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Li2ZrF6 protective layer enabled high-voltage LiCoO2 positive electrode in sulfide all-solid-state batteries

Author

Listed:
  • Xing Zhou

    (Fudan University
    Contemporary Amperex Technology Ltd. (CATL))

  • Chia-Yu Chang

    (National Taiwan University of Science and Technology (NTUST))

  • Dongfang Yu

    (Westlake University)

  • Kai Zhang

    (Fudan University)

  • Zhi Li

    (Fudan University)

  • Shi-Kai Jiang

    (National Taiwan University of Science and Technology (NTUST))

  • Yizhou Zhu

    (Westlake University)

  • Yongyao Xia

    (Fudan University)

  • Bing Joe Hwang

    (National Taiwan University of Science and Technology (NTUST)
    National Taiwan University of Science and Technology (NTUST)
    National Synchrotron Radiation Research Center (NSRRC)
    National Taiwan University of Science and Technology (NTUST))

  • Yonggang Wang

    (Fudan University)

Abstract

The application of high-voltage positive electrode materials in sulfide all-solid-state lithium batteries is hindered by the limited oxidation potential of sulfide-based solid-state electrolytes (SSEs). Consequently, surface coating on positive electrode materials is widely applied to alleviate detrimental interfacial reactions. However, most coating layers also react with sulfide-based SSEs, generating electronic conductors and causing gradual interface degradation and capacity fading. To address this, we propose a Li2ZrF6 coating layer on LiCoO2, which exhibits minimal reaction with SSEs, and its decomposition products are electron-conductive-free. Furthermore, this coating layer also efficiently mitigates the layered-to-spinel/rock-salt surface structural transformation in LiCoO2. As a result, the In-Li|Li6PS5Cl | Li2ZrF6-LiCoO2 all-solid-state cell demonstrates an initial areal capacity of 5.2 mAh cm−2 and a capacity retention of 80.5% after 1500 cycles at 70 mA/g with high LiCoO2 areal mass loading (30.19 mg cm−2) and a cut-off voltage of 3.9 V (corresponding to potential of 4.5 V versus Li+/Li), at 25 °C.

Suggested Citation

  • Xing Zhou & Chia-Yu Chang & Dongfang Yu & Kai Zhang & Zhi Li & Shi-Kai Jiang & Yizhou Zhu & Yongyao Xia & Bing Joe Hwang & Yonggang Wang, 2025. "Li2ZrF6 protective layer enabled high-voltage LiCoO2 positive electrode in sulfide all-solid-state batteries," Nature Communications, Nature, vol. 16(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-024-55695-9
    DOI: 10.1038/s41467-024-55695-9
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