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The rates of Sb(III) oxidation by O2 and H2O2 were determined in homogeneous aqueous solutions. Above pH 10, the oxidation reaction of Sb(III) with O2 was first order with respect to the Sb(III) concentration and inversely proportional to the H+ concentrations at a constant O2 content of 0.22 × 10−3 M. Pseudo-first-order rate coefficients, kobs, ranged from 3.5 × 10−8 s−1 to 2.5 × 10−6 s−1 at pH values between 10.9 and 12.9. The relationship between kobs and pH was:
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Andreas C. Scheinost Andre Rossberg Irene Xifra Ann-Kathrin Leuz C. Annette Johnson 《Geochimica et cosmochimica acta》2006,70(13):3299-3312
The Sb speciation in soil samples from Swiss shooting ranges was determined using Sb K-edge X-ray absorption spectroscopy (XAS) and advanced statistical data analysis methods (iterative transformation factor analysis, ITFA). The XAS analysis was supported by a spectral data set of 13 Sb minerals and 4 sorption complexes. In spite of a high variability in geology, soil pH (3.1-7.5), Sb concentrations (1000-17,000 mg/kg) and shooting-range history, only two Sb species were identified. In the first species, Sb is surrounded solely by other Sb atoms at radial distances of 2.90, 3.35, 4.30 and 4.51 Å, indicative of metallic Sb(0). While part of this Sb(0) may be hosted by unweathered bullet fragments consisting of PbSb alloy, Pb LIII-edge XAS of the soil with the highest fraction (0.75) of Sb(0) showed no metallic Pb, but only Pb2+ bound to soil organic matter. This suggests a preferential oxidation of Pb in the alloy, driven by the higher standard reduction potential of Sb. In the second species, Sb is coordinated to 6 O-atoms at a distance of 1.98 Å, indicative of Sb(V). This oxidation state is further supported by an edge energy of 30,496-30,497 eV for the soil samples with <10% Sb(0). Iron atoms at radial distances of 3.10 and 3.56 Å from Sb atoms are in line with edge-sharing and bidentate corner-sharing linkages between Sb(O,OH)6 and Fe(O,OH)6 octahedra. While similar structural units exist in tripuhyite, the absence of Sb neighbors contradicts formation of this Fe antimonate. Hence the second species most likely consists of inner-sphere sorption complexes on Fe oxides, with edge and corner-sharing configuration occurring simultaneously. This pentavalent Sb species was present in all samples, suggesting that it is the prevailing species after weathering of metallic Sb(0) in oxic soils. No indication of Sb(III) was found. 相似文献
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As a contribution to a project on the role of aerobic heterotrophic bacteria in the organic matter turnover within cyanobacterial mats, we investigated selected lipid classes of five morphologically different microbial mats from the intertidal area of Abu Dhabi, United Arab Emirates. The mats thrive under extreme environmental conditions as they are exposed to salinity up to 200 and shadowless sunshine for nearly 12 h per day. The total extractable organic matter is characterised by heavy δ13C values of −17‰ to −10‰, suggesting CO2 limitation. The lipids reflect the biomass of the principal mat-building phototrophic and heterotrophic microorganisms. Moderate amounts of hydrocarbons, mainly cyanobacterial n-heptadecane, short chain monomethyl alkanes and diploptene were detected in all the mats. The ubiquitous n-hexadecanoic acid is dominant amongst the free and ester-bound phospholipid fatty acids (PLFAs), whereas the overall acid composition varies due to differences in the extreme environmental conditions. Additionally, the top layers of two of the five mats were analysed separately to compare their lipid compositions with those of the whole mats. As would be expected, the concentrations of cyanobacterial biomarkers exceed those found in the total mats. Noteworthy is the presence of n-heneicosadiene as predominant hydrocarbon in the top layer of the so called gelatinous mat, which thrives under the locally most extreme conditions. As the n-alkadiene was present to a much lesser extent in the intact mat, it may provide a new biomarker for a so far unknown important aerobic organism. 相似文献
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