New insight into the interaction of sulfur with diesel NOx storage catalysts

Rohr, F.; Göbel, U.; Kattwinkel, Peter; Kreuzer, Thomas; Müller, W.; Philipp, S.; Gélin, P.

doi:10.1016/j.apcatb.2005.12.033

Cited by 31 publications

(15 citation statements)

References 13 publications

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“…A drawback to this system is the catalyst deactivation, mainly due to (i) sulfur poisoning [1,2] even if the sulfur content in fuels is lowered and (ii) thermal aging [3]. Another problem arises from ammonia emissions.…”

Section: Introductionmentioning

confidence: 99%

Influence of Mn and Fe Addition on the NO x Storage–Reduction Properties and SO2 Poisoning of a Pt/Ba/Al2O3 Model Catalyst

Corbos

Courtois

et al. 2009

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This work deals with the effect of Mn or Fe addition on the NO x storage-reduction properties of a Pt/Ba/Al 2 O 3 model catalyst. NO x storage capacity, SO 2 poisoning and regeneration and NO x removal efficiency under rich/lean cycling conditions are studied. Fe addition to Pt/Ba/Al 2 O 3 leads only to a small increase of NO x storage capacity, and more interestingly, to a better sulfur removal due to the inhibition of bulk barium sulfate formation. Unfortunately, the NO x storage property cannot be fully recovered. Moreover, Fe addition results in a decrease in the NO x removal efficiency. Mn addition also improves the NO x storage capacity, but no significant influence on the sulfur elimination is observed. Mn-doped catalyst does not improve the NO x removal efficiency, but NH 3 selectivity is found to drastically decrease at 400°C, from 20 to 3%. In addition, the NO x conversion can be improved at higher H 2 concentration in the rich pulse, always keeping NH 3 selectivity at low level.

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Section: Introductionmentioning

confidence: 99%

Influence of Mn and Fe Addition on the NO x Storage–Reduction Properties and SO2 Poisoning of a Pt/Ba/Al2O3 Model Catalyst

Corbos

Courtois

et al. 2009

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“…Although first commercial applications for spark-ignition engines have been successful and applications for diesel engines are planned, today's NSR catalysts still suffer from numerous shortcomings. These include for example the limited possibilities of tuning the temperature windows for NO x storage and release, the low storage efficiency, the limited thermal stability of the NSR catalysts, as well as deactivation and poisoning [9].…”

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confidence: 99%

Strong Size Effects in Supported Ionic Nanoparticles: Tailoring the Stability of NO x Storage Catalysts

et al. 2007

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Based on a well-defined model-catalyst approach, we study the particle size dependent properties of NO x storage materials. The single-crystal based model systems are prepared on an ordered Al 2 O 3 film, on which BaO nanoparticles are grown under ultrahigh-vacuum (UVH) conditions. Particle size and density are characterized by scanning tunneling microscopy (STM). The interaction with NO 2 is probed by molecular beam (MB) methods in combination with time-resolved IR reflection absorption spectroscopy (TR-IRAS). It is found that both, the stability and the formation kinetics of alumina supported barium nitrate nanoparticles show a strong dependence on particle size. Very small BaO particles are rapidly converted into nitrates, however, the resulting aggregates exhibit a strongly reduced thermal stability. Surface and bulk nitrate and nitrate features are identified by means of vibrational spectroscopy. It is concluded that the size dependencies are related to the formation and decomposition of surface-related BaNO x species the decomposition temperature of which can be tuned over an exceptionally large temperature interval. It is suggested that the stability of these surface NO x species is strongly modified by the underlying support.

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“…As seen from Figure 5, SO 3 desorption starts from 800°C, a temperature slightly higher than typical desulfation temperatures for Pt/Rh/BaO/CeO 2 /Al 2 O 3 catalysts [15]. A higher desulfation temperature can be expected given the fact that synergic effects between noble metal and storage material may facilitate thermal decomposition of BaSO 4 [16].…”

Section: Bulk Bao 67%mentioning

confidence: 93%

“…Desulfation of the accumulated SO x involves heating the catalyst to the temperature above 700°C or switching to a reducing atmosphere (CO or H 2 ) [12][13][14][15][16]. The main issue for the high-temperature desulfation is the loss of the catalytic activity caused by thermal aging (precious metal sintering and formation of BaAl 2 O 4 [17]).…”

