Citation: Jiyuan Liu, Xueqing Gong. Relationships between the activities and Ce³⁺ concentrations of CeO₂(111) for CO oxidation: A first-principle investigation[J]. Chinese Chemical Letters, ;2021, 32(3): 1127-1130. doi: 10.1016/j.cclet.2020.08.033 shu

Relationships between the activities and Ce³⁺ concentrations of CeO₂(111) for CO oxidation: A first-principle investigation

Jiyuan Liu ,
Xueqing Gong ^*,

Key Laboratory for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China

xgong@ecust.edu.cn

Received Date: 20 July 2020
Revised Date: 16 August 2020
Accepted Date: 19 August 2020
Available Online: 20 August 2020

Figures(4)

CO oxidation at ceria surfaces has been studied for decades, and many efforts have been devoted to understanding the effect of surface reduction on the catalytic activity. In this work, we theoretically studied the CO oxidation on the clean and reduced CeO₂(111) surfaces using different surface cells to determine the relationships between the reduction degrees and calculated reaction energetics. It is found that the calculated barrier for the direct reaction between CO and surface lattice O drastically decreases with the increase of surface reduction degree. From electronic analysis, we found that the surface reduction can lead to the occurrence of localized electrons at the surface Ce, which affects the charge distribution at surface O. As the result, the surface O becomes more negatively charged and therefore more active in reacting with CO. This work then suggests that the localized 4f electron reservoir of Ce can act as the "pseudo-anion" at reduced CeO₂ surfaces to activate surface lattice O for catalytic oxidative reactions.
- CO oxidation,
- CeO₂(111),
- Mars-van krevelen mechanism,
- DFT+U,
- Surface reduction
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Relationships between the activities and Ce3+ concentrations of CeO2(111) for CO oxidation: A first-principle investigation

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Relationships between the activities and Ce³⁺ concentrations of CeO₂(111) for CO oxidation: A first-principle investigation