Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 14, Issue 36, Pages 11565-11572Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.200801584
Keywords
catalysis; decomposition; kinetics; olefin metathesis; ruthenium
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Funding
- NSERC of Canada
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The four-coordinate ruthenium phosphonium alkylidenes 1-Cy and 1-iPr, differing in the substituent on the phosphorus center. were observed to decompose thermally in the presence of 1,1-dichloroethylene to produce [H3CPR3][Cl]. The Major ruthenium-containing product was a trichloro-bridged ruthenium dimer that incorporates the elements of the 1,1-dichloro-ethylene as a dichlorocarbene ligand and a styrenic vinyl group on the supporting NHC ligand. Spectroscopic, kinetic, and deuterium-labeling experiments probed the mechanism of this process, which involves a rate-limiting C-H activation of an NHC mesityl ortho methyl group. These studies provide insight into intrinsic decomposition processes of active Grubbs type olefin metathesis catalysts, pointing, the way to new catalyst design directions.
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