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<p>All-solid-state lithium batteries (ASSBs) that integrate Ni-rich single crystal cathode (e.g. LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811)) with sulfide solid electrolyte (e.g. Li<sub>6</sub>PS<sub>5</sub>Cl, LPSCL) are emerging as primary contenders for the next generation rechargeable batteries due to their superior safety and energy density. Their development, however, is impeded by complex capacity fading mechanisms. Here, we systematically investigate the NCM811 cathode degradation in sulfide-based ASSBs by tracking performance at four key capacity retention levels (100%, 90%, 80%, and 70%). The failure evolves through distinct stages: initial interfacial degradation and active lithium loss increase the cell resistance, which is then correlated with the initiation of bulk cathode damage characterized by anisotropic lattice strain and oxygen release. The newly created surfaces from bulk damage are postulated to feedback and intensify interfacial decomposition, thereby suggesting a potential feedback loop that warrants further investigation. Our findings highlight that the capacity fading is a coupled process between interfacial chemistry and bulk degradation, emphasizing the critical need for co-stabilization strategies to develop durable ASSBs. </p>

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Degradation mechanism of Ni-rich cathode in all-solid-state batteries at different capacity retention

  • 期刊论文

  • 发表日期：

    2026年3月2日

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  • Yuan Tian,
  • Chunrong Zhao,
  • Jinling Zhao,
  • Chengyu Zhang,
  • Minjuan Yuan,
  • Qian Zhao,
  • Ling Tang,
  • Lve Wang,
  • Rong Yang

摘要

All-solid-state lithium batteries (ASSBs) that integrate Ni-rich single crystal cathode (e.g. LiNi0.8Co0.1Mn0.1O2 (NCM811)) with sulfide solid electrolyte (e.g. Li6PS5Cl, LPSCL) are emerging as primary contenders for the next generation rechargeable batteries due to their superior safety and energy density. Their development, however, is impeded by complex capacity fading mechanisms. Here, we systematically investigate the NCM811 cathode degradation in sulfide-based ASSBs by tracking performance at four key capacity retention levels (100%, 90%, 80%, and 70%). The failure evolves through distinct stages: initial interfacial degradation and active lithium loss increase the cell resistance, which is then correlated with the initiation of bulk cathode damage characterized by anisotropic lattice strain and oxygen release. The newly created surfaces from bulk damage are postulated to feedback and intensify interfacial decomposition, thereby suggesting a potential feedback loop that warrants further investigation. Our findings highlight that the capacity fading is a coupled process between interfacial chemistry and bulk degradation, emphasizing the critical need for co-stabilization strategies to develop durable ASSBs.