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<p>The sulfate radical-based advanced oxidation process (SR-AOP) has gained prominence in antibiotic wastewater treatment owing to its operational efficiency, cost-effectiveness, and environmental safety. In this study, we developed a novel composite material comprising Sulfidized Nanoscale Zero-valent Iron supported on Activated Carbon (S-nZVI/AC) for Persulfate (PS) activation to degrade Ciprofloxacin (CIP). Comprehensive characterization confirmed the successful synthesis of composites with uniform S-nZVI dispersion on the AC substrate. Optimization experiments revealed maximum degradation performance at a S/Fe molar ratio of 0.07 and an AC/S-nZVI mass ratio of 0.5:1. Under optimal conditions (0.6&#xa0;g/L S-nZVI/AC, 2&#xa0;mM PS, 10&#xa0;mg/L CIP), the system achieved&#xa0;96% Degradation Efficiency (DE) within 90&#xa0;min. The system demonstrated robust pH adaptability, maintaining high DE across a broad pH range (3–9). Coexisting anions exhibited differential inhibitory effects: CO<sub>3</sub><sup>2−</sup> and NO<sub>3</sub><sup>−</sup> significantly suppressed CIP degradation in a concentration-dependent manner, while SO<sub>4</sub><sup>2−</sup> and Cl<sup>−</sup> showed negligible impacts. Through radical quenching experiments and Electron Paramagnetic Resonance (EPR) analysis, we identified four reactive species, ranked by contribution to CIP degradation as follows: SO<sub>4</sub>•⁻ &lt; •OH &lt; <sup>1</sup>O<sub>2</sub> &lt; •O<sub>2</sub>⁻. Ultra-performance Liquid Chromatography-mass Spectrometry (UPLC-MS) analysis revealed sequential oxidation and ring-opening of the quinolone and piperazine moieties of CIP, generating 12 identifiable intermediates before complete mineralization. This study presents a novel PS activation strategy and demonstrates the potential of highly catalytically active nanomaterials for efficient antibiotic degradation in aqueous environments.</p> Graphical Abstract <p></p>

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Enhance Degradation of Ciprofloxacin in Aqueous Solutions Using Persulfate Activated by Sulfidized Nanoscale Zero-Valent Iron Supported on Activated Carbon

  • 期刊论文

  • 发表日期：

    2025年6月7日

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  • Yiqun Xu,
  • Weilong Lin,
  • Huixin Xiong,
  • Jie Dai,
  • Yunlong Zhu,
  • Leixin Huang,
  • Congyi Wen,
  • Shishuo Wang,
  • Yang Gao,
  • Wenjing Xue

摘要

The sulfate radical-based advanced oxidation process (SR-AOP) has gained prominence in antibiotic wastewater treatment owing to its operational efficiency, cost-effectiveness, and environmental safety. In this study, we developed a novel composite material comprising Sulfidized Nanoscale Zero-valent Iron supported on Activated Carbon (S-nZVI/AC) for Persulfate (PS) activation to degrade Ciprofloxacin (CIP). Comprehensive characterization confirmed the successful synthesis of composites with uniform S-nZVI dispersion on the AC substrate. Optimization experiments revealed maximum degradation performance at a S/Fe molar ratio of 0.07 and an AC/S-nZVI mass ratio of 0.5:1. Under optimal conditions (0.6 g/L S-nZVI/AC, 2 mM PS, 10 mg/L CIP), the system achieved 96% Degradation Efficiency (DE) within 90 min. The system demonstrated robust pH adaptability, maintaining high DE across a broad pH range (3–9). Coexisting anions exhibited differential inhibitory effects: CO32− and NO3− significantly suppressed CIP degradation in a concentration-dependent manner, while SO42− and Cl− showed negligible impacts. Through radical quenching experiments and Electron Paramagnetic Resonance (EPR) analysis, we identified four reactive species, ranked by contribution to CIP degradation as follows: SO4•⁻ < •OH < 1O2 < •O2⁻. Ultra-performance Liquid Chromatography-mass Spectrometry (UPLC-MS) analysis revealed sequential oxidation and ring-opening of the quinolone and piperazine moieties of CIP, generating 12 identifiable intermediates before complete mineralization. This study presents a novel PS activation strategy and demonstrates the potential of highly catalytically active nanomaterials for efficient antibiotic degradation in aqueous environments.

Graphical Abstract