Hydrogel Polymer Electrolytes for Aqueous Zinc-Ion Batteries: Recent Progress and Remaining Challenges
Zhaoxuan Zhu, Sihan Xiong, Jing Li, Lixin Wang, Xiaoning Tang, Long Li, Qi Sun, Yan Shi, Jiao‐Jing Shao
Abstract
Aqueous zinc-ion batteries (ZIBs) have attracted growing interest as promising candidates for large-scale and flexible energy storage due to their intrinsic safety, low cost, and environmental sustainability. However, several persistent issues—such as uncontrolled Zn dendrite growth, hydrogen evolution-induced anode corrosion, and cathode dissolution—continue to hinder their commercial deployment. To address these challenges, hydrogel polymer electrolytes (HPEs) have emerged as an effective strategy. Their unique three-dimensional polymer networks not only retain water and confine ion transport, but also provide a solid–liquid hybrid environment that enhances ionic conductivity and interfacial compatibility. These features enable HPEs to suppress side reactions and improve both electrochemical stability and mechanical adaptability, which are especially valuable for flexible ZIB devices. This review first summarizes fundamental energy storage mechanisms in aqueous ZIBs, including reversible Zn2+ insertion/extraction, proton co-insertion, and cathode phase evolution. It then highlights recent progress in HPE design, with emphasis on polyacrylamide (PAM), polyvinyl alcohol (PVA), and polyacrylic acid (PAA)-based systems, with strategies for dendrite suppression, interfacial regulation, and mechanical robustness. Finally, current challenges and future directions are discussed, with a forward-looking perspective on scalable fabrication methods, advanced electrolyte design, and deeper mechanistic understanding necessary to fully realize the potential of HPE-enabled aqueous ZIBs.