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Smart metallo-supramolecular hydrogels offer attractive possibilities to combine the properties of hydrogels with the self-assembly features offered by metal–ligand coordination. The preparation of metal-bis(terpyridine-poly(N,N-dimethylacrylamide)-b-poly(N-isopropylacrylamide)) ([M(Tpy-PDMA-b-PNIPAM)2]2+) complexes in aqueous media and their use for the elaboration of hydrogels by thermo-induced micellar aggregation is investigated in this study. The rheological behaviour suggested that the metal-bis complexes based on a copolymer having two distinct hydrophilic blocks self-assemble into flower-like micelles. Moreover, the control of the viscoelastic properties of the hydrogels is notably achieved via an appropriate choice of the nature and the molar equivalent composition of metal ions.

Graphical abstract: The effect of metal ions on the viscoelastic properties of thermosensitive sol-to-gel reversible metallo-supramolecular hydrogels

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