First Principles Study of Amorphous Al₂O₃ Coating in Li-S Battery Electrode Design

The lithium-sulfur (Li-S) battery is exceptionally appealing as an alternative candidate in beyond lithium-ion (Li-ion) battery technology due to its promising high specific energy capacity. However, several obstacles (e.g. polysulfides dissolution, shuttle effect, high volume expansion of the cathode, etc.) remain and thus hinder the commercialization of Li-S batteries. To overcome these challenges, a fundamental study based on atomistic simulation can be very useful. In this work, a comprehensive investigation of the interaction of electrolyte (solvent and salt) molecules, lithium sulfide, and polysulfide molecules with an amorphous Al₂O₃ surface was performed based on first principles density functional theory (DFT) calculations. The results based on the DFT calculations suggest that the amorphous Al₂O₃ can be used as a likely coating material in Li-S battery electrode design to tackle these problems.