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

Science.gov (United States)

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.

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

Science.gov (United States)

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

Seasonal and Diurnal Variations of Atmospheric Non-Methane Hydrocarbons in Guangzhou, China

Directory of Open Access Journals (Sweden)

Longfeng Li

2012-05-01

Full Text Available In recent decades, high ambient ozone concentrations have become one of the major regional air quality issues in the Pearl River Delta (PRD region. Non-methane hydrocarbons (NMHCs, as key precursors of ozone, were found to be the limiting factor in photochemical ozone formation for large areas in the PRD. For source apportioning of NMHCs as well as ozone pollution control strategies, it is necessary to obtain typical seasonal and diurnal patterns of NMHCs with a large pool of field data. To date, few studies have focused on seasonal and diurnal variations of NMHCs in urban areas of Guangzhou. This study explored the seasonal variations of most hydrocarbons concentrations with autumn maximum and spring minimum in Guangzhou. The diurnal variations of most anthropogenic NMHCs typically showed two-peak pattern with one at 8:00 in the morning and another at 20:00 in the evening, both corresponding to traffic rush hours in Guangzhou, whereas isoprene displayed a different bimodal diurnal curve. Propene, ethene, m, p-xylene and toluene were the four largest contributors to ozone formation in Guangzhou, based on the evaluation of individual NMHCs’ photochemical reactivity. Therefore, an effective strategy for controlling ozone pollution may be achieved by the reduction of vehicle emissions in Guangzhou.

Subsurface biogenic gas rations associated with hydrocarbon contamination

International Nuclear Information System (INIS)

Marrin, D.L.

1991-01-01

Monitoring the in situ bioreclamation of organic chemicals in soil is usually accomplished by collecting samples from selected points during the remediation process. This technique requires the installation and sampling of soil borings and does not allow for continuous monitoring. The analysis of soil vapor overlying hydrocarbon-contaminated soil and groundwater has been used to detect the presence of nonaqueous phase liquids (NAPL) and to locate low-volatility hydrocarbons that are not directly detected by more conventional soil gas methods. Such soil vapor sampling methods are adaptable to monitoring the in situ bioremediation of soil and groundwater contamination. This paper focuses on the use of biogenic gas ratio in detecting the presence of crude oil and gasoline in the subsurface

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

Directory of Open Access Journals (Sweden)

B. Wang

2010-07-01

Full Text Available 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

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

Science.gov (United States)

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

Modeling of microbial gas generation: application to the eastern Mediterranean “Biogenic Play”

Energy Technology Data Exchange (ETDEWEB)

Schneider, M.; Dubille, M.; Montadert, L.

2016-07-01

Biogenic gas is becoming increasingly important as an exploration target in the petroleum industry because it occurs in geologically predictable circumstances and in large quantities at shallow depths as free gas or gas hydrates. As accumulations of biogenic gas result in a subtle synchronization between early generation and early trapping, we integrated a macroscopic model of microbial gas generation within a 3D basin and petroleum system forward simulator. The macroscopic model is based on a microscopic model, which consists in a 1D sedimentary column that accounts for sedimentation, compaction, Darcy flow and Diffusion flow. The organic carbon is the only non-soluble element considered in this version of the model. The dissolved elements are O2, SO4 2-, H2, CH3COOH, and CH4. Methane is dissolved in water or present as a free phase if its concentration exceeds its solubility at given pressure and temperature. In this microscopic model, the transformation of substrate into biomass is described through a set of logistic equations coupled with the transport equations (advection and diffusion). Based on the microscopic considerations we developed the macroscopic model of low maturity/biogenic gas generation in which hydrocarbons are generated through first order kinetic reactions at low maturity. This macroscopic model is adapted to petroleum system modeling at basin scale with TemisFlow®, which aims to understand and predict hydrocarbon generation, migration, and accumulation. It is composed of: i) A source rock criteria which allow defining the biogenic gas source rocks potential and ii) A kinetic model of methane generation. The previous model has been successfully applied on different basins such as the Carupano Basin from the offshore Venezuela, the Magdalena Delta (offshore Colombia) and the offshore Vietnam where direct observations of low-maturity gas were available. Furthermore, it has been applied in the offshore Lebanon in order to check the viability of

Estimating Biogenic Non-Methane Hydrocarbon Emissions for the Wasatch Front Through a High-Resolution. Gridded, Biogenic Vola Tile Organic Compound Emissions Inventory

Science.gov (United States)

2002-01-01

1-hour and proposed 8-hour National Ambient Air Quality Standards. Reactive biogenic (natural) volatile organic compounds emitted from plants have...uncertainty in predicting plant species composition and frequency. Isoprene emissions computed for the study area from the project’s high-resolution...Landcover Database (BELD 2), while monoterpene and other reactive volatile organic compound emission rates were almost 26% and 28% lower, respectively

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

Science.gov (United States)

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

2018-01-01

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

Cordierite-supported metal oxide for non-methane hydrocarbon oxidation in cooking oil fumes.

Science.gov (United States)

Huang, Yonghai; Yi, Honghong; Tang, Xiaolong; Zhao, Shunzheng; Gao, Fengyu; Wang, Jiangen; Yang, Zhongyu

2018-05-21

Cooking emission is an important reason for the air quality deterioration in the metropolitan area in China. Transition metal oxide and different loading of manganese oxide supported on cordierite were prepared by incipient wetness impregnation method and were used for non-methane hydrocarbon (NMHC) oxidation in cooking oil fumes (COFs). The effects of different calcination temperature and different Mn content were also studied. The SEM photographs and CO 2 temperature-programmed desorption revealed 5 wt% Mn/cordierite had the best pore structure and the largest number of the weak and moderate basic sites so it showed the best performance for NMHC oxidation. XRD analysis exhibited 5 wt% Mn/cordierite had the best dispersion of active phase and the active phase was MnO 2 when the calcination temperature was 400℃ which were good for the catalytic oxidation of NMHC.

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

Science.gov (United States)

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.

Biogenic gas in the Cambrian-Ordovcian Alum Shale (Denmark and Sweden)

Energy Technology Data Exchange (ETDEWEB)

Schulz, H.M.; Wirth, R.; Biermann, S.; Arning, E.T. [Helmholtz-Zentrum Potsdam - Deutsches GeoForschungsZentrum GFZ, Potsdam (Germany); Krueger, M.; Straaten, N. [BGR Hannover (Germany); Bechtel, A. [Montanuniv. Leoben (Austria); Berk, W. van [Technical Univ. of Clausthal (Germany); Schovsbo, N.H. [Geological Survey of Denmark and Greenland - GEUS, Copenhagen (Denmark); Crabtree, Stephen [Gripen Gas (Sweden)

2013-08-01

Shale gas is mainly produced from thermally mature black shales. However, biogenic methane also represents a resource which is often underestimated. Today biogenic methane is being produced from the Upper Devonian Antrim Shale in the Michigan Basin which was the most successfully exploited shale gas system during the 1990-2000 decade in the U.S.A. before significant gas production from the Barnett Shale started (Curtis et al., 2008). The Cambro-Ordovician Alum Shale in northern Europe has thermal maturities ranging from overmature in southern areas (Denmark and southern Sweden) to immature conditions (central Sweden). Biogenic methane is recorded during drilling in central Sweden. The immature Alum Shale in central Sweden has total organic carbon (TOC) contents up to 20 wt%. The hydrogen index HI ranges from 380 to 560 mgHC/gTOC at very low oxygen index (OI) values of around 4 mg CO{sub 2}/gTOC, Tmax ranges between 420 - 430 C. The organic matter is highly porous. In general, the Alum Shale is a dense shale with intercalated sandy beds which may be dense due to carbonate cementation. Secondary porosity is created in some sandy beds due to feldspar dissolution and these beds serve as gas conduits. Methane production rates with shale as substrate in the laboratory are dependent on the kind of hydrocarbon-degrading microbial enrichment cultures used in the incubation experiments, ranging from 10-620 nmol/(g*d). In these experiments, the CO{sub 2} production rate was always higher than for methane. Like the northern part of North America, also Northern European has been covered by glaciers during the Pleistocene and similar geological processes may have developed leading to biogenic shale gas formation. For the Antrim Shale one hypothesis suggests that fresh waters, recharged from Pleistocene glaciation and modern precipitation, suppressed basinal brine salinity along the northern margins of the Michigan Basin to greater depths and thereby enhancing methanogenesis

Non-methane hydrocarbons in a controlled ecological life support system.

Science.gov (United States)

Dai, Kun; Yu, Qingni; Zhang, Zhou; Wang, Yuan; Wang, Xinming

2018-02-01

Non-methane hydrocarbons (NMHCs) are vital to people's health and plants' growth, especially inside a controlled ecological life support system (CELSS) built for long-term space explorations. In this study, we measured 54 kinds of NMHCs to study their changing trends in concentration levels during a 4-person-180-day integrated experiment inside a CELSS with four cabins for plants growing and other two cabins for human daily activities and resources management. During the experiment, the total mixing ratio of measured NMHCs was 423 ± 283 ppbv at the first day and it approached 2961 ± 323 ppbv ultimately. Ethane and propane were the most abundant alkanes and their mixing ratios kept growing from 27.5 ± 19.4 and 31.0 ± 33.6 ppbv to 2423 ± 449 ppbv and 290 ± 10 ppbv in the end. For alkenes, ethylene and isoprene presented continuously fluctuating states during the experimental period with average mixing ratios of 30.4 ± 19.3 ppbv, 7.4 ± 5.8 ppbv. For aromatic hydrocarbons, the total mixing ratios of benzene, toluene, ethylbenzene and xylenes declined from 48.0 ± 44 ppbv initially to 3.8 ± 1.1 ppbv ultimately. Biomass burning, sewage treatment, construction materials and plants all contributed to NMHCs inside CELSS. In conclusion, the results demonstrate the changing trends of NMHCs in a long-term closed ecological environment's atmosphere which provides valuable information for both the atmosphere management of CELSS and the exploration of interactions between humans and the total environment. Copyright © 2017 Elsevier Ltd. All rights reserved.

Characteristics of atmospheric non-methane hydrocarbons during high PM 10 episodes and normal days in Foshan, China

Science.gov (United States)

Guo, Songjun; Tan, Jihua; Ma, Yongliang; Yang, Fumo; Yu, Yongchan; Wang, Jiewen

2011-08-01

Atmospheric non-methane hydrocarbons (NMHCs) were firstly studied during high PM 10 episodes and normal days in December 2008 in Foshan, China. Ethyne, ethene, i-pentane, toluene, ethane and propane are six abundant hydrocarbons, accounting for round 80% of total NMHCs. Both diurnal variations and concentration ratios of morning (evening)/afternoon implied vehicular emission for most hydrocarbons. Correlation coefficients (R 2) of ethene, propene, i-butene, benzene, toluene and i-/n-butanes with ethyne were 0.60-0.88 (they were 0.64-0.88 during high PM 10 episode and 0.60-0.85 in normal days) except for ethene and i-butene in normal days, indicating these hydrocarbons are mainly related to vehicular emission. It suggests liquefied petroleum gas (LPG) and natural gas (NG) leakages are responsible for propane and ethane, respectively. The measured mean benzene/toluene (B/T) ratio (wt/wt) was 0.45 ± 0.29 during total sampling periods together with R 2 analysis, again indicating vehicular emission is main contributor to ambient hydrocarbons. And the lower B/T ratio (0.29 ± 0.11) during high PM 10 episodes than that (0.75 ± 0.29) in normal days is likely caused by air transport containing low B/T value (0.23) from Guangzhou as well as solvent application containing toluene in Foshan.

The distribution of methane in groundwater in Alberta (Canada) and associated aqueous geochemistry conditions

Science.gov (United States)

Humez, Pauline; Mayer, Bernhard; Nightingale, Michael; Becker, Veith; Kingston, Andrew; Taylor, Stephen; Millot, Romain; Kloppmann, Wolfram

2016-04-01

Development of unconventional energy resources such as shale gas and coalbed methane has generated some public concern with regard to the protection of groundwater and surface water resources from leakage of stray gas from the deep subsurface. In terms of environmental impact to and risk assessment of shallow groundwater resources, the ultimate challenge is to distinguish: (a) natural in-situ production of biogenic methane, (b) biogenic or thermogenic methane migration into shallow aquifers due to natural causes, and (c) thermogenic methane migration from deep sources due to human activities associated with the exploitation of conventional or unconventional oil and gas resources. We have conducted a NSERC-ANR co-funded baseline study investigating the occurrence of methane in shallow groundwater of Alberta (Canada), a province with a long record of conventional and unconventional hydrocarbon exploration. Our objective was to assess the occurrence and sources of methane in shallow groundwaters and to also characterize the hydrochemical environment in which the methane was formed or transformed through redox processes. Ultimately our aim was to determine whether methane was formed in-situ or whether it migrated from deeper formations into shallow aquifers. Combining hydrochemical and dissolved and free geochemical gas data from 372 groundwater samples obtained from 186 monitoring wells of the provincial groundwater observation well network (GOWN) in Alberta, it was found that methane is ubiquitous in groundwater in Alberta and is predominantly of biogenic origin. The highest concentrations of dissolved biogenic methane (> 0.01 mM or > 0.2 mg/L), characterized by δ13CCH4 values deep thermogenic gas that had migrated in significant amounts into shallow aquifers either naturally or via anthropogenically induced pathways. This study shows that the combined interpretation of aqueous geochemistry data in concert with the chemical and isotopic composition of dissolved and

Estimating the biogenic emissions of non-methane volatile organic compounds from the North Western Mediterranean vegetation of Catalonia, Spain

International Nuclear Information System (INIS)

Parra, R.; Gasso, S.; Baldasano, J.M.

2004-01-01

An estimation of the magnitude of non-methane volatile organic compounds (NMVOCs) emitted by vegetation in Catalonia (NE of the Iberian Peninsula, Spain), in addition to their superficial and temporal distribution, is presented for policy and scientific (photochemical modelling) purposes. It was developed for the year 2000, for different time resolutions (hourly, daily, monthly and annual) and using a high-resolution land-use map (1-km 2 squared cells). Several meteorological surface stations provided air temperature and solar radiation data. An adjusted mathematical emission model taking account of Catalonia's conditions was built into a geographic information system (GIS) software. This estimation uses the latest information, mainly relating to: (1) emission factors; (2) better knowledge of the composition of Catalonia's forest cover; and (3) better knowledge of the particular emission behaviour of some Mediterranean vegetal species. Results depict an annual cycle with increasing values in the March-April period with the highest emissions in July-August, followed by a decrease in October-November. Annual biogenic NMVOCs emissions reach 46.9 kt, with monoterpenes the most abundant species (24.7 kt), followed by other biogenic volatile organic compounds (e.g. alcohols, aldehydes and acetone) (16.3 kt), and isoprene (5.9 kt). These compounds signify 52%, 35% and 13%, respectively, of total emission estimates. Peak hourly total emission for a winter day could be less than 10% of the corresponding value for a summer day

Non-oxidative conversion of methane into higher hydrocarbons over ...

Indian Academy of Sciences (India)

SOURABH MISHRA

2017-09-27

Sep 27, 2017 ... ... in the Design and Development of Catalysts and their Applications ... of methane (natural gas) into transportable chemicals ... molybdenum (Mo) catalyst under non-oxidative condi- ... Micromeritics ASAP 2010 apparatus at liquid nitrogen tem- ... fixed-bed tubular reactor (500 mm length & 15 mm ID) at.

Characterization of non-methane hydrocarbons in Asian summer monsoon outflow observed by the CARIBIC aircraft

Directory of Open Access Journals (Sweden)

A. K. Baker

2011-01-01

Full Text Available Between April and December 2008 the CARIBIC commercial aircraft conducted monthly measurement flights between Frankfurt, Germany and Chennai, India. These flights covered the period of the Asian summer monsoon (June–September, during which enhancements in a number of atmospheric species were observed in the upper troposphere over southwestern Asia. In addition to in situ measurements of trace gases and aerosols, whole air samples were collected during the flights, and these were subsequently analyzed for a suite of trace gases that included a number of C₂–C₈ non-methane hydrocarbons. Non-methane hydrocarbons are relatively short-lived compounds and the large enhancements in their mixing ratios in the upper troposphere over southwestern Asia during the monsoon, sometimes more than double their spring and fall means, provides qualitative evidence for the influence of convectively uplifted boundary layer air. The particularly large enhancements of the combustion tracers benzene and ethyne, along with the similarity of their ratios with carbon monoxide and emission ratios from the burning of household biofuels, indicate a strong influence of biofuel burning to NMHC emissions in this region. Conversely, the ratios of ethane and propane to carbon monoxide, along with the ratio between i-butane and n-butane, indicate a significant source of these compounds from the use of fossil fuels, and comparison to previous campaigns suggests that this source could be increasing. Photochemical aging patterns of NMHCs showed that the CARIBIC samples were collected in two distinctly different regions of the monsoon circulation: a southern region where air masses had been recently influenced by low level contact and a northern region, where air parcels had spent substantial time in transit in the upper troposphere before being probed. Estimates of age using ratios of individual NMHCs have ranges of 3–6 days in the south and 9–12 days in

Conversion of Methane to C2 Hydrocarbons and Hydrogen Using a Gliding Arc Reactor

International Nuclear Information System (INIS)

Hu Shuanghui; Wang Baowei; Lv Yijun; Yan Wenjuan

2013-01-01

Methane conversion has been studied using gliding arc plasma in the presence of argon. The process was conducted at atmospheric pressure and ambient temperature. The focus of this research was to develop a process of converting methane to C 2 hydrocarbons and hydrogen. The main parameters, including the CH 4 /Ar mole ratio, the CH 4 flow rate, the input voltage, and the minimum electrode gap, were varied to investigate their effects on methane conversion rate, product distribution, energy consumption, carbon deposit, and reaction stability. The specific energy requirement (SER) was used to express the energy utilization efficiency of the process and provided a practical guidance for optimizing reaction conditions for improving energy efficiency. It was found that the carbon deposition was not conducive to methane conversion, and the gliding arc plasma discharge reached a stable state twelve minutes later. Optimum conditions for methane conversion were suggested. The maximum methane conversion rate of 43.39% was obtained under the optimum conditions. Also, C 2 hydrocarbons selectivity, C 2 hydrocarbons yield, H 2 selectivity, H 2 yield and SER were 87.20%, 37.83%, 81.28%, 35.27%, and 2.09 MJ/mol, respectively.

Interactive chemistry in the Laboratoire de Météorologie Dynamique general circulation model: model description and impact analysis of biogenic hydrocarbons on tropospheric chemistry

Directory of Open Access Journals (Sweden)

G. A. Folberth

2006-01-01

Full Text Available We present a description and evaluation of LMDz-INCA, a global three-dimensional chemistry-climate model, pertaining to its recently developed NMHC version. In this substantially extended version of the model a comprehensive representation of the photochemistry of non-methane hydrocarbons (NMHC and volatile organic compounds (VOC from biogenic, anthropogenic, and biomass-burning sources has been included. The tropospheric annual mean methane (9.2 years and methylchloroform (5.5 years chemical lifetimes are well within the range of previous modelling studies and are in excellent agreement with estimates established by means of global observations. The model provides a reasonable simulation of the horizontal and vertical distribution and seasonal cycle of CO and key non-methane VOC, such as acetone, methanol, and formaldehyde as compared to observational data from several ground stations and aircraft campaigns. LMDz-INCA in the NMHC version reproduces tropospheric ozone concentrations fairly well throughout most of the troposphere. The model is applied in several sensitivity studies of the biosphere-atmosphere photochemical feedback. The impact of surface emissions of isoprene, acetone, and methanol is studied. These experiments show a substantial impact of isoprene on tropospheric ozone and carbon monoxide concentrations revealing an increase in surface O3 and CO levels of up to 30 ppbv and 60 ppbv, respectively. Isoprene also appears to significantly impact the global OH distribution resulting in a decrease of the global mean tropospheric OH concentration by approximately 0.7×105 molecules cm-3 or roughly 8% and an increase in the global mean tropospheric methane lifetime by approximately seven months. A global mean ozone net radiative forcing due to the isoprene induced increase in the tropospheric ozone burden of 0.09 W m-2 is found. The key role of isoprene photooxidation in the global tropospheric redistribution of NOx is demonstrated. LMDz

Fingerprinting of petroleum hydrocarbons (PHC) and other biogenic organic compounds (BOC) in oil-contaminated and background soil samples.

Science.gov (United States)

Wang, Zhendi; Yang, C; Yang, Z; Hollebone, B; Brown, C E; Landriault, M; Sun, J; Mudge, S M; Kelly-Hooper, F; Dixon, D G

2012-09-01

Total petroleum hydrocarbons (TPH) or petroleum hydrocarbons (PHC) are one of the most widespread soil contaminants in Canada, the United States and many other countries worldwide. Clean-up of PHC-contaminated soils costs the Canadian economy hundreds of millions of dollars annually. In Canada, most PHC-contaminated site evaluations are based on the methods developed by the Canadian Council of the Ministers of the Environment (CCME). However, the CCME method does not differentiate PHC from BOC (the naturally occurring biogenic organic compounds), which are co-extracted with petroleum hydrocarbons in soil samples. Consequently, this could lead to overestimation of PHC levels in soil samples. In some cases, biogenic interferences can even exceed regulatory levels (300 μg g(-1) for coarse soils and 1300 μg g(-1) for fine soils for Fraction 3, C(16)-C(34) range, in the CCME Soil Quality Level). Resulting false exceedances can trigger unnecessary and costly cleanup or remediation measures. Therefore, it is critically important to develop new protocols to characterize and quantitatively differentiate PHC and BOC in contaminated soils. The ultimate objective of this PERD (Program of Energy Research and Development) project is to correct the misconception that all detectable hydrocarbons should be regulated as toxic petroleum hydrocarbons. During 2009-2010, soil and plant samples were collected from over forty oil-contaminated and paired background sites in various provinces. The silica gel column cleanup procedure was applied to effectively remove all target BOC from the oil-contaminated sample extracts. Furthermore, a reliable GC-MS method in combination with the derivatization technique, developed in this laboratory, was used for identification and characterization of various biogenic sterols and other major biogenic compounds in these oil-contaminated samples. Both PHC and BOC in these samples were quantitatively determined. This paper reports the characterization

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

Science.gov (United States)

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

2014-12-01

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

Discovery of Widespread Biogenic Methane Emissions and Authigenic Carbonate Mound-like Structures at the Aquitaine Shelf (Bay of Biscay)

Science.gov (United States)

Dupré, S.; Loubrieu, B.; Scalabrin, C.; Ehrhold, A.; Gautier, E.; Ruffine, L.; Pierre, C.; Battani, A.; Le Bouffant, N.; Berger, L.

2014-12-01

Fishery acoustic surveys conducted in the Bay of Biscay (1998-2012) and dedicated to monitoring and predicting pelagic ecosystem evolution reveal numerous active seeps on the Aquitaine Shelf, east of the shelf break (Dupré et al. 2014). Seafloor and water column acoustic investigation with the use of ship-borne multibeam echosounder in 2013 (Gazcogne1 marine expedition) confirmed the presence of numerous (> 3000) persistent and widespread gas emission sites at water depths ranging from ~140 to 180 m. These fluid emissions are associated at the seafloor with high backscatter subcircular small-scale mounds, on average less than 2 m high and a few meters in diameter. Near-bottom visual observations and samplings were conducted with the ROV (Remotely Operated Vehicle) Victor (Gazcogne2 expedition). The whole mounds cover an area of ~200 km2 of the seabed, and are by-products of gas seepage, i.e. methane-derived authigenic carbonates. The spatial distribution of the seeps and related structures, based on water column acoustic gas flares and high backscatter seabed patches, appears to be relatively broad, with a North-South extension of ~80 km across the Parentis Basin and the Landes High, and a West-East extension along a few kilometers wide on the shelf, up to 8 km. Gas bubbles sampled at in situ conditions are principally composed of biogenic methane, possibly originated from Late Pleistocene deposits. The volume of methane emitted into the water column is abundant i) with an average gas flux varying locally from 0.035 to 0.37 Ln/min and ii) with regard to the time needed for the precipitation of the authigenic carbonates identified both at the seabed and in the upper most sedimentary column. The GAZCOGNE study is co-funded by TOTAL and IFREMER as part of the PAMELA (Passive Margin Exploration Laboratories) scientific project. ReferenceDupré, S., Berger, L., Le Bouffant, N., Scalabrin, C., and Bourillet, J.-F., 2014. Fluid emissions at the Aquitaine Shelf (Bay of

The effects of fire on biogenic emissions of methane and nitric oxide from wetlands

Science.gov (United States)

Levine, Joel S.; Cofer, Wesley R., III; Sebacher, Daniel I.; Rhinehart, Robert P.; Winstead, Edward L.; Sebacher, Shirley; Hinkle, C. Ross; Schmalzer, Paul A.; Koller, Albert M., Jr.

1990-01-01

Enhanced emissions of methane (CH4) and nitric oxide (NO) were measured following three controlled burns in a Florida wetlands in 1987 and 1988. Wetlands are the major global source of methane resulting from metabolic activity of methanogenic bacteria. Methanogens require carbon dioxide, acetate, or formate for their growth and the metabolic production of methane. All three water-soluble compounds are produced in large concentrations during biomass burning. Postfire methane emissions exceeded 0.15 g CH 4/sq m per day. Preburn and postburn measurements of soil nutrients indicate significant postburn increases in soil ammonium, from 8.35 to 13.49 parts per million (ppm) in the upper 5 cm of the Juncus marsh and from 8.83 to 23.75 ppm in the upper 5 cm of the Spartina marsh. Soil nitrate concentrations were found to decrease in both marshes after the fire. These measurements indicate that the combustion products of biomass burning exert an important 'fertilizing' effect on the biosphere and on the biogenic production of environmentally significant atmospheric gases.

Sensitivity of modeled ozone concentrations to uncertainties in biogenic emissions

International Nuclear Information System (INIS)

Roselle, S.J.

1992-06-01

The study examines the sensitivity of regional ozone (O3) modeling to uncertainties in biogenic emissions estimates. The United States Environmental Protection Agency's (EPA) Regional Oxidant Model (ROM) was used to simulate the photochemistry of the northeastern United States for the period July 2-17, 1988. An operational model evaluation showed that ROM had a tendency to underpredict O3 when observed concentrations were above 70-80 ppb and to overpredict O3 when observed values were below this level. On average, the model underpredicted daily maximum O3 by 14 ppb. Spatial patterns of O3, however, were reproduced favorably by the model. Several simulations were performed to analyze the effects of uncertainties in biogenic emissions on predicted O3 and to study the effectiveness of two strategies of controlling anthropogenic emissions for reducing high O3 concentrations. Biogenic hydrocarbon emissions were adjusted by a factor of 3 to account for the existing range of uncertainty in these emissions. The impact of biogenic emission uncertainties on O3 predictions depended upon the availability of NOx. In some extremely NOx-limited areas, increasing the amount of biogenic emissions decreased O3 concentrations. Two control strategies were compared in the simulations: (1) reduced anthropogenic hydrocarbon emissions, and (2) reduced anthropogenic hydrocarbon and NOx emissions. The simulations showed that hydrocarbon emission controls were more beneficial to the New York City area, but that combined NOx and hydrocarbon controls were more beneficial to other areas of the Northeast. Hydrocarbon controls were more effective as biogenic hydrocarbon emissions were reduced, whereas combined NOx and hydrocarbon controls were more effective as biogenic hydrocarbon emissions were increased

Process for manufacture of a catalyst suitable for the steam reforming of hydrocarbons and for obtaining methane

Energy Technology Data Exchange (ETDEWEB)

Golebiowski, A.; Romotowski, T.; Hennel, W.; Wroblewska-Wroblewska, T.; Polanski, A.; Janecki, Z.; Paluch-Paluch, S.

1982-07-29

The invention concerns a process for the manufacture of a catalyst suitable for the steam reforming of hydrocarbons or for obtaining methane, by the deposition of the catalytic components on a metal carrier with a large surface area, particularly a process for the manufacture of a solid nickel catalyst, which is suitable for the steam reforming of hydrocarbons, particularly of methane. The following steps of the process are carried out: producing a highly porous layer of spongy metal from Ni powder on the side of a metal wall away from a heat medium, which separates the reaction mixture from the heat medium, then separate application of a non-reducing oxide (Al/sub 2/O/sub 3/) and a reducing oxide (nickel oxide) on the spongy metal by soaking with metal salt solution and then roasting in the temperature range of 400 to 1200/sup 0/C.

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

Science.gov (United States)

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

2018-01-01

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

Hydrocarbon-degrading sulfate-reducing bacteria in marine hydrocarbon seep sediments

OpenAIRE

Kleindienst, Sara

2012-01-01

Microorganisms are key players in our biosphere because of their ability to degrade various organic compounds including a wide range of hydrocarbons. At marine hydrocarbon seeps, more than 90% of sulfate reduction (SR) is potentially coupled to non-methane hydrocarbon oxidation. Several hydrocarbon-degrading sulfate-reducing bacteria (SRB) were enriched or isolated from marine sediments. However, in situ active SRB remained largely unknown. In the present thesis, the global distribution and a...

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

Science.gov (United States)

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.

The ABAG biogenic emissions inventory project

Science.gov (United States)

Carson-Henry, C. (Editor)

1982-01-01

The ability to identify the role of biogenic hydrocarbon emissions in contributing to overall ozone production in the Bay Area, and to identify the significance of that role, were investigated in a joint project of the Association of Bay Area Governments (ABAG) and NASA/Ames Research Center. Ozone, which is produced when nitrogen oxides and hydrocarbons combine in the presence of sunlight, is a primary factor in air quality planning. In investigating the role of biogenic emissions, this project employed a pre-existing land cover classification to define areal extent of land cover types. Emission factors were then derived for those cover types. The land cover data and emission factors were integrated into an existing geographic information system, where they were combined to form a Biogenic Hydrocarbon Emissions Inventory. The emissions inventory information was then integrated into an existing photochemical dispersion model.

Modeling and direct sensitivity analysis of biogenic emissions impacts on regional ozone formation in the Mexico-U.S. border area.

Science.gov (United States)

Mendoza-Dominguez, A; Wilkinson, J G; Yang, Y J; Russell, A G

2000-01-01

A spatially and temporally resolved biogenic hydrocarbon and nitrogen oxides (NOx) emissions inventory has been developed for a region along the Mexico-U.S. border area. Average daily biogenic non-methane organic gases (NMOG) emissions for the 1700 x 1000 km2 domain were estimated at 23,800 metric tons/day (62% from Mexico and 38% from the United States), and biogenic NOx was estimated at 1230 metric tons/day (54% from Mexico and 46% from the United States) for the July 18-20, 1993, ozone episode. The biogenic NMOG represented 74% of the total NMOG emissions, and biogenic NOx was 14% of the total NOx. The CIT photochemical airshed model was used to assess how biogenic emissions impact air quality. Predicted ground-level ozone increased by 5-10 ppb in most rural areas, 10-20 ppb near urban centers, and 20-30 ppb immediately downwind of the urban centers compared to simulations in which only anthropogenic emissions were used. A sensitivity analysis of predicted ozone concentration to emissions was performed using the decoupled direct method for three dimensional air quality models (DDM-3D). The highest positive sensitivity of ground-level ozone concentration to biogenic volatile organic compound (VOC) emissions (i.e., increasing biogenic VOC emissions results in increasing ozone concentrations) was predicted to be in locations with high NOx levels, (i.e., the urban areas). One urban center--Houston--was predicted to have a slight negative sensitivity to biogenic NO emissions (i.e., increasing biogenic NO emissions results in decreasing local ozone concentrations). The highest sensitivities of ozone concentrations to on-road mobile source VOC emissions, all positive, were mainly in the urban areas. The highest sensitivities of ozone concentrations to on-road mobile source NOx emissions were predicted in both urban (either positive or negative sensitivities) and rural (positive sensitivities) locations.

Non-aromatic hydrocarbons in surface sediments near the Pearl River estuary in the South China Sea

International Nuclear Information System (INIS)

Gao Xuelu; Chen Shaoyong; Xie Xueliang; Long Aimin; Ma Fujun

2007-01-01

Surface sediment samples at 4 sites along an offshore transect from outer continental shelf off the Pearl River estuary to the shelf slope region of the northern South China Sea, have been analyzed for total organic carbon (TOC), total nitrogen (TN), solvent extractable organic matter (EOM) and non-aromatic hydrocarbons. TOC, TN and EOM show distinct spatial variations. Their highest values are all recorded at the shelf slope region. EOM varies from 18.70-38.58 μg g -1 dry sediment and accounts for 0.20-0.72% of the TOC contents. The non-aromatic hydrocarbons are an important fraction of EOM. Their contents range from 3.43-7.06 μg g -1 dry sediment. n-Alkanes with carbon number ranging from 15-38 are identified. They derive from both biogenic and petrogenic sources in different proportions. Results of isoprenoid hydrocarbons, hopanes and steranes also suggest possible petroleum contamination. - Anthropogenic activities have influences on the composition of non-aromatic hydrocarbons in the surface sediments of the northern South China Sea outer continental shelf

Methylotrophic methanogenesis governs the biogenic coal bed methane formation in Eastern Ordos Basin, China

Energy Technology Data Exchange (ETDEWEB)

Guo, Hongguang; Yu, Zhisheng; Liu, Ruyin [Graduate Univ. of Chinese Academy of Sciences, Beijing (China). College of Resources and Environment; Zhang, Hongxun [Graduate Univ. of Chinese Academy of Sciences, Beijing (China). College of Resources and Environment; Chinese Academy of Sciences, Beijing (China). Research Center for Eco-Environmental Sciences; Zhong, Qiding; Xiong, Zhenghe [China National Research Institute of Food and Fermentation Industries, Beijing (China). Food Analysis using Isotope Technology Lab

2012-12-15

To identify the methanogenic pathways present in a deep coal bed methane (CBM) reservoir associated with Eastern Ordos Basin in China, a series of geochemical and microbiological studies was performed using gas and water samples produced from the Liulin CBM reservoir. The composition and stable isotopic ratios of CBM implied a mixed biogenic and thermogenic origin of the methane. Archaeal 16S rRNA gene analysis revealed the dominance of the methylotrophic methanogen Methanolobus in the water produced. The high potential of methane production by methylotrophic methanogens was found in the enrichments using the water samples amended with methanol and incubated at 25 and 35 C. Methylotrophic methanogens were the dominant archaea in both enrichments as shown by polymerase chain reaction (PCR)-denaturing gradient gel electrophoresis (DGGE). Bacterial 16S rRNA gene analysis revealed that fermentative, sulfate-reducing, and nitrate-reducing bacteria inhabiting the water produced were a factor in coal biodegradation to fuel methanogens. These results suggested that past and ongoing biodegradation of coal by methylotrophic methanogens and syntrophic bacteria, as well as thermogenic CBM production, contributed to the Liulin CBM reserves associated with the Eastern Ordos Basin. (orig.)

Biochemically enhanced methane production from coal

Science.gov (United States)

Opara, Aleksandra

For many years, biogas was connected mostly with the organic matter decomposition in shallow sediments (e.g., wetlands, landfill gas, etc.). Recently, it has been realized that biogenic methane production is ongoing in many hydrocarbon reservoirs. This research examined microbial methane and carbon dioxide generation from coal. As original contributions methane production from various coal materials was examined in classical and electro-biochemical bench-scale reactors using unique, developed facultative microbial consortia that generate methane under anaerobic conditions. Facultative methanogenic populations are important as all known methanogens are strict anaerobes and their application outside laboratory would be problematic. Additional testing examined the influence of environmental conditions, such as pH, salinity, and nutrient amendments on methane and carbon dioxide generation. In 44-day ex-situ bench-scale batch bioreactor tests, up to 300,000 and 250,000 ppm methane was generated from bituminous coal and bituminous coal waste respectively, a significant improvement over 20-40 ppm methane generated from control samples. Chemical degradation of complex hydrocarbons using environmentally benign reagents, prior to microbial biodegradation and methanogenesis, resulted in dissolution of up to 5% bituminous coal and bituminous coal waste and up to 25% lignite in samples tested. Research results confirm that coal waste may be a significant underutilized resource that could be converted to useful fuel. Rapid acidification of lignite samples resulted in low pH (below 4.0), regardless of chemical pretreatment applied, and did not generate significant methane amounts. These results confirmed the importance of monitoring and adjusting in situ and ex situ environmental conditions during methane production. A patented Electro-Biochemical Reactor technology was used to supply electrons and electron acceptor environments, but appeared to influence methane generation in a

Hydrogen generation from biogenic and fossil fuels by autothermal reforming

Science.gov (United States)

Rampe, Thomas; Heinzel, Angelika; Vogel, Bernhard

Hydrogen generation for fuel cell systems by reforming technologies from various fuels is one of the main fields of investigation of the Fraunhofer ISE. Suitable fuels are, on the one hand, gaseous hydrocarbons like methane, propane but also, on the other hand, liquid hydrocarbons like gasoline and alcohols, e.g., ethanol as biogenic fuel. The goal is to develop compact systems for generation of hydrogen from fuel being suitable for small-scale membrane fuel cells. The most recent work is related to reforming according to the autothermal principle — fuel, air and steam is supplied to the reactor. Possible applications of such small-scale autothermal reformers are mobile systems and also miniature fuel cell as co-generation plant for decentralised electricity and heat generation. For small stand-alone systems without a connection to the natural gas grid liquid gas, a mixture of propane and butane is an appropriate fuel.

Evidence for the microbial in situ conversion of oil to methane in the Dagang oilfield

Energy Technology Data Exchange (ETDEWEB)

Jimenez, N.; Richnow, H.H. [Helmholtz-Zentrum fuer Umweltforschung (UFZ), Leipzig (Germany). Abt. Isotopenbiogeochemie; Cai, M. [Helmholtz-Zentrum fuer Umweltforschung (UFZ), Leipzig (Germany). Abt. Isotopenbiogeochemie; University of Science and Technology, Beijing (China). School of Civil and Environment Engineering; Straaten, N.; Krueger, M. [Bundesanstalt fuer Geowissenschaften und Rohstoffe BGR Geozentrum (BGR), Hannover (Germany). Fachbereich Geochemie der Rohstoffe; Yao, Jun [University of Science and Technology, Beijing (China). School of Civil and Environment Engineering

2013-08-01

In situ biotransformation of oil to methane was investigated in a reservoir in Dagang, China using chemical fingerprinting, isotopic analyses, and molecular and biological methods. The reservoir is highly methanogenic despite chemical indications of advanced oil degradation, such as depletion of n-alkanes, alkylbenzenes, and light polycyclic aromatic hydrocarbon (PAHs) fractions or changes in the distribution of several alkylated polycyclic aromatic hydrocarbons. The degree of degradation strongly varied between different parts of the reservoir, ranging from severely degraded to nearly undegraded oil compositions. Geochemical data from oil, water and gas samples taken from the reservoir are consistent with in situ biogenic methane production linked to aliphatic and aromatic hydrocarbon degradation. Microcosms were inoculated with production and injection waters in order to characterize these processes in vitro. Subsequent degradation experiments revealed that autochthonous microbiota are capable of producing methane from {sup 13}C-labelled n-hexadecane or 2-methylnaphthalene, and suggest that further methanogenesis may occur from the aromatic and polyaromatic fractions of Dagang reservoir fluids. The microbial communities from produced oil-water samples were composed of high numbers of microorganisms (on the order to 10{sup 7}), including methane-producing Archaea within the same order of magnitude. In summary, the investigated sections of the Dagang reservoir may have significant potential for testing the viability of in situ conversion of oil to methane as an enhanced recovery method, and biodegradation of the aromatic fractions of the oil may be an important methane source. (orig.)

New life in old reservoirs - the microbial conversion of oil to methane

Science.gov (United States)

Gründger, Friederike; Feisthauer, Stefan; Richnow, Hans Hermann; Siegert, Michael; Krüger, Martin

2010-05-01

Since almost 20 years it is known from stable isotope studies that large amounts of biogenic methane are formed in oil reservoirs. The investigation of this degradation process and of the underlying biogeochemical controls are of economical and social importance, since even under optimal conditions, not more than 30-40 % of the oil in a reservoir is actually recovered. The conversion of parts of this non-recoverable oil via an appropriate biotechnological treatment into easily recoverable methane would provide an extensive and ecologically sound energy resource. Laboratory mesocosm as well as high pressure autoclave experiments with samples from different geosystems showed high methane production rates after the addition of oils, single hydrocarbons or coals. The variation of parameters, like temperature, pressure or salinity, showed a broad tolerance to environmental conditions. The fingerprinting of the microbial enrichments with DGGE showed a large bacterial diversity while that of Archaea was limited to three to four dominant species. The Q-PCR results showed the presence of high numbers of Archaea and Bacteria. To analyse their function, we measured the abundances of genes indicative of metal reduction (16S rRNA gene for Geobacteraceae), sulphate reduction (sulphate reductase, dsr), and methanogenesis (methyl coenzyme M-reductase, mcrA). The methanogenic consortia will be further characterised to determine enzymatic pathways and the individual role of each partner. Degradation pathways for different compounds will be studied using 13C-labelled substrates and molecular techniques. Our stable isotope data from both, methane produced in our incubations with samples from various ecosystems and field studies, implies a common methanogenic biodegradation mechanism, resulting in consistent patterns of hydrocarbon alteration.

Microbial conversion of higher hydrocarbons to methane in oil and coal reservoirs

Energy Technology Data Exchange (ETDEWEB)

Kruger, Martin; Beckmaann, Sabrina; Siegert, Michael; Grundger, Friederike; Richnow, Hans [Geomicrobiology Group, Federal Institute for Geosciences and Natural Resources (Germany)

2011-07-01

In recent years, oil production has increased enormously but almost half of the oil now remaining is heavy/biodegraded and cannot be put into production. There is therefore a need for new technology and for diversification of energy sources. This paper discusses the microbial conversion of higher hydrocarbons to methane in oil and coal reservoirs. The objective of the study is to identify microbial and geochemical controls on methanogenesis in reservoirs. A graph shows the utilization of methane for various purposes in Germany from 1998 to 2007. A degradation process to convert coal to methane is shown using a flow chart. The process for converting oil to methane is also given. Controlling factors include elements such as Fe, nitrogen and sulfur. Atmospheric temperature and reservoir pressure and temperature also play an important role. From the study it can be concluded that isotopes of methane provide exploration tools for reservoir selection and alkanes and aromatic compounds provide enrichment cultures.

Organic pollutants in the coastal environment off San Diego, California. 2: Petrogenic and biogenic sources of aliphatic hydrocarbons

International Nuclear Information System (INIS)

Tran, K.; Yu, C.C.; Zeng, E.Y.

1997-01-01

The results from the measurements of aliphatic hydrocarbons suggest that hydrocarbons suggest that hydrocarbons in the Point Loma Wastewater Treatment Plant (PLWTP) effluents are mainly petroleum derived; those in the Tijuana River runoff have largely originated from terrestrial plants with visible petroleum contamination; and those in the sea surface microlayer, sediment traps, and sediments at various coastal locations off San Diego have mostly resulted from biogenic contributions with enhanced microbial products in the summer season. Rainfall in the winter season appeared to amplify the inputs from terrestrial higher plants to the coastal areas. The PLWTP discharged approximately 3.85 metric tons of n-alkanes (C 10 -C 35 ) in 1994, well below the level (136 metric tons) estimated in 1979. The input of aliphatic hydrocarbons from the Tijuana River was about 0.101 metric tons in 1994. Diffusion, solubilization, evaporation, and microbial degradation seemed partially responsible for the difference in the concentrations and compositions of aliphatic hydrocarbons in different sample media, although the relative importance of each mechanism cannot be readily discerned from the available data. The results from analyses of aliphatic hydrocarbon compositional indices are generally consistent with those of polycyclic aromatic hydrocarbons

Occurrence and origin of methane in groundwater in Alberta (Canada): Gas geochemical and isotopic approaches

International Nuclear Information System (INIS)

Humez, P.; Mayer, B.; Ing, J.; Nightingale, M.; Becker, V.; Kingston, A.; Akbilgic, O.; Taylor, S.

2016-01-01

To assess potential future impacts on shallow aquifers by leakage of natural gas from unconventional energy resource development it is essential to establish a reliable baseline. Occurrence of methane in shallow groundwater in Alberta between 2006 and 2014 was assessed and was ubiquitous in 186 sampled monitoring wells. Free and dissolved gas sampling and measurement approaches yielded comparable results with low methane concentrations in shallow groundwater, but in 28 samples from 21 wells methane exceeded 10 mg/L in dissolved gas and 300,000 ppmv in free gas. Methane concentrations in free and dissolved gas samples were found to increase with well depth and were especially elevated in groundwater obtained from aquifers containing coal seams and shale units. Carbon isotope ratios of methane averaged − 69.7 ± 11.1‰ (n = 63) in free gas and − 65.6 ± 8.9‰ (n = 26) in dissolved gas. δ"1"3C values were not found to vary with well depth or lithology indicating that methane in Alberta groundwater was derived from a similar source. The low δ"1"3C values in concert with average δ"2H_C_H_4 values of − 289 ± 44‰ (n = 45) suggest that most methane was of biogenic origin predominantly generated via CO_2 reduction. This interpretation is confirmed by dryness parameters typically > 500 due to only small amounts of ethane and a lack of propane in most samples. Comparison with mud gas profile carbon isotope data revealed that methane in the investigated shallow groundwater in Alberta is isotopically similar to hydrocarbon gases found in 100–250 meter depths in the WCSB and is currently not sourced from thermogenic hydrocarbon occurrences in deeper portions of the basin. The chemical and isotopic data for methane gas samples obtained from Alberta groundwater provide an excellent baseline against which potential future impact of deeper stray gases on shallow aquifers can be assessed. - Highlights: • Analysis of gas geochemical data from 186 monitoring wells in

Occurrence and origin of methane in groundwater in Alberta (Canada): Gas geochemical and isotopic approaches

Energy Technology Data Exchange (ETDEWEB)

Humez, P., E-mail: phumez@ucalgary.ca [Department of Geoscience, University of Calgary, 2500 University Drive NW, Calgary, Alberta T2N 1N4 (Canada); Mayer, B.; Ing, J.; Nightingale, M.; Becker, V.; Kingston, A. [Department of Geoscience, University of Calgary, 2500 University Drive NW, Calgary, Alberta T2N 1N4 (Canada); Akbilgic, O. [Department of Geoscience, University of Calgary, 2500 University Drive NW, Calgary, Alberta T2N 1N4 (Canada); UTHSC-ORNL Center for Biomedical Informatics, 910 Madison Avenue, Memphis, TN, 38104 (United States); Taylor, S. [Department of Geoscience, University of Calgary, 2500 University Drive NW, Calgary, Alberta T2N 1N4 (Canada)

2016-01-15

To assess potential future impacts on shallow aquifers by leakage of natural gas from unconventional energy resource development it is essential to establish a reliable baseline. Occurrence of methane in shallow groundwater in Alberta between 2006 and 2014 was assessed and was ubiquitous in 186 sampled monitoring wells. Free and dissolved gas sampling and measurement approaches yielded comparable results with low methane concentrations in shallow groundwater, but in 28 samples from 21 wells methane exceeded 10 mg/L in dissolved gas and 300,000 ppmv in free gas. Methane concentrations in free and dissolved gas samples were found to increase with well depth and were especially elevated in groundwater obtained from aquifers containing coal seams and shale units. Carbon isotope ratios of methane averaged − 69.7 ± 11.1‰ (n = 63) in free gas and − 65.6 ± 8.9‰ (n = 26) in dissolved gas. δ{sup 13}C values were not found to vary with well depth or lithology indicating that methane in Alberta groundwater was derived from a similar source. The low δ{sup 13}C values in concert with average δ{sup 2}H{sub CH4} values of − 289 ± 44‰ (n = 45) suggest that most methane was of biogenic origin predominantly generated via CO{sub 2} reduction. This interpretation is confirmed by dryness parameters typically > 500 due to only small amounts of ethane and a lack of propane in most samples. Comparison with mud gas profile carbon isotope data revealed that methane in the investigated shallow groundwater in Alberta is isotopically similar to hydrocarbon gases found in 100–250 meter depths in the WCSB and is currently not sourced from thermogenic hydrocarbon occurrences in deeper portions of the basin. The chemical and isotopic data for methane gas samples obtained from Alberta groundwater provide an excellent baseline against which potential future impact of deeper stray gases on shallow aquifers can be assessed. - Highlights: • Analysis of gas geochemical data from 186

Source rock hydrocarbons. Present status

International Nuclear Information System (INIS)

Vially, R.; Maisonnier, G.; Rouaud, T.

2013-01-01

This report first presents the characteristics of conventional oil and gas system, and the classification of liquid and gaseous non conventional hydrocarbons, with the peculiar case of coal-bed methane. The authors then describe how source rock hydrocarbons are produced: production of shale oils and gases (horizontal drilling, hydraulic fracturing, exploitation) and of coal-bed methane and coal mine methane. In the next part, they address and discuss the environmental impact of source rock hydrocarbon production: installation footprint, water resource management, drilling fluids, fracturing fluids composition, toxicity and recycling, air pollution, induced seismicity, pollutions from other exploitation and production activities. They propose an overview of the exploitation and production of source rock gas, coal-bed gas and other non conventional gases in the world. They describe the current development and discuss their economic impacts: world oil context and trends in the USA, in Canada and other countries, impacts on the North American market, on the world oil industry, on refining industries, on the world oil balance. They analyse the economic impacts of non conventional gases: development potential, stakes for the world gas trade, consequence for gas prices, development opportunities for oil companies and for the transport sector, impact on CO 2 emissions, macro-economic impact in the case of the USA

Analysis of carbon stable isotope to determine the origin and migration of gaseous hydrocarbon in the Brazilian sedimentary basins

International Nuclear Information System (INIS)

Takaki, T.; Rodrigues, R.

1986-01-01

The carbon isotopic composition of natural gases to determine the origin and gaseous hydrocarbon migration of Brazilian sedimentar basins is analysed. The carbon isotopic ratio of methane from natural gases depends on the process of gas formation and stage of organic matter maturation. In the geochemical surface exploration the biogenic gases are differentiated from thermogenic gases, because the last one is isotopically heavier. As the isotopic composition of methane has not changed during migration, the migrated gases from deeper and more mature source rocks are identified by its relative 13 C enrichment. The methane was separated from chromatography and and the isotopic analysis was done with mass spectrometer. (M.C.K.) [pt

Formation of polycyclic aromatic hydrocarbons and soot in fuel-rich oxidation of methane in a laminar flow reactor

DEFF Research Database (Denmark)

Skjøth-Rasmussen, Martin Skov; Glarborg, Peter; Østberg, M.

2004-01-01

Conversion of methane to higher hydrocarbons, polycyclic aromatic hydrocarbons (PAHs), and soot was investigated under fuel-rich conditions in a laminar flow reactor. The effects of stoichiometry, dilution, and water vapor addition were studied at temperatures between 1073 and 1823 K. A chemical...... kinetic mechanism was established for methane oxidation, with emphasis on formation of higher hydrocarbons and PAH. A submodel for soot formation was adopted from the work of Frenklach and co-workers without changes. Modeling predictions showed good agreement with experimental results. Reactants, stable...... decrease with increasing addition of water vapor. The effect is described qualitatively by the reaction mechanism. The enhanced oxidation of acetylene is attributed to higher levels of hydroxyl radicals, formed from the reaction between the water vapor and hydrogen atoms....

Methane Conversion to C2 Hydrocarbons by Abnormal Glow Discharge at Atmospheric Pressure

International Nuclear Information System (INIS)

Dai Wei; Yu Hui; Chen Qi; Yin Yongxiang; Dai Xiaoyan

2005-01-01

Methane conversion to C 2 hydrocarbons has been investigated with the addition of hydrogen in a plasma reactor of abnormal glow discharge at atmospheric pressure. The aim of this experiment is to minimize coke formation and improve discharge stability. The typical conditions in the experiment are 300 ml of total feed flux and 400 W of discharge power. The experimental results show that methane conversion is from 91.6% to 35.2% in mol, acetylene selectivity is from 90.2% to 57.6%, and ethylene selectivity is approximately from 7.8% to 3.6%, where the coke increases gradually along with the increase of CH 4 /H 2 from 2: 8 to 9: 1. A stable discharge for a considerable running time can be obtained only at a lower ratio of CH 4 /H 2 2: 8 or 3: 7. These phenomena indicate that the coke deposition during methane conversion is obviously reduced by adding a large amount of hydrogen during an abnormal glow discharge. A qualitative interpretation is presented, namely, with abundant hydrogen, the possibility that hydrogen molecules are activated to hydrogen radicals is increased with the help of the abnormal glow discharge. These hydrogen radicals react with carbon radicals to form C 2 hydrocarbon products. Therefore, the deposition of coke is restrained

Responses of non-methane biogenic volatile organic compound emissions to climate change in boreal and subarctic ecosystems

Energy Technology Data Exchange (ETDEWEB)

Faubert, P.

2010-07-01

Non-methane biogenic volatile organic compound emissions (BVOCs) have important roles in the global atmospheric chemistry but their feedbacks to climate change are still unknown. This thesis reports one of the first estimates of BVOC emissions from boreal and subarctic ecosystems. Most importantly, this thesis assesses the BVOC emission responses to four effects of climate change in these ecosystems: (1) the direct effect of warming, and its indirect effects via (2) water table drawdown, (3) change in the vegetation composition, and (4) enhanced UV-B radiation. BVOC emissions were measured using a conventional chamber method in which the compounds were collected on adsorbent and later analyzed by gas chromatography-mass spectrometry. On a subarctic heath, warming by only 1.9-2.5 degC doubled the monoterpene and sesquiterpene emissions. Such a high increase of BVOC emissions under a conservative warming cannot be predicted by the current models, which underlines the importance of a focus on BVOC emissions from the Subarctic under climate change. On a subarctic peatland, enhanced UV-B did not affect the BVOC emissions but the water table level exerted the major effect. The water table drawdown experimentally applied on boreal peatland microcosms decreased the emissions of monoterpenes and other VOCs (BVOCs with a lifetime>1 d) for the hollows (wet microsites) and that of all BVOC groups for the lawns (moderately wet microsites). The warming treatment applied on the lawn microcosms decreased the isoprene emission. The removal of vascular plants in the hummock (dry microsites) microcosms decreased the emissions of monoterpenes while the emissions between the microcosms covered with Sphagnum moss and bare peat were not different. In conclusion, the results presented in this thesis indicate that climate change has complex effects on the BVOC emissions. These results make a significant contribution to improving the modeling of BVOC emissions for a better understanding of

Plasma conversion of methane into higher hydrocarbons at surfaces

Energy Technology Data Exchange (ETDEWEB)

Sackinger, W.M.; Kamath, V.A. [Univ. of Alaska, Fairbanks, AK (United States)

1995-12-31

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

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

NARCIS (Netherlands)

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 1250m 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

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

Science.gov (United States)

Hoerger, C. C.; Claude, 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.

2015-07-01

The performance of 18 European institutions involved in long-term non-methane hydrocarbon (NMHC) measurements in ambient air within the framework of the Global Atmosphere Watch (GAW) and the European Monitoring and Evaluation Programme (EMEP) was assessed with respect to data quality objectives (DQOs) of ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) and GAW. Compared to previous intercomparison studies the DQOs define a novel approach to assess and ensure a high quality of the measurements. Having already been adopted by GAW, the ACTRIS DQOs are demanding with deviations to a reference value of less than 5 % and a repeatability of better than 2 % for NMHC mole fractions above 0.1 nmol mol-1. The participants of the intercomparison analysed two dry gas mixtures in pressurised cylinders, a 30-component NMHC mixture in nitrogen (NMHC_N2) at approximately 1 nmol mol-1 and a whole air sample (NMHC_air), following a standardised operation procedure including zero- and calibration gas measurements. Furthermore, participants had to report details on their instruments and assess their measurement uncertainties. The NMHCs were analysed either by gas chromatography-flame ionisation detection (GC-FID) or by gas chromatography-mass spectrometry (GC-MS). For the NMHC_N2 measurements, 62 % of the reported values were within the 5 % deviation class corresponding to the ACTRIS DQOs. For NMHC_air, generally more frequent and larger deviations to the assigned values were observed, with 50 % of the reported values within the 5 % deviation class. 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). The performance of the participating laboratories were affected by the different measurement procedures such as the usage of a two-step vs. a one-step calibration, breakthroughs of C2-C3 hydrocarbons in the focussing trap, blank values in zero

Carbon and hydrogen isotope composition and C-14 concentration in methane from sources and from the atmosphere: Implications for a global methane budget

Science.gov (United States)

Wahlen, Martin

1994-01-01

The topics covered include the following: biogenic methane studies; forest soil methane uptake; rice field methane sources; atmospheric measurements; stratospheric samples; Antarctica; California; and Germany.

Investigation of Biogenic and Non-biogenic Methane Sources in Texas

Science.gov (United States)

Yang, S.; Talbot, R. W.; Liu, L.; Lan, X.

2016-12-01

Methane (CH4) is a potent greenhouse gas with its mixing ratio increasing in the global atmosphere. Texas is one of the significant areas where underestimation of CH4 emissions by the U.S. inventories are pronounced. This study focused on two areas of Texas: Houston, the energy capital of the world, and the Barnett Shale area which is one of the largest onshore natural gas fields in the United States. The investigation of background CH4 and the fingerprints of CH4 emissions are critical to understanding potential impacts of extensive nature gas operations in these two areas. One-year of stationary CH4 measurements were studied to deduce the regional background CH4 characteristics and to identify the principle CH4 sources in Houston. Key information concerning CH4 sources can be obtained through the stable carbon isotope δ13CH4 during two field campaigns using a state-of-the-art mobile laboratory. CH4 mixing ratio and δ13C in CH4 were sampled by two cavity ring-down spectrometers (CRDS), one of which is coupled to a custom air core 13C sampling device which can supply more than 600 measurements for each plume analysis. Here, we report results of the overall δ13CH4 values and CH4 emission signatures derived from thirty-three sources in the two studied areas, ranging from oil production and processing, waste managements and landfills, to livestock. δ13CH4 signatures of these sources vary from -76‰ to -23‰. Several repeated measurements were sampled to investigate the variability of source signatures. We investigated a case of unexpected massive CH4 leaking detected near the San Jacinto River Fleet site. At the regional scale, the comparison of background δ13CH4 signatures were conducted to obtain the difference of dominate CH4 sources in two study areas. At the local scale, the combination of tower and mobile lab measurements were used to estimate and characterize CH4 emissions in Houston. The results and findings can supply valuable references for the local

Non-enzymatic U(VI) interactions with biogenic mackinawite

Science.gov (United States)

Veeramani, H.; Qafoku, N. P.; Kukkadapu, R. K.; Murayama, M.; Hochella, M. F.

