Carbon materials are effective catalysts to activate peroxymonosulfate (PMS) for organic pollutants degradation. Both nitrogen doping and structure defects could enhance their catalytic performances for PMS activation. In this study, nitrogen-doped graphene (NG) is firstly synthesized by the calcination of graphene oxide (GO) with ammonium nitrate (NH4NO3). The obtained NG is then annealed further at a higher temperature under N2 atmosphere to remove partial doped N atoms and create new structure defects. The obtained defective nitrogen-doped graphene (D-NG) can activate PMS for bisphenol A (BPA) degradation more effectively. Different annealing temperatures from 850 to 1150 oC are investigated, and D-NG synthesized at 1050 oC exhibits the highest activity. The enhanced catalytic performance is proposed to be origin from the synergistic effect between doped N atoms and created structure defects. According to the radical quenching, electron paramagnetic resonance (EPR), and electrochemical results, both radical and non-radical pathways are present during the PMS activation, and the non-radical pathway acts as the dominated role. This study provides a facile method for metal-free catalyst synthesis, which also enriches the synergistic mechanism between doped N and structure defects, thus should have great potential in wastewater remediation.

Thermal removal of partial nitrogen atoms in N-doped graphene for enhanced catalytic oxidation

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