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

2.
Ordos Basin, the second largest sedimentary basin in China, contains enormous natural gas resources. Each of the four giant gas fields discovered so far in this basin (i.e., Sulige, Yulin, Wushenqi and Jingbian) has over 100 billion cubic meters (bcm) or 3.53 trillion cubic feet (tcf) of proven gas reserves. This study examines the stable carbon isotope data of 125 gas samples collected from the four giant gas fields in the Ordos Basin. Source rocks in the Upper Paleozoic coal measures are suggested by the generally high δ13C values of C1–C4 gaseous hydrocarbons in the gases from the Sulige, Yulin and Wushenqi gas fields. While the δ13CiC4 value is higher than that of the δ13CnC4, the dominant ranges for the δ13C1, δ13C2, and δ13C3 values in these Upper Paleozoic reservoired gases are −34 to −32‰, −27 to −23‰, and −25 to −24‰, respectively. The δ13C values of methane, benzene and toluene in gases from the Lower Paleozoic reservoirs of the Jingbian field indicate a significant contribution from humic source rocks, as they are similar to those in the Upper Paleozoic reservoirs of the Sulige, Yulin and Wushenqi gas fields. However, the wide variation and reversal in the δ13C1, δ13C2 and δ13C3 values in the Jinbian gases cannot be explained using a single source scenario, thus the gases were likely derived dominantly from the Carboniferous-Permian coal measures with some contribution from the carbonates in the Lower Permian Taiyuan Formation. The gas isotope data and extremely low total organic carbon contents (<0.2% TOC) suggest that the Ordovician Majiagou Formation carbonates are unlikely to be a significant gas source rock, thus almost all of the economic gas accumulations in the Ordos Basin were derived from Upper Paleozoic source rocks.  相似文献   

3.
Previous studies on the coal-bed methane potential of the Zonguldak basin have indicated that the gases are thermogenic and sourced by the coal-bearing Carboniferous units. In this earlier work, the origin of coal-bed gas was only defined according to the molecular composition of gases and to organic geochemical properties of the respective source rocks, since data on isotopic composition of gases were not available. Furthermore, in the western Black Sea region there also exist other source rocks, which may have contributed to the coal-bed gas accumulations. The aim of this study is to determine the origin of coal-bed gas and to try a gas-source rock correlation. For this purpose, the molecular and isotopic compositions of 13 headspace gases from coals and adjacent sediments of two wells in the Amasra region have been analyzed. Total organic carbon (TOC) measurements and Rock-Eval pyrolysis were performed in order to characterize the respective source rocks. Coals and sediments are bearing humic type organic matter, which have hydrogen indices (HI) of up to 300 mgHC/gTOC, indicating a certain content of liptinitic material. The stable carbon isotope ratios (δ13C) of the kerogen vary from −23.1 to −27.7‰. Air-free calculated gases contain hydrocarbons up to C5, carbon dioxide (<1%) and a considerable amount of nitrogen (up to 38%). The gaseous hydrocarbons are dominated by methane (>98%). The stable carbon isotope ratios of methane, ethane and propane are defined as δ13C1: −51.1 to −48.3‰, δ13C2: −37.9 to −25.3‰, δ13C3: −26.0 to −19.2 ‰, respectively. The δD1 values of methane range from −190 to −178‰. According to its isotopic composition, methane is a mixture, partly generated bacterially, partly thermogenic. Molecular and isotopic composition of the gases and organic geochemical properties of possible source rocks indicate that the thermogenic gas generation took place in coals and organic rich shales of the Westphalian-A Kozlu formation. The bacterial input can be related to a primary bacterial methane generation during Carboniferous and/or to a recent secondary bacterial methane generation. However, some peculiarities of respective isotope values of headspace gases can also be related to the desorption process, which took place by sampling.  相似文献   

