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.

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

A five year record of high-frequency in situ measurements of non-methane hydrocarbons at Mace Head, Ireland

Directory of Open Access Journals (Sweden)

A. Grant

2011-05-01

Full Text Available Continuous high-frequency in situ measurements of a range of non-methane hydrocarbons have been made at Mace Head since January 2005. Mace Head is a background Northern Hemispheric site situated on the eastern edge of the Atlantic. Five year measurements (2005–2009 of six C₂–C₅ non-methane hydrocarbons have been separated into baseline Northern Hemispheric and European polluted air masses, among other sectors. Seasonal cycles in baseline Northern Hemispheric air masses and European polluted air masses arriving at Mace Head have been studied. Baseline air masses show a broad summer minima between June and September for shorter lived species, longer lived species show summer minima in July/August. All species displayed a winter maxima in February. European air masses showed baseline elevated mole fractions for all non-methane hydrocarbons. Largest elevations (of up to 360 ppt for ethane maxima from baseline data were observed in winter maxima, with smaller elevations observed during the summer. Analysis of temporal trends using the Mann-Kendall test showed small (<6 % yr⁻¹ but statistically significant decreases in the butanes and i-pentane between 2005 and 2009 in European air. No significant trends were found for any species in baseline air.

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

Continuous flow IRMS application to CH4, MNHCS, and N2O in the atmosphere and the oceans

International Nuclear Information System (INIS)

Yoshida, N.; Tsunogai, U.; Toyoda, S.

2001-01-01

The application of CF-IRMS to measurement of methane (CH4), non-methane hydrocarbons (NMHCS), and nitrous oxide (N 2 O) is outlined and preliminary information on isotopic variations in the atmosphere and oceans is presented. Labelling of these compounds is expected to provide a robust method for tracing sources, sinks and controlling processes in the environment. (author)

Photochemically consumed hydrocarbons and their relationship with ozone formation in two megacities of China

Science.gov (United States)

Chang, C.; Wang, J.; Liu, S.; Shao, M.; Zhang, Y.; Zhu, T.; Shiu, C.; Lai, C.

2010-12-01

Two on-site continuous measurements of ozone and its precursors in two megacities of China were carried out in an urban site of Beijing and a suburban site near Guangzhou in the Pearl River Delta (PRD) to estimate precursor consumption and to assess its relationship with oxidant (O3+NO2) formation level. An observation-based method (OBM) with the precursor consumption concept was adopted to assess the relationship between oxidant production and amounts of photochemically consumed non-methane hydrocarbons (NMHCs). In this approach, the ratio of ethylbenzene to m,p-xylenes was used to estimate the degree of photochemical processing, as well as the amounts of photochemically consumed NMHCs by reacting with OH. By trying to correlate the observed oxidant with the observed NMHC concentration, the two areas both revealed nearly no to low correlation between them. However, it existed fair to good correlations (R2=0.68 for Beijing, 0.53 for PRD) between the observed oxidant level and the degree of photochemical processing (ethylbenzene/m,p-xylenes). Furthermore, after taking the approach of consumption to estimate the consumed amounts of NMHCs, an interesting finding reveals that the definite correlation existed between the observed oxidant level and the total consumed NMHCs. The good correlations (R2=0.83 for Beijing, 0.81 for PRD) implies that the ambient oxidant level correlated to the amount of consumed NMHCs. The results of the two megacities in China by using the OBM with the precursor consumption concept can provide another pathway to explore the relationship between photochemically produced oxidant and consumed precursors, and will be helpful to validate model results and to reduce uncertainty of model predictions. However, the method has some room for uncertainty, as injection of fresh precursor emissions and additional boundary ozone involved, etc. could affect the estimation of consumed NMHCs and observed oxidant levels. Assistance of approaches in assessing the

Biogenic, biomass and biofuel sources of trace gases in southern Africa

CSIR Research Space (South Africa)

Otter, LB

2001-03-01

Full Text Available Biogenic processes in southern African savannas are estimated to produce 1.0 Tg NO yr(-1), 44.2-87.8 Tg C yr(-1) as non-methane hydrocarbons (NMHCs) and to consume 0.23 Tg CH4 yr(-1). Floodplains and wetlands in southern Africa are estimated...

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-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.

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.

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

Science.gov (United States)

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

2017-06-20

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

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.

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...

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.

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

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

Characterization of Nonmethane Hydrocarbons at Three Urban Sites in Western Saudi Arabia, in Lahore (Pakistan), and in Singapore

Science.gov (United States)

Barletta, B.; Simpson, I. J.; Blake, N. J.; Meinardi, S.; Aburizaiza, O. S.; Siddique, A.; Zeb, J.; Yu, L. E.; Khwaja, H. A.; Farrukh, M. A.; Blake, D. R.

2014-12-01

Favorable conditions to tropospheric ozone (O3) formation are present over the Persian Gulf Region. Ozone is a well known pollutant affecting human health and natural ecosystems. Among the several factors contributing to the formation of the O3 hot spot over the Middle East, the presence of local emissions of its precursors needs to be considered. We report initial measurements of a suite of nonmethane hydrocarbons (NMHCs), an important component of volatile organic compounds (VOCs), which, coupled with nitrogen oxides in the presence of sunlight, are key chemical precursors of tropospheric O3. We measured 63 speciated C2-C10 NMHCs, in addition to methane (CH4) and carbon monoxide (CO) in three cities of Saudi Arabia (Jeddah, Mecca, and Madina; October-November 2012 and April 2013) and in the city of Lahore (Pakistan; December 2012). To put these data into perspective, we compare our results to data collected in Singapore (August-November 2012). We observed enhanced levels in all three Saudi Arabian cities compared to the local background and to those measured in Singapore. However, the Saudi levels are much lower than those measured in Lahore, where the sum of quantified NMHCs is about six times higher. For Madina, enhanced levels of the alkenes, ethyne and CO indicated that vehicle exhaust was the dominant source. In Jeddah and Mecca, the most abundant NMHC were the alkanes (47-61% of total measured NMHCs), which are more closely associated with emissions from natural gas, liquid petroleum gas (LPG), and gasoline evaporation. In Lahore, the hydroxyl radical (OH) reactivity, used to evaluate the importance of the different measured species toward ozone production, is three to six times higher than for the Saudi cities, and more than 20 times higher than for Singapore. For all urban areas reported here, among the measured compounds, the alkenes (especially ethene and propene) dominate in terms of OH reactivity because of a combination of their great abundance and

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

Science.gov (United States)

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

2017-09-05

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

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

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.

O3, CH4, CO2, CO, NO2 and NMHC aircraft measurements in the Uinta Basin oil and gas region under low and high ozone conditions in winter 2012 and 2013

Directory of Open Access Journals (Sweden)

S. J. Oltmans

2016-10-01

Full Text Available Abstract Instrumented aircraft measuring air composition in the Uinta Basin, Utah, during February 2012 and January-February 2013 documented dramatically different atmospheric ozone (O3 mole fractions. In 2012 O3 remained near levels of ∼40 ppb in a well-mixed 500–1000 m deep boundary layer while in 2013, O3 mole fractions >140 ppb were measured in a shallow (∼200 m boundary layer. In contrast to 2012 when mole fractions of emissions from oil and gas production such as methane (CH4, non-methane hydrocarbons (NMHCs and combustion products such as carbon dioxide (CO2 were moderately elevated, in winter 2013 very high mole fractions were observed. Snow cover in 2013 helped produce and maintain strong temperature inversions that capped a shallow cold pool layer. In 2012, O3 and CH4 and associated NMHCs mole fractions were not closely related. In 2013, O3 mole fractions were correlated with CH4 and a suite of NMHCs identifying the gas field as the primary source of the O3 precursor NMHC emissions. In 2013 there was a strong positive correlation between CH4 and CO2 suggesting combustion from oil and natural gas processing activities. The presence of O3 precursor NMHCs through the depth of the boundary layer in 2013 led to O3 production throughout the layer. In 2013, O3 mole fractions increased over the course of the week-long episodes indicating O3 photochemical production was larger than dilution and deposition rates, while CH4 mole fractions began to level off after 3 days indicative of some air being mixed out of the boundary layer. The plume of a coal-fired power plant located east of the main gas field was not an important contributor to O3 or O3 precursors in the boundary layer in 2013.

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

Emission and profile characteristic of volatile organic compounds emitted from coke production, iron smelt, heating station and power plant in Liaoning Province, China.

Science.gov (United States)

Shi, Jianwu; Deng, Hao; Bai, Zhipeng; Kong, Shaofei; Wang, Xiuyan; Hao, Jiming; Han, Xinyu; Ning, Ping

2015-05-15

107 kinds of C₂-C₁₂ volatile organic compound (VOC) mass concentrations and profiles for four types of coal-fired stationary sources in Liaoning Province were studied by a dilution sampling system and GC-MS analysis method, which are of significant importance with regard to VOC emissions in northeast of China. The results showed that there were some differences among these VOC source profiles. The total mass concentrations of analyzed 107 VOC species varied from 10,917 to 19,652 μg m(-3). Halogenated hydrocarbons exhibited higher mass percentages for the VOC source profiles of iron smelt (48.8%) and coke production plant (37.7%). Aromatic hydrocarbons were the most abundant in heating station plant (69.1%). Ketones, alcohols and acetates held 45.0% of total VOCs in thermal power plant. For non-methane hydrocarbons (NMHCs), which are demanded for photochemical assessment in the USA, toluene and n-hexane were the most abundant species in the iron smelt, coke production and thermal power plant, with the mass percentages of 64.8%, 52.7% and 38.6%, respectively. Trimethylbenzene, n-propylbenzene and o,m-ethyltoluene approximately accounted for 70.0% in heating station plant. NMHCs emitted from coke production, iron smelt, heating station and power plant listed above presented different chemical reactivities. The average OH loss rate of NMHCs from heating station, was 4 to 5.6 times higher than that of NMHCs from iron smelt, coke production and power plant, which implies that VOCs emitted from heating station in northeast of China should be controlled firstly to avoid photochemical ozone pollution and protect human health. There are significant variations in the ratios of benzene/toluene and m, p-xylene/ethylbenzene of these coal-fired source profiles. The representativeness of the coal-fired sources studied and the VOC samples collected should be more closely examined. The accuracy of VOC source profiles related to coal-fired processes is highly dependent on

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

Estimating the Biogenic Non-Methane Hydrocarbon Emissions over Greece

Directory of Open Access Journals (Sweden)

Ermioni Dimitropoulou

2018-01-01

Full Text Available Biogenic emissions affect the urban air quality as they are ozone and secondary organic aerosol (SOA precursors and should be taken into account when applying photochemical pollution models. The present study presents an estimation of the magnitude of non-methane volatile organic compounds (BNMVOCs emitted by vegetation over Greece. The methodology is based on computation developed with the aid of a Geographic Information System (GIS and theoretical equations in order to produce an emission inventory on a 6 × 6 km2 spatial resolution, in a temporal resolution of 1 h covering one year (2016. For this purpose, a variety of input data was used: updated satellite land-use data, land-use specific emission potentials, foliar biomass densities, temperature, and solar radiation data. Hourly, daily, and annual isoprene, monoterpenes, and other volatile organic compounds (OVOCs were estimated. In the area under study, the annual biogenic emissions were estimated up to 472 kt, consisting of 46.6% isoprene, 28% monoterpenes, and 25.4% OVOCs. Results delineate an annual cycle with increasing values from March to April, while maximum emissions were observed from May to September, followed by a decrease from October to January.

Estimates of global biomass burning emissions for reactive greenhouse gases (CO, NMHCs, and NOx) and CO2

Science.gov (United States)

Jain, Atul K.; Tao, Zhining; Yang, Xiaojuan; Gillespie, Conor

2006-03-01

Open fire biomass burning and domestic biofuel burning (e.g., cooking, heating, and charcoal making) algorithms have been incorporated into a terrestrial ecosystem model to estimate CO2 and key reactive GHGs (CO, NOx, and NMHCs) emissions for the year 2000. The emissions are calculated over the globe at a 0.5° × 0.5° spatial resolution using tree density imagery, and two separate sets of data each for global area burned and land clearing for croplands, along with biofuel consumption rate data. The estimated global and annual total dry matter (DM) burned due to open fire biomass burning ranges between 5221 and 7346 Tg DM/yr, whereas the resultant emissions ranges are 6564-9093 Tg CO2/yr, 438-568 Tg CO/yr, 11-16 Tg NOx/yr (as NO), and 29-40 Tg NMHCs/yr. The results indicate that land use changes for cropland is one of the major sources of biomass burning, which amounts to 25-27% (CO2), 25 -28% (CO), 20-23% (NO), and 28-30% (NMHCs) of the total open fire biomass burning emissions of these gases. Estimated DM burned associated with domestic biofuel burning is 3,114 Tg DM/yr, and resultant emissions are 4825 Tg CO2/yr, 243 Tg CO/yr, 3 Tg NOx/yr, and 23 Tg NMHCs/yr. Total emissions from biomass burning are highest in tropical regions (Asia, America, and Africa), where we identify important contributions from primary forest cutting for croplands and domestic biofuel burning.

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.

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 ...

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

Importance of data comparability for multi-year trends and source apportionment of NMHC concentrations observed in France

Science.gov (United States)

Sauvage, Stéphane; Waked, Antoine; Leonardis, Thierry; Locoge, Nadine

2017-04-01

Non Methane Hydrocarbon Compounds (NMHCs) are of interest due to their potential health impact and their key role in atmospheric processes as precursors of secondary pollutants such as ozone (O3) and secondary organic aerosols (SOA). Hourly measurements of 31 non-methane hydrocarbons (NMHCs) were carried out at three urban sites in France over the period of a decade. The trends analysis 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 known as tracers of distant sources and natural gas remained constant. These trends are consistent with those recently described at urban and background sites in the northern mid-latitudes and with emission inventories. They are compared with the ones reported for 3 French rural sites (EMEP). A year per year source apportionment study using PMF was also conducted for 2 of the urban sites over the period 2005-2013. Using source fingerprints, five common anthropogenic sources were identified for Paris and Strasbourg: traffic-exhaust emissions (21±5%, 18±5%), evaporative sources (17±4%, 24±7%), natural gas & background (22±5%, 25±5%), residential heating (17±4%, 17±5%) and solvent use (19±7%, 12±5%). Biogenic sources were also identified and accounted for 4±1% of the total measured NMHC's at both sites. Along the presentation, the robustness of these results will be discussed regarding the site representativeness, the data comparability, and the temporal variation of the data quality

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

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.

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.

SUPPLEMENTARY INFORMATION Non-oxidative methane ...

Indian Academy of Sciences (India)

dell

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

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)

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...

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.

Variations and sources of ambient formaldehyde for the 2008 Beijing Olympic games

Science.gov (United States)

Li, Yang; Shao, Min; Lu, Sihua; Chang, Chih-Chung; Dasgupta, Purnendu K.

2010-07-01

As the host city of the 2008 Olympic games, Beijing implemented a series of air pollution control measures before and during the Olympic games. Ambient formaldehyde (HCHO) concentrations were measured using a fluorometric instrument based on a diffusion scrubber and the Hantzsch reaction; hydrocarbons were simultaneously measured using gas chromatography-mass spectrometry (GC-MS). Meteorological parameters, CO, O 3, and NO 2 concentrations were measured by standard commercial instrumentation. In four separate periods: (a) before the vehicle plate number control (3-19 July); (b) during the Olympic Games (8-24 August); (c) during the Paralympic Games (6-17 September) and (d) after the vehicle control was ceased (21-28 September), the average HCHO mixing ratios were 7.31 ± 2.67 ppbv, 5.54 ± 2.41 ppbv, 8.72 ± 2.48 ppbv, and 6.42 ± 2.79 ppbv, while the total non-methane hydrocarbons (NMHCs) measured were 30.41 ± 18.08 ppbv, 18.12 ± 9.38 ppbv, 30.50 ± 13.37 ppbv, and 33.33 ± 15.85 ppbv, respectively. Both HCHO and NMHC levels were the lowest during the Olympic games, and increased again during the Paralympic games even with the same vehicle control measures operative. Similar diurnal HCHO and O 3 patterns indicated that photo-oxidation of NMHCs may be the major source of HCHO. The diurnal profile of total NMHCs was very similar to that of NO 2 and CO: morning and evening peaks appeared in rush hours, indicating even after strict vehicle control, automobile emission may still be the dominant source of the HCHO precursors. The contributions of HCHO, alkanes, alkenes, and aromatics to OH loss rates were also calculated. HCHO contributed 22 ± 3% to the total VOCs and 24 ± 1% to the total OH loss rate. HCHO was not only important in term of abundance, but also important in chemical reactivity in the air.

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.

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.

Averaged emission factors for the Hungarian car fleet

Energy Technology Data Exchange (ETDEWEB)

Haszpra, L. [Inst. for Atmospheric Physics, Budapest (Hungary); Szilagyi, I. [Central Research Inst. for Chemistry, Budapest (Hungary)

1995-12-31

The vehicular emission of non-methane hydrocarbon (NMHC) is one of the largest anthropogenic sources of NMHC in Hungary and in most of the industrialized countries. Non-methane hydrocarbon plays key role in the formation of photo-chemical air pollution, usually characterized by the ozone concentration, which seriously endangers the environment and human health. The ozone forming potential of the different NMHCs differs from each other significantly, while the NMHC composition of the car exhaust is influenced by the fuel and engine type, technical condition of the vehicle, vehicle speed and several other factors. In Hungary the majority of the cars are still of Eastern European origin. They represent the technological standard of the 70`s, although there are changes recently. Due to the long-term economical decline in Hungary the average age of the cars was about 9 years in 1990 and reached 10 years by 1993. The condition of the majority of the cars is poor. In addition, almost one third (31.2 %) of the cars are equipped with two-stroke engines which emit less NO{sub x} but much more hydrocarbon. The number of cars equipped with catalytic converter was negligible in 1990 and is slowly increasing only recently. As a consequence of these facts the traffic emission in Hungary may differ from that measured in or estimated for the Western European countries and the differences should be taken into account in the air pollution models. For the estimation of the average emission of the Hungarian car fleet a one-day roadway tunnel experiment was performed in the downtown of Budapest in summer, 1991. (orig.)

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.

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.

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

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

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)

Biogenic non-methane hydrocarbons (NMHC). Nature`s contribution to regional and global atmospheric chemistry

Energy Technology Data Exchange (ETDEWEB)

Klockow, D.; Hoffman, T. [Inst. of Spectrochemistry and Applied Spectroscopy, Dortmund (Germany)

1995-12-31

Terrestrial vegetation provides an important source of volatile hydrocarbons, especially isoprene, monoterpenes and in addition possibly sesquiterpenes as well as oxygenated compounds. Although there exist considerable uncertainties in the estimation of the magnitude of these biogenic NMHC emissions, it is generally accepted that the majority of global NMHC release is from natural and not from anthropogenic sources. Taking into consideration the high reactivity of the mostly unsaturated biogenic emissions, their impact on tropospheric processes can be assumed to be of great importance. Together with anthropogenic NO{sub x} emissions, the highly reactive natural alkenes can act as precursors in photochemical oxidant formation and contribute to regional-scale air pollution. Their oxidation in the atmosphere and the subsequent gas-to-particle conversion of the products lead to the formation of organic aerosols. Because of the formation of phytotoxic compounds, the interaction of the biogenic hydrocarbons with ozone inside or outside the leaves and needles of plants has been suggested to play a role in forest decline. (author)

Biogenic non-methane hydrocarbons (NMHC). Nature`s contribution to regional and global atmospheric chemistry

Energy Technology Data Exchange (ETDEWEB)

Klockow, D; Hoffman, T [Inst. of Spectrochemistry and Applied Spectroscopy, Dortmund (Germany)

1996-12-31

Terrestrial vegetation provides an important source of volatile hydrocarbons, especially isoprene, monoterpenes and in addition possibly sesquiterpenes as well as oxygenated compounds. Although there exist considerable uncertainties in the estimation of the magnitude of these biogenic NMHC emissions, it is generally accepted that the majority of global NMHC release is from natural and not from anthropogenic sources. Taking into consideration the high reactivity of the mostly unsaturated biogenic emissions, their impact on tropospheric processes can be assumed to be of great importance. Together with anthropogenic NO{sub x} emissions, the highly reactive natural alkenes can act as precursors in photochemical oxidant formation and contribute to regional-scale air pollution. Their oxidation in the atmosphere and the subsequent gas-to-particle conversion of the products lead to the formation of organic aerosols. Because of the formation of phytotoxic compounds, the interaction of the biogenic hydrocarbons with ozone inside or outside the leaves and needles of plants has been suggested to play a role in forest decline. (author)

Effect of traffic restriction on reducing ambient volatile organic compounds (VOCs): Observation-based evaluation during a traffic restriction drill in Guangzhou, China

Science.gov (United States)

Huang, Xinyu; Zhang, Yanli; Yang, Weiqiang; Huang, Zuzhao; Wang, Yujun; Zhang, Zhou; He, Quanfu; Lü, Sujun; Huang, Zhonghui; Bi, Xinhui; Wang, Xinming

2017-07-01

Traffic restriction (TR) is a widely adopted control measure in case of heavy air pollution particularly in urban areas, yet it is hard to evaluate the effect of TR on reducing VOC emissions based on monitoring data since ambient VOC mixing ratios are influenced not only by source emissions but also by meteorological conditions and atmospheric degradation. Here we collected air samples for analysis of VOCs before, during and after a TR drill carried out in Guangzhou in September 2010 at both a roadside and a rooftop (∼50 m above the ground) site. TR measures mainly included the "odd-even license" rule and banning high-emitting "yellow label" vehicles. The mixing ratios of non-methane hydrocarbons (NMHCs) did not show significant changes at the roadside site with total NMHCs of 39.0 ± 11.8 ppbv during non-TR period and 39.1 ± 14.8 ppbv during TR period, whereas total NMHCs decreased from 30.4 ± 14.3 ppbv during the non-TR period to 22.1 ± 10.6 ppbv during the TR period at rooftop site. However, the ratios of methyl tert-butyl ether (MTBE), benzene and toluene against carbon monoxide (MTBE/CO, T/CO and B/CO) at the both sampling sites dropped significantly. The ratios of toluene to benzene (T/B) instead increased significantly. Changes in these ratios all consistently indicated reduced input from traffic emissions particularly gasoline vehicles. Source attribution by positive matrix factorization (PMF) confirmed that during the TR period gasoline vehicles contributed less VOCs in percentages while industrial sources, biomass burning and LPG shared larger percentages. Assuming that emissions from industrial sources remained unchanged during the TR and non-TR periods, we further used the PMF-retrieved contribution percentages to deduce the reduction rate of traffic-related VOC emissions, and obtained a reduction rate of 31% based on monitoring data at the roadside site and of 34% based on the monitoring data at the rooftop site. Considering VOC emissions from all

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...

Open burning of rice, corn and wheat straws: primary emissions, photochemical aging, and secondary organic aerosol formation

Science.gov (United States)

Fang, Zheng; Deng, Wei; Zhang, Yanli; Ding, Xiang; Tang, Mingjin; Liu, Tengyu; Hu, Qihou; Zhu, Ming; Wang, Zhaoyi; Yang, Weiqiang; Huang, Zhonghui; Song, Wei; Bi, Xinhui; Chen, Jianmin; Sun, Yele; George, Christian; Wang, Xinming

2017-12-01

Agricultural residues are among the most abundant biomass burned globally, especially in China. However, there is little information on primary emissions and photochemical evolution of agricultural residue burning. In this study, indoor chamber experiments were conducted to investigate primary emissions from open burning of rice, corn and wheat straws and their photochemical aging as well. Emission factors of NOx, NH3, SO2, 67 non-methane hydrocarbons (NMHCs), particulate matter (PM), organic aerosol (OA) and black carbon (BC) under ambient dilution conditions were determined. Olefins accounted for > 50 % of the total speciated NMHCs emission (2.47 to 5.04 g kg-1), indicating high ozone formation potential of straw burning emissions. Emission factors of PM (3.73 to 6.36 g kg-1) and primary organic carbon (POC, 2.05 to 4.11 gC kg-1), measured at dilution ratios of 1300 to 4000, were lower than those reported in previous studies at low dilution ratios, probably due to the evaporation of semi-volatile organic compounds under high dilution conditions. After photochemical aging with an OH exposure range of (1.97-4.97) × 1010 molecule cm-3 s in the chamber, large amounts of secondary organic aerosol (SOA) were produced with OA mass enhancement ratios (the mass ratio of total OA to primary OA) of 2.4-7.6. The 20 known precursors could only explain 5.0-27.3 % of the observed SOA mass, suggesting that the major precursors of SOA formed from open straw burning remain unidentified. Aerosol mass spectrometry (AMS) signaled that the aged OA contained less hydrocarbons but more oxygen- and nitrogen-containing compounds than primary OA, and carbon oxidation state (OSc) calculated with AMS resolved O / C and H / C ratios increased linearly (p < 0.001) with OH exposure with quite similar slopes.

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.

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

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...

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.

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).

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).

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.

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.

Volatile Organic Compounds (VOCs) Measurements in Karachi, Pakistan (2006): a Comparison With Previous Urban Sampling Campaigns Worldwide.

Science.gov (United States)

Barletta, B.; Meinardi, S.; Khwaja, H. A.; Beyersdorf, A. J.; Baker, A. K.; Zou, S.; Rowland, F.; Blake, D. R.

2008-12-01

Mixing ratios of carbon monoxide (CO), carbon dioxide (CO2), methane (CH4), and 47 nonmethane hydrocarbons - NMHCs - (19 alkanes, 13 alkenes, ethyne, and 14 aromatics) were determined for ground level whole air samples collected during the winter of 2006 in Karachi, Pakistan. Pakistan is among the fastest growing economies in Asia, and Karachi is one of the largest cities in the world with a rapidly expanding population of over 14 million in the whole metropolitan area, and a large industrial base. Samples were collected in January 2006 throughout the urban area to characterize the overall air composition of the city, and along the busiest road to determine the traffic signature of Karachi. This sampling campaign follows a previous study carried out in the winter of 1998-1999 in the same city, when elevated concentrations of many NMHCs were observed. Exceptionally high levels of methane were still observed in 2006 with an average mixing ratio of 5.0 ppmv (6.3 ppmv were observed in 1999). The overall air composition of the Karachi urban environment characterized during this 2006 sampling is compared to 1999 aiming to highlight any possible change in the main VOC sources present throughout the city. In particular, we want to evaluate the impact of the heavy usage of natural gas on the overall air quality of Karachi and the recently increased use of liquefied petroleum gas (LPG) as alternative source of energy. We also compare the composition of the urban troposphere of Karachi to other major urban centers worldwide such as Guangzhou (China), Mexico City (Mexico), and Milan (Italy).

