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We investigated thermal properties of the epoxy-based composites with a highloading fraction - up to f=45 vol.% - of the randomly oriented electricallyconductive graphene fillers and electrically insulating boron nitride fillers.It was found that both types of the composites revealed a distinctive thermalpercolation threshold at the loading fraction f>20 vol.%. The graphene loadingrequired for achieving the thermal percolation was substantially higher thanthe loading for the electrical percolation. Graphene fillers outperformed boronnitride fillers in the thermal conductivity enhancement. It was establishedthat thermal transport in composites with the high filler loading, above thethermal percolation threshold, is dominated by heat conduction via the networkof percolating fillers. Unexpectedly, we determined that the thermal transportproperties of the high loading composites were influenced strongly by thecross-plane thermal conductivity of the quasi-two-dimensional fillers. Theobtained results shed light on the debated mechanism of the thermalpercolation, and facilitate the development of the next generation of theefficient thermal interface materials for electronic applications.

Thermal Percolation Threshold and Thermal Properties of Composites with Graphene and Boron Nitride Fillers