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Clarification of migration process of lithium ions in all-solid-state lithium ion secondary batteries during charging and discharging

Research Project

Project/Area Number 17K06846
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Research Field Structural/Functional materials
Research InstitutionMeijo University

Principal Investigator

TSUCHIYA Bun  名城大学, 理工学部, 教授 (90302215)

Project Period (FY) 2017-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥3,770,000 (Direct Cost: ¥2,900,000、Indirect Cost: ¥870,000)
Fiscal Year 2019: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2018: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000)
Fiscal Year 2017: ¥1,170,000 (Direct Cost: ¥900,000、Indirect Cost: ¥270,000)
Keywordsリチウム酸化物 / リチウムイオン二次電池 / リチウムイオン移動機構 / 飛行時間型反跳粒子検出法 / リチウム蓄積量その場測定 / 飛行時間型反跳粒子法 / その場測定 / リチウム蓄積量
Outline of Final Research Achievements

The lithium (Li) concentrations for both of Au/LiCoO2/Li1.4Al0.4Ge0.7Ti0.9P3O12(LATP) positive electrode side and Pt/LATP negative one in Au/LiCoO2/LATP/Pt all-solid-state Li+ ion secondary batteries were in situ measured under charging various voltages from 1.65 to 2.04 V in a vacuum using the high-energy time-of-flight elastic recoil detection (ToF-ERD) technique with 9.0-MeV Cu10+ ion-probe beams. The ToF-ERD spectra significantly revealed that the Li concentration in the LiCoO2 positive electrode decreased with an increase in the charged voltages and the Li concentration in the LATP negative one increased. Therefore, it could be concluded that the Li migration from the LiCoO2 positive electrode to the LATP negative one in the battery was dynamically observed under the various charges using the ToF-ERD technique with the reliable depth resolution in approximately a tens of nanometer scale.

Academic Significance and Societal Importance of the Research Achievements

マグネトロンスパッタリング装置を用いて、厚さ約150 μmの全固体リチウムイオン二次電池を作製し、イオンビーム分析手法を利用して正・負極/固体電解質間のリチウムイオンの移動をその場で観測するという明確な目標があり、新たな発想で従来にはない取り組みを行った。
また、この提案した手法を用いることで、充放電時における正極、負極および固体電解質中の過渡的なリチウム濃度を評価することが可能となるため、より優れたリチウムイオン導電性能を有するリチウム電池の開発へとつながることが期待される。従って、本研究は、今後の活気ある持続可能な社会の構築を実現するための極めて重要かつ不可欠な研究であった。

Report

(7 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Research-status Report
  • 2020 Research-status Report
  • 2019 Research-status Report
  • 2018 Research-status Report
  • 2017 Research-status Report
  • Research Products

    (46 results)

All 2023 2022 2021 2020 2019 2018 2017

All Journal Article (13 results) (of which Int'l Joint Research: 3 results,  Peer Reviewed: 13 results,  Open Access: 2 results) Presentation (31 results) (of which Int'l Joint Research: 16 results,  Invited: 10 results) Book (2 results)

  • [Journal Article] Behaviors of H, D, and Li in water-soaked LATP solid electrolytes at room temperature2023

    • Author(s)
      Kodera Taku、Tsuchiya Bun、Takahiro Katsumi、Hosoda Akifumi
    • Journal Title

      Journal of Alloys and Compounds

      Volume: 949 Pages: 169774-169774

    • DOI

      10.1016/j.jallcom.2023.169774

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Thermal desorption processes of H2 and CH4 from Li2ZrO3 and Li4SiO4 materials absorbed H2O and CO2 in air at room temperature2023

    • Author(s)
      Tsuchiya B.、Kodera T.、Miyaoka H.、Ichikawa T.、Kojima Y.
    • Journal Title

      International Journal of Hydrogen Energy

      Volume: 48 Issue: 24 Pages: 8830-8836

    • DOI

      10.1016/j.ijhydene.2022.11.217

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Hydrogen Absorption in Near Surface of Lithium-ion Conductive Glass Ceramics by Water Uptake at Room Temperature2022

