No abstract

A strategy of electrostatic self-assembly and two-step synergism was proposed to significantly improve the thermal conductivity of the PI composite film.

The accumulation of heat in electronic devices puts forward an urgent demand for thermal interface materials. It is still a great challenge to achieve the good comprehensive performance of high thermal conductivity (TC), insulation, flexibility and tensile strength. In this work, polyester‐based nonwoven fabric (NWF) was coated with boron nitride nanosheets (BNNS) by dispersion and interfacial reinforcement of cellulose nanofibers to obtain a three‐dimensional thermally conductive network skeleton (BNNS@NWF). The sandwich‐structured composite film was assembled by introducing alumina (Al2O3)/polydimethylsiloxane (PDMS) layers on the top and bottom surfaces of BNNS@NWF using scratch coating and hot pressing processes. The composite film has a high TC of 6.42 W/mK at 45.8 wt% BNNS content, and has excellent insulation with a volume resistivity of 1.06 × 1015 Ω cm. This is due to the long‐range effective thermal conduction path constructed by BNNS, the bridging effect of Al2O3 and the synergistic effect of the two fillers. PDMS helps the composite film maintain good flexibility and good TC stability after 30 bending cycles. The PET nonwoven interlayer gives the composite film good mechanical properties with a tensile strength of 17.5 MPa. This work provides a strategy for the efficient preparation of flexible composite films with high TC and insulation properties, which is of great importance for the development of innovative thermal interface materials.Highlights A sandwich‐structured composite film was prepared by a simple scale‐up method. Al2O3 and BNNS achieves synergistic enhancement of thermal conductivity. The film has a high thermal conductivity of 6.42 W/mK and electrical insulation. The film shows good flexibility, high tensile and thermal management properties.