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1.
The carbon isotopic composition of CO2 inclusions trapped in minerals reflects the origin and evolution of CO2-bearing fluids and melts, and records the multiple-stages carbon geodynamic cycle, as CO2 took part in various geological processes widely. However, the practical method for determination isotope composition of individual CO2 inclusion is still lacking. Developing a microanalytical technique with spatial resolution in micrometers to precisely determinate the δ13C value of individual CO2 inclusion, will make it possible to analyze a tiny portion of a zoning mineral crystal, distinguish the differences in micro-scale, and possible to find many useful information that could not be obtained with the bulk extraction and analysis techniques. In this study, we systematically collected Raman spectra of CO2 standards with different δ13C values (?34.9 ‰ to 3.58 ‰) at 32.0 °C and from ～7.0 MPa to 120.0 MPa, and developed a new procedure to precisely determinate the δ13C value of individual CO2 inclusion. We investigated the relationship among the Raman peak intensity ratio, δ13C value, and CO2 density, and established a calibration model with high accuracy (0.5 ‰?1.5 ‰), sufficient for geological application to distinguish different source of CO2 with varying δ13CO2. As a demonstration, we measured the δ13C values and the density of CO2 inclusions in the growth zones of alkali basalt-hosted corundum megacrysts from Changle, Shandong Province. We found the significant differences of density and δ13C between the CO2 inclusions in the core of corundum and those inclusions in the outer growth zones, the δ13C value decreases from core to rim with decreasing density: δ13C values are from ?7.5 ‰ to ?9.2 ‰ for the inclusions in the core, indicating the corundum core was crystallized from mantle-derived magmas; from ?13.5 ‰ to ?18.5 ‰ for CO2 inclusions in zone 1 and from ?16.5 ‰ to –22.0 ‰ for inclusions in zone 2, indicating the outer zones of corundum grew in a low δ13C value environment, resulted from an infilling of low δ13C value fluid and/or degassing of the ascending basaltic magma.  相似文献   

2.
As an indicator for terrestrial paleovegetation, the stable isotopic composition of total organic matter (δ13Corg) in loess sediments has been widely used for paleoclimatic reconstruction in western Europe, the Great Plains of North America and the Chinese Loess Plateau (CLP). However, little is known about the variation and paleoclimatic significance of the loess δ13Corg in arid Central Asia (ACA). We report δ13Corg data from an Axike (AXK) loess/paleosol profile from the eastern Ili Basin, eastern Central Asia. Along the profile, the δ13Corg values were more negative in the paleosol layers observed in the field and were confirmed by environmental magnetic proxies and a higher concentration of total organic carbon (TOC), consistent with results for western Europe and the northwestern CLP. Our results demonstrate that the loess δ13Corg in this region documents mainly the response of δ13C of locally predominant C3 plants to paleoclimatic variation, especially paleoprecipitation. Our results also suggest that the loess δ13Corg values in the area have the potential for quantitative paleoprecipitation reconstruction on the basis of detailed δ13Corg results from modern plants and surface soils in the future.  相似文献   

3.
《Applied Geochemistry》2005,20(3):519-527
Pleistocene vegetation history on the Chinese Loess Plateau has been traditionally investigated using palynological methods, and questions remain regarding whether an extensive broadleaf deciduous forest ever developed on the loess table under favorable climatic conditions. The authors have employed a C isotope approach to address this question by comparing δ13C values in soil organic matter from different loess ecological domains with known source vegetation to the C isotope values obtained from a paleosol section that can be dated back to 130 ka. The C isotopic compositions of modern soils from the loess table and the loess–desert transition gave δ13C values of −24.5‰ to −18.2‰ and −25.7‰ to −20.7‰, respectively. These C isotopic ratios are consistent with the standing modern vegetation that is dominated by a mixture of C3 and C4 plants and can be distinguished from that in the patchy forest areas where exclusive C3 trees yield a narrow δ13C value range from −26.9‰ to −25‰ (average −26.1‰). Obtained δ13C compositions from paleosols and loess sediments in the Lantian and the Luochuan profiles vary from −24‰ to −16.9‰, indicating a grass-dominated steppe with shifting C3 and C4 contributions controlled mainly by paleoclimatic changes during the late Pleistocene. The present results suggest no extensive forest coverage on the loess table during the past 130 ka even under the most suitable conditions for forest development. This conclusion supports the explanation of natural causes for the development of only patchy forests on the modern loess table and provides critical historical information toward the vegetation restoration project that is currently underway on the Chinese Loess Plateau.  相似文献   

