Design of Intrinsically Flame-Retardant Vanillin-Based Epoxy Resin for Thermal-Conductive Epoxy/Graphene Aerogel Composites

• Published in: ACS applied materials & interfaces 2021-12, Vol.13 (49), p.59341-59351
• Main Authors: Yang, Weijun, Ding, Hui, Liu, Tianxi, Ou, Rongxian, Lin, Jieying, Puglia, Debora, Xu, Pengwu, Wang, Qingwen, Dong, Weifu, Du, Mingliang, Ma, Piming
• Format: Article
• Language: English
• Subjects: Applications of Polymer, Composite, and Coating Materials
• ISSN: 1944-8244; 1944-8252
• DOI: 10.1021/acsami.1c19727

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.