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Evaluation of a Detailed Reaction Mechanism for Partial and Total Evaluation of a Detailed Reaction Mechanism for Partial and Total Oxidation of C1 - C4 Alkanes DISSERTATION Submitted to the Faculty of Chemistry of the Rupertus-Carola University of Heidelberg, Germany For the degree of Doctor of Natural Sciences Presented by Raúl Quiceno González Born in Medellín, Colombia Examiners: Prof. Dr. Dr. h. c. Jürgen Warnatz Prof. Dr. Olaf Deutschmann Heidelberg, November 16, 2007 Interdisziplinäres Zentrum für Wissenschaftliches Rechnen Ruprecht – Karls – Universität Heidelberg 2007 DISSERTATION Submitted to the Faculty of Chemistry of the Rupertus-Carola University of Heidelberg, Germany For the degree of Doctor of Natural Sciences Presented by Raúl Quiceno González, Ms, Sciences Born in Medellín, Colombia Heidelberg, November 16, 2007 Title Evaluation of a Detailed Reaction Mechanism for Partial and Total Oxidation of C1 - C4 Alkanes Examiners: Prof. Dr. Dr. h. c. Jürgen Warnatz Prof. Dr. Olaf Deutschmann ACKNOWLEDGMENTS I would like to acknowledge to all the people who helped me directly or indirectly to accomplish this dissertation: First and foremost, I would like to express all my gratitude towards Prof. Dr. Dr. h. c. Jürgen Warnatz for giving the opportunity to share an unforgettable time in his group in Heidelberg. To Prof. Dr. Olaf Deutschmann and his family, for his support during my time in Heidelberg, for the useful comments and great support in the development of my work and for his friendship during difficult moments. To Farid Chejne, my former tutor in Colombia, for his tireless compromise with all of us, for being more than a tutor, a friend. I am also thankful to my colleagues at IWR: Ingrid for her collaboration with all the administrative details, to Barbara for her unvaluable help, to Jürgen Moldenhauer, Till Katzenmeier, Volker Karbach, Shaik and all my coworkers for their help and understanding. Este pequeño parrafo me gustaria dedicarlo a mi familia, solo tengo palabras de agradecimiento para ellos por acompañarme desde la distancia, por brindarme amor y comprension, por sufrir el dolor de la separacion, por aceptarlo y ayudarme a sobre llevarlo de la mejor manera posible; solo tengo palabras de agradecimiento para ustedes, y dificilmente podria describir cuanto los quiero, respecto y admiro: mil gracias. Finally, I would like to thank Sophia, for her boundless love, faith in me, and encouragement and for bring to my life the most beautiful thing that ever happen to me: Madeleine, without both of you this work would still not be completed. i ii ABSTRACT In the present work a chemical kinetic mechanism was developed, suitable for modeling com- bustion and partial oxidation processes of C1 – C4 alkanes. The gas-phase kinetic mechanism describes intermediate and high temperature chemistry. Accordingly, the formation and evo- lution of important intermediate gas-phase species: Olefins and oxygenates were described in terms of different pathways typical at those temperature regimes. A previously developed mechanism suitable for high temperature conditions was extended by including reactions which described the chemistry of total and partial oxidation of methane, ethane, propane, butane, lower alkenes and formation and consumption of their characteristic organic hydro-peroxide radicals and cyclical compounds. The kinetic mechanism was vali- dated by comparing calculated results of ignition delay times, against experimental data ob- tained in shock tubes, for various hydrocarbons and their mixtures, over a wide range of reac- tion conditions (temperature, pressure and mixture composition). Further, the kinetic mecha- nism was evaluated by comparing numerical simulations against experimentally obtained concentration profiles of the main gas-phase species, measured in jet stirred reactors for dif- ferent hydrocarbons and their mixtures during partial oxidation. Next, the mechanism was applied to get a better understanding of the interactions between flow, mass transfer and homogeneous-heterogeneous chemistries during the catalytic partial oxidation of methane in a short contact time reactor, which has recently attracted strong scien- tific and technological interest. The detailed study of the catalytic partial oxidation of methane to syngas in a single gauze reactor was based on three-dimensional numerical simulations of the flow field coupled with heat transport and multi-step gas-phase and surface reaction mechanisms, including the com- putation of the surface coverage. Results from the model were compared with experimental data reported in the literature. The gas-phase mechanism was modeled using a reduced mechanism, and for the surface a previously developed mechanism was adapted. The results from the simulation of the partial