Youd, Arthur Boyd; (2022) Atomistic Insights into Solid-State Lithium and Sodium-Ion Cathodes and Electrolytes. Doctoral thesis (Ph.D), UCL (University College London).

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Abstract

Solid-state batteries have the potential to revolutionise energy storage. Their rapid development requires a multidisciplinary scientific effort. Computational materials science operates at the confluence of computational science, materials chemistry, physics and environmental science. This thesis was tasked with deploying the best of these approaches and gaining insight into electrochemical problems which have hitherto not been accounted for by conventional techniques. This work specifically focussed on the fundamental properties of cathodes and electrolytes pertaining to their electrochemical performance. The cathodes studies were divided into mixed cation, simple and correlated electronic cathodes. Key electronic characteristics were identified in the mixed cation cathode NNMST in a collaborative study on the cathode material. A simple layered cathode NaxCoO2 was studied where its phase behaviour was quantitatively tested while surveying a wide selection of functionals to inform a more general theoretical approach to deintercalation. The more exotic phase behaviour and correlated electronic material were further studied with ab-initio lessons learned in the earlier studies. These thorough investigations yielded actionable insights on the description of sodium ion cathodes and will inform future studies. High-throughput studies of electrolytes evaluated the electrochemical attributes of three materials' unique materials, informing future laboratory studies to ascertain their suitability as a real-world solid-state electrolyte.

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