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<p>The environmental persistence of per- and polyfluoroalkyl substances (PFASs), driven by the exceptional stability of their C–F bonds, presents a formidable challenge for remediation. Herein, we report the 5,10,15,20-tetraphenyl (4-aminophenyl) porphyrin (TAPP) aggregates as visible-light-driven photocatalysts capable of achieving almost-100% defluorination of PFASs without chemical additives. Central to this process is the ultra-stable TAPP radical species (TAPP<sup>•</sup>), which exhibits a lifetime exceeding 7 days under ambient conditions. Under visible-light irradiation, TAPP<sup>•</sup> generates reductive electrons with a potential of −2.68 V<sub>NHE</sub>, enabling injection into the C–F antibonding orbitals to initiate defluorination. The exceptional stability of TAPP<sup>•</sup> arises from intramolecular charge delocalization mediated by the synergistic overlap between the lone-pair electrons distribution of the amino groups and the highest occupied molecular orbital. This work develops a steady radical strategy that leverages charge-delocalization to engineer photocatalysts with highly reductive electron, offering an approach to address persistent environmental contaminants.</p>

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Complete defluorination of PFASs via photocatalytic reduction in water

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月23日

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  • MeiChi Chong,
  • Qixin Zhou,
  • Jingyi Xu,
  • Zhaohui Wu,
  • Enwei Zhu,
  • Wenlu Li,
  • Ling Zhang,
  • Yan Guo,
  • Yongfa Zhu

摘要

The environmental persistence of per- and polyfluoroalkyl substances (PFASs), driven by the exceptional stability of their C–F bonds, presents a formidable challenge for remediation. Herein, we report the 5,10,15,20-tetraphenyl (4-aminophenyl) porphyrin (TAPP) aggregates as visible-light-driven photocatalysts capable of achieving almost-100% defluorination of PFASs without chemical additives. Central to this process is the ultra-stable TAPP radical species (TAPP•), which exhibits a lifetime exceeding 7 days under ambient conditions. Under visible-light irradiation, TAPP• generates reductive electrons with a potential of −2.68 VNHE, enabling injection into the C–F antibonding orbitals to initiate defluorination. The exceptional stability of TAPP• arises from intramolecular charge delocalization mediated by the synergistic overlap between the lone-pair electrons distribution of the amino groups and the highest occupied molecular orbital. This work develops a steady radical strategy that leverages charge-delocalization to engineer photocatalysts with highly reductive electron, offering an approach to address persistent environmental contaminants.