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Performance enhancement of cathodes for all-solid-state sintered lithium-ion secondary batteries using oxide solid electrolytes.

Research Project

Project/Area Number 22K04739
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 26040:Structural materials and functional materials-related
Research InstitutionKyushu University

Principal Investigator

WATANABE KEN  九州大学, 総合理工学研究院, 准教授 (90552480)

Project Period (FY) 2022-04-01 – 2025-03-31
Project Status Completed (Fiscal Year 2024)
Budget Amount *help
¥3,770,000 (Direct Cost: ¥2,900,000、Indirect Cost: ¥870,000)
Fiscal Year 2024: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2023: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2022: ¥1,690,000 (Direct Cost: ¥1,300,000、Indirect Cost: ¥390,000)
Keywords一括焼結型全固体電池 / Liインサーション / 劣化挙動 / ガーネット / 層状岩塩 / 機械劣化 / 全固体電池 / Liイオン伝導体 / 層状岩塩構造 / ガーネット型酸化物 / 一括焼結
Outline of Research at the Start

申請者は、これまでにガーネット型酸化物(Li7La3Zr2O12:LLZ)を固体電解質、Ni系層状岩塩酸化物を正極活物質とした一括焼結型全固体Liイオン二次電池(Co-fired all solid-state Li-ion battery: Cf-AssLiB)の作製プロセスを確立した。本研究では、Cf-AssLiBにしか実現できない活物質緻密正極や活物質緻密層と活物質/固体電解質複合層を積層した二層正極など正極微細構造や活物質組成が電池特性に与える影響を調査し、Cf-AssLiBの高性能化に資する設計指針を得ることを目的とする。

Outline of Final Research Achievements

In all-solid-state sintered batteries, battery characteristics are considered controllable based on the mixing state of cathode active material and LLZ within the composite cathode, microstructure, and mixed conductivity of the cathode active material. In particular, since sintering is used, various electrode structures can be applied, such as dense electrodes formed by densifying only the cathode active material, or layered structures consisting of LLZ/cathode active material mixed electrodes and dense layers.
Therefore, this study focuses on designing electrode structures unique to all-solid-state sintered batteries. It has been observed that using only a dense layer of active material as the electrode leads to cycle degradation. However, it was found that cycle degradation could be suppressed by forming a buffer layer consisting of a mixture of solid electrolyte and active material between the solid electrolyte and the dense layer of active material.

Academic Significance and Societal Importance of the Research Achievements

本研究では、酸化物系固体電解質からなる一括焼結型全固体電池の正極に注目し、その高性能化につながる材料設計指針を、作製条件、正極活物質のLi組成、電極の構造の観点から精査したもので、酸化物系焼結型電池において、活物質の欠陥制御、活物質の体積変化の緩和が電池性能に寄与することを見出したもの、焼結型全固体電池における学術的知見を開拓した。また、得られた成果は、社会実装に向けた課題抽出およびその解決の糸口になり、今後の発展が期待される。

Report

(4 results)
  • 2024 Annual Research Report   Final Research Report ( PDF )
  • 2023 Research-status Report
  • 2022 Research-status Report
  • Research Products

    (16 results)

All 2025 2024 2023 2022 Other

All Journal Article (2 results) (of which Peer Reviewed: 2 results,  Open Access: 2 results) Presentation (12 results) (of which Int'l Joint Research: 6 results,  Invited: 6 results) Remarks (2 results)

  • [Journal Article] Thickly and densely sintered Li<sub>3</sub><i><sub>x</sub></i>La<sub>2/3−</sub><i><sub>x</sub></i>TiO<sub>3</sub> electrodes for the anode of Li-ion batteries2025

    • Author(s)
      Takeno Shinichi、Watanabe Ken、Suematsu Koichi、Shimanoe Kengo
    • Journal Title

      Journal of the Ceramic Society of Japan

      Volume: 133 Issue: 3 Pages: 80-85

    • DOI

      10.2109/jcersj2.24116

    • ISSN
      1348-6535, 1882-0743
    • Year and Date
      2025-03-01
    • Related Report
      2024 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] New insight into designing a thick-sintered cathode for Li-ion batteries: the impact of excess lithium in LiCoO<sub>2</sub> on its electrode performance2025

