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Material design and mechanistic study of carbon electro-catalysts for fuel cells

Research Project

Project/Area Number 20H00316
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section一般
Review Section Medium-sized Section 27:Chemical engineering and related fields
Research InstitutionKyushu University (2021-2022)
University of Tsukuba (2020)

Principal Investigator

Nakamura Junji  九州大学, カーボンニュートラル・エネルギー国際研究所, 教授 (40227905)

Co-Investigator(Kenkyū-buntansha) 有賀 克彦  国立研究開発法人物質・材料研究機構, 国際ナノアーキテクトニクス研究拠点, MANA主任研究者 (50193082)
岡田 晋  筑波大学, 数理物質系, 教授 (70302388)
近藤 寛  慶應義塾大学, 理工学部(矢上), 教授 (80302800)
神原 貴樹  筑波大学, 数理物質系, 教授 (90204809)
武安 光太郎  筑波大学, 数理物質系, 助教 (90739327)
Project Period (FY) 2020-04-01 – 2023-03-31
Project Status Completed (Fiscal Year 2022)
Budget Amount *help
¥44,980,000 (Direct Cost: ¥34,600,000、Indirect Cost: ¥10,380,000)
Fiscal Year 2022: ¥14,300,000 (Direct Cost: ¥11,000,000、Indirect Cost: ¥3,300,000)
Fiscal Year 2021: ¥15,210,000 (Direct Cost: ¥11,700,000、Indirect Cost: ¥3,510,000)
Fiscal Year 2020: ¥15,470,000 (Direct Cost: ¥11,900,000、Indirect Cost: ¥3,570,000)
Keywords燃料電池 / 窒素ドープカーボン触媒 / 酸素還元反応 / ピリジン型窒素 / カーボン触媒 / 酸素還元
Outline of Research at the Start

燃料電池の非白金触媒として窒素ドープカーボン触媒に注目が集まっている。その触媒活性はアルカリ電解質中において白金に近い値を示すが、酸性電解質中では活性が大きく低下する。その活性劣化の克服およびその原因解明が最大の課題である。本研究では、触媒作用の全容解明する基礎研究と高度な触媒作製技術の開拓を連動したプロジェクトを実施する。

Outline of Final Research Achievements

Carbon catalysts are promising as non-platinum cathode catalysts for fuel cells, but the biggest problem is the decrease in activity in acid electrolytes. In this study, we clarified that the origin of the decrease in activity lies in the following equation.
pyri-NH+ + O2 + e- →pyri-NH +O2,a
Here, pyri-NH+ means pyridinium ion, and the new point is that the reduction of pyri-NH+ and oxygen adsorption (thermal reaction) are coupled. Since the redox potential of this reaction is lowered by hydration of pyri-NH+, we prepared nitrogen-doped graphene catalysts with a caged structure to keep the active site hydrophobic. Furthermore, by introducing proton-conducting microparticles into the caged structure, we achieved high activity of the catalyst.

Academic Significance and Societal Importance of the Research Achievements

地球温暖化の危機に瀕してカーボンニュートラル社会構築が必須であるが、そのなかで燃料電池が大きな役割を担う。安価で耐久性の高い触媒材料の開発が必要であるが、そのなかでカーボン触媒が最も期待されており世界中で活発に研究されている。本研究では、これまで不明であった窒素ドープカーボン触媒の機能を詳細に解明し、その知見に基づいて世界トップクラスの触媒を設計した。この成果は、燃料電池の普及に大きく貢献するものと期待される。さらに、ピリジン型窒素のプロトン化およびその還元過程による電子励起は、エネルギー捕捉・貯蔵の機能として、光合成を含む生体系エネルギーシステムに類似しており、今後の学術的発展に貢献する。

Report

(5 results)
  • 2022 Annual Research Report   Final Research Report ( PDF )
  • 2021 Annual Research Report
  • 2020 Comments on the Screening Results   Annual Research Report
  • Research Products

    (44 results)

All 2023 2022 2021 2020 Other

All Journal Article (7 results) (of which Int'l Joint Research: 6 results,  Peer Reviewed: 7 results,  Open Access: 5 results) Presentation (35 results) (of which Int'l Joint Research: 7 results,  Invited: 10 results) Remarks (1 results) Patent(Industrial Property Rights) (1 results)

  • [Journal Article] Nanoporous Hollow Carbon Spheres Derived from Fullerene Assembly as Electrode Materials for High-Performance Supercapacitors2023

    • Author(s)
      Lok Kumar Shrestha, Zexuan Wei, Gokulnath Subramaniam, Rekha Goswami Shrestha, Ravi Singh, Marappan Sathish, Renzhi Ma, Jonathan P. Hill, Junji Nakamura and Katsuhiko Ariga
    • Journal Title

