dc.contributor.author |
Albani, Davide |
dc.contributor.author |
Shahrokhi, Masoud |
dc.contributor.author |
Chen, Zupeng |
dc.contributor.author |
Mitchell, Sharon |
dc.contributor.author |
Hauert, Roland |
dc.contributor.author |
López, Núria |
dc.contributor.author |
Pérez-Ramírez, Javier |
dc.date.accessioned |
2019-07-26T13:46:20Z |
dc.date.available |
2019-07-26T13:46:20Z |
dc.date.issued |
2018-07-06 |
dc.identifier.uri |
http://hdl.handle.net/2072/359784 |
dc.format.extent |
2634 p. |
dc.language.iso |
eng |
dc.rights |
L'accés als continguts d'aquest document queda condicionat a l'acceptació de les condicions d'ús establertes per la següent llicència Creative Commons:http://creativecommons.org/licenses/by-nc-nd/4.0/ |
dc.source |
RECERCAT (Dipòsit de la Recerca de Catalunya) |
dc.subject.other |
54 |
dc.title |
Selective ensembles in supported palladium sulfide nanoparticles for alkyne semi-hydrogenation |
dc.type |
info:eu-repo/semantics/article |
dc.type |
info:eu-repo/semantics/acceptedVersion |
dc.embargo.terms |
cap |
dc.identifier.doi |
10.1038/s41467-018-05052-4 |
dc.rights.accessLevel |
info:eu-repo/semantics/openAccess |
dc.description.abstract |
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. |