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1.
We report on the isotopic composition of dissolved inorganic carbon (DIC) in pore-water samples recovered by gravity coring from near-bottom sediments at gas hydrate-bearing mud volcanoes/gas flares (Malenky, Peschanka, Peschanka 2, Goloustnoe, and Irkutsk) in the Southern Basin of Lake Baikal. The δ13C values of DIC become heavier with increasing subbottom depth, and vary between ?9.5 and +21.4‰ PDB. Enrichment of DIC in 13C indicates active methane generation in anaerobic environments near the lake bottom. These data confirm our previous assumption that crystallization of carbonates (siderites) in subsurface sediments is a result of methane generation. Types of methanogenesis (microbial methyl-type fermentation versus CO2-reduction) were revealed by determining the offset of δ13C between dissolved CH4 and CO2, and also by using δ13C and δD values of dissolved methane present in the pore waters. Results show that both mechanisms are most likely responsible for methane generation at the investigated locations.  相似文献   

2.
Paola Ridge, along the NW Calabrian margin (southern Tyrrhenian Sea), is one of the few reported deep sea sites of precipitation of authigenic carbonates in the Tyrrhenian Sea. Here, the changing composition of the seeping fluids and the dynamic nature of the seepage induced the precipitation of pyrite, siderite and other carbonate phases. The occurrence of this array of authigenic precipitates is thought to be related to fluctuation of the sulfate-methane transition zone (SMTZ).Concretions of authigenic minerals formed in the near sub-bottom sediments of the Paola Ridge were investigated for their geochemical and isotopic composition. These concretions were collected in an area characterized by the presence of two alleged mud volcanoes and three mud diapirs. The mud diapirs are dotted by pockmarks and dissected by normal faults, and are known for having been a site of fluid seepage for at least the past 40 kyrs. Present-day venting activity occurs alongside the two alleged mud volcanoes and is dominated by CO2-rich discharging fluids. This discover led us to question the hypothesis of the mud volcanoes and investigate the origin of the fluids in each different domed structure of the study area.In this study, we used stable isotopes (carbon and oxygen) of carbonates coupled with rare earth element (REE) composition of different carbonate and non-carbonate phases for tracing fluid composition and early diagenesis of authigenic precipitates. The analyses on authigenic precipitates were coupled with chemical investigation of venting gas and sea-water.Authigenic calcite/aragonite concretions, from surficial sediments on diapiric structures, have depleted 13C isotopic composition and slightly positive δ18O values. By contrast, siderite concretions, generally found within the first 6 m of sediments on the alleged mud volcanoes, yielded positive δ13C and δ18O values. The siderite REE pattern shows consistent LREE (light REE) fractionation, MREE (medium REE) enrichment and positive Gd and La anomalies. As shown by the REE distribution, the 13C-depleted composition and their association with chemosymbiotic fauna, calcite/aragonite precipitated at time of moderate to high methane flux close to the seafloor, under the influence of bottom seawater. Authigenic siderite, on the other hand, formed in the subseafloor, during periods of lower gas discharges under prolonged anoxic conditions within sediments in equilibrium with 13C-rich dissolved inorganic carbon (DIC) and 18O-rich water, likely related to methanogenesis and intermittent venting of deep-sourced CO2.  相似文献   

3.
Hydrate-bearing sediment cores were retrieved from recently discovered seepage sites located offshore Sakhalin Island in the Sea of Okhotsk. We obtained samples of natural gas hydrates and dissolved gas in pore water using a headspace gas method for determining their molecular and isotopic compositions. Molecular composition ratios C1/C2+ from all the seepage sites were in the range of 1,500–50,000, while δ13C and δD values of methane ranged from ?66.0 to ?63.2‰ VPDB and ?204.6 to ?196.7‰ VSMOW, respectively. These results indicate that the methane was produced by microbial reduction of CO2. δ13C values of ethane and propane (i.e., ?40.8 to ?27.4‰ VPDB and ?41.3 to ?30.6‰ VPDB, respectively) showed that small amounts of thermogenic gas were mixed with microbial methane. We also analyzed the isotopic difference between hydrate-bound and dissolved gases, and discovered that the magnitude by which the δD hydrate gas was smaller than that of dissolved gas was in the range 4.3–16.6‰, while there were no differences in δ13C values. Based on isotopic fractionation of guest gas during the formation of gas hydrate, we conclude that the current gas in the pore water is the source of the gas hydrate at the VNIIOkeangeologia and Giselle Flare sites, but not the source of the gas hydrate at the Hieroglyph and KOPRI sites.  相似文献   

