Light- and Solvent-Responsive Bilayer Hydrogel Actuators with Reversible Bending Behaviors

Light-responsive hydrogel systems have gained significant attention due to their unique ability to undergo controlled and reversible swelling behavior in response to light stimuli. Combining light-responsive hydrogels with nonresponsive polymers offers a unique self-folding feature that can be used in soft robotic actuator designs. However, simple formulation of such systems with rapid response time is still a challenging task. Herein, we demonstrate a simple but versatile bilayer polymeric design combining light-responsive spiropyran-polyacrylamide (SP-PAAm) with polyacrylamide (PAAm) hydrogels. The photochromic spiropyran in our polymer design is a closed-ring, hydrophobic compound and turns into an open-ring, hydrophilic merocyanine isomer under light irradiation. The swelling degree of SP-PAAm and PAAm hydrogels was evaluated using LED lights with different wavelengths and solvent media (e.g., water, ethanol, DMF, and DMSO). We observed that SP-PAAm hydrogels reached a swelling ratio of similar to 370% with the illumination of the blue LED in the DMF medium. By combining light-responsive SP-PAAm hydrogels with nonresponsive PAAm, a proof-of-concept demonstration was performed to demonstrate the applicability of our fabricated platforms. Although fabricated one-armed bilayer hydrogels possessed self-folding ability with a folding angle of similar to 40 degrees in 30 min, the four-armed bilayer platforms demonstrated more efficient and rapid folding behavior and reached a folding angle of similar to 75 degrees in similar to 15 min. Given their simplicity and efficiency, we believe that such polymeric designs may offer new avenues for the fields of polymeric actuators and soft robotic systems.