<p>Refractory wastewater treatment via Fenton reactions is hindered by iron sludge. Herein, fluorinated UiO-66(Zr)-F4 was employed as a hydrogen-storage carrier to confine Pd⁰ catalytic centers, and an [H]-mediated (H<sub>2</sub>-precursored) Fenton-like system was constructed for carbamazepine degradation under ambient conditions. With 25&#xa0;μM Fe<sup>2</sup> + and 60&#xa0;mL min⁻<sup>1</sup> H<sub>2</sub> flow, 53% carbamazepine removal was achieved in 1&#xa0;h via ⋅OH/<sup>1</sup>O<sub>2</sub> oxidation, and &gt; 59% efficiency was retained over six 3-h cycles. However, [H]-driven hydrogen spillover reduced C-F bonds, causing a 92.3% drop in specific surface area that compromised long-term stability. It was concluded that fluorination is suboptimal; modulating the carrier’s hydrophobicity via electron-donating groups (instead of fluorination) is critical for stable Zr-MOF-based catalysts in [H]-assisted advanced oxidation, offering alternative perspectives for process optimization.</p> Graphical abstract <p></p>

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Nano Pd0 particle confined within the pores of UiO-66(Zr)-F4 for efficient destruction of carbamazepine by the hydrogen-accelerated catalytic Fenton reaction

  • Jiahao Wang,
  • Feng Liu,
  • Lei Xie,
  • Hailiang Yang,
  • Sanjian Ma,
  • Zixia Lin,
  • Xin Liu,
  • Suqin Wang

摘要

Refractory wastewater treatment via Fenton reactions is hindered by iron sludge. Herein, fluorinated UiO-66(Zr)-F4 was employed as a hydrogen-storage carrier to confine Pd⁰ catalytic centers, and an [H]-mediated (H2-precursored) Fenton-like system was constructed for carbamazepine degradation under ambient conditions. With 25 μM Fe2 + and 60 mL min⁻1 H2 flow, 53% carbamazepine removal was achieved in 1 h via ⋅OH/1O2 oxidation, and > 59% efficiency was retained over six 3-h cycles. However, [H]-driven hydrogen spillover reduced C-F bonds, causing a 92.3% drop in specific surface area that compromised long-term stability. It was concluded that fluorination is suboptimal; modulating the carrier’s hydrophobicity via electron-donating groups (instead of fluorination) is critical for stable Zr-MOF-based catalysts in [H]-assisted advanced oxidation, offering alternative perspectives for process optimization.

Graphical abstract