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Experimental investigation and thermodynamic assessment of the BaCl₂–CeCl₃ system

Alders, D.C. (author), Vlieland, J. (author), Thijs, M.A. (author), Konings, R. (author), Smith, A.L. (author)

The thermodynamic and thermo-physical properties of the molten salt system [Formula presented] have been investigated using an experimental and modelling approach. This molten salt system includes a single intermediate compound [Formula presented], whose structure has been investigated using X-ray and neutron diffraction. Furthermore, this...

journal article 2024

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Low-Temperature Heat Capacity of CsPbI₃, Cs₄PbI₆, and Cs₃Bi₂I₉

van Hattem, A. (author), Griveau, Jean Christophe (author), Colineau, Eric (author), Lefering, A.J.E. (author), Konings, R. (author), Smith, A.L. (author)

The heat capacities of CsPbI₃, Cs₄PbI₆, and Cs₃Bi₂I₉ were studied using low-temperature thermal relaxation calorimetry in the temperature range of 1.9-300 K. The three compounds are insulators, with no electronic contribution to the heat capacity. None of them show detectable...

journal article 2023

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Structural Studies and Thermal Analysis in the Cs₂MoO₄-PbMoO₄ System with Elucidation of β-Cs₂Pb(MoO₄)₂

van Hattem, A. (author), Vlieland, J. (author), Dankelman, B.J.R. (author), Thijs, M.A. (author), Wallez, Gilles (author), Dardenne, Kathy (author), Rothe, Jörg (author), Konings, R. (author), Smith, A.L. (author)

The quaternary compound Cs₂Pb(MoO₄)₂ was synthesized and its structure was characterized using X-ray and neutron diffraction from 298 to 773 K, while thermal expansion was studied from 298 to 723 K. The crystal structure of the high-temperature phase β-Cs₂Pb(MoO₄)₂ was...

journal article 2023

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Ternary System CsI-PbI₂-BiI₃ and Thermodynamic Stability of Cesium Metal Halide Perovskites

van Hattem, A. (author), Alders, D.C. (author), Konings, R. (author), Smith, A.L. (author)

The thermochemistry of the ternary system CsI-PbI₂-BiI₃, of interest for applications in photovoltaics, memory devices, and nuclear applications, among other things, is investigated in this work. The binary phase diagrams CsI-PbI₂ and CsI-BiI₃ were subjected to renewed experimental investigation,...

journal article 2023

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Correction: Ocádiz Flores et al. Thermodynamic Description of the ACl-ThCl4 (A = Li, Na, K) Systems: Thermodynamic Description of the ACl-ThCl4 (A = Li, Na, K) Systems (Thermo, (2021), 1, 2, (122-133), 10.3390/thermo1020009)

Ocadiz flores, J.A. (author), Rooijakkers, B.A.S. (author), Konings, R. (author), Smith, A.L. (author)

Corrected excess Gibbs energies of the liquid solutions in the ACl-ThCl4 (A = Li, Na, K), as well as revised standard enthalpies of formation and standard entropies of the intermediate phases occurring in the binary systems, are presented. The phase diagrams are reproduced to a similar level of accuracy as in the original publication, and the...

journal article 2022

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Using the Quasi-chemical formalism beyond the phase Diagram: Density and viscosity models for molten salt fuel systems

Ocadiz flores, J.A. (author), Konings, R. (author), Smith, A.L. (author)

CALPHAD models to compute the density and viscosity of four keystone systems related to Molten Salt Reactor (MSR) technology have been optimized: NaCl-UCl₃, LiF-ThF₄, LiF-UF₄, and LiF-ThF₄-UF₄. Revised thermodynamic assessments of all four systems, using the modified quasichemical...

journal article 2022

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A promising fuel for fast neutron spectrum Molten Salt Reactor: NaCl-ThCl₄-PuCl₃

Dumaire, T. (author), Ocadiz flores, J.A. (author), Konings, R. (author), Smith, A.L. (author)

