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Gleb S PokrovskiDenis Testemale Jean-Louis HazemannAndrew Y.u Bychkov Galina V Golikova 《Geochimica et cosmochimica acta》2002,66(19):3453-3480
The stoichiometry and stability of arsenic gaseous complexes were determined in the system As-H2O ± NaCl ± HCl ± H2S at temperatures up to 500°C and pressures up to 600 bar, from both measurements of As(III) and As(V) vapor-liquid and vapor-solid partitioning, and X-ray absorption fine structure (XAFS) spectroscopic study of As(III)-bearing aqueous fluids. Vapor-aqueous solution partitioning for As(III) was measured from 250 to 450°C at the saturated vapor pressure of the system (Psat) with a special titanium reactor that allows in situ sampling of the vapor phase. The values of partition coefficients for arsenious acid (H3AsO3) between an aqueous solution (pure H2O) and its saturated vapor (K = mAsvapor /mAsliquid) were found to be independent of As(III) solution concentrations (up to ∼1 to 2 mol As/kg) and equal to 0.012 ± 0.003, 0.063 ± 0.023, and 0.145 ± 0.020 at 250, 300, and 350°C, respectively. These results are interpreted by the formation, in the vapor phase, of As(OH)3(gas), similar to the aqueous As hydroxide complex dominant in the liquid phase. Arsenic chloride or sulfide gaseous complexes were found to be negligible in the presence of HCl or H2S (up to ∼0.5 mol/kg of vapor). XAFS spectroscopic measurements carried out on As(III)-H2O (±NaCl) solutions up to 500°C demonstrate that the As(OH)3 complex dominates As speciation both in dense H2O-NaCl fluids and low-density supercritical vapor. Vapor-liquid partition coefficients for As(III) measured in the H2O-NaCl system up to 450°C are consistent with the As speciation derived from these spectroscopic measurements and can be described by a simple relationship as a function of the vapor-to-liquid density ratio and temperature. Arsenic(III) partitioning between vapor and As-concentrated solutions (>2 mol As/kg) or As2O3 solid is consistent with the formation, in the vapor phase, of both As4O6 and As(OH)3. Arsenic(V) (arsenic acid, H3AsO4) vapor-liquid partitioning at 350°C for dilute aqueous solution was interpreted by the formation of AsO(OH)3 in the vapor phase.The results obtained were combined with the corresponding properties for the aqueous As(III) hydroxide species to generate As(OH)3(gas) thermodynamic parameters. Equilibrium calculations carried out by using these data indicate that As(OH)3(gas) is by far the most dominant As complex in both volcanic gases and boiling hydrothermal systems. This species is likely to be responsible for the preferential partition of arsenic into the vapor phase as observed in fluid inclusions from high-temperature (400 to 700°C) Au-Cu (-Sn, -W) magmatic-hydrothermal ore deposits. The results of this study imply that hydrolysis and hydration could be also important for other metals and metalloids in the H2O-vapor phase. These processes should be taken into account to accurately model element fractionation and chemical equilibria during magma degassing and fluid boiling. 相似文献
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N. A. Kurentsova T. I. Frolova G. B. Udintsev I. A. Roshchina 《Russian Journal of Pacific Geology》2007,1(5):435-443
This work is devoted to the results of the joint Russian-German geodynamic research carried out in the Weddell Sea and West Antarctica during cruise ANT-XXII/3 of the R/V Polarstern in 2005. The study of rock samples collected from the sea floor showed that a heterogeneous structure of the Weddell Sea was formed by spatiotemporal combination of the destruction of continental crust, progressive thalassogenesis (oceanization-taphrogenesis), and rifting, as opposed to a spreading origin. High postconsolidation mobility during the destruction stage led to the areal dismembering and high permeability of the continental crust, as well as to tectonomagmatic activation. The main mechanism of reworking of the continental crust is recognized to be the magmatic replacement by basic-ultrabasic mantle material with formation of a secondary oceanic crust and preservation of relics of the continental crust. The Earth’s endogenous activity was driven by transmagmatic fluid flows, which ascended from the melted core and caused transformation of the Earth’s crust and mantle. 相似文献
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The stability and structure of aqueous complexes formed by trivalent antimony (SbIII) with carboxylic acids (acetic, adipic, malonic, lactic, oxalic, tartaric, and citric acid), phenols (catechol), and amino acids (glycine) having O- and N-functional groups (carboxyl, alcoholic hydroxyl, phenolic hydroxyl and amine) typical of natural organic matter, were determined at 20 and 60 °C from solubility and X-ray absorption fine structure (XAFS) spectroscopy measurements. In organic-free aqueous solutions and in the presence of acetic, adipic, malonic acids and glycine, both spectroscopic and solubility data are consistent with the dominant formation of SbIII hydroxide species, , at strongly acid, acid-to-neutral and basic pH, respectively, demonstrating negligible complexing with mono-functional organic ligands (acetic) or those having non adjacent carboxylic groups (adipic, malonic). In contrast, in the presence of poly-functional carboxylic and hydroxy-carboxylic acids and catechol, SbIII forms stable 1:1 and 1:2 complexes with the studied organic ligands over a wide pH range typical of natural waters (3 < pH < 9). XAFS spectroscopy measurements show that in these species the central SbIII atom has a distorted pseudo-trigonal pyramidal geometry composed of the lone pair of 5s2 electrons of Sb and four oxygen atoms from two adjacent functional groups of the ligand (OC-OH and/or COH), forming a five-membered bidendate chelate cycle. Stability constants for these species, generated from Sb2O3 (rhomb.) solubility experiments, were used to model Sb complexing with natural humic acids possessing the same functional groups as those investigated in this study. Our predictions show that in an aqueous solution of pH between 2 and 10, containing 1 μg/L of Sb and 5 mg/L of dissolved organic carbon (DOC), up to 35% of total dissolved Sb binds to aqueous organic matter via carboxylic and hydroxy-carboxylic groups. This amount of complexed Sb for typical natural DOC concentrations is in agreement with that estimated from dialysis experiments performed with commercial humic acid in our work and those available in the literature for a range of standardized IHSS humic acids. Our results imply that a significant part of Sb is likely to be bound with humic acids via hydroxy-carboxylic moieties, in the form of bidendate complexes. However, following the strong chemical affinity of SbIII for reduced sulfur, some undefined fraction of SbIII might also be bound to the minor thiol-bearing moieties of humic acids; further studies are required to check this hypothesis. 相似文献
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Jordan Van Aalsburg John B. Rundle Lisa B. Grant Paul B. Rundle Gleb Yakovlev Donald L. Turcotte Andrea Donnellan Kristy F. Tiampo Jose Fernandez 《Pure and Applied Geophysics》2010,167(8-9):967-977
In weather forecasting, current and past observational data are routinely assimilated into numerical simulations to produce ensemble forecasts of future events in a process termed “model steering”. Here we describe a similar approach that is motivated by analyses of previous forecasts of the Working Group on California Earthquake Probabilities (WGCEP). Our approach is adapted to the problem of earthquake forecasting using topologically realistic numerical simulations for the strike-slip fault system in California. By systematically comparing simulation data to observed paleoseismic data, a series of spatial probability density functions (PDFs) can be computed that describe the probable locations of future large earthquakes. We develop this approach and show examples of PDFs associated with magnitude M > 6.5 and M > 7.0 earthquakes in California. 相似文献
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