Solution Processing via Dynamic Sulfide Radical Anions for Sulfide Solid Electrolytes

Solution processing technology for the manufacturing of all‐solid‐state batteries (ASSBs) holds great promise of scalability and low cost over ball milling and solid‐state methods. However, conventional liquid‐phase synthesis for solid electrolytes has yet to translate into large‐scale manufacturing...

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Main Authors: Hirotada Gamo, Jin Nishida, Atsushi Nagai, Kazuhiro Hikima, Atsunori Matsuda
Format: Article
Language:English
Published: Wiley-VCH 2022-07-01
Series:Advanced Energy & Sustainability Research
Subjects:
Online Access:https://doi.org/10.1002/aesr.202200019
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author Hirotada Gamo
Jin Nishida
Atsushi Nagai
Kazuhiro Hikima
Atsunori Matsuda
author_facet Hirotada Gamo
Jin Nishida
Atsushi Nagai
Kazuhiro Hikima
Atsunori Matsuda
author_sort Hirotada Gamo
collection DOAJ
description Solution processing technology for the manufacturing of all‐solid‐state batteries (ASSBs) holds great promise of scalability and low cost over ball milling and solid‐state methods. However, conventional liquid‐phase synthesis for solid electrolytes has yet to translate into large‐scale manufacturing to address commercialization challenges. Herein, solution processing via dynamic sulfide radical anions is developed, providing rapid and scalable manufacturing of Li7P3S11 solid electrolytes (SEs). A mixture of Li2S, P2S5, and excess elemental sulfur in a mixed solvent of acetonitrile, tetrahydrofuran, and ethanol forms a homogenous precursor solution containing the S3 ·− radical anion. The presence of ethanol enhances the chemical stability of S3 ·−. The resulting sulfide radical anions serve as a mediator with two strategies: the soluble polysulfide formation and activation of P2S5, and thus allows the generation of the precursor solution in 2 min. The Li7P3S11 is prepared in 2 h without the need for ball milling or high‐energy treatment, which shows higher ionic conductivity (1.2 mS cm−1 at 25 °C) and excellent cell performance of ASSBs cells than Li7P3S11 prepared by ball milling. The solution processing technology reported here paves the way for the accelerated adoption of practical ASSBs manufacturing.
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spelling doaj.art-76fe41c604794bd98ccba674cc0435752022-12-22T02:29:23ZengWiley-VCHAdvanced Energy & Sustainability Research2699-94122022-07-0137n/an/a10.1002/aesr.202200019Solution Processing via Dynamic Sulfide Radical Anions for Sulfide Solid ElectrolytesHirotada Gamo0Jin Nishida1Atsushi Nagai2Kazuhiro Hikima3Atsunori Matsuda4Department of Electrical and Electronic Information Engineering Toyohashi University of Technology 1-1 Hibarigaoka Tempaku-cho Toyohashi Aichi 441-8580 JapanDepartment of Electrical and Electronic Information Engineering Toyohashi University of Technology 1-1 Hibarigaoka Tempaku-cho Toyohashi Aichi 441-8580 JapanDepartment of Electrical and Electronic Information Engineering Toyohashi University of Technology 1-1 Hibarigaoka Tempaku-cho Toyohashi Aichi 441-8580 JapanDepartment of Electrical and Electronic Information Engineering Toyohashi University of Technology 1-1 Hibarigaoka Tempaku-cho Toyohashi Aichi 441-8580 JapanDepartment of Electrical and Electronic Information Engineering Toyohashi University of Technology 1-1 Hibarigaoka Tempaku-cho Toyohashi Aichi 441-8580 JapanSolution processing technology for the manufacturing of all‐solid‐state batteries (ASSBs) holds great promise of scalability and low cost over ball milling and solid‐state methods. However, conventional liquid‐phase synthesis for solid electrolytes has yet to translate into large‐scale manufacturing to address commercialization challenges. Herein, solution processing via dynamic sulfide radical anions is developed, providing rapid and scalable manufacturing of Li7P3S11 solid electrolytes (SEs). A mixture of Li2S, P2S5, and excess elemental sulfur in a mixed solvent of acetonitrile, tetrahydrofuran, and ethanol forms a homogenous precursor solution containing the S3 ·− radical anion. The presence of ethanol enhances the chemical stability of S3 ·−. The resulting sulfide radical anions serve as a mediator with two strategies: the soluble polysulfide formation and activation of P2S5, and thus allows the generation of the precursor solution in 2 min. The Li7P3S11 is prepared in 2 h without the need for ball milling or high‐energy treatment, which shows higher ionic conductivity (1.2 mS cm−1 at 25 °C) and excellent cell performance of ASSBs cells than Li7P3S11 prepared by ball milling. The solution processing technology reported here paves the way for the accelerated adoption of practical ASSBs manufacturing.https://doi.org/10.1002/aesr.202200019all-solid-state batterieslithium polysulfidessolution processingsolution synthesissulfide solid electrolytes
spellingShingle Hirotada Gamo
Jin Nishida
Atsushi Nagai
Kazuhiro Hikima
Atsunori Matsuda
Solution Processing via Dynamic Sulfide Radical Anions for Sulfide Solid Electrolytes
Advanced Energy & Sustainability Research
all-solid-state batteries
lithium polysulfides
solution processing
solution synthesis
sulfide solid electrolytes
title Solution Processing via Dynamic Sulfide Radical Anions for Sulfide Solid Electrolytes
title_full Solution Processing via Dynamic Sulfide Radical Anions for Sulfide Solid Electrolytes
title_fullStr Solution Processing via Dynamic Sulfide Radical Anions for Sulfide Solid Electrolytes
title_full_unstemmed Solution Processing via Dynamic Sulfide Radical Anions for Sulfide Solid Electrolytes
title_short Solution Processing via Dynamic Sulfide Radical Anions for Sulfide Solid Electrolytes
title_sort solution processing via dynamic sulfide radical anions for sulfide solid electrolytes
topic all-solid-state batteries
lithium polysulfides
solution processing
solution synthesis
sulfide solid electrolytes
url https://doi.org/10.1002/aesr.202200019
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AT jinnishida solutionprocessingviadynamicsulfideradicalanionsforsulfidesolidelectrolytes
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AT kazuhirohikima solutionprocessingviadynamicsulfideradicalanionsforsulfidesolidelectrolytes
AT atsunorimatsuda solutionprocessingviadynamicsulfideradicalanionsforsulfidesolidelectrolytes