Mikolášek, Miroslav; Váry, Michal; Huran, Jozef

2018-01-01

Due to the particular advantages of amorphous silicon or its alloys with carbon in comparison to conventional crystalline materials makes such a material still interesting for study. The amorphous silicon carbide may be used in a number of micro-mechanical and micro-electronics applications and also for photovoltaic energy conversion devices. Boron doped thin layers of amorphous silicon carbide, presented in this paper, were prepared due to the optimization process for preparation of heterojunction solar cell structure. DC and AC measurement and subsequent evaluation were carried out in order to comprehensively assess the electrical transport processes in the prepared a-SiC/c-Si structures. We have investigated the influence of methane content in deposition gas mixture and different electrode configuration.

Application of rumen microorganisms for anaerobic bioconversion of lignocellulosic biomass.

PubMed

Yue, Zheng-Bo; Li, Wen-Wei; Yu, Han-Qing

2013-01-01

Rumen in the mammalian animals is a natural cellulose-degrading system and the microorganisms inside have been found to be able to effectively digest lignocellulosic biomass. Furthermore, methane or volatile fatty acids, which could be further converted to other biofuels, are the two major products in such a system. This paper offers an overview of recent development in the application of rumen microorganisms for lignocellulosic biomass conversion. Application of recent molecular tools in the analysis of rumen microbial community, progress in the development of artificial rumen reactors, the latest research results about characterizing rumen-dominated anaerobic digestion process and energy products are summarized. Also, the potential application of such a rumen-dominated process is discussed. Copyright © 2012 Elsevier Ltd. All rights reserved.

Process, including membrane separation, for separating hydrogen from hydrocarbons

DOEpatents

Baker, Richard W.; Lokhandwala, Kaaeid A.; He, Zhenjie; Pinnau, Ingo

2001-01-01

Processes for providing improved methane removal and hydrogen reuse in reactors, particularly in refineries and petrochemical plants. The improved methane removal is achieved by selective purging, by passing gases in the reactor recycle loop across membranes selective in favor of methane over hydrogen, and capable of exhibiting a methane/hydrogen selectivity of at least about 2.5 under the process conditions.

Microbial diversity in methanogenic hydrocarbon-degrading enrichment cultures isolated from a water-flooded oil reservoir (Dagang oil field, China)

NASA Astrophysics Data System (ADS)

Jiménez, Núria; Cai, Minmin; Straaten, Nontje; Yao, Jun; Richnow, Hans H.; Krüger, Martin

2015-04-01

Microbial transformation of oil to methane is one of the main degradation processes taking place in oil reservoirs, and it has important consequences as it negatively affects the quality and economic value of the oil. Nevertheless, methane could constitute a recovery method of carbon from exhausted reservoirs. Previous studies combining geochemical and isotopic analysis with molecular methods showed evidence for in situ methanogenic oil degradation in the Dagang oil field, China (Jiménez et al., 2012). However, the main key microbial players and the underlying mechanisms are still relatively unknown. In order to better characterize these processes and identify the main microorganisms involved, laboratory biodegradation experiments under methanogenic conditions were performed. Microcosms were inoculated with production and injection waters from the reservoir, and oil or 13C-labelled single hydrocarbons (e.g. n-hexadecane or 2-methylnaphthalene) were added as sole substrates. Indigenous microbiota were able to extensively degrade oil within months, depleting most of the n-alkanes in 200 days, and producing methane at a rate of 76 ± 6 µmol day-1 g-1 oil added. They could also produce heavy methane from 13C-labeled 2-methylnaphthalene, suggesting that further methanogenesis may occur from the aromatic and polyaromatic fractions of Dagang reservoir fluids. Microbial communities from oil and 2-methyl-naphthalene enrichment cultures were slightly different. Although, in both cases Deltaproteobacteria, mainly belonging to Syntrophobacterales (e.g. Syntrophobacter, Smithella or Syntrophus) and Clostridia, mostly Clostridiales, were among the most represented taxa, Gammaproteobacteria could be only identified in oil-degrading cultures. The proportion of Chloroflexi, exclusively belonging to Anaerolineales (e.g. Leptolinea, Bellilinea) was considerably higher in 2-methyl-naphthalene degrading cultures. Archaeal communities consisted almost exclusively of representatives of Methanomicrobia (mainly belonging to genera Methanosaeta and Methanoculleus). As both syntrophic Bacteria and methanogenic Archaea are abundant in Dagang, the studied areas of this oil field may have a significant potential to test the in situ conversion of oil into methane as a possible way to increase total hydrocarbon recovery.

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

Methane Pyrolysis and Disposing Off Resulting Carbon

NASA Technical Reports Server (NTRS)

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

1999-01-01

Sabatier/Electrolysis (S/E) is a leading process for producing methane and oxygen for application to Mars ISPP. One significant problem with this process is that it produces an excess of methane for combustion with the amount of oxygen that is produced. Therefore, one must discard roughly half of the methane to obtain the proper stoichiometric methane/oxygen mixture for ascent from Mars. This is a waste of hydrogen, which must be brought from Earth and is difficult to transport to Mars and store on Mars. To reduce the problem of transporting hydrogen to Mars, the S/E process can be augmented by another process which reduces overall hydrogen requirement. Three conceptual approaches for doing this are (i) recover hydrogen from the excess methane produced by the S/E process, (ii) convert the methane to a higher hydrocarbon or other organic with a lower H/C ratio than methane, and (iii) use a separate process (such as zirconia or reverse water gas shift reaction) to produce additional oxygen, thus utilizing all the methane produced by the Sabatier process. We report our results here on recovering hydrogen from the excess methane using pyrolysis of methane. Pyrolysis has the advantage that it produces almost pure hydrogen, and any unreacted methane can pass through the S/E process reactor. It has the disadvantage that disposing of the carbon produced by pyrolysis presents difficulties. The goals of a research program on recovery of hydrogen from methane are (in descending priority order): 1) Study the kinetics of pyrolysis to arrive at a pyrolysis reactor design that produces high yields in a confined volume at the lowest possible operating temperature; 2) Study the kinetics of carbon burnoff to determine whether high yields can be obtained in a confined volume at acceptable operating temperatures; and 3) Investigate catalytic techniques for depositing carbon as a fine soot which can be physically separated from the reactor. In the JPL program, we have made significant measurements in regard to goal 1, cursory measurements in regard to goal 2, and would plan to pursue goal 3 if additional resources are secured.

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.

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.

Evaluation of microbial community composition in thermophilic methane-producing incubation of production water from a high-temperature oil reservoir.

PubMed

Zhou, Fang; Mbadinga, Serge Maurice; Liu, Jin-Feng; Gu, Ji-Dong; Mu, Bo-Zhong

2013-01-01

Investigation of petroleum microbes is fundamental for the development and utilization of oil reservoirs' microbial resources, and also provides great opportunities for research and development of bio-energy. Production water from a high-temperature oil reservoir was incubated anaerobically at 55 degrees C for more than 400 days without amendment of any nutrients. Over the time of incubation, about 1.6 mmol of methane and up to 107 micromol of hydrogen (H2) were detected in the headspace. Methane formation indicated that methanogenesis was likely the predominant process in spite of the presence of 23.4 mM SO4(2-) in the production water. Microbial community composition of the incubation was characterized by means of 16S rRNA gene clone libraries construction. Bacterial composition changed from Pseudomonales as the dominant population initially to Hydrogenophilales-related microorganisms affiliated to Petrobacter spp. closely. After 400 days of incubation, other bacterial members detected were related to Anareolineales, beta-, gamma-, and delta-Proteobacteria. The archaeal composition of the original production water was essentially composed of obligate acetoclastic methanogens of the genus Methanosaeta, but the incubation was predominantly composed of CO2-reducing methanogens of the genus Methanothermobacter and Crenarchaeotes-related microorganisms. Our results suggest that methanogenesis could be more active than expected in oil reservoir environments and methane formation from CO2-reduction played a significant role in the methanogenic community. This conclusion is consistent with the predominant role played by H2-oxidizing methanogens in the methanogenic conversion of organic matter in high-temperature petroleum reservoirs.

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

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.

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.

Enhanced hydrolysis and methane yield by applying microaeration pretreatment to the anaerobic co-digestion of brown water and food waste

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

Lim, Jun Wei; School of Civil and Environmental Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798; Wang, Jing-Yuan, E-mail: jywang@ntu.edu.sg

2013-04-15

Highlights: ► Microaeration pretreatment was effective for brown water and food waste mixture. ► The added oxygen was consumed fully by facultative microorganisms. ► Enhanced solubilization, acidification and breakdown of SCFAs to acetate. ► Microaeration pretreatment improved methane yield by 10–21%. ► Nature of inoculum influenced the effects of microaeration. - Abstract: Microaeration has been used conventionally for the desulphurization of biogas, and recently it was shown to be an alternative pretreatment to enhance hydrolysis of the anaerobic digestion (AD) process. Previous studies on microaeration pretreatment were limited to the study of substrates with complex organic matter, while little hasmore » been reported on its effect on substrates with higher biodegradability such as brown water and food waste. Due to the lack of consistent microaeration intensities, previous studies were not comparable and thus inconclusive in proving the effectiveness of microaeration to the overall AD process. In this study, the role of microaeration pretreatment in the anaerobic co-digestion of brown water and food waste was evaluated in batch-tests. After a 4-day pretreatment with 37.5 mL-O{sub 2}/L{sub R}-d added to the liquid phase of the reactor, the methane production of substrates were monitored in anaerobic conditions over the next 40 days. The added oxygen was consumed fully by facultative microorganisms and a reducing environment for organic matter degradation was maintained. Other than higher COD solubilization, microaeration pretreatment led to greater VFA accumulation and the conversion of other short chain fatty acids to acetate. This could be due to enhanced activities of hydrolytic and acidogenic bacteria and the degradation of slowly biodegradable compounds under microaerobic conditions. This study also found that the nature of inoculum influenced the effects of microaeration as a 21% and 10% increase in methane yield was observed when pretreatment was applied to inoculated substrates, and substrates without inoculum, respectively.« less

Sustainable Transportation Fuels from Natural Gas (H{sub 2}), Coal and Biomass

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

Huffman, Gerald

2012-12-31

This research program is focused primarily on the conversion of coal, natural gas (i.e., methane), and biomass to liquid fuels by Fischer-Tropsch synthesis (FTS), with minimum production of carbon dioxide. A complementary topic also under investigation is the development of novel processes for the production of hydrogen with very low to zero production of CO{sub 2}. This is in response to the nation's urgent need for a secure and environmentally friendly domestic source of liquid fuels. The carbon neutrality of biomass is beneficial in meeting this goal. Several additional novel approaches to limiting carbon dioxide emissions are also being explored.

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.

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

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

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.

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.

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.

Hydraulic and Mechanical Effects from Gas Hydrate Conversion and Secondary Gas Hydrate Formation during Injection of CO2 into CH4-Hydrate-Bearing Sediments

NASA Astrophysics Data System (ADS)

Bigalke, N.; Deusner, C.; Kossel, E.; Schicks, J. M.; Spangenberg, E.; Priegnitz, M.; Heeschen, K. U.; Abendroth, S.; Thaler, J.; Haeckel, M.

2014-12-01

The injection of CO2 into CH4-hydrate-bearing sediments has the potential to drive natural gas production and simultaneously sequester CO2 by hydrate conversion. The process aims at maintaining the in situ hydrate saturation and structure and causing limited impact on soil hydraulic properties and geomechanical stability. However, to increase hydrate conversion yields and rates it must potentially be assisted by thermal stimulation or depressurization. Further, secondary formation of CO2-rich hydrates from pore water and injected CO2 enhances hydrate conversion and CH4 production yields [1]. Technical stimulation and secondary hydrate formation add significant complexity to the bulk conversion process resulting in spatial and temporal effects on hydraulic and geomechanical properties that cannot be predicted by current reservoir simulation codes. In a combined experimental and numerical approach, it is our objective to elucidate both hydraulic and mechanical effects of CO2 injection and CH4-CO2-hydrate conversion in CH4-hydrate bearing soils. For the experimental approach we used various high-pressure flow-through systems equipped with different online and in situ monitoring tools (e.g. Raman microscopy, MRI and ERT). One particular focus was the design of triaxial cell experimental systems, which enable us to study sample behavior even during large deformations and particle flow. We present results from various flow-through high-pressure experimental studies on different scales, which indicate that hydraulic and geomechanical properties of hydrate-bearing sediments are drastically altered during and after injection of CO2. We discuss the results in light of the competing processes of hydrate dissociation, hydrate conversion and secondary hydrate formation. Our results will also contribute to the understanding of effects of temperature and pressure changes leading to dissociation of gas hydrates in ocean and permafrost systems. [1] Deusner C, Bigalke N, Kossel E, Haeckel M. Methane Production from Gas Hydrate Deposits through Injection of Supercritical CO2. Energies 2012:5(7): 2112-2140.

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.

Potential of Ni supported on KH zeolite catalysts for carbon dioxide reforming of methane

NASA Astrophysics Data System (ADS)

Kaengsilalai, Athiya; Luengnaruemitchai, Apanee; Jitkarnka, Sirirat; Wongkasemjit, Sujitra

The catalytic activity of Ni on a series of catalysts supported on the synthesized KH zeolite for the CO 2 reforming of methane has been investigated. The KH zeolite supports were previously synthesized via silatrane and alumatrane precursors using the sol-gel process and hydrothermal microwave treatment. Eight percent Ni was impregnated onto the synthesized KH zeolites, which have different morphologies: called dog-bone, flower, and disordered shapes. The prepared Ni/KH zeolites were tested for their catalytic activity at 700 °C, at atmospheric pressure, and at a CH 4/CO 2 ratio of 1. The results showed that Ni supported on dog-bone and flower-shaped KH zeolites provided better activity than that of disordered KH zeolite due to higher CH 4 and CO 2 conversions, a higher H 2 production, and a smaller amount of coke formation on the catalyst surface. Furthermore, the stability of the Ni/KH zeolite was greatly superior to that of Ni supported on alumina and clinoptiolite catalysts after 65 h on stream.

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.

Fabrication and application of mesoporous TiO2 film coated on Al wire by sol-gel method with EISA

NASA Astrophysics Data System (ADS)

Zhao, Linkang; Lu, Jianjun

2017-04-01

Mesoporous TiO2 film on Al wire was fabricated by sol-gel method with evaporation induced self assembly (EISA) process using F127 as templating agent in the mixed solution of ethanol and Tetra-n-butyl Titanate. The Ni/TiO2 film catalyst supported on Al wire was prepared by impregnation and the catalytic performance on methanation was carried out in a titanium alloy micro-reactor tube. It was shown that anatase mesoporous TiO2 film was prepared in this conditions (1 g F127,calcined at 400 °C and aged for 24 h), which has specific surface area of 127 m2 g-1 and narrow pore size distribution of 5.3 nm. Low calcined temperature (300 °C) cannot transfer film to anatase and decompose F127 completely. Ni/TiO2 film on Al wire catalyst was proved to be active in CO methanation reaction. And the CO conversion reaches 99% and CH4 selectivity close is to 80% when the reaction temperature is higher 360 °C.

Methane fermentation process for utilization of organic waste

NASA Astrophysics Data System (ADS)

Frąc, M.; Ziemiński, K.

