Direct observation of reaction intermediates for a well defined heterogeneous alkene metathesis catalyst.
basic_science · Level V
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- Record sourced from PubMed, PMID 18723685.
- Also identified by DOI 10.1073/pnas.0802147105 and PMC identifier 2527876.
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Abstract
Grafting of [W([triple bond]NAr)(=CHtBu)(2,5-Me(2)NC(4)H(2))(2)] on a silica partially dehydroxylated at 700 degrees C (SiO(2- (700))) generates the corresponding monosiloxy complex [([triple bond]SiO)W([triple bond]NAr)(=CHtBu)(2,5-Me(2)NC(4)H(2))] as the major species (approximately 90%) along with [([triple bond]SiO)W([triple bond]NAr)(CH(2)tBu)(2,5-Me(2)NC(4)H(2))(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 [([triple bond]SiO)W([triple bond]NAr)(=CHtBu)(2,5-Me(2)NC(4)H(2))], which shows that they are the key intermediates of alkene metathesis.