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1.
The San Juan Basin natural gas field, located in northwestern New Mexico and southwestern Colorado in the USA, is a case-type coalbed methane system. Groundwater is thought to play a key role in both biogenic methane generation and the CO2 sequestration potential of coalbed systems. We show here how noble gases can be used to construct a physical model that describes the interaction between the groundwater system and the produced gas. We collected 28 gas samples from producing wells in the artesian overpressured high production region of the basin together with 8 gas samples from the underpressured low production zone as a control. Stable isotope and major species determination clearly characterize the gas in the high production region as dominantly biogenic in origin, and the underpressured low producing region as having a significant admix of thermogenic coal gas. 3He/4He ratios increase from 0.0836Ra at the basin margin to 0.318Ra towards the center, indicating a clear but small mantle He signature in all gases. Coherent fractionation of water-derived 20Ne/36Ar and crustal 4He/40Ar* are explained by a simple Rayleigh fractionation model of open system groundwater degassing. Low 20Ne concentrations compared to the model predicted values are accounted for by dilution of the groundwater-associated gas by desorbed coalbed methane. This Rayleigh fractionation and dilution model together with the gas production history allows us to quantify the amount of water involved in gas production at each well. The quantified water volumes in both underpressured and overpressured zones range from 1.7 × 103 m3 to 4.2 × 105 m3, with no clear distinction between over- and underpressured production zones. These results conclusively show that the volume of groundwater seen by coal does not play a role in determining the volume of methane produced by secondary biodegradation of these coalbeds. There is no requirement of continuous groundwater flow for renewing the microbes or nutrient components. We furthermore observe strong mass related isotopic fractionation of 20Ne/22Ne and 38Ar/36Ar isotopic ratios. This can be explained by a noble gas concentration gradient in the groundwater during gas production, which causes diffusive partial re-equilibration of the noble gas isotopes. It is important for the study of other systems in which extensive groundwater degassing may have occurred to recognize that severe isotopic fractionation of air-derived noble gases can occur when such concentration gradients are established during gas production. Excess air-derived Xe and Kr in our samples are shown to be related to the diluting coalbed methane and can only be accounted for if Xe and Kr are preferentially and volumetrically trapped within the coal matrix and released during biodegradation to form CH4.  相似文献   

2.
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   

3.
A pockmark field extending over 35 km2 at 74°54N, 27°3E, described by Solheim and Elverhøi (1993), was re-surveyed and found to be covered with more than 30 steep-sided craters between 300 and 700 m in diameter and up to 28 m deep. The craters are thought to have been formed by an explosive gas eruption. Anomalously high concentrations of methane in the shelf waters around the craters suggest that a strong methane source near this area is still active today. Methane enrichment more than 10 km away from the crater field indicates the large dimensions of a plume and the amount of gas released from sources below the seafloor of the Barents Sea shelf. From the characteristic vertical decrease of methane towards the sea surface, it is concluded that biota are extensively using this energy pool and reducing the methane concentration within the water column by about 98% between 300 m depth and the sea surface. Degassing to the atmosphere is minimal based on the shape of the methane concentration gradient. Nevertheless, the net flux of methane from this area of the Barents Sea is about 2.9 × 104 g CH4 km–2 yr–1 and thus in the upper range of the presently estimated global marine methane release. This flux is a minimum estimate and is likely to increase seasonally when rough weather leads to more effective vertical mixing during autumn and winter. The amount of methane consumed in the water column, however, is about 50 times greater and hence should significantly contribute to the marine carbon inventory.  相似文献   

4.
This study provides new estimates for the global offshore methane hydrate inventory formed due to microbial CH4 production under Quaternary and Holocene boundary conditions. A multi-1D model for particular organic carbon (POC) degradation, gas hydrate formation and dissolution is presented. The novel reaction-transport model contains an open three-phase system of two solid compounds (organic carbon, gas hydrates), three dissolved species (methane, sulfates, inorganic carbon) and one gaseous phase (free methane). The model computes time-resolved concentration profiles for all compounds by accounting for chemical reactions as well as diffusive and advective transport processes. The reaction module builds upon a new kinetic model of POC degradation which considers a down-core decrease in reactivity of organic matter. Various chemical reactions such as organic carbon decay, anaerobic oxidation of methane, methanogenesis, and sulfate reduction are resolved using appropriate kinetic rate laws and constants. Gas hydrates and free gas form if the concentration of dissolved methane exceeds the pressure, temperature, and salinity-dependent solubility limits of hydrates and/or free gas, with a rate given by kinetic parameters. Global input grids have been compiled from a variety of oceanographic, geological and geophysical data sets including a new parameterization of sedimentation rates in terms of water depth.We find prominent gas hydrate provinces offshore Central America where sediments are rich in organic carbon and in the Arctic Ocean where low bottom water temperatures stabilize methane hydrates. The world’s total gas hydrate inventory is estimated at (at STP conditions) or, equivalently, 4.18-995 Gt of methane carbon. The first value refers to present day conditions estimated using the relatively low Holocene sedimentation rates; the second value corresponds to a scenario of higher Quaternary sedimentation rates along continental margins.Our results clearly show that in-situ POC degradation is at present not an efficient hydrate forming process. Significant hydrate deposits in marine settings are more likely to have formed at times of higher sedimentation during the Quaternary or as a consequence of upward fluid transport at continental margins.  相似文献   

