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1.
K.R. Baiju C.G. Nambiar G.N. Jadhav H. Kagi M. Satish-Kumar 《Journal of Asian Earth Sciences》2009,36(4-5):332-340
Characterization of fluid inclusions in graphite-bearing charnockites from the southwestern part of the Madurai Granulite Block in southern India reveals a probable relation with the formation and break down of graphite during the high-grade metamorphism. The first-generation monophase pure CO2 inclusions, the composition of which is confirmed by laser Raman spectroscopy, recorded moderate density (0.77–0.87 g/cc) corresponding to low tapping pressure (around 2 kb) than that of the peak granulite-facies metamorphism. The precipitation of graphite, as inferred from graphite inclusions and δ13C values of the graphite from the outcrops, is interpreted as the cause of this lowering of fluid density. An intermediate generation of pseudosecondary inclusions resulted from the re-equilibration or modification of the first-generation fluids and the CO2 formed is interpreted to be the oxidation product from graphite. The youngest generation of fluids which caused widespread retrogression of the granulites is a low-temperature (350 °C) high-saline (32.4–52.0 wt% NaCl equivalent) brine. Carbon isotope data on the graphite from the charnockites show δ13C values ranging from −11.3 to −19.9‰, suggesting a possibility of mixing of carbon sources, relating to earlier biogenic and later CO2 fluid influx. Combining the information gathered from petrologic, fluid inclusion and carbon stable isotope data, we model the fluid evolution in the massive charnockites of the southwestern Madurai Granulite Block. 相似文献
2.
Traditionally, the application of stable isotopes in Carbon Capture and Storage (CCS) projects has focused on δ13C values of CO2 to trace the migration of injected CO2 in the subsurface. More recently the use of δ18O values of both CO2 and reservoir fluids has been proposed as a method for quantifying in situ CO2 reservoir saturations due to O isotope exchange between CO2 and H2O and subsequent changes in δ18OH2O values in the presence of high concentrations of CO2. To verify that O isotope exchange between CO2 and H2O reaches equilibrium within days, and that δ18OH2O values indeed change predictably due to the presence of CO2, a laboratory study was conducted during which the isotope composition of H2O, CO2, and dissolved inorganic C (DIC) was determined at representative reservoir conditions (50 °C and up to 19 MPa) and varying CO2 pressures. Conditions typical for the Pembina Cardium CO2 Monitoring Pilot in Alberta (Canada) were chosen for the experiments. Results obtained showed that δ18O values of CO2 were on average 36.4 ± 2.2‰ (1σ, n = 15) higher than those of water at all pressures up to and including reservoir pressure (19 MPa), in excellent agreement with the theoretically predicted isotope enrichment factor of 35.5‰ for the experimental temperatures of 50 °C. By using 18O enriched water for the experiments it was demonstrated that changes in the δ18O values of water were predictably related to the fraction of O in the system sourced from CO2 in excellent agreement with theoretical predictions. Since the fraction of O sourced from CO2 is related to the total volumetric saturation of CO2 and water as a fraction of the total volume of the system, it is concluded that changes in δ18O values of reservoir fluids can be used to calculate reservoir saturations of CO2 in CCS settings given that the δ18O values of CO2 and water are sufficiently distinct. 相似文献
3.
Y.K. Kharaka D.R. Cole J.J. Thordsen E. Kakouros H.S. Nance 《Journal of Geochemical Exploration》2006,89(1-3):183
To investigate the potential for the geologic storage of CO2 in saline sedimentary aquifers, 1600 ton of CO2 were injected at 1500 m depth into a 24-m sandstone section of the Frio Formation — a regional reservoir in the US Gulf Coast. Fluid samples obtained from the injection and observation wells before, during and after CO2 injection show a Na–Ca–Cl type brine with 93,000 mg/L TDS and near saturation of CH4 at reservoir conditions. As injected CO2 gas reached the observation well, results showed sharp drops in pH (6.5 to 5.7), pronounced increases in alkalinity (100 to 3000 mg/L as HCO3) and Fe (30 to 1100 mg/L), and significant shifts in the isotopic compositions of H2O and DIC. Geochemical modeling indicates that brine pH would have dropped lower, but for buffering by dissolution of calcite and Fe oxyhydroxides. Post-injection results show the brine gradually returning to its pre-injection composition. 相似文献
4.
