Overall Performance Enhancement of Epoxy Resins Loaded with Non-Covalently Modified Carbon Nanotubes and Graphene Nanosheets

In this work, we demonstrate that both carbon nanotubes (CNT) and graphene nanosheets (G) were successfully modified by π-stacking interactions with a pyrene derivative (PY), yielding the functionalized nanofillers CNT-PY and G-PY, which were subsequently dispersed within an aeronautical epoxy matrix. This functionalization is highly effective in preserving the remarkable electronic properties of carbon nanotubes and graphene nanosheets. At the same time, the non-covalent functionalization reduces the resin viscosity, enabling a more effective dispersion of the nanofillers. This results in improved rheological behavior and an overall enhancement of the structural performance of the nanocomposites compared to the resin containing unfunctionalized carbon nanofillers (CNT and G). Additional improvements are also observed in electrical properties, self-healing efficiency, and thermal stability. In particular, the samples containing functionalized carbon nanotubes (TBD + 1%CNT-PY) and functionalized graphene nanosheets (TBD + 1%G-PY) exhibit higher conductivities—0.391 S/m and 0.1 S/m, respectively—than the samples loaded with unfunctionalized carbon nanotubes (TBD + 1%CNT) and unfunctionalized graphene nanosheets (TBD + 1%G), which show conductivity values of 0.292 S/m and 4.82 × 10−3 S/m, respectively. The functionalized graphene nanosheets (G-PY) display significantly greater thermal stability, with degradation temperatures reaching 670 °C, compared to 310 °C for unfunctionalized ones (G). The functionalized carbon nanotubes (CNT-PY) show a 10% weight loss at 520 °C due to the degradation of the pyrene groups. Significant improvements in the final properties can be achieved when carbon-based nanofillers are homogeneously dispersed in the matrix and the external load is efficiently transferred through strong filler–polymer interfacial interactions, leading to composites with superior characteristics suitable for advanced applications. Tunneling Atomic Force Microscopy (TUNA) highlights the morphological features of the two types of carbon nanofillers, their dispersion within the polymer matrix and the effect of the functionalization on the electrical pathways and conductivity of the samples at both the micro- and nanometer-scale. The measured electrical conductivities are consistent with the electric currents detected at the micro/nanoscale.