4.
This study performed a detailed geochemical analyses of the components, stable carbon isotopes of alkane gas and CO2, stable hydrogen isotopes of alkane gas and helium isotopes of reproducing gas from the largest tight gas field (Sulige) and shale gas (Fuling) field in China. The comparative study shows that tight gas from the Sulige gas field in the Ordos Basin is of coal-derived origin, which is characterized by a positive carbon and hydrogen isotopic distribution pattern (δ13C1 > δ13C2 > δ13C3 > δ13C4; δ2H1 > δ2H2 > δ2H3), i.e., the carbon and hydrogen isotopes increase with increasing carbon numbers. Carbon dioxide from this field are of biogenic origin and the helium is crust-derived. Shale gas from the Fuling shale gas field belongs to oil-derived gas which has complete carbon and hydrogen isotopic reversal of secondary alteration origin (δ13C1 < δ13C2 < δ13C3; δ2H1 < δ2H2 < δ2H3), i.e., the carbon and hydrogen isotopes decrease with increasing carbon numbers. Such complete isotopic reversal distribution pattern is due to the secondary alteration like oil or gas cracking, diffusion and so on under high temperature. In that case, positive carbon or hydrogen isotopic distribution pattern will change into complete isotopic reversal as the temperature increases. Carbon dioxide is of abiogenic origin resulting from the thermal metamorphism of carbonates and helium is crust-derived.  相似文献   

5.
Authigenic carbonates are frequently associated with methane cold-seep systems, which extensively occur in various geologic settings worldwide. Of interest is the relation between the fluids involved in their formation and the isotopic signals recorded in the carbonate cements. Along the Northern Apennines foothills (Italy), hydrocarbons and connate waters still seeping nowadays are believed to be the primary sources for the formation of fossil authigenic carbonate found in Plio-Pleistocene marine sediments. Four selected outcrops of dolomitic authigenic carbonates were analysed to compare signature of seeping fluids with fractionation of stable carbon and oxygen isotopes recorded in the carbonate.Along the foothills, deep methane-rich fluids spontaneously rise to the surface through mud volcanoes or are exploited in wells drilled nearby to the fossil Plio-Pleistocene authigenic carbonates. The plumbing system providing fluids to present-day cold seeps was structurally achieved in Late Miocene and Plio-Pleistocene. δ13C values of methane, which vary from −51.9 to −43.0‰ VPDB, indicate that gas composition from the deep hydrocarbon reservoirs is relatively uniform along the foothills. On the contrary, δ13C in fossil authigenic carbonates strongly varies among different areas and also within the same outcrop.The different carbon sources that fed the investigated carbonates were identified and include: thermogenic methane from the deep Miocene reservoirs, 13C-enriched CO2 derived from secondary methanogenesis and microbial methane from Pliocene successions buried in the Po Plain. The δ13C variability documented among samples from a single outcrop testifies that the authigenic carbonates might represent a record of varying biogeochemical processes in the hydrocarbon reservoirs. The sources of stable oxygen isotopes in authigenic carbonates are often ascribed to marine water. Oxygen isotopic fractionation in the dolomite cements indicates that marine pore water couldn't be the sole source of oxygen. δ18O values provide a preliminary evidence that connate waters had a role in the carbonates precipitation. The concomitant occurrence of active cold seepages and fossil record of former plumbing systems suggests that generation and migration of hydrocarbons are long-lasting and very effective processes along the Northern Apennines foothills.  相似文献   

