Precursor Controlled Strategy for N, S, F-Reduced Graphene Oxide (RGO) Preparation and Its Electro-Degradation Toward Bisphenol A

Abstract

The performance of electrocatalytic-oxidation process depends on the anode characteristics, so the preparation of active anode materials is an attractive method to enhance the efficiency of this process. However, the high catalytic properties of graphene and its derivatives have been well confirmed, an efficient method of controlling catalytic activity and stability remains to be established. In this research, the relationship between the precursor and catalytic performance was clarified by regulating the oxygen-containing groups in the precursor. Results indicated that the surface O groups on the precursor were sensitive to controlling the catalytic activity and stability of tri-doped reduced graphene oxide (RGO). With more O groups in the precursor (catalysts from graphene oxide), the doped heteroatom species is vulnerable involved into reaction, leading to the flaking of active sites, and ultimately decreasing the activity and stability performance. By contrast, the fewer O groups in the precursor (catalysts from RGO) created stable and active defects for oxidation activity. The interactions of O groups in the C precursor with those in the heteroatom precursor were further confirmed by DFT calculations. The findings of this research presented a new strategy for controlling the stability and performance of the resulting catalysts. DEME-TFSI-coated GO and GN are first formed via covalent bonds through functional groups (O groups) on the graphene surface, non-covalent ionic bonds, and π–π stacking interactions. In this step, N, S, and F groups are weakly bonded with graphene. Stable pyridine and pyrrole structures could then be generated via dehydration and decarbonylation under a controlled temperature and pressure in the hydrothermal process. Finally, cyclization rearrangement is carried out to form graphite with a tri-doped structure.