Sammendrag
A significant goal for the development of sustainable chemistry and for enhancement of the economic benefits of the Norwegian natural gas reserves is the direct catalytic functionalization of light alkanes, such as methane, to oxygenates, such as methanol. While homogeneous catalytic systems based on Pt(II) exist, unsuitable activities, co-reagents, or reaction conditions prevent the industrial implementation of these catalytic processes. In order to develop new alkane activation and functionalization systems as an alternative to the (diimine)Pt systems which have been investigated by the Oslo group over the past 10 years, a program for the discovery of new Au-based alkane activation and functionalization catalysts has been initiated. Isoelectronic analogies and literature precedent strongly suggests that Au-complexes may indeed provide robust alkane functionalization catalysts. As with our earlier efforts on the Pt(II) chemistry, both synthetic and computational methodologies are utilized in this program. Our initial focus as been on N-ligated Au(III) complexes, and a series of new Au(III) complexes has been synthesized and completely characterized. In particular, Au(III) systems ligated with β-diketiminates and bipyridines have shown a rich chemistry in synthesis and modeling experiments, respectively. This presentation will provide details of these experiments and their relevance to the discovery of new Au-based C-H bond activating species.