Section: Introductionmentioning

confidence: 99%

Sulfur Deactivation of NO_xStorage Catalysts: A Multiscale Modeling Approach

Rankovic

Chizallet

Nicolle

et al. 2013

Oil Gas Sci. Technol. – Rev. IFP Energies nouvelles

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Re´sume´-Empoisonnement des mate´riaux de stockage des NO x par le soufre : approche multi-e´chelles -Les pie`ges a`NO x repre´sentent une technologie prometteuse pour la re´duction des e´missions d'oxydes d'azote issus des moteurs ope´rant en me´lange pauvre. Leur utilisation est limite´e par la pre´sence de compose´s soufre´s dans les gaz d'e´chappement. Le soufre contenu dans le carburant et le lubrifiant est oxyde´lors de la combustion en SO 2 et SO 3 . Ces oxydes de soufre pre´sentent une forte affinite´pour le mate´riau de stockage du pie`ge, la formation de sulfate e´tant favorise´e thermodynamiquement. Cette formation contribue au blocage des sites d'adsorption des NO x et influence l'ope´ration de l'organe de post-traitement. La mode´lisation mole´culaire repre´sente un outil pre´cieux pour pre´dire le comportement et les performances du syste`me catalytique. Notre e´tude pre´sente une me´thodologie d'exploitation des calculs ab initio pour la formulation de mode`les cine´tiques de´veloppe´s dans la librairie de post-traitement ve´hicule IFP Exhaust. Nous illustrons notre approche par le cas de l'adsorption de SO 3 sur un mate´riau mode`le, BaO. Afin d'obtenir une description fide`le du mate´riau de stockage re´el, l'adsorption de SO 3 est de´crite sur plusieurs sites : terrasses, marches, crans et le site massique. Des analyses de sensibilite´et de vitesses de re´actions permettent d'obtenir une compre´hension plus approfondie des phe´nome`nes d'empoisonnement mis en jeu.Abstract -Sulfur Deactivation of NO x Storage Catalysts: A Multiscale Modeling ApproachLean NO x Trap (LNT) catalysts, a promising solution for reducing the noxious nitrogen oxide emissions from the lean burn and Diesel engines, are technologically limited by the presence of sulfur in the exhaust gas stream. Sulfur stemming from both fuels and lubricating oils is oxidized during the combustion event and mainly exists as SO x (SO 2 and SO 3 ) in the exhaust. Sulfur oxides interact strongly with the NO x trapping material of a LNT to form thermodynamically favored sulfate species, consequently leading to the blockage of NO x sorption sites and altering the catalyst operation. Molecular and kinetic modeling represent a valuable tool for predicting system behavior and evaluating catalytic performances. The present paper demonstrates how fundamental ab initio calculations can be used as a valuable source for designing kinetic models developed in the IFP Exhaust library, intended for vehicle simulations. The concrete example we chose to illustrate our

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New insight into the interaction of sulfur with diesel NOx storage catalysts

Cited by 31 publications

References 13 publications

Influence of Mn and Fe Addition on the NO x Storage–Reduction Properties and SO2 Poisoning of a Pt/Ba/Al2O3 Model Catalyst

Influence of Mn and Fe Addition on the NO x Storage–Reduction Properties and SO2 Poisoning of a Pt/Ba/Al2O3 Model Catalyst

Strong Size Effects in Supported Ionic Nanoparticles: Tailoring the Stability of NO x Storage Catalysts

Sulfur Deactivation of NO_xStorage Catalysts: A Multiscale Modeling Approach

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New insight into the interaction of sulfur with diesel NOx storage catalysts

Cited by 31 publications

References 13 publications

Influence of Mn and Fe Addition on the NO x Storage–Reduction Properties and SO2 Poisoning of a Pt/Ba/Al2O3 Model Catalyst

Influence of Mn and Fe Addition on the NO x Storage–Reduction Properties and SO2 Poisoning of a Pt/Ba/Al2O3 Model Catalyst

Strong Size Effects in Supported Ionic Nanoparticles: Tailoring the Stability of NO x Storage Catalysts

Sulfur Deactivation of NOxStorage Catalysts: A Multiscale Modeling Approach

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Sulfur Deactivation of NO_xStorage Catalysts: A Multiscale Modeling Approach