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2010 Fiscal Year Final Research Report

Interdisciplinary study for the elucidation of metalloenzyme reaction mechanism in dioxygen activation and highly efficient molecular catalyst creation

Research Project

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Project/Area Number 20200050
Research Category

Grant-in-Aid for Scientific Research on Innovative Areas (Research a proposed research project)

Allocation TypeSingle-year Grants
Research Field Chemistry related to living body
Inorganic chemistry
Research InstitutionKyushu University

Principal Investigator

LIU Jin-Gang  Kyushu University, 先導物質化学研究所, 特任准教授 (70380540)

Co-Investigator(Kenkyū-buntansha) OHTA Takehiro  九州大学, 先導物質化学研究所, 助教 (70509950)
Co-Investigator(Renkei-kenkyūsha) OGURA Takashi  兵庫県立大学, 生命理学研究科, 教授 (70183770)
YODA Yoshitaka  (財)高輝度光科学研究センター, 主幹研究員 (90240366)
Project Period (FY) 2008 – 2010
Keywords酵素 / モデル化 / 生体分子 / 生体機能化学 / 生物無機化学 / 分子触媒化学 / 酸化触媒
Research Abstract

The O_2 activation/reduction reaction is one of the most important reactions involved in both of life processes and in energy converting systems such as fuel cells. This project is intended to further elucidation of the O_2 activation mechanism of metalloenzymes and creation of highly efficient molecular catalyst for O_2-reduction. Using well designed heme enzyme chemical models, we have successfully captured and fully characterized key intermediates involved in the O_2-activation processes of heme-containing enzymes by various kinds of spectroccopies as well as quantum chemical calculations. These studies have contributed significantly to the understanding of the mechanism of dioxygen activation by heme enzymes and their models. The prepared non-precious-metal catalysts will have prosperous applications as the cathode oxygen reduction reaction (ORR) catalysts in fuel cells.

  • Research Products

    (47 results)

All 2011 2010 2009 2008

All Journal Article (5 results) (of which Peer Reviewed: 4 results) Presentation (42 results)

  • [Journal Article] Probing dioxygen activation mechanisms in heme- containing enzymes by heme models2011

    • Author(s)
      J.-G.Liu ; Y.Naruta
    • Journal Title

      Indian J.Chem. 50A

      Pages: 363-373

    • Peer Reviewed
  • [Journal Article] Formation of an End-On Ferric Peroxo Intermediate upon One-Electron Reduction of a Ferric Superoxo Heme2010

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

      J.Am.Chem.Soc. 132

      Pages: 3672-3673

    • Peer Reviewed
  • [Journal Article]2009

    • Author(s)
      J.-G.Liu ; T.Ohta ; Y.Yamaguchi ; T.Ogura ; S.Sakamoto ; Y.Maeda; Y.Naruta
    • Journal Title

      Angew.Chem.Int.Ed. 48

      Pages: 9262-9267

    • Peer Reviewed
  • [Journal Article] Using Synthetic Models to Probe the O_2 Metabolic Mechanism in Heme-Containing Enzymes2009

    • Author(s)
      J.-G.Liu ; T.Ohta ; F.Tani ; Y.Naruta
    • Journal Title

      G-COE Journal 3

      Pages: 30-36

  • [Journal Article] Synthesis and Characterization of a New Prostaglandin H Synthase Model2009

    • Author(s)
      J.J.Reddy, T.Ohta, Y.Naruta
    • Journal Title

      Tetrahedron Letters 50

      Pages: 3418-3421

    • Peer Reviewed
  • [Presentation] 酸素活性化ヘム酵素モデル錯体の振動分光学的研究2011

    • Author(s)
      太田雄大・劉勁剛・成田吉徳・依田芳卓・斎藤真器名・小林康浩・瀬戸誠
    • Organizer
      日本化学会第91春季年会
    • Place of Presentation
      横浜
    • Year and Date
      2011-03-29
  • [Presentation] 新規三核化配位子を用いた多核銅酸化酵素モデル錯体の合成と性質2011

    • Author(s)
      安部慶郎・太田雄大・成田吉徳
    • Organizer
      日本化学会第91春季年会
    • Place of Presentation
      横浜
    • Year and Date
      2011-03-29
  • [Presentation] Preparation and spectroscopic characterization of the elusive heme-nitroxyl complexes2011

    • Author(s)
      J.-G.Liu, T.Ohta, Y.Naruta
    • Organizer
      The 91^<th> Annual Meeting of Chemical Society of Japan
    • Place of Presentation
      Yokohama
    • Year and Date
      2011-03-26
  • [Presentation] Preparation of Bio-inspired Catalyst for O_2 Reduction2011

