Tough and Self-Healing Waterborne Polyurethane Elastomers via Dynamic Hydrogen Bonds Design for Flexible Conductive Substrate Applications

Balancing the mechanical strength and self-healing performance of polyurethane (PU) remains a significant challenge in achieving excellent self-repairing PU materials. In this study, a self-healing waterborne PU elastomer was designed from a bionic concept by incorporating 2'-deoxythymidine (2'-dT) and isophorone diamine (IPDA) into the polymer chain. The loose stacking of IPDA's irregular cycloaliphatic structure resulted in the irregular arrangement of urethane bonds in the hard domain. The formation of sextuple hydrogen bonds between 2'-dT and urethane bonds, as well as quadruple hydrogen bonds between urethane bonds themselves, enhanced the mechanical properties of the material. The multiple hydrogen bonds can dissociate, recombine, and dissipate energy, thereby improving the material's repair capability. The hierarchical self-assembly of hydrogen bonds enabled the PU to achieve a tensile strength of 15.3 MPa and toughness of 100.75 MJ/m³. The prepared PU film is highly transparent and has a transmittance of more than 90%. Additionally, it can undergo rapid repair under high temperatures or under trace solvent conditions. When used as a flexible conductive substrate, it quickly restored the conductivity and enhanced the material's lifespan after surface damage. This environmentally friendly and self-healing waterborne PU elastomer will hold broad application prospects in the field of flexible electronic devices.