A facile and on-demand optimizing strategy for polyurethane elastomers via programmable hydrogen bonding

Polyurethane elastomers address important significance in a wide range of applications. The mechanical properties including strength and toughness are of great importance, which are closely related to their unique hydrogen bonding structure. Unfortunately, the poor designability of hydrogen bonding structure in existing polyurethane severely restricts the on-demand regulation of their properties. Herein, a facile, universal and efficient modifying strategy based on stimuli-responsive polyphenol aggregates was proposed. Through precisely manipulated heat-induced aggregate division and/or photo-induced interfacial hydrogen bonding upgrading, programmable strengthening and toughening effect on the derived polyurethane elastomers could be achieved with high precision. Typically, the tensile strength and toughness of our proposed polyurethane elastomers could be enhanced by 3.23 and 2.22 times comparing with neat samples, respectively. The relevant results were supported by various characterizations and mathematical modeling. In addition, our polyurethane exhibited unique selective biocompatibility, rapid self-healing capability and recyclability, which could fulfill varieties of functions. Our proposed modifying strategy by using polyphenol aggregates can not only programmatically optimize the comprehensive properties of polyurethane, but also inspire programmable regulation of polymer performance through programmable design of its certain microstructure in the future.