▎ 摘　　要

Any industrial application aiming at exploiting the exceptional properties of graphene in composites or coatings is currently limited by finding viable production methods for large volumes of good quality and high aspect ratio graphene, few layer graphene (FLG) or graphite nanoplatelets (GNP). Final properties of the resulting composites are inherently related to those of the initial graphitic nanoparticles, which typically depend on time-consuming, resource-demanding and/or low yield liquid exfoliation processes. In addition, efficient dispersion of these nanofillers in polymer matrices, and their interaction, is of paramount importance. Here we show that it is possible to produce graphene/epoxy nanocomposites in situ and with high conversion of graphite to FLG/GNP through the process of three-roll milling (TRM), without the need of any additives, solvents, compatibilisers or chemical treatments. This readily scalable production method allows for more than 5 wt % of natural graphite (NG) to be directly exfoliated into FLG/GNP and dispersed in an epoxy resin. The in situ exfoliated graphitic nanoplatelets, with average aspect ratios of 300-1000 and thicknesses of 5-17 nm, were demonstrated to conferee exceptional enhancements in mechanical and electrical properties to the epoxy resin. The above conclusions are discussed and interpreted in terms of simple analytical models.