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Enhancing the steam-reforming process with acoustics : an investigation for fuel cell vehicle applications PDF

182 Pages·2002·8.7 MB·English
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ENHANCING THE STEAM-REFORMING PROCESS WITH ACOUSTICS: AN INVESTIGATION FOR FUEL CELL VEHICLE APPLICATIONS By PAUL ANDERS ERICKSON A DISSERTATION PRESENTED TO THE GRADUATE SCHOOL OF THE UNIVERSITY OF FLORIDA IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY UNIVERSITY OF FLORIDA 2002 |p» UNIVERSITY OF FLORIDA 3 1262 08554 4335 Copyright 2002 by Paul Anders Erickson This dissertation is dedicated to my wife, Dena. ACKNOWLEDGMENTS Anyone with a semblance oftrue wisdom knows that one in and ofoneselfis a very small thing. Such is the case with this study, as many people have contributed directly or indirectly to this dissertation. I acknowledge the following individuals and institutions who have extended themselves to give support to the present study. I acknowledge the support, encouragement, and patience put forth by my advising professor, Dr. Vernon P. Roan. Dr. Roan is truly a scholar and I am honored to have had him as my mentor for the duration ofmy time at the University ofFlorida. Similarly, I would like to thank my doctoral committee (Dr. Jean M. Andino, Dr. D.Yogi Goswami, Dr. Ulrich H. Kurzweg and Dr. William E. Lear, Jr) for their support in this research project and in my personal education. I acknowledge the State ofFlorida, through the University ofFlorida and the Mechanical Engineering Department for funding my education and allowing me to serve as an instructor and teaching assistant. The research has been funded in part by Ford Motor Company with their generous grant to the University ofFlorida Fuel Cell Research and Training Laboratory for studies dealing with reformation ofhydrocarbon fuels. I acknowledge the support and guidance I have received from my parents Lloyd and Virginia Erickson and my siblings. Words cannot express my thanks to my wife Dena, to whom I have dedicated this work, and my children Timothy, Eliani, and Kari. They provide me with inspiration to fulfill my potential. My family has sacrificed much iv that I might pursue my education. Truly my family is the center ofmyjoy and happiness. I also acknowledge support from my in-laws Fred and Jacque Wright as well as Les Meinzer who provided computer hardware for the publication ofthe project. I acknowledge my colleagues at the Fuel Cell Research and Training Laboratory, with special mention ofTimothy Simmons, Daniel Betts. and Michael Heckwolfwho gave much needed assistance with the project and encouragement at critical times. No acknowledgment would be complete without thanking God for enlightenment, wisdom, and vision to see me through this project. My sincere hope is that He will find that I have used my knowledge, time and resources to help His children here on earth, and that I will be found worthy ofHis approval through the Messiah. Despite any small amount ofearthly knowledge I have obtained, I consider myselfa "Tool before God" and I understand that eternal knowledge and wisdom is His to give to those who humbly and diligently seek His will. TABLE OF CONTENTS page ACKNOWLEDGMENTS iv LIST OF TABLES ix LIST OF FIGURES xi LIST OF SYMBOLS AND NOMENCLATURE xiv ABSTRACT xv CHAPTER INTRODUCTION 1 1 Background 1 Fuel Cells 1 Vehicle Applications 4 Fueling Options 5 Reforming 8 Problem Definition 9 Research Objectives 10 LITERATURE REVIEW AND THEORETICAL APPROACH 2 12 Steam Reforming 12 Limiting Steps in the Reformation Process 13 Acoustics in Past Processes 18 Steam-Reforming in Combination with Acoustics 21 Increased Particle Path Length due to Acoustics 22 Increased Heat Transfer Rate due to Acoustics 25 Increased Overall Reaction Rate due to Acoustics 27 Extension ofCatalyst Life by Using Acoustics 29 Summary 30 Contribution 31 VI 3 EXPERIMENTAL APPROACH AND FACILITY 32 Experimental Approach 32 Experimental Facility 33 Pumping Subassembly 35 Vaporizer Subassembly 36 Reactor Subassembly 39 Catalyst bed 39 Acoustic components 41 Condensing Unit Subassembly 43 Instrumentation and Control Subassembly 44 Temperature control 45 Acoustic control 50 Analysis ofData 51 Gas Chromatography 52 Conversion 55 Space Velocity 56 Removal ofData Points 57 Procedures 57 Modeling the Acoustically Enhanced Reformation Process 57 Factorial Experiment Design 58 Further Data and Verification ofthe Model 60 4 PROPERTIES OF THE ACOUSTIC FIELD 62 The Use ofResonance within the Catalyst Bed 62 Transfer Functions 65 Modal Analysis 70 5 EMPIRICAL MODEL DEVELOPMENT AND ANALYSIS 73 Experimental Results and Model Correlation Factors 73 Uncertainty Analysis 76 Midpoint Curvature 78 Flow Rate 78 Sound Pressure 79 Catalyst Bed Length 80 The Effect ofFrequency 81 Summary 83 6 THE EFFECTS OF ACOUSTICS ON THE REFORMATION PROCESS 84 The Effect on Temperature Profile 84 The Effect on Conversion 88 The Effect on Controllability 92 vii The Effect on Heat Band Power Draw 93 The Effect on Power Output 95 The Effect on Catalyst Degradation 98 Potential Benefits for a Fuel Cell Vehicle 100 7 CONCLUSIONS AND RECOMMENDATIONS 103 Conclusions 103 Recommendations 104 APPENDIX A COMPUTER PROGRAMS 107 B CHECKLISTS AND PROCEDURES 123 C STATISTICAL DESIGN OF EXPERIMENTS 127 D EXPERIMENT RUN ORDERS 135 E TRANSFER FUNCTIONS 137 F TEMPERATURE PROFILES 147 REFERENCES 153 BIOGRAPHICAL SKETCH 158 vin 11 LIST OF TABLES Table page 1. Types offuel cells and their operating parameters 3 1.2 Energy densities offuels (LHV) 7 3.1 Control setpoint matrix 48 3.2 Average and standard deviation for all catalyst bed temperatures utilizing a 250°C setpoint 49 3.3 Gas chromatograph calibration levels 54 3.4 Volume percent species ofthe dry product outlet gas 55 3.5 Factorial input matrix and run order 59 4.1 Waveforms and boundary conditions for a 33°C reactor containing only air .... 72 5. The input matrix and methanol conversion percentage data obtained from the factorial experiments 74 5.2 Total average conversion, pooled standard deviation, standard error, and total degrees offreedom from the factorial experiments 75 5.3 The effects and interactions found from the factorial experimentation 75 5.4 Signal-to-noise t-ratios and statistical significance 77 5.5 Static and kinematic Reynolds numbers and methanol conversion levels for three frequencies 82 6.1 Extent ofconversion for catalyst bed length with and without acoustics 89 6.2 Average and standard deviation ofthe centerline temperatures with a setpoint temperature of250°C at various locations both with and without a 165dB acoustic field 93 IX

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