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1.
We collected sediment samples and pore water samples from the surface sediment on the Daini Atsumi Knoll, and analyzed the sediments for CH4, C2H6, and δ13CCH4, and the pore fluids for CH4, C2H6, δ13CCH4, Cl−, SO42−, δ18OH2O, and δDH2O, respectively. A comparison of the measured concentration and isotopic composition of methane in pore water samples with those in sediment samples revealed that methane was present in the sediment samples at a higher concentration and was isotopically heavier than those in the pore water samples. It suggests that the effect of the release of a sorbed gas bound to organic particles when heated prior to analysis of hydrocarbons was larger than that of the degassing process. A large amount of a sorbed gas would be a significant source of natural gas. Two striking features are the chemical and isotopic composition of the pore water samples taken from the different sites around the Daini Atsumi Knoll. In the KL09, KL10, and KP07 samples, Cl− concentrations in the pore water samples showed depletion to a minimum of 460 mmol/kg, correspond to  17% dilution of seawater, however the latter was not enriched in CH4. The isotopic compositions of pore water samples suggested the low-Cl− fluids in the pore water were not derived from dissociation of methane hydrate, but were derived from input of meteoric water. In contrast, in the KP05 samples from the north flank of the Daini Atsumi Knoll, pore water were characterized by CH4 enrichment more than 370 μmol/kg, but not depleted in Cl− concentrations. The observed methane concentration in the KP05 samples is not sufficient for methane hydrate to form in situ, indicating that the existence of methane hydrate in the surface sediment is negligible, as supported by Cl− concentration. Based on the stable carbon isotope ratio of methane in the pore fluid from the KP05 site (δ13CCH4 < − 50‰PDB), methane is thought to be of microbial origin. The pore waters in the surface sediments in the north flank of the Daini Atsumi Knoll were not directly influenced by upward fluid bearing methane of thermogenic origin from a deeper part of the sedimentary layer. However, extremely high methane concentration in the north flank site as compared with the concentration of pore water taken from the normal seafloor suggests that the north flank site is not the normal seafloor. We hypothesize that upward migration of chemically-reduced fluids from a deeper zone of the sedimentary layer reduces chemically-oxidized solutes in the surface sediment. As a consequence methane production replaced sulfate reduction as the microbial metabolism in the reduced environment of the surface sediment.  相似文献   

2.
Previous studies on the coal-bed methane potential of the Zonguldak basin have indicated that the gases are thermogenic and sourced by the coal-bearing Carboniferous units. In this earlier work, the origin of coal-bed gas was only defined according to the molecular composition of gases and to organic geochemical properties of the respective source rocks, since data on isotopic composition of gases were not available. Furthermore, in the western Black Sea region there also exist other source rocks, which may have contributed to the coal-bed gas accumulations. The aim of this study is to determine the origin of coal-bed gas and to try a gas-source rock correlation. For this purpose, the molecular and isotopic compositions of 13 headspace gases from coals and adjacent sediments of two wells in the Amasra region have been analyzed. Total organic carbon (TOC) measurements and Rock-Eval pyrolysis were performed in order to characterize the respective source rocks. Coals and sediments are bearing humic type organic matter, which have hydrogen indices (HI) of up to 300 mgHC/gTOC, indicating a certain content of liptinitic material. The stable carbon isotope ratios (δ13C) of the kerogen vary from −23.1 to −27.7‰. Air-free calculated gases contain hydrocarbons up to C5, carbon dioxide (<1%) and a considerable amount of nitrogen (up to 38%). The gaseous hydrocarbons are dominated by methane (>98%). The stable carbon isotope ratios of methane, ethane and propane are defined as δ13C1: −51.1 to −48.3‰, δ13C2: −37.9 to −25.3‰, δ13C3: −26.0 to −19.2 ‰, respectively. The δD1 values of methane range from −190 to −178‰. According to its isotopic composition, methane is a mixture, partly generated bacterially, partly thermogenic. Molecular and isotopic composition of the gases and organic geochemical properties of possible source rocks indicate that the thermogenic gas generation took place in coals and organic rich shales of the Westphalian-A Kozlu formation. The bacterial input can be related to a primary bacterial methane generation during Carboniferous and/or to a recent secondary bacterial methane generation. However, some peculiarities of respective isotope values of headspace gases can also be related to the desorption process, which took place by sampling.  相似文献   

