Publication date: 10th April 2024
Despite their relatively simple stoichiometries, compounds in the barium–group(V) oxide series Ba4M2O9 (M = V, Nb, Ta) adopt three distinct structure types depending on composition and synthetic conditions: a completely unique and complex γ phase; [1,2] a uniquely distorted 6H-perovskite; [3] and a partially disordered α phase related to Sr4Ru2O9-type. [4] They all hydrate to very high degrees of up to 1/3 (γ) or 1/2 (6H and α) H2O per formula unit and show appreciable mixed oxide/proton conductivity. Intriguingly, none of these structure types contain oxide vacancies that would explain their hydration and conductivity in terms of a conventional hydroxylation mechanism, nor layers for intercalation. We have used diffraction, electron microscopy, physical property measurements, NMR, inelastic neutron scattering and DFT calculations to show how water is incorporated into the crystal lattices in ways that depend upon and guide their temperature-dependent structural distortions. The potential significance of these results extends beyond their ionic conductivity to the Earth sciences, because even at ppm levels, the pressure- and temperature-dependencies of lattice hydration processes mean that they affect the total amount of water available on Earth and the rheological properties of the lithosphere (plate tectonics, earthquakes etc.).
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