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

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2016年 / 18卷 / 30期

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

页码：20708 / 20712

页数：5

共 43 条

[1] BAND THEORY AND MOTT INSULATORS - HUBBARD-U INSTEAD OF STONER-I [J].