A novel biobased epoxy vitrimer (Gte-VA) with desirable mechanical properties was synthesized from glycerol triglycidyl ether (Gte) and an imine-containing hardener (VA), which was also a biobased compound from vanillin and 4aminophenol. The biobased epoxy vitrimer shows Young's modulus of 1.6 GPa and tensile strength of 62 MPa, which is close to the value of amine-cured bisphenol A diglycidyl ether. In addition, it shows excellent reprocessability, recyclability, and UV shielding performance and can be used as a matrix to prepare carbon fiber (CF)-reinforced composites. Based on the amine− imine reversible exchange reaction of the imine bonds, the CF fabric could be recycled without damage from the composite, after degrading the resin in an amine solution. Especially, after recombining the degraded resin with recycled carbon fiber fabric, a regenerated carbon fiber reinforced composite with similar mechanical properties to the original composite can be obtained, achieving full recycling of the carbon fiber reinforced composite. This work will open a door to the development of simple procedures of high-performance biobased epoxy vitrimer and its application in fully recycled carbon fiber reinforced composite.

The substitution of petroleum-based self-healing elastomers with biobased counterparts is crucial to the global sustainable development of the rubber industry, which highly depends on the ease of the synthesis procedure. Herein, we show that highly stretchable, recyclable, and self-healable biobased elastomers were synthesized via condensation polymerization of succinic acid, adipic acid, sebacic acid, and 1,4-butanediol in the presence of a small amount of glycerol as a curing agent and 3,3′-dithiodipropionic acid as a dynamic covalent monomer. The macroscopic properties of our elastomers, including thermal, mechanical, stress relaxation, and self-healing performance, were finely regulated via microscopic chemical and topological structure. As such, a highly stretchable (up to ∼1700%), recyclable (almost without degradation of the mechanical performance over several repeats), rapid room temperature self-healable (in 20 min) biobased vitrimeric elastomer was achieved, which is the first aliphatic disulfide metathesis assisted self-healing polymer achieved at such low temperatures. The ease of the polycondensation with which the elastomers can be readily scaled up points to exciting opportunities for sustainable polymers with minimal environmental impact.