Efficient activation of PAA by FeS for fast removal of pharmaceuticals: The dual role of sulfur species in regulating the reactive oxidized species
•Satisfactory degradation efficiency of pollutants was achieved by FeS/PAA system.•S(-II) and H2S (aq) played a significant role in Fe(II) regeneration.••OH played a dominant role in pharmaceuticals degradation.•The R-O• generated was supposed to be quickly consumed by sulfur specie.•Degradation pro...
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| Published in | Water research (Oxford) Vol. 217; p. 118402 |
|---|---|
| Main Authors | , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
England
Elsevier Ltd
15.06.2022
|
| Subjects | |
| Online Access | Get full text |
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| Abstract | •Satisfactory degradation efficiency of pollutants was achieved by FeS/PAA system.•S(-II) and H2S (aq) played a significant role in Fe(II) regeneration.••OH played a dominant role in pharmaceuticals degradation.•The R-O• generated was supposed to be quickly consumed by sulfur specie.•Degradation products of three pharmaceuticals were successfully detoxified.
As peracetic acid (PAA) is being increasingly used as an alternative disinfectant, efficient activation of PAA by low-cost and environmentally friendly catalysts over a wide pH range is potentially useful for simultaneous sterilization and pharmaceutical degradation in wastewater, such as hospital wastewater. In this study, peracetic acid (PAA) was successfully activated by low-cost and environmental-friendly FeS (25 mg/L) for efficient oxidative removal of three pharmaceuticals over a wide pH range (3.0∼9.0) as indicated by 80∼100% removal rate within 5 min. As expected, Fe(II) rather than sulfur species was the primary reactive site for PAA activation, while unlike the homogeneous Fe2+/PAA system with organic radicals (R-O·) and ·OH as the dominant reactive oxidized species (ROS), ·OH is the key reactive species in the FeS/PAA system. Interestingly and surprisingly, in-depth investigation revealed the dual role of sulfur species in regulating the reactive oxidized species: (1) S(-II) and its conversion product H2S (aq) played a significant role in Fe(II) regeneration with a result of accelerated PAA activation; (2) however, the R-O· generated in the initial seconds of the FeS/PAA process was supposed to be quickly consumed by sulfur species, resulting in ·OH as the dominant ROS over the whole process. The selective reaction of sulfur species with R-O· instead of ·OH was supported by the obviously lower Gibbs free energy of CH3COO· and sulfur species than ·OH, suggesting the preference of CH3COO· to react with sulfur species with electron transfer. After treatment with the FeS/PAA system, the products obtained from the three pharmaceuticals were detoxified and even facilitated the growth of E. coli probably due to the supply of numerous carbon sources by activated PAA. This study significantly advances the understanding of the reaction between PAA and sulfur-containing catalysts and suggests the practical application potential of the FeS/PAA process combined with biotreatment processes.
