SEM-Drude Model for the Accurate and Efficient Simulation of MgCl 2 -KCl Mixtures in the Condensed Phase.

Autor: Sharma S; Department of Chemistry, The University of Iowa, Iowa City, Iowa 52242, United States., Emerson MS; Department of Chemistry, The University of Iowa, Iowa City, Iowa 52242, United States., Wu F; Department of Chemistry, The University of Iowa, Iowa City, Iowa 52242, United States., Wang H; Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana 46556, United States., Maginn EJ; Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, Indiana 46556, United States., Margulis CJ; Department of Chemistry, The University of Iowa, Iowa City, Iowa 52242, United States.
Jazyk: angličtina
Zdroj: The journal of physical chemistry. A [J Phys Chem A] 2020 Sep 24; Vol. 124 (38), pp. 7832-7842. Date of Electronic Publication: 2020 Sep 11.
DOI: 10.1021/acs.jpca.0c06721
Abstrakt: There is a long history of models that to different extents reproduce structural and dynamical properties of high-temperature molten salts. Whereas rigid ion models can work fairly well for some of the monovalent salts, polarizability is fundamentally important when small divalent or multivalent cations are combined with significantly polarizable anions such as Cl - to form networked liquids that display a first sharp diffraction peak. There are excellent polarizable ion models (PIMs) for these systems, but there has been little success with the less expensive Core-Shell type models, which are often described as unwieldy or difficult to fit. In this article, we present the Sharma-Emerson-Margulis (SEM)-Drude model for MgCl 2 /KCl mixtures that with the same ingredients used in the latest and most accurate PIM models overcome the aforementioned obstacles at significantly less computational cost; structural and dynamical properties are for all practical purposes very similar to what we obtain from the PIM but typical simulations can be more than 30 times faster. This has allowed us not only to expand our recent studies on the temperature and composition dependence of intermediate range order in MgCl 2 /KCl mixtures but also to access transport properties that were simply too costly to properly sample in our recently published studies.
Databáze: MEDLINE
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