UC Santa Barbara

Lithium-ion batteries are a cornerstone of modern society. As the demand for batteries increases, and the types of applications expand and diversify, there is a huge momentum to improve and optimize all aspects of a battery. The electrode materials within a lithium-ion battery largely dictate the maximum capacity that can be stored and the charge rate. To improve these properties, it is necessary to develop accurate electrode material design strategies. This work examines a variety of refractory oxides as anode material candidates to develop a deeper understanding of the relationships between crystal structure and battery performance. Wadsley-Roth materials are a burgeoning class of high voltage anode materials, that are championed for their ability to store large amounts of charge at fast cycling rates. A variety of these materials are experimentally examined to understand the impact of transition metal selection, crystallographic features, disorder, and particle size on material performance. Data-mining efforts pulled a large number of published experimental data sets together to draw broader insight and design strategies for this material family. Inspired by crystallographic motifs in the Wadsley-Roth family, metal-metal bonding is evaluated as an alternative design strategy for fast-charging materials, using the Mo cluster compound LiScMo3O8. Detailed studies explore the unusual relationship between electrochemistry and magnetism in this material, illuminating the coupled relationship between lithium insertion, disorder, and electronic structure in this frustrated magnet. Together, this work develops more nuanced understanding on the relationship between crystallographic features and high-rate properties, informing future material design strategies for fast-charging Li-ion batteries.