Solvation Barrier Remodeling‐Dictated Fast‐Kinetics Top–Down Zn Stripping/Plating in Water‐Lean Organic Electrolytes

Author:

Feng Zhenfeng1,Tang Yongchao12,Wei Yue3,Liu Guigui1,Li Hongqing1,Yan Jianping1,Qi Jintu1,Liu Xiaoqing12,Wen Zhipeng12,Ye Minghui12,Zhang Yufei12,Li Cheng Chao12ORCID

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

Publisher

Wiley

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