2012-07-01

Biogas is a renewable and sustainable energy carrier generated via anaerobic digestion of biomass. This fuel is derived from various biomass resources and depending on its origin it contains methane (40-75%), carbon dioxide (20-45%) and some other compounds. The aim of this paper is to present the current knowledge and prospects of using the methane fermentation process to dispose of various types of organic wastes as well as conditions and factors affecting the methane fermentation process.

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...

Environmental and microbial factors influencing methane and nitrous oxide fluxes in Mediterranean cork oak woodlands: trees make a difference.

PubMed

Shvaleva, Alla; Siljanen, Henri M P; Correia, Alexandra; Costa E Silva, Filipe; Lamprecht, Richard E; Lobo-do-Vale, Raquel; Bicho, Catarina; Fangueiro, David; Anderson, Margaret; Pereira, João S; Chaves, Maria M; Cruz, Cristina; Martikainen, Pertti J

2015-01-01

Cork oak woodlands (montado) are agroforestry systems distributed all over the Mediterranean basin with a very important social, economic and ecological value. A generalized cork oak decline has been occurring in the last decades jeopardizing its future sustainability. It is unknown how loss of tree cover affects microbial processes that are consuming greenhouse gases in the montado ecosystem. The study was conducted under two different conditions in the natural understory of a cork oak woodland in center Portugal: under tree canopy (UC) and open areas without trees (OA). Fluxes of methane and nitrous oxide were measured with a static chamber technique. In order to quantify methanotrophs and bacteria capable of nitrous oxide consumption, we used quantitative real-time PCR targeting the pmoA and nosZ genes encoding the subunit of particulate methane mono-oxygenase and catalytic subunit of the nitrous oxide reductase, respectively. A significant seasonal effect was found on CH4 and N2O fluxes and pmoA and nosZ gene abundance. Tree cover had no effect on methane fluxes; conversely, whereas the UC plots were net emitters of nitrous oxide, the loss of tree cover resulted in a shift in the emission pattern such that the OA plots were a net sink for nitrous oxide. In a seasonal time scale, the UC had higher gene abundance of Type I methanotrophs. Methane flux correlated negatively with abundance of Type I methanotrophs in the UC plots. Nitrous oxide flux correlated negatively with nosZ gene abundance at the OA plots in contrast to that at the UC plots. In the UC soil, soil organic matter had a positive effect on soil extracellular enzyme activities, which correlated positively with the N2O flux. Our results demonstrated that tree cover affects soil properties, key enzyme activities and abundance of microorganisms and, consequently net CH4 and N2O exchange.

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

NASA Astrophysics Data System (ADS)

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

2016-12-01

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

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.

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.

Producing Hydrogen by Plasma Pyrolysis of Methane

NASA Technical Reports Server (NTRS)

Atwater, James; Akse, James; Wheeler, Richard

2010-01-01

Plasma pyrolysis of methane has been investigated for utility as a process for producing hydrogen. This process was conceived as a means of recovering hydrogen from methane produced as a byproduct of operation of a life-support system aboard a spacecraft. On Earth, this process, when fully developed, could be a means of producing hydrogen (for use as a fuel) from methane in natural gas. The most closely related prior competing process - catalytic pyrolysis of methane - has several disadvantages: a) The reactor used in the process is highly susceptible to fouling and deactivation of the catalyst by carbon deposits, necessitating frequent regeneration or replacement of the catalyst. b) The reactor is highly susceptible to plugging by deposition of carbon within fixed beds, with consequent channeling of flow, high pressure drops, and severe limitations on mass transfer, all contributing to reductions in reactor efficiency. c) Reaction rates are intrinsically low. d) The energy demand of the process is high.

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

PubMed Central

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

2018-01-01

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

Methane production by anaerobic digestion of Bermuda grass

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

Klass, D.L.; Ghosh, S.

1981-01-01

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

Pilot-scale testing of a leachbed for anaerobic digestion of livestock residues on-farm.

PubMed

Yap, S D; Astals, S; Jensen, P D; Batstone, D J; Tait, S

2016-04-01

A leachbed is a relatively simple anaerobic digester suitable for high-solids residues and on-farm applications. However, performance characteristics and optimal configuration of leachbeds are not well-understood. In this study, two 200 L pilot-scale leachbeds fed with spent straw bedding from pigs/swine (methane potential, B0 = 195-218 L CH4 kg(-1) VS fed) were used to assess the effects of leachate recirculation mode (trickling vs. flood-and-drain) on the digestion performance. Results showed comparable substrate solubilisation extents (30-45% of total chemical oxygen demand fed) and methane conversion (50% of the B0) for the trickling and flood-and-drain modes, indicating that digestion performance was insensitive to the mode of leachate flow. However, the flood-and-drain leachbed mobilised more particulates into the leachate than the trickling leachbed, an undesirable outcome, because these particulates were mostly non-biodegradable. Inoculation with solid residues from a previous leachbed (inoculum-to-substrate ratio of 0.22 on a VS basis) hastened the leachbed start-up, but methane recovery remained at 50% of the B0 regardless of the leachate recirculation mode. Post-digestion testing indicated that the leachbeds may have been limited by microbial activity/inhibition. The high residual methane potential of leachate from the trickling (residual Bo = 732 ± 7 L CH4 kg(-1) VS fed) and flood-and-drain leachbeds (582 ± 8 L CH4 kg(-1) VS fed) indicated an opportunity for further processing of leachate via a separate methanogenic step. Overall, a trickling leachbed appeared to be more favourable than the flood-and-drain leachbed for treating spent bedding at farm-scale due to easier operation. Copyright © 2016 Elsevier Ltd. All rights reserved.

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.

A Process-based, Climate-Sensitive Model to Derive Methane Emissions from Natural Wetlands: Application to 5 Wetland Sites, Sensitivity to Model Parameters and Climate

NASA Technical Reports Server (NTRS)

Walter, Bernadette P.; Heimann, Martin

1999-01-01

Methane emissions from natural wetlands constitutes the largest methane source at present and depends highly on the climate. In order to investigate the response of methane emissions from natural wetlands to climate variations, a 1-dimensional process-based climate-sensitive model to derive methane emissions from natural wetlands is developed. In the model the processes leading to methane emission are simulated within a 1-dimensional soil column and the three different transport mechanisms diffusion, plant-mediated transport and ebullition are modeled explicitly. The model forcing consists of daily values of soil temperature, water table and Net Primary Productivity, and at permafrost sites the thaw depth is included. The methane model is tested using observational data obtained at 5 wetland sites located in North America, Europe and Central America, representing a large variety of environmental conditions. It can be shown that in most cases seasonal variations in methane emissions can be explained by the combined effect of changes in soil temperature and the position of the water table. Our results also show that a process-based approach is needed, because there is no simple relationship between these controlling factors and methane emissions that applies to a variety of wetland sites. The sensitivity of the model to the choice of key model parameters is tested and further sensitivity tests are performed to demonstrate how methane emissions from wetlands respond to climate variations.

Secondary fermentation in the runen of a sheep given a diet based on molasses.

PubMed

Rowe, J B; Loughnan, M L; Nolan, J V; Leng, R A

1979-03-01

1. The extent of conversion of acetate-carbon to carbon dioxide in the rumen of a 40 kg wether consuming 1 kg molasses/d was estimated using isotope-tracer-dilution techniques. 2. There was a high rate of conversion of acetate to CO2 (6.0 g C/d) in the rumen. There were high concentrations in the rumen of Methanosarcina approximately 6 x 10(9)/ml which represents a significant proportion of the rumen bacterial biomass. These organisms are usually found in mud and sludge and are capable of oxidizing acetate. 3. The most likely explanation of these results was that there was an extensive secondary or sludge-type fermentation occurring in the rumen which results in volatile fatty acids being converted to CO2 and methane. In similar studies with sheep given lucerne (Medicago sativa) diets, conversion of acetate-C to CO2 within the rumen was not evident. 4. It is suggested that a major effect of the presence of secondary fermentation processes in the rumen may be to reduce availability of energy nutrients to the animal, and to alter the ratio protein:energy in the absorbed nutrients.

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.

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.

Effect of temperature on methanogenesis stage of two-stage anaerobic digestion of palm oil mill effluent (POME) into biogas

NASA Astrophysics Data System (ADS)

Trisakti, B.; Irvan, Mahdalena; Taslim; Turmuzi, M.

2017-06-01

This study aimed to determine the effect of temperature on methanogenesis stage of conversion of palm oil mill effluent into biogas. Methanogenesis is the second stage of methanogenic anaerobic digestion. Improved performance of the methanogenesis process was determined by measuring the growth of microorganisms, degradation of organic materials, biogas production and composition. Initially, the suitable loading up was determined by varying the HRT 100, 40, 6, and 4.0 days in the continuous stirred tank reactor (CSTR) with mixing rate 100 rpm, pH 6.7-7.5 at room temperature. Next, effect of temperature on the process was determined by varying temperature at mesophilic range (30-42°C) and thermophilic range (43-55°C). Analysis of total solids (TS), volatile solids (VS), total suspended solids (TSS), volatile suspended solids (VSS), and chemical oxygen demand (COD) were conducted in order to study the growth of microorganisms and their abilities in converting organic compound to produce biogas. Degradation of organic content i.e. VS decomposition and COD removal increased with the increasing of temperature. At mesophilic range, VS decomposition and COD removal were 51.56 ± 8.30 and 79.82 ± 6.03, respectively. Meanwhile at thermopilic range, VS decomposition and COD removal were 67.44 ± 3.59 and 79.16 ± 1.75, respectively. Biogas production and its methane content also increased with the increasing of temperature, but CO2 content also increased. Biogas production at mesophilic range was 31.77 ± 3.46 L/kg-ΔVS and methane content was 75 . Meanwhile, biogas production at thermopilic range was 37.03 ± 5.16 L/kg-ΔVS and methane content was 62.25 ± 5.50 .

Enhanced hydrolysis and methane yield by applying microaeration pretreatment to the anaerobic co-digestion of brown water and food waste.

PubMed

Lim, Jun Wei; Wang, Jing-Yuan

2013-04-01

Microaeration has been used conventionally for the desulphurization of biogas, and recently it was shown to be an alternative pretreatment to enhance hydrolysis of the anaerobic digestion (AD) process. Previous studies on microaeration pretreatment were limited to the study of substrates with complex organic matter, while little has been reported on its effect on substrates with higher biodegradability such as brown water and food waste. Due to the lack of consistent microaeration intensities, previous studies were not comparable and thus inconclusive in proving the effectiveness of microaeration to the overall AD process. In this study, the role of microaeration pretreatment in the anaerobic co-digestion of brown water and food waste was evaluated in batch-tests. After a 4-day pretreatment with 37.5 mL-O2/L(R)-d added to the liquid phase of the reactor, the methane production of substrates were monitored in anaerobic conditions over the next 40 days. The added oxygen was consumed fully by facultative microorganisms and a reducing environment for organic matter degradation was maintained. Other than higher COD solubilization, microaeration pretreatment led to greater VFA accumulation and the conversion of other short chain fatty acids to acetate. This could be due to enhanced activities of hydrolytic and acidogenic bacteria and the degradation of slowly biodegradable compounds under microaerobic conditions. This study also found that the nature of inoculum influenced the effects of microaeration as a 21% and 10% increase in methane yield was observed when pretreatment was applied to inoculated substrates, and substrates without inoculum, respectively. Copyright © 2012 Elsevier Ltd. All rights reserved.

Methane-Stimulated Benthic Marine Nitrogen Fixation at Deep-Sea Methane Seeps

NASA Astrophysics Data System (ADS)

Dekas, A. E.; Orphan, V.

2011-12-01

Biological nitrogen fixation (the conversion of N2 to NH3) is a critical process in the oceans, counteracting the production of N2 gas by dissimilatory bacterial metabolisms and providing a source of bioavailable nitrogen to many nitrogen-limited ecosystems. Although current measurements of N2 production and consumption in the oceans indicate that the nitrogen cycle is not balanced, recent findings on the limits of nitrogen fixation suggest that the perceived imbalance is an artifact of an incomplete assessment of marine diazotrophy. One currently poorly studied and potentially underappreciated habitat for diazotrophic organisms is the sediments of the deep-sea. In the present study we investigate the distribution and magnitude of benthic marine diazotrophy at several active deep-sea methane seeps (Mound 12, Costa Rica; Eel River Basin, CA, USA; Hydrate Ridge, OR, USA; and Monterey Canyon, CA, USA). Using 15N2 and 15NH4 sediment incubation experiments followed by single-cell (FISH-NanoSIMS) and bulk isotopic analysis (EA-IRMS), we observed total protein synthesis (15N uptake from 15NH4) and nitrogen fixation (15N update from 15N2). The highest rates of nitrogen fixation observed in the methane seep sediment incubation experiments were over an order of magnitude greater than those previously published from non-seep deep-sea sediments (Hartwig and Stanley, Deep-Sea Research, 1978, 25:411-417). However, methane seep diazotrophy appears to be highly spatially variable, with sediments exhibiting no nitrogen fixation originating only centimeters away from sediments actively incorporating 15N from 15N2. The greatest spatial variability in diazotrophy was observed with depth in the sediment, and corresponded to steep gradients in sulfate and methane. The maximum rates of nitrogen fixation were observed within the methane-sulfate transition zone, where organisms mediating the anaerobic oxidation of methane are typically in high abundance. Additionally, incubation experiments without added methane were observed to have little to no nitrogen fixation activity. In previous work, we demonstrated the capability of uncultured methanotrophic archaea (ANME-2) to fix nitrogen when associated with sulfate reducing bacterial symbionts. These new results suggest that these microbes may be the dominant nitrogen-fixing organisms in methane seep sediment. Intriguingly, characterization of the diversity of nifH genes from our sediment incubations as well as published nifH sequences reported from other seep habitats suggest the potential for other diazotrophic microorganisms in addition to the ANME-2 archaea. To further explore this possibility, FISH-NanoSIMS analyses were conducted on two dominant free-living sulfate-reducing lineages from seep incubations demonstrating nitrogen fixation activity. Preliminary results from this analysis suggest that single cells belonging to the Desulfobulbaceae may also be involved in nitrogen fixation in methane seeps. Despite this demonstrated potential, the extent of methane-independent diazotrophy by non-ANME diazotrophs appears to be low within the methane seep environment. Further studies are necessary to assess the greater diversity and activity of diazotrophs in other deep-sea sedimentary habitats.

Enhancement of waste activated sludge (WAS) anaerobic digestion by means of pre- and intermediate treatments. Technical and economic analysis at a full-scale WWTP.

