New Gold Catalysts for the Activation and Functionalization of Alkanes

Since 1995, a series of projects involving primarily the group of Prof. Mats Tilset at the University of Olso and scientists from the Department of Hydrocarbon Process Chemistry at SINTEF Materials and Chemistry have lead to the discovery, development and understanding of a unique class of Pt cations capable of efficiently activating the C-H bonds of methane. Despite this breakthrough and continued efforts by groups in both Oslo and elsewhere, development of a catalytic transformation of methane to metha nol based on these Pt species has not yet occured. In order to expand the range of possibilities for a selective catalytic oxidation of methane, we propose a program for the development of new class of alkane C-H bond activation and functionalization com plexes based on gold. Catalytic functionalization of methane involving gold is actually already known, but the conditions are far from industrially relevant. Furthermore, it is unknown whether the active species in the catalysis is Au(I) or Au(III). We propose an integrated project involving both experimental and theoretical modelling activities to discover well-described Au complexes capable of activating and functionalizing the C-H bonds of light alkanes. This combined experimental and theoretical ap proach was used with extreme success in the development of the original Pt chemistry. We aim to synthesize a range of Au(I) and Au(III) methyl and phenyl complexes, explore their ability to activate C-H bonds, determine the mechanism of activation, and p robe the catalytic activity of the most promising of these species. The theoretical modelling activities will be integrated in the experimental approach to guide the selection of the most promising species and provide a theoretical understanding of the e xperimentally determined mechanisms. The project will educate two Ph. D. students, one in the experimental work and one in the theoretical work, and one post-doctoral student. Up to 15 publications are expected.