Self‐Healing Ionogel‐Enabled Self‐Healing and Wide‐Temperature Flexible Zinc‐Air Batteries with Ultra‐Long Cycling Lives

Abstract Hydrogel‐based zinc‐air batteries (ZABs) are promising flexible rechargeable batteries. However, the practical application of hydrogel‐based ZABs is limited by their short service life, narrow operating temperature range, and repair difficulty. Herein, a self‐healing ionogel is synthesized by the photopolymerization of acrylamide and poly(ethylene glycol) monomethyl ether acrylate in 1‐ethyl‐3‐methylimidazolium dicyanamide with zinc acetate dihydrate and first used as an electrolyte to fabricate self‐healing ZABs. The obtained self‐healing ionogel has a wide operating temperature range, good environmental and electrochemical stability, high ionic conductivity, satisfactory mechanical strength, repeatable and efficient self‐healing properties enabled by the reversibility of hydrogen bonding, and the ability to inhibit the production of dendrites and by‐products. Notably, the self‐healing ionogel has the highest ionic conductivity and toughness compared to other reported self‐healing ionogels. The prepared self‐healing ionogel is used to assemble self‐healing flexible ZABs with a wide operating temperature range. These ZABs have ultra‐long cycling lives and excellent stability under harsh conditions. After being damaged, the ZABs can repeatedly self‐heal to recover their battery performance, providing a long‐lasting and reliable power supply for wearable devices. This work opens new opportunities for the development of electrolytes for ZABs.