PubMed

Campo, Giuseppe; Cerutti, Alberto; Zanetti, Mariachiara; Scibilia, Gerardo; Lorenzi, Eugenio; Ruffino, Barbara

2018-06-15

Anaerobic digestion (AD) is the most commonly applied end-treatment for the excess of waste activated sludge (WAS) generated in biological wastewater treatment processes. The efficacy of different typologies of pre-treatments in liberating intra-cellular organic substances and make them more usable for AD was demonstrated in several studies. However, the production of new extracellular polymeric substances (EPSs) that occur during an AD process, due to microbial metabolism, self-protective reactions and cell lysis, partially neutralizes the benefit of pre-treatments. The efficacy of post- and inter-stage treatments is currently under consideration to overcome the problems due to this unavoidable byproduct. This work compares three scenarios in which low-temperature (<100 °C) thermal and hybrid (thermal+alkali) lysis treatments were applied to one sample of WAS and two samples of digestate with hydraulic retention times (HRTs) of 7 and 15 days. Batch mesophilic digestibility tests demonstrated that intermediate treatments were effective in making the residual organic substance of a 7-day digestate usable for a second-stage AD process. In fact, under this scenario, the methane generated in a two-stage AD process, with an in-between intermediate treatment, was 23% and 16% higher than that generated in the scenario that considers traditional pre-treatments carried out with 4% NaOH at 70 and 90 °C respectively. Conversely, in no cases (70 or 90 °C) the combination of a 15-day AD process, followed by an intermediate treatment and a second-stage AD process, made possible to obtain specific methane productions (SMPs) higher than those obtained with pre-treatments. The results of the digestibility tests were used for a tecno-economic assessment of pre- and intermediate lysis treatments in a full scale wastewater treatment plant (WWTP, 2,000,000 p.e.). It was demonstrated that the introduction of thermal or hybrid pre-treatments could increase the revenues from the electricity sale by between 13% and 25%, in comparison with the present scenario (no lysis treatments). Conversely, intermediate treatments on a 7-day digestate could provide a gain of 26% or 32%, depending on the process temperature (70 or 90 °C). Copyright © 2017 Elsevier Ltd. All rights reserved.

Membrane-augmented cryogenic methane/nitrogen separation

DOEpatents

Lokhandwala, Kaaeid

1997-01-01

A membrane separation process combined with a cryogenic separation process for treating a gas stream containing methane, nitrogen and at least one other component. The membrane separation process works by preferentially permeating methane and the other component and rejecting nitrogen. The process is particularly useful in removing components such as water, carbon dioxide or C.sub.3+ hydrocarbons that might otherwise freeze and plug the cryogenic equipment.

Achieving Simultaneous CO2 and H2 S Conversion via a Coupled Solar-Driven Electrochemical Approach on Non-Precious-Metal Catalysts.

PubMed

Ma, Weiguang; Wang, Hong; Yu, Wei; Wang, Xiaomei; Xu, Zhiqiang; Zong, Xu; Li, Can

2018-03-19

Carbon dioxide (CO 2 ) and hydrogen sulfide (H 2 S) are generally concomitant with methane (CH 4 ) in natural gas and traditionally deemed useless or even harmful. Developing strategies that can simultaneously convert both CO 2 and H 2 S into value-added products is attractive; however it has not received enough attention. A solar-driven electrochemical process is demonstrated using graphene-encapsulated zinc oxide catalyst for CO 2 reduction and graphene catalyst for H 2 S oxidation mediated by EDTA-Fe 2+ /EDTA-Fe 3+ redox couples. The as-prepared solar-driven electrochemical system can realize the simultaneous conversion of CO 2 and H 2 S into carbon monoxide and elemental sulfur at near neutral conditions with high stability and selectivity. This conceptually provides an alternative avenue for the purification of natural gas with added economic and environmental benefits. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

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

PubMed

Kalyanasundaram, K; Graetzel, M

2010-06-01

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

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

PubMed

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

2017-05-01

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

Pilot-scale conversion of lime-treated wheat straw into bioethanol: quality assessment of bioethanol and valorization of side streams by anaerobic digestion and combustion

PubMed Central

Maas, Ronald HW; Bakker, Robert R; Boersma, Arjen R; Bisschops, Iemke; Pels, Jan R; de Jong, Ed; Weusthuis, Ruud A; Reith, Hans

2008-01-01

Introduction The limited availability of fossil fuel sources, worldwide rising energy demands and anticipated climate changes attributed to an increase of greenhouse gasses are important driving forces for finding alternative energy sources. One approach to meeting the increasing energy demands and reduction of greenhouse gas emissions is by large-scale substitution of petrochemically derived transport fuels by the use of carbon dioxide-neutral biofuels, such as ethanol derived from lignocellulosic material. Results This paper describes an integrated pilot-scale process where lime-treated wheat straw with a high dry-matter content (around 35% by weight) is converted to ethanol via simultaneous saccharification and fermentation by commercial hydrolytic enzymes and bakers' yeast (Saccharomyces cerevisiae). After 53 hours of incubation, an ethanol concentration of 21.4 g/liter was detected, corresponding to a 48% glucan-to-ethanol conversion of the theoretical maximum. The xylan fraction remained mostly in the soluble oligomeric form (52%) in the fermentation broth, probably due to the inability of this yeast to convert pentoses. A preliminary assessment of the distilled ethanol quality showed that it meets transportation ethanol fuel specifications. The distillation residue, which contained non-hydrolysable and non-fermentable (in)organic compounds, was divided into a liquid and solid fraction. The liquid fraction served as substrate for the production of biogas (methane), whereas the solid fraction functioned as fuel for thermal conversion (combustion), yielding thermal energy, which can be used for heat and power generation. Conclusion Based on the achieved experimental values, 16.7 kg of pretreated wheat straw could be converted to 1.7 kg of ethanol, 1.1 kg of methane, 4.1 kg of carbon dioxide, around 3.4 kg of compost and 6.6 kg of lignin-rich residue. The higher heating value of the lignin-rich residue was 13.4 MJ thermal energy per kilogram (dry basis). PMID:18699996

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.

Conversion of cellulosic wastes to liquid hydrocarbon fuels. Progress report, January-February 1981

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

Kuester, J.L.

1981-01-01

The following materials were processed thru gasification: sugarcane bagasse, smooth sumac, coralberry, wild bergamot, pokeweed, cornstarch, Portugese oak cork and hog fuel. A data summary is given. The high H/sub 2//CO ratio at low temperature for pokeweed is of significance (>T, >H/sub 2/). Also the high olefin content of Portugese oak cork (commercial cork) is of major interest. The most promising feedstock to date with regard to synthesis gas composition has been guayule cork. A comparison of data for the two cork materials is given. A detailed breakdown for corn starch is given revealing an exceptionally high methane content (35.50more » mole %). (MHR)« less

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

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

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

1995-12-31

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

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

NASA Astrophysics Data System (ADS)

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

2003-11-01

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

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

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

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

NOVEL MEMBRANE PROCESS TO UTILIZE DILUTE METHANE STREAMS - PHASE II

EPA Science Inventory

Process-based modelling of the methane balance in periglacial landscapes (JSBACH-methane)

NASA Astrophysics Data System (ADS)

Kaiser, Sonja; Göckede, Mathias; Castro-Morales, Karel; Knoblauch, Christian; Ekici, Altug; Kleinen, Thomas; Zubrzycki, Sebastian; Sachs, Torsten; Wille, Christian; Beer, Christian

2017-01-01

A detailed process-based methane module for a global land surface scheme has been developed which is general enough to be applied in permafrost regions as well as wetlands outside permafrost areas. Methane production, oxidation and transport by ebullition, diffusion and plants are represented. In this model, oxygen has been explicitly incorporated into diffusion, transport by plants and two oxidation processes, of which one uses soil oxygen, while the other uses oxygen that is available via roots. Permafrost and wetland soils show special behaviour, such as variable soil pore space due to freezing and thawing or water table depths due to changing soil water content. This has been integrated directly into the methane-related processes. A detailed application at the Samoylov polygonal tundra site, Lena River Delta, Russia, is used for evaluation purposes. The application at Samoylov also shows differences in the importance of the several transport processes and in the methane dynamics under varying soil moisture, ice and temperature conditions during different seasons and on different microsites. These microsites are the elevated moist polygonal rim and the depressed wet polygonal centre. The evaluation shows sufficiently good agreement with field observations despite the fact that the module has not been specifically calibrated to these data. This methane module is designed such that the advanced land surface scheme is able to model recent and future methane fluxes from periglacial landscapes across scales. In addition, the methane contribution to carbon cycle-climate feedback mechanisms can be quantified when running coupled to an atmospheric model.

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.

Anaerobic Methane Oxidation in Soils - revealed using 13C-labelled methane tracers

NASA Astrophysics Data System (ADS)

Riekie, G. J.; Baggs, E. M.; Killham, K. S.; Smith, J. U.

2008-12-01

In marine sediments, anaerobic methane oxidation is a significant biogeochemical process limiting methane flux from ocean to atmosphere. To date, evidence for anaerobic methane oxidation in terrestrial environments has proved elusive, and its significance is uncertain. In this study, an isotope dilution method specifically designed to detect the process of anaerobic methane oxidation in methanogenic wetland soils is applied. Methane emissions of soils from three contrasting permanently waterlogged sites in Scotland are investigated in strictly anoxic microcosms to which 13C- labelled methane is added, and changes in the concentration and 12C/13C isotope ratios of methane and carbon dioxide are subsequently measured and used to calculate separate the separate components of the methane flux. The method used takes into account the 13C-methane associated with methanogenesis, and the amount of methane dissolved in the soil. The calculations make no prior assumptions about the kinetics of methane production or oxidation. The results indicate that methane oxidation can take place in anoxic soil environments. The clearest evidence for anaerobic methane oxidation is provided by soils from a minerotrophic fen site (pH 6.0) in Bin Forest underlain by ultra-basic and serpentine till. In the fresh soil anoxic microcosms, net consumption methane was observed, and the amount of headspace 13C-CO2 increased at a greater rate than the 12+13C-CO2, further proof of methane oxidation. A net increase in methane was measured in microcosms of soil from Murder Moss, an alkaline site, pH 6.5, with a strong calcareous influence. However, the 13C-CH4 data provided evidence of methane oxidation, both in the disappearance of C- CH4 and appearance of smaller quantities of 13C-CO2. The least alkaline (pH 5.5) microcosms, of Gateside Farm soil - a granitic till - exhibited net methanogenesis and the changes in 13C-CH4 and 13C-CO2 here followed the pattern expected if no methane is consumed. Overall, this study provides good evidence for anaerobic methane oxidation in certain wetland soils, and suggests that models predicting methane flux from wetland soils to the atmosphere could be improved by better understanding of this process.

Membrane-augmented cryogenic methane/nitrogen separation

DOEpatents

Lokhandwala, K.

1997-07-15

A membrane separation process is described which is combined with a cryogenic separation process for treating a gas stream containing methane, nitrogen and at least one other component. The membrane separation process works by preferentially permeating methane and the other component and rejecting nitrogen. The process is particularly useful in removing components such as water, carbon dioxide or C{sub +2} hydrocarbons that might otherwise freeze and plug the cryogenic equipment. 10 figs.

Microbiology, ecology, and application of the nitrite-dependent anaerobic methane oxidation process

PubMed Central

Shen, Li-Dong; He, Zhan-Fei; Zhu, Qun; Chen, Dong-Qing; Lou, Li-Ping; Xu, Xiang-Yang; Zheng, Ping; Hu, Bao-Lan

2012-01-01

Nitrite-dependent anaerobic methane oxidation (n-damo), which couples the anaerobic oxidation of methane to denitrification, is a recently discovered process mediated by “Candidatus Methylomirabilis oxyfera.” M. oxyfera is affiliated with the “NC10” phylum, a phylum having no members in pure culture. Based on the isotopic labeling experiments, it is hypothesized that M. oxyfera has an unusual intra-aerobic pathway for the production of oxygen via the dismutation of nitric oxide into dinitrogen gas and oxygen. In addition, the bacterial species has a unique ultrastructure that is distinct from that of other previously described microorganisms. M. oxyfera-like sequences have been recovered from different natural habitats, suggesting that the n-damo process potentially contributes to global carbon and nitrogen cycles. The n-damo process is a process that can reduce the greenhouse effect, as methane is more effective in heat-trapping than carbon dioxide. The n-damo process, which uses methane instead of organic matter to drive denitrification, is also an economical nitrogen removal process because methane is a relatively inexpensive electron donor. This mini-review summarizes the peculiar microbiology of M. oxyfera and discusses the potential ecological importance and engineering application of the n-damo process. PMID:22905032

Serial completely stirred tank reactors for improving biogas production and substance degradation during anaerobic digestion of corn stover.

PubMed

Li, YuQian; Liu, ChunMei; Wachemo, Akiber Chufo; Yuan, HaiRong; Zou, DeXun; Liu, YanPing; Li, XiuJin

2017-07-01

Several completely stirred tank reactors (CSTR) connected in series for anaerobic digestion of corn stover were investigated in laboratory scale. Serial anaerobic digestion systems operated at a total HRT of 40days, and distribution of HRT are 10+30days (HRT10+30d), 20+20days (HRT20+20d), and 30+10days (HRT30+10d) were compared to a conventional one-step CSTR at the same HRT of 40d. The results showed that in HRT10+30d serial system, the process became very unstable at organic load of 50gTS·L -1 . The HRT20+20d and HRT30+10d serial systems improved methane production by 8.3-14.6% compared to the one-step system in all loads of 50, 70, 90gTS·L -1 . The conversion rates of total solid, cellulose, and hemicellulose were increased in serial anaerobic digestion systems compared to single system. The serial systems showed more stable process performance in high organic load. HRT30+10d system showed the best biogas production and conversions among all systems. Copyright © 2017. Published by Elsevier Ltd.

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.

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.

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.

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.

Laboratory formation of non-cementing, methane hydrate-bearing sands

USGS Publications Warehouse

Waite, William F.; Bratton, Peter M.; Mason, David H.

2011-01-01

Naturally occurring hydrate-bearing sands often behave as though methane hydrate is acting as a load-bearing member of the sediment. Mimicking this behavior in laboratory samples with methane hydrate likely requires forming hydrate from methane dissolved in water. To hasten this formation process, we initially form hydrate in a free-gas-limited system, then form additional hydrate by circulating methane-supersaturated water through the sample. Though the dissolved-phase formation process can theoretically be enhanced by increasing the pore pressure and flow rate and lowering the sample temperature, a more fundamental concern is preventing clogs resulting from inadvertent methane bubble formation in the circulation lines. Clog prevention requires careful temperature control throughout the circulation loop.

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

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

PubMed

Fu, Shan-Fei; Ding, Jian-Nan; Zhang, Yun; Li, Yi-Fei; Zhu, Rong; Yuan, Xian-Zheng; Zou, Hua

2018-06-01

In this study, impacts of nanoplastic on the pure and mixed anaerobic digestion systems were investigated. Results showed the growth and metabolism of Acetobacteroides hydrogenigenes were partly inhibited by nanoplastic existed in the pure anaerobic digestion system. The anaerobic digestion of sewage sludge was also obviously inhibited by nanoplastic existed in the mixed anaerobic digestion system. Both the methane yield and methane production rate of the mixed anaerobic digestion system showed negative correlation with the nanoplastic concentration. Compared with anaerobic digestion system without nanoplastic, methane yield and maximum daily methane yield at the nanoplastic concentration of 0.2g/L decreased for 14.4% and 40.7%, respectively. In addition, the start-up of mixed anaerobic digestion system was prolonged by addition of nanoplastic. Microbial community structure analysis indicated the microbial community structures were also affected by nanoplastic existed in the system. At the nanoplastic concentration of 0.2g/L, the relative abundances of family Cloacamonaceae, Porphyromonadaceae, Anaerolinaceae and Gracilibacteraceae decreased partly. Conversely, the relative abundances of family Anaerolinaceae, Clostridiaceae, Geobacteraceae, Dethiosulfovibrionaceae and Desulfobulbaceae improved partly. Copyright © 2017 Elsevier B.V. All rights reserved.

