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Computational discovery of stable Na-ion sulfide solid electrolytes with high conductivity at room temperature
The search for inorganic solid electrolytes suitable for the realization of solid-state batteries with structural stability and high ion conductivity at room temperature remains a significant challenge. In this study, we employed a multi-stage density functional theory molecular dynamics (DFT-MD) sampling workflow, focusing on Na-ion sulfides NanMmM0m0S4 with trivalent (M) and pentavalent (M0) metal ions and an expanded selection of parent structures (U). This led to the identification of two promising sampling spaces (M,M0,U) = (Ga,P,Na4SiS4)
and (Si,Ta,Na4SiS4). The predictions were validated through multitemperature DFT-MD calculations, wherein sNa,300K T 10−3 S cm−1 are attained within a thermodynamic phase stability range of 9 < Ehull < 25 meV per atom (Ehull is convex hull decomposition energy): Na4-Ga0.5P0.5S4, Na3.75Ga0.375P0.625S4, Na4.25Ga0.625P0.375S4, Na3.75Si0.75-Ta0.25S4, Na3.625Si0.625Ta0.375S4, and Na3.5Si0.5Ta0.5S4. These compounds are highly suggested for experimental synthesis and investigation. Moreover, our brute-force and highly generalized sampling technique is expected to be applicable in uncovering other solid electrolyte classes, thus potentially contributing to the advancement of solid-state battery technology.
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- 05/08/2024
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jmca2024_NaSulfideConductor_rj.pdf | 2.97 MB | MDR Open |
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