Both Fe(IV) and Radicals Are Active Oxidants in the Fe(II)/Peroxydisulfate Process
The question of whether Fe(IV) or SO4 •– is the dominant intermediate in the Fe(II)-activated peroxydisulfate process [Fe(II)/PDS process] remains unanswered. In this study, besides Fe(IV), SO4 •– and HO• were shown to be produced in the Fe(II)/PDS process by using multiple probes [dimethyl sul...
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| Published in | Environmental science & technology letters Vol. 7; no. 3; pp. 219 - 224 |
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| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Chemical Society
10.03.2020
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| Subjects | |
| Online Access | Get full text |
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| Abstract | The question of whether Fe(IV) or SO4 •– is the dominant intermediate in the Fe(II)-activated peroxydisulfate process [Fe(II)/PDS process] remains unanswered. In this study, besides Fe(IV), SO4 •– and HO• were shown to be produced in the Fe(II)/PDS process by using multiple probes [dimethyl sulfoxide, methyl phenyl sulfoxide, p-nitrobenzoic acid (p-NBA), and benzoic acid (BA)]. The removal of p-NBA and BA and the influence of BA on the yield of methyl phenyl sulfone (PMSO2) indicated that the major oxidizing intermediate changed from Fe(IV) to SO4 •–/HO• with an increase in the PDS/Fe(II) molar ratio at pH 3.0. Fe(IV), SO4 •–, and HO• were all involved in this process at pH 3.0–6.5, but their available amounts that contributed to abating organic contaminants decreased with an increase in pH considering the influence of pH on the generation of PMSO2 and p-hydroxybenzoic acid. Furthermore, Fe(IV), SO4 •–, and HO• contributed differently to abating different organic contaminants because of the different reactivities of these oxidizing oxidants toward different organic contaminants. Overall, this study demonstrates that multiple oxidizing species [Fe(IV), SO4 •–, and HO•] are generated in the Fe(II)/PDS process, which was significant for the application of this process and understanding the mechanisms of Fe(II)-activated peroxide processes. |
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| AbstractList | The question of whether Fe(IV) or SO4 •– is the dominant intermediate in the Fe(II)-activated peroxydisulfate process [Fe(II)/PDS process] remains unanswered. In this study, besides Fe(IV), SO4 •– and HO• were shown to be produced in the Fe(II)/PDS process by using multiple probes [dimethyl sulfoxide, methyl phenyl sulfoxide, p-nitrobenzoic acid (p-NBA), and benzoic acid (BA)]. The removal of p-NBA and BA and the influence of BA on the yield of methyl phenyl sulfone (PMSO2) indicated that the major oxidizing intermediate changed from Fe(IV) to SO4 •–/HO• with an increase in the PDS/Fe(II) molar ratio at pH 3.0. Fe(IV), SO4 •–, and HO• were all involved in this process at pH 3.0–6.5, but their available amounts that contributed to abating organic contaminants decreased with an increase in pH considering the influence of pH on the generation of PMSO2 and p-hydroxybenzoic acid. Furthermore, Fe(IV), SO4 •–, and HO• contributed differently to abating different organic contaminants because of the different reactivities of these oxidizing oxidants toward different organic contaminants. Overall, this study demonstrates that multiple oxidizing species [Fe(IV), SO4 •–, and HO•] are generated in the Fe(II)/PDS process, which was significant for the application of this process and understanding the mechanisms of Fe(II)-activated peroxide processes. The question of whether Fe(IV) or SO₄•– is the dominant intermediate in the Fe(II)-activated peroxydisulfate process [Fe(II)/PDS process] remains unanswered. In this study, besides Fe(IV), SO₄•– and HO• were shown to be produced in the Fe(II)/PDS process by using multiple probes [dimethyl sulfoxide, methyl phenyl sulfoxide, p-nitrobenzoic acid (p-NBA), and benzoic acid (BA)]. The removal of p-NBA and BA and the influence of BA on the yield of methyl phenyl sulfone (PMSO₂) indicated that the major oxidizing intermediate changed from Fe(IV) to SO₄•–/HO• with an increase in the PDS/Fe(II) molar ratio at pH 3.0. Fe(IV), SO₄•–, and HO• were all involved in this process at pH 3.0–6.5, but their available amounts that contributed to abating organic contaminants decreased with an increase in pH considering the influence of pH on the generation of PMSO₂ and p-hydroxybenzoic acid. Furthermore, Fe(IV), SO₄•–, and HO• contributed differently to abating different organic contaminants because of the different reactivities of these oxidizing oxidants toward different organic contaminants. Overall, this study demonstrates that multiple oxidizing species [Fe(IV), SO₄•–, and HO•] are generated in the Fe(II)/PDS process, which was significant for the application of this process and understanding the mechanisms of Fe(II)-activated peroxide processes. |
| Author | Xie, Yifan Guan, Xiaohong Wang, Shuchang Zhou, Gongming Liu, Weifan Li, Yang Dong, Hongyu |
| AuthorAffiliation | Shanghai Institute of Pollution Control and Ecological Security State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering Tongji University International Joint Research Center for Sustainable Urban Water System |
| AuthorAffiliation_xml | – name: Shanghai Institute of Pollution Control and Ecological Security – name: International Joint Research Center for Sustainable Urban Water System – name: State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering – name: Tongji University |
| Author_xml | – sequence: 1 givenname: Hongyu surname: Dong fullname: Dong, Hongyu organization: Shanghai Institute of Pollution Control and Ecological Security – sequence: 2 givenname: Yang surname: Li fullname: Li, Yang organization: Shanghai Institute of Pollution Control and Ecological Security – sequence: 3 givenname: Shuchang surname: Wang fullname: Wang, Shuchang organization: Shanghai Institute of Pollution Control and Ecological Security – sequence: 4 givenname: Weifan surname: Liu fullname: Liu, Weifan organization: Shanghai Institute of Pollution Control and Ecological Security – sequence: 5 givenname: Gongming surname: Zhou fullname: Zhou, Gongming organization: Shanghai Institute of Pollution Control and Ecological Security – sequence: 6 givenname: Yifan surname: Xie fullname: Xie, Yifan organization: Shanghai Institute of Pollution Control and Ecological Security – sequence: 7 givenname: Xiaohong orcidid: 0000-0001-5296-423X surname: Guan fullname: Guan, Xiaohong email: guanxh@tongji.edu.cn organization: Tongji University |
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| Snippet | The question of whether Fe(IV) or SO4 •– is the dominant intermediate in the Fe(II)-activated peroxydisulfate process [Fe(II)/PDS process] remains... The question of whether Fe(IV) or SO₄•– is the dominant intermediate in the Fe(II)-activated peroxydisulfate process [Fe(II)/PDS process] remains unanswered.... |
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| SubjectTerms | 4-hydroxybenzoic acid benzoic acid dimethyl sulfoxide free radicals hydroxyl radicals iron nitrobenzoic acids oxidants |
| Title | Both Fe(IV) and Radicals Are Active Oxidants in the Fe(II)/Peroxydisulfate Process |
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