New Insights into the Combination of Permanganate and Bisulfite as a Novel Advanced Oxidation Process: Importance of High Valent Manganese-Oxo Species and Sulfate Radical
Recently, it has been reported that the combination of permanganate (Mn(VII)) and bisulfite can lead to a rapid degradation of organic contaminants, where soluble Mn(III) is proposed to be responsible. Interestingly, in this work, we demonstrated the involvement of high-valent Mn-oxo species (poss...
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| Published in | Environmental science & technology Vol. 53; no. 7; pp. 3689 - 3696 |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
02.04.2019
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Recently, it has been reported that the combination of permanganate (Mn(VII)) and bisulfite can lead to a rapid degradation of organic contaminants, where soluble Mn(III) is proposed to be responsible. Interestingly, in this work, we demonstrated the involvement of high-valent Mn-oxo species (possibly Mn(V)) as well as sulfate radical in the Mn(VII)/bisulfite system, by using methyl phenyl sulfoxide (PMSO) as a chemical probe. It was found that the combination of Mn(VII) and bisulfite resulted in appreciable degradation of PMSO under various conditions, while negligible PMSO was degraded by manganese dioxide (MnO2) in the presence of bisulfite under similar conditions. This result indicated that Mn(III) intermediate formed in situ in both Mn(VII)/bisulfite and MnO2/bisulfite systems as proposed in literature exhibited sluggish reactivity toward PMSO. In parallel, the formation of methyl phenyl sulfone (PMSO2) product in the Mn(VII)/bisulfite system was observed, suggesting the role of high-valent Mn-oxo species as an oxygen-atom donor in conversion of PMSO to PMSO2. Moreover, the yield of PMSO2 (i.e., mole of PMSO2 produced per mole of PMSO degraded) was quantified to be 20–100%, strongly depending on the [Mn(VII)]/[bisulfite] ratio as well as solution pH. The competitive contribution of sulfate radical, which oxidized PMSO to hydroxylated and/or polymeric products but not to PMSO2, accounted for the yield of PMSO2 less than 100%. This work advances the fundamental understanding of a novel class of oxidation technology based on the combination of Mn(VII) and bisulfite for environmental decontamination. |
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| AbstractList | Recently, it has been reported that the combination of permanganate (Mn(VII)) and bisulfite can lead to a rapid degradation of organic contaminants, where soluble Mn(III) is proposed to be responsible. Interestingly, in this work, we demonstrated the involvement of high-valent Mn-oxo species (possibly Mn(V)) as well as sulfate radical in the Mn(VII)/bisulfite system, by using methyl phenyl sulfoxide (PMSO) as a chemical probe. It was found that the combination of Mn(VII) and bisulfite resulted in appreciable degradation of PMSO under various conditions, while negligible PMSO was degraded by manganese dioxide (MnO
) in the presence of bisulfite under similar conditions. This result indicated that Mn(III) intermediate formed in situ in both Mn(VII)/bisulfite and MnO
/bisulfite systems as proposed in literature exhibited sluggish reactivity toward PMSO. In parallel, the formation of methyl phenyl sulfone (PMSO
) product in the Mn(VII)/bisulfite system was observed, suggesting the role of high-valent Mn-oxo species as an oxygen-atom donor in conversion of PMSO to PMSO
. Moreover, the yield of PMSO
(i.e., mole of PMSO
produced per mole of PMSO degraded) was quantified to be 20-100%, strongly depending on the [Mn(VII)]/[bisulfite] ratio as well as solution pH. The competitive contribution of sulfate radical, which oxidized PMSO to hydroxylated and/or polymeric products but not to PMSO
, accounted for the yield of PMSO
less than 100%. This work advances the fundamental understanding of a novel class of oxidation technology based on the combination of Mn(VII) and bisulfite for environmental decontamination. Recently, it has been reported that the combination of permanganate (Mn(VII)) and bisulfite can lead to a rapid degradation of organic contaminants, where soluble Mn(III) is proposed to be responsible. Interestingly, in this work, we demonstrated the involvement of high-valent Mn-oxo species (possibly Mn(V)) as well as sulfate radical in the Mn(VII)/bisulfite system, by using methyl phenyl sulfoxide (PMSO) as a chemical probe. It was found that the combination of Mn(VII) and bisulfite resulted in appreciable degradation of PMSO under various conditions, while negligible PMSO was degraded by manganese dioxide (MnO2) in the presence of bisulfite under similar conditions. This result indicated that Mn(III) intermediate formed in situ in both Mn(VII)/bisulfite and MnO2/bisulfite systems as proposed in literature exhibited sluggish reactivity toward PMSO. In parallel, the formation of methyl phenyl sulfone (PMSO2) product in the Mn(VII)/bisulfite system was observed, suggesting the role of high-valent Mn-oxo species as an oxygen-atom donor in conversion of PMSO to PMSO2. Moreover, the yield of PMSO2 (i.e., mole of PMSO2 produced per mole of PMSO degraded) was quantified to be 20–100%, strongly depending on the [Mn(VII)]/[bisulfite] ratio as well as solution pH. The competitive contribution of sulfate radical, which oxidized PMSO to hydroxylated and/or