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金属ポルフィリン錯体触媒による超高エネルギー効率での水分解/酸素発生

Research Project

Project/Area Number 10F00037
Research Category

Grant-in-Aid for JSPS Fellows

Allocation TypeSingle-year Grants
Section外国
Research Field Inorganic chemistry
Research InstitutionKyushu University

Principal Investigator

成田 吉徳  九州大学, 先導物質化学研究所, 教授

Co-Investigator(Kenkyū-buntansha) ZAHRAN ZakiN.  九州大学, 先導物質化学研究所, 外国人特別研究員
ZAHRAN Zaki N  九州大学, 先導物質化学研究所, 外国人特別研究員
Project Period (FY) 2010 – 2012
Project Status Completed (Fiscal Year 2012)
Budget Amount *help
¥2,300,000 (Direct Cost: ¥2,300,000)
Fiscal Year 2012: ¥400,000 (Direct Cost: ¥400,000)
Fiscal Year 2011: ¥900,000 (Direct Cost: ¥900,000)
Fiscal Year 2010: ¥1,000,000 (Direct Cost: ¥1,000,000)
Keywords水分解 / 過電圧 / 電解触媒 / 水素生成 / エネルギー効率 / 水の酸化 / 卑金属イオン / 水の分解触媒 / 電解
Research Abstract

水の4電子酸化反応は、植物等の光合成における当該反応の研究から水素エネルギー社会におけるグリーン水素の効率的生産に至るまで、環境に負荷を与えず、かつ理論的に高効率で物理エネルギー(光、電力など)を化学エネルギー(燃焼等によりへと変換する反応として重要であり、世界中で急速に研究展開されている領域である。現在、世界中で競って研究がされている「人工光合成」反応の成否は如何に水を低エネルギーで完全分解できるかにかかっている。この目的を実現するため本年度は次の目標で研究を進め、以下の成果を得た。
1.開発した水分解触媒の人工光合成系への適用
本研究で開発したマンガンポルフィリン二量体は極めて低過電圧で水分解を触媒的に行える。この電気化学的特性は、色素増感型太陽電池における増感色素の酸化体の還元電位と水の酸化電位の中間に位置する。そこで色素増感太陽電池の原理を適用し、ルテニウム錯体とマンガンポルフィリン二量体を二酸化チタンナノ粒子表面に共修飾した電極を用いて水溶液中において可視光照射による水分解反応を行った。その結果、バイアス電位を電極間に適用すること無く、光照射により色素吸収長波長末端670nmまで光応答電流が観測され、475nmにおける量子収率は約3%に達した。また、光照射による酸素/水素発生が観測され、その定量により90%以上の電流効率で水分解が可能となった。
2.コバルト錯体による水分解反応
各種金属錯体を検討することにより、新たに含窒素配位子を持つコバルト錯体が水分解に適した性能を有することを見いだした。水溶性錯体として均一水溶液中での電解を行うと中性溶液付近で過電圧が最小となった。また、この電極を用いて連続水分解反応を行うと24時間後においても電解電流の低下は見られず高い耐久性を有していることが明らかとなった。

Report

(3 results)
  • 2012 Annual Research Report
  • 2011 Annual Research Report
  • 2010 Annual Research Report
  • Research Products

    (27 results)

All 2013 2012 2011 2010 Other

All Journal Article (5 results) (of which Peer Reviewed: 5 results) Presentation (21 results) Remarks (1 results)

  • [Journal Article] Axial Ligand Effects on Vibrational Dynamics of Iron in Heme Carbonyl Studied by Nuclear Resonance Vibrational Spectroscopy2013

    • Author(s)
      T. Ohta, J. -G. Liu, and Y. Naruta
    • Journal Title

      Coord. Chem. Rev.

      Volume: 257 Issue: 2 Pages: 407-413

    • DOI

      10.1016/j.ccr.2012.05.009

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Crystal structure and catalytic mechanism of aldoxime dehydratase involved in carbon-nitrogen triple bond synthesis2013

    • Author(s)
      J. Nomura, H. Hashimoto, T. Ohta, Y. Hashimoto, K. Wada, Y. Naruta, K. Oinuma M. Kobayashi
    • Journal Title

      Proc. Natl. Acad. Sci. USA,

      Volume: 110 Pages: 2810-2815

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Molecular Engineering of indoline based organic panchromatic sensitizers for highly efficient dye-sensitized solar cells2012

    • Author(s)
      B. Liu, Q. Liu, X. Li, D. You, Y. Naruta, W. Zhu
    • Journal Title

      J. Material. Chem.

      Volume: 22 Issue: 26 Pages: 13348-13356

    • DOI

      10.1039/c2jm31704d

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Photophysical Analyses of 1,10-Phenanthroline- Embedded Porphyrin Analogues and Their Magnesium(II) Complexes2012

    • Author(s)
      M. Ishida, J. -M. Lim, B. -S. Lee, F. Tani, J. L Sessler, D. Kim, Y. Naruta
    • Journal Title

      Chem. Eur. J.

