A highly active, robust photocatalyst heterogenized in discrete cages of metal-organic polyhedra for CO2 reduction
- Authors
- Lee, Hyeon Shin; Jee, Seohyeon; Kim, Raekyung; Hoang-Tran Bui; Kim, Bupmo; Kim, Jung-Keun; Park, Kyo Sung; Choi, Wonyong; Kim, Wooyul; Choi, Kyung Min
- Issue Date
- Feb-2020
- Publisher
- ROYAL SOC CHEMISTRY
- Citation
- ENERGY & ENVIRONMENTAL SCIENCE, v.13, no.2, pp 519 - 526
- Pages
- 8
- Journal Title
- ENERGY & ENVIRONMENTAL SCIENCE
- Volume
- 13
- Number
- 2
- Start Page
- 519
- End Page
- 526
- URI
- https://scholarworks.sookmyung.ac.kr/handle/2020.sw.sookmyung/1664
- DOI
- 10.1039/c9ee02619c
- ISSN
- 1754-5692
1754-5706
- Abstract
- 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 [Re-I(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.
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