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Experimental and Computational Exploration of the NaF–ThF(4) Fuel System: Structure and Thermochemistry

[Image: see text] The structural, thermochemical, and thermophysical properties of the NaF–ThF(4) fuel system were studied with experimental methods and molecular dynamics (MD) simulations. Equilibrium MD (EMD) simulations using the polarizable ion model were performed to calculate the density, mola...

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Autores principales: Schreuder, Maarten B. J. W., Ocádiz Flores, Jaén A., Gheribi, Aimen E., Beneš, Ondrej, Griveau, Jean-Christophe, Colineau, Eric, Konings, Rudy J. M., Smith, Anna Louise
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2021
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8350910/
https://www.ncbi.nlm.nih.gov/pubmed/34318676
http://dx.doi.org/10.1021/acs.jpcb.1c04830
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author Schreuder, Maarten B. J. W.
Ocádiz Flores, Jaén A.
Gheribi, Aimen E.
Beneš, Ondrej
Griveau, Jean-Christophe
Colineau, Eric
Konings, Rudy J. M.
Smith, Anna Louise
author_facet Schreuder, Maarten B. J. W.
Ocádiz Flores, Jaén A.
Gheribi, Aimen E.
Beneš, Ondrej
Griveau, Jean-Christophe
Colineau, Eric
Konings, Rudy J. M.
Smith, Anna Louise
author_sort Schreuder, Maarten B. J. W.
collection PubMed
description [Image: see text] The structural, thermochemical, and thermophysical properties of the NaF–ThF(4) fuel system were studied with experimental methods and molecular dynamics (MD) simulations. Equilibrium MD (EMD) simulations using the polarizable ion model were performed to calculate the density, molar volume, thermal expansion, mixing enthalpy, heat capacity, and distribution of [ThF(n)](m−) complexes in the (Na,Th)F(x) melt over the full concentration range at various temperatures. The phase equilibria in the 10–50 mol % ThF(4) and 85–95 mol % ThF(4) regions of the NaF–ThF(4) phase diagram were measured using differential scanning calorimetry, as were the mixing enthalpies at 1266 K of (NaF/ThF(4)) = (0.8:0.2), (0.7:0.3) mixtures. Furthermore, the β-Na(2)ThF(6) and NaTh(2)F(9) compounds were synthesized and subsequently analyzed with the use of X-ray diffraction. The heat capacities of both compounds were measured in the temperature ranges (2–271 K) and (2–294 K), respectively, by thermal relaxation calorimetry. Finally, a CALPHAD model coupling the structural and thermodynamic data was developed using both EMD and experimental data as input and a quasichemical formalism in the quadruplet approximation. Here, 7- and 8-coordinated Th(4+) cations were introduced on the cationic sublattice alongside a 13-coordinated dimeric species to reproduce the chemical speciation, as calculated by EMD simulations and to provide a physical description of the melt.
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spelling pubmed-83509102021-08-10 Experimental and Computational Exploration of the NaF–ThF(4) Fuel System: Structure and Thermochemistry Schreuder, Maarten B. J. W. Ocádiz Flores, Jaén A. Gheribi, Aimen E. Beneš, Ondrej Griveau, Jean-Christophe Colineau, Eric Konings, Rudy J. M. Smith, Anna Louise J Phys Chem B [Image: see text] The structural, thermochemical, and thermophysical properties of the NaF–ThF(4) fuel system were studied with experimental methods and molecular dynamics (MD) simulations. Equilibrium MD (EMD) simulations using the polarizable ion model were performed to calculate the density, molar volume, thermal expansion, mixing enthalpy, heat capacity, and distribution of [ThF(n)](m−) complexes in the (Na,Th)F(x) melt over the full concentration range at various temperatures. The phase equilibria in the 10–50 mol % ThF(4) and 85–95 mol % ThF(4) regions of the NaF–ThF(4) phase diagram were measured using differential scanning calorimetry, as were the mixing enthalpies at 1266 K of (NaF/ThF(4)) = (0.8:0.2), (0.7:0.3) mixtures. Furthermore, the β-Na(2)ThF(6) and NaTh(2)F(9) compounds were synthesized and subsequently analyzed with the use of X-ray diffraction. The heat capacities of both compounds were measured in the temperature ranges (2–271 K) and (2–294 K), respectively, by thermal relaxation calorimetry. Finally, a CALPHAD model coupling the structural and thermodynamic data was developed using both EMD and experimental data as input and a quasichemical formalism in the quadruplet approximation. Here, 7- and 8-coordinated Th(4+) cations were introduced on the cationic sublattice alongside a 13-coordinated dimeric species to reproduce the chemical speciation, as calculated by EMD simulations and to provide a physical description of the melt. American Chemical Society 2021-07-28 2021-08-05 /pmc/articles/PMC8350910/ /pubmed/34318676 http://dx.doi.org/10.1021/acs.jpcb.1c04830 Text en © 2021 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/).
spellingShingle Schreuder, Maarten B. J. W.
Ocádiz Flores, Jaén A.
Gheribi, Aimen E.
Beneš, Ondrej
Griveau, Jean-Christophe
Colineau, Eric
Konings, Rudy J. M.
Smith, Anna Louise
Experimental and Computational Exploration of the NaF–ThF(4) Fuel System: Structure and Thermochemistry
title Experimental and Computational Exploration of the NaF–ThF(4) Fuel System: Structure and Thermochemistry
title_full Experimental and Computational Exploration of the NaF–ThF(4) Fuel System: Structure and Thermochemistry
title_fullStr Experimental and Computational Exploration of the NaF–ThF(4) Fuel System: Structure and Thermochemistry
title_full_unstemmed Experimental and Computational Exploration of the NaF–ThF(4) Fuel System: Structure and Thermochemistry
title_short Experimental and Computational Exploration of the NaF–ThF(4) Fuel System: Structure and Thermochemistry
title_sort experimental and computational exploration of the naf–thf(4) fuel system: structure and thermochemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8350910/
https://www.ncbi.nlm.nih.gov/pubmed/34318676
http://dx.doi.org/10.1021/acs.jpcb.1c04830
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