High-energy rechargeable lithium metal batteries have attracted soaring attention because of high specific capacity and low electrochemical potential of lithium metal. Unfortunately, the lithium dendrite growth upon Li plating severely hinders its practical application. Herein, we report the preparation of ionic liquid (IL) immobilized polymer gel electrolytes with strong ion-dipole interactions between imidazolium-based IL and fluorinated copolymer gel for stable and dendrite-free Li⁺ plating/stripping. The adoption of IL leads to the formation of a tightly cross-linked gel framework with tethered anions, providing greatly-improved mechanical strength, good heat resistance, favorable self-healing capability, high ionic conductivity, and a stable electrochemical window up to 4.5 V vs. Li⁺/Li that can satisfy the demand of high-voltage cathodes. The membrane of IL-immobilized polymer gel electrolyte enabled dendrite-free Li deposition, showing stable cycling durability for 1000 h at 0.5 mA cm⁻², and the functional mechanism was carefully investigated. By coupling with this gel electrolyte membrane, the LiFePO₄/Li cell exhibit much superior cycling stability and rate performance. Moreover, the lithium-sulfur batteries assembled with the IL-immobilized polymer gel electrolyte also show efficient suppression of polysulfide shuttling and self-discharge, bringing high specific capacity and long cycling life.

高能量可充电锂金属电池由于锂金属的高比容量和低电化学势而引起了人们的极大关注。不幸的是，锂镀覆时锂枝晶的生长严重阻碍了其实际应用。在这里，我们报告离子液体（IL）固定的聚合物凝胶电解质的制备，该电解质在咪唑基IL和氟化共聚物凝胶之间具有很强的离子-偶极相互作用，用于稳定且无枝晶的Li ⁺电镀/剥离。IL的采用导致与束缚阴离子形成紧密交联的凝胶骨架，从而大大提高了机械强度，良好的耐热性，良好的自愈能力，高离子电导率以及高达4.5 V的稳定电化学窗口与李⁺/ Li，可以满足高压阴极的需求。固定有IL的聚合物凝胶电解质的膜可实现无枝晶的Li沉积，在0.5 mA cm ^{-2的条件下}显示1000个小时的稳定循环耐久性，并仔细研究了其作用机理。通过与该凝胶电解质膜偶联，LiFePO ₄ / Li电池表现出非常优异的循环稳定性和倍率性能。此外，与固定有IL的聚合物凝胶电解质组装的锂硫电池也显示出对多硫化物的穿梭和自放电的有效抑制，带来了高比容量和长循环寿命。