Transport Properties of Polysulfide Species in Lithium-Sulfur Battery Electrolytes: Coupling of Experiment and Theory

Abstract

A comprehensive experimental and theoretical analysis of the isothermal transport of species for the two model ternary-electrolytes with LiTFSILi2S4/dioxolane (DOL)-dimethoxyethane (DME) and LiTFSI-Li2S6/DOL-DME formulations is presented. An unambiguous picture of the polysulfide’s mobility is set forth after a detailed investigation of the macroscopic transference number and diffusion coefficients. The new findings of incongruent diffusion for Li2S4 species and high significance of cross-term diffusion coefficients reformulate a fledgling view of the prevalent redox-shuttle phenomena. The practical implications of this complex mechanism are discussed in detail.