Interfacial-Bonding-Regulated CO Oxidation over Pt Atoms Immobilized on Gas-Exfoliated Hexagonal Boron Nitride
Type
ArticleKAUST Department
Advanced Membranes and Porous Materials Research CenterChemical Science Program
Nanostructured Functional Materials (NFM) laboratory
Physical Science and Engineering (PSE) Division
Date
2017-10-12Online Publication Date
2017-10-12Print Publication Date
2017-10-11Permanent link to this record
http://hdl.handle.net/10754/626038
Metadata
Show full item recordAbstract
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.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.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
Publisher
WileyJournal
ChemistrySelectAdditional Links
http://onlinelibrary.wiley.com/doi/10.1002/slct.201701663/abstractae974a485f413a2113503eed53cd6c53
10.1002/slct.201701663