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<p> A&#xa0;novel colorimetric sensor was designed&#xa0;for sensitive perfluorooctanoic&#xa0;acid (PFOA) detection based on a fluorine-functionalized Ce-metal–organic framework (F-Ce-UiO-66-NH<sub>2</sub>) with oxidase-like activity, using 3,3′,5,5′-tetramethylbenzidine (TMB) as the chromogenic substrate. This F-Ce-UiO-66-NH<sub>2</sub> was synthesized through ligand exchange and post-modification with pentafluorobenzaldehyde (PFBA) on the basis of Ce-terephthalic acid (Ce-UiO-66), incorporating pentafluorophenyl groups that enhance the material’s affinity for PFOA, leading to a more sensitive absorbance change in the presence of PFOA. Experimental and computational assays revealed that oxidase-like activity of F-Ce-UiO-66-NH<sub>2</sub> primarily arises from hydroxyl radicals (•OH) generated through the conversion of superoxide radicals (•O<sub>2</sub><sup>−</sup>). Furthermore, PFOA molecules were shown to undergo self-aggregation on the F-Ce-UiO-66-NH<sub>2</sub> surface via fluorine-fluorine (F-F) interactions between PFOA molecules and the pentafluorophenyl groups as well as between PFOA themselves, blocking the active Ce sites and hindering the interaction of O<sub>2</sub> and TMB with F-Ce-UiO-66-NH<sub>2</sub>, thereby diminishing its oxidase-like activity. Owing to these sophisticated mechanisms, this colorimetric sensor demonstrated a broad linear detection range from 0.5 to 210&#xa0;µM with a low detection limit of 0.41&#xa0;µM for PFOA, enabling precise quantification of PFOA concentrations in real environmental water samples. This work introduces a new strategy for constructing field-deployable colorimetric sensors based on F-F interaction, offering very valuable insights into the design and operational principle for PFAS detection.</p> Graphical Abstract <p></p>

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Fluorine-fluorine interaction-driven colorimetric sensor for PFOA-sensitive detection using F-functionalized Ce-UiO-66-NH2 MOF with oxidase-like activity

  • 期刊论文

  • 发表日期：

    2025年2月6日

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  • Nairong Yang,
  • Xinyu Lin,
  • Xiaomei Zheng,
  • Wenqiang Lai,
  • Youxiu Lin,
  • Zehua Zou,
  • Qingxiang Wang,
  • Xuan Zheng

摘要

A novel colorimetric sensor was designed for sensitive perfluorooctanoic acid (PFOA) detection based on a fluorine-functionalized Ce-metal–organic framework (F-Ce-UiO-66-NH2) with oxidase-like activity, using 3,3′,5,5′-tetramethylbenzidine (TMB) as the chromogenic substrate. This F-Ce-UiO-66-NH2 was synthesized through ligand exchange and post-modification with pentafluorobenzaldehyde (PFBA) on the basis of Ce-terephthalic acid (Ce-UiO-66), incorporating pentafluorophenyl groups that enhance the material’s affinity for PFOA, leading to a more sensitive absorbance change in the presence of PFOA. Experimental and computational assays revealed that oxidase-like activity of F-Ce-UiO-66-NH2 primarily arises from hydroxyl radicals (•OH) generated through the conversion of superoxide radicals (•O2−). Furthermore, PFOA molecules were shown to undergo self-aggregation on the F-Ce-UiO-66-NH2 surface via fluorine-fluorine (F-F) interactions between PFOA molecules and the pentafluorophenyl groups as well as between PFOA themselves, blocking the active Ce sites and hindering the interaction of O2 and TMB with F-Ce-UiO-66-NH2, thereby diminishing its oxidase-like activity. Owing to these sophisticated mechanisms, this colorimetric sensor demonstrated a broad linear detection range from 0.5 to 210 µM with a low detection limit of 0.41 µM for PFOA, enabling precise quantification of PFOA concentrations in real environmental water samples. This work introduces a new strategy for constructing field-deployable colorimetric sensors based on F-F interaction, offering very valuable insights into the design and operational principle for PFAS detection.

Graphical Abstract