Reversing Redox Responsiveness of Hydrogels due to Supramolecular Interactions by Utilizing Double-Network Structures

Stimuli-responsive hydrogels have been actively researched, and some of them have been put into practical use. When we create and use stimuli-responsive hydrogel materials, controlling stimuli responsiveness of hydrogels is a very important issue. In this research, we prepared hydrogels having single-network (SN) or double-network (DN) gel structures with the host–guest interaction groups cyclodextrin and methyl viologen and evaluated their stimuli responsiveness. The results of the tensile and compression tests showed that the hydrogels with SN and DN structures exhibited opposite stimuli responsiveness in response to the redox reaction of methyl viologen through the association and dissociation of the host molecule, β-cyclodextrin, and the guest molecule, methyl viologen. Spectroscopic measurements and rheological studies all indicated that this difference in stimuli responsiveness originated from the polymer-network structures. In addition, a chemically cross-linked DN gel was prepared and its redox responsiveness was evaluated.