Supercritical water oxidation of chlorophenols: Catalytic effect, auxiliary fuels, reaction mechanism, and degradation pathway
In this study, the supercritical water oxidation (SCWO) processes of monochlorophenols (ortho-, meta-, and para-chlorophenol, 2-, 3-, and 4-CP), dichlorophenol (2,4-DCP), and trichlorophenol (2,4,6-TCP) were investigated on the basis of experimental data combined with density functional theory (DFT)...
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Elsevier
2025-04-01
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| Series: | Desalination and Water Treatment |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S1944398625002498 |
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| author | Xin Peng Huiyin Luo Li Zeng Zhiwen Cheng Qingyuan Wang Bowen Yang |
| author_facet | Xin Peng Huiyin Luo Li Zeng Zhiwen Cheng Qingyuan Wang Bowen Yang |
| author_sort | Xin Peng |
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| description | In this study, the supercritical water oxidation (SCWO) processes of monochlorophenols (ortho-, meta-, and para-chlorophenol, 2-, 3-, and 4-CP), dichlorophenol (2,4-DCP), and trichlorophenol (2,4,6-TCP) were investigated on the basis of experimental data combined with density functional theory (DFT). SCWO experiments were performed in a coiled tubular reactor at 650–800 K, 24 MPa, and 300 % excess oxygen within 5 min with or without catalysts and/or auxiliary fuels. The results indicated that i) the removal efficiency for trichlorophenol was better than those for dichlorophenol and the monochlorophenols; ii) for the three monochlorophenols, the removal efficiencies were in the order of 4-CP > 2-CP > 3-CP; and iii) the chlorophenol removal efficiency increased in the presence of Cu(II) and isopropyl alcohol (IPA). The Fukui index data supported the experimental findings, which showed that i) Cl atoms in the para-position were more susceptible to radical attack than those in the ortho- and meta-positions; ii) the Fukui values of Cl atom(s) were greater than those of carbon, hydrogen, and oxygen atoms; and iii) 2,4-DCP and 2,4,6-TCP could provide more active sites than the monochlorophenols because they possessed more Cl atoms. On the basis of these results, a pathway for the degradation of chlorophenols involving dechlorination, ring opening, and mineralization was proposed. |
| format | Article |
| id | doaj-art-670d3522a88d4ec0b2796eaff0d1e1b9 |
| institution | DOAJ |
| issn | 1944-3986 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Elsevier |
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| series | Desalination and Water Treatment |
| spelling | doaj-art-670d3522a88d4ec0b2796eaff0d1e1b92025-08-20T03:07:51ZengElsevierDesalination and Water Treatment1944-39862025-04-0132210123310.1016/j.dwt.2025.101233Supercritical water oxidation of chlorophenols: Catalytic effect, auxiliary fuels, reaction mechanism, and degradation pathwayXin Peng0Huiyin Luo1Li Zeng2Zhiwen Cheng3Qingyuan Wang4Bowen Yang5Sichuan Provincial Engineering Research Center of City Solid Waste Energy and Building Materials Conversion and Utilization Technology, Chengdu University, Chengdu 610106, China; State Key Laboratory of Subtropical Silviculture, Zhejiang A&F University, Hangzhou, Zhejiang 311300, China; College of Architecture & Environment, Sichuan University, Chengdu 61000, ChinaSichuan Provincial Engineering Research Center of City Solid Waste Energy and Building Materials Conversion and Utilization Technology, Chengdu University, Chengdu 610106, ChinaSichuan Provincial Engineering Research Center of City Solid Waste Energy and Building Materials Conversion and Utilization Technology, Chengdu University, Chengdu 610106, ChinaSchool of Chemical and Environmental Engineering, Shanghai Institute of Technology, 100 Haiquan Road, Shanghai 201418, ChinaSichuan Provincial Engineering Research Center of City Solid Waste Energy and Building Materials Conversion and Utilization Technology, Chengdu University, Chengdu 610106, China; College of Architecture & Environment, Sichuan University, Chengdu 61000, China; Correspondence to: Chengdu University, 2025 Chengluo Road, Chengdu 610106, China.Sichuan Provincial Engineering Research Center of City Solid Waste Energy and Building Materials Conversion and Utilization Technology, Chengdu University, Chengdu 610106, China; Guangxi Key Laboratory of Environmental Pollution Control Theory and Technology, Guilin University of Technology, Guilin 541004, China; Correspondence to: School of Architecture and Civil Engineering, Chengdu University, 2025 Chengluo Road, Chengdu 610106, China.In this study, the supercritical water oxidation (SCWO) processes of monochlorophenols (ortho-, meta-, and para-chlorophenol, 2-, 3-, and 4-CP), dichlorophenol (2,4-DCP), and trichlorophenol (2,4,6-TCP) were investigated on the basis of experimental data combined with density functional theory (DFT). SCWO experiments were performed in a coiled tubular reactor at 650–800 K, 24 MPa, and 300 % excess oxygen within 5 min with or without catalysts and/or auxiliary fuels. The results indicated that i) the removal efficiency for trichlorophenol was better than those for dichlorophenol and the monochlorophenols; ii) for the three monochlorophenols, the removal efficiencies were in the order of 4-CP > 2-CP > 3-CP; and iii) the chlorophenol removal efficiency increased in the presence of Cu(II) and isopropyl alcohol (IPA). The Fukui index data supported the experimental findings, which showed that i) Cl atoms in the para-position were more susceptible to radical attack than those in the ortho- and meta-positions; ii) the Fukui values of Cl atom(s) were greater than those of carbon, hydrogen, and oxygen atoms; and iii) 2,4-DCP and 2,4,6-TCP could provide more active sites than the monochlorophenols because they possessed more Cl atoms. On the basis of these results, a pathway for the degradation of chlorophenols involving dechlorination, ring opening, and mineralization was proposed.http://www.sciencedirect.com/science/article/pii/S1944398625002498ChlorophenolsSupercritical water oxidationCationsIsopropyl alcoholDensity functional theory |
| spellingShingle | Xin Peng Huiyin Luo Li Zeng Zhiwen Cheng Qingyuan Wang Bowen Yang Supercritical water oxidation of chlorophenols: Catalytic effect, auxiliary fuels, reaction mechanism, and degradation pathway Desalination and Water Treatment Chlorophenols Supercritical water oxidation Cations Isopropyl alcohol Density functional theory |
| title | Supercritical water oxidation of chlorophenols: Catalytic effect, auxiliary fuels, reaction mechanism, and degradation pathway |
| title_full | Supercritical water oxidation of chlorophenols: Catalytic effect, auxiliary fuels, reaction mechanism, and degradation pathway |
| title_fullStr | Supercritical water oxidation of chlorophenols: Catalytic effect, auxiliary fuels, reaction mechanism, and degradation pathway |
| title_full_unstemmed | Supercritical water oxidation of chlorophenols: Catalytic effect, auxiliary fuels, reaction mechanism, and degradation pathway |
| title_short | Supercritical water oxidation of chlorophenols: Catalytic effect, auxiliary fuels, reaction mechanism, and degradation pathway |
| title_sort | supercritical water oxidation of chlorophenols catalytic effect auxiliary fuels reaction mechanism and degradation pathway |
| topic | Chlorophenols Supercritical water oxidation Cations Isopropyl alcohol Density functional theory |
| url | http://www.sciencedirect.com/science/article/pii/S1944398625002498 |
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