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<p>Currently, the efficient production of photocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) via covalent organic frameworks (COFs) primarily focuses on the efficiency and selectivity of oxygen reduction reaction (ORR), often neglecting the significance of water oxidation reaction (WOR) step. In this work, we introduce the concept of N-site engineering and construct four COFs that share similar chemical structures but differ in their N-sites: COF-TpBpa (containing benzidine unit), COF-TpApy (containing 2-bipyridine unit), COF-TpBpy (containing 2,2′-bipyridine unit), and COF-TpEABD (containing 3,3′-bipyridine unit) to explore the position of N sites for the influence on WOR. Theoretical calculations and experimental results indicate that COF-TpBpy containing 2,2′-bipyridine unit exhibits a stronger water adsorption capacity and enhanced charge transfer capability, thereby improving the WOR process. This enhanced WOR capacity is more favorable for the protonation of N atoms within the 2,2′-bipyridine unit, playing a crucial role in promoting the one-step 2e<sup>−</sup> ORR to produce H<sub>2</sub>O<sub>2</sub>. Thus, COF-TpBpy achieved a more excellent production rate of 2558 µM h<sup>−1</sup>, a high solar-to-chemical conversion (SCC) value of 0.043 % under natural sunlight conditions. This work provides valuable insights into the subtle structural changes of COFs for optimizing H<sub>2</sub>O<sub>2</sub> production.</p>

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N-site engineering: a key to boosting water oxidation for photocatalytic production of hydrogen peroxide

  • 期刊论文

  • 发表日期：

    2026年2月2日

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  • Fang Ma,
  • Niu Huang,
  • Binbin Jia,
  • Yongye Wang,
  • Mingzhu Wu,
  • Pan Wang,
  • Yihan Deng,
  • Ziyi Jiang,
  • Chunqiu Han,
  • Fang Chen,
  • Yingping Huang,
  • Hongwei Huang,
  • Liqun Ye

摘要

Currently, the efficient production of photocatalytic hydrogen peroxide (H2O2) via covalent organic frameworks (COFs) primarily focuses on the efficiency and selectivity of oxygen reduction reaction (ORR), often neglecting the significance of water oxidation reaction (WOR) step. In this work, we introduce the concept of N-site engineering and construct four COFs that share similar chemical structures but differ in their N-sites: COF-TpBpa (containing benzidine unit), COF-TpApy (containing 2-bipyridine unit), COF-TpBpy (containing 2,2′-bipyridine unit), and COF-TpEABD (containing 3,3′-bipyridine unit) to explore the position of N sites for the influence on WOR. Theoretical calculations and experimental results indicate that COF-TpBpy containing 2,2′-bipyridine unit exhibits a stronger water adsorption capacity and enhanced charge transfer capability, thereby improving the WOR process. This enhanced WOR capacity is more favorable for the protonation of N atoms within the 2,2′-bipyridine unit, playing a crucial role in promoting the one-step 2e− ORR to produce H2O2. Thus, COF-TpBpy achieved a more excellent production rate of 2558 µM h−1, a high solar-to-chemical conversion (SCC) value of 0.043 % under natural sunlight conditions. This work provides valuable insights into the subtle structural changes of COFs for optimizing H2O2 production.