The poor anti-interference ability of radical-dominated processes continues to be a hindrance to the effectiveness of purification and practical use of Peroxymonosulfate-based advanced oxidation processes (PMS-AOPs). Here, iron, nitrogen, and sulfur co-doped porous carbon sheets (Fe‒SNC) were successfully synthesized via one-step pyrolysis process by adopting Mohr′s salt and ZIF-8 sheets as precursors to efficiently activate PMS. The quenching experiments and electron paramagnetic resonance (EPR) characterization displayed that singlet oxygen (1O2) played the most important role in phenol degradation. Based on the variation in material structure and the density functional theory (DFT) calculations, the study conducted the specific mechanism of sulfur embedded in rich Fe3C, Fe4N, and Fe‒Nx catalytic sites as an activator of PMS in the degradation of the pollutant of interest. In addition, the S-doping sites were shown to shorten the distance between the PMS and the catalyst due to electron polarization of the catalyst surface, which facilitated PMS adsorption. In addition, according to ultra-high-resolution electro-spray time-of-flight mass spectrometry and ECOSAR software 's predictions, the aquatic ecological environment would not be harmed by the degradation intermediates. As a consequence, this heterogeneous system possesses admirable anti-interference in pollutant elimination. These conclusions offered instructions for the creation of S-doping porous carbon sheets for effective water treatment.

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