Structure, Energetics, and Dynamics of Smectite Clay Interlayer Hydration: Molecular Dynamics and Metadynamics Investigation of Na-Hectorite Journal: The Journal of Physical Chemistry Manuscript ID: jp-2012-12286g.R1 Manuscript Type: Article Date Submitted by the Author: 04-Feb-2013 Complete List of Authors: Morrow, Christin; Michigan State University, Chemistry Yazaydin, Ahmet; Michigan State University, Department of Chemistry; University of Surrey, Chemical Engineering Krishnan, Marimuthu; International Institute of Information Technology, Center for Computational Natural Sciences and Bioinformatics Bowers, Geoffrey; Alfred University, Chemistry; Alfred University, Department of Materials Engineering Kalinichev, Andrey; Michigan State University, Department of Chemistry; Ecole des Mines de Nantes, Laboratoire SUBATECH - Groupe de Radiochimie Kirkpatrick, R.; Michigan State University, Natural Science ACS Paragon Plus Environment The Journal of Physical Chemistry
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Structure, Energetics, and Dynamics of Smectite Clay Interlayer Hydration: Molecular Dynamics and
Metadynamics Investigation of Na-Hectorite
Journal: The Journal of Physical Chemistry
Manuscript ID: jp-2012-12286g.R1
Manuscript Type: Article
Date Submitted by the Author: 04-Feb-2013
Complete List of Authors: Morrow, Christin; Michigan State University, Chemistry Yazaydin, Ahmet; Michigan State University, Department of Chemistry; University of Surrey, Chemical Engineering
Krishnan, Marimuthu; International Institute of Information Technology, Center for Computational Natural Sciences and Bioinformatics Bowers, Geoffrey; Alfred University, Chemistry; Alfred University, Department of Materials Engineering Kalinichev, Andrey; Michigan State University, Department of Chemistry; Ecole des Mines de Nantes, Laboratoire SUBATECH - Groupe de Radiochimie Kirkpatrick, R.; Michigan State University, Natural Science
ACS Paragon Plus Environment
The Journal of Physical Chemistry
1
Structure, Energetics, and Dynamics of Smectite Clay Interlayer Hydration: Molecular Dynamics and Metadynamics Investigation of Na-Hectorite
Christin P. Morrow,1,* A. Özgür Yazaydin,1,2 Marimuthu Krishnan,1,3 Geoffrey M. Bowers,4,5
Andrey G. Kalinichev,1,6 and R. James Kirkpatrick7
1Department of Chemistry, Michigan State University, East Lansing, MI USA 48824
2Department of Chemical Engineering, University of Surrey, Guildford, UK GU2 7XH 3Center for Computational Natural Sciences and Bioinformatics, International Institute of
Information Technology, Gachibowli, Hyderabad India 500 032
4Division of Chemistry, Alfred University, Alfred, NY USA 14802 5Department of Materials Engineering, Alfred University, Alfred, NY USA 14802
6Laboratoire SUBATECH, École des Mines de Nantes, Nantes Cedex 3, France 44307 7College of Natural Science, Michigan State University, East Lansing, MI USA 48824
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Figure Captions Figure 1: Snapshots of Na-hectorite with (a) 0 H2O/Na+, (b) 0.6 H2O/Na+, (c) 3 H2O/Na+, (d) 5.5
H2O/Na+, and (e) 10 H2O/Na+ samples viewed parallel to the clay layers down the b-axis. Mg octahedra are yellow, Li octahedra lilac, Si tetrahedra green, O atoms red, H atoms white, and Na ions cyan.
Figure 2: Schematic diagrams of (a) SN–Na–OH2O, θ, (b) SN–OH2O–HHBi, ω, and (c) OH2O–Na–OH2O, φ,
angles, illustrating the geometry of the Na+ ion octahedra and the orientation of the H2O molecules. The color scheme is the same as Figure 1.
Figure 3: Hydration energy of Na-hectorite versus hydration level (H2O/Na+), where the dehydrated
sample was used as the reference state and values were calculated according to Equation 1. The hydration energy (-40 kJ/mol) of bulk water with the SPC potential is shown as the dashed black line.
Figure 3: Hydration energy of Na-hectorite versus hydration level (H2O/Na+), where the dehydrated
sample was used as the reference state and values were calculated according to Equation 1. The hydration energy (-40 kJ/mol) of bulk water with the SPC potential is shown as the dashed black line.
