title: Atomistic Description of Reaction Intermediates for Supported Metathesis Catalysts Enabled by DNP SENS.
abstract: Obtaining detailed structural information of reaction intermediates remains a key challenge in heterogeneous catalysis because of the amorphous nature of the support and/or the support interface that prohibits the use of diffraction-based techniques. Combining isotopic labeling and dynamic nuclear polarization (DNP) increases the sensitivity of surface enhanced solid-state NMR spectroscopy (SENS) towards surface species in heterogeneous alkene metathesis catalysts; this in turn allows direct determination of the bond connectivity and measurement of the carbon-carbon bond distance in metallacycles, which are the cycloaddition intermediates in the alkene metathesis catalytic cycle. Furthermore, this approach makes possible the understanding of the slow initiation and deactivation steps in these heterogeneous metathesis catalysts.
authors.affiliation: Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1-5, 8093, Zürich, Switzerland.
authors.forename: Ta-Chung
authors.identifier: http://orcid.org/0000-0001-9463-4765
authors.initials: TC
authors.lastname: Ong
authors.affiliation: Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1-5, 8093, Zürich, Switzerland.
authors.forename: Wei-Chih
authors.initials: WC
authors.lastname: Liao
authors.affiliation: Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1-5, 8093, Zürich, Switzerland.
authors.forename: Victor
authors.initials: V
authors.lastname: Mougel
authors.affiliation: Centre de RMN à Très Hauts Champs, Institut de Sciences Analytiques (CNRS/ENS Lyon/UCB Lyon 1), Université de Lyon, 69100, Villeurbanne, France.
authors.forename: David
authors.initials: D
authors.lastname: Gajan
authors.affiliation: Centre de RMN à Très Hauts Champs, Institut de Sciences Analytiques (CNRS/ENS Lyon/UCB Lyon 1), Université de Lyon, 69100, Villeurbanne, France.
authors.forename: Anne
authors.initials: A
authors.lastname: Lesage
authors.affiliation: Institut des Sciences et Ingénierie Chimiques, École Polytechnique Fédérale de Lausanne (EPFL), 1015, Lausanne, Switzerland.
authors.forename: Lyndon
authors.initials: L
authors.lastname: Emsley
authors.affiliation: Department of Chemistry and Applied Biosciences, ETH Zürich, Vladimir-Prelog-Weg 1-5, 8093, Zürich, Switzerland. ccoperet@inorg.chem.ethz.ch.
authors.forename: Christophe
authors.initials: C
authors.lastname: Copéret
keywords: DFT calculation; dynamic nuclear polarization; metathesis; solid-state NMR; surface chemistry