Activation of Peroxodisulfate Coupled with Photocatalysis by Pyrrolic N‐Rich Fe‐N4 Sites for High Efficiency Degradation of Tetracycline Hydrochloride

Photocatalysis is an efficient technology for the degradation of pollutants. However, there is still much room for improvement in its degradation efficiency. In this study, a pyrrolic N‐rich g‐C3N4 (PN‐g‐C3N4) framework was synthesized with transition metal M (M=Fe, Co, Ni, Cu, Cr, and Mn) atomic sites coordinated onto it. Then, a series of single atomic metals M anchored to PN‐g‐C3N4 (M/PN‐g‐C3N4) are constructed for peroxodisulfate activation. Their order of catalytic activity follows Fe>Cr>Ni>Cu≈Co>Mn, in particular the degradation rates of the TCH for Fe‐PN‐g‐C3N4 are 3.74 times higher than that of undoped PN‐g‐C3N4. These carefully regulated pyrrolic N‐rich Fe sites demonstrate outstanding performance in degrading organic pollutant. As an exemplary model, the Fe/PN‐g‐C3N4 catalyst efficiently drives the catalytic oxidation of TCH through Fenton‐like reaction under visible light, showcasing exceptional cycle stability and a broad effective pH range of 3.0–11.0. The synergy between photocatalysis and Fe doped catalysis results in increased generation and separation of charge carriers, along with the cyclic transformation of the Fe3+/Fe2+ couple. This combination significantly enhances the Fenton‐like performance, making it a highly effective process for pollutant degradation. Synopsis: A pyrrolic N‐rich g‐C3N4 (PN‐g‐C3N4) framework is synthesized with transition metal M (M=Fe, Co, Ni, Cu, Cr, and Mn) atomic sites coordinated onto it. M/PN‐g‐C3N4 are constructed for peroxodisulfate activation. The synergy between photocatalysis and Fe/PN‐g‐C3N4 catalyst results in increased generation and separation of charge carriers, along with the cyclic transformation of the Fe3+/Fe2+ couple.