Vanillin-Based Epoxy Vitrimer with High Performance and Closed-Loop Recyclability

It is of great importance to develop epoxy vitrimers with the combination of high performance and versatile recyclability. Herein, two imine-containing hardeners were synthesized from bio-based vanillin and petroleum-based p-hydroxy benzaldehyde. The epoxy resins cured by these two hardeners show high Tg (>120 °C), tensile strength (>60 MPa), Young’s modulus (>2500 MPa), and good solvent resistance. Owing to the incorporation of imine dynamic covalent bond, the cured epoxy resins are reprocessable and degradable. Notably, the chemical degradation products can be reused to prepare new epoxy resins, thus achieving a closed-loop recycling process. Both the reprocessed and chemically recycled epoxy resins exhibit high-percentage retention of thermal and mechanical properties. Finally, this study demonstrates that the epoxy resin cured by the vanillin-based hardener shows comparable thermal, mechanical, and recycling properties compared with the epoxy resin cured by the petroleum-based counterpart.