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The Zinc/Bromine Flow Battery

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The Zinc/Bromine Flow Battery THE ZINC/BROMINE FLOW BATTERY: FUNDAMENTALS AND NOVEL MATERIALS FOR TECHNOLOGY ADVANCEMENT A thesis submitted in partial fulfilment of requirements for the degree of Doctor of Philosophy by Gobinath Pillai Rajarathnam The University of Sydney Faculty of Engineering & Information Technologies School of Chemical & Biomolecular Engineering 2016 Supervisor: Prof. Anthony Vassallo © Copyright by Gobinath Pillai Rajarathnam 2016 All Rights Reserved ii To Amma and Appa. iii Summary Redox flow batteries are a promising solution for solving intermittency challenges and increasing uptake of renewable power sources such as wind and solar. In particular, zinc/bromine batteries are an attractive option for large-scale electrical energy storage due to their relatively low cost of primary electrolyte and high theoretical specific energy of 440 Wh kg-1 of zinc bromide electrolyte. However, inefficient materials of construction hinder practical utilization of this capability and reduce power delivery. Challenges include inefficient electrodeposition and stripping in the zinc half-cell. The work presented in this thesis aims to overcome these limitations by providing an understanding of the fundamental physical and electrochemical processes governing interactions within the bulk electrolyte and at the electrode–electrolyte interface. Suitable alternative materials to improve system performance are developed via electrochemical investigations (voltammetry, impedance spectroscopy), physical characterization (scanning electron microscopy, X-ray diffraction) and molecular modelling (density functional theory). It is shown that conventional chloride-based supporting electrolytes employed to maintain electrolyte conductivity during charging significantly influence the morphology of zinc electrodeposits generated. High chloride concentration causes removal of zinc from the bulk, causing coulombic losses in the system. Following from this point, it is shown that sulfates, phosphates or even a higher proportion of bromides, are suitable alternative supporting electrolytes capable of improving performance. Single-halide type tetrahedral zinc complexes exist in conventional electrolytes, and a previously unreported Raman vibrational band at 220 cm-1 is identified and assigned – to the [ZnBr2Cl(H2O)] complex. iv Alternative ionic liquid additives are also investigated, and it is proven that while they are conventionally considered to be spectators in the zinc half-cell, the reality is in fact otherwise due to the effects of their chemical structures. Studies using hybrid ionic liquid mixtures indicate that each half-cell benefits from the use of different compounds. Cost is an important consideration for battery system, and adding expensive ionic liquids would increase unit electrolyte costs, however improved performance could lead to a lower normalized cost per kW and kWh of the battery. It is expected that the approaches and findings presented in this thesis contribute towards an increased understanding of Zn/Br systems, aiding and guiding the future search for novel materials to further improve this technology. v Statement of Originality I hereby declare that the intellectual content of this thesis is my original work unless stated otherwise, and that all assistance received in preparing this thesis and sources have been acknowledged. No part of this work has been submitted to any institution for the award of a degree. Chapter inputs from collaborative work are outlined as follows (as well as acknowledged in the next section): Chapter 1: All work carried out by the author under the supervision of Prof. Anthony Vassallo. Chapter 2: All work carried out by the author under the supervision of Prof. Anthony Vassallo, with the use of some benchtop full-cell experimental data provided by Martin Schneider (School of Chemical and Biomolecular Engineering, The University of Sydney). Chapter 3: All work carried out by the author under the supervision of Prof. Anthony Vassallo and Dr. Alejandro Montoya (School of Chemical and Biomolecular Engineering, The University of Sydney). Chapter 4: All work carried out by the author under the supervision of Prof. Anthony Vassallo. Chapter 5: All work carried out by the author under the supervision of Prof. Anthony Vassallo, with the use of some Raman experimental data provided by Matthew Suprawinata (School of Chemical and Biomolecular Engineering, The University of Sydney). Chapter 6: All work carried out by the author under the supervision of Prof. Anthony Vassallo using electrolytes provided, and SEM images taken, by Max Easton (School of Chemistry, The University of Sydney). vi Chapter 7: All work carried out by the author under the supervision