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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

Title
Visible-Light Photocatalytic Conversion of Carbon Dioxide by Ni(II) Complexes with N4S2 Coordination: Highly Efficient and Selective Production of Formate
Authors
Lee, Sung EunNasirian, AzamKim, Ye EunFard, Pegah TavakoliKim, YoungmeeJeong, ByeongmoonKim, Sung-JinBaeg, Jin-OokKim, Jinheung
Ewha Authors
김성진김영미정병문김진흥
SCOPUS Author ID
김성진scopus; 김영미scopus; 정병문scopus; 김진흥scopus
Issue Date
2020
Journal Title
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN
0002-7863JCR Link

1520-5126JCR Link
Citation
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY vol. 142, no. 45, pp. 19142 - 19149
Publisher
AMER CHEMICAL SOC
Indexed
SCIE; SCOPUS WOS
Document Type
Article
Abstract
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.
DOI
10.1021/jacs.0c08145
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자연과학대학 > 화학·나노과학전공 > Journal papers
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