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Stabilization of proton carriers in rare-earth elements containing glasses; new developments of intermediate-temperature fuel cells

Research Project

Project/Area Number 17H03381
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Inorganic materials/Physical properties
Research InstitutionHokkaido University

Principal Investigator

Nishii Junji  北海道大学, 電子科学研究所, 教授 (60357697)

Co-Investigator(Kenkyū-buntansha) 藤岡 正弥  北海道大学, 電子科学研究所, 助教 (40637740)
海住 英生  北海道大学, 電子科学研究所, 准教授 (70396323)
小俣 孝久  東北大学, 多元物質科学研究所, 教授 (80267640)
Project Period (FY) 2017-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥17,940,000 (Direct Cost: ¥13,800,000、Indirect Cost: ¥4,140,000)
Fiscal Year 2019: ¥3,380,000 (Direct Cost: ¥2,600,000、Indirect Cost: ¥780,000)
Fiscal Year 2018: ¥6,240,000 (Direct Cost: ¥4,800,000、Indirect Cost: ¥1,440,000)
Fiscal Year 2017: ¥8,320,000 (Direct Cost: ¥6,400,000、Indirect Cost: ¥1,920,000)
Keywords酸化物 / ガラス / イオン / イオン伝導 / プロトン / プロトン伝導 / 結晶化 / 分相 / 燃料電池 / 希土類元素 / アルカリイオン
Outline of Final Research Achievements

The purpose of this study is the development of high proton conductive electrolyte glass for the intermediate temperature fuel cell operating between 250-500℃. Using our original alkali-proton substitution method (APS), following two research issues were conducted; (1) optimization of composition of phosphate glass containing rare-earth elements, (2) sustention of high proton conductivity for long time. A phosphate glass containing 35 mol% NaO1/2 and 5 mol% GdO3/2 exhibited the conductivity of 0.002 S/cm for 500 h at 310℃. The phase separation and subsequent crystallization were occurred after 500 h. On the other hand, the quadrupole mass spectrometry revealed that the desorption temperature of H2O molecule from the glass were located above 450℃. Therefore, the progress of proton conductivity is expected by the further composition improvement.

Academic Significance and Societal Importance of the Research Achievements

従来、電解質としてのガラスは結晶材料に比べて劣ると認識されてきたが、申請者らは独自に開発したプロトン導入法により、これを覆す成果を得ており、本研究はその基礎をなすものである。本研究の実施によって得られる プロトン伝導体は、中温域燃料電池の実現だけでなく水蒸気電解や水素分離へも応用可能であり、その効果はエネルギー関連技術全体へと波及する。本研究の成果は、エネルギーシステム構築に必要な基盤技術とそれを支える基礎科学に大きな進展をもたらし、学術上はもちろんのこと、エネルギー問題に直面する社会の未来に対しても有益な礎を築くことが期待される。

Report

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

    (23 results)

All 2020 2019 2018 2017 Other

All Int'l Joint Research (2 results) Journal Article (10 results) (of which Int'l Joint Research: 3 results,  Peer Reviewed: 10 results,  Open Access: 8 results,  Acknowledgement Compliant: 1 results) Presentation (11 results) (of which Int'l Joint Research: 4 results)

  • [Int'l Joint Research] 西安理工大学(中国)

    • Related Report
      2018 Annual Research Report
  • [Int'l Joint Research] 西安理工大学(中国)

    • Related Report
      2017 Annual Research Report
  • [Journal Article] Thermal stability and proton conductivity of densely proton injected phosphate glasses containing rare-earth elements2020

    • Author(s)
      Atsushi Miyazaki, Takuya Kinoshita, Takashi Tatebayashi, Tong Fang, Yang Ren, Tomohiro Ishiyama, Takuya Yamaguchi, Takahisa Omata, Masaya Fujioka, Kaiju Hideo, Gaoyang Zhao and Junji Nishii
    • Journal Title

      Journal of Non-Crystalline Solids

      Volume: 541 Pages: 120064-120064

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] Proton transport properties of proton-conducting phosphate glasses at their glass transition temperatures2019