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

PubMed

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

2015-04-01

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

Oxidative coupling of methane using inorganic membrane reactor

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

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

1995-12-31

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

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.

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

The Potential of Biodiesel Production derived from Fish Waste

NASA Astrophysics Data System (ADS)

Farzana Samat, Amira; Amirah Safiah Muhamad, Nor; Rasib, Nur Aziera Abd; Hassan, Siti Aminah Mohd; Sohaimi, Khairunissa Syairah Ahmad; Izzati Iberahim, Nur

2018-03-01

Petroleum based diesel is one of the largest greenhouse emitters in the worlds based on its contribution to more likely of all carbon, methane and other greenhouse emissions. Besides, the depletion of fossil fuel that indirectly increased its price has force the global oil industry not to be so dependent on the fossil fuel but instead start focusing on alternative sources. Biodiesel is recognized as a clean alternative fuel or as a fuel additive to reduce pollutant from combustion equipment. In this study, the discarded parts of mixed marine fish species were used as the raw material to produce biodiesel. Marine fish oil was extracted from the discarded part of fish and if refined through a series of pretreatment process. The refined marine fish oil undergoes esterification process to reduce the amount of free fatty acid. The oil was then transesterified with methanol and sodium hydroxide as an alkaline catalyst that will speed up the conversion of oil to methyl ester. The three process parameters considered for this study were reaction time, reaction temperature and methanol to oil molar ratio. Biodiesel obtained was then analyzed using gas chromatography (GC). Statistical analyses were performed using SPSS software. The data obtained was analyzed by using one way analysis of variance (ANOVA) repeated measure. The results obtained showed that the conversion of FAME yield is the highest at reaction time 180 minutes, reaction temperature 60°C and methanol to oil molar ratio at 15:1 with FAME yield 80.16%, 80.03% and 80.39%. Thus, it can be concluded that the conversion of biodiesel increased as the reaction time, temperature and

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

Trade Study of Five In-Situ Propellant Production System for a Mars Sample Return Mission

NASA Technical Reports Server (NTRS)

Green, S. T.; Deffenbaugh, D. M.; Miller, M. A.

1999-01-01

One of the goals of NASA''s HEDS enterprise is to establish a long-term human presence on Mars at a fraction of the cost of employing today''s technology. The most direct method of reducing mission cost is to reduce the launch mass of the spacecraft. If the propellants for the return phase of the mission are produced on Mars, the total spacecraft mass could be reduced significantly. An interim goal is a Mars Sample Return (MSR) mission, which is proposed to demonstrate the feasibility of in-situ propellant production (ISPP). Five candidate ISPP systems for producing two fuels and oxygen from the Martian atmosphere are considered in this design trade-off study:(1) Zirconia cell with methanol synthesis, (2) Reverse water gas shift (RWGS) with water electrolysis and methanol synthesis, (3) Sabatier process for methane production with water electrolysis, (4) Sabatier process with water electrolysis and partial methane pyrolysis, and (5) Sabatier/RWGS combination with water electrolysis. These systems have been the subject of numerous previous analytical studies and laboratory demonstrations. In this investigation, the systems are objectively compared on the basis of thermochemical performance models using a commonly used chemical plant analysis software package. The realistic effects of incomplete chemical conversion and gas phase separator performance are included in these models. This study focuses on the chemical processing and product separation subsystems. The CO2 compression upstream of the chemical plane and the liquefaction/storage components are not included here.

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

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

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.

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.

Organics in hydrothermal fluids from ultramafics on the Mid-Atlantic Ridge (MAR) - Abiogenic and/or biogenic origin?

NASA Astrophysics Data System (ADS)

Charlou, J.; Donval, J.; Fouquet, Y.; Jean-Baptiste, P.; Dehairs, F.; Holm, N.; Godfroy, A.

2005-12-01

Between 12°N and the Azores Triple Junction along the MAR, CH4 anomalies over axial ultramafic sites are common and point to the association of high or low temperature hydrothermal activity and mantle degassing indicative of ongoing serpentinization process. The general occurrence of isotopically-heavy methane shows the possible abiogenic synthesis of hydrocarbons in hydrothermal systems. The abiogenic formation of CH4 and more complex organic compounds is related to the process of serpentinization of mantellic rocks. Three sites (Logachev, 14°45'N; Rainbow, 36°14'N; Lost City Field, 30°N) are known on the MAR. New fresh fluids were recently sampled at Rainbow and Lost City by the French ROV-Victor during EXOMAR cruise (July 24 to August 28, 2005). The Rainbow and Lost City fluids issued from contrasted ultramafic environments are both enriched in H2, CH4 and hydrocarbons. Hydrogen gas represents more than 40 per cent total gas volume extracted from fluids. SPME (Solid Phase Micro-Extraction) and SBSE (Stir-Bar Sorptive Extraction) extraction techniques were used on board for organic recovery and the analysis was performed on shore by direct GC/MS or by Thermo-Desorption/GC/MS. The hydration of olivine and pyroxen minerals with conversion of Fe(II) to Fe(III) in magnetite during serpentinization leads to production of H2 and conversion of dissolved CO2 to reduced-C species including methane, ethane, propane. In addition heavier straight chain hydrocarbons as alcohols, aldehydes, ketones, aromatics, and cyclic compounds are identified at Rainbow. These compounds may be generated in ultramafic rocks through catalytic reactions (Fischer-Tropsch type reactions), but a biogenic contribution cannot be excluded. Abiogenic organic compounds may be produced from crystalline basement, from volcanic structures, from riftogenic zones and probably from sedimented margins.

Cryptic Methane Emissions from Upland Forest Ecosystems

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

Megonigal, Patrick; Pitz, Scott

This exploratory research on Cryptic Methane Emissions from Upland Forest Ecosystems was motivated by evidence that upland ecosystems emit 36% as much methane to the atmosphere as global wetlands, yet we knew almost nothing about this source. The long-term objective was to refine Earth system models by quantifying methane emissions from upland forests, and elucidate the biogeochemical processes that govern upland methane emissions. The immediate objectives of the grant were to: (i) test the emerging paradigm that upland trees unexpectedly transpire methane, (ii) test the basic biogeochemical assumptions of an existing global model of upland methane emissions, and (iii) developmore » the suite of biogeochemical approaches that will be needed to advance research on upland methane emissions. We instrumented a temperate forest system in order to explore the processes that govern upland methane emissions. We demonstrated that methane is emitted from the stems of dominant tree species in temperate upland forests. Tree emissions occurred throughout the growing season, while soils adjacent to the trees consumed methane simultaneously, challenging the concept that forests are uniform sinks of methane. High frequency measurements revealed diurnal cycling in the rate of methane emissions, pointing to soils as the methane source and transpiration as the most likely pathway for methane transport. We propose the forests are smaller methane sinks than previously estimated due to stem emissions. Stem emissions may be particularly important in upland tropical forests characterized by high rainfall and transpiration, resolving differences between models and measurements. The methods we used can be effectively implemented in order to determine if the phenomenon is widespread.« less

Volcanic Destabilisation of Methane Clathrate Hydrate on Titan: the Mechanism for Resupplying Atmospheric NH3?

NASA Astrophysics Data System (ADS)

Davies, A. G.; Sotin, C.; Choukroun, M.; Matson, D. L.; Johnson, T. V.

2013-09-01

As previously noted [1-3], Titan may have an upper crust rich in methane clathrates which would have formed early in Titan's history [2, 3]. With an estimated mass of ~2 x 1017 kg, methane is a major component of Titan's atmosphere. The abundance of methane, which photo-dissociates under the influence of solar UV, and the presence of 40Ar require replenishment of these atmospheric components over geologic timescales. One possibility is that volcanic processes release these gases from Titan's interior, although so far there is no conclusive evidence of ongoing volcanic activity: no "smoking gun" has been observed. Still, some process has recently supplied a considerable amount of methane to Titan's atmosphere. We have been investigating the emplacement of proposed "cryolavas" of varying composition to, firstly, examine how such a volcanic process behaves thermally in order to determine event detectability via remote sensing, and, secondly, to model the penetration of the thermal wave into a methane-rich substrate. Destabilisation of clathrates would release methane into the atmosphere and liberate trapped argon.

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.

Effects of different nitrogen sources on the biogas production - a lab-scale investigation.

PubMed

Wagner, Andreas Otto; Hohlbrugger, Peter; Lins, Philipp; Illmer, Paul

2012-12-20

For anaerobic digestion processes nitrogen sources are poorly investigated although they are known as possible process limiting factors (in the hydrolysis phase) but also as a source for fermentations for subsequent methane production by methanogenic archaea. In the present study different complex and defined nitrogen sources were investigated in a lab-scale experiment in order to study their potential to build up methane. The outcome of the study can be summarised as follows: from complex nitrogen sources yeast extract and casamino acids showed the highest methane production with approximately 600 ml methane per mole of nitrogen, whereas by the use of skim milk no methane production could be observed. From defined nitrogen sources L-arginine showed the highest methane production with almost 1400 ml methane per mole of nitrogen. Moreover it could be demonstrated that the carbon content and therefore C/N-ratio has only minor influence for the methane production from the used substrates. Copyright © 2011 Elsevier GmbH. All rights reserved.

Microwave Heating-Assisted Catalytic Dry Reforming of Methane to Syngas.

PubMed

Hamzehlouia, Sepehr; Jaffer, Shaffiq A; Chaouki, Jamal

2018-06-12

Natural gas is a robust and environmentally friendlier alternative to oil resources for energy and chemicals production. However, gas is distributed globally within shales and hydrates, which are generally remote and difficult reserves to produce. The accessibility, transportation, and distribution, therefore, bring major capital costs. With today's low and foreseen low price of natural gas, conversion of natural gas to higher value-added chemicals is highly sought by industry. Dry reforming of methane (DRM) is a technology pathway to convert two critical greenhouse gas components, CH 4 and CO 2 , to syngas, a commodity chemical feedstock. To date, the challenges of carbon deposition on the catalyst and evolution of secondary gas-phase products have prevented the commercial application of the DRM process. The recent exponential growth of renewable electricity resources, wind and solar power, provides a major opportunity to activate reactions by harnessing low-cost carbon-free energy via microwave-heating. This study takes advantage of differences in dielectric properties of materials to enable selective heating by microwave to create a large thermal gradient between a catalyst surface and the gas phase. Consequently, the reaction kinetics at the higher temperature catalyst surface are promoted while the reactions of lower temperature secondary gas-phase are reduced.

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

Stapleton, J.

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

Carbon-13 Isotopic Abundance and Concentration of Atmospheric Methane for Background Air in the Southern and Northern Hemispheres from 1978 to 1989 (NDP-049)

DOE Data Explorer

Stevens, C. M. [Chemical Technology Division, Argonne National Laboratory, Argonne, Illinois (USA)

2012-01-01

This data package presents atmospheric CH4 concentration and 13C isotopic abundance data derived from air samples collected over the period 1978-1989 at globally distributed clean-air sites. The data set comprises 201 records, 166 from the Northern Hemisphere and 35 from the Southern Hemisphere. The air samples were collected mostly in rural or marine locations remote from large sources of CH4 and are considered representative of tropospheric background conditions. The air samples were processed by isolation of CH4 from air and conversion to CO2 for isotopic analysis by isotope ratio mass spectrometry. These data represent one of the earliest records of 13C isotopic yy!measurements for atmospheric methane and have been used to refine estimates of CH4 emissions, calculate annual growth rates of emissions from changing sources, and provide evidence for changes in the rate of atmospheric removal of CH4. The data records consist of sample collection date; number of samples combined for analysis; sampling location; analysis date; CH4 concentration; 13C isotopic abundance; and flag codes to indicate outliers, repeated analyses, and other information.

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

Relevance of deep-subsurface microbiology for underground gas storage and geothermal energy production.

PubMed

Gniese, Claudia; Bombach, Petra; Rakoczy, Jana; Hoth, Nils; Schlömann, Michael; Richnow, Hans-Hermann; Krüger, Martin

2014-01-01

This chapter gives the reader an introduction into the microbiology of deep geological systems with a special focus on potential geobiotechnological applications and respective risk assessments. It has been known for decades that microbial activity is responsible for the degradation or conversion of hydrocarbons in oil, gas, and coal reservoirs. These processes occur in the absence of oxygen, a typical characteristic of such deep ecosystems. The understanding of the responsible microbial processes and their environmental regulation is not only of great scientific interest. It also has substantial economic and social relevance, inasmuch as these processes directly or indirectly affect the quantity and quality of the stored oil or gas. As outlined in the following chapter, in addition to the conventional hydrocarbons, new interest in such deep subsurface systems is rising for different technological developments. These are introduced together with related geomicrobiological topics. The capture and long-termed storage of large amounts of carbon dioxide, carbon capture and storage (CCS), for example, in depleted oil and gas reservoirs, is considered to be an important options to mitigate greenhouse gas emissions and global warming. On the other hand, the increasing contribution of energy from natural and renewable sources, such as wind, solar, geothermal energy, or biogas production leads to an increasing interest in underground storage of renewable energies. Energy carriers, that is, biogas, methane, or hydrogen, are often produced in a nonconstant manner and renewable energy may be produced at some distance from the place where it is needed. Therefore, storing the energy after its conversion to methane or hydrogen in porous reservoirs or salt caverns is extensively discussed. All these developments create new research fields and challenges for microbiologists and geobiotechnologists. As a basis for respective future work, we introduce the three major topics, that is, CCS, underground storage of gases from renewable energy production, and the production of geothermal energy, and summarize the current stat of knowledge about related geomicrobiological and geobiotechnological aspects in this chapter. Finally, recommendations are made for future research.

Integrated Ceramic Membrane System for Hydrogen Production

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

Schwartz, Joseph; Lim, Hankwon; Drnevich, Raymond

2010-08-05

Phase I was a technoeconomic feasibility study that defined the process scheme for the integrated ceramic membrane system for hydrogen production and determined the plan for Phase II. The hydrogen production system is comprised of an oxygen transport membrane (OTM) and a hydrogen transport membrane (HTM). Two process options were evaluated: 1) Integrated OTM-HTM reactor – in this configuration, the HTM was a ceramic proton conductor operating at temperatures up to 900°C, and 2) Sequential OTM and HTM reactors – in this configuration, the HTM was assumed to be a Pd alloy operating at less than 600°C. The analysis suggestedmore » that there are no technical issues related to either system that cannot be managed. The process with the sequential reactors was found to be more efficient, less expensive, and more likely to be commercialized in a shorter time than the single reactor. Therefore, Phase II focused on the sequential reactor system, specifically, the second stage, or the HTM portion. Work on the OTM portion was conducted in a separate program. Phase IIA began in February 2003. Candidate substrate materials and alloys were identified and porous ceramic tubes were produced and coated with Pd. Much effort was made to develop porous substrates with reasonable pore sizes suitable for Pd alloy coating. The second generation of tubes showed some improvement in pore size control, but this was not enough to get a viable membrane. Further improvements were made to the porous ceramic tube manufacturing process. When a support tube was successfully coated, the membrane was tested to determine the hydrogen flux. The results from all these tests were used to update the technoeconomic analysis from Phase I to confirm that the sequential membrane reactor system can potentially be a low-cost hydrogen supply option when using an existing membrane on a larger scale. Phase IIB began in October 2004 and focused on demonstrating an integrated HTM/water gas shift (WGS) reactor to increase CO conversion and produce more hydrogen than a standard water gas shift reactor would. Substantial improvements in substrate and membrane performance were achieved in another DOE project (DE-FC26-07NT43054). These improved membranes were used for testing in a water gas shift environment in this program. The amount of net H2 generated (defined as the difference of hydrogen produced and fed) was greater than would be produced at equilibrium using conventional water gas shift reactors up to 75 psig because of the shift in equilibrium caused by continuous hydrogen removal. However, methanation happened at higher pressures, 100 and 125 psig, and resulted in less net H2 generated than would be expected by equilibrium conversion alone. An effort to avoid methanation by testing in more oxidizing conditions (by increasing CO2/CO ratio in a feed gas) was successful and net H2 generated was higher (40-60%) than a conventional reactor at equilibrium at all pressures tested (up to 125 psig). A model was developed to predict reactor performance in both cases with and without methanation. The required membrane area depends on conditions, but the required membrane area is about 10 ft2 to produce about 2000 scfh of hydrogen. The maximum amount of hydrogen that can be produced in a membrane reactor decreased significantly due to methanation from about 2600 scfh to about 2400 scfh. Therefore, it is critical to eliminate methanation to fully benefit from the use of a membrane in the reaction. Other modeling work showed that operating a membrane reactor at higher temperature provides an opportunity to make the reactor smaller and potentially provides a significant capital cost savings compared to a shift reactor/PSA combination.« less

Simulation of anaerobic digestion processes using stochastic algorithm.

