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Development of garnet type mixed anionic solid electrolytes challenging from an atomistic crystal growth technique

Publicly Offered Research

Project AreaSynthesis of Mixed Anion Compounds toward Novel Functionalities
Project/Area Number 17H05479
Research Category

Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)

Allocation TypeSingle-year Grants
Review Section Science and Engineering
Research InstitutionShinshu University

Principal Investigator

是津 信行  信州大学, 学術研究院工学系, 教授 (10432519)

Project Period (FY) 2017-04-01 – 2019-03-31
Project Status Completed (Fiscal Year 2018)
Budget Amount *help
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2018: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
Fiscal Year 2017: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
Keywords結晶工学 / 結晶成長 / イオン結晶 / 表面・界面物性 / セラミックス / 固体電解質 / 全固体電池
Outline of Annual Research Achievements

平成29年度の成果を基に,ガーネット型固体電解質結晶表面の酸硫化について検討した。具体的には,1. 硫黄源にヘキサンジチオールを用いた単分子膜修飾手法,2. Na2Sフラックスからの再結晶法,3.メカニカルミリング法についてそれぞれ検討した。加えて,第一原理計算による,相安定性の観点から,反応ルート探索を進めた。結果として,すべての手法において,ガーネット型固体電解質結晶表面を酸硫化できる可能性を明らかにした。1で処理した酸硫化表面をもつ,Al0.25Li6.25La3Zr2O12では,酸化物と比較して,焼結後のペレット成型体の相対密度は63 %から87 %に向上した。ペレット破断面のFE-SEM像では,粒子間のネッキング成長においてチオール処理の優位な差が認められた。この結果は,酸硫化表面の形成による表面拡散速度の促進を示唆している。酸硫化表面による効果と推察する。2の手法では,XRD測定から,副相として,La2Zr2O7に帰属されるピークを観測した。Na2Sのモル分率が大きくなるほど,La2Zr2O7に帰属されるピーク強度は増加した。硫黄の固溶限界によりLi6.75La3Zr1.75Nb0.25O12が分解して,La2Zr2O7が生成した可能性が高い。3では,Li6.75La3Zr1.75Nb0.25O12とLi2Sのメカニカルミリングにより,酸硫化表面の形成を試みた。処理後の粉末のXPS-La 3dコアレベルスペクトルから,La-S結合に帰属するピークを検出した。これにより,酸硫化表面の生成を明らかにできた。これらの成果の一部は,現在特許出願準備中である。出願後,速やかに論文投稿する。

Research Progress Status

平成30年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

平成30年度が最終年度であるため、記入しない。

Report

(2 results)
  • 2018 Annual Research Report
  • 2017 Annual Research Report
  • Research Products

    (28 results)

All 2020 2019 2018 2017 Other

All Int'l Joint Research (2 results) Journal Article (9 results) (of which Int'l Joint Research: 1 results,  Peer Reviewed: 9 results,  Open Access: 2 results) Presentation (14 results) (of which Int'l Joint Research: 6 results,  Invited: 10 results) Patent(Industrial Property Rights) (3 results)

  • [Int'l Joint Research] モンペリエ大学(フランス)

    • Related Report
      2018 Annual Research Report
  • [Int'l Joint Research] 香港城市大学(中国)

    • Related Report
      2018 Annual Research Report
  • [Journal Article] Molecular Dynamics Studies on the Lithium Ion Conduction Behaviors Depending on Tilted Grain Boundaries with various symmetries in Garnet-Type Li7La3Zr2O122020

    • Author(s)
      H. Shiiba, N. Zettsu, M. Yamashita, H. Onodera, R. Jalem, M. Nakayama, K. Teshima
    • Journal Title

      The Journal of Physical Chemistry C.

