Interfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitride

Handle URI:
http://hdl.handle.net/10754/626038
Title:
Interfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitride
Authors:
Liu, Xin; Zhu, Hongdan; Linguerri, Roberto; Han, Yu ( 0000-0003-1462-1118 ) ; Chambaud, Gilberte; Meng, Changgong
Abstract:
We compared the electronic structure and CO oxidation mechanisms over Pt atoms immobilized by both B-vacancies and N-vacancies on gas-exfoliated hexagonal boron nitride. We showed that chemical bonds are formed between the B atoms associated with dangling bonds around the vacancies and Pt atoms. These bonds not only alter the thermodynamics and kinetics for the aggregation and effectively immobilize Pt atoms, but also significantly change the composition and energetic distribution of the electronic states of the composites to circumvent CO poisoning and to favour coadsorption of CO and O2, which further regulates the reactions to proceed through a Langmuir-Hinshelwood mechanism. The CO oxidation over Pt atoms immobilized at N-vacancies involves formation of an intermediate with –C(O)-O−O- bonded to Pt, the generation of CO2 by peroxo O−O bond scission and the reduction of the remnant oxygen, and the calculated energy barriers are 0.49, 0.23 and 0.18 eV, respectively. Such small energy barriers are comparable to those over Pt atoms trapped at B-vacancies, showing the effectiveness of Pt/hexagonal boron nitride atomic composites as catalysts for CO oxidation. These findings also suggest the feasibility of regulating the reaction pathways over single atom catalysts via interfacial engineering.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division
Citation:
Liu X, Zhu H, Linguerri R, Han Y, Chambaud G, et al. (2017) Interfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitride. ChemistrySelect 2: 9412–9419. Available: http://dx.doi.org/10.1002/slct.201701663.
Publisher:
Wiley-Blackwell
Journal:
ChemistrySelect
Issue Date:
12-Oct-2017
DOI:
10.1002/slct.201701663
Type:
Article
ISSN:
2365-6549
Sponsors:
National Natural Science Foundation of China[21771030, 21573034, 21373036, 21103015, 21771029]; China Scholarship Council[201706060254]; Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund[U1501501]; Fundamental Research Funds for the Central Universities[DUT15LK18, DUT14LK09, DUT12LK14]; Special Academic Partner GCR Program from King Abdullah University of Science and Technology; Université Paris-Est
Additional Links:
http://onlinelibrary.wiley.com/doi/10.1002/slct.201701663/abstract
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division

Full metadata record

DC FieldValue Language
dc.contributor.authorLiu, Xinen
dc.contributor.authorZhu, Hongdanen
dc.contributor.authorLinguerri, Robertoen
dc.contributor.authorHan, Yuen
dc.contributor.authorChambaud, Gilberteen
dc.contributor.authorMeng, Changgongen
dc.date.accessioned2017-10-30T08:39:52Z-
dc.date.available2017-10-30T08:39:52Z-
dc.date.issued2017-10-12en
dc.identifier.citationLiu X, Zhu H, Linguerri R, Han Y, Chambaud G, et al. (2017) Interfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitride. ChemistrySelect 2: 9412–9419. Available: http://dx.doi.org/10.1002/slct.201701663.en
dc.identifier.issn2365-6549en
dc.identifier.doi10.1002/slct.201701663en
dc.identifier.urihttp://hdl.handle.net/10754/626038-
dc.description.abstractWe compared the electronic structure and CO oxidation mechanisms over Pt atoms immobilized by both B-vacancies and N-vacancies on gas-exfoliated hexagonal boron nitride. We showed that chemical bonds are formed between the B atoms associated with dangling bonds around the vacancies and Pt atoms. These bonds not only alter the thermodynamics and kinetics for the aggregation and effectively immobilize Pt atoms, but also significantly change the composition and energetic distribution of the electronic states of the composites to circumvent CO poisoning and to favour coadsorption of CO and O2, which further regulates the reactions to proceed through a Langmuir-Hinshelwood mechanism. The CO oxidation over Pt atoms immobilized at N-vacancies involves formation of an intermediate with –C(O)-O−O- bonded to Pt, the generation of CO2 by peroxo O−O bond scission and the reduction of the remnant oxygen, and the calculated energy barriers are 0.49, 0.23 and 0.18 eV, respectively. Such small energy barriers are comparable to those over Pt atoms trapped at B-vacancies, showing the effectiveness of Pt/hexagonal boron nitride atomic composites as catalysts for CO oxidation. These findings also suggest the feasibility of regulating the reaction pathways over single atom catalysts via interfacial engineering.en
dc.description.sponsorshipNational Natural Science Foundation of China[21771030, 21573034, 21373036, 21103015, 21771029]en
dc.description.sponsorshipChina Scholarship Council[201706060254]en
dc.description.sponsorshipSpecial Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund[U1501501]en
dc.description.sponsorshipFundamental Research Funds for the Central Universities[DUT15LK18, DUT14LK09, DUT12LK14]en
dc.description.sponsorshipSpecial Academic Partner GCR Program from King Abdullah University of Science and Technologyen
dc.description.sponsorshipUniversité Paris-Esten
dc.publisherWiley-Blackwellen
dc.relation.urlhttp://onlinelibrary.wiley.com/doi/10.1002/slct.201701663/abstracten
dc.titleInterfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitrideen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalChemistrySelecten
dc.contributor.institutionState Key Laboratory of Fine Chemicals, School of Chemistry; Dalian University of Technology; Dalian 116024, P. R. Chinaen
dc.contributor.institutionUniversité Paris-Est; Laboratoire Modélisation et Simulation Multi Echelle, MSME UMR 8208 CNRS; 5 bd Descartes, F- 77454 Marne-la-Vallée Franceen
kaust.authorHan, Yuen
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