<p>The Fenton-like reaction has always been hampered by limitations related to its narrow pH range and poor stability. In this study, we successfully developed a novel catalyst composed of Prussian blue (PB) nanoparticles anchored onto carbon-defective g-C<sub>3</sub>N<sub>4</sub> (CD-C<sub>3</sub>N<sub>4</sub>) nanosheets with a porous structure. Under visible light irradiation for 120&#xa0;min, the removal efficiencies of tetracycline can achieve remarkably high removal rates as 93.3%. Significantly, this catalyst attains exceptional long-term stability enabling up to 20 cycles, while consistently maintaining a degradation efficiency exceeding 99%. Furthermore, this system exhibits a wide pH tolerance ranging from 3 to 9. Efficient charge separation and the introduction of carbon defects on the g-C<sub>3</sub>N<sub>4</sub> nanosheets contribute to the robust Fe<sup>3+</sup>/Fe<sup>2+</sup> cycles in PB, which support prolonged multiple recycles. ESR and quenching tests indicated that •O<sub>2</sub><sup>−</sup> species play a significant role in catalytic degradation, with •OH and h<sup>+</sup> also being involved in the photo-Fenton reaction. Finally, we proposed potential photo-Fenton degradation pathways for tetracycline(TC) and conducted a comprehensive investigation into the toxicity changes of TC degradation through full-scale zebrafish toxicology assays. This work presents an innovative approach to construct highly stable Fenton-like catalysts through structural defect engineering combined with Fe-Metal organic frameworks(MOFs) loading strategies.</p>

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Fe-MOF nanoparticles supported with carbon-defective g-C3N4 nanosheet as visible-light driven photo-Fenton catalyst for efficient degradation of tetracycline hydrochloride

  • Zhengzheng Shi,
  • Jia Li,
  • Yupeng Pan,
  • Xuewei Li,
  • Zile Zhuang,
  • Yihan Li,
  • Zheng Zhang,
  • Zirui Wang,
  • Qizhi Luo,
  • Xuncai Chen

摘要

The Fenton-like reaction has always been hampered by limitations related to its narrow pH range and poor stability. In this study, we successfully developed a novel catalyst composed of Prussian blue (PB) nanoparticles anchored onto carbon-defective g-C3N4 (CD-C3N4) nanosheets with a porous structure. Under visible light irradiation for 120 min, the removal efficiencies of tetracycline can achieve remarkably high removal rates as 93.3%. Significantly, this catalyst attains exceptional long-term stability enabling up to 20 cycles, while consistently maintaining a degradation efficiency exceeding 99%. Furthermore, this system exhibits a wide pH tolerance ranging from 3 to 9. Efficient charge separation and the introduction of carbon defects on the g-C3N4 nanosheets contribute to the robust Fe3+/Fe2+ cycles in PB, which support prolonged multiple recycles. ESR and quenching tests indicated that •O2 species play a significant role in catalytic degradation, with •OH and h+ also being involved in the photo-Fenton reaction. Finally, we proposed potential photo-Fenton degradation pathways for tetracycline(TC) and conducted a comprehensive investigation into the toxicity changes of TC degradation through full-scale zebrafish toxicology assays. This work presents an innovative approach to construct highly stable Fenton-like catalysts through structural defect engineering combined with Fe-Metal organic frameworks(MOFs) loading strategies.