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

Xing Zhou, Chia-Yu Chang, Dongfang Yu, Kai Zhang, Zhi Li, Shi-Kai Jiang, Yizhou Zhu (), Yongyao Xia (), Bing Joe Hwang () and Yonggang Wang ()
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Xing Zhou: Fudan University
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)
Yonggang Wang: Fudan University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: 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.

Date: 2025
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DOI: 10.1038/s41467-024-55695-9

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