Catalytic degradation of ciprofloxacin by a visible-light-assisted peroxymonosulfate activation system: Performance and mechanism
Peroxymonosulfate (PMS) is extensively used as an oxidant to develop the sulfate radical-based advanced oxidation processes in the decontamination of organic pollutants and various PMS activation methods have been explored. Visible-light-assisted PMS activation to construct a Fenton-like process has...
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| Published in | Water research (Oxford) Vol. 173; p. 115559 |
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| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
England
Elsevier Ltd
15.04.2020
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| Subjects | |
| Online Access | Get full text |
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| Abstract | Peroxymonosulfate (PMS) is extensively used as an oxidant to develop the sulfate radical-based advanced oxidation processes in the decontamination of organic pollutants and various PMS activation methods have been explored. Visible-light-assisted PMS activation to construct a Fenton-like process has shown a great potential for pollution control. In our work, BiVO4 nanosheets were prepared using a hydrothermal process and used to activate PMS under visible light. A rapid degradation of ciprofloxacin (CIP) was achieved by dosing PMS (0.96 g/L), BiVO4 (0.32 g/L) under visible light with a reaction rate constant of 77.72-fold higher than that in the BiVO4/visible light process. The electron spin resonance and free radical quenching experiments indicate that reactive species of •O2−, h+, •OH and SO4•− all worked, where h+, •OH and SO4•− were found as the dominant contributors to the CIP degradation. The spectroscopic analyses further demonstrate that the photoinduced electrons were directly involved in the PMS activation process. The generated •O2− was partially utilized to activate PMS and more •OH was produced because of the chain reactions between SO4•− and H2O/OH−. In this process, PMS acted as an electron acceptor to transfer the photo-induced charges from the conduction band of BiVO4 and PMS was successfully activated to yield the high-powered oxidative species. From the degradation intermediates of CIP detected by a liquid-chromatography-mass spectrometer, the possible degradation pathways were proposed. The substantially decreased toxicity of CIP after the reaction was also observed. This work might provide new insights into the visible-light-assisted PMS activation mechanisms and is useful to construct environmentally-friendly catalytic processes for the efficient degradation of organic pollutants.
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•PMS was effectively activated by BiVO4 nanosheets for water purification under visible light.•Separation of electron/hole pairs and generation of oxidative species were enhanced.•Visible-light-assisted PMS activation Fenton-like mechanism was elucidated.•High mineralization and low biotoxicity validated the application potential of the system. |
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| AbstractList | Peroxymonosulfate (PMS) is extensively used as an oxidant to develop the sulfate radical-based advanced oxidation processes in the decontamination of organic pollutants and various PMS activation methods have been explored. Visible-light-assisted PMS activation to construct a Fenton-like process has shown a great potential for pollution control. In our work, BiVO4 nanosheets were prepared using a hydrothermal process and used to activate PMS under visible light. A rapid degradation of ciprofloxacin (CIP) was achieved by dosing PMS (0.96 g/L), BiVO4 (0.32 g/L) under visible light with a reaction rate constant of 77.72-fold higher than that in the BiVO4/visible light process. The electron spin resonance and free radical quenching experiments indicate that reactive species of •O2−, h+, •OH and SO4•− all worked, where h+, •OH and SO4•− were found as the dominant contributors to the CIP degradation. The spectroscopic analyses further demonstrate that the photoinduced electrons were directly involved in the PMS activation process. The generated •O2− was partially utilized to activate PMS and more •OH was produced because of the chain reactions between SO4•− and H2O/OH−. In this process, PMS acted as an electron acceptor to transfer the photo-induced charges from the conduction band of BiVO4 and PMS was successfully activated to yield the high-powered oxidative species. From the degradation intermediates of CIP detected by a liquid-chromatography-mass spectrometer, the possible degradation pathways were proposed. The substantially decreased toxicity of CIP after the reaction was also observed. This work might provide new insights into the visible-light-assisted PMS activation mechanisms and is useful to construct environmentally-friendly catalytic processes for the efficient degradation of organic pollutants.