    • Author(s)
      P.Nagaraju, J.-G.Liu, T.Ohta, Y.Naruta
    • Organizer
      The 91^<th> Annual Meeting of Chemical Society of Japan
    • Place of Presentation
      Yokohama
    • Year and Date
      2011-03-26
  • [Presentation] Bio-inspired Model Compounds for Oxygen Activation and Reduction2011

    • Author(s)
      J.-G.Liu,T.Ohta, Y.Naruta
    • Organizer
      I2CNER Workshop, Kyushu University
    • Place of Presentation
      Fukuoka
    • Year and Date
      2011-02-04
  • [Presentation] Solution Capturing End-On Peroxo and Hydroperoxo Intermediates of Heme Enzymes2010

    • Author(s)
      J.-G.Liu, T.Ohta; Y.Shimizu,uta
    • Organizer
      2010 International Chemical Congress of Pacific Basin Societies (PACIFICHEM 2010)
    • Place of Presentation
      Honolulu/USA
    • Year and Date
      2010-12-19
  • [Presentation] Activation and catalytic reduction of dioxygen : Lessons from heme enzyme chemical models2010

    • Author(s)
      Y.Naruta, J.-G.Liu, T.Ohta, A.C.Maity, Y.Shimizu, F.Tani
    • Organizer
      2010 International Chemical Congress of Pacific Basin Societies (PACIFICHEM 2010)
    • Place of Presentation
      Honolulu/USA
    • Year and Date
      2010-12-17
  • [Presentation] 酸素活性化ヘム酵素のモデル化学と分光学2010

    • Author(s)
      太田雄大
    • Organizer
      第一回統合物質シンポジウム「統合創製物質化学の現状と展望」
    • Place of Presentation
      京都
    • Year and Date
      2010-12-03
  • [Presentation] Capturing Ferrous-Superoxo, Ferric- Peroxo and Ferric-Hydroperoxo Intermediates in Heme Models2010

    • Author(s)
      J.-G.Liu, T.Ohta ; Y.Naruta
    • Organizer
      60th Anniversary Conference on Coordination Chemistry Chem.Commun.Symposium
    • Place of Presentation
      Osaka
    • Year and Date
      2010-09-28
  • [Presentation] Efficient Electrocatalytic Water Oxidation with Manganese and Cobalt Porphyrin Dimers-ITO Assembly2010

    • Author(s)
      Z.N.Zaharan・太田雄大・成田吉徳
    • Organizer
      第60回錯体化学討会
    • Place of Presentation
      大阪
    • Year and Date
      2010-09-28
  • [Presentation] Synthetic Heme Models Mimic the Formation of Peroxo- and Hydroperoxo- heme Intermediates Relevant to Dioxygen Activation in Heme-containing Enzymes2010

    • Author(s)
      J.-G.Liu, T.Ohta ; Y.Naruta
    • Organizer
      Asian International Symposium on Inorganic Chemistry and Coordination Chemistry, Organo-metallic Chemistry
    • Place of Presentation
      Osaka
    • Year and Date
      2010-03-28
  • [Presentation] Spectroscopic characteri- zation of side-on and end-on (hydro)peroxo-heme intermediates2010

    • Author(s)
      J.-G.Liu ; T.Ohta ; Y.Shimizu ; Y.Naruta
    • Organizer
      The 90^<th> Annual Meeting of Chemical Society of Japan
    • Place of Presentation
      Osaka
    • Year and Date
      2010-03-28
  • [Presentation] 三座窒素配位子配位銅錯体を有するヘム-銅二核錯体の酸素活性化反応2010

    • Author(s)
      太田雄大・千代健文・谷文都・成田吉徳
    • Organizer
      日本化学会第90春季年会
    • Place of Presentation
      大阪
    • Year and Date
      2010-03-28
  • [Presentation] 新規銅三核化配位子誘導体を用いた多核銅酸化酵素モデル錯体の合成と性質2010

    • Author(s)
      安部慶郎・太田雄大・成田吉徳
    • Organizer
      日本化学会第90春季年会
    • Place of Presentation
      大阪
    • Year and Date
      2010-03-28
  • [Presentation] 鉄ポルフィリンニトリド架橋錯体の合成と酸化反応2010

    • Author(s)
      王昂・太田雄大・成田吉徳
    • Organizer
      日本化学会第90春季年会
    • Place of Presentation
      大阪
    • Year and Date
      2010-03-28
  • [Presentation] マンガンポルフィリンダイマー修飾ITO電極を用いる低過電圧での水の酸化反応2010

    • Author(s)
      Z.N.Zahran・太田雄大・王昂・成田吉徳
    • Organizer
      日本化学会第90春季年会
    • Place of Presentation
      大阪
    • Year and Date
      2010-03-28
  • [Presentation] 新規マンガンコロネットポルフィリン錯体によるプロスタグランジン-H合成酵素のモデル反応2010