    • Author(s)
      T. Omata, T. Yamaguchi, S. Tsukuda, T. Ishiyama, J. Nishii, T. Yamashita and H. Kawazoe
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 21 Issue: 20 Pages: 10744-10749

    • DOI

      10.1039/c9cp01502g

    • Related Report
      2019 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Surface relief hologram formed by selective SiO2 deposition on soda-lime silicate glass2019

    • Author(s)
      D. Sakai, K. Harada, H. Shibata, K. Kawaguchi, and J. Nishii
    • Journal Title

      PLOS ONE

      Volume: 14 Issue: 1 Pages: e0210340-e0210340

    • DOI

      10.1371/journal.pone.0210340

    • Related Report
      2019 Annual Research Report 2018 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Proton-conducting phosphate glass and its melt exhibiting high electrical conductivity at intermediate temperatures2018

    • Author(s)
      T. Yamaguchi,S. Tsukuda,T. Ishiyama,J. Nishii,T. Yamashita,H. Kawazoe,T. Omata
    • Journal Title

      Journal of Materials Chemistry A

      Volume: 6 Issue: 46 Pages: 23628-23637

    • DOI

      10.1039/c8ta08162j

    • Related Report
      2018 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Dense proton injection into phosphate glasses using corona discharge treatment2018

    • Author(s)
      T. Kinoshita, A. Miyazaki, K. Kawaguchi, D. Sakai, T. Yamaguchi, T. Omata, T. Ishiyama, M. Fujioka, H. Kaiju, J. Nishii
    • Journal Title

      Applied Surface Science

      Volume: 428 Pages: 718-722

    • DOI

      10.1016/j.apsusc.2017.09.186

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Mobility of Proton Carriers in Phosphate Glasses Depends on Polymerization of Phosphate Framework2017

    • Author(s)
      T. Yamaguchi, T. Kataoka, S.Tsukuda, T. Ishiyama, J. Nishii, T. Yamashita, H. Kawazoe, T. Omata
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 19 Issue: 43 Pages: 29669-29675

    • DOI

      10.1039/c7cp05241c

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Formation of Amorphous H3Zr2Si2PO12 by Electrochemical Substitution of Sodium Ions in Na3Zr2Si2PO12 with Protons2017

    • Author(s)
      S. Tsukuda, K. Miyake, T. Yamaguchi, M. Kita, T. Ishiyama, J. Nishii, T. Yamashita, H. Kawazoe, T. Omata
    • Journal Title

      Inorganic Chemistry

      Volume: 56 Issue: 22 Pages: 13949-13954

    • DOI

      10.1021/acs.inorgchem.7b02060

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Effect of F/Ba ratio of precursor solution on the properties of solution-processed YBCO superconducting films2017

    • Author(s)
      W. Bian, Y. Chen, W. Huang, G. Zhao, J. Nishii, H. Kaiju, M. Fujioka, L. Li, N. Li, F. Yan
    • Journal Title

      Ceramics International

      Volume: 43 Issue: 11 Pages: 8433-8439

    • DOI

      10.1016/j.ceramint.2017.03.193

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Effect of alkaline-earth species in phosphate glasses on mobility of proton carriers2017

    • Author(s)
      T. Yamaguchi, Y. Saito, Y. Kuwahara, H. Yamashita, T. Ishiyama, J. Nishii, T. Yamashita, H. Kawazoe, T. Omata
    • Journal Title

      Journal of Materials Chemistry A

      Volume: 5 Issue: 24 Pages: 12385-12392

    • DOI

      10.1039/c7ta01475a

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Nano-imprinting of surface relief gratings on soda-aluminosilicate and soda-lime silicate glasses2017

    • Author(s)
      N. Kubo, N. Ikutame, M. Takei, B. Weibai, S. Ikeda, K. Yamamoto, K. Uraji, T. Misawa, M. Fujioka, H. Kaiju, G. Zhao, J. Nishii
    • Journal Title

      Optical Materials Express

      Volume: 7 Issue: 5 Pages: 1438-1445

    • DOI

      10.1364/ome.7.001438

    • Related Report
      2017 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research / Acknowledgement Compliant
  • [Presentation] Thermal Stability of Proton Conductive Phosphate Glasses2019

