Modeling Nanostructure in Graphene Oxide: Inhomogeneity and the Percolation Threshold

Abstract

Graphene oxide (GO) is an amorphous 2D material, which has found widespread use in the fields of chemistry, physics, and materials science due to its similarity to graphene with the benefit of being far easier to synthesize and process. However, the standard of GO characterization is very poor because its structure is irregular, being sensitive to the preparation method, and it has a propensity to transform due to its reactive nature. Atomistic simulations of GO are common, but the nanostructure in these simulations is often based on little evidence or thought. We have written a computer program to generate graphene oxide nanostructures for general purpose atomistic simulation based on theoretical and experimental evidence. The structures generated offer a significant improvement to the current standard of randomly placed oxidized functional groups and successfully recreate the two-phase nature of oxidized and unoxidized graphene domains observed in microscopy experiments. Using this model, we reveal new features of GO structure and predict that a critical point in the oxidation reaction exists as the oxidized region reaches a percolation threshold. Even by a conservative estimate, we show that, if the carbon to oxygen ratio is kept above 6, a continuous aromatic network will remain, preserving many of graphene’s desirable properties, irrespective of the oxidation method or the size distribution of graphene sheets. This is an experimentally achievable degree of oxidation and should aid better GO synthesis for many applications.