Studies of the Activation and Functionalization of Hydrocarbons at Multinuclear Metal Sites in Transition Metal-Gold Complexes

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In this project funded by the Chemical Synthesis Program of the Chemistry Division, Professor Richard D. Adams of the Department of Chemistry and Biochemistry at the University of South Carolina is developing new methods for the synthesis of bimetallic transition metal cluster complexes containing gold to be used to create new catalysts for the transformations and reforming of hydrocarbons. Simple hydrocarbons such as methane and ethane are now available from today's abundant supplies of natural gas. There is a great need to develop catalysts to transform these resources efficiently into higher value commodity chemicals. Studies will be focused on the development of new catalysts for selective oxidation reactions that will convert simple hydrocarbons into oxygenated compounds, such as alcohols and carboxylic acids, via environmentally-friendly chemical processes. Precious metal elements, such as ruthenium, rhodium, rhenium, iridium, and platinum will be studied because of their well-known ability to activate the CH bonds of hydrocarbons. Gold will be chemically incorporated into the new catalysts because of its recently discovered ability to active oxygen and transfer it to carbon atoms. Broader impacts include the development of new processes for the conversion of natural gas and related resources into valuable chemicals for use as additives to produce higher octane fuels and for feedstocks for the synthesis of new polymers and materials. Graduate and undergraduate students are trained in the latest methods of scientific inquiry and analysis as preparation for careers in academia or the chemical industry. Hydrocarbyl containing gold-transtion metal clusters are prepared by the reaction of organogold compounds with metal carbonyl cluster complexes of the precious transition metals. These heterometallic cluster complexes are converted into bi- and multimetallic nanoparticles for use as nanocatalysts for the selective oxidation of hydrocarbons. The controlled addition of oxygen to the carbon atoms is central understanding the nature of metal-catalyzed selective oxidation reactions. Mechanistic studies are carried out and focus on understanding the nature of transformations of the CH bonds of the hydrocarbon by complexes containing two or more metal atoms. These studies include investigations of the formation of C - O bonds. The complexes and catalysts are studied by X-ray diffraction and high resolution transmission electron microscopy.