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
相关论文
共 48 条
[1]   Role of Pt in Pt/Ba/Al2O3 NOx storage and reduction traps [J].
Anderson, JA ;
Bachiller-Baeza, B ;
Fernández-García, M .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2003, 5 (20) :4418-4427
[2]   THE DETERMINATION OF PORE VOLUME AND AREA DISTRIBUTIONS IN POROUS SUBSTANCES .1. COMPUTATIONS FROM NITROGEN ISOTHERMS [J].
BARRETT, EP ;
JOYNER, LG ;
HALENDA, PP .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1951, 73 (01) :373-380
[3]   Removal of nitrogen oxides from the exhaust of a lean-tune gasoline engine [J].
Bogner, W ;
Kramer, M ;
Krutzsch, B ;
Pischinger, S ;
Voigtlander, D ;
Wenninger, G ;
Wirbeleit, F ;
Brogan, MS ;
Brisley, RJ ;
Webster, DE .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1995, 7 (1-2) :153-171
[4]   Heats of adsorption of the linear CO species adsorbed on a Pt/Al2O3 catalyst in the presence of coadsorbed species using FTIR spectroscopy [J].
Bourane, A ;
Dulaurent, O ;
Bianchi, D .
LANGMUIR, 2001, 17 (18) :5496-5502
[5]   Heats of adsorption of linear and multibound adsorbed CO species on a Pt/Al2O3 catalyst using in Situ infrared spectroscopy under adsorption equilibrium [J].
Bourane, A ;
Dulaurent, O ;
Bianchi, D .
JOURNAL OF CATALYSIS, 2000, 196 (01) :115-125
[6]   A review of the selective reduction of NOx, with hydrocarbons under lean-burn conditions with non-zeolitic oxide and platinum group metal catalysts [J].
Burch, R ;
Breen, JP ;
Meunier, FC .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2002, 39 (04) :283-303
[7]   Study of the effect of Ba loading for catalytic activity of Pt-Ba/Al2O3 model catalysts [J].
Castoldi, L ;
Nova, I ;
Lietti, L ;
Forzatti, P .
CATALYSIS TODAY, 2004, 96 (1-2) :43-52
[8]  
CHEN X, 2005, APPL CATAL B-ENVIRON, V61, P189
[9]   Platinum dispersion measurements for Pt/BaO/Al2O3, NOx storage catalysts [J].
Dawody, J ;
Eurenius, L ;
Abdulhamid, H ;
Skoglundh, M ;
Olsson, E ;
Fridell, E .
APPLIED CATALYSIS A-GENERAL, 2005, 296 (02) :157-168
[10]   Fundamental investigations of thermal aging phenomena of model NOx storage systems [J].
Eberhardt, M ;
Riedel, R ;
Göbel, U ;
Theis, J ;
Lox, ES .
TOPICS IN CATALYSIS, 2004, 30-1 (1-4) :135-142