Multifunctional Thermoplastic Polyurea Based on the Synergy of Dynamic Disulfide Bonds and Hydrogen Bond Cross-Links.

Integrating the self-healing property with the shape-memory effect is a strategy that extends the service lifetime of shape-memory materials. However, this strategy is inadequate to reshape and recycle through the self-healing property or liquid-state remoldability. For more types of damage, solid-state plasticity is needed as a complementary mechanism to broaden the reprocessing channels of smart materials. In this study, multifunctional thermoplastic polyureas cross-linked by urea hydrogen bonds are prepared, which possess the multipathway remodeling property. The shape transition can be triggered after heating above 65 °C. The synergistic effect of dynamic disulfide bonds and hydrogen bonds causes the thermoplastic polyureas to possess characteristics similar to those of associative covalent adaptable networks. Thus, the polyureas can repair the damage or reconfigure the shape at 75 °C in 15 min by solid-state plasticity, instead of going into a viscous flow state. Soft grippers with various shapes are prepared by integration of solid-state plasticity, and the structure and function of the grippers can be repaired. The integration of solid-state plasticity and the self-healing property broadens the paths of shape-memory polymers in recyclability and reshapability.