From Bonding and Structure to Mechanism and Catalytic Reactivity of Late Transition Metal Complexes

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One of the grand challenges in chemistry involves the discovery of mild, economically-viable processes for the conversion of readily-available raw materials into higher value products. Further functionalization of these value-added products can allows the manufacturing of life-saving pharmaceuticals and materials that enhance everyday life. As pressures grow to minimize waste production, there is a significant need to develop new, “greener” reaction methods. Catalytic reactions are particularly desirable, since by definition they use a small amount of catalyst that is regenerated at the conclusion of the reaction, and in principle can be reused. Transition metal catalysts are increasingly used in the industrial synthesis of pharmaceuticals, materials and fine chemicals, yet the factors that control catalyst activity and the individual steps of a catalytic reaction are often poorly understood. This lack of catalytic insight greatly impedes the ability for designed (as opposed to serendipitous) reaction discovery. The goal of my research program is to discover fundamental reactivity of transition metal catalysts and to use this knowledge to develop useful and efficient reactions of broad utility in the synthesis of chemicals with interesting biological or materials properties. This proposal describes three areas of research focused on translating fundamental knowledge of metal-ligand bonding into synthetically useful catalytic reactions. During the five year window for this proposal, we will synthesize, isolate and characterize numerous ligands and metal complexes. We will explore the relationship between electron structure and reactivity. We will use the insight from these studies to guide our design of new reactions, both catalytic and stoichiometric. We will explore the mechanisms of these reactions as a way to improve reaction conditions and ligand design, as well as a means to uncover new reactivity. Ultimately, we will demonstrate the utility of these reactions in the synthesis of bioactive targets. Overall, the proposed studies will provide the basis for us to achieve several long-standing goals in organometallic chemistry. This unique research program provides excellent training for HQP at all levels. Our results will be of interest to a broad range of chemical industries, particularly fine chemicals, pharmaceuticals and agrochemicals.