Solar-driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproducts
Abstract The recalcitrance of fluorinated organic pollutants—featuring robust Csp²-F and Csp³-F bonds—poses critical challenges to aquatic ecosystems due to their extreme persistence and bioaccumulation. Whereas current destruction strategies suffer from high energy consumption and non-selective, he...
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Nature Portfolio
2025-08-01
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| Series: | Communications Chemistry |
| Online Access: | https://doi.org/10.1038/s42004-025-01655-3 |
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| author | Lei Zheng Jing-Lan Zhang Zhixin Zheng Chujie Huang Yi-Lin Xie Xu-Bing Li Wondu Dagnaw Fentahun Tieyu Wang Qing-Xiao Tong Jing-Xin Jian |
| author_facet | Lei Zheng Jing-Lan Zhang Zhixin Zheng Chujie Huang Yi-Lin Xie Xu-Bing Li Wondu Dagnaw Fentahun Tieyu Wang Qing-Xiao Tong Jing-Xin Jian |
| author_sort | Lei Zheng |
| collection | DOAJ |
| description | Abstract The recalcitrance of fluorinated organic pollutants—featuring robust Csp²-F and Csp³-F bonds—poses critical challenges to aquatic ecosystems due to their extreme persistence and bioaccumulation. Whereas current destruction strategies suffer from high energy consumption and non-selective, here we present a solar-powered mineralization strategy utilizing cerium oxide/mesoporous silica (CeO2/mSiO2) heterojunction photocatalysts for complete defluorination of organofluorine contaminants, including fluorinated e-waste, fluoro-antibiotics and perfluorinated surfactant. Under visible light irradiation, the optimized 5%CeO2/mSiO2 achieved 91.1 ± 3.2% octafluorobiphenyl (OFB) and 97.7 ± 2.8% fleroxacin (FLE) degradations within 6 h. Notably, the ‘forever chemical’ perfluorooctanesulfonic acid (PFOS) can be effectively destructed, achieving a maximum of 25.9 ± 2.7% reduction in 5 days under sunshine, outperforming parallel experiments conducted without a catalyst (~0%). This process notably avoids the evolution of fluoride ions. Theoretical calculations reveal that the removal of C-F bonds by photogenerated hydroxyl radical is thermodynamically superior to hydroxyl-mediated defluorination. This work establishes an energy-efficient paradigm for eradicating “forever chemicals” without secondary pollution, advancing sustainable water remediation technologies. |
| format | Article |
| id | doaj-art-b61ccf2ade1a41ebb85cf278585d0e91 |
| institution | Kabale University |
| issn | 2399-3669 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Communications Chemistry |
| spelling | doaj-art-b61ccf2ade1a41ebb85cf278585d0e912025-08-20T03:46:54ZengNature PortfolioCommunications Chemistry2399-36692025-08-018111110.1038/s42004-025-01655-3Solar-driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproductsLei Zheng0Jing-Lan Zhang1Zhixin Zheng2Chujie Huang3Yi-Lin Xie4Xu-Bing Li5Wondu Dagnaw Fentahun6Tieyu Wang7Qing-Xiao Tong8Jing-Xin Jian9Department of Chemistry, Shantou UniversityDepartment of Chemistry, Shantou UniversityGuangdong Provincial Key Laboratory of Marine Disaster Prediction and Prevention, Shantou UniversityGuangdong Provincial Key Laboratory of Marine Disaster Prediction and Prevention, Shantou UniversityDepartment of Chemistry, Shantou UniversityKey Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of SciencesDepartment of Chemistry, Shantou UniversityGuangdong Provincial Key Laboratory of Marine Disaster Prediction and Prevention, Shantou UniversityDepartment of Chemistry, Shantou UniversityDepartment of Chemistry, Shantou UniversityAbstract The recalcitrance of fluorinated organic pollutants—featuring robust Csp²-F and Csp³-F bonds—poses critical challenges to aquatic ecosystems due to their extreme persistence and bioaccumulation. Whereas current destruction strategies suffer from high energy consumption and non-selective, here we present a solar-powered mineralization strategy utilizing cerium oxide/mesoporous silica (CeO2/mSiO2) heterojunction photocatalysts for complete defluorination of organofluorine contaminants, including fluorinated e-waste, fluoro-antibiotics and perfluorinated surfactant. Under visible light irradiation, the optimized 5%CeO2/mSiO2 achieved 91.1 ± 3.2% octafluorobiphenyl (OFB) and 97.7 ± 2.8% fleroxacin (FLE) degradations within 6 h. Notably, the ‘forever chemical’ perfluorooctanesulfonic acid (PFOS) can be effectively destructed, achieving a maximum of 25.9 ± 2.7% reduction in 5 days under sunshine, outperforming parallel experiments conducted without a catalyst (~0%). This process notably avoids the evolution of fluoride ions. Theoretical calculations reveal that the removal of C-F bonds by photogenerated hydroxyl radical is thermodynamically superior to hydroxyl-mediated defluorination. This work establishes an energy-efficient paradigm for eradicating “forever chemicals” without secondary pollution, advancing sustainable water remediation technologies.https://doi.org/10.1038/s42004-025-01655-3 |
| spellingShingle | Lei Zheng Jing-Lan Zhang Zhixin Zheng Chujie Huang Yi-Lin Xie Xu-Bing Li Wondu Dagnaw Fentahun Tieyu Wang Qing-Xiao Tong Jing-Xin Jian Solar-driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproducts Communications Chemistry |
| title | Solar-driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproducts |
| title_full | Solar-driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproducts |
| title_fullStr | Solar-driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproducts |
| title_full_unstemmed | Solar-driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproducts |
| title_short | Solar-driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproducts |
| title_sort | solar driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproducts |
| url | https://doi.org/10.1038/s42004-025-01655-3 |
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