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Development of high-capacity cathodes for rechargeable batteries by controlling microstructure of oxides

Research Project

Project/Area Number 21H01646
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Review Section Basic Section 26040:Structural materials and functional materials-related
Research InstitutionTohoku University

Principal Investigator

Kawaguchi Tomoya  東北大学, 金属材料研究所, 助教 (00768103)

Co-Investigator(Kenkyū-buntansha) 市坪 哲  東北大学, 金属材料研究所, 教授 (40324826)
Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥17,680,000 (Direct Cost: ¥13,600,000、Indirect Cost: ¥4,080,000)
Fiscal Year 2023: ¥1,690,000 (Direct Cost: ¥1,300,000、Indirect Cost: ¥390,000)
Fiscal Year 2022: ¥4,940,000 (Direct Cost: ¥3,800,000、Indirect Cost: ¥1,140,000)
Fiscal Year 2021: ¥11,050,000 (Direct Cost: ¥8,500,000、Indirect Cost: ¥2,550,000)
Keywordsマグネシウム蓄電池 / ハイエントロピー酸化物 / 岩塩型構造 / 蓄電池 / 拡散 / パーコレーション / 酸化物電極材料 / 二次電池 / 酸化物正極材料 / 微細組織構造 / ハイエントロピー / 酸化物正極 / 微細組織
Outline of Research at the Start

リチウムイオン電池などで用いられる遷移金属酸化物正極材料では,整合界面を有する微細な複相から構成されるナノドメイン微細組織をもつ材料が優れた比容量を示す.ナノドメイン微細構造は,多数の元素を固溶した結果得られるハイエントロピー効果により,柔軟に制御できる可能性がある.そこで本研究では,ナノドメイン微細構造を用いた高容量化機構をより広範な材料群において利用するために,酸化物正極材料におけるハイエントロピー効果が,相分離・固溶挙動,微細組織形成機構,そして電極性能に与える影響を,実験と理論計算の両面から明らかにする.

Outline of Final Research Achievements

In this study, we investigated the high-entropy effects on capabilities in oxide electrode materials used for rechargeable batteries. Mixing many elements in a single phase leads to a high configurational entropy state in the materials. In the present study, we focused on oxide cathode materials for rechargeable magnesium batteries, which utilize abundant magnesium instead of lithium used for current lithium-ion batteries. The high-entropy effects enable the synthesis of a material with a targeted structure and a composition, in which insertion and extraction of magnesium were demonstrated. The activation mechanism also revealed in the present study paves the path to developing more promising materials for practical rechargeable magnesium batteries.

Academic Significance and Societal Importance of the Research Achievements

これまでの研究より,マグネシウム蓄電池の酸化物正極材料はマグネシウムを挿入できるものの,初期の構造から岩塩型構造に相転移することが知られていた.岩塩型構造は陽イオンが密に詰まった構造であるため,もともと酸素副格子との相互作用の強い二価のマグネシウムの脱離は非常に困難であり,繰り返し充放電特性の悪化の原因となっていた.本研究ではそのような岩塩型構造を有する正極材料をあえて合成し,その活性化機構を明らかにした.この活性化機構は材料科学的に有意義であるだけでなく,ポストリチウムイオン電池として期待されるマグネシウム蓄電池の実現に貢献し,ひいては持続可能社会実現に資する結果であると考えられる.

