Degradation of atrazine by electro-peroxone enhanced by Fe and N co-doped carbon nanotubes with simultaneous catalysis of H2O2 and O3

Abstract

Fe and N co-doped carbon nanotubes (Fe-N-CNT) was synthesized and attempted as efficient heterogeneous catalysts for simultaneous catalysis of H2O2 and O3 to improve electro-peroxone (Fe-N-CNT/EP) process efficiency for atrazine (ATZ) degradation. The removal and mineralization of ATZ was significantly enhanced, obtaining the degradation rate constant (k) by Fe-N-CNT/EP (0.23 min−1) about two times that of EP (0.12 min−1) owing to the formation of Fe0 and Fe-N coordination in Fe-N-CNT catalyst for co-catalysis of H2O2 and O3. The important factors such as applied current and ozone concentration were investigated, demonstrating that the optimized performance could be achieved at current of 30 mA and ozone concentration of 55 mg L−1. The oxidation capacity of Fe-N-CNT/EP maintained stably under wide pH range of 3∼7, obtaining the degradation rate constant 1.23–1.92 times that of EP and overcoming the defect of EP at acidic and neutral conditions. Capture experiments and electron paramagnetic resonance (EPR) experiments verified that .OH, generated by accelerating decomposition of H2O2/O3 and peroxone reaction, was the dominant active specie in Fe-N-CNT/EP. Besides, Fe-N-CNT showed high catalytic activity and good stability during six cycles. This work provides an efficient activator for enhanced EP process, exhibiting a promising prospect for water and wastewater purification.