Ruthenium nanoparticles canopied by heptagon-containing saddle-shaped nanographenes as efficient aromatic hydrogenation catalysts
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AuthorCerezo Navarrete, Christian; H. G David, Arthur; Domínguez Codesal, Marcos; González Campaña, Araceli
Royal Society of Chemistry
Chem. Sci., 2022, 13, 13046. DOI: [10.1039/d2sc04228b]
SponsorshipEuropean Research Council (ERC) GA 677023; FEDER(EDRF) Junta de Andalucia-Consejeria de Transformacion Economica, Industria, Conocimiento y Universidades P18-FR2877; Agencia Estatal de Investigacion (AEI); Center for Forestry Research & Experimentation (CIEF) GVA: ACIF/2019/076; HPC CALcul en MIdi-Pyrenees (CALMIP) P0611; Spanish Government RYC2020-030031-I
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 heptagoncontaining 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]CH2 instead of C]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.