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Abstract <p>Designing highly effective cathodic catalysts that can efficiently generate H<sub>2</sub>O<sub>2</sub> in situ and promptly convert it to hydroxyl radicals (·OH) poses a significant challenge within the heterogeneous electro-Fenton (EF) systems. Herein, we fabricate a bifunctional core–shell catalyst featuring Co<sup>0</sup> species encapsulated within N, P-codoped carbon shells through a hydrothermal-pyrolysis strategy, utilizing bamboo shoots as biomass-derived precursors. Density functional theory (DFT) calculations elucidate that the protonation of pyridinic nitrogen modifies the adsorption energy of the OOH* intermediate, positioning it optimally at the peak (3.81&#xa0;eV) on the two-electron oxygen reduction reaction (2e<sup>−</sup> ORR) volcano plot, thereby significantly boosting H<sub>2</sub>O<sub>2</sub> production. Moreover, the Co<sup>0</sup> species embedded within the catalyst function as electron donors, catalyzing the activation of H<sub>2</sub>O<sub>2</sub> to produce ·OH by efficiently facilitating the transfer of electrons to Fe<sup>3+</sup>. Consequently, the synthesized catalyst exhibits a minimum electron transfer number of 2.06 and a maximum H<sub>2</sub>O<sub>2</sub> selectivity of 97.4%. Moreover, the degradation for the methylene blue solution exceeds 95% within 15&#xa0;min, with only an 11.3% reduction in degradation efficiency after 180&#xa0;min of continuous operation (9 cycles). This bifunctional catalyst design provides valuable insights that can accelerate the development of EF-based degradation systems.</p> Graphical Abstract <p></p>

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Accelerated generation and activation of H2O2 by the synergetic effect of pyridine-N protonation and Co0 species toward efficient electro-Fenton

  • 期刊论文

  • 发表日期：

    2025年7月14日

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  • Miao Tian,
  • Shi-Long Li,
  • Ye Chen,
  • Cong-Xin Xia,
  • Ya-Xin Guo,
  • Jia-Yao Qiu,
  • Xu-Po Liu,
  • Xin Chen,
  • Yang Lu,
  • Shi-Xue Dou

摘要

Abstract

Designing highly effective cathodic catalysts that can efficiently generate H2O2 in situ and promptly convert it to hydroxyl radicals (·OH) poses a significant challenge within the heterogeneous electro-Fenton (EF) systems. Herein, we fabricate a bifunctional core–shell catalyst featuring Co0 species encapsulated within N, P-codoped carbon shells through a hydrothermal-pyrolysis strategy, utilizing bamboo shoots as biomass-derived precursors. Density functional theory (DFT) calculations elucidate that the protonation of pyridinic nitrogen modifies the adsorption energy of the OOH* intermediate, positioning it optimally at the peak (3.81 eV) on the two-electron oxygen reduction reaction (2e− ORR) volcano plot, thereby significantly boosting H2O2 production. Moreover, the Co0 species embedded within the catalyst function as electron donors, catalyzing the activation of H2O2 to produce ·OH by efficiently facilitating the transfer of electrons to Fe3+. Consequently, the synthesized catalyst exhibits a minimum electron transfer number of 2.06 and a maximum H2O2 selectivity of 97.4%. Moreover, the degradation for the methylene blue solution exceeds 95% within 15 min, with only an 11.3% reduction in degradation efficiency after 180 min of continuous operation (9 cycles). This bifunctional catalyst design provides valuable insights that can accelerate the development of EF-based degradation systems.

Graphical Abstract