Application of Voltammetry for Quantitative Analysis of Actinides in Molten Salts

Abstract

Our previous work (“Method Development for Quantitative Analysis of Actinides in Molten Salts” 2015) demonstrated that by following a set of developed procedures and a refined data analysis method, cyclic voltammetry can be used for very precise, real-time quantitative concentration measurements of actinides in molten salts. This work examines the suitability of the established procedures over a wider range of concentrations comparable to those expected in the normal operation of an electrorefiner used in the pyrochemical processing of used nuclear fuel. We found that electrochemical methods can be used for very precise concentration measurements up to approximately 2 wt%. For higher actinide concentrations, the value of the diffusion coefficient decreases and these variations have to be taken into consideration. We also investigated the application of voltammetry for analyzing systems containing multiple elements (U3+ and Pu3+) and found that a zero current baseline determination of the second or succeeding peak in the voltammogram is not a correct approach, since that peak is affected by the tail from the peak that preceded it. We then used a different method of data analysis that allows for an accurate baseline determination and can be used to analyze systems involving more than one component.