Engineering Light-responsive Azo-polyurethane Actuators: Integrated Self-healing and Reshaping via Synergistic Disulfide-hydrogen Bonding
摘要
Azobenzene-based polymer actuators show great promise for photoactuation owing to their unique photoisomerization behavior and tailorable molecular programmability. However, conventional systems are limited by inadequate mechanical robustness, self-healing, and recyclability, hindering their practical implementation. Herein, we present a high-performance azobenzene-functionalized polyurethane (AzoPU) elastomer actuator designed via molecular engineering of photoactive azobenzene moieties and dynamic disulfide bonds. AzoPU exhibits exceptional mechanical properties with retained performance after multiple reshaping cycles, enabled by well-engineered hard-soft segments and synergistic stress dissipation from weak covalent bonds/hierarchical hydrogen bonds. It achieves over 93% self-healing efficiency at room temperature owing to the synergistic interplay of disulfide bonds in the polymer backbone and intermolecular hydrogen bonds. Furthermore, it demonstrates remarkable light-triggered actuation behavior, achieving a phototropic bending angle exceeding 180° toward the light source within 45 s. To showcase its practical potential, proof-of-concept photoactuated devices with flower-, hook-, and gripper-like and local-orientation processed strip-shaped structures were fabricated, which exhibited rapid and reversible light-triggered deformation. This study proposes a novel strategy for the development of intelligent polymeric materials that integrate light responsiveness, self-healing, and recyclability, thus holding great promise for applications in flexible electronics, smart actuators, and sustainable functional materials.