Methane clumped isotopes in the Songliao Basin (China): New insights into abiotic vs. biotic hydrocarbon formation

NASA Astrophysics Data System (ADS)

Shuai, Yanhua; Etiope, Giuseppe; Zhang, Shuichang; Douglas, Peter M. J.; Huang, Ling; Eiler, John M.

2018-01-01

Abiotic hydrocarbon gas, typically generated in serpentinized ultramafic rocks and crystalline shields, has important implications for the deep biosphere, petroleum systems, the carbon cycle and astrobiology. Distinguishing abiotic gas (produced by chemical reactions like Sabatier synthesis) from biotic gas (produced from degradation of organic matter or microbial activity) is sometimes challenging because their isotopic and molecular composition may overlap. Abiotic gas has been recognized in numerous locations on the Earth, although there are no confirmed instances where it is the dominant source of commercially valuable quantities in reservoir rocks. The deep hydrocarbon reservoirs of the Xujiaweizi Depression in the Songliao Basin (China) have been considered to host significant amounts of abiotic methane. Here we report methane clumped-isotope values (Δ18) and the isotopic composition of C1-C3 alkanes, CO2 and helium of five gas samples collected from those Xujiaweizi deep reservoirs. Some geochemical features of these samples resemble previously suggested identifiers of abiotic gas (13C-enriched CH4; decrease in 13C/12C ratio with increasing carbon number for the C1-C4 alkanes; abundant, apparently non-biogenic CO2; and mantle-derived helium). However, combining these constraints with new measurements of the clumped-isotope composition of methane and careful consideration of the geological context, suggests that the Xujiaweizi depression gas is dominantly, if not exclusively, thermogenic and derived from over-mature source rocks, i.e., from catagenesis of buried organic matter at high temperatures. Methane formation temperatures suggested by clumped-isotopes (167-213 °C) are lower than magmatic gas generation processes and consistent with the maturity of local source rocks. Also, there are no geological conditions (e.g., serpentinized ultramafic rocks) that may lead to high production of H2 and thus abiotic production of CH4 via CO2 reduction. We propose

The Hydrocarbon Fingerprints of Organic-rich Shales

NASA Astrophysics Data System (ADS)

Davies, S. J.; Sommariva, R.; Blake, R.; Ortega, M.; Cuss, R. J.; Harrington, J.; Emmings, J.; Lovell, M.; Monks, P.

2016-12-01

Geological characterization of key source rocks and potential unconventional reservoirs from the UK Mississippian has shed new light on the heterogeneous character of shales (mudstones) and also on the mechanisms for preserving organic matter of different types and abundances. Sedimentological studies of these mudstones suggest that systematic variations in total organic carbon (TOC) content are related to the dominant sediment delivery process (hemipelagic suspension settling vs. sediment gravity flows). Questions remain, however, as to how the physical character and chemical composition (e.g. lithology, mineralogy, organic matter type, maturity and abundance) of a mudstone relates to the volume and type of hydrocarbon gas that could be released. Using novel proof-of-principle laboratory experiments, we demonstrate that it is possible to quantify, in real-time (second by second), methane and a wide range of non-methane hydrocarbons (NMHC) gases as they are released from a crushed mudstone sample. Real time measurements are undertaken using proton-transfer-reaction time-of-flight mass spectrometry (PTR- TOF- MS). The PTR technique is not sensitive to some classes of NHMC and the whole range of hydrocarbons is analyzed using thermal desorption gas chromatography mass spectrometry (TD- GC- MS). Our data indicate that NMHC gases (mostly alkanes and aromatics) are released with temperature and humidity-dependent release rates, which depend on the physio-chemical characteristics of the different hydrocarbons classes and on the mode of storage within the shale. Knowledge of the abundance of methane and the speciated NMHC, and how that relates to geological characteristics of a mudstone is important to understand both the source rock potential and the potential pollutants. Ultimately, we aim to link these results to the geomechanical properties of shales. We discuss the implications of our findings for the environment and for the industrial and commercial exploitation of

Equilibrium and non-equilibrium controls on the abundances of clumped isotopologues of methane during thermogenic formation in laboratory experiments: Implications for the chemistry of pyrolysis and the origins of natural gases

NASA Astrophysics Data System (ADS)

Shuai, Yanhua; Douglas, Peter M. J.; Zhang, Shuichang; Stolper, Daniel A.; Ellis, Geoffrey S.; Lawson, Michael; Lewan, Michael D.; Formolo, Michael; Mi, Jingkui; He, Kun; Hu, Guoyi; Eiler, John M.

2018-02-01

Multiply isotopically substituted molecules ('clumped' isotopologues) can be used as geothermometers because their proportions at isotopic equilibrium relative to a random distribution of isotopes amongst all isotopologues are functions of temperature. This has allowed measurements of clumped-isotope abundances to be used to constrain formation temperatures of several natural materials. However, kinetic processes during generation, modification, or transport of natural materials can also affect their clumped-isotope compositions. Herein, we show that methane generated experimentally by closed-system hydrous pyrolysis of shale or nonhydrous pyrolysis of coal yields clumped-isotope compositions consistent with an equilibrium distribution of isotopologues under some experimental conditions (temperature-time conditions corresponding to 'low,' 'mature,' and 'over-mature' stages of catagenesis), but can have non-equilibrium (i.e., kinetically controlled) distributions under other experimental conditions ('high' to 'over-mature' stages), particularly for pyrolysis of coal. Non-equilibrium compositions, when present, lead the measured proportions of clumped species to be lower than expected for equilibrium at the experimental temperature, and in some cases to be lower than a random distribution of isotopes (i.e., negative Δ18 values). We propose that the consistency with equilibrium for methane formed by relatively low temperature pyrolysis reflects local reversibility of isotope exchange reactions involving a reactant or transition state species during demethylation of one or more components of kerogen. Non-equilibrium clumped-isotope compositions occur under conditions where 'secondary' cracking of retained oil in shale or wet gas hydrocarbons (C2-5, especially ethane) in coal is prominent. We suggest these non-equilibrium isotopic compositions are the result of the expression of kinetic isotope effects during the irreversible generation of methane from an alkyl

Temperature and injection water source influence microbial community structure in four Alaskan North Slope hydrocarbon reservoirs

PubMed Central

Piceno, Yvette M.; Reid, Francine C.; Tom, Lauren M.; Conrad, Mark E.; Bill, Markus; Hubbard, Christopher G.; Fouke, Bruce W.; Graff, Craig J.; Han, Jiabin; Stringfellow, William T.; Hanlon, Jeremy S.; Hu, Ping; Hazen, Terry C.; Andersen, Gary L.

2014-01-01

A fundamental knowledge of microbial community structure in petroleum reservoirs can improve predictive modeling of these environments. We used hydrocarbon profiles, stable isotopes, and high-density DNA microarray analysis to characterize microbial communities in produced water from four Alaskan North Slope hydrocarbon reservoirs. Produced fluids from Schrader Bluff (24–27°C), Kuparuk (47–70°C), Sag River (80°C), and Ivishak (80–83°C) reservoirs were collected, with paired soured/non-soured wells sampled from Kuparuk and Ivishak. Chemical and stable isotope data suggested Schrader Bluff had substantial biogenic methane, whereas methane was mostly thermogenic in deeper reservoirs. Acetoclastic methanogens (Methanosaeta) were most prominent in Schrader Bluff samples, and the combined δD and δ13C values of methane also indicated acetoclastic methanogenesis could be a primary route for biogenic methane. Conversely, hydrogenotrophic methanogens (e.g., Methanobacteriaceae) and sulfide-producing Archaeoglobus and Thermococcus were more prominent in Kuparuk samples. Sulfide-producing microbes were detected in all reservoirs, uncoupled from souring status (e.g., the non-soured Kuparuk samples had higher relative abundances of many sulfate-reducers compared to the soured sample, suggesting sulfate-reducers may be living fermentatively/syntrophically when sulfate is limited). Sulfate abundance via long-term seawater injection resulted in greater relative abundances of Desulfonauticus, Desulfomicrobium, and Desulfuromonas in the soured Ivishak well compared to the non-soured well. In the non-soured Ivishak sample, several taxa affiliated with Thermoanaerobacter and Halomonas predominated. Archaea were not detected in the deepest reservoirs. Functional group taxa differed in relative abundance among reservoirs, likely reflecting differing thermal and/or geochemical influences. PMID:25147549

Clouds, hazes, and the stratospheric methane abundance in Neptune

NASA Technical Reports Server (NTRS)

Baines, Kevin H.; Hammel, Heidi B.

1994-01-01

Analysis of high-spatial-resolution (approximately 0.8 arcsec) methane band and continuum imagery of Neptune's relatively homogeneous Equatorial Region yields significant constraints on (1) the stratospheric gaseous methane mixing ratio (f(sub CH4, S)), (2) the column abundances and optical properties of stratospheric and tropospheric hydrocarbon hazes, and (3) the wavelength-dependent single-scattering albedo of the 3-bar opaque cloud. From the center-to-limb behavior of the 7270-A and 8900-A CH4 bands, the stratospheric methane mixing ratios is limited to f(sub CH4, S) less than 1.7 x 10(exp -3), with a nominal value of f(sub CH4, S) = 3.5 x 10(exp -4), one to two orders of magnitude less than pre-Voyager estimates, but in agreement with a number of recent ultraviolet and thermal infrared measurements, and largely in agreement with the tropopause mixing ratio implied by Voyager temperature measurements. Upper limits to the stratospheric haze mass column abundance and 6190-A and 8900-A haze opacities are 0.61 micrograms/sq cm and 0.075 and 0.042, respectively, with nominal values of 0.20 micrograms/sq cm and 0.025 and 0.014 for the 0.2 micrometers radius particles preferred by the recent Voyager PPS analysis of Pryor et al. (1992). The tropospheric CH4 haze opacities are comparable to that found in the stratosphere, i.e., upper limits of 0.104 and 0.065 at 6190 A and 8900 A, respectively, with nominal values of 0.085 and 0.058. This indicates a column abundance less than 11.0 micrograms/sq cm, corresponding to the methane gas content within a well-mixed 3% methane tropospheric layer only 0.1 cm thick near the 1.5-bar CH4 condensation level. Conservative scattering is ruled out for the opaque cloud near 3 bars marking the bottom of the visible atmosphere. Specifically, we find cloud single-scattering albedos of 0.915 +/- 0.006 at 6340 A, 0.775 +/- 0.012 at 7490 A, and 0.803 +/- 0.010 at 8260 A. Global models utilizing a complete global spectrum confirm the red

Equilibrium and non-equilibrium controls on the abundances of clumped isotopologues of methane during thermogenic formation in laboratory experiments: Implications for the chemistry of pyrolysis and the origins of natural gases

USGS Publications Warehouse

Shuai, Yanhua; Douglas, Peter M.J.; Zhang, Shuichang; Stolper, Daniel A.; Ellis, Geoffrey S.; Lawson, Michael; Lewan, Michael; Formolo, Michael; Mi, Jingkui; He, Kun; Hu, Guoyi; Eiler, John M.

2018-01-01

Multiply isotopically substituted molecules (‘clumped’ isotopologues) can be used as geothermometers because their proportions at isotopic equilibrium relative to a random distribution of isotopes amongst all isotopologues are functions of temperature. This has allowed measurements of clumped-isotope abundances to be used to constrain formation temperatures of several natural materials. However, kinetic processes during generation, modification, or transport of natural materials can also affect their clumped-isotope compositions. Herein, we show that methane generated experimentally by closed-system hydrous pyrolysis of shale or nonhydrous pyrolysis of coal yields clumped-isotope compositions consistent with an equilibrium distribution of isotopologues under some experimental conditions (temperature–time conditions corresponding to ‘low,’ ‘mature,’ and ‘over-mature’ stages of catagenesis), but can have non-equilibrium (i.e., kinetically controlled) distributions under other experimental conditions (‘high’ to ‘over-mature’ stages), particularly for pyrolysis of coal. Non-equilibrium compositions, when present, lead the measured proportions of clumped species to be lower than expected for equilibrium at the experimental temperature, and in some cases to be lower than a random distribution of isotopes (i.e., negative Δ18 values). We propose that the consistency with equilibrium for methane formed by relatively low temperature pyrolysis reflects local reversibility of isotope exchange reactions involving a reactant or transition state species during demethylation of one or more components of kerogen. Non-equilibrium clumped-isotope compositions occur under conditions where ‘secondary’ cracking of retained oil in shale or wet gas hydrocarbons (C2-5, especially ethane) in coal is prominent. We suggest these non-equilibrium isotopic compositions are the result of the expression of kinetic isotope effects during the irreversible generation

Nitrogen oxides and methane treatment by non-thermal plasma

NASA Astrophysics Data System (ADS)

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

2015-03-01

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

Quantifying a Total Non-Methane Hydrocarbon Signal using Low-Cost VOC Sensors in an Effort to Help Communities Learn More About their Air Quality

NASA Astrophysics Data System (ADS)

Collier, A. M.; Hannigan, M.; Piedrahita, R.; Casey, J. G.; Johnston, J.; Chiang, S.

2016-12-01

The growing accessibility of low-cost air quality monitoring technologies has led to their increased usage among community-based organizations, particularly for the monitoring of pollutants dangerous to human health (e.g., hazardous air pollutants or HAPS). However, often these low-cost sensors are `off-the-shelf' and are being utilized in a manner that differs from their intended purpose - necessitating high quality calibrations. For example, VOC sensors intended for the detection of high levels of a particular compound in an industrial setting may instead be used for ambient monitoring of a group of VOCs. Academic/community partnerships can be an ideal way to improve this type of sensor quantification while providing a community with not only the opportunity to use these technologies with additional support around data quality, but also the opportunity for education around the abilities and applications of low-cost sensors. In the spring of 2016, our lab at the University of Colorado, Boulder partnered with communities in Los Angeles and Kern County to deploy low-cost air quality monitors for the purpose of quantifying methane and non-methane hydrocarbon signals in an effort to learn more about potential impacts from local sources (e.g., nearby highways and oil & gas development). The monitoring platform was developed in our lab and is capable of logging multiple gas phase species as well as some environmental parameters. The monitors include two different metal oxide VOC sensors - each with slightly different sensing capabilities. Calibration was achieved using a pre- and post-deployment field normalization to reference monitoring equipment maintained by the South Coast Air Quality Management District. Monitors were then deployed at locations throughout the community. We will present results on our efforts to quantify a total non-methane hydrocarbon signal, observations from the field data, and recommendations for academic/community partnerships formed around

Methane and benzene in drinking-water wells overlying the Eagle Ford, Fayetteville, and Haynesville Shale hydrocarbon production areas

USGS Publications Warehouse

McMahon, Peter B.; Barlow, Jeannie R.; Engle, Mark A.; Belitz, Kenneth; Ging, Patricia B.; Hunt, Andrew G.; Jurgens, Bryant; Kharaka, Yousif K.; Tollett, Roland W.; Kresse, Timothy M.

2017-01-01

Water wells (n = 116) overlying the Eagle Ford, Fayetteville, and Haynesville Shale hydrocarbon production areas were sampled for chemical, isotopic, and groundwater-age tracers to investigate the occurrence and sources of selected hydrocarbons in groundwater. Methane isotopes and hydrocarbon gas compositions indicate most of the methane in the wells was biogenic and produced by the CO2 reduction pathway, not from thermogenic shale gas. Two samples contained methane from the fermentation pathway that could be associated with hydrocarbon degradation based on their co-occurrence with hydrocarbons such as ethylbenzene and butane. Benzene was detected at low concentrations (<0.15 μg/L), but relatively high frequencies (2.4–13.3% of samples), in the study areas. Eight of nine samples containing benzene had groundwater ages >2500 years, indicating the benzene was from subsurface sources such as natural hydrocarbon migration or leaking hydrocarbon wells. One sample contained benzene that could be from a surface release associated with hydrocarbon production activities based on its age (10 ± 2.4 years) and proximity to hydrocarbon wells. Groundwater travel times inferred from the age-data indicate decades or longer may be needed to fully assess the effects of potential subsurface and surface releases of hydrocarbons on the wells.

Methane and Benzene in Drinking-Water Wells Overlying the Eagle Ford, Fayetteville, and Haynesville Shale Hydrocarbon Production Areas.

PubMed

McMahon, Peter B; Barlow, Jeannie R B; Engle, Mark A; Belitz, Kenneth; Ging, Patricia B; Hunt, Andrew G; Jurgens, Bryant C; Kharaka, Yousif K; Tollett, Roland W; Kresse, Timothy M

2017-06-20

Water wells (n = 116) overlying the Eagle Ford, Fayetteville, and Haynesville Shale hydrocarbon production areas were sampled for chemical, isotopic, and groundwater-age tracers to investigate the occurrence and sources of selected hydrocarbons in groundwater. Methane isotopes and hydrocarbon gas compositions indicate most of the methane in the wells was biogenic and produced by the CO 2 reduction pathway, not from thermogenic shale gas. Two samples contained methane from the fermentation pathway that could be associated with hydrocarbon degradation based on their co-occurrence with hydrocarbons such as ethylbenzene and butane. Benzene was detected at low concentrations (<0.15 μg/L), but relatively high frequencies (2.4-13.3% of samples), in the study areas. Eight of nine samples containing benzene had groundwater ages >2500 years, indicating the benzene was from subsurface sources such as natural hydrocarbon migration or leaking hydrocarbon wells. One sample contained benzene that could be from a surface release associated with hydrocarbon production activities based on its age (10 ± 2.4 years) and proximity to hydrocarbon wells. Groundwater travel times inferred from the age-data indicate decades or longer may be needed to fully assess the effects of potential subsurface and surface releases of hydrocarbons on the wells.

Separation of C2 hydrocarbons from methane in a microporous metal-organic framework

NASA Astrophysics Data System (ADS)

Tang, Fu-Shun; Lin, Rui-Biao; Lin, Rong-Guang; Zhao, John Cong-Gui; Chen, Banglin

2018-02-01

The recovery of C2 hydrocarbons including acetylene, ethylene and ethane is challenging but important for natural gas upgrading. The separation of C2 hydrocarbons over methane was demonstrated here by using a microporous metal-organic framework [Zn3(OH)2(SDB)2] (H2SDB = 4,4'-sulfonyldibenzoic acid) consisting narrow one-dimensional pore channels. Gas sorption experiments revealed that this MOF material showed considerable uptake capacity for C2H2, C2H4 and C2H6 under ambient conditions, while its capacity for CH4 was very low. High selectivity from IAST calculations for C2H2/CH4, C2H4/CH4 and C2H6/CH4 binary mixtures demonstrated that this MOF material were promising for efficiently separating important separation of C2 hydrocarbons from methane in natural gas processing.

Biodegradation of individual and multiple chlorinated aliphatic hydrocarbons by methane-oxidizing cultures.

PubMed Central

Chang, H L; Alvarez-Cohen, L

1996-01-01

The microbial degradation of chlorinated and nonchlorinated methanes, ethanes, and ethanes by a mixed methane-oxidizing culture grown under chemostat and batch conditions is evaluated and compared with that by two pure methanotrophic strains: CAC1 (isolated from the mixed culture) and Methylosinus trichosporium OB3b. With the exception of 1,1-dichloroethylene, the transformation capacity (Tc) for each chlorinated aliphatic hydrocarbon was generally found to be in inverse proportion to its chlorine content within each aliphatic group (i.e., methanes, ethanes, and ethenes), whereas similar trends were not observed for degradation rate constants. Tc trends were similar for all methane-oxidizing cultures tested. None of the cultures were able to degrade the fully chlorinated aliphatics such as perchloroethylene and carbon tetrachloride. Of the four cultures tested, the chemostat-grown mixed culture exhibited the highest Tc for trichloroethylene, cis-1,2-dichloroethylene, tetrachloroethane, 1,1,1-trichloroethane, and 1,2-dichloroethane, whereas the pure batch-grown OB3b culture exhibited the highest Tc for all other compounds tested. The product toxicity of chlorinated aliphatic hydrocarbons in a mixture containing multiple compounds was cumulative and predictable when using parameters measured from the degradation of individual compounds. The Tc for each chlorinated aliphatic hydrocarbon in a mixture (Tcmix) and the total Tc for the mixture (sigma Tcmix) are functions of the individual Tc, the initial substrate concentration (S0), and the first-order rate constant (k/Ks) of each compound in the mixture, indicating the importance of identifying the properties and compositions of all potentially degradable compounds in a contaminant mixture. PMID:8795228

Vertical Distribution of Non-Methane Hydrocarbons During Winter Ozone Production Events in the Uintah Basin

NASA Astrophysics Data System (ADS)

Stephens, C. R.; Helmig, D.; Evans, J.; Hueber, J.; Park, J.; Boylan, P.

2013-12-01

Emissions of non-methane hydrocarbons (NMHC) are primarily linked to anthropogenic fossil fuel activities, such as oil and natural gas extraction and distribution, and are important tropospheric ozone precursors. The Uintah Basin, Utah, is a region of heavy oil and natural gas development where high winter-time ozone production events have been observed during strong inversions when there is snow cover present. In the winters of 2012 and 2013, we conducted measurements of methane and NMHC during the Uintah Basin Winter Ozone Study. NMHC were monitored along a vertical gradient up to 150 m using a flux tower and tethered balloon. In 2013, measurements of NMHC were also conducted from within the snowpack. In 2012, no high ozone events were observed. In contrast, during the 2013 study, several periods of high ozone occurred concurrently with strong increases in ambient NMHC. Here, we present vertical profile measurements of C2-C5 alkanes, benzene and toluene comparing 2012 and 2013. Data from 2013 show strong vertical gradients with build-up of NMHC and ozone near the surface during inversion events, with wash out of both ozone and ozone precursors during low pressure front passage from the west. The NOAA/INSTAAR global flask network provides a useful comparison for expected regional background values of NMHC, and we find up to a 570-fold enhancement in Uintah, providing evidence for the importance of local emissions sources. Investigation of NMHC ratios reveals distinctly different values in the ambient air and within the snowpack, suggesting active radical chemistry occurring in the snow. Analysis of butane and pentane isomer ratios points towards the presence of chlorine radicals, indicating that the snow may serve as a reactive chlorine reservoir that may enhance ozone production chemistry.

Chemical models of interstellar gas-grain processes. II - The effect of grain-catalysed methane on gas phase evolution

NASA Technical Reports Server (NTRS)

Brown, Paul D.; Charnley, S. B.

1991-01-01

The effects on gas phase chemistry which result from the continuous desorption of methane molecules from grain surfaces are studied. Significant and sustained enhancements in the abundances of several complex hydrocarbon molecules are found, in good agreement with their observed values in TMC-1. The overall agreement is, however, just as good for the case of zero CH4 desorption efficiency. It is thus impossible to determine from the models whether or not the grain-surface production of methane is responsible for the observed abundances of some hydrocarbon molecules.

Impact of natural oil and higher hydrocarbons on microbial diversity, distribution, and activity in Gulf of Mexico cold-seep sediments

NASA Astrophysics Data System (ADS)

Orcutt, Beth N.; Joye, Samantha B.; Kleindienst, Sara; Knittel, Katrin; Ramette, Alban; Reitz, Anja; Samarkin, Vladimir; Treude, Tina; Boetius, Antje

2010-11-01

Gulf of Mexico cold seeps characterized by variable compositions and magnitudes of hydrocarbon seepage were sampled in order to investigate the effects of natural oils, methane, and non-methane hydrocarbons on microbial activity, diversity, and distribution in seafloor sediments. Though some sediments were characterized by relatively high quantities of oil, which may be toxic to some microorganisms, high rates of sulfate reduction (SR, 27.9±14.7 mmol m-2 d-1), anaerobic oxidation of methane (AOM, 16.2±6.7 mmol m-2 d-1), and acetate oxidation (2.74±0.76 mmol m-2 d-1) were observed in radiotracer measurements. In many instances, the SR rate was higher than the AOM rate, indicating that non-methane hydrocarbons fueled SR. Analysis of 16S rRNA gene clone libraries revealed phylogenetically diverse communities that were dominated by phylotypes of sulfate-reducing bacteria (SRB) and anaerobic methanotrophs of the ANME-1 and ANME-2 varieties. Another group of archaea form a Gulf of Mexico-specific clade (GOM ARC2) that may be important in brine-influenced, oil-impacted sediments from deeper water. Additionally, species grouping within the uncultivated Deltaproteobacteria clades SEEP-SRB3 and -SRB4, as well as relatives of Desulfobacterium anilini, were observed in relatively higher abundance in the oil-impacted sediments, suggesting that these groups of SRB may be involved in or influenced by degradation of higher hydrocarbons or petroleum byproducts.

Catalytic co-aromatization of ethanol and methane

DOE PAGES

Wang, Aiguo; He, Peng; Yung, Matthew; ...

2016-06-06

This study demonstrates the technical feasibility of simultaneously converting ethanol and methane into liquid hydrocarbons at mild reaction conditions (400 °C and 1 atm) over silver and/or zinc modified zeolite catalysts. After GC-MS analysis, it is worth noting that aromatics are the major compounds contained in the liquid product collected from the run when 1%Ag/ZSM-5, particularly after H 2 pretreatment, is charged. Compared to the performance exhibited from the run with pure HZSM-5 support engaged, Ag addition into the HZSM-5 framework favors aromatics formation, which might be closely associated with better Ag dispersion and more abundance of strong surface acidicmore » sites where aromatization might take place while Zn loading exerts a detrimental effect on the production of aromatics but promotes the ether generation possibly through dehydration reaction. Referred to that from its N 2 counterpart, the increased aromatics formation of the collected liquid product when methane is present indicates that methane existence might facilitate ethanol aromatization. Moreover, combined with the increased carbon number in the formed aromatics from CH 4 run when H 2 run is referred and zero liquid formation from CH 4-alone test as well as more prominent endothermic feature of methane run and more importantly the notably increased 13C signals in 13C NMR spectra of the liquid product collected during ethanol conversion under 13CH 4 environment, all the observations suggest that methane might be activated nonoxidatively and converted into higher hydrocarbons, preferentially into aromatics if suitable catalyst is charged under the assistance of co-existing oxygenated hydrocarbon. Lastly, the reported synergetic effect could potentially lead to the more economic utilization of abundant natural gas and cellulosic ethanol.« less

Methane-oxidizing seawater microbial communities from an Arctic shelf

NASA Astrophysics Data System (ADS)

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

2018-06-01

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

Methane Provenance Determined by CH2D2 and 13CH3D Abundances

NASA Astrophysics Data System (ADS)

Kohl, I. E.; Giunta, T.; Warr, O.; Ash, J. L.; Ruffine, L.; Sherwood Lollar, B.; Young, E. D.

2017-12-01

Determining the provenance of naturally occurring methane gases is of major interest to energy companies and atmospheric climate modelers, among others. Bulk isotopic compositions and other geochemical tracers sometimes fail to provide definitive determinations of sources of methane due to complications from mixing and complicated chemical pathways of origin. Recent measurements of doubly-substituted isotopologues of methane, CH2D2 (UCLA) and 13CH3D (UCLA, CalTech, and MIT) have allowed for major improvements in sourcing natural methane gases. Early work has focused on formation temperatures obtained when the relative abundances of both doubly-substituted mass-18 species are consistent with internal equilibrium. When methane gases do not plot on the thermodynamic equilibrium curve in D12CH2D2 vs D13CH3D space, temperatures determined from D13CH3D values alone are usually spurious, even when appearing reasonable. We find that the equilibrium case is actually rare and almost exclusive to thermogenic gases produced at temperatures exceeding 100°C. All other relevant methane production processes appear to generate gases that are not in isotopologue-temperature equilibrium. When gases show departures from equilibrium as determined by the relationship between CH2D2 and 13CH3D abundances, data fall within empirically defined fields representing formation pathways. These fields are thus far consistent between different geological settings and and between lab experiments and natural samples. We have now defined fields for thermogenic gas production, microbial methanogenesis, low temperature abiotic (Sabatier) synthesis and higher temperature FTT synthesis. The majority of our natural methane data can be explained by mixing between end members originating within these production fields. Mixing can appear complex, resulting in both hyper-clumped and anti-clumped isotopologue abundances. In systems where mixtures dominate and end-members are difficult to sample, mixing models

The importance of the southern ocean on distributions and lifetimes of non-methane organic compounds

NASA Astrophysics Data System (ADS)

Apel, E. C.; Asher, E.; Hills, A. J.; Hornbrook, R. S.; Emmons, L. K.; Blake, N. J.; Stephens, B. B.

2017-12-01

During the ORCAS (O2/N2 Ratio and CO2 Airborne Southern Ocean) campaign, a large number of volatile organic compounds (VOCs) were observed using Trace Organic Gas Analyzer (TOGA) including non-methane hydrocarbons (NMHCs), halogenated volatile organic compounds (HVOCs), oxygenated VOCs (OVOCs), alkyl nitrates, and nitriles. Mixing ratios of VOCs with known continental sources observed during ORCAS were very low in comparison to measurements made over tropical and mid-latitude Pacific Ocean using the same instrumentation during previous January-February field campaigns, TORERO (Tropical Ocean tRoposphere Exchange of Reactive halogen species and Oxygenated VOC, 2012) and CONTRAST (CONvective Transport of Active Species in the Tropics, 2014). The ORCAS dataset provides some of the first observations of Southern Hemisphere distributions of several of the most abundant non-methane VOCs in the atmosphere including acetone, hydrogen cyanide (HCN), methanol, and acetonitrile. Although the majority of the sources for these species are continental, the ocean's role as a sink for HCN and acetonitrile and as a net source or sink for methanol and acetone is not fully understood and this will be investigated using CAM-chem (Community Atmosophere model with chemistry). The southern oceans studied during ORCAS will provide key missing information on this and relationships of these VOCs to CO2 and O2 will provide a means to constrain the influence of continental emissions and transport from mid-latitudes on air masses encountered over the Southern Ocean.

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

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

Wilson, R.B. Jr.; Posin, B.M.; Chan, Yee Wai

The goal of this research is to develop catalysts that directly convert methane and light hydrocarbons to intermediates that later can be converted to either liquid fuels or value-added chemicals, as economics dictate. During this reporting period, we completed our IR spectroscopic examination of the Ru{sub 4}/MgO and FeRu{sub 3}/MgO systems under nitrogen and methane by examining FeRu{sub 3}/MgO under methane. This system behaved quite differently than the same system under nitrogen. Under methane, only one very broad peak is observed at room temperature. Upon heating, the catalyst transformed so that by 300{degrees}C, the spectrum of FeRu{sub 3}/MgO under methanemore » was the same as that of Ru{sub 4}/MgO. This suggests that methane promotes the segregation of the metals in the mixed metal system. The differences in catalytic activity between the FeRu{sub 3}/MgO and Ru{sub 4}/MgO systems may then be due to the presence of IR transparent species such as iron ions which cause different nucleation in the ruthenium clusters. We examined several systems for activity in the methane dehydrogenation reaction. Focusing on systems which produce C{sub 6} hydrocarbons since this is the most useful product. These systems all displayed low activity so that the amount of hydrocarbon product is very low. Some C{sub 6} hydrocarbon is observed over zeolite supports, but its production ceases after the first few hours of reaction. We prepared a new system, Ru{sub 4} supported on carbon, and examined its reactivity. Its activity was very low and in fact the carbon support had the same level of activity. We synthesized four new systems for examination as catalysts in the partial oxidation of methane. Three of these (PtTSPC/MgO, PtTSPC and PdTSPC on carbon) are analogs of PdTSPC/MgO. This system is of interest because we have observed the production of ethane from methane oxidation over PdTSPC/MgO at relatively low temperatures and we wished to explore its generality among close

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.

Shallow Gas Migration along Hydrocarbon Wells-An Unconsidered, Anthropogenic Source of Biogenic Methane in the North Sea.

PubMed

Vielstädte, Lisa; Haeckel, Matthias; Karstens, Jens; Linke, Peter; Schmidt, Mark; Steinle, Lea; Wallmann, Klaus

2017-09-05

Shallow gas migration along hydrocarbon wells constitutes a potential methane emission pathway that currently is not recognized in any regulatory framework or greenhouse gas inventory. Recently, the first methane emission measurements at three abandoned offshore wells in the Central North Sea (CNS) were conducted showing that considerable amounts of biogenic methane originating from shallow gas accumulations in the overburden of deep reservoirs were released by the boreholes. Here, we identify numerous wells poking through shallow gas pockets in 3-D seismic data of the CNS indicating that about one-third of the wells may leak, potentially releasing a total of 3-17 kt of methane per year into the North Sea. This poses a significant contribution to the North Sea methane budget. A large fraction of this gas (∼42%) may reach the atmosphere via direct bubble transport (0-2 kt yr -1 ) and via diffusive exchange of methane dissolving in the surface mixed layer (1-5 kt yr -1 ), as indicated by numerical modeling. In the North Sea and in other hydrocarbon-prolific provinces of the world shallow gas pockets are frequently observed in the sedimentary overburden and aggregate leakages along the numerous wells drilled in those areas may be significant.

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

Methane-Oxidizing Bacteria Shunt Carbon to Microbial Mats at a Marine Hydrocarbon Seep

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

Paul, Blair G.; Ding, Haibing; Bagby, Sarah C.

The marine subsurface is a reservoir of the greenhouse gas methane. While microorganisms living in water column and seafloor ecosystems are known to be a major sink limiting net methane transport from the marine subsurface to the atmosphere, few studies have assessed the flow of methane-derived carbon through the benthic mat communities that line the seafloor on the continental shelf where methane is emitted. We analyzed the abundance and isotope composition of fatty acids in microbial mats grown in the shallow Coal Oil Point seep field off Santa Barbara, CA, USA, where seep gas is a mixture of methane andmore » CO 2. We further used stable isotope probing (SIP) to track methane incorporation into mat biomass. We found evidence that multiple allochthonous substrates supported the rich growth of these mats, with notable contributions from bacterial methanotrophs and sulfur-oxidizers as well as eukaryotic phototrophs. Fatty acids characteristic of methanotrophs were shown to be abundant and 13C-enriched in SIP samples, and DNA-SIP identified members of the methanotrophic family Methylococcaceae as major 13CH 4 consumers. Members of Sulfuricurvaceae, Sulfurospirillaceae, and Sulfurovumaceae are implicated in fixation of seep CO 2. The mats’ autotrophs support a diverse assemblage of co-occurring bacteria and protozoa, with Methylophaga as key consumers of methane-derived organic matter. This study identifies the taxa contributing to the flow of seep-derived carbon through microbial mat biomass, revealing the bacterial and eukaryotic diversity of these remarkable ecosystems.« less

Methane-Oxidizing Bacteria Shunt Carbon to Microbial Mats at a Marine Hydrocarbon Seep

DOE PAGES

Paul, Blair G.; Ding, Haibing; Bagby, Sarah C.; ...

2017-02-27

The marine subsurface is a reservoir of the greenhouse gas methane. While microorganisms living in water column and seafloor ecosystems are known to be a major sink limiting net methane transport from the marine subsurface to the atmosphere, few studies have assessed the flow of methane-derived carbon through the benthic mat communities that line the seafloor on the continental shelf where methane is emitted. We analyzed the abundance and isotope composition of fatty acids in microbial mats grown in the shallow Coal Oil Point seep field off Santa Barbara, CA, USA, where seep gas is a mixture of methane andmore » CO 2. We further used stable isotope probing (SIP) to track methane incorporation into mat biomass. We found evidence that multiple allochthonous substrates supported the rich growth of these mats, with notable contributions from bacterial methanotrophs and sulfur-oxidizers as well as eukaryotic phototrophs. Fatty acids characteristic of methanotrophs were shown to be abundant and 13C-enriched in SIP samples, and DNA-SIP identified members of the methanotrophic family Methylococcaceae as major 13CH 4 consumers. Members of Sulfuricurvaceae, Sulfurospirillaceae, and Sulfurovumaceae are implicated in fixation of seep CO 2. The mats’ autotrophs support a diverse assemblage of co-occurring bacteria and protozoa, with Methylophaga as key consumers of methane-derived organic matter. This study identifies the taxa contributing to the flow of seep-derived carbon through microbial mat biomass, revealing the bacterial and eukaryotic diversity of these remarkable ecosystems.« less

Methane-Oxidizing Bacteria Shunt Carbon to Microbial Mats at a Marine Hydrocarbon Seep

PubMed Central

Paul, Blair G.; Ding, Haibing; Bagby, Sarah C.; Kellermann, Matthias Y.; Redmond, Molly C.; Andersen, Gary L.; Valentine, David L.

2017-01-01

The marine subsurface is a reservoir of the greenhouse gas methane. While microorganisms living in water column and seafloor ecosystems are known to be a major sink limiting net methane transport from the marine subsurface to the atmosphere, few studies have assessed the flow of methane-derived carbon through the benthic mat communities that line the seafloor on the continental shelf where methane is emitted. We analyzed the abundance and isotope composition of fatty acids in microbial mats grown in the shallow Coal Oil Point seep field off Santa Barbara, CA, USA, where seep gas is a mixture of methane and CO2. We further used stable isotope probing (SIP) to track methane incorporation into mat biomass. We found evidence that multiple allochthonous substrates supported the rich growth of these mats, with notable contributions from bacterial methanotrophs and sulfur-oxidizers as well as eukaryotic phototrophs. Fatty acids characteristic of methanotrophs were shown to be abundant and 13C-enriched in SIP samples, and DNA-SIP identified members of the methanotrophic family Methylococcaceae as major 13CH4 consumers. Members of Sulfuricurvaceae, Sulfurospirillaceae, and Sulfurovumaceae are implicated in fixation of seep CO2. The mats’ autotrophs support a diverse assemblage of co-occurring bacteria and protozoa, with Methylophaga as key consumers of methane-derived organic matter. This study identifies the taxa contributing to the flow of seep-derived carbon through microbial mat biomass, revealing the bacterial and eukaryotic diversity of these remarkable ecosystems. PMID:28289403

Methane Leakage From Hydrocarbon Wellbores into Overlying Groundwater: Numerical Investigation of the Multiphase Flow Processes Governing Migration

NASA Astrophysics Data System (ADS)

Rice, Amy K.; McCray, John E.; Singha, Kamini

2018-04-01

Methane leakage due to compromised hydrocarbon well integrity can lead to impaired groundwater quality. Here we use a three-dimensional, multiphase (vapor and aqueous), multicomponent (methane, water, salt), numerical model (TOUGH2 EOS7C) to investigate hydrogeological conditions that could result in groundwater contamination from natural gas wellbore leakage that migrates upward toward a freshwater aquifer. The conceptual model used for the simulations assumes methane leakage at 20-30 m below groundwater. We perform 180 simulations for a sensitivity analysis, examining (1) multiphase flow parameters related to storage, capillarity, and relative permeability, including porosity (ϕ), initial fluid-phase saturation (SL), and van Genuchten n and α, (2) geostatistical variations in intrinsic permeability (ki), and (3) methane source-zone pressure. Simulated mean ki values are 10-18 and 10-13 m2 with variances of 1 and 5 m4. Simulated source-zone pressures range from just over ambient hydrostatic pressure at the depth of leakage (100 kPa) to the maximum pressure that steel casings are commonly rated to withstand (20,340 kPa). ki, initial SL, ϕ, and van Genuchten's n and α were the most important parameters in determining the volume of methane reaching groundwater during a given time period. Multiphase parameterization of formations underlying freshwater aquifers and overlying hydrocarbon production zones is fundamental to assessing aquifer vulnerability to methane leakage.

Methanotrophic gastropods from a bathyal hydrocarbon seep, Gulf of Mexico

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

Anderson, L.C.; Aharon, P.; Gupta, S.

Two gastropods, Neritina sp. and Truncatella sp., collected live from a Gulf of Mexico active gas seep with the submersible Johnson Sea Link in September 1991, apparently incorporate methane-derived carbon in their soft tissues. Flesh of an individual Neritina sp. had a delta C-13 of [minus]50.92 per mil PDB, and that of two coexisting individuals of Truncatella sp. had values of [minus]45.11 and [minus]49.27 per mil. These isotope values are comparable to those reported for the methanotrophic mytilid bivalve Bathymodiolus sp. from other hydrocarbon seeps on the Gulf of Mexico, and are lighter than published isotopic values of chemosynthetic organismsmore » with sulfur-oxidizing symbionts. The anomalously light carbon-isotopic values of Neritina sp. and Truncatella sp. may steam from one of three causes: (1) these gastropods host symbiotic methanotrophic bacteria, (2) their chief food is methane-oxidizing bacteria present at the seep, or (3) they incorporate some carbon from the periostracum of mussels on which they may graze. The presence of abundant juveniles of Bathymodiolus, reported to settle preferentially in areas of active seepage and high methane release, indicates that methane was abundant and supported a community with multiple trophic levels. Generally, studies of hydrocarbon-seep communities have focused on larger community members, especially bivalves and tube worms. The presence of living Neritina and Truncatella at the authors sampling site, however, draws attention to the fact that these gastropods are integral and significant parts of hydrocarbon-seep communities. Both gastropod species are members of genera that characteristically inhabit shallow marine, intertidal, and semiterrestrial environments. The presence of these genera in bathyal hydrocarbon seeps indicates that they have very broad environmental ranges, thus limiting their utility in paleoecologic reconstructions.« less

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

PubMed Central

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

2016-01-01

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

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

ACTRIS non-methane hydrocarbon intercomparison experiment in Europe to support WMO-GAW and EMEP observation networks

NASA Astrophysics Data System (ADS)

Hoerger, C. C.; Werner, A.; Plass-Duelmer, C.; Reimann, S.; Eckart, E.; Steinbrecher, R.; Aalto, J.; Arduini, J.; Bonnaire, N.; Cape, J. N.; Colomb, A.; Connolly, R.; Diskova, J.; Dumitrean, P.; Ehlers, C.; Gros, V.; Hakola, H.; Hill, M.; Hopkins, J. R.; Jäger, J.; Junek, R.; Kajos, M. K.; Klemp, D.; Leuchner, M.; Lewis, A. C.; Locoge, N.; Maione, M.; Martin, D.; Michl, K.; Nemitz, E.; O'Doherty, S.; Pérez Ballesta, P.; Ruuskanen, T. M.; Sauvage, S.; Schmidbauer, N.; Spain, T. G.; Straube, E.; Vana, M.; Vollmer, M. K.; Wegener, R.; Wenger, A.

2014-10-01

The performance of 20 European laboratories involved in long-term non-methane hydrocarbon (NMHC) measurements within the framework of Global Atmosphere Watch (GAW) and European Monitoring and Evaluation Programme (EMEP) was assessed with respect to the ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) and GAW data quality objectives (DQOs). Compared to previous intercomparisons the DQOs of ACTRIS are much more demanding with deviations to a reference value of less than 5% and repeatability of better than 2% for mole fractions above 0.1 nmol mol-1. The participants were asked to measure both a 30 component NMHC mixture in nitrogen (NMHC_N2) at approximately 1 nmol mol-1 and whole air (NMHC_air), following a standardised operation procedure including zero- and calibration gas measurements. Furthermore, they had to report details on their instruments and they were asked to assess measurement uncertainties. The NMHCs were analysed either by gas chromatography-flame ionisation detection or gas chromatography-mass spectrometer methods. Most systems performed well for the NMHC_N2 measurements (88% of the reported values were within the GAW DQOs and even 58% within the ACTRIS DQOs). For NMHC_air generally more frequent and larger deviations to the assigned values were observed compared to NMHC_N2 (77% of the reported values were within the GAW DQOs, but only 48% within the ACTRIS DQOs). Important contributors to the poorer performance in NMHC_air compared to NMHC_N2 were a more complex matrix and a larger span of NMHC mole fractions (0.03-2.5 nmol mol-1). Issues, which affected both NMHC mixtures, are the usage of direct vs. two-step calibration, breakthrough of C2-C3 hydrocarbons, blank values in zero-gas measurements (especially for those systems using a Nafion® Dryer), adsorptive losses of aromatic compounds, and insufficient chromatographic resolution. Essential for high-quality results are experienced operators, a comprehensive quality

Poster 12: Nitrile and Hydrocarbon Spatial Abundance Variations in Titan's Atmosphere

NASA Astrophysics Data System (ADS)

Thelen, Alexander E.; Nixon, Conor A.; Molter, Edward; Serigano, Joseph; Cordiner, Martin A.; Charnley, Steven B.; Teanby, Nick; Chanover, Nancy

2016-06-01

Many minor constituents of Titan's atmosphere exhibit latitudinal variations in abundance as a result of atmospheric circulation, photochemical production and subsequent destruction throughout Titan's seasonal cycle [1,2]. Species with observed spatial abundance variations include hydrocarbons - such as CH3CCH - and nitriles - HCN, HC3N, CH3CN, and C2H5CN - as found by Cassini [3,4]. Recent calibration images of Titan taken by the Atacama Large Millimeter/Submillimeter Array (ALMA) allow for measurements of rotational transition lines of these species in spatially resolved regions of Titan's disk [5]. Abundance profiles in Titan's lower/middle atmosphere are retrieved by modeling high resolution ALMA spectra using the Non-linear Optimal Estimator for MultivariatE Spectral analySIS (NEMESIS) radiative transfer code [6]. We present continuous abundance profiles for various species in Titan's atmosphere obtained from ALMA data in 2014. These species show polar abundance enhancements which can be compared to studies using Cassini data [7]. Measurements in the mesosphere will constrain molecular photochemical and dynamical models, while temporal variations inform our knowledge of chemical lifetimes for the large inventory of organic species produced in Titan's atmosphere. The synthesis of the ALMA and Cassini datasets thus allow us to observe the important changes in production and circulation of numerous trace components of Titan's atmosphere, which are attributed to Titan's seasons.

Microbial Community Dynamics in Methane-Oxidizing Mesocosms from the Gulf of Mexico and U.S. Atlantic Margin

NASA Astrophysics Data System (ADS)

Redmond, M. C.; Sorgen, A. A.; Chan, E. W.; Kessler, J. D.

2016-12-01

Microbial methane oxidation at natural gas seeps plays an important role in reducing the amount of this greenhouse gas that reaches the atmosphere, but questions remain about the factors that control methane oxidation rates and organisms responsible. We collected water samples from methane seeps on the U.S. Atlantic Margin (Hudson Canyon) and the Gulf of Mexico and tracked aerobic methane oxidation with high resolution measurements of methane, carbon dioxide, and oxygen concentrations, stable isotopic changes in methane and carbon dioxide, trace metals and nutrients in ten replicate mesocosms from each site. At several time points, we collected DNA for 16S rRNA gene and metagenomic sequencing. Hudson Canyon seep mesocosm communities were dominated by methanotrophs from the family Methylococcaceae (>75% of 16S rRNA gene sequences in all samples). Methylococcaceae were also present in the Gulf of Mexico mesocosms, but were much less abundant (<50% of 16S rRNA gene sequences) and methane was consumed less rapidly than in the Hudson Canyon mesocosms. The Hudson Canyon seeps emit only methane, whereas the Gulf of Mexico seeps also emit ethane, propane, and other hydrocarbons. Consistent with this differing geochemistry, hydrocarbon degraders such as Colwellia and Cycloclasticus were also abundant in the Gulf of Mexico mesocosms, as were genes for the oxidation of longer chain alkanes and aromatic compounds.

Volatile hydrocarbons inhibit methanogenic crude oil degradation

PubMed Central

Sherry, Angela; Grant, Russell J.; Aitken, Carolyn M.; Jones, D. Martin; Head, Ian M.; Gray, Neil D.

2014-01-01

Methanogenic degradation of crude oil in subsurface sediments occurs slowly, but without the need for exogenous electron acceptors, is sustained for long periods and has enormous economic and environmental consequences. Here we show that volatile hydrocarbons are inhibitory to methanogenic oil biodegradation by comparing degradation of an artificially weathered crude oil with volatile hydrocarbons removed, with the same oil that was not weathered. Volatile hydrocarbons (nC5–nC10, methylcyclohexane, benzene, toluene, and xylenes) were quantified in the headspace of microcosms. Aliphatic (n-alkanes nC12–nC34) and aromatic hydrocarbons (4-methylbiphenyl, 3-methylbiphenyl, 2-methylnaphthalene, 1-methylnaphthalene) were quantified in the total hydrocarbon fraction extracted from the microcosms. 16S rRNA genes from key microorganisms known to play an important role in methanogenic alkane degradation (Smithella and Methanomicrobiales) were quantified by quantitative PCR. Methane production from degradation of weathered oil in microcosms was rapid (1.1 ± 0.1 μmol CH4/g sediment/day) with stoichiometric yields consistent with degradation of heavier n-alkanes (nC12–nC34). For non-weathered oil, degradation rates in microcosms were significantly lower (0.4 ± 0.3 μmol CH4/g sediment/day). This indicated that volatile hydrocarbons present in the non-weathered oil inhibit, but do not completely halt, methanogenic alkane biodegradation. These findings are significant with respect to rates of biodegradation of crude oils with abundant volatile hydrocarbons in anoxic, sulphate-depleted subsurface environments, such as contaminated marine sediments which have been entrained below the sulfate-reduction zone, as well as crude oil biodegradation in petroleum reservoirs and contaminated aquifers. PMID:24765087

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

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

PubMed

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

2010-10-01

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

Hydrocarbon sensors and materials therefor

DOEpatents

Pham, Ai Quoc; Glass, Robert S.

2000-01-01

An electrochemical hydrocarbon sensor and materials for use in sensors. A suitable proton conducting electrolyte and catalytic materials have been found for specific application in the detection and measurement of non-methane hydrocarbons. The sensor comprises a proton conducting electrolyte sandwiched between two electrodes. At least one of the electrodes is covered with a hydrocarbon decomposition catalyst. Two different modes of operation for the hydrocarbon sensors can be used: equilibrium versus non-equilibrium measurements and differential catalytic. The sensor has particular application for on-board monitoring of automobile exhaust gases to evaluate the performance of catalytic converters. In addition, the sensor can be utilized in monitoring any process where hydrocarbons are exhausted, for instance, industrial power plants. The sensor is low cost, rugged, sensitive, simple to fabricate, miniature, and does not suffer cross sensitivities.

Determining the Local Abundance of Martian Methane and its 13-C/l2-C and D/H Isotopic Ratios for Comparison with Related Gas and Soil Analysis on the 2011 Mars Science Laboratory (MSL) Mission

NASA Technical Reports Server (NTRS)

Webster, Christopher R.; Mahaffy, Paul R.

2011-01-01

Understanding the origin of Martian methane will require numerous complementary measurements from both in situ and remote sensing investigations and laboratory work to correlate planetary surface geophysics with atmospheric dynamics and chemistry. Three instruments (Quadrupole Mass Spectrometer (QMS), Gas Chromatograph (GC) and Tunable Laser Spectrometer (TLS)) with sophisticated sample handling and processing capability make up the Sample Analysis at Mars (SAM) analytical chemistry suite on NASA s 2011 Mars Science Laboratory (MSL) Mission. Leveraging off the SAM sample and gas processing capability that includes methane enrichment, TLS has unprecedented sensitivity for measuring absolute methane (parts-per-trillion), water, and carbon dioxide abundances in both the Martian atmosphere and evolved from heated soil samples. In concert with a wide variety of associated trace gases (e.g. SO2, H2S, NH3, higher hydrocarbons, organics, etc.) and other isotope ratios measured by SAM, TLS will focus on determining the absolute abundances of methane, water and carbon dioxide, and their isotope ratios: 13C/12C and D/H in methane; 13C/12C and 18O/17O/16O in carbon dioxide; and 18O/17O/16O and D/H in water. Measurements near the MSL landing site will be correlated with satellite (Mars Express, Mars 2016) and ground-based observations.

Non-methane hydrocarbons source apportionment at different sites in Mexico City during 2002-2003

NASA Astrophysics Data System (ADS)

Vega, E.; Sanchez, G.; Molina, L.

