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<p>Oxide solid-state electrolytes (OSSEs) are widely regarded as key enabling materials for next-generation all-solid-state lithium batteries (ASSLBs) with high specific energy, owing to their excellent thermal stability, wide electrochemical window, and intrinsic safety. Nevertheless, the intrinsically rigid ceramic nature of OSSEs leads to critical challenges—high interfacial impedance, chemical/electrochemical instability, and mechanical contact degradation—which severely hinder practical performance. This review systematically summarizes the structural evolution and ion-transport mechanisms of OSSEs, with an emphasis on unraveling failure mechanisms at both cathode and anode interfaces. On the cathode side, interfacial Li⁺-transport limitations arising from space-charge-layer effects, lattice-mismatch-induced stress, and oxidative interfacial decomposition are critically discussed. On the anode side, the coupled effects of poor mechanical wettability, interfacial side-reaction-induced electronic leakage, and lithium dendrite penetration are elucidated. To address these issues, state-of-the-art multiscale engineering strategies are highlighted, including surface physical/chemical modifications, the design of multifunctional artificial interfacial layers, advanced composite electrolyte architectures, and emerging data-driven materials discovery and screening approaches. Finally, perspectives are provided on future directions spanning fundamental interfacial science and key enabling technologies toward practical ASSLB deployment, aiming to offer theoretical insights and viable pathways to overcome solid–solid interfacial bottlenecks.</p>

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Interfacial problems and optimization strategies at the oxide solid-state electrolyte-electrode interface

  • 期刊论文

  • 发表日期：

    2026年5月11日

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  • Liubin Song,
  • Xinyang Qin,
  • Daoxin Wu,
  • Xingli Xiao,
  • Zhongliang Xiao,
  • Yinjie Kuang,
  • Tingting Zhao,
  • Xue Wen

摘要

Oxide solid-state electrolytes (OSSEs) are widely regarded as key enabling materials for next-generation all-solid-state lithium batteries (ASSLBs) with high specific energy, owing to their excellent thermal stability, wide electrochemical window, and intrinsic safety. Nevertheless, the intrinsically rigid ceramic nature of OSSEs leads to critical challenges—high interfacial impedance, chemical/electrochemical instability, and mechanical contact degradation—which severely hinder practical performance. This review systematically summarizes the structural evolution and ion-transport mechanisms of OSSEs, with an emphasis on unraveling failure mechanisms at both cathode and anode interfaces. On the cathode side, interfacial Li⁺-transport limitations arising from space-charge-layer effects, lattice-mismatch-induced stress, and oxidative interfacial decomposition are critically discussed. On the anode side, the coupled effects of poor mechanical wettability, interfacial side-reaction-induced electronic leakage, and lithium dendrite penetration are elucidated. To address these issues, state-of-the-art multiscale engineering strategies are highlighted, including surface physical/chemical modifications, the design of multifunctional artificial interfacial layers, advanced composite electrolyte architectures, and emerging data-driven materials discovery and screening approaches. Finally, perspectives are provided on future directions spanning fundamental interfacial science and key enabling technologies toward practical ASSLB deployment, aiming to offer theoretical insights and viable pathways to overcome solid–solid interfacial bottlenecks.