Solvent-Responsive Functionally Graded Hydrogel Thin Films for Programmed Actuation

Shape-shifting solvent-responsive hydrogels have emerged as a crucial material platform for the design of soft robots, sensors, and actuators. Generally, to achieve actuation under different environments, using a layered structure with heterogeneous properties is a prevalent approach. However, the nonuniform force distribution at the interface between the layers can induce material delamination, thus greatly compromising the system’s stability and applicability. Here, we present the fabrication, design, and analysis of a reversible and structurally stable single-component functionally graded (FG) hydrogel thin film. The gradation is in terms of the modulus and diffusion coefficient. The FG film exhibits a fast actuation rate and is capable of actuating in both immersed and nonimmersed aqueous environments. The fabricated FG film can eliminate the requirement for a layered structure yet retain all its functionalities. A coupled diffusion–deformation framework using the finite element (FE) method is employed to comprehend the mechanism and understand the factors governing the actuation of a FG film. The displacement profiles obtained from the simulations are successfully compared with the experiments for a FG–chitosan–water system. The rate of concentration change in different layers of the FG film is shown to play a pivotal role in steering the direction of actuation as well as the reversibility of folding under different conditions. The differential strain obtained from the length change between the different layers of the FG films is identified as a contributing factor for different actuation rates. Additionally, the simulation curvatures from different scenarios elucidate the influence of cross-linking gradation, water diffusion, and thickness on the folding of a FG film. As a prospective application, we demonstrate the design of different underwater grippers using geometrically engineered symmetric and asymmetric FG films.