Epoxy Nanocomposites with Reduced Graphene Oxide-Constructed Three-Dimensional Networks of Single Wall Carbon Nanotube for Enhanced Thermal Management Capability with Low Filler Loading

Thermal management materials are solutions to heat dissipation issues in electronic devices, which are key to the device reliability and lifetime. Epoxy-based materials have been widely used but suffer from their intrinsically low thermal conductivity. In this work, we employ the combined hydrothermal reduction, ice-templated assembly, and vacuum-assisted infiltration methods to construct well-aligned rigid three-dimensional (3D) networks of reduced graphene oxide (RGO) walls bridged by (functional) single wall carbon nanotubes ((f)SWCNTs) in the epoxy resin. The 3D RGO/(f)SWCNT aerogel notably enhances thermal conductivity, reduces the coefficient of thermal expansion (CTE), and increases the glass-transition temperature (Tg) without deteriorating the electrical insulating property. Remarkably, the (RGO/fSWCNT)1:2.5 epoxy nanocomposite reaches a thermal conductivity of 0.63 to 0.69 W m-1 K-1 from 300 to 390 K at a very low filler loading of 3.65 vol %, which is more than four times enhancement over the pure epoxy resin. The CTE decreases by 11.2 ppm K-1 and Tg increases by 20 K. We also show that the functional groups associated with the 3D RGO/fSWCNT aerogel are beneficial for improvement in thermal conductivity, dimensional stability, and thermal stability. The epoxy nanocomposites reported by this work demonstrate strong potential for thermal management application in electronic packaging.