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Ab initio calculations of relative stabilities of different structural arrangements in dioctahedral phyllosilicates

Published online by Cambridge University Press:  01 January 2024

Daniel Tunega
Affiliation:
Institute for Theoretical Chemistry, University of Vienna, Währingerstrasse 17, A-1090 Vienna, Austria Department of Environmental Research, Austrian Research Centers GmbH — ARC, A-2444 Seibersdorf, Austria
Bernard A. Goodman*
Affiliation:
Department of Environmental Research, Austrian Research Centers GmbH — ARC, A-2444 Seibersdorf, Austria Department of Natural Resources and Environmental Sciences, University of Illinois at Urbana-Champaign, Urbana, IL 61801, USA
Georg Haberhauer
Affiliation:
Department of Environmental Research, Austrian Research Centers GmbH — ARC, A-2444 Seibersdorf, Austria
Thomas G. Reichenauer
Affiliation:
Department of Environmental Research, Austrian Research Centers GmbH — ARC, A-2444 Seibersdorf, Austria
Martin H. Gerzabek
Affiliation:
Institute of Soil Research, University of Natural Resources and Applied Life Sciences, Peter-Jordan-Strasse 82b, A-1190 Vienna, Austria
Hans Lischka
Affiliation:
Institute for Theoretical Chemistry, University of Vienna, Währingerstrasse 17, A-1090 Vienna, Austria
*
*E-mail address of corresponding author: bernard_a_goodman@yahoo.com

Abstract

An ab initio theoretical approach has been used to calculate optimized geometries and the relative energies of various compositional arrangements in structures of dioctahedral smectites based on models consisting of two unit-cells. These calculations indicate that the energy differences between structures having vacancies in sites with cis- or trans-OH coordination are small and that their relative energies vary with the chemical nature of the substitutions. For example, a cis-OH coordination for the vacancy was the most stable when the interlayer charge originated from substitution of Al for Si in the tetrahedral sheet, whereas the trans-coordination was the more stable for most cases of substitution in the octahedral sheet, an exception being Fe(II) for Al where the cis-OH coordination was favored. It seems likely, therefore, that long-range structural disorder will be a common phenomenon in natural phyllosilicate specimens.

Type
Research Article
Copyright
Copyright © 2007, The Clay Minerals Society

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