Interfacial Chemistry in Bipolar Membrane-Containing Redox Flow Battery Systems

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Degree type
Doctor of Philosophy (PhD)
Graduate group
Chemistry
Discipline
Chemistry
Subject
Bipolar membrane
Carbon electrodes
Charge transfer kinetics
Graphite oxide
Redox flow battery
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Copyright date
01/01/2024
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Author
Metlay, Amy
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Abstract

Bipolar Membranes (BPMs) are a promising membrane technology that is currently being integrated into a variety of electrochemical energy conversion and storage devices. The acid-base redox flow battery utilizes a BPM to separate its anolyte and catholyte chambers. In the charged state of the redox flow battery, the anolyte is strongly acidic and the catholyte is strongly basic, adding a cross-membrane potential to the system of ~830 mV. A major benefit of all flow battery technologies is the separation of the reaction volume from the electrolyte tank, enabling individual optimization for capacity and power. However, this architecture results in several components and interactions that must be controlled before critical performance metrics can be met. A fundamental investigation of three such components is the primary topic of this dissertation.Chapter 1 provides a brief review of currently studied BPM devices and systems as well as open questions for research. In chapter 2, the role of graphite oxide as a water dissociation catalyst in BPMs is investigated. The ideal GO catalytic loading density and orientation inside a BPM’s interface as well as the movement of ions around individual GO nanosheets is discussed. Chapter 3 focuses on the entirety of the acid-base redox flow battery system, utilizing engineered design of a new three-chamber system to mitigate effects of membrane fouling and strict catholyte restrictions. Chapter 4 presents a study of the fundamental electrochemical processes that occur at a graphitic carbon electrode surface. Chemically functionalized graphitic electrodes with hydrophilic properties display higher values of capacity and faster heterogeneous charge transfer kinetics. Finally, in chapter 5, conclusions and outlooks derived from this dissertation are discussed. A better understanding of these individual components – BPMs, engineered system design, and electrode kinetics – will allow for the optimization of the acid-base redox flow battery as well as the possible integration of fundamental discoveries from this research into other electrochemical systems that utilize at least one of these components.

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Mallouk, Thomas, E
Date of degree
2024
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