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| AbstractList | As peracetic acid (PAA) is being increasingly used as an alternative disinfectant, efficient activation of PAA by low-cost and environmentally friendly catalysts over a wide pH range is potentially useful for simultaneous sterilization and pharmaceutical degradation in wastewater, such as hospital wastewater. In this study, peracetic acid (PAA) was successfully activated by low-cost and environmental-friendly FeS (25 mg/L) for efficient oxidative removal of three pharmaceuticals over a wide pH range (3.0∼9.0) as indicated by 80∼100% removal rate within 5 min. As expected, Fe(II) rather than sulfur species was the primary reactive site for PAA activation, while unlike the homogeneous Fe2+/PAA system with organic radicals (R-O·) and ·OH as the dominant reactive oxidized species (ROS), ·OH is the key reactive species in the FeS/PAA system. Interestingly and surprisingly, in-depth investigation revealed the dual role of sulfur species in regulating the reactive oxidized species: (1) S(-II) and its conversion product H2S (aq) played a significant role in Fe(II) regeneration with a result of accelerated PAA activation; (2) however, the R-O· generated in the initial seconds of the FeS/PAA process was supposed to be quickly consumed by sulfur species, resulting in ·OH as the dominant ROS over the whole process. The selective reaction of sulfur species with R-O· instead of ·OH was supported by the obviously lower Gibbs free energy of CH3COO· and sulfur species than ·OH, suggesting the preference of CH3COO· to react with sulfur species with electron transfer. After treatment with the FeS/PAA system, the products obtained from the three pharmaceuticals were detoxified and even facilitated the growth of E. coli probably due to the supply of numerous carbon sources by activated PAA. This study significantly advances the understanding of the reaction between PAA and sulfur-containing catalysts and suggests the practical application potential of the FeS/PAA process combined with biotreatment processes.As peracetic acid (PAA) is being increasingly used as an alternative disinfectant, efficient activation of PAA by low-cost and environmentally friendly catalysts over a wide pH range is potentially useful for simultaneous sterilization and pharmaceutical degradation in wastewater, such as hospital wastewater. In this study, peracetic acid (PAA) was successfully activated by low-cost and environmental-friendly FeS (25 mg/L) for efficient oxidative removal of three pharmaceuticals over a wide pH range (3.0∼9.0) as indicated by 80∼100% removal rate within 5 min. As expected, Fe(II) rather than sulfur species was the primary reactive site for PAA activation, while unlike the homogeneous Fe2+/PAA system with organic radicals (R-O·) and ·OH as the dominant reactive oxidized species (ROS), ·OH is the key reactive species in the FeS/PAA system. Interestingly and surprisingly, in-depth investigation revealed the dual role of sulfur species in regulating the reactive oxidized species: (1) S(-II) and its conversion product H2S (aq) played a significant role in Fe(II) regeneration with a result of accelerated PAA activation; (2) however, the R-O· generated in the initial seconds of the FeS/PAA process was supposed to be quickly consumed by sulfur species, resulting in ·OH as the dominant ROS over the whole process. The selective reaction of sulfur species with R-O· instead of ·OH was supported by the obviously lower Gibbs free energy of CH3COO· and sulfur species than ·OH, suggesting the preference of CH3COO· to react with sulfur species with electron transfer. After treatment with the FeS/PAA system, the products obtained from the three pharmaceuticals were detoxified and even facilitated the growth of E. coli probably due to the supply of numerous carbon sources by activated PAA. This study significantly advances the understanding of the reaction between PAA and sulfur-containing catalysts and suggests the practical application potential of the FeS/PAA process combined with biotreatment processes. •Satisfactory degradation efficiency of pollutants was achieved by FeS/PAA system.•S(-II) and H2S (aq) played a significant role in Fe(II) regeneration.••OH played a dominant role in pharmaceuticals degradation.•The R-O• generated was supposed to be quickly consumed by sulfur specie.