High Yield Controlled Synthesis of Nano-Graphene Oxide by Water Electrolytic Oxidation of Glassy Carbon for Metal-Free Catalysis

The strong quantum confinement effect as well as abundant edges and oxygen functional groups enable nano-graphene oxide (NGO) a variety of intriguing applications such as catalysis, bioimaging, drug delivery and photovoltaic devices. However, the development of NGO is severely hindered because of the difficulty in controlled mass production. Here, we report the efficient synthesis of NGO with a high yield of ∼40 wt % by water electrolytic oxidation of glassy carbon (GC). The NGO shows a high oxidation degree (C/O atomic ratio, ∼1.4) and excellent dispersion stability. Moreover, its size can be easily tuned by the graphitization degree of GC, which enables the controlled synthesis of NGO with average size of 4, 8, and 13 nm and different oxygen functional groups. As metal-free catalysts, the 13 nm sized NGO is found to be beneficial for the oxidative coupling reaction of benzylamine, while the 4 nm sized NGO shows a conversion rate of 88 times higher than 13 nm sized NGO for the oxidation reaction of benzene. In addition, the water electrolytic oxidation mechanism of graphitic materials is systematically studied. It is found that sulfuric acid has a protective effect on the graphite electrode during the water electrolytic oxidation process, and 50 wt % sulfuric acid solution well balances the protection and oxidation processes, leading to the highest oxidation efficiency and production rate.