<p>Nitro-functionalized NO<sub>2</sub>-MIL-53(Fe) was synthesized by modifying MIL-53(Fe) to enhance persulfate activation for the degradation of tetracycline (TCN). Comparative studies with NH<sub>2</sub>-MIL-53(Fe) and pristine MIL-53(Fe), it was found that NO<sub>2</sub>-MIL-53(Fe) is categorized as an ideal type I isotherm, without observable hysteresis loop. The introduction of nitro-group incorporation significantly increased specific surface area clocking in at 298.3&#xa0;m<sup>2</sup>/g and an average pore diameter of 3.3&#xa0;nm, created uniform micropores, and improved adsorption capacity. Structural characterization confirmed Fe(II) generation and electron transfer in NO<sub>2</sub>-MIL-53(Fe), enabling 82.1% TCN removal within 30&#xa0;min. Radical (SO<sub>4</sub><sup>·−</sup>, ·OH, O<sub>2</sub><sup>·⁻</sup>) and non-radical (<sup>1</sup>O<sub>2</sub>, charge transfer) pathways synergistically drove degradation, as evidenced by quenching experiments and EPR analysis. ESI-Q-TOF MS identified key intermediates, proposing plausible TCN degradation pathways. This study highlights the potential of nitro-functionalized metal-organic frameworks (MOFs) in advanced oxidation processes, emphasizing their enhanced catalytic activity and performance mechanisms, and provides new ideas for the remediation of pollutants in water bodies.</p> Graphical abstract <p></p>

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The Nitro-Modified NO2-MIL-53(Fe) Activating Persulfate for the Efficient Degradation of Tetracycline: Performance and Mechanism

  • Yizhuo Bai,
  • Shiyu Zhang,
  • Kaifan Zhang,
  • Jiali Li,
  • Jiehe Zhang,
  • Mingxu Hao,
  • Haisheng Tao

摘要

Nitro-functionalized NO2-MIL-53(Fe) was synthesized by modifying MIL-53(Fe) to enhance persulfate activation for the degradation of tetracycline (TCN). Comparative studies with NH2-MIL-53(Fe) and pristine MIL-53(Fe), it was found that NO2-MIL-53(Fe) is categorized as an ideal type I isotherm, without observable hysteresis loop. The introduction of nitro-group incorporation significantly increased specific surface area clocking in at 298.3 m2/g and an average pore diameter of 3.3 nm, created uniform micropores, and improved adsorption capacity. Structural characterization confirmed Fe(II) generation and electron transfer in NO2-MIL-53(Fe), enabling 82.1% TCN removal within 30 min. Radical (SO4·−, ·OH, O2·⁻) and non-radical (1O2, charge transfer) pathways synergistically drove degradation, as evidenced by quenching experiments and EPR analysis. ESI-Q-TOF MS identified key intermediates, proposing plausible TCN degradation pathways. This study highlights the potential of nitro-functionalized metal-organic frameworks (MOFs) in advanced oxidation processes, emphasizing their enhanced catalytic activity and performance mechanisms, and provides new ideas for the remediation of pollutants in water bodies.

Graphical abstract