A structural coarse-grained model for clays using simple iterative Boltzmann inversion

Schaettle, Karl; Ruiz Pestana, Luis; Head-Gordon, Teresa; Lammers, Laura Nielsen

doi:10.1063/1.5011817

Title: A structural coarse-grained model for clays using simple iterative Boltzmann inversion

Journal Article · 20 February 2018 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/1.5011817 · OSTI ID:1532325

^[1]; Ruiz Pestana, Luis ^[2];

^[3]; Lammers, Laura Nielsen ^[3]

Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Cesium-137 is a crucial byproduct of nuclear energy generation and is environmentally threatening due to its long half-life and affinity for naturally occurring micaceous clays. Current experimental observations of illite and phlogopite mica indicate that Cs+ is capable of exchanging with K+ bound in the anhydrous interlayers of layered silicates, forming sharp exchange fronts, leading to interstratification of Cs- and K-illite. We introduce here a coarse-grained (CG) model of the anhydrous illite interlayer developed using iterative Boltzmann inversion that qualitatively and quantitatively reproduces features of a previously proposed feedback mechanism of ion exchange. The CG model represents a 70-fold speedup over all-atom models of clay systems and predicts interlayer expansion for K-illite near ion exchange fronts. Contrary to the longstanding theory that ion exchange in a neighboring layer increases the binding of K in lattice counterion sites leading to interstratification, we find that the presence of neighboring exchanged layers leads to short-range structural relaxations that increase basal spacing and decrease cohesion of the neighboring K-illite layers. We also provide evidence that the formation of alternating Cs- and K-illite interlayers (i.e., ordered interstratification) is both thermodynamically and mechanically favorable compared to exchange in adjacent interlayers.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1532325

Alternate ID(s):: OSTI ID: 1421881

Journal Information:: Journal of Chemical Physics, Vol. 148, Issue 22; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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