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<p>Artificial photosynthesis of acetaldehyde from atmospheric CO<sub>2</sub> is highly promising, yet remains severely limited by low CO<sub>2</sub> concentration in air and sluggish proton transfer kinetics. Herein, we report metallo hydrogen-bonded organic frameworks (MHOFs) of HNNU-X (X = O, S, Se) which enable acetaldehyde synthesis directly from air, water, and natural sunlight. Among them, HNNU-Se exhibits a competitive acetaldehyde production rate of 557.1 μmol g⁻¹ h⁻¹ with high electron-based selectivity of 95% under outdoor conditions, without need of sacrificial agents. Mechanistic studies reveal that HNNU-X creates a proton-rich microenvironment in which [Zn(tpy)]<sup>2+</sup> cations function as CO<sub>2</sub> capture and activation sites for direct air capture, while [XCN]<sup>–</sup> anions serve as proton shuttles, facilitating rapid transfer of in-situ generated H⁺ from solar-driven water oxidation to adsorbed CO<sub>2</sub>. This work enables the synergistic coupling of CO<sub>2</sub> reduction and H<sub>2</sub>O oxidation, thereby achieving efficient artificial photosynthesis of acetaldehyde.</p>

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Atmospheric CO₂-to-acetaldehyde artificial photosynthesis in metallo hydrogen-bonded organic frameworks

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年7月12日

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  • Jun Pang,
  • Xinyu Bai,
  • Junjie Dai,
  • Sijie Liu,
  • Shuangfeng Yin,
  • Yong Pei,
  • Rong Tan

摘要

Artificial photosynthesis of acetaldehyde from atmospheric CO2 is highly promising, yet remains severely limited by low CO2 concentration in air and sluggish proton transfer kinetics. Herein, we report metallo hydrogen-bonded organic frameworks (MHOFs) of HNNU-X (X = O, S, Se) which enable acetaldehyde synthesis directly from air, water, and natural sunlight. Among them, HNNU-Se exhibits a competitive acetaldehyde production rate of 557.1 μmol g⁻¹ h⁻¹ with high electron-based selectivity of 95% under outdoor conditions, without need of sacrificial agents. Mechanistic studies reveal that HNNU-X creates a proton-rich microenvironment in which [Zn(tpy)]2+ cations function as CO2 capture and activation sites for direct air capture, while [XCN]– anions serve as proton shuttles, facilitating rapid transfer of in-situ generated H⁺ from solar-driven water oxidation to adsorbed CO2. This work enables the synergistic coupling of CO2 reduction and H2O oxidation, thereby achieving efficient artificial photosynthesis of acetaldehyde.