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1.
Methane and CO2 emissions from the two most active mud volcanoes in central Japan, Murono and Kamou (Tokamachi City, Niigata Basin), were measured in from both craters or vents (macro-seepage) and invisible exhalation from the soil (mini- and microseepage). Molecular and isotopic compositions of the released gases were also determined. Gas is thermogenic (δ13CCH4 from −32.9‰ to −36.2‰), likely associated with oil, and enrichments of 13C in CO2 (δ13CCO2 up to +28.3‰) and propane (δ13CC3H8 up to −8.6‰) suggest subsurface petroleum biodegradation. Gas source and post-genetic alteration processes did not change from 2004 to 2010. Methane flux ranged within the orders of magnitude of 101-104 g m−2 d−1 in macro-seeps, and up to 446 g m−2 d−1 from diffuse seepage. Positive CH4 fluxes from dry soil were widespread throughout the investigated areas. Total CH4 emission from Murono and Kamou were estimated to be at least 20 and 3.7 ton a−1, respectively, of which more than half was from invisible seepage surrounding the mud volcano vents. At the macro-seeps, CO2 fluxes were directly proportional to CH4 fluxes, and the volumetric ratios between CH4 flux and CO2 flux were similar to the compositional CH4/CO2 volume ratio. Macro-seep flux data, in addition to those of other 13 mud volcanoes, supported the hypothesis that molecular fractionation (increase of the “Bernard ratio” C1/(C2 + C3)) is inversely proportional to gas migration fluxes. The CH4 “emission factor” (total measured output divided by investigated seepage area) was similar to that derived in other mud volcanoes of the same size and activity. The updated global “emission-factor” data-set, now including 27 mud volcanoes from different countries, suggests that previous estimates of global CH4 emission from mud volcanoes may be significantly underestimated.  相似文献   

2.
Mud volcanoes are important pathways for CH4 emission from deep buried sediments; however, the importance of gas fluxes have hitherto been neglected in atmospheric source budget considerations. In this study, gas fluxes have been monitored to examine the stability of their chemical compositions and fluxes spatially, and stable C isotopic ratios of CH4 were determined, for several mud volcanoes on land in Taiwan. The major gas components are CH4 (>90%), “air” (i.e. N2 + O2 + Ar, 1–5%) and CO2 (1–5%) and these associated gas fluxes varied slightly at different mud volcanoes in southwestern Taiwan. The Hsiao-kun-shui (HKS) mud volcano emits the highest CH4 concentration (CH4 > 97%). On the other hand, the Chung-lun mud volcano (CL) shows CO2 up to 85%, and much lower CH4 content (<37%). High CH4 content (>90%) with low CO2 (<0.2%) are detected in the mud volcano gases collected in eastern Taiwan. It is suggestive that these gases are mostly of thermogenic origin based on C1 (methane)/C2 (ethane) + C3 (propane) and δ13CCH4 results, with the exception of mud volcanoes situated along the Gu-ting-keng (GTK) anticline axis showing unique biogenic characteristics. Only small CH4 concentration variations, <2%, were detected in four on-site short term field-monitoring experiments, at Yue-shi-jie A, B, Kun-shui-ping and Lo-shan A. Preliminary estimation of CH4 emission fluxes for mud volcanoes on land in Taiwan fall in a range between 980 and 2010 tons annually. If soil diffusion were taken into account, the total amount of mud volcano CH4 could contribute up to 10% of total natural CH4 emissions in Taiwan.  相似文献   

3.
Composition and exhalation flux of gases from mud volcanoes in Taiwan   总被引：3，自引：0，他引：3  
Many mud volcanoes are distributed along the tectonic sutures in southern Taiwan and can be divided into five zones based on their relative positions in different tectonic domains. Most active mud volcanoes are exhaling methane-dominated gases. Nevertheless, some gases show unusual carbon dioxide-dominated and/or nitrogen-excess compositions. This implies that there are multiple sources for the gas compositions of mud volcanoes in Taiwan.For better understanding the total amount of exhalation gases and its flux, the gas flow and compositions were continuously measured in the interval of two minutes at Chung-lun (CL) bubbling mud pool for a few months. The major compositions of gases exhaling from this site were 75~90% of CO2 and 5~12% of CH4. The amount of gases exhaling from the mud pool can be estimated to be about 1.4 ton/year for CH4 and 28 ton/year for CO2, respectively. The preliminary results of exhaling gas flux from the major vents of representative active mud volcanoes, yielded an estimated total CH4 output of the mud volcanoes in Taiwan of ca. 29 ton/year during quiescent period.  相似文献   

