Rapid photo‐responsive dynamic disulfide strategy for accessing self‐healing, reconfigurable shape of high‐strength shape memory polyurethane

Abstract Enabling soft shape memory polyurethane (SMPU) with self‐healing is an effective strategy to extend its service life; however, the tradeoff between high mechanical strength and rapid self‐healing to meet the practical applications remains a challenge. Herein, we prepared a polyurethane (PU) with polycarbonate diol as a soft segment, incorporating urea bonds and dynamic disulfide bonds through chain extenders. This material, denoted as PU‐NSS75, exhibited a remarkable tensile strength of 51.4 MPa, attributed to the synergistic energy dissipation effect of urea hydrogen bonding and dynamic disulfide bonds during stretching, leading to enhanced mechanical properties of the PU. The dynamic nature of the bonds, including hydrogen bonding and disulfide bonds, endowed the PU with exceptional self‐healing capabilities. Furthermore, leveraging the reversible mechanism of disulfide bonds under UV irradiation at room temperature, PU‐NSS75 achieved complete self‐healing within 1 min. This photoinduced dynamic chemical bonding also facilitated rapid reconfigure the original shape of the soft SMPU at room temperature, thus broadening its potential applications. This study offers a design approach to enhance soft shape memory polyurethane materials, while the rapid self‐healing and shape reconfiguration provide new avenues for expanding the applications of shape memory polyurethanes.