3.
Groundwaters in the confined aquifers of the Chianan and Ilan coastal plains of Taiwan are rich in dissolved methane (CH4). Serious endemic “blackfoot disease”, which occurred in the Chianan plain, especially during AD1950-1970, has been demonstrated to have arisen from drinking highly reducing groundwater with abnormal arsenic and humic substance levels. In order to explore the origin of CH4 and its hydrological implications, stable carbon isotope ratios (δ13C) and radiocarbon (14C) ages of exsolved CH4, dissolved inorganic carbon (DIC), and sedimentary biogenic sediments from a total of 34 newly completed water wells at 16 sites were determined. The main results obtained are as follows: (1) The δ13CCH4 (−65‰ to −75‰) values indicate that, except for one thermogenic sample (δ13CCH4=38.2‰) from the Ilan plain, all CH4 samples analyzed were produced via microbially mediated CO2 reduction. Many δ13CDIC values are considerably greater than −10‰ and even up to 10‰ due to Rayleigh enrichment during CO2 reduction. (2) Almost all the 14C ages of CH4 samples from the shallow aquifer (I) (<60 m depth) are greater than the 14C ages of coexisting DIC and sediments, suggesting the presence of CH4 from underlying aquifers. (3) The 14C ages of coexisting CH4, DIC and sediments from aquifer (II) of the Chianan plain are essentially equal, reflecting in-situ generation of CH4 and DIC from decomposition of sedimentary organic matter and sluggishness of the groundwater flow. On the other hand, both CH4 and DIC from each individual well of the relatively deep aquifers (III) and (IV) in the Chianan plain are remarkably younger than the deposition of their coexisting sediments, indicating that current groundwaters entered these two aquifers much later than the deposition of aquifer sediments. (4) Each CH4 sample collected from the Ilan plain is older than coexisting DIC, which in turn is distinctly older than the deposition of respective aquifer sediments, demonstrating the presence of much older CO2 and CH4 from underlying strata.  相似文献   

4.
Gas flux measurements have for the first time been taken from vents and soil of eastern Romania mud volcanoes, the largest geological structures in Europe releasing methane into the atmosphere. In the quiescent phase, the methane emission from single vents is up to 28 t yr?1. Diffuse soil microseepage is of the order of 102?105 mg m?2 day?1. A total output of at least 1200 tonnes of CH4 per year can be conservatively estimated over the area investigated alone (～ 2.3 km2). Helium fluxes are up to five orders of magnitude higher than the average flux in a stable continental area, pointing to a close link between mud volcanoes and crustal degassing through faults crossing the deep hydrocarbon reservoirs. These data represent a key contribution towards refining global CH4‐emission estimates, which indicate mud volcanoes as a significant and unavoidable source of greenhouse gases for the atmosphere.  相似文献   

5.
Widespread mud volcanism across the thick (≤ 14 km) seismically active sedimentary prism of the Gulf of Cadiz is driven by tectonic activity along extensive strike–slip faults and thrusts associated with the accommodation of the Africa–Eurasia convergence and building of the Arc of Gibraltar, respectively. An investigation of eleven active sites located on the Moroccan Margin and in deeper waters across the wedge showed that light volatile hydrocarbon gases vented at the mud volcanoes (MVs) have distinct, mainly thermogenic, origins. Gases of higher and lower thermal maturities are mixed at Ginsburg and Mercator MVs on the Moroccan Margin, probably because high maturity gases that are trapped beneath evaporite deposits are transported upwards at the MVs and mixed with shallower, less mature, thermogenic gases during migration. At all other sites except for the westernmost Porto MV, δ13C–CH4 and δ2H–CH4 values of ~ − 50‰ and − 200‰, respectively, suggest a common origin for methane; however, the ratio of CH4/(C2H6 + C3H8) varies from ~ 10 to > 7000 between sites. Mixing of shallow biogenic and deep thermogenic gases cannot account for the observed compositions which instead result mainly from extensive migration of thermogenic gases in the deeply-buried sediments, possibly associated with biodegradation of C2+ homologues and secondary methane production at Captain Arutyunov and Carlos Ribeiro MVs. At the deep-water Bonjardim, Olenin and Carlos Ribeiro MVs, generation of C2+-enriched gases is probably promoted by high heat flux anomalies which have been measured in the western area of the wedge. At Porto MV, gases are highly enriched in CH4 having δ13C–CH4 ~ − 50‰, as at most sites, but markedly lower δ2H–CH4 values < − 250‰, suggesting that it is not generated by thermal cracking of n-alkanes but rather that it has a deep Archaeal origin. The presence of petroleum-type hydrocarbons is consistent with a thermogenic origin, and at sites where CH4 is predominant support the suggestion that gases have experienced extensive transport during which they mobilized oil from sediments ~ 2–4 km deep. These fluids then migrate into shallower, thermally immature muds, driving their mobilization and extrusion at the seafloor. At Porto MV, the limited presence of petroleum in mud breccia sediments further supports the hypothesis of a predominantly deep microbial origin of CH4.  相似文献   