    • Author(s)
      Tong Fang, Yang Ren, Melbert Jeem, 藤岡正弥, 小野円佳, 西井準治
    • Organizer
      The 13th Pacific Rim Conference of Ceramic Societies(PACRIM13)
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 希土類元素を含有するプロトン伝導リン酸塩ガラスの熱的安定性2019

    • Author(s)
      Tong Fang, Yang Ren, Melbert Jeem, 藤岡正弥, 小野円佳, 西井準治
    • Organizer
      令和元年度 日本セラミックス協会 東北北海道支部研究発表会
    • Related Report
      2019 Annual Research Report
  • [Presentation] Effect of GeO2 additive on the properties of phosphate proton conductors prepared by alkali-proton substitution approach2019

    • Author(s)
      Yang Ren, Masaya Fujioka, Melbert Jeem, Takuya Kinoshita, Tong Fang, Yasuhito Tanabe,Gaoyang Zhao, Junji Nishii
    • Organizer
      The 20th RIES-HOKUDAI International Symposium
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 希土類含有リン酸塩ガラスのプロトン伝導性と熱的安定性2019

    • Author(s)
      舘林 尭、Fang Tong、Fang Xinxiong、藤岡 正弥、海住 英生、Zhao Gaoyang、西井 準治
    • Organizer
      日本セラミックス協会2019年年会
    • Related Report
      2018 Annual Research Report
  • [Presentation] 希土類及びアルカリ土類含有リン酸塩ガラスのプロトン伝導度の長時間維持2019

    • Author(s)
      舘林 尭、Fang Xinxiong、藤岡 正弥、海住 英生、Zhao Gaoyang、西井 準治
    • Organizer
      化学系学協会北海道支部2019年冬季研究発表会
    • Related Report
      2018 Annual Research Report
  • [Presentation] Thermal stability of high-proton-conductive phosphate glasses containing rare earth elements2018

    • Author(s)
      T. Tatebayashi, X. Fang, M. Fujioka, H. Kaiju, G. Zhao, J. Nishii
    • Organizer
      The 19th RIES-HOKUDAI International Symposium
    • Related Report
      2018 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Nb添加リン酸塩ガラスにおける高プロトン伝導性の長時間維持2018

    • Author(s)
      舘林 尭、Fang Xinxiong、藤岡 正弥、海住 英生、Zhao Gaoyang、西井 準治
    • Organizer
      平成30年度日本セラミックス協会東北北海道支部研究発表会
    • Related Report
      2018 Annual Research Report
  • [Presentation] リン酸塩ガラスにおけるプロトン伝導特性と含有プロトン濃度の相関2018

    • Author(s)
      舘林 尭, Fang Xinxiong, Bian Weibai, 藤岡 正弥, 海住 英生, Zhao Gaoyang, 西井 準治
    • Organizer
      化学系学協会北海道支部2018年冬季研究発表会
    • Related Report
      2017 Annual Research Report
  • [Presentation] Effect of alkaline-earth and rare-earth ions on proton conductivity of phosphate2017

    • Author(s)
      T. Tatebayashi, T. Yamaguchi, M. Fujioka, H. Kaiju, T. Omata, J. Nishii
    • Organizer
      The 18th RIES-HOKUDAI International Symposium
    • Related Report
      2017 Annual Research Report
    • Int'l Joint Research
  • [Presentation] リン酸塩ガラスのプロトン伝導におけるアルカリ土類及び希土類イオンの影響2017

    • Author(s)
      舘林 尭, Bian Weibai, 山口 拓哉, 藤岡 正弥, 海住 英生, 小俣 孝久, 西井 準治
    • Organizer
      第49回日本セラミックス協会ガラス部会夏季若手セミナー
    • Related Report
      2017 Annual Research Report
  • [Presentation] リン酸塩ガラスのプロトン伝導におけるアルカリ土類及び希土類イオンの影響2017

    • Author(s)
      舘林 尭, Bian Weibai, 藤岡 正弥, 海住 英生, 西井 準治, 山口 拓哉, 小俣 孝久
    • Organizer
      日本化学会北海道支部2017年夏季研究発表会
    • Related Report
      2017 Annual Research Report

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Published: 2017-04-28   Modified: 2023-03-16  

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