A strategy to improve homogeneous molecular catalyst stability, efficiency, and selectivity is the immobilization on supporting surfaces or within host matrices. Herein, we examine the co-immobilization of a CO2 reduction catalyst [ReBr(CO)3(4,4′-dcbpy)] and a photosensitizer [Ru(bpy)2(5,5′-dcbpy)]Cl2 using the isoreticular series of metal–organic frameworks (MOFs) UiO-66, -67, and -68. Specific host pore size choice enables distinct catalyst and photosensitizer spatial location—either at the outer MOF particle surface or inside the MOF cavities—affecting catalyst stability, electronic communication between reaction center and photosensitizer, and consequently the apparent catalytic rates. These results allow for a rational understanding of an optimized supramolecular layout of catalyst, photosensitizer, and host matrix.
Digital Object Identifier (DOI)
Published in Angewandte Chemie International Edition, Volume 60, Issue 33, 2021, pages 17854-17860.
© 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH
This is an open access article under the terms of the Creative Commons Attribution-NonCommercial-NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made.
Stanley, P. M., Haimerl, J., Thomas, C., Urstoeger, A., Schuster, M., Shustova, N. B., Casini, A., Rieger, B., Warnan, J., & Fischer, R. A. (2021). Host–guest interactions in a metal–organic framework ISORETICULAR series for molecular photocatalytic CO2 reduction. Angewandte Chemie International Edition, 60(33), 17854–17860. https://doi.org/10.1002/anie.202102729