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Chemistry of Lithium-ion conducting sulfide-based solid electrolyte by solution process

Research Project

Project/Area Number 21H01610
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 26020:Inorganic materials and properties-related
Research InstitutionHokkaido University

Principal Investigator

Tadanaga Kiyoharu  北海道大学, 工学研究院, 教授 (90244657)

Co-Investigator(Kenkyū-buntansha) 藤井 雄太  北海道大学, 工学研究院, 助教 (90982653)
ROSERO CAROLINA  北海道大学, 工学研究院, 助教 (50791381)
Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥17,420,000 (Direct Cost: ¥13,400,000、Indirect Cost: ¥4,020,000)
Fiscal Year 2023: ¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2022: ¥4,290,000 (Direct Cost: ¥3,300,000、Indirect Cost: ¥990,000)
Fiscal Year 2021: ¥8,840,000 (Direct Cost: ¥6,800,000、Indirect Cost: ¥2,040,000)
Keywords硫化物固体電解質 / 全固体電池 / 液相法 / 液相合成
Outline of Research at the Start

全固体電池用固体電解質として期待されているリチウムイオン伝導性硫化物固体電解質の液相法での合成における「化学」を、結晶構造・熱力学・速度論・結晶成長・界面形成といった観点から総合的に明らかにする。これによって、液相による様々な硫化物固体電解質の反応経路を設計する指針を得る。低温合成に速度論的な制御によって準安定相の合成が可能といった液相法の特徴を生かして、高イオン伝導性を示す新奇結晶相の探索を行う。

Outline of Final Research Achievements

The main objectives of the present study are to elucidate the reactions of precursors and solvents in solution during the liquid-phase synthesis of sulfide-based solid electrolytes, to design reaction pathways for various sulfide solid electrolytes, and to explore novel solid electrolytes.

The structure of the precursor complexes formed during the liquid-phase synthesis was analyzed, and the relationship between their thermal decomposition behavior and the resulting phase was clarified. By using both a suspension process and a dissolution-reprecipitation process, we demonstrated that the particle size of the resulting sulfide solid electrolytes can be controlled. We also showed that by using alcohol as a reaction solvent, oxythiophosphate-based solid electrolytes with oxygen incorporated into their structure were obtained.

Academic Significance and Societal Importance of the Research Achievements

液相法を用いて硫化物系固体電解質を合成する場合に、その前駆体の構造や前駆体の溶解挙動を理解することにより、固相法で合成が困難な結晶祖を合成できること、あるいは、得られた固体電解質の粒径を制御できることを示し、液相法の特徴を活かした硫化物系固体電解質を合成できることを明らかにした。

Report

(4 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Annual Research Report
  • 2021 Annual Research Report
  • Research Products

    (24 results)

All 2023 2022 2021

All Journal Article (5 results) (of which Peer Reviewed: 4 results,  Open Access: 2 results) Presentation (17 results) (of which Int'l Joint Research: 5 results,  Invited: 7 results) Book (2 results)

  • [Journal Article] Synthesis of lithium oxy-thiophosphate solid electrolytes with Li10GeP2S12 structure by a liquid phase process using 2-propanol2023

    • Author(s)
      Shiba Shunichiro、Miura Akira、Fujii Yuta、Tadanaga Kiyoharu、Terai Kota、Utsuno Futoshi、Higuchi Hiroyuki
    • Journal Title

      RSC Advances

      Volume: 13 Issue: 33 Pages: 22895-22900

    • DOI

      10.1039/d3ra03929c

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Inorganic-organic hybrid solid electrolytes in the tetramethylammonium iodide-LiI-Li2S-P2S5 system for all-solid-state lithium batteries2023

    • Author(s)
      Fang Tong、Tokiwa Hikaru、Miura Akira、Tadanaga Kiyoharu
    • Journal Title

      Sustainable Energy & Fuels

      Volume: 7 Issue: 17 Pages: 4297-4302

    • DOI

      10.1039/d3se00453h

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Liquid-phase Synthesis of Sulfide Electrolytes and Synthesis Mechanism2022

    • Author(s)
      MIURA Akira、CALPA Marcela、ROSERO-NAVARRO Nataly Carolina、TADANAGA Kiyoharu
    • Journal Title

      Journal of the Japan Society of Powder and Powder Metallurgy

      Volume: 69 Issue: 3 Pages: 95-98

    • DOI

      10.2497/jjspm.69.95

    • ISSN
      0532-8799, 1880-9014
    • Year and Date
      2022-03-15
    • Related Report
      2022 Annual Research Report
    • Open Access
  • [Journal Article] Formation Mechanism of β-Li3PS4 through Decomposition of Complexes2021

    • Author(s)
      Calpa Marcela、Nakajima Hiroshi、Mori Shigeo、Goto Yosuke、Mizuguchi Yoshikazu、Moriyoshi Chikako、Kuroiwa Yoshihiro、Rosero-Navarro Nataly Carolina、Miura Akira、Tadanaga Kiyoharu
    • Journal Title

      Inorganic Chemistry

      Volume: 60 Issue: 10 Pages: 6964-6970

    • DOI

      10.1021/acs.inorgchem.1c00294

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Two-step liquid-phase synthesis of argyrodite Li6PS5Cl solid electrolyte using nonionic surfactant2021

    • Author(s)
      Rosero-Navarro Nataly Carolina、Niwa Hazuki、Miura Akira、Tadanaga Kiyoharu
    • Journal Title