4.
Data are presented on the molecular composition of drill-mud gas from the lower sedimentary section (1800–3987 m) of the SAFOD (San Andreas Fault Observatory at Depth) Main Hole measured on-line during drilling, as well as C and H isotope data from off-line mud gas samples. Hydrocarbons, H2 and CO2 are the most abundant non-atmospheric gases in drill-mud when drilling seismogenic zones. Gas influx into the well at depth is related to the lithology and permeability of the drilled strata: larger formation gas influx was detected when drilling through organic-rich shales and permeable sandstones. The SAF (San Andreas Fault), encountered between approximately 3100 m and 3450 m borehole depth, is generally low in gas, but is encompassed by two gas-rich zones (2700–2900 m and below 3550 m) at the fault margins with enhanced 222Rn activities and distinct gas compositions. Within the fault, two interstratified gas-rich lenses (3150–3200 m and 3310–3340 m) consist of CO2 and hydrocarbons (upper zone), but almost exclusively of hydrocarbons (lower zone).  相似文献   

5.
The South Caspian sedimentary basin is a unique area with thick Mesozoic-Cenozoic sediments (up to 30–32 km) characterized by an extremely high fluid generation potential. The large amount of active mud volcanoes and the volumes of their gas emissions prove the vast scale of fluid generation. Onshore and offshore mud volcanoes annually erupt more than 109 cubic meters of gases consisting of CH4 (79–98%), and a small admixture of C2H6, C3H8, C4H10, C5H12, CO2, N, H2S, Ar, He. Mud volcanism is closely connected to the processes occurring in the South Caspian depression, its seismicity, fluctuations of the Caspian Sea level, solar activity and hydrocarbon generation.The large accumulations of gas hydrates are confined to the bottom sediments of the Caspian Sea, mud volcanoes crater fields (interval 0–0.4 m, sea depth 480 m) and to the volcanoes body at the depth of 480–800 from the sea bottom. Resources of HC gases in hydrates saturated sediments up to a depth of 100 m and are estimated at 0.2×1015–8×1015 m3. The amount of HC gases concentrated in them is 1011–1012 m3.The Caspian Sea, being an inland closed basin is very sensitive to climatic and tectonic events expressed in sea level fluctuations. During regressive stages as a result of sea level fall and the reducing of hydrostatic pressure the decomposition of gas hydrates and the releasing of a great volume of HC gases consisting mainly of methane are observed.From the data of deep drilling, seismoacoustics, and deep seismic mud volcanic activity in the South Caspian Basin started in the Lower Miocene. Activity reached its highest intensity at the boundary between the Miocene and Pliocene and was associated with dramatic Caspian Sea level fall in the Lower Pliocene of up to 600 m, which led to the isolation of the PaleoCaspian from the Eastern ParaTethys. Catastrophic reduction of PaleoCaspian size combined with the increasing scale of mud volcanic activity caused the oversaturation and intoxication of water by methane and led to the mass extinction of mollusks, fishes and other groups of sea inhabitants. In the Upper Pliocene and Quaternary mud volcanism occurred under the conditions of a semi-closed sea periodically connected with the Pontian and Mediterranean Basins. Those stages of Caspian Sea history are characterized by the revival of the Caspian organic world.Monitoring of mud volcanoes onshore of the South Caspian demonstrated that any eruption is predicted by seismic activation in the region (South-Eastern Caucasus) and intensive fluid dynamics on the volcanoes.  相似文献   

