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1.
《Organic Geochemistry》2012,42(12):1277-1284
Compound-specific isotope measurements of organic compounds are increasingly important in palaeoclimate reconstruction. Searching for more accurate peat-based palaeoenvironmental proxies, compound-specific fractionation of stable C, H and O isotopes of organic compounds synthesized by Sphagnum were determined in a greenhouse study. Three Sphagnum species were grown under controlled climate conditions. Stable isotope ratios of cellulose, bulk organic matter (OM) and C21–C25 n-alkanes were measured to explore whether fractionation in Sphagnum is species-specific, as a result of either environmental conditions or genetic variation. The oxygen isotopic composition (δ18O) of cellulose was equal for all species and all treatments. The hydrogen isotopic composition (δD) of the n-alkanes displayed an unexpected variation among the species, with values between −154‰ for Sphagnum rubellum and −184‰ for Sphagnum fallax for the C23 n-alkane, irrespective of groundwater level. The stable carbon isotopic composition (δ13C) of the latter also showed a species-specific pattern. The pattern was similar for the carbon isotope fractionation of bulk OM, although the C23 n-alkane was >10‰ more depleted than the bulk OM. The variation in H fractionation may originate in the lipid biosynthesis, whereas C fractionation is also related to humidity conditions. Our findings clearly emphasize the importance of species identification in palaeoclimate studies based on stable isotopes from peat cores.  相似文献   

2.
《Organic Geochemistry》2012,42(12):1269-1276
This study sought to characterize hydrogen isotopic fractionation during biosynthesis of leaf wax n-alkanes in succulent plants capable of crassulacean acid metabolism (CAM). The metabolic and physiological features of CAM represent crucial strategies for survival in hot and dry climates and have been hypothesized to impact hydrogen isotope fractionation. We measured the stable carbon and hydrogen isotopic compositions (δ13C and δD, respectively) of individual n-alkanes in 20 species of succulent plants from a global collection of the Huntington Botanical Gardens, San Marino, California. Greenhouse conditions and irrigation with water of constant δD value enabled determination of interspecies differences in net D/H fractionation between source water and leaf wax products. Carbon isotope ratios provide constraints on the extent of CAM vs. C3 photosynthesis and indicate a wide range of CAM use, with δ13C values ranging from −33.01‰ to −18.54‰ (C27–C33 n-alkanes) and −26.66‰ to −17.64‰ (bulk tissue). Despite the controlled growth environment, we observed ca. 90‰ interspecies range in δD values from −193‰ to −107‰. A positive correlation between δ13Cbulk and δDC31 values with R2 = 0.60 (δ13CC31 and δDC31 values with R2 = 0.41) implicates a metabolic isotope effect as the dominant cause of interspecies variation in the hydrogen isotopic composition of leaf wax n-alkanes in CAM-intermediate plants.  相似文献   

3.
Biodegradation is one of the main natural attenuation processes in groundwater contaminated with petroleum hydrocarbons. In this work, preliminary studies have been carried out by analyzing the concentrations of total petroleum hydrocarbons (TPH), dissolved inorganic carbon (DIC), dominant terminal electron accepters or donors, as well as δ 13CDIC and δ 34SSO4, to reveal the biodegradation mechanism of petroleum hydrocarbons in a contaminated site. The results show that along groundwater flow in the central line of the plume, the concentrations of electron acceptors, pH, and E h increased but TPH and DIC decreased. The δ 13CDIC values of the contaminated groundwater were in the range of ?14.02 to ?22.28 ‰PDB and ?7.71 to 8.36 ‰PDB, which reflected a significant depletion and enrichment of 13C, respectively. The increase of DIC is believed to result from the non-methanogenic and methanogenic biodegradation of petroleum hydrocarbon in groundwater. Meanwhile, from the contaminated source to the downgradient of the plume, the 34S in the contaminated groundwater became more depleted. The Rayleigh model calculation confirmed the occurrence of bacterial sulfate reduction as a biodegradation pathway of the petroleum hydrocarbon in the contaminated aquifers. It was concluded that stable isotope measurements, combined with other biogeochemical measurements, can be a useful tool to prove the occurrence of the biodegradation process and to identify the dominant terminal electron-accepting process in contaminated aquifers.  相似文献   

