Date of Award

Summer 2020

Document Type

Open Access Dissertation

Department

Chemistry and Biochemistry

First Advisor

Hans-Conrad zur Loye

Abstract

While the use of nuclear technology has proven useful for energy generation and for military use, the proper disposal and storage of the resulting nuclear waste requires serious attention to ensure radioactive species are indefinitely sequestered to protect the biosphere. There are several classifications of nuclear waste such as spent nuclear fuel (from industrial power plants), low level waste (slightly contaminated trash), and high level waste (HLW) which is in the form of a sludge, precipitated salt, or liquid. Each of these requires a different approach to processing and storage. Of these, HLW requires the most attention because it is the most expensive, highest risk, and will take longest to process and store. While the current method of incorporating the HLW into a glass is very successful, it is inefficient for a few of the species found in this waste such as Cs, I, and Tc.

The lack of a universal waste storage material not only calls us to further characterize known materials that are good candidates for waste sequestration, but also to discover new materials with potentially better properties than those of existing materials. Crystal growth, in general, is well suited for material discovery as it facilitates the preparation of new complex compositions in the absence of a fully established crystal chemistry and crystals can be efficiently characterized by single crystal X-ray diffraction. This work explores the exploratory flux crystal growth of uranium oxide framework structures and characterizes their structures as well as thermal and ion exchange properties which are useful for preliminary screening of potential wasteforms and discovering structure-property relationships.

Rights

© 2020, Christian A. Juillerat

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