As a very prospective solid‐state electrolyte, Li10GeP2S12 (LGPS) exhibits high ionic conductivity comparable to liquid electrolytes. However, severe self‐decomposition and Li dendrite propagation of LGPS will be triggered due to the thermodynamic incompatibility with Li metal anode. Herein, by adopting a facile chemical vapor deposition method, an artificial solid electrolyte interphase composed of Li2S is proposed as a single ionic conductor to promote the interface stability of LGPS toward Li. The good electronic insulation coupled with ionic conduction property of Li2S effectively blocks electron transfer from Li to LGPS while enabling smooth passage of Li ions. Meanwhile, the generated Li2S layer remains good interface compatibility with LGPS, which is verified by the stable Li‐plating/stripping operation for over 500 h at 0.15 mA cm−2. Consequently, the all‐solid‐state Li–S batteries (ASSLSBs) with a Li2S layer demonstrate superb capacity retention of 90.8% at 0.2 mA cm−2 after 100 cycles. Even at the harsh condition of 90 °C, the cell can deliver a high reversible capacity of 1318.8 mAh g−1 with decent capacity retention of 88.6% after 100 cycles. This approach offers a new insight for interface modification between LGPS and Li and the realization of ASSLSBs with stable cycle life.

中文翻译：

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将硫化锂集成为单离子导体界面以实现稳定的全固态锂硫电池

Li作为一种非常有前景的固态电解质10GeP2S12(LGPS) 表现出与液体电解质相当的高离子电导率。然而，由于与锂金属阳极的热力学不相容，LGPS会发生严重的自分解和锂枝晶生长。在此，通过采用简便的化学气相沉积方法，制备了由Li组成的人造固体电解质界面。2S被提议作为单一离子导体以促进LGPS对Li的界面稳定性。 Li良好的电子绝缘性和离子导电性2S有效地阻止电子从Li到LGPS的转移，同时使Li离子顺利通过。同时，生成的Li2S层与LGPS保持良好的接口兼容性，这通过在0.15 mA cm下稳定的镀/脱锂操作超过500小时得到验证−2。因此，具有Li的全固态Li-S电池（ASSLSB）2S 层在 0.2 mA cm 电流下表现出 90.8% 的卓越容量保持率−2100个循环后。即使在90℃的恶劣条件下，电池也能提供1318.8mAh g的高可逆容量−1100次循环后容量保持率高达88.6%。这种方法为LGPS和Li之间的界面修饰以及实现具有稳定循环寿命的ASSLSB提供了新的见解。