Year
2011
Abstract
A method for the accurate and timely analysis of accountable materials is critical for safeguards measurements in nuclear fuel reprocessing plants. Non-destructive analysis (NDA) methods, such as gamma spectroscopy, are desirable for their ability to produce near real-time data. However, the high gamma background of the actinides and fission products in spent nuclear fuel limits the use of NDA for real-time online measurements. A simple approach for at-line separation of materials would facilitate the use of at-line detection methods. A promising at-line separation method for plutonium and uranium is electrochemically modulated separations (EMS). Using an electrochemical cell with an anodized glassy carbon electrode, Pu and U oxidation states can be altered by applying an appropriate voltage. Because the affinity of the actinides for the electrode depends on their oxidation states, selective deposition can be turned “on” and “off” with changes in the applied target electrode voltage. A high surface-area cell was designed in house for the separation of Pu from spent nuclear fuel. The cell is shown to capture over 1 µg of material, increasing the likelihood for gamma spectroscopic detection of Pu extracted from dissolver solutions. The large surface area of the electrode also reduces the impact of competitive interferences from some fission products. Flow rates of up to 1 mL min -1 with >50% analyte deposition efficiency are possible, allowing for rapid separations to be effected. Results from the increased surface-area EMS cell are presented, including dilute dissolver solution simulant data