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亚胺膦亚胺型稀土双烷基配合物对丁二烯1,2-选择性聚合

刘博1,2,李世辉2,李丹凤2,吕奎2,崔冬梅2*,孙广平1*   

  1. (1.吉林大学材料科学与工程学院，教育部汽车材料重点实验室 长春 130025;
    2.中国科学院长春应用化学研究所高分子物理和化学重点实验室 长春 130022)
  • 收稿日期:2012-09-27 修回日期:2012-10-16 出版日期:2012-12-10 发布日期:2012-12-10
  • 通讯作者: CUI Dongmei， professor; Tel:0431-85262774; Fax:0431-85262773; E-mail:dmcui@ciac.jl.cn; Research Interests：polymer physics and chemistry

Highly 1,2-Selective Polymerization of 1,3-Butadiene with Rare-earth Metal Bis(alkyl)s Bearing an Iminophosphonamide Ligand

LIU Bo1,2, LI Shihui2, LI Danfeng2, LV Kui2, CUI Dongmei2*, SUN Guangping1*   

  1. (1.Key Laboratory of Automobile Materials of Ministry of Education,Department of
    Materials Science and Engineering,Jilin University,Changchun 130025,China;
    2.State Key Laboratory of Polymer Physics and Chemistry,Changchun Institute of
    Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China)
  • Received:2012-09-27 Revised:2012-10-16 Published:2012-12-10 Online:2012-12-10
  • Contact: DongMei Cui

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摘要： 以三烷基钪Sc(CH2SiMe3)3(THF)2和胺基膦亚胺配体为原料，经烷基消去反应合成了胺基膦亚胺(NPN)型配体螯合钪烷基配合物。 其结构用1H NMR、13C NMR、元素分析和X射线衍射分析进行了表征。 在助催化剂有机硼盐和烷基铝的作用下，该配合物对丁二烯聚合表现出了较高的催化活性。 并且随着聚合温度的降低，催化剂的1,2-选择性也随之升高。 聚合温度为-75 ℃时，产物的1,2-结构含量高达98.0%，聚合物的分子量为2.95×104，分子量分布为1.65。

关键词: 丁二烯, 选择性, 催化活性

Abstract: Treatment of scandium tris(alkyl)s, Sc(CH2SiMe3)3(THF)2, with 2-Me-C6H4NHPPh2=NC6H2-2,4,6-Me3(NPNArH) via deprotonation affords the bis(alkyl) derivative[NPNAr]Sc(CH2SiMe3)2(THF). The complex structure was characterized by means of 1H NMR, 13C NMR, elemental analysis and X-ray diffraction analysis. Complex activated with [Ph3C][B(C6F5)4] and AliBu3 exhibited highly catalytic activity to the polymerization of butadiene. The 1,2-selectivity of polybutadiene noticeably increased with decrease of temperature. The molecular mass is 2.95 ×104 and the molecular mass distribution(Mw/Mn) is 1.65 at -75 ℃.

Key words: butadiene, selectivity, catalytic activity

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