4.
An existing method of detecting microgas seeps was applied in a free soil gas investigation above the Löningen oilfield, NW-Germany. Simple gas surveying was combined with sampling of soil gases for gas-chromatographic treatment and examination of the carbon isotopic composition. A zone of biological gas formation and an area of thermocatalytic methane were discovered, the latter probably caused by migration from the subsurface petroleum accumulation.The methane in the reservoir differs in isotopic composition depending on its origin: gas from gascap or petroleum. Methane dissolved from petroleum is depleted in 12C by about 5 ppt compared to methane from the gascap. In relation to the reservoir a general 13C-enrichment between 2.5 and 4.6 ppt is observed in the soil gas methanes which is supposedly due to isotopic fractionation during migration. The two species of reservoir methane are still distinguishable on the surface by their different composition. Gaseous hydrocarbons from C2 to C4 seem to be restricted by migration. Bacterial oxidation appears not to affect the isotopic composition of the thermocatalytic methane seriously.  相似文献   

5.
《Geochimica et cosmochimica acta》1999,63(13-14):2001-2007
Stable oxygen isotope ratios of foraminiferal calcite are widely used in paleoceanography to provide a chronology of temperature changes during ocean history. It was recently demonstrated that the stable oxygen isotope ratios in planktonic foraminifera are affected by changes of the seawater chemistry carbonate system: the δ18O of the foraminiferal calcite decreases with increasing CO32− concentration or pH. This paper provides a simple explanation for seawater chemistry dependent stable oxygen isotope variations in the planktonic foraminifera Orbulina universa which is derived from oxygen isotope partitioning during inorganic precipitation. The oxygen isotope fractionation between water and the dissolved carbonate species S = [H2CO3] + [HCO3−] + [CO32−] decreases with increasing pH. Provided that calcium carbonate is formed from a mixture of the carbonate species in proportion to their relative contribution to S, the oxygen isotopic composition of CaCO3 also decreases with increasing pH. The slope of shell δ18O vs. [CO32−] of Orbulina universa observed in culture experiments is −0.0022‰ (μmol kg−1)−1 (Spero et al., 1997), whereas the slope derived from inorganic precipitation is −0.0024‰ (μmol kg−1)−. The theory also provides an explanation of the nonequilibrium fractionation effects in synthetic carbonates described by Kim and O’Neil (1997) which can be understood in terms of equilibrium fractionation at different pH. The results presented here emphasize that the oxygen isotope fractionation between calcium carbonate and water does not only depend on the temperature but also on the pH of the solution from which it is formed.  相似文献   

6.
The photosynthetic fractionation of carbon isotopes by blue-green algae in laboratory culture is dependent in a non-linear fashion on the CO2 concentration in the feed gas. For the three species tested, the minimum fractionation occurred at a CO2 concentration of 0.2% in air and was approximately zero for the two marine species tested. Enrichment of C12 in the reduced carbon is not an inevitable result of photosynthetic carbon fixation. Temperature and pH had no detectable effect on fractionation. The maximum fractionation observed in the laboratory cultures or in recent blue-green algal mats was 18‰. Differences in the isotope ratio of coexisting oxidized and reduced carbon in Precambrian stromatolites are as great as 31‰. Present carbon isotopic evidence is not consistent with the idea that blue-green algae were major contributors to the organic matter in Precambrian sediments.  相似文献   

