异丙胺为核合成超支化水杨醛亚胺镍系催化剂及其催化乙烯齐聚性能

doi:10.16085/j.issn.1000-6613.2017.05.022

化工进展 ›› 2017, Vol. 36 ›› Issue (05): 1727-1733.DOI: 10.16085/j.issn.1000-6613.2017.05.022

异丙胺为核合成超支化水杨醛亚胺镍系催化剂及其催化乙烯齐聚性能

施伟光¹, 符子剑¹, 王斯晗², 梁红姣¹, 侯爽¹, 李翠勤¹, 王俊¹

1. 东北石油大学化学化工学院石油与天然气化工省重点实验室, 黑龙江大庆 163318;
2. 中国石油大庆化工研究中心, 黑龙江大庆 163714

收稿日期:2016-09-18 修回日期:2017-01-11 出版日期:2017-05-05 发布日期:2017-05-05
通讯作者: 王俊,教授,博士生导师。
作者简介:施伟光(1979-),男,博士,副教授。
基金资助:
国家自然科学基金（21576048）、中国石油科技创新基金（2014D-5006-0503）及东北石油大学青年科学基金（2013NQ130）项目

Synthesis of hyperbranched nickel complex with isopropylamine as a core and its catalytic performance of ethylene oligomerization

SHI Weiguang¹, FU Zijian¹, WANG Sihan², LIANG Hongjiao¹, HOU Shuang¹, LI Cuiqin¹, WANG Jun¹

1. Key Laboratory of Oil & Gas Chemical Technology, College of Chemistry & Chemical Engineering, Northeast Petroleum University, Daqing 163318, Heilongjiang, China;
2. Daqing Petrochemical Research Center, CNPC, Daqing 163714, Heilongjiang, China

Received:2016-09-18 Revised:2017-01-11 Online:2017-05-05 Published:2017-05-05

摘要/Abstract

摘要： 以异丙胺为核合成了一种1.0代聚酰胺-胺型超支化大分子骨架，并进一步与水杨醛和六水合氯化镍通过 “一锅法” 合成了一种具有新型支链结构的超支化水杨醛亚胺镍系催化剂。采用FTIR、¹H NMR和ESI-MS表征方法证明了合成产物的结构与理论结构相符。在甲基铝氧烷为助催化剂、甲苯为溶剂的催化体系内确定了催化乙烯齐聚的最佳反应条件，在Al/Ni摩尔比1000、反应温度25℃、反应压力0.5MPa、反应时间30min的条件下，催化乙烯齐聚的活性达3.8×10⁵gOlig/（mol Ni·h），齐聚产物主要是C₈及以下烯烃，含量高达99%。在相同条件下，通过对比不同骨架结构的超支化镍配合物，初步确定了超支化镍配合物催化乙烯齐聚反应体系催化性能的影响因素。

关键词: 聚合, 催化剂, 选择性, 活性

Abstract: A novel 1.0G poly (amidoamine) hyperbranched molecule with isopropylamine as the core was synthesized,and its corresponding salicylaldimine nickel complex was synthesized by one-pot method with salicylaldehyde and nickel chloride hexahydrate. The intermediate and nickel complex were characterized by FTIR,¹H NMR and ESI-MS. The optimal reaction conditions of this catalytic system were determined with methylaluminoxane as co-catalyst and toluene as solvent. The best conditions of oligomerization reaction were Al/Ni ratio of 1000,25℃,0.5MPa and 30min. Under these conditions,the catalytic activity was 3.8×10⁵g Olig/(mol Ni·h),and the selectivity of olefin under C₈ was as high as 99%. Through comparing the hyperbranched nickel complexes with different backbones,we preliminarily determined the influencing factors for hyperbranched nickel complexes in the oligomerization of ethylene.

Key words: polymerization, catalyst, selectivity, reactivity

中图分类号:

O643.3

施伟光, 符子剑, 王斯晗, 梁红姣, 侯爽, 李翠勤, 王俊. 异丙胺为核合成超支化水杨醛亚胺镍系催化剂及其催化乙烯齐聚性能[J]. 化工进展, 2017, 36(05): 1727-1733.

SHI Weiguang, FU Zijian, WANG Sihan, LIANG Hongjiao, HOU Shuang, LI Cuiqin, WANG Jun. Synthesis of hyperbranched nickel complex with isopropylamine as a core and its catalytic performance of ethylene oligomerization[J]. Chemical Industry and Engineering Progress, 2017, 36(05): 1727-1733.

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异丙胺为核合成超支化水杨醛亚胺镍系催化剂及其催化乙烯齐聚性能

Synthesis of hyperbranched nickel complex with isopropylamine as a core and its catalytic performance of ethylene oligomerization

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