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.

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.

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)

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.

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

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.

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.)

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.)

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

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)

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.

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 .

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

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.

Ozone production in summer in the megacities of Tianjin and Shanghai, China: a comparative study

Directory of Open Access Journals (Sweden)

L. Ran

2012-08-01

Full Text Available Rapid economic growth has given rise to a significant increase in ozone precursor emissions in many regions of China, especially in the densely populated North China Plain (NCP and Yangtze River Delta (YRD. Improved understanding of ozone formation in response to different precursor emissions is imperative to address the highly nonlinear ozone problem and to provide a solid scientific basis for efficient ozone abatement in these regions. A comparative study on ozone photochemical production in summer has thus been carried out in the megacities of Tianjin (NCP and Shanghai (YRD. Two intensive field campaigns were carried out respectively at an urban and a suburban site of Tianjin, in addition to routine monitoring of trace gases in Shanghai, providing data sets of surface ozone and its precursors including nitrogen oxides (NO_x and various non-methane hydrocarbons (NMHCs. Ozone pollution in summer was found to be more severe in the Tianjin region than in the Shanghai region, based on either the frequency or the duration of high ozone events. Such differences might be attributed to the large amount of highly reactive NMHCs in Tianjin. Industry related species like light alkenes were of particular importance in both urban and suburban Tianjin, while in Shanghai aromatics dominated. In general, the ozone problem in Shanghai is on an urban scale. Stringent control policies on local emissions would help reduce the occurrence of high ozone concentrations. By contrast, ozone pollution in Tianjin is probably a regional problem. Combined efforts to reduce ozone precursor emissions on a regional scale must be undertaken to bring the ozone problem under control.

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.

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.

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.

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.

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.

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.

Biomass burning contribution to ambient volatile organic compounds (VOCs) in the Chengdu-Chongqing Region (CCR), China

Science.gov (United States)

Li, Lingyu; Chen, Yuan; Zeng, Limin; Shao, Min; Xie, Shaodong; Chen, Wentai; Lu, Sihua; Wu, Yusheng; Cao, Wei

2014-12-01

Ambient volatile organic compounds (VOCs) were measured intensively using an online gas chromatography-mass spectrometry/flame ionization detector (GC-MS/FID) at Ziyang in the Chengdu-Chongqing Region (CCR) from 6 December 2012 to 4 January 2013. Alkanes contributed the most (59%) to mixing ratios of measured non-methane hydrocarbons (NMHCs), while aromatics contributed the least (7%). Methanol was the most abundant oxygenated VOC (OVOC), contributing 42% to the total amount of OVOCs. Significantly elevated VOC levels occurred during three pollution events, but the chemical composition of VOCs did not differ between polluted and clean days. The OH loss rates of VOCs were calculated to estimate their chemical reactivity. Alkenes played a predominant role in VOC reactivity, among which ethylene and propene were the largest contributors; the contributions of formaldehyde and acetaldehyde were also considerable. Biomass burning had a significant influence on ambient VOCs during our study. We chose acetonitrile as a tracer and used enhancement ratio to estimate the contribution of biomass burning to ambient VOCs. Biomass burning contributed 9.4%-36.8% to the mixing ratios of selected VOC species, and contributed most (>30% each) to aromatics, formaldehyde, and acetaldehyde.

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)

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

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.

Characterization of volatile organic compounds at a roadside environment in Hong Kong: An investigation of influences after air pollution control strategies

Science.gov (United States)

Huang, Yu; Ling, Zhen Hao; Lee, Shun Cheng; Ho, Steven Sai Hang; Cao, Jun Ji; Blake, Donald R.; Cheng, Yan; Lai, Sen Chao; Ho, Kin Fai; Gao, Yuan; Cui, Long; Louie, Peter K. K.

2015-12-01

Vehicular emission is one of the important anthropogenic pollution sources for volatile organic compounds (VOCs). Four characterization campaigns were conducted at a representative urban roadside environment in Hong Kong between May 2011 and February 2012. Carbon monoxide (CO) and VOCs including methane (CH4), non-methane hydrocarbons (NMHCs), halocarbons, and alkyl nitrates were quantified. Both mixing ratios and compositions of the target VOCs show ignorable seasonal variations. Except CO, liquefied petroleum gas (LPG) tracers of propane, i-butane and n-butane are the three most abundant VOCs, which increased significantly as compared with the data measured at the same location in 2003. Meanwhile, the mixing ratios of diesel- and gasoline tracers such as ethyne, alkenes, aromatics, halogenated, and nitrated hydrocarbons decreased by at least of 37%. The application of advanced multivariate receptor modeling technique of positive matrix factorization (PMF) evidenced that the LPG fuel consumption is the largest pollution source, accounting for 60 ± 5% of the total quantified VOCs at the roadside location. The sum of ozone formation potential (OFP) for the target VOCs was 300.9 μg-O3 m-3, which was 47% lower than the value of 567.3 μg-O3 m-3 measured in 2003. The utilization of LPG as fuel in public transport (i.e., taxis and mini-buses) contributed 51% of the sum of OFP, significantly higher than the contributions from gasoline- (16%) and diesel-fueled (12%) engine emissions. Our results demonstrated the effectiveness of the switch from diesel to LPG-fueled engine for taxis and mini-buses implemented by the Hong Kong Special Administrative Region (HKSAR) Government between the recent ten years, in additional to the execution of substitution to LPG-fueled engine and restrictions of the vehicular emissions in compliance with the updated European emission standards.

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.

Multi-year (2004–2008 record of nonmethane hydrocarbons and halocarbons in New England: seasonal variations and regional sources

Directory of Open Access Journals (Sweden)

R. S. Russo

2010-05-01

Full Text Available Multi-year time series records of C₂-C₆ alkanes, C₂-C₄ alkenes, ethyne, isoprene, C₆-C₈ aromatics, trichloroethene (C₂HCl₃, and tetrachloroethene (C₂Cl₄ from canister samples collected during January 2004–February 2008 at the University of New Hampshire (UNH AIRMAP Observatory at Thompson Farm (TF in Durham, NH are presented. The objectives of this work are to identify the sources of nonmethane hydrocarbons (NMHCs and halocarbons observed at TF, characterize the seasonal and interannual variability in ambient mixing ratios and sources, and estimate regional emission rates of NMHCs. Analysis of correlations and comparisons with emission ratios indicated that a ubiquitous and persistent mix of emissions from several anthropogenic sources is observed throughout the entire year. The highest C₂-C₈ anthropogenic NMHC mixing ratios were observed in mid to late winter. Following the springtime minimums, the C₃-C₆ alkanes, C₇-C₈ aromatics, and C₂HCl₃ increased in early to mid summer, presumably reflecting enhanced evaporative emissions. Mixing ratios of C₂Cl₄ and C₂HCl₃ decreased by 0.7±0.2 and 0.3±0.05 pptv/year, respectively, which is indicative of reduced usage and emissions of these halogenated solvents. Emission rates of C₃-C₈ NMHCs were estimated to be 10⁹ to 10¹⁰ molecules cm⁻² s⁻¹ in winter 2006. The emission rates extrapolated to the state of New Hampshire and New England were ~2–60 Mg/day and ~12–430 Mg/day, respectively. Emission rates of benzene, toluene, ethylbenzene, xylenes, and ethyne in the 2002 and 2005 EPA National Emissions Inventories were within ±50% of the TF emission rates.

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

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

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

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.

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.

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.

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)

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.

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

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

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.

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...

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

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.

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.)

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

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.

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.

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.

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.

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 (

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.

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

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

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)

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

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

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 (...

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.

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.

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)

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

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.

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.

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.

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

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)

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.

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

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.

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.

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.

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.

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.

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.

Chemical evolution of volatile organic compounds in the outflow of the Mexico City Metropolitan area

Energy Technology Data Exchange (ETDEWEB)

Apel, Eric; Emmons, L.; Karl, Thomas G.; Flocke, Frank M.; Hills, A. J.; Madronich, Sasha; Lee-Taylor, J.; Fried, Alan; Weibring, P.; Walega, J.; Richter, Dirk; Tie, X.; Mauldin, L.; Campos, Teresa; Weinheimer, Andrew J.; Knapp, David; Sive, B.; Kleinman, Lawrence I.; Springston, S.; Zaveri, Rahul A.; Ortega, John V.; Voss, Paul B.; Blake, D. R.; Baker, Angela K.; Warneke, Carsten; Welsh-Bon, Daniel; de Gouw, Joost A.; Zheng, J.; Zhang, Renyi; Rudolph, Jochen; Junkermann, W.; Riemer, D.

2010-01-01

The volatile organic compound (VOC) distribution in the Mexico City Metropolitan Area (MCMA) and its evolution as it is uplifted and transported out of the MCMA basin was studied during the 2006 MILAGRO/MIRAGE-Mex field campaign. The results show that in the morning hours in the city center, the VOC distribution is dominated by non-methane hydrocarbons (NMHCs) but with a substantial contribution from oxygenated volatile organic compounds (OVOCs), predominantly from primary emissions. Alkanes account for a large part of the NMHC distribution in terms of mixing ratios. In terms of reactivity, NMHCs also dominate overall, especially in the morning hours. However, in the afternoon, as the boundary layer lifts and air is mixed and aged within the basin, the distribution changes as secondary products are formed. The WRF-Chem (Weather Research and Forecasting with Chemistry) model and MOZART (Model for Ozone and Related chemical Tracers) were able to reproduce the general features of the daytime cycle of the VOC OH reactivity distribution showing that NMHCs dominate the distribution except in the afternoon hours and that the VOC OH reactivity peaks in the early morning due to high morning emissions from the city into a shallow boundary layer. The WRF-Chem and MOZART models showed higher reactivity than the experimental data during the nighttime cycle, perhaps indicating problems with the modeled nighttime boundary layer height. In addition, a plume was studied in which air was advected out of the MCMA and intercepted downwind with the DOE G1 on March 18 and the NCAR C130 one day later on March 19. A number of identical species measured aboard each aircraft gave insight into the chemical evolution of the plume as it aged and was transported as far as 1000 km downwind. Ozone and many OVOCs were photochemically produced in the plume. The WRF-Chem and MOZART models were used to examine the spatial and temporal extent of the March 19 plume and to help interpret the OH

Chemical evolution of volatile organic compounds in the outflow of the Mexico City Metropolitan area

Energy Technology Data Exchange (ETDEWEB)

Apel, E.; Springston, S.; Karl, T.; Emmons, L.; Flocke, F.; Hills, A. J.; Madronich, S.; Lee-Taylor, J.; Fried, A.; Weibring, P.; Walega, J.; Richter, D., Tie, X.; Mauldin, L.; Campos, T.; Sive, B.; Kleinman, L.; Springston, S., Zaveri, R.; deGouw, J.; Zheng, J.; Zhang, R.; Rudolph, J.; Junkermann, W.; Riemer, D. D.

2009-11-01

The volatile organic compound (VOC) distribution in the Mexico City Metropolitan Area (MCMA) and its evolution as it is uplifted and transported out of the MCMA basin was studied during the 2006 MILAGRO/MIRAGE-Mex field campaign. The results show that in the morning hours in the city center, the VOC distribution is dominated by non-methane hydrocarbons (NMHCs) but with a substantial contribution from oxygenated volatile organic compounds (OVOCs), predominantly from primary emissions. Alkanes account for a large part of the NMHC distribution in terms of mixing ratios. In terms of reactivity, NMHCs also dominate overall, especially in the morning hours. However, in the afternoon, as the boundary layer lifts and air is mixed and aged within the basin, the distribution changes as secondary products are formed. The WRF-Chem (Weather Research and Forecasting with Chemistry) model and MOZART (Model for Ozone and Related chemical Tracers) were able to reproduce the general features of the daytime cycle of the VOC OH reactivity distribution showing that NMHCs dominate the distribution except in the afternoon hours and that the VOC OH reactivity peaks in the early morning due to high morning emissions from the city into a shallow boundary layer. The WRF-Chem and MOZART models showed higher reactivity than the experimental data during the nighttime cycle, perhaps indicating problems with the modeled nighttime boundary layer height. In addition, a plume was studied in which air was advected out of the MCMA and intercepted downwind with the DOE G1 on 18 March and the NCAR C130 one day later on 19 March. A number of identical species measured aboard each aircraft gave insight into the chemical evolution of the plume as it aged and was transported as far as 1000 km downwind. Ozone and many OVOCs were photochemically produced in the plume. The WRF-Chem and MOZART models were used to examine the spatial and temporal extent of the 19 March plume and to help interpret the OH

Chemical evolution of volatile organic compounds in the outflow of the Mexico City Metropolitan area

Directory of Open Access Journals (Sweden)

E. C. Apel

2010-03-01

Full Text Available The volatile organic compound (VOC distribution in the Mexico City Metropolitan Area (MCMA and its evolution as it is uplifted and transported out of the MCMA basin was studied during the 2006 MILAGRO/MIRAGE-Mex field campaign. The results show that in the morning hours in the city center, the VOC distribution is dominated by non-methane hydrocarbons (NMHCs but with a substantial contribution from oxygenated volatile organic compounds (OVOCs, predominantly from primary emissions. Alkanes account for a large part of the NMHC distribution in terms of mixing ratios. In terms of reactivity, NMHCs also dominate overall, especially in the morning hours. However, in the afternoon, as the boundary layer lifts and air is mixed and aged within the basin, the distribution changes as secondary products are formed. The WRF-Chem (Weather Research and Forecasting with Chemistry model and MOZART (Model for Ozone and Related chemical Tracers were able to approximate the observed MCMA daytime patterns and absolute values of the VOC OH reactivity. The MOZART model is also in agreement with observations showing that NMHCs dominate the reactivity distribution except in the afternoon hours. The WRF-Chem and MOZART models showed higher reactivity than the experimental data during the nighttime cycle, perhaps indicating problems with the modeled nighttime boundary layer height.

A northeast transport event was studied in which air originating in the MCMA was intercepted aloft with the Department of Energy (DOE G1 on 18 March and downwind with the National Center for Atmospheric Research (NCAR C130 one day later on 19 March. A number of identical species measured aboard each aircraft gave insight into the chemical evolution of the plume as it aged and was transported as far as 1000 km downwind; ozone was shown to be photochemically produced in the plume. The WRF-Chem and MOZART models were used to examine the spatial extent and temporal evolution of the plume

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

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.

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.

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

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.

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

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.

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

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.

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.

Investigations of Methane Production in Hypersaline Environments

Science.gov (United States)

Bebout, Brad M.

2015-01-01

produced by these sediments. Substrate limitation of methanogenesis in these environments, and not methane oxidation, would explain the isotopic values of the methane in these environments. Incubations with both isotopically labeled and unlabeled putative substrates for methanogenesis have shown that the substrates most important for methanogenesis in these environments are the so-called non-competitive substrates, e.g., methylamines, dimethylsulfide, and methanol. Acetate and bicarbonate appear not to be important substrates for methanogens in these environments. Extraction of DNA and analysis of a gene used for methane production (mcrA) has revealed that the community composition of methanogens is consistent with organisms known to use non-competitive substrates. Our work has shown that hypersaline environments have the potential to both produce and preserve methane for analysis, e.g., by capable rovers. Our work expends the range of methane isotopic values now known to be produced by active methanogenesis

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

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.

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.

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.

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.

Coalbed methane: Clean energy for the world

Science.gov (United States)

Ahmed, A.-J.; Johnston, S.; Boyer, C.; Lambert, S.W.; Bustos, O.A.; Pashin, J.C.; Wray, A.

2009-01-01

Coalbed methane (CBM) has the potential to emerge as a significant clean energy resource. It also has the potential to replace other diminishing hydrocarbon reserves. The latest developments in technologies and methodologies are playing a key role in harnessing this unconventional resource. Some of these developments include adaptations of existing technologies used in conventional oil and gas generations, while others include new applications designed specifically to address coal's unique properties. Completion techniques have been developed that cause less damage to the production mechanisms of coal seams, such as those occurring during cementing operations. Stimulation fluids have also been engineered specifically to enhance CBM production. Deep coal deposits that remain inaccessible by conventional mining operations offer CBM development opportunities.

Community Structure in Methanogenic Enrichments Provides Insight into Syntrophic Interactions in Hydrocarbon-Impacted Environments

DEFF Research Database (Denmark)

Fowler, Jane; Toth, Courtney R. A.; Gieg, Lisa M.

2016-01-01

, but such information has important implications for bioremediation and microbial enhanced energy recovery technologies. Many factors such as changing environmental conditions or substrate variations can influence the composition and biodegradation capabilities of syntrophic microbial communities in hydrocarbon......The methanogenic biodegradation of crude oil involves the conversion of hydrocarbons to methanogenic substrates by syntrophic bacteria and subsequent methane production by methanogens. Assessing the metabolic roles played by various microbial species in syntrophic communities remains a challenge......-impacted environments. In this study, a methanogenic crude oil-degrading enrichment culture was successively transferred onto the single long chain fatty acids palmitate or stearate followed by their parent alkanes, hexadecane or octadecane, respectively, in order to assess the impact of different substrates...

Intrinsic bioremediation of petroleum hydrocarbons in a gas condensate-contaminated aquifer

International Nuclear Information System (INIS)

Gieg, L.M.; McInerney; Tanner, R.S.; Harris, S.H. Jr.; Sublette, K.L.; Suflita, J.M.; Kolhatkar, R.V.

1999-01-01

A study was designed to determine if the intrinsic bioremediation of gas condensate hydrocarbons represented an important fate process in a shallow aquifer underlying a natural gas production site. For over 4 yr, changes in the groundwater, sediment, and vadose zone chemistry in the contaminated portion of the aquifer were interpreted relative to a background zone. Changes included decreased dissolved oxygen and sulfate levels and increased alkalinity, Fe(II), and methane concentrations in the contaminated groundwater, suggesting that aerobic heterotrophic respiration depleted oxygen reserves leaving anaerobic conditions in the hydrocarbon-impacted subsurface. Dissolved hydrogen levels in the contaminated groundwater indicated that sulfate reduction and methanogenesis were predominant biological processes, corroborating the geochemical findings. Furthermore, 10--1000-fold higher numbers of sulfate reducers and methanogens were enumerated in the contaminated sediment relative to background. Putative metabolites were also detected in the contaminated groundwater, including methylbenzylsuccinic acid, a signature intermediate of anaerobic xylene decay. Laboratory incubations showed that benzene, toluene, ethylbenzene, and each of the xylene isomers were biodegraded under sulfate-reducing conditions as was toluene under methanogenic conditions. These results coupled with a decrease in hydrocarbon concentrations in contaminated sediment confirm that intrinsic bioremediation contributes to the attenuation of hydrocarbons in this aquifer

Kinetics of Hydrocarbon formation in a-C:H film deposition plasmas

International Nuclear Information System (INIS)

De la Cal, E.; Tabares, F.L.

1993-01-01

The formation of C 2 and C 3 hydrocarbons during the PACVD of a-C-H films from admixtures of methane with H 2 and He has been investigated by mass spectrometry under several deposition condition. The time evolution of the observed species indicates that the formation mechanism of ethylene and acetylene are sensitive to the conditions of the wall during the growing of the film. Acetylene are sensitive to the conditions of the wall during the growing of the carburized metal. (Author)

When immiscible becomes miscible-Methane in water at high pressures.

Science.gov (United States)

Pruteanu, Ciprian G; Ackland, Graeme J; Poon, Wilson C K; Loveday, John S

2017-08-01

At low pressures, the solubility of gases in liquids is governed by Henry's law, which states that the saturated solubility of a gas in a liquid is proportional to the partial pressure of the gas. As the pressure increases, most gases depart from this ideal behavior in a sublinear fashion, leveling off at pressures in the 1- to 5-kbar (0.1 to 0.5 GPa) range with solubilities of less than 1 mole percent (mol %). This contrasts strikingly with the well-known marked increase in solubility of simple gases in water at high temperature associated with the critical point (647 K and 212 bar). The solubility of the smallest hydrocarbon, the simple gas methane, in water under a range of pressure and temperature is of widespread importance, because it is a paradigmatic hydrophobe and occurs widely in terrestrial and extraterrestrial geology. We report measurements up to 3.5 GPa of the pressure dependence of the solubility of methane in water at 100°C-well below the latter's critical temperature. Our results reveal a marked increase in solubility between 1 and 2 GPa, leading to a state above 2 GPa where the maximum solubility of methane in water exceeds 35 mol %.

Reduction of Non-CO2 Gas Emissions Through The In Situ Bioconversion of Methane

Energy Technology Data Exchange (ETDEWEB)

Scott, A R; Mukhopadhyay, B; Balin, D F

2012-09-06

The primary objectives of this research were to seek previously unidentified anaerobic methanotrophs and other microorganisms to be collected from methane seeps associated with coal outcrops. Subsurface application of these microbes into anaerobic environments has the potential to reduce methane seepage along coal outcrop belts and in coal mines, thereby preventing hazardous explosions. Depending upon the types and characteristics of the methanotrophs identified, it may be possible to apply the microbes to other sources of methane emissions, which include landfills, rice cultivation, and industrial sources where methane can accumulate under buildings. Finally, the microbes collected and identified during this research also had the potential for useful applications in the chemical industry, as well as in a variety of microbial processes. Sample collection focused on the South Fork of Texas Creek located approximately 15 miles east of Durango, Colorado. The creek is located near the subsurface contact between the coal-bearing Fruitland Formation and the underlying Pictured Cliffs Sandstone. The methane seeps occur within the creek and in areas adjacent to the creek where faulting may allow fluids and gases to migrate to the surface. These seeps appear to have been there prior to coalbed methane development as extensive microbial soils have developed. Our investigations screened more than 500 enrichments but were unable to convince us that anaerobic methane oxidation (AMO) was occurring and that anaerobic methanotrophs may not have been present in the samples collected. In all cases, visual and microscopic observations noted that the early stage enrichments contained viable microbial cells. However, as the levels of the readily substrates that were present in the environmental samples were progressively lowered through serial transfers, the numbers of cells in the enrichments sharply dropped and were eliminated. While the results were disappointing we acknowledge that

Impact of pollution controls in Beijing on atmospheric oxygenated volatile organic compounds (OVOCs) during the 2008 Olympic Games: observation and modeling implications

Science.gov (United States)

Liu, Y.; Yuan, B.; Li, X.; Shao, M.; Lu, S.; Li, Y.; Chang, C.-C.; Wang, Z.; Hu, W.; Huang, X.; He, L.; Zeng, L.; Hu, M.; Zhu, T.

2015-03-01

Oxygenated volatile organic compounds (OVOCs) are important products of the photo-oxidation of hydrocarbons. They influence the oxidizing capacity and the ozone-forming potential of the atmosphere. In the summer of 2008, 2 months of emission restrictions were enforced in Beijing to improve air quality during the Olympic Games. Observational evidence reported in related studies that these control measures were efficient in reducing the concentrations of primary anthropogenic pollutants (CO, NOx and non-methane hydrocarbons, i.e., NMHCs) by 30-40%. In this study, the influence of the emission restrictions on ambient levels of OVOCs was explored using a neural network analysis with consideration of meteorological conditions. Statistically significant reductions in formaldehyde (HCHO), acetaldehyde (CH3CHO), methyl ethyl ketone (MEK) and methanol were found to be 12.9, 15.8, 17.1 and 19.6%, respectively, when the restrictions were in place. The effect of emission controls on acetone was not detected in neural network simulations, probably due to pollution transport from surrounding areas outside Beijing. Although the ambient levels of most NMHCs were reduced by ~35% during the full control period, the emission ratios of reactive alkenes and aromatics closely related to automobile sources did not present much difference (zero-dimensional box model based on the Master Chemical Mechanism version 3.2 (MCM3.2) was applied to evaluate how OVOC production responds to the reduced precursors during the emissions control period. On average, secondary HCHO was produced from the oxidation of anthropogenic alkenes (54%), isoprene (30%) and aromatics (15%). The importance of biogenic sources for the total HCHO formation was almost on par with that of anthropogenic alkenes during the daytime. Anthropogenic alkenes and alkanes dominated the photochemical production of other OVOCs such as acetaldehyde, acetone and MEK. The relative changes of modeled HCHO, CH3CHO, methyl vinyl ketone

Catalytic combustion for the elimination of methane, BTEX and other VOC : IV

International Nuclear Information System (INIS)

Hayes, R.E.; Wanke, S.E.

2008-01-01

Options for volatile organic compound combustion include homogeneous combustion (flaring) or catalytic combustion involving a flameless combustion process that uses a solid catalyst to promote the combustion reaction. This presentation discussed relative reactivity testing for volatile organic compounds (VOCs) over commercial catalysts. Several commercial pad catalysts were tested, as well as other powders. The relative reactivity of methane as well as benzene, toluene, ethylbenzene, and xylene (BTEX) were investigated. The purpose of the project was to evaluate combustion of concentrated methane streams that contained BTEX compounds; evaluate catalytic combustion using a counter diffusive radiant heater; develop mathematical models for the reactor to enhance design and understanding; improve the catalyst for BTEX combustion; and target application-dehydrator units. Topics that were addressed in the presentation included methane and benzene conversion; catalytic radiant heaters; small industrial and commercial units; measured temperature distribution; fuel slippage, methane conversion; the effect of water and hydrocarbons; the effect of water-liquid injection; and water addition as vapour. Several observations were offered, including that high percentages of injected liquid water can reduce reactor operating temperature; combustion of BTEX remained highly efficient, however liquid injection could also cause temperature reductions and ultimately the reactor would extinguish; and pre-heating the feed can eliminate the temperature drop and pad wetness problem. It was concluded that BTEX compounds are reactive, and the technology appears promising. 19 figs

Catalytic combustion for the elimination of methane, BTEX and other VOC : IV

Energy Technology Data Exchange (ETDEWEB)

Hayes, R.E.; Wanke, S.E. [Alberta Univ., Edmonton, AB (Canada). Dept. of Chemical and Materials Engineering

2008-07-01

Options for volatile organic compound combustion include homogeneous combustion (flaring) or catalytic combustion involving a flameless combustion process that uses a solid catalyst to promote the combustion reaction. This presentation discussed relative reactivity testing for volatile organic compounds (VOCs) over commercial catalysts. Several commercial pad catalysts were tested, as well as other powders. The relative reactivity of methane as well as benzene, toluene, ethylbenzene, and xylene (BTEX) were investigated. The purpose of the project was to evaluate combustion of concentrated methane streams that contained BTEX compounds; evaluate catalytic combustion using a counter diffusive radiant heater; develop mathematical models for the reactor to enhance design and understanding; improve the catalyst for BTEX combustion; and target application-dehydrator units. Topics that were addressed in the presentation included methane and benzene conversion; catalytic radiant heaters; small industrial and commercial units; measured temperature distribution; fuel slippage, methane conversion; the effect of water and hydrocarbons; the effect of water-liquid injection; and water addition as vapour. Several observations were offered, including that high percentages of injected liquid water can reduce reactor operating temperature; combustion of BTEX remained highly efficient, however liquid injection could also cause temperature reductions and ultimately the reactor would extinguish; and pre-heating the feed can eliminate the temperature drop and pad wetness problem. It was concluded that BTEX compounds are reactive, and the technology appears promising. 19 figs.