      Boletin de la Sociedad Espanola de Cerrmica y Vidrio

      Volume: - Issue: 2 Pages: 187-193

    • DOI

      10.1016/j.bsecv.2021.12.001

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed
  • [Presentation] Preparation of sulfide-based solid electrolytes for all solid-state lithium batteries using solution processes(2023

    • Author(s)
      Kiyoharu TADANAGA
    • Organizer
      International Conference on Sustainable Energy Materials,2023 Sapporo
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Tetramethylammonium Iodide Doped Li7P2S8I Hybrid Electrolytes for All-solid-state Lithium Batteries2023

    • Author(s)
      Tong FANG, Hikaru TOKIWA, Akira MIURA, Kiyoharu TADANAGA
    • Organizer
      11th International Conference on Materials for Advanced Technologies (ICMAT2023), Singapore
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Preparation of Sulfide-Based Li-ion Conductive Solid Electrolytes Using Solution Processes2023

    • Author(s)
      Kiyoharu TADANAGA
    • Organizer
      International Commission on Glass Annual Meeting, Hangzhou, China
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Inorganic-Organic Hybrid Sulfide Electrolytes Based on the Tetraalkylammonium Iodide-LiI-Li2S-P2S5 System2023

    • Author(s)
      TONG FANG,Kiyoharu TADANAGA,Yuta FUJII,AKIRA MIURA
    • Organizer
      第64回電池討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] 液相法による硫化物固体電解質-Si 負極複合体の合成と全固体電池への応用2023

    • Author(s)
      常盤 輝、カルパ マルセラ、藤井 雄太、三浦 章、忠永 清治
    • Organizer
      第64回電池討論会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Preparation of organic cation-doped LiI-Li2S-P2S5-based hybrid solid electrolytes2023

    • Author(s)
      ファン トン、常盤 輝、掛須 雅子、三浦 章、忠永 清治
    • Organizer
      電気化学会第90回大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Preparation of sulfide-based solid electrolytes using solution process for all solid state battery2022

    • Author(s)
      Kiyoharu Tadanaga
    • Organizer
      26th International Congress on Glass (ICG2022)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 液相プロセスを用いた全固体電池用硫化物固体電解質-Si負極複合体の作製2022

    • Author(s)
      常盤輝・マルセラカルパ・三浦章・ナタリーカロリーナロゼロナバロ・忠永清治
    • Organizer
      日本化学会北海道支部2022年夏季研究発表会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 液相法による硫化物系固体電解質の合成と全固体リチウム電池への応用2022

    • Author(s)
      忠永清治
    • Organizer
      第83回応用物理学会秋季学術講演会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] 液相プロセスによる硫化物固体電解質-Si負極複合体の作製と全固体電池への応用2022

    • Author(s)
      常盤 輝、カルパ マルセラ、ロゼロナバロ ナタリーカロリーナ、三浦 章、忠永 清治
    • Organizer
      第63回電池討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Inorganic Material Synthesis for Electrochemical Devices using solution processes or low temperature processes2022

    • Author(s)
      Kiyoharu TADANAGA
    • Organizer
      MIRAI2.0 Research & Innovation Week
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] 液相法によるLi-P-S-O系固体電解質の合成2022

    • Author(s)
      柴 駿一郎・ 三浦 章・忠永 清治・寺井 恒太・ 宇都野 太・ 樋口 弘幸
    • Organizer
      第48回 固体イオニクス討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 液相法によるLi3PS4-LiCl系固体電解質の合成2021

    • Author(s)
      柴 駿一郎・大嶋 智・マルセラ カルパ・ロゼロ ナバロ ナタリー カロリーナ・三浦 章・忠永清治・寺井恒太・宇都野 太・樋口弘幸
    • Organizer
      日本化学会北海道支部2021年夏季研究発表会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 液相法によるLi3PS4-LiCl系固体電解質の合成と評価2021

    • Author(s)
      柴 駿一郎、大嶋 智、カルパ マルセラ、ロゼロナバロ ナタリーカロリーナ、三浦 章、忠永 清治、寺井 恒太、宇都野 太、樋口 弘幸
    • Organizer
      電気化学会2021年秋季大会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Li2S-P2S5 Solutions for Forming Solid Electrolyte Coating Layers on Electrode Materials for All-Solid-State Batteries2021

    • Author(s)
      Marcela Calpa, Nataly Rosero-Navarro, Akira Miura, Kiyoharu Tadanaga
    • Organizer
      240th ECS Meeting
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 硫化物系固体電解質の液相合成と全固体リチウム電池への応用2021

    • Author(s)
      忠永清治
    • Organizer
      2021年度電気化学会九州支部シンポジウム
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Preparation of sulfide-based lithium ion conductive solid electrolyte by solution process2021

    • Author(s)
      Kiyoharu Tadanaga
    • Organizer
      International Conference on Materials and Systems for Sustainability 2021
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Book] 第13章 電池材料(分担執筆)、ゾル-ゲル法の最新動向2023

    • Author(s)
      忠永清治(監修 中西和樹)
    • Total Pages
      436
    • Publisher
      シーエムシー出版
    • ISBN
      9784781317434
    • Related Report
      2023 Annual Research Report
  • [Book] Solid State Batteries Volume 1: Emerging Materials and Applications Chapter 13 "Sulfide-Based Solid-State Electrolytes", pp 319-3512022

    • Author(s)
      Rosero-Navarro N. C.、Calpa M.、Miura A.、Tadanaga K.
    • Total Pages
      440
    • Publisher
      American Chemical Society
    • Related Report
      2022 Annual Research Report

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Published: 2021-04-28   Modified: 2025-01-30  

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