LAPSE:2023.33681
Published Article
LAPSE:2023.33681
Molecular Dye-Sensitized Photocatalysis with Metal-Organic Framework and Metal Oxide Colloids for Fuel Production
Philip M. Stanley, Julien Warnan
April 21, 2023
Colloidal dye-sensitized photocatalysis is a promising route toward efficient solar fuel production by merging properties of catalysis, support, light absorption, and electron mediation in one. Metal-organic frameworks (MOFs) are host materials with modular building principles allowing scaffold property tailoring. Herein, we combine these two fields and compare porous Zr-based MOFs UiO-66-NH2(Zr) and UiO-66(Zr) to monoclinic ZrO2 as model colloid hosts with co-immobilized molecular carbon dioxide reduction photocatalyst fac-ReBr(CO)3(4,4′-dcbpy) (dcbpy = dicarboxy-2,2′-bipyridine) and photosensitizer Ru(bpy)2(5,5′-dcbpy)Cl2 (bpy = 2,2′-bipyridine). These host-guest systems demonstrate selective CO2-to-CO reduction in acetonitrile in presence of an electron donor under visible light irradiation, with turnover numbers (TONs) increasing from ZrO2, to UiO-66, and to UiO-66-NH2 in turn. This is attributed to MOF hosts facilitating electron hopping and enhanced CO2 uptake due to their innate porosity. Both of these phenomena are pronounced for UiO-66-NH2(Zr), yielding TONs of 450 which are 2.5 times higher than under MOF-free homogeneous conditions, highlighting synergistic effects between supramolecular photosystem components in dye-sensitized MOFs.
Keywords
artificial photosystems, dye-sensitized, fuel production, host-guest photosystems, metal oxides, metal-organic frameworks, molecular catalysis
Subject
Suggested Citation
Stanley PM, Warnan J. Molecular Dye-Sensitized Photocatalysis with Metal-Organic Framework and Metal Oxide Colloids for Fuel Production. (2023). LAPSE:2023.33681
Author Affiliations
Stanley PM: Chair of Inorganic and Metal-Organic Chemistry, Department of Chemistry, Technical University of Munich, 85748 Garching, Germany [ORCID]
Warnan J: Chair of Inorganic and Metal-Organic Chemistry, Department of Chemistry, Technical University of Munich, 85748 Garching, Germany
Journal Name
Energies
Volume
14
Issue
14
First Page
4260
Year
2021
Publication Date
2021-07-14
Published Version
ISSN
1996-1073
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Original Submission
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PII: en14144260, Publication Type: Journal Article
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doi:10.3390/en14144260
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Apr 21, 2023
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CC BY 4.0
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