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Elaboration de nouveaux complexes de coordination d'éléments de transititon d et f : synthèses, structures, propriétés magnétiques et optiques

Abstract : Coordination chemistry of transition metals gives an access to numerous molecular magnetic materials that exhibit varied properties. During this work, several ligands with intrinsic properties have been chosen and their chemistry has been developed in order to get specific magnetic behavior.
Solvothermal syntheses allowed the characterization of several complexes based on macrocycles. Two dinuclear CoII and FeIII complexes were isolated. Their molecular structures are built from metal ions located like in a "sandwich" between two calixarenes units. These complexes considered as molecular starting blocks were used for the synthesis of clusters with higher nuclearity. An original complex associating six CoII ions has been then isolated.
The complexation of Schiff base ligands resulting from the condensation of the acetylacetone with various amino acids has been performed. From one of these original ligands, an almost perfect triangular trinuclear CuII complex has been then isolated and fully characterized. Ab initio calculations have been carried out in order to explain its magnetic properties.
Finally, the complexation of β-diketone based ligands with various metals was explored. It has been then possible to control the nuclearity of molecular buildings block. The use of a preformed brick (cubane type) gave an access to a heptanuclear NiII complex. This latter presents the characteristics of a single molecule magnet. The last stage of these researches was to modify the steric effect of these β-diketone ligands in order to control the final cluster size. Three families of polynuclear 4f complexes (Ln5, Ln8 and Ln9) were obtained. Structural, magnetic studies and detailed analysis of the spectroscopic characteristics of these europium(III) complexes were achieved. A completely original work has been carried out on Y9 clusters doped with Eu (Y9-xEux) by linking molecular structures with luminescence properties.
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Submitted on : Monday, March 17, 2008 - 5:53:16 PM
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Sarah Petit. Elaboration de nouveaux complexes de coordination d'éléments de transititon d et f : synthèses, structures, propriétés magnétiques et optiques. Chimie. Université Claude Bernard - Lyon I, 2007. Français. ⟨tel-00264233⟩

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