Transfer Hydrogenation with a Carbon‐Nitride‐Supported Palladium Single‐Atom Photocatalyst and Water as a Proton Source
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. Show more
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publishedExternal links
Journal / series
Angewandte ChemieVolume
Pages / Article No.
Publisher
Wiley-VCHSubject
Carbon nitride; Operando NMR; Photocatalysis; Single-Atom Catalysts; Transfer hydrogenationOrganisational unit
03871 - Pérez-Ramírez, Javier / Pérez-Ramírez, Javier
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Is identical to: http://hdl.handle.net/20.500.11850/568887
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