Hollow‐Particles Quasi‐Solid‐State Electrolytes with Biomimetic Ion Channels for High‐Performance Lithium‐Metal Batteries

Abstract Solid‐state electrolytes (SSEs) are the core material of solid‐state lithium metal batteries (SLMBs), which are being researched urgently owing to their high energy and safety. Both high ionic conductivity and excellent cycling stability remain the primary goal of solid‐state electrolytes. Herein, inspired by K+/Na+ ion channels in cell membrane of eukaryotes, a novel hollow UiO‐66 with biomimetic ion channels based on quasi‐solid‐state electrolytes (QSSEs) is designed. The hollow UiO‐66 spheres containing biomimetic ion channels can spontaneously combine anions and incorporate more lithium ions, creating improved ionic conductivity (1.15 × 10−3 S cm−1) and lithium‐ion transference number (0.70) at room temperature. The long‐term cycling of symmetric batteries and COMSOL simulations demonstrate that this biomimetic strategy enables uniform ion flux to suppress Li dendrites. Furthermore, the Li metal full cells paired with LiFePO4 cathode exhibit excellent cycling stability and rate performance. Consequently, the strategy of designing biomimetic QSSEs opens up a new path for developing high‐performance electrolytes for SLMBs.