Mechanochemical Regulated Origami with Tough Hydrogels by Ion Transfer Printing

Stimuli-responsive hydrogels that undergo programmable shape deformation are of great importance for a wide variety of applications spanning from soft robotics and biomedical devices to tissue engineering and drug delivery. To guide shape morphing, anisotropic elements need to be encoded into the hydrogels during fabrication, which are extremely difficult to alter afterward. This study reports a simple and reliable mechanochemical regulation strategy to postengineer the hydrogels by encoding structures of high stiffness locally into prestretched tough hydrogels through ion transfer printing with a paper-cut. During printing, trivalent ions (Fe³⁺) were patterned and diffused into the prestretched tough gels, which dramatically increased the local stiffness by forming the second trivalent ionically cross-linked network. By removing the applied stretching force, the stiff anisotropy-encoded prestretched tough hydrogels underwent programmable shape morphing into complex three-dimensional origami structures due to the stiffness mismatch.