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Molten fluoride salts such as Li₂BeF₄ (FLiBe) are used in molten salt reactors, fluoride-salt-cooled high-temperature reactors and fusion reactors as a fuel solvent, coolant and/or tritium breeding medium. In engineered systems that use molten salt, solid-state material will be present during melting and freezing scenarios, and therefore the temperature-dependent properties of the solid and solid/liquid phase transition merit investigation. To observe the behavior of the solid state of Li₂BeF₄ from room temperature to melting, this work used neutron and X-ray diffraction to measure the changes in the lattice parameters and volume of the crystalline unit cell and compared the resultsmore » with prior low-temperature data for solid Li₂BeF₄. From neutron diffraction data it is also possible to identify anisotropy: centimetre-scaled crystals align preferentially with the a axes parallel to the direction of freezing front propagation, and the c axes expand 54% more than the a axes. This work provides the lattice constants as a function of temperature, quantifies the thermal expansion, and determines the equation describing the change in density for solid Li₂BeF₄ from room temperature to 459°C to be ρ_solid (kg m⁻³) = 2182 (3) − 0.115 (2) T (°C) and the volume expansion upon melting to be less than 5%. Furthermore, this density changes depending on molecular weight and enrichment.« less

The use of molten salts as coolants, fuels, and tritium breeding blankets in the next generation of fission and fusion nuclear reactors benefits from furthering the characterization of the molecular structure of molten halide salts, paving the way to predictive capability of the chemical and thermophysical properties of molten salts. Due to its neutronic, chemical, and thermochemical properties, 2 $\mathrm{Li}\mathrm{F}$ - $\mathrm{Be}\mathrm{F}$ ${}_2$ is a candidate molten salt for several fusion- and fission-reactor designs. We performed neutron and x-ray total-scattering measurements tomore » determine the atomic structure of liquid 2 $\mathrm{Li}\mathrm{F}$ - $\mathrm{Be}\mathrm{F}$ ${}_2$ . We also performed and neural-network molecular-dynamics simulations to predict the structure obtained by neutron- and x-ray-diffraction experiments. The use of machine learning provides improvements to the efficiency in predicting the structure at a longer length scales than is achievable with simulations at significantly lower computational expense while retaining near accuracy. We found that the NNMD simulations accurately predicted the ${\mathrm{Be}\mathrm{F}}_4^{2-}$ oligomer formations seen in the experimental first-structure-factor peak. Our combination of high-resolution measurements with large-scale molecular dynamics provided an avenue to explore and experimentally verify the intermediate-range ordering beyond the first-nearest neighbor that has posed too many experimental and computational challenges in previous works. With a deeper understanding of the salt structure and ion ordering, the evolution of salt chemistry over the lifetime of a reactor can be better predicted, which is crucial to the licensing and operation of advanced fission and fusion reactors that employ molten salts. To this end, this work will serve as a reference for future studies of salt structure and macroscopic properties with and without the addition of solutes. Published by the American Physical Society 2024« less