High‐performance shape memory characteristics by integrating urea linkages into the polyurethane elastomer

Shape memory polymers have been widely researched to develop multifunctional materials that respond smartly to external stimulations and programmed signals. Among them, shape memory polyurethane (SMPU) is drawing great attention owing to its highly tunable properties and ease of integrating new functions. However, the effect of urea bonds on SMPU elastomers has rarely been investigated because of the extreme reactivity of amine crosslinkers. In this study, we used diethanolamine (DEOA), which contains a secondary amine, as the crosslinker for SMPU synthesis. Unlike other crosslinkers containing primary amines, they can form urea bonds in a more gentle manner. The urea bonds reinforce the intermolecular interactions between the hard segments with strong hydrogen bonding, thus increasing the phase separation and degree of crystallization. Consequently, the urea‐containing SMPU exhibits improved mechanical strength and shape memory abilities for both fixing and recovery. Moreover, the transcarbamoylation reaction, which enables the reconfiguration of the original shape, is observed. The introduction of the urea bonds into the SMPU elastomer can be beneficial in achieving flawless shape memory performances in various sensitive applications.