5.
Enhanced coalbed methane (ECBM) involves the injection of a gas, such as nitrogen or carbon dioxide, into the coal reservoir to displace the methane present. Potentially this strategy can offer greater recovery of the coal seam methane and higher rates of recovery due to pressure maintenance of the reservoir. While reservoir simulation forms an important part of the planning and assessment of ECBM, a key question is the accuracy of existing approaches to characterising and representing the gas migration process. Laboratory core flooding allows the gas displacement process to be investigated on intact coal core samples under conditions analogous to those in the reservoir. In this paper a series of enhanced drainage core floods are presented and history matched using an established coal seam gas reservoir simulator, SIMED II. The core floods were performed at two pore pressures, 2 MPa and 10 MPa, and involve either nitrogen or flue gas (90% nitrogen and 10% CO2) flooding of core samples initially saturated with methane. At the end of the nitrogen floods the core flood was reversed by flooding with methane to investigate the potential for hysteresis in the gas displacement process. Prior to the core flooding an independent characterisation programme was performed on the core sample where the adsorption isotherm, swelling with gas adsorption, cleat compressibility and geomechanical properties were measured. This information was used in the history matching of the core floods; the properties adjusted in the history matching were related to the affect of sorption strain on coal permeability and the transfer of gas between cleat and matrix. Excellent agreement was obtained between simulated and observed gas rates, breakthrough times and total mass balances for the nitrogen/methane floods. It was found that a triple porosity model improved the agreement with observed gas migration over the standard dual porosity Warren-Root model. The Connell, Lu and Pan hydrostatic permeability model was used in the simulations and improved history match results by representing the contrast between pore and bulk sorption strains for the 10 MPa cases but this effect was not apparent for the 2 MPa cases. There were significant differences between the simulations and observations for CO2 flow rates and mass balances for the flue gas core floods. A possible explanation for these results could be that there may be inaccuracy in the representation of mixed gas adsorption using the extended Langmuir adsorption model.  相似文献   

6.
This paper reports on the performance comparison for different CO2-ECBM schemes in relatively thin unminable seams typical of Northern Appalachian coal basin using a horizontal well configuration. Numerical simulations based upon public-domain coalbed reservoir properties indicated that injection of pure CO2 is likely to result in only limited incremental methane recovery if any over primary recovery, due to the low injection rates that can be achieved. On the other hand, the presence of the nitrogen component in the injected gas stream is capable of improving the efficiency of enhanced methane recovery significantly without compromising the net CO2 injection rates, as a result of improved injectivity over pure CO2 injection. There is, however, a trade off between incremental methane recovery and produced gas purity due to early nitrogen breakthrough.  相似文献   

7.
Around half of world’s endowment of in-place oil and bitumen experienced biodegradation, which is now believed to be largely an anaerobic methanogenic process. However, the distribution and scale of methanogenic biodegradation in the world’s petroleum accumulations and the significance of its terminal product, secondary microbial methane, in the global gas endowment and carbon cycle are largely unknown. Here, I present geological and geochemical criteria to recognize secondary microbial methane in conventional petroleum reservoirs. These include the presence of biodegraded oil (as pools, legs or shows) in the reservoir or down-dip, the relatively dry (methane dominated) gas containing methane with δ13C values between −55‰ and −35‰ and, most importantly, CO2 with δ13C > +2‰. Based on these criteria, the presence of secondary microbial methane is apparent in 22 basins, probable in 12 basins and possible in six basins worldwide. Reservoirs apparently containing secondary microbial methane are mostly Cenozoic and clastic and occur at depths of 37-1834 m below surface/mudline and temperatures of 12-71 °C. Using the current global endowment of in-place oil and bitumen and reasonable assumptions about conversion of oil into methane during biodegradation, I estimated that ∼65,500 tcf of secondary microbial methane could have been generated in existing worldwide accumulations of oil and bitumen through their geological history. From 1461-2760 tcf in-place (845-1644 tcf recoverable) of secondary microbial methane may be accumulated as free and oil-dissolved gas in petroleum reservoirs. I also updated the inventory of primary microbial methane and estimated that the global primary microbial gas endowment (free and oil-dissolved) is from 676-797 tcf in-place (407-589 tcf recoverable). Secondary microbial methane may account for ∼5-11% of the global conventional recoverable gas endowment and appears more abundant than primary microbial gas (∼3-4% of the global gas endowment). Most of the generated secondary microbial methane probably is aerobically and anaerobically oxidized to CO2 in the overburden above petroleum reservoirs. However, some secondary microbial methane may escape from shallow reservoirs into the atmosphere and affect present and past global climate.  相似文献   

