Self-healable, stretchable, and nonvolatile solid polymer electrolytes for sustainable energy storage and sensing applications

Self-healing materials that autonomously recover physical and functional failures have been investigated to im-prove 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 challeng-ing. In this work, highly conductive, stretchable, self-supporting, transparent, and nonvolatile polymer elec-trolytes, 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, respec-tively. Both devices completely recovered their electrical/electrochemical performance even after repetitive cut-ting/healing cycles. Therefore, these results offer an effective strategy for developing both mechanically and elec-trically sustainable solid electrolytes for high-performance stretchable and wearable electronic/electrochemical devices.