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Development of methods for lithium self-diffusion coefficient measurements in mixed conductors using isotope exchange

Research Project

Project/Area Number 15H03872
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Inorganic industrial materials
Research InstitutionTohoku University

Principal Investigator

Kuwata Naoaki  東北大学, 多元物質科学研究所, 准教授 (00396459)

Co-Investigator(Renkei-kenkyūsha) KAWAMURA JUNICHI  東北大学, 多元物質科学研究所, 教授 (50142683)
MIYAZAKI TAKAMICHI  東北大学, 工学研究科, 技術職員 (20422090)
Project Period (FY) 2015-04-01 – 2018-03-31
Project Status Completed (Fiscal Year 2017)
Budget Amount *help
¥17,420,000 (Direct Cost: ¥13,400,000、Indirect Cost: ¥4,020,000)
Fiscal Year 2017: ¥2,990,000 (Direct Cost: ¥2,300,000、Indirect Cost: ¥690,000)
Fiscal Year 2016: ¥9,100,000 (Direct Cost: ¥7,000,000、Indirect Cost: ¥2,100,000)
Fiscal Year 2015: ¥5,330,000 (Direct Cost: ¥4,100,000、Indirect Cost: ¥1,230,000)
Keywords混合伝導体 / 拡散係数 / 空孔拡散機構 / LiCoO2 / LiMn2O4 / 二次イオン質量分析 / 全固体電池 / インターカレーション / 同位体交換 / 化学拡散係数 / 化学ポテンシャル / リチウムイオン電池 / 混合導電体 / 固体イオニクス / トレーサー拡散係数 / 薄膜リチウム電池 / 同位体 / 二次電池 / イオニクス / 薄膜電池 / イオン交換 / 固体電解質
Outline of Final Research Achievements

Lithium-ion battery electrode materials are mixed conductors which have significant conduction of both ionic and electronic. It is proved that a measurement of lithium diffusion coefficient in the mixed conductors is difficult, and the method for the diffusion measurement has not been established. The aim of this study is to develop the method to measure the tracer diffusion coefficient of the mixed conductors by using secondary ion mass spectrometry (SIMS), based on the idea that 6Li in the cathode material can be replaced with 7Li by electrochemical charge-discharge. As a result of this study, we succeeded to develop three kinds of ion-exchange methods and to clarify the diffusion coefficient of thin films a-Li3PO4, LiMn2O4 and LiCoO2 by using the developed methods. It has been found that the temperature and composition dependence of the diffusion coefficients in the intercalation electrodes are able to explain by vacancy diffusion mechanism.

Report

(4 results)
  • 2017 Annual Research Report   Final Research Report ( PDF )
  • 2016 Annual Research Report
  • 2015 Annual Research Report
  • Research Products

    (40 results)

All 2018 2017 2016 2015 Other

All Int'l Joint Research (2 results) Journal Article (10 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 10 results,  Open Access: 2 results,  Acknowledgement Compliant: 1 results) Presentation (28 results) (of which Int'l Joint Research: 9 results,  Invited: 2 results)

  • [Int'l Joint Research] Institute for Basic Science (IBS)(韓国)

    • Related Report
      2016 Annual Research Report
  • [Int'l Joint Research] Institute for Basic Science (IBS)(韓国)

    • Related Report
      2015 Annual Research Report
  • [Journal Article] Lithium diffusion coefficient in LiMn 2 O 4 thin films measured by secondary ion mass spectrometry with ion-exchange method2018

    • Author(s)
      Kuwata Naoaki、Nakane Masakatsu、Miyazaki Takamichi、Mitsuishi Kazutaka、Kawamura Junichi
    • Journal Title

      Solid State Ionics

      Volume: 320 Pages: 266-271

    • DOI

      10.1016/j.ssi.2018.03.012

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Thin-film lithium batteries with 0.3-30 μm thick LiCoO2 films fabricated by high-rate pulsed laser deposition2018

    • Author(s)
      Matsuda Yasutaka、Kuwata Naoaki、Kawamura Junichi
    • Journal Title

      Solid State Ionics

      Volume: 320 Pages: 38-44

    • DOI

      10.1016/j.ssi.2018.02.024

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Milling effect on the local structure, site occupation, and site migration in aluminum substituted lithium manganese oxides2018

    • Author(s)
      Nakamura Koichi、Shimokita Kosuke、Sakamoto Yoichi、Koyama Kuniyuki、Moriga Toshihiro、Kuwata Naoaki、Iwai Yoshiki、Kawamura Junichi
    • Journal Title

      Solid State Ionics

      Volume: 317 Pages: 214-220

    • DOI

      10.1016/j.ssi.2018.01.019

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electrochemical properties of LiCoO2 thin film surface modified by lithium tantalate and lithium niobate coatings2017

