Small-Nanostructure-Size-Limited Phonon Transport within Composite Films Made of Single-Wall Carbon Nanotubes and Reduced Graphene Oxides

Nanocarbon materials have been widely used for nanoelectronics and energy-related applications. In this work, composite films consisting of reduced graphene oxides (rGOs) and single-wall carbon nanotubes (SWCNTs) are synthesized and studied for their in-plane thermal conductivities. Different from pristine carbon nanotubes or graphene with decreased thermal conductivities above 300 K, the in-plane thermal conductivities of these composite films are found to follow the trend of the specific heat of graphene from 100 to 400 K, i.e., monotonously increasing at elevated temperatures. Such a trend can often be found within amorphous solids but has seldom been observed for nanocarbon. This unique temperature dependence of thermal conductivities is attributed to the largely restricted phonon mean free paths within the graphene sheets that mainly contribute to the in-plane thermal transport. The highest in-plane thermal conductivity among samples with different synthesis conditions is 62.8 W/(m·K) at 300 K. Such a high thermal conductivity, combined with its unique temperature dependency, can be ideal for applications such as flexible film-like thermal diodes based on the junction between two materials with a large contrast for their temperature dependence of the thermal conductivity.