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Catalytic Partial Oxidation in Novel Non-Premixed Counter-Flow Reactor Configurations

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Catalytic Partial Oxidation in Novel Non-Premixed Counter-Flow Reactor Configurations Catalytic Partial Oxidation in Novel Non-Premixed Counter-Flow Reactor Configurations A Dissertation SUBMITTED TO THE FACULTY OF UNIVERSITY OF MINNESOTA BY Ying Lin IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY Advisor: William F. Northrop September. 2020 © Copyright by Ying Lin, 2020 Acknowledgements This work was only made possible under the help of my advisor, collaborators, colleagues, friends and family members. I am very grateful for the privilege of joining Murphy Engine Research Laboratory and being advised by Dr. Will Northrop. The education and training I received has defined who I am for my life and career. Dr. Northrop taught me the most important skills and knowledge for being an independent researcher, and his vision and attitude towards work and life will always inspire me. I want to thank him for his patience, trust, persistence and guidance during these years. Thanks to my collaborators for their generous contribution to this work. Dr. Xuesong Li and Dr. David Kittelson provided insightful directions to my research. Dr. Xuesong Li was also deeply involved in my projects and provided important data. The numerical modeling work was conducted under tremendous help of Dr. Robert Kee, Dr. Gandhali Kogekar and Dr. Canan Karakay. My doctoral training would not be made possible without the funding resources. Sincere thanks to the Minnesota Corn Growers Association and the National Science Foundation. I would also like to acknowledge current and former members of our lab. They are all intelligent and supporting people who inspired me a lot by their work and ideas. To my parents and my wife Yiru Wang, your contained, unconditional love supported me going through the uncertainty and anxiety of these years. You believe in me, celebrate the smallest progress I make, and never stop shaping me into a better person i Abstract Catalytic partial oxidation (CPOx) is established processes for generating synthesis gas (i.e. the mixtures of hydrogen and carbon oxides). It is used to convert heavier hydrocarbon fuels into lighter ones or synthesis gas for a variety of applications. CPOx systems usually incorporate metal catalysts, such as nickel, platinum, rhodium, etc., impregnated on wash-coated porous media to enhance surface reaction rates. The rapid reforming kinetics and expedient light-off characteristics of CPOx make it suitable not only for large-scale industrial applications, but also for on-board vehicle reforming and other portable applications where compactness and simplicity are advantageous. There are different CPOx schemes for desired reforming reactions, including plug-flow reactors, wire gauge reactors, and flash volatilization techniques. Most CPOx reactors reported in the literature implement premixed schemes that mix fuel, oxidizer (usually oxygen), and other species (such as steam) prior reaching the catalyst inlet. Such implementations enjoy benefits of simple structures and flow patterns. However, disadvantages of premixed reformers are also exist including autoignition caused by preheating the mixture before reactions and catalyst deactivation through surface carbon formation and coking. To overcome the disadvantages of premixed CPOx, novel, non-premixed reactor type has been conceived and studied in this body of work. The reactor design is inspired by the canonical counter-flow burner commonly used in flame studies but has a catalyst-coated metal mesh ii located between the air and fuel inlets. The counter-flow CPOx reactor has unique temperature gradients and residence times that tend to reduce coking by avoiding thermal and mixture conditions where carbon is formed. This counter-flow configuration has the potential in both fundamental studies like investigating reforming kinetics and practical applications like enabling advanced combustion modes in internal combustion engines. iii Table of Contents Acknowledgements .............................................................................................................. i Abstract ............................................................................................................................... ii List of Tables.......................................................................................................................vi List of Figures ................................................................................................................... vii Chapter 1 Introduction ................................................................................................. 10 1.1 Motivation ......................................................................................................... 10 1.2 Project Objective Statement .............................................................................. 12 1.3 Significance of Work......................................................................................... 13 Chapter 2 Background ................................................................................................. 15 2.1 Catalytic partial oxidation and fuel reforming .................................................. 15 2.2 Small Scale Reactors......................................................................................... 20 2.3 Catalytic Deactivation and Soot Formation ...................................................... 25 2.4 Ethanol Autothermal Reaction and Reaction Pathway ..................................... 26 2.5 Advanced Laser-based Diagnostics .................................................................. 30 2.6 Applications of Fuel Reforming ....................................................................... 34 Chapter 3 Experimental Apparatus .............................................................................. 39 3.1 Reactor Setup .................................................................................................... 39 3.2 Emission Measurement Equipment .................................................................. 43 3.3 Laser Diagnostic System................................................................................... 44 Chapter 4 Characterization of Hydrocarbon CPOx Using Gas Phase Counter-flow Reactor ……. ..................................................................................................................... 46 iv 4.1 Experimental Procedure .................................................................................... 47 4.2 Results and Discussion ..................................................................................... 50 4.3 Conclusions ....................................................................................................... 63 Chapter 5 Application of Dual Mesh Counter-flow Reactor ....................................... 65 5.1 Experimental Procedure .................................................................................... 66 5.2 Result and Discussion ....................................................................................... 68 5.3 Conclusion ........................................................................................................ 74 Chapter 6 Planar Laser-induced Fluorescence (PLIF) for Noncontact Temperature Measurement ..................................................................................................................... 75 6.1 Experimental Procedure .................................................................................... 76 6.2 Image Processing .............................................................................................. 78 6.3 Results and Discussion ..................................................................................... 82 6.4 Conclusion ........................................................................................................ 89 Chapter 7 Hydrocarbon CPOX with Atomization Reactor .......................................... 91 7.1 Experimental Procedure .................................................................................... 92 7.2 Results and Discussion ..................................................................................... 96 7.3 Conclusions ......................................................................................................114 Chapter 8 Suggested Future Work ..............................................................................116 Bibliography ................................................................................................................... 120 v List of Tables Table 2.1 Summary of pros/cons and industrial developer of popular methane reforming technologies ...................................................................................................................... 36 Table 4.1 Experimental conditions to study mesh location effect .................................... 54 Table 5.1 Dual mesh configuration ignition study conditions .......................................... 73 Table 6.1 Filter and Camera Specifications ...................................................................... 77 Table 6.2 Experimental Conditions for PLIF Thermometer in the Counter-flow Reactor 86 Table 7.1 Liquid fuel reactor characterization conditions ................................................ 95 vi List of Figures Figure 1.1 Reformer efficiency (ηreformer) versus the ϕ of partial oxidation of n-heptane when exhaust gas recirculation (EGR) from an engine operating at ϕ=0.5 .......................11 Figure 2.1 Spatially resolved species and temperature profiles for
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