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<p>Single-atom catalysts (SACs) are state-of-the-art for peroxymonosulfate-based advanced oxidation processes (PMS-AOPs) in environmental mediation. Accordingly, designing SACs that efficiently activate PMS and generate reactive oxygen species is crucial for enhancing the oxidative removal of contaminants. Herein, we develop a structured SAC comprising cobalt single-atom sites with an asymmetric Co-N<sub>3</sub>O<sub>1</sub> coordination onto a polyurethane foam (PUF)-nitrogen-doped graphene (NG) matrix. Owing to its superior activity and mass-diffusion kinetics, the resultant Co<sub>1</sub>/PUF-NG structured SAC can be facilely engineered as a fixed-bed reactor for the continuous-flow catalysis. The corresponding fixed-bed reactor effectively promotes continuous-flow degradation of antibiotics and organic dyes via a catalytic Fenton reaction. It also exhibits remarkable durability with over 90% tetracycline degradation efficiency after 15 days of continuous operation. Detailed mechanistic investigations reveal a relatively low adsorption energy of PMS over the asymmetric Co-N<sub>3</sub>O<sub>1</sub> sites, favoring the production of singlet oxygen (<sup>1</sup>O<sub>2</sub>) and sulfate radicals (SO<sub>4</sub>·<sup>−</sup>). This work provides an effective strategy for constructing structured SAC-based reactorsthat combine high activity, stability, and scalability for continuous-flow treatment of antibiotic wastewater.</p>

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A structured single-atom catalyst with asymmetric Co-N3O1 sites for continuous-flow Fenton-like reactions

  • 期刊论文

  • 发表日期：

    2026年7月29日

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  • Guangyuan Feng,
  • Zhengxin Long,
  • Fangrun Jin,
  • Yin Li,
  • Wenxuan Xue,
  • Jiangbo Xi,
  • Zhongxin Chen

摘要

Single-atom catalysts (SACs) are state-of-the-art for peroxymonosulfate-based advanced oxidation processes (PMS-AOPs) in environmental mediation. Accordingly, designing SACs that efficiently activate PMS and generate reactive oxygen species is crucial for enhancing the oxidative removal of contaminants. Herein, we develop a structured SAC comprising cobalt single-atom sites with an asymmetric Co-N3O1 coordination onto a polyurethane foam (PUF)-nitrogen-doped graphene (NG) matrix. Owing to its superior activity and mass-diffusion kinetics, the resultant Co1/PUF-NG structured SAC can be facilely engineered as a fixed-bed reactor for the continuous-flow catalysis. The corresponding fixed-bed reactor effectively promotes continuous-flow degradation of antibiotics and organic dyes via a catalytic Fenton reaction. It also exhibits remarkable durability with over 90% tetracycline degradation efficiency after 15 days of continuous operation. Detailed mechanistic investigations reveal a relatively low adsorption energy of PMS over the asymmetric Co-N3O1 sites, favoring the production of singlet oxygen (1O2) and sulfate radicals (SO4·−). This work provides an effective strategy for constructing structured SAC-based reactorsthat combine high activity, stability, and scalability for continuous-flow treatment of antibiotic wastewater.