2011-12-01

Reductive immobilization of hexavalent uranium [U(VI)] by stimulation of dissimilatory metal and/or sulfate reducing bacteria (DMRB or DSRB) has been extensively researched as a remediation strategy for subsurface U(VI) contamination. These bacteria derive energy by reducing oxidized metals as terminal electron acceptors, often utilizing organic substrates as electron donors. Thus, when evaluating the potential for in-situ uranium remediation in heterogeneous subsurface media, it is important to understand how the presence of alternative electron acceptors such as Fe(III) and sulfate affect U(VI) remediation and the long term behavior and reactivity of reduced uranium. Iron, an abundant subsurface element, represents a substantial sink for electrons from DMRB, and the reduction of Fe(III) leads to the formation of dissolved Fe(II) or to reactive biogenic Fe(II)- and mixed Fe(II)/Fe(III)- mineral phases. Consequently, abiotic U(VI) reduction by reactive forms of biogenic Fe(II) minerals could be a potentially important process for uranium immobilization. In our study, the DMRB Shewanella putrefaciens CN32 was used to synthesize a biogenic Fe(II)-bearing sulfide mineral: mackinawite, that has been characterized by XRD, SEM, HRTEM and Mössbauer spectroscopy. Batch experiments involving treated biogenic mackinawite and uranium (50:1 molar ratio) were carried out at room temperature under strict anoxic conditions. Following complete removal of uranium from solution, the biogenic mackinawite was analyzed by a suite of analytical techniques including XAS, HRTEM and Mössbauer spectroscopy to determine the speciation of uranium and investigate concomitant Fe(II)-phase transformation. Determining the speciation of uranium is critical to success of a remediation strategy. The present work elucidates non-enzymatic/abiotic molecular scale redox interactions between biogenic mackinawite and uranium.

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

Science.gov (United States)

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.

Approaching Mars-like geochemical conditions in the laboratory: omission of artificial buffers and reductants in a study of biogenic methane production on a smectite clay.

Science.gov (United States)

Chastain, Brendon K; Kral, Timothy A

2010-11-01

Methanogens have not been shown to metabolize in conditions exactly analogous to those present in Mars' subsurface. In typical studies of methanogenic metabolism, nutrient-rich buffered media and reducing agents are added to the cultures in an attempt to optimize the environment for methanogen survival and growth. To study methanogens in more Mars-relevant laboratory conditions, efforts should be made to eliminate artificial media, buffers, and reducing agents from investigations of methanogenic metabolism. After preliminary work to compare methanogen viability on montmorillonite clay and JSC Mars-1 regolith simulant, a study was conducted to determine whether biological methanogenesis could occur in non-reduced, non-buffered environments containing only H(2), CO(2), montmorillonite, and the liquid fraction extracted from a montmorillonite/deionized water suspension. Biogenic methane was observed in the microenvironments despite the omission of traditional media, buffers, and reducing agents. Mean headspace methane concentration after 96 days of observation was 10.23% ± 0.64% (% vol ± SEM, n = 4). However, methane production was severely decreased with respect to reduced, buffered microenvironments (Day 28: 31.98% ± 0.19%, n = 3). Analysis of results and comparison to previous work indicate that montmorillonite clay has a strong ability to supply micronutrients necessary for methanogenic metabolism, and the liquid fraction from a montmorillonite/deionized water slurry can successfully be used as an alternative to reduced and buffered nutritive media in Mars-relevant studies of methanogenic metabolism.

Non-oxidative conversion of methane into higher hydrocarbons over ...

Indian Academy of Sciences (India)

SOURABH MISHRA

2017-09-27

Sep 27, 2017 ... (Syn-gas, CO+H2) formation via steam reforming, dry reforming or partial oxidation of methane ... Micromeritics ASAP 2010 apparatus at liquid nitrogen tem- perature. Nitrogen (N2) was the adsorbate ... some runs were carried out in triplicate and mass balance for all the runs was measured. Runs with a ...

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

Science.gov (United States)

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.

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

Science.gov (United States)

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

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

Science.gov (United States)

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.

The Potential for Methane Isotopologue Channels in GOSAT-2

Science.gov (United States)

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

The influence of macroscopic texture on biogenically-derived coalbed methane, Huntly coalfield, New Zealand

Energy Technology Data Exchange (ETDEWEB)

Mares, Tennille E. [Department of Geological Sciences, University of Canterbury, Private Bag 4800, Christchurch (New Zealand); Moore, Tim A. [Department of Geological Sciences, University of Canterbury, Private Bag 4800, Christchurch (New Zealand); Solid Energy NZ Ltd., P.O. Box 1303, Christchurch (New Zealand)

2008-10-02

Secondary biogenic gas content can be related to textural characteristics in Eocene age subbituminous coals from the Huntly coalfield, New Zealand. However, the relationships between the two major coal seams in the basin are considerably different despite their close stratigraphic proximity (less than 25 m). In this study, 163 coal samples were collected and desorbed from eight drill holes. Gas adsorption capacity and proximate analyses were conducted as well as macroscopic logging for coal type and vitrain banding characteristics. Vitrain bands were quantitatively point counted and the longest dimension of the shortest axis measured. Three coal types were recognized: bright luster non-banded, bright moderately banded and bright highly banded. Vitrain band thickness, converted to the phi (- log{sub 2}) scale, was found to increase across the coal types with the thickest bands being associated with the most banded coal type. Overall, when normalized by seam and location, the dataset reveals a relationship between coal type and gas content with the non-banded coal type having the highest gas contents and conversely, the coal types with the most vitrain bands having the lowest gas contents. However, when the seams are considered separately, it can be seen that in the stratigraphically higher Renown coal seam, gas has an indirect association with increasing band thickness, in agreement with the overall trend, while the stratigraphically lower Kupakupa coal seam appears to have a direct relationship. Interestingly the Renown seam, which has a greater percentage of non-banded material, generally has a greater methane adsorption capacity as well as a greater gas content compared to the Kupakupa seam. It is believed these differences are related to macroscopic texture and that the differing proportions of the coal types between the two seams has a fundamental effect on microporosity, ultimately controlling the available surface area for gas adsorption. (author)

Production of biogenic manganese oxides coupled with methane oxidation in a bioreactor for removing metals from wastewater.

Science.gov (United States)

Matsushita, Shuji; Komizo, Daisuke; Cao, Linh Thi Thuy; Aoi, Yoshiteru; Kindaichi, Tomonori; Ozaki, Noriatsu; Imachi, Hiroyuki; Ohashi, Akiyoshi

2018-03-01

Biogenic manganese oxide (BioMnO x ) can efficiently adsorb various minor metals. The production of BioMnO x in reactors to remove metals during wastewater treatment processes is a promising biotechnological method. However, it is difficult to preferentially enrich manganese-oxidizing bacteria (MnOB) to produce BioMnO x during wastewater treatment processes. A unique method of cultivating MnOB using methane-oxidizing bacteria (MOB) to produce soluble microbial products is proposed here. MnOB were successfully enriched in a methane-fed reactor containing MOB. BioMnO x production during the wastewater treatment process was confirmed. Long-term continual operation of the reactor allowed simultaneous removal of Mn(II), Co(II), and Ni(II). The Co(II)/Mn(II) and Ni(II)/Mn(II) removal ratios were 53% and 19%, respectively. The degree to which Mn(II) was removed indicated that the enriched MnOB used utilization-associated products and/or biomass-associated products. Microbial community analysis revealed that methanol-oxidizing bacteria belonging to the Hyphomicrobiaceae family played important roles in the oxidation of Mn(II) by using utilization-associated products. Methane-oxidizing bacteria were found to be inhibited by MnO 2 , but the maximum Mn(II) removal rate was 0.49 kg m -3  d -1 . Copyright © 2017 Elsevier Ltd. All rights reserved.

Conversion of methane to methanol in an ac dielectric barrier discharge

International Nuclear Information System (INIS)

Aghamir, F M; Matin, N S; Jalili, A H; Esfarayeni, M H; Khodagholi, M A; Ahmadi, R

2004-01-01

A dielectric barrier discharge (DBD) has been used to investigate the conversion of methane to methanol and higher hydrocarbons in ac non-equilibrium plasmas. Experiments were carried out at atmospheric pressure and ambient temperature. A non-equilibrium plasma was generated in a DBD reactor by applying a high voltage to the reactor electrodes. Activation of methane molecules led to the production of C 2 hydrocarbons and methanol. The effect of the applied voltage, residence time and feed mixture such as helium and oxygen on the methane conversion and product selectivity was studied. Helium appears to have no effect on the conversion and selectivity at our applied voltages. The methane conversion increases significantly on introduction of oxygen in the feed stream. Inclusion of oxygen leads to the formation of methanol. Our results show that production of methanol is initiated around an applied voltage of 12 kV and the conversion of methane increases with increasing voltage and residence time, while the product selectivity is independent of the applied voltage

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

Science.gov (United States)

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

Carbon and hydrogen isotope composition and C-14 concentration in methane from sources and from the atmosphere: Implications for a global methane budget. Final report, 1 January-30 June 1991

International Nuclear Information System (INIS)

Wahlen, M.

1994-03-01

The topics covered include the following: biogenic methane studies; forest soil methane uptake; rice field methane sources; atmospheric measurements; stratospheric samples; Antarctica; California; and Germany

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

Science.gov (United States)

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

Process for recovery of liquid hydrocarbons

Energy Technology Data Exchange (ETDEWEB)

Millar, J.F.; Cockshott, J.E.

1978-04-11

Methane is recovered as a gas for discharge to a pipeline from a gas stream containing methane and heavier hydrocarbons, principally ethane and propane. Separation is accomplished by condensing the heavier hydrocarbons and distilling the methane therefrom. A liquid product (LPG) comprising the heavier hydrocarbons is subsequently recovered and transferred to storage. Prior to being discharged to a pipeline, the recovered methane gas is compressed and in undergoing compression the gas is heated. The heat content of the gas is employed to reboil the refrigerant in an absorption refrigeration unit. The refrigeration unit is used to cool the LPG prior to its storage.

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

Science.gov (United States)

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

Analysis of petroleum hydrocarbons in soil from view of bioremediation process

International Nuclear Information System (INIS)

Mracnova, R.; Sojak, L.; Kubinec, R.; Kraus, A.; Eszenyiova, A.; Ostrovsky, I.

2002-01-01

The pollution of the environment by petroleum hydrocarbons is the most often pollution of them all. Nevertheless, hydrocarbons present in environment can be not only of petroleum or anthropogenic origin, but of biogenic as well. Typically the hydrocarbons are presented in the environment as very complex mixtures of individual compounds with very different chemical structure, wide range of the boiling points (∼800 0 C) as well as with the wide range of the number of carbon atoms. Immediately they are spread in any environmental matrix the complex physical, chemical and biochemical reactions start. A lot of methods have been developed and new are permanently in progress for the monitoring and control of petroleum hydrocarbons contamination and/or soils bioremediation. Generally, all methods by whose the hydrocarbons contaminants are determined in GC-FID system do not satisfied recommendations for enough accurate and precise results. Hyphenation of capillary gas chromatography and mass selective detector operated in the selective ion monitoring mode essentially allows detailed specification of non-polar extractable hydrocarbons. Isoprenoid alkanes, alkylhomologues of aromatic hydrocarbons and polycyclic alkanes hopanes-like were investigated as markers for recognition of petroleum and biogenic contamination. C 30 17α(H)21β(H)-hopane (C 30 -hopane) seems to be a suitable marker to identify hydrocarbons origin, to determine composting rates for nonpolar extractable compounds and to calculate real content of non-polar extractable compounds in final composting status on the assumption that the contamination is of mineral oil type. This is the survey into the results obtained in this field published in the literature as well as reached in our laboratory. (author)

Demonstration of an ethane spectrometer for methane source identification.

Science.gov (United States)

Yacovitch, Tara I; Herndon, Scott C; Roscioli, Joseph R; Floerchinger, Cody; McGovern, Ryan M; Agnese, Michael; Pétron, Gabrielle; Kofler, Jonathan; Sweeney, Colm; Karion, Anna; Conley, Stephen A; Kort, Eric A; Nähle, Lars; Fischer, Marc; Hildebrandt, Lars; Koeth, Johannes; McManus, J Barry; Nelson, David D; Zahniser, Mark S; Kolb, Charles E

2014-07-15

Methane is an important greenhouse gas and tropospheric ozone precursor. Simultaneous observation of ethane with methane can help identify specific methane source types. Aerodyne Ethane-Mini spectrometers, employing recently available mid-infrared distributed feedback tunable diode lasers (DFB-TDL), provide 1 s ethane measurements with sub-ppb precision. In this work, an Ethane-Mini spectrometer has been integrated into two mobile sampling platforms, a ground vehicle and a small airplane, and used to measure ethane/methane enhancement ratios downwind of methane sources. Methane emissions with precisely known sources are shown to have ethane/methane enhancement ratios that differ greatly depending on the source type. Large differences between biogenic and thermogenic sources are observed. Variation within thermogenic sources are detected and tabulated. Methane emitters are classified by their expected ethane content. Categories include the following: biogenic (6%), pipeline grade natural gas (30%). Regional scale observations in the Dallas/Fort Worth area of Texas show two distinct ethane/methane enhancement ratios bridged by a transitional region. These results demonstrate the usefulness of continuous and fast ethane measurements in experimental studies of methane emissions, particularly in the oil and natural gas sector.

Non-mine technology of hydrocarbon resources production at complex development of gas and coal deposits

International Nuclear Information System (INIS)

Saginov, A.S.; Adilov, K.N.; Akhmetbekov, Sh.U.

1997-01-01

Non-mine technology of coal gas seams exploitation is new geological technological method of complex exploitation of coal gas deposits. The method allows sequentially to extract hydrocarbon resources in technological aggregative-mobile condensed states. According to natural methane content in seams the technology includes: methane extraction from sorption volume where it is bounded up with coal; gas output intensification of coal is due to structural changes of substance at the cost of physico-chemical treatment of seam; increase of seam permeability by the methods of active physical and physico-chemical actions on coal seam (hydro-uncovering, pneumatic hydro action etc.). Pilot testing shows efficiency of well mastering with help of depth pumps. In this case works of action of pumping out of operating liquid and gas extraction from coal seam are integrated

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

Directory of Open Access Journals (Sweden)

J. Felden

2013-05-01

Full Text Available 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.

Influence of oil and gas emissions on ambient atmospheric non-methane hydrocarbons in residential areas of Northeastern Colorado

Directory of Open Access Journals (Sweden)

Chelsea R. Thompson

2014-11-01

Full Text Available Abstract The Northern Front Range (NFR region of Colorado has experienced rapid expansion of oil and gas extraction from shale and tight sands reservoirs in recent years due to advances in hydraulic fracturing technology, with over 25,000 wells currently in operation. This region has also been designated as a federal ozone non-attainment area by the U.S. EPA. High ozone levels are a significant health concern, as are potential health impacts from chronic exposure to primary emissions of non-methane hydrocarbons (NMHC for residents living near wells. From measurements of ambient atmospheric NMHC present in residential areas located in close proximity to wells in Erie, Colorado, we find that mean mole fractions of the C2–C5 alkanes are enhanced by a factor of 18–77 relative to the regional background, and present at higher levels than typically found in large urban centers. When combined with NMHC observations from downtown Denver and Platteville, it is apparent that these compounds are elevated across the NFR, with highest levels within the Greater Wattenberg Gas Field. This represents a large area source for ozone precursors in the NFR. The BTEX aromatic compounds in Erie were comparable to (e.g., benzene or lower than (e.g., toluene, ethylbenzene, xylene in large urban centers, however, benzene was significantly higher in Platteville, and within the range of chronic health-based exposure levels. An initial look at comparisons with data sets from previous years reveal that ambient levels for oil and gas-related NMHC in Erie, as well as further downwind in Boulder, have not decreased, but appear to have been increasing, despite tightening of emissions standards for the oil and gas industries in 2008.

Carbon and hydrogen isotopic composition of methane and C2+ alkanes in electrical spark discharge: implications for identifying sources of hydrocarbons in terrestrial and extraterrestrial settings.

Science.gov (United States)

Telling, Jon; Lacrampe-Couloume, Georges; Sherwood Lollar, Barbara

2013-05-01

The low-molecular-weight alkanes--methane, ethane, propane, and butane--are found in a wide range of terrestrial and extraterrestrial settings. The development of robust criteria for distinguishing abiogenic from biogenic alkanes is essential for current investigations of Mars' atmosphere and for future exobiology missions to other planets and moons. Here, we show that alkanes synthesized during gas-phase radical recombination reactions in electrical discharge experiments have values of δ(2)H(methane)>δ(2)H(ethane)>δ(2)H(propane), similar to those of the carbon isotopes. The distribution of hydrogen isotopes in gas-phase radical reactions is likely due to kinetic fractionations either (i) from the preferential incorporation of (1)H into longer-chain alkanes due to the more rapid rate of collisions of the smaller (1)H-containing molecules or (ii) by secondary ion effects. Similar δ(13)C(C1-C2+) and δ(2)H(C1-C2+) patterns may be expected in a range of extraterrestrial environments where gas-phase radical reactions dominate, including interstellar space, the atmosphere and liquid hydrocarbon lakes of Saturn's moon Titan, and the outer atmospheres of Jupiter, Saturn, Neptune, and Uranus. Radical recombination reactions at high temperatures and pressures may provide an explanation for the combined reversed δ(13)C(C1-C2+) and δ(2)H(C1-C2+) patterns of terrestrial alkanes documented at a number of high-temperature/pressure crustal sites.

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

Science.gov (United States)

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

14C measurements in aquifers with methane

International Nuclear Information System (INIS)

Barker, J.F.; Fritz, P.; Brown, R.M.

1978-01-01

A survey of various groundwater systems indicates that methane is a common trace constituent and occasionally a major carbon species in groundwaters. Thermocatalytic methane had delta 13 CCH 4 > -45% 0 and microbially-produced or biogenic methane had delta 13 CCH 4 0 . Groundwaters containing significant biogenic methane had abnormally heavy delta 13 C values for the inorganic carbon. Thermocatalytic methane had no apparent effect on the inorganic carbon. Because methanogenesis seriously affects the carbon isotope geochemistry of groundwaters, the correction of raw 14 C ages of affected groundwaters must consider these effects. Conceptual models are developed which adjust the 14 C activity of the groundwater for the effects of methanogenesis and for the dilution of carbon present during infiltration by simple dissolution of rock carbonate. These preliminary models are applied to groundwaters from the Alliston sand aquifer where methanogenesis has affected most samples. In this system, methanogenic bacteria using organic matter present in the aquifer matrix as substrate, have added inorganic carbon to the groundwater which has initiated further carbonate rock dissolution. These processes have diluted the inorganic carbon 14 C activity. (orig.) [de

Methane anomalies in seawaters of the Ragay Gulf, Philippines: methane cycling and contributions to atmospheric greenhouse gases

International Nuclear Information System (INIS)

Heggie, D.T.; Evans, D.; Bishop, J.H.

1999-01-01

The vertical distribution of methane has been measured in the water column of a semi-enclosed basin, the Ragay Gulf, in the Philippines archipelago. The methane distribution is characterised by unusual mid-water and bottom-water plumes, between 80 and 100 m thick. The plumes are confined to water depths between about 100 and 220 m. where the temperature-depth (a proxy for seawater density) gradient is steepest. Plumes of high methane are 'trapped' within the main thermocline; these are local features, persisting over kilometre-scale distances. Geochemical and geological evidence suggests that the elevated methane concentrations are thermogenic in origin (although an oxidised biogenic origin cannot be ruled out for some of the methane anomalies), and have migrated from the sea floor into the overlying water. The mid and bottom-water methane maxima support fluxes of methane from depth into surface waters and, subsequently, from the oceans to the atmosphere. The average supersaturation of methane in the top 5 m of the sea, at nine locations, was 206±16.5%; range 178-237%. The average estimated sea-air flux was 101 nmole.cm -2 .y -1 and probably represents a minimum flux, because of low wind speeds of <10 knots. These fluxes, we suggest, are supported by seepage from the sea floor and represent naturally occurring fluxes of mostly fossil methane (in contrast to anthropogenic fossil methane), from the sea to the atmosphere. The estimated minimum fluxes of naturally occurring fossil methane are comparable to those biogenic fluxes measured elsewhere in the surface oceans, but are less than those naturally occurring methane inputs from sediments of the Barents Sea. Ragay Gulf fluxes are also less than anthropogenic fluxes measured in areas of petroleum exploration and development, such as the Texas and Louisiana, USA shelf areas

Investigation of Methane and Soil Carbon Dynamics Using Near Surface Geophysical Methods at the Tanoma Educational Wetland Site, Tanoma, Pennsylvania

Science.gov (United States)

Seidel, A. D.; Mount, G.

2017-12-01

Studies to constrain methane budgets of Pennsylvania have sought to quantify the amount and rate of fugitive methane released during industrial natural gas development. However, contributions from other environmental systems such as artificial wetlands used to treat part of the 300 million gallons per day of acid mine drainage (AMD) are often not understated or not considered. The artificial wetlands are sources of both biogenic and thermogenic methane and are used to treat AMD which would otherwise flow untreated into Pennsylvania surface waters. Our research utilizes a combination of indirect non-invasive geophysical methods (ground penetrating radar, GPR) and the complex refractive index model, aerial imagery, and direct measurements (coring and gas traps) to estimate the contribution of biogenic methane from wetlands and legacy thermogenic methane from acid mine drainage from a flooded coal mine at an artificial wetland designed to treat these polluted waters at Tanoma, Pennsylvania. Our approach uses (3D) GPR surveys to define the thickness of the soil from the surface to the regolith-bedrock interface to create a volume model of potential biogenic gas stores. Velocity data derived from the GPR is then used to calculate the dielectric permittivity of the soil and then modeled for gas content when considering the saturation, porosity and amount of soil present. Depth-profile cores are extracted to confirm soil column interfaces and determine changes in soil carbon content. Comparisons of gas content are made with gas traps placed across the wetlands that measure the variability of gaseous methane released. In addition, methane dissolved in the waters from biogenic processes in the wetland and thermogenic processes underground are analyzed by a gas chromatograph to quantify those additions. In sum, these values can then be extrapolated to estimate carbon stocks in AMD areas such as those with similar water quality and vegetation types in the Appalachian region

SUPPLEMENTARY INFORMATION Non-oxidative methane ...

Indian Academy of Sciences (India)

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SUPPLEMENTARY INFORMATION. Non-oxidative methane dehydroaromatization reaction over highly active α-MoC1-x ZSM-5 derived from pretreatment. BUDDE PRADEEP KUMAR, ARVIND KUMAR SINGH and SREEDEVI UPADHYAYULA*. Heterogeneous Catalysis & Reaction Engineering Laboratory, Department of ...

Reaction-transport simulations of non-oxidative methane conversion with continuous hydrogen removal: Homogeneous-heterogeneous methane reaction pathways

International Nuclear Information System (INIS)

Li, Lin; Borry, Richard W.; Iglesia, Enrique

2000-01-01

Detailed kinetic-transport models were used to explore thermodynamic and kinetic barriers in the non-oxidative conversion of CH4 via homogeneous and homogeneous-heterogeneous pathways and the effects of continuous hydrogen removal and of catalytic sites on attainable yields of useful C2-C10 products. The homogeneous kinetic model combines separately developed models for low-conversion pyrolysis and for chain growth to form large aromatics and carbon. The H2 formed in the reaction decreases CH4 pyrolysis rates and equilibrium conversions and it favors the formation of lighter products. The removal of H2 along tubular reactors with permeable walls increases reaction rates and equilibrium CH4 conversions. C2-C10 yields reach values greater than 90 percent at intermediate values of dimensionless transport rates (delta=1-10), defined as the ratio hydrogen transport and methane conversion rates. Homogeneous reactions require impractical residence times, even with H2 removal, because of slow initiation and chain transfer rates. The introduction of heterogeneous chain initiation pathways using surface sites that form methyl radicals eliminates the induction period without influencing the homogeneous product distribution. Methane conversion, however, occurs predominately in the chain transfer regime, within which individual transfer steps and the formation of C2 intermediates become limited by thermodynamic constraints. Catalytic sites alone cannot overcome these constraints. Catalytic membrane reactors with continuous H2 removal remove these thermodynamic obstacles and decrease the required residence time. Reaction rates become limited by homogeneous reactions of C2 products to form C6+ aromatics. Higher delta values lead to subsequent conversion of the desired C2-C10 products to larger polynuclear aromatics. We conclude that catalytic methane pyrolysis at the low temperatures required for restricted chain growth and the elimination of thermodynamics constraints via

A 21st-century shift from fossil-fuel to biogenic methane emissions indicated by ¹³CH₄.

Science.gov (United States)

Schaefer, Hinrich; Mikaloff Fletcher, Sara E; Veidt, Cordelia; Lassey, Keith R; Brailsford, Gordon W; Bromley, Tony M; Dlugokencky, Edward J; Michel, Sylvia E; Miller, John B; Levin, Ingeborg; Lowe, Dave C; Martin, Ross J; Vaughn, Bruce H; White, James W C

2016-04-01

Between 1999 and 2006, a plateau interrupted the otherwise continuous increase of atmospheric methane concentration [CH4] since preindustrial times. Causes could be sink variability or a temporary reduction in industrial or climate-sensitive sources. We reconstructed the global history of [CH4] and its stable carbon isotopes from ice cores, archived air, and a global network of monitoring stations. A box-model analysis suggests that diminishing thermogenic emissions, probably from the fossil-fuel industry, and/or variations in the hydroxyl CH4 sink caused the [CH4] plateau. Thermogenic emissions did not resume to cause the renewed [CH4] rise after 2006, which contradicts emission inventories. Post-2006 source increases are predominantly biogenic, outside the Arctic, and arguably more consistent with agriculture than wetlands. If so, mitigating CH4 emissions must be balanced with the need for food production. Copyright © 2016, American Association for the Advancement of Science.

Geochemical assessment of light gaseous hydrocarbons in near-surface soils of Kutch-Saurashtra: Implication for hydrocarbon prospects

Science.gov (United States)

Rao, P. Lakshmi Srinivasa; Madhavi, T.; Srinu, D.; Kalpana, M. S.; Patil, D. J.; Dayal, A. M.

2013-02-01

Light hydrocarbons in soil have been used as direct indicators in geochemical hydrocarbon exploration, which remains an unconventional path in the petroleum industry. The occurrence of adsorbed soil gases, methane and heavier homologues were recorded in the near-surface soil samples collected from Kutch-Saurashtra, India. Soil gas alkanes were interpreted to be derived from deep-seated hydrocarbon sources and have migrated to the surface through structural discontinuities. The source of hydrocarbons is assessed to be thermogenic and could have been primarily derived from humic organic matter with partial contribution from sapropelic matter. Gas chromatographic analyses of hydrocarbons desorbed from soil samples through acid extraction technique showed the presence of methane through n-butane and the observed concentrations (in ppb) vary from: methane (C1) from 4-291, ethane (C2) from 0-84, propane (C3) from 0-37, i-butane (iC4) from 0-5 and n-butane (nC4) from 0-4. Carbon isotopes measured for methane and ethane by GC-C-IRMS, range between -42.9‰ to -13.3‰ (Pee Dee Belemnite - PDB) and -21.2‰ to -12.4‰ (PDB), respectively. The increased occurrence of hydrocarbons in the areas near Anjar of Kutch and the area south to Rajkot of Saurashtra signifies the area potential for oil and gas.

Radiation effects on methane in the presence of molecular sieves

International Nuclear Information System (INIS)

Shimizu, Y.; Nagai, S.; Hatada, M.

1983-01-01

Product analysis has been carried out for the radiation-induced reaction of methane in the presence of molecular sieves (MS) 3A, 4A, 5A and 13X. Irradiation of methane over MS 4A selectively produces C 2 hydrocarbons, while the use of MS 5A leads to C 2 and C 3 hydrocarbons. The selectivity and yields of these hydrocarbons, however, decrease with irradiation time, owing to deposition of carbonaceous solid produced from methane on the surface of the molecular sieves. The carbonaceous solid is decomposed to low-molecular-weight hydrocarbons when irradiated in an H 2 atmosphere. Material balance estimated for the radiation-chemical reaction of argon containing 2 mol% methane over MS 5A reveals that the carbonaceous solid is highly abundant in carbon atoms. On the other hand the formation of carbonaceous solids plays a less important role in the radiation-chemical reaction of methane in the presence of silica gel, which is found to exhibit greater activity for the formation of hydrocarbons than the molecular sieves. (author)

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

Directory of Open Access Journals (Sweden)

C. Liu

2017-09-01

Full Text Available 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

Long-lasting Microbial Methane Release at the Aquitaine Shelf Break (Bay of Biscay): Relation with the (Plio)-Pleistocene Sedimentary Progradation of the Continental Margin

Science.gov (United States)

Dupré, S.; Michel, G.; Pierre, C.; Ruffine, L.; Scalabrin, C.; Ehrhold, A.; Loubrieu, B.; Gautier, E.; Baltzer, A.; Imbert, P.; Battani, A.; Deville, E.; Dupont, P.; Thomas, Y.; Théréau, E.

2017-12-01

The recent identification of acoustic and visual gas release in the water column at the Aquitaine Shelf (140 and 220 m water depths) led to the discovery of a 200 km2 fluid system at the seafloor with 3000 bubbling sites associated with microbial methane (Dupré et al 2014; Ruffine et al. 2017). The moderate methane fluxes (measured in situ, on average 200 mLn/min per bubbling site) contribute to the formation of small-scale sub-circular authigenic carbonate mounds (with reliefs < 1 m in height) (Pierre et al. 2017). The emitted gases have neither a genetic link with thermogenic hydrocarbons from the Parentis Basin beneath, nor are issued from gas hydrate dissociation, but originate from microbial CO2 reduction. Based on estimated thickness and growth rate of authigenic carbonates, this system has lasted for at least several tens to possibly hundreds of kyears with a volume of escaping methane reaching 3.1012 Ln per 10 kyr. Seismic evidences for gas-charged layers and fossil authigenic carbonates point to organic matter source levels within the sedimentary deposits of the Late Pleistocene progradation system. The Aquitaine Shelf fluid system highlights the edge of continental shelves as preferential areas for bio-geological processes. The GAZCOGNE project is co-funded by TOTAL and IFREMER as part of the PAMELA (Passive Margin Exploration Laboratories) scientific project. References Dupré S, Berger L, Le Bouffant N, Scalabrin C, Bourillet J-F (2014) Fluid emissions at the Aquitaine Shelf (Bay of Biscay, France): a biogenic origin or the expression of hydrocarbon leakage? Cont. Shelf Res. 88:24-33 Pierre C, Demange J, Blanc-Valleron M-M, Dupré S (2017) Authigenic carbonate mounds from active methane seeps on the southern Aquitaine Shelf (Bay of Biscay, France): Evidence for anaerobic oxidation of biogenic methane and submarine groundwater discharge during formation. Cont. Shelf Res. 133:13-25 Ruffine L, Donval J-P, Croguennec C, Bignon L, Birot D, Battani A, Bayon

On morphology of methane-derived authigenic carbonates

Science.gov (United States)

Logvina, E.; Matveeva, T.

2009-04-01

Studies of methane-derived carbonates revealed a great variety their morphological types. Although the processes of these carbonates formation is not clearly understood, it has been suggested that in general bacterially mediated processes of hydrocarbon oxidation, coupled with sulphate reduction, produce unusually high levels of alkalinity and dissolved inorganic carbon in the pore fluids that is partitioned between the precipitating carbonate and CO2 rich plumes which emanate into the water column (Aharon, 1994). These carbonates consist by three main CaCO3 polymorphs - calcite, aragonite and dolomite. Carbonates with different petrography cemented from these polymorphs can be classified according to their specific locality mode of formation and biogenic or non-biogenic origin (Greinert et al., 2002). There are classifications for the authigenic carbonates which are based on petrography, morphology, or based on age and origin. In this work we will consider the petrographical and morphological differences of authigenic carbonates. The large structures vary from 10 to 200 m size, named as chemoherm carbonates. Usually they cemented by pure aragonite with minor Mg-calcite admixture. These chemoherms rise up to 50 m above the seafloor. The structures are irregular in shape and have numerous pores and open pathways resulting from plumbing system of fluid expulsion. This type of authigenic carbonates was observed in the NE Black Sea (Michaelis et al., 2002), at the Hydrate Ridge area (Greinert et al., 2001), at Aleutian accretionary margin (Greinert et al., 2002). Diagenetic carbonates - carbonate cemented sediments both growing at the seafloor or within the sediment framework and showing a large variety of shapes (chimneys, crusts, concretions est.), with grey to dark-grey color. Petrographically the carbonate cement represents by Mg-calcite, protodolomite and dolomite. The diagenetic carbonates occur widely in the fluid venting areas. In particular, diagenetic

Catalytic generation of methane at 60-100 °C and 0.1-300 MPa from source rocks containing kerogen Types I, II, and III

Science.gov (United States)

Wei, Lin; Schimmelmann, Arndt; Mastalerz, Maria; Lahann, Richard W.; Sauer, Peter E.; Drobniak, Agnieszka; Strąpoć, Dariusz; Mango, Frank D.

2018-06-01

Low temperature (60 and 100 °C) and long-term (6 months to 5 years) heating of pre-evacuated and sterilized shales and coals containing kerogen Types I (Mahogany Shale), II (Mowry Shale and New Albany Shale), and III (Springfield Coal and Wilcox Lignite) with low initial maturities (vitrinite reflectance Ro 0.39-0.62%) demonstrates that catalytically generated hydrocarbons may explain the occurrence of some non-biogenic natural gas accumulations where insufficient thermal maturity contradicts the conventional thermal cracking paradigm. Extrapolation of the observed rate of catalytic methanogenesis in the laboratory suggests that significant amounts of sedimentary organic carbon can be converted to relatively dry natural gas over tens of thousands of years in sedimentary basins at temperatures as low as 60 °C. Our laboratory experiments utilized source rock (shale and coal) chips sealed in gold and Pyrex® glass tubes in the presence of hydrogen-isotopically contrasting waters. Parallel heating experiments applied hydrostatic pressures from 0.1 to 300 MPa. Control experiments constrained the influence of pre-existing and residual methane in closed pores of rock chips that was unrelated to newly generated methane. This study's experimental methane yields at 60 and 100 °C are 5-11 orders of magnitude higher than the theoretically predicted yields from kinetic models of thermogenic methane generation, which strongly suggests a contribution of catalytic methanogenesis. Higher temperature, longer heating time, and lower hydrostatic pressure enhanced catalytic methanogenesis. No clear relationships were observed between kerogen type or total organic carbon content and methane yields via catalysis. Catalytic methanogenesis was strongest in Mowry Shale where methane yields at 60 °C amounted to ∼2.5 μmol per gram of organic carbon after one year of hydrous heating at ambient pressure. In stark contrast to the earlier findings of hydrogen isotopic exchange between

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

Science.gov (United States)

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...

Operation of Marine Diesel Engines on Biogenic Fuels: Modification of Emissions and Resulting Climate Effects

OpenAIRE

Petzold, A.; Lauer, P.; Fritsche, U.; Hasselbach, J.; Lichtenstern, M.; Schlager, H.; Fleischer, F.

2011-01-01

The modification of emissions of climate-sensitive exhaust compounds such as CO2, NOx, hydrocarbons, and particulate matter from medium-speed marine diesel engines was studied for a set of fossil and biogenic fuels. Applied fossil fuels were the reference heavy fuel oil (HFO) and the low-sulfur marine gas oil (MGO); biogenic fuels were palm oil, soybean oil, sunflower oil, and animal fat. Greenhouse gas (GHG) emissions related to the production of biogenic fuels were treated by means of a fue...

The Extent of CH4 Emission and Oxidation in Thermogenic and Biogenic Gas Hydrate Environments

Science.gov (United States)

Kastner, M.; Solem, C.; Bartlett, D.; MacDonald, I.; Valentine, D.

2003-12-01

The role of methane hydrate in the global methane budget is poorly understood, because relatively little is known about the transport of gaseous and dissolved methane through the seafloor into the ocean, from the water column into the atmosphere, and the extent of water-column methanotrophy that occurs en route. We characterize the transport and consumption of methane in three distinct gas hydrate environments, spanning the spectrum of thermogenic and biogenic methane occurrences: Bush Hill in the Gulf of Mexico, Eel River off the coast of Northern California, and the Noth and South Hydrate Ridges on the Cascadia Oregon margin. At all the sites studied a significant enrichment in δ 13CH4 with distance along isopycnals away from the methane source is observed, indicative of extensive aerobic bacterial methane oxidation in the water column. The effects of this process are principally pronounced in the mostly biogenic methane setting, with δ 13C-CH4 measured as high as -12 permil (PDB) between North and South Hydrate Ridge. The δ 13C-CH4 values ranged from -12 to -67 permil at Hydrate Ridge, -34 to -52 permil at Eel River, and -41 to -49 permil at Bush Hill. The large variation in methane carbon isotope ranges between the sites suggest that major differences exist in both the rates of aerobic methane oxidation and system openness at the studied locations. A mean kinetic isotope fractionation factor is being determined using a closed-system Rayleigh distillation model. An approximate regional methane flux from the ocean into the atmosphere is being estimated for the Gulf of Mexico, by extrapolation of the flux value from the Bush Hill methane plume over 390 plume locations having persistent oil slicks on the ocean surface, mapped by time series satellite data.

Estimating methane gas production in peat soils of the Florida Everglades using hydrogeophysical methods

Science.gov (United States)

Wright, William; Comas, Xavier

2016-04-01

The spatial and temporal variability in production and release of greenhouse gases (such as methane) in peat soils remains uncertain, particularly for low-latitude peatlands like the Everglades. Ground penetrating radar (GPR) is a hydrogeophysical tool that has been successfully used in the last decade to noninvasively investigate carbon dynamics in peat soils; however, application in subtropical systems is almost non-existent. This study is based on four field sites in the Florida Everglades, where changes in gas content within the soil are monitored using time-lapse GPR measurements and gas releases are monitored using gas traps. A weekly methane gas production rate is estimated using a mass balance approach, considering gas content estimated from GPR, gas release from gas traps and incorporating rates of diffusion, and methanotrophic consumption from previous studies. Resulting production rates range between 0.02 and 0.47 g CH4 m-2 d-1, falling within the range reported in literature. This study shows the potential of combining GPR with gas traps to monitor gas dynamics in peat soils of the Everglades and estimate methane gas production. We also show the enhanced ability of certain peat soils to store gas when compared to others, suggesting that physical properties control biogenic gas storage in the Everglades peat soils. Better understanding biogenic methane gas dynamics in peat soils has implications regarding the role of wetlands in the global carbon cycle, particularly under a climate change scenario.

Selective coke combustion by oxygen pulsing during Mo/ZSM‐5‐catalyzed methane dehydroaromatization

NARCIS (Netherlands)

Kosinov, N.; Coumans, F.J.A.G.; Uslamin, E.A.; Kapteijn, F.; Hensen, E.J.M.

2016-01-01

Non-oxidative methane dehydroaromatization is a promising reaction to directly convert natural gas into aromatic hydrocarbons and hydrogen. Commercialization of this technology is hampered by rapid catalyst deactivation because of coking. A novel approach is presented involving selective oxidation

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

Science.gov (United States)

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.

Direct Aromaization of Methane

Energy Technology Data Exchange (ETDEWEB)

George Marcelin

1997-01-15

The thermal decomposition of methane offers significant potential as a means of producing higher unsaturated and aromatic hydrocarbons when the extent of reaction is limited. Work in the literature previous to this project had shown that cooling the product and reacting gases as the reaction proceeds would significantly reduce or eliminate the formation of solid carbon or heavier (Clo+) materials. This project studied the effect and optimization of the quenching process as a means of increasing the amount of value added products during the pyrolysis of methane. A reactor was designed to rapidly quench the free-radical combustion reaction so as to maximize the yield of aromatics. The use of free-radical generators and catalysts were studied as a means of lowering the reaction temperature. A lower reaction temperature would have the benefits of more rapid quenching as well as a more feasible commercial process due to savings realized in energy and material of construction costs. It was the goal of the project to identify promising routes from methane to higher hydrocarbons based on the pyrolysis of methane.

In search of thermogenic methane in groundwater in the Netherlands, with emphasis on the location of a historic gas well blowout

Science.gov (United States)

Schout, G.; Griffioen, J.; Hassanizadeh, S. M.; Hartog, N.

2017-12-01

Similar to the US, the Netherlands has a long history of oil & gas production, with around 2500 onshore hydrocarbon wells drilled since the late 1930s. While conventional reserves are diminishing, a governmental moratorium was put in place on shale gas exploration and production until 2023, in part due to concerns about its effects on groundwater quality. To investigate the industry's historic and potential future impact on groundwater quality in the country, a study was carried out to assess i) baseline methane concentrations and origin ii) the natural connectivity of deeper gas-bearing layers with the shallower groundwater systems. Through datamining, a dataset consisting of 12,200 groundwater analyses with methane concentrations was assembled. Furthermore, 25 additional samples were collected at targeted locations and analysed for dissolved gas molecular and isotopic composition. Methane concentrations are positively skewed with median, mean and maximum concentrations of 0.28, 2.17 and 120 mg/L, respectively. No correlation between methane concentrations and distance to hydrocarbon wells or faults is observed. In general, concentrations cannot be readily explained by factors such as the depth, geographic location, host formation and depositional environment. Thermogenic methane was first encountered at several hundred meters depth, below thick successions of marine Paleogene and Neogene clays that are present throughout the country and impede vertical flow. All methane encountered above these formations was found to be biogenic in origin, with one notable exception - a sample taken at the site of a catastrophic gas well blowout that occurred in 1965 near the village of Sleen. Combined, these findings suggest that thermogenic methane does not naturally occur in Dutch shallow groundwater and its presence can be used as an indicator of anthropogenic gas leakage. The unique Sleen blowout site was selected for a detailed investigation of the long-term effects of

Distribution and origin of hydrocarbons in water and sediment in Sao Sebastiao, SP, Brazil

International Nuclear Information System (INIS)

Zanardi, Eliete; Bicego, Marcia Caruso; Miranda, Luiz Bruner de; Weber, Rolf Roland

1999-01-01

This study describes the dissolved/dispersed petroleum hydrocarbons (DDPH) in surface water and the origin and distribution of aliphatic and aromatic hydrocarbons in samples from the surface bottom sediments. The main objective was to verify the anthropogenic contribution on the adjacent inner shelf of Sao Sebastiao, taking into account the distribution of hydrographic properties and knowledge of the main circulation. The DDPH concentration range of the 20 samples were from 0.35 to 2.50 m u g . L -1 , characterising this region as slightly affected by the contribution of petroleum hydrocarbons. Considering sediment hydrocarbon results, sites located in the inner shelf were divided into three groups: one with mainly biogenic hydrocarbons, a second one with biogenic and petroleum hydrocarbons and a third with significant contribution of petroleum hydrocarbons. These results show an influence of human activities in the Sao Sebastiao Channel on the surrounding areas of the inner shelf. (Author)

Development of a System for the Analysis of Hydrocarbons Different to the Methane in Air

International Nuclear Information System (INIS)

Rodriguez Harrison, F. A.

2001-01-01

In the air there are more than 3000 organic compounds produced by the natural emissions and anthropoid-genetics. Many of these organic compounds are saturated and unsaturated hydrocarbons; the volcanoes and the plants emit some, while others are emitted for the industrial processes and for the mobile sources. The hydrocarbons play a very important role in the Atmospheric Chemistry, since they take place through their oxidation a series of substances that affect the living beings, they sensitize the human being, producing him illnesses and they contribute to alter the climate of the planet. A sampling method by adsorption about cartridges that contained Tenax, Carbopack B, and molecular sieve, and a system for the analysis of hydrocarbons in the air for thermal desertion and cryogenic concentration was developed with the purpose of identifying and quantifying the hydrocarbons different to the methane present in the winds that travel San Jose Central Valley, Costa Rica. The effect of the ozone in these determinations was studied by taking samples with destroyer of ozone made with iodize of potassium and comparing them with samples taken without the destroyer. The samples were taken simultaneously between April 20 and 29 1999 in 3 sampling stations located in the northwest side of the Volcano Irazu, in Escazu and in Turrucares. There were eleven hydrocarbons being among the most abundant anthropoid-genetics the isooctane (among 34 y 149 μg/m 3 ) and etilbenceno while (among 13 y 231 μg/m 3 ), while the one α-pineno (among 25 y 153 μg/m 3 ), β-pineno (among 60 y 192 μg/m 3 ) y el limoneno (among 34 y 244 μg/m 3 ). It was also found that the ozone didn't affect the concentrations of the unsaturated hydrocarbons in the cartridges, since there were not significant differences in the concentrations of the measured hydrocarbons when the destroyer of ozone was used. (Author) [es

Methane as a climate gas

Energy Technology Data Exchange (ETDEWEB)

Karlsdottir, S.

1996-03-01

This paper was read at the workshop ``The Norwegian Climate and Ozone Research Programme`` held on 11-12 March 1996. Methane is a key component in the atmosphere where its concentration has increased rapidly since pre-industrial time. About 2/3 of it is caused by human activities. Changes in methane will affect the concentrations of other gases, and a model is a very important tool to study sensitivity due to changes in concentration of gases. The author used a three-dimensional global chemistry transport model to study the effect of changes in methane concentration on other trace gases. The model includes natural and anthropogenic emissions of NOx, CO, CH{sub 4} and non-methane hydrocarbons. Wet and dry deposition are also included. The chemical scheme in the model includes 49 compounds, 101 reactions, and 16 photolytic reactions. The trace gas concentrations are calculated every 30 min, using a quasi steady state approximation. Model calculations of three cases are reported and compared. Enhanced methane concentration will have strongest effect in remote regions. In polluted areas local chemistry will have remarked effect. The feedback was always positive. Average atmospheric lifetime calculated in the model was 7.6 years, which agrees with recent estimates based on observations. 8 refs.

Stimulation by ammonium-based fertilizers of methane oxidation in soil around rice roots

NARCIS (Netherlands)

Bodelier, P.L.E.; Roslev, P.; Henckel, T.; Frenzel, P.

2000-01-01

Methane is involved in a number of chemical and physical processes in the Earths atmosphere, including global warming(1), Atmospheric methane originates mainly from biogenic sources, such as rice paddies and natural wetlands; the former account for at least 30% of the global annual emission of

Distribution and origin of hydrocarbons in water and sediment in Sao Sebastiao, SP, Brazil

Energy Technology Data Exchange (ETDEWEB)

Zanardi, Eliete [Universidade de Sao Paulo, Instituto Oceanografico, Sao Paulo, SP (Brazil); Bicego, Marcia Caruso; Miranda, Luiz Bruner de; Weber, Rolf Roland [Miami Univ., RSMAS/NAC, Miami, FL (United States)

1999-04-01

This study describes the dissolved/dispersed petroleum hydrocarbons (DDPH) in surface water and the origin and distribution of aliphatic and aromatic hydrocarbons in samples from the surface bottom sediments. The main objective was to verify the anthropogenic contribution on the adjacent inner shelf of Sao Sebastiao, taking into account the distribution of hydrographic properties and knowledge of the main circulation. The DDPH concentration range of the 20 samples were from 0.35 to 2.50 {sup m}u{sup g}. L{sup -1}, characterising this region as slightly affected by the contribution of petroleum hydrocarbons. Considering sediment hydrocarbon results, sites located in the inner shelf were divided into three groups: one with mainly biogenic hydrocarbons, a second one with biogenic and petroleum hydrocarbons and a third with significant contribution of petroleum hydrocarbons. These results show an influence of human activities in the Sao Sebastiao Channel on the surrounding areas of the inner shelf. (Author)

Plasma devices for hydrocarbon reformation

KAUST Repository

Cha, Min Suk

2017-02-16

Plasma devices for hydrocarbon reformation are provided. Methods of using the devices for hydrocarbon reformation are also provided. The devices can include a liquid container to receive a hydrocarbon source, and a plasma torch configured to be submerged in the liquid. The plasma plume from the plasma torch can cause reformation of the hydrocarbon. The device can use a variety of plasma torches that can be arranged in a variety of positions in the liquid container. The devices can be used for the reformation of gaseous hydrocarbons and/or liquid hydrocarbons. The reformation can produce methane, lower hydrocarbons, higher hydrocarbons, hydrogen gas, water, carbon dioxide, carbon monoxide, or a combination thereof.

Fugitive Methane Emission Identification and Source Attribution: Ethane-to-Methane Analysis Using a Portable Cavity Ring-Down Spectroscopy Analyzer

Science.gov (United States)

Kim-Hak, D.; Fleck, D.

2017-12-01

Natural gas analysis and methane specifically have become increasingly important by virtue of methane's 28-36x greenhouse warming potential compared to CO2 and accounting for 10% of total greenhouse gas emissions in the US alone. Additionally, large uncontrolled leaks, such as the recent one from Aliso Canyon in Southern California, originating from uncapped wells, storage facilities and coal mines have increased the total global contribution of methane missions even further. Determining the specific fingerprint of methane sources by quantifying the ethane to methane (C2:C1) ratios provides us with means to understand processes yielding methane and allows for sources of methane to be mapped and classified through these processes; i.e. biogenic or thermogenic, oil vs. gas vs. coal gas-related. Here we present data obtained using a portable cavity ring-down spectrometry analyzer weighing less than 25 lbs and consuming less than 35W that simultaneously measures methane and ethane in real-time with a raw 1-σ precision of plane gas propagation.

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

Science.gov (United States)

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

Directory of Open Access Journals (Sweden)

T. Salameh

2016-03-01

Full Text Available 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.

Developmental geology of coalbed methane from shallow to deep in Rocky Mountain basins and in Cook Inlet-Matanuska Basin, Alaska, USA and Canada

Science.gov (United States)

Johnson, R.C.; Flores, R.M.

1998-01-01

from hydrocarbon generation as they form, and this overpressuring is probably responsible for driving out most of the water. Sandstone permeabilities are low, in part because of diagenesis caused by highly reactive water given off during the early stages of coalification. Coals within these basin-centered deposits commonly have high gas contents and produce little water, but they generally occur at depths greater than 5000 ft and have low permeabilities. Significant uplift and removal of overburden has occurred throughout the Rocky Mountain region since the end of the Eocene, and much of this erosion occurred after regional uplift began about 10 Ma. The removal of overburden generally causes methane saturation levels in coals to decrease, and thus a significant drop in pressure is required to initiate methane production. The most successful coalbed methane production in the Rocky Mountain region occurs in areas where gas contents were increased by post-Eocene thermal events and/or the generation of late-stage biogenic gas. Methane-generating bacteria were apparently reintroduced into the coals in some areas after uplift and erosion, and subsequent changes in pressure and temperature, allowed surface waters to rewater the coals. Groundwater may also help open up cleat systems making coals more permeable to methane. If water production is excessive, however, the economics of producing methane are impacted by the cost of water disposal.The Rocky Mountain basins of western North America contain vast deposits of coal of Cretaceous through early Tertiary age. Coalbed methane is produced in Rocky Mountain basins at depths ranging from 45 to 1981 m from coal of lignite to low volatile bituminous rank. Despite more than two decades of exploration for coalbed methane in Rocky Mountain region, it is still difficult to predict production characteristics of coalbed methane wells prior to drilling. Sources of coalbed gases can be early biogenic, formed during the main stages of coa

Ground truthing for methane hotspots at Railroad Valley, NV - application to Mars

Science.gov (United States)

Detweiler, A. M.; Kelley, C. A.; Bebout, B.; McKay, C. P.; DeMarines, J.; Yates, E. L.; Iraci, L. T.

2011-12-01

During the 2010 Greenhouse gas Observing SATellite (GOSAT) calibration and validation campaign at Railroad Valley (RRV) playa, NV, unexpected methane and carbon dioxide fluctuations were observed at the dry lakebed. Possible sources included the presence of natural gas (thermogenic methane) from oil deposits in the surrounding playa, and/or methane production from microbial activity (biogenic) in the subsurface of the playa. In the summer of 2011, measurements were undertaken to identify potential methane sources at RRV. The biogenicity of the methane was determined based on δ13C values and methane/ethane ratios. Soil gas samples and sediments were collected at different sites in the playa and surrounding areas. The soils of the playa consist of a surface crust layer (upper ~ 10 cm) grading to a dense clay below about 25 cm. Soil gas from the playa, sampled at about 20 and 80 cm depths, reflected atmospheric methane concentrations, ranging from 2 to 2.4 ppm, suggesting that no methane was produced within the playa. Natural springs on the northeast and western border of the playa, detected as methane hotspots from a flyover by the Sensor Integrated Environmental Remote Research Aircraft (SIERRA), were also sampled. Bubbles in these springs had methane concentrations that ranged from 69 to 84% by volume. In addition, ethane was detected at very low concentrations, giving methane/ethane ratios in excess of 100,000, indicating biogenic methane in the springs. Soils and sediments collected at the playa and spring sites were incubated in vials over a period of ~23 days. Methane production was observed in the spring sites (avg. 228.6 ± 49.1 nmol/g/d at Kate Springs), but was not evident for the playa sites. The incubation data, therefore, corroborated in situ methane concentration measurements. Particulate organic carbon (POC) was low for all sites samples (0.05-0.38%), with the exception of Kate Springs, which had a much higher POC concentration of 3.4 ± 0

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

Science.gov (United States)

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.

Opportunities for development of non-traditional hydrocarbon resources in the Timan-North Ural region, taking into account ecosystem services

Directory of Open Access Journals (Sweden)

I. G. Burtseva

2017-12-01

Full Text Available The authors formulate the definition of non-traditional resources from geological-genetic, technological and economic viewpoints. The authors present a detailed assessment of the resource potential of non-traditional hydrocarbon raw material in the Timan-Severouralsk region, including hydrocarbons in the deposits of the domanic type, methane of coal seams, liquid and gaseous hydrocarbons potentially extracted from black, brown coal and combustible shales. The authors also show the main directions of industrial use of coal and oil shales. The assessment of the resource potential of hydrocarbon raw materials in the deposits of the domanic type varies widely; the recoverable resources may amount to about 1 billion tons. Bituminous coals with a high volatile yield have the highest degree of conversion to liquid hydrocarbons, and brown and black coals of with a low degree of metamorphism usually serve for the production of combustible gas and primary resin. The paper describes the option of developing oil shale deposits as a possible investment project. The determined components and overall values of the economic effect from the implementation of the projects under consideration allow us to estimate that the payback period of investments does not exceed seven years. There is also a social effect: the creation of an additional 550 jobs in the operation of the quarry and about 700 jobs – in the enrichment and processing of oil shales. The estimated annual volume of output is 25–30 billion rubles, and the volume of tax revenues – up to 100 billion rubles. The authors evaluated ecosystem services in the territories of potential industrial development of coal and oil shale deposits; identified the beneficiaries of the benefits from the use of environmental services and the possibility of calculating payments.

Mitigation and recovery of methane emissions from tropical hydroelectric dams

Energy Technology Data Exchange (ETDEWEB)

Bambace, L.A.W.; Ramos, F.M.; Lima, I.B.T.; Rosa, R.R. [Instituto Nacional de Pesquisas Espaciais (INPE), Sao Jose dos Campos (Brazil)

2007-06-15

Tropical hydroelectric reservoirs generally constitute an appreciable source of methane to the atmosphere. This paper proposes simple mitigation and recovery procedures to substantially reduce atmospheric methane emissions from hydroelectric reservoirs. We aim at transforming existing methane stocks of tropical reservoirs into a clean, renewable energy source. The recovered gas methane may be pumped to large consuming centers, stocked locally and burned in gas turbines to generate electricity during high demand periods, or even purified for transport applications. Our simulations show that the use of biogenic methane may increase considerably the energy supply in countries like Brazil. As a result, it would be possible to reduce the need of additional hydroelectric dams, protecting important pristine biomes, and avoiding the resettlement of villages and indigenous reserves. (author)

Methane production, recovery and emission from two Danish landfills

DEFF Research Database (Denmark)

Fathi Aghdam, Ehsan

(TC), total organic carbon (TOC) and biogenic carbon (BioC). SW samples were incubated to measure their first-order decay kinetic constant (k-value), under different operating conditions (temperature and moisture), and their biochemical methane potential (BMP). In addition, four main metals present...

PC-BEIS: a personal computer version of the biogenic emissions inventory system

International Nuclear Information System (INIS)

Pierce, T.E.; Waldruff, P.S.

1991-01-01

The US Environmental Protection Agency's Biogenic Emissions Inventory System (BEIS) has been adapted for use on IBM-compatible personal computers (PCs). PC-BEIS estimates hourly emissions of isoprene, α-pinene, other monoterpenes, and unidentified hydrocarbons for any county in the contiguous United States. To run the program, users must provide hourly data on ambient temperature, relative humidity, wind speed, cloud cover, and a code that identifies the particular county. This paper provides an overview of the method used to calculate biogenic emissions, shows an example application, and gives information on how to obtain a copy of the program

High-temperature removal of sulphur for biogenic gas products; Hochtemperatur-Entschwefelung fuer biogene Produktgase. Design und Optimierung - Schlussbericht/Jahresbericht

Energy Technology Data Exchange (ETDEWEB)

Schildhauer, T.; Biollaz, S.

2009-12-15

This final report for the Swiss Federal Office of Energy (SFOE) presents the results of a project concerning the development of basics ideas on the design and optimisation of high-temperature methods for the removal of sulphur from biogenic gas products. Tests made as part of the 'Methane from Wood' project at pilot installations in Switzerland and Austria are discussed. Low temperature and high-temperature methods are examined and discussed. A number of sulphur compounds were tested. Also, experiments made using nickel, HDS and CPO catalysers are discussed.

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

Science.gov (United States)

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

Science.gov (United States)

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

Emission of Methane and Heavier Alkanes From the La Brea Tar Pits Seepage Area, Los Angeles

Science.gov (United States)

Etiope, G.; Doezema, L. A.; Pacheco, C.

2017-11-01

Natural hydrocarbon (oil and gas) seeps are widespread in Los Angeles, California, due to gas migration, along faults, from numerous subsurface petroleum fields. These seeps may represent important natural contributors of methane (CH4) and heavier alkanes (C2-C4) to the atmosphere, in addition to anthropogenic fossil fuel and biogenic sources. We measured the CH4 flux by closed-chamber method from the La Brea Tar Pits park (0.1 km2), one of the largest seepage sites in Los Angeles. The gas seepage occurs throughout the park, not only from visible oil-asphalt seeps but also diffusely from the soil, affecting grass physiology. About 500 kg CH4 d-1 is emitted from the park, especially along a belt of enhanced degassing that corresponds to the 6th Street Fault. Additional emissions are from bubble plumes in the lake within the park (order of 102-103 kg d-1) and at the intersection of Wilshire Boulevard and Curson Avenue (>130 kg d-1), along the same fault. The investigated area has the highest natural gas flux measured thus far for any onshore seepage zone in the USA. Gas migration, oil biodegradation, and secondary methanogenesis altered the molecular composition of the original gas accumulated in the Salt Lake Oil Field (>300 m deep), leading to high C1/C2+ and i-butane/n-butane ratios. These molecular alterations can be important tracers of natural seepage and should be considered in the atmospheric modeling of the relative contribution of fossil fuel (anthropogenic fugitive emission and natural geologic sources) versus biogenic sources of methane, on local and global scales.