6.
We investigated gas hydrate in situ inventories as well as the composition and principal transport mechanisms of fluids expelled at the Amsterdam mud volcano (AMV; 2,025 m water depth) in the Eastern Mediterranean Sea. Pressure coring (the only technique preventing hydrates from decomposition during recovery) was used for the quantification of light hydrocarbons in near-surface deposits. The cores (up to 2.5 m in length) were retrieved with an autoclave piston corer, and served for analyses of gas quantities and compositions, and pore-water chemistry. For comparison, gravity cores from sites at the summit and beyond the AMV were analyzed. A prevalence of thermogenic light hydrocarbons was inferred from average C1/C2+ ratios <35 and δ13C-CH4 values of ?50.6‰. Gas venting from the seafloor indicated methane oversaturation, and volumetric gas–sediment ratios of up to 17.0 in pressure cores taken from the center demonstrated hydrate presence at the time of sampling. Relative enrichments in ethane, propane, and iso-butane in gas released from pressure cores, and from an intact hydrate piece compared to venting gas suggest incipient crystallization of hydrate structure II (sII). Nonetheless, the co-existence of sI hydrate can not be excluded from our dataset. Hydrates fill up to 16.7% of pore volume within the sediment interval between the base of the sulfate zone and the maximum sampling depth at the summit. The concave-down shapes of pore-water concentration profiles recorded in the center indicate the influence of upward-directed advection of low-salinity fluids/fluidized mud. Furthermore, the SO 4 2? and Ba2+ pore-water profiles in the central part of the AMV demonstrate that sulfate reduction driven by the anaerobic oxidation of methane is complete at depths between 30 cm and 70 cm below seafloor. Our results indicate that methane oversaturation, high hydrostatic pressure, and elevated pore-water activity caused by low salinity promote fixing of considerable proportions of light hydrocarbons in shallow hydrates even at the summit of the AMV, and possibly also of other MVs in the region. Depending on their crystallographic structure, however, hydrates will already decompose and release hydrocarbon masses if sediment temperatures exceed ca. 19.3°C and 21.0°C, respectively. Based on observations from other mud volcanoes, the common occurrence of such temperatures induced by heat flux from below into the immediate subsurface appears likely for the AMV.  相似文献   

7.
This article reviews the abnormal characteristics of shale gases (natural gases produced from organic-rich shales) and discusses the cause of the anomalies and mechanisms for gas enrichment and depletion in high-maturity organic-rich shales. The reported shale gas geochemical anomalies include rollover of iso-alkane/normal alkane ratios, rollover of ethane and propane isotopic compositions, abnormally light ethane and propane δ13C values as well as isotope reversals among methane, ethane and propane. These anomalies reflect the complex histories of gas generation and associated isotopic fractionation as well as in-situ “mixing and accumulation” of gases generated from different precursors at different thermal maturities. A model was proposed to explain the observed geochemical anomalies. Gas generation from kerogen cracking at relatively low thermal maturity accounted for the increase of iso-alkane/normal alkane ratios and ethane and propane δ13C values (normal trend). Simultaneous cracking of kerogen, retained oil and wet gas and associated isotopic fractionation at higher maturity caused decreasing iso-alkane/normal alkane ratios, lighter ethane and propane δ13C and corresponding conversion of carbon isotopic distribution patterns from normal through partial reversal to complete reversal. Relatively low oil expulsion efficiency at peak oil generation, low expulsion efficiency at peak gas generation and little gas loss during post-generation evolution are necessary for organic-rich shales to display the observed geochemical anomalies. High organic matter richness, high thermal maturity (high degrees of kerogen-gas and oil-gas conversions) and late-stage (the stage of peak gas generation and post-generation evolution) closed system accounted for gas enrichment in shales. Loss of free gases during post-generation evolution may result in gas depletion or even undersaturation (total gas content lower than the gas sorption capacity) in high-maturity organic-rich shales.  相似文献   

