Solvation Barrier Remodeling‐Dictated Fast‐Kinetics Top–Down Zn Stripping/Plating in Water‐Lean Organic Electrolytes
Zhenfeng Feng, Yongchao Tang, Yue Wei, Guigui Liu, Hongqing Li, Jianping Yan, Jintu Qi, Xiaoqing Liu, Zhipeng Wen, Minghui Ye, Yufei Zhang, Cheng Chao Li
Abstract
Abstract Different from “bottom–up” Zn plating/stripping, “top–down” Zn stripping/plating provides a new perspective to reinvent current aqueous Zn batteries (AZBs), yet related studies remain absent. Herein, a chelation‐induced solvation barrier remodeling strategy is initiated toward fast‐kinetics “top–down” Zn stripping/plating in original Zn 2+ ‐free water‐lean organic electrolytes (WLOE) for durable Zn batteries. It is found that in WLOE, the initial Zn stripping kinetics of the Zn anode remarkably limits the “top–down” Zn stripping/plating. The intervention of multidentate chelant (2‐methoxyethylamine, MEA) in WLOE greatly lowers the solvation reorganization energy of in situ stripped Zn 2+ from the Zn anode, enabling the fast‐kinetics “top–down” Zn stripping/plating. Spectral characterization and fitted overpotential‐reorganization energy correlation strongly confirm the underlying mechanism. As such, the Zn stripping/plating in the MEA‐mediated WLOE shows a 90‐fold‐enhanced current response, triple‐lowered overpotential, and 170‐fold‐prolonged cyclability (over 1700 h at 0.5 mA cm −2 ) of those in MEA‐free counterpart. The assembled Zn||LiFePO 4 hybrid full cell in MEA‐regulated WLOE exhibits a distinct and high voltage plateau of 1.50 V and a low polarization voltage of 0.14 V, far surpassing those in conventional WLOE. This work opens a new avenue to break the kinetics bottleneck of Zn stripping/plating in WLOE for durable Zn batteries.