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.