Report

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

    (20 results)

All 2024 2023 2022 2021

All Journal Article (8 results) (of which Int'l Joint Research: 2 results,  Peer Reviewed: 6 results,  Open Access: 4 results) Presentation (10 results) (of which Int'l Joint Research: 3 results,  Invited: 4 results) Patent(Industrial Property Rights) (2 results) (of which Overseas: 1 results)

  • [Journal Article] Securing cation vacancies to enable reversible Mg insertion/extraction in rocksalt oxides2024

    • Author(s)
      Kawaguchi Tomoya、Yasuda Masaya、Nemoto Natsumi、Shimokawa Kohei、Li Hongyi、Okamoto Norihiko L.、Ichitsubo Tetsu
    • Journal Title

      Journal of Materials Chemistry A

      Volume: - Issue: 15 Pages: 9088-9101

    • DOI

      10.1039/d3ta07942b

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Alkali Cation Additives Assisting Magnesium Cation Intercalation in Hollandite-Type Manganese Dioxide Cathodes2023

    • Author(s)
      Qi Yue、Li Hongyi、Shimokawa Kohei、Ye Xiatong、Kawaguchi Tomoya、Ichitsubo Tetsu
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: 127 Issue: 43 Pages: 21271-21278

    • DOI

      10.1021/acs.jpcc.3c03803

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Optimizing LiMn1.5M0.5O4 cathode materials for aqueous photo-rechargeable batteries2023

    • Author(s)
      Shimokawa Kohei、Matsubara Shogo、Kawaguchi Tomoya、Okamoto Akihiro、Ichitsubo Tetsu
    • Journal Title

      Chemical Communications

      Volume: 59 Issue: 51 Pages: 7947-7950

    • DOI

      10.1039/d3cc01902k

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Evaluating the Validity of a Hydrogen Mapping Method Based on Laser-induced Breakdown Spectroscopy2022

    • Author(s)
      Imashuku Susumu、Kamimura Takumi、Kawaguchi Tomoya、Ichitsubo Tetsu
    • Journal Title

      e-Journal of Surface Science and Nanotechnology

      Volume: 20 Issue: 1 Pages: 7-12

    • DOI

      10.1380/ejssnt.2022-007

    • NAID

      130008161061

    • ISSN
      1348-0391
    • Year and Date
      2022-02-17
    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Influences of enhanced entropy in layered rocksalt oxide cathodes for lithium-ion batteries2022

    • Author(s)
      Tomoya Kawaguchi, Xiao Bian, Takuya Hatakeyama, Hongyi Li, Tetsu Ichitsubo
    • Journal Title

      ACS Applied Energy Materials

      Volume: TBD Issue: 4 Pages: 4369-4381

    • DOI

      10.1021/acsaem.1c03968

    • Related Report
      2022 Annual Research Report 2021 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Operando Nanoscale Imaging of Electrochemically Induced Strain in a Locally Polarized Pt Grain2022

    • Author(s)
      Sheyfer Dina、Mariano Ruperto G.、Kawaguchi Tomoya、Cha Wonsuk、Harder Ross J.、Kanan Matthew W.、Hruszkewycz Stephan O.、You Hoydoo、Highland Matthew J.
    • Journal Title

      Nano Letters

      Volume: 23 Issue: 1 Pages: 1-7

    • DOI

      10.1021/acs.nanolett.2c01015

    • Related Report
      2022 Annual Research Report
  • [Journal Article] Electrochemically Induced Strain Evolution in Pt-Ni Alloy Nanoparticles Observed by Bragg Coherent Diffraction Imaging2021

    • Author(s)
      Kawaguchi Tomoya、Komanicky Vladimir、Latyshev Vitalii、Cha Wonsuk、Maxey Evan R.、Harder Ross、Ichitsubo Tetsu、You Hoydoo
    • Journal Title

      Nano Letters

      Volume: 21 Issue: 14 Pages: 5945-5951

    • DOI

      10.1021/acs.nanolett.1c00778

    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research
  • [Journal Article] pH- and Cation-Dependent Water Oxidation on Rutile RuO2(110)2021

    • Author(s)
      Rao Reshma R.、Huang Botao、Katayama Yu、Hwang Jonathan、Kawaguchi Tomoya、Lunger Jaclyn R.、Peng Jiayu、Zhang Yirui、Morinaga Asuka、Zhou Hua、You Hoydoo、Shao-Horn Yang
    • Journal Title

