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Selective Light-Driven CO2 to CO Reduction by a [FeFe]-Hydrogenase Mimic in Water
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DOI：10.1002/cctc.202401947.png)
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Abstract
En 中文
We report a biomimetic system for light-driven CO2 conversion in lipid bilayers using a [FeFe]-hydrogenase-inspired molecular dyad (PS-CAT) acting simultaneously as photosensitizer and catalyst. The molecular design of PS-CAT consists of both light-harvesting and catalytically active moieties in a single molecule. This structure allows for efficient charge transfer between these two moieties. The PS-CAT consists of only an organic chromophore and an iron complex. Photocatalytic reduction of CO2 to CO (CO2RR) as well as H-2 production (HER) was traced over 56 h to determine CO2RR/HER selectivity. The presence of water in the lipid bilayer system allows for CO2RR selectivity >99 % over the competitive HER, outperforming previous molecular, and liposome-based systems for light-driven CO2 to CO conversion. The product selectivity in CO2RR (e.g., CO, HCOO-, and CH4) was determined via gas chromatography and NMR spectroscopy with C-13-labeled carbon sources. The Stern-Volmer quenching studies on the initial light-driven electron-transfer revealed static quenching and indicated a preassembly of the PS-CAT with the electron donor at the membrane-water interface.
Keywords:
[FeFe]-Hydrogenase mimics
CO2 reduction
Photocatalysis
Selectivity
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