Elucidating the Mechanism of Ruthenium-Complex catalyzed Olefin Metathesis Reactions

Olefin metathesis employing ruthenium or molybdenum-based catalyst complexes is one of the most important synthetic methods for the preparation of substituted olefins. From a mechanistic point of view, this organic transformation involves numerous transition metal-containing species, generated during the olefin metathesis reaction. Three major phases of the olefin metathesis reaction can be distinguished: a) the initiation reaction, i. e. the conversion of the precatalyst into catalytically active species; b) the catalytic cycle, involving the conversion of organic substrates into the respective olefin metathesis products, which include different active transition metal complexes as well as possible off-cycle resting states; and c) the decomposition of the catalytically active species, be it the intrinsic decomposition of the catalytically active species or decomposition reactions induced by adventitious impurities in the reaction mixture.

We are interested in understanding the mechanism of this reaction and how those three stages of olefin metathesis influence the outcome the organic transformation. Based on this knowledge, we finally aim to synthesize improved catalysts for more efficient chemical transformations. Experimental kinetic studies using different spectroscopic techniques with a focus on UV/Vis-spectroscopy and using stopped-flow methods for the experimental determination of fast reactions form the base of our scientific studies, which are complemented with theoretical methods and specialized experimental techniques in collaboration with other research groups.

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The Initiation Reaction of Hoveyda–Grubbs Complexes with Ethene, N. Peschek, K.-J. Wannowius, H. Plenio, ACS Catal. 2019, 9, 951-959.