6.
Vertical profiles of concentration and C-isotopic composition of dissolved methane and carbon dioxide were observed over 26 months in the catotelm of a deep (6.5 m) peat bog in Switzerland. The dissolved concentrations of these gases increase with depth while CO2 predominates over CH4 (CO2 ca. 5 times CH4). This pattern can be reproduced by a reaction-advection-ebullition model, where CO2 and CH4 are formed in a ratio of 1:1. The less soluble methane is preferentially lost via outgassing (bubbles). The isotopic fractionation between CO2 and CH4 also increases with depth, with αC values ranging from 1.045 to 1.075. The isotopic composition of the gases traces the passage of respiration-derived CO2 (from the near surface) through a shallow zone with methanogenesis of low isotopic fractionation (splitting of fermentation-derived acetate). This solution then moves through the catotelm, where methanogenesis occurs by CO2 reduction (large isotopic fractionation). In the upper part of the catotelm the C-13-depleted respiration-derived CO2 pool buffers the isotopic composition of CO2; the δ13C of CO2 increases only slowly. At the same time strongly depleted CH4 is formed as CO2 reduction consumes the depleted CO2. In the lower part of the catotelm, the respiration-derived CO2 and shallow CH4 become less important and CO2 reduction is the dominant source of CO2 and CH4. Now, the δ13C values of both gases increase until equilibrium is reached with respect to the isotopic composition of the substrate. Thus, the δ13C values of methane reach a minimum at intermediate depth, and the deep methane has δ13C values comparable to shallow methane. A simple mixing model for the isotopic evolution is suggested. Only minor changes of the observed patterns of methanogenesis (in terms of concentration and isotopic composition) occur over the seasons. The most pronounced of these is a slightly higher rate of acetate splitting in spring.  相似文献   

7.
Inorganic gases are commonly seen in eastern China and occasionally in southern China from the shallow water columns above hot and cold springs. The gases contain 68% to nearly 100% CO2, with δ13CCO2 and δ13C1 values in the range of −1.18‰ to −6.00‰ and −19.48‰ to −24.94‰, respectively. All of the 34 large inorganic CO2 and one inorganic methane accumulations discovered in China are distributed in eastern parts of the country, from both onshore and continental shelf basins. No commercial inorganic gas accumulation has been found in central and western China. This is a review of the occurrence and geochemical characteristics of inorganic gas accumulations in Chinese sedimentary basins. A detailed study of gas samples collected from four representative inorganic CO2 pools and one possible inorganic methane pool indicates that inorganic alkane gases typically show δ13C1 values greater than −10‰ versus PDB (mostly −30‰), with a positive stable carbon isotope sequence of δ13C1 < δ 13C2 < δ13C3 < δ 13C4. In contrast, the δ13C1 values of biogenic alkane gases are lighter than −30‰, with a negative isotope sequence (i.e. δ13C1 > δ13C2 > δ 13C3 > δ13C4). Inorganic gases also tend to show less negative δ13CCO2 values (−10‰) than biogenic gases (<−10‰).  相似文献   