      The Journal of Physical Chemistry C

      Volume: - Issue: 15 Pages: 8195-8207

    • DOI

      10.1021/acs.jpcc.1c00413

    • Related Report
      2021 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] ブラッグコヒーレント回折イメージングを用いた触媒合金ナノ粒子の組成分布とひずみの可視化2024

    • Author(s)
      河口 智也
    • Organizer
      第37回日本放射光学会年会放射光科学合同シンポジウム
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] ハイエントロピー酸化物を用いた蓄電池電極材料2023

    • Author(s)
      河口智也, 市坪哲
    • Organizer
      日本金属学会2023年秋期(第173回)講演大会
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] 放射光 X 線散乱・分光手法を用いた電気化学系の解析2023

    • Author(s)
      河口智也
    • Organizer
      第6回MIRCフォーラム ナノマテリアルの計測技術
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] Reaction-driven restructuring of Pt-Rh nanoparticles: Bragg coherent diffraction imaging (BCDI) during gas-surface reactions2023

    • Author(s)
      Tomoya Kawaguchi, Thomas F. Keller, Henning Runge, Luca Gelisio, Christoph Seitz, Young Y. Kim, Wonsuk Cha, Stephan O. Hruszkewycz, Ross Harder, Ivan A. Vartanyants, Andreas Stierle and Hoydoo You
    • Organizer
      APS March Meeting 2023
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ハイエントロピー酸化物を用いた蓄電池正極材料2023

    • Author(s)
      河口智也,安田優哉,根本菜摘,下川航平,李弘毅,岡本範彦,市坪哲
    • Organizer
      電気化学会第90回大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Strain Evolution in Pt-Ni Alloy Nanoparticles During Electrochemical Ni Leaching Revealed by Bragg Coherent Diffraction Imaging2022

    • Author(s)
      Tomoya Kawaguchi, Vladimir Komanicky, Vitalii Latyshev, Wonsuk Cha, Evan R. Maxey, Ross Harder, Tetsu Ichitsubo, and Hoydoo You
    • Organizer
      241st ECS meeting
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Bragg Coherent Diffraction Imaging Studies of Catalytic Alloy Nanoparticles2022

    • Author(s)
      Tomoya Kawaguchi
    • Organizer
      MIRAI2.0 Research & Innovation Week 2022
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] リチウムイオン電池用酸化物正極材料におけるハイエントロピー化効果2022

    • Author(s)
      河口智也, 卞篠, 安田優哉, 畠山拓也, 李弘毅, 市坪哲
    • Organizer
      第48回 固体イオニクス討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 混合エントロピー効果を利用した多元素酸化物正極材料2021

    • Author(s)
      卞篠,河口智也,李弘毅,市坪哲
    • Organizer
      金研講演会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Effects of Enhanced-Entropy in Cathode Materials for Lithium-Ion Batteries2021

    • Author(s)
      X. Bian, T. Kawaguchi, T. Hatakeyama, H. Li , T. Ichitsubo
    • Organizer
      材料科学拠点シンポジウム
    • Related Report
      2021 Annual Research Report
  • [Patent(Industrial Property Rights)] 正極活物質、マグネシウム蓄電池の製造方法2024

    • Inventor(s)
      市坪哲,河口智也,安田優哉
    • Industrial Property Rights Holder
      市坪哲,河口智也,安田優哉
    • Industrial Property Rights Type
      特許
    • Filing Date
      2024
    • Related Report
      2023 Annual Research Report
    • Overseas
  • [Patent(Industrial Property Rights)] 正極活物質、マグネシウム蓄電池の製造方法2023

    • Inventor(s)
      市坪哲,河口智也,安田優哉
    • Industrial Property Rights Holder
      市坪哲,河口智也,安田優哉
    • Industrial Property Rights Type
      特許
    • Filing Date
      2023
    • Related Report
      2022 Annual Research Report

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

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