Photoredox-Mediated Designing and Regulating Metal-Coordinate Hydrogels for Programmable Soft 3D-Printed Actuators.

Metal-organic coordination is widely applied for designing responsive polymers and soft devices. But it is still a challenge to prepare redox-responsive actuators with complicated structures, limiting their advanced applications in material and engineering fields. Here, we report a photoredox-mediated designing and regulating strategy to fabricate metal-coordinate hydrogels with the catalysis of Ru(II)/Co(III) under visible-light irradiation in seconds. Meanwhile, multiple polymer networks are formed and penetrated by each other, enabling as-prepared hydrogels excellent mechanical properties and toughness. This rapid, one-step, and controllable process is highly compatible with standard photography and printing techniques to make hierarchical 2D/3D structures. Importantly, the oxidization decomposition of Co(III) benefits the formation of cobalt cation-based redox-responsive networks, which have the potential for designing shape-memory materials and actuators by the regulation of Co 3+/2+ states via tuning redox environmental conditions. As a proof-of-concept, a programmable air-driven actuator is successfully demonstrated to control cargo capturing/releasing by designing complicated, asymmetric structures and optimizing their performance with the combination of a typical extrusion 3D printing approach. In this Letter, we report a simple and general metal-organic coordination strategy for designing high-performance actuators, which shows promising applications in smart soft devices and electronics.