Publication date: 10th April 2024
The development of solid state battery has been witnessed an increasing demand owing to the merits of solid electrolytes, including the intrinsic safety to avoid thermal runaway, the superior mechanical properties to suppress bidirectional crosstalk inside the batteries, and the high transference number to eliminate the concentration polarization at high current densities.[1] Apart from the lithium battery technologies, magnesium batteries using multivalent cations as charge carriers are also of great research interest due to the high earth abundance of magnesium source, and high theoretical energy density given by multi-electron redox reactions.[2] Nevertheless, the large charge density of Mg2+ cations inevitably causes sluggish kinetics of the ion migration, compared to the lithium counterpart.[3] A solid electrolyte material with high ionic conductivity, is thus the prerequisite for the development of solid state Mg batteries. In this study, we prepared a new Mg-ion conducting NASICON-structured material, Mg0.5Sn2(PO4)3.[4] By combining it with a small amount of Mg ionic liquid to improve the Mg2+ migration at grain boundary, the prepared Mg-ion conducting hybrid solid electrolyte shows superior room-temperature ionic conductivity of 1.1 · 10–4 S cm–1 and an activation energy of 0.36 eV. Reversible Mg plating/stripping is realized at room temperature with stable cycling performance. Surface analysis demonstrates a stable interface between the electrolyte and Mg metal anode, suggesting good compatibility. Using in situ electrochemical scanning electron microscopy, for the first time we observed the room temperature Mg growth inside a solid-state cell by the evidence of clear-cut metal particle formation and electrolyte particle cracking. The key parameters that affect the Mg metal deposition properties are also explored. The results shown here can act as a good starting point for the understanding of Mg transport behavior in solid-state batteries.
This work was funded by the German Research Foundation (DFG) under Project ID 390874152 (POLiS Cluster of Excellence).
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