A facile path from fast synthesis of Li-argyrodite conductor to dry forming ultrathin electrolyte membrane for high-energy-density all-solid-state lithium batteries

Abstract

All-solid-state lithium batteries (ASSLBs), utilizing sulfide solid electrolyte, are considered as the promising design on account of their superior safety and high energy density, whereas the time-consuming preparation process of sulfide electrolyte powders and the thickness of electrolyte layer hinder their practical application. Herein, an innovative ultimate-energy mechanical alloying plus rapid thermal processing approach is employed to rapidly synthesize the crystalline Argyrodite-type conductor Li5.3PS4.3ClBr0.7 (LPSClBr) with superior ionic conductivity (11.7 mS cm−1). Furthermore, to realize the higher energy density of the battery, an ultrathin LPSClBr sulfide electrolyte membrane with superior ionic conductivity of 6.5 mS cm−1 is fabricated with the aid of polytetrafluoroethylene (PTFE) binder and the reinforced cellulose mesh. Moreover, a simple solid electrolyte interphase (SEI) is constructed on the surface of lithium metal to enhance anodic stability. Benefiting from the joint efforts of these merits, the modified ASSLBs with a high cell-level energy density of 311 Wh kg−1 show an excellent cyclic stability. The assembled all-solid-state Li2S/Li pouch cell can operate even under the severe conditions of bending and cutting, demonstrating the enormous potential of the sulfide electrolyte membrane for ASSLBs application.