    • Author(s)
      Kato Mikako、Hayashi Tetsutaro、Hasegawa Gen、Lu Xiaoli、Miyazaki Takamichi、Matsuda Yasutaka、Kuwata Naoaki、Kurihara Koji、Kawamura Junichi
    • Journal Title

      Solid State Ionics

      Volume: 308 Pages: 54-60

    • DOI

      10.1016/j.ssi.2017.05.008

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] High-power durability of LiCoO2 thin film electrode modified with amorphous lithium tungsten oxide2017

    • Author(s)
      Tetsutaro Hayashi, Yasutaka Matsuda, Naoaki Kuwata, Junichi Kawamura
    • Journal Title

      Journal of Power Sources

      Volume: 354 Pages: 41-47

    • DOI

      10.1016/j.jpowsour.2017.04.036

    • Related Report
      2017 Annual Research Report 2016 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Lithium diffusion coefficient in amorphous lithium phosphate thin films measured by secondary ion mass spectroscopy with isotope exchange methods2016

    • Author(s)
      N Kuwata, X Lu, T Miyazaki, Y Iwai, T Tanabe, J Kawamura
    • Journal Title

      Solid State Ionics

      Volume: 294 Pages: 59-66

    • DOI

      10.1016/j.ssi.2016.06.015

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed / Open Access / Acknowledgement Compliant
  • [Journal Article] Effect of lithium-ion diffusibility on interfacial resistance of LiCoO2 thin film electrode modified with lithium tungsten oxides2016

    • Author(s)
      Tetsutaro Hayashi, Takamichi Miyazaki, Yasutaka Matsuda, Naoaki Kuwata, Motoaki Saruwatari, Yuki Furuichi, Koji Kurihara, Ryuichi Kuzuo, Junichi Kawamura
    • Journal Title

      Journal of Power Sources

      Volume: 305 Pages: 46-53

    • DOI

      10.1016/j.jpowsour.2015.11.075

    • Related Report
      2016 Annual Research Report 2015 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Direct measurement of nanoscale lithium diffusion in solid battery materials using radioactive tracer of 8Li2016

    • Author(s)
      H. Ishiyama, S.C. Jeong, Y.X. Watanabe, Y. Hirayama, N. Imai, H.S. Jung, H. Miyatake, M. Oyaizu, A. Osa, Y. Otokawa, M. Matsuda, K. Nishio, H. Makii, T.K. Sato, N. Kuwata, J. Kawamura, H. Ueno, Y.H. Kim, S. Kimura, M. Mukai
    • Journal Title

      Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms

      Volume: - Pages: 379-381

    • DOI

      10.1016/j.nimb.2015.12.036

    • Related Report
      2016 Annual Research Report 2015 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Relationship between structure and mobility of proton carriers injected by electrochemical substitution of sodium ions with protons in 35NaO 1/2-1 WO 3-8NbO 5/2-5LaO 3/2-51PO 5/2-based glasses2016

    • Author(s)
      Takuya Yamaguchi, Tomohiro Ishiyama, Kanji Sakuragi, Junji Nishii, Toshiharu Yamashita, Hiroshi Kawazoe, Naoaki Kuwata, Junichi Kawamura, Takahisa Omata
    • Journal Title

      Solid State Ionics

      Volume: 288 Pages: 281-285

    • DOI

      10.1016/j.ssi.2016.01.024

    • Related Report
      2016 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Electromotive force measurements of LiCoO2 electrode on a lithium ion-conducting glass ceramics under mechanical stress2016

    • Author(s)
      Keita Funayama, Takashi Nakamura, Naoaki Kuwata, Junichi Kawamura, Tatsuya Kawada, Koji Amezawa
    • Journal Title

      Solid State Ionics

      Volume: 285 Pages: 75-78

    • DOI

      10.1016/j.ssi.2015.09.009

    • Related Report
      2016 Annual Research Report 2015 Annual Research Report
    • Peer Reviewed
  • [Presentation] 二次イオン質量分析法によるLixCoO2薄膜のLi自己拡散係数の組成依存性測定2017

    • Author(s)
      長谷川源, 桑田直明, 石垣範和, 河村純一
    • Organizer
      日本物理学会第72回年次大会
    • Place of Presentation
      大阪大学豊中キャンパス(大阪府吹田市)
    • Year and Date
      2017-03-17
    • Related Report
      2016 Annual Research Report
  • [Presentation] LixMn2O4薄膜におけるリチウムイオン拡散係数の組成依存性2017