2007-09-01

The atmospheric concentrations of a variety of non-methane hydrocarbons (NMHC) collected at different sites, representing urban and rural environments within Mexico City Metropolitan Area (MCMA) during 1997, 2002 and 2003 field campaigns, were compared and used as an input for the Chemical Mass Balance (CMB) receptor model to determine the source contribution of NMHC to the atmosphere. A common feature at all the locations was the dominance of alkenes (59%), aromatics (16%) and olefins (9%) in the average NMHC burden. At the urban sites the interquartile range of NMHC concentrations showed stabilization over this period with a slight increase in the concentrations of propane and butanes in the southwest site of the MCMA in 2003 due to the increased use of liquefied petroleum gas (LPG). The receptor model CMB version 8.0 was used to apportion the NMHC sources at six locations within the MCMA, representing the heavily industrialized, commercial, residential and rural areas. For the 2003 field campaign, the contribution of vehicular emissions dominated the NMHC concentrations (19.7%±7.1% for gasoline vehicles and 35.4%±17.5% for diesel vehicles) followed by the emissions of marketing and handling of LPG (29.9%±8.0%). The NMHC concentrations showed a weekly cycle with the highest levels towards the end of the week and lowest at weekend and beginning of the week, suggesting that both emissions and accumulations process play a key role in building up NMHC levels. The toluene to benzene ratio was used to determine photochemical ageing of the air samples during the 2003 field campaign. The database was divided into periods with similar wind circulation pattern; the results suggest that ageing process within the MCMA is generally suppressed by the amount of fresh emissions.

Compositional and stable carbon isotopic fractionation during non-autocatalytic thermochemical sulfate reduction by gaseous hydrocarbons

USGS Publications Warehouse

Xia, Xinyu; Ellis, Geoffrey S.; Ma, Qisheng; Tang, Yongchun

2014-01-01

The possibility of autocatalysis during thermochemical sulfate reduction (TSR) by gaseous hydrocarbons was investigated by examination of previously reported laboratory and field data. This reaction was found to be a kinetically controlled non-autocatalytic process, and the apparent lack of autocatalysis is thought to be due to the absence of the required intermediate species. Kinetic parameters for chemical and carbon isotopic fractionations of gaseous hydrocarbons affected by TSR were calculated and found to be consistent with experimentally derived values for TSR involving long-chain hydrocarbons. Model predictions based on these kinetic values indicate that TSR by gaseous hydrocarbon requires high-temperature conditions. The oxidation of C2–5 hydrocarbons by sulfate reduction is accompanied by carbon isotopic fractionation with the residual C2–5 hydrocarbons becoming more enriched in 13C. Kinetic parameters were calculated for the stable carbon isotopic fractionation of gaseous hydrocarbons that have experienced TSR. Model predictions based on these kinetics indicate that it may be difficult to distinguish the effects of TSR from those of thermal maturation at lower levels of hydrocarbon oxidation; however, unusually heavy δ13C2+ values (>−10‰) can be diagnostic of high levels of conversion (>50%). Stoichiometric and stable carbon isotopic data show that methane is stable under the investigated reaction conditions and is likely a product of TSR by other gaseous hydrocarbons rather than a significant reactant. These results indicate that the overall TSR reaction mechanism for oxidation of organic substrates containing long-chain hydrocarbons involves three distinct phases as follows: (1) an initial slow and non-autocatalytic stage characterized by the reduction of reactive sulfate by long-chain saturated hydrocarbons; (2) a second autocatalytic reaction phase dominated by reactions involving reduced sulfur species and partially oxidized hydrocarbons; (3

Multi-year levels and trends of non-methane hydrocarbon concentrations observed in ambient air in France

NASA Astrophysics Data System (ADS)

Waked, Antoine; Sauvage, Stéphane; Borbon, Agnès; Gauduin, Julie; Pallares, Cyril; Vagnot, Marie-Pierre; Léonardis, Thierry; Locoge, Nadine

2016-09-01

Measurements of 31 non-methane hydrocarbons (NMHCs) were carried out at three urban (Paris, 2003-2014, Strasbourg, 2002-2014 and Lyon, 2007-2014) sites in France over the period of a decade. A trend analysis was applied by means of the Mann-Kendall non-parametric test to annual and seasonal mean concentrations in order to point out changes in specific emission sources and to assess the impact of emission controls and reduction strategies. The trends were compared to those from three rural sites (Peyrusse-Vieille, 2002-2013, Tardière, 2003-2013 and Donon, 1997-2007). The results obtained showed a significant yearly decrease in pollutant concentrations over the study period and for the majority of species in the range of -1 to -7% in accordance with the decrease of NMHC emissions in France (-5 to -9%). Concentrations of long-lived species such as ethane and propane which are recognized as tracers of distant sources and natural gas remained constant. Compounds associated with combustion processes such as acetylene, propene, ethylene and benzene showed a significant decline in the range of -2% to -5% yr-1. These trends are consistent with those recently described at urban and background sites in the northern mid-latitudes and with emission inventories. C7-C9 aromatics such as toluene and xylenes as well as C4-C5 alkanes such as isopentane and isobutane also showed a significant decrease in the range of -3% to -7% yr-1. The decreasing trends in terms of % yr-1 observed at these French urban sites were typically higher for acetylene, ethylene and benzene than those reported for French rural sites of the national observatory of Measurement and Evaluation in Rural areas of trans-boundary Air pollution (MERA). The study also highlighted the difficult choice of a long term sampling site representative of the general trends of pollutant concentrations.

Variation of ambient non-methane hydrocarbons in Beijing city in summer 2008

NASA Astrophysics Data System (ADS)

Wang, B.; Shao, M.; Lu, S. H.; Yuan, B.; Zhao, Y.; Wang, M.; Zhang, S. Q.; Wu, D.

2010-02-01

In conjunction with hosting the 2008 Beijing Olympics, the municipal government implemented a series of stringent air quality control measures. To assess the impacts on variation of ambient non-methane hydrocarbons (NMHCs), the whole air was sampled by canisters at one urban site and two suburban sites in Beijing, and 55 NMHC species were quantified by gas chromatography equipped with a quadrupole mass spectrometer and a flame ionization detector (GC/MSD/FID) as parts of the field Campaign for the Beijing Olympic Games Air Quality program (CareBeijing). According to the control measures, the data were presented according to four periods: 18-30 June, 8-19 July, 15-24 August (during the Olympic Games), and 6-15 September (during the Paralympic Games). Compared with the levels in June, the mixing ratios of NMHCs obtained in the Olympic and Paralympic Games periods were reduced by 35% and 25%, respectively. Source contributions were calculated using a chemical mass balance model (CMB 8.2). After implementing the control measures, emissions from target sources were obviously reduced, and reductions in vehicle exhaust could explain 48-82% of the reductions of ambient NMHCs. Reductions in emissions from gasoline evaporation, paint and solvent use, and the chemical industry contributed 9-40%, 3-24%, and 1-5%, respectively, to reductions of ambient NMHCs. Sources of liquefied petroleum gas (LPG) and biogenic emissions were not controlled, and contributions from these sources from July to September were stable or even higher than in June. Ozone formation potentials (OFPs) were calculated for the measured NMHCs. The total OFPs during the Olympic and Paralympic Games were reduced by 48% and 32%, respectively, compared with values in June. Reductions in the OFPs of alkenes and aromatics explained 77-92% of total OFP reductions. The alkenes and aromatics were mainly from vehicle exhausts, and reductions of vehicle exhaust gases explained 67-87% of reductions in alkenes and 38

Variation of ambient non-methane hydrocarbons in Beijing city in summer 2008

NASA Astrophysics Data System (ADS)

Wang, B.; Shao, M.; Lu, S. H.; Yuan, B.; Zhao, Y.; Wang, M.; Zhang, S. Q.; Wu, D.

2010-07-01

In conjunction with hosting the 2008 Beijing Olympics, the municipal government implemented a series of stringent air quality control measures. To assess the impacts on variation of ambient non-methane hydrocarbons (NMHCs), the whole air was sampled by canisters at one urban site and two suburban sites in Beijing, and 55 NMHC species were quantified by gas chromatography equipped with a quadrupole mass spectrometer and a flame ionization detector (GC/MSD/FID) as parts of the field Campaign for the Beijing Olympic Games Air Quality program (CareBeijing). According to the control measures, the data were presented according to four periods: 18-30 June, 8-19 July, 15-24 August (during the Olympic Games), and 6-15 September (during the Paralympic Games). Compared with the levels in June, the mixing ratios of NMHCs obtained in the Olympic and Paralympic Games periods were reduced by 35% and 25%, respectively. Source contributions were calculated using a chemical mass balance model (CMB 8.2). After implementing the control measures, emissions from target sources were obviously reduced, and reductions in vehicle exhaust could explain 48-82% of the reductions of ambient NMHCs. Reductions in emissions from gasoline evaporation, paint and solvent use, and the chemical industry contributed 9-40%, 3-24%, and 1-5%, respectively, to reductions of ambient NMHCs. Sources of liquefied petroleum gas (LPG) and biogenic emissions were not controlled, and contributions from these sources from July to September were stable or even higher than in June. Ozone formation potentials (OFPs) were calculated for the measured NMHCs. The total OFPs during the Olympic and Paralympic Games were reduced by 48% and 32%, respectively, compared with values in June. Reductions in the OFPs of alkenes and aromatics explained 77-92% of total OFP reductions. The alkenes and aromatics were mainly from vehicle exhausts, and reductions of vehicle exhaust gases explained 67-87% of reductions in alkenes and 38

Methane photochemistry and methane production on Neptune

NASA Technical Reports Server (NTRS)

Romani, P. N.; Atreya, S. K.

1988-01-01

The Neptune stratosphere's methane photochemistry is presently studied by means of a numerical model in which the observed mixing ratio of methane prompts photolysis near the CH4 homopause. Haze generation by methane photochemistry has its basis in the formation of hydrocarbon ices and polyacetylenes; the hazes can furnish the requisite aerosol haze at the appropriate pressure levels required by observations of Neptune in the visible and near-IR. Comparisons of model predictions with Uranus data indicate a lower ratio of polyacetylene production to hydrocarbon ice, as well as a lower likelihood of UV postprocessing of the acetylene ice to polymers on Neptune, compared to Uranus.

Contribution of deep sourced carbon from hydrocarbon seeps to sedimentary organic carbon: Evidence from Δ14C and δ13C isotopes

NASA Astrophysics Data System (ADS)

Feng, D.; Peckmann, J.; Peng, Y.; Liang, Q.; Roberts, H. H.; Chen, D.

2017-12-01

Sulfate-driven anaerobic oxidation of methane (AOM) limits the release of methane from marine sediments and promotes the formation of carbonates close to the seafloor along continental margins. It has been established that hydrocarbon seeps are a source of dissolved inorganic and organic carbon to marine environments. However, questions remain about the contribution of deep sourced carbon from hydrocarbon seeps to the sedimentary organic carbon pool. For a number of hydrocarbon seeps from the South China Sea and the Gulf of Mexico, the portion of modern carbon was determined based on natural radiocarbon abundances (Δ14C) and stable carbon isotope (δ13Corganic carbon) compositions of the non-carbonate fractions extracted from authigenic carbonates. Samples from both areas show a mixing trend between ideal planktonic organic carbon (δ13C = -22‰ VPDB and 90% modern carbon) and the ambient methane. The δ13Corganic carbon values of non-carbonate fractions from three ancient seep deposits (northern Italy, Miocene; western Washington State, USA, Eocene to Oligocene) confirm that the proxy can be used to constrain the record of sulfate-driven AOM through most of Earth history by measuring the δ13C values of organic carbon. This study reveals the potential of using δ13C values of organic carbon to discern seep and non-seep environments. This new approach is particularly promising when authigenic carbonate is not present in ancient sedimentary environments. Acknowledgments: The authors thank BOEM and NOAA for their years' support of the deep-sea dives. Funding was provided by the NSF of China (Grants: 41422602 and 41373085).

Analysis of Non-Methane Hydrocarbon Data from 2004-2016 in a Subtropical Area close to the Gulf of Mexico

NASA Astrophysics Data System (ADS)

Rappenglueck, B.

2017-12-01

Speciated C2-C11 non-methane hydrocarbons (NMHC) have been measured online on an hourly basis at Lake Jackson/TX close to the Gulf of Mexico. Altogether 48 NMHCs along with NO, NO2, NOx, O3 have been collected continuously from January 2004-December 2016 under the auspices of the Texas Commission on Environmental Quality. Data was screened for background conditions representing marine wind sectors. The data set represents a combination of marine air masses mixed with local biogenic emissions. The data analysis addresses photochemical processing of air masses as reflected in the relationship of ln(n-butane/ethane) vs. ln(propane/ethane) and ln(i-butane/ethane) vs. ln(n-butane/ethane). In addition, key NMHC relationships for radical chemistry, e.g. i-butane vs n-butane for OH and Cl chemistry and i-pentane vs. n-pentane for NO3 chemistry, are discussed. Seasonal analysis revealed a clear trend with maximum NMHC mixing ratios in winter time and lowest mixing ratios in summer reflecting the impact of photochemical processes in summer. Propene equivalents were highest during summertime, with significant contributions from alkenes, including isoprene. The relation of propane/ethane vs ethane indicates seasonal variation with lowest values (i.e. most aged air masses) in winter.

Summary of measurement results of ozone, methane, and nonmethane hydrocarbons for C-54 aircraft. 1979 Southeastern Virginia Urban Plume Study

NASA Technical Reports Server (NTRS)

Cofer, W. R., III; Purgold, G. C.; Gregory, G. L.

1981-01-01

Methane, nonmethane hydrocarbon, and ozone data collected in a C-54 aircraft during the 1979 Southeastern Virginia Urban Plume Study are presented. Three major aircraft experiments were flown on five separate days in August collecting 20 hours of flight data. Direct correlation between ozone and hydrocarbon plumes was observed on several occasions.

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

PubMed Central

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

2010-01-01

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

Novel hydrocarbon monooxygenase genes in the metatranscriptome of a natural deep-sea hydrocarbon plume.

PubMed

Li, Meng; Jain, Sunit; Baker, Brett J; Taylor, Chris; Dick, Gregory J

2014-01-01

Particulate membrane-associated hydrocarbon monooxygenases (pHMOs) are critical components of the aerobic degradation pathway for low molecular weight hydrocarbons, including the potent greenhouse gas methane. Here, we analysed pHMO gene diversity in metagenomes and metatranscriptomes of hydrocarbon-rich hydrothermal plumes in the Guaymas Basin (GB) and nearby background waters in the deep Gulf of California. Seven distinct phylogenetic groups of pHMO were present and transcriptionally active in both plume and background waters, including several that are undetectable with currently available polymerase chain reaction (PCR) primers. The seven groups of pHMOs included those related to a putative ethane oxidizing Methylococcaceae-like group, a group of the SAR324 Deltaproteobacteria, three deep-sea clades (Deep sea-1/symbiont-like, Deep sea-2/PS-80 and Deep sea-3/OPU3) within gammaproteobacterial methanotrophs, one clade related to Group Z and one unknown group. Differential abundance of pHMO gene transcripts in plume and background suggests niche differentiation between groups. Corresponding 16S rRNA genes reflected similar phylogenetic and transcriptomic abundance trends. The novelty of transcriptionally active pHMOs we recovered from a hydrocarbon-rich hydrothermal plume suggests there are significant gaps in our knowledge of the diversity and function of these enzymes in the environment. © 2013 Society for Applied Microbiology and John Wiley & Sons Ltd.

Limitations of microbial hydrocarbon degradation at the Amon mud volcano (Nile deep-sea fan)

NASA Astrophysics Data System (ADS)

Felden, J.; Lichtschlag, A.; Wenzhöfer, F.; de Beer, D.; Feseker, T.; Pop Ristova, P.; de Lange, G.; Boetius, A.

2013-05-01

The Amon mud volcano (MV), located at 1250 m water depth on the Nile deep-sea fan, is known for its active emission of methane and non-methane hydrocarbons into the hydrosphere. Previous investigations showed a low efficiency of hydrocarbon-degrading anaerobic microbial communities inhabiting the Amon MV center in the presence of sulfate and hydrocarbons in the seeping subsurface fluids. By comparing spatial and temporal patterns of in situ biogeochemical fluxes, temperature gradients, pore water composition, and microbial activities over 3 yr, we investigated why the activity of anaerobic hydrocarbon degraders can be low despite high energy supplies. We found that the central dome of the Amon MV, as well as a lateral mud flow at its base, showed signs of recent exposure of hot subsurface muds lacking active hydrocarbon degrading communities. In these highly disturbed areas, anaerobic degradation of methane was less than 2% of the methane flux. Rather high oxygen consumption rates compared to low sulfide production suggest a faster development of more rapidly growing aerobic hydrocarbon degraders in highly disturbed areas. In contrast, the more stabilized muds surrounding the central gas and fluid conduits hosted active anaerobic hydrocarbon-degrading microbial communities. The low microbial activity in the hydrocarbon-vented areas of Amon MV is thus a consequence of kinetic limitations by heat and mud expulsion, whereas most of the outer MV area is limited by hydrocarbon transport.

Non-methane hydrocarbon characteristics of motor vehicular emissions in the Pearl River Delta region

NASA Astrophysics Data System (ADS)

Tsai, Wai Yan

2007-12-01

Air pollution problem in Hong Kong and the Pearl River Delta (PRD) region has raised much concern from the public in recent years. The primary aim of this research is to use field measurement data to characterize non-methane hydrocarbons (NMHCs) in emission from motor vehicles. Fuel vapor compositions for several commonly used vehicular fuels in Hong Kong, Macau, Guangzhou and Zhuhai were analyzed in 2003, and they are believed to be the first one reported for the PRD region. These profiles were used to study the impact of evaporative loss of the fuels on air quality. From the roadside and tunnel samples collected in the four cities mentioned above from 2000 to 2003, results showed that vehicular engine combustion was a main NMHC source, while gasoline evaporative losses also contributed much to the total NMHC emission, besides, LPG leakage was also found to be significant from the tunnel measurement data collected in Hong Kong. Characteristics of vehicular engine exhaust emissions were also studied. Measurements of diesel emission showed a large influence on the emission profile due to the change of diesel compositions. The E/E ratios implied that gasoline-powered vehicles in Hong Kong were equipped with well functioning catalysts, while those in Guangzhou and Zhuhai, especially the motorcycles, were found dirtier in NMHC emission. Although the E/E ratios showed that private cars in Hong Kong had high combustion efficiency, the existence of significant amounts of unburned gasoline in their exhaust stream pointed out that they still had low fuel economy. From the results of a simple model, it was found that the evaporative losses of gasoline and LPG contributed much to the total NMHC pollution from vehicle. The preliminary results from the dynamometer study conducted in Hong Kong showed large variations of exhaust characteristics for private cars and taxis during different driving speeds. The results can be used as scientific basis for regulatory parties in

Microbial communities along biogeochemical gradients in a hydrocarbon-contaminated aquifer.

PubMed

Tischer, Karolin; Kleinsteuber, Sabine; Schleinitz, Kathleen M; Fetzer, Ingo; Spott, Oliver; Stange, Florian; Lohse, Ute; Franz, Janett; Neumann, Franziska; Gerling, Sarah; Schmidt, Christian; Hasselwander, Eyk; Harms, Hauke; Wendeberg, Annelie

2013-09-01

Micro-organisms are known to degrade a wide range of toxic substances. How the environment shapes microbial communities in polluted ecosystems and thus influences degradation capabilities is not yet fully understood. In this study, we investigated microbial communities in a highly complex environment: the capillary fringe and subjacent sediments in a hydrocarbon-contaminated aquifer. Sixty sediment sections were analysed using terminal restriction fragment length polymorphism (T-RFLP) fingerprinting, cloning and sequencing of bacterial and archaeal 16S rRNA genes, complemented by chemical analyses of petroleum hydrocarbons, methane, oxygen and alternative terminal electron acceptors. Multivariate statistics revealed concentrations of contaminants and the position of the water table as significant factors shaping the microbial community composition. Micro-organisms with highest T-RFLP abundances were related to sulphate reducers belonging to the genus Desulfosporosinus, fermenting bacteria of the genera Sedimentibacter and Smithella, and aerobic hydrocarbon degraders of the genus Acidovorax. Furthermore, the acetoclastic methanogens Methanosaeta, and hydrogenotrophic methanogens Methanocella and Methanoregula were detected. Whereas sulphate and sulphate reducers prevail at the contamination source, the detection of methane, fermenting bacteria and methanogenic archaea further downstream points towards syntrophic hydrocarbon degradation. © 2013 John Wiley & Sons Ltd and Society for Applied Microbiology.

The levels, variation characteristics, and sources of atmospheric non-methane hydrocarbon compounds during wintertime in Beijing, China

NASA Astrophysics Data System (ADS)

Liu, Chengtang; Ma, Zhuobiao; Mu, Yujing; Liu, Junfeng; Zhang, Chenglong; Zhang, Yuanyuan; Liu, Pengfei; Zhang, Hongxing

2017-09-01

Atmospheric non-methane hydrocarbon compounds (NMHCs) were measured at a sampling site in Beijing city from 15 December 2015 to 14 January 2016 to recognize their pollution levels, variation characteristics, and sources. We quantified 53 NMHCs, and the proportions of alkanes, alkenes, acetylene, and aromatics to the total NMHCs were 49.8-55.8, 21.5-24.7, 13.5-15.9, and 9.3-10.7 %, respectively. The variation trends in the NMHC concentrations were basically identical and exhibited remarkable fluctuation, which was mainly ascribed to the variation in meteorological conditions, especially wind speed. The diurnal variations in NMHCs on clear days exhibited two peaks during the morning and evening rush hours, whereas the rush hours' peaks diminished or even disappeared on the haze days, implying that the relative contribution of the vehicular emissions to atmospheric NMHCs depended on the pollution status. Two evident peaks of the propane / propene ratios appeared in the early morning before sun rise and at noontime on clear days, whereas only one peak occurred in the afternoon during the haze days, which were attributed to the relatively fast reactions of propene with OH, NO3, and O3. Based on the chemical kinetic equations, the daytime OH concentrations were calculated to be in the range of 3. 47 × 105-1. 04 × 106 molecules cm-3 on clear days and 6. 42 × 105-2. 35 × 106 molecules cm-3 on haze days. The nighttime NO3 concentrations were calculated to be in the range of 2. 82 × 109-4. 86 × 109 molecules cm-3 on clear days. The correlation coefficients of typical hydrocarbon pairs (benzene / toluene, o-xylene / m,p-xylene, isopentane / n-pentane, etc.) revealed that vehicular emissions and coal combustion were important sources for atmospheric NMHCs in Beijing during the wintertime. Five major emission sources for atmospheric NMHCs in Beijing during the wintertime were further identified by positive matrix factorization (PMF), including gasoline-related emissions

TOWARD THE FORMATION OF CARBONACEOUS REFRACTORY MATTER IN HIGH TEMPERATURE HYDROCARBON-RICH ATMOSPHERES OF EXOPLANETS UPON MICROMETEOROID IMPACT

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

Dangi, Beni B.; Kim, Yong S.; Krasnokutski, Serge A.

2015-05-20

We report on laboratory simulation experiments mimicking the chemical processing of model atmospheres of exoplanets containing C3 and C4 hydrocarbons at moderate temperatures of 400 K upon interaction of catalytic surfaces of micrometeoroids. By utilizing an ultrasonic levitator device and heating singly levitated particles under simulated microgravity conditions, Raman spectroscopy is utilized as a non-invasive tool to probe on line and in situ the conversion of C3 and C4 hydrocarbons to refractory carbonaceous matter on the surfaces of levitated particles. Secondary Ion Mass Spectrometry and electron microscopic imaging were also conducted to gain further insight into the elementary composition andmore » structures of the refractories formed. Our results provide compelling evidence that in the presence of a catalytic surface, which can be supplied in the form of micrometeoroids and atmospheric dust particles, hydrocarbon gases present in the atmospheres of exoplanets can be converted to refractory, carbon-rich carbonaceous matter of mainly graphitic structure with a carbon content of at least 90% at elevated temperatures. This finding might explain the low methane to carbon monoxide (CH{sub 4}–CO) ratio in the hot Neptune GJ 436b, where the abundant methane photochemically converts to higher order hydrocarbons and ultimately to refractory graphite-like carbon in the presence of a silicon surface.« less

Abundance and δ13C values of fatty acids in lacustrine surface sediments: Relationships with in-lake methane concentrations

NASA Astrophysics Data System (ADS)

Stötter, Tabea; Bastviken, David; Bodelier, Paul L. E.; van Hardenbroek, Maarten; Rinta, Päivi; Schilder, Jos; Schubert, Carsten J.; Heiri, Oliver

2018-07-01

Proxy-indicators in lake sediments provide the only approach by which the dynamics of in-lake methane cycling can be examined on multi-decadal to centennial time scales. This information is necessary to constrain how lacustrine methane production, oxidation and emissions are expected to respond to global change drivers. Several of the available proxies for reconstructing methane cycle changes of lakes rely on interpreting past changes in the abundance or relevance of methane oxidizing bacteria (MOB), either directly (e.g. via analysis of bacterial lipids) or indirectly (e.g. via reconstructions of the past relevance of MOB in invertebrate diet). However, only limited information is available about the extent to which, at the ecosystem scale, variations in abundance and availability of MOB reflect past changes in in-lake methane concentrations. We present a study examining the abundances of fatty acids (FAs), particularly of 13C-depleted FAs known to be produced by MOB, relative to methane concentrations in 29 small European lakes. 39 surface sediment samples were obtained from these lakes and FA abundances were compared with methane concentrations measured at the lake surface, 10 cm above the sediments and 10 cm within the sediments. Three of the FAs in the surface sediment samples, C16:1ω7c, C16:1ω5c/t, and C18:1ω7c were characterized by lower δ13C values than the remaining FAs. We show that abundances of these FAs, relative to other short-chain FAs produced in lake ecosystems, are related with sedimentary MOB concentrations assessed by quantitative polymerase chain reaction (qPCR). We observed positive relationships between methane concentrations and relative abundances of C16:1ω7c, C16:1ω5c/t, and C18:1ω7c and the sum of these FAs. For the full dataset these relationships were relatively weak (Spearman's rank correlation (rs) of 0.34-0.43) and not significant if corrected for multiple testing. However, noticeably stronger and statistically significant

Methane seeps along boundaries of arctic permafrost thaw and melting glaciers

NASA Astrophysics Data System (ADS)

Anthony, P.; Walter Anthony, K. M.; Grosse, G.; Chanton, J.

2014-12-01

Methane, a potent greenhouse gas, accumulates in subsurface hydrocarbon reservoirs. In the Arctic, impermeable icy permafrost and glacial overburden form a 'cryosphere cap' that traps gas leaking from these reservoirs, restricting flow to the atmosphere. We document the release of geologic methane to the atmosphere from abundant gas seeps concentrated along boundaries of permafrost thaw and receding glaciers in Alaska. Through aerial and ground surveys we mapped >150,000 seeps identified as bubbling-induced open holes in lake ice. Subcap methane seeps had anomalously high fluxes, 14C-depletion, and stable isotope values matching known coalbed and thermogenic methane accumulations in Alaska. Additionally, we observed younger subcap methane seeps in Greenland that were associated with ice-sheet retreat since the Little Ice Age. These correlations suggest that in a warming climate, continued disintegration of permafrost, glaciers, and parts of the polar ice sheets will relax pressure on subsurface seals and further open conduits, allowing a transient expulsion of geologic methane currently trapped by the cryosphere cap.

Physical Chemical Controls of Methane and other Hydrocarbon gases in Outer Solar System Water-Ice Systems

NASA Astrophysics Data System (ADS)

Osegovic, J. P.; Max, M. D.

2012-12-01

Saturn's moon Enceladus appear to have liquid water under its thin icy surface that has venting water and complex hydrocarbons. Jupiter's moon Europa is locked under a very thick layer of surface ice. Because Saturn's moon Titan contains abundant hydrocarbon gasses and liquids and both Saturn and Jupiter contain abundant hydrocarbon gases, it is likely that Europa also may have significant quantities of hydrocarbon gases in their water-ice systems. Both of these moons have the potential for life. We have begun to explore the impact that gas hydrate, which is a crystalline material composed of water and gas molecules, has on the availability of liquid water on a planet's surface: what conditions need to be present to initiate hydrate formation from a primordial selection of gases, salts, and water, how isolated hydrate systems evolve under the condition of mass transfer from ex-hydrate stability conditions to pro-hydrate stability conditions, the timespan of conditions that hydrate formation can host liquid solutions in an otherwise cooling regime; and the impact that additional chemistry, such as primitive chemosynthesis, may have on the sequestered hydrocarbon gases in hydrate. The analog for gas hydrate on these moons is the Permafrost hydrate system of Earth. Gas hydrate and water ice are stable in a compound cryosphere with ice extending downward from cold surface conditions to about the 273 K isotherm. Hydrate, depending on the mixture of gases in it, is stable from some depth below the surface to some isotherm that could be considerably in excess of 273 K. Salinity may strongly affect stability conditions. In order to estimate the thickness of the gas hydrate stability zone and its effect on 'planetary' heat flow, we model heat production as a function of mass flow. Variables are gravity, ice thickness, temperature of the surrounding medium (space, ice, and water), the thickness of the "ocean", the and the thermophysical properties of the gas being

Abundance Profiles for C3 Hydrocarbons in Titan's Atmosphere

NASA Astrophysics Data System (ADS)

Lombardo, Nicholas; Nixon, Conor A.; Achterberg, Richard; Jolly, Antoine; Sung, Keeyoon; Irwin, Patrick; Flasar, F. Michael

2017-10-01

The atmosphere of Titan is of astrobiological importance. Its highly reducing composition and prebiotic chemistry make it analogous to that of the early Earth. Since the Voyager era, several complex hydrocarbons and nitriles have been detected, in some cases making Titan the only known planetary body where these gasses occur naturally. In this work, we report abundance profiles of four major C3 gasses expected to occur in Titan’s atmosphere, derived from Cassini/Composite Infrared Spectrometer (CIRS) data.Using the NEMESIS iterative radiative transfer module, we retrieved vertical abundance profiles for propane (C3H8) and propyne (CHCCH3), both initially detected by the Voyager IRIS instrument. Using newly available line data, we were also able to determine the first vertical abundance profiles for propene (C3H6), initially detected in 2013. We present profiles for several latitudes and times and compare to photochemical model predictions and previous observations. We also discuss our efforts to further the search for allene (CH2CCH2), an isomer of propyne. The abundances we retrieved will help to further our understanding of the chemical pathways that occur in Titan's atmosphere.

Non-Detection of Methane in the Mars Atmosphere by the Curiosity Rover

NASA Technical Reports Server (NTRS)

Webster, Chris R.; Mahaffy, Paul R.; Atreya, Sushil K.; Flesch, Gregory J.; Farley, Kenneth A.

2014-01-01

By analogy with Earth, methane in the atmosphere of Mars is a potential signature of ongoing or past biological activity on the planet. During the last decade, Earth-based telescopic and Mars orbit remote sensing instruments have reported significant abundances of methane in the Martian atmosphere ranging from several to tens of parts-per-billion by volume (ppbv). Observations from Earth showed plumes of methane with variations on timescales much faster than expected and inconsistent with localized patches seen from orbit, prompting speculation of sources from sub-surface methanogen bacteria, geological water-rock reactions or infall from comets, micro-meteorites or interplanetary dust. From measurements on NASAs Curiosity Rover that landed near Gale Crater on 5th August 2012, we here report no definitive detection of methane in the near-surface Martian atmosphere. Our in situ measurements were made using the Tunable Laser Spectrometer (TLS) in the Sample Analysis at Mars (SAM) instrument suite6 that made three separate searches on Martian sols 79, 81 and 106 after landing. The measured mean value of 0.39 plus or minus 1.4 ppbv corresponds to an upper limit for methane abundance of 2.7 ppbv at the 95 confidence level. This result is in disagreement with both the remote sensing spacecraft observations taken at lower sensitivity and the telescopic observations that relied on subtraction of a very large contribution from terrestrial methane in the intervening observation path. Since the expected lifetime of methane in the Martian atmosphere is hundreds of years, our results question earlier observations and set a low upper limit on the present day abundance, reducing the probability of significant current methanogenic microbial activity on Mars.

Archaeal abundance in post-mortem ruminal digesta may help predict methane emissions from beef cattle

NASA Astrophysics Data System (ADS)

Wallace, R. John; Rooke, John A.; Duthie, Carol-Anne; Hyslop, Jimmy J.; Ross, David W.; McKain, Nest; de Souza, Shirley Motta; Snelling, Timothy J.; Waterhouse, Anthony; Roehe, Rainer

2014-07-01

Methane produced from 35 Aberdeen-Angus and 33 Limousin cross steers was measured in respiration chambers. Each group was split to receive either a medium- or high-concentrate diet. Ruminal digesta samples were subsequently removed to investigate correlations between methane emissions and the rumen microbial community, as measured by qPCR of 16S or 18S rRNA genes. Diet had the greatest influence on methane emissions. The high-concentrate diet resulted in lower methane emissions (P < 0.001) than the medium-concentrate diet. Methane was correlated, irrespective of breed, with the abundance of archaea (R = 0.39), bacteria (-0.47), protozoa (0.45), Bacteroidetes (-0.37) and Clostridium Cluster XIVa (-0.35). The archaea:bacteria ratio provided a stronger correlation (0.49). A similar correlation was found with digesta samples taken 2-3 weeks later at slaughter. This finding could help enable greenhouse gas emissions of large animal cohorts to be predicted from samples taken conveniently in the abattoir.

Summary of 1978 Southeastern Virginia Urban Plume study: Aircraft results for carbon monoxide, methane, nonmethane hydrocarbons, and ozone

NASA Technical Reports Server (NTRS)

Hill, G. F.; Sachse, G. W.; Cofer, W. R., III

1981-01-01

The characteristics of the Southeastern Virginia urban plume were defined with emphasis on the photon-oxidant species. The measurement area was a rectangle, approximately 150 km by 100 km centered around Cape Charles, Virginia. Included in this area are the cities of Norfolk, Virginia Beach, Chesapeake, Newport News, and Hampton. The area is bounded on the north by Wallops Island, Virginia, and on the south by the Hampton Roads area of Tidewater Virginia. The major axis of the rectangle is oriented in the southwest-northeast direction. The data set includes aircraft measurements for carbon monoxide, methane, nonmethane hydrocarbons, and ozone. The experiment shows that CO can be successfully measured as a tracer gas and used as an index for determining localized and urban plumes. The 1978 data base provided sufficient data to assess an automated chromatograph with flame ionization detection used for measuring methane and nonmethane hydrocarbons in flight.

Facultative methanotrophs are abundant at terrestrial natural gas seeps.

PubMed

Farhan Ul Haque, Muhammad; Crombie, Andrew T; Ensminger, Scott A; Baciu, Calin; Murrell, J Colin

2018-06-28

Natural gas contains methane and the gaseous alkanes ethane, propane and butane, which collectively influence atmospheric chemistry and cause global warming. Methane-oxidising bacteria, methanotrophs, are crucial in mitigating emissions of methane as they oxidise most of the methane produced in soils and the subsurface before it reaches the atmosphere. Methanotrophs are usually obligate, i.e. grow only on methane and not on longer chain alkanes. Bacteria that grow on the other gaseous alkanes in natural gas such as propane have also been characterised, but they do not grow on methane. Recently, it was shown that the facultative methanotroph Methylocella silvestris grew on ethane and propane, other components of natural gas, in addition to methane. Therefore, we hypothesised that Methylocella may be prevalent at natural gas seeps and might play a major role in consuming all components of this potent greenhouse gas mixture before it is released to the atmosphere. Environments known to be exposed to biogenic methane emissions or thermogenic natural gas seeps were surveyed for methanotrophs. 16S rRNA gene amplicon sequencing revealed that Methylocella were the most abundant methanotrophs in natural gas seep environments. New Methylocella-specific molecular tools targeting mmoX (encoding the soluble methane monooxygenase) by PCR and Illumina amplicon sequencing were designed and used to investigate various sites. Functional gene-based assays confirmed that Methylocella were present in all of the natural gas seep sites tested here. This might be due to its ability to use methane and other short chain alkane components of natural gas. We also observed the abundance of Methylocella in other environments exposed to biogenic methane, suggesting that Methylocella has been overlooked in the past as previous ecological studies of methanotrophs often used pmoA (encoding the alpha subunit of particulate methane monooxygenase) as a marker gene. New biomolecular tools designed in

Non-methane hydrocarbons in the atmosphere of Mexico City: Results of the 2012 ozone-season campaign

NASA Astrophysics Data System (ADS)

Jaimes-Palomera, Mónica; Retama, Armando; Elias-Castro, Gabriel; Neria-Hernández, Angélica; Rivera-Hernández, Olivia; Velasco, Erik

2016-05-01

With the aim to strengthen the verification capabilities of the local air quality management, the air quality monitoring network of Mexico City has started the monitoring of selected non-methane hydrocarbons (NMHCs). Previous information on the NMHC characterization had been obtained through individual studies and comprehensive intensive field campaigns, in both cases restricted to sampling periods of short duration. This new initiative will address the NMHC pollution problem during longer monitoring periods and provide robust information to evaluate the effectiveness of new control measures. The article introduces the design of the monitoring network and presents results from the first campaign carried out during the first six months of 2012 covering the ozone-season (Mar-May). Using as reference data collected in 2003, results show reductions during the morning rush hour (6-9 h) in the mixing ratios of light alkanes associated with the consumption and distribution of liquefied petroleum gas and aromatic compounds related with the evaporation of fossil fuels and solvents, in contrast to olefins from vehicular traffic. The increase in mixing ratios of reactive olefins is of relevance to understand the moderate success in the ozone and fine aerosols abatement in recent years in comparison to other criteria pollutants. In the case of isoprene, the typical afternoon peak triggered by biogenic emissions was clearly observed for the first time within the city. The diurnal profiles of the monitored compounds are analyzed in terms of the energy balance throughout the day as a surrogate of the boundary layer evolution. Particular features of the diurnal profiles and correlation between individual NMHCs and carbon monoxide are used to investigate the influence of specific emission sources. The results discussed here highlight the importance of monitoring NMHCs to better understand the drivers and impacts of air pollution in large cities like Mexico City.

Limitations of microbial hydrocarbon degradation at the Amon Mud Volcano (Nile Deep Sea Fan)

NASA Astrophysics Data System (ADS)

Felden, J.; Lichtschlag, A.; Wenzhöfer, F.; de Beer, D.; Feseker, T.; Pop Ristova, P.; de Lange, G.; Boetius, A.

2013-01-01

The Amon mud volcano (MV), located at 1250 m water depth on the Nile Deep Sea Fan, is known for its active emission of methane and non-methane hydrocarbons into the hydrosphere. Previous investigations showed a low efficiency of hydrocarbon-degrading anaerobic microbial communities inhabiting the Amon MV center in the presence of sulphate and hydrocarbons in the seeping subsurface fluids. By comparing spatial and temporal patterns of in situ biogeochemical fluxes, temperature gradients, pore water composition and microbial activities over three years, we investigated why the activity of anaerobic hydrocarbon degraders can be low despite high energy supplies. We found that the central dome of the Amon MV, as well as a lateral mud flow at its base, showed signs of recent exposure of hot subsurface muds lacking active hydrocarbon degrading communities. In these highly disturbed areas, anaerobic degradation of methane was less than 2% of the methane flux. Rather high oxygen consumption rates compared to low sulphide production suggest a faster development of more rapidly growing aerobic hydrocarbon degraders in highly disturbed areas. In contrast, the more stabilized muds surrounding the central gas and fluid conduits hosted active anaerobic hydrocarbon-degrading microbial communities. Furthermore, within three years, cell numbers and hydrocarbon degrading activity increased at the gas-seeping sites. The low microbial activity in the hydrocarbon-vented areas of Amon mud volcano is thus a consequence of kinetic limitations by heat and mud expulsion, whereas most of the outer mud volcano area is limited by hydrocarbon transport.

Three-dimensional numerical simulations of methane gas migration from decommissioned hydrocarbon production wells into shallow aquifers

NASA Astrophysics Data System (ADS)

Roy, N.; Molson, J.; Lemieux, J.-M.; Van Stempvoort, D.; Nowamooz, A.

2016-07-01

Three-dimensional numerical simulations are used to provide insight into the behavior of methane as it migrates from a leaky decommissioned hydrocarbon well into a shallow aquifer. The conceptual model includes gas-phase migration from a leaky well, dissolution into groundwater, advective-dispersive transport and biodegradation of the dissolved methane plume. Gas-phase migration is simulated using the DuMux multiphase simulator, while transport and fate of the dissolved phase is simulated using the BIONAPL/3D reactive transport model. Methane behavior is simulated for two conceptual models: first in a shallow confined aquifer containing a decommissioned leaky well based on a monitored field site near Lindbergh, Alberta, Canada, and secondly on a representative unconfined aquifer based loosely on the Borden, Ontario, field site. The simulations show that the Lindbergh site confined aquifer data are generally consistent with a 2 year methane leak of 2-20 m3/d, assuming anaerobic (sulfate-reducing) methane oxidation and with maximum oxidation rates of 1 × 10-5 to 1 × 10-3 kg/m3/d. Under the highest oxidation rate, dissolved methane decreased from solubility (110 mg/L) to the threshold concentration of 10 mg/L within 5 years. In the unconfined case with the same leakage rate, including both aerobic and anaerobic methane oxidation, the methane plume was less extensive compared to the confined aquifer scenarios. Unconfined aquifers may therefore be less vulnerable to impacts from methane leaks along decommissioned wells. At other potential leakage sites, site-specific data on the natural background geochemistry would be necessary to make reliable predictions on the fate of methane in groundwater.

Sonolysis of hydrocarbons in aqueous solution

NASA Astrophysics Data System (ADS)

Hart, Edwin J.; Fischer, Christian-Herbert; Henglein, Arnim

Water was irradiated with 300 kHz ultrasound under an argon atmosphere containing various amounts of methane and ethane. Limited studies were also made on ethylene, acetylene, propane and butane. The methane and ethane irradiations were carried out over the hydrocarbon-argon range of 2-100%. Maximum decomposition occurs at 15% for methane and 10% for ethane. While hydrogen is a dominant product in both cases, acetylene, ethylene and ethane are prominent products, too. Propane, propene and propin form in lesser quantities. 2-methyl-propane, n-butane, l-butene, 2-methyl-butene, butadiene and n-butin have also been identified. These hydrocarbons are similar to those found in pyrolysis and in fuel rich combustion experiments. Carbon monoxide is an important product at hydrocarbon concentrations less than 40% establishing water was an oxygen delivering reactant under these conditions. In the case of methane, the ratio of ethylene plus acetylene to ethane is used to estimate the effective temperature in the cavitation bubble. A temperature of about 2800 K is obtained for bubbles containing argon (plus water vapor and 20% CH 4) and T = 2000 K for pure methane. The rate of decomposition for unsaturated hydrocarbons is substantially greater than for the saturated ones. Low molecular weight products are mainly formed from saturated hydrocarbons whereas polymerization products are mainly formed from the unsaturated hydrocarbons. The decomposition of acetylene in argon bubbles is one of the fastest sonolytic processes.

Formation of Hydrocarbons in the Outflows from Red Giants

NASA Technical Reports Server (NTRS)

Roberge, Wayne; Kress, Monika; Tielens, Alexander G.

1995-01-01

The formation of hydrocarbons in the oxygen-rich outflows from red giants was studied. The existence of organic molecules in such outflows has been known for several years; however, their surprisingly high abundances has been a mystery since all of the carbon had been thought to be irretrievably locked up in CO, the most strongly bound molecule. CO is the first molecule to form from the atoms present in the star's extended atmosphere, and as strong stellar winds drive a cooling outflow, dust grains condense out. In oxygen-rich outflows, the dust is thought to be composed mainly of silicates and other metal oxides. Perhaps the noble metals can condense out in metallic form, in particular the relatively abundant transition metals iron and nickel. We proposed that perhaps the carbon reservoir held as CO can be accessed through a catalytic process involving the chemisorption of CO and H2 onto grains rich in metallic iron. CO and H2 are the two most abundant molecules in circumstellar outflows, and they both are known to dissociate on transition metal surfaces at elevated temperatures, freeing carbon to form organic molecules such as methane. We believe methane is a precursor molecule to the organics observed in oxygen-rich red giants. We have developed a nonequilibrium numerical model of a surface chemical (catalytic) process. Based on this model, we believe that methane can be formed under the conditions present in circumstellar outflows. Although the methane formation rates are exceptionally low under these conditions, over dynamical timescales, a significant amount of CO can be converted to methane and driven further out in the envelope, explaining the presence of organics there.

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.

Influence of different salt marsh plants on hydrocarbon degrading microorganisms abundance throughout a phenological cycle.

PubMed

Ribeiro, Hugo; Almeida, C Marisa R; Mucha, Ana Paula; Bordalo, Adriano A

2013-01-01

The influence of Juncus maritimus, Phragmites australis, and Triglochin striata on hydrocarbon degrading microorganisms (HD) in Lima River estuary (NW Portugal) was investigated through a year-long plant life cycle. Sediments un-colonized and colonized (rhizosediments) by those salt marsh plants were sampled for HD, total cell counts (TCC), and total petroleum hydrocarbons (TPHs) assessment. Generally, TCC seemed to be markedly thriving by the presence of roots, but without significant (p > 0.05) differences among rhizosediments. Nevertheless, plants seemed to have a distinct influence on HD abundance, particularly during the flowering season, with higher HD abundance in the rhizosediments of the fibrous roots plants (J. maritimus < P. australis < T. striata). Our data suggest that different plants have distinct influence on the dynamics of HD populations within its own rhizosphere, particularly during the flowering season, suggesting a period of higher rhizoremediation activity. Additionally, during the vegetative period, plants with fibrous and dense root system tend to retain hydrocarbons around their belowground tissues more efficiently than plants with adventitious root system. Overall results indicate that fibrous root plants have a higher potential to promote hydrocarbons degradation, and that seasonality should be taken into account when designing long-term rhizoremediation strategies in estuarine areas.

A field experimental study on non-methane hydrocarbon (NMHC) emissions from a straw-returned maize cropping system.

PubMed

Zhang, Shuangqi; Deng, Mengsi; Shan, Ming; Zhou, Chuang; Liu, Wei; Xu, Xiaoqiu; Yang, Xudong

2018-04-28

Non-methane hydrocarbons (NMHCs) play an important role in the atmospheric environment. However, NMHC emissions from agricultural fields, especially their variations with straw return, are poorly understood. Therefore, a field study comprising two treatments, i.e., (1) S0 (straw removal) and (2) S1 (incorporation of maize straw at a rate of 9000 kg ha -1 ), was conducted in a straw-returned maize cropping system to characterize NMHC emissions as well as to estimate the effect of straw return on those emissions. Using a Gas Chromatography-Mass Spectrometer (GC-MS) method, 28 types of NMHCs were identified. The total NMHC emission from S0 was 2018 g ha -1 , where 1-methyl-3-propyl-benzene, (1-methylethyl)-benzene, and toluene were obviously predominant, whereas the total NMHC emission from S1 was 1903 g ha -1 , where 1-methyl-3-propyl-benzene, 2-methyl-pentane, and (1-methylethyl)-benzene were the main species. The results showed that straw return had opposing effects on NMHC emissions, ranging from -55.4% to 478.6%. Overall, the total NMHC emission with returned straw alone decreased by 2963 ng kg straw -1  h -1 . Furthermore, NMHC fluxes had higher correlations with soil temperature than with soil moisture or pH. Notably, the higher correlations of NMHC fluxes with 10 cm soil temperature than with 5 cm soil temperature indicate that soil in the deeper layer might play a more important role in NMHC fluxes. The results also suggest that more field study is needed to accurately estimate the effect of straw return on NMHC emissions from agroecosystems and fully understand its underlying mechanism. Copyright © 2018 Elsevier B.V. All rights reserved.

Temperature-dependent ozone chemiluminescence: A new approach for hydrocarbon monitoring

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

Marley, N.; Gaffney, J.

1996-12-31

Ozone chemiluminescent reactions have been used for some time to detect oxides of nitrogen, ozone, and olefins in air quality studies. Current procedures use non-methane hydrocarbon analyzers based on the flame ionization detector (FID), which quantitate total non-methane hydrocarbons but do not differentiate between the wide variety of volatile organic classes and oxygenates. The other methodology that has been used, gas chromatography/mass spectroscopy (GC/MS), can measure a variety of individual hydrocarbon species and classes, but it is costly, time-consuming, and labor intensive and is not amenable to real-time measurements. Presented here is preliminary research aimed at the development of anmore » alternative to FID and GC/MS: the ozone chemiluminescent detector (OCD) for measurement of a variety of hydrocarbon species and classes by use of the temperature dependence of ozone chemiluminescent reactions. Responses for various hydrocarbon classes obtained with an OCD operated at 170 C or the FID were compared. The results indicate that the OCD detector responds like a total carbon detector at this temperature, with sensitivities 10-100 times higher than those of a FID. Use of the temperature dependence of the chemiluminescent reaction and prereactors will apparently make a real-time hydrocarbon analyzer based on this approach feasible for determination of high-, moderate-, and low-reactivity hydrocarbon levels in ambient air. The OCD approach may be very useful in determining oxygenate emissions from motor vehicles, particularly alternative fuels. The OCD may also be useful in monitoring of ambient air for natural hydrocarbon emissions.« less

Methane and carbon at equilibrium in source rocks

PubMed Central

2013-01-01

Methane in source rocks may not exist exclusively as free gas. It could exist in equilibrium with carbon and higher hydrocarbons: CH4 + C < = > Hydrocarbon. Three lines of evidence support this possibility. 1) Shales ingest gas in amounts and selectivities consistent with gas-carbon equilibrium. There is a 50% increase in solid hydrocarbon mass when Fayetteville Shale is exposed to methane (450 psi) under moderate conditions (100°C): Rock-Eval S2 (mg g-1) 8.5 = > 12.5. All light hydrocarbons are ingested, but with high selectivity, consistent with competitive addition to receptor sites in a growing polymer. Mowry Shale ingests butane vigorously from argon, for example, but not from methane under the same conditions. 2) Production data for a well producing from Fayetteville Shale declines along the theoretical curve for withdrawing gas from higher hydrocarbons in equilibrium with carbon. 3) A new general gas-solid equilibrium model accounts for natural gas at thermodynamic equilibrium, and C6-C7 hydrocarbons constrained to invariant compositions. The results make a strong case for methane in equilibrium with carbon and higher hydrocarbons. If correct, the higher hydrocarbons in source rocks are gas reservoirs, raising the possibility of substantially more gas in shales than analytically apparent, and far more gas in shale deposits than currently recognized. PMID:24330266

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

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.

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

Experimental Assessment of Carbon Isotopes of Light Hydrocarbons under Different Redox Conditions

NASA Astrophysics Data System (ADS)

Fu, Q.; Chen, X.

