Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 23, Pages 10261-10266Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c03097
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Funding
- Japanese Society for the Promotion of Science (JSPS) [18K14241, 19H02713, 16H02268]
- Asahi Glass Foundation (Step-Up Grant)
- Japanese Ministry of Education, Culture, Sports, Science and Technology (MEXT) [18H04247]
- Ministry of the Environment of the Government of Japan
- Grants-in-Aid for Scientific Research [18K14241, 19H02713, 18H04247] Funding Source: KAKEN
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A highly efficient tetradentate PNNP-type Ir photocatalyst, Mes-IrPCY2, was developed for the reduction of carbon dioxide. The photocatalyst furnished formic acid (HCO2H) with 87% selectivity together with carbon monoxide to achieve a turnover number of 2560, which is the highest among CO, reduction photocatalysts without an additional photosensitizer. Mes-IrPCY2 exhibited outstanding photocatalytic CO2 reduction activity in the presence of the sacrificial electron source 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[d]imidazole (BIH) in CO2-saturated N,N-dimethylacetamide under irradiation with visible light. The quantum yield was determined to be 49% for the generation of HCO2H and CO. Electron paramagnetic resonance and UV-vis spectroscopy studies of Mes-IrPCY2 with a sacrificial electron donor revealed that the one-electron-reduced species is the key intermediate for the selective formation of HCO2H.
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