The interphase formed between solid polymer electrolyte (SPE) and highly reductive lithium metal largely determines the overall performance of the battery. Although various types of nanoparticles have been continuously employed as fillers to achieve a stable interphase for long cycling performance, the irregular growth of lithium dendrites cannot be completely suppressed due to uneven lithium deposition. Herein, a new type of zwitter-ion modified metal-organic framework (NH₃⁺·SO₃^-@ZIFs) is prepared as a modifier for PEO-LiTFSI. Due to the unique ionic structure of NH₃⁺·SO₃^-@ZIFs, the formed electrostatic interaction could inhibit the movement of TFSI^-, enhance the ion migration number. More importantly, TOF-SIMS effectively confirms the formation of Li⁺-conductive LiF-rich SEI due to the catalytic effect of NH₃⁺·SO₃^-@ZIFs, which could homogenize the lithium flux, inhibit the growth of Li dendrite. Results show that the PEO-NH₃⁺·SO₃^-@ZIFs exhibits high ion migration number (t_Li+ = 0.78). The Li/Li symmetric cells equipped NH₃⁺·SO₃^-@ZIFs SPE can be stably operated for more than 4600 h at 60 °C while the full cell with LiFePO₄ cathode also enables long-term stability over 1200 cycles with capacity stabilizing at around 103 mAh g⁻¹, demonstrating the great potential of this kind of SPEs for preparing high-performance LMBs.

固体聚合物电解质（SPE）和高还原性锂金属之间形成的界面在很大程度上决定了电池的整体性能。尽管各种类型的纳米颗粒已被连续用作填料以获得稳定的界面以实现长循环性能，但由于锂沉积不均匀，锂枝晶的不规则生长无法完全抑制。在此，制备了一种新型两性离子改性金属有机骨架（NH ₃ ⁺ ·SO ₃ ^- @ZIFs）作为PEO-LiTFSI的改性剂。由于NH ₃ ⁺ ·SO ₃ ^- @ZIFs独特的离子结构，形成的静电相互作用可以抑制TFSI ^-的移动, 提高离子迁移数。更重要的是，TOF-SIMS 有效地证实了由于 NH ₃ ⁺ ·SO ₃ ^- @ZIFs的催化作用形成了 Li ⁺ - 导电的富含 LiF 的 SEI ，它可以使锂通量均匀化，抑制 Li 枝晶的生长。结果表明，PEO-NH ₃ ⁺ ·SO ₃ ^- @ZIFs表现出高离子迁移数(t _Li+ = 0.78)。_{配备 NH 3} ⁺ ·SO ₃ ^- @ZIFs SPE的 Li/Li 对称电池可在 60 °C 下稳定运行超过 4600 小时，而配备 LiFePO _{4的全电池}阴极还能够实现超过 1200 次循环的长期稳定性，容量稳定在 103 mAh g ^-1左右，证明了这种 SPEs 在制备高性能 LMBs 方面的巨大潜力。