8.
Hydrocarbon gases were determined in sediments from three mud volcanoes in the Sorokin Trough. In comparison to a reference station outside the mud volcano area, the deposits are characterized by an enrichment of high-molecular hydrocarbons (C2–C4), an absence of unsaturated homologues, a predominance of iso-butane in comparison with n-butane, and the presence of gas hydrate. The molecular composition of the hydrocarbon gases suggests their deep sources and thermogenic origin. In the pelagic sediments at the reference station, the methane concentration is relatively low (up to 49 ml/l); maximum concentrations are reached in deposits of the Dvurechenskii mud volcano (up to 400 ml/l). It was the first time that gas hydrate was sampled at the Dvurechenskii mud volcano. The gas extracted by dissociation of hydrate samples was dominated by methane (99.5%) with low amounts of ethane and propane (less than 0.5%). The isotopic composition of the methane varies between –62 and –66 PDB in 13C, and between –185 and –209 SMOW in D, indicating a mainly biogenic origin with an admixture of thermogenic gas.  相似文献   

9.
We investigated the molecular composition (methane, ethane, and propane) and stable isotope composition (methane and ethane) of hydrate-bound gas in sediments of Lake Baikal. Hydrate-bearing sediment cores were retrieved from eight gas seep sites, located in the southern and central Baikal basins. Empirical classification of the methane stable isotopes (δ13C and δD) for all the seep sites indicated the dominant microbial origin of methane via methyl-type fermentation; however, a mixture of thermogenic and microbial gases resulted in relatively high methane δ13C signatures at two sites where ethane δ13C indicated a typical thermogenic origin. At one of the sites in the southern Baikal basin, we found gas hydrates of enclathrated microbial ethane in which 13C and deuterium were both highly depleted (mean δ13C and δD of –61.6‰ V-PDB and –285.4‰ V-SMOW, respectively). To the best of our knowledge, this is the first report of C2 δ13C–δD classification for hydrate-bound gas in either freshwater or marine environments.  相似文献   

10.
To study the sedimentary environment of the Lower Cambrian organic-rich shales and isotopic geochemical characteristics of the residual shale gas, 20 black shale samples from the Niutitang Formation were collected from the Youyang section, located in southeastern Chongqing, China. A combination of geochemical, mineralogical, and trace element studies has been performed on the shale samples from the Lower Cambrian Niutitang Formation, and the results were used to determine the paleoceanic sedimentary environment of this organic-rich shale. The relationships between total organic carbon (TOC) and total sulfur (TS) content, carbon isotope value (δ13Corg), trace element enrichment, and mineral composition suggest that the high-TOC Niutitang shale was deposited in an anoxic environment and that the organic matter was well preserved after burial. Stable carbon isotopes and biomarkers both indicate that the organic matter in the Niutitang black shales was mainly derived from both lower aquatic organisms and algaes and belong to type I kerogen. The oil-prone Niutitang black shales have limited residual hydrocarbons, with low values of S2, IH, and bitumen A. The carbon isotopic distribution of the residual gas indicate that the shale gas stored in the Niutitang black shale was mostly generated from the cracking of residual bitumen and wet gas during a stage of significantly high maturity. One of the more significant observations in this work involves the carbon isotope compositions of the residual gas (C1, C2, and C3) released by rock crushing. A conventional δ13C1–δ13C2 trend was observed, and most δ13C2 values of the residual gases are heavier than those of the organic matter (OM) in the corresponding samples, indicating the splitting of ethane bonds and the release of smaller molecules, leading to 13C enrichment in the residual ethane.  相似文献   

