Principles of Heterogeneous Catalysis

Dumesic, James A.; Huber, George W.; Boudart, M.

doi:10.1002/9783527610044.hetcat0001

Cited by 133 publications

(174 citation statements)

References 78 publications

(79 reference statements)

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“…In the catalysis field, the mean field approximation is often used to describe an ensemble of molecules and translate microscopic processes with continuum variables such as surface coverage and temperature [55]. Splitting the overall reaction in its individual steps, and modeling the rate of these steps individually yields a so called microkinetic [56] or adsorption-desorption model. Adsorption-desorption models are commonly used to make simulation studies of catalytic reactions under periodic operation [57].…”

Section: Modeling Pulsed Activationmentioning

confidence: 99%

“…This means the time constants associated with temperature pulses are in the order of 10µs. The kinetic parameters used in microkinetic models for each of the surface reactions [56] suggest that the dynamics of surface processes are in the order of 0.1 − 1 ns. Therefore, it may be expected that the temperature pulses created in the setup are relatively slow as compared to surface dynamics.…”

Section: Time Scales Of Pulsed Activation and Catalysismentioning

confidence: 99%

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Pulsed activation in heterogeneous catalysis

Stolte¹,

Özkan²,

Thüne³

et al. 2013

Applied Thermal Engineering

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Section: Modeling Pulsed Activationmentioning

confidence: 99%

Section: Time Scales Of Pulsed Activation and Catalysismentioning

confidence: 99%

Pulsed activation in heterogeneous catalysis

Stolte¹,

Özkan²,

Thüne³

et al. 2013

Applied Thermal Engineering

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“…First parameters that we discuss are the pre-exponential factors used for the global simulation. Surface adsorptions are modeled with a pre-exponential factor of 1:0 Â 10 6 s À1 , corresponding to a typical transition state theory-based value for an immobile precursor molecular adsorption [42]. The pre-exponential factor for adsorption on bulk BaO sites of 1:0 Â 10 7 s À1 was based on a typical value for a mobile precursor mediated adsorption, knowing that the formation of bulk sulfate commences with a surface adsorption, and therefore requires the molecule to diffuse into deeper layers.…”

Section: Kinetic Studymentioning

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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“…The overall approach for surface reaction mechanism development was derived from microkinetic modeling concepts proposed by Dumesic and colleagues in the early 1990s [56], which was further extended by various researchers through hierarchical multiscale modeling [13][14][15][16][17]. Microkinetic modeling has been applied in the past for a variety of chemical processes such as methane partial oxidation and reforming [14,57,58], selective catalytic reduction of NO x [59,60], NO oxidation [61], ammonia decomposition [13,62], ethylene hydrogenation [63], and Water-Gas Shift [64][65][66], to name a few recent applications.…”

Section: Chapter 3: Surface Reaction Mechanism Developmentmentioning

confidence: 99%

Microkinetic modeling and analysis of ethanol partial oxidation and reforming reaction pathways on platinum at short contact times

Koehle

Mhadeshwar

2012

Chemical Engineering Science

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2013iii ACKNOWLDGEMENTSThere are many people without whom this thesis would not have been possible. I must thank Ashish Mhadeshwar for the incredible amount of knowledge he imparted and the guidance he provided in order for this research to be conducted, shared at conferences and published. Many thanks to Doug Cooper, Bill Mustain and Ranjan Srivastava for standing in as advisors and providing support that was above and beyond expectations. I want to thank everyone that has become part of my UConn family, without whom this project would have been possible but much less fun:

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Principles of Heterogeneous Catalysis

Abstract: The sections in this article are Introduction Definitions of Catalysis and Turnover Steps in a Heterogeneous Catalytic Reaction Desired Characteristics of a Catalyst Reaction Schemes and Adsorbed Species Conditions for Catalyst Optimality Catalyst Design … Show more

Cited by 133 publications

References 78 publications

Pulsed activation in heterogeneous catalysis

Pulsed activation in heterogeneous catalysis

Sulfur Deactivation of NO_xStorage Catalysts: A Multiscale Modeling Approach

Microkinetic modeling and analysis of ethanol partial oxidation and reforming reaction pathways on platinum at short contact times

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Principles of Heterogeneous Catalysis

Abstract: The sections in this article are Introduction Definitions of Catalysis and Turnover Steps in a Heterogeneous Catalytic Reaction Desired Characteristics of a Catalyst Reaction Schemes and Adsorbed Species Conditions for Catalyst Optimality Catalyst Design … Show more

Cited by 133 publications

References 78 publications

Pulsed activation in heterogeneous catalysis

Pulsed activation in heterogeneous catalysis

Sulfur Deactivation of NOxStorage Catalysts: A Multiscale Modeling Approach

Microkinetic modeling and analysis of ethanol partial oxidation and reforming reaction pathways on platinum at short contact times

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Product

Resources

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Sulfur Deactivation of NO_xStorage Catalysts: A Multiscale Modeling Approach