Occurrence of methane in groundwater of south-central New York State, 2012-systematic evaluation of a glaciated region by hydrogeologic setting

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 hydrogeologic setting within a glaciated 1,810-square-mile area of south-central New York along the Pennsylvania border. Sixty-six wells were sampled during the summer of 2012. All wells were at least 1 mile from any known gas well (active, exploratory, or abandoned). Results indicate strong positive and negative associations between hydrogeologic settings and methane occurrence. The hydrogeologic setting classes are based on topographic position (valley and upland), confinement or non-confinement of groundwater by glacial deposits, well completion in fractured bedrock or sand and gravel, and hydrogeologic subcategories. Only domestic wells and similar purposed supply wells with well-construction and log information were selected for classification. 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) of methane. Results of sampling indicate that occurrence of methane in groundwater of the region is common—greater than or equal to 0.001 mg/L in 78 percent of the groundwater samples. Concentrations of methane ranged over five orders of magnitude. Methane concentrations at which monitoring or mitigation are indicated (greater than or equal to 10 mg/L) were measured in 15 percent of the samples. Methane concentrations greater than 0.1 mg/L were associated with specific hydrogeologic settings. Wells completed in bedrock within valleys and under confined groundwater conditions were most closely associated with the highest methane concentrations. Fifty-seven percent of valley wells had greater than or equal to 0.1 mg/L of methane, whereas only 10 percent of upland wells

MethaneSat: Detecting Methane Emissions in the Barnett Shale Region

Science.gov (United States)

Propp, A. M.; Benmergui, J. S.; Turner, A. J.; Wofsy, S. C.

2017-12-01

In this study, we investigate the new information that will be provided by MethaneSat, a proposed satellite that will measure the total column dry-air mole fraction of methane at 1x1 km or 2x2 km spatial resolution with 0.1-0.2% random error. We run an atmospheric model to simulate MethaneSat's ability to characterize methane emissions from the Barnett Shale, a natural gas province in Texas. For comparison, we perform observation system simulation experiments (OSSEs) for MethaneSat, the National Oceanic and Atmospheric administration (NOAA) surface and aircraft network, and Greenhouse Gases Observing Satellite (GOSAT). The results demonstrate the added benefit that MethaneSat would provide in our efforts to monitor and report methane emissions. We find that MethaneSat successfully quantifies total methane emissions in the region, as well as their spatial distribution and steep gradients. Under the same test conditions, both the NOAA network and GOSAT fail to capture this information. Furthermore, we find that the results for MethaneSat depend far less on the prior emission estimate than do those for the other observing systems, demonstrating the benefit of high sampling density. The results suggest that MethaneSat would be an incredibly useful tool for obtaining detailed methane emission information from oil and gas provinces around the world.

Study on radiation degradation of hydroxylamine derivatives. Pt.2: The qualitative and quantitative analysis of light hydrocarbons produced by radiation degradation of N, N-diethyl hydroxylamine

International Nuclear Information System (INIS)

Wang Jinhua; Bao Borong; Wu Minghong; Sun Xilian

2004-01-01

The qualitative and quantitative analysis of light hydrocarbons produced by radiation degradation of N,N-diethyl hydroxylamine are reported. These analyses are performed on the gas chromatography in which a porous layer open tubular column coated with aluminum oxide and a flame-ionization detector are used. When the doses are between 10 and 1000 kGy, the main hydrocarbons produced by radiation degradation of N,N-diethyl hydroxylamine are methane, ethane, ethene, propane and n-butane. The volume fraction of methane, ethane, n-butane and propane are increased with the increase of dose. The volume fraction of ethene is also increased with the increase of dose at first, however, when the absorbed dose is higher than 500 kGy. The volume fraction of ethene is decreased with the increase of dose

Chemical kinetic models for combustion of hydrocarbons and formation of nitric oxide

Science.gov (United States)

Jachimowski, C. J.; Wilson, C. H.

1980-01-01

The formation of nitrogen oxides NOx during combustion of methane, propane, and a jet fuel, JP-4, was investigated in a jet stirred combustor. The results of the experiments were interpreted using reaction models in which the nitric oxide (NO) forming reactions were coupled to the appropriate hydrocarbon combustion reaction mechanisms. Comparison between the experimental data and the model predictions reveals that the CH + N2 reaction process has a significant effect on NO formation especially in stoichiometric and fuel rich mixtures. Reaction models were assembled that predicted nitric oxide levels that were in reasonable agreement with the jet stirred combustor data and with data obtained from a high pressure (5.9 atm (0.6 MPa)), prevaporized, premixed, flame tube type combustor. The results also suggested that the behavior of hydrocarbon mixtures, like JP-4, may not be significantly different from that of pure hydrocarbons. Application of the propane combustion and nitric oxide formation model to the analysis of NOx emission data reported for various aircraft gas turbines showed the contribution of the various nitric oxide forming processes to the total NOx formed.

Thermodynamic analysis of synthetic hydrocarbon fuel production in pressurized solid oxide electrolysis cells

DEFF Research Database (Denmark)

Sun, Xiufu; Chen, Ming; Jensen, Søren Højgaard

2012-01-01

A promising way to store wind and solar electricity is by electrolysis of H2O and CO2 using solid oxide electrolysis cells (SOECs) to produce synthetic hydrocarbon fuels that can be used in existing fuel infrastructure. Pressurized operation decreases the cell internal resistance and enables...... improved system efficiency, potentially lowering the fuel production cost significantly. In this paper, we present a thermodynamic analysis of synthetic methane and dimethyl ether (DME) production using pressurized SOECs, in order to determine feasible operating conditions for producing the desired......, and outlet gas composition. For methane production, low temperature and high pressure operation could improve the system efficiency, but might lead to a higher capital cost. For DME production, high pressure SOEC operation necessitates higher operating temperature in order to avoid carbon formation at higher...

Temporal variations of methane concentration and isotopic composition in groundwater of the St. Lawrence Lowlands, eastern Canada

Science.gov (United States)

Rivard, Christine; Bordeleau, Geneviève; Lavoie, Denis; Lefebvre, René; Malet, Xavier

2018-03-01

Dissolved methane concentrations in shallow groundwater are known to vary both spatially and temporally. The extent of these variations is poorly documented although this knowledge is critical for distinguishing natural fluctuations from anthropogenic impacts stemming from oil and gas activities. This issue was addressed as part of a groundwater research project aiming to assess the risk of shale gas development for groundwater quality over a 500-km2 area in the St. Lawrence Lowlands (Quebec, Canada). A specific study was carried out to define the natural variability of methane concentrations and carbon and hydrogen isotope ratios in groundwater, as dissolved methane is naturally ubiquitous in aquifers of this area. Monitoring was carried out over a period of up to 2.5 years in seven monitoring wells. Results showed that for a given well, using the same sampling depth and technique, methane concentrations can vary over time from 2.5 to 6 times relative to the lowest recorded value. Methane isotopic composition, which is a useful tool to distinguish gas origin, was found to be stable for most wells, but varied significantly over time in the two wells where methane concentrations are the lowest. The use of concentration ratios, as well as isotopic composition of methane and dissolved inorganic carbon (DIC), helped unravel the processes responsible for these variations. This study indicates that both methane concentrations and isotopic composition, as well as DIC isotopes, should be regularly monitored over at least 1 year to establish their potential natural variations prior to hydrocarbon development.

Fluid flow and methane occurrences in the Disko Bugt area offshore West Greenland: indications for gas hydrates?

Science.gov (United States)

Nielsen, Tove; Laier, Troels; Kuijpers, Antoon; Rasmussen, Tine L.; Mikkelsen, Naja E.; Nørgård-Pedersen, Niels

2014-12-01

The present study is the first to directly address the issue of gas hydrates offshore West Greenland, where numerous occurrences of shallow hydrocarbons have been documented in the vicinity of Disko Bugt (Bay). Furthermore, decomposing gas hydrate has been implied to explain seabed features in this climate-sensitive area. The study is based on archive data and new (2011, 2012) shallow seismic and sediment core data. Archive seismic records crossing an elongated depression (20×35 km large, 575 m deep) on the inner shelf west of Disko Bugt (Bay) show a bottom simulating reflector (BSR) within faulted Mesozoic strata, consistent with the occurrence of gas hydrates. Moreover, the more recently acquired shallow seismic data reveal gas/fluid-related features in the overlying sediments, and geochemical data point to methane migration from a deeper-lying petroleum system. By contrast, hydrocarbon signatures within faulted Mesozoic strata below the strait known as the Vaigat can be inferred on archive seismics, but no BSR was visible. New seismic data provide evidence of various gas/fluid-releasing features in the overlying sediments. Flares were detected by the echo-sounder in July 2012, and cores contained ikaite and showed gas-releasing cracks and bubbles, all pointing to ongoing methane seepage in the strait. Observed seabed mounds also sustain gas seepages. For areas where crystalline bedrock is covered only by Pleistocene-Holocene deposits, methane was found only in the Egedesminde Dyb (Trough). There was a strong increase in methane concentration with depth, but no free gas. This is likely due to the formation of gas hydrate and the limited thickness of the sediment infill. Seabed depressions off Ilulissat Isfjord (Icefjord) previously inferred to express ongoing gas release from decomposing gas hydrate show no evidence of gas seepage, and are more likely a result of neo-tectonism.

Hydrocarbon Status of Alluvial Soils in the Istra Morphostructural Node (Moscow Oblast)

Science.gov (United States)

Pikovskiy, Yu. I.; Gennadiev, A. N.; Kovach, R. G.; Khlynina, N. I.; Khlynina, A. V.

2017-12-01

The effect of the current block structure of the earth's crust and its most active sites (morphostructural nodes) on the natural hydrocarbon status of alluvial soils has been considered. Studies have been performed in the Istra district of Moscow oblast within the Istra morphostructural node. The node represents an area of increased geodynamic activity of the earth's crust located at the convergence or intersection of block boundaries: mobile linear zones following large river valleys with alluvial soils. Soil cover mainly consists of alluvial humic-gley soils (Eutric Gleyic Fluvisols) of different depths and alluvial mucky-gley soils (Eutric Gleyic Histic Fluvisols). Some soils manifest stratification. Two factors forming the hydrocarbon status of soils are considered: soil processes and the effect of geodynamic activity, which is manifested within the morphostructural node. The contents of bitumoids and retained methane and butanes in alluvial soils appreciably increase at the entry of river valley into the node. The occurrence frequency of 5-6-ring polycyclic aromatic hydrocarbons (perylene and benzo[ghi]perylene) in mineral horizons increases. It has been concluded that alluvial soils within the Istra morphostructural node are characterized by the biogeochemical type of hydrocarbon status with signs of emanation type at sites with the highest geodynamic activity.

Characterization of Methane Degradation and Methane-Degrading Microbes in Alaska Coastal Water

Energy Technology Data Exchange (ETDEWEB)

Kirchman, David L. [Univ. of Delaware, Lewes, DE (United States)

2012-03-29

The net flux of methane from methane hydrates and other sources to the atmosphere depends on methane degradation as well as methane production and release from geological sources. The goal of this project was to examine methane-degrading archaea and organic carbon oxidizing bacteria in methane-rich and methane-poor sediments of the Beaufort Sea, Alaska. The Beaufort Sea system was sampled as part of a multi-disciplinary expedition (Methane in the Arctic Shelf or MIDAS) in September 2009. Microbial communities were examined by quantitative PCR analyses of 16S rRNA genes and key methane degradation genes (pmoA and mcrA involved in aerobic and anaerobic methane degradation, respectively), tag pyrosequencing of 16S rRNA genes to determine the taxonomic make up of microbes in these sediments, and sequencing of all microbial genes (metagenomes ). The taxonomic and functional make-up of the microbial communities varied with methane concentrations, with some data suggesting higher abundances of potential methane-oxidizing archaea in methane-rich sediments. Sequence analysis of PCR amplicons revealed that most of the mcrA genes were from the ANME-2 group of methane oxidizers. According to metagenomic data, genes involved in methane degradation and other degradation pathways changed with sediment depth along with sulfate and methane concentrations. Most importantly, sulfate reduction genes decreased with depth while the anaerobic methane degradation gene (mcrA) increased along with methane concentrations. The number of potential methane degradation genes (mcrA) was low and inconsistent with other data indicating the large impact of methane on these sediments. The data can be reconciled if a small number of potential methane-oxidizing archaea mediates a large flux of carbon in these sediments. Our study is the first to report metagenomic data from sediments dominated by ANME-2 archaea and is one of the few to examine the entire microbial assemblage potentially involved in

Co-conversion of Ethane and Methanol into Higher Hydrocarbons over Ga/H-ZSM-5, Mo/H-ZSM-5 and Ga-Mo/H-ZSM-5

DEFF Research Database (Denmark)

Mentzel, Uffe Vie; Rovik, Anne; Christensen, Claus H.

2009-01-01

Ethane and methanol are converted simultaneously over Ga/H-ZSM-5, Mo/H-ZSM-5 and Ga-Mo/H-ZSM-5 to produce light olefins and aromatics. The presence of methanol in the reactant stream is intended to facilitate activation of ethane following literature reports on co-conversion of methane and methan...... and in the carbonaceous compounds deposited on the catalysts. This indicates that both reactants take part in the formation of the hydrocarbon pool, which is the origin of all products....

Sources and turnover of organic carbon and methane in fjord and shelf sediments off northern Norway

Science.gov (United States)

Sauer, Simone; Hong, Wei-Li; Knies, Jochen; Lepland, Aivo; Forwick, Matthias; Klug, Martin; Eichinger, Florian; Baranwal, Soma; Crémière, Antoine; Chand, Shyam; Schubert, Carsten J.

2016-10-01

To better understand the present and past carbon cycling and transformation processes in methane-influenced fjord and shelf areas of northern Norway, we compared two sediment cores from the Hola trough and from Ullsfjorden. We investigated (1) the organic matter composition and sedimentological characteristics to study the sources of organic carbon (Corg) and the factors influencing Corg burial, (2) pore water geochemistry to determine the contribution of organoclastic sulfate reduction and methanogenesis to total organic carbon turnover, and (3) the carbon isotopic signature of hydrocarbons to identify the carbon transformation processes and gas sources. High sedimentation and Corg accumulation rates in Ullsfjorden support the notion that fjords are important Corg sinks. The depth of the sulfate-methane-transition (SMT) in the fjord is controlled by the supply of predominantly marine organic matter to the sediment. Organoclastic sulfate reduction accounts for 60% of the total depth-integrated sulfate reduction in the fjord. In spite of the presence of ethane, propane, and butane, we suggest a purely microbial origin of light hydrocarbons in the sediments based on their low δ13C values. In the Hola trough, sedimentation and Corg accumulation rates changed during the deglacial-to-post-glacial transition from approximately 80 cm ka-1 to erosion at present. Thus, Corg burial in this part of the shelf is presently absent. Low organic matter content in the sediment and low rates of organoclastic sulfate reduction (only 3% of total depth-integrated sulfate reduction) entail that the shallow depth of the SMT is controlled mostly by ascending thermogenic methane from deeper sources.

Methane activation on palladium and mercury loaded solid supports

Energy Technology Data Exchange (ETDEWEB)

Kataja, K; Huuska, M; Karinto, K; Maijanen, A; Reinikainen, M; Kiviaho, J; Hase, A [VTT Chemical Technology, Espoo (Finland)

1997-12-31

Methane activation by non-radical method and especially possibilities to heterogenize the homogeneous non-radical system of Periana et al. was studied. Varied loadings of Pd and Hg were ion exchanged to acidic ZSM-5 zeolites with two different Si/A1 ratios. Activation was tested in tubular flow reactor and the outcoming gas was analyzed with quadrupole mass spectrometer. Catalysts, fresh and used, were characterized by XRF and XRD spectroscopies. The methane activation was observed on tested catalysts. However, the activation was concluded to occur mainly through radical reaction and only to some extent by the expected non-radical mechanism. (author) (9 refs.)

Methane activation on palladium and mercury loaded solid supports

Energy Technology Data Exchange (ETDEWEB)

Kataja, K.; Huuska, M.; Karinto, K.; Maijanen, A.; Reinikainen, M.; Kiviaho, J.; Hase, A. [VTT Chemical Technology, Espoo (Finland)

1996-12-31

Methane activation by non-radical method and especially possibilities to heterogenize the homogeneous non-radical system of Periana et al. was studied. Varied loadings of Pd and Hg were ion exchanged to acidic ZSM-5 zeolites with two different Si/A1 ratios. Activation was tested in tubular flow reactor and the outcoming gas was analyzed with quadrupole mass spectrometer. Catalysts, fresh and used, were characterized by XRF and XRD spectroscopies. The methane activation was observed on tested catalysts. However, the activation was concluded to occur mainly through radical reaction and only to some extent by the expected non-radical mechanism. (author) (9 refs.)

Methane oxidation coupled to oxygenic photosynthesis in anoxic waters

Science.gov (United States)

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

2015-01-01

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

Prediction of vapour-liquid and vapour-liquid-liquid equilibria of nitrogen-hydrocarbon mixtures used in J-T refrigerators

Science.gov (United States)

Narayanan, Vineed; Venkatarathnam, G.

2018-03-01

Nitrogen-hydrocarbon mixtures are widely used as refrigerants in J-T refrigerators operating with mixtures, as well as in natural gas liquefiers. The Peng-Robinson equation of state has traditionally been used to simulate the above cryogenic process. Multi parameter Helmholtz energy equations are now preferred for determining the properties of natural gas. They have, however, been used only to predict vapour-liquid equilibria, and not vapour-liquid-liquid equilibria that can occur in mixtures used in cryogenic mixed refrigerant processes. In this paper the vapour-liquid equilibrium of binary mixtures of nitrogen-methane, nitrogen-ethane, nitrogen-propane, nitrogen-isobutane and three component mixtures of nitrogen-methane-ethane and nitrogen-methane-propane have been studied with the Peng-Robinson and the Helmholtz energy equations of state of NIST REFPROP and compared with experimental data available in the literature.

Geology and coal-bed methane resources of the northern San Juan Basin, Colorado and New Mexico

International Nuclear Information System (INIS)

Fassett, J.E.

1988-01-01

This guidebook is the first of its kind: A focused look at coal-bed methane in a large Rocky Mountain Laramide basin. The papers in this volume cover every aspect of coal-bed methane in the San Juan Basin, including: The geology, environments of deposition, and geometry of the coal beds that contain the resource; the origin and migration history of the gas; basin-wide resource estimates; the engineering aspects of getting the gas out of the ground; the marketing and economics of producing coal-bed methane in the San Juan Basin; the legal ownership of the gas; state regulations governing well spacing and field rules; disposal of produced water; and land and mineral ownership patterns in the northern part of the basin. Also included are detailed papers on all of the major coal-bed methane fields in the basin, and in a paper on the history of Fruitland gas production, a discussion of most of the not-so-major fields. A small section of the book deals with geophysical methods, as yet still experimental, for surface detection of underground hydrocarbon resources. Individual papers have been processed separately for inclusion on the data base

Methane Metabolizing Microbial Communities in the Cold Seep Areas in the Northern Continental Shelf of South China Sea

Science.gov (United States)

Wang, F.; Liang, Q.

2016-12-01

Marine sediment contains large amount of methane, estimated approximately 500-2500 gigatonnes of dissolved and hydrated methane carbon stored therein, mainly in continental margins. In localized specific areas named cold seeps, hydrocarbon (mainly methane) containing fluids rise to the seafloor, and support oases of ecosystem composed of various microorganisms and faunal assemblages. South China Sea (SCS) is surrounded by passive continental margins in the west and north and convergent margins in the south and east. Thick organic-rich sediments have accumulated in the SCS since the late Mesozoic, which are continuing sources to form gas hydrates in the sediments of SCS. Here, Microbial ecosystems, particularly those involved in methane transformations were investigated in the cold seep areas (Qiongdongnan, Shenhu, and Dongsha) in the northern continental shelf of SCS. Multiple interdisciplinary analytic tools such as stable isotope probing, geochemical analysis, and molecular ecology, were applied for a comprehensive understanding of the microbe mediated methane transformation in this project. A variety of sediments cores have been collected, the geochemical profiles and the associated microbial distribution along the sediment cores were recorded. The major microbial groups involved in the methane transformation in these sediment cores were revealed, known methane producing and oxidizing archaea including Methanosarcinales, anaerobic methane oxidizing groups ANME-1, ANME-2 and their niche preference in the SCS sediments were found. In-depth comparative analysis revealed the presence of SCS-specific archaeal subtypes which probably reflected the evolution and adaptation of these methane metabolizing microbes to the SCS environmental conditions. Our work represents the first comprehensive analysis of the methane metabolizing microbial communities in the cold seep areas along the northern continental shelf of South China Sea, would provide new insight into the

Hydrocarbon Degradation and Sulfate Reduction in a Coastal Marsh of North Florida

Science.gov (United States)

Hsieh, Y.; Bugna, G. C.; Robinson, L.

2001-05-01

Hydrocarbon contamination of coastal waters has been an environmental concern for sometime. Coastal wetlands, which are rich in organic matter and microbial activities, have been considered natural systems that could degrade hydrocarbon in contaminated coastal waters. This study was initiated to investigate the potential of hydrocarbon degradation in a coastal salt marsh of North Florida with special reference to sulfate reduction. Freshly collected surface marsh sediments (0-20 cm) were incubated in a laboratory at ambient temperature (23.2° C) with the treatments of: 1) Control (i.e., no treatment), 2) +(crude) oil, 3) +NO3-1+oil, and 4) +MoO4-2+oil. Carbon dioxide evolution from the incubation was collected and analyzed for the total amount and the 13C signature. The NO3-1 and MoO4-2 treatments were intended to block the sulfate reduction activity. The results show that the indigenous organic matter and the crude oil have distinct δ 13C values of -19.8 and -27.6 \\permil, respectively, relative to PDB. Evolved CO2 concentrations and δ 13C values also indicate that microbial populations can adapt to the presence of anthropogenic hydrocarbons. Blocking of sulfate reducers by MoO4-2 addition started to reduce the carbon dioxide evolution rates after a 4-d incubation. After a 48-d incubation, the carbon dioxide evolution of the MoO4-2-treated samples was reduced to only 23 % of the non-MoO4-2-treated samples, indicating the increased significant role of sulfate reducers in digesting older soil organic matter and the hydrocarbons. T-tests also indicated that in NO3-1 treatment, δ 13C values significantly depleted (p=0.1) while CO2 concentration remained relatively constant. These indicate that while denitrifiers played a role in the degradation, the microbial population is predominantly composed of sulfate reducers. Salt marshes would be a much more significant source of CH4 if SO4-2 is suppressed. All MoO4-2-treated samples produced significant amount of methane

Options for cost-effectively reducing atmospheric methane concentrations from anthropogenic biomass sources

International Nuclear Information System (INIS)

Roos, K.F.; Jacobs, C.; Orlic, M.

1993-01-01

Methane is a major greenhouse gas, second only to carbon dioxide in its contribution to future global warming. Methane concentrations have more than doubled over the last two centuries and continue to rise annually. These increases are largely correlated with increasing human populations. Methane emissions from human related activities currently account for about 70 percent of annual emissions. Of these human related emissions, biomass sources account for about 75 percent and non-biomass sources about 25 percent. Because methane has a shorter lifetime than other major greenhouse gases, efforts to reduce methane emissions may fairly quickly be translated into lower atmospheric concentrations of methane and lower levels of radiative forcing. This fairly quick response would have the benefit of slowing the rate of climate change and hence allow natural ecosystems more time to adapt. Importantly, methane may be cost-effectively reduced from a number of biomass and non-biomass sources in the United States and worldwide. Methane is a valuable fuel, not just a waste by-product, and often systems may be reconfigured to reap the fuel value of the methane and more than justify the necessary expenditures. Such options for reducing methane emission from biomass sources exist for landfills, livestock manures, and ruminant livestock, and have been implemented to varying degrees in countries around the world. However, there are a number of barriers that hinder the more widespread use of technologies, including institutional, financial, regulatory, informational, and other barriers. This paper describes an array of available options that may be cost-effectively implemented to reduce methane emissions from biomass sources. This paper also discusses a number of programs that have been developed in the United States and internationally to promote the implementation of these methane reduction options and overcome existing barriers

Methane Recycling During Burial of Methane Hydrate-Bearing Sediments

Science.gov (United States)

You, K.; Flemings, P. B.

2017-12-01

We quantitatively investigate the integral processes of methane hydrate formation from local microbial methane generation, burial of methane hydrate with sedimentation, and methane recycling at the base of the hydrate stability zone (BHSZ) with a multiphase multicomponent numerical model. Methane recycling happens in cycles, and there is not a steady state. Each cycle starts with free gas accumulation from hydrate dissociation below the BHSZ. This free gas flows upward under buoyancy, elevates the hydrate saturation and capillary entry pressure at the BHSZ, and this prevents more free gas flowing in. Later as this layer with elevated hydrate saturation is buried and dissociated, the large amount of free gas newly released and accumulated below rapidly intrudes into the hydrate stability zone, drives rapid hydrate formation and creates three-phase (gas, liquid and hydrate) equilibrium above the BHSZ. The gas front retreats to below the BHSZ until all the free gas is depleted. The shallowest depth that the free gas reaches in one cycle moves toward seafloor as more and more methane is accumulated to the BHSZ with time. More methane is stored above the BHSZ in the form of concentrated hydrate in sediments with relatively uniform pore throat, and/or with greater compressibility. It is more difficult to initiate methane recycling in passive continental margins where the sedimentation rate is low, and in sediments with low organic matter content and/or methanogenesis reaction rate. The presence of a permeable layer can store methane for significant periods of time without recycling. In a 2D system where the seafloor dips rapidly, the updip gas flow along the BHSZ transports more methane toward topographic highs where methane gas and elevated hydrate saturation intrude deeper into the hydrate stability zone within one cycle. This could lead to intermittent gas venting at seafloor at the topographic highs. This study provides insights on many phenomenon associated with

Methane emissions from MBT landfills

Energy Technology Data Exchange (ETDEWEB)

Heyer, K.-U., E-mail: heyer@ifas-hamburg.de; Hupe, K.; Stegmann, R.

