期刊
ORGANOMETALLICS
卷 27, 期 16, 页码 4238-4247出版社
AMER CHEMICAL SOC
DOI: 10.1021/om800398e
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资金
- Australian Research Council
The mechanism of ethylene oligomerization with chromium(III) complexes of bis(carbene)pyridine ligands in combination with MAO has been investigated. Oligomerization with mixtures of CH2CH2/ CD2CD2, reveals that this system produces alpha-olefins via an extended metallacycle mechanism. Deviation form a Schulz-Flory distribution has been explained on the basis of less favorable product release at the early stages of metallacycle growth (Cr-C-4 (+/- Cr-C-6)). Significant amounts of branched olefins (methylidenes) and linear internal olefins are produced at the high catalyst loadings employed in this study, and these result from secondary incorporation of alpha-olefins into the metallacycle mechanism. Changing the ligand (CNC)-N-Lambda-C-Lambda coordination mode in any way resulted in a sharp loss of activity. In the case of bidentate carbene-pyridine and carbene-thiophene ligands, this is due to a change in the mechanism from metallacycle to linear chain growth. Thus, only those catalysts which support a metallacycle mechanism promote oligomerization with high activity.
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