Dynamic Non-Covalent Bonds Powering Enhanced Temporary Shape Retention Temperature and Mechanical Robustness in Shape Memory Polyurethane

Shape memory polyurethane (SMPU) with excellent mechanical properties holds significant application value in engineering. However, achieving high strength and toughness typically relies on hydrogen bonding for energy dissipation, which limits the application of such PUs due to their deformation temperature being below room temperature. Here, we introduce a rigid long-chain polyamide acid with a rich aromatic structure as a chain extender, combined with metal coordination, to develop a shape memory polyurethane with a phase transition temperature of 50 °C and outstanding mechanical performance. The presence of rigid segments of polyamic acid (PAA) and −COOH not only increases the rigidity of the polyurethane chains but also promotes the formation of hydrogen bonds and π–π conjugation, leading to physical cross-linking points and significant microphase separation, resulting in superior mechanical properties for PU-PAA. The dynamic bonding characteristics impart self-healing and solvent recyclability to PU-PAA. The coordination interactions enhance the cross-linking points, enabling PU-PAA-Eu to exhibit excellent shape fixation and recovery rates, as well as fluorescence properties. Additionally, due to the presence of −COOH, PU-PAA demonstrates remarkable adhesion to various metals. This work provides a strategy toward the development of high performance SMPU and holds promising potential for applications such as anticounterfeit coatings.