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http://hdl.handle.net/11375/25193
Title: | Magnetic Resonance Investigations of Ion Transport Phenomena in Lithium-Ion Battery Electrolyte Materials |
Authors: | Bazak, Jonathan David |
Advisor: | Goward, Gillian |
Department: | Chemistry and Chemical Biology |
Keywords: | lithium ion batteries;magnetic resonance;MRI;PFG-NMR;ion transport;electrochemical modelling |
Publication Date: | 2020 |
Abstract: | The subject of this thesis is the application of magnetic resonance methods to the characterization and quantification of lithium-ion transport in a wide range of lithium-ion battery electrolyte materials relevant to the electromobility and energy storage sectors. In particular, field-gradient magnetic resonance techniques, in the form of PFG-NMR diffusivity measurements of both liquid- and solid-state electrolytes and in situ MRI of electrochemical cells, comprise the core means by which these characterizations were performed. PFG-NMR and ionic conductivity studies of a range of liquid-state electrolyte mixtures were performed, as a function of temperature, to assess how key mass and charge transport properties reflect differences in composition. In situ MRI was used to study the effect of temperature on steady-state concentration gradient formation in polarized liquid electrolytes, with the results quantitatively compared to model predictions. This approach was then extended, using a combination of MRI and spatially-resolved PFG-NMR, to study the interlinked effects of temperature and current density on concentration gradient formation, and to attempt a comprehensive characterization of the ion transport parameters with spatial resolution. Finally, PFG-NMR and MAS-NMR were applied in a solid-state electrolyte context to investigate compositional effects on ion transport in the argyrodite family of lithium-sulphide ion conductors, and the influence of macroscopic sample format (glass, crystalline powder, compressed crystalline pellet) on micro-scale ion transport in a thio-LISICON ion conductor. Taken together, the studies demonstrate the effectiveness of magnetic resonance methods for the robust elucidation of the means by which material properties impact ion transport in technologically-relevant lithium-ion electrolyte systems. |
URI: | http://hdl.handle.net/11375/25193 |
Appears in Collections: | Open Access Dissertations and Theses |
Files in This Item:
File | Description | Size | Format | |
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Bazak_Jonathan_D_finalsubmission202001_PhD.pdf | 36.27 MB | Adobe PDF | View/Open |
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