Abstract

Self-healing materials that autonomously recover physical and functional failures have been investigated to improve the operational durability of stretchable and wearable devices. Although various self-healable materials have been reported, imparting self-healability to solid-state nonvolatile polymer electrolytes remains challenging. In this work, highly conductive, stretchable, self-supporting, transparent, and nonvolatile polymer electrolytes, or ionogels, capable of repairing physical and functional damages over 50% in 10 min and full recovery in 1 h without external stimuli were successfully developed using dynamic disulfide metathesis. Self-healable ionogels consisting of a cross-linked tetra-arm polyethylene glycol possessing disulfide linkages and 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, were successfully employed in stretchable/self-healable strain sensors and solid-state supercapacitors as piezoresistive components and electrolyte membranes, respectively. Both devices completely recovered their electrical/electrochemical performance even after repetitive cutting/healing cycles. Therefore, these results offer an effective strategy for developing both mechanically and electrically sustainable solid electrolytes for high-performance stretchable and wearable electronic/electrochemical devices.

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