Details

Autor(en) / Beteiligte

• Stanley, Philip M.
• Haimerl, Johanna
• Thomas, Christopher
• Urstoeger, Alexander
• Schuster, Michael
• Shustova, Natalia B.
• Casini, Angela
• Rieger, Bernhard
• Warnan, Julien
• Fischer, Roland A.

Titel

Host–Guest Interactions in a Metal–Organic Framework Isoreticular Series for Molecular Photocatalytic CO2 Reduction

Ist Teil von

• Angewandte Chemie (International ed.), 2021-08, Vol.60 (33), p.17854-17860

Auflage

International ed. in English

Ort / Verlag

Germany: Wiley Subscription Services, Inc

Erscheinungsjahr

2021

Link zum Volltext

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• 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. The search for more efficient and stable catalysts often yields hybrid host–guest systems. This work rationally engineered a series of metal–organic frameworks as hosts and selectively positioned guests, a CO2 reduction catalyst and a photosensitizer, on the surface or inside the pores for photocatalytic solar fuel production. The results help understand host–guest interactions and provide transferrable criteria for material design.