Electrochemically-Modulated Separations For Destructive And Nondestructive Analysis For Process Monitoring And Safeguards Measurments

A timely, accurate, and precise analysis of uranium reprocessing streams is import for process monitoring and nuclear material accountability. For material accountancy, it is critical to detect both acute and chronic diversions of nuclear materials. Therefore, both on-line nondestructive (NDA) and destructive analysis (DA) approaches are desirable. Current methods for DA involve grab sampling and laboratory based column extractions that are costly, hazardous, and time consuming. Direct on-line gamma measurements of Pu, while desirable, are not possible due to contributions from other actinides and fission products. Electrochemically-modulated separation (EMS) is a straightforward, cost effective alternative technology being investigated at Pacific Northwest National Laboratory for highly selective, slip-stream sampling of U or Pu from reprocessing streams. The EMS selectivity results from simultaneous surface and redox chemistry that allows the affinity of the electrode to be turned 'on' or 'off' under potential control. Once isolated, the accumulated Pu can be measured by gamma spectroscopy or retained in a small quantity (nanogram-milligram) to reduce radiological concerns and to facilitate transport to laboratory based mass spectrometry instrumentation. In this study, we investigate both destructive and nondestructive applications of EMS. First, nondestructive Pu gamma analysis is performed using dissolved BWR spent fuel. Reduction factors for actinide and fission products and initial estimates of measurement uncertainties were measured. The methodology for DA sampling will also be reported for both Pu and U.