dc.contributor.author |
Lari, Giacomo M. |
dc.contributor.author |
Puertolas, Begoña |
dc.contributor.author |
Shahrokhi, Masoud |
dc.contributor.author |
López, Núria |
dc.contributor.author |
Pérez- Ramirez, Javier |
dc.date.accessioned |
2019-07-26T10:01:03Z |
dc.date.available |
2019-07-26T10:01:03Z |
dc.date.issued |
2017-02-06 |
dc.identifier.uri |
http://hdl.handle.net/2072/359765 |
dc.format.extent |
1775 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 |
Hybrid Palladium Nanoparticles for Direct Hydrogen Peroxide Synthesis: The Key Role of the Ligand |
dc.type |
info:eu-repo/semantics/article |
dc.type |
info:eu-repo/semantics/acceptedVersion |
dc.embargo.terms |
12 mesos |
dc.identifier.doi |
10.1002/anie.201610552 |
dc.rights.accessLevel |
info:eu-repo/semantics/openAccess |
dc.description.abstract |
Ligand-modified palladium nanoparticles deposited
on a carbon carrier efficiently catalyze the direct synthesis of
H2O2 and the unique performance is due to their hybrid
nanostructure. Catalytic testing demonstrated that the selectivity
increases with the HHDMA ligand content from 10% for
naked nanoparticles up to 80%, rivalling that obtained with
state-of-the-art bimetallic catalysts (HHDMA=C20H46NO5P).
Furthermore, it remains stable over five consecutive reaction
runs owing to the high resistance towards leaching of the
organic moiety, arising from its bond with the metal surface. As
rationalized by density functional theory, this behavior is
attributed to the adsorption mode of the reaction intermediates
on the metal surface. Whereas they lie flat in the absence of the
organic shell, their electrostatic interaction with the ligand
result in a unique vertical configuration which prevents further
dissociation and over-hydrogenation. These findings demonstrate
the importance of understanding substrate–ligand interactions
in capped nanoparticles to develop smart catalysts for
the sustainable manufacture of hydrogen peroxide. |