8.
The component and carbon isotope compositions were studied in the hydrocabon gases from sediments of the underwater high Posolskaya Bank (Lake Baikal). It was established that sediments of this Baikal area contain methane of microbial (C1/C2 >16000; δ13C 70 ± 3‰) and thermocatalytic (C1/C2 <100; δ13C–46 ± 3‰) origin. Some samples represent a gas mixture of thermocatalytic and microbial origin. This gas is characterized by δ13C of methane varying from–60 to–70‰ and contains a significant amount of ethane. The main homolog of methane in the thermocatalytic and mixed gas is ethane. Owing to biodegradation, propane and butanes are present in trace amounts.  相似文献   

9.
The sensitivity of coal permeability to the effective stress means that changes in stress as well as pore pressure within a coal seam lead to changes in permeability. In addition coal swells with gas adsorption and shrinks with desorption; these sorption strains impact on the coal stress state and thus the permeability. Therefore the consideration of gas migration in coal requires an appreciation of the coupled geomechanical behaviour. A number of approaches to representing coal permeability incorporate the geomechanical response and have found widespread use in reservoir simulation. However these approaches are based on two simplifying assumptions; uniaxial strain (i.e. zero strain in the horizontal plane) and constant vertical stress. This paper investigates the accuracy of these assumptions for reservoir simulation of enhanced coalbed methane through CO2 sequestration. A coupled simulation approach is used where the coalbed methane simulator SIMED II is coupled with the geomechanical model FLAC3D. This model is applied to three simulation case studies assembled from information presented in the literature. Two of these are for 100% CO2 injection, while the final example is where a flue gas (12.5% CO2 and 87.5% N2) is injected. It was found that the horizontal contrast in sorption strain within the coal seam caused by spatial differences in the total gas content leads to vertical stress variation. Thus the permeability calculated from the coupled simulation and that using an existing coal permeability model, the Shi–Durucan model, are significantly different; for the region in the vicinity of the production well the coupled permeability is greater than the Shi–Durucan model. In the vicinity of the injection well the permeability is less than that calculated using the Shi–Durucan model. This response is a function of the magnitude of the strain contrast within the seam and dissipates as these contrasts diminish.  相似文献   

10.
Rising methane gas bubbles form massive hydrate layers at the seafloor   总被引：3，自引：0，他引：3  
Extensive methane hydrate layers are formed in the near-surface sediments of the Cascadia margin. An undissociated section of such a layer was recovered at the base of a gravity core (i.e. at a sediment depth of 120 cm) at the southern summit of Hydrate Ridge. As a result of salt exclusion during methane hydrate formation, the associated pore waters show a highly elevated chloride concentration of 809 mM. In comparison, the average background value is 543 mM.A simple transport-reaction model was developed to reproduce the Cl− observations and quantify processes such as hydrate formation, methane demand, and fluid flow. From this first field observation of a positive Cl− anomaly, high hydrate formation rates (0.15-1.08 mol cm−2 a−1) were calculated. Our model results also suggest that the fluid flow rate at the Cascadia accretionary margin is constrained to 45-300 cm a−1. The amount of methane needed to build up enough methane hydrate to produce the observed chloride enrichment exceeds the methane solubility in pore water. Thus, most of the gas hydrate was most likely formed from ascending methane gas bubbles rather than solely from CH4 dissolved in the pore water.  相似文献   