PubMed

Palanichamy, Jegathambal; Palani, Sundarambal

2014-01-01

The Anaerobic Digestion (AD) processes involve numerous complex biological and chemical reactions occurring simultaneously. Appropriate and efficient models are to be developed for simulation of anaerobic digestion systems. Although several models have been developed, mostly they suffer from lack of knowledge on constants, complexity and weak generalization. The basis of the deterministic approach for modelling the physico and bio-chemical reactions occurring in the AD system is the law of mass action, which gives the simple relationship between the reaction rates and the species concentrations. The assumptions made in the deterministic models are not hold true for the reactions involving chemical species of low concentration. The stochastic behaviour of the physicochemical processes can be modeled at mesoscopic level by application of the stochastic algorithms. In this paper a stochastic algorithm (Gillespie Tau Leap Method) developed in MATLAB was applied to predict the concentration of glucose, acids and methane formation at different time intervals. By this the performance of the digester system can be controlled. The processes given by ADM1 (Anaerobic Digestion Model 1) were taken for verification of the model. The proposed model was verified by comparing the results of Gillespie's algorithms with the deterministic solution for conversion of glucose into methane through degraders. At higher value of 'τ' (timestep), the computational time required for reaching the steady state is more since the number of chosen reactions is less. When the simulation time step is reduced, the results are similar to ODE solver. It was concluded that the stochastic algorithm is a suitable approach for the simulation of complex anaerobic digestion processes. The accuracy of the results depends on the optimum selection of tau value.

Converting solid wastes into liquid fuel using a novel methanolysis process.

PubMed

Xiao, Ye; He, Peng; Cheng, Wei; Liu, Jacqueline; Shan, Wenpo; Song, Hua

2016-03-01

Biomass fast pyrolysis followed by hydrodeoxygenation upgrading is the most popular way to produce upgraded bio-oil from biomass. This process requires large quantities of expensive hydrogen and operates under high pressure condition (70-140 atm). Therefore, a novel methanolysis (i.e., biomass pyrolysis under methane environment) process is developed in this study, which is effective in upgraded bio-oil formation at atmospheric pressure and at about 400-600°C. Instead of using pure methane, simulated biogas (60% CH4+40% CO2) was used to test the feasibility of this novel methanolysis process for the conversion of different solid wastes. The bio-oil obtained from canola straw is slightly less than that from sawdust in term of quantity, but the oil quality from canola straw is better in terms of lower acidity, lower Bromine Number, higher H/C atomic ratio and lower O/C atomic ratio. The municipal solid waste and newspaper can also obtain relatively high oil yields, but the oil qualities of them are both lower than those from sawdust and canola straw. Compared with catalysts of 5%Zn/ZSM-5 and 1%Ag/ZSM-5, the 5%Zn-1%Ag/ZSM-5 catalyst performed much better in terms of upgraded bio-oil yield as well as oil quality. During the methanolysis process, the metal silver may be used to reduce the total acid number of the oil while the metal zinc might act to decrease the bromine number of the oil. The highly dispersed Zn and Ag species on/in the catalyst benefit the achievement of better upgrading performance and make it be a very promising catalyst for bio-oil upgrading by biogas. Copyright © 2015 Elsevier Ltd. All rights reserved.

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.

Methane Seepage on Mars: Where to Look and Why

NASA Astrophysics Data System (ADS)

Oehler, Dorothy Z.; Etiope, Giuseppe

2017-12-01

Methane on Mars is a topic of special interest because of its potential association with microbial life. The variable detections of methane by the Curiosity rover, orbiters, and terrestrial telescopes, coupled with methane's short lifetime in the martian atmosphere, may imply an active gas source in the planet's subsurface, with migration and surface emission processes similar to those known on Earth as "gas seepage." Here, we review the variety of subsurface processes that could result in methane seepage on Mars. Such methane could originate from abiotic chemical reactions, thermogenic alteration of abiotic or biotic organic matter, and ancient or extant microbial metabolism. These processes can occur over a wide range of temperatures, in both sedimentary and igneous rocks, and together they enhance the possibility that significant amounts of methane could have formed on early Mars. Methane seepage to the surface would occur preferentially along faults and fractures, through focused macro-seeps and/or diffuse microseepage exhalations. Our work highlights the types of features on Mars that could be associated with methane release, including mud-volcano-like mounds in Acidalia or Utopia; proposed ancient springs in Gusev Crater, Arabia Terra, and Valles Marineris; and rims of large impact craters. These could have been locations of past macro-seeps and may still emit methane today. Microseepage could occur through faults along the dichotomy or fractures such as those at Nili Fossae, Cerberus Fossae, the Argyre impact, and those produced in serpentinized rocks. Martian microseepage would be extremely difficult to detect remotely yet could constitute a significant gas source. We emphasize that the most definitive detection of methane seepage from different release candidates would be best provided by measurements performed in the ground or at the ground-atmosphere interface by landers or rovers and that the technology for such detection is currently available.

Recent development of anaerobic digestion processes for energy recovery from wastes.

PubMed

Nishio, Naomichi; Nakashimada, Yutaka

2007-02-01

Anaerobic digestion leads to the overall gasification of organic wastewaters and wastes, and produces methane and carbon dioxide; this gasification contributes to reducing organic matter and recovering energy from organic carbons. Here, we propose three new processes and demonstrate the effectiveness of each process. By using complete anaerobic organic matter removal process (CARP), in which diluted wastewaters such as sewage and effluent from a methane fermentation digester were treated under anaerobic condition for post-treatment, the chemical oxygen demand (COD) in wastewater was decreased to less than 20 ppm. The dry ammonia-methane two-stage fermentation process (Am-Met process) is useful for the anaerobic treatment of nitrogen-rich wastes such as waste excess sludge, cow feces, chicken feces, and food waste without the dilution of the ammonia produced by water or carbon-rich wastes. The hydrogen-methane two-stage fermentation (Hy-Met process), in which the hydrogen produced in the first stage is used for a fuel cell system to generate electricity and the methane produced in the second stage is used to generate heat energy to heat the two reactors and satisfy heat requirements, is useful for the treatment of sugar-rich wastewaters, bread wastes, and biodiesel wastewaters.

Light-induced diurnal pattern of methane exchange in a boreal forest

NASA Astrophysics Data System (ADS)

Sundqvist, Elin; Crill, Patrick; Mölder, Meelis; Vestin, Patrik; Lindroth, Anders

2013-04-01

Boreal forests represents one third of the Earth's forested land surface area and is a net sink of methane and an important component of the atmospheric methane budget. Methane is oxidized in well-aerated forest soils whereas ponds and bog soils are sources of methane. Besides the microbial processes in the soil also forest vegetation might contribute to methane exchange. Due to a recent finding of methane consumption by boreal plants that correlated with photosynthetic active radiation (PAR), we investigate the impact of PAR on soil methane exchange at vegetated plots on the forest floor. The study site, Norunda in central Sweden, is a 120 years old boreal forest stand, dominated by Scots pine and Norway spruce. We used continuous chamber measurements in combination with a high precision laser gas analyzer (Los Gatos Research), to measure the methane exchange at four different plots in July-November 2009, and April-June 2010. The ground vegetation consisted almost entirely of mosses and blueberry-shrubs. Two of the plots acted as stable sinks of methane whereas the other two plots shifted from sinks to sources during very wet periods. The preliminary results show a clear diurnal pattern of the methane exchange during the growing season, which cannot be explained by temperature. The highest consumption occurs at high PAR levels. The amplitude of the diurnal methane exchange during the growing season is in the order of 10 μmol m-2 h-1. This indicates that besides methane oxidation by methanotrophs in the soil there is an additional removal of methane at soil level by a process related to ground vegetation.

METHOD FOR PRODUCING ISOTOPIC METHANES AND PARTIALLY HALOGENATED DERIVATIVES THEROF

DOEpatents

Frazer, J.W.

1959-08-18

A method is given for producing isotopic methanes and/ or partially halogenated derivatives. Lithium hydride, deuteride, or tritide is reacted with a halogenated methane or with a halogenated methane in combination with free halogen. The process is conveniently carried out by passing a halogenated methane preferably at low pressures or in an admixture with an inert gas through a fixed bed of finely divided lithium hydride heated initially to temperatures of 100 to 200 deg C depending upon the halogenated methane used.

Methane storage capacity of the early martian cryosphere

NASA Astrophysics Data System (ADS)

Lasue, Jeremie; Quesnel, Yoann; Langlais, Benoit; Chassefière, Eric

2015-11-01

Methane is a key molecule to understand the habitability of Mars due to its possible biological origin and short atmospheric lifetime. Recent methane detections on Mars present a large variability that is probably due to relatively localized sources and sink processes yet unknown. In this study, we determine how much methane could have been abiotically produced by early Mars serpentinization processes that could also explain the observed martian remanent magnetic field. Under the assumption of a cold early Mars environment, a cryosphere could trap such methane as clathrates in stable form at depth. The extent and spatial distribution of these methane reservoirs have been calculated with respect to the magnetization distribution and other factors. We calculate that the maximum storage capacity of such a clathrate cryosphere is about 2.1 × 1019-2.2 × 1020 moles of CH4, which can explain sporadic releases of methane that have been observed on the surface of the planet during the past decade (∼1.2 × 109 moles). This amount of trapped methane is sufficient for similar sized releases to have happened yearly during the history of the planet. While the stability of such reservoirs depends on many factors that are poorly constrained, it is possible that they have remained trapped at depth until the present day. Due to the possible implications of methane detection for life and its influence on the atmospheric and climate processes on the planet, confirming the sporadic release of methane on Mars and the global distribution of its sources is one of the major goals of the current and next space missions to Mars.

Anaerobic digestion of municipal solid waste: Utility of process residues as a soil amendment

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

Rivard, C.J.; Nagle, N.J.; Kay, B.D.

1995-12-31

Tuna processing wastes (sludges high in fat, oil, and grease [FOG]) and municipal solid waste (MSW) generated on Tutuila Island, American Samoa, represent an ongoing disposal challenge. The biological conversion of the organic fraction of these wastes to useful products, including methane and fertilizer-grade residue, through anaerobic high-solids digestion is currently in scale-up development. The suitability of the anaerobic digestion residues as a soil amendment was evaluated through extensive chemical analysis and greenhouse studies using corn as an indicator crop. Additionally, native Samoan soil was used to evaluate the specific application rates for the compost. Experiments established that anaerobic residuesmore » increase crop yields in direct proportion to increases in the application rate. Additionally, nutrient saturation was not demonstrated within the range of application rates evaluated for the Samoan soil. Beyond nutrient supplementation, organic residue amendment to Samoan soil imparts enhanced water and nutrient-binding capacities.« less

Solid methane in neutron radiation: Cryogenic moderators and cometary cryo volcanism

NASA Astrophysics Data System (ADS)

Kirichek, O.; Lawson, C. R.; Jenkins, D. M.; Ridley, C. J. T.; Haynes, D. J.

2017-12-01

The effect of ionizing radiation on solid methane has previously been an area of interest in the astrophysics community. In the late 1980s this interest was further boosted by the possibility of using solid methane as a moderating medium in spallation neutron sources. Here we present test results of solid methane moderators commissioned at the ISIS neutron source, and compare them with a model based on the theory of thermal explosion. Good agreement between the moderator test data and our model suggests that the process of radiolysis defect recombination happens at two different temperature ranges: the ;lower temperature; recombination process occurs at around 20 K, with the ;higher temperature; process taking place between 50 and 60 K. We discuss consequences of this mechanism for the designing and operation of solid methane moderators used in advanced neutron sources. We also discuss the possible role of radiolysis defect recombination processes in cryo-volcanism on comets, and suggest an application based on this phenomenon.

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

Influence of process parameters on the extraction of soluble substances from OFMSW and methane production.

PubMed

Campuzano, Rosalinda; González-Martínez, Simón

2017-04-01

Microorganisms involved in anaerobic digestion require dissolved substrates to transport them through the cell wall to different processing units and finally to be disposed as waste, such as methane and carbon dioxide. In order to increase methane production, this work proposes to separate the soluble substances from OFMSW and analyse methane production from extracts and OFMSW. Using water as solvent, four extraction parameters were proposed: (1) Number of consecutive extractions, (2) Duration of mixing for every consecutive extraction, (3) OFMSW to water mass ratios 1:1, 1:2, and 1:3 and, (4) The influence of temperature on the extraction process. Results indicated that is possible to separate 40% of VS from OFMSW with only three consecutive extraction with mixing of 30min in every extraction using ambient temperature water. For every OFMSW to water combination, the first three consecutive extracts were analysed for biochemical methane potential test during 21days at 35°C; OFMSW was also tested as reference. Methane production from all substrates is highest during the first day and then it slowly decreases to increase again during a second stage. This was identified as diauxic behaviour. Specific methane production at day 21 increased with increasing water content of the extracts where OFMSW methane production was the lowest of all with 535NL/kgVS. These results indicate that it is feasible to rapidly produce methane from extracted substances. Copyright © 2017 Elsevier Ltd. All rights reserved.

Enhancement of methane production from co-digestion of chicken manure with agricultural wastes.

PubMed

Abouelenien, Fatma; Namba, Yuzaburo; Kosseva, Maria R; Nishio, Naomichi; Nakashimada, Yutaka

2014-05-01

The potential for methane production from semi-solid chicken manure (CM) and mixture of agricultural wastes (AWS) in a co-digestion process has been experimentally evaluated at thermophilic and mesophilic temperatures. To the best of author(')s knowledge, it is the first time that CM is co-digested with mixture of AWS consisting of coconut waste, cassava waste, and coffee grounds. Two types of anaerobic digestion processes (AD process) were used, process 1 (P1) using fresh CM (FCM) and process 2 (P2) using treated CM (TCM), ammonia stripped CM, were conducted. Methane production in P1 was increased by 93% and 50% compared to control (no AWS added) with maximum methane production of 502 and 506 mL g(-1)VS obtained at 55°C and 35°C, respectively. Additionally, 42% increase in methane production was observed with maximum volume of 695 mL g(-1)VS comparing P2 test with P2 control under 55°C. Ammonia accumulation was reduced by 39% and 32% in P1 and P2 tests. Copyright © 2014 Elsevier Ltd. All rights reserved.