    • Author(s)
      Kodera Taku、Tsuchiya Bun、Kato Ryo、Usami Taiki、Takahiro Katsumi
    • Journal Title

      e-Journal of Surface Science and Nanotechnology

      Volume: 20 Issue: 4 Pages: 237-242

    • DOI

      10.1380/ejssnt.2022-045

    • ISSN
      1348-0391
    • Year and Date
      2022-10-08
    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Sensitive In-operando Observation of Li and O Transport in Thin-film Li-ion Batteries2021

    • Author(s)
      V. Mathayan, K. Morita, B. Tsuchiya, R. Ye, M. Baba and D. Primetzhofer
    • Journal Title

      Materials Today Energy

      Volume: 21 Pages: 1-9

    • DOI

      10.1016/j.mtener.2021.100844

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Dynamic Behavior of Li Depth Profiles in Solid State Li Ion Battery Under Charging and Discharging by Means of ERD and RBS Techniques2021

    • Author(s)
      K. Morita, B. Tsuchiya, R. Ye, H. Tsuchida and T. Majima
    • Journal Title

      Solid State Ionics

      Volume: 370 Pages: 1-7

    • DOI

      10.1016/j.ssi.2021.115730

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] In-operando Observation of Li Depth Distribution and Li Transport in Thin Film Li Ion Batteries2020

    • Author(s)
      V. Mathayan, M. V. Moro, K. Morita, B. Tsuchiya, R. Ye, M. Baba and D. Primetzhofer
    • Journal Title

      Appl. Phys. Lett.

      Volume: 117 Pages: 1-5

    • Related Report
      2020 Research-status Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Light Element Analysis of Ceramics Using in-air ERDA and TOF-ERDA2020

    • Author(s)
      K. Suzuki, B. Tsuchiya, K. Yasuda and Y. Nakata
    • Journal Title

      Nucl. Instr. and Meth. in Phys. Res., B

      Volume: 478 Pages: 169-173

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Li Depth Profiles of Metal/Li-electrolyte/Metal Capacitors Under Biasing Studied by Means of MeV Ion Beam Analysis Techniques2020

    • Author(s)
      K. Morita, B. Tsuchiya, H. Tsuchida and T. Majima
    • Journal Title

      Solid State Ionics

      Volume: 344

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] Change in Li Depth Profiles of Au/LCO/mixed LATP-LAGP/Pt Battery Under Discharging Studied by Ion Beam Analysis Techniques with 9 MeV O4+ Ions2020

    • Author(s)
      K. Morita, B. Tsuchiya, H. Tsuchida and T. Majima
    • Journal Title

      Solid State Ionics

      Volume: 344

    • Related Report
      2020 Research-status Report
    • Peer Reviewed
  • [Journal Article] In-situ Direct Lithium Distribution Analysis Around Interfaces in an All-Solid-State Rechargeable Lithium Battery by Combined Ion-Beam Method2019

    • Author(s)
      B. Tsuchiya, J. Ohnishi, Y. Sasaki, T. Yamamoto, Y. Yamamoto, M. Motoyama, Y. Iriyama and K. Morita
    • Journal Title

      Adv. Mater. Interfaces

      Volume: 6 Pages: 1-7

    • Related Report
      2019 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Dependence of Hydrogen-absorption and -desorption Characteristics on Density of Lithium-zirconium Oxides Exposed in Air at Room Temperature2018

    • Author(s)
      B. Tsuchiya, S. Nagata, Y. Mizoguchi, Y. Takagi, M. Ito, Y. Oya, K. Okuno and K. Morita
    • Journal Title

      Acta Mater.

      Volume: 148 Pages: 185-192

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] High Resolution Li Depth Profiling of Solid State Li Ion Battery by TERD Technique with High Energy Light Ions2018

    • Author(s)
      K. Morita, B. Tsuchiya, J. Ohnishi, T. Yamamoto, Y. Iriyama, H. Tsuchida, T. Majima and K. Suzuki
    • Journal Title

      Nucl. Instr. and Meth. in Phys. Res.

