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

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. (C) 2022 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

Automated summary

A rapid synthesis method using mechanical alloying and rapid thermal processing is employed to produce a crystalline Argyrodite-type conductor Li5.3PS4.3ClBr0.7 (LPSClBr) with superior ionic conductivity for all-solid-state lithium batteries (ASSLBs). An ultrathin LPSClBr sulfide electrolyte membrane with high ionic conductivity is fabricated using a polytetrafluoroethylene (PTFE) binder and reinforced cellulose mesh. The modified ASSLBs show high cell-level energy density and excellent cyclic stability, demonstrating the potential of the sulfide electrolyte membrane for ASSLBs application.