Carbonate formation and stability on a Pt/BaO/γ-Al2O3 NOX storage/reduction catalyst

被引:49
作者
Epling, William S. [1 ]
Peden, Charles H. F.
Szanyi, Janos
机构
[1] Univ Waterloo, Dept Chem Engn, Waterloo, ON N2L 3G1, Canada
[2] Pacific NW Natl Lab, Inst Interfacial Catalysis, Richland, WA 99352 USA
关键词
D O I
10.1021/jp712180q
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
There has been recent debate regarding the role or influence of BaCO3 species on the performance or operation of Pt/BaO/Al2O3 model NOX storage/reduction (NSR) catalysts. This influence is primarily regarded as negative, but the extent of its impact is not clear. For this reason, the formation and stability of barium carbonate species on a Pt/BaO/Al2O3 model NSR catalyst were characterized using Fourier transform infrared (FTIR) spectroscopy. The catalyst sample was exposed to CO2, CO, and CO + O-2 at various temperatures, from 300 to >500 K. Bidentate carbonate species readily form under all conditions, while at higher temperatures, unidentate species were also observed and likely formed from bidentate species as a result of a change in their coordination to the oxide surface. Reaction of COX species with residual hydroxide species on the catalyst led to the formation of bicarbonates, and when the sample was exposed to CO at low temperature, formate species were also formed. These formate species decomposed at elevated temperatures and contributed to the formation of carbonates. H2O exposure resulted in the agglomeration of various COX-containing phases to larger particles.
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收藏
页码:10952 / 10959
页数:8
相关论文
共 43 条
[1]   NOx release from a noble metal/BaO catalyst:: dependence on gas composition [J].
Amberntsson, A ;
Persson, H ;
Engström, P ;
Kasemo, B .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2001, 31 (01) :27-38
[3]   Influence of CO2 on storage and release of NOx on barium-containing catalyst [J].
Balcon, S ;
Potvin, C ;
Salin, L ;
Tempère, JF ;
Djéga-Mariadassou, G .
CATALYSIS LETTERS, 1999, 60 (1-2) :39-43
[4]   IR-SPECTROSCOPIC DETECTION OF LEWIS ACID SITES ON AL2O3 USING ADSORBED CO - CORRELATION WITH AL-OH GROUP REMOVAL [J].
BALLINGER, TH ;
YATES, JT .
LANGMUIR, 1991, 7 (12) :3041-3045
[5]   FTIR Spectroscopy combined with isotope labeling and quantum chemical calculations to investigate adsorbed bicarbonate formation following reaction of carbon dioxide with surface hydroxyl groups on Fe2O3 and Al2O3 [J].
Baltrusaitis, J ;
Jensen, JH ;
Grassian, VH .
JOURNAL OF PHYSICAL CHEMISTRY B, 2006, 110 (24) :12005-12016
[6]  
Broqvist P, 2005, J PHYS CHEM B, V109, P9613, DOI 10.1021/jp0503841
[7]   INFRARED SPECTROSCOPIC IDENTIFICATION OF SPECIES ARISING FROM REACTIVE ADSORPTION OF CARBON OXIDES ON METAL-OXIDE SURFACES [J].
BUSCA, G ;
LORENZELLI, V .
MATERIALS CHEMISTRY, 1982, 7 (01) :89-126
[8]   The effect of water and reductants on the release of nitrogen oxides stored on BaO/Al2O3 [J].
Cant, NW ;
Patterson, MJ .
CATALYSIS LETTERS, 2003, 85 (3-4) :153-157
[9]   Overview of the fundamental reactions and degradation mechanisms of NOx storage/reduction catalysts [J].
Epling, WS ;
Campbell, LE ;
Yezerets, A ;
Currier, NW ;
Parks, JE .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2004, 46 (02) :163-245
[10]   The effects of CO2 and H2O on the NOx destruction performance of a model NOx storage/reduction catalyst [J].
Epling, WS ;
Campbell, GC ;
Parks, JE .
CATALYSIS LETTERS, 2003, 90 (1-2) :45-56