Novel fast Li-ion conductors for solid-state electrolytes from first-principles

Area of Science:

• Materials Science
• Computational Chemistry
• Solid-State Chemistry

Background:

• All-solid-state electrolytes are crucial for next-generation batteries.
• Identifying fast lithium-ion conductors is key to their practical application.
• High-throughput computational screening offers an efficient approach to discover novel materials.

Purpose of the Study:

• To perform a high-throughput computational screening for fast lithium-ion conductors.
• To identify promising candidate materials for all-solid-state electrolytes.
• To develop and refine a computational protocol for material discovery.

Main Methods:

• Sourced over 30,000 Li-containing experimental structures from multiple databases.
• Employed automated calculations to identify electronic insulators.
• Utilized molecular dynamics simulations with the pinball model for diffusivity estimation.
• Validated promising candidates with first-principles molecular dynamics simulations.

Main Results:

• Identified approximately 1000 electronic insulators from the initial dataset.
• Estimated Li-ion diffusivities for ~1000 structures using the fast pinball model.
• Selected ~60 promising fast conductors for further investigation.
• Detailed analysis of 9 fastest conductors, including Li7NbO6 with ~5 mS cm-1 ionic conductivity at room temperature.

Conclusions:

• The high-throughput screening protocol successfully identified novel fast lithium-ion conductors.
• Li7NbO6 emerges as a highly promising material for solid-state electrolytes.
• The developed computational workflow accelerates the discovery of advanced battery materials.