Molecular Dynamics Modeling of the Structure and Na+-Ion Transport in Na2S + SiS2 Glassy Electrolytes

Dive, A.; Benmore, C.; Wilding, M.; Martin, S. W.; Beckman, S.; Banerjee, Soumik

doi:10.1021/acs.jpcb.8b04353

Title: Molecular Dynamics Modeling of the Structure and Na⁺-Ion Transport in Na₂S + SiS₂ Glassy Electrolytes

Journal Article · Wed Jun 20 00:00:00 EDT 2018 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/acs.jpcb.8b04353· OSTI ID:1480490

^[1]; Benmore, C. ^[2]; Wilding, M. ^[3]; Martin, S. W. ^[4]; Beckman, S. ^[1];

^[1]

Washington State Univ., Pullman, WA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. College London, London (United Kingdom)
Iowa State Univ., Ames, IA (United States)

Solid-state sodium batteries, a relatively safe and potentially cost-effective energy-storage technology, have attracted increasing scientific attention recently for application in stationary grid-scale energy storage. Identifying solid electrolytes with high electrochemical stability and high Na+-ion conductivity at room temperature is critically important to enable high energy densities with enhanced rate capabilities. We evaluated sodium sulfide silicon sulfide, xNa₂S + (1 - x)SiS₂, glasses as potential glassy solid electrolytes (GSEs) using molecular dynamics (MD) simulations. We employed ab initio MD to determine ion conduction mechanisms, to calculate energy barriers for ion hops, and to correlate these to the local short-range structure of 0.50Na₂S + 0.50SiS₂ glass. To simulate much larger systems for accurately calculating the ionic conductivity, we parameterized empirical Buckingham-type potential and performed classical MD simulations. After validating these calculations by comparing the structure obtained from MD to that from X-ray scattering data, we calculated the ionic conductivity of these glasses for the range of 0.33 ≤ x ≤ 0.67 compositions. The calculated ionic conductivities at room temperature were in the range of similar to 10^-5 S/cm for the x = 0.50 composition and increased significantly with sodium sulfide (x) content. Furthermore, these calculations provide theoretical insights into the role of Na₂S content on the ionic conductivity of GSEs aiding in the selection of specific compositions to enhance the ionic conductivity.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Advanced Research Projects Agency - Energy (ARPA-E)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1480490

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 122, Issue 30; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 12 works

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