Computational investigation of CO adsorption and oxidation on Mn/CeO 2(111) surface

Ling Chieh Hsu; Ming Kang Tsai; Yu Huan Lu; Hsin Tsung Chen

doi:10.1021/jp310457g

Computational investigation of CO adsorption and oxidation on Mn/CeO ₂(111) surface

Ling Chieh Hsu, Ming Kang Tsai, Yu Huan Lu, Hsin Tsung Chen^*

^*Corresponding author for this work

Department of Chemistry

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

78 Citations (Scopus)

Abstract

The interaction and mechanism for CO oxidation on the Mn/CeO ₂(111) surface have been studied by using periodic density functional theory calculations corrected with the on-site Coulomb interaction via a Hubbard term (DFT + U). It is found that the Mn dopant facilitates oxygen vacancy formation, while the Mn adatoms may restrain oxygen vacancy formation. In addition, physisorbed CO, physisorbed CO₂,and chemisorbed CO (carbonite, CO₂^-) species are observed on the Mn-doped CeO₂(111) surface, in contrast, only physisorbed CO is found on the pure CeO₂(111) surface. The vibrational frequency calculations as well as the calculated adsorption energies are carried to characterize these species. The Mn dopant promotes CO oxidation without any activation energy leading to O vacancy formation and CO₂ desorption. The Bader charge analysis is carried to characterize the oxidation state of Mn ions along the catalytic cycle.

Original language	English
Pages (from-to)	433-441
Number of pages	9
Journal	Journal of Physical Chemistry C
Volume	117
Issue number	1
DOIs	https://doi.org/10.1021/jp310457g
Publication status	Published - 2013 Jan 10

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
General Energy
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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title = "Computational investigation of CO adsorption and oxidation on Mn/CeO 2(111) surface",

abstract = "The interaction and mechanism for CO oxidation on the Mn/CeO 2(111) surface have been studied by using periodic density functional theory calculations corrected with the on-site Coulomb interaction via a Hubbard term (DFT + U). It is found that the Mn dopant facilitates oxygen vacancy formation, while the Mn adatoms may restrain oxygen vacancy formation. In addition, physisorbed CO, physisorbed CO2,and chemisorbed CO (carbonite, CO2-) species are observed on the Mn-doped CeO2(111) surface, in contrast, only physisorbed CO is found on the pure CeO2(111) surface. The vibrational frequency calculations as well as the calculated adsorption energies are carried to characterize these species. The Mn dopant promotes CO oxidation without any activation energy leading to O vacancy formation and CO2 desorption. The Bader charge analysis is carried to characterize the oxidation state of Mn ions along the catalytic cycle.",

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T1 - Computational investigation of CO adsorption and oxidation on Mn/CeO 2(111) surface

AU - Hsu, Ling Chieh

AU - Tsai, Ming Kang

AU - Lu, Yu Huan

AU - Chen, Hsin Tsung

PY - 2013/1/10

Y1 - 2013/1/10

N2 - The interaction and mechanism for CO oxidation on the Mn/CeO 2(111) surface have been studied by using periodic density functional theory calculations corrected with the on-site Coulomb interaction via a Hubbard term (DFT + U). It is found that the Mn dopant facilitates oxygen vacancy formation, while the Mn adatoms may restrain oxygen vacancy formation. In addition, physisorbed CO, physisorbed CO2,and chemisorbed CO (carbonite, CO2-) species are observed on the Mn-doped CeO2(111) surface, in contrast, only physisorbed CO is found on the pure CeO2(111) surface. The vibrational frequency calculations as well as the calculated adsorption energies are carried to characterize these species. The Mn dopant promotes CO oxidation without any activation energy leading to O vacancy formation and CO2 desorption. The Bader charge analysis is carried to characterize the oxidation state of Mn ions along the catalytic cycle.

AB - The interaction and mechanism for CO oxidation on the Mn/CeO 2(111) surface have been studied by using periodic density functional theory calculations corrected with the on-site Coulomb interaction via a Hubbard term (DFT + U). It is found that the Mn dopant facilitates oxygen vacancy formation, while the Mn adatoms may restrain oxygen vacancy formation. In addition, physisorbed CO, physisorbed CO2,and chemisorbed CO (carbonite, CO2-) species are observed on the Mn-doped CeO2(111) surface, in contrast, only physisorbed CO is found on the pure CeO2(111) surface. The vibrational frequency calculations as well as the calculated adsorption energies are carried to characterize these species. The Mn dopant promotes CO oxidation without any activation energy leading to O vacancy formation and CO2 desorption. The Bader charge analysis is carried to characterize the oxidation state of Mn ions along the catalytic cycle.

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Computational investigation of CO adsorption and oxidation on Mn/CeO ₂(111) surface

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