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<p>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 Li<sub>2</sub>ZrF<sub>6</sub> coating layer on LiCoO<sub>2</sub>, 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 LiCoO<sub>2</sub>. As a result, the In-Li|Li<sub>6</sub>PS<sub>5</sub>Cl | Li<sub>2</sub>ZrF<sub>6</sub>-LiCoO<sub>2</sub> all-solid-state cell demonstrates an initial areal capacity of 5.2 mAh cm<sup>−2</sup> and a capacity retention of 80.5% after 1500 cycles at 70 mA/g with high LiCoO<sub>2</sub> areal mass loading (30.19 mg cm<sup>−2</sup>) and a cut-off voltage of 3.9 V (corresponding to potential of 4.5 V versus Li<sup>+</sup>/Li), at 25 °C.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年1月2日

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  • Xing Zhou,
  • Chia-Yu Chang,
  • Dongfang Yu,
  • Kai Zhang,
  • Zhi Li,
  • Shi-Kai Jiang,
  • Yizhou Zhu,
  • Yongyao Xia,
  • Bing Joe Hwang,
  • Yonggang Wang

摘要

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.