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Membraneless Hydrogen Bromine Laminar Flow Battery for Large Membraneless Hydrogen Bromine Laminar Flow Battery for Large-Scale Energy Storage by William Allan Braff Submitted to the Department of Mechanical Engineering in partial fulfillment of the requirements for the degree of Doctor of Philosophy at the MASSACHUSETTS INSTITUTE OF TECHNOLOGY February 2014 c Massachusetts Institute of Technology 2014. All rights reserved. Author.............................................................. Department of Mechanical Engineering December 19, 2013 Certified by. Cullen R. Buie Assistant Professor of Mechanical Engineering Thesis Supervisor Certified by. Martin Z. Bazant Professor of Chemical Engineering and Mathematics Thesis Supervisor Accepted by . David E. Hardt Chairman, Department Committee on Graduate Theses 2 Membraneless Hydrogen Bromine Laminar Flow Battery for Large-Scale Energy Storage by William Allan Braff Submitted to the Department of Mechanical Engineering on December 19, 2013, in partial fulfillment of the requirements for the degree of Doctor of Philosophy Abstract Electrochemical energy storage systems have been considered for a range of potential large-scale energy storage applications. These applications vary widely, both in the order of magnitude of energy storage that is required and the rate at which energy must be charged and discharged. One such application aids the integration of renew- able energy technologies onto the electrical grid by shifting the output from renewable energy resources to periods of high demand, relaxing transmission and distribution requirements and reducing the need for fossil fuel burning plants. Although the mar- ket need for such solutions is well known, existing technologies are still too expensive to compete with conventional combustion-based solutions. In this thesis, the hydrogen bromine laminar flow battery (HBFLB) is proposed and examined for its potential to provide low cost energy storage using the rapid reaction kinetics of hydrogen-bromine reaction pairs and a membrane-less laminar flow battery architecture. In this architecture, fluid reactants and electrolyte flow through a small channel at sufficiently low Reynolds number that laminar flow is maintained and the liquid electrolyte acts as a separator between the reactants. Experimental results from a proof of concept cell are presented, and compared with numerical and analytical modeling results to better understand discharging and recharging behavior. General theoretical principles for the design and optimization of laminar flow batteries are also developed. These results indicate that the HBLFB can efficiently store and discharge energy at very high power densities compared to existing battery technologies using low cost reactants and stack materials at room temperature and atmospheric pressure. Thesis Supervisor: Cullen R. Buie Title: Assistant Professor of Mechanical Engineering Thesis Supervisor: Martin Z. Bazant Title: Professor of Chemical Engineering and Mathematics 3 4 Acknowledgments The work that I've done for my Ph.D. would never have been possible without the support of a number of people. I am deeply indebted to my coadvisors, Professors Cullen Buie and Martin Bazant, from whom I've learned a great deal, and whose advice and guidance have helped me grow as an engineer. I am also very grateful to Professor Jessika Trancik for her help to better understand grid-scale storage, and to Bill Aulet, Tod Hynes, Frank O'Sullivan, Lucas DiLeo, Louis Goldish, Roman Lybinsky, and Tom Pounds for their mentorship and advice about the entrepreneurial implications of the work. I must also thank Dr. Cortney Mittelsteadt, whose support and advice set me on the road to becoming an engineer in the first place, and without whom I would never have had the chance to pursue a Ph.D. I would also like to acknowledge the support of my colleagues in the Buie and Bazant groups. Thanks to Dr. Matthew Suss, Laura Gilson, Gregoire Jacquot, Ricardo Charles, and Kameron Conforti for their past and future contributions to the flow battery project. I am also grateful for the advice and support I have received from my other labmates, Dr. Peng Bai, Dr. Daosheng Deng, Naga Dingari, Dr. Todd Ferguson, Zhifei Ge, Dr. Jihyung Han, Dr. Paulo Garcia, Laura Gilson, Youngsoo Joung, Andrew Jones, Edwin Khoo, Dr. Jeff Moran, Dr. Sourav Padhy, Matthew Pinson, Carlos Sauer, Sven Schlumpberger, Alisha Schor, Ray Smith, Qianru Wang, Yi Zeng, and Dr. Pei Zhang. Thanks as well to my colleagues at the Sloan School of Management, Jamie Fordyce and Dave Parkin, from whom I learned a great deal. In addition to the excellent professional mentorship and guidance I have received, my deepest gratitude goes to my family for their unending patience and belief in me over the past years. My mother and father, Florence and Allan, and my siblings and their spouses, Jen, Joe, Jon, and Julie, have been constant sources of support for me, and I am grateful to all of them. Lastly, my wife Georgiana has been with me every step of the way, from the moment I applied to MIT onwards. Her love and support has been invaluable to me, and no words can describe how grateful I am to her. 5 6 Contents 1 Introduction 25 1.1 Large-Scale Energy Storage . 