4.
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   

5.
Stable isotope ratios of oxygen and carbon were determined for CO2 in soil gas in the vicinity of the massive sulfide deposit at Crandon, Wisconsin with the objective of determining the source of anomalously high CO2 concentrations detected previously by McCarthy et al. (1986). Values of δ13C in soil gas CO2 from depths between 0.5 and 1.0 m were found to range from −12.68‰ to −20.03‰ (PDB). Organic carbon from the uppermost meter of soil has δ13C between −24.1 and −25.8‰ (PDB), indicating derivation from plant species with the C3 (Calvin) type of photosynthetic pathway. Microbial decomposition of the organic carbon and root respiration from C3 and C4 (Hatch-Slack) plants, together with atmospheric CO2 are the likely sources of carbon in soil gas CO2. Values of δ18O in soil-gas CO2 range from 32 to 38‰ (SMOW). These δ18O values are intermediate between that calculated for CO2 gas in isotopic equilibrium with local groundwaters and that for atmospheric CO2. The δ18O data indicate that atmospheric CO2 has been incorporated by mixing or diffusion. Any CO2 generated by microbial oxidation of organic matter has equilibrated its oxygen isotopes with the local groundwaters.The isotopic composition of soil-gas CO2 taken from directly above the massive sulfide deposit was not distinguishable from that of background samples taken 1 to 2 km away. No enrichment of the δ13C value of soil-gas CO2 was observed, contrary to what would be expected if the anomalous CO2 were derived from the dissolution of Proterozoic marine limestone country rock or of Paleozoic limestone clasts in glacial till. Therefore, it is inferred that root respiration and decay of C3 plant material were responsible for most CO2 generation both in the vicinity of the massive sulfide and in the “background” area, on the occasion of our sampling. Interpretation of our data is complicated by the effects of rainfall, which significantly reduced the magnitude of the CO2 anomaly. Therefore, we cannot rule out the possible mechanism of carbonate dissolution driven by pyrite oxidation, as proposed by Lovell et al. (1983) and McCarthy et al. (1986). Further work is needed on seasonal and daily variations of CO2 concentrations and stable isotope ratios in various hydrogeologic and ecologic settings so that more effective sampling strategies can be developed for mineral exploration using soil gases.  相似文献   

6.
Chemical and isotopic compositions have been measured on 62 microbial gases from Tertiary hemipelagic sediments in the Middle America Trench off Guatemala and from decaying kelp and surf grass currently accumulating in Scripps Submarine Canyon off southern California. Gases from the Middle America Trench have been generated primarily by the reduction of carbon dioxide; methane δ13C varies from −84‰ to −39‰, methane δD varies from −208‰ to −145‰, and carbon dioxide δ13 C varies from −27‰ to +28‰. Gases from Scripps Submarine Canyon have been generated primarily by acetate dissimilation; methane δ13 C varies from −63‰ to −43‰, methane δD varies from −331‰ to −280‰, and carbon dioxide δ13C varies from −17‰ to +3‰.Methane δ13C values as heavy as −40‰ appear to be uncommon for gases produced by carbon dioxide reduction and, in the Middle America Trench, are associated with unusually positive carbon dioxide δ13C values. However, based on the 25‰ intramolecular fractionation between acetate car☐yl carbon and methyl carbon estimated from the Scripps Submarine Canyon data, methane produced by acetate dissimilation may commonly have heavy δ13C values. The δD of methane derived from acetate is more negative than natural methanes from other origins. Microbial methane δD values appear to be controlled primarily by interstitial water δD and by the relative proportions of methane derived from carbon dioxide and acetate.The chemical and isotopic compositions of microbial gas and thermogenic gas overlap, making it difficult to determine the origins of many commercial natural gases from methane δ13C and C2+ hydrocarbon concentrations alone. Measurements of methane δD and carbon dioxide δ13C can provide useful additional information, and together with ethane δ13C data, help identify gases with mixed microbial and thermogenic origins.  相似文献   

7.
Carbon isotope and molecular compositions of Mississippian to Upper Cretaceous mud gases have been examined from four depth profiles across the Western Canada Sedimentary Basin (WCSB). The profiles range from the shallow oil sands in the east (R0 = 0.25) to the very mature sediments in the overthrust zone to the west (R0 = 2.5). In the undisturbed WCSB, δ13C1–δ13C2 and δ13C2–δ13C3 cross-plots show three maturity and alteration trends: (1) pre-Cretaceous gas sourced from type II kerogen; (2) Cretaceous Colorado Group gas; and (3) Lower Cretaceous Mannville Group biodegraded gas. A fourth set of distinctly different maturity trends is recognized for Lower Cretaceous gas sourced from type III kerogen in the disturbed belt of the WCSB. Displacement of these latter maturity trends to high δ13C2 values suggests that the sampled gas was trapped after earlier formed gas escaped, probably as a result of overthrusting. Unusually 13C-enriched gas (δ13C1 = −34‰, δ13C2 = −13‰, and δ13C3 = 0‰), from the Gething Formation in the disturbed belt, is the result of late stage gas cracking in a closed system. In general, gas maturity is consistent with the maturity of the host sediments in the WCSB, suggesting that migration and mixing of gases was not pervasive on a broad regional and stratigraphic scale. The ‘Deep Basin’ portion of the WCSB is an exception. Here extensive cross-formational homogenization of gases has occurred, in addition to updip migration along the most permeable stratigraphic units.  相似文献   

