Efficient degradation of sulfadiazine via facilitated electron transfer by iron-carbon catalyst with highly exposed...

The inaccessible active sites, excessive metal leaching and radical mediated degradation pathway greatly hinder the performances of Fe-C composite catalyst oxidation process in the advanced oxidation water treatment. Herein, a facile method was developed to in situ growth of MIL-53 (Fe) on the powder active carbon (PAC) surface by a mild condition, which finally yields PAC supported Fe₃O₄@C particles (PAC@MOFs-2T) after heat treatment. The detailed characterizations indicate that the fine Fe₃O₄ particles encapsulated with carbon layers were evenly anchored on the PAC as active sites, which made the catalytic centers highly accessible for the peroxydisulfate activation and sulfadiazine degradation. In addition, the carbon layers, coated on the active sites could prevent the metal leaching during the catalytic process resulting in the high stability in a wide pH range. More attractively, the density functional theory (DFT) simulations and emperimental evidences further proved that the oxidation was dominated by a electron transfer process (ETP), during which, the peroxydisulfate (PDS) was adsorbed on Fe₃O₄ to form PDS∗ with high oxidation potential to initiate the ETP. Meanwhile, it was also demonstrated that the optimized sample PAC@MOFs-2T enriched with electron donating groups could selectively degrade the sulfadiazine, which avoid the negative impacts from the co-existed foreign ions and organic matters during the oxidation process. In addition, the toxicity analysis of intermediate products revealed that the sulfadiazine can be degradated into low-toxic or non-toxic products, which further permits viability of this ETP mediated advanced oxidation processes.