Zhang Sida, Chen Jiashu, Chen Weigen, Su Yiwen, Gou Qianzhi, Yuan Ruduan, Wang Ziyi, Wang Kaixin, Zhang Wentao, Hu Xiqian, Zhang Zhixian, Wang Pinyi, Wan Fu, Liu Jie, Li Beibei, Wang Yifei, Zheng Guangping, Li Meng, Sun Jingyu
State Key Laboratory of Power Transmission Equipment Technology, School of Electrical Engineering, National Innovation Center for Industry-Education Integration of Energy Storage, Chongqing University, Chongqing, 400044, China.
Department of Mechanical Engineering, Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong 999077, China.
Angew Chem Int Ed Engl. 2025 Apr 1;64(14):e202424184. doi: 10.1002/anie.202424184. Epub 2025 Jan 28.
The Zn metal anode in aqueous zinc-ion batteries (AZIBs) faces daunting challenges including undesired water-induced parasitic reactions and sluggish ion migration kinetics. Herein, we develop three-dimensional covalent organic framework (COF) membranes with bioinspired ion channels toward stabilized Zn anodes. These COFs, featured by zincophilic pyridine-N sites, enable effective regulation of water molecules at the anode-electrolyte interphase. Systematic experimental analysis and theoretical simulations reveal the optimized COF-320N membrane functions as ion pumps, accordingly facilitating Zn transport and inhibiting direct contact between Zn anode and free water molecules. Consequently, the bio-inspired strategy achieves improved Zn transference number (0.61), rapid de-solvation kinetics, and suppressed hydrogen evolution. The assembled Zn||MnO pouch cell integrated with COF-320N membrane exhibits favorable electrochemical performances. Such a bioinspired concept for optimizing Zn anodes opens new pathways in developing advanced energy storage devices.
水系锌离子电池（AZIBs）中的锌金属负极面临着诸多严峻挑战，包括不希望发生的水诱导寄生反应和缓慢的离子迁移动力学。在此，我们开发了具有仿生离子通道的三维共价有机框架（COF）膜，用于稳定锌负极。这些以亲锌吡啶-N位点为特征的COFs能够有效调节阳极-电解质界面处的水分子。系统的实验分析和理论模拟表明，优化后的COF-320N膜起到离子泵的作用，从而促进锌的传输并抑制锌负极与游离水分子的直接接触。因此，这种仿生策略实现了更高的锌迁移数（0.61）、快速的去溶剂化动力学以及抑制析氢。集成了COF-320N膜的组装式Zn||MnO软包电池展现出良好的电化学性能。这种用于优化锌负极的仿生概念为开发先进储能装置开辟了新途径。
