Intelligent Polymer Electrolytes for Next-Generation Zinc-Based Energy Storage Devices

Intelligent polymer electrolytes for zinc-based energy-storage devices have attracted considerable attention as multifunctional platforms capable of simultaneously regulating ion transport, water activity, interfacial chemistry, and mechanical stability. This review presents a comprehensive overview of intelligent polymer electrolytes for zinc-ion batteries (ZIBs), zinc-air batteries (ZABs), and zinc-ion hybrid capacitors (ZIHCs), encompassing hydrogels, organo-hydrogels, composite polymer electrolytes, and solid-state polymer systems. Particular attention is given to the molecular and structural strategies underlying ion-solvation regulation, selective ion transport, dendrite suppression, corrosion inhibition, antifreezing behavior, self-healing, adhesion, and mechanical adaptability. Emerging functionalities, including self-healing, antifreezing, self-adhesive, stretchable, and temperature-responsive behavior, are highlighted in the context of improving operational durability under mechanical deformation and extreme temperatures. Bio-derived polymer electrolytes and the growing use of artificial intelligence, machine learning, and computational simulations for electrolyte discovery and optimization are also discussed. Finally, key challenges associated with scalability, reproducibility, manufacturing, cost, sustainability, and practical full-cell validation are critically assessed. Future research should prioritize multifunctional, adaptive, sustainable, and scalable polymer architectures that concurrently regulate ion transport, interfacial reactions, mechanical integrity, and environmental stability. Collectively, this review provides a framework for the rational design of intelligent polymer electrolytes toward safer, more durable, flexible, and commercially viable zinc-based energy-storage technologies.