Issue 44, 2016

Sol–gel reversible metallo-supramolecular hydrogels based on a thermoresponsive double hydrophilic block copolymer

Abstract

A well-defined poly(N,N-dimethylacrylamide)-b-poly(N-isopropylacrylamide-co-2-vinyl-4,4-dimethylazlactone) thermoresponsive double hydrophilic block copolymer bearing a terpyridine entity (Tpy-PDMA-b-P(NIPAM-co-VDM)) was synthesized by successive RAFT polymerizations. An amphiphilic macro-chain transfer agent bearing a terpyridine moiety (Tpy-PDMA-CTA) was synthesized and used for the preparation of a double hydrophilic block copolymer (Tpy-PDMA-b-P(NIPAM-co-VDM)) by RAFT dispersion polymerization. The RAFT dispersion polymerization of water-soluble monomers showed good control over the molar mass and dispersity, as characterized by size exclusion chromatography (SEC) and 1H-NMR spectroscopy. Complexation in the presence of metal ions (Fe2+) and self-assembly of the Tpy-PDMA-b-P(NIPAM-co-VDM) copolymer in diluted solution (0.5% w/v) were investigated. The formation of dynamic metallo-supramolecular flower-like micelles was demonstrated by UV-Vis spectrophotometry and dynamic light scattering (DLS). The effect of the addition of Fe2+ ions to a concentrated solution (8% w/v) of the Tpy-PDMA-b-P(NIPAM-co-VDM) copolymer at low temperature was investigated and the thermal profile of the metallic bis-terpyridine complex ([Fe(Tpy-PDMA-b-P(NIPAM-co-VDM))2]2+) has been studied by differential scanning calorimetry (DSC). The influence of temperature on the aqueous solution (8% w/v) of the ([Fe(Tpy-PDMA-b-P(NIPAM-co-VDM))2]2+) metallic complex was investigated by rotational rheometry. The results show that the self-assembly of the thermoresponsive block of the metallic bis-terpyridine complex formed a dynamic hydrogel with a sol–gel thermoreversible transition.

Graphical abstract: Sol–gel reversible metallo-supramolecular hydrogels based on a thermoresponsive double hydrophilic block copolymer

Supplementary files

Article information

Article type
Paper
Submitted
18 Sep 2016
Accepted
18 Oct 2016
First published
19 Oct 2016
This article is Open Access
Creative Commons BY-NC license

Polym. Chem., 2016,7, 6834-6842

Sol–gel reversible metallo-supramolecular hydrogels based on a thermoresponsive double hydrophilic block copolymer

M. Le Bohec, M. Banère, S. Piogé, S. Pascual, L. Benyahia and L. Fontaine, Polym. Chem., 2016, 7, 6834 DOI: 10.1039/C6PY01639A

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