石油化工2025,Vol.54Issue(3):325-332,8.DOI:10.3969/j.issn.1000-8144.2025.03.005
PCSiN/Ni(Ⅱ)配合物/一氯二乙基铝催化乙烯二聚
Ethylene dimerization catalyzed by PCSiN/Ni(Ⅱ)complex/diethylaluminum chloride
摘要
Abstract
A series of PCSiN-type ligands were synthesized and complexed with nickel(Ⅱ)bromide to obtain the corresponding nickel complexes.The structure of the complexes was characterized with GC,NMR,FTIR,and UV-Vis.The effects of reaction conditions on the reactivity and selectivity of ethylene dimerization catalyzed by the complexes were investigated.The experimental results were verified by density functional theory.The results show that the complex Ni3,where a silicon atom is bonded to two methyl groups and one tetrahydropyrrole functional group,has the smallest embedding volume fraction and therefore exhibits higher activity.The optimal reaction conditions for ethylene dimerization catalyzed by the complex Ni3 are as follows:reaction temperature of 30℃,diethylaluminum chloride as co-catalyst,n(Al)∶n(Ni)=1 000∶1,catalyst amount of 0.6 μmol,and reaction time of 15 min.Under these conditions,the catalytic activity of Ni3 reaches 24.31×106 g/(mol·h),with a butene selectivity of 85.50%,of which the selectivity of 1-butene is 65.56%.The mechanism of ethylene dimerization may be a metal-catalyzed cyclization mechanism.关键词
乙烯二聚/PCSiN型配体/1-丁烯/镍系催化剂Key words
ethylene dimerization/PCSiN-type ligand/1-butene/nickel-based catalyst分类
化学化工引用本文复制引用
邵若星,张钰,李俊辰,姜涛..PCSiN/Ni(Ⅱ)配合物/一氯二乙基铝催化乙烯二聚[J].石油化工,2025,54(3):325-332,8.基金项目
国家自然科学基金项目(22071178) (22071178)
中国石油科技计划项目(2020B2512). (2020B2512)