11.
An existing method of detecting microgas seeps was applied in a free soil gas investigation above the Löningen oilfield, NW-Germany. Simple gas surveying was combined with sampling of soil gases for gas-chromatographic treatment and examination of the carbon isotopic composition. A zone of biological gas formation and an area of thermocatalytic methane were discovered, the latter probably caused by migration from the subsurface petroleum accumulation.The methane in the reservoir differs in isotopic composition depending on its origin: gas from gascap or petroleum. Methane dissolved from petroleum is depleted in 12C by about 5 ppt compared to methane from the gascap. In relation to the reservoir a general 13C-enrichment between 2.5 and 4.6 ppt is observed in the soil gas methanes which is supposedly due to isotopic fractionation during migration. The two species of reservoir methane are still distinguishable on the surface by their different composition. Gaseous hydrocarbons from C2 to C4 seem to be restricted by migration. Bacterial oxidation appears not to affect the isotopic composition of the thermocatalytic methane seriously.  相似文献   

12.
Methane emissions and oxidation were measured during the wet and dry seasons at the Air Hitam, Jeram, and Sungai Sedu landfills in Malaysia. The resulting levels of methane emissions and oxidation were then modeled using the Inter-governmental Panel on Climate Change 1996 first order decay (FOD) model to obtain methane generation rate and potential values. Emissions measurements were performed using a fabricated static flux chamber. A combination of gas concentrations in soil profiles and surface methane and carbon dioxide emissions at four monitoring locations in each landfill was used to estimate the methane oxidation capacity. The methane potential value was 151.7 m3 t?1 for the Air Hitam and Jeram sanitary landfills and 75.9 m3 t?1 for the Sungai Sedu open dumping landfill. The methane generation rate value of the Jeram and Air Hitam sanitary landfills during the wet season was 0.136 year?1, while that of Jeram during the dry season was 0.072 year?1. The methane generation rate values of the Sungai Sedu open dumping landfill during the wet and dry seasons were 0.008 and 0.0049 year?1, respectively. The observed values of methane generation rate and potential assist to accurately estimate total methane emissions from Malaysian landfills using the Inter-governmental Panel on Climate Change FOD model.  相似文献   

13.
天然气水合物气候效应研究进展   总被引：2，自引：1，他引：1  
天然气水合物富含温室气体甲烷,且资源量巨大,对气候变化又十分敏感,在全球变暖的背景下其气候效应倍受关注,近年来的研究工作又取得了一些新进展.首先,天然气水合物资源量的估算进一步精确,海洋中天然气水合物资源量的最新估算值仅为原先的1/5,从根本上限制了其气候效应的显著性;其次,大气中来自天然气水合物的甲烷通量被重新评估,...  相似文献   

14.
《Chemical Geology》1992,94(4):315-319
In order to estimate the isotope fractionation effect between coals and methane during coalification a maturity-related fractionation model has been developed for coals and reservoir gases of NW Germany which is based on empirical data. Assuming that observed isotope shifts of the convertible carbon of coals of different maturities are related to a loss of methane during coalification and that this shift can be described by a Rayleigh distillation process, functions with preselected fractionation factors were fitted to measured isotope data of the convertible carbon of coals. The best approximation of theoretical and measured data was achieved with a low fractionation factor (αc= 1.003). Using this model theoretical methane carbon isotope data were determined and compared to the isotopic composition of reservoir methanes of NW Germany. Although the methane isotope data of reservoir gases and the related maturity of the coals show a slight scatter, the theoretical data plot within the same range and follow the increase of the 13C concentration of reservoir gases with increasing maturity of the coals.  相似文献   

15.
甲烷水合物生成过程中海水常量离子浓度的变化规律   总被引：3，自引：2，他引：1  
本文自行研制了一套甲烷水合物合成装置,模拟海洋环境甲烷水合物的生成过程,对该过程水合物生成位置、形态、反应时间、环境温压条件进行观测,同时连续测试体系海水中常量离子K+、Na+、Ca2+、Mg2+、C1-、SO42-的浓度及海水盐度,探讨水合物生成过程的温压变化及离子浓度变化之间的关系和离子浓度的变化规律.结果表明,海水中甲烷水合物生成具有很大的随机性,在相同的初始条件下可能有不同的水合物成核、聚集过程;甲烷水合物在生成过程中,耗气量不断增加,孔隙水的盐度和海水中常量阴阳离子的浓度也在不断增加,这种变化具有较高的线性相关性(相关系数为0.9848～0.9950),且不受甲烷水合物生成位置及状态的影响;在水合物生成过程的微环境下耗气量相同时,离子浓度存在细微的差异.这些特征为通过测定海底水合物周围孔隙水中常量离子的浓度初步推算水合物的甲烷耗气量提供了依据.  相似文献   

