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<p>H<sub>2</sub>O<sub>2</sub> photosynthesis through oxygen reduction reaction (ORR) and water oxidation reaction (WOR) from water and air represents an attractive alternative in the H<sub>2</sub>O<sub>2</sub> production. However, the inherent imbalance resulting from the fast O<sub>2</sub> reduction process in ORR and the sluggish H<sub>2</sub>O oxidation process in WOR often leads to inferior photocatalytic efficiency. To this end, we report here the synthesis of aliphatic acylhydrazone covalent organic frameworks (AA-COFs) by coupling aliphatic hydrazide and benzotrithiophene motifs using acylhydrazone linkage. Notably, rich S, O, and N heteroatoms located on the pore wall of AA-COFs are found to give a high affinity towards both O<sub>2</sub> and H<sub>2</sub>O, thus improving the kinetics of both oxygen reduction and water oxidation. As a result, the optimized aliphatic acylhydrazone material through single-carbon atomic engineering achieves a trade-off in the kinetics of ORR and WOR, thus enabling an efficient overall H<sub>2</sub>O<sub>2</sub> photosynthesis from water and air in the absence of any sacrificial agent with a H<sub>2</sub>O<sub>2</sub> production rate of as high as 4777 µmol g<sup>−1</sup> h<sup>−1</sup> and 99.3% O<sub>2</sub> utilization and conversion efficiency.</p>

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Optimizing oxygen and water affinity in aliphatic acylhydrazone covalent organic frameworks for efficient H2O2 photosynthesis from water and air

  • 期刊论文

  • 发表日期：

    2026年1月15日

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  • Yuanzhe Jia,
  • Yuxuan Liu,
  • Lele Gong,
  • Yuting Yang,
  • Zhiwu Yu,
  • Zhanggao Le,
  • Feng Luo

摘要

H2O2 photosynthesis through oxygen reduction reaction (ORR) and water oxidation reaction (WOR) from water and air represents an attractive alternative in the H2O2 production. However, the inherent imbalance resulting from the fast O2 reduction process in ORR and the sluggish H2O oxidation process in WOR often leads to inferior photocatalytic efficiency. To this end, we report here the synthesis of aliphatic acylhydrazone covalent organic frameworks (AA-COFs) by coupling aliphatic hydrazide and benzotrithiophene motifs using acylhydrazone linkage. Notably, rich S, O, and N heteroatoms located on the pore wall of AA-COFs are found to give a high affinity towards both O2 and H2O, thus improving the kinetics of both oxygen reduction and water oxidation. As a result, the optimized aliphatic acylhydrazone material through single-carbon atomic engineering achieves a trade-off in the kinetics of ORR and WOR, thus enabling an efficient overall H2O2 photosynthesis from water and air in the absence of any sacrificial agent with a H2O2 production rate of as high as 4777 µmol g−1 h−1 and 99.3% O2 utilization and conversion efficiency.