The absence of a gap state and enhancement of the Mars-van Krevelen reaction on oxygen defective Cu/CeO2 surfaces

被引:4
作者
Koizumi, Kenichi [1 ,2 ]
Nobusada, Katsuyuki [1 ,2 ]
Boero, Mauro [3 ,4 ]
机构
[1] Inst Mol Sci, Dept Theoret & Computat Mol Sci, Okazaki, Aichi 4448585, Japan
[2] Kyoto Univ, ESICB, Kyoto 6158520, Japan
[3] Univ Strasbourg, Inst Phys & Chim Mat Strasbourg, UMR 7504, 23 Rue Loess, F-67034 Strasbourg, France
[4] CNRS, 23 Rue Loess, F-67034 Strasbourg, France
关键词
SPACE GAUSSIAN PSEUDOPOTENTIALS; DENSITY-FUNCTIONAL THEORY; MOLECULAR-DYNAMICS; ELECTRONIC-STRUCTURE; NO DECOMPOSITION; CO OXIDATION; SIMULATIONS; TEMPERATURE; CATALYSTS; OXIDE;
D O I
10.1039/c6cp03880h
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We report a detailed first-principles analysis of the electronic structures of oxygen defective CeO2 and Cu/CeO2 surfaces aimed at elucidating the disappearance of the gap state of defective CeO2 when a Cu atom is added at the surface. The top of the valence band of Cu/CeO2 originates from the O 2p states around this Cu atom. We show that this redistribution of electronic states at the defective Cu/CeO2 surface enhances the reactivity of the surface O atoms. Indeed, dynamical simulations show an acceleration of catalytic NO oxidation occurring via the Mars-van Krevelen mechanism mediated by these highly reactive oxygens.
引用
收藏
页码:20708 / 20712
页数:5
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