Mechanisms of Homogeneous Hydrocarbon Activation and Functionalization by Transition Metal Complexes

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In this project in the Inorganic, Bioinorganic, and Organometallic Program of the Chemistry Division, Flood will continue his studies of how transition metal complexes may form and break C-H, C-C, and C-O bonds in homogeneous solution. The major emphasis will be careful and fundamental mechanistic investigations, which should be generally applicable to organometallic chemistry. These results should be useful in the rational design of industrial catalysts for the transformation of hydrocarbons into useful compounds. Synthetic and mechanistic studies of the reactions of hydrocarbons in the coordination sphere of soluble complexes of transition metals will be pursued. The work will focus on intermolecular and intramolecular C-H activations, reversible alkene insertions into metal-carbon bonds, and alpha-eliminations and insertions at metal-bound carbon and oxygen centers. Metal, oxidation state, steric bulk and electronic effects of ancillary ligands, alkyl group structure, charge, chelate ring size, and other factors will be investigated. The possibility of stabilizing higher oxidation states and oxo-containing species will be tested by use of amine-ligated organometallic species rather than more conventional ligands. Targeted systems include Os, Ir, and Pt complexes. In all cases a thorough investigation of mechanisms will be conducted through a variety of probes.