Highly Correlated Hydride Ion Tracer Diffusion in SrTiO_(3-x)H_x Oxyhydrides

摘要

Mixed oxide hydride anion systems constitute a novel class of materials exhibiting intriguing properties such as solid-state hydride ion conduction and fast anion exchange. In this contribution we derive the kinetics of hydride ion transport in a mixed oxide-hydride system, SrTiO3-xHx, through isotope exchange and depth profiling. Density functional theory (DFT) calculations indicate that migration of H- to neighboring vacant oxygen lattice sites is fast, but that long-range transport is impeded by slow reorganization of the oxygen sublattice. From measured hydride tracer-diffusion coefficients and the correlation factors derived from DFT, we are able to derive the hydrogen self-diffusion coefficients in SrTiO3-xHx. More generally, the explicit description of hydride ion transport in SrTiO3-xHx through combination of experimental and computational methods reported in this work can be applied to explore anion diffusion in other mixed anion systems.