2017-12-01

Hydrocarbons can be derived from a variety of carbon sources, by different processes, and under a wide range of physicochemical conditions. Other than bacterial activities facilitating biogenic hydrocarbon formation at low temperatures, decomposition of complex organic matter in sedimentary rocks at elevated temperatures produce thermogenic hydrocarbons, whereas abiogenic hydrocarbons are mainly generated through Fischer-Tropsch type synthesis with mineral catalysts. The carbon isotope has been used extensively to distinguish hydrocarbons of different origins and their formation conditions. For each type of hydrocarbons, however, environmental conditions may change reaction pathways and corresponding isotope fractionations. To better understand the variation of carbon isotopes caused by environmental variables, mineral constraints in particular, a series of laboratory experiments are conducted. In experiments where thermogenic hydrocarbons are formed, oil shale is the source material with different gypsum contents (0, 0.3, 0.5, and 1 wt.%). The abundance of generated light straight chain hydrocarbons decreases with increasing gypsum content, but their carbon isotopes become heavier. For example, the δ13C value of methane increases from -55.1‰ to -41.4‰ with gypsum varying between 0 and 1 wt.%. In similar experiments with the presence of MnO2, carbon isotope values of light alkanes are also higher, but with limited magnitudes (e.g., 3 to 4‰ for methane). In another experiment with dissolved H2 gas of 100 mmol/kg, light alkanes become depleted in 13C than experiments without H2. For example, there is a depletion of 2.7‰ for methane. The variation of carbon isotope values of light alkanes suggests the redox condition, constrained by mineral assemblage, fluid composition, and physical environment, play an important role in isotope fractionation. The pathway of hydrocarbon generation may be different under oxidized or reducing conditions. A set of experiments

Non-methane hydrocarbons at a high-altitude rural site in the Mediterranean (Greece)

NASA Astrophysics Data System (ADS)

Moschonas, Nektarios; Glavas, Sotirios

Acetylene, C 3-C 10 paraffins, olefins, aromatic hydrocarbons and the biogenic isoprene, were determined in six sampling periods from May to October in 1996-1997. The concentrations of the determined species were generally lower than those measured in southeastern US and western France, but higher than those measured in more remote regions. Acetylene and C 3-C 5 hydrocarbons exhibited seasonal variation with higher concentrations in the late October sampling period. The aromatic hydrocarbons, except benzene, exhibited maximum concentrations in the summer. Isoprene had maximum concentrations in the summer, with its concentration linearly increasing as a function of the logarithm of temperature, in agreement with past studies. Its emission flux was calculated to be on the lower end of similar studies in US. The main destruction route of all hydrocarbons was determined to be due to their photochemical reactions. The photochemical reactivity, calculated in terms of propylene equivalent concentration, was in the summer dominated by isoprene which accounts for 69% of the total, aromatics with 16%, olefins with 11% and paraffins with 4%. In the May and October periods, the aromatics contributed the most (˜37%) to the photochemical reactivity. Air mass back trajectories indicated higher concentrations when air masses arrived from northwestern and northeastern, compared to southern, directions.

Bacterial Degradation of Phosphonates Bound to High-Molecular-Weight Dissolved Organic Matter Produces Methane and Other Hydrocarbons

NASA Astrophysics Data System (ADS)

Sosa, O.; Ferron Smith, S.; Karl, D. M.; DeLong, E.; Repeta, D.

2016-02-01

The biological degradation of dissolved organic matter (DOM) plays important roles in the carbon cycle and energy balance of the ocean. Yet, the biochemical pathways that drive DOM turnover remain to be fully characterized. In this study, we tested the ability of two open ocean bacterial isolates (a Pseudomonas stutzeri strain (Gammaproteobacteria) and a Sulfitobacter isolate (Alphaproteobacteria)) to degrade DOM phosphonates. Each isolate encoded a complete phosphonate degradation pathway in its genome, and each was able to degrade simple alkyl-phosphonates like methyl phosphonate, releasing methane (or other short chain hydrocarbon gases) as a result. We found that cultures incubated in the presence of HMW DOM polysaccharides also produced methane and other trace gases under aerobic conditions. To demonstrate that phosphonates were the source of these gases, we constructed a P. stutzeri mutant disabled in the phosphonate degradation pathway. Unlike the wild type, the mutant strain was deficient in the production of methane and other gases from HMW DOM-associated phosphonates. These observations support the hypothesis that DOM-bound methyl phosphonates may be a significant source of methane in the water column, and that bacterial degradation of these compounds likely contribute to the subsurface methane maxima observed throughout the world's oceans.

Recent decreases in fossil-fuel emissions of ethane and methane derived from firn air.

PubMed

Aydin, Murat; Verhulst, Kristal R; Saltzman, Eric S; Battle, Mark O; Montzka, Stephen A; Blake, Donald R; Tang, Qi; Prather, Michael J

2011-08-10

Methane and ethane are the most abundant hydrocarbons in the atmosphere and they affect both atmospheric chemistry and climate. Both gases are emitted from fossil fuels and biomass burning, whereas methane (CH(4)) alone has large sources from wetlands, agriculture, landfills and waste water. Here we use measurements in firn (perennial snowpack) air from Greenland and Antarctica to reconstruct the atmospheric variability of ethane (C(2)H(6)) during the twentieth century. Ethane levels rose from early in the century until the 1980s, when the trend reversed, with a period of decline over the next 20 years. We find that this variability was primarily driven by changes in ethane emissions from fossil fuels; these emissions peaked in the 1960s and 1970s at 14-16 teragrams per year (1 Tg = 10(12) g) and dropped to 8-10 Tg  yr(-1) by the turn of the century. The reduction in fossil-fuel sources is probably related to changes in light hydrocarbon emissions associated with petroleum production and use. The ethane-based fossil-fuel emission history is strikingly different from bottom-up estimates of methane emissions from fossil-fuel use, and implies that the fossil-fuel source of methane started to decline in the 1980s and probably caused the late twentieth century slow-down in the growth rate of atmospheric methane.

Origin of Methane and Sources of High Concentrations in Los Angeles Groundwater

NASA Astrophysics Data System (ADS)

Kulongoski, J. T.; McMahon, P. B.; Land, M.; Wright, M. T.; Johnson, T. A.; Landon, M. K.

2018-03-01

In 2014, samples from 37 monitoring wells at 17 locations, within or near oil fields, and one site >5 km from oil fields, in the Los Angeles Basin, California, were analyzed for dissolved hydrocarbon gas isotopes and abundances. The wells sample a variety of depths of an aquifer system composed of unconsolidated and semiconsolidated sediments under various conditions of confinement. Concentrations of methane in groundwater samples ranged from 0.002 to 150 mg/L—some of the highest concentrations reported in a densely populated urban area. The δ13C and δ2H of the methane ranged from -80.8 to -45.5 per mil (‰) and -249.8 to -134.9‰, respectively, and, along with oxidation-reduction processes, helped to identify the origin of methane as microbial methanogenesis and CO2 reduction as its main formation pathway. The distribution of methane concentrations and isotopes is consistent with the high concentrations of methane in Los Angeles Basin groundwater originating from relatively shallow microbial production in anoxic or suboxic conditions. Source of the methane is the aquifer sediments rather than the upward migration or leakage of thermogenic methane associated with oil fields in the basin.

Methane cycling. Nonequilibrium clumped isotope signals in microbial methane.

PubMed

Wang, David T; Gruen, Danielle S; Lollar, Barbara Sherwood; Hinrichs, Kai-Uwe; Stewart, Lucy C; Holden, James F; Hristov, Alexander N; Pohlman, John W; Morrill, Penny L; Könneke, Martin; Delwiche, Kyle B; Reeves, Eoghan P; Sutcliffe, Chelsea N; Ritter, Daniel J; Seewald, Jeffrey S; McIntosh, Jennifer C; Hemond, Harold F; Kubo, Michael D; Cardace, Dawn; Hoehler, Tori M; Ono, Shuhei

2015-04-24

Methane is a key component in the global carbon cycle, with a wide range of anthropogenic and natural sources. Although isotopic compositions of methane have traditionally aided source identification, the abundance of its multiply substituted "clumped" isotopologues (for example, (13)CH3D) has recently emerged as a proxy for determining methane-formation temperatures. However, the effect of biological processes on methane's clumped isotopologue signature is poorly constrained. We show that methanogenesis proceeding at relatively high rates in cattle, surface environments, and laboratory cultures exerts kinetic control on (13)CH3D abundances and results in anomalously elevated formation-temperature estimates. We demonstrate quantitatively that H2 availability accounts for this effect. Clumped methane thermometry can therefore provide constraints on the generation of methane in diverse settings, including continental serpentinization sites and ancient, deep groundwaters. Copyright © 2015, American Association for the Advancement of Science.

ACCUMULATION OF POLY-B-HYDROXYBUTYRATE IN A METHANE- ENRICHED, HALOGENATED, HYDROCARBON-DEGRADING SOIL COLUMN: IMPLICATIONS FOR MICROBIAL COMMUNITY STRUCTURE AND NUTRITIONAL STATUS

EPA Science Inventory

The prokarotic, endogenous storage polymer poly--hydroxybutyrate (PHB) accumulated in soil from a methane-enriched, halogenated hydrocarbon-degrading soil column. Based on phospholipid ester-linked fatty acid (PLFA) profiles, this mocrocosm has been previously reported to be sign...

Compositions and methods for hydrocarbon functionalization

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

Gunnoe, Thomas Brent; Fortman, George; Boaz, Nicholas C.

Embodiments of the present disclosure provide for methods of hydrocarbon functionalization, methods and systems for converting a hydrocarbon into a compound including at least one group ((e.g., hydroxyl group) (e.g., methane to methanol)), functionalized hydrocarbons, and the like.

Methane anomalies in the oxygenated upper waters of the central Baltic Sea associated with zooplankton abundance

NASA Astrophysics Data System (ADS)

Schmale, Oliver; Wäge, Janine; Morholz, Volker; Rehder, Gregor; Wasmund, Norbert; Gräwe, Ulf; Labrenz, Matthias; Loick-Wilde, Natalie

2017-04-01

of the subthermocline methane anomaly showed a clear correlation between seston concentration (i.e. abundance of copepods) and methane production rates.

High molecular weight non-polar hydrocarbons as pure model substances and in motor oil samples can be ionized without fragmentation by atmospheric pressure chemical ionization mass spectrometry.

PubMed

Hourani, Nadim; Kuhnert, Nikolai

2012-10-15

High molecular weight non-polar hydrocarbons are still difficult to detect by mass spectrometry. Although several studies have targeted this problem, lack of good self-ionization has limited the ability of mass spectrometry to examine these hydrocarbons. Failure to control ion generation in the atmospheric pressure chemical ionization (APCI) source hampers the detection of intact stable gas-phase ions of non-polar hydrocarbon in mass spectrometry. Seventeen non-volatile non-polar hydrocarbons, reported to be difficult to ionize, were examined by an optimized APCI methodology using nitrogen as the reagent gas. All these analytes were successfully ionized as abundant and intact stable [M-H](+) ions without the use of any derivatization or adduct chemistry and without significant fragmentation. Application of the method to real-life hydrocarbon mixtures like light shredder waste and car motor oil was demonstrated. Despite numerous reports to the contrary, it is possible to ionize high molecular weight non-polar hydrocarbons by APCI, omitting the use of additives. This finding represents a significant step towards extending the applicability of mass spectrometry to non-polar hydrocarbon analyses in crude oil, petrochemical products, waste or food. Copyright © 2012 John Wiley & Sons, Ltd.

Methane Pyrolysis and Disposing Off Resulting Carbon

NASA Technical Reports Server (NTRS)

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

1999-01-01

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

Detection of abundant ethane and methane, along with carbon monoxide and water, in comet C/1996 B2 Hyakutake: evidence for interstellar origin

NASA Technical Reports Server (NTRS)

Mumma, M. J.; DiSanti, M. A.; Dello Russo, N.; Fomenkova, M.; Magee-Sauer, K.; Kaminski, C. D.; Xie, D. X.

1996-01-01

The saturated hydrocarbons ethane (C2H6) and methane (CH4) along with carbon monoxide (CO) and water (H2O) were detected in comet C/1996 B2 Hyakutake with the use of high-resolution infrared spectroscopy at the NASA Infrared Telescope Facility on Mauna Kea, Hawaii. The inferred production rates of molecular gases from the icy, cometary nucleus (in molecules per second) are 6.4 X 10(26) for C2H6, 1.2 X 10(27) for CH4, 9.8 X 10(27) for CO, and 1.7 X 10(29) for H2O. An abundance of C2H6 comparable to that of CH4 implies that ices in C/1996 B2 Hyakutake did not originate in a thermochemically equilibrated region of the solar nebula. The abundances are consistent with a kinetically controlled production process, but production of C2H6 by gas-phase ion molecule reactions in the natal cloud core is energetically forbidden. The high C2H6/CH4 ratio is consistent with production of C2H6 in icy grain mantles in the natal cloud, either by photolysis of CH4-rich ice or by hydrogen-addition reactions to acetylene condensed from the gas phase.

Diversity and abundance of aerobic and anaerobic methane oxidizers at the Haakon Mosby Mud Volcano, Barents Sea.

PubMed

Lösekann, Tina; Knittel, Katrin; Nadalig, Thierry; Fuchs, Bernhard; Niemann, Helge; Boetius, Antje; Amann, Rudolf

2007-05-01

Submarine mud volcanoes are formed by expulsions of mud, fluids, and gases from deeply buried subsurface sources. They are highly reduced benthic habitats and often associated with intensive methane seepage. In this study, the microbial diversity and community structure in methane-rich sediments of the Haakon Mosby Mud Volcano (HMMV) were investigated by comparative sequence analysis of 16S rRNA genes and fluorescence in situ hybridization. In the active volcano center, which has a diameter of about 500 m, the main methane-consuming process was bacterial aerobic oxidation. In this zone, aerobic methanotrophs belonging to three bacterial clades closely affiliated with Methylobacter and Methylophaga species accounted for 56%+/-8% of total cells. In sediments below Beggiatoa mats encircling the center of the HMMV, methanotrophic archaea of the ANME-3 clade dominated the zone of anaerobic methane oxidation. ANME-3 archaea form cell aggregates mostly associated with sulfate-reducing bacteria of the Desulfobulbus (DBB) branch. These ANME-3/DBB aggregates were highly abundant and accounted for up to 94%+/-2% of total microbial biomass at 2 to 3 cm below the surface. ANME-3/DBB aggregates could be further enriched by flow cytometry to identify their phylogenetic relationships. At the outer rim of the mud volcano, the seafloor was colonized by tubeworms (Siboglinidae, formerly known as Pogonophora). Here, both aerobic and anaerobic methane oxidizers were found, however, in lower abundances. The level of microbial diversity at this site was higher than that at the central and Beggiatoa species-covered part of the HMMV. Analysis of methyl-coenzyme M-reductase alpha subunit (mcrA) genes showed a strong dominance of a novel lineage, mcrA group f, which could be assigned to ANME-3 archaea. Our results further support the hypothesis of Niemann et al. (54), that high methane availability and different fluid flow regimens at the HMMV provide distinct niches for aerobic and

Diversity and Abundance of Aerobic and Anaerobic Methane Oxidizers at the Haakon Mosby Mud Volcano, Barents Sea▿

PubMed Central

Lösekann, Tina; Knittel, Katrin; Nadalig, Thierry; Fuchs, Bernhard; Niemann, Helge; Boetius, Antje; Amann, Rudolf

2007-01-01

Submarine mud volcanoes are formed by expulsions of mud, fluids, and gases from deeply buried subsurface sources. They are highly reduced benthic habitats and often associated with intensive methane seepage. In this study, the microbial diversity and community structure in methane-rich sediments of the Haakon Mosby Mud Volcano (HMMV) were investigated by comparative sequence analysis of 16S rRNA genes and fluorescence in situ hybridization. In the active volcano center, which has a diameter of about 500 m, the main methane-consuming process was bacterial aerobic oxidation. In this zone, aerobic methanotrophs belonging to three bacterial clades closely affiliated with Methylobacter and Methylophaga species accounted for 56% ± 8% of total cells. In sediments below Beggiatoa mats encircling the center of the HMMV, methanotrophic archaea of the ANME-3 clade dominated the zone of anaerobic methane oxidation. ANME-3 archaea form cell aggregates mostly associated with sulfate-reducing bacteria of the Desulfobulbus (DBB) branch. These ANME-3/DBB aggregates were highly abundant and accounted for up to 94% ± 2% of total microbial biomass at 2 to 3 cm below the surface. ANME-3/DBB aggregates could be further enriched by flow cytometry to identify their phylogenetic relationships. At the outer rim of the mud volcano, the seafloor was colonized by tubeworms (Siboglinidae, formerly known as Pogonophora). Here, both aerobic and anaerobic methane oxidizers were found, however, in lower abundances. The level of microbial diversity at this site was higher than that at the central and Beggiatoa species-covered part of the HMMV. Analysis of methyl-coenzyme M-reductase alpha subunit (mcrA) genes showed a strong dominance of a novel lineage, mcrA group f, which could be assigned to ANME-3 archaea. Our results further support the hypothesis of Niemann et al. (54), that high methane availability and different fluid flow regimens at the HMMV provide distinct niches for aerobic and

The long-term evolution of hydrocarbons in Jupiter's stratosphere

NASA Astrophysics Data System (ADS)

Melin, Henrik; Fletcher, Leigh N.; Greathouse, Thomas K.; Giles, Rohini Sara; Sinclair, James; Orton, Glenn S.; Irwin, Patrick Gerard Joseph

2016-10-01

We present the global distribution of hydrocarbons in Jupiter's stratosphere using ground-based mid-infrared R~15,000 TEXES observations from the NASA Infrared Telescope Facility (IRTF), obtained between 2013 and 2016. Ethane and acetylene are the primary products of methane photolysis in Jupiter's stratosphere, and their spatial distribution can be used to trace atmospheric circulation and the lifetimes of chemical constituents. Zonal mean distributions of these species have been previously studied from the Voyager and Cassini spacecraft (Nixon et al., 2010, doi: 10.1016/j.pss.2010.05.008), but the TEXES dataset now provides the opportunity to track the evolution of the hydrocarbons from Earth (Fletcher et al., 2016, doi:10.1016/j.icarus.2016.06.008 ). Global spectral maps of methane, ethane and acetylene emission are used to characterize the temporal evolution of large scale features in Jupiter's stratosphere (0.5-20 mbar?), including: equator to pole contrasts driven by large-scale stratospheric overturning; mid-latitude bands of elevated hydrocarbon emission; small-scale wave phenomena driven by meteorological activity in the underlying troposphere; and the tropical changes in emission related to Jupiter's Quasi-Quadrennial Oscillation. The NEMESIS spectral inversion tool (Irwin et al., 2008, doi: 10.1016/j.jqsrt.2007.11.006) is used to derive stratospheric temperatures and hydrocarbon abundances from spatially-resolved spectra at 744, 819, and 1247 cm-1. We use these to investigate the changes in the vertical temperature and ethane and acetylene distributions over time, with the aim of providing the global and temporal context for Juno's exploration of the jovian atmosphere in 2016/17.

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

Origin of methane and sources of high concentrations in Los Angeles groundwater

USGS Publications Warehouse

Kulongoski, Justin; McMahon, Peter B.; Land, Michael; Wright, Michael; Johnson, Theodore; Landon, Matthew K.

2018-01-01

In 2014, samples from 37 monitoring wells at 17 locations, within or near oil fields, and one site >5 km from oil fields, in the Los Angeles Basin, California, were analyzed for dissolved hydrocarbon gas isotopes and abundances. The wells sample a variety of depths of an aquifer system composed of unconsolidated and semiconsolidated sediments under various conditions of confinement. Concentrations of methane in groundwater samples ranged from 0.002 to 150 mg/L—some of the highest concentrations reported in a densely populated urban area. The δ13C and δ2H of the methane ranged from −80.8 to −45.5 per mil (‰) and −249.8 to −134.9‰, respectively, and, along with oxidation‐reduction processes, helped to identify the origin of methane as microbial methanogenesis and CO2 reduction as its main formation pathway. The distribution of methane concentrations and isotopes is consistent with the high concentrations of methane in Los Angeles Basin groundwater originating from relatively shallow microbial production in anoxic or suboxic conditions. Source of the methane is the aquifer sediments rather than the upward migration or leakage of thermogenic methane associated with oil fields in the basin.

Geologic methane seeps along boundaries of Arctic permafrost thaw and melting glaciers

NASA Astrophysics Data System (ADS)

Walter Anthony, Katey M.; Anthony, Peter; Grosse, Guido; Chanton, Jeffrey

2012-06-01

Methane, a potent greenhouse gas, accumulates in subsurface hydrocarbon reservoirs, such as coal beds and natural gas deposits. In the Arctic, permafrost and glaciers form a `cryosphere cap' that traps gas leaking from these reservoirs, restricting flow to the atmosphere. With a carbon store of over 1,200Pg, the Arctic geologic methane reservoir is large when compared with the global atmospheric methane pool of around 5Pg. As such, the Earth's climate is sensitive to the escape of even a small fraction of this methane. Here, we document the release of 14C-depleted methane to the atmosphere from abundant gas seeps concentrated along boundaries of permafrost thaw and receding glaciers in Alaska and Greenland, using aerial and ground surface survey data and in situ measurements of methane isotopes and flux. We mapped over 150,000 seeps, which we identified as bubble-induced open holes in lake ice. These seeps were characterized by anomalously high methane fluxes, and in Alaska by ancient radiocarbon ages and stable isotope values that matched those of coal bed and thermogenic methane accumulations. Younger seeps in Greenland were associated with zones of ice-sheet retreat since the Little Ice Age. Our findings imply that in a warming climate, disintegration of permafrost, glaciers and parts of the polar ice sheets could facilitate the transient expulsion of 14C-depleted methane trapped by the cryosphere cap.

Hydrocarbon Plume Dynamics in the Worldś Most Spectacular Hydrocarbon Seeps, Santa Barbara Channel, California

NASA Astrophysics Data System (ADS)

Mau, S.; Reed, J.; Clark, J.; Valentine, D.

2006-12-01

Large quantities of natural gas are emitted from the seafloor into the coastal ocean near Coal Oil Point, Santa Barbara Channel (SBC), California. Methane, ethane, and propane were quantified in the surface water at 79 stations in a 270 km2 area in order to map the surficial hydrocarbon plume and to quantify air-sea exchange of these gases. A time series was initiated for 14 stations to identify the variability of the mapped plume, and biologically-mediated oxidation rates of methane were measured to quantify the loss of methane in surface water. The hydrocarbon plume was found to comprise ~70 km2 and extended beyond study area. The plume width narrowed from 3 km near the source to 0.7 km further from the source, and then expanded to 6.7 km at the edge of the study area. This pattern matches the cyclonic gyre which is the normal current flow in this part of the Santa Barbara Channel - pushing water to the shore near the seep field and then broadening the plume while the water turns offshore further from the source. Concentrations of gaseous hydrocarbons decrease as the plume migrates. Time series sampling shows similar plume width and hydrocarbon concentrations when normal current conditions prevail. In contrast, smaller plume width and low hydrocarbon concentrations were observed when an additional anticyclonic eddy reversed the normal current flow, and a much broader plume with higher hydrocarbon concentrations was observed during a time of diminished speed within the current gyre. These results demonstrate that surface currents control hydrocarbon plume dynamics in the SBC, though hydrocarbon flux to the atmosphere is likely less dependent on currents. Estimates of air- sea hydrocarbon flux and biological oxidation rates will also be presented.

C3 Hydrocarbon Abundance in Titan's Atmosphere with Cassini Infrared Spectra

NASA Astrophysics Data System (ADS)

Lombardo, Nicholas; Nixon, Conor; Achterberg, Richard; Jolly, Antoine; Sung, Keeyoon; Irwin, Patrick; Flasar, F. M.

2018-01-01

Titan, the largest moon of the Saturn system, has an astrobiologically important atmosphere. The anoxic nature and high N2 abundance make it a strong analog to the early Earth. The secondary species, CH4, is easily photodissociated, and reactions between its dissociated products give rise to highly complex hydrocarbons and nitriles. The Voyager flyby and 14 year Cassini campaign allowed for the intense study of several of these molecules, enabling scientists to increase our understanding of the chemical pathways present above Titan. In this work, we report abundance profiles of four major C3 gasses expected to occur in Titan’s atmosphere, derived from Cassini/Composite Infrared Spectrometer (CIRS) data, allowing us to fill the gaps in the photochemical zoo that is Titan’s atmosphere.Using the NEMESIS iterative radiative transfer module, we retrieved vertical abundance profiles for propane (C3H8) and propyne (CHCCH3) both initially detected by the Voyager IRIS instrument. Using newly available line data, we were also able to determine the first vertical abundance profiles for propene (C3H6), initially detected in 2013. We present profiles for several latitudes and times and compare to photochemical model predictions and previous observations. We also discuss our ongoing search for allene (CH2CCH2), an isomer of propyne, which has yet to be definitively detected. The abundances we determined will help to further our understanding of the chemical pathways that occur in Titan's atmosphere.

Airborne Measurements of Atmospheric Methane Column Abundance Made Using a Pulsed IPDA Lidar

NASA Technical Reports Server (NTRS)

Riris, Haris; Numata, Kenji; Li, Steve; Wu, Stewart; Ramanathan, Anamd; Dawsey, Martha; Mao, Jianping; Kawa, Randolph; Abshire, James B.

2012-01-01

We report airborne measurements of the column abundance of atmospheric methane made over an altitude range of 3-11 km using a direct detection IPDA lidar with a pulsed laser emitting at 1651 nm. The laser transmitter was a tunable, seeded optical parametric amplifier (OPA) pumped by a Nd:YAG laser and the receiver used a photomultiplier detector and photon counting electronics. The results follow the expected changes with aircraft altitude and the measured line shapes and optical depths show good agreement with theoretical calculations.

Low upper limit to methane abundance on Mars.

PubMed

Webster, Christopher R; Mahaffy, Paul R; Atreya, Sushil K; Flesch, Gregory J; Farley, Kenneth A

2013-10-18

By analogy with Earth, methane in the Martian atmosphere is a potential signature of ongoing or past biological activity. During the past decade, Earth-based telescopic observations reported "plumes" of methane of tens of parts per billion by volume (ppbv), and those from Mars orbit showed localized patches, prompting speculation of sources from subsurface bacteria or nonbiological sources. From in situ measurements made with the Tunable Laser Spectrometer (TLS) on Curiosity using a distinctive spectral pattern specific to methane, we report no detection of atmospheric methane with a measured value of 0.18 ± 0.67 ppbv corresponding to an upper limit of only 1.3 ppbv (95% confidence level), which reduces the probability of current methanogenic microbial activity on Mars and limits the recent contribution from extraplanetary and geologic sources.

Long-term decline of global atmospheric ethane concentrations and implications for methane.

PubMed

Simpson, Isobel J; Sulbaek Andersen, Mads P; Meinardi, Simone; Bruhwiler, Lori; Blake, Nicola J; Helmig, Detlev; Rowland, F Sherwood; Blake, Donald R

2012-08-23

After methane, ethane is the most abundant hydrocarbon in the remote atmosphere. It is a precursor to tropospheric ozone and it influences the atmosphere's oxidative capacity through its reaction with the hydroxyl radical, ethane's primary atmospheric sink. Here we present the longest continuous record of global atmospheric ethane levels. We show that global ethane emission rates decreased from 14.3 to 11.3 teragrams per year, or by 21 per cent, from 1984 to 2010. We attribute this to decreasing fugitive emissions from ethane's fossil fuel source--most probably decreased venting and flaring of natural gas in oil fields--rather than a decline in its other major sources, biofuel use and biomass burning. Ethane's major emission sources are shared with methane, and recent studies have disagreed on whether reduced fossil fuel or microbial emissions have caused methane's atmospheric growth rate to slow. Our findings suggest that reduced fugitive fossil fuel emissions account for at least 10-21 teragrams per year (30-70 per cent) of the decrease in methane's global emissions, significantly contributing to methane's slowing atmospheric growth rate since the mid-1980s.

High abundance and diversity of nitrite-dependent anaerobic methane-oxidizing bacteria in a paddy field profile.

PubMed

Zhou, Leiliu; Wang, Yu; Long, Xi-En; Guo, Jianhua; Zhu, Guibing

2014-11-01

The discovery of nitrite-dependent anaerobic methane oxidation (n-damo) mediated by 'Candidatus Methylomirabilis oxyfera' with nitrite and methane as substrates has connected biogeochemical carbon and nitrogen cycles in a new way. The paddy fields often carry substantial methane and nitrate, thus may be a favorable habitat for n-damo bacteria. In this paper, the vertical-temporal molecular fingerprints of M. oxyfera-like bacteria, including abundance and community composition, were investigated in a paddy soil core in Jiangyin, near the Yangtze River. Through qPCR investigation, high abundance of M. oxyfera-like bacteria up to 1.0 × 10(8) copies (g d.w.s.)(-1) in summer and 8.5 × 10(7) copies (g d.w.s.)(-1) in winter was observed in the ecotone of soil and groundwater in the paddy soil core, which was the highest in natural environments to our knowledge. In the ecotone, the ratio of M. oxyfera-like bacteria to total bacteria reached peak values of 2.80% in summer and 4.41% in winter. Phylogenetic analysis showed n-damo bacteria in the paddy soil were closely related to M. oxyfera and had high diversity in the soil/groundwater ecotone. All of the results indicated the soil/groundwater ecotone of the Jiangyin paddy field was a favorable environment for the growth of n-damo bacteria. © 2014 Federation of European Microbiological Societies. Published by John Wiley & Sons Ltd. All rights reserved.

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

Bacterial methane oxidation in sea-floor gas hydrate: Significance to life in extreme environments

NASA Astrophysics Data System (ADS)

Sassen, Roger; MacDonald, Ian R.; Guinasso, Norman L., Jr.; Joye, Samantha; Requejo, Adolfo G.; Sweet, Stephen T.; Alcalá-Herrera, Javier; Defreitas, Debra A.; Schink, David R.

1998-09-01

Samples of thermogenic hydrocarbon gases, from vents and gas hydrate mounds within a sea-floor chemosynthetic community on the Gulf of Mexico continental slope at about 540 m depth, were collected by research submersible. Our study area is characterized by low water temperature (mean =7 °C), high pressure (about 5400 kPa), and abundant structure II gas hydrate. Bacterial oxidation of hydrate-bound methane (CH4) is indicated by three isotopic properties of gas hydrate samples. Relative to the vent gas from which the gas hydrate formed, (1) methane-bound methane is enriched in 13C by as much as 3.8‰ PDB (Peedee belemnite), (2) hydrate-bound methane is enriched in deuterium (D) by as much as 37‰ SMOW (standard mean ocean water), and (3) hydrate-bound carbon dioxide (CO2) is depleted in 13C by as much as 22.4‰ PDB. Hydrate-associated authigenic carbonate rock is also depleted in 13C. Bacterial oxidation of methane is a driving force in chemosynthetic communities, and in the concomitant precipitation of authigenic carbonate rock that modifies sea-floor geology. Bacterial oxidation of hydrate-bound methane expands the potential boundaries of life in extreme environments.

The Potential for Methane Isotopologue Channels in GOSAT-2

NASA Astrophysics Data System (ADS)

Malina, Edward; Yoshida, Yukio; Matsunaga, Tsuneo; Muller, Jan-Peter

2017-04-01

Of the major Greenhouse Gases (GHGs) currently considered as having a major impact on atmospheric chemistry, Methane is amongst the most important (IPCC, 2014). Methane concentration in the atmosphere has been documented to be rising steadily over the past century, aside from an unexplained short period in the middle of the last decade (Heimann., 2011), leading to renewed efforts to understand global atmospheric Methane. Atmospheric Methane is primarily composed of two key isotopologues, 12CH4 and 13CH4, which have a natural abundance of about 98% and 1.1% respectively. It is a well-established fact that different sources of Methane (i.e. biogenic sources such as methanogens, or non-biogenic such as industrial hydrocarbon burning) vary in the abundance of these isotopologues (Etiope, 2009). The global identification of the ratios of these isotopologues could vastly increase knowledge of global Methane sources, and shed some light on global Methane growth. GOSAT-2 due to be launched in 2018 is a follow on from the original GOSAT mission launched in 2009. GOSAT-2 aims to continue the legacy of GOSAT by providing global measurements of Methane and Carbon Dioxide on a global basis in order to monitor GHG emissions. GOSAT-2 in the context of this study has a significant advantage over GOSAT, which is the extension of the sensitivity of band 3 to 2330nm from 2080nm where significant numbers of Methane spectral lines are located. In this study we apply the well-established Information Content (IC) analysis techniques originally proposed by Rodgers (2000) to determine the potential benefit of retrieving total column Methane isotopologue concentrations assuming bands 2 and 3 of the GOSAT-2/TANSO-FTS-2 instrument. The value of such studies has been proven on multiple occasions and can provide guidance on appropriate potential retrieval setups. Due to the fact that there has been limited research in this area, no 'a priori' state vectors or Variance Covariance Matrices (VCMs

Gene and transcript abundances of bacterial type III secretion systems from the rumen microbiome are correlated with methane yield in sheep.

PubMed

Kamke, Janine; Soni, Priya; Li, Yang; Ganesh, Siva; Kelly, William J; Leahy, Sinead C; Shi, Weibing; Froula, Jeff; Rubin, Edward M; Attwood, Graeme T

2017-08-08

Ruminants are important contributors to global methane emissions via microbial fermentation in their reticulo-rumens. This study is part of a larger program, characterising the rumen microbiomes of sheep which vary naturally in methane yield (g CH 4 /kg DM/day) and aims to define differences in microbial communities, and in gene and transcript abundances that can explain the animal methane phenotype. Rumen microbiome metagenomic and metatranscriptomic data were analysed by Gene Set Enrichment, sparse partial least squares regression and the Wilcoxon Rank Sum test to estimate correlations between specific KEGG bacterial pathways/genes and high methane yield in sheep. KEGG genes enriched in high methane yield sheep were reassembled from raw reads and existing contigs and analysed by MEGAN to predict their phylogenetic origin. Protein coding sequences from Succinivibrio dextrinosolvens strains were analysed using Effective DB to predict bacterial type III secreted proteins. The effect of S. dextrinosolvens strain H5 growth on methane formation by rumen methanogens was explored using co-cultures. Detailed analysis of the rumen microbiomes of high methane yield sheep shows that gene and transcript abundances of bacterial type III secretion system genes are positively correlated with methane yield in sheep. Most of the bacterial type III secretion system genes could not be assigned to a particular bacterial group, but several genes were affiliated with the genus Succinivibrio, and searches of bacterial genome sequences found that strains of S. dextrinosolvens were part of a small group of rumen bacteria that encode this type of secretion system. In co-culture experiments, S. dextrinosolvens strain H5 showed a growth-enhancing effect on a methanogen belonging to the order Methanomassiliicoccales, and inhibition of a representative of the Methanobrevibacter gottschalkii clade. This is the first report of bacterial type III secretion system genes being associated with high

Heavy-machinery traffic impacts methane emissions as well as methanogen abundance and community structure in oxic forest soils.

PubMed

Frey, Beat; Niklaus, Pascal A; Kremer, Johann; Lüscher, Peter; Zimmermann, Stephan

2011-09-01

Temperate forest soils are usually efficient sinks for the greenhouse gas methane, at least in the absence of significant amounts of methanogens. We demonstrate here that trafficking with heavy harvesting machines caused a large reduction in CH(4) consumption and even turned well-aerated forest soils into net methane sources. In addition to studying methane fluxes, we investigated the responses of methanogens after trafficking in two different forest sites. Trafficking generated wheel tracks with different impact (low, moderate, severe, and unaffected). We found that machine passes decreased the soils' macropore space and lowered hydraulic conductivities in wheel tracks. Severely compacted soils yielded high methanogenic abundance, as demonstrated by quantitative PCR analyses of methyl coenzyme M reductase (mcrA) genes, whereas these sequences were undetectable in unaffected soils. Even after a year after traffic compression, methanogen abundance in compacted soils did not decline, indicating a stability of methanogens here over time. Compacted wheel tracks exhibited a relatively constant community structure, since we found several persisting mcrA sequence types continuously present at all sampling times. Phylogenetic analysis revealed a rather large methanogen diversity in the compacted soil, and most mcrA gene sequences were mostly similar to known sequences from wetlands. The majority of mcrA gene sequences belonged either to the order Methanosarcinales or Methanomicrobiales, whereas both sites were dominated by members of the families Methanomicrobiaceae Fencluster, with similar sequences obtained from peatland environments. The results show that compacting wet forest soils by heavy machinery causes increases in methane production and release.

Experimental determination of methane dissolution from simulated subsurface oil leakages

NASA Astrophysics Data System (ADS)

Sauthoff, W.; Peltzer, E. T.; Walz, P. M.; Brewer, P. G.

2013-12-01

Subsurface oil leakages and increased offshore drilling efforts have raised concern over the fate of hydrocarbon mixtures of oil and gas in ocean environments. Recent wellhead and pipeline failures in the Gulf of Mexico are extreme examples of this problem. Understanding the mechanism and rate of vertical transport of hydrocarbon chemical species is necessary to predict the environmental impact of subsurface leakages. In a series of controlled experiments, we carried out a deep-sea field experiment in Monterey Canyon to investigate the behavior of a gas-saturated liquid hydrocarbon mass rising from the seafloor. Aboard the R/V Rachel Carson, we used the ROV Ventana to transport a laboratory prepared volume of decane (C10H22) saturated with methane gas (CH4) to mimic a subsurface seafloor discharge. We released the oil and gas mixture into a vertically oriented open bottom glass tube followed by methane loss rate measurements both at discrete depths, and during rapid, continuous vehicle ascent from 800 to 100 m water depth to monitor changes in dissolution and bubble nucleation. Using laser Raman techniques and HD video we quantified the chemical state of the hydrocarbon fluid, including rate of methane gas dissolution. The primary methane Raman peak was readily observable within the decane C-H stretching complex. Variation in the amount of gas dissolved in the oil greatly influences oil plume density and in turn oil plume vertical rise rate. Our results show that the rise rate of the hydrocarbon mass significantly exceeds the rate at which the excess methane was lost by dissolution. This result implies that vertical transport of methane in the saturated hydrocarbon liquid phase can greatly exceed a gas bubble plume ascending the water column from a seafloor source. These results and observations may be applicable to improved understanding of the composition, distribution, and environmental fate of leaked hydrocarbon mixtures and inform remediation efforts.

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

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.

Distribution, abundance and carbon isotopic composition of gaseous hydrocarbons in Big Soda Lake, Nevada - An alkaline, meromictic lake

NASA Technical Reports Server (NTRS)

Oremland, R. S.; Des Marais, D. J.

1983-01-01

The study of the distribution and isotopic composition of low molecular weight hydrocarbon gases at the Big Soda Lake, Nevada, has shown that while neither ethylene nor propylene were found in the lake, ethane, propane, isobutane and n-butane concentrations all increased with water column depth. It is concluded that methane has a biogenic origin in both the sediments and the anoxic water column, and that C2-C4 alkanes have biogenic origins in the monimolimnion water and shallow sediments. The changes observed in delta C-13/CH4/ and CH4/(C2H6 + C3H8) with depth in the water column and sedimeents are probably due to bacterial processes, which may include anaerobic methane oxidation and different rates of methanogenesis, and C2-to-C4 alkane production by microorganisms.

Mapping Pluto Methane Ice

NASA Image and Video Library

2015-09-24

The Ralph/LEISA infrared spectrometer on NASA's New Horizons spacecraft mapped compositions across Pluto's surface as it flew past the planet on July 14, 2015. On the left, a map of methane ice abundance shows striking regional differences, with stronger methane absorption indicated by the brighter purple colors, and lower abundances shown in black. Data have only been received so far for the left half of Pluto's disk. At right, the methane map is merged with higher-resolution images from the spacecraft's Long Range Reconnaissance Imager (LORRI). http://photojournal.jpl.nasa.gov/catalog/PIA19953

Natural gas fugitive emissions rates constrained by global atmospheric methane and ethane.

PubMed

Schwietzke, Stefan; Griffin, W Michael; Matthews, H Scott; Bruhwiler, Lori M P

2014-07-15

The amount of methane emissions released by the natural gas (NG) industry is a critical and uncertain value for various industry and policy decisions, such as for determining the climate implications of using NG over coal. Previous studies have estimated fugitive emissions rates (FER)--the fraction of produced NG (mainly methane and ethane) escaped to the atmosphere--between 1 and 9%. Most of these studies rely on few and outdated measurements, and some may represent only temporal/regional NG industry snapshots. This study estimates NG industry representative FER using global atmospheric methane and ethane measurements over three decades, and literature ranges of (i) tracer gas atmospheric lifetimes, (ii) non-NG source estimates, and (iii) fossil fuel fugitive gas hydrocarbon compositions. The modeling suggests an upper bound global average FER of 5% during 2006-2011, and a most likely FER of 2-4% since 2000, trending downward. These results do not account for highly uncertain natural hydrocarbon seepage, which could lower the FER. Further emissions reductions by the NG industry may be needed to ensure climate benefits over coal during the next few decades.

Source apportionment vs. emission inventories of non-methane hydrocarbons (NMHC) in an urban area of the Middle East: local and global perspectives

NASA Astrophysics Data System (ADS)

Salameh, Thérèse; Sauvage, Stéphane; Afif, Charbel; Borbon, Agnès; Locoge, Nadine

2016-03-01

We applied the positive matrix factorization model to two large data sets collected during two intensive measurement campaigns (summer 2011 and winter 2012) at a sub-urban site in Beirut, Lebanon, in order to identify NMHC (non-methane hydrocarbons) sources and quantify their contribution to ambient levels. Six factors were identified in winter and five factors in summer. PMF-resolved source profiles were consistent with source profiles established by near-field measurements. The major sources were traffic-related emissions (combustion and gasoline evaporation) in winter and in summer accounting for 51 and 74 wt %, respectively, in agreement with the national emission inventory. The gasoline evaporation related to traffic source had a significant contribution regardless of the season (22 wt % in winter and 30 wt % in summer). The NMHC emissions from road transport are estimated from observations and PMF results, and compared to local and global emission inventories. The PMF analysis finds reasonable differences on emission rates, of 20-39 % higher than the national road transport inventory. However, global inventories (ACCMIP, EDGAR, MACCity) underestimate the emissions up to a factor of 10 for the transportation sector. When combining emission inventory to our results, there is strong evidence that control measures in Lebanon should be targeted on mitigating the NMHC emissions from the traffic-related sources. From a global perspective, an assessment of VOC (volatile organic compounds) anthropogenic emission inventories for the Middle East region as a whole seems necessary as these emissions could be much higher than expected at least from the road transport sector.

40 CFR 86.121-90 - Hydrocarbon analyzer calibration.

Code of Federal Regulations, 2013 CFR

2013-07-01

... used operating range with propane in air calibration gases (either methanol or methane in air as... response factor to methane. When the FID analyzer is to be used for the analysis of gasoline, diesel, methanol, ethanol, liquefied petroleum gas, and natural gas-fueled vehicle hydrocarbon samples, the methane...

40 CFR 86.121-90 - Hydrocarbon analyzer calibration.

Code of Federal Regulations, 2014 CFR

2014-07-01

... used operating range with propane in air calibration gases (either methanol or methane in air as... response factor to methane. When the FID analyzer is to be used for the analysis of gasoline, diesel, methanol, ethanol, liquefied petroleum gas, and natural gas-fueled vehicle hydrocarbon samples, the methane...

40 CFR 86.121-90 - Hydrocarbon analyzer calibration.

Code of Federal Regulations, 2012 CFR

2012-07-01

... used operating range with propane in air calibration gases (either methanol or methane in air as... response factor to methane. When the FID analyzer is to be used for the analysis of gasoline, diesel, methanol, ethanol, liquefied petroleum gas, and natural gas-fueled vehicle hydrocarbon samples, the methane...

Molecular carbon isotopic evidence for the origin of geothermal hydrocarbons

USGS Publications Warehouse

Des Marais, D.J.; Donchin, J.H.; Nehring, N.L.; Truesdell, A.H.

1981-01-01

Previous interest in light hydrocarbons from geothermal systems has focused principally on the origin of the methane1 and the estimation of subsurface temperatures from the carbon isotopic content of coexisting methane and carbon dioxide1-3. Higher molecular weight hydrocarbons were first reported in gases from Yellowstone National Park4, and have since been found to occur commonly in geothermal emanations in the western United States5. Isotopic measurements of individual geothermal hydrocarbons are now reported which help to explain the origin of these hydrocarbons. The thermal decomposition of sedimentary or groundwater organic matter is a principal source of hydrocarbons in four geothermal areas in western North America. ?? 1981 Nature Publishing Group.

Abundances of Jupiter's trace hydrocarbons from Voyager and Cassini

NASA Astrophysics Data System (ADS)

Nixon, C. A.; Achterberg, R. K.; Romani, P. N.; Allen, M.; Zhang, X.; Teanby, N. A.; Irwin, P. G. J.; Flasar, F. M.

2010-11-01

The flybys of Jupiter by the Voyager spacecraft in 1979, and over two decades later by Cassini in 2000, have provided us with unique datasets from two different epochs, allowing the investigation of seasonal change in the atmosphere. In this paper we model zonal averages of thermal infrared spectra from the two instruments, Voyager 1 IRIS and Cassini CIRS, to retrieve the vertical and meridional profiles of temperature, and the abundances of the two minor hydrocarbons, acetylene (C 2H 2) and ethane (C 2H 6). The spatial variation of these gases is controlled by both chemistry and dynamics, and therefore their observed distribution gives us an insight into both processes. We find that the two gases paint quite different pictures of seasonal change. Whilst the 2-D cross-section of C 2H 6 abundance is slightly increased and more symmetric in 2000 (northern summer solstice) compared to 1979 (northern fall equinox), the major trend of equator to pole increase remains. For C 2H 2 on the other hand, the Voyager epoch exhibits almost no latitudinal variation, whilst the Cassini era shows a marked decrease polewards in both hemispheres. At the present time, these experimental findings are in advance of interpretation, as there are no published models of 2-D Jovian seasonal chemical variation available for comparison.

Abundances of Jupiter's Trace Hydrocarbons from Voyager and Cassini

NASA Technical Reports Server (NTRS)

Nixon, C. A.; Achterberg, R. K.; Romani, P. N.; Allen, M.; Zhang, X.; Teanby, N. A.; Irwin, P. G. J.; Flasar, F. M.

2010-01-01

The flybys of Jupiter by the Voyager spacecraft in 1979, and over two decades later by Cassini in 2000, have provided us with unique datasets from two different epochs, allowing the investigation of seasonal change in the atmosphere. In this paper we model zonal averages of thermal infrared spectra from the two instruments, Voyager 1 IRIS and Cassini CIRS, to retrieve the vertical and meridional profiles of temperature, and the abundances of the two minor hydrocarbons, acetylene (C2H2) and ethane (C2H6). The spatial variation of these gases is controlled by both chemistry and dynamics, and therefore their observed distribution gives us an insight into both processes, We find that the two gases paint quite different pictures of seasonal change. Whilst the 2-D cross-section of C2H6 abundance is slightly increased and more symmetric in 2000 (northern summer solstice) compared to 1979 (northern fall equinox), the major trend of equator to pole increase remains. For C2H2 on tile other hand, the Voyager epoch exhibits almost no latitudinal variation, whilst the Cassini era shows a marked decrease polewards in both hemispheres. At the present time, these experimental findings are in advance of interpretation, as there are no published models of 2-D Jovian seasonal chemical variation available for comparison.

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

NASA Astrophysics Data System (ADS)

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

2014-12-01

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

Production of low molecular weight hydrocarbons by volcanic eruptions on early Mars.

PubMed

Segura, Antígona; Navarro-González, Rafael

2005-10-01

Methane and other larger hydrocarbons have been proposed as possible greenhouse gases on early Mars. In this work we explore if volcanic processes may have been a source for such molecules based on theoretical and experimental considerations. Geologic evidence and numerical simulations indicate that explosive volcanism was widely distributed throughout Mars. Volcanic lightning is typically produced in such explosive volcanism. Therefore this geologic setting was studied to determine if lightning could be a source for hydrocarbons in volcanic plumes. Volcanic lightning was simulated by focusing a high-energy infrared laser beam inside of a Pyrex reactor that contained the proposed volcanic gas mixture composed of 64% CH(4), 24% H(2), 10% H(2)O and 2% N(2), according to an accretion model and the nitrogen content measured in Martian meteorites. The analysis of products was performed by gas chromatography coupled to infrared and mass spectroscopy. Eleven hydrocarbons were identified among the products, of which acetylene (C(2)H(2)) was the most abundant. A thermochemical model was used to determine which hydrocarbons could arise only from volcanic heat. In this case, acetylene and ethylene are formed at magmatic temperatures. Our results indicate that explosive volcanism may have injected into the atmosphere of early Mars approximately 6 x 10(12) g yr(-1) of acetylene, and approximately 2 x 10(12) g yr(-1) of 1,3-butadiyne, both produced by volcanic lightning, approximately 5 x 10(11) g yr(-1) of ethylene produced by volcanic heat, and 10(13) g yr(-1) of methane.

Nutrients Can Enhance the Abundance and Expression of Alkane Hydroxylase CYP153 Gene in the Rhizosphere of Ryegrass Planted in Hydrocarbon-Polluted Soil

PubMed Central

Arslan, Muhammad; Afzal, Muhammad; Amin, Imran; Iqbal, Samina; Khan, Qaiser M.

2014-01-01

Plant-bacteria partnership is a promising strategy for the remediation of soil and water polluted with hydrocarbons. However, the limitation of major nutrients (N, P and K) in soil affects the survival and metabolic activity of plant associated bacteria. The objective of this study was to explore the effects of nutrients on survival and metabolic activity of an alkane degrading rhizo-bacterium. Annual ryegrass (Lolium multiflorum) was grown in diesel-contaminated soil and inoculated with an alkane degrading bacterium, Pantoea sp. strain BTRH79, in greenhouse experiments. Two levels of nutrients were applied and plant growth, hydrocarbon removal, and gene abundance and expression were determined after 100 days of sowing of ryegrass. Results obtained from these experiments showed that the bacterial inoculation improved plant growth and hydrocarbon degradation and these were further enhanced by nutrients application. Maximum plant biomass production and hydrocarbon mineralization was observed by the combined use of inoculum and higher level of nutrients. The presence of nutrients in soil enhanced the colonization and metabolic activity of the inoculated bacterium in the rhizosphere. The abundance and expression of CYP153 gene in the rhizosphere of ryegrass was found to be directly associated with the level of applied nutrients. Enhanced hydrocarbon degradation was associated with the population of the inoculum bacterium, the abundance and expression of CYP153 gene in the rhizosphere of ryegrass. It is thus concluded that the combination between vegetation, inoculation with pollutant-degrading bacteria and nutrients amendment was an efficient approach to reduce hydrocarbon contamination. PMID:25360680

Formation of hydrocarbon compounds during the hydrocracking of non-edible vegetable oils with cobalt-nickel supported on hierarchical HZSM-5 catalyst

NASA Astrophysics Data System (ADS)

Marlinda, L.; Al-Muttaqii, M.; Roesyadi, A.; Prajitno, D. H.

2017-05-01

The hierarchical Co-Ni/HZSM-5 catalyst with hierarchical pore structure was prepared by desilication and incipient wetness impregnation. Hydrocracking of non-edible vegetable oils at temperature of 400 °C, 20±5 bar for 2 h was performed in the presence of this type of catalyst under hydrogen initial pressure in pressured batch reactor. Non-edible vegetable oils, such as Reutealis trisperma (Blanco) airy shaw (sunan candlenut) and Hevea brasiliensis (rubber seed) were chosen to study the effect of the degree of saturation and lateral chain length on hydrocarbon compounds obtained through hydrocracking. Cerbera manghas oil was also tested for comparison because the composition of fatty acid was different with the other oils The hydrocracking test indicated that liquid product produced has a similar hydrocarbon compounds with petroleum diesel. The most abundant hydrocarbon is pentadecane (n-C15) and heptadecane (n-C17). The high aromatic compounds were found in liquid product produced in hydrocracking of Sunan candlenut oil.

Formation of diamonds in laser-compressed hydrocarbons at planetary interior conditions

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

Kraus, D.; Vorberger, J.; Pak, A.

