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Pore structure control of support-free catalyst utilizing neither platinum nor carbon and the performance enhancement of the catalyst layer for fuel cells

Research Project

Project/Area Number 17K06180
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeMulti-year Fund
Section一般
Research Field Thermal engineering
Research InstitutionHirosaki University

Principal Investigator

Chisaka Mitsuharu  弘前大学, 理工学研究科, 准教授 (20513310)

Project Period (FY) 2017-04-01 – 2020-03-31
Project Status Completed (Fiscal Year 2019)
Budget Amount *help
¥4,810,000 (Direct Cost: ¥3,700,000、Indirect Cost: ¥1,110,000)
Fiscal Year 2019: ¥780,000 (Direct Cost: ¥600,000、Indirect Cost: ¥180,000)
Fiscal Year 2018: ¥1,040,000 (Direct Cost: ¥800,000、Indirect Cost: ¥240,000)
Fiscal Year 2017: ¥2,990,000 (Direct Cost: ¥2,300,000、Indirect Cost: ¥690,000)
Keywords酸素還元 / 酸化チタン / 窒化チタン / カソード / 酸素還元反応 / 非白金 / 非貴金属 / 固体高分子形燃料電池 / 酸窒化物
Outline of Final Research Achievements

Oxide catalysts have been developed in polymer electrolyte fuel cell cathodes to replace platinum-group-metal catalysts, while both the oxygen reduction reaction activity and the surface area remained moderate. In this study, the pore structure of titanium oxide catalysts was controlled by two methods; the one is the use of silica templates and the other is codoping of phosphor and nitrogen atoms.
The latter significantly enhanced the activity and increased the surface area. A recently reported facile combustion method was modified by simply adding H3PO4 to the precursor dispersion. Pentavalent phosphor atoms were doped into both the bulk and surface to form new active sites without alternating the number of oxygen vacancy on the surface rutile TiO2, which was formed by nitrogen-doping. The catalyst loading was reduced to less than half of the previous phosphor-free catalysts while the activity was successfully enhanced by the phosphor-doping.

Academic Significance and Societal Importance of the Research Achievements

固体高分子形燃料電池正極に用いられている白金系触媒の希少性と、炭素担体の低い耐久性は、燃料電池車の本格普及に対する大きな障壁と考えられてきた。白金系触媒と炭素担体のいずれも用いない酸化物系材料は、燃料電池正極で安定であるものの、性能と比表面積が低いことが課題だった。新たにリン原子を酸化チタン相へ置換導入することにより、その性能と比表面積のどちらも向上することを初めて見出した点が、本研究の学術的意義である。上述した本格普及に対する二つの課題を解決し得る材料を、安価で簡易な手法で合成した点が社会的な意義である。

Report

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

    (21 results)

All 2019 2018 2017 Other

All Journal Article (3 results) (of which Peer Reviewed: 3 results,  Open Access: 3 results) Presentation (14 results) (of which Int'l Joint Research: 9 results,  Invited: 3 results) Book (1 results) Remarks (2 results) Patent(Industrial Property Rights) (1 results)

  • [Journal Article] Phosphor and Nitrogen Co-doped Rutile TiO2 Covered on TiN for Oxygen Reduction Reaction in Acidic Media2019

    • Author(s)
      Mitsuharu Chisaka* and Hiroyuki Morioka
    • Journal Title

      Catalysis Science & Technology

      Volume: 9 Issue: 3 Pages: 611-619

    • DOI

      10.1039/c8cy01973h

    • Related Report
      2018 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Active Site Formation for Oxygen Reduction Reaction on Carbon-Support-Free Titanium Oxynitride with Boosted Activity in Acidic Media2018

    • Author(s)
      Mitsuharu Chisaka, Yusuke Yamamoto, Noriaki Itagaki and Yuhei Hattori
    • Journal Title

      ACS Applied Energy Materials

      Volume: 1 Issue: 1 Pages: 211-219

    • DOI

      10.1021/acsaem.7b00100

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Open Access
  • [Journal Article] Creation of Oxygen Reduction Reaction Active Sites on Titanium Oxynitride Without Increasing the Nitrogen Doping Level2018

    • Author(s)
      Mitsuharu Chisaka
    • Journal Title

      Physical Chemistry Chemical Physics

      Volume: 20 Issue: 23 Pages: 15613-15617

    • DOI

      10.1039/c8cp01420e

    • Related Report
      2017 Research-status Report
    • Peer Reviewed / Open Access
  • [Presentation] Group IV Metal Oxynitride Catalysts for Polymer Electrolyte Fuel Cells Cathodes2019

    • Author(s)
      Mitsuharu Chisaka
    • Organizer
      ACS 257th National meeting
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research / Invited
  • [Presentation] Creation of Active Sites on Phosphor and Nitrogen Co-doped Rutile TiO2 for Polymer Electrolyte Fuel Cell Cathodes2019

    • Author(s)
      Mitsuharu Chisaka and Hiroyuki Morioka
    • Organizer
      25th Topical meeting of ISE
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] リン・窒素共置換による酸化チタン酸素還元触媒の高活性化2019