8.
The CO2 gas reservoir sandstones in the Hailaer Basin contain abundant dawsonite and provide an ideal laboratory to study whether any genetic relationship exists between dawsonite and the modern gas phase of CO2. The origins of dawsonite and CO2 in these sandstones were studied by petrographic and isotopic analysis. According to the paragenetic sequence of the sandstones, dawsonite grew later than CO2 charging at 110–85 Ma. The dawsonite δ18O value is 7.4‰ (SMOW), and the calculated δ18O values of the water present during dawsonite growth are from −11.4‰ to −9.2‰ (SMOW). This, combined with the NaHCO3-dominated water linked to dawsonite growth, suggests meteoric water being responsible for dawsonite growth. The δ13C values of gas phase CO2 and the ratios of 3He/4He of the associated He suggest a mantle magmatic origin of CO2-rich natural gas in Hailaer basin. Dawsonite δ13C values are −5.3‰ to −1.5‰ (average −3.4‰), and the calculated δ13C values of CO2 gas in isotopic equilibrium with dawsonite are −11.4‰ to −7.3‰. These C isotopic values are ambiguous for the dawsonite C source. From the geological context, the timing of events, together with formation water conditions for dawsonite growth, dawsonite possibly grew in meteoric-derived water, atmospherically-derived CO2 maybe, or at least the dominant, C source for dawsonite. It seems that there are few relationships between dawsonite and the modern gas phase of CO2 in the Hailaer basin.  相似文献   

9.
Groundwaters in the confined aquifers of the Chianan and Ilan coastal plains of Taiwan are rich in dissolved methane (CH4). Serious endemic “blackfoot disease”, which occurred in the Chianan plain, especially during AD1950-1970, has been demonstrated to have arisen from drinking highly reducing groundwater with abnormal arsenic and humic substance levels. In order to explore the origin of CH4 and its hydrological implications, stable carbon isotope ratios (δ13C) and radiocarbon (14C) ages of exsolved CH4, dissolved inorganic carbon (DIC), and sedimentary biogenic sediments from a total of 34 newly completed water wells at 16 sites were determined. The main results obtained are as follows: (1) The δ13CCH4 (−65‰ to −75‰) values indicate that, except for one thermogenic sample (δ13CCH4=38.2‰) from the Ilan plain, all CH4 samples analyzed were produced via microbially mediated CO2 reduction. Many δ13CDIC values are considerably greater than −10‰ and even up to 10‰ due to Rayleigh enrichment during CO2 reduction. (2) Almost all the 14C ages of CH4 samples from the shallow aquifer (I) (<60 m depth) are greater than the 14C ages of coexisting DIC and sediments, suggesting the presence of CH4 from underlying aquifers. (3) The 14C ages of coexisting CH4, DIC and sediments from aquifer (II) of the Chianan plain are essentially equal, reflecting in-situ generation of CH4 and DIC from decomposition of sedimentary organic matter and sluggishness of the groundwater flow. On the other hand, both CH4 and DIC from each individual well of the relatively deep aquifers (III) and (IV) in the Chianan plain are remarkably younger than the deposition of their coexisting sediments, indicating that current groundwaters entered these two aquifers much later than the deposition of aquifer sediments. (4) Each CH4 sample collected from the Ilan plain is older than coexisting DIC, which in turn is distinctly older than the deposition of respective aquifer sediments, demonstrating the presence of much older CO2 and CH4 from underlying strata.  相似文献   