The effects of hydrocarbon reactions and diamond precipitation on the internal structure and evolution of icy giant planets such as Neptune and Uranus have been discussed for more than three decades. Inside these celestial bodies, simple hydrocarbons such as methane, which are highly abundant in the atmospheres, are believed to undergo structural transitions that release hydrogen from deeper layers and may lead to compact stratified cores. Indeed, from the surface towards the core, the isentropes of Uranus and Neptune intersect a temperature–pressure regime in which methane first transforms into a mixture of hydrocarbon polymers, whereas, in deeper layers, a phasemore » separation into diamond and hydrogen may be possible. Here in this paper, we show experimental evidence for this phase separation process obtained by in situ X-ray diffraction from polystyrene (C 8H 8) n samples dynamically compressed to conditions around 150 GPa and 5,000 K; these conditions resemble the environment around 10,000 km below the surfaces of Neptune and Uranus. Our findings demonstrate the necessity of high pressures for initiating carbon–hydrogen separation and imply that diamond precipitation may require pressures about ten times as high as previously indicated by static compression experiments. In conclusion, our results will inform mass–radius relationships of carbon-bearing exoplanets, provide constraints for their internal layer structure and improve evolutionary models of Uranus and Neptune, in which carbon–hydrogen separation could influence the convective heat transport.« less

Formation of diamonds in laser-compressed hydrocarbons at planetary interior conditions

DOE PAGES

Kraus, D.; Vorberger, J.; Pak, A.; ...

2017-08-21

The effects of hydrocarbon reactions and diamond precipitation on the internal structure and evolution of icy giant planets such as Neptune and Uranus have been discussed for more than three decades. Inside these celestial bodies, simple hydrocarbons such as methane, which are highly abundant in the atmospheres, are believed to undergo structural transitions that release hydrogen from deeper layers and may lead to compact stratified cores. Indeed, from the surface towards the core, the isentropes of Uranus and Neptune intersect a temperature–pressure regime in which methane first transforms into a mixture of hydrocarbon polymers, whereas, in deeper layers, a phasemore » separation into diamond and hydrogen may be possible. Here in this paper, we show experimental evidence for this phase separation process obtained by in situ X-ray diffraction from polystyrene (C 8H 8) n samples dynamically compressed to conditions around 150 GPa and 5,000 K; these conditions resemble the environment around 10,000 km below the surfaces of Neptune and Uranus. Our findings demonstrate the necessity of high pressures for initiating carbon–hydrogen separation and imply that diamond precipitation may require pressures about ten times as high as previously indicated by static compression experiments. In conclusion, our results will inform mass–radius relationships of carbon-bearing exoplanets, provide constraints for their internal layer structure and improve evolutionary models of Uranus and Neptune, in which carbon–hydrogen separation could influence the convective heat transport.« less

Comparison between Hydrogen and Methane Fuels in a 3-D Scramjet at Mach 8

DTIC Science & Technology

2016-06-24

performance of small chained hydrocarbons ( ethylene and methane) was compared with hydrogen to establish the importance of its lower specific energy...Report Comparison between hydrogen, methane and ethylene fuels in a 3-D Scramjet at Mach 8 Professor Michael K. Smart Chair of Hypersonic Propulsion...hydrocarbons ( ethylene and methane) was compared with hydrogen to establish the importance of its lower specific energy content and slower reaction

Microbiological Survey of Coalbed Methane Basins Across the United States

NASA Astrophysics Data System (ADS)

Tucker, Y.

2017-12-01

Methanogenic organisms exist in the subsurface and produce at least a portion of the methane found within coal seams. This methane is a valuable resource, currently being produced as coal bed methane (CBM) in various sedimentary basins across the United States. This methane is produced by microorganisms that live in coal sediments and can potentially do so at rates that are faster than most themorgenic processes, especially if encouraged. An investigation of microbial communities found within coalbeds across the United States used Illumina 16s-rRNA gene sequencing of DNA extracted coal and water samples from several sedimentary rock basins: Appalachian, Black Warrior, Illinois, San Juan, and Powder River. Chemical analyses of samples were also performed using LC-MS techniques to reveal the chemical composition of these samples. Of the microorganisms found in these samples, up to 60 percent were found to be methanogenic Archaea. The remainder of the microbial community included hydrogen producers as well as hydrocarbon degraders that nicely complement the bio-methane production process in the coal seams. Despite a wide variation in both the percentages of methane producers and in the species diversity, this study indicates that the microbial communities in these CBM reservoirs could be ideal for converting coal to methane. Moreover, methane production data from various wells correlated to the relative abundance of methanogens present. . Information from this research may help field operators to prolong CBM output from existing wells, predict production on future wells and, design methods to restart production in depleted wells. Thus field operators could significantly enhance the lifespan of their existing wells and continue to produce income rather than paying to plug and abandon wells.

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.

Multi-scale monitoring of a marine geologic methane source in the Santa Barbara Channel using imaging spectrometry, ARCTAS-CARB in situ sampling and coastal hourly total hydrocarbon measurements

NASA Astrophysics Data System (ADS)

Bradley, E. S.; Leifer, I.; Roberts, D.; Dennison, P. E.; Margolis, J.; Moritsch, M.; Diskin, G. S.; Sachse, G. W.

2009-12-01

The Coal Oil Point (COP) hydrocarbon seep field off the coast of Santa Barbara, CA is one of the most active and best-studied marine geologic methane sources in the world and contributes to elevated terrestrial methane concentrations downwind. In this study, we investigate the spatiotemporal variability of this local source and the influence of meteorological conditions on transport and concentration. A methane plume emanating from Trilogy Seep was mapped with the Airborne Visible Infrared Imaging Spectrometer at a 7.5 m resolution with a short-wave infrared band ratio technique. This structure agrees with the local wind speed and direction and is orthogonal to the surface currents. ARCTAS-CARB aircraft in situ sampling of lower-troposphere methane is compared to sub-hour total hydrocarbon concentration (THC) measurements from the Santa Barbara Air Pollution Control District (SBAPCD) station located near COP. Hourly SBAPCD THC values from 1980-2008 demonstrate a decrease in seep source strength until the late 1990s, followed by a consistent increase. The occurrence of elevated SBAPCD THC values for onshore wind conditions as well as numerous positive outliers as high as 17 ppm suggests that seep field emissions are both quasi-steady state and transient, direct (bubble) and diffuse (outgassing). As demonstrated for the COP seeps, the combination of imaging spectrometry, aircraft in situ sampling, and ground-based monitoring provides a powerful approach for understanding local methane sources and transport processes.

Non-methane hydrocarbons (NMHCs) and their contribution to ozone formation potential in a petrochemical industrialized city, Northwest China

NASA Astrophysics Data System (ADS)

Jia, Chenhui; Mao, Xiaoxuan; Huang, Tao; Liang, Xiaoxue; Wang, Yanan; Shen, Yanjie; Jiang, Wanyanhan; Wang, Huiqin; Bai, Zhilin; Ma, Minquan; Yu, Zhousuo; Ma, Jianmin; Gao, Hong

2016-03-01

Hourly air concentrations of fifty-three non-methane hydrocarbons (NMHCs) were measured at downtown and suburb of Lanzhou, a petrochemical industrialized city, Northwest China in 2013. The measured data were used to investigate the seasonal characteristics of NMHCs air pollution and their contributions to the ozone formation in Lanzhou. Annually averaged NMHCs concentration was 38.29 ppbv in downtown Lanzhou. Among 53 NMHCs, alkanes, alkenes, and aromatics accounted for 57%, 23% and 20% of the total NMHCs air concentration, respectively. The atmospheric levels of toluene and propane with mean values of 4.62 and 4.56 ppbv were higher than other NMHCs, respectively. The ambient levels of NMHCs in downtown Lanzhou were compared with measured NMHCs data collected at a suburban site of Lanzhou, located near a large-scale petrochemical industry. Results show that the levels of alkanes, alkenes, and aromatics in downtown Lanzhou were lower by factors of 3-11 than that in west suburb of the city. O3-isopleth plots show that ozone was formed in VOCs control area in downtown Lanzhou and NOx control area at the west suburban site during the summertime. Propylene-equivalent (Prop-Equiv) concentration and the maximum incremental reactivity (MIR) in downtown Lanzhou indicate that cis-2-butene, propylene, and m/p-xylene were the first three compounds contributing to ozone formation potentials whereas in the petrochemical industrialized west suburb, ethane, propene, and trans-2-Butene played more important role in the summertime ozone formation. Principal component analysis (PCA) and multiple linear regression (MLR) were further applied to identify the dominant emission sources and examine their fractions in total NMHCs. Results suggest that vehicle emission, solvent usage, and industrial activities were major sources of NMHCs in the city, accounting for 58.34%, 22.19%, and 19.47% of the total monitored NMHCs in downtown Lanzhou, respectively. In the west suburb of the city

Estimates of methane and ethane emissions from the Texas Barnett Shale

NASA Astrophysics Data System (ADS)

Karion, A.; Sweeney, C.; Yacovitch, T.; Petron, G.; Wolter, S.; Conley, S. A.; Hardesty, R. M.; Brewer, A.; Kofler, J.; Newberger, T.; Herndon, S.; Miller, B. R.; Montzka, S. A.; Rella, C.; Crosson, E.; Tsai, T.; Tans, P. P.

2013-12-01

The recent development of horizontal drilling technology by the oil and gas industry has dramatically increased onshore U.S. natural gas and oil production in the last several years. This production boom has led to wide-spread interest from the policy and scientific communities in quantifying the climate impact of the use of natural gas as a replacement for coal. Because the primary component of natural gas is methane, a powerful greenhouse gas, natural gas leakage into the atmosphere affects its climate impact. Several recent scientific field studies have focused on using atmospheric measurements to estimate this leakage in different producing basins. Methane can be measured precisely with commercial analyzers, and deployment of such analyzers on aircraft, coupled with meteorological measurements, can allow scientists to estimate emissions from regions of concentrated production. Ethane and other light hydrocarbons, also components of raw gas, can be used as tracers for differentiating natural gas emissions from those of other methane sources, such as agriculture or landfills, which do not contain any non-methane hydrocarbons such as ethane. Here we present results from one such field campaign in the Barnett Shale near Fort Worth, Texas, in March 2013. Several 4-hour flights were conducted over the natural gas and oil production region with a small single-engine aircraft instrumented with analyzers for measuring ambient methane, carbon monoxide, carbon dioxide, and ethane at high frequencies (0.3-1Hz). The aircraft also measured horizontal winds, temperature, humidity, and pressure, and collected whole air samples in flasks analyzed later for several light hydrocarbons. In addition to the aircraft, a ground-based High-Resolution Doppler Lidar was deployed in the basin to measure profiles of horizontal winds and estimate the boundary layer height 24 hours a day over the campaign period. The aircraft and lidar measurements are used together to estimate methane and

Characterization of methane emissions in Los Angeles with airborne hyperspectral imaging

NASA Astrophysics Data System (ADS)

Saad, K.; Tratt, D. M.; Buckland, K. N.; Roehl, C. M.; Wennberg, P. O.; Wunch, D.

2017-12-01

As urban areas develop regulations to limit atmospheric methane (CH4), accurate quantification of anthropogenic emissions will be critical for program development and evaluation. However, relating emissions derived from process-level metadata to those determined from assimilating atmospheric observations of CH4 concentrations into models is particularly difficult. Non-methane hydrocarbons (NMHCs) can help differentiate between thermogenic and biogenic CH4 emissions, as they are primarily co-emitted with the former; however, these trace gases are subject to the same limitations as CH4. Remotely-sensed hyperspectral imaging bridges these approaches by measuring emissions plumes directly with spatial coverage on the order of 10 km2 min-1. We identify the sources of and evaluate emissions plumes measured by airborne infrared hyperspectral imagers flown over the Los Angeles (LA) metropolitan area, which encompasses various CH4 sources, including petroleum and natural gas wells and facilities. We quantify total CH4 and NMHC emissions, as well as their relative column densities, at the point-source level to create fingerprints of source types. We aggregate these analyses to estimate the range of variability in chemical composition across source types. These CH4 and NMHC emissions factors are additionally compared to their tropospheric column abundances measured by the Total Carbon Column Observing Network (TCCON) Pasadena Fourier transform infrared spectrometer, which provides a footprint for the LA basin.

Hydrocarbons Emissions Due to Wellbore and other Subsurface Leakage in the Uintah Basin, Utah

NASA Astrophysics Data System (ADS)

Watkins, C.; Lyman, S. N.

2015-12-01

The explosive growth of oil and gas production in the United States has focused public and regulatory attention on environmental impacts of hydrocarbon extraction, including air quality and climate impacts. One potentially important emissions source is subsurface leakage of natural gas. Better understanding of wellbore and other subsurface leaks are important in providing ways to decrease pollution while increasing the efficiency of oil and gas production. Soil gas measurements carried out by USGS over the last several years in Utah's oil and gas fields have shown that, while concentrations of methane in soils near wells are typically low, soil gas near some wells can contain more than 50% methane. In the summers of 2013-2015 we carried out campaigns to measure the emission rate of methane and other hydrocarbons from soils near wells in the Uintah Basin, Utah. We also measured emissions at several locations on individual well pads and determined that concentrations of hydrocarbons tend to decrease with distance from the well head. Soil emissions were also measured at non-well sites in the same area to determine background emission rates. Emissions from exposed coal, oil shale, gilsonite, and fault zone surfaces were also measured. Relationships of emissions with soil gas concentrations, meteorological conditions, and soil properties were also investigated.

Microbial Abundances Predict Methane and Nitrous Oxide Fluxes from a Windrow Composting System

PubMed Central

Li, Shuqing; Song, Lina; Gao, Xiang; Jin, Yaguo; Liu, Shuwei; Shen, Qirong; Zou, Jianwen

2017-01-01

Manure composting is a significant source of atmospheric methane (CH4) and nitrous oxide (N2O) that are two potent greenhouse gases. The CH4 and N2O fluxes are mediated by methanogens and methanotrophs, nitrifying and denitrifying bacteria in composting manure, respectively, while these specific bacterial functional groups may interplay in CH4 and N2O emissions during manure composting. To test the hypothesis that bacterial functional gene abundances regulate greenhouse gas fluxes in windrow composting systems, CH4 and N2O fluxes were simultaneously measured using the chamber method, and molecular techniques were used to quantify the abundances of CH4-related functional genes (mcrA and pmoA genes) and N2O-related functional genes (amoA, narG, nirK, nirS, norB, and nosZ genes). The results indicate that changes in interacting physicochemical parameters in the pile shaped the dynamics of bacterial functional gene abundances. The CH4 and N2O fluxes were correlated with abundances of specific compositional genes in bacterial community. The stepwise regression statistics selected pile temperature, mcrA and NH4+ together as the best predictors for CH4 fluxes, and the model integrating nirK, nosZ with pmoA gene abundances can almost fully explain the dynamics of N2O fluxes over windrow composting. The simulated models were tested against measurements in paddy rice cropping systems, indicating that the models can also be applicable to predicting the response of CH4 and N2O fluxes to elevated atmospheric CO2 concentration and rising temperature. Microbial abundances could be included as indicators in the current carbon and nitrogen biogeochemical models. PMID:28373862

LOX/Hydrocarbon Combustion Instability Investigation

NASA Technical Reports Server (NTRS)

Jensen, R. J.; Dodson, H. C.; Claflin, S. E.

1989-01-01

The LOX/Hydrocarbon Combustion Instability Investigation Program was structured to determine if the use of light hydrocarbon combustion fuels with liquid oxygen (LOX) produces combustion performance and stability behavior similar to the LOX/hydrogen propellant combination. In particular methane was investigated to determine if that fuel can be rated for combustion instability using the same techniques as previously used for LOX/hydrogen. These techniques included fuel temperature ramping and stability bomb tests. The hot fire program probed the combustion behavior of methane from ambient to subambient temperatures. Very interesting results were obtained from this program that have potential importance to future LOX/methane development programs. A very thorough and carefully reasoned documentation of the experimental data obtained is contained. The hot fire test logic and the associated tests are discussed. Subscale performance and stability rating testing was accomplished using 40,000 lb. thrust class hardware. Stability rating tests used both bombs and fuel temperature ramping techniques. The test program was successful in generating data for the evaluation of the methane stability characteristics relative to hydrogen and to anchor stability models. Data correlations, performance analysis, stability analyses, and key stability margin enhancement parameters are discussed.

Direct use of methane in coal liquefaction

DOEpatents

Sundaram, Muthu S.; Steinberg, Meyer

1987-01-01

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

Quantification of methane fluxes from hydrocarbon seeps to the ocean and atmosphere: Development of an in situ and online gas flux measuring system

NASA Astrophysics Data System (ADS)

Di, Pengfei; Chen, Qinghua; Chen, Duofu

2017-06-01

Natural hydrocarbon seeps in the marine environment are important contributors to greenhouse gases in the atmosphere. Such gases include methane, which plays a significant role in global carbon cycling and climate change. To accurately quantify the methane flux from hydrocarbon seeps on the seafloor, a specialized in situ and online gas flux measuring (GFM) device was designed to obtain high-resolution time course gas fluxes using the process of equal volume exchange. The device consists of a 1.0-m diameter, 0.9-m tall, inverted conical tent and a GFM instrument that contains a solenoid valve, level transducer, and gas collection chamber. Rising gas bubbles from seeps were measured by laboratory-calibrated GFM instruments attached to the top of the tent. According to the experimental data, the optimal anti-shake time interval was 5 s. The measurement range of the device was 0-15 L min-1, and the relative error was ± 1.0%. The device was initially deployed at an active seep site in the Lingtou Promontory seep field in South China Sea. The amount of gas released from a single gas vent was 30.5 m3 during the measurement period, and the gas flow rate ranged from 22 to 72 L h-1, depending on tidal period, and was strongly negatively correlated with water depth. The measurement results strongly suggest that oceanic tides and swells had a significant forcing effect on gas flux. Low flow rates were associated with high tides and vice versa. The changes in gas volume escaping from the seafloor seeps could be attributed to the hydrostatic pressure induced by water depth. Our findings suggest that in the marine environment, especially in the shallow shelf area, sea level variation may play an important role in controlling methane release into the ocean. Such releases probably also affect atmospheric methane levels.

Methane Clathrate Hydrate Prospecting

NASA Technical Reports Server (NTRS)

Duxbury, N.; Romanovsky, V.

2003-01-01

A method of prospecting for methane has been devised. The impetus for this method lies in the abundance of CH4 and the growing shortages of other fuels. The method is intended especially to enable identification of subpermafrost locations where significant amounts of methane are trapped in the form of methane gas hydrate (CH4(raised dot)6H2O). It has been estimated by the U.S. Geological Survey that the total CH4 resource in CH4(raised dot) 6H2O exceeds the energy content of all other fossil fuels (oil, coal, and natural gas from non-hydrate sources). Also, CH4(raised dot)6H2O is among the cleanest-burning fuels, and CH4 is the most efficient fuel because the carbon in CH4 is in its most reduced state. The method involves looking for a proxy for methane gas hydrate, by means of the combination of a thermal-analysis submethod and a field submethod that does not involve drilling. The absence of drilling makes this method easier and less expensive, in comparison with prior methods of prospecting for oil and natural gas. The proposed method would include thermoprospecting in combination with one more of the other non-drilling measurement techniques, which could include magneto-telluric sounding and/or a subsurface-electrical-resistivity technique. The method would exploit the fact that the electrical conductivity in the underlying thawed region is greater than that in the overlying permafrost.

Widespread abiotic methane in chromitites.

PubMed

Etiope, G; Ifandi, E; Nazzari, M; Procesi, M; Tsikouras, B; Ventura, G; Steele, A; Tardini, R; Szatmari, P

2018-06-07

Recurring discoveries of abiotic methane in gas seeps and springs in ophiolites and peridotite massifs worldwide raised the question of where, in which rocks, methane was generated. Answers will impact the theories on life origin related to serpentinization of ultramafic rocks, and the origin of methane on rocky planets. Here we document, through molecular and isotopic analyses of gas liberated by rock crushing, that among the several mafic and ultramafic rocks composing classic ophiolites in Greece, i.e., serpentinite, peridotite, chromitite, gabbro, rodingite and basalt, only chromitites, characterized by high concentrations of chromium and ruthenium, host considerable amounts of 13 C-enriched methane, hydrogen and heavier hydrocarbons with inverse isotopic trend, which is typical of abiotic gas origin. Raman analyses are consistent with methane being occluded in widespread microfractures and porous serpentine- or chlorite-filled veins. Chromium and ruthenium may be key metal catalysts for methane production via Sabatier reaction. Chromitites may represent source rocks of abiotic methane on Earth and, potentially, on Mars.

Methane heat transfer investigation

NASA Technical Reports Server (NTRS)

1984-01-01

Future high chamber pressure LOX/hydrocarbon booster engines require copper base alloy main combustion chamber coolant channels similar to the SSME to provide adequate cooling and reusable engine life. Therefore, it is of vital importance to evaluate the heat transfer characteristics and coking thresholds for LNG (94% methane) cooling, with a copper base alloy material adjacent to he fuel coolant. High pressure methane cooling and coking characteristics recently evaluated at Rocketdyne using stainless steel heated tubes at methane bulk temperatures and coolant wall temperatures typical of advanced engine operation except at lower heat fluxes as limited by the tube material. As expected, there was no coking observed. However, coking evaluations need be conducted with a copper base surface exposed to the methane coolant at higher heat fluxes approaching those of future high chamber pressure engines.

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

PubMed

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

2014-12-01

Chlorinated aliphatic hydrocarbons (CAHs) are common groundwater contaminants that can be removed from the environment by natural attenuation processes. CAH biodegradation can occur in wetland environments by reductive dechlorination as well as oxidation pathways. In particular, CAH oxidation may occur in vegetated wetlands, by microorganisms that are naturally associated with the roots of wetland plants. The main objective of this study was to evaluate the cometabolic degradation kinetics of the CAHs, cis-1,2-dichloroethene (cisDCE), trichloroethene (TCE), and 1,1,1-trichloroethane (1,1,1TCA), by methane-oxidizing bacteria associated with the roots of a typical wetland plant in soil-free system. Laboratory microcosms with washed live roots investigated aerobic, cometabolic degradation of CAHs by the root-associated methane-oxidizing bacteria at initial aqueous [CH4] ~1.9mgL(-1), and initial aqueous [CAH] ~150μgL(-1); cisDCE and TCE (in the presence of 1,1,1TCA) degraded significantly, with a removal efficiency of approximately 90% and 46%, respectively. 1,1,1TCA degradation was not observed in the presence of active methane oxidizers. The pseudo first-order degradation rate-constants of TCE and cisDCE were 0.12±0.01 and 0.59±0.07d(-1), respectively, which are comparable to published values. However, their biomass-normalized degradation rate constants obtained in this study were significantly smaller than pure-culture studies, yet they were comparable to values reported for biofilm systems. The study suggests that CAH removal in wetland plant roots may be comparable to processes within biofilms. This has led us to speculate that the active biomass may be on the root surface as a biofilm. The cisDCE and TCE mass losses due to methane oxidizers in this study offer insight into the role of shallow, vegetated wetlands as an environmental sink for such xenobiotic compounds. Copyright © 2014 Elsevier B.V. All rights reserved.

Carbon isotope geochemistry of hydrocarbons in the Cerro Prieto geothermal field, Baja California Norte, Mexico

NASA Technical Reports Server (NTRS)

Des Marais, D. J.; Stallard, M. L.; Nehring, N. L.; Truesdell, A. H.

1988-01-01

Hydrocarbon abundances and stable-isotopic compositions were measured in wells M5, M26, M35 and M102, which represent a range of depths (1270-2000 m) and temperatures (275-330 degrees C) in the field. In order to simulate the production of the geothermal hydrocarbons, gases were collected from the pyrolysis of lignite in the laboratory. This lignite was obtained from a well which sampled rock strata which are identical to those occurring in the field, but which have experienced much lower subsurface temperatures. In both the well and the laboratory observations, high-temperature environments favored higher relative concentrations of methane, ethane and benzene and generally higher delta 13C-values in the individual hydrocarbons. The best correlation between the laboratory and well data is obtained when laboratory-produced gases from experiments conducted at lower (400 degrees C) and higher (600 degrees C) temperatures are mixed. This improved correlation suggests that the wells are sampling hydrocarbons produced from a spectrum of depths and temperatures in the sediments.

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.

The Application of Methane Clumped Isotope Measurements to Determine the Source of Large Methane Seeps in Alaskan Lakes

NASA Astrophysics Data System (ADS)

Douglas, P. M.; Stolper, D. A.; Eiler, J. M.; Sessions, A. L.; Walter Anthony, K. M.

2014-12-01

Natural methane emissions from the Arctic present an important potential feedback to global warming. Arctic methane emissions may come from either active microbial sources or from deep fossil reservoirs released by the thawing of permafrost and melting of glaciers. It is often difficult to distinguish between and quantify contributions from these methane sources based on stable isotope data. Analyses of methane clumped isotopes (isotopologues with two or more rare isotopes such as 13CH3D) can complement traditional stable isotope-based classifications of methane sources. This is because clumped isotope abundances (for isotopically equilibrated systems) are a function of temperature and can be used to identify pathways of methane generation. Additionally, distinctive effects of mixing on clumped isotope abundances make this analysis valuable for determining the origins of mixed gasses. We find large variability in clumped isotope compositions of methane from seeps in several lakes, including thermokarst lakes, across Alaska. At Lake Sukok in northern Alaska we observe the emission of dominantly thermogenic methane, with a formation temperature of at least 100° C. At several other lakes we find evidence for mixing between thermogenic methane and biogenic methane that forms in low-temperature isotopic equilibrium. For example, at Eyak Lake in southeastern Alaska, analysis of three methane samples results in a distinctive isotopic mixing line between a high-temperature end-member that formed between 100-170° C, and a biogenic end-member that formed in isotopic equilibrium between 0-20° C. In this respect, biogenic methane in these lakes resembles observations from marine gas seeps, oil degradation, and sub-surface aquifers. Interestingly, at Goldstream Lake in interior Alaska, methane with strongly depleted clumped-isotope abundances, indicative of disequilibrium gas formation, is found, similar to observations from methanogen culture experiments.

Process for the production of ethylene and other hydrocarbons from coal

DOEpatents

Steinberg, Meyer; Fallon, Peter

1986-01-01

A process for the production of economically significant amounts of ethyl and other hydrocarbon compounds, such as benzene, from coal is disclosed wherein coal is reacted with methane at a temperature in the approximate range of 500.degree. C. to 1100.degree. C. at a partial pressure less than about 200 psig for a period of less than 10 seconds. Ethylene and other hydrocarbon compounds may be separated from the product stream so produced, and the methane recycled for further production of ethylene. In another embodiment, other compounds produced, such as by-product tars, may be burned to heat the recycled methane.

Paleozoic Hydrocarbon-Seep Limestones

NASA Astrophysics Data System (ADS)

Peckmann, J.

2007-12-01

To date, five Paleozoic hydrocarbon-seep limestones have been recognized based on carbonate fabrics, associated fauna, and stable carbon isotopes. These are the Middle Devonian Hollard Mound from the Antiatlas of Morocco [1], Late Devonian limestone lenses with the dimerelloid brachiopod Dzieduszyckia from the Western Meseta of Morocco [2], Middle Mississippian limestones with the dimerelloid brachiopod Ibergirhynchia from the Harz Mountains of Germany [3], Early Pennsylvanian limestones from the Tantes Mound in the High Pyrenees of France [4], and Late Pennsylvanian limestone lenses from the Ganigobis Shale Member of southern Namibia [5]. Among these examples, the composition of seepage fluids varied substantially as inferred from delta C-13 values of early diagenetic carbonate phases. Delta C-13 values as low as -50 per mil from the Tantes Mound and -51 per mil from the Ganigobis limestones reveal seepage of biogenic methane, whereas values of -12 per mil from limestones with Dzieduszyckia associated with abundant pyrobitumen agree with oil seepage. Intermediate delta C-13 values of carbonate cements from the Hollard Mound and Ibergirhynchia deposits probably reflect seepage of thermogenic methane. It is presently very difficult to assess the faunal evolution at seeps in the Paleozoic based on the limited number of examples. Two of the known seeps were typified by extremely abundant rhynchonellide brachiopods of the superfamily Dimerelloidea. Bivalve mollusks and tubeworms were abundant at two of the known Paleozoic seep sites; one was dominated by bivalve mollusks (Hollard Mound, Middle Devonian), another was dominated by tubeworms (Ganigobis Shale Member, Late Pennsylvanian). The tubeworms from these two deposits are interpreted to represent vestimentiferan worms, based on studies of the taphonomy of modern vestimentiferans. However, this interpretation is in conflict with the estimated evolutionary age of vestimentiferans based on molecular clock methods

Direct use of methane in coal liquefaction

DOEpatents

Sundaram, M.S.; Steinberg, M.

1985-06-19

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

40 CFR 88.102-94 - Definitions.

Code of Federal Regulations, 2010 CFR

2010-07-01

... standard. Non-methane Hydrocarbon Equivalent means the sum of the carbon mass emissions of non-oxygenated non-methane hydrocarbons plus the carbon mass emissions of alcohols, aldehydes, or other organic..., expressed as gasoline-fueled vehicle non-methane hydrocarbons. In the case of exhaust emissions, the...

40 CFR 88.102-94 - Definitions.

Code of Federal Regulations, 2012 CFR

2012-07-01

... standard. Non-methane Hydrocarbon Equivalent means the sum of the carbon mass emissions of non-oxygenated non-methane hydrocarbons plus the carbon mass emissions of alcohols, aldehydes, or other organic..., expressed as gasoline-fueled vehicle non-methane hydrocarbons. In the case of exhaust emissions, the...

40 CFR 88.102-94 - Definitions.

Code of Federal Regulations, 2013 CFR

2013-07-01

... standard. Non-methane Hydrocarbon Equivalent means the sum of the carbon mass emissions of non-oxygenated non-methane hydrocarbons plus the carbon mass emissions of alcohols, aldehydes, or other organic..., expressed as gasoline-fueled vehicle non-methane hydrocarbons. In the case of exhaust emissions, the...

40 CFR 88.102-94 - Definitions.

Code of Federal Regulations, 2014 CFR

2014-07-01

... standard. Non-methane Hydrocarbon Equivalent means the sum of the carbon mass emissions of non-oxygenated non-methane hydrocarbons plus the carbon mass emissions of alcohols, aldehydes, or other organic..., expressed as gasoline-fueled vehicle non-methane hydrocarbons. In the case of exhaust emissions, the...

mcrA Gene abundance correlates with hydrogenotrophic methane production rates in full-scale anaerobic waste treatment systems.

PubMed

Morris, R L; Tale, V P; Mathai, P P; Zitomer, D H; Maki, J S

2016-02-01

Anaerobic treatment is a sustainable and economical technology for waste stabilization and production of methane as a renewable energy. However, the process is under-utilized due to operational challenges. Organic overload or toxicants can stress the microbial community that performs waste degradation, resulting in system failure. In addition, not all methanogenic microbial communities are equally capable of consistent, maximum biogas production. Opinion varies as to which parameters should be used to monitor the fitness of digester biomass. No standard molecular tools are currently in use to monitor and compare full-scale operations. It was hypothesized that determining the number of gene copies of mcrA, a methanogen-specific gene, would positively correlate with specific methanogenic activity (SMA) rates from biomass samples from six full-scale anaerobic digester systems. Positive correlations were observed between mcrA gene copy numbers and methane production rates against H2  : CO2 and propionate (R(2)  = 0·67-0·70, P < 0·05) but not acetate (R(2)  = 0·49, P > 0·05). Results from this study indicate that mcrA gene targeted qPCR can be used as an alternate tool to monitor and compare certain methanogen communities in anaerobic digesters. Using quantitative PCR (qPCR), we demonstrate that the abundance of mcrA, a gene specific to methane producing archaea, correlated with specific methanogenic activity (SMA) measurements when H2 and CO2 , or propionate were provided as substrates. However, mcrA abundance did not correlate with SMA with acetate. SMA values are often used as a fitness indicator of anaerobic biomass. Results from qPCR can be obtained within a day while SMA analysis requires days to weeks to complete. Therefore, qPCR for mcrA abundance is a sensitive and fast method to compare and monitor the fitness of certain anaerobic biomass. As a monitoring tool, qPCR of mcrA will help anaerobic digester operators optimize treatment and encourage

40 CFR 86.1221-90 - Hydrocarbon analyzer calibration.

Code of Federal Regulations, 2012 CFR

2012-07-01

... methane. When the FID analyzer to be used for the analysis of natural gas-fueled vehicle hydrocarbon... and liquefied petroleum gas-fuel shall be optimized using propane. Analyzers used with natural gas... air (or methane in air as appropriate) calibration gases having nominal concentrations of 15, 30, 45...

40 CFR 86.1221-90 - Hydrocarbon analyzer calibration.

Code of Federal Regulations, 2013 CFR

2013-07-01

... methane. When the FID analyzer to be used for the analysis of natural gas-fueled vehicle hydrocarbon... and liquefied petroleum gas-fuel shall be optimized using propane. Analyzers used with natural gas... air (or methane in air as appropriate) calibration gases having nominal concentrations of 15, 30, 45...

Assessing the Efficacy of the Aerobic Methanotrophic Biofilter in Methane Hydrate Environments

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

Valentine, David

2012-09-30

In October 2008 the University of California at Santa Barbara (UCSB) initiated investigations of water column methane oxidation in methane hydrate environments, through a project funded by the National Energy Technology Laboratory (NETL) entitled: assessing the efficacy of the aerobic methanotrophic biofilter in methane hydrate environments. This Final Report describes the scientific advances and discoveries made under this award as well as the importance of these discoveries in the broader context of the research area. Benthic microbial mats inhabit the sea floor in areas where reduced chemicals such as sulfide reach the more oxidizing water that overlies the sediment. Wemore » set out to investigate the role that methanotrophs play in such mats at locations where methane reaches the sea floor along with sulfide. Mats were sampled from several seep environments and multiple sets were grown in-situ at a hydrocarbon seep in the Santa Barbara Basin. Mats grown in-situ were returned to the laboratory and used to perform stable isotope probing experiments in which they were treated with 13C-enriched methane. The microbial community was analyzed, demonstrating that three or more microbial groups became enriched in methane?s carbon: methanotrophs that presumably utilize methane directly, methylotrophs that presumably consume methanol excreted by the methanotrophs, and sulfide oxidizers that presumably consume carbon dioxide released by the methanotrophs and methylotrophs. Methanotrophs reached high relative abundance in mats grown on methane, but other bacterial processes include sulfide oxidation appeared to dominate mats, indicating that methanotrophy is not a dominant process in sustaining these benthic mats, but rather a secondary function modulated by methane availability. Methane that escapes the sediment in the deep ocean typically dissolved into the overlying water where it is available to methanotrophic bacteria. We set out to better understand the efficacy of

Reservoir simulation with the cubic plus (cross-) association equation of state for water, CO2, hydrocarbons, and tracers

NASA Astrophysics Data System (ADS)

Moortgat, Joachim

2018-04-01

This work presents an efficient reservoir simulation framework for multicomponent, multiphase, compressible flow, based on the cubic-plus-association (CPA) equation of state (EOS). CPA is an accurate EOS for mixtures that contain non-polar hydrocarbons, self-associating polar water, and cross-associating molecules like methane, ethane, unsaturated hydrocarbons, CO2, and H2S. While CPA is accurate, its mathematical formulation is highly non-linear, resulting in excessive computational costs that have made the EOS unfeasible for large scale reservoir simulations. This work presents algorithms that overcome these bottlenecks and achieve an efficiency comparable to the much simpler cubic EOS approach. The main applications that require such accurate phase behavior modeling are 1) the study of methane leakage from high-pressure production wells and its potential impact on groundwater resources, 2) modeling of geological CO2 sequestration in brine aquifers when one is interested in more than the CO2 and H2O components, e.g. methane, other light hydrocarbons, and various tracers, and 3) enhanced oil recovery by CO2 injection in reservoirs that have previously been waterflooded or contain connate water. We present numerical examples of all those scenarios, extensive validation of the CPA EOS with experimental data, and analyses of the efficiency of our proposed numerical schemes. The accuracy, efficiency, and robustness of the presented phase split computations pave the way to more widespread adoption of CPA in reservoir simulators.

In Situ Hydrocarbon Degradation by Indigenous Nearshore Bacterial Populations

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

Cherrier, J.

). Results from these time series experiments demonstrated that short-term exposure of petroleum to UV light enhanced hydrocarbon degradation by 48% over that observed for non-photo-oxidized petroleum. Despite the greater bio-availability of the photo-oxidized over the non-photo-oxidized petroleum, an initial lag in CO{sub 2} production was observed indicating potential phototoxicity of the photo- by-products. {delta}{sup 13}C analysis and mass balance calculations reveal that co-metabolism with pinfish resulted in increased hydrocarbon degradation for both photo-oxidized and non-photo-oxidized petroleum each by over 100%. These results demonstrate the cumulative effect of photo-oxidation and co-metabolism on petroleum hydrocarbon degradation by natural bacterial populations indigenous to systems chronically impacted by hydrocarbon input. To address the second objective of this proposal bacterial concentrates were collected from Bayboro Harbor in April 2001 for nucleic acid extraction and subsequent natural radiocarbon abundance analyses. Unfortunately, however, all of these samples were lost due to a faulty compressor in our -70 freezer. The freezer was subsequently repaired and samples were again collected from Bayboro Harbor in June 2002 and again December 2002. Several attempts were made to extract the nucleic acid samples--however, the student was not able to successfully extract and an adequate amount of uncontaminated nucleic acid samples for subsequent natural radiocarbon abundance measurements of the bacterial carbon by accelerator mass spectrometry (i.e. require at least 50 {micro}g carbon for AMS measurement). Consequently, we were not able to address the second objective of this proposed work.« less

2015 Survey of Non-Starch Ethanol and Renewable Hydrocarbon Biofuels Producers

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

Schwab, Amy; Warner, Ethan; Lewis, John

In order to understand the anticipated status of the industry for non-starch ethanol and renewable hydrocarbon biofuels as of the end of calendar year 2015, the National Renewable Energy Laboratory (NREL) conducted its first annual survey update of U.S. non-starch ethanol and renewable hydrocarbon biofuels producers. This report presents the results of this survey, describes the survey methodology, and documents important changes since the 2013 survey.

Abiogenic formation of alkanes in the Earth's crust as a minor source for global hydrocarbon reservoirs.

PubMed

Sherwood Lollar, B; Westgate, T D; Ward, J A; Slater, G F; Lacrampe-Couloume, G

2002-04-04

Natural hydrocarbons are largely formed by the thermal decomposition of organic matter (thermogenesis) or by microbial processes (bacteriogenesis). But the discovery of methane at an East Pacific Rise hydrothermal vent and in other crustal fluids supports the occurrence of an abiogenic source of hydrocarbons. These abiogenic hydrocarbons are generally formed by the reduction of carbon dioxide, a process which is thought to occur during magma cooling and-more commonly-in hydrothermal systems during water-rock interactions, for example involving Fischer-Tropsch reactions and the serpentinization of ultramafic rocks. Suggestions that abiogenic hydrocarbons make a significant contribution to economic hydrocarbon reservoirs have been difficult to resolve, in part owing to uncertainty in the carbon isotopic signatures for abiogenic versus thermogenic hydrocarbons. Here, using carbon and hydrogen isotope analyses of abiogenic methane and higher hydrocarbons in crystalline rocks of the Canadian shield, we show a clear distinction between abiogenic and thermogenic hydrocarbons. The progressive isotopic trends for the series of C1-C4 alkanes indicate that hydrocarbon formation occurs by way of polymerization of methane precursors. Given that these trends are not observed in the isotopic signatures of economic gas reservoirs, we can now rule out the presence of a globally significant abiogenic source of hydrocarbons.

Post-Shock Sampling of Shock-Heated Hydrocarbon Fuels

DTIC Science & Technology

2016-07-07

on the ability to measure key hydrocarbon fragments (e.g. ethylene , methane, and acetylene) over a wide range of temperatures and pressures. The...series of experiments was conducted to validate the sampling system results and explore the thermal decomposition of ethylene and methane. Initially, a...1% ethylene /0.1% methane/balance argon fuel mixture was shock-heated to ~960 K – a temperature low enough that no reaction would occur. GC analysis

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

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.

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

PubMed Central

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

2013-01-01

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

Atmospheric pressure chemical ionization studies of non-polar isomeric hydrocarbons using ion mobility spectrometry and mass spectrometry with different ionization techniques

NASA Technical Reports Server (NTRS)

Borsdorf, H.; Nazarov, E. G.; Eiceman, G. A.

2002-01-01

The ionization pathways were determined for sets of isomeric non-polar hydrocarbons (structural isomers, cis/trans isomers) using ion mobility spectrometry and mass spectrometry with different techniques of atmospheric pressure chemical ionization to assess the influence of structural features on ion formation. Depending on the structural features, different ions were observed using mass spectrometry. Unsaturated hydrocarbons formed mostly [M - 1]+ and [(M - 1)2H]+ ions while mainly [M - 3]+ and [(M - 3)H2O]+ ions were found for saturated cis/trans isomers using photoionization and 63Ni ionization. These ionization methods and corona discharge ionization were used for ion mobility measurements of these compounds. Different ions were detected for compounds with different structural features. 63Ni ionization and photoionization provide comparable ions for every set of isomers. The product ions formed can be clearly attributed to the structures identified. However, differences in relative abundance of product ions were found. Although corona discharge ionization permits the most sensitive detection of non-polar hydrocarbons, the spectra detected are complex and differ from those obtained with 63Ni ionization and photoionization. c. 2002 American Society for Mass Spectrometry.

Secondary migration and leakage of methane from a major tight-gas system

NASA Astrophysics Data System (ADS)

Wood, James M.; Sanei, Hamed

2016-11-01

Tight-gas and shale-gas systems can undergo significant depressurization during basin uplift and erosion of overburden due primarily to the natural leakage of hydrocarbon fluids. To date, geologic factors governing hydrocarbon leakage from such systems are poorly documented and understood. Here we show, in a study of produced natural gas from 1,907 petroleum wells drilled into a Triassic tight-gas system in western Canada, that hydrocarbon fluid loss is focused along distinct curvilinear pathways controlled by stratigraphic trends with superior matrix permeability and likely also structural trends with enhanced fracture permeability. Natural gas along these pathways is preferentially enriched in methane because of selective secondary migration and phase separation processes. The leakage and secondary migration of thermogenic methane to surficial strata is part of an ongoing carbon cycle in which organic carbon in the deep sedimentary basin transforms into methane, and ultimately reaches the near-surface groundwater and atmosphere.

40 CFR 88.103-94 - Abbreviations.

Code of Federal Regulations, 2014 CFR

2014-07-01

... Vehicle LDT—Light-Duty Truck LDV—Light-Duty Vehicle NMHC—Non-Methane Hydrocarbon NMHCE—Non-Methane Hydrocarbon Equivalent NMOG—Non-Methane Organic Gas NOx—Nitrogen Oxides PM—Particulate Matter GVWR—Gross...

40 CFR 88.103-94 - Abbreviations.

Code of Federal Regulations, 2011 CFR

2011-07-01

... Vehicle LDT—Light-Duty Truck LDV—Light-Duty Vehicle NMHC—Non-Methane Hydrocarbon NMHCE—Non-Methane Hydrocarbon Equivalent NMOG—Non-Methane Organic Gas NOx—Nitrogen Oxides PM—Particulate Matter GVWR—Gross...

40 CFR 88.103-94 - Abbreviations.

Code of Federal Regulations, 2013 CFR

2013-07-01

... Vehicle LDT—Light-Duty Truck LDV—Light-Duty Vehicle NMHC—Non-Methane Hydrocarbon NMHCE—Non-Methane Hydrocarbon Equivalent NMOG—Non-Methane Organic Gas NOx—Nitrogen Oxides PM—Particulate Matter GVWR—Gross...

40 CFR 88.103-94 - Abbreviations.

Code of Federal Regulations, 2012 CFR

2012-07-01

... Vehicle LDT—Light-Duty Truck LDV—Light-Duty Vehicle NMHC—Non-Methane Hydrocarbon NMHCE—Non-Methane Hydrocarbon Equivalent NMOG—Non-Methane Organic Gas NOx—Nitrogen Oxides PM—Particulate Matter GVWR—Gross...

40 CFR 88.103-94 - Abbreviations.

Code of Federal Regulations, 2010 CFR

2010-07-01

... Vehicle LDT—Light-Duty Truck LDV—Light-Duty Vehicle NMHC—Non-Methane Hydrocarbon NMHCE—Non-Methane Hydrocarbon Equivalent NMOG—Non-Methane Organic Gas NOx—Nitrogen Oxides PM—Particulate Matter GVWR—Gross...

Methane in Pluto's Atmosphere

NASA Astrophysics Data System (ADS)

Roe, Henry G.

2006-09-01

The abundance of methane in Pluto's atmosphere has not been remeasured since its initial detection in 1992 by Young et al. (1997). As Pluto recedes from the Sun its atmosphere should eventually collapse and freeze out on the surface, but recent occultation observations (Elliot et al. 2003) show an expansion of the atmosphere rather than contraction. New measurements of Pluto's atmospheric methane abundance are warranted. We obtained high resolution (R=25000) near-infrared spectra of Pluto in July 2006 with NIRSPEC at the W.M. Keck II telescope and will report our initial analysis and results.

2016 Survey of Non-Starch Alcohol and Renewable Hydrocarbon Biofuels Producers

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

Warner, Ethan; Schwab, Amy; Bacovsky, Dina

In order to understand the anticipated status of the industry for non-starch ethanol and renewable hydrocarbon biofuels as of the end of calendar year 2015, the National Renewable Energy Laboratory (NREL) updated its annual survey of U.S. non-starch ethanol and renewable hydrocarbon biofuels producers. This report presents the results of this survey update, describes the survey methodology, and documents important changes since the 2015 survey published at the end of 2015 (Schwab et al. 2015).

Engineering of Methane Metabolism in Pichia Pastoris Through Methane Monooxygenase Expression

NASA Technical Reports Server (NTRS)

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

2017-01-01

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

Nonequilibrium clumped isotope signals in microbial methane

USGS Publications Warehouse

Wang, David T.; Gruen, Danielle S.; Lollar, Barbara Sherwood; Hinrichs, Kai-Uwe; Stewart, Lucy C.; Holden, James F.; Hristov, Alexander N.; Pohlman, John W.; Morrill, Penny L.; Könneke, Martin; Delwiche, Kyle B.; Reeves, Eoghan P.; Sutcliffe, Chelsea N.; Ritter, Daniel J.; Seewald, Jeffrey S.; McIntosh, Jennifer C.; Hemond, Harold F.; Kubo, Michael D.; Cardace, Dawn; Hoehler, Tori M.; Ono, Shuhei

2015-01-01

Methane is a key component in the global carbon cycle with a wide range of anthropogenic and natural sources. Although isotopic compositions of methane have traditionally aided source identification, the abundance of its multiply-substituted “clumped” isotopologues, e.g., 13CH3D, has recently emerged as a proxy for determining methane-formation temperatures; however, the impact of biological processes on methane’s clumped isotopologue signature is poorly constrained. We show that methanogenesis proceeding at relatively high rates in cattle, surface environments, and laboratory cultures exerts kinetic control on 13CH3D abundances and results in anomalously elevated formation temperature estimates. We demonstrate quantitatively that H2 availability accounts for this effect. Clumped methane thermometry can therefore provide constraints on the generation of methane in diverse settings, including continental serpentinization sites and ancient, deep groundwaters.

Limnological structure of Titan's hydrocarbon lakes and its astrobiological implication.

PubMed

Tokano, Tetsuya

2009-03-01

Cassini radar recently detected several putative liquid hydrocarbon lakes in the polar region of Saturn's moon Titan. Such lakes may contain organic sediments deposited from the atmosphere that would promote prebiotic-type chemistry driven by cosmic rays, the result of which could be the production of more complex molecules such as nitrogen-bearing organic polymer or azides. The physical properties of the lake and their temporal evolution under Titan's present climatic setting were investigated by means of a one-dimensional lake thermal stratification model. Lakes can undergo various evolutions, depending on the initial composition and depth of the lake and hydrocarbon abundance in the near-surface atmosphere. Pure methane ponds, which may occasionally form when heavy methane hailstones reach the surface, would be transitory in that they would evaporate, freeze up, and eventually dry up. On the other hand, lakes filled with a mixture of methane, ethane, and nitrogen would be more stable; and freezing or drying would not necessarily occur in most cases. Such lakes undergo a seasonal cycle of thermal stratification in spring and early summer and convective overturning in other seasons. The summer thermal stratification near the lake surface could be destabilized by bottom heating as a result of an enhanced geothermal heat flux, e.g., in the vicinity of cryovolcanoes. Most likely the composition of the lake and atmosphere would come to equilibrium by way of a small amount of evaporation, but the lake-atmosphere system could be repeatedly brought out of equilibrium by irregular precipitation. The viability of prebiotic-like chemistry in the lake may depend on many lake parameters, such as temperature, liquid or frozen state, and convective mixing. Moreover, convective mixing may drive suspension of solid acetylene and other sediments on the lake bottom and redistribution of dissolved gases, which might be relevant for putative life-forms that consume hydrogen and solid

Methane on Mars: Measurements and Possible Origins

NASA Technical Reports Server (NTRS)

Mumma, Michael J.; Villanueva, Geronimo L.; Novak, Robert E.; Radeva, Yana L.; Kaufl, H. Ulrich; Tokunaga, Alan; Encrenaz, Therese; Hartogh, Paul

2011-01-01

The presence of abundant methane in Earth's atmosphere (1.6 parts per million) requires sources other than atmospheric chemistry. Living systems produce more than 90% of Earth's atmospheric methane; the balance is of geochemical origin. On Mars, methane has been sought for nearly 40 years because of its potential biological significance, but it was detected only recently [1-5]. Its distribution on the planet is found to be patchy and to vary with time [1,2,4,5], suggesting that methane is released recently from the subsurface in localized areas, and is then rapidly destroyed [1,6]. Before 2000, searchers obtained sensitive upper limits for methane by averaging over much of Mars' dayside hemisphere, using data acquired by Marsorbiting spacecraft (Mariner 9) and Earth-based observatories (Kitt Peak National Observatory, Canada- France-Hawaii Telescope, Infrared Space Observatory). These negative findings suggested that methane should be searched at higher spatial resolution since the local abundance could be significantly larger at active sites. Since 2001, searches for methane have emphasized spatial mapping from terrestrial observatories and from Mars orbit (Mars Express).

Constraining Methane Abundance and Cloud Properties from the Reflected Light Spectra of Directly Imaged Exoplanets

NASA Astrophysics Data System (ADS)

Lupu, R.; Marley, M. S.; Lewis, N. K.

2015-12-01

We have assembled an atmospheric retrieval package for the reflected light spectra of gas- and ice- giants in order to inform the design and estimate the scientific return of future space-based coronagraph instruments. Such instruments will have a working bandpass of ~0.4-1 μm and a resolving power R~70, and will enable the characterization of tens of exoplanets in the Solar neighborhood. The targets will be chosen form known RV giants, with estimated effective temperatures of ~100-600 K and masses between 0.3 and 20 MJupiter. In this regime, both methane and clouds will have the largest effects on the observed spectra. Our retrieval code is the first to include cloud properties in the core set of parameters, along with methane abundance and surface gravity. We consider three possible cloud structure scenarios, with 0, 1 or 2 cloud layers, respectively. The best-fit parameters for a given model are determined using a Monte Carlo Markov Chain ensemble sampler, and the most favored cloud structure is chosen by calculating the Bayes factors between different models. We present the performance of our retrieval technique applied to a set of representative model spectra, covering a SNR range form 5 to 20 and including possible noise correlations over a 25 or 100 nanometer scale. Further, we apply the technique to more realistic cases, namely simulated observations of Jupiter, Saturn, Uranus, and the gas-giant HD99492c. In each case, we determine the confidence levels associated with the methane and cloud detections, as a function of SNR and noise properties.

