Shvo-Type Metal-Ligand Cooperative Catalysts: Tethered eta(5)-Oxocyclohexadienyl Ruthenium Complexes
Résumé
Diverse synthetic routes of tethered eta(5)-oxocyclo-hexadienyl ruthenium complexes, which are the extended version of the eta(4)-cyclopentadienone Shvo-type active catalyst, are described and their reactivity studies are reported. An original dimeric eta(5)-oxocyclohexadienyl compound has been isolated and its solid-state structure was established by X-ray analysis. DFT computational data suggested that this dimeric compound is prone to generate a coordinatively unsaturated mononuclear Lewis acid metal complex bearing a Lewis basic pi-coordinated eta(5)-oxocyclohexadienyl Iigand. Preliminary studies in (transfer)-hydrogenation of acetophenone confirmed that the dimeric eta(5)-oxocyclohexadienyl complex behaves as a bifunctional catalyst with metal-ligand cooperativity. Promising results were obtained under base-free conditions using dihydrogen, iPrOH, and formic acid as hydrogen highlighting the robustness and stability of the catalyst and opening perspectives donors, the latter being active in water, hence toward sustainable catalytic transformations.
Domaines
Chimie| Origine | Fichiers produits par l'(les) auteur(s) |
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