2013-09-15

Highlights: • Compilation of methane generation potential of mechanical biological treated (MBT) municipal solid waste. • Impacts and kinetics of landfill gas production of MBT landfills, approach with differentiated half-lives. • Methane oxidation in the waste itself and in soil covers. • Estimation of methane emissions from MBT landfills in Germany. - Abstract: Within the scope of an investigation for the German Federal Environment Agency (“Umweltbundesamt”), the basics for the estimation of the methane emissions from the landfilling of mechanically and biologically treated waste (MBT) were developed. For this purpose, topical research including monitoring results regarding the gas balance at MBT landfills was evaluated. For waste treated to the required German standards, a methane formation potential of approximately 18–24 m{sup 3} CH{sub 4}/t of total dry solids may be expected. Monitoring results from MBT landfills show that a three-phase model with differentiated half-lives describes the degradation kinetics in the best way. This is due to the fact that during the first years of disposal, the anaerobic degradation processes still proceed relatively intensively. In addition in the long term (decades), a residual gas production at a low level is still to be expected. Most of the soils used in recultivation layer systems at German landfills show a relatively high methane oxidation capacity up to 5 l CH{sub 4}/(m{sup 2} h). However, measurements at MBT disposal sites indicate that the majority of the landfill gas (in particular at non-covered areas), leaves the landfill body via preferred gas emission zones (hot spots) without significant methane oxidation. Therefore, rather low methane oxidation factors are recommended for open and temporarily covered MBT landfills. Higher methane oxidation rates can be achieved when the soil/recultivation layer is adequately designed and operated. Based on the elaborated default values, the First Order Decay (FOD

Light Hydrocarbons Adsorption Mechanisms in Two Calcium-based Microporous Metal Organic Frameworks

KAUST Repository

Plonka, Anna M.

2016-01-25

The adsorption mechanism of ethane, ethylene and acetylene (C2Hn; n=2, 4, 6) on two microporous metal organic frameworks (MOFs) is described here that is consistent with observations from single crystal and powder X-ray diffraction, calorimetric measurments and gas adsorption isotherm measurements. Two calcium-based MOFs, designated as SBMOF-1 and SBMOF-2 (SB: Stony Brook), form three-dimensional frameworks with one-dimensional open channels. As determined form single crystal diffraction experiments channel geometries of both SBMOF-1 and SBMOF-2 provide multiple adsorption sites for hydrocarbon molecules trough C-H…π and C-H…O interactions, similarly to interactions in the molecular and protein crystals. Both materials selectively adsorb C2 hydrocarbon gases over methane as determined with IAST and breakthrough calculations, with C2H6/CH4 selectivity as high as 74 in SBMOF-1.

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

gases. However, in most cases only ethane has been detected and the remaining less than 15 samples demonstrate an uncommon ratio of ethane to propane compared to typical thermogenic hydrocarbons. These data do not suggest a migration of deeper sourced gases, but a thermogenic source cannot be excluded entirely for some samples. However, ethane and propane can also be generated by microbial processes and might therefore represent ubiquitous background groundwater abundances of these gases. Nevertheless, our data suggest that due to the exceedingly low concentration of ethane and propane, respective concentration changes might prove to be a more sensitive parameter than methane to detect possible migration of deeper sourced (thermally generated) hydrocarbons into a groundwater aquifer. - Highlights: • Baseline concentration of CH 4 , C 2 H 6 & C 3 H 8 in 1000 groundwater wells were determined. • Dissolved methane concentrations cover a range of ∼7 orders of magnitude. • Ethane and propane have been detected in a subset of our samples. • Mean δ 13 C of methane is −70‰ vs PDB with a large variation between −110‰ and +20‰.

Absolute fragmentation cross sections in atom-molecule collisions : Scaling laws for non-statistical fragmentation of polycyclic aromatic hydrocarbon molecules

NARCIS (Netherlands)

Chen, T.; Gatchell, M.; Stockett, M. H.; Alexander, J. D.; Zhang, Y.; Rousseau, P.; Domaracka, A.; Maclot, S.; Delaunay, R.; Adoui, L.; Huber, B. A.; Schlathölter, T.; Schmidt, H. T.; Cederquist, H.; Zettergren, H.

2014-01-01

We present scaling laws for absolute cross sections for non-statistical fragmentation in collisions between Polycyclic Aromatic Hydrocarbons (PAH/PAH+) and hydrogen or helium atoms with kinetic energies ranging from 50 eV to 10 keV. Further, we calculate the total fragmentation cross sections

40 CFR 86.094-3 - Abbreviations.

Science.gov (United States)

2010-07-01

..., and for 1985 and Later Model Year New Gasoline Fueled, Natural Gas-Fueled, Liquefied Petroleum Gas... of this part, and have the following meanings: ALVW—Adjusted Loaded Vehicle Weight LPG—Liquefied Petroleum Gas NMHC—Nonmethane Hydrocarbons NMHCE—Non-Methane Hydrocarbon Equivalent PM—Particulate Matter...

Generalized hypothesis of the origin of the living-matter simplest elements, transformation of the Archean atmosphere, and the formation of methane-hydrate deposits

International Nuclear Information System (INIS)

Ostrovskii, Viktor E; Kadyshevich, Elena A

2007-01-01

The original hydrate hypothesis of the origin of living-matter simplest elements (LMSEs), i.e., the 'Life Origination Hydrate hypothesis,' abbreviated as the LOH hypothesis, is discussed. It includes notions of the interdependence and interconditionality of processes leading to the life origin, to the transformation of the primary atmosphere, and to the underground methane-hydrate formation. Saturation of the young earth's crust with nebular hydrogen is taken into consideration for the first time. The origin of LMSEs is regarded as a result of regular and thermodynamically caused inevitable chemical transformations and of the universal physical and chemical laws. According to the LOH hypothesis, LMSEs originated repeatedly and, maybe, are now originating from methane (or other simple hydrocarbons), niter, and phosphate within boundary layers of the solid phases of the hydrates of the simplest hydrocarbons. It is assumed that the phenomenon of monochirality of nucleic acids is caused by geometric features of the structure matrix. (reviews of topical problems)

Generalized hypothesis of the origin of the living-matter simplest elements, transformation of the Archean atmosphere, and the formation of methane-hydrate deposits

Energy Technology Data Exchange (ETDEWEB)

Ostrovskii, Viktor E [L. Ya. Karpov Institute of Physical Chemistry, Moscow (Russian Federation); Kadyshevich, Elena A [A.M. Obukhov Institute of Atmospheric Physics, Russian Academy of Sciences, Moscow (Russian Federation)

2007-02-28

The original hydrate hypothesis of the origin of living-matter simplest elements (LMSEs), i.e., the 'Life Origination Hydrate hypothesis,' abbreviated as the LOH hypothesis, is discussed. It includes notions of the interdependence and interconditionality of processes leading to the life origin, to the transformation of the primary atmosphere, and to the underground methane-hydrate formation. Saturation of the young earth's crust with nebular hydrogen is taken into consideration for the first time. The origin of LMSEs is regarded as a result of regular and thermodynamically caused inevitable chemical transformations and of the universal physical and chemical laws. According to the LOH hypothesis, LMSEs originated repeatedly and, maybe, are now originating from methane (or other simple hydrocarbons), niter, and phosphate within boundary layers of the solid phases of the hydrates of the simplest hydrocarbons. It is assumed that the phenomenon of monochirality of nucleic acids is caused by geometric features of the structure matrix. (reviews of topical problems)

Corrosion resistance of magnesium treated by hydrocarbon plasma immersion ion implantation

International Nuclear Information System (INIS)

Yekehtaz, M.; Baba, K.; Hatada, R.; Flege, S.; Sittner, F.; Ensinger, W.

2009-01-01

Due to its low weight, magnesium is increasingly being used as construction materials for e.g. automobile bodies or cell phone housings. However, the material suffers from poor tribological features and particularly from poor corrosion resistance. In order to protect magnesium from corrosion, it was treated by hydrocarbon plasma immersion ion implantation. Magnesium samples were implanted with methane and acetylene at different process times at ambient temperature. Electrochemical corrosion measurements in dilute buffered acetic acid showed that the treatment led to well-adhering films with an effective corrosion protection.

Corrosion resistance of magnesium treated by hydrocarbon plasma immersion ion implantation

Energy Technology Data Exchange (ETDEWEB)

Yekehtaz, M. [Technische Universitaet Darmstadt, Department of Materials Science, Petersenstr. 23, 64287 Darmstadt (Germany)], E-mail: Yekehtaz@ca.tu-darmstadt.de; Baba, K. [Nagasaki Center of Industrial Technology, 2-1303-8 Ikeda, Omura, Nagasaki 856-0026 (Japan); Hatada, R. [Technische Universitaet Darmstadt, Department of Materials Science, Petersenstr. 23, 64287 Darmstadt (Germany); Nagasaki Center of Industrial Technology, 2-1303-8 Ikeda, Omura, Nagasaki 856-0026 (Japan); Flege, S.; Sittner, F.; Ensinger, W. [Technische Universitaet Darmstadt, Department of Materials Science, Petersenstr. 23, 64287 Darmstadt (Germany)

2009-05-01

Due to its low weight, magnesium is increasingly being used as construction materials for e.g. automobile bodies or cell phone housings. However, the material suffers from poor tribological features and particularly from poor corrosion resistance. In order to protect magnesium from corrosion, it was treated by hydrocarbon plasma immersion ion implantation. Magnesium samples were implanted with methane and acetylene at different process times at ambient temperature. Electrochemical corrosion measurements in dilute buffered acetic acid showed that the treatment led to well-adhering films with an effective corrosion protection.

Hydrogen--deuterium exchange in saturated hydrocarbons on α-chromia catalyst

International Nuclear Information System (INIS)

Kalman, J.; Guczi, L.

1977-01-01

The kinetics of hydrogen--deuterium exchange in methane, ethane, and propane have been studied with unsupported α-chromia as catalyst in the temperature range of 598 to 688 0 K. The apparent activation energies for methane, ethane, and propane are 88, 130, and 84 kJ mol -1 , respectively, similar to those found on chromia gel. The order of reaction with respect to hydrocarbons and deuterium has been determined as also having the kinetic isotope effect. The main initial products are CH 3 D and CD 4 with methane, C 2 H 4 D 2 and C 2 D 6 with ethane, and C 3 H 7 D and C 3 D 8 with propane. A change in product distribution as a function of temperature, conversion, aging, and oxygen--deuterium treatment has been observed. In agreement with the kinetic data and the effect of oxygen, Cr 3+ has been assumed as the active species of the chromia catalyst, whereas Cr 2+ is an inactive site on the surface. There is no direct proof that chromium ion in a valence state higher than 3+ plays an important role in the exchange reaction. It was established that dual Cr 3+ -- Cr 3+ sites are responsible for the formation of ethane-d 2 . After a long deuterium treatment the number of dual sites is decreased, the effect being revealed in the decreased rate of exchange and the small amount of ethane-d 2 . On the contrary, the formation of methane-d 4 is interpreted by the formation of Cr = C bonds by analogy with homogeneous complexes. In the case of propane, the exchange reaction can be adequately interpreted by a π-allyl mechanism

A kinetically blocked 1,14:11,12-dibenzopentacene: A persistent triplet diradical of a non-Kekulé polycyclic benzenoid hydrocarbon

KAUST Repository

Li, Yuan; Huang, Kuo-Wei; Sun, Zhe; Webster, Richard D.; Zeng, Zebing; Zeng, Wangdong; Chi, Chunyan; Furukawa, Ko; Wu, Jishan

2014-01-01

The synthesis of high-spin polycyclic hydrocarbons is very challenging due to their extremely high reactivity. Herein, we report the synthesis and characterization of a kinetically blocked 1,14:11,12-dibenzopentacene, DP-Mes, which represents a rare persistent triplet diradical of a non-Kekulé polycyclic benzenoid hydrocarbon. In contrast to its structural isomer 1,14:7,8-dibenzopentacene (heptazethrene) with a singlet biradical ground state, DP-Mes is a triplet diradical as confirmed by ESR and ESTN measurements and density functional theory calculations. DP-Mes also displays intermolecular antiferromagnetic spin interactions in solution at low temperature. © 2014 the Partner Organisations.

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

Science.gov (United States)

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

2002-01-01

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

Soil Iodine Determination in Deccan Syneclise, India: Implications for Near Surface Geochemical Hydrocarbon Prospecting

International Nuclear Information System (INIS)

Mani, Devleena; Kumar, T. Satish; Rasheed, M. A.; Patil, D. J.; Dayal, A. M.; Rao, T. Gnaneshwar; Balaram, V.

2011-01-01

The association of iodine with organic matter in sedimentary basins is well documented. High iodine concentration in soils overlying oil and gas fields and areas with hydrocarbon microseepage has been observed and used as a geochemical exploratory tool for hydrocarbons in a few studies. In this study, we measure iodine concentration in soil samples collected from parts of Deccan Syneclise in the west central India to investigate its potential application as a geochemical indicator for hydrocarbons. The Deccan Syneclise consists of rifted depositional sites with Gondwana–Mesozoic sediments up to 3.5 km concealed under the Deccan Traps and is considered prospective for hydrocarbons. The concentration of iodine in soil samples is determined using ICP-MS and the values range between 1.1 and 19.3 ppm. High iodine values are characteristic of the northern part of the sampled region. The total organic carbon (TOC) content of the soil samples range between 0.1 and 1.3%. The TOC correlates poorly with the soil iodine (r 2 < 1), indicating a lack of association of iodine with the surficial organic matter and the possibility of interaction between the seeping hydrocarbons and soil iodine. Further, the distribution pattern of iodine compares well with two surface geochemical indicators: the adsorbed light gaseous hydrocarbons (methane through butane) and the propane-oxidizing bacterial populations in the soil. The integration of geochemical observations show the occurrence of elevated values in the northern part of the study area, which is also coincident with the presence of exposed dyke swarms that probably serve as conduits for hydrocarbon microseepage. The corroboration of iodine with existing geological, geophysical, and geochemical data suggests its efficacy as one of the potential tool in surface geochemical exploration of hydrocarbons. Our study supports Deccan Syneclise to be promising in terms of its hydrocarbon prospects.

Physics of coal methane: decisive role of iron compounds

Energy Technology Data Exchange (ETDEWEB)

Gavriljuk, V. G., E-mail: gavr@imp.kiev.ua; Skoblik, A. P. [G.V. Kurdyumov Institute for Metal Physics (Ukraine); Shanina, B. D.; Konchits, A. A. [V. Ye. Lashkarev Institute for Semiconductor Physics (Ukraine)

2016-12-15

The role of iron in formation of the coal methane is clarified based on the studies performed on the coal samples taken from different mines in Donetsk coal basin. Using Mössbauer spectroscopy, a correlation is found between the iron content and methane capacity of coal seams. By means of electron paramagnetic resonance, it is found that iron increases the concentration of non-compensated electron spins, i.e. dangled bonds at the carbon atoms. These bonds can be occupied by hydrogen atoms as a prerequisite of methane formation. The two-valence iron is shown to be the most effective in the increase of spin concentration. By using the ion mass spectrometry, the modelling of methane formation is carried out on the mechanical mixture of the iron-free reactor graphite, iron compounds and diluted sulphuric acid as a source of hydrogen atoms. The proposed mechanism is also confirmed by methane formation in the mixture of iron compounds and the coal from the mine where the iron and methane are practically absent.

Thermocatalytic CO2-Free Production of Hydrogen from Hydrocarbon Fuels

Energy Technology Data Exchange (ETDEWEB)

University of Central Florida

2004-01-30

The main objective of this project is the development of an economically viable thermocatalytic process for production of hydrogen and carbon from natural gas or other hydrocarbon fuels with minimal environmental impact. The three major technical goals of this project are: (1) to accomplish efficient production of hydrogen and carbon via sustainable catalytic decomposition of methane or other hydrocarbons using inexpensive and durable carbon catalysts, (2) to obviate the concurrent production of CO/CO{sub 2} byproducts and drastically reduce CO{sub 2} emissions from the process, and (3) to produce valuable carbon products in order to reduce the cost of hydrogen production The important feature of the process is that the reaction is catalyzed by carbon particulates produced in the process, so no external catalyst is required (except for the start-up operation). This results in the following advantages: (1) no CO/CO{sub 2} byproducts are generated during hydrocarbon decomposition stage, (2) no expensive catalysts are used in the process, (3) several valuable forms of carbon can be produced in the process depending on the process conditions (e.g., turbostratic carbon, pyrolytic graphite, spherical carbon particles, carbon filaments etc.), and (4) CO{sub 2} emissions could be drastically reduced (compared to conventional processes).

Methane cycling. Nonequilibrium clumped isotope signals in microbial methane.

Science.gov (United States)

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

2015-04-24

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

Reconsideration of methane isotope signature as a criterion for the genesis of natural gas: influence of migration on isotopic signatures

International Nuclear Information System (INIS)

Pernaton, E.; Prinzhofer, A.; Schneider, F.

1996-01-01

Experiments were performed in the purpose of studying the isotopic consequences of the diffusional transport of hydrocarbon gases through sediment rocks. Linked to a numerical model, these gas diffusion experiments through as shale porous plug allowed us to correlate porosity and diffusivity of the migration medium. Significant isotopic fractionations (carbon and hydrogen) of methane, and ethane at a lesser degree were observed. This is in contradiction with the actual dogma of isotope geochemistry of natural gases which claims that no fractionation occurs during gas migration. The genetic characterization of natural gases by using the isotopic signature of methane appears as an ambiguous method. (author)

Mobile geophysics for searching and exploration of Domanic hydrocarbon deposits

Science.gov (United States)

Borovsky, M. Ya; Uspensky, B. V.; Valeeva, S. E.; Borisov, A. S.

2018-05-01

There are noted features of shale hydrocarbons occurrence. It is shown the role of geophysical prospecting in the geological prospecting process for non-traditional sources of hydrocarbon. There are considered the possibilities of non-seismic methods for forecasting, prospecting, exploration and preparation of Domanikovian hydrocarbons accumulations for exploration. It is emphasized the need for geophysical studies of tectonic disturbances. Modern aerogeophysical instrumentation and methodological support allows to combine high-precision magneto-prospecting with gravimetric and gamma spectrometry. This combination of geophysical methods contributes to the diagnosis of active and latent faults.

Significance of dissolved methane in effluents of anaerobically ...

Science.gov (United States)

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

Origin and mobility of hydrocarbon gases in alkaline plutons : the example of the Khibina complex, NW Russia

Energy Technology Data Exchange (ETDEWEB)

Treloar, P.J.; Beeskow, B.; Rankin, A.H. [Kingston Univ., Kingston upon Thames (United Kingdom). School of Earth Sciences; Potter, J. [Western Ontario Univ., London, ON (Canada). Dept. of Earth Science; Nivin, V. [Geological Inst., Apatity (Russian Federation). Kola Science Centre

2006-07-01

The origin and distribution of abiogenic hydrocarbon gases (HCGs) was discussed with particular reference to HCGs in the Khibina pluton which are dominated by methane (CH{sub 4}) with minor amounts of higher hydrocarbons and hydrogen (H{sub 2}). Although isotopic data and hydrocarbon species ratios point to an abiogenic source, they do not distinguish between primary magmatic hydrocarbons and those generated by late magmatic re-speciation or post-magmatic Fischer-Tropsch (FT) synthesis. Some rock textures suggest limited CH{sub 4} production by FT synthesis, but the presence of primary, syn-magmatic CH{sub 4}-rich fluid inclusions, and the absence of primary and secondary carbon dioxide (CO{sub 2}) rich inclusions, suggest a dominantly early magmatic origin for the HCGs. The permeability and porosity in the Khibina pluton can be constrained by the distribution and geometry of fluid inclusion planes (FIPs) and open cracks (OCs), as well as by the magnitude and pathways of fluid flow. Orientation data for FIPs and OCs, obtained from oriented thin sections, revealed a range of orientations in sub-parallel arrays, suggesting continual re-activation of old fracture systems. The extensive occurrence of OCs and sealed FIPs points to long lived porosities and permeabilities with large fluid fluxes integrated over time. FIP and OC density values were found to be consistent with gas release patterns characterized by spontaneous release during mining of large volumes of HCG stored in a network of interconnected, sealed microfractures and fluid inclusion planes that unzip during stress. It was determined that the HCGs have a primary magmatic origin although there is local evidence for limited post-magmatic FT synthesis. Long term continuous gas migration has occurred within the complex through an interconnected set of fractures. FIPs represent aliquots of gas sealed during open system migration. It was concluded that the complex contains a potentially economically viable

Two-stage Catalytic Reduction of NOx with Hydrocarbons

Energy Technology Data Exchange (ETDEWEB)

Umit S. Ozkan; Erik M. Holmgreen; Matthew M. Yung; Jonathan Halter; Joel Hiltner

2005-12-21

A two-stage system for the catalytic reduction of NO from lean-burn natural gas reciprocating engine exhaust is investigated. Each of the two stages uses a distinct catalyst. The first stage is oxidation of NO to NO{sub 2} and the second stage is reduction of NO{sub 2} to N{sub 2} with a hydrocarbon. The central idea is that since NO{sub 2} is a more easily reduced species than NO, it should be better able to compete with oxygen for the combustion reaction of hydrocarbon, which is a challenge in lean conditions. Early work focused on demonstrating that the N{sub 2} yield obtained when NO{sub 2} was reduced was greater than when NO was reduced. NO{sub 2} reduction catalysts were designed and silver supported on alumina (Ag/Al{sub 2}O{sub 3}) was found to be quite active, able to achieve 95% N{sub 2} yield in 10% O{sub 2} using propane as the reducing agent. The design of a catalyst for NO oxidation was also investigated, and a Co/TiO{sub 2} catalyst prepared by sol-gel was shown to have high activity for the reaction, able to reach equilibrium conversion of 80% at 300 C at GHSV of 50,000h{sup -1}. After it was shown that NO{sub 2} could be more easily reduced to N{sub 2} than NO, the focus shifted on developing a catalyst that could use methane as the reducing agent. The Ag/Al{sub 2}O{sub 3} catalyst was tested and found to be inactive for NOx reduction with methane. Through iterative catalyst design, a palladium-based catalyst on a sulfated-zirconia support (Pd/SZ) was synthesized and shown to be able to selectively reduce NO{sub 2} in lean conditions using methane. Development of catalysts for the oxidation reaction also continued and higher activity, as well as stability in 10% water, was observed on a Co/ZrO{sub 2} catalyst, which reached equilibrium conversion of 94% at 250 C at the same GHSV. The Co/ZrO{sub 2} catalyst was also found to be extremely active for oxidation of CO, ethane, and propane, which could potential eliminate the need for any separate

Microbiology and geochemistry of hydrocarbon-rich sediments erupted from the deep geothermal Lusi site, Indonesia

Science.gov (United States)

Krüger, Martin; Straten, Nontje; Mazzini, Adriano; Scheeder, Georg; Blumenberg, Martin

2016-04-01

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 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 offshore microbial colonies that commonly thrive at offshore methane and oil seeps and mud volcanoes, however very little has been done for 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 heavier liquid hydrocarbons originating from one or more km below the surface. While the source of the methane at Lusi is clear (Mazzini et al., 2012), the origin of the seeping oil, either form the deep mature Eocene Ngimbang (type II kerogen) or from the less mature Pleistocene Upper Kalibeng Fm. (type III kerogen), is still discussed. In the framework of the Lusi Lab project (ERC grant n° 308126) we analysed an oil film and found that carbon preference indices among n-alkanes, sterane and hopane isomers (C29-steranes: 20S/(20S+20R) and α,β-C32 Hopanes (S/(S+R), respectively) are indicative of a low thermal maturity of the oil source rock (~0.5 to 0.6 % vitrinite reflectance equivalents = early oil window maturity). Furthermore, sterane distributions, the pristane to phytane ratio and a relatively high oleanane index, which is an indication of an angiosperm input, demonstrate a strong terrestrial component in the organic matter. Together, hydrocarbons suggest that the source of the oil film is predominantly terrestrial organic matter. Both, source and maturity estimates from biomarkers, are in favor of a type III organic matter source and are therefore suggestive of a mostly Pleistocene Upper Kalibeng Fm. origin. We also conducted a sampling campaign at the Lusi site collecting samples of fresh mud close to the erupting crater

Mid-IR Absorption Cross-Section Measurements of Hydrocarbons

KAUST Repository

Alrefae, Majed Abdullah

2013-05-01

Laser diagnostics are fast-response, non-intrusive and species-specific tools perfectly applicable for studying combustion processes. Quantitative measurements of species concentration and temperature require spectroscopic data to be well-known at combustion-relevant conditions. Absorption cross-section is an important spectroscopic quantity and has direct relation to the species concentration. In this work, the absorption cross-sections of basic hydrocarbons are measured using Fourier Transform Infrared (FTIR) spectrometer, tunable Difference Frequency Generation laser and fixed wavelength helium-neon laser. The studied species are methane, methanol, acetylene, ethylene, ethane, ethanol, propylene, propane, 1-butene, n-butane, n-pentane, n-hexane, and n-heptane. The Fourier Transform Infrared (FTIR) spectrometer is used for the measurements of the absorption cross-sections and the integrated band intensities of the 13 hydrocarbons. The spectral region of the spectra is 2800 – 3400 cm-1 (2.9 – 3.6 μm) and the temperature range is 673 – 1100 K. These valuable data provide huge opportunities to select interference-free wavelengths for measuring time-histories of a specific species in a shock tube or other combustion systems. Such measurements can allow developing/improving chemical kinetics mechanisms by experimentally determining reaction rates. The Difference Frequency Generation (DFG) laser is a narrow line-width, tunable laser in the 3.35 – 3.53 μm wavelength region which contains strong absorption features for most hydrocarbons due to the fundamental C-H vibrating stretch. The absorption cross-sections of propylene are measured at seven different wavelengths using the DFG laser. The temperature range is 296 – 460 K which is reached using a Reflex Cell. The DFG laser is very attractive for kinetic studies in the shock tube because of its fast time response and the potential possibility of making species-specific measurements. The Fixed wavelength

Methane activation using Kr and Xe in a dielectric barrier discharge reactor

International Nuclear Information System (INIS)

Jo, Sungkwon; Lee, Dae Hoon; Kim, Kwan-Tae; Kang, Woo Seok; Song, Young-Hoon

2014-01-01

Methane has interested many researchers as a possible new energy source, but the high stability of methane causes a bottleneck in methane activation, limiting its practical utilization. To determine how to effectively activate methane using non-thermal plasma, the conversion of methane is measured in a planar-type dielectric barrier discharge reactor using three different noble gases—Ar, Kr, and Xe—as additives. In addition to the methane conversion results at various applied voltages, the discharge characteristics such as electron temperature and electron density were calculated through zero-dimensional calculations. Moreover, the threshold energies of excitation and ionization were used to distinguish the dominant particle for activating methane between electrons, excited atoms, and ionized atoms. From the experiments and calculations, the selection of the additive noble gas is found to affect not only the conversion of methane but also the selectivity of product gases even under similar electron temperature and electron density conditions

Baseline Geochemistry of Natural Occurring Methane and Saline Groundwater in an Area of Unconventional Shale Gas Development Through Time

Science.gov (United States)

Harkness, J.; Darrah, T.; Warner, N. R.; Whyte, C. J.; Moore, M. T.; Millot, R.; Kloppmann, W.; Jackson, R. B.; Vengosh, A.