40 CFR 86.1710-99 - Fleet average non-methane organic gas exhaust emission standards for light-duty vehicles and...

Code of Federal Regulations, 2012 CFR

2012-07-01

... 40 Protection of Environment 20 2012-07-01 2012-07-01 false Fleet average non-methane organic gas....1710-99 Fleet average non-methane organic gas exhaust emission standards for light-duty vehicles and... follows: Table R99-15—Fleet Average Non-Methane Organic Gas Standards (g/mi) for Light-Duty Vehicles and...

40 CFR 86.1710-99 - Fleet average non-methane organic gas exhaust emission standards for light-duty vehicles and...

Code of Federal Regulations, 2011 CFR

2011-07-01

... 40 Protection of Environment 19 2011-07-01 2011-07-01 false Fleet average non-methane organic gas....1710-99 Fleet average non-methane organic gas exhaust emission standards for light-duty vehicles and... follows: Table R99-15—Fleet Average Non-Methane Organic Gas Standards (g/mi) for Light-Duty Vehicles and...

40 CFR 86.1710-99 - Fleet average non-methane organic gas exhaust emission standards for light-duty vehicles and...

Code of Federal Regulations, 2013 CFR

2013-07-01

... 40 Protection of Environment 20 2013-07-01 2013-07-01 false Fleet average non-methane organic gas....1710-99 Fleet average non-methane organic gas exhaust emission standards for light-duty vehicles and... follows: Table R99-15—Fleet Average Non-Methane Organic Gas Standards (g/mi) for Light-Duty Vehicles and...

40 CFR 86.1710-99 - Fleet average non-methane organic gas exhaust emission standards for light-duty vehicles and...

Code of Federal Regulations, 2010 CFR

2010-07-01

... 40 Protection of Environment 19 2010-07-01 2010-07-01 false Fleet average non-methane organic gas....1710-99 Fleet average non-methane organic gas exhaust emission standards for light-duty vehicles and... follows: Table R99-15—Fleet Average Non-Methane Organic Gas Standards (g/mi) for Light-Duty Vehicles and...

Biodegradation of petroleum hydrocarbons in estuarine sediments: metal influence.

PubMed

Almeida, Raquel; Mucha, Ana P; Teixeira, Catarina; Bordalo, Adriano A; Almeida, C Marisa R

2013-02-01

In this work, the potential effect of metals, such as Cd, Cu and Pb, on the biodegradation of petroleum hydrocarbons in estuarine sediments was investigated under laboratory conditions. Sandy and muddy non-vegetated sediments were collected in the Lima River estuary (NW Portugal) and spiked with crude oil and each of the metals. Spiked sediments were left in the dark under constant shaking for 15 days, after which crude oil biodegradation was evaluated. To estimate microbial abundance, total cell counts were obtained by DAPI staining and microbial community structure was characterized by ARISA. Culturable hydrocarbon degraders were determined using a modified most probable number protocol. Total petroleum hydrocarbons concentrations were analysed by Fourier Transform Infrared Spectroscopy after their extraction by sonication, and metal contents were determined by atomic absorption spectrometry. The results obtained showed that microbial communities had the potential to degrade petroleum hydrocarbons, with a maximum of 32 % degradation obtained for sandy sediments. Both crude oil and metals changed the microbial community structure, being the higher effect observed for Cu. Also, among the studied metals, only Cu displayed measurable deleterious effect on the hydrocarbons degradation process, as shown by a decrease in the hydrocarbon degrading microorganisms abundance and in the hydrocarbon degradation rates. Both degradation potential and metal influence varied with sediment characteristics probably due to differences in contaminant bioavailability, a feature that should be taken into account in developing bioremediation strategies for co-contaminated estuarine sites.

Secondary migration and leakage of methane from a major tight-gas system

PubMed Central

Wood, James M.; Sanei, Hamed

2016-01-01

Tight-gas and shale-gas systems can undergo significant depressurization during basin uplift and erosion of overburden due primarily to the natural leakage of hydrocarbon fluids. To date, geologic factors governing hydrocarbon leakage from such systems are poorly documented and understood. Here we show, in a study of produced natural gas from 1,907 petroleum wells drilled into a Triassic tight-gas system in western Canada, that hydrocarbon fluid loss is focused along distinct curvilinear pathways controlled by stratigraphic trends with superior matrix permeability and likely also structural trends with enhanced fracture permeability. Natural gas along these pathways is preferentially enriched in methane because of selective secondary migration and phase separation processes. The leakage and secondary migration of thermogenic methane to surficial strata is part of an ongoing carbon cycle in which organic carbon in the deep sedimentary basin transforms into methane, and ultimately reaches the near-surface groundwater and atmosphere. PMID:27874012

Retrievals of abundances of hydrocarbon and nitrile species in Titan’s upper atmosphere

NASA Astrophysics Data System (ADS)

Yung, Yuk; Fan, Siteng; Shemansky, D. E.; Li, Cheng; Gao, Peter

2017-10-01

We develop an innovative retrieval method for Titan occultation measurements by the Cassini UVIS experiment. The T35 occultation is analyzed to illustrate the methodology. A significant number of occultations observed using the UVIS spectrographs show loss of pointing control required for correction of the spectral vectors. Consequently, only three stellar occultations have been analyzed to date. We use the Markov Chain Monte-Carlo (MCMC) method to retrieve the abundances or upper limits of thirteen hydrocarbon and nitrile species (N2, CH4, C2H2, C2H4, C2H6, HCN, C4H2, C6N2, C6H6, tholin, HC3N, C2N2, NH3) along with the pointing error using the Cassini/UVIS simulator. These numbers are derived for the fast T35 occultation, which has never been analyzed because of large pointing errors. Uncertainty in the retrievals is determined using an intrinsic fitting probability distribution function. The Caltech/JPL photochemical and kinetics model, KINETICS, is used to calculate the atmospheric aforementioned species. Comparisons between model and observations reveal gaps in our current understanding of the chemical kinetics of hydrocarbons and nitrile species, especially for C6H6.

2013 Survey of Non-Starch Ethanol and Renewable Hydrocarbon Biofuels Producers

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

Schwab, Amy; Geiger, Jesse; Lewis, John

In order to understand the status of the industry for non-starch ethanol and renewable hydrocarbon biofuels as of the end of calendar year 2013, the National Renewable Energy Laboratory (NREL) conducted the first of what is anticipated to be an annual survey of U.S. non-starch ethanol and renewable hydrocarbon biofuels producers. This report presents the results of this initial survey and describes the survey methodology. Subsequent surveys will report on the progress over time of the development of these facilities and companies.

40 CFR 86.1342-94 - Calculations; exhaust emissions.

Code of Federal Regulations, 2012 CFR

2012-07-01

..., if appropriate, the weighted mass total hydrocarbon equivalent, formaldehyde, or non-methane... see § 86.1342-90. (b)(8) Non-methane hydrocarbon mass: NMHCmass = Vmix × DensityNMHC × (NMHCconc/1,000... non-methane hydrocarbon, is 1.1771(12.011 + H/C (1.008)) g/ft3-carbon atom (0.04157(12.011 + H/C (1...

Formation of hydrocarbons under upper mantle conditions: experimental view

NASA Astrophysics Data System (ADS)

Kolesnikov, Anton; Kutcherov, Vladimir G.

2010-05-01

Main postulates of the theory of abiogenic abyssal origin of petroleum have been developed in the last 50 years in Russia and Ukraine. According to this theory, hydrocarbon compounds were generated in the mantle and migrated through the deep faults into the Earth's crust. There they formed oil and gas deposits in any kinds of rocks and in any kind of their structural positions. Until recently the main obstacle to accept the theory was the lack of reliable and reproducible experimental data confirming the possibility of the synthesis of complex hydrocarbon systems under the mantle conditions. The results received in the last decade by different groups of researchers from Russia, U.S.A. and China have confirmed the possibility of generation of hydrocarbons from inorganic materials, highly distributed in the Earth's mantle, under thermobaric conditions of 70-250 km: 2 - 5 GPa and 1000-1500 K. Experiments made in the CONAC chamber at pressures of 3-5 GPa and temperatures of 1000-1500 K by Kutcherov et al. [1, 2] have demonstrated that the mixtures of hydrocarbons with composition similar to natural hydrocarbon systems have been received as a result of chemical reactions between CaCO3, FeO and H2O. Methane formation from the same compounds was registered after heating up to 600-1500 K at pressures of 4-11 GPa in diamond anvil cells [4, 5, 6]. Influence of oxidation state of carbon donor and cooling rate of the fluid synthesized at high pressure were studied using different types of high pressure equipments. It was shown that composition of the final hydrocarbon mixture depends on these parameters. Experimental investigations of transformation of methane and ethane at 2-5 GPa and 1000-1500 K [3] confirmed thermodynamic stability of heavy hydrocarbons in the upper mantle and showed the possibility of hydrocarbon chain growth even at oxidative environment. For development of the theory of abiogenic abyssal origin of petroleum it is necessary to arrange a set of new

Steps toward identifying a biogeochemical signal in non-equilibrium methane clumped isotope measurements

NASA Astrophysics Data System (ADS)

Douglas, P. M.; Eiler, J. M.; Sessions, A. L.; Dawson, K.; Walter Anthony, K. M.; Smith, D. A.; Lloyd, M. K.; Yanay, E.

2016-12-01

Microbially produced methane is a globally important greenhouse gas, energy source, and biological substrate. Methane clumped isotope measurements have recently been developed as a new analytical tool for understanding the source of methane in different environments. When methane forms in isotopic equilibrium clumped isotope values are determined by formation temperature, but in many cases microbial methane clumped isotope values deviate strongly from expected equilibrium values. Indeed, we observe a very wide range of clumped isotope values in microbial methane, which are likely strongly influenced by kinetic isotope effects, but thus far the biological and environmental parameters controlling this variability are not understood. We will present data from both culture experiments and natural environments to explore patterns of variability in non-equilibrium clumped isotope values on temporal and spatial scales. In methanogen batch cultures sampled at different time points along a growth curve we observe significant variability in clumped isotope values, with values decreasing from early to late exponential growth. Clumped isotope values then increase during stationary growth. This result is consistent with previous work suggesting that differences in the reversibility of methanogenesis related to metabolic rates control non-equilibrium clumped isotope values. Within single lakes in Alaska and Sweden we observe substantial variability in clumped isotope values on the order of 5‰. Lower clumped isotope values are associated with larger 2H isotopic fractionation between water and methane, which is also consistent with a kinetic isotope effect determined by the reversibility of methanogenesis. Finally, we analyzed a time-series clumped isotope compositions of methane emitted from two seeps in an Alaskan lake over several months. Temporal variability in these seeps is on the order of 2‰, which is much less than the observed spatial variability within the lake

An Aerial ``Sniffer Dog'' for Methane

NASA Astrophysics Data System (ADS)

Nathan, Brian; Schaefer, Dave; Zondlo, Mark; Khan, Amir; Lary, David

2012-10-01

The Earth's surface and its atmosphere maintain a ``Radiation Balance.'' Any factor which influences this balance is labeled as a mechanism of ``Radiative Forcing'' (RF). Greenhouse Gas (GHG) concentrations are among the most important forcing mechanisms. Methane, the second-most-abundant noncondensing greenhouse gas, is over 25 times more effective per molecule at radiating heat than the most abundant, Carbon Dioxide. Methane is also the principal component of Natural Gas, and gas leaks can cause explosions. Additionally, massive quantities of methane reside (in the form of natural gas) in underground shale basins. Recent technological advancements--specifically the combination of horizontal drilling and hydraulic fracturing--have allowed drillers access to portions of these ``plays'' which were previously unreachable, leading to an exponential growth in the shale gas industry. Presently, very little is known about the amount of methane which escapes into the global atmosphere from the extraction process. By using remote-controlled robotic helicopters equipped with specially developed trace gas laser sensors, we can get a 3-D profile of where and how methane is being released into the global atmosphere.

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

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

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

Hydrocarbon seeps in petroliferous basins in China: A first inventory

NASA Astrophysics Data System (ADS)

Zheng, Guodong; Xu, Wang; Etiope, Giuseppe; Ma, Xiangxian; Liang, Shouyun; Fan, Qiaohui; Sajjad, Wasim; Li, Yang

2018-01-01

Natural hydrocarbon seepage is a widespread phenomenon in sedimentary basins, with important implications in petroleum exploration and emission of greenhouse gases to the atmosphere. China has vast petroleum (oil and gas) bearing sedimentary basins, but hydrocarbon seepage has rarely been the object of systematic studies and measurements. Based on the available Chinese literature, we report a first inventory of 932 hydrocarbon seeps or seepage zones (710 onshore seeps and 222 offshore seeps), including 81 mud volcanoes, 449 oil seeps, 215 gas seeps, and 187 solid seeps (bitumen outcrops). The seeps are located within the main 20 Mesozoic-Cenozoic petroliferous sedimentary basins, especially along the marginal, regional and local faults. The type of manifestations (oil, gas or mud volcano) reflects the type and maturity of the subsurface petroleum system and the sedimentary conditions of the basin. Oil seeps are particularly abundant in the Junggar Basin. Gas seeps mostly developed in the Lunpola Basin, in smaller basins of the eastern Guizhou and Yunnan provinces, onshore Taiwan and in the offshore Yinggehai Basin. Mud volcanoes developed in basins (Junggar, Qaidam, Qiangtang, onshore and offshore Taiwan) that experienced rapid sedimentation, which induced gravitative instability of shales and diapirism. In comparison to available global onshore seep data-bases, China results to be the country with the highest number of seeps in the world. The massive gas seepage in China could represent a considerable natural source of methane to the atmosphere, and a key process that may drive future hydrocarbon exploration.

Hydrothermal synthesis of hydrocarbons at low temperature. Implications for sustaining a biosphere in Europa

NASA Astrophysics Data System (ADS)

Navarro-Gonzalez, Rafael; Montoya, Lilia; Davis, Wanda; McKay, Chris

Observational evidence from Earth-borne systems and space missions as well as theoretical arguments suggest that Jupiter's satellite Europa could be geologically active today and may possess an ocean of liquid water of about 100 km deep underneath the icy surface about 10 km thickness. The existence of an aqueous ocean is an important requirement for life, as we know it. However, a biosphere also depends of an adequate energy source to drive the most fundamental biological processes such as metabolism, growth, reproduction, etc. Methanogenesis associated with hydrothermal vents may potentially drive a biosphere in an European ocean. We report here on the production of a large variety of hydrocarbons in hydrothermal systems at low temperatures (150° C). The chemical composition of the hydrothermal vent gases was derived from a thermochemical model that assumes that Europa had a cometary (solar, less H) abundance at high temperatures characteristic of a vent. Specifically the following gas mixture was used: 45% CO2 , 45% CH4, and 10 % N2 . A 500 ml stainless steel reactor was filled with 200 ml triply distilled water and the gas mixture at 1 bar at 25° C. In some experiments 3 g of pyrite were added into the reaction vessel. The system was heated for 24 hrs in the temperature range from 100 to 375° C. At the completion of the experiment, the reaction was quenched to 25° C and the gas mixture was analyzed by GC-FTIR-MS techniques. In the absence of pyrite, methane is oxidized to carbon dioxide with the possible production of hydrogen. In contrast in the presence of pyrite, methane is converted into a suite of hydrocarbons from C2 to C7 containing all possible isomers. The production of these compounds was found at temperatures as low as 150° C. In order to get a better understanding of the chemical mechanism involved in the synthesis of hydrocarbons and explore the effect on the initial oxidation state of the carbon used, we performed additional experiments in

Methane as a biomarker in the search for extraterrestrial life: Lessons learned from Mars analog hypersaline environments

NASA Astrophysics Data System (ADS)

Bebout, B.; Tazaz, A.; Kelley, C. A.; Poole, J. A.; Davila, A.; Chanton, J.

2010-12-01

Methane released from discrete regions on Mars, together with previous reports of methane determined with ground-based telescopes, has revived the possibility of past or even extant life near the surface on Mars, since 90% of the methane on Earth has a biological origin. This intriguing possibility is supported by the abundant evidence of large bodies of liquid water, and therefore of conditions conducive to the origin of life, early in the planet's history. The detection and analysis of methane is at the core of NASA’s strategies to search for life in the solar system, and on extrasolar planets. Because methane is also produced abiotically, it is important to generate criteria to unambiguously assess biogenicity. The stable carbon and hydrogen isotopic signature of methane, as well as its ratio to other low molecular weight hydrocarbons (the methane/(ethane + propane) ratio: C1/(C2 + C3)), has been suggested to be diagnostic for biogenic methane. We report measurements of the concentrations and stable isotopic signature of methane from hypersaline environments. We focus on hypersaline environments because spectrometers orbiting Mars have detected widespread chloride bearing deposits resembling salt flats. Other evaporitic minerals, e.g., sulfates, are also abundant in several regions, including those studied by the Mars Exploration Rovers. The presence of evaporitic minerals, together with the known evolution of the Martian climate, from warmer and wetter to cold and hyper-arid, suggest that evaporitic and hypersaline environments were common in the past. Hypersaline environments examined to date include salt ponds located in Baja California, the San Francisco Bay, and the Atacama Desert. Methane was found in gas produced both in the sediments, and in gypsum- and halite-hosted (endolithic) microbial communities. Maximum methane concentrations were as high as 40% by volume. The methane carbon isotopic (δ13C) composition showed a wide range of values, from about

Methane oxidation coupled to oxygenic photosynthesis in anoxic waters

PubMed Central

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

2015-01-01

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

METABOLISM OF CHLORINATED METHANES, ETHANES, AND ETHYLENES BY A MIXED BACTERIAL CUTLURE GROWING ON METHANE

EPA Science Inventory

Soil was taken from the top 10 cm of a soil column that removed halogenated aliphatic hydrocarbons in the presence of natural gas. This soil was used as an enrichment inoculum to determine that the removals seen in the soil column were in fact of a microbiological nature. Methane...

Optoelectronics sensors of hydrocarbons based on NDIR technique

NASA Astrophysics Data System (ADS)

Prokopiuk, Artur

2017-08-01

Saturated hydrocarbons are mainly nontoxic, but as extremely flammable gases forming explosive mixtures with air. The Lower Explosive Level (LEL) for methane is 4.4%, which is very dangerous in the mining industry. Methane is also an asphyxiant gas causing coma or death. Therefore, continuous monitoring of the hydrocarbons concentration is very important. Optoelectronic methods are very attractive for this application, especially nondispersive infrared (NDIR) technique. It enables a direct, fast, and selective measurement of different gas concentrations. NDIR sensors have many advantages, which make them very promising for use as hydrocarbon detectors. Despite a lot of benefits, common used NDIR sensors have some disadvantages. They need periodic calibration and have limited detection range, from 100ppm. These parameters can be improved thanks to modernization detection scheme and use of newest IR sources and detectors. During Analyses selected IR sources and detectors were taken into account. Absorption spectra of analyzed hyrdrocarbons were studied to minimize impact interfering gases like carbon dioxide and water.

The bulk isotopic composition of hydrocarbons in subaerial volcanic-hydrothermal emissions from different tectonic settings

NASA Astrophysics Data System (ADS)

Fiebig, J.; Tassi, F.; Vaselli, O.; Viveiros, M. F.; Silva, C.; Lopez, T. M.; D'Alessandro, W.; Stefansson, A.

2015-12-01

Assuming that methane and its higher chain homologues derive from a common source, carbon isotope patterns have been applied as a criterion to identify occurrences of abiogenic hydrocarbons. Based on these, it has been postulated that abiogenic hydrocarbon production occurs within several (ultra)mafic environments. More evolved volcanic-hydrothermal systems may also provide all the prerequisites necessary for abiogenic hydrocarbon production, such as availability of inorganic CO2, hydrogen and heat. We have investigated the chemical and isotopic composition of n-alkanes contained within subaerial hydrothermal discharges emitted from a range of hot spot, subduction and rift-related volcanoes to determine the origin of hydrocarbons in these systems. Amongst these are Nisyros (Greece), Vesuvio, Campi Flegrei, Ischia, Pantelleria and Vulcano (all Italy), Mt. Mageik and Trident (USA), Copahue (Argentina), Teide (Spain), Furnas and Fogo (Portugal). The carbon isotopic composition of methane emitted from these sites varies from -65 to -8‰ , whereas δ13C of ethane and propane exhibit a much narrower variation from -17‰ to -31‰. Methane that occurs most enriched in 13C is also characterized by relatively positive δD values ranging up to -80‰. Carbon isotope reversals between methane and ethane are only observed for locations exhibiting δ13C-CH4 values > -20‰, such as Teide, Pantelleria, Trident and Furnas. At Furnas, δ13C-CH4 varies by 50‰ within a relatively short distance of <50m between two vents, whereas δ13C-C2H6 varies by less than 2‰ only. For some of the investigated locations apparent carbon isotopic temperatures between methane and CO2 are in agreement with those derived from gas concentration geothermometers. At these locations methane, however seems to be in disequilibrium with ethane and propane. These findings imply that methane on the one hand and the C2+ hydrocarbons on the other hand often might derive from distinct sources.

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

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

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

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

76 FR 68381 - Approval and Promulgation of Air Quality Implementation Plans; Pennsylvania; Pennsylvania Clean...

Federal Register 2010, 2011, 2012, 2013, 2014

2011-11-04

... period within which vehicle manufacturers could comply with the program's fleet average non-methane... year meets the specified phase-in requirements according to the fleet average non- methane hydrocarbon requirement for that year. The fleet average non- methane hydrocarbon emission limits become progressively...

Subarctic Lake Sediment Microbial Community Contributions to Methane Emission Patterns

NASA Astrophysics Data System (ADS)

Emerson, J. B.; Varner, R. K.; Parks, D.; Wik, M.; Neumann, R.; Johnson, J. E.; Singleton, C. M.; Woodcroft, B. J.; Tollerson, R., II; Owusu-Dommey, A.; Binder, M.; Freitas, N. L.; Crill, P. M.; Saleska, S. R.; Tyson, G. W.; Rich, V. I.

2017-12-01

Northern post-glacial lakes have recently been identified as a significant and increasing source of carbon to the atmosphere, largely through ebullition (bubbling) of microbially produced methane from the sediments. Ebullitive methane flux has been shown to correlate significantly with sediment surface temperatures, suggesting that solar radiation is the primary driver of methane emissions from these lakes. However, the slope of this relationship (i.e., the extent to which increasing temperature increases ebullitive methane emissions) differs spatially, both within and among lakes. As microbes are responsible for both methane generation and removal in lakes, we hypothesized that microbial communities—previously uncharacterized in post-glacial lake sediments—could be contributing to spatiotemporal differences in methane emission responses to temperature. We compared methane emission data with sediment microbial (metagenomic and amplicon), isotopic, and geochemical characterizations across two post-glacial lakes in Northern Sweden. With increasing temperatures, the increase in methane emissions was greater in lake middles (deeper water) than lake edges (shallower water), consistent with higher abundances of methanogens in sediments from lake middles than edges, along with significant differences in microbial community composition between these regions. Using sparse partial least squares statistical modeling, microbial abundances (including the abundances of methane-cycling microorganisms and of reconstructed population genomes, e.g., from Planctomycetes, Thermoplasmatales, and Candidate Phylum Aminicenantes) were better predictors of porewater methane concentrations than abiotic variables. These results suggest that, although temperature controls methane emissions, microbial community composition and function may drive the rate and magnitude of this temperature response in subarctic post-glacial lakes.

Microbial diversity and dynamics during methane production from municipal solid waste

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

Bareither, Christopher A., E-mail: christopher.bareither@colostate.edu; Geological Engineering, University of Wisconsin-Madison, Madison, WI 53706; Wolfe, Georgia L., E-mail: gwolfe@wisc.edu

2013-10-15

Highlights: ► Similar bacterial communities developed following different start-up operation. ► Total methanogens in leachate during the decelerated methane phase reflected overall methane yield. ► Created correlations between methanogens, methane yield, and available substrate. ► Predominant bacteria identified with syntrophic polysaccharide degraders. ► Hydrogenotrophic methanogens were dominant in the methane generation process. - Abstract: The objectives of this study were to characterize development of bacterial and archaeal populations during biodegradation of municipal solid waste (MSW) and to link specific methanogens to methane generation. Experiments were conducted in three 0.61-m-diameter by 0.90-m-tall laboratory reactors to simulate MSW bioreactor landfills. Pyrosequencing ofmore » 16S rRNA genes was used to characterize microbial communities in both leachate and solid waste. Microbial assemblages in effluent leachate were similar between reactors during peak methane generation. Specific groups within the Bacteroidetes and Thermatogae phyla were present in all samples and were particularly abundant during peak methane generation. Microbial communities were not similar in leachate and solid fractions assayed at the end of reactor operation; solid waste contained a more abundant bacterial community of cellulose-degrading organisms (e.g., Firmicutes). Specific methanogen populations were assessed using quantitative polymerase chain reaction. Methanomicrobiales, Methanosarcinaceae, and Methanobacteriales were the predominant methanogens in all reactors, with Methanomicrobiales consistently the most abundant. Methanogen growth phases coincided with accelerated methane production, and cumulative methane yield increased with increasing total methanogen abundance. The difference in methanogen populations and corresponding methane yield is attributed to different initial cellulose and hemicellulose contents of the MSW. Higher initial cellulose and

Molecular carbon isotopic evidence for the origin of geothermal hydrocarbons

NASA Technical Reports Server (NTRS)

Des Marais, D. J.; Donchin, J. H.; Nehring, N. L.; Truesdell, A. H.

1981-01-01

Isotopic measurements of individual geothermal hydrocarbons that are, as a group, of higher molecular weight than methane are reported. It is believed in light of this data that the principal source of hydrocarbons in four geothermal areas in western North America is the thermal decomposition of sedimentary or groundwater organic matter.

Aerobic microorganism for the degradation of chlorinated aliphatic hydrocarbons

DOEpatents

Fliermans, Carl B.

1989-01-01

A chlorinated aliphatic hydrocarbon-degrading microorganism, having American Type Culture Collection accession numbers ATCC 53570 and 53571, in a biologically pure culture aseptically collected from a deep subsurface habitat and enhanced, mineralizes trichloroethylene and tetrachloroethylene to HCl, H.sub.2 O and Co.sub.2 under aerobic conditions stimulated by methane, acetate, methanol, tryptone-yeast extract, propane and propane-methane.

Emissions of organic compounds from produced water ponds I: Characteristics and speciation.

PubMed

Lyman, Seth N; Mansfield, Marc L; Tran, Huy N Q; Evans, Jordan D; Jones, Colleen; O'Neil, Trevor; Bowers, Ric; Smith, Ann; Keslar, Cara

2018-04-01

We measured fluxes of methane, a suite of non-methane hydrocarbons (C2-C11), light alcohols, and carbon dioxide from oil and gas produced water storage and disposal ponds in Utah (Uinta Basin) and Wyoming (Upper Green River Basin) United States during 2013-2016. In this paper, we discuss the characteristics of produced water composition and air-water fluxes, with a focus on flux chamber measurements. In companion papers, we will (1) report on inverse modeling methods used to estimate emissions from produced water ponds, including comparisons with flux chamber measurements, and (2) discuss the development of mass transfer coefficients to estimate emissions and place emissions from produced water ponds in the context of all regional oil and gas-related emissions. Alcohols (made up mostly of methanol) were the most abundant organic compound group in produced water (91% of total volatile organic concentration, with upper and lower 95% confidence levels of 89 and 93%) but accounted for only 34% (28 to 41%) of total organic compound fluxes from produced water ponds. Non-methane hydrocarbons, which are much less water-soluble than methanol and less abundant in produced water, accounted for the majority of emitted organics. C6-C9 alkanes and aromatics dominated hydrocarbon fluxes, perhaps because lighter hydrocarbons had already volatilized from produced water prior to its arrival in storage or disposal ponds, while heavier hydrocarbons are less water soluble and less volatile. Fluxes of formaldehyde and other carbonyls were low (1% (1 to 2%) of total organic compound flux). The speciation and magnitude of fluxes varied strongly across the facilities measured and with the amount of time water had been exposed to the atmosphere. The presence or absence of ice also impacted fluxes. Copyright © 2017 Elsevier B.V. All rights reserved.

A search for interstellar CH3D: Limits to the methane abundance in Orion-KL

NASA Technical Reports Server (NTRS)

Womack, Maria; Ziurys, L. M.; Apponi, A. J.

1995-01-01

A search has been performed for interstellar CH3D via its J(K) = 1(0) - 0(0) transition at 230 GHz and its J(K) = 2(0) - l(0) and J(K) = 2(1) - 1(1) lines at 465 GHz using the NRAO 12 m and CSO 10 m telescopes towards Orion-KL. This search was done in conjunction with laboratory measurements of all three transitions of CH3D using mm/sub-mm direct absorption spectroscopy. The molecule was not detected down to a 3 sigma level of T(A) less than 0.05 K towards Orion, which suggests an upper limit to the CH3D column density of N less than 6 x 10(exp 18)/sq cm in the hot core region and a fractional abundance (with respect to H2) of less than 6 x 10(exp -6). These measurements suggest that the methane abundance in the Orion hot core is f less than 6 x 10-4, assuming D/H approximately 0.01. Such findings are in agreement with recent hot core chemical models, which suggest CH4/H2 approximately 10(exp -4).

Methane source identification in Boston, Massachusetts using isotopic and ethane measurements

NASA Astrophysics Data System (ADS)

Down, A.; Jackson, R. B.; Plata, D.; McKain, K.; Wofsy, S. C.; Rella, C.; Crosson, E.; Phillips, N. G.

2012-12-01

Methane has substantial greenhouse warming potential and is the principle component of natural gas. Fugitive natural gas emissions could be a significant source of methane to the atmosphere. However, the cumulative magnitude of natural gas leaks is not yet well constrained. We used a combination of point source measurements and ambient monitoring to characterize the methane sources in the Boston urban area. We developed distinct fingerprints for natural gas and multiple biogenic methane sources based on hydrocarbon concentration and isotopic composition. We combine these data with periodic measurements of atmospheric methane and ethane concentration to estimate the fractional contribution of natural gas and biogenic methane sources to the cumulative urban methane flux in Boston. These results are used to inform an inverse model of urban methane concentration and emissions.

40 CFR 86.1804-01 - Acronyms and abbreviations.

Code of Federal Regulations, 2012 CFR

2012-07-01

...—Nonmethane Hydrocarbons. NMHCE—Non-Methane Hydrocarbon Equivalent. NMOG—Non-methane organic gases. NO—nitric....—Degree(s). DNPH—2,4-dinitrophenylhydrazine. EDV—Emission Data Vehicle. EP—End point. ETW—Equivalent test...—dispensed fuel temperature. THC—Total Hydrocarbons. THCE—Total Hydrocarbon Equivalent. TLEV—Transitional Low...

40 CFR 86.1804-01 - Acronyms and abbreviations.

Code of Federal Regulations, 2014 CFR

2014-07-01

...—Nonmethane Hydrocarbons. NMHCE—Non-Methane Hydrocarbon Equivalent. NMOG—Non-methane organic gases. NO—nitric....—Degree(s). DNPH—2,4-dinitrophenylhydrazine. EDV—Emission Data Vehicle. EP—End point. ETW—Equivalent test...—dispensed fuel temperature. THC—Total Hydrocarbons. THCE—Total Hydrocarbon Equivalent. TLEV—Transitional Low...

Emissions of organic carbon and methane from petroleum and dairy operations in California's San Joaquin Valley

NASA Astrophysics Data System (ADS)

Gentner, D. R.; Ford, T. B.; Guha, A.; Boulanger, K.; Brioude, J.; Angevine, W. M.; de Gouw, J. A.; Warneke, C.; Gilman, J. B.; Ryerson, T. B.; Peischl, J.; Meinardi, S.; Blake, D. R.; Atlas, E.; Lonneman, W. A.; Kleindienst, T. E.; Beaver, M. R.; St. Clair, J. M.; Wennberg, P. O.; VandenBoer, T. C.; Markovic, M. Z.; Murphy, J. G.; Harley, R. A.; Goldstein, A. H.

2014-05-01

Petroleum and dairy operations are prominent sources of gas-phase organic compounds in California's San Joaquin Valley. It is essential to understand the emissions and air quality impacts of these relatively understudied sources, especially for oil/gas operations in light of increasing US production. Ground site measurements in Bakersfield and regional aircraft measurements of reactive gas-phase organic compounds and methane were part of the CalNex (California Research at the Nexus of Air Quality and Climate Change) project to determine the sources contributing to regional gas-phase organic carbon emissions. Using a combination of near-source and downwind data, we assess the composition and magnitude of emissions, and provide average source profiles. To examine the spatial distribution of emissions in the San Joaquin Valley, we developed a statistical modeling method using ground-based data and the FLEXPART-WRF transport and meteorological model. We present evidence for large sources of paraffinic hydrocarbons from petroleum operations and oxygenated compounds from dairy (and other cattle) operations. In addition to the small straight-chain alkanes typically associated with petroleum operations, we observed a wide range of branched and cyclic alkanes, most of which have limited previous in situ measurements or characterization in petroleum operation emissions. Observed dairy emissions were dominated by ethanol, methanol, acetic acid, and methane. Dairy operations were responsible for the vast majority of methane emissions in the San Joaquin Valley; observations of methane were well correlated with non-vehicular ethanol, and multiple assessments of the spatial distribution of emissions in the San Joaquin Valley highlight the dominance of dairy operations for methane emissions. The petroleum operations source profile was developed using the composition of non-methane hydrocarbons in unrefined natural gas associated with crude oil. The observed source profile is

Catalytic cracking of non-edible sunflower oil over ZSM-5 for hydrocarbon bio-jet fuel.

PubMed

Zhao, Xianhui; Wei, Lin; Julson, James; Qiao, Qiquan; Dubey, Ashish; Anderson, Gary

2015-03-25

Non-edible sunflower oils that were extracted from sunflower residual wastes were catalytically cracked over a ZSM-5 catalyst in a fixed-bed reactor at three different reaction temperatures: 450°C, 500°C and 550°C. The catalyst was characterized using XRD, FT-IR, BET and SEM. Characterizations of the upgraded sunflower oils, hydrocarbon fuels, distillation residues and non-condensable gases were carried out. The effect of the reaction temperature on the yield and quality of liquid products was discussed. The results showed that the reaction temperature affected the hydrocarbon fuel yield but had a minor influence on its properties. The highest conversion efficiency from sunflower oils to hydrocarbon fuels was 30.1%, which was obtained at 550°C. The reaction temperature affected the component content of the non-condensable gases. The non-condensable gases generated at 550°C contained the highest content of light hydrocarbons (C1-C5), CO, CO2 and H2. Compared to raw sunflower oils, the properties of hydrocarbon fuels including the dynamic viscosity, pH, moisture content, density, oxygen content and heating value were improved. Copyright © 2015 Elsevier B.V. All rights reserved.

Volatile non-terpenoid hydrocarbons from Ligusticum grayi roots

USDA-ARS?s Scientific Manuscript database

The root essential oil of Ligusticum grayi Coult. & Rose (Apiaceae) contains three volatile non-terpenoid hydrocarbons: the known C11 compound viridene, whose structure is hereby corrected to 1-[(2Z)-pent-2-en-1-yl]cyclohexa-1,3-diene; and the heretofore unreported C10 compounds 1-[(2Z)-but-2-en-1-y...

Raney Ni-Sn catalyst for H2 production from biomass-derived hydrocarbons.

PubMed

Huber, G W; Shabaker, J W; Dumesic, J A

2003-06-27

Hydrogen (H2) was produced by aqueous-phase reforming of biomass-derived oxygenated hydrocarbons at temperatures near 500 kelvin over a tin-promoted Raney-nickel catalyst. The performance of this non-precious metal catalyst compares favorably with that of platinum-based catalysts for production of hydrogen from ethylene glycol, glycerol, and sorbitol. The addition of tin to nickel decreases the rate of methane formation from C-O bond cleavage while maintaining the high rates of C-C bond cleavage required for hydrogen formation.

Apparatus for hydrocarbon extraction

DOEpatents

Bohnert, George W.; Verhulst, Galen G.

2013-03-19

Systems and methods for hydrocarbon extraction from hydrocarbon-containing material. Such systems and methods relate to extracting hydrocarbon from hydrocarbon-containing material employing a non-aqueous extractant. Additionally, such systems and methods relate to recovering and reusing non-aqueous extractant employed for extracting hydrocarbon from hydrocarbon-containing material.

Hydrocarbon gas in sediment of the Southern Pacific Ocean

USGS Publications Warehouse

Kvenvolden, K.A.

1988-01-01

Methane, ethane, ethene, propane, and propene are common hydrocarbon gases in near-surface sediment from offshore areas in the southern Pacific Ocean near Papua New Guinea, the Solomon Islands, Vanuatu, Tonga, New Zealand, and Antarctica. Sea floor sites for sampling of sediment were selected on the basis of anomalies in marine seismic records, and the samples were intentionally biased toward finding possible thermogenic hydrocarbon gases. In none of the areas, however, were thermogenic hydrocarbons clearly identified. The hydrocarbon gases that were found appear to be mainly the products of in situ microbial processes. ?? 1988 Springer-Verlag New York Inc.

Non-solar noble gas abundances in the atmosphere of Jupiter

NASA Technical Reports Server (NTRS)

Lunine, Jonathan I.; Stevenson, David J.

1986-01-01

The thermodynamic stability of clathrate hydrate is calculated to predict the formation conditions corresponding to a range of solar system parameters. The calculations were performed using the statistical mechanical theory developed by van der Waals and Platteeuw (1959) and existing experimental data concerning clathrate hydrate and its components. Dissociation pressures and partition functions (Langmuir constants) are predicted at low pressure for CO clathrate (hydrate) using the properties of chemicals similar to CO. It is argued that nonsolar but well constrained noble gas abundances may be measurable by the Galileo spacecraft in the Jovian atmosphere if the observed carbon enhancement is due to bombardment of the atmosphere by clathrate-bearing planetesimals sometime after planetary formation. The noble gas abundances of the Jovian satellite Titan are predicted, assuming that most of the methane in Titan is accreted as clathrate. It is suggested that under thermodynamically appropriate conditions, complete clathration of water ice could have occurred in high-pressure nebulas around giant planets, but probably not in the outer solar nebula. The stability of clathrate in other pressure ranges is also discussed.

When Can Species Abundance Data Reveal Non-neutrality?

PubMed Central

Al Hammal, Omar; Alonso, David; Etienne, Rampal S.; Cornell, Stephen J.

2015-01-01

Species abundance distributions (SAD) are probably ecology’s most well-known empirical pattern, and over the last decades many models have been proposed to explain their shape. There is no consensus over which model is correct, because the degree to which different processes can be discerned from SAD patterns has not yet been rigorously quantified. We present a power calculation to quantify our ability to detect deviations from neutrality using species abundance data. We study non-neutral stochastic community models, and show that the presence of non-neutral processes is detectable if sample size is large enough and/or the amplitude of the effect is strong enough. Our framework can be used for any candidate community model that can be simulated on a computer, and determines both the sampling effort required to distinguish between alternative processes, and a range for the strength of non-neutral processes in communities whose patterns are statistically consistent with neutral theory. We find that even data sets of the scale of the 50 Ha forest plot on Barro Colorado Island, Panama, are unlikely to be large enough to detect deviations from neutrality caused by competitive interactions alone, though the presence of multiple non-neutral processes with contrasting effects on abundance distributions may be detectable. PMID:25793889

The rumen microbial metagenome associated with high methane production in cattle.

PubMed

Wallace, R John; Rooke, John A; McKain, Nest; Duthie, Carol-Anne; Hyslop, Jimmy J; Ross, David W; Waterhouse, Anthony; Watson, Mick; Roehe, Rainer

2015-10-23

Methane represents 16 % of total anthropogenic greenhouse gas emissions. It has been estimated that ruminant livestock produce ca. 29 % of this methane. As individual animals produce consistently different quantities of methane, understanding the basis for these differences may lead to new opportunities for mitigating ruminal methane emissions. Metagenomics is a powerful new tool for understanding the composition and function of complex microbial communities. Here we have applied metagenomics to the rumen microbial community to identify differences in the microbiota and metagenome that lead to high- and low-methane-emitting cattle phenotypes. Four pairs of beef cattle were selected for extreme high and low methane emissions from 72 animals, matched for breed (Aberdeen-Angus or Limousin cross) and diet (high or medium concentrate). Community analysis was carried out by qPCR of 16S and 18S rRNA genes and by alignment of Illumina HiSeq reads to the GREENGENES database. Total genomic reads were aligned to the KEGG genes databasefor functional analysis. Deep sequencing produced on average 11.3 Gb per sample. 16S rRNA gene abundances indicated that archaea, predominantly Methanobrevibacter, were 2.5× more numerous (P = 0.026) in high emitters, whereas among bacteria Proteobacteria, predominantly Succinivibrionaceae, were 4-fold less abundant (2.7 vs. 11.2 %; P = 0.002). KEGG analysis revealed that archaeal genes leading directly or indirectly to methane production were 2.7-fold more abundant in high emitters. Genes less abundant in high emitters included acetate kinase, electron transport complex proteins RnfC and RnfD and glucose-6-phosphate isomerase. Sequence data were assembled de novo and over 1.5 million proteins were annotated on the subsequent metagenome scaffolds. Less than half of the predicted genes matched matched a domain within Pfam. Amongst 2774 identified proteins of the 20 KEGG orthologues that correlated with methane emissions, only 16 showed

Latitudinal variations in Titan's methane and haze from Cassini VIMS observations

USGS Publications Warehouse

Penteado, P.F.; Griffith, C.A.; Tomasko, M.G.; Engel, S.; See, C.; Doose, L.; Baines, K.H.; Brown, R.H.; Buratti, B.J.; Clark, R.; Nicholson, P.; Sotin, Christophe

2010-01-01

We analyze observations taken with Cassini's Visual and Infrared Mapping Spectrometer (VIMS), to determine the current methane and haze latitudinal distribution between 60??S and 40??N. The methane variation was measured primarily from its absorption band at 0.61 ??m, which is optically thin enough to be sensitive to the methane abundance at 20-50 km altitude. Haze characteristics were determined from Titan's 0.4-1.6 ??m spectra, which sample Titan's atmosphere from the surface to 200 km altitude. Radiative transfer models based on the haze properties and methane absorption profiles at the Huygens site reproduced the observed VIMS spectra and allowed us to retrieve latitude variations in the methane abundance and haze. We find the haze variations can be reproduced by varying only the density and single scattering albedo above 80 km altitude. There is an ambiguity between methane abundance and haze optical depth, because higher haze optical depth causes shallower methane bands; thus a family of solutions is allowed by the data. We find that haze variations alone, with a constant methane abundance, can reproduce the spatial variation in the methane bands if the haze density increases by 60% between 20??S and 10??S (roughly the sub-solar latitude) and single scattering absorption increases by 20% between 60??S and 40??N. On the other hand, a higher abundance of methane between 20 and 50 km in the summer hemisphere, as much as two times that of the winter hemisphere, is also possible, if the haze variations are minimized. The range of possible methane variations between 27??S and 19??N is consistent with condensation as a result of temperature variations of 0-1.5 K at 20-30 km. Our analysis indicates that the latitudinal variations in Titan's visible to near-IR albedo, the north/south asymmetry (NSA), result primarily from variations in the thickness of the darker haze layer, detected by Huygens DISR, above 80 km altitude. If we assume little to no latitudinal methane

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.

Metagenomic Analysis of Hot Springs in Central India Reveals Hydrocarbon Degrading Thermophiles and Pathways Essential for Survival in Extreme Environments.

PubMed

Saxena, Rituja; Dhakan, Darshan B; Mittal, Parul; Waiker, Prashant; Chowdhury, Anirban; Ghatak, Arundhuti; Sharma, Vineet K

2016-01-01

Extreme ecosystems such as hot springs are of great interest as a source of novel extremophilic species, enzymes, metabolic functions for survival and biotechnological products. India harbors hundreds of hot springs, the majority of which are not yet explored and require comprehensive studies to unravel their unknown and untapped phylogenetic and functional diversity. The aim of this study was to perform a large-scale metagenomic analysis of three major hot springs located in central India namely, Badi Anhoni, Chhoti Anhoni, and Tattapani at two geographically distinct regions (Anhoni and Tattapani), to uncover the resident microbial community and their metabolic traits. Samples were collected from seven distinct sites of the three hot spring locations with temperature ranging from 43.5 to 98°C. The 16S rRNA gene amplicon sequencing of V3 hypervariable region and shotgun metagenome sequencing uncovered a unique taxonomic and metabolic diversity of the resident thermophilic microbial community in these hot springs. Genes associated with hydrocarbon degradation pathways, such as benzoate, xylene, toluene, and benzene were observed to be abundant in the Anhoni hot springs (43.5-55°C), dominated by Pseudomonas stutzeri and Acidovorax sp., suggesting the presence of chemoorganotrophic thermophilic community with the ability to utilize complex hydrocarbons as a source of energy. A high abundance of genes belonging to methane metabolism pathway was observed at Chhoti Anhoni hot spring, where methane is reported to constitute >80% of all the emitted gases, which was marked by the high abundance of Methylococcus capsulatus . The Tattapani hot spring, with a high-temperature range (61.5-98°C), displayed a lower microbial diversity and was primarily dominated by a nitrate-reducing archaeal species Pyrobaculum aerophilum . A higher abundance of cell metabolism pathways essential for the microbial survival in extreme conditions was observed at Tattapani. Taken together, the

Metagenomic Analysis of Hot Springs in Central India Reveals Hydrocarbon Degrading Thermophiles and Pathways Essential for Survival in Extreme Environments

PubMed Central

Saxena, Rituja; Dhakan, Darshan B.; Mittal, Parul; Waiker, Prashant; Chowdhury, Anirban; Ghatak, Arundhuti; Sharma, Vineet K.

2017-01-01

Extreme ecosystems such as hot springs are of great interest as a source of novel extremophilic species, enzymes, metabolic functions for survival and biotechnological products. India harbors hundreds of hot springs, the majority of which are not yet explored and require comprehensive studies to unravel their unknown and untapped phylogenetic and functional diversity. The aim of this study was to perform a large-scale metagenomic analysis of three major hot springs located in central India namely, Badi Anhoni, Chhoti Anhoni, and Tattapani at two geographically distinct regions (Anhoni and Tattapani), to uncover the resident microbial community and their metabolic traits. Samples were collected from seven distinct sites of the three hot spring locations with temperature ranging from 43.5 to 98°C. The 16S rRNA gene amplicon sequencing of V3 hypervariable region and shotgun metagenome sequencing uncovered a unique taxonomic and metabolic diversity of the resident thermophilic microbial community in these hot springs. Genes associated with hydrocarbon degradation pathways, such as benzoate, xylene, toluene, and benzene were observed to be abundant in the Anhoni hot springs (43.5–55°C), dominated by Pseudomonas stutzeri and Acidovorax sp., suggesting the presence of chemoorganotrophic thermophilic community with the ability to utilize complex hydrocarbons as a source of energy. A high abundance of genes belonging to methane metabolism pathway was observed at Chhoti Anhoni hot spring, where methane is reported to constitute >80% of all the emitted gases, which was marked by the high abundance of Methylococcus capsulatus. The Tattapani hot spring, with a high-temperature range (61.5–98°C), displayed a lower microbial diversity and was primarily dominated by a nitrate-reducing archaeal species Pyrobaculum aerophilum. A higher abundance of cell metabolism pathways essential for the microbial survival in extreme conditions was observed at Tattapani. Taken together

Temperature- and pressure-dependent absorption cross sections of gaseous hydrocarbons at 3.39 µm

NASA Astrophysics Data System (ADS)

Klingbeil, A. E.; Jeffries, J. B.; Hanson, R. K.

2006-07-01

The pressure- and temperature-dependent absorption cross sections of several neat hydrocarbons and multi-component fuels are measured using a 3.39 µm helium-neon laser. Absorption cross section measurements are reported for methane, ethylene, propane, n-heptane, iso-octane, n-decane, n-dodecane, JP-10, gasoline and jet-A with an estimated uncertainty of less than 3.5%. The experimental conditions range from 298 to 673 K and from 500 to 2000 Torr with nitrogen as the bath gas. An apparatus is designed to facilitate these measurements, and specific care is taken to ensure the compositional accuracy of the hydrocarbon/N2 mixtures. The absorption cross sections of the smallest hydrocarbons, methane and ethylene, vary with temperature and pressure. The cross sections of larger hydrocarbons show negligible dependence on pressure and only a weak dependence on temperature. The reported data increase the range of conditions and the number of hydrocarbons for which cross section measurements are available at the HeNe laser wavelength.

Impact of Peat Mining and Restoration on Methane Turnover Potential and Methane-Cycling Microorganisms in a Northern Bog.

PubMed

Reumer, Max; Harnisz, Monika; Lee, Hyo Jung; Reim, Andreas; Grunert, Oliver; Putkinen, Anuliina; Fritze, Hannu; Bodelier, Paul L E; Ho, Adrian

2018-02-01

Ombrotrophic peatlands are a recognized global carbon reservoir. Without restoration and peat regrowth, harvested peatlands are dramatically altered, impairing their carbon sink function, with consequences for methane turnover. Previous studies determined the impact of commercial mining on the physicochemical properties of peat and the effects on methane turnover. However, the response of the underlying microbial communities catalyzing methane production and oxidation have so far received little attention. We hypothesize that with the return of Sphagnum spp. postharvest, methane turnover potential and the corresponding microbial communities will converge in a natural and restored peatland. To address our hypothesis, we determined the potential methane production and oxidation rates in natural (as a reference), actively mined, abandoned, and restored peatlands over two consecutive years. In all sites, the methanogenic and methanotrophic population sizes were enumerated using quantitative PCR (qPCR) assays targeting the mcrA and pmoA genes, respectively. Shifts in the community composition were determined using Illumina MiSeq sequencing of the mcrA gene and a pmoA -based terminal restriction fragment length polymorphism (t-RFLP) analysis, complemented by cloning and sequence analysis of the mmoX gene. Peat mining adversely affected methane turnover potential, but the rates recovered in the restored site. The recovery in potential activity was reflected in the methanogenic and methanotrophic abundances. However, the microbial community composition was altered, being more pronounced for the methanotrophs. Overall, we observed a lag between the recovery of the methanogenic/methanotrophic activity and the return of the corresponding microbial communities, suggesting that a longer duration (>15 years) is needed to reverse mining-induced effects on the methane-cycling microbial communities. IMPORTANCE Ombrotrophic peatlands are a crucial carbon sink, but this environment

Hydrocarbon emissions characterization in the Colorado Front Range: A pilot study

NASA Astrophysics Data System (ADS)

Pétron, Gabrielle; Frost, Gregory; Miller, Benjamin R.; Hirsch, Adam I.; Montzka, Stephen A.; Karion, Anna; Trainer, Michael; Sweeney, Colm; Andrews, Arlyn E.; Miller, Lloyd; Kofler, Jonathan; Bar-Ilan, Amnon; Dlugokencky, Ed J.; Patrick, Laura; Moore, Charles T., Jr.; Ryerson, Thomas B.; Siso, Carolina; Kolodzey, William; Lang, Patricia M.; Conway, Thomas; Novelli, Paul; Masarie, Kenneth; Hall, Bradley; Guenther, Douglas; Kitzis, Duane; Miller, John; Welsh, David; Wolfe, Dan; Neff, William; Tans, Pieter

2012-02-01

The multispecies analysis of daily air samples collected at the NOAA Boulder Atmospheric Observatory (BAO) in Weld County in northeastern Colorado since 2007 shows highly correlated alkane enhancements caused by a regionally distributed mix of sources in the Denver-Julesburg Basin. To further characterize the emissions of methane and non-methane hydrocarbons (propane, n-butane, i-pentane, n-pentane and benzene) around BAO, a pilot study involving automobile-based surveys was carried out during the summer of 2008. A mix of venting emissions (leaks) of raw natural gas and flashing emissions from condensate storage tanks can explain the alkane ratios we observe in air masses impacted by oil and gas operations in northeastern Colorado. Using the WRAP Phase III inventory of total volatile organic compound (VOC) emissions from oil and gas exploration, production and processing, together with flashing and venting emission speciation profiles provided by State agencies or the oil and gas industry, we derive a range of bottom-up speciated emissions for Weld County in 2008. We use the observed ambient molar ratios and flashing and venting emissions data to calculate top-down scenarios for the amount of natural gas leaked to the atmosphere and the associated methane and non-methane emissions. Our analysis suggests that the emissions of the species we measured are most likely underestimated in current inventories and that the uncertainties attached to these estimates can be as high as a factor of two.

