Date of Award

Fall 2025

Document Type

Open Access Dissertation

Department

Chemistry and Biochemistry

First Advisor

Hans-Conrad zur Loye

Abstract

The United States owns a substantial amount of radioactive waste as a result of decades of research, weapons manufacturing, and nuclear energy production. As nuclear energy and research continue to add to our stockpiles of waste, the issue of remediating this waste becomes more pressing. Many of the radioactive constituents of this waste, such as the transuranic (Z > 92) elements, will give off radioactivity at harmful levels for millennia. Thus, a robust method of storing this waste is paramount to ensuring public safety. Currently, nuclear waste is being processed by vitrifying it in borosilicate glass. However, this method has shortcomings that may be improved upon by instead utilizing crystalline waste forms as matrices to hold radioactive elements.

Some of the most long-lived radionuclides in our radioactive waste are the minor actinides – the transuranic elements, excluding plutonium. The design of crystalline waste forms for such elements in inherently difficult due to the dearth of information available for their crystal chemistries – their rarity, limited quantity, and radiotoxicity make them difficult to study. However, by indirectly studying the crystal chemistry by utilizing non-radioactive surrogate elements with similar properties, we can make inferences on the properties of minor actinide-containing crystals and make future syntheses utilizing minor actinides more likely to succeed. More details will be discussed in Chapter 1.

In this dissertation, the syntheses, crystal structures, and nuclear waste form-relevant properties of different lanthanide-containing compositions – as analogues of minor actinide compositions – will be presented and discussed (Chapters 2-6) before culminating in the presentation and discussion of successful americium-containing crystal syntheses, structure determinations, and property measurements (Chapter 7).

Rights

© 2025, Hunter Bernard Tisdale

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