Thermal interface materials (TIMs) play an irreplaceable role in highly integrated microelectronic devices. In this work, the addition of acidified carbon nanotubes modified by 3-aminopropyl triethoxysilane (KH550) had an effective enhancement to the thermal conductivity, thermal stability, and electrical insulation performance of silicone grease. On this basis, multi-filled silicone grease composites with better thermal conductivity and electrical insulation were prepared by introducing zinc oxide (ZnO) and Graphene nanoflakes (GNFs). The thermal conductivity of silicone grease achieved 1.438 W m−1 K−1, while the volume resistivity still exceeded 1013 Ω·cm. Additionally, the study explored the impact of varying filler parameters, temperature, and contact pressure on the interface thermal contact resistance of silicone grease. The best performance silicone grease applied to the cooling of the high-power LED exhibited excellent heat dissipation. This work presented a reference for the design and development of low cost, high performance TIMs.
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