Ruthenium nanoparticles canopied by heptagon-containing saddle-shaped nanographenes as efficient aromatic hydrogenation catalysts

The search for new ligands capable of modifying the metal nanoparticle (MNP) catalytic behavior is of increasing interest. Herein we present the first example of RuNPs stabilized with non-planar heptagon-containing saddle-shaped nanographenes ( Ru@1 and Ru@2 ). The resemblance to graphene-supported...

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Bibliographic Details
Published in:Chemical science (Cambridge) 2022-11, Vol.13 (44), p.1346-1359
Main Authors: Cerezo-Navarrete, Christian, David, Arthur H. G, García-Zaragoza, Adrián, Codesal, Marcos D, Oña-Burgos, Pascual, del Rosal, Iker, Poteau, Romuald, Campaña, Araceli G, Martínez-Prieto, Luis M
Format: Article
Language:English
Subjects:
Catalysts
Chemical Sciences
Chemistry
Graphene
Hydrogenation
Ligands
Nanoparticles
Ruthenium
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Summary:The search for new ligands capable of modifying the metal nanoparticle (MNP) catalytic behavior is of increasing interest. Herein we present the first example of RuNPs stabilized with non-planar heptagon-containing saddle-shaped nanographenes ( Ru@1 and Ru@2 ). The resemblance to graphene-supported MNPs makes these non-planar nanographene-stabilized RuNPs very attractive systems to further investigate graphene-metal interactions. A combined theoretical/experimental study allowed us to explore the coordination modes and dynamics of these nanographenes at the Ru surface. The curvature of these saddle-shaped nanographenes makes them efficient MNP stabilizers. The resulting RuNPs were found to be highly active catalysts for the hydrogenation of aromatics, including platform molecules derived from biomass ( i.e. HMF) or liquid organic hydrogen carriers ( i.e. N -indole). A significant ligand effect was observed since a minor modification on the hept-HBC structure (C&z.dbd;CH 2 instead of C&z.dbd;O) was reflected in a substantial increase in the MNP activity. Finally, the stability of these canopied RuNPs was investigated by multiple addition experiments, proving to be stable catalysts for at least 96 h. Ruthenium nanoparticles stabilized with non-planar polycyclic aromatic hydrocarbons (PAHs) are active catalysts in the hydrogenation of aromatic substrates under mild conditions.
ISSN:2041-6520
2041-6539
DOI:10.1039/d2sc04228b