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Development of super high temperature-type proton conductor based on alpha alumina.

Research Project

Project/Area Number 13450308
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Metal making engineering
Research InstitutionNagoya Institute of Technology

Principal Investigator

FUKATSU Norihiko  Nagoya Institute of Technology, Engg, Materials Sci.and Engg., Prof., 工学研究科, 教授 (80029355)

Co-Investigator(Kenkyū-buntansha) KURITA Noriaki  Nagoya Institute of Technology, Engg, Materials Sci.& Engg., Res.Assistant, 工学研究科, 助手 (20242901)
栗田 典明  名古屋工業大学, 工学研究科, 助手 (20292401)
大橋 照男  名古屋工業大学, 工学部, 教授 (70024263)
Project Period (FY) 2001 – 2003
Project Status Completed (Fiscal Year 2003)
Budget Amount *help
¥14,800,000 (Direct Cost: ¥14,800,000)
Fiscal Year 2003: ¥2,500,000 (Direct Cost: ¥2,500,000)
Fiscal Year 2002: ¥7,900,000 (Direct Cost: ¥7,900,000)
Fiscal Year 2001: ¥4,400,000 (Direct Cost: ¥4,400,000)
Keywordsalpha-alumina / proton conduction / hydrogen solubility / solid electrolyte / hydrogen sensor / Proton conductor / hydrogen concentration cell / OH stretching vibration / プロトン電導 / スピネル
Research Abstract

Firstly, the most appropriate dopant for incorporation of hydrogen was studied using single crystal of alpha alumina. With the measurements of IR absorption of OH stretching vibration, the magnesium is found most effective dopant among Mg,Ni,Co, and Ti. In order to improve the low yield of crystal growth due to the thermal stress, the additions of Cr,Y,B,Sm,Nd,La,Ce as the second dopant were examined. However, the any explicit improvements were not obtained.
The location of the incorporated hydrogen in the crystal structure of alpha-alumina was investigated with the Mg doped samples. The polarization angle dependency of the absorption of OH stretching vibration was examined for several sets of the directions of the incident beam and crystal faces. The comparison between the measurement and the theoretically calculated results showed that hydrogen is located between one of the 0-0 bond constituting the edges of oxygen octahedron in the corundum structure with making the hydrogen bond. Am … More ong the four 0-0 bonds of different spacing, one whose spacing is 272 pm is found preferred for hydrogen location. The same tendency was observed for Ti doped alpha-alumina.
The H/D isotope effect of electrical conductivity was examined for Mg doped single crystal samples. The proton was confirmed to be the most dominant charge carrier in the low oxygen potentials region. The anisotropy was observed also in the electrical conduction. The conductivity was higher when the direction of the electric field is perpendicular to c-axis than pararell, which was reasonably explained by the preference of hydrogen location among the O-O bonds.
As the Mg was found to be the most appropriate dopant, the electrochemical properties were studied with the commercially supplied polycrystalline- alumina tube whose main impurities were magnesium. The emf of the hydrogen concentration cells using these tubes as the electrolyte were measured for various hydrogen and oxygen potential gradients. These values were analyzed theoretically based on the model of the crystal defects and the equation between the emf of the cell and the potentials difference on the electrodes was derived. The parameter appeared in the equation was determined as a function of the temperature.
The electrochemical properties of magnesium-aluminate spinel which is almost always the co-existing phase of Mg-doped polycrystalline -alumina were also studied to know the effect of second phase on the properties of the proton conduction. It was confirmed that hydrogen might be incorporated into magnesium-aluminate spinel as proton and that the it was movable. However, the conductivity due to magnesium ion was found far higher and the contribution of proton to the electrical conductivity could be ignored. Less

Report

(4 results)
  • 2003 Annual Research Report   Final Research Report Summary
  • 2002 Annual Research Report
  • 2001 Annual Research Report
  • Research Products

    (29 results)

All 2003 2002 2001 Other

All Journal Article (12 results) Publications (17 results)

  • [Journal Article] Incorporation of hydrogen into magnesium doped α-alumina.2003

    • Author(s)
      N.Fuka t su, N.kurita, Y.Oka, S.Yamamoto
    • Journal Title

      Solid State Ionics 162-163

      Pages: 147-159

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] Hydrogen concentration cell using a-alumina as a solid electrolyte.2003

    • Author(s)
      N.Kurita, N.Fukatsu, N.Miyamoto, M.Takada, M.Kato, T.Ohashi
    • Journal Title

      Solid State Ionics 162-163

      Pages: 135-145

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] Incorporation of hydrogen into magnesium doped α-alumina.2003

    • Author(s)
      N.Fukatsu, N.Kurita, Y.Oka, S.Yamamoto
    • Journal Title

      Solid State Ionics Vol.162-163

      Pages: 147-159

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] Hydrogen concentration cell using α-alumina as a solid electrolyte.2003

    • Author(s)
      N.Kurita, N.Fukatsu, N.Miyamoto, M.Takada, M.Kato, T.Ohashi
    • Journal Title

      Solid State Ionics Vol.162-163

      Pages: 135-145

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] Incorporation of hydrogen into magnesium aluminate spinel.2002

    • Author(s)
      N.Fukatsu, N.Kurita, H.Shiga, Y.Murai, T.Ohashi
    • Journal Title

