Production of sulfate radical from peroxymonosulfate induced by a magnetically separable CuFe2O4 spinel in water: Efficiency, stability, and mechanism

Handle URI:
http://hdl.handle.net/10754/562685
Title:
Production of sulfate radical from peroxymonosulfate induced by a magnetically separable CuFe2O4 spinel in water: Efficiency, stability, and mechanism
Authors:
Zhang, Tao; Zhu, Haibo; Croue, Jean-Philippe
Abstract:
A simple, nonhazardous, efficient and low energy-consuming process is desirable to generate powerful radicals from peroxymonosulfate (PMS) for recalcitrant pollutant removal. In this work, the production of radical species from PMS induced by a magnetic CuFe2O4 spinel was studied. Iopromide, a recalcitrant model pollutant, was used to investigate the efficiency of this process. CuFe2O4 showed higher activity and 30 times lower Cu2+ leaching (1.5 μg L-1 per 100 mg L-1) than a well-crystallized CuO at the same dosage. CuFe 2O4 maintained its activity and crystallinity during repeated batch experiments. In comparison, the activity of CuO declined significantly, which was ascribed to the deterioration in its degree of crystallinity. The efficiency of the PMS/CuFe2O4 was highest at neutral pH and decreased at acidic and alkaline pHs. Sulfate radical was the primary radical species responsible for the iopromide degradation. On the basis of the stoichiometry of oxalate degradation in the PMS/CuFe 2O4, the radical production yield from PMS was determined to be near 1 mol/mol. The PMS decomposition involved an inner-sphere complexation with the oxide's surface Cu(II) sites. In situ characterization of the oxide surface with ATR-FTIR and Raman during the PMS decomposition suggested that surface Cu(II)-Cu(III)-Cu(II) redox cycle was responsible for the efficient sulfate radical generation from PMS. © 2013 American Chemical Society.
KAUST Department:
Water Desalination and Reuse Research Center (WDRC); KAUST Catalysis Center (KCC); Water Desalination and Reuse Research Center; Biological and Environmental Sciences and Engineering (BESE) Division
Publisher:
American Chemical Society
Journal:
Environmental Science and Technology
Issue Date:
19-Mar-2013
DOI:
10.1021/es304721g
PubMed ID:
23439015
Type:
Article
ISSN:
0013936X
Appears in Collections:
Articles; KAUST Catalysis Center (KCC); Water Desalination and Reuse Research Center (WDRC); Biological and Environmental Sciences and Engineering (BESE) Division

Full metadata record

DC FieldValue Language
dc.contributor.authorZhang, Taoen
dc.contributor.authorZhu, Haiboen
dc.contributor.authorCroue, Jean-Philippeen
dc.date.accessioned2015-08-03T11:01:24Zen
dc.date.available2015-08-03T11:01:24Zen
dc.date.issued2013-03-19en
dc.identifier.issn0013936Xen
dc.identifier.pmid23439015en
dc.identifier.doi10.1021/es304721gen
dc.identifier.urihttp://hdl.handle.net/10754/562685en
dc.description.abstractA simple, nonhazardous, efficient and low energy-consuming process is desirable to generate powerful radicals from peroxymonosulfate (PMS) for recalcitrant pollutant removal. In this work, the production of radical species from PMS induced by a magnetic CuFe2O4 spinel was studied. Iopromide, a recalcitrant model pollutant, was used to investigate the efficiency of this process. CuFe2O4 showed higher activity and 30 times lower Cu2+ leaching (1.5 μg L-1 per 100 mg L-1) than a well-crystallized CuO at the same dosage. CuFe 2O4 maintained its activity and crystallinity during repeated batch experiments. In comparison, the activity of CuO declined significantly, which was ascribed to the deterioration in its degree of crystallinity. The efficiency of the PMS/CuFe2O4 was highest at neutral pH and decreased at acidic and alkaline pHs. Sulfate radical was the primary radical species responsible for the iopromide degradation. On the basis of the stoichiometry of oxalate degradation in the PMS/CuFe 2O4, the radical production yield from PMS was determined to be near 1 mol/mol. The PMS decomposition involved an inner-sphere complexation with the oxide's surface Cu(II) sites. In situ characterization of the oxide surface with ATR-FTIR and Raman during the PMS decomposition suggested that surface Cu(II)-Cu(III)-Cu(II) redox cycle was responsible for the efficient sulfate radical generation from PMS. © 2013 American Chemical Society.en
dc.publisherAmerican Chemical Societyen
dc.titleProduction of sulfate radical from peroxymonosulfate induced by a magnetically separable CuFe2O4 spinel in water: Efficiency, stability, and mechanismen
dc.typeArticleen
dc.contributor.departmentWater Desalination and Reuse Research Center (WDRC)en
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentWater Desalination and Reuse Research Centeren
dc.contributor.departmentBiological and Environmental Sciences and Engineering (BESE) Divisionen
dc.identifier.journalEnvironmental Science and Technologyen
kaust.authorZhang, Taoen
kaust.authorZhu, Haiboen
kaust.authorCroue, Jean-Philippeen
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