Stabilization of active Rh2O3 species for catalytic decomposition of N2O on La-, Pr-doped CeO2

被引:121
作者
Bueno-Lopez, A. [1 ]
Such-Basanez, I. [1 ]
Salinas-Martinez de Lecea, C. [1 ]
机构
[1] Univ Alicante, Dept Inorgan Chem, E-03080 Alicante, Spain
关键词
N2O decomposition; rhodium catalyst; Rh2O3; ceria support; lanthanum; praseodymium doping; solid solution; in situ XPS;
D O I
10.1016/j.jcat.2006.08.021
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
CeO2 and La- or Pr-doped CeO2 were prepared at calcination temperatures of 600, 800, and 1000 degrees C. The samples were characterized by Raman, XRD, and N-2 adsorption and tested as Rh2O3 support for the catalytic decomposition of N2O at low temperature (starting at 200 degrees C). Catalyst characterization was done by XPS analysis of fresh and in situ treated catalysts, TPR, and TEM. As deduced by XPS analysis and catalytic tests, Rh2O3 is more active than Rho for N2O decomposition. Pure CeO2 calcined at low temperature (600 'Q and La or Pr-doped CeO2 calcined at 600, 800 or 1000 degrees C can keep Rh2O3 stable under reaction conditions. In contrast, Rh2O3 supported on pure CeO2 calcined at high temperature (800 or 1000 degrees C) is reduced to Rho under reaction conditions. The redox properties of the support are decisive forRh(2)O(3) stabilization and catalytic performance; the larger the reducible surface CeO2 (determined by TPR), the better the catalytic activity. In addition, structural and textural features of the support (crystallinity, BET surface area, and particle size) affect Rh2O3 dispersion, the smaller the support particle size (the higher the surface area), the better the dispersion and the catalytic activity. The redox properties and particle size of supports depend on calcination temperature. Doping improves thermal stability with regard to pure CeO2. La and Pr form solid solutions with CeO2, preventing sintering and maintaining a high percentage of reducible CeO2 at high calcination temperatures (800 and 1000 'Q. (c) 2006 Elsevier Inc. All rights reserved.
引用
收藏
页码:102 / 112
页数:11
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