Repairable, Degradable and Recyclable Carbon Fiber-Reinforced Bio-Based Epoxy Vitrimer Composites Enabled by Facile Transesterification

Developing high-performance bio-based epoxy resins as sustainable alternatives to petroleum-derived bisphenol A (BPA) epoxies for recyclable carbon fiber-reinforced polymers (CFRPs) is pivotal in materials research. Herein, the bio-based bisphenol monomer BDEF was synthesized from the lignin derivative 4-propylguaiacol. The derived epoxy monomer BDEF-EP was cured with adipic acid to form a bio-based vitrimer. Stress relaxation synergistically accelerates through intrinsic dynamic carboxylic acid ester exchange and enhanced chain mobility from the flexible propyl structure. At 220 °C, this vitrimer shows rapid stress relaxation (τ* < 30 s) and repairs ~90% of surface scratches in 30 min. It exhibits tensile and flexural strengths of 69 MPa and 105 MPa, respectively. BDEF-EP's low viscosity reduces diluent needs in composite fabrication, lowering costs and improving efficiency. The resulting bio-based CFRP achieves tensile and flexural strengths of 543 MPa and 414 MPa, respectively, which are comparable to commercially available petroleum-derived CFRP. In addition, CFRP containing dynamic crosslinked networks demonstrates degradable recyclability in ethylene glycol solvent, preserving the surface morphology and chemical structure of recovered carbon fibers. The results demonstrate that this bio-based epoxy vitrimer has promising potential for developing sustainable, degradable, and recyclable CFRP composites.