Smog chamber studies on the air chemistry of biogenic hydrocarbons in the presence of ozone, NOx and SO2

International Nuclear Information System (INIS)

Nolting, F.; Zetzsch, C.

1990-01-01

The influence of SO 2 on the photochemical degradation processes of the biogenic hydrocarbon α-pinene was studied with respect to the present forest decline. For that purpose premixed air was irradiated with simulated sunlight in laboratory experiments using a modified smog chamber. The performance of a novel semi continuous analyzer for H 2 SO 4 /sulfate was tested for smog chamber studies of the transformation of SO 2 to sulfuric acid and sulfur containing aerosol. An influence of SO 2 on the formation of ozone was not detected. The rates of degradation cannot be described by gas phase reactions alone, and, in addition, they are faster in the presence of humidity. Depending on humidity, 30-50% of the consumed SO 2 can be recovered in the suspended aerosol. In the presence of 60% relative humidity the nearly exclusive product is sulfur aerosol that needs further characterization. (orig.) With 9 figs., 42 refs [de

Strong geologic methane emissions from discontinuous terrestrial permafrost in the Mackenzie Delta, Canada.

Science.gov (United States)

Kohnert, Katrin; Serafimovich, Andrei; Metzger, Stefan; Hartmann, Jörg; Sachs, Torsten

2017-07-19

Arctic permafrost caps vast amounts of old, geologic methane (CH 4 ) in subsurface reservoirs. Thawing permafrost opens pathways for this CH 4 to migrate to the surface. However, the occurrence of geologic emissions and their contribution to the CH 4 budget in addition to recent, biogenic CH 4 is uncertain. Here we present a high-resolution (100 m × 100 m) regional (10,000 km²) CH 4 flux map of the Mackenzie Delta, Canada, based on airborne CH 4 flux data from July 2012 and 2013. We identify strong, likely geologic emissions solely where the permafrost is discontinuous. These peaks are 13 times larger than typical biogenic emissions. Whereas microbial CH 4 production largely depends on recent air and soil temperature, geologic CH 4 was produced over millions of years and can be released year-round provided open pathways exist. Therefore, even though they only occur on about 1% of the area, geologic hotspots contribute 17% to the annual CH 4 emission estimate of our study area. We suggest that this share may increase if ongoing permafrost thaw opens new pathways. We conclude that, due to permafrost thaw, hydrocarbon-rich areas, prevalent in the Arctic, may see increased emission of geologic CH 4 in the future, in addition to enhanced microbial CH 4 production.

Characterization of the vadose zone above a shallow aquifer contaminated with gas condensate hydrocarbons

International Nuclear Information System (INIS)

Sublette, K.; Duncan, K.; Thoma, G.; Todd, T.

2002-01-01

A gas production site in the Denver Basin near Ft. Lupton, Colorado has leaked gas condensate hydrocarbons from an underground concrete tank used to store produced water. The leak has contaminated a shallow aquifer. Although the source of pollution has been removed, a plume of hydrocarbon contamination still remains for nearly 46 m from the original source. An extensive monitoring program was conducted in 1993 of the groundwater and saturated sediments. The objective was to determine if intrinsic aerobic or anaerobic bioremediation of hydrocarbons occurred at the site at a rate that would support remediation. Geochemical indicators of hydrogen biodegradation by microorganisms in the saturated zone included oxygen depletion, increased alkalinity, sulfate depletion, methane production and Fe2+ production associated with hydrogen contamination. The presence of sulfate-reducing bacteria and methanogens was also much higher in the contaminated sediments. Degraded hydrocarbon metabolites were found in contaminated groundwater. An extensive characterization of the vadose zone was conducted in which the vadose zone was sample in increments of 15 cm from the surface to the water table at contaminated and non contaminated sites. The samples were tested for individual C3+ hydrocarbons, methane, CO2, total organic carbon, total inorganic carbon, and total petroleum hydrocarbons. The vadose zone consisted of an active and aerobic bioreactor fueled by condensate hydrocarbons transported into the unsaturated zone by evaporation of hydrocarbons at the water table. It was concluded that the unsaturated zone makes an important contribution to the natural attenuation of gas condensate hydrocarbons in the area. 17 refs., 2 tabs., 28 figs

Investigations of Methane Production in Hypersaline Environments

Science.gov (United States)

Bebout, Brad M.

2015-01-01

The recent reports of methane in the atmosphere of Mars, as well as the findings of hypersaline paleo-environments on that planet, have underscored the need to evaluate the importance of biological (as opposed to geological) trace gas production and consumption. Methane in the atmosphere of Mars may be an indication of life but might also be a consequence of geologic activity and/or the thermal alteration of ancient organic matter. Hypersaline environments have now been reported to be extremely likely in several locations in our solar system, including: Mars, Europa, and Enceladus. Modern hypersaline microbial mat communities, (thought to be analogous to those present on the early Earth at a period of time when Mars was experiencing very similar environmental conditions), have been shown to produce methane. However, very little is known about the physical and/or biological controls imposed upon the rates at which methane, and other important trace gases, are produced and consumed in these environments. We describe here the results of our investigations of methane production in hypersaline environments, including field sites in Chile, Baja California Mexico, California, USA and the United Arab Emirates. We have measured high concentrations of methane in bubbles of gas produced both in the sediments underlying microbial mats, as well as in areas not colonized by microbial mats in the Guerrero Negro hypersaline ecosystem, Baja California Mexico, in Chile, and in salt ponds on the San Francisco Bay. The carbon isotopic (d13C) composition of the methane in the bubbles exhibited an extremely wide range of values, (ca. -75 per mille ca. -25 per mille). The hydrogen isotopic composition of the methane (d2H) ranged from -60 to -30per mille and -450 to -350per mille. These isotopic values are outside of the range of values normally considered to be biogenic, however incubations of the sediments in contact with these gas bubbles reveals that the methane is indeed being

Information content analysis: the potential for methane isotopologue retrieval from GOSAT-2

Science.gov (United States)

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

2018-02-01

Atmospheric methane is comprised of multiple isotopic molecules, with the most abundant being 12CH4 and 13CH4, making up 98 and 1.1 % of atmospheric methane respectively. It has been shown that is it possible to distinguish between sources of methane (biogenic methane, e.g. marshland, or abiogenic methane, e.g. fracking) via a ratio of these main methane isotopologues, otherwise known as the δ13C value. δ13C values typically range between -10 and -80 ‰, with abiogenic sources closer to zero and biogenic sources showing more negative values. Initially, we suggest that a δ13C difference of 10 ‰ is sufficient, in order to differentiate between methane source types, based on this we derive that a precision of 0.2 ppbv on 13CH4 retrievals may achieve the target δ13C variance. Using an application of the well-established information content analysis (ICA) technique for assumed clear-sky conditions, this paper shows that using a combination of the shortwave infrared (SWIR) bands on the planned Greenhouse gases Observing SATellite (GOSAT-2) mission, 13CH4 can be measured with sufficient information content to a precision of between 0.7 and 1.2 ppbv from a single sounding (assuming a total column average value of 19.14 ppbv), which can then be reduced to the target precision through spatial and temporal averaging techniques. We therefore suggest that GOSAT-2 can be used to differentiate between methane source types. We find that large unconstrained covariance matrices are required in order to achieve sufficient information content, while the solar zenith angle has limited impact on the information content.

Methane Formation by Flame-Generated Hydrogen Atoms in the Flame Ionization Detector

DEFF Research Database (Denmark)

Holm, Torkil; Madsen, Jørgen Øgaard

1996-01-01

, and conceivably all hydrocarbons are quantitatively converted into methane at temperatures below 600 C, that is, before the proper combustion has started. The splitting of the C-C bonds is preceded by hydrogenation of double and triple bonds and aromatic rings. The reactions, no doubt, are caused by hydrogen...... atoms, which are formed in the burning hydrogen and which diffuse into the inner core of the flame. The quantitative formation of methane appears to explain the "equal per carbon" rule for the detector response of hydrocarbons, since all carbons are "exchanged" for methane molecules....

First principles modeling of hydrocarbons conversion in non-equilibrium plasma

Energy Technology Data Exchange (ETDEWEB)

Deminsky, M.A.; Strelkova, M.I.; Durov, S.G.; Jivotov, V.K.; Rusanov, V.D.; Potapkin, B.V. [Russian Research Centre Kurchatov Inst., Moscow (Russian Federation)

2001-07-01

Theoretical justification of catalytic activity of non-equilibrium plasma in hydrocarbons conversion process is presented in this paper. The detailed model of highest hydrocarbons conversion includes the gas-phase reactions, chemistry of the growth of polycyclic aromatic hydrocarbons (PAHs), precursor of soot particles formation, neutral, charged clusters and soot particle formation, ion-molecular gas-phase and heterogeneous chemistry. The results of theoretical analysis are compared with experimental results. (authors)

Hydrocarbon pollution from marinas in estuarine sediments

Science.gov (United States)

Voudrias, Evangelos A.; Smith, Craig L.

1986-03-01

A measure of the impact of marinas on three Eastern Virginia estuarine creeks was obtained by a study of hydrocarbons in their sediments. Two of the creeks support considerable marine activity, including pleasure boat marinas, boat repair facilities, and commercial fishing operations. The third creek, which served as a control, is seldom used by boats, and is surrounded by marsh and woodland. Sediments from the creeks with marinas contained significantly higher levels of both aromatic and aliphatic hydrocarbons than did the control. Differences in the concentrations of certain oil-pollution indicators, such as the 17α,21β-hopane homologs and phytane, and low molecular weight aromatic hydrocarbons, are indicative of light petroleum fractions. Most of the aromatic hydrocarbons from all creeks, however, appear to have a pyrogenic origin. Although hydrocarbons from three probable origins (petroleum, pyrogenesis, and recent biosynthesis) were detected in all locations, the petroleum-derived and pyrogenic hydrocarbons were of only minor importance relative to the biogenic hydrocarbons in the control creek.

The effect of gas-phase polycyclic aromatic hydrocarbons on the formation and properties of biogenic secondary organic aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Zelenyuk, Alla [Pacific Northwest National Laboratory; USA; Imre, Dan G. [Imre Consulting; USA; Wilson, Jacqueline [Pacific Northwest National Laboratory; USA; Bell, David M. [Pacific Northwest National Laboratory; USA; Suski, Kaitlyn J. [Pacific Northwest National Laboratory; USA; Shrivastava, Manish [Pacific Northwest National Laboratory; USA; Beránek, Josef [Pacific Northwest National Laboratory; USA; Alexander, M. Lizabeth [Pacific Northwest National Laboratory; USA; Kramer, Amber L. [Department of Chemistry; Oregon State University; USA; Massey Simonich, Staci L. [Department of Chemistry; Oregon State University; USA; Environmental and Molecular Toxicology; Oregon State University

2017-01-01

When secondary organic aerosol (SOA) particles are formed by ozonolysis in the presence of gas-phase polycyclic aromatic hydrocarbons (PAHs), their formation and properties are significantly different from SOA particles formed without PAHs. For all SOA precursors and all PAHs, discussed in this study, the presence of the gas-phase PAHs during SOA formation significantly affects particle mass loadings, composition, growth, evaporation kinetics, and viscosity. SOA particles formed in the presence of PAHs have, as part of their compositions, trapped unreacted PAHs and products of heterogeneous reactions between PAHs and ozone. Compared to ‘pure’ SOA particles, these particles exhibit slower evaporation kinetics, have higher fractions of non-volatile components, like oligomers, and higher viscosities, assuring their longer atmospheric lifetimes. In turn, the increased viscosity and decreased volatility provide a shield that protects PAHs from chemical degradation and evaporation, allowing for the long-range transport of these toxic pollutants. The magnitude of the effect of PAHs on SOA formation is surprisingly large. The presence of PAHs during SOA formation increases mass loadings by factors of two to five, and particle number concentrations, in some cases, by more than a factor of 100. Increases in SOA mass, particle number concentrations, and lifetime have important implications to many atmospheric processes related to climate, weather, visibility, and human health, all of which relate to the interactions between biogenic SOA and anthropogenic PAHs. The synergistic relationship between SOA and PAHs presented here are clearly complex and call for future research to elucidate further the underlying processes and their exact atmospheric implications.

Concentrations and carbon isotope compositions of methane in the cored sediments from offshore SW Taiwan

Energy Technology Data Exchange (ETDEWEB)

Chuang, P.C.; Yang, T.F.; Hong, W.L. [National Taiwan Univ., Taipei, Taiwan (China). Dept. of Geosciences; Lin, S.; Chen, J.C. [National Taiwan Univ., Taipei, Taiwan (China). Inst. of Oceanography; Sun, C.H. [CPC Corp., Wen Shan, Miaoli, Taiwan (China). Exploration and Development Research Inst.; Wang, Y. [Central Geological Survey, MOEA, Taipei, Taiwan (China)

2008-07-01

Gas hydrates are natural occurring solids that contain natural gases, mainly methane, within a rigid lattice of water molecules. They are a type of non-stoichiometric clathrates and metastable crystal products in low temperature and high pressure conditions and are widely distributed in oceans and in permafrost regions around the world. Gas hydrates have been considered as potential energy resources for the future since methane is the major gas inside gas hydrates. Methane is also a greenhouse gas that might affect the global climates from the dissociations of gas hydrates. Bottom simulating reflections (BSRs) have been found to be widely distributed in offshore southwestern Taiwan therefore, inferring the existence of potential gas hydrates underneath the seafloor sediments. This paper presented a study that involved the systematic collection of sea waters and cored sediments as well as the analysis of the gas composition of pore-space of sediments through ten cruises from 2003 to 2006. The paper discussed the results in terms of the distribution of methane concentrations in bottom waters and cored sediments; methane fluxes in offshore southwestern Taiwan; and isotopic compositions of methane in pore spaces of cored sediments. It was concluded that the carbon isotopic compositions of methane demonstrated that biogenic gas source was dominated at shallower depth. However, some thermogenic gases might be introduced from deeper source in this region. 15 refs., 5 figs.

An intercomparison of biogenic emissions estimates from BEIS2 and BIOME: Reconciling the differences

Energy Technology Data Exchange (ETDEWEB)

Wilkinson, J.G. [Alpine Geophysics, Pittsburgh, PA (United States); Emigh, R.A. [Alpine Geophysics, Boulder, CO (United States); Pierce, T.E. [Atmospheric Characterization and Modeling Division/NOAA, Research Triangle Park, NC (United States)

1996-12-31

Biogenic emissions play a critical role in urban and regional air quality. For instance, biogenic emissions contribute upwards of 76% of the daily hydrocarbon emissions in the Atlanta, Georgia airshed. The Biogenic Emissions Inventory System-Version 2.0 (BEIS2) and the Biogenic Model for Emissions (BIOME) are two models that compute biogenic emissions estimates. BEIS2 is a FORTRAN-based system, and BIOME is an ARC/INFO{reg_sign} - and SAS{reg_sign}-based system. Although the technical formulations of the models are similar, the models produce different biogenic emissions estimates for what appear to be essentially the same inputs. The goals of our study are the following: (1) Determine why BIOME and BEIS2 produce different emissions estimates; (2) Attempt to understand the impacts that the differences have on the emissions estimates; (3) Reconcile the differences where possible; and (4) Present a framework for the use of BEIS2 and BIOME. In this study, we used the Coastal Oxidant Assessment for Southeast Texas (COAST) biogenics data which were supplied to us courtesy of the Texas Natural Resource Conservation Commission (TNRCC), and we extracted the BEIS2 data for the same domain. We compared the emissions estimates of the two models using their respective data sets BIOME Using TNRCC data and BEIS2 using BEIS2 data.

Halite as a Methane Sequestration Host: A Possible Explanation for Periodic Methane Release on Mars, and a Surface-accessible Source of Ancient Martian Carbon

Science.gov (United States)

Fries, M. D.; Steele, Andrew; Hynek, B. M.

2015-01-01

We present the hypothesis that halite may play a role in methane sequestration on the martian surface. In terrestrial examples, halite deposits sequester large volumes of methane and chloromethane. Also, examples of chloromethane-bearing, approximately 4.5 Ga old halite from the Monahans meteorite show that this system is very stable unless the halite is damaged. On Mars, methane may be generated from carbonaceous material trapped in ancient halite deposits and sequestered. The methane may be released by damaging its halite host; either by aqueous alteration, aeolian abrasion, heating, or impact shock. Such a scenario may help to explain the appearance of short-lived releases of methane on the martian surface. The methane may be of either biogenic or abiogenic origin. If this scenario plays a significant role on Mars, then martian halite deposits may contain samples of organic compounds dating to the ancient desiccation of the planet, accessible at the surface for future sample return missions.

Hydrocarbon pollution in the sediment from the Jarzouna-Bizerte coastal area of Tunisia (Mediterranean Sea).

Science.gov (United States)

Zrafi-Nouira, I; Khedir-Ghenim, Z; Zrafi, F; Bahri, R; Cheraeif, I; Rouabhia, M; Saidane-Mosbahi, D

2008-06-01

This study investigated the presence and origin of hydrocarbon pollution in industrial waste water sediments found near the Jarzouna (Bizerte, Tunisia) oil refinery. Analyses of surface sediments (layer 1) and deep sediments (layer 2) showed that Total Hydrocarbon (TH) concentrations ranged from 602 +/- 7.638 microg/g in layer-1 to 1270 +/- 2.176 microg/g in layer-2. The results suggest that the deeper the sediment, the higher the level of total hydrocarbon found. The sedimentary Non Aromatic Hydrocarbon (NAH) and Aromatic Hydrocarbon (AH) concentrations ranged from 66.22 +/- 1.516 to 211.82 +/- 10.670 microg/g for NAH, and from 13.84 +/- 0.180 to 115.60 +/- 2.479 microg/g for AH. The high variability of these concentrations was associated with the location of the sediment collection sites. Aliphatic biomarker analysis revealed petroleum contamination close to the refinery rejection site, and biogenic sources further away. Petroleum contamination may be associated with increased industrial activity in the area of Jarzouna-Bizerte in the Mediterranean Sea.

Vapor-Liquid Equilibrium of Methane with Water and Methanol. Measurements and Modeling

DEFF Research Database (Denmark)

Frost, Michael Grynnerup; Karakatsani, Eirini; von Solms, Nicolas

2014-01-01

that rely on phase equilibrium data for optimization. The objective of this work is to provide experimental data for hydrocarbon systems with polar chemicals such as alcohols, glycols, and water. New vapor-liquid equilibrium data are reported for methane + water, methane + methanol, and methane + methanol...

Eddy Covariance Measurements of Methane Flux at a Tropical Peat Forest in Sarawak, Malaysian Borneo

Science.gov (United States)

Tang, Angela C. I.; Stoy, Paul C.; Hirata, Ryuichi; Musin, Kevin K.; Aeries, Edward B.; Wenceslaus, Joseph; Melling, Lulie

2018-05-01

Tropical biogenic sources are a likely cause of the recent increase in global atmospheric methane concentration. To improve our understanding of tropical methane sources, we used the eddy covariance technique to measure CH4 flux (FCH4) between a tropical peat forest ecosystem and the atmosphere in Malaysian Borneo over a 2-month period during the wet season. Mean daily FCH4 during the measurement period, on the order of 0.024 g C-CH4·m-2·day-1, was similar to eddy covariance FCH4 measurements from tropical rice agroecosystems and boreal fen ecosystems. A linear modeling analysis demonstrated that air temperature (Tair) was critical for modeling FCH4 before the water table breached the surface and that water table alone explained some 20% of observed FCH4 variability once standing water emerged. Future research should measure FCH4 on an annual basis from multiple tropical ecosystems to better constrain tropical biogenic methane sources.

Information content analysis: the potential for methane isotopologue retrieval from GOSAT-2

Directory of Open Access Journals (Sweden)

E. Malina

2018-02-01

Full Text Available Atmospheric methane is comprised of multiple isotopic molecules, with the most abundant being 12CH4 and 13CH4, making up 98 and 1.1 % of atmospheric methane respectively. It has been shown that is it possible to distinguish between sources of methane (biogenic methane, e.g. marshland, or abiogenic methane, e.g. fracking via a ratio of these main methane isotopologues, otherwise known as the δ13C value. δ13C values typically range between −10 and −80 ‰, with abiogenic sources closer to zero and biogenic sources showing more negative values. Initially, we suggest that a δ13C difference of 10 ‰ is sufficient, in order to differentiate between methane source types, based on this we derive that a precision of 0.2 ppbv on 13CH4 retrievals may achieve the target δ13C variance. Using an application of the well-established information content analysis (ICA technique for assumed clear-sky conditions, this paper shows that using a combination of the shortwave infrared (SWIR bands on the planned Greenhouse gases Observing SATellite (GOSAT-2 mission, 13CH4 can be measured with sufficient information content to a precision of between 0.7 and 1.2 ppbv from a single sounding (assuming a total column average value of 19.14 ppbv, which can then be reduced to the target precision through spatial and temporal averaging techniques. We therefore suggest that GOSAT-2 can be used to differentiate between methane source types. We find that large unconstrained covariance matrices are required in order to achieve sufficient information content, while the solar zenith angle has limited impact on the information content.

Estimation of Methane from Hydrocarbon Exploration and Production in India

OpenAIRE

A. K. Pathak; K. Ojha

2012-01-01

Methane is the second most important greenhouse gas (GHG) after carbon dioxide. Amount of methane emission from energy sector is increasing day by day with various activities. In present work, various sources of methane emission from upstream, middle stream and downstream of oil & gas sectors are identified and categorised as per IPCC-2006 guidelines. Data were collected from various oil & gas sector like (i) exploration & production of oil & gas (ii) supply through pipel...

Active hydrocarbon (methane) seepage at the Alboran Sea mud volcanoes indicated by specific lipid biomarkers.

Science.gov (United States)

Lopez-Rodriguez, C.; Stadnitskaia, A.; De Lange, G. J.; Martínez-Ruiz, F.; Comas, M.; Sinninghe Damsté, J. S.

2012-04-01

Mud volcanoes (MVs) and pockmark fields are known to occur in the Alboran Basin (Westernmost Mediterranean). These MVs occur above a major sedimentary depocenter that includes up to 7 km thick early Miocene to Holocene sequences. MVs located on the top of diapiric structures that originated from undercompacted Miocene clays and olistostromes. Here we provide results from geochemical data-analyses of four gravity cores acquired in the Northern Mud Volcano Field (north of the 36°N): i.e. Perejil, Kalinin and Schneiderś Heart mud expulsion structures. Extruded materials include different types of mud breccias. Specific lipid biomarkers (n-alkanes, hopanes, irregular isoprenoid hydrocarbons and Dialkyl Glycerol Diethers (DGDs) were analysed by gas chromatography (GC) and gas chromatography mass spectrometry (GC-MS). Determination of Glycerol Dialkyl Glycerol Tetraethers (GDGTs) by high performance liquid chromatography-spectrometry (HPLC-MS), and analysis of biomarker δ13C values were performed in selected samples. Lipid biomarker analysis from the three MVs revealed similar n-alkane distributions in all mud breccia intervals, showing significant hydrocarbon-derived signals and the presence of thermally immature organic-matter admixture. This suggests that similar strata fed these MVs. The hemipelagic drapes reveal comparable n-alkane distributions, suggesting that significant upward diffusion of fluids occurs. Distributions of GDGTs are generally accepted as usefull biomarkers to locate the anaerobic oxidation of methane (AOM) in marine sediments. However, our GDGT profiles only reflect the marine thaumarchaeotal signature. There seems to be no archaea producing specific GDGTs involved in AOM in the recovered interval. Evidence of recent activity (i.e., methane gas-bubbling and chemosynthetic fauna at the Perejil MV) and the presence of specific lipid biomarker related with methanotropic archaea (Irregular Isoprenoids and DGDs), however, suggest the existence of

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

Science.gov (United States)

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.

Aliphatic hydrocarbon and polycyclic aromatic hydrocarbon geochemistry of twelve major rivers in the Northwest Territories

International Nuclear Information System (INIS)

Backus, S.; Swyripa, M.; Peddle, J.; Jeffries, D.S.

1995-01-01

Suspended sediment and water samples collected from twelve major rivers in the Northwest Territories were analyzed for aliphatic hydrocarbons and polycyclic aromatic hydrocarbons (PAHs) to assess the sources and transport of hydrocarbons entering the Arctic Ocean. Three stations on the Mackenzie River and one station near the mouth of eleven other northern rivers were selected for sampling. Samples were collected on the Mackenzie River on four occasions to characterize spring, summer and fall flow conditions and once on the remaining eleven rivers during high flow conditions. The Mackenzie River is distinctively different then the other eleven rivers. Naturally occurring hydrocarbons predominate in the river. These hydrocarbons include biogenic alkanes, diagenic PAHs, petrogenic alkanes, and PAHs from oil seeps and/or bitumens. Anthropogenic inputs of PAHs are low as indicated by low concentrations of combustion PAHs. Alkyl PAH distributions indicate that a significant component of the lower molecular weight PAH fraction is petrogenic. The majority of the high molecular weight PAHs, together with the petrogenic PAHs have a principal source in the Mackenzie River

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

Energy Technology Data Exchange (ETDEWEB)

Schwab, Amy [National Renewable Energy Lab. (NREL), Golden, CO (United States); Warner, Ethan [National Renewable Energy Lab. (NREL), Golden, CO (United States); Lewis, John [National Renewable Energy Lab. (NREL), Golden, CO (United States)

2016-01-22

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.

A PROCESS FOR THE CATALYTIC OXIDATION OF HYDROCARBONS

DEFF Research Database (Denmark)

1999-01-01

A process for producing an alcohol from a gaseous hydrocarbon, e.g. a lower alkane such as methane, via oxidative reaction of the hydrocarbon in a concentrated sulfuric acid medium in the presence of a catalyst employs an added catalyst comprising a substance selected from iodine, iodine compounds...

Operation of marine diesel engines on biogenic fuels: modification of emissions and resulting climate effects.

Science.gov (United States)

Petzold, Andreas; Lauer, Peter; Fritsche, Uwe; Hasselbach, Jan; Lichtenstern, Michael; Schlager, Hans; Fleischer, Fritz

2011-12-15

The modification of emissions of climate-sensitive exhaust compounds such as CO(2), NO(x), hydrocarbons, and particulate matter from medium-speed marine diesel engines was studied for a set of fossil and biogenic fuels. Applied fossil fuels were the reference heavy fuel oil (HFO) and the low-sulfur marine gas oil (MGO); biogenic fuels were palm oil, soybean oil, sunflower oil, and animal fat. Greenhouse gas (GHG) emissions related to the production of biogenic fuels were treated by means of a fuel life cycle analysis which included land use changes associated with the growth of energy plants. Emissions of CO(2) and NO(x) per kWh were found to be similar for fossil fuels and biogenic fuels. PM mass emission was reduced to 10-15% of HFO emissions for all low-sulfur fuels including MGO as a fossil fuel. Black carbon emissions were reduced significantly to 13-30% of HFO. Changes in emissions were predominantly related to particulate sulfate, while differences between low-sulfur fossil fuels and low-sulfur biogenic fuels were of minor significance. GHG emissions from the biogenic fuel life cycle (FLC) depend crucially on energy plant production conditions and have the potential of shifting the overall GHG budget from positive to negative compared to fossil fuels.

Addressing biogenic greenhouse gas emissions from hydropower in LCA.

Science.gov (United States)

Hertwich, Edgar G

2013-09-03

The ability of hydropower to contribute to climate change mitigation is sometimes questioned, citing emissions of methane and carbon dioxide resulting from the degradation of biogenic carbon in hydropower reservoirs. These emissions are, however, not always addressed in life cycle assessment, leading to a bias in technology comparisons, and often misunderstood. The objective of this paper is to review and analyze the generation of greenhouse gas emissions from reservoirs for the purpose of technology assessment, relating established emission measurements to power generation. A literature review, data collection, and statistical analysis of methane and CO2 emissions are conducted. In a sample of 82 measurements, methane emissions per kWh hydropower generated are log-normally distributed, ranging from micrograms to 10s of kg. A multivariate regression analysis shows that the reservoir area per kWh electricity is the most important explanatory variable. Methane emissions flux per reservoir area are correlated with the natural net primary production of the area, the age of the power plant, and the inclusion of bubbling emissions in the measurement. Even together, these factors fail to explain most of the variation in the methane flux. The global average emissions from hydropower are estimated to be 85 gCO2/kWh and 3 gCH4/kWh, with a multiplicative uncertainty factor of 2. GHG emissions from hydropower can be largely avoided by ceasing to build hydropower plants with high land use per unit of electricity generated.

Oxidative coupling of methane using inorganic membrane reactor

Energy Technology Data Exchange (ETDEWEB)

Ma, Y.H.; Moser, W.R.; Dixon, A.G. [Worcester Polytechnic Institute, MA (United States)] [and others

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 gas 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.

Methanogens and Martian natural resources: Investigations regarding the possibility of biogenic methane on Mars

Science.gov (United States)

Chastain, Brendon Kelly

Archaeal methanogens were suggested as terrestrial models of possible subsurface martian microbial life prior to the actual detection of methane in Mars' atmosphere. This idea gained even more interest after the methane on Mars was observed. However, the amount of methane detected was very small, and release of methane was localized and episodic. This led some scientists to doubt that an active or ancient biosphere could be the source of the methane. Moreover, even extremophilic methanogens have not been shown to metabolize in conditions exactly analogous to those known to be available on Mars. The following chapters present a realistic and viable mechanism that allows a large or ancient biosphere to be the original source of the observed methane, and they detail experimental work that was done in order to systematically investigate nutritional and conditional variables related to those that might be available in the martian subsurface. The results of the experimental work indicate that some components of Mars' regolith can support methanogenic metabolism without being detrimental to the organisms, and that certain known components of Mars' regolith can promote periods of methanogenic dormancy without being lethal to the methanogens. The results of the experimental studies also show that material known to exist at and near Mars' surface has the potential to supply electrons for biological methanogenesis and that methanogenic metabolism can occur even when artificial media, buffers, and reductants are omitted in order to create more Mars-relevant conditions. These findings may have implications regarding the viability of methanogenic organisms as a source of the observed methane and should assist future efforts to study methanogenic metabolism in conditions exactly analogous to those available in niches on Mars.

Electrocatalytic oxidation of methane: investigations of new catalysts to be used in a solid polymer electrolyte methane fuel-cell; Oxydation electrocatalytique du methane: recherche de catalyseurs en vue d'une application a une pile au methane a electrolyte polymere solide

Energy Technology Data Exchange (ETDEWEB)

Berthelot, S

1998-07-01

This thesis evaluated the performances of many catalysts facing the methane oxidation which is a critical step in methane fuel cells development. In a first part the study of the methane electro-oxidation has been realized by classical electrochemical technics on many electrodes to determine the most active ones. In a second part the in situ reflection infra-red spectroscopy allowed to identify, during the methane oxidation, the adsorbed species on the electrode and the reaction products. These results also help the understanding of the part of the concerned materials mechanisms in the methane oxidation and then to optimize them for a whole oxidation of the methane in carbon dioxide. The final objective is the use of the methane in a PEMFC fuel cell type. A comparison with the methanol and C2 hydrocarbons behaviour, such as the ethane the ethylene and the acetylene, has been done to evaluate the performances. (A.L.B.)

Radiation-induced chemical reaction of methane in the presence of X-and Y-type molecular sieves

International Nuclear Information System (INIS)

Shimizu, Y.; Nagai, S.

1990-01-01

The radiolysis of methane was investigated in the presence of X (13X) and Y (SK-40) type molecular sieves at 300 0 C. Product analysis showed that irradiation of methane over 13X and SK-40 produces hydrogen and hydrocarbons up to C 5 . The yields of hydrocarbons, except for ethylene, over 13X and SK-40 slightly increased with irradiation time. The yields of the main hydrocarbon products over SK-40 were larger than those in the absence of molecular sieve in contrast to those over 13X. It was found that no 13X shows catalytic activity for the radiolysis of methane; on the other hand, SK-40 shows it. The relations between the proportion of hydrocarbon yield of each carbon number to the hydrocarbon total yield over 13X and SK-40 and the carbon number were the same as those in the absence of molecular sieve. It was proved by comparison of these results with those over A-type molecular sieve (5A) that the order of the catalytic activities of the molecular sieves for the radiolysis of methane differs considerably from that found in thermal catalytic reactions. These results are discussed in terms of the concept of energy transfer and the relation between the pore size of the molecular sieves and the molecular diameters of the hydrocarbons produced. (author)

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

Energy Technology Data Exchange (ETDEWEB)

Warner, Ethan [National Renewable Energy Lab. (NREL), Golden, CO (United States); Schwab, Amy [National Renewable Energy Lab. (NREL), Golden, CO (United States); Bacovsky, Dina [Bioenergy 2020+ GmbH (Germany)

2017-02-01

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).

Microbial methane from in situ biodegradation of coal and shale: A review and reevaluation of hydrogen and carbon isotope signatures

Science.gov (United States)

Vinson, David S.; Blair, Neal E.; Martini, Anna M.; Larter, Steve; Orem, William H.; McIntosh, Jennifer C.

2017-01-01

Stable carbon and hydrogen isotope signatures of methane, water, and inorganic carbon are widely utilized in natural gas systems for distinguishing microbial and thermogenic methane and for delineating methanogenic pathways (acetoclastic, hydrogenotrophic, and/or methylotrophic methanogenesis). Recent studies of coal and shale gas systems have characterized in situ microbial communities and provided stable isotope data (δD-CH4, δD-H2O, δ13C-CH4, and δ13C-CO2) from a wider range of environments than available previously. Here we review the principal biogenic methane-yielding pathways in coal beds and shales and the isotope effects imparted on methane, document the uncertainties and inconsistencies in established isotopic fingerprinting techniques, and identify the knowledge gaps in understanding the subsurface processes that govern H and C isotope signatures of biogenic methane. We also compare established isotopic interpretations with recent microbial community characterization techniques, which reveal additional inconsistencies in the interpretation of microbial metabolic pathways in coal beds and shales. Collectively, the re-assessed data show that widely-utilized isotopic fingerprinting techniques neglect important complications in coal beds and shales.Isotopic fingerprinting techniques that combine δ13C-CH4 with δD-CH4 and/or δ13C-CO2have significant limitations: (1) The consistent ~ 160‰ offset between δD-H2O and δD-CH4 could imply that hydrogenotrophic methanogenesis is the dominant metabolic pathway in microbial gas systems. However, hydrogen isotopes can equilibrate between methane precursors and coexisting water, yielding a similar apparent H isotope signal as hydrogenotrophic methanogenesis, regardless of the actual methane formation pathway. (2) Non-methanogenic processes such as sulfate reduction, Fe oxide reduction, inputs of thermogenic methane, anaerobic methane oxidation, and/or formation water interaction can cause the apparent carbon

Effect of substrate temperature on the structure of amorphous oxygenated hydrocarbon films grown with a pulsed supersonic methane plasma flow

Energy Technology Data Exchange (ETDEWEB)

Fedoseeva, Yu. V., E-mail: fedoseeva@niic.nsc.ru [Nikolaev Institute of Inorganic Chemistry SB RAS, Novosibirsk 630090 (Russian Federation); Novosibirsk State University, Novosibirsk 630090 (Russian Federation); Pozdnyakov, G.A. [Khristianovich Institute of Theoretical and Applied Mechanics, SB RAS, Novosibirsk 630090 (Russian Federation); Okotrub, A.V.; Kanygin, M.A. [Nikolaev Institute of Inorganic Chemistry SB RAS, Novosibirsk 630090 (Russian Federation); Novosibirsk State University, Novosibirsk 630090 (Russian Federation); Nastaushev, Yu. V. [Rzhanov Institute of Semiconductor Physics SB RAS, Novosibirsk 630090 (Russian Federation); Vilkov, O.Y. [St. Petersburg State University, St. Petersburg 198504 (Russian Federation); Bulusheva, L.G. [Nikolaev Institute of Inorganic Chemistry SB RAS, Novosibirsk 630090 (Russian Federation); Novosibirsk State University, Novosibirsk 630090 (Russian Federation)

2016-11-01

Highlights: • A deposition of supersonic methane plasma flow on silicon substrate produces amorphous oxygenated hydrocarbon (CO{sub x}H{sub y}) film. • The thickness, composition, and wettability of the film depend on the substrate temperature. • A rise of the substrate temperature from 500 to 700 °C promotes the sp{sup 3}-hybridization carbon formation. - Abstract: Since amorphous oxygenated hydrocarbon (CO{sub x}H{sub y}) films are promising engineering materials a study of the structure and composition of the films depending on the conditions of synthesis is important for controlling of their physicochemical properties. Here, we used the methods of scanning and transmission electron microscopy, X-ray photoelectron, near-edge X-ray absorption fine structure, Fourier transform infrared and Raman spectroscopy to reveal changes in the chemical connectivity of CO{sub x}H{sub y} films grown on silicon substrates heated to 300, 500, and 700 °C using a supersonic flow of methane plasma. It was found that the CO{sub x}H{sub y} films, deposited at 300 and 500 °C, were mainly composed of the sp{sup 2}-hybridized carbon areas with various oxygen species. A rise of the substrate temperature caused an increase of the portion of tetrahedral carbon atoms as well as carboxyl and hydroxyl groups. With growth of the substrate temperature, the film thickness reduced monotonically from 400 to 180 nm, while the film adhesion improved substantially. The films, deposited at lower temperatures, showed high hydrophilicity due to porosity and presence of oxygenated groups both at the surface and in the bulk.

Effect of Cooling Methods on Methane Conversion via Dielectric-Barrier Discharges

International Nuclear Information System (INIS)

Wang Baowei; Yang Kuanhui; Xu Genhui

2008-01-01

Effects of cooling methods on stability and methane conversion rate using dielectric-barrier discharges (DBD) were systematically investigated in this article. The results showed that the methane conversion rate was as high as 44.43% in a pure methane system at a flow rate of 100 mL ± min -1 and an input power of 234.2 W with air cooling. A dark greenish and soft film-like carbon was deposited on the outer surface of quartz tube when the outer electrode was water-cooled, which decreased the methane conversion. With air cooling of inner electrode the selectivity of C 2 hydrocarbons was higher than that with other cooling methods, while the C 3 hydrocarbons had higher selectivity with flowing water cooling. Cooling the inner electrode could restrain the carbon deposition, but would decrease the methane conversion rate. The stability of both reaction and plasma operation can be improved through cooling the reactor. From thermodynamic analysis, it was found that the effective collisions frequency among the reactant molecules and free electrons (e - ) increased with temperature, which in turn led to a higher methane conversion rate and a change in the distribution of products.

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

Science.gov (United States)

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).

Distribution and origin of dissolved methane, ethane and propane in shallow groundwater of Lower Saxony, Germany

International Nuclear Information System (INIS)

Schloemer, S.; Elbracht, J.; Blumenberg, M.; Illing, C.J.

2016-01-01

More than 90% of Germany's domestic natural gas production and reserves are located in Lower Saxony, North Germany. Recently, research has been intensified with respect to unconventional shale gas, revealing a large additional resource potential in northern Germany. However, many concerns arise within the general public and government/political institutions over potential groundwater contamination from additional gas wells through hydraulic fracturing operations. In order to determine the naturally occurring background methane concentrations, ∼1000 groundwater wells, covering ∼48 000 km 2 , have been sampled and subsequently analyzed for dissolved methane, ethane and propane and the isotopic composition of methane (δ 13 C). Dissolved methane concentrations cover a range of ∼7 orders of magnitude between the limit of quantification at ∼20 nl/l and 60 ml/l. The majority of groundwater wells exhibit low concentrations (<1 μl/l), a small number of samples (65) reveal concentration in the range >10 ml/l. In 27% of all samples ethane and in 8% ethane and propane was detected. The median concentration of both components is generally very low (ethane 50 nl/l, propane 23 nl/l). Concentrations reveal a bimodal distribution of the dissolved gas, which might mirror a regional trend due to different hydrogeological settings. The isotopic composition of methane is normally distributed (mean ∼ −70‰ vs PDB), but shows a large variation between −110‰ and +20‰. Samples with δ 13 C values lower than −55‰ vs PDB (66%) are indicative for methanogenic biogenic processes. 5% of the samples are unusually enriched in 13 C (≥25‰ vs PDB) and can best be explained by microbial methane oxidation. According to a standard diagnostic diagram based on methane δ 13 C values and the ratio of methane over the sum over ethane plus propane (“Bernard”-diagram) less than 4% of the samples plot into the diagnostic field of typical thermogenic natural

The indirect global warming potential and global temperature change potential due to methane oxidation

International Nuclear Information System (INIS)

Boucher, Olivier; Collins, Bill; Friedlingstein, Pierre; Shine, Keith P

2009-01-01

Methane is the second most important anthropogenic greenhouse gas in the atmosphere next to carbon dioxide. Its global warming potential (GWP) for a time horizon of 100 years is 25, which makes it an attractive target for climate mitigation policies. Although the methane GWP traditionally includes the methane indirect effects on the concentrations of ozone and stratospheric water vapour, it does not take into account the production of carbon dioxide from methane oxidation. We argue here that this CO 2 -induced effect should be included for fossil sources of methane, which results in slightly larger GWP values for all time horizons. If the global temperature change potential is used as an alternative climate metric, then the impact of the CO 2 -induced effect is proportionally much larger. We also discuss what the correction term should be for methane from anthropogenic biogenic sources.

Methane - quick fix or tough target? New methods to reduce emissions.

Science.gov (United States)

Nisbet, E. G.; Lowry, D.; Fisher, R. E.; Brownlow, R.

2016-12-01

Methane is a cost-effective target for greenhouse gas reduction efforts. The UK's MOYA project is designed to improve understanding of the global methane budget and to point to new methods to reduce future emissions. Since 2007, methane has been increasing rapidly: in 2014 and 2015 growth was at rates last seen in the 1980s. Unlike 20thcentury growth, primarily driven by fossil fuel emissions in northern industrial nations, isotopic evidence implies present growth is driven by tropical biogenic sources such as wetlands and agriculture. Discovering why methane is rising is important. Schaefer et al. (Science, 2016) pointed out the potential clash between methane reduction efforts and food needs of a rising, better-fed (physically larger) human population. Our own work suggests tropical wetlands are major drivers of growth, responding to weather changes since 2007, but there is no acceptable way to reduce wetland emission. Just as sea ice decline indicates Arctic warming, methane may be the most obvious tracker of climate change in the wet tropics. Technical advances in instrumentation can do much in helping cut urban and industrial methane emissions. Mobile systems can be mounted on vehicles, while drone sampling can provide a 3D view to locate sources. Urban land planning often means large but different point sources are typically clustered (e.g. landfill or sewage plant near incinerator; gas wells next to cattle). High-precision grab-sample isotopic characterisation, using Keeling plots, can separate source signals, to identify specific emitters, even where they are closely juxtaposed. Our mobile campaigns in the UK, Kuwait, Hong Kong and E. Australia show the importance of major single sources, such as abandoned old wells, pipe leaks, or unregulated landfills. If such point sources can be individually identified, even when clustered, they will allow effective reduction efforts to occur: these can be profitable and/or improve industrial safety, for example in the

OXIDATIVE COUPLING OF METHANE USING INORGANIC MEMBRANE REACTORS

Energy Technology Data Exchange (ETDEWEB)

Dr. Y.H. Ma; Dr. W.R. Moser; Dr. A.G. Dixon; Dr. A.M. Ramachandra; Dr. Y. Lu; C. Binkerd

1998-04-01

The objective of this research is to study the oxidative coupling of methane in catalytic inorganic membrane reactors. A specific target is to achieve conversion of methane to C{sub 2} hydrocarbons at very high selectivity and higher yields than in conventional non-porous, co-feed, 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 gas phase reactions, which are believed to be a main route for the formation of CO{sub x} products. Such gas phase reactions are a cause of decreased selectivity in the 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. Membrane reactor technology also offers the potential for modifying the membranes both to improve catalytic properties as well as to regulate the rate of the permeation/diffusion of reactants through the membrane to minimize by-product generation. Other benefits also exist with membrane reactors, such as the mitigation of thermal hot-spots for highly exothermic reactions such as the oxidative coupling of methane. The application of catalytically active inorganic membranes has potential for drastically increasing the yield of reactions which are currently limited by either thermodynamic equilibria, product inhibition, or kinetic selectivity.

Emissions of hydrocarbons from marine phytoplankton—Some results from controlled laboratory experiments

Science.gov (United States)

McKay, W. A.; Turner, M. F.; Jones, B. M. R.; Halliwell, C. M.

Laboratory experiments have been carried out to help assess and quantify the role of marine phytoplankton in the production of non-methane hydrocarbons. Evidence is presented here that supports the hypothesis that some short-chain hydrocarbons are produced during diatom and dinoflagellate lifecycles. The pattern of their emissions to the air above axenic unicultures of diatoms and dinoflagellates has been followed. The results suggest that ethane, ethene, propane and propene are produced during the autolysis of some phytoplankton, possibly by the oxidation of polyunsaturated lipids released into their culture medium. In contrast, isoprene and hexane appear during phytoplankton growth and are thus most likely produced either directly by the plankton or through the oxidation of exuded dissolved organic carbon.

Development of oil hydrocarbon fingerprinting and identification techniques

International Nuclear Information System (INIS)

Wang Zhendi; Fingas, Merv F.

2003-01-01

Oil, refined product, and pyrogenic hydrocarbons are the most frequently discovered contaminants in the environment. To effectively determine the fate of spilled oil in the environment and to successfully identify source(s) of spilled oil and petroleum products is, therefore, extremely important in many oil-related environmental studies and liability cases. This article briefly reviews the recent development of chemical analysis methodologies which are most frequently used in oil spill characterization and identification studies and environmental forensic investigations. The fingerprinting and data interpretation techniques discussed include oil spill identification protocol, tiered analytical approach, generic features and chemical composition of oils, effects of weathering on hydrocarbon fingerprinting, recognition of distribution patterns of petroleum hydrocarbons, oil type screening and differentiation, analysis of 'source-specific marker' compounds, determination of diagnostic ratios of specific oil constituents, stable isotopic analysis, application of various statistical and numerical analysis tools, and application of other analytical techniques. The issue of how biogenic and pyrogenic hydrocarbons are distinguished from petrogenic hydrocarbons is also addressed

Geologic Emissions of Methane and C2 - C5 Alkanes at the La Brea Tar Pits, Los Angeles, CA

Science.gov (United States)

Doezema, L. A.; Etiope, G.; Pacheco, C.

2017-12-01

Natural hydrocarbon (oil and gas) seeps are widespread in Los Angeles due to gas migration, along faults, from numerous subsurface petroleum fields. These seeps may represent important natural contributors of methane (CH4) and heavier alkanes (C2-C4) for the atmosphere. Methane flux measurements were made from various locations at the La Brea Tar Pits in Los Angeles, CA. Measurements were made using a closed-chamber method and spectroscopic sensors for CH4 and CO2, at 26 oil-asphalt seeps and 188 other sites, without gas manifestations, homogeneously distributed throughout the park. The molecular C1 - C5 composition of gas released from seeps and soil was also analyzed using either FTIR spectroscopy or gas chromatography (GC-FID). Methane emissions from seeps varied from approximately 7 to 54,000 g m-2 day-1, while emissions from soil degassing were between 0 and 9,000 g m-2 day-1. Total emissions were estimated to be in the order of 103 kg day-1 for methane, and at least 10 and 5 kg day-1 for ethane and propane, respectively. The seeping gas exhibited high C1/(C2 + C3) ratios, likely due to molecular fractionation during gas migration from a subsurface petroleum reservoir. Evidence for biodegredation in certain samples was indicated by large i-butane to n-butane ratios. These molecular alterations can be important tracers of natural seepage and should be considered in the atmospheric modelling of the relative contribution of fossil fuel (anthropogenic fugitive emission and natural geologic sources) vs biogenic sources, on local and global scales.

Methane synthesis under mild conditions for decentralized applications

International Nuclear Information System (INIS)

Schlueter, Michael; Roensch, Stefan

2016-01-01

It is a central aim of the German government to significantly reduce the emission of greenhouse gases in the next years. One possibility to reach this aim is the substitution of fossil fuels, especially natural gas, by fuels from biogenic sources (Bio-SNG). However, it is a drawback of Bio-SNG that the production costs are considerably higher than those of fossil natural gas. This work provides an approach to reduce the production costs of Bio-SNG. It is the aim to reduce the process parameters of the methane synthesis. At the same time, it has to be ensured that high methane yields are achieved even at those mild conditions. A procedure for the optimization of the methanation catalyst activity will be presented. If the catalyst is as active as possible even at mild conditions, it will be possible to produce Bio-SNG cost efficient even in small, decentralized scale.

Ceramic Proppant Design for In-situ Microbially Enhanced Methane Recovery

Energy Technology Data Exchange (ETDEWEB)

Sparks, Taylor D. [Univ. of Utah, Salt Lake City, UT (United States); Mclennan, John [Univ. of Utah, Salt Lake City, UT (United States); Fuertez, John [Univ. of Utah, Salt Lake City, UT (United States); Han, Kyu-Bum [Univ. of Utah, Salt Lake City, UT (United States)

2017-12-29

This project designed a new type of multi-functional lightweight proppant. The proppant is utilized as the conventional lightweight proppant but also transports microorganisms to coalbed reservoirs. The proppant is coated with a polymer which protects the methanogenic microorganisms and serves as a time-release delivery for methane generation. To produce the multifunctional proppant, we assigned five tasks: 1) culturing methanogenic microbes from natural carbon sources; 2) identifying optimized growth and methanogenesis conditions for the microbial consortia; 3) synthesizing the lightweight ceramic proppant; 4) encapsulating the consortia and proppant; and 5) demonstrating lab scale simulated performance by monitoring in-situ methane generation and hydraulic conductivity. Task 1) To evaluate the feasibility of ex-situ cultivation, natural microbial populations were collected from various hydrocarbon-rich environments and locations characterized by natural methanogenesis. Different rank coals, complex hydrocarbon sources, hydrocarbon seeps, and natural biogenic environments were incorporated in the sampling. Three levels of screening allowed selection of microbial populations, favorable nutrient amendments, sources of the microbial community, and quantification of methane produced from various coal types. Incubation periods of up to 24 weeks were evaluated at 23°C. Headspace concentrations of CH₄ and CO₂ were analyzed by gas chromatography. After a two-week incubation period of the most promising microbes, generated headspace gas concentrations reached 873,400 ppm for methane and 176,370 ppm for carbon dioxide. Task 2) A central composite design (CCD) was used to explore a broad range of operational conditions, examine the effects of the important environmental factors, such as temperature, pH and salt concentration, and query a feasible region of operation to maximize methane production from coal. Coal biogasification was optimal for this

Emission of the main biogenic volatile organic compounds in France

International Nuclear Information System (INIS)

Luchetta, L.; Simon, V.; Torres, L.

2000-01-01

An estimation of biogenic emissions of the main non-methanic Volatile Organic Compounds (VOCs) due to the forest cover in France has been realized. 32 species representing 98% of French forest have been considered for the estimation. The latter dealt on a net made of 93 irregular spatial grids (Departments) with an average size of 75 km x 75 km. We assigned emission rates and foliar biomass densities specific to each of the 32 species. The environmental variables (temperature, light intensity) have been collected for the whole of French Departments. A special effort was extended so as to use ''Guenther's'' calculation algorithms, and specific emitting factors to species growing in France or in bordering countries. Along the way of the five years (1994-1998) of the study we have calculated the yearly mean of isoprene, mono-terpenes and Other Volatile Organic Compounds (OVOCs) emissions on the scale of the French Departments. At the national level isoprene emission is reckoned at 457 kt yr -1 and represents nearly 49% of the total emission, whereas mono-terpenes with 350 kt yr -1 and OVOCs with 129 kt yr -1 represent respectively 37% and 14% of the total. The yearly biogenic emission of VOCs in France represents virtually half the anthropic source. However in some regions (Mediterranean area) natural emissions can widely exceed anthropic emissions during certain periods. Let's note the whole of our results remains tinged with a great uncertainty because the estimations carried out are presented with correction factors that can reach values comprised between 4 and 7. (author)

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

Science.gov (United States)

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.

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

Science.gov (United States)

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 (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 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.

Hydrothermal waste package interactions with methane-containing basalt groundwater

International Nuclear Information System (INIS)

McGrail, B.P.

1984-01-01

Hydrothermal waste package interaction tests were conducted with a mixture of crushed glass, basalt, and steel in methane-containing synthetic basalt groundwater. In the absence of gamma radiolysis, methane was found to have little influence on the corrosion behavior of the waste package constituents. Under gamma radiolysis, methane was found to significantly lower the solution oxidation potential when compared to identical tests without methane. In addition, colloidal hydrocarbon polymers that have been produced under the irradiation conditions of these experiments were not formed. The presence of the waste package constituents apparently inhibited the formation of the polymers. However, the mechanism which prevented their formation was not determined

Origin of the Ability of α-Fe2 O3 Mesopores to Activate C-H Bonds in Methane.

Science.gov (United States)

Dong, Bing; Han, Zhen; Zhang, Yongbo; Yu, Youyi; Kong, Aiguo; Shan, Yongkui

2016-02-01

Methane is a most abundant and inexpensive hydrocarbon feedstock for the production of chemicals and fuels. However, it is extremely difficult to directly convert methane to higher hydrocarbons because the C-H bonds in methane are the most stable C-H bonds of all hydrocarbons. The activation of the C-H bonds in methane by using an efficient and mild route remains a daunting challenge. Here, we show that the inner surface structures of the pore walls in mesoporous α-Fe 2 O 3 possess excellent catalytic performance for methane activation and convert C-H bonds into the C-O bonds in an O 2 atmosphere at 140 °C. We found that such unusual structures are mainly comprised of turbostratic ribbons and K crystal faces and have higher catalytic activity than the (110) plane. These results are without precedent in the history of catalysis chemistry and will provide a new pathway for designing and preparing highly efficient catalytic materials. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Effects of water vapor on the radiolysis of methane over molecular sieve 5A

International Nuclear Information System (INIS)

Shimizu, Y.; Nagai, S.

1989-01-01

Effects of the addition of H 2 O on the radiation-induced chemical reaction of methane over molecular sieve 5A at 460 0 C have been studied by product analysis. Hydrogen, carbon monoxide, carbon dioxide and hydrocarbons consisting mainly of C 2 and C 3 alkanes and alkenes were produced from CH 4 + H 2 O mixtures at high conversion levels. The yields of hydrocarbons from 3:1 and 3:2 CH 4 + H 2 O mixtures decreased slightly with time but those from 3:4 mixture showed no decrease with time. When the molecular sieve 5A that had been irradiated in flowing methane was reirradiated in the presence of H 2 O, carbonaceous solid produced from methane on molecular sieve 5A was readily decomposed to carbon dioxide, carbon monoxide, hydrogen and hydrocarbons, mainly alkanes. Therefore, it is concluded that the suppression of decrease of product yields with time by the addition of H 2 O is mainly ascribed to decomposition of the carbonaceous solid by H 2 O under electron beam irradiation. The role of added H 2 O is also discussed in connection with the conventional methane-steam reforming reaction. (author)

An advanced method of contributing emissions to short-lived chemical species (OH and HO2: the TAGGING 1.1 submodel based on the Modular Earth Submodel System (MESSy 2.53

Directory of Open Access Journals (Sweden)

V. S. Rieger

2018-06-01

Full Text Available To mitigate the human impact on climate change, it is essential to determine the contribution of emissions to the concentration of trace gases. In particular, the source attribution of short-lived species such as OH and HO2 is important as they play a crucial role for atmospheric chemistry. This study presents an advanced version of a tagging method for OH and HO2 (HOx which attributes HOx concentrations to emissions. While the former version (V1.0 only considered 12 reactions in the troposphere, the new version (V1.1, presented here, takes 19 reactions in the troposphere into account. For the first time, the main chemical reactions for the HOx chemistry in the stratosphere are also regarded (in total 27 reactions. To fully take into account the main HO2 source by the reaction of H and O2, the tagging of the H radical is introduced. In order to ensure the steady-state assumption, we introduce rest terms which balance the deviation of HOx production and loss. This closes the budget between the sum of all contributions and the total concentration. The contributions to OH and HO2 obtained by the advanced tagging method V1.1 deviate from V1.0 in certain source categories. For OH, major changes are found in the categories biomass burning, biogenic emissions and methane decomposition. For HO2, the contributions differ strongly in the categories biogenic emissions and methane decomposition. As HOx reacts with ozone (O3, carbon monoxide (CO, reactive nitrogen compounds (NOy, non-methane hydrocarbons (NMHCs and peroxyacyl nitrates (PAN, the contributions to these species are also modified by the advanced HOx tagging method V1.1. The contributions to NOy, NMHC and PAN show only little change, whereas O3 from biogenic emissions and methane decomposition increases in the tropical troposphere. Variations for CO from biogenic emissions and biomass burning are only found in the Southern Hemisphere.

Plasma Thermal Conversion of Methane to Acetylene

International Nuclear Information System (INIS)

Fincke, James Russell; Anderson, Raymond Paul; Hyde, Timothy Allen; Detering, Brent Alan; Wright, Randy Ben; Bewley, Randy Lee; Haggard, Delon C; Swank, William David

2002-01-01

This paper describes a re-examination of a known process for the direct plasma thermal conversion of methane to acetylene. Conversion efficiencies (% methane converted) approached 100% and acetylene yields in the 90-95% range with 2-4% solid carbon production were demonstrated. Specificity for acetylene was higher than in prior work. Improvements in conversion efficiency, yield, and specificity were due primarily to improved injector design and reactant mixing, and minimization of temperature gradients and cold boundary layers. At the 60-kilowatt scale cooling by wall heat transfer appears to be sufficient to quench the product stream and prevent further reaction of acetylene resulting in the formation of heavier hydrocarbon products or solid carbon. Significantly increasing the quenching rate by aerodynamic expansion of the products through a converging-diverging nozzle led to a reduction in the yield of ethylene but had little effect on the yield of other hydrocarbon products. While greater product selectivity for acetylene has been demonstrated, the specific energy consumption per unit mass of acetylene produced was not improved upon. A kinetic model that includes the reaction mechanisms resulting in the formation of acetylene and heavier hydrocarbons, through benzene, is described

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

Science.gov (United States)

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

Composition and Sources of Particulate Matter Measured near Houston, TX: Anthropogenic-Biogenic Interactions

Directory of Open Access Journals (Sweden)

Jeffrey K. Bean

2016-05-01

Full Text Available Particulate matter was measured in Conroe, Texas (~60 km north of downtown Houston, Texas during the September 2013 DISCOVER-AQ campaign to determine the sources of particulate matter in the region. The measurement site is influenced by high biogenic emission rates as well as transport of anthropogenic pollutants from the Houston metropolitan area and is therefore an ideal location to study anthropogenic-biogenic interactions. Data from an Aerosol Chemical Speciation Monitor (ACSM suggest that on average 64 percent of non-refractory PM1 was organic material, including a high fraction (27%–41% of organic nitrates. There was little diurnal variation in the concentrations of ammonium sulfate; however, concentrations of organic and organic nitrate aerosol were consistently higher at night than during the day. Potential explanations for the higher organic aerosol loadings at night include changing boundary layer height, increased partitioning to the particle phase at lower temperatures, and differences between daytime and nighttime chemical processes such as nitrate radical chemistry. Positive matrix factorization was applied to the organic aerosol mass spectra measured by the ACSM and three factors were resolved—two factors representing oxygenated organic aerosol and one factor representing hydrocarbon-like organic aerosol. The factors suggest that the measured aerosol was well mixed and highly processed, consistent with the distance from the site to major aerosol sources, as well as the high photochemical activity.

