High-performance Sustainable Polymer Materials: From Layer-by-layer Assembled Films to Reversibly Crosslinked Polymers

Yi-xuan Li; Jun-qi Sun

doi:10.11777/j.issn1000-3304.2025.25255

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High-performance Sustainable Polymer Materials: From Layer-by-layer Assembled Films to Reversibly Crosslinked Polymers

Feature Article | 更新时间：2025-12-18

- High-performance Sustainable Polymer Materials: From Layer-by-layer Assembled Films to Reversibly Crosslinked Polymers
- Acta Polymerica Sinica Vol. 56, Issue 12, Pages: 2110-2124(2025)
- 作者机构：
  
  吉林大学化学学院超分子结构与材料全国重点实验室长春 130012
- 作者简介：
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2025.25255
  CLC：
- CSTR：32057.14.GFZXB.2025.7508
- Received：03 October 2025，
  
  Accepted：24 October 2025，
  
  Published Online：20 November 2025，
  
  Published：20 December 2025
- 稿件说明：
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李懿轩, 孙俊奇. 高性能可持续聚合物材料：从层层组装膜到可逆交联聚合物. 高分子学报, 2025, 56(12), 2110-2124

Li, Y. X.; Sun, J. Q. High-performance sustainable polymer materials: from layer-by-layer assembled films to reversibly crosslinked polymers. Acta Polymerica Sinica, 2025, 56(12), 2110-2124
李懿轩, 孙俊奇. 高性能可持续聚合物材料：从层层组装膜到可逆交联聚合物. 高分子学报, 2025, 56(12), 2110-2124 DOI： 10.11777/j.issn1000-3304.2025.25255. CSTR： 32057.14.GFZXB.2025.7508.

Li, Y. X.; Sun, J. Q. High-performance sustainable polymer materials: from layer-by-layer assembled films to reversibly crosslinked polymers. Acta Polymerica Sinica, 2025, 56(12), 2110-2124 DOI： 10.11777/j.issn1000-3304.2025.25255. CSTR： 32057.14.GFZXB.2025.7508.

摘要

为了满足现代社会对聚合物材料优异力学性能与稳定性的要求，可持续聚合物材料在保持良好动态性的基础上，还需要具备媲美传统聚合物的力学性能与稳定性，甚至展现出传统聚合物不具备的独特力学性能. 本专论系统地介绍了我们在高性能可逆交联聚合物材料方面的研究进展. 从基于层层组装技术构建的自/可修复可逆交联聚合物膜出发，发展了基于聚合物复合物直接构筑具有自/可修复与可循环利用性的可逆交联塑料、弹性体及凝胶的有效方法，最终提出了基于多种可逆作用力与原位生成的纳米相分离结构的协同制备高性能可逆交联聚合物材料的概念. 通过调控纳米相分离结构的刚性、可变形性与动态解离性，制备了力学强度媲美或优于传统聚合物的可逆交联聚合物材料，还获得了具有独特力学性能的可逆交联聚合物材料，如兼具高强度与极低滞后性的水凝胶/离子凝胶、具有优异抗撕裂与抗损伤性的弹性体以及低温超韧且抗冲击的塑料等. 由于交联网络的可逆性，高性能可逆交联聚合物材料具有优异的修复、重复加工以及解聚回收等性能，为创制高性能可持续聚合物材料提供了全新方法.

Abstract

To address the growing

demands of modern society for polymer materials with high mechanical performance and stability

it is imperative to develop sustainable polymers that combine dynamic functionalities with properties comparable to or exceeding those of traditional polymers. Here

we propose a new concept of reversibly crosslinked polymers (RCPs). RCPs are three-dimensional polymer networks in which polymer chains are reversibly crosslinked through noncovalent interactions and/or dynamic covalent bonds. By constructing RCPs from polymeric building blocks

the fraction of stable covalent bonds relative to reversible interactions is increased

thereby ensuring satisfactory strength and stability. This feature article comprehensively summarizes our advances in designing and fabricating high-performance RCPs. Using a layer-by-layer assembly strategy

we fabricated a series of self-healing/healable RCP films and elucidated their healing mechanisms. Inspired by this method

we further developed an efficient solution-based polymer complexation approach to produce bulk RCPs

extending healability from films to plastics

elastomers

and hydrogels/ionogels. Moreover

we demonstrate that high-performance RCPs can be achieved by combining multiple types of reversible interactions with reinforcement from carefully engineered

in situ

-formed phase-separated nanostructures. By tailoring the rigidity

deformability

and dynamic dissociability of these nanostructures

we obtained RCPs with strengths comparable to or exceeding those of conventional polymers

as well as materials with unique mechanical properties rarely achieved in traditional systems

such as high-strength

low-hysteresis hydrogels/ionogels

damage-resistant elastomers

and ultra-tough plastics with superior low-temperature impact resistance. Importantly

the dynamic nature of the crosslinking network imparts excellent healing

reprocessing

and recycling capabilities to these RCPs. We believe that RCPs open a new avenue for the development of high-performance sustain

able polymers.

关键词

Keywords

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Yu-zhong Wang

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(The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials (MOE), National Engineering Laboratory of Eco-Friendly Polymeric Materials (Sichuan), State Key Laboratory of Advanced Polymer Materials, College of Chemistry, Sichuan University, )

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