Ethylene oligomerization using quinoline-imine nickel(II) complex immobilized in fluorotetrasilicic mica interlayer by one-pot preparation method

Ethylene oligomerization using quinoline-imine nickel(II) complex immobilized in fluorotetrasilicic mica interlayer by one-pot preparation method
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DOI:
10.1016/j.molcata.2016.10.005
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发表时间:
2016-12
影响因子:
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通讯作者:
H. Yamanaka;Kazuhiro Yamamoto;Tsutomu Sakuragi;Masa–aki Ohshima;S. Nagashima;H. Kurokawa;H. Miura
H. Yamanaka;Kazuhiro Yamamoto;Tsutomu Sakuragi;Masa–aki Ohshima;S. Nagashima;H. Kurokawa;H. Miura
中科院分区:
化学2区
文献类型:
--
作者:
H. Yamanaka;Kazuhiro Yamamoto;Tsutomu Sakuragi;Masa–aki Ohshima;S. Nagashima;H. Kurokawa;H. Miura

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喹啉-亚胺镍(II)配合物通过镍离子交换的氟四云母(Ni 2 +-云母)与相应的喹啉和苯胺衍生物的反应通过一锅法合成固定在氟四云母夹层中。在用助催化剂(Et 3Al、iBu 3Al或Et 2AlCl)活化所制备的预催化剂之后,其显示出对于乙烯低聚的高催化活性,并形成具有4-20个碳数的低聚物。在40 °C和1.0 MPa下,在Et 3Al存在下,使用由Ni 2 +-云母、2-乙酰基喹啉和2,6-二甲基苯胺制备的预催化剂进行齐聚,获得最大活性(168 g-产物g-cat-1h-1)。在所有的低聚运行中,观察到一个长的诱导期,诱导时间显着依赖于助催化剂。这种诱导期可能是由催化剂前体的特征结构引起的。红外光谱和X射线衍射分析表明,在云母层间形成了镍配合物。
Quinoline-imine nickel (II) complexes were immobilized in fluorotetrasilicic mica interlayers by a one-pot synthesis through the reaction of a nickel ion-exchanged fluorotetrasilicic mica (Ni2+-mica) with the corresponding quinoline and aniline derivatives. After activation of the prepared precatalyst by a co-catalyst (Et3Al,iBu3Al, or Et2AlCl), it showed a high catalytic activity for the oligomerization of ethylene with the formation of oligomers having carbon numbers 4–20. The maximum activity (168 g-product g-cat−1h−1) was obtained by the oligomerization at 40 °C and 1.0 MPa in the presence of Et3Al using the precatalyst prepared from Ni2+-mica, 2-acetylquinoline, and 2, 6-dimethylaniline. In all the oligomerization runs, a long induction period was observed, and the induction time significantly depended on the co-catalyst. This induction period might be caused by the characteristic structure of the precatalysts. The FT-IR and XRD spectra of the precatalysts indicated the formation of the intended nickel complexes in the mica interlayer.