11.
The stable carbon isotopic ratios (δ13C) of methane (CH4) and carbon dioxide (CO2) of gas-rich fluid inclusions hosted in fracture-fill mineralization from the southern part of the Lower Saxony Basin, Germany have been measured online using a crushing device interfaced to an isotopic ratio mass spectrometer (IRMS). The data reveal that CH4 trapped in inclusions seems to be derived from different source rocks with different organic matter types. The δ13C values of CH4 in inclusions in quartz hosted by Carboniferous rocks range between −25 and −19‰, suggesting high-maturity coals as the source of methane. Methane in fluid inclusions in minerals hosted by Mesozoic strata has more negative carbon isotope ratios (−45 to −31‰) and appears to represent primary cracking products from type II kerogens, i.e., marine shales. There is a positive correlation between increasing homogenization temperatures of aqueous fluid inclusions and less negative δ13C(CH4) values of in co-genetic gas inclusions probably indicating different mtaturity of the potential source rocks at the time the fluids were released. The CO2 isotopic composition of CH4-CO2-bearing inclusions shows slight negative or even positive δ13C values indicating an inorganic source (e.g., water-rock interaction and dissolution of detrital, marine calcite) for CO2 in inclusions. We conclude that the δ13C isotopic ratios of CH4-CO2-bearing fluid inclusions can be used to trace migration pathways, sources of gases, and alteration processes. Furthermore, the δ13C values of methane can be used to estimate the maturity of the rocks from which it was sourced. Results presented here are further supported by organic geochemical analysis of surface bitumens which coexist with the gas inclusion-rich fracture-fill mineralization and confirm the isotopic interpretations with respect to fluid source, type and maturity.  相似文献   

12.
The Qiongdongnan Basin, South China Sea has received huge thickness (>12 km) of Tertiary-Quaternary sediments in the deepwater area to which great attention has been paid due to the recent discoveries of the SS22-1 and the SS17-2 commercial gas fields in the Pliocene-Upper Miocene submarine canyon system with water depth over 1300 m. In this study, the geochemistry, origin and accumulation models of these gases were investigated. The results reveal that the gases are predominated by hydrocarbon gases (98%–99% by volume), with the ratio of C1/C1-5 ranging from 0.92 to 0.94, and they are characterized by relatively heavy δ13C1 (−36.8‰ to −39.4‰) and δDCH4 values (−144‰ to −147‰), similar to the thermogenic gases discovered in the shallow water area of the basin. The C5-7 light hydrocarbons associated with these gases are dominated by isoparaffins (35%–65%), implying an origin from higher plants. For the associated condensates, carbon isotopic compositions and high abundance of oleanane and presence of bicadinanes show close affinity with those from the YC13-1 gas field in the shallow water area. All these geochemical characteristics correlate well with those found in the shales of the Oligocene Yacheng Formation in the Qiongdongnan Basin. The Yacheng Formation in the deepwater area has TOC values in the range of 0.4–21% and contains type IIb–III gas-prone kerogens, indicating an excellent gas source rock. The kinetic modeling results show that the δ13C1 values of the gas generated from the Yacheng source rock since 3 or 4 Ma are well matched with those of the reservoir gases, indicating that the gas pool is young and likely formed after 4 Ma. The geologic and geochemical data show that the mud diapirs and faults provide the main pathways for the upward migration of gases from the deep gas kitchen into the shallow, normally pressured reservoirs, and that the deep overpressure is the key driving force for the vertical and lateral migration of gas. This gas migration pattern implies that the South Low Uplift and the No.2 Fault zone near the deepwater area are also favorable for gas accumulation because they are located in the pathway of gas migration, and therefore more attention should be paid to them in the future.  相似文献   

