Self-Healing Materials from V- and H-Shaped Supramolecular Architectures.

Integrating self-healing capability into supramolecular architectures is an interesting strategy, and can considerably enhance the performance and broaden the scope of applications for this important class of polymers. Herein we report the rational design of novel V-shaped barbiturate (Ba) functionalized soft-hard-soft triblock copolymers with a reversible supramolecular healing motif (Ba) in the central part of the hard block, which undergoes autonomic repair at 30 °C. The designed synthesis also offers a suitable macromolecular building block to further self-assemble with heterocomplementary α,ω-Hamilton wedge (HW) functionalized polyisoprene (PI; HW-PI-HW), resulting in an H-shaped supramolecular architecture with efficient self-healing capabilities that can recover up to around 95 % of the original mechanical performance at 30 °C within 24 h.