of Prof. Anthony Vassallo. Chapter 8: All work carried out by the author under the supervision of Prof. Anthony Vassallo. Gobinath Pillai Rajarathnam 8th July 2016 vii List of Publications This thesis contains work which has been accepted or submitted for publication and in external conferences, and edited/expanded for use in the following chapters: Chapter 1: G. P. Rajarathnam and A. M. Vassallo, “Storing Electricity”, Chapter 1, The Zinc/Bromine Flow Battery: Materials Challenges and Practical Solutions for Technology Advancement, 1st ed., p. 97, Springer Singapore, Singapore, (2016). Chapter 2: G. P. Rajarathnam and A. M. Vassallo, “Description of the Zn/Br RFB System”, Chapter 2, The Zinc/Bromine Flow Battery: Materials Challenges and Practical Solutions for Technology Advancement, 1st ed., p. 97, Springer Singapore, Singapore, (2016). Chapter 3: G. P. Rajarathnam, A. Montoya, and A. M. Vassallo, The Influence of a Chloride-Based Supporting Electrolyte on Electrodeposited Zinc in Zinc/Bromine Flow Batteries, Journal of The Electrochemical Society (2016). Manuscript submitted. G. P. Rajarathnam, A. Montoya, and A. M. Vassallo, The Interactions Between Chlorides and Zn (001) Surfaces in Zinc/Bromine Flow Battery Electrolytes, in 229th Meeting of the Electrochemical Society, The Electrochemical Society, San Diego, California, USA (29th May–2nd June 2016). viii Chapter 4: G. P. Rajarathnam, M. Schneider, X. Sun, and A. M. Vassallo, The Influence of Supporting Electrolytes on Zinc Half-Cell Performance in Zinc/Bromine Flow Batteries, Journal of The Electrochemical Society, 163, A5112–A5117 (2016). Chapter 5: G. P. Rajarathnam, M. Easton, M. Schneider, A. Masters, T. Maschmeyer, and A. M. Vassallo, The Influence of Ionic Liquid Additives on Zinc Half-Cell Electrochemical Performance in Zinc/Bromine Flow Batteries, RSC Advances, 6, 27788–27797 (2016). G. P. Rajarathnam, M. Schneider, M. E. Easton, and A. M. Vassallo, Electrochemical Characterization and Comparison of Three Bromine- Sequestering Agents for Zinc/Bromine Flow Battery Applications (Paper No. 3133088), in APCChE 2015 Congress incorporating Chemeca 27 Sept – 01 Oct 2015, Melbourne, Australia (2015). G. P. Rajarathnam, M. Schneider, M. E. Easton, and A. M. Vassallo, Electrochemical Performance of Three Novel Bromine-Sequestering Agents for Zinc/Bromine Flow Battery Electrolytes, in 228th Meeting of the Electrochemical Society, The Electrochemical Society, Phoenix, Arizona, USA (2015). Chapter 6: G. P. Rajarathnam, M. D. Suprawinata, and A. M. Vassallo, Raman Analysis of Electrolyte Speciation in Zinc/Bromine Flow Batteries, in Oz Energy Future Conference, University of New South Wales, Sydney, Australia (4-6th July 2016). Chapter 7: ix G. P. Rajarathnam, and A. M. Vassallo, Half-Cell Electrochemical Performance of Hybridized Ionic Liquid Additives for Zinc/Bromine Flow Battery Applications, in 229th Meeting of the Electrochemical Society, The Electrochemical Society, San Diego, California, USA (29th May–2nd June 2016). Manuscript accepted. Chapter 8: G. P. Rajarathnam and A. M. Vassallo, “Strategies for Studying and Improving the Zn/Br RFB”, Chapter 6, The Zinc/Bromine Flow Battery: Materials Challenges and Practical Solutions for Technology Advancement, 1st ed., p. 97, Springer Singapore, Singapore, (2016). x Authorship Attribution Statement In addition to the statements above, in cases where I am not the corresponding author of a published item, permission to include the published material has been granted by the corresponding author. Gobinath Pillai Rajarathnam 8th July 2016 As supervisor for the candidature upon which this thesis is based, I can confirm that the authorship attribution statements above are correct. Prof. Anthony Vassallo 8th July 2016 xi Author’s Note I have seen some authors choose to add a witty quote at the beginning of their thesis, while others prefer to go with a wise saying. Personally, I find myself inclined to include one or the other as well. However, I believe it would be more meaningful to share something which attempts to explain part of the strong motivational force I feel to pursue my chosen field of research. When I first started working with flow batteries in August 2013 for my PhD, I took it to be just an interesting project that happened to be available and an opportunity to expand my engineering knowledge and skills via research. I soon learnt the ability to harness and store electricity is one of the most powerful tools we have at our disposal to quite literally change the world around us. Below is a brief essay I wrote one afternoon in May 2015 as part of an entry for an energy storage conference scholarship. I’m including this here as a reminder to myself, and to share with the reader, on the importance of each and every individual’s contribution towards
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