The development of high-performance sulfide electrolyte-based all-solid-state lithium-ion batteries (ASSLIBs) has been inhibited by problematic ionic transport and side reactions at the cathode interface, and their success is dependent on the functionalized interface upon charging and discharging. Despite recent progresses, it has proven challenging to design a favorable interface that can suppress the side reactions and enable smooth motion of Li⁺ ions. Herein, a favorable Zr-based cathode interface is elaborately manipulated by the atomic layer deposition (ALD) for sulfide-based ASSLIBs. Flexile control over the Li sub-cycle during the preparation process is demonstrated to be crucial for achieving a robust cathode interface with a desirable Li⁺ ionic conductivity. The ASSLIBs equipped with this functional interface exhibit excellent cycling stability and rate capability at room temperature (RT). Various electrochemical and spectroscopic characterizations reveal that the ionic conductive interface can significantly limit side reactions and induce a low polarization of the (de)intercalation toward cathode materials. The interfacial manipulation regarding ionic conductivity and structure realized by ALD provides a new strategy to achieve high-performance ASSLIBs.

高性能硫化物电解质基全固态锂离子电池（ASSLIB）的开发受到阴极界面处离子传输和副反应问题的困扰，其成功取决于充电和放电时功能化的界面。尽管有最新进展，但事实证明，设计出一种有利的界面以抑制副反应并实现Li ⁺离子的平滑运动具有挑战性。在本文中，通过基于原子的硫化物的ASSLIBs的原子层沉积（ALD）精心操纵了良好的Zr基阴极界面。已证明在制备过程中灵活控制Li子循环对于实现具有理想Li ⁺的坚固阴极界面至关重要离子电导率。配备此功能接口的ASSLIB在室温（RT）下具有出色的循环稳定性和速率能力。各种电化学和光谱学表征表明，离子导电界面可以显着限制副反应，并引起向阴极材料的（脱）插层的低极化。ALD实现的有关离子电导率和结构的界面处理为实现高性能ASSLIB提供了新的策略。