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<p>Single-atom catalyst (SAC)-based Fenton-like systems offer sustainable solutions for water purification, but challenges remain in large-scale SAC production and precise structure engineering. Here we present a facile strategy for laboratory-scale mass production of Co-SACs with multidimensional coordination engineering, where atomically dispersed Co–N<sub>4</sub> sites are spontaneously modulated by axial Cl and second-shell S (Co<sub>1</sub>CNCl/S). The configuration downshifts the <i>d</i>-band centre of active Co sites, enhances charge-transfer capacity and significantly strengthens the Co–O bond with peroxymonosulfate, forming a surface electrophilic intermediate with mild oxidation potential. Consequently, Co<sub>1</sub>CNCl/S steers peroxymonosulfate activation via a non-radical electron-transfer pathway, achieving selective phenol degradation within 5 min with a turnover frequency of 1.82 min<sup>−1</sup>, outperforming state-of-the-art catalysts. In a continuous flow, the Co<sub>1</sub>CNCl/S-packed column achieves effective organic wastewater treatment at just $US0.22 per tonne. This work demonstrates a scalable approach for developing cost-effective SACs for environmental remediation.</p>

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Multidimensional engineering of single-atom cobalt catalysts for ultrafast Fenton-like reactions

  • 期刊论文

  • 发表日期：

    2025年1月22日

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  • Zhong-Shuai Zhu,
  • Yantao Wang,
  • Pengtang Wang,
  • Shuang Zhong,
  • Kunsheng Hu,
  • Shiying Ren,
  • Jitraporn Pimm Vongsvivut,
  • Hongqi Sun,
  • Xiaoguang Duan,
  • Shaobin Wang

摘要

Single-atom catalyst (SAC)-based Fenton-like systems offer sustainable solutions for water purification, but challenges remain in large-scale SAC production and precise structure engineering. Here we present a facile strategy for laboratory-scale mass production of Co-SACs with multidimensional coordination engineering, where atomically dispersed Co–N4 sites are spontaneously modulated by axial Cl and second-shell S (Co1CNCl/S). The configuration downshifts the d-band centre of active Co sites, enhances charge-transfer capacity and significantly strengthens the Co–O bond with peroxymonosulfate, forming a surface electrophilic intermediate with mild oxidation potential. Consequently, Co1CNCl/S steers peroxymonosulfate activation via a non-radical electron-transfer pathway, achieving selective phenol degradation within 5 min with a turnover frequency of 1.82 min−1, outperforming state-of-the-art catalysts. In a continuous flow, the Co1CNCl/S-packed column achieves effective organic wastewater treatment at just $US0.22 per tonne. This work demonstrates a scalable approach for developing cost-effective SACs for environmental remediation.