As an essential part of the performance improvement of lithium metal batteries, the acquisition of dense (LiF-rich solid electrolyte interphase (SEI)) has always been an urgent problem to be solved. Herein, we synthesized Zeolitic Imidazolate Frameworks (ZIFs) modified by two different functional groups (–NH₂, –CH₃) and used them as the fillers of polyethylene oxide (PEO) composite solid electrolytes to explore the catalytic effect of groups on LiF generation at the Li/electrolytes interface. In a LiFePO₄||SPE||Li cell test, the PEO-ZIF-NH₂ with LiF-rich SEI exhibits enhanced cycling performance, which was 3.8 times longer than that of PEO-ZIF-CH₃. The formation mechanism of LiF-rich SEI was investigated using first-principles calculation, revealing that ZIFs-NH₂ makes the C–F bond in TFSI^– longer compared with ZIFs-CH₃, which leads to easier breakage of the C–F bond and promoted the formation of LiF. The simple design idea of using organic catalysis to generate more stable SEI provides a new aspect for preparing high-performance lithium metal batteries.

作为锂金属电池性能提升的重要组成部分，致密（富含LiF的固体电解质界面（SEI））的获取一直是亟待解决的问题。_{在此，我们合成了由两种不同官能团（-NH 2}、-CH ₃）修饰的沸石咪唑骨架（ZIFs） ，并将其用作聚环氧乙烷（PEO）复合固体电解质的填料，以探索基团对LiF生成的催化作用。在锂/电解质界面。在 LiFePO ₄ ||SPE||Li 电池测试中，富含 LiF 的 SEI 的 PEO-ZIF-NH ₂表现出增强的循环性能，比 PEO-ZIF-CH _{3长 3.8 倍}. 使用第一性原理计算研究了富含 LiF 的 SEI 的形成机制，表明 ZIFs-NH ₂使 TFSI 中的 C-F 键^-与 ZIFs-CH ₃相比更长，这导致 C-F 键更容易断裂并促进了LiF的形成。利用有机催化产生更稳定的SEI的简单设计思想为制备高性能锂金属电池提供了新的思路。