The chemistry, kinetics, and implications of oxygen defects in Li-excess oxides

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Abstract/Contents

Abstract
Li-excess layered oxides are a promising class of positive electrode materials with the potential to simultaneously improve both the energy density and cost of Li-ion battery systems. However, these materials suffer from several adverse electrochemical properties resulting from a host structure that becomes unstable at low lithium contents. In this dissertation, a comprehensive view of the role of oxygen defects in Li-excess oxides will be developed. First, the coupling of oxygen and lithium defects will be rationalized from thermodynamic principles. Using X-ray spectroscopy and ptychography, the continuous loss of oxygen from Li-excess materials over cycling will then be demonstrated. Surprisingly, a variety of characterization techniques indicate that the oxygen-deficient bulk structure contains persistent oxygen vacancies, offering a unified framework for understanding previous observations of transition metal reduction and cation disordering with cycling. I will then investigate other factors which affect the oxygen release process, including the lithium content and the particle morphology. Overall, the results presented in this dissertation inform the design and utilization of Li-excess oxides and illuminate promising chemical, structural, and morphological approaches for mitigating oxygen release in layered oxide materials.

Description

Type of resource text
Form electronic resource; remote; computer; online resource
Extent 1 online resource.
Place California
Place [Stanford, California]
Publisher [Stanford University]
Copyright date 2021; ©2021
Publication date 2021; 2021
Issuance monographic
Language English

Creators/Contributors

Author Csernica, Peter Michael
Degree supervisor Chueh, William
Thesis advisor Chueh, William
Thesis advisor Lindenberg, Aaron Michael
Thesis advisor Salleo, Alberto
Degree committee member Lindenberg, Aaron Michael
Degree committee member Salleo, Alberto
Associated with Stanford University, Department of Materials Science and Engineering

Subjects

Genre Theses
Genre Text

Bibliographic information

Statement of responsibility Peter Michael Csernica.
Note Submitted to the Department of Materials Science and Engineering.
Thesis Thesis Ph.D. Stanford University 2021.
Location https://purl.stanford.edu/cf776vd7593

Access conditions

Copyright
© 2021 by Peter Michael Csernica
License
This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).

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