The geochemistry of dissolved and suspended loads in river catchments of two low mountain ranges in Central Europe allows comparison of pertinent chemical weathering rates. Distinct differences in lithology, i.e. granites prevailing in the Black Forest compared to Palaeozoic sediments in the Rhenish Massif, provide the possibility to examine the influence of lithology on weathering. Here we determine the origin of river water using the stable isotope ratio δ18OH2O and we quantify the geogenic proportions of sulphate from stable isotope ratios δ34SSO4 and δ18OSO4. Particularly in catchments with abundant pyrite, determination of the geogenic amount of sulphate is important, since oxidation of pyrite leads to acidity, which increases weathering. Our results show that spatially averaged silicate weathering rates are higher for the river catchments Acher and Gutach in the Black Forest (10–12 t/km2/yr) compared to the river catchments of the Möhne dam and the Aabach dam in the Rhenish Massif (2–6 t/km2/yr). Correspondingly, the CO2 consumption by silicate weathering in the Black Forest (334–395 × 103 mol/km2/yr) is more than twice as high as in the Rhenish Massif (28–151 × 103 mol/km2/yr). These higher rates for watersheds of the Black Forest are likely due to steeper slopes leading to higher mechanical erosion with respective higher amounts of fresh unweathered rock particulates and due to the fact that the sediments in the Rhenish Massif have already passed through at least one erosion cycle. Carbonate weathering rates vary between 12 and 38 t/km2/yr in the catchments of the Rhenish Massif. The contribution of sulphuric acid to the silicate weathering is higher in the catchments of the Rhenish Massif (9–16%) than in the catchments of the Black Forest (5–7%) due to abundant pyrite in the sediments of the Rhenish Massif. Three times higher long-term erosion rates derived from cosmogenic nuclides compared to short-term erosion rates derived from river loads in Central Europe point to three times higher CO2 consumption during the past 103 to 104 years. 相似文献
5.
Four different types of parageneses of the minerals calcite, dolomite, diopside, forsterite, spinel, amphibole (pargasite), (Ti–)clinohumite and phlogopite were observed in calcite–dolomite marbles collected in the Kimi-Complex of the Rhodope Metamorphic Province (RMP). The presence of former aragonite can be inferred from carbonate inclusions, which, in combination with an analysis of phase relations in the simplified system CaO–MgO–Al2O3–SiO2–CO2 (CMAS–CO2) show that the mineral assemblages preserved in these marbles most likely equilibrated at the aragonite–calcite transition, slightly below the coesite stability field, at ca. 720 °C, 25 kbar and aCO2 ~ 0.01. The thermodynamic model predicts that no matter what activity of CO2, garnet has to be present in aluminous calcite–dolomite-marble at UHP conditions. 相似文献
6.
Pedogenic needle-fiber calcite was studied regarding its morphology, texture and stable isotope composition from the paleosol of the Quaternary Várhegy travertine (Budapest, Hungary). The needle-fiber calcite is composed of 40–200 μm long monocrystals. Smooth rods as well as serrated-edged crystals with calcite overgrowths were identified by SEM. Needles have several textural varieties: randomly distributed crystals in vugs and pores with calcite hypocoatings, bundles of subparallel crystals forming coatings around grains and alveolar structure with bridging needles in vugs.The morphological study of needle-fiber calcite suggests that needles are calcified fungal sheaths and produced by fungal biomineralization, a common process in recent and fossil soils and calcretes. The stable isotope composition of needle-fiber calcite (average: δ18O=-7.1‰ and δ13C=-7.3‰ vs. V-PDB) indicates significant incorporation of organically derived CO2 and probably biological influence on needle genesis. Dissolved host rock travertine and/or atmospheric CO2 could also contribute some carbon to the acicular calcite. 相似文献
7.
