Palladium nanoparticles/defective graphene composites as oxygen reduction electrocatalysts: A first-principles study

Handle URI:
http://hdl.handle.net/10754/562085
Title:
Palladium nanoparticles/defective graphene composites as oxygen reduction electrocatalysts: A first-principles study
Authors:
Liu, Xin; Li, Lin; Meng, Changgong; Han, Yu ( 0000-0003-1462-1118 )
Abstract:
The impact of graphene substrate-Pd nanoparticle interaction on the O, OH, and OOH adsorption that is directly related to the electrocatalytic performance of these composites in oxygen reduction reaction (ORR) has been investigated by first-principles-based calculations. The calculated binding energy of a Pd 13 nanoparticle on a single vacancy graphene is as high as -6.10 eV, owing to the hybridization between the dsp states of the Pd particles with the sp 2 dangling bonds at the defect sites. The strong interaction results in the averaged d-band center of the deposited Pd nanoparticles shifted away from the Fermi level from -1.02 to -1.45 eV. Doping the single vacancy graphene with B or N will further tune the average d-band center and also the activity of the composite toward O, OH, and OOH adsorption. The adsorption energies of O, OH, and OOH are reduced from -4.78, -4.38, and -1.56 eV on the freestanding Pd 13 nanoparticle to -4.57, -2.66, and -1.39 eV on Pd 13/single vacancy graphene composites, showing that the defective graphene substrate will not only stabilize the Pd nanoparticles but also reduce the adsorption energies of the O-containing species to the Pd particle, and so as the poisoning of the ORR active sites. © 2011 American Chemical Society.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; Nanostructured Functional Materials (NFM) laboratory
Publisher:
American Chemical Society
Journal:
Journal of Physical Chemistry C
Issue Date:
2-Feb-2012
DOI:
10.1021/jp2096983
Type:
Article
ISSN:
19327447
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 like to thank NSFC of China (11174045, 21103015), Chinese Scholarship Council (2009606533), Young Teacher Training Program of Dalian University of Technology (1000-893238, 1000-893374), and Fundamental Research Funds for the Central Universities (DUT11LK19) for financial support.
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Chemical Science Program

Full metadata record

DC FieldValue Language
dc.contributor.authorLiu, Xinen
dc.contributor.authorLi, Linen
dc.contributor.authorMeng, Changgongen
dc.contributor.authorHan, Yuen
dc.date.accessioned2015-08-03T09:44:26Zen
dc.date.available2015-08-03T09:44:26Zen
dc.date.issued2012-02-02en
dc.identifier.issn19327447en
dc.identifier.doi10.1021/jp2096983en
dc.identifier.urihttp://hdl.handle.net/10754/562085en
dc.description.abstractThe impact of graphene substrate-Pd nanoparticle interaction on the O, OH, and OOH adsorption that is directly related to the electrocatalytic performance of these composites in oxygen reduction reaction (ORR) has been investigated by first-principles-based calculations. The calculated binding energy of a Pd 13 nanoparticle on a single vacancy graphene is as high as -6.10 eV, owing to the hybridization between the dsp states of the Pd particles with the sp 2 dangling bonds at the defect sites. The strong interaction results in the averaged d-band center of the deposited Pd nanoparticles shifted away from the Fermi level from -1.02 to -1.45 eV. Doping the single vacancy graphene with B or N will further tune the average d-band center and also the activity of the composite toward O, OH, and OOH adsorption. The adsorption energies of O, OH, and OOH are reduced from -4.78, -4.38, and -1.56 eV on the freestanding Pd 13 nanoparticle to -4.57, -2.66, and -1.39 eV on Pd 13/single vacancy graphene composites, showing that the defective graphene substrate will not only stabilize the Pd nanoparticles but also reduce the adsorption energies of the O-containing species to the Pd particle, and so as the poisoning of the ORR active sites. © 2011 American Chemical Society.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 like to thank NSFC of China (11174045, 21103015), Chinese Scholarship Council (2009606533), Young Teacher Training Program of Dalian University of Technology (1000-893238, 1000-893374), and Fundamental Research Funds for the Central Universities (DUT11LK19) for financial support.en
dc.publisherAmerican Chemical Societyen
dc.titlePalladium nanoparticles/defective graphene composites as oxygen reduction electrocatalysts: A first-principles studyen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentNanostructured Functional Materials (NFM) laboratoryen
dc.identifier.journalJournal of Physical Chemistry Cen
dc.contributor.institutionSchool of Chemistry, Dalian University of Technology, Dalian, 116024, Chinaen
kaust.authorLiu, Xinen
kaust.authorHan, Yuen
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