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1.
Hydrocarbon compositions and δ13C values for methane of fourteen natural seep gases and four underwater vents in the northwestern Gulf of Mexico are reported. The C1/(C2 + C3) ratios of the seep gas samples ranged from 68 to greater than 1000, whereas δPDB13C values varied from ?39.9 to ?65.5‰. Compositions suggest that eleven of the natural gas seeps are produced by microbial degradation whereas the remaining three have a significant thermocatalytically produced component. Contradictions in the inferences drawn from molecular and isotopic compositions make strict interpretation of the origins of a few of the samples impossible.  相似文献   

2.
Three physical quantities define the essentials of the cosmic ray exposure history of a sample of an iron meteorite: (1) the cosmic ray exposure age T, (2) the pre-atmospheric “size” S of the irradiated body, and (3) the location, i.e. the “depth” D, of the samples within the body. To establish these quantities for a given sample three independent quantities must be determined experimentally. In the present work T is ascertained by the 41K/40K method and the 4He and 21Ne concentrations (C4 and C21) are measured by the isotope dilution method. Signer and Nier's evaluation of the rare gas distribution in the meteorite Grant and the measured exposure age for this meteorite provide the relationships allowing to ascertain for any meteorite the quantities S and D from the 21Ne production rate (P21 = C21/T) and the 4He/21Ne ratio.Earlier measurements have provided data on the isotopic composition of potassium in 74 different iron meteorites. New rare gas measurements are reported for some 40 samples. Results on the age, size and depth are obtained for almost 60 samples. These data suggest that Signer and Nier's model is well suited for describing not only the rare gas distribution in a single selected meteorite (Grant) but also the exposure histories of the great majority of all irons. For a few samples, however, secondary breakups of the meteoroid and a two- or multiple-stage irradiation must be invoked. Further measurements are proposed for testing and, possibly, refining the still somewhat uncertain relationships between the abundances of cosmogenic nuclides and the quantities T, S, and D in very large meteorites.Histograms are presented showing the age distributions for irons of different chemical groups and of different size ranges.The feasibility and the relative merits of other methods for the determination of T, S, and D are discussed.  相似文献   

3.
According to gas compositional and carbon isotopic measurement of 114 gas samples from the Kuqa depression, accumulation of the natural gases in the depression is dominated by hydrocarbon gases, with high gas dryness (C1/C1–4) at the middle and northern parts of the depression and low one towards east and west sides and southern part. The carbon isotopes of methane and its homologues are relatively enriched in 13C, and the distributive range of δ 13C1, δ 13C2 and δ 13C3 is ?32‰–?36‰, ?22‰–?24‰ and ?20‰–?22‰, respectively. In general, the carbon isotopes of gaseous alkanes become less negative with the increase of carbon numbers. The δ 13 \(C_{CO_2 } \) value is less than ?10‰ in the Kuqa depression, indicating its organogenic origin. The distributive range of 3He/4He ratio is within n × 10?8 and a decrease in 3He/4He ratio from north to south in the depression is observed. Based on the geochemical parameters of natural gas above, natural gas in the Kuqa depression is of characteristics of coal-type gas origin. The possible reasons for the partial reversal of stable carbon isotopes of gaseous alkanes involve the mixing of gases from one common source rock with different thermal maturity or from two separated source rock intervals of similar kerogen type, multistages accumulation of natural gas under high-temperature and over-pressure conditions, and sufficiency and diffusion of natural gas.  相似文献   

4.
A new technique for high-precision isotopic analyses of Ni was developed and applied to terrestrial samples, Allende inclusions and materials from other meteorites. Most of the Allende inclusions analysed here were previously reported to contain isotopically anomalous Ti. In contrast, the Ni isotopic abundances are indistinguishable from normal within presently obtainable precision with only one possible exception. The latter inclusion was shown by others to contain a significantly fractionated magnesium isotopic pattern of 9‰/amu. A normal Ni isotopic pattern has also been observed for the chromite/carbon fraction of an Allende acid residue which is known to contain heavy noble gases of highly anomalous isotopic composition. All other meteoritic samples analysed (Khohar matrix and chondrules, Murray matrix, a Tieschitz chondrule and an Orgueil magnetic fraction) also show normal isotopic compositions of Ni; no evidence for effects from now extinct60Fe could be detected. In spite of ubiquitous isotopic anomalies in Ti from normal Allende inclusions, there is no signature of isotopic variations in Ni from the same samples. Possible constraints for the nucleosynthesis of iron peak elements and for astrophysical and cosmochemical conditions during formation of the solar system are discussed.  相似文献   

