Effective hole conductivity in nitrogen-doped CVD-graphene by singlet oxygen treatment under photoactivation conditions

Abstract

Abstract Nitrogen substitutional doping in the π-basal plane of graphene has been used to modulate the material properties and in particular the transition from hole to electron conduction, thus enlarging the field of potential applications. Depending on the doping procedure, nitrogen moieties mainly include graphitic-N, combined with pyrrolic-N and pyridinic-N. However, pyridine and pyrrole configurations of nitrogen are predominantly introduced in monolayer graphene:N lattice as prepared by CVD. In this study, we investigate the possibility of employing pyridinic-nitrogen as a reactive site as well as activate a reactive center at the adjacent carbon atoms in the functionalized C–N bonds, for additional post reaction like oxidation. Furthermore, the photocatalytic activity of the graphene:N surface in the production of singlet oxygen (1O2) is fully exploited for the oxidation of the graphene basal plane with the formation of pyridine N-oxide and pyridone structures, both having zwitterion forms with a strong p-doping effect. A sheet resistance value as low as 100 Ω/□ is reported for a 3-layer stacked graphene:N film.