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With the development of microelectronic devices, the insufficient heat dissipation ability becomes one of the major bottlenecks for further miniaturization. Although graphene-assisted epoxy resin (ER) display promising potential to enhance the thermal performances, some limitations of the reduced graphene oxide (RGO) nanosheets and three-dimensional graphene networks (3DGNs) hinder the further improvement of the resulting thermal interface materials (TIMs). In this study, both the RGO nanosheets and 3DGNs are adopted as co-modifiers to improve the thermal conductivity of the ER. The 3DGNs provide a fast transport network for phonon, while the presence of RGO nanosheets enhances the heat transport at the interface between the graphene basal plane and the ER. The synergy of these two modifiers is achieved by selecting a proper proportion and an optimized reduction degree of the RGO nanosheets. Moreover, both the high stability of the thermal conductivity and well mechanical properties of the resulting TIM indicate the potential application prospect in the practical field.   Electronic supplementary material  The online version of this article (10.1186/s11671-017-2298-z) contains supplementary material, which is available to authorized users.

RGO and Three-Dimensional Graphene Networks Co-modified TIMs with High Performances