Effect of layer bending on montmorillonite hydration and structure from molecular simulation

Greathouse, Jeffery A.; Ho, Tuan A.; Jové-Colón, Carlos F.

doi:10.1017/cmn.2024.22

Title: Effect of layer bending on montmorillonite hydration and structure from molecular simulation

Journal Article · 20 November 2024 · Clays and Clay Minerals

DOI: https://doi.org/10.1017/cmn.2024.22 · OSTI ID:2479030

^[1];

^[1]; Jové-Colón, Carlos F. ^[1]

Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Conceptual models of smectite hydration include planar (flat) clay layers that undergo stepwise expansion as successive monolayers of water molecules fill the interlayer regions. However, X-ray diffraction (XRD) studies indicate the presence of interstratified hydration states, suggesting non-uniform interlayer hydration in smectites. Additionally, recent theoretical studies have shown that clay layers can adopt bent configurations over nanometer-scale lateral dimensions with minimal effect on mechanical properties. Therefore, in this study we used molecular simulations to evaluate structural properties and water adsorption isotherms for montmorillonite models composed of bent clay layers in mixed hydration states. Results are compared with models consisting of planar clay layers with interstratified hydration states (e.g. 1W–2W). The small degree of bending in these models (up to 1.5 Å of vertical displacement over a 1.3 nm lateral dimension) had little or no effect on bond lengths and angle distributions within the clay layers. Except for models that included dry states, porosities and simulated water adsorption isotherms were nearly identical for bent or flat clay layers with the same averaged layer spacing. Similar agreement was seen with Na- and Ca-exchanged clays. In conclusion, while the small bent models did not retain their configurations during unconstrained molecular dynamics simulation with flexible clay layers, we show that bent structures are stable at much larger length scales by simulating a 41.6×7.1 nm² system that included dehydrated and hydrated regions in the same interlayer.

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Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE), Office of Spent Fuel and Waste Disposition. Office of Spent Fuel and Waste Science and Technology

Grant/Contract Number:: NA0003525

OSTI ID:: 2479030

Report Number(s):: SAND--2024-15984J

Journal Information:: Clays and Clay Minerals, Journal Name: Clays and Clay Minerals Vol. 72; ISSN 0009-8604

Publisher:: The Clay Minerals Society - IngentaCopyright Statement

Country of Publication:: United States

Language:: English

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58 GEOSCIENCES
X-ray diffraction
bending
clay
grand canonical Monte Carlo
hydration
molecular dynamics
montmorillonite
simulation

Title: Effect of layer bending on montmorillonite hydration and structure from molecular simulation

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