4D-Printed Hydrogel Actuators through Diffusion-Path Architecture Design.

Recently, smart hydrogels have garnered considerable attention as biomedical devices, and several approaches have been introduced for their fabrication, including the incorporation of stimulus-responsive additives, utilization of molecular imprinting techniques, and application of multilayered hydrogels. However, the nonuniform properties resulting from these approaches limit the practical applications of hydrogels by causing inconsistent performance and behavior. In this study, we propose a novel approach to manipulating the swelling kinetics of hydrogels by engineering their diffusion-path architecture. By simply adjusting the diffusion path length within the hydrogel, we achieved a significant change in swelling kinetics. This approach enables precise control over the diffusion and transport processes within the hydrogel, resulting in enhanced swelling kinetics when reducing the diffusion path length. Furthermore, by strategically designing the diffusion-path architecture of a 3D-printed hydrogel specimen, we can fabricate smart hydrogel actuators that exhibit reversible shape transformations during swelling and deswelling through a nonequilibrium differential swelling. The proposed approach eliminates the need to modify the spatial properties of hydrogel structures such as cross-linking density, polymer, or additive compositions, thereby achieving uniform properties throughout the hydrogel and creating new possibilities for the development of advanced 4D-printed biomedical devices.