      Volume: B426 Pages: 30-32

    • Related Report
      2018 Research-status Report
    • Peer Reviewed
  • [Journal Article] 反跳粒子検出法による全固体リチウムイオン二次電池内の軽元素の動的解析2017

    • Author(s)
      土屋文
    • Journal Title

      J. The Surface Science Society of Japan

      Volume: 38 Pages: 182-187

    • NAID

      130005606244

    • Related Report
      2017 Research-status Report
    • Peer Reviewed
  • [Presentation] イオンビーム分析法を用いた電極/固体電解質界面のリチウム濃度分布その場測定2023

    • Author(s)
      土屋文、小寺拓、鈴木耕拓、佐々木知子
    • Organizer
      応用物理学会 春の大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] In-situ Measurement of Lithium Transfer at Electrode/Solid Electrolyte Interfaces in All-solid-state Batteries Under Charging and Discharging by ToF-ERD Technique2022

    • Author(s)
      B. Tsuchiya, T. Kodera, K. Suzuki and T. Sasaki
    • Organizer
      IC on Materials Science, Engineering & Technology '22 (ICMSET’22)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Absorption Process of Hydrogen Isotopes in Solid Electrolyte Materials by Water Splitting2022

    • Author(s)
      T. Kodera, B. Tsuchiya, K. Suzuki and T. Sasaki
    • Organizer
      IC on Materials Science, Engineering & Technology '22 (ICMSET’22)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] In-situ Hydrogen Distribution Analysis in LiCoO2 by Water Uptake at Room Temperature Using Elastic Recoil Detection in Air Atmosphere2022

    • Author(s)
      B. Tsuchiya, T. Kodera, T. Sasaki, and K. Suzuki
    • Organizer
      応用物理学会 薄膜・表面物理分科会 イオンビームによる表面・界面の解析と改質 特別研究会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Hydrogen and Lithium Measurements in Near Surface of Water-soaked LATP Solid Electrolytes Using Elastic Recoil Detection Techniques2022

    • Author(s)
      T. Kodera, B. Tsuchiya, T. Sasaki, and K. Suzuki
    • Organizer
      応用物理学会 薄膜・表面物理分科会 イオンビームによる表面・界面の解析と改質 特別研究会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Dynamic Behaviors of Lithium and Hydrogen at Electrode/Solid Electrolyte Interfaces Using Elastic Recoil Detection Techniques2022

    • Author(s)
      B. Tsuchiya, T. Kodera, T. Sasaki, S. Yamamoto, and K. Takahiro
    • Organizer
      14th International Symposium on Atomic Level Characterizations for New Materials and Devices '22 (ALC’22)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Absorption and Desorption Processes of H in LiCoO2 by H2O Splitting at Room Temperature2022

    • Author(s)
      B. Tsuchiya, T. Kodera, and K. Suzuki
    • Organizer
      14th International Symposium on Atomic Level Characterizations for New Materials and Devices '22 (ALC’22)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Behaviors of Hydrogen and Lithium in Near Surface of Lithium-ion Conductive Glass-ceramics by Water Uptake at Room Temperature2022

    • Author(s)
      T. Kodera, R. Kato, T. Usami and B. Tsuchiya
    • Organizer
      14th International Symposium on Atomic Level Characterizations for New Materials and Devices '22(ALC’22)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 常温水分解によるコバルト酸リチウムの水素吸収特性2022

    • Author(s)
      土屋文、小寺拓、鈴木耕拓、佐々木知子
    • Organizer
      日本金属学会 秋の大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 室温において水浸漬されたリチウムイオン伝導性ガラスセラミックスの水素およびリチウム挙動2022

    • Author(s)
      小寺拓、加藤僚、宇佐見太毅、土屋文、鈴木耕拓、佐々木知子
    • Organizer
      日本金属学会 秋の大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 電圧印加されたリチウムイオン伝導性ガラスセラミックス中のリチウムイオン移動機構2022

