The Exponential Shapeshifting Response of N-Vinylcaprolactam Hydrogel Bilayers Due to Temperature Change for...

Poly (N-vinylcaprolactam) (PNVCL) and poly (N-isopropylacrylamide) (PNIPAm) are two popular negatively temperature-responsive hydrogels, due to their biocompatibility, softness, hydrophilicity, superabsorbency, viscoelasticity, and near-physiological lower critical solution temperature (LCST). These characteristics make them ideal for biomedical applications. When combined with other materials, hydrogel expansion induces the morphing of the assembly due to internal stress differences. Our recent developments in NVCL hydrogel, enhanced by nanoclay incorporation, have driven us to the creation of a bilayer structure to study its shapeshifting response across various temperatures. This study focused on the bending behaviour of bilayer samples composed of an active hydrogel layer and a passive non-swellable layer. Using photopolymerisation, circular discs and rectangular bilayer samples of varying sizes were fabricated. Homogeneous circular samples demonstrated that hydrogel density increased proportionally with temperature, with the swelling ratio exhibiting two distinct rates of change below and above its LCST. In bilayer samples, the volume of the passive layer influenced bending, and its optimal volume was identified. The investigation revealed that geometry affected the overall bending effect due to changes in the passive layer stiffness. Lastly, a temperature-responsive gripper capable of picking up objects several times its own weight was demonstrated, highlighting the potential of NVCL hydrogels as bioactuators for minimally invasive surgery.