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

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. © The Author(s) 2025.