A Series of Ternary Metal Chloride Superionic Conductors for High-Performance All-Solid-State Lithium Batteries

Journal article (2022)

Authors

Jianwen Liang University of Western Ontario
E.L. van der Maas RST/Storage of Electrochemical Energy - AS
W. Zhao RST/Storage of Electrochemical Energy - AS
S.R. Parnell RID/TS/Instrumenten groep
S. Ganapathy RID/TS/Instrumenten groep
M. Wagemaker RST/Storage of Electrochemical Energy - AS
Jing Luo University of Western Ontario
Xiaona Li University of Western Ontario
Ning Chen Canadian Ligth Source, Saskatoon
Keegan R. Adair University of Western Ontario
Weihan Li University of Western Ontario
Junjie Li University of Western Ontario
Jue Liu Oak Ridge National Laboratory
Research Group
RST/Storage of Electrochemical Energy (AS) (TU Delft)
Copyright: © 2022 Jianwen Liang, E.L. van der Maas, Jing Luo, Xiaona Li, Ning Chen, Keegan R. Adair, Weihan Li, Junjie Li, Yongfeng Hu, Jue Liu, Li Zhang, W. Zhao, S.R. Parnell, S. Ganapathy, M. Wagemaker
DOI: https://doi.org/10.1002/aenm.202103921
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Published Date

2022

Language

English

Reuse Rights

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Faculty

Applied Sciences

Department

RST/Radiation, Science and Technology

Research Group

RST/Storage of Electrochemical Energy

Abstract

Understanding the relationship between structure, ionic conductivity, and synthesis is the key to the development of superionic conductors. Here, a series of Li3-3xM1+xCl6 (−0.14 < x ≤ 0.5, M = Tb, Dy, Ho, Y, Er, Tm) solid electrolytes with orthorhombic and trigonal structures are reported. The orthorhombic phase of Li–M–Cl shows an approximately one order of magnitude increase in ionic conductivities when compared to their trigonal phase. Using the Li–Ho–Cl components as an example, their structures, phase transition, ionic conductivity, and electrochemical stability are studied. Molecular dynamics simulations reveal the facile diffusion in the z-direction in the orthorhombic structure, rationalizing the improved ionic conductivities. All-solid-state batteries of NMC811/Li2.73Ho1.09Cl6/In demonstrate excellent electrochemical performance at both 25 and −10 °C. As relevant to the vast number of isostructural halide electrolytes, the present structure control strategy guides the design of halide superionic conductors.

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