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Synthèse de complexes inspirés des formiate déshydrogénases à Mo/W : application à la catalyse moléculaire de la réduction du CO2

Abstract : In the context of global warming, the development of new sources of energy, clean and sustainable, is a key challenge of our society. The reduction of CO2 could allow the storage of renewable energies and offer an answer to the dramatic increase of CO2 in the atmosphere. Development of molecular catalysts offers the possibility of studying the structure-reactivity relationships. However, the library of existing homogeneous catalysts in the literature is quite limited. In order to find new potential catalysts, we decided to take inspiration from the active site of formate dehydrogenases (FDH). The synthesis of molecules mimicking this active site is an interesting challenge. In this thesis, we described the synthesis of two ligands inspired from the molybdopterin (chapter I). The synthesis of CoCp(dithiolène) complexes allows us to better characterize these ligands (chapter II). Moreover, the observation of the reactivity of these ligands allows us to understand their behaviour during electrocatalysis. The [MoO(dithiolene)2]2- complexes obtained from the bio-inspired ligands are,so far, the best mimics of the active site of FDH in the literature (chapter III). In this chapter, the generalization of synthetic procedure was also explored. Finally, [Ni(dithiolene)2]- synthesize from the bio-inspired ligands are the first dithiolene complexes able to reduce CO2 (chapter IV). They are among the few non-nobles metal complexes catalyzing the reduction of CO2 into formate.
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Thibault Fogeron. Synthèse de complexes inspirés des formiate déshydrogénases à Mo/W : application à la catalyse moléculaire de la réduction du CO2. Catalyse. Sorbonne Université, 2018. Français. ⟨NNT : 2018SORUS132⟩. ⟨tel-02922949⟩

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