Issue 11, 2023

New insights into aliovalent substituted halide solid electrolytes for cobalt-free all-solid state batteries

Abstract

Halide solid electrolytes (SEs) have garnered significant attention due to their decent ionic conductivity and exceptional high-voltage stability. However, their structure–property relationship remains enigmatic. In this work, we synthesize a range of Li3−xLu1−xZrxCl6 (LLZC, 0 < x < 1) solid solutions to investigate the influence of lithium ion and vacant site contents on ionic conductivity. Contrary to our previous understanding, it is found that achieving a balance in lithium ion and vacant site content, rather than aliovalent substitution-induced structural changes that introduce stacking faults, plays a crucial role in optimizing ion transport in a hexagonal close packing (hcp) anion framework. This balance culminates in the highest ionic conductivity (1.5 mS cm−1) and lowest activation energy (0.285 eV) of LLZC. In addition, aliovalent substitution strengthens the oxidative stability of halide SSEs but reduces their reduction stability. Using LLZC as SEs and LiMn2O4 as cathodes, cobalt-free all-solid-state batteries undergo 1000 cycles of stable cycling at 0.3 C with negligible capacity decay.

Graphical abstract: New insights into aliovalent substituted halide solid electrolytes for cobalt-free all-solid state batteries

Supplementary files

Article information

Article type
Paper
Submitted
08 Apr 2023
Accepted
21 Aug 2023
First published
15 Sep 2023

Energy Environ. Sci., 2023,16, 5136-5143

New insights into aliovalent substituted halide solid electrolytes for cobalt-free all-solid state batteries

C. Wang, S. Wang, X. Liu, Y. Wu, R. Yu, H. Duan, J. T. Kim, H. Huang, J. Wang, Y. Mo and X. Sun, Energy Environ. Sci., 2023, 16, 5136 DOI: 10.1039/D3EE01119D

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