8.
Coal-derived hydrocarbons from Middle–Lower Jurassic coal-bearing strata in northwestern China are distributed in the Tarim, Junggar, Qaidam, and Turpan-Harmi basins. The former three basins are dominated by coal-derived gas fields, distributed in Cretaceous and Tertiary strata. Turpan-Harmi basin is characterized by coal-derived oil fields which occur in the coal measures. Based on analysis of gas components and carbon isotopic compositions from these basins, three conclusions are drawn in this contribution: 1) Alkane gases with reservoirs of coal measures have no carbon isotopic reversal, whereas alkane gases with reservoirs not of coal measures the extent of carbon isotopic reversal increases with increasing maturity; 2) Coal-derived alkane gases with high δ13C values are found in the Tarim and Qaidam basins (δ13C1: − 19.0 to − 29.9‰; δ13C2: − 18.8 to − 27.1‰), and those with lowest δ13C values occur in the Turpan-Harmi and Junggar basins (δ13C1: − 40.1 to − 44.0‰; δ13C2: − 24.7 to − 27.9‰); and 3) Individual specific carbon isotopic compositions of light hydrocarbons (C5–8) in the coal-derived gases are lower than those in the oil-associated gases. The discovered carbon isotopic reversal of coal-derived gases is caused by isotopic fractionation during migration and secondary alteration. The high and low carbon isotopic values of coal-derived gases in China may have some significance on global natural gas research, especially the low carbon isotope value of methane may provide some information for early thermogenic gases. Coal-derived methane typically has much heavier δ13C than that of oil-associated methane, and this can be used for gas–source rock correlation. The heavy carbon isotope of coal-derived ethane is a common phenomenon in China and it shed lights on the discrimination of gas origin. Since most giant gas fields are of coal-derived origin, comparative studies on coal-derived and oil-associated gases have great significance on future natural gas exploration in the world.  相似文献   

9.
Atmospheric methane, a more effective heat-trapping gas than CO2 that may affect climate change, has its greatest man-made source in the US from municipal solid waste (MSW) landfills. Consequently, the wise management of landfills can reduce these greenhouse gas emissions to the atmosphere. Methane from modern MSW landfills built with composite covers is frequently vented directly to the atmosphere. Biofiltration of landfill gas could oxidize CH4 to CO2 and water. Methane oxidation in old landfills with conventional soil covers can be effective in reducing the amount of CH4 emitted. In this study, comparison of methane emissions from three different landfill covers was conducted. Methane emissions from old landfills constructed with conventional soil covers, modern MSW landfills constructed with composite covers, and modern MSW landfills constructed with composite covers plus biofilters were calculated using the calculated CH4 oxidation rates. The results showed that an average of only 14% of the generated CH4 was emitted from landfills with modern composite covers plus biofilters, and an average of 85% of the generated CH4 was emitted from landfills with conventional covers when 100% of the generated CH4 emissions to the atmosphere from landfills with modern composite covers was assumed. By comparing the CH4 emission rates from three different landfill types, the use of a properly sized biofilter should be an effective technique to reduce CH4 emissions from landfills across the USA and potentially in many other areas of the world.  相似文献   

10.
A unique dataset from paired low- and high-temperature vents at 9°50′N East Pacific Rise provides insight into the microbiological activity in low-temperature diffuse fluids. The stable carbon isotopic composition of CH4 and CO2 in 9°50′N hydrothermal fluids indicates microbial methane production, perhaps coupled with microbial methane consumption. Diffuse fluids are depleted in 13C by ∼10‰ in values of δ13C of CH4, and by ∼0.55‰ in values of δ13C of CO2, relative to the values of the high-temperature source fluid (δ13C of CH4 =−20.1 ± 1.2‰, δ13C of CO2 =−4.08 ± 0.15‰). Mixing of seawater or thermogenic sources cannot account for the depletions in 13C of both CH4 and CO2 at diffuse vents relative to adjacent high-temperature vents. The substrate utilization and 13C fractionation associated with the microbiological processes of methanogenesis and methane oxidation can explain observed steady-state CH4 and CO2 concentrations and carbon isotopic compositions. A mass-isotope numerical box model of these paired vent systems is consistent with the hypothesis that microbial methane cycling is active at diffuse vents at 9°50′N. The detectable 13C modification of fluid geochemistry by microbial metabolisms may provide a useful tool for detecting active methanogenesis.  相似文献   

