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1.
A detailed geochemical study on river waters of the Australian Victorian Alps was carried out to determine: (i) the relative significance of silicate, carbonate, evaporite and sulfide weathering in controlling the major ion composition and; (ii) the factors regulating seasonal and spatial variations of CO2 consumption via silicate weathering in the catchments. Major ion chemistry implies that solutes are largely derived from evaporation of precipitation and chemical weathering of carbonate and silicate lithologies. The input of solutes from rock weathering was determined by calculating the contribution of halite dissolution and atmospheric inputs using local rain and snow samples. Despite the lack of carbonate outcrops in the study area and waters being undersaturated with respect to calcite, the dissolution of vein calcite accounts for up to 67% of the total dissolved cations, generating up to 90% of dissolved Ca and 97% of Mg. Dissolved sulfate has δ34S values of 16 to 20‰CDT, indicating that it is derived predominantly from atmospheric deposition and minor gypsum weathering and not from bacterial reduction of FeS2. This militates against sulphuric acid weathering in Victorian rivers. Ratios of Si vs. the atmospheric corrected Na and K concentrations range from ~ 1.1 to ~ 4.3, suggesting incongruent weathering from plagioclase to smectite, kaolinite and gibbsite.Estimated long-term average CO2 fluxes from silicate weathering range from ~ 0.012 × 106 to 0.039 × 106 mol/km2/yr with the highest values in rivers draining the basement outcrops rather than sedimentary rocks. This is about one order of magnitude below the global average which is due to low relief, and the arid climate in that region. Time series measurements show that exposure to lithology, high physical erosion and long water–rock contact times dominate CO2 consumption fluxes via silicate weathering, while variations in water temperature are not overriding parameters controlling chemical weathering. Because the atmospheric corrected concentrations of Na, K and Mg act non-conservative in Victorian rivers the parameterizations of weathering processes, and net CO2 consumption rates in particular, based on major ion abundances, should be treated with skepticism. 相似文献
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Nils Moosdorf Jens Hartmann Benjamin Hagedorn 《Geochimica et cosmochimica acta》2011,75(24):7829-7854
CO2 consumption by chemical weathering is an integral part of the boundless carbon cycle, whose spatial patterns and controlling factors on continental scale are still not fully understood. A dataset of 338 river catchments throughout North America was used to empirically identify predictors of bicarbonate fluxes by chemical weathering and interpret the underlying controlling factors. Detailed analysis of major ion ratios enables distinction of the contributions of silicate and carbonate weathering and thus quantifying CO2 consumption. Extrapolation of the identified empirical model equations to North America allows the analysis of the spatial patterns of the CO2 consumption by chemical weathering.Runoff, lithology and land cover were identified as the major predictors of the riverine bicarbonate fluxes and the associated CO2 consumption. Other influence factors, e.g. temperature, could not be established in the models. Of the distinguished land cover classes, artificial surfaces, dominated by urban areas, increase bicarbonate fluxes most, followed by shrubs, grasslands, managed lands, and forests. The extrapolation results in an average specific bicarbonate flux of 0.3 Mmol km−2 a−1 by chemical weathering in North America, of which 64% originates from atmospheric CO2, and 36% from carbonate mineral dissolution. Chemical weathering in North America thus consumes 50 Mt atmospheric CO2-C per year. About half of that originates from 10% of the area of North America.The estimated strength of individual predictors differs from previous studies. This highlights the need for a globally representative set of regionally calibrated models of CO2 consumption by chemical weathering, which apply very detailed spatial data to resolve the heterogeneity of earth surface processes. 相似文献
