Theoretical and experimental investigations on single-atom catalysis: Ir1/FeOxfor CO oxidation

Jin Xia Liang; Jian Lin; Xiao Feng Yang; Ai Qin Wang; Bo Tao Qiao; Jingyue Liu; Tao Zhang; Jun Li

doi:10.1021/jp503769d

Theoretical and experimental investigations on single-atom catalysis: Ir₁/FeO_xfor CO oxidation

Jin Xia Liang, Jian Lin, Xiao Feng Yang, Ai Qin Wang, Bo Tao Qiao, Jingyue Liu, Tao Zhang, Jun Li

Physics

Research output: Contribution to journal › Article › peer-review

142 Scopus citations

Abstract

Through periodic density functional theory (DFT) calculations we have investigated the catalytic mechanism of CO oxidation on an Ir₁/FeO_xsingle-atom catalyst (SAC). The rate-determining step in the catalytic cycle of CO oxidation is shown to be the formation of the second CO₂between the adsorbed CO on the surface of Ir₁/FeO_xand the dissociated O atom from gas phase. Comparing with Pt₁/FeO_xcatalyst, the reaction activation barrier for CO oxidation is higher by 0.62 eV and the adsorption energy for CO molecule is larger by 0.69 eV on Ir₁/FeO_x. These results reveal that Ir₁/FeO_xcatalyst has a lower activity for CO oxidation than Pt₁/FeO_x, which is consistent with our experimental results. The results can help to understand the fundamental mechanism of monodispersed surface atoms and to design highly active single-atom catalysts.

Original language	English (US)
Pages (from-to)	21945-21951
Number of pages	7
Journal	Journal of Physical Chemistry C
Volume	118
Issue number	38
DOIs	https://doi.org/10.1021/jp503769d
State	Published - Sep 25 2014

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Energy(all)
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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title = "Theoretical and experimental investigations on single-atom catalysis: Ir1/FeOxfor CO oxidation",

abstract = "Through periodic density functional theory (DFT) calculations we have investigated the catalytic mechanism of CO oxidation on an Ir1/FeOxsingle-atom catalyst (SAC). The rate-determining step in the catalytic cycle of CO oxidation is shown to be the formation of the second CO2between the adsorbed CO on the surface of Ir1/FeOxand the dissociated O atom from gas phase. Comparing with Pt1/FeOxcatalyst, the reaction activation barrier for CO oxidation is higher by 0.62 eV and the adsorption energy for CO molecule is larger by 0.69 eV on Ir1/FeOx. These results reveal that Ir1/FeOxcatalyst has a lower activity for CO oxidation than Pt1/FeOx, which is consistent with our experimental results. The results can help to understand the fundamental mechanism of monodispersed surface atoms and to design highly active single-atom catalysts.",

author = "Liang, {Jin Xia} and Jian Lin and Yang, {Xiao Feng} and Wang, {Ai Qin} and Qiao, {Bo Tao} and Jingyue Liu and Tao Zhang and Jun Li",

note = "Publisher Copyright: {\textcopyright} 2014 American Chemical Society.",

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doi = "10.1021/jp503769d",

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TY - JOUR

T1 - Theoretical and experimental investigations on single-atom catalysis

T2 - Ir1/FeOxfor CO oxidation

AU - Liang, Jin Xia

AU - Lin, Jian

AU - Yang, Xiao Feng

AU - Wang, Ai Qin

AU - Qiao, Bo Tao

AU - Liu, Jingyue

AU - Zhang, Tao

AU - Li, Jun

PY - 2014/9/25

Y1 - 2014/9/25

N2 - Through periodic density functional theory (DFT) calculations we have investigated the catalytic mechanism of CO oxidation on an Ir1/FeOxsingle-atom catalyst (SAC). The rate-determining step in the catalytic cycle of CO oxidation is shown to be the formation of the second CO2between the adsorbed CO on the surface of Ir1/FeOxand the dissociated O atom from gas phase. Comparing with Pt1/FeOxcatalyst, the reaction activation barrier for CO oxidation is higher by 0.62 eV and the adsorption energy for CO molecule is larger by 0.69 eV on Ir1/FeOx. These results reveal that Ir1/FeOxcatalyst has a lower activity for CO oxidation than Pt1/FeOx, which is consistent with our experimental results. The results can help to understand the fundamental mechanism of monodispersed surface atoms and to design highly active single-atom catalysts.

AB - Through periodic density functional theory (DFT) calculations we have investigated the catalytic mechanism of CO oxidation on an Ir1/FeOxsingle-atom catalyst (SAC). The rate-determining step in the catalytic cycle of CO oxidation is shown to be the formation of the second CO2between the adsorbed CO on the surface of Ir1/FeOxand the dissociated O atom from gas phase. Comparing with Pt1/FeOxcatalyst, the reaction activation barrier for CO oxidation is higher by 0.62 eV and the adsorption energy for CO molecule is larger by 0.69 eV on Ir1/FeOx. These results reveal that Ir1/FeOxcatalyst has a lower activity for CO oxidation than Pt1/FeOx, which is consistent with our experimental results. The results can help to understand the fundamental mechanism of monodispersed surface atoms and to design highly active single-atom catalysts.

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Theoretical and experimental investigations on single-atom catalysis: Ir₁/FeO_xfor CO oxidation

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