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Understanding the Charge-Discharge Processes for Alloy Negative Electrode Thin Films on Oxide Solid Electrolytes

Research Project

Project/Area Number 17H04894
Research Category

Grant-in-Aid for Young Scientists (A)

Allocation TypeSingle-year Grants
Research Field Inorganic industrial materials
Research InstitutionNagoya University

Principal Investigator

Motoyama Munekazu  名古屋大学, 工学研究科, 講師 (30705752)

Project Period (FY) 2017-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥24,830,000 (Direct Cost: ¥19,100,000、Indirect Cost: ¥5,730,000)
Fiscal Year 2019: ¥5,720,000 (Direct Cost: ¥4,400,000、Indirect Cost: ¥1,320,000)
Fiscal Year 2018: ¥5,720,000 (Direct Cost: ¥4,400,000、Indirect Cost: ¥1,320,000)
Fiscal Year 2017: ¥13,390,000 (Direct Cost: ¥10,300,000、Indirect Cost: ¥3,090,000)
Keywords全固体型Li電池 / 走査型電子顕微鏡 / その場観察 / 合金負極 / Li金属負極 / 合金化反応 / Li金属の析出溶解反応 / その場走査型電子顕微鏡観察 / 全固体電池 / Au / Li / LiPON / 反射電子像 / 全固体リチウム電池 / リチウムイオン伝導性固体電解質 / その場SEM観察 / Si / Pt / 合金化・脱合金化反応 / 電気化学 / 全固体型リチウム電池 / その場観察測定
Outline of Final Research Achievements

In-situ observations of the alloying process of Li and Au on lithium oxynitride glass (LiPON) electrolytes using scanning electron microscopy (SEM) revealed that Li partly re-dissolved in Au after the Li nucleation. Moreover, in-situ SEM observations revealed that no Li was grown from Ta-doped Li7La3Zr2O12 (LLZT) surfaces polished with SiC papers. It was also found that immersing a LLZT pellet in an acid aqueous solution for a short period of time removed the damaged layer on the surface that resulted from SiC polishing. The acid-etched-LLZT surface showed high wettability with molten Li, and acid-etched LLZT showed Li plating/stripping cycles with high stability.

Academic Significance and Societal Importance of the Research Achievements

酸化物系無機固体電解質上で起こるLiとAuの合金化反応は、その初期において、面内の合金組成が極めて不均一であることを明らかにした。また、Liが核生成した直後には、一部のLiがLi-Au合金中へ再溶解することを明らかにした。これは、動的観察を通じて初めてとらえることができた現象であり 、合金化反応に対する理解を新たにさせる観察結果であった。
本研究で用いたその場走査型電子顕微鏡観察(SEM)技術は、合金負極材料の充放電過程を解析する上で有効であることを実証した。

Report

(4 results)
  • 2019 Annual Research Report   Final Research Report ( PDF )
  • 2018 Annual Research Report
  • 2017 Annual Research Report
  • Research Products

    (40 results)

All 2020 2019 2018 2017 Other

All Journal Article (5 results) (of which Peer Reviewed: 3 results) Presentation (32 results) (of which Int'l Joint Research: 16 results,  Invited: 6 results) Book (2 results) Remarks (1 results)

  • [Journal Article] Understanding the short-circuiting mechanism of solid-state electrolytes for realizing high performance of an all-solid-state-lithium battery2020

    • Author(s)
      本山 宗主、山本 貴之、入山 恭寿
    • Journal Title

      Oyo Buturi

      Volume: 89 Issue: 4 Pages: 213-217

    • DOI

      10.11470/oubutsu.89.4_213

    • NAID

      130007830116

    • ISSN
      0369-8009, 2188-2290
    • Year and Date
      2020-04-10
    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 酸化物系全固体Li電池におけるLi金属負極の課題2020

    • Author(s)
      本山宗主、山本貴之、入山恭寿
    • Journal Title

      工業材料

      Volume: 68 Pages: 41-46

    • Related Report
      2019 Annual Research Report
  • [Journal Article] The Active Interface of Ta-Doped Li7La3Zr2O12 for Li Plating/Stripping Revealed by Acid Aqueous Etching2019

    • Author(s)
      Motoyama Munekazu、Tanaka Yuki、Yamamoto Takayuki、Tsuchimine Nobuo、Kobayashi Susumu、Iriyama Yasutoshi
    • Journal Title

      ACS Applied Energy Materials

      Volume: 2 Issue: 9 Pages: 6720-6731

    • DOI

      10.1021/acsaem.9b01193

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed
  • [Journal Article] In situ scanning electron microscope observations of Li plating/stripping reactions with Pt current collectors on LiPON electrolyte2018

    • Author(s)
      M. Motoyama, M. Ejiri, T. Yamamoto, and Y. Iriyama
    • Journal Title

