Examination of the short-range structure of molten salts: ThF4, UF4, and related alkali actinide fluoride systems

J. A. Ocádiz-Flores; A. E. Gheribi; J. Vlieland; D. De Haas; K. Dardenne; J. Rothe; R. J.M. Konings; A. L. Smith

doi:10.1039/d1cp00566a

Examination of the short-range structure of molten salts: ThF₄, UF₄, and related alkali actinide fluoride systems

J. A. Ocádiz-Flores, A. E. Gheribi, J. Vlieland, D. De Haas, K. Dardenne, J. Rothe, R. J.M. Konings, A. L. Smith^*

^*Corresponding author for this work

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Abstract

The short-range structures of LiF-ThF4, NaF-AnF4, KF-AnF4, and Cs-AnF4 (An = Th, U), were probed using in situ high temperature Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy. Signally, the EXAFS spectra of pure molten ThF4 and UF4 were measured for the first time. The data were interpreted with the aid of Molecular Dynamics (MD) and standard fitting of the EXAFS equation. As in related studies, a speciation distribution dominated by [AnFx]4-x (x = 7, 8, 9) coordination complexes was observed. The average coordination number was found to decrease with the increasing size of the alkali cation, and increase with AnF4 content. An average coordination number close to 6, which had not been detected before in melts of alkali actinide fluorides, was seen when CsF was used as solvent. This journal is

Original language	English
Pages (from-to)	11091-11103
Number of pages	13
Journal	Physical Chemistry Chemical Physics
Volume	23
Issue number	18
DOIs	https://doi.org/10.1039/d1cp00566a
Publication status	Published - 2021

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title = "Examination of the short-range structure of molten salts: ThF4, UF4, and related alkali actinide fluoride systems",

abstract = "The short-range structures of LiF-ThF4, NaF-AnF4, KF-AnF4, and Cs-AnF4 (An = Th, U), were probed using in situ high temperature Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy. Signally, the EXAFS spectra of pure molten ThF4 and UF4 were measured for the first time. The data were interpreted with the aid of Molecular Dynamics (MD) and standard fitting of the EXAFS equation. As in related studies, a speciation distribution dominated by [AnFx]4-x (x = 7, 8, 9) coordination complexes was observed. The average coordination number was found to decrease with the increasing size of the alkali cation, and increase with AnF4 content. An average coordination number close to 6, which had not been detected before in melts of alkali actinide fluorides, was seen when CsF was used as solvent. This journal is ",

author = "Oc{\'a}diz-Flores, {J. A.} and Gheribi, {A. E.} and J. Vlieland and {De Haas}, D. and K. Dardenne and J. Rothe and Konings, {R. J.M.} and Smith, {A. L.}",

year = "2021",

doi = "10.1039/d1cp00566a",

language = "English",

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T2 - ThF4, UF4, and related alkali actinide fluoride systems

AU - Ocádiz-Flores, J. A.

AU - Gheribi, A. E.

AU - Vlieland, J.

AU - De Haas, D.

AU - Dardenne, K.

AU - Rothe, J.

AU - Konings, R. J.M.

AU - Smith, A. L.

PY - 2021

Y1 - 2021

N2 - The short-range structures of LiF-ThF4, NaF-AnF4, KF-AnF4, and Cs-AnF4 (An = Th, U), were probed using in situ high temperature Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy. Signally, the EXAFS spectra of pure molten ThF4 and UF4 were measured for the first time. The data were interpreted with the aid of Molecular Dynamics (MD) and standard fitting of the EXAFS equation. As in related studies, a speciation distribution dominated by [AnFx]4-x (x = 7, 8, 9) coordination complexes was observed. The average coordination number was found to decrease with the increasing size of the alkali cation, and increase with AnF4 content. An average coordination number close to 6, which had not been detected before in melts of alkali actinide fluorides, was seen when CsF was used as solvent. This journal is

AB - The short-range structures of LiF-ThF4, NaF-AnF4, KF-AnF4, and Cs-AnF4 (An = Th, U), were probed using in situ high temperature Extended X-ray Absorption Fine Structure (EXAFS) spectroscopy. Signally, the EXAFS spectra of pure molten ThF4 and UF4 were measured for the first time. The data were interpreted with the aid of Molecular Dynamics (MD) and standard fitting of the EXAFS equation. As in related studies, a speciation distribution dominated by [AnFx]4-x (x = 7, 8, 9) coordination complexes was observed. The average coordination number was found to decrease with the increasing size of the alkali cation, and increase with AnF4 content. An average coordination number close to 6, which had not been detected before in melts of alkali actinide fluorides, was seen when CsF was used as solvent. This journal is

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SN - 1463-9076

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JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

IS - 18

ER -

Examination of the short-range structure of molten salts: ThF₄, UF₄, and related alkali actinide fluoride systems

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