Interfacial Compatibility of Core-Shell Cellulose Nanocrystals for Improving Dynamic Covalent Adaptable Networks' Fracture Resistance in Nanohybrid Vitrimer Composites

The development of polymeric nanocomposites with dynamic covalent adaptable networks and biobased nanomaterials has been a promising approach toward sustainable advanced materials, enabling reprogramming and recycling capabilities. Herein, a core-shell nanohybrid of functionalized cellulose nanocrystals (CNCs) is explored to provide crucial interfacial compatibility for improving the covalent adaptable networks of epoxy-thiol vitrimers in fracture resistance. The poly(e-caprolactone) (PCL) shells grafted from CNC surfaces can be cross-linked with the covalent adaptable networks via a hot-pressing transesterification process. According to the additive concentration and annealing temperature, the stress relaxation behavior of nanohybrid vitrimer composites can be effectively regulated by the core-shell PCL-grafted CNC (CNC-PCL) nanohybrids from a dispersed to cross-linked interaction. The addition of 15 wt % of the core-shell CNC-PCLs exhibits the reinforced improvement of nanohybrid vitrimer composites in the average Young's modulus of 2.5x, fracture stress of 5.4x, and fracture strain of 2.0x. The research findings might have profound implications for developing synergistic interfacial compatibility between dynamic vitrimer networks and functional nanoparticles for advanced polymeric nanocomposites.