Next-Generation Sustainable Composites with Flax Fibre and Biobased Vitrimer Epoxy Polymer Matrix

This work presents the development of two vanillin-based vitrimer epoxy flax fibre-reinforced composites, with both the VER1-1-FFRC (a vitrimer-to-epoxy ratio of 1:1) and VER1-2-FFRC (a vitrimer-to-epoxy ratio of 1:2), via a vacuum-assisted resin infusion. The thermal and mechanical properties of the resulting vitrimer epoxy flax composites were characterised using thermal gravimetric analysis (TGA), differential scanning calorimetry (DSC), dynamic mechanical analysis (DMA), and mechanical four-point bending tests, alongside studies of solvent resistance and chemical recyclability. Both the VER1-1-FFRC (degradation temperature T_deg of 377.0 °C) and VER1-2-FFRC (T_deg of 395.9 °C) exhibited relatively high thermal stability, which is comparable to the reference ER-FFRC (T_deg of 396.7 °C). The VER1-1-FFRC, VER1-2-FFRC, and ER-FFRC demonstrated glass transition temperatures T_g of 54.1 °C, 68.8 °C, and 83.4 °C, respectively. The low T_g of the vitrimer composite is due to the low crosslink density in the vitrimer epoxy resin. Particularly, the crosslinked density of the VER1-1-FFRC was measured to be 319.5 mol·m^-3, which is lower than that obtained from the VER1-2-FFRC (434.7 mol·m^-3) and ER-FFRC (442.9 mol·m^-3). Furthermore, the mechanical properties of these composites are also affected by the low crosslink density. Indeed, the flexural strength of the VER1-1-FFRC was found to be 76.7 MPa, which was significantly lower than the VER1-2-FFRC (116.2 MPa) and the ER-FFRC (138.3 MPa). Despite their lower thermal and mechanical performance, these vitrimer composites offer promising recyclability and contribute to advancing sustainable composite materials.