    • Author(s)
      小寺拓、加藤僚、宇佐見太毅、土屋文、鈴木耕拓、佐々木知子
    • Organizer
      日本金属学会 春の大会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 充電時における正負極/固体電解質界面のリチウムイオン移動機構2021

    • Author(s)
      土屋文、宇佐見太毅、加藤僚、鈴木耕拓、佐々木知子
    • Organizer
      第47回固体イオニクス討論会 講演番号 1A-09 (口頭講演)
    • Related Report
      2021 Research-status Report
  • [Presentation] Dynamics of Lithium Around Electrode/Solid Electrolyte Interface in All-solid-state Batteries Under Charging and Discharging by Ion Beam Analysis2021

    • Author(s)
      B. Tsuchiya, T. Usami, R. Kato, T. Kodera, T. Sasaki and K. Morita
    • Organizer
      2nd Advanced Materials Science World Congress 2021
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Dynamics of Lithium Around Electrode/Solid Electrolyte Interface in All-solid-state Batteries Under Charging and Discharging by Ion Beam Analysis2021

    • Author(s)
      T. Usami, R. Kato, T. Kodera, T. Sasaki and B. Tsuchiya
    • Organizer
      Symposium on Atomic Level Characterizations for New Materials and Devices'21 (ALC’21)
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] Hydrogen Storage in LiCoO2 by H2O Splitting at Room Temperature2021

    • Author(s)
      R. Kato, T. Usami, T. Kodera, K. Suzuki and B. Tsuchiya
    • Organizer
      Symposium on Atomic Level Characterizations for New Materials and Devices'21 (ALC’21)
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] Hydrogen Absorption Process in Near Surface of Lithium-ion Conductive Glass-ceramics by Water Uptake at Room Temperature2021

    • Author(s)
      T. Kodera, R. Kato, T. Usami and B. Tsuchiya
    • Organizer
      Symposium on Atomic Level Characterizations for New Materials and Devices'21 (ALC’21)
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] 飛行時間型反跳粒子検出法を用いたリチウム電池内のリチウムイオン移動その場観察2021

    • Author(s)
      土屋文
    • Organizer
      応用物理学会 春季大会 シンポジウム(口頭講演)
    • Related Report
      2020 Research-status Report
    • Invited
  • [Presentation] In-situ Direct Measurement of Lithium Transfer at Interface between LiCoO2 Positive Electrode and LATP Solid Electrolyte by Ion Beam Analysis2020

    • Author(s)
      T. Usami, R. Kato, B. Tsuchiya, T. Sasaki
    • Organizer
      イオンビームによる表面・界面の解析と改質 特別研究会
    • Related Report
      2020 Research-status Report
  • [Presentation] 反跳粒子検出法を用いたLiCoO2正極/LATP固体電解質界面におけるLi+イオン移動量その場測定2020

    • Author(s)
      宇佐見太毅、加藤僚、土屋文、佐々木知子
    • Organizer
      日本金属学会 秋期大会
    • Related Report
      2020 Research-status Report
  • [Presentation] Dynamic Behavior of Lithium Ions in All-solid-state Batteries with Charging and Discharging Using Ion Beam Analysis2019

    • Author(s)
      B. Tsuchiya, T. Usami, R. Kato, S. Iwane, S. Yamamoto, K. Takahiro, Y. Sasaki, T. Majima, H. Tsuchida and K. Morita
    • Organizer
      23rd International Workshop on Inelastic Ion-Surface Collisions (IISC)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] イオンビーム分析手法を用いた全固体リチウムイオン二次電池内の正極/固体電解質界面近傍におけるリチウムイオン移動その場解析2019

    • Author(s)
      土屋文
    • Organizer
      京都アカデミアフォーラム
    • Related Report
      2019 Research-status Report
    • Invited
  • [Presentation] Dynamic Analysis of Lithium and Hydrogen Migrations at Au/LiCoO2, LiCoO2/LATP, LATP/Pt Interfaces in All-solid-state Batteries with Charging by Elastic Recoil Detection Technique2019