10.
Oil and gas exploration in eastern Tarim Basin, NW China has been successful in recent years, with several commercial gas accumulations being discovered in a thermally mature to over-mature region. The Yingnan2 (YN2) gas field, situated in the Yingnan structure of the Yingjisu Depression, produces gases that are relatively enriched in nitrogen and C2+ alkanes. The δ13C1 (−38.6‰ to −36.2‰) and δ13C2 values (−30.9‰ to −34.7‰) of these gases are characteristic of marine sourced gases with relatively high maturity levels. The distributions of biomarkers in the associated condensates suggest close affinities with the Cambrian–Lower Ordovician source rocks which, in the Yingjisu Sag, are currently over-mature (with 3–4%Ro). Burial and thermal maturity modeling results indicate that paleo-temperatures of the Cambrian–Lower Ordovician source rocks had increased from 90 to 210 °C during the late Caledonian orogeny (458–438 Ma), due to rapid subsidence and sediment loading. By the end of Ordovician, hydrocarbon potential in these source rocks had been largely exhausted. The homogenization temperatures of hydrocarbon fluid inclusions identified from the Jurassic reservoirs of the YN2 gas field suggest a hydrocarbon emplacement time as recent as about 10 Ma, when the maturity levels of Middle–Lower Jurassic source rocks in the study area were too low (<0.7%Ro) to form a large quantity of oil and gas. The presence of abundant diamondoid hydrocarbons in the associated condensates and the relatively heavy isotopic values of the oils indicate that the gases were derived from thermal cracking of early-formed oils. Estimation from the stable carbon isotope ratios of gaseous alkanes suggests that the gases may have been formed at temperatures well above 190 °C. Thus, the oil and gas accumulation history in the study area can be reconstructed as follows: (1) during the late Caledonian orogeny, the Cambrian–Lower Ordovician marine source rocks had gone through the peak oil, wet gas and dry gas generation stages, with the generated oil and gas migrating upwards along faults and fractures to form early oil and gas accumulations in the Middle–Upper Ordovician and Silurian sandstone reservoirs; (2) since the late Yanshanian orogeny, the early oil accumulations have been buried deeper and oil has undergone thermal cracking to form gas; (3) during the late Himalayan orogeny, the seals for the deep reservoirs were breached; and the gas and condensates migrated upward and eventually accumulating in the relatively shallow Jurassic reservoirs.  相似文献   

11.
Lime mortar and plaster were sampled from Roman, medieval and early modern buildings in Styria. The historical lime mortar and plaster consist of calcite formed in the matrix during setting and various aggregates. The stable C and O isotopic composition of the calcite matrix was analyzed to get knowledge about the environmental conditions during calcite formation. The δ13Cmatrix and δ18Omatrix values range from −31 to 0‰ and −26 to −3‰(VPDB), respectively. Obviously, such a range of isotope values does not represent the local natural limestone assumed to be used for producing the mortar and plaster. In an ideal case, the calcite matrix in lime mortar and plaster is isotopically lighter in the exterior vs. the interior mortar layer according to the relationship δ18Omatrix = 0.61 · δ13Cmatrix − 3.3 (VPDB). Calcite precipitation by uptake of gaseous CO2 into alkaline Ca(OH)2 solutions shows a similar relationship, δ18Ocalcite = 0.67 · δ13Ccalcite − 6.4 (VPDB). Both relationships indicate that the 13C/12C and 18O/16O values of the calcite reflect the setting behaviour of the lime mortar and plaster. Initially, CO2 from the atmosphere is fixed as calcite, which is accompanied by kinetic isotope fractionation mostly due to the hydroxylation of CO2 (δ13Cmatrix ≈  −25‰ and δ18Omatrix ≈ −20‰). As calcite formation continued the remaining gaseous CO2 is subsequently enriched in 13C and 18O causing later formed calcite to be isotopically heavier along the setting path in the matrix. Deviations from such an ideal isotopic behaviour may be due to the evolution of H2O, e.g. evaporation, the source of CO2, e.g. from biogenic origin, relicts of the natural limestone, and secondary effects, such as recrystallization of calcite. The results of the field and experimental study suggest that isotope values can be used as overall proxies to decipher the origin of carbonate and the formation conditions of calcite in the matrix of ancient and recent lime mortar and plaster. Moreover, these proxies can be used to select calcite matrix from historical lime mortar and plaster for 14C dating.  相似文献   