6.
Microbial methane turnover at mud volcanoes of the Gulf of Cadiz   总被引：2，自引：0，他引：2  
The Gulf of Cadiz is a tectonically active area of the European continental margin and characterised by a high abundance of mud volcanoes, diapirs, pockmarks and carbonate chimneys. During the R/V SONNE expedition “GAP-Gibraltar Arc Processes (SO-175)” in December 2003, several mud volcanoes were surveyed for gas seepage and associated microbial methane turnover. Pore water analyses and methane oxidation measurements on sediment cores recovered from the centres of the mud volcanoes Captain Arutyunov, Bonjardim, Ginsburg, Gemini and a newly discovered, mud volcano-like structure called “No Name” show that thermogenic methane and associated higher hydrocarbons rising from deeper sediment strata are completely consumed within the seabed. The presence of a distinct sulphate-methane transition zone (SMT) overlapping with high sulphide concentrations suggests that methane oxidation is mediated under anaerobic conditions with sulphate as the electron acceptor. Anaerobic oxidation of methane (AOM) and sulphate reduction (SR) rates show maxima at the SMT, which was found between 20 and 200 cm below seafloor at the different mud volcanoes. In comparison to other methane seeps, AOM activity (<383 mmol m−2 year−1) and diffusive methane fluxes (<321 mmol m−2 year−1) in mud volcano sediments of the Gulf of Cadiz are low to mid range. Corresponding lipid biomarker and 16S rDNA clone library analysis give evidence that AOM is mediated by a mixed community of anaerobic methanotrophic archaea and associated sulphate reducing bacteria (SRB) in the studied mud volcanoes. Little is known about the variability of methane fluxes in this environment. Carbonate crusts littering the seafloor of mud volcanoes in the northern part of the Gulf of Cadiz had strongly 13C-depleted lipid signatures indicative of higher seepage activities in the past. However, actual seafloor video observations showed only scarce traces of methane seepage and associated biological processes at the seafloor. No active fluid or free gas escape to the hydrosphere was observed visually at any of the surveyed mud volcanoes, and biogeochemical measurements indicate a complete methane consumption in the seafloor. Our observations suggest that the emission of methane to the hydrosphere from the mud volcano structures studied here may be insignificant at present.  相似文献   

7.
The molecular and stable isotope compositions of coalbed gases from the Upper Carboniferous strata and natural gases accumulated within the autochthonous Upper Miocene Skawina Formation of the D?bowiec-Simoradz gas deposit were determined, as well as the chemical and stable isotope compositions of waters from the Skawina Formation and waters at the top of the Upper Carboniferous strata of the Kaczyce Ridge (the abandoned “Morcinek” coal mine) in the South-Western part of the Upper Silesian Coal Basin. Two genetic types of natural gases within the Upper Carboniferous coal-bearing strata were identified: thermogenic (CH4, small amounts of higher gaseous hydrocarbons, and CO2) and microbial (CH4, very small amounts of ethane, and CO2). Thermogenic gases were generated during the bituminous stage of coalification and completed at the end of the Variscan orogeny. Degassing (desorption) of thermogenic gases began at the end of late Carboniferous until the late Miocene time-period and extended to the present-day. This process took place in the Upper Carboniferous strata up to a depth of about 550 m under the sealing Upper Miocene cover. A primary accumulation zone of indigenous, thermogenic gases is present below the degassing zone. Up to 200 m depth from the top of the Upper Carboniferous strata, within the weathered complex, an accumulation zone of secondary, microbial gas occurs. Waters within these strata are mainly of meteoric origin of the infiltration period just before the last sea transgression in the late Miocene and partly of marine origin having migrated from the Upper Miocene strata. Then, both methanogenic archaebacteria and their nutrients were transported by meteoric water into the near-surface Carboniferous strata where the generated microbial CH4 saturated coal seams. Waters within the Miocene strata of the D?bowiec-Simoradz and Zab?ocie are of marine origin, and natural gases accumulated within autochthonous Miocene strata of the D?bowiec-Simoradz gas deposit were most probably generated by microbial processes of on organic matter dispersed within the strata, though some contribution of gases migrating from the Carboniferous coal-bearing strata cannot be excluded.  相似文献   

