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<p>Li-rich Mn-based oxide (LRMO) cathodes represent promising candidates for high-energy-density all-solid-state lithium batteries (ASSLBs). Nonetheless, irreversible oxygen release and sluggish transport kinetics result in faded voltage and degraded cycling stability, severely impeding their practical applications in ASSLBs. Herein, a high-quality artificial interface layer was constructed on the LRMO surface via a facile sol–gel method followed by thermal treatment, yielding a Li<sub>3</sub>ScF<sub>6</sub> protective layer comprising a Li<sub>3</sub>ScF<sub>6</sub> surface coating region and a subsurface Sc doping region. Specifically, Li<sub>3</sub>ScF<sub>6</sub> surface coating effectively suppresses continuous interfacial side reactions between the cathode and solid electrolyte, thereby improving interfacial transport kinetics; the strong Sc–O bond stabilizes the lattice oxygen framework and inhibits oxygen release, thereby enhancing the reversibility of the oxygen redox reaction. Consequently, the ASSLBs with the modified LRMO cathode exhibit remarkable fast-charging capability (136.8 mAh g<sup>−1</sup> at 1.0 C) and excellent capacity retention (83.9% after 500 cycles at 0.3 C). In addition, the ASSLBs achieve outstanding long-term cycling stability at a high areal capacity of 4.17&#xa0;mAh&#xa0;cm<sup>−2</sup>, retaining 81.8% of its capacity after 300 cycles at 60&#xa0;°C. This study offers new insights into the rational design of high-capacity and high-voltage LRMO cathode materials for high-energy-density ASSLBs. <InlineMediaObject> <ImageObject Color="Color" FileRef="MediaObjects/40820_2026_2209_Figa_HTML.gif" Format="GIF" Height="382" Rendition="HTML" Resolution="120" Type="LinedrawHalftone" Width="968" /> </InlineMediaObject></p>

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Modulating Lattice Oxygen and Transport Kinetics of Li-Rich Cathodes in All-Solid-State Batteries Through Multifunctional Li3ScF6 Protective Layer

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月21日

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  • Peng Lei,
  • Gang Wu,
  • Xiang Qi,
  • Yang Li,
  • Meng Wu,
  • Wanqing Ren,
  • Huan Li,
  • Lei Gao,
  • Dan Zhou,
  • Li-Zhen Fan

摘要

Li-rich Mn-based oxide (LRMO) cathodes represent promising candidates for high-energy-density all-solid-state lithium batteries (ASSLBs). Nonetheless, irreversible oxygen release and sluggish transport kinetics result in faded voltage and degraded cycling stability, severely impeding their practical applications in ASSLBs. Herein, a high-quality artificial interface layer was constructed on the LRMO surface via a facile sol–gel method followed by thermal treatment, yielding a Li3ScF6 protective layer comprising a Li3ScF6 surface coating region and a subsurface Sc doping region. Specifically, Li3ScF6 surface coating effectively suppresses continuous interfacial side reactions between the cathode and solid electrolyte, thereby improving interfacial transport kinetics; the strong Sc–O bond stabilizes the lattice oxygen framework and inhibits oxygen release, thereby enhancing the reversibility of the oxygen redox reaction. Consequently, the ASSLBs with the modified LRMO cathode exhibit remarkable fast-charging capability (136.8 mAh g−1 at 1.0 C) and excellent capacity retention (83.9% after 500 cycles at 0.3 C). In addition, the ASSLBs achieve outstanding long-term cycling stability at a high areal capacity of 4.17 mAh cm−2, retaining 81.8% of its capacity after 300 cycles at 60 °C. This study offers new insights into the rational design of high-capacity and high-voltage LRMO cathode materials for high-energy-density ASSLBs.