Molecular catalyst coordinatively bonded to organic semiconductors for selective light-driven CO2 reduction in water
The selective photoreduction of CO 2 in aqueous media based on earth-abundant elements only, is today a challenging topic. Here we present the anchoring of discrete molecular catalysts on organic polymeric semiconductors via covalent bonding, generating molecular hybrid materials with well-defined a...
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Veröffentlicht in: | Nature communications 2024-11, Vol.15 (1), p.9779-14, Article 9779 |
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Sprache: | eng |
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Zusammenfassung: | The selective photoreduction of CO
2
in aqueous media based on earth-abundant elements only, is today a challenging topic. Here we present the anchoring of discrete molecular catalysts on organic polymeric semiconductors via covalent bonding, generating molecular hybrid materials with well-defined active sites for CO
2
photoreduction, exclusively to CO in purely aqueous media. The molecular catalysts are based on aryl substituted Co phthalocyanines that can be coordinated by dangling pyridyl attached to a polymeric covalent triazine framework that acts as a light absorber. This generates a molecular hybrid material that efficiently and selectively achieves the photoreduction of CO
2
to CO in KHCO
3
aqueous buffer, giving high yields in the range of 22 mmol g
−1
(458 μmol g
−1
h
−1
) and turnover numbers above 550 in 48 h, with no deactivation and no detectable H
2
. The electron transfer mechanism for the activation of the catalyst is proposed based on the combined results from time-resolved fluorescence spectroscopy, in situ spectroscopies and quantum chemical calculations.
The selective CO
2
photoreduction in water mediated by earth-abundant photocatalysts remains highly challenging. Here the authors present the coordinative anchorage of molecular catalysts on a pyridine-armed covalent triazine framework for CO
2
photoreduction to CO in fully aqueous solutions. |
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ISSN: | 2041-1723 2041-1723 |
DOI: | 10.1038/s41467-024-54026-2 |