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With a trend of continuing improvement in the development of electronic devices, a problem of serious heat accumulation has emerged which has created the need for more efficient thermal management. Graphene sheets (GNS) have drawn much attention with regard to heat transfer because of their excellent in-plane thermal conductivity; however, the ultrahigh interfacial thermal resistance between graphene lamellae has seriously restricted its practical applications. Herein, we describe heat transfer membranes composed of graphene which have been modified by intrinsic thermally conductive polymers with different molecular weights. The presence of macromolecular surface modifiers not only constructed the graphene heat transfer interface by π–π interactions, but also significantly enhanced the membranes’ in-plane thermal conductivity by utilizing their intrinsic heat transfer properties. Such results indicated that the in-plane thermal conductivity of the fabricated membrane exhibits a high in-plane thermal conductivity of 4.17 W m −1  K −1 , which, containing the GNS modified with 6000 g/mol (M n ) of poly(3-hexylthiophene) (P3HT), was 26 times higher that of poly (vinylidene fluoride) (PVDF). The P3HT molecular chain with specific molecular weight can form more matching structure π–π interactions, which promotes thermal conductivity. The investigation of different molecular weights has provided a new pathway for designing effective interfacial structures to relieve interface thermal resistance in thermally conductive membranes.

Interfacial Modulation of Graphene by Polythiophene with Controlled Molecular Weight to Enhance Thermal Conductivity