Monodisperse Pt atoms anchored on N-doped graphene as efficient catalysts for CO oxidation: A first-principles investigation

Handle URI:
http://hdl.handle.net/10754/563951
Title:
Monodisperse Pt atoms anchored on N-doped graphene as efficient catalysts for CO oxidation: A first-principles investigation
Authors:
Liu, Xin; Sui, Yanhui; Duan, Ting; Meng, Changgong; Han, Yu ( 0000-0003-1462-1118 )
Abstract:
We performed first-principles based calculations to investigate the electronic structure and the potential catalytic performance of Pt atoms monodispersed on N-doped graphene in CO oxidation. We showed that N-doping can introduce localized defect states in the vicinity of the Fermi level of graphene which will effectively stabilize the deposited Pt atoms. The binding energy of a single Pt atom onto a stable cluster of 3 pyridinic N (PtN3) is up to -4.47 eV, making the diffusion and aggregation of anchored Pt atoms difficult. Both the reaction thermodynamics and kinetics suggest that CO oxidation over PtN3 would proceed through the Langmuir-Hinshelwood mechanism. The reaction barriers for the formation and dissociation of the peroxide-like intermediate are determined to be as low as 0.01 and 0.08 eV, respectively, while that for the regeneration is only 0.15 eV, proving the potential high catalytic performance of PtN3 in CO oxidation, especially at low temperatures. The Pt-d states that are up-shifted by the Pt-N interaction account for the enhanced activation of O2 and the efficient formation and dissociation of the peroxide-like intermediate.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; Nanostructured Functional Materials (NFM) laboratory
Publisher:
Royal Society of Chemistry (RSC)
Journal:
Catal. Sci. Technol.
Issue Date:
2015
DOI:
10.1039/c4cy01327a
Type:
Article
ISSN:
20444753
Sponsors:
This work was supported by the NSFC (21373036, 21103015, and 21271037), the Fundamental Research Funds for the Central Universities (DUT12LK14 and DUT14LK09), the Key Laboratory of Coastal Zone Environmental Processes YICCAS (201203), the Key Science and Technology International Co-operation Foundation of Hainan Province, China (KJHZ2014-08) and the Special Academic Partner GCR Program from King Abdullah University of Science and Technology. Y. H would also like to thank Dalian University of Technology for the Seasky Professorship.
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.authorSui, Yanhuien
dc.contributor.authorDuan, Tingen
dc.contributor.authorMeng, Changgongen
dc.contributor.authorHan, Yuen
dc.date.accessioned2015-08-03T12:20:39Zen
dc.date.available2015-08-03T12:20:39Zen
dc.date.issued2015en
dc.identifier.issn20444753en
dc.identifier.doi10.1039/c4cy01327aen
dc.identifier.urihttp://hdl.handle.net/10754/563951en
dc.description.abstractWe performed first-principles based calculations to investigate the electronic structure and the potential catalytic performance of Pt atoms monodispersed on N-doped graphene in CO oxidation. We showed that N-doping can introduce localized defect states in the vicinity of the Fermi level of graphene which will effectively stabilize the deposited Pt atoms. The binding energy of a single Pt atom onto a stable cluster of 3 pyridinic N (PtN3) is up to -4.47 eV, making the diffusion and aggregation of anchored Pt atoms difficult. Both the reaction thermodynamics and kinetics suggest that CO oxidation over PtN3 would proceed through the Langmuir-Hinshelwood mechanism. The reaction barriers for the formation and dissociation of the peroxide-like intermediate are determined to be as low as 0.01 and 0.08 eV, respectively, while that for the regeneration is only 0.15 eV, proving the potential high catalytic performance of PtN3 in CO oxidation, especially at low temperatures. The Pt-d states that are up-shifted by the Pt-N interaction account for the enhanced activation of O2 and the efficient formation and dissociation of the peroxide-like intermediate.en
dc.description.sponsorshipThis work was supported by the NSFC (21373036, 21103015, and 21271037), the Fundamental Research Funds for the Central Universities (DUT12LK14 and DUT14LK09), the Key Laboratory of Coastal Zone Environmental Processes YICCAS (201203), the Key Science and Technology International Co-operation Foundation of Hainan Province, China (KJHZ2014-08) and the Special Academic Partner GCR Program from King Abdullah University of Science and Technology. Y. H would also like to thank Dalian University of Technology for the Seasky Professorship.en
dc.publisherRoyal Society of Chemistry (RSC)en
dc.titleMonodisperse Pt atoms anchored on N-doped graphene as efficient catalysts for CO oxidation: A first-principles investigationen
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.journalCatal. Sci. Technol.en
dc.contributor.institutionSchool of Chemistry, Dalian University of TechnologyDalian, Chinaen
kaust.authorHan, Yuen
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