We herein report on the preparation of epoxy nanocomposites, which had enhanced thermal conductivities but were still electrical insulators, incorporating hybrid nanosheets (NSs) with sandwich structures composed of thermally reduced graphene oxide (TRGO) and silica. The silica layer covered the surface of the TRGO, hindering electrical conduction and effectively forming a 3D phonon transport channel that had a unique effect on the electrical and thermal properties of the epoxy matrix. A 1 wt% TRGO-silica NS epoxy nanocomposite maintained an electrical resistivity of 2.96 × 10(11)Ω cm, and its thermal conductivity was 0.322 W m(-1) K(-1), which is 61% higher than the conductivity of an epoxy nanocomposite without TRGO-silica NSs (0.2 W m(-1) K(-1)).

Coupling agent-functionalized boron nitride (f-BN) and glycidyl methacrylate-grafted graphene (g-TrG) are simultaneously blended with polyimide (PI) to fabricate a flexible, electrically insulating and thermally conductive PI composite film. The silk-like g-TrG successfully fills in the gap between PI and f-BN to complete the thermal conduction network. In addition, the strong interaction between surface functional groups on f-BN and g-TrG contributes to the effective phonon transfer in the PI matrix. The thermal conductivity (TC) of the PI/f-BN composite films containing additional 1 wt % of g-TrG is at least doubled to the value of PI/f-BN and as high as 16 times to that of the pure PI. The hybrid film PI/f-BN-50/g-TrG-1 exhibits excellent flexibility, sufficient insulating property, the highest TC of 2.11 W/mK, and ultralow coefficient of thermal expansion of 11 ppm/K, which are perfect conditions for future flexible substrate materials requiring efficient heat dissipation.

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A facile technique was developed to improve the water barrier properties of transparent polyimide (PI) films. Transparent and organo‐soluble PI films were synthesized from an alicyclic tetracarboxylic dianhydride (bicyclo[2.2.2]oct‐7‐ene‐2,3,5,6‐tetracarboxylic dianhydride) and an aromatic diamine (3,4′‐oxydianiline) in a co‐solvent of dimethylacetamide (DMAc) and γ‐butyrolactone via a one‐step process. Thermally reduced graphene (RG) was then blended with the PI in DMAc solution to fabricate PI/RG nanocomposite films without the addition of coupling agent. With the incorporation of only 0.1 wt% highly exfoliated RG in the PI matrix, the resultant PI/RG‐0.1 nanocomposite exhibited a superior barrier to moisture and retained high transmittance in the visible light region. The surface of PI/RG was more hydrophobic than that of pure PI and simultaneously the water vapor transmission rate was significantly reduced to 13 g m−2 day−1 for the PI/RG‐0.1 nanocomposite compared to 181 g m−2 day−1 for pure PI. Notably, the PI/RG‐0.1 nanocomposite also exhibited favorable thermal stability with a lower coefficient of thermal expansion and a higher thermal degradation temperature compared to pure PI. The easy processing of PI solution and RG nanosheets, the good orientation of RG in PI and the excellent barrier and thermal properties of PI/RG make the transparent PI nanocomposite films potential substrate materials in flexible electronic applications.

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