Preparation of high-performance thermosetting resins via bio-based resources is important for the development of a sustainable world. In this work, we proposed the introduction of cyanide structure groups into the molecular structure of epoxy resins to give them excellent heat resistance. A eugenol-based epoxy-phthalonitrile (EEPN) resin was synthesized by a two-step process using the bio-based renewable resource of eugenol, and a series of EEPN/Epoxide resin (E51) blend resins with different EEPN contents were prepared. The structure of the EEPN monomer was characterized and confirmed by Fourier transform infrared (FTIR), nuclear magnetic resonance (NMR), and elemental analysis. The thermal stability and dynamic mechanical properties of the cured resins were investigated by thermogravimetric analysis and dynamic mechanical thermal analysis. The experimental results showed that EEPN had excellent heat resistance; the char yield at 800 °C was 67.9 wt%, which was much higher than that of E51 at 26.3 wt%; and the heat resistance of the blended resins was significantly improved with the increase in the EEPN content.
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