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Mechanistic investigations of the ethylene tetramerisation reaction. 2005

Matthew J Overett, and Kevin Blann, and Annette Bollmann, and John T Dixon, and Daleen Haasbroek, and Esna Killian, and Hulisani Maumela, and David S McGuinness, and David H Morgan
Sasol Technology (Pty) Ltd, R&D Division, 1 Klasie Havenga Road, Sasolburg 1947, South Africa. Matthew.Overett@Sasol.com

The unprecedented selective tetramerisation of ethylene to 1-octene was recently reported. In the present study various mechanistic aspects of this novel transformation were investigated. The unusually high 1-octene selectivity in chromium-catalyzed ethylene tetramerisation reactions is caused by the unique extended metallacyclic mechanism in operation. Both 1-octene and higher 1-alkenes are formed by further ethylene insertion into a metallacycloheptane intermediate, whereas 1-hexene is formed by elimination from this species as in other reported trimerisation reactions. This is supported by deuterium labeling studies, analysis of the molar distribution of 1-alkene products, and identification of secondary co-oligomerization reaction products. In addition, the formation of two C6 cyclic products, methylenecyclopentane and methylcyclopentane, is discussed, and a bimetallic disproportionation mechanism to account for the available data is proposed.

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