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Preparation and Evaluation of Proton Conductive Membranes for Medium Temperature Fuel Cells

Research Project

Project/Area Number 14550669
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Inorganic materials/Physical properties
Research InstitutionToyohashi University of Technology

Principal Investigator

MATSUDA Atsunori  Toyohashi University of Technology, Department of Engineering, Associate Professor, 工学部, 助教授 (70295723)

Co-Investigator(Kenkyū-buntansha) MUTO Hiroyuki  Toyohashi University of Technology, Department of Engineering, Research Associate, 工学部, 助手 (20293756)
辰巳砂 昌弘  大阪府立大学, 大学院・工学研究科, 教授 (50137238)
TADANAGA Kiyoharu  Osaka Prefecture University, Graduate School of Engineering, Associate Professor, 大学院・工学研究科, 助教授 (90244657)
SAKAI Mototsugu  Toyohashi University of Technology, Department of Engineering, Professor, 工学部, 教授 (50124730)
Project Period (FY) 2002 – 2003
Project Status Completed (Fiscal Year 2003)
Budget Amount *help
¥3,600,000 (Direct Cost: ¥3,600,000)
Fiscal Year 2003: ¥1,000,000 (Direct Cost: ¥1,000,000)
Fiscal Year 2002: ¥2,600,000 (Direct Cost: ¥2,600,000)
KeywordsProton conductor / Inorganic-organic composite / Thermally stable polymer / Fuel cell / Medium temperature range / Phosphosilicate gel / Sol-gel method / Polyimide / 無機-有機複合体 / ホスドホシリケートゲル / ゾル-ゲル法
Research Abstract

Solid state proton-conductive membranes with high conductivity in the medium temperature range (100-200ーC) even under low humidity are highly required as the electrolytes for PEFCs. Since the operation of PEFCs in the medium temperature range improves the utilization of total electric power generated in the cells. and depresses the poisoning of Pt catalysts with CO in the fuel gases. In addition, working of PEFCs under low humidity permits to reduce the weight and volume of humidifiers. In the present work, proton conducting membranes based on sol-gel derived phosphosilicate (P_2O_5-SiO_2) gel have been fabricated for the application to medium temperature fuel cells as an electrolyte.
Two types of proton conductive membranes, which show high conductivities even at medium temperatures with low humidity, have been successfully prepared. One is a composite sheet composed of phosphosilicate gel powder and organic polymer such as heat resistant polyimide. The other is a hybrid sheet in which inorganic and organic components derived from an organosilane such as 3-Glycidoxypropyltrimethoxysilane and phosphoric acid are covalently bonded.
Fuel cells using a composite sheet composed of phosphosilicate (P_2O_5-SiO_2, P/Si=1 in mole ratio) gel powder and polyimide operated up to 150ーC under a relatively low water vapor, pressure. Maximum power density of the fuel cell increased with increasing operation temperature and was 28 mW cm^<-2> at 150 ℃ and 18 %RH. With respect to the hybrid type, fuel cells using a hybrid sheet derived from 3-Glycidoxypropyltrimethoxysilane and phosphoric, acid also continuously operated at 130 ℃.
It was found that the addition of tin and tantalum as well as aluminum improved the chemical durability of phosphosilicate gels by depressing the leaching of phosphoric acid from the gels. At the same time, the improvement of durability of the gels resulted in a decrease in the proton conductivity.

Report

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

    (36 results)

All Other

All Publications (36 results)

