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DOI10.1039/c9ee02619c
A highly active, robust photocatalyst heterogenized in discrete cages of metal-organic polyhedra for CO2 reduction
Lee H.S.; Jee S.; Kim R.; Bui H.-T.; Kim B.; Kim J.-K.; Park K.S.; Choi W.; Kim W.; Choi K.M.
发表日期2020
ISSN17545692
起始页码519
结束页码526
卷号13期号:2
英文摘要The heterogenization of photocatalytic molecules typically enhances stability at the expense of activity. Therefore, a new approach to stabilizing molecular catalysts without compromising their original catalytic features is highly desired. In this study, we found that Zr-based metal-organic polyhedra (MOP) stabilized the photocatalytic compound ReTC [ReI(CO)3(BPYDC)(Cl), BPYDC = 2,2′-bipyridine-5,5′-dicarboxylate] without degrading its catalytic activity. ReTC was chemically bound to discrete cages of the MOP and was found to maintain its maximum CO2-to-CO conversion activity (660 h-1 turnover frequency (TOF)) for at least 24 h under visible light irradiation. The free molecular form of the same compound (H2ReTC) initially showed an activity of 131 h-1 TOF, which was lost within 2 h. The cumulative turnover number of ReTC-MOP after a 24 h reaction was 12 847, which was 42.0 times the value of 306 for molecular ReTC. The high catalytic activity and stability of ReTC-MOP are attributed to the fact that this MOP material provides an extremely small framework for chemical binding of ReTC, such that the catalyst has a high degree of motional freedom and enhanced light absorption while being protected in the reaction solution. © 2020 The Royal Society of Chemistry.
英文关键词Carbon dioxide; Carboxylation; Chemical stability; Geometry; Light; Light absorption; Organometallics; Photocatalytic activity; Chemical binding; Cumulative turnover; Enhanced light absorptions; Metal-organic polyhedron; Molecular catalysts; Reaction solutions; Turnover frequency; Visible-light irradiation; Catalyst activity; carbon dioxide; carbon emission; catalysis; chemical binding; emission control; molecular analysis; photochemistry
语种英语
来源期刊Energy & Environmental Science
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/189697
作者单位Department of Chemical and Biological Engineering, Sookmyung Women's University, Seoul, 04310, South Korea; Division of Environmental Science and Engineering, Pohang University of Science and Technology (POSTECH), Pohang, 37673, South Korea; LG Science Park 30, Magokjungang 10-ro, Gangseo-gu Seoul, 07796, South Korea
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Lee H.S.,Jee S.,Kim R.,et al. A highly active, robust photocatalyst heterogenized in discrete cages of metal-organic polyhedra for CO2 reduction[J],2020,13(2).
APA Lee H.S..,Jee S..,Kim R..,Bui H.-T..,Kim B..,...&Choi K.M..(2020).A highly active, robust photocatalyst heterogenized in discrete cages of metal-organic polyhedra for CO2 reduction.Energy & Environmental Science,13(2).
MLA Lee H.S.,et al."A highly active, robust photocatalyst heterogenized in discrete cages of metal-organic polyhedra for CO2 reduction".Energy & Environmental Science 13.2(2020).
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