Developing the eco-friendly catalyst-adsorption iron-based materials with improved catalytic activity and minimal Fe leaching is fascinating for roxarsone (ROX) removal. Herein, Fe3O4 nanoparticles were encapsulated in flexible N, S-modified carbon chamber (Fe3O4@NS4C) through the “hydrothermal + pyrolysis” process to form a catalyst with multi-active sites. ROX could be degraded nearly 100 % at pH 5.0 −11.0 and secondary inorganic As species concentration is lower than 0.09 mg/L by efficient adsorption. Especially, the Fe ion leaching concentration in Fe3O4@NS4C/PMS after ROX removal is decreased to 0.08 mg/L. Combined with quenching experiment, EPR, Raman spectroscopy and electrochemical analysis, the non-radical activation mechanism dominated by 1O2 and electron transfer was determined. The synergistic interaction between the N doped sites and the S anchored sites within the carbon matrix not only improves the adsorption of PMS on the catalyst but also facilitates the direct activation of PMS to 1O2, while the surface electron transfer improves the Fe2+/Fe3+ redox cycling in PMS activation. The active sites of ROX attacked by 1O2 were examined through Fukui function computations. Combined with HPLC-MS, the ROX degradation pathway was determined, and the toxicity of intermediates was evaluated. Furthermore, the removal performance of ROX in Fe3O4@NS4C/PMS system was also assessed in different environment for practical application, indicating that the advantages in the synergy between N, S co-doping carbon chamber and encapsulated iron oxide for water purification.
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