Selective ensembles in supported palladium sulfide nanoparticles for alkyne semi-hydrogenation
| Autor: | Albani, Davide, Shahrokhi, Masoud, Chen, Zupeng, Mitchell, Sharon, Hauert, Roland, López, Núria, Pérez-Ramírez, Javier |
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| Rok vydání: | 2017 |
| Předmět: | |
| Zdroj: | Nature Communications Nature Communications, Vol 9, Iss 1, Pp 1-11 (2018) RECERCAT (Dipòsit de la Recerca de Catalunya) Recercat. Dipósit de la Recerca de Catalunya instname Nature Communications, 9 (1) |
| ISSN: | 2041-1723 |
| Popis: | Ensemble control has been intensively pursued for decades to identify sustainable alternatives to the Lindlar catalyst (PdPb/CaCO3) applied for the partial hydrogenation of alkynes in industrial organic synthesis. Although the geometric and electronic requirements are known, a literature survey illustrates the difficulty of transferring this knowledge into an efficient and robust catalyst. Here, we report a simple treatment of palladium nanoparticles supported on graphitic carbon nitride with aqueous sodium sulfide, which directs the formation of a nanostructured Pd3S phase with controlled crystallographic orientation, exhibiting unparalleled performance in the semi-hydrogenation of alkynes in the liquid phase. The exceptional behavior is linked to the multifunctional role of sulfur. Apart from defining a structure integrating spatially-isolated palladium trimers, the active ensembles, the modifier imparts a bifunctional mechanism and weak binding of the organic intermediates. Similar metal trimers are also identified in Pd4S, evidencing the pervasiveness of these selective ensembles in supported palladium sulfides. Nature Communications, 9 (1) ISSN:2041-1723 |
| Databáze: | OpenAIRE |
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