Formulation of Sugar/Hydrogel Inks for Rapid Thermal Response 4D Architectures with Sugar-derived Macropores

Programmed, reshaping hydrogel architectures were fabricated from sugar/hydrogel inks via a three-dimensional printing method involving a stimuli-responsive polymer. We developed a new hydrogel ink composed of monomers (acrylamide [AAm]) and N-isopropylacrylamide [NIPAAm]), and sugar (mixture of glucose and sucrose) as a pore-generator, enabling to improve printability by increasing the ink's viscoelastic properties and induce the formation of macropores in the hydrogel architectures. This study demonstrated that creating macropores in such architectures enables rapid responses to stimuli that can facilitate four-dimensional printing. We printed bilayer structures from monomer inks to which we had added sugar, and we exposed them to processes that cross-linked the monomers and leached out the sugar to create macropores. In comparison with a conventional poly(N-isopropylacrylamide) hydrogel, the macroporous hydrogels prepared using polymerization in the presence of a high concentration of sugar showed higher swelling ratios and exhibited much faster response rates to temperature changes. We used rheometry and scanning electron microscopy to characterize the properties of these inks and hydrogels. The results suggest that this method may provide a readily available route to the rapid design and fabrication of shape-morphing hydrogel architectures with potential application in soft robotics, hydrogel actuators, and tissue engineering.