7.
The Deccan Syneclise is considered to have significant hydrocarbon potential.However,significant hydrocarbon discoveries,particularly for Mesozoic sequences,have not been established through conventional exploration due to the thick basalt cover over Mesozoic sedimentary rocks.In this study,near-surface geochemical data are used to understand the petroleum system and also investigate type of source for hydrocarbons generation of the study area.Soil samples were collected from favorable areas identified by integrated geophysical studies.The compositional and isotopic signatures of adsorbed gaseous hydrocarbons(methane through butane) were used as surface indicators of petroleum micro-seepages.An analysis of 75 near-surface soil-gas samples was carried out for light hydrocarbons(C1-C4) and their carbon isotopes from the western part of Tapti graben,Deccan Syneclise,India.The geochemical results reveal sites or clusters of sites containing anomalously high concentrations of light hydrocarbon gases.High concentrations of adsorbed thermogenic methane(C_1 = 518 ppb) and ethane plus higher hydrocarbons(ΣC_(2+) = 977 ppb) were observed.Statistical analysis shows that samples from 13% of the samples contain anomalously high concentrations of light hydrocarbons in the soil-gas constituents.This seepage suggests largest magnitude of soil gas anomalies might be generated/source from Mesozoic sedimentary rocks,beneath Deccan Traps.The carbon isotopic composition of methane,ethane and propane ranges are from-22.5‰ to-30.2‰ PDB,-18.0‰to 27.1‰ PDB and 16.9‰-32.1‰ PDB respectively,which are in thermogenic source.Surface soil sample represents the intersection of a migration conduit from the deep subsurface to the surface connected to sub-trappean Mesozoic sedimentary rocks.Prominent hydrocarbon concentrations were associated with dykes,lineaments and presented on thinner basaltic cover in the study area,which probably acts as channel for the micro-seepage of hydrocarbons.  相似文献   

8.
《China Geology》2020,3(4):602-610
Thirty-nine crude oils and twenty-one rock samples from Niger Delta Basin, Nigeria have been characterized based on their isotope compositions by elemental analysis-isotope ratio mass spectrometry and gas chromatography-isotope ratio mass spectrometry. The bulk carbon isotopic values of the whole rock extracts, saturate and aromatic fractions range from –28.7‰ to –26.8‰, –29.2‰ to –27.2 ‰ and –28.5 ‰ to –26.7 ‰, respectively while the bulk carbon isotopic values of the whole oils, saturate and aromatic fractions range from –25.4 ‰ to –27.8 ‰, –25.9 ‰ to –28.4 ‰ and –23.5 ‰ to –26.9 ‰, respectively. The average carbon isotopic compositions of individual alkanes (nC12-nC33) in the rock samples range from –34.9‰ to –28.2‰ whereas the average isotopic values of individual n-alkanes in the oils range from –31.1‰ to –23.8‰. The δ13C isotope ratios of pristane and phytane in the rock samples range from –29.2 ‰ to –28.2 ‰ and –30.2 ‰ to –27.4 ‰ respectively while the pristane and phytane isotopic values range from –32.1‰ to –21.9‰ and –30.5‰ to –26.9‰, respectively. The isotopic values recorded for the samples indicated that the crude oils were formed from the mixed input of terrigenous and marine organic matter and deposited under oxic to sub-oxic condition in lacustrine-fluvial/deltaic environments. The stable carbon isotopic compositions were found to be effective in assessing the origin and depositional environments of crude oils in the Niger Delta Basin.  相似文献   

9.
Equilibrium Zn isotope fractionation was investigated using first-principles quantum chemistry methods at the B3LYP/6-311G* level. The volume variable cluster model method was used to calculate isotope fractionation factors of sphalerite, smithsonite, calcite, anorthite, forsterite, and enstatite. The water-droplet method was used to calculate Zn isotope fractionation factors of Zn2+-bearing aqueous species; their reduced partition function ratio factors decreased in the order \(\left[ {{\text{Zn}}\left( {{\text{H}}_{2} {\text{O}}} \right)_{6} } \right]^{2 + } > \left[ {{\text{ZnCl}}\left( {{\text{H}}_{2} {\text{O}}} \right)_{5} } \right]^{ + } > \left[ {{\text{ZnCl}}_{2} \left( {{\text{H}}_{2} {\text{O}}} \right)_{4} } \right] > \left[ {{\text{ZnCl}}_{3} \left( {{\text{H}}_{2} {\text{O}}} \right)_{2} } \right]^{ - } > {\text{ZnCl}}_{4} ]^{2 - }\). Gaseous ZnCl2 was also calculated for vaporization processes. Kinetic isotope fractionation of diffusional processes in a vacuum was directly calculated using formulas provided by Richter and co-workers. Our calculations show that in addition to the kinetic isotope effect of diffusional processes, equilibrium isotope fractionation also contributed nontrivially to observed Zn isotope fractionation of vaporization processes. The calculated net Zn isotope fractionation of vaporization processes was 7–7.5‰, with ZnCl2 as the gaseous species. This matches experimental observations of the range of Zn isotope distribution of lunar samples. Therefore, vaporization processes may be the cause of the large distribution of Zn isotope signals found on the Moon. However, we cannot further distinguish the origin of such vaporization processes; it might be due either to igneous rock melting in meteorite bombardments or to a giant impact event. Furthermore, isotope fractionation between Zn-bearing aqueous species and minerals that we have provided helps explain Zn isotope data in the fields of ore deposits and petrology.  相似文献   