•Degradation products of three pharmaceuticals were successfully detoxified. As peracetic acid (PAA) is being increasingly used as an alternative disinfectant, efficient activation of PAA by low-cost and environmentally friendly catalysts over a wide pH range is potentially useful for simultaneous sterilization and pharmaceutical degradation in wastewater, such as hospital wastewater. In this study, peracetic acid (PAA) was successfully activated by low-cost and environmental-friendly FeS (25 mg/L) for efficient oxidative removal of three pharmaceuticals over a wide pH range (3.0∼9.0) as indicated by 80∼100% removal rate within 5 min. As expected, Fe(II) rather than sulfur species was the primary reactive site for PAA activation, while unlike the homogeneous Fe2+/PAA system with organic radicals (R-O·) and ·OH as the dominant reactive oxidized species (ROS), ·OH is the key reactive species in the FeS/PAA system. Interestingly and surprisingly, in-depth investigation revealed the dual role of sulfur species in regulating the reactive oxidized species: (1) S(-II) and its conversion product H2S (aq) played a significant role in Fe(II) regeneration with a result of accelerated PAA activation; (2) however, the R-O· generated in the initial seconds of the FeS/PAA process was supposed to be quickly consumed by sulfur species, resulting in ·OH as the dominant ROS over the whole process. The selective reaction of sulfur species with R-O· instead of ·OH was supported by the obviously lower Gibbs free energy of CH3COO· and sulfur species than ·OH, suggesting the preference of CH3COO· to react with sulfur species with electron transfer. After treatment with the FeS/PAA system, the products obtained from the three pharmaceuticals were detoxified and even facilitated the growth of E. coli probably due to the supply of numerous carbon sources by activated PAA. This study significantly advances the understanding of the reaction between PAA and sulfur-containing catalysts and suggests the practical application potential of the FeS/PAA process combined with biotreatment processes. [Display omitted] As peracetic acid (PAA) is being increasingly used as an alternative disinfectant, efficient activation of PAA by low-cost and environmentally friendly catalysts over a wide pH range is potentially useful for simultaneous sterilization and pharmaceutical degradation in wastewater, such as hospital wastewater. In this study, peracetic acid (PAA) was successfully activated by low-cost and environmental-friendly FeS (25 mg/L) for efficient oxidative removal of three pharmaceuticals over a wide pH range (3.0∼9.0) as indicated by 80∼100% removal rate within 5 min. As expected, Fe(II) rather than sulfur species was the primary reactive site for PAA activation, while unlike the homogeneous Fe²⁺/PAA system with organic radicals (R-O·) and ·OH as the dominant reactive oxidized species (ROS), ·OH is the key reactive species in the FeS/PAA system. Interestingly and surprisingly, in-depth investigation revealed the dual role of sulfur species in regulating the reactive oxidized species: (1) S(-II) and its conversion product H₂S (aq) played a significant role in Fe(II) regeneration with a result of accelerated PAA activation; (2) however, the R-O· generated in the initial seconds of the FeS/PAA process was supposed to be quickly consumed by sulfur species, resulting in ·OH as the dominant ROS over the whole process. The selective reaction of sulfur species with R-O· instead of ·OH was supported by the obviously lower Gibbs free energy of CH₃COO· and sulfur species than ·OH, suggesting the preference of CH₃COO· to react with sulfur species with electron transfer. After treatment with the FeS/PAA system, the products obtained from the three pharmaceuticals were detoxified and even facilitated the growth of E. coli probably due to the supply of numerous carbon sources by activated PAA. This study significantly advances the understanding of the reaction between PAA and sulfur-containing catalysts and suggests the practical application potential of the FeS/PAA process combined with biotreatment processes. As peracetic acid (PAA) is being increasingly used as an alternative disinfectant, efficient activation of PAA by low-cost and environmentally friendly catalysts over a wide pH range is potentially useful for simultaneous sterilization and pharmaceutical degradation in wastewater, such as hospital wastewater. In this study, peracetic acid (PAA) was successfully activated by low-cost and environmental-friendly FeS (25 mg/L) for efficient oxidative removal of three pharmaceuticals over a wide pH range (3.0∼9.0) as indicated by 80∼100% removal rate within 5 min. As expected, Fe(II) rather than sulfur species was the primary reactive site for PAA activation, while unlike the homogeneous Fe /PAA system with organic radicals (R-O·) and ·OH as the dominant reactive oxidized species (ROS), ·OH is the key reactive species in the FeS/PAA