We have developed a quantitative model of CO2 and H2O isotopic mixing between magmatic and hydrothermal gases for the fumarolic emissions of the La Fossa crater (Vulcano Island, Italy). On the basis of isotope balance equations, the model takes into account the isotope equilibrium between H2O and CO2 and extends the recent model of chemical and energy two-end-member mixing by Nuccio et al. (1999). As a result, the H2O and CO2 content and the δD, δ18O, and δ13C isotope compositions for both magmatic and hydrothermal end-members have been assessed. Low contributions of meteoric steam, added at a shallow depth, have been also recognized and quantified in the fumaroles throughout the period from 1988 to 1998. Nonequilibrium oxygen isotope exchange also seems to be occurring between ascending gases and wall rocks along some fumarolic conduits.The δ13CCO2 of the magmatic gases varies around −3 to 1‰ vs. Peedee belemnite (PDB), following a perfect synchronism with the variations of the CO2 concentration in the magmatic gases. This suggests a process of isotope fractionation because of vapor exsolution caused by magma depressurization. The hydrogen isotopes in the magmatic gases (−1 to −‰ vs. standard mean ocean water [SMOW]), as well as the above δ13CCO2 value, are coherent with a convergent tectonic setting of magma generation, where the local mantle is widely contaminated by fluids released from the subducted slab. Magma contamination in the crust probably amplifies this effect.The computed isotope composition of carbon and hydrogen in the hydrothermal vapors has been used to calculate the δD and δ13C of the entire hydrothermal system, including mixed H2O-CO2 vapor, liquid water, and dissolved carbon. We have computed values of about 10‰ vs. SMOW for water and −2 to −6.5‰ vs. PDB for CO2. On these grounds, we think that Mediterranean marine water (δDH2O ≈ 10‰) feeds the hydrothermal system. It infiltrates at depth throughout the local rocks, reaching oxygen isotope equilibrium at high temperatures. Interaction processes between magmatic gases and the evolving seawater also seem to occur, causing the dissolution of isotopically fractionated aqueous CO2 and providing the source for hydrothermal carbon. These results have important implications concerning fluid circulation beneath Vulcano and address the more convenient routine of geochemical surveillance. 相似文献
8.
Reactions of CO2 with carbonate and silicate minerals in continental sediments and upper part of the crystalline crust produce HCO3− in river and ground waters. H2SO4 formed by the oxidation of pyrite and reacting with carbonates may produce CO2 or HCO3−. The ratio, ψ, of atmospheric or soil CO2 consumed in weathering to HCO3− produced depends on the mix of CO2 and H2SO4, and the proportions of the carbonates and silicates in the source rock. An average sediment has a CO2 uptake potential of ψ = 0.61. The potential increases by inclusion of the crystalline crust in the weathering source rock. A mineral dissolution model for an average river gives ψ = 0.68 to 0.72 that is within the range of ψ = 0.63 to 0.75, reported by other investigators using other methods. These results translate into the CO2 weathering flux of 20 to 24 × 1012mol/yr. 相似文献
9.
Stable carbon and oxygen isotope investigation in historical lime mortar and plaster – Results from field and experimental study 总被引:1,自引:1,他引:0
Lime mortar and plaster were sampled from Roman, medieval and early modern buildings in Styria. The historical lime mortar and plaster consist of calcite formed in the matrix during setting and various aggregates. The stable C and O isotopic composition of the calcite matrix was analyzed to get knowledge about the environmental conditions during calcite formation. The δ13Cmatrix and δ18Omatrix values range from −31 to 0‰ and −26 to −3‰(VPDB), respectively. Obviously, such a range of isotope values does not represent the local natural limestone assumed to be used for producing the mortar and plaster. In an ideal case, the calcite matrix in lime mortar and plaster is isotopically lighter in the exterior vs. the interior mortar layer according to the relationship δ18Omatrix = 0.61 · δ13Cmatrix − 3.3 (VPDB). Calcite precipitation by uptake of gaseous CO2 into alkaline Ca(OH)2 solutions shows a similar relationship, δ18Ocalcite = 0.67 · δ13Ccalcite − 6.4 (VPDB). Both relationships indicate that the 13C/12C and 18O/16O values of the calcite reflect the setting behaviour of the lime mortar and plaster. Initially, CO2 from the atmosphere is fixed as calcite, which is accompanied by kinetic isotope fractionation mostly due to the hydroxylation of CO2 (δ13Cmatrix ≈ −25‰ and δ18Omatrix ≈ −20‰). As calcite formation continued the remaining gaseous CO2 is subsequently enriched in 13C and 18O causing later formed calcite to be isotopically heavier along the setting path in the matrix. Deviations from such an ideal isotopic behaviour may be due to the evolution of H2O, e.g. evaporation, the source of CO2, e.g. from biogenic origin, relicts of the natural limestone, and secondary effects, such as recrystallization of calcite. The results of the field and experimental study suggest that isotope values can be used as overall proxies to decipher the origin of carbonate and the formation conditions of calcite in the matrix of ancient and recent lime mortar and plaster. Moreover, these proxies can be used to select calcite matrix from historical lime mortar and plaster for 14C dating. 相似文献
10.
