Journal
TOPICS IN CATALYSIS
Volume 61, Issue 3-4, Pages 213-224Publisher
SPRINGER/PLENUM PUBLISHERS
DOI: 10.1007/s11244-018-0891-8
Keywords
Heterogeneous catalysis; Chromium amide; 1-Hexene; Trimerisation; Oligomerisation; Polymerisation
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Funding
- Engineering and Physical Sciences Research Council [1353008, 1355451] Funding Source: researchfish
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Sequential treatment of a previously-calcined solid oxide support (i.e. SiO2, gamma-Al2O3, or mixed SiO2-Al2O3) with solutions of Cr{N(SiMe3)(2)}(3) (0.71 wt% Cr) and a Lewis acidic alkyl aluminium-based co-catalyst (15 molar equivalents) affords initiator systems active for the oligomerisation and/or polymerisation of ethylene. The influence of the oxide support, calcination temperature, co-catalyst, and reaction diluent on both the productivity and selectivity of the immobilised chromium initiator systems have been investigated, with the best performing combination (SiO2-600, modified methyl aluminoxane-12 {MMAO-12}, heptane) producing a mixture of hexenes (61 wt%; 79% 1-hexene), and polyethylene (16 wt%) with an activity of 2403 g g(Cr) (-1) h(-1). The observed product distribution is rationalised by two competing processes: trimerisation via a supported metallacycle-based mechanism and polymerisation through a classical Cossee-Arlman chain-growth pathway. This is supported by the indirect observation of two distinct chromium environments at the surface of the oxide support by a solid-state Si-29 NMR spectroscopic study of the Cr{N(SiMe3)(2)}(x)/SiO2-600 pro-initiator.
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