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synthesis and cyrstal structure of a new proton solid electrolyte that operates in a wide temperature range

Research Project

Project/Area Number 21K05246
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Review Section Basic Section 36020:Energy-related chemistry
Research InstitutionChiba Institute of Technology (2022-2023)
Osaka Institute of Technology (2021)

Principal Investigator

Matsuda Yasuaki  千葉工業大学, 工学部, 准教授 (10731101)

Project Period (FY) 2021-04-01 – 2024-03-31
Project Status Completed (Fiscal Year 2023)
Budget Amount *help
¥4,030,000 (Direct Cost: ¥3,100,000、Indirect Cost: ¥930,000)
Fiscal Year 2023: ¥650,000 (Direct Cost: ¥500,000、Indirect Cost: ¥150,000)
Fiscal Year 2022: ¥910,000 (Direct Cost: ¥700,000、Indirect Cost: ¥210,000)
Fiscal Year 2021: ¥2,470,000 (Direct Cost: ¥1,900,000、Indirect Cost: ¥570,000)
Keywordsプロトン導電体 / 中温作動 / 機能性セラミックス / リン酸塩 / 固体電解質 / 結晶構造 / 燃料電池 / 新規物質 / 中性子
Outline of Research at the Start

次世代エネルギーインフラの基幹技術として切望されている150-200℃付近を作動温度とする燃料電池の実現は、中低温の広域温度帯で作動するプロトン固体電解質の開発にかかっている。本研究は、室温から500℃の温度域で高プロトン導電率を発現するトンネル型リン酸塩KNi1-xH2x(PO3)3・yH2Oを合成し、この物質優れた熱安定性とプロトン導電性の発現に関する結晶学的知見を得る。①骨格構成カチオンのサイズと相転移温度との相関、②プロトン量と結晶水の最適比率とプロトン導電率の最高値③プロトンの情報まで結晶構造を決定し、イオン拡散経路のエネルギー障壁を見積もり、プロトン拡散の律速過程を明らかにする。

Outline of Final Research Achievements

This study aimed to develop mixed-cation phosphates exhibiting high proton conductivity in the temperature range from room temperature to 500°C, and to extract crystalline insights into their thermal stability and proton conductivity. As a result of systematic investigation of phosphates with substituted cations of different sizes, we discovered tunnel-type phosphate, KNi1-xH2x(PO3)3yH2O, exhibiting proton conductivity reaching 10-2 Scm-1 from room temperature to 500°C, along with other novel proton-conductive crystalline phases. The thermal stability of these phosphates was found to depend on the constituent cations, and the arrangement of PO4 tetrahedra serves as templates for crystalline water chains, which are pathways for fast proton diffusion.

Academic Significance and Societal Importance of the Research Achievements

次世代エネルギーインフラとして切望されている150-300°Cで作動温度する燃料電池の実現は、中温域でプロトン導電体の熱安定性と高プロトン導電率を両立するプロトン固体電解質の開発にかかっているが、これは未だ困難な課題である。本研究では、200度付近で高プロトン導電率を発現するリン酸塩に着目し、その結晶構造を、骨格、プロトン拡散経路と分けて物質設計、開発することで、室温から500度で作動する新規プロトン導電体群を開発するとともに、その熱安定性とプロトン導電特性の発現要因を結晶学的視点から提示した。これにより、次世代エネルギーデバイスおよびその構成材料開発の加速化が期待される。

Report

(4 results)
  • 2023 Annual Research Report   Final Research Report ( PDF )
  • 2022 Research-status Report
  • 2021 Research-status Report
  • Research Products

    (16 results)

All 2024 2023 2022 2021

All Journal Article (4 results) (of which Peer Reviewed: 4 results,  Open Access: 1 results) Presentation (12 results) (of which Int'l Joint Research: 5 results,  Invited: 1 results)

  • [Journal Article] A tunnel-structured phosphate exhibiting high proton conductivity and thermal stability over a wide intermediate temperature range2024

    • Author(s)
      Yasuaki Matsuda, Jun Nakajima, Yuta Inoue, Akihisa Ishikawa, Naoya Ueta, Daisuke Mori, Sou Taminato, Nobuyuki Imanishi, Takashi Fukushima and Shinya Higashimoto
    • Journal Title

      Inorganic chemistry

      Volume: -

    • Related Report
      2023 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Synthesis and Proton Conductivity of the Mixed Cation Phosphate, KCo<sub>1−<i>x</i></sub>H<sub>2<i>x</i></sub>(PO<sub>3</sub>)<sub>3</sub> • <i>y</i>H<sub>2</sub>O with a with a One-dimensional Tunnel Structure2022

    • Author(s)
      Jun Nakajima, Naoya Ueda, Sou Taminato, Daisuke Mori, Nobuyuki Imanishi, Shinya Ueda, Yasuaki Matsuda
    • Journal Title

      Journal of the Japan Society of Powder and Powder Metallurgy

      Volume: 69 Issue: 3 Pages: 99-103

    • DOI

      10.2497/jjspm.69.99

    • ISSN
      0532-8799, 1880-9014
    • Year and Date
      2022-03-15
    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Journal Article] High proton conductivity of NaMg1-xLixHx (PO3)3yH2O with a three-dimensional open framework in the intermediate temperature range2021