13.
The Coal Oil Point seep field located offshore Santa Barbara, CA, consists of dozens of named seeps, including a peripheral ～200 m2 area known as Brian Seep, located in 10 m water depth. A single comprehensive survey of gas flux at Brian Seep yielded a methane release rate of ～450 moles of CH4 per day, originating from 68 persistent gas vents and 23 intermittent vents, with gas flux among persistent vents displaying a log normal frequency distribution. A subsequent series of 33 repeat surveys conducted over a period of 6 months tracked eight persistent vents, and revealed substantial temporal variability in gas venting, with flux from each individual vent varying by more than a factor of 4. During wintertime surveys sediment was largely absent from the site, and carbonate concretions were exposed at the seafloor. The presence of the carbonates was unexpected, as the thermogenic seep gas contains 6.7% CO2, which should act to dissolve carbonates. The average δ13C of the carbonates was ?29.2?±?2.8‰ VPDB, compared to a range of ?1.0 to +7.8‰ for CO2 in the seep gas, indicating that CO2 from the seep gas is quantitatively not as important as 13C-depleted bicarbonate derived from methane oxidation. Methane, with a δ13C of approximately ?43‰, is oxidized and the resulting inorganic carbon precipitates as high-magnesium calcite and other carbonate minerals. This finding is supported by 13C-depleted biomarkers typically associated with anaerobic methanotrophic archaea and their bacterial syntrophic partners in the carbonates (lipid biomarker δ13C ranged from ?84 to ?25‰). The inconsistency in δ13C between the carbonates and the seeping CO2 was resolved by discovering pockets of gas trapped near the base of the sediment column with δ13C-CO2 values ranging from ?26.9 to ?11.6‰. A mechanism of carbonate formation is proposed in which carbonates form near the sediment–bedrock interface during times of sufficient sediment coverage, in which anaerobic oxidation of methane is favored. Precipitation occurs at a sufficient distance from active venting for the molecular and isotopic composition of seep gas to be masked by the generation of carbonate alkalinity from anaerobic methane oxidation.
Figure
Processes modulating carbonate formation at Brian Seep (California) during times of high and low sediment burden  相似文献   

14.
The worlds >1500 mud volcanoes are normally in a dormant stage due to the short duration of eruptions. Their dormant stage activity is often characterized by vigorous seepage of water, gas, and petroleum. However, the source of the fluids and the fluid–rock interactions within the mud volcano conduit remain poorly understood. In order to investigate this type of activity, we have combined satellite images with fieldwork and extensive sampling of water and gas at seeping gryphons, pools and salsa lakes at the Dashgil mud volcano in Azerbaijan. We find that caldera collapse faults and E–W oriented faults determine the location of the seeps. The seeping gas is dominated by methane (94.9–99.6%), with a δ13C (‰ V-PDB) in the −43.9 to −40.4‰ range, consistent throughout the 12 analysed seeps. Ethane and carbon dioxide occur in minor amounts. Seventeen samples of seeping water show a wide range in solute content and isotopic composition. Pools and salsa lakes have the highest salinities (up to 101,043 ppm Cl) and the lowest δ18O (‰ V-SMOW) values (1–4‰). The mud-rich gryphons have low salinities (<18,000 ppm Cl) and are enriched in 18O (δ18O = 4–6‰).  相似文献   

15.
The Western Desert of Egypt is one of the world’s most prolific Jurassic and Cretaceous hydrocarbon provinces. It is one of many basins that experienced organic-rich sedimentation during the late Cenomanian/early Turonian referred to as oceanic anoxic event 2 (OAE2). The Razzak #7 oil well in the Razzak Field in the northern part of the Western Desert encountered the Upper Cretaceous Abu Roash Formation. This study analyzed 23 samples from the upper “G”, “F”, and lower “E” members of the Abu Roash Formation for palynomorphs, particulate organic matter, total organic carbon (TOC) and δ13Corg in order to identify the OAE2, determine hydrocarbon source rock potential, and interpret the depositional environment. The studied samples are generally poor in palynomorphs, but show a marked biofacies change between the lower “E” member and the rest of the studied samples. Palynofacies analysis (kerogen quality and quantity) indicates the presence of oil- and gas-prone materials (kerogen types I and II/III, respectively), and implies reducing marine paleoenvironmental conditions. Detailed carbon stable isotopic and organic carbon analyses indicate that fluctuations in the δ13Corg profile across the Abu Roash upper “G”, “F”, and lower “E” members correspond well with changes in TOC values. A positive δ13Corg excursion (∼2.01‰) believed to mark the short-term global OAE2 was identified within the organic-rich shaly limestone in the basal part of the Abu Roash “F” member. This excursion also coincides with the peak TOC measurement (24.61 wt.%) in the samples.  相似文献   

