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Transfer Hydrogenation with a Carbon‐Nitride‐Supported Palladium Single‐Atom Photocatalyst and Water as a Proton Source
Transfer Hydrogenation with a Carbon‐Nitride‐Supported Palladium Single‐Atom Photocatalyst and Water as a Proton Source
- Source :
- Angewandte Chemie. 134
- Publication Year :
- 2022
- Publisher :
- Wiley, 2022.
-
Abstract
- Solar-driven transfer hydrogenation of unsaturated bonds has received considerable attention in the research area of sustainable organic synthesis; however, water, the ultimate green source of hydrogen, has rarely been investigated due to the high barrier associated with splitting of water molecules. We report a carbon-nitride-supported palladium single-atom heterogeneous catalyst with unparalleled performance in photocatalytic water-donating transfer hydrogenation compared to its nanoparticle counterparts. Isotopic-labeling experiments and operando nuclear magnetic resonance measurements confirm the direct hydrogenation mechanism using in situ-generated protons from water splitting under visible-light irradiation. Density functional theory calculations attribute the high activity to lower barriers for hydrogenation, facilitated desorption of ethylbenzene, and facile hydrogen replenishment from water on the atomic palladium sites.
- Subjects :
- General Chemistry
General Medicine
Catalysis
Subjects
Details
- ISSN :
- 15213757 and 00448249
- Volume :
- 134
- Database :
- OpenAIRE
- Journal :
- Angewandte Chemie
- Accession number :
- edsair.doi.dedup.....0aecdfa8111133a53a594b2e45208051
- Full Text :
- https://doi.org/10.1002/ange.202207410