In this paper, a non-covalent π–π interaction between graphene nanoparticles (G) and a pyrene-based molecule (py) has been successfully accomplished to give the functionalized nanofillers (G-py). The proposed modification has proven to be a winning solution aimed at safeguarding the graphene’s notable electronic properties, while promoting a more effective nanofiller dispersion attributable to a decrease in viscosity with consequent improvement of the rheological properties of the formulated nanocomposites filled with G-py. The electrical current maps of the G-py based epoxy composites, loaded with filler weight percentages both above and below the electric percolation threshold (EPT), were obtained by tunneling atomic force microscopy (TUNA) technique. The possibility to detect low currents also for the sample at lower concentration (0.1 wt%) confirms the good electrical performance of the nanocomposites and, consequently, the successful performed functionalization. The non-covalent modification significantly improves the thermal stability of the unfunctionalized G of about 70 °C, thus causing an increase in the composite oxidative thermostability since the evolution of CO2 shifts to higher values. Moreover, non-covalent functionalization proved to be impactful in imparting an overall enhancement of the nanocomposite mechanical properties due to good bonding between graphene and epoxy matrix, also showing a greater roughness which is decisive in influencing the interface adhesion efficiency.
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