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Efficient Oligomerization of Ethylene to Linear
α -Olefins with High Molecular Weight by Bis(β -ketiminato) Zirconium Catalysts- Acta Polymerica Sinica Vol. 51, Issue 11, Pages: 1285-1294(2020)
- 作者机构：
天津大学材料科学与工程学院 天津 300350
- 作者简介：
- 基金信息：
DOI：10.11777/j.issn1000-3304.2020.20070
CLC：Published：30 September 2020，
Published Online：21 July 2020，
Received：16 March 2020，
Revised：7 May 2020，
扫 描 看 全 文
Jin Zhang, Fei Yang, Bin Wang, Li Pan, Yue-sheng Li. Efficient Oligomerization of Ethylene to Linear
α -Olefins with High Molecular Weight by Bis(β -ketiminato) Zirconium Catalysts. [J]. Acta Polymerica Sinica 51(11):1285-1294(2020)Jin Zhang, Fei Yang, Bin Wang, Li Pan, Yue-sheng Li. Efficient Oligomerization of Ethylene to Linear
α -Olefins with High Molecular Weight by Bis(β -ketiminato) Zirconium Catalysts. [J]. Acta Polymerica Sinica 51(11):1285-1294(2020) DOI： 10.11777/j.issn1000-3304.2020.20070.
摘要
通过两分子
β
-酮亚胺盐与ZrCl
4
的配位反应，合成了一系列具有环状骨架的新型非茂锆配合物. 通过核磁共振谱(
1
H、
13
C和
19
F-NMR)以及单晶X-射线衍射实验，详细表征了双(
β
-酮亚胺)锆氯化物的结构. 在干燥的甲基铝氧烷(dMAO)活化下，双(
β
-酮亚胺)锆可高效催化乙烯齐聚，合成高分子量的线性
α
-烯烃，催化性能明显优于相应的二苄基锆催化剂. 研究表明，
β
-酮亚胺配体取代基的电子效应和空间位阻对乙烯齐聚的催化性能存在显著影响. 在苯亚胺环上对位引入氯原子，Cl的拉电子效应可显著提高乙烯齐
聚催化活性；在苯亚胺对位引入叔丁基，叔丁基的远程位阻效应可大幅度提高乙烯齐聚物的分子量. dMAO用量、齐聚温度、乙烯压力和反应时间等条件也对乙烯齐聚物的分子量和分子量分布有较大影响. 通过改变
β
-酮亚胺配体结构和低齐反应条件，可在较宽范围内调节齐聚效率和乙烯齐聚物的分子量及其分子量分布指数.
Abstract
A series of novel zirconium complexes containing bis(
β
-ketiminato) ligands with cyclic skeleton were efficiently synthesized through the coordination reaction of
β
-ketimine salt with ZrCl
4
. The structures of bis(
β
-ketiminato) zirconium chloride were characterized in detail by
1
H
13
C and
19
F-NMR and single crystal X-ray diffraction. Under the activation of dried methylaluminoxane (dMAO)
they can efficiently catalyze ethylene oligomerization to produce linear
α
-olefins with high molecular weight. Its catalytic performance was much better than that of the corresponding dibenzylzirconium catalyst. The electronic effect and steric hindrance of ligand substituents have a significant effect on the catalytic performance for ethylene oligomerization. When chlorine atom was introduced into 4-position of the benzene imine ring
the withdrawing electron effect remarkably improved the catalytic activity; when tertbutyl was introduced into 4-position of the benzene imine ring
the remote steric hindrance effect of tertbutyl could greatly increase the molecular weight of oligomers while maintaining high catalytic activity. The amount of dMAO
reaction temperature
ethylene pressure and reaction time also greatly influenced the oligomerization of ethylene. Thus
changing the structure of
β
-ketiminato ligands and oligomerization conditions
the catalytic efficiency
molecular weight and molecular weight distribution of oligomers could be adjusted in a wide range.
关键词
乙烯齐聚非茂锆催化剂高分子量线性α-烯烃
Keywords
Ethylene oligomerizationNon-zirconocene catalystHigh α-olefins
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