Kinetic Modeling of the Oxidative Coupling of Methane

Simon, Yves; Baronnet, F.; Marquaire, Paul-Marie

doi:10.1021/ie060151w

Cited by 46 publications

(21 citation statements)

References 53 publications

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“…With simultaneous concentration analysis of the gas‐phase components by SVUV‐PIMS, the concentrations of gas‐phase methyl radical, ethylene and ethane were found to vary in the same trend that they simultaneously increase with the reaction temperature (Figure B). These results suggest that ethylene and ethane should be the products of secondary reactions of gas‐phase methyl radicals, thereby providing the direct evidence in supporting the methyl radicals involved OCM reaction mechanism as predicted before …”

Section: Applications Of Vuv‐pims System In Heterogeneous Catalysissupporting

confidence: 72%

“…These results suggest that ethylene and ethane should be the products of secondary reactions of gas-phase methyl radicals, thereby providing the direct evidence in supporting the methyl radicals involved OCM reaction mechanism as predicted before. [80][81][82] The successful detection of methyl radicals in OCM reaction stimulates the interest of research into the gas-phase radical chemistry how methyl radicals convert to ethylene, ethane, and also to CO x in the gas phase. Same to the radical chemistry studied in the combustion chemistry, homogeneous chemical process starts from the collision between radicals and other molecules in the gas phase that should generate a series of secondary intermediate species or stable products.…”

Section: Methane Conversionmentioning

confidence: 99%

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Photoionization Mass Spectrometry for Online Detection of Reactive and Unstable Gas‐Phase Intermediates in Heterogeneous Catalytic Reactions

You

Huang

2019

ChemCatChem

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Heterogeneous catalytic reactions always involve surface intermediates on catalyst surfaces, and some of them also involve reactive and unstable gas-phase intermediates such as radicals and alkyl hydroperoxides. Online detection of these gas-phase intermediates is of great importance for fundamentally understanding reaction mechanisms of relevant heterogeneous catalytic reactions, designing structures of efficient catalysts and optimizing reactors. However, it has remained a long-time challenge due to the lack of routine characterization techniques. Herein we review recent progress on applications of photoionization mass spectrometry in online detection of reactive and unstable gas-phase intermediates in heterogeneous catalytic reactions. The development and advantages of photoionization mass spectrometry and the relevant equipment setup for heterogeneous catalysis studies are also described. Finally, a future perspective is given.[a] Dr. * (m/z = 15), C 2 H 5 * (m/z = 29) and allyl radical (CH 2 CHCH 2 * 4 5 6 7 8

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Section: Applications Of Vuv‐pims System In Heterogeneous Catalysissupporting

confidence: 72%

Section: Methane Conversionmentioning

confidence: 99%

Photoionization Mass Spectrometry for Online Detection of Reactive and Unstable Gas‐Phase Intermediates in Heterogeneous Catalytic Reactions

You

Huang

2019

ChemCatChem

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“…Most previous studies on OCM surface kinetics focus on catalysts with relatively simple crystal structures, such as Li/MgO and La 2 O 3 . Simon et al . proposed a detailed surface mechanism for La 2 O 3 , which is coupled with 450 gas‐phase reactions.…”

Section: Previous Studies On Ocm Reaction Kineticsmentioning

confidence: 99%

Detailed Reaction Mechanisms for the Oxidative Coupling of Methane over La₂O₃/CeO₂ Nanofiber Fabric Catalysts

et al. 2017

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We develop and validate detailed reaction mechanisms to represent the oxidative coupling of methane (OCM) over a La2O3/CeO2 nanofabric catalyst. The reaction mechanism includes 39 reversible gas‐phase reactions and 52 irreversible surface reactions between 22 gas‐phase species and 11 surface species. We use a model‐based interpretation of spatially resolved concentration and temperature profiles measured by using a laboratory‐scale packed‐bed reactor. The reaction mechanisms are validated for inlet feed compositions in the range of 7≤CH4/O2≤11. The results are supported by a reaction pathway analysis that provides insight into the relative contributions of the gas‐phase and surface reactions to form the desired C2+ and the undesired COx products. The results provide new quantitative insights into the complex nature of the OCM chemistry, which can assist practical process and reactor development.