      Nanomaterials

      Volume: 13 Issue: 5 Pages: 946-946

    • DOI

      10.3390/nano13050946

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] A newly designed compact CEY-XAFS cell in the soft X-ray region and its application to surface XAFS measurements under ambient-pressure conditions without photoinduced side effects2022

    • Author(s)
      Hiroshi Shimizu, Ryo Toyoshima, Kazuhisa Isegawa, Kazuhiko Mase, Junji Nakamura and Hiroshi Kondoh
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 24 Issue: 5 Pages: 2988-2996

    • DOI

      10.1039/d1cp04823f

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access
  • [Journal Article] Versatile nanoarchitectonics of Pt with morphology control of oxygen reduction reaction catalysts2022

    • Author(s)
      Guoping Chen, Santosh K. Singh, Kotaro Takeyasu, Jonathan P. Hill, Junji Nakamura and Katsuhiko Ariga
    • Journal Title

      Science and Technology of Advanced Materials

      Volume: 23 Issue: 1 Pages: 413-423

    • DOI

      10.1080/14686996.2022.2088040

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Hollow Spherical Fullerene Obtained by Kinetically Controlled Liquid-Liquid Interfacial Precipitation2022

    • Author(s)
      Guoping Chen, Flavien Sciortino, Kotaro Takeyasu, Junji Nakamura, Jonathan P. Hill, Lok Kumar Shrestha, and Katsuhiko Ariga
    • Journal Title

      Chemistry Asian Journal

      Volume: 17 Issue: 20

    • DOI

      10.1002/asia.202200756

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Activating Nitrogen-doped Graphene Oxygen Reduction Electrocatalysts in Acidic Electrolytes using Hydrophobic Cavities and Proton-conductive Particles2022

    • Author(s)
      Santosh K. Singh, Kotaro Takeyasu, Kaito Homma, Shigeharu Ito, Takashi Morinaga, Yuto Endo, Moeko Furukawa, Toshiyuki Mori, Hirohito Ogasawara and Junji Nakamura
    • Journal Title

      Angewandte Chemie. Int. Ed.

      Volume: 61 Issue: 51

    • DOI

      10.1002/anie.202212506

    • Related Report
      2022 Annual Research Report
    • Peer Reviewed / Open Access / Int'l Joint Research
  • [Journal Article] Role of Pyridinic Nitrogen in the Mechanism of the Oxygen Reduction Reaction on Carbon Electrocatalysts2021

    • Author(s)
      Takeyasu Kotaro、Furukawa Moeko、Shimoyama Yuto、Singh Santosh K.、Nakamura Junji
    • Journal Title

      Angewandte Chemie International Edition

      Volume: 60 Issue: 10 Pages: 5121-5124

    • DOI

      10.1002/anie.202014323

    • Related Report
      2021 Annual Research Report 2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Journal Article] CoOx electro-catalysts anchored on nitrogen-doped carbon nanotubes for the oxygen evolution reaction2021

    • Author(s)
      Singh Santosh K.、Takeyasu Kotaro、Paul Bappi、Sharma Sachin K.、Nakamura Junji
    • Journal Title

      Sustainable Energy & Fuels

      Volume: 5 Issue: 3 Pages: 820-827

    • DOI

      10.1039/d0se01285h

    • Related Report
      2020 Annual Research Report
    • Peer Reviewed / Int'l Joint Research
  • [Presentation] 窒素ドープカーボンのユニークな触媒機能2022

    • Author(s)
      中村潤児
    • Organizer
      第130回触媒討論会
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Mechanism of Heterogeneous Catalysis Clarified by Surface Science Technique2022

    • Author(s)
      中村潤児
    • Organizer
      日本化学会秋季事業 第12回CSJ化学フェスタ2022
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] Mechanism of Heterogeneous Catalysis Clarified by Surface Science Technique2022

    • Author(s)
      中村潤児
    • Organizer
      三井化学触媒科学フォーラム
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Catalysts for Energy and Environmental2022

    • Author(s)
      Junji Nakamura
    • Organizer
      The Second International Conference on Natural Resources for Sustainable Development
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 表面科学と触媒化学の融合の研究例2022

    • Author(s)
      中村潤児
    • Organizer
      触媒道場(触媒学会)
    • Related Report
      2022 Annual Research Report
    • Invited
  • [Presentation] 酸電解液中での窒素ドープカーボン酸素還元触媒の活性低下メカニズム2022