Figure 4: Atomic density profiles of Na+ ions, OH2O atoms, and HH2O atoms in the interlayers of the Na-
hectorite samples. The positions of the basal O atoms are vertical black dashed lines. Na+ ions are green lines, OH2O atoms red, and HH2O atoms blue.
Figure 5: Interlayer spacing (Å) versus hydration level (H2O/Na+) for interlayer Na-hectorite samples. Figure 6: Radial distribution functions (solid lines) and coordination numbers (dashed lines) for (a) Na–
OMIN and (b) Na–OH2O for Na+ ions in the interlayers of Na-hectorite. Figure 7: (a) Number of hydrogen bonds per water molecule (HBs/H2O) as a function of H2O/Na+. (b)
Fraction of water molecules with given number of HBs as a function of H2O/Na+. Figure 8: Distribution of (a) SN–Na–OH2O (°) and (b) SN–OH2O–HHBi (°) angles as a function of
hydration level. Figure 9: Atomic positions of the (a) Na+ ions in the 0, 0.6 and 3 H2O/Na+ samples, (b) OH2O atoms in
the 0.6 and 10 H2O/Na+ samples, and (c) HH2O atoms 10 H2O/Na+ sample. Si atoms are closed circles, OMIN atoms open circles, Na+ ions turquoise plus signs, OH2O atoms red plus signs, and HH2O atoms blue plus signs. Solid and dashed lines mark Si–O hexagonal rings of the top and bottom sides of the interlayer, respectively.
Figure 10: Free energies for the SN–Na–OH2O angles, θ, from metadynamics calculations, showing the
energy minima (kJ/mol) for the (a) 1 WL and (b) 2 WL samples. Figure 11: Free energies for the OH2O–Na–OH2O angles, φ, from metadynamics calculations, showing the
energy minima (kJ/mol) for the (a) 1 WL and (b) 2 WL samples.
Figure 1: Snapshots of Na-hectorite with (a) 0 H2O/Na+, (b) 0.6 H2O/Na+, (c) 3 H2O/Na+, (d) 5.5 H2O/Na+, and (e) 10 H2O/Na+ samples viewed parallel to the clay layers down the b-axis. Mg octahedra are yellow, Li octahedra lilac, Si tetrahedra green, O atoms red, H atoms white, and Na ions cyan.
Figure 2: Schematic diagrams of (a) SN–Na–OH2O, θ, (b) SN–OH2O–HHBi, ω, and (c) OH2O–Na–OH2O, φ, angles, illustrating the geometry of the Na+ ion octahedra and the orientation of the H2O molecules. The color scheme is the same as Figure 1.
Figure 3: Hydration energy of Na-hectorite versus hydration level (H2O/Na+), where the dehydrated sample was used as the reference state and values were calculated according to Equation 1. The hydration energy (-40 kJ/mol) of bulk water with the SPC potential is shown as the dashed black line.
Figure 4: Atomic density profiles of Na+ ions, OH2O atoms, and HH2O atoms in the interlayers of the Na-hectorite samples. The positions of the basal O atoms are vertical black dashed lines. Na+ ions are green lines, OH2O atoms red, and HH2O atoms blue.
Figure 6: Radial distribution functions (solid lines) and coordination numbers (dashed lines) for (a) Na–OMIN and (b) Na–OH2O for Na+ ions in the interlayers of Na-hectorite.
Figure 7: (a) Number of hydrogen bonds per water molecule (HBs/H2O) as a function of H2O/Na+. (b) Fraction of water molecules with given number of HBs as a function of H2O/Na+.
Figure 9: Atomic positions of the (a) Na+ ions in the 0, 0.6 and 3 H2O/Na+ samples, (b) OH2O atoms in the 0.6 and 10 H2O/Na+ samples, and (c) HH2O atoms 10 H2O/Na+ sample. Si atoms are closed circles, OMIN atoms open circles, Na+ ions turquoise plus signs, OH2O atoms red plus signs, and HH2O atoms blue plus signs. Solid and dashed lines mark Si–O hexagonal rings of the top and bottom sides of the interlayer, respectively.
Figure 10: Free energies for the SN–Na–OH2O angles, θ, from metadynamics calculations, showing the energy minima (kJ/mol) for the (a) 1 WL and (b) 2 WL samples.
Figure 11: Free energies for the OH2O–Na–OH2O angles, φ, from metadynamics calculations, showing the energy minima (kJ/mol) for the (a) 1 WL and (b) 2 WL samples.