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Issue 2, 2020
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A highly active, robust photocatalyst heterogenized in discrete cages of metal–organic polyhedra for CO2 reduction

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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 [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.

Graphical abstract: A highly active, robust photocatalyst heterogenized in discrete cages of metal–organic polyhedra for CO2 reduction

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Supplementary files

Article information


Submitted
14 Aug 2019
Accepted
29 Oct 2019
First published
29 Oct 2019

Energy Environ. Sci., 2020,13, 519-526
Article type
Paper

A highly active, robust photocatalyst heterogenized in discrete cages of metal–organic polyhedra for CO2 reduction

H. S. Lee, S. Jee, R. Kim, H. Bui, B. Kim, J. Kim, K. S. Park, W. Choi, W. Kim and K. M. Choi, Energy Environ. Sci., 2020, 13, 519
DOI: 10.1039/C9EE02619C

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