Flame-made Pt-Ba/Al2O3 catalysts:: Structural properties and behavior in lean-NOx storage-reduction

被引:70
|
作者
Piacentini, M.
Strobel, R.
Maciejewski, M.
Pratsinis, S. E.
Baiker, A. [1 ]
机构
[1] ETH, Dept Chem & Appl Biosci, Inst Chem & Bioengn, Honggerberg HCI, CH-8093 Zurich, Switzerland
[2] ETH, Dept Mech & Proc Engn, Particle Technol Lab, CH-8092 Zurich, Switzerland
关键词
NOx storage-reduction; Pt-Ba/Al2O3; effect of Ba loading; stability of Ba-containing phases; pulse thermal analysis; temperature programmed reaction-desorption; barium carbonate; barium nitrate; flame spray pyrolysis; two-nozzle system;
D O I
10.1016/j.jcat.2006.07.005
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
A series of Pt-Ba/Al2O3 catalysts with Ba loadings in the range of 4.5-33 wt% was prepared using a two-nozzle flame spray pyrolysis method. The structural properties and activities of these catalysts in NOx storage-reduction (NSR) were compared to corresponding standard Pt-Ba/Al2O3 catalysts prepared conventionally via wet impregnation. The catalysts were characterized by XRD, TEM, ESI, DRIFT, TG-MS, TPRD, and gas adsorption. Calcined flame-derived catalysts were composed of agglomerated spherical nanoparticles of alumina and Pt/barium carbonate of low thermal stability (LT-BaCO3), whereas barium carbonate of high stability (HT BaCO3) was absent. In contrast, in the corresponding conventionally prepared catalysts, the Ba-containing phases were composed of BaO, LT-BaCO3, and HT-BaCO3. DRIFTS measurements of CO adsorption revealed distinct differences in the distribution of CO chemisorbing sites on Pt particles depending on the preparation method applied. The CO:Pt ratio varied between 0.8 and 0.7 depending on the Ba loading and the preparation method. Decreased Pt dispersion at higher Ba loadings was observed for the wet-impregnated catalysts, whereas Pt dispersion increased only slightly at higher Ba loadings for the flame-made catalysts. The structural differences of flame-made and conventionally prepared catalysts affected strongly their NO, storage efficiency. Investigation of the behavior of the catalysts in NSR showed that the larger Ba/Al2O3 interface existing in conventionally prepared catalysts results in a higher NOx storage efficiency of these catalysts at Ba loadings up to ca. 17 wt%, whereas the absence of the HT-BaCO3 phase in flame-made catalysts lead to improved NOx storage potential at higher Ba loadings. (c) 2006 Elsevier Inc. All rights reserved.
引用
收藏
页码:43 / 56
页数:14
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