Characterization of VOCs Across Pennsylvania: Assessing Emissions from Rural, Forested, Agricultural and Natural Gas Drilling-Impacted Areas

Science.gov (United States)

Grannas, A. M.; Fuentes, J. D.; Ramos-Garcés, F.; Wang, D. K.; Martins, D. K.

2012-12-01

Volatile organic compounds (VOCs) of both biogenic and anthropogenic origin are important to troposphere chemistry, particularly the formation of photochemical smog and secondary organic aerosol. There is concern that increased natural gas exploration may lead to increased emissions of certain VOCs during well development and due to fugitive emissions from operational well sites and pipelines. For a six-day period in June 2012, a variety of VOCs were measured using canister sampling from a mobile measurement platform. Transects from southwestern to northeastern Pennsylvania were studied, with samples obtained in rural, forested, urban, farm-impacted and gas well-impacted sites. As expected, biogenic VOCs and isoprene oxidation products were enhanced in forested regions, while anthropogenic non-methane hydrocarbons were enhanced in urban areas. BTEX (benzene, toluene, ethylbenzene and xylenes) was enhanced in urban areas, but the concentrations of BTEX measured near developing and existing natural gas sites were similar to rural and forested sites. Halogenated hydrocarbons and Freon compounds were consistent at all site locations. We will discuss the specific concentrations and signatures of these compounds and assess the potential impact of agricultural activities and gas well development on the observed VOC concentrations and variability.

Raman Spectra of Methane, Ethylene, Ethane, Dimethyl ether, Formaldehyde and Propane for Combustion Applications

KAUST Repository

Magnotti, G.

2015-05-09

Spontaneous Raman scattering measurements of temperature and major species concentration in hydrocarbon-air flames require detailed knowledge of the Raman spectra of the hydrocarbons present when fuels more complex than methane are used. Although hydrocarbon spectra have been extensively studied at room temperature, there are no data available at higher temperatures. Quantum mechanical calculations, when available are not sufficiently accurate for combustion applications. This work presents experimental measurements of spontaneous Stokes-Raman scattering spectra of methane, ethylene, ethane, dimethyl ether, formaldehyde and propane in the temperature range 300-860 K. Raman spectra from heated hydrocarbons jets have been collected with a higher resolution than is generally employed for Raman measurements in combustion applications. A set of synthetic spectra have been generated for each hydrocarbon, providing the basis for extrapolation to higher temperatures. The spectra provided here will enable simultaneous measurements of multiple hydrocarbons in flames. This capability will greatly extend the range of applicability of Raman measurements in combustion applications. In addition, the experimental spectra provide a validation dataset for quantum mechanical models.

Raman Spectra of Methane, Ethylene, Ethane, Dimethyl ether, Formaldehyde and Propane for Combustion Applications

KAUST Repository

Magnotti, G.; KC, Utsav; Varghese, P.L.; Barlow, R.S.

2015-01-01

Spontaneous Raman scattering measurements of temperature and major species concentration in hydrocarbon-air flames require detailed knowledge of the Raman spectra of the hydrocarbons present when fuels more complex than methane are used. Although hydrocarbon spectra have been extensively studied at room temperature, there are no data available at higher temperatures. Quantum mechanical calculations, when available are not sufficiently accurate for combustion applications. This work presents experimental measurements of spontaneous Stokes-Raman scattering spectra of methane, ethylene, ethane, dimethyl ether, formaldehyde and propane in the temperature range 300-860 K. Raman spectra from heated hydrocarbons jets have been collected with a higher resolution than is generally employed for Raman measurements in combustion applications. A set of synthetic spectra have been generated for each hydrocarbon, providing the basis for extrapolation to higher temperatures. The spectra provided here will enable simultaneous measurements of multiple hydrocarbons in flames. This capability will greatly extend the range of applicability of Raman measurements in combustion applications. In addition, the experimental spectra provide a validation dataset for quantum mechanical models.

Mobile Measurement of Methane and Ethane for the Detection and Attribution of Natural Gas Pipeline Leaks Using Off-Axis Integrated Output Spectroscopy

Science.gov (United States)

Leen, J. B.; Spillane, S.; Gardner, A.; Hansen, P. C.; Gupta, M.; Baer, D. S.

2015-12-01

Natural gas leaks pose a risk to public safety both because of potential explosions as well as from the greenhouse gas potential of fugitive methane. The rapid and cost effective detection of leaks in natural gas distribution is critical to providing a system that is safe for the public and the environment. Detection of methane from a mobile platform (vehicles, aircraft, etc.) is an accepted method of identifying leaks. A robust approach to differentiating pipeline gas (thermogenic) from other biogenic sources is the detection of ethane along with methane. Ethane is present in nearly all thermogenic gas but not in biogenic sources and its presence can be used to positively identify a gas sample. We present a mobile system for the simultaneous measurement of methane and ethane that is capable of detecting pipeline leaks and differentiating pipeline gas from other biogenic sources such as landfills, swamps, sewers, and enteric fermentation. The mobile system consists of a high precision GPS, sonic anemometer, and methane/ethane analyzer based on off-axis integrated cavity output spectroscopy (OA-ICOS). In order to minimize the system cost and facilitate the wide use of mobile leak detection, the analyzer operates in the near-infrared portion of the spectrum where lasers and optics are significantly less costly than in the mid-infrared. The analyzer is capable of detecting methane with a precision of detecting ethane with a precision of detection of leaks at speeds up to 50 mph. The sonic anemometer, GPS and analyzer inlet are mounted to a generic roof rack for attachment to available fleet vehicles. The system can detect leaks having a downwind concentration of as little as 10 ppb of methane above ambient, while leaks 500 ppb above ambient can be identified as thermogenic with greater than 99% certainty (for gas with 6% ethane). Finally, analysis of wind data provides an estimate of leak direction and distance. The system presented provides a robust, cost effective

SHS-produced intermetallides as catalysts for hydrocarbons synthesis from CO and H{sub 2}

Energy Technology Data Exchange (ETDEWEB)

Eliseev, O.L.; Kazantsev, R.V.; Davydov, P.E.; Lapidus, A.L. [Russian Academy of Sciences, Moscow (Russian Federation). N.D. Zelinsky Institute of Organic Chemistry; Borshch, V.N.; Pugacheva, E.V. [Russian Academy of Sciences, Chernogolovka (Russian Federation). Inst. of Structural Macrokinetics and Materials Science

2012-07-01

Raney-type polymetallic alloys were prepared by Self-Propagating High-Temperature Synthesis followed by alkaline treating. Surface morphology and composition of were studied using XRD, BET, SEM and EMPA techniques. The samples were tested in Fischer-Tropsch synthesis demonstrated rather high activity and very high selectivity to heavy paraffins. High selectivity to C{sub 5+} hydrocarbons is attributed to high thermal conductivity of alloys which prevents hot spots formation and therefore suppresses formation of methane and light hydrocarbons. Selectivity can be further improved by adding some d-metals in catalyst composition. Promotion with La seems to be particularly suitable for lowering methane formation while doping with Ni enhances methane yield greatly. (orig.)

Non-Controlled Biogenic Emission of CO, H2S, NH3 and Hg0 from Lazareto's Landfill, Tenerife, Canary Islands

Science.gov (United States)

Nolasco, D.; Lima, R.; Salazar, J.; Hernández, P. A.; Pérez, N. M.

2002-12-01

Landfills are important sources of contaminant gases to the surrounding environment and a significant amount of them could be released to the atmosphere through the surface environment in a diffuse form, also known as non-controlled emission of landfill gases. CH4 and CO2 are major components in landfill gases and other gas species are only present in minor amounts. Trace compounds include both inorganic and a large number of volatile organic components. The goal of this study is to evaluate the non-controlled biogenic emission of inorganic toxic gases from Lazareto's landfill. Which is located in the city of Santa Cruz de Tenerife, with a population of about 150,000, and is used as a Palm tree park. Lazareto's landfill has an extension of 0.22 Km2 and it is not operative since 1980. A non-controlled biogenic gas emission survey of 281 sampling sites was carried out from February tod March, 2002. Surface CO2 efflux measurements were performed by means of a portable NDIR sensor according with the accumulation chamber method. Surface CO2 efflux ranged from negligible values up to 30,600 gm-2d-1. At each sampling site, surface landfill gas samples were collected at 40 cm depth using a metallic soil probe. These gas samples were analyzed within 24 hours for major and inorganic toxic gas species by means of microGC and specific electrochemical sensors. The highest concentrations of CO, H2S, NH3 and Hg0 were 3, 20, 2,227, 0.010 ppmV, respectively. Non-controlled biogenic emission rate of CO, H2S, NH3, and Hg0 were estimated by multiplying the observed surface CO2 efflux times (Inorganic Toxic Gas)i/CO2 weight ratio at each sampling site, respectively. The highest surface inorganic toxic gas efllux rates were 699 gm-2d-1 for NH3, 81, 431 and 4 mgm-2d-1 for CO, H2S and Hg0, respectively. Taking into consideration the spatial distribution of the inorganic toxic gas efflux values as well as the extension of the landfill, the non-controlled biogenic emission of CO, H2S, NH3

Non conventional hydrocarbons in Maghreb - an announced ecocide

International Nuclear Information System (INIS)

Balvet, Jacqueline; Espagne, Vincent; Rondeleux, Nejma; Dupont, Stephane

2015-01-01

Whereas gas and oil companies did not succeed in the development of shale gas exploration and exploitation in Europe for different reasons (citizen mobilisation against these projects, resources much smaller than expected), these companies are looking in other directions, notably the Maghreb region (North Africa) which is an important hydrocarbon supplier for European countries. This publication proposes an overview of the situation in Algeria, Morocco and Tunisia regarding this exploitation. It first recalls health and pollution impacts and consequences of hydraulic fracturing, and also the impact of hydrocarbon consumption on climate change. It indicates assessments made by the EIA of resources of shale gas and shale oil in the three countries, and outlines that these assessments might be too high as it has been the case in other countries. An overview of the situation of the three countries is then proposed, starting with Algeria: the third world shale gas reserve, presence of Total and GDF-Suez as investors with Sonatrach (the Algerian company) keeping a large majority, existence of a law which authorises the exploitation of non conventional hydrocarbons, and a very strong mobilisation of populations in the Algerian Sahara. The case of Morocco is then addressed: high dependence on imports but important non conventional reserves, exploitation of several sites, good conditions awarded to multinational companies, a focus on two important investors (Chevron and Repsol), start of a citizen mobilisation. The case of Tunisia is finally addressed: discovery of 'miraculous' deposits, overview of investors, a new but absolutely iniquitous legal framework, mobilisation of local associations

Carbon-14 measurements in aquifers with methane

International Nuclear Information System (INIS)

Barker, J.F.; Fritz, P.; Brown, R.M.

1979-01-01

A survey of various groundwater systems indicates that methane is a common trace constituent and occasionally a major carbon species in groundwaters. Thermocatalytic methane had delta 13 Csub(CH 4 )>-45 per mille and microbially produced or biogenic methane had delta 13 Csub(CH 4 ) 13 C values for the inorganic carbon. Thermocatalytic methane had no apparent effect on the inorganic carbon. Because methanogenesis seriously affects the carbon isotope geochemistry of groundwaters, the correction of raw 14 C ages of affected groundwaters must consider these effects. Conceptual models are developed which adjust the 14 C activity of the groundwater for the effects of methanogenesis and for the dilution of carbon present during infiltration by simple dissolution of rock carbonate. These preliminary models are applied to groundwaters from the Alliston sand aquifer where methanogenesis has affected most samples. In this system, methanogenic bacteria using organic matter present in the aquifer matrix as substrate have added inorganic carbon to the groundwater which has initiated further carbonate rock dissolution. These processes have diluted the inorganic carbon 14 C activity. The adjusted groundwater ages can be explained in terms of the complex hydrogeology of this aquifer, but also indicate that these conceptual models must be more rigorously tested to evaluate their appropriateness. (author)

Radiolytic degradation of chlorinated hydrocarbons in water

Energy Technology Data Exchange (ETDEWEB)

Wu, Xing-Zheng; Yamamoto, Takeshi [Fukui Univ., Faculty of Engineering, Dept. of Materials Science and Engineering, Fukui (Japan); Hatashita, Masanori [The Wakasa Wan Energy Research Center, Research Dept., Tsuruga, Fukui (Japan)

2002-11-01

Radiolytic degradation of chlorinated hydrocarbons (chloroform, trichloroethylene, and tetrachloroethylene) in water was carried out. Water solutions of the chlorinated hydrocarbons with different concentrations were irradiated with {gamma} rays. Concentrations of methane, ethane, CO, CO{sub 2}, H{sub 2}, and O{sub 2} after the irradiation were determined by gas chromatography. Concentration of chloride ion in the irradiated sample was determined by ion chromatography. Experimental results show that radiolytic degradation of the chlorinated hydrocarbon increased with the radiation dose. Methane, ethane, CO{sub 2}, H{sub 2}, and Cl{sup -} concentrations increased with the radiation dose and the sample concentration. On the other hand, O{sub 2} concentration decreased with the radiation dose and the sample concentration. When sample concentration was high, dissolved oxygen might be not enough for converting most of the C atoms in the sample into CO{sub 2}. This resulted in a low decomposition ratio. Addition of H{sub 2}O{sub 2} as an oxygen resource could increase the decomposition ratio greatly. Furthermore, gas chromatography-mass spectroscopy was applied to identify some intermediates of the radiolytic dehalogenation. Radiolytic degradation mechanisms are also discussed. (author)

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

Science.gov (United States)

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

Syntrophic biodegradation of hydrocarbon contaminants.

Science.gov (United States)

Gieg, Lisa M; Fowler, S Jane; Berdugo-Clavijo, Carolina

2014-06-01

Anaerobic environments are crucial to global carbon cycling wherein the microbial metabolism of organic matter occurs under a variety of redox conditions. In many anaerobic ecosystems, syntrophy plays a key role wherein microbial species must cooperate, essentially as a single catalytic unit, to metabolize substrates in a mutually beneficial manner. Hydrocarbon-contaminated environments such as groundwater aquifers are typically anaerobic, and often methanogenic. Syntrophic processes are needed to biodegrade hydrocarbons to methane, and recent studies suggest that syntrophic hydrocarbon metabolism can also occur in the presence of electron acceptors. The elucidation of key features of syntrophic processes in defined co-cultures has benefited greatly from advances in 'omics' based tools. Such tools, along with approaches like stable isotope probing, are now being used to monitor carbon flow within an increasing number of hydrocarbon-degrading consortia to pinpoint the key microbial players involved in the degradative pathways. The metagenomic sequencing of hydrocarbon-utilizing consortia should help to further identify key syntrophic features and define microbial interactions in these complex communities. Copyright © 2013 Elsevier Ltd. All rights reserved.

Methane Release and Pingo-Like Feature Across the South kara Sea Shels, an Area of Thawing Offshore Permafrost

Science.gov (United States)

Serov, P.; Portnov, A.; Mienert, J.

2015-12-01

Thawing subsea permafrost controls methane release from the Russian Arctic shelf having a considerable impact on the climate-sensitive Arctic environment. Our recent studies revealed extensive gas release over an area of at least 7500 km2and presence of pingo-like features (PLFs), showing severe methane leakage, in the South Kara Sea in water depths >20m (Serov et al., 2015). Specifically, we detected shallow methane ebullition sites expressed in water column acoustic anomalies (gas flares and gas fronts) and areas of increased dissolved methane concentrations in bottom water, which might be sufficient sources of carbon for seawater-atmosphere exchange. A study of nature and source of leaking gas was focused on two PLFs, which are acoustically transparent circular mounds towering 5-9 m above the surrounding seafloor. One PLF (PLF 2) connects to biogenic gas from deeper sources, which is reflected in δ13CCH4 values ranging from -55,1‰ to -88,0‰ and δDCH4values varied from -175‰ to -246‰. Low organic matter content (0.52-1.69%) of seafloor sediments restricts extensive in situ methane production. The formation of PLF 2 is directly linked to the thawing of subsea permafrost and, possibly, decomposition of permafrost related gas hydrates. High accumulations of biogenic methane create the necessary forces to push the remaining frozen layers upwards and, therefore, form a topographic feature. We speculate that PLF 1, which shows ubiquitously low methane concentrations, is either a relict submerged terrestrial pingo, or a PLF lacking the necessary underlying methane accumulations. Our model of glacial-interglacial permafrost evolution supports a scenario in which subsea permafrost tapers seaward and pinches out at 20m isobaths, controlling observed methane emissions and development of PLFs. Serov. P., A. Portnov, J. Mienert, P. Semenov, and P. Ilatovskaya (2015), Methane release from pingo-like features across the South Kara Sea shelf, an area of thawnig

The Global Search for Abiogenic GHGs, via Methane Isotopes and Ethane

Science.gov (United States)

Malina, Edward; Muller, Jan-Peter; Walton, David; Potts, Dale

2015-04-01

The importance of Methane as an anthropogenic Green House Gas (GHG) is well recognized in the scientific community, and is second only to Carbon Dioxide in terms of influence on the Earth's radiation budget (Parker, et al, 2011) suggesting that the ability to apportion the source of the methane (whether it is biogenic, abiogenic or thermogenic) has never been more important. It has been proposed (Etiope, 2009) that it may be possible to distinguish between a biogenic methane source (e.g. bacteria fermentation) and an abiogenic source (e.g. gas seepage or fugitive emissions) via the retrieval of the abundances of methane isotopes (12CH4 and 13CH4) and through the ratio of ethane (C2H6) to methane (CH4) concentrations. Using ultra fine spectroscopy (simulations, we show that it is possible to distinguish between methane isotopes using the FTS based instruments on ACE and GOSAT, and retrieve the abundances in the Short Wave Infra-red (SWIR) at 1.65μm, 2.3μm, 3.3μm and Thermal IR, 7.8μm wavebands for methane, and the 3.3μm and 7μm wavebands for ethane. Initially we use the spectral line database HITRAN to determine the most appropriate spectral waveband to retrieve methane isotopes (and ethane) with minimal water vapour, CO2 and NO2 impact. Following this, we have evaluated the detectability of these trace gases using the more sophisticated Radiative Transfer Models (RTMs) SCIATRAN, the Oxford RFM and MODTRAN 5 in the SWIR, in order to determine the barriers to retrieving methane isotopes in both ACE (limb profile) and GOSAT (nadir measurements) instruments, including a preliminary investigation into the effects of clouds, aerosols, surface reflectance on the retrieval of methane isotopes. The aim of these RTM simulations is to further narrow down the spectral regions (originally identified in the HITRAN assessment) where methane isotopes can/may be retrieved from orbit. The key outputs from the RTM study are absorption and radiance data, which allow us to

Measurement of the first Townsend ionization coefficient in a methane-based tissue-equivalent gas

Energy Technology Data Exchange (ETDEWEB)

Petri, A.R. [Instituto de Pesquisas Energéticas e Nucleares, Cidade Universitária, 05508-000 São Paulo (Brazil); Gonçalves, J.A.C. [Instituto de Pesquisas Energéticas e Nucleares, Cidade Universitária, 05508-000 São Paulo (Brazil); Departamento de Física, Pontifícia Universidade Católica de São Paulo, 01303-050 São Paulo (Brazil); Mangiarotti, A. [Instituto de Física - Universidade de São Paulo, Cidade Universitária, 05508-080 São Paulo (Brazil); Botelho, S. [Instituto de Pesquisas Energéticas e Nucleares, Cidade Universitária, 05508-000 São Paulo (Brazil); Bueno, C.C., E-mail: ccbueno@ipen.br [Instituto de Pesquisas Energéticas e Nucleares, Cidade Universitária, 05508-000 São Paulo (Brazil)

2017-03-21

Tissue-equivalent gases (TEGs), often made of a hydrocarbon, nitrogen, and carbon dioxide, have been employed in microdosimetry for decades. However, data on the first Townsend ionization coefficient (α) in such mixtures are scarce, regardless of the chosen hydrocarbon. In this context, measurements of α in a methane-based tissue-equivalent gas (CH{sub 4} – 64.4%, CO{sub 2} – 32.4%, and N{sub 2} – 3.2%) were performed in a uniform field configuration for density-normalized electric fields (E/N) up to 290 Td. The setup adopted in our previous works was improved for operating at low pressures. The modifications introduced in the apparatus and the experimental technique were validated by comparing our results of the first Townsend ionization coefficient in nitrogen, carbon dioxide, and methane with those from the literature and Magboltz simulations. The behavior of α in the methane-based TEG was consistent with that observed for pure methane. All the experimental results are included in tabular form in the .

Characterization and speciation of non-methane hydrocarbons (NMHCs) and their implications on the atmosphere of South China

Science.gov (United States)

Tang, Jianhui

2007-12-01

A large pool of ambient and source NMHC data was obtained for the first time in various environments of South China, extending from less developed Yunnan and Hainan Provinces to more developed Guangdong and Zhejiang Provinces. The source and source regions of these C2-C10 NMHC species were assessed through comparison of the profiles and characteristic ratios of NMHC species in ambient and source samples. Tools such as backward air trajectory and satellite images are utilized. Analysis of NMHC profiles in these regions unveiled that there were complex characteristics of NMHCs involving different extents of contributions from urban vehicular and industrial emissions, local biofuel combustion and biogenic emissions, and biomass burning emissions. At the developed sites, such as Guangzhou in Pearl River Delta (PRD) and Lin'an in Yangtze River Delta (YRD), vehicular and industrial emissions were the major contributors. However, in rural and remote areas such as at Jiangfeng Mountain on Hainan Island and Tengchong Mountain in southwest of China, long-range transports of biomass burning pollution from the SE Asia subcontinent in addition to contributions from in situ biogenic and other local anthropogenic emissions from South China, are important sources of NMHCs in spring. More in depth studies were conducted in the urban sites of Guangzhou and at the rural site of Dinghu Mountain during 2001 to 2005. The levels of toluene increased in Dinghu Mountain but decreased in Guangzhou urban sites, which was contrary to the increase of industrial activities in this region. This was in part due to the implementation of stringent emission standards for polluting industries especially in the urban areas and the relocation of polluting industries from urban to the less developed parts of the PRD. We had found for the first time significant increase of propane levels in the urban air of Guangzhou, due to the introduction of LPG-fueled buses and taxis. The signatures of LPG influence

Hydrothermal waste package interactions with methane-containing basalt groundwater

International Nuclear Information System (INIS)

McGrail, B.P.

1984-11-01

Hydrothermal waste package interaction tests with methane-containing synthetic basalt groundwater have shown that in the absence of gamma radiolysis, methane has little influence on the glass dissolution rate. Gamma radiolysis tests at fluxes of 5.5 x 10 5 and 4.4 x 10 4 R/hr showed that methane-saturated groundwater was more reducing than identical experiments where Ar was substituted for CH 4 . Dissolved methane, therefore, may be beneficial to the waste package in limiting the solubility of redox sensitive radionuclides such a 99 Tc. Hydrocarbon polymers known to form under the irradiation conditions of these tests were not produced. The presence of the waste package constituents apparently inhibited the formation of the polymers, however, the mechanism which prevented their formation was not determined

Model study of the impact of biogenic emission on regional ozone and the effectiveness of emission reduction scenarios over eastern China

International Nuclear Information System (INIS)

Han, Zhiwei; Matsuda, Kazuhide; Ueda, Hiromasa

2005-01-01

The impact of biogenic emission on regional ozone and emission control scenarios has been numerically studied through a series of sensitivity model simulations. A typical episode with elevated ozone over eastern China from 12 to 16 August 2001 was investigated by using a tropospheric chemistry and transport model (TCTM), driven by a non-hydrostatic mesoscale model MM5. The meteorological conditions during this period were characterized by high-pressure systems associated with low wind speeds, high temperatures and clear skies. Afternoon ozone concentrations exceeding 80 parts per billion (ppb) occurred over broad areas of eastern China. There is a generally good agreement between simulation and observation, indicating that the TCTM is able to represent major physical and chemical processes of tropospheric ozone and well reproduce the diurnal and day-to-day variability associated with synoptic conditions. The sensitivity analysis reveals a significant influence of biogenic hydrocarbons on regional ozone. Ozone levels are apparently enhanced by biogenic emission over large areas of eastern China. The largest increase up to 30 ppb in daytime average concentration is found in portions of the middle reaches of the Yangtze River, Yangtze Delta and northeast China. However, the response of ozone to biogenic emission varies spatially, showing more sensitivity in polluted areas than that in clean rural areas. The regimes limited by nitrogen oxides (NO x ) and volatile organic carbon (VOC) in eastern China are further investigated with respect to biogenic emission. Ozone shows a clear tendency to shift from VOC limitation to NO x limitation as it moves from urban and industrial areas to rural areas. Most of the rural areas in southern China tend to be NO x limited, whereas most of the northern parts of China appear to be VOC limited. By considering biogenic emission, ozone tends to become more NO x limited and less VOC limited, both in extent and intensity, over eastern

Biogenic Methane Generation Potential in the Eastern Nankai Trough, Japan: Effect of Reaction Temperature and Total Organic Carbon

Science.gov (United States)

Aung, T. T.; Fujii, T.; Amo, M.; Suzuki, K.

2017-12-01

Understanding potential of methane flux from the Pleistocene fore-arc basin filled turbiditic sedimentary formation along the eastern Nankai Trough is important in the quantitative assessment of gas hydrate resources. We considered generated methane could exist in sedimentary basin in the forms of three major components, and those are methane in methane hydrate, free gas and methane dissolved in water. Generation of biomethane strongly depends on microbe activity and microbes in turn survive in diverse range of temperature, salinity and pH. This study aims to understand effect of reaction temperature and total organic carbon on generation of biomethane and its components. Biomarker analysis and cultural experiment results of the core samples from the eastern Nankai Trough reveal that methane generation rate gets peak at various temperature ranging12.5°to 35°. Simulation study of biomethane generation was made using commercial basin scale simulator, PetroMod, with different reaction temperature and total organic carbon to predict how these effect on generation of biomethane. Reaction model is set by Gaussian distribution with constant hydrogen index and standard deviation of 1. Series of simulation cases with peak reaction temperature ranging 12.5°to 35° and total organic carbon of 0.6% to 3% were conducted and analyzed. Simulation results show that linear decrease in generation potential while increasing reaction temperature. But decreasing amount becomes larger in the model with higher total organic carbon. At higher reaction temperatures, >30°, extremely low generation potential was found. This is due to the fact that the source formation modeled is less than 1 km in thickness and most of formation do not reach temperature more than 30°. In terms of the components, methane in methane hydrate and free methane increase with increasing TOC. Drastic increase in free methane was observed in the model with 3% of TOC. Methane amount dissolved in water shows almost

High Time Resolution Measurements of Methane Fluxes From Enteric Fermentation in Cattle Rumen

Science.gov (United States)

Floerchinger, C. R.; Herndon, S.; Fortner, E.; Roscioli, J. R.; Kolb, C. E.; Knighton, W. B.; Molina, L. T.; Zavala, M.; Castelán, O.; Ku Vera, J.; Castillo, E.

2013-12-01

Methane accounts for roughly 20% of the global radiative climate forcing in the last two and a half centuries. Methane emissions arise from a number of anthropogenic and biogenic sources. In some areas enteric fermentation in livestock produces over 90% of agricultural methane. In the spring of 2013, as a part of the Short Lived Climate Forcer-Mexico field campaign, the Aerodyne Mobile Laboratory in partnership with the Molina Center for the Environment studied methane production associated with enteric fermentation in the rumen of cattle. A variety of different breeds and stocks being raised in two agricultural and veterinary research facilities located in different areas of Mexico were examined. Methane fluxes were quantified using two methods: 1) an atmospherically stable gaseous tracer release was collocated with small herds in a pasture, allowing tracer ratio flux measurements; 2) respiratory CO2 was measured in tandem with methane in the breath of individual animals allowing methane production to be related to metabolism. The use of an extensive suite of very high time response instruments allows for differentiation of individual methane producing rumination events and respiratory CO2 from possible background interferences. The results of these studies will be presented and compared to data from traditional chamber experiments.

H2S mediated thermal and photochemical methane activation

Science.gov (United States)

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.

Science.gov (United States)

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.

Process for producing ethane and/or ethylene from methane. Verfahren zur Herstellung von Ethan und bzw. oder Ethylen aus Methan

Energy Technology Data Exchange (ETDEWEB)

Baerns, M.; Hinsen, W.

1984-04-12

According to the invention, methane is converted into hydrocarbons with oxygen with high selectivity. This is done in the presence of a catalyst fluidized in a fluidized bed - preferably lead oxide or a mixture of this with antimony oxide - at temperatures between 600 and 800/sup 0/C and at oxygen partial pressures preferably below 0.1-0.2 bar. The ratio of methane partial pressure to oxygen partial pressure should be greater than 2 to 5 if possible. The reactor is operated with gas feedback, in order to raise the selectivity even more.

Non-microbial methane emissions from soils

Science.gov (United States)

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 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 from the well-known microbial CH4 formation in order to define both roles in the atmospheric CH4 global budget.

High atmosphere–ocean exchange of semivolatile aromatic hydrocarbons

KAUST Repository

González-Gaya, Belén

2016-05-16

Polycyclic aromatic hydrocarbons, and other semivolatile aromatic-like compounds, are an important and ubiquitous fraction of organic matter in the environment. The occurrence of semivolatile aromatic hydrocarbons is due to anthropogenic sources such as incomplete combustion of fossil fuels or oil spills, and other biogenic sources. However, their global transport, fate and relevance for the carbon cycle have been poorly assessed, especially in terms of fluxes. Here we report a global assessment of the occurrence and atmosphere-ocean fluxes of 64 polycyclic aromatic hydrocarbons analysed in paired atmospheric and seawater samples from the tropical and subtropical Atlantic, Pacific and Indian oceans. The global atmospheric input of polycyclic aromatic hydrocarbons to the global ocean is estimated at 0.09 Tg per month, four times greater than the input from the Deepwater Horizon spill. Moreover, the environmental concentrations of total semivolatile aromatic-like compounds were 10 2 -10 3 times higher than those of the targeted polycyclic aromatic hydrocarbons, with a relevant contribution of an aromatic unresolved complex mixture. These concentrations drive a large global deposition of carbon, estimated at 400 Tg C yr -1, around 15% of the oceanic CO2 uptake. © 2016 Macmillan Publishers Limited.

Organic compounds in aerosols from selected European sites - Biogenic versus anthropogenic sources

Science.gov (United States)

Alves, Célia; Vicente, Ana; Pio, Casimiro; Kiss, Gyula; Hoffer, Andras; Decesari, Stefano; Prevôt, André S. H.; Minguillón, María Cruz; Querol, Xavier; Hillamo, Risto; Spindler, Gerald; Swietlicki, Erik

2012-11-01

Atmospheric aerosol samples from a boreal forest (Hyytiälä, April 2007), a rural site in Hungary (K-puszta, summer 2008), a polluted rural area in Italy (San Pietro Capofiume, Po Valley, April 2008), a moderately polluted rural site in Germany located on a meadow (Melpitz, May 2008), a natural park in Spain (Montseny, March 2009) and two urban background locations (Zurich, December 2008, and Barcelona, February/March 2009) were collected. Aliphatics, polycyclic aromatic hydrocarbons, carbonyls, sterols, n-alkanols, acids, phenolic compounds and anhydrosugars in aerosols were chemically characterised by gas chromatography-mass spectrometry, along with source attribution based on the carbon preference index (CPI), the ratios between the unresolved and the chromatographically resolved aliphatics, the contribution of wax n-alkanes, n-alkanols and n-alkanoic acids from plants, diagnostic ratios of individual target compounds and source-specific markers to organic carbon ratios. In spite of transboundary pollution episodes, Hyytiälä registered the lowest levels among all locations. CPI values close to 1 for the aliphatic fraction of the Montseny aerosol suggest that the anthropogenic input may be associated with the transport of aged air masses from the surrounding industrial/urban areas, which superimpose the locally originated hydrocarbons with biogenic origin. Aliphatic and aromatic hydrocarbons in samples from San Pietro Capofiume reveal that fossil fuel combustion is a major source influencing the diel pattern of concentrations. This source contributed to 25-45% of the ambient organic carbon (OC) at the Po Valley site. Aerosols from the German meadow presented variable contributions from both biogenic and anthropogenic sources. The highest levels of vegetation wax components and biogenic secondary organic aerosol (SOA) products were observed at K-puszta, while anthropogenic SOA compounds predominated in Barcelona. The primary vehicular emissions in the Spanish

Screening of hydrocarbons as supercritical ORCs working fluids by thermal stability

International Nuclear Information System (INIS)

Dai, Xiaoye; Shi, Lin; An, Qingsong; Qian, Weizhong

2016-01-01

Highlights: • A rapid evaluation method for thermal stability of hydrocarbons for ORCs. • Methane and hydrogen are confirmed to be decomposition indicators. • The decomposition temperatures for some hydrocarbons using the rapid method. • Long carbon chain hydrocarbons are not suitable for supercritical ORCs. - Abstract: Organic Rankine Cycle (ORC) systems are widely used for industrial waste heat recovery and renewable energy utilization. The supercritical ORC is currently one of the main development directions due to its low exergy loss, high thermal efficiency and high work output. The thermal stability is the major limitation of organic working fluid selection with high temperature heat sources. This paper presents a rapid experimental method for assessing the thermal stability of hydrocarbons for ORCs. The fluids were tested in a high temperature reactor with methane and hydrogen theoretically and experimentally confirmed to be the indicators of thermal decomposition. The thermal decomposition temperatures were obtained for n-hexane, n-pentane, isopentane, cyclopentane, n-butane and isobutane using the rapid experimental method. The results show that cycloalkanes are not the good choices by thermal stability and long carbon chain hydrocarbons (longer than C6) are not suitable for supercritical ORCs due to the thermal stability limitation.

CYANOBACTERIA FOR MITIGATING METHANE EMISSION FROM SUBMERGED PADDY FIELDS

Energy Technology Data Exchange (ETDEWEB)

Upasana Mishra; Shalini Anand [Department of Environmental Studies, Inderprastha Engineering College, Sahibabad, Ghaziabad (India)

2008-09-30

Atmospheric methane, a potent greenhouse gas with high absorption potential for infrared radiation, is responsible for one forth of the total anticipated warming. It is forming a major part of green house gases, next after carbon dioxide. Its concentration has been increasing alarmingly on an average at the rate of one percent per year. Atmospheric methane, originating mainly from biogenic sources such as paddy fields, natural wetlands and landfills, accounts for 15-20% of the world's total anthropogenic methane emission. With intensification of rice cultivation in coming future, methane emissions from paddy fields are anticipated to increase. India's share in world's rice production is next after to China and likewise total methane emission from paddy fields also. Methane oxidation through planktophytes, particularly microalgae which are autotrophic and abundant in rice rhizospheres, hold promise in controlling methane emission from submerged paddy fields. The present study is focused on the role of nitrogen fixing, heterocystous cyanobacteria and Azolla (a water fern harboring a cyanobacterium Anabaena azollae) as biological sink for headspace concentration of methane in flooded soils. In this laboratory study, soil samples containing five potent nitrogen fixer cyanobacterial strains from paddy fields, were examined for their methane reducing potential. Soil sample without cyanobacterial strain was tested and taken as control. Anabaena sp. was found most effective in inhibiting methane concentration by 5-6 folds over the control. Moist soil cores treated with chemical nitrogen, urea, in combination with cyanobacteria mixture, Azolla microphylla or cyanobacteria mixture plus Azolla microphylla exhibited significance reduction in the headspace concentration of methane than the soil cores treated with urea alone. Contrary to other reports, this study also demonstrates that methane oxidation in soil core samples from paddy fields was stimulated by

Distribution of MEG and methanol in well-defined hydrocarbon and water systems: Experimental measurement and modeling using the CPA EoS

DEFF Research Database (Denmark)

Riaz, Muhammad; Yussuf, Mustafe A.; Kontogeorgis, Georgios

2013-01-01

+ water. These data are satisfactorily correlated (binaries) and predicted (ternaries) using Cubic Plus Association (CPA) equation of state (EoS). CPA is also applied to binary LLE of aromatic hydrocarbon + water and VLE of methane + methanol. Finally the distribution of water and inhibitors (methanol...... and MEG) in various phases is modeled using CPA. The hydrocarbon phase consists of mixture-1 (methane, ethane, n-butane) or mixture-2 (methane, ethane, propane, n-butane, n-heptane, toluene and n-decane). CPA can satisfactorily predict the water content in the gas phase of the multicomponent systems...

Predicting hydrocarbon potential of an earth formation underlying a body of water

International Nuclear Information System (INIS)

Kaplan, I.R.; Demaison, G.J.

1983-01-01

A method for the on-site collection and examination of small concentrations of methane dissolved in water so as to predict hydrocarbon potential of an earth formation underlying a body of water, said formation being a source of said methane, comprises: (i) sampling the water; (ii) continuously vacuum separating said water into liquid and gas phases; (iii) quantitatively separating interfering gas species from methane; (iv) quantitatively oxidising said methane; (v) cryogenically trapping the resulting gaseous carbon dioxide and water vapor at a trapping station, and (vi) isotopically examining said trapped carbon dioxide and water vapour for carbon and deuterium distribution. (author)

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

Science.gov (United States)

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

EMG System for Production of Methane From Carbon Dioxide, Phase I

Data.gov (United States)

National Aeronautics and Space Administration — Sustainable Innovations, LLC, is developing an Electrochemical Methane Generator (EMG), which comprises a novel method of converting CO2 and H2O to hydrocarbon fuels...

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

Science.gov (United States)

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.

Field Exploration of Methane Seep Near Atqasuk

Energy Technology Data Exchange (ETDEWEB)

Katey Walter, Dennis Witmer, Gwen Holdmann

2008-12-31

Methane (CH{sub 4}) in natural gas is a major energy source in the U.S., and is used extensively on Alaska's North Slope, including the oilfields in Prudhoe Bay, the community of Barrow, and the National Petroleum Reserve, Alaska (NPRA). Smaller villages, however, are dependent on imported diesel fuel for both power and heating, resulting in some of the highest energy costs in the U.S. and crippling local economies. Numerous CH{sub 4} gas seeps have been observed on wetlands near Atqasuk, Alaska (in the NPRA), and initial measurements have indicated flow rates of 3,000-5,000 ft{sup 3} day{sup -1} (60-100 kg CH{sub 4} day{sup -1}). Gas samples collected in 1996 indicated biogenic origin, although more recent sampling indicated a mixture of biogenic and thermogenic gas. In this study, we (1) quantified the amount of CH{sub 4} generated by several seeps and evaluated their potential use as an unconventional gas source for the village of Atqasuk; (2) collected gas and analyzed its composition from multiple seeps several miles apart to see if the source is the same, or if gas is being generated locally from isolated biogenic sources; and (3) assessed the potential magnitude of natural CH{sub 4} gas seeps for future use in climate change modeling.

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

Energy Technology Data Exchange (ETDEWEB)

Douglas, Peter M. J.; Stolper, Daniel A.; Eiler, John M.; Sessions, Alex L.; Lawson, Michael; Shuai, Yanhua; Bishop, Andrew; Podlaha, Olaf G.; Ferreira, Alexandre A.; Santos Neto, Eugenio V.; Niemann, Martin; Steen, Arne S.; Huang, Ling; Chimiak, Laura; Valentine, David L.; Fiebig, Jens; Luhmann, Andrew J.; Seyfried, William E.; Etiope, Giuseppe; Schoell, Martin; Inskeep, William P.; Moran, James J.; Kitchen, Nami

2017-11-01

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 we 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.

Hydropower's Biogenic Carbon Footprint.

Science.gov (United States)

Scherer, Laura; Pfister, Stephan

2016-01-01

Global warming is accelerating and the world urgently needs a shift to clean and renewable energy. Hydropower is currently the largest renewable source of electricity, but its contribution to climate change mitigation is not yet fully understood. Hydroelectric reservoirs are a source of biogenic greenhouse gases and in individual cases can reach the same emission rates as thermal power plants. Little is known about the severity of their emissions at the global scale. Here we show that the carbon footprint of hydropower is far higher than previously assumed, with a global average of 173 kg CO2 and 2.95 kg CH4 emitted per MWh of electricity produced. This results in a combined average carbon footprint of 273 kg CO2e/MWh when using the global warming potential over a time horizon of 100 years (GWP100). Nonetheless, this is still below that of fossil energy sources without the use of carbon capture and sequestration technologies. We identified the dams most promising for capturing methane for use as alternative energy source. The spread among the ~1500 hydropower plants analysed in this study is large and highlights the importance of case-by-case examinations.

Hydropower's Biogenic Carbon Footprint

Science.gov (United States)

Pfister, Stephan

2016-01-01

Global warming is accelerating and the world urgently needs a shift to clean and renewable energy. Hydropower is currently the largest renewable source of electricity, but its contribution to climate change mitigation is not yet fully understood. Hydroelectric reservoirs are a source of biogenic greenhouse gases and in individual cases can reach the same emission rates as thermal power plants. Little is known about the severity of their emissions at the global scale. Here we show that the carbon footprint of hydropower is far higher than previously assumed, with a global average of 173 kg CO2 and 2.95 kg CH4 emitted per MWh of electricity produced. This results in a combined average carbon footprint of 273 kg CO2e/MWh when using the global warming potential over a time horizon of 100 years (GWP100). Nonetheless, this is still below that of fossil energy sources without the use of carbon capture and sequestration technologies. We identified the dams most promising for capturing methane for use as alternative energy source. The spread among the ~1500 hydropower plants analysed in this study is large and highlights the importance of case-by-case examinations. PMID:27626943

Using biogenic sulfur gases as remotely detectable biosignatures on anoxic planets.

Science.gov (United States)

Domagal-Goldman, Shawn D; Meadows, Victoria S; Claire, Mark W; Kasting, James F

2011-06-01

We used one-dimensional photochemical and radiative transfer models to study the potential of organic sulfur compounds (CS(2), OCS, CH(3)SH, CH(3)SCH(3), and CH(3)S(2)CH(3)) to act as remotely detectable biosignatures in anoxic exoplanetary atmospheres. Concentrations of organic sulfur gases were predicted for various biogenic sulfur fluxes into anoxic atmospheres and were found to increase with decreasing UV fluxes. Dimethyl sulfide (CH(3)SCH(3), or DMS) and dimethyl disulfide (CH(3)S(2)CH(3), or DMDS) concentrations could increase to remotely detectable levels, but only in cases of extremely low UV fluxes, which may occur in the habitable zone of an inactive M dwarf. The most detectable feature of organic sulfur gases is an indirect one that results from an increase in ethane (C(2)H(6)) over that which would be predicted based on the planet's methane (CH(4)) concentration. Thus, a characterization mission could detect these organic sulfur gases-and therefore the life that produces them-if it could sufficiently quantify the ethane and methane in the exoplanet's atmosphere.

Reduced biomass burning emissions reconcile conflicting estimates of the post-2006 atmospheric methane budget.

Science.gov (United States)

Worden, John R; Bloom, A Anthony; Pandey, Sudhanshu; Jiang, Zhe; Worden, Helen M; Walker, Thomas W; Houweling, Sander; Röckmann, Thomas

2017-12-20

Several viable but conflicting explanations have been proposed to explain the recent ~8 p.p.b. per year increase in atmospheric methane after 2006, equivalent to net emissions increase of ~25 Tg CH 4 per year. A concurrent increase in atmospheric ethane implicates a fossil source; a concurrent decrease in the heavy isotope content of methane points toward a biogenic source, while other studies propose a decrease in the chemical sink (OH). Here we show that biomass burning emissions of methane decreased by 3.7 (±1.4) Tg CH 4 per year from the 2001-2007 to the 2008-2014 time periods using satellite measurements of CO and CH 4 , nearly twice the decrease expected from prior estimates. After updating both the total and isotopic budgets for atmospheric methane with these revised biomass burning emissions (and assuming no change to the chemical sink), we find that fossil fuels contribute between 12-19 Tg CH 4 per year to the recent atmospheric methane increase, thus reconciling the isotopic- and ethane-based results.

Preliminary Geospatial Analysis of Arctic Ocean Hydrocarbon Resources

Energy Technology Data Exchange (ETDEWEB)

Long, Philip E.; Wurstner, Signe K.; Sullivan, E. C.; Schaef, Herbert T.; Bradley, Donald J.

2008-10-01

Ice coverage of the Arctic Ocean is predicted to become thinner and to cover less area with time. The combination of more ice-free waters for exploration and navigation, along with increasing demand for hydrocarbons and improvements in technologies for the discovery and exploitation of new hydrocarbon resources have focused attention on the hydrocarbon potential of the Arctic Basin and its margins. The purpose of this document is to 1) summarize results of a review of published hydrocarbon resources in the Arctic, including both conventional oil and gas and methane hydrates and 2) develop a set of digital maps of the hydrocarbon potential of the Arctic Ocean. These maps can be combined with predictions of ice-free areas to enable estimates of the likely regions and sequence of hydrocarbon production development in the Arctic. In this report, conventional oil and gas resources are explicitly linked with potential gas hydrate resources. This has not been attempted previously and is particularly powerful as the likelihood of gas production from marine gas hydrates increases. Available or planned infrastructure, such as pipelines, combined with the geospatial distribution of hydrocarbons is a very strong determinant of the temporal-spatial development of Arctic hydrocarbon resources. Significant unknowns decrease the certainty of predictions for development of hydrocarbon resources. These include: 1) Areas in the Russian Arctic that are poorly mapped, 2) Disputed ownership: primarily the Lomonosov Ridge, 3) Lack of detailed information on gas hydrate distribution, and 4) Technical risk associated with the ability to extract methane gas from gas hydrates. Logistics may control areas of exploration more than hydrocarbon potential. Accessibility, established ownership, and leasing of exploration blocks may trump quality of source rock, reservoir, and size of target. With this in mind, the main areas that are likely to be explored first are the Bering Strait and Chukchi

Hydrogen production by reforming of hydrocarbons and alcohols in a dielectric barrier discharge

Energy Technology Data Exchange (ETDEWEB)

Sarmiento, Belen; Brey, J. Javier; Viera, Inmaculada G. [Hynergreen Technologies, S.A. Avda. de la Buhaira, 2. 41018 Sevilla (Spain); Gonzalez-Elipe, Agustin R.; Cotrino, Jose; Rico, Victor J. [Instituto de Ciencia de los Materiales de Sevilla (CSIC-University Sevilla), Avda. Americo Vespucio, 49, 41092 Sevilla (Spain)

2007-06-10

This work reports about the use of plasmas to obtain hydrogen by reforming of hydrocarbons or alcohols in mixtures with CO{sub 2} or H{sub 2}O. The plasma is activated in a dielectric barrier discharge (DBD) reactor working at atmospheric pressure and low temperatures (i.e., about 100 C). The reactor presents a great versatility in operation and a low manufacturing cost. Results are presented for the reforming of methane, methanol and ethanol. Methane transforms up to a 70% into CO and H{sub 2} without formation of any kind of superior hydrocarbon. For the two alcohols 100% conversion into the same products is found for flows much higher than in the case of methane. The work reports a description of the reactor and the operational conditions of the power supply enabling the ignition of the plasma and its steady state operation. (author)

Advanced oxygen-hydrocarbon Earth-to-orbit propulsion

Science.gov (United States)

Obrien, C. J.

1981-01-01

Liquid oxygen/hydrocarbon (LO2/HC) rocket engine cycles for a surface to orbit transportation system were evaluated. A consistent engine system data base is established for defining advantages and disadvantages, system performance and operating limits, engine parametric data, and technology requirements for candidate engine systems. Preliminary comparisons of the engine cycles utilizing delivered specific impulse values are presented. Methane and propane staged combustion cycles are the highest LO2/HC performers. The hydrogen cooled LO2/methane dual throat engine was found to be the highest performing. Technology needs identified in the study include: high temperature turbines; oxidizer-rich preburners; LO2, methane, and propane cooling; methane and propane fuel-rich preburners; the HC fuel turbopump; and application of advanced composite materials to the engine system. Parametric sensitivity analysis data are displayed which show the effect of variations in engine thrust, mixture ratio, chamber pressure, area ratio, cycle life, and turbine inlet temperature on specific impulse and engine weight.

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

Energy Technology Data Exchange (ETDEWEB)

McCormick, R.L. [Colorado School of Mines, Golden, CO (United States)

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 the 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.

Properties of plasma flames sustained by microwaves and burning hydrocarbon fuels

International Nuclear Information System (INIS)

Hong, Yong Cheol; Uhm, Han Sup

2006-01-01

Plasma flames made of atmospheric microwave plasma and a fuel-burning flame were presented and their properties were investigated experimentally. The plasma flame generator consists of a fuel injector and a plasma flame exit connected in series to a microwave plasma torch. The plasma flames are sustained by injecting hydrocarbon fuels into a microwave plasma torch in air discharge. The microwave plasma torch in the plasma flame system can burn a hydrocarbon fuel by high-temperature plasma and high atomic oxygen density, decomposing the hydrogen and carbon containing fuel. We present the visual observations of the sustained plasma flames and measure the gas temperature using a thermocouple device in terms of the gas-fuel mixture and flow rate. The plasma flame volume of the hydrocarbon fuel burners was more than approximately 30-50 times that of the torch plasma. While the temperature of the torch plasma flame was only 868 K at a measurement point, that of the diesel microwave plasma flame with the addition of 0.019 lpm diesel and 30 lpm oxygen increased drastically to about 2280 K. Preliminary experiments for methane plasma flame were also carried out, measuring the temperature profiles of flames along the radial and axial directions. Finally, we investigated the influence of the microwave plasma on combustion flame by observing and comparing OH molecular spectra for the methane plasma flame and methane flame only

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

Energy Technology Data Exchange (ETDEWEB)

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. We set out to investigate the role that methanotrophs play in such mats at locations where methane reaches the sea floor along with sulfide. Mats were sampled from several seep environments and multiple sets were grown in-situ at a hydrocarbon seep in the Santa Barbara Basin. Mats grown in-situ were returned to the laboratory and used to perform stable isotope probing experiments in which they were treated with 13C-enriched methane. The microbial community was analyzed, demonstrating that three or more microbial groups became enriched in methane?s carbon: methanotrophs that presumably utilize methane directly, methylotrophs that presumably consume methanol excreted by the methanotrophs, and sulfide oxidizers that presumably consume carbon dioxide released by the methanotrophs and methylotrophs. Methanotrophs reached high relative abundance in mats grown on methane, but other bacterial processes include sulfide oxidation appeared to dominate mats, indicating that methanotrophy is not a dominant process in sustaining these benthic mats, but rather a secondary function modulated by methane availability. Methane that escapes the sediment in the deep ocean typically dissolved into the overlying water where it is available to methanotrophic bacteria. We set out to better understand the efficacy of this

Two-step processing of oil shale to linear hydrocarbons

Energy Technology Data Exchange (ETDEWEB)

Eliseev, O.L.; Ryzhov, A.N.; Latypova, D.Zh.; Lapidus, A.L. [Russian Academy of Sciences, Moscow (Russian Federation). N.D. Zelinsky Institute of Organic Chemistry; Avakyan, T.A. [Gubkin Russian State University of Oil and Gas, Moscow (Russian Federation)

2013-11-01

Thermal and catalytic steam reforming of oil shale mined from Leningrad and Kashpir deposits was studied. Experiments were performed in fixed bed reactor by varying temperature and steam flow rate. Data obtained were approximated by empirical formulas containing some parameters calculated by least-squares method. Thus predicting amount of hydrogen, carbon monoxide and methane in producer gas is possible for given particular kind of oil shale, temperature and steam flow rate. Adding Ni catalyst enriches hydrogen and depletes CO content in effluent gas at low gasification temperatures. Modeling gas simulating steam reforming gases (H{sub 2}, CO, CO{sub 2}, and N{sub 2} mixture) was tested in hydrocarbon synthesis over Co-containing supported catalyst. Selectivity of CO conversion into C{sub 5+} hydrocarbons reaches 84% while selectivity to methane is 7%. Molecular weight distribution of synthesized alkanes obeys Anderson-Schulz-Flory equation and chain growth probability 0.84. (orig.)

Interference-free mid-IR laser absorption detection of methane

International Nuclear Information System (INIS)

Pyun, Sung Hyun; Cho, Jungwan; Davidson, David F; Hanson, Ronald K

2011-01-01

A novel, mid-IR scanned-wavelength laser absorption diagnostic was developed for time-resolved, interference-free, absorption measurement of methane concentration. A differential absorption (peak minus valley) scheme was used that takes advantage of the structural differences of the absorption spectrum of methane and other hydrocarbons. A peak and valley wavelength pair was selected to maximize the differential cross-section (σ peak minus valley ) of methane for the maximum signal-to-noise ratio, and to minimize that of the interfering absorbers. Methane cross-sections at the peak and valley wavelengths were measured over a range of temperatures, 1000 to 2000 K, and pressures 1.3 to 5.4 atm. The cross-sections of the interfering absorbers were assumed constant over the small wavelength interval between the methane peak and valley features. Using this diagnostic, methane concentration time histories during n-heptane pyrolysis were measured behind reflected shock waves in a shock tube. The differential absorption scheme efficiently rejected the absorption interference and successfully recovered the vapor-phase methane concentration. These measurements allowed the comparison with methane concentration time-history simulations derived from a current n-heptane reaction mechanism (Sirjean et al 2009 A high-temperature chemical kinetic model of n-alkane oxidation JetSurF version 1.0)

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

Science.gov (United States)

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.

Relationships between water and gas chemistry in mature coalbed methane reservoirs of the Black Warrior Basin

Science.gov (United States)

Pashin, Jack C.; McIntyre-Redden, Marcella R.; Mann, Steven D.; Kopaska-Merkel, David C.; Varonka, Matthew S.; Orem, William H.

2014-01-01

Water and gas chemistry in coalbed methane reservoirs of the Black Warrior Basin reflects a complex interplay among burial processes, basin hydrodynamics, thermogenesis, and late-stage microbial methanogenesis. These factors are all important considerations for developing production and water management strategies. Produced water ranges from nearly potable sodium-bicarbonate water to hypersaline sodium-chloride brine. The hydrodynamic framework of the basin is dominated by structurally controlled fresh-water plumes that formed by meteoric recharge along the southeastern margin of the basin. The produced water contains significant quantities of hydrocarbons and nitrogen compounds, and the produced gas appears to be of mixed thermogenic-biogenic origin.Late-stage microbial methanogenesis began following unroofing of the basin, and stable isotopes in the produced gas and in mineral cements indicate that late-stage methanogenesis occurred along a CO2-reduction metabolic pathway. Hydrocarbons, as well as small amounts of nitrate in the formation water, probably helped nourish the microbial consortia, which were apparently active in fresh to hypersaline water. The produced water contains NH4+ and NH3, which correlate strongly with brine concentration and are interpreted to be derived from silicate minerals. Denitrification reactions may have generated some N2, which is the only major impurity in the coalbed gas. Carbon dioxide is a minor component of the produced gas, but significant quantities are dissolved in the formation water. Degradation of organic compounds, augmented by deionization of NH4+, may have been the principal sources of hydrogen facilitating late-stage CO2 reduction.

Formation of diamonds out of hydrocarbon gas in the earth's mantle

International Nuclear Information System (INIS)

Krason, J.; Szymanski, A.; Savkevitch, S.S.

1991-01-01

This paper discusses the concept of formation of polycrystalline diamonds being discussed dint he context of a very rapid, dynamic decomposition of the hydrocarbon gas, initially biogenic or thermogenic condensed in gas hydrates, naturally locked and highly compressed in the hosting rocks. Gas hydrates are of solid, ice-like composition, mostly of hydrocarbon. Gas hydrates, composed of polyhedral cages, may have two types of structural forms: the body-centered structure or Structure I (small molecules) and diamond lattice or Structure II (large molecules). The crystal structure of the gas hydrate depends on the geometry of gas molecules. The thermodynamic conditions required for stabilization and preservation of the gas hydrates can be changed. Thus, in this concept, the principal source for at least some diamond deposits can originally be highly condensed hydrocarbons. In this case, if all the above indicated thermodynamic conditions and processes are met, naturally precondensed hydrocarbons can be directly converted into polycrystalline, extremely coherent diamonds

Aliphatic and polycyclic aromatic hydrocarbons in Gulf of Trieste sediments (northern Adriatic): potential impacts of maritime traffic.

Science.gov (United States)

Bajt, Oliver

2014-09-01

The Gulf of Trieste (northern Adriatic) is one of the most urbanized and industrialized areas in the northern Adriatic, with intense maritime traffic experienced at multiple ports. The impact of maritime traffic on contamination by hydrocarbons in this area was assessed. Concentrations of hydrocarbons were higher near the expected contamination sources and still elevated in the adjacent offshore areas. Aliphatic hydrocarbons were mainly of petrogenic origin, with some contribution of biogenic origin. A continuous contamination by aliphatic hydrocarbons and degradation processes were hypothesized. Concentrations of total polycyclic aromatic hydrocarbons (PAH) were generally greater near the contamination sources. Compared to the prevailing pyrolytic origin, the petrogenic PAH origin seemed to be less important, but not negligible. Results revealed that intensive maritime traffic is a probable source of contamination by hydrocarbons in the investigated area, which is largely limited to areas near the contamination sources.

Impact of biogenic terpene emissions from Brassica napus on tropospheric ozone over Saxony (Germany): numerical investigation.