[Display omitted]
•PMS was effectively activated by BiVO4 nanosheets for water purification under visible light.•Separation of electron/hole pairs and generation of oxidative species were enhanced.•Visible-light-assisted PMS activation Fenton-like mechanism was elucidated.•High mineralization and low biotoxicity validated the application potential of the system. Peroxymonosulfate (PMS) is extensively used as an oxidant to develop the sulfate radical-based advanced oxidation processes in the decontamination of organic pollutants and various PMS activation methods have been explored. Visible-light-assisted PMS activation to construct a Fenton-like process has shown a great potential for pollution control. In our work, BiVO4 nanosheets were prepared using a hydrothermal process and used to activate PMS under visible light. A rapid degradation of ciprofloxacin (CIP) was achieved by dosing PMS (0.96 g/L), BiVO4 (0.32 g/L) under visible light with a reaction rate constant of 77.72-fold higher than that in the BiVO4/visible light process. The electron spin resonance and free radical quenching experiments indicate that reactive species of •O2-, h+, •OH and SO4•- all worked, where h+, •OH and SO4•- were found as the dominant contributors to the CIP degradation. The spectroscopic analyses further demonstrate that the photoinduced electrons were directly involved in the PMS activation process. The generated •O2- was partially utilized to activate PMS and more •OH was produced because of the chain reactions between SO4•- and H2O/OH-. In this process, PMS acted as an electron acceptor to transfer the photo-induced charges from the conduction band of BiVO4 and PMS was successfully activated to yield the high-powered oxidative species. From the degradation intermediates of CIP detected by a liquid-chromatography-mass spectrometer, the possible degradation pathways were proposed. The substantially decreased toxicity of CIP after the reaction was also observed. This work might provide new insights into the visible-light-assisted PMS activation mechanisms and is useful to construct environmentally-friendly catalytic processes for the efficient degradation of organic pollutants.Peroxymonosulfate (PMS) is extensively used as an oxidant to develop the sulfate radical-based advanced oxidation processes in the decontamination of organic pollutants and various PMS activation methods have been explored. Visible-light-assisted PMS activation to construct a Fenton-like process has shown a great potential for pollution control. In our work, BiVO4 nanosheets were prepared using a hydrothermal process and used to activate PMS under visible light. A rapid degradation of ciprofloxacin (CIP) was achieved by dosing PMS (0.96 g/L), BiVO4 (0.32 g/L) under visible light with a reaction rate constant of 77.72-fold higher than that in the BiVO4/visible light process. The electron spin resonance and free radical quenching experiments indicate that reactive species of •O2-, h+, •OH and SO4•- all worked, where h+, •OH and SO4•- were found as the dominant contributors to the CIP degradation. The spectroscopic analyses further demonstrate that the photoinduced electrons were directly involved in the PMS activation process. The generated •O2- was partially utilized to activate PMS and more •OH was produced because of the chain reactions between SO4•- and H2O/OH-. In this process, PMS acted as an electron acceptor to transfer the photo-induced charges from the conduction band of BiVO4 and PMS was successfully activated to yield the high-powered oxidative species. From the degradation intermediates of CIP detected by a liquid-chromatography-mass spectrometer, the possible degradation pathways were proposed. The substantially decreased toxicity of CIP after the reaction was also observed. This work might provide new insights into the visible-light-assisted PMS activation mechanisms and is useful to construct environmentally-friendly catalytic processes for the efficient degradation of organic pollutants. Peroxymonosulfate (PMS) is extensively used as an oxidant to develop the sulfate radical-based advanced oxidation processes in the decontamination of organic pollutants and various PMS activation methods have been explored. Visible-light-assisted PMS activation to construct a Fenton-like process has shown a great potential for pollution control. In our work, BiVO₄ nanosheets were prepared using a hydrothermal process and used to activate PMS under visible light. A rapid degradation of ciprofloxacin (CIP) was achieved by dosing PMS (0.96 g/L), BiVO₄ (0.32 g/L) under visible light with a reaction rate constant of 77.72-fold higher than that in the BiVO₄/visible light process. The electron spin resonance and free radical quenching experiments indicate that reactive species of •O₂⁻, h⁺, •OH and SO₄•⁻ all worked, where h⁺, •OH and SO₄•⁻ were found as the dominant contributors to the CIP