Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 55, Issue 15, Pages 4743-4747Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201510821
Keywords
DFT calculation; dynamic nuclear polarization; metathesis; solid-state NMR; surface chemistry
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Funding
- SNF [200020_149704]
- ERC Advanced Grant [320860]
- Swiss National Science Foundation (SNF) [200020_149704] Funding Source: Swiss National Science Foundation (SNF)
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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.
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