Development of Pyrochemical Separation Processes for Recovery of Actinides from Spent Nuclear Fuel in Molten LiCl-KCl

Glatz, Jean‐Paul; Malmbeck, Rikard; Souček, P.; Claux, Benoît; Meier, Roland; Ougier, Michel; Murakami, Teppei

doi:10.1016/b978-0-12-398538-5.00026-3

Cited by 24 publications

(22 citation statements)

References 38 publications

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“…Curve (2) shows the electrochemical spectra obtained at the interface between the LiCl-KCl melt and liquid metal in absence of TbCl 3 . Scan rate: 0.075 V s-1; temperature 723 K.…”

Section: Resultsmentioning

confidence: 99%

“…TbðIIIÞ þ Cdþ3e À $Tb ðin liquid CdÞ (2) The potential shift of the electrochemical system in the positive direction compared with the reduction potential Tb(III)/Tb at the inert electrode, it is due to a lowering of the activity of the dissolved Tb metal in the Cd phase as described in equation (3) [ ( F i g . _ 1 ) T D $ F I G ] …”

Section: Resultsmentioning

confidence: 99%

“…In this way, partitioning and transmutation (P&T) of Minor Actinides (MAs) and Long-Lived Fission Products (LLFP) arising out of the back-end of the fuel cycle would be one of the key-steps in any future sustainable nuclear fuel cycle [1,2] Pyrochemical separation methods, using molten chloride or fluoride electrolyte systems, would form a critical stage of P&T by recovering long-lived elements and thus reducing the radiotoxicity and volume of the nuclear wastes [2]. To this end, research and development is needed for molten salt electrorefining, electroextraction with inert and reactive cathodes, as well as reductive extraction process that are foreseen as partitioning methods for irradiated nuclear fuel [2][3][4][5][6][7][8][9][10][11].…”

Section: Introductionmentioning

confidence: 99%

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Electrochemical behaviour of terbium in the eutectic LiCl-KCl in Cd liquid electrodes.- Evaluation of the thermochemical properties of the TbCdx intermetallic compounds

Castrillejo

Hernández

Fernández

et al. 2014

Electrochimica Acta

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“…Curve (2) shows the electrochemical spectra obtained at the interface between the LiCl-KCl melt and liquid metal in absence of TbCl 3 . Scan rate: 0.075 V s-1; temperature 723 K.…”

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Electrochemical behaviour of terbium in the eutectic LiCl-KCl in Cd liquid electrodes.- Evaluation of the thermochemical properties of the TbCdx intermetallic compounds

Castrillejo

Hernández

Fernández

et al. 2014

Electrochimica Acta

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“…(ii) The compact equipment and recyclability of the molten salt lead to cost-effective reduction of radioactive waste from the process. (iii) The incapability to recover pure plutonium with a liquid electrode fulfills proliferation resistance. − Therefore, further development of the pyrochemical process is crucial to achieving a closed fuel cycle that aims to reduce the volume and long-term radiotoxicity of spent nuclear fuel as well as attain sustainable nuclear energy.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical Formation of Divalent Samarium Cation and Its Characteristics in LiCl–KCl Melt

et al. 2018

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The electrochemical reduction of trivalent samarium in a LiCl-KCl eutectic melt produced highly stable divalent samarium, whose electrochemical properties and electronic structure in the molten salt were investigated using cyclic voltammetry, UV-vis absorption spectroscopy, laser-induced emission spectroscopy, and density functional theory (DFT) calculations. Diffusion coefficients of Sm and Sm were electrochemically measured to be 0.92 × 10 and 1.10 × 10 cm/s, respectively, and the standard apparent potential of the Sm couple was estimated to be -0.82 V vs Ag|Ag at 450 °C. The spectroelectrochemical study demonstrated that the redox behavior of the samarium cations obeys the Nernst equation ( E°' = -0.83 V, n = 1) and the trivalent samarium cation was successfully converted to the divalent cation having characteristic absorption bands at 380 and 530 nm with molar absorptivity values of 1470 and 810 M cm, respectively. Density function theory calculations for the divalent samarium complex revealed that the absorption signals originated from the 4f to 4f5d transitions. Additionally, laser-induced emission measurements for the Sm cations in the LiCl-KCl matrix showed that the Sm ion in the LiCl-KCl melt at 450 °C emitted an orange color of fluorescence, whereas a red colored emission was observed from the Sm ion in the solidified LCl-KCl salt at room temperature.

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“…The excellent chemical, radiochemical, and thermal stabilities, together with their high heat capacities, high boiling points, and low vapor pressure, make MSs an excellent choice as coolants and/or fuels in nuclear reactors. , Spent nuclear fuel reprocessing is another important nuclear application of MSs mostly due to their low chemical sensitivity to high levels of radiation and proliferation resistance . Currently, our knowledge of these systems is limited; therefore, a better understanding of the molecular properties of Ans in MSs is key toward fundamental insights and maximizing their practical use in many modern materials and processes. ,− …”

Section: Introductionmentioning

confidence: 99%

Actinide Molten Salts: A Machine-Learning Potential Molecular Dynamics Study

Nguyen

Rousseau

Paviet

et al. 2021

ACS Appl. Mater. Interfaces

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Actinide molten salts represent a class of important materials in nuclear energy. Understanding them at a molecular level is critical for the proper and optimal design of relevant technological applications. Yet, owing to the complexity of electronic structure due to the 5f orbitals, computational studies of heavy elements in condensed phases using ab initio potentials to study the structure and dynamics of these elements embedded in molten salts are difficult. This lack of efficient computational protocols makes it difficult to obtain information on properties that require extensive statistical sampling like transport properties. To tackle this problem, we adopted a machine-learning approach to study ThCl 4 −NaCl and UCl 3 −NaCl binary systems. The machine-learning potential with the density functional theory accuracy allows us to obtain long molecular dynamics trajectories (ns) for large systems (10 3 atoms) at a considerably low computing cost, thereby efficiently gaining information about their bonding structures, thermodynamics, and dynamics at a range of temperatures. We observed a considerable change in the coordination environments of actinide elements and their characteristic coordination sphere lifetime. Our study also suggests that actinides in molten salts may not follow well-known entropyscaling laws.

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Development of Pyrochemical Separation Processes for Recovery of Actinides from Spent Nuclear Fuel in Molten LiCl-KCl

Cited by 24 publications

References 38 publications

Electrochemical behaviour of terbium in the eutectic LiCl-KCl in Cd liquid electrodes.- Evaluation of the thermochemical properties of the TbCdx intermetallic compounds

Electrochemical behaviour of terbium in the eutectic LiCl-KCl in Cd liquid electrodes.- Evaluation of the thermochemical properties of the TbCdx intermetallic compounds

Electrochemical Formation of Divalent Samarium Cation and Its Characteristics in LiCl–KCl Melt

Actinide Molten Salts: A Machine-Learning Potential Molecular Dynamics Study

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