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Visible-Light Photocatalytic Conversion of Carbon Dioxide by Ni(II) Complexes with N4S2 Coordination: Highly Efficient and Selective Production of Formate
- Visible-Light Photocatalytic Conversion of Carbon Dioxide by Ni(II) Complexes with N4S2 Coordination: Highly Efficient and Selective Production of Formate
- Lee, Sung Eun; Nasirian, Azam; Kim, Ye Eun; Fard, Pegah Tavakoli; Kim, Youngmee; Jeong, Byeongmoon; Kim, Sung-Jin; Baeg, Jin-Ook; Kim, Jinheung
- Ewha Authors
- 김성진; 김영미; 정병문; 김진흥
- SCOPUS Author ID
- 김성진; 김영미; 정병문; 김진흥
- Issue Date
- Journal Title
- JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
- JOURNAL OF THE AMERICAN CHEMICAL SOCIETY vol. 142, no. 45, pp. 19142 - 19149
- AMER CHEMICAL SOC
- SCIE; SCOPUS
- Document Type
- The efficient and selective light-driven conversion of carbon dioxide to formate is a scientific challenge for green chemistry and energy science, especially utilizing visible-light energy and earth-abundant catalytic materials. In this report, two mononuclear Ni(II) complexes of pyridylbenzimidazole (pbi) and pyridylbenzothiazole (pbt), such as Ni(pbt)(pyS)(2) (1) and Ni(pbi)(pyS)(2) (2) (pyS = pyridine-2-thiolate), were prepared and their reactivities studied. The two Ni complexes were examined for CO2 conversion using eosin Y as a photosensitizer upon visible-light irradiation in a H2O/ethanol solvent. The photoreaction of CO2 catalyzed by complexes 1 and 2 selectively affords formate with a high efficiency (14000 turnover number) and a high catalytic selectivity of -99%. Undesirable proton reduction pathways were completely suppressed in the photocatalytic reactions with these sulfur-rich Ni catalysts under CO2. Hydrogen photoproduction was also studied under argon. Their kinetic isotope effects and influence of solution pH for formate and H-2 production in the photocatalytic reactions are described in relation to the reaction mechanisms. These bioinspired Ni(II) catalysts with N/S ligation in relation to [NiFe]-hydrogenases are the first examples of early transition metal complexes affording such high selectivity and efficiencies, providing a future path to design solar-to-fuel processes for artificial photosynthesis.
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