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.