Atmospheric CO₂-to-acetaldehyde artificial photosynthesis in metallo hydrogen-bonded organic frameworks.
basic_science · Level V
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- Record sourced from PubMed, PMID 42436109.
- Also identified by DOI 10.1038/s41467-026-75384-z.
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Abstract
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.