    • Author(s)
      Naoya Ueda, Jun Nakajima, Daisuke Mori, Sou Taminato, Nobuyuki Imanishi, Shinya Higashimoto and Yasuaki Matsuda
    • Journal Title

      Materials Advances

      Volume: 2 Issue: 20 Pages: 6603-6612

    • DOI

      10.1039/d1ma00592h

    • Related Report
      2021 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Proton conductivity in mixed cation phosphate, KMg1-xH2x(PO3)yH2O, with a layered structure at low-intermediate temperatures2021

    • Author(s)
      Yasuaki Matsuda, Naoya Ueda, Kousei Funakoshi, Jun Nakajima, Daisuke Mori, Sou Taminato and Shinya Higashimoto
    • Journal Title

      Dalton Transactions

      Volume: 50 Issue: 22 Pages: 7678-7685

    • DOI

      10.1039/d1dt01187a

    • Related Report
      2021 Research-status Report
    • Peer Reviewed
  • [Presentation] 複合カチオンリン酸塩の合成、結晶構造、プロトン導電特性2024

    • Author(s)
      松田 泰明,廣瀬和彦,黄 優香,石川 晃久,大塚 啓太
    • Organizer
      第6回固体化学フォーラム研究会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Synthesis, crystal structure and proton conductivity of the Benitoite-type phosphate, KMg1-xLixHx(PO3)3・yH2O2024

    • Author(s)
      Kazuhiko Hirose, Yuuka Kou, Yasuyuki Matsuda
    • Organizer
      日本化学会第104春季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Benitoite型リン酸塩KCa1-xH2x(PO3)3yH2Oの合成とプロトン導電特性2024

    • Author(s)
      黄 友香・廣瀬 和彦・松田 泰明
    • Organizer
      日本化学会第104春季大会
    • Related Report
      2023 Annual Research Report
  • [Presentation] Synthesis and proton conductivity of Benitoite-type Mixed-cation phosphate2023

    • Author(s)
      Kazuhiko Hirose, Yasuaki Matsuda
    • Organizer
      JSPMIC2023
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Crystal structure and thermal stability of proton conducting phosphate, KNi1-xH2x(PO3)3・yH2O2023

    • Author(s)
      Yasuaki Matsuda, Jun Nakajima, Shinya Higashimoto and Daisuke Mori
    • Organizer
      SSPC21
    • Related Report
      2023 Annual Research Report
    • Int'l Joint Research
  • [Presentation] ポリアニオンエンジニアリングによる中温作動型プロトン導電体の創成2023

    • Author(s)
      松田 泰明
    • Organizer
      第54回中部化学関係学協会支部連合秋季大会
    • Related Report
      2023 Annual Research Report
    • Invited
  • [Presentation] トンネル型構造をもつプロトン導電性リン酸塩の合成、熱安定性と電気化学特性2023

    • Author(s)
      松田 泰明 、中島 潤 、上田 直哉 、東本 慎也 、森 大輔
    • Organizer
      第61回セラミックス基礎科学討論会
    • Related Report
      2022 Research-status Report
  • [Presentation] Relationship between the crystal structure and constituent elements of mixed cation phosphates2022

    • Author(s)
      Yasuaki Matuda, Rihito Nakamura, Souichiro Kondo, Tomoya Yoshimura, Naoya Ueta, Jun Nakajima, Daisuke Mori, Shinya Higshimoto
    • Organizer
      17th Asian conference on solid state ionics
    • Related Report
      2022 Research-status Report
    • Int'l Joint Research
  • [Presentation] トンネル型リン酸塩の合成と中低温での高プロトン導電特性2021

    • Author(s)
      中島 潤、上田 直哉、東本 慎也、松田 泰明、森大輔
    • Organizer
      2021年度 粉体粉末冶金 春季大会
    • Related Report
      2021 Research-status Report
  • [Presentation] PO4 四面体鎖をもつ複合カチオンリン酸塩の 合成、結晶構造とプロトン導電特性2021

    • Author(s)
      松田 泰明、上田 直哉、中島 潤、森 大輔、東本 慎也
    • Organizer
      第47 回固体イオニクス討論会
    • Related Report
      2021 Research-status Report
  • [Presentation] Proton conductivity in mixed cation phosphate with a layered strcuture2021

    • Author(s)
      Yasuaki Matsuda, Naoya Ueda, Jun Nakajima, Daisuke Mori, Shinya Higashimoto
    • Organizer
      Solid State Proton Conductors (SSPC-20)
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research
  • [Presentation] Synthesis, structure and proton conductivity of Mixed cation phosphate with the three-dimensional open framework2021

    • Author(s)
      Yasuaki Matsuda, Naoya Ueda, Daisuke Mori, Shinya Higashimoto
    • Organizer
      Solid State Proton Conductors (SSPC-20)
    • Related Report
      2021 Research-status Report
    • Int'l Joint Research

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Published: 2021-04-28   Modified: 2025-01-30  

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