4.
Based on the pyrolysis products for the Jurassic low-mature coal under programmed temperature,and chemical and carbon isotopic compositions of natural gas from the Kuqa Depression, the genetic origin of natural gas was determined,and then a gas filling model was established,in combination with the geological background of the Kuqa Depression.The active energy of CH_4,C_2H_6 and C_3H_8 was gotten after the data of pyrolysis gas products under different heating rates(2℃/h and 20℃/h)were fitted by the Gas O...  相似文献   

5.
A depth- and particle size-specific analysis of soil organic carbon (SOC) and its isotopic composition was undertaken to investigate the effects of soil texture (or particle size) on the depth profile of stable carbon isotopic composition of SOC (δ13CSOC) in two tropical soils. Depth-specific samples from two soil profiles of markedly different texture (coarse grained and fine grained) were separated into particle size classes and analyzed for the (mass/mass) concentration of SOC (C) and δ13CSOC. Within 1 m of the soil surface, δ13CSOC in the coarse-textured soil increases by 1.3 to 1.6‰, while δ13CSOC from the fine-textured soil increase by as much as 3.8 to 5.5‰. This increasing depth trend in the coarse-textured soil is approximately linear with respect to normalized C, while the increase in the fine-textured soil follows a logarithmic function with respect to normalized C. A model of Rayleigh distillation describing isotope fractionation during decomposition of soil organic matter (SOM) accounts for the depth profile of δ13CSOC in the fine-textured soil, but does not account for the depth profile observed in the coarse-textured soil despite their similar climate, vegetation, and topographic position. These results suggest that kinetic fractionation during humification of SOM leads to preferential accumulation of 13C in association with fine mineral particles, or aggregates of fine mineral particles in fine-textured soils. In contrast, the coarse-textured soil shows very little applicability of the Rayleigh distillation model. Rather, the depth profile of δ13CSOC in the coarse-textured soil can be accounted for by mixing of soil carbon with different isotopic ratios.  相似文献   

6.
《International Geology Review》2012,54(15):1909-1921
This paper reports the carbon and oxygen isotope compositions of lacustrine carbonate sediments from the Palaeogene Shahejie Formation, Qikou depression, Bohaiwan Basin, with the aim of determining the palaeoenvironmental conditions in the region. Results from Es2, the second member of the Shahejie Formation, showed values of δ13C and δ18O from –1.2‰ to +2.4‰ (average +0.6‰) and from –6.8‰ to –4.7‰ (average –5.7‰), respectively, suggesting a relatively hot climate attending deposition. The slightly closed nature of the lake, which contains brackish water, resulted in higher carbonate δ13C and δ18O values than in a meteoric environment. The values of δ13C and δ18O preserved within the carbonates of the overlying lower Shahejie I (Es1) varied between +1.3‰ and +4.9‰ (average +3.2‰) and from ?4.4‰ to ?1.8‰ (average ?3.1‰), respectively, indicating that the climate became colder at that time. Subsequently, a marine transgression caused the salinity of the lake water to increase. The values of δ13C and δ18O were controlled by salinity. The high δ13C values were also influenced by the rapid burial of the lake organisms and by algal photosynthesis. Values of δ13C and δ18O from carbonates in upper Es1 ranged from ?8.0‰ to +11.0‰ (average +10.1‰) and from ?5.0‰ to ?1.5‰ (average ?3.4‰), respectively, indicating a slight increase in the temperature over time. In the closed and reducing environment, extremes in δ13C values resulted from biochemical fermentation. The positive δ13C excursion recorded in the carbonates of the Shahejie Formation in the Qikou depression indicates that the palaeoclimate underwent a significant transformation during the Eocene and the Oligocene.  相似文献   

