Stimuli‐Responsive Polypeptide‐Based Supramolecular Hydrogels Mediated by Ca2+ Ion Cross‐Linking

Summary of main observation and conclusion Hydrogels cross‐linked with metal ions ( e.g ., Ca 2+ ) represent a promising class of bioinspired materials for a wide range of biomedical applications. Herein, we report a facile approach to obtain cross‐linked stimuli‐responsive supramolecular polypeptide hydrogels. The hydrogel is prepared by statistical/block copoly( L ‐glutamate)s based copolymers cross‐linked with calcium ions. The incorporation of both oligo(ethylene glycol) (OEG) and glutamic acid residues in the polymer offers thermal‐responsive property and cooperative binding sites with Ca 2+ ions simultaneously. We present a systematic study of the influence of calcium ions on the gelation behaviors of these copolymers. It is observed that the addition of calcium ions induces the formation of hydrogels. Increasing the concentration of Ca 2+ ions can significantly enhance the gelation ability of the samples as indicated by increased storage modulus and decreased sol‐to‐gel transition temperature ( T sol‐gel ). We further demonstrate that the influence of monomer distribution on the gelation behavior is trivial, which is possibly due to similar morphology of the self‐assemblies. The obtained hydrogels exhibit thermal‐responsive gelation behavior mediated by ion cross‐linking, which enables them to be ideal smart hydrogel system for many applications.