11.
This study investigates the occurrence of greenhouse gases (GHGs) and the role of groundwater as an indirect pathway of GHG emissions into surface waters in a gaining stretch of the Triffoy River agricultural catchment (Belgium). To this end, nitrous oxide (N2O), methane (CH4) and carbon dioxide (CO2) concentrations, the stable isotopes of nitrate, and major ions were monitored in river and groundwater over 8 months. Results indicated that groundwater was strongly oversaturated in N2O and CO2 with respect to atmospheric equilibrium (50.1 vs. 0.55 μg L?1 for N2O and 14,569 vs. 400 ppm for CO2), but only marginally for CH4 (0.45 vs. 0.056 μg L?1), suggesting that groundwater can be a source of these GHGs to the atmosphere. Nitrification seemed to be the main process for the accumulation of N2O in groundwater. Oxic conditions prevailing in the aquifer were not prone for the accumulation of CH4. In fact, the emissions of CH4 from the river were one to two orders of magnitude higher than the inputs from groundwater, meaning that CH4 emissions from the river were due to CH4 in-situ production in riverbed or riparian zone sediments. For CO2 and N2O, average emissions from groundwater were 1.5?×?105 kg CO2 ha?1 year?1 and 207 kg N2O ha?1 year?1, respectively. Groundwater is probably an important source of N2O and CO2 in gaining streams but when the measures are scaled at catchment scale, these fluxes are probably relatively modest. Nevertheless, their quantification would better constrain nitrogen and carbon budgets in natural systems.  相似文献   

12.
The CO2 gas reservoir sandstones in the Hailaer Basin contain abundant dawsonite and provide an ideal laboratory to study whether any genetic relationship exists between dawsonite and the modern gas phase of CO2. The origins of dawsonite and CO2 in these sandstones were studied by petrographic and isotopic analysis. According to the paragenetic sequence of the sandstones, dawsonite grew later than CO2 charging at 110–85 Ma. The dawsonite δ18O value is 7.4‰ (SMOW), and the calculated δ18O values of the water present during dawsonite growth are from −11.4‰ to −9.2‰ (SMOW). This, combined with the NaHCO3-dominated water linked to dawsonite growth, suggests meteoric water being responsible for dawsonite growth. The δ13C values of gas phase CO2 and the ratios of 3He/4He of the associated He suggest a mantle magmatic origin of CO2-rich natural gas in Hailaer basin. Dawsonite δ13C values are −5.3‰ to −1.5‰ (average −3.4‰), and the calculated δ13C values of CO2 gas in isotopic equilibrium with dawsonite are −11.4‰ to −7.3‰. These C isotopic values are ambiguous for the dawsonite C source. From the geological context, the timing of events, together with formation water conditions for dawsonite growth, dawsonite possibly grew in meteoric-derived water, atmospherically-derived CO2 maybe, or at least the dominant, C source for dawsonite. It seems that there are few relationships between dawsonite and the modern gas phase of CO2 in the Hailaer basin.  相似文献   

13.
A review of the geochemistry of methane in natural gas hydrate   总被引：7，自引：0，他引：7  
The largest accumulations on Earth of natural gas are in the form of gas hydrate, found mainly offshore in outer continental margin sediment and, to a lesser extent, in polar regions commonly associated with permafrost. Measurements of hydrocarbon gas compositions and of carbon-isotopic compositions of methane from natural gas hydrate samples, collected in subaquatic settings from around the world, suggest that methane guest molecules in the water clathrate structures are mainly derived by the microbial reduction of CO2 from sedimentary organic matter. Typically, these hydrocarbon gases are composed of > 99% methane, with carbon-isotopic compositions (δ13CPDB) ranging from − 57 to − 73‰. In only two regions, the Gulf of Mexico and the Caspian Sea, has mainly thermogenic methane been found in gas hydrate. There, hydrocarbon gases have methane contents ranging from 21 to 97%, with δ13C values ranging from − 29 to − 57‰. At a few locations, where the gas hydrate contains a mixture of microbial and thermal methane, microbial methane is always dominant. Continental gas hydrate, identified in Alaska and Russia, also has hydrocarbon gases composed of > 99% methane, with carbon-isotopic compositions ranging from − 41 to − 49‰. These gas hydrate deposits also contain a mixture of microbial and thermal methane, with thermal methane likely to be dominant. Published by Elsevier Science Ltd  相似文献   

