Macromolecularly Engineered Thermoreversible Heterogeneous Self-Healable Networks Encapsulating Reactive Multidentate Block Copolymer-Stabilized Carbon Nanotubes.

The development of heterogeneous covalent adaptable networks (CANs) embedded with carbon nanotubes (CNTs) that undergo reversible dissociation/recombination through thermoreversibility has been significantly explored. However, the carbon nanotube (CNT)-incorporation methods based on physical mixing and chemical modification could result in either phase separation due to structural incompatibility or degrading conjugation due to a disruption of π-network, thus lowering their intrinsic charge transport properties. To address this issue, the versatility of a macromolecular engineering approach through thermoreversibility by physical modification of CNT surfaces with reactive multidentate block copolymers (rMDBCs) is demonstrated. The formed CNTs stabilized with rMDBCs (termed rMDBC/CNT colloids) bearing reactive furfuryl groups is functioned as a multicrosslinker that reacts with a polymaleimide to fabricate robust heterogeneous polyurethane (PU) networks crosslinked through dynamic Diels-Alder (DA)/retro-DA chemistry. Promisingly, the fabricated PU network gels in which CNTs through rMDBC covalently embedded are flexible and robust to be bendable as well as exhibit self-healing elasticity and enhanced conductivity.