Key Takeaways & Executive Findings
- •• 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. • 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). • 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. • The manipulation of water coordination chemistry enables advanced, highly adaptable batteries for wide-temperature applications.
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.
1. Introduction
Aqueous zinc-ion batteries are promising candidates as stationary storage systems for power-grid applications due to their high safety and low cost. However, the practical implementation of Zn-ion batteries currently still faces formidable challenges because of Zn dendrite growth, hydrogen evolution, and inadequate environmental adaptability. 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.
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Jianghe Liu, Qianxi Dang, Jodie Yuwono, Shilin Zhang, Zhixin Tai, Zaiping Guo, 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. https://doi.org/10.1007/s40820-025-01810-4
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Frequently Asked Questions
What is the main challenge addressed in this paper?
The paper addresses the challenges of Zn dendrite growth, hydrogen evolution, and inadequate environmental adaptability in aqueous zinc-ion batteries.
How does the proposed hydrogel electrolyte improve performance?
The hydrogel electrolyte disrupts hydrogen bonds among water molecules and binds them strongly to a polymer matrix, reducing water activity, suppressing side reactions, and enhancing anti-freezing ability.
What are the key performance metrics achieved?
The Zn||Cu cell achieves 99.4% coulombic efficiency over 900 cycles, Zn||Zn symmetric cell operates over 1,700 h, and Zn||PANI device cycles over 30,000 times at -40 °C.
What is the significance of this work?
This work demonstrates a strategy to regulate water coordination chemistry, enabling highly adaptable and stable zinc-based energy storage devices for wide-temperature applications.
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