    • Author(s)
      前田大輝, 中根正勝, 長谷川源, 石垣範和, 桑田直明, 河村純一
    • Organizer
      日本物理学会 第72回年次大会
    • Place of Presentation
      大阪大学豊中キャンパス(大阪府吹田市)
    • Year and Date
      2017-03-17
    • Related Report
      2016 Annual Research Report
  • [Presentation] 二次イオン質量分析法によるLixMn2O4薄膜のリチウム拡散係数の組成依存性測定2017

    • Author(s)
      桑田直明,前田大輝,中根正勝,長谷川源,宮崎孝道,石垣範和,河村純一
    • Organizer
      第20回 超イオン導電体物性研究会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 二次イオン質量分析を用いたLiMn2O4薄膜のリチウム拡散係数測定2017

    • Author(s)
      中根正勝,桑田直明,宮崎孝道,河村純一
    • Organizer
      第20回 超イオン導電体物性研究会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 二次イオン質量分析法によるLi脱離LixMn2O4正極のリチウム拡散係数測定2017

    • Author(s)
      桑田直明,前田大輝,中根正勝,長谷川源,宮崎孝道,河村純一
    • Organizer
      日本物理学会2017年秋季大会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 5V級正極LiCoMnO4薄膜の軟X線XAFSによる局所構造解析2017

    • Author(s)
      石垣範和,山中恵介,桑田直明,河村純一
    • Organizer
      日本物理学会2017年秋季大会
    • Related Report
      2017 Annual Research Report
  • [Presentation] LixCoO2薄膜におけるLi自己拡散係数の組成依存性2017

    • Author(s)
      長谷川源,桑田直明,宮崎孝道,石垣範和,河村純一
    • Organizer
      日本物理学会2017年秋季大会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 二次イオン質量分析法を用いたLixMn2O4薄膜のリチウム拡散係数の測定2017

    • Author(s)
      桑田 直明、前田 大輝、中根 正勝、長谷川 源、宮崎 孝道、河村 純一
    • Organizer
      第58回 電池討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] LixCoO2薄膜におけるLi自己拡散係数の組成依存性2017

    • Author(s)
      長谷川源,桑田直明,宮崎孝道,石垣範和,河村純一
    • Organizer
      電気化学会東北支部 第30回 東北若手の会
    • Related Report
      2017 Annual Research Report
  • [Presentation] LixMn2O4薄膜におけるリチウム拡散係数の組成依存性2017

    • Author(s)
      前田大輝、中根正勝、長谷川源、宮崎孝道、石垣範和、桑田直明、河村純一
    • Organizer
      第43回 固体イオニクス討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] LixCoO2薄膜におけるLi自己拡散係数の組成依存性2017

    • Author(s)
      長谷川源、桑田直明、宮崎孝道、石垣範和、河村純一
    • Organizer
      第43回 固体イオニクス討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 薄膜電池にみる固体電池の材料化学: 5Vリチウム電池と自己拡散係数2017

    • Author(s)
      桑田 直明,河村 純一
    • Organizer
      第 99回 新電池構想部会
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] Lithium Diffusion Coefficient of Thin-Film Lithium Battery Materials Measured by Secondary Ion Mass Spectrometry2017

    • Author(s)
      Naoaki Kuwata, Xiaoli Lu, Masakatsu Nakane, Gen Hasegawa, Daiki Maeda, Takamichi Miyazaki, Junichi Kawamura
    • Organizer
      21th International Conference on Solid State Ionics
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 5 V all-solid-state thin-film battery with LixCoMnO4 prepared by PLD and post annealing2017

    • Author(s)
      Norikazu Ishigaki, Naoaki Kuwata, Junichi Kawamura
    • Organizer
      21th International Conference on Solid State Ionics
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] High-Rate Pulsed Laser Deposition for Thin-Film Solid-State Battery2017

    • Author(s)
      Naoaki Kuwata, Yasutaka Matsuda, Junichi Kawamura
    • Organizer
      21th International Conference on Solid State Ionics
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Composition dependence of Li self-diffusion coefficient in LixCoO2 thin films measured by secondary ion mass spectrometry2017

    • Author(s)
      Gen Hasegawa, Naoaki Kuwata, Takamichi Miyazaki, Rie Shishido, Norikazu Ishigaki, Junichi Kawamura
    • Organizer
      21th International Conference on Solid State Ionics
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Lithium Tracer Diffusion Coefficients in LixMn2O4 thin films2017

    • Author(s)
      Daiki Maeda, Masakatsu Nakane, Gen Hasegawa, Norikazu Ishigaki, Takamichi Miyazaki, Naoaki Kuwata, Junichi Kawamura
    • Organizer
      21th International Conference on Solid State Ionics
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 二次イオン質量分析を用いたa-Li3PO4薄膜のリチウム拡散係数測定2016