Modeling methane emissions from Arctic lakes under warming conditions

NASA Astrophysics Data System (ADS)

Zhuang, Qianlai; Tan, Zeli

2014-05-01

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

Zero valent iron significantly enhances methane production from waste activated sludge by improving biochemical methane potential rather than hydrolysis rate.

PubMed

Liu, Yiwen; Wang, Qilin; Zhang, Yaobin; Ni, Bing-Jie

2015-02-05

Anaerobic digestion has been widely applied for waste activated sludge (WAS) treatment. However, methane production from anaerobic digestion of WAS is usually limited by the slow hydrolysis rate and/or poor biochemical methane potential of WAS. This work systematically studied the effects of three different types of zero valent iron (i.e., iron powder, clean scrap and rusty scrap) on methane production from WAS in anaerobic digestion, by using both experimental and mathematical approaches. The results demonstrated that both the clean and the rusty iron scrap were more effective than the iron powder for improving methane production from WAS. Model-based analysis showed that ZVI addition significantly enhanced methane production from WAS through improving the biochemical methane potential of WAS rather than its hydrolysis rate. Economic analysis indicated that the ZVI-based technology for enhancing methane production from WAS is economically attractive, particularly considering that iron scrap can be freely acquired from industrial waste. Based on these results, the ZVI-based anaerobic digestion process of this work could be easily integrated with the conventional chemical phosphorus removal process in wastewater treatment plant to form a cost-effective and environment-friendly approach, enabling maximum resource recovery/reuse while achieving enhanced methane production in wastewater treatment system.

Zero Valent Iron Significantly Enhances Methane Production from Waste Activated Sludge by Improving Biochemical Methane Potential Rather Than Hydrolysis Rate

PubMed Central

Liu, Yiwen; Wang, Qilin; Zhang, Yaobin; Ni, Bing-Jie

2015-01-01

Anaerobic digestion has been widely applied for waste activated sludge (WAS) treatment. However, methane production from anaerobic digestion of WAS is usually limited by the slow hydrolysis rate and/or poor biochemical methane potential of WAS. This work systematically studied the effects of three different types of zero valent iron (i.e., iron powder, clean scrap and rusty scrap) on methane production from WAS in anaerobic digestion, by using both experimental and mathematical approaches. The results demonstrated that both the clean and the rusty iron scrap were more effective than the iron powder for improving methane production from WAS. Model-based analysis showed that ZVI addition significantly enhanced methane production from WAS through improving the biochemical methane potential of WAS rather than its hydrolysis rate. Economic analysis indicated that the ZVI-based technology for enhancing methane production from WAS is economically attractive, particularly considering that iron scrap can be freely acquired from industrial waste. Based on these results, the ZVI-based anaerobic digestion process of this work could be easily integrated with the conventional chemical phosphorus removal process in wastewater treatment plant to form a cost-effective and environment-friendly approach, enabling maximum resource recovery/reuse while achieving enhanced methane production in wastewater treatment system. PMID:25652244

Zero Valent Iron Significantly Enhances Methane Production from Waste Activated Sludge by Improving Biochemical Methane Potential Rather Than Hydrolysis Rate

NASA Astrophysics Data System (ADS)

Liu, Yiwen; Wang, Qilin; Zhang, Yaobin; Ni, Bing-Jie

2015-02-01

Anaerobic digestion has been widely applied for waste activated sludge (WAS) treatment. However, methane production from anaerobic digestion of WAS is usually limited by the slow hydrolysis rate and/or poor biochemical methane potential of WAS. This work systematically studied the effects of three different types of zero valent iron (i.e., iron powder, clean scrap and rusty scrap) on methane production from WAS in anaerobic digestion, by using both experimental and mathematical approaches. The results demonstrated that both the clean and the rusty iron scrap were more effective than the iron powder for improving methane production from WAS. Model-based analysis showed that ZVI addition significantly enhanced methane production from WAS through improving the biochemical methane potential of WAS rather than its hydrolysis rate. Economic analysis indicated that the ZVI-based technology for enhancing methane production from WAS is economically attractive, particularly considering that iron scrap can be freely acquired from industrial waste. Based on these results, the ZVI-based anaerobic digestion process of this work could be easily integrated with the conventional chemical phosphorus removal process in wastewater treatment plant to form a cost-effective and environment-friendly approach, enabling maximum resource recovery/reuse while achieving enhanced methane production in wastewater treatment system.

A synthesis of growing-season, non-growing season, and annual methane emission measurements among temperate, boreal, and tundra wetlands and uplands

NASA Astrophysics Data System (ADS)

Treat, C. C.; Bloom, A. A.; Marushchak, M. E.

2017-12-01

Wetlands are the largest natural source of methane to the atmosphere, while upland soils are a consistent sink of atmospheric methane. Wetland methane emissions are highly variable among sites, years, and temporal scales due to differences in production, oxidation, and transport pathways. Currently, process model predictions of methane emissions from wetlands remain challenging due to uncertain parameterizations of net methane production and emission processes. Here, we synthesize growing season, non-growing season, and annual methane emissions from chamber and eddy-covariance measurements for more than 150 sites in undisturbed temperate, boreal, and tundra wetlands and uplands. We compare the magnitude of fluxes among regions, wetland classifications, vegetation classifications, and environmental variables. Growing season measurements were most abundant in bogs, fens, and tundra sites, while marshes and swamps were relatively undersampled. Annual methane emissions were largest from marshes and lowest from upland mineral soils. Non-growing season emissions accounted for large fraction of annual methane emissions, especially in tundra sites. These results provide constraints for methane emissions from temporal, boreal, and arctic wetlands utilizing the numerous flux measurements conducted over the past 25 years. We find that state-of-the-art model ensembles are seasonally biased; in particular, the vast majority of models overestimate predictions of the growing season to annual wetland methane emission ratio across all biomes.

Landscape-level terrestrial methane flux observed from a very tall tower

Treesearch

Ankur R. Desai; Ke Xu; Hanqin Tian; Peter Weishampel; Jonathan Thom; Dan Baumann; Arlyn E. Andrews; Druce D. Cook; Jennifer Y. King; Randall Kolka

2015-01-01

Simulating the magnitude and variability of terrestrial methane sources and sinks poses a challenge to ecosystem models because the biophysical and biogeochemical processes that lead to methane emissions from terrestrial and freshwater ecosystems are, by their nature, episodic and spatially disjunct. As a consequence, model predictions of regional methane emissions...

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.

Ultraviolet-radiation-induced methane emissions from meteorites and the Martian atmosphere.

PubMed

Keppler, Frank; Vigano, Ivan; McLeod, Andy; Ott, Ulrich; Früchtl, Marion; Röckmann, Thomas

2012-05-30

Almost a decade after methane was first reported in the atmosphere of Mars there is an intensive discussion about both the reliability of the observations--particularly the suggested seasonal and latitudinal variations--and the sources of methane on Mars. Given that the lifetime of methane in the Martian atmosphere is limited, a process on or below the planet's surface would need to be continuously producing methane. A biological source would provide support for the potential existence of life on Mars, whereas a chemical origin would imply that there are unexpected geological processes. Methane release from carbonaceous meteorites associated with ablation during atmospheric entry is considered negligible. Here we show that methane is produced in much larger quantities from the Murchison meteorite (a type CM2 carbonaceous chondrite) when exposed to ultraviolet radiation under conditions similar to those expected at the Martian surface. Meteorites containing several per cent of intact organic matter reach the Martian surface at high rates, and our experiments suggest that a significant fraction of the organic matter accessible to ultraviolet radiation is converted to methane. Ultraviolet-radiation-induced methane formation from meteorites could explain a substantial fraction of the most recently estimated atmospheric methane mixing ratios. Stable hydrogen isotope analysis unambiguously confirms that the methane released from Murchison is of extraterrestrial origin. The stable carbon isotope composition, in contrast, is similar to that of terrestrial microbial origin; hence, measurements of this signature in future Mars missions may not enable an unambiguous identification of biogenic methane.

Automatic Carbon Dioxide-Methane Gas Sensor Based on the Solubility of Gases in Water

PubMed Central

Cadena-Pereda, Raúl O.; Rivera-Muñoz, Eric M.; Herrera-Ruiz, Gilberto; Gomez-Melendez, Domingo J.; Anaya-Rivera, Ely K.

2012-01-01

Biogas methane content is a relevant variable in anaerobic digestion processing where knowledge of process kinetics or an early indicator of digester failure is needed. The contribution of this work is the development of a novel, simple and low cost automatic carbon dioxide-methane gas sensor based on the solubility of gases in water as the precursor of a sensor for biogas quality monitoring. The device described in this work was used for determining the composition of binary mixtures, such as carbon dioxide-methane, in the range of 0–100%. The design and implementation of a digital signal processor and control system into a low-cost Field Programmable Gate Array (FPGA) platform has permitted the successful application of data acquisition, data distribution and digital data processing, making the construction of a standalone carbon dioxide-methane gas sensor possible. PMID:23112626

Automatic carbon dioxide-methane gas sensor based on the solubility of gases in water.

PubMed

Cadena-Pereda, Raúl O; Rivera-Muñoz, Eric M; Herrera-Ruiz, Gilberto; Gomez-Melendez, Domingo J; Anaya-Rivera, Ely K

2012-01-01

Biogas methane content is a relevant variable in anaerobic digestion processing where knowledge of process kinetics or an early indicator of digester failure is needed. The contribution of this work is the development of a novel, simple and low cost automatic carbon dioxide-methane gas sensor based on the solubility of gases in water as the precursor of a sensor for biogas quality monitoring. The device described in this work was used for determining the composition of binary mixtures, such as carbon dioxide-methane, in the range of 0-100%. The design and implementation of a digital signal processor and control system into a low-cost Field Programmable Gate Array (FPGA) platform has permitted the successful application of data acquisition, data distribution and digital data processing, making the construction of a standalone carbon dioxide-methane gas sensor possible.

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

Can we reconcile our understanding of the atmospheric methane budget over the past decades with atmospheric observations?

NASA Astrophysics Data System (ADS)

Bruhwiler, L. M.; Matthews, E.

2007-12-01

The balance of methane in the atmosphere is determined by surface emission, and losses due to uptake in soils and reaction with the hydroxyl radical. The atmospheric abundance of methane has risen by about a factor of three since pre-industrial times, but the growth rate has decreased substantially since the 1990's. Thus, global atmospheric methane appears to have equilibrated to around 1780 ppb subject to considerable interannual variability, the causes of which are not well-understood. Methane emissions are expected to increase in the future due to increases in fossil fuel use and possible changes in wetlands at high-latitudes, and it is therefore important to test our understanding of the methane budget over the last two decades against network observations of atmospheric methane. Issues of interest are whether we can match the rise in methane over the 1980's, whether we can explain the decrease in growth rate during the 1990's, and whether we are able to simulate the observed interannual variability in the observations. We will show results from a multi-decade model simulation using analyzed meteorology from the ERA-40 reanalysis over this period. New times series of methane sources for 1980 through the early 2000's are used in the simulation. Anthropogenic sources include fossil fuels with a total of 7 fuel-process emission combinations associated with mining, processing, transport and distribution of coal, natural gas and oil; ruminant animals and manure based on regionally-representative profiles of bovine populations ; landfills including the impact of on- site methane capture; and irrigated rice cultivation based on seasonal rice-cropping calendars. Natural sources we include are biomass burning from the GFED emission data base, oceans, termites, and natural wetlands using a multiple-regression model derived from a process-based model. If time permits, we will also show preliminary results of a methane data assimilation using the Cooperative Air-Sampling and GMD network observations, and our new estimates of methane sources.

Methane Seepage on Mars: Where to Look and Why.

PubMed

Oehler, Dorothy Z; Etiope, Giuseppe

2017-12-01

Methane on Mars is a topic of special interest because of its potential association with microbial life. The variable detections of methane by the Curiosity rover, orbiters, and terrestrial telescopes, coupled with methane's short lifetime in the martian atmosphere, may imply an active gas source in the planet's subsurface, with migration and surface emission processes similar to those known on Earth as "gas seepage." Here, we review the variety of subsurface processes that could result in methane seepage on Mars. Such methane could originate from abiotic chemical reactions, thermogenic alteration of abiotic or biotic organic matter, and ancient or extant microbial metabolism. These processes can occur over a wide range of temperatures, in both sedimentary and igneous rocks, and together they enhance the possibility that significant amounts of methane could have formed on early Mars. Methane seepage to the surface would occur preferentially along faults and fractures, through focused macro-seeps and/or diffuse microseepage exhalations. Our work highlights the types of features on Mars that could be associated with methane release, including mud-volcano-like mounds in Acidalia or Utopia; proposed ancient springs in Gusev Crater, Arabia Terra, and Valles Marineris; and rims of large impact craters. These could have been locations of past macro-seeps and may still emit methane today. Microseepage could occur through faults along the dichotomy or fractures such as those at Nili Fossae, Cerberus Fossae, the Argyre impact, and those produced in serpentinized rocks. Martian microseepage would be extremely difficult to detect remotely yet could constitute a significant gas source. We emphasize that the most definitive detection of methane seepage from different release candidates would be best provided by measurements performed in the ground or at the ground-atmosphere interface by landers or rovers and that the technology for such detection is currently available. Key Words: Mars-Methane-Seepage-Clathrate-Fischer-Tropsch-Serpentinization. Astrobiology 17, 1233-1264.

METHOD FOR PRODUCING ISOTOPIC METHANES FROM LITHIUM CARBONATE AND LITHIUM HYDRIDE

DOEpatents

Frazer, J.W.

1959-10-27

A process is descrlbed for the production of methane and for the production of methane containing isotopes of hydrogen and/or carbon. Finely divided lithium hydrlde and litldum carbonate reactants are mixed in intimate contact and subsequently compacted under pressures of from 5000 to 60,000 psl. The compacted lithium hydride and lithium carbenate reactunts are dispised in a gas collecting apparatus. Subsequently, the compact is heated to a temperature in the range 350 to 400 deg C whereupon a solid-solid reaction takes place and gaseous methane is evolved. The evolved methane is contaminated with gaseous hydrogen and a very small amount of CO/sub 2/; however, the desired methane product is separated from sald impurities by well known chemical processes, e.g., condensation in a cold trap. The product methane contalns isotopes of carbon and hydrogen, the Isotopic composition being determined by the carbon isotopes originally present In the lithium carbonate and the hydrogen isotopes originally present in the lithium hydride.

