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Thermodynamics of mixing and ordering in pyrope — grossular solid solution

Published online by Cambridge University Press:  05 July 2018

V. L. Vinograd ,
M. H. F. Sluiter ,
B. Winkler ,
A. Putnis ,
U. Hålenius ,
J. D. Gale  and
U. Becker
V. L. Vinograd*
Affiliation:
Institute of Mineralogy, University of Frankfurt, Senckenberganlage 30, 60054 Frankfurt/Main, Germany Department of Mineralogy, Swedish Museum of Natural History, Frescativägen 40, SE-10405, Stockholm, Sweden
M. H. F. Sluiter
Affiliation:
Institute for Materials Research, Tohoku University, Katahira 2-1-1, Aoba-ku, Sendai 980-8577, Japan
B. Winkler
Affiliation:
Institute of Mineralogy, University of Frankfurt, Senckenberganlage 30, 60054 Frankfurt/Main, Germany
A. Putnis
Affiliation:
Institute of Mineralogy, University of Muenster, Correnstrasse 24, 49149, Muenster, Germany
U. Hålenius
Affiliation:
Department of Mineralogy, Swedish Museum of Natural History, Frescativägen 40, SE-10405, Stockholm, Sweden
J. D. Gale
Affiliation:
Department of Chemistry, Imperial College of Science, Technology and Medicine, London SW7 2AZ, UK
U. Becker
Affiliation:
Department of Geological Sciences, University of Michigan, 2534 C.C. Little Building, 425 E. University Ave., Ann Arbor, MI 48109-1063, USA
*
*E-mail: [email protected]
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Abstract

Static lattice energy calculations have been combined with cluster expansion formalism to predict pairwise ordering interactions in the pyrope–grossular solid solution. The ordering interactions, the Js, have been then used to calculate the activity-composition relations over a wide temperature range with the help of the Cluster Variation Method. It is shown that short-range ordering in the system is driven by size mismatch. The prediction of the right signs and magnitudes of the ordering interaction energies requires separation of the mixing enthalpy into the configuration-dependent (chemical) and the configuration-independent (elastic) components. The study predicts the existence of a miscibility gap below 500°C.

Keywords

interatomic potentialspyrope–grossularactivity-composition relations
Type
Research Article
Information
Mineralogical Magazine , Volume 68 , Issue 1 , February 2004 , pp. 101 - 121
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 2004

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Footnotes

†

present address: Nanochemistry Research Institute, Curtin University of Technology, U1987, Perth 6845, Western Australia

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