16.
Seafloor methane emission from the Quepos Slide on the submarine segment of the Costa Rica fore-arc margin was estimated by extrapolating flux measurements from individual seeps to the total area covered by bacterial mats. This approach is based on the combination of detailed mapping to determine the abundance of seeps and the application of a numerical model to estimate the amount of benthic methane fluxes. Model results suggest that the majority of the studied seeps transport rather limited amount of methane (on average: ~177 μmol cm?2 a?1) into the water column due to moderate upward advection, allowing for intense anaerobic oxidation of methane (AOM; on average: 53 % of the methane flux is consumed). Depth-integrated AOM rates (56–1,538 μmol CH4 cm?2 a?1) are comparable with values reported from other active seep sites. The overall amount of dissolved methane released into the water column from the entire area covered by bacterial mats on the Quepos Slide is estimated to be about 0.28 × 106 mol a?1. This conservative estimate which relies on rather accurate determinations of seafloor methane fluxes emphasizes the potential importance of submarine slides as sites of natural methane seepage; however, at present the global extent of methane seepage from submarine slides is largely unknown.  相似文献   

17.
It is a typical multiphase flow process for hydrate formation in seeping seafloor sediments. Free gas can not only be present but also take part in formation of hydrate. The volume fraction of free gas in local pore of hydrate stable zone (HSZ) influences the formation of hydrate in seeping seafloor area, and methane flux determines the abundance and resource of hydrate-bearing reservoirs. In this paper, a multiphase flow model including water (dissolved methane and salt)-free gas hydrate has been established to describe this kind of flow-transfer-reaction process where there exists a large scale of free gas migration and transform in seafloor pore. In the order of three different scenarios, the conversions among permeability, capillary pressure, phase saturations and salinity along with the formation of hydrate have been deducted. Furthermore, the influence of four sorts of free gas saturations and three classes of methane fluxes on hydrate formation and the resource has also been analyzed and compared. Based on the rules drawn from the simulation, and combined information gotten from drills in field, the methane hydrate(MH) formation in Shenhu area of South China Sea has been forecasted. It has been speculated that there may breed a moderate methane flux below this seafloor HSZ. If the flux is about 0.5 kg m−2 a−1, then it will go on to evolve about 2700 ka until the hydrate saturation in pore will arrive its peak (about 75%). Approximately 1.47 × 109 m3 MH has been reckoned in this marine basin finally, is about 13 times over preliminary estimate.  相似文献   

18.
Formation of the Carbon-13 (13C) and deuterium (D) doubly-substituted methane isotopologues (13CH3D) in natural gases is studied utilizing both first-principle quantum mechanism molecular calculation and direct FTIR laboratorial measurements of specifically synthesized high isotope concentration methane gas. For 13CH3D, the symmetrically breathing mode A0 emerges as IR-detectable attributed to the molecular symmetry lowering to C3v from Td of the non-isotopic methane (CH4), along with a large vibrational frequency shift from ∼3000 to ∼2250 cm−1. Our studies also indicate that the concentration of 13CH3D is dependent on the environmental temperature through isotope exchanges among methane isotopologues; and the Gibbs’ Free Energy difference due to Quantum Mechanics Zero-Point vibrational motions has the major contribution to this temperature dependency. Potential geologic applications of the 13CH3D measurement to natural gas exploration and assessments are also discussed. In order to detect the 13CH3D concentration change of each 50 °C in the natural gas system, a 10−9 resolution is desirable. Such a measurement could provide important add-on information to distinguish natural gas origin and distribution.  相似文献   

19.
A detailed model is presented of methane photochemistry in the primitive terrestrial atmosphere along with speculation about its interpretation. Steady-state CH4 mixing ratios of 10−6–10−4 could have been maintained by a methane source of about 1011 cm−2 s−1, which is comparable to the modern biogenic methane production rate. In the absence of a source, methane would have disappeared in <104 years, being either oxidized, or polymerized into more complex hydrocarbons. The source strength needed to maintain a steady CH4 mixing ratio and the degree to which methane could have polymerized to form higher hydrocarbons depend upon the amount of CO2 present in the early atmosphere. The dependence on H2 is much weaker. Infrared absorption by methane, and especially by other hydrocarbon species, may have supplemented the greenhouse warming due to carbon dioxide. A radiative model is needed to establish this effect quantitatively. The destruction of the methane greenhouse early in the Proterozoic may have triggered the Huronian glaciation.These calculations also suggest that atmospheres rich in both CO2 and CH4 may be photochemically unstable with respect to conversion to CO.  相似文献   

20.
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   

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