Microbial and Isotopic Evidence for Methane Cycling in Hydrocarbon-Containing Groundwater from the Pennsylvania Region

PubMed Central

Vigneron, Adrien; Bishop, Andrew; Alsop, Eric B.; Hull, Kellie; Rhodes, Ileana; Hendricks, Robert; Head, Ian M.; Tsesmetzis, Nicolas

2017-01-01

The Pennsylvania region hosts numerous oil and gas reservoirs and the presence of hydrocarbons in groundwater has been locally observed. However, these methane-containing freshwater ecosystems remain poorly explored despite their potential importance in the carbon cycle. Methane isotope analysis and analysis of low molecular weight hydrocarbon gases from 18 water wells indicated that active methane cycling may be occurring in methane-containing groundwater from the Pennsylvania region. Consistent with this observation, multigenic qPCR and gene sequencing (16S rRNA genes, mcrA, and pmoA genes) indicated abundant populations of methanogens, ANME-2d (average of 1.54 × 104 mcrA gene per milliliter of water) and bacteria associated with methane oxidation (NC10, aerobic methanotrophs, methylotrophs; average of 2.52 × 103 pmoA gene per milliliter of water). Methane cycling therefore likely represents an important process in these hydrocarbon-containing aquifers. The microbial taxa and functional genes identified and geochemical data suggested that (i) methane present is at least in part due to methanogens identified in situ; (ii) Potential for aerobic and anaerobic methane oxidation is important in groundwater with the presence of lineages associated with both anaerobic an aerobic methanotrophy; (iii) the dominant methane oxidation process (aerobic or anaerobic) can vary according to prevailing conditions (oxic or anoxic) in the aquifers; (iv) the methane cycle is closely associated with the nitrogen cycle in groundwater methane seeps with methane and/or methanol oxidation coupled to denitrification or nitrate and nitrite reduction. PMID:28424678

Methodology of Estimation of Methane Emissions from Coal Mines in Poland

NASA Astrophysics Data System (ADS)

Patyńska, Renata

2014-03-01

Based on a literature review concerning methane emissions in Poland, it was stated in 2009 that the National Greenhouse Inventory 2007 [13] was published. It was prepared firstly to meet Poland's obligations resulting from point 3.1 Decision no. 280/2004/WE of the European Parliament and of the Council of 11 February 2004, concerning a mechanism for monitoring community greenhouse gas emissions and for implementing the Kyoto Protocol and secondly, for the United Nations Framework Convention on Climate Change (UNFCCC) and Kyoto Protocol. The National Greenhouse Inventory states that there are no detailed data concerning methane emissions in collieries in the Polish mining industry. That is why the methane emission in the methane coal mines of Górnośląskie Zagłębie Węglowe - GZW (Upper Silesian Coal Basin - USCB) in Poland was meticulously studied and evaluated. The applied methodology for estimating methane emission from the GZW coal mining system was used for the four basic sources of its emission. Methane emission during the mining and post-mining process. Such an approach resulted from the IPCC guidelines of 2006 [10]. Updating the proposed methods (IPCC2006) of estimating the methane emissions of hard coal mines (active and abandoned ones) in Poland, assumes that the methane emission factor (EF) is calculated based on methane coal mine output and actual values of absolute methane content. The result of verifying the method of estimating methane emission during the mining process for Polish coal mines is the equation of methane emission factor EF.

Freshwater wetland sediments support substantial rates of anaerobic oxidation of methane (AOM)

NASA Astrophysics Data System (ADS)

Segarra, K. E.; Samarkin, V.; Schubotz, F.; Yoshinaga, M. Y.; Hinrichs, K.; Joye, S. B.

2012-12-01

Freshwater wetlands are characterized by high rates of methanogenesis and are the single largest source of atmospheric methane. Anaerobic oxidation of methane (AOM), a previously underappreciated process in these systems, may be an important component in freshwater methane budgets. Here we report some of the first direct measurements of AOM in wetland sediments. We examined seasonal methane cycling within three freshwater wetlands (two peat wetlands and one tidal, freshwater creekbank) along the eastern coast of the US. Rates of AOM were high (up to 286 nmol per cubic cm per day) and varied on a seasonal basis. Despite low sulfate concentrations, rates of sulfate reduction were sufficient to support all the observed AOM activity, though rates of these two processes were not correlated. This study highlights the importance of AOM in freshwater sediments, where this process, in conjunction with sulfate reduction, may control emissions of methane to the atmosphere through competitive interactions with methanogens and the consumption of large fractions of the methane produced from acetate and hydrogen. The zone of maximum AOM activity was marked by enriched stable carbon isotopic signatures (δ13C) of methane and depleted signatures of DIC. However, the δ13C of archaeal and bacterial lipids were not indicative of methanotrophy. Studies that evaluate the role of AOM in wetlands using lipid and isotope-based approaches may therefore underestimate its importance.

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

PubMed

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

2017-11-07

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

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.

Optical-cell evidence for superheated ice under gas-hydrate-forming conditions

USGS Publications Warehouse

Stern, L.A.; Hogenboom, D.L.; Durham, W.B.; Kirby, S.H.; Chou, I.-Ming

1998-01-01

We previously reported indirect but compelling evidence that fine-grained H2O ice under elevated CH4 gas pressure can persist to temperatures well above its ordinary melting point while slowly reacting to form methane clathrate hydrate. This phenomenon has now been visually verified by duplicating these experiments in an optical cell while observing the very slow hydrate-forming process as the reactants were warmed from 250 to 290 K at methane pressures of 23 to 30 MPa. Limited hydrate growth occurred rapidly after initial exposure of the methane gas to the ice grains at temperatures well within the ice subsolidus region. No evidence for continued growth of the hydrate phase was observed until samples were warmed above the equilibrium H2O melting curve. With continued heating, no bulk melting of the ice grains or free liquid water was detected anywhere within the optical cell until hydrate dissociation conditions were reached (292 K at 30 MPa), even though full conversion of the ice grains to hydrate requires 6-8 h at temperatures approaching 290 K. In a separate experimental sequence, unreacted portions of H2O ice grains that had persisted to temperatures above their ordinary melting point were successfully induced to melt, without dissociating the coexisting hydrate in the sample tube, by reducing the pressure overstep of the equilibrium phase boundary and thereby reducing the rate of hydrate growth at the ice-hydrate interface. Results from similar tests using CO2 as the hydrate-forming species demonstrated that this superheating effect is not unique to the CH4-H2O system.

Low nitrogen fertilization adapts rice root microbiome to low nutrient environment by changing biogeochemical functions.

PubMed

Ikeda, Seishi; Sasaki, Kazuhiro; Okubo, Takashi; Yamashita, Akifumu; Terasawa, Kimihiro; Bao, Zhihua; Liu, Dongyan; Watanabe, Takeshi; Murase, Jun; Asakawa, Susumu; Eda, Shima; Mitsui, Hisayuki; Sato, Tadashi; Minamisawa, Kiwamu

2014-01-01

Reduced fertilizer usage is one of the objectives of field management in the pursuit of sustainable agriculture. Here, we report on shifts of bacterial communities in paddy rice ecosystems with low (LN), standard (SN), and high (HN) levels of N fertilizer application (0, 30, and 300 kg N ha(-1), respectively). The LN field had received no N fertilizer for 5 years prior to the experiment. The LN and HN plants showed a 50% decrease and a 60% increase in biomass compared with the SN plant biomass, respectively. Analyses of 16S rRNA genes suggested shifts of bacterial communities between the LN and SN root microbiomes, which were statistically confirmed by metagenome analyses. The relative abundances of Burkholderia, Bradyrhizobium and Methylosinus were significantly increased in root microbiome of the LN field relative to the SN field. Conversely, the abundance of methanogenic archaea was reduced in the LN field relative to the SN field. The functional genes for methane oxidation (pmo and mmo) and plant association (acdS and iaaMH) were significantly abundant in the LN root microbiome. Quantitative PCR of pmoA/mcrA genes and a (13)C methane experiment provided evidence of more active methane oxidation in the rice roots of the LN field. In addition, functional genes for the metabolism of N, S, Fe, and aromatic compounds were more abundant in the LN root microbiome. These results suggest that low-N-fertilizer management is an important factor in shaping the microbial community structure containing key microbes for plant associations and biogeochemical processes in paddy rice ecosystems.

Low Nitrogen Fertilization Adapts Rice Root Microbiome to Low Nutrient Environment by Changing Biogeochemical Functions

PubMed Central

Ikeda, Seishi; Sasaki, Kazuhiro; Okubo, Takashi; Yamashita, Akifumu; Terasawa, Kimihiro; Bao, Zhihua; Liu, Dongyan; Watanabe, Takeshi; Murase, Jun; Asakawa, Susumu; Eda, Shima; Mitsui, Hisayuki; Sato, Tadashi; Minamisawa, Kiwamu

2014-01-01

Reduced fertilizer usage is one of the objectives of field management in the pursuit of sustainable agriculture. Here, we report on shifts of bacterial communities in paddy rice ecosystems with low (LN), standard (SN), and high (HN) levels of N fertilizer application (0, 30, and 300 kg N ha−1, respectively). The LN field had received no N fertilizer for 5 years prior to the experiment. The LN and HN plants showed a 50% decrease and a 60% increase in biomass compared with the SN plant biomass, respectively. Analyses of 16S rRNA genes suggested shifts of bacterial communities between the LN and SN root microbiomes, which were statistically confirmed by metagenome analyses. The relative abundances of Burkholderia, Bradyrhizobium and Methylosinus were significantly increased in root microbiome of the LN field relative to the SN field. Conversely, the abundance of methanogenic archaea was reduced in the LN field relative to the SN field. The functional genes for methane oxidation (pmo and mmo) and plant association (acdS and iaaMH) were significantly abundant in the LN root microbiome. Quantitative PCR of pmoA/mcrA genes and a 13C methane experiment provided evidence of more active methane oxidation in the rice roots of the LN field. In addition, functional genes for the metabolism of N, S, Fe, and aromatic compounds were more abundant in the LN root microbiome. These results suggest that low-N-fertilizer management is an important factor in shaping the microbial community structure containing key microbes for plant associations and biogeochemical processes in paddy rice ecosystems. PMID:24463575

Methane emission from flooded soils - from microorganisms to the atmosphere

NASA Astrophysics Data System (ADS)

Conrad, Ralf

2016-04-01

Methane is an important greenhouse gas that is affected by anthropogenic activity. The annual budget of atmospheric methane, which is about 600 million tons, is by more than 75% produced by methanogenic archaea. These archaea are the end-members of a microbial community that degrades organic matter under anaerobic conditions. Flooded rice fields constitute a major source (about 10%) of atmospheric methane. After flooding of soil, anaerobic processes are initiated, finally resulting in the disproportionation of organic matter to carbon dioxide and methane. This process occurs in the bulk soil, on decaying organic debris and in the rhizosphere. The produced methane is mostly ventilated through the plant vascular system into the atmosphere. This system also allows the diffusion of oxygen into the rizosphere, where part of the produced methane is oxidized by aerobic methanotrophic bacteria. More than 50% of the methane production is derived from plant photosynthetic products and is formed on the root surface. Methanocellales are an important group of methanogenic archaea colonizing rice roots. Soils lacking this group seem to result in reduced root colonization and methane production. In rice soil methane is produced by two major paths of methanogenesis, the hydrogenotrophic one reducing carbon dioxide to methane, and the aceticlastic one disproportionating acetate to methane and carbon dioxide. Theoretically, at least two third of the methane should be produced by aceticlastic and the rest by hydrogenotrophic methanogenesis. In nature, however, the exact contribution of the two paths can vary from zero to 100%. Several environmental factors, such as temperature and quality of organic matter affect the path of methane production. The impact of these factors on the composition and activity of the environmental methanogenic microbial community will be discussed.

40 CFR 63.496 - Back-end process provisions-procedures to determine compliance using control or recovery devices.

Code of Federal Regulations, 2010 CFR

2010-07-01

... total organic HAP (or TOC, minus methane and ethane) emissions in all process vent streams and primary... TOC (minus methane and ethane) may be measured instead of total organic HAP. (C) The mass rates shall... and outlet of the control device shall be the sum of all total organic HAP (or TOC, minus methane and...

Industrial symbiosis: corn ethanol fermentation, hydrothermal carbonization, and anaerobic digestion.

PubMed

Wood, Brandon M; Jader, Lindsey R; Schendel, Frederick J; Hahn, Nicholas J; Valentas, Kenneth J; McNamara, Patrick J; Novak, Paige M; Heilmann, Steven M

2013-10-01

The production of dry-grind corn ethanol results in the generation of intermediate products, thin and whole stillage, which require energy-intensive downstream processing for conversion into commercial animal feed products. Hydrothermal carbonization of thin and whole stillage coupled with anaerobic digestion was investigated as alternative processing methods that could benefit the industry. By substantially eliminating evaporation of water, reductions in downstream energy consumption from 65% to 73% were achieved while generating hydrochar, fatty acids, treated process water, and biogas co-products providing new opportunities for the industry. Processing whole stillage in this manner produced the four co-products, eliminated centrifugation and evaporation, and substantially reduced drying. With thin stillage, all four co-products were again produced, as well as a high quality animal feed. Anaerobic digestion of the aqueous product stream from the hydrothermal carbonization of thin stillage reduced chemical oxygen demand (COD) by more than 90% and converted 83% of the initial COD to methane. Internal use of this biogas could entirely fuel the HTC process and reduce overall natural gas usage. Copyright © 2013 Wiley Periodicals, Inc.

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.

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

PubMed Central

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

2014-01-01

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

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

PubMed

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

2014-12-23

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

Novel applications for biogeophysics: Prospects for detecting key subseafloor geomicrobiological processes or habitats

NASA Astrophysics Data System (ADS)

Colwell, F. S.; Ntarlagiannis, D.

2007-05-01

The new subdiscipline of biogeophysics has focused mostly on the geophysical signatures of microbial processes in contaminated subsurface environments usually undergoing remediation. However, the use of biogeophysics to examine the biogeochemistry of marine sediments has not yet been well-integrated into conceptual models that describe subseafloor processes. Current examples of geophysical measurements that have been used to detect geomicrobiological processes or infer their location in the seafloor include sound surveillance system (SOSUS)-derived data that detect seafloor eruptive events, deep and shallow cross-sectional seismic surveys that determine the presence of hydraulically conductive zones or gas-bearing sediments (e.g., bottom-simulating reflectors or bubble-rich strata), and thermal profiles. One possible area for innovative biogeophysical characterization of the seafloor involves determining the depth of the sulfate-methane interface (SMI) in locations where sulfate diffuses from the seawater and methane emanates from subsurface strata. The SMI demarcates a stratum where microbially-driven anaerobic methane oxidation (AMO) is dependent upon methane as an electron donor and sulfate as an electron acceptor. AMO is carried out by a recently defined, unique consortium of microbes that metabolically temper the flux of methane into the overlying seawater. The depth of the SMI is, respectively, shallow or deep according to whether a high or low rate of methane flux occurs from the deep sediments. Presently, the SMI can only be determined by direct measurements of methane and sulfate concentrations in the interstitial waters or by molecular biological techniques that target the microbes responsible for creating the SMI. Both methods require collection and considerable analysis of sediment samples. Therefore, detection of the SMI by non-destructive methods would be advantageous. As a key biogeochemical threshold in marine sediments, the depth of the SMI defines methane charge in marine sediments, whether it is from dissolved methane or from methane hydrates. As such, a biogeophysical strategy for determining SMI depth would represent an important contribution to assessing methane charge with respect to climate change, sediment stability, or potential energy resources.

