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<p>Per- and polyfluoroalkyl substances (PFAS) are among the most persistent and challenging environmental pollutants. Compared with conventional oxidative or homogeneous reduction processes, electrochemical and photoelectrochemical reduction (ER and PER) offer reagent-free routes for PFAS destruction but remain limited by poor PFAS removal and sluggish defluorination under cathodic conditions. Here, we report a Pd-decorated TiO<sub>2</sub> cathode that enables highly efficient photoelectrochemical degradation of perfluorooctane sulfonic acid (PFOS) under ambient conditions. Operando spectroscopy and density functional theory (DFT) calculations uncover a previously unrecognized mechanism in which cathodic potentials promote PFAS adsorption on TiO<sub>2</sub>, while UV<sub>254</sub>-excited Pd sites generate hot electrons that directly drive C–F bond cleavage or form hydrated electrons for indirect reduction. This dual-electron pathway leads to rapid and deep defluorination, outperforming previously reported ER and PER systems even in complex matrices such as reverse osmosis concentrate (ROC) and aqueous film-forming foam (AFFF)-impacted water. The study further demonstrates scalable single-chamber reactor designs and mesh-type cathodes, advancing the practical implementation of photoelectrochemical PFAS destruction technologies.</p>

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Photo-electrochemical reduction of PFAS in complex water matrices

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年3月28日

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  • Yunqiao Guan,
  • Ankush Jain,
  • Xiaotian Xu,
  • Aidan Francis Meese,
  • Yu Yan,
  • Jae-Hong Kim,
  • Christopher Muhich,
  • Yang Yang

摘要

Per- and polyfluoroalkyl substances (PFAS) are among the most persistent and challenging environmental pollutants. Compared with conventional oxidative or homogeneous reduction processes, electrochemical and photoelectrochemical reduction (ER and PER) offer reagent-free routes for PFAS destruction but remain limited by poor PFAS removal and sluggish defluorination under cathodic conditions. Here, we report a Pd-decorated TiO2 cathode that enables highly efficient photoelectrochemical degradation of perfluorooctane sulfonic acid (PFOS) under ambient conditions. Operando spectroscopy and density functional theory (DFT) calculations uncover a previously unrecognized mechanism in which cathodic potentials promote PFAS adsorption on TiO2, while UV254-excited Pd sites generate hot electrons that directly drive C–F bond cleavage or form hydrated electrons for indirect reduction. This dual-electron pathway leads to rapid and deep defluorination, outperforming previously reported ER and PER systems even in complex matrices such as reverse osmosis concentrate (ROC) and aqueous film-forming foam (AFFF)-impacted water. The study further demonstrates scalable single-chamber reactor designs and mesh-type cathodes, advancing the practical implementation of photoelectrochemical PFAS destruction technologies.