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作 者:施伟光[1] 符子剑 王斯晗 梁红姣 侯爽[1] 李翠勤[1] 王俊[1]
机构地区:[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
出 处:《化工进展》2017年第5期1727-1733,共7页Chemical Industry and Engineering Progress
基 金:国家自然科学基金(21576048);中国石油科技创新基金(2014D-5006-0503);东北石油大学青年科学基金(2013NQ130)项目
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3.8×10~5g Olig/(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。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 × 10^5g 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.
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