In situ three-roll mill exfoliation approach for fabricating asphalt/graphite nanoplatelet composites as thermal interface materials

Thermal interface materials (TIMs) are vital to dissipate excess heat generated by electronic components with ever-growing power density to ensure their reliability and performance. However, the limited dispersibility of nano-sized thermal conductive fillers hinders further enhancement of thermal conductivity in TIMs. It remains challenging to manufacture high-performance TIMs with simultaneous high thermal conductivity, low cost, and capability of large-scale production. Herein, a solvent-free and scalable approach was adopted to fabricate asphalt/graphite nanoplatelets (GNPs) composites by in situ exfoliating graphite in asphalt melt using a three-roll mill. During exfoliation, asphalt was adsorbed onto the surface of GNPs via π-π interaction and improved their dispersibility. Hence, GNPs formed integrated thermal conductive pathways with reduced interfacial thermal resistance, which significantly improved the thermal conductivity of asphalt/GNP composites. At 25 vol% loading, the asphalt/GNP composite displayed a thermal conductivity of 1.95 W m⁻¹ K⁻¹, showing a 114 % increase compared to the asphalt/commercial GNP (c-GNP) composite prepared by conventional mechanical mixing. Moreover, the heat-resistant and mechanical properties of the asphalt/GNP composites were also enhanced due to the improved filler dispersion and filler-matrix interactions. Thus, the asphalt/GNP composites fabricated by in situ three-roll milling possessed remarkable advantages as TIMs compared with asphalt/c-GNP composites and commercial silicone rubber thermal pads.