10.
Compound-specific isotope analysis has become an important tool in environmental studies and is an especially powerful way to evaluate biodegradation of hydrocarbons. Here, carbon isotope ratios of light hydrocarbons were used to characterise in-reservoir biodegradation in the Gullfaks oil field, offshore Norway. Increasing biodegradation, as characterised, for example, by increasing concentration ratios of Pr/n-C17 and Ph/n-C18, and decreasing concentrations of individual light hydrocarbons were correlated to 13C-enrichment of the light hydrocarbons. The δ13C values of C4 to C9n-alkanes increase by 7-3‰ within the six oil samples from the Brent Group of the Gullfaks oil field, slight changes (1-3‰) being observed for several branched alkanes and benzene, whereas no change (<1‰) in δ13C occurs for cyclohexane, methylcyclohexane, and toluene. Application of the Rayleigh equation demonstrated high to fair correlation of concentration and isotope data of i- and n-pentane, n-hexane, and n-heptane, documenting that biodegradation in reservoirs can be described by the Rayleigh model. Using the appropriate isotope fractionation factor of n-hexane, derived from laboratory experiments, quantification of the loss of this petroleum constituent due to biodegradation is possible. Toluene, which is known to be highly susceptible to biodegradation, is not degraded within the Gullfaks oil field, implying that the local microbial community exhibits rather pronounced substrate specificities. The evaluation of combined molecular and isotopic data expands our understanding of the anaerobic degradation processes within this oil field and provides insight into the degradative capabilities of the microorganisms. Additionally, isotope analysis of unbiodegraded to slightly biodegraded crude oils from several oil fields surrounding Gullfaks illustrates the heterogeneity in isotopic composition of the light hydrocarbons due to source effects. This indicates that both source and also maturity effects have to be well constrained when using compound-specific isotope analysis for the assessment of biodegradation.  相似文献   

11.
The stable hydrogen isotopic compositions (δD) of selected aliphatic hydrocarbons (n-alkanes and isoprenoids) in eight crude oils of similar source and thermal maturity from the Upper Indus Basin (Pakistan) were measured. The oils are derived from a source rock deposited in a shallow marine environment. The low level of biodegradation under natural reservoir conditions was established on the basis of biomarker and aromatic hydrocarbon distributions. A plot of pristane/n-C17 alkane (Pr/n-C17) and/or phytane/n-C18 alkane (Ph/n-C18) ratios against American Petroleum Institute (API) gravity shows an inverse correlation. High Pr/n-C17 and Ph/n-C18 values and low API gravity values in some of the oils are consistent with relatively low levels of biodegradation. For the same oils, δD values for the n-alkanes relative to the isoprenoids are enriched in deuterium (D). The data are consistent with the removal of D-depleted low molecular weight (LMW) n-alkanes (C14–C22) from the oils. The δD values of isoprenoids do not change with progressive biodegradation and are similar for all the samples. The average D enrichment for n-alkanes with respect to the isoprenoids is found to be as much as 35‰ for the most biodegraded sample. For example, the moderately biodegraded oils show an unresolved complex mixture (UCM), loss of LMW n-alkanes (<C15) and moderate changes in the alkyl naphthalene distributions. The relative susceptibility of alkyl naphthalenes at low levels of biodegradation is discussed. The alkyl naphthalene biodegradation ratios were determined to assess the effect of biodegradation. The dimethyl, trimethyl and tetramethyl naphthalene biodegradation ratios show significant differences with increasing extent of biodegradation.  相似文献   

