Sulfite activation by N-doped reduced graphene oxide for As(III) oxidation: Synthesis, efficiency, and mechanisms

Abstract

As a metal-free alternative, graphene-based catalysts have attracted increasing attention for minimizing the risk of heavy metal exposure. In this study, a nitrogen–doped reduced graphene oxide (N-rGO) material was synthesized by a one–pot hydrothermal method using dicyandiamide as the precursor. N-rGO has been adopted for sulfite activation for the first time, to our knowledge. The established N–rGO/sulfite system could effectively remove As(III) in water, and the solution pH and dissolved oxygen were the most important factors affecting the removal. The results of density functional theory calculations indicated that sulfite activation was more likely to occur on C atoms adjacent to the N dopant. It was inferred that the generated hydroxyl radical (HO•) played a vital role in As(III) oxidation. In addition, the conversion of pyridinic nitrogen to pyrrolic nitrogen was responsible for the poor long–term stability of N-rGO. These results demonstrated that N-rGO was a promising catalyst for water treatment.