Lithium-Ion Transport and Exchange between Phases in a Concentrated Liquid Electrolyte Containing Lithium-Ion-Conducting Inorganic Particles.

Abstract

Understanding Li+ transport in organic-inorganic hybrid electrolytes, where Li+ has to lose its organic solvation shell to enter and transport through the inorganic phase, is crucial to the design of high-performance batteries. As a model system, we investigate a range of Li+-conducting particles suspended in a concentrated electrolyte. We show that large Li1.3Al0.3Ti1.7P3O12 and Li6PS5Cl particles can enhance the overall conductivity of the electrolyte. When studying impedance using a cell with a large cell constant, the Nyquist plot shows two semicircles: a high-frequency semicircle related to ion transport in the bulk of both phases and a medium-frequency semicircle attributed to Li+ transporting through the particle/liquid interfaces. Contrary to the high-frequency resistance, the medium-frequency resistance increases with particle content and shows a higher activation energy. Furthermore, we show that small particles, requiring Li+ to overcome particle/liquid interfaces more frequently, are less effective in facilitating Li+ transport. Overall, this study provides a straightforward approach to study the Li+ transport behavior in hybrid electrolytes.