Dynamically Resettable Electrode‐Electrolyte Interface through Supramolecular Sol‐Gel Transition Electrolyte for Flexible Zinc Batteries

Abstract Flexible batteries based on gel electrolytes with high safety are promising power solutions for wearable electronics but suffer from vulnerable electrode‐electrolyte interfaces especially upon complex deformations, leading to irreversible capacity loss or even battery collapse. Here, a supramolecular sol‐gel transition electrolyte (SGTE) that can dynamically accommodate deformations and repair electrode‐electrolyte interfaces through its controllable rewetting at low temperatures is designed. Mediated by the micellization of polypropylene oxide blocks in Pluronic and host‐guest interactions between α‐cyclodextrin (α‐CD) and polyethylene oxide blocks, the high ionic conductivity and compatibility with various salts of SGTE afford resettable electrode‐electrolyte interfaces and thus constructions of a series of highly durable, flexible aqueous zinc batteries. The design of this novel gel electrolyte provides new insights for the development of flexible batteries.