Supramolecular Fabrication of Complex 3D Hollow Polymeric Hydrogels with Shape and Function Diversity

Inspired by the high importance of hollow structures in nature such as blood vessels and bamboos in matter transportation, properties enhancement, or even survival of living creatures, the creation of hollow materials remains of considerable interest. However, constructing hollow unique living-like soft and wet polymeric hydrogels with desirable structures and functionalities is still a big challenge. Here, we reported a robust and effective strategy to fabricate complex three-dimensional (3D) hollow polymeric hydrogel with designed shape and function diversity on the basis of supramolecular interactions. By placing a Ca²⁺ included gelatin core into the solution of alginate, hydrogel shell could be formed along with the shape of the gelatin core via coordination between alginate chains and Ca²⁺ diffused from gelatin. The hollow hydrogel could finally be obtained by dissolving the gelatin core. Various complex 3D hollow structures could be achieved by designing/constructing assembled gelatin core as a building block with adjustable supramolecular metal coordination position and strength. Moreover, hollow hydrogels with function diversity could be developed by introducing functional polymers or nanoparticles into the hydrogel wall. This work has made important progress in developing hollow polymeric hydrogel with desirable structures, shapes, and various functional applications including soft actuators and chemical reaction containers.