Abstract
AbstractA recent finding shows that lattice deformation could transform the mixed electronic/hydride (H−) conducting lanthanum trihydride (LaH3) to a superionic H− conductor. Such a feature would enable the development of a brand‐new all‐solid‐state hydride ion battery. It is essential to elucidate the mechanism of such a phenomenon. Here, we disclose an abnormal freezing effect on the electronic conductivity (σe) of the ball‐milled LaH3; that is, σe can be lowered by over 2 orders of magnitude upon a low‐temperature treatment. Low‐temperature Raman reveals that at low temperatures, lattice deformation has a noticeable influence on the interaction of hydrogen at octahedral (Ho) and tetrahedral (Ht) sites, which may play a crucial role in hindering electron conduction. This freezing effect can significantly improve the ionic transfer number of rare earth‐based H− conductors and provide a new direction to the development of solid electrolytes for low‐temperature all‐solid‐state batteries.
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