5.
Individual vertical profiles and north-south sections for the distribution of theδ13C of total dissolved inorganic carbon are presented for the Atlantic stations of the GEOSECS program. In most cases theδ13C data parallel the distribution of dissolved O2. Differences are attributed to in-situ oxidation of organic matter and dissolution of particles of CaCO3. Antarctic Bottom and Intermediate Waters have aδ13C value of near 0.5‰ relative to the PDB isotopic standard. The lowest values in the Atlantic ocean were found in the Antarctic Circumpolar waters which haveδ13C values as low as 0.2‰. The core of the North Atlantic Deep Water has aδ13C value of 1.0‰.  相似文献   

6.
Natural gases discovered up to now in Lishui Sag, the East China Sea Basin, differ greatly in gaseous compositions, of which hydrocarbon gases amount to 2%–94% while non-hydrocarbon gases are dominated by CO2. Their hydrocarbon gases, without exception, contain less than 90% of methane and over 10% of C2 + heavier hydrocarbons, indicating a wet gas. Carbon isotopic analyses on these hydrocarbon gases showed that δ 13C1, δ 13C2 and δ 13C3 are basically lighter than ?44‰, ?29‰ and ?26‰, respectively. The difference in carbon isotopic values between methane and ethane is great, suggesting a biogenic oil-type gas produced by the mixed organic matter at peak generation. δ 13 \(C_{CO_2 } \) values of nonhydrocarbon gases are all heavier than ?10‰, indicating a typical abiogenic gas. The simulation experiment on hydrocarbon generation of organic matter in a closed gold-tube system showed that the proportion of methane in natural gases produced by terrigenous organic matter in the Lingfeng Formation marine deposit is obviously higher than that in natural gases derived from the aquatic and terrigenous mixed organic matter in the Yueguifeng Formation lacustrine deposit, consequently the proportion of heavier hydrocarbons of the former is remarkably lower than that of the latter. Moreover, δ 13C1 values of natural gases produced by terrigenous organic matter in the Lingfeng Formation marine deposit are about 5‰ heavier than those of natural gases derived from the aquatic and terrigenous mixed organic matter in the Yueguifeng Formation lacustrine deposit while δ 13C2 and δ 13C3 values of the former are over 9‰ heavier than those of the latter. Currently the LS36-1 oil-gas pool is the only commercial oil-gas reservoir in Lishui Sag, where carbon isotopic compositions of various hydrocarbon components differ greatly from those of natural gases produced by the Lingfeng Formation organic matter but are very similar to those of natural gases derived from the Yueguifeng Formation organic matter, therefore, natural gases in the LS36-1 oil-gas pool are mainly derived from the Yueguifeng Formation lacustrine source rock rather than the Lingfeng Formation marine or Mingyuefeng Formation coal-measures source rocks.  相似文献   

7.
The potential for trichloroethene (TCE) biodegradation in a fractured dolomite aquifer at a former chemical disposal site in Smithville, Ontario, Canada, is assessed using chemical analysis and TCE and cis‐DCE compound‐specific isotope analysis of carbon and chlorine collected over a 16‐month period. Groundwater redox conditions change from suboxic to much more reducing environments within and around the plume, indicating that oxidation of organic contaminants and degradation products is occurring at the study site. TCE and cis‐DCE were observed in 13 of 14 wells sampled. VC, ethene, and/or ethane were also observed in ten wells, indicating that partial/full dechlorination has occurred. Chlorine isotopic values (δ37Cl) range between 1.39 to 4.69‰ SMOC for TCE, and 3.57 to 13.86‰ SMOC for cis‐DCE. Carbon isotopic values range between ?28.9 and ?20.7‰ VPDB for TCE, and ?26.5 and ?11.8‰ VPDB for cis‐DCE. In most wells, isotopic values remained steady over the 15‐month study. Isotopic enrichment from TCE to cis‐DCE varied between 0 and 13‰ for carbon and 1 and 4‰ for chlorine. Calculated chlorine‐carbon isotopic enrichment ratios (?Cl/?C) were 0.18 for TCE and 0.69 for cis‐DCE. Combined, isotopic and chemical data indicate very little dechlorination is occurring near the source zone, but suggest bacterially mediated degradation is occurring closer to the edges of the plume.  相似文献   

