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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

Authors :
En Zhao
Manman Li
Beibei Xu
Xue‐Lu Wang
Yu Jing
Ding Ma
Sharon Mitchell
Javier Pérez‐Ramírez
Zupeng Chen
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.

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