Iron and Zinc Complexes of Bulky Bis-Imidazole Ligands: Enzyme Mimicry and Ligand-Centered Redox Activity

Abstract

The research described in this thesis is directed to the development of cheap and non-toxic iron-based homogeneous catalysts, using enzyme models and redox non-innocent ligands. Inspired by nature, the first approach focuses on the synthesis of structural models of the active site of non-heme iron enzymes with the intention to mimic the enzymes’ catalytic properties. In the second approach, redox non-innocent ligands are used to overcome one of the major differences between noble and base metals. Noble metals generally prefer to undergo two-electron changes, matching bond making and breaking events. In contrast, first-row transition metals generally undergo one-electron changes that might induce unselective radical reactions. Redox non-innocent ligands that can function as an electron reservoir allow two-electron changes on base metal complexes.