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Co-Laminar Flow Cells for Electrochemical Energy Conversion

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Co-Laminar Flow Cells for Electrochemical Energy Conversion Co-laminar flow cells for electrochemical energy conversion by Marc-Antoni Goulet M.Sc. (Physics), McMaster University, 2008 B.Sc., McGill University, 2006 Dissertation Submitted in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy in the School of Engineering Science Faculty of Applied Sciences Marc-Antoni Goulet 2016 SIMON FRASER UNIVERSITY Summer 2016 Approval Name: Marc-Antoni Goulet Degree: Doctor of Philosophy Title: Co-laminar flow cells for electrochemical energy conversion Examining Committee: Chair: Amr Marzouk Lecturer Erik Kjeang Senior Supervisor Associate Professor Michael Eikerling Supervisor Professor Gary Wang Supervisor Professor Edward Park Internal Examiner Professor Matthew Mench External Examiner Professor Department of Mechanical, Aerospace and Biomedical Engineering University of Tennessee, Knoxville Date Defended/Approved: May 2nd, 2016 ii Abstract A recently developed class of electrochemical cell based on co-laminar flow of reactants through porous electrodes is investigated. New architectures are designed and assessed for fuel recirculation and rechargeable battery operation. Extensive characterization of cells is performed to determine most sources of voltage loss during operation. To this end, a specialized flow cell technique is developed to mitigate mass transport limitations and measure kinetic rates of reaction on flow-through porous electrodes. This technique is used in in conjunction with cyclic voltammetry and electrochemical impedance spectroscopy to evaluate different treatments for enhancing the rates of vanadium redox reactions on carbon paper electrodes. It is determined that surface area enhancements are the most effective way for increasing redox reaction rates and thus a novel in situ flowing deposition method is conceived to achieve this objective at minimal cost. It is demonstrated that flowing deposition of carbon nanotubes can increase the electrochemical surface area of carbon paper by over an order of magnitude. It is also demonstrated that flowing deposition can be achieved dynamically during cell operation, leading to considerably improved kinetics and mass transport properties. To take full advantage of this deposition method, the total ohmic resistance of the cell is considerably reduced through design optimization with reduced channel width, integration of current collectors and reduction of reactant concentration. With electrodes enhanced by dynamic flowing deposition the cell presented in this study demonstrates nearly a fourfold improvement in power density over the baseline design. Producing more than twice the power density of the leading co-laminar flow cell without the use of catalysts or elevated temperatures and pressures, this cell provides a low- cost standard for further research into system scale-up and implementation of co-laminar flow cell technology. More generally, the experimental technique and deposition method developed in this work are expected to find broader use in other fields of electrochemical energy conversion. Keywords: fuel cell; flow battery; laminar flow; microfluidic; flow-through porous electrodes; vanadium iii Dedication I would like to dedicate this thesis to all the natural wonders which have been sacrificed for the sake of human endeavors such as this. It is hoped that the minor results contained within will eventually help to alleviate our collective environmental burden. Et ma mère. Merci maman. iv Acknowledgements First and foremost, I would like to thank my supervisor Erik Kjeang for giving me this opportunity and helping me along the way. His gentle supervision and unwavering faith in my abilities allowed me the necessary freedom to explore the new ideas that have been essential to the success of this project. On a more personal level, I would like to thank him for setting such a good example of dedication and persistence. I would also like to express my sincere gratitude to my co-supervisor Michael Eikerling who took the time to see me and patiently answer my infinite questions. Without his reliable intellectual support, my research could easily have become mired in endless confusion and pointless digressions. I would similarly like to acknowledge Gary Wang for his sympathetic ear and judicious advice. In addition, I would like to express my appreciation to Prof. Em. Maria Skyllas-Kazacos for her general kindness, and for sharing some of her extensive experience with me during many pleasant discussions throughout my internship at UNSW. In relation to this, I would like to acknowledge the sponsorship provided by the Australia Endeavour program which made it possible for me to broaden my experience and the perspective of my research. Similarly, I would like to acknowledge the Natural Sciences and Engineering Research Council of Canada (NSERC) for their generous support during my degree. I’d also like to thank my predecessor Jin who kindly got me started on this project and helped me to avoid unnecessary pitfalls. Of course this project would never have been completed without the hard work and assistance of all the co-op students passing through the lab in the past four years, namely: Jeffrey To, Chris de Torres, Stephen Rayner, Spencer Arbour, Aronne Habisch and Will Kim. Being able to share the frustrations of experimental work with them made it all the more enjoyable. Likewise, I am also very grateful to my graduate colleagues at SFU and friends in FCRel, with a special mention to Omar in particular, for all the pleasant conversations and good times. I wish there had been more. Last but not least, I’d like to acknowledge all the family and friends I was unable to spend quality time with due to this work. I look forward to seeing you all again. v Table of Contents Approval .......................................................................................................................... ii Abstract .......................................................................................................................... iii Dedication ...................................................................................................................... iv Acknowledgements ......................................................................................................... v Table of Contents ........................................................................................................... vi List of Tables ................................................................................................................. viii List of Figures................................................................................................................. ix List of Acronyms .............................................................................................................. x Chapter 1. Introduction ............................................................................................. 1 1.1. Background ............................................................................................................ 1 1.2. Review of co-laminar flow cells ............................................................................... 3 1.3. Research perspectives ........................................................................................... 8 1.4. Motivation and objective ....................................................................................... 10 Chapter 2. Theory .................................................................................................... 12 2.1. Electrochemical cells ............................................................................................ 12 2.1.1. Kinetics .................................................................................................... 15 2.1.2. Ohmic resistance ..................................................................................... 17 2.1.3. Mass transport ......................................................................................... 18 2.1.4. Reactant crossover .................................................................................. 19 2.2. Co-laminar flow cells ............................................................................................ 20 Chapter 3. Summary of contributions .................................................................... 23 3.1. Microfluidic redox battery ...................................................................................... 23 3.2. Reactant recirculation in electrochemical co-laminar flow cells ............................. 25 3.3. Direct measurement of electrochemical reaction kinetics in flow-through porous electrodes ................................................................................................. 27 3.4. The importance of wetting in carbon paper electrodes for vanadium redox reactions ............................................................................................................... 29 3.5. In situ enhancement of flow-through porous electrodes with carbon nanotubes via flowing deposition .......................................................................... 31 3.6. Approaching the power density limits of aqueous electrochemical flow cells ........ 34 Chapter 4. Conclusions ........................................................................................... 37 4.1. Present work ........................................................................................................ 37 4.2. Future work .........................................................................................................
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