UV production of methane from surface and sedimenting IDPs on Mars in light of REMS data and with insights for TGO

NASA Astrophysics Data System (ADS)

Moores, John E.; Smith, Christina L.; Schuerger, Andrew C.

2017-11-01

This paper refines model predictions for the production of methane from UV-irradiated interplanetary dust particles (IDPs) now that the Rover Environmental Monitoring Station (REMS) instrument onboard the Mars Science Laboratory (MSL) Rover has made the first measurements of the UV environment on the surface of Mars, at Gale Crater. Once these measurements are included in a UV radiative transfer model, we find that modelled UV sol-integrated energies across the planet are lower than pre-measurement estimates by 35% on average, considering all latitudes and seasons. This reduction, in turn, reduces the predicted production of methane from individual accreting IDPs, extending their lifetimes and increasing the surface concentration of organics that must accumulate in order to emit sufficient methane to balance the accretion of organic compounds to Mars. Emission from reasonable accumulations of IDPs could range up to ∼7.9 × 10-4 ppbv sol-1. Richer deposits of organic carbon at the surface may emit methane at no more than 3.9 ppbv sol-1. An examination of IDP-derived methane production during atmospheric settling indicates that no more than 0.32% of organic carbon from meteor streams may be deposited in the atmosphere. Thus, such a process cannot explain either the spikes observed in methane nor the low equilibrium values observed by MSL. Instead, this discrepancy may be explained if < 80 tons per year of organic carbon survives to the surface, the atmospheric lifetime of methane is < 110 years or the efficiency of the UV-CH4 process is <7%. Under the assumption of reduced carbon input cycling in the Martian system from these processes, both soil concentrations of organic carbon and atmospheric measurements of methane observed by MSL are consistent with the UV-CH4 process. This refinement of methane production from IDPs and its geographical and vertical distribution will be an important input for models attempting to understand the results to be derived from the Trace Gas Orbiter (TGO) mission that will map methane concentrations in the martian atmosphere in 2018 at 0.01 ppbv.

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.

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.

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

PubMed

Wang, Dongbo; Zhao, Jianwei; Zeng, Guangming; Chen, Yinguang; Bond, Philip L; Li, Xiaoming

2015-10-20

Recent studies demonstrate that, besides being used for production of biodegradable plastics, poly(hydroxyalkanoate) (PHA) that is accumulated in heterotrophic microorganisms during wastewater treatment has another novel application direction, i.e., being utilized for enhancing methane yield during the anaerobic digestion of waste-activated sludge (WAS). To date, however, the underlying mechanism of how PHA affects methane production remains largely unknown, and this limits optimization and application of the strategy. This study therefore aims to fill this knowledge gap. Experimental results showed that with the increase of sludge PHA levels from 21 to 184 mg/g of volatile suspended solids (VSS) the methane yield linearly increased from 168.0 to 246.1 mL/g of VSS (R(2) = 0.9834). Compared with protein and carbohydrate (the main components of a cell), PHA exhibited a higher biochemical methane potential on a unit VSS basis. It was also found that the increased PHA not only enhanced cell disruption of PHA cells but also benefited the soluble protein conversion of both PHA- and non-PHA cells. Moreover, the reactor fed with higher PHA sludge showed greater sludge hydrolysis and acidification than those fed with the lower PHA sludges. Further investigations using fluorescence in situ hybridization and enzyme analysis revealed that the increased PHA enhanced the abundance of methanogenic Archaea and increased the activities of protease, acetate kinase, and coenzyme F420, which were consistent with the observed methane yield. This work provides insights into PHA-involved WAS digestion systems and may have important implications for future operation of wastewater treatment plants.

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

NASA Astrophysics Data System (ADS)

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

2009-08-01

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

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

PubMed

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

2015-03-01

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

Novel Catalysts and Processing Technologies for Production of Aerospace Fuels from Non-Petroleum Raw Materials

NASA Technical Reports Server (NTRS)

Hepp, Aloysius F.; Kulis, Michael J.; Psarras, Peter C.; Ball, David W.; Timko, Michael T.; Wong, Hsi-Wu; Peck, Jay; Chianelli, Russell R.

2014-01-01

Transportation fuels production (including aerospace propellants) from non-traditional sources (gases, waste materials, and biomass) has been an active area of research and development for decades. Reducing terrestrial waste streams simultaneous with energy conversion, plentiful biomass, new low-cost methane sources, and/or extra-terrestrial resource harvesting and utilization present significant technological and business opportunities being realized by a new generation of visionary entrepreneurs. We examine several new approaches to catalyst fabrication and new processing technologies to enable utilization of these nontraditional raw materials. Two basic processing architectures are considered: a single-stage pyrolysis approach that seeks to basically re-cycle hydrocarbons with minimal net chemistry or a two-step paradigm that involves production of supply or synthesis gas (mainly carbon oxides and H2) followed by production of fuel(s) via Sabatier or methanation reactions and/or Fischer-Tröpsch synthesis. Optimizing the fraction of product stream relevant to targeted aerospace (and other transportation) fuels via modeling, catalyst fabrication and novel reactor design are described. Energy utilization is a concern for production of fuels for either terrestrial or space operations; renewable sources based on solar energy and/or energy efficient processes may be mission enabling. Another important issue is minimizing impurities in the product stream(s), especially those potentially posing risks to personnel or operations through (catalyst) poisoning or (equipment) damage. Technologies being developed to remove (and/or recycle) heteroatom impurities are briefly discussed as well as the development of chemically robust catalysts whose activities are not diminished during operation. The potential impacts on future missions by such new approaches as well as balance of system issues are addressed.

Novel Catalysts and Processing Technologies for Production of Aerospace Fuels from Non-Petroleum Raw Materials

NASA Technical Reports Server (NTRS)

Hepp, A. F.; Kulis, M. J.; Psarras, P. C.; Ball, D. W.; Timko, M. T.; Wong, H.-W.; Peck, J.; Chianelli, R. R.

2014-01-01

Transportation fuels production (including aerospace propellants) from non-traditional sources (gases, waste materials, and biomass) has been an active area of research and development for decades. Reducing terrestrial waste streams simultaneous with energy conversion, plentiful biomass, new low-cost methane sources, and/or extra-terrestrial resource harvesting and utilization present significant technological and business opportunities being realized by a new generation of visionary entrepreneurs. We examine several new approaches to catalyst fabrication and new processing technologies to enable utilization of these non-traditional raw materials. Two basic processing architectures are considered: a single-stage pyrolysis approach that seeks to basically re-cycle hydrocarbons with minimal net chemistry or a two-step paradigm that involves production of supply or synthesis gas (mainly carbon oxides and hydrogen) followed by production of fuel(s) via Sabatier or methanation reactions and/or Fischer-Tropsch synthesis. Optimizing the fraction of product stream relevant to targeted aerospace (and other transportation) fuels via modeling, catalyst fabrication and novel reactor design are described. Energy utilization is a concern for production of fuels for either terrestrial or space operations; renewable sources based on solar energy and/or energy efficient processes may be mission enabling. Another important issue is minimizing impurities in the product stream(s), especially those potentially posing risks to personnel or operations through (catalyst) poisoning or (equipment) damage. Technologies being developed to remove (and/or recycle) heteroatom impurities are briefly discussed as well as the development of chemically robust catalysts whose activity are not diminished during operation. The potential impacts on future missions by such new approaches as well as balance of system issues are addressed.

Sulfide and methane production in sewer sediments: Field survey and model evaluation.

PubMed

Liu, Yiwen; Tugtas, A Evren; Sharma, Keshab R; Ni, Bing-Jie; Yuan, Zhiguo

2016-02-01

Sewer sediment processes have been reported to significantly contribute to overall sulfide and methane production in sewers, at a scale comparable to that of sewer biofilms. The physiochemical and biological characteristics of sewer sediments are heterogeneous; however, the variability of in-sediments sulfide and methane production rates among sewers has not been assessed to date. In this study, five sewer sediment samples were collected from two cities in Australia with different climatic conditions. Batch assays were conducted to determine the rates of sulfate reduction and methane production under different flow velocity (shear stress) conditions as well as under completely mixed conditions. The tests showed substantial and variable sulfate reduction and methane production activities among different sediments. Sulfate reduction and methane production from sewer sediments were confirmed to be areal processes, and were dependent on flow velocity/shear stress. Despite of the varying characteristics and reactions kinetics, the sulfate reduction and methane production processes in all sediments could be well described by a one-dimensional sewer sediment model recently developed based on results obtained from a laboratory sewer sediment reactor. Model simulations indicated that the in-situ contribution of sewer sediment emissions could be estimated without the requirement of measuring the specific sediment characteristics or the sediment depths. Copyright © 2015 Elsevier Ltd. All rights reserved.

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

NASA Astrophysics Data System (ADS)

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

2003-12-01

In order to mimic and study the process of anaerobic methane oxidation in methane hydrate regions we developed four high-pressure anaerobic bioreactors, designed to incubate environmental sediment samples, and enrich for populations of microbes associated with anaerobic methane oxidation (AMO). We obtained sediment inocula from a bacterial mat at the southern Hydrate Ridge, Cascadia, having cell counts approaching 1010 cells/cc. Ultimately, our goal is to produce an enriched culture of these microbes for characterization of the biochemical processes and chemical fluxes involved, as well as the unique adaptations required for, AMO. Molecular phylogenetic information along with results from fluorescent in situ hybridization indicate that consortia of Archaea and Bacteria are present which are related to those previously described for marine sediment AMO environments. Using a medium of enriched seawater and sediment in a 3:1 ratio, the system was incubated at 4° C under 43 atm of methane pressure; the temperature and pressure were kept constant. We have followed the reactions for seven months, particularly the vigorous consumption rates of dissolved sulfate and alkalinity production, as well as increases in HS-, and decreases in Ca concentrations. We also monitored the dissolved inorganic C (DIC) δ 13C values. The data were reproduced, and indicated that the process is extremely sensitive to changes in methane pressure. The rates of decrease in sulfate and increase in alkalinity concentrations were complimentary and showed considerable linearity with time. When the pressure in the reactor was decreased below the methane hydrate stability field, following the methane hydrate dissociation, sulfate reduction abruptly decreased. When the pressure was restored all the reactions returned to their previous rates. Much of the methane oxidation activity in the reactor is believed to occur in association with the methane hydrate. Upon the completion of one of the experiments, the chamber methane hydrate, liquid phase, and sediment were separated. FISH analyses of the dissociated hydrate fluid indicate a significant presence of Archaea in or on the hydrate. The cell densities in the bioreactor medium liquid phase were 7.2 x 107 cells/cc, and with the methane hydrate, 2.8 x 108 cells/cc.

Role of Biochar in Mitigation of Climate Change

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

Lehmann, Johannes C.; Amonette, James E.; Roberts, Kelli G.

2010-09-30

By virtue of the large fraction of the terrestrial carbon (C) cycle controlled by human activities, agroecosystems are both sources and sinks for greenhouse gases. Their potential role in mitigation of climate change thus depends on a dual strategy of decreasing greenhouse gas emissions while increasing sinks so that the net impact on climate warming is less than at present. Emissions of carbon dioxide, methane and nitrous oxide arise from various agricultural activities, ranging from land clearing to ploughing, fertilization, and animal husbandry. Reductions in these emissions can be achieved by decreasing the heterotrophic conversion of organic C to carbonmore » dioxide, and by better management of agricultural waste streams to minimize release of methane and nitrous oxide. Current sinks include C stored in standing biomass and soil organic matter, and the oxidation of atmospheric methane by soil bacteria. These sinks can be enhanced by increasing net primary productivity, thereby actively withdrawing more carbon dioxide from the atmosphere, and by promoting more oxidation of methane by soils. Judicious biochar management may contribute to both strategies, reductions of emissions by agriculture and active withdrawal of atmospheric carbon dioxide, as part of a comprehensive scheme in agricultural and forestry watersheds. Biochar is a carbon-rich organic material generated by heating biomass in the absence, or under a limited supply, of oxygen. This so-called charring or pyrolysis process has been used to produce charcoal as a source of fuel for millennia. Recently, interest has grown in understanding the potential of this process to improve soil health by adding biochar as an amendment to soil, to manage agricultural and forestry wastes, to generate energy, to decrease net emissions of nitrous oxide and methane, and to store carbon (C). The main incentive of biochar systems for mitigation of climate change is to increase the stability of organic matter or biomass. This stability is achieved by the conversion of fresh organic materials, which mineralize comparatively quickly, into biochar, which mineralizes much more slowly. The difference between the mineralization of uncharred and charred material results in a greater amount of carbon storage in soils and a lower amount of carbon dioxide, the major greenhouse gas, in the atmosphere. The principle of creating and managing biochar systems may address multiple environmental constraints. Biochar may help not only in mitigating climate change, but also fulfill a role in management of agricultural and forestry wastes, enhancement of soil sustainability, and generation of energy. Pyrolysis is a comparatively low-technology intervention. Deployment on a global scale, however, must be done carefully if the full mitigation potential is to be reached. Critical aspects of a successful implementation are that: 1) the biochar is sufficiently stable to reduce greenhouse gases in the atmosphere for an appropriate length of time. 2) the storage of carbon as biochar in soil is not offset by greenhouse gas emissions along the value chain of the system, such as mineralization of soil carbon or emissions of other greenhouse gases (e.g., methane and nitrous oxide). 3) net emission reductions are achieved for the entire life cycle of the system including indirect land use. 4) the biochar product does not cause unwanted side effects in soil. 5) the handling and production of biochar are in compliance with health and safety standards and do not pose hurdles to implementation. and 6) the biochar system is financially viable. This chapter discusses these issues in separate sections, identifies knowledge gaps, and proposes a road map to fully evaluate an environmentally and socially safe exploration of the biochar potential to mitigate climate change if adopted widely around the world.« less

Stimulation of methane generation from nonproductive coal by addition of nutrients or a microbial consortium

USGS Publications Warehouse

Jones, Elizabeth J.P.; Voytek, Mary A.; Corum, Margo D.; Orem, William H.

2010-01-01

Biogenic formation of methane from coal is of great interest as an underexploited source of clean energy. The goal of some coal bed producers is to extend coal bed methane productivity and to utilize hydrocarbon wastes such as coal slurry to generate new methane. However, the process and factors controlling the process, and thus ways to stimulate it, are poorly understood. Subbituminous coal from a nonproductive well in south Texas was stimulated to produce methane in microcosms when the native population was supplemented with nutrients (biostimulation) or when nutrients and a consortium of bacteria and methanogens enriched from wetland sediment were added (bioaugmentation). The native population enriched by nutrient addition included Pseudomonas spp., Veillonellaceae, and Methanosarcina barkeri. The bioaugmented microcosm generated methane more rapidly and to a higher concentration than the biostimulated microcosm. Dissolved organics, including long-chain fatty acids, single-ring aromatics, and long-chain alkanes accumulated in the first 39 days of the bioaugmented microcosm and were then degraded, accompanied by generation of methane. The bioaugmented microcosm was dominated by Geobacter sp., and most of the methane generation was associated with growth of Methanosaeta concilii. The ability of the bioaugmentation culture to produce methane from coal intermediates was confirmed in incubations of culture with representative organic compounds. This study indicates that methane production could be stimulated at the nonproductive field site and that low microbial biomass may be limiting in situ methane generation. In addition, the microcosm study suggests that the pathway for generating methane from coal involves complex microbial partnerships.