The thermally conductive properties of silicone thermal grease enhanced by hexagonal boron nitride (hBN) nanosheets as a filler are relevant to the field of lightweight polymer-based thermal interface materials. However, the enhancements are restricted by the amount of hBN nanosheets added, owing to a dramatic increase in the viscosity of silicone thermal grease. To this end, a rational structural design of the filler is needed to ensure the viable development of the composite material. Using reduced graphene oxide (RGO) as substrate, three-dimensional (3D) heterostructured reduced graphene oxide-hexagonal boron nitride (RGO-hBN)-stacking material was constructed by self-assembly of hBN nanosheets on the surface of RGO with the assistance of binder for silicone thermal grease. Compared with hBN nanosheets, 3D RGO-hBN more effectively improves the thermally conductive properties of silicone thermal grease, which is attributed to the introduction of graphene and its phonon-matching structural characteristics. RGO-hBN/silicone thermal grease with lower viscosity exhibits higher thermal conductivity, lower thermal resistance and better thermal management capability than those of hBN/silicone thermal grease at the same filler content. It is feasible to develop polymer-based thermal interface materials with good thermal transport performance for heat removal of modern electronics utilising graphene-supported hBN as the filler at low loading levels.

With developments of the electronics industry, more components are being included in electronic devices, which has led to challenges in thermal management. Using reduced graphene oxide embedded with MQ silicone resin (RGO/MQ) nano-aggregates as the composite filler and silicone rubber (SR) as the matrix, a simple approach is designed to prepare RGO/MQ/SR composites. Reduced graphene oxide (RGO) was first used as a substrate for the growth of MQ silicone resin by hybridization, forming sandwich-like micro structured RGO/MQ nano-aggregates successfully. Then, RGO/MQ was integrated into α,ω-dihydroxylpolydimethylsiloxane based on the in situ solvent-free blending method, followed by condensation and vulcanization, fabricating the final RGO/MQ/SR composites. The effective strategy could enhance the adaptability between graphene and silicone matrix under external stimuli at room temperature by embedding nanoscale MQ into the interface of graphene/silicone as the buffer layer. Obvious improvements were found in both thermal conductivity and mechanical properties due to excellent dispersion and interfacial compatibility of RGO/MQ in the host materials. These attractive results suggest that this RGO/MQ/SR composite has potential as a thermal interface material for heat dissipation applications.