12.
This paper reports the isotope effects in an open-system Fischer-Tropsch type (FTT) synthesis, with implications for the origin of natural abiogenic hydrocarbons. The starting form of carbon was CO2, with carbon and hydrogen isotopic compositions measured for products of catalytic hydrogenation of CO2 on iron and cobalt catalysts (FTCO2-Fe and FTCO2-Co) at 350 and 245 °C, respectively, and 10 MPa. The carbon isotopic composition of the resulting saturated hydrocarbons (alkanes) as a function of carbon number shows a positive trend for both FTCO2-Fe and FTCO2-Co, with a fractionation of 2-4‰ and 3-6‰ between CH4 and C2H6 over the Fe and Co catalysts, respectively. The unsaturated hydrocarbons (alkenes) do not show any trend. A strong kinetic isotope fractionation (>40‰) occurred between CO2 and CH4 in both experiments. The hydrogen isotope fractionation between alkanes appeared to be similar to that found in natural (thermogenic and biogenic) gases, with enrichment in deuterium of longer hydrocarbon chains; the dominant H/D fractionation occurred between CH4 and C2H6. Alkenes in the products of the FTCO2-Fe reaction are enriched in deuterium (∼50‰) and do not show any trend versus carbon number. We suggest that other than FTT reactions or a simple mixing are responsible for the occurrence of the inverse isotopic trends in both δ13C and δD found in light hydrocarbons in some terrestrial environments and meteorites.  相似文献   

13.
Theory is derived from the work of Urey (Urey H. C. [1947] The thermodynamic properties of isotopic substances. J. Chem. Soc. 562-581) to calculate equilibrium constants commonly used in geochemical equilibrium and reaction-transport models for reactions of individual isotopic species. Urey showed that equilibrium constants of isotope exchange reactions for molecules that contain two or more atoms of the same element in equivalent positions are related to isotope fractionation factors by α = (Kex)1/n, where n is the number of atoms exchanged. This relation is extended to include species containing multiple isotopes, for example 13C16O18O and 1H2H18O. The equilibrium constants of the isotope exchange reactions can be expressed as ratios of individual isotope equilibrium constants for geochemical reactions. Knowledge of the equilibrium constant for the dominant isotopic species can then be used to calculate the individual isotope equilibrium constants.Individual isotope equilibrium constants are calculated for the reaction CO2g = CO2aq for all species that can be formed from 12C, 13C, 16O, and 18O; for the reaction between 12C18O2aq and 1H218Ol; and among the various 1H, 2H, 16O, and 18O species of H2O. This is a subset of a larger number of equilibrium constants calculated elsewhere (Thorstenson D. C. and Parkhurst D. L. [2002] Calculation of individual isotope equilibrium constants for implementation in geochemical models. Water-Resources Investigation Report 02-4172. U.S. Geological Survey). Activity coefficients, activity-concentration conventions for the isotopic variants of H2O in the solvent 1H216Ol, and salt effects on isotope fractionation have been included in the derivations. The effects of nonideality are small because of the chemical similarity of different isotopic species of the same molecule or ion. The temperature dependence of the individual isotope equilibrium constants can be calculated from the temperature dependence of the fractionation factors.The derivations can be extended to calculation of individual isotope equilibrium constants for ion pairs and equilibrium constants for isotopic species of other chemical elements. The individual isotope approach calculates the same phase isotopic compositions as existing methods, but also provides concentrations of individual species, which are needed in calculations of mass-dependent effects in transport processes. The equilibrium constants derived in this paper are used to calculate the example of gas-water equilibrium for CO2 in an acidic aqueous solution.  相似文献   

