Sulfur oxidation state and solubility in silicate melts
Sulfur oxidation state and solubility in silicate melts
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硫的氧化态和在硅酸盐熔体中的溶解度
DOI：
10.1007/s00410-023-02033-9
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发表时间：
2023
影响因子：
3.5
通讯作者：
Boulliung J
中科院分区：
文献类型：
--
作者：
Boulliung J
We have determined the solubility of sulfur (S) as sulfide (S2–) for 13 different natural melt compositions at temperatures of 1473–1773 K under controlled conditions of oxygen and sulfur fugacities (fO2andfS2, respectively). The S and major element contents of the quenched glasses were determined by electron microprobe. The sulfide capacity parameter (CS2–) was used to express S2–solubility as a function of the oxygen and sulfur fugacities according to the equation: \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\log C_{{S^{2 - } }} = \log S_{melt} \left( {wt\% } \right) + 0.5\log \left( {\frac{{fO_{2} }}{{fS_{2} }}} \right)$$\end{document}. Sulfide capacities of silicate melts were found to increase with temperature and the FeO content of the melt. We combined our sulfide data at 1473–1773 K with (O’Neill and Mavrogenes, J Petrol 43:1049–1087, 2002) results at 1673 K, and obtained by stepwise linear regression the following equation for sulfide capacity \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\log C_{{S^{2 - } }} = 0.225 + \left( {25237X_{FeO} + 5214X_{CaO} + 12705X_{MnO} + 19829X_{{K_{2} O}} - 1109X_{{Si_{0.5} O}} - 8879} \right)/T{ }$$\end{document}.XMOis the mole fraction of the oxide of M on a single-oxygen basis, andTis in Kelvin. The sulfide capacity equation was combined with sulfate capacity (CS6+) data for similar compositions and at the same temperatures (Boulliung and Wood, Geochim Cosmochim Acta 336:150–164, 2022), to estimate the S redox state (S6+/S2–ratio) as a function of melt composition, temperature and oxygen fugacity. Results obtained are in good agreement with earlier measurements of S6+/S2–for basaltic and andesitic compositions. We observe a significant increase, however, relative to FMQ of the oxygen fugacity of the S2–to S6+transition as temperature is lowered from 1773 to 1473 K. We used our results to simulate sulfur-degassing paths for basaltic compositions under various redox conditions (FMQ –2 logfO2units to FMQ + 2). The calculations indicate that, given an initial concentration of 0.12 wt% S in an ascending melt at 250 MPa, most of the S (> 80%) will be degassed before the magma reaches 100 MPa pressure.
We have determined the solubility of sulfur (S) as sulfide (S2–) for 13 different natural melt compositions at temperatures of 1473–1773 K under controlled conditions of oxygen and sulfur fugacities (fO2andfS2, respectively). The S and major element contents of the quenched glasses were determined by electron microprobe. The sulfide capacity parameter (CS2–) was used to express S2–solubility as a function of the oxygen and sulfur fugacities according to the equation: \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\log C_{{S^{2 - } }} = \log S_{melt} \left( {wt\% } \right) + 0.5\log \left( {\frac{{fO_{2} }}{{fS_{2} }}} \right)$$\end{document}. Sulfide capacities of silicate melts were found to increase with temperature and the FeO content of the melt. We combined our sulfide data at 1473–1773 K with (O’Neill and Mavrogenes, J Petrol 43:1049–1087, 2002) results at 1673 K, and obtained by stepwise linear regression the following equation for sulfide capacity \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\log C_{{S^{2 - } }} = 0.225 + \left( {25237X_{FeO} + 5214X_{CaO} + 12705X_{MnO} + 19829X_{{K_{2} O}} - 1109X_{{Si_{0.5} O}} - 8879} \right)/T{ }$$\end{document}.XMOis the mole fraction of the oxide of M on a single-oxygen basis, andTis in Kelvin. The sulfide capacity equation was combined with sulfate capacity (CS6+) data for similar compositions and at the same temperatures (Boulliung and Wood, Geochim Cosmochim Acta 336:150–164, 2022), to estimate the S redox state (S6+/S2–ratio) as a function of melt composition, temperature and oxygen fugacity. Results obtained are in good agreement with earlier measurements of S6+/S2–for basaltic and andesitic compositions. We observe a significant increase, however, relative to FMQ of the oxygen fugacity of the S2–to S6+transition as temperature is lowered from 1773 to 1473 K. We used our results to simulate sulfur-degassing paths for basaltic compositions under various redox conditions (FMQ –2 logfO2units to FMQ + 2). The calculations indicate that, given an initial concentration of 0.12 wt% S in an ascending melt at 250 MPa, most of the S (> 80%) will be degassed before the magma reaches 100 MPa pressure.
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DOI：
10.1029/2022gc010552
发表时间：
2023
期刊：
Geosystems
影响因子：
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