Yang Weijun, Ding Hui, Liu Tianxi, Ou Rongxian, Lin Jieying, Puglia Debora, Xu Pengwu, Wang Qingwen, Dong Weifu, Du Mingliang, Ma Piming
The Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China.
Key Laboratory for Biobased Materials and Energy of Ministry of Education, College of Materials and Energy, South China Agricultural University, Guangzhou 510642, China.
ACS Appl Mater Interfaces. 2021 Dec 15;13(49):59341-59351. doi: 10.1021/acsami.1c19727. Epub 2021 Dec 3.
Vanillin, as a lignin-derived mono-aromatic compound, has attracted increasing attention due to its special role as an intermediate for the synthesis of different biobased polymers. Herein, intrinsically flame-retardant and thermal-conductive vanillin-based epoxy/graphene aerogel (GA) composites were designed. First, a bifunctional phenol intermediate (DN-bp) was synthesized by coupling vanillin with 4, 4'-diaminodiphenylmethane and DOPO, and the epoxy monomer (MEP) was obtained by the epoxidation reaction with DN-bp and epichlorohydrin. Then, various amounts of MEP and diglycidyl ether of bisphenol A (DER) were mixed and cured. Interestingly, the flexural strength and modulus were greatly enhanced from 72.8 MPa and 1.3 GPa to 90.3 MPa and 2.8 GPa, respectively, at 30 wt % MEP, due to the rigidity of MEP and strong intermolecular N-H hydrogen bonding interactions. Meanwhile, the cured epoxy achieved a UL-94 V0 rating with a low P content of 1.06%. The flame-retardant vanillin-based epoxy was then impregnated into the thermal conductive 3D GA networks. The obtained epoxy/graphene composite showed excellent flame retardancy and thermal conductivity [λ = 0.592 W/(m·K)] with only 0.5 wt % graphene in the system. Based on these results, we believe that this work would represent a novel solution for the preparation of high-performance biobased flame-retardant multipurpose epoxies.
香草醛作为一种木质素衍生的单芳族化合物，因其作为合成不同生物基聚合物的中间体的特殊作用而受到越来越多的关注。在此，设计了具有本征阻燃性和导热性的香草醛基环氧/石墨烯气凝胶（GA）复合材料。首先，通过香草醛与4,4'-二氨基二苯甲烷和9,10-二氢-9-氧杂-10-磷杂菲-10-氧化物（DOPO）偶联合成了双功能酚中间体（DN-bp），并通过DN-bp与环氧氯丙烷的环氧化反应得到环氧单体（MEP）。然后，将不同量的MEP和双酚A二缩水甘油醚（DER）混合并固化。有趣的是，由于MEP的刚性和强烈的分子间N-H氢键相互作用，在30 wt% MEP时，弯曲强度和模量分别从72.8 MPa和1.3 GPa大幅提高到90.3 MPa和2.8 GPa。同时，固化后的环氧树脂达到了UL-94 V0等级，磷含量低至1.06%。然后将阻燃性香草醛基环氧树脂浸渍到导热的三维GA网络中。所制备的环氧/石墨烯复合材料在体系中仅含0.5 wt%石墨烯时就表现出优异的阻燃性和导热性[λ = 0.592 W/(m·K)]。基于这些结果，我们认为这项工作将为制备高性能生物基阻燃多功能环氧树脂提供一种新的解决方案。
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