Responsive Gel-like Supramolecular Network Based on Pillar[6]arene–Ferrocenium Recognition Motifs in Polymeric Matrix

A dual-responsive supramolecular network based on pillar[6]arene–ferrocenium redox-controllable recognition motifs in polymeric backbones is constructed with a ferrocenium-functionalized copolymer and a pillar[6]arene copolymer, in which the first example of pillar[6]arene-functionalized copolymer was synthesized through the reversible addition/fragmentation chain-transfer copolymerization of an acrylate-functionalized pillar[6]arene and methyl acrylate. The resulting supramolecular network exhibits dramatically increased viscosity than the non-cross-linked mixtures and demonstrates a gel-like behavior on macroscale with a transient-network behavior revealed by rheology study. Furthermore, the viscoelastic properties of such supramolecular network can be easily controlled by different external stimuli including redox stimulus and competing host/guest reagents.