Citation: SuHong Zhong, Guanzhong Lu, XueQing Gong. A DFT+U study of the structures and reactivities of polar CeO₂(100) surfaces[J]. Chinese Journal of Catalysis, ;2017, 38(7): 1138-1147. doi: 10.1016/S1872-2067(17)62843-2 shu

A DFT+U study of the structures and reactivities of polar CeO₂(100) surfaces

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

Received Date: 28 February 2017
Revised Date: 17 April 2017

Fund Project: This work was supported the National Natural Science Foundation of China (21421004, 21573067).

Density functional theory calculations corrected by on-site Coulomb interactions were carried out to study the structures of polar CeO₂(100) surfaces as well as activities during catalytic CO oxida-tion. The stabilities of various CeO₂(100) termination structures are discussed, and calculated ener-getics are presented. The most stable CeO₂(100) surface was obtained by removing half the outer-most full layer of oxygen and the surface stability was found to decrease as the exposed oxygen concentration was increased. Assessing the reaction pathways leading to different final products during CO oxidation over the most stable CeO₂(100) surface, we determined that the formation of carbonate species competed with CO₂ desorption. However, during CO oxidation on the less stable CeO₂(100) surfaces having more exposed oxygen, the CO is evidently able to react with surface oxygen, leading to CO₂ formation and desorption. The calculation results and electronic analyses reported herein also indicate that the characteristic Ce 4ƒ orbitals are directly involved in deter-mining the surface stabilities and reactivities.
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A DFT+U study of the structures and reactivities of polar CeO2(100) surfaces

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通讯作者: 陈斌, bchen63@163.com

A DFT+U study of the structures and reactivities of polar CeO₂(100) surfaces