Journal
ENERGY & ENVIRONMENTAL SCIENCE
Volume 15, Issue 1, Pages 225-233Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ee02073k
Keywords
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Funding
- National Natural Science Foundation of China [61904167]
- Natural Science Foundation of Guangdong Province [2019A1515012081]
- Science and Technology Program of Guangzhou [202002030017]
- GDAS' Project of Science and Technology Development
- China Postdoctoral Science Foundation [2020M672638]
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This study presents a new strategy for designing carbon nitrides for highly selective and sustainable conversion of CO2 to CH3CHO, achieved through the selective photocatalytic hydrogenation of CO2 to CH3CHO using a modified polymeric carbon nitride under mild conditions.
Photocatalytic conversion of CO2 to CH3CHO is of increasing interest but confronts the significant challenges of forming C-C bonds and keeping the C=O bond intact throughout the process. Here, we report the selective photocatalytic hydrogenation of CO2 to CH3CHO using a modified polymeric carbon nitride (PCN) under mild conditions. The locally crystallized PCN offers a photocatalytic activity of 1814.7 mu mol h(-1) g(-1) with a high selectivity of 98.3% for CH3CHO production and a quantum efficiency of 22.4% at 385 nm, outperforming all the state-of-art CO2 photocatalysts. The promoted formation of the *OCCHO intermediate on the locally crystallized PCN is disclosed as the key factor leading to the highly selective CH3CHO generation. The locally crystallized PCN favors spontaneous C-C coupling towards *OCCHO formation rather than *CHO protonation, thus preventing HCHO formation. This work provides a new strategy for designing carbon nitrides for highly selective and sustainable conversion of CO2 to CH3CHO.
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