Abstract

To develop thermal interface materials with both high thermal conductivity and electromagnetic interference shielding, the polyvinylidene fluoride (PVDF) composite film was prepared by electrospinning and hot-pressing, using strategies of multi-layered structure and two fillers synergy of nickel modified carbon nanotube (Ni-CNT) and Al2O3 microspheres. The composite film consisted of a Ni-CNT filled PVDF electrospun fiber film as the top and bottom surface layers, and a PVDF electrospun fiber film electrostatically adsorbing Al2O3 microspheres and surface-sprayed with Ni-CNT as the middle layer. At a 20 wt% Ni-CNT in the surface layers and a 16.7 wt% Al2O3 and 5 wt% Ni-CNT in the middle layer, the composite film with a thickness of 0.1 mm exhibited optimal performances with electromagnetic wave shielding efficiency of 65 dB in the frequency range of 8.2–12.4 GHz, with 86% of the electromagnetic waves being absorbed. At the same time, the composite film had a high in-plane thermal conductivity of 4.02 W m−1 K−1, while maintaining a tensile strength of 25 MPa and flexibility.

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