7.
Carbon stable-isotope compositions of coexisting carbon dioxide and methane from geothermal springs across the Central Andes of northern Chile and Bolivia are reported. A total of 60 samples were analyzed for δ13CCO2 and, of these, 10 were selected for δ13CCH4 analyses. The Central Andes are characterized by an active volcanic arc and an unusually thick (up to 75 km) continental crust behind the arc, beneath the high plateau region of the Altiplano. Furthermore, helium-isotope evidence suggests active mantle degassing in a 350-km-wide zone beneath the thick continental crust in the Central Andes (Hoke et al., 1994).

The present results show a wide range of δ13CCO2 (-14.9 to -0.6‰) and a surprisingly heavy δ13CCH4 (?20.9 to ?12.3‰). The difference between δ13CCO2 and δ13CCH4 (δ13CCO2-CH4 ) for individual samples varies between 1.5‰ and 13.5‰. The δ13CCO2 results show wide and overlapping ranges in the samples collected from the Precordillera, the Volcanic Arc (or Western Cordillera), the Altiplano, and the Eastern Cordillera. The widest ranges occur in the Eastern Cordillera (?15.0 to ?4.8‰) and the Altiplano (?20 to ?6‰). The δ13CCO2 results for geothermal samples from the Volcanic Arc range between ?8.0‰ (Surire) and ?0.6‰ (Abra de Nappa), whereas δ13CCO2 measured in gases collected from geothermal springs in the Precordillera range from ?10 to ?5‰.

The relationships between 3He/4He, δ13CCO2 , and δ13CCH4 are used to distinguish between crustal and mantle origins. The wide (21‰) range in the is interpreted to reflect contributions from different CO2 sources that include organic and inorganic crustal and mantle carbon. Assuming isotopic equilibrium between coexisting methane and carbon dioxide, Δ13CCO2-CH4 suggests very high equilibrium temperatures, in excess of 530°C, for some geothermal systems that also are characterized by a high (up to 63%) mantle-derived helium component.

δ13CCH4 results suggest that methane has not formed by bacteriogenic processes or by thermal decomposition of organic matter, but rather abiogenically through the high-temperature reaction between H2 and CO2. The δ13CCH4 results for the samples from the Volcanic Arc and from two CO2-rich geothermal springs in the Altiplano (Coipasa-2 and Belen de Andamarca) are similar to those reported from hydrothermal fluids emitted from the East Pacific Rise (Welhan, 1988) and White Island, New Zealand (Hulston and McCabe, 1962), suggesting a mantle-derived carbon component in the methane.  相似文献   

8.
Variations in the carbon isotope composition in gases and waters of mud volcanoes in the Taman Peninsula are studied. The δ13C values in CH4 and CO2 vary from ?59.5 to ?44.0‰ (δ13Cav = ?52.4 ± 5.4‰) and from ?17.8 to +22.8‰ (δ13Cav = +6.9 ± 9.3‰), respectively. In waters from most mud volcanoes of the peninsula, this parameter ranges from +3.3 to +33.1‰, although locally lower values are also recorded (up to ?12‰. Fractionation of carbon isotopes in the CO2-HCO3 system corresponds to the isotope equilibrium under Earth’s surface temperatures. The growth of carbon dioxide concentration in the gaseous phase and increase in the HCO3 ion concentration in their water phase is accompanied by the enrichment of the latter with the heavy 13C isotope. The δ13CTDIC value in the water-soluble carbon depends on the occurrence time of water on the Earth’s surface (exchange with atmospheric CO2, methane oxidation, precipitation of carbonates, and other processes), in addition to its primary composition. In this connection, fluctuations in δ13CTDIC values in mud volcanoes with stagnant waters may amount to 10–20‰. In the clayey pulp, concentrations of carbonate matter recalculated to CaCO3 varies from 1–4 to 36–50 wt %. The δ13C value in the latter ranges from ?3.6 to +8.4‰. Carbonate matter of the clayey pulp represents a mixture of sedimentogenic and authigenic carbonates. Therefore, it is usually unbalanced in terms of the carbon isotope composition with the water-soluble CO2 forms.  相似文献   

