Synthesis of L2Ni(ORF)2 (RF = C(CF3)3) Complexes and Their Reactivity in Ethylene Oligomerization

被引:3
作者
Petit, Julien [1 ,2 ]
Saffon-Merceron, Nathalie [3 ]
Magna, Lionel [2 ]
Mezailles, Nicolas [1 ]
机构
[1] Univ Paul Sabatier, UMR 5069 CNRS, Lab Heterochimie Fondamentale & Appliquee, F-31062 Toulouse, France
[2] IFP Energies Nouvelles Rond Pint Iechangeur Sola, BP3, F-69360 Solaize, France
[3] Univ Paul Sabatier, Inst Chim Toulouse ICT FR2599, F-31062 Toulouse, France
关键词
NICKEL-COMPLEXES; TRIMERIZATION REACTION; ALPHA-OLEFINS; DIMERIZATION; OXIDATION; MECHANISM; CATALYSIS; ALKOXIDE; LIGANDS; TETRAFLUOROETHYLENE;
D O I
10.1021/acs.organomet.1c00575
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
A family of L2Ni(ORF)(2) (L-2: (Cy3PO)(2) 4, dcpmS 5, dppf 9, bipyMe(2) 10; R-F = C(CF3)(3)) complexes is synthesized via selective substitution of 2 equiv of (DME)NaORF from homoleptic [Ni(ORF)(4)][Na(DME)](2) complex 1, all characterized by F-19 and H-1 NMR and SCXRD analyses as well as elemental analyses. These L2Ni(ORF)(2) precursors, activated by 2 equiv of PhF -> Al(ORF)(3), were active in ethylene oligomerization with selectivity toward butenes up to 97% and activities ranging from 10 to 50 kg(C2H4).g(Ni).h(-1). Mechanistic investigations, involving experiments with C2H4/C2D4 (1/1) coupled with GC-MS analysis, revealed the formation of a Ni-H fragment in the catalytic process. The L2Ni(ORF)(2)/2PhF -> Al(ORF)(3) catalytic system thus dimerizes ethylene through a Cossee-Arlman mechanism.
引用
收藏
页码:4133 / 4142
页数:10
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