14.
Natural gas in the Xujiahe Formation of the Sichuan Basin is dominated by hydrocarbon (HC) gas, with 78–79% methane and 2–19% C2+ HC. Its dryness coefficient (C1/C1–5) is mostly < 0.95. The gas in fluid inclusions, which has low contents of CH4 and heavy hydrocarbons (C2+) and higher contents of non-hydrocarbons (e.g. CO2), is a typical wet gas produced by thermal degradation of kerogen. Gas produced from the Upper Triassic Xujiahe Formation (here denoted field gas) has light carbon isotope values for methane (δ13C1: −45‰ to −36‰) and heavier values for ethane (δ13C2: −30‰ to −25‰). The case is similar for gas in fluid inclusions, but δ13C1 = −36‰ to −45‰ and δ13C2 = −24.8‰ to −28.1‰, suggesting that the gas experienced weak isotopic fractionation due to migration and water washing. The field gas has δ13CCO2 values of −15.6‰ to −5.6‰, while the gas in fluid inclusions has δ13CCO2 values of −16.6‰ to −9‰, indicating its organic origin. Geochemical comparison shows that CO2 captured in fluid inclusions mainly originated from source rock organic matter, with little contribution from abiogenic CO2. Fluid inclusions originate in a relatively closed system without fluid exchange with the outside following the gas capture process, so that there is no isotopic fractionation. They thus present the original state of gas generated from the source rocks. These research results can provide a theoretical basis for gas generation, evolution, migration and accumulation in the basin.  相似文献   

15.
We have developed a new approach to quantitatively reconstruct past changes in evaporation based on compound-specific hydrogen isotope ratios of vascular plant and Sphagnum biomarkers in ombrotrophic peatland sediments. We show that the contrast in H isotopic ratios of water available to living Sphagnum (top 20 cm) and in the rooting zone of peatland vascular plants can be used to estimate “?”—the fraction of water remaining after evaporation. Vascular plant leaf waxes record H isotopic ratios of acrotelm water, which carries the D/H ratio signature of precipitation and is little affected by evaporation, whereas the Sphagnum biomarker, C23n-alkane, records H isotopic ratios of the water inside its cells and between its leaves, which is strongly affected by evaporation at the bog surface. Evaporation changes can then be deduced by comparing H isotopic ratios of the two types of biomarkers. We calibrated D/H ratios of C23n-alkane to source water with lab-grown Sphagnum. We also tested our isotopic model using modern surface samples from 18 ombrotrophic peatlands in the Midwestern United States. Finally, we generated a 3000-year downcore reconstruction from Minden Bog, Michigan, USA. Our new record is consistent with records of other parameters from the same peatland derived from different proxies and allows us to differentiate precipitation supply and evaporative loss.  相似文献   

16.
Molecular transport (diffusion) of methane in water-saturated sedimentary rocks results in carbon isotope fractionation. In order to quantify the diffusive isotope fractionation effect and its dependence on total organic carbon (TOC) content, experimental measurements have been performed on three natural shale samples with TOC values ranging from 0.3 to 5.74%. The experiments were conducted at 90°C and fluid pressures of 9 MPa (90 bar). Based on the instantaneous and cumulative composition of the diffused methane, effective diffusion coefficients of the 12CH4 and 13CH4 species, respectively, have been calculated.Compared with the carbon isotopic composition of the source methane (δ13C1 = −39.1‰), a significant depletion of the heavier carbon isotope (13C) in the diffused methane was observed for all three shales. The degree of depletion is highest during the initial non-steady state of the diffusion process. It then gradually decreases and reaches a constant difference (Δ δ = δ13Cdiff −δ13Csource) when approaching the steady-state. The degree of the isotopic fractionation of methane due to molecular diffusion increases with the TOC content of the shales. The carbon isotope fractionation of methane during molecular migration results practically exclusively from differences in molecular mobility (effective diffusion coefficients) of the 12CH4 and 13CH4 entities. No measurable solubility fractionation was observed.The experimental isotope-specific diffusion data were used in two hypothetical scenarios to illustrate the extent of isotopic fractionation to be expected as a result of molecular transport in geological systems with shales of different TOC contents. The first scenario considers the progression of a diffusion front from a constant source (gas reservoir) into a homogeneous “semi-infinite” shale caprock over a period of 10 Ma.In the second example, gas diffusion across a 100 m caprock sequence is analyzed in terms of absolute quantities and isotope fractionation effects. The examples demonstrate that methane losses by molecular diffusion are small in comparison with the contents of commercial size gas accumulations. The degree of isotopic fractionation is related inversely to the quantity of diffused gas so that strong fractionation effects are only observed for relatively small portions of gas.The experimental data can be readily used in numerical basin analysis to examine the effects of diffusion-related isotopic fractionation on the composition of natural gas reservoirs.  相似文献   

