MOCA-Based Poly(Urethane–Urea) Elastomers With High Stretchability, Strength, and Self-Healing via Synergistic Dynamic Bonds

Simultaneously achieving high strength and efficient self-healing in a single material remains a fundamental challenge in the field of elastomeric materials. In this study, self-healing poly(urethane-urea) (PU) elastomers were successfully prepared through the strategic incorporation of both rigid MOCA (4,4'-methylenebis(2-chloroaniline)) structures and thermo-reversible oxime-urethane bonds into the main chains, coupled with dynamic zinc-ion coordination. Due to the synergistic interactions among hydrogen bonding networks, oxime-amino ester bonds, and metal-ligand bonds, PU elastomers exhibited high tensile strength (8.07 MPa), elongation at break (771.72%), and healing efficiency (92.29%). Moreover, an excessively high content of MOCA can lead to a transition from hydrophilic to a hydrophobic state. With the exceptional performance, PU materials demonstrated strong potential for practical implementation in protective coatings, flexible electronic substrates, stimuli-responsive thin films, and related advanced functional material systems.