Controlling Electrostatics To Enhance Conductivity in Structured Electrolytes

Abstract

Solid-state electrolytes are currently being explored as a safe material capable of addressing consumer energy-storage demands. Solid polymer electrolytes, in particular, offer a high energy density and improved safety when compared to liquid-based electrolytes, but tend to have a significantly lower ionic conductivity. We hypothesize structured ionic liquids can enhance conductivity compared to polymer electrolytes. Here, we explore the performance of these materials through coarse-grained molecular dynamics simulation. While we observe similar phase behavior (incorporating solid, smectic, and liquid phases) to that seen in experiments, we also observe significantly more mobility in the cationic species compared to the anionic species before the system reaches an arrest transition. We further discuss how the general results within this paper can guide further studies and target the design of new highly conductive solid electrolytes with the potential to enable the use of multivalent ionic species as ion conductors.