Journal
ADVANCED MATERIALS
Volume 34, Issue 16, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202200083
Keywords
all-solid-state batteries; inorganic solid electrolytes; solution syntheses; sulfides; wet-chemical methods
Categories
Funding
- Technology Development Program to Solve Climate Changes
- Basic Science Research Program of the National Research Foundation (NRF) - Ministry of Science ICT [NRF-2017M1A2A2044501]
- Materials and Components Technology Development Program of MOTIE/KEIT [10076731, 20007045]
- Yonsei University [2021-22-0326]
- UNIST [1.220022.01]
- Individual Basic Science and Engineering Research Program [NRF-2019R1C1C1009324]
- KISTI [KSC-2021-CRE-0184]
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The wet-chemical processability of sulfide solid electrolytes (SEs) presents a promising opportunity for all-solid-state batteries. This study introduces a universal solution synthesis method for preparing sulfide SEs from various precursors, including Li2S, P2S5, LiCl, Na2S, as well as metal sulfides such as GeS2 and SnS2. The solution-synthesized sulfide SEs exhibit high ionic conductivities and show potential for application in all-solid-state batteries.
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 degrees C, respectively), and their application for all-solid-state batteries is successfully demonstrated.
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