degradation. The spectroscopic analyses further demonstrate that the photoinduced electrons were directly involved in the PMS activation process. The generated •O₂⁻ was partially utilized to activate PMS and more •OH was produced because of the chain reactions between SO₄•⁻ and H₂O/OH⁻. In this process, PMS acted as an electron acceptor to transfer the photo-induced charges from the conduction band of BiVO₄ and PMS was successfully activated to yield the high-powered oxidative species. From the degradation intermediates of CIP detected by a liquid-chromatography-mass spectrometer, the possible degradation pathways were proposed. The substantially decreased toxicity of CIP after the reaction was also observed. This work might provide new insights into the visible-light-assisted PMS activation mechanisms and is useful to construct environmentally-friendly catalytic processes for the efficient degradation of organic pollutants. Peroxymonosulfate (PMS) is extensively used as an oxidant to develop the sulfate radical-based advanced oxidation processes in the decontamination of organic pollutants and various PMS activation methods have been explored. Visible-light-assisted PMS activation to construct a Fenton-like process has shown a great potential for pollution control. In our work, BiVO nanosheets were prepared using a hydrothermal process and used to activate PMS under visible light. A rapid degradation of ciprofloxacin (CIP) was achieved by dosing PMS (0.96 g/L), BiVO (0.32 g/L) under visible light with a reaction rate constant of 77.72-fold higher than that in the BiVO /visible light process. The electron spin resonance and free radical quenching experiments indicate that reactive species of O , h , •OH and SO all worked, where h , •OH and SO were found as the dominant contributors to the CIP degradation. The spectroscopic analyses further demonstrate that the photoinduced electrons were directly involved in the PMS activation process. The generated O was partially utilized to activate PMS and more •OH was produced because of the chain reactions between SO and H O/OH . In this process, PMS acted as an electron acceptor to transfer the photo-induced charges from the conduction band of BiVO and PMS was successfully activated to yield the high-powered oxidative species. From the degradation intermediates of CIP detected by a liquid-chromatography-mass spectrometer, the possible degradation pathways were proposed. The substantially decreased toxicity of CIP after the reaction was also observed. This work might provide new insights into the visible-light-assisted PMS activation mechanisms and is useful to construct environmentally-friendly catalytic processes for the efficient degradation of organic pollutants. |
| ArticleNumber | 115559 |
| Author | Chen, Fei Yu, Han-Qing Huang, Gui-Xiang Zheng, Yu-Ming Yang, Qi Yao, Fu-Bing Zhao, Quan-Bao |
| Author_xml | – sequence: 1 givenname: Fei surname: Chen fullname: Chen, Fei organization: CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science & Technology of China, Hefei, China – sequence: 2 givenname: Gui-Xiang surname: Huang fullname: Huang, Gui-Xiang organization: CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science & Technology of China, Hefei, China – sequence: 3 givenname: Fu-Bing surname: Yao fullname: Yao, Fu-Bing organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, China – sequence: 4 givenname: Qi orcidid: 0000-0001-6781-770X surname: Yang fullname: Yang, Qi organization: College of Environmental Science and Engineering, Hunan University, Changsha, 410082, China – sequence: 5 givenname: Yu-Ming orcidid: 0000-0002-3858-1037 surname: Zheng fullname: Zheng, Yu-Ming organization: CAS Key Laboratory of Urban Pollutant Conversion, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, 361021, China – sequence: 6 givenname: Quan-Bao surname: Zhao fullname: Zhao, Quan-Bao organization: CAS Key Laboratory of Urban Pollutant Conversion, Institute of Urban Environment, Chinese Academy of Sciences, Xiamen, 361021, China – sequence: 7 givenname: Han-Qing orcidid: 0000-0001-5247-6244 surname: Yu fullname: Yu, Han-Qing email: hqyu@ustc.edu.cn organization: CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science & Technology of China, Hefei, China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/32028250$$D View this record in MEDLINE/PubMed |
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| SubjectTerms | BiVO4 Catalysis Catalytic degradation Ciprofloxacin decontamination electron paramagnetic resonance spectroscopy free radicals Light Mechanism nanosheets oxidants oxidation Peroxides Peroxymonosulfate pollution control spectrometers sulfates toxicity Visible light water Water treatment |
| Title | Catalytic degradation of ciprofloxacin by a visible-light-assisted peroxymonosulfate activation system: Performance and mechanism |
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