Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 105, Issue 34, Pages 12123-12127Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0802147105
Keywords
alkylidene; heterogeneous catalysis; metallacyclobutanes; solid state NMR
Categories
Funding
- Ministere de la Recherche et de l'Education
- Centre National de la Recherche Scientifique
- Ecole Superieure Chimie Physique Electronique de Lyon
- French Agence Nationale del la Recherche [ANR JC05_46372]
- National Science Foundation [CHE-0138495]
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Grafting of [W( NAr)(=CHtBu)(2,5-Me2NC4H2)(2)] on a silica partially clehydroxylated at 700 degrees C (SiO2-(700)) generates the corresponding monosiloxy complex [( SiO)W( NAr)(=CHtBu)(2,5-Me2NC4H2)] as the major species (approximate to 90%) along with [( SiO)W( NAr)(CH(2)tBu)(2,5-Me2NC4H2)(2)], according to mass balance analysis, IR, and NMR studies. This heterogeneous catalyst displays good activity and stability in the metathesis of propene. Very importantly, solid state NMR spectroscopy allows observation of the propagating alkylidene as well as stable metallacyclobutane intermediates. These species have the same reactivity as the initial surface complex [( SiO)W( NAr)(=CHtBu)(2,5-Me2NC4H2)], which shows that they are the key intermediates of alkene metathesis.
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