Relevance and Significance of Extraterrestrial Abiological Hydrocarbon Chemistry.

PubMed

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

2016-06-08

Astrophysical observations show similarity of observed abiological "organics"-i.e., hydrocarbons, their derivatives, and ions (carbocations and carbanions)-with studied terrestrial chemistry. Their formation pathways, their related extraterrestrial hydrocarbon chemistry originating from carbon and other elements after the Big Bang, their parent hydrocarbon and derivative (methane and methanol, respectively), and transportation of derived building blocks of life by meteorites or comets to planet Earth are discussed in this Perspective. Their subsequent evolution on Earth under favorable "Goldilocks" conditions led to more complex molecules and biological systems, and eventually to humans. The relevance and significance of extraterrestrial hydrocarbon chemistry to the limits of science in relation to the physical aspects of evolution on our planet Earth are also discussed.

Sampling, storage, and analysis of C2-C7 non-methane hydrocarbons from the US National Oceanic and Atmospheric Administration Cooperative Air Sampling Network glass flasks.

PubMed

Pollmann, Jan; Helmig, Detlev; Hueber, Jacques; Plass-Dülmer, Christian; Tans, Pieter

2008-04-25

An analytical technique was developed to analyze light non-methane hydrocarbons (NMHC), including ethane, propane, iso-butane, n-butane, iso-pentane, n-pentane, n-hexane, isoprene, benzene and toluene from whole air samples collected in 2.5l-glass flasks used by the National Oceanic and Atmospheric Administration, Earth System Research Laboratory, Global Monitoring Division (NOAA ESRL GMD, Boulder, CO, USA) Cooperative Air Sampling Network. This method relies on utilizing the remaining air in these flasks (which is at below-ambient pressure at this stage) after the completion of all routine greenhouse gas measurements from these samples. NMHC in sample aliquots extracted from the flasks were preconcentrated with a custom-made, cryogen-free inlet system and analyzed by gas chromatography (GC) with flame ionization detection (FID). C2-C7 NMHC, depending on their ambient air mixing ratios, could be measured with accuracy and repeatability errors of generally < or =10-20%. Larger deviations were found for ethene and propene. Hexane was systematically overestimated due to a chromatographic co-elution problem. Saturated NMHC showed less than 5% changes in their mixing ratios in glass flask samples that were stored for up to 1 year. In the same experiment ethene and propene increased at approximately 30% yr(-1). A series of blank experiments showed negligible contamination from the sampling process and from storage (<10 pptv yr(-1)) of samples in these glass flasks. Results from flask NMHC analyses were compared to in-situ NMHC measurements at the Global Atmospheric Watch station in Hohenpeissenberg, Germany. This 9-months side-by-side comparison showed good agreement between both methods. More than 94% of all data comparisons for C2-C5 alkanes, isoprene, benzene and toluene fell within the combined accuracy and precision objectives of the World Meteorological Organization Global Atmosphere Watch (WMO-GAW) for NMHC measurements.

Solubility of polyethers in hydrocarbons at low temperatures. A model for potential genetic backbones on warm titans.

PubMed

McLendon, Christopher; Opalko, F Jeffrey; Illangkoon, Heshan I; Benner, Steven A

2015-03-01

Ethers are proposed here as the repeating backbone linking units in linear genetic biopolymers that might support Darwinian evolution in hydrocarbon oceans. Hydrocarbon oceans are found in our own solar system as methane mixtures on Titan. They may be found as mixtures of higher alkanes (propane, for example) on warmer hydrocarbon-rich planets in exosolar systems ("warm Titans"). We report studies on the solubility of several short polyethers in propane over its liquid range (from 85 to 231 K, or -188 °C to -42 °C). These show that polyethers are reasonably soluble in propane at temperatures down to ca. 200 K. However, their solubilities drop dramatically at still lower temperatures and become immeasurably low below 170 K, still well above the ∼ 95 K in Titan's oceans. Assuming that a liquid phase is essential for any living system, and genetic biopolymers must dissolve in that biosolvent to support Darwinism, these data suggest that we must look elsewhere to identify linear biopolymers that might support genetics in Titan's surface oceans. However, genetic molecules with polyether backbones may be suitable to support life in hydrocarbon oceans on warm Titans, where abundant organics and environments lacking corrosive water might make it easier for life to originate.

Source apportionment of ambient non-methane hydrocarbons in Hong Kong: application of a principal component analysis/absolute principal component scores (PCA/APCS) receptor model.

PubMed

Guo, H; Wang, T; Louie, P K K

2004-06-01

Receptor-oriented source apportionment models are often used to identify sources of ambient air pollutants and to estimate source contributions to air pollutant concentrations. In this study, a PCA/APCS model was applied to the data on non-methane hydrocarbons (NMHCs) measured from January to December 2001 at two sampling sites: Tsuen Wan (TW) and Central & Western (CW) Toxic Air Pollutants Monitoring Stations in Hong Kong. This multivariate method enables the identification of major air pollution sources along with the quantitative apportionment of each source to pollutant species. The PCA analysis identified four major pollution sources at TW site and five major sources at CW site. The extracted pollution sources included vehicular internal engine combustion with unburned fuel emissions, use of solvent particularly paints, liquefied petroleum gas (LPG) or natural gas leakage, and industrial, commercial and domestic sources such as solvents, decoration, fuel combustion, chemical factories and power plants. The results of APCS receptor model indicated that 39% and 48% of the total NMHCs mass concentrations measured at CW and TW were originated from vehicle emissions, respectively. 32% and 36.4% of the total NMHCs were emitted from the use of solvent and 11% and 19.4% were apportioned to the LPG or natural gas leakage, respectively. 5.2% and 9% of the total NMHCs mass concentrations were attributed to other industrial, commercial and domestic sources, respectively. It was also found that vehicle emissions and LPG or natural gas leakage were the main sources of C(3)-C(5) alkanes and C(3)-C(5) alkenes while aromatics were predominantly released from paints. Comparison of source contributions to ambient NMHCs at the two sites indicated that the contribution of LPG or natural gas at CW site was almost twice that at TW site. High correlation coefficients (R(2) > 0.8) between the measured and predicted values suggested that the PCA/APCS model was applicable for estimation

Some advantages of methane in an aircraft gas turbine

NASA Technical Reports Server (NTRS)

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

1980-01-01

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

Determination of microbial carbon sources and cycling during remediation of petroleum hydrocarbon impacted soil using natural abundance (14)C analysis of PLFA.

PubMed

Cowie, Benjamin R; Greenberg, Bruce M; Slater, Gregory F

2010-04-01

In a petroleum impacted land-farm soil in Sarnia, Ontario, compound-specific natural abundance radiocarbon analysis identified biodegradation by the soil microbial community as a major pathway for hydrocarbon removal in a novel remediation system. During remediation of contaminated soils by a plant growth promoting rhizobacteria enhanced phytoremediation system (PEPS), the measured Delta(14)C of phospholipid fatty acid (PLFA) biomarkers ranged from -793 per thousand to -897 per thousand, directly demonstrating microbial uptake and utilization of petroleum hydrocarbons (Delta(14)C(PHC) = -1000 per thousand). Isotopic mass balance indicated that more than 80% of microbial PLFA carbon was derived from petroleum hydrocarbons (PHC) and a maximum of 20% was obtained from metabolism of more modern carbon sources. These PLFA from the contaminated soils were the most (14)C-depleted biomarkers ever measured for an in situ environmental system, and this study demonstrated that the microbial community in this soil was subsisting primarily on petroleum hydrocarbons. In contrast, the microbial community in a nearby uncontaminated control soil maintained a more modern Delta(14)C signature than total organic carbon (Delta(14)C(PLFA) = +36 per thousand to -147 per thousand, Delta(14)C(TOC) = -148 per thousand), indicating preferential consumption of the most modern plant-derived fraction of soil organic carbon. Measurements of delta(13)C and Delta(14)C of soil CO(2) additionally demonstrated that mineralization of PHC contributed to soil CO(2) at the contaminated site. The CO(2) in the uncontaminated control soil exhibited substantially more modern Delta(14)C values, and lower soil CO(2) concentrations than the contaminated soils, suggesting increased rates of soil respiration in the contaminated soils. In combination, these results demonstrated that biodegradation in the soil microbial community was a primary pathway of petroleum hydrocarbon removal in the PEPS system. This study

Non-LTE aluminium abundances in late-type stars

NASA Astrophysics Data System (ADS)

Nordlander, T.; Lind, K.

2017-11-01

Aims: Aluminium plays a key role in studies of the chemical enrichment of the Galaxy and of globular clusters. However, strong deviations from LTE (non-LTE) are known to significantly affect the inferred abundances in giant and metal-poor stars. Methods: We present non-local thermodynamic equilibrium (NLTE) modeling of aluminium using recent and accurate atomic data, in particular utilizing new transition rates for collisions with hydrogen atoms, without the need for any astrophysically calibrated parameters. For the first time, we perform 3D NLTE modeling of aluminium lines in the solar spectrum. We also compute and make available extensive grids of abundance corrections for lines in the optical and near-infrared using one-dimensional model atmospheres, and apply grids of precomputed departure coefficients to direct line synthesis for a set of benchmark stars with accurately known stellar parameters. Results: Our 3D NLTE modeling of the solar spectrum reproduces observed center-to-limb variations in the solar spectrum of the 7835 Å line as well as the mid-infrared photospheric emission line at 12.33 μm. We infer a 3D NLTE solar photospheric abundance of A(Al) = 6.43 ± 0.03, in exact agreement with the meteoritic abundance. We find that abundance corrections vary rapidly with stellar parameters; for the 3961 Å resonance line, corrections are positive and may be as large as +1 dex, while corrections for subordinate lines generally have positive sign for warm stars but negative for cool stars. Our modeling reproduces the observed line profiles of benchmark K-giants, and we find abundance corrections as large as -0.3 dex for Arcturus. Our analyses of four metal-poor benchmark stars yield consistent abundances between the 3961 Å resonance line and lines in the UV, optical and near-infrared regions. Finally, we discuss implications for the galactic chemical evolution of aluminium.

Diverse, rare microbial taxa responded to the Deepwater Horizon deep-sea hydrocarbon plume.

PubMed

Kleindienst, Sara; Grim, Sharon; Sogin, Mitchell; Bracco, Annalisa; Crespo-Medina, Melitza; Joye, Samantha B

2016-02-01

The Deepwater Horizon (DWH) oil well blowout generated an enormous plume of dispersed hydrocarbons that substantially altered the Gulf of Mexico's deep-sea microbial community. A significant enrichment of distinct microbial populations was observed, yet, little is known about the abundance and richness of specific microbial ecotypes involved in gas, oil and dispersant biodegradation in the wake of oil spills. Here, we document a previously unrecognized diversity of closely related taxa affiliating with Cycloclasticus, Colwellia and Oceanospirillaceae and describe their spatio-temporal distribution in the Gulf's deepwater, in close proximity to the discharge site and at increasing distance from it, before, during and after the discharge. A highly sensitive, computational method (oligotyping) applied to a data set generated from 454-tag pyrosequencing of bacterial 16S ribosomal RNA gene V4-V6 regions, enabled the detection of population dynamics at the sub-operational taxonomic unit level (0.2% sequence similarity). The biogeochemical signature of the deep-sea samples was assessed via total cell counts, concentrations of short-chain alkanes (C1-C5), nutrients, (colored) dissolved organic and inorganic carbon, as well as methane oxidation rates. Statistical analysis elucidated environmental factors that shaped ecologically relevant dynamics of oligotypes, which likely represent distinct ecotypes. Major hydrocarbon degraders, adapted to the slow-diffusive natural hydrocarbon seepage in the Gulf of Mexico, appeared unable to cope with the conditions encountered during the DWH spill or were outcompeted. In contrast, diverse, rare taxa increased rapidly in abundance, underscoring the importance of specialized sub-populations and potential ecotypes during massive deep-sea oil discharges and perhaps other large-scale perturbations.

Diverse, rare microbial taxa responded to the Deepwater Horizon deep-sea hydrocarbon plume

PubMed Central

Kleindienst, Sara; Grim, Sharon; Sogin, Mitchell; Bracco, Annalisa; Crespo-Medina, Melitza; Joye, Samantha B

2016-01-01

The Deepwater Horizon (DWH) oil well blowout generated an enormous plume of dispersed hydrocarbons that substantially altered the Gulf of Mexico's deep-sea microbial community. A significant enrichment of distinct microbial populations was observed, yet, little is known about the abundance and richness of specific microbial ecotypes involved in gas, oil and dispersant biodegradation in the wake of oil spills. Here, we document a previously unrecognized diversity of closely related taxa affiliating with Cycloclasticus, Colwellia and Oceanospirillaceae and describe their spatio-temporal distribution in the Gulf's deepwater, in close proximity to the discharge site and at increasing distance from it, before, during and after the discharge. A highly sensitive, computational method (oligotyping) applied to a data set generated from 454-tag pyrosequencing of bacterial 16S ribosomal RNA gene V4–V6 regions, enabled the detection of population dynamics at the sub-operational taxonomic unit level (0.2% sequence similarity). The biogeochemical signature of the deep-sea samples was assessed via total cell counts, concentrations of short-chain alkanes (C1–C5), nutrients, (colored) dissolved organic and inorganic carbon, as well as methane oxidation rates. Statistical analysis elucidated environmental factors that shaped ecologically relevant dynamics of oligotypes, which likely represent distinct ecotypes. Major hydrocarbon degraders, adapted to the slow-diffusive natural hydrocarbon seepage in the Gulf of Mexico, appeared unable to cope with the conditions encountered during the DWH spill or were outcompeted. In contrast, diverse, rare taxa increased rapidly in abundance, underscoring the importance of specialized sub-populations and potential ecotypes during massive deep-sea oil discharges and perhaps other large-scale perturbations. PMID:26230048

Studies of Methane Counterflow Flames at Low Pressures

NASA Astrophysics Data System (ADS)

Burrell, Robert Roe

Methane is the smallest hydrocarbon molecule, the fuel most widely studied in fundamental flame structure studies, and a major component of natural gas. Despite many decades of research into the fundamental chemical kinetics involved in methane oxidation, ongoing advancements in research suggest that more progress can be made. Though practical combustors of industrial and commercial significance operate at high pressures and turbulent flow conditions, fundamental understanding of combustion chemistry in flames is more readily obtained for low pressure and laminar flow conditions. Measurements were performed from 1 to 0.1 atmospheres for premixed methane/air and non-premixed methane-nitrogen/oxygen flames in a counterflow. Comparative modeling with quasi-one-dimensional strained flame codes revealed bias-induced errors in measured velocities up to 8% at 0.1 atmospheres due to tracer particle phase velocity slip in the low density gas reacting flow. To address this, a numerically-assisted correction scheme consisting of direct simulation of the particle phase dynamics in counterflow was implemented. Addition of reactions describing the prompt dissociation of formyl radicals to an otherwise unmodified USC Mech II kinetic model was found to enhance computed flame reactivity and substantially improve the predictive capability of computed results for measurements at the lowest pressures studied. Yet, the same modifications lead to overprediction of flame data at 1 atmosphere where results from the unmodified USC Mech II kinetic mechanism agreed well with ambient pressure flame data. The apparent failure of a single kinetic model to capture pressure dependence in methane flames motivates continued skepticism regarding the current understanding of pressure dependence in kinetic models, even for the simplest fuels.

40 CFR 86.1816-08 - Emission standards for complete heavy-duty vehicles.

Code of Federal Regulations, 2014 CFR

2014-07-01

... hydrocarbon equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty Vehicles, Light...

Chasing Sources and Transports of Methane Plumes in the Northern Gulf of Mexico Using In Situ Sensors on Untethered Landers

NASA Astrophysics Data System (ADS)

Martens, C. S.; Mendlovitz, H.; Seim, H.; Lapham, L.; Magen, C.; Joye, S. B.; MacDonald, I. R.; Asper, V. L.; Diercks, A. R.

2016-02-01

In situ time-series measurements of light hydrocarbons, oxygen, temperature and bottom currents from landers and elevators in the benthic boundary layer (BBL) at multiple sites in the northern Gulf of Mexico reveal spatial and temporal variability in methane concentrations controlled by horizontal advection of methane-rich plumes originating from nearby natural oil and gas seeps. Multi-sensor systems deployed for several weeks within 1m of the seafloor at depths from 882 to 1622m revealed methane concentrations ranging from near atmospheric saturation (<3 nM) to over 4000 nM depending on seep proximity, current speed and direction. Methane concentrations observed in the BBL equal or exceed maximum near-bottom values seen in shipboard water column profiles analyzed by conventional gas chromatography. Continuous laser sensor methane measurements from mini-landers deployed in September 2015 at our Horn Dome and Bush Hill sites featuring numerous gas seeps revealed methane concentrations ranging from <3 to over 300 nM over two-week periods. Net current speeds in the BBL at our six lander sites in blocks GC600, OC26 and MC118 ranged from near zero to over 5 cm/s; instantaneous speeds ranged from near zero to over 30 cm/s. Near real-time acquisition of continuous hydrocarbon concentration and current data within the BBL and friction layer from untethered platforms provides important new opportunities for monitoring the impacts of natural seeps and accidental hydrocarbon releases. The instrumented approaches we have developed to simultaneously monitor methane sources and physical processes controlling plume development and transport will enable more effective responses to further accidental hydrocarbon releases.

Inhibition of methane consumption in forest soils by monoterpenes

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

Amaral, J.A.; Knowles, R.

1998-04-01

Selected monoterpenes were tested for their ability to inhibit atmospheric methane consumption by three forest soils from different vegetation types and by the cultured methanotrophic strain, Methylosinus trichosporium OB3b. Subsurface soil from coniferous (Pinus banksiana), deciduous (Populus tremuloides), and mixed hardwood (Tsuga canadensis and Prunus pensylvanica) stands was used under field-moist and slurry conditions. Most of the hydrocarbon monoterpenes tested significantly inhibited methane consumption by soils at environmentally relevant levels, with ({minus})-{alpha}-pinene being the most effective. With the exception of {beta}-myrcene, monoterpenes also strongly inhibited methane oxidation by Methylosinus trichosporium OB3b. Carbon dioxide production was stimulated in all of themore » soils by the monoterpenes tested. In one case, methane production was stimulated by ({minus})-{alpha}-pinene in an intact, aerobic core. Oxide and alcohol monoterpenoids stimulated methane production. Thus, monoterpenes appear to be potentially important regulators of methane consumption and carbon metabolism in forest soils.« less

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

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

Wilson, R.B. Jr.; Posin, B.M.; Chan, Yee Wai

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

Methane Hydrates: More Than a Viable Aviation Fuel Feedstock Option

NASA Technical Reports Server (NTRS)

Hendricks, Robert C.

2007-01-01

Demand for hydrocarbon fuels is steadily increasing, and greenhouse gas emissions continue to rise unabated with the energy demand. Alternate fuels will be coming on line to meet that demand. This report examines the recovering of methane from methane hydrates for fuel to meet this demand rather than permitting its natural release into the environment, which will be detrimental to the planet. Some background on the nature, vast sizes, and stability of sedimentary and permafrost formations of hydrates are discussed. A few examples of the severe problems associated with methane recovery from these hydrates are presented along with the potential impact on the environment and coastal waters. Future availability of methane from hydrates may become an attractive option for aviation fueling, and so future aircraft design associated with methane fueling is considered.

Bacterial dominance in subseafloor sediments characterized by methane hydrates

USGS Publications Warehouse

Briggs, Brandon R.; Inagaki, Fumio; Morono, Yuki; Futagami, Taiki; Huguet, Carme; Rosell-Mele, Antoni; Lorenson, T.D.; Colwell, Frederick S.

2015-01-01

The degradation of organic carbon in subseafloor sediments on continental margins contributes to the largest reservoir of methane on Earth. Sediments in the Andaman Sea are composed of ~ 1% marine-derived organic carbon and biogenic methane is present. Our objective was to determine microbial abundance and diversity in sediments that transition the gas hydrate occurrence zone (GHOZ) in the Andaman Sea. Microscopic cell enumeration revealed that most sediment layers harbored relatively low microbial abundance (103–105 cells cm−3). Archaea were never detected despite the use of both DNA- and lipid-based methods. Statistical analysis of terminal restriction fragment length polymorphisms revealed distinct microbial communities from above, within, and below the GHOZ, and GHOZ samples were correlated with a decrease in organic carbon. Primer-tagged pyrosequences of bacterial 16S rRNA genes showed that members of the phylum Firmicutes are predominant in all zones. Compared with other seafloor settings that contain biogenic methane, this deep subseafloor habitat has a unique microbial community and the low cell abundance detected can help to refine global subseafloor microbial abundance.

Dissolved methane occurrences in aquifers in the footprint of Texas shale plays and their controls

NASA Astrophysics Data System (ADS)

Nicot, J. P.; Mickler, P. J.; Larson, T.; Darvari, R.; Smyth, R. C.

2015-12-01

Many constituents typically associated with oil and gas production, such as methane and higher-order hydrocarbons, exist naturally in shallow groundwater. Recent studies of aquifers in the footprint of several gas plays across the US have showed that (1) dissolved thermogenic methane may or may not be present in the shallow subsurface and (2) shallow thermogenic methane could be naturally occurring and emplaced through mostly vertical migration over geologic time and is not necessarily a consequence of gas production from a gas play. A total of 800+ water wells have been sampled across the state of Texas to characterize shallow methane in fresh-water aquifers overlying shale plays and other tight formations (Barnett, Eagle Ford, Haynesville shale areas as well as in the Delaware Basin of West Texas). Analytical results suggest that dissolved methane is not widespread in shallow groundwater and that, when present at concentration greater than 10 mg/L, is often of natural but thermogenic or mixed origin according to the isotopic signature and to the presence of other light hydrocarbons.

H2S mediated thermal and photochemical methane activation

PubMed Central

Baltrusaitis, Jonas; de Graaf, Coen; Broer, Ria; Patterson, Eric

2013-01-01

Sustainable, low temperature methods of natural gas activation are critical in addressing current and foreseeable energy and hydrocarbon feedstock needs. Large portions of natural gas resources are still too expensive to process due to their high content of hydrogen sulfide gas (H2S) in mixture with methane, CH4, altogether deemed as sub-quality or “sour” gas. We propose a unique method for activating this “sour” gas to form a mixture of sulfur-containing hydrocarbon intermediates, CH3SH and CH3SCH3, and an energy carrier, such as H2. For this purpose, we computationally investigated H2S mediated methane activation to form a reactive CH3SH species via direct photolysis of sub-quality natural gas. Photoexcitation of hydrogen sulfide in the CH4+H2S complex results in a barrier-less relaxation via a conical intersection to form a ground state CH3SH+H2 complex. The resulting CH3SH can further be heterogeneously coupled over acidic catalysts to form higher hydrocarbons while the H2 can be used as a fuel. This process is very different from a conventional thermal or radical-based processes and can be driven photolytically at low temperatures, with enhanced controllability over the process conditions currently used in industrial oxidative natural gas activation. Finally, the proposed process is CO2 neutral, as opposed to the currently industrially used methane steam reforming (SMR). PMID:24150813

H2S-mediated thermal and photochemical methane activation.

PubMed

Baltrusaitis, Jonas; de Graaf, Coen; Broer, Ria; Patterson, Eric V

2013-12-02

Sustainable, low-temperature methods for natural gas activation are critical in addressing current and foreseeable energy and hydrocarbon feedstock needs. Large portions of natural gas resources are still too expensive to process due to their high content of hydrogen sulfide gas (H2S) mixed with methane, deemed altogether as sub-quality or "sour" gas. We propose a unique method of activation to form a mixture of sulfur-containing hydrocarbon intermediates, CH3SH and CH3SCH3 , and an energy carrier such as H2. For this purpose, we investigated the H2S-mediated methane activation to form a reactive CH3SH species by means of direct photolysis of sub-quality natural gas. Photoexcitation of hydrogen sulfide in the CH4 + H2S complex resulted in a barrierless relaxation by a conical intersection to form a ground-state CH3SH + H2 complex. The resulting CH3SH could further be coupled over acidic catalysts to form higher hydrocarbons, and the resulting H2 used as a fuel. This process is very different from conventional thermal or radical-based processes and can be driven photolytically at low temperatures, with enhanced control over the conditions currently used in industrial oxidative natural gas activation. Finally, the proposed process is CO2 neutral, as opposed to the current industrial steam methane reforming (SMR). Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Coal-Packed Methane Biofilter for Mitigation of Green House Gas Emissions from Coal Mine Ventilation Air

PubMed Central

Limbri, Hendy; Gunawan, Cindy; Thomas, Torsten; Smith, Andrew; Scott, Jason; Rosche, Bettina

2014-01-01

Methane emitted by coal mine ventilation air (MVA) is a significant greenhouse gas. A mitigation strategy is the oxidation of methane to carbon dioxide, which is approximately twenty-one times less effective at global warming than methane on a mass-basis. The low non-combustible methane concentrations at high MVA flow rates call for a catalytic strategy of oxidation. A laboratory-scale coal-packed biofilter was designed and partially removed methane from humidified air at flow rates between 0.2 and 2.4 L min−1 at 30°C with nutrient solution added every three days. Methane oxidation was catalysed by a complex community of naturally-occurring microorganisms, with the most abundant member being identified by 16S rRNA gene sequence as belonging to the methanotrophic genus Methylocystis. Additional inoculation with a laboratory-grown culture of Methylosinus sporium, as investigated in a parallel run, only enhanced methane consumption during the initial 12 weeks. The greatest level of methane removal of 27.2±0.66 g methane m−3 empty bed h−1 was attained for the non-inoculated system, which was equivalent to removing 19.7±2.9% methane from an inlet concentration of 1% v/v at an inlet gas flow rate of 1.6 L min−1 (2.4 min empty bed residence time). These results show that low-cost coal packing holds promising potential as a suitable growth surface and contains methanotrophic microorganisms for the catalytic oxidative removal of methane. PMID:24743729

Coupling Oxygen Consumption with Hydrocarbon Oxidation in Bacterial Multicomponent Monooxygenases.

PubMed

Wang, Weixue; Liang, Alexandria D; Lippard, Stephen J

2015-09-15

A fundamental goal in catalysis is the coupling of multiple reactions to yield a desired product. Enzymes have evolved elegant approaches to address this grand challenge. A salient example is the biological conversion of methane to methanol catalyzed by soluble methane monooxygenase (sMMO), a member of the bacterial multicomponent monooxygenase (BMM) superfamily. sMMO is a dynamic protein complex of three components: a hydroxylase, a reductase, and a regulatory protein. The active site, a carboxylate-rich non-heme diiron center, is buried inside the 251 kDa hydroxylase component. The enzyme processes four substrates: O2, protons, electrons, and methane. To couple O2 activation to methane oxidation, timely control of substrate access to the active site is critical. Recent studies of sMMO, as well as its homologues in the BMM superfamily, have begun to unravel the mechanism. The emerging and unifying picture reveals that each substrate gains access to the active site along a specific pathway through the hydroxylase. Electrons and protons are delivered via a three-amino-acid pore located adjacent to the diiron center; O2 migrates via a series of hydrophobic cavities; and hydrocarbon substrates reach the active site through a channel or linked set of cavities. The gating of these pathways mediates entry of each substrate to the diiron active site in a timed sequence and is coordinated by dynamic interactions with the other component proteins. The result is coupling of dioxygen consumption with hydrocarbon oxidation, avoiding unproductive oxidation of the reductant rather than the desired hydrocarbon. To initiate catalysis, the reductase delivers two electrons to the diiron(III) center by binding over the pore of the hydroxylase. The regulatory component then displaces the reductase, docking onto the same surface of the hydroxylase. Formation of the hydroxylase-regulatory component complex (i) induces conformational changes of pore residues that may bring protons to the

Methane oxidation and abundance of methane oxidizers in tropical agricultural soil (vertisol) in response to CuO and ZnO nanoparticles contamination.

PubMed

Mohanty, Santosh Ranjan; Rajput, Parul; Kollah, Bharati; Chourasiya, Dipanti; Tiwari, Archana; Singh, Muneshwar; Rao, A Subba

2014-06-01

There is worldwide concern over the increase use of nanoparticles (NPs) and their ecotoxicological effect. It is not known if the annual production of tons of industrial nanoparticles (NPs) has the potential to impact terrestrial microbial communities, which are so necessary for ecosystem functioning. Here, we have examined the consequences of adding the NPs particularly the metal oxide (CuO, ZnO) on CH4 oxidation activity in vertisol and the abundance of heterotrophs, methane oxidizers, and ammonium oxidizers. Soil samples collected from the agricultural field located at Madhya Pradesh, India, were incubated with either CuO and ZnO NPs or ionic heavy metals (CuCl2, ZnCl2) separately at 0, 10, and 20 μg g(-1) soil. CH4 oxidation activity in the soil samples was estimated at 60 and 100 % moisture holding capacity (MHC) in order to link soil moisture regime with impact of NPs. NPs amended to soil were highly toxic for the microbial-mediated CH4 oxidation, compared with the ionic form. The trend of inhibition was Zn 20 > Zn 10 > Cu 20 > Cu 10. NPs delayed the lag phase of CH4 oxidation to a maximum of 4-fold and also decreased the apparent rate constant k up to 50 % over control. ANOVA and Pearson correlation analysis (α = 0.01) revealed significant impact of NPs on the CH4 oxidation activity and microbial abundance (p < 0.0001, and high F statistics). Principal component analysis (PCA) revealed that PC1 (metal concentration) rendered 76.06 % of the total variance, while 18.17 % of variance accounted by second component (MHC). Biplot indicated negative impact of NPs on CH4 oxidation and microbial abundance. Our result also confirmed that higher soil moisture regime alleviates toxicity of NPs and opens new avenues of research to manage ecotoxicity and environmental hazard of NPs.

Process for converting light alkanes to higher hydrocarbons

DOEpatents

Noceti, Richard P.; Taylor, Charles E.

1988-01-01

A process is disclosed for the production of aromatic-rich, gasoline boiling range hydrocarbons from the lower alkanes, particularly from methane. The process is carried out in two stages. In the first, alkane is reacted with oxygen and hydrogen chloride over an oxyhydrochlorination catalyst such as copper chloride with minor proportions of potassium chloride and rare earth chloride. This produces an intermediate gaseous mixture containing water and chlorinated alkanes. The chlorinated alkanes are contacted with a crystalline aluminosilicate catalyst in the hydrogen or metal promoted form to produce gasoline range hydrocarbons with a high proportion of aromatics and a small percentage of light hydrocarbons (C.sub.2 -C.sub.4). The light hydrocarbons can be recycled for further processing over the oxyhydrochlorination catalyst.

Methanogenic Hydrocarbon Degradation: Evidence from Field and Laboratory Studies.

PubMed

Jiménez, Núria; Richnow, Hans H; Vogt, Carsten; Treude, Tina; Krüger, Martin

2016-01-01

Microbial transformation of hydrocarbons to methane is an environmentally relevant process taking place in a wide variety of electron acceptor-depleted habitats, from oil reservoirs and coal deposits to contaminated groundwater and deep sediments. Methanogenic hydrocarbon degradation is considered to be a major process in reservoir degradation and one of the main processes responsible for the formation of heavy oil deposits and oil sands. In the absence of external electron acceptors such as oxygen, nitrate, sulfate or Fe(III), fermentation and methanogenesis become the dominant microbial metabolisms. The major end product under these conditions is methane, and the only electron acceptor necessary to sustain the intermediate steps in this process is CO2, which is itself a net product of the overall reaction. We are summarizing the state of the art and recent advances in methanogenic hydrocarbon degradation research. Both the key microbial groups involved as well as metabolic pathways are described, and we discuss the novel insights into methanogenic hydrocarbon-degrading populations studied in laboratory as well as environmental systems enabled by novel cultivation-based and molecular approaches. Their possible implications on energy resources, bioremediation of contaminated sites, deep-biosphere research, and consequences for atmospheric composition and ultimately climate change are also addressed. © 2016 S. Karger AG, Basel.

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

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.

Molar tooth carbonates and benthic methane fluxes in Proterozoic oceans.

PubMed

Shen, Bing; Dong, Lin; Xiao, Shuhai; Lang, Xianguo; Huang, Kangjun; Peng, Yongbo; Zhou, Chuanming; Ke, Shan; Liu, Pengju

2016-01-07

Molar tooth structures are ptygmatically folded and microspar-filled structures common in early- and mid-Proterozoic (∼2,500-750 million years ago, Ma) subtidal successions, but extremely rare in rocks <750 Ma. Here, on the basis of Mg and S isotopes, we show that molar tooth structures may have formed within sediments where microbial sulphate reduction and methanogenesis converged. The convergence was driven by the abundant production of methyl sulphides (dimethyl sulphide and methanethiol) in euxinic or H2S-rich seawaters that were widespread in Proterozoic continental margins. In this convergence zone, methyl sulphides served as a non-competitive substrate supporting methane generation and methanethiol inhibited anaerobic oxidation of methane, resulting in the buildup of CH4, formation of degassing cracks in sediments and an increase in the benthic methane flux from sediments. Precipitation of crack-filling microspar was driven by methanogenesis-related alkalinity accumulation. Deep ocean ventilation and oxygenation around 750 Ma brought molar tooth structures to an end.

Molar tooth carbonates and benthic methane fluxes in Proterozoic oceans

PubMed Central

Shen, Bing; Dong, Lin; Xiao, Shuhai; Lang, Xianguo; Huang, Kangjun; Peng, Yongbo; Zhou, Chuanming; Ke, Shan; Liu, Pengju

2016-01-01

Molar tooth structures are ptygmatically folded and microspar-filled structures common in early- and mid-Proterozoic (∼2,500–750 million years ago, Ma) subtidal successions, but extremely rare in rocks <750 Ma. Here, on the basis of Mg and S isotopes, we show that molar tooth structures may have formed within sediments where microbial sulphate reduction and methanogenesis converged. The convergence was driven by the abundant production of methyl sulphides (dimethyl sulphide and methanethiol) in euxinic or H2S-rich seawaters that were widespread in Proterozoic continental margins. In this convergence zone, methyl sulphides served as a non-competitive substrate supporting methane generation and methanethiol inhibited anaerobic oxidation of methane, resulting in the buildup of CH4, formation of degassing cracks in sediments and an increase in the benthic methane flux from sediments. Precipitation of crack-filling microspar was driven by methanogenesis-related alkalinity accumulation. Deep ocean ventilation and oxygenation around 750 Ma brought molar tooth structures to an end. PMID:26739600

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,

Distinct Aqueous and Hydrocarbon Cryovolcanism on Titan and Other Icy Satellites (Invited)

NASA Astrophysics Data System (ADS)

Kargel, J. S.; Furfaro, R.; Candelaria, P.

2010-12-01

icy shells, stable aqueous liquids are mainly confined to deep levels and cryovolcanism does not occur unless ammonia is abundant, as it may be on Triton. On Titan, we think the icy shell is thick, ammonia might not be abundant, and aqueous cryovolcanism might occur rarely, if at all. However, many hydrocarbons are abundant on Titan—both photolytic and endogenic—and may melt in the icy crust and form low-temperature, buoyant liquids. Hydrocarbon cryovolcanism is likely. Hydrocarbon lavas may range from exceeding low viscosity unimolecular types to highly viscous and possibly asphalt-, wax-, or plastic-like solid-liquid mixtures of complex and highly polymerized compositions. Some hydrocarbons may melt just hundreds of meters to a few kilometers beneath Titan’s surface. Shallow hydrocarbon deposits may melt or crystallize when insulating surface hydrocarbon deposits are emplaced or removed by sublimation, fluvial, or eolian processes. Deep interior endogenic hydrocarbons may erupt if they evade a gauntlet of physical and chemical barriers during ascent. Hydrocarbon cryovolcanic landforms may resemble skating ponds, silicate lava flows, salt extrusions, asphalt flows, or glaciers.

Large Abundances of Polycyclic Aromatic Hydrocarbons in Titan's Upper Atmosphere

NASA Technical Reports Server (NTRS)

Lopez-Puertas, M.; Dinelli, B. M.; Adriani, A.; Funke, B.; Garcia-Comas, M.; Moriconi, M. L.; D'Aversa, E.; Boersma, C.; Allamandola, L. J.

2013-01-01

In this paper, we analyze the strong unidentified emission near 3.28 micron in Titan's upper daytime atmosphere recently discovered by Dinelli et al.We have studied it by using the NASA Ames PAH IR Spectroscopic Database. The polycyclic aromatic hydrocarbons (PAHs), after absorbing UV solar radiation, are able to emit strongly near 3.3 micron. By using current models for the redistribution of the absorbed UV energy, we have explained the observed spectral feature and have derived the vertical distribution of PAH abundances in Titan's upper atmosphere. PAHs have been found to be present in large concentrations, about (2-3) × 10(exp 4) particles / cubic cm. The identified PAHs have 9-96 carbons, with a concentration-weighted average of 34 carbons. The mean mass is approx 430 u; the mean area is about 0.53 sq. nm; they are formed by 10-11 rings on average, and about one-third of them contain nitrogen atoms. Recently, benzene together with light aromatic species as well as small concentrations of heavy positive and negative ions have been detected in Titan's upper atmosphere. We suggest that the large concentrations of PAHs found here are the neutral counterpart of those positive and negative ions, which hence supports the theory that the origin of Titan main haze layer is located in the upper atmosphere.

The methane distribution on Titan: high resolution spectroscopy in the near-IR with Keck NIRSPEC/AO

NASA Astrophysics Data System (ADS)

Adamkovics, Mate; Mitchell, Jonathan L.

2014-11-01

The distribution of methane on Titan is a diagnostic of regional scale meteorology and large scale atmospheric circulation. The observed formation of clouds and the transport of heat through the atmosphere both depend on spatial and temporal variations in methane humidity. We have performed observations to measure the the distribution on methane Titan using high spectral resolution near-IR (H-band) observations made with NIRSPEC, with adaptive optics, at Keck Observatory in July 2014. This work builds on previous attempts at this measurement with improvement in the observing protocol and data reduction, together with increased integration times. Radiative transfer models using line-by-line calculation of methane opacities from the HITRAN2012 database are used to retrieve methane abundances. We will describe analysis of the reduced observations, which show latitudinal spatial variation in the region the spectrum that is thought to be sensitive to methane abundance. Quantifying the methane abundance variation requires models that include the spatial variation in surface albedo and meridional haze gradient; we will describe (currently preliminary) analysis of the the methane distribution and uncertainties in the retrieval.

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

PubMed Central

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

2017-01-01

and hydrocarbon exploitation. Nonetheless, quantifying methane metabolism typically involves logistically challenging methods and/or specialized equipment; these impediments have limited our understanding of methane fluxes and reservoirs in natural systems, making effective management difficult. Here, we offer an easily implementable, precise method using monodeuterated methane (CH3D) that advances three specific aims. First, it allows users to directly compare methane consumption rates between different experimental treatments of the same inoculum. Second, by empirically linking the CH3D procedure with the well-established 14C radiocarbon approach, we determine absolute scaling factors that facilitate rate measurements for several aerobic and anaerobic systems of interest. Third, CH3D represents a helpful tool in evaluating the relationship between methane activation and full oxidation in methanotrophic metabolisms. The procedural advantages, consistency, and novel research questions enabled by the CH3D method should prove useful in a wide range of culture-based and environmental microbial systems to further elucidate methane metabolism dynamics. PMID:28861523

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

PubMed

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

2017-01-01

and hydrocarbon exploitation. Nonetheless, quantifying methane metabolism typically involves logistically challenging methods and/or specialized equipment; these impediments have limited our understanding of methane fluxes and reservoirs in natural systems, making effective management difficult. Here, we offer an easily implementable, precise method using monodeuterated methane (CH 3 D) that advances three specific aims. First, it allows users to directly compare methane consumption rates between different experimental treatments of the same inoculum. Second, by empirically linking the CH 3 D procedure with the well-established 14 C radiocarbon approach, we determine absolute scaling factors that facilitate rate measurements for several aerobic and anaerobic systems of interest. Third, CH 3 D represents a helpful tool in evaluating the relationship between methane activation and full oxidation in methanotrophic metabolisms. The procedural advantages, consistency, and novel research questions enabled by the CH 3 D method should prove useful in a wide range of culture-based and environmental microbial systems to further elucidate methane metabolism dynamics.

Characterization of the Hydrocarbon Potential and Non-Potential Zones Using Wavelet-Based Fractal Analysis

NASA Astrophysics Data System (ADS)

Mukherjee, Bappa; Roy, P. N. S.

The identification of prospective and dry zone is of major importance from well log data. Truthfulness in the identification of potential zone is a very crucial issue in hydrocarbon exploration. In this line, the problem has received considerable attention and many conventional techniques have been proposed. The purpose of this study is to recognize the hydrocarbon and non-hydrocarbon bearing portion within a reservoir by using the non-conventional technique. The wavelet based fractal analysis (WBFA) has been applied on the wire-line log data in order to obtain the pre-defined hydrocarbon (HC) and non-hydrocarbon (NHC) zones by their self-affine signal nature is demonstrated in this paper. The feasibility of the proposed technique is tested with the help of most commonly used logs, like self-potential, gamma ray, resistivity and porosity log responses. These logs are obtained from the industry to make out several HC and NHC zones of all wells in the study region belonging to the upper Assam basin. The results obtained in this study for a particular log response, where in the case of HC bearing zones, it is found that they are mainly situated in a variety of sandstones lithology which leads to the higher Hurst exponent. Further, the NHC zones found to be analogous to lithology with higher shale content having lower Hurst exponent. The above proposed technique can overcome the chance of miss interpretation in conventional reservoir characterization.

Bi-reforming of methane from any source with steam and carbon dioxide exclusively to metgas (CO-2H2) for methanol and hydrocarbon synthesis.

PubMed

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

2013-01-16

A catalyst based on nickel oxide on magnesium oxide (NiO/MgO) thermally activated under hydrogen is effective for the bi-reforming with steam and CO(2) (combined steam and dry reforming) of methane as well as natural gas in a tubular flow reactor at elevated pressures (5-30 atm) and temperatures (800-950 °C). By adjusting the CO(2)-to-steam ratio in the gas feed, the H(2)/CO ratio in the produced syn-gas could be easily adjusted in a single step to the desired value of 2 for methanol and hydrocarbon synthesis.

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

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

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

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

EDTA addition enhances bacterial respiration activities and hydrocarbon degradation in bioaugmented and non-bioaugmented oil-contaminated desert soils.

PubMed

Al Kharusi, Samiha; Abed, Raeid M M; Dobretsov, Sergey

2016-03-01

The low number and activity of hydrocarbon-degrading bacteria and the low solubility and availability of hydrocarbons hamper bioremediation of oil-contaminated soils in arid deserts, thus bioremediation treatments that circumvent these limitations are required. We tested the effect of Ethylenediaminetetraacetic acid (EDTA) addition, at different concentrations (i.e. 0.1, 1 and 10 mM), on bacterial respiration and biodegradation of Arabian light oil in bioaugmented (i.e. with the addition of exogenous alkane-degrading consortium) and non-bioaugmented oil-contaminated desert soils. Post-treatment shifts in the soils' bacterial community structure were monitored using MiSeq sequencing. Bacterial respiration, indicated by the amount of evolved CO2, was highest at 10 mM EDTA in bioaugmented and non-bioaugmented soils, reaching an amount of 2.2 ± 0.08 and 1.6 ± 0.02 mg-CO2 g(-1) after 14 days of incubation, respectively. GC-MS revealed that 91.5% of the C14-C30 alkanes were degraded after 42 days when 10 mM EDTA and the bacterial consortium were added together. MiSeq sequencing showed that 78-91% of retrieved sequences in the original soil belonged to Deinococci, Alphaproteobacteria, Gammaproteobacteia and Bacilli. The same bacterial classes were detected in the 10 mM EDTA-treated soils, however with slight differences in their relative abundances. In the bioaugmented soils, only Alcanivorax sp. MH3 and Parvibaculum sp. MH21 from the exogenous bacterial consortium could survive until the end of the experiment. We conclude that the addition of EDTA at appropriate concentrations could facilitate biodegradation processes by increasing hydrocarbon availability to microbes. The addition of exogenous oil-degrading bacteria along with EDTA could serve as an ideal solution for the decontamination of oil-contaminated desert soils. Copyright © 2016 Elsevier Ltd. All rights reserved.

Warmer and drier conditions and nitrogen fertilizer application altered methanotroph abundance and methane emissions in a vegetable soil.

PubMed

Ran, Yu; Xie, Jianli; Xu, Xiaoya; Li, Yong; Liu, Yapeng; Zhang, Qichun; Li, Zheng; Xu, Jianming; Di, Hongjie

2017-01-01

Methane (CH 4 ) is a potent greenhouse gas, and soil can both be a source and sink for atmospheric CH 4 . It is not clear how future climate change may affect soil CH 4 emissions and related microbial communities. The aim of this study was to determine the interactive effects of a simulated warmer and drier climate scenarios and the application of different nitrogen (N) sources (urea and manure) on CH 4 emissions and related microbial community abundance in a vegetable soil. Greenhouses were used to control simulated climate conditions which gave 2.99 °C warmer and 6.2% lower water content conditions. The field experiment was divided into two phases. At the beginning of phase II, half of the greenhouses were removed to study possible legacy effects of the simulated warmer and drier conditions. The responses in methanogen and methanotroph abundance to a simulated climate change scenario were determined using real-time PCR. The results showed that the simulated warmer and drier conditions in the greenhouses significantly decreased CH 4 emissions largely due to the lower soil moisture content. For the same reason, CH 4 emissions of treatments in phase I were much lower than the same treatments in phase II. The abundance of methanotrophs showed a more significant response than methanogens to the simulated climate change scenario, increasing under simulated drier conditions. Methanogenic community abundance remained low, except where manure was applied which provided a source of organic C that stimulated methanogen growth. Soil moisture content was a major driver for methanotroph abundance and strongly affected CH 4 emissions. The application of N source decreased CH 4 emissions probably because of increased methanotrophic activity. CH 4 emissions were positively correlated to methanogenic abundance and negatively correlated to methanotrophic abundance. These results demonstrate that projected future climate change conditions can have a feedback impact on CH 4

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.

Methanogenic degradation of petroleum hydrocarbons in subsurface environments remediation, heavy oil formation, and energy recovery.

PubMed

Gray, N D; Sherry, A; Hubert, C; Dolfing, J; Head, I M

2010-01-01

Hydrocarbons are common constituents of surface, shallow, and deep-subsurface environments. Under anaerobic conditions, hydrocarbons can be degraded to methane by methanogenic microbial consortia. This degradation process is widespread in the geosphere. In comparison with other anaerobic processes, methanogenic hydrocarbon degradation is more sustainable over geological time scales because replenishment of an exogenous electron acceptor is not required. As a consequence, this process has been responsible for the formation of the world's vast deposits of heavy oil, which far exceed conventional oil assets such as those found in the Middle East. Methanogenic degradation is also a potentially important component of attenuation in hydrocarbon contamination plumes. Studies of the organisms, syntrophic partnerships, mechanisms, and geochemical signatures associated with methanogenic hydrocarbon degradation have identified common themes and diagnostic markers for this process in the subsurface. These studies have also identified the potential to engineer methanogenic processes to enhance the recovery of energy assets as biogenic methane from residual oils stranded in petroleum systems. Copyright 2010 Elsevier Inc. All rights reserved.

Raman and FTIR spectroscopy of methane in olivine

NASA Astrophysics Data System (ADS)

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

2017-12-01

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

Evidence of Sulfate-Dependent Anaerobic Methane Oxidation within an Area Impacted by Coalbed Methane-Related Gas Migration

NASA Astrophysics Data System (ADS)

Wolfe, A. L.; Wikin, R. T.

2017-12-01

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. Over a 17-month study period, water samples were obtained from domestic water wells and monitoring wells located within the impacted area, and analyzed for 245 constituents, including organic compounds, nutrients, major and trace elements, dissolved gases, and isotopic tracers for carbon, sulfur, oxygen, and hydrogen. Multiple lines of evidence suggest that sulfate-dependent methane biodegradation, which involves the oxidation of methane (CH4) to carbon dioxide (CO2) using sulfate (SO42-) as the terminal electron acceptor, is occurring: (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. Groundwater-methane attenuation is linked to the production of dissolved sulfide, and elevated dissolved sulfide concentrations represent an undesirable secondary water quality impact. The biogeochemical response of the aquifer system has not mobilized naturally occurring trace metals, including arsenic, chromium, cobalt, nickel, and lead, likely due to the microbial production of hydrogen sulfide, which favors stabilization of metals in aquifer solids.

Distribution, abundance and carbon isotopic composition of gaseous hydrocarbons in Big Soda Lake, Nevada: An alkaline, meromictic lake

USGS Publications Warehouse

Oremland, R.S.; Des Marais, D.J.

1983-01-01

Distribution and isotopic composition (??13C) of low molecular weight hydrocarbon gases were studied in Big Soda Lake (depth = 64 m), an alkaline, meromictic lake with permanently anoxic bottom waters. Methane increased with depth in the anoxic mixolimnion (depth = 20-35 m), reached uniform concentrations (55 ??M/l) in the monimolimnion (35-64 m) and again increased with depth in monimolimnion bottom sediments (>400 ??M/kg below 1 m sub-bottom depth). The ??13C[CH4] values in bottom sediment below 1 m sub-bottom depth (<-70 per mil) increased with vertical distance up the core (??13C[CH4] = -55 per mil at sediment surface). Monimolimnion ??13C[CH4] values (-55 to -61 per mil) were greater than most ??13C[CH4] values found in the anoxic mixolimnion (92% of samples had ??13C[CH4] values between -20 and -48 per mil). No significant concentrations of ethylene or propylene were found in the lake. However ethane, propane, isobutane and n-butane concentrations all increased with water column depth, with respective maximum concentrations of 260, 80, 23 and 22 nM/l encountered between 50-60 m depth. Concentrations of ethane, propane and butanes decreased with depth in the bottom sediments. Ratios of CH4 [C2H6 + C3H8] were high (250-620) in the anoxic mixolimnion, decreased to ~161 in the monimolimnion and increased with depth in the sediment to values as high as 1736. We concluded that methane has a biogenic origin in both the sediments and the anoxic water column and that C2-C4 alkanes have biogenic origins in the monimolimnion water and shallow sediments. The changes observed in ??13C[CH4] and CH4 (C2H6 + C3H8) with depth in the water column and sediments are probably caused by bacteria] processes. These might include anaerobic methane oxidation and different rates of methanogenesis and C2 to C4 alkane production by microorganisms. ?? 1983.

The Effects of Surface Properties and Albedo on Methane Retrievals with the Airborne Visible/Infrared Imaging Spectrometer Next Generation (AVIRIS-NG)

NASA Astrophysics Data System (ADS)

Ayasse, A.; Thorpe, A. K.; Roberts, D. A.

