Graduate Thesis Or Dissertation
 

Using Metal-Oxo Clusters to Expand Actinide Chemistry

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https://ir.library.oregonstate.edu/concern/graduate_thesis_or_dissertations/xg94hx76w

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  • A molecular approach to metal oxides allows to the study to fundamental bonding and formation behavior for such metals. Moreover, the molecular nature of such oxides or metal-oxo clusters allows the possibility of exploitation of the properties of the parent oxides. The tetravalent metals, in specific, (M=Zr, Hf, Ce, Th, U, Np, Pu) have been chemist’s choice in bottoms-up material design, catalysis, and elucidating reaction pathways in nature and in synthesis. Actinide-oxide clusters, colloids, and materials are particularly sought after and studied for 1) nuclear materials applications, 2) understanding environmental fate and transport of actinides, and 3) exploring the complex bonding behavior of open-shell f-elements. Synthesis of these metal-oxo cluster depend on controlling the hydrolysis and condensation reactions the govern oxide formation. Herein we demonstrate control over the reactions can be met by using counterions and strongly coordinating oxo-anions. As such we demonstrate three new crystal structure families, M6, M84, and M70, and how to access them. The study using three tetravalent metals (Th, U, Ce) additionally allows to probe differences between the metals in the tetravalent group.
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