Computational design of a mixed A-site cation halide solid electrolyte for all-solid-state lithium batteries
Publication Name
Journal of Materials Chemistry A
Abstract
All-solid-state Li-ion batteries (ASSBs) are considered as ideal next-generation energy storage devices owing to their safe operation and high energy densities. Recently, halide-based solid electrolytes (SEs) have come under the spotlight because of their wide electrochemical stability windows and high ionic conductivities. However, their usage as coating materials for cathodes is limited. To examine the wide electrochemical stability window of SEs for lithium-metal anodes and their interfacial stability with high-voltage cathodes, a systematic first-principles investigation of A-site cation and anion exchange in Li3MX6 (M: Lu, Sc, Bi, In, Y, Tm, Dy, Ho, Er, Tm, Sm, Tb; X: Br, Cl, and I) was conducted. The systematic analysis showed that the electrochemical behavior of chloride SEs can be modulated by mixing M3+ cations. Furthermore, the replacement of M3+ by Zr4+ and the anionic blending of Br with Cl, which exhibits a relatively high ionic conductivity, was also computed for comparison with the A-site cation-mixed halide electrolyte. Our computational work provides an overview of the evolution of lithium halide SEs in high-voltage ASSBs.
Open Access Status
This publication is not available as open access
Funding Number
2022M3J1A1085409
Funding Sponsor
Chung-Ang University