Affiliation:
1. School of Chemical Engineering and Light Industry Guangdong University of Technology Guangzhou 510006 P. R. China
2. Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center Jieyang 515200 P. R. China
3. School of Environment and Civil Engineering Dongguan University of Technology Dongguan Guangdong 523808 P. R. China
Abstract
AbstractDifferent 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 Zn2+‐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 Zn2+ 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||LiFePO4 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.
Funder
National Natural Science Foundation of China
Basic and Applied Basic Research Foundation of Guangdong Province
Science and Technology Foundation of Shenzhen City