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Passivation of magnesium metal anode is one of the critical challenges for the development of magnesium batteries. Here we investigated the passivation process of an intermetallic anode: Mg 3 Bi 2  synthesized by solid-state and thin film process. The Mg 3 Bi 2  composite electrode shows excellent reversibility in magnesium bis(trifluoromethansulfonylamide) dissolved in acetonitrile, while Mg 3 Sb 2 , which has same crystal structure and similar chemical properties, is electrochemically inactive. We also fabricated the Mg 3 Bi 2  thin film electrodes, which show reversibility with low overpotential not only in the acetonitrile solution but also glyme-based solutions. Surface layer corresponding to the decomposed TFSA anion is slightly suppressed in the case of the Mg 3 Bi 2  thin film electrode, compared with Mg metal. Comparative study of hydrolysis process of the Mg 3 Bi 2  and the Mg 3 Sb 2  suggests that the both intermetallic anodes are not completely passivated. The bond valence sum mapping of the Mg 3 Bi 2  indicates that the fast Mg 2+  diffusion pathway between 2 d  tetrahedral sites is formed. The electrochemical properties of the Mg 3 Bi 2  anode is mainly due to the less passivation surface with the fast Mg 2+  diffusion pathways.

Destabilized Passivation Layer on Magnesium-Based Intermetallics as Potential Anode Active Materials for Magnesium Ion Batteries