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

13 Citations (Scopus)


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
Issue number16
Publication statusPublished - 2022 Apr 21

Bibliographical note

Funding Information:
J.E.L., K.‐H.P., and J.C.K. contributed equally to this work. This work was supported by the Technology Development Program to Solve Climate Changes and by the Basic Science Research Program of the National Research Foundation (NRF) funded by the Ministry of Science & ICT (Grant No. NRF‐2017M1A2A2044501), the Materials and Components Technology Development Program of MOTIE/KEIT (Grant Nos. 10076731 and 20007045), and by the Yonsei University Research Fund of 2021 (2021‐22‐0326). H.‐W.L. acknowledges support from the 2022 Research Fund (1.220022.01) of UNIST and the Individual Basic Science and Engineering Research Program (NRF‐2019R1C1C1009324). The computational resources were provided by UNIST‐HPC and KISTI (KSC‐2021‐CRE‐0184).

Publisher Copyright:
© 2022 Wiley-VCH GmbH.

All Science Journal Classification (ASJC) codes

  • Materials Science(all)
  • Mechanics of Materials
  • Mechanical Engineering


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