Hydrogel actuators have gained considerable interest and experienced significant advancements in recent years. However, the programming of their actuating behaviors is still challenging. Herein, we report the development and regulation of gradient structures of hydrogels for programmable thermally responsive actuating behaviors. The hydrogel actuators are developed by controlling the photoreduction of Fe3+ ions coordinated with carboxylate groups from the substrates and their limited diffusion into the precursor solutions to act as both initiators and crosslinkers. The developed hydrogels show well-defined external geometries and controllable thicknesses under spatiotemporal control of ultraviolet irradiation. The shapes and the actuation amplitudes of the hydrogel actuators can be independently regulated by controlling the formation and photodissociation of Fe3+-carboxylate coordination in the formed gradient networks. Some interesting applications such as the lifting of an object with a specific shape and directional walking are realized. The proposed method can be extended to other hydrogel actuators with different compositions and stimuli-responsive behaviors.
Keywords: Fe3+−carboxylate coordination; gradient; hydrogel; shape memory; thermally responsive actuation.