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Synthèse et caractérisation de nouveaux amorceurs basés sur des complexes de métaux de transition bivalents : vers la synthèse de polyesters stéréoréguliers par polymérisation par ouverture de cycle

Abstract : A large part of the plastic materials produced every year in the world are disposed in landfill, representing a serious menace for the environment. Since several decades, industrial and academic scientists are interested in the synthesis of biodegradable polyesters via the ring opening polymerization of biobased cyclic esters like lactide. Despite a large number of initiators described in the literature, several metals remains not well studied. The goals of this thesis were to synthetize and study the polymerization properties of new iron and cobalt (II) initiators with a trigonal bipyramidal geometry. The different initiators were active at room temperature and polymers with a large variety of tacticity were obtained depending on the steric hindrance of the pro-ligand and the metallic center used, with very good activity and in a controlled manner. Highly isotactic-rich PLA (Pm = 0,86-0,91) were obtained with iron (II) based initiators for the first time. Moreover, cobalt (II) initiators gave isotactic and heterotactic-rich PLA with moderate selectivity, constituting two new cases of stereoselectivity switch. These initiators constitute a good starting point for the development of new productive initiators for the stereoselective polymerization of rac-lactide based on non-toxic and abundant metals and easily accessible pro-ligands.
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Paul Marin. Synthèse et caractérisation de nouveaux amorceurs basés sur des complexes de métaux de transition bivalents : vers la synthèse de polyesters stéréoréguliers par polymérisation par ouverture de cycle. Polymères. Université Pierre et Marie Curie - Paris VI, 2016. Français. ⟨NNT : 2016PA066703⟩. ⟨tel-01954806⟩

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