Publication date: 10th April 2024
According to increasing demands for both high energy density and safety, solid electrolytes have been attracted to them. In the various types of solid electrolytes, the study of sulfide solid electrolytes including Li6PS5X (X = CI, Br, and I) and Li10GePS12 have been widely progressed due to their high Li ionic conductivity and processability. However, because of their poor oxidation stability them, the undesirable interfacial reaction, which deteriorates cell performance, occurs, so it should be needed to develop new types of solid electrolytes.
Herein, the halide solid electrolytes, Li3MX6 (M = Sc, Y, In, Er, X= CI, Br) have garnered increasing interest for their relatively good ionic conductivity, and oxidation stability. However, the cost of trivalent metals in Li3MX6 is high to apply large-scale industrial level, and the compositional effects on ionic conductivity are unclear in halide solid electrolytes. Also, previously reported Li3MX6 structures with high ionic conductivity were exhibited only by Li-deficient composition, which results are different from other types of SSEs having high ionic conductivity in both high and low Li concentrations.
In this study, Li-ion conduction mechanisms are studied with first-principles calculations for cost-effective Mg, and Zr-based halide solid electrolytes containing various Li concentrations. Through computational simulations, the ionic conductivities are affected by both Li channel size and bonding characteristics. Furthermore, a new halide solid electrolyte with a high calculated ionic conductivity, 25.3mS/cm, is reported. These findings suggest that the ionic conductivity of Li3MX6 with CCP can be improved by reducing Li-concentration enabling enough Li channel size.
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