ORCID

https://orcid.org/0000-0002-6504-3920

Date of Award

Fall 2024

Language

English

Embargo Period

10-8-2025

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

College/School/Department

Department of Chemistry

Program

Chemistry

First Advisor

Evgeny V. Dikarev

Committee Members

Marina A. Petrukhina, Paul J. Toscano, Michael Yeung, Evgeny V. Dikarev

Keywords

Heterometallic Complex, Precursors, Cathode Materials, Li-Ion Battery, Isomerization, Crystallography

Subject Categories

Inorganic Chemistry | Materials Chemistry

Abstract

The synthetic methods for rechargeable battery cathodes are rapidly evolving along with the continuous advancement of the materials themselves. Utilizing precursors for the synthesis of Li- and Na-ion cathode materials are known to ensure a phase-pure product with isotropic element distribution, thereby further enhancing the electrochemical properties of the cathode material. As more cathode materials with complex compositions continue to emerge, the strategies for designing the corresponding precursors are also getting diversified. One of the most promising directions is the employment of single-source precursors (SSPs), defined as molecules that contain all necessary elements in the proper ratio and decomposable under mild conditions to yield phase-pure target compounds upon the low-temperature decomposition. This method both optimizes the synthetic pathways to existing materials and provides an access to new materials that are not accessible by conventional techniques.

In this dissertation, the advancement of multiple SSPs through appropriate methods with delicate design steps is described. In general, this work contributes to developing new preparation techniques for prospective Li- and Na-ion metal oxides for rechargeable batteries, as well as to applying the SSP approach to synthesize and characterize unknown materials. At the same time, this thesis provides a detailed analysis of the structure and properties of different SSPs and highlights some unusual cases of isomerism. The isomerization phenomenon not only alter the precursor design approach but also affects the thermal decomposition properties related to the synthesis of target materials.

License

Creative Commons Attribution 4.0 International License
This work is licensed under a Creative Commons Attribution 4.0 International License.

Available for download on Wednesday, October 08, 2025

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