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Water samples from the Fraser, Skeena and Nass River basins of the Canadian Cordillera were analyzed for dissolved major element concentrations (HCO3−, SO42−, Cl−, Ca2+, Mg2+, K+, Na+), δ13C of dissolved inorganic carbon (δ13CDIC), and δ34S of dissolved sulfate (δ34SSO4) to quantify chemical weathering rates and exchanges of CO2 between the atmosphere, hydrosphere, and lithosphere. Weathering rates of silicates and carbonates were determined from major element mass balance. Combining the major element mass balance with δ34SSO4 (−8.9 to 14.1‰CDT) indicates sulfide oxidation (sulfuric acid production) and subsequent weathering of carbonate and to a lesser degree silicate minerals are important processes in the study area. We determine that on average, 81% of the riverine sulfate can be attributed to sulfide oxidation in the Cordilleran rivers, and that 25% of the total weathering cation flux can be attributed to carbonate and silicate dissolution by sulfuric acid. This result is validated by δ13CDIC values (−9.8 to −3.7‰ VPDB) which represents a mixture of DIC produced by the following weathering pathways: (i) carbonate dissolution by carbonic acid (−8.25‰) > (ii) silicate dissolution by carbonic acid (−17‰) ≈ (iii) carbonate dissolution by sulfuric acid derived from the oxidation of sulfides (coupled sulfide-carbonate weathering) (+0.5‰).δ34SSO4 is negatively correlated with δ13CDIC in the Cordilleran rivers, which further supports the hypothesis that sulfuric acid produced by sulfide oxidation is primarily neutralized by carbonates, and that sulfide-carbonate weathering impacts the δ13CDIC of rivers. The negative correlation between δ34SSO4 and δ13CDIC is not observed in the Ottawa and St. Lawrence River basins. This suggests other factors such as landscape age (governed by tectonic uplift) and bedrock geology are important controls on regional sulfide oxidation rates, and therefore also on the magnitude of sulfide-carbonate weathering—i.e., it is more significant in tectonically active areas.Calculated DIC fluxes due to Ca and Mg silicate weathering by carbonic acid (38.3 × 103 mol C · km−2 · yr−1) are similar in magnitude to DIC fluxes due to sulfide-carbonate weathering (18.5 × 103 mol C · km−2 · yr−1). While Ca and Mg silicate weathering facilitates a transfer of atmospheric CO2 to carbonate rocks, sulfide-carbonate weathering can liberate CO2 from carbonate rocks to the atmosphere when sulfide oxidation exceeds sulfide deposition. This implies that in the Canadian Cordillera, sulfide-carbonate weathering can offset up to 48% of the current CO2 drawdown by silicate weathering in the region. 相似文献
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Anne-Sophie Perrin Anne Probst Jean-Luc Probst 《Geochimica et cosmochimica acta》2008,72(13):3105-3123
The goal of this study was to highlight the occurrence of an additional proton-promoted weathering pathway of carbonate rocks in agricultural areas where N-fertilizers are extensively spread, and to estimate its consequences on riverine alkalinity and uptake of CO2 by weathering. We surveyed 25 small streams in the calcareous molassic Gascogne area located in the Garonne river basin (south-western France) that drain cultivated or forested catchments for their major element compositions during different hydrologic periods. Among these catchments, the Hay and the Montoussé, two experimental catchments, were monitored on a weekly basis. Studies in the literature from other small carbonate catchments in Europe were dissected in the same way. In areas of intensive agriculture, the molar ratio (Ca + Mg)/HCO3 in surface waters is significantly higher (0.7 on average) than in areas of low anthropogenic pressure (0.5). This corresponds to a decrease in riverine alkalinity, which can reach 80% during storm events. This relative loss of alkalinity correlates well with the content in surface waters. In cultivated areas, the contribution of atmospheric/soil CO2 to the total riverine alkalinity (CO2 ATM-SOIL/HCO3) is less than 50% (expected value for carbonate basins), and it decreases when the nitrate concentration increases. This loss of alkalinity can be attributed to the substitution of carbonic acid (natural weathering pathway) by protons produced by nitrification of N-fertilizers (anthropogenic weathering pathway) occurring in soils during carbonate dissolution. As a consequence of these processes, the alkalinity over the last 30 years shows a decreasing trend in the Save river (one of the main Garonne river tributaries, draining an agricultural catchment), while the nitrate and calcium plus magnesium contents are increasing.We estimated that the contribution of atmospheric/soil CO2 to riverine alkalinity decreased by about 7-17% on average for all the studied catchments. Using these values, the deficit of CO2 uptake can be estimated as up to 0.22-0.53 and 12-29 Tg1 yr−1 CO2 on a country scale (France) and a global scale, respectively. These losses represent up to 5.7-13.4% and only 1.6-3.8% of the total CO2 flux naturally consumed by carbonate dissolution, for France and on a global scale, respectively. Nevertheless, this loss of alkalinity relative to the Ca + Mg content relates to carbonate weathering by protons from N-fertilizers nitrification, which is a net source of CO2 for the atmosphere. This anthropogenic CO2 source is not negligible since it could reach 6-15% of CO2 uptake by natural silicate weathering and could consequently partly counterbalance this natural CO2 sink. 相似文献
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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
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Peter J. Wyllie 《Geochimica et cosmochimica acta》1976,40(2):129-132
The melting temperatures of calcite and magnesite in the presence of excess CO2 have been measured using Ag2C2O4 in sealed capsules m a piston-cylinder apparatus. At 27 kbar, 11.5 wt % CO2 dissolves in molten CaCO2, depressing the freezing temperature from 1610 to 1505°C; and 6.5 wt % CO2 dissolves in molten MgCO3, depressing the freezing temperature from 1590 to 1510°C. The eutectic between calcite and lime was located at 1385°C at 27 kbar. These and other new results, combined with previously published data, permit completion of PT diagrams for the systems CaO-CO2 and MgO-CO2 from 1 bar to 35 kbar. The dissociation curve for each carbonate terminates at an invariant point where melting begins, at 40 bars and 1230°C for CaO-CO2 and 23 kbar and 1550°C for MgO-CO2 The differences between the two systems are explained by the different solubilities of CO2 in the invariant liquids consequent upon the large pressure difference between the locations of these two invariant points. The results show that the temperatures for the beginning of melting of carbonates in the asthenosphere are lowered by about 100°C in the presence of CO2. 相似文献
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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
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G.L. Macpherson J.A. Roberts M.A. Townsend K.R. Beisner 《Geochimica et cosmochimica acta》2008,72(23):5581-5599
In a mid-continental North American grassland, solute concentrations in shallow, limestone-hosted groundwater and adjacent surface water cycle annually and have increased steadily over the 15-year study period, 1991-2005, inclusive. Modeled groundwater CO2, verified by measurements of recent samples, increased from 10−2.05 atm to 10−1.94 atm, about a 20% increase, from 1991 to 2005. The measured groundwater alkalinity and alkaline-earth element concentrations also increased over that time period. We propose that carbonate minerals dissolve in response to lowered pH that occurs during an annual carbonate-mineral saturation cycle. The cycle starts with low saturation during late summer and autumn when dissolved CO2 is high. As dissolved CO2 decreases in the spring and early summer, carbonates become oversaturated, but oversaturation does not exceed the threshold for precipitation. We propose that groundwater is a CO2 sink through weathering of limestone: soil-generated CO2 is transformed to alkalinity through dissolution of calcite or dolomite. The annual cycle and long-term increase in shallow groundwater CO2 is similar to, but greater than, atmospheric CO2. 相似文献