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“…-coke formation (Moustafa and Froment, 2003;QuintanaSolórzano et al, 2005), -biomass conversion (Rangarajan et al, 2010), -oxidative coupling of methane (Simon et al, 2007), -silicon hydride clustering (Wong et al, 2004), -hydrocarboxylation , -carbonylation (Bruk et al, 1998), -organic synthesis (Fontain and Reitsam, 1991), -biological processes (Valdes-Perez, 1992b;Klein et al, 2002;Faeder et al, 2003Faeder et al, , 2005Li et al, 2004;Hatzimanikatis et al, 2004Hatzimanikatis et al, , 2005Blinov et al, 2005a, b;Mayeno et al, 2005;Henry et al, 2007Henry et al, , 2010Hill et al, 2008;Finley et al, 2009), -and many more.…”

Section: Simulation Of Large Complex Reaction Network 421 Network mentioning

confidence: 99%

A Review of Kinetic Modeling Methodologies for Complex Processes

Oliveira

Hudebine

Denis

et al. 2016

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

122

113

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-In this paper, kinetic modeling techniques for complex chemical processes are reviewed. After a brief historical overview of chemical kinetics, an overview is given of the theoretical background of kinetic modeling of elementary steps and of multistep reactions. Classic lumping techniques are introduced and analyzed. Two examples of lumped kinetic models (atmospheric gasoil hydrotreating and residue hydroprocessing) developed at IFP Energies nouvelles (IFPEN) are presented. The largest part of this review describes advanced kinetic modeling strategies, in which the molecular detail is retained, i.e. the reactions are represented between molecules or even subdivided into elementary steps. To be able to retain this molecular level throughout the kinetic model and the reactor simulations, several hurdles have to be cleared first: (i) the feedstock needs to be described in terms of molecules, (ii) large reaction networks need to be automatically generated, and (iii) a large number of rate equations with their rate parameters need to be derived. For these three obstacles, molecular reconstruction techniques, deterministic or stochastic network generation programs, and single-event micro-kinetics and/or linear free energy relationships have been applied at IFPEN, as illustrated by several examples of kinetic models for industrial refining processes.Résumé -Une revue de méthodes de modélisation cinétique pour des procédés complexesDans cet article, les techniques de modélisation cinétique des processus chimiques complexes sont examinées. Après un bref aperçu historique de la cinétique chimique, un aperçu des bases théoriques de la modélisation cinétique d'étapes élémentaires et de réactions globales est présenté. Les techniques classiques de regroupement (lumping) sont ensuite présentées et analysées. Deux exemples de modèles cinétiques regroupés (pour l'hydrotraitement de gazole atmosphérique et pour l'hydrotraitement de résidus) développés à IFP Energies nouvelles (IFPEN) sont présentés. La plus grande partie de cette revue décrit des stratégies avancées de modélisation cinétique, dans lesquelles le détail moléculaire est retenu : les réactions entre les molécules sont représentées ou même subdivisées en étapes élémentaires. Pour être en mesure de conserver ce niveau moléculaire à la fois dans le modèle cinétique et dans les simulations de réacteurs, plusieurs obstacles doivent d'abord être éliminés : (i) la charge doit être décrite en termes de molécules, (ii) les grands réseaux réactionnels doivent être générés automatiquement et (iii) un grand nombre d'équations de vitesse avec leurs paramètres de vitesse doit être dérivé. Pour ces trois obstacles, des techniques de reconstruction moléculaire, des programmes de génération de réseaux déterministes ou stochastiques, et des modèles microcinétiques basés sur des événements constitutifs (single events) et/ou des

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Kinetic Modeling of the Oxidative Coupling of Methane

Cited by 46 publications

References 53 publications

Photoionization Mass Spectrometry for Online Detection of Reactive and Unstable Gas‐Phase Intermediates in Heterogeneous Catalytic Reactions

Photoionization Mass Spectrometry for Online Detection of Reactive and Unstable Gas‐Phase Intermediates in Heterogeneous Catalytic Reactions

Detailed Reaction Mechanisms for the Oxidative Coupling of Methane over La₂O₃/CeO₂ Nanofiber Fabric Catalysts

A Review of Kinetic Modeling Methodologies for Complex Processes

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Kinetic Modeling of the Oxidative Coupling of Methane

Cited by 46 publications

References 53 publications

Photoionization Mass Spectrometry for Online Detection of Reactive and Unstable Gas‐Phase Intermediates in Heterogeneous Catalytic Reactions

Photoionization Mass Spectrometry for Online Detection of Reactive and Unstable Gas‐Phase Intermediates in Heterogeneous Catalytic Reactions

Detailed Reaction Mechanisms for the Oxidative Coupling of Methane over La2O3/CeO2 Nanofiber Fabric Catalysts

A Review of Kinetic Modeling Methodologies for Complex Processes

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Resources

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Detailed Reaction Mechanisms for the Oxidative Coupling of Methane over La₂O₃/CeO₂ Nanofiber Fabric Catalysts