High-performance, Low-Cost Polyolefins Based on Dynamic Covalent Bonds and Ionic Bonds Dual Cross-linking

Shi-yu Wang; Xuan-wei Zhang; Xiao-pei Li; Shi-ji Gao; Yong-jie Zhang

doi:10.11777/j.issn1000-3304.2025.25096

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High-performance, Low-Cost Polyolefins Based on Dynamic Covalent Bonds and Ionic Bonds Dual Cross-linking

更新时间：2025-07-10

- High-performance, Low-Cost Polyolefins Based on Dynamic Covalent Bonds and Ionic Bonds Dual Cross-linking
- Acta Polymerica Sinica Pages: 1-13(2025)
- 作者机构：
  
  1.大连工业大学纺织与材料工程学院大连 116034
  2.大连工业大学实验仪器中心大连 116034
- 作者简介：
  
  Yong-jie Zhang, E-mail: yjzhang@dlpu.edu.cn
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2025.25096
  CLC：
- CSTR：32057.14.GFZXB.2025.7439
- Received：11 April 2025，
  
  Accepted：16 June 2025，
  
  Published Online：09 July 2025，
- 稿件说明：
移动端阅览
王诗雨, 张璇玮, 李晓佩, 高世纪, 张勇杰. 高性能、低成本动态共价键/离子键双重交联聚烯烃制备与性能. 高分子学报, doi: 10.11777/j.issn1000-3304.2025.25096

Wang S. Y.; Zhang, X. W.; Li, X. P.; Gao, S. J.; Zhang, Y. J. High-performance, low-cost polyolefins based on dynamic covalent bonds and ionic bonds dual cross-linking. Acta Polymerica Sinica, doi: 10.11777/j.issn1000-3304.2025.25096
王诗雨, 张璇玮, 李晓佩, 高世纪, 张勇杰. 高性能、低成本动态共价键/离子键双重交联聚烯烃制备与性能. 高分子学报, doi: 10.11777/j.issn1000-3304.2025.25096 DOI： CSTR： 32057.14.GFZXB.2025.7439.

Wang S. Y.; Zhang, X. W.; Li, X. P.; Gao, S. J.; Zhang, Y. J. High-performance, low-cost polyolefins based on dynamic covalent bonds and ionic bonds dual cross-linking. Acta Polymerica Sinica, doi: 10.11777/j.issn1000-3304.2025.25096 DOI： CSTR： 32057.14.GFZXB.2025.7439.

摘要

交联聚烯烃的力学性能、热性能、电气性能、耐溶剂性能十分优异，在电缆绝缘、热收缩管等领域应用广泛；但传统交联聚烯烃具有不可逆的三维交联网络结构，服役后交联聚烯烃无法进行回收再利用，造成环境污染及资源浪费. 类玻璃体高分子(vitrimer)是一种具有可逆动态交联网络结构的新型高分子材料，兼具热塑性聚合物的可再加工特性以及热固性聚合物优良的力学性能、热性能、耐溶剂性能，得到了学术界与产业界的广泛关注. 作为下一代交联聚烯烃，聚烯烃基类玻璃体高分子取得了丰硕研究成果. 然而，低成本、高性能聚烯烃基类玻璃体高分子的实用制备仍面临挑战. 相较于单重交联网络，双重交联网络结构赋予了类玻璃体高分子更大的综合性能调控空间. 本文以富含反应性羧基的商品化大宗产品乙烯-丙烯酸共聚物(EAA)为原料，以生物基环氧大豆油(ESO)和氧化锌为交联剂，通过一步反应性共混制备出具备

-羟基酯和羧酸锌双重动态交联结构的EAA基类玻璃体高分子(EAA-ESO-ZnO). 红外分析和溶胀测试证实了共价键交联网络和离子键交联网络的形成. 动态热机械分析(DMA)表明，EAA-ESO-ZnO具有典型交联聚合物的动态机械性能及优异的高温耐蠕变性能，证明其具有三维交联网络结构. 通过应力松弛实验，估算得到键交换活化能为70.8 kJ·mol

-1

，与文献值接近. 相较于EAA，EAA-ESO-ZnO的拉伸强度和弹性模量分别提高了41.8%和54.5%. 经过3次再加工，EAA-ESO-ZnO的拉伸强度提升13.8%，断裂伸长率保持率达92.0%，证明其具有优异的再加工性能. 综上所述，本文提出了一种低成本、高性能聚烯烃基类玻璃体高分子的高效、易放大的制备路线，为可循环利用交联聚烯烃的制备提供了新思路.

Abstract

Cross-linked polyolefins possess excellent mechanical properties

thermal properties

electrical properties

and solvent resistance

thus widely used in diverse fields such as cable insulation and heat shrinkable tubes. However

traditional cross-linked polyolefins have an irreversible three-dimensional cross-linked network structure. Post-consumption cross-linked polyolefins cannot be recycled or reused

resulting in environmental pollution and resource wastage. Vitrimer

a type of novel polymer material

has a reversible dynamic cross-linked network structure. It combines the reprocessability of thermoplastic polymers with the excellent mechanical properties

thermal properties

and solvent resistance of thermosetting polymers

thus attracting extensive attention from both the academia and industry. As the emerging next-generation cross-linked polyolefin

polyolefin-based vitrimer has achieved fruitful research results. Nevertheless

the practical preparation of polyolefin-based vitrimer with low cost and high performance remains a challenging task. Compared with a single cross-linked network

a dual cross-linked network structure endows vitrimers with easily adjustable comprehensive properties. In this study

starting from commodity ethylene acrylic acid copolymer (EAA) with abundant reactive carboxyl groups

bio-based epoxidized soybean oil (ESO)

and zinc oxide

a dual cross-linked EAA-based vitrimer (EAA-ESO-ZnO) with dynamic

-hydroxy ester and zinc carboxylate cross-linkages was prepared through a one-step reactive blending approach. FTIR analysis and gel fraction testing confirmed the formation of covalently and ionically cross-linked networks of EAA-ESO-ZnO. Dynamic mechanical analysis (DMA) revealed that EAA-ESO-ZnO exhibit

ed the dynamic mechanical properties of typical cross-linked polymers and excellent creep resistance at high temperatures

confirming the presence of a three-dimensional cross-linked network structure. Through stress relaxation experiments

the bond exchange activation energy was estimated to be 70.8 kJ·mol

-1

which is close to the reported value. Compared with EAA

the tensile strength and Young's modulus of EAA-ESO-ZnO increased by 41.8% and 54.5%

respectively. After being reprocessed three times

the tensile strength of EAA-ESO-ZnO increased by 13.8%

and the retention rate of the elongation at break reached 92.0%

demonstrating excellent reprocessing performance. In conclusion

this study proposes an efficient and easily scalable preparation route for polyolefin-based vitrimer with low cost and high performance

providing a new avenue for the preparation of reprocessable cross-linked polyolefins.

关键词

Keywords

references

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