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In situ X-ray absorption spectroscopy measurement of vapour-brine fractionation of antimony at hydrothermal conditions

Published online by Cambridge University Press:  05 July 2018

G. S. Pokrovski ,
J. Roux ,
J.-L. Hazemann ,
A. YU. Borisova ,
A. A. Gonchar  and
M. P. Lemeshko
G. S. Pokrovski*
Affiliation:
Experimental Geochemistry and Biogeochemistry Group, LMTG - Université de Toulouse - CNRS - IRD - OMP, Laboratoire des Mécanismes et Transferts en Géologie, 14 Av. E. Belin, F-31400 Toulouse, France
J. Roux
Affiliation:
Equipe PMM - Institut de Physique du Globe de Paris, 4 Place Jussieu, F-75252 Paris, cedex 05, France
J.-L. Hazemann
Affiliation:
Institut Néel, CNRS, 25 avenue des Martyrs, 38042 Grenoble Cedex 9, France
A. YU. Borisova
Affiliation:
Experimental Geochemistry and Biogeochemistry Group, LMTG - Université de Toulouse - CNRS - IRD - OMP, Laboratoire des Mécanismes et Transferts en Géologie, 14 Av. E. Belin, F-31400 Toulouse, France Geological Department, Moscow State University, Moscow, Russia
A. A. Gonchar
Affiliation:
Department of Chemical Physics, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, D-14195 Berlin, Germany
M. P. Lemeshko
Affiliation:
Department of Molecular Physics, Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, D-14195 Berlin, Germany
*
*E-mail: [email protected]
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Abstract

Despite the growing geological evidence that fluid boiling and vapour-liquid separation affect the distribution of metals in magmatic-hydrothermal systems significantly, there are few experimental data on the chemical status and partitioning of metals in the vapour and liquid phases. Here we report on an in situ measurement, using X-ray absorption fine structure (XAFS) spectroscopy, of antimony speciation and partitioning in the system Sb2O3-H2O-NaCl-HCl at 400°C and pressures 270—300 bar corresponding to the vapour-liquid equilibrium. Experiments were performed using a spectroscopic cell which allows simultaneous determination of the total concentration and atomic environment of the absorbing element (Sb) in each phase. Results show that quantitative vapour-brine separation of a supercritical aqueous salt fluid can be achieved by a controlled decompression and monitoring the X-ray absorbance of the fluid phase. Antimony concentrations in equilibrium with Sb2O3 (cubic, senarmontite) in the coexisting vapour and liquid phases and corresponding SbIII vapour-liquid partitioning coefficients are in agreement with recent data obtained using batch-reactor solubility techniques. The XAFS spectra analysis shows that hydroxy-chloride complexes, probably Sb(OH)2Cl0, are dominant both in the vapour and liquid phase in a salt-water system at acidic conditions. This first in situ XAFS study of element fractionation between coexisting volatile and dense phases opens new possibilities for systematic investigations of vapour-brine and fluid-melt immiscibility phenomena, avoiding many experimental artifacts common in less direct techniques.

Keywords

antimonyX-ray absorption spectroscopyvapour-liquid fractionationSb hydroxy-chloride complexesH2O-NaCl systemmagmatic-hydrothermal deposit
Type
Research Article
Information
Mineralogical Magazine , Volume 72 , Issue 2 , April 2008 , pp. 667 - 681
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 2008

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