      Volume: 18 Issue: 45 Pages: 14329-14341

    • DOI

      10.1002/chem.201201793

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Journal Article] Axial Ligand Effects on Vibrational Dynamics of Iron in Heme Carbonyl Studied by Nuclear Resonance Vibrational Spectroscopy2012

    • Author(s)
      T. Ohta, J.-G, Liu, M. Saito, Y. Kobayashi, Y. Yoda, M. Seto, Y. Naruta
    • Journal Title

      J. Phys. Chem. B

      Volume: 116 Pages: 13831-13838

    • Related Report
      2012 Annual Research Report
    • Peer Reviewed
  • [Presentation] Studying the mechanism of molecular catalyst fixation on the nanoporous Ti02 thin film developed by chemical and thermal treatments of titanium metal for water splitting and fuel cell applications2013

    • Author(s)
      R. Khanna, S. Yamaguch, T. Matsushita, T. Kokubo, Y. Naruta, T. Ohta, and H. Takadama
    • Organizer
      The 37th International Conference and Exposition on Advanced Ceramics and Composites
    • Place of Presentation
      Florida (USA)
    • Related Report
      2012 Annual Research Report
  • [Presentation] 金属酵素活性中心化学モデルから分子触媒へ2013

    • Author(s)
      成田 吉徳
    • Organizer
      分子抖学研究所研究会「生体配位化学の最前線と展望」
    • Place of Presentation
      分子科学研究所(岡崎)(招待講演) )
    • Related Report
      2012 Annual Research Report
  • [Presentation] 色素-触媒共修飾電極を用いた効率的な水の光分解反応2013

    • Author(s)
      劉 博、ZAHRAN, Zaki, N.、太田雄大、成田 吉徳
    • Organizer
      第93回日本化学会春期年会
    • Place of Presentation
      立命館大学(滋賀)
    • Related Report
      2012 Annual Research Report
  • [Presentation] Efficient p-CuO photocathode for solar hydrogen production2013

    • Author(s)
      Z. N. Zahran, E. A. Mohamed, T. Ohta, Y. Naruta
    • Organizer
      第93回日本化学会春期年会
    • Place of Presentation
      立命館大学(滋賀)
    • Related Report
      2012 Annual Research Report
  • [Presentation] 太陽光による二酸化炭素還元を目指したRu-Re光触媒系2013

    • Author(s)
      MOHAMED, Eman, A., ZAHRAN, Zaki, N., 太田雄大, 成田 吉徳
    • Organizer
      第93回日本化学会春期年会
    • Place of Presentation
      立命館大学(滋賀)
    • Related Report
      2012 Annual Research Report
  • [Presentation] Oxygen Reduction : From Cytochrome c Oxidase to Molecular Catalysts for Fuel Cells2012

    • Author(s)
      Y. Naruta
    • Organizer
      The 6th Asian Symposium on Biological Inorganic Chemistry
    • Place of Presentation
      Hong Kong Polytech University (Hong Kong)(招待講演) )
    • Year and Date
      2012-11-06
    • Related Report
      2012 Annual Research Report
  • [Presentation] 色素/触媒共修飾電極を用いた光化学的水分解反応2012

    • Author(s)
      劉博、Zaharan Zaki、太田雄大、成田吉徳
    • Organizer
      2012年 光化学討論会
    • Place of Presentation
      東京工業大学(東京)
    • Year and Date
      2012-09-12
    • Related Report
      2012 Annual Research Report
  • [Presentation] Catalytic dloxygen reduction : From metalloenzyme models to molecular catalysts2012

    • Author(s)
      Y. Naruta, T. Ohta, J. -G. Liu, A. C. Maity and N. Permandla
    • Organizer
      The 7th Internatiolnal Conference on Porphyrins and Phthalocvanines
    • Place of Presentation
      Jeju (Korea)(招待講演) )
    • Year and Date
      2012-07-03
    • Related Report
      2012 Annual Research Report
  • [Presentation] Bio-inspired 分子触媒による酸素還元反応2012

    • Author(s)
      成田 吉徳
    • Organizer
      第3回統合物質シンポジウム「新エネルギと物質創製」
    • Place of Presentation
      九州大学西新プラザ(福岡)(招待講演) )
    • Related Report
      2012 Annual Research Report
  • [Presentation] Synthesis of a Ru dye-Re Catalyst dyad for photochemical C02 reduction2012

    • Author(s)
      Eman A. Mohamed, Z. N. Zahran, B. Liu, T. Ohta, Y. Naruta
    • Organizer
      第62回錯体化学討論会
    • Place of Presentation
      富山大学(富山)
    • Related Report
      2012 Annual Research Report
  • [Presentation] Molecular catalyst catalyst fixation mechanism on the surfaces surfaces of chemically and of chemically and thermally treated titanium electrodefor2012

