Mechano-responsive hydrogen-bonding array of thermoplastic polyurethane elastomer captures both strength and self-healing

Abstract Self-repairable materials strive to emulate curable and resilient biological tissue; however, their performance is currently insufficient for commercialization purposes because mending toughening are mutually exclusive. Herein, we report a carbonate-type thermoplastic polyurethane elastomer that self-heals at 35 °C exhibits tensile strength of 43 MPa; this as strong the soles used in footwear. Distinctively, it has abundant carbonyl groups soft-segments fully amorphous with negligible phase separation due poor hard-segment stacking. It operates dual mechano-responsive mode through reversible disorder-to-order transition its hydrogen-bonding array; heals when static toughens dynamic. In mode, non-crystalline hard segments promote dynamic exchange disordered hydrogen-bonds self-healing. The forms stiff crystals stretched orders inter-chain hydrogen bonding. strain return pre-stressed state after release repeat healing process.