9.
The major ionic and dissolved inorganic carbon (DIC) concentrations and the stable carbon isotope composition of DIC (δ13CDIC) were measured in a freshwater aquifer contaminated by produced water brine with petroleum hydrocarbons. Our aim was to determine the effects of produced water brine contamination on the carbonate evolution of groundwater. The groundwater was characterized by three distinct anion facies: HCO3−-rich, SO42−-rich and Cl−-rich. The HCO3−-rich groundwater is undergoing closed system carbonate evolution from soil CO2(g) and weathering of aquifer carbonates. The SO42−-rich groundwater evolves from gypsum induced dedolomitization and pyrite oxidation. The Cl−-rich groundwater is contaminated by produced water brine and undergoes common ion induced carbonate precipitation. The δ13CDIC of the HCO3−-rich groundwater was controlled by nearly equal contribution of carbon from soil CO2(g) and the aquifer carbonates, such that the δ13C of carbon added to the groundwater was −11.6‰. In the SO42−-rich groundwater, gypsum induced dedolomitization increased the 13C such that the δ13C of carbon added to the groundwater was −9.4‰. In the produced water brine contaminated Cl−-rich groundwater, common ion induced precipitation of calcite depleted the 13C such that the δ13C of carbon added to the groundwater was −12.7‰. The results of this study demonstrate that produced water brine contamination of fresh groundwater in carbonate aquifers alters the carbonate and carbon isotopic evolution.  相似文献   

10.
Monitoring and sampling of main plants,soil CO2,soil water,bedrock,spring water,drip water and its corresponding speleothem were performed at four cave systems of Guizhou,Southwest China,from April 2003 to May 2004,in order to understand stable carbon isotope ratios variations of dissolved inorganic Carbon(DIC) in cave percolation waters(δ13CDIC) and their implications for paleoclimate.Stable carbon isotopic compositions and ions(Ca,Mg,Sr,SO4,Cl etc.) were measured for all samples.The results indicate that there are significant differences among the δ13CDIC values from inter-cave,even inter-drip of intra-cave in the four caves.The δ13CDIC values from the Liangfeng Cave(LFC) is lightest among the four caves,where vegetation type overlying the cave is primary forest dominated by tall trees with lighter average δ13C value(–29.9‰).And there are remarkable differences in δ13CDIC values of different drip waters in the Qixing Cave(QXC) and Jiangjun Cave(JJC),up to 6.9‰ and 7.8‰,respectively.Further analyses show that the δ13CDIC values in cave drip waters are not only controlled by vegetation biomass overlying the cave,but also hydro-geochemical processes.Therefore,accurate interpreting of δ13C recorded in speleothems cannot be guaranteed if these effects of the above mentioned factors are not taken into consideration.  相似文献   

11.
The terrestrial carbon cycle and the role of atmospheric CO2 concentrations in controlling global temperatures can be inferred from the study of ancient soils (paleosols). Soil-formed goethite and calcite have been the primary minerals used as a geochemical proxy for reconstructing atmospheric pCO2 from ancient terrestrial records. In the case of goethite, optimum sampling strategies for reconstructing pCO2 focus on the portion of the soil profile that displays steep gradients in both soil CO2 concentration and δ13C values of soil CO2 such that a keeling plot can be developed for a given soil and atmospheric pCO2 can be calculated from it. We report data from a Carboniferous paleosol that depart from the expected linear trends. The results indicate that pedogenic goethite is sensitive to variations in the isotopic composition of soil CO2, over a range of timescales, and can record these variations in the carbon isotope composition and mole fraction of Fe(CO3)OH in solid solution with goethite. We explore possible environmental conditions that can drive these changes as a function of either moisture controlled variations in soil respired CO2 or in the residence time of carbon in soils. The implications of this result are overestimation of paleoatmospheric pCO2 from pedogenic goethite.  相似文献   

