Abstract
A series of five one-component catalysts has been investigated: (η 3-C 8H 13)Ni(CH 3COCHCOCH 3) ( 1a), (η 3-C 8H 13)Ni(CF 3COCHCOCH 3) ( 1b), (η 3-C 8H 13)Ni(CF 3COCHCOCF 3) ( 1c), (PPh 3)C 6H 5Ni(PPh 2CHCOPh) ( 2) and (η 3-C 8H 13)Ni(PPh 2CH 2COO) ( 3). Their catalytic activity and selectivity in the oligomerization of small alkenes are discussed: 1 catalyzes the dimerization of but-1-ene to 80% linear octenes (turnover number at 75 °C for 1c: 0.2 s −1); 2 and 3 oligomerize ethylene to 99% linear α-olefins in the C 4 - C 20 range (turnover number at 75 °C for 3: 0.8 s −1). Compound 3 is a model for the catalyst system employed in the SHELL-Higher-Olefins-Process. K-edge XAS and ESCA spectra of 1– 3 show square-planar d 8-configuration in all cases and allow an inverse volcano-type correlation between ESCA chemical shifts and catalytic activity and selectivity. A mechanistic explanation with regard to the insertion step and the chain growth terminating β-H elimination reaction is undertaken.
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