Redox‐Responsive Macroscopic Gel Assembly Based on Discrete Dual Interactions

The macroscopic self-assembly of polymeric hydrogels modified with β-cyclodextrin (βCD gel), ferrocene (Fc gel), and styrenesulfonic acid sodium salt (SSNa gel) was investigated. Under reductive conditions, the Fc gel selectively adhered to the βCD gel through a host-guest interaction. On the other hand, the oxidized ferrocenium (Fc(+)) gel selectively adhered to the SSNa gel through an ionic interaction under oxidative conditions. The adhesion strength was estimated by a tensile test. We finally succeeded in forming an ABC-type macroscopic assembly of all three gels through two discrete noncovalent interactions.