Boosting singlet oxygen generation for salinity wastewater treatment through co-activation of oxygen and peroxymonosulfate in photoelectrochemical process
High concentrations of inorganic ions in saline wastewater pose adverse effects on hydroxyl radical (HO•)-dominated technologies. Here, we report a unique strategy for boosting singlet oxygen (1O2) generation via coactivation of oxygen and peroxymonosulfate (PMS) by regulating the electron transfer...
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KeAi Communications Co. Ltd.
2025-01-01
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| Series: | Fundamental Research |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2667325822004514 |
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| author | Qianqian Yang Zhiyuan Feng Yanbo Zhou Hongying Zhao Guohua Zhao |
| author_facet | Qianqian Yang Zhiyuan Feng Yanbo Zhou Hongying Zhao Guohua Zhao |
| author_sort | Qianqian Yang |
| collection | DOAJ |
| description | High concentrations of inorganic ions in saline wastewater pose adverse effects on hydroxyl radical (HO•)-dominated technologies. Here, we report a unique strategy for boosting singlet oxygen (1O2) generation via coactivation of oxygen and peroxymonosulfate (PMS) by regulating the electron transfer regime in the photoelectrochemical process. The Fe-N bridge in atomic Fe-modified graphitic carbon nitride (denoted SA-FeCN) favors the construction of electron-defective Fe and electron-rich N vacancies (Nvs) to accelerate directional electron transfer. The produced intermediate (HSO4O···Fe−Nvs···OO) as a chemical channel accelerates the directional electron transfer from PMS to further reduce O2 to form activated products (SO5•−, O2•−), thereby transforming O2 into 1O2. An optimized 1O2 generation rate of 39.4 μmol L−1s−1 is obtained, which is 15.7–945.0 times higher than that in traditional advanced oxidation processes. Fast kinetics are achieved for removing various phenolic pollutants in a nonradical oxidation pathway, which is less susceptible to the coexistence of natural organic matter and inorganic ions. The COD removal for coal wastewater and complex industrial wastewater in real scenarios is found to reach a value of 90%-96% in 3 h. This work provides a new direction for boosting the 1O2 generation rate, especially for the selective degradation of target electron-rich contaminants in saline wastewater. |
| format | Article |
| id | doaj-art-1438c8ab54b34c6fa703a4c58d99ee20 |
| institution | Kabale University |
| issn | 2667-3258 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | KeAi Communications Co. Ltd. |
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| series | Fundamental Research |
| spelling | doaj-art-1438c8ab54b34c6fa703a4c58d99ee202025-01-29T05:02:29ZengKeAi Communications Co. Ltd.Fundamental Research2667-32582025-01-0151165173Boosting singlet oxygen generation for salinity wastewater treatment through co-activation of oxygen and peroxymonosulfate in photoelectrochemical processQianqian Yang0Zhiyuan Feng1Yanbo Zhou2Hongying Zhao3Guohua Zhao4Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering, Tongji University, Shanghai 200092, ChinaShanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering, Tongji University, Shanghai 200092, ChinaKey Laboratory of Coal Gasification and Energy Chemical Engineering of Ministry of Education, East China University of Science and Technology, Shanghai 200092, ChinaShanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering, Tongji University, Shanghai 200092, China; Corresponding author.Shanghai Key Lab of Chemical Assessment and Sustainability, Key Laboratory of Yangtze River Water Environment, School of Chemical Science and Engineering, Tongji University, Shanghai 200092, ChinaHigh concentrations of inorganic ions in saline wastewater pose adverse effects on hydroxyl radical (HO•)-dominated technologies. Here, we report a unique strategy for boosting singlet oxygen (1O2) generation via coactivation of oxygen and peroxymonosulfate (PMS) by regulating the electron transfer regime in the photoelectrochemical process. The Fe-N bridge in atomic Fe-modified graphitic carbon nitride (denoted SA-FeCN) favors the construction of electron-defective Fe and electron-rich N vacancies (Nvs) to accelerate directional electron transfer. The produced intermediate (HSO4O···Fe−Nvs···OO) as a chemical channel accelerates the directional electron transfer from PMS to further reduce O2 to form activated products (SO5•−, O2•−), thereby transforming O2 into 1O2. An optimized 1O2 generation rate of 39.4 μmol L−1s−1 is obtained, which is 15.7–945.0 times higher than that in traditional advanced oxidation processes. Fast kinetics are achieved for removing various phenolic pollutants in a nonradical oxidation pathway, which is less susceptible to the coexistence of natural organic matter and inorganic ions. The COD removal for coal wastewater and complex industrial wastewater in real scenarios is found to reach a value of 90%-96% in 3 h. This work provides a new direction for boosting the 1O2 generation rate, especially for the selective degradation of target electron-rich contaminants in saline wastewater.http://www.sciencedirect.com/science/article/pii/S2667325822004514Photoelectrochemical processSinglet oxygenOxygen activationPeroxymonosulfate activationElectron transferSaline wastewater |
| spellingShingle | Qianqian Yang Zhiyuan Feng Yanbo Zhou Hongying Zhao Guohua Zhao Boosting singlet oxygen generation for salinity wastewater treatment through co-activation of oxygen and peroxymonosulfate in photoelectrochemical process Fundamental Research Photoelectrochemical process Singlet oxygen Oxygen activation Peroxymonosulfate activation Electron transfer Saline wastewater |
| title | Boosting singlet oxygen generation for salinity wastewater treatment through co-activation of oxygen and peroxymonosulfate in photoelectrochemical process |
| title_full | Boosting singlet oxygen generation for salinity wastewater treatment through co-activation of oxygen and peroxymonosulfate in photoelectrochemical process |
| title_fullStr | Boosting singlet oxygen generation for salinity wastewater treatment through co-activation of oxygen and peroxymonosulfate in photoelectrochemical process |
| title_full_unstemmed | Boosting singlet oxygen generation for salinity wastewater treatment through co-activation of oxygen and peroxymonosulfate in photoelectrochemical process |
| title_short | Boosting singlet oxygen generation for salinity wastewater treatment through co-activation of oxygen and peroxymonosulfate in photoelectrochemical process |
| title_sort | boosting singlet oxygen generation for salinity wastewater treatment through co activation of oxygen and peroxymonosulfate in photoelectrochemical process |
| topic | Photoelectrochemical process Singlet oxygen Oxygen activation Peroxymonosulfate activation Electron transfer Saline wastewater |
| url | http://www.sciencedirect.com/science/article/pii/S2667325822004514 |
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