Sulfate Radical-Mediated Degradation of Sulfadiazine by CuFeO2 Rhombohedral Crystal-Catalyzed Peroxymonosulfate: Synergistic Effects and Mechanisms

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Department of Civil Engineering, The University of Hong Kong, Pokfulam Road, Hong Kong, People’s Republic of China
State Key Laboratory of Pollution Control and Resources Reuse, School of Environmental Science & Engineering, Tongji University, Shanghai 200092, People’s Republic of China
*Phone: +852-2859-1973; fax: +852-2559-5337; e-mail: [email protected]
Cite this: Environ. Sci. Technol. 2016, 50, 6, 3119–3127
Publication Date (Web):February 23, 2016
https://doi.org/10.1021/acs.est.5b05974
Copyright © 2016 American Chemical Society
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Abstract

Copper–iron bimetallic oxides have shown great potential for powerful radical production by activating peroxides. In this work, CuFeO2 rhombohedral crystals (RCs) were synthesized and used as heterogeneous catalysts for peroxymonosulfate (PMS) activation under various conditions. Sulfadiazine, a widely used veterinary sulfonamide, was used as a target pollutant to evaluate the efficiency of this combination. The results showed that of all the catalysts tested, the CuFeO2 RCs had the greatest reactivity. Under conditions of 0.1 g L–1 CuFeO2 RCs and 33.0 μM PMS, the nearly complete degradation of sulfadiazine occurred within 24 min. A synergistic catalytic effect was found between solid Cu(I) and Fe(III), probably due to the accelerated reduction of Fe(III). The two activation stages that produced different radicals (hydroxyl radicals followed by sulfate radicals) existed when solid Cu(I) was used as the catalyst. The CuFeO2 RCs had a higher PMS utilization efficiency than CuFe2O4, probably because the Cu(I)-promoted reduction of solid Fe(III). A total of 10 products were identified, and their evolution was explored. On the basis of the evidence of oxidative product formation, we proposed four possible pathways of sulfadiazine degradation.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.est.5b05974.

  • Text S1–S5: details regarding the procedures for CuFe2O4 preparation, SDZ analysis, degradation product identification, crystallinity and morphology, and ATR-FTIR characterization; Tables S1–S4: properties of the catalysts, rate constants for alcohol oxidation by radicals, effects of TBA, and products of SDZ degradation identified with UPLC-MS/MS; Figures S1–S13: characterization of the catalysts, SDZ adsorption, effect of phosphate buffer and TBA on SDZ degradation, XPS spectra of Cu 2p, UPLC–MS/MS multiple reaction monitoring chromatograms and product ion of some degradation products, concentration profile of SDZ and its degradation products, the reusability of the CuFeO2 RCs, and XRD patterns of the used CuFeO2 RCs. (PDF)

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