14.
Amazonian hydroelectric reservoirs produce abundant carbon dioxide and methane from large quantities of flooded biomass that decompose anaerobically underwater. Emissions are extreme the first years after impounding and progressively decrease with time. To date, only water-to-air fluxes have been considered in these estimates. Here, we investigate in two Amazonian reservoirs (Balbina and Petit Saut) the fate of above water standing dead trees, by combining a qualitative analysis of wood state and density through time and a quantitative analysis of the biomass initially flooded. Dead wood was much more decomposed in the Balbina reservoir 23 years after flooding than in the Petit Saut reservoir 10 years after flooding. Termites apparently played a major role in wood decomposition, occurring mainly above water, and resulting in a complete conversion of this carbon biomass into CO2 and CH4 at a timescale much shorter than reservoir operation. The analysis of pre-impounding wood biomass reveals that above-water decomposition in Amazonian reservoirs is a large, previously unrecognized source of carbon emissions to the atmosphere, representing 26–45% of the total reservoir flux integrated over 100 years. Accounting for both below- and above-water fluxes, we could estimate that each km2 of Amazonian forest converted to reservoir would emit over 140 Gg CO2-eq in 100 years. Hydropower plants in the Amazon should thus generate 0.25–0.4 MW h per km2 flooded area to produce lower greenhouse gas emissions than gas power plants. They also have the disadvantage to emit most of their greenhouse gases the earliest years of operation.  相似文献   

15.
Greenhouse gases and greenhouse effect   总被引：1，自引：0，他引：1  
Conventional theory of global warming states that heating of atmosphere occurs as a result of accumulation of CO2 and CH4 in atmosphere. The writers show that rising concentration of CO2 should result in the cooling of climate. The methane accumulation has no essential effect on the Earth’s climate. Even significant releases of the anthropogenic carbon dioxide into the atmosphere do not change average parameters of the Earth’s heat regime and the atmospheric greenhouse effect. Moreover, CO2 concentration increase in the atmosphere results in rising agricultural productivity and improves the conditions for reforestation. Thus, accumulation of small additional amounts of carbon dioxide and methane in the atmosphere as a result of anthropogenic activities has practically no effect on the Earth’s climate.  相似文献   

16.
Reactions of CO2 with carbonate and silicate minerals in continental sediments and upper part of the crystalline crust produce HCO3− in river and ground waters. H2SO4 formed by the oxidation of pyrite and reacting with carbonates may produce CO2 or HCO3−. The ratio, ψ, of atmospheric or soil CO2 consumed in weathering to HCO3− produced depends on the mix of CO2 and H2SO4, and the proportions of the carbonates and silicates in the source rock. An average sediment has a CO2 uptake potential of ψ = 0.61. The potential increases by inclusion of the crystalline crust in the weathering source rock. A mineral dissolution model for an average river gives ψ = 0.68 to 0.72 that is within the range of ψ = 0.63 to 0.75, reported by other investigators using other methods. These results translate into the CO2 weathering flux of 20 to 24 × 1012mol/yr.  相似文献   

17.
The Ledong gas field, consisting of three gas pools in a shale diapir structure zone, is the largest gas discovery in the Yinggehai Basin. The gases produced from the Pliocene and Quaternary marine sandstone reservoirs show a considerable variation in chemical composition, with 5.4–88% CH4, 0–93% CO2, and 1–23.7% N2. The CO2-enriched gases often display heavier methane δ13C values than those with low CO2 contents. The δ15N values of the gases range from −8 to −2‰, and the N2 content correlates negatively with the CO2 content. The high geothermal gradient associated with a relatively great burial depth in this area has led to the generation of hydrocarbon and nitrogen gases from the Lower–Middle Miocene source rocks and the formation of abundant CO2 from the Tertiary calcareous-shales and pre-Tertiary carbonates. The compositional heterogeneities and stable carbon isotope data of the produced gases indicate that the formation of the LD221 gas field is attributed to three phases of gas migration: initially biogenic gas, followed by thermogenic hydrocarbon gas, and then CO2-rich gas. The filling processes occurred within a short period approximately from 1.2 to 0.1 Ma based on the results of the kinetics modeling. Geophysical and geochemical data show that the diapiric faults that cut through Miocene sediments act as the main pathways for upward gas migration from the deep overpressured system into the shallow normal pressure reservoirs, and that the deep overpressure is the main driving force for vertical and lateral migration of the gases. This gas migration pattern implies that the transitional pressure zone around the shale diapir structures was on the pathway of upward migrating gases, and is also a favorable place for gas accumulation. The proposed multiple sources and multiple phases of gas migration and accumulation model for the Ledong gas field potentially provide useful information for the future exploration efforts in this area.  相似文献   

