Pressure-induced transition from pure electronic to mixed ionic-electronic conduction in strontium hydride

The heavier alkaline-earth hydrides AeH2 (Ae = Ca, Sr, and Ba) are considered as promising materials for hydrogen energy storage. Pressure-induced structural changes in AeH2 materials could improve hydrogen transport properties and result in a better understanding of the structure-property relationship. In this work, pressure evolution of carrier transport properties of SrH2 was investigated using impedance spectroscopy measurements at room temperature and first-principles calculations. The pressure-induced structure phase transition from a Pnma phase to a P63/mmc phase was accompanied by a transition from pure electronic conduction to mixed ionic-electronic conduction, which was related to the ionic migration barrier energy. In the P63/mmc phase, the H− ionic and electronic resistances of bulk and grain boundaries were distinguished, respectively. The total resistance of SrH2 decreased by about four orders of magnitude after the phase transition. This work provides critical insight into the structure-conduction relationship and the role of grain boundaries in the transport process of alkaline-earth hydrides under high pressure.