Chloride salts are considered a good alternative to fluoride salts as fuel carrier in the Molten Salt Fast Reactor concepts. The NaCl–ThCl4–PuCl3 fuel salt solution seems very promising, with low melting temperature eutectic compositions, and the potential to be used in a breeder and burner type of reactor design. This work focuses on the...

journal article 2022

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New insights and coupled modelling of the structural and thermodynamic properties of the LiF-UF4 system

Ocadiz flores, J.A. (author), Gheribi, A. E. (author), Vlieland, J. (author), Dardenne, K. (author), Rothe, J. (author), Konings, R. (author), Smith, A.L. (author)

© 2021 The Authors LiF-UF4 is a key binary system for molten fluoride reactor technology, which has not been scrutinized as thoroughly as the closely related LiF-ThF4 system. The phase diagram equilibria in the system LiF-UF4 are explored in this work with X-ray diffraction (XRD) and differential scanning calorimetry (DSC). The short-range...

journal article 2021

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Thermodynamic Description of the ACl-ThCl4 (A = Li, Na, K) Systems

Ocadiz flores, J.A. (author), Rooijakkers, B.A.S. (author), Konings, R. (author), Smith, A.L. (author)

The ACl-ThCl (Formula presented.) (A = Li, Na, K) systems could be of relevance to the nuclear industry in the near future. A thermodynamic investigation of the three binary systems is presented herein. The excess Gibbs energy of the liquid solutions is described using the quasi-chemical formalism in the quadruplet approximation. The phase...

journal article 2021

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

Ocadiz flores, J.A. (author), Gheribi, A. E. (author), Vlieland, J. (author), de Haas, D.W. (author), Dardenne, K. (author), Rothe, J. (author), Konings, R. (author), Smith, A.L. (author)

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 ...

journal article 2021

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Experimental and Computational Exploration of the NaF-ThF₄Fuel System: Structure and Thermochemistry

Schreuder, Maarten B.J.W. (author), Ocadiz flores, J.A. (author), Gheribi, Aimen E. (author), Beneš, Ondrej (author), Griveau, Jean Christophe (author), Colineau, Eric (author), Konings, R. (author), Smith, A.L. (author)

The structural, thermochemical, and thermophysical properties of the NaF-ThF4 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...

journal article 2021

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Experimental studies and thermodynamic assessment of the Ba-Mo-O system by the CALPHAD method

Smith, A.L. (author), Rutten, M. (author), Herrmann, L. (author), Epifano, E. (author), Konings, R. (author), Colineau, E. (author), Griveau, J. C. (author), Guéneau, C. (author), Dupin, N. (author)

Thermodynamic measurements on BaMoO₄, BaMoO₃ and BaMo₃O₁₀ are reported, that served as input for the development of a thermodynamic model of the Ba-Mo-O system using the CALPHAD methodology. The valence states of molybdenum in BaMoO₄ and BaMoO₃ were confirmed to be VI and IV,...

journal article 2021

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A new approach for coupled modelling of the structural and thermo-physical properties of molten salts. Case of a polymeric liquid LiF-BeF₂

Smith, A.L. (author), Capelli, E. (author), Konings, R. (author), Gheribi, A. E. (author)

The (Li,Be)F_x fluoride salt is an ionic liquid with complex non-ideal thermodynamic behaviour due to the formation of short-range order. In this work, we explore the relationship between local structure, thermo-physical and thermodynamic properties in this system using a multidisciplinary approach that couples molecular dynamics...

journal article 2020

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Structural and thermodynamic study of Cs₃Na(MoO₄)₂: Margin to the safe operation of sodium cooled fast reactors

Smith, A.L. (author), Kauric, G.P.T.F. (author), van Eijck, L. (author), Goubitz, K. (author), Clavier, N. (author), Wallez, G. (author), Konings, R. (author)

Neutron diffraction measurements of the double molybdate Cs₃Na(MoO₄)₂ have been performed for the first time in this work and the crystal structure refined using the Rietveld method. The thermal expansion of this trigonal phase, in space group P3¯m1, measured using high temperature X-ray diffraction (XRD),...

