Aging Property of Halide Solid Electrolyte at the Cathode Interface,Advanced Materials

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Aging Property of Halide Solid Electrolyte at the Cathode Interface
Advanced Materials ( IF 27.4 ) Pub Date : 2023-04-30 , DOI: 10.1002/adma.202301631
Wonju Kim ₁ , Joohyeon Noh ₁ , Sunyoung Lee ₁ , Kyungho Yoon ₁ , Sangwook Han ₁ , Seungju Yu ₁ , Kun-Hee Ko ₁ , Kisuk Kang _{1,

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Affiliation

Halide solid electrolytes have recently emerged as a promising option for cathode-compatible catholytes in solid-state batteries (SSBs), owing to their superior oxidation stability at high voltage and their interfacial stability. However, their day- to month-scale aging at the cathode interface has remained unexplored until now, while its elucidation is indispensable for practical deployment. Herein, the stability of halide solid electrolytes (e.g., Li₃InCl₆) when used with conventional layered oxide cathodes during extended calendar aging is investigated. It is found that, contrary to their well-known oxidation stability, halide solid electrolytes can be vulnerable to reductive side reactions with oxide cathodes (e.g., LiNi_0.8Co_0.1Mn_0.1O₂) in the long term. More importantly, the calendar aging at a low state of charge or as-fabricated state causes more significant degradation than at a high state of charge, in contrast to typical lithium-ion batteries, which are more susceptible to high-state-of-charge calendar aging. This unique characteristic of halide-based SSBs is related to the reduction propensity of metal ions in halide solid electrolytes and correlated to the formation of an interphase due to the reductive decomposition triggered by the oxide cathode in a lithiated state. This understanding of the long-term aging properties provides new guidelines for the development of cathode-compatible halide solid electrolytes.

中文翻译：

卤化物固体电解质阴极界面的老化性能

卤化物固体电解质最近已成为固态电池（SSB）中阴极兼容阴极电解液的有前途的选择，因为它们在高电压下具有优异的氧化稳定性和界面稳定性。然而，迄今为止，它们在阴极界面的日至月规模老化仍未得到探索，而其阐明对于实际部署是必不可少的。在此，研究了卤化物固体电解质（例如Li ₃ InCl ₆ ）与常规层状氧化物阴极一起使用时在延长的日历老化过程中的稳定性。研究发现，与众所周知的氧化稳定性相反，卤化物固体电解质长期容易与氧化物阴极（例如LiNi _0.8 Co _0.1 Mn _0.1 O _{2 ）发生还原副反应。}更重要的是，与更容易受到高充电状态影响的典型锂离子电池相比，在低充电状态或制造状态下的日历老化会比在高充电状态下导致更显着的退化。日历老化。卤化物基SSB的这种独特特性与卤化物固体电解质中金属离子的还原倾向有关，并且与由于锂化状态的氧化物阴极触发的还原分解而形成中间相有关。这种对长期老化性能的理解为阴极兼容卤化物固体电解质的开发提供了新的指导方针。

更新日期：2023-04-30

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