      Journal of the Electrochemical Society

      Volume: 165 Issue: 7 Pages: A1338-A1347

    • DOI

      10.1149/2.0411807jes

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] 酸化物系無機固体電解質を介したLi金属の析出溶解機構2018

    • Author(s)
      本山宗主、入山恭寿
    • Journal Title

      電気化学

      Volume: 86 Pages: 286-292

    • Related Report
      2018 Annual Research Report
  • [Presentation] In-Situ SEM Studies on Electrochemical Li Nucleation, Growth, and Dissolution in Oxide Solid Electrolyte Systems2020

    • Author(s)
      Munekazu Motoyama, Takayuki Yamamoto, and Yasutoshi Iriyama
    • Organizer
      44th International Conference and Expo on Advanced Ceramics and Composites (ICACC 2020)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] LiPONガラス電解質上におけるLiの析出溶解反応に及ぼす温度の影響2020

    • Author(s)
      本山宗主,廣田正陽,山本貴之,入山恭寿
    • Organizer
      電気化学会第87回大会
    • Related Report
      2019 Annual Research Report
  • [Presentation] 酸化物系無機固体電解質上におけるLiの析出溶解反応に及ぼす温度と圧力の影響2019

    • Author(s)
      本山宗主,北川瑞貴,廣田正陽,山本貴之,入山恭寿
    • Organizer
      第60回電池討論会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Li Plating/Stripping Reactions on Li6.6La3Ta0.4Zr1.6O122019

    • Author(s)
      Munekazu Motoyama
    • Organizer
      236th ECS Meeting
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Temperature Effects on the Nucleation and Growth of Li at Cu/LiPON Interface2019

    • Author(s)
      Masaharu Hirota, Munekazu Motoyama, Takayuki Yamamoto, and Yasutoshi Iriyama
    • Organizer
      2nd World Conference on Solid Electrolytes for Advanced Applications: Garnets and Competitors
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Measurements of Critical Current Densities for Ta-Doped Li7La3Zr2O122019

    • Author(s)
      Mizuki Kitagawa, Yuki Tanaka, Takayuki Yamamoto, Munekazu Motoyama, and Yasutoshi Iriyama
    • Organizer
      2nd World Conference on Solid Electrolytes for Advanced Applications: Garnets and Competitors
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] In-Situ SEM Studies on Li Plating/Stripping Reactions on Oxide Solid Electrolytes2019

    • Author(s)
      Munekazu Motoyama, Takayuki Yamamoto, and Yasutoshi Iriyama
    • Organizer
      2nd World Conference on Solid Electrolytes for Advanced Applications: Garnets and Competitors
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Li6.6La3Zr1.6Ta0.4O12の短絡に及ぼす温度と圧力の影響2019

    • Author(s)
      本山宗主,北川瑞貴,山本貴之,入山恭寿
    • Organizer
      2019年電気化学会秋季大会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Temperature Effects on the Nucleation and Growth of Li at Cu/LiPON Interface2019

    • Author(s)
      Masaharu Hirota,Munekazu Motoyama,Takayuki Yamamoto, and Yasutoshi Iriyama
    • Organizer
      SSDM2019
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] In-Situ Scanning Electron Microscope Observations of Li Plating/Stripping Reactions on Ta-doped Li7La3Zr2O122019

    • Author(s)
      Munekazu Motoyama
    • Organizer
      22nd International Conference on Solid State Ionics
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Temperature Effects on the Nucleation and Growth of Li at Cu/LiPON Interface2019

    • Author(s)
      Masaharu Hirota, Munekazu Motoyama, Takayuki Yamamoto, and Yasutoshi Iriyama
    • Organizer
      22nd International Conference on Solid State Ionics
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ガーネット型酸化物固体電解質上におけるLiの析出溶解反応に及ぼす温度と圧力の影響2019

    • Author(s)
      本山宗主,田中佑樹,山本貴之,入山恭寿
    • Organizer
      電気化学会第86回大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Li6.6La3Zr1.6Ta0.4O12上におけるLiの析出溶解反応2018

    • Author(s)
      本山宗主,田中佑樹,山本貴之,入山恭寿
    • Organizer
      第20回化学電池材料研究会ミーティング
    • Related Report
      2018 Annual Research Report
  • [Presentation] Li Plating/Stripping Reactions on Oxide Solid Electrolytes2018

    • Author(s)
      M. Motoyama,Y. Tanaka,T. Yamamoto,and Y. Iriyama
    • Organizer
      IMLB2018
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 酸化物系全固体リチウム電池のためのリチウム金属負極に関する研究2018

    • Author(s)
      本山宗主
    • Organizer
      平成30年度日本金属学会・日本鉄鋼協会両北海道支部合同サマーセッション
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] Li6.6La3Zr1.6Ta0.4O12 上におけるLiの析出溶解反応に及ぼす温度と圧力の影響2018

