Solid polymer electrolytes (SPEs) are considered to be the key to solve the safety hazards and cycling performance of liquid high‐voltage lithium metal batteries (HVLMBs), but still suffer from low conductivity and poor interfacial compatibility. Here, polyvinylidene fluoride–polyvinyl acetate‐based (PVDF–PVAC) rigid–flexible coupling SPE selectively wetted by a tetramethylene sulfone (TMS) is prepared for high‐performance and superior‐safety HVLMBs. The intermolecular interactions in such SPE significantly facilitate lithium‐ion conductivity and electrolyte/electrode interface wettability. Moreover, PVAC selectively wetted with the TMS enhances interface compatibility with Li anodes and high‐voltage LiCoO₂ cathodes. As a result, the as‐assembled LiCoO₂/lithium‐metal solid‐state batteries present excellent cyclability with 85% capacity retention after 200 cycles between 3.0 and 4.5 V at room temperature. Furthermore, pouch cells with the as‐prepared SPE exhibit brilliant safety and superior interfacial compatibility. This study offers a promising and general selectively wetted design strategy to handle the compatibility and safety issues in HVLMBs.

中文翻译：

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选择性润湿的刚柔耦合聚合物电解质，可实现高压锂金属电池的卓越稳定性和兼容性

固态聚合物电解质（SPE）被认为是解决液体高压锂金属电池（HVLMBs）的安全隐患和循环性能的关键，但仍然存在导电率低和界面相容性差的问题。在这里，聚四氟乙烯-聚乙酸乙烯酯基（PVDF-PVAC）刚性-挠性偶合SPE被四亚甲基砜（TMS）选择性润湿，为高性能和高安全性的HVLMB做好了准备。这种SPE中的分子间相互作用显着促进了锂离子传导性和电解质/电极界面的润湿性。此外，用TMS选择性润湿的PVAC增强了与Li阳极和高压LiCoO ₂阴极的界面兼容性。结果，组装后的LiCoO ₂/锂金属固态电池具有出色的可循环性，在室温下在3.0至4.5 V之间进行200次循环后，容量保持率为85％。此外，具有制备好的SPE的袋式电池具有出色的安全性和出色的界面相容性。这项研究提供了一种有前途的通用选择性浸润设计策略，以处理HVLMB中的兼容性和安全性问题。