Electrochemical and Thermodynamic Properties of U in LiCl-KCl-UCl{sub 3} salt system

Journal Article · Sat Jul 01 04:00:00 EDT 2017 · Transactions of the American Nuclear Society

OSTI ID:23047368

Yoon, Dalsung; Phongikaroon, Supathorn ^[1]

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1. Department of Mechanical and Nuclear Engineering, Virginia Commonwealth University, Richmond, VA 23284 (United States)

Pyro-processing technology has been considered and examined by several countries as a promising method for the recovery and recycle of uranium and actinide elements from used nuclear fuel. One of the key processes in pyro-processing is an electro-refiner (ER) where the metallic fission products are loaded into an anode basket and dissolved into lithium-potassium chloride (LiCl-KCl) eutectic salt at 773 K. Many researchers have been exploring the fundamental characterizations of U in LiCl-KCl system by using various electrochemical methods, resulting in several reported values of diffusion coefficient, apparent standard potential, and activity coefficient of U in the salt system. In addition, several researchers measured kinetic parameter of U (exchange current density, i{sub 0}) by using Tafel and linear polarization (LP) methods. Despite available data sets on this ternary salt system, there are discrepancies due to different experimental conditions, design, size of the cell, and measurement techniques. In addition, the i{sub 0} for U/U{sup 3+} reaction has only been measured since 2009; therefore, only few data sets are available to date although the i{sub 0} is critical for the development of dynamic ER model. The value of i{sub 0} is a kinetic characteristic in an ideal equilibrium state; therefore, it is very challenging to be measured by experiments. The authors have estimated the values of i{sub 0} via Tafel and linear polarization methods (LP); however, these methods are lack of maintaining electrode surface area during the measurements. In addition, some data are not following the trends from other literature studies due to its difficulties of the measurement. Therefore, further experimental determinations have to be accomplished to understand the i{sub 0} kinetics and the database for the i{sub 0} of U/U{sup 3+} couple in LiCl-KCl eutectic salt needs to be established systematically. In the present study, an experimental setup was designed and used in a consistent manner to build a meaningful database for U in LiCl-KCl system. LiCl-KCl-UCl{sub 3} salt was prepared at different concentrations and temperatures ranging from 0.5 wt% to 4 wt% and 723 K to 798 K, respectively. Then, CV, open circuit potential (OCP), and electrochemical impedance spectroscopy (EIS) were performed to understand the electrochemical, thermodynamic, and kinetic properties of U. Specially, i{sub 0} values have not been measured via EIS method; therefore, this study provides a good chance to confirm the i{sub 0} values with the new technique.

• OSTI ID: 23047368
• Journal Information: Transactions of the American Nuclear Society, Journal Name: Transactions of the American Nuclear Society Vol. 116; ISSN 0003-018X
• Country of Publication: United States
• Language: English

Related Subjects

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
ANODES
ELECTROCHEMISTRY
EUTECTICS
FISSION PRODUCTS
LITHIUM
LITHIUM CHLORIDES
MATERIALS RECOVERY
NUCLEAR FUELS
POLARIZATION
POTASSIUM CHLORIDES
REACTION KINETICS
SALTS
SPECTROSCOPY
THERMODYNAMIC ACTIVITY
THERMODYNAMIC PROPERTIES
THERMODYNAMICS
URANIUM
URANIUM CHLORIDES
URANIUM IONS