Structure-activity relationships of Pt/Al2O3 catalysts for CO and NO oxidation at diesel exhaust conditions

被引:147
作者
Boubnov, Alexey [2 ,3 ]
Dahl, Soren [1 ]
Johnson, Erik [3 ]
Molina, Anna Puig [2 ]
Simonsen, Soren Bredmose [1 ,2 ]
Cano, Fernando Morales [2 ]
Helveg, Stig [2 ]
Lemus-Yegres, Lived J. [2 ]
Grunwaldt, Jan-Dierk [4 ,5 ]
机构
[1] Tech Univ Denmark, Dept Phys, Ctr Individual Nanoparticle Funct, DK-2800 Lyngby, Denmark
[2] Haldor Topsoe Res Labs, DK-2800 Lyngby, Denmark
[3] Univ Copenhagen, Niels Bohr Inst, Nano Sci Ctr, DK-2100 Copenhagen O, Denmark
[4] Karlsruhe Inst Technol, Inst Catalysis Res & Technol, D-76344 Eggenstein Leopoldshafen, Germany
[5] KIT, Inst Chem Technol & Polymer Chem, D-76131 Karlsruhe, Germany
来源
APPLIED CATALYSIS B-ENVIRONMENTAL | 2012年 / 126卷
关键词
Platinum; Alumina; Particle size; CO oxidation; NO oxidation; Lean burn; Surface oxide; TEM; Chemisorption; In situ XAFS; RAY-ABSORPTION SPECTROSCOPY; CARBON-MONOXIDE; IN-SITU; STRUCTURE SENSITIVITY; ELEMENTARY STEPS; PLATINUM; OXYGEN; SIZE; ADSORPTION; DISPERSION;
D O I
10.1016/j.apcatb.2012.07.029
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070305 [高分子化学与物理];
摘要
Structure-performance relationships for Pt/Al2O3 catalysts with mean Pt particle sizes of 1, 2, 3, 5 and 10 nm are investigated for the catalytic oxidation of CO and NO under lean-burning diesel exhaust conditions. The most active catalysts for CO oxidation exhibit Pt particles of 2-3 nm, having a large fraction of low-coordinated and reactive surface Pt atoms. Exploiting in situ XAFS, we find that a reversible Pt surface oxidation is connected to high CO conversion. NO oxidation is most efficient over the catalysts with the largest Pt particles mainly exhibiting surface Pt atoms on planar facets. An irreversible Pt oxide formation observed during NO oxidation is a possible deactivation route and we suggest that the most active sites for NO oxidation are the ones least prone to surface oxidation. When both CO and NO are present in the reaction mixture, activity is increased for both reactions, suggesting that CO oxidation actively regenerates the Pt surface for NO oxidation and vice versa. The effect is strongest for the NO oxidation activity. (C) 2012 Elsevier B.V. All rights reserved.
引用
收藏
页码:315 / 325
页数:11
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