Synthesis of Polyethylene Elastomers <italic style="font-style: italic">via</italic> <italic style="font-style: italic">α</italic>-Diimine Ni(II) Catalysts with Electronic and Steric Synergistic Effects

Jing-feng Yue; Xiao-qiang Hu; Jia-jun Qi; Yu-yin Wang; Zhong-bao Jian

doi:10.11777/j.issn1000-3304.2025.25058

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Synthesis of Polyethylene Elastomers via α-Diimine Ni(II) Catalysts with Electronic and Steric Synergistic Effects

Research Article | 更新时间：2025-08-28

- Synthesis of Polyethylene Elastomers via α-Diimine Ni(II) Catalysts with Electronic and Steric Synergistic Effects
- Acta Polymerica Sinica Vol. 56, Issue 9, Pages: 1505-1517(2025)
- 作者机构：
  
  1.中国科学院长春应用化学研究所高分子科学与技术全国重点实验室长春 130022
  2.中国科学技术大学应用化学与工程学院合肥 230026
  3.西华师范大学化学化工学院化学合成与污染控制四川省重点实验室南充 637002
- 作者简介：
  
  Yu-yin Wang, E-mail:yuyinwang@cwnu.edu.cn
  Zhong-bao Jian, E-mail: zbjian@ciac.ac.cn
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2025.25058
  CLC：
- CSTR：32057.14.GFZXB.2025.7396
- Received：02 March 2025，
  
  Accepted：07 April 2025，
  
  Published Online：08 May 2025，
  
  Published：20 September 2025
- 稿件说明：
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岳静峰, 胡小强, 齐佳俊, 王玉银, 简忠保. 电子和空间位阻协同的α-二亚胺镍催化制备聚乙烯弹性体.高分子学报, 2025, 56(9), 1505-1517

Yue, J. F.; Hu, X. Q.; Qi, J. J.; Wang, Y. Y.; Jian, Z. B. Synthesis of polyethylene elastomers via α-diimine Ni(II) catalysts with electronic and steric synergistic effects. Acta Polymerica Sinica, 2025, 56(9), 1505-1517
岳静峰, 胡小强, 齐佳俊, 王玉银, 简忠保. 电子和空间位阻协同的α-二亚胺镍催化制备聚乙烯弹性体.高分子学报, 2025, 56(9), 1505-1517 DOI： 10.11777/j.issn1000-3304.2025.25058. CSTR： 32057.14.GFZXB.2025.7396.

Yue, J. F.; Hu, X. Q.; Qi, J. J.; Wang, Y. Y.; Jian, Z. B. Synthesis of polyethylene elastomers via α-diimine Ni(II) catalysts with electronic and steric synergistic effects. Acta Polymerica Sinica, 2025, 56(9), 1505-1517 DOI： 10.11777/j.issn1000-3304.2025.25058. CSTR： 32057.14.GFZXB.2025.7396.

摘要

-二亚胺镍配合物因其特有的“链行走”聚合机理对聚合物主链结构中的支化密度与支化类型进行原位调节而备受关注，目前已被广泛用于聚烯烃弹性体(POE)合成研究. 在本工作中，合成了一系列基于电子和空间位阻协同效应的对称/不对称

-二亚胺镍催化剂，并将其用于乙烯聚合反应. 通过在苯胺3

5-位点引入甲氧基，一方面使其具有给电子效应，另一方面甲氧基与2

6-位点取代基具有排斥作用，从而将轴向位阻基团推向活性中心，对中心金属进行有效屏蔽. 基于3

5-三甲氧基取代的电子和空间位阻协同策略有效促进了乙烯链增长，并抑制链转移副反应的发生，这类催化剂普遍表现出很高的催化活性(高达1.1×10

g·mol

-1

·h

-1

)，可制备出分子量可调(

= 124~2106 kDa)，支化密度可调(41/1000C~103/1000C)的聚乙烯弹性体材料. 通过高温核磁共振碳谱分析，发现聚合物微观结构以甲基支化为主，乙基、正丙基、正丁基等短支链占比约20%. 对不同分子量梯度和支化梯度的聚乙烯样品进行了力学性能测试，这些高支化聚乙烯表现出低至中等的拉伸强度(2.16~12.33 MPa)和高断裂伸长率(339%~1339%)，表明聚合物具有非常好的韧性. 这些聚乙烯材料普遍具有良好的弹性回复性能，应变回复率最高可达91%.

Abstract

Nickel(II)

-diimine complexes have attracted significant attention due to their unique "chain-walking" polymerization mechanism

which enables

in situ

regulation of branching density and branching type in polymer backbone

and have been widely investigated for polyolefin elastomer (POE) synthesis. In this work

a series of symmetric/asymmetric

α‍

-diimi

ne nickel catalysts based on electronic and steric synergistic effects were synthesized and applied in ethylene polymerization. By introducing methoxy groups at the 3

5-positions of the aniline moiety

these substituents not only exhibit electron-donating effects

but also generate steric repulsion with 2

6-position substituents

thereby pushing axial steric groups close to the active center for effectively shielding the central metal. The 3

‍4

‍5-trimethoxy substitution strategy combining electronic and steric effects significantly promotes chain propagation while suppressing chain transfer reactions. These catalysts generally demonstrate high catalytic activities (up to 1.1×10

g·mol

-1

·h

-1

)

producing polyethylene elastomers with tunable molecular weights (

=124-2106 kDa) and tunable branching densities (41-103 branches/1000C). High-temperature

C-NMR analysis reveals that the polymer microstructure is dominated by methyl branches

with around 20% of short-chain branches (ethyl

-propyl

-butyl

etc.

) in total branches. Tensile testing of polyethylene samples with different molecular weights and branching densities show that these highly branched polyethylenes exhibit low-to-moderate tensile strength (2.16-12.33 MPa) and high elongation at break (339%-1339%)

indicating excellent toughness. These polyethylene materials generally demonstrate favorable elastic recovery properties

achieving a maximum strain recovery of 91%.

关键词

Keywords

references

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Synthesis of Polyethylene Elastomers via α-Diimine Ni(II) Catalysts with Electronic and Steric Synergistic Effects

DOI：10.11777/j.issn1000-3304.2025.25058

摘要

Abstract

关键词

Keywords

references