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<p>Non-noble-based single atomic catalysts have exhibited significant potential in electrochemical production of H<sub>2</sub>O<sub>2</sub> via two-electron oxygen reduction reactions (2e<sup>−</sup> ORR). However, constructing highly efficient and acid-resistant catalysts remains a challenge but significant. In this work, fullerene (C<sub>60</sub>) with abundant pentagonal inherent defects was employed as a carbon substrate to synthesize defect-rich nanocarbon electrocatalysts doped with NSCo single atoms and accompanied by metallic Co nanoparticles (CoSA/CoNP-NSDNC) for the first time. The electrochemical experiments demonstrate that the active sites of CoSA/CoNP-NSDNC are formed through the synergistic interaction between NSCo single atoms and Co nanoparticle clusters embedded within the carbon framework. The obtained CoSA/CoNP-NSDNC catalyst exhibits an onset potential as 0.72&#xa0;V versus RHE and achieves up to 90% H<sub>2</sub>O<sub>2</sub> selectivity over a wide potential range of 500&#xa0;mV. Moreover, the as-obtained CoSA/CoNP-NSDNC configured as the cathode in a self-assembled flow cell under acidic conditions achieves a high H<sub>2</sub>O<sub>2</sub> production rate of 4206.96&#xa0;mmol g<sub>cat</sub>⁻<sup>1</sup>&#xa0;h⁻<sup>1</sup> with a Faraday efficiency of ∼ 95% and exhibit ultra fast degradation of organic pollutants. This work focuses on the synergistic effect of non-noble metal nanoparticles, metal single-atom sites, and topological defects on the 2e<sup>−</sup> ORR process, which provides a new direction for designing carbon-based catalysts for efficient H<sub>2</sub>O<sub>2</sub> electrosynthesis.</p>

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Synergistic Single-Atom and Clustered Cobalt Sites on N/S Co-Doped Defect Nano-Carbon for Efficient H2O2 Electrosynthesis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年2月12日

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  • Yuzhong Huang,
  • Chang Zhang,
  • Xingyu Wang,
  • Yuji Wu,
  • Jun Lv,
  • Jian Zhang,
  • Wangqiang Shen,
  • Xing Lu

摘要

Non-noble-based single atomic catalysts have exhibited significant potential in electrochemical production of H2O2 via two-electron oxygen reduction reactions (2e− ORR). However, constructing highly efficient and acid-resistant catalysts remains a challenge but significant. In this work, fullerene (C60) with abundant pentagonal inherent defects was employed as a carbon substrate to synthesize defect-rich nanocarbon electrocatalysts doped with NSCo single atoms and accompanied by metallic Co nanoparticles (CoSA/CoNP-NSDNC) for the first time. The electrochemical experiments demonstrate that the active sites of CoSA/CoNP-NSDNC are formed through the synergistic interaction between NSCo single atoms and Co nanoparticle clusters embedded within the carbon framework. The obtained CoSA/CoNP-NSDNC catalyst exhibits an onset potential as 0.72 V versus RHE and achieves up to 90% H2O2 selectivity over a wide potential range of 500 mV. Moreover, the as-obtained CoSA/CoNP-NSDNC configured as the cathode in a self-assembled flow cell under acidic conditions achieves a high H2O2 production rate of 4206.96 mmol gcat⁻1 h⁻1 with a Faraday efficiency of ∼ 95% and exhibit ultra fast degradation of organic pollutants. This work focuses on the synergistic effect of non-noble metal nanoparticles, metal single-atom sites, and topological defects on the 2e− ORR process, which provides a new direction for designing carbon-based catalysts for efficient H2O2 electrosynthesis.