The prevailing theory for the formation of trona [Na3(CO3)(HCO3) · 2(H2O)] relies on evaporative concentration of water produced by silicate hydrolysis of volcanic rock or volcaniclastic sediments. Given the abundance of closed drainage basins dominated by volcanics, it is puzzling that there are so few trona deposits and present-day lakes that would yield dominantly Na–CO3 minerals upon evaporation. Groundwater in the San Bernardino Basin (southeastern Arizona, USA and northeastern Sonora, Mexico) would yield mainly Na–CO3 minerals upon evaporation, but waters in the surrounding basins would not. Analysis of the chemical evolution of this groundwater shows that the critical difference from the surrounding basins is not lithology, but the injection of magmatic CO2. Many major deposits of trona and Na–CO3-type lakes appear to have had “excess” CO2 input, either from magmatic sources or from the decay of organic matter. It is proposed that, along with the presence of volcanics, addition of “excess” CO2 is an important pre-condition for the formation of trona deposits. 相似文献
11.
Organic sulfur in marine sediment is 34S enriched relative to the co-existing pyrite. This phenomenon is still enigmatic. Timing of the sulfur incorporation, immobilization and different sulfur species involved are part of the explanations. The reduced sulfur species incorporation into organic matter (OM) is generally assumed to have negligible δ34S fractionation. This assumption has never been confirmed by laboratory experimental data. The present study measures the δ34S changes resulting from reduced sulfur species (sulfides and polysulfide anions) incorporation into organic model compounds in an aquatic and low temperature (25 °C) system that simulates diagenetic marine environment. In addition, we also investigate the δ34S fractionation and the isotope chemical mixing in the formation of polysulfide anions produced from elemental sulfur and sulfide anions. The results showed total isotope mixing between the two species in the formation of polysulfides. Acidification of the polysulfides solution caused δ34S fractionation between the released elemental sulfur and H2S. The incorporation of polysulfides and sulfides into carbonyl groups, caused 34S enrichment relative to the starting polysulfides and sulfide of 4–5‰. The 34S enrichment of the sulfurized carbonyl groups showed a minimal effect by temperature (0–70 °C) and is not affected by salinity, polysulfides composition, reaction time or solubility in water. The incorporation of polysulfides and sulfides into brominated organic compounds was negligibly 34S enriched. The chemical mechanisms controlling the polysulfides incorporation into OM depend mostly on the functional groups and determine the 34S enrichment of the sulfurized OM. The results presented in this study can explain part of the difference between pyrite δ34S and sulfurized OM δ34S in natural marine sediments. 相似文献
12.
Stable isotope evidence for the atmospheric origin of CO2 involved in carbonation of MSWI bottom ash
Stable isotopes were used to constrain the origin of CO2 involved in the ageing process of municipal solid waste incineration (MSWI) bottom ash under open-air conditions. The δ13C and δ18O values of CaCO3 occurring in MSWI bottom ash samples of variable age and the δ13C of the residual organic matter content were measured, and laboratory assessments made of the isotopic fractionation accompanying CaCO3 neo-formation during accelerated carbonation experiments of bottom ash or pure lime with atmospheric or industrial CO2. The results indicate that stable isotopic compositions exhibited by fresh and aged bottom ash samples reflect non-equilibrium processes resembling those described in the carbonation of concrete and mortar. They also lead to conclusions on the prevalent involvement of atmospheric CO2 in the open-air carbonation of MSWI bottom ash. 相似文献
13.