Science.gov (United States)

Renner, Eberhard; Münzenberg, Annette

2003-01-01

The role of biogenic emissions in tropospheric ozone production is currently under discussion and major aspects are not well understood yet. This study aims towards the estimation of the influence of biogenic emissions on tropospheric ozone concentrations over Saxony in general and of biogenic emissions from brassica napus in special. MODELLING TOOLS: The studies are performed by utilizing a coupled numerical modelling system consisting of the meteorological model METRAS and the chemistry transport model MUSCAT. For the chemical part, the Euro-RADM algorithm is used. EMISSIONS: Anthropogenic and biogenic emissions are taken into account. The anthropogenic emissions are introduced by an emission inventory. Biogenic emissions, VOC and NO, are calculated within the chemical transport model MUSCAT at each time step and in each grid cell depending on land use type and on the temperature. The emissions of hydrocarbons from forest areas as well as biogenic NO especially from agricultural grounds are considered. Also terpene emissions from brassica napus fields are estimated. SIMULATION SETUP AND METEOROLOGICAL CONDITIONS: The simulations were performed over an area with an extension of 160 x 140 km2 which covers the main parts of Saxony and neighboring areas of Brandenburg, Sachsen-Anhalt and Thuringia. Summer smog with high ozone concentrations can be expected during high pressure conditions on hot summer days. Typical meteorological conditions for such cases were introduced in an conceptual way. It is estimated that biogenic emissions change tropospheric ozone concentrations in a noticeable way (up to 15% to 20%) and, therefore, should not be neglected in studies about tropospheric ozone. Emissions from brassica napus do have a moderate potential to enhance tropospheric ozone concentrations, but emissions are still under consideration and, therefore, results vary to a high degree. Summing up, the effect of brassica napus terpene emissions on ozone concentrations is

Surface geochemical data evaluation and integration with geophysical observations for hydrocarbon prospecting, Tapti graben, Deccan Syneclise, India

Directory of Open Access Journals (Sweden)

T. Satish Kumar

2014-05-01

Full Text Available The Deccan Syneclise is considered to have significant hydrocarbon potential. However, significant hydrocarbon discoveries, particularly for Mesozoic sequences, have not been established through conventional exploration due to the thick basalt cover over Mesozoic sedimentary rocks. In this study, near-surface geochemical data are used to understand the petroleum system and also investigate type of source for hydrocarbons generation of the study area. Soil samples were collected from favorable areas identified by integrated geophysical studies. The compositional and isotopic signatures of adsorbed gaseous hydrocarbons (methane through butane were used as surface indicators of petroleum micro-seepages. An analysis of 75 near-surface soil-gas samples was carried out for light hydrocarbons (C1–C4 and their carbon isotopes from the western part of Tapti graben, Deccan Syneclise, India. The geochemical results reveal sites or clusters of sites containing anomalously high concentrations of light hydrocarbon gases. High concentrations of adsorbed thermogenic methane (C1 = 518 ppb and ethane plus higher hydrocarbons (ΣC2+ = 977 ppb were observed. Statistical analysis shows that samples from 13% of the samples contain anomalously high concentrations of light hydrocarbons in the soil-gas constituents. This seepage suggests largest magnitude of soil gas anomalies might be generated/source from Mesozoic sedimentary rocks, beneath Deccan Traps. The carbon isotopic composition of methane, ethane and propane ranges are from −22.5‰ to −30.2‰ PDB, −18.0‰ to 27.1‰ PDB and 16.9‰–32.1‰ PDB respectively, which are in thermogenic source. Surface soil sample represents the intersection of a migration conduit from the deep subsurface to the surface connected to sub-trappean Mesozoic sedimentary rocks. Prominent hydrocarbon concentrations were associated with dykes, lineaments and presented on thinner basaltic cover in the study area

Conversion of hydrocarbons in solid oxide fuel cells

DEFF Research Database (Denmark)

Mogensen, Mogens Bjerg; Kammer Hansen, K.

2003-01-01

Recently, a number of papers about direct oxidation of methane and hydrocarbon in solid oxide fuel cells (SOFC) at relatively low temperatures (about 700degreesC) have been published. Even though the conversion of almost dry CH4 at 1000degreesC on ceramic anodes was demonstrated more than 10 years...

Catalytic aromatization of methane.

Science.gov (United States)

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.

Methane leakage during the evolution of petroleum systems in the Western Canada Sedimentary Basin and the Central Graben area of the North Sea

Science.gov (United States)

Berbesi, L. A.; di Primio, R.; Anka, Z.; Horsfield, B.

2012-04-01

Around 500 to 600 Tg (1 Tg = 1012 g) of methane enter the atmosphere every year, mainly as product of microbial processes and combustion of fossil fuels and burning biomass. The importance of another source, the geologic emissions of methane, is up to now only loosely constrained. In this study, we addressed the potential methane emissions during the geological evolution of the Western Canada sedimentary basin (WCSB), which holds the largest oil sand accumulations in the world, and the Central Graben area of the North Sea. In the case of the WCSB, thermogenic gas generation and leakage at the sediment surface were addressed through 3D petroleum systems modeling. In this basin, the accumulated oil experienced intense biodegradation that resulted in large masses of biogenic methane. We quantified this latter mass though a two-step mass balance approach. Firstly, we estimated the rate of petroleum degradation and the magnitude of petroleum loss. After this, we calculated the mass of biogenic methane generated using a model that assumes hexadecane (C16H34) as representative of the saturated compounds (Zengler et al., 1999). Our 3D model suggests that 90000-150000 Tg of dry gas (mostly methane) could have leaked during the interval from 80 Ma to 60 Ma. Therefore, uniform leakage rates would have been in the order of 10-3-10-2 Tg yr-1. Biogenic methane generation could have taken place at rates of 10-4 to 10-2 Tg yr-1. However, the effective mass of thermogenic and biogenic methane reaching the atmosphere might have been up to 90% lower than calculated here due to methanotrophic consumption in soils (Etiope and Klusman, 2002). We addressed the thermogenic gas generation and leakage in the Central Graben through two different methods. The first is based on a previous 3D petroleum system modeling of the region (Neumann, 2006). The second consisted of calculating the mass of generated petroleum based on source rock extension and properties (Schmoker, 1994), and then

Spatial structure and activity of sedimentary microbial communities underlying a Beggiatoa spp. mat in a Gulf of Mexico hydrocarbon seep.

Directory of Open Access Journals (Sweden)

Karen G Lloyd

Full Text Available 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 ( approximately 400 cm and approximately 10 cm from the mat's edge contrasted with sharply diminished activity at approximately 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

Impacts of biogenic emissions of VOC and NOx on tropospheric ozone during summertime in eastern China.

Science.gov (United States)

Wang, Qin'geng; Han, Zhiwei; Wang, Tijian; Zhang, Renjian

2008-05-20

This study is intended to understand and quantify the impacts of biogenic emissions of volatile organic compounds (VOC) and nitrogen oxides (NO(x)) on the formation of tropospheric ozone during summertime in eastern China. The model system consists of the non-hydrostatic mesoscale meteorological model (MM5) and a tropospheric chemical and transport model (TCTM) with the updated carbon-bond chemical reaction mechanism (CBM-IV). The spatial resolution of the system domain is 30 km x 30 km. The impacts of biogenic emissions are investigated by performing simulations (36 h) with and without biogenic emissions, while anthropogenic emissions are constant. The results indicate that biogenic emissions have remarkable impacts on surface ozone in eastern China. In big cities and their surrounding areas, surface ozone formation tends to be VOC-limited. The increase in ozone concentration by biogenic VOC is generally 5 ppbv or less, but could be more than 10 ppbv or even 30 ppbv in some local places. The impacts of biogenic NO(x) are different or even contrary in different regions, depending on the relative availability of NO(x) and VOC. The surface ozone concentrations reduced or increased by the biogenic NO(x) could be as much as 10 ppbv or 20 ppbv, respectively. The impacts of biogenic emissions on ozone aloft are generally restricted to the boundary layer and generally more obvious during the daytime than during the nighttime. This study is useful for understanding the role of biogenic emissions and for planning strategies for surface ozone abatement in eastern China. Due to limitations of the emission inventories used and the highly non-linear nature of zone formation, however, some uncertainties remain in the results.

Subduction zone earthquake probably triggered submarine hydrocarbon seepage offshore Pakistan

Science.gov (United States)

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

National Gas Hydrate Program Expedition 01 offshore India; gas hydrate systems as revealed by hydrocarbon gas geochemistry

Science.gov (United States)

Lorenson, Thomas; Collett, Timothy S.

2018-01-01

The National Gas Hydrate Program Expedition 01 (NGHP-01) targeted gas hydrate accumulations offshore of the Indian Peninsula and along the Andaman convergent margin. The primary objectives of coring were to understand the geologic and geochemical controls on the accumulation of methane hydrate and their linkages to underlying petroleum systems. Four areas were investigated: 1) the Kerala-Konkan Basin in the eastern Arabian Sea, 2) the Mahanadi and 3) Krishna-Godavari Basins in the western Bay of Bengal, and 4) the Andaman forearc Basin in the Andaman Sea.Upward flux of methane at three of the four of the sites cored during NGHP-01 is apparent from the presence of seafloor mounds, seismic evidence for upward gas migration, shallow sub-seafloor geochemical evidence of methane oxidation, and near-seafloor gas composition that resembles gas from depth.The Kerala-Konkan Basin well contained only CO2 with no detectable hydrocarbons suggesting there is no gas hydrate system here. Gas and gas hydrate from the Krishna-Godavari Basin is mainly microbial methane with δ13C values ranging from −58.9 to −78.9‰, with small contributions from microbial ethane (−52.1‰) and CO2. Gas from the Mahanadi Basin was mainly methane with lower concentrations of C2-C5 hydrocarbons (C1/C2 ratios typically >1000) and CO2. Carbon isotopic compositions that ranged from −70.7 to −86.6‰ for methane and −62.9 to −63.7‰ for ethane are consistent with a microbial gas source; however deeper cores contained higher molecular weight hydrocarbon gases suggesting a small contribution from a thermogenic gas source. Gas composition in the Andaman Basin was mainly methane with lower concentrations of ethane to isopentane and CO2, C1/C2 ratios were mainly >1000 although deeper samples were exploration and occurs in a forearc basin. Each of these hydrate-bearing systems overlies and is likely supported by the presence and possible migration of gas from deeper gas-prone petroleum

Fluxed of nitrous oxide and methane in a lake border ecosystem in northern Germany

Energy Technology Data Exchange (ETDEWEB)

Rusch, H.; Rembges, D.; Papke, H.; Rennenberg, H. [Fraunhofer Inst. for Atmospheric Environmental Research, Garmisch-Partenkirchen (Germany)

1995-12-31

Methane and nitrous oxide are radiatively active trace gases. This accounts for approximately 20 % of the total anticipated greenhouse effect. The atmospheric mixing ratio of both gases has increased significantly during the last decades at a rate of 0.25 % yr{sup -l} for N{sub 2}O and a rate of 1 % yr{sup -1} for CH{sub 4}. Whether this increase is caused by enhanced biogenic production of both gases or is due to decreased global sinks, has not been definitely elucidated. Soils are an important source of methane and nitrous oxide. Natural wetlands, e.g., have a similar global source strength of methane as rice paddies. On the other hand, well aerated grasslands have been shown to be a sink for atmospheric methane due to methane oxidation. Nitrous oxide is emitted by a wide range of soil types. Its rate of emission is strongly enhanced by nitrogen fertilization. In the present study, fluxes of methane and nitrous oxide were determined in a lake border ecosystem along a toposequence from reed to dry pasture. The aim of this study was to characterize the influence of soil type, land use and season on the flux rates of these greenhouse gases. (author)

Fluxed of nitrous oxide and methane in a lake border ecosystem in northern Germany

Energy Technology Data Exchange (ETDEWEB)

Rusch, H; Rembges, D; Papke, H; Rennenberg, H [Fraunhofer Inst. for Atmospheric Environmental Research, Garmisch-Partenkirchen (Germany)

1996-12-31

Methane and nitrous oxide are radiatively active trace gases. This accounts for approximately 20 % of the total anticipated greenhouse effect. The atmospheric mixing ratio of both gases has increased significantly during the last decades at a rate of 0.25 % yr{sup -l} for N{sub 2}O and a rate of 1 % yr{sup -1} for CH{sub 4}. Whether this increase is caused by enhanced biogenic production of both gases or is due to decreased global sinks, has not been definitely elucidated. Soils are an important source of methane and nitrous oxide. Natural wetlands, e.g., have a similar global source strength of methane as rice paddies. On the other hand, well aerated grasslands have been shown to be a sink for atmospheric methane due to methane oxidation. Nitrous oxide is emitted by a wide range of soil types. Its rate of emission is strongly enhanced by nitrogen fertilization. In the present study, fluxes of methane and nitrous oxide were determined in a lake border ecosystem along a toposequence from reed to dry pasture. The aim of this study was to characterize the influence of soil type, land use and season on the flux rates of these greenhouse gases. (author)

Microbial community structure and soil pH correspond to methane production in Arctic Alaska soils.

Science.gov (United States)

Wagner, Robert; Zona, Donatella; Oechel, Walter; Lipson, David

2017-08-01

While there is no doubt that biogenic methane production in the Arctic is an important aspect of global methane emissions, the relative roles of microbial community characteristics and soil environmental conditions in controlling Arctic methane emissions remains uncertain. Here, relevant methane-cycling microbial groups were investigated at two remote Arctic sites with respect to soil potential methane production (PMP). Percent abundances of methanogens and iron-reducing bacteria correlated with increased PMP, while methanotrophs correlated with decreased PMP. Interestingly, α-diversity of the methanogens was positively correlated with PMP, while β-diversity was unrelated to PMP. The β-diversity of the entire microbial community, however, was related to PMP. Shannon diversity was a better correlate of PMP than Simpson diversity across analyses, while rarefied species richness was a weak correlate of PMP. These results demonstrate the following: first, soil pH and microbial community structure both probably control methane production in Arctic soils. Second, there may be high functional redundancy in the methanogens with regard to methane production. Third, iron-reducing bacteria co-occur with methanogens in Arctic soils, and iron-reduction-mediated effects on methanogenesis may be controlled by α- and β-diversity. And finally, species evenness and rare species abundances may be driving relationships between microbial groups, influencing Arctic methane production. © 2017 Society for Applied Microbiology and John Wiley & Sons Ltd.

The direct aromatization of methane

Energy Technology Data Exchange (ETDEWEB)

Marcelin, G.; Oukaci, R.; Migone, R.A.; Kazi, A.M. [Altamira Instruments, Pittsburgh, PA (United States)

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 as 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.

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

Science.gov (United States)

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.

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

Science.gov (United States)

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.

The origin of the methane in deep aquifers of the Pannonian Basin

International Nuclear Information System (INIS)

Futo, I.; Svingor, E.; Szanto, Zs.

2004-01-01

Complete text of publication follows. Bacterial methanogenesis and thermally induced generation of gaseous and liquid hydrocarbons have long been considered as processes strictly separated in space and time [1]. As the compositional and isotopic analysis of the hydrocarbon gas (HC) became a routinely used technique in petroleum exploration, the beginning of thermal gas generation in relatively cold and immature strata was recognized [2]. The discovery of living bacteria at temperatures as high as 50-55 deg C implied that bacterial methane may be formed at temperatures considerably higher than previously supposed. The great number of water wells penetrating the deep aquifers of the hot Pannonian Basin, which is at the same time a mature petroleum province, offers a unique possibility for studying the spatial and temporal relationships between bacterial methanogenesis and thermal generation of HC gases. H and O isotope ratios of water and H and C isotope ratios of methane as well as the abundances of some major and minor dissolved components were measured in 26 subsurface waters from SE Hungary, produced from late Neogene aquifers within the upper two kilometers in depth [3]. The HC gas content of the great majority of the waters is dominated by isotopically light bacterial methane. The depth of the onset of thermal gas generation varies from 0.7 to 1.2 km but the amount of thermogenic methane leaving the kerogen was not sufficient to overprint the light isotopic signature of the methane in the waters. About two thirds of the waters are characterised by low sulfate content ( 20) and methane δD values less negative than - 260%. They also show a direct relationship between the H isotope ratio of the methane and that of the water. These waters experienced exhaustive bacterial sulfate reduction followed by a relatively shallow bacterial methanogenesis. The methanogens started to operate immediately after the sulfate content dropped below 0.1 mmol/l due to bacterial

Emission of Biogenic Volatile Organic Compounds in the Arctic

DEFF Research Database (Denmark)

Lindwall, Frida

, emitted in order to communicate within and between trophic levels and as protection against biotic and abiotic stresses, or as byproducts. Some BVOCs are very reactive, and when entering the atmosphere they rapidly react with for example hydroxyl radicals and ozone, affecting the oxidative capacity......Emissions of biogenic volatile organic compounds (BVOCs) from arctic ecosystems are scarcely studied and the effect of climate change on BVOC emissions even less so. BVOCs are emitted from all living organisms and play a role for atmospheric chemistry. The major part of BVOCs derives from plants...... in the atmosphere. This may warm the climate due to a prolonged lifetime of the potent greenhouse gas methane in the atmosphere. However, oxidized BVOCs may participate in formation or growth of aerosols, which in turn may mitigate climate warming. Climate change in the Arctic, an area characterized by short...

Improved processes of light hydrocarbon separation from LNG with its cryogenic energy utilized

International Nuclear Information System (INIS)

Gao Ting; Lin Wensheng; Gu Anzhong

2011-01-01

Research highlights: → We propose two new light hydrocarbon separation processes utilizing LNG cold energy. → Both processes produce liquefied ethane and LPG with high ethane recovery rate. → CH 4 -riched gas from the high pressure process is compressed to final pressure. → Re-liquefied CH 4 -riched gas from the low pressure one is pumped to final pressure. → Both processes have good performance; the low pressure one is economically better. -- Abstract: Liquefied natural gas (LNG) often consists of some kinds of light hydrocarbons other than methane, such as ethane, propane and butane, which are of high additional value. By efficiently utilization of LNG cryogenic energy, these light hydrocarbons (C 2 + ) can be separated from LNG with low power consumption and LNG is gasified meanwhile. Two novel light hydrocarbon separation processes are proposed in this paper. The first process uses a demethanizer working at higher pressure (about 4.5 MPa). The methane-riched natural gas from the demethanizer can be compressed to pipeline pressure with low power consumption. The other one uses a demethanizer working at lower pressure (about 2.4 MPa). By cascade utilization of LNG cryogenic energy, the methane-riched natural gas from the demethanizer is entirely re-liquefied. Then the liquid product is pressurized to pipeline pressure by pumps instead of compressors, reducing the power consumption greatly. By both of the two processes, liquefied ethane and LPG (liquefied petroleum gas, i.e. C 3 + ) at atmosphere pressure can be obtained directly, and high ethane recovery rate can be gained. On the basis of one typical feed gas composition, the effects of the ethane content and the ethane price to the economics of the light hydrocarbon separation plants are studied, and the economics are compared for these two processes. The results show that recovering light hydrocarbons from LNG can gain great profits by both of the two processes, and from the view of economics, the

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

Science.gov (United States)

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.

Mapping urban pipeline leaks: Methane leaks across Boston

International Nuclear Information System (INIS)

Phillips, Nathan G.; Ackley, Robert; Crosson, Eric R.; Down, Adrian; Hutyra, Lucy R.; Brondfield, Max; Karr, Jonathan D.; Zhao Kaiguang; Jackson, Robert B.

2013-01-01

Natural gas is the largest source of anthropogenic emissions of methane (CH 4 ) in the United States. To assess pipeline emissions across a major city, we mapped CH 4 leaks across all 785 road miles in the city of Boston using a cavity-ring-down mobile CH 4 analyzer. We identified 3356 CH 4 leaks with concentrations exceeding up to 15 times the global background level. Separately, we measured δ 13 CH 4 isotopic signatures from a subset of these leaks. The δ 13 CH 4 signatures (mean = −42.8‰ ± 1.3‰ s.e.; n = 32) strongly indicate a fossil fuel source rather than a biogenic source for most of the leaks; natural gas sampled across the city had average δ 13 CH 4 values of −36.8‰ (±0.7‰ s.e., n = 10), whereas CH 4 collected from landfill sites, wetlands, and sewer systems had δ 13 CH 4 signatures ∼20‰ lighter (μ = −57.8‰, ±1.6‰ s.e., n = 8). Repairing leaky natural gas distribution systems will reduce greenhouse gas emissions, increase consumer health and safety, and save money. Highlights: ► We mapped 3356 methane leaks in Boston. ► Methane leaks in Boston carry an isotopic signature of pipeline natural gas. ► Replacing failing gas pipelines will provide safety, environmental, and economic benefits. - We identified 3356 methane leaks in Boston, with isotopic characteristics consistent with pipeline natural gas.

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

Science.gov (United States)

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.

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

Science.gov (United States)

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.

Methane production from coal by a single methanogen

Science.gov (United States)

Sakata, S.; Mayumi, D.; Mochimaru, H.; Tamaki, H.; Yamamoto, K.; Yoshioka, H.; Suzuki, Y.; Kamagata, Y.

2017-12-01

Previous geochemical studies indicate that biogenic methane greatly contributes to the formation of coalbed methane (CBM). It is unclear, however, what part of coal is used for the methane production and what types of microbes mediate the process. Here we hypothesized that methylotrophic methanogens use methoxylated aromatic compounds (MACs) derived from lignin. We incubated 11 species of methanogens belonging to order Methanosarcinales with 7 types of MACs. Two strains of methanogens, i.e., Methermicoccus shengliensis AmaM and ZC-1, produced methane from the MACs. In fact, these methanogens used over 30 types of commercially available MACs in addition to methanol and methylamines. To date, it is widely believed that methanogens use very limited number of small compounds such as hydrogen plus carbon dioxide, acetate, and methanol, and only three methanogenic pathways are recognized accordingly. Here, in contrast, two Methermicoccus strains used many types of MACs. We therefore propose this "methoxydotrophic" process as the fourth methanogenic pathway. Incubation of AmaM with 2-methoxybenzoate resulted in methanogenesis associated with the stoichiometric production of 2-hydroxybenzoate. Incubation with 2-methoxy-[7-13C] benzoate and with [13C] bicarbonate indicated that two thirds of methane carbon derived from the methoxy group and one third from CO2. Furthermore, incubation with [2-13C] acetate resulted in significant increases of 13C in both methane and CO2. These results suggest the occurrence of O-demethylation, CO2 reduction and acetyl-CoA metabolism in the methoxydotrophic methanogenesis. Furthermore, incubation of AmaM with lignite, subbituminous or bituminous coals in the bicarbonate-buffered media revealed that AmaM produced methane directly from coals via the methoxydotrophic pathway. Although 4 types of MACs were detected in the coal media in addition to methanol and methylamines, their total concentrations were too low to account for the methane

Qualitative and quantitative analysis of light hydrocarbons produced by radiation degradation of N, N-dimethyl hydroxylamine

International Nuclear Information System (INIS)

Wang Jinhua; Bao Borong; Wu Minghong; Sun Xilian; Zhang Xianye; Hu Jingxin; Ye Guoan

2004-01-01

This paper reports the qualitative and quantitative analysis of light hydrocarbons produced by radiation degradation of N, N-dimethyl hydroxylamine. These analyses were performed on the gas chromatograph, in which porous layer open tubular column coated with aluminum oxide and flame-ionization detector are used. For the doses between 10 and 1000 kGy, the light hydrocarbons produced by radiation degradation of N,N-dimethyl hydroxylamine are methane, ethane, ethene, propane, propene and n-butane. When the concentration of N,N-dimethyl hydroxylamine is 0.2 mol/L, the volume fraction of methane is (9.996-247.5) x 10 -6 , the volume fraction of ethane, propane and n-butane is lower and that of ethene and propene is much lower. With the increase of dose the volume fraction of methane is increased but the volume fraction of ethane, ethene, propane, propene and n-butane is not obviously changed. (authors)

Natural Gas Seepage Along the Edge of the Aquitaine Shelf (France): Origin and Flux Measurements

Science.gov (United States)

Ruffine, L.; Donval, J. P.; Battani, A.; Bignon, L.; Croguennec, C.; Caprais, J. C.; Birot, D.; Bayon, G.; Lantéri, N.; Levaché, D.; Dupré, S.

2014-12-01

A newly discovered and highly active seepage area has been acoustically mapped at the western edge of the Aquitaine Shelf in the Bay of Biscay [Dupré et al., 2014]. Three selected seeping sites have been investigated with a Remotely Operated Vehicle. All sites were characterized by vigorous gas emissions, and the occurrence of massive carbonate crusts and bacterial mats at the seafloor. Nine seeps have been sampled with the PEGAZ sampler. The latter allowed gas-bubble sampling and preservation at in situpressure, together with gas-flux measurement through its graduated transparent cone. The C2+ fraction of the gas samples accounts for less than 0.06 %-mol of the total composition. Both the abundance of methane and dD and d13C isotopic analyses of the hydrocarbons indicate a biogenic source generated by microbial reduction of carbon dioxide [Whiticar et al., 1986]. The analyses of the associated noble gases also provide further support for a shallow-depth generation. While sharing the same origin, the collected samples are different in other respects, such as the measured d13C values for carbon dioxide and the hydrocarbons. This is the case in particular for methane, with displays values in between -66.1 and -72.7 ‰. We hypothesized that such variations are the result of multiple gas-transport processes along with the occurrence of hydrocarbon oxidation at different rates within the sedimentary column. The measured gas fluxes are extremely heterogeneous from one seep to another, ranging from 18 to 193 m3.yr-1. These values will be discussed in detail by comparing them with values obtained from different measurement techniques at other gas-seeping sites. The GAZCOGNE study is co-funded by TOTAL and IFREMER as part of the PAMELA (Passive Margin Exploration Laboratories) scientific project. References:Dupré, S., L. Berger, N. Le Bouffant, C. Scalabrin, and J. F. Bourillet (2014), Fluid emissions at the Aquitaine Shelf (Bay of Biscay, France): a biogenic origin or

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

Science.gov (United States)

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.

Science.gov (United States)

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.

Gas hydrates: entrance to a methane age or climate threat?

International Nuclear Information System (INIS)

Krey, Volker; Nakicenovic, Nebojsa; Grubler, Arnulf; O'Neill, Brian; Riahi, Keywan; Canadell, Josep G; Abe, Yuichi; Andruleit, Harald; Archer, David; Hamilton, Neil T M; Johnson, Arthur; Kostov, Veselin; Lamarque, Jean-Francois; Langhorne, Nicholas; Nisbet, Euan G; Riedel, Michael; Wang Weihua; Yakushev, Vladimir

2009-01-01

Methane hydrates, ice-like compounds in which methane is held in crystalline cages formed by water molecules, are widespread in areas of permafrost such as the Arctic and in sediments on the continental margins. They are a potentially vast fossil fuel energy source but, at the same time, could be destabilized by changing pressure-temperature conditions due to climate change, potentially leading to strong positive carbon-climate feedbacks. To enhance our understanding of both the vulnerability of and the opportunity provided by methane hydrates, it is necessary (i) to conduct basic research that improves the highly uncertain estimates of hydrate occurrences and their response to changing environmental conditions, and (ii) to integrate the agendas of energy security and climate change which can provide an opportunity for methane hydrates-in particular if combined with carbon capture and storage-to be used as a 'bridge fuel' between carbon-intensive fossil energies and zero-emission energies. Taken one step further, exploitation of dissociating methane hydrates could even mitigate against escape of methane to the atmosphere. Despite these opportunities, so far, methane hydrates have been largely absent from energy and climate discussions, including global hydrocarbon assessments and the Fourth Assessment Report of the Intergovernmental Panel on Climate Change.

Evaluation of Biogenic Amines in Organic and Non-Organic Wines by HPLC OPA Derivatization

Directory of Open Access Journals (Sweden)

Ali Üren

2007-01-01

Full Text Available Organic and non-organic wines, selected on the basis of consumers’ preference towards healthy products, were produced from the grapes of Vitis vinifera varieties Semillon, Colombard, Cabernet Sauvignon, Merlot and Carignan and possible effects of different wine making techniques were considered. Concentrations of histamine, tyramine, putrescine, cadaverine, ethylamine, methylamine, tryptamine, agmatine and β-phenylethylamine were quantified by HPLC fluorescence detection of o-phthaldialdehyde (OPA derivatives. The order of analyzed parameters in all wines from the highest to the lowest quantities was determined as follows: putrescine > histamine > ethylamine > methylamine > agmatine > tyramine > cadaverine > tryptamine. One of the analyzed compounds (β-phenylethylamine was not detected. The highest average values for organic and non-organic wines were found as follows (in mg/L: putrescine 5.55, ethylamine 0.825 and histamine 0.628 in organic wines, and putrescine 3.68, histamine 1.14 and agmatine 0.662 in non-organic wines. Considering the wine type (organic/non-organic, an important difference was determined for putrescine. Putrescine content in organic wines was significantly greater than in non-organic ones (p=0.008. Evaluating colour of wines (white/red, a statistically significant difference was obtained for methylamine (p=0.028. Taking into account only grape varieties, statistically significant differences were found for histamine, methylamine, tyramine and cadaverine (p<0.05. The results of principal component analysis demonstrated close relations between the following biogenic amines and wines: agmatine and non-organic Colombard; tryptamine or cadaverine and both organic and non-organic Cabernet Sauvignon wines.

Methane synthesis under mild conditions for decentralized applications; Methansynthese unter milden Bedingungen fuer dezentrale Anwendungen

Energy Technology Data Exchange (ETDEWEB)

Schlueter, Michael [DBFZ Deutsches Biomasseforschungszentrum gGmbH, Leipzig (Germany); Roensch, Stefan

2016-08-01

It is a central aim of the German government to significantly reduce the emission of greenhouse gases in the next years. One possibility to reach this aim is the substitution of fossil fuels, especially natural gas, by fuels from biogenic sources (Bio-SNG). However, it is a drawback of Bio-SNG that the production costs are considerably higher than those of fossil natural gas. This work provides an approach to reduce the production costs of Bio-SNG. It is the aim to reduce the process parameters of the methane synthesis. At the same time, it has to be ensured that high methane yields are achieved even at those mild conditions. A procedure for the optimization of the methanation catalyst activity will be presented. If the catalyst is as active as possible even at mild conditions, it will be possible to produce Bio-SNG cost efficient even in small, decentralized scale.

Can introduction of hydraulic fracturing fluids induce biogenic methanogenesis in the shale reservoirs?

Science.gov (United States)

Sharma, S.; Wilson, T.; Wrighton, K. C.; Borton, M.; O'Banion, B.

2017-12-01

The hydraulic fracturing fluids (HFF) injected into the shale formation are composed primarily of water, proppant and some chemical additives ( 0.5- 2% by volume). The additives contain a lot of organic and inorganic compounds like ammonium sulfate, guar gum, boric acid, hydrochloric acid, citric acid, potassium carbonate, glutaraldehyde, ethylene glycols which serve as friction reducers, gelling agents, crosslinkers, biocides, corrosion/scale inhibitors, etc. The water and additives introduced into the formation ensue a variety of microbiogechmical reactions in the reservoir. For this study produced, water and gas samples were collected from several old and new Marcellus wells in SE Pennsylvania and NE West Virginia to better understand these microbe-water-rock interactions. The carbon isotopic composition of dissolved inorganic carbon (δ13CDIC) in the produced fluids and CO2 in produced gas (δ13CCO2) are highly enriched with values > +10‰ and +14 ‰ V-PDB respectively. The injected hydraulic fracturing fluid had low δ13CDIC values of detectable carbon in them. The drilling mud and carbonate veins had δ13C values of -1.8 and < 2.0 ‰ V-PDB respectively. Therefore, the high δ13CDIC signatures in produced water are possibly due to the microbial utilization of lighter carbon (12C) by microbes or methanogenic bacteria in the reservoir. It is possible that introduction of C containing nutrients like guar, methanol, methylamines, etc. stimulates certain methanogen species in the reservoir to produce biogenic methane. Genomic analysis reveals that methanogen species like Methanohalophilus or Methanolobus could be the possible sources of biogenic methane in these shale reservoirs. The evidence of microbial methanogenesis raises the possibility of enhanced gas recovery from these shales using biological amendments.

Kinetics of biological methane oxidation in the presence of non-methane organic compounds in landfill bio-covers

International Nuclear Information System (INIS)

Albanna, Muna; Warith, Mostafa; Fernandes, Leta

2010-01-01

In this experimental program, the effects of non-methane organic compounds (NMOCs) on the biological methane (CH 4 ) oxidation process were examined. The investigation was performed on compost experiments incubated with CH 4 and selected NMOCs under different environmental conditions. The selected NMOCs had different concentrations and their effects were tested as single compounds and mixtures of compounds. The results from all experimental sets showed a decrease in CH 4 oxidation capacity of the landfill bio-cover with the increase in NMOCs concentrations. For example, in the experiment using compost with 100% moisture content at 35 deg. C without any NMOCs the V max value was 35.0 μg CH 4 h -1 g wetwt -1 . This value was reduced to 19.1 μg CH 4 h -1 g wetwt -1 when mixed NMOCs were present in the batch reactors under the same environmental conditions. The experimental oxidation rates of CH 4 in the presence of single and mixed NMOCs were modeled using the uncompetitive inhibition model and kinetic parameters, including the dissociation constants, were obtained. Additionally, the degradation rates of the NMOCs and co-metabolic abilities of methanotrophic bacteria were estimated.

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

Science.gov (United States)

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.

Emissions of Volatile Organic Compounds from Oil and Gas Operations in Northeastern Oklahoma - Wintertime Ambient Air Studies from Three Consecutive Years

Science.gov (United States)

Ghosh, B.

2017-12-01

Volatile organic compounds (VOCs) are emitted into the atmosphere from a variety of sources including oil and gas (O&G) operations, vehicle exhausts, industrial processes, and biogenic sources. Understanding of emission sources and their air quality impact is crucial for effective environmental policymaking and its implementation. Three consecutive wintertime campaigns to study ambient air were conducted in Northeastern Oklahoma during February-March of 2015, 2016, and 2017. The goals of these campaigns were to study ambient VOCs in the region, estimate their air quality impact, and understand how the impact changes over a span of three years. This presentation highlights results from the 2017 campaign. In-situ measurements of methane, ethane, and CO were conducted by an Aerodyne Dual QCL Analyzer while ozone and NOx were measured using Teledyne monitors. In addition, 392 whole air samples were collected and non-methane hydrocarbons (NMHCs) in the samples were analyzed using GC-MS (Agilent). High levels of methane (> 8 ppm) were observed during the study. Correlation with ethane indicated that methane primarily originated from O&G operations with little biogenic contributions. Among NMHCs, C2-C5 alkanes were the most dominant with mean mixing ratios ranging from 0.9 to 6.8 ppb. Chemical tracers (propane, ethyne, CO) and isomeric ratios (iC5/nC5, Figure 1) identified oil and gas activity as the primary source of NMHCs. Photochemical age was calculated to estimate emission source composition. Ozone showed strong diurnal variation characteristic of photochemical production with a maximum mixing ratio of 58 ppb. The results from the 2017 study will be compared with results from studies in 20151 and 20162 and their significance on local air quality will be discussed. References Ghosh, B.; Volatile Organic Compound Emissions from Oil and Gas Production Sources: A Pilot Study in Northeastern Oklahoma; Poster presentation at AGU Fall Meeting; 2015; A11M-0249; (Link) Ghosh

Conversion of methane to hydrogen by a pulsed plasma reactor

International Nuclear Information System (INIS)

Ghorbanzadeh, A. M.; Matin, N.; Parandvar, M. R.; Rasouli, C.; Mazouchi, A. M.

2003-01-01

A pulsed atmospheric glow discharge, employing corona as a preionization, was used to convert methane to hydrogen and higher hydrocarbons. The experimental results showed that the overall conversion and specific energy, defined as energy needed to dissociate one mole methane, was mainly dependent on E/P, banking capacitance, repetition rate and flow rate. The dependence on E/P, especially, is more pronounced. The minimum specific energy was less than 1 MJ and it is expected that it could be further lowered by choosing higher E/P, lower banking capacitance and introducing an oxidizer to enhance the conversion efficiency

C2-C10 hydrocarbon emissions from a boreal wetland and forest floor

Directory of Open Access Journals (Sweden)

H. Hellén

2006-01-01

Full Text Available Emissions of various C2-C10 hydrocarbons (VOCs and halogenated hydrocarbons (VHOCs from a boreal wetland and a Scots pine forest floor in south-western Finland were measured by the static chamber technique. Isoprene was the main non-methane hydrocarbon emitted by the wetland, but small emissions of ethene, propane, propene, 1-butene, 2-methylpropene, butane, pentane and hexane were also detected. The isoprene emission from the wetland was observed to follow the commonly-used isoprene emission algorithm. The mean emission potential of isoprene was 224 µg m-2 h-1 for the whole season. This is lower than the emission potentials published earlier; that is probably at least partly due to the cold and cloudy weather during the measurements. No emissions were detected of monoterpenes or halogenated hydrocarbons from the wetland. The highest hydrocarbon emissions from the Scots pine forest floor were measured in spring and autumn. However, only a few measurements were conducted during summer. The main compounds emitted were monoterpenes. Isoprene emissions were negligible. The total monoterpene emission rates varied from zero to 373 µg m-2 h-1. The results indicated that decaying plant litter may be the source for these emissions. Small emissions of chloroform (100-800 ng m-2 h-1, ethene, propane, propene, 2-methylpropene, cis-2-butene, pentane, hexane and heptane were detected. Comparison with Scots pine emissions showed that the forest floor may be an important monoterpene source, especially in spring.

Conversion of Crude Oil to Methane by a Microbial Consortium Enriched From Oil Reservoir Production Waters

Directory of Open Access Journals (Sweden)

Carolina eBerdugo-Clavijo

2014-05-01

Full Text Available 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 gene (assA 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 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 versus sessile within a subsurface crude oil reservoir.

Characterization of light gaseous hydrocarbons of the surface soils of Krishna-Godavari basin, India.

Science.gov (United States)

Lakshmi, M; Rasheed, M A; Madhavi, T; Kalpana, M S; Patil, D J; Dayal, A M

2012-01-01

Several techniques are used for the exploration of hydrocarbons, of which; the geochemical techniques involving the microbiological technique use the principle of detecting the light hydrocarbon seepage activities for indication of sub-surface petroleum accumulations. Asurvey was carried out to characterize the light gaseous hydrocarbons seeping in oil and gas fields of Krishna-Godavari basin ofAndhra Pradesh. Aset of 50 sub-soil samples were collected at depths of about 3 m for geochemical analyses and 1m for microbiological analysis. The microbial prospecting studies showed the presence of high bacterial population for methane 2.5 x 10(2) to 6.0 x 10(6) cfu g(-1), propane 1x10(2) to 8.0 x 10(6) cfu g(-1) in soil samples. The adsorbed soil gas analysis showed the presence of moderate to low concentrations of methane (26 to 139 ppb), ethane (0 to 17 ppb), propane (0 to 8 ppb), butane (0 to 5 ppb) and pentane (0 to 2 ppb) in the soil samples of the study area. Carbon isotope analysis for methane ('13C1) ranging from -36.6 to -22.7 per hundred Pee Dee Belemnite (PDB) suggests these gases are of thermogenic origin. Geo-microbial prospecting method coupled with adsorbed soil gas and carbon isotope ratio analysis have thus shown good correlation with existing oil/gas fields of Krishna-Godavari basin.

Response of the Black Sea methane budget to massive short-term submarine inputs of methane

DEFF Research Database (Denmark)

Schmale, O.; Haeckel, M.; McGinnis, D. F.

2011-01-01

A steady state box model was developed to estimate the methane input into the Black Sea water column at various water depths. Our model results reveal a total input of methane of 4.7 Tg yr(-1). The model predicts that the input of methane is largest at water depths between 600 and 700 m (7......% of the total input), suggesting that the dissociation of methane gas hydrates at water depths equivalent to their upper stability limit may represent an important source of methane into the water column. In addition we discuss the effects of massive short-term methane inputs (e. g. through eruptions of deep......-water mud volcanoes or submarine landslides at intermediate water depths) on the water column methane distribution and the resulting methane emission to the atmosphere. Our non-steady state simulations predict that these inputs will be effectively buffered by intense microbial methane consumption...

Constraining gas hydrate occurrence in the northern Gulf of Mexico continental slope : fine scale analysis of grain-size in hydrate-bearing sediments

Energy Technology Data Exchange (ETDEWEB)

Hangsterfer, A.; Driscoll, N.; Kastner, M. [Scripps Inst. of Oceanography, La Jolla, CA (United States). Geosciences Research Division

2008-07-01

Methane hydrates can form within the gas hydrate stability zone (GHSZ) in sea beds. The Gulf of Mexico (GOM) contains an underlying petroleum system and deeply buried, yet dynamic salt deposits. Salt tectonics and fluid expulsion upward through the sediment column result in the formation of fractures, through which high salinity brines migrate into the GHSZ, destabilizing gas hydrates. Thermogenic and biogenic hydrocarbons also migrate to the seafloor along the GOMs northern slope, originating from the thermal and biogenic degradation of organic matter. Gas hydrate occurrence can be controlled by either primary permeability, forming in coarse-grained sediment layers, or by secondary permeability, forming in areas where hydrofracture and faulting generate conduits through which hydrocarbon-saturated fluids flow. This paper presented a study that attempted to determine the relationship between grain-size, permeability, and gas hydrate distribution. Grain-size analyses were performed on cores taken from Keathley Canyon and Atwater Valley in the GOM, on sections of cores that both contained and lacked gas hydrate. Using thermal anomalies as proxies for the occurrence of methane hydrate within the cores, samples of sediment were taken and the grain-size distributions were measured to see if there was a correlation between gas hydrate distribution and grain-size. The paper described the methods, including determination of hydrate occurrence and core analysis. It was concluded that gas hydrate occurrence in Keathley Canyon and Atwater Valley was constrained by secondary permeability and was structurally controlled by hydrofractures and faulting that acted as conduits through which methane-rich fluids flowed. 11 refs., 2 tabs., 5 figs.

The genetic source and timing of hydrocarbon formation in gas hydrate reservoirs in Green Canyon, Block GC955

Science.gov (United States)

Moore, M. T.; Darrah, T.; Cook, A.; Sawyer, D.; Phillips, S.; Whyte, C. J.; Lary, B. A.

2017-12-01

Although large volumes of gas hydrates are known to exist along continental slopes and below permafrost, their role in the energy sector and the global carbon cycle remains uncertain. Investigations regarding the genetic source(s) (i.e., biogenic, thermogenic, mixed sources of hydrocarbon gases), the location of hydrocarbon generation, (whether hydrocarbons formed within the current reservoir formations or underwent migration), rates of clathrate formation, and the timing of natural gas formation/accumulation within clathrates are vital to evaluate economic potential and enhance our understanding of geologic processes. Previous studies addressed some of these questions through analysis of conventional hydrocarbon molecular (C1/C2+) and stable isotopic (e.g., δ13C-CH4, δ2H-CH4, δ13C-CO2) composition of gases, water chemistry and isotopes (e.g., major and trace elements, δ2H-H2O, δ18O-H2O), and dissolved inorganic carbon (δ13C-DIC) of natural gas hydrate systems to determine proportions of biogenic and thermogenic gas. However, the effects from contributions of mixing, transport/migration, methanogenesis, and oxidation in the subsurface can complicate the first-order application of these techniques. Because the original noble gas composition of a fluid is preserved independent of microbial activity, chemical reactions, or changes in oxygen fugacity, the integration of noble gas data can provide both a geochemical fingerprint for sources of fluids and an additional insight as to the uncertainty between effects of mixing versus post-genetic modification. Here, we integrate inert noble gases (He, Ne, Ar, and associated isotopes) with these conventional approaches to better constrain the source of gas hydrate formation and the residence time of fluids (porewaters and natural gases) using radiogenic 4He ingrowth techniques in cores from two boreholes collected as part of the University of Texas led UT-GOM2-01 drilling project. Pressurized cores were extracted from

Framework for Assessing Biogenic CO2 Emissions from ...

Science.gov (United States)

This revision of the 2011 report, Accounting Framework for Biogenic CO2 Emissions from Stationary Sources, evaluates biogenic CO2 emissions from stationary sources, including a detailed study of the scientific and technical issues associated with assessing biogenic carbon dioxide emissions from stationary sources. EPA developed the revised report, Framework for Assessing Biogenic CO2 Emissions from Stationary Sources, to present a methodological framework for assessing the extent to which the production, processing, and use of biogenic material at stationary sources for energy production results in a net atmospheric contribution of biogenic CO2 emissions. Biogenic carbon dioxide emissions are defined as CO2 emissions related to the natural carbon cycle, as well as those resulting from the production, harvest, combustion, digestion, decomposition, and processing of biologically-based materials. The EPA is continuing to refine its technical assessment of biogenic CO2 emissions through another round of targeted peer review of the revised study with the EPA Science Advisory Board (SAB). This study was submitted to the SAB's Biogenic Carbon Emissions Panel in February 2015. http://yosemite.epa.gov/sab/sabproduct.nsf/0/3235dac747c16fe985257da90053f252!OpenDocument&TableRow=2.2#2 The revised report will inform efforts by policymakers, academics, and other stakeholders to evaluate the technical aspects related to assessments of biogenic feedstocks used for energy at s

Methane oxidation over noble metal catalysts as related to controlling natural gas vehicle exhaust emissions

International Nuclear Information System (INIS)

Oh, S.H.; Mitchell, P.J.; Siewert, R.M.

1992-01-01

Natural gas has considerable potential as an alternative automotive fuel. This paper reports on methane, the principal hydrocarbon species in natural-gas engine exhaust, which has extremely low photochemical reactivity but is a powerful greenhouse gas. Therefore, exhaust emissions of unburned methane from natural-gas vehicles are of particular concern. This laboratory reactor study evaluates noble metal catalysts for their potential in the catalytic removal of methane from natural-gas vehicle exhaust. Temperature run-up experiments show that the methane oxidation activity decreases in the order Pd/Al 2 O 3 > Rh/Al 2 O 3 > Pt/Al 2 O 3 . Also, for all the noble metal catalysts studied, methane conversion can be maximized by controlling the O 2 concentration of the feedstream at a point somewhat rich (reducing) of stoichiometry

Conditions allowing the formation of biogenic amines in cheese

NARCIS (Netherlands)

Joosten, H.M.L.J.

1988-01-01

A study was undertaken to reveal the conditions that allow the formation of biogenic amines in cheese.

The starters most commonly used in the Dutch cheese industry do not have decarboxylative properties. Only if the milk or curd is contaminated with non-starter bacteria, amine

Biochemical methane potential and anaerobic biodegradability of non-herbaceous and herbaceous phytomass in biogas production

DEFF Research Database (Denmark)

Triolo, Jin Mi; Pedersen, Lene; Qu, Haiyan

2012-01-01

The suitability of municipal plant waste for anaerobic digestion was examined using 57 different herbaceous and non-herbaceous samples. Biochemical methane potential (BMP) and anaerobic biodegradability were related to the degree of lignification and crystallinity of cellulose. The BMP of herbace...

Process, including PSA and membrane separation, for separating hydrogen from hydrocarbons

Science.gov (United States)

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

2001-01-01

An improved process for separating hydrogen from hydrocarbons. The process includes a pressure swing adsorption step, a compression/cooling step and a membrane separation step. The membrane step relies on achieving a methane/hydrogen selectivity of at least about 2.5 under the conditions of the process.

Methane Occurrence in a Drinking Water Aquifer Before and During Natural Gas Production from the Marcellus Shale

Science.gov (United States)

Saiers, J. E.; Barth-Naftilan, E.

2017-12-01

More than 4,000 thousand wells have punctured aquifers of Pennsylvania's northern tier to siphon natural gas from the underlying Marcellus Shale. As drilling and hydraulic fracturing ramped up a decade ago, homeowner reports of well water contamination by methane and other contaminants began to emerge. Although made infrequently compared to the number of gas wells drilled, these reports were troubling and motivated our two-year, prospective study of groundwater quality within the Marcellus Shale Play. We installed multi-level sampling wells within a bedrock aquifer of a 25 km2 area that was targeted for shale gas development. These wells were sampled on a monthly basis before, during, and after seven shale gas wells were drilled, hydraulically fractured, and placed into production. The groundwater samples, together with surface water samples collected from nearby streams, were analyzed for hydrocarbons, trace metals, major ions, and the isotopic compositions of methane, ethane, water, strontium, and dissolved inorganic carbon. With regard to methane in particular, concentrations ranged from under 0.1 to over 60 mg/L, generally increased with aquifer depth, and, at some sites, exhibited considerable temporal variability. The isotopic composition of methane and hydrocarbon ratios also spanned a large range, suggesting that methane origins are diverse and, notably, shift on the time scale of this study. We will present inferences on factors governing methane occurrence across our study area by interpreting time-series data on methane concentrations and isotopic composition in context of local hydrologic variation, companion measurements of groundwater chemistry, and the known timing of key stages of natural gas extraction.

Using Biogenic Sulfur Gases as Remotely Detectable Biosignatures on Anoxic Planets

Science.gov (United States)

Meadows, Victoria S.; Claire, Mark W.; Kasting, James F.

2011-01-01

Abstract We used one-dimensional photochemical and radiative transfer models to study the potential of organic sulfur compounds (CS2, OCS, CH3SH, CH3SCH3, and CH3S2CH3) to act as remotely detectable biosignatures in anoxic exoplanetary atmospheres. Concentrations of organic sulfur gases were predicted for various biogenic sulfur fluxes into anoxic atmospheres and were found to increase with decreasing UV fluxes. Dimethyl sulfide (CH3SCH3, or DMS) and dimethyl disulfide (CH3S2CH3, or DMDS) concentrations could increase to remotely detectable levels, but only in cases of extremely low UV fluxes, which may occur in the habitable zone of an inactive M dwarf. The most detectable feature of organic sulfur gases is an indirect one that results from an increase in ethane (C2H6) over that which would be predicted based on the planet's methane (CH4) concentration. Thus, a characterization mission could detect these organic sulfur gases—and therefore the life that produces them—if it could sufficiently quantify the ethane and methane in the exoplanet's atmosphere. Key Words: Exoplanets—Biosignatures—Anoxic atmospheres—Planetary atmospheres—Remote life detection—Photochemistry. Astrobiology 11, 419–441. PMID:21663401

Evaluation of Methane Sources in Groundwater in Northeastern Pennsylvania

Science.gov (United States)

Molofsky, Lisa J; Connor, John A; Wylie, Albert S; Wagner, Tom; Farhat, Shahla K

2013-01-01

Testing of 1701 water wells in northeastern Pennsylvania shows that methane is ubiquitous in groundwater, with higher concentrations observed in valleys vs. upland areas and in association with calcium-sodium-bicarbonate, sodium-bicarbonate, and sodium-chloride rich waters—indicating that, on a regional scale, methane concentrations are best correlated to topographic and hydrogeologic features, rather than shale-gas extraction. In addition, our assessment of isotopic and molecular analyses of hydrocarbon gases in the Dimock Township suggest that gases present in local water wells are most consistent with Middle and Upper Devonian gases sampled in the annular spaces of local gas wells, as opposed to Marcellus Production gas. Combined, these findings suggest that the methane concentrations in Susquehanna County water wells can be explained without the migration of Marcellus shale gas through fractures, an observation that has important implications for understanding the nature of risks associated with shale-gas extraction. PMID:23560830

Methane Post-Processing for Oxygen Loop Closure

Science.gov (United States)

Greenwood, Zachary W.; Abney, Morgan B.; Miller, Lee

2016-01-01

State-of-the-art United States Atmospheric Revitalization carbon dioxide (CO2) reduction is based on the Sabatier reaction process, which recovers approximately 50% of the oxygen (O2) from crew metabolic CO2. Oxygen recovery from carbon dioxide is constrained by the limited availability of reactant hydrogen. Post-processing of methane to recover hydrogen with the Umpqua Research Company Plasma Pyrolysis Assembly (PPA) has the potential to further close the Atmospheric Revitalization oxygen loop. The PPA decomposes methane into hydrogen and hydrocarbons, predominantly acetylene, and a small amount of solid carbon. The hydrogen must then be purified before it can be recycled for additional oxygen recovery. Long duration testing and evaluation of a four crew-member sized PPA and a discussion of hydrogen recycling system architectures are presented.

Isotopic and geochemical tools to assess the feasibility of methanogenesis as a way to enhance hydrocarbon recovery in oil reservoirs

Energy Technology Data Exchange (ETDEWEB)

Jimenez, N.; Morris, B.E.L.; Richnow, H.H. [Helmholtz-Zentrum fuer Umweltforschung (UFZ), Leipzig (Germany). Abt. Isotopenbiogeochemie; Cai, M.; Yao, Jun [Helmholtz-Zentrum fuer Umweltforschung (UFZ), Leipzig (Germany). Abt. Isotopenbiogeochemie; University of Sicence and Technology, Beijing (China). School of Civil and Environment Engineering; Straaten, N.; Krueger, M. [Bundesanstalt fuer Geowissenschaften und Rohstoffe (BGR), Hannover (Germany). Fachbereich Geochemie

2013-08-01

In situ biotransformation of oil to methane was investigated in a thermophilic reservoir in Dagang, China using isotopic analyzes, chemical fingerprinting and molecular and biological methods. Our first results, which were already published, demonstrated that anaerobic oil degradation concomitant with methane production was occurring. The reservoir was highly methanogenic and the oil exhibited varying degrees of degradation between different parts of the reservoir, although it was mainly highly weathered, and nearly devoid of nalkanes, alkylbenzenes, alkyltoluenes, and light PAHs. In addition, the isotopic data from reservoir oil, water and gas was used to elucidate the origin of the methane. The average {delta}{sup 13}C for methane was around -47 permille and CO{sub 2} was highly enriched in {sup 13}C. The bulk isotopic discrimination ({Delta}{delta}{sup 13}C) between methane and CO{sub 2} was between 32 and 65 permille, in accordance with previously reported results for methane formation during hydrocarbon degradation. Subsequent microcosm experiments revealed that autochthonous microbiota are capable of degrading oil under methanogenic conditions and of producing methane and/or CO{sub 2} from {sup 13}C-labelled n-hexadecane, 2-methylnaphthalene or toluene ({delta}{sup 13}C values up to 550 permille). These results demonstrate that methanogenesis is linked to aliphatic and aromatic hydrocarbon degradation. Further experiments will elucidate the activation mechanisms for the different compounds. (orig.)

Material constraints related to storage of future European renewable electricity surpluses with CO_2 methanation

International Nuclear Information System (INIS)

Meylan, Frédéric D.; Moreau, Vincent; Erkman, Suren

2016-01-01

The main challenges associated with a growing production of renewable electricity are intermittency and dispersion. Intermittency generates spikes in production, which need to be curtailed when exceeding consumption. Dispersion means electricity has to be transported over long distances between production and consumption sites. In the Directive 2009/28/EC, the European Commission recommends sustainable and effective measures to prevent curtailments and facilitate transportation of renewable electricity. This article explores the material constraints of storing and transporting surplus renewable electricity by conversion into synthetic methane. Europe is considered for its mix of energy technologies, data availability and multiple energy pathways to 2050. Results show that the requirements for key materials and land remain relatively low, respecting the recommendations of the EU Commission. By 2050, more than 6 million tons of carbon dioxide might be transformed into methane annually within the EU. The efficiency of renewable power methane production is also compared to the natural process of converting solar into chemical energy (i.e. photosynthesis), both capturing and reenergizing carbon dioxide. Overall, the production of renewable methane (including carbon dioxide capture) is more efficient and less material intensive than the production of biofuels derived from photosynthesis and biomass conversion. - Highlights: •The potential of methanation to store renewable electricity surpluses is assessed. •Material constraints are relatively low. •Biogenic CO_2 will probably be insufficient. •Production of renewable power methane is more efficient than conventional biofuels. •Renewable power methane can help decarbonizing the global energy sector.

Methane-oxidizing seawater microbial communities from an Arctic shelf

Science.gov (United States)

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.

Retention efficiencies of halogenated and non-halogenated hydrocarbons in selected wetland ecosystem in Lake Victoria Basin

Directory of Open Access Journals (Sweden)

Shadrack Mule

2015-06-01

Full Text Available The determination of retention efficiencies of halogenated and non-halogenated hydrocarbon in selected wetland ecosystems in Lake Victoria basin was carried out. Qualitative and quantitative determination of the presence of residual hydrocarbons in Kigwal/Kimondi, Nyando and Nzoia wetland ecosystems using Gas Chromatography - Mass Spectrometer (GC-MS instrument indicated the presence of residual organochlorines, organophosphorus, carbamates and synthetic pyrethroid hydrocarbons in water, sediment and plant materials. In order to compare the retention efficiencies of the wetlands, the wetland ecosystems were divided into three different sections, namely: inlet, mid and outlet. Calculations of mass balances of residual halogenated and non-halogenated hydrocarbons at the respective sections was done taking into account the partition of the studied compounds in samples of water, sediments and papyrus reed plant materials and analyzed using validated Gas Chromatography - Mass Spectrometer (GC-MS method. From the analysis, several residual hydrocarbons namely: bendiocarb, benzene hexachloride (BHC, carbaryl, cypermethrin, decis, deltamethrin, diazinon, dieldrin, DDT, DDD, DDE, malathion, propoxur, sumithion, 5-phenylrhodanine, 1,3,5-trichlorobenzene, 1-(2-phenoxybenzylhydrazine were detected and quantified. The levels of the selected residual hydrocarbons in water samples were used to calculate the retention efficiencies of a specific hydrocarbon and the values recorded. Generally, River Nyando wetland recorded mean percentage retention efficiencies of 76 and 94% for dry and rainy seasons respectively; Kigwal/Kimondi wetland had seasonal mean percentage retention efficiencies of 63 to 78%. River Nzoia also had calculated seasonal mean percentage retention efficiencies of between 56 to 88%. Dry season had lower mean percentages retention efficiencies as compared to rainy season in the three wetlands of interest during the period of study. The study

Effects of composition of labile organic matter on biogenic production of methane in the coastal sediments of the Arabian Sea.

Science.gov (United States)

Gonsalves, Maria-Judith; Fernandes, Christabelle E G; Fernandes, Sheryl Oliveira; Kirchman, David L; Bharathi, P A Loka

2011-11-01

Coastal regions are potential zones for production of methane which could be governed by ecological/environmental differences or even sediment properties of a niche. In order to test the hypothesis that methanogenesis in most marine sediments could be driven more by proteins than by carbohydrates and lipid content of labile organic matter (LOM), incubation experiments were carried out with sediments from different environmental niches to measure methane production. The methane production rates were examined in relationship to the sediment biochemistry, i.e., carbohydrates, proteins, and lipids. The gas production measured by head space method ranged from 216 ng g( -1) day( -1) in the mangrove sediments to 3.1 μg g( -1) day( -1) in the shallow Arabian Sea. LOM ranged from 1.56 to 2.85 mg g( -1) in the shallow Arabian Sea, from 3.35 to 5.43 mg g( -1) in the mangrove estuary, and from 0.66 to 0.70 mg g( -1) in the sandy sediments with proteins contributing maximum to the LOM pool. Proteins influenced methane production in the clayey sediments of shallow depths of the Arabian Sea (r = 0.933, p methane production. The gas production was more pronounced in shallow and surface sediments and it decreased with depth apparently governed by the decrease in lability index. Thus, the lability index and protein content are important factors that determine methane production rates in these coastal ecosystems.

