Enhanced H2O2 formation and norfloxacin removal by electro-Fenton process using a surface-reconstructed graphite felt cathode: New insight into synergistic mechanism of defective active sites

Abstract

The efficient catalytic activity and strong durability possibility of carbon-based three-dimensional fiber materials remains an important challenge in Electro-Fenton advanced oxidation technology. Graphite felt (GF) is a promising electrode material for 2-electron oxygen reduction reaction but with higher catalytic inertia. Anodizing modification of GF has been proved to enhance it electro-catalytic property, but the disadvantages of excessive or insufficient oxidation of GF need further improved. Herein, the surface reconstituted graphite felt by anodizing and HNO3 ultrasonic integrated treatment was used as cathode to degrade norfloxacin (NOR) and the substantial role of different modification processes was essentially investigated. Compared with the single modification process, the synergistic interaction between these two methods can generate more defective active sites (DASs) on GF surface and greatly improved 2-electron ORR activity. The H2O2 can be further co-activated by Fe2+ and DASs into •OH(ads and free) and •O2− to efficiently degrade NOR. The treated GF with 20 min anodizing and 1 h HNO3 ultrasound had the highest electrocatalytic activity in a wide electric potential (−0.4 V to −0.8 V) and pH range (3–9) in system and the efficient removal rate of NOR was basically maintained after 5 cycles. Under optimal reaction conditions, 50 mg L−1 NOR achieved 93% degradation and almost 63% of NOR was completely mineralized within 120 min. The possible NOR degradation pathways and ecotoxicity of intermediates were analyzed by LC-MS and T.E.S.T. theoretical calculation. This paper provided the underlying insights into designing a high-efficiency carbon-based cathode materials for commercial antibiotic wastewater treatment.