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<p>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 (CeO<sub>2</sub>/mSiO<sub>2</sub>) heterojunction photocatalysts for complete defluorination of organofluorine contaminants, including fluorinated e-waste, fluoro-antibiotics and perfluorinated surfactant. Under visible light irradiation, the optimized 5%CeO<sub>2</sub>/mSiO<sub>2</sub> 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.</p>

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Solar-driven defluorination via hydroxyl radical spillover for complete mineralization of organofluorine pollutants without fluoride byproducts

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年8月16日

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  • 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

摘要

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.