稀土催化乙烯与极性烯烃共聚合研究

梁旦; 姜洋; 李世辉; 崔冬梅

doi:10.11777/j.issn1000-3304.2024.24092

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稀土催化乙烯与极性烯烃共聚合研究

研究论文 | 更新时间：2024-12-24

- 稀土催化乙烯与极性烯烃共聚合研究
- Copolymerization of Ethylene and Polar Vinyl Monomers by Rare-earth Metal Catalysts
- 高分子学报 2024年55卷第11期页码：1487-1494
- 作者机构：
  
  1.中国科学院长春应用化学研究所高分子物理与化学国家重点实验室长春 130022
  2.中国科学技术大学应用化学与工程学院合肥230026
- 作者简介：
  
  E-mail: shihui-li@ciac.ac.cn
  dmcui@ciac.ac.cn
- 基金信息：
  
  国家自然科学基金(基金号 ┣52073275;U23B6011;U21A20279);22331010┫
- DOI：10.11777/j.issn1000-3304.2024.24092
  中图分类号：
- CSTR：32057.14.GFZXB.2024.7254
- 收稿日期：2024-03-27，
  
  录用日期：2024-04-30，
  
  网络出版日期：2024-06-19，
  
  纸质出版日期：2024-11-20
- 稿件说明：
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梁旦, 姜洋, 李世辉, 崔冬梅. 稀土催化乙烯与极性烯烃共聚合研究. 高分子学报, 2024, 55(11), 1487-1494

Liang, D.; Jiang, Y.; Li， S. H.; Cui, D. M. Copolymerization of ethylene and polar vinyl monomers by rare-earth metal catalysts. Acta Polymerica Sinica, 2024, 55(11), 1487-1494
梁旦, 姜洋, 李世辉, 崔冬梅. 稀土催化乙烯与极性烯烃共聚合研究. 高分子学报, 2024, 55(11), 1487-1494 DOI： 10.11777/j.issn1000-3304.2024.24092. CSTR： 32057.14.GFZXB.2024.7254.

Liang, D.; Jiang, Y.; Li， S. H.; Cui, D. M. Copolymerization of ethylene and polar vinyl monomers by rare-earth metal catalysts. Acta Polymerica Sinica, 2024, 55(11), 1487-1494 DOI： 10.11777/j.issn1000-3304.2024.24092. CSTR： 32057.14.GFZXB.2024.7254.

摘要

考察了(Flu-CH

-Ph)Sc(CH

SiMe

)

(THF) (

)、(Flu-CH

-C

N)Sc(CH

SiMe

)

(

)、(Flu-CH

-NHC-C

-2

6)Sc(CH

SiMe

)

(

)、(Flu-CH

-NHC-C

Me)Sc(CH

SiMe

)

(

)空间位阻大小不等的4种稀土催化剂，对乙烯与1.1倍摩尔量Al

保护的5-己烯-1-醇(

)的共聚合行为. 其中，催化剂

的催化活性最高，达到1.32×10

g·mol

-1

·h

-1

，但产生的是乙烯均聚物，催化剂

无催化活性，催化剂

和

的活性分别为0.38×10

和1.24×10

g·mol

-1

·h

-1

，生成了

插入率分别为0.7 mol%和

1.8 mol%的共聚物. 对不同烷烃链长间隔的极性烯烃单体，催化剂

对9碳烷烃间隔的10-十一烯-1-醇(

)与乙烯共聚合活性最高(1.19×10

g·mol

-1

·h

-1

)、共聚能力最强(

插入率为4.9 mol%). 系统研究了极性单体

浓度、聚合温度、乙烯压力等，对催化剂

催化乙烯与

共聚合活性及其插入率的影响规律. 通过NMR、GPC和DSC对所得的乙烯-极性烯烃共聚物进行了微观结构、热性能分析.

Abstract

The copolymerization of ethylene and 5-hexen-1-ol (

) masked by 1.1 equivalents of Al

is carried out by four rare-earth metal catalysts bearing different steric hindrances: (Flu-CH

-Ph)Sc(CH

- SiMe

)

(THF) (

)

(Flu-CH

-C

N)Sc(CH

SiMe

)

(

)

(Flu-CH

-NHC-C

-2

6)Sc(CH

SiMe

)

(

)

(Flu-CH

-NHC-C

Me)Sc(CH

SiMe

)

(

). Among them

complex

shows the hi

ghest catalytic activity (1.32×10

g·mol

-1

·h

-1

) but gives pure polyethylene without detectable

unit

and

in contrast

complex

is nearly inert. Under same conditions

the bulkier complex

shows moderate activity (0.38×10

g·mol

-1

·h

-1

) and low comonomer incorporation (0.7 mol%). On switching to the bulkiest complex

the copolymerization process is obviously promoted with a catalytic activity of 1.24×10

g·mol

-1

·h

-1

and generates a copolymer with 1.8 mol%

. For the polar vinyl monomers having different CH

spacers between polar and vinyl groups

complex

exhibits the best catalytic performance for the copolymerization of ethylene with 10-undecene-1-ol with the highest catalytic activity (1.19×10

g·mol

-1

·h

-1

) and the strongest incorporation ability (4.9 mol%). The influence of reaction conditions such as comonomer concentration

polymerization temperature and ethylene pressures on the catalytic performance of complex

are screened. The microstructures and thermal properties of the resultant copolymers are well-characterized by nuclear magnetic resonance (NMR)

gel permeation chromatography (GPC) and differential scanning calorimeter (DSC).

关键词

Keywords

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