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<p>Fluoroarenes persist in aquatic environments because aromatic delocalization and aqueous speciation suppress selective C-F bond cleavage, limiting both reductive activation and direct hole oxidation. Hydroxyl radicals (·OH) can mineralize these contaminants, yet near-neutral·OH generation typically relies on added oxidants or Fenton chemistry, creating chemical demand and secondary residues. Here we report a carboxyl-functionalized crystalline perylene diimide photocatalyst (Carboxyl-PDI) that produces ·OH via a catalytic carboxyl-peroxyacid cycle under visible light. Carboxyl-PDI delivers a 50.94% apparent quantum yield for ·OH at 600 nm, achieves complete defluorination of 100 mg L<sup>−1</sup> perfluorophenol under AM1.5 G irradiation, and retains stable capacity for &gt;500 h. Isotope labelling mass spectrometry and theoretical calculation identify a -COOOH intermediate and show hydrogen-bond gating to a neighbouring PDI carbonyl weakens the O-O bond by ~0.31 eV, enabling low-barrier homolysis for producing ·OH. A continuous-flow outdoor-sunlight reactor reaches 95.85% degradation, 90.67% defluorination and 79.68% mineralization, demonstrating scalable oxidant-free defluorination of perfluorophenol.</p>

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Solar-driven peroxyacid group activation enables＞ 500 h stable hydroxyl-radical defluorination of industrial perfluorophenol wastewater

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月24日

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  • Yunning Chen,
  • Qixin Zhou,
  • Yan Guo,
  • Zhengkai Wu,
  • Haoying Wang,
  • Yizhou Yan,
  • Xinghao Qi,
  • Liping Liu,
  • Jingbin Han,
  • Qingkun Shang,
  • Yongfa Zhu

摘要

Fluoroarenes persist in aquatic environments because aromatic delocalization and aqueous speciation suppress selective C-F bond cleavage, limiting both reductive activation and direct hole oxidation. Hydroxyl radicals (·OH) can mineralize these contaminants, yet near-neutral·OH generation typically relies on added oxidants or Fenton chemistry, creating chemical demand and secondary residues. Here we report a carboxyl-functionalized crystalline perylene diimide photocatalyst (Carboxyl-PDI) that produces ·OH via a catalytic carboxyl-peroxyacid cycle under visible light. Carboxyl-PDI delivers a 50.94% apparent quantum yield for ·OH at 600 nm, achieves complete defluorination of 100 mg L−1 perfluorophenol under AM1.5 G irradiation, and retains stable capacity for >500 h. Isotope labelling mass spectrometry and theoretical calculation identify a -COOOH intermediate and show hydrogen-bond gating to a neighbouring PDI carbonyl weakens the O-O bond by ~0.31 eV, enabling low-barrier homolysis for producing ·OH. A continuous-flow outdoor-sunlight reactor reaches 95.85% degradation, 90.67% defluorination and 79.68% mineralization, demonstrating scalable oxidant-free defluorination of perfluorophenol.