期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 105, 期 34, 页码 12123-12127出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0802147105
关键词
alkylidene; heterogeneous catalysis; metallacyclobutanes; solid state NMR
资金
- 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]
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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