Vanillin-derived multifunctional reinforcing agent enabling recyclable epoxy vitrimer composites via hydrogen/dynamic covalent collaborative networks

IF 7.4 2区化学 Q1 POLYMER SCIENCE

Polymer Degradation and Stability Pub Date : 2025-08-15 DOI:10.1016/j.polymdegradstab.2025.111608

Kai Dong, Di Zhao, Yang Pang, Chengji Zhao

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引用次数: 0

Abstract

Epoxy vitrimers impart dynamic functionality to thermoset polymers and carbon fiber-reinforced composites (CFRC) through reversible crosslinking networks. However, this often results in reduced stability and a trade-off between dynamic performance and mechanical strength. Herein, a novel reinforcing agent (Bio-based Vanillin-Tyramine, BVT) containing Schiff base and tetraphenol hydroxyl groups was synthesized to address this challenge. The incorporation of BVT constructs the hierarchical crosslinking networks that simultaneously enhance the strength and toughness of bio-based vitrimers (Tensile strength and impact strength were increased by 44 % and 225 %, respectively.). The synergistic effect of dual dynamic imine and siloxane bonds further optimizes dynamic behaviors, resulting in a 51 s stress relaxation time and a 14 % decrease in activation energy for the dynamic bond exchange reaction. In addition, CFRC containing dynamic crosslinked networks demonstrate closed-loop recyclability under mild conditions, preserving the surface morphology and chemical structure of recovered carbon fibers, while maintaining the crosslinking architecture of the recycled vitrimer for reshaping. This work presents a simple and efficient strategy for constructing hybrid hydrogen-bonding/covalent adaptable networks, providing valuable insights into the development of high-performance, multifunctional, and recyclable bio-based epoxy vitrimers and CFRC.

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香草素衍生的多功能增强剂通过氢/动态共价协同网络实现可回收的环氧玻璃体复合材料

环氧玻璃体通过可逆交联网络赋予热固性聚合物和碳纤维增强复合材料（CFRC）动态功能。然而，这通常会导致稳定性降低，并在动态性能和机械强度之间进行权衡。为此，我们合成了一种含有希夫碱和四酚羟基的新型补强剂（生物基香兰素酪胺，BVT）。BVT的加入构建了分层交联网络，同时提高了生物基玻璃体的强度和韧性（拉伸强度和冲击强度分别提高了44%和225%）。双动态亚胺键和硅氧烷键的协同作用进一步优化了动态行为，使得动态键交换反应的应力松弛时间为51 s，活化能降低14%。此外，含有动态交联网络的CFRC在温和条件下表现出闭环可回收性，保留了回收碳纤维的表面形态和化学结构，同时保持了再生玻璃体的交联结构以进行重塑。这项工作提出了一种简单有效的构建氢键/共价自适应杂化网络的策略，为高性能、多功能、可回收的生物基环氧树脂和CFRC的发展提供了有价值的见解。

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来源期刊

Polymer Degradation and Stability 化学-高分子科学

CiteScore

10.10

自引率

10.20%

发文量

325

审稿时长

23 days

期刊介绍： Polymer Degradation and Stability deals with the degradation reactions and their control which are a major preoccupation of practitioners of the many and diverse aspects of modern polymer technology. Deteriorative reactions occur during processing, when polymers are subjected to heat, oxygen and mechanical stress, and during the useful life of the materials when oxygen and sunlight are the most important degradative agencies. In more specialised applications, degradation may be induced by high energy radiation, ozone, atmospheric pollutants, mechanical stress, biological action, hydrolysis and many other influences. The mechanisms of these reactions and stabilisation processes must be understood if the technology and application of polymers are to continue to advance. The reporting of investigations of this kind is therefore a major function of this journal. However there are also new developments in polymer technology in which degradation processes find positive applications. For example, photodegradable plastics are now available, the recycling of polymeric products will become increasingly important, degradation and combustion studies are involved in the definition of the fire hazards which are associated with polymeric materials and the microelectronics industry is vitally dependent upon polymer degradation in the manufacture of its circuitry. Polymer properties may also be improved by processes like curing and grafting, the chemistry of which can be closely related to that which causes physical deterioration in other circumstances.