Fluorine Substitution in Magnesium Hydride as a Tool for Thermodynamic Control
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© 2020 American Chemical Society.
Metal hydrides continue to vie for attention as materials in multiple technological applications including hydrogen storage media, thermal energy storage (TES) materials, and hydrogen compressors. These applications depend on the temperature at which the materials desorb and reabsorb hydrogen. Magnesium hydride is ideal as a TES material, although its practical operating temperature is capped at ∼450 °C because of material degradation and high operating pressure. Fluorine substitution for hydrogen in magnesium hydride has previously been shown to increase the operating temperature of the metal hydride while limiting degradation, although full characterization is required before technological application can be ensured. The present study characterizes Mg(HxF1-x)2 solid solutions (x = 1, 0.95, 0.70, 0.85, 0.50, and 0) by inelastic neutron spectroscopy, powder X-ray diffraction, and thermal conductivity measurements, with the results being verified by density functional theory. For each experiment, a clear trend is observed throughout a series of solid solutions, showing the possibility of tuning the properties of MgH2. As F- substitution increases, the average Mg-H(F) bond distance elongates along the axial positions of the Mg-H(F) octahedra. Overall, this leads to an increase in Mg-H bond strength and thermal stability, improving the viability of Mg-H-F as potential TES materials.
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