Anion-Engineering Toward High-Voltage-Stable Halide Superionic Conductors for All-Solid-State Lithium Batteries

Liang Shen, Jin Liang Li, Wei Jin Kong, Chen Xi Bi, Pan Xu, Xue Yan Huang, Wen Ze Huang, Fang Fu, Yi Cheng Le, Chen Zi Zhao*, Hong Yuan, Jia Qi Huang, Qiang Zhang*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

3 Citations (Scopus)

Abstract

Halide solid electrolytes (SEs) are attracting strong attention as one of the compelling candidates for the next-generation of inorganic SEs due to their high ionic conductivity. Nevertheless, unsatisfactory high-voltage stability restricts the further applications of halide SEs. Herein, the anion-engineering of F/O2− is evolved to construct the high-voltage stable zirconium-based halide superionic conductors (Li2.5ZrCl5F0.5O0.5, LZCFO). Benefiting from the thermodynamic/kinetic high-voltage stability of F-containing SE and the disordered localized structure introduced by O2−, LZCFO displays a practical electrochemical limit of 4.87 V versus Li/Li+ and an ionic conductivity of 1.17 mS cm−1 at 30 °C. With LZCFO and NCM955, the all-solid-state lithium battery exhibits a high discharge capacity of 207.1 mAh g−1 at 0.1C and a capacity retention of 81.2% after 500 cycles at 0.5C. The interfacial characterization further demonstrates the formation of the F-rich cathode–electrolyte interphase (CEI), which inhibits side reactions between the cathode and the SE and boosts excellent cycling stability. This work affords fresh insights on the engineering of SEs with high-voltage stability, high ionic conductivity, and stable CEI in all-solid-state lithium batteries.

Original languageEnglish
Article number2408571
JournalAdvanced Functional Materials
Volume34
Issue number48
DOIs
Publication statusPublished - 26 Nov 2024

Keywords

  • all-solid-state lithium batteries
  • anion-engineering
  • cathode–electrolyte interphase
  • halide solid electrolyte
  • high-voltage stabililty

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