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Atomistic Description of Reaction Intermediates for Supported Metathesis Catalysts Enabled by DNP SENS
Author(s) -
Ong TaChung,
Liao WeiChih,
Mougel Victor,
Gajan David,
Lesage Anne,
Emsley Lyndon,
Copéret Christophe
Publication year - 2016
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201510821
Subject(s) - alkene , metathesis , cycloaddition , catalysis , chemistry , salt metathesis reaction , heterogeneous catalysis , reaction intermediate , combinatorial chemistry , photochemistry , organic chemistry , polymerization , polymer
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.