    • Author(s)
      林田健志、清水玲、引田悠介、中村潤児、武安光太郎
    • Organizer
      第130回触媒討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 窒素ドープグラフェン酸素還元反応触媒の疎水性効果とプロトン伝導2022

    • Author(s)
      本間海斗、藤田翔子、遠藤悠人、Singh Santosh、武安光太郎、伊藤滋啓、森永隆志、中村潤児
    • Organizer
      第130回触媒討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 窒素ドープカーボンモデル触媒の酸素還元反応におけるpH及び温度依存性2022

    • Author(s)
      清水玲、林田健志、中村潤児、武安光太郎
    • Organizer
      第130回触媒討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 疎水性窒素ドープグラフェン触媒のかご状構造の制御2022

    • Author(s)
      藤田翔子、本間海斗、遠藤悠人、Singh Santosh、武安光太郎、伊藤滋啓、森永隆志、中村潤児
    • Organizer
      第130回触媒討論会
    • Related Report
      2022 Annual Research Report
  • [Presentation] ミトコンドリア呼吸鎖における熱産生の物理化学的メカニズム(Physicochemical mechanism of heat generation in mitochondrial respiratory chain)2022

    • Author(s)
      武安光太郎、 Namari Nuning、中村潤児
    • Organizer
      第60回日本生物物理学会年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] Overpotential Estimation in Enzymatic Reactions of Mitochondrial Respiratory Chains2022

    • Author(s)
      Nuning Anugrah Putri Namari, Kotaro Takeyasu, Junji Nakamura
    • Organizer
      第60回日本生物物理学会年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 窒素ドープカーボン触媒の酸素還元活性とpH依存性2022

    • Author(s)
      林田健志、清水玲、中村潤児、武安光太郎
    • Organizer
      第49回炭素材料学会年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 酸素還元反応に対する窒素ドープグラフェン触媒の疎水性効果とプロトン伝導の両立による活性向上2022

    • Author(s)
      本間海斗、藤田翔子、遠藤悠人、Singh Santosh、武安光太郎、伊藤滋啓、森永隆志、中村潤児
    • Organizer
      第49回炭素材料学会年会
    • Related Report
      2022 Annual Research Report
  • [Presentation] 窒素ドープカーボン触媒のpHによる活性決定過程の変化2022

    • Author(s)
      林田健志、清水玲、中村潤児、武安光太郎
    • Organizer
      表面・界面スペクトロスコピー2022
    • Related Report
      2022 Annual Research Report
  • [Presentation] 疎水性効果とプロトン伝導の両立による窒素ドープグラフェン酸素還元反応触媒の活性向上2022

    • Author(s)
      本間海斗、Singh Santosh、藤田翔子、伊藤滋啓、森永隆志、武安光太郎、中村潤児
    • Organizer
      表面・界面スペクトロスコピー2022
    • Related Report
      2022 Annual Research Report
  • [Presentation] 電極触媒反応解析用 in-situ CARS装置の開発2022

    • Author(s)
      齋藤詳太、林田健志、中村潤児、武安光太郎
    • Organizer
      表面・界面スペクトロスコピー2022
    • Related Report
      2022 Annual Research Report
  • [Presentation] Deactivation mechanism of N-doped carbon catalyst in acidic media2022

    • Author(s)
      Kenji Hayashida, Rei Shimizu, Yusuke Hikita, Kotaro Takeyasu, Junji Nakamura
    • Organizer
      The 22nd International Vacuum Congress (IVC-22)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Design of N-doped carbon for ORR catalysts with hydrophobicity and proton conductivity2022

    • Author(s)
      Kaito Homma, Shoko Fujita, Santosh Singh, Kotaro Takeyasu, Junji Nakamura
    • Organizer
      The 22nd International Vacuum Congress (IVC-22)
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Deactivation Mechanism of Pyridinic Nitrogen-Doped Carbon for ORR in Acidic Media2022

    • Author(s)
      Kenji Hayashida, Rei Shimizu, Yusuke Hikita, Kotaro Takeyasu, Junji Nakamura
    • Organizer
      The 242nd ECS Meeting
    • Related Report
      2022 Annual Research Report
    • Int'l Joint Research
  • [Presentation] Mechanism of oxygen reduction reaction on nitrogen-doped carabon catalysts2022

    • Author(s)
      Junji Nakamura
    • Organizer
      ACS Spring 2022
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] 窒素ドープカーボン酸素還元触媒の酸電解液中での活性低下メカニズム2022

    • Author(s)
      林田健志、引田悠介、Santosh K Singh、武安光太郎、中村潤児
    • Organizer
      電気化学会第89回大会
    • Related Report
      2021 Annual Research Report
  • [Presentation] Mechanism of oxygen reduction reaction on N-doped carbon catalysts2021