      Volume: 0 Issue: 38 Pages: 21755-21762

    • DOI

      10.1021/acs.jpcc.8b06275

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Impact of trace extrinsic defect formation on the local symmetry transition in spinel LiNi0.5Mn1.5O4-δ and their electrochemical characteristics2018

    • Author(s)
      Hiromasa Shiiba,Nobuyuki Zettsu, Satoru Kida, Dae-wook Kim, and Katsuya Teshima
    • Journal Title

      Journal of Materials Chemistry A

      Volume: 6 Issue: 45 Pages: 22749-22757

    • DOI

      10.1039/c8ta07825d

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] One-Dimensional Growth of Li2NiPO4F Single Crystals from Intermediate LiNiPO4 Crystal Surface Using KCl-KI Molten Fluxes2018

    • Author(s)
      Tetsuya Yamada,Nobuyuki Zettsu, Hye-min Kim, Yuta Hagano, Nobuyuki Handa, Kunio Yubuta, and Katsuya Teshima
    • Journal Title

      Crystal Growth & Design

      Volume: 18 Issue: 11 Pages: 6777-6785

    • DOI

      10.1021/acs.cgd.8b01031

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Thin and dense solid-solid heterojunction formation promoted by crsytal grwoth in flux on a substrate2018

    • Author(s)
      Nobuyuki Zettsu, Hiromasa Shiiba, Hitoshi Onodera, Kazune Nemoto, Takeshi Kimijima, Kunio Yubuta, Masanobu Nakayama, Katsuya Teshima
    • Journal Title

      Scientific Reports

      Volume: 96 Issue: 1 Pages: 1-11

    • DOI

      10.1038/s41598-017-18250-9

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Full picture discovery for mixed-fluorine anion effects on high-voltage spinel lithium nickel manganese oxide cathodes2017

    • Author(s)
      Kim Dae-wook、Shiiba Hiromasa、Zettsu Nobuyuki、Yamada Tetsuya、Kimijima Takeshi、S?nchez-Santolino Gabriel、Ishikawa Ryo、Ikuhara Yuichi、Teshima Katsuya
    • Journal Title

      NPG Asia Materials

      Volume: 9 Issue: 7 Pages: e398-e398

    • DOI

      10.1038/am.2017.90

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Intrinsic electrochemical characteristics of one LiNi0.5Mn1.5O4 spinel particle2017

    • Author(s)
      Kei Nishikawa, Nobuyuki Zettsu, Katsuya Teshima, Kiyoshi Kanamura
    • Journal Title

      Journal of Electroanalytical Chemistry

      Volume: 799 Pages: 468-472

    • DOI

      10.1016/j.jelechem.2017.06.042

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] フラックス法が拓くリチウムイオン二次電池用材料革新2017

    • Author(s)
      手嶋勝弥,是津信行
    • Journal Title

      C&I Commun

      Volume: 42 Pages: 30-33

    • NAID

      40021626148

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] テンプレートを導入したフラックス法による無機結晶の形態制御育成2017

    • Author(s)
      山田哲也,鈴木清香,是津信行,手嶋勝弥
    • Journal Title

      日本結晶成長学会誌

      Volume: 42 Pages: 88-95

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Journal Article] リチウムイオン二次電池の高電圧作動を可能にする電極表面処理技術2017

    • Author(s)
      手嶋勝弥,是津信行
    • Journal Title

      車載テクノロジー

      Volume: 4 Pages: 41-45

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed
  • [Presentation] Space control for Li+ storage and transport in spinel LiNi0.5Mn1.5O4 systems through synergistic effects of dually-incorporated Fvo and CuMn defects2018

    • Author(s)
      Nobuyuki Zettsu
    • Organizer
      Hong Kong Symposium of Batteries
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 超空間制御から完全表面創成まで,リチウムイオン電池材料に求められる結晶技術2018

    • Author(s)
      是津信行
    • Organizer
      第47回結晶成長国内会議
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] 電池材料分野におけるコマンドサーフェス型機能創発2018

    • Author(s)
      是津信行
    • Organizer
      表面技術協会第138回講演大会
    • Related Report
      2018 Annual Research Report
    • Invited
  • [Presentation] Mixed anion compounds for the promotion of new battery materials chemistry2018

