An ultra-thin quasi-solid electrolyte (QSE) with dendrite-inhibiting properties is a requirement for achieving high energy density quasi-solid lithium metal batteries (LMBs). Here, a 5.1 µm rigid QSE layer is directly designed on the cathode, in which Kevlar (poly(p-phenylene terephthalate)) nanofibers (KANFs) with negatively charged groups bridging metal-organic framework (MOF) particles are served as a rigid skeleton, and non-flammable deep eutectic solvent is selected to be encapsulated into the MOF channels, combined with in situ polymerization to complete safe electrolyte system with high rigidness and stability. The QSE with constructed topological network demonstrates high rigidity (5.4 GPa), high ionic conductivity (0.73 mS cm⁻¹ at room temperature), good ion-regulated properties, and improved structural stability, contributing to homogenized Li-ion flux, excellent dendrite suppression, and prolonged cyclic performance for LMB. Additionally, ion regulation influences the Li deposition behavior, exhibiting a uniform morphology on the Li-metal surface after cycling. According to density-functional theory, KANFs bridging MOFs as hosts play a vital function in the free-state and fast diffusion dynamics of Li-ions. This work provides an effective strategy for constructing ultrathin robust electrolytes with a novel ionic conduction mode.

中文翻译：

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通过桥接锂金属电池快速锂离子传输通道构建的 5.1 µm 离子调节刚性准固态电解质

具有抑制枝晶特性的超薄准固体电解质（QSE）是实现高能量密度准固体锂金属电池（LMB）的必要条件。这里，直接在阴极上设计了 5.1 µm 的刚性 QSE 层，其中带有桥接金属有机框架 (MOF) 颗粒的带负电基团的 Kevlar（聚对苯二甲酸乙二醇酯）纳米纤维 (KANF) 作为刚性骨架，并选择不易燃的低共熔溶剂封装到MOF通道中，结合原位聚合，完成具有高刚性和稳定性的安全电解质体系。具有拓扑网络的QSE表现出高刚性（5.4 GPa）、高离子电导率（室温下0.73 mS cm ^-1）、良好的离子调节特性和改善的结构稳定性，有助于均匀的锂离子通量、优异的枝晶抑制，并延长 LMB 的循环性能。此外，离子调节影响锂沉积行为，循环后锂金属表面表现出均匀的形态。根据密度泛函理论，以 MOF 为主体桥接的 KANF 在锂离子的自由态和快速扩散动力学中发挥着至关重要的作用。这项工作为构建具有新型离子传导模式的超薄坚固电解质提供了有效的策略。