Synthetic and Mechanistic Studies of High Valent Organotransition Metal Compounds

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In this project supported by the Inorganic, Bioinorganic and Organometallic Chemistry Program, John E. Bercaw of the Calif- ornia Institute of Technology will investigate the synthesis and properties of new types of dioxygen-compatible transition metal compounds which may be capable of selectively oxidizing hydrocarbons. The eventual aim of this research is to develop a useful catalytic method for converting hydrocarbons from coal, petroleum or natural gas sources to alcohols (in particular, methane to methanol), which may be more readily transportable and useful energy sources or chemical feedstocks. The project has two thrusts: (1) synthesis of new soluble oxo or peroxo derivatives of ruthenium, which could smoothly convert olefins to epoxides or carbonyl compounds and hydro- carbons to alcohols, and (2) mechanistic studies which involve carbon-oxygen bond formation or carbon-oxygen bond cleavage at hafnium and tantalum. The latter project would lead to an understanding of the kinetic and thermodynamic factors influencing carbon-oxygen and hydrogen-oxygen bond formation at transition metal centers which would aid in design of the catalysts in part (1). Related studies are also proposed which could provide some model compounds and transformations of relevance to catalytic hydrodesulfurization chemistry.