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化学进展 2019, Vol. 31 Issue (12): 1737-1748 DOI: 10.7536/PC190442 前一篇   后一篇

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同核双金属烯烃聚合催化剂

袁世芳1,2,**(), 闫艺2   

  1. 1. 山西大学应用化学研究所 太原 030006
    2. 山西大学化学化工学院 太原 030006
  • 收稿日期:2019-04-29 出版日期:2019-12-15 发布日期:2019-10-15
  • 通讯作者: 袁世芳
  • 基金资助:
    国家自然科学基金项目(21101101)
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Homonuclear Bimetallic Complex Catalysts for Olefin Polymerization

Shifang Yuan1,2,**(), Yi Yan2   

  1. 1. Institute of Applied Chemistry, Shanxi University, Taiyuan 030006, China
    2. School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, China
  • Received:2019-04-29 Online:2019-12-15 Published:2019-10-15
  • Contact: Shifang Yuan
  • About author:
    ** E-mail:
  • Supported by:
    National Natural Science Foundation of China(21101101)

与单核金属配合物催化剂相比,双核金属配合物催化剂所具的双金属活性中心对烯烃聚合催化活性和所得聚合物的性能(包括聚合物微结构、分子量大小和分子量分布)产生了重要影响。本文综述了双金属配合物作为均相催化剂催化乙烯聚合及共聚合的最新研究,归纳思路包括不同的金属类型,即基于前过渡金属(Zr, Ti, Hf) 和后过渡金属(Ni, Fe, Co) 的双核金属组合; 不同的配体化合物,即CGC配体、酚氧亚胺配体、氮杂环胺配体、α-二亚胺和亚胺吡啶配体等。这些研究表明,前过渡金属催化剂不仅解决了乙烯自聚还实现了乙烯与α-烯烃共聚;后过渡金属催化剂高效催化乙烯自聚合,其中铁和钴催化剂获得高度线性聚乙烯,镍催化剂则产生多支链聚乙烯。

关键词： 双金属配合物, 同核, 催化活性, 聚烯烃微结构, 特征

In comparison with mononuclear metal catalysts in olefin polymerization, bimetallic catalysts having two active species significantly affect catalytic activities and properties of resulting polyolefins(such as microstructure of polymer, molecular weight and polydispersity). Herein we highlight the recent progress of bimetallic catalysts in ethylene polymerization and co-polymerization, which have been illustrated through the differences of metals used either early transition metals(Zr, Ti, Hf) or late transition metals(Ni, Fe, Co), and the varieties of ligands including constrained-geometry catalyst(CGC), phenoxyimines, azaallyl, a-diimines as well as iminopyridines. On the basis of these results, the early-transition metal catalysts have achieved not only homo-polymerization of ethylene but also co-polymerization of ethylene with α-olefin, while the late transition metal catalysts catalyze efficiently polymerization of ethylene, resulting in highly linear polyethylene by iron and cobalt catalysts or higher branched polyethylenes by nickel catalysts.

Key words: bimetallic complex catalyst, homonuclear, catalytic activity, microstructure of polyolefin, characteristics
()
图1 双核钛和锆CGC金属配合物催化剂1和2[26,27,28,29,30,31,32,33,34,35]
Fig. 1 Dinuclear titanium and zirconium CGC metal complex catalysts 1 and 2[26,27,28,29,30,31,32,33,34,35]
图2 双核吡啶胺基铪金属配合物催化剂3和4[34,35,36,37,38]
Fig. 2 Binuclear pyridine amino hafnium metal complex catalysts 3 and 4[34,35,36,37,38]
图3 双核苯酚亚胺金属配合物催化剂5[38,39]
Fig. 3 Dinuclear phenol imine metal complex catalysts 5[38,39]
图4 双核钛配合物催化剂6和7[40]
Fig. 4 Dinuclear titanium complex catalysts 6 and 7[40]
图5 氮杂环双核锆金属配合物催化剂8~11[41,42,43,44]
Fig. 5 Nitrogen heterocyclic dinuclear zirconium metal complex catalysts 8~11[41,42,43,44]
图6 亚甲基桥联α-二亚胺双核镍预催化剂12a~12f[45,46,47,48,49,50,51,52,53,54,55,56,57]
Fig. 6 Methylene-bridged bis(α-diimine) dinickel pre-catalysts 12a~12f[45,46,47,48,49,50,51,52,53,54,55,56,57]
图7 双α-二亚胺双核镍预催化剂13、14[58,59]
Fig. 7 Bis(α-diimine) dinuclear nickel pre-catalysts 13,14[58,59]
图8 α-二亚胺双核镍预催化剂15和16[60,61]
Fig. 8 Bis(α-diimine) dinuclear nickel pre-catalysts 15 and 16[60,61]
图9 双α-二亚胺双核镍预催化剂17和18[62,63]
Fig. 9 Bis(α-diimine) dinuclear nickel pre-catalysts 17 and 18[62,63]
图10 双α-二亚胺双核镍预催化剂19~21[64,65]
Fig. 10 Bis(α-diimine) dinuclear nickel pre-catalysts 19~21[64,65]
图11 双金属镍(Ⅱ)预催化剂22、23[66,67,68]
Fig. 11 Bimetallic nickel(Ⅱ) precatalysts 22,23[66,67,68]
图12 含有苯氧基亚胺的双核镍配合物24[71]
Fig. 12 Phenoxyimine-containing binuclear nickel complexes 24[71]
图13 双核苯氧亚胺-镍配合物25~27[72,73,74,75,76]
Fig. 13 Binuclear phenoxyimine-nickel complexes 25~27[72,73,74,75,76]
图14 双核苯氧亚胺-镍配合物28~30[72,73,74,75,76]
Fig. 14 Binuclear phenoxyimine-nickel complexes 28~30[72,73,74,75,76]
图15 双核镍配合物31带有刚性连接体[72,73,74,75,76]
Fig. 15 Binuclear nickel complexes 31 bearing rigid linkers[72,73,74,75,76]
图16 大环双金属镍配合物32和33[77,78]
Fig. 16 Macrocyclic bimetallic nickel complexes 32,33[77,78]
图17 双金属(Fe和Co)配合物34~36[79,80,81]
Fig. 17 Bimetallic(Fe and Co) complexes 34~36[79,80,81]
图18 双金属Fe和Co配合物37和38[82,83,84]
Fig. 18 Bimetallic(Fe and Co) complexes 37,38[82,83,84]
图19 双金属(Fe和Co)配合物39和40[85,86,87]
Fig. 19 Bimetallic(Fe and Co) complexes 39,40[85,86,87]
图20 亚胺双金属配合物催化剂41[88]
Fig. 20 Imine bimetallic complex catalysts 41[88]
图21 亚胺双金属配合物催化剂42[89,90]
Fig. 21 Imine bimetallic complex catalysts 42[89,90]
图22 亚胺双金属配合物催化剂43~45[93,94,95]
Fig. 22 Imine bimetallic complex catalysts 43~45[93,94,95]
图23 亚胺双金属配合物催化剂46[96]
Fig. 23 Imine bimetallic complex catalysts 46[96]
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摘要

同核双金属烯烃聚合催化剂