Investigation of glass-ceramic lithium thiophosphate solid electrolytes using NMR and neutron scattering

Self, Ethan C.; Chien, Po-Hsiu; O'Donnell, Lauren F.; Morales, Daniel; Liu, Jue; Brahmbhatt, Teerth; Greenbaum, Steven; Nanda, Jagjit

doi:10.1016/j.mtphys.2021.100478

Investigation of glass-ceramic lithium thiophosphate solid electrolytes using NMR and neutron scattering

Journal Article · Wed Jul 07 04:00:00 EDT 2021 · Materials Today Physics

DOI:https://doi.org/10.1016/j.mtphys.2021.100478· OSTI ID:1823360

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Tennessee, Knoxville, TN (United States)
City Univ. of New York (CUNY), NY (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

Solid-state Li batteries require solid electrolytes which have high Li+ conductivity and good chemical/mechanical compatibility with Li metal anodes and high energy cathodes. Structure/function correlations which relate local bonding to macroscopic properties are needed to guide development of new solid electrolyte materials. This study combines diffraction measurements with solid-state nuclear magnetic resonance spectroscopy (ssNMR) and neutron pair distribution function (nPDF) analysis to probe the short-range vs. long-range structure of glass-ceramic Li₃PS₄-based solid electrolytes. Here, we demonstrate how different synthesis conditions (e.g., solvent selection and thermal processing) affect the resulting polyanionic network. More specifically, structures with high P coordination numbers (e.g., PS₄^3– and P₂S₇^4–) correlate with higher Li⁺ mobility compared to other polyanions (e.g., (PS₃)_n^n– chains and P₂S₆^4–). Overall, this work demonstrates how ssNMR and nPDF can be used to draw key structure/function correlations for solid-state superionic conductors.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; US Department of the Navy, Office of Naval Research (ONR); National Institutes of Health (NIH)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1823360

Alternate ID(s):: OSTI ID: 1810168

Journal Information:: Materials Today Physics, Journal Name: Materials Today Physics Vol. 21; ISSN 2542-5293

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
NMR
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pair distribution function
solid electrolytes
solvent-mediated synthesis

Investigation of glass-ceramic lithium thiophosphate solid electrolytes using NMR and neutron scattering

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