With numerous reports on protecting films for stable lithium (Li) metal electrodes, the key attributes for how to construct these efficient layers have rarely been fully investigated. Here, we report a rationally designed hybrid protective layer (HPL) with each component aligning with one key attribute; i.e., cross-linked poly(dimethylsiloxane) (PDMS) enhances flexibility, polyethylene glycol (PEG) provides homogeneous ion-conducting channels, and glass fiber (GF) affords mechanical robustness. A significant improvement of the electrochemical performance of HPL-modified electrodes can be achieved in Li/HPL@Cu half cells, HPL@Li/HPL@Li symmetric cells, and HPL@Li/LiFePO₄ full cells. Even with an industrial standard LiFePO₄ cathode (96.8 wt % active material), the assembled cell still exhibits a capacity retention of 90% after 100 cycles at 1 C. More importantly, the functionality of each component has been studied comprehensively via electrochemical and physical experiments and simulations, which will provide useful guidance on how to construct efficient protective layers for next-generation energy storage devices.

随着大量关于稳定锂 (Li) 金属电极保护膜的报道，很少有人充分研究如何构建这些有效层的关键属性。在这里，我们报告了一种合理设计的混合保护层 (HPL)，每个组件都与一个关键属性对齐；即，交联的聚二甲基硅氧烷 (PDMS) 增强了柔韧性，聚乙二醇 (PEG) 提供了均匀的离子传导通道，而玻璃纤维 (GF) 提供了机械强度。HPL 修饰电极的电化学性能可以在 Li/HPL@Cu 半电池、HPL@Li/HPL@Li 对称电池和 HPL@Li/LiFePO ₄全电池中实现。即使采用工业标准 LiFePO ₄ 正极（96.8 wt % 活性材料），组装电池在 1 C 下循环 100 次后仍表现出 90% 的容量保持率。更重要的是，通过电化学和物理实验和模拟对每个组件的功能进行了全面研究，这将提供关于如何为下一代储能设备构建高效保护层的有用指南。