12.
The Kalatongke Cu–Ni sulfide deposits located in the East Junggar terrane, northern Xinjiang, western China are the largest magmatic sulfide deposits in the Central Asian Orogenic Belt (CAOB). The chemical and carbon isotopic compositions of the volatiles trapped in olivine, pyroxene and sulfide mineral separates were analyzed by vacuum stepwise-heating mass spectrometry. The results show that the released volatiles are concentrated at three temperature intervals of 200–400°C, 400–900°C and 900–1200°C. The released volatiles from silicate mineral separates at 400–900°C and 900–1200°C have similar chemical and carbon isotopic compositions, which are mainly composed of H2O (av. ~92 mol%) with minor H2, CO2, H2S and SO2, and they are likely associated with the ore-forming magmatic volatiles. Light δ13CCO2 values (from ?20.86‰ to ?12.85‰) of pyroxene indicate crustal contamination occurred prior to or synchronous with pyroxene crystallization of mantle-derived ore-forming magma. The elevated contents of H2 and H2O in the olivine and pyroxene suggest a deep mantle-originated ore-forming volatile mixed with aqueous volatiles from recycled subducted slab. High contents of CO2 in the ore-forming magma volatiles led to an increase in oxygen fugacity, and thereby reduced the solubility of sulfur in the magma, then triggered sulfur saturation followed by sulfide melt segregation; CO2 contents correlated with Cu contents in the whole rocks suggest that a supercritical state of CO2 in the ore-forming magma system under high temperature and pressure conditions might play a key role in the assemblage of huge Cu and Ni elements. The volatiles released from constituent minerals of intrusion 1# have more CO2 and SO2 oxidized gases, higher CO2/CH4 and SO2/H2S ratios and lighter δ13CCO2 than those of intrusions 2# and 3#. This combination suggests that the higher oxidation state of the volatiles in intrusion 1# than intrusions 2# and 3#, which could be one of key ore-forming factors for large amounts of ores and high contents of Cu and Ni in intrusion 1#. The volatiles released at 200–400°C are dominated by H2O with minor CO2, N2+CO and SO2, with δ13CCO2 values (?25.66‰ to ?22.98‰) within the crustal ranges, and are considered to be related to secondary tectonic– hydrothermal activities.  相似文献   

13.
The natural gases in the Upper Paleozoic strata of the Ordos basin are characterized by relatively heavy C isotope of gaseous alkanes with δ 13C1 and δ13C2 values ranging mainly from ?35‰ to ?30‰ and ?27‰ to ?22‰, respectively, high δ13C excursions (round 10) between ethane and methane and predominant methane in hydrocarbon gases with most C1/(C1-C5) ratios in excess of 0.95, suggesting an origin of coal-derived gas. The gases exhibit different carbon isotopic profiles for C1-C4 alkanes with those of the natural gases found in the Lower Paleozoic of this basin, and believed to be originated from Carboniferous-Permian coal measures. The occurrence of regionally pervasive gas accumulation is distinct in the gently southward-dipping Shanbei slope of the central basin. It is noted that molecular and isotopic composition changes of the gases in various gas reservoirs are associated with the thermal maturities of gas source rocks. The abundances and δ13C values of methane generally decline northwards and from the basin center to its margins, and the effects of hydrocarbon migration on compositional modification seem insignificant. However, C isotopes of autogenetic calcites in the vertical and lateral section of reservoirs show a regular variation, and are as a whole depleted upwards and towards basin margins. Combination with gas maturity gradient, the analysis could be considered to be a useful tool for gas migration.  相似文献   

