Mechanically robust, self-reporting and healable polyurethane elastomers by incorporating symmetric/asymmetric chain extenders

Abstract

Self-healing elastomers usually show poor mechanical properties and environmental stability, and they cannot self-report mechanical/chemical damage. Herein, an innovative design strategy is reported that combines symmetric/asymmetric chain extenders to create large yet disordered hard domains within polyurethane (PU) elastomers, enabling the integration of mechanical robustness and self-reporting and self-healing capabilities to overcome both mechanical and chemical damage. Specifically, large yet disordered hard domains were created by governing the molar contents of asymmetric fluorescent 2-(4-aminophenyl)-5-aminobenzimidazole (PABZ) and symmetric 4-aminophenyl disulfide (APDS). Such a structural feature led to a small free-volume fraction, prominent strain-induced crystallization (SIC), and high energy of dissipation, enabling the PU elastomer to display outstanding mechanical strength (60.7 MPa) and toughness (177.9 MJ m⁻³). Meanwhile, the loose stacking of disordered hard domains imposed small restriction on network chains and imparted the network with high relaxation dynamics, leading to high healing efficiency (97.8%). More importantly, the fluorescence intensity was stimulus-responsive and thus the PU elastomer could self-report mechanical/chemical damage and healing processes. The PU elastomer also showed potential application prospects in information encoding and encryption. Furthermore, selecting polydimethylsiloxane as one of the soft segments could effectively endow the PU elastomer with intrinsic hydrophobicity. Therefore, this work provides valuable guidance for designing multi-functional materials with anti-counterfeiting, self-reporting, and healing properties as well as high mechanical properties and hydrophobicity.