Reference : Contribution of cobalt-mediated radical polymerization to macromolecular engineering ...
Dissertations and theses : Doctoral thesis
Physical, chemical, mathematical & earth Sciences : Chemistry
Contribution of cobalt-mediated radical polymerization to macromolecular engineering and photodynamic therapy
[fr] Apport de la polymérisation radicalaire contrôlée par des complexes de cobalt à l'ingénierie macromoléculaire et à la thérapie photodynamique
Hurtgen, Marie mailto [Université de Liège - ULiège > > Centre d'études et de rech. sur les macromolécules (CERM) >]
Université de Liège, ​Liège, ​​Belgique
Docteur en Sciences
xx, 229
Detrembleur, Christophe mailto
Luxen, André mailto
Mouithys-Mickalad, Ange mailto
Heuts, Hans mailto
Junkers, Thomas mailto
Jérôme, Christine mailto
[en] controlled radical polymerization ; transition metals ; fullerenes ; photodynamic therapy ; macromolecular engineering ; biocompatible polymers ; water-soluble polymers ; thermo-responsive polymers ; copolymers
[en] Cobalt-mediated radical polymerization (CMRP) is an emerging class of controlled radical polymerization technique based on the reversible deactivation of the propagating radicals by a cobalt complex. This thesis aims at broadening the nature, the structure, the properties and the end-use of (co)polymers accessible by CMRP. The first part of this work is devoted to the synthesis of novel statistical, graft and block copolymers by CMRP. First, the statistical copolymerization of conjugated (n-butyl acrylate) with a non-conjugated one (vinyl acetate) has been successfully controlled by bis(acetylacetonato)cobalt(II). The optimal experimental conditions were then implemented to the copolymerization of vinyl acetate with poly(ethylene glycol) acrylate, which yielded (quasi-)diblock amphiphilic graft copolymers for potential biomedical applications in one step. CMRP also revealed successful for the synthesis of well-defined thermo-responsive copolymers based on poly(N-vinylcaprolactam), either amphiphilic or double-hydrophilic at room temperature. In the second part of this thesis, we investigated the potential of CMRP for the synthesis of new agents for cancer photodynamic therapy. The synthesis of such photosensitizers relied on the chain-end functionalization by [60]fullerene of water-soluble (co)polymers (or precursors) prepared by CMRP. The photodynamic activity of poly(vinyl alcohol)/C60, poly(N-vinylpyrrolidone-co-vinyl acetate)/C60 and poly(PEG acrylate-co-vinyl acetate)/C60 nanohybrids were assessed through photophysical and in vitro experiments. Also, the ability of the nanohybrids to avoid recognition by the immune system was evaluated by a protein adsorption test. Finally, some hints on how to improve the synthesis of the nanohybrids - and therefore, their photodynamic activity - were provided by a mechanistic study of the grafting onto C60 of macroradicals released by cobalt end-capped polymers
Centre d'étude et de recherche sur les macromolécules (CERM)
Fonds de la Recherche Scientifique (Communauté française de Belgique) - F.R.S.-FNRS ; Politique Scientifique Fédérale (Belgique) = Belgian Federal Science Policy
Novel multifunctional nanohybrids based on fullerene and polyvinyl alcohol: synthesis and application to photodynamic therapy

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