2017-12-01

Naturally occurring methane is nearly ubiquitous in most sedimentary basins and delineating the effects of anthropogenic contamination sources from geogenic sources is a major challenge for evaluating the impact of unconventional shale gas development on water quality. This study employs a broadly integrated study of various geochemical techniques to investigate the geochemical variations of groundwater and surface water before, during, and after hydraulic fracturing.This approache combines inorganic geochemistry (major cations and anions), stable isotopes of select inorganic constituents including strontium (87Sr/86Sr), boron (δ11B), lithium (δ7Li), and carbon (δ13C-DIC), select hydrocarbon molecular (methane, ethane, propane, butane, and pentane) and isotopic tracers (δ13C-CH4, δ13C-C2H6), tritium (3H), and noble gas elemental and isotopic composition (He, Ne, Ar) to apportion natural and anthropogenic sources of natural gas and salt contaminants both before and after drilling. Methane above 1 ccSTP/L in groundwater samples awas strongly associated with elevated salinity (chloride >50 mg/L).The geochemical and isotopic analysis indicate saline groundwater originated via naturally occurring processes, presumably from the migration of deeper methane-rich brines that have interacted extensively with coal lithologies. The chemistry and gas compostion of both saline and fresh groundwater wells did not change following the installation of nearby shale-gas wells.The results of this study emphasize the value of baseline characterization of water quality in areas of fossil fuel exploration. Overall this study presents a comprehensive geochemical framework that can be used as a template for assessing the sources of elevated hydrocarbons and salts to water resources in areas potentially impacted by oil and gas development.

Heritability for enteric methane emission from Danish Holstein cows using a non-invasive FTIR method

DEFF Research Database (Denmark)

Lassen, Jan; Løvendahl, Peter

2013-01-01

Enteric methane emission from ruminants contributes substantially to the greenhouse effect. Few studies have focused on the genetic variation in enteric methane emission from dairy cattle. One reason for that is the limited number of methods appropriate for large scale phenotyping to measure...

Phytoremediation of hydrocarbon-contaminated soil using plants adapted to western Canadian climate

International Nuclear Information System (INIS)

Robson, D.B.

2003-01-01

Phytoremediation relies on the use of plants for in-situ treatment of hydrocarbon contaminated soils. It is based on relationships between plants, microorganisms and the environment. The advantages of the process are its low cost and minimal soil disturbance. Phytoremediation has not been widely implemented in Canada because only a few native or non-native plant species have been tested for hydrocarbon tolerance or degradation ability. More studies are needed to fully understand why some plants are more tolerant of hydrocarbons than others, and whether tolerant species increase hydrocarbon degradation. In this study, several field and growth chamber experiments were conducted to examine hydrocarbon tolerance in plants. Hydrocarbon contaminated field plots had higher soil pH, carbon to nitrogen ratio and bare ground, lower total nitrogen, available phosphorous and litter cover. The mean diversity at the uncontaminated sites was 0.52. It was 0.45 at the contaminated sites. Mean species similarity between contaminated and uncontaminated sites was 31.1 per cent and cover similarity was 22.2 per cent. The common plants in the contaminated field included kochia, wild barley, salt grass, bluegrass, and wheatgrass. The plants that formed most plant cover on contaminated plots were non-mycorrhizal, self-pollinating, and large seeded. The species with the highest survival after 5 weeks in hydrocarbon contaminated soils included one native and 4 non-native grasses, 2 native and 3 non-native legumes and 2 native forbs. All plants (with the exception of Indian breadroot) grown in hydrocarbon contaminated potting soil had lower total biomass and lower growth rates compared to the control

Phytoremediation of hydrocarbon-contaminated soil using plants adapted to western Canadian climate

Energy Technology Data Exchange (ETDEWEB)

Robson, D.B.

2003-07-01

Phytoremediation relies on the use of plants for in-situ treatment of hydrocarbon contaminated soils. It is based on relationships between plants, microorganisms and the environment. The advantages of the process are its low cost and minimal soil disturbance. Phytoremediation has not been widely implemented in Canada because only a few native or non-native plant species have been tested for hydrocarbon tolerance or degradation ability. More studies are needed to fully understand why some plants are more tolerant of hydrocarbons than others, and whether tolerant species increase hydrocarbon degradation. In this study, several field and growth chamber experiments were conducted to examine hydrocarbon tolerance in plants. Hydrocarbon contaminated field plots had higher soil pH, carbon to nitrogen ratio and bare ground, lower total nitrogen, available phosphorous and litter cover. The mean diversity at the uncontaminated sites was 0.52. It was 0.45 at the contaminated sites. Mean species similarity between contaminated and uncontaminated sites was 31.1 per cent and cover similarity was 22.2 per cent. The common plants in the contaminated field included kochia, wild barley, salt grass, bluegrass, and wheatgrass. The plants that formed most plant cover on contaminated plots were non-mycorrhizal, self-pollinating, and large seeded. The species with the highest survival after 5 weeks in hydrocarbon contaminated soils included one native and 4 non-native grasses, 2 native and 3 non-native legumes and 2 native forbs. All plants (with the exception of Indian breadroot) grown in hydrocarbon contaminated potting soil had lower total biomass and lower growth rates compared to the control.

High-temperature measurements of methane and acetylene using quantum cascade laser absorption near 8 μm

International Nuclear Information System (INIS)

Sajid, M.B.; Javed, T.; Farooq, A.

2015-01-01

The mid-infrared wavelength region near 8 μm 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 ν 4 band of methane and the ν 4 +ν 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. - Highlights: • Methane measured at the peak of Q(12) transition in the ν 4 band. • Acetylene measured at the peak of P(23) transition in the ν 4 +ν 5 band. • Differential absorption strategy employed to eliminate broadband interference absorption. • Absorption cross-sections measured over 1200–2200 K and 1–4 atm. • Methane and acetylene time-histories measured during the pyrolysis of n-pentane

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

Science.gov (United States)

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

2015-04-01

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

Methane sources in gas hydrate-bearing cold seeps: Evidence from radiocarbon and stable isotopes

Science.gov (United States)

Pohlman, J.W.; Bauer, J.E.; Canuel, E.A.; Grabowski, K.S.; Knies, D.L.; Mitchell, C.S.; Whiticar, Michael J.; Coffin, R.B.

2009-01-01

Fossil methane from the large and dynamic marine gas hydrate reservoir has the potential to influence oceanic and atmospheric carbon pools. However, natural radiocarbon (14C) measurements of gas hydrate methane have been extremely limited, and their use as a source and process indicator has not yet been systematically established. In this study, gas hydrate-bound and dissolved methane recovered from six geologically and geographically distinct high-gas-flux cold seeps was found to be 98 to 100% fossil based on its 14C content. Given this prevalence of fossil methane and the small contribution of gas hydrate (??? 1%) to the present-day atmospheric methane flux, non-fossil contributions of gas hydrate methane to the atmosphere are not likely to be quantitatively significant. This conclusion is consistent with contemporary atmospheric methane budget calculations. In combination with ??13C- and ??D-methane measurements, we also determine the extent to which the low, but detectable, amounts of 14C (~ 1-2% modern carbon, pMC) in methane from two cold seeps might reflect in situ production from near-seafloor sediment organic carbon (SOC). A 14C mass balance approach using fossil methane and 14C-enriched SOC suggests that as much as 8 to 29% of hydrate-associated methane carbon may originate from SOC contained within the upper 6??m of sediment. These findings validate the assumption of a predominantly fossil carbon source for marine gas hydrate, but also indicate that structural gas hydrate from at least certain cold seeps contains a component of methane produced during decomposition of non-fossil organic matter in near-surface sediment.

Light-Dependent Aerobic Methane Oxidation Reduces Methane Emissions from Seasonally Stratified Lakes

Science.gov (United States)

Oswald, Kirsten; Milucka, Jana; Brand, Andreas; Littmann, Sten; Wehrli, Bernhard; Kuypers, Marcel M. M.; Schubert, Carsten J.

2015-01-01

Lakes are a natural source of methane to the atmosphere and contribute significantly to total emissions compared to the oceans. Controls on methane emissions from lake surfaces, particularly biotic processes within anoxic hypolimnia, are only partially understood. Here we investigated biological methane oxidation in the water column of the seasonally stratified Lake Rotsee. A zone of methane oxidation extending from the oxic/anoxic interface into anoxic waters was identified by chemical profiling of oxygen, methane and δ13C of methane. Incubation experiments with 13C-methane yielded highest oxidation rates within the oxycline, and comparable rates were measured in anoxic waters. Despite predominantly anoxic conditions within the zone of methane oxidation, known groups of anaerobic methanotrophic archaea were conspicuously absent. Instead, aerobic gammaproteobacterial methanotrophs were identified as the active methane oxidizers. In addition, continuous oxidation and maximum rates always occurred under light conditions. These findings, along with the detection of chlorophyll a, suggest that aerobic methane oxidation is tightly coupled to light-dependent photosynthetic oxygen production both at the oxycline and in the anoxic bottom layer. It is likely that this interaction between oxygenic phototrophs and aerobic methanotrophs represents a widespread mechanism by which methane is oxidized in lake water, thus diminishing its release into the atmosphere. PMID:26193458

Synergistic methane formation on pyrolytic graphite due to combined H+ ion and H0 atom impact

International Nuclear Information System (INIS)

Haasz, A.A.; Davis, J.W.; Auciello, O.; Strangeby, P.C.; Vietzke, E.; Flaskamp, K.; Philipps, V.

1986-06-01

Exposure of graphite to multispecies hydrogenic impact, as is the case in tokamaks, could lead to synergistic mechanisms resulting in an enhancement of methane formation, and consequently in increased carbon erosion. We present results obtained in controlled experiments in our laboratories in Toronto and Juelich for the synergistic methane production due to combined sub-eV H 0 atoms and energetic H + ion impact on pyrolytic graphite. Flux densities were 10 14 -2x10 16 H 0 /cm 2 s for the sub-eV H 0 atoms and 6x10 12 -5x10 15 H + /cm 2 for H + ions of 300 eV to 2.5 keV energy. Synergistic factors (defined as the ratio of methane formation rate due to combined H 0 and H + fluxes to the sum of the formation rates due to separate species impact) ranged from about 1.5-15 for the experimental parameters used. In addition, a spectrum of formed hydrocarbons in the synergistic reaction of H + and H 0 on graphite is presented

Non-covalent Interactions of Graphene with Polycyclic Aromatic Hydrocarbons

NARCIS (Netherlands)

Zygouri, Panagiota; Potsi, Georgia; Mouzourakis, Eleftherios; Spyrou, Konstantinos; Gournis, Dimitrios; Rudolf, Petra

2015-01-01

In this mini review we discuss the interactions of polyaromatic hydrocarbons (PAHs) with graphene and the experimental approaches developed so far to create novel graphene/PAH hybrids and composite systems. The utilization of these systems in electrical, biomedical and polymer-reinforcement

Ozone Production and Control Strategies for Southern Taiwan

Science.gov (United States)

Shiu, C.; Liu, S.; Chang, C.; Chen, J.; Chou, C. C.; Lin, C.

2006-12-01

An observation-based modeling (OBM) approach is used to estimate the ozone production efficiency and production rate of O3 (P(O3)) in southern Taiwan. The approach can also provide an indirect estimate of the concentration of OH. Measured concentrations of two aromatic hydrocarbons, i.e. ethylbenzene/m,p-xylene, are used to estimate the degree of photochemical processing and the amounts of photochemically consumed NOx and NMHCs. In addition, a one-dimensional (1d) photochemical model is used to compare with the OBM results. The average ozone production efficiency during the field campaign in Kaohsiung-Pingtung area in Fall 2003 is found to be about 5, comparable to previous works. The relationship of P(O3) with NOx is examined in detail and compared to previous studies. The derived OH concentrations from this approach are in fair agreement with values calculated from the 1d photochemical model. The relationship of total oxidants (e.g. O3+NO2) versus initial NOx and NMHCs suggests that reducing NMHCs are more effective in controlling total oxidants than reducing NOx. For O3 control, reducing NMHC is even more effective than NOx due to the NO titration effect. This observation-based approach provides a good alternative for understanding the production of ozone and formulating ozone control strategy in urban and suburban environment without measurements of peroxy radicals.

Methane in the Northern West Siberian Basin. Generation, dynamics of the reservoirs and exchange with the atmosphere

International Nuclear Information System (INIS)

Cramer, B.

1997-07-01

Based on compositional data and isotope geochemistry natural gas in northern West Siberia can be divided into three groups. These are: natural gas in Jurassic rocks, natural gas in Neocomian rocks and natural gas from the Aptian to Cenomanian Pokur Formation. Natural gas in Jurassic rocks was generated thermogenically from rocks of the Jurassic Tyumen Formation. Natural gas in Neocomian rocks is also of thermogenic origin, possibly being generated from the organic matter of Lower Cretaceous sediments. The largest accumulation of natural gas occurs in sandstone reservoirs in the Pokur Formation. This gas can be described as a mixture between thermogenic gas from deeper strata and isotopically light almost pure methane. 98.6% of this gas consists of methane with an unusual isotope signature of -51.2 permille. It is not possible to explain the existence of this methane with established concepts of gas generation. A new model was developed to examine the possibility of a thermogenic origin of the isotopically light methane in early mature rocks of the Pokur Formation. Based on pyrolysis experiments and reaction kinetic calculations the model enables the simulation of stable carbon isotope ratios of hydrocarbon components in natural gas. The temperature dependent kinetic isotope fractionation is defined by a difference in the activation energies of 12 C-and 13 C-methane generation. The application of the new method to two coaly sandstones of the Pokur Formation results in a good correspondence between modelled carbon isotope ratios of δ 13 C values of methane in the reservoirs. The mass of methane thermogenically generated within the Pokur Formation under the gas field structures, however, is not sufficient to explain the mass of accumulated methane. (orig./SR) [de

Biogenic methane leakage on the Aquitaine Shelf: fluid system characterization from source to emission

Science.gov (United States)

Michel, Guillaume; Dupré, Stéphanie; Baltzer, Agnès; Imbert, Patrice; Ehrhold, Axel; Battani, Anne; Deville, Eric

2017-04-01

The recent discovery of biogenic methane emissions associated with methane-derived authigenic carbonate mounds along the Aquitaine Shelf edge offshore SW France (140 to 220 m water depth) questions about the initiation and temporal evolution of this fluid system (80 km N-S and 8 km E-W). Based on a multi-data study (including multibeam echosounder, subbottom profiler, single channel sparker seismic, 80 traces air gun seismic data and well cuttings and logs), different scenarii are proposed for the organic matter source levels and migration pathways of the methane. Several evidence of the presence of gas are observed on seismic data and interpreted to be linked to the biogenic system. Single channel sparker seismic lines exhibit an acoustic blanking (between 75-100 ms TWT below seafloor and the first multiple) below the present-day seepage area and westwards up to 8 km beyond the shelf-break. An air gun seismic line exhibits chaotic reflections along 8 km below the seepage area from the seabed down to 700 ms TWT below seafloor. Based on 1) the local geothermal gradient about 26 °C/km and 2) the window for microbial methanogenesis ranging from 4 to 56 °C, the estimation of the bottom limit for biogenic generation window is about 1.5 km below seafloor. Cuttings from 3 wells of the area within the methanogenesis window show average TOC (Total Organic Carbon) of 0.5 %; however, one well shows some coal levels with 30-35 % TOC in the Oligocene between 1490 and 1540 m below seafloor. Geochemical analysis on crushed cuttings evidenced heavy hydrocarbons up to mid-Paleogene, while shallower series did not evidence any. In the first scenario, we propose that methane is sourced from the Neogene prograding system. The 0.5% average TOC is sufficient to generate a large volume of methane over the thickness of this interval (up to 1 km at the shelf break area). In the second scenario, methane would be sourced from the Oligocene coals; however their spatial extension with regard

Kinetics of Hydrocarbon formation in a-C:H Film deposition plasmas

International Nuclear Information System (INIS)

Cal, E. de la; Tabares, F. L.

1993-01-01

The formation of C2 and Cp hydrocarbons during the PACVD of a-C:H films from admixtures of methane with H2 and He has been investigated by mass spectrometry under several deposition condition. The time evolution of the observed species indicates that the formation mechanisms of ethylene and acetylene are sensitive to the conditions of the wall during the growing of the film. Acetylene are sensitive to the conditions of the wall during the growing of the film. Acetylene formation was found to be directly related to the formation of the film on top of the carburized metal. (Author) 12 refs

Kinetics of Hydrocarbon formation in a- C:H Film deposition plasmas

Energy Technology Data Exchange (ETDEWEB)

Cal, E de la; Tabares, F L

1993-07-01

The formation of C2 and Cp hydrocarbons during the PACVD of a-C:H films from admixtures of methane with H2 and He has been investigated by mass spectrometry under several deposition condition. The time evolution of the observed species indicates that the formation mechanisms of ethylene and acetylene are sensitive to the conditions of the wall during the growing of the film. Acetylene are sensitive to the conditions of the wall during the growing of the film. Acetylene formation was found to be directly related to the formation of the film on top of the carburized metal. (Author) 12 refs.

Isotope reversals in hydrocarbon gases of natural shale systems and well head production data

Energy Technology Data Exchange (ETDEWEB)

Berner, U.; Schloemer, S.; Stiller, E. [Bundesanstalt fuer Geowissenschaften und Rohstoffe (BGR), Hannover (Germany); Marquardt, D. [Rijksuniversiteit Utrecht (Netherlands)

2013-08-01

Relationships between gas geochemical signatures and the thermal maturity of source rocks containing aquatic organic matter are based on on pyrolysis experiments and have been successfully used in conventional hydrocarbon exploration since long. We demonstrate how these models can be applied to the evaluation of unconventional shale resources. For this purpose hydrocarbon gases have been extracted from low and high mature source rocks (type II kerogens) using laboratory desorption techniques. We determined the molecular composition of the gases as well as the carbon isotope ratios of methane to propane. In the extracted gases we observe an increase of {sup 13}C content in methane with increasing dry gas ratio (C1/{Sigma}C1-6). The carbon isotope ratios of ethane and propane initially increase with increasing dryness but start to become isotopically lighter above a dry gas ratio of 0.8. We show that oil-to-gas cracking explains the observed gas geochemical data, and that mixing between gases from different processes is a key factor to describe natural hydrocarbon systems of shales. However, data from published case studies using well head gases which show 'isotope roll-over' effects indicate that the isotopic reversal observed in well head samples deviate from those observed in natural shale systems in a fundamental way. We show that isotope reversals related to well head gases are best explained by an additional isotope fractionation effect induced through hydraulic fracturing and gas migration from the shale to the well head. Although, this induced isotope fractionation is an artifact which obscures isotopic information of natural systems to a large extend, we suggest a simple classification scheme which allows distinguishing between hot and cool spot areas using well head or mud line gas data. (orig.)

Oxidative coupling of methane over alkali-promoted simple molybdate catalysts

International Nuclear Information System (INIS)

Discoll, S.A.; Zhang, L.; Ozkan, U.S.

1992-01-01

The study of various metal oxides and alkali promoted metal oxide catalysts has received much interest in recent years after the earlier reports of ethylene synthesis through oxidative coupling of methane, and of achieving high selectivities over a Li/MgO catalyst under methane and oxygen cofeed conditions. The addition of promoter ions to several oxide catalysts has been studied to determine the effect of the promoter ion on catalytic activity and selectivity. The authors' work has focused on the use of alkali promoters for a simple molybdate catalyst. MnMoO 4 . A study of Na, Li, K, Mg, Ba, Mn, Co, Fe, Cu, Zn, and Ni molybdates by Kiwi et al showed that with the exception of NiMoO 4 , the molybdates were stable for long periods of time under reaction conditions for oxidative coupling. At a conversion level of about 60%, selectivities ranged from 9.8% to 16.6%. The MnMoO 4 and K 2 MnMoO 4 molybdates were the least selective catalysts. Another molybdate, PbMoO 4 , was studied by Baerns et al., with 19% selectivity to C 2 hydrocarbons at 1% conversion. An 11.4% conversion to form aldehyde was also reported. In this paper the authors report the characterization and catalytic behavior of MnMoO 4 catalysts promoted with either Li, Na, or K in oxidative coupling of methane

Source analysis of peroxyacetyl nitrate (PAN) in Guangzhou, China: a yearlong observation study

Science.gov (United States)

Wang, B. G.; Zhu, D.; Zou, Y.; Wang, H.; Zhou, L.; Ouyang, X.; Shao, H. F.; Deng, X. J.

2015-06-01

In recent years, photochemical smog has been a major cause of air pollution in the metropolitan area of Guangzhou, China, with a continuing increase in the concentrations of photochemical pollutants. The concentration of peroxyacetyl nitrate (PAN) has often been found to reach very high levels, posing a potential threat to the public health. To better understand the changes in PAN concentration and its sources, a study was carried from January to December of 2012 at the Guangzhou Panyu Atmospheric Composition Station (GPACS) to measure the atmospheric concentrations of PAN as well as those of ozone (O3), nitrogen oxides (NOx), and non-methane hydrocarbon (NMHC). These data were analyzed to investigate the quantitative relationships between PAN and its precursors. In the study period, the hourly concentrations of PAN varied from below instrument detection limit to 12.0 ppbv. The yearly mean concentration of PAN was 0.84 ppbv, with the daily mean concentration exceeding 5 ppbv in 32 of the total observation days. Calculations indicate that among the measured NMHC species, alkenes accounted for 53 % of the total NMHC contribution to the PAN production, with aromatics and alkanes accounting for about 11 and 7 % of the total, respectively. During the period of our observation only a modest correlation was found between the concentrations of PAN and O3 for daytime hours, and observed PAN concentrations were relatively high even though the observed NMHCs/NOx ratio was low. This suggests regional air mass transport of pollutants had a major impact on the PAN concentrations in Guangzhou area.

File: non conventional hydrocarbons - Between concerns and opportunities

International Nuclear Information System (INIS)

Deflandre, Jean-Pierre; Heidmann, Jean-Claude; Vially, Roland; Duflot, Sylvie; Lions, Renaud; Speirs, Julie; Bauquis, Pierre-Rene; Brunelle, Nathalie

2015-01-01

A first article proposes an overview of gas and oil resources with respect to their geological context. The authors address the origins of hydrocarbons, their underground migration and possible trapping, thus scanning the whole spectrum of conventional and non conventional resources. A second article, signed by representatives of companies working on shale gas in Europe as well as in the USA, examines whether the development of shale gases, if it ever emerges in Europe, will be the same as it is in the USA. They notably outline differences regarding several legal aspects on land property and on the environment. Based on a study on shale supply chain which identified costs, needed skills, existing capabilities, and recommendations for closing identified gaps, the third article discusses the perspective and opportunity of a possible development of shale gas in the UK. The fourth article discusses the impacts of the exploitation of source rock oils and gases on the American and World economies, and the fifth one discusses the perspectives for the petrochemicals and refining industries in a context of development of shale gases and oils in the USA, of an over-capacity situation for the refining industry, of decline of the European oil product market, and of competition with new polymer production capacities (notably in the Middle East where ethane extracted from natural gas is available in large quantities and at very low prices)

Methane production and methane consumption: a review of processes underlying wetland methane fluxes.

NARCIS (Netherlands)

Segers, R.

1998-01-01

Potential rates of both methane production and methane consumption vary over three orders of magnitude and their distribution is skew. These rates are weakly correlated with ecosystem type, incubation temperature, in situ aeration, latitude, depth and distance to oxic/anoxic interface. Anaerobic

New materials for methane capture from dilute and medium-concentration sources

Energy Technology Data Exchange (ETDEWEB)

Kim, J; Maiti, A; Lin, LC; Stolaroff, JK; Smit, B; Aines, RD

2013-04-16

Methane (CH4) is an important greenhouse gas, second only to CO2, and is emitted into the atmosphere at different concentrations from a variety of sources. However, unlike CO2, which has a quadrupole moment and can be captured both physically and chemically in a variety of solvents and porous solids, methane is completely non-polar and interacts very weakly with most materials. Thus, methane capture poses a challenge that can only be addressed through extensive material screening and ingenious molecular-level designs. Here we report systematic in silico studies on the methane capture effectiveness of two different materials systems, that is, liquid solvents (including ionic liquids) and nanoporous zeolites. Although none of the liquid solvents appears effective as methane sorbents, systematic screening of over 87,000 zeolite structures led to the discovery of a handful of candidates that have sufficient methane sorption capacity as well as appropriate CH4/CO2 and/or CH4/N-2 selectivity to be technologically promising.

