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

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

doi:10.1016/j.mtphys.2021.100478

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

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

Research output: Contribution to journal › Article › peer-review

13 Scopus citations

Abstract

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. This work demonstrates 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., PS₄³⁻ and P₂S₇⁴⁻) correlate with higher Li⁺ mobility compared to other polyanions (e.g., (PS₃)_n^n– chains and P₂S₆⁴⁻). Overall, this work demonstrates how ssNMR and nPDF can be used to draw key structure/function correlations for solid-state superionic conductors.

Original language	English
Article number	100478
Journal	Materials Today Physics
Volume	21
DOIs	https://doi.org/10.1016/j.mtphys.2021.100478
State	Published - Nov 2021

Funding

Research conducted at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) was sponsored by the Office of Energy Efficiency and Renewable Energy (EERE) in the Vehicle Technologies Office (VTO) through the Advanced Battery Materials Research (BMR) Program. Neutron scattering experiments were performed on the NOMAD beamline at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory. The NMR work at Hunter College was also supported by the U.S. Office of Naval Research (grant #N00014-20-1-2186 ). D.M. acknowledges financial support from the National Institutes of Health RISE program at Hunter College (grant GM060665 ). Research conducted at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) was sponsored by the Office of Energy Efficiency and Renewable Energy (EERE) in the Vehicle Technologies Office (VTO) through the Advanced Battery Materials Research (BMR) Program. Neutron scattering experiments were performed on the NOMAD beamline at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory. The NMR work at Hunter College was also supported by the U.S. Office of Naval Research (grant #N00014-20-1-2186). D.M. acknowledges financial support from the National Institutes of Health RISE program at Hunter College (grant GM060665).

Keywords

Lithium thiophosphate
NMR
Pair distribution function
Solid electrolytes
Solvent-mediated synthesis

Access to Document

10.1016/j.mtphys.2021.100478

Cite this

@article{7880d9b408c144c6b3ee53f5f9adfaf3,

title = "Investigation of glass-ceramic lithium thiophosphate solid electrolytes using NMR and neutron scattering",

abstract = "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. This work demonstrates 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., PS43− and P2S74−) correlate with higher Li+ mobility compared to other polyanions (e.g., (PS3)nn– chains and P2S64−). Overall, this work demonstrates how ssNMR and nPDF can be used to draw key structure/function correlations for solid-state superionic conductors.",

keywords = "Lithium thiophosphate, NMR, Pair distribution function, Solid electrolytes, Solvent-mediated synthesis",

author = "Self, \{Ethan C.\} and Chien, \{Po Hsiu\} and O'Donnell, \{Lauren F.\} and Daniel Morales and Jue Liu and Teerth Brahmbhatt and Steven Greenbaum and Jagjit Nanda",

note = "Publisher Copyright: {\textcopyright} 2021 Elsevier Ltd",

year = "2021",

month = nov,

doi = "10.1016/j.mtphys.2021.100478",

language = "English",

volume = "21",

journal = "Materials Today Physics",

issn = "2542-5293",

publisher = "Elsevier",

}

TY - JOUR

T1 - Investigation of glass-ceramic lithium thiophosphate solid electrolytes using NMR and neutron scattering

AU - Self, Ethan C.

AU - Chien, Po Hsiu

AU - O'Donnell, Lauren F.

AU - Morales, Daniel

AU - Liu, Jue

AU - Brahmbhatt, Teerth

AU - Greenbaum, Steven

AU - Nanda, Jagjit

PY - 2021/11

Y1 - 2021/11

N2 - 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. This work demonstrates 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., PS43− and P2S74−) correlate with higher Li+ mobility compared to other polyanions (e.g., (PS3)nn– chains and P2S64−). Overall, this work demonstrates how ssNMR and nPDF can be used to draw key structure/function correlations for solid-state superionic conductors.

AB - 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. This work demonstrates 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., PS43− and P2S74−) correlate with higher Li+ mobility compared to other polyanions (e.g., (PS3)nn– chains and P2S64−). Overall, this work demonstrates how ssNMR and nPDF can be used to draw key structure/function correlations for solid-state superionic conductors.

KW - Lithium thiophosphate

KW - NMR

KW - Pair distribution function

KW - Solid electrolytes

KW - Solvent-mediated synthesis

UR - https://www.scopus.com/pages/publications/85111068745

U2 - 10.1016/j.mtphys.2021.100478

DO - 10.1016/j.mtphys.2021.100478

M3 - Article

AN - SCOPUS:85111068745

SN - 2542-5293

VL - 21

JO - Materials Today Physics

JF - Materials Today Physics

M1 - 100478

ER -

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

Abstract

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Cite this