Bio-inspired self-healing polyurethane system: Mimicking connective tissue with hydrogen-bonding mechanism

Achieving a balance between mechanical strength and self-healing efficiency in self-healing materials is challenging yet crucial. This work introduces PCL-HBU, a polyurethane material designed for the first time to mimic collagen fibers, elastic fibers, and vascular networks of connective tissue, with excellent mechanical properties and self-healing efficiency. Meanwhile, by adjusting the 2-ureido-4-[1H]-pyrimidinone (UPy) and N,N-bis(2hydroxyethyl)oxamide (BHO) ratio, this work creatively developed PCL-HBU3 with three distinct phase structures: amorphous region, soft segment crystallisation, and hard segment crystallisation, which approach confers excellent mechanical properties to the material. PCL-HBU3 exhibits a tensile strength of 70.0 MPa and elongation at break of 1500 %. It can recover from 600 % elongation within 20 s, achieving 100 % elongation at break selfhealing efficiency. Furthermore, the composite conductive material fabricated using PCL-HBU3 as the matrix showcases self-healing abilities and holds promise in motion detection and sound recognition applications.