    • Author(s)
      B. Tsuchiya, T. Usami, S. Yamamoto and K. Takahiro
    • Organizer
      4th International Symposium on Materials for Energy Storage and Conversion (mESC-IS 2019)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Density Dependence in Hydrogen-storage Characteristic of Lithium-rich Zirconium Oxides2019

    • Author(s)
      B. Tsuchiya, S. Iwane, T. Sugiyam, H. Miyaoka, T. Ichikawa and Y. Kojima
    • Organizer
      4th International Symposium on Materials for Energy Storage and Conversion (mESC-IS 2019)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] Thermal Behavior of Lithium and Hydrogen in LiCoO2 Positive Electrode and LATP Electrolyte at Charging Process2019

    • Author(s)
      B. Tsuchiya, R. Kato, S. Yamamoto and K. Takahiro
    • Organizer
      4th International Symposium on Materials for Energy Storage and Conversion (mESC-IS 2019)
    • Related Report
      2019 Research-status Report
    • Int'l Joint Research
  • [Presentation] リチウム-ジルコニウム酸化物セラミックスの常温水分解・水素吸蔵特性2019

    • Author(s)
      土屋文、杉山知子、大矢恭久、奥野健二、宮岡裕樹、小島由継、市川貴之、徳永和俊
    • Organizer
      日本金属学会
    • Related Report
      2018 Research-status Report
  • [Presentation] 反跳粒子検出法を用いた全固体リチウムイオン二次電池内のリチウム移動その場測定2018

    • Author(s)
      土屋文、山本春也、高廣克己
    • Organizer
      日本金属学会
    • Related Report
      2018 Research-status Report
  • [Presentation] Defect Formation Energies Due to Hydrogen-dopants on Interstitial Sites in Uranium Intermetallic Compounds2018

    • Author(s)
      B. Tsuchiya, T. Yamamoto, K. Ohsawa and M. Yamawaki
    • Organizer
      The 2018 Energy Material Nanotechnology (EMN) Meeting on Computation and Theory
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Dependence of Hydrogen-storage and -release on Density of Oxide Ceramics Exposed in Air at Room Temperature2018

    • Author(s)
      B. Tsuchiya, S. Yamaguchi, H. Miyaoka, T. Ichikawa and Y. Kojima
    • Organizer
      The International Conference on Processing and Manufacturing of Advanced Materials (THERMEC-2018)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] ERDAによるリチウムの動的挙動の研究2017

    • Author(s)
      土屋文
    • Organizer
      日本物理学会
    • Related Report
      2017 Research-status Report
    • Invited
  • [Presentation] Dynamic Behavior Analysis of Hydrogen and Lithium in All-solid- state Li+ Ion Secondary Batteries under Charging Using Elastic Recoil Detection2017

    • Author(s)
      B. Tsuchiya, S. Yamamoto, K. Takahiro and S. Nagata
    • Organizer
      21th Int. Conf. on Secondary Ion Mass Spectrometry (ICSIMS 2017)
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] 加熱された全固体リチウムイオン二次電池中のリチウムイオン伝導挙動2017

    • Author(s)
      土屋文、高廣克己、山本春也
    • Organizer
      日本金属学会
    • Related Report
      2017 Research-status Report
  • [Book] 「リチウム分析」、第8章 リチウムイオン電池の分析、解析と評価技術、第2節 全固体リチウムイオン電池の充電時におけるリチウムイオン移動機構2019

    • Author(s)
      土屋文
    • Total Pages
      7
    • Publisher
      技術情報協会
    • Related Report
      2019 Research-status Report
  • [Book] 「全固体電池のイオン伝導性向上技術と材料、製造プロセスの開発」、第11章 全固体電池、材料の分析・解析技術、4節 金属/Li電解質/金属キャパシタの電圧印加によるLi濃度分布変化のMeV重イオンビームその場・解析2017

    • Author(s)
      森田健治、土屋文
    • Publisher
      技術情報協会
    • Related Report
      2017 Research-status Report

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Published: 2017-04-28   Modified: 2024-01-30  

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