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A Mixed-Dimensionality Modeling Approach for Interaction of Heterogeneous Steam Reforming Reactions and Heat Transfer Jeroen Valensa Marquette University

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A Mixed-Dimensionality Modeling Approach for Interaction of Heterogeneous Steam Reforming Reactions and Heat Transfer Jeroen Valensa Marquette University Marquette University e-Publications@Marquette Master's Theses (2009 -) Dissertations, Theses, and Professional Projects A Mixed-Dimensionality Modeling Approach for Interaction of Heterogeneous Steam Reforming Reactions and Heat Transfer Jeroen Valensa Marquette University Recommended Citation Valensa, Jeroen, "A Mixed-Dimensionality Modeling Approach for Interaction of Heterogeneous Steam Reforming Reactions and Heat Transfer" (2009). Master's Theses (2009 -). Paper 17. http://epublications.marquette.edu/theses_open/17 A MIXED-DIMENSIONALITY MODELING APPROACH FOR INTERACTION OF HETEROGENEOUS STEAM REFORMING REACTIONS AND HEAT TRANSFER by Jeroen Valensa, B.S.M.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 December 2009 ABSTRACT A MIXED-DIMENSIONALITY MODELING APPROACH FOR INTERACTION OF HETEROGENEOUS STEAM REFORMING REACTIONS AND HEAT TRANSFER Jeroen Valensa, B.S.M.E. Marquette University, 2009 Hydrogen is most often produced on an industrial scale by catalytic steam methane reforming, an equilibrium-limited, highly endothermic process requiring the substantial addition of heat at elevated temperatures. The extent of reaction, or conversion efficiency, of this process is known to be heat transfer limited. Scaling the industrial process equipment down to the size required for small, compact fuel cell systems has encountered difficulties due to increased heat losses at smaller scales. One promising approach to effectively scale down the reforming process is to coat the catalyst directly onto the heat exchange surfaces of an integrated reactor/heat exchanger. In this way, heat can be effectively transferred to the catalytic reaction sites and conversion efficiency can be greatly improved. Optimizing a small-scale integrated reactor requires an understanding of the interactions between the steam reformer reaction kinetics and the heat and mass transfer effects within the heat exchanger. Past studies of these interactions have predominantly focused on highly simplified flow channel geometries, and are unable to account for devices having augmented heat exchange surfaces. Full three-dimensional methods are possible, but require excessive computational resources. In this work, a mixed-dimensionality modeling approach is developed in order to better address the problems posed by these integrated devices. This modeling approach is implemented using a commercially available thermal finite element code. The solid domain is modeled in three dimensions, while the fluid is treated as a one-dimensional plug flow. The catalyst layer is treated as a surface coating over the three-dimensional surfaces. A subroutine to solve the surface reaction kinetics using a LHHW kinetic model is developed and incorporated into the code in order to address the highly non- linear thermal/kinetic interactions. Validation of the modeling approach is accomplished through comparison of model results to test data obtained from an integrated reactor/heat exchanger test unit. Analysis of the results indicates that the modeling approach is able to adequately capture the complex interactions within the test unit. iii ACKNOWLEDGMENTS Jeroen Valensa, B.S.M.E. I would like to thank my thesis committee – Dr. S. Scott Goldsborough, Dr. John Borg and Dr. Hyunjae Park. Your thorough review and suggestions helped to shape the final end product of this thesis, and is much appreciated. Annette Wolak was always there in the Mechanical Engineering office to make sure that I complied with all of the requirements. Thank you, Annette, for all of your assistance over these past several years. I would like to thank Modine Manufacturing Company, and especially the Fuel Cell Products Group, for financially supporting this work. Over the years I have been blessed with managers who were very supportive of me in my efforts to complete this thesis, and I am especially grateful to Mike Reinke, Mark Voss, Mark Baffa, Joe Stevenson and Eric Steinbach for their support. Adam Kimmel was both a professional colleague and a fellow grad student. Thank you, Adam, for both your technical assistance and your moral support. Having someone in the same boat as me to commiserate with certainly helped a lot. I owe a debt of gratitude to Paul Barnard and Giles Hall for facilitating all of the experimental testing, and to Dr. Liping Cao for her fine CFD work to determine Nusselt number correlations. Finally, a heartfelt thank-you to the most important people in my life – my three boys, Colin, Darren and Preston, and my wonderful wife Amy. Thank you all for supporting me, for believing in me, for letting me work on this thesis when I needed to, and for not letting me quit. iv TABLE OF CONTENTS ACKNOWLEDGMENTS .................................................................................................iii TABLE OF CONTENTS................................................................................................... iv NOMENCLATURE .......................................................................................................... vi 1. INTRODUCTION / MOTIVATION............................................................................. 1 1.1 National Vision of a Hydrogen Economy........................................................ 1 1.2 Hydrogen Production Methods........................................................................ 6 1.3 Process Intensification of Steam Methane Reforming................................... 10 1.4 Catalyzed Heat Exchange Surfaces ............................................................... 13 1.5 Need For Modeling Capabilities.................................................................... 15 1.6 Outline for the Thesis..................................................................................... 16 2. BACKGROUND ......................................................................................................... 18 2.1 Technical Background .................................................................................... 18 2.2 Review of Historical Approaches and State of the Art................................... 29 2.2.1 Model Dimensionality .................................................................... 30 2.2.2 Kinetics ............................................................................................ 42 2.2.3 Heat Transfer and Thermal Boundary Conditions.......................... 48 2.3 Problem Statement.......................................................................................... 53 3. APPROACH ................................................................................................................ 55 3.1 Overview of the Approach.............................................................................. 55 3.2 Detailed Description of the Modeling Approach........................................... 59 3.3 Detailed Description Of the Experimental Test Unit..................................... 72 v 3.4 Description of the Computational Model ...................................................... 82 3.5 Design Optimization Study............................................................................ 93 4. RESULTS .................................................................................................................... 97 4.1 Experimental Unit Test Results ...................................................................... 97 4.2 Reaction Calibration Sample Test Results.................................................... 105 4.3 Computational Model Results....................................................................... 107 4.4 Comparison of Computational and Experimental Results............................ 115 4.5 Factorial Study Results ................................................................................. 124 5. CONCLUSIONS AND RECOMMENDATIONS .................................................... 127 5.1 Conclusions.................................................................................................. 127 5.2 Recommendations for Future Work............................................................. 129 BIBLIOGRAPHY........................................................................................................... 131 APPENDIX A – DETERMINATION OF FIN CHANNEL NUSSELT NUMBER ..... 136 APPENDIX B – CODE FOR SOLVING SMR REACTION ........................................ 142 vi NOMENCLATURE A pre-exponential constant in Arrhenius equation Ac fluid cross-sectional area in flow channel Ai,j conductivity interaction factor for species i and j cp specific heat Dh hydraulic diameter Ea activation energy Fi molar flow rate of species i g acceleration due to gravity gi,T Gibbs function for species i at temperature T o gi,T molar Gibbs function for species i at temperature T and standard-state pressure G Gibbs free energy GHSV Gas Hourly Space Velocity hf convective film coefficient o hi,T molar enthalpy of species i at temperature T and standard-state pressure ja mass flux of species a k kinetic rate factor ka rate of adsorption kinetic factor kd rate of desorption kinetic factor K equilibrium constant L conduction height of the fin Mi molecular weight of species i N number of moles Nu Nusselt number P pressure Pi partial pressure of species i Po standard-state pressure Pr Prandtl number Q rate of heat flow q′ rate of heat flow per unit length q′′ rate of heat flow per unit area (heat flux) r, z spatial coordinates
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