▎ 摘　　要

Density functional theory is employed to model the chemisorption of ammonia on epoxy-containing polycyclic aromatic hydrocarbons (PAHs) and understand the reaction mechanism of ammonia addition on partially reduced graphene oxide flakes. Coronene (C24H12) and ovalene (C32H14) based four-epoxy group containing molecules are used to mimic the RGO surface properties. The reaction mechanism changing effect of a second ammonia molecule as well as explicit water molecules is considered. The proposed reaction mechanism consists of two steps: the migration of one epoxy group out of the modelled four-epoxy group formation to a thermodynamically less stable one and the nucleophilic addition of the ammonia molecule. The second step involves forming an amine group and reducing an epoxy group to a hydroxyl one. Interestingly, the forming amine group bonds to the carbon atom with the smallest bond order among the available ones and not necessarily to the carbon atom of the opening epoxy ring. Incorporating a second ammonia molecule has a negligible effect on the overall reaction mechanism, while in the presence of one water molecule, the reaction goes through a different pathway involving a trimolecular state during the nucleophilic addition. Including more than one water molecule or applying an implicit solvent model does not cause further changes in the reaction.