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<p>The photocatalytic oxygen reduction reaction (ORR) for hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production via the two-electron pathway offers an environmentally friendly oxidant and a clean fuel. However, the challenge exists in optimal oxygen (O<sub>2</sub>) adsorption capacities and maintaining O–O bond during O<sub>2</sub> activation. Herein, we present a zinc single-atom catalyst (Zn/V<sub>N</sub>-CN) incorporating nitrogen vacancies (V<sub>N</sub>), which is designed to modulate the electronic structure of the photocatalyst, leading to optimized O<sub>2</sub> adsorption energy and a remarkable enhancement in H<sub>2</sub>O<sub>2</sub> yield. Benefitting from the synergistic effect between nitrogen vacancies and Zn single atoms, the optimized Zn/V<sub>N</sub>-CN catalyst exhibits a photocatalytic H<sub>2</sub>O<sub>2</sub> production rate of 2.399 mmol g<sup>−1</sup> h<sup>−1</sup> under visible-light irradiation, representing a 12-fold enhancement compared to pristine g-C<sub>3</sub>N<sub>4</sub> (CN), along with a high H<sub>2</sub>O<sub>2</sub> selectivity of 87.4%. Combined experimental and theoretical studies indicate that the Zn-N<sub>3</sub> sites act as highly active reaction centers, while nitrogen vacancies increase the charge density and downshift the d-band center of the Zn sites, thereby moderating O<sub>2</sub> adsorption strength, lowering the activation energy barrier for the formation of *H<sub>2</sub>O<sub>2</sub>, and further converting it to H<sub>2</sub>O<sub>2</sub>. This work proposes an effective strategy for tuning O<sub>2</sub> adsorption behavior to achieve highly selective and active photocatalytic H<sub>2</sub>O<sub>2</sub> production.</p>

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N-vacancy engineering Zn single-atom site boosts efficient photosynthesis of hydrogen peroxide

  • 期刊论文

  • 发表日期：

    2026年3月25日

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  • Xiaoyan Zhong,
  • Donghai Wu,
  • Tianwen Liu,
  • Shiyu Li,
  • Yiwen Chen,
  • Ruiyu Liu,
  • Meihuan Liu,
  • Shixun Lian,
  • Hui Su

摘要

The photocatalytic oxygen reduction reaction (ORR) for hydrogen peroxide (H2O2) production via the two-electron pathway offers an environmentally friendly oxidant and a clean fuel. However, the challenge exists in optimal oxygen (O2) adsorption capacities and maintaining O–O bond during O2 activation. Herein, we present a zinc single-atom catalyst (Zn/VN-CN) incorporating nitrogen vacancies (VN), which is designed to modulate the electronic structure of the photocatalyst, leading to optimized O2 adsorption energy and a remarkable enhancement in H2O2 yield. Benefitting from the synergistic effect between nitrogen vacancies and Zn single atoms, the optimized Zn/VN-CN catalyst exhibits a photocatalytic H2O2 production rate of 2.399 mmol g−1 h−1 under visible-light irradiation, representing a 12-fold enhancement compared to pristine g-C3N4 (CN), along with a high H2O2 selectivity of 87.4%. Combined experimental and theoretical studies indicate that the Zn-N3 sites act as highly active reaction centers, while nitrogen vacancies increase the charge density and downshift the d-band center of the Zn sites, thereby moderating O2 adsorption strength, lowering the activation energy barrier for the formation of *H2O2, and further converting it to H2O2. This work proposes an effective strategy for tuning O2 adsorption behavior to achieve highly selective and active photocatalytic H2O2 production.