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液相法によるリチウムイオン伝導性酸化物の低温合成

Research Project

Project/Area Number 13F03371
Research Category

Grant-in-Aid for JSPS Fellows

Allocation TypeSingle-year Grants
Section外国
Research Field Inorganic materials/Physical properties
Research InstitutionHokkaido University

Principal Investigator

忠永 清治  北海道大学, 工学(系)研究科(研究院), 教授 (90244657)

Co-Investigator(Kenkyū-buntansha) ROSERO-NAVARRO NATALY CAROLINA  北海道大学, 工学(系)研究科(研究院), 外国人特別研究員
ROSERO-NAVARRO Nataly Carolina  北海道大学, 工学(系)研究科(研究院), 外国人特別研究員
ROSERO-NAVARRO Nataly Carolina  北海道大学, 大学院工学研究院, 外国人特別研究員
Project Period (FY) 2013-04-01 – 2016-03-31
Project Status Completed (Fiscal Year 2015)
Budget Amount *help
¥2,300,000 (Direct Cost: ¥2,300,000)
Fiscal Year 2015: ¥700,000 (Direct Cost: ¥700,000)
Fiscal Year 2014: ¥1,100,000 (Direct Cost: ¥1,100,000)
Fiscal Year 2013: ¥500,000 (Direct Cost: ¥500,000)
Keywords固体電解質 / リチウム電池 / ゾル-ゲル法 / 低温合成 / リチウムイオン電池 / ゾルーゲル法
Outline of Annual Research Achievements

Lithium garnet-type oxides Li7-xLa3Zr2-xNbxO12 (LLZNbO, x=0-1) were prepared by a sol-gel process at low temperatures. Then, glass additives, LiO2-B2O3-SiO2 glass and BaO-B2O3-SiO2 glass, were used to stimulate the sintering of the ceramic electrolyte retaining the cubic phase stable at low temperatures.
The cubic garnet phase was formed by a heat-treatment of sol-gel derived precursor powders at 600 - 700 degree C. The presursor powders and glass additives, 53LiO2・31B2O3・12SiO2 (mol%) (LiO2-B2O3-SiO2 glass) or 35BaO・10CaO・5Al2O3・15B2O3・10SiO2 (mol%) (BaO-B2O3-SiO2 glass) were pressed into pellets and sintered at 900 degree C.
The relatative density of 86% was achieved by the sintering with glass additives at 900 degree C. In the composites sintered with the BaO-B2O3-SiO2 glass, the presence of La2Zr2O7 was detected at concentration higher of 4 wt%, while the single cubic phase was obtained for the composites sintered with the LiO2-B2O3-SiO2 glass.
The ionic conductivity of the obtained composite was 8x10^-5 S/cm at 30 degree C using 4 wt.% of LiO2-B2O3-SiO2 glass. The conductivity is 20% lower than the material reported by the solid state reaction process, but the heat treatment used is about 300 degree C lower than that required by the conventional solid state reaction process. This represents an important contribution to further application of the LLZNbO solid electlolyte to all-solid-state battery.

Research Progress Status

27年度が最終年度であるため、記入しない。

Strategy for Future Research Activity

27年度が最終年度であるため、記入しない。

Report

(3 results)
  • 2015 Annual Research Report
  • 2014 Annual Research Report
  • 2013 Annual Research Report
  • Research Products

    (9 results)

All 2016 2015 2014 Other

All Int'l Joint Research (1 results) Journal Article (1 results) (of which Peer Reviewed: 1 results,  Acknowledgement Compliant: 1 results) Presentation (7 results) (of which Int'l Joint Research: 4 results)

  • [Int'l Joint Research] Institute of Ceramics and Glass, CSIC(Spain)

    • Related Report
      2015 Annual Research Report
  • [Journal Article] Preparation of Li7La3(Zr2-x,Nb-x)O-12 (x=0-1.5) and Li3BO3/LiBO2 composites at low temperatures using a sol-gel process2016

    • Author(s)
      N. C. Rosero Navarro, T. Yamashita, A. Miura, M. Higuchi and K. Tadanaga
    • Journal Title

      Solid State Ionics

      Volume: 285 Pages: 6-12

    • DOI

      10.1016/j.ssi.2015.06.015

    • Related Report
      2015 Annual Research Report
    • Peer Reviewed / Acknowledgement Compliant
  • [Presentation] Low temperature sintering of sol-gel derived Li7-xLa3Zr2-xNbxO12 solid electrolyte by using sintering additives2016

    • Author(s)
      Nataly Carolina Rosero Navarro, Taira Yamashita, Akira Miura, Mikio Higuchi and Kiyoharu Tadanaga
    • Organizer
      13th International Conference on Ceramics Processing Science
    • Place of Presentation
      東大寺総合文化センター(奈良県・奈良市)
    • Year and Date
      2016-05-08
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Effects of glass additives for low temperature sintering of sol-gel derived Li7-xLa3Zr2-xNbxO12 solid electrolyte2016

    • Author(s)
      N.C. Rosero Navarro, T. Yamashita, A. Miura, M. Higuchi, K. Tadanaga
    • Organizer
      The 24th International Congress on Glass
    • Place of Presentation
      Shanghai(China)
    • Year and Date
      2016-04-07
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Sol-gel synthesis of Li7-xLa3Zr2-xNbxO12 solid electrolyte at low temperature. Effect of glass additives on relative density and Li-ion conductivity2015

    • Author(s)
      N. C. Rosero Navarro, T. Yamashita, A. Miura, M. Higuchi, K. Tadanaga
    • Organizer
      XVIII International Sol-Gel Conference
    • Place of Presentation
      メルパルク京都(京都府・京都市)
    • Year and Date
      2015-09-06
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Effect of glass additives on relative dnesity and Li-ion conductivity of Li7-xLa3Zr2-xNbxO12 solid electrolyte2015

    • Author(s)
      N.C. Rosero Navarro, T. Yamashita, A. Miura, M. Higuchi, K. Tadanaga
    • Organizer
      20th International Conference on Solid State Ionics
    • Place of Presentation
      Colorado(USA)
    • Year and Date
      2015-06-14
    • Related Report
      2015 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Synthesis of Li7La3(Zr2-X, NbX)O12 (X = 0 - 1) at Low Temperatures Using a Sol-Gel Process2014

    • Author(s)
      N.C. Rosero-Navarro, T. Yamashita, M. Higuchi, K. Tadanaga
    • Organizer
      226th Meeting of The Electrochemical Society
    • Place of Presentation
      メキシコ・カンクン
    • Year and Date
      2014-10-05 – 2014-10-09
    • Related Report
      2014 Annual Research Report
  • [Presentation] ゾル-ゲル法によって作製したNb置換Li7La3Zr2O12の低温焼結2014

    • Author(s)
      忠永清治、Resero Carolina、山下 平、樋口幹雄
    • Organizer
      日本セラミックス協会第27回秋季シンポジウム
    • Place of Presentation
      鹿児島大学(鹿児島県鹿児島市)
    • Year and Date
      2014-09-09 – 2014-09-11
    • Related Report
      2014 Annual Research Report
  • [Presentation] ゾルゲル法によるLi_7La_3(Zr_<2-x>Nb_x)O_<12>の低温合成2014

    • Author(s)
      山下平, Carorina Resero, 樋口幹雄, 忠永清治
    • Organizer
      電気化学会第81回大会
    • Place of Presentation
      関西大学(大阪府吹田市)
    • Related Report
      2013 Annual Research Report

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Published: 2014-01-29   Modified: 2024-03-26  

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