14.
The Mayuan stratabound Pb-Zn deposit in Nanzheng,Shaanxi Province,is located in the northern margin of the Yangtze Plate,in the southern margin of the Beiba Arch.The orebodies are stratiform and hosted in breciated dolostone of the Sinian Dengying Formation.The ore minerals are primarily sphalerite and galena,and the gangue minerals comprise of dolomite,quartz,barite,calcite and solid bitumen.Fluid inclusions from ore-stage quartz and calcite have homogenization tempreatures from 98 to 337℃ and salinities from 7.7 wt%to 22.2 wt%(NaCl equiv.).The vapor phase of the inclusions is mainly composed of CH_4 with minor CO_2 and H_2S.The δD_(fluid) values of fluid inclusions in quartz and calcite display a range from-68‰ to-113‰(SMOW),and the δ~(18)O_(fluid)values calculated from δ~(18)O_(quartz) and δ~(18)O_(calcite) values range from 4.5‰ to 16.7‰(SMOW).These data suggest that the ore-forming fluids may have been derived from evaporitic sea water that had reacted with organic matter.The δ~(13)C_(CH4) values of CH_4 in fluid inclusions range from-37.2‰ to-21.0‰(PDB),suggesting that the CH_4 in the ore-forming fluids was mainly derived from organic matter.This,together with the abundance of solid bitumen in the ores,suggest that organic matter played an important role in mineralization,and that the thermochemical sulfate reduction(TSR) was the main mechanism of sulfide precipitation.The Mayuan Pb-Zn deposit is a carbonate-hosted epigenetic deposit that may be classified as a Mississippi Valley type(MVT) deposit.  相似文献   

15.
Recent (<50 years old) freshwater cyanobacterial carbonates from diverse environments (streams, lakes, waterfalls) throughout Britain and Ireland were analysed for their stable carbon and oxygen isotope compositions. The mean δ18O value of ?5–9‰ PDB for river and stream data represents calcite precipitation in equilibrium with the mean oxygen isotopic composition of precipitation in central Britain (?7–5‰SMOW) assuming a mean water temperature of 9°C. The mean δ18O of lake data, ?4–5‰ PDB, is statistically different, reflecting the effects of residence time and/or variations in the oxygen isotopic composition of rainfall. Carbon isotopes have wide variations in both fluviatile and lake data sets (+ 3 to ?12‰ PDB). These variations are principally controlled in the fluviatile samples by contribution of isotopically light ‘soil zone’ carbon relative to isotopically heavier carbon from limestone aquifer rock dissolution. Lake samples have the heaviest carbon isotope values, reflecting a trend toward isotopic equilibrium between atmospheric CO2 and aqueous HCO?3. We infer that isotopic compositions of ancient cyanobacterial carbonates should also record environmental information, although the effects of stabilization and diagenesis on primary δ18O values will need careful consideration. Primary carbon isotope compositions should be well preserved, although in marine samples values will be buffered by the isotopic composition of aqueous marine bicarbonate.  相似文献   

16.
The results of isotope-geochemical studies of carbonates of different mineral types from manganese and host rocks of the Famennian manganiferous formation of Pai-Khoi are reported. Kutnahorite ores are characterized by δ13C values from–6.6 to 1.3‰ and δ18O from 20.0 to 27.4‰. Rhodonite–rhodochrosite rocks of the Silovayakha ore occurrence have δ13C from–5.2 to–2.9 and δ18O from 25.4 to 24.3‰. Mineralogically similar rocks of the Nadeiyakha ore occurrence show the lighter carbon and oxygen isotopic compositions: δ13C from–16.4 to–13.1 and δ18O from 24.8 to 22.5‰. Similar isotopic compositions were also obtained for rhodochrosite–kutnahorite rocks of this ore occurrence: δ13C from–13.0 to–10.4‰ and δ18O from 24.6 to 21.7‰. Siderorodochrosite ores differ in the lighter oxygen and carbon isotopic compositions: δ18O from 18.7 to 17.6‰ and δ13C from–10.2 to–9.3‰, respectively. In terms of the carbon and oxygen isotopic compositions, host rocks in general correspond to marine sedimentary carbonates. Geological-mineralogical and isotope data indicate that the formation of the manganese carbonates was related to the hydrothermal ore-bearing fluids with the light isotopic composition of oxygen and carbon dissolved in CO2. The isotopic features indicate an authigenic formation of manganese carbonates under different isotopegeochemical conditions.  相似文献   