2017-12-01

Atmospheric methane has increased by a factor of 2.5 since the beginning of the industrial era in response to anthropogenic emissions (Ciais et al., 2013). Although it is less abundant than carbon dioxide it is 86 time more potent on a 20 year time scale (Myhre et al., 2013) and is therefore responsible for about 20% of the total global warming induced by anthropogenic greenhouse gasses (Kirschke et al., 2013). Given the importance of methane to global climate change, monitoring and measuring methane emissions using techniques such as remote sensing is of increasing interest. Recently the Airborne Visible-Infrared Imaging Spectrometer - Next Generation (AVIRIS-NG) has proven to be a valuable instrument for quantitative mapping of methane plumes (Frankenberg et al., 2016; Thorpe et al., 2016; Thompson et al., 2015). In this study, we applied the Iterative Maximum a Posterior Differential Optical Spectroscopy (IMAP-DOAS) methane retrieval algorithm to a synthetic image with variable methane concentrations, albedo, and land cover. This allowed for characterizing retrieval performance, including potential sensitivity to variable land cover, low albedo surfaces, and surfaces known to cause spurious signals. We conclude that albedo had little influence on the IMAP-DOAS results except at very low radiance levels. Water (without sun glint) was found to be the most challenging surface for methane retrievals while hydrocarbons and some green vegetation also caused error. Understanding the effect of surface properties on methane retrievals is important given the increased use of AVIRIS-NG to map gas plumes over diverse locations and methane sources. This analysis could be expanded to include additional gas species like carbon dioxide and to further investigate gas sensitivity of proposed instruments for dedicated gas mapping from airborne and spaceborne platforms.

Apparatus and methods for hydrocarbon extraction

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

Bohnert, George W.; Verhulst, Galen G.

Systems and methods for hydrocarbon extraction from hydrocarbon-containing material. Such systems and methods relate to extracting hydrocarbon from hydrocarbon-containing material employing a non-aqueous extractant. Additionally, such systems and methods relate to recovering and reusing non-aqueous extractant employed for extracting hydrocarbon from hydrocarbon-containing material.

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

Liquid Hydrocarbons on Titan's Surface? How Cassini ISS Observations Fit into the Story (So Far)

NASA Technical Reports Server (NTRS)

Turtle, E. P.; Dawson, D. D.; Fussner, S.; Hardegree-Ullman, E.; Ewen, A. S.; Perry, J.; Porco, C. C.; West, R. A.

2005-01-01

Titan is the only satellite in our Solar System with a substantial atmosphere, the origins and evolution of which are still not well understood. Its primary (greater than 90%) component is nitrogen, with a few percent methane and lesser amounts of other species. Methane and ethane are stable in the liquid state under the temperature and pressure conditions in Titan s lower atmosphere and at the surface; indeed, clouds, likely composed of methane, have been detected. Photochemical processes acting in the atmosphere convert methane into more complex hydrocarbons, creating Titan s haze and destroying methane over relatively short timescales. Therefore, it has been hypothesized that Titan s surface has reservoirs of liquid methane which serve to resupply the atmosphere. Early observations of Titan s surface revealed albedo patterns which have been interpreted as dark hydrocarbon liquids occupying topographically low regions between higher-standing exposures of bright, water-ice bedrock, although this is far from being the only explanation for the observed albedo contrast. Observations made by the Imaging Science Subsystem during Cassini's approach to Saturn and its first encounters with Titan show the bright and dark regions in greater detail but have yet to resolve the question of whether there are liquids on the surface.

Methyl-coenzyme M reductase A as an indicator to estimate methane production from dairy cows.

PubMed

Aguinaga Casañas, M A; Rangkasenee, N; Krattenmacher, N; Thaller, G; Metges, C C; Kuhla, B

2015-06-01

The evaluation of greenhouse gas mitigation strategies requires the quantitative assessment of individual methane production. Because methane measurement in respiration chambers is highly accurate, but also comprises various disadvantages such as limited capacity and high costs, the establishment of an indicator for estimating methane production of individual ruminants would provide an alternative to direct methane measurement. Methyl-coenzyme M reductase is involved in methanogenesis and the subunit α of methyl-coenzyme M reductase is encoded by the mcrA gene of rumen archaea. We therefore examined the relationship between methane emissions of Holstein dairy cows measured in respiration chambers with 2 different diets (high- and medium-concentrate diet) and the mcrA DNA and mcrA cDNA abundance determined from corresponding rumen fluid samples. Whole-body methane production per kilogram of dry matter intake and mcrA DNA normalized to the abundance of the rrs gene coding for 16S rRNA correlated significantly when using qmcrA primers. Use of qmcrA primers also revealed linear correlation between mcrA DNA copy number and methane yield. Regression analyses based on normalized mcrA cDNA abundances revealed no significant linear correlation with methane production per kilogram of dry matter intake. Furthermore, the correlations between normalized mcrA DNA abundance and the rumen fluid concentration of acetic and isobutyric acid were positive, whereas the correlations with propionic and lactic acid were negative. These data suggest that the mcrA DNA approach based on qmcrA primers could potentially be a molecular proxy for methane yield after further refinement. Copyright © 2015 American Dairy Science Association. Published by Elsevier Inc. All rights reserved.

Methane-rich syngas production from hydrocarbon fuels using multi-functional catalyst/capture agent

DOEpatents

Siefert, Nicholas S.; Shekhawat, Dushyant; Berry, David A.; Surdoval, Wayne A.

2017-02-07

The disclosure provides a gasification process for the production of a methane-rich syngas at temperatures exceeding 400.degree. C. through the use of an alkali hydroxide MOH, using a gasification mixture comprised of at least 0.25 moles and less than 2 moles of water for each mole of carbon, and at least 0.15 moles and less than 2 moles of alkali hydroxide MOH for each mole of carbon. These relative amounts allow the production of a methane-rich syngas at temperatures exceeding 400.degree. C. by enabling a series of reactions which generate H.sub.2 and CH.sub.4, and mitigate the reforming of methane. The process provides a methane-rich syngas comprised of roughly 20% (dry molar percentage) CH.sub.4 at temperatures above 400.degree. C., and may effectively operate within an IGFC cycle at reactor temperatures between 400-900.degree. C. and pressures in excess of 10 atmospheres.

Characterizing Methane Emissions at Local Scales with a 20 Year Total Hydrocarbon Time Series, Imaging Spectrometry, and Web Facilitated Analysis

NASA Astrophysics Data System (ADS)

Bradley, Eliza Swan

Methane is an important greenhouse gas for which uncertainty in local emission strengths necessitates improved source characterizations. Although CH4 plume mapping did not motivate the NASA Airborne Visible InfraRed Imaging Spectrometer (AVIRIS) design and municipal air quality monitoring stations were not intended for studying marine geological seepage, these assets have capabilities that can make them viable for studying concentrated (high flux, highly heterogeneous) CH4 sources, such as the Coal Oil Point (COP) seep field (˜0.015 Tg CH4 yr-1) offshore Santa Barbara, California. Hourly total hydrocarbon (THC) data, spanning 1990 to 2008 from an air pollution station located near COP, were analyzed and showed geologic CH4 emissions as the dominant local source. A band ratio approach was developed and applied to high glint AVIRIS data over COP, resulting in local-scale mapping of natural atmospheric CH4 plumes. A Cluster-Tuned Matched Filter (CTMF) technique was applied to Gulf of Mexico AVIRIS data to detect CH4 venting from offshore platforms. Review of 744 platform-centered CTMF subsets was facilitated through a flexible PHP-based web portal. This dissertation demonstrates the value of investigating municipal air quality data and imaging spectrometry for gathering insight into concentrated methane source emissions and highlights how flexible web-based solutions can help facilitate remote sensing research.

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.

40 CFR 86.521-90 - Hydrocarbon analyzer calibration.

Code of Federal Regulations, 2014 CFR

2014-07-01

.... Analyzers used with petroleum fuels and liquefied petroleum gas-fuel shall be optimized using propane. Analyzers used with natural gas-fuel for measurement of hydrocarbons shall be optimized using methane. If a... gas-fuel. Alternate methods yielding equivalent results may be used, if approved in advance by the...

40 CFR 86.521-90 - Hydrocarbon analyzer calibration.

Code of Federal Regulations, 2012 CFR

2012-07-01

.... Analyzers used with petroleum fuels and liquefied petroleum gas-fuel shall be optimized using propane. Analyzers used with natural gas-fuel for measurement of hydrocarbons shall be optimized using methane. If a... gas-fuel. Alternate methods yielding equivalent results may be used, if approved in advance by the...

40 CFR 86.521-90 - Hydrocarbon analyzer calibration.

Code of Federal Regulations, 2013 CFR

2013-07-01

.... Analyzers used with petroleum fuels and liquefied petroleum gas-fuel shall be optimized using propane. Analyzers used with natural gas-fuel for measurement of hydrocarbons shall be optimized using methane. If a... gas-fuel. Alternate methods yielding equivalent results may be used, if approved in advance by the...

Air Quality measurements near the Gulf of Mexico Deep Water Horizon Oil Spill site in July 2010

NASA Astrophysics Data System (ADS)

Schade, G. W.; Rasmussen, R.; Conlee, D.; Seroka, G.; Delao, D.

2010-12-01

Eight whole air samples were acquired within several kilometers of the Deepwater Horizon well head location between 5 and 13 July 2010. A Teflon coated pump was used to pressurize 0.8 L volume stainless steel canisters to approximately 2 bar. Various amounts of oil were visible on the water surface during most sampling times, and some samples were accompanied by strong hydrocarbon smells. The air samples were analyzed over the next two months using high sensitivity GC-FID and GC-MS methods for C1-C30 hydrocarbons and selected hetero-atomic compounds. Highest concentrations reached several ppm for total hydrocarbons, comparable to concentrations in highway road tunnels. None of the samples showed elevated concentrations suggestive of hazardous concentrations, or near OSHA PEL or NIOSH REL levels. Consistent with studies of seawater methane concentrations at different depths, atmospheric methane mixing ratios were close to background abundances at 1.75-1.78 ppm, suggesting that the spill’s methane emissions had not reached the surface at that time. Non-methane hydrocarbons presented a highly complex mixture (100+ species) of dominantly alkanes, as expected. Linear alkanes were detected at elevated mixing ratios from C4 up to C30, and were dominated by nonane (C9). Aromatic hydrocarbons showed a pattern suggestive of a significant retention by seawater of benzene and toluene, the compounds with the highest water solubilities. While benzene was hardly and toluene only slightly elevated, lower solubility compounds such as the xylenes and naphthalene were clearly elevated. Data will be presented relative to an upwind sample taken on 5 July.

Estimating Emissions of Toxic Hydrocarbons from Natural Gas Production Sites in the Barnett Shale Region of Northern Texas.

PubMed

Marrero, Josette E; Townsend-Small, Amy; Lyon, David R; Tsai, Tracy R; Meinardi, Simone; Blake, Donald R

2016-10-04

Oil and natural gas operations have continued to expand and move closer to densely populated areas, contributing to growing public concerns regarding exposure to hazardous air pollutants. During the Barnett Shale Coordinated Campaign in October, 2013, ground-based whole air samples collected downwind of oil and gas sites revealed enhancements in several potentially toxic volatile organic compounds (VOCs) when compared to background values. Molar emissions ratios relative to methane were determined for hexane, benzene, toluene, ethylbenzene, and xylene (BTEX compounds). Using methane leak rates measured from the Picarro mobile flux plane (MFP) system and a Barnett Shale regional methane emissions inventory, the rates of emission of these toxic gases were calculated. Benzene emissions ranged between 51 ± 4 and 60 ± 4 kg h -1 . Hexane, the most abundantly emitted pollutant, ranged from 642 ± 45 to 1070 ± 340 kg h -1 . While observed hydrocarbon enhancements fall below federal workplace standards, results may indicate a link between emissions from oil and natural gas operations and concerns about exposure to hazardous air pollutants. The larger public health risks associated with the production and distribution of natural gas are of particular importance and warrant further investigation, particularly as the use of natural gas increases in the United States and internationally.

On the Theory of Accumulation of Hydrocarbons in a Dome Used to Eliminate a Technogenic Spill at the Bottom of the Ocean

NASA Astrophysics Data System (ADS)

Gimaltdinov, I. K.; Kil'dibaeva, S. R.

2018-01-01

Consideration is given to the operation of a dome separator installed at the bottom of the World Ocean and intended to eliminate the effects of technogenic spill of hydrocarbons. It is assumed that oil and gas (methane) escape from the damaged well on the ocean floor. Under the conditions of stable existence of a hydrate, a hydration sheath is formed on the surface of methane bubbles. To collect the entering hydrocarbons, a dome from a soft polyurethane shell is installed above the spill site, inside which the hydrocarbons are accumulated. In the regime of steady-state operation of the dome, provision is made for pumping out of hydrocarbons for transportation and further utilization. In the work, temperature fields of the hydrocarbon layers accumulated in the dome are investigated.

Non-linear dynamics of stable carbon and hydrogen isotope signatures based on a biological kinetic model of aerobic enzymatic methane oxidation.

PubMed

Vavilin, Vasily A; Rytov, Sergey V; Shim, Natalia; Vogt, Carsten

2016-06-01

The non-linear dynamics of stable carbon and hydrogen isotope signatures during methane oxidation by the methanotrophic bacteria Methylosinus sporium strain 5 (NCIMB 11126) and Methylocaldum gracile strain 14 L (NCIMB 11912) under copper-rich (8.9 µM Cu(2+)), copper-limited (0.3 µM Cu(2+)) or copper-regular (1.1 µM Cu(2+)) conditions has been described mathematically. The model was calibrated by experimental data of methane quantities and carbon and hydrogen isotope signatures of methane measured previously in laboratory microcosms reported by Feisthauer et al. [ 1 ] M. gracile initially oxidizes methane by a particulate methane monooxygenase and assimilates formaldehyde via the ribulose monophosphate pathway, whereas M. sporium expresses a soluble methane monooxygenase under copper-limited conditions and uses the serine pathway for carbon assimilation. The model shows that during methane solubilization dominant carbon and hydrogen isotope fractionation occurs. An increase of biomass due to growth of methanotrophs causes an increase of particulate or soluble monooxygenase that, in turn, decreases soluble methane concentration intensifying methane solubilization. The specific maximum rate of methane oxidation υm was proved to be equal to 4.0 and 1.3 mM mM(-1) h(-1) for M. sporium under copper-rich and copper-limited conditions, respectively, and 0.5 mM mM(-1) h(-1) for M. gracile. The model shows that methane oxidation cannot be described by traditional first-order kinetics. The kinetic isotope fractionation ceases when methane concentrations decrease close to the threshold value. Applicability of the non-linear model was confirmed by dynamics of carbon isotope signature for carbon dioxide that was depleted and later enriched in (13)C. Contrasting to the common Rayleigh linear graph, the dynamic curves allow identifying inappropriate isotope data due to inaccurate substrate concentration analyses. The non-linear model pretty adequately described experimental

Understanding the physiological and molecular mechanisms of rice-microbial interactions that produce methane

USDA-ARS?s Scientific Manuscript database

The second most abundant greenhouse gas, methane, is ~25 times more potent in global warming potential than carbon dioxide, and 7-17% of atmospheric methane comes from flooded rice fields. Methane emissions can be greatly reduced by using alternate wetting and drying irrigation management and/or cul...

Methane Emissions from Upland Forests

NASA Astrophysics Data System (ADS)

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

2016-04-01

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

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

Transpiration cooled throat for hydrocarbon rocket engines

NASA Technical Reports Server (NTRS)

May, Lee R.; Burkhardt, Wendel M.

1991-01-01

The objective for the Transpiration Cooled Throat for Hydrocarbon Rocket Engines Program was to characterize the use of hydrocarbon fuels as transpiration coolants for rocket nozzle throats. The hydrocarbon fuels investigated in this program were RP-1 and methane. To adequately characterize the above transpiration coolants, a program was planned which would (1) predict engine system performance and life enhancements due to transpiration cooling of the throat region using analytical models, anchored with available data; (2) a versatile transpiration cooled subscale rocket thrust chamber was designed and fabricated; (3) the subscale thrust chamber was tested over a limited range of conditions, e.g., coolant type, chamber pressure, transpiration cooled length, and coolant flow rate; and (4) detailed data analyses were conducted to determine the relationship between the key performance and life enhancement variables.

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.

Hydrocarbon Emission from Oil and Gas Production Activity in Northeastern Oklahoma - Wintertime Measurements in 2015 and 2016

NASA Astrophysics Data System (ADS)

Ghosh, B.

2016-12-01

Hydrocarbons can be emitted into the atmosphere from various sources and play a crucial role in local and regional air quality through formation of secondary pollutants such as ozone and particulate matter. Understanding their sources and their potential air quality impact is essential for effective environmental policymaking. A ground based ambient air measurement campaign was conducted in February-March of 2016 at the Phillips 66 Research Center in Northeastern Oklahoma to study ambient hydrocarbons in the region, understand their sources, as well as estimate their air quality impact. This study is a follow-up to a study conducted during the same time in 2015 and aims to understand the variation of hydrocarbons levels in ambient air over time and the corresponding air quality impact. Various trace gases were measured using a suite of instrumentation. Non-methane hydrocarbons (NMHCs) were sampled using two-hour time integrated whole air sampling. A total of 375 air samples were collected during the study and were analyzed offline with GC-MS (Agilent) following cold-trap dehydration (Entech Instruments). In addition, higher time resolution measurement of methane, ethane, CO, CO2, N2O, and H2O was achieved by a 1Hz Dual QCL Monitor (Aerodyne) along with a 0.1 Hz ozone monitor (2B Technologies). Levels of methane of 7 ppm and above were observed in this study. Among NMHCs, C2-C5 alkanes were the most dominant with their mean concentrations ranging from 1.9 to 17 ppb (Figure 1). Chemical tracers (ethane, propane, ethyne, CO) and isomeric ratios (i-C5/ n-C5) suggest that oil and gas production activity probably was the source of hydrocarbon emissions measured in this study. Photochemical age was determined using hydrocarbon ratios and its significance will be discussed. While the 2016 winter was warmer compared to 2015, overall levels of NMHCs are higher in 2016 compared to 2015 and have a different distribution in mixing ratios. The results from 2016 study will be

40 CFR 86.005-10 - Emission standards for 2005 and later model year Otto-cycle heavy-duty engines and vehicles.

Code of Federal Regulations, 2013 CFR

2013-07-01

... Non-methane Hydrocarbon Equivalent (NO X + NMHCE) for engines fueled with methanol. 1.0 grams per... megajoule). (ii) Oxides of Nitrogen plus Non-methane Hydrocarbon Equivalent (NO X + NMHCE) for engines... Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW...

40 CFR 86.005-10 - Emission standards for 2005 and later model year Otto-cycle heavy-duty engines and vehicles.

Code of Federal Regulations, 2012 CFR

2012-07-01

... Non-methane Hydrocarbon Equivalent (NO X + NMHCE) for engines fueled with methanol. 1.0 grams per... megajoule). (ii) Oxides of Nitrogen plus Non-methane Hydrocarbon Equivalent (NO X + NMHCE) for engines... Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW...

Root biomass as a major means of affecting methane emissions

USDA-ARS?s Scientific Manuscript database

Human activities are contributing to greenhouse gas emissions. Methane, the second most abundant greenhouse gas, is ~25 times more potent in global warming potential than carbon dioxide, and 7-17% of atmospheric methane comes from paddy rice fields. The purpose of the study was to investigate gene...

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.

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.

An analytical solubility model for nitrogen-methane-ethane ternary mixtures

NASA Astrophysics Data System (ADS)

Hartwig, Jason; Meyerhofer, Peter; Lorenz, Ralph; Lemmon, Eric

2018-01-01

Saturn's moon Titan has surface liquids of liquid hydrocarbons and a thick, cold, nitrogen atmosphere, and is a target for future exploration. Critical to the design and operation of vehicles for this environment is knowledge of the amount of dissolved nitrogen gas within the cryogenic liquid methane and ethane seas. This paper rigorously reviews experimental data on the vapor-liquid equilibrium of nitrogen/methane/ethane mixtures, noting the possibility for split liquid phases, and presents simple analytical models for conveniently predicting solubility of nitrogen in pure liquid ethane, pure liquid methane, and a mixture of liquid ethane and methane. Model coefficients are fit to three temperature ranges near the critical point, intermediate range, and near the freezing point to permit accurate predictions across the full range of thermodynamic conditions. The models are validated against the consolidated database of 2356 experimental data points, with mean absolute error between data and model less than 8% for both binary nitrogen/methane and nitrogen/ethane systems, and less than 17% for the ternary nitrogen/methane/ethane system. The model can be used to predict the mole fractions of ethane, methane, and nitrogen as a function of location within the Titan seas.

Spatial Structure and Activity of Sedimentary Microbial Communities Underlying a Beggiatoa spp. Mat in a Gulf of Mexico Hydrocarbon Seep

PubMed Central

Lloyd, Karen G.; Albert, Daniel B.; Biddle, Jennifer F.; Chanton, Jeffrey P.; Pizarro, Oscar; Teske, Andreas

2010-01-01

Background Subsurface fluids from deep-sea hydrocarbon seeps undergo methane- and sulfur-cycling microbial transformations near the sediment surface. Hydrocarbon seep habitats are naturally patchy, with a mosaic of active seep sediments and non-seep sediments. Microbial community shifts and changing activity patterns on small spatial scales from seep to non-seep sediment remain to be examined in a comprehensive habitat study. Methodology/Principal Findings We conducted a transect of biogeochemical measurements and gene expression related to methane- and sulfur-cycling at different sediment depths across a broad Beggiatoa spp. mat at Mississippi Canyon 118 (MC118) in the Gulf of Mexico. High process rates within the mat (∼400 cm and ∼10 cm from the mat's edge) contrasted with sharply diminished activity at ∼50 cm outside the mat, as shown by sulfate and methane concentration profiles, radiotracer rates of sulfate reduction and methane oxidation, and stable carbon isotopes. Likewise, 16S ribosomal rRNA, dsrAB (dissimilatory sulfite reductase) and mcrA (methyl coenzyme M reductase) mRNA transcripts of sulfate-reducing bacteria (Desulfobacteraceae and Desulfobulbaceae) and methane-cycling archaea (ANME-1 and ANME-2) were prevalent at the sediment surface under the mat and at its edge. Outside the mat at the surface, 16S rRNA sequences indicated mostly aerobes commonly found in seawater. The seep-related communities persisted at 12–20 cm depth inside and outside the mat. 16S rRNA transcripts and V6-tags reveal that bacterial and archaeal diversity underneath the mat are similar to each other, in contrast to oxic or microoxic habitats that have higher bacterial diversity. Conclusions/Significance The visual patchiness of microbial mats reflects sharp discontinuities in microbial community structure and activity over sub-meter spatial scales; these discontinuities have to be taken into account in geochemical and microbiological inventories of seep environments. In

Subduction zone earthquake probably triggered submarine hydrocarbon seepage offshore Pakistan

NASA Astrophysics Data System (ADS)

Fischer, David; José M., Mogollón; Michael, Strasser; Thomas, Pape; Gerhard, Bohrmann; Noemi, Fekete; Volkhard, Spiess; Sabine, Kasten

2014-05-01

Seepage of methane-dominated hydrocarbons is heterogeneous in space and time, and trigger mechanisms of episodic seep events are not well constrained. It is generally found that free hydrocarbon gas entering the local gas hydrate stability field in marine sediments is sequestered in gas hydrates. In this manner, gas hydrates can act as a buffer for carbon transport from the sediment into the ocean. However, the efficiency of gas hydrate-bearing sediments for retaining hydrocarbons may be corrupted: Hypothesized mechanisms include critical gas/fluid pressures beneath gas hydrate-bearing sediments, implying that these are susceptible to mechanical failure and subsequent gas release. Although gas hydrates often occur in seismically active regions, e.g., subduction zones, the role of earthquakes as potential triggers of hydrocarbon transport through gas hydrate-bearing sediments has hardly been explored. Based on a recent publication (Fischer et al., 2013), we present geochemical and transport/reaction-modelling data suggesting a substantial increase in upward gas flux and hydrocarbon emission into the water column following a major earthquake that occurred near the study sites in 1945. Calculating the formation time of authigenic barite enrichments identified in two sediment cores obtained from an anticlinal structure called "Nascent Ridge", we find they formed 38-91 years before sampling, which corresponds well to the time elapsed since the earthquake (62 years). Furthermore, applying a numerical model, we show that the local sulfate/methane transition zone shifted upward by several meters due to the increased methane flux and simulated sulfate profiles very closely match measured ones in a comparable time frame of 50-70 years. We thus propose a causal relation between the earthquake and the amplified gas flux and present reflection seismic data supporting our hypothesis that co-seismic ground shaking induced mechanical fracturing of gas hydrate-bearing sediments

40 CFR 86.1815-01 - Emission standards for light-duty trucks 4.

Code of Federal Regulations, 2013 CFR

2013-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1816-05 - Emission standards for complete heavy-duty vehicles.

Code of Federal Regulations, 2010 CFR

2010-07-01

... references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a) Exhaust emission... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1813-01 - Emission standards for light-duty trucks 2.

Code of Federal Regulations, 2011 CFR

2011-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1812-01 - Emission standards for light-duty trucks 1.

Code of Federal Regulations, 2011 CFR

2011-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1815-02 - Emission standards for light-duty trucks 4.

Code of Federal Regulations, 2013 CFR

2013-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1813-01 - Emission standards for light-duty trucks 2.

Code of Federal Regulations, 2010 CFR

2010-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1814-01 - Emission standards for light-duty trucks 3.

Code of Federal Regulations, 2012 CFR

2012-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1811-01 - Emission standards for light-duty vehicles.

Code of Federal Regulations, 2012 CFR

2012-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1814-02 - Emission standards for light-duty trucks 3.

Code of Federal Regulations, 2013 CFR

2013-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1812-01 - Emission standards for light-duty trucks 1.

Code of Federal Regulations, 2012 CFR

2012-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1816-05 - Emission standards for complete heavy-duty vehicles.

Code of Federal Regulations, 2011 CFR

2011-07-01

... references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a) Exhaust emission... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1815-01 - Emission standards for light-duty trucks 4.

Code of Federal Regulations, 2011 CFR

2011-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1815-01 - Emission standards for light-duty trucks 4.

Code of Federal Regulations, 2010 CFR

2010-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1814-01 - Emission standards for light-duty trucks 3.

Code of Federal Regulations, 2010 CFR

2010-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1816-05 - Emission standards for complete heavy-duty vehicles.

Code of Federal Regulations, 2013 CFR

2013-07-01

... references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a) Exhaust emission... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1813-01 - Emission standards for light-duty trucks 2.

Code of Federal Regulations, 2012 CFR

2012-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1811-01 - Emission standards for light-duty vehicles.

Code of Federal Regulations, 2011 CFR

2011-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1816-05 - Emission standards for complete heavy-duty vehicles.

Code of Federal Regulations, 2012 CFR

2012-07-01

... references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a) Exhaust emission... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1811-01 - Emission standards for light-duty vehicles.

Code of Federal Regulations, 2013 CFR

2013-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1814-01 - Emission standards for light-duty trucks 3.

Code of Federal Regulations, 2013 CFR

2013-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1814-02 - Emission standards for light-duty trucks 3.

Code of Federal Regulations, 2011 CFR

2011-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1812-01 - Emission standards for light-duty trucks 1.

Code of Federal Regulations, 2013 CFR

2013-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1815-02 - Emission standards for light-duty trucks 4.

Code of Federal Regulations, 2011 CFR

2011-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1814-02 - Emission standards for light-duty trucks 3.

Code of Federal Regulations, 2012 CFR

2012-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1814-01 - Emission standards for light-duty trucks 3.

Code of Federal Regulations, 2011 CFR

2011-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1812-01 - Emission standards for light-duty trucks 1.

Code of Federal Regulations, 2010 CFR

2010-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1816-05 - Emission standards for complete heavy-duty vehicles.

Code of Federal Regulations, 2014 CFR

2014-07-01

... references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a) Exhaust emission... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty Vehicles, Light...

40 CFR 86.1813-01 - Emission standards for light-duty trucks 2.

Code of Federal Regulations, 2013 CFR

2013-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1815-02 - Emission standards for light-duty trucks 4.

Code of Federal Regulations, 2012 CFR

2012-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1814-02 - Emission standards for light-duty trucks 3.

Code of Federal Regulations, 2010 CFR

2010-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1811-01 - Emission standards for light-duty vehicles.

Code of Federal Regulations, 2010 CFR

2010-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1815-02 - Emission standards for light-duty trucks 4.

Code of Federal Regulations, 2010 CFR

2010-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. This... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1815-01 - Emission standards for light-duty trucks 4.

Code of Federal Regulations, 2012 CFR

2012-07-01

... equivalents and references to non-methane hydrocarbons shall mean non-methane hydrocarbon equivalents. (a... (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty...

40 CFR 86.1342-94 - Calculations; exhaust emissions.

Code of Federal Regulations, 2011 CFR

2011-07-01

..., if appropriate, the weighted mass total hydrocarbon equivalent, formaldehyde, or non-methane... PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED... see § 86.1342-90. (b)(8) Non-methane hydrocarbon mass: NMHCmass = Vmix × DensityNMHC × (NMHCconc/1,000...

40 CFR 86.005-10 - Emission standards for 2005 and later model year Otto-cycle heavy-duty engines and vehicles.

Code of Federal Regulations, 2014 CFR

2014-07-01

... megajoule). (B) Oxides of Nitrogen plus Non-methane Hydrocarbon Equivalent (NO X + NMHCE) for engines fueled... Nitrogen plus Non-methane Hydrocarbon Equivalent (NO X + NMHCE) for engines fueled with methanol. 1.5 grams... Environment ENVIRONMENTAL PROTECTION AGENCY (CONTINUED) AIR PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW...

40 CFR 86.1342-94 - Calculations; exhaust emissions.

Code of Federal Regulations, 2010 CFR

2010-07-01

..., if appropriate, the weighted mass total hydrocarbon equivalent, formaldehyde, or non-methane... PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED... see § 86.1342-90. (b)(8) Non-methane hydrocarbon mass: NMHCmass = Vmix × DensityNMHC × (NMHCconc/1,000...

40 CFR 86.1342-94 - Calculations; exhaust emissions.

Code of Federal Regulations, 2013 CFR

2013-07-01

..., if appropriate, the weighted mass total hydrocarbon equivalent, formaldehyde, or non-methane... PROGRAMS (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED... see § 86.1342-90. (b)(8) Non-methane hydrocarbon mass: NMHCmass = Vmix × DensityNMHC × (NMHCconc/1,000...

Hydrocarbon gas seeps of the convergent Hikurangi margin, North Island, New Zealand

USGS Publications Warehouse

Kvenvolden, K.A.; Pettinga, J.R.

1989-01-01

Two hydrocarbon gas seeps, located about 13 km apart, have distinctive molecular and isotopic compositions. These seeps occur within separate tectonic melange units of narrow parallel trending and structurally complex zones with incorporated upper Cretaceous and Palaeogene passive continental margin deposits which are now compressively deformed and imbricated along the convergent Hikurangi margin of North Island, New Zealand. At Brookby Station within the Coastal High, the seeping hydrocarbon gas has a methane/ethane ratio of 48 and ??13C and ??D values of methane of -45.7 and -188???, respectively (relative to the PDB and SMOW standards). Within the complex core of the Elsthorpe Anticline at Campbell Station seep, gas has a methane/ethane ratio of about 12000, and the methane has ??13C and ??D values of -37.4 and -170???, respectively. The source of the gases cannot be positively identified, but the gases probably originate from the thermal decomposition of organic matter in tectonically disturbed upper Cretaceous and/or lower Tertiary sedimentary rocks of passive margin affinity and reach the surface by migration along thrust faults associated with tectonic melange. The geochemical differences between the two gases may result from differences in burial depths of similar source sediment. ?? 1989.

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

Anaerobic methane oxidation in low-organic content methane seep sediments

USGS Publications Warehouse

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

2013-01-01

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

The direct aromatization of methane

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

Marcelin, G.; Oukaci, R.; Migone, R.A.

1995-12-31

The thermal decomposition of methane shows significant potential as a process for the production of higher unsaturated and aromatic hydrocarbons when the extent of the reaction is limited. Thermodynamic calculations have shown that when the reaction is limited to the formation of C{sub 2} to C{sub 10} products, yields of aromatics can exceed 40% at temperatures of 1200{degrees}C. Preliminary experiments have shown that when the reaction is limited to the formation of C{sub 2} to C{sub 10} products, yields of aromatics can exceed 40% at temperatures of 1200{degrees}C. Preliminary experiments have shown that cooling the product and reacting gases asmore » the reaction proceeds can significantly reduce or eliminate the formation of solid carbon and heavier (C{sub 10+}) materials. Much work remains to be done in optimizing the quenching process and this is one of the goals of this program. Means to lower the temperature of the reaction are being studied as this result in a more feasible commercial process due to savings realized in energy and material of construction costs. The use of free-radical generators and catalysts will be investigated as a means of lowering the reaction temperature thus allowing faster quenching. It is highly likely that such studies will lead to a successful direct methane to higher hydrocarbon process.« less

[Atmospheric non-methane hydrocarbons near plants of crude oil first treatment].

PubMed

Bustaffa, Elisa; De Marinis Loiotile, Annamaria; Farella, Genoveffa; Petraccone, Stefania; De Gennaro, Gianluigi; Bianchi, Fabrizio

2016-01-01

La continua espansione delle attività di perforazione ai fini dell'estrazione petrolifera in prossimità di aree abitate ha fatto sì che negli ultimi anni l'attenzione si focalizzasse sull'impatto di questo processo fortemente industrializzato sulla salute pubblica. Le comunità che vivono nei dintorni di impianti di questo tipo devono, infatti, fronteggiare diversi problemi, quali l'inquinamento atmosferico e acustico, la contaminazione del suolo e delle acque sotterranee, il traffico dei camion da e verso il sito, incidenti e malfunzionamenti all'interno dell'impianto. In questo contesto, la valutazione del rischio per la salute è ostacolata dal fatto che l'esposizione alle sostanze chimiche presenti non può essere valutata in via definitiva, poiché non sempre si è a conoscenza di tutti i composti immessi nell'ambiente né delle loro concentrazioni, per non parlare del problema delle coesposizioni ad altri inquinanti. Nonostante l'oramai conclamato e vasto interesse generato da questo argomento, ad oggi esistono pochi studi basati su popolazioni riguardanti gli effetti sulla salute delle comunità che vivono in prossimità dei siti di perforazione ed estrazione; ciò genera la necessità di condurre campagne di monitoraggio mirate e studi epidemiologici che verifichino l'eventuale esistenza e natura di pattern di malattie associati a tali attività. La presente rassegna bibliografica individua, quindi, i principali inquinanti atmosferici presenti in prossimità di un impianto di primo trattamento del greggio e cerca di fornire un quadro generale delle loro potenziali sorgenti e caratteristiche.

Structure, function and carcinogenicity of metabolites of methylated and non-methylated polycyclic aromatic hydrocarbons: a comprehensive review.

PubMed

Flesher, James W; Lehner, Andreas F

2016-01-01

The Unified Theory of PAH Carcinogenicity accommodates the activities of methylated and non-methylated polycyclic aromatic hydrocarbons (PAHs) and states that substitution of methyl groups on meso-methyl substituted PAHs with hydroxy, acetoxy, chloride, bromide or sulfuric acid ester groups imparts potent cancer producing properties. It incorporates specific predictions from past researchers on the mechanism of carcinogenesis by methyl-substituted hydrocarbons, including (1) requirement for metabolism to an ArCH2X type structure where X is a good leaving group and (2) biological substitution of a meso-methyl group at the most reactive center in non-methylated hydrocarbons. The Theory incorporates strong inferences of Fieser: (1) The mechanism of carcinogenesis involves a specific metabolic substitution of a hydrocarbon at its most reactive center and (2) Metabolic elimination of a carcinogen is a detoxifying process competitive with that of carcinogenesis and occurring by a different mechanism. According to this outlook, chemical or biochemical substitution of a methyl group at the reactive meso-position of non-methylated hydrocarbons is the first step in the mechanism of carcinogenesis for most, if not all, PAHs and the most potent metabolites of PAHs are to be found among the meso methyl-substituted hydrocarbons. Some PAHs and their known or potential metabolites and closely related compounds have been tested in rats for production of sarcomas at the site of subcutaneous injection and the results strongly support the specific predictions of the Unified Theory.

Some advantages of methane in an aircraft gas turbine

NASA Technical Reports Server (NTRS)

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

1980-01-01

Because liquid methane may be obtained from existing natural gas sources or produced synthetically from a range of other hydrocarbon sources (coal, biomass, shale, organic waste), it is considered as an aviation fuel in a simplified cycle analysis of the performance of a turboprop engine intended for operation at Mach 0.8 and 10,688 m altitude. Performance comparisons are given for four cases in which the turbine cooling air is either not cooled or cooled to -111, -222, and -333 K, and the advantages and problems that may be expected from direct use of the cryogenic fuel in turbine cooling are discussed. It is shown that while (1) methane combustion characteristics are appreciably different from those of Jet A fuel and will require the development of different combustor designs, and (2) the safe integration of methane cryotanks into transport aircraft structures poses a major design problem, a highly fuel-efficient turboprop engine fueled by methane appears to be feasible.

CARS technique for geological exploration of hydrocarbons deposits

NASA Astrophysics Data System (ADS)

Zhevlakov, A. P.; Bespalov, Victor; Elizarov, V. V.; Grishkanich, A. S.; Kascheev, S. V.; Makarov, E. A.; Bogoslovsky, S. A.; Il'inskiy, A. A.

2014-10-01

We developed a Raman lidar with ultraspectral resolution for automatic airborne monitoring of pipeline leaks and for oil and gas exploration. Experiments were carried out under the CARS circuit. Minimal concentrations of 200 ppb of heavy hydrocarbon gas have been remotely measured in laboratory tests. Test flights indicate that a sensitivity of 6 ppm for methane and 2 ppm for hydrogen sulfide has been reached for leakage detection. As estimations have shown the reliability of heavy hydrocarbon gas detection by the integration method of seismic prospecting and remote laser sensing in CARS circuit can exceed 80%.

40 CFR 86.007-11 - Emission standards and supplemental requirements for 2007 and later model year diesel heavy-duty...

Code of Federal Regulations, 2011 CFR

2011-07-01

... family are derived from averaging, banking, or trading programs. (ii)(A) Non-Methane Hydrocarbons (NMHC... brake horsepower-hour (0.052 grams per megajoule). (B) Non-Methane Hydrocarbon Equivalent (NMHCE) for... of the given hardware and lead time and production cycles including phase-in or phase-out of engines...

40 CFR 86.007-11 - Emission standards and supplemental requirements for 2007 and later model year diesel heavy-duty...

Code of Federal Regulations, 2013 CFR

2013-07-01

... family are derived from averaging, banking, or trading programs. (ii)(A) Non-Methane Hydrocarbons (NMHC... brake horsepower-hour (0.052 grams per megajoule). (B) Non-Methane Hydrocarbon Equivalent (NMHCE) for... of the given hardware and lead time and production cycles including phase-in or phase-out of engines...

40 CFR 86.007-11 - Emission standards and supplemental requirements for 2007 and later model year diesel heavy-duty...

Code of Federal Regulations, 2010 CFR

2010-07-01

... family are derived from averaging, banking, or trading programs. (ii)(A) Non-Methane Hydrocarbons (NMHC... brake horsepower-hour (0.052 grams per megajoule). (B) Non-Methane Hydrocarbon Equivalent (NMHCE) for... of the given hardware and lead time and production cycles including phase-in or phase-out of engines...

40 CFR 86.007-11 - Emission standards and supplemental requirements for 2007 and later model year diesel heavy-duty...

Code of Federal Regulations, 2014 CFR

2014-07-01

... family are derived from averaging, banking, or trading programs. (ii)(A) Non-Methane Hydrocarbons (NMHC... brake horsepower-hour (0.052 grams per megajoule). (B) Non-Methane Hydrocarbon Equivalent (NMHCE) for... of the given hardware and lead time and production cycles including phase-in or phase-out of engines...

40 CFR 86.007-11 - Emission standards and supplemental requirements for 2007 and later model year diesel heavy-duty...

Code of Federal Regulations, 2012 CFR

2012-07-01

... family are derived from averaging, banking, or trading programs. (ii)(A) Non-Methane Hydrocarbons (NMHC... brake horsepower-hour (0.052 grams per megajoule). (B) Non-Methane Hydrocarbon Equivalent (NMHCE) for... of the given hardware and lead time and production cycles including phase-in or phase-out of engines...

40 CFR 86.1804-01 - Acronyms and abbreviations.

Code of Federal Regulations, 2013 CFR

2013-07-01

...—Nonmethane Hydrocarbons. NMHCE—Non-Methane Hydrocarbon Equivalent. NMOG—Non-methane organic gases. NO—nitric... (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty Vehicles, Light-Duty Trucks...

40 CFR 86.1804-01 - Acronyms and abbreviations.

Code of Federal Regulations, 2010 CFR

2010-07-01

...—Nonmethane Hydrocarbons. NMHCE—Non-Methane Hydrocarbon Equivalent. NMOG—Non-methane organic gases. NO—nitric... (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty Vehicles, Light-Duty Trucks...

40 CFR 86.1804-01 - Acronyms and abbreviations.

Code of Federal Regulations, 2011 CFR

2011-07-01

...—Nonmethane Hydrocarbons. NMHCE—Non-Methane Hydrocarbon Equivalent. NMOG—Non-methane organic gases. NO—nitric... (CONTINUED) CONTROL OF EMISSIONS FROM NEW AND IN-USE HIGHWAY VEHICLES AND ENGINES (CONTINUED) General Compliance Provisions for Control of Air Pollution From New and In-Use Light-Duty Vehicles, Light-Duty Trucks...

Constraints on hydrocarbon and organic acid abundances in hydrothermal fluids at the Von Damm vent field, Mid-Cayman Rise (Invited)

NASA Astrophysics Data System (ADS)

McDermott, J. M.; Seewald, J.; German, C. R.; Sylva, S. P.

2013-12-01

The generation of organic compounds in vent fluids has been of interest since the discovery of seafloor hydrothermal systems, due to implications for the sustenance of present-day microbial populations and their potential role in the origin of life on early Earth. Possible sources of organic compounds in hydrothermal systems include microbial production, thermogenic degradation of organic material, and abiotic synthesis. Abiotic organic synthesis reactions may occur during active circulation of seawater-derived fluids through the oceanic crust or within olivine-hosted fluid inclusions containing carbon-rich magmatic volatiles. H2-rich end-member fluids at the Von Damm vent field on the Mid-Cayman Rise, where fluid temperatures reach 226°C, provide an exciting opportunity to examine the extent of abiotic carbon transformations in a highly reducing system. Our results indicate multiple sources of carbon compounds in vent fluids at Von Damm. An ultramafic-influenced hydrothermal system located on the Mount Dent oceanic core complex at 2350 m depth, Von Damm vent fluids contain H2, CH4, and C2+ hydrocarbons in high abundance relative to basalt-hosted vent fields, and in similar abundance to other ultramafic-hosted systems, such as Rainbow and Lost City. The CO2 content and isotopic composition in end-member fluids are virtually identical to bottom seawater, suggesting that seawater DIC is unchanged during hydrothermal circulation of seawater-derived fluids. Accordingly, end-member CH4 that is present in slightly greater abundance than CO2 cannot be generated from reduction of aqueous CO2 during hydrothermal circulation. We postulate that CH4 and C2+ hydrocarbons that are abundantly present in Von Damm vent fluids reflect leaching of fluids from carbon- and H2-rich fluid inclusions hosted in plutonic rocks. Geochemical modeling of carbon speciation in the Von Damm fluids suggests that the relative abundances of CH4, C2+ hydrocarbons, and CO2 are consistent with

40 CFR 86.1321-94 - Hydrocarbon analyzer calibration.

Code of Federal Regulations, 2012 CFR

2012-07-01

... to be used for the analysis of natural gas-fueled vehicle hydrocarbon samples, the methane response... following initial and periodic calibration. The HFID used with petroleum-fueled, natural gas-fueled and liquefied petroleum gas-fueled diesel engines shall be operated to a set point ±10 °F (±5.5 °C) between 365...

40 CFR 86.1321-94 - Hydrocarbon analyzer calibration.

Code of Federal Regulations, 2013 CFR

2013-07-01

... to be used for the analysis of natural gas-fueled vehicle hydrocarbon samples, the methane response... following initial and periodic calibration. The HFID used with petroleum-fueled, natural gas-fueled and liquefied petroleum gas-fueled diesel engines shall be operated to a set point ±10 °F (±5.5 °C) between 365...

A new solar carbon abundance based on non-LTE CN molecular spectra

NASA Technical Reports Server (NTRS)

Mount, G. H.; Linsky, J. L.

1975-01-01

A detailed non-LTE analysis of solar CN spectra strongly suggest a revised carbon abundance for the sun. We recommend a value of log carbon abundance = 8.35 plus or minus 0.15 which is significantly lower than the presently accepted value of log carbon abundance = 8.55. This revision may have important consequences in astrophysics.

Can hydrocarbons entrapped in seep carbonates serve as gas geochemistry recorder?

NASA Astrophysics Data System (ADS)

Blumenberg, Martin; Pape, Thomas; Seifert, Richard; Bohrmann, Gerhard; Schlömer, Stefan

2018-04-01

The geochemistry of seep gases is useful for an understanding of the local petroleum system. Here it was tested whether individual light hydrocarbons in seep gases are representatively entrapped in authigenic carbonates that formed near active seep sites. If applicable, it would be possible to extract geochemical information not only on the origin but also on the thermal maturity of the hydrocarbon source rocks from the gases entrapped in carbonates in the past. Respective data could be used for a better understanding of paleoenvironments and might directly serve as calibration point for, amongst others, petroleum system modeling. For this approach, (sub)-recent seep carbonates from the Black Sea (Paleodnjepr region and Batumi seep area), two sites of the Campeche Knoll region in the Gulf of Mexico, and the Venere mud volcano (Mediterranean Sea) were selected. These seep carbonates derive from sites for which geochemical data on the currently seeping gases exist. During treatment with phosphoric acid, methane and higher hydrocarbons were released from all carbonates, but in low concentrations. Compositional studies demonstrate that the ratio of methane to the sum of higher hydrocarbons (C1/(C2+C3)) is (partly strongly) positively biased in the entrapped gas fraction. δ13C values of C1 were determined for all samples and, for the samples from the Gulf of Mexico and the Mediterranean Sea, also of C2 and C3. The present dataset from six seep sites indicates that information on the seeped methane can be—although with a scatter of several permil—recorded in seep carbonate matrices, but other valuable information like the composition and δ13C of ethane and propane appears to be modified or lost during, for example, enclosure or at an early stage of diagenesis.

Biogeochemistry of microbial coal-bed methane

USGS Publications Warehouse

Strc, D.; Mastalerz, Maria; Dawson, K.; MacAlady, J.; Callaghan, A.V.; Wawrik, B.; Turich, C.; Ashby, M.

2011-01-01

Microbial methane accumulations have been discovered in multiple coal-bearing basins over the past two decades. Such discoveries were originally based on unique biogenic signatures in the stable isotopic composition of methane and carbon dioxide. Basins with microbial methane contain either low-maturity coals with predominantly microbial methane gas or uplifted coals containing older, thermogenic gas mixed with more recently produced microbial methane. Recent advances in genomics have allowed further evaluation of the source of microbial methane, through the use of high-throughput phylogenetic sequencing and fluorescent in situ hybridization, to describe the diversity and abundance of bacteria and methanogenic archaea in these subsurface formations. However, the anaerobic metabolism of the bacteria breaking coal down to methanogenic substrates, the likely rate-limiting step in biogenic gas production, is not fully understood. Coal molecules are more recalcitrant to biodegradation with increasing thermal maturity, and progress has been made in identifying some of the enzymes involved in the anaerobic degradation of these recalcitrant organic molecules using metagenomic studies and culture enrichments. In recent years, researchers have attempted lab and subsurface stimulation of the naturally slow process of methanogenic degradation of coal. Copyright ?? 2011 by Annual Reviews. All rights reserved.

Crenothrix are major methane consumers in stratified lakes.

PubMed

Oswald, Kirsten; Graf, Jon S; Littmann, Sten; Tienken, Daniela; Brand, Andreas; Wehrli, Bernhard; Albertsen, Mads; Daims, Holger; Wagner, Michael; Kuypers, Marcel Mm; Schubert, Carsten J; Milucka, Jana

2017-09-01

Methane-oxidizing bacteria represent a major biological sink for methane and are thus Earth's natural protection against this potent greenhouse gas. Here we show that in two stratified freshwater lakes a substantial part of upward-diffusing methane was oxidized by filamentous gamma-proteobacteria related to Crenothrix polyspora. These filamentous bacteria have been known as contaminants of drinking water supplies since 1870, but their role in the environmental methane removal has remained unclear. While oxidizing methane, these organisms were assigned an 'unusual' methane monooxygenase (MMO), which was only distantly related to 'classical' MMO of gamma-proteobacterial methanotrophs. We now correct this assignment and show that Crenothrix encode a typical gamma-proteobacterial PmoA. Stable isotope labeling in combination swith single-cell imaging mass spectrometry revealed methane-dependent growth of the lacustrine Crenothrix with oxygen as well as under oxygen-deficient conditions. Crenothrix genomes encoded pathways for the respiration of oxygen as well as for the reduction of nitrate to N 2 O. The observed abundance and planktonic growth of Crenothrix suggest that these methanotrophs can act as a relevant biological sink for methane in stratified lakes and should be considered in the context of environmental removal of methane.

Methane oxidation in Saanich Inlet during summer stratification

NASA Technical Reports Server (NTRS)

Ward, B. B.; Kilpatrick, K. A.; Wopat, A. E.; Minnich, E. C.; Lidstrom, M. E.

1989-01-01

Saanich Inlet, British Columbia, an fjord on the southeast coast of Vancouver Island, typically stratifies in summer, leading to the formation of an oxic-anoxic interface in the water column and accumulation of methane in the deep water. The results of methane concentration measurements in the water column of the inlet at various times throughout the summer months in 1983 are presented. Methane gradients and calculated diffusive fluxes across the oxic-anoxic interface increased as the summer progressed. Methane distribution and consumption in Saanich Inlet were studied in more detail during August 1986. At this time, a typical summer stratification with an oxic-anoxic interface around 140 m was present. At the interface, steep gradients in nutrient concentrations, bacterial abundance and methane concentration were observed. Methane oxidation was detected in the aerobic surface waters and in the anaerobic deep layer, but highest rates occurred in a narrow layer at the oxic-anoxic interface. Estimated methane oxidation rates were suffcient to consume 100 percent of the methane provided by diffusive flux from the anoxic layer. Methane oxidation is thus a mechanism whereby atmospheric flux from anoxic waters is minimized.

Aqueous geochemistry of low molecular weight hydrocarbons at elevated temperatures and pressures: constraints from mineral buffered laboratory experiments

NASA Astrophysics Data System (ADS)

Seewald, Jeffrey S.

2001-05-01

molecular weight hydrocarbons and the production of methane-rich ("dry") natural gas. Evaluation of aqueous reaction products generated during the experiments within a thermodynamic framework indicates that alkane-alkene, alkene-ketone, and alkene-alcohol reactions attained metastable thermodynamic equilibrium states. This equilibrium included water and iron-bearing minerals, demonstrating the direct involvement of inorganic species as reactants during organic transformations. The high reactivity of water and iron-bearing minerals suggests that they represent abundant sources of hydrogen and oxygen available for the formation of hydrocarbons and oxygenated alteration products. Thus, variations in elemental kerogen composition may not accurately reflect the timing and extent of hydrocarbon, carbon dioxide, and organic acid generation in sedimentary basins. This study demonstrates that the stabilities of aqueous hydrocarbons are strongly influenced by inorganic sediment composition at elevated temperatures. Incorporation of such interactions into geochemical models will greatly improve prediction of the occurrence of hydrocarbons in natural environments over geologic time.