8.
The Caucasian orogenic wedge formed as a consequence of the closure of the Tethyan Ocean, and numerous fields of active mud volcanoes pepper the area adjacent to the Black and Caspian Seas. Stable isotope ratios of boron, helium, and carbon have been measured for gas, fluid and sediment samples from active mud volcanoes of Taman Peninsula and Georgia to estimate the sources and mobilization depths of the fluid phase and mud. Boron concentrations in mud volcano fluids were found to be 5–35× higher than seawater. Fluid isotope ratios vary between 11B=22 and 39, while isotope ratios of the smectite- and illite-rich extruded mud are considerably depleted in heavy 11B (11B=–8 to +7). B contents of these muds are ~8× higher than modern marine sediments. This suggests that liquefaction prior to mud volcanism was accompanied by both B enrichment and isotope fractionation, most likely at an intermediate depth mud reservoir at 2–4 km.The hydrocarbon-generating source beds to the mud volcanoes are located at 7 to >10 km depth in the folded Maikop Formation and are of proposed Oligocene–Miocene age. The most likely mechanism is re-hydration of these shales by both hydrocarbons and a geochemically mature fluid from greater depth within the orogenic wedge. Such a deep fluid source is supported by our results from gas analyses, which imply an admixture of minor amounts (less than 1%vol) of 3He (Georgia), thermogenic 13C in methane as well as "ultraheavy" 13C in CO2 (both Taman and Georgia). The overall results attest active local flow of geochemically different fluids along deep-seated faults penetrating the two study areas in the Caucasian orogenic wedge, with the waters as well as the gases coming from below the Maikop Formation.  相似文献   

9.
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   

10.
Formation waters of the 14 km thick late Cretaceous–Cenozoic Beaufort–Mackenzie basin were examined as part of a larger project to better understand the petroleum potential of the region, where early exploration defined petroleum reserves of 744 × 109 bbls recoverable crude oil and 11.74 tcf gas. Historical water analyses (2583 samples from 250 wells drilled up to 5 km depth) were compiled and culled to remove incomplete and poor quality samples. The resultant database shows a broad range of salinity and water chemistry that has no systematic relationship with depth. Three main water types are defined, paleo seawater, and freshwaters related to a Miocene age gravity-driven flow system, and low TDS–high alkalinity waters. High alkalinity waters are isolated in overpressured fault blocks that were rapidly buried by post-Miocene Iperk shale deposition. The high alkalinities (up to 9000 mg/L) are interpreted to be related to in situ CO2 generation through anaerobic methanogenesis in response to freshwater invasion. The dominant control on biogenic gas generation appears to be maximum burial temperature rather than the modern temperature distribution. This is consistent with the paleopasteurization model that suggests once critical burial temperatures are reached, sterilized rocks are inhibited from further biodegradation, even when temperatures subsequently drop back into the habitable zone.  相似文献   

11.
A large suite of natural gases (93) from the North West Shelf and Gippsland and Otway Basins in Australia have been characterised chemically and isotopically resulting in the elucidation of two types of gases. About 26% of these gases have anomalous stable carbon isotope compositions in the C1–C4 hydrocarbons and CO2 components, and are interpreted to have a secondary biogenic history. The characteristics include unusually large isotopic separations between successive n-alkane homologues (up to +29‰ PDB) and isotopically heavy CO2 (up to +19.5‰ PDB). Irrespective of geographic location, these anomalous gases are from the shallower accumulations (600–1700 m) where temperatures are lower than 75°C. The secondary biogenic gases are readily distinguishable from thermogenic gases (74% of this sample suite), which should assist in the appraisal of hydrocarbons during exploration where hydrocarbon accumulations are under 2000 m. While dissolution effects may have contributed to the high 13C enrichment of the CO2 component in the secondary biogenic gases, the primary signature of this CO2 is attributed to biochemical fractionation associated with anaerobic degradation and methanogenesis. Correlation between biodegraded oils and biodegraded “dry” gas supports the concept that gas is formed from the bacterial destruction of oil, resulting in “secondary biogenic gas”. Furthermore, the prominence of methanogenic CO2 in these types of accumulations along with some isotopically-depleted methane provides evidence that the processes of methanogenesis and oil biodegradation are linked. It is further proposed that biodegradation of oil proceeds via a complex anaerobic coupling that is integral to and supports methanogenesis.  相似文献   