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Various iron-bearing primary phases and rocks have been weathered experimentally to simulate possible present and past weathering processes occurring on Mars. We used magnetite, monoclinic and hexagonal pyrrhotites, and metallic iron as it is suggested that meteoritic input to the martian surface may account for an important source of reduced iron. The phases were weathered in two different atmospheres: one composed of CO2 + H2O, to model the present and primary martian atmosphere, and a CO2 + H2O + H2O2 atmosphere to simulate the effect of strong oxidizing agents. Experiments were conducted at room temperature and a pressure of 0.75 atm. Magnetite is the only stable phase in the experiments and is thus likely to be released on the surface of Mars from primary rocks during weathering processes. Siderite, elemental sulfur, ferrous sulfates and ferric (oxy)hydroxides (goethite and lepidocrocite) are the main products in a water-bearing atmosphere, depending on the substrate. In the peroxide atmosphere, weathering products are dominated by ferric sulfates and goethite. A kinetic model was then developed for iron weathering in a water atmosphere, using the shrinking core model (SCM). This model includes competition between chemical reaction and diffusion of reactants through porous layers of secondary products. The results indicate that for short time scales, the mechanism is dominated by a chemical reaction with second order kinetics (k = 7.75 × 10−5 g−1/h), whereas for longer time scales, the mechanism is diffusion-controlled (DeA = 2.71 × 10−10 m2/h). The results indicate that a primary CO2- and H2O-rich atmosphere should favour sulfur, ferrous phases such as siderite or Fe2+-sulfates, associated with ferric (oxy)hydroxides (goethite and lepidocrocite). Further evolution to more oxidizing conditions may have forced these precursors to evolve into ferric sulfates and goethite/hematite. 相似文献
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Harald Behrens Susanne Ohlhorst Michel Champenois 《Geochimica et cosmochimica acta》2004,68(22):4687-4703
The solubility of CO2 in dacitic melts equilibrated with H2O-CO2 fluids was experimentally investigated at 1250°C and 100 to 500 MPa. CO2 is dissolved in dacitic glasses as molecular CO2 and carbonate. The quantification of total CO2 in the glasses by mid-infrared (MIR) spectroscopy is difficult because the weak carbonate bands at 1430 and 1530 cm−1 can not be reliably separated from background features in the spectra. Furthermore, the ratio of CO2,mol/carbonate in the quenched glasses strongly decreases with increasing water content. Due to the difficulties in quantifying CO2 species concentrations from the MIR spectra we have measured total CO2 contents of dacitic glasses by secondary ion mass spectrometry (SIMS).At all pressures, the dependence of CO2 solubility in dacitic melts on xfluidCO2,total shows a strong positive deviation from linearity with almost constant CO2 solubility at xCO2fluid > 0.8 (maximum CO2 solubility of 795 ± 41, 1376 ± 73 and 2949 ± 166 ppm at 100, 200 and 500 MPa, respectively), indicating that dissolved water strongly enhances the solubility of CO2. A similar nonlinear variation of CO2 solubility with xCO2fluid has been observed for rhyolitic melts in which carbon dioxide is incorporated exclusively as molecular CO2 (Tamic et al., 2001). We infer that water species in the melt do not only stabilize carbonate groups as has been suggested earlier but also CO2 molecules.A thermodynamic model describing the dependence of the CO2 solubility in hydrous rhyolitic and dacitic melts on T, P, fCO2 and the mol fraction of water in the melt (xwater) has been developed. An exponential variation of the equilibrium constant K1 with xwater is proposed to account for the nonlinear dependence of xCO2,totalmelt on xCO2fluid. The model reproduces the CO2 solubility data for dacitic melts within ±14% relative and the data for rhyolitic melts within 10% relative in the pressure range 100-500 MPa (except for six outliers at low xCO2fluid). Data obtained for rhyolitic melts at 75 MPa and 850°C show a stronger deviation from the model, suggesting a change in the solubility behavior of CO2 at low pressures (a Henrian behavior of the CO2 solubility is observed at low pressure and low H2O concentrations in the melt). We recommend to use our model only in the pressure range 100-500 MPa and in the xCO2fluid range 0.1-0.95. The thermodynamic modeling indicates that the partial molar volume of total CO2 is much lower in rhyolitic melts (31.7 cm3/mol) than in dacitic melts (46.6 cm3/mol). The dissolution enthalpy for CO2 in hydrous rhyolitic melts was found to be negligible. This result suggests that temperature is of minor importance for CO2 solubility in silicic melts. 相似文献
