Abstract

This work focused on the mechanism of photogenerated hole (h+) mediating the generation of active species in visible-light-assisted photocatalytic peroxymonosulfate (PMS) activation. Ferrous gluconate derived iron-doped carbon dots (Fe-CDs) were synthesized to investigate the vital role of h+ in the process of photocatalytic PMS activation for acetaminophen degradation by quenching experiments, ESR spectra, and DFT calculations. Within 20 minutes, Fe-CDs/PMS/Vis system can achieve a 100 % degradation of acetaminophen (15 μM) with low-addition of PMS (0.2 mM) and Fe-CDs (12 μg/L). The Fe3+ sites on Fe-CDs reduce the activation energy for the generation of SO5−• from PMS, increase the concentration and utilization of h+ in the system, and make the direct activation of PMS by h+ be the dominant pathway to mediate the generation of •OH and 1O2. This work provides mechanistic insights for further research on h+ mediated regulation of active species in photocatalytic PMS activation process for micropollutants removal.

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