Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume -, Issue -, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202218720
Keywords
Acetaldehyde Generation; Atomic Economy; Ethanol Oxidation; Identical C-2 Product; Photocatalytic CO2 Reduction
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A potassium and rubidium co-modified carbon nitride (CN-KRb) was reported for the simultaneous co-photocatalytic CO2 reduction and ethanol oxidation to produce the same product, CH3CHO. The CN-KRb showed record photocatalytic activity and high selectivity, with the involvement of rubidium and potassium. The study confirmed the participation of H+ from ethanol oxidation in the CO2 reduction process, achieving near ideal overall atomic economy. This work provides a new strategy for effective and sustainable conversion of CO2 into the same product through photoexcited electron and hole utilization.
Photocatalytic conversion of CO2 is of great interest but it often suffers sluggish oxidation half reaction and undesired by-products. Here, we report for the first the simultaneous co-photocatalytic CO2 reduction and ethanol oxidation towards one identical value-added CH3CHO product on a rubidium and potassium co-modified carbon nitride (CN-KRb). The CN-KRb offers a record photocatalytic activity of 1212.3 mu mol h(-1)g(-1) with a high selectivity of 93.3 % for CH3CHO production, outperforming all the state-of-art CO2 photocatalysts. It is disclosed that the introduced Rb boosts the *OHCCHO fromation and facilitates the CH3CHO desorption, while K promotes ethanol adsorption and activation. Moreover, the H+ stemming from ethanol oxidation is confirmed to participate in the CO2 reduction process, endowing near ideal overall atomic economy. This work provides a new strategy for effective use of the photoexcited electron and hole for high selective and sustainable conversion of CO2 paired with oxidation reaction into identical product.
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