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.

Non-microbial methane emissions from soils

NASA Astrophysics Data System (ADS)

Wang, Bin; Hou, Longyu; Liu, Wei; Wang, Zhiping

2013-12-01

Traditionally, methane (CH4) is anaerobically formed by methanogenic archaea. However, non-microbial CH4 can also be produced from geologic processes, biomass burning, animals, plants, and recently identified soils. Recognition of non-microbial CH4 emissions from soils remains inadequate. To better understand this phenomenon, a series of laboratory incubations were conducted to examine effects of temperature, water, and hydrogen peroxide (H2O2) on CH4 emissions under both aerobic and anaerobic conditions using autoclaved (30 min, 121 °C) soils and aggregates (>2000 μm, A1; 2000-250 μm, A2; 250-53 μm, M1; and <53 μm, M2). Results show that applying autoclaving to pre-treat soils is effective to inhibit methanogenic activity, ensuring the CH4 emitted being non-microbial. Responses of non-microbial CH4 emissions to temperature, water, and H2O2 were almost identical between aerobic and anaerobic conditions. Increasing temperature, water of proper amount, and H2O2 could significantly enhance CH4 emissions. However, the emission rates were inhibited and enhanced by anaerobic conditions without and with the existence of H2O2, respectively. As regards the aggregates, aggregate-based emission presented an order of M1 > A2 > A1 > M2 and C-based emission an order of M2 > M1 > A1 > A2, demonstrating that both organic carbon quantity and property are responsible for CH4 emissions from soils at the scale of aggregate. Whole soil-based order of A2 > A1 > M1 > M2 suggests that non-microbial CH4 release from forest soils is majorly contributed by macro-aggregates (i.e., >250 μm). The underlying mechanism is that organic matter through thermal treatment, photolysis, or reactions with free radicals produce CH4, which, in essence, is identical with mechanisms of other non-microbial sources, indicating that non-microbial CH4 production may be a widespread phenomenon in nature. This work further elucidates the importance of non-microbial CH4 formation which should be distinguished

Accelerated methanogenesis from aliphatic and aromatic hydrocarbons under iron- and sulfate-reducing conditions.

PubMed

Siegert, Michael; Cichocka, Danuta; Herrmann, Steffi; Gründger, Friederike; Feisthauer, Stefan; Richnow, Hans-Hermann; Springael, Dirk; Krüger, Martin

2011-02-01

The impact of four electron acceptors on hydrocarbon-induced methanogenesis was studied. Methanogenesis from residual hydrocarbons may enhance the exploitation of oil reservoirs and may improve bioremediation. The conditions to drive the rate-limiting first hydrocarbon-oxidizing steps for the conversion of hydrocarbons into methanogenic substrates are crucial. Thus, the electron acceptors ferrihydrite, manganese dioxide, nitrate or sulfate were added to sediment microcosms acquired from two brackish water locations. Hexadecane, ethylbenzene or 1-(13)C-naphthalene were used as model hydrocarbons. Methane was released most rapidly from incubations amended with ferrihydrite and hexadecane. Ferrihydrite enhanced only hexadecane-dependent methanogenesis. The rates of methanogenesis were negatively affected by sulfate and nitrate at concentrations of more than 5 and 1 mM, respectively. Metal-reducing Geobacteraceae and potential sulfate reducers as well as Methanosarcina were present in situ and in vitro. Ferrihydrite addition triggered the growth of Methanosarcina-related methanogens. Additionally, methane was removed concomitantly by anaerobic methanotrophy. ANME-1 and -2 methyl coenzyme M reductase genes were detected, indicating anaerobic methanotrophy as an accompanying process [Correction added 16 December after online publication: 'methyl coenzyme A' changed to 'methyl coenzyme M' in this sentence]. The experiments presented here demonstrate the feasibility of enhancing methanogenic alkane degradation by ferrihydrite or sulfate addition in different geological settings. © 2010 Federation of European Microbiological Societies. Published by Blackwell Publishing Ltd. All rights reserved.

Inter-comparison of network measurements of non-methane organic compounds with model simulations

NASA Astrophysics Data System (ADS)

Chen, Sheng-Po; Su, Yuan-Chang; Chiu, Ching-Jui; Lin, Ching-Ho; Chang, Julius S.; Chang, Chih-Chung; Wang, Jia-Lin

2015-12-01

Ambient levels of total non-methane organic carbons (NMOCs) at air quality stations (AQSs, called AQS NMOCs) are compared with the summed concentrations of 56 NMHCs obtained from the Photochemical Assessment Monitoring Stations (called total PAMS). For mutual validation of the two networks, the total PAMS were compared with the AQS NMOCs at four sites on the island of Taiwan for the period 2007-2012. The inter-comparison of total PAMS and AQS NMOCs has been discussed previously, which reported that the total PAMS accounted for approximately 30% of the AQS NMOCs on average (Chen et al., 2014b). In this study, both the observed total PAMS and AQS NMOCs were further compared with the emissions and model simulations for mutual validation. A three-dimensional Eulerian air quality model was used to simulate total PAMS and total VOCs, which were then inter-compared with the observed total PAMS and AQS NMOCs, respectively. We found closely agreeing results between the observed and simulated total PAMS, affirming that the treatment of meteorology and VOC emissions in the model was sufficiently robust. Further, although the modeled VOC data agreed with the AQS NMOC observations for the sites in urban settings, a significant discrepancy existed for the industrial sites, particularly at the concentration spikes. Such a discrepancy was presumably attributed to high emissions of OVOCs from industrial complexes compounded by the lower sensitivity of AQS measurements for OVOCs compared with hydrocarbons. Consequently, using AQS NMOCs to represent ambient VOC levels should be limited to environments where the amounts of OVOCs are relatively small relative to total VOCs.

Production of methane-rich syngas from hydrocarbon fuels using multi-functional catalyst/capture agent

DOEpatents

Siefert, Nicholas S; Shekhawat, Dushyant; Berry, David A; Surdoval, Wayne A

2014-12-30

The disclosure provides a gasification process for the production of a methane-rich syngas at temperatures exceeding 700.degree. C. through the use of an alkali hydroxide MOH, using a gasification mixture comprised of at least 0.25 moles and less than 2 moles of water for each mole of carbon, and at least 0.15 moles and less than 2 moles of alkali hydroxide MOH for each mole of carbon. These relative amounts allow the production of a methane-rich syngas at temperatures exceeding 700.degree. C. by enabling a series of reactions which generate H.sub.2 and CH.sub.4, and mitigate the reforming of methane. The process provides a methane-rich syngas comprised of roughly 20% (dry molar percentage) CH.sub.4 at temperatures above 700.degree. C., and may effectively operate within an IGFC cycle at reactor temperatures between 700-900.degree. C. and pressures in excess of 10 atmospheres.

Hydrocarbon emissions in the Bakken oil field in North Dakota

NASA Astrophysics Data System (ADS)

Mielke-Maday, I.; Petron, G.; Miller, B.; Frost, G. J.; Peischl, J.; Kort, E. A.; Smith, M. L.; Karion, A.; Dlugokencky, E. J.; Montzka, S. A.; Sweeney, C.; Ryerson, T. B.; Tans, P. P.; Schnell, R. C.

2014-12-01

Within the past five years, the production of oil and natural gas in the United States from tight formations has increased rapidly due to advances in technology, such as horizontal drilling and hydraulic fracturing. With the expansion of oil and natural gas extraction operations comes the need to better quantify their emissions and potential impacts on climate forcing and air quality. The Bakken formation within the Williston Basin in North Dakota has emerged as a large contributor to the recent growth in oil production and accounts for over 10% of domestic production. Close to 30% of associated gas co-produced with the oil is flared. Very little independent information is currently available to assess the oil and gas industry emissions and their impacts on regional air quality. In May 2014, an airborne field campaign was conducted by the National Oceanic and Atmospheric Administration's (NOAA) Earth System Research Laboratory and the University of Michigan to investigate hydrocarbon emissions from operations in the oil field. Here, we present results from the analysis for methane, several non-methane hydrocarbons and combustion tracers in 72 discrete air samples collected by the aircraft on nine different flights. Samples were obtained in the boundary layer upwind and downwind of the operations and in the free troposphere. We will show results of a multiple species analysis and compare them with field campaign data from other U.S. oil and gas fields, measurements from NOAA's Global Monitoring Division long-term observing network, and available bottom-up information on emissions from oil and gas operations.

Flammulina velutipes treatment of non-sterile tall wheat grass for enhancing biodegradability and methane production.

PubMed

Kasprzycka, Agnieszka; Lalak-Kańczugowska, Justyna; Tys, Jerzy

2018-05-09

In this study fungal pretreatment of non-sterile tall wheat grass via the white rot fungi Flammulina velutipes was studied and the effect on biodegradability of lignocellulosic biomass and methane production, was evaluated. Degradation of lignin, cellulose, hemicellulose, and dry matter in non-sterile tall wheat grass during 28 days of fungal pretreatment using different inoculum ratio (0%-50%) and moisture content (MC) (45% MC, 65% MC, and 75% MC) were assessed via comparison to untreated biomass. Pretreatment with F. velutipes was most effective at 65% MC and 40% inoculum ratio, resulting in 22% lignin removal. The corresponding methane yields were 181.3 Ndm 3 ·kg VS -1 , which were 280% higher than for the untreated tall wheat grass. Copyright © 2018 Elsevier Ltd. All rights reserved.

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.

Modeling of hydrocarbon sputtering in Tore Supra

NASA Astrophysics Data System (ADS)

Hogan, J.; Gauthier, E.; Cambe, A.; Layet, J.-M.

2002-11-01

The use of carbon in fusion devices introduces problems of erosion and tritium retention which are related to chemical sputtering. The in-situ chemical sputtering yield of carbon has recently been measured in a well-diagnosed SOL plasma near the neutralizer plate in the Tore-Supra Outboard Pump Limiter. Methane and heavier hydrocarbon (C2DX and C3DY) emission has been measured in ohmic and lower hybrid heated discharges, using mass and optical molecular spectroscopy [1]. The Monte Carlo code BBQ has been used both to validate the method used to obtain the sputtering yields, and for direct comparison with available values reported for accelerator-based sputtering yields. A comparison with predicted surface temperature and particle flux dependence is also presented, for both CD4 and the heavier hydrocarbon yields. The particle flux dependence comparison is found to be complex, since changes in mean free path also accompany variation in particle flux. For the temperature dependence of methane erosion, the Roth annealing model is found to provide a better fit than the hydrogenation-moderated model. [1] A. Cambe, thesis, 2002; ORNL: Supported by U.S.DOE Contract DE-AC05-00OR22725

A New Global Open Source Marine Hydrocarbon Emission Site Database

NASA Astrophysics Data System (ADS)

Onyia, E., Jr.; Wood, W. T.; Barnard, A.; Dada, T.; Qazzaz, M.; Lee, T. R.; Herrera, E.; Sager, W.

2017-12-01

Hydrocarbon emission sites (e.g. seeps) discharge large volumes of fluids and gases into the oceans that are not only important for biogeochemical budgets, but also support abundant chemosynthetic communities. Documenting the locations of modern emissions is a first step towards understanding and monitoring how they affect the global state of the seafloor and oceans. Currently, no global open source (i.e. non-proprietry) detailed maps of emissions sites are available. As a solution, we have created a database that is housed within an Excel spreadsheet and use the latest versions of Earthpoint and Google Earth for position coordinate conversions and data mapping, respectively. To date, approximately 1,000 data points have been collected from referenceable sources across the globe, and we are continualy expanding the dataset. Due to the variety of spatial extents encountered, to identify each site we used two different methods: 1) point (x, y, z) locations for individual sites and; 2) delineation of areas where sites are clustered. Certain well-known areas, such as the Gulf of Mexico and the Mediterranean Sea, have a greater abundance of information; whereas significantly less information is available in other regions due to the absence of emission sites, lack of data, or because the existing data is proprietary. Although the geographical extent of the data is currently restricted to regions where the most data is publicly available, as the database matures, we expect to have more complete coverage of the world's oceans. This database is an information resource that consolidates and organizes the existing literature on hydrocarbons released into the marine environment, thereby providing a comprehensive reference for future work. We expect that the availability of seafloor hydrocarbon emission maps will benefit scientific understanding of hydrocarbon rich areas as well as potentially aiding hydrocarbon exploration and environmental impact assessements.

A post-Cassini view of Titan's methane-based hydrologic cycle

NASA Astrophysics Data System (ADS)

Hayes, Alexander G.; Lorenz, Ralph D.; Lunine, Jonathan I.

2018-05-01

The methane-based hydrologic cycle on Saturn's largest moon, Titan, is an extreme analogue to Earth's water cycle. Titan is the only planetary body in the Solar System, other than Earth, that is known to have an active hydrologic cycle. With a surface pressure of 1.5 bar and temperatures of 90 to 95 K, methane and ethane condense out of a nitrogen-based atmosphere and flow as liquids on the moon's surface. Exchange processes between atmospheric, surface and subsurface reservoirs produce methane and ethane cloud systems, as well as erosional and depositional landscapes that have strikingly similar forms to their terrestrial counterparts. Over its 13-year exploration of the Saturn system, the Cassini-Huygens mission revealed that Titan's hydrocarbon-based hydrology is driven by nested methane cycles that operate over a range of timescales, including geologic, orbital (for example, Croll-Milankovitch cycles), seasonal and that of a single convective storm. In this Review Article, we describe the dominant exchange processes that operate over these timescales and present a post-Cassini view of Titan's methane-based hydrologic system.

Microbial communities involved in methane production from hydrocarbons in oil sands tailings.

PubMed

Siddique, Tariq; Penner, Tara; Klassen, Jonathan; Nesbø, Camilla; Foght, Julia M

2012-09-04

Microbial metabolism of residual hydrocarbons, primarily short-chain n-alkanes and certain monoaromatic hydrocarbons, in oil sands tailings ponds produces large volumes of CH(4) in situ. We characterized the microbial communities involved in methanogenic biodegradation of whole naphtha (a bitumen extraction solvent) and its short-chain n-alkane (C(6)-C(10)) and BTEX (benzene, toluene, ethylbenzene, and xylenes) components using primary enrichment cultures derived from oil sands tailings. Clone libraries of bacterial 16S rRNA genes amplified from these enrichments showed increased proportions of two orders of Bacteria: Clostridiales and Syntrophobacterales, with Desulfotomaculum and Syntrophus/Smithella as the closest named relatives, respectively. In parallel archaeal clone libraries, sequences affiliated with cultivated acetoclastic methanogens (Methanosaetaceae) were enriched in cultures amended with n-alkanes, whereas hydrogenotrophic methanogens (Methanomicrobiales) were enriched with BTEX. Naphtha-amended cultures harbored a blend of these two archaeal communities. The results imply syntrophic oxidation of hydrocarbons in oil sands tailings, with the activities of different carbon flow pathways to CH(4) being influenced by the primary hydrocarbon substrate. These results have implications for predicting greenhouse gas emissions from oil sands tailings repositories.

Genomic and Transcriptomic Analysis of Growth-Supporting Dehalogenation of Chlorinated Methanes in Methylobacterium

PubMed Central

Chaignaud, Pauline; Maucourt, Bruno; Weiman, Marion; Alberti, Adriana; Kolb, Steffen; Cruveiller, Stéphane; Vuilleumier, Stéphane; Bringel, Françoise

2017-01-01

Bacterial adaptation to growth with toxic halogenated chemicals was explored in the context of methylotrophic metabolism of Methylobacterium extorquens, by comparing strains CM4 and DM4, which show robust growth with chloromethane and dichloromethane, respectively. Dehalogenation of chlorinated methanes initiates growth-supporting degradation, with intracellular release of protons and chloride ions in both cases. The core, variable and strain-specific genomes of strains CM4 and DM4 were defined by comparison with genomes of non-dechlorinating strains. In terms of gene content, adaptation toward dehalogenation appears limited, strains CM4 and DM4 sharing between 75 and 85% of their genome with other strains of M. extorquens. Transcript abundance in cultures of strain CM4 grown with chloromethane and of strain DM4 grown with dichloromethane was compared to growth with methanol as a reference C1 growth substrate. Previously identified strain-specific dehalogenase-encoding genes were the most transcribed with chlorinated methanes, alongside other genes encoded by genomic islands (GEIs) and plasmids involved in growth with chlorinated compounds as carbon and energy source. None of the 163 genes shared by strains CM4 and DM4 but not by other strains of M. extorquens showed higher transcript abundance in cells grown with chlorinated methanes. Among the several thousand genes of the M. extorquens core genome, 12 genes were only differentially abundant in either strain CM4 or strain DM4. Of these, 2 genes of known function were detected, for the membrane-bound proton translocating pyrophosphatase HppA and the housekeeping molecular chaperone protein DegP. This indicates that the adaptive response common to chloromethane and dichloromethane is limited at the transcriptional level, and involves aspects of the general stress response as well as of a dehalogenation-specific response to intracellular hydrochloric acid production. Core genes only differentially abundant in either

Genomic and Transcriptomic Analysis of Growth-Supporting Dehalogenation of Chlorinated Methanes in Methylobacterium.

PubMed

Chaignaud, Pauline; Maucourt, Bruno; Weiman, Marion; Alberti, Adriana; Kolb, Steffen; Cruveiller, Stéphane; Vuilleumier, Stéphane; Bringel, Françoise

2017-01-01

Bacterial adaptation to growth with toxic halogenated chemicals was explored in the context of methylotrophic metabolism of Methylobacterium extorquens , by comparing strains CM4 and DM4, which show robust growth with chloromethane and dichloromethane, respectively. Dehalogenation of chlorinated methanes initiates growth-supporting degradation, with intracellular release of protons and chloride ions in both cases. The core, variable and strain-specific genomes of strains CM4 and DM4 were defined by comparison with genomes of non-dechlorinating strains. In terms of gene content, adaptation toward dehalogenation appears limited, strains CM4 and DM4 sharing between 75 and 85% of their genome with other strains of M. extorquens . Transcript abundance in cultures of strain CM4 grown with chloromethane and of strain DM4 grown with dichloromethane was compared to growth with methanol as a reference C 1 growth substrate. Previously identified strain-specific dehalogenase-encoding genes were the most transcribed with chlorinated methanes, alongside other genes encoded by genomic islands (GEIs) and plasmids involved in growth with chlorinated compounds as carbon and energy source. None of the 163 genes shared by strains CM4 and DM4 but not by other strains of M. extorquens showed higher transcript abundance in cells grown with chlorinated methanes. Among the several thousand genes of the M. extorquens core genome, 12 genes were only differentially abundant in either strain CM4 or strain DM4. Of these, 2 genes of known function were detected, for the membrane-bound proton translocating pyrophosphatase HppA and the housekeeping molecular chaperone protein DegP. This indicates that the adaptive response common to chloromethane and dichloromethane is limited at the transcriptional level, and involves aspects of the general stress response as well as of a dehalogenation-specific response to intracellular hydrochloric acid production. Core genes only differentially abundant in

Real-time drilling mud gas monitoring for qualitative evaluation of hydrocarbon gas composition during deep sea drilling in the Nankai Trough Kumano Basin.

PubMed

Hammerschmidt, Sebastian B; Wiersberg, Thomas; Heuer, Verena B; Wendt, Jenny; Erzinger, Jörg; Kopf, Achim

2014-01-01

Integrated Ocean Drilling Program Expedition 338 was the second scientific expedition with D/V Chikyu during which riser drilling was conducted as part of the Nankai Trough Seismogenic Zone Experiment. Riser drilling enabled sampling and real-time monitoring of drilling mud gas with an onboard scientific drilling mud gas monitoring system ("SciGas"). A second, independent system was provided by Geoservices, a commercial mud logging service. Both systems allowed the determination of (non-) hydrocarbon gas, while the SciGas system also monitored the methane carbon isotope ratio (δ(13)CCH4). The hydrocarbon gas composition was predominated by methane (> 1%), while ethane and propane were up to two orders of magnitude lower. δ(13)CCH4 values suggested an onset of thermogenic gas not earlier than 1600 meter below seafloor. This study aims on evaluating the onboard data and subsequent geological interpretations by conducting shorebased analyses of drilling mud gas samples. During shipboard monitoring of drilling mud gas the SciGas and Geoservices systems recorded up to 8.64% and 16.4% methane, respectively. Ethane and propane concentrations reached up to 0.03 and 0.013%, respectively, in the SciGas system, but 0.09% and 0.23% in the Geoservices data. Shorebased analyses of discrete samples by gas chromatography showed a gas composition with ~0.01 to 1.04% methane, 2 - 18 ppmv ethane, and 2 - 4 ppmv propane. Quadruple mass spectrometry yielded similar results for methane (0.04 to 4.98%). With δD values between -171‰ and -164‰, the stable hydrogen isotopic composition of methane showed little downhole variability. Although the two independent mud gas monitoring systems and shorebased analysis of discrete gas sample yielded different absolute concentrations they all agree well with respect to downhole variations of hydrocarbon gases. The data point to predominantly biogenic methane sources but suggest some contribution from thermogenic sources at depth, probably due

Comet Impacts as a Source of Methane on Titan

NASA Astrophysics Data System (ADS)

Howard, Michael; Goldman, N.; Vitello, P. A.

2006-12-01

We model comet impacts on Titan as a possible source of atmospheric methane. That is, we study the formation of methane in comet impacts using chemical equilibrium calculations coupled with arbitrary Lagrange-Eulerian (ALE) hydrodynamics. That is, we study the chemical transformation of comet material under high pressure and temperature conditions as it impacts Titan. We assume that the comet is composed of ice, graphite, nitrogen and some hydrocarbons. For certain pressure and temperature regimes, in chemical equilibrium, a significant amount of ice and graphite can be transformed into methane. As a result, we find that a significant amount of methane can be formed in comet collisions on Titan. The methane is formed in the post-impact vapor clouds that form as the comet material expands and cools. We use molecular dynamics to construct an equation of state for the ice surface structures and the comet material. We also study kinetic processes for methane formation during the expansion and cooling phase. We discuss the implication of our results for comets as a possible source of abiotic methane on Titan and its implications on the origin of life. We also discuss the various uncertainties in our model. * This work was performed under the auspices of the U.S. Department of Energy by University of California, Lawrence Livermore National Laboratory under Contract W-7405-Eng-48.

Demonstration of Technologies for Remote and in Situ Sensing of Atmospheric Methane Abundances - a Controlled Release Experiment

NASA Astrophysics Data System (ADS)

Aubrey, A. D.; Thorpe, A. K.; Christensen, L. E.; Dinardo, S.; Frankenberg, C.; Rahn, T. A.; Dubey, M.

2013-12-01

It is critical to constrain both natural and anthropogenic sources of methane to better predict the impact on global climate change. Critical technologies for this assessment include those that can detect methane point and concentrated diffuse sources over large spatial scales. Airborne spectrometers can potentially fill this gap for large scale remote sensing of methane while in situ sensors, both ground-based and mounted on aerial platforms, can monitor and quantify at small to medium spatial scales. The Jet Propulsion Laboratory (JPL) and collaborators recently conducted a field test located near Casper, WY, at the Rocky Mountain Oilfield Test Center (RMOTC). These tests were focused on demonstrating the performance of remote and in situ sensors for quantification of point-sourced methane. A series of three controlled release points were setup at RMOTC and over the course of six experiment days, the point source flux rates were varied from 50 LPM to 2400 LPM (liters per minute). During these releases, in situ sensors measured real-time methane concentration from field towers (downwind from the release point) and using a small Unmanned Aerial System (sUAS) to characterize spatiotemporal variability of the plume structure. Concurrent with these methane point source controlled releases, airborne sensor overflights were conducted using three aircraft. The NASA Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) participated with a payload consisting of a Fourier Transform Spectrometer (FTS) and an in situ methane sensor. Two imaging spectrometers provided assessment of optical and thermal infrared detection of methane plumes. The AVIRIS-next generation (AVIRIS-ng) sensor has been demonstrated for detection of atmospheric methane in the short wave infrared region, specifically using the absorption features at ~2.3 μm. Detection of methane in the thermal infrared region was evaluated by flying the Hyperspectral Thermal Emission Spectrometer (Hy

Hydrocarbon-Fueled Rocket Engine Plume Diagnostics: Analytical Developments and Experimental Results

NASA Technical Reports Server (NTRS)

Tejwani, Gopal D.; McVay, Gregory P.; Langford, Lester A.; St. Cyr, William W.

2006-01-01

A viewgraph presentation describing experimental results and analytical developments about plume diagnostics for hydrocarbon-fueled rocket engines is shown. The topics include: 1) SSC Plume Diagnostics Background; 2) Engine Health Monitoring Approach; 3) Rocket Plume Spectroscopy Simulation Code; 4) Spectral Simulation for 10 Atomic Species and for 11 Diatomic Molecular Electronic Bands; 5) "Best" Lines for Plume Diagnostics for Hydrocarbon-Fueled Rocket Engines; 6) Experimental Set Up for the Methane Thruster Test Program and Experimental Results; and 7) Summary and Recommendations.

Hydrocarbon and Carbon Dioxide Fluxes from Natural Gas Well Pad Soils and Surrounding Soils in Eastern Utah.

PubMed

Lyman, Seth N; Watkins, Cody; Jones, Colleen P; Mansfield, Marc L; McKinley, Michael; Kenney, Donna; Evans, Jordan

2017-10-17

We measured fluxes of methane, nonmethane hydrocarbons, and carbon dioxide from natural gas well pad soils and from nearby undisturbed soils in eastern Utah. Methane fluxes varied from less than zero to more than 38 g m -2 h -1 . Fluxes from well pad soils were almost always greater than from undisturbed soils. Fluxes were greater from locations with higher concentrations of total combustible gas in soil and were inversely correlated with distance from well heads. Several lines of evidence show that the majority of emission fluxes (about 70%) were primarily due to subsurface sources of raw gas that migrated to the atmosphere, with the remainder likely caused primarily by re-emission of spilled liquid hydrocarbons. Total hydrocarbon fluxes during summer were only 39 (16, 97)% as high as during winter, likely because soil bacteria consumed the majority of hydrocarbons during summer months. We estimate that natural gas well pad soils account for 4.6 × 10 -4 (1.6 × 10 -4 , 1.6 × 10 -3 )% of total emissions of hydrocarbons from the oil and gas industry in Utah's Uinta Basin. Our undisturbed soil flux measurements were not adequate to quantify rates of natural hydrocarbon seepage in the Uinta Basin.

Hydrocarbon geochemistry of cold seeps in the Monterey Bay National Marine Sanctuary

USGS Publications Warehouse

Lorenson, T.D.; Kvenvolden, K.A.; Hostettler, F.D.; Rosenbauer, R.J.; Orange, D.L.; Martin, J.B.

2002-01-01

Samples from four geographically and tectonically discrete cold seeps named Clam Flat, Clamfield, Horseshoe Scarp South, and Tubeworm City, within the Monterey Bay National Marine Sanctuary were analyzed for their hydrocarbon content. The sediment contains gaseous hydrocarbons and CO2, as well as high molecular weight aliphatic and aromatic hydrocarbons with various combinations of thermogenic and biogenic contributions from petroleum, marine, and terrigenous sources. Of particular interest is the cold seep site at Clamfield which is characterized by the presence of thermogenic hydrocarbons including oil that can likely be correlated with oil-saturated strata at Majors Creek near Davenport, CA, USA. At Clam Flat, the evidence for thermogenic hydrocarbons is equivocal. At Horseshoe Scarp South and Tubeworm City, hydrocarbon gases, mainly methane, are likely microbial in origin. These varied sources of hydrocarbon gases highlight the diverse chemical systems that appear at cold seep communities. ?? 2002 Elsevier Science B.V. All rights reserved.

Methane hydrate formation in confined nanospace can surpass nature

DOE PAGES

Casco, Mirian E.; Silvestre-Albero, Joaquín; Ramírez-Cuesta, Anibal J.; ...

2015-03-02

Natural methane hydrates are believed to be the largest source of hydrocarbons on Earth. These structures are formed in specific locations such as deep-sea sediments and the permafrost based on demanding conditions of high pressure and low temperature. We report that, by taking advantage of the confinement effects on nanopore space, synthetic methane hydrates grow under mild conditions (3.5 MPa and 2 degrees C), with faster kinetics (within minutes) than nature, fully reversibly and with a nominal stoichiometry that mimics nature. Furthermore, the formation of the hydrate structures in nanospace and their similarity to natural hydrates is confirmed using inelasticmore » neutron scattering experiments and synchrotron X-ray powder diffraction. Our findings may be a step towards the application of a smart synthesis of methane hydrates in energy-demanding applications (for example, transportation).« less

Nitrate decreases ruminal methane production with slight changes to ruminal methanogen composition of nitrate-adapted steers.

PubMed

Zhao, Liping; Meng, Qingxiang; Li, Yan; Wu, Hao; Huo, Yunlong; Zhang, Xinzhuang; Zhou, Zhenming

2018-03-20

This study was conducted to examine effects of nitrate on ruminal methane production, methanogen abundance, and composition. Six rumen-fistulated Limousin×Jinnan steers were fed diets supplemented with either 0% (0NR), 1% (1NR), or 2% (2NR) nitrate (dry matter basis) regimens in succession. Rumen fluid was taken after two-week adaptation for evaluation of in vitro methane production, methanogen abundance, and composition measurements. Results showed that nitrate significantly decreased in vitro ruminal methane production at 6 h, 12 h, and 24 h (P < 0.01; P < 0.01; P = 0.01). The 1NR and 2NR regimens numerically reduced the methanogen population by 4.47% and 25.82% respectively. However, there was no significant difference observed between treatments. The alpha and beta diversity of the methanogen community was not significantly changed by nitrate either. However, the relative abundance of the methanogen genera was greatly changed. Methanosphaera (P L  = 0.0033) and Methanimicrococcus (P L  = 0.0113) abundance increased linearly commensurate with increasing nitration levels, while Methanoplanus abundance was significantly decreased (P L  = 0.0013). The population of Methanoculleus, the least frequently identified genus in this study, exhibited quadratic growth from 0% to 2% when nitrate was added (P Q  = 0.0140). Correlation analysis found that methane reduction was significantly related to Methanobrevibacter and Methanoplanus abundance, and negatively correlated with Methanosphaera and Methanimicrococcus abundance.

Noteworthy Facts about a Methane-Producing Microbial Community Processing Acidic Effluent from Sugar Beet Molasses Fermentation.

PubMed

Chojnacka, Aleksandra; Szczęsny, Paweł; Błaszczyk, Mieczysław K; Zielenkiewicz, Urszula; Detman, Anna; Salamon, Agnieszka; Sikora, Anna

2015-01-01

Anaerobic digestion is a complex process involving hydrolysis, acidogenesis, acetogenesis and methanogenesis. The separation of the hydrogen-yielding (dark fermentation) and methane-yielding steps under controlled conditions permits the production of hydrogen and methane from biomass. The characterization of microbial communities developed in bioreactors is crucial for the understanding and optimization of fermentation processes. Previously we developed an effective system for hydrogen production based on long-term continuous microbial cultures grown on sugar beet molasses. Here, the acidic effluent from molasses fermentation was used as the substrate for methanogenesis in an upflow anaerobic sludge blanket bioreactor. This study focused on the molecular analysis of the methane-yielding community processing the non-gaseous products of molasses fermentation. The substrate for methanogenesis produces conditions that favor the hydrogenotrophic pathway of methane synthesis. Methane production results from syntrophic metabolism whose key process is hydrogen transfer between bacteria and methanogenic Archaea. High-throughput 454 pyrosequencing of total DNA isolated from the methanogenic microbial community and bioinformatic sequence analysis revealed that the domain Bacteria was dominated by Firmicutes (mainly Clostridia), Bacteroidetes, δ- and γ-Proteobacteria, Cloacimonetes and Spirochaetes. In the domain Archaea, the order Methanomicrobiales was predominant, with Methanoculleus as the most abundant genus. The second and third most abundant members of the Archaeal community were representatives of the Methanomassiliicoccales and the Methanosarcinales. Analysis of the methanogenic sludge by scanning electron microscopy with Energy Dispersive X-ray Spectroscopy and X-ray diffraction showed that it was composed of small highly heterogeneous mineral-rich granules. Mineral components of methanogenic granules probably modulate syntrophic metabolism and methanogenic

The Relative Abundances of Resolved 12CH2D2 and 13CH3D and Mechanisms Controlling Isotopic Bond Ordering in Abiotic and Biotic Methane Gases

NASA Astrophysics Data System (ADS)

Young, E. D.; Kohl, I. E.; Sherwood Lollar, B.; Etiope, G.; Rumble, D.; Li, S.; Haghnegahdar, M. A.; Schauble, E. A.; McCain, K.; Foustoukos, D.; Sutcliffe, C. N.; Warr, O.; Ballentine, C. J.; Onstott, T. C.; Hosgormez, H.; Neubeck, A.; Marques, J. M.; Perez-Rodriguez, I. M.; Rowe, A. R.; LaRowe, D.; Magnabosco, C.; Bryndzia, T.

2016-12-01

We report measurements of resolved 12CH2D2 and 13CH3D at natural abundances in a variety of methane gases produced naturally and in the laboratory. The ability to resolve 12CH2D2 from 13CH3D provides unprecedented insights into the origin and evolution of CH4. The results identify conditions under which either isotopic bond order disequilibrium or equilibrium are expected. Where equilibrium obtains, concordant Δ12CH2D2 and Δ13CH3D temperatures can be used reliably for thermometry. We find that concordant temperatures do not always match previous hypotheses based on indirect estimates of temperature of formation nor temperatures derived from CH4/H2 D/H exchange, underscoring the importance of reliable thermometry based on the CH4 molecules themselves. Where Δ12CH2D2 and Δ13CH3D values are inconsistent with thermodynamic equilibrium, temperatures of formation derived from these species are spurious. In such situations, while formation temperatures are unavailable, disequilibrium isotopologue ratios nonetheless provide important information about the formation mechanism of the gas and the presence or absence of multiple sources or sinks. In particular, disequilibrium isotopologue ratios may provide the means for differentiating between methane produced by abiotic synthesis versus biological processes. Deficits in 12CH2D2 compared with equilibrium values in CH4 gas made by surface-catalyzed abiotic reactions are so large as to point towards a quantum tunneling origin. Tunneling also accounts for the more moderate depletions in 13CH3D that accompany the low 12CH2D2 abundances produced by abiotic reactions. The tunneling signature of abiotic CH4 formation may prove to be an important tracer of abiotic methane formation, especially where it is preserved by dissolution of gas in cool hydrothermal systems (e.g., Mars). Isotopologue signatures of abiotic methane production can be erased by infiltration of microbial communities, and Δ12CH2D2 values are a key tracer of

Methane absorption in the visible spectra of the outer planets and Titan

NASA Technical Reports Server (NTRS)

Owen, T.; Cess, R. D.

1975-01-01

New spectra of Jupiter, Saturn, and Titan show weak methane bands in the region below 6000 A which have been known for many years in the spectra of Uranus and Neptune. Adopting the known abundance of methane on Jupiter, we have used a band model to determine CH4 abundances and broadening pressures for the other objects. The results indicate high values of the CH4 to H2 concentration ratio for Uranus and Neptune; for Titan, a surface pressure in excess of 1 atm is implied.

Novel insights into freshwater hydrocarbon-rich sediments using metatranscriptomics: Opening the black box.

PubMed

Reid, Thomas; Chaganti, Subba Rao; Droppo, Ian G; Weisener, Christopher G

2018-06-01

Baseline biogeochemical surveys of natural environments is an often overlooked field of environmental studies. Too often research begins once contamination has occurred, with a knowledge gap as to how the affected area behaved prior to outside (often anthropogenic) influences. These baseline characterizations can provide insight into proposed bioremediation strategies crucial in cleaning up chemical spill sites or heavily mined regions. Hence, this study was conducted to survey the in-situ microbial activity within freshwater hydrocarbon-rich environments cutting through the McMurray formation - the geologic strata constituting the oil sands. We are the first to report in-situ functional variations among these freshwater microbial ecosystems using metatranscriptomics, providing insight into the in-situ gene expression within these naturally hydrocarbon-rich sites. Key genes involved in energy metabolism (nitrogen, sulfur and methane) and hydrocarbon degradation, including transcripts relating to the observed expression of methane oxidation are reported. This information provides better linkages between hydrocarbon impacted environments, closing knowledge gaps for optimizing not only oil sands mine reclamation but also enhancing microbial reclamation strategies in various freshwater environments. These finding can also be applied to existing contaminated environments, in need of efficient reclamation efforts. Copyright © 2018 Elsevier Ltd. All rights reserved.

Methane dynamics regulated by microbial community response to permafrost thaw.

PubMed

McCalley, Carmody K; Woodcroft, Ben J; Hodgkins, Suzanne B; Wehr, Richard A; Kim, Eun-Hae; Mondav, Rhiannon; Crill, Patrick M; Chanton, Jeffrey P; Rich, Virginia I; Tyson, Gene W; Saleska, Scott R

2014-10-23

Permafrost contains about 50% of the global soil carbon. It is thought that the thawing of permafrost can lead to a loss of soil carbon in the form of methane and carbon dioxide emissions. The magnitude of the resulting positive climate feedback of such greenhouse gas emissions is still unknown and may to a large extent depend on the poorly understood role of microbial community composition in regulating the metabolic processes that drive such ecosystem-scale greenhouse gas fluxes. Here we show that changes in vegetation and increasing methane emissions with permafrost thaw are associated with a switch from hydrogenotrophic to partly acetoclastic methanogenesis, resulting in a large shift in the δ(13)C signature (10-15‰) of emitted methane. We used a natural landscape gradient of permafrost thaw in northern Sweden as a model to investigate the role of microbial communities in regulating methane cycling, and to test whether a knowledge of community dynamics could improve predictions of carbon emissions under loss of permafrost. Abundance of the methanogen Candidatus 'Methanoflorens stordalenmirensis' is a key predictor of the shifts in methane isotopes, which in turn predicts the proportions of carbon emitted as methane and as carbon dioxide, an important factor for simulating the climate feedback associated with permafrost thaw in global models. By showing that the abundance of key microbial lineages can be used to predict atmospherically relevant patterns in methane isotopes and the proportion of carbon metabolized to methane during permafrost thaw, we establish a basis for scaling changing microbial communities to ecosystem isotope dynamics. Our findings indicate that microbial ecology may be important in ecosystem-scale responses to global change.

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

Screening for Dissolved Methane in Groundwater Across Texas Shale Plays

NASA Astrophysics Data System (ADS)

Nicot, J. P.; Mickler, P. J.; Hildenbrand, Z.; Larson, T.; Darvari, R.; Uhlman, K.; Smyth, R. C.; Scanlon, B. R.

2014-12-01

There is considerable interest in methane concentrations in groundwater, particularly as they relate to hydraulic fracturing in shale plays. Recent studies of aquifers in the footprint of several gas plays across the US have shown that (1) dissolved thermogenic methane may or may not be present in the shallow groundwater and (2) shallow thermogenic methane may be naturally occurring and emplaced through mostly vertical migration over geologic time and not necessarily a consequence of recent unconventional gas production. We are currently conducting a large sampling campaign across the state of Texas to characterize shallow methane in fresh-water aquifers overlying shale plays and other tight formations. We collected a total of ~800 water samples, ~500 in the Barnett, ~150 in the Eagle Ford, ~80 in the Haynesville shale plays as well as ~50 in the Delaware Basin of West Texas. Preliminary analytical results suggest that dissolved methane is not widespread in shallow groundwater and that, when present at concentrations exceeding 10 mg/L, it is often of thermogenic origin according to the isotopic signature and to the presence of other light hydrocarbons. The Barnett Shale contains a large methane hotspot (~ 2 miles wide) along the Hood-Parker county line which is likely of natural origin whereas the Eagle Ford and Haynesville shales, neglecting microbial methane, show more distributed methane occurrences. Samples from the Delaware Basin show no methane except close to blowouts.

AVO in North of Paria, Venezuela: Gas methane versus condensate reservoirs

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

Regueiro, J.; Pena, A.

1996-07-01

The gas fields of North of Paria, offshore eastern Venezuela, present a unique opportunity for amplitude variations with offset (AVO) characterization of reservoirs containing different fluids: gas-condensate, gas (methane) and water (brine). AVO studies for two of the wells in the area, one with gas-condensate and the other with gas (methane) saturated reservoirs, show interesting results. Water sands and a fluid contact (condensate-water) are present in one of these wells, thus providing a control point on brine-saturated properties. The reservoirs in the second well consist of sands highly saturated with methane. Clear differences in AVO response exist between hydrocarbon-saturated reservoirsmore » and those containing brine. However, it is also interesting that subtle but noticeable differences can be interpreted between condensate-and methane-saturated sands. These differences are attributed to differences in both in-situ fluid density and compressibility, and rock frame properties.« less

Crenothrix are major methane consumers in stratified lakes

PubMed Central

Oswald, Kirsten; Graf, Jon S; Littmann, Sten; Tienken, Daniela; Brand, Andreas; Wehrli, Bernhard; Albertsen, Mads; Daims, Holger; Wagner, Michael; Kuypers, Marcel MM; Schubert, Carsten J; Milucka, Jana

2017-01-01

Methane-oxidizing bacteria represent a major biological sink for methane and are thus Earth’s natural protection against this potent greenhouse gas. Here we show that in two stratified freshwater lakes a substantial part of upward-diffusing methane was oxidized by filamentous gamma-proteobacteria related to Crenothrix polyspora. These filamentous bacteria have been known as contaminants of drinking water supplies since 1870, but their role in the environmental methane removal has remained unclear. While oxidizing methane, these organisms were assigned an ‘unusual’ methane monooxygenase (MMO), which was only distantly related to ‘classical’ MMO of gamma-proteobacterial methanotrophs. We now correct this assignment and show that Crenothrix encode a typical gamma-proteobacterial PmoA. Stable isotope labeling in combination swith single-cell imaging mass spectrometry revealed methane-dependent growth of the lacustrine Crenothrix with oxygen as well as under oxygen-deficient conditions. Crenothrix genomes encoded pathways for the respiration of oxygen as well as for the reduction of nitrate to N2O. The observed abundance and planktonic growth of Crenothrix suggest that these methanotrophs can act as a relevant biological sink for methane in stratified lakes and should be considered in the context of environmental removal of methane. PMID:28585934

Surface Interactions and Confinement of Methane: A High Pressure Magic Angle Spinning NMR and Computational Chemistry Study

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

Ok, Salim; Hoyt, David W.; Andersen, Amity

Characterization and modeling of the molecular-level behavior of simple hydrocarbon gases, such as methane, in the presence of both nonporous and nano-porous mineral matrices allows for predictive understanding of important processes in engineered and natural systems. In this study, changes in local electromagnetic environments of the carbon atoms in methane under conditions of high pressure (up to 130 bar) and moderate temperature (up to 346 K) were observed with 13C magic-angle spinning (MAS) NMR spectroscopy while the methane gas was mixed with two model solid substrates: a fumed non-porous, 12 nm particle size silica and a mesoporous silica with 200more » nm particle size and 4 nm average pore diameter. Examination of the interactions between methane and the silica systems over temperatures and pressures that include the supercritical regime was allowed by a novel high pressure MAS sample containment system, which provided high resolution spectra collected under in situ conditions. For pure methane, no significant thermal effects were found for the observed 13C chemical shifts at all pressures studied here (28.2 bar, 32.6 bar, 56.4 bar, 65.1 bar, 112.7 bar, and 130.3 bar). However, the 13C chemical shifts of resonances arising from confined methane changed slightly with changes in temperature in mixtures with mesoporous silica. The chemical shift values of 13C nuclides in methane change measurably as a function of pressure both in the pure state and in mixtures with both silica matrices, with a more pronounced shift when meso-porous silica is present. Molecular-level simulations utilizing GCMC, MD and DFT confirm qualitatively that the experimentally measured changes are attributed to interactions of methane with the hydroxylated silica surfaces as well as densification of methane within nanopores and on pore surfaces.« less

Freezing and hungry? Hydrocarbon degrading microbial communities in Barents Sea sediments around Svalbard

NASA Astrophysics Data System (ADS)

Krueger, Martin; Straaten, Nontje

2017-04-01

The Polar Regions are characterised by varying temperatures and changing ice coverage, so most of the primary production take place in the warmer season. Consequently, sedimentation rates and nutrient input are low. The diversity and metabolic potentials of the microbial communities inhabiting these sediments in the Northern Barents Sea are largely unknown. Recent reports on natural methane seeps as well as the increase in hydrocarbon exploration activities in the Arctic initiated our studies on the potential of indigenous microbial communities to degrade methane and higher hydrocarbons under in situ pressure and temperature conditions. Furthermore, the subseafloor geochemistry in these areas was studied, together with important microbial groups, like methanotrophs, methanogens, metal and sulfate reducers, which may drive seafloor ecosystems in the Northern Barents Sea. Sediment samples were collected in several areas around Svalbard in the years 2013-2016 ranging from shallow (200m) areas on the Svalbard shelf to deep sea areas on the eastern Yermak Plateau (3200m water depths). Shelf sediments showed the highest organic carbon content which decreased with increasing depths. Iron and manganese as potential electron acceptors were found in the porewater especially in the top 50 cm of the cores, while sulfate was always present in substantial amounts in porewater samples down to the end of the up to two metre long cores. Concentrations of dissolved methane and carbon dioxide were low. The potential of the indigenous microorganisms to degrade methane and higher hydrocarbons as well as different oils under in situ temperatures and pressures was widespread in surface sediments. Degradation rates were higher under aerobic than under anaerobic conditions, and decreased with increasing sediment as well as water depths. Similar pattern were found for other metabolic processes, including sulfate, Fe and Mn reduction as well as carbon dioxide and methane production rates

Primitive bodies - Molecular abundances in Comet Halley as probes of cometary formation environments

NASA Technical Reports Server (NTRS)

Lunine, Jonathan I.

1989-01-01

The most recent results on abundances of molecules in Halley's comet are examined in the context of various models for the environment in which comets formed. These environments include molecular clouds associated with star-forming regions, the solar nebula, gaseous disks around proto-planets, and combinations of these. Of all constituents in a cometary nucleus, the highly volatile molecules such as methane, ammonia, molecular nitrogen, and carbon monoxide are most sensitive to the final episode of cometary grain formation and incorporation in the comet's nucleus; hence they likely reflect at least some chemical processing in the solar nebula. Proper interpretation requires modeling of a number of physical processes including gas phase chemistry, chemistry on grain surfaces, and fractionation effects resulting from preferential incorporation of certain gases in proto-cometary grains. The abundance of methane in Halley's comet could be a key indicator of where that comet formed, provided the methane abundance on grains in star-forming regions can be observationally constrained.

Cassini/Huygens Investigations of Titan's Methane Cycle

NASA Astrophysics Data System (ADS)

Griffith, C. A.; Penteado, P.

2008-12-01

In Titan's atmosphere, the second most abundant constituent, methane, exists as a gas, liquid and solid, and cycles between the atmosphere and surface. Similar to Earth's hydrological cycle, Titan sports clouds, rain, and lakes. Yet, Titan's cycle differs dramatically from its terrestrial counterpart, and reveals the workings of weather in an atmosphere that is ten times thicker than Earth's atmosphere, that is two orders of magnitude less illuminated, and that involves a different condensable. Measurements of Titan's troposphere, where the methane cycle plays out, are limited largely to spectral images of Titan's clouds, several temperature profiles by Voyager, Huygens and Cassini, recent Keck spectra of the surface methane humidity, and one vertical profile of Titan's methane abundance, measured on a summer afternoon in Titan's tropical atmosphere by the Huygens probe. The salient features of Titan's methane cycle are distinctly alien: clouds have predominated the northern and southern polar atmospheres; the one humidity profile precisely matches the profile (of cartoonish simplicity) used in pre-Cassini models, and surface features correlate with latitude. Data of Titan's troposphere are analyzed with thermodynamic and radiative transfer calculations, and synthesized with other studies of Titan's stratosphere and surface, to investigate the workings of Titan's methane cycle. At the end of Cassini's nominal mission, we find that Titan's weather, climate and surface-to-atmosphere exchange of volatiles vastly differs from the manifestation of these processes on Earth, largely as a result of different basic characteristics of these planetary bodies. The talk ends with a comparison between Titan and Earth's tropospheres, their fundamental properties, the energetics of their condensible cycles, their weather and climates. References: Griffith C.A. et al. Titan's Tropical Storms in an Evolving Atmosphere. Ap.J. In Press (2008). Griffith C.A. Storms, Polar Deposits, and

Hydrocarbons of aquatic and terrestrial origin in mountain streams of the Marmot Basin

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

Telang, S.A.; Hodgson, G.W.; Baker, B.L.

1981-01-01

The abundance of n-alkanes in stream waters of the Marmot Creek drainage basin was studied to develop an understanding of the source of hydrocarbons in a pristine mountain stream. The n-alkanes varied in concentration from 0.02 ..mu..g/liter to 0.06 ..mu..g/liter and exhibited a bimodal distribution with one grouping in the range of C/sub 15/-C/sub 23/ and the other between C/sub 25/-C/sub 32/. Carbon preference indices (1.2 and 4.0, respectively) suggested that the first group was largely produced by nonphotosynthetic aquatic organisms and second was from soil and terrestrial vegetation. The contributions from stream and soil were roughly equal. Hydrocarbons inmore » pristine mountain streams thus appeared to be derived both from autochthonous and allochthonous sources. Isoprenoid hydrocarbons were present in lesser abundance than alkane hydrocarbons. Abundance of the isoprenoids relative to n-alkanes indicated that little, if any, degradation of n-alkanes occurs in the stream waters. Aromatic hydrocarbons were not present above detection limits of 1 ng/liter.« less

Contribution of cyanobacterial alkane production to the ocean hydrocarbon cycle

PubMed Central

Lea-Smith, David J.; Biller, Steven J.; Davey, Matthew P.; Cotton, Charles A. R.; Perez Sepulveda, Blanca M.; Turchyn, Alexandra V.; Scanlan, David J.; Smith, Alison G.; Chisholm, Sallie W.; Howe, Christopher J.

2015-01-01

Hydrocarbons are ubiquitous in the ocean, where alkanes such as pentadecane and heptadecane can be found even in waters minimally polluted with crude oil. Populations of hydrocarbon-degrading bacteria, which are responsible for the turnover of these compounds, are also found throughout marine systems, including in unpolluted waters. These observations suggest the existence of an unknown and widespread source of hydrocarbons in the oceans. Here, we report that strains of the two most abundant marine cyanobacteria, Prochlorococcus and Synechococcus, produce and accumulate hydrocarbons, predominantly C15 and C17 alkanes, between 0.022 and 0.368% of dry cell weight. Based on global population sizes and turnover rates, we estimate that these species have the capacity to produce 2–540 pg alkanes per mL per day, which translates into a global ocean yield of ∼308–771 million tons of hydrocarbons annually. We also demonstrate that both obligate and facultative marine hydrocarbon-degrading bacteria can consume cyanobacterial alkanes, which likely prevents these hydrocarbons from accumulating in the environment. Our findings implicate cyanobacteria and hydrocarbon degraders as key players in a notable internal hydrocarbon cycle within the upper ocean, where alkanes are continually produced and subsequently consumed within days. Furthermore we show that cyanobacterial alkane production is likely sufficient to sustain populations of hydrocarbon-degrading bacteria, whose abundances can rapidly expand upon localized release of crude oil from natural seepage and human activities. PMID:26438854