12.
《Applied Geochemistry》2004,19(5):695-707
Taiwan is located at the collision boundary between the Philippine Sea Plate and the Asian Continental Plate and is one of the most active orogenic belts in the world. Fluids sampled from 9 sub-aerial mud volcanoes distributed along two major geological structures in southwestern Taiwan, the Chishan fault and the Gutingkeng anticline, were analyzed to evaluate possible sources of water and the degree of fluid-sediment interaction at depth in an accretionary prism. Overall, the Taiwanese mud volcano fluids are characterized by high Cl contents, up to 347 mM, suggesting a marine origin from actively de-watering sedimentary pore waters along major structures on land. The fluids obtained from the Gutingkeng anticline, as well as from the Coastal Plain area, show high Cl, Na, K, Ca, Mg and NH4, but low SO4 and B concentrations. In contrast, the Chishan fault fluids are much less saline (1/4 seawater value), but show much heavier O isotope compositions (δ18O=5.1–6.5 ‰). A simplified scenario of mixing between sedimentary pore fluids and waters affected by clay dehydration released at depth can explain several crucial observations including heavy O isotopes, radiogenic Sr contents (87Sr/86Sr=0.71136–0.71283), and relatively low salinities in the Chishan fluids. Gases isolated from the mud volcanoes are predominantly CH4 and CO2, where the CH4–C isotopic compositions show a thermogenic component of δ13C=−38 ‰. These results demonstrate that active mud volcano de-watering in Taiwan is a direct product of intense sediment accretion and plate collision in the region.  相似文献   

13.
A suite of natural gases from the northern Songliao Basin in NE China were characterized for their molecular and carbon isotopic composition. Gases from shallow reservoirs display clear geochemical evidence of alteration by biodegradation, with very high dryness (C1/C2+ > 100), high C2/C3 and i-C4/n-C4 ratios, high nitrogen content and variable carbon dioxide content. Isotopic values show wide range variations (δ13CCH4 from −79.5‰ to −45.0‰, δ13CC2H6 from −53.7‰ to −32.2‰, δ13CC3H8 from −36.5‰ to −20.1‰, δ13CnC4H10 from −32.7‰ to −24.5‰, and δ13CCO2 from −21.6‰ to +10.5‰). A variety of genetic types can be recognized on the basis of chemical and isotopic composition together with their geological occurrence. Secondary microbial gas generation was masked by primary microbial gas and the mixing of newly generated methane with thermogenic methane already in place in the reservoir can cause very complicated isotopic signatures. System openness also was considered for shallow biodegraded gas accumulations. Gases from the Daqing Anticline are relatively wet with 13C enriched methane and 13C depleted CO2, representing typically thermogenic origin. Gases within the Longhupao-Da’an Terrace have variable dryness, 13C enriched methane and variable δ13C of CO2, suggesting dominant thermogenic origin and minor secondary microbial methane augment. The Puqian-Ao’nan Uplift contains relatively dry gas with 13C depleted methane and 13C enriched CO2, typical for secondary microbial gas with a minor part of thermogenic methane. Gas accumulations in the Western Slope are very dry with low carbon dioxide concentrations. Some gases contain 13C depleted methane, ethane and propane, indicating low maturity/primary microbial origin. Recognition of varying genetic gas types in the Songliao Basin helps explain the observed dominance of gas in the shallow reservoir and could serve as an analogue for other similar shallow gas systems.  相似文献   

