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

Youngho Eom, Seon-Mi Kim, Minkyung Lee, Hyeonyeol Jeon, Jaeduk Park, Eun Seong Lee, Sung Yeon Hwang (), Jeyoung Park () and Dongyeop X. Oh ()
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Youngho Eom: Pukyong National University
Seon-Mi Kim: Korea Research Institute of Chemical Technology (KRICT)
Minkyung Lee: Korea Research Institute of Chemical Technology (KRICT)
Hyeonyeol Jeon: Korea Research Institute of Chemical Technology (KRICT)
Jaeduk Park: The Catholic University of Korea (CUK)
Eun Seong Lee: The Catholic University of Korea (CUK)
Sung Yeon Hwang: Korea Research Institute of Chemical Technology (KRICT)
Jeyoung Park: Korea Research Institute of Chemical Technology (KRICT)
Dongyeop X. Oh: Korea Research Institute of Chemical Technology (KRICT)

Nature Communications, 2021, vol. 12, issue 1, 1-11

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

Date: 2021
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DOI: 10.1038/s41467-021-20931-z

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