High-density dispersion of CuNx sites for H2O2 activation toward enhanced Photo-Fenton performance in antibiotic contaminant degradation

Abstract

In this study, a copper-based catalyst (CuCN) with CuN_x active sites highly dispersed in a porous carbon nitride matrix was synthesized and applied to a heterogeneous photo-assisted Photo-Fenton (PF) system to degrade tetracycline (TET). The results showed that the CuCN/PF system degraded up to 93.6% of TET within 60 min for ultrapure water matrix under the best experimental conditions, and more than 70% of TET for both river and lake water matrix. Toxicological tests suggested that the environmental risk caused by TET can be effectively inhibited by the CuCN/PF system. The good visible-light response and charge transport abilities of CuCN catalyst were identified in photoelectrochemical experiments. Free radical scavenging experiments and electron paramagnetic resonance (EPR) spectroscopy indicated that the active species in the degradation process were·OH, h⁺,·O₂^- and ¹O₂. Density functional theory (DFT) calculations revealed the positive effect of CuN_x sites in CuCN on the formation of hydroxyl radicals by activating H₂O₂. This work will provide a new insight for the development of high-efficiency heterogeneous catalysts in wastewater environmental remediation.

Keywords: CuN(x) site; H(2)O(2) activation; Photo-Fenton; Tetracycline; Toxicological test.