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Copolymerization of Ethylene and Polar Vinyl Monomers by Rare-earth Metal Catalysts
- Acta Polymerica Sinica Vol. 55, Issue 11, Pages: 1487-1494(2024)
- 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：
Shi-hui Li, E-mail: shihui-li@ciac.ac.cn
- 基金信息：
DOI：10.11777/j.issn1000-3304.2024.24092
CLC：- CSTR：32057.14.GFZXB.2024.7254
Received：27 March 2024，
Accepted：2024-04-30，
Published Online：19 June 2024，
Published：20 November 2024
- 稿件说明：
移动端阅览
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
2
-Ph)Sc(CH
2
SiMe
3
)
2
(THF) (
1
)、(Flu-CH
2
-C
5
H
4
N)Sc(CH
2
SiMe
3
)
2
(
2
)、(Flu-CH
2
CH
2
-NHC-C
6
H
2
Me
3
-2
4
6)Sc(CH
2
SiMe
3
)
2
(
3
)、(Flu-CH
2
CH
2
-NHC-C
6
H
4
Me)Sc(CH
2
SiMe
3
)
2
(
4
)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
i
Bu
3
保护的5-己烯-1-醇(
M2
)的共聚合行为. 其中，催化剂
1
的催化活性最高，达到1.32×10
6
g·mol
Sc
-1
·h
-1
，但产生的是乙烯均聚物，催化剂
2
无催化活性，催化剂
3
和
4
的活性分别为0.38×10
6
和1.24×10
6
g·mol
Sc
-1
·h
-1
，生成了
M2
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
4
对9碳烷烃间隔的10-十一烯-1-醇(
M3
)与乙烯共聚合活性最高(1.19×10
7
g·mol
Sc
-1
·h
-1
)、共聚能力最强(
M3
插入率为4.9 mol%). 系统研究了极性单体
M3
浓度、聚合温度、乙烯压力等，对催化剂
4
催化乙烯与
M3
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 (
M2
) masked by 1.1 equivalents of Al
i
Bu
3
is carried out by four rare-earth metal catalysts bearing different steric hindrances: (Flu-CH
2
-Ph)Sc(CH
2
- SiMe
3
)
2
(THF) (
1
)
(Flu-CH
2
-C
5
H
4
N)Sc(CH
2
SiMe
3
)
2
(
2
)
(Flu-CH
2
CH
2
-NHC-C
6
H
2
Me
3
-2
4
6)Sc(CH
2
SiMe
3
)
2
(
3
)
(Flu-CH
2
CH
2
-NHC-C
6
H
4
Me)Sc(CH
2
SiMe
3
)
2
(
4
). Among them
complex
1
shows the hi
ghest catalytic activity (1.32×10
6
g·mol
Sc
-1
·h
-1
) but gives pure polyethylene without detectable
M2
unit
and
in contrast
complex
2
is nearly inert. Under same conditions
the bulkier complex
3
shows moderate activity (0.38×10
6
g·mol
Sc
-1
·h
-1
) and low comonomer incorporation (0.7 mol%). On switching to the bulkiest complex
4
the copolymerization process is obviously promoted with a catalytic activity of 1.24×10
6
g·mol
Sc
-1
·h
-1
and generates a copolymer with 1.8 mol%
M2
. For the polar vinyl monomers having different CH
2
spacers between polar and vinyl groups
complex
4
exhibits the best catalytic performance for the copolymerization of ethylene with 10-undecene-1-ol with the highest catalytic activity (1.19×10
7
g·mol
Sc
-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
4
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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