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Ab Initio Molecular Dynamics Study of Fe-Containing Smectites

Published online by Cambridge University Press:  01 January 2024

Xiandong Liu ,
Evert Jan Meijer ,
Xiancai Lu  and
Rucheng Wang
Xiandong Liu*
Affiliation:
State Key Laboratory for Mineral Deposit Research, School of Earth Sciences and Engineering, Nanjing University, Nanjing 210093, P.R. China
Evert Jan Meijer*
Affiliation:
Van’t Hoff Institute for Molecular Sciences and Amsterdam Center for Multiscale Modeling, University of Amsterdam, Nieuwe Achtergracht 166, 1018 WV Amsterdam, The Netherlands
Xiancai Lu
Affiliation:
State Key Laboratory for Mineral Deposit Research, School of Earth Sciences and Engineering, Nanjing University, Nanjing 210093, P.R. China
Rucheng Wang
Affiliation:
State Key Laboratory for Mineral Deposit Research, School of Earth Sciences and Engineering, Nanjing University, Nanjing 210093, P.R. China
*
* E-mail address of corresponding author: xiandongliu@gmail.com
† e.j.meijer@uva.nl
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Abstract

In order to identify the influences imposed by Fe substitution, density functional theory-based Car-Parrinello molecular dynamics simulations were employed to study both oxidized and reduced Febearing smectites. The following basic properties were investigated: local structures in the clay layer, hydroxyl orientations, and the vibration dynamics of H and Si. Structural analyses indicated that the average Fe-O bond lengths are ~2.08 Å and 2.02 Å in the reduced and oxidized models, respectively, and the Fe substitutions did not affect the coordination structures of the Al-O and Si-O polyhedra. For hydroxyl orientations, Fe(III) substitution had no obvious influence but Fe(II) forces the coordinated hydroxyls to present a wide-angle distribution. Furthermore, the present work has shown that both substitutions can red-shift the hydroxyl in-plane bending mode. The analyses also revealed that Fe(III) substitution has no effect on the Si-O stretching, while Fe reduction causes a blue-shift of the out-of-plane stretching mode. The results provide quantitative constraints and clues for future research.

Keywords

CPMDDensity Functional TheoryHydroxyl OrientationIronSmectiteVibration Dynamics
Type
Article
Information
Clays and Clay Minerals , Volume 58 , Issue 1 , February 2010 , pp. 89 - 96
Copyright
Copyright © Clay Minerals Society 2010

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