Tough, self‐healing, and recyclable cross‐linked polyurethane elastomers via synergistic effect of dual dynamic covalent bonds

Abstract Based on the irresistible inherent trade‐off between the mechanical and self‐healing performances of cross‐linked polyurethane materials, there is still an intractable challenge to design efficient self‐healing and tough elastomers, especially in flexible sensors. Herein, a tough, efficient self‐healing, and recyclable cross‐linked polyurethane elastomer (DTPU) was prepared by integrating oxime‐carbamate bonds and thiourethane bonds into the network. The extraordinary mechanical properties and self‐healing performances of DTPU elastomers were related to the synergistic effect of oxime‐carbamate bonds in the main chain and thiourethane bonds in the chemical cross‐linked sites. The existence of dynamic cross‐linked points not only optimized the mechanical properties of DTPU but also provided support for the reversible cleavage and formation of oxime carbamate bond, thus endowing DTPU with efficient self‐healing performance and recyclability. After self‐healing at mild temperatures for 6 h, the self‐healed DTPU elastomers had a tensile strength of 30.27 MPa and a self‐healing efficiency of 95.5%. After multiple hot‐pressing, the original mechanical strength of DTPU was restored to over 100%, exhibiting excellent recyclable characteristics. Additionally, strain sensors based on self‐healing flexible elastomers were fabricated by introducing conductive carbon nanotubes. The strain sensors maintained their electrical conductivity after 3 times self‐healing, demonstrating great potential in healable flexible electronics.