Chloride solid electrolytes (CSEs) have good compatibility with commercial oxide cathode materials and show great potential for application in all-solid-state Li metal batteries (ASSLMBs). However, achieving simultaneously low cost, high ionic conductivity, excellent moisture tolerance, and robust electrochemical stability with >4 V-class cathodes for CSEs remains challenging. Herein, we report a facile Zr substitution strategy to increase the degree of preferred orientation and lower the Li diffusion barrier of the (001) plane, i.e. the ab plane, of LiScCl, thus boosting the ion conduction kinetics and framework stability. As such, LiScZrCl exhibits a high conductivity of 2.23 mS cm and low activation energy of 0.26 eV at room temperature (RT). ASSLMBs are constructed using a LiNiCoMnOcathode, LiScZrCl electrolyte, and Li-In anode, and deliver an exceptional initial Coulombic efficiency of 89.6 % at RT and can run stably over 200 cycles with 90 % capacity retention at 0.2C. In-situ electrochemical impedance inspection of the battery further reveals a high interfacial stability between LiScZrCl and LiNiCoMnO. Moreover, LiScZrCl demonstrates high wet fatness with a preserved structure stability and high ionic conductivity after exposure to atmosphere with 5 % relative humidity. Such humidity tolerance and cost-effectiveness solve two major obstacles for the application of CSEs.

中文翻译：

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用于锂电池的优选取向的高压超离子和耐湿Li2.5Sc0.5Zr0.5Cl6导体


氯化物固体电解质（CSE）与商业氧化物正极材料具有良好的兼容性，在全固态锂金属电池（ASSLMB）中显示出巨大的应用潜力。然而，使用用于 CSE 的 >4 V 级阴极同时实现低成本、高离子电导率、出色的耐湿性和强大的电化学稳定性仍然具有挑战性。在此，我们报告了一种简单的Zr取代策略，以增加择优取向程度并降低LiScCl的（001）面（即ab面）的Li扩散势垒，从而提高离子传导动力学和框架稳定性。因此，LiScZrCl 在室温 (RT) 下表现出 2.23 mS cm 的高电导率和 0.26 eV 的低活化能。 ASSLMB 使用 LiNiCoMnO 阴极、LiScZrCl 电解质和 Li-In 阳极构建，在室温下具有 89.6% 的出色初始库仑效率，并且可以在 0.2C 下稳定运行 200 多个循环，容量保持率为 90%。电池的原位电化学阻抗检查进一步揭示了 LiScZrCl 和 LiNiCoMnO 之间的高界面稳定性。此外，LiScZrCl在暴露于相对湿度为5%的大气后表现出高湿脂性，并保持结构稳定性和高离子电导率。这种耐湿性和成本效益解决了 CSE 应用的两大障碍。