High-Performance Recyclable and Malleable Epoxy Resin with Vanillin-Based Hyperbranched Epoxy Resin Containing Dual Dynamic Bonds

Dynamic covalent polymer networks represent new opportunities in the design of sustainable epoxy resins due to their excellent malleability and reprocessability; however, the adaptable network is usually accompanied by low glass transition temperature, poor creep resistance, and mechanical brittleness. Herein, we demonstrate a vanillin-based hyperbranched epoxy resin (VEHBP) containing disulfide and imine dynamic covalent bonds for recyclable and malleable epoxy resin with high glass transition temperature (Tg), significantly improved creep resistance, and mechanical properties. The dynamic covalent epoxy resin containing 5%VEHBP exhibited a high glass transition temperature of 175 °C and a creep temperature of 130 °C and a 34.1, 19.7, and 173.3% increase in tensile strength, storage modulus, and tensile toughness respectively, compared with the neat resin. Meanwhile, the hyperbranched topological structure of VEHBP complemented by dual dynamic bonds endowed these materials with excellent self-healing ability, reprocessability, and degradability, which represents an important step toward the design and fabrication of high-performance epoxy covalent adaptable networks.