Tailoring the Interface between Sulfur and Sulfide Solid Electrolyte for High-Areal-Capacity All-Solid-State Lithium–Sulfur Batteries

Abstract

Fabricating high-capacity all-solid-state lithium-sulfur batteries (ASSLSBs) with long lifetimes is realistically challenging because of the poor ionic contact between the insulating element sulfur (S8) and the solid electrolyte at the solid–solid interface. Herein, an inorganic Li-ion-conducting species composed of polysulfido-intermediate compounds (3Li+-PS4+n 3– (n ≥ 0)) is incorporated between S8 and the sulfide solid electrolyte (SSE) of Li6PS5Cl (LPSCl) to enhance the ionic contact of S8. A weakly polar solvent which is included in the mixing process but eventually removed promotes interfacial chemical reactions between S8 and LPSCl, significantly enhancing the wettability of LPSCl toward the active material (S8). This maximizes the utilization of S8, facilitates interfacial Li-ion transport, and enhances the mechanical properties of the solid-state S cathode. As a result, a high-performance ASSLSB with a high areal capacity (5.1 mAh cm–2) and promising lifetime (250 cycles) at room temperature, operating at a current density of 1 mA cm–2, is successfully developed.

Advances in All-Solid-State Lithium–Sulfur Batteries for Commercialization

“…Additionally, the chemical compatibility between S and sulfide SSEs at the interface is advantageous for ASSLSBs (Fig. 4 a) [ 151 ]. It is noteworthy that S materials were not exclusively used as the cathode active material in the earliest phases of ASSLSB development.…”

“…4 a A scheme of inorganic Li-ion-conducting species (3Li + -PS 4+ n 3– ( n ≥ 0)) incorporated between S 8 and the SSE of Li 6 PS 5 Cl (LPSCl) to enhance the ionic contact of S 8 . Copyright 2023, American Chemical Society [ 151 ]. b Atomic force microscopy (AFM) image of an amorphous rGO@S-40 composite on a Si substrate.…”

Bridging the gap between academic research and industrial development in advanced all-solid-state lithium–sulfur batteries

“…202 Meanwhile, Kim et al pointed out the importance of solvent selection in the solution processing of sulfur cathode. 160 Wet milling of cathode composites with a weakly polar solvent induced a chemical reaction between elemental sulfur and sulfide solid electrolytes. As a result, a polysulfido-intermediate phase formed at the interfaces, establishing excellent solid–solid contacts (Fig.…”

Constructing the Interconnected Charge Transfer Pathways in Sulfur Composite Cathode for All-Solid-State Lithium–Sulfur Batteries

“…However, realization of the anticipated performance of ASSLSBs is challenging owing to the electrical and ionic insulating nature of sulfur. − The effective electrochemical utilization of sulfur requires simultaneous contact between the sulfur, solid electrolyte, and conductive materials. Unfortunately, the difficulty of forming such triple-phase interfaces poses a significant obstacle to the efficient utilization of sulfur.…”