Abstract
The functionalized PCCP backbone-based ligands L1-L6 with high activity and selectivity were prepared for ethylene tri-/tetramerization. Functionalized C-F bonds were found to contribute the reactivity when the asymmetric dialkylphosphine ligands exhibited a tunable selectivity towards C6/C8 fractions. Notably, the high-temperature tolerance (under 100 ℃) of the catalyst was enhanced due to the introduction of the C-F bonds. Modified ligand L6 exhibited a high activity of 2119 kg/g Cr/h with a high combined (1-C6+1-C8) selectivity of 90.25 % at 100 ℃ and under an ethylene pressure of 5.0 MPa. The high-temperature resistance of such catalysts is essential in preventing pipeline clogging and is promising for industrialization. Density functional theory (DFT) calculations showed that lower energy barriers would be consumed due to the introduction of C-F bonds, resulting in a tendency to trimerization.
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