A non-acid-assisted and non-hydroxyl-radical-related catalytic ozonation with ceria supported copper oxide in efficient oxalate degradation in water

Handle URI:
http://hdl.handle.net/10754/562209
Title:
A non-acid-assisted and non-hydroxyl-radical-related catalytic ozonation with ceria supported copper oxide in efficient oxalate degradation in water
Authors:
Zhang, Tao; Li, Weiwei; Croue, Jean-Philippe
Abstract:
Oxalate is usually used as a refractory model compound that cannot be effectively removed by ozone and hydroxyl radical oxidation in water. In this study, we found that ceria supported CuO significantly improved oxalate degradation in reaction with ozone. The optimum CuO loading amount was 12%. The molar ratio of oxalate removed/ozone consumption reached 0.84. The catalytic ozonation was most effective in a neutral pH range (6.7-7.9) and became ineffective when the water solution was acidic or alkaline. Moreover, bicarbonate, a ubiquitous hydroxyl radical scavenger in natural waters, significantly improved the catalytic degradation of oxalate. Therefore, the degradation relies on neither hydroxyl radical oxidation nor acid assistance, two pathways usually proposed for catalytic ozonation. These special characters of the catalyst make it suitable to be potentially used for practical degradation of refractory hydrophilic organic matter and compounds in water and wastewater. With in situ characterization, the new surface Cu(II) formed from ozone oxidation of the trace Cu(I) of the catalyst was found to be an active site in coordination with oxalate forming multi-dentate surface complex. It is proposed that the complex can be further oxidized by molecular ozone and then decomposes through intra-molecular electron transfer. The ceria support enhanced the activity of the surface Cu(I)/Cu(II) in this process. © 2012 Elsevier B.V.
KAUST Department:
Water Desalination and Reuse Research Center (WDRC); Water Desalination and Reuse Research Center; Biological and Environmental Sciences and Engineering (BESE) Division
Publisher:
Elsevier
Journal:
Applied Catalysis B: Environmental
Issue Date:
Jun-2012
DOI:
10.1016/j.apcatb.2012.03.021
Type:
Article
ISSN:
09263373
Appears in Collections:
Articles; 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.authorLi, Weiweien
dc.contributor.authorCroue, Jean-Philippeen
dc.date.accessioned2015-08-03T09:47:19Zen
dc.date.available2015-08-03T09:47:19Zen
dc.date.issued2012-06en
dc.identifier.issn09263373en
dc.identifier.doi10.1016/j.apcatb.2012.03.021en
dc.identifier.urihttp://hdl.handle.net/10754/562209en
dc.description.abstractOxalate is usually used as a refractory model compound that cannot be effectively removed by ozone and hydroxyl radical oxidation in water. In this study, we found that ceria supported CuO significantly improved oxalate degradation in reaction with ozone. The optimum CuO loading amount was 12%. The molar ratio of oxalate removed/ozone consumption reached 0.84. The catalytic ozonation was most effective in a neutral pH range (6.7-7.9) and became ineffective when the water solution was acidic or alkaline. Moreover, bicarbonate, a ubiquitous hydroxyl radical scavenger in natural waters, significantly improved the catalytic degradation of oxalate. Therefore, the degradation relies on neither hydroxyl radical oxidation nor acid assistance, two pathways usually proposed for catalytic ozonation. These special characters of the catalyst make it suitable to be potentially used for practical degradation of refractory hydrophilic organic matter and compounds in water and wastewater. With in situ characterization, the new surface Cu(II) formed from ozone oxidation of the trace Cu(I) of the catalyst was found to be an active site in coordination with oxalate forming multi-dentate surface complex. It is proposed that the complex can be further oxidized by molecular ozone and then decomposes through intra-molecular electron transfer. The ceria support enhanced the activity of the surface Cu(I)/Cu(II) in this process. © 2012 Elsevier B.V.en
dc.publisherElsevieren
dc.subjectAcid assistanceen
dc.subjectBicarbonateen
dc.subjectCatalytic ozonationen
dc.subjectHydroxyl radical oxidationen
dc.subjectOxalateen
dc.titleA non-acid-assisted and non-hydroxyl-radical-related catalytic ozonation with ceria supported copper oxide in efficient oxalate degradation in wateren
dc.typeArticleen
dc.contributor.departmentWater Desalination and Reuse Research Center (WDRC)en
dc.contributor.departmentWater Desalination and Reuse Research Centeren
dc.contributor.departmentBiological and Environmental Sciences and Engineering (BESE) Divisionen
dc.identifier.journalApplied Catalysis B: Environmentalen
dc.contributor.institutionResearch Center for Eco-Environmental Sciences (RCEES), Chinese Academy of Sciences (CAS), Beijing 100085, Chinaen
kaust.authorZhang, Taoen
kaust.authorCroue, Jean-Philippeen
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