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Structure and Dynamics of Water—Smectite Interfaces: Hydrogen Bonding and the Origin of the Sharp O-Dw/O—Hw Infrared Band From Molecular Simulations

Published online by Cambridge University Press:  01 January 2024

Marek Szczerba ,
Artur Kuligiewicz ,
Arkadiusz Derkowski ,
Vassilis Gionis ,
Georgios D. Chryssikos  and
Andrey G. Kalinichev
Marek Szczerba*
Affiliation:
Institute of Geological Sciences, Polish Academy of Sciences, Kraków, Poland
Artur Kuligiewicz
Affiliation:
Institute of Geological Sciences, Polish Academy of Sciences, Kraków, Poland
Arkadiusz Derkowski
Affiliation:
Institute of Geological Sciences, Polish Academy of Sciences, Kraków, Poland
Vassilis Gionis
Affiliation:
Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, Athens, Greece
Georgios D. Chryssikos
Affiliation:
Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, Athens, Greece
Andrey G. Kalinichev
Affiliation:
Laboratoire SUBATECH (UMR 6457), Ecole des Mines de Nantes, Nantes, France
*
*E-mail address of corresponding author: [email protected]
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Abstract

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Experimental studies have shown that a sharp, high-frequency IR band at ~3615 cm-1 (in H2O form) and at ~2685 cm-1 (in D2O form) is a common feature for all smectites, and its position correlates with layer charge. In order to explain the molecular origin of this band in terms of total layer charge, charge localization, as well as nature of interlayer cations influencing the position and intensity of this peak, a series of classical molecular dynamics (MD) simulations was performed for several smectite models. The smectite layers were described using a modified CLAYFF force field, where the intramolecular vibrations of H2O were described more accurately by the Toukan-Rahman potential. The power spectra of molecular vibrations of hydrogens were calculated for selected sub-sets of interlayer H2O to analyze quantitatively their contribution to the observed spectral features. The statistics of hydrogen bonds in the smectite interlayers were also analyzed to support the spectral calculations.

The simulation results demonstrated clearly that only the H2O molecules in close proximity to the smectite surface are responsible for the sharp vibrational band observed. Other hypotheses for the possible origins of this band were considered carefully and eventually rejected. Two orientations of H2O molecules donating one or two H bonds to the basal oxygens of the smectite surface (monodentate and bidentate orientations, respectively) were observed. In both orientations, these H bonds are quite weak, pointing to a generally hydrophobic character of the smectite surface. Both orientations contributed to the high-frequency band, but the monodentate orientation provided the predominant contribution because surface H2O molecules in this orientation were much more abundant. In good agreement with experiment, only a small difference in the peak position was observed between smectites with different charge localization. The effect of the total layer charge, i.e. the red-shift for higher-charge smectites, was also confirmed. This shift arose from the decrease in the H-bonding distances of H2O in monodentate and bidentate orientation.

Keywords

Adsorbed WaterClay—Water InterfaceInfrared SpectroscopyMolecular DynamicsSmectite
Type
Article
Information
Clays and Clay Minerals , Volume 64 , Issue 4 , August 2016 , pp. 452 - 471
Copyright
Copyright © The Clay Minerals Society 2016

Footnotes

This paper is published as part of a special issue on the subject of ‘Computational Molecular Modeling.’ Some of the papers were presented during the 2015 Clay Minerals Society-Euroclay Conference held in Edinburgh, UK.

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