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Functional bio-based vitrimer with excellent healing and recyclability based on conjugated deflection self-toughening
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2023-08-28 , DOI: 10.1016/j.cej.2023.145680
Picheng Chen , Yu Ding , Yanqing Wang , Hongzhe Zhao , Pengcheng Li , Yuetao Liu , Chuanhui Gao

The three-dimensional network crosslinking structure of a vitrimer provides excellent mechanical strength and thermal stability, which are crucial for practical applications. However, achieving a harmonious balance between rigidity and toughness presents coordination difficulties that impede their broad applications. Herein, we propose a new regulatory strategy for high toughness using a functional vitrimer based on vanillin and dihydroxy fatty monoamines. The electron delocalization effect of the conjugated structures was used to coordinate the design of the crosslinking points to adjust the topological transformation temperature of the materials. The conjugate complement of the rigid benzene ring and imine bond caused a shift in the electron cloud distribution in the material, which effectively lowered the energy barrier for the exchange of imine bonds in the crosslinked network. The imine bond dissociation energy decreased from 170.75 to 97.80 kcal/mol compared with the uniform conjugation. The exchange rate of dynamic covalent bonds was accelerated at the same temperature, which is conducive to the functionalization of materials under realistic conditions. The strain in the vitrimer obtained in this study increased significantly under the action of external forces. Furthermore, the crosslinking density of the system was improved using multiple epoxy groups to avoid stress loss. The vitrimer obtained in this study exhibited a tensile strength of 35.6 MPa and an elongation at break of 247.7%. In addition, the synthesized vitrimer showed excellent welding, healing, and shape memory performance.



中文翻译:

基于共轭偏转自增韧的功能性生物基玻璃体,具有优异的愈合性和可回收性

玻璃体的三维网络交联结构提供了优异的机械强度和热稳定性,这对于实际应用至关重要。然而,在刚性和韧性之间实现和谐平衡会带来协调困难,从而阻碍了其广泛应用。在此,我们提出了一种新的高韧性调控策略,使用基于香草醛和二羟基脂肪单胺的功能性玻璃体。利用共轭结构的电子离域效应来协调交联点的设计来调节材料的拓扑转变温度。刚性苯环和亚胺键的共轭互补引起材料中电子云分布的偏移,有效降低了交联网络中亚胺键交换的能垒。与均匀共轭相比,亚胺键解离能从170.75 kcal/mol降低至97.80 kcal/mol。相同温度下动态共价键的交换速率加快,有利于材料在现实条件下的功能化。本研究获得的vitrimer中的应变在外力作用下显着增加。此外,使用多个环氧基团提高了系统的交联密度以避免应力损失。本研究中获得的 vitrimer 的拉伸强度为 35.6 MPa,断裂伸长率为 247.7%。此外,合成的vitrimer表现出优异的焊接、愈合和形状记忆性能。

更新日期:2023-08-30
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