8.
The light hydrocarbon composition of 209 natural gas samples and individual light hydrocarbon carbon isotopes of 53 natural gas samples from typical humic-sourced gas and sapropelic-sourced gas in the four basins of China have been determined and analyzed. Some identification parameters for humic-sourced gas and sapropelic-sourced gas are proposed or corrected. The differences of compound-specific δ 13C value of individual light hydrocarbon between humic-sourced gas and sapropelic-sourced gas have been founded. The humic-sourced gas has the distribution of δ 13Cbenzene> ?24‰, δ 13Ctoluene >?23‰, δ 13Ccyclohexane > ?24‰ and δ 13Cmethyl cyclohexane> ?24‰, while the sapropelic-sourced gas has the distribution of δ 13Cbenzene <?24‰, δ 13Ctoluene< ?24‰, δ 13Ccyclohexane< ?24‰ and δ 13Cmethyl cyclohexane< ?24‰. Among the components of C7 light hydrocarbon compound, such as normal heptane (nC7), methyl cyclohexane (MCH) and dimethyl cyclopentane (ΣDMCP), etc, relative contents of nC7 and MCH are influenced mainly by the source organic matter type of natural gas. Therefore, it is suggested that the gas with relative content of nC7 of more than 30% and relative content of MCH of less than 70% is sapropelic-sourced gas, while gas with relative content of nC7 of less than 35% and relative content of MCH of more than 50% is humic-sourced gas. Among components of C5–7 aliphatics, the gas with relative content of C5–7 normal alkane of more than 30% is sapropelic-sourced gas, while the gas with relative content of C5–7 normal alkane of less than 30% is humic-sourced gas. These paremeters have been suggested to identify humic-sourced gas and sapropelic-sourced gas.  相似文献   

9.
Current research efforts to explore and account for the distribution of nitrogen isotope abundances in the ancient and present-day solar wind and in meteorites often require measurement of nitrogen abundances and isotopic compositions in very small samples of rare extraterrestrial materials. Isotopic analysis of ～ 1 μg of N2 is possible with modern techniques of dynamic mass spectrometry, but even this high sensitivity is a limiting factor for certain critical samples. We have utilized a statistically operated mass spectrometer coupled to an ultrahigh vacuum gas extraction and processing system to lower this limit by approximately four orders of magnitude. Quantities of N2 ranging from ～ 100 ng to < 100 pg are measurable with permil to percent precision in isotope ratios. Nitrogen and all noble gases evolved during stepwise combustion of fine-grained matrix material separated from the Allende meteorite have been meausred simultaneously in a pilot experiment using this technique. Isotopically heavy H-Xe (CCF-Xe) and isotopically light N are co-sited in a carbonaceous carrier phase, supporting a nucleosynthetic origin for15N-depleted nitrogen in Allende. The great isotopic uniformity of trapped Ar in all carrier phases indicates that simple, physical mass fractionation in gravitational escape of volatiles from the primitive nebula cannot have played a significant role in generating the nitrogen compositions observed in solar system matter.  相似文献   

10.