      Solid State Ionics 152-153

      Pages: 809-817

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] Measurements of hydrogen permeation through fused silica and borosilicate glass by electrochemical pumping using oxide protonic conductor2002

    • Author(s)
      N.Kurita, N.Fukatsu, H.Otsuka, T.Ohashi
    • Journal Title

      Solis State Ionics 146

      Pages: 101-111

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] Analysis of defect structure of the proton conducting oxide CaZr_<0.9>In_<0.1>O_<3-d> by DC-polarization technique.2002

    • Author(s)
      N.Kurita, N.Fukatsu, T.Kawahara, T.Ohashi
    • Journal Title

      Journal of the Electrochemical Society 149

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] Incorporation of hydrogen into magnesium aluminate spinel.2002

    • Author(s)
      N.Fukatsu, N.Kurita, H.Shiga, Y.Murai, T.Ohashi
    • Journal Title

      Solid State Ionics Vol.152-153

      Pages: 809-817

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] Measurements of hydrogen permeation through fused silica and borosilicate glass by electrochemical pumping using oxide protonic conductor.2002

    • Author(s)
      N.Kurita, N.Fukatsu, H.Otsuka, T.Ohashi
    • Journal Title

      Solis State Ionics Vol.146

      Pages: 101-111

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] Analysis of defect structure of the proton conducting oxide CaZr_<0.9>In_<0.1>O_<3-d> by DC-polarization technique.2002

    • Author(s)
      N.Kurita, N.Fukatsu, T.Kawahara, T.Ohashi
    • Journal Title

      J.Electrochem.Soc. Vol.149

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] プロトン導電性酸化物とその高温化学への応用2001

    • Author(s)
      武津典彦
    • Journal Title

      溶融塩および高温化学 44

      Pages: 167-185

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Journal Article] Proton conducting oxides and their applications to high-temperature physical chemistry.2001

    • Author(s)
      N.Fukatsu
    • Journal Title

      Molten Salt Vol.44

      Pages: 167-185

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] N.Fukatsu, N.Kurita, Y.Oka, S.Yamamoto: "Incorporation of hydrogen into magnesium doped α-alumina"Solid State Ionics. 162/163. 147-159 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] N.Kurita et al.: "Hydrogen concentration cell using α-alumina as a solid electrolyte"Solid State Ionics. 162/163. 135-145 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 奥山勇治, 栗田典明, 武津典彦: "アルミナ過剰の不定比マグネシウム・アルミネートスピネルの欠陥構造"日本金属学会講演概要. 133. 481-481 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 奥山勇治, 栗田典明, 武津典彦: "アルミナ過剰の不定比マグネシウム・アルミネートスピネルの欠陥構造"固体イオニクス討論会講演要旨集. 29. 152-153 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 堀田和宏, 栗田典明, 武津典彦: "鉄基合金の表面に生じたアルミナ膜の起電力特性"日本金属学会講演概要. 132. 160-160 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 栗田典明, 堀田和宏, 武津典彦: "アルミナ表面酸化膜の電気化学的特性"日本金属学会講演概要. 134(発表予定). (2004)

    • Related Report
      2003 Annual Research Report
  • [Publications] N.Fukatsu et al.: "Incorporation of Hydrogen into Magnesium Aluminate Spinel"Solid State Ionics. 152-153C. 809-817 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] N.Kurita et al.: "Measurements of Hydrogen Permeation through Fused Silica and Borosilicate Glass by Electrochemical Pumping using Oxide Protonic Conductor"Solid State Ionics. 146巻. 101-111 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] N.Kurita et al.: "Anlysis of Defect Structure of the Proton Conducting Oxide CaZr_<0.9>In_<0.1>O_<3-δ> by DC-Polarization Technique"J.Electroche.Soc.. 149巻. D104-D111 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] N.Fukatsu et al.: "Incorporation of Hydrogen into Magnesium Doped α-alumina"Extended Abstract of 11^<th> International Conference on Solid State Protonic Conductors. PA2 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] N.Kurita et al.: "Hydrogen Concentration Cell using α-Alumina as a Solid Electrolyte"Extended Abstract of 11^<th> International Conference on Solid State Protonic Conductors. PA3 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] N.Fukatsu, N.Kurita: "Hydrogen Sensor Based on Oxide Proton Conductors and its Application to Metallurgical Engineering"Extended Abstract of 9^<th> Euro Conference on Ionics. 28-29 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] N. Fukatsu et al.: "Incorporation of Hydrogen into Magnesium Aluminate Spinel"Extended Abstract of International Conference on Solid State Ionics, SSI 2001. 200-200 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] 栗田典明 他: "プロトン導電体としてのα-アルミナ"日本金属学会講演概要(2001年秋季大会). 129巻. 256-256 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] 栗田典明 他: "α-アルミナを固体電解質とした溶融銅用水素センサーの開発"資源・素材2001(札幌) 一般発表(C)、(D) 講演資料. 195-196 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] 武津典彦: "プロトン導電性酸化物とその高温物理化学への応用"溶融塩および高温化学. 44巻3号. 167-185 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] 栗田典明 他: "α-アルミナを電解質としたガルバニ電池型水素センサーの開発"日本金属学会2002年春季大会. 130回(発表予定). (2002)

    • Related Report
      2001 Annual Research Report

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Published: 2001-04-01   Modified: 2016-04-21  

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