16.
Vodyanitskii mud volcano is located at a depth of about 2070 m in the Sorokin Trough, Black sea. It is a 500-m wide and 20-m high cone surrounded by a depression, which is typical of many mud volcanoes in the Black Sea. 75 kHz sidescan sonar show different generations of mud flows that include mud breccia, authigenic carbonates, and gas hydrates that were sampled by gravity coring. The fluids that flow through or erupt with the mud are enriched in chloride (up to ∼650 mmol L−1 at ∼150-cm sediment depth) suggesting a deep source, which is similar to the fluids of the close-by Dvurechenskii mud volcano. Direct observation with the remotely operated vehicle Quest revealed gas bubbles emanating at two distinct sites at the crest of the mud volcano, which confirms earlier observations of bubble-induced hydroacoustic anomalies in echosounder records. The sediments at the main bubble emission site show a thermal anomaly with temperatures at ∼60 cm sediment depth that were 0.9 °C warmer than the bottom water. Chemical and isotopic analyses of the emanated gas revealed that it consisted primarily of methane (99.8%) and was of microbial origin (δD-CH4 = −170.8‰ (SMOW), δ13C-CH4 = −61.0‰ (V-PDB), δ13C-C2H6 = −44.0‰ (V-PDB)). The gas flux was estimated using the video observations of the ROV. Assuming that the flux is constant with time, about 0.9 ± 0.5 × 106 mol of methane is released every year. This value is of the same order-of-magnitude as reported fluxes of dissolved methane released with pore water at other mud volcanoes. This suggests that bubble emanation is a significant pathway transporting methane from the sediments into the water column.  相似文献   

17.
Detailed lithological, biogeochemical and molecular biological analyses of core sediments collected in 2002–2006 from the vicinity of the Malenky mud volcano, Lake Baikal, reveal considerable spatial variations in pore water chemical composition, with total concentrations of dissolved salts varying from 0.1 to 1.8‰. Values of methane δ13С in the sediments suggest a biogenic origin (δ13Сmin. ?61.3‰, δ13Сmax. ?72.9‰). Rates of sulphate reduction varied from 0.001 to 0.7 nmol cm?3 day?1, of autotrophic methanogenesis from 0.01 to 2.98 nmol CH4 cm?3 day?1, and of anaerobic oxidation of methane from 0 to 12.3 nmol cm?3 day?1. These results indicate that methanogenic processes dominate in gas hydrate-bearing sediments of Lake Baikal. Based on clone libraries of 16S rRNA genes amplified with Bacteria- and Archaea-specific primers, investigation of microbial diversity in gas hydrate-bearing sediments revealed bacterial 16S rRNA clones classified as Deltaproteobacteria, Gammaproteobacteria, Chloroflexi and OP11. Archaeal clone sequences are related to the Crenarchaeota and Euryarchaeota. Baikal sequences of Archaea form a distinct cluster occupying an intermediate position between the marine groups ANME-2 and ANME-3 of anaerobic methanotrophs.  相似文献   