    • Author(s)
      本山宗主,田中佑樹,山本貴之,入山恭寿
    • Organizer
      2018年電気化学秋季大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] LiPONガラス電解質上で起こるLi析出溶解反応の温度依存性2018

    • Author(s)
      廣田正陽,山本貴之,本山宗主,入山恭寿
    • Organizer
      第49回中部化学関係学協会支部連合秋季大会
    • Related Report
      2018 Annual Research Report
  • [Presentation] In Situ Scanning Electron Microscope Observations of Li Plating/Stripping Reactions on Oxide Solid Electrolytes2018

    • Author(s)
      M. Motoyama
    • Organizer
      2018 MRS Fall Meeting & Exhibit
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Li6.6La3Zr1.6Ta0.4O12上で起こるLiの析出溶解反応2018

    • Author(s)
      田中佑樹,本山宗主,山本貴之,入山恭寿
    • Organizer
      第59回電池討論会
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 酸化物系固体電解質上におけるLi析出溶解反応の温度依存性2018

    • Author(s)
      本山宗主,廣田正陽,田中佑樹,髙倉武朗,山本貴之,入山恭寿
    • Organizer
      第59回電池討論会
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Li6.6La3Zr1.6Ta0.4O12上におけるLiの析出溶解反応2018

    • Author(s)
      本山宗主
    • Organizer
      電気化学会第85回大会
    • Related Report
      2017 Annual Research Report
  • [Presentation] 酸化物系無機固体電解質上におけるLi金属の析出溶解反応2017

    • Author(s)
      本山宗主
    • Organizer
      第19回化学電池材料研究会ミーティング
    • Related Report
      2017 Annual Research Report
  • [Presentation] In-Situ SEM Observations of Electrochemical Li Deposition/Dissolution on Solid State Electrolytes2017

    • Author(s)
      Munekazu Motoyama
    • Organizer
      A Modern Look at Energy, Nano/Rapid Manufacturing, and Robotics
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Li Plating/Stripping Reactions on Ta-Doped Li7La3Zr2O122017

    • Author(s)
      Yuki Tanaka
    • Organizer
      1st World Conference on Solid Electrolytes for Advanced Applications: Garnets and Competitors
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ガーネット型酸化物固体電解質上におけるLi析出溶解反応のin-situ SEM観察2017

    • Author(s)
      本山宗主
    • Organizer
      2017年電気化学秋季大会
    • Related Report
      2017 Annual Research Report
  • [Presentation] グラフェン/LiPON界面におけるLi+挿入脱離反応2017

    • Author(s)
      三好啓太
    • Organizer
      2017年電気化学秋季大会
    • Related Report
      2017 Annual Research Report
  • [Presentation] TaドープしたLi7La3Zr2O12上におけるLi析出溶解反応2017

    • Author(s)
      田中佑樹
    • Organizer
      電気化学会九州支部・東海支部合同シンポジウム
    • Related Report
      2017 Annual Research Report
  • [Presentation] 酸化物系固体電解質上におけるLi金属の析出溶解反応2017

    • Author(s)
      本山宗主
    • Organizer
      日本セラミックス協会第30回秋季シンポジウム
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] 酸化物系固体電解質上におけるLi金属の析出溶解反応2017

    • Author(s)
      本山宗主
    • Organizer
      電池技術委員会
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] 酸化物系固体電解質上におけるLi金属の析出溶解反応2017

    • Author(s)
      本山宗主
    • Organizer
      第58回電池討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] In-Situ Scanning Electron Microscope Observations of the Nucleation and Growth of Li metal on Oxide Solid Electrolytes2017

    • Author(s)
      Munekazu Motoyama
    • Organizer
      2017 MRS Fall Meeting & Exhibit
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Li+ Intercalation and Deintercalation Reactions with Graphene Films on LiPON2017

    • Author(s)
      Keita Miyoshi
    • Organizer
      2017 MRS Fall Meeting & Exhibit
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Book] 全固体リチウム電池の開発動向と応用展望2019

    • Author(s)
      本山 宗主、入山 恭寿
    • Total Pages
      12
    • Publisher
      シーエムシー出版
    • Related Report
      2019 Annual Research 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:LiPONガラス電解質上で起こるLiの核生成・成長過程のその場走査型電子顕微鏡観察2017

    • Author(s)
      本山宗主
    • Total Pages
      7
    • Publisher
      技術情報協会
    • Related Report
      2017 Annual Research Report
  • [Remarks]

    • URL

      http://profs.provost.nagoya-u.ac.jp/view/html/100006615_ja.html

    • Related Report
      2018 Annual Research Report

URL: 

Published: 2017-04-28   Modified: 2021-02-19  

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