Effects of non-thermal plasmas and electric field on hydrocarbon/air flames

Science.gov (United States)

Ganguly, Biswa

2009-10-01

Need to improve fuel efficiency, and reduce emission from hydrocarbon combustor in automotive and gas turbine engines have reinvigorated interest in reducing combustion instability of a lean flame. The heat generation rate in a binary reaction is HQ =N^2 c1c2 Q exp(-E/RT), where N is the density, c1 and c2 are mol fractions of the reactants, Q is the reaction heat release, E is the activation energy, R is the gas constant and T is the average temperature. For hydrocarbon-air reactions, the typical value of E/R ˜20, so most heat release reactions are confined to a thin reaction sheet at T >=1400 K. The lean flame burning condition is susceptible to combustion instability due to a critical balance between heat generation and heat loss rates, especially at high gas flow rate. Radical injection can increase flame speed by reducing the hydrocarbon oxidation reaction activation barrier and it can improve flame stability. Advances in nonequilibrium plasma generation at high pressure have prompted its application for energy efficient radical production to enhance hydrocarbon-air combustion. Dielectric barrier discharges and short pulse excited corona discharges have been used to enhance combustion stability. Direct electron impact dissociation of hydrocarbon and O2 produces radicals with lower fuel oxidation reaction activation barriers, initiating heat release reaction CnHm+O CnHm-1+ OH (and other similar sets of reactions with partially dissociated fuel) below the typical cross-over temperature. Also, N2 (A) produced in air discharge at a moderate E/n can dissociate O2 leading to oxidation of fuel at lower gas temperature. Low activation energy reactions are also possible by dissociation of hydrocarbon CnHm+e -> CnHm-2+H2+e, where a chain propagation reaction H2+ O OH+H can be initiated at lower gas temperature than possible under thermal equilibrium kinetics. Most of heat release comes from the reaction CO+OH-> CO2 +H, nonthermal OH production seem to improve

Reducing Open Cell Landfill Methane Emissions with a Bioactive Alternative Daily

Energy Technology Data Exchange (ETDEWEB)

Helene Hilger; James Oliver; Jean Bogner; David Jones

2009-03-31

made but prone to rapid desiccation. Bacterial adsorption onto foam padding, natural sponge, and geotextile was successful. The most important factor for success appeared to be water holding capacity. Prototype biotarps made with geotextiles plus adsorbed methane oxidizing bacteria were tested for their responses to temperature, intermittent starvation, and washing (to simulate rainfall). The prototypes were mesophilic, and methane oxidation activity remained strong after one cycle of starvation but then declined with repeated cycles. Many of the cells detached with vigorous washing, but at least 30% appeared resistant to sloughing. While laboratory landfill simulations showed that four-layer composite biotarps made with two different types of geotextile could remove up to 50% of influent methane introduced at a flux rate of 22 g m{sup -2} d{sup -1}, field experiments did not yield high activity levels. Tests revealed that there were high hour-to-hour flux variations in the field, which, together with frequent rainfall events, confounded the field testing. Overall, the findings suggest that a methanotroph embedded biotarp appears to be a feasible strategy to mitigate methane emission from landfill cells, although the performance of field-tested biotarps was not robust here. Tarps will likely be best suited for spring and summer use, although the methane oxidizer population may be able to shift and adapt to lower temperatures. The starvation cycling of the tarp may require the capacity for intermittent reinoculation of the cells, although it is also possible that a subpopulation will adapt to the cycling and become dominant. Rainfall is not expected to be a major factor, because a baseline biofilm will be present to repopulate the tarp. If strong performance can be achieved and documented, the biotarp concept could be extended to include interception of other compounds beyond methane, such as volatile aromatic hydrocarbons and chlorinated solvents.

Volatilisation of aromatic hydrocarbons from soil

DEFF Research Database (Denmark)

Lindhardt, B.; Christensen, T.H.

1996-01-01

The non-steady-state fluxes of aromatic hydrocarbons were measured in the laboratory from the surface of soils contaminated with coal tar Four soil samples from a former gasworks site were used for the experiments. The fluxes were quantified for 11 selected compounds, 4 mono- and 7 polycyclic...... aromatic hydrocarbons, for a period of up to 8 or 16 days. The concentrations of the selected compounds in the soils were between 0.2 and 3,100 mu g/g. The study included the experimental determination of the distribution coefficient of the aromatic hydrocarbons between the sorbed phase and the water under...... saturated conditions. The determined distribution coefficients showed that the aromatic hydrocarbons were more strongly sorbed to the total organic carbon including the coal tar pitch - by a factor of 8 to 25 - than expected for natural organic matter. The fluxes were also estimated using an analytical...

A new equation of correction of the specific volume of the hydrocarbons C1 to C8 liquids for the equation of state of Peng-Robinson

International Nuclear Information System (INIS)

Hoyos Madrigal, Bibian

2000-01-01

A new generalized correction equation for specific volume of hydrocarbon pure liquids is proposed. Which can be used in a wide temperature range and that do not require additional parameters for each substance. The equation was developed for the normal hydrocarbon series from methane to octane and the obtained results applied to other substances are analysed. A comparison is also made with the equation proposed by Peneloux et al. (1982) resulting. In all cases, in a better performance of the equation proposed in this work

Pumping of hydrocarbons using non-evaporable getters

International Nuclear Information System (INIS)

Emerson, L.C.; Knize, R.J.; Cecchi, J.L.

1986-01-01

Pumping speed measurements have been obtained for a number of gaseous hydrocarbons including members of the alkene, alkadiene, and cycloalkane groups as a function of temperature using a Zr-Al alloy getter. Pumping speeds were obtained by analysis of an exponential least squares fit to the pressure decay curve following introduction of each gas. It was found that these pumping speeds are relatively high (up to 400 1/s) and exhibit, with only a few exceptions, little temperature dependence. This is in contrast to the earlier reported results for the alkane series

Measurements of atmospheric hydrocarbons and biogenic emission fluxes in the Amazon boundary layer

Science.gov (United States)

Zimmerman, P. R.; Greenberg, J. P.; Westberg, C. E.

1988-01-01

Tropospheric mixing ratios of methane, C2-C10 hydrocarbons, and carbon monoxide were measured over the Amazon tropical forest near Manaus, Amazonas, Brazil, in July and August 1985. The measurements, consisting mostly of altitude profiles of these gases, were all made within the atmospheric boundary layer up to an altitude of 1000 m above ground level. Data characterize the diurnal hydrocarbon composition of the boundary layer. Biogenic emissions of isoprene control hydroxyl radical concentrations over the forest. Biogenic emission fluxes of isoprene and terpenes are estimated to be 25,000 micrograms/sq m per day and 5600 micrograms/sq m per day, respectively. This isoprene emission is equivalent to 2 percent of the net primary productivity of the tropical forest. Atmospheric oxidation of biogenic isoprene and terpenes emissions from the Amazon forest may account for daily increases of 8-13 ppb for carbon monoxide in the planetary boundary layer.

Performance of an auto refrigerant cascade refrigerator operating in gas refrigerant supply (GRS) mode with nitrogen-hydrocarbon and argon-hydrocarbon refrigerants

Science.gov (United States)

Gurudath Nayak, H.; Venkatarathnam, G.

2009-07-01

There is a worldwide interest in the development of auto refrigerant cascade (ARC) refrigerators operating with refrigerant mixtures. Both flammable and non-flammable refrigerant mixtures can be used in these systems. The performance of an ARC system with optimum nitrogen-hydrocarbon and argon-hydrocarbon mixtures between 90 and 160 K is presented in this paper.

77 FR 11039 - Proposed Confidentiality Determinations for the Petroleum and Natural Gas Systems Source Category...

Science.gov (United States)

2012-02-24

... liquids (NGLs) or non-methane gases from produced natural gas, or the separation of NGLs into one or more... than or reveal the composition of the hydrocarbon equal to 10 barrels per liquid or the reporter's... composition of the hydrocarbon equal to 10 barrels per liquid or the reporter's productivity. Data on day...

Coal-packed methane biofilter for mitigation of green house gas emissions from coal mine ventilation air.

Science.gov (United States)

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

2014-01-01

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

Effect of hydrogen on hydrogen-methane turbulent non-premixed flame under MILD condition

Energy Technology Data Exchange (ETDEWEB)

Mardani, Amir; Tabejamaat, Sadegh [Department of Aerospace engineering, Amirkabir university of technology (Tehran polytechnic), Hafez Ave., PO. Box: 15875-4413, Tehran (Iran)

2010-10-15

Energy crises and the preservation of the global environment are placed man in a dilemma. To deal with these problems, finding new sources of fuel and developing efficient and environmentally friendly energy utilization technologies are essential. Hydrogen containing fuels and combustion under condition of the moderate or intense low-oxygen dilution (MILD) are good choices to replace the traditional ones. In this numerical study, the turbulent non-premixed CH{sub 4}+H{sub 2} jet flame issuing into a hot and diluted co-flow air is considered to emulate the combustion of hydrogen containing fuels under MILD conditions. This flame is related to the experimental condition of Dally et al. [Proc. Combust. Inst. 29 (2002) 1147-1154]. In general, the modelling is carried out using the EDC model, to describe turbulence-chemistry interaction, and the DRM-22 reduced mechanism and the GRI2.11 full mechanism to represent the chemical reactions of H{sub 2}/methane jet flame. The effect of hydrogen content of fuel on flame structure for two co-flow oxygen levels is studied by considering three fuel mixtures, 5%H{sub 2}+95%CH{sub 4}, 10%H{sub 2}+90%CH{sub 4} and 20% H{sub 2}+80%CH{sub 4}(by mass). In this study, distribution of species concentrations, mixture fraction, strain rate, flame entrainment, turbulent kinetic energy decay and temperature are investigated. Results show that the hydrogen addition to methane leads to improve mixing, increase in turbulent kinetic energy decay along the flame axis, increase in flame entrainment, higher reaction intensities and increase in mixture ignitability and rate of heat release. (author)

Multiparametric methane sensor for environmental monitoring

Science.gov (United States)

Borecki, M.; Duk, M.; Kociubiński, A.; Korwin-Pawlowski, M. L.

2016-12-01

Today, methane sensors find applications mostly in safety alarm installations, gas parameters detection and air pollution classification. Such sensors and sensors elements exists for industry and home use. Under development area of methane sensors application is dedicated to ground gases monitoring. Proper monitoring of soil gases requires reliable and maintenance-free semi-constant and longtime examination at relatively low cost of equipment. The sensors for soil monitoring have to work on soil probe. Therefore, sensor is exposed to environment conditions, as a wide range of temperatures and a full scale of humidity changes, as well as rain, snow and wind, that are not specified for classical methane sensors. Development of such sensor is presented in this paper. The presented sensor construction consists of five commercial non dispersive infra-red (NDIR) methane sensing units, a set of temperature and humidity sensing units, a gas chamber equipped with a micro-fan, automated gas valves and also a microcontroller that controls the measuring procedure. The electronics part of sensor was installed into customized 3D printed housing equipped with self-developed gas valves. The main development of proposed sensor is on the side of experimental evaluation of construction reliability and results of data processing included safety procedures and function for hardware error correction. Redundant methane sensor units are used providing measurement error correction as well as improved measurement accuracy. The humidity and temperature sensors are used for internal compensation of methane measurements as well as for cutting-off the sensor from the environment when the conditions exceed allowable parameters. Results obtained during environment sensing prove that the gas concentration readings are not sensitive to gas chamber vertical or horizontal position. It is important as vertical sensor installation on soil probe is simpler that horizontal one. Data acquired during six

Atmospheric methane removal by methane-oxidizing bacteria immobilized on porous building materials.

Science.gov (United States)

Ganendra, Giovanni; De Muynck, Willem; Ho, Adrian; Hoefman, Sven; De Vos, Paul; Boeckx, Pascal; Boon, Nico

2014-04-01

Biological treatment using methane-oxidizing bacteria (MOB) immobilized on six porous carrier materials have been used to mitigate methane emission. Experiments were performed with different MOB inoculated in building materials at high (~20 % (v/v)) and low (~100 ppmv) methane mixing ratios. Methylocystis parvus in autoclaved aerated concrete (AAC) exhibited the highest methane removal rate at high (28.5 ± 3.8 μg CH₄ g⁻¹ building material h⁻¹) and low (1.7 ± 0.4 μg CH₄ g⁻¹ building material h⁻¹) methane mixing ratio. Due to the higher volume of pores with diameter >5 μm compared to other materials tested, AAC was able to adsorb more bacteria which might explain for the higher methane removal observed. The total methane and carbon dioxide-carbon in the headspace was decreased for 65.2 ± 10.9 % when M. parvus in Ytong was incubated for 100 h. This study showed that immobilized MOB on building materials could be used to remove methane from the air and also act as carbon sink.

Rain increases methane production and methane oxidation in a boreal thermokarst bog

Science.gov (United States)

Neumann, R. B.; Moorberg, C.; Turner, J.; Wong, A.; Waldrop, M. P.; Euskirchen, E. S.; Edgar, C.; Turetsky, M. R.

2017-12-01

Bottom-up biogeochemical models of wetland methane emissions simulate the response of methane production, oxidation and transport to wetland conditions and environmental forcings. One reason for mismatches between bottom-up and top-down estimates of emissions is incomplete knowledge of factors and processes that control microbial rates and methane transport. To advance mechanistic understanding of wetland methane emissions, we conducted a multi-year field investigation and plant manipulation experiment in a thermokarst bog located near Fairbanks, Alaska. The edge of the bog is experiencing active permafrost thaw, while the center of the bog thawed 50 to 100 years ago. Our study, which captured both an average year and two of the wettest years on record, revealed how rain interacts with vascular vegetation and recently thawed permafrost to affect methane emissions. In the floating bog, rain water warmed and oxygenated the subsurface, but did not alter soil saturation. The warmer peat temperatures increased both microbial methane production and plant productivity at the edge of the bog near the actively thawing margin, but minimally altered microbial and plant activity in the center of the bog. These responses indicate processes at the edge of the bog were temperature limited while those in the center were not. The compounding effect of increased microbial activity and plant productivity at the edge of the bog doubled methane emissions from treatments with vascular vegetation during rainy years. In contrast, methane emissions from vegetated treatments in the center of the bog did not change with rain. The oxygenating influence of rain facilitated greater methane oxidation in treatments without vascular vegetation, which offset warming-induced increases in methane production at the edge of the bog and decreased methane emissions in the center of the bog. These results elucidate the complex and spatially variable response of methane production and oxidation in

Novel techniques for characterization of hydrocarbon emission sources in the Barnett Shale

Science.gov (United States)

Nathan, Brian Joseph

Changes in ambient atmospheric hydrocarbon concentrations can have both short-term and long-term effects on the atmosphere and on human health. Thus, accurate characterization of emissions sources is critically important. The recent boom in shale gas production has led to an increase in hydrocarbon emissions from associated processes, though the exact extent is uncertain. As an original quantification technique, a model airplane equipped with a specially-designed, open-path methane sensor was flown multiple times over a natural gas compressor station in the Barnett Shale in October 2013. A linear optimization was introduced to a standard Gaussian plume model in an effort to determine the most probable emission rate coming from the station. This is shown to be a suitable approach given an ideal source with a single, central plume. Separately, an analysis was performed to characterize the nonmethane hydrocarbons in the Barnett during the same period. Starting with ambient hourly concentration measurements of forty-six hydrocarbon species, Lagrangian air parcel trajectories were implemented in a meteorological model to extend the resolution of these measurements and achieve domain-fillings of the region for the period of interest. A self-organizing map (a type of unsupervised classification) was then utilized to reduce the dimensionality of the total multivariate set of grids into characteristic one-dimensional signatures. By also introducing a self-organizing map classification of the contemporary wind measurements, the spatial hydrocarbon characterizations are analyzed for periods with similar wind conditions. The accuracy of the classification is verified through assessment of observed spatial mixing ratio enhancements of key species, through site-comparisons with a related long-term study, and through a random forest analysis (an ensemble learning method of supervised classification) to determine the most important species for defining key classes. The hydrocarbon

Designing and implementing science-based methane policies

Science.gov (United States)

George, F.

2017-12-01

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

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

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

Science.gov (United States)

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

2018-01-01

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

The Boston Methane Project: Mapping Surface Emissions to Inform Atmospheric Estimation of Urban Methane Flux

Science.gov (United States)

Phillips, N.; Crosson, E.; Down, A.; Hutyra, L.; Jackson, R. B.; McKain, K.; Rella, C.; Raciti, S. M.; Wofsy, S. C.

2012-12-01

Lost and unaccounted natural gas can amount to over 6% of Massachusetts' total annual greenhouse gas inventory (expressed as equivalent CO2 tonnage). An unknown portion of this loss is due to natural gas leaks in pipeline distribution systems. The objective of the Boston Methane Project is to estimate the overall leak rate from natural gas systems in metropolitan Boston, and to compare this flux with fluxes from the other primary methane emissions sources. Companion talks at this meeting describe the atmospheric measurement and modeling framework, and chemical and isotopic tracers that can partition total atmospheric methane flux into natural gas and non-natural gas components. This talk focuses on estimation of surface emissions that inform the atmospheric modeling and partitioning. These surface emissions include over 3,300 pipeline natural gas leaks in Boston. For the state of Massachusetts as a whole, the amount of natural gas reported as lost and unaccounted for by utility companies was greater than estimated landfill emissions by an order of magnitude. Moreover, these landfill emissions were overwhelmingly located outside of metro Boston, while gas leaks are concentrated in exactly the opposite pattern, increasing from suburban Boston toward the urban core. Work is in progress to estimate spatial distribution of methane emissions from wetlands and sewer systems. We conclude with a description of how these spatial data sets will be combined and represented for application in atmospheric modeling.

Methane emissions from a high arctic valley: findings and challenges

DEFF Research Database (Denmark)

Mastepanov, Mikhail; Sigsgaard, Charlotte; Ström, Lena

2008-01-01

Wet tundra ecosystems are well-known to be a significant source of atmospheric methane. With the predicted stronger effect of global climate change on arctic terrestrial ecosystems compared to lower-latitudes, there is a special obligation to study the natural diversity and the range of possible...... feedback effects on global climate that could arise from Arctic tundra ecosystems. One of the prime candidates for such a feedback mechanism is a potential change in the emissions of methane. Long-term datasets on methane emissions from high arctic sites are almost non-existing but badly needed...... for analyses of controls on interannual and seasonal variations in emissions. To help fill this gap we initiated a measurement program in a productive high arctic fen in the Zackenberg valley, NE Greenland. Methane flux measurements have been carried out at the same location since 1997. Compared...

Design and evaluation of a porous burner for the mitigation of anthropogenic methane emissions.

Science.gov (United States)

Wood, Susie; Fletcher, David F; Joseph, Stephen D; Dawson, Adrian; Harris, Andrew T

2009-12-15

Methane constitutes 15% of total global anthropogenic greenhouse gas emissions. The mitigation of these emissions could have a significant near-term effect on slowing global warming, and recovering and burning the methane would allow a wasted energy resource to be exploited. The typically low and fluctuating energy content of the emission streams makes combustion difficult; however porous burners-an advanced combustion technology capable of burning low-calorific value fuels below the conventional flammability limit-are one possible mitigation solution. Here we discuss a pilot-scale porous burner designed for this purpose. The burner comprises a cylindrical combustion chamber filled with a porous bed of alumina saddles, combined with an arrangement of heat exchanger tubes for preheating the incoming emission stream. A computational fluid dynamics model was developed to aid in the design process. Results illustrating the burner's stable operating range and behavior are presented: stable ultralean combustion is demonstrated at natural gas concentrations as low as 2.3 vol%, with transient combustion at concentrations down to 1.1 vol%; the system is comparatively stable to perturbations in the operating conditions, and emissions of both carbon monoxide and unburned hydrocarbons are negligible. Based on this pilot-scale demonstration, porous burners show potential as a methane mitigation technology.

Methane and sulfate dynamics in sediments from mangrove-dominated tropical coastal lagoons, Yucatan, Mexico

Science.gov (United States)

Chuang, P. C.; Young, Megan B.; Dale, Andrew W.; Miller, Laurence G.; Herrera-Silveira, Jorge A.; Paytan, Adina

2016-01-01

Porewater profiles in sediment cores from mangrove-dominated coastal lagoons (Celestún and Chelem) on the Yucatán Peninsula, Mexico, reveal the widespread coexistence of dissolved methane and sulfate. This observation is interesting since dissolved methane in porewaters is typically oxidized anaerobically by sulfate. To explain the observations we used a numerical transport-reaction model that was constrained by the field observations. The model suggests that methane in the upper sediments is produced in the sulfate reduction zone at rates ranging between 0.012 and 31 mmol m−2 d−1, concurrent with sulfate reduction rates between 1.1 and 24 mmol SO42− m−2 d−1. These processes are supported by high organic matter content in the sediment and the use of non-competitive substrates by methanogenic microorganisms. Indeed sediment slurry incubation experiments show that non-competitive substrates such as trimethylamine (TMA) and methanol can be utilized for microbial methanogenesis at the study sites. The model also indicates that a significant fraction of methane is transported to the sulfate reduction zone from deeper zones within the sedimentary column by rising bubbles and gas dissolution. The shallow depths of methane production and the fast rising methane gas bubbles reduce the likelihood for oxidation, thereby allowing a large fraction of the methane formed in the sediments to escape to the overlying water column.

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

Science.gov (United States)

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

2014-01-01

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

Measurements of VOCs in Mexico City during the MILAGRO Campaign

Science.gov (United States)

Baker, A. K.; Beyersdorf, A. J.; Blake, N. J.; Meinardi, S.; Atlas, E.; Rowland, F.; Blake, D. R.

2006-12-01

During March of 2006 we participated in MILAGRO (Megacities Initiative: Local and Global Research Observations), a multi-platform campaign to measure pollutants in and in outflow from the Mexico City metropolitan area. As part of MILAGRO we collected whole air canister samples at two Mexico City ground sites: the Instituto Mexicano del Petroleo, located in the city, northeast of the center, and the Universidad Technologica de Tecamac, a suburban site approximately 50 km northeast of the city center. Samples were also collected in various other locations throughout Mexico City. Over 300 whole air samples were collected and analyzed for a wide range of volatile organic compounds (VOCs) including methane, carbon monoxide, nonmethane hydrocarbons (NMHCs) and halocarbons. Propane was the most abundant NMHC at both the urban and suburban locations, with mixing ratios frequently in excess of 10 parts per billion at both locations. This is likely the result of the widespread use of liquefied petroleum gas (LPG) of which propane is the major component. For most species, median mixing ratios at the urban sites were significantly greater than at the suburban site. Here we compare results from both urban and suburban locations and also examine the influence of transport on the composition of outflow from Mexico City.

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

Data.gov (United States)

National Aeronautics and Space Administration — In situ production of methane as propellant and oxygen as life support consumables from the atmospheric CO2 and water on Mars is a key enabling technology required...

Utilization of coalbed methane

Energy Technology Data Exchange (ETDEWEB)

Gustavson, J.B. [Gustavson Associates Inc., Boulder, CO (United States)

1996-02-01

Substantial progress has been made in capturing coalbed methane (CBM gas), which constitutes a valuable source of clean burning energy. It is of importance to study the various potential uses of coalbed methane and to understand the various technologies required, as well as their economics and any institutional constraints. In industrialised countries, the uses of coalbed methane are almost solely dependent on microeconomics; coalbed methane must compete for a market against natural gas and other energy sources - and frequently, coalbed methane is not competitive against other energy sources. In developing countries, on the other hand, particularly where other sources of energy are in short supply, coalbed methane economics yield positive results. Here, constraints to development of CBM utilization are mainly lack of technology and investment capital. Sociological aspects such as attitude and cultural habits, may also have a strong negative influence. This paper outlines the economics of coalbed methane utilization, particularly its competition with natural gas, and touches upon the many different uses to which coalbed methane may be applied. 24 refs., 4 figs.

Doses from radioactive methane

International Nuclear Information System (INIS)

Phipps, A.W.; Kendall, G.M.; Fell, T.P.; Harrison, J.D.

1990-01-01

A possible radiation hazard arises from exposure to methane labelled with either a 3 H or a 14 C nuclide. This radioactive methane could be released from a variety of sources, e.g. land burial sites containing radioactive waste. Standard assumptions adopted for vapours would not apply to an inert alkane like methane. This paper discusses mechanisms by which radioactive methane would irradiate tissues and provides estimates of doses. Data on skin thickness and metabolism of methane are discussed with reference to these mechanisms. It is found that doses are dominated by dose from the small fraction of methane which is inhaled and metabolised. This component of dose has been calculated under rather conservative assumptions. (author)

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

Science.gov (United States)

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

2016-03-01

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

Martian methane plume models for defining Mars rover methane source search strategies

Science.gov (United States)

Nicol, Christopher; Ellery, Alex; Lynch, Brian; Cloutis, Ed

2018-07-01

The detection of atmospheric methane on Mars implies an active methane source. This introduces the possibility of a biotic source with the implied need to determine whether the methane is indeed biotic in nature or geologically generated. There is a clear need for robotic algorithms which are capable of manoeuvring a rover through a methane plume on Mars to locate its source. We explore aspects of Mars methane plume modelling to reveal complex dynamics characterized by advection and diffusion. A statistical analysis of the plume model has been performed and compared to analyses of terrestrial plume models. Finally, we consider a robotic search strategy to find a methane plume source. We find that gradient-based techniques are ineffective, but that more sophisticated model-based search strategies are unlikely to be available in near-term rover missions.

Co-generation of synthesis gas and C{sub 2+} hydrocarbons from methane and carbon dioxide in a hybrid catalytic-plasma reactor: A review

Energy Technology Data Exchange (ETDEWEB)

Istadi; Nor Aishah Saidina Amin [Universiti Teknologi Malaysia, Johor Bahru (Malaysia). Chemical Reaction Engineering Group (CREG), Faculty of Chemical and Natural Resources Engineering

2006-03-15

The topics on conversion and utilization of methane and carbon dioxide are important issues in tackling the global warming effects from the two greenhouse gases. Several technologies including catalytic and plasma have been proposed to improve the process involving conversion and utilization of methane and carbon dioxide. In this paper, an overview of the basic principles, and the effects of CH{sub 4}/CO{sub 2} feed ratio, total feed flow rate, discharge power, catalyst, applied voltage, wall temperature, and system pressure in dielectric-barrier discharge (DBD) plasma reactor are addressed. The discharge power, discharge gap, applied voltage and CH{sub 4}/CO{sub 2} ratio in the feed showed the most significant effects on the reactor performance. Co-feeding carbon dioxide with the methane feed stream reduced coking and increased methane conversion. The H{sub 2}/CO ratio in the products was significantly affected by CH{sub 4}/CO{sub 2} ratio. The synergism of the catalyst placed in the discharge gap and the plasma affected the products distribution significantly. Methane and carbon dioxide conversions were influenced significantly by discharge power and applied voltage. The drawbacks of DBD plasma application in the CH{sub 4}-CO{sub 2} conversion should be taken into consideration before a new plausible reactor system can be implemented. 76 refs., 4 figs., 2 tabs.

Design and Use of a Full Flow Sampling System (FFS) for the Quantification of Methane Emissions.

Science.gov (United States)

Johnson, Derek R; Covington, April N; Clark, Nigel N

2016-06-12

The use of natural gas continues to grow with increased discovery and production of unconventional shale resources. At the same time, the natural gas industry faces continued scrutiny for methane emissions from across the supply chain, due to methane's relatively high global warming potential (25-84x that of carbon dioxide, according to the Energy Information Administration). Currently, a variety of techniques of varied uncertainties exists to measure or estimate methane emissions from components or facilities. Currently, only one commercial system is available for quantification of component level emissions and recent reports have highlighted its weaknesses. In order to improve accuracy and increase measurement flexibility, we have designed, developed, and implemented a novel full flow sampling system (FFS) for quantification of methane emissions and greenhouse gases based on transportation emissions measurement principles. The FFS is a modular system that consists of an explosive-proof blower(s), mass airflow sensor(s) (MAF), thermocouple, sample probe, constant volume sampling pump, laser based greenhouse gas sensor, data acquisition device, and analysis software. Dependent upon the blower and hose configuration employed, the current FFS is able to achieve a flow rate ranging from 40 to 1,500 standard cubic feet per minute (SCFM). Utilization of laser-based sensors mitigates interference from higher hydrocarbons (C2+). Co-measurement of water vapor allows for humidity correction. The system is portable, with multiple configurations for a variety of applications ranging from being carried by a person to being mounted in a hand drawn cart, on-road vehicle bed, or from the bed of utility terrain vehicles (UTVs). The FFS is able to quantify methane emission rates with a relative uncertainty of ± 4.4%. The FFS has proven, real world operation for the quantification of methane emissions occurring in conventional and remote facilities.

