Transuranic Actinide Reactions with Simple Gas-Phase Molecules

摘要

The intent of this research is to conduct an experimental study of f-element chemistry for the purpose of identifying reaction trends and mechanisms of the early actinide metals with simple-gas phase molecules. Previous research has elucidated some of the fundamental chemistry of the 4f elements; however, more complex chemistry is expected for the 5f series due to the inclusion of the 5f electrons in the valence shell. The matrix isolation approach, which is well-suited to the experimental study of transient species, will be used for sample collection, and IR/NIR/VIS spectroscopy will be employed to interrogate deposited matrices. The strength of this method lies in the use of isotopes of reactants, which permits the identification of guest molecules in a noble gas matrix by observation of vibrational frequency shifts and patterns upon isotopic substitution. Using this technique at the University of Virginia, the first noble gas-actinide bond has recently been identified, a weak U-Ar bond on the CUO molecule. Uranium has similarly been observed to bond to krypton and xenon, whereas thorium and the lanthanides have not exhibited this activity. It is expected that plutonium will be even more reactive in this respect. We will extend the body of actinide experimental evidence to include the tranuranic elements neptunium, plutonium, and americium reacted with isotopes of oxygen, nitrogen, hydrogen, carbon monoxide, and carbon dioxide.