Progress in Developing Polymer Electrolytes for Advanced Zn Batteries

Aqueous Zn batteries (ZBs) are promising candidates for large-scale energy storage, considering their intrinsically safe features, competitive cost, and environmental friendliness. However, the fascinating metallic Zn anode is subjected to severe issues, such as dendrite growth, hydrogen evolution, and corrosion. Additionally, traditional aqueous electrolytes' narrow electrochemical windows and temperature ranges further hinder the practical application of ZBs. Solid-state electrolytes, including solid polymer electrolytes and hydrogel electrolytes, offer distinct paths to mitigate these issues and simultaneously endow the ZBs with customizable functions such as flexibility, self-healing, anti-freezing, and regulated Zn deposition, etc, due to their tuneable structures. This review summarizes the latest progress in developing polymer electrolytes for ZBs, focusing on modifying the ionic conductivity, interfacial compatibility, Zn anode stability, electrochemical stability windows, and improving the environmental adaptability under harsh conditions. Although some achievements are obtained, many critical challenges still exist, and it is hoped to offer guidance for future research, accelerating the development and application of polymer electrolytes. © 2025 The Author(s). Small Methods published by Wiley-VCH GmbH.