18.
One of the proposals for large-scale sequestration of fossil fuel-derived CO2 is deep geologic disposal in depleted oil/gas reservoirs or deep aquifers. Previously published scenarios for this inadequately proven technology have either ignored or dismissed the possibility of vertical migration of gases caused by overpressure. Overpressuring of a reservoir or aquifer will be necessary in order to have acceptable rates for dispersal of injected CO2. This research describes methodology and the results of measurement of microseepage of CO2 and CH4 at a large-scale CO2-enhanced oil recovery (EOR) operation at Rangely, Colorado, USA. Shallow and deep soil gas concentrations, and direct transport of CO2 and CH4 into the atmosphere were measured. The interpretation of the measurements was complemented by both stable and radiogenic isotopic measurements of C. The results have demonstrated an estimated microseepage to the atmosphere of approximately 400 metric tonnes of CH4/a from the 78 km2 area of the Rangely field. Preliminary estimates of deep-sourced CO2 losses are <3800 tonnes/a, based on stable isotope measurements of soil gases. Several holes up to 10 m deep were drilled on, and off the field for nested gas sampling of composition and stable C isotopic ratios for CO2 and CH4. Carbon-14 measurements on CO2 from these holes indicate that deep-sourced CO2 microseepage losses were approximately 170 tonnes/a.  相似文献   

19.
The Huntly coalfield has significant coal deposits that contain biogenically-sourced methane. The coals are subbituminous in rank and Eocene in age and have been previously characterised with relatively low to moderate measured gas (CH4) contents (2–4 m3/ton). The CO2 holding capacity is relatively high (18.0 m3/ton) compared with that of CH4 (2.6 m3/ton) and N2 (0.7 m3/ton) at the same pressure (4 MPa; all as received basis). The geothermal gradient is also quite high at 55 °C/km.A study has been conducted which simulates enhancement of methane recovery (ECBM) from these deposits using a new version of the TOUGH2 (version 2) reservoir simulator (ECBM-TOUGH2) that can handle non-isothermal, multi-phase flows of mixtures of water, CH4, CO2 and N2. The initial phase of the simulation is CH4 production for the first 5 years of the field history. The model indicates that methane production can be significantly improved (from less than 80% recovery to nearly 90%) through injection of CO2. However, although an increase in the rate of CO2 injection increases the amount of CO2 sequestered, the methane recovery (because of earlier breakthrough with increasing injection rate) decreases. Modeling of pure N2 injection produced little enhanced CH4 production. The injection of a hypothetical flue gas mixture (CO2 and N2) also produced little increase in CH4 production. This is related to the low adsorption capacity of the Huntly coal to N2 which results in almost instantaneous breakthrough into the production well.  相似文献   

20.
A series of laboratory experiments were performed to investigate the relative contributions of CO and other single-carbon compounds to abiotic synthesis of organic compounds in hydrothermal environments. Experiments were conducted by heating aqueous solutions of CO, CO2, HCOOH, or CH4 at 250 °C under reducing conditions, and observing production of CH4 and other hydrocarbons. Native Fe was included in the experiments as a source of H2 through reaction with water and as a potential catalyst. Experiments with CO or HCOOH as the carbon source resulted in rapid generation of CH4 and other hydrocarbons that closely resembled typical products of Fischer-Tropsch organic synthesis. In contrast, experiments using CO2 or CH4 as the carbon source yielded no detectable hydrocarbon products. Carbon isotope measurements of reaction products from the CO experiments indicate that the CH4 and other hydrocarbons were substantially depleted in 13C, with CH4 δ13C values 30 to 34‰ lighter than the initial CO. Most of the fractionation apparently occurs during attachment of CO to the catalyst surface and subsequent reduction to surface-bound methylene. The initial step in polymerization of these methylene units to form hydrocarbons involves a small, positive fractionation, so that ethane and ethene are slightly enriched in 13C relative to CH4. However, subsequent addition of carbon molecules to the growing hydrocarbon chain proceeds with no net observable fractionation, so that the isotopic compositions of the C3+ light hydrocarbons are controlled by isotopic mass balance. This result is consistent with a previously proposed model for carbon isotopic patterns of light hydrocarbons in natural samples. The abundance and isotopic composition of light hydrocarbons produced with HCOOH as the carbon source were similar to those generated with CO, but the isotopic compositions of non-volatile hydrocarbons diverged, suggesting that the higher hydrocarbons were formed by different mechanisms in the CO and HCOOH experiments. The experiments indicate that CO, and possibly HCOOH, may be critical intermediates in the abiotic formation of organic compounds in geologic environments, and suggest that the low levels of these compounds present in most hydrothermal systems could represent a bottleneck restricting the extent of abiotic organic synthesis in some circumstances.  相似文献   

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