Natural gases discovered up to now in Lishui Sag, the East China Sea Basin, differ greatly in gaseous compositions, of which hydrocarbon gases amount to 2%–94% while non-hydrocarbon gases are dominated by CO2. Their hydrocarbon gases, without exception, contain less than 90% of methane and over 10% of C2 + heavier hydrocarbons, indicating a wet gas. Carbon isotopic analyses on these hydrocarbon gases showed that δ 13C1, δ 13C2 and δ 13C3 are basically lighter than −44‰, −29‰ and −26‰, respectively. The difference in carbon isotopic values between methane and ethane is great, suggesting a biogenic oil-type gas produced by the mixed organic matter at peak generation. δ 13 \( C_{CO_2 } \) values of nonhydrocarbon gases are all heavier than −10‰, indicating a typical abiogenic gas. The simulation experiment on hydrocarbon generation of organic matter in a closed gold-tube system showed that the proportion of methane in natural gases produced by terrigenous organic matter in the Lingfeng Formation marine deposit is obviously higher than that in natural gases derived from the aquatic and terrigenous mixed organic matter in the Yueguifeng Formation lacustrine deposit, consequently the proportion of heavier hydrocarbons of the former is remarkably lower than that of the latter. Moreover, δ 13C1 values of natural gases produced by terrigenous organic matter in the Lingfeng Formation marine deposit are about 5‰ heavier than those of natural gases derived from the aquatic and terrigenous mixed organic matter in the Yueguifeng Formation lacustrine deposit while δ 13C2 and δ 13C3 values of the former are over 9‰ heavier than those of the latter. Currently the LS36-1 oil-gas pool is the only commercial oil-gas reservoir in Lishui Sag, where carbon isotopic compositions of various hydrocarbon components differ greatly from those of natural gases produced by the Lingfeng Formation organic matter but are very similar to those of natural gases derived from the Yueguifeng Formation organic matter, therefore, natural gases in the LS36-1 oil-gas pool are mainly derived from the Yueguifeng Formation lacustrine source rock rather than the Lingfeng Formation marine or Mingyuefeng Formation coal-measures source rocks.

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11.
The expanding use of horizontal drilling and hydraulic fracturing technology to produce oil and gas from tight rock formations has increased public concern about potential impacts on the environment, especially on shallow drinking water aquifers. In eastern Kentucky, horizontal drilling and hydraulic fracturing have been used to develop the Berea Sandstone and the Rogersville Shale. To assess baseline groundwater chemistry and evaluate methane detected in groundwater overlying the Berea and Rogersville plays, we sampled 51 water wells and analyzed the samples for concentrations of major cations and anions, metals, dissolved methane, and other light hydrocarbon gases. In addition, the stable carbon and hydrogen isotopic composition of methane (δ13C‐CH4 and δ2H‐CH4) was analyzed for samples with methane concentration exceeding 1 mg/L. Our study indicates that methane is a relatively common constituent in shallow groundwater in eastern Kentucky, where methane was detected in 78% of the sampled wells (40 of 51 wells) with 51% of wells (26 of 51 wells) exhibiting methane concentrations above 1 mg/L. The δ13C‐CH4 and δ2H‐CH4 ranged from ?84.0‰ to ?58.3‰ and from ?246.5‰ to ?146.0‰, respectively. Isotopic analysis indicated that dissolved methane was primarily microbial in origin formed through CO2 reduction pathway. Results from this study provide a first assessment of methane in the shallow aquifers in the Berea and Rogersville play areas and can be used as a reference to evaluate potential impacts of future horizontal drilling and hydraulic fracturing activities on groundwater quality in the region.  相似文献   

12.
He, Ne, and Ar have been measured in seven iron meteorites for which anomalous Ag isotopic compositions were reported, in order to determine if107Ag excesses could be related to galactic cosmic-ray bombardment of these meteorites. Our results show that no correlation exists between107Ag excess and either the fluence or the energy spectrum of the particles producing spallogenic rare gases. Cosmic-ray-produced107Ag estimated from38Ar concentrations can account for only about 1% of the observed excess. Elimination of cosmic-ray bombardment as a production mechanism for107Ag excess strengthens the conclusion that the excess107Ag is the decay product of short-lived107Pd (τ1/2=6.5Myr). The iron meteorite Pin?on is shown to contain trapped rare gases with4He/20Ne～600.  相似文献   

