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.

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