Influence of Ceria on the NOx Storage/Reduction Behavior of Lean NOx Trap Catalysts

The effect of La 2 O 3 -stabilized ceria incorporation on the functioning of fully formulated lean NO x trap catalysts was investigated. Monolithic catalysts were prepared, corresponding to loadings of 0, 50 and 100 g CeO 2 /L, together with a catalyst containing 100 g/L of ceria-zirconia (Ce 0.7 Zr 0.3 O 2 ). Loadings of the other main components (Pt, Rh and BaO) were held constant. Catalyst evaluation was performed on a bench flow reactor under simulated diesel exhaust conditions, employing NO x storage/reduction cycles. NO x storage efficiency in the temperature range 150-350 °C was observed to increase with ceria loading, resulting in higher NO x conversion levels. At 150 °C, high rich phase NO x slip was observed for all of the catalysts, resulting from an imbalance in the rates of nitrate decomposition and NO x reduction. Optimal NO x conversion was obtained in the range 250-350 °C for all the catalysts, while at 450 °C high rich phase NO x slip from the most highly loaded ceria-containing catalyst resulted in lower NO x conversion than for the ceria-free formulation. N 2 O was the major NO x reduction product at 150 °C over all of the catalysts, although low NO x conversion levels limited the N 2 O yield. At higher temperatures N 2 was the main product of NO x reduction, although NH 3 formation was also observed. Selectivity to NH 3 decreased with increasing ceria loading, indicating that NH 3 is consumed by reaction with stored oxygen in the rear of the catalyst.

[1]  Pio Forzatti,et al.  STUDY OF THE EFFECT OF BA LOADING FOR CATALYTIC ACTIVITY OF PT–BA/AL2O3 MODEL CATALYSTS , 2004 .

[2]  Jae-Soon Choi,et al.  Intra-channel evolution of carbon monoxide and its implication on the regeneration of a monolithic Pt/K/Al2O3 NOx storage-reduction catalyst , 2006 .

[3]  Russell G. Tonkyn,et al.  Nitrogen release from a NOx storage and reduction catalyst , 2006 .

[4]  W. Epling,et al.  The effects of regeneration conditions on NOX and NH3 release from NOX storage/reduction catalysts , 2007 .

[5]  D. Duprez,et al.  NOx storage capacity, SO2 resistance and regeneration of Pt/(Ba)/CeZr model catalysts for NOx-trap system , 2007 .

[6]  R. Riedel,et al.  Fundamental investigations of thermal aging phenomena of model NOx storage systems , 2004 .

[7]  R. Gorte,et al.  A calorimetric study of oxygen-storage in Pd/ceria and Pd/ceria–zirconia catalysts , 2001 .

[8]  A. Baiker,et al.  NOx storage-reduction behavior of Pt–Ba/MO2 (MO2 = SiO2, CeO2, ZrO2) catalysts , 2007 .

[9]  J. Kašpar,et al.  Modification of the Redox Behaviour of CeO2Induced by Structural Doping with ZrO2 , 1996 .

[10]  J. Hanson,et al.  Reduction of stored NOx on Pt/Al2O3 and Pt/BaO/Al2O3 catalysts with H2 and CO , 2006 .

[11]  Todd J. Toops,et al.  Effect of Ceria on the Storage and Regeneration Behavior of a Model Lean NOx Trap Catalyst , 2007 .

[12]  H. Vogel,et al.  IR-study of formation of nitrite and nitrate during NOx-adsorption on NSR-catalysts-compounds CeO2 and BaO/CeO2 , 2007 .

[13]  C. Pitois,et al.  Rare earths based oxides as alternative materials to Ba in NOx-trap catalysts , 2007 .

[14]  H. Vogel,et al.  Investigation of NO adsorption and NO/O2 co-adsorption on NOx-storage-components by DRIFT-spectroscopy , 2004 .

[15]  R. Cataluña,et al.  NO reaction at surface oxygen vacancies generated in cerium oxide , 1995 .

[16]  H. Hamada,et al.  CeO2–ZrO2 binary oxides for NOx removal by sorption , 2001 .

[17]  W. Schneider,et al.  Thermal decomposition of dispersed and bulk-like NOx species in model NOx trap materials , 2005 .

[18]  Todd J. Toops,et al.  A kinetic and DRIFTS study of supported Pt catalysts for NO oxidation , 2006 .

[19]  Jae-Soon Choi,et al.  Spatially resolved in situ measurements of transient species breakthrough during cyclic, low-temperature regeneration of a monolithic Pt/K/Al2O3 NOx storage-reduction catalyst , 2005 .

[20]  Neal W. Currier,et al.  Ammonia is a hydrogen carrier in the regeneration of Pt/BaO/Al2O3 NOx traps with H2 , 2007 .

[21]  G. Eigenberger,et al.  Experimental results concerning the role of Pt, Rh, Ba, Ce and Al2O3 on NOx-storage catalyst behaviour , 2007 .

[22]  J. Grunwaldt,et al.  Formation and stability of barium aluminate and cerate in NOx storage-reduction catalysts , 2006 .

[23]  Carla E. Hori,et al.  Thermal stability of oxygen storage properties in a mixed CeO2-ZrO2 system , 1998 .

[24]  Sara U Erkfeldt,et al.  Influence of the storage material on the storage of NOx at low temperatures , 2004 .

[25]  Gary Jacobs,et al.  Low temperature water–gas shift: in situ DRIFTS-reaction study of ceria surface area on the evolution of formates on Pt/CeO2 fuel processing catalysts for fuel cell applications , 2003 .

[26]  Robert J. Farrauto,et al.  Kinetics of the water-gas shift reaction on Pt catalysts supported on alumina and ceria , 2007 .