13.
Elemental and isotopic composition of organic matter from a terrestrial sequence including the palynological Cretaceous/Tertiary (K-T) boundary together with an Ir anomaly at York Canyon, New Mexico, record information about paleoclimatological and environmental conditions. Six layers of coal, carbonaceous shale and mudstone with high contents of organic material were selected for analysis. A Late Cretaceous coal bed 10 m below the K-T boundary and an Early Tertiary coal bed containing the K-T iridium anomaly at its base were sampled intensively. In the lower bed, the isotopic ratios13C/12C,15N/14N,andD/H and the elemental ratiosC/N andN/H, all varied sympathetically with one another over depth. In contrast, in the upper coal layer, only theD/H,C/N,andN/H ratios showed some coupling. Immediately above the K-T boundary, theδ13C values displayed a long-term shift of 1.8‰ to more negative values, while the hydrogen isotope ratios in these samples did not change significantly. We interpret the covariations in both coal layers as sympathetic responses of the isotopic and elemental ratios to climatic and environmental changes, as have been observed for younger sedimentary organic matter. The long-termδ13C shift during the early Tertiary is similar to the trend observed forδ13C values of marine carbonates. Our data thus support the proposal that the carbon cycle was perturbed globally by the effects of a drastically decreased marine bioproductivity along the K-T transition. The uncoupling of variations in the climatically sensitive isotopic and elemental ratios seen in the Early Tertiary coal bed provides evidence for major geochemical and environmental changes in the York Canyon area at the end of the Mesozoic. On the other hand, the constancy of δD values in the organic matter deposited at and above the K-T boundary gives no indication of significant changes in the hydrologic/climatic regimes as recorded in theD/H ratios at the site for several thousand years following the event which produced the high Ir concentrations. Our results provide constraints on models that have been advanced to explain that event and its consequences.  相似文献   

14.
The impact of landfill contaminated groundwater along a reach of a small stream adjacent to a municipal landfill was investigated using stable carbon isotopes as a tracer. Groundwater below the stream channel, groundwater seeping into the stream, groundwater from the stream banks and stream water were sampled and analysed for dissolved inorganic carbon (DIC) and the isotope ratio of DIC (δ13CDIC). Representative samples of groundwater seeping into the stream were collected using a device (a ‘seepage well’) specifically designed for collecting samples of groundwater seeping into shallow streams with soft sediments. The DIC and δ13CDIC of water samples ranged from 52 to 205 mg C/L and ?16·9 to +5·7‰ relative to VPDB standard, respectively. Groundwater from the stream bank adjacent to the landfill and some samples of groundwater below the stream channel and seepage into the stream showed evidence of δ13C enriched DIC (δ13CDIC = ?2·3 to +5·7‰), which we attribute to landfill impact. Stream water and groundwater from the stream bank opposite the landfill did not show evidence of landfill carbon (δ13CDIC = ?10·0 to ?16·9‰). A simple mixing model using DIC and δ13CDIC showed that groundwater below the stream and groundwater seeping into the stream could be described as a mixture of groundwater with a landfill carbon signature and uncontaminated groundwater. This study suggests that the hyporheic zone at the stream–groundwater interface probably was impacted by landfill contaminated groundwater and may have significant ecological implications for this ecotone. Copyright © 2004 John Wiley & Sons, Ltd.  相似文献   

15.
Carbon and oxygen isotopic determinations have been made of 29 species of Recent Indian Ocean planktonic foraminifera. Fourteen core-top samples were used and as many as 18 species were chosen from a single core-top sample. The δ13C of the foraminifera was compared with that of total dissolved CO2 (ΣCO2) and of calcite precipitated in isotopic equilibrium with ΣCO2. The foraminiferal calcite is always at least 1.2‰ less than the value estimated for equilibrium calcite. This carbon isotopic disequilibrium suggests the partial utilization of13C-depleted metabolic CO2. The calcite tests of several species, however, have δ13C values which are similar to the δ13C of ΣCO2 in seawater. This relationship suggests that important paleohydrographic information may be obtained from carbon isotope records based on analyses of several foraminiferal species from single deep-sea sediment samples.  相似文献   

16.
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17.
Organic carbon isotope(δ13Corg) data from two well-preserved sections across a shallow-to-deep water transect of the late Ediacaran-Early Cambrian Yangtze Platform in South China show significant temporal and spatial variations. In the shallow-water Jiulongwan-Jijiapo section, δ13Corg values of the late Ediacaran Dengying Formation range from -29‰ to -24‰. In the deep-water Longbizui section, δ13Corg values from time-equivalent strata of the Dengying Formation are mostly between –35‰ and -32‰. These new data, in combination with δ13Corg data reported from other sections in South China, reveal a 6‰–8‰ shallow-to-deep water δ13Corg gradient. High δ13Corg values(-30‰) occur mostly in shallow-water carbonate rocks, whereas low δ13Corg values(-32‰) dominate the deep-water black shale and chert. The large temporal and spatial δ13Corg variations imply limited buffering effect from a large dissolved organic carbon(DOC) reservoir that was inferred to have existed in Ediacaran-Early Cambrian oceans. Instead, δ13Corg variations between platform and basin sections are more likely caused by differential microbial biomass contribution to total organic matter. High δ13Corg values(-30‰) documented from shallow-water carbonates are within the range of typical Phanerozoic δ13Corg data and may record the isotope signature of organic matter from primary(photosynthetic) production. In contrast, low δ13Corg values(-32‰) from deep-water sections may have resulted from higher chemoautotrophic or methanotrophic biomass contribution to bulk organic matter in anoxic environments. The δ13Corg data provide indirect evidence for ocean stratification and episodic chemocline fluctuations in the Ediacaran-Early Cambrian Yangtze Platform.  相似文献   