    • Author(s)
      千坂光陽
    • Organizer
      第12回新電極触媒シンポジウム&宿泊セミナー
    • Related Report
      2019 Annual Research Report
    • Invited
  • [Presentation] Enhancement of Oxygen Reduction Reaction Activity on Phosphor and Nitrogen Co-doped TiO2 catalyst for Polymer Electrolyte Fuel Cell Cathodes2019

    • Author(s)
      Mitsuharu Chisaka
    • Organizer
      8th European Fuel Cell Technology and Applications Piero Lunghi Conference
    • Related Report
      2019 Annual Research Report
    • Int'l Joint Research
  • [Presentation] 酸化チタン系酸素還元触媒の活性点形成過程に関する研究2019

    • Author(s)
      千坂光陽、盛岡弘幸
    • Organizer
      電気化学会第86回大会
    • Related Report
      2018 Research-status Report
  • [Presentation] Enhanced Oxygen Reduction Reaction Activity of Carbon-Support-Free Titanium Oxynitride Catalyst by Phosphor Doping2018

    • Author(s)
      Mitsuharu Chisaka
    • Organizer
      69th annual meeting of ISE
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] Phosphor and Nitrogen Codoped Rutile TiO2 on TiN for Oxygen Reduction Reaction in Acidic Media2018

    • Author(s)
      Mitsuharu Chisaka
    • Organizer
      AiMES2018 (234th ECS and 2018 SMEQ joint meeting)
    • Related Report
      2018 Research-status Report
    • Int'l Joint Research
  • [Presentation] リン・窒素共置換による酸化チタン触媒の高活性化2018

    • Author(s)
      千坂光陽
    • Organizer
      第59回電池討論会
    • Related Report
      2018 Research-status Report
  • [Presentation] Enhancement of Oxygen Reduction Reaction Activity on Carbon-Support-Free Titanium Oxynitride Catalyst by Pyrolysis under Reductive Atmosphere2018

    • Author(s)
      Mitsuharu Chisaka
    • Organizer
      EHEC 2018
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] Nitrogen-Doped Titanium Oxide as Cathode Catalyst for Polymer Electrolyte Fuel Cells2017

    • Author(s)
      Mitsuharu Chisaka
    • Organizer
      EMN meeting on fuel cells 2017
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research / Invited
  • [Presentation] Titanium Oxynitride for Polymer Electrolyte Fuel Cell Cathodes Utilizing Neither Platinum Catalyst Nor Carbon Supports2017

    • Author(s)
      Mitsuharu Chisaka, Yusuke Yamamoto and Noriaki Itagaki
    • Organizer
      HYPOTHESIS XII
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] Oxygen Reduction Reaction Activity of Carbon-Support-Free Titanium Oxynitride with Reduced Catalyst Loading2017

    • Author(s)
      Mitsuharu Chisaka and Yusuke Yamamoto
    • Organizer
      232nd ECS meeting
    • Related Report
      2017 Research-status Report
    • Int'l Joint Research
  • [Presentation] チタン酸窒化物酸素還元触媒の活性点と耐久性に関する研究2017

    • Author(s)
      千坂 光陽,服部 裕平
    • Organizer
      第10回 新電極触媒シンポジウム&宿泊セミナー
    • Related Report
      2017 Research-status Report
  • [Presentation] 担体フリーチタン酸窒化物触媒の使用量低減と酸素還元活性2017

    • Author(s)
      千坂 光陽,山本 悠介
    • Organizer
      第58回電池討論会
    • Related Report
      2017 Research-status Report
  • [Book] Electrocatalysts for Low Temperature Fuel Cells: Fundamentals and Recent Trends2017

    • Author(s)
      Claude Lamy, N. Rajalakshmi, R. Imran Jafri, K.S. Dhathathreyan, Ayan Mukherjee, Suddhasatwa Basu, Thandavarayan Maiyalagan, Subbiah Maheswari, Viswanathan S. Saji, Mitsuharu Chisaka, Chilan Ngo, Michael J. Dzara, Sarah Shulda, Radoslav R. Adzic et al.
    • Total Pages
      588
    • Publisher
      Wiley-VCH
    • ISBN
      9783527341320
    • Related Report
      2017 Research-status Report
  • [Remarks] 弘前大学 大学院理工学研究科千坂研究室ホームページ

    • URL

      http://www.eit.hirosaki-u.ac.jp/~chisaka/

    • Related Report
      2019 Annual Research Report
  • [Remarks] 弘前大学千坂研究室ホームページ

    • URL

      http://www.eit.hirosaki-u.ac.jp/~chisaka/

    • Related Report
      2018 Research-status Report 2017 Research-status Report
  • [Patent(Industrial Property Rights)] 燃料電池用触媒、電極触媒層、膜電極接合体、固体高分子形燃料電池、燃料電池用触媒の製造方法、および、電極触媒層の製造方法2019

    • Inventor(s)
      盛岡弘幸,小澤まどか,千坂光陽
    • Industrial Property Rights Holder
      弘前大学他
    • Industrial Property Rights Type
      特許
    • Industrial Property Number
      2019-200163
    • Filing Date
      2019
    • Related Report
      2019 Annual Research Report

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Published: 2017-04-28   Modified: 2021-02-19  

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