Solubility of Au in Cl- and S-bearing hydrous silicate melts

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Original languageEnglish
Pages (from-to)2396-2411
Number of pages16
JournalGeochimica et Cosmochimica Acta
Volume74
Issue number8
Early online date22 Sept 2009
Publication statusPublished - 15 Apr 2010

Abstract

The solubility of Au in Cl- and S-bearing hydrous rhyodacitic and andesitic melts has been experimentally investigated at 1050 °C, 200 MPa and log fO2 close to the Ni/NiO solid oxygen buffer (NNO). The concentrations of Au in the experimental glasses have been determined using Laser Ablation ICP-MS (LA) with special efforts to avoid incorporation of Au micronuggets in the analysis. It is concluded that metal micronuggets are an experimental artefact and produced by Au partitioning into the fluids during heating with consequent precipitation on fluid dissolution in the melting glass powder. Hence, the micronuggets do not represent quench phases and must be excluded from the analysis. The micro-analytical data obtained by LA show that Au concentrations vary from ∼0.2 to ∼2.5 ppm by weight, generally consistent with the literature data for other melt compositions. The measured Au concentrations increase with increasing amounts of Cl and S dissolved in the silicate melt and show a correlation with the apparent activities of Cl and S in the system. The apparent activities of Cl and S are defined by the simplified linear relationship between volatile concentrations in the melt and activity of volatiles. The maximum activity (a* = 1) is assumed to be reached at the saturation of the systems in respect of Cl-rich brine or FeS liquid for Cl and S, respectively. The dependence of Au solubility on the concentrations/activities of Cl and S at the fixed redox conditions shows that Au may form not only oxide- but also Cl- and S-bearing complexes in silicate melts. Furthermore, it indicates that exsolution of S and Cl from the melt by degassing/segregation/crystallization processes may lead to mobilization and extraction of Au into the fluid, liquid and/or mineral phase(s).

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Solubility of Au in Cl- and S-bearing hydrous silicate melts. / Botcharnikov, R. E.; Linnen, Robert L.; Holtz, Francois.
In: Geochimica et Cosmochimica Acta, Vol. 74, No. 8, 15.04.2010, p. 2396-2411.

Research output: Contribution to journalArticleResearchpeer review

Botcharnikov RE, Linnen RL, Holtz F. Solubility of Au in Cl- and S-bearing hydrous silicate melts. Geochimica et Cosmochimica Acta. 2010 Apr 15;74(8):2396-2411. Epub 2009 Sept 22. doi: 10.1016/j.gca.2009.09.021
Botcharnikov, R. E. ; Linnen, Robert L. ; Holtz, Francois. / Solubility of Au in Cl- and S-bearing hydrous silicate melts. In: Geochimica et Cosmochimica Acta. 2010 ; Vol. 74, No. 8. pp. 2396-2411.
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abstract = "The solubility of Au in Cl- and S-bearing hydrous rhyodacitic and andesitic melts has been experimentally investigated at 1050 °C, 200 MPa and log fO2 close to the Ni/NiO solid oxygen buffer (NNO). The concentrations of Au in the experimental glasses have been determined using Laser Ablation ICP-MS (LA) with special efforts to avoid incorporation of Au micronuggets in the analysis. It is concluded that metal micronuggets are an experimental artefact and produced by Au partitioning into the fluids during heating with consequent precipitation on fluid dissolution in the melting glass powder. Hence, the micronuggets do not represent quench phases and must be excluded from the analysis. The micro-analytical data obtained by LA show that Au concentrations vary from ∼0.2 to ∼2.5 ppm by weight, generally consistent with the literature data for other melt compositions. The measured Au concentrations increase with increasing amounts of Cl and S dissolved in the silicate melt and show a correlation with the apparent activities of Cl and S in the system. The apparent activities of Cl and S are defined by the simplified linear relationship between volatile concentrations in the melt and activity of volatiles. The maximum activity (a* = 1) is assumed to be reached at the saturation of the systems in respect of Cl-rich brine or FeS liquid for Cl and S, respectively. The dependence of Au solubility on the concentrations/activities of Cl and S at the fixed redox conditions shows that Au may form not only oxide- but also Cl- and S-bearing complexes in silicate melts. Furthermore, it indicates that exsolution of S and Cl from the melt by degassing/segregation/crystallization processes may lead to mobilization and extraction of Au into the fluid, liquid and/or mineral phase(s).",
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note = "Funding Information: We thank O. Diedrich for the preparation of the samples for analysis; R. Schoenberg for the bulk ICP-MS analyses of experimental glasses; Z. Yang and B. Fryer from Great Lakes Institute for Environmental Research, University of Windsor, Canada for the help with LA-ICP-MS measurements; D. Kosanke and A. Husen for the help with determination of Fe 2+ / Σ Fe ratios in the glasses. A. Simon and J. Webster are gratefully acknowledged for the constructive reviews. The financial support for this research was provided by the DFG ( BO2941/1 ). Copyright: Copyright 2011 Elsevier B.V., All rights reserved.",
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AU - Botcharnikov, R. E.

AU - Linnen, Robert L.

AU - Holtz, Francois

N1 - Funding Information: We thank O. Diedrich for the preparation of the samples for analysis; R. Schoenberg for the bulk ICP-MS analyses of experimental glasses; Z. Yang and B. Fryer from Great Lakes Institute for Environmental Research, University of Windsor, Canada for the help with LA-ICP-MS measurements; D. Kosanke and A. Husen for the help with determination of Fe 2+ / Σ Fe ratios in the glasses. A. Simon and J. Webster are gratefully acknowledged for the constructive reviews. The financial support for this research was provided by the DFG ( BO2941/1 ). Copyright: Copyright 2011 Elsevier B.V., All rights reserved.

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N2 - The solubility of Au in Cl- and S-bearing hydrous rhyodacitic and andesitic melts has been experimentally investigated at 1050 °C, 200 MPa and log fO2 close to the Ni/NiO solid oxygen buffer (NNO). The concentrations of Au in the experimental glasses have been determined using Laser Ablation ICP-MS (LA) with special efforts to avoid incorporation of Au micronuggets in the analysis. It is concluded that metal micronuggets are an experimental artefact and produced by Au partitioning into the fluids during heating with consequent precipitation on fluid dissolution in the melting glass powder. Hence, the micronuggets do not represent quench phases and must be excluded from the analysis. The micro-analytical data obtained by LA show that Au concentrations vary from ∼0.2 to ∼2.5 ppm by weight, generally consistent with the literature data for other melt compositions. The measured Au concentrations increase with increasing amounts of Cl and S dissolved in the silicate melt and show a correlation with the apparent activities of Cl and S in the system. The apparent activities of Cl and S are defined by the simplified linear relationship between volatile concentrations in the melt and activity of volatiles. The maximum activity (a* = 1) is assumed to be reached at the saturation of the systems in respect of Cl-rich brine or FeS liquid for Cl and S, respectively. The dependence of Au solubility on the concentrations/activities of Cl and S at the fixed redox conditions shows that Au may form not only oxide- but also Cl- and S-bearing complexes in silicate melts. Furthermore, it indicates that exsolution of S and Cl from the melt by degassing/segregation/crystallization processes may lead to mobilization and extraction of Au into the fluid, liquid and/or mineral phase(s).

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