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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.

Rights:

• https://creativecommons.org/licenses/by-nc/3.0/legalcode
  

Keyword: all solid state batteries, solid electrolytes, high-throughput first-principles calculation, computational materials search, machine learning, sodium ion conductors

Date published: 2024-08-05

Publisher: Royal Society of Chemistry (RSC)

Journal:

• Journal of Materials Chemistry A (ISSN: 20507488) vol. 12 issue. 32 p. 20879-20886

Funding:

• Japan Science and Technology Agency JPMJGX23S4
• Ministry of Education, Culture, Sports, Science and Technology JPMXP0219207397
• Ministry of Education, Culture, Sports, Science and Technology JPMXP1020230325
• Ministry of Education, Culture, Sports, Science and Technology JPMXP1122712807
• Japan Society for the Promotion of Science JP21K14729
• Japan Society for the Promotion of Science JP24H02203
• Co-creation place formation support program JPMJPF2016
• Advanced Low Carbon Technology Research and Development Program JPMJAL1301

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1039/d4ta02522a

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Updated at: 2024-10-10 16:30:52 +0900

Published on MDR: 2024-10-10 16:30:52 +0900