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Vol. 16 (2024)

Critical Solvation Structures Arrested Active Molecules for Reversible Zn Electrochemistry

https://doi.org/10.1007/s40820-024-01361-0
Junjie Zhang
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Bao Zhang
School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore
Xin Chen
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Wenyu Hao
School of Optical and Electronic Information, Huazhong University of Science and Technology, Wuhan 430074, People’s Republic of China
Jia Yao
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Jingying Li
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Yi Gan
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Xiaofang Wang
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Xingtai Liu
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Ziang Wu
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Youwei Liu
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Lin Lv
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Li Tao
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Pei Liang
Institute of Optoelectronics Technology, China Jiliang University, Hangzhou 310018, People’s Republic of China
Xiao Ji
School of Optical and Electronic Information, Huazhong University of Science and Technology, Wuhan 430074, People’s Republic of China
Hao Wang
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China
Houzhao Wan
Hubei Yangtze Memory Laboratories, Wuhan 430205, People’s Republic of China

Corresponding Author: Houzhao Wan

houzhaow@hubu.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 145

Abstract

Aqueous Zn-ion batteries (AZIBs) have attracted increasing attention in next-generation energy storage systems due to their high safety and economic. Unfortunately, the side reactions, dendrites and hydrogen evolution effects at the zinc anode interface in aqueous electrolytes seriously hinder the application of aqueous zinc-ion batteries. Here, we report a critical solvation strategy to achieve reversible zinc electrochemistry by introducing a small polar molecule acetonitrile to form a “catcher” to arrest active molecules (bound water molecules). The stable solvation structure of [Zn(H2O)6]2+ is capable of maintaining and completely inhibiting free water molecules. When [Zn(H2O)6]2+ is partially desolvated in the Helmholtz outer layer, the separated active molecules will be arrested by the “catcher” formed by the strong hydrogen bond N–H bond, ensuring the stable desolvation of Zn2+. The Zn||Zn symmetric battery can stably cycle for 2250 h at 1 mAh cm−2, Zn||V6O13 full battery achieved a capacity retention rate of 99.2% after 10,000 cycles at 10 A g−1. This paper proposes a novel critical solvation strategy that paves the route for the construction of high-performance AZIBs.


Highlights:
1 Critical solvation structure changes the hydrogen bond network through “catchers”.
2 Catcher further arrests the active molecules to promote Zn2+ deposition.
3 The Zn||Zn symmetric battery can stably cycle for 2250 h. Zn||V6O13 full battery achieved a capacity retention rate of 99.2% after 10,000 cycles.

Keywords

Zinc-ion battery Critical solvation Helmholtz layer Arrest active molecule Reversible zinc anode
Zhang, Junjie, Bao Zhang, Xin Chen, Wenyu Hao, Jia Yao, Jingying Li, Yi Gan, Xiaofang Wang, Xingtai Liu, Ziang Wu, Youwei Liu, Lin Lv, Li Tao, Pei Liang, Xiao Ji, Hao Wang, and Houzhao Wan. 2024. “Critical Solvation Structures Arrested Active Molecules for Reversible Zn Electrochemistry”. Nano-Micro Letters 16 (March):145. https://doi.org/10.1007/s40820-024-01361-0.
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