18.
Closely spaced samples (285 in number) of varved sediments from the Upper Permian in Delaware Basin, Texas, have been analyzed for δ13Ccarb, δ13Corg, δ18Ocarb, Corg, Ccarb, and calcite/dolomite. δ13C records a dramatic rise from ?2.8 to +5.7‰ in only 4400 years, detected in three sections across the basin, extrapolating smoothly through a 600-year interruption by a local (west side of the basin) fresh-water inflow evidenced by low δ18O. This continuity and low Corg within the basin, both indicate that the excess net deposition of Corg, necessary to generate the rise in δ13C, took place in the ocean external to the Delaware Basin. Correlation with similar records from the Zechstein Basin suggest that the event was world-wide, although this poses obvious difficulties for the carbon cycle. The rate of rise of δ13C, and its sustained high level, must imply conversions of oxidized carbon to reduced carbon that are very large depending on which reservoirs were involved.  相似文献   

19.
A theoretical model is derived in which isotopic fractionations can be calculated as a function of variations in dissolved carbonate species on CO2 degassing and calcite precipitation. This model is tested by application to a calcite-depositing spring system near Westerhof, Germany. In agreement with the model,13C of the dissolved carbonate species changes systematically along the flow path. The difference in δ values between the upper and lower part of the stream is about 1‰. The13C content of the precipitated calcite is different from that expected from the theoretical partitioning. The isotopic composition of the solid CaCO3 is similar to that of the dissolved carbonate, though in theory it should be isotopically heavier by about 2.4‰. The18O composition of dissolved carbonate and H2O is constant along the stream. Calculated calcite-water temperatures differ by about +5°C from the observed temperatures demonstrating isotopic disequilibrium between the water and precipitated solid. This is attributed to kinetic effects during CaCO3 deposition from a highly supersaturated solution, in which precipitation is faster than equilibration with respect to isotopes.Plant populations in the water have virtually no influence on CO2 degassing, calcite saturation and isotopic fractionation. Measurements of PCO2, SC and13C within a diurnal cycle demonstrate that metabolic effects are below the detection limit in a system with a high supply-rate of dissolved carbonate species. The observed variations are due to differences in CO2 degassing and calcite precipitation, caused by continuously changing hydrodynamic conditions and carbonate nucleation rates.  相似文献   

20.
Non-dispersive infrared(NDIR) and cavity ring-down spectroscopy(CRDS) CO_2 analyzers use 12CO_2 isotopologue absorption lines and are insensitive to all or part of other CO_2-related isotopologues. This may produce biases in CO_2 mole fraction measurements of a sample if its carbon isotopic composition deviates from that of the standard gases being used. To evaluate and compare the effects of carbon isotopic composition on NDIR and CRDS CO_2 analyzers, we prepared three test sample air cylinders with varying carbon isotopic abundances and calibrated them against five standard cylinders with ambient carbon isotopic composition using CRDS and NDIR systems. We found that the CO_2 mole fractions of the sample cylinders measured by G1301(CRDS) were in good agreement with those measured by Lo Flo(NDIR). The CO_2 values measured by both instruments were higher than that of a CO_2 isotope measured by G2201i(CRDS) analyzer for a test cylinder with depleted carbon isotopic composition δ~(13)C =-36.828‰, whereas no obvious difference was found for other two test cylinders with δ~(13)C=-8.630‰ and δ~(13)C=-15.380‰, respectively. According to the theoretical and experimental results, we concluded that the total CO_2 mole fractions of samples with depleted isotopic compositions can be corrected on the basis of their 12CO_2 values calibrated by standard gases using Lo Flo and G1301 if the δ~(13)C and δ18O values are known.  相似文献   

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