Programmed Transformations of Strong Polyvinyl Alcohol/Sodium Alginate Hydrogels via Ionic Crosslink Lithography

A versatile ionic crosslink lithography (ICL) approach is reported to achieve geometry transitions of strong polyvinyl alcohol/sodium alginate (PVA/SA) hydrogels in a controllable and programmable manner. Specifically, localized PVA/SA and PVA/SA/Fe³⁺ hydrogel domains of significantly different swellabilities (i.e., in-plane gradient) are created by patterning and selective ionic crosslinking of one single type of PVA/SA hydrogel. A simple two-step sequential pre- and free-swelling, or each alone, directs the patterned, inhomogeneous hydrogel to transform in various programmable and quasi-quantitative ways through local bulging and/or global buckling. All types of shape changing are reversible and repeatable due to the reversible nature of ionic coordination in the hydrogel networks. The flexibility and versatility of 3D printing is also demonstrated in creating through-thickness gradient in PVA and PVA/SA hydrogel assemblies with similar morphing capability. The ICL approach developed in this work may help shed some light on developing strong and shape morphing hydrogels as soft sensors and actuators and for potentially biomimetic transformations. The ICL approach may also be transferable to fabrication of many other types of hydrogel materials for similar applications.