Sustainable fuel production by thermocatalytic decomposition of methane – A review

Directory of Open Access Journals (Sweden)

K. Srilatha

2017-12-01

Full Text Available Thermocatalytic Decomposition of Methane (TCD is a completely green single step technology for producing hydrogen and carbon nanomaterials. This paper review about the research in laboratory-scale on TCD, specifically the recent advances like co-feeding effect and regeneration of catalyst for enhancing the productivity of the entire process. Although a remarkable success on the laboratory-scale has been fulfilled, TCD for free greenhouse gas (GHG hydrogen production is still in its infancy. The necessity for commercialization of TCD is more than ever in the present-day condition of massive GHG emission. TCD generally studied over several types of catalysts, for example mono, bi, trimetallic, combination of metal–metal oxide, carbon and metal doped carbon catalysts. Catalyst Deactivation is the main problem found in TCD process. Regeneration of catalyst and co-feeding of methane with other hydrocarbon are the two main solutions placed helped in accordance to overcome deactivation problem. Higher amount of co-feed hydrocarbon in situ produce more amount of highly active carbon deposits which support further methane decomposition to produce extra hydrogen. The conversion rate of methane increases with increasing temperature and decreases with the flow rate in the co-feeding process in a comparable manner as observed in normal TCD. The presence of co-components in the post-reaction stream is an important challenge attempted in the co-feeding and regeneration. Keywords: Hydrogen, Catalysts, Thermocatalytic decomposition

Combustion and emissions control in diesel-methane dual fuel engines: The effects of methane supply method combined with variable in-cylinder charge bulk motion

International Nuclear Information System (INIS)

Carlucci, Antonio P.; Laforgia, Domenico; Saracino, Roberto; Toto, Giuseppe

2011-01-01

Highlights: → We studied dual fuel combustion in diesel engines. → Bulk flow structure of in-cylinder charge and methane supply method were investigated. → Swirl charge motion is capable to enhance air-methane mixture oxidation at low loads. → Methane port injection is capable to reduce unburned hydrocarbons and nitric oxides. - Abstract: In this paper, the results of an extensive experimental campaign about dual fuel combustion development and the related pollutant emissions are reported, paying particular attention to the effect of both the in-cylinder charge bulk motion and methane supply method. A diesel common rail research engine was converted to operate in dual fuel mode and, by activating/deactivating the two different inlet valves of the engine (i.e. swirl and tumble), three different bulk flow structures of the charge were induced inside the cylinder. A methane port injection method was proposed, in which the gaseous fuel was injected into the inlet duct very close to the intake valves, in order to obtain a stratified-like air-fuel mixture up to the end of the compression stroke. For comparison purposes, a homogeneous-like air-fuel mixture was obtained injecting methane more upstream the intake line. Combining the different positions of the methane injector and the three possible bulk flow structures, seven different engine inlet setup were tested. In this way, it was possible to evaluate the effects on dual fuel combustion due to the interaction between methane injector position and charge bulk motion. In addition, methane injection pressure and diesel pilot injection parameters were varied setting the engine at two operating conditions. For some interesting low load tests, the combustion development was studied more in detail by means of direct observation of the process, using an in-cylinder endoscope and a digital CCD camera. Each combustion image was post-processed by a dedicated software, in order to extract only those portions with flame

Coupling and reforming of methane by means of low pressure radio-frequency plasmas

Energy Technology Data Exchange (ETDEWEB)

Pedro Patino; Yasnahir Perez; Manuel Caetano [Universidad Central de Venezuela, Caracas (Venezuela). Escuela de Quimica, Facultad de Ciencias

2005-11-01

Non-oxidative coupling of CH{sub 4}/H{sub 2} mixtures was carried out by means of radio frequency (rf) glow discharges for the first time. A central composite design was employed to determine the best experimental conditions for methane transformation into higher hydrocarbons and to fit the experimental data. RF power was the factor showing the highest effect on the results while CH{sub 4}/H{sub 2} mole ratio showed the lowest. Conversion was 46.4% at 100 W, 0.07 mbar and CH{sub 4}/H{sub 2} mole ratio of . Selectivity was 56.9% for C{sub 2}, 6.9% for C{sub 3}, and 36.2% for C{sub 4} hydrocarbons. Least squares fits of quadratic equations yielded approximating functions permitting to predict results of random experiments with errors of about 5%. The same rf system was used for the reforming of methane with CO{sub 2}, O{sub 2}, and steam plasmas, respectively. The highest oxidation was observed with oxygen whilst steam plasma produced the best results. H{sub 2}/CO mole ratio was adjusted by setting specific experimental parameters of the latter. CO{sub 2} free synthesis gas was produced at higher H{sub 2}O and CH{sub 4} flow rates, i.e. 0.8 mmol/h and higher power, i.e. 100 W. CO{sub 2} and CO free H{sub 2} was produced at 0.3 and 0.6 mmol/h flow rates of H{sub 2}O and CH{sub 4}, respectively, and 50 W. 26 refs., 3 figs., 6 tabs.

Determination of Henry’s law constant of light hydrocarbon gases at low temperatures

International Nuclear Information System (INIS)

Mohebbi, V.; Naderifar, A.; Behbahani, R.M.; Moshfeghian, M.

2012-01-01

Highlights: ► Henry’s constants of light hydrocarbon gases are reported at low temperatures. ► Solubility of iso-butane in water at low temperatures (275 K to 293 K) was measured. ► An expression of Krichevsky–Kasarnovsky equation is reported. - Abstract: The solubility of i-butane in water at the low temperatures was measured (274 K to 293 K). Additionally, Henry’s law constants of light hydrocarbons (methane, ethane, propane, i-butane, and n-butane) in water at the low temperatures are reported. A modified equation based on Krichevsky–Kasarnovsky equation is proposed to consider the effect of pressure and temperature on the equation parameters. Results show that Henry’s law constant of the selected components depends on temperature. It is deduced that pressure has a considerable effect on Henry’s law constant for methane, ethane, and propane, whereas this dependency for butanes is negligible.

Petroleum pollution in surface sediments of Daya Bay, South China, revealed by chemical fingerprinting of aliphatic and alicyclic hydrocarbons

Science.gov (United States)

Gao, Xuelu; Chen, Shaoyong

2008-10-01

Nine surface sediments collected from Daya Bay have been Soxhlet-extracted with 2:1 (v/v) dichloromethane-methanol. The non-aromatic hydrocarbon (NAH) fraction of solvent extractable organic matter (EOM) and some bulk geochemical parameters have been analyzed to determine petroleum pollution of the bay. The NAH content varies from 32 to 276 μg g -1 (average 104 μg g -1) dry sediment and accounts for 5.8-64.1% (average 41.6%) of the EOM. n-Alkanes with carbon number ranging from 15 to 35 are identified to be derived from both biogenic and petrogenic sources in varying proportions. The contribution of marine authigenic input to the sedimentary n-alkanes is lower than the allochthonous input based on the average n-C 31/ n-C 19 alkane ratio. 25.6-46.5% of the n-alkanes, with a mean of 35.6%, are contributed by vascular plant wax. Results of unresolved complex mixture, isoprenoid hydrocarbons, hopanes and steranes also suggest possible petroleum contamination. There is strong evidence of a common petroleum contamination source in the bay.

Can sediments at hydrocarbon seep sites represent a source for marine bioavailable iron? — A case study from the South China Sea

Science.gov (United States)

Li, N.; Feng, D.; Chen, D.

2017-12-01

Niu Li1, Dong Feng1,2, and Duofu Chen2,31CAS Key Laboratory of Ocean and Marginal Sea Geology, South China Sea Institute of Oceanology, Chinese Academy of Sciences, Guangzhou 510301, China. 2Laboratory for Marine Geology, Qingdao National Laboratory for Marine Science and Technology, Qingdao 266061, China. 3Hadal Science and Technology Research Center, College of Marine Sciences, Shanghai Ocean University, Shanghai 201306, China. Iron is an essential micronutrient and commonly considered to be one of the key-limiting factors for biological productivity in many ocean regions. Seafloor Fe supply should be most efficient in suboxic conditions. Recent studies shown that widely spread anoxic environments can develop in hydrocarbon seep sediment and local bottom water, owing to the occurrence of aerobic and/or anaerobic methane oxidation. Under this condition, the iron in sediment can be reduced to dissolved Fe2+ in the ocean. However, questions remain about whether the hydrocarbon seep sediment can represent a source for bioavailable iron to the ocean, and the control factor for the transformation of iron in the sediment remains largely unexplored. For a number of hydrocarbon seeps from the northern and southern South China Sea, the iron speciation, pyrite sulfur isotope, and iron isotope, as well as the major and trace elements are used to constrain the intensity of cold seep, and its impact on transformation of iron in sediment. Samples from both areas show sediment iron lost during the high methane flux conditions, owing to the suboxic conditions cause by aerobic methane oxidation. On the other hand, high sediment iron content accompanied by high sulfur content can be seen during the conditions of high methane flux without the occurrence of aerobic methane oxidation, which is possible ascribed to the anaerobic methane oxidation and the release of iron through seep activity. This study reveals the transformation of iron in the sediment is closely related to the

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

Science.gov (United States)

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.

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

Energy Technology Data Exchange (ETDEWEB)

Gunnoe, Thomas Brent [Univ. of Virginia, Charlottesville, VA (United States)

2016-11-11

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

HYFLUX: Satellite Exploration of Natural Hydrocarbon Seeps and Discovery of a Methane Hydrate Mound at GC600

Science.gov (United States)

Garcia-Pineda, O. G.; MacDonald, I. R.; Shedd, W.; Zimmer, B.

2009-12-01

Analysis of natural hydrocarbon seeps is important to improve our understanding of methane flux from deeper sediments to the water column. In order to quantify natural hydrocarbon seep formations in the Northern Gulf of Mexico, a set of 686 Synthetic Aperture Radar (SAR) images was analyzed using the Texture Classifying Neural Network Algorithm (TCNNA), which processes SAR data to delineate oil slicks. This analysis resulted in a characterization of 396 natural seep sites distributed in the northern GOM. Within these sites, a maximum of 1248 individual vents where identified. Oil reaching the sea-surface is deflected from its source during transit through the water column. This presentation describes a method for estimating locations of active oil vents based on repeated slick detection in SAR. One of the most active seep formations was detected in MMS lease block GC600. A total of 82 SAR scenes (collected by RADARSAT-1 from 1995 to 2007) was processed covering this region. Using TCNNA the area covered by each slick was computed and Oil Slicks Origins (OSO) were selected as single points within detected oil slicks. At this site, oil slick signatures had lengths up to 74 km and up to 27 km^2 of area. Using SAR and TCNNA, four active vents were identified in this seep formation. The geostatistical mean centroid among all detections indicated a location along a ridge-line at ~1200m. Sea truth observations with an ROV, confirmed that the estimated location of vents had a maximum offset of ~30 m from their actual locations on the seafloor. At the largest vent, a 3-m high, 12-m long mound of oil-saturated gas hydrate was observed. The outcrop contained thousands of ice worms and numerous semi-rigid chimneys from where oily bubbles were escaping in a continuous stream. Three additional vents were found along the ridge; these had lower apparent flow, but were also plugged with gas hydrate mounds. These results support use of SAR data for precise delineation of active seep

Effect of pendant isophthalic acid moieties on the adsorption properties of light hydrocarbons in HKUST-1-like tbo -MOFs: Application to methane purification and storage

KAUST Repository

Belmabkhout, Youssef

2014-01-01

Equilibrium adsorption of methane (CH4), C2+ gases (ethane (C2H6), ethylene (C2H4), propane (C3H8), and propylene (C3H6)), and carbon dioxide (CO2) was measured on a series of tbo-MOFs (topological analogues of the prototypical MOF, HKUST-1, correspondingly dubbed tbo-MOF-1), which were developed via the supermolecular building layer (SBL) pillaring strategy. Specifically, tbo-MOF-2 and its isoreticular, functionalized analogue, tbo-MOF-2-{CH2O[Ph(CO2H)2]}2 (or tbo-MOF-3), which is characterized by pendant isophthalic acid moieties freely pointing into the cavities, were evaluated on the basis of potential use in methane storage and C2+/CH4 separation. The parent, tbo-MOF-2, showed high gravimetric and volumetric CH4 uptake, close to the U.S. Department of Energy (DOE) target for methane storage at 35 bar and room temperature. Though the presence of the pendant isophthalic acid moiety in the analogous compound, tbo-MOF-3, led to a decrease in total CH4 uptake, due mainly to the reduced size of the cavities, interestingly, it increased the affinity of the SBL-based tbo-MOF platform for propane, propene, ethane, and ethylene at low pressures compared with CH4, due additionally to the enhanced interactions of the highly polarizable light hydrocarbons with the isophthalic acid moiety. Using Ideal Adsorption Solution Theory (IAST), the predicted mixture adsorption equilibria for the C3H8/CH4, C3H6/CH4, C2H6/CH4, C2H4/CH4, and C3H8/CO2 systems showed high adsorption selectivity for C2+ over methane for tbo-MOF-3 compared with tbo-MOF-2. The high working storage capacity of tbo-MOF-2 and the high affinity of tbo-MOF-3 for C2+ over CH4 and CO2 make tbo-MOF an ideal platform for studies in gas storage and separation.

Biogenic nanomaterials from photosynthetic microorganisms.

Science.gov (United States)

Jeffryes, Clayton; Agathos, Spiros N; Rorrer, Gregory

2015-06-01

The use of algal cell cultures represents a sustainable and environmentally friendly platform for the biogenic production of nanobiomaterials and biocatalysts. For example, advances in the production of biogeneic nanomaterials from algal cell cultures, such as crystalline β-chitin nanofibrils and gold and silver nanoparticles, could enable the 'green' production of biomaterials such as tissue-engineering scaffolds or drug carriers, supercapacitors and optoelectric materials. The in vivo functionalization, as well as newly demonstrated methods of production and modification, of biogenic diatom biosilica have led to the development of organic-inorganic hybrid catalytic systems as well as new biomaterials for drug delivery, biosensors and heavy-metal adsorbents. Copyright © 2014 Elsevier Ltd. All rights reserved.

Urban sources and emissions of nitrous oxide and methane in southern California, USA

Science.gov (United States)

Townsend-Small, A.; Pataki, D.; Tyler, S. C.; Czimczik, C. I.; Xu, X.; Christensen, L. E.

2012-12-01

Anthropogenic activities have resulted in increasing levels of greenhouse gases, including carbon dioxide, methane, and nitrous oxide. While global and regional emissions sources of carbon dioxide are relatively well understood, methane and nitrous oxide are less constrained, particularly at regional scales. Here we present the results of an investigation of sources and emissions of methane and nitrous oxide in Los Angeles, California, USA, one of Earth's largest urban areas. The original goal of the project was to determine whether isotopes are useful tracers of agricultural versus urban nitrous oxide and methane sources. For methane, we found that stable isotopes (carbon-13 and deuterium) and radiocarbon are good tracers of biogenic versus fossil fuel sources. High altitude observations of methane concentration, measured continuously using tunable laser spectroscopy, and isotope ratios, measured on discrete flask samples using mass spectrometry, indicate that the predominant methane source in Los Angeles is from fossil fuels, likely from "fugitive" emissions from geologic formations, natural gas pipelines, oil refining, or power plants. We also measured nitrous oxide emissions and isotope ratios from urban (landscaping and wastewater treatment) and agricultural sources (corn and vegetable fields). There was no difference in nitrous oxide isotope ratios between the different types of sources, although stable isotopes did differ between nitrous oxide produced in oxic and anoxic wastewater treatment tanks. Our nitrous oxide flux data indicate that landscaped turfgrass emits nitrous oxide at rates equivalent to agricultural systems, indicating that ornamental soils should not be disregarded in regional nitrous oxide budgets. However, we also showed that wastewater treatment is a much greater source of nitrous oxide than soils regionally. This work shows that global nitrous oxide and methane budgets are not easily downscaled to regional, urban settings, which has

Shock tube/laser absorption measurements of methane, acetylene and ethylene during the pyrolysis of n-pentane and iso-pentane

KAUST Repository

Sajid, Muhammad Bilal

2015-11-09

Pentane isomers are important constituents of distillate gasoline, compressed natural gas and liquefied petroleum gas. Pentane chemistry is integral component of the chemical kinetic mechanisms of larger hydrocarbons. Existing kinetic mechanisms differ in their predictions of the oxidative and pyrolysis behavior of pentane isomers. This work provides new species time-history data to validate and improve pentane chemistry models. Methane, acetylene and ethylene are measured during the high-temperature pyrolysis of n-pentane and iso-pentane. Experiments are performed behind reflected shock waves over 1400–2100 K and pressures near 1 atm. Methane and acetylene are measured using a quantum cascade laser operating near 8 µm, whereas ethylene is measured with a CO2 gas laser operating near 10.6 µm. A two-color technique is used to eliminate broadband interference caused by large hydrocarbons. Measurements are compared with predictions of existing chemical kinetic mechanisms which underpredict the formation of methane and acetylene but overpredict ethylene formation.

Sub-Antarctic marine aerosol: dominant contributions from biogenic sources

Directory of Open Access Journals (Sweden)

J. Schmale

2013-09-01

Full Text Available Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS, was 21% non-sea-salt sulfate, 2% nitrate, 8% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea spray signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA profiles could be isolated: an amino acid/amine factor (AA-OA, 18% of OA mass, a methanesulfonic acid OA factor (MSA-OA, 25%, a marine oxygenated OA factor (M-OOA, 41%, a sea spray OA fraction (SS-OA, 7% and locally produced hydrocarbon-like OA (HOA, 9%. The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (N : C ratio = 0.13, has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea spray aerosol was identified (SS-OA. However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not

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

Science.gov (United States)

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.

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.

Science.gov (United States)

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.

Distribution of aliphatic hydrocarbons, polycyclic aromatic hydrocarbons and organochlorinated pollutants in deep-sea sediments of the Southern Cretan margin, Eastern Mediterranean Sea: a baseline assessment.

Science.gov (United States)

Mandalakis, Manolis; Polymenakou, Paraskevi N; Tselepides, Anastasios; Lampadariou, Nikolaos

2014-07-01

Deep sediments from the southern Cretan margin were analyzed to establish baseline levels for various types of organic pollutants before the anticipated intensification of anthropogenic activities. The total concentration of aliphatic hydrocarbons (ΣAH:326-3758ngg(-1), dry weight) was similar to those reported for deep sediments of the western Mediterranean Sea, while considerably lower levels were measured for polycyclic aromatic hydrocarbons (ΣPAH:9-60ngg(-1)). Source-diagnostic ratios suggested that the aliphatic hydrocarbons in sediments were mainly of terrestrial biogenic origin, while polycyclic aromatic hydrocarbons stemmed from the deposition of long-range transported combustion aerosols. Among the organochlorinated compounds analyzed, β-hexachlorocyclohexane (β-HCH:222-7052pgg(-1)), 1,1,1-trichloro-2,2-bis(4-chlorophenyl)ethane (p,p'-DDT:37-2236pgg(-1)) and polychlorinated biphenyls (ΣPCB:38-1182pgg(-1)) showed the highest abundance in sediments. The presence of HCHs and PCBs was attributed to historical inputs that have undergone extensive weathering, whereas an ongoing fresh input was suggested for p,p'-DDT. Multiple linear regression analysis revealed that the levels of the various pollutants in sediments were controlled by different factors, but with organic carbon content playing a prominent role in most cases. Copyright © 2014 Elsevier Ltd. All rights reserved.

Sources, extent and history of methane seepage on the continental shelf off northern Norway

Science.gov (United States)

Sauer, Simone; Lepland, Aivo; Chand, Shyam; Schubert, Carsten J.; Eichinger, Florian; Knies, Jochen

2014-05-01

Active natural hydrocarbon gas seepage was recently discovered in the Hola area on the continental shelf off Vesterålen, northern Norway. We conducted acoustic and geochemical investigations to assess the modern and past extent, source and pathways of the gas seepage . Water column echosounder surveys showed bubble plumes up to several tens of metres above the seafloor. Analyses of dissolved methane in the water column indicated slightly elevated concentrations (50 nM) close to the seafloor. To identify fluxes and origin of methane in the sediments we analysed sediment pore water chemistry, the isotopic composition of methane and of dissolved inorganic carbon (d13CCH4, d2HCH4, d13CDIC) in three closely spaced (

Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits

Science.gov (United States)

Bhattacharyya, Amrita; Campbell, Kate M.; Kelly, Shelly D.; Roebbert, Yvonne; Weyer, Stefan; Bernier-Latmani, Rizlan; Borch, Thomas

2017-06-01

Historically, it is believed that crystalline uraninite, produced via the abiotic reduction of hexavalent uranium (U(VI)) is the dominant reduced U species formed in low-temperature uranium roll-front ore deposits. Here we show that non-crystalline U(IV) generated through biologically mediated U(VI) reduction is the predominant U(IV) species in an undisturbed U roll-front ore deposit in Wyoming, USA. Characterization of U species revealed that the majority (~58-89%) of U is bound as U(IV) to C-containing organic functional groups or inorganic carbonate, while uraninite and U(VI) represent only minor components. The uranium deposit exhibited mostly 238U-enriched isotope signatures, consistent with largely biotic reduction of U(VI) to U(IV). This finding implies that biogenic processes are more important to uranium ore genesis than previously understood. The predominance of a relatively labile form of U(IV) also provides an opportunity for a more economical and environmentally benign mining process, as well as the design of more effective post-mining restoration strategies and human health-risk assessment.

Methane occurrence in groundwater of south-central New York State, 2012: summary of findings

Science.gov (United States)

Heisig, Paul M.; Scott, Tia-Marie

2013-01-01

A survey of methane in groundwater was undertaken to document methane occurrence on the basis of hydrogeologic setting within a glaciated 1,810-square-mile area of south-central New York that has not seen shale-gas resource development. The adjacent region in northeastern Pennsylvania has undergone shale-gas resource development from the Marcellus Shale. Well construction and subsurface data were required for each well sampled so that the local hydrogeologic setting could be classified. All wells were also at least 1 mile from any known gas well (active, exploratory, or abandoned). Sixty-six domestic wells and similar purposed supply wells were sampled during summer 2012. Field water-quality characteristics (pH, specific conductance, dissolved oxygen, and temperature) were measured at each well, and samples were collected and analyzed for dissolved gases, including methane and short-chain hydrocarbons. Carbon and hydrogen isotopic ratios of methane were measured in 21 samples that had at least 0.3 milligram per liter (mg/L) methane.

Secondary biological coalbed gas in the Xinji area, Anhui province, China: Evidence from the geochemical features and secondary changes

Energy Technology Data Exchange (ETDEWEB)

Tao, Mingxin [Key Laboratory of Environmental Change and Natural Disaster of Ministry of Education, College of Resources Sciences and Technology, Beijing Normal University, Beijing 100875 (China); Key Laboratory of Gas Geochemistry, Institute of Geology and Geophysics, Chinese Academy of Sciences, Lanzhou 730000 (China); Shi, Baoguang; Wang, Wanchun; Li, Xiaobin; Gao, Bo [Key Laboratory of Gas Geochemistry, Institute of Geology and Geophysics, Chinese Academy of Sciences, Lanzhou 730000 (China); Li, Jinying [Material and Environment College, Qindao University of Science and Technology, Qindao 266042 (China)

2007-07-02

In order to ascertain the origin of the coalbed gas in the Xinji area, Anhui Province of China, the paper examined the geochemical features and secondary changes of CH{sub 4}, C{sub 2}H{sub 6}, CO{sub 2} and N{sub 2} from the coalbed gas. The related gas composition, carbon isotope and tracer geochemical data are as follows: 0.993 to 1.0 for C{sub 1}/C{sub 1-n}, 188.6 to 2993.7 for C{sub 1}/C{sub 2}, < 2% for CO{sub 2}, 0.64 to 3.06% for [CO{sub 2}/(CO{sub 2} + CH{sub 4})]100%, - 50.7 permille to - 61.3 permille for {delta}{sup 13}C{sub 1} with the average value of - 56.6 permille, - 15.9 permille to - 26.7 permille for {delta}{sup 13}C{sub 2}, - 10.8 permille to - 25.3 permille for {delta}{sup 13}C{sub 3}, - 6.0 permille to - 39.0 permille for {delta}{sup 13}C{sub CO2} with the average value of - 17.9 permille, 30.7 permille to 43.9 permille for {delta}{delta}{sup 13}C{sub C2-C1}, and 17.2 permille to 50 permille for {delta}{delta}{sup 13}C{sub CO2-C1}, - 1 permille to + 1 permille for {delta}{sup 15}N{sub N2}, 1.13 x 10{sup -7} to 3.20 x 10{sup -7} for {sup 3}He/{sup 4}He with R/Ra ratios range from 0.08 to 0.23. The Ro values of the coal range from 0.88% to 0.91%. The trends of the {delta}{sup 13}C{sub 1} values and {delta}{sup 13}C{sub CO2} values downward in the stratigraphic profile are opposite: the former appears as a slight light-heavy-light trend, but the latter appears as a heavy-light-heavy trend. The {delta}{sup 13}C{sub 1} values have a negative correlation with the {delta}{sup 13}C{sub CO2} values. However, the {delta}{sup 13}C{sub 2} values have no correlation with the {delta}{sup 13}C{sub 1} values due to its complicated variation. The thermal evolution of the coal in the Xinji area is in the phase of a lot of wet gas generation, but most of the CO{sub 2} and heavy hydrocarbons have been reduced or degraded by microbes and have changed into biogenic methane. The coalbed gas is comprised of secondary biogenic methane, thermogenic methane, the

Biogenic amines degradation by microorganisms isolated from cheese

Directory of Open Access Journals (Sweden)

Irena Butor

2017-01-01

Full Text Available The aim of this study was the isolation and characterization of microorganisms able to degrade biogenic amines and their identification. Individual microorganisms were obtained by isolation from commercially available foodstuffs and food produced in the technological laboratories of Faculty of Technology, Tomas Bata University in Zlín and subsequently identified by MALDI-TOF MS. The results of MALDI-TOF MS identification were verified by 16S rRNA sequenation. In this work was studied the ability of 5 bacterial strains positive to biogenic amines degradation isolated from dairy products to decrease biogenic amines content in vitro and quantified reduction in the concentration of biogenic amines tryptamine, β-phenylethylamine, putrescine, cadaverine, histamine and tyramine. The level of degradation (decrease of biogenic amines was determined on the base of the ability to grow in media with biogenic amines as the sole source carbon and nitrogen. The isolated strains with the ability of degradation of one or more biogenic amines were cultured in medium supplemented with relevant biogenic amines, the media derivatized with dansyl chloride and these amines separated by HPLC at a wavelength of 254 nm. From five tested strains identified as Bacillus subtilis, Bacillus pumilus, Enterobacter cloacae, Rhizobium radiobacter and Acinetobacter pitii, isolated from gouda type cheese, the greatest ability of degradation was observed in Bacillus subtilis, which was capable to degrade almost all amount of histamine, cadaverine and putrescine. Other four strains showed a lower rate of degradation than Bacillus subtilis, but the ability to degrade biogenic amines with these microorganisms was still significant.

Methane hydrates and the future of natural gas

Science.gov (United States)

Ruppel, Carolyn

2011-01-01

For decades, gas hydrates have been discussed as a potential resource, particularly for countries with limited access to conventional hydrocarbons or a strategic interest in establishing alternative, unconventional gas reserves. Methane has never been produced from gas hydrates at a commercial scale and, barring major changes in the economics of natural gas supply and demand, commercial production at a large scale is considered unlikely to commence within the next 15 years. Given the overall uncertainty still associated with gas hydrates as a potential resource, they have not been included in the EPPA model in MITEI’s Future of Natural Gas report. Still, gas hydrates remain a potentially large methane resource and must necessarily be included in any consideration of the natural gas supply beyond two decades from now.

Catalytic removal of methane and NO{sub x} in lean-burn natural-gas engine exhaust; Elimination par catalyse du methane et des NO{sub x} dans les echappements de moteur au gaz naturel a basse combustion

Energy Technology Data Exchange (ETDEWEB)

Yamamoto, H.; Satokawa, S.; Yahagi, M.; Yamaseki, K.; Hoshi, F.; Uchida, H.; Yokota, H. [Tokyo Gas Co., Ltd. (Japan)

2000-07-01

We have developed a new catalytic system to reduce the emissions of hydrocarbons, carbon monoxide (CO), and nitrogen oxides (NO{sub x}) contained in the exhaust gases from a lean-burn natural-gas engine. Catalytic oxidation of unburned hydrocarbons and CO in the exhaust has been studied for noble metals supported on alumina. (1) A low-loading catalyst comprising platinum supported on alumina (Pt/alumina) was efficient for the oxidation of CO and hydrocarbons without methane. The CO conversions were maintained at more than 98 % for 20,000 hours over the Pt/alumina. (2) A catalyst comprising platinum and palladium supported on alumina (Pt-Pd/alumina) exhibited higher levels of oxidation of hydrocarbons (including methane) than a catalyst comprising only palladium supported on alumina (Pd/alumina). Its oxidation also lasted longer. The combined effects of the platinum and palladium metals achieved high sulfur dioxide resistance. Increasing the palladium content in the Pt-Pd/alumina catalyst increased the level of oxidation and extended the lifetime of the catalyst. (3) A catalyst comprising silver supported on alumina (Ag/alumina) was effective at reducing the amount of NO{sub X} by using the unburned hydrocarbons in the exhaust gas. The NO{sub x} conversions over Ag/alumina were maintained at more than 30 % for 3,500 hours. We describe a total clean-up system consisting of a Ag/alumina catalyst and a Pt-Pd/alumina catalyst in series on the exhaust gas stream. (authors)

Characterization of hydrocarbons, halocarbons and carbonyls in the atmosphere of Hong Kong.

Science.gov (United States)

Guo, H; Lee, S C; Louie, P K K; Ho, K F

2004-12-01

Ambient air quality measurements of 156 species including 39 alkanes, 32 alkenes, 2 alkynes, 24 aromatic hydrocarbons, 43 halocarbons and 16 carbonyls, were carried out for 120 air samples collected at two sampling stations (CW and TW) in 2001 throughout Hong Kong. Spatial variations of volatile organic compounds (VOCs) in the atmosphere were investigated. Levels of most alkanes and alkenes at TW site were higher than that at the CW site, while the BTEX concentrations at the two sites were close. The BTEX ratios at CW and TW were 1.6:10.1:1.0:1.6 and 2.1:10.8:1.0:2.0, respectively. For major halogenated hydrocarbons, the mean concentrations of chloromethane, CFCs 12 and 22 did not show spatial variations at the two sites. However, site-specific differences were observed for trichloroethene and tetrachloroethene. Furthermore, there were no significant differences for carbonyls such as formaldehyde, acetaldehyde and acetone between the two sites. The levels of selected hydrocarbons in winter were 1-5 times that in summer. There were no common seasonal trends for carbonyls in Hong Kong. The ambient level of formaldehyde, the most abundant carbonyl, was higher in summer. However, levels of acetaldehyde, acetone and benzaldehyde in winter were 1.6-3.8 times that in summer. The levels of CFCs 11 and 12, and chloromethane in summer were higher than that in winter. Strong correlation of most hydrocarbons with propene and n-butane suggested that the primary contributors of hydrocarbons were vehicular emissions in Hong Kong. In addition, gasoline evaporation, use of solvents, leakage of liquefied petroleum gas (LPG), natural gas leakage and other industrial emissions, and even biogenic emissions affected the ambient levels of hydrocarbons. The sources of halocarbons were mainly materials used in industrial processes and as solvents. Correlation analysis suggested that photochemical reactions made significant contributions to the ambient levels of carbonyls in summer whereas

National Gas Hydrate Program Expedition 01 offshore India; gas hydrate systems as revealed by hydrocarbon gas geochemistry

Science.gov (United States)

Lorenson, Thomas; Collett, Timothy S.

2018-01-01

The National Gas Hydrate Program Expedition 01 (NGHP-01) targeted gas hydrate accumulations offshore of the Indian Peninsula and along the Andaman convergent margin. The primary objectives of coring were to understand the geologic and geochemical controls on the accumulation of methane hydrate and their linkages to underlying petroleum systems. Four areas were investigated: 1) the Kerala-Konkan Basin in the eastern Arabian Sea, 2) the Mahanadi and 3) Krishna-Godavari Basins in the western Bay of Bengal, and 4) the Andaman forearc Basin in the Andaman Sea.Upward flux of methane at three of the four of the sites cored during NGHP-01 is apparent from the presence of seafloor mounds, seismic evidence for upward gas migration, shallow sub-seafloor geochemical evidence of methane oxidation, and near-seafloor gas composition that resembles gas from depth.The Kerala-Konkan Basin well contained only CO2 with no detectable hydrocarbons suggesting there is no gas hydrate system here. Gas and gas hydrate from the Krishna-Godavari Basin is mainly microbial methane with δ13C values ranging from −58.9 to −78.9‰, with small contributions from microbial ethane (−52.1‰) and CO2. Gas from the Mahanadi Basin was mainly methane with lower concentrations of C2-C5 hydrocarbons (C1/C2 ratios typically >1000) and CO2. Carbon isotopic compositions that ranged from −70.7 to −86.6‰ for methane and −62.9 to −63.7‰ for ethane are consistent with a microbial gas source; however deeper cores contained higher molecular weight hydrocarbon gases suggesting a small contribution from a thermogenic gas source. Gas composition in the Andaman Basin was mainly methane with lower concentrations of ethane to isopentane and CO2, C1/C2 ratios were mainly >1000 although deeper samples were compositions range from −65.2 to −80.7‰ for methane, −53.1 to −55.2‰ for ethane is consistent with mainly microbial gas sources, although one value recorded of −35.4‰ for propane

Non-oxidative methane dehydroaromatization reaction over highly ...

Indian Academy of Sciences (India)

Pradeep Kumar Budde

2018-03-02

Mar 2, 2018 ... damental science to advanced engineering technology for conversion of .... C using an automatic micropore physisorption ana- lyzer (Micrometrics ASAP ..... MoO2 species with methane to form molybdenum car- bide species.

Assessing methods to estimate emissions of non-methane organic compounds from landfills

DEFF Research Database (Denmark)

Saquing, Jovita M.; Chanton, Jeffrey P.; Yazdani, Ramin

2014-01-01

The non-methane organic compound (NMOC) emission rate is used to assess compliance with landfill gas emission regulations by the United States Environmental Protection Agency (USEPA). A recent USEPA Report (EPA/600/R-11/033) employed a ratio method to estimate speciated NMOC emissions (i...... and speciated NMOC concentration and flux data from 2012/2013 field sampling of four landfills, an unpublished landfill study, and literature data from three landfills. The ratio method worked well for landfills with thin covers (...

Coupling spectroscopic and chromatographic techniques for evaluation of the depositional history of hydrocarbons in a subtropical estuary

International Nuclear Information System (INIS)

Martins, César C.; Doumer, Marta E.; Gallice, Wellington C.; Dauner, Ana Lúcia L.; Cabral, Ana Caroline; Cardoso, Fernanda D.

2015-01-01

Spectroscopic and chromatographic techniques can be used together to evaluate hydrocarbon inputs to coastal environments such as the Paranaguá estuarine system (PES), located in the SW Atlantic, Brazil. Historical inputs of aliphatic hydrocarbons (AHs) and polycyclic aromatic hydrocarbons (PAHs) were analyzed using two sediment cores from the PES. The AHs were related to the presence of biogenic organic matter and degraded oil residues. The PAHs were associated with mixed sources. The highest hydrocarbon concentrations were related to oil spills, while relatively low levels could be attributed to the decrease in oil usage during the global oil crisis. The results of electron paramagnetic resonance were in agreement with the absolute AHs and PAHs concentrations measured by chromatographic techniques, while near-infrared spectroscopy results were consistent with unresolved complex mixture (UCM)/total n-alkanes ratios. These findings suggest that the use of a combination of techniques can increase the accuracy of assessment of contamination in sediments. - Highlights: • Historical inputs of hydrocarbons in a subtropical estuary were evaluated. • Spectroscopic and chromatographic methods were used in combination. • High hydrocarbon concentrations were related to anthropogenic activities. • Low hydrocarbon levels could be explained by the 1970s global oil crisis. - Spectroscopic and chromatographic techniques could be used together to evaluate hydrocarbon inputs to coastal environments

Efficient Reservoir Simulation with Cubic Plus Association and Cross-Association Equation of State for Multicomponent Three-Phase Compressible Flow with Applications in CO2 Storage and Methane Leakage

Science.gov (United States)

Moortgat, J.

2017-12-01

We present novel simulation tools to model multiphase multicomponent flow and transport in porous media for mixtures that contain non-polar hydrocarbons, self-associating polar water, and cross-associating molecules like methane, ethane, unsaturated hydrocarbons, CO2 and H2S. Such mixtures often occur when CO2 is injected and stored in saline aquifers, or when methane is leaking into groundwater. To accurately predict the species transfer between aqueous, gaseous and oleic phases, and the subsequent change in phase properties, the self- and cross-associating behavior of molecules needs to be taken into account, particularly at the typical temperatures and pressures in deep formations. The Cubic-Plus-Association equation-of-state (EOS) has been demonstrated to be highly accurate for such problems but its excessive computational cost has prevented widespread use in reservoir simulators. We discuss the thermodynamical framework and develop sophisticated numerical algorithms that allow reservoir simulations with efficiencies comparable to a simple cubic EOS. This approach improves our predictive powers for highly nonlinear fluid behavior related to geological carbon sequestration, such as density driven flow and natural convection (solubility trapping), evaporation of water into the CO2-rich gas phase, and competitive dissolution-evaporation when CO2 is injected in, e.g., methane saturated aquifers. Several examples demonstrate the accuracy and robustness of this EOS framework for complex applications.

Chemical and isotopic fractionations of natural gases during their migration. Importance of methane solubilization and diffusion during geological times; Fractionnements chimiques et isotopiques des gaz naturels lors de leur migration. Importance de la solubilisation et de la diffusion du methane au cours des temps geologiques

Energy Technology Data Exchange (ETDEWEB)

Pernaton, E

1998-09-09

Two experimental devices have been elaborated in the purpose of simulating in laboratory the solubilization of methane in water and the migration by solubilization/diffusion of some gas species (methane, ethane, propane and nitrogen) through porous media saturated with water. Significant shifts in isotopic ratios of diffused methane (carbon and hydrogen) have been observed. Those fractionations for carbon isotopes, which in most cases are characterised by a {sup 12}C-enriched diffused methane, have fundamental consequences about the interpretation of the origin of methane in sedimentary basins and, in a more general way, about the genetic characterisation of hydrocarbon gases in reservoirs. Indeed, this gives an ambiguous origin for any gas having {sup 12}C-enriched methane, two different interpretations are possible: mixing between thermogenic and bacterial hydrocarbon gases and a diffusive trend during migration. Using a diagram C2/C1 versus {delta}{sup 13}C1, we have shown that in some geological cases, these two processes, mixing and diffusion, exist and that it is possible to discern them.The chemical and isotopic compositions of natural gases do not only reflect genetic processes but are also an indication of their migration. Moreover, the experiments have shown that the gas transport by solubilization/diffusion is a potential operator of gas leakage from natural accumulations. In consequence, a numerical model of gas migration through cap rocks of reservoirs has been elaborated and will be integrated into sedimentary basin models. (author)

Emissions of biogenic sulfur gases from northern bogs and fens

Science.gov (United States)

Demello, William Zamboni; Hines, Mark E.; Bayley, Suzanne E.

1992-01-01

Sulfur gases are important components of the global cycle of S. They contribute to the acidity of precipitation and they influence global radiation balance and climate. The role of terrestrial sources of biogenic S and their effect on atmospheric chemistry remain as major unanswered questions in our understanding of the natural S cycle. The role of northern wetlands as sources and sinks of gaseous S by measuring rates of S gas exchange as a function of season, hydrologic conditions, and gradients in tropic status was investigated. Experiments were conducted in wetlands in New Hampshire, particularly a poor fen, and in Mire 239, a poor fen at the Experimental Lakes Area (ELA) in Ontario. Emissions were determined using Teflon enclosures, gas cryotrapping methods and gas chromatography (GC) with flame photometric detection. Dynamic (sweep flow) and static enclosures were employed which yielded similar results. Dissolved S gases and methane were determined by gas stripping followed by GC.

Preliminary reservoir model of enhanced coalbed methane (ECBM) in a subbituminous coal seam, Huntly Coalfield, New Zealand

Energy Technology Data Exchange (ETDEWEB)

Zarrouk, Sadiq J. [Department of Engineering Science, University of Auckland, Private Bag 92019, Auckland (New Zealand); Moore, Tim A. [Solid Energy New Zealand Ltd, PO Box. 1303, Christchurch (New Zealand)]|[Department of Geological Sciences, University of Canterbury, Christchurch (New Zealand)

2009-01-07

The Huntly coalfield has significant coal deposits that contain biogenically-sourced methane. The coals are subbituminous in rank and Eocene in age and have been previously characterised with relatively low to moderate measured gas (CH{sub 4}) contents (2-4 m{sup 3}/ton). The CO{sub 2} holding capacity is relatively high (18.0 m{sup 3}/ton) compared with that of CH{sub 4} (2.6 m{sup 3}/ton) and N{sub 2} (0.7 m{sup 3}/ton) at the same pressure (4 MPa; all as received basis). The geothermal gradient is also quite high at 55 C/km. A study has been conducted which simulates enhancement of methane recovery (ECBM) from these deposits using a new version of the TOUGH2 (version 2) reservoir simulator (ECBM-TOUGH2) that can handle non-isothermal, multi-phase flows of mixtures of water, CH{sub 4}, CO{sub 2} and N{sub 2}. The initial phase of the simulation is CH{sub 4} production for the first 5 years of the field history. The model indicates that methane production can be significantly improved (from less than 80% recovery to nearly 90%) through injection of CO{sub 2}. However, although an increase in the rate of CO{sub 2} injection increases the amount of CO{sub 2} sequestered, the methane recovery (because of earlier breakthrough with increasing injection rate) decreases. Modeling of pure N{sub 2} injection produced little enhanced CH{sub 4} production. The injection of a hypothetical flue gas mixture (CO{sub 2} and N{sub 2}) also produced little increase in CH{sub 4} production. This is related to the low adsorption capacity of the Huntly coal to N{sub 2} which results in almost instantaneous breakthrough into the production well. (author)

Kinetics of Chlorinated Hydrocarbon Degradation by Methylosinus trichosporium OB3b and Toxicity of Trichloroethylene

NARCIS (Netherlands)

Oldenhuis, Roelof; Oedzes, Johannes Y.; Waarde, Jacob J. van der; Janssen, Dick B.

The kinetics of the degradation of trichloroethylene (TCE) and seven other chlorinated aliphatic hydrocarbons by Methylosinus trichosporium OB3b were studied. All experiments were performed with cells grown under copper stress and thus expressing soluble methane monooxygenase. Compounds that were

Source apportionment of secondary organic aerosol in China using a regional source-oriented chemical transport model and two emission inventories.

Science.gov (United States)

Wang, Peng; Ying, Qi; Zhang, Hongliang; Hu, Jianlin; Lin, Yingchao; Mao, Hongjun

2018-06-01

A Community Multiscale Air Quality (CMAQ) model with source-oriented lumped SAPRC-11 (S11L) photochemical mechanism and secondary organic aerosol (SOA) module was applied to determine the contributions of anthropogenic and biogenic sources to SOA concentrations in China. A one-year simulation of 2013 using the Multi-resolution Emission Inventory for China (MEIC) shows that summer SOA are generally higher (10-15 μg m -3 ) due to large contributions of biogenic (country average 60%) and industrial sources (17%). In winter, SOA formation was mostly due to anthropogenic emissions from industries (40%) and residential sources (38%). Emissions from other countries in southeast China account for approximately 14% of the SOA in both summer and winter, and 46% in spring due to elevated open biomass burning in southeast Asia. The Regional Emission inventory in ASia v2.1 (REAS2) was applied in this study for January and August 2013. Two sets of simulations with the REAS2 inventory were conducted using two different methods to speciate total non-methane carbon into model species. One approach uses total non-methane hydrocarbon (NMHC) emissions and representative speciation profiles from the SPECIATE database. The other approach retains the REAS2 speciated species that can be directly mapped to S11L model species and uses source specific splitting factors to map other REAS2 lumped NMHC species. Biogenic emissions are still the most significant contributor in summer based on these two sets of simulations. However, contributions from the transportation sector to SOA in January are predicted to be much more important based on the two REAS2 emission inventories (∼30-40% vs. ∼5% by MEIC), and contributions from residential sources according to REAS2 was much lower (∼21-24% vs. ∼42%). These discrepancies in source contributions to SOA need to be further investigated as the country seeks for optimal emission control strategies to fight severe air pollution. Copyright �

Biogeochemistry of Halogenated Hydrocarbons

Science.gov (United States)

Adriaens, P.; Gruden, C.; McCormick, M. L.

2003-12-01

Halogenated hydrocarbons originate from both natural and industrial sources. Whereas direct anthropogenic emissions to the atmosphere and biosphere are often easy to assess, particularly when they are tied to major industrial activities, the attribution of emissions to other human activities (e.g., biomass burning), diffuse sources (e.g., atmospheric discharge, run off), and natural production (e.g., soils, fungi, algae, microorganisms) are difficult to quantify. The widespread occurrence of both alkyl and aryl halides in groundwater, surface water, soils, and various trophic food chains, even those not affected by known point sources, suggests a substantial biogeochemical cycling of these compounds (Wania and Mackay, 1996; Adriaens et al., 1999; Gruden et al., 2003). The transport and reactive fate mechanisms controlling their reactivity are compounded by the differences in sources of alkyl-, aryl-, and complex organic halides, and the largely unknown impact of biogenic processes, such as enzymatically mediated halogenation of organic matter, fungal production of halogenated hydrocarbons, and microbial or abiotic transformation reactions (e.g., Asplund and Grimvall, 1991; Gribble, 1996; Watling and Harper, 1998; Oberg, 2002). The largest source may be the natural halogenation processes in the terrestrial environment, as the quantities detected often exceed the amount that can be explained by human activities in the surrounding areas ( Oberg, 1998). Since biogeochemical processes result in the distribution of a wide range of halogenated hydrocarbon profiles, altered chemical structures, and isomer distributions in natural systems, source apportionment (or environmental forensics) can often only be resolved using multivariate statistical methods (e.g., Goovaerts, 1998; Barabas et al., 2003; Murphy and Morrison, 2002).This chapter will describe the widespread occurrence of halogenated hydrocarbons, interpret their distribution and biogeochemical cycling in light of

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

Science.gov (United States)

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.

MOLECULAR DIAGNOSTIC RATIOS TO ASSESS THE APPORTIONMENT OF PETROLEUM HYDROCARBONS CONTAMINANTION IN MARINE SEDIMENT

Directory of Open Access Journals (Sweden)

Agung Dhamar Syakti

2016-11-01

Full Text Available As maritime fulcrum nation, in Indonesia, marine environmental analytical chemistry field is still under developed. So that why, this review paper aims to provide basic understanding of the use some molecular diagnostic indices using n-alkanes indexes and polycyclic aromatic hydrocarbons (PAHs diagnostic ratios to estimate the source of apportionment of the hydrocarbons contamination and origin. The n-alkane chromatograms were then used to characterize the predominance of petrogenic or biogenic either terrestrial or aquatic. Furthermore, characterization allowed to discriminate riverine versus marine input. The occurrence of a broad unresolved complex mixture can be an evidence of biodegraded petroleum residues. For aromatic compounds, the prevalence of petrogenic, pyrolitic, and combustion-derived can be easily plotted by using isomers ratio calculation. This paper thus provides useful information on the hydrocarbon contamination origin, especially in marine sediments. Further researches should be undertaken in order to validate the use of molecular diagnostic ratio with isotopic approach.

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

Science.gov (United States)

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.

Detection of hydrocarbons in irradiated foods

International Nuclear Information System (INIS)

Miyahara, Makoto; Maitani, Tamio; Saito, Akiko; Kamimura, Tomomi; Nagasawa, Taeko; Kobayashi, Yasuo; Ito, Hitoshi

2003-01-01

The hydrocarbon method for the detection of irradiated foods is now recognized as the international technique. This method is based on radiolysis of fatty acids in food to give hydrocarbons. In order to expand this technique's application, ten foods (butter, cheese, chicken, pork, beef, tuna, dry shrimp, avocado, papaya, and mango) were irradiated in the range from 0.5 to 10 kGy and the hydrocarbons in them were detected. Recoveries of the hydrocarbons from most foods were acceptable (38-128%). Some hydrocarbons were found in non-irradiated foods, particularly, in butter, cheese, tuna, and shrimp. Seven irradiated foods, butter, cheese, chicken, beef, pork, tuna, dry shrimp, and avocado were detectable at their practical doses by measuring the appropriate marker hydrocarbons. In most case, marker hydrocarbon will be 1,7-hexadecadiene. However, the marker hydrocarbons produced only in irradiated foods varied from food to food; therefore, it is necessary to check a specific irradiated food for marker hydrocarbons. On the other hand, two irradiated foods (papaya and mango which were irradiated at their practical doses) were difficult to distinguish from non-irradiated foods using this method. (author)

Detection of hydrocarbons in irradiated foods

Energy Technology Data Exchange (ETDEWEB)

Miyahara, Makoto; Maitani, Tamio [National Inst. of Health Sciences, Tokyo (Japan); Saito, Akiko; Kamimura, Tomomi; Nagasawa, Taeko [Kitasato Univ., Sagamihara, Kanagawa (Japan). School of Allied Health Sciences; Kobayashi, Yasuo; Ito, Hitoshi [Japan Atomic Energy Research Inst., Takasaki, Gunma (Japan). Takasaki Radiation Establishment

2003-06-01

The hydrocarbon method for the detection of irradiated foods is now recognized as the international technique. This method is based on radiolysis of fatty acids in food to give hydrocarbons. In order to expand this technique's application, ten foods (butter, cheese, chicken, pork, beef, tuna, dry shrimp, avocado, papaya, and mango) were irradiated in the range from 0.5 to 10 kGy and the hydrocarbons in them were detected. Recoveries of the hydrocarbons from most foods were acceptable (38-128%). Some hydrocarbons were found in non-irradiated foods, particularly, in butter, cheese, tuna, and shrimp. Seven irradiated foods, butter, cheese, chicken, beef, pork, tuna, dry shrimp, and avocado were detectable at their practical doses by measuring the appropriate marker hydrocarbons. In most case, marker hydrocarbon will be 1,7-hexadecadiene. However, the marker hydrocarbons produced only in irradiated foods varied from food to food; therefore, it is necessary to check a specific irradiated food for marker hydrocarbons. On the other hand, two irradiated foods (papaya and mango which were irradiated at their practical doses) were difficult to distinguish from non-irradiated foods using this method. (author)

Pool Boiling of Hydrocarbon Mixtures on Water

Energy Technology Data Exchange (ETDEWEB)

Boee, R.

1996-09-01

In maritime transport of liquefied natural gas (LNG) there is a risk of spilling cryogenic liquid onto water. The present doctoral thesis discusses transient boiling experiments in which liquid hydrocarbons were poured onto water and left to boil off. Composition changes during boiling are believed to be connected with the initiation of rapid phase transition in LNG spilled on water. 64 experimental runs were carried out, 14 using pure liquid methane, 36 using methane-ethane, and 14 using methane-propane binary mixtures of different composition. The water surface was open to the atmosphere and covered an area of 200 cm{sup 2} at 25 - 40{sup o}C. The heat flux was obtained by monitoring the change of mass vs time. The void fraction in the boiling layer was measured with a gamma densitometer, and a method for adapting this measurement concept to the case of a boiling cryogenic liquid mixture is suggested. Significant differences in the boil-off characteristics between pure methane and binary mixtures revealed by previous studies are confirmed. Pure methane is in film boiling, whereas the mixtures appear to enter the transitional boiling regime with only small amounts of the second component added. The results indicate that the common assumption that LNG will be in film boiling on water because of the high temperature difference, may be questioned. Comparison with previous work shows that at this small scale the results are influenced by the experimental apparatus and procedures. 66 refs., 76 figs., 28 tabs.

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

Science.gov (United States)

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

2017-04-01

Apart from the sediment as the dominant source of methane in the aquatic realm the process of methane production in well-oxygenated waters has received considerable attention during the last years. The paradox of methane accumulation in these relatively shallow waters, commonly termed as "oceanic methane paradox", has been sporadically observed in lakes as well as in marine ecosystems like the Gulf of Mexico, the Black Sea, the Baltic Sea, Arctic waters or above the continental shelf off the coast of Spain and Africa. Even if this phenomenon has been described in the literature over the last decades, the potential sources of shallow methane accumulation are still controversially discussed. We report on methane enrichments that were observed during summer in the upper water column of the Gotland Basin, central Baltic Sea. In the eastern part of the basin methane concentrations just below the thermocline (in about 30 m water depth) varied between 15 and 77 nM, in contrast to the western part of the basin where no methane enrichments could be detected. Stable carbon isotope ratios of methane (delta 13C-CH4 of -67.6‰) clearly indicated its in situ biogenic origin. This is supported by clonal sequences from the depth with high methane concentrations in the eastern Gotland Basin, which cluster with the clade Methanomicrobiacea, a family of methanogenic Archaea. Hydroacoustic observation in combination with plankton net tows displayed a seston enrichment (size >100 micro meter) in a layer between 30-50 m depth. The dominant species in the phytoplankton, Dinophysis norvegica, was concentrated at 10-20 m depth, and showed higher concentrations in the eastern Gotland Basin in comparison with the western part of the basin. In contrast to the western Gotland Basin, the zooplankton community in the eastern part was dominated by the copepod species Temora longicornis. Laboratory incubations of a T. longicornis dominated seston fraction (>100 micro meter) sampled in the depth

Biogenic Emission Sources

Science.gov (United States)

Biogenic emissions sources come from natural sources and need to accounted for in photochemical grid models. They are computed using a model which utilizes spatial information on vegetation and land use.

Ice nuclei in marine air: biogenic particles or dust?

Directory of Open Access Journals (Sweden)

S. M. Burrows

2013-01-01

Full Text Available Ice nuclei impact clouds, but their sources and distribution in the atmosphere are still not well known. Particularly little attention has been paid to IN sources in marine environments, although evidence from field studies suggests that IN populations in remote marine regions may be dominated by primary biogenic particles associated with sea spray. In this exploratory model study, we aim to bring attention to this long-neglected topic and identify promising target regions for future field campaigns. We assess the likely global distribution of marine biogenic ice nuclei using a combination of historical observations, satellite data and model output. By comparing simulated marine biogenic immersion IN distributions and dust immersion IN distributions, we predict strong regional differences in the importance of marine biogenic IN relative to dust IN. Our analysis suggests that marine biogenic IN are most likely to play a dominant role in determining IN concentrations in near-surface-air over the Southern Ocean, so future field campaigns aimed at investigating marine biogenic IN should target that region. Climate-related changes in the abundance and emission of biogenic marine IN could affect marine cloud properties, thereby introducing previously unconsidered feedbacks that influence the hydrological cycle and the Earth's energy balance. Furthermore, marine biogenic IN may be an important aspect to consider in proposals for marine cloud brightening by artificial sea spray production.

Ecological, energetic and economical comparison of fermentation, composting and incineration of solid biogenic waste materials; Oekologischer, energetischer und oekonomischer Vergleich von Vergaerung, Kompostierung und Verbrennung fester biogener Abfallstoffe

Energy Technology Data Exchange (ETDEWEB)

Edelmann, W. [Arbeitsgemeinschaft Bioenergie GmbH, Arbi, Baar (Switzerland); Schleiss, K. [Umwelt- und Kompostberatung Schleiss, Baar (Switzerland)

2001-07-01

This study compares different technologies for the treatment of biogenic wastes, including open windrow and enclosed tunnel composting, anaerobic digestion, the combination of both these methods and burning in waste incineration plants. The methods are compared from the points of view of environmental impact, energy use and production, and economics. The environmental impact, calculated for normalised quantities of waste using the 'Ecoindicator 95+' tool, are discussed and the methane and carbon dioxide emissions of the different methods of treatment are compared. Also, the considerable differences to be found in the energy balances of the different systems are discussed in the light of efforts to substitute nuclear and fossil-fuel generated power. Cost and energetic comparisons are also made between compost and artificial fertilisers. The report is concluded with recommendations for adapting bio-technological methods for the treatment of wastes with an emphasis on anaerobic processes.

CHNC - the information and documentation platform of the non conventional hydrocarbons Centre. Technical files

International Nuclear Information System (INIS)

2015-07-01

This publication proposes a focus on various topics related to the exploitation of non conventional hydrocarbons. The first technical file addresses seismicity: definition of natural seismicity and induced seismicity, discussion of seismicity induced by hydraulic fracturing and by the re-injection of flow-back waters. Orders of magnitude of involved water volumes for hydraulic fracturing and flow-back water re-injection are given and regulatory aspects are evoked for hydraulic fracturing (definition of new rules after the Blackpool incident) and flow-back water re-injection (existing decrees in France). The second technical file addresses the techniques and evolutions in the field of hydraulic fracturing: brief presentation, detailed description of the principle and techniques of hydraulic fracturing with horizontal drilling, discussion of the used raw products (water, sand, additives, risks, progresses to be made), discussion of the environmental impact (fracture propagation and micro-seismic effects, seismicity, flow-back water treatment, gas emissions, noise pollution), discussion of the use of alternate fluids (fuel oil, jellied propane or butane, pure propane, hepta-fluoro-propane, CO 2 or liquid nitrogen based foams). Orders of magnitudes are given for the involved products and regulatory information is provided. The third file addresses water consumption and management: necessary water quantities for the exploitation of non conventional hydrocarbons, water supply, storage and evacuation, water use in agriculture, in energy production or in industry. Some figures are given and elements of the European directive on water are indicated. The fourth file addresses the protection of surface aquifers: risks of surface pollution, risks related to drilling operations, risks of surface water pollution related to hydraulic fracturing. Orders of magnitude and regulatory elements are given. The fifth technical file addresses the activity footprint and discusses how the

HyFlux - Part I: Regional Modeling of Methane Flux From Near-Seafloor Gas Hydrate Deposits on Continental Margins

Science.gov (United States)

MacDonald, I. R.; Asper, V.; Garcia, O. P.; Kastner, M.; Leifer, I.; Naehr, T.; Solomon, E.; Yvon-Lewis, S.; Zimmer, B.

