Reversible Switching CuII /CuI Single Sites Catalyze High-rate and Selective CO2 Photoreduction.
Angew Chem Int Ed Engl
; 62(1): e202215247, 2023 Jan 02.
Article
in En
| MEDLINE
| ID: mdl-36347791
ABSTRACT
Herein, we first design a model of reversible redox-switching metal-organic framework single-unit-cell sheets, where the abundant metal single sites benefit for highly selective CO2 reduction, while the reversible redox-switching metal sites can effectively activate CO2 molecules. Taking the synthetic Cu-MOF single-unit-cell sheets as an example, synchrotron-radiation quasi in situ X-ray photoelectron spectra unravel the reversible switching CuII /CuI single sites initially accept photoexcited electrons and then donate them to CO2 molecules, which favors the rate-liming activation into CO2 δ- , verified by in situ FTIR spectra and Gibbs free energy calculations. As an outcome, Cu-MOF single-unit-cell sheets achieve near 100 % selectivity for CO2 photoreduction to CO with a high rate of 860â
µmol g-1 h-1 without any sacrifice reagent or photosensitizer, where both the activity and selectivity outperform previously reported photocatalysts evaluated under similar conditions.
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Database:
MEDLINE
Language:
En
Journal:
Angew Chem Int Ed Engl
Year:
2023
Type:
Article