system. Interestingly and surprisingly, in-depth investigation revealed the dual role of sulfur species in regulating the reactive oxidized species: (1) S(-II) and its conversion product H S (aq) played a significant role in Fe(II) regeneration with a result of accelerated PAA activation; (2) however, the R-O· generated in the initial seconds of the FeS/PAA process was supposed to be quickly consumed by sulfur species, resulting in ·OH as the dominant ROS over the whole process. The selective reaction of sulfur species with R-O· instead of ·OH was supported by the obviously lower Gibbs free energy of CH COO· and sulfur species than ·OH, suggesting the preference of CH COO· to react with sulfur species with electron transfer. After treatment with the FeS/PAA system, the products obtained from the three pharmaceuticals were detoxified and even facilitated the growth of E. coli probably due to the supply of numerous carbon sources by activated PAA. This study significantly advances the understanding of the reaction between PAA and sulfur-containing catalysts and suggests the practical application potential of the FeS/PAA process combined with biotreatment processes. |
| ArticleNumber | 118402 |
| Author | Li, Ling-Li Jiang, Feng Yang, Shu-Run Xie, Zhi-Hui Mu, Yang Xiong, Zhao-Kun He, Chuan-Shu Zhang, Heng Zhou, Peng Lai, Bo |
| Author_xml | – sequence: 1 givenname: Shu-Run surname: Yang fullname: Yang, Shu-Run organization: State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China – sequence: 2 givenname: Chuan-Shu surname: He fullname: He, Chuan-Shu email: hecs@scu.edu.cn organization: State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China – sequence: 3 givenname: Zhi-Hui surname: Xie fullname: Xie, Zhi-Hui organization: State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China – sequence: 4 givenname: Ling-Li orcidid: 0000-0003-0228-2550 surname: Li fullname: Li, Ling-Li organization: State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China – sequence: 5 givenname: Zhao-Kun surname: Xiong fullname: Xiong, Zhao-Kun organization: State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China – sequence: 6 givenname: Heng surname: Zhang fullname: Zhang, Heng organization: State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China – sequence: 7 givenname: Peng surname: Zhou fullname: Zhou, Peng organization: State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China – sequence: 8 givenname: Feng surname: Jiang fullname: Jiang, Feng organization: Guangdong Provincial Key Lab of Environmental Pollution Control and Remediation Technology, School of Environmental Science and Engineering, Sun Yat-Sen University, Guangzhou, China – sequence: 9 givenname: Yang surname: Mu fullname: Mu, Yang organization: Department of Environmental Science and Engineering, CAS Key Laboratory of Urban Pollutant Conversion, University of Science and Technology of China, Hefei 230026, China – sequence: 10 givenname: Bo surname: Lai fullname: Lai, Bo email: laibo@scu.edu.cn organization: State Key Laboratory of Hydraulics and Mountain River Engineering, College of Architecture and Environment, Sichuan University, Chengdu 610065, China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/35417819$$D View this record in MEDLINE/PubMed |
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| IngestDate | Fri Jul 11 07:03:12 EDT 2025 Fri Jul 11 01:47:36 EDT 2025 Thu Apr 03 07:06:53 EDT 2025 Tue Jul 01 01:21:12 EDT 2025 Thu Apr 24 22:58:38 EDT 2025 Fri Feb 23 02:35:26 EST 2024 |
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| Keywords | Organic radicals Pharmaceuticals degradation Sulfur species Peracetic acid FeS Reactive oxidized species |
| Language | English |
| License | Copyright © 2022 Elsevier Ltd. All rights reserved. |
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| Snippet | •Satisfactory degradation efficiency of pollutants was achieved by FeS/PAA system.•S(-II) and H2S (aq) played a significant role in Fe(II) regeneration.••OH... As peracetic acid (PAA) is being increasingly used as an alternative disinfectant, efficient activation of PAA by low-cost and environmentally friendly... |
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| SubjectTerms | carbon disinfectants drugs electron transfer Escherichia coli FeS Gibbs free energy hospitals Organic radicals oxidation Peracetic acid Pharmaceuticals degradation Reactive oxidized species sulfur Sulfur species wastewater water |
| Title | Efficient activation of PAA by FeS for fast removal of pharmaceuticals: The dual role of sulfur species in regulating the reactive oxidized species |
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