Terminally cross‐linking polyrotaxane hydrogels applicable for cellular microenvironments

Abstract

AbstractPolyrotaxanes, composed of multiple cyclic molecules threaded onto a polymer chain axis capped with bulky molecules, exhibit unique structural features wherein cyclic molecules can move along a chain. We have previously constructed biointerfaces that utilize the molecular mobility of polyrotaxanes for controlling cellular responses. To implement the features in a three‐dimensionally engineered cellular microenvironment, this study developed supramolecular hydrogels using polyrotaxane cross‐linkers capped with 4‐vinylbenzyl groups at the terminals of a polymer chain axis, where the 4‐vinylbenzyl groups in the polyrotaxane allow polymerization with other polyrotaxanes to form polyrotaxane networks. Polyrotaxane hydrogels are successfully prepared without any additional monomers via redox polymerization. The dynamic viscoelasticity and swellability of the hydrogels can be varied depending on the concentration of the polyrotaxanes. When fibroblasts are cultured on hydrogels, sufficient adhesion for cultivation is observed. Therefore, polyrotaxane hydrogels demonstrate suitable potential as new supramolecular biomaterials with dynamic structural features.