Defect engineering of metal-organic framework-based electrolytes to expose abundant active sites is an effective strategy to optimize the electrochemical performance of lithium metal batteries. Herein, a three-dimensional (3D) cluster-based framework (Ni-MOF (II), (H2N (CH3) 22Ni3 (μ3-O) (XN) (BPDC) 3·12DMFn) ) has been harvested, and a ligand defect strategy was further employed to form three defective Ni-MOF (II) -X (X = 30, 50, 70) materials. The generation of open metal sites may provide favorable conditions for the dissociation of lithium salt and the immobilization of anions, thereby enabling efficient single-ion conduction. In electrochemical performance investigations, Ni-MOF (II) -50 presents outstanding ionic conductivity, high Li+ transference number and broad electrochemical stability window over a wide temperature range (1. 25 × 10-3 S cm-1, 0. 83, 5. 1 V at 25 °C; 1. 08 × 10-4 S cm-1, 0. 74, 5. 0 V at -30 °C). Moreover, the Li|Ni-MOF (II) -50|Li symmetric cell demonstrated stable cycling over 800 h at 0. 5 mA cm-2. This work provides a rational defect-engineering pathway for designing high-performance MOF-based quasi-solid-state electrolytes with a wide operational temperature range.
Gu et al. (2026) studied this question.