Speiser Fredy, Braunstein Pierre, Saussine Lucien
Laboratoire de Chimie de Coordination (UMR 7513 CNRS), Université Louis Pasteur, 4 rue Blaise Pascal, F-67070 Strasbourg Cédex, France.
Inorg Chem. 2004 Jul 12;43(14):4234-40. doi: 10.1021/ic049921r.
The new dicationic dinuclear complexes [Ni(micro-Cl)(2)(N,OH)(2)]Cl(2) (11, N,OH = 2-(4,4-dimethyl-4,5-dihydrooxazol-2-yl)-propan-2-ol; 12, N,OH = 2-pyridin-2-yl-propan-2-ol) were prepared in good yields and evaluated as precatalyts in the oligomerization of ethylene, using MAO or AlEtCl(2) as cocatalyst. These paramagnetic complexes were characterized by single-crystal X-ray diffraction in the solid state and in solution with the help of the Evans method, which revealed agreement between the octahedral coordination spheres found in solution and in the solid state. The N donor atoms of each chelating ligand are in mutual cis position, and the OH donors are mutually trans situated. Selectivities for 1-butene within the C(4) fraction of 61% (11) and 58% (12) were observed in the presence of 200 equiv of MAO, but better turnover frequencies (28 300 (11) and 20 400 (12) mol of C(2)H(4)/(mol of Ni.h)) were obtained when 800 equiv of MAO was used. In the presence of 6 equiv of AlEtCl(2), the activities were considerably increased, up to 174 300 (11) and 97 100 (12) mol of C(2)H(4)/(mol of Ni.h), and the selectivity for C(4) olefins was 70% and 64%, respectively.
制备了新型双阳离子双核配合物[Ni(μ-Cl)₂(N,OH)₂]Cl₂(11,N,OH = 2-(4,4-二甲基-4,5-二氢恶唑-2-基)-丙-2-醇;12,N,OH = 2-吡啶-2-基-丙-2-醇),产率良好,并以MAO或AlEtCl₂作为助催化剂,评估其作为乙烯齐聚预催化剂的性能。这些顺磁性配合物通过固态和溶液中的单晶X射线衍射以及埃文斯方法进行表征,结果表明在溶液和固态中发现的八面体配位球之间具有一致性。每个螯合配体的N供体原子相互处于顺式位置,OH供体相互处于反式位置。在200当量的MAO存在下,在C₄馏分中观察到1-丁烯的选择性分别为61%(11)和58%(12),但当使用800当量的MAO时,可获得更好的周转频率(28300(11)和20400(12)mol C₂H₄/(mol Ni·h))。在6当量的AlEtCl₂存在下,活性显著提高,分别高达174300(11)和97100(12)mol C₂H₄/(mol Ni·h),并且对C₄烯烃的选择性分别为70%和64%。