Self‐Healing Polyurethanes With Tunable Mechanical Properties via a Rigid–Dynamic Dual Network Strategy

ABSTRACT A self‐healing and reprocessable polyurethane elastomer was developed via a rigid–dynamic dual network strategy, which integrates a covalent adaptive network (CAN) based on dynamic crosslinkers dimethylglyoxime (DMG) and with the rigid aromatic structure of tetrabromobisphenol A bis(2‐hydroxyethyl) ether (TBBPA‐BHEE). This work systematically examines the influence of TBBPA‐BHEE and DMG on the mechanical characteristics, dynamic reorganization behavior, and self‐healing capabilities of the resulting elastomers. Through compositional adjustments, a series of tunable elastomers were synthesized and evaluated. The optimized elastomer demonstrates a tensile strength of 14.8 MPa, a toughness of 58.9 MJ/m 3 , and an elongation at break of 927.9%. These results highlight the efficacy of incorporating CAN structures into polyurethane systems to achieve multifunctional performance. The developed elastomers exhibit excellent reprocessing and recyclability, addressing environmental concerns associated with traditional polyurethanes. Reversible oxime urethane bonds make reshaping and reuse of the new polyurethanes available under mild thermal conditions.