Sustainable Self-Healing Thermosetting Polymers from Renewable Carvone-Derived Diepoxides

Conventional epoxy thermosets are typically synthesized from toxic and nonrenewable petroleum-derived resources. Their permanent cross-linked networks make them difficult to reprocess or recycle, posing significant environmental challenges. In this study, we report the development of a series of fully biobased thermosetting polymers derived from carvone, a renewable terpenoid compound. A series of carvone-derived monomers were synthesized and oxidized to obtain diepoxide derivatives. These epoxides were subsequently cured with glutaric anhydride in the presence of imidazole, yielding four distinct fully biobased thermosetting polymers. Mechanical characterization revealed that the polymer containing hydroxyl functionalities exhibited the best overall performance. Notably, this hydroxyl-containing thermoset demonstrated excellent crack-healing capabilities without the need for additional catalysts. Our results present a renewable, environmentally friendly platform for the development of self-healing epoxy thermosets derived from natural terpenes.