14.
Identification of the source of CO2 in natural reservoirs and development of physical models to account for the migration and interaction of this CO2 with the groundwater is essential for developing a quantitative understanding of the long term storage potential of CO2 in the subsurface. We present the results of 57 noble gas determinations in CO2 rich fields (>82%) from three natural reservoirs to the east of the Colorado Plateau uplift province, USA (Bravo Dome, NM., Sheep Mountain, CO. and McCallum Dome, CO.), and from two reservoirs from within the uplift area (St. John’s Dome, AZ., and McElmo Dome, CO.). We demonstrate that all fields have CO2/3He ratios consistent with a dominantly magmatic source. The most recent volcanics in the province date from 8 to 10 ka and are associated with the Bravo Dome field. The oldest magmatic activity dates from 42 to 70 Ma and is associated with the McElmo Dome field, located in the tectonically stable centre of the Colorado Plateau: CO2 can be stored within the subsurface on a millennia timescale.The manner and extent of contact of the CO2 phase with the groundwater system is a critical parameter in using these systems as natural analogues for geological storage of anthropogenic CO2. We show that coherent fractionation of groundwater 20Ne/36Ar with crustal radiogenic noble gases (4He, 21Ne, 40Ar) is explained by a two stage re-dissolution model: Stage 1: Magmatic CO2 injection into the groundwater system strips dissolved air-derived noble gases (ASW) and accumulated crustal/radiogenic noble gas by CO2/water phase partitioning. The CO2 containing the groundwater stripped gases provides the first reservoir fluid charge. Subsequent charges of CO2 provide no more ASW or crustal noble gases, and serve only to dilute the original ASW and crustal noble gas rich CO2. Reservoir scale preservation of concentration gradients in ASW-derived noble gases thus provide CO2 filling direction. This is seen in the Bravo Dome and St. John’s Dome fields. Stage 2: The noble gases re-dissolve into any available gas stripped groundwater. This is modeled as a Rayleigh distillation process and enables us to quantify for each sample: (1) the volume of groundwater originally ‘stripped’ on reservoir filling; and (2) the volume of groundwater involved in subsequent interaction. The original water volume that is gas stripped varies from as low as 0.0005 cm3 groundwater/cm3 gas (STP) in one Bravo Dome sample, to 2.56 cm3 groundwater/cm3 gas (STP) in a St. John’s Dome sample. Subsequent gas/groundwater equilibration varies within all fields, each showing a similar range, from zero to ∼100 cm3 water/cm3 gas (at reservoir pressure and temperature).  相似文献   

15.
In this study, the geochemistry and origin of natural gas and formation waters in Devonian age organic-rich shales and reservoir sandstones across the northern Appalachian Basin margin (western New York, eastern Ohio, northwestern Pennsylvania, and eastern Kentucky) were investigated. Additional samples were collected from Mississippian Berea Sandstone, Silurian Medina Sandstone and Ordovician Trenton/Black River Group oil and gas wells for comparison. Dissolved gases in shallow groundwaters in Devonian organic-rich shales along Lake Erie contain detectable CH4 (0.01–50.55 mol%) with low δ13C–CH4 values (−74.68 to −57.86‰) and no higher chain hydrocarbons, characteristics typical of microbial gas. Nevertheless, these groundwaters have only moderate alkalinity (1.14–8.72 meq/kg) and relatively low δ13C values of dissolved inorganic C (DIC) (−24.8 to −0.6‰), suggesting that microbial methanogenesis is limited. The majority of natural gases in Devonian organic-rich shales and sandstones at depth (>168 m) in the northern Appalachian Basin have a low CH4 to ethane and propane ratios (3–35 mol%; C1/C2 + C3) and high δ13C and δD values of CH4 (−53.35 to −40.24‰, and −315.0 to −174.6‰, respectively), which increase in depth, reservoir age and thermal maturity; the molecular and isotopic signature of these gases show that CH4 was generated via thermogenic processes. Despite this, the geochemistry of co-produced brines shows evidence for microbial activity. High δ13C values of DIC (>+10‰), slightly elevated alkalinity (up to 12.01 meq/kg) and low SO4 values (<1 mmole/L) in select Devonian organic-rich shale and sandstone formation water samples suggest the presence of methanogenesis, while low δ13C–DIC values (<−22‰) and relatively high SO4 concentrations (up to 12.31 mmole/L) in many brine samples point to SO4 reduction, which likely limits microbial CH4 generation in the Appalachian Basin. Together the formation water and gas results suggest that the vast majority of CH4 in the Devonian organic-rich shales and sandstones across the northern Appalachian Basin margin is thermogenic in origin. Small accumulations of microbial CH4 are present at shallow depths along Lake Erie and in western NY.  相似文献   