2008-12-01

HyFlux - Part I: Regional modeling of methane flux from near-seafloor gas hydrate deposits on continental margins MacDonald, I.R., Asper, V., Garcia, O., Kastner, M., Leifer, I., Naehr, T.H., Solomon, E., Yvon-Lewis, S., and Zimmer, B. The Dept. of Energy National Energy Technology Laboratory (DOE/NETL) has recently awarded a project entitled HyFlux: "Remote sensing and sea-truth measurements of methane flux to the atmosphere." The project will address this problem with a combined effort of satellite remote sensing and data collection at proven sites in the Gulf of Mexico where gas hydrate releases gas to the water column. Submarine gas hydrate is a large pool of greenhouse gas that may interact with the atmosphere over geologic time to affect climate cycles. In the near term, the magnitude of methane reaching the atmosphere from gas hydrate on continental margins is poorly known because 1) gas hydrate is exposed to metastable oceanic conditions in shallow, dispersed deposits that are poorly imaged by standard geophysical techniques and 2) the consumption of methane in marine sediments and in the water column is subject to uncertainty. The northern GOM is a prolific hydrocarbon province where rapid migration of oil, gases, and brines from deep subsurface petroleum reservoirs occurs through faults generated by salt tectonics. Focused expulsion of hydrocarbons is manifested at the seafloor by gas vents, gas hydrates, oil seeps, chemosynthetic biological communities, and mud volcanoes. Where hydrocarbon seeps occur in depths below the hydrate stability zone (~500m), rapid flux of gas will feed shallow deposits of gas hydrate that potentially interact with water column temperature changes; oil released from seeps forms sea-surface features that can be detected in remote-sensing images. The regional phase of the project will quantify verifiable sources of methane (and oil) the Gulf of Mexico continental margin and selected margins (e.g. Pakistan Margin, South China Sea

A non-LTE model for the Jovian methane infrared emissions at high spectral resolution

Science.gov (United States)

Halthore, Rangasayi N.; Allen, J. E., Jr.; Decola, Philip L.

1994-01-01

High resolution spectra of Jupiter in the 3.3 micrometer region have so far failed to reveal either the continuum or the line emissions that can be unambiguously attributed to the nu(sub 3) band of methane (Drossart et al. 1993; Kim et al. 1991). Nu(sub 3) line intensities predicted with the help of two simple non-Local Thermodynamic Equilibrium (LTE) models -- a two-level model and a three-level model, using experimentally determined relaxation coefficients, are shown to be one to three orders of magnitude respectively below the 3-sigma noise level of these observations. Predicted nu(sub 4) emission intensities are consistent with observed values. If the methane mixing ratio below the homopause is assumed as 2 x 10(exp -3), a value of about 300 K is derived as an upper limit to the temperature of the high stratosphere at microbar levels.

BIOGENIC AMINES CONTENT IN DIFFERENT WINE SAMPLES

Directory of Open Access Journals (Sweden)

Attila Kántor

2015-02-01

Full Text Available Twenty-five samples of different Slovak wines before and after filtration were analysed in order to determine the content of eight biogenic amines (tryptamine, phenylalanine, putrescine, cadaverine, histamine, tyramine, spermidine and spermine. The method involves extraction of biogenic amines from wine samples with used dansyl chloride. Ultra-high performance liquid chromatography (UHPLC was used for determination of biogenic amines equipped with a Rapid Resolution High Definition (RRHD, DAD detectors and Extend-C18 LC column (50 mm x 3.0 mm ID, 1.8 μm particle size. In this study the highest level of biogenic amine in all wine samples represent tryptamine (TRM with the highest content 170.9±5.3 mg/L in Pinot Blanc wine. Phenylalanine (PHE cadaverine (CAD, histamine (HIS and spermidine (SPD were not detected in all wines; mainly SPD was not detected in 16 wines, HIS not detected in 14 wines, PHE and CAD not detected in 2 wines. Tyramine (TYR, spermine (SPN and putrescine (PUT were detected in all wines, but PUT and SPN in very low concentration. The worst wine samples with high biogenic amine content were Saint Laurent (BF, Pinot Blanc (S and Pinot Noir (AF.

Adsorption and methanation of carbon dioxide on a nickel/silica catalyst

Energy Technology Data Exchange (ETDEWEB)

Falconer, J.L.; Zagli, A.E.

1980-04-01

Temperature-programed desorption and reaction studies showed that increasing amounts of CO/sub 2/ adsorbed on silica-supported 6.9% nickel with increasing temperature to a maximum adsorption at approx. 443/sup 0/K, i.e., that the adsorption was activated; that CO/sub 2/ desorbed partly as CO/sub 2/ with the peak at 543/sup 0/K, and partly as CO with several peaks; that in the presence of hydrogen, nearly all adsorbed CO/sub 2/ desorbed as methane, and a small amount as CO; and that the methane desorption peaks from adsorbed CO and CO/sub 2/ both occurred at 473/sup 0/K. These results suggested that carbon dioxide adsorbed dissociatively as a carbon monoxide and an oxygen species. An observed absence of higher hydrocarbons in the methanation products of carbon dioxide was attributed to a high hydrogen/carbon monoxide surface ratio caused by the activated carbon dioxide adsorption.

First experience with the new solid methane moderator at the IBR-2 reactor

International Nuclear Information System (INIS)

Beliakov, A.A.; Shabalin, E.P.; Tretyakov, I.T.

2001-01-01

In the 1999 Fall the solid methane moderator (CM) has been installed and tested at full power at the IBR-2 pulsed reactor. Its main features are a beryllium reflector and a light water premoderator. Radiation load on the methane was three times as much as that of IPNS facility, namely, 0.1 W/g. Effects of temperature, operation time, concentration of a hydrogen scavenger, and annealing procedure on both neutron and service performances were studied. Maximum operation time of a newly loaded portion of methane was 4 days. In this time around 30% of methane is transformed into hydrogen, ethane, and high molecular hydrocarbons, and yet no deterioration in cold neutron intensity was detected. Among new knowledge, the most important are two facts observed: two-fold decrease in hydrogen formation rate when methane is poisoned with 2.5% to 5% of ethylene, and low formation rate of solid, inremovable products of radiolysis - (1.5/3)10 -7 g/J, which means that after 10 years of operation the methane chamber will be filled with only 100 g of residue. Gain of factor 20 in cold neutron flux was obtained as compared to the routine grooved light water moderator. Presently, it is the highest among the intense pulsed neutron sources. (author)

Just scratching the surface: If recent experiments are any indication, the real hydrocarbon bonanza could lie ten times deeper than our deepest wells

Energy Technology Data Exchange (ETDEWEB)

Smith, M.

2004-11-01

A recent report from the Lawrence Livermore National Laboratory suggests that methane could be formed in the Earth's searing upper mantle, at depths ten times deeper than the deepest wells ever drilled, containing virtually inexhaustible reserves of energy for future generations to exploit. While the findings are not expected to set off any immediate drilling rush, they do give rise to intriguing questions as to where future drilling will take place and the ultimate volumes of methane that might be found. Various scenarios have been advanced as to the portions of the mantle where conditions for methane formation are met. The most intriguing scenario would be if the mantle-derived hydrocarbons slowly replenished current reservoirs, since it is very difficult to imagine technologies that could significantly extend the currently reachable depths. There are also questions about the origin of these hydrocarbon deposits, and there is lively debate between adherents of biological and abiogenic formation theories. Indeed, there is substantial experimental evidence that hydrocarbons can form and be stable at the high pressures and temperatures of the Earth's mantle. Studies with a diamond anvil cell at temperatures from 500 to 1,500 degrees C and pressures between five and eleven gigapascals (50,000 to 110,000 times atmospheric pressure) demonstrate the existence of abiogenetic pathways for the formation of hydrocarbons and suggest that the hydrocarbon budget of the Earth may be larger than conventionally assumed. These experimental results confirm earlier findings by the late Cornell astronomer Thomas Gold and American physicists John Kenney and Russian researchers Kutcherov, Bendeliani and Aleksev in 2002. Notwithstanding the possibility that hydrocarbons may exist 100 km or deeper underground, it is most unlikely that they could be reached anytime soon. Even if the requisite technology were available, the economics would be prohibitive.

Laboratory Studies of Methane and Its Relationship to Prebiotic Chemistry.

Science.gov (United States)

Kobayashi, Kensei; Geppert, Wolf D; Carrasco, Nathalie; Holm, Nils G; Mousis, Olivier; Palumbo, Maria Elisabetta; Waite, J Hunter; Watanabe, Naoki; Ziurys, Lucy M

2017-08-01

To examine how prebiotic chemical evolution took place on Earth prior to the emergence of life, laboratory experiments have been conducted since the 1950s. Methane has been one of the key molecules in these investigations. In earlier studies, strongly reducing gas mixtures containing methane and ammonia were used to simulate possible reactions in the primitive atmosphere of Earth, producing amino acids and other organic compounds. Since Earth's early atmosphere is now considered to be less reducing, the contribution of extraterrestrial organics to chemical evolution has taken on an important role. Such organic molecules may have come from molecular clouds and regions of star formation that created protoplanetary disks, planets, asteroids, and comets. The interstellar origin of organics has been examined both experimentally and theoretically, including laboratory investigations that simulate interstellar molecular reactions. Endogenous and exogenous organics could also have been supplied to the primitive ocean, making submarine hydrothermal systems plausible sites of the generation of life. Experiments that simulate such hydrothermal systems where methane played an important role have consequently been conducted. Processes that occur in other Solar System bodies offer clues to the prebiotic chemistry of Earth. Titan and other icy bodies, where methane plays significant roles, are especially good targets. In the case of Titan, methane is both in the atmosphere and in liquidospheres that are composed of methane and other hydrocarbons, and these have been studied in simulation experiments. Here, we review the wide range of experimental work in which these various terrestrial and extraterrestrial environments have been modeled, and we examine the possible role of methane in chemical evolution. Key Words: Methane-Interstellar environments-Submarine hydrothermal systems-Titan-Origin of life. Astrobiology 17, 786-812.

Distribution of hydrocarbon-utilizing microorganisms and hydrocarbon biodegradation potentials in Alaskan continental shelf areas

International Nuclear Information System (INIS)

Roubal, G.; Atlas, R.M.

1978-01-01

Hydrocarbon-utilizing microogranisms were enumerated from Alaskan continental shelf areas by using plate counts and a new most-probable-number procedure based on mineralization of 14 C-labeled hydrocarbons. Hydrocarbon utilizers were ubiquitously distributed, with no significant overall concentration differences between sampling regions or between surface water and sediment samples. There were, however, significant seasonal differences in numbers of hydrocarbon utilizers. Distribution of hydrocarbon utilizers within Cook Inlet was positively correlated with occurrence of hydrocarbons in the environment. Hydrocarbon biodegradation potentials were measured by using 14 C-radiolabeled hydrocarbon-spiked crude oil. There was no significant correlation between numbers of hydrocarbon utilizers and hydrocarbon biodegradation potentials. The biodegradation potentials showed large seasonal variations in the Beaufort Sea, probably due to seasonal depletion of available nutrients. Non-nutrient-limited biodegradation potentials followed the order hexadecane > naphthalene >> pristane > benzanthracene. In Cook Inlet, biodegradation potentials for hexadecane and naphthalene were dependent on availability of inorganic nutrients. Biodegradation potentials for pristane and benzanthracene were restricted, probably by resistance to attack by available enzymes in the indigenous population

Anaerobic degradation of propane and butane by sulfate-reducing bacteria enriched from marine hydrocarbon cold seeps.

Science.gov (United States)

Jaekel, Ulrike; Musat, Niculina; Adam, Birgit; Kuypers, Marcel; Grundmann, Olav; Musat, Florin

2013-05-01

The short-chain, non-methane hydrocarbons propane and butane can contribute significantly to the carbon and sulfur cycles in marine environments affected by oil or natural gas seepage. In the present study, we enriched and identified novel propane and butane-degrading sulfate reducers from marine oil and gas cold seeps in the Gulf of Mexico and Hydrate Ridge. The enrichment cultures obtained were able to degrade simultaneously propane and butane, but not other gaseous alkanes. They were cold-adapted, showing highest sulfate-reduction rates between 16 and 20 °C. Analysis of 16S rRNA gene libraries, followed by whole-cell hybridizations with sequence-specific oligonucleotide probes showed that each enrichment culture was dominated by a unique phylotype affiliated with the Desulfosarcina-Desulfococcus cluster within the Deltaproteobacteria. These phylotypes formed a distinct phylogenetic cluster of propane and butane degraders, including sequences from environments associated with hydrocarbon seeps. Incubations with (13)C-labeled substrates, hybridizations with sequence-specific probes and nanoSIMS analyses showed that cells of the dominant phylotypes were the first to become enriched in (13)C, demonstrating that they were directly involved in hydrocarbon degradation. Furthermore, using the nanoSIMS data, carbon assimilation rates were calculated for the dominant cells in each enrichment culture.

Adsorption of chlorinated hydrocarbons from aqueous solutions by wetted and non-wetted synthetic sorbents:dynamics

NARCIS (Netherlands)

Rexwinkel, G.; Rexwinkel, Glenn; Berkhout, J.T.A.M.; Heesink, Albertus B.M.

2003-01-01

In the present investigation the dynamics of the adsorption of several chlorinated hydrocarbons onto wetted and non-wetted synthetic sorbents was studied. A single particle model was developed to describe the adsorption behavior. The values of the mass transfer coefficient, needed to describe the

Intolerance to dietary biogenic amines: A review

NARCIS (Netherlands)

Jansen, S.C.; Dusseldorp, M. van; Bottema, K.C.; Dubois, A.E.J.

2003-01-01

Objective: To evaluate the scientific evidence for purported intolerance to dietary biogenic amines. Data Sources: MEDLINE was searched for articles in the English language published between January 1966 and August 2001. The keyword biogenic amin* was combined with hypersens*, allerg*, intoler*, and

Intolerance to dietary biogenic amines : a review

NARCIS (Netherlands)

Jansen, SC; van Dusseldorp, M; Bottema, KC; Dubois, AEJ

Objective: To evaluate the scientific evidence for purported intolerance to dietary biogenic amines. Data Sources: MEDLINE was searched for articles in the English language published between January 1966 and August 2001. The keyword biogenic amin* was combined with hypersens*, allergen intoler*, and

Laboratory Studies of Methane and Its Relationship to Prebiotic Chemistry

Science.gov (United States)

Kobayashi, Kensei; Geppert, Wolf D.; Carrasco, Nathalie; Holm, Nils G.; Mousis, Olivier; Palumbo, Maria Elisabetta; Waite, J. Hunter; Watanabe, Naoki; Ziurys, Lucy M.

2017-08-01

To examine how prebiotic chemical evolution took place on Earth prior to the emergence of life, laboratory experiments have been conducted since the 1950s. Methane has been one of the key molecules in these investigations. In earlier studies, strongly reducing gas mixtures containing methane and ammonia were used to simulate possible reactions in the primitive atmosphere of Earth, producing amino acids and other organic compounds. Since Earth's early atmosphere is now considered to be less reducing, the contribution of extraterrestrial organics to chemical evolution has taken on an important role. Such organic molecules may have come from molecular clouds and regions of star formation that created protoplanetary disks, planets, asteroids, and comets. The interstellar origin of organics has been examined both experimentally and theoretically, including laboratory investigations that simulate interstellar molecular reactions. Endogenous and exogenous organics could also have been supplied to the primitive ocean, making submarine hydrothermal systems plausible sites of the generation of life. Experiments that simulate such hydrothermal systems where methane played an important role have consequently been conducted. Processes that occur in other Solar System bodies offer clues to the prebiotic chemistry of Earth. Titan and other icy bodies, where methane plays significant roles, are especially good targets. In the case of Titan, methane is both in the atmosphere and in liquidospheres that are composed of methane and other hydrocarbons, and these have been studied in simulation experiments. Here, we review the wide range of experimental work in which these various terrestrial and extraterrestrial environments have been modeled, and we examine the possible role of methane in chemical evolution.

Irradiation of Methane by Recoiling Fission-Fragments

Energy Technology Data Exchange (ETDEWEB)

Hall, G. R.; Galley, M. R. [Imperial College of Science and Technology, London (United Kingdom)

1963-11-15

Pure methane gas (containing <0.003% oxygen and <5 mg H{sub 2}O per m{sup 3}) has been irradiated at pressures ranging from 5 to 50 atmospheres pressure and at 30{sup o}C with recoiling fission - fragments. The gas is contained in a silica ampoule of volume about 9 cm{sup 3} and which also contains a platinum cylinder coated on the inside with 0.5 mg/cm{sup 2} highly enriched uranium oxide. When the ampoule is irradiated in a nuclear reactor with thermal neutrons, about half the fission-fragments recoil from the uranium and dissipate their energy in the methane. In a typical irradiation, methane at 10 atm pressure receives a dose of 5 x 10{sup 21} eV at an integrated reactor flux of 5 x 10{sup 15} neutrons/cm{sup 2}. Neutron flux i s measured by means of a gold-foil flux monitor. The activity of the Au{sup 198} is counted in a 4 {pi} proportional counter. The irradiation products have been detected by using beta-ionization detectors for gas-phase chromatography with suitable columns. The following products have been found: hydrogen, ethane, propane, n-butane, isobutane, n-pentane, iso-pentane, neo-pentane, the seven hexanes. Traces of higher hydrocarbons are undoubtedly present but the analysis of these has not been attempted. Hydrogen is present in greatest yield and the yields of the hydrocarbons decrease in the order given above. Despite previously reported yields of ethylene (G-value-0.1) from gamma and fast - electron irradiations, no ethylene or other unsaturated products have been detected in this work. It would have been possible to detect 10 ppm in the products. This is to be expected as any double bonds which may be produced would almost immediately be hydrogenated by the hydrogen present. Yields for hydrogen, ethane and propane lie within the range of values that have been reported by other workers for gamma and fast electron irradiations. (author)

Reconstructing Methane Emission Events in the Arctic Ocean: Observations from the Past to Present

Science.gov (United States)

Panieri, G.; Mienert, J.; Fornari, D. J.; Torres, M. E.; Lepland, A.

2015-12-01

Methane hydrates are ice-like crystals that are present along continental margins, occurring in the pore space of deep sediments or as massive blocks near the seafloor. They form in high pressure and low temperature environments constrained by thermodynamic stability, and supply of methane. In the Arctic, gas hydrates are abundant, and the methane released by their destabilization can affect local to global carbon budgets and cycles, ocean acidification, and benthic community survival. With the aim to locate in space and time the periodicity of methane venting, CAGE is engaged in a vast research program in the Arctic, a component of which comprises the analyses of numerous sediment cores and correlative geophysical and geochemical data from different areas. Here we present results from combined analyses of biogenic carbonate archives along the western Svalbard Margin, which reveal past methane venting events in this region. The reconstruction of paleo-methane discharge is complicated by precipitation of secondary carbonate on foraminifera shells, driven by an increase in alkalinity during anaerobic oxidation of methane (AOM). The biogeochemical processes involved in methane cycling and processes that drive methane migration affect the depth where AOM occurs, with relevance to secondary carbonate formation. Our results show the value and complexity of separating primary vs. secondary signals in bioarchives with relevance to understanding fluid-burial history in methane seep provinces. Results from our core analyses are integrated with observations made during the CAGE15-2 cruise in May 2015, when we deployed a towed vehicle equipped with camera, multicore and water sampling capabilities. The instrument design was based on the Woods Hole Oceanographic Institution (WHOI) MISO TowCam sled equipped with a deep-sea digital camera and CTD real-time system. Sediment sampling was visually-guided using this system. In one of the pockmarks along the Vestnesa Ridge where high

Potential sources of hydrocarbons and their microbial degradation in sediments from the deep geothermal Lusi site, Indonesia

Science.gov (United States)

Krueger, Martin; Mazzini, Adriano; Scheeder, Georg; Blumenberg, Martin

2017-04-01

The Lusi eruption represents one of the largest ongoing sedimentary hosted geothermal systems, which started in 2006 following an earthquake on Java Island. Since then it has been continuously producing hot and hydrocarbon rich mud from a central crater with peaks reaching 180.000 m3 per day. Numerous investigations focused on the study of microbial communities which thrive at offshore methane and oil seeps and mud volcanoes, however very little has been done on onshore seeping structures. Lusi represents a unique opportunity to complete a comprehensive study of onshore microbial communities fed by the seepage of CH4 as well as of liquid hydrocarbons originating from one or more km below the surface. While the source of the methane at Lusi is unambiuous, the origin of the seeping oil is still discussed. Both, source and maturity estimates from biomarkers, are in favor of a type II/III organic matter source. Likely the oils were formed from the studied black shales (deeper Ngimbang Fm.) which contained a Type III component in the Type II predominated organic matter. In all samples large numbers of active microorganisms were present. Rates for aerobic methane oxidation were high, as was the potential of the microbial communities to degrade different hydrocarbons. The data suggests a transition of microbial populations from an anaerobic, hydrocarbon-driven metabolism in fresher samples from center or from small seeps to more generalistic, aerobic microbial communities in older, more consolidated sediments. Ongoing microbial activity in crater sediment samples under high temperatures (80-95C) indicate a deep origin of the involved microorganisms. First results of molecular analyses of the microbial community compositions confirm the above findings. This study represents an initial step to better understand onshore seepage systems and provides an ideal analogue for comparison with the better investigated offshore structures.

Liquid hydrocarbons from coal beds – risk factor for the underground work environment - Case study

Directory of Open Access Journals (Sweden)

Tomescu Cristian

2017-01-01

Full Text Available Liquid hydrocarbons from the coal bed and surrounding rocks, besides the stored gases, methane, carbon dioxide, carbon oxide, generate the increase of the risk factor from the occupational health and safety point of view. If for reducing the gas concentrations level and the methane emissions in order to increase the safety in exploitation exist well-known solutions and methods, the oxidation or self-oxidation of the hydrocarbons from the coal bed generate a series of compounds, reaction products over maximum admitted concentrations which give birth to a toxic atmosphere and which is hazardous for workers, at the same time inducing an error in noting the occurrence of a spontaneous combustion phenomena, a major risk for the workers and for the mineral resource. This paper represents a case study performed in one underground mine unit from Jiu Valley and presents the analysis for underground environment factors monitoring and for solutions for diminishing the OHS risk factors.

Phase behaviour in water/hydrocarbon mixtures involved in gas production systems; etude des equilibres des systemes: eau-hydrocarbures-gaz acides dans le cadre de la production de gaz

Energy Technology Data Exchange (ETDEWEB)

Chapoy, A.

2004-11-15

Inside wells, natural gases frequently coexist with water. The gases are in equilibrium with the sub-adjacent aquifer. Many problems are associated with the presence of water during the production, transport and processing of natural gases. Accurate knowledge of the thermodynamic properties of the water/hydrocarbon and water-inhibitor/hydrocarbon equilibria near the hydrate forming conditions, at sub-sea pipeline conditions and during the transport is crucial for the petroleum industry. An apparatus based on a static/analytic method combined with a dilutor apparatus to calibrate on the gas chromatograph (GC) detectors with water was used to measure the water content of binary systems (i.e.: water - methane, ethane - water, nitrogen - water...) as well of a synthetic hydrocarbon gas mixture (i.e.: 94% methane, 4% ethane and 2% n-butane) with and without inhibitor. This same apparatus was also used generate data of methane, ethane, propane, n-butane and nitrogen solubility in water and also the solubilities of a synthetic mixture in water. In-house software has been developed in order to fit and model the experimental data. (author)

Non Thermal Plasma Assisted Catalytic Reactor for CO2 Methanation, Phase II

Data.gov (United States)

National Aeronautics and Space Administration — In situ production of methane as propellant by methanation of CO2, also called Sabatier reaction, is a key enabling technology required for sustainable and...

Experimental validation of large-eddy simulation for swirling methane-air non-premixed combustion

Energy Technology Data Exchange (ETDEWEB)

Hu, L.Y.; Luo, Y.H.; Xu, C.S. [Shanghai Jiaotong Univ. (China). School of Mechanical Engineering; Zhou, L.X. [Tsinghua Univ., Beijing (China). Dept. of Engineering Mechanics

2013-07-01

Large-eddy simulation of swirling methane-air non-premixed combustion was carried out using a Smagorinsky-Lilly subgrid scale stress model and a presumed-PDF fast-chemistry combustion model. The LES statistical results are validated by PIV, temperature and species concentration measurements made by the present authors. The results indicate that in the present case the presumed-PDF fast-chemistry combustion model is a fairish one. The instantaneous vorticity and temperature maps show clearly the development and the interaction between coherent structures and combustion.

Rapid analysis of dissolved methane, ethylene, acetylene and ethane using partition coefficients and headspace-gas chromatography.

Science.gov (United States)

Lomond, Jasmine S; Tong, Anthony Z

2011-01-01

Analysis of dissolved methane, ethylene, acetylene, and ethane in water is crucial in evaluating anaerobic activity and investigating the sources of hydrocarbon contamination in aquatic environments. A rapid chromatographic method based on phase equilibrium between water and its headspace is developed for these analytes. The new method requires minimal sample preparation and no special apparatus except those associated with gas chromatography. Instead of Henry's Law used in similar previous studies, partition coefficients are used for the first time to calculate concentrations of dissolved hydrocarbon gases, which considerably simplifies the calculation involved. Partition coefficients are determined to be 128, 27.9, 1.28, and 96.3 at 30°C for methane, ethylene, acetylene, and ethane, respectively. It was discovered that the volume ratio of gas-to-liquid phase is critical to the accuracy of the measurements. The method performance can be readily improved by reducing the volume ratio of the two phases. Method validation shows less than 6% variation in accuracy and precision except at low levels of methane where interferences occur in ambient air. Method detection limits are determined to be in the low ng/L range for all analytes. The performance of the method is further tested using environmental samples collected from various sites in Nova Scotia.

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

Science.gov (United States)

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.

Using Ionic Liquids in Selective Hydrocarbon Conversion Processes

Energy Technology Data Exchange (ETDEWEB)

Tang, Yongchun; Periana, Roy; Chen, Weiqun; van Duin, Adri; Nielsen, Robert; Shuler, Patrick; Ma, Qisheng; Blanco, Mario; Li, Zaiwei; Oxgaard, Jonas; Cheng, Jihong; Cheung, Sam; Pudar, Sanja

2009-09-28

This is the Final Report of the five-year project Using Ionic Liquids in Selective Hydrocarbon Conversion Processes (DE-FC36-04GO14276, July 1, 2004- June 30, 2009), in which we present our major accomplishments with detailed descriptions of our experimental and theoretical efforts. Upon the successful conduction of this project, we have followed our proposed breakdown work structure completing most of the technical tasks. Finally, we have developed and demonstrated several optimized homogenously catalytic methane conversion systems involving applications of novel ionic liquids, which present much more superior performance than the Catalytica system (the best-to-date system) in terms of three times higher reaction rates and longer catalysts lifetime and much stronger resistance to water deactivation. We have developed in-depth mechanistic understandings on the complicated chemistry involved in homogenously catalytic methane oxidation as well as developed the unique yet effective experimental protocols (reactors, analytical tools and screening methodologies) for achieving a highly efficient yet economically feasible and environmentally friendly catalytic methane conversion system. The most important findings have been published, patented as well as reported to DOE in this Final Report and our 20 Quarterly Reports.

Hydrocarbon contamination of coastal sediments from the Sfax area (Tunisia), Mediterranean Sea.

Science.gov (United States)

Louati, A; Elleuch, B; Kallel, M; Saliot, A; Dagaut, J; Oudot, J

2001-06-01

The coastal area off the city of Sfax (730,000 inhabitants), well-known for fisheries and industrial activities, receives high inputs of organic matter mostly anthropogenic. Eighteen stations were selected in the vicinity of the direct discharge of industrial sewage effluents in the sea in order to study the spatial distribution of the organic contamination. Surface sediments sampled in the shallow shelf were analysed for hydrocarbons by Fourier transform infrared spectroscopy, gas chromatography and gas chromatography/mass spectrometry. Total hydrocarbon distributions revealed high contamination as compared to other coastal Mediterranean sites, with an average concentration of 1865 ppm/dry weight sediment. Gas chromatographic distribution patterns, values of unresolved mixture/n-alkane ratio and distributions of steranes and hopanes confirmed a petroleum contamination of the Arabian light crude oil type. Biogenic compounds were also identified with a series of short-chain carbon-numbered n-alkenes in the carbon range 16-24.

Framework for Assessing Biogenic CO2 Emissions from Stationary Sources

Science.gov (United States)

This revision of the 2011 report, Accounting Framework for Biogenic CO2 Emissions from Stationary Sources, evaluates biogenic CO2 emissions from stationary sources, including a detailed study of the scientific and technical issues associated with assessing biogenic carbon dioxide...

Decentralized production of hydrogen from hydrocarbons with reduced CO2 emission

International Nuclear Information System (INIS)

Nazim Muradov; Franklyn Smith; Cunping Huang; Ali T-Raissi

2006-01-01

Currently, most of the industrial hydrogen production is based on steam methane reforming process that releases significant amount of CO 2 into the atmosphere. CO 2 sequestration is one approach to solving the CO 2 emission problem for large centralized hydrogen plants, but it would be impractical for decentralized H 2 production units. The objective of this paper is to explore new routes to hydrogen production from natural gas without (or drastically reduced) CO 2 emissions. One approach analyzed in this paper is based on thermo-catalytic decomposition (TCD) of hydrocarbons (e.g., methane) to hydrogen gas and elemental carbon. The paper discusses some technological aspects of the TCD process development: (1) thermodynamic analysis of TCD using AspenPlus chemical process simulator, (2) heat input options to the endothermic process, (3) catalyst activity issues, etc. Production of hydrogen and carbon via TCD of methane was experimentally verified using carbon-based catalysts. (authors)

Tröger’s Base Ladder Polymer for Membrane-Based Hydrocarbon Separation

KAUST Repository

Alhazmi, Abdulrahman

2017-05-01

The use of polymeric membranes for natural gas separation has rapidly increased during the past three decades, particularly for carbon dioxide separation from natural gas. Another valuable application is the separation of heavy hydrocarbons from methane (fuel gas conditioning), more importantly for remote area and off-shore applications. A new potential polymeric membrane that might be utilized for natural gas separations is a Tröger’s base ladder polymer (PIM-Trip-TB-2). This glassy polymeric membrane was synthesized by the polymerization reaction of 9, 10-dimethyl-2,6 (7) diaminotriptycene with dimethoxymethane. In this research, the polymer was selected due to its high surface area and highly interconnected microporous structure. Sorption isotherms of nitrogen (N2), oxygen (O¬2), methane (CH4), carbon dioxide (CO2), ethane (C2H6), propane (C3H8), and n-butane (n-C4H10) were measured at 35 °C over a range of pressures using a Hiden Intelligent Gravimetric Analyzer, IGA. The more condensable gases (C2H6, CO2, C3H8, and n-C4H10) showed high solubility due to their high affinity to the polymer matrix. The permeation coefficients were determined for various gases at 35 °C and pressure difference of 5 bar via the constant-pressure/variable-volume method. The PIM-Trip-TB-2 film exhibited high performance for several high-impact applications, such as O2/N2, H2/N2 and H2/CH4. Also, physical aging for several gases was examined by measuring the permeability coefficients at different periods of time. Moreover, a series of mixed-gas permeation tests was performed using 2 vol.% n-C4H10/98 vol.% CH4 and the results showed similar transport characteristics to other microporous polymers with pores of less than 2 nm. The work performed in this research suggested that PIM-Trip-TB-2 is suitable for the separation of: (i) higher hydrocarbons from methane and (ii) small, non-condensable gases such as O2/N2 and H2/CH4.

BIOGENIC AMINES CONTENT IN SELECTED WINES DURING WINEMAKING

Directory of Open Access Journals (Sweden)

Radka Flasarová

2012-02-01

Full Text Available The aim of this study was to describe the development of selected biogenic amines (histamine; tyramine; phenylethylamine; putrescine; agmatine; and cadaverine during the winemaking in 10 selected species grown in Central Europe in 2008. The analysis was performed using ion-exchange chromatography by the sodium-citrate buffers with the post-column ninhydrin derivatization and photometric detection. A comparison of the content of biogenic amines in red and wine varieties showed that red wines have higher concentrations of biogenic amines.

Oceanic hydrates: more questions than answers

International Nuclear Information System (INIS)

Laherrere, Jean

2000-01-01

Methane hydrates create problems by blocking pipelines and casing; they are also accused of contributing to environmental problems (e.g. global warming). Methane hydrates are also found in permafrost areas and in oceanic sediments where the necessary temperature and pressure for stability occur. Claims for the widespread occurrence in thick oceanic deposits are unfounded: apparently indirect evidence from seismic reflectors, seismic hydrocarbon indicators, logs and free samples is unreliable. At one time, hydrate was seen as a static, biogenic, continuous, huge resource but that view is changing to one of a dynamic, overpressurised, discontinuous and unreliable resource. Only Japan and India are currently showing any serious interest in hydrates. Academic research has raised more questions than answers. It is suggested that more hard exploratory evidence rather than theoretical study is required

Biogenic nonmethane hydrocarbon emissions estimated from tethered balloon observations

Science.gov (United States)

Davis, K. J.; Lenschow, D. H.; Zimmerman, P. R.

1994-01-01

A new technique for estimating surface fluxes of trace gases, the mixed-layer gradient technique, is used to calculate isoprene and terpene emissions from forests. The technique is applied to tethered balloon measurements made over the Amazon forest and a pine-oak forest in Alabama at altitudes up to 300 m. The observations were made during the dry season Amazon Boundary Layer Experiment (ABLE 2A) and the Rural Oxidants in the Southern Environment 1990 experiment (ROSE I). Results from large eddy simulations of scalar transport in the clear convective boundary layer are used to infer fluxes from the balloon profiles. Profiles from the Amazon give a mean daytime emission of 3630 +/- 1400 micrograms isoprene sq m/h, where the uncertainty represents the standard deviation of the mean of eight flux estimates. Twenty profiles from Alabama give emissions of 4470 +/- 3300 micrograms isoprene sq m/h, 1740 +/- 1060 micrograms alpha-pinene sq m/h, and 790 +/- 560 micrograms beta-pinene sq m/h, respectively. These results are in agreement with emissions derived from chemical budgets. The emissions may be overestimated because of uncertainty about how to incorporate the effects of the canopy on the mixed-layer gradients. The large variability in these emission estimates is probably due to the relatively short sampling times of the balloon profiles, though spatially heterogeneous emissions may also play a role. Fluxes derived using this technique are representative of an upwind footprint of several kilometers and are independent of hydrocarbon oxidation rate and mean advection.

Solubility of Methane, Ethane, and Propane in Pure Water Using New Binary Interaction Parameters

Directory of Open Access Journals (Sweden)

Masoud Behrouz

2015-07-01

Full Text Available Solubility of hydrocarbons in water is important due to ecological concerns and new restrictions on the existence of organic pollutants in water streams. Also, the creation of a thermodynamic model has required an advanced study of the phase equilibrium between water (as a basis for the widest spread muds and amines and gas hydrocarbon phases in wide temperature and pressure ranges. Therefore, it is of great interest to develop semi-empirical correlations, charts, or thermodynamic models for estimating the solubility of hydrocarbons in liquid water. In this work, a thermodynamic model based on Mathias modification of Sova-Redlich-Kwong (SRK equation of state is suggested using classical mixing rules with new binary interaction parameters which were used for two-component systems of hydrocarbons and water. Finally, the model results and their deviations in comparison with the experimental data are presented; these deviations were equal to 5.27, 6.06, and 4.1% for methane, ethane, and propane respectively.

Study of hydrocarbons in bottom sediments of the northern Dvina River-White Sea geochemical barrier during spring flood. Volume 2

International Nuclear Information System (INIS)

Nemirovskaya, I.; Shevchenko, V.

2007-01-01

The Northern Dvina in Northern Russia is the main river of the White Sea reservoir. The water discharge is 108 km 3 per year. With active shipping and several large pulp and paper mills that operate in the region, the river is a supplier of polluting substances. Weathered oil and pyrogenic compounds dominate the composition of hydrocarbons. During flooding, the Northern Dvina - Dvina Bay geochemical barrier becomes a filter, which prevents pollutants from penetrating to the White Sea. This paper summarized data on the concentration and composition of hydrocarbons, aliphatic hydrocarbons (AHC) and polycyclic aromatic hydrocarbons (PAH) in the marine water and bottom sediments at the mouth of the Northern Dvina/White Sea. Nearly similar concentrations of organic compounds were found in the Northern Dvina River water and in the near-mouth White Sea water area. However, their distribution conforms to the marginal filter rules. Natural terrigenous hydrocarbon compounds were found to dominate in all forms. Biogenic autochthonous hydrocarbons were detected in the near-shore areas and in the outer zone of the marginal filter of the Northern Dvina River, where PAH are formed together with AHC. 20 refs., 2 tabs., 4 figs

Reconciling Top-Down and Bottom-Up Estimates of Oil and Gas Methane Emissions in the Barnett Shale

Science.gov (United States)

Hamburg, S.

2015-12-01

Top-down approaches that use aircraft, tower, or satellite-based measurements of well-mixed air to quantify regional methane emissions have typically estimated higher emissions from the natural gas supply chain when compared to bottom-up inventories. A coordinated research campaign in October 2013 used simultaneous top-down and bottom-up approaches to quantify total and fossil methane emissions in the Barnett Shale region of Texas. Research teams have published individual results including aircraft mass-balance estimates of regional emissions and a bottom-up, 25-county region spatially-resolved inventory. This work synthesizes data from the campaign to directly compare top-down and bottom-up estimates. A new analytical approach uses statistical estimators to integrate facility emission rate distributions from unbiased and targeted high emission site datasets, which more rigorously incorporates the fat-tail of skewed distributions to estimate regional emissions of well pads, compressor stations, and processing plants. The updated spatially-resolved inventory was used to estimate total and fossil methane emissions from spatial domains that match seven individual aircraft mass balance flights. Source apportionment of top-down emissions between fossil and biogenic methane was corroborated with two independent analyses of methane and ethane ratios. Reconciling top-down and bottom-up estimates of fossil methane emissions leads to more accurate assessment of natural gas supply chain emission rates and the relative contribution of high emission sites. These results increase our confidence in our understanding of the climate impacts of natural gas relative to more carbon-intensive fossil fuels and the potential effectiveness of mitigation strategies.

Light hydrocarbons vertical profiles and fluxes in a french rural area

Science.gov (United States)

Kanakidou, M.; Bonsang, B.; Lambert, G.

By means of manned hot air balloon flights, in July 1986, an experiment was conducted in a rural area of southwest France in order to determine the production at ground level of non-methane hydrocarbons in the C 2-C 6 range. Flux determinations were based on vertical profiles before and after the development of a temperature inversion layer which allowed the measurement of the NMHC accumulation close to ground level. The main species produced in the late afternoon were acetylene, propane, ethene, propene and ethane with production rates of the order of 0.5 to 2 × 10 -4g of C m -2 h -1. Isoprene was found to be the main other unsaturated species also produced. The fluxes and the atmospheric content of the air column before the inversion are consistent with an average OH radical concentration of 2 × 10 6 cm -3.

Effect of vegetation removal and water table drawdown on the non-methane biogenic volatile organic compound emissions in boreal peatland microcosms

Science.gov (United States)

Faubert, Patrick; Tiiva, Päivi; Rinnan, Åsmund; Räty, Sanna; Holopainen, Jarmo K.; Holopainen, Toini; Rinnan, Riikka

2010-11-01

Biogenic volatile organic compound (BVOC) emissions are important in the global atmospheric chemistry and their feedbacks to global warming are uncertain. Global warming is expected to trigger vegetation changes and water table drawdown in boreal peatlands, such changes have only been investigated on isoprene emission but never on other BVOCs. We aimed at distinguishing the BVOCs released from vascular plants, mosses and peat in hummocks (dry microsites) and hollows (wet microsites) of boreal peatland microcosms maintained in growth chambers. We also assessed the effect of water table drawdown (-20 cm) on the BVOC emissions in hollow microcosms. BVOC emissions were measured from peat samples underneath the moss surface after the 7-week-long experiment to investigate whether the potential effects of vegetation and water table drawdown were shown. BVOCs were sampled using a conventional chamber method, collected on adsorbent and analyzed with GC-MS. In hummock microcosms, vascular plants increased the monoterpene emissions compared with the treatment where all above-ground vegetation was removed while no effect was detected on the sesquiterpenes, other reactive VOCs (ORVOCs) and other VOCs. Peat layer from underneath the surface with intact vegetation had the highest sesquiterpene emissions. In hollow microcosms, intact vegetation had the highest sesquiterpene emissions. Water table drawdown decreased monoterpene and other VOC emissions. Specific compounds could be closely associated to the natural/lowered water tables. Peat layer from underneath the surface of hollows with intact vegetation had the highest emissions of monoterpenes, sesquiterpenes and ORVOCs whereas water table drawdown decreased those emissions. The results suggest that global warming would change the BVOC emission mixtures from boreal peatlands following changes in vegetation composition and water table drawdown.

Biogenic sulfur compounds and the global sulfur cycle

International Nuclear Information System (INIS)

Aneja, V.P.; Aneja, A.P.; Adams, D.F.

1982-01-01

Field measurements of biogenic sulfur compounds shows a great variation in concentrations and emission rates for H 2 S, DMS, CS 2 and COS. Measurements by the chamber method and estimates from micrometeorological sampling are employed to determine the earth-atmosphere flux of these gases. Much of the variation can be attributed to differences of climate and surface conditions, with marshes being a large source of biogenic sulfur (mean contribution 4 x 10 to the 6th ton/year maximum contribution 142 x 10 to the 6th ton/year). Considering that the estimated biogenic contribution needed to balance the global sulfur cycle ranges from 40- 230 x 10 to the 6th tons/year, the mean values are not sufficient to balance this cycle. Further experimental investigations are suggested in order to characterize the biogenic processes adequately

The MUMBA campaign: measurements of urban, marine and biogenic air

Science.gov (United States)

Paton-Walsh, Clare; Guérette, Élise-Andrée; Kubistin, Dagmar; Humphries, Ruhi; Wilson, Stephen R.; Dominick, Doreena; Galbally, Ian; Buchholz, Rebecca; Bhujel, Mahendra; Chambers, Scott; Cheng, Min; Cope, Martin; Davy, Perry; Emmerson, Kathryn; Griffith, David W. T.; Griffiths, Alan; Keywood, Melita; Lawson, Sarah; Molloy, Suzie; Rea, Géraldine; Selleck, Paul; Shi, Xue; Simmons, Jack; Velazco, Voltaire

2017-06-01

The Measurements of Urban, Marine and Biogenic Air (MUMBA) campaign took place in Wollongong, New South Wales (a small coastal city approximately 80 km south of Sydney, Australia) from 21 December 2012 to 15 February 2013. Like many Australian cities, Wollongong is surrounded by dense eucalyptus forest, so the urban airshed is heavily influenced by biogenic emissions. Instruments were deployed during MUMBA to measure the gaseous and aerosol composition of the atmosphere with the aim of providing a detailed characterisation of the complex environment of the ocean-forest-urban interface that could be used to test the skill of atmospheric models. The gases measured included ozone, oxides of nitrogen, carbon monoxide, carbon dioxide, methane and many of the most abundant volatile organic compounds. The aerosol characterisation included total particle counts above 3 nm, total cloud condensation nuclei counts, mass concentration, number concentration size distribution, aerosol chemical analyses and elemental analysis.The campaign captured varied meteorological conditions, including two extreme heat events, providing a potentially valuable test for models of future air quality in a warmer climate. There was also an episode when the site sampled clean marine air for many hours, providing a useful additional measure of the background concentrations of these trace gases within this poorly sampled region of the globe. In this paper we describe the campaign, the meteorology and the resulting observations of atmospheric composition in general terms in order to equip the reader with a sufficient understanding of the Wollongong regional influences to use the MUMBA datasets as a case study for testing a chemical transport model. The data are available from PANGAEA (pangaea.de/10.1594/PANGAEA.871982" target="_blank">http://doi.pangaea.de/10.1594/PANGAEA.871982).

Report on a survey in fiscal 1999. Direct oxidation of hydrocarbons by manifestation of functions of methane mono-oxygenase (MMO); 1999 nendo metamonookishinaze (MMO) no kino hatsugen ni yoru tanka suiso no chokusetsu sanka seika hokokusho

Energy Technology Data Exchange (ETDEWEB)

NONE

2000-03-01

The metallic enzyme, methane mono-oxygenase (MMO) collected from methanotrophic bacteria, may perform a reaction that has a possibility to proceed direct conversion from methane to methanol under normal temperatures and pressures. However, its utilization of biological bacteria makes massive cultivation and handling difficult, not having realized its practical use. Therefore, research and development has been carried out on a process that can convert directly and selectively hydrocarbons including methane under normal temperatures and pressures, mimicking the excellent functions of MMO. To achieve the development, surveys and discussions were given on the following elementary researches: elucidation of the reaction mechanism in the activation point in microorganism enzymes; analysis of structures in microorganism MMO; creation of a technology to develop a bio-mimetic catalyst; improvement in selectivity of the bio-mimetic catalyst; and international joint research (basic analysis of the catalyst mechanism). As a result, technological problems in developing the mimetic catalyst were put into order, and guidelines and measures for specific catalyst designing are being proposed. Furthermore, a way was opened for international joint research with the complex synthesis research group in CNRS in France, and progress into the step of demonstrating and discussing the feasibility thereof is now ready. (NEDO)

Diverse origins of Arctic and Subarctic methane point source emissions identified with multiply-substituted isotopologues

Science.gov (United States)

Douglas, P. M. J.; Stolper, D. A.; Smith, D. A.; Walter Anthony, K. M.; Paull, C. K.; Dallimore, S.; Wik, M.; Crill, P. M.; Winterdahl, M.; Eiler, J. M.; Sessions, A. L.

2016-09-01

Methane is a potent greenhouse gas, and there are concerns that its natural emissions from the Arctic could act as a substantial positive feedback to anthropogenic global warming. Determining the sources of methane emissions and the biogeochemical processes controlling them is important for understanding present and future Arctic contributions to atmospheric methane budgets. Here we apply measurements of multiply-substituted isotopologues, or clumped isotopes, of methane as a new tool to identify the origins of ebullitive fluxes in Alaska, Sweden and the Arctic Ocean. When methane forms in isotopic equilibrium, clumped isotope measurements indicate the formation temperature. In some microbial methane, however, non-equilibrium isotope effects, probably related to the kinetics of methanogenesis, lead to low clumped isotope values. We identify four categories of emissions in the studied samples: thermogenic methane, deep subsurface or marine microbial methane formed in isotopic equilibrium, freshwater microbial methane with non-equilibrium clumped isotope values, and mixtures of deep and shallow methane (i.e., combinations of the first three end members). Mixing between deep and shallow methane sources produces a non-linear variation in clumped isotope values with mixing proportion that provides new constraints for the formation environment of the mixing end-members. Analyses of microbial methane emitted from lakes, as well as a methanol-consuming methanogen pure culture, support the hypothesis that non-equilibrium clumped isotope values are controlled, in part, by kinetic isotope effects induced during enzymatic reactions involved in methanogenesis. Our results indicate that these kinetic isotope effects vary widely in microbial methane produced in Arctic lake sediments, with non-equilibrium Δ18 values spanning a range of more than 5‰.

Anaerobic oxidation of methane at a marine methane seep in a forearc sediment basin off Sumatra, Indian Ocean

Directory of Open Access Journals (Sweden)

Michael eSiegert

2011-12-01

Full Text Available 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 centre 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 AOM was reflected by 13C depleted isotopic signatures of dissolved inorganic carbon (DIC. The anaerobic conversion of methane to CO2 was confirmed in a 13C-labelling experiment. Methane fuelled a vital microbial and invertebrate community which was reflected in cell numbers of up to 4 x 109 cells cm 3 sediment and 13C depleted guts of crabs populating the seep area. The microbial community was analysed by total cell counting, catalyzed reporter deposition – fluorescence in situ hybridisation (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.

Production of hydrogen via conversion of hydrocarbons using a microwave plasma

International Nuclear Information System (INIS)

Jasinski, Mariusz; Dors, Miroslaw; Nowakowska, Helena; Mizeraczyk, Jerzy; Nichipor, Gerietta V

2011-01-01

In this paper, results of hydrogen production from hydrocarbons in an atmospheric pressure microwave plasma are presented. As sources of hydrogen, both methane CH 4 and tetrafluoroethane C 2 H 2 F 4 were tested. A new waveguide-based nozzleless cylinder-type microwave plasma source was used to convert hydrocarbons into hydrogen. The processed gaseous hydrocarbons were introduced into the plasma by four gas ducts which formed a swirl flow in the plasma reactor. The absorbed microwave power was up to 5 kW. The gas flow rate was up to 212 L min -1 . The hydrogen mass yield rate and the corresponding energetic hydrogen mass yield were up to 866 g[H 2 ] h -1 and 577 g [H 2 ] kWh -1 of microwave energy absorbed by the plasma, respectively. These parameters are better than our previous results when nitrogen was used as a swirl gas and much better than those typical for other plasma methods of hydrogen production (electron beam, gliding arc, plasmatron).

A suggestion to assess spilled hydrocarbons as a greenhouse gas source

Energy Technology Data Exchange (ETDEWEB)

McAlexander, Benjamin L., E-mail: bmcalexander@trihydro.com

2014-11-15

Petroleum-contaminated site management typically counts destruction of hydrocarbons by either natural or engineered processes as a beneficial component of remediation. While such oxidation of spilled hydrocarbons is often necessary for achieving risk reduction for nearby human and ecological receptors, site assessments tend to neglect that this also means that the pollutants are converted to greenhouse gases and emitted to the atmosphere. This article presents a suggestion that the current and long term greenhouse gas emissions from spilled hydrocarbons be incorporated to petroleum site assessments. This would provide a more complete picture of pollutant effects that could then be incorporated to remedial objectives. At some sites, this additional information may affect remedy selection. Possible examples include a shift in emphasis to remedial technologies that reduce pollutant greenhouse gas effects (e.g., by conversion of methane to carbon dioxide in the subsurface), and a more holistic context for considering remedial technologies with low emission footprints.

Recent changes in carbon dioxide, carbon monoxide and methane and the implications for global climate change

Energy Technology Data Exchange (ETDEWEB)

Novelli, P.C.; Conway, T.J.; Dlugokencky, E.J.; Tans, P.P. [National Oceanic and Atmospheric Administration, Boulder, CO (United States). Climate Monitoring and Diagnostics Lab.

1995-01-01

The article reviews figures for published data on recent changes of atmospheric levels of carbon dioxide, carbon monoxide and methane in terms of their sources and sinks. The largest source of CO{sub 2} is the combustion of fossil fuels, followed by emissions from deforestation and the oxidation of CO to CO{sub 2}. Carbon monoxide has an indirect influence on the earth`s radiative balance, as if levels of CO increase, levels of OH radicals decline which affects removal of other gases oxidised by this radical, notably CH{sub 4}. Major sources of CO are fossil fuel combustion, emissions from biomass, and oxidation of atmospheric CH{sub 4} and other non-methane hydrocarbons. The latest measurements suggest the depressed growth rates of CO{sub 2}, CO and CH{sub 4} have began to recover. Reasons for this are suggested. Future monitoring of atmospheric species in laboratories around the world, coupled with information on the isotopic signature of the trace gases, will improve our understanding of possible causes for trends in these gases. This will be invaluable in making policy decisions regarding future climate change. 34 refs., 4 figs.

Hydrocarbon-degrading bacteria isolation and surfactant influence ...

African Journals Online (AJOL)

Hydrocarbons are substantially insoluble in water, often remaining partitioned in the non-aqueous phase liquid (NAPL). However, there had been little or no attempts to advance the bioavailability of hydrocarbons through the use of surfactants. This study was conducted based on the need to isolate hydrocarbon degrading ...

Steady-state and transient hydrocarbon production in graphite by low energy impact of atomic and molecular deuterium projectiles

International Nuclear Information System (INIS)

Zhang, H.; Meyer, F.W.

2009-01-01

We report measurements of steady-state yields of methyl, methane and heavier hydrocarbons for deuterium atomic and molecular ions incident on ATJ graphite, HOPG, and a-C:D thin films in the energy range 10-200 eV/D. The yields were determined using a QMS technique in conjunction with calibrated hydrocarbon leaks. We have also studied transient hydrocarbon production and hydrogen (deuterium) re-emission for 80 and 150 eV/D D + , D 2 + , and D 3 + projectiles incident on ATJ graphite surfaces pre-loaded to steady state by 20 eV/D beams of the corresponding species. Immediately after starting the higher-energy beams, transient hydrocarbon and D 2 re-emission yields significantly larger than steady-state values were observed, which exponentially decayed as a function of beam fluence. The initial yield values were related to the starting hydrocarbon and deuterium densities in the prepared sample, while the exponential decay constants provided information on the hydrocarbon kinetic release and hydrogen (deuterium) detrapping cross-sections.

Methyl chavicol: characterization of its biogenic emission rate

NARCIS (Netherlands)

Bouvier-Brown, N.C.; Goldstein, A.H.; Worton, D.R.; Matross, D.M.; Gilman, J.B.; Kuster, W.C.; Welsh-Bon, D.; Warneke, C.; de Gouw, J.A.; Cahill, M.J.; Holzinger, R.

2009-01-01

We report measurements of ambient atmospheric mixing ratios for methyl chavicol and determine its biogenic emission rate. Methyl chavicol, a biogenic oxygenated aromatic compound, is abundant within and above Blodgett Forest, a ponderosa pine forest in the Sierra Nevada Mountains of California.

Large emissions from floodplain trees close the Amazon methane budget

Science.gov (United States)

Pangala, Sunitha R.; Enrich-Prast, Alex; Basso, Luana S.; Peixoto, Roberta Bittencourt; Bastviken, David; Hornibrook, Edward R. C.; Gatti, Luciana V.; Marotta, Humberto; Calazans, Luana Silva Braucks; Sakuragui, Cassia Mônica; Bastos, Wanderley Rodrigues; Malm, Olaf; Gloor, Emanuel; Miller, John Bharat; Gauci, Vincent

2017-12-01

Wetlands are the largest global source of atmospheric methane (CH4), a potent greenhouse gas. However, methane emission inventories from the Amazon floodplain, the largest natural geographic source of CH4 in the tropics, consistently underestimate the atmospheric burden of CH4 determined via remote sensing and inversion modelling, pointing to a major gap in our understanding of the contribution of these ecosystems to CH4 emissions. Here we report CH4 fluxes from the stems of 2,357 individual Amazonian floodplain trees from 13 locations across the central Amazon basin. We find that escape of soil gas through wetland trees is the dominant source of regional CH4 emissions. Methane fluxes from Amazon tree stems were up to 200 times larger than emissions reported for temperate wet forests and tropical peat swamp forests, representing the largest non-ebullitive wetland fluxes observed. Emissions from trees had an average stable carbon isotope value (δ13C) of -66.2 ± 6.4 per mil, consistent with a soil biogenic origin. We estimate that floodplain trees emit 15.1 ± 1.8 to 21.2 ± 2.5 teragrams of CH4 a year, in addition to the 20.5 ± 5.3 teragrams a year emitted regionally from other sources. Furthermore, we provide a ‘top-down’ regional estimate of CH4 emissions of 42.7 ± 5.6 teragrams of CH4 a year for the Amazon basin, based on regular vertical lower-troposphere CH4 profiles covering the period 2010-2013. We find close agreement between our ‘top-down’ and combined ‘bottom-up’ estimates, indicating that large CH4 emissions from trees adapted to permanent or seasonal inundation can account for the emission source that is required to close the Amazon CH4 budget. Our findings demonstrate the importance of tree stem surfaces in mediating approximately half of all wetland CH4 emissions in the Amazon floodplain, a region that represents up to one-third of the global wetland CH4 source when trees are combined with other emission sources.

Large emissions from floodplain trees close the Amazon methane budget.

Science.gov (United States)

Pangala, Sunitha R; Enrich-Prast, Alex; Basso, Luana S; Peixoto, Roberta Bittencourt; Bastviken, David; Hornibrook, Edward R C; Gatti, Luciana V; Marotta, Humberto; Calazans, Luana Silva Braucks; Sakuragui, Cassia Mônica; Bastos, Wanderley Rodrigues; Malm, Olaf; Gloor, Emanuel; Miller, John Bharat; Gauci, Vincent

2017-12-14

Wetlands are the largest global source of atmospheric methane (CH 4 ), a potent greenhouse gas. However, methane emission inventories from the Amazon floodplain, the largest natural geographic source of CH 4 in the tropics, consistently underestimate the atmospheric burden of CH 4 determined via remote sensing and inversion modelling, pointing to a major gap in our understanding of the contribution of these ecosystems to CH 4 emissions. Here we report CH 4 fluxes from the stems of 2,357 individual Amazonian floodplain trees from 13 locations across the central Amazon basin. We find that escape of soil gas through wetland trees is the dominant source of regional CH 4 emissions. Methane fluxes from Amazon tree stems were up to 200 times larger than emissions reported for temperate wet forests and tropical peat swamp forests, representing the largest non-ebullitive wetland fluxes observed. Emissions from trees had an average stable carbon isotope value (δ 13 C) of -66.2 ± 6.4 per mil, consistent with a soil biogenic origin. We estimate that floodplain trees emit 15.1 ± 1.8 to 21.2 ± 2.5 teragrams of CH 4 a year, in addition to the 20.5 ± 5.3 teragrams a year emitted regionally from other sources. Furthermore, we provide a 'top-down' regional estimate of CH 4 emissions of 42.7 ± 5.6 teragrams of CH 4 a year for the Amazon basin, based on regular vertical lower-troposphere CH 4 profiles covering the period 2010-2013. We find close agreement between our 'top-down' and combined 'bottom-up' estimates, indicating that large CH 4 emissions from trees adapted to permanent or seasonal inundation can account for the emission source that is required to close the Amazon CH 4 budget. Our findings demonstrate the importance of tree stem surfaces in mediating approximately half of all wetland CH 4 emissions in the Amazon floodplain, a region that represents up to one-third of the global wetland CH 4 source when trees are combined with other emission sources.

A DFT study of Ru, Rh, Pd, Os, Ir, and Pt clusters as catalysts for methane dissociation in a direct methane fuel cell (DMHFC)

Energy Technology Data Exchange (ETDEWEB)

Psofogiannakisa, G. [Ottawa Univ., Ottawa, ON (Canada). Dept. of Chemical Engineering; Ottawa, Univ., Ottawa, ON (Canada). Centre for Catalysis Research and Innovation; St-Amant, A. [Ottawa Univ., Ottawa, ON (Canada). Dept. of Chemistry; Ternan, M. [Ottawa Univ., Ottawa, ON (Canada). Centre for Catalysis Research and Innovation; EnPross Inc., Ottawa, ON (Canada)

2008-07-01

The rate limiting step in a direct methane hydrocarbon fuel cell (DMHFC) is the dissociative chemisorption of methane. Quantum mechanical computations were used to examine the terrace, kink, and step sites on 6 different clusters of group 8 transition metals, notably Ru, Rh, Pd, Os, Ir, and Pt. The computations involved the anodic reaction of a DMHFC with a polymer electrolyte that operates at atmospheric pressure and temperatures higher than 120 degrees C. The interaction between molecular fragments and a surface (Pt) were described and density functional theory (DFT) calculations were performed using Guassian software. The geometries of 5 different platinum clusters were examined along with their electronic energy barriers. The biggest contribution to the stabilization energy came from the overlap between the sigma bond in methane and unoccupied sd hybrid orbitals in the Pt bonding atom. The study showed that when relaxation was allowed, the displacement of the bonding metal atom was 0.36 to 0.52 A. The electronic energy barrier often increased as d-orbital occupancy increased. For the kink surface sites, the energy barriers were considerably smaller for the 5d transition metals than for the 4d transition metals. 5 refs., 1 tab.

