High-Performance All-Solid-State Lithium–Sulfur Batteries Enabled by Slurry-Coated Li6PS5Cl/S/C Composite Electrodes

Abstract

Among many lithium secondary batteries, lithium–sulfur batteries stand out because of their high theoretical specific energy, low cost, non-toxicity and the fact that they cause no environmental pollution. However, due to poor electronic and ionic conductivity, shuttle effect, lithium dendrites and other defects, it remains a big challenge to achieve large-scale application of lithium-sulfur batteries. Here we report an all-solid-state lithium–sulfur battery based on Li-argyrodite Li6PS5Cl solid-state electrolytes through a slurry-coating method. Li6PS5Cl with a high ionic conductivity of 1.3 × 10–3 S cm−1 at room temperature is used as the solid electrolyte and the ion conductive additive in the electrode. The sulfur-based composite cathode is fabricated through a slurry-coating process by dispersing sulfur, Li6PS5Cl, ethyl cellulose, and carbon black in 1,3-dioxolane (DOL). This method can disperse the Li6PS5Cl around sulfur particles well, and the solvent does not react with any component of composite cathodes during preparation. The battery delivers a high discharge capacity of 962 mA h g−1 at room temperature for the first cycle at 80 mA g−1. While the Coulombic efficiency is approximately 99.5% during 100 cycles. This work provides a new insight into the combination method between the sulfide-type SSEs and sulfur cathodes, which is critical to the electrochemical performance of all-solid-state lithium-sulfur batteries.

Argyrodite Solid Electrolyte-Integrated Ni-Rich Oxide Cathode with Enhanced Interfacial Compatibility for All-Solid-State Lithium Batteries

“…In addition, to determine the porosity of the LPSCl 1.5 – x NBR electrolyte films, the Archimedes drainage method was adopted . First, the obtained electrolyte films were soaked into a 1,3-dioxolane (DOL) solvent for 12 h since LPSCl 1.5 cannot dissolve in the DOL solution, as well as it does not react with the DOL solution . After that, the LPSCl 1.5 – x NBR electrolyte films were taken out from the DOL solvent and dried using a filter paper until no solvent dropped.…”

“…31 First, the obtained electrolyte films were soaked into a 1,3-dioxolane (DOL) solvent for 12 h since LPSCl 1.5 cannot dissolve in the DOL solution, as well as it does not react with the DOL solution. 32 After that, the LPSCl 1.5 −xNBR electrolyte films were taken out from the DOL solvent and dried using a filter paper until no solvent dropped. The solvent uptake could be calculated by the mass difference of the electrolyte films before/after soaking in the DOL solvent.…”

Thermodynamics and Kinetics of the Cathode–Electrolyte Interface in All-Solid-State Li–S Batteries

“…28−30 be stable. Zheng et al 31 found that the Li 6 PS 5 Cl/S interface undergoes reductive degradation to form Li 3 P, LiP, Li 3 P 7 , or LiP 7 along with Li 2 S and LiCl. It also undergoes oxidative degradation, resulting in thiosulfate oligomerization, which releases polysulfides that lead to sluggish Li-ion transport and cathode overpotential.…”

“…The volatility of sulfur makes experimental characterization of these interfaces using traditional tools such as scanning electron microscopy and transmission electron microscopy challenging. − Nevertheless, existing studies suggest that these interfaces might not be stable. Zheng et al . found that the Li 6 PS 5 Cl/S interface undergoes reductive degradation to form Li 3 P, LiP, Li 3 P 7 , or LiP 7 along with Li 2 S and LiCl.…”

Recent Progress in Quasi/All-Solid-State Electrolytes for Lithium–Sulfur Batteries

“…et al, 2021;Pang et al, 2021). Therefore, significant research effort into LSB has potential advantages for future energy storage (Wang H. et al, 2017;Fan et al, 2021;Zheng et al, 2021;Phuc et al, 2022).…”