Microscopic origin of graphene nanosheets derived from coal-tar pitch by treating Al4C3 as the intermediate

Abstract

The development of environmental friendly, simply processed and low cost synthesis methods for graphene nanosheets (GNs) has attracted global interest. In this work, a simple and efficient method to synthesize GNs deriving from coal-tar pitch has been proposed from both experimental and theoretical point of views. The XRD, TEM and Raman results demonstrate that precursor Al₄C₃ could provide a growth environment for the final product of GNs. Innovatively, we have unraveled the microscopic origin for the decomposition of Al₄C₃ based on density functional theory calculations. It is highlighted that the surface energies and elastic constants analysis indicate the fact that the chemical etching process in Al₄C₃ can be happened, which is similar to the exfoliation of well-known transition metal carbides MXenes. Furthermore, different bond breaking mechanisms have been found in Al₄C₃ at applied tensile and shear strains from the electron localization functions and stress-strain results. Our study not only offers an efficient method to synthesize GNs, but also unravel the microscopic mechanism of fabrication by theoretical calculations.