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火山岩吸附CO2气的成藏潜力及实例分析 总被引:4,自引:0,他引:4
火山岩的脱气实验和对昌德东CO2气藏气源的分析结果表明加热火山岩到250℃时,脱出挥发分总量为0.0299~0.0790mL/g,其中CO2脱出量为0.0218~0.0706mL/g(0.429~1.387wt%);挥发组分以CO2为主,还含有H2、CO、CH4等还原性气体,以及少量低碳烷烃,CO2含量和总烃呈现反比关系;基性岩的CO2脱出量、脱出率高于中、酸性岩;CO2脱出量与岩石碱质含量正相关.松辽盆地北部昌德东CO2气藏成藏模式为"自生自储",成藏CO2气主要来自深部被火山岩吸附的气.随岩浆上升,在岩浆冷凝成火山岩的过程中被吸附于火山岩的节理、劈理和晶体位错之中的CO2气,连同火山岩包体中的残留气,成为高纯CO2气藏的主要补给源,并非地幔气体沿大断裂上来直接充注成藏. 相似文献
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Tarun K. DalaiSunil K. Singh J.R. TrivediS. Krishnaswami 《Geochimica et cosmochimica acta》2002,66(1):29-43
Extensive measurements of dissolved Re and major ion abundances in the Yamuna River System (YRS), a major tributary of the Ganga, have been performed along its entire stretch in the Himalaya, from its source near the Yamunotri Glacier to its outflow at the foothills of the Himalaya at Saharanpur. In addition, Re analysis has been made in granites and Precambrian carbonates, some of the major lithologies of the drainage basin. These data, coupled with those available for black shales in the Lesser Himalaya, allow an assessment of these lithologies’ contributions to the Re budget of the YRS.The Re concentrations in the YRS range from 0.5 to 35.7 pM with a mean of 9.4 pM, a factor of ∼4 higher than that reported for its global average concentration in rivers. Dissolved Re and ΣCations∗ (= Na∗+K+Ca+Mg) are strongly correlated in the YRS, indicating that they are released to these waters in roughly the same proportion throughout their course. The Re/ΣCations∗ in most of these rivers are one to two orders of magnitude higher than the (Re/Na+K+Mg+Ca) measured in granites of the Yamuna basin. This leads to the conclusion that, on average, granites/crystallines make only minor contributions to the dissolved Re budget of the YRS on a basin-wide scale, though they may be important for rivers with low dissolved Re. Similarly, Precambrian carbonates of the Lesser Himalaya do not seem to be a major contributor to dissolved Re in these rivers, as their Re/(Ca+Mg) is much less than those in the rivers. The observation that Re concentrations in rivers flowing through black shales and in groundwaters percolating through phosphorite-black shale-carbonate layers in phosphorite mines are high, and that Re and SO4 are significantly correlated in YRS, seems to suggest that the bulk of the dissolved Re is derived from black shale/carbonaceous sediments. Material balance considerations, based on average Re of 30 ng g−1 in black shales from the Lesser Himalaya, require that its abundance in the drainage basin of the YRS needs to be a few percent to yield average Re of 9.4 pM. Furthermore, the positive correlation between Re and ΣCations∗ would require that these Re-rich sediments (e.g., black shales) and Re-poor lithologies (e.g., crystallines, Precambrian carbonates) contribute Re and cations in roughly the same proportion throughout the drainage basin. The available data on the abundance and distribution of black shales in the basin are not adequate to test if these requirements can be met.The annual fluxes of dissolved Re at the base of the Himalaya from the Yamuna are ∼150 mol at Batamandi and ∼100 mol at Saharanpur, compared to ∼120 mol from the Ganga at Rishikesh. The total flux from the Yamuna and the Ganga account for ∼0.4% of the global riverine Re flux, much higher than their contribution to global water discharge. This is also borne out from the mobilization rate of Re: ∼1 to 3 g km−2 y−1 in the Ganga and Yamuna basins in the Himalaya, compared to the global average of ∼0.1 g km−2 y−1.Black shale weathering can also significantly influence the budgets of Os and U in rivers and CO2 in rivers and the atmosphere. Using dissolved Re in rivers as a proxy, it is estimated that ∼(6-9) × 108 kg y−1 of black shales are being weathered in the Ganga and Yamuna basins in the Himalaya. Weathering of such amounts of black shales can account for the reported concentrations of Os and U in these rivers. Furthermore, if the weathering results in the conversion of organic carbon in the black shales to CO2, it would release ∼2 × 105 mol of CO2 km−2 y−1 in the Yamuna and Ganga basins in the Himalaya, comparable to the CO2 consumption from silicate weathering. 相似文献
