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<p>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is a common and important oxidizing agent, which is widely used in environmental protection fields. In this study, the COF framework catalysts with nickel-cobalt bimetallic sites, Co@phthalocyanine (PcNi) - tetrahydroxybenzene (THB), were synthesized through the hydrothermal method. These catalysts were applied as the particulate electrodes in the electrocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) generation system. Scanning electron microscope (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) were used to characterized the Co@PcNi-THB particle electrodes. Scanning electron microscope (SEM) images showed the Co@PcNi-THB particle electrodes featured the porous structure. The electrochemical active area of Co@PcNi-THB increased to (3.97 µF/cm<sup>2</sup>), which was 2.39 times higher than that of PcNi-THB catalyst (1.66 µF/cm<sup>2</sup>). The maximum H<sub>2</sub>O<sub>2</sub> yield of 3340 µmol/g was obtained with the addition of Co@PcNi-THB catalyst content of 10&#xa0;mg, current density of 15&#xa0;mA/cm<sup>2</sup>, pH 11.03, continuous stirring for 1&#xa0;h at 200 r/min using a magnetic stirrer, and 0.1&#xa0;M Na<sub>2</sub>SO<sub>4</sub> electrolyte, with an energy consumption (EEC) of 3.201 kWh/kg. The acidic atmosphere, Cl<sup>−</sup> and NO<sub>3</sub><sup>−</sup> ions have the inhibitory effect on the H<sub>2</sub>O<sub>2</sub> yields. After five cycles of Co@PcNi-THB, the H<sub>2</sub>O<sub>2</sub> production decreased to 3153 µmol/g, and the retention ratio of Co in Co@PcNi-THB reduced to 94%. Under the same reaction conditions, the Faraday efficiency (FE) obtained using the gas diffusion electrode (GDE) for the Co@PcNi-THB method was 76.4%, and the hydrogen peroxide yield was 3885 µmol/g. The synergistic Co-Ni effect generated by the introduction of the metal Co enhanced the two-electron Oxygen Reduction Reaction (2e<sup>−</sup>ORR) process. This study provides new insights for designing particle electrodes with bimetallic atomic synergistic effects.</p> Graphical Abstract <p></p>

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Electrocatalytic Production of H2O2 Using COF Particle Electrodes with Co-Ni Bimetallic Sites

  • 期刊论文

  • 发表日期：

    2026年2月21日

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  • Tongxi Xu,
  • Yuzhan Luo,
  • Zihao Wang,
  • Chenglong Wang,
  • Hao Huo,
  • Yaobin Huang,
  • Weijin Zheng,
  • Guangli Liu,
  • Jiasheng Fang,
  • Yanliang Li,
  • Yongfu Qiu,
  • Guofen Sun,
  • Qiongfang Zhuo

摘要

Hydrogen peroxide (H2O2) is a common and important oxidizing agent, which is widely used in environmental protection fields. In this study, the COF framework catalysts with nickel-cobalt bimetallic sites, Co@phthalocyanine (PcNi) - tetrahydroxybenzene (THB), were synthesized through the hydrothermal method. These catalysts were applied as the particulate electrodes in the electrocatalytic hydrogen peroxide (H2O2) generation system. Scanning electron microscope (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) were used to characterized the Co@PcNi-THB particle electrodes. Scanning electron microscope (SEM) images showed the Co@PcNi-THB particle electrodes featured the porous structure. The electrochemical active area of Co@PcNi-THB increased to (3.97 µF/cm2), which was 2.39 times higher than that of PcNi-THB catalyst (1.66 µF/cm2). The maximum H2O2 yield of 3340 µmol/g was obtained with the addition of Co@PcNi-THB catalyst content of 10 mg, current density of 15 mA/cm2, pH 11.03, continuous stirring for 1 h at 200 r/min using a magnetic stirrer, and 0.1 M Na2SO4 electrolyte, with an energy consumption (EEC) of 3.201 kWh/kg. The acidic atmosphere, Cl− and NO3− ions have the inhibitory effect on the H2O2 yields. After five cycles of Co@PcNi-THB, the H2O2 production decreased to 3153 µmol/g, and the retention ratio of Co in Co@PcNi-THB reduced to 94%. Under the same reaction conditions, the Faraday efficiency (FE) obtained using the gas diffusion electrode (GDE) for the Co@PcNi-THB method was 76.4%, and the hydrogen peroxide yield was 3885 µmol/g. The synergistic Co-Ni effect generated by the introduction of the metal Co enhanced the two-electron Oxygen Reduction Reaction (2e−ORR) process. This study provides new insights for designing particle electrodes with bimetallic atomic synergistic effects.

Graphical Abstract