Electrode Interface Engineering of Hydrophilic and Zincophilic Bifunctionality for High‐Efficiency and Low‐Polarization Zn Anodes

作者：Tan Wang, Chen Wang, Gabriel Vinicius De Oliveira Silva, Yuanlin Xu, Haoyun Wei, Guo‐Xing Miao, Jing Fu · 发表于：Advanced Functional Materials · 年份：2024 · DOI：10.1002/adfm.202408662 · 被引用次数：10 · 研究领域：Advanced battery technologies research、Supercapacitor Materials and Fabrication、Advanced Battery Materials and Technologies

Abstract Aqueous rechargeable Zn batteries offer a promising technological route as a safe and low‐cost energy storage system for grid energy storage. However, major challenges of Zn dendrites and parasitic side reactions upon cycling in aqueous environments remain unsolved. Here, a design of a bifunctional electrode interface consisting of heterostructured zinc hydroxide chloride (ZHC) and Cu, as well as their synergy in promoting high‐efficiency and low‐polarization Zn deposition is reported. Hydrophilic/zincophobic ZHC promotes the desolvation of hydrated Zn 2+ prior to Zn nucleation, meanwhile adjacent Cu acts as a zincophilic site for subsequent nucleation and deposition. Consequently, the reduction polarization of Zn 2+ at the bifunctional layer (ZHC‐Cu) features ten times lower nucleation overpotential of 3 mV than bare Zn. Meanwhile, the water‐induced hydrogen evolution side reactions on Zn are significantly hindered by the bifunctionality of the electrode interface. Accordingly, the ZHC‐Cu@Zn symmetric cells exhibit a superior cycling stability for over 3500 cycles at 10 mA cm −2 /3 mAh cm −2 . The ZHC‐Cu@Zn full‐cell with MnO 2 cathode can stably operate for low C‐rate cycling with a high average Coulombic efficiency of 99.5% over 600 cycles. This work provides an effective approach to rational design of heterostructured bifunctional electrode interfaces to obtain high‐efficiency and low‐polarization Zn anodes.