P. Bertier R. Swennen B. Laenen D. Lagrou R. Dreesen 《Journal of Geochemical Exploration》2006,89(1-3):10
Geological sequestration of CO2 is one of the options studied to reduce greenhouse gas emissions. Although the feasibility of this concept is proven, apart from literature data on modelling still little is known about the CO2–water–rock interactions induced by CO2-injection.To evaluate the effect of CO2–water–rock interactions on three sandstone aquifers in NE-Belgium an experimental setup was built. Eighteen experiments were performed in which sandstones were exposed to supercritical CO2. CO2–water–rock interactions were deduced from the evolution of aqueous concentrations of 25 species and a thorough characterisation of the sandstones before and after treatment. The results show that dissolution of ankerite/dolomite and Al-silicates could enhance porosity/permeability. The observed precipitation of end-member carbonates could increase storage capacity if it exceeds carbonate dissolution. Precipitation of the latter and of K-rich clays as observed, however, can hamper the injection. 相似文献
14.
It is widely recognised that a significant limitation to the ultimate precision of carbon stable isotope ratio measurements, as obtained from dual-inlet mass spectrometric measurements of CO2 isotopologue ion abundances at m/z 44, 45, and 46, is the correction for interference from 17O-bearing molecular ions. Two long-established, alternative procedures for determining the magnitude of this correction are in widespread use (although only one has IAEA approval); their differences lead to small but potentially significant discrepancies in the magnitude of the resulting correction. Furthermore, neither approach was designed to accommodate oxygen three-isotope distributions which do not conform to terrestrial mass-dependent behaviour. Stratospheric CO2, for example, contains a strongly ‘mass-independent’ oxygen isotope composition. A new strategy for determining the 17O-bearing ion correction is presented, for application where the oxygen three-isotope characteristics of the analyte CO2 are accurately known (or assigned) in terms of the slope λ of the three-isotope fractionation line and the ordinate axis intercept 103 ln(1 + k) on a 103 ln(1 + δ17O) versus 103 ln(1 + δ18O) plot. At the heart of the approach is the relationship between 17R, which is the 17O/16O ratio of the sample CO2, and other assigned or empirically determined parameters needed for the δ13C evaluation:
15.
The chromites from the alpine type ultramafic intrusive of Sukinda, India, display a typical partly inverse spinel form and occur in two distinct zones: Brown Ore Zone (BOZ) and Grey Ore Zone (GOZ). The host ultramafites are mostly altered and are represented by the serpentinite, tremolite-talc(chlorite) schist, talc-serpentine schist and chlorite rock. The less altered variants are dunite, harzburgite and websterite. A dyke of orthopyroxenite runs through the main ultramafic body.The composition of olivine (Fo92), orthopyroxene (En92–89) and Al2O3 contents of the parental liquid (10.40–11.45%) determined from chromites, suggest that the parent melt is of boninitic affinity. The chemical plot of TiO2 content against cr# of chromites corroborates a boninitic parental melt. The Fe–Mg partitioning in olivine and chromite depicts the temperature for chromitites as 1200 °C. A compositional plot of mg# and cr# suggests crystallization at high pressure conditions, corresponding to the kimberlite xenolith field. From the P–T diagram of pyrolite melting and mineral assemblage, the pressure of crystallization is stipulated to be ≥1.2 GPa. The fO2 values estimated from Fe3+/Cr+Al+Fe3+ ratios range from 10−8.3 to 10−9.3 for the GOZ and 10−7.1 to 10−7.3 for the BOZ. The fO2 values together with the pressure range suggest crystallization at upper mantle conditions. The heterogeneity in chemical composition and fO2 conditions for the GOZ and BOZ could be linked to heterogeneity in the upper mantle. 相似文献
16.
Brad E. Rosenheim Peter K. Swart Philippe Willenz 《Geochimica et cosmochimica acta》2009,73(18):5308-5319
A revised calibration is presented relating the oxygen isotope composition of the aragonite-secreting sclerosponge Ceratoporella nicholsoni, oxygen isotope composition of seawater, and ambient water temperature. This new relationship has been obtained using high-resolution δ18O data measured in sclerosponges from the Bahamas and Jamaica compared to ambient temperature measurements and δ18O values of seawater from the two locations, both measured and published. New data improve an existing calibration which was determined using measurements of salinity rather than directly measured δ18O values of the seawater and was composed of measurements from different species of sclerosponge and other aragonite-secreting organisms. The updated calibration (n = 12, r2 = 0.95) is:
T(°C)=16.1(±3.1)-[6.5(±1.1)](δarag-δsw),