17.
Ammonia-oxidizing archaea (AOA) are abundant and widely distributed microorganisms in aquatic and terrestrial habitats. By catalyzing the first and rate limiting step in nitrification, these chemolithoautotrophs play a significant role in the global nitrogen cycle and contribute to primary production. Here, the carbon isotopic fractionation relative to inorganic carbon source was determined for bulk biomass, biphytanes and polar lipid bound sugars of a marine AOA pure culture. Bulk biomass and biphytanes from Nitrosopumilus maritimus showed identical carbon isotope fractionation (εDIC/bulk and εDIC/byphytanes) of ca. −20‰. The glycoside head groups were mainly glucose, mannose and inositol, and exhibited different carbon isotopic composition. In general, these monosaccharides were enriched in 13C (ε −6.1‰ to −13.8‰) relative to bulk biomass and biphytanes. The fact that the carbon isotope composition of the biphytanes reflected that of the bulk biomass of N. maritimus suggests that the depletion of 13C in both biomass and biphytanes resulted mainly from the carbon isotope discrimination by the bicarbonate-fixing enzyme in the autotrophic hydroxypropionate/hydroxybutyrate cycle. Our results further revealed that lipid compounds represent suitable biomarkers for determining δ13C values of archaeal ammonia oxidizers without biosynthetic correction.  相似文献   

18.
The degradation of acyclic petroleum hydrocarbons was studied during a 24-month experiment in Mediterranean coastal sediments (Gulf of Fos). Sediment cores entirely contaminated with oil (Arabian Light Crude Oil) were incubated in situ. The use of conservative tracers of sediment's particles reworking (luminophores) allowed the distinction of the reworked layer from the anoxic deeper sediments. Using the 17α,21βC30 hopane (C30H) as an inert internal reference, we could demonstrate that, after 24 months of experiment, acyclic petroleum hydrocarbons can be degraded under natural anaerobic conditions. The reactivity of individual alkanes appeared to depend on their chemical structure. To cite this article: D. Massias et al., C. R. Geoscience 335 (2003).To cite this article: D. Massias et al., C. R. Geoscience 335 (2003).  相似文献   

19.
《Applied Geochemistry》2002,17(11):1457-1466
Ocean Drilling Program (ODP) Leg 169, which was conducted in 1996 provided an opportunity to study the gas geochemistry in the deeper part of the sediment-rich hydrothermal system in Escanaba Trough. Gas void samples obtained from the core liner were analyzed and their results were compared with analytical data of vent fluid samples collected by a submersible dive program in 1988. The gas geochemistry of the pore fluids consisted mostly of a hydrothermal component and was basically the same as that of the vent fluids. The He isotope ratios (R/RA=5.6–6.6) indicated a significant mantle He contribution and the C isotopic compositions of the hydrocarbons [δ13C(CH4)=−43‰, δ13C(C2H6)=−20‰] were characterized as a thermogenic origin caused by hydrothermal activity. On the other hand, the pore fluids in sedimentary layers away from the hydrothermal fields showed profiles which reflected lateral migration of the hydrothermal hydrocarbons and abundant biogenic CH4. Helium and C isotope systematics were shown to represent a hydrothermal component and useful as indicators for their distribution beneath the seafloor. Similarities in He and hydrocarbon signatures to that of the Escanaba Trough hydrothermal system were found in some terrestrial natural gases, which suggested that seafloor hydrothermal activity in sediment-rich environments would be one of the possible petroleum hydrocarbon generation scenarios in unconventional geological settings.  相似文献   

20.
DH and 13C12C ratios were measured for 114 petroleum samples and for several samples of related organic matter. δD of crude oil ranges from ?85 to ?181‰, except for one distillate (?250‰) from the Kenai gas field; δ13C of crude oil ranges from ?23.3 to ?32.5‰, Variation in δD and δ13C values of compound-grouped fractions of a crude oil is small, 3 and 1.1%., respectively, and the difference in δD and δ13C between oil and coeval wax is slight. Gas fractions are 53–70 and 22.6–23.2‰ depleted in D and 13C, respectively, relative to the coexisting oil fractions.The δD and δ13C values of the crude oils appear to be largely determined by the isotopic compositions of their organic precursors. The contribution of terrestrial organic debris to the organic precursors of most marine crude oils may be significant.  相似文献   

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