Thermally Reduced Graphene Oxide/Carbon Nanotube Composite Films for Thermal Packaging Applications

Thermally reduced graphene oxide/carbon nanotube (rGO/CNT) composite films were successfully prepared by a high-temperature annealing process. Their microstructure, thermal conductivity and mechanical properties were systematically studied at different annealing temperatures. As the annealing temperature increased, more oxygen-containing functional groups were removed from the composite film, and the percentage of graphene continuously increased. When the annealing temperature increased from 1100 to 1400 degrees C, the thermal conductivity of the composite film also continuously increased from 673.9 to 1052.1 W m(-1) K-1. Additionally, the Young's modulus was reduced by 63.6%, and the tensile strength was increased by 81.7%. In addition, the introduction of carbon nanotubes provided through-plane thermal conduction pathways for the composite films, which was beneficial for the improvement of their through-plane thermal conductivity. Furthermore, CNTs apparently improved the mechanical properties of rGO/CNT composite films. Compared with the rGO film, 1 wt% CNTs reduced the Young's modulus by 93.3% and increased the tensile strength of the rGO/CNT composite film by 60.3%, which could greatly improve its flexibility. Therefore, the rGO/CNT composite films show great potential for application as thermal interface materials (TIMs) due to their high in-plane thermal conductivity and good mechanical properties.