    • Author(s)
      桑田直明, 芦小麗, 宮崎孝道, 河村純一
    • Organizer
      第42回固体イオニクス討論会
    • Place of Presentation
      名古屋国際会議場(愛知県名古屋市)
    • Year and Date
      2016-12-05
    • Related Report
      2016 Annual Research Report
  • [Presentation] SIMSを用いたa-Li3PO4薄膜のリチウムトレーサー拡散係数測定2016

    • Author(s)
      桑田直明, 芦小麗, 宮崎孝道, 岩井良樹, 河村純一
    • Organizer
      第57回電池討論会
    • Place of Presentation
      幕張メッセ国際会議場(千葉県千葉市)
    • Year and Date
      2016-11-29
    • Related Report
      2016 Annual Research Report
  • [Presentation] Electrochemical Property of LiCoMnO4 Cathode Thin Film Prepared By PLD and Oxygen Post Annealing2016

    • Author(s)
      N. Ishigaki, N. Kuwata, J. Kawamura
    • Organizer
      PRiME 2016 / 230th ECS Meeting
    • Place of Presentation
      Hawaii (USA)
    • Year and Date
      2016-10-02
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Lithium Diffusion Coefficient of Amorphous Lithium Phosphate Thin Films Measured By Secondary Ion Mass Spectroscopy2016

    • Author(s)
      X. Lu, N. Kuwata, T. Miyazaki, J. Kawamura
    • Organizer
      PRiME 2016 / 230th ECS Meeting
    • Place of Presentation
      Hawaii (USA)
    • Year and Date
      2016-10-02
    • Related Report
      2016 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 二次イオン質量分析とマスク法によるa-Li3PO4のリチウム拡散係数測定2016

    • Author(s)
      桑田直明, 芦小麗, 宮崎孝道, 岩井良樹, 河村純一
    • Organizer
      日本物理学会2016年秋季大会
    • Place of Presentation
      金沢大学角間キャンパス(石川県金沢市)
    • Year and Date
      2016-09-13
    • Related Report
      2016 Annual Research Report
  • [Presentation] 二次イオン質量分析法によるLiCoO2薄膜のリチウム拡散係数測定2015

    • Author(s)
      桑田直明, 西尾仁志, 宮崎孝道, 河村純一
    • Organizer
      第41回 固体イオニクス討論会
    • Place of Presentation
      北海道札幌市、北海道大学工学部フロンティア応用科学研究棟
    • Year and Date
      2015-11-25
    • Related Report
      2015 Annual Research Report
  • [Presentation] 高速PLD製膜LiCoO2正極を用いた全固体薄膜リチウム電池の特性2015

    • Author(s)
      松田康孝, 桑田直明, 河村純一
    • Organizer
      第41回 固体イオニクス討論会
    • Place of Presentation
      北海道札幌市、北海道大学工学部フロンティア応用科学研究棟
    • Year and Date
      2015-11-25
    • Related Report
      2015 Annual Research Report
  • [Presentation] パルスレーザー堆積法による全固体リチウム電池の高速製膜2015

    • Author(s)
      桑田 直明, 松田 康孝, 河村 純一
    • Organizer
      第56回 電池討論会
    • Place of Presentation
      愛知県名古屋市、愛知県産業労働センター ウインクあいち
    • Year and Date
      2015-11-11
    • Related Report
      2015 Annual Research Report
  • [Presentation] Solid-state Lithium Batteries with Thin-Film Amorphous Electrolyte2015

    • Author(s)
      Naoaki Kuwata
    • Organizer
      Twelfth International Conference on Flow Dynamics
    • Place of Presentation
      Sendai, Sendai international center
    • Year and Date
      2015-10-27
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 二次イオン質量分析法を用いたLiCoO2薄膜のリチウム拡散係数測定2015

    • Author(s)
      桑田直明, 西尾仁志, 宮崎孝道, 河村純一
    • Organizer
      日本物理学会 2015年秋季大会
    • Place of Presentation
      大阪府吹田市、関西大学千里山キャンパス
    • Year and Date
      2015-09-16
    • Related Report
      2015 Annual Research Report
  • [Presentation] In Situ Raman Spectroscopy of Thin-Film Battery Li/Li3PO4/LiMn2O4 Using a Transparent Electrode2015

    • Author(s)
      Naoaki Kuwata, Tatsunori Okawa, Yasutaka Matsuda, Osamu Kamishima and Junichi Kawamura
    • Organizer
      20th International Conference on Solid State Ionics (SSI-20)
    • Place of Presentation
      Keystone, Colorado, USA
    • Year and Date
      2015-06-14
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research

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Published: 2015-04-16   Modified: 2022-08-30  

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