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湿地是温室气体二氧化碳(CO2)和甲烷(CH4)的主要来源之一,在全球碳循环中发挥着重要作用。由于CH4在百年尺度上的全球增温潜势是CO2的45倍,因此深入研究湿地CO2:CH4的排放比例及其影响因素对准确理解和预测湿地碳循环过程及其对未来全球变化的响应具有重要意义。本文采用文献整合分析方法,对比了不同类型湿地中CO2:CH4排放比例的特征及其影响因素。结果表明,藓类泥炭沼泽、滨海湿地和稻田中CO2:CH4排放比例显著高于草本沼泽、河流湿地和湖泊湿地等其他类型湿地;相关性分析研究发现,湿地CO2:CH4排放比例与pH和水位显著负相关,与盐度显著正相关。可见,藓类泥炭沼泽低水位和低pH抑制CH4排放是导致其CO2:CH4排放比例较高的重要原因,而滨海湿地高盐分抑制CH4排放是其CO2:CH4排放比例高的重要原因。与自然湿地相比,稻田CO2:CH4排放比例高与其人为施肥和稻草还田抑制CH4排放有关。此外,大气温度、土壤温度、降水量、土壤含水率等因子也对湿地CO2:CH4排放比例具有重要影响,尽管它们之间的线性相关关系不显著。目前,湿地CO2:CH4排放比例和影响因素仍存在很大的不确定性,未来亟待加强不同类型湿地CO2:CH4排放比例及其关键影响因素研究。
相似文献17.
Robert A. Berner 《Comptes Rendus Geoscience》2003,335(16):1173-1177
The rise of large vascular plants during the mid-Paleozoic brought about a major increase in the rates of weathering of silicate minerals that induced a drop in the level of atmospheric CO2 and contributed, via the atmospheric greenhouse effect, to global cooling and the initiation of the most long lived and a really extensive glaciation of the past 550 million years. Sedimentary burial of the microbiologically resistant remains of the plants resulted during the Permo-Carboniferous in both further lowering of CO2 and in elevation of atmospheric O2. Evidence of changes in CO2 and O2 are provided by mathematical models, studies of paleosols, fossil plants, fossil insects, and the effects of modern plants on silicate weathering, and by laboratory studies of the effects of changes in O2 on plants and insects. To cite this article: R.A. Berner, C. R. Geoscience 335 (2003). 相似文献
18.
Domenik Wolff-Boenisch Emmanuel J. Gabet Heiko Langner 《Geochimica et cosmochimica acta》2009,73(11):3148-7854
The major ion chemistry of the Marsyandi basin and six of its tributaries in the Nepalese Himalaya have been investigated during the monsoon months of 2002. Weekly water samples taken at 10 river monitoring stations in the Annapurna watershed over the course of 4 months provide chemical weathering data for the region at an unprecedented temporal and spatial resolution. The river chemistry of all but one basin is heavily dominated by carbonate weathering which, compared to silicate weathering, contributes 80 to 97% of the total solute load. This prevalence is due to a combination of (a) intrinsically faster dissolution kinetics of carbonates, (b) relatively high runoff and (c) glacial meltwater and low temperatures at high altitudes resulting in enhanced carbonate solubilities. Monitoring stations with headwaters in the Tethyan Sedimentary Series (TSS) are particularly carbonate-rich and slightly supersaturated with respect to calcite through half of the monsoon season. Silicate weathering in the TSS is driven largely by sulfuric acid and therefore does not contribute significantly to the drawdown of atmospheric CO2. With respect to the tributaries in the Greater Himalayan Sequence (GHS), carbonate weathering is practically as predominant as for the TSS, in spite of the largely felsic lithology of the GHS. Relative to the TSS, the primary proton source in the GHS has shifted, with at least 80% of the protons derived from carbonic acid. Averaged over the whole field area, the CO2 fluxes, based on silicate-derived Ca and Mg, are considerably lower than the global average. Assuming that this study area is representative of the entire range, we conclude that in situ weathering of the High Himalayas does not represent a significant sink of atmospheric carbon dioxide, despite the presence of a watershed south of the GHS that is characterized by a four times higher CO2 consumption rate than the global average. Silicate weathering rates of all basins appear to be climate controlled, displaying a tight correlation with runoff and temperature. Given the extremely low chemical weathering under transport-limited conditions in high-altitude crystalline terrains outside of the monsoon season, this would result in virtually no chemical exhumation for 2/3 of the year in such a cold and arid climate, north of the rain shadow cast by the High Himalayas. 相似文献
19.
