Unravelling the Different Reaction Pathways for Low Temperature CO Oxidation on Pt/CeO2 and Pt/Al2O3 by Spatially Resolved Structure-Activity Correlations

被引：68
作者：
Gaenzler, Andreas M. [1 ]
Casapu, Maria [1 ]
Doronkin, Dmitry E. [1 ,2 ]
Maurer, Florian [1 ]
Lott, Patrick [1 ]
Glatzel, Pieter [3 ]
Votsmeier, Martin [4 ]
Deutschmann, Olaf [1 ,2 ]
Grunwaldt, Jan-Dierk [1 ,2 ]
机构：
[1] KIT, Inst Chem Technol & Polymer Chem ITCP, Engesserstr 20, D-76131 Karlsruhe, Germany
[2] KIT, Inst Catalysis Res & Technol IKFT, Hermann von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany
[3] European Synchrotron Radiat Facil, 71 Ave Martyrs,CS 40220, F-38000 Grenoble 9, France
[4] Umicore AG & Co KG, Rodenbacher Chaussee 4, D-63457 Hanau, Germany
来源：
JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2019年 / 10卷 / 24期
关键词：
RAY-ABSORPTION SPECTROSCOPY; SELECTIVE CATALYTIC-REDUCTION; METAL-SUPPORT INTERACTION; IN-SITU; CARBON-MONOXIDE; OXIDE INTERFACES; HERFD-XANES; PLATINUM; TIME; RESOLUTION;
D O I：
10.1021/acs.jpclett.9b02768
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：
Spatially resolved operando HERFD-XANES (high energy resolution fluorescence detected X-ray absorption near edge structure) complemented by CO concentration gradient profiles along the catalyst bed (SpaciPro) was used to identify the dominant reaction paths for the low and high temperature CO oxidation on Pt/CeO2 and Pt/Al2O3. At low temperatures, features associated with CO adsorption on Pt were found for both catalysts. During the oxidation reaction light-off, the evolution of the spectral and catalytic profile diverged along the catalyst bed. The CO oxidation rate was high on Pt/CeO2 from the beginning of the catalyst bed with CO being adsorbed on Pt, whereas low CO conversion due to strong CO poisoning was found on Pt/Al2O3. This correlation of the CO concentration gradient with unique insight by HERFD-XANES gave direct proof of the crucial contribution of the Pt-CeO2 perimeter sites overcoming the CO self-inhibition effect at low temperatures.
引用
收藏
页码：7698 / 7705
页数：15
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