  • [Publications] A.Matsuda et al.: "Phosphosilicate Gels as a Solid State Proton Conductor at Elevated Temperature and Low Humidity"Journal of Ceramic Society of Japan. 110. 131-134 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Preparation of Copolymerized Phenylsilsesquioxane-Benzylsilsesquioxane Particles"Journal of Sol-Gel Science and Technology. 23. 247-252 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Sol-Gel Derived Porous Silica Gels Impregnated with Sulfuric Acid : Pore Structure and Proton Conductivities at Medium Temperatures"Journal of Electrochemical Society. 149. E292-E297 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Proton Conductivities of Sol-Gel Derived Phosphosilicate Gels in Medium Temperature Range with Low Humidity"Solid State Ionics. 154-155. 687-692 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Tadanaga et al.: "Proton Conductive Inorganic-Organic Hybrid Membranes as an Electrolyte for Fuel Cells Prepared from 3-Glycidoxylpropyltriethoxysilane and Orthophosphoric Acid"Electrochemictry. 70. 998-1000 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Tadanaga et al.: "Preparation of Proton Conductive Inorganic-Organic Hybrid Films form Glycidoxylpropyltriethoxysilane and Orthophosphoric Acid"Chemistry of Materials. 15. 1910-1912 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] C.Iwakura et al.: "All Solid State Nickel/Metal Hydride Battery with a Proton Conductive Phosphoric Acid-Doped Silica Gel Electrolyte"Electrochimica Acta. 48. 1499-1503 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Preparation and Characterization of Thermally Stable Proton-Conducting Composite Sheets Composed of Phosphosilicate Gel and Polyimide"Solid State Ionics. 162-163. 247-252 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Proton Conductivity at Medium Temperature Range and Chemical Durability of Phosphosilicate Gels Added with a Third Component"Solid State Ionics. 162-163. 253-259 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] 松田厚範, 他: "ホスホシリケートゲルおよび無機-有機ハイブリッド(解説)"工業材料. 50. 39-42 (2002)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] 忠永清治, 他: "中温作動燃料電池用プロトン伝導性無機-有機複合体電解質膜(解説)"工業材料. 51. 35-38 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] 松田厚範, 他(分担執筆): "最新燃料電池部材その最先端技術と信頼性評価"技術情報協会. 234 (2003)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Phosphosilicate Gels as a Solid State Proton Conductor at Elevated Temperature and Low Humidity"Journal of Ceramic Society of Japan. 110. 131-134 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Preparation of Copolymerized Phenylsilsesquioxane-Benzylsilsesquioxane Particles"Journal of Sol-Gel Science and Technology. 23. 247-252 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Sol-Gel Derived Porous Silica Gels Impregnated with Sulfuric Acid : Pore Structure and Proton Coductivities at Medium Temperatures"Journal of Electrochemical Society. 149. E292-E297 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Proton Conductivities of Sot-Gel Derived Phosphosilicate Gels in Medium Temperature Range with Low Humidity"Solid State Ionics. 154-155. 687-692 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Tadanaga et al.: "Proton Conductive Inorganic-Organic Hybrid Membranes as an Electrolyte for Fuel Cells Prepared from 3-Glycidoxylpropyltriethoxysilane and Orthophosphoric Acid"Electrochemictry. 70. 998-1000 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Tadanaga et al.: "Preparation of Proton Conductive Inorganic-Organic Hybrid Films from 3-Glycidoxylpropyltriethoxysilane and Orthophosphoric Acid"Chemistry of Materials. 15. 1910-1912 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] C.Iwakura et al.: "All Solid State Nickel/Metal Hydride Battery with a Proton Conductive Phosphoric Acid-Doped Silica Gel Electrolyte"Electrochimica Acta. 48. 1499-1503 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Preparation and Characterization of Thermally Stable Proton-Conducting Composite Sheets Composed of Phosphosilicate Gel and Polyimide"Solid State Ionics. 162-163. 247-252 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Proton Conductivity at Medium Temperature Range and Chemical Durability of Phosphosilicate Gels Added with a Third Component"Solid State Ionics. 162-163. 253-259 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Phosphosilicate gels and Inorganic-Organic Hybrids"Kogyo Zairyo. 50. 39-42 (2002)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] K.Tadanaga et al.: "Inorganic-Organic Membranes for Medium Temperature Fuel Cells"Kogyo Zairyo. 51. 35-38 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda et al.: "Up-To-Date Fuel Cell Components and Their Reliability"Gijutu Joho Kyokai. 41-51 (2003)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2003 Final Research Report Summary
  • [Publications] A.Matsuda, et al.: "Preparation and Characterization of Thermally Stable Proton-Conducting Composite Sheets Composed of Phosphosilicate Gel and Polyimide"Solid State Ionics. 162-163. 247-252 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] A.Matsuda, et al.: "Proton Conductivity at Medium Temp erature Range and Chemical Durability of Phosnhosilicate Added with a Third Component"Solid State Ionics. 162-163. 253-259 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Tadanaga, et al.: "Preparation of Proton Conductive Inorganic-Organic Hybrid Films from 3-Glycidoxylpropyltriethoxysilane and Orthophosphoric Acid"Chemistry of Materials. 15・[9]. 1910-1912 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] K.Tadanaga, et al.: "Inorganic-Organic Hybrid Films from 3-Glycidoxypropyltrimethoxysilane and Orthophosphoric Acid as Medium Temperature Fuel Cells"Electrochemistry Communications. 5・[8]. 644-646 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 忠永清治 他: "中温作動燃料電池用プロトン伝導性無機-有機複合体電解質膜"工業材料. 51, No.4. 35-38 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] 松田厚範 他(分担執筆): "ゾル-ゲル法により作製したプロトン伝導性無機-有機複合体電解質シート"技術情報協会. 234 (2003)

    • Related Report
      2003 Annual Research Report
  • [Publications] A.Matsuda, et al.: "Phosphosilicate Gels as a Solid State Proton Conductor at Elevated Temperature and Low Humidity"Journal of Ceramic Society of Japan. 110[2]. 131-134 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] A.Matsuda, et al.: "Sol-Gel Derived Porous Silica Gels Impregnated with Sulfuric Acid : Pore Structure and Proton Coductivities at Medium Temperatures"Journal of Electrochemical Society. 149[8]. E292-E297 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] A.Matsuda, et al.: "Proton Conductivities of Sol-Gel Derived Phosphosilicate Gels in Medium Temperature Range with Low Humidity"Solid State Ionics. 154-155[12]. 687-692 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] K.Tadanaga, et al.: "Proton Conductive Inorganic-Organic Hybrid Membranes ad an Electrolyte for Fuel Cells Prepared by from 3-Glycidoxylpropyltriethoxysilane and Orthophosphoric Acid"Electrochemictry. 70[12]. 998-1000 (2002)

    • Related Report
      2002 Annual Research Report
  • [Publications] A.Matsuda, et al.: "Preparation and Characterization of Thermally Stable Proton-Conducting Composite Sheets Composed of Phosphosilicate Gel and Polyimide"Solid State Ionics. (印刷中). (2003)

    • Related Report
      2002 Annual Research Report
  • [Publications] A.Matsuda, et al.: "Proton Conductivity at Medium Temperature Range and Chemical Durability of Phosphosilicate Gels Added with a Third Component"Solid State Ionics. (印刷中). (2003)

    • Related Report
      2002 Annual Research Report

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Published: 2002-04-01   Modified: 2016-04-21  

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