17.
Carbohydrates are major organic components of dung and are likely to contribute substantially to increased carbon stocks in manured soils. To investigate this hypothesis, a field-scale experiment was conducted on a temperate grassland site in Devon, UK. C4 dung (bulk δ13C value ?12.6‰) was applied to a temperate grassland C3 soil (bulk δ13C value ?30.3‰) in April and the surface soil beneath cow pats sampled at seven dates over a year. Total carbohydrates were extracted as their monosaccharide components and analysed as the alditol acetates using gas chromatography. The δ13C values of the major monosaccharides glucose (?11.5 ±0.6‰), xylose (?10.4 ±0.4‰), arabinose (?10.4 ±0.5‰) and galactose (?8.3 ±1.6‰) extracted from the C4 dung via acid hydrolysis were indicative of their source. Their weighted mean δ13C value was ?10.8‰, 1.8‰ more 13C-enriched than the bulk dung value. The δ13C values of individual monosaccharides recovered by acid hydrolysis in the 0–1 cm and 1–5 cm soil horizons beneath C4 cow pats, compared with control soils determined over 372 days, allowed assessment of the extent of incorporation and fluxes of dung-derived monosaccharides. A maximum of 60% of the dung C in soil was derived from carbohydrates after 56 days, declining to around 20% after 372 days. Incorporation dynamics varied between monosaccharide species. Glucose, xylose and arabinose behaved in a similar manner because of their predominantly plant cell wall derived provenance in the dung, whilst dung-derived galactose and mannose appeared to have a microbial source in the soil. The dynamics of total dung-derived monosaccharides in the top 5 cm was comparable to incorporation and flux of bulk dung C, previously estimated using bulk δ13C values. The movement of dung-derived carbohydrates into the soil was inequivalent between the 0–1 cm and 1–5 cm horizons. The lack of a significant difference in concentration, but the evidence for the persistence of dung-derived monosaccharides in soil based on δ13C values, indicated replacement of existing pools in the soil, suggesting that the ability of this particular soil to sequester further C derived from carbohydrates was limited.  相似文献   

18.
Permian Khuff reservoirs along the east coast of Saudi Arabia and in the Arabian Gulf produce dry sour gas with highly variable nitrogen concentrations. Rough correlations between N2/CH4, CO2/CH4 and H2S/CH4 suggest that non-hydrocarbon gas abundances are controlled by thermochemical sulfate reduction (TSR). In Khuff gases judged to be unaltered by TSR, methane δ13C generally falls between −40‰ and −35‰ VPDB and carbon dioxide δ13C between −3‰ and 0‰ VPDB. As H2S/CH4 increases, methane δ13C increases to as much as −3‰ and carbon dioxide δ13C decreases to as little as −28‰. These changes are interpreted to reflect the oxidation of methane to carbon dioxide.Khuff reservoir temperatures, which locally exceed 150 °C, appear high enough to drive the reduction of sulfate by methane. Anhydrite is abundant in the Khuff and fine grained nodules are commonly rimmed with secondary calcite cement. Some cores contain abundant pyrite, sphalerite and galena. Assuming that nitrogen is inert, loss of methane by TSR should increase N2/CH4 of the residual gas and leave δ15N unaltered. δ15N of Paleozoic gases in Saudi Arabia varies from −7‰ to 1‰ vs. air and supports the TSR hypothesis. N2/CH4 in gases from stacked Khuff reservoirs varies by a factor of 19 yet the variation in δ15N (0.3–0.5‰) is trivial.Because the relative abundance of hydrogen sulfide is not a fully reliable extent of reaction parameter, we have attempted to assess the extent of TSR using plots of methane δ13C versus log(N2/CH4). Observed variations in these parameters can be fitted using simple Rayleigh models with kinetic carbon isotope fractionation factors between 0.98 and 0.99. We calculate that TSR may have destroyed more than 90% of the original methane charge in the most extreme instance. The possibility that methane may be completely destroyed by TSR has important implications for deep gas exploration and the origin of gases rich in nitrogen as well as hydrogen sulfide.  相似文献   

