Substrate-mediated enhanced activity of Ru nanoparticles in catalytic hydrogenation of benzene

Handle URI:
http://hdl.handle.net/10754/561984
Title:
Substrate-mediated enhanced activity of Ru nanoparticles in catalytic hydrogenation of benzene
Authors:
Liu, Xin; Meng, Changgong; Han, Yu ( 0000-0003-1462-1118 )
Abstract:
The impact of carbon substrate-Ru nanoparticle interactions on benzene and hydrogen adsorption that is directly related to the performance in catalytic hydrogenation of benzene has been investigated by first-principles based calculations. The stability of Ru 13 nanoparticles is enhanced by the defective graphene substrate due to the hybridization between the dsp states of the Ru 13 particle with the sp 2 dangling bonds at the defect sites. The local curvature formed at the interface will also raise the Ru atomic diffusion barrier, and prohibit the particle sintering. The strong interfacial interaction results in the shift of averaged d-band center of the deposited Ru nanoparticle, from -1.41 eV for a freestanding Ru 13 particle, to -1.17 eV for the Ru/Graphene composites, and to -1.54 eV on mesocellular foam carbon. Accordingly, the adsorption energies of benzene are increased from -2.53 eV for the Ru/mesocellular foam carbon composites, to -2.62 eV on freestanding Ru 13 particles, to -2.74 eV on Ru/graphene composites. A similar change in hydrogen adsorption is also observed, and all these can be correlated to the shift of the d-band center of the nanoparticle. Thus, Ru nanoparticles graphene composites are expected to exhibit both high stability and superior catalytic performance in hydrogenation of arenes. © 2012 The Royal Society of Chemistry.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Advanced Nanofabrication, Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; Nanostructured Functional Materials (NFM) laboratory
Publisher:
Royal Society of Chemistry
Journal:
Nanoscale
Issue Date:
2012
DOI:
10.1039/c2nr00031h
PubMed ID:
22392351
Type:
Article
ISSN:
20403364
Sponsors:
This work was supported by the Special Academic Partner GCR Program from the King Abdullah University of Science and Technology. X.L. would also thank the Chinese Scholarship Council (2009606533), NSFC of China (20273012, and 21103015) and Fundamental Research Funds for the Central Universities (DUT11LK19) for financial support.
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Advanced Nanofabrication, Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division; Chemical Science Program

Full metadata record

DC FieldValue Language
dc.contributor.authorLiu, Xinen
dc.contributor.authorMeng, Changgongen
dc.contributor.authorHan, Yuen
dc.date.accessioned2015-08-03T09:35:36Zen
dc.date.available2015-08-03T09:35:36Zen
dc.date.issued2012en
dc.identifier.issn20403364en
dc.identifier.pmid22392351en
dc.identifier.doi10.1039/c2nr00031hen
dc.identifier.urihttp://hdl.handle.net/10754/561984en
dc.description.abstractThe impact of carbon substrate-Ru nanoparticle interactions on benzene and hydrogen adsorption that is directly related to the performance in catalytic hydrogenation of benzene has been investigated by first-principles based calculations. The stability of Ru 13 nanoparticles is enhanced by the defective graphene substrate due to the hybridization between the dsp states of the Ru 13 particle with the sp 2 dangling bonds at the defect sites. The local curvature formed at the interface will also raise the Ru atomic diffusion barrier, and prohibit the particle sintering. The strong interfacial interaction results in the shift of averaged d-band center of the deposited Ru nanoparticle, from -1.41 eV for a freestanding Ru 13 particle, to -1.17 eV for the Ru/Graphene composites, and to -1.54 eV on mesocellular foam carbon. Accordingly, the adsorption energies of benzene are increased from -2.53 eV for the Ru/mesocellular foam carbon composites, to -2.62 eV on freestanding Ru 13 particles, to -2.74 eV on Ru/graphene composites. A similar change in hydrogen adsorption is also observed, and all these can be correlated to the shift of the d-band center of the nanoparticle. Thus, Ru nanoparticles graphene composites are expected to exhibit both high stability and superior catalytic performance in hydrogenation of arenes. © 2012 The Royal Society of Chemistry.en
dc.description.sponsorshipThis work was supported by the Special Academic Partner GCR Program from the King Abdullah University of Science and Technology. X.L. would also thank the Chinese Scholarship Council (2009606533), NSFC of China (20273012, and 21103015) and Fundamental Research Funds for the Central Universities (DUT11LK19) for financial support.en
dc.publisherRoyal Society of Chemistryen
dc.titleSubstrate-mediated enhanced activity of Ru nanoparticles in catalytic hydrogenation of benzeneen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentAdvanced Nanofabrication, Imaging and Characterization Core Laben
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentNanostructured Functional Materials (NFM) laboratoryen
dc.identifier.journalNanoscaleen
dc.contributor.institutionSchool of Chemistry, Dalian University of Technology, 116024, Chinaen
kaust.authorLiu, Xinen
kaust.authorHan, Yuen
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