In Situ Welding Ionic Conductive Breakpoints for Highly Reversible All-Solid-State Lithium-Sulfur Batteries.

Abstract

Poly(ethylene oxide) (PEO)-based solid-state lithium-sulfur batteries (SSLSBs) have garnered considerable interest owing to their impressive energy density and high safety. However, the dissolved lithium polysulfide (LiPS) together with sluggish reaction kinetics disrupts the electrolyte network, bringing about ionic conductive breakpoints and severely limiting battery performance. To cure this, we propose an in situ welding strategy by introducing phosphorus pentasulfide (P₂S₅) as the welding filler into PEO-based solid cathodes. P₂S₅ can react with LiPS to form ion-conducting lithium polysulfidophosphate (LSPS), which suppresses the interaction with PEO and in situ weld breakpoints within the ionic conductive network. Of interest, LSPS also shows another function, that is, to catalyze sulfur redox reactions by decreasing the activation energy of sulfur reduction reaction from 0.87 to 0.75 eV, mitigating the shuttle effect. The in situ welding strategy helps the assembled SSLSB to feature exceptional cycling stability and a high energy density of up to 358 Wh·kg^-1 due to the high sulfur utilization. Our findings pave an avenue for practical high-performance SSLSBs with a novel welding filler for in situ welding of ionic conductive network.