Elementary steps of NOx adsorption and surface reaction on a commercial storage-reduction catalyst

被引:256
作者
Sedlmair, C
Seshan, K
Jentys, A
Lercher, JA
机构
[1] Tech Univ Munich, Inst Tech Chem 2, D-85747 Garching, Germany
[2] Univ Twente, Fac Chem Technol, NL-7500 AE Enschede, Netherlands
关键词
nitrates; nitrites; in situ FFIR spectroscopy; NOx storage; adsorption; barium-oxide; mechanism;
D O I
10.1016/S0021-9517(02)00085-4
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
The surface species formed during adsorption of NOx on a commercial NSR catalyst (containing barium oxide, Pt, and alumina as the main components) were investigated by in situ IR spectroscopy. During adsorption of NO, mainly linear and bridged bonded nitrites of Ba-O-NO-Ba type were formed on Al and Ba oxide components. Nitrites were detected during the initial phase of the NO/O-2 and NO2 adsorption, whereas with further exposure nitrates were the dominant surface species. Using the different surface species and reaction intermediates identified by IR spectroscopy a series of sequential reaction steps during the sorption of NOx on a NSR catalyst was derived. Initially, NO is stored in the form of nitrites on the storage component (Ba oxide). NO2 formed by oxidation on the noble metal component (Pt) sorbs either molecularly by forming nitrate species or dissociatively by forming nitrites. After a certain concentration of NOx is adsorbed, the transformation and further oxidation of the surface nitrites into surface nitrates by NO2 Occur. The stability of the NO, surface species was found to increase in the order Al nitrites < Ba nitrites < Al nitrates < Ba nitrates. (C) 2003 Elsevier Science (USA). All rights reserved.
引用
收藏
页码:308 / 316
页数:9
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