12.
Late Pleistocene terrestrial climate records in India may be preserved in oxygen and carbon stable isotopes in pedogenic calcrete. Petrography shows that calcrete nodules in Quaternary sediments of the Thar Desert in Rajasthan are pedogenic, with little evidence for postpedogenic alteration. The calcrete occurs in four laterally persistent and one nonpersistent eolian units, separated by colluvial gravel. Thermoluminescence and infrared- and green-light-stimulated luminescence of host quartz and feldspar grains gave age brackets for persistent eolian units I–IV of ca. 70,000–60,000, ca. 60,000–55,000, ca. 55,000–43,000, and ca. 43,000–25,000 yr, respectively. The youngest eolian unit (V) is <10,000 yr old and contains no calcrete. Stable oxygen isotope compositions of calcretes in most of eolian unit I, in the upper part of eolian unit IV, and in the nonpersistent eolian unit, range between −4.6 and −2.1‰ PDB. These values, up to 4.4‰ greater than values from eolian units II and III, are interpreted as representing nonmonsoonal18O-enriched “normal continental” waters during climatic phases when the monsoon weakened or failed. Conversely, 25,000–60,000-yr-old calcretes (eolian units II and III) probably formed under monsoonal conditions. The two periods of weakened monsoon are consistent with other paleoclimatic data from India and may represent widespread aridity on the Indian subcontinent during isotope stages 2 and 4. The total variation in δ13C is 1.7‰ (0.0–1.7‰), and δ13C covaries positively and linearly with δ18O. δ13C values are highest when δ18O values indicate the most arid climatic conditions. This is best explained by expansion of C4grasses at the expense of C3plants at low latitudes during glacial periods when atmosphericpCO2was lowered. C4dominance was overridingly influenced by global change in atmosphericpCO2despite the lowered summer rainfall.  相似文献   

13.
H2S and CO2 are found in elevated concentrations in the reservoirs near the Carboniferous–Ordovician unconformity in the Hetianhe Field of the Tarim Basin, NW China. Chemical and isotopic analyses have been performed on produced gases, formation waters and reservoir rocks to determine the origin of CO2 and H2S and to explain the heterogeneous distribution of isotopic and geochemical characteristics of petroleum fluids. It is unlikely that H2S and CO2 had a mantle component since associated helium has an isotope ratio totally uncharacteristic of this source. Instead, H2S and CO2 are probably the result of sulphate reduction of the light hydrocarbon gases (LHG). Increasing H2S concentrations and CO2/(CO2+ΣC1–4) values to the west of the Hetianhe Field occur commensurately with increasingly heavy hydrocarbon gas δ13C values. However, thermochemical sulphate reduction is unlikely because the temperatures of the reservoirs are too low, no H2S or rare pyrite was detected in deeper reservoirs (where more TSR should have occurred) and inferred δ34S values of H2S (from late-stage pyrite in the Carboniferous and Ordovician reservoirs) are as low as −24.9‰. Such low δ34S values discount the decomposition of organic matter as a major source of H2S and CO2. Bacterial sulphate reduction of the light hydrocarbon gases in the reservoir, possibly coupled indirectly with the consumption of organic acids and anions is most likely. The result is the preferential oxidation of 12C-rich alkanes (due to the kinetic isotope effect) and decreasing concentration of organic acids and anions. Modern formation water stable isotope data reveal that it is possible that sulphate-reducing bacteria were introduced into the reservoir by an influx of meteoric water from the west by way of an inversion-related unconformity. This may account for the apparently stronger influence of bacterial sulphate reduction to the west of the Hetianhe Field, and the consequent greatest decrease of the δ13C-CO2 values and the greatest increase in δ13C values of the alkane gases.  相似文献   

