王俊,李环宇,刘宪红,李翠勤,张娜.化学通报,2017,80(2):196-201. |
树枝状钴系催化剂的合成及催化乙烯齐聚性能 |
Synthesis of Novel Dendrimer-based Cobalt Catalyst for Ethylene Oligomerization |
投稿时间:2016-07-07 修订日期:2016-08-17 |
DOI: |
中文关键词: 树枝状大分子 水杨醛亚胺配体 催化剂 乙烯齐聚 催化活性 |
英文关键词:dendrimer, salicylaldimine ligand, catalyst, ethylene oligomerization, catalytic activity |
基金项目:国家自然科学基金项目(21576048) |
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中文摘要: |
以1,8-辛二胺为核的1.0代(1.0G)树枝状大分子、水杨醛和六水氯化钴为原料,依次通过席夫碱反应和配位反应合成了一种新型的树枝状水杨醛亚胺配体和钴系催化剂;并对目标产物进行FT-IR、UV、1H NMR和MS表征,证实其合成产物的结构与理论结构相符。考察了助催化剂种类、溶剂种类、反应条件及金属活性中心对乙烯齐聚性能的影响。结果表明,当以一氯二乙基铝(Et2AlCl)为助催化剂,甲苯为溶剂时,催化剂具有良好的催化乙烯齐聚性能,并在反应温度为25℃、Al/Co摩尔比为1500、压力为1.0 MPa、时间为0.5 h时,催化活性达到6.84×105 g/(mol Co?h),齐聚产物中C8及C8以上的烯烃含量为52.77%。 |
英文摘要: |
The novel dendritic salicylaldimine ligand was synthesized by Schiff’s base reaction using 1.0 generation dendrimer as bridged group, and the cobalt catalyst with 1,8-octanediamine as core based on dendritic salicylaldimine ligand was prepared by cobalt metallic coordination reaction. The structures of the dendritic ligand and the cobalt catalyst were characterized by FT-IR, UV, 1H NMR and MS, and the structures of synthetic products were consistent with the theory of structures. The catalyst was evaluated as precursor for ethylene oligomerization with various co-catalysts, solvents, reaction conditions and metallic active centers. The results showed that the catalyst exhibited better catalytic performance after activation with Et2AlCl in toluene. Under the conditions of 25℃, Al/Co mole ratio 1500, 1.0 MPa and 0.5 h employed for the cobalt catalyst, the catalytic activity showed a maximum value of 6.84×105 g/(mol Co?h), and the selectivity for ≥C8 olefins was 52.77%. |
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