Design and Use of a Full Flow Sampling System (FFS) for the Quantification of Methane Emissions

Science.gov (United States)

Johnson, Derek R.; Covington, April N.; Clark, Nigel N.

2016-01-01

The use of natural gas continues to grow with increased discovery and production of unconventional shale resources. At the same time, the natural gas industry faces continued scrutiny for methane emissions from across the supply chain, due to methane's relatively high global warming potential (25-84x that of carbon dioxide, according to the Energy Information Administration). Currently, a variety of techniques of varied uncertainties exists to measure or estimate methane emissions from components or facilities. Currently, only one commercial system is available for quantification of component level emissions and recent reports have highlighted its weaknesses. In order to improve accuracy and increase measurement flexibility, we have designed, developed, and implemented a novel full flow sampling system (FFS) for quantification of methane emissions and greenhouse gases based on transportation emissions measurement principles. The FFS is a modular system that consists of an explosive-proof blower(s), mass airflow sensor(s) (MAF), thermocouple, sample probe, constant volume sampling pump, laser based greenhouse gas sensor, data acquisition device, and analysis software. Dependent upon the blower and hose configuration employed, the current FFS is able to achieve a flow rate ranging from 40 to 1,500 standard cubic feet per minute (SCFM). Utilization of laser-based sensors mitigates interference from higher hydrocarbons (C2+). Co-measurement of water vapor allows for humidity correction. The system is portable, with multiple configurations for a variety of applications ranging from being carried by a person to being mounted in a hand drawn cart, on-road vehicle bed, or from the bed of utility terrain vehicles (UTVs). The FFS is able to quantify methane emission rates with a relative uncertainty of ± 4.4%. The FFS has proven, real world operation for the quantification of methane emissions occurring in conventional and remote facilities. PMID:27341646

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

Science.gov (United States)

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

2017-12-01

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

Oil shale, shale oil, shale gas and non-conventional hydrocarbons

Directory of Open Access Journals (Sweden)

Clerici A.

2015-01-01

Full Text Available In recent years there has been a world “revolution” in the field of unconventional hydrocarbon reserves, which goes by the name of “shale gas”, gas contained inside clay sediments micropores. Shale gas finds particular development in the United States, which are now independent of imports and see a price reduction to less than one third of that in Europe. With the high oil prices, in addition to the non-conventional gas also “oil shales” (fine-grained sedimentary rocks that contain a large amount of organic material to be used both to be directly burned or to extract liquid fuels which go under the name of shale oil, extra heavy oils and bitumen are becoming an industrial reality. Both unconventional gas and oil reserves far exceed in the world the conventional oil and gas reserves, subverting the theory of fossil fuels scarcity. Values and location of these new fossil reserves in different countries and their production by comparison with conventional resources are presented. In view of the clear advantages of unconventional fossil resources, the potential environmental risks associated with their extraction and processing are also highlighted.

Decadal changes in emissions of volatile organic compounds (VOCs) from on-road vehicles with intensified automobile pollution control: Case study in a busy urban tunnel in south China.

Science.gov (United States)

Zhang, Yanli; Yang, Weiqiang; Simpson, Isobel; Huang, Xinyu; Yu, Jianzhen; Huang, Zhonghui; Wang, Zhaoyi; Zhang, Zhou; Liu, Di; Huang, Zuzhao; Wang, Yujun; Pei, Chenglei; Shao, Min; Blake, Donald R; Zheng, Junyu; Huang, Zhijiong; Wang, Xinming

2018-02-01

In the efforts at controlling automobile emissions, it is important to know in what extent air pollutants from on-road vehicles could be truly reduced. In 2014 we conducted tests in a heavily trafficked tunnel in south China to characterize emissions of volatile organic compounds (VOC) from on-road vehicle fleet and compared our results with those obtained in the same tunnel in 2004. Alkanes, aromatics, and alkenes had average emission factors (EFs) of 338, 63, and 42 mg km -1 in 2014 against that of 194, 129, and 160 mg km -1 in 2004, respectively. In 2014, LPG-related propane, n-butane and i-butane were the top three non-methane hydrocarbons (NMHCs) with EFs of 184 ± 21, 53 ± 6 and 31 ± 3 mg km -1 ; the gasoline evaporation marker i-pentane had an average EF of 17 ± 3 mg km -1 ; ethylene and propene were the top two alkenes with average EFs of 16 ± 1 and 9.7 ± 0.9 mg km -1 , respectively; isoprene had no direct emission from vehicles; toluene showed the highest EF of 11 ± 2 mg km -1 among the aromatics; and acetylene had an average EF of 7 ± 1 mg km -1 . While EFs of total NMHCs decreased only 9% from 493 ± 120 mg km -1 in 2004 to 449 ± 40 mg km -1 in 2014, their total ozone formation potential (OFP) decreased by 57% from 2.50 × 10 3  mg km -1 in 2004 to 1.10 × 10 3  mg km -1 in 2014, and their total secondary organic aerosol formation potential (SOAFP) decreased by 50% from 50 mg km -1 in 2004 to 25 mg km -1 in 2014. The large drop in ozone and SOA formation potentials could be explained by reduced emissions of reactive alkenes and aromatics, due largely to fuel transition from gasoline/diesel to LPG for taxis/buses and upgraded vehicle emission standards. Copyright © 2017 Elsevier Ltd. All rights reserved.

Thermochemical performance analysis of solar driven CO_2 methane reforming

International Nuclear Information System (INIS)

Fuqiang, Wang; Jianyu, Tan; Huijian, Jin; Yu, Leng

2015-01-01

Increasing CO_2 emission problems create urgent challenges for alleviating global warming, and the capture of CO_2 has become an essential field of scientific research. In this study, a finite volume method (FVM) coupled with thermochemical kinetics was developed to analyze the solar driven CO_2 methane reforming process in a metallic foam reactor. The local thermal non-equilibrium (LTNE) model coupled with radiative heat transfer was developed to provide more temperature information. A joint inversion method based on chemical process software and the FVM coupled with thermochemical kinetics was developed to obtain the thermochemical reaction parameters and guarantee the calculation accuracy. The detailed thermal and thermochemical performance in the metal foam reactor was analyzed. In addition, the effects of heat flux distribution and porosity on the solar driven CO_2 methane reforming process were analyzed. The numerical results can serve as theoretical guidance for the solar driven CO_2 methane reforming application. - Highlights: • Solar driven CO_2 methane reforming process in metal foam reactor is analyzed. • FVM with chemical reactions was developed to analyze solar CO_2 methane reforming. • A joint inversion method was developed to obtain thermochemical reaction parameters. • Results can be a guidance for the solar driven CO_2 methane reforming application.

Singler-chamber SOFCs based on gadolinia doped ceria operated on methane and propane; Pilas de combustible de una sola camara, basadas en electrolitos de ceria dopada con gadolinia y operadas con metano y propano

Energy Technology Data Exchange (ETDEWEB)

Morales, M.; Roa, J. J.; Capdevila, X. G.; Segarra, M.; Pinol, S.

2010-07-01

The main advantages of single-chamber solid oxide fuel cells (SOFCs) respect to dual-chamber SOFCs, are to simplify the device design and to operate in mixtures of hydrocarbon (methane, propane...) and air, with no separation between fuel and oxidant. However, this design requires the use of selective electrodes for the fuel oxidation and the oxidant reduction. In this work, electrolyte-supported SOFCs were fabricated using gadolinia doped ceria (GDC) as the electrolyte, Ni + GDC as the anode and LSC(La{sub 0}.5Sr{sub 0}.5CoO{sub 3}-{delta})-GDC-Ag{sub 2}O as the cathode. The electrical properties of the cell were determined in mixtures of methane + air and propane + air. The influence of temperature, gas composition and total flow rate on the fuel cell performance was investigated. As a result, the power density was strongly increased with increasing temperature, total flow rate and hydrocarbon composition. Under optimized gas compositions and total flow conditions, power densities of 70 and 320 mW/cm{sup 2} operating on propane at a temperature of 600 degree centigrade and methane (795 degree centigrade) were obtained, respectively. (Author)

Aromatic hydrocarbons

International Nuclear Information System (INIS)

Roder, M.

1985-01-01

Papers dealing with radiolysis of aromatic hydrocarbons of different composition (from benzene to terphenyls and hydrocarbons with condensed rings) as well as their mixtures (with alkanes, alkenes, other aromatic hydrocarbons) are reviewed. High radiation stability of aromatic hydrocarbons in condensed phases associated with peculiarities of molecular structure of compounds is underlined. Mechanisms of radiolytic processes, vaues of product yields are considered

CARVE Measurements of Atmospheric Methane Concentrations and Emissions in Arctic and Boreal Alaska

Science.gov (United States)

Miller, C. E.; Miller, J. B.; Chang, R. Y.; Sweeney, C.; Karion, A.; Wofsy, S. C.; Henderson, J.; Eluszkiewicz, J.; Mountain, M.; Oechel, W. C.

2013-12-01

The Carbon in Arctic Reservoirs Vulnerability Experiment (CARVE) is a NASA Earth Ventures (EV-1) investigation designed to quantify correlations between atmospheric and surface state variables for the Alaskan terrestrial ecosystems through intensive seasonal aircraft campaigns, ground-based observations, and analysis sustained over a 5-year mission. CARVE bridges critical gaps in our knowledge and understanding of Arctic ecosystems, linkages between the Arctic hydrologic and terrestrial carbon cycles, and the feedbacks from fires and thawing permafrost. We present CARVE airborne measurements of spatial and temporal patterns in atmospheric CH4 concentrations and estimated surface-atmosphere emissions for Arctic and Boreal Alaska. Continuous in situ CH4, CO2 and CO data are supplemented by periodic whole air flask samples from which 13CH4 and non-methane hydrocarbons are used to assess the relative contributions of wetlands, fossil fuel combustion, and oil and gas production to the observed CH4 signals. The CARVE project has also initiated monthly 14CH4 sampling at Barrow, AK (BRW) and the CARVE Tower in Fox, AK (CRV) to evaluate seasonal changes in the fraction of old carbon being mobilized via methanogenesis.

Atmospheric methane removal by methane-oxidizing bacteria immobilized on porous building materials

NARCIS (Netherlands)

Ganendra, G; De Muynck, W; Ho, A.; Hoefman, S.; De Vos, P.; Boeckx, P.; Boon, N.

2014-01-01

Biological treatment using methane-oxidizing bacteria (MOB) immobilized on six porous carrier materials have been used to mitigate methane emission. Experiments were performed with different MOB inoculated in building materials at high (similar to 20 % (v/v)) and low (similar to 100 ppmv) methane

Methane oxidation and methane fluxes in the ocean surface layer and deep anoxic waters

Science.gov (United States)

Ward, B. B.; Kilpatrick, K. A.; Novelli, P. C.; Scranton, M. I.

1987-01-01

Measured biological oxidation rates of methane in near-surface waters of the Cariaco Basin are compared with the diffusional fluxes computed from concentration gradients of methane in the surface layer. Methane fluxes and oxidation rates were investigated in surface waters, at the oxic/anoxic interface, and in deep anoxic waters. It is shown that the surface-waters oxidation of methane is a mechanism which modulates the flux of methane from marine waters to the atmosphere.

Coalbed Methane Outreach Program

Science.gov (United States)

Coalbed Methane Outreach Program, voluntary program seeking to reduce methane emissions from coal mining activities. CMOP promotes profitable recovery/use of coal mine methane (CMM), addressing barriers to using CMM instead of emitting it to atmosphere.

Contribution of emissions to concentrations: the TAGGING 1.0 submodel based on the Modular Earth Submodel System (MESSy 2.52)

Science.gov (United States)

Grewe, Volker; Tsati, Eleni; Mertens, Mariano; Frömming, Christine; Jöckel, Patrick

2017-07-01

Questions such as what is the contribution of road traffic emissions to climate change? or what is the impact of shipping emissions on local air quality? require a quantification of the contribution of specific emissions sectors to the concentration of radiatively active species and air-quality-related species, respectively. Here, we present a diagnostics package, implemented in the Modular Earth Submodel System (MESSy), which keeps track of the contribution of source categories (mainly emission sectors) to various concentrations. The diagnostics package is implemented as a submodel (TAGGING) of EMAC (European Centre for Medium-Range Weather Forecasts - Hamburg (ECHAM)/MESSy Atmospheric Chemistry). It determines the contributions of 10 different source categories to the concentration of ozone, nitrogen oxides, peroxyacytyl nitrate, carbon monoxide, non-methane hydrocarbons, hydroxyl, and hydroperoxyl radicals ( = tagged tracers). The source categories are mainly emission sectors and some other sources for completeness. As emission sectors, road traffic, shipping, air traffic, anthropogenic non-traffic, biogenic, biomass burning, and lightning are considered. The submodel obtains information on the chemical reaction rates, online emissions, such as lightning, and wash-out rates. It then solves differential equations for the contribution of a source category to each of the seven tracers. This diagnostics package does not feed back to any other part of the model. For the first time, it takes into account chemically competing effects: for example, the competition between NOx, CO, and non-methane hydrocarbons (NMHCs) in the production and destruction of ozone. We show that the results are in-line with results from other tagging schemes and provide plausibility checks for concentrations of trace gases, such as OH and HO2, which have not previously been tagged. The budgets of the tagged tracers, i.e. the contribution from individual source categories (mainly emission

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

Science.gov (United States)

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

2018-05-01

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

Methane emissions from rice paddies : experiments and modelling

NARCIS (Netherlands)

Bodegom, van P.M.

2000-01-01

This thesis describes model development and experimentation on the comprehension and prediction of methane (CH ₄ ) emissions from rice paddies. The large spatial and temporal variability in CH ₄ emissions and the dynamic non-linear relationships

Simplifiying global biogeochemistry models to evaluate methane emissions

Science.gov (United States)

Gerber, S.; Alonso-Contes, C.

2017-12-01

Process-based models are important tools to quantify wetland methane emissions, particularly also under climate change scenarios, evaluating these models is often cumbersome as they are embedded in larger land-surface models where fluctuating water table and the carbon cycle (including new readily decomposable plant material) are predicted variables. Here, we build on these large scale models but instead of modeling water table and plant productivity we provide values as boundary conditions. In contrast, aerobic and anaerobic decomposition, as well as soil column transport of oxygen and methane are predicted by the model. Because of these simplifications, the model has the potential to be more readily adaptable to the analysis of field-scale data. Here we determine the sensitivity of the model to specific setups, parameter choices, and to boundary conditions in order to determine set-up needs and inform what critical auxiliary variables need to be measured in order to better predict field-scale methane emissions from wetland soils. To that end we performed a global sensitivity analysis that also considers non-linear interactions between processes. The global sensitivity analysis revealed, not surprisingly, that water table dynamics (both mean level and amplitude of fluctuations), and the rate of the carbon cycle (i.e. net primary productivity) are critical determinants of methane emissions. The depth-scale where most of the potential decomposition occurs also affects methane emissions. Different transport mechanisms are compensating each other to some degree: If plant conduits are constrained, methane emissions by diffusive flux and ebullition compensate to some degree, however annual emissions are higher when plants help to bypass methanotrophs in temporally unsaturated upper layers. Finally, while oxygen consumption by plant roots help creating anoxic conditions it has little effect on overall methane emission. Our initial sensitivity analysis helps guiding

Project identification for methane reduction options

Energy Technology Data Exchange (ETDEWEB)

Kerr, T.

1996-12-31

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

Investigation Status of Heat Exchange while Boiling Hydrocarbon Fuel

Directory of Open Access Journals (Sweden)

D. S. Obukhov

2006-01-01

Full Text Available The paper contains analysis of heat exchange investigations while boiling hydrocarbon fuel. The obtained data are within the limits of the S.S. Kutateladze dependence proposed in 1939. Heat exchange at non-stationary heat release has not been investigated. The data for hydrocarbon fuel with respect to critical density of heat flow are not available even for stationary conditions.

Mensuration of the propagation speed of mixed flames of Methane-air and gas natural, Guajira - air using the method of the angle of the cone

International Nuclear Information System (INIS)

Benjumea Hernandez, Pedro Nel; Higuita Bedoya Carlos Mario; Cordoba Perez, Camilo Andres

2004-01-01

In this work, the burning velocity of premixed laminar flames of methane-air and Guajira natural gas-air mixtures was measured by the cone's angle method using a cylindrical Bunsen burner. In the development of the experiments, a fuel concentration in the fuel-air mixture ranging from 9% -11% was taken. The maximum value of the burning velocity was obtained for mixtures a little bit richer than the stoichiometric case. For methane, this flame velocity was 44.1 cm/s and for the Guajira natural gas was 43.1 cm/s. From the results, it was possible to see that the Guajira natural gas inert content led to a burning velocity value lesser than the methane's, in spite of the Guajira natural gas having a higher heavy hydrocarbon content. Methane burning velocity values following similar trends to those reported by the literature were obtained. The systematic error found in the results is mainly a consequence of inaccuracies in the method used to measure the fuel-gas mixture velocity at the burner exit

Emission sources of non-methane volatile organic compounds (NMVOCs) and their contribution to photochemical ozone (O3) formation at an urban atmosphere in western India.

Science.gov (United States)

Yadav, R.; Sahu, L. K.; Tripathi, N.; Pal, D.

2017-12-01

Atmospheric non-methane volatile organic compounds (NMVOCs) were measured at a sampling site in Udaipur city of western India during 2015 to recognize their pollution levels, variation characteristics, sources and photochemical reactivity. The samples were analyzed for NMVOCs using a Gas Chromatograph equipped with Flame Ionization Detector (GC/FID) and Thermal Desorption (TD) system. The main focus on understand the sources responsible for NMVOC emissions, and evaluating the role of the identified sources towards ozone formation. Hourly variations of various NMVOC species indicate that VOCs mixing ratios were influenced by photochemical removal with OH radicals for reactive species, secondary formation for oxygenated VOCs. In general, higher mixing ratios were observed during winter/pre-monsoon and lower levels during the monsoon season due to the seasonal change in meteorological, transport path of air parcel and boundary layer conditions. The high levels of propane (C3H8) and butane (C4H10) show the dominance of LPG over the study location. The correlation coefficients of typical NMVOC pairs (ethylene/propylene, propylene/isoprene, and ethane/propane) depicted that vehicular emission and natural gas leakages were important sources for atmospheric hydrocarbons in Udaipur. Based on the annual data, PMF analysis suggest the source factors namely biomass burning/ bio-fuel, automobile exhaust, Industrial/ natural gas/power plant emissions, petrol/Diesel, gasoline evaporation, and use of liquid petroleum gas (LPG) contribute to NMVOCs loading. The propylene-equivalent and ozone formation potential of NMVOCs have also been calculated in order to find out their OH reactivity and contribution to the photochemical ozone formation.

H2-rich and Hydrocarbon Gas Recovered in a Deep Precambrian Well in Northeastern Kansas

International Nuclear Information System (INIS)

Newell, K. David; Doveton, John H.; Merriam, Daniel F.; Lollar, Barbara Sherwood; Waggoner, William M.; Magnuson, L. Michael

2007-01-01

In late 2005 and early 2006, the WTW Operating, LLC (W.T.W. Oil Co., Inc.) no. 1 Wilson well (T.D. = 5772 ft; 1759.3 m) was drilled for 1826 ft (556.6 m) into Precambrian basement underlying the Forest City Basin in northeastern Kansas. Approximately 4500 of the 380,000 wells drilled in Kansas penetrate Precambrian basement. Except for two previous wells drilled into the arkoses and basalts of the 1.1-Ga Midcontinent Rift and another well drilled in 1929 in basement on the Nemaha Uplift east of the Midcontinent Rift, this well represents the deepest penetration into basement rocks in the state to date. Granite is the typical lithology observed in wells that penetrate the Precambrian in the northern Midcontinent. Although no cores were taken to definitively identify lithologies, well cuttings and petrophysical logs indicate that this well encountered basement metamorphic rocks consisting of schist, gneiss, and amphibolitic gneiss, all cut by aplite dikes.The well was cased and perforated in the Precambrian, and then acidized. After several days of swabbing operations, the well produced shows of low-Btu gas, dominated by the non-flammable component gases of nitrogen (20%), carbon dioxide (43%), and helium (1%). Combustible components include methane (26%), hydrogen (10%), and higher molecular-weight hydrocarbons (1%). Although Coveney and others [Am. Assoc. Petroleum Geologists Bull., v. 71, no, 1, p. 39-48, 1987] identified H 2 -rich gas in two wells located close to the Midcontinent Rift in eastern Kansas, this study indicates that high levels of H 2 may be a more widespread phenomenon than previously thought. Unlike previous results, the gases in this study have a significant component of hydrocarbon gas, as well as H 2 , N 2 , and CO 2 . Although redox reactions between iron-bearing minerals and groundwater are a possible source of H 2 in the Precambrian basement rocks, the hydrocarbon gas does not exhibit the characteristics typically associated with proposed

Investigation of Underground Hydrocarbon Leakage using Ground Penetrating Radar

Science.gov (United States)

Srigutomo, Wahyu; Trimadona; Agustine, Eleonora

2016-08-01

Ground Penetrating Radar (GPR) survey was carried out in several petroleum plants to investigate hydrocarbon contamination beneath the surface. The hydrocarbon spills are generally recognized as Light Non-Aqueous Phase Liquids (LNAPL) if the plume of leakage is distributed in the capillary fringe above the water table and as Dense Non-Aqueous Phase Liquids (DNAPL) if it is below the water table. GPR antennas of 200 MHz and 400 MHz were deployed to obtain clear radargrams until 4 m deep. In general, the interpreted radargram sections indicate the presence of surface concrete layer, the compacted silty soill followed by sand layer and the original clayey soil as well as the water table. The presence of hydrocarbon plumes are identified as shadow zones (radar velocity and intensity contrasts) in the radargram that blur the layering pattern with different intensity of reflected signal. Based on our results, the characteristic of the shadow zones in the radargram is controlled by several factors: types of hydrocarbon (fresh or bio-degraded), water moisture in the soil, and clay content which contribute variation in electrical conductivity and dielectric constants of the soil.

Characterisation of coking activity during supercritical hydrocarbon pyrolysis

Energy Technology Data Exchange (ETDEWEB)

Gascoin, Nicolas; Gillard, Philippe; Bernard, Stephane [Laboratoire Energetique, Explosion, Structure, UPRES-EA 1205, 63, avenue de Lattre de Tassigny, 18020 Bourges Cedex (France); Bouchez, Marc [MBDA France, 8, rue Le Brix, 18000 Bourges (France)

2008-12-15

The active cooling of the Supersonic Combustion Ramjet engine, for hypersonic flight purpose, is ensured thanks to fuel, n-dodecane for the present study. The endothermic fuel pyrolysis, starting above 800 K, could generate an unwanted coke formation. Experimental tests up to 1125 K and between 1 MPa and 6 MPa have been performed on the hydrocarbon fuel pyrolysis to evaluate the coking activity. 316L stainless steel, low carbon steel and titanium reactors have been considered. A witness of the coke formation, based on its thermal insulation and pressure loss effects, has been found. A correlation between methane production and coke deposit was found. The coke has been studied with Scanning Electron Microscope (SEM), Energy Dispersion Spectroscopy (EDS), X-ray diffractometer and Fourier Transform Infrared (FTIR) spectroscopy. The porosity, the density and the permeability of the coke have been estimated. (author)

Global Methane Initiative

Science.gov (United States)

The Global Methane Initiative promotes cost-effective, near-term methane recovery through partnerships between developed and developing countries, with participation from the private sector, development banks, and nongovernmental organizations.

Predicting hydrocarbon potential of an earth formation underlying water

International Nuclear Information System (INIS)

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

1981-01-01

A method for the on-site collection and examination of small concentrations of a carbonaceous gas, e.g. methane, dissolved in a body of water overlying an earth formation to predict hydrocarbon potential of the earth formation under the body of water, the formation being a source of carbonaceous gas, comprises at a known geographic location sampling the water at a selected flow rate and at a selected depth; continuously vacuum separating the water into liquid and gas phases; separating a selected carbonaceous gas from interfering gas species in the presence of an air carrier vented to atmosphere at a known flow rate; and quantitatively oxidizing the selected gas and then cryogenically trapping an oxidant thereof in the presence of said air carrier to provide for an accurate isotopic examination. (author)

Determining the flux of methane into Hudson Canyon at the edge of methane clathrate hydrate stability

Science.gov (United States)

Weinsten, A.; Navarrete, L; Ruppel, Carolyn D.; Weber, T.C.; Leonte, M.; Kellermann, M.; Arrington, E.; Valentine, D.L.; Scranton, M.L; Kessler, John D.

2016-01-01

Methane seeps were investigated in Hudson Canyon, the largest shelf-break canyon on the northern US Atlantic Margin. The seeps investigated are located at or updip of the nominal limit of methane clathrate hydrate stability. The acoustic identification of bubble streams was used to guide water column sampling in a 32 km2 region within the canyon's thalweg. By incorporating measurements of dissolved methane concentration with methane oxidation rates and current velocity into a steady-state box model, the total emission of methane to the water column in this region was estimated to be 12 kmol methane per day (range: 6 – 24 kmol methane per day). These analyses suggest this methane is largely retained inside the canyon walls below 300 m water depth, and that it is aerobically oxidized to near completion within the larger extent of Hudson Canyon. Based on estimated methane emissions and measured oxidation rates, the oxidation of this methane to dissolved CO2 is expected to have minimal influences on seawater pH. This article is protected by copyright. All rights reserved.

Uncertainty assessment of the breath methane concentration method to determine methane production of dairy cows

NARCIS (Netherlands)

Wu, Liansun; Groot Koerkamp, Peter W.G.; Ogink, Nico

2018-01-01

The breath methane concentration method uses the methane concentrations in the cow's breath during feed bin visits as a proxy for the methane production rate. The objective of this study was to assess the uncertainty of a breath methane concentration method in a feeder and its capability to measure

State Air Quality Standards.

