Thermally Conductive Graphene-Polymer Composites: Size, Percolation, and Synergy Effects

The rapidly increasing device densities in electronics dictate the need for efficient thermal management. If successfully exploited, graphene, which possesses extraordinary thermal properties, can be commercially utilized in polymer composites with ultrahigh thermal conductivity (TC). The total potential of graphene to enhance TC, however, is restricted by the large interfacial thermal resistance between the polymer mediated graphene boundaries. We report a facile and scalable dispersion of commercially available graphene nanoplatelets (GnPs) in a polymer matrix, which formed composite with an ultrahigh TC of 12.4 W/m K (vs 0.2 W/m K for neat polymer). This ultrahigh TC was achieved by applying high compression forces during the dispersion that resulted in the closure of gaps between adjacent GnPs with large lateral dimensions and low defect densities. We also found strong evidence for the existence of a thermal percolation threshold. Finally, the addition of electrically insulating boron-nitride nanoparticles to the thermally conductive GnP-polymer composite significantly reduces its electrical conductivity (to avoid short circuit) and synergistically increases the TC. The efficient dispersion of commercially available GnPs in polymer matrix provides the ideal framework for substantial progress toward the large-scale production and commercialization of GnP-based thermally conductive composites.