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Rappleye, Devin,Jeong, Sang-Mun,Simpson, Michael Electrochemical Society 2016 Journal of the Electrochemical Society Vol.163 No.9
<P>Electroanalytical measurements, such as cyclic voltammetry and chronopotentiometry, have been applied by other researchers tomany eutectic LiCl-KCl mixtures containing a single analyte, typically a rare earth or actinide ion. These measurements have demonstrated the applicability of electroanalytical measurements of concentration in molten LiCl-KCl eutectic, which is prevalently used as an electrolyte in the electrorefining of used nuclear fuel (UNF). However, UNF electrorefiners contain multiple actinide and rare earth ions, necessitating the ability to make electroanalytical measurements in multi-analyte mixtures. The presence of multiple analytes creates interferences and overlapping signals. Chronoamperometry, cyclic voltammetry (CV), chronopotentiometry and open-circuit potential measurements were performed in eutectic LiCl-KCl mixtures containing a range of GdCl3 and LaCl3 concentrations to explore the issues associated with applying electroanalytical techniques in multi-analyte molten salt mixtures and to develop possible solutions. CV was found to be most promising for separating and analyzing each ion's signal. CV measurements were semi-differentiated and correlated to concentration using peak heights and principal component regression (PCR) to determine the concentration from electrochemical signals. The lowest average relative error was obtained using PCR for Gd3+ (6.21%) and using peak height correlations for La3+ (10.4%). (C) 2016 The Electrochemical Society. All rights reserved.</P>
Simulated real-time process monitoring of a molten salt electrorefiner
Rappleye, D.,Simpson, M.,Cumberland, R.,McNelis, D.,Yim, M.S. North-Holland Pub. Co 2014 Nuclear engineering and design Vol.273 No.-
An alternative approach to monitoring the pyrochemical process (pyroprocessing) for spent nuclear fuel treatment is proposed and examined. This approach relies on modeling and the real-time analysis of process readings. Using an electrorefiner model, named ERAD, cathode potential and cell current were identified as useful process readings. To provide a real-time analysis of these two process readings, an inverse model was developed based on fundamental electrochemical relations. The model was applied to the following operating modes: pure uranium deposition, co-deposition of uranium and plutonium, and co-deposition of uranium and zirconium. Using the cell current and cathode potential, the model predicted which species were depositing and their rates. The deposition rates predicted by the inverse model compared favorably to those calculated by ERAD.
Devin Rappleye,Sang-Mun Jeong,Mario Gonzalez,Lauryn C. Hansen,Michael F. Simpson 한국방사성폐기물학회 2015 방사성폐기물학회지 Vol.13 No.S
Voltammetry has shown promise as a method to estimate the concentrations of actinides in the molten LiCl-KCl used as an electrolyte in spent nuclear fuel electrorefiners. This salt typically contains several actinides in addition to many active metal fission products (rare earths, Group I & II metals). However, most of the voltammetry studies to date have focused on a single actinide or lanthanide in eutectic LiCl-KCl. This paper examines experimental and analytical techniques that can be used to estimate the concentration of a molten salt mixture containing both lanthanum (III)- and gadolinium(III)-chloride in eutectic LiCl-KCl. The aspects of the experimental procedures and setup that are unique to a multi-lanthanide mixture are briefly discussed. Experimental results from qualitative and quantitative analyses of cyclic voltammetry and open-circuit potentiometry are presented. Due to the close proximity of their standard potentials, extensive analytical work is required to estimate the concentrations. Two approaches are used in this work: peak separation and multivariate analysis. The merits of these two methods will be analyzed and discussed.
Scale Up of Ceramic Waste Forms for Electrorefiner Salts Produced during Spent Fuel Treatment
Kenneth J. Bateman,Matthew C. Morrisona,Devin S. Rappleye,Michael F. Simpson,Steven M. Frank 한국방사성폐기물학회 2015 방사성폐기물학회지 Vol.13 No.S
A full-scale process has been developed to immobilize fission products that accumulate within the Mark IV electrorefiner (ER) electrolyte at Idaho National Laboratory. ER salt was blended with treatment additives, followed by pressureless consolidation (PC) in a furnace to produce a durable ceramic waste form (CWF). The goal is the development of a process to consolidate actual radioactive ER salt into a form suitable for transportation and disposal. Four batches (300 to 400 kg per batch) of full-scale pre-qualification material preparation runs have been prepared. From these four batches of nonradioactive salt-loaded surrogate material, three full-scale PC trials have been conducted. The first PC test run, established equipment parameters with a basic CWF container design. The second trial included a modified CWF container design, real-time measurement of CWF consolidation, and an audio recording to identify cracking during the CWF cool-down. During the third trial, salt was doped (from the fourth material preparation batch) to create a nonradioactive salt material and to more closely represent actual ER salt. The second and third trials were also used to validate a model developed for the CWF. The CWF model is beneficial for understanding and predicting the physical processes that occur during the heat cycle. This would be particularly useful when the CWF is located in a hot cell, which makes accessing and examining a CWF difficult.