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Heat and Mass Transfer Correlations for Steam Methane Reforming in Non-Adiabatic, Process-Intensified Catalytic Reactors" (2011)

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Heat and Mass Transfer Correlations for Steam Methane Reforming in Non-Adiabatic, Process-Intensified Catalytic Reactors Marquette University e-Publications@Marquette Master's Theses (2009 -) Dissertations, Theses, and Professional Projects Heat and Mass Transfer Correlations for Steam Methane Reforming in Non-Adiabatic, Process- Intensified aC talytic Reactors Adam Stephen Kimmel Marquette University Recommended Citation Kimmel, Adam Stephen, "Heat and Mass Transfer Correlations for Steam Methane Reforming in Non-Adiabatic, Process-Intensified Catalytic Reactors" (2011). Master's Theses (2009 -). Paper 103. http://epublications.marquette.edu/theses_open/103 HEAT AND MASS TRANSFER CORRELATIONS FOR STEAM METHANE REFORMING IN NON-ADIABATIC, PROCESS-INTENSIFIED CATALYTIC REACTORS by Adam S. Kimmel, B.S.Ch.E. A Thesis submitted to the Faculty of the Graduate School, Marquette University, in Partial Fulfillment of the Requirements for the Degree of Master of Science Milwaukee, Wisconsin August 2011 ABSTRACT HEAT AND MASS TRANSFER CORRELATIONS FOR STEAM METHANE REFORMING IN NON-ADIABATIC, PROCESS-INTENSIFIED CATALYTIC REACTORS Adam S. Kimmel, B.S.Ch.E. Marquette University, 2011 Because of its high energy density, hydrogen is a desirable energy source for the achievement of a renewable energy landscape. Though production methods like thermolysis, electrolysis and biomass conversion, among others, are thought to be long term renewable solutions, catalytic steam methane reforming (SMR) is currently the predominant mechanism to produce hydrogen on an industrial scale. The highly endothermic, transport-limited reforming process has also been scaled down through process intensification to create efficient small-scale hydrogen-generating systems. One proposed geometry utilizes a catalytic finned cylinder that provides a manufacturable solution to enable high-efficiency heat exchange and SMR reaction. An accurate representation of the reactor performance characteristics is imperative to the design of small-scale systems. The Nusselt and Sherwood numbers, the respective dimensionless temperature and concentration gradients, are commonly used to model the transport characteristics. Previous works have outlined the significance of modeling techniques that include radial diffusion to capture the bulk-phase diffusive resistance. However, prior studies have either over-simplified the transport to neglect diffusion in the bulk fluid or employed CFD to include the relevant effects. A considerable limitation of CFD-derived solutions is a high degree of computational intensity. In the current study, local transport coefficients are determined for the SMR reaction in a catalytic microchannel. The 2-D cylindrical transport equations are simplified based on approximations from prior work to represent the channel geometry. The applied assumptions dramatically decrease the model’s computation time. A finite central-differencing scheme is implemented to solve the coupled transport equations with the reaction kinetics, and is solved through simultaneous matrix inversion. A kinetic model for SMR reactions is included as a model subroutine to describe the highly non- linear transport/kinetic interactions, while accounting for species adsorption/desorption to and from the catalyst. The transport model is compared to known solutions for the desired boundary conditions to validate the diffusive effects. The full model is validated against experimental data, and is able to reasonably predict the expected transport behavior and chemical kinetic interactions in the catalytic microchannel. i ACKNOWLEDGEMENTS Adam S. Kimmel, B.S.Ch.E. Foremost, I would like to thank God, with whom all things are possible. I would like to thank my thesis committee – Dr. S. Scott Goldsborough, Dr. John Borg and Dr. Jon Koch. The effort and time you put in to reviewing this work is much appreciated, and your suggestions significantly helped to improve its completeness. Special thanks to Dr. Goldsborough for project guidance and crucial technical assistance during the programming phase. I am grateful for your time and effort to help me complete this project. I would like to express most sincere gratitude to Dr. Aroon Viswanathan and Mr. Jeroen Valensa for their superb technical assistance, time, friendship and support, which were critical to this study. Jeroen compiled much of the experimental setup description that was described in this study, for which I am grateful. I would also like to express most sincere thanks to Marquette University and Modine Manufacturing for providing financial support toward completion of this research. Without their support this project would not be possible. Also, I would like to thank Drs. Philip Voglewede, Ashvinikumar Mudaliar and Liping Cao for technical advice and assistance. I would like to thank my parents and family, who have always supported and encouraged me while teaching me the importance of education. Finally, I would like to dedicate this thesis to my wonderful wife, Katie, whose love, encouragement and selfless perseverance afforded me the opportunity to pursue my goals, and to my children Cole and Kennedy, who always have time for a smile and a hug for their dad. ii TABLE OF CONTENTS ACKNOWLEDGEMENTS .................................................................................................... i TABLE OF CONTENTS ....................................................................................................... ii NOMENCLATURE ...............................................................................................................v 1. INTRODUCTION / BACKGROUND ..............................................................................1 1.1 Industrial Applications of Hydrogen .........................................................................1 1.1.1 Common Industrial Uses...................................................................................1 1.1.2 Fuel Cells ..........................................................................................................2 1.2 Hydrogen Production Methods ..................................................................................3 1.2.1 Steam Methane Reforming (SMR) ...................................................................3 1.2.2 Catalytic Partial Oxidation (CPOX) .................................................................6 1.2.3 Autothermal Reforming (ATR) ........................................................................7 1.2.4 SMR and ATR Comparison ..............................................................................7 1.3 Catalytic Reactor Design ...........................................................................................8 1.3.1 Reactor Type and Design Approaches ..............................................................8 1.3.1.1 Packed Bed Reactor .................................................................................8 1.3.1.2 Catalytic Monolith .................................................................................10 1.3.2 Reaction Mechanisms and Kinetics ................................................................14 1.3.2.1 Chemical Equilibrium ............................................................................19 1.4 Modine Catalytic Finned Cylinder Reactor .............................................................21 1.5 Transport Coefficient Derivation Methods ..............................................................24 1.5.1 Definition of Transport Coefficients ...............................................................25 1.6 Thesis Objectives and Manuscript Summary ..........................................................26 iii 2. STATE OF THE ART IN TRANSPORT COEFFICIENT FORMULATION ...............28 2.1 1-D Two-Phase Analytical Approach ......................................................................30 2.2 2-D Convection-Diffusion with Wall Reaction Approach ......................................37 3. MODEL FORMULATION AND SOLUTION METHODOLOGY ..............................52 3.1 Transport Equations and Transport Coefficient Definition .....................................52 3.1.1 Boundary Layer Equations and Fundamental Assumptions ...........................52 3.1.2 Boundary and Initial Conditions .....................................................................57 3.1.3 Bulk Fluid Parameters.....................................................................................59 3.1.4 Thermophysical Properties .............................................................................60 3.2 Catalytic Surface Reactions and the LHHW Kinetic Mechanism ...........................61 3.3 Solution Methodology .......................................................................................68 3.3.1 Code Development..........................................................................................68 3.3.2 Full Matrix Finite Difference Method ............................................................69 3.3.3 Validation Plan................................................................................................76 3.3.4 Experimental Testing Description ..................................................................77 3.3.5 Approach Justification ....................................................................................85 3.4 Application of Catalytic Minichannel Reactor ........................................................91 3.5 Novelty of the Current Research ..............................................................................92 4. COMPUTATIONAL MODEL RESULTS......................................................................94
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