Robert A. Berner 《Geochimica et cosmochimica acta》2006,70(23):5653-5664
A model for the combined long-term cycles of carbon and sulfur has been constructed which combines all the factors modifying weathering and degassing of the GEOCARB III model [Berner R.A., Kothavala Z., 2001. GEOCARB III: a revised model of atmospheric CO2 over Phanerozoic time. Am. J. Sci. 301, 182-204] for CO2 with rapid recycling and oxygen dependent carbon and sulfur isotope fractionation of an isotope mass balance model for O2 [Berner R.A., 2001. Modeling atmospheric O2 over Phanerozoic time. Geochim. Cosmochim. Acta65, 685-694]. New isotopic data for both carbon and sulfur are used and new feedbacks are created by combining the models. Sensitivity analysis is done by determining (1) the effect on weathering rates of using rapid recycling (rapid recycling treats carbon and sulfur weathering in terms of young rapidly weathering rocks and older more slowly weathering rocks); (2) the effect on O2 of using different initial starting conditions; (3) the effect on O2 of using different data for carbon isotope fractionation during photosynthesis and alternative values of oceanic δ13C for the past 200 million years; (4) the effect on sulfur isotope fractionation and on O2 of varying the size of O2 feedback during sedimentary pyrite formation; (5) the effect on O2 of varying the dependence of organic matter and pyrite weathering on tectonic uplift plus erosion, and the degree of exposure of coastal lands by sea level change; (6) the effect on CO2 of adding the variability of volcanic rock weathering over time [Berner, R.A., 2006. Inclusion of the weathering of volcanic rocks in the GEOCARBSULF model. Am. J. Sci.306 (in press)]. Results show a similar trend of atmospheric CO2 over the Phanerozoic to the results of GEOCARB III, but with some differences during the early Paleozoic and, for variable volcanic rock weathering, lower CO2 values during the Mesozoic. Atmospheric oxygen shows a major broad late Paleozoic peak with a maximum value of about 30% O2 in the Permian, a secondary less-broad peak centered near the Silurian/Devonian boundary, variation between 15% and 20% O2 during the Cambrian and Ordovician, a very sharp drop from 30% to 15% O2 at the Permo-Triassic boundary, and a more-or less continuous rise in O2 from the late Triassic to the present. 相似文献
20.
We have analysed the kinetics of Argon and CO2 diffusion in simplified iron free rhyolitic to hawaiitic melts using the diffusion couple technique. The concentration distance profiles of Ar and CO2 were measured with electron microprobe analysis and Fourier Transform Infrared Spectroscopy, respectively. Error functions were fitted to the symmetrical concentration distance profiles to extract the diffusion coefficients.In the temperature range 1373 to 1773 K the activation energies for Ar diffusion range from 169 ± 20 to 257 ± 62 kJ mol−1. Ar diffusivity increases exponentially with the degree of depolymerisation. In contrast, the mobility of total CO2, that is identical to Ar mobility in rhyolitic melt, keeps constant with changing bulk composition from rhyolite to hawaiite. CO2 speciation at 1623 K and 500 MPa was modeled for the range of compositions studied using the diffusion data of Ar and total CO2 in combination with network former diffusion calculated from viscosity data. Within error this model is in excellent agreement with CO2 speciation data extrapolated from temperatures near the glass transition temperature for dacitic melt composition. This model shows that even in highly depolymerised hawaiitic and tholeiitic melts molecular CO2 is a stable species and contributes 70 to 80% to the total CO2 diffusion, respectively. 相似文献