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

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          Abstract

          A new thermoresponsive double hydrophilic block copolymer bearing a terpyridine moiety formed a hydrogel with a sol–gel thermoreversible transition in the presence of Fe 2+ ions.

          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 (Fe 2+) 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 Fe 2+ 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.

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          Most cited references49

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          Micellization of block copolymers

          G Riess (2003)
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            Multistimuli, multiresponsive metallo-supramolecular polymers.

            The use of metal ion-induced polymerizations of a ditopic ligand offers a facile route to the preparation of organic/inorganic hybrid materials. Such metallo-supramolecular polymers potentially offer the functionality of the metal ion along with the processibility of a polymer. We report, herein, the preparation of gellike metallo-supramolecular polymers prepared from a monomer unit, which consists of a 2,6-bis-(benzimidazolyl)-4-hydroxypyridine unit attached to either end of a polyether chain, mixed with a transition metal ion (e.g., Co(II) or Zn(II)) and a small percentage of a lanthanoid metal (e.g., La(III), Eu(III)). Such materials show dramatic reversible responses to a variety of stimuli, including thermal, mechanical, chemo, and photo. The nature of the response can be controlled by the nature of the combination of transition metal ion and lanthanide metal ion used.
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              Self-healing polymer coatings based on crosslinked metallosupramolecular copolymers.

              Self-healing coating based on metallopolymers are prepared and fully characterized. Iron bisterpyridine complexes are incorporated into a polymer network based on methacrylates, resulting in self-healing properties of these materials. Moreover, the influence of the comonomers on the thermal properties is studied in detail. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
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                Author and article information

                Journal
                PCOHC2
                Polymer Chemistry
                Polym. Chem.
                Royal Society of Chemistry (RSC)
                1759-9954
                1759-9962
                2016
                2016
                : 7
                : 44
                : 6834-6842
                Article
                10.1039/C6PY01639A
                7e6e3af1-04d8-4f7a-b860-dcf34edc1604
                © 2016
                History

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