Multistimuli‐Responsive, Moldable Supramolecular Hydrogels Cross‐Linked by Ultrafast Complexation of Metal Ions and Biopolymers

A new type of multistimuli-responsive hydrogels cross-linked by metal ions and biopolymers is reported. By mixing the biopolymer chitosan (CS) with a variety of metal ions at the appropriate pH values, we obtained a series of transparent and stable hydrogels within a few seconds through supramolecular complexation. In particular, the CS-Ag hydrogel was chosen as the model and the gelation mechanism was revealed by various measurements. It was found that the facile association of Ag(+) ions with amino and hydroxy groups in CS chains promoted rapid gel-network formation. Interestingly, the CS-Ag hydrogel exhibits sharp phase transitions in response to multiple external stimuli, including pH value, chemical redox reactions, cations, anions, and neutral species. Furthermore, this soft matter showed a remarkable moldability to form shape-persistent, free-standing objects by a fast in situ gelation procedure.