Organometallic Cluster Chemistry: Higher Nuclearity Derivatives

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9414217 Shapley Univ. of Ill. Urbana-Champaign Dr. John R. Shapley, Univ. of Ill. Urbana-Champaign, is supported by the Inorganic, Bioinorganic, and Organometallic Chemistry Program of the Chemistry Division to develop the organometallic chemistry of intermediate sized transition metal carbonyl cluster compounds which contain six to twelve metal atoms. The specific systems to be studied include: (1) compounds which are related to a carbido heptarhenium cluster and which contain a methylene moiety; (2) hydrocarbon ligand derivatives of a decaruthenium cluster system which adopts a unique structure that apparently can 'reconstruct' in order to bind a hydrocarbon group; (3) compounds in which a heptarhenium cluster unit mimics the common cyclopentadienyl ligand in binding a metal complex fragment but engenders enhanced reactivity at the metal vertex; and (4) the process of carbon monoxide disproportionation on a hexaruthenium framework, a reaction that is a direct molecular analog of the surface Boudouard reaction and one that may be important for initiating the Fischer-Tropsch hydrocarbon synthesis process. Metals are used as catalysts in a number of important industrial chemical processes including the refining of petroleum. However, the details of how metal surfaces are able to carry out and facilitate chemical reactions is not yet clearly understood. This project focuses on a series of compounds which contain six to twelve metal atoms. These complexes are small enough to permit the details of their interactions with other species to be studied in great detail, but large enough to model metal surfaces. The species chosen for investigation represent particularly suitable models for the sites on roughened metal surfaces that are most active in breaking C-C, C-N, and C-O bonds. In addition to providing a basic understanding of metal mediated chemical reactions, new classes of organometallic cluster compounds, which themselves may show catalytic properties will be prepared.