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Lee, Ji Eun; Park, Kern‐Ho; Kim, Jin Chul; Wi, Tae‐Ung; Ha, A. Reum; Song, Yong Bae; Oh, Dae Yang; Woo, Jehoon; Kweon, Seong Hyeon; Yeom, Su Jeong; Cho, Woosuk; Kim, KyungSu; Lee, Hyun‐Wook; Kwak, Sang Kyu; Jung, Yoon Seok
Advanced materials (Weinheim), 04/2022, Letnik: 34, Številka: 16Journal Article
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 GeS 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. The universal solution synthesis of sulfide solid electrolytes is first demonstrated. The alkahest solvent, 1,2‐ethylenediamine–1,2‐ethanedithiol, fully dissolves not only Li2S (or Na2S), P2S5, and LiCl, but also metal sulfides (e.g., GeS2 and SnS2), forming homogeneous solid electrolyte solutions. Solution‐synthesized Li10GeP2S12, Li6PS5Cl, and Na11Sn2PS12 exhibit high ionic conductivities, and their applicability to all‐solid‐state batteries is successfully demonstrated.
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in: SICRIS
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