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Microfluidic Fuel Cells Microfluidic Fuel Cells by Erik Kjeang M.Sc., Umeå University, 2004 A Dissertation Submitted in Partial Fulfillment of the Requirements for the Degree of DOCTOR OF PHILOSOPHY in the Department of Mechanical Engineering © Erik Kjeang, 2007 University of Victoria All rights reserved. This thesis may not be reproduced in whole or in part, by photocopy or other means, without the permission of the author. ii Supervisory Committee Microfluidic Fuel Cells by Erik Kjeang M.Sc., Umeå University, 2004 Supervisory Committee Dr. David Sinton, Department of Mechanical Engineering Supervisor Dr. Ned Djilali, Department of Mechanical Engineering Supervisor Dr. Peter Oshkai, Department of Mechanical Engineering Departmental Member Dr. David A. Harrington, Department of Chemistry Outside Member Dr. Shelley D. Minteer, Department of Chemistry, Saint Louis University External Examiner iii Abstract Supervisory Committee Dr. David Sinton, Department of Mechanical Engineering Supervisor Dr. Ned Djilali, Department of Mechanical Engineering Supervisor Dr. Peter Oshkai, Department of Mechanical Engineering Departmental Member Dr. David A. Harrington, Department of Chemistry Outside Member Dr. Shelley D. Minteer, Department of Chemistry, Saint Louis University External Examiner Microfluidic fuel cell architectures are presented in this thesis. This work represents the mechanical and microfluidic portion of a microfluidic biofuel cell project. While the microfluidic fuel cells developed here are targeted to eventual integration with biocatalysts, the contributions of this thesis have more general applicability. The cell architectures are developed and evaluated based on conventional non-biological electrocatalysts. The fuel cells employ co-laminar flow of fuel and oxidant streams that do not require a membrane for physical separation, and comprise carbon or gold electrodes compatible with most enzyme immobilization schemes developed to date. The demonstrated microfluidic fuel cell architectures include the following: a single cell with planar gold electrodes and a grooved channel architecture that accommodates gaseous product evolution while preventing crossover effects; a single cell with planar carbon electrodes based on graphite rods; a three-dimensional hexagonal array cell based on multiple graphite rod electrodes with unique scale-up opportunities; a single cell with porous carbon electrodes that provides enhanced power output mainly attributed to the increased active area; a single cell with flow-through porous carbon electrodes that iv provides improved performance and overall energy conversion efficiency; and a single cell with flow-through porous gold electrodes with similar capabilities and reduced ohmic resistance. As compared to previous results, the microfluidic fuel cells developed in this work show improved fuel cell performance (both in terms of power density and efficiency). In addition, this dissertation includes the development of an integrated electrochemical velocimetry approach for microfluidic devices, and a computational modeling study of strategic enzyme patterning for microfluidic biofuel cells with consecutive reactions. v Table of Contents Supervisory Committee ...................................................................................................... ii Abstract..............................................................................................................................iii Table of Contents................................................................................................................ v Acknowledgments.............................................................................................................. vi Dedication......................................................................................................................... vii Organization.....................................................................................................................viii Chapter 1 Introduction ..................................................................................................... 1 1.1 Aims and Motivation .......................................................................................... 1 1.1.1 Objective..................................................................................................... 1 1.1.2 Overview of Fuel Cells for Portable Power................................................ 2 1.1.3 Overview of Biofuel Cells .......................................................................... 2 1.2 Review of Microfluidic Fuel Cells ..................................................................... 8 1.2.1 Definition and Fundamentals...................................................................... 8 1.2.2 Microfluidic Fuel Cell Developments ........................................................ 9 1.2.7 Microfluidic Biofuel Cell Developments.................................................. 15 Chapter 2 Summary of Contributions............................................................................ 18 2.1 Integrated Electrochemical Velocimetry for Microfluidic Devices.................. 18 2.2 Hydrogen Peroxide as an Oxidant for Microfluidic Fuel Cells ........................ 19 2.3 Planar and Three-Dimensional Microfluidic Fuel Cell Architectures Based on Graphite Rod Electrodes............................................................................................... 20 2.4 High-Performance Microfluidic Vanadium Redox Fuel Cell........................... 22 2.5 A Microfluidic Fuel Cell with Flow-Through Porous Electrodes .................... 23 2.6 An Alkaline Microfluidic Fuel Cell Based on Formic Acid and Hypochlorite Bleach ........................................................................................................................... 24 2.7 Strategic Enzyme Patterning for Microfluidic Biofuel Cells............................ 26 Chapter 3 Conclusions and Future Work....................................................................... 28 3.1 Conclusions and Contributions......................................................................... 28 3.2 Future Work...................................................................................................... 34 Bibliography ..................................................................................................................... 39 Appendix A Integrated Electrochemical Velocimetry for Microfluidic Devices............ A Appendix B Hydrogen Peroxide as an Oxidant for Microfluidic Fuel Cells....................B Appendix C Planar and Three-Dimensional Microfluidic Fuel Cell Architectures Based on Graphite Rod Electrodes................................................................................................C Appendix D High-Performance Microfluidic Vanadium Redox Fuel Cell..................... D Appendix E A Microfluidic Fuel Cell with Flow-Through Porous Electrodes................E Appendix F An Alkaline Microfluidic Fuel Cell Based on Formic Acid and Hypochlorite Bleach ........................................................................................................... F Appendix G Strategic Enzyme Patterning for Microfluidic Biofuel Cells...................... G vi Acknowledgments I would like to express my greatest appreciation to my supervisors, Dr. David Sinton and Dr. Ned Djilali, for their excellent support and guidance throughout all aspects of my research. It has been a true privilege to work with them and share their combined expertise and experience essential to this dissertation. I would also like to thank all my other coworkers within the biofuel cell project: Dr. Alexandre G. Brolo, Dr. David B. Levin, Dr. Manuel Marechal, Amanda Finn, Robert Sacci, Meikun Fan, Dan Sanderson, David Harrison, Jonathan McKechnie, and most of all, Dr. David A. Harrington, the chair of the biofuel cell project, for effectively acting as a ‘third supervisor’ and great mentor in the field of electrochemistry. I would like to thank all my colleagues at the Department of Mechanical Engineering, and all past and present members of the microfluidics group and the CFCE group, in particular Marc Secanell and Ron Songprakorp for sharing joy and frustration in our graduate office, and undergraduate students Jesse Musial, Brent Proctor and Raphaelle Michel who worked under my supervision. I would also like to acknowledge financial support from the Natural Science and Engineering Research Council of Canada (NSERC), Angstrom Power Inc., and Bengt Ingeströms Stipendiefond. Finally, I would like to express my gratitude and love to my family in Sweden for their endless support and care regardless of how far away from home I may go, and to my kiwi girlfriend Nicky Collins who has contributed tremendously to my quality of life and wellbeing as a graduate student in Canada. vii Dedication This dissertation is dedicated to Dr. Mohammad R. Golriz, who was my graduate supervisor during my Master’s degree at Umeå University in Sweden and Carleton University in Ottawa, Canada. It was Dr. Golriz who brought me to where I am today, and without his inspiration and enthusiasm I would never have started my doctoral studies. Many thanks, Mohammad, for your continuous support and guidance. viii Organization This dissertation has the following organization: Chapter 1 provides an introduction, including the overall objectives, motivation of the work, an overview of previous research, and specific objectives of this dissertation based on current research trends.
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