Improving the interfacial stability between layered oxide cathodes and sulfide electrolytes (SEs) and the structural stability of the cathode active material is critical for developing high-performance all-solid-state lithium batteries (ASSLBs). Coating and bulk doping are considered effective approaches; however, creating innovative buffer coatings and bulk doping using economical and scalable fabrication processes to address these issues is a comprehensive and challenging task. This article firstly proposes a coupling design of new Li₇TaO₆ (L7TaO) surface buffer coating with bulk Ta-doping for LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) by a simple one-step in situ synthesis method to tackle the interfacial issues of ASSLBs using Li₆PS₅Cl (LPSCl) electrolyte. The L7TaO buffer coating can not only promote interfacial Li-ion transport, but also effectively suppresses interfacial side reactions and reduces interfacial impedance. Simultaneously, Ta-doping into NCM811 reduces lithium–nickel mixing, thus boosting its structural stability. Therefore, the designed ASSLBs employing the NCM811 cathode coupled L7TaO-1 wt% buffer coating with bulk Ta-doping exhibit a high initial discharge capacity of 203.02 mA h g⁻¹ with initial coulombic efficiency of 85.42% at 0.1C and remarkable cycling stability up to 5650 cycles with decay rate per cycle of 0.0069% at 1C.

中文翻译：

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将新型 Li7TaO6 表面缓冲与块状 Ta 掺杂耦合以实现长寿命硫化物基全固态锂电池

提高层状氧化物正极和硫化物电解质（SEs）之间的界面稳定性以及正极活性材料的结构稳定性对于开发高性能全固态锂电池（ASSLBs）至关重要。涂层和体掺杂被认为是有效的方法；然而，使用经济且可扩展的制造工艺来创建创新的缓冲涂层和批量掺杂来解决这些问题是一项全面且具有挑战性的任务。本文首次提出了一种通过简单的一步原位耦合设计新型Li ₇ TaO ₆ (L7TaO) 表面缓冲涂层与块体Ta 掺杂的LiNi _0.8 Co _0.1 Mn _0.1 O _{2 (NCM811)。一种使用 Li 6} PS ₅ Cl (LPSCl) 电解质解决 ASSLBs 界面问题的合成方法。L7TaO缓冲涂层不仅可以促进界面锂离子传输，还可以有效抑制界面副反应，降低界面阻抗。同时，在 NCM811 中掺杂 Ta 可减少锂镍混合，从而提高其结构稳定性。因此，设计的 ASSLBs 采用 NCM811 阴极耦合 L7TaO-1 wt% 缓冲涂层和块状 Ta 掺杂，表现出 203.02 mA hg ^-1的高初始放电容量， 0.1C 时的初始库仑效率为 85.42%，循环稳定性高达5650 次循环，在 1C 时每个循环的衰减率为 0.0069%。