星形吡啶亚胺铁系催化剂的合成及催化乙烯齐聚性能  

Synthesis and Catalytic Performance of Star Pyridinimine Iron Catalyst in Ethylene Oligomerization

作　　者：张娜[1] 吴岩松 宋振博 毛国梁[1] 李翠勤[1] 陈丽铎 王俊[1] Na Zhang;Yansong Wu;Zhenbo Song;Guoliang Mao;Cuiqin Li;Liduo Chen;Jun Wang(Provincial Key Laboratory of Oil&Gas Chemical Technology,College of Chemistry and Chemical Engineering,Northeast Petroleum University,Daqing 163318,China)

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

出　　处：《高分子材料科学与工程》2021年第2期15-22,共8页Polymer Materials Science & Engineering

基　　金：黑龙江省博士后科学基金(16190016);东北石油大学青年科学基金(2018QNL-13)。

摘　　要：采用1.0 G星形大分子、吡啶-2-甲醛和FeCl_(2)·4H_(2)O为原料,依次经席夫碱反应和络合反应合成了一种新型星形吡啶亚胺配体及其铁系催化剂,利用红外光谱、核磁共振氢谱、紫外光谱、电喷雾电离质谱及电感耦合等离子体质谱等方法对合成产物的结构进行表征。考察了反应体系和反应条件对催化乙烯齐聚性能的影响。研究结果表明,催化体系及反应条件对催化乙烯齐聚性能均有较大的影响,当以甲苯为溶剂、甲基铝氧烷(MAO)为助催化剂时,在最佳反应条件下,星形吡啶亚胺铁系催化剂催化乙烯齐聚的活性可达3.96×10^(5)g/(mol Fe·h),产物主要为丁烯和己烯。此外,在对星形吡啶亚胺铁系催化剂催化性能评价的基础上,对其催化乙烯齐聚的机理也进行了推断。A kind of novel star iminopyridyl ligand and the corresponding iron catalyst were prepared with 1.0 G star macromolecule,pyridine-2-carboxaldehyde and FeCl_(2)·4H_(2)O as raw material,and the structures were fully characterized by FT-IR,1H-NMR,UV,ESI-MS and ICP-MS.The effects of the reaction systems and reaction conditions on catalytic properties of ethylene oligomerization were investigated.The result shows that the catalytic systems and reaction conditions have a significant effect on catalytic properties.Under the optimum reaction condition,the catalytic activity can reach up to 3.96×10^(5) g/(mol Fe·h),and the products are mainly butene and hexene when toluene is used as solvent and MAO is used as co-catalyst.In addition,the mechanism of catalytic ethylene oligomerization was deduced on the base of the evaluation of catalytic performance of star iminopyridyl iron catalysts.

关 键 词：星形大分子 吡啶亚胺配体 铁系催化剂 乙烯齐聚 活性 

分 类 号：TQ221.21[化学工程—有机化工]