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.

Highlights

  • With the rapid increase in the energy requirements for energy storage devices, it has been difficult to meet these needs using traditional lithium-ion batteries (LIBs) due to low energy density, poor cycle stability, and high cost

  • Many cathode active materials such as LiCoO2, LiNi0.8Co0.1Mn0.1O2, S, and Li2S have been used in all-solidstate lithium batteries (ASSLBs) with Li6PS5Cl (Boulineau et al, 2012; Boulineau et al, 2013; Huang et al, 2015; Yubuchi et al, 2015; Han et al, 2016a; Yu et al, 2016; Zhang et al, 2018a; Zhao et al, 2019; Zhang et al, 2020)

  • Argyrodite Li6PS5Cl is an ionic conductor with high ionic conductivity and a wide electrochemical window

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Summary

INTRODUCTION

With the rapid increase in the energy requirements for energy storage devices, it has been difficult to meet these needs using traditional lithium-ion batteries (LIBs) due to low energy density, poor cycle stability, and high cost. The low electronic conductivity of metal oxides and the high cost of conductive polymers are still not optimal solutions to the serious capacity decay during cycling for a lithium-sulfur battery. Many cathode active materials such as LiCoO2, LiNi0.8Co0.1Mn0.1O2, S, and Li2S have been used in all-solidstate lithium batteries (ASSLBs) with Li6PS5Cl (Boulineau et al, 2012; Boulineau et al, 2013; Huang et al, 2015; Yubuchi et al, 2015; Han et al, 2016a; Yu et al, 2016; Zhang et al, 2018a; Zhao et al, 2019; Zhang et al, 2020). The stability of lithium against Li6PS5Cl was tested by the Neware using symmetric Li/Li6PS5Cl/Li cell at a current density of 0.1 mA cm−2

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DATA AVAILABILITY STATEMENT
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