oxidation of methane in a short contact time reactor were carried out using the commercial computational fluid dynamics code Fluent, which was cou- pled with external subroutines to model the detailed gas-phase and surface chemistry. Today, the production of synthesis gas (carbon monoxide + hydrogen) is currently carried out via steam reforming. In that process steam passes over a carbon source, often methane or coal, and is heated to produce the synthesis gas. Synthesis gas is extremely valuable commercially iii for the production of methanol, hydrocarbons, higher alcohols for use in detergents, and am- monia to use in fertilizers. There is also a significant interest in the production of hydrogen for fuel cells. However, steam reforming has the major disadvantage of being endothermic and hence requires a large amount of wasted energy to drive the reaction. An alternative to steam reforming is the partial oxidation of the hydrocarbons, especially methane in short con- tact time reactors. This promising route for natural gas conversion into more useful chemicals has the advantage of being auto thermal. iv KURZFASSUNG In der vorliegenden Arbeit wurde ein chemischer Reaktionsmechanismus entwickelt, mit dem Verbrennungsprozesse und Partialoxidationsprozesse von C1 – C4 Alkanen modelliert werden können. Der Reaktionsmechanismus der Gasphase beschreibt Prozesse für mittlere und hohe Temperaturen. Die Ausbildung und Entwicklung wichtiger Zwischenprodukte der Gasphase wie Olefine und sauerstoffhaltige Produkte werden hinsichtlich verschiedener Temperaturbereiche geschildert. Ein bereits entwickelter Mechanismus für Hochtemperaturbedingungen wurde erweitert, indem Reaktionen eingefügt wurden, die die chemischen Reaktionen der vollständigen und partiellen Oxidation von Methan, Ethan, Propan, Butan und kurzkettigen Alkene sowie die Ausbildung und den Verbrauch ihrer charakteristischen organischen hydro-Peroxid Radikalen und zyklische Komponenten beschreibt. Die Überprüfung des Reaktionsmechanismus erfolgte durch Vergleich mit errechneten Ergebnissen von Zündverzugszeiten gegenüber experimentell ermittelte Daten aus Versuchen mit Stossrohren für verschiedene Kohlenwasserstoffe und ihre Mischungen unter verschiedensten Reaktionsbedingungen (Temperatur, Druck und Aufbau der Zusammensetzung). Weiterhin wurde der Reaktionsmechanismus durch Vergleich mit numerischen Simulationen gegenüber experimentell erhaltende Konzentrationsprofile der wichtigsten Spezies in der Gasphase evaluiert. Die Messungen fanden in Reaktionsbehältern für verschiedene Kohlenwassserstoffe und deren Mischungen während der Partialoxidation statt. Als nächster Schritt wurde der Mechanismus angewandt, um ein besseres Verständnis von den ablaufenden Prozessen und deren Wechselwirkungen (Strömungsfeld, Massentransport, homogener und heterogener Reaktionen) während der katalytischen Partialoxidation von Methan in einem Short Contact Time Reactor (SCTR), der derzeit von großem wissenschaftlichen sowie technologischen Interesse ist, zu erlangen. Die detaillierte Studie der katalytischen Partialoxidation von Methan zu Synthesgas auf einer Platinoberfläche, Gauze Reactor, basierte auf dreidimensionale numerische Simulationen reaktiver Strömungen verbunden mit Wärmetransport und mehrstufigen Gasphasenmechanismen sowie Oberflächenreaktionen einschließlich der Berechnung der Oberflächenabdeckung. Die Ergebnisse des Modells wurden mit experimentell ermittelten Daten aus der Literatur verglichen. Der Mechanismus der Gasphase wurde mit einem reduzierten Mechanismus modelliert. Für die Reaktionen auf der Oberfläche wurde ein vorher entwickelter Mechanismus adaptiert. Die Ergebnisse der Partialoxidation von Methan in v einem SCTR wurden mit dem kommerziell erhältlichen CFD-Programm FLUENT simuliert, in dem detaillierte Gasphasen- und Oberflächen-Reaktionsmechanismen berücksichtigt werden. Derzeit wird die Produktion von Synthesegas (Kohlenstoffmonoxid + Wasserstoff) mit dem Verfahren der Dampfreformierung realisiert. In diesem Prozess passiert Dampf eine Kohlenstoffquelle, oft Methan oder Kohle, und wird erhitzt, um Synthesegas zu produzieren. Synthesegas ist kommerziell sehr nützlich für die Produktion von Methanol, Kohlenwasserstoffe, längerkettige Alkohole für Detergentien sowie Ammoniak für Düngemittel. Außerdem besteht ein erhebliches Interesse an der Produktion von Wasserstoffe für Brennstoffzellen. Allerdings hat die Dampfreformierung den großen Nachteil, daß es ein endothermer Prozess ist und folglich viel Energie benötigt, um die Reaktion zu betreiben. Eine Alternative zur Dampfreformierung stellt die Partialoxidation von Kohlenwasserstoffen dar, insbesondere die Umwandlung von Methan in SCTR. Diese vielversprechende Möglichkeit, Erdgas in wertvollere chemische Grundstoffe zu konvertieren, hat den
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