Simulated real-time process monitoring of a molten salt electrorefiner

Rappleye, Devin; Simpson, Michael F.; Cumberland, Riley; McNelis, David; Yim, Man‐Sung

doi:10.1016/j.nucengdes.2014.02.024

Cited by 11 publications

(7 citation statements)

References 16 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Studies on pyroprocessing technology have been stimulated in several countries including analysis, and U and Pu concentrations were precisely quantified up to approximately 2 wt%. In addition to the experimental efforts, computational models for ER have been actively developed in order to predict the material distribution in the system [8][9][10][11]. Zhang [8][9] developed kinetic ranging from 69.5 ± mA cm -2 to 220 ± 32 mA cm -2 .…”

Section: Introductionmentioning

confidence: 99%

Measurement and Analysis of Exchange Current Density for U/U3+ Reaction in LiCl-KCl Eutectic Salt via Various Electrochemical Techniques

Yoon

Phongikaroon

2017

Electrochimica Acta

View full text Add to dashboard Cite

Electrochemical impedance spectroscopy (EIS), linear polarization (LP), Tafel and cyclic voltammetry (CV) were performed to investigate the exchange current density (i 0) of U/U 3+ reaction in LiCl-KCl eutectic salt under different UCl 3 concentrations (0.5 wt%-4 wt%) and temperature conditions (723 K-798 K). The EIS spectra were measured by applying minimum overpotential from equilibrium potential and fitted to the proposed equivalent circuit. From the EIS experiments, the calculated values of i 0 were ranging from 0.0054 A cm-2 to 0.102 A cm-2. For the LP and Tafel methods, i 0 values were determined from the linear fitting at small and large overpotential ranges of the current-potential curves. The measurement for i 0 via CV was done analogously to the LP method. All i 0 values have the linear trend with the change of concentration and temperature; however, these values measured by LP, Tafel, and CV methods are greatly influenced by the change in electrode surface area. Overall, i 0 agreed within 33% relative error range with the EIS method being the most consistent and accurate in comparison to reported literature values. Dimensionless analysis was done on the EIS data sets providing insightful correlations for prediction of i 0 under various experimental conditions.

show abstract

Section: Introductionmentioning

confidence: 99%

Measurement and Analysis of Exchange Current Density for U/U3+ Reaction in LiCl-KCl Eutectic Salt via Various Electrochemical Techniques

Yoon

Phongikaroon

2017

Electrochimica Acta

View full text Add to dashboard Cite

show abstract

“…As part of the quest to further develop the pyroprocessing program, several researchers around the world have investigated the thermodynamic and electrochemical behavior of rare earth, uranium, and minor actinide elements to develop a knowledge database for advancing applications of near-real time monitoring of the ER for material accountability purposes [3][4][5] and supporting model efforts. [6][7][8][9][10] Kim and coworkers investigated the use of cyclic voltammetry (CV) and chronoamperometry (CA) as methods of online monitoring of the concentrations of species in the ER. 3 A linear relationship between CV peak currents and the concentration of neodymium-III (Nd 3+ ) was shown, reflecting the ability to use CV as a method of concentration monitoring.…”

mentioning

confidence: 99%

Comparison of Exchange Current Density Acquisition Methods for LaCl₃in Molten LiCl-KCl Eutectic Salt

Andrews

Phongikaroon

2018

J. Electrochem. Soc.

View full text Add to dashboard Cite

The exchange current density values (i 0 ) of the La/La 3+ in LiCl-KCl eutectic salts at different temperatures (723-798 K) and concentrations (0.229-0.597 mol%) were measured by using cyclic voltammetry (CV), linear polarization (LP), and Tafel methods. The Tafel i 0 values had the largest relative error on an average of 27%, while the LP values, found at the same scan rates, had a lower relative error, ranging from 10-17%. The LP and Tafel results were found to be highly affected by an unstable surface area. The CV i 0 values were less affected by this issue due to higher scan rates, mainly 50-200 mV s −1 . The relative error of CV was the least among the three, averaging 6.5-11%. Linear correlations for i 0 versus temperature and concentration were developed from these results.

show abstract

“…DREP is derived to use parameters, such as exchange current density and the mass transfer coefficient, with observed potential and current of the UNF electrorefining operation to determine the number of metals depositing and their individual deposition rates. The derivation of DREP has been presented elsewhere [18], but has yet to be compared to experimental results. DREP's key assumptions are a stable, well-defined diffusion layer and constant bulk concentration of each analyte over the duration of each current step cycle.…”

Section: Rcementioning

confidence: 99%

“…The superscript indicates the oxidized state. The expression in 7was derived elsewhere [18] and was modified slightly to better match IUPAC convention [45]. Therefore the previous expression was multiplied by negative one so that negative current indicated a cathodic current.…”

Section: Kinetic Parametersmentioning

confidence: 99%

Application of the rotating cylinder electrode in molten LiCl-KCl eutectic containing uranium(III)- and magnesium(II)-chloride

Rappleye

Simpson

2017

Journal of Nuclear Materials

Self Cite

View full text Add to dashboard Cite

The application of the rotating cylinder electrode (RCE) to molten LiCl-KCl eutectic mixtures for electroanlytical measurements is presented. This enabled the measurement of the limiting current which was observed to follow a linear trend with the rotational rate raised to 0.64-0.65 power on average, which closely agrees with existing RCE mass-transfer correlations. This is the first publication of electroanalytical RCE measurements in LiCl-KCl eutectic based molten salt mixtures, to our knowledge. These measurements were made in mixtures of molten LiCl-KCl eutectic containing UCl 3 and MgCl 2. Kinetic parameters were calculated for Mg 2+ in LiCl-KCl eutectic. The exchange current density (i o) of Mg 2+ deposition varied with mole fraction (x) according to i o (A cm-2) = 1.64x 0.689. The parameters from RCE measurements were also applied in an electrochemical co-deposition model entitled DREP to detect and predict the deposition rate of U and Mg. DREP succeeded in detecting the co-deposition of U and Mg, even when Mg constituted less than 0.5 wt% of the deposit.

show abstract

Simulated real-time process monitoring of a molten salt electrorefiner

Cited by 11 publications

References 16 publications

Measurement and Analysis of Exchange Current Density for U/U3+ Reaction in LiCl-KCl Eutectic Salt via Various Electrochemical Techniques

Measurement and Analysis of Exchange Current Density for U/U3+ Reaction in LiCl-KCl Eutectic Salt via Various Electrochemical Techniques

Comparison of Exchange Current Density Acquisition Methods for LaCl₃in Molten LiCl-KCl Eutectic Salt

Application of the rotating cylinder electrode in molten LiCl-KCl eutectic containing uranium(III)- and magnesium(II)-chloride

Contact Info

Product

Resources

About

Simulated real-time process monitoring of a molten salt electrorefiner

Cited by 11 publications

References 16 publications

Measurement and Analysis of Exchange Current Density for U/U3+ Reaction in LiCl-KCl Eutectic Salt via Various Electrochemical Techniques

Measurement and Analysis of Exchange Current Density for U/U3+ Reaction in LiCl-KCl Eutectic Salt via Various Electrochemical Techniques

Comparison of Exchange Current Density Acquisition Methods for LaCl3in Molten LiCl-KCl Eutectic Salt

Application of the rotating cylinder electrode in molten LiCl-KCl eutectic containing uranium(III)- and magnesium(II)-chloride

Contact Info

Product

Resources

About

Comparison of Exchange Current Density Acquisition Methods for LaCl₃in Molten LiCl-KCl Eutectic Salt