Science.gov (United States)

Pollution Engineering, 1978

1978-01-01

This article presents in tabular form the air quality standards for sulfur dioxide, carbon monoxide, nitrogen dioxide, photochemicals, non-methane hydrocarbons and particulates for each of the 50 states and the District of Columbia. (CS)

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

Science.gov (United States)

Hwang, In Yeub; Lee, Seung Hwan; Choi, Yoo Seong; Park, Si Jae; Na, Jeong Geol; Chang, In Seop; Kim, Choongik; Kim, Hyun Cheol; Kim, Yong Hwan; Lee, Jin Won; Lee, Eun Yeol

2014-12-28

Methane is considered as a next-generation carbon feedstock owing to the vast reserves of natural and shale gas. Methane can be converted to methanol by various methods, which in turn can be used as a starting chemical for the production of value-added chemicals using existing chemical conversion processes. Methane monooxygenase is the key enzyme that catalyzes the addition of oxygen to methane. Methanotrophic bacteria can transform methane to methanol by inhibiting methanol dehydrogenase. In this paper, we review the recent progress made on the biocatalytic conversion of methane to methanol as a key step for methane-based refinery systems and discuss future prospects for this technology.

Nitric Oxide and Oxygen Air-Contamination Effects on Extinction Limits of Non-Premixed Hydrocarbon-Air Flames for a HIFiRE Scramjet

Science.gov (United States)

Pellett, Gerald L.; Dawson, Lucy C.; Vaden, Sarah N.; Wilson, Lloyd G.

2009-01-01

Unique nitric oxide (NO) and oxygen air-contamination effects on the extinction Flame Strength (FS) of non-premixed hydrocarbon (HC) vs. air flames are characterized for 7 gaseous HCs, using a new idealized 9.3 mm straight-tube Opposed Jet Burner (OJB) at 1 atm. FS represents a laminar strain-induced extinction limit based on cross-section-average air jet velocity, Uair, that sustains combustion of a counter jet of gaseous fuel just before extinction. Besides ethane, propane, butane, and propylene, the HCs include ethylene, methane, and a 64 mole-% ethylene / 36 % methane mixture, the writer s previously recommended gaseous surrogate fuel for HIFiRE scramjet tests. The HC vs. clean air part of the work is an extension of a May 2008 JANNAF paper that characterized surrogates for the HIFiRE project that should mimic the flameholding of reformed (thermally- or catalytically-cracked) endothermic JP-like fuels. The new FS data for 7 HCs vs. clean air are thus consolidated with the previously validated data, normalized to absolute (local) axial-input strain rates, and co-plotted on a dual kinetically dominated reactivity scale. Excellent agreement with the prior data is obtained for all 7 fuels. Detailed comparisons are also made with recently published (Univ. Va) numerical results for ethylene extinction. A 2009-revised ethylene kinetic model (Univ. Southern Cal) led to predicted limits within approx. 5 % (compared to 45 %, earlier) of this writer s 2008 (and present) ethylene FSs, and also with recent independent data (Univ. Va) obtained on a new OJB system. These +/- 5 % agreements, and a hoped-for "near-identically-performing" reduced kinetics model, would greatly enhance the capability for accurate numerical simulations of surrogate HC flameholding in scramjets. The measured air-contamination effects on normalized FS extinction limits are projected to assess ongoing Arc-Heater-induced "facility test effects" of NO production (e.g., 3 mole-%) and resultant oxygen

A simple one-step chemistry model for partially premixed hydrocarbon combustion

Energy Technology Data Exchange (ETDEWEB)

Fernandez-Tarrazo, Eduardo [Instituto Nacional de Tecnica Aeroespacial, Madrid (Spain); Sanchez, Antonio L. [Area de Mecanica de Fluidos, Universidad Carlos III de Madrid, Leganes 28911 (Spain); Linan, Amable [ETSI Aeronauticos, Pl. Cardenal Cisneros 3, Madrid 28040 (Spain); Williams, Forman A. [Department of Mechanical and Aerospace Engineering, University of California San Diego, La Jolla, CA 92093-0411 (United States)

2006-10-15

This work explores the applicability of one-step irreversible Arrhenius kinetics with unity reaction order to the numerical description of partially premixed hydrocarbon combustion. Computations of planar premixed flames are used in the selection of the three model parameters: the heat of reaction q, the activation temperature T{sub a}, and the preexponential factor B. It is seen that changes in q with equivalence ratio f need to be introduced in fuel-rich combustion to describe the effect of partial fuel oxidation on the amount of heat released, leading to a universal linear variation q(f) for f>1 for all hydrocarbons. The model also employs a variable activation temperature T{sub a}(f) to mimic changes in the underlying chemistry in rich and very lean flames. The resulting chemistry description is able to reproduce propagation velocities of diluted and undiluted flames accurately over the whole flammability limit. Furthermore, computations of methane-air counterflow diffusion flames are used to test the proposed chemistry under nonpremixed conditions. The model not only predicts the critical strain rate at extinction accurately but also gives near-extinction flames with oxygen leakage, thereby overcoming known predictive limitations of one-step Arrhenius kinetics. (author)

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)

Mechanics of coalbed methane production

Energy Technology Data Exchange (ETDEWEB)

Creel, J C; Rollins, J B [Crawley, Gillespie and Associates, Inc. (United Kingdom)

1994-12-31

Understanding the behaviour of coalbed methane reservoirs and the mechanics of production is crucial to successful management of coalbed methane resources and projects. This paper discusses the effects of coal properties and coalbed methane reservoir characteristics on gas production rates and recoveries with a review of completion techniques for coalbed methane wells. 4 refs., 17 figs.

In Situ Hydrocarbon Degradation by Indigenous Nearshore Bacterial Populations

International Nuclear Information System (INIS)

Cherrier, J.

2005-01-01

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

Investigation of non-volatile additives on the process of distillation of hydrocarbon mixtures

Directory of Open Access Journals (Sweden)

М.Б. Степанов

2009-02-01

Full Text Available  The given results of researches of influence of nonvolatile additives on processes of distillation of individual hydrocarbons and their mixes, including petroleum and mineral oil. With the help of the developed computer system of the continuous control of distillation it is shown, that at the presence of small amounts of the additive decrease of temperature of the beginning of boiling of hydrocarbons is observed, their speeds of banish and exits of light fuel mineral oil grow during initial oil refining

Anaerobic methane oxidation rates at the sulfate-methane transition in marine sediments from Kattegat and Skagerrak (Denmark)

International Nuclear Information System (INIS)

Iversen, N.; Jorgensen, B.B.

1985-01-01

Concomitant radiotracer measurements were made of in situ rates of sulfate reduction and anaerobic methane oxidation in 2-3-m-long sediment cores. Methane accumulated to high concentrations (> 1 mM CH 4 ) only below the sulfate zone, at 1 m or deeper in the sediment. Sulfate reduction showed a broad maximum below the sediment surface and a smaller, narrow maximum at the sulfate-methane transition. Methane oxidation was low (0.002-0.1 nmol CH 4 cm -3 d -1 ) throughout the sulfate zone and showed a sharp maximum at the sulfate-methane transition, coinciding with the sulfate reduction maximum. Total anaerobic methane oxidation at two stations was 0.83 and 1.16 mmol CH 4 m -2 d -1 , of which 96% was confined to the sulfate-methane transition. All the methane that was calculated to diffuse up into the sulfate-methane transition was oxidized in this zone. The methane oxidation was equivalent to 10% of the electron donor requirement for the total measured sulfate reduction. A third station showed high sulfate concentrations at all depths sampled and the total methane oxidation was only 0.013 mmol m -2 d -1 . From direct measurements of rates, concentration gradients, and diffusion coefficients, simple calculations were made of sulfate and methane fluxes and of methane production rates

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

Science.gov (United States)

2010-07-01

... family are derived from averaging, banking, or trading programs. (ii)(A) Non-Methane Hydrocarbons (NMHC...) Operation within the NTE zone (defined in § 86.1370-2007) must comply with a filter smoke number of 1.0...

Job satisfaction and perceived autonomy for nurse practitioners working in nurse-managed health centers.

Science.gov (United States)

Pron, Ann Linguiti

2013-04-01

More primary care providers are needed to deliver health care to Americans living in poverty and those soon to be insured under the Affordable Care Act. Nurse practitioners (NPs) in nurse-managed health centers (NMHCs) are poised to meet this need. This research study examined the characteristics of NPs working in NMHCs and measured job satisfaction and perceived level of autonomy. No studies about job satisfaction or autonomy for NPs working in NMHCs had been previously reported. This descriptive, quantitative study surveyed primary care NPs working in NMHCs that are part of the National Nursing Centers Consortium (NNCC). NP e-mail addresses were obtained from NNCC center directors. Of 198 NPs invited to the electronic survey, 99 completed the Misener Nurse Practitioner Job Satisfaction Scale, demographic questionnaire, questions about perceived autonomy, and whether they would recommend working in an NMHC. Participants came from 16 states and 46 NMHCs. NPs working in NMHCs have job satisfaction, perceive their role as autonomous, and are satisfied with the autonomy they have. NMHCs can provide access to primary health care for many Americans. More NPs may choose employment in NMHCs for job satisfaction and autonomy. ©2012 The Author(s) Journal compilation ©2012 American Association of Nurse Practitioners.

Methane-fueled vehicles: A promising market for coalbed methane

International Nuclear Information System (INIS)

Deul, M.

1993-01-01

The most acceptable alternative fuel for motor vehicles is compressed natural gas (CNG). An important potential source of such gas is coalbed methane, much of which is now being wasted. Although there are no technological impediments to the use of CNG it has not been adequately promoted for a variety of reasons: structural, institutional and for coalbed gas, legal. The benefits of using CNG fuel are manifold: clean burning, low cost, abundant, and usable in any internal combustion engine. Even though more than 30,000 CNG vehicles are now in use in the U.S.A., they are not readily available, fueling stations are not easily accessible, and there is general apathy on the part of the public because of negligence by such agencies as the Department of Energy, the Department of Transportation and the Environmental Protection Agency. The economic benefits of using methane are significant: 100,000 cubic feet of methane is equivalent to 800 gallons of gasoline. Considering the many millions of cubic feet methane wasted from coal mines conservation and use of this resource is a worthy national goal

Is methane a new therapeutic gas?

Directory of Open Access Journals (Sweden)

Liu Wenwu

2012-09-01

Full Text Available Abstract Background Methane is an attractive fuel. Biologically, methanogens in the colon can use carbon dioxide and hydrogen to produce methane as a by-product. It was previously considered that methane is not utilized by humans. However, in a recent study, results demonstrated that methane could exert anti-inflammatory effects in a dog small intestinal ischemia-reperfusion model. Point of view Actually, the bioactivity of methane has been investigated in gastrointestinal diseases, but the exact mechanism underlying the anti-inflammatory effects is required to be further elucidated. Methane can cross the membrane and is easy to collect due to its abundance in natural gas. Although methane is flammable, saline rich in methane can be prepared for clinical use. These seem to be good news in application of methane as a therapeutic gas. Conclusion Several problems should be resolved before its wide application in clinical practice.

Determination of soil-entrapped methane

Energy Technology Data Exchange (ETDEWEB)

Alberto, M.C.R.; Neue, H.U.; Lantin, R.S.; Aduna, J.B. [Soil and Water Sciences Division, Manila (Philippines)

1996-12-31

A sampling method was developed and modified to sample soil from paddy fields for entrapped methane determination. A 25-cm long plexiglass tube (4.4-cm i.d.) fitted with gas bag was used to sample soil and entrapped gases to a depth of 15-cm. The sampling tube was shaken vigorously to release entrapped gases. Headspace gas in sampling tube and gas bag was analyzed for methane. The procedure was verified by doing field sampling weekly at an irrigated ricefield in the IRRI Research Farm on a Maahas clay soil. The modified sampling method gave higher methane concentration because it eliminated gas losses during sampling. The method gave 98% {+-} 5 recovery of soil-entrapped methane. Results of field sampling showed that the early growth stage of the rice plant, entrapped methane increased irrespective of treatment. This suggests that entrapped methane increased irrespective of treatment. This suggests that entrapped methane was primarily derived from fermentation of soil organic matter at the early growth stage. At the latter stage, the rice plant seems to be the major carbon source for methane production. 7 refs., 4 figs., 4 tabs.

Assessment of Surface Water Contamination from Coalbed Methane Fracturing-Derived Volatile Contaminants in Sullivan County, Indiana, USA.

Science.gov (United States)

Meszaros, Nicholas; Subedi, Bikram; Stamets, Tristan; Shifa, Naima

2017-09-01

There is a growing concern over the contamination of surface water and the associated environmental and public health consequences from the recent proliferation of hydraulic fracturing in the USA. Petroleum hydrocarbon-derived contaminants of concern [benzene, toluene, ethylbenzene, and xylenes (BTEX)] and various dissolved cations and anions were spatially determined in surface waters around 15 coalbed methane fracking wells in Sullivan County, IN, USA. At least one BTEX compound was detected in 69% of sampling sites (n = 13) and 23% of sampling sites were found to be contaminated with all of the BTEX compounds. Toluene was the most common BTEX compound detected across all sampling sites, both upstream and downstream from coalbed methane fracking wells. The average concentration of toluene at a reservoir and its outlet nearby the fracking wells was ~2× higher than other downstream sites. However, one of the upstream sites was found to be contaminated with BTEX at similar concentrations as in a reservoir site nearby the fracking well. Calcium (~60 ppm) and sulfates (~175 ppm) were the dominant cations and anions, respectively, in surface water around the fracking sites. This study represents the first report of BTEX contamination in surface water from coalbed methane hydraulic fracturing wells.

Determination of heavy polycyclic aromatic hydrocarbons by non-aqueous reversed phase liquid chromatography: Application and limitation in refining streams.

Science.gov (United States)

Panda, Saroj K; Muller, Hendrik; Al-Qunaysi, Thunayyan A; Koseoglu, Omer R

2018-01-19

The heavy polycyclic aromatic hydrocarbons (HPAHs) cause detrimental effects to hydrocracker operations by deactivating the catalysts and depositing in the downstream of the reactor/ exchangers. Therefore, it is essential to continuously monitor the accumulation of HPAHs in a hydrocracker unit. To accurately measure the concentration of HPAHs, the development of a fast and reliable analytical method is inevitable. In this work, an analytical method based on non-aqueous reversed phase chromatography in combination with high resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) was developed. As a first step, five different types of stationary phases were evaluated for the separation of HPAHs in non-aqueous mode and the best suited phase was further used for the fractionation of HPAHs in a fractionator bottom sample obtained from a refinery hydrocracker unit. The eight major fractions or peaks obtained from the separation were further characterized by UV spectroscopy and FT-ICR MS and the compounds in the fractions were tentatively confirmed as benzoperylene, coronene, methylcoronene, naphthenocoronene, benzocoronene, dibenzoperylene, naphthocoronene and ovalene. The developed liquid chromatography method can be easily adapted in a refinery laboratory for the quantitation of HPAHs in hydrocracking products. The method was further tested to check the interference of sulfur aromatics and/or large alkylated aromatic hydrocarbons on the determination of HPAHs in hydrocracking products. Copyright © 2017 Elsevier B.V. All rights reserved.

Detection of Abiotic Methane in Terrestrial Continental Hydrothermal Systems: Implications for Methane on Mars

Science.gov (United States)

Socki, Richard A.; Niles, Paul B.; Gibson, Everett K., Jr.; Romanek, Christopher S.; Zhang, Chuanlun L.; Bissada, Kadry K.

2008-01-01

The recent detection of methane in the Martian atmosphere and the possibility that its origin could be attributed to biological activity, have highlighted the importance of understanding the mechanisms of methane formation and its usefulness as a biomarker. Much debate has centered on the source of the methane in hydrothermal fluids, whether it is formed biologically by microorganisms, diagenetically through the decomposition of sedimentary organic matter, or inorganically via reduction of CO2 at high temperatures. Ongoing research has now shown that much of the methane present in sea-floor hydrothermal systems is probably formed through inorganic CO2 reduction processes at very high temperatures (greater than 400 C). Experimental results have indicated that methane might form inorganically at temperatures lower still, however these results remain controversial. Currently, methane in continental hydrothermal systems is thought to be formed mainly through the breakdown of sedimentary organic matter and carbon isotope equilibrium between CO2 and CH4 is thought to be rarely present if at all. Based on isotopic measurements of CO2 and CH4 in two continental hydrothermal systems, we suggest that carbon isotope equilibration exists at temperatures as low as 155 C. This would indicate that methane is forming through abiotic CO2 reduction at lower temperatures than previously thought and could bolster arguments for an abiotic origin of the methane detected in the martian atmosphere.

Electron localization in liquid hydrocarbons: The Anderson model

International Nuclear Information System (INIS)

Hug, Gordon L.; Mozumder, A.

2008-01-01

Anderson's model is applied for initial localization in liquid hydrocarbons (particularly n-alkanes) in conjunction with certain results of scaling theory. Medium connectivity is calculated using experimental X-ray data on liquid structure, from which critical disorder (W/V) c is computed, where W is diagonal disorder and V is the transfer energy. Actual W prevailing in the liquid is computed from anisotropic molecular polarizability. V is estimated by a heuristic procedure originating in scaling theory. These values are used to compute the percentage of initially delocalized states available for low-energy electrons in alkane liquids. This percentage decreases monotonically from methane (100%) to n-pentane and beyond (0%). In ethane and propane, the initial states are highly delocalized (97.6% and 83.9%, respectively). Subsequent trapping changes the situation as evidenced in mobility studies. Butane presents a partially, intermediate delocalized case (53.2%)

Comparison of forcefields for molecular dynamics simulations of hydrocarbon phase diagrams

Science.gov (United States)

Pisarev, V. V.; Zakharov, S. A.

2018-01-01

Molecular dynamics calculations of vapor-liquid equilibrium of methane-n-butane mixture are performed. Three force-field models are tested: the TraPPE-UA united-atom forcefield, LOPLS-AA all-atom forcefield and a fully flexible version of the TraPPE-EH all-atom forcefield. All those forcefields reproduce well the composition of liquid phase in the mixture as a function of pressure at the 300 K isotherm, while significant discrepancies from experimental data are observed in the saturated vapor compositions with OPLS-AA and TraPPE-UA forcefields. The best agreement with the experimental phase diagram is found with TraPPE-EH forcefield which accurately reproduces compositions of both liquid and vapor phase. This forcefield can be recommended for simulation of two-phase hydrocarbon systems.

The analysis of semi-volatile and non-volatile petroleum hydrocarbons in a soil/sediment matrix by capillary column gas chromatography/flame ionization detection (GC/FID)

International Nuclear Information System (INIS)

George, J.E. III; Thoma, J.J.; Hastings, M.

1990-01-01

A comprehensive analysis for semi-volatile and non-volatile fractions of petroleum hydrocarbons can be achieved by a solvent extraction/concentration techniques that will effectively extract these high molecular weight fractions from a soil matrix. The prepared extract is then injected directly into a gas chromatograph equipped with a capillary column and flame ionization detector. This technique applies to the following types of commercially available petroleum hydrocarbons: Diesel Nos. 2,4,5, and 6, fuel oils and several grades of lubrication oil. The identification of a particular petroleum hydrocarbon is determined visually by comparison of the samples with known hydrocarbon standards. Accurate quantitation of the chromatograms is possible by using peak area summation and the presence of an internal standard. The practical quantitation limit for the method is 10 mg/Kg for most fuel types. This paper presents a method for determining the concentration of these fuel types in soil. Data will be presented only on 10W40 lubrication oil in terms of method validation, calibration, percent recovery, and method detection limits. A discussion of the quatitation techniques used will also be included

Fungal degradation of coal as a pretreatment for methane production

Science.gov (United States)

Haider, Rizwan; Ghauri, Muhammad A.; SanFilipo, John R.; Jones, Elizabeth J.; Orem, William H.; Tatu, Calin A.; Akhtar, Kalsoom; Akhtar, Nasrin

2013-01-01

Coal conversion technologies can help in taking advantage of huge low rank coal reserves by converting those into alternative fuels like methane. In this regard, fungal degradation of coal can serve as a pretreatment step in order to make coal a suitable substrate for biological beneficiation. A fungal isolate MW1, identified as Penicillium chrysogenum on the basis of fungal ITS sequences, was isolated from a core sample of coal, taken from a well drilled by the US. Geological Survey in Montana, USA. The low rank coal samples, from major coal fields of Pakistan, were treated with MW1 for 7 days in the presence of 0.1% ammonium sulfate as nitrogen source and 0.1% glucose as a supplemental carbon source. Liquid extracts were analyzed through Excitation–Emission Matrix Spectroscopy (EEMS) to obtain qualitative estimates of solubilized coal; these analyses indicated the release of complex organic functionalities. In addition, GC–MS analysis of these extracts confirmed the presence of single ring aromatics, polyaromatic hydrocarbons (PAHs), aromatic nitrogen compounds and aliphatics. Subsequently, the released organics were subjected to a bioassay for the generation of methane which conferred the potential application of fungal degradation as pretreatment. Additionally, fungal-mediated degradation was also prospected for extracting some other chemical entities like humic acids from brown coals with high huminite content especially from Thar, the largest lignite reserve of Pakistan.

Reaction of methane with coal

Energy Technology Data Exchange (ETDEWEB)

Yang, K.; Batts, B.D.; Wilson, M.A.; Gorbaty, M.L.; Maa, P.S.; Long, M.A.; He, S.J.X.; Attala, M.I. [Macquarie University, Macquarie, NSW (Australia). School of Chemistry

1997-10-01

A study of the reactivities of Australian coals and one American coal with methane or methane-hydrogen mixtures, in the range 350-400{degree}C and a range of pressures (6.0-8.3 MPa, cold) is reported. The effects of aluminophosphates (AIPO) or zeolite catalysts, with and without exchanged metals, on reactivity have also been examined. Yields of dichloromethane extractable material are increased by using a methane rather than a nitrogen atmosphere and different catalysts assist dissolution to various extends. It appears that surface exchanged catalysts are effective, but incorporating metals during AIPO lattice formation is detrimental. Aluminium phosphate catalysts are unstable to water produced during coal conversion, but are still able to increase extraction yields. For the American coal, under methane-hydrogen and a copper exchanged zeolite, 51.5% conversion was obtained, with a product selectivity close to that obtained under hydrogen alone, and with only 2% hydrogen consumption. The conversion under methane-hydrogen was also to that obtained under hydrogen alone, while a linear dependence of conversion on proportion of methane would predict a 43% conversion under methane-hydrogen. This illustrates a synergistic effect of the methane-hydrogen atmosphere for coal liquefaction using this catalyst systems. 31 refs., 5 figs., 7 tabs.

Continuous methane measurements from a late Holocene Greenland ice core

DEFF Research Database (Denmark)

Rhodes, R.H.; Mitchell, L.E.; Brook, E.J.

2013-01-01

Ancient air trapped inside bubbles in ice cores can now be analysed for methane concentration utilising a laser spectrometer coupled to a continuous melter system. We present a new ultra-high resolution record of atmospheric methane variability over the last 1800yr obtained from continuous analysis...... of a shallow ice core from the North Greenland Eemian project (NEEM-2011-S1) during a 4-week laboratory-based measurement campaign. Our record faithfully replicates the form and amplitudes of multi-decadal oscillations previously observed in other ice cores and demonstrates the detailed depth resolution (5.3cm......), rapid acquisition time (30mday) and good long-term reproducibility (2.6%, 2s) of the continuous measurement technique.In addition, we report the detection of high frequency ice core methane signals of non-atmospheric origin. Firstly, measurements of air from the firn-ice transition region...

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

Non-CO2 greenhouse gas emissions associated with food production: methane (CH4) and nitrous oxide (N2O)

International Nuclear Information System (INIS)

Carlsson-Kanyama, Annika

2007-01-01

It is well known that the agriculture and livestock sectors are large contributors of N 2 O and CH 4 emissions in countries with agricultural activities and that remedial measures are needed in these sectors in order to curb contributions to global warming. This study examines non- CO 2 greenhouse gas emissions associated with the production of food. Methane (CH 4 ) and nitrous oxide (N 2 O) are the most relevant greenhouse gases in this category, and they are emitted mainly in the agricultural sector. These greenhouse gases have a Global Warming Potential much higher than CO 2 itself (25- and 298-fold higher, respectively, in a 100-year perspective). Emission intensities and the corresponding uncertainties were calculated based on the latest procedures and data published by the Intergovernmental Panel on Climate Change and used to facilitate calculations comparing greenhouse gas emissions for food products and diets. When the proposed emission intensities were applied to agricultural production, the results showed products of animal origin and the cultivation of rice under water to have high emissions compared with products of vegetable origin cultivated on upland soils, such as wheat and beans. In animal production the main source of greenhouse gas emissions was methane from enteric fermentation, while emissions of nitrous oxides from fertilisers were the main sources of greenhouse gas emissions for cereal and legume cultivation. For rice cultivation, methane emissions from flooded rice fields contributed most. Other significant sources of greenhouse gas emissions during animal production were manure storage and management. We suggest that the proposed emission factors, together with the associated uncertainties, can be a tool for better understanding the potential to mitigate emissions of greenhouse gases through changes in the diet

Multidimensional gas chromatography for the characterization of permanent gases and light hydrocarbons in catalytic cracking process.

Science.gov (United States)

Luong, J; Gras, R; Cortes, H J; Shellie, R A

2013-01-04

An integrated gas chromatographic system has been successfully developed and implemented for the measurement of oxygen, nitrogen, carbon monoxide, carbon dioxide and light hydrocarbons in one single analysis. These analytes are frequently encountered in critical industrial petrochemical and chemical processes like catalytic cracking of naphtha or diesel fuel to lighter components used in gasoline. The system employs a practical, effective configuration consisting of two three-port planar microfluidic devices in series with each other, having built-in fluidic gates, and a mid-point pressure source. The use of planar microfluidic devices offers intangible advantages like in-oven switching with no mechanical moving parts, an inert sample flow path, and a leak-free operation even with multiple thermal cycles. In this way, necessary features such as selectivity enhancement, column isolation, column back-flushing, and improved system cleanliness were realized. Porous layer open tubular capillary columns were employed for the separation of hydrocarbons followed by flame ionization detection. After separation has occurred, carbon monoxide and carbon dioxide were converted to methane with the use of a nickel-based methanizer for detection with flame ionization. Flow modulated thermal conductivity detection was employed to measure oxygen and nitrogen. Separation of all the target analytes was achieved in one single analysis of less than 12 min. Reproducibility of retention times for all compounds were found to be less than 0.1% (n=20). Reproducibility of area counts at two levels, namely 100 ppm(v) and 1000 ppm(v) over a period of two days were found to be less than 5.5% (n=20). Oxygen and nitrogen were found to be linear over a range from 20 ppm(v) to 10,000 ppm(v) with correlation coefficients of at least 0.998 and detection limits of less than 10 ppm(v). Hydrocarbons of interest were found to be linear over a range from 200 ppb(v) to 1000 ppm(v) with correlation

Photocatalytic conversion of methane to methanol