Efficient peroxydisulfate activation process not relying on sulfate radical generation for water pollutant degradation

Handle URI:
http://hdl.handle.net/10754/563554
Title:
Efficient peroxydisulfate activation process not relying on sulfate radical generation for water pollutant degradation
Authors:
Zhang, Tao; Chen, Yin; Wang, Yuru; Le Roux, Julien ( 0000-0003-0245-8536 ) ; Yang, Yang; Croue, Jean-Philippe
Abstract:
Peroxydisulfate (PDS) is an appealing oxidant for contaminated groundwater and toxic industrial wastewaters. Activation of PDS is necessary for application because of its low reactivity. Present activation processes always generate sulfate radicals as actual oxidants which unselectively oxidize organics and halide anions reducing oxidation capacity of PDS and producing toxic halogenated products. Here we report that copper oxide (CuO) can efficiently activate PDS under mild conditions without producing sulfate radicals. The PDS/CuO coupled process is most efficient at neutral pH for decomposing a model compound, 2,4-dichlorophenol (2,4-DCP). In a continuous-flow reaction with an empty-bed contact time of 0.55 min, over 90% of 2,4-DCP (initially 20 μM) and 90% of adsorbable organic chlorine (AOCl) can be removed at the PDS/2,4-DCP molar ratio of 1 and 4, respectively. Based on kinetic study and surface characterization, PDS is proposed to be first activated by CuO through outer-sphere interaction, the rate-limiting step, followed by a rapid reaction with 2,4-DCP present in the solution. In the presence of ubiquitous chloride ions in groundwater/industrial wastewater, the PDS/CuO oxidation shows significant advantages over sulfate radical oxidation by achieving much higher 2,4-DCP degradation capacity and avoiding the formation of highly chlorinated degradation products. This work provides a new way of PDS activation for contaminant removal. © 2014 American Chemical Society.
KAUST Department:
Water Desalination and Reuse Research Center (WDRC); Solar and Photovoltaic Engineering Research Center (SPERC); Advanced Nanofabrication, Imaging and Characterization Core Lab; Water Desalination and Reuse Research Center; Water Desalination & Reuse Research Cntr; Core Labs; Biological and Environmental Sciences and Engineering (BESE) Division
Publisher:
American Chemical Society (ACS)
Journal:
Environmental Science & Technology
Issue Date:
20-May-2014
DOI:
10.1021/es501218f
PubMed ID:
24779765
Type:
Article
ISSN:
0013936X
Appears in Collections:
Articles; Advanced Nanofabrication, Imaging and Characterization Core Lab; Solar and Photovoltaic Engineering Research Center (SPERC); 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.authorChen, Yinen
dc.contributor.authorWang, Yuruen
dc.contributor.authorLe Roux, Julienen
dc.contributor.authorYang, Yangen
dc.contributor.authorCroue, Jean-Philippeen
dc.date.accessioned2015-08-03T11:54:21Zen
dc.date.available2015-08-03T11:54:21Zen
dc.date.issued2014-05-20en
dc.identifier.issn0013936Xen
dc.identifier.pmid24779765en
dc.identifier.doi10.1021/es501218fen
dc.identifier.urihttp://hdl.handle.net/10754/563554en
dc.description.abstractPeroxydisulfate (PDS) is an appealing oxidant for contaminated groundwater and toxic industrial wastewaters. Activation of PDS is necessary for application because of its low reactivity. Present activation processes always generate sulfate radicals as actual oxidants which unselectively oxidize organics and halide anions reducing oxidation capacity of PDS and producing toxic halogenated products. Here we report that copper oxide (CuO) can efficiently activate PDS under mild conditions without producing sulfate radicals. The PDS/CuO coupled process is most efficient at neutral pH for decomposing a model compound, 2,4-dichlorophenol (2,4-DCP). In a continuous-flow reaction with an empty-bed contact time of 0.55 min, over 90% of 2,4-DCP (initially 20 μM) and 90% of adsorbable organic chlorine (AOCl) can be removed at the PDS/2,4-DCP molar ratio of 1 and 4, respectively. Based on kinetic study and surface characterization, PDS is proposed to be first activated by CuO through outer-sphere interaction, the rate-limiting step, followed by a rapid reaction with 2,4-DCP present in the solution. In the presence of ubiquitous chloride ions in groundwater/industrial wastewater, the PDS/CuO oxidation shows significant advantages over sulfate radical oxidation by achieving much higher 2,4-DCP degradation capacity and avoiding the formation of highly chlorinated degradation products. This work provides a new way of PDS activation for contaminant removal. © 2014 American Chemical Society.en
dc.publisherAmerican Chemical Society (ACS)en
dc.titleEfficient peroxydisulfate activation process not relying on sulfate radical generation for water pollutant degradationen
dc.typeArticleen
dc.contributor.departmentWater Desalination and Reuse Research Center (WDRC)en
dc.contributor.departmentSolar and Photovoltaic Engineering Research Center (SPERC)en
dc.contributor.departmentAdvanced Nanofabrication, Imaging and Characterization Core Laben
dc.contributor.departmentWater Desalination and Reuse Research Centeren
dc.contributor.departmentWater Desalination & Reuse Research Cntren
dc.contributor.departmentCore Labsen
dc.contributor.departmentBiological and Environmental Sciences and Engineering (BESE) Divisionen
dc.identifier.journalEnvironmental Science & Technologyen
kaust.authorZhang, Taoen
kaust.authorChen, Yinen
kaust.authorWang, Yuruen
kaust.authorLe Roux, Julienen
kaust.authorYang, Yangen
kaust.authorCroue, Jean-Philippeen
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