25 1.2 Electrochemical Energy Storage . 26 1.2.1 Lithium Ion Batteries . 27 1.2.2 Hydrogen Oxygen Regenerative Fuel Cells . 28 1.2.3 Vanadium Redox Flow Batteries . 29 1.2.4 Hydrogen Bromine Redox Flow Batteries . 31 1.3 Membrane-less Electrochemical Systems . 32 1.4 Hydrogen Bromine Laminar Flow Battery . 35 1.5 Study Objectives and Organization . 36 2 Experimental Investigation of the Hydrogen Bromine Laminar Flow Battery 39 2.1 Introduction . 39 2.2 Methods . 41 2.2.1 Cell fabrication . 41 2.2.2 Numerical model details . 41 2.3 Results . 43 2.3.1 Numerical model . 43 2.3.2 Discharge experiments . 43 2.3.3 Analytical limiting current . 44 2.3.4 High power operation . 47 2.3.5 Recharging and round-trip efficiency . 47 7 2.4 Discussion . 50 3 Boundary Layer Analysis of Membrane-less Electrochemical Cells 53 3.1 Introduction . 53 3.2 Mathematical Model . 55 3.2.1 Example: Hydrogen bromine laminar flow battery . 56 3.2.2 Governing equations in the electrolyte . 58 3.2.3 Anode boundary conditions . 60 3.2.4 Cathode boundary conditions . 61 3.2.5 Inlet and outlet boundary conditions . 62 3.3 Boundary Layer Analysis . 63 3.3.1 Plug flow . 63 3.3.2 Poiseuille Flow . 65 3.3.3 Reactant crossover . 66 3.3.4 Coulombic efficiency . 68 3.3.5 Under-limiting current . 69 3.4 Results and Discussion . 71 3.5 Conclusion . 75 4 Inertial Effects on the Generation of Co-laminar Flows 77 4.1 Introduction . 77 4.2 Numerical Solution . 78 4.3 Results and Discussion . 79 4.3.1 Comparison with fully developed flow . 79 4.3.2 Three-dimensional effects . 87 4.3.3 Mitigation strategies . 88 4.4 Conclusion . 92 5 Guidelines for Stationary Energy Storage Technology Development 95 5.1 Introduction . 95 5.2 Experimental . 96 8 5.2.1 Introduction . 96 5.2.2 Site selection . 97 5.2.3 Optimization routine . 97 5.2.4 Establishing performance parameters . 100 5.2.5 Optimal system selection . 101 5.3 Results . 102 5.3.1 Introduction . 102 5.3.2 Storage shifts output into periods of high prices . 103 5.3.3 Balancing increased revenue with storage cost . 104 5.3.4 Comparing storage performance at the technology level . 106 5.4 Discussion . 108 6 Perspectives and Conclusions 111 6.1 Summary of Conclusions . 111 6.2 Perspectives . 112 A Guidelines for Energy Storage: Supplemental Information 119 A.1 Balancing increased revenue with storage cost . 119 A.2 Comparison of hybrid storage with pure arbitrage . 138 A.3 Performance and Design of Optimally Sized Systems . 140 A.4 Tradeoffs in system behavior along an isoperformance line . 146 9 10 List of Figures 1-1 Exemplar schematic of a lithium-ion battery. During discharge, lithium ions pass from the graphene anode into the electrolyte, and then in- tercalate into a spinel cathode, forcing electrons through an external load. Figure reproduced from [1]. 28 1-2 Schematic of a vanadium redox flow battery. The anolyte and catholyte are flowed past their respective electrodes to produce electrical en- ergy. Figure reproduced with permission by the Electrochemical Soci- ety from Skyllas-Kazacos et al. [2]. 30 1-3 Cell schematic for a hydrogen bromine redox flow battery. During discharge, hydrogen is oxidized at the anode to produce protons and bromine is reduced at the cathode to generate hydrobromic acid. Elec- trons are forced through an external load. During charging, electrical energy is pumped back into the system to reverse the process and replenish the reactants. Figure reproduced with permission by the Electrochemical Society from Cho et al. [3]. 31 1-4 Reproduced schematic of the cell employed by Ferrigno et al. with coplanar electrodes and a vanadium redox pair [4] (a). The revised cell developed by Choban et al. employed vertical, electrodes to enhance utilization along with formic acid and dissolved oxygen as its fuel and oxidant, respectively [5] (b). Part (a) reprinted with permission from Ferrigno et al. [4]. Copyright 2002 American Chemical Society. Part (b) reproduced with permission from Choban et al. [5]. Copyright 2004 Elsevier. 33 11 1-5 Reproduced schematic of the cell employed by Jayashree et al. com- pared to the earlier design employed by Choban et al. [5,6] (a and b). The new cell design incorporated a gas diffusion electrode (GDE) to allow gaseous oxygen to reach the cathode. The independent current- voltage behavior of the anode and cathode of the new cell incorporating the GDE was drastically improved compared to the original cell (c). Figures reprinted with permission from Jayashree et al. [6]. Copyright 2005 American Chemical Society. 34 1-6 Schematic of a hydrogen-bromine laminar flow battery (HBLFB) [7].
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