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Topic

Computational Models of Nanostructured Materials for Energy Storage and Conversion

Department of Chemistry

Date & location

• Wednesday, April 23, 2025
• 8:00 A.M.
• Virtual Defence

Examining Committee

Supervisory Committee

• Dr. Irina Paci, Department of Chemistry, University of Victoria (Supervisor)
• Dr. Thomas Baker, Department of Chemistry, UVic (Member)
• Dr. Ulrike Stege, Department of Computer Science, UVic (Outside Member)

External Examiner

• Dr. Toon Verstraelen, Department of Physics and Astronomy, Ghent University

Chair of Oral Examination

• Dr. Lincoln Shlensky, Department of English, UVic

Abstract

This dissertation develops and benchmarks computational methods for the rational design of materials for energy storage and conversion. The first portion of the text presents three projects aimed at introducing computationally efficient methods for studying the mechanisms of capacitive energy storage in nanocomposite dielectric materials. Studying model systems consisting of alkaline earth metal oxides with nanoscopic silver inclusions using Density Functional Theory reveals that manipulating the composition and morphology of a nanocomposite’s components permits large increases in electric permittivity. A continuum model for such composites is introduced and shown to reproduce many of the effects of inclusion morphology on permittivity. Finally, a model based on inducible atomic dipoles is studied for several types of inorganic cluster, and its accuracy is shown to be dependent in part upon the degree of charge transfer within the clusters. The second portion of the dissertation benchmarks the performance of various Density Functional Approximations in the prediction of the activity of metal–nitrogen–carbon (M–N–C) catalysts for the oxygen reduction reaction. The calculated activity trends of M–N–C catalysts—specifically metalloporphyrins—are found to by highly method-dependent. The primary drivers of this dependence are explored, and best practices for similar systems are suggested while also highlighting the importance of benchmarking for new systems.