Muhr, Magdalena
(2025)
Analysing Organosulfur-based Additives to advance Lithium Sulfur Batteries and achieve superior cell performance.
PhD thesis, University of Nottingham.
Abstract
The development of batteries is a crucial interim goal against climate change, and with lithium-ion batteries approaching their limits, new technologies are needed. Lithium-sulfur batteries (LSB) have enormous potential: sulfur is environmentally benign, economic, abundant, and most importantly, has a high theoretical energy density of 1675 mAh/g. Out of all next-generation battery types, LSB technologies have the highest technology readiness level - a system used to assess a technology's maturity. A range of challenges have still to be tackled, such as poor electrical conductivity in the positive electrode, slow conversion kinetics, dendrite formation, and the polysulfide shuttle effect. This project seeks to develop novel electrolyte additives, and explore new ways of enhancing LSB cell performance.
The challenges revolving around upscaling cell production are often overlooked in material development. While the underlying chemistry is identical, the engineering aspects often tremendously impact the cell performance. In Chapter 2, two cell formats will be compared, and hypothesis tests will be applied to enhance galvanostatic cell data reliability.
In Chapter 3, a new approach for developing targeted additives using molecular organosulfur-based compounds will be proposed. Complementing bottom-up and top-down methodologies are combined to accelerate additive design by establishing structure-property relationships, with the ultimate goal of enabling the efficient development of additives with tailored properties.
In Chapter 4, various electrochemical and spectroscopic techniques are employed to analyse the composition of two thiophosphate-based additive mixtures. Galvanostatic cell cycling is conducted to investigate potential cell performance-enhancing properties,
Chapter 5 investigates the potential of ammonium diethoxydithiophosphate (Additive DEDP) in LSB technologies. In continuation of the previous chapter, Additive DEDP and its interaction with S8, Li2S8, and Li2S sulfur species endemic to LSB technologies will be assessed. Special attention will also be given to the complex chemistry of polysulfides in correlation to cell performance.
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