19.
Stable isotopes of injected CO2 act as useful tracers in carbon capture and storage (CCS) because the CO2 itself is the carrier of the tracer signal and remains unaffected by sorption or partitioning effects. At the Ketzin pilot site (Germany), carbon stable isotope composition (δ13C) of injected CO2 at the injection well was analyzed over a time period of 4 months. Occurring isotope variances resulted from the injection of CO2 from two different sources (an oil refinery and a natural gas-reservoir). The two gases differed in their carbon isotope composition by more than 27‰. In order to find identifiable patterns of these variances in the reservoir, more than 250 CO2-samples were collected and analyzed for their carbon isotope ratios at an observation well 100 m distant from the injection well. An isotope ratio mass spectrometer connected to a modified Thermo Gasbench system allowed quick and cost effective isotope analyses of a high number of CO2 gas specimens. CO2 gas from the oil refinery (δ13C = −30.9‰, source A) was most frequently injected and dominated the reservoir δ13C values at the injection site. Sporadic injection of the CO2 from the natural gas-reservoir (δ13C = −3.5‰, source B) caused isotope shifts of up to +5‰ at the injection well. These variances provided a potential ideal tracer for CO2 migration behavior. Based on these findings, tracer input signals that were injected during the last 2 years of injection could be reconstructed with the aid of an isotope mixing model and CO2 delivery schedules. However, in contrast to the injection well, δ13C values at the observation well showed no variances and a constant value of −28.5‰ was measured at 600 m depth. This is in disagreement with signals that would be expected if the input signals from the injection would arrive at the observation well. The lack of isotope signals at the observation well suggests that parts of the reservoir are filled with CO2 that is immobilized.  相似文献   

20.
The origin and evolution of CO2 inclusions and calcite veins in peridotite xenoliths of the Pannonian Basin, Hungary, were investigated by means of petrographic investigation and stable isotope analyses. The fluid inclusions recovered in paragenetic olivine and clinopyroxene belong to distinct populations: type A (texturally early) inclusions with regular shapes (often with negative crystal forms) forming intragranular trails; type B (texturally late) inclusions defining randomly oriented trails that reach grain boundaries. Type B inclusions are often associated with silicate melt (type C) inclusions. Stable carbon isotope compositions in inclusion-hosted CO2 were obtained by vacuum crushing followed by conventional dual inlet as well as continuous flow mass spectrometry in order to eliminate possible lab artifacts. Olivines, clino- and orthopyroxenes of the host peridotite have oxygen isotope compositions from 5.3 to 6.0‰ (relative to V-SMOW), without any relationship with xenolith texture. Some of the xenoliths contained calcite in various forms: veins and infillings in silicate globules in veins, secondary carbonate veins filling cracks and metasomatic veins with diffuse margins. The former two carbonate types have δ13C values around –13‰ (relative to V-PDB) and low Sr contents (< 0.5 wt.%), whereas the third type,veins with high-temperature metasomatic features have a δ13C value of –5.0‰ and high Sr contents up to 3.4 wt.%. In spite of the mantle-like δ13C value and the unusually high Sr content typical for mantle-derived carbonate, trace element compositions have proven a crustal origin. This observation supports the conclusions of earlier studies that the carbonate melt droplets found on peridotite xenoliths in the alkaline basalts represent mobilized sedimentary carbonate. The large δ13C range and the 12C-enrichment in the carbonates can be attributed to devolatilization of the migrating carbonate or infiltration of surficial fluids containing 12C-rich dissolved carbon.Carbon isotope compositions of inclusion-hosted CO2 range from –17.8 to –4.8‰ (relative to V-PDB) with no relation to the amount of CO2 released by vacuum crushing. Low-δ13C values measured by stepwise heating under vacuum suggest that the carbon component is pristine and not related to surficial contamination, and that primary mantle fluids with δ13C values around –5‰ were at least partly preserved in the xenoliths. Tectonic reworking and heating by the basaltic magma resulted in partial CO2 release and local 13C-depletion.  相似文献   

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