journal article 2019

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Thermodynamic assessment of the LiF-NiF₂, NaF-NiF₂ and KF-NiF₂ systems

Ocadiz flores, J.A. (author), Capelli, E. (author), Raison, P. E. (author), Konings, R. (author), Smith, A.L. (author)

Using the modified quasi-chemical model in the quadruplet approximation, three new thermodynamic assessments of binary systems useful for the detailed operational design of the Molten Salt Reactor are presented: AF-NiF₂ (A = Li, Na, K). These systems are particularly relevant for the study of the molten salt-structural materials...

journal article 2018

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Thermodynamic study of Cs3Na(MoO4)2: Determination of the standard enthalpy of formation and standard entropy at 298.15 K

Smith, A.L. (author), Pignié, M.C.F.C.O. (author), van Eijck, L. (author), Griveau, Jean Christophe (author), Colineau, Eric (author), Konings, R. (author)

The enthalpy of formation at 298.15 K and low temperature heat capacity of Cs3Na(MoO4)2 have been measured for the first time in this work using solution calorimetry and thermal-relaxation calorimetry in the temperature range T = (1.9–299.6) K, respectively. The solution calorimetry measurements, performed in 2 M HNO3 solution, have yielded an...

journal article 2018

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Thermodynamic assessment of the Na-O and Na-U-O systems: Margin to the safe operation of SFRs

Smith, A.L. (author), Guéneau, C (author), Flèche, J. L. (author), Chatain, S. (author), Beneš, O. (author), Konings, R. (author)

A thermodynamic model for the Na-O system was developed for the first time using the CALPHAD method after review of the structural, thermodynamic, and phase diagram data available on this system. Differential Scanning Calorimetry measurements were moreover performed to assess the phase equilibria and liquidus temperature in the Na<sub>2</sub...

journal article 2017

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A New Look at the Structural and Magnetic Properties of Potassium Neptunate K₂NpO₄ Combining XRD, XANES Spectroscopy, and Low-Temperature Heat Capacity

Smith, A.L. (author), Colineau, Eric (author), Griveau, Jean Christophe (author), Popa, Karin (author), Kauric, Guilhem (author), Martin, Philippe M. (author), Scheinost, Andreas C. (author), Cheetham, Anthony K. (author), Konings, Rudy J.M. (author)

The physicochemical properties of the potassium neptunate K₂NpO₄ have been investigated in this work using X-ray diffraction, X-ray absorption near edge structure (XANES) spectroscopy at the Np-L₃ edge, and low-temperature heat capacity measurements. A Rietveld refinement of the crystal structure is reported...

journal article 2017

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Structural Properties and Charge Distribution of the Sodium Uranium, Neptunium, and Plutonium Ternary Oxides: A Combined X-ray Diffraction and XANES Study

Smith, A.L. (author), Martin, Philippe M. (author), Prieur, Damien (author), Scheinost, Andreas C. (author), Raison, Philippe E. (author), Cheetham, Anthony K. (author), Konings, R. (author)

The charge distributions in α-Na₂UO₄, Na₃NpO₄, α-Na₂NpO₄, Na₄NpO₅, Na₅NpO₆, Na₂PuO₃, Na₄PuO₅, and Na₅PuO₆ are investigated in this work using X-ray absorption near-edge...

journal article 2016

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Mössbauer spectroscopy, magnetization, magnetic susceptibility, and low temperature heat capacity of α-Na₂NpO₄

Smith, A.L. (author), Hen, Amir (author), Magnani, Nicola (author), Sanchez, Jean Pierre (author), Colineau, Eric (author), Griveau, Jean Christophe (author), Raison, Philippe E. (author), Caciuffo, Roberto (author), Konings, R. (author), Cheetham, Anthony K. (author)

The physical and chemical properties at low temperatures of hexavalent disodium neptunate α-Na₂NpO₄ are investigated for the first time in this work using Mössbauer spectroscopy, magnetization, magnetic susceptibility, and heat capacity measurements. The Np(VI) valence state is confirmed by the isomer shift value of the...

journal article 2016