Interfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitride
KAUST DepartmentAdvanced Membranes and Porous Materials Research Center
Physical Sciences and Engineering (PSE) Division
Permanent link to this recordhttp://hdl.handle.net/10754/626038
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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.
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.
SponsorsNational Natural Science Foundation of China[21771030, 21573034, 21373036, 21103015, 21771029]
China Scholarship Council
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