    • Author(s)
      R. Khanna, T. Matsushita, T. Kokubo, Y. Naruta, and H.
    • Organizer
      IUMRS-International Conference on Electronic
    • Place of Presentation
      パシフィコ(横浜)
    • Related Report
      2012 Annual Research Report
  • [Presentation] Molecular catalyst design for efficient energy conversion2011

    • Author(s)
      Y.Naruta
    • Organizer
      The 2011Global COE International Symposium on Future Molecular Systems
    • Place of Presentation
      九州大学(招待講演)
    • Year and Date
      2011-11-25
    • Related Report
      2011 Annual Research Report
  • [Presentation] Oxygen activation with bio-inspired molecular catalysts2011

    • Author(s)
      Y.Naruta
    • Organizer
      3rd Dalton Transactions International Symposium Bioinorganic Chemistry
    • Place of Presentation
      九州大学(招待講演)
    • Year and Date
      2011-11-16
    • Related Report
      2011 Annual Research Report
  • [Presentation] Electrocatalytic water oxidation with a cobalt porphyrin dimer catalyst assembled on metal oxide electrodes2011

    • Author(s)
      Z.N.Zahran, T.Ohta, Y.Naruta
    • Organizer
      錯体化学会第61回討論会
    • Place of Presentation
      岡山理科大学
    • Year and Date
      2011-09-17
    • Related Report
      2011 Annual Research Report
  • [Presentation] Efficient water oxidation with a robust hexaphosphonate-manganese porphyrin dimer catalyst anchored to ITO surface2011

    • Author(s)
      E.A.Mohamed, Z.N.Zahran, T.Ohta, Y.Naruta
    • Organizer
      錯体化学会第61回討論会
    • Place of Presentation
      岡山理科大学
    • Year and Date
      2011-09-17
    • Related Report
      2011 Annual Research Report
  • [Presentation] Development of Water-Oxidation Molecular Catalysts toward Artificial Photosynthesis2011

    • Author(s)
      Y.Naruta
    • Organizer
      The 1st International Conference on MEXT Project of Integrated Research on Chemical Synthesis
    • Place of Presentation
      札幌 invited
    • Year and Date
      2011-01-25
    • Related Report
      2010 Annual Research Report
  • [Presentation] Efficient water oxidation with cobalt and manganese porphyrin dimers assembled on metal oxide surface2011

    • Author(s)
      Z.N.Zahran, T.Ohta, Y.Naruta
    • Organizer
      International Conference on Activation of Dioxygen and Homogeneous Catalytic Oxidation-2011
    • Place of Presentation
      沖縄・万国津梁館
    • Related Report
      2011 Annual Research Report
  • [Presentation] Efficient water oxidation with a robust hexaphosphonate-manganese porphyrin dimer catalyst anchored to ITO surface2011

    • Author(s)
      E.A.Mohamed, Z.N.Zahran, T.Ohta, Y.Naruta
    • Organizer
      International Conference on Activation of Dioxygen and Homogeneous Catalytic Oxidation-2011
    • Place of Presentation
      沖縄・万国津梁館
    • Related Report
      2011 Annual Research Report
  • [Presentation] Efficient Electrocatalytic Water Oxidation with Manganese and Cobalt Porphyrin Dimers-ITO assembly2010

    • Author(s)
      Zaki N.Zahran, Takehiro Ohta, Yoshinori Naruta
    • Organizer
      The 60th Anniversary Conference on Coordination Chemistry
    • Place of Presentation
      大阪
    • Related Report
      2010 Annual Research Report
  • [Presentation] Efficient Electrocatalytic Water Oxidation with Manganese and Cobalt Porphyrin Dimers Assembled to Metal Oxide Electrodes2010

    • Author(s)
      Zaki N.Zahran, Takehiro Ohta, Yoshinori Naruta
    • Organizer
      第43回酸化反応討論会
    • Place of Presentation
      東京
    • Related Report
      2010 Annual Research Report
  • [Presentation] Electrocatalytic water oxidation at low overpotentials by modified manganese porphyrin dimers assembled on ITO electrode2010

    • Author(s)
      Zaki N.Zahran, Takehiro Ohta, Yoshinori Naruta
    • Organizer
      The 2010 International Chemical Congress of Pacific Basin Societies (PACIFICHEM-2010)
    • Place of Presentation
      ホノルル、米国
    • Related Report
      2010 Annual Research Report
  • [Remarks]

    • URL

      http://narutalab.ifoc.kyushu-u.ac.jp

    • Related Report
      2010 Annual Research Report

URL: 

Published: 2010-12-03   Modified: 2024-03-26  

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