14.
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   

15.
Variations in the carbon isotopic composition (δ13C) of pristane, phytane, n-heptadecane (n-C17), C29 ααα 20R sterane, and aryl isoprenoids provide evidence for a diverse community of algal and bacterial organisms in organic matter of the Upper Ordovician Maquoketa Group of the Illinois Basin. Carbon isotopic compositions of pristane and phytane from the Maquoketa are positively covariant (r = 0.964), suggesting that these compounds were derived from a common source inferred to be primary producers (algae) from the oxygenated photic zone. A variation of 3‰ in δ13C values (−31 to −34‰) for pristane and phytane indicates that primary producers utilized variable sources of inorganic carbon. Average isotopic compositions of n-C17 (−32‰) and C29 ααα 20R sterane (−31‰) are enriched in 13C relative to pristane and phytane (−33‰) suggesting that these compounds were derived from a subordinate group of primary producers, most likely eukaryotic algae. In addition, a substantial enrichment of 13C in aryl isoprenoids (−14 to −18‰) and the identification of tetramethylbenzene in pyrolytic products of Maquoketa kerogen indicate a contribution from photosynthetic green sulfur bacteria to the organic matter. The presence of anaerobic, photosynthetic green sulfur bacteria in organic matter of the Maquoketa indicates that anoxic conditions extended into the photic zone.The δ13C of n-alkanes and the identification of an unusual suite of straight-chain n-alkylarenes in the m/z 133 fragmentograms of Ordovician rocks rich in Gloeocapsomorpha prisca (G. prisca) indicate that G. prisca did not contribute to the organic matter of the Maquoketa Group.  相似文献   

16.
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   

17.
For the ammonia-oxidizing bacterium Nitrosomonas europaea, grown autotrophically using semicontinuous culturing, average biomass was depleted in 13C relative to CO2 dissolved in the medium by ca. 20‰ and the total-lipid extract was depleted in 13C relative to biomass by 3.7‰. The n-alkyl lipids (weighted average of fatty acids) and isoprenoid lipids (weighted average of hopanoids) were both depleted in 13C relative to biomass by about 9‰. The large depletion in the isoprenoid lipids seems to indicate that isotopic fractionations associated with the biosynthesis of methylerythritol phosphate (MEP) affected at least two carbon positions in each isoprene unit. Among the fatty acids, trans-9-hexadecenoic acid was most depleted (13.0‰ relative to biomass), followed by cis-9- hexadecenoic acid (9.6‰) and hexadecanoic acid (6.9‰). Isotopic relationships between the three acids suggest that significant isotope effects were associated with the desaturation and cis to trans isomerization of fatty acids. Given these observations, hopanoids produced by ammonia-oxidizing bacteria growing in natural waters are likely to be depleted in 13C by 26–30‰ relative to dissolved CO2. Since CO2 at aquatic oxyclines is often depleted in 13C, the range of δ values expected for hopanoids is ca. −34‰ to −55‰. The δ values of geohopanoids observed in numerous studies and attributed to unspecified chemoautotrophs fall within this range.  相似文献   

18.
Twenty two samples of calcretes from seven depth-profiles in the Menindee catchment, Broken Hill region, Australia were analysed for their inorganic and organic carbon contents and inorganic carbon and oxygen isotopes. The organic carbon content is very low (from 0.06 to 0.31 wt.%) while inorganic carbon (carbonate) is up to 3.9 wt.%. Both δ13C and δ18O become more positive closer to the surface. Carbon isotopes vary from − 8.5‰ to −5.5‰ PDB. Oxygen isotopes vary from − 6‰ to − 1.8‰ V-PDB. Depth-related δ13C and δ18O variations correlate over at least 15 km and show no significant variation along the flow path. δ13C values increase by 3‰ and δ18O values increase by 4‰ with decreasing depth in a 1.40 m thick soil profile. The variation is interpreted to indicate an increasingly elevated air temperature, greater water stress and subsequently an aridification of the area through time. The Broken Hill calcrete data confirm that climatic evolution can be deduced from isotopic series and be applied successfully to the Broken Hill region.  相似文献   

19.
A reversal of the conventional carbon isotope relationship, “terrestrial-lighter-than-marine” organic matter, has been documented for two Pennsylvanian (Desmoinesian) cyclothemic sequence cores from the Midcontinent craton of the central United States. “Deep” water organic-rich phosphatic black shales contain a significant proportion of algal-derived marine organic matter (as indicated by organic petrography, Rock-Eval hydrogen index and ratios) and display the lightest δ13C-values (max −27.80‰ for kerogen) while shallower water, more oxic facies (e.g. fossiliferous shales and limestones) contain dominantly terrestrial organic matter and have heavier δ13Ckerogen-values (to −22.87‰ for a stratigraphically adjacent coal). δ13C-values for extract fractions were relatively homogeneous for the organic-rich black shales with the lightest fraction (often the aromatics) being only 1‰, or less, more negative than the kerogen. Differences between extract fractions and kerogens were much greater for oxic facies and coals (e.g. saturates nearly 5‰ lighter than the kerogen).A proposed depositional model for the black shales calls upon a large influx of nutrients and humic detritus to the marine environment from the laterally adjacent, extremely widespread Pennsylvanian (peat) swamps which were rapidly submerged by transgression of the epicontinental seas. In this setting marine organisms drew upon a CO2-reservoir which was in a state of disequilibrium with the atmosphere, being affected by isotopically light “recycled-CO2” derived from the decomposition of peaty material in the water column and possibly from the anoxic diagenesis of organic matter in the sediments.  相似文献   

