Synthetic and Mechanistic Studies on the Homogenous Catalysis of Transition Metal Complexes (Chemistry)

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This research on transition metals for homogeneous catalysis will be supported by the Organic and Macromolecular Chemistry Program. The development of new synthetic tools based on catalytic systems has the potential to provide more economic, pollution-free methods for the synthesis of the complex materials for industry and agriculture. The ultimate goal is to design and develop multi-functional multicatalyst systems which will permit multi-step synthesis in one-pot in a highly organized manner. This project includes three sub-projects: (i) mechanistic study of mixed metal catalyst systems focusing on the mechanism of CoRh(CO)7 catalysis including high pressure FT-IR study on the behavior of this unique mixed-metal complex regarding the hydroformylation-amido-carbonylation process; (ii) elucidation of the mechanism of amidocarbonylation by stereochemical approach which will resolve a historical mystery, i.e., water cleaves acylcobalt bond selectively in the presence of high pressure hydrogen, by designing bicyclic intermediates bearing strict steric requirements that can unambiguously distinguish among the possible mechanisms proposed; (iii) chelation-directed regio- and stereocontrol in carbonylations, which will systematically introduce chelation control, for the first time, to carbonylations and apply it to the catalytic asymmetric synthesis.