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<p>Neutral H<sub>2</sub>O<sub>2</sub> electrosynthesis via two-electron oxygen reduction reaction (2e<sup>−</sup>-ORR) is a promising alternative to replace traditional anthraquinone processes. However, it still remains significantly challenging to develop efficient electrocatalysts due to sluggish neutral 2e<sup>−</sup>-ORR kinetics. Herein, we reported abundant ultrafine Co/Co<sub>2</sub>O<sub>3</sub> nanoparticles (NPs) anchored oxidic nitrogen-doped carbon nanotubes (Co/Co<sub>2</sub>O<sub>3</sub>@OCNT) derived from the pyrolysis of the mixed OCNT and Co@Tpy, presenting synergistical enhancement effect on the water dissociation to supply active hydrogen coupling with O<sub>2</sub> to produce H<sub>2</sub>O<sub>2</sub> at positive onset potential of 0.66&#xa0;V vs. RHE. As a result, Co/Co<sub>2</sub>O<sub>3</sub>@OCNT achieves a record current density of 4.0&#xa0;mA&#xa0;cm<sup>−2</sup> at 0.2&#xa0;V vs. RHE and nearly 100% H<sub>2</sub>O<sub>2</sub> selectivity at the potential from 0 to 0.5&#xa0;V vs. RHE. In situ observations demonstrated that ultrafine Co/Co<sub>2</sub>O<sub>3</sub> NPs and nitrogen-doped carbon supports would synergistically improve the active hydrogen feeding further to facilitate the formation of key intermediate *OOH. Furthermore, based on the sandwiched configuration of the flow cell, Co/Co<sub>2</sub>O<sub>3</sub>@OCNT shows a superior performance with the yield rate of salt-free aqueous H<sub>2</sub>O<sub>2</sub> solution around 63.4&#xa0;mol&#xa0;g<sub>cat</sub><sup>−1</sup>&#xa0;h<sup>−1</sup> at 200&#xa0;mA&#xa0;cm<sup>−2</sup> and the corresponding Faradaic efficiency of 85%. Moreover, integration of Co/Co<sub>2</sub>O<sub>3</sub>@OCNT into this cell achieves high real-time production concentration of H<sub>2</sub>O<sub>2</sub> around 20&#xa0;mM at 200&#xa0;mA&#xa0;cm<sup>−2</sup> by varying the pure water flow rate to 1&#xa0;mL&#xa0;min<sup>−1</sup>, suggesting the huge potential of salt-free H<sub>2</sub>O<sub>2</sub> solution production. This work provides a novel strategy for developing efficient neutral electrocatalysts and feasible process of neutral H<sub>2</sub>O<sub>2</sub> production.</p> Graphical Abstract <p></p>

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Boosting hydrogen spillover over carbon nanotube anchored ultrafine Co/Co2O3 nanoparticles for efficient neutral H2O2 electrosynthesis

  • 期刊论文

  • 发表日期：

    2025年8月22日

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  • Zhuoqi Zhou,
  • Yu Han,
  • Manman Zou,
  • Ronglan Pan,
  • Xin Ge,
  • Chuanxun Du,
  • Jili Yuan,
  • Tao Wang,
  • Hao Zhang,
  • Hu Li,
  • Jian Zhang

摘要

Neutral H2O2 electrosynthesis via two-electron oxygen reduction reaction (2e−-ORR) is a promising alternative to replace traditional anthraquinone processes. However, it still remains significantly challenging to develop efficient electrocatalysts due to sluggish neutral 2e−-ORR kinetics. Herein, we reported abundant ultrafine Co/Co2O3 nanoparticles (NPs) anchored oxidic nitrogen-doped carbon nanotubes (Co/Co2O3@OCNT) derived from the pyrolysis of the mixed OCNT and Co@Tpy, presenting synergistical enhancement effect on the water dissociation to supply active hydrogen coupling with O2 to produce H2O2 at positive onset potential of 0.66 V vs. RHE. As a result, Co/Co2O3@OCNT achieves a record current density of 4.0 mA cm−2 at 0.2 V vs. RHE and nearly 100% H2O2 selectivity at the potential from 0 to 0.5 V vs. RHE. In situ observations demonstrated that ultrafine Co/Co2O3 NPs and nitrogen-doped carbon supports would synergistically improve the active hydrogen feeding further to facilitate the formation of key intermediate *OOH. Furthermore, based on the sandwiched configuration of the flow cell, Co/Co2O3@OCNT shows a superior performance with the yield rate of salt-free aqueous H2O2 solution around 63.4 mol gcat−1 h−1 at 200 mA cm−2 and the corresponding Faradaic efficiency of 85%. Moreover, integration of Co/Co2O3@OCNT into this cell achieves high real-time production concentration of H2O2 around 20 mM at 200 mA cm−2 by varying the pure water flow rate to 1 mL min−1, suggesting the huge potential of salt-free H2O2 solution production. This work provides a novel strategy for developing efficient neutral electrocatalysts and feasible process of neutral H2O2 production.

Graphical Abstract