Theses and Dissertations Collection

Uranium can be recovered from uranium oxide (UO2) spent fuel through the combination of oxide reduction and electrorefining processes. During oxide reduction, the spent fuel is introduced to molten LiCl-Li2O salt at 650°C and the UO2 is reduced to uranium metal via two routes: (1) electrochemically, and (2) chemically by lithium metal (Li°) that is produced electrochemically. However, the hygroscopic nature of both LiCl and Li2O leads to the formation of LiOH, contributing hydroxyl anions (OH-), the reduction of which interferes with the Li° generation required for the chemical reduction of UO2. In order for the oxide reduction process to be an effective method for the treatment of uranium oxide fuel, the role of moisture in the LiCl-Li2O system must be understood. The behavior of moisture in the LiCl-Li2O molten salt system was studied using cyclic voltammetry, chronopotentiometry and chronoamperometry, while reduction to hydrogen was confirmed with gas chromatography.