TY - JOUR
T1 - Solubility and transport of platinum-group elements in supercritical fluids
T2 - Summary and estimates of thermodynamic properties for ruthenium, rhodium, palladium, and platinum solids, aqueous ions, and complexes to 1000°C and 5 kbar
AU - Sassani, David C.
AU - Shock, Everett L.
N1 - Funding Information:
—The research described above represents a portion of the senior author’s Ph.D. dissertation at Washington University and benefitted greatly from discussions with Jill Pasteris, Dimitri Sverjensky, Dennis Bird, Craig Manning, Marc Willis, Craig Schiffries, Lee Hsu, Drew Tait, Alan Boudreau, and Jim Johnson. Critical comments from Jill Pasteris, Chris Gammons, Attila Kilinc, and Scott Wood greatly enhanced the present manuscript. Discussions with Dimitri Sverjensky on aqueous complex formation and correlation of thermodynamic properties provided the groundwork for this study. We are indebted to Mitch Schulte for translations, and to Carla Koretsky, Patty Dubois, Heidi Betz, Jen Barmann, Bill Winston, ifer Thieme, Brian Zaleski, Dee Becker, and Barbara Winston for their technical assistance. This research was supported by NSF grants EAR-8905018 and OCE-9220337. This is GEOPIG contribution #57.
PY - 1998/8
Y1 - 1998/8
N2 - Several correlation methods are used to estimate data and equation-of-state parameters that permit calculation of standard state thermodynamic properties at high pressures and temperatures for metals, oxides, and sulfides, as well as ions, and aqueous chloride, hydroxide, and sulfate complexes of Ru+2, Ru+3, Rh+2, Rh+3, Pd+2, and Pt+2. Estimates are based on a critical review of data from the literature at 25°C and 1 bar. The combined data for 14 minerals, 6 cations, and 56 aqueous complexes provide a foundation for quantitative predictions of aqueous speciation of these platinum group elements (PGE), as well as platinum group mineral (PGM) solubilities as functions of pH, oxidation state, and chloride and sulfate content of geologic fluids at temperatures to 1000°C and pressures to 5 kbar. Therefore, these estimates are the first to address PGE speciation at the pressure and temperatures of most PGM deposits. Comparisons are made to other theoretical predictions of platinum-group element (PGE) complex formation in aqueous solutions and to pertinent experimental data. We conclude that Pd-chloride complexes may be less stable at lower temperatures than previously predicted by other investigators, but that Pt-chloride complexes may be considerably more stable.
AB - Several correlation methods are used to estimate data and equation-of-state parameters that permit calculation of standard state thermodynamic properties at high pressures and temperatures for metals, oxides, and sulfides, as well as ions, and aqueous chloride, hydroxide, and sulfate complexes of Ru+2, Ru+3, Rh+2, Rh+3, Pd+2, and Pt+2. Estimates are based on a critical review of data from the literature at 25°C and 1 bar. The combined data for 14 minerals, 6 cations, and 56 aqueous complexes provide a foundation for quantitative predictions of aqueous speciation of these platinum group elements (PGE), as well as platinum group mineral (PGM) solubilities as functions of pH, oxidation state, and chloride and sulfate content of geologic fluids at temperatures to 1000°C and pressures to 5 kbar. Therefore, these estimates are the first to address PGE speciation at the pressure and temperatures of most PGM deposits. Comparisons are made to other theoretical predictions of platinum-group element (PGE) complex formation in aqueous solutions and to pertinent experimental data. We conclude that Pd-chloride complexes may be less stable at lower temperatures than previously predicted by other investigators, but that Pt-chloride complexes may be considerably more stable.
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U2 - 10.1016/S0016-7037(98)00049-0
DO - 10.1016/S0016-7037(98)00049-0
M3 - Article
AN - SCOPUS:0032464845
SN - 0016-7037
VL - 62
SP - 2643
EP - 2671
JO - Geochmica et Cosmochimica Acta
JF - Geochmica et Cosmochimica Acta
IS - 15
ER -