2D Conductive Cu‐MOF as a Multifunctional Regulator of Both Cathode and Anode to Synergistically Enhance the Performance of High‐Loading Aqueous Zinc‐Iodine Batteries

ABSTRACT Aqueous zinc‐iodine batteries (AZIBs) have gained widespread attention in large‐scale energy storage and other fields owing to their high safety, low cost, and environmental friendliness. However, AZIBs still face challenges such as iodine shuttling effect and zinc dendrite growth. Herein, a 2D conductive copper metal–organic framework (Cu‐MOF) with the unique Cu─O 4 coordination motif is used as a multifunctional regulator of both cathode and anode to synergistically enhance the comprehensive performances of high‐loading AZIBs. For the iodine cathode regulator, the full cell of AZIBs with 2D Cu‐MOF exhibits the improved capacity and rate performance. For the zinc anode regulator, the Zn//Zn symmetric cell and Zn//Cu half‐cell with 2D Cu‐MOF show the enhanced cycle stability and excellent coulombic efficiency, respectively. With the 2D Cu‐MOF as a multifunctional regulator for both cathode and anode, the resulting high‐loading AZIBs exhibit superior electrochemical performances and the assembled 3 × 3 cm 2 pouch cell also demonstrates long‐term cycling stability. The experimental and theoretical analyses reveal that the Cu─O 4 coordination center in 2D Cu‐MOF can provide strong anchoring effect toward iodine species and facilitate the uniform zinc deposition/stripping. This work provides a new approach to improve the comprehensive performance of AZIBs by utilizing 2D MOFs as multifunctional regulators.