polymeric products but not to PMSO2, accounted for the yield of PMSO2 less than 100%. This work advances the fundamental understanding of a novel class of oxidation technology based on the combination of Mn(VII) and bisulfite for environmental decontamination. Recently, it has been reported that the combination of permanganate (Mn(VII)) and bisulfite can lead to a rapid degradation of organic contaminants, where soluble Mn(III) is proposed to be responsible. Interestingly, in this work, we demonstrated the involvement of high-valent Mn-oxo species (possibly Mn(V)) as well as sulfate radical in the Mn(VII)/bisulfite system, by using methyl phenyl sulfoxide (PMSO) as a chemical probe. It was found that the combination of Mn(VII) and bisulfite resulted in appreciable degradation of PMSO under various conditions, while negligible PMSO was degraded by manganese dioxide (MnO2) in the presence of bisulfite under similar conditions. This result indicated that Mn(III) intermediate formed in situ in both Mn(VII)/bisulfite and MnO2/bisulfite systems as proposed in literature exhibited sluggish reactivity toward PMSO. In parallel, the formation of methyl phenyl sulfone (PMSO2) product in the Mn(VII)/bisulfite system was observed, suggesting the role of high-valent Mn-oxo species as an oxygen-atom donor in conversion of PMSO to PMSO2. Moreover, the yield of PMSO2 (i.e., mole of PMSO2 produced per mole of PMSO degraded) was quantified to be 20–100%, strongly depending on the [Mn(VII)]/[bisulfite] ratio as well as solution pH. The competitive contribution of sulfate radical, which oxidized PMSO to hydroxylated and/or polymeric products but not to PMSO2, accounted for the yield of PMSO2 less than 100%. This work advances the fundamental understanding of a novel class of oxidation technology based on the combination of Mn(VII) and bisulfite for environmental decontamination. |
| Author | Gao, Yuan Zhou, Yang Wang, Zhen Yang, Zhifeng Jiang, Jin Wang, Li-Hong Wang, Pan-Xin Shen, Yongming Pang, Su-Yan |
| AuthorAffiliation | State Key Laboratory of Urban Water Resource and Environment, School of Environment Jilin Jianzhu University Key Laboratory of Songliao Aquatic Environment, Ministry of Education, School of Municipal and Environmental Engineering Dalian University of Technology Institute of Environmental and Ecological Engineering State Key Laboratory of Coastal and Offshore Engineering |
| AuthorAffiliation_xml | – name: Key Laboratory of Songliao Aquatic Environment, Ministry of Education, School of Municipal and Environmental Engineering – name: State Key Laboratory of Urban Water Resource and Environment, School of Environment – name: Jilin Jianzhu University – name: Dalian University of Technology – name: State Key Laboratory of Coastal and Offshore Engineering – name: Institute of Environmental and Ecological Engineering |
| Author_xml | – sequence: 1 givenname: Yuan orcidid: 0000-0002-0890-8705 surname: Gao fullname: Gao, Yuan organization: Institute of Environmental and Ecological Engineering – sequence: 2 givenname: Yang surname: Zhou fullname: Zhou, Yang organization: Institute of Environmental and Ecological Engineering – sequence: 3 givenname: Su-Yan surname: Pang fullname: Pang, Su-Yan organization: Jilin Jianzhu University – sequence: 4 givenname: Jin orcidid: 0000-0003-2355-4244 surname: Jiang fullname: Jiang, Jin email: jiangjinhit@126.com, jiangjin@gdut.edu.cn organization: Institute of Environmental and Ecological Engineering – sequence: 5 givenname: Zhifeng surname: Yang fullname: Yang, Zhifeng organization: Institute of Environmental and Ecological Engineering – sequence: 6 givenname: Yongming surname: Shen fullname: Shen, Yongming organization: Dalian University of Technology – sequence: 7 givenname: Zhen surname: Wang fullname: Wang, Zhen organization: State Key Laboratory of Urban Water Resource and Environment, School of Environment – sequence: 8 givenname: Pan-Xin surname: Wang fullname: Wang, Pan-Xin organization: State Key Laboratory of Urban Water Resource and Environment, School of Environment – sequence: 9 givenname: Li-Hong surname: Wang fullname: Wang, Li-Hong organization: State Key Laboratory of Urban Water Resource and Environment, School of Environment |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/30888798$$D View this record in MEDLINE/PubMed |
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| Snippet | Recently, it has been reported that the combination of permanganate (Mn(VII)) and bisulfite can lead to a rapid degradation of organic contaminants, where... Recently, it has been reported that the combination of permanganate (Mn(VII)) and bisulfite can lead to a rapid degradation of organic contaminants, where... |
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| SubjectTerms | Biodegradation Bisulfite Contaminants Decontamination Degradation Manganese Manganese dioxide New combinations Organic chemistry Organic contaminants Oxidation Oxidation process Species Sulfates |
| Title | New Insights into the Combination of Permanganate and Bisulfite as a Novel Advanced Oxidation Process: Importance of High Valent Manganese-Oxo Species and Sulfate Radical |
| URI | http://dx.doi.org/10.1021/acs.est.8b05306 https://www.ncbi.nlm.nih.gov/pubmed/30888798 https://www.proquest.com/docview/2216875505 https://search.proquest.com/docview/2194590775 |
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