The practical application of solid‐state polymer lithium‐metal batteries (LMBs) is plagued by the inferior ionic conductivity of the applied polymer electrolytes (PEs), which is caused by the coupling of ion transport with the motion of polymer segments. Here, solvated molecules based on ionic liquid and lithium salt with strong Li+‐solvent interaction are inserted into an elaborately engineered perfluoropolymer electrolyte via ionic dipole interaction, extensively facilitating Li+ transport and improving mechanical properties. The intensified formation of solvation structures of contact ion pairs and ionic aggregates, as well as the strong electron‐withdrawal properties of the F atoms in perfluoropolymers, give the PE high electrochemical stability and excellent interfacial stability. As a result, Li||Li symmetric cells demonstrate a lifetime of 2500 h and an exceptionally high critical current density above 2.3 mA cm‐2, Li||LiFePO4 batteries exhibit consistent cycling for 550 cycles at 10 C, and Li||uncoated LiNi0.8Co0.1Mn0.1O2 cells achieve 1000 cycles at 0.5 C with an average Coulombic efficiency of 98.45%, one of the best results reported to date based on PEs. Our discovery sheds fresh light on the targeted synergistic regulation of the electro‐chemo‐mechanical properties of PEs to extend the cycle life of LMBs.

中文翻译：

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用于固态锂金属电池的具有强锂+溶剂相互作用的有机阳离子配位全氟聚合物电解质


固态聚合物锂金属电池（LMB）的实际应用受到聚合物电解质（PE）离子电导率较差的困扰，这是由离子传输与聚合物链段运动的耦合引起的。在这里，基于具有强Li+-溶剂相互作用的离子液体和锂盐的溶剂化分子通过离子偶极相互作用插入精心设计的全氟聚合物电解质中，广泛促进Li+传输并改善机械性能。接触离子对和离子聚集体的溶剂化结构的强化形成，以及全氟聚合物中F原子的强吸电子特性，赋予PE较高的电化学稳定性和优异的界面稳定性。因此，Li||Li 对称电池表现出 2500 小时的寿命和高于 2.3 mA cm-2 的极高临界电流密度，Li||LiFePO4 电池在 10 C 下表现出 550 个循环的一致循环，并且 Li|| 无涂层LiNi0.8Co0.1Mn0.1O2电池在0.5 C下实现1000次循环，平均库仑效率为98.45%，这是迄今为止基于PE报告的最佳结果之一。我们的发现为有针对性地协同调节 PE 的电化学机械性能以延长 LMB 的循环寿命提供了新的思路。