He Pan, Li Boxin, Wang Bingwu, Xie Dong, Wang Ke, Ai Wei
Frontiers Science Center for Flexible Electronics, Xi'an Institute of Flexible Electronics, Northwestern Polytechnical University, 127 West Youyi Road, Xi'an 710072, China.
ACS Appl Mater Interfaces. 2025 Jan 8;17(1):2556-2565. doi: 10.1021/acsami.4c17415. Epub 2024 Dec 25.
The irreversible chemistry of the Zn anode, attributed to parasitic reactions and the growth of zinc dendrites, is the bottleneck in the commercialization of aqueous zinc-ion batteries. Herein, an efficient strategy via constructing an organic protective layer configured with a honeycomb-like globular-covalent organic framework (G-COF) was constructed to enhance the interfacial stability of Zn anodes. Theoretical analyses disclose that the methoxy and imine groups in G-COF have more negative adsorption energy and electrostatic potential distribution, favorable Zn adsorption, and diffusion. Experimental results demonstrate that G-COF effectively protects the Zn anode from dendrite formation and surface corrosion, leading to a stable and homogeneous Zn deposition. Notably, the G-COF@Zn||G-COF@Zn symmetric cell obtained high stability for over 1650 h under 3 mA cm for 1 mA h cm. Full cells assembled with the δ-MnO cathode and G-COF@Zn anode demonstrates exceptional rate capability and consistent cycling over 1000 cycles at a current density of 1 A g, achieving a specific capacity of 217 mA h g. Our work provides novel insight into interfacial regulation of Zn anodes for the implementation of practical aqueous zinc-ion batteries with long-term cycling characteristics.
锌负极的不可逆化学反应，归因于寄生反应和锌枝晶的生长，是水系锌离子电池商业化的瓶颈。在此，通过构建一种由蜂窝状球状共价有机框架（G-COF）构成的有机保护层的有效策略，来增强锌负极的界面稳定性。理论分析表明，G-COF中的甲氧基和亚胺基团具有更负的吸附能和静电势分布，有利于锌的吸附和扩散。实验结果表明，G-COF有效地保护锌负极不形成枝晶和表面腐蚀，从而实现稳定且均匀的锌沉积。值得注意的是，G-COF@Zn||G-COF@Zn对称电池在3 mA cm下1 mA h cm的条件下保持了超过1650 h的高稳定性。用δ-MnO阴极和G-COF@Zn阳极组装的全电池在1 A g的电流密度下表现出优异的倍率性能和超过1000次循环的一致性循环，实现了217 mA h g的比容量。我们的工作为锌负极的界面调控提供了新的见解，以实现具有长期循环特性的实用水系锌离子电池。
