Thermal Transport in Graphene Oxide – From Ballistic Extreme to Amorphous Limit

Abstract

Graphene oxide is being used in energy, optical, electronic and sensor devices due to its unique properties. However, unlike its counterpart – graphene – the thermal transport properties of graphene oxide remain unknown. In this work, we use large-scale molecular dynamics simulations with reactive potentials to systematically study the role of oxygen adatoms on the thermal transport in graphene oxide. For pristine graphene, highly ballistic thermal transport is observed. As the oxygen coverage increases, the thermal conductivity is significantly reduced. An oxygen coverage of 5% can reduce the graphene thermal conductivity by ~90% and a coverage of 20% lower it to ~8.8 W/mK. This value is even lower than the calculated amorphous limit (~11.6 W/mK for graphene), which is usually regarded as the minimal possible thermal conductivity of a solid. Analyses show that the large reduction in thermal conductivity is due to the significantly enhanced phonon scattering induced by the oxygen defects which introduce dramatic structural deformations. These results provide important insight to the thermal transport physics in graphene oxide and offer valuable information for the design of graphene oxide-based materials and devices.