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oai:null:10339/574452026-04-21T20:54:41Zcom_10339_14934col_10339_38132

Lepley, Nicholas D. 2016-01-11T09:35:29Z 2016-01-11T09:35:29Z 2015 https://wakespace.lib.wfu.edu/handle/10339/57445 This work explains some of the current issues driving the development of Li batteries and some of the current research opportunities. In particular it focuses on using ab initio theoretical methods to model electrode/electrolyte interfaces for inorganic solid electrolyte materials, especially those related to Li$_3$PS$_4$. I develop a general scheme based on the interface energy for analyzing interfaces between crystalline solids, quantitatively including the effects of varying configurations and lattice strain. This scheme is successfully applied to the modeling of likely interface geometries of several solid state battery materials including Li metal, Li$_3$PO$_4$, Li$_3$PS$_4$, Li$_2$O, and Li$_2$S. This formalism, together with partial density of states analysis, allows me to characterize the extent, stability, and transport properties of these interfaces. My investigation finds that all of the interfaces in this study are stable with the exception of Li$_3$PS$_4$/Li. For this chemically unstable interface, the partial density of states helps to identify mechanisms associated with the interface reactions. The energetic measure of interfaces and analysis of the band alignment between interface materials indicate multiple factors which may be predictors of interface stability, an important property of electrolyte systems. en Wake Forest University Density Functional Theory Interfaces Lithium batteries Solid electrolytes First Principles Investigations of Solid-Solid Interfaces in Lithium Battery Materials Dissertation Holzwarth, Natalie Salsbury, Freddie Kerr, William Thonhauser, Timo Salam, Akbar Physics open.access