Sulfur and temperature effects on the spatial distribution of reactions inside a lean NOx trap and resulting changes in global performance

作者: Jae-Soon Choi , William P. Partridge , Josh A. Pihl , C. Stuart Daw

DOI: 10.1016/J.CATTOD.2008.01.008

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摘要: Abstract We experimentally studied the influence of temperature and sulfur loading on axial distribution reactions inside a commercial lean NOx trap (LNT) catalyst to better understand global performance trends. Our measurements were made monolith core, bench-flow reactor under cycling conditions (60-s lean/5-s rich) at 200, 325, 400 °C with intra-catalyst reactor-outlet gas speciation. Postmortem elemental diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) analyses also supplemented our species measurements. For unsulfated catalyst, storage/reduction (NSR) localized in front (upstream) portion monolith, whereas oxygen distributed more evenly along entire length. As result, two axially distinct reaction zones developed working catalyst: an upstream “NSR zone” where both took place downstream storage capacity (OSC)-only zone NSR did not penetrate. The involved less than half LNT 325 400 °C, but it included almost length 200 °C. Sulfation poisoned OSC beginning edge, degradation occurring rapidly distinctly OSC. sulfation proceeded, third (the sulfated zone) moved downstream, concomitant decrease OSC-only conversion. impact conversion was greatest 200 °C, when largest. Ammonia selectivity increased sulfation, which we attributed shortened resultantly reduced consumption NH3, slipping from zone, by Lower temperatures NH3 selectivity. Nitrous oxide decreasing showed little dependence sulfation. proposed explanations for these trends N2O based shifts competing rates three zones.

参考文章(27)
C Courson, A Khalfi, H Mahzoul, S Hodjati, N Moral, A Kiennemann, P Gilot, Experimental study of the SO2 removal over a NOx trap catalyst Catalysis Communications. ,vol. 3, pp. 471- 477 ,(2002) , 10.1016/S1566-7367(02)00180-2
A LINDHOLM, N CURRIER, E FRIDELL, A YEZERETS, L OLSSON, NOx storage and reduction over Pt based catalysts with hydrogen as the reducing agent: Influence of H2O and CO2 Applied Catalysis B-environmental. ,vol. 75, pp. 78- 87 ,(2007) , 10.1016/J.APCATB.2007.03.008
L CUMARANATUNGE, S MULLA, A YEZERETS, N CURRIER, W DELGASS, F RIBEIRO, Ammonia is a hydrogen carrier in the regeneration of Pt/BaO/Al2O3 NOx traps with H2 Journal of Catalysis. ,vol. 246, pp. 29- 34 ,(2007) , 10.1016/J.JCAT.2006.11.008
William S. Epling, Aleksey Yezerets, Neal W. Currier, The effect of exothermic reactions during regeneration on the NOx trapping efficiency of a NOx storage/reduction catalyst Catalysis Letters. ,vol. 110, pp. 143- 148 ,(2006) , 10.1007/S10562-006-0102-2
Jae-Soon Choi, William P. Partridge, C. Stuart Daw, Sulfur impact on NOx storage, oxygen storage, and ammonia breakthrough during cyclic lean/rich operation of a commercial lean NOx trap Applied Catalysis B-environmental. ,vol. 77, pp. 145- 156 ,(2007) , 10.1016/J.APCATB.2007.07.025
Isabella Nova, Lidia Castoldi, Luca Lietti, Enrico Tronconi, Pio Forzatti, How to control the selectivity in the reduction of NOx with H2 over Pt-Ba/Al2O3 Lean NOx Trap catalysts Topics in Catalysis. ,vol. 42, pp. 21- 25 ,(2007) , 10.1007/S11244-007-0144-8
Stephen Poulston, Raj R. Rajaram, Regeneration of NOx trap catalysts Catalysis Today. ,vol. 81, pp. 603- 610 ,(2003) , 10.1016/S0920-5861(03)00158-5
Todd J. Toops, D. Barton Smith, William P. Partridge, NOx adsorption on Pt/K/Al2O3 Catalysis Today. ,vol. 114, pp. 112- 124 ,(2006) , 10.1016/J.CATTOD.2006.02.006
L. Castoldi, I. Nova, L. Lietti, P. Forzatti, STUDY OF THE EFFECT OF BA LOADING FOR CATALYTIC ACTIVITY OF PT–BA/AL2O3 MODEL CATALYSTS Catalysis Today. ,vol. 96, pp. 43- 52 ,(2004) , 10.1016/J.CATTOD.2004.05.006
H ABDULHAMID, E FRIDELL, J DAWODY, M SKOGLUNDH, In situ FTIR study of SO2 interaction with Pt/BaCO3/Al2O3 NOx storage catalysts under lean and rich conditions Journal of Catalysis. ,vol. 241, pp. 200- 210 ,(2006) , 10.1016/J.JCAT.2006.04.034