Quantifying the Global Marine Biogenic Nitrogen Oxides Emissions

Science.gov (United States)

Su, H.; Wang, S.; Lin, J.; Hao, N.; Poeschl, U.; Cheng, Y.

2017-12-01

Nitrogen oxides (NOx) are among the most important molecules in atmospheric chemistry and nitrogen cycle. The NOx over the ocean areas are traditionally believed to originate from the continental outflows or the inter-continental shipping emissions. By comparing the satellite observations (OMI) and global chemical transport model simulation (GEOS-Chem), we suggest that the underestimated modeled atmospheric NO2 columns over biogenic active ocean areas can be possibly attributed to the biogenic source. Nitrification and denitrification in the ocean water produces nitrites which can be further reduced to NO through microbiological processes. We further report global distributions of marine biogenic NO emissions. The new added emissions improve the agreement between satellite observations and model simulations over large areas. Our model simulations manifest that the marine biogenic NO emissions increase the atmospheric oxidative capacity and aerosol formation rate, providing a closer link between atmospheric chemistry and ocean microbiology.

Production of biogenic amines in "Salamini italiani alla cacciatora PDO".

Science.gov (United States)

Coı X0308 Sson, Jean Daniel; Cerutti, Caterina; Travaglia, Fabiano; Arlorio, Marco

2004-06-01

Various fermented and seasoned foods such as cheese, sauerkraut, wine, beer and meat products may contain biogenic amines. The aim of this paper was to describe the presence of some biogenic amines (histamine, tyramine, tryptamine, 2-phenylethylamine) in "Salamini italiani alla cacciatora PDO", a typical fermented-ripened dry sausage widely consumed in Italy. Total level of biogenic amines in commercial samples ranged from 71 to 586 mg kg(-1). The amine recovered in higher concentrations was tyramine (372 mg kg(-1)) followed by histamine (165 mg kg(-1)). The second aim of this work was the quality control of the production in order to determine the parameters influencing the presence of biogenic amines in ripened salami. Sausages sampled for analysis during production, manipulation and ripening showed the presence of tyramine (64.4 mg kg(-1)) only after 15 days of fermentation. All investigated biogenic amines were detected in "Salamini" after 21 days of fermentation. We suggest the control of biogenic as important tool to establish the better condition of preservation of "Salamini italiani alla cacciatore PDO" during their shelf-life.

Non-Faradaic electrochemical promotion of catalytic methane reforming for methanol production

Science.gov (United States)

Fan, Qinbai

2016-11-22

A method of converting methane to methanol at low temperatures utilizes a reactor including an anode, a cathode, a membrane separator between the anode and cathode, a metal oxide catalyst at the anode and a hydrogen recovery catalyst at the cathode. The method can convert methane to methanol at as rate exceeding the theoretical Faradaic rate due to the contribution of an electrochemical reaction occurring in tandem with a Faradaic reaction.

Facultative methanotrophs are abundant at terrestrial natural gas seeps.

Science.gov (United States)

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

Methane emissions and climate compatibility of fossil fuels

International Nuclear Information System (INIS)

Meier, B.

1992-01-01

Methane contributes directly and indirectly to the additional greenhouse effect caused by human activities. The vast majority of the anthropogenic methane release occurs worldwide in non-fossil sources such as rice cultivation, livestock operations, sanitary landfills and combustion of bio-mass. Methane emissions also occur during production, distribution and utilisation of fossil fuels. Also when considering the methane release and CO 2 -emissions of processes upstream of combustion, the ranking of environmental compatibility of natural gas, fuel oil and cool remains unchanged. Of all fossil fuels, natural gas contributes the least to the greenhouse effect. (orig.) [de

Quantification of Methane and Nitrous Oxide Emissions from Wastewater Collection Systems (Cincinnati, Ohio, USA)

Science.gov (United States)

Fries, A. E.; Townsend-Small, A.; Shuster, W.; Schifman, L. A.

2016-12-01

Greenhouse gas emissions from urban areas is an emerging topic in environmental science, but source apportionment of these emissions, particularly for methane (CH4) and nitrous oxide (N2O), is still underway. Here we present an analysis of CH4 and N2O sources from urban pipelines in Cincinnati, Ohio, USA. Leaks from manholes and sewer grates in Cincinnati are found by using a Bascom Turner Gas Rover to indicate CH4 enhancements, along with spatial data for CH4 enhancements at street level from previously published work. When possible, the atmospheric flux of CH4 and N2O of these leaks are quantified by using a flux chamber method. Source apportionment is determined by using carbon and hydrogen stable isotope ratios (13C and D) and CH4 to N2O ratios. Biogenic CH4 has a δ13C of approximately -55‰ and δD of approximately -270‰, whereas thermogenic CH4 has a δ13C of approximately -45‰ and δD of approximately -150‰. Biogenic CH4 may also co-occur with N2O, whereas thermogenic natural gas does not contain N2O. Contrary to our expectations, we found a portion of CH4 enhancements that are biogenic CH4, presumably from sewer gas, whereas most studies have assumed them to be natural gas leaks. In the future we will be working on determining the exact proportion of biogenic and thermogenic CH4 in street leaks and further quantifying CH4 and N2O emissions throughout Cincinnati. Our work indicates that CH4 leaks in cities may be a mixture of sewer gas and natural gas, especially in cities like Cincinnati where natural gas pipelines have been replaced with less leak-prone pipe materials.

Hydrous pyrolysis/oxidation process for in situ destruction of chlorinated hydrocarbon and fuel hydrocarbon contaminants in water and soil

Science.gov (United States)

Knauss, Kevin G.; Copenhaver, Sally C.; Aines, Roger D.

2000-01-01

In situ hydrous pyrolysis/oxidation process is useful for in situ degradation of hydrocarbon water and soil contaminants. Fuel hydrocarbons, chlorinated hydrocarbons, polycyclic aromatic hydrocarbons, petroleum distillates and other organic contaminants present in the soil and water are degraded by the process involving hydrous pyrolysis/oxidation into non-toxic products of the degradation. The process uses heat which is distributed through soils and water, optionally combined with oxygen and/or hydrocarbon degradation catalysts, and is particularly useful for remediation of solvent, fuel or other industrially contaminated sites.

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

Energy Technology Data Exchange (ETDEWEB)

Fields, Matthew [Montana State Univ., Bozeman, MT (United States)

2018-01-17

Currently, coal bed methane (CBM) wells have a limited lifetime since the rate of methane removal via the installed wells is much faster than the in situ methane production rates. Along with water issues created by large amounts of CBM production water, the short life span of CBM wells is a huge deterrent to the environmental and economic feasibility of CBM production. The process of biogenic methanogenesis can be enhanced via the stimulation of the associated microbial communities that can convert the organic fractions of coal to methane. This process is termed Microbially-Enhanced Coal Bed Methane (MECBM). However, the rates of methane production are still limited and long incubation times are necessary. We hypothesized that the elucidation of chemical and biological parameters that limited MECBM together with thermodynamic considerations would inform strategies to optimize the process under flow conditions. We incorporated microbiological, physicochemical, and engineering processes to develop a more sustainable CBM production scheme with native coal and native microorganisms. The proposed combination of microbial ecology and physiology as well as optimized engineering principles minimized key constraints that impact microbial coal conversion to methane under environmentally relevant conditions. The combined approach for bench-scale tests resulted in more effective and less environmentally burdensome coal-dependent methane production with the potential for H2O and CO2 management.

Physiology and Genetics of Biogenic Methane-Production from Acetate

Energy Technology Data Exchange (ETDEWEB)

Sowers, Kevin R

2013-04-04

Biomass conversion catalyzed by methanogenic consortia is a widely available, renewable resource for both energy production and waste treatment. The efficiency of this process is directly dependent upon the interaction of three metabolically distinct groups of microorganisms; the fermentative and acetogenic Bacteria and the methanogenic Archaea. One of the rate limiting steps in the degradation of soluble organic matter is the dismutation of acetate, a predominant intermediate in the process, which accounts for 70 % or more of the methane produced by the methanogens. Acetate utilization is controlled by regulation of expression of carbon monoxide dehydrogensase (COdh), which catalyzes the dismutation of acetate. However, physiological and molecular factors that control differential substrate utilization have not been identified in these Archaea. Our laboratory has identified sequence elements near the promoter of the gene (cdh) encoding for COdh and we have confirmed that these sequences have a role in the in vivo expression of cdh. The current proposal focuses on identifying the regulatory components that interact with DNA and RNA elements, and identifying the mechanisms used to control cdh expression. We will determine whether expression is controlled at the level of transcription or if it is mediated by coordinate interaction of transcription initiation with other processes such as transcription elongation rate and differential mRNA stability. Utilizing recently sequenced methanosarcinal genomes and a DNA microarray currently under development genes that encode regulatory proteins and transcription factors will be identified and function confirmed by gene disruption and subsequent screening on different substrates. Functional interactions will be determined in vivo by assaying the effects of gene dosage and site-directed mutagenesis of the regulatory gene on the expression of a cdh::lacZ operon fusion. Results of this study will reveal whether this critical

Estimation of biogenic volatile organic compounds emissions in subtropical island--Taiwan.

Science.gov (United States)

Chang, Ken-Hui; Chen, Tu-Fu; Huang, Ho-Chun

2005-06-15

Elevated tropospheric ozone is harmful to human health and plants. It is formed through the photochemical reactions involving volatile organic compounds (VOCs) and nitrogen oxides (NO(x)). The elevated ozone episodes occur mainly in summer months in the United States, while the high-ozone episodes frequently occur during the fall in Taiwan. The unique landscape of Taiwan produces tremendous amounts of biogenic VOCs in the mountain regions that are adjacent to concentrated urban areas. The urban areas, in turn, generate prodigious amounts of anthropogenic emissions. Biogenic VOC emissions have direct influence on tropospheric ozone formation. To explore the air quality problems in Taiwan, this study attempts to develop a biogenic VOC emission model suitable for air quality applications in Taiwan. The emission model is based on the Biogenic Emissions Inventory System Version 2 and coupled with a detailed Taiwan land use database. The 1999 total Taiwan biogenic VOC emissions were estimated at 214,000 metric tons. The emissions of isoprene, monoterpenes, and other VOCs were about 37.2%, 30.4%, and 32.4% of total biogenic VOC emissions, respectively. The annual total biogenic VOC emission per unit area was more than two times the value of that in any European country, implying that detailed emissions estimates in any size of region will benefit the global biogenic emission inventories.

Microbial growth yield estimates from thermodynamics and its importance for degradation of pesticides and formation of biogenic non-extractable residues

DEFF Research Database (Denmark)

Brock, Andreas Libonati; Kästner, M.; Trapp, Stefan

2017-01-01

NER. Formation of microbial mass can be estimated from the microbial growth yield, but experimental data is rare. Instead, we suggest using prediction methods for the theoretical yield based on thermodynamics. Recently, we presented the Microbial Turnover to Biomass (MTB) method that needs a minimum...... and using the released CO2 as a measure for microbial activity, we predicted a range for the formation of biogenic NER. For the majority of the pesticides, a considerable fraction of the NER was estimated to be biogenic. This novel approach provides a theoretical foundation applicable to the evaluation...

Characterization of methane emissions from five cold heavy oil production with sands (CHOPS) facilities.

Science.gov (United States)

Roscioli, Joseph R; Herndon, Scott C; Yacovitch, Tara I; Knighton, W Berk; Zavala-Araiza, Daniel; Johnson, Matthew R; Tyner, David R

2018-03-07

Cold heavy oil production with sands (CHOPS) is a common oil extraction method in the Canadian provinces of Alberta and Saskatchewan that can result in significant methane emissions due to annular venting. Little is known about the magnitude of these emissions, nor their contributions to the regional methane budget. Here the authors present the results of field measurements of methane emissions from CHOPS wells and compare them with self-reported venting rates. The tracer ratio method was used not only to analyze total site emissions but at one site it was also used to locate primary emission sources and quantify their contributions to the facility-wide emission rate, revealing the annular vent to be a dominant source. Emissions measured from five different CHOPS sites in Alberta showed large discrepancies between the measured and reported rates, with emissions being mainly underreported. These methane emission rates are placed in the context of current reporting procedures and the role that gas-oil ratio (GOR) measurements play in vented volume estimates. In addition to methane, emissions of higher hydrocarbons were also measured; a chemical "fingerprint" associated with CHOPS wells in this region reveals very low emission ratios of ethane, propane, and aromatics versus methane. The results of this study may inform future studies of CHOPS sites and aid in developing policy to mitigate regional methane emissions. Methane measurements from cold heavy oil production with sand (CHOPS) sites identify annular venting to be a potentially major source of emissions at these facilities. The measured emission rates are generally larger than reported by operators, with uncertainty in the gas-oil ratio (GOR) possibly playing a large role in this discrepancy. These results have potential policy implications for reducing methane emissions in Alberta in order to achieve the Canadian government's goal of reducing methane emissions by 40-45% below 2012 levels within 8 yr.

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

Science.gov (United States)

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

2010-05-01

Traditional petroleum recovery techniques are unable to extract the majority of oil in most petroliferous deposits. The recovery of even a fraction of residual hydrocarbon in conventional reserves could represent a substantive energy supply. To this end, the microbial conversion of residual oil to methane has gained increasing relevance in recent years [1,2]. Worldwide demand for methane is expected to increase through 2030 [3], as it is a cleaner-burning alternative to traditional fuels [4]. To investigate the microbial physiology of hydrocarbon-decomposition and ultimate methanogenesis, we initiated a two-pronged approach. First, a model alkane-degrading sulfate-reducing bacterium, Desulfoglaeba alkanexedens, was used to interrogate the predominant metabolic pathway(s) differentially expressed during growth on either n-decane or butyrate. A total of 81 proteins were differentially expressed during bacterial growth on butyrate, while 100 proteins were unique to the alkane-grown condition. Proteins related to alkylsuccinate synthase, or the homologous 1-methyl alkylsuccinate synthase, were identified only in the presence of the hydrocarbon. Secondly, we used a newly developed stable isotope probing technique [5] targeted towards proteins to monitor the flux of carbon through a residual oil-degrading bacterial consortium enriched from a gas-condensate contaminated aquifer [1]. Combined carbon and hydrogen stable isotope fractionation identified acetoclastic methanogenesis as the dominant process in this system. Such findings agree with the previous clone library characterization of the consortium. Furthermore, hydrocarbon activation was determined to be the rate-limiting process during the net conversion of residual oil to methane. References 1. Gieg, L.M., K.E. Duncan, and J.M. Suflita, Bioenegy production via microbial conversion of residual oil to natural gas. Appl Environ Micro, 2008. 74(10): p. 3022-3029. 2. Jones, D.M., et al., Crude-oil biodegradation via

Fundamental Flame Velocities of Pure Hydrocarbons I : Alkanes, Alkenes, Alkynes Benzene, and Cyclohexane

Science.gov (United States)

Gerstein, Melvin; Levine, Oscar; Wong, Edgar L

1950-01-01

The flame velocities of 37 pure hydrocarbons including normal and branched alkanes, alkenes, and alkynes; as well as benzene and cyclohexane, together with the experimental technique employed are presented. The normal alkanes have about the same flame velocity from ethane through heptane with methane being about 16 percent lower. Unsaturation increases the flame velocity in the order of alkanes, alkenes, and alkynes. Branching reduces the flame velocity.

Catalytic-Dielectric Barrier Discharge Plasma Reactor For Methane and Carbon Dioxide Conversion

Directory of Open Access Journals (Sweden)

Istadi Istadi

2007-10-01

Full Text Available A catalytic - DBD plasma reactor was designed and developed for co-generation of synthesis gas and C2+ hydrocarbons from methane. A hybrid Artificial Neural Network - Genetic Algorithm (ANN-GA was developed to model, simulate and optimize the reactor. Effects of CH4/CO2 feed ratio, total feed flow rate, discharge voltage and reactor wall temperature on the performance of catalytic DBD plasma reactor was explored. The Pareto optimal solutions and corresponding optimal operating parameters ranges based on multi-objectives can be suggested for catalytic DBD plasma reactor owing to two cases, i.e. simultaneous maximization of CH4 conversion and C2+ selectivity, and H2 selectivity and H2/CO ratio. It can be concluded that the hybrid catalytic DBD plasma reactor is potential for co-generation of synthesis gas and higher hydrocarbons from methane and carbon dioxide and showed better than the conventional fixed bed reactor with respect to CH4 conversion, C2+ yield and H2 selectivity for CO2 OCM process. © 2007 BCREC UNDIP. All rights reserved.[Presented at Symposium and Congress of MKICS 2007, 18-19 April 2007, Semarang, Indonesia][How to Cite: I. Istadi, N.A.S. Amin. (2007. Catalytic-Dielectric Barrier Discharge Plasma Reactor For Methane and Carbon Dioxide Conversion. Bulletin of Chemical Reaction Engineering and Catalysis, 2 (2-3: 37-44.  doi:10.9767/bcrec.2.2-3.8.37-44][How to Link/DOI: http://dx.doi.org/10.9767/bcrec.2.2-3.8.37-44 || or local: http://ejournal.undip.ac.id/index.php/bcrec/article/view/8][Cited by: Scopus 1 |

Molecular and carbon isotopic variability of hydrocarbon gases from mud volcanos in the Gulf of Cadiz, NE Atlantic.

NARCIS (Netherlands)

Stadnitskaia, A.; Ivanov, M.K.; Blinova, V.; Kreulen, R.; van Weering, T.C.E.

2006-01-01

Investigations of molecular and carbon isotopic variability of hydrocarbon gases from methane through butanes (pentanes) have been performed on six mud volcanoes from two fluid venting provinces located in the Gulf of Cadiz, NE Atlantic. The main aims were to define the basic gas types, to describe

Origin and in situ concentrations of hydrocarbons in the Kumano forearc basin from drilling mud gas monitoring during IODP NanTroSEIZE Exp. 319

International Nuclear Information System (INIS)

Wiersberg, Thomas; Schleicher, Anja M.; Horiguchi, Keika; Doan, Mai-Linh; Eguchi, Nobuhisa; Erzinger, Jörg

2015-01-01

Highlights: • Exp. 319 of IODP was the first cruise in the history of scientific ocean drilling with drilling mud gas monitoring. • Hydrocarbons were the only formation-derived gases identified in drilling mud. • Chemical and isotopic compositions of hydrocarbons exhibit a microbial origin. • Absolute CH 4 concentrations in the formation reaching up to 24 L gas /L sediment . - Abstract: NanTroSEIZE Exp. 319 of the Integrated Ocean Drilling Program (IODP) was the first cruise in the history of scientific ocean drilling with drilling mud circulation through a riser. Drilling mud was pumped through the drill string and returned to the drill ship through the riser pipe during drilling of hole C0009A from 703 to 1604 mbsf (meter below sea floor) and hole enlargement from 703 to 1569 mbsf. During riser drilling, gas from returning drilling mud was continuously extracted, sampled and analyzed in real time to reveal information on the gas composition and gas concentrations at depth. Hydrocarbons were the only formation-derived gases identified in drilling mud and reached up to 14 vol.% of methane and 48 ppmv of ethane. The chemical and isotopic compositions of hydrocarbons exhibit a microbial origin. Hydrocarbons released from drilling mud and cuttings correlate with visible allochthonous material (wood, lignite) in drilling cuttings. At greater depth, addition of small but increasing amounts of hydrocarbons probably from low-temperature thermal degradation of organic matter is indicated. The methane content is also tightly correlated with several intervals of low Poisson’s ratio from Vp/Vs observed in sonic velocity logs, suggesting that the gas is situated in the pore space of the rock as free gas. The gas concentrations in the formation, determined from drilling mud gas monitoring, reaching up to 24 L gas /L sediment for methane in hole C0009A, in line with gas concentrations from interpreted downhole sonic logs

Anaerobic Transformation of Chlorinated Aliphatic Hydrocarbons in a Sand Aquifer Based on Spatial Chemical Distributions

Science.gov (United States)

Semprini, Lewis; Kitanidis, Peter K.; Kampbell, Don H.; Wilson, John T.

1995-04-01

We estimated the distribution of chlorinated aliphatic hydrocarbons (CAHs) from groundwater samples collected along three transects in a sand aquifer. Trichloroethylene (TCE) leaked and contaminated the aquifer probably more than a decade before we collected the measurements. The data show significant concentrations of TCE, cis-l,2-dichloroethylene (c-DCE), vinyl chloride (VC), and ethene. We attributed DCE, VC, and ethene to the reductive dehalogenation of TCE. The CAH concentrations varied significantly with depth and correlate with sulfate and methane concentrations. Anoxic aquifer conditions exist with methane present at relatively high concentrations at depth. High concentrations of TCE correspond with the absence of methane or low methane concentrations, whereas products of TCE dehalogenation are associated with higher methane concentrations and low sulfate concentrations. Indications are that the dechlorination of TCE and DCE to VC and ethene is associated with sulfate reduction and active methanogenesis. TCE dechlorination to DCE is likely occurring under the less reducing conditions of sulfate reduction, with further reductions to VC and ethene occurring under methanogenic conditions. We estimated that about 20% of TCE has dechlorinated to ethene. The analysis of the data enhanced our knowledge of natural in situ transformation and transport processes of CAHs.

The potential of methane-oxidizing bacteria for applications in environmental biotechnology

Energy Technology Data Exchange (ETDEWEB)

Wendlandt, Karin-Dagmar; Stottmeister, Ulrich; Jechorek, Mirko [Helmholtz-Center for Environmental Research UFZ, Leipzig (Germany); Helm, Jana [School of Physics and Astronomy, The University of Edinburgh, Edinburgh (United Kingdom); Soltmann, Bettina [Institute for Materials Science, Dresden University of Technology, Dresden (Germany); Beck, Matthias [Oncotec, Pharma Production GmbH, Dessau-Rosslau (Germany)

2010-04-15

Methanotrophic bacteria possess a unique set of enzymes enabling them to oxidize, degrade and transform organic molecules and synthesize new compounds. Therefore, they have great potential in environmental biotechnology. The application of these unique properties was demonstrated in three case studies: (i) Methane escaping from leaky gas pipes may lead to massive mortality of trees in urban areas. Lack of oxygen within the soil surrounding tree roots caused by methanotrophic activity was identified as one of the reasons for this phenomenon. The similarity between metabolic reactions performed by the key enzymes of methanotrophs (methane monooxygenase) and ammonium oxidizers (ammonium monooxygenase) might offer a solution to this problem by applying commercially available nitrification and urease inhibitors. (ii) Methanotrophs are able to co-metabolically degrade contaminants such as low-molecular-weight-chlorinated hydrocarbons in soil and water in the presence of methane. Batch and continuous trichloroethylene degradation experiments in laboratory-scale reactors using Methylocystis sp. GB 14 were performed, partly with cells entrapped in a polymer matrix. (iii) Using a short, two-stage pilot-scale process, the intracellular polymer accumulation of poly-{beta}-hydroxybutyrate (PHB) in methanotrophs reached a maximum of 52%. Interestingly, an ultra-high-molecular-weight PHB of 3.1 MDa was accumulated under potassium deficiency. Under strictly controlled conditions (temperature, pH and methane supply) this process can be nonsterile because of the establishment of a stable microbial community (dominant species Methylocystis sp. GB 25 {>=}86% by biomass). The possibility to substitute methane with biogas from renewable sources facilitates the development of a methane-based PHB production process that yields a high-quality biopolymer at competitive costs. (Abstract Copyright [2010], Wiley Periodicals, Inc.)

Energy efficient selective reforming of hydrocarbons. ERA-NET Bioenergy. Final report

Energy Technology Data Exchange (ETDEWEB)

Rodin, J.

2010-07-15

The research project 'Energy efficient selective reforming of hydrocarbons', funded by the Swedish and Energinet.dk Agency has now reached its end. The report is an overview of the work. Details of the work within the different areas can be found in the reports from each part. In this project, an innovative method for tar removal and reformation of hydrocarbons was investigated: Chemical Looping Reforming (CLR). This gas treatment has the potential to be economically competitive, reliable and environmentally friendly (due to higher energy efficiency, amongst others). The aim of the CLR is to 1) eliminate downstream problems with tar 2) simplify the energy recovery from the hot product gas 3) selectively save lighter hydrocarbons for the production of synthetic natural gas (SNG). A guarantor for the outcome of the project is the engagement of Goeteborg Energi, which has a commitment to build a 20 MW output SNG plant by 2012. DTU (Danish Technical University) is responsible for carrying out the laboratorial part, where different oxygen carriers for the CLR have been considering their capability of selectively reforming hydrocarbons. The conclusion was that, of the four carriers tested, the Mn and Ni40 was the most promising. CUT (Chalmers University of Technology) has installed a 600 W CLR unit connected to a slipstream from the gasifier. During the firing season 2010 the CLR has been tested with raw gas for 36 hours and the results so far show that the equipment works as intended and that it can reduce the amount of tars substantially. GE (Goeteborg Energi AB) together with SEP (Scandinavian Energy Project AB) and CUT have studied the integration of a methane production plant to an existing boiler. The main focus of the study has been the gasifier and the CLR. The integration of a 100 MW methane production plant is estimated to cost 1.3-2.4 billion SEK. The different work packages have altogether shown that a CLR is a possible solution to the tar problem

Shallow Aquifer Methane Gas Source Assessment

Science.gov (United States)

Coffin, R. B.; Murgulet, D.; Rose, P. S.; Hay, R.

2014-12-01

Shale gas can contribute significantly to the world's energy demand. Hydraulic fracturing (fracking) on horizontal drill lines developed over the last 15 years makes formerly inaccessible hydrocarbons economically available. From 2000 to 2035 shale gas is predicted to rise from 1% to 46% of the total natural gas for the US. A vast energy resource is available in the United States. While there is a strong financial advantage to the application of fracking there is emerging concern about environmental impacts to groundwater and air quality from improper shale fracking operations. Elevated methane (CH4) concentrations have been observed in drinking water throughout the United States where there is active horizontal drilling. Horizontal drilling and hydraulic-fracturing can increase CH4 transport to aquifers, soil and the vadose zone. Seepage can also result from casing failure in older wells. However, there is strong evidence that elevated CH4 concentrations can be associated with topographic and hydrogeologic features, rather than shale-gas extraction processes. Carbon isotope geochemistry can be applied to study CH4source(s) in shallow vadose zone and groundwater systems. A preliminary TAMU-CC isotope data set from samples taken at different locations in southern Texas shows a wide range of CH4 signatures suggesting multiple sources of methane and carbon dioxide. These data are interpreted to distinguish regions with methane contributions from deep-sourced horizontal drilling versus shallow system microbial production. Development of a thorough environmental assessment using light isotope analysis can provide understanding of shallow anthropogenic versus natural CH4sources and assist in identifying regions that require remedial actions.

Biogenic emissions of isoprenoids and NO in China and comparison to anthropogenic emissions

International Nuclear Information System (INIS)

Tie Xuexi; Li Guohui; Ying, Zhuming; Guenther, Alex; Madronich, Sasha

2006-01-01

In this study, a regional dynamical model (WRF) is used to drive biogenic emission models to calculate high resolution (10 x 10 km) biogenic emissions of isoprene (C 5 H 8 ), monoterpenes (C 1 H 16 ), and nitric oxide (NO) in China. This high resolution biogenic inventory will be available for the community to study the effect of biogenic emissions on photochemical oxidants in China. The biogenic emissions are compared to anthropogenic emissions to gain insight on the potential impact of the biogenic emissions on tropospheric chemistry, especially ozone production in this region. The results show that the biogenic emissions in China exhibit strongly diurnal, seasonal, and spatial variations. The isoprenoid (including both isoprene and monoterpenes) emissions are closely correlated to tree density and strongly vary with season and local time. During winter (January), the biogenic isoprenoid emissions are the lowest, resulting from lower temperature and solar radiation, and highest in summer (July) due to higher temperature and solar radiation. The biogenic NO emissions are also higher during summer and lower during winter, but the magnitude of the seasonal variation is smaller than the emissions of isoprene and monoterpenes. The biogenic emissions of NO are widely spread out in the northern, eastern, and southern China regions, where high-density agricultural soil lands are located. Both biogenic NO and isoprenoid emissions are very small in western China. The calculated total biogenic emission budget is smaller than the total anthropogenic VOC emission budget in China. The biogenic isoprenoid and anthropogenic VOC emissions are 10.9 and 15.1 Tg year -1 , respectively. The total biogenic and anthropogenic emissions of NO are 5.9 and 11.5 Tg(NO) year -1 , respectively. The study shows that in central eastern China, the estimated biogenic emissions of isoprenoids are very small, and the anthropogenic emissions of VOCs are dominant in this region. However, in

Biogenic emissions of isoprenoids and NO in China and comparison to anthropogenic emissions.

Science.gov (United States)

Tie, Xuexi; Li, Guohui; Ying, Zhuming; Guenther, Alex; Madronich, Sasha

2006-12-01

In this study, a regional dynamical model (WRF) is used to drive biogenic emission models to calculate high resolution (10x10 km) biogenic emissions of isoprene (C(5)H(8)), monoterpenes (C(10)H(16)), and nitric oxide (NO) in China. This high resolution biogenic inventory will be available for the community to study the effect of biogenic emissions on photochemical oxidants in China. The biogenic emissions are compared to anthropogenic emissions to gain insight on the potential impact of the biogenic emissions on tropospheric chemistry, especially ozone production in this region. The results show that the biogenic emissions in China exhibit strongly diurnal, seasonal, and spatial variations. The isoprenoid (including both isoprene and monoterpenes) emissions are closely correlated to tree density and strongly vary with season and local time. During winter (January), the biogenic isoprenoid emissions are the lowest, resulting from lower temperature and solar radiation, and highest in summer (July) due to higher temperature and solar radiation. The biogenic NO emissions are also higher during summer and lower during winter, but the magnitude of the seasonal variation is smaller than the emissions of isoprene and monoterpenes. The biogenic emissions of NO are widely spread out in the northern, eastern, and southern China regions, where high-density agricultural soil lands are located. Both biogenic NO and isoprenoid emissions are very small in western China. The calculated total biogenic emission budget is smaller than the total anthropogenic VOC emission budget in China. The biogenic isoprenoid and anthropogenic VOC emissions are 10.9 and 15.1 Tg year(-1), respectively. The total biogenic and anthropogenic emissions of NO are 5.9 and 11.5 Tg(NO) year(-1), respectively. The study shows that in central eastern China, the estimated biogenic emissions of isoprenoids are very small, and the anthropogenic emissions of VOCs are dominant in this region. However, in

Optimized CO{sub 2} miscible hydrocarbon fracturing fluids

Energy Technology Data Exchange (ETDEWEB)

Taylor, R.S.; Funkhouser, G.P.; Fyten, G.; Attaway, D.; Watkins, H. [Halliburton Energy Services, Calgary, AB (Canada); Lestz, R.S. [Chevron Canada Resources, Calgary, AB (Canada); Loree, D. [FracEx Inc. (Canada)

2006-07-01

Carbon dioxide (CO{sub 2}) miscible hydrocarbon fracturing fluids address issues of fluid retention in low-permeability gas reservoirs, including undersaturated and underpressured reservoirs. An optimized surfactant gel technology using carbon dioxide (CO{sub 2}) hydrocarbon fracturing fluids applicable to all gas-well stimulation applications was discussed in this paper. The crosslinked surfactant gel technology improved proppant transport, leakoff control, and generation of effective fracture half-length. Tests indicated that application of the surfactant cooled the fracture face, which had the effect of extending break times and increasing viscosity during pumping periods. Rapid recovery of the fracturing fluid eliminated the need for swabbing in some cases, and the fluid system was not adversely affected by shear. However, rheological test equipment capable of mixing liquid CO{sub 2} and viscosified hydrocarbons at downhole temperatures is required to determine rheology and required chemical concentrations. It was recommended that to achieve an effective methane-drive cleanup mechanism, treatments should be designed so that the gellant system can be effective with up to 50 per cent CO{sub 2} dissolved in oil. It was concluded that it should be possible to apply the technology to low permeability gas reservoirs. Viscosity curves and friction data were presented. Issues concerning the selection of tubulars and flowback procedures were also discussed. It was suggested that the cost of the hydrocarbon fracturing fluid can be recovered by the sale of recovered load fluid. 6 refs., 4 figs.

Development of a Raman spectroscopy technique to detect alternate transportation fuel hydrocarbon intermediates in complex combustion environments.

Energy Technology Data Exchange (ETDEWEB)

Ekoto, Isaac W.; Barlow, Robert S.

2012-12-01

Spontaneous Raman spectra for important hydrocarbon fuels and combustion intermediates were recorded over a range of low-to-moderate flame temperatures using the multiscalar measurement facility located at Sandia/CA. Recorded spectra were extrapolated to higher flame temperatures and then converted into empirical spectral libraries that can readily be incorporated into existing post-processing analysis models that account for crosstalk from overlapping hydrocarbon channel signal. Performance testing of the developed libraries and reduction methods was conducted through an examination of results from well-characterized laminar reference flames, and was found to provide good agreement. The diagnostic development allows for temporally and spatially resolved flame measurements of speciated hydrocarbon concentrations whose parent is more chemically complex than methane. Such data are needed to validate increasingly complex flame simulations.

Reconnaissance survey for lightweight and carbon tetrachloride extractable hydrocarbons in the central and eastern basins of Lake Erie: September 1978

Energy Technology Data Exchange (ETDEWEB)

Zapotosky, J.E.; White, W.S.

1980-10-01

A reconnaissance survey of the central and eastern basins of Lake Erie (22,240 km/sup 2/) was conducted from September 17 to 27, 1978. The survey provided baseline information on natural gas and oil losses from geologic formations, prior to any potential development of natural gas resources beneath the United States portion of the Lake. Lightweight hydrocarbons indicative of natural gas (methane, ethane, propane, isobutane, and n-butane) are introduced into the waters of Lake Erie by escape from geologic formations and by biological/photochemical processes. The geochemical exploration technique of hydrocarbon sniffing provided enough data to reveal significant distribution patterns, approximate concentrations, and potential sources. Twelve sites with elevated lightweight hydrocarbon concentrations had a composition similar to natural gas. In one area of natural gas input, data analysis suggested a potential negative effect of natural gas on phytoplanktonic metabolism (i.e., ethylene concentration). Samples taken for liquid hydrocarbon analysis (carbon tetrachloride extractable hydrocarbons) correlated best with biologically derived lightweight hydrocarbons.

Water Management Strategies for Improved Coalbed Methane Production in the Black Warrior Basin

Energy Technology Data Exchange (ETDEWEB)

Pashin, Jack [Geological Survey Of Alabama, Tuscaloosa, AL (United States); McIntyre-Redden, Marcella [Geological Survey Of Alabama, Tuscaloosa, AL (United States); Mann, Steven [Geological Survey Of Alabama, Tuscaloosa, AL (United States); Merkel, David [Geological Survey Of Alabama, Tuscaloosa, AL (United States)

2013-10-31

The modern coalbed methane industry was born in the Black Warrior Basin of Alabama and has to date produced more than 2.6 trillion cubic feet of gas and 1.6 billion barrels of water. The coalbed gas industry in this area is dependent on instream disposal of co-produced water, which ranges from nearly potable sodium-bicarbonate water to hypersaline sodium-chloride water. This study employed diverse analytical methods to characterize water chemistry in light of the regional geologic framework and to evaluate the full range of water management options for the Black Warrior coalbed methane industry. Results reveal strong interrelationships among regional geology, water chemistry, and gas chemistry. Coalbed methane is produced from multiple coal seams in Pennsylvanian-age strata of the Pottsville Coal Interval, in which water chemistry is influenced by a structurally controlled meteoric recharge area along the southeastern margin of the basin. The most important constituents of concern in the produced water include chlorides, ammonia compounds, and organic substances. Regional mapping and statistical analysis indicate that the concentrations of most ionic compounds, metallic substances, and nonmetallic substances correlate with total dissolved solids and chlorides. Gas is effectively produced at pipeline quality, and the only significant impurity is N{sub 2}. Geochemical analysis indicates that the gas is of mixed thermogenic-biogenic origin. Stable isotopic analysis of produced gas and calcite vein fills indicates that widespread late-stage microbial methanogenesis occurred primarily along a CO{sub 2} reduction metabolic pathway. Organic compounds in the produced water appear to have helped sustain microbial communities. Ammonia and ammonium levels increase with total dissolved solids content and appear to have played a role in late-stage microbial methanogenesis and the generation of N{sub 2}. Gas production tends to decline exponentially, whereas water production

Insights into hydrocarbon formation by nitrogenase cofactor homologs.

Science.gov (United States)

Lee, Chi Chung; Hu, Yilin; Ribbe, Markus W

2015-04-14

The L-cluster is an all-iron homolog of nitrogenase cofactors. Driven by europium(II) diethylenetriaminepentaacetate [Eu(II)-DTPA], the isolated L-cluster is capable of ATP-independent reduction of CO and CN(-) to C1 to C4 and C1 to C6 hydrocarbons, respectively. Compared to its cofactor homologs, the L-cluster generates considerably more CH4 from the reduction of CO and CN(-), which could be explained by the presence of a "free" Fe atom that is "unmasked" by homocitrate as an additional site for methanation. Moreover, the elevated CH4 formation is accompanied by a decrease in the amount of longer hydrocarbons and/or the lengths of the hydrocarbon products, illustrating a competition between CH4 formation/release and C-C coupling/chain extension. These observations suggest the possibility of designing simpler synthetic clusters for hydrocarbon formation while establishing the L-cluster as a platform for mechanistic investigations of CO and CN(-) reduction without complications originating from the heterometal and homocitrate components. Nitrogenase is a metalloenzyme that is highly complex in structure and uniquely versatile in function. It catalyzes two reactions that parallel two important industrial processes: the reduction of nitrogen to ammonia, which parallels the Haber-Bosch process in ammonia production, and the reduction of carbon monoxide to hydrocarbons, which parallels the Fischer-Tropsch process in fuel production. Thus, the significance of nitrogenase can be appreciated from the perspective of the useful products it generates: (i) ammonia, the "fixed" nitrogen that is essential for the existence of the entire human population; and (ii) hydrocarbons, the "recycled" carbon fuel that could be used to directly address the worldwide energy shortage. This article provides initial insights into the catalytic characteristics of various nitrogenase cofactors in hydrocarbon formation. The reported assay system provides a useful tool for mechanistic

Selection of nutrient used in biogenic healing agent for cementitious materials

Science.gov (United States)

Tziviloglou, Eirini; Wiktor, Virginie; Jonkers, Henk M.; Schlangen, Erik

2017-06-01

Biogenic self-healing cementitious materials target on the closure of micro-cracks with precipitated inorganic minerals originating from bacterial metabolic activity. Dormant bacterial spores and organic mineral compounds often constitute a biogenic healing agent. The current paper focuses on the investigation of the most appropriate organic carbon source to be used as component of a biogenic healing agent. It is of great importance to use an appropriate organic source, since it will firstly ensure an optimal bacterial performance in terms of metabolic activity, while it should secondly affect the least the properties of the cementitious matrix. The selection is made among three different organic compounds, namely calcium lactate, calcium acetate and sodium gluconate. The methodology that was used for the research was based on continuous and non-continuous oxygen consumption measurements of washed bacterial cultures and on compressive strength tests on mortar cubes. The oxygen consumption investigation revealed a preference for calcium lactate and acetate, but an indifferent behaviour for sodium gluconate. The compressive strength on mortar cubes with different amounts of either calcium lactate or acetate (up to 2.24% per cement weight) was not or it was positively affected when the compounds were dissolved in the mixing water. In fact, for calcium lactate the increase in compressive strength reached 8%, while for calcium acetate the maximum strength increase was 13.4%.

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

Science.gov (United States)

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.

Green chemistry perspectives of methane conversion via oxidative methylation of aromatics over zeolite catalysts

Energy Technology Data Exchange (ETDEWEB)

Adebajo, M.O. [University of Queensland, St Lucia, Qld. (Australia)

2007-06-15

This paper provides a general overview of the recent work that we and other researchers have done on the utilisation of methane for catalytic methylation of aromatic compounds and for direct coal liquefaction for the production of liquid hydrocarbons. In particular, the paper presents a detailed description of more recent substantial experimental evidence that we have provided for the requirement of oxygen as a stoichiometry reactant for benzene methylation with methane over moderately acidic zeolite catalysts. The reaction, which has been termed 'oxidative methylation', was thus postulated to involve a two-step mechanism involving intermediate methanol formation by methane partial oxidation, followed by benzene methylation with methanol in the second step. However, strongly acidic zeolites can cause cracking of benzene to yield methylated products in the absence of oxygen. The participation of methane and oxygen, and the effective use of zeolite catalysts in this methylation reaction definitely have some positive green chemistry implications. Thus, the results of these previous studies are also discussed in this review in light of the principles and tools of green chemistry. Various metrics were used to evaluate the greenness, cost-effectiveness, and material and energy efficiency of the oxidative methylation reaction.

Microplasma reforming of hydrocarbons for fuel cell power

Science.gov (United States)

Besser, R. S.; Lindner, P. J.

The implementation of a microplasma approach for small scale reforming processes is explored as an alternative to more standard catalyst-based processes. Plasmas are a known approach to activating a chemical reaction in place of catalysts, and microplasmas are particularly attractive owing to their extremely high electron and power densities. Their inherent compactness gives them appeal for portable applications, but their modularity leads to scalability for higher capacity. We describe the realization of experimental microplasma reactors based on the microhollow cathode discharge (MHCD) structure by silicon micromachining for device fabrication. Experiments were carried out with model hydrocarbons methane and butane in the reactors within a microfluidic flow and analytical setup. We observe several key phenomena, including the ability to liberate hydrogen from the hydrocarbons at temperatures near ambient and sub-Watt input power levels, the tendency toward hydrocarbon decomposition rather than oxidation even in the presence of oxygen, and the need for a neutral carrier to obtain conversion. Mass and energy balances on these experiments revealed conversions up to nearly 50%, but the conversion of electrical power input to chemical reaction enthalpy was only on the order of 1%. These initial, exploratory results were recorded with devices and at process settings without optimization, and are hence promising for an emerging, catalyst-free reforming approach.

Measurements of Carbon Dioxide, Methane, and Other Related Tracers at High Spatial and Temporal Resolution in an Urban Environment

Science.gov (United States)

Yasuhara, Scott; Forgeron, Jeff; Rella, Chris; Franz, Patrick; Jacobson, Gloria; Chiao, Sen; Saad, Nabil

2013-04-01

The ability to quantify sources and sinks of carbon dioxide and methane on the urban scale is essential for understanding the atmospheric drivers to global climate change. In the 'top-down' approach, overall carbon fluxes are determined by combining remote measurements of carbon dioxide concentrations with complex atmospheric transport models, and these emissions measurements are compared to 'bottom-up' predictions based on detailed inventories of the sources and sinks of carbon, both anthropogenic and biogenic in nature. This approach, which has proven to be effective at continental scales, becomes challenging to implement at urban scales, due to poorly understood atmospheric transport models and high variability of the emissions sources in space (e.g., factories, highways, green spaces) and time (rush hours, factory shifts and shutdowns, and diurnal and seasonal variation in residential energy use). New measurement and analysis techniques are required to make sense of the carbon dioxide signal in cities. Here we present detailed, high spatial- and temporal- resolution greenhouse gas measurements made by multiple Picarro-CRDS analyzers in Silicon Valley in California. Real-time carbon dioxide data from a 20-month period are combined with real-time carbon monoxide, methane, and acetylene to partition the observed carbon dioxide concentrations between different anthropogenic sectors (e.g., transport, residential) and biogenic sources. Real-time wind rose data are also combined with real-time methane data to help identify the direction of local emissions of methane. High resolution WRF models are also included to better understand the dynamics of the boundary layer. The ratio between carbon dioxide and carbon monoxide is shown to vary over more than a factor of two from season to season or even from day to night, indicating rapid but frequent shifts in the balance between different carbon dioxide sources. Additional information is given by acetylene, a fossil fuel

Study of non-catalytic thermal decomposition of triglyceride at hydroprocessing condition

International Nuclear Information System (INIS)

Palanisamy, Shanmugam; Gevert, Borje S.

2016-01-01

Highlights: • Thermolysis of triglycerides occurs above 300 °C and cracking intensify above 350 °C. • Decomposition of carboxylic group observed, and β-H abstraction gives radical. • Product contains aldehyde, ketonic, saturated/unsaturated, cyclic, glycerol group. • Gasoline fraction contains lighter, cyclic and unsaturated hydrocarbons. • Residues contain ester, dimer and carboxylic groups. - Abstract: Non-catalytic thermal decomposition of triglyceride is studied between 300 and 410 °C at 0.1 and 5 MPa in the presence of H 2 or inert gas. This test is carried in tubular reactor filled with inert material (borosilicate glass pellet). The qualitative and analytical results showed that n-alkanes and alkenes with oxygenated olefins were primary products, consistent with thermal cracking to lighter hydrocarbons. The resulting outlet fuel gas obtained mainly from the radical reaction and had high concentration of CO, ethylene and methane. The decomposition forms a large number of radical compounds containing acids, aldehydes, ketones, aliphatic and aromatic hydrocarbon groups. Lighter fraction contains mostly naphthenic group, and heavy fraction contains straight chain paraffinic hydrocarbons. When H 2 partial pressure raised, the cracking of heavy fractions is low, and products contain low concentration of the lighter and gasoline fractions. Here, the thermal decomposition of triglyceride yields lighter fractions due to cracking, decarboxylation and decarbonylation.

High-temperature measurements of methane and acetylene using quantum cascade laser absorption near 8μm

KAUST Repository

Sajid, M.B.

2015-04-01

The mid-infrared wavelength region near 8 mu m contains absorption bands of several molecules such as water vapor, hydrogen peroxide, nitrous oxide, methane and acetylene. A new laser absorption sensor based on the v(4) band of methane and the v(4)+v(5) band of acetylene is reported for interference-free, time-resolved measurements under combustion-relevant conditions. A detailed line-selection procedure was used to identify optimum transitions. Methane and acetylene were measured at the line centers of Q12 (1303.5 cm(-1)) and P23 (1275.5 cm(-1)) transitions, respectively. High-temperature absorption cross sections of methane and acetylene were measured at peaks (on-line) and valleys (off-line) of the selected absorption transitions. The differential absorption strategy was employed to eliminate interference absorption from large hydrocarbons. Experiments were performed behind reflected shock waves over a temperature range of 1200-2200 K, between pressures of 1-4 atm. The diagnostics were then applied to measure the respective species time-history profiles during the shock-heated pyrolysis of n-pentane. (C) 2015 Elsevier Ltd. All rights reserved.

Global Inverse Modeling of CH4 and δ13C-CH4 Measurements to Understand Recent Trends in Methane Emissions

Science.gov (United States)

Karmakar, S.; Butenhoff, C. L.; Rice, A. L.; Khalil, A. K.

2017-12-01

Methane (CH4) is the second most important greenhouse gas with a radiative forcing of 0.97 W/m2 including both direct and indirect effects and a global warming potential of 28 over a 100-year time horizon. After a decades-long period of decline beginning in the 1980s, the methane growth rate rebounded in 2007 for reasons that are of current debate. During this same growth period atmospheric methane became less enriched in the 13CH4 isotope suggesting the recent CH4 growth was caused by an increase in 13CH4-depleted biogenic emissions. Recent papers have attributed this growth to increasing emissions from wetlands, rice agriculture, and ruminants. In this work we provide additional insight into the recent behavior of atmospheric methane and global wetland emissions by performing a three-dimensional Bayesian inversion of surface CH4 and 13CH4/12CH4 ratios using NOAA Global Monitoring Division (GMD) "event-level" CH4 measurements and the GEOS-Chem chemical-transport model (CTM) at a horizontal grid resolution of 2ox2.5o. The spatial pattern of wetland emissions was prescribed using soil moisture and temperature from GEOS-5 meteorology fields and soil carbon pools from the Lund-Potsdam-Jena global vegetation model. In order to reduce the aggregation error caused by a potentially flawed distribution and to account for isotopic measurements that indicate northern high latitude wetlands are isotopically depleted in 13CH4 relative to tropical wetlands we separated our pattern into three latitudinal bands (90-30°N, 30°N-0, 0-90°S). Our preliminary results support previous claims that the recent increase in atmospheric methane is driven by increases in biogenic CH4 emissions. We find that while wetland emissions from northern high latitudes (90-30°N) remained relatively constant during this time, southern hemisphere wetland emissions rebounded from a decade-long decline and began to rise again in 2007 and have remained elevated to the present. Emissions from rice

Performance evaluation and comparison of fuel processors integrated with PEM fuel cell based on steam or autothermal reforming and on CO preferential oxidation or selective methanation

International Nuclear Information System (INIS)

Ercolino, Giuliana; Ashraf, Muhammad A.; Specchia, Vito; Specchia, Stefania

2015-01-01

Highlights: • Modeling of different fuel processors integrated with PEM fuel cell stack. • Steam or autothermal reforming + CO selective methanation or preferential oxidation. • Reforming of different hydrocarbons: gasoline, light diesel oil, natural gas. • 5 kW e net systems comparison via energy efficiency and primary fuel rate consumed. • Highest net efficiency: steam reformer + CO selective methanation based system. - Abstract: The performances of four different auxiliary power unit (APU) schemes, based on a 5 kW e net proton exchange membrane fuel cell (PEM-FC) stack, are evaluated and compared. The fuel processor section of each APU is characterized by a reformer (autothermal ATR or steam SR), a non-isothermal water gas shift (NI-WGS) reactor and a final syngas catalytic clean-up step: the CO preferential oxidation (PROX) reactor or the CO selective methanation (SMET) one. Furthermore, three hydrocarbon fuels, the most commonly found in service stations (gasoline, light diesel oil and natural gas) are considered as primary fuels. The comparison is carried out examining the results obtained by a series of steady-state system simulations in Aspen Plus® of the four different APU schemes by varying the fed fuel. From the calculated data, the performance of CO-PROX is not very different compared to that of the CO-SMET, but the performance of the SR based APUs is higher than the scheme of the ATR based APUs. The most promising APU scheme with respect to an overall performance target is the scheme fed with natural gas and characterized by a fuel processor chain consisting of SR, NI-WGS and CO-SMET reactors. This processing reactors scheme together with the fuel cell section, notwithstanding having practically the same energy efficiency of the scheme with SR, NI-WGS and CO-PROX reactors, ensures a less complex scheme, higher hydrogen concentration in the syngas, lower air mass rate consumption, the absence of nitrogen in the syngas and higher potential

Production of hydrogen via conversion of hydrocarbons using a microwave plasma

Energy Technology Data Exchange (ETDEWEB)

Jasinski, Mariusz; Dors, Miroslaw; Nowakowska, Helena; Mizeraczyk, Jerzy [Centre for Plasma and Laser Engineering, The Szewalski Institute of Fluid-Flow Machinery, Polish Academy of Sciences, Fiszera 14, 80-952 Gdansk (Poland); Nichipor, Gerietta V, E-mail: mj@imp.gda.pl [Joint Institute of Power and Nuclear Research, Academy of Sciences of Belarus, Minsk, Sosny 220109 (Belarus)

2011-05-18

In this paper, results of hydrogen production from hydrocarbons in an atmospheric pressure microwave plasma are presented. As sources of hydrogen, both methane CH{sub 4} and tetrafluoroethane C{sub 2}H{sub 2}F{sub 4} were tested. A new waveguide-based nozzleless cylinder-type microwave plasma source was used to convert hydrocarbons into hydrogen. The processed gaseous hydrocarbons were introduced into the plasma by four gas ducts which formed a swirl flow in the plasma reactor. The absorbed microwave power was up to 5 kW. The gas flow rate was up to 212 L min{sup -1}. The hydrogen mass yield rate and the corresponding energetic hydrogen mass yield were up to 866 g[H{sub 2}] h{sup -1} and 577 g [H{sub 2}] kWh{sup -1} of microwave energy absorbed by the plasma, respectively. These parameters are better than our previous results when nitrogen was used as a swirl gas and much better than those typical for other plasma methods of hydrogen production (electron beam, gliding arc, plasmatron).

High performance direct absorption spectroscopy of pure and binary mixture hydrocarbon gases in the 6-11 μm range

Science.gov (United States)

Heinrich, Robert; Popescu, Alexandru; Hangauer, Andreas; Strzoda, Rainer; Höfling, Sven

2017-08-01

The availability of accurate and fast hydrocarbon analyzers, capable of real-time operation while enabling feedback-loops, would lead to a paradigm change in the petro-chemical industry. Primarily gas chromatographs measure the composition of hydrocarbon process streams. Due to sophisticated gas sampling, these analyzers are limited in response time. As hydrocarbons absorb in the mid-infrared spectral range, the employment of fast spectroscopic systems is highly attractive due to significantly reduced maintenance costs and the capability to setup real-time process control. New developments in mid-infrared laser systems pave the way for the development of high-performance analyzers provided that accurate spectral models are available for multi-species detection. In order to overcome current deficiencies in the availability of spectroscopic data, we developed a laser-based setup covering the 6-11 μm wavelength range. The presented system is designated as laboratory reference system. Its spectral accuracy is at least 6.6× 10^{-3} cm^{-1} with a precision of 3× 10^{-3} cm^{-1}. With a "per point" minimum detectable absorption of 1.3× 10^{-3} cm^{-1} Hz^{{-}{1/2}} it allows us to perform systematic measurements of hydrocarbon spectra of the first 7 alkanes under conditions which are not tabulated in spectroscopic database. We exemplify the system performance with measured direct absorption spectra of methane, propane, iso-butane, and a mixture of methane and propane.

Studies on the pore water sulfate, chloride and sedimentary methane to understand the sulfate reduction process in the eastern Arabian Sea

Digital Repository Service at National Institute of Oceanography (India)

Karisiddaiah, S.M.; Borole, D.V.; Rao, B.R.; Paropkari, A.L.; Joao, H; Kocherla, M.; Sarkar, G.P.; Biswas, G.; Kumar, N.

Sediment cores (~5 m length) from ten stations collected in the water depths of 2665-3210 m in the eastern Arabian Sea were studied for pore water sulfate (SO42-), chloride (Cl-) and lighter-hydrocarbons (methane: C1, ethane:C2 and propane: C3...

Net Ecosystem Fluxes of Hydrocarbons from a Ponderosa Pine Forest in Colorado

Science.gov (United States)

Rhew, R. C.; Turnipseed, A. A.; Ortega, J. V.; Smith, J. N.; Guenther, A. B.; Shen, S.; Martinez, L.; Koss, A.; Warneke, C.; De Gouw, J. A.; Deventer, M. J.

2015-12-01

Light (C2-C4) alkenes, light alkanes and isoprene (C5H8) are non-methane hydrocarbons that play important roles in the photochemical production of tropospheric ozone and in the formation of secondary organic aerosols. Natural terrestrial fluxes of the light hydrocarbons are poorly characterized, with global emission estimates based on limited field measurements. In 2014, net fluxes of these compounds were measured at the Manitou Experimental Forest Observatory, a semi-arid ponderosa pine forest in the Colorado Rocky Mountains and site of the prior BEACHON campaigns. Three field intensives were conducted between June 17 and August 10, 2014. Net ecosystem flux measurements utilized a relaxed eddy accumulation system coupled to an automated gas chromatograph. Summertime average emissions of ethene and propene were up to 90% larger than those observed from a temperate deciduous forest. Ethene and propene fluxes were also correlated to each other, similar to the deciduous forest study. Emissions of isoprene were small, as expected for a coniferous forest, and these fluxes were not correlated with either ethene or propene. Unexpected emissions of light alkanes were also observed, and these showed a distinct diurnal cycle. Understory flux measurements allowed for the partitioning of fluxes between the surface and the canopy. Full results from the three field intensives will be compared with environmental variables in order to parameterize the fluxes for use in modeling emissions.

Non-controlled biogenic emissions to the atmosphere from Lazareto landfill, Tenerife, Canary Islands.

Science.gov (United States)

Nolasco, Dácil; Lima, R Noemí; Hernández, Pedro A; Pérez, Nemesio M

2008-01-01

[corrected] Historically, landfills have been the simplest form of eliminating urban solid waste with the minimum cost. They have been the most usual method for discarding solid waste. However, landfills are considered authentic biochemical reactors that introduce large amounts of contaminants into the environment in the form of gas and leachates. The dynamics of generation and the movement of gas in landfills depend on the input and output parameters, as well as on the structure of the landfill and the kind of waste. The input parameters include water introduced through natural or artificial processes, the characteristics of the urban solid waste, and the input of atmospheric air. The main output parameters for these biochemical reactors include the gases and the leachates that are potentially pollutants for the environment. Control systems are designed and installed to minimize the impact on the environment. However, these systems are not perfect and a significant amount of landfill gas could be released to the atmosphere through the surface in a diffuse form, also known as Non-controlled emission. In this paper, the results of the Non-controlled biogenic gas emissions from the Lazareto landfill in Tenerife, Canary Islands, are presented. The purpose of this study was to evaluate the concentration of CH4 and CO2 in the soil gas of the landfill cover, the CH4 and CO2 efflux from the surface of the landfill and, finally, to compare these parameters with other similar landfills. In this way, a better understanding of the process that controls biogenic gas emissions in landfills is expected. A Non-controlled biogenic gas emission survey of 281 sampling sites was carried out during February and March, 2002. The sampling sites were selected in order to obtain a well-distributed sampling grid. Surface landfill CO2 efflux measurements were carried out at each sampling site on the surface landfill together with soil gas collection and ground temperatures at a depth of 30

Catalytic and Noncatalytic Conversion of Methane to Olefins and Synthesis Gas in an AC Parallel Plate Discharge Reactor

Directory of Open Access Journals (Sweden)

Mohammad Ali Khodagholi

2013-01-01

Full Text Available Direct conversion of methane to ethylene, acetylene, and synthesis gas at ambient pressure and temperature in a parallel plate discharge reactor was investigated. The experiments were carried out using a quartz reactor of outer diameter of 9 millimeter and a driving force of ac current of 50 Hz. The input power to the reactor to establish a stable gas discharge varied from 9.6 to maximum 15.3 watts (w. The effects of ZSM5, Fe–ZSM5, and Ni–ZSM5 catalysts combined with corona discharge for conversion of methane to more valued products have been addressed. It was found that in presence or absence of a catalyst in gas discharge reactor, the rate of methane and oxygen conversion increased upon higher input power supplied to the reactor. The effect of Fe–ZSM5 catalyst combined with gas discharge plasma yields C2 hydrocarbons up to 21.9%, which is the highest productions of C2 hydrocarbons in this work. The effect of combined Ni–ZSM5 and gas discharge plasma was mainly production of synthesis gas. The advantage of introducing ZSM5 to the plasma zone was increase in synthesis gas and acetylene production. The highest energy efficiency was 0.22 mmol/kJ, which belongs to lower rate of energy injection to the reactor.

Process for separating nitrogen from methane using microchannel process technology

Science.gov (United States)

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

2007-07-31

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