Comparative study of structural properties and NOx storage-reduction behavior of Pt/Ba/CeO2 and Pt/Ba/Al2O3

被引:37
|
作者
Casapu, A. [1 ]
Grunwaldt, J. -D. [1 ]
Maciejewski, M. [1 ]
Krumeich, F. [1 ]
Baiker, A. [1 ]
Wittrock, M. [2 ]
Eckhoff, S. [2 ]
机构
[1] ETH, Inst Chem & Bioengn, Dept Chem & Appl Biosci, CH-8093 Zurich, Switzerland
[2] Umicore AG & Co KG, D-63403 Hanau, Germany
关键词
NOx storage-reduction catalyst; ceria; pre-treatment; thermal analysis; X-ray absorption spectroscopy;
D O I
10.1016/j.apcatb.2007.09.030
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
Differences in the NOx storage-reduction (NSR) behavior of Pt/Ba/CeO2 and Pt/Ba/Al2O3 have been identified and traced to their different chemical and structural properties. The results show that Pt/Ba/CeO2 exhibits inferior NO, storage and, particularly, reduction (regeneration) activity compared to the Al2O3 supported catalyst. The incomplete reduction of the stored NOx-species in Pt/Ba/CeO2 seems to be caused by a faster and more profound reoxidation of Pt particles during the lean period as evidenced by in situ X-ray absorption spectroscopy. Interestingly, the reduction activity could be significantly improved by a pre-reduction step at mild conditions. Exposure of the Pt/Ba/CeO2 catalyst to reducing H-2 atmosphere in the temperature range 300-500 degrees C lead to a moderate increase of Pt particle size which beneficially influenced the regeneration activity. In contrast, pre-reduction at temperatures above 500 degrees C was unfavorable and resulted in a severe decrease of the regeneration activity, probably due to migration of the partially reduced CeO2 onto the surface of Pt particles. (c) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:288 / 300
页数:13
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