    • Author(s)
      Takeno Shinichi、Suematsu Taiki、Kunisaki Ryusei、Hasegawa Gen、Watanabe Ken、Kuwata Naoaki、Mitsuishi Kazutaka、Ohnishi Tsuyoshi、Takada Kazunori、Suematsu Kohichi、Shimanoe Kengo
    • Journal Title

      Journal of Materials Chemistry A

      Volume: 13 Issue: 4 Pages: 2943-2949

    • DOI

      10.1039/d4ta07377k

    • Related Report
      2024 Annual Research Report
    • Peer Reviewed / Open Access
  • [Presentation] ガーネット固体電解質を用いた焼結型全固体電池2024

    • Author(s)
      渡邉賢
    • Organizer
      2024年度日本セラミックス協会春季特別講演
    • Related Report
      2024 Annual Research Report
    • Invited
  • [Presentation] 全固体電池向け易焼結性ガーネット型固体電解質の開発2024

    • Author(s)
      渡邉賢
    • Organizer
      第122回新電池構想部会
    • Related Report
      2024 Annual Research Report
    • Invited
  • [Presentation] Electrochemical property of Li3xLa2/3-xTiO3 sintered anode for all-solid batteries2024

    • Author(s)
      竹野 慎一、渡邉 賢、末松 昂一、島ノ江 憲剛
    • Organizer
      PRIME2024
    • Related Report
      2024 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Co-Sintering Anode Materials with Garnet Electrolytes for Solid-State Batteries2024

    • Author(s)
      何宗琦、渡邉 賢、末松 昂一、島ノ江 憲剛
    • Organizer
      PRiME2024
    • Related Report
      2024 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ガーネット固体電解質を用いた焼結型全固体電池2024

    • Author(s)
      渡邉賢
    • Organizer
      第62回セラミックス基礎科学討論会
    • Related Report
      2023 Research-status Report
    • Invited
  • [Presentation] ガーネット型固体電解質を用いた全固体電池の充放電サイクル特性2023

    • Author(s)
      福野佑斗, 渡邉賢, 末松昴一, 島ノ江憲剛
    • Organizer
      2023電気化学秋季大会
    • Related Report
      2023 Research-status Report
  • [Presentation] 一括焼結型全固体電池の充放電サイクル特性の検討2023

    • Author(s)
      福野佑斗, 渡邉賢, 末松昴一, 島ノ江憲剛
    • Organizer
      第60回化学関連支部合同九州大会
    • Related Report
      2023 Research-status Report
  • [Presentation] True all-solid-state battery based on Li-stuffed garnet electrolytes: What can we do by sintering?2023

    • Author(s)
      Ken Watanabe
    • Organizer
      Energy summit 2023
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Tuning the grain boundary of Li-stuffed garnet typed Li-ion conductors for all-solid-state batteries2023

    • Author(s)
      Ken Watanabe
    • Organizer
      The 37th International Korea-Japan Seminar on Ceramics
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Co-Sintered Solid-State Batteries based on Li-Stuffed Garnet Electrolytes2023

    • Author(s)
      Ken Watanabe, Koichi Suematsu, Kazutaka Mitsuishi, Kengo Shimanoe
    • Organizer
      The 4th World Conference on Solid Electrolytes for Advanced Applications: Garnets and Competitors
    • Related Report
      2023 Research-status Report
    • Int'l Joint Research
  • [Presentation] Co-fired solid-state batteries based on Li-stuffed garnet electrolyte2023

    • Author(s)
      Ken Watanabe
    • Organizer
      International Conference on Energy Conversion and Storage 2023
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Ta-Bi共置換ガーネット型酸化物固体電解質を用いた一括焼結全固体Liイオン電池の作製2022

    • Author(s)
      渡邉賢、田代歩夢、竹野慎一、福野佑斗、末松昂一、島ノ江憲剛
    • Organizer
      日本セラミックス協会第35回秋季シンポジウム
    • Related Report
      2022 Research-status Report
  • [Remarks] 島ノ江・渡邉・末松研究室ホームページ

    • URL

      https://igses.kyushu-u.ac.jp/shimanoe/index.html

    • Related Report
      2024 Annual Research Report
  • [Remarks] 研究室ホームページ

    • URL

      https://www.mm.kyushu-u.ac.jp/lab_03/index.html

    • Related Report
      2023 Research-status Report

URL: 

Published: 2022-04-19   Modified: 2026-01-16  

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