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Willit, J.

Publications and source records attributed to Willit, J..

A Parametric Study of Operating Carbon Anodes in the Oxide Reduction Process

A parametric study of the electrolytic reduction of uranium dioxide in molten lithium chloride – lithium oxide using carbon anodes was conducted to determine the operational parameter values necessary for high yields. Operational parameters evaluated in this study include anode and cathode current densities, anodic polarization, UO 2 batch size, and method of electrochemical control. Seven oxide reduction experiments were conducted with between 25 g and 100 g UO 2 . The current density on the cathode was the critical parameter, which indicates the reduction process is kinetically controlled by cathodic reactions. High cell currents were achieved without the application of high anodic potentials by using a large anode surface area. As a result, this approach facilitates efficient reduction at high throughput without production of chlorine or other corrosive gasses.

36 MATERIALS SCIENCE↗

Voltammetry Method Evaluation

The purpose of the ANL MPACT Voltammetry project is to evaluate the suitability of previously developed cyclic voltammetry techniques to provide electroanalytical measurements of actinide concentrations in realistic used fuel processing scenarios. The molten salts in these scenarios are very challenging as they include high concentrations of multiple electrochemically active species, thereby creating a variety of complications. Some of the problems that arise therein include issues related to uncompensated resistance, cylindrical diffusion, and alloying of the electrodeposited metals. Improvements to the existing voltammetry technique to account for these issues have been implemented, resulting in good measurements of actinide concentrations across a wide range of adverse conditions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Experiments in anodic film effects during electrorefining of scrap U-10Mo fuels in support of modeling efforts

A monolithic uranium molybdenum alloy clad in zirconium has been proposed as a low enriched uranium (LEU) fuel option for research and test reactors, as part of the Reduced Enrichment for Research and Test Reactors program. Scrap from the fuel's manufacture will contain a significant portion of recoverable LEU. Pyroprocessing has been identified as an option to perform this recovery. A model of a pyroprocessing recovery procedure has been developed to assist in refining the LEU recovery process and designing the facility. Corrosion theory and a two mechanism transport model were implemented on a Mat-Lab platform to perform the modeling. In developing this model, improved anodic behavior prediction became necessary since a dense uranium-rich salt film was observed at the anode surface during electrorefining experiments. Experiments were conducted on uranium metal to determine the film's character and the conditions under which it forms. The electro-refiner salt used in all the experiments was eutectic LiCl/KCl containing UCl{sub 3}. The anodic film material was analyzed with ICP-OES to determine its composition. Both cyclic voltammetry and potentiodynamic scans were conducted at operating temperatures between 475 and 575 C. degrees to interrogate the electrochemical behavior of the uranium. The results show that an anodic film was produced on the uranium electrode. The film initially passivated the surface of the uranium on the working electrode. At high over potentials after a trans-passive region, the current observed was nearly equal to the current observed at the initial active level. Analytical results support the presence of K{sub 2}UCl{sub 6} at the uranium surface, within the error of the analytical method.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