Elucidating the Mechanism of Nitrogen Doping in Graphene Oxide: Structural Evolution of Dopants and the Role of Oxygen

Doping graphene oxide is a cost-effective method of producing materials that combines novel properties with graphene-like stability, conductivity, and surface area. Nitrogen-doped graphene (oxide) has emerged as an important material for various applications; however, the doping mechanism of nitrogen into a graphene (oxide) lattice is ill-understood. In this work, using a combined reactive molecular dynamics (MD) and experimental approach, we aim to elucidate this mechanism. MD simulations are able to provide an unbiased atomistic mechanism of nitrogen association that is oxide environment- and dopant-dependent. These results are correlated to experiments via spectroscopic characterization on corresponding experimentally annealed samples. Overall, a good correlation between experimental and computational analyses strengthens the validity of mechanisms derived from simulations.