Universal Solution Synthesis of Sulfide Solid Electrolytes Using Alkahest for All-Solid-State Batteries

Ji Eun Lee, Kern Ho Park, Jin Chul Kim, Tae Ung Wi, A. Reum Ha, Yong Bae Song, Dae Yang Oh, Jehoon Woo, Seong Hyeon Kweon, Su Jeong Yeom, Woosuk Cho, Kyung Su Kim, Hyun Wook Lee, Sang Kyu Kwak, Yoon Seok Jung

Research output: Contribution to journalArticlepeer-review

46 Citations (Scopus)

Abstract

The wet-chemical processability of sulfide solid electrolytes (SEs) provides intriguing opportunities for all-solid-state batteries. Thus far, sulfide SEs are wet-prepared either from solid precursors suspended in solvents (suspension synthesis) or from homogeneous solutions using SEs (solution process) with restricted composition spaces. Here, a universal solution synthesis method for preparing sulfide SEs from precursors, not only Li2S, P2S5, LiCl, and Na2S, but also metal sulfides (e.g., GeS2 and SnS2), fully dissolved in an alkahest: a mixture solvent of 1,2-ethylenediamine (EDA) and 1,2-ethanedithiol (EDT) (or ethanethiol). Raman spectroscopy and theoretical calculations reveal that the exceptional dissolving power of EDA–EDT toward GeS2 is due to the nucleophilicity of the thiolate anions that is strong enough to dissociate the Ge-S bonds. Solution-synthesized Li10GeP2S12, Li6PS5Cl, and Na11Sn2PS12 exhibit high ionic conductivities (0.74, 1.3, and 0.10 mS cm−1 at 30 °C, respectively), and their application for all-solid-state batteries is successfully demonstrated.

Original languageEnglish
Article number2200083
JournalAdvanced Materials
Volume34
Issue number16
DOIs
Publication statusPublished - 2022 Apr 21

Bibliographical note

Publisher Copyright:
© 2022 Wiley-VCH GmbH.

All Science Journal Classification (ASJC) codes

  • General Materials Science
  • Mechanics of Materials
  • Mechanical Engineering

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