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<p>Atomically dispersed metal catalysts (ADMCs) with dual reaction sites have been extensively utilized in permonosulfate (PMS)-based Fenton-like systems for the degradation of antibiotic wastewater, yet challenges remain in synthesizing cost-effective and highly active Cu-based catalysts. Herein, atomically dispersed Cu catalysts supported on N-doped cellulose-derived carbon (Cu<sub>1</sub>/NC-700) are synthesized via a sol-gel combined with high-temperature pyrolysis method. The formed Cu–N<sub><i>x</i></sub> and pyrrolic N dual reaction sites enhance the activation of PMS and adsorption of oxytetracycline (OTC), thereby shortening the migration distance of radicals towards the OTC. Moreover, graphitic N accelerates electron transfer to facilitate the Cu<sup>2+</sup>/Cu<sup>+</sup> cycle for the generation of highly efficient active species, including •OH, <sup>1</sup>O<sub>2</sub>, SO<sub>4</sub><sup>•−</sup>, and O<sub>2</sub><sup>•−</sup>. The Cu<sub>1</sub>/NC-700 exhibits significant catalytic activity for the degradation of OTC, achieving 96.6% degradation efficiency within 60 min at an initial substrate concentration of 50 mg/L, a high turnover frequency (0.279/min) and apparent rate constant (0.0827/min), which markedly surpassed those of Cu<sub>1</sub>/NC-600, Cu<sub>1</sub>/NC-800, and Cu<sub>NPs</sub>/NC. The results of chemical quenching experiments, electron paramagnetic resonance, and electrochemical analysis show that <sup>1</sup>O<sub>2</sub>-dominated non-radical pathway is the main mechanism rather than the radical pathway in the Cu<sub>1</sub>/NC-700+PMS+OTC system. This work presents a straightforward and cost-effective strategy for the synthesis of ADMCs for the treatment of tetracyclines wastewater.</p>

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Atomically dispersed copper catalysts with dual reaction sites and high mass transfer efficiency for highly-efficient Fenton-like degradation

  • 期刊论文

  • 发表日期：

    2026年1月5日

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  • Haiyang Xie,
  • Yiming Liu,
  • Yuhan Chen,
  • Yaolong Chen,
  • Yanjuan Zhang,
  • Zuqiang Huang,
  • Huayu Hu,
  • Tao Gan

摘要

Atomically dispersed metal catalysts (ADMCs) with dual reaction sites have been extensively utilized in permonosulfate (PMS)-based Fenton-like systems for the degradation of antibiotic wastewater, yet challenges remain in synthesizing cost-effective and highly active Cu-based catalysts. Herein, atomically dispersed Cu catalysts supported on N-doped cellulose-derived carbon (Cu1/NC-700) are synthesized via a sol-gel combined with high-temperature pyrolysis method. The formed Cu–Nx and pyrrolic N dual reaction sites enhance the activation of PMS and adsorption of oxytetracycline (OTC), thereby shortening the migration distance of radicals towards the OTC. Moreover, graphitic N accelerates electron transfer to facilitate the Cu2+/Cu+ cycle for the generation of highly efficient active species, including •OH, 1O2, SO4•−, and O2•−. The Cu1/NC-700 exhibits significant catalytic activity for the degradation of OTC, achieving 96.6% degradation efficiency within 60 min at an initial substrate concentration of 50 mg/L, a high turnover frequency (0.279/min) and apparent rate constant (0.0827/min), which markedly surpassed those of Cu1/NC-600, Cu1/NC-800, and CuNPs/NC. The results of chemical quenching experiments, electron paramagnetic resonance, and electrochemical analysis show that 1O2-dominated non-radical pathway is the main mechanism rather than the radical pathway in the Cu1/NC-700+PMS+OTC system. This work presents a straightforward and cost-effective strategy for the synthesis of ADMCs for the treatment of tetracyclines wastewater.