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Vol. 17 (2025)

Regulating the Coordination Environment of H2O in Hydrogel Electrolyte for a High-Environment-Adaptable and High-Stability Flexible Zn Devices

https://doi.org/10.1007/s40820-025-01810-4
Jianghe Liu
Advanced Energy Storage Materials and Technology Research Center, Guangdong‑Hong Kong Joint Laboratory for Carbon Neutrality, Jiangmen Laboratory of Carbon Science and Technology, Jiangmen 529199, Guangdong, People’s Republic of China
Qianxi Dang
Shenzhen Key Laboratory of Advanced Materials, School of Materials Science and Engineering, Harbin Institute of Technology, Shenzhen 518055, Guangdong, People’s Republic of China
Jodie Yuwono
Faculty of Sciences, Engineering and Technology, School of Chemical Engineering, University of Adelaide, Adelaide, SA 5005, Australia
Shilin Zhang
Faculty of Sciences, Engineering and Technology, School of Chemical Engineering, University of Adelaide, Adelaide, SA 5005, Australia
Zhixin Tai
Advanced Energy Storage Materials and Technology Research Center, Guangdong‑Hong Kong Joint Laboratory for Carbon Neutrality, Jiangmen Laboratory of Carbon Science and Technology, Jiangmen 529199, Guangdong, People’s Republic of China
Zaiping Guo
Faculty of Sciences, Engineering and Technology, School of Chemical Engineering, University of Adelaide, Adelaide, SA 5005, Australia
Yajie Liu
Advanced Energy Storage Materials and Technology Research Center, Guangdong‑Hong Kong Joint Laboratory for Carbon Neutrality, Jiangmen Laboratory of Carbon Science and Technology, Jiangmen 529199, Guangdong, People’s Republic of China

Corresponding Author: Yajie Liu

liuyajie@hkustgz-jcl.ac.cn

Nano-Micro Letters, Vol. 17 (2025), Article Number: 292

Abstract

Aqueous zinc-ion batteries are promising candidates as stationary storage systems for power-grid applications due to their high safety and low cost. The practical implementation of Zn-ion batteries currently still faces formidable challenges because of Zn dendrite growth, hydrogen evolution, and inadequate environmental adaptability. Herein, to address these challenges, a strategy of regulation of water molecules coordination in electrolyte is proposed via developing a cross-linked hydrophilic hydrogel polymer electrolyte. Within this system, the continuous hydrogen bond among H2O molecules is disrupted and the isolated H2O molecules are strongly bound with a polymeric matrix comprised of polyacrylamide, carboxymethyl cellulose, and ethylene glycol, which can restrain the activity of H2O molecules, thus effectively alleviating Zn dendrite growth and hydrogen evolution and enhancing the anti-freezing ability. With this electrolyte, the Zn||Cu cell presents a high coulombic efficiency of 99.4% over 900 cycles and Zn||Zn symmetric cell exhibits high cycling stability, maintaining plating/stripping for over 1,700 h. Moreover, the assembled Zn||PANI device also demonstrates outstanding electrochemical performance over a wide-temperature range, including a long cycling life over 14,120 cycles at room temperature and an ultralong cycling surpassing 30,000 cycles even at − 40 °C. This showcases the manipulation of water coordination chemistry for advanced, highly adaptable batteries.


Highlights:
1 A hydrogel electrolyte regulation strategy of the water coordination environment can effectively restrain the hydrogen evolution reaction, Zn corrosion and dendrite formation in the wide-temperature ranges.
2 Prepared high-environment-adaptable hydrogel electrolytes (HEA-3) exhibits a high reversibility of zinc deposition/stripping (coulombic efficiency of 99.4% for Zn||Cu cell).
3 Zn-based device using HEA-3 electrolyte can do cycling over 30,000 cycles at a large current density of 2 A g−1 at − 40 °C and also can do normal cycling even at -70 °C.

Keywords

Coordination environment of water High environmental adaptability Hydrogel electrolyte Side reactions Low-temperature performance
Liu, Jianghe, Qianxi Dang, Jodie Yuwono, Shilin Zhang, Zhixin Tai, Zaiping Guo, and Yajie Liu. 2025. “Regulating the Coordination Environment of H2O in Hydrogel Electrolyte for a High-Environment-Adaptable and High-Stability Flexible Zn Devices”. Nano-Micro Letters 17 (June):292. https://doi.org/10.1007/s40820-025-01810-4.
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