Mechanism Exploration of Spider-Silk-Inspired Multiple-Hydrogen-Bond Polyurethane Healable Elastomers for...

Spider-silk-inspired multiple-hydrogen-bond polyurethane (PU) healable elastomers have garnered significant attention across various industries. While individual hydrogen bonds are relatively weak, their collective cooperation generates strong interaction forces with geometrically hydrogen-bond-confined arrays. Under the guidance of this discovery, the synthesized PU elastomer (PU-MDI) had superior mechanical characteristics and a self-healing efficiency of 98%, which can provide a robust barrier to effectively delay the penetration of corrosive ions and resist external impact energy dissipation. PU-MDI exhibited excellent anticorrosion and anticavitation performance at conventional temperature. However, as temperature rose, the intensive multiple hydrogen bonds weakened and cracked, leading to a significant degradation in the functional properties of PU-MDI. This breakdown rendered PU-MDI unsuitable for elevated-temperature anticorrosion applications, and the study elucidated the inadequacy reasons. These findings offer critical insights into the practical application, directional development, and inadequacy prevention of multiple-hydrogen-bonded healable polymer materials, with implications for future anticorrosion and self-healing material innovation.