16.
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   

17.
The Dvurechenskii mud volcano (DMV) is located in permanently anoxic waters at 2060 m depth (Sorokin Trough, Black Sea). The DMV was studied during the RV Meteor expedition M72/2 as an example of an active mud volcano system, to investigate the significance of submarine mud volcanism for the methane and sulfide budget of the anoxic Black Sea hydrosphere. Our studies included benthic fluxes of methane and sulfide, as well as the factors controlling transport, consumption and production of both compounds within the sediment. The pie-shaped mud volcano showed temperature anomalies as well as solute and gas fluxes indicating high fluid flow at its summit north of the geographical center. The anaerobic oxidation of methane (AOM) coupled to sulfate reduction (SR) was repressed in this zone due to the upward flow of sulfate-depleted fluids through recently deposited subsurface muds, apparently limiting microbial methanotrophic activity. Consequently, the emission of dissolved methane into the water column was high, with an estimated rate of 0.46 mol m−2 d−1. On the wide plateau and edge of the mud volcano surrounding the summit, fluid flow and total methane flux were lower, allowing higher SR and AOM rates correlated with an increase in sulfate penetration into the sediment. Here, between 50% and 70% of the methane flux (0.07-0.1 mol m−2 d−1) was consumed within the upper 10 cm of the sediment. The overall amount of dissolved methane released from the entire mud volcano structure into the water column was significant with a discharge of 1.3 × 107 mol yr−1. The DMV maintains also high areal rates of methane-fueled sulfide production and emission of on average 0.05 mol m−2 d−1. This is a difference to mud volcanoes in oxic waters, which emit similar amounts of methane, but not sulfide. However, based on a comparison of this and other mud volcanoes of the Black Sea, we conclude that sulfide and methane emission into the hydrosphere from deep-water mud volcanoes does not significantly contribute to the sulfide and methane inventory of the Black Sea.  相似文献   

18.
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   

19.
The gases emitted from mud volcanoes in the Copper River Basin of Alaska fall into two distinct types which are not mixed during vertical migration. The gases in the eastern volcanoes are nearly pure carbon dioxide, whereas the western ones contain methane and nitrogen and almost no carbon dioxide. Chemical and carbon isotopic compositions suggest the carbon dioxide rich gases originated by solution of limestones and that methane rich gases probably formed by thermal decomposition of coals.Permafrost may be a strong factor in separating the Copper River Basin gases. Extending downward for several hundred feet, the permafrost would prevent shallow lateral migration and focus the energy of the gas into occasional mud volcano vents. Soil gas analyses show rapidly decreasing amounts of the methane to about 150 m and of carbon dioxide to about 20–40 m away from the mud volcano pools. Isotopic variations of these natural methane and carbon dioxide gases, which are not intermixed, indicate that calculations of formation temperatures based on δ13C ratios cannot be used generally.  相似文献   

20.
A methodology has been developed to determine chemical and carbon isotopic compositions of trace amounts of hydrocarbon gas compounds (methane, ethane, propane, iso- and normal-butane) present as dissolved compounds in the porewater of the low permeability Callovo-Oxfordian argillites in eastern Paris Basin, France. Results indicate that the studied hydrocarbons contain significant amounts of ethane, butane and propane, in addition to methane. Carbon isotopic compositions reflect primarily thermogenic origin (thermal cracking of organic matter), and lack of any significant biodegradation. Because temperature did not exceed 50 °C in the studied argillites, investigated hydrocarbons must have originated in hotter/deeper organic-bearing formations, possibly Stephanian coals. Data supports the predominance of high maturity thermogenic gas in the upper part of the Callovo-Oxfordian, and low maturity thermogenic gas mixed with minor bacterially produced methane in the lower part of the formation. A mixing between three end-member gases models quite well the data: one thermogenic gas with a low maturity (42% methane, with a δ13C of − 53‰), a gas with higher maturity (55% methane, with a δ13C of − 47‰) and a bacterial gas (99.45% methane, with a δ13C of − 80‰). This study illustrates that migration of hydrocarbon gases can take place in rocks with very low permeability and porosity, such as compacted mudrocks, given enough time. It further suggests that the studied fluid migration and transfer in aquitards would help characterization and understanding of fluid movements in sedimentary basins, as a complement to studies focused on water aquifers and hydrocarbon reservoirs. Chemical and isotopic composition of dissolved hydrocarbons in porewater can be used as natural tracers of fluid circulation in sedimentary basins, in addition to more conventional tracers.  相似文献   

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