Synergetic Hybridization Strategy to Enhance the Dynamicity of Poorly Dynamic CO2-derived Vitrimers achieved by a Simple Copolymerization Approach

Copolymerization allows tuning polymer's properties and a synergetic effect may be achieved for the resulting hybrid, i.e., outperforming the properties of its parents as often observed in natural materials. This synergetic concept is herein applied to enhance both dynamicity and properties of vitrimeric materials using poorly dynamic hydroxyurethane and non-dynamic epoxy thermosets. The latter generates activated hydroxyl, promoting exchange reactions 15 times faster than pure polyhydroxyurethanes. This strategy allows obtaining catalyst-free high-performance vitrimers from conventional epoxy-amine formulations and an easily scalable (bio-)CO2-based yet poorly efficient dynamic network. The resulting hybrid network exhibits modulus retention superior to 95% with fast relaxation (<10 min). The hydroxyurethane moieties actively participate in the network to enhance the properties of the hybrid. The material can be manufactured as any conventional epoxy formulation. This new strategy to design dynamic networks opens the door to large-scale circular high-performance structural carbon fiber composites (CFRP). The CFRP can be easily reshaped and welded from flat plates to complex geometries. The network is degradable under mild conditions, facilitating the recovery and re-use of high-added-value fibers. This accessible and cost-effective approach provides a versatile range of tunable dynamic epoxides, applicable across various industries with minimal adjustments to existing marketed products.