Precise U and Pu Isotope Ratio Measurements in Nuclear Samples by Hyphenating Capillary Electrophoresis and MC-ICPMS

• Published in: Analytical chemistry (Washington) Vol. 90; no. 14; pp. 8622 - 8628
• Main Authors: Martelat, Benoit, Isnard, Hélène, Vio, Laurent, Dupuis, Erwan, Cornet, Terence, Nonell, Anthony, Chartier, Frédéric
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 17.07.2018
• Subjects: Acetic acid; Actinides; Capillary electrophoresis; Chemistry; Electrophoresis; Fission products; Inductively coupled plasma mass spectrometry; Instrumentation; Ion exchange; Ionization; Isotope ratios; Isotopes; Liquid wastes; Mass spectrometry; Mass spectroscopy; Nuclear Experiment; Nuclear fuels; Nuclear Theory; Physics; Plutonium; Reduction; Resins; Separation; Spectroscopy; Spent nuclear fuels; Uranium; Waste management; couplage; mesures isotopiques U et Pu; combustible nucleaire use; electrophorese capillaire
• ISSN: 0003-2700; 1520-6882
• DOI: 10.1021/acs.analchem.8b01884

Precise isotopic and elemental characterization of spent nuclear fuel is a major concern for the validation of the neutronic calculation codes and waste management strategy in the nuclear industry. Generally, the elements of interest, particularly U and Pu which are the two major elements present in spent fuel, are purified by ion exchange or extractant resins before off-line measurements by thermal ionization mass spectrometry. The aim of the present work was to develop a new analytical approach based on capillary electrophoresis (CE) hyphenated to a multicollector inductively coupled plasma mass spectrometer (MC-ICPMS) for online isotope ratio measurements. An electrophoretic separation protocol of U, Pu, and the fraction containing fission products and minor actinides (Am and Cm) was developed using acetic acid as the electrolyte and complexing agent. The instrumentation for CE was designed to be used in a glovebox, and a laboratory-built interface was developed for hyphenation with MC-ICPMS. The separation was realized with only a few nL of a solution of spent nuclear fuel, and the reproducibilities obtained on the U and Pu isotope ratios were on the order of a few ‰ which is comparable to those obtained by thermal ionization mass spectrometry (TIMS). This innovative protocol allowed a tremendous reduction of the analyte masses from μg to ng and also a drastic reduction of the liquid waste production from mL to μL. In addition, the time of analysis was shorted by at least a factor of three. All of these improved parameters are of major interest for nuclear applications.