    • Author(s)
      Junji Nakamura
    • Organizer
      ACS Fall 2021
    • Related Report
      2021 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] カーボン電極触媒上の酸素還元反応におけるピリジン型窒素の機能2021

    • Author(s)
      武安光太郎
    • Organizer
      第128回触媒討論会(特別企画:研究会横断若手シンポジウム)
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] Role of pyridinic nitrogen as an active site of carbon catalysts2021

    • Author(s)
      Kotaro Takeyasu
    • Organizer
      物理学会 2021年秋季大会 企画シンポジウム
    • Related Report
      2021 Annual Research Report
    • Invited
  • [Presentation] 窒素ドープカーボン触媒のORRに対するpH依存性と反応機構2021

    • Author(s)
      林田健志、引田悠介、武安光太郎、Singh Santosh、近藤剛弘、中村潤児
    • Organizer
      第128回触媒討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 酸化還元反応に対する窒素ドープグラフェン触媒の疎水性効果2021

    • Author(s)
      遠藤悠人、久保一史、SINGH Santosh Kumar、武安光太郎、中村潤児
    • Organizer
      第128回触媒討論会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 窒素ドープグラフェン触媒の酸素還元反応に対する疎水性効果2021

    • Author(s)
      本間海斗、遠藤悠人、Santosh Singh、武安光太郎、中村潤児
    • Organizer
      2021年日本表面真空学会学術講演会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 窒素ドープカーボン触媒のpHに対する反応メカニズムの変化2021

    • Author(s)
      林田健志、引田悠介、武安光太郎、近藤剛弘、中村潤児
    • Organizer
      2021年日本表面真空学会学術講演会
    • Related Report
      2021 Annual Research Report
  • [Presentation] 酸・塩基電解液中での窒素ドープカーボン触媒の反応機構の解明2021

    • Author(s)
      林田健志、引田悠介、武安光太郎、中村潤児
    • Organizer
      表面界面スペクトロスコピー2021
    • Related Report
      2021 Annual Research Report
  • [Presentation] 窒素ドープグラフェン触媒の疎水性効果による酸素還元反応活性の向上2021

    • Author(s)
      本間海斗、遠藤悠人、Santosh Singh、武安光太郎、中村潤児
    • Organizer
      表面界面スペクトロスコピー2021
    • Related Report
      2021 Annual Research Report
  • [Presentation] 酸・塩基電解質溶液中での窒素ドープカーボンの挙動2021

    • Author(s)
      林田健志、引田悠介、武安光太郎、近藤剛弘、中村潤児
    • Organizer
      日本化学会第101春季年会(2021)
    • Related Report
      2020 Annual Research Report
  • [Presentation] 燃料電池用窒素ドープカーボン触媒の活性点 (Active site of nitrogen-doped carbon catalysts for fuel cell)2020

    • Author(s)
      中村潤児
    • Organizer
      第59回 フラーレン・ナノチューブ・グラフェン総合シンポジウム
    • Related Report
      2020 Annual Research Report
    • Invited
  • [Presentation] ピリジン型窒素ドープカーボンモデル触媒における酸素還元反応素過程2020

    • Author(s)
      引田悠介、秋光上歩、渋谷陸、武安光太郎、近藤剛弘、中村潤児
    • Organizer
      第126回触媒討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 窒素ドープグラフェン触媒における酸化還元反応での疎水性の効果2020

    • Author(s)
      遠藤悠人、SINGH, Santosh、武安光太郎、中村潤児
    • Organizer
      第126回触媒討論会
    • Related Report
      2020 Annual Research Report
  • [Presentation] 籠状窒素ドープグラフェン触媒の高活性化メカニズム2020

    • Author(s)
      久保一史、SINGH, Santosh、武安光太郎、中村潤児
    • Organizer
      第126回触媒討論会
    • Related Report
      2020 Annual Research Report
  • [Remarks] 筑波大学数理物質系 触媒表面科学研究グループ

    • URL

      https://www.ims.tsukuba.ac.jp/~nakamura_lab/

    • Related Report
      2021 Annual Research Report 2020 Annual Research Report
  • [Patent(Industrial Property Rights)] 酸素還元触媒およびその製造方法2022

    • Inventor(s)
      中村潤児,サントーシュ クマル シン,武安光太郎,本間海斗 他
    • Industrial Property Rights Holder
      中村潤児,サントーシュ クマル シン,武安光太郎,本間海斗 他
    • Industrial Property Rights Type
      特許
    • Filing Date
      2022
    • Related Report
      2022 Annual Research Report

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Published: 2020-04-28   Modified: 2024-01-30  

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