Surface Patterning of Hydrogels for Programmable and Complex Shape Deformations by Ion Inkjet Printing

Convenient patterning and precisely programmable shape deformations are crucial for the practical applications of shape deformable hydrogels. Here, a facile and versatile computer‐assisted ion inkjet printing technique is described that enables the direct printing of batched, very complicated patterns, especially those with well‐defined, programmable variation in cross‐linking densities, on one or both surfaces of a large‐sized hydrogel sample. A mechanically strong hydrogel containing poly(sodium acrylate) is first prepared, and then digital patterns are printed onto the hydrogel surfaces by using a commercial inkjet printer and an aqueous ferric solution. The complexation between the polyelectrolyte and ferric ions increases the cross‐linking density of the printed regions, and hence the gel sample can undergo shape deformation upon swelling/deswelling. The deformation rates and degrees of the hydrogels can be conveniently adjusted by changing the printing times or the different/gradient grayscale distribution of designed patterns. By printing appropriate patterns on one or both surfaces of the hydrogel sheets, many complex 3D shapes are obtained from shape deformations upon swelling/deswelling, such as cylindrical shell and forsythia flower (patterns on one surface), ding (patterns on both surfaces), blooming flower (different/gradient grayscale distributive patterns on one surface), and non‐Euclidean plates (different/gradient grayscale distributive patterns on both surfaces). Computer‐assisted ion inkjet printing technique enables the direct printing of complicated patterns, especially those with different or gradient grayscale distributions. By printing with appropriate patterns on one or both surfaces of the hydrogel sheets, many complex 3D shapes are obtained from the shape deformations upon swelling/deswelling, such as protuberant hexagon with sexfoil patterns, ding, blooming flower, and non‐Euclidean plate shapes.