    • Author(s)
      J.J.Reddy・太田雄大・成田吉徳
    • Organizer
      日本化学会第90春季年会
    • Place of Presentation
      大阪
    • Year and Date
      2010-03-26
  • [Presentation] Spectroscopic Characterization of Peroxo/Hydroperoxo Heme Intermediates : Opening a Closed Side-on Peroxy to an End-on Hydroperoxy2010

    • Author(s)
      J.-G.Liu, T.Ohta ; Y.Naruta
    • Organizer
      The 10^<th> International Workshop on Future Molecular Systems-Recent Development in Phorphyrin-related Chemistry
    • Place of Presentation
      Fukuoka
    • Year and Date
      2010-02-19
  • [Presentation] Mn-Porphyrin as a New Prostaglandin H Synthase Model : Its Catalytic Oxygenation of All-cis-Polyenes2010

    • Author(s)
      J.J.Reddy, T.Ohta, Y.Naruta
    • Organizer
      大学間連携第3回物質合成国際シンポジウム
    • Place of Presentation
      名古屋
    • Year and Date
      2010-01-07
  • [Presentation] ヘムーペルオキソ種の合成と分光学による同定2009

    • Author(s)
      太田雄大・劉勁剛・千代健文・谷文都・成田吉徳
    • Organizer
      大学間連携第5回物質合成シンポジウム
    • Place of Presentation
      京都府
    • Year and Date
      2009-11-19
  • [Presentation] Efficient Electrolytic Water Oxidation with Manganese Porphyrin Dimer Catalysts Assembled on ITO Electrodes2009

    • Author(s)
      Z.N.Zahran, T.Ohta, A.Wang, Y.Naruta
    • Organizer
      第42回酸化反応討論会
    • Place of Presentation
      仙台
    • Year and Date
      2009-11-15
  • [Presentation] 鉄ポリフィリンニトリド架橋錯体の合成と酸化反応2009

    • Author(s)
      王昂・太田雄大・成田吉徳
    • Organizer
      第42回酸化反応討論会
    • Place of Presentation
      仙台
    • Year and Date
      2009-11-15
  • [Presentation] 位フッ素置換されたマンガンポルフィリン二量体の合成と高原子価種の同定2009

    • Author(s)
      田尾和也・太田雄大・成田吉徳
    • Organizer
      第59回錯体化学討論会
    • Place of Presentation
      長崎
    • Year and Date
      2009-09-26
  • [Presentation] Synthetic heme models to mimic the formation of ferric peroxo and hydroperoxo intermediates involved in heme-containing enzymes2009

    • Author(s)
      J.-G.Liu, T.Ohta, Y.Shimizu, Y.Naruta
    • Organizer
      The 59^<th> Symposium of Coordination Chemical Society of Japan
    • Place of Presentation
      Nagasaki
    • Year and Date
      2009-09-26
  • [Presentation] 鉄ポルフィリンニトリド架橋錯体の合成と酸化反応2009

    • Author(s)
      王昂・太田雄大・成田吉徳
    • Organizer
      第59回錯体化学討論会
    • Place of Presentation
      長崎
    • Year and Date
      2009-09-25
  • [Presentation] Mn-Porphyrin models of prostaglandin H synthases and their catalytic oxygenation of all-cis-polyenes2009

    • Author(s)
      J.J.Reddy, T.Ohta, Y.Naruta
    • Organizer
      第24回生体機能関連化学シンポジウム
    • Place of Presentation
      福岡
    • Year and Date
      2009-09-15
  • [Presentation] Preparation of Low-spin End-on Ferric-Peroxo and Ferric- Hydroperoxo Species by a Heme Model Complex Bearing an Imidazole Tail2009

    • Author(s)
      J.-G.Liu, T.Ohta, S.Yamaguchi, T.Ogura, Y.Naruta
    • Organizer
      The 14^<th> International Conference on Biological Inorganic Chemistry (ICBIC-14)
    • Place of Presentation
      Nagoya
    • Year and Date
      2009-07-27
  • [Presentation] A novel dioxygen activation by a heme-copper binuclear complex2009

    • Author(s)
      T.Ohta, T.Chishiro, F.Tani, Y.Naruta
    • Organizer
      14th International Conference on Biological Inorganic Chemistry (ICBIC-14)
    • Place of Presentation
      Nagoya
    • Year and Date
      2009-07-27
  • [Presentation] Simulation of O_2 activation/reduction with enzyme active site models of terminal oxidases2009

    • Author(s)
      Y.Naruta, J.-G.Liu, T.Ohta, T.Ogura
    • Organizer
      The 14^<th> International Conference on Biological Inorganic Chemistry (ICBIC-14)
    • Place of Presentation
      Nagoya
    • Year and Date
      2009-07-26
  • [Presentation] Spectroscopic Characterization of End-on Heme Peroxide and Hydroperoxide Intermediates Relevant to Dioxygen Activation Mechanism of Heme-containing Enzymes2009

