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dc.contributor.authorLiu, Xin
dc.contributor.authorZhu, Hongdan
dc.contributor.authorLinguerri, Roberto
dc.contributor.authorHan, Yu
dc.contributor.authorChambaud, Gilberte
dc.contributor.authorMeng, Changgong
dc.date.accessioned2017-10-30T08:39:52Z
dc.date.available2017-10-30T08:39:52Z
dc.date.issued2017-10-12
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.
dc.identifier.issn2365-6549
dc.identifier.doi10.1002/slct.201701663
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.
dc.description.sponsorshipNational Natural Science Foundation of China[21771030, 21573034, 21373036, 21103015, 21771029]
dc.description.sponsorshipChina Scholarship Council[201706060254]
dc.description.sponsorshipSpecial Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund[U1501501]
dc.description.sponsorshipFundamental Research Funds for the Central Universities[DUT15LK18, DUT14LK09, DUT12LK14]
dc.description.sponsorshipSpecial Academic Partner GCR Program from King Abdullah University of Science and Technology
dc.description.sponsorshipUniversité Paris-Est
dc.publisherWiley
dc.relation.urlhttp://onlinelibrary.wiley.com/doi/10.1002/slct.201701663/abstract
dc.titleInterfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitride
dc.typeArticle
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Center
dc.contributor.departmentChemical Science Program
dc.contributor.departmentNanostructured Functional Materials (NFM) laboratory
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalChemistrySelect
dc.contributor.institutionState Key Laboratory of Fine Chemicals, School of Chemistry; Dalian University of Technology; Dalian 116024, P. R. China
dc.contributor.institutionUniversité Paris-Est; Laboratoire Modélisation et Simulation Multi Echelle, MSME UMR 8208 CNRS; 5 bd Descartes, F- 77454 Marne-la-Vallée France
kaust.personHan, Yu
dc.date.published-online2017-10-12
dc.date.published-print2017-10-11


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