    • Author(s)
      Nobuyuki Zettsu
    • Organizer
      IUMRS-ICEM2018
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Surface oxysulfidation of LiNi0.5Mn1.5O4 single crystals and characterization of their electrochemical properties2018

    • Author(s)
      Dae-wook Kim, Hiromasa Shiiba, Nobuyuki Zettsu, Katsuya Teshima
    • Organizer
      第59回電池討論会
    • Related Report
      2018 Annual Research Report
  • [Presentation] フラックス法を援用した電池材料革新:超空間制御5Vスピネル結晶2017

    • Author(s)
      是津信行,手嶋勝弥
    • Organizer
      第12回日本フラックス成長研究発表会
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] Electrolyte/electrode interface engineering toward advanced Lithium-ion batteries2017

    • Author(s)
      N. Zettsu, K. Teshima
    • Organizer
      Surface Treatment and Modification Technology 2017
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Mixed anion effects on high-voltage spinel manganese cathodes2017

    • Author(s)
      N. Zettsu, D.W. Kim, H. Shiiba, K. Teshima
    • Organizer
      The 4th International Symposium on Hybrid Materials and Processing
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 超空間制御5Vスピネル結晶材料の開発2017

    • Author(s)
      是津信行,手嶋勝弥
    • Organizer
      電気化学会九州支部・東海支部合同シンポジウム2017
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Presentation] Crystal growth of advanced LIB materials in molten fluxes offer a new way for discovering cutting-edge materials2017

    • Author(s)
      N. Zettsu, K. Teshima
    • Organizer
      8th International Conference on Electroceramics
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 高容量および長サイクル寿命のためのリチウム過剰 5V スピネルの電気化学的性能に及ぼす元素置換効果2017

    • Author(s)
      是津信行,キムデウク,椎葉寛将,手嶋勝弥
    • Organizer
      第58回電池討論会
    • Related Report
      2017 Annual Research Report
  • [Presentation] カチオン・アニオン空間制御したLiNi0.5Mn1.5O4結晶のフラックス育成とその電気化学特性2017

    • Author(s)
      是津信行,キムデウク,椎葉寛将,手嶋勝弥
    • 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
  • [Presentation] Full Picture Discovery for Mixed-Fluorine Anion Effects on High-Voltage Spinel Manganese Cathodes2017

    • Author(s)
      T. Yamada, N. Zettsu, D. Kim, S. Kaneko, K. Teshima
    • Organizer
      The 21st International Conference of Solid State Ionics
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 複合アニオン化合物結晶材料の創製と新機能2017

    • Author(s)
      是津信行
    • Organizer
      第二回複合アニオン公開シンポジウム
    • Related Report
      2017 Annual Research Report
    • Invited
  • [Patent(Industrial Property Rights)] リチウム複合酸化物,二次電池用電極活物質,二次電池,およびリチウム複合酸化物の製造方法2019

    • Inventor(s)
      手嶋勝弥,是津信行,キムヘミン
    • Industrial Property Rights Holder
      信州大学
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2019-069187
    • Filing Date
      2019
    • Related Report
      2018 Annual Research Report
  • [Patent(Industrial Property Rights)] リチウム複合酸化物、二次電池用電極材料、二次電池及びリチウム複合酸化物の製造方法2018

    • Inventor(s)
      手嶋勝弥,是津信行,キムデウク,キムヘミン
    • Industrial Property Rights Holder
      信州大学
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2018-066581
    • Filing Date
      2018
    • Related Report
      2017 Annual Research Report
  • [Patent(Industrial Property Rights)] リチウム複合酸化物、二次電池用正極活物質及び二次電池2018

    • Inventor(s)
      手嶋勝弥,是津信行,金大旭,寛将椎葉
    • Industrial Property Rights Holder
      信州大学
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2018-066494
    • Filing Date
      2018
    • Related Report
      2017 Annual Research Report

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Published: 2017-04-28   Modified: 2021-01-27  

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