Introduction of Constrained Cyclic Skeleton into <italic style="font-style: italic">β</italic>-Enaminoketonato Vanadium Complexes:A Strategy for Stabilization of Active Centre of Vanadium Catalyst for Ethylene Polymerization

Kai-ti Wang; Yong-xia Wang; Bin Wang; Yan-guo Li; Yue-sheng Li

doi:10.1007/s10118-017-1956-z

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Introduction of Constrained Cyclic Skeleton into β-Enaminoketonato Vanadium Complexes:A Strategy for Stabilization of Active Centre of Vanadium Catalyst for Ethylene Polymerization

Papers | Updated：2021-02-18

- Introduction of Constrained Cyclic Skeleton into β-Enaminoketonato Vanadium Complexes:A Strategy for Stabilization of Active Centre of Vanadium Catalyst for Ethylene Polymerization
- Introduction of Constrained Cyclic Skeleton into β-Enaminoketonato Vanadium Complexes:A Strategy for Stabilization of Active Centre of Vanadium Catalyst for Ethylene Polymerization
- Chinese Journal of Polymer Science 2017年35卷第9期页码：1110-1121
- Affiliations：
  
  a.Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
  b.Tianjin Key Lab of Composite & Functional Materials, School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
  c.University of Chinese Academy of Sciences, Beijing 100049, China
- Author bio：
  
  Yue-sheng Li (李悦生), E-mail:ysli@tju.edu.cn
- Funds：
  
  This work was financially supported by the National Natural Science Foundation of China(21234006);China National High-tech R&D Program(2015AA034002);Supplementary material is available in the online version of this article at http://dx.doi.org/10.1007/s10118-017-1956-z.
- DOI：10.1007/s10118-017-1956-z
  中图分类号：
- 收稿：2017-02-20，
  
  修回：2017-3-6，
  
  录用：2017-3-7，
  
  纸质出版：2017-09-05
- Accepted：
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Kai-ti Wang, Yong-xia Wang, Bin Wang, 等. Introduction of Constrained Cyclic Skeleton into β-Enaminoketonato Vanadium Complexes:A Strategy for Stabilization of Active Centre of Vanadium Catalyst for Ethylene Polymerization[J]. Chinese Journal of Polymer Science, 2017,35(9):1110-1121. DOI: 10.1007/s10118-017-1956-z.

Kai-ti Wang, Yong-xia Wang, Bin Wang, et al. Introduction of Constrained Cyclic Skeleton into β-Enaminoketonato Vanadium Complexes:A Strategy for Stabilization of Active Centre of Vanadium Catalyst for Ethylene Polymerization[J]. Chinese Journal of Polymer Science, 2017, 35(9): 1110-1121. DOI: 10.1007/s10118-017-1956-z.
Kai-ti Wang, Yong-xia Wang, Bin Wang, 等. Introduction of Constrained Cyclic Skeleton into β-Enaminoketonato Vanadium Complexes:A Strategy for Stabilization of Active Centre of Vanadium Catalyst for Ethylene Polymerization[J]. Chinese Journal of Polymer Science, 2017,35(9):1110-1121. DOI: 10.1007/s10118-017-1956-z. DOI：

Kai-ti Wang, Yong-xia Wang, Bin Wang, et al. Introduction of Constrained Cyclic Skeleton into β-Enaminoketonato Vanadium Complexes:A Strategy for Stabilization of Active Centre of Vanadium Catalyst for Ethylene Polymerization[J]. Chinese Journal of Polymer Science, 2017, 35(9): 1110-1121. DOI: 10.1007/s10118-017-1956-z. DOI：

摘要

Abstract

Several novel mono(

-enaminoketonato) vanadium complexes bearing constrained cyclic skeleton

including[(C

C(O)=C(CH

)

CH=N-Ar]VCl

(THF)

(

V3a

Ar=C

;

V4a

Ar=C

;

V4b

Ar=C

;

V4c

Ar=(C

)

;

V5a

Ar=C

)

were synthesized and their structure and properties were characterized. The structures of

V4c

and

V5a

in solid-state were further confirmed by X-ray crystallographic analysis. Density functional theory (DFT) results indicated that these complexes showed enhanced steric hindrance around the metal center as compared with the acyclic analogues. Upon activation with Et2AlCl and in the presence of ethyl trichloroacetate as a reactivator

all of the complexes exhibited high catalytic activities (10

gPE/(molV·h)) toward ethylene polymerization

and the obtained polymers exhibited unimodal distributions (

n=2.0-2.3) even produced at elevated temperatures (70-100℃) and prolonged reaction time. When MAO was employed as a cocatalyst

they only showed moderate catalytic activities (10

gPE/(molV·h))

but the resulting polymers had higher molecular weights (168-241 kg/mol). These vanadium complexes with cyclic skeleton also showed high catalytic activities toward ethylene/norbornene copolymerization. The produced copolymers displayed approximate alternating structure at high in-feed concentration of norbornene. The catalytic capabilities of these complexes could be tuned conveniently by varying ligand structure. Furthermore

the cyclic voltammetry results also proved that these complexes exhibited better redox stabilities than the complexes bearing linear skeleton.

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Introduction of Constrained Cyclic Skeleton into β-Enaminoketonato Vanadium Complexes:A Strategy for Stabilization of Active Centre of Vanadium Catalyst for Ethylene Polymerization

Introduction of Constrained Cyclic Skeleton into β-Enaminoketonato Vanadium Complexes:A Strategy for Stabilization of Active Centre of Vanadium Catalyst for Ethylene Polymerization

DOI：10.1007/s10118-017-1956-z

摘要

Abstract

关键词

Keywords

references