Abstract
Fundamental aspects of the oxidation chemistry of plutonium have been explored by investigating small ternary oxide clusters, M a X Pu Y O Z +, where X+ Y≤3 and 1≤ Z≤7. The metals, M a, that were combined with plutonium to synthesize oxide cluster ions were cerium, lanthanum, uranium, strontium, and zirconium. The compositions and abundances of the clusters formed are interpreted in the context of the relative oxidation state stabilities of the constituent metals, and comparison is made between the gas-phase clusters and solid state oxides. Plutonium combined readily with cerium and uranium to form ternary oxide clusters; this reflects the redox compatibility of plutonium with these two elements and is reminiscent of their solid state behaviors. Although smaller quantities of La X Pu Y O Z +, Sr X Pu Y O Z +, and Zr X Pu Y O Z + clusters were formed, their compositions and abundances revealed the relative redox characteristics of the metal pairs, La/Pu, Sr/Pu and Zr/Pu. It was possible to assign confidently oxidation states to the component metals for several oxide clusters. Our results demonstrate the value of elementary clusters for elucidating plutonium chemistry, and extending the fundamental understanding of the chemical nature of its materials chemistry.
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