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DOI | 10.1039/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 |
ISSN | 1754-5692 |
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. |
语种 | 英语 |
scopus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 |
来源期刊 | Energy and Environmental Science
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文献类型 | 期刊论文 |
条目标识符 | http://gcip.llas.ac.cn/handle/2XKMVOVA/162583 |
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 |
推荐引用方式 GB/T 7714 | 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 and 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 and Environmental Science 13.2(2020). |
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