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Development of all-solid-state thin-film secondary batteries and high energy density cathode materials for all-solid-state lithium secondary batteries

Research Project

Project/Area Number 21K05226
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 36010:Inorganic compounds and inorganic materials chemistry-related
Research InstitutionMie University

Principal Investigator

Taminato Sou  三重大学, 工学研究科, 助教 (60771201)

Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2023: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000)
Fiscal Year 2022: ¥650,000 (Direct Cost: ¥500,000、Indirect Cost: ¥150,000)
Fiscal Year 2021: ¥2,600,000 (Direct Cost: ¥2,000,000、Indirect Cost: ¥600,000)
Keywords全固体リチウム二次電池 / 正極材料 / 薄膜電池 / LiCoO2 / 高電圧動作 / リチウム脱挿入反応 / パルスレーザー堆積法 / RFマグネトロンスパッタ法 / 固体界面
Outline of Research at the Start

これまでに見出した「蓄電池の全固体化による正極反応の可逆性とサイクル安定性向上」に基づき,反応性の高い有機電解液との副反応で分解するため使用が見送られてきた材料(反応)に着目して,可逆的かつ安定な高エネルギー密度正極反応を示す材料を開拓する.本研究では,高電位側に電位窓が広く化学的に安定なリン酸塩電解質と全固体モデル薄膜電池を構築して,正極反応と構造を評価し,固体電解質と組み合わせることで可逆的な高エネルギー密度反応を示す全固体Li二次電池用の正極材料を見出す.

Outline of Final Research Achievements

Thin-film all-solid-state batteries were prepared using a ca. 30 nm thick LiCoO2 thin-film electrode with a layered rock salt structure and an amorphous Li3PO4 solid electrolyte. The LiCoO2 thin-film electrode was tested for high-voltage operation in the all-solid-state battery configuration. The same electrode was also tested in a liquid electrolyte system. In the all-solid- state configuration operating in the range of 3-4.6 V, no significant change in discharge capacity even after 50 cycles of charge-discharge measurements. Furthermore, Li/Li3PO4/LiCoO2/SrRuO3/SrTiO3(100) cell provide high-energy reaction with small degradation in the range of 3-4.8 V by introduction of the solid electrolyte layer between LiCoO2/Li3PO4 interface. Our experimental study suggests the potential of a stable high energy density battery reaction in the all-solid-state battery configuration.

Academic Significance and Societal Importance of the Research Achievements

LiCoO2およびLi5FeO4は高電圧,高容量電極反応過程において,いずれも充電時のLi+脱離以外に反応性の高い有機電解液との副反応で不可逆な酸素脱離が進行して正極自身が分解する.その結果,放電時に容量が取り出せずサイクル安定性も低く,液系電池では材料(反応)の使用が見送られてきた.本検討では,特にLiCoO2について,電位窓の広いリン酸塩固体電解質と組み合わせて固体電池として動作させることで高電圧動作条件においても,高容量反応の可逆特性が向上することを見出した.得られた知見は正極材料の高エネルギー密度化に向けた材料探索や反応制御に貢献すると考えられる.

Report

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

    (11 results)

All 2024 2023 2022 2021 Other

All Journal Article (1 results) (of which Peer Reviewed: 1 results,  Open Access: 1 results) Presentation (8 results) (of which Int'l Joint Research: 1 results,  Invited: 2 results) Remarks (2 results)

  • [Journal Article] Synthesis and electrochemical properties of Li5+xFe1-xMnxO4 with an antifluorite-type structure as a lithium battery cathode2024

    • Author(s)
      Goto Ryosuke、Taminato Sou、Mori Daisuke、Imanishi Nobuyuki
    • Journal Title

      Chemistry Letters

      Volume: 53 Issue: 4

    • DOI

      10.1093/chemle/upae046

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] 逆蛍石型構造を有する Li5+xFe1-xMnxO4 正極活物質の合成と電気化学特性2023

    • Author(s)
      田港聡・後藤綾介・森大輔・今西誠之
    • Organizer
      日本セラミックス協会第36回秋季シンポジウム
    • Related Report
      2023 Annual Research Report
  • [Presentation] Synthesis and electrochemical properties of Li5+xFe1-xMnxO4 with anti-fluorite type structure for lithium battery cathode2023

    • Author(s)
      Sou Taminato,Ryosuke Goto,Daisuke Mori,Nobuyuki Imanishi
    • Organizer
      15th Pacific Rim Conference of Ceramic Societies (PACRIM15)
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 逆蛍石型構造を有する Li5+xFe1-xMnxO4 正極材料の充放電特性2023

    • Author(s)
      後藤綾介,田港聡,森大輔,今西誠之
    • Organizer
      2023電気化学秋季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] LiCoO2薄膜を用いた全固体薄膜電池の高電圧動作下における充放電特性2023

    • Author(s)
      西村優輝,田港聡,森大輔,今西誠之
    • Organizer
      日本セラミックス協会2022年年会
    • Related Report
      2022 Research-status Report
  • [Presentation] 固体電解質を用いた高エネルギー密度蓄電池の構築2022

    • Author(s)
      田港聡
    • Organizer
      低温排熱エネルギー有効活用システム研究会
    • Related Report
      2022 Research-status Report
    • Invited
  • [Presentation] LiCoO2薄膜を用いた全固体薄膜二次電池の作製と高電位動作下におけるリチウム脱挿入特性2021

    • Author(s)
      田港聡、林優仁、森大輔、今西誠之
    • Organizer
      日本セラミックス協会2022年年会
    • Related Report
      2021 Research-status Report
  • [Presentation] 固体電解質を用いた高エネルギー密度蓄電池の構築2021

    • Author(s)
      田港聡
    • Organizer
      「全固体電池実用化に向けた固体電解質の開発」研究会
    • Related Report
      2021 Research-status Report
    • Invited
  • [Presentation] 固体電解質を用いた高エネルギー密度蓄電池の構築2021

    • Author(s)
      田港聡
    • Organizer
      「あいち産業科学技術総合センター」技術指導
    • Related Report
      2021 Research-status Report
  • [Remarks] Researchmap田港聡

    • URL

      https://researchmap.jp/60771201

    • Related Report
      2023 Annual Research Report
  • [Remarks] 三重大学エネルギー変換化学研究室

    • URL

      https://www.energy.chem.mie-u.ac.jp/

    • Related Report
      2022 Research-status Report 2021 Research-status Report

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

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