Self-healable and mechanically robust supramolecular-covalent poly(oxime-urethane) elastomers with information encryption via hydrogen bonds and coordinate interactions

Self-healing polyurethane-elastomers are highly desired in various fields. However, there is often a trade-off between mechanical properties and dynamic self-healing due to the mutually exclusive mechanism. Herein, we develop a self-healable and mechanically robust poly(oxime-urethane) elastomer (Zn-DAPU) to circumvent this inherent trade-off by incorporating zinc-pyridinyl cross-links into the hydrogen bonding and dynamic oxime-urethane supramolecular-covalent hybrid network. Benefiting from the synergistic strengthening of H-bonding and coordinate interactions, Zn-DAPU network performs tunable toughness with metal ion concentration change, which improves 345.2% and reaches 82.2 MJ m ⁻³, with robust tensile strength of 22.8 MPa, Young’s modulus of 37.1 MPa, and satisfactory elongation of 815.7%. The healing efficiency can be reached at 91.7% with a restored toughness of 75.4 MJ m ⁻³ at 80 °C for 10 h. Furthermore, zinc-contained networks exhibit photolysis behavior due to the homolytic cleavage of N–O bonds in oxime-urethane moieties, which can be functionalized further with fluorescamine as the specific information encryption coating with quick response codes (QRs) upon polyester fabric. This work provides valuable guidance towards the development of high-performance self-healing polyurethane and wearable functional materials.