    • Author(s)
      J.-G.Liu, T.Ohta ; Y.Naruta
    • Organizer
      PreICBIC-Frontiers in Bioinorganic Chemistry
    • Place of Presentation
      Fukuoka
    • Year and Date
      2009-07-24
  • [Presentation] ヘム含有酸化酵素活性部位モデルとしてのフッ素化ポルフィリン鉄錯体の合成2009

    • Author(s)
      劉歓・劉勁剛・成田吉徳
    • Organizer
      日本化学会第89春季年会
    • Place of Presentation
      石川県
    • Year and Date
      2009-03-29
  • [Presentation] カルボキシル基を導入した鉄ポルフィリンの合成および酸素との反応2009

    • Author(s)
      清水雄太・太田雄大・劉勁剛・谷文都・成田吉徳
    • Organizer
      日本化学会第89春季年会
    • Place of Presentation
      石川県
    • Year and Date
      2009-03-28
  • [Presentation] side-onおよびend-on型ペルオキソ-およびヒドロペルオキソヘムの合成と分光法による同定2009

    • Author(s)
      劉勁剛・太田雄大・山口悟・小倉尚志・成田吉徳
    • Organizer
      日本化学会第89春季年会
    • Place of Presentation
      千葉県
    • Year and Date
      2009-03-27
  • [Presentation] ヘム鉄・銅二核錯体における新規酸素活性化反応2009

    • Author(s)
      太田雄大・千代建文・谷文都・成田吉徳
    • Organizer
      日本化学会第89春季年会
    • Place of Presentation
      千葉県
    • Year and Date
      2009-03-27
  • [Presentation] 酸素活性化金属酵素の反応機構解明に向けてのモデル化学と分光学2009

    • Author(s)
      太田雄大
    • Organizer
      第3回核共鳴散乱研究会
    • Place of Presentation
      兵庫県
    • Year and Date
      2009-03-11
  • [Presentation] 生体金属のダイナミックな配位・電子構造の制御-ヘム、非ヘム鉄蛋白質を例に2008

    • Author(s)
      太田雄大
    • Organizer
      第46回日本生物物理学会(シンポジウム:遷移金属の生物物理-若手研究者の挑戦)
    • Place of Presentation
      福岡県
    • Year and Date
      2008-12-03
  • [Presentation] ヘム、非ヘム鉄酵素の分光学とモデル錯体化学、物質合成研究拠点機関関連事業2008

    • Author(s)
      太田雄大
    • Organizer
      第3回大学間連携若手フォーラム
    • Place of Presentation
      福岡県
    • Year and Date
      2008-11-21
  • [Presentation] Using Synthetic Models to Probe the Dioxygen Metabolic Mechanism in the Terminal Enzyme of Respiratory2008

    • Author(s)
      劉 勁剛
    • Organizer
      G-COE「物質・エネルギー変換ユニット」ワークショップ
    • Place of Presentation
      福岡県
    • Year and Date
      2008-11-12
  • [Presentation] Near-IR MCD of the Non-Heme Ferrous Active Site in Naphthalene 1,2-Dioxygenase : Correlation to Crystallography and Structural Insight into the Mechanism of Rieske Dioxygenases2008

    • Author(s)
      T.Ohta, S.Chakrabarty, J.D.Lipscomb, E.I.Solomon
    • Organizer
      The 4^<th> Asian Biological Inorganic Chemistry Conference
    • Place of Presentation
      Jeju/Korea
    • Year and Date
      2008-11-11
  • [Presentation] 生体金属酵素活性中心の分光学とモデル錯体化学2008

    • Author(s)
      太田雄大
    • Organizer
      バイオミメティックス-東北大多元研、九大先導研、北大電子研合同研究会
    • Place of Presentation
      東京都
    • Year and Date
      2008-10-30
  • [Presentation] Selective Preparation of Superoxo, Peroxo, and Hydroperoxo Species Relating to Heme-Containing Oxygenase and Peroxidase2008

    • Author(s)
      劉勁剛・太田雄大・小倉尚志・成田吉徳
    • Organizer
      第58回錯体化学討論会
    • Place of Presentation
      石川県
    • Year and Date
      2008-09-21
  • [Presentation] カルボキシル基を導入した鉄ポルフィリンの合成および酸素との反応2008

    • Author(s)
      清水雄太・太田雄大・劉勁剛・谷文都・成田吉徳
    • Organizer
      第58回錯体化学討論会
    • Place of Presentation
      石川県
    • Year and Date
      2008-09-20

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Published: 2012-02-13   Modified: 2016-04-21  

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