18.
Natural gas samples from two gas fields located in Eastern Kopeh-Dagh area were analyzed for molecular and stable isotope compositions. The gaseous hydrocarbons in both Lower Cretaceous clastic reservoir and Upper Jurassic carbonate reservoir are coal-type gases mainly derived from type III kerogen, however enriched δD values of methane implies presence of type II kerogen related material in the source rock. In comparison Upper Jurassic carbonate reservoir gases show higher dryness coefficient resulted through TSR, while presence of C1C5 gases in Lower Cretaceous clastic reservoir exhibit no TSR phenomenon. Carbon isotopic values indicate gas to gas cracking and TSR occurrence in the Upper Jurassic carbonate reservoir, as the result of elevated temperature experienced, prior to the following uplifts in last 33–37 million years. The δ13C of carbon dioxide and δ34S of hydrogen sulfide in Upper Jurassic carbonate reservoir do not primarily reflect TSR, as uplift related carbonate rock dissolution by acidic gases and reaction/precipitation of light H2S have changed these values severely. Gaseous hydrocarbons in both reservoirs exhibit enrichment in C2 gas member, with the carbonate reservoir having higher values resulted through mixing with highly-mature-completely-reversed shale gases. It is likely that the uplifts have lifted off the pressure on shale gases, therefore facilitated the migration of the gases into overlying horizons. However it appears that the released gases during the first major uplift (33–37 million years ago) have migrated to both reservoirs, while the second migrated gases have only mixed with Upper Jurassic carbonate reservoir gases. The studied data suggesting that economic accumulations of natural gas/shale gases deeper than Upper Jurassic carbonate reservoir would be unlikely.  相似文献   

19.
Significant offshore asphaltic deposits with active seepage occur in the Santa Barbara Channel offshore southern California. The composition and isotopic signatures of gases sampled from the oil and gas seeps reveal that the coexisting oil in the shallow subsurface is anaerobically biodegraded, generating CO2 with secondary CH4 production. Biomineralization can result in the consumption of as much as 60% by weight of the original oil, with 13C enrichment of CO2. Analyses of gas emitted from asphaltic accumulations or seeps on the seafloor indicate up to 11% CO2 with 13C enrichment reaching +24.8‰. Methane concentrations range from less than 30% up to 98% with isotopic compositions of –34.9 to –66.1‰. Higher molecular weight hydrocarbon gases are present in strongly varying concentrations reflecting both oil-associated gas and biodegradation; propane is preferentially biodegraded, resulting in an enriched 13C isotopic composition as enriched as –19.5‰. Assuming the 132 million barrels of asphaltic residues on the seafloor represent ~40% of the original oil volume and mass, the estimated gas generated is 5.0×1010 kg (~76×109 m3) CH4 and/or 1.4×1011 kg CO2 over the lifetime of seepage needed to produce the volume of these deposits. Geologic relationships and oil weathering inferences suggest the deposits are of early Holocene age or even younger. Assuming an age of ~1,000 years, annual fluxes are on the order of 5.0×107 kg (~76×106 m3) and/or 1.4×108 kg for CH4 and CO2, respectively. The daily volumetric emission rate (2.1×105 m3) is comparable to current CH4 emission from Coal Oil Point seeps (1.5×105 m3/day), and may be a significant source of both CH4 and CO2 to the atmosphere provided that the gas can be transported through the water column.  相似文献   

20.
The data on the isotopic composition of particulate organic carbon (δ13CPOC) in the Caspian Sea water in summer–autumn 2008, 2010, 2012, and 2013 are discussed in the paper. These data allowed as to reveal the predominant genesis of organic carbon in suspended particulate matter of the active seawater layer (from 0 to 40 m). The δ13CPOC =–27‰ (PDB) and δ13CPOC =–20.5‰ (PDB) values were taken as the reference data for terrigenous and planktonogenic organic matter, respectively. Seasonal (early summer, late summer, and autumn) variations in the composition of suspended particulate matter in the active sea layer were revealed. A shift of δ13CPOC towards greater values was seen in autumn (with a slight outburst in the development (bloom) of phytoplankton) in comparison with summer (with large accumulations and an extraordinary phytoplankton bloom confined to the thermocline area). The seasonal dynamics of autochthonous and allochthonous components in the suspended particulate matter of the Middle and Southern Caspian Sea was studied with the use of data on the concentration of particulate matter and chlorophyll a, the phytoplankton biomass and the POC content.  相似文献   

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