Significant advances have been made in the last 15 years in the development of catalysts for the hydrogenation of polar molecules, based on a design principle of metal-ligand cooperativity. This seminar describes mechanistic studies of CNN- and PNN-pincer-ruthenium catalysts for ester hydrogenation, which feature dialkylamino groups on the pincer ligand. Both CNN- and PNN-based precatalysts undergo an unexpected transformation, resulting in the release of ethane or propane and the formation of five-coordinate ruthenium(0) species containing a nascent imine functional group. The ruthenium(0)-imine derivatives catalyze ester hydrogenation either at either the same or a higher rate as their ruthenium(II)-amine precursors. The PNN-ruthenium(0) species reacts reversibly with two equivalents of hydrogen at room temperature to generate a ruthenium(II)-dihydride species, where the imine functionality has been hydrogenated to produce a protic amine. These results have potentially broad implications for our understanding of the mechanisms of hydrogenation and dehydrogenation reactions catalyzed by ruthenium-pincer complexes.

Uncovering the identity of the active species in ruthenium-catalyzed ester hydrogenation

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.