Lithium polysulfide conformer analysis in ether-based solvents for Li?S batteries

JAVIER LUQUE DI SALVO; GUILLERMINA LUQUE; GIORGIO DE LUCA

Molecular Systems Design & Engineering

Royal Society of Chemistry

Año: 2022

2058-9689

fundamental understanding of polysulfide conformers in common (ether-based) solvents used inprototype lithium?sulfur batteries is mandatory to push the technology towards practical applications. Inthis work, molecular dynamics simulations were used to perform a detailed conformational analysis anddynamics ascertainment of lithium hexasulfide Li2S6 as a representative of soluble long-chain lithiumpolysulfides. This novel conformational dynamics study based on 106 structures per studied systemprovides important insights into open questions such as how many Li+ coordinate polysulfides arecorrelated to lithium transport and polysulfide clustering. The simulations predict that monoanionic LiS6− inits closed conformation is the predominant structure in 1,2-dioxolane and dimethoxyethane equimolarmixtures. If a second Li+ approaches, that leads to the opening of the polysulfide chain and the formationof neutral Li2S6 (open conformer). By changing the electrolyte composition, the relati