20.
The Changkeng Au and Fuwang Ag deposits represent an economically significant and distinct member of the Au–Ag deposit association in China. The two deposits are immediately adjacent, but the Au and Ag orebodies separated from each other. Ores in the Au deposit, located at the upper stratigraphic section and in the southern parts of the orefield, contain low Ag contents (< 11 ppm); the Ag orebodies, in the lower stratigraphic section, are Au-poor (< 0.2 ppm). Changkeng is hosted in brecciated cherts and jasperoidal quartz and is characterized by disseminated ore minerals. Fuwang, hosted in the Lower Carboniferous Zimenqiao group bioclastic limestone, has vein and veinlet mineralization associated with alteration comprised of quartz, carbonate, sericite, and sulfides. Homogenization temperatures of fluid inclusions from quartz veinlets in the Changkeng and Fuwang deposits are in the range of 210 ± 80 °C and 230 ± 50 °C, respectively. Salinities of fluid inclusions from the two deposits range from 1.6 to 7.3 wt.% and 1.6 to 2.6 wt.% equiv. NaCl, respectively. The δDH2O, δ18OH2O, δ13CCO2 and 3He/4He values of the fluid inclusions from the Changkeng deposit range from − 80‰ to − 30‰, − 7.8‰ to − 3.0‰, − 16.6‰ to − 17.0‰ and 0.0100 to 0.0054 Ra, respectively. The δDH2O, δ18OH2O, δ13CCO2 and 3He/4He values of fluid inclusions from the Fuwang deposit range from − 59‰ to − 45‰, − 0.9‰ to 4.1‰, − 6.7‰ to − 0.6‰ and 0.5930 to 0.8357 Ra, respectively. The δDH2O, δ18OH2O, δ13CCO2 and 3He/4He values of the fluid inclusions suggest the ore fluids of the Changkeng Au-ore come from the meteoric water and the ore fluids of the Fuwang Ag-ore are derived from mixing of magmatic water and meteoric water. The two deposits also show different Pb-isotopic signatures. The Changkeng deposit has Pb isotope ratios (206Pb/204Pb: 18.580 to 19.251, 207Pb/204Pb: 15.672 to 15.801, 208Pb/204Pb: 38.700 to 39.104) similar to those (206Pb/204Pb: 18.578 to 19.433, 207Pb/204Pb: 15.640 to 15.775, 208Pb/204Pb: 38.925 to 39.920) of its host rocks and different from those (206Pb/204Pb: 18.820 to 18.891, 207Pb/204Pb: 15.848 to 15.914, 208Pb/204Pb: 39.579 to 39.786) of the Fuwang deposit. The different signatures indicate different sources of ore-forming material. Rb–Sr isochron age (68 ± 6 Ma) and 40Ar–39Ar age (64.3 ± 0.1 Ma) of the ore-related quartz veins from the Ag deposit indicate that the Fuwang deposit formed during the Cenozoic Himalayan tectonomagmatic event. Crosscutting relationships suggests that Au-ore predates Ag-ore. The adjacent Changkeng and Fuwang deposits could, however, represent a single evolved hydrothermal system. The ore fluids initially deposited Au in the brecciated siliceous rocks, and then mixing with the magmatic water resulted in Ag deposition within fracture zones in the limestone. The deposits are alternatively the product of the superposition of two different geological events. Age evidence for the Fuwang deposit, together with the Xiqiaoshan Tertiary volcanic-hosted Ag deposit in the same area, indicates that the Pacific Coastal Volcanic Belt in the South China Fold Belt has greater potential for Himalayan precious metal mineralization than previous realized.  相似文献   

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