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Formation Mechanism of Thiophosphate Anions in the Liquid-Phase Synthesis of Sulfide Solid Electrolytes Using Polar Aprotic Solvents

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Title: Formation Mechanism of Thiophosphate Anions in the Liquid-Phase Synthesis of Sulfide Solid Electrolytes Using Polar Aprotic Solvents
Authors: Calpa, Marcela Browse this author
Rosero-Navarro, Nataly Carolina Browse this author
Miura, Akira Browse this author →KAKEN DB
Terai, Kota Browse this author
Utsuno, Futoshi Browse this author
Tadanaga, Kiyoharu Browse this author →KAKEN DB
Issue Date: 24-Nov-2020
Publisher: American Chemical Society
Journal Title: Chemistry of materials
Volume: 32
Issue: 22
Start Page: 9627
End Page: 9632
Publisher DOI: 10.1021/acs.chemmater.0c03198
Abstract: Preparation of sulfide-based Li-ion conductive solid electrolytes by a liquid-phase process has been proposed as an effective route for industrial scaling-up. However, reaction mechanisms in the liquid-phase synthesis or the role of solvents in the reactions is not yet well understood. Here, the reaction between Li2S and P2S5 in the composition of 50:50 mol % mediated by a polar aprotic solvent (acetonitrile) was investigated. The study of the crystal and local structure of the 50Li(2)S.50P(2)S(5) sample revealed large chemical changes upon crystallization, highlighting the initial formation of a polymer-like (PS3-) n intermediate. On the basis of the (PS3-) n intermediate, the reaction pathways for the formation of P2S62-, PS43-, and P2S74- anions are elucidated. These findings give a deeper insight into the reaction mechanisms governing the liquid-phase synthesis of sulfide solid electrolytes and provide more specific criteria for designing novel materials with superior characteristics through this liquid-phase approach.
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright c American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see, see
Type: article (author version)
Appears in Collections:工学院・工学研究院 (Graduate School of Engineering / Faculty of Engineering) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: Nataly Carolina Rosero Navarro

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