芘环基二亚胺镍催化剂的合成及其乙烯聚合/共聚的性能研究

王文兵; 邹陈; 陈昶乐

doi:10.11777/j.issn1000-3304.2023.23118

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芘环基二亚胺镍催化剂的合成及其乙烯聚合/共聚的性能研究

研究论文 | 更新时间：2023-11-03

- 芘环基二亚胺镍催化剂的合成及其乙烯聚合/共聚的性能研究
  增强出版
- Synthesis of Pyrene Based α-Diimide Nickel Catalysts for Ethylene Polymerization/Copolymerization
- 高分子学报 2023年54卷第11期页码：1697-1707
- 作者机构：
  
  中国科学技术大学高分子科学与工程系合肥 230026
- 作者简介：
  
  E-mail: chen1215@ustc.edu.cn
  changle@ustc.edu.cn
- 基金信息：
  
  国家自然科学基金(基金号 ┣52203016);U1904212┫;中国博士后基金(基金号 ┣2021M703072);2022T150617┫;中国科学技术大学统筹推进世界一流大学和一流学科建设专项资金(基金号 YD9990002018)
- DOI：10.11777/j.issn1000-3304.2023.23118
  中图分类号：
- 纸质出版日期：2023-11-20，
  
  网络出版日期：2023-09-01，
  
  收稿日期：2023-04-28，
  
  录用日期：2023-06-15
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王文兵,邹陈,陈昶乐.芘环基二亚胺镍催化剂的合成及其乙烯聚合/共聚的性能研究[J].高分子学报,2023,54(11):1697-1707.

Wang Wen-bing,Zou Chen,Chen Chang-le.Synthesis of Pyrene Based α-Diimide Nickel Catalysts for Ethylene Polymerization/Copolymerization[J].Acta Polymerica Sinica,2023,54(11):1697-1707.
王文兵,邹陈,陈昶乐.芘环基二亚胺镍催化剂的合成及其乙烯聚合/共聚的性能研究[J].高分子学报,2023,54(11):1697-1707. DOI： 10.11777/j.issn1000-3304.2023.23118.

Wang Wen-bing,Zou Chen,Chen Chang-le.Synthesis of Pyrene Based α-Diimide Nickel Catalysts for Ethylene Polymerization/Copolymerization[J].Acta Polymerica Sinica,2023,54(11):1697-1707. DOI： 10.11777/j.issn1000-3304.2023.23118.

摘要

选用不同结构的芳香烃基团，可以便捷地设计合成一系列具有不同催化性能的后过渡金属催化剂. 芘环芳香烃的结构特征之一是芘环芳香烃分子之间存在

堆积作用，因而具有调节过渡金属催化剂性能的潜力. 本文设计合成了一系列具有芘环结构的

-二亚胺镍催化剂，利用这些芘环基二亚胺镍催化剂的

堆积效应，可使镍催化剂的乙烯聚合活性高达3.12×10

g·mol

-1

·h

-1

，制备的聚乙烯的重均相对分子质量高达1.98×10

g·mol

-1

. 这些催化剂还可以实现乙烯与10-十一烯酸甲酯的共聚，并对有

堆积效应的10-十一烯酸芘基酯单体共聚性能更佳.

Abstract

The transition metal catalysts required for coordination polymerization to prepare polyolefins have received high attention from academia and industry with the continuous development of the polyolefin industry. Among them

late transition metal catalysts represented by nickel and palladium have been widely studied in olefin/polar monomer copolymerization reactions due to their low oxygen affinity and high tolerance to polar groups. By selecting aromatic hydrocarbon groups with different structures

a series of late transition metal catalysts with different catalytic properties can be conveniently designed and synthesized. One of the structural characteristics of pyrene ring aromatic hydrocarbons is the

π‍

-‍

stacking effect between pyrene ring aromatic hydrocarbon molecules

which has the potential to regulate the performance of transition metal catalysts. This article introduced the pyrene ring group into the ligand structure and designed and synthesized a series of

α‍

-diimine nickel catalysts with pyrene ring structure

and the structures of these ligands and catalysts were characterized in detail by nuclear magnetic resonance spectrometer (NMR)

electrospray ionization mass spectrometry (ESI-MS)

X-ray diffraction (XRD)

etc

. Subsequently

the ethylene polymerization reaction of these catalysts was studied in heptane solvent. Due to the interaction of pyrene ring groups

the

π‍

-‍

stacking effect may be formed between these nickel complexes. In addition

adding pyrene molecules to the aggregation system may also form the

π‍

-‍

stacking effect with the complexes. By utilizing the

π‍

-‍

stacking effect of these pyrene ring based

α‍

-diimide nickel catalysts

the ethylene polymerization activity of the nickel catalysts was as high as 3.12×10

g·mol

-1

·h

-1

with a weight average relative molecular weight of up to 1.98×10

g·mol

-1

for the prepared polyethylene

and the branching degree of polyethylene was 4-77 C/1000 C. These catalysts can also achieve copolymerization of ethylene with methyl 10-undecanoate

with a copolymerization activity of up to 3.30×10

g·mol

-1

·h

-1

. Moreover

the copolymerization performance of 10-undecylenoic acid pyrene ester monomers with

π‍

-‍

stacking effect was better

which once again proved the possibility of

stacking effect in this type of catalyst.

关键词

镍催化剂芘乙烯聚合共聚合聚乙烯

Keywords

Nickel catalystPyreneEthylene polymerizationCopolymerizationPolyethylene

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