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<p>The transition from laboratory-scale to industrial hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production hinges on achieving ultra-high photocatalytic efficiency. Herein, we demonstrate a nitrogen-substitution engineering strategy for photocatalysts by repacing partial carbon atoms in benzene-1,3,5-triamine by nitrogen atoms, showing dual synergistic effects: (1) electronic structure modification upon electronegativity and dipole moment of the building blocks, creating built-in electric fields that promote charge separation and interfacial electron transfer; (2) enhancement in adsorption of reaction intermediate significantly boosting oxygen reduction reaction (ORR) and water oxidation reaction (WOR) kinetics. This dual-modification system exhibits broadband light absorption extending to 700 nm (near-infrared), enabling outstanding performance under ambient conditions with a H<sub>2</sub>O<sub>2</sub> production rate of 12099 µmol g<sup>−1</sup> h<sup>−1</sup> from water and O<sub>2</sub> without any Sacrificial agent, an apparent quantum efficiency (AQE) of 19% at 500 nm, and a solar-to-chemical energy (SCC) efficiency of 1.38%. This work establishes atom-engineered nitrogen substitution as a general approach for designing high-performance photocatalysts, offering a viable pathway for large-scale H<sub>2</sub>O<sub>2</sub> production with solar-driven chemical synthesis paradigm.</p>

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Nitrogen-substitution engineering enabling efficient H2O2 photosynthesis

  • 期刊论文

  • 发表日期：

    2026年5月18日

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  • Yuxuan Liu,
  • Yuanzhe Jia,
  • Lele Gong,
  • Feng Luo

摘要

The transition from laboratory-scale to industrial hydrogen peroxide (H2O2) production hinges on achieving ultra-high photocatalytic efficiency. Herein, we demonstrate a nitrogen-substitution engineering strategy for photocatalysts by repacing partial carbon atoms in benzene-1,3,5-triamine by nitrogen atoms, showing dual synergistic effects: (1) electronic structure modification upon electronegativity and dipole moment of the building blocks, creating built-in electric fields that promote charge separation and interfacial electron transfer; (2) enhancement in adsorption of reaction intermediate significantly boosting oxygen reduction reaction (ORR) and water oxidation reaction (WOR) kinetics. This dual-modification system exhibits broadband light absorption extending to 700 nm (near-infrared), enabling outstanding performance under ambient conditions with a H2O2 production rate of 12099 µmol g−1 h−1 from water and O2 without any Sacrificial agent, an apparent quantum efficiency (AQE) of 19% at 500 nm, and a solar-to-chemical energy (SCC) efficiency of 1.38%. This work establishes atom-engineered nitrogen substitution as a general approach for designing high-performance photocatalysts, offering a viable pathway for large-scale H2O2 production with solar-driven chemical synthesis paradigm.