Modulating electron density enable efficient cascade conversion from peroxymonosulfate to superoxide radical driven by electron-rich/poor dual sites.

J Hazard Mater

Key Laboratory of Groundwater Resources and Environment (Jilin University), Ministry of Education, Jilin University, Changchun 130021, Jilin, China; Jilin Provincial Key Laboratory of Water Resources and Environment, Jilin University, Changchun 130021, Jilin, China. Electronic address:

Published: April 2024

The superoxide radical (•O)-mediated peroxymonosulfate (PMS)-based photo-Fenton-like reaction enables highly selective water decontamination. Nevertheless, the targeted construction of •O-mediated photo-Fenton-like system has been challenging. Herein, we developed an electron-rich/-poor dual sites driven •O-mediated cascade photo-Fenton-like system by modulating electron density. Experimental and theoretical results demonstrated that PMS was preferentially adsorbed on electron-poor Co site. This adsorption promoted O-O bond cleavage of PMS to generate hydrogen peroxide (HO), which then migrated to electron-rich O site to extract e electrons for O-H bond cleavage, rather than competing with PMS for Co site. The developed versatile cascade reaction system could selectively eliminate contaminants with low n-octanol/water partition constants (K) and dissociation constants (pKa) and remarkably resist inorganics (Cl, HPO and NO), humic acid (HA) and even real water matrices (tap water and secondary effluent). This finding provided a novel and plausible strategy to accurately and efficiently generate •O for the selective water decontamination.

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http://dx.doi.org/10.1016/j.jhazmat.2024.133749DOI Listing

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