Issue